Valley Selectivity Manipulation via Interfacial Magnon-Exciton Interactions in TMD/CrSBr Antiferromagnetic van der Waals Heterostructures

Valley Selectivity Manipulation via Interfacial Magnon-Exciton Interactions in TMD/CrSBr Antiferromagnetic van der Waals Heterostructures | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Article Valley Selectivity Manipulation via Interfacial Magnon-Exciton Interactions in TMD/CrSBr Antiferromagnetic van der Waals Heterostructures Chongyun Jiang, Xilin Zhang, Yaojie Zhu, Ruixue Bai, Runcheng Mao, and 7 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-5909229/v1 This work is licensed under a CC BY 4.0 License Status: Posted Version 1 posted You are reading this latest preprint version Abstract Valley properties of monolayer (ML) transition metal dichalcogenide (TMDs) can be effectively manipulated via magnetic proximity effects in van der Waals (vdW) heterostructures (HS) stacked with 2D ferromagnetic materials and ML TMDs. Antiferromagnetic materials with high-frequency and long-lived coherent magnons, allowing interactions between distinct excitations at the heterointerface, potentially serve as an alternative to valley manipulation via heterostructure constructions, however this remains elusive. Here, we demonstrated the existence of interfacial magnon-exciton interaction (IMEI) in the vdW heterostructure composed of ML MoSe 2 and A-type antiferromagnetic CrSBr with in-plane magnetization. We proposed two mechanisms of IMEI, i.e., magnon-exciton scattering (MES), which induces the blueshift of excitonic states of MoSe 2 below the Néel temperature of CrSBr, and magnon-assisting dark exciton recombination (MADER), which leads to the formation of magnon-exciton complexes. We found that MES induces a remarkable valley polarization (VP) enhancement of excitonic states from a completely quenched level, and the magnon-exciton complexes exhibit an increase in valley-contrasting circular dichroism when the spin orientation of CrSBr switched from in-plane to out-of-plane. Our work provides a new platform for manipulating excitonic and valley properties in non-magnetic semiconductors without external fields, opening up fresh opportunities of hybridized quasiparticles in quantum interconnects and opto-spintronics. Physical sciences/Physics/Electronics, photonics and device physics/Electronic and spintronic devices Physical sciences/Physics/Optical physics/Magneto-optics Physical sciences/Nanoscience and technology/Nanoscale materials/Two-dimensional materials valley selectivity manipulation interfacial magnon-exciton interaction van der Waals heterostructure antiferromagnet transition metal dichalcogenides Figures Figure 1 Figure 2 Figure 3 Figure 4 Introduction TMDs exhibit a number of unique optical features, including strong excitonic effects and valley-contrasting exciton selection rules, making them a promising platform for quantum optics and nanophotonics 1 , 2 . VdW heterostructures, offering the advantage of freely constructing preferred 2D materials independently of their crystal structure, provide new avenues for achieving novel physical properties at their interfaces 3 , 4 . Heterostructures that integrate ML TMDs with 2D magnetic materials are anticipated to effectively manipulate the valley properties of ML TMDs via magnetic proximity effects (MPE) 5 – 7 . Recent reports have demonstrated spontaneous valley splitting and enhanced VP in heterostructures such as MoSe 2 /CrBr 3 8,9 , WSe 2 /CrI 3 10 , WSe 2 /EuS 11 , MoSe 2 /Cr 2 Ge 2 Te 6 12 , WSe 2 /YIG 13 . However, previous studies have primarily focused on the vdW heterointerfaces consisting of the ferromagnetic layers, and the impact of antiferromagnets (AFMs) on the TMD valley properties in AFM/TMD vdW heterostructures remains elusive. AFMs are magnetically ordered, yet with zero net magnetization, which makes them less susceptible to external field perturbation. More importantly, AFMs have high-frequency spin dynamics up to the terahertz (THz) range 14 , which are generally two or three orders of magnitude higher than ferromagnets, along with long-lived coherent magnons 15 , leading to the prominent magnon effect 16 . The hybridization of magnons with other quasiparticles provides potential avenues for the investigation and manipulation of other quasiparticles in TMD/AFM vdW heterostructures 17 – 20 . One example is the IMEI, which have been demonstrated in the heterostructures formed by ML TMDs and Néel-type AFMs 21 – 24 . However, researches on IMEI in TMD/AFM vdW heterostructures are still in its infancy, with studies have primarily revealed the spectral signature and offering limited attention to the process involved in IMEI. In addition, investigations of IMEI remain confined to the vdW heterostructures integrated with TMDs and Néel-type AFMs, which are expected to extend to other types of AFMs, such as the A-type AFM CrSBr 25 , 26 , recently reported to possess strong magnon effect 27 , 28 , enabling a more comprehensive understanding of IMEI involving various magnetic orderings. Furthermore, magnons hold magnetic dipole moments, which enable them directly couple to spin-based qubits through magnetic dipolar coupling 29 . This feature of magnons provides a promising way to manipulate the valley selection properties of TMD via heterointerface exciton-magnon coupling, which, however, remains elusive. In this work, we choose the A-type AFM CrSBr to vertically stack with ML MoSe 2 . The CrSBr crystal is composed of layers with rectangular unit cells in the a-b plane, and stacked along the c axis to produce an orthorhombic structure 14 (Fig. 1 a). Spins within each layer are ferromagnetically align along the crystal b axis, while the interlayer coupling is antiferromagnetic. The in-plane magnetization of CrSBr is misaligned with the out-of-plane spin texture of K (-K) valleys in ML MoSe 2 , which suppresses the impact of spin-dependent charge transfer in MoSe 2 /CrSBr heterostructures, and facilitates the investigation of IMEI and their impact on valley selectivity of ML MoSe 2 . In MoSe 2 /CrSBr heterostructures, we observed a blueshift of MoSe 2 excitonic states (excitons and trions) in the photoluminescence (PL) spectra below the Néel temperature ( T N ~ 132 K) 30 of CrSBr, along with the emergency of a magnon-exciton complex on the low-energy side below 80 K. These phenomena cannot be explained by the magnetic exchange fields (MEF) as observed in ferromagnetic vdW interfaces. Instead, they indicate the existence of IMEI. Based on the exciton g-factors in the ML TMDs and heterostructures, and the comparison of exciton energy shift with magnon energy, we suggest two mechanisms of IMEI: MES and MADER, which result in the blueshift of excitonic states and the formation of magnon-exciton complexes, respectively. We found that MES remarkably enhances the complete quenched zero-field VP of the excitonic states in MoSe 2 /CrSBr, regardless of left-handed ( σ ⁻) or right-handed ( σ + ) circular polarized excitations. The valley-contrasting circular dichroism of magnon-exciton complexes can be increased by switching the spin orientation of CrSBr from in-plane to out-of-plane. Our work sheds light on the process of heterointerface exciton-magnon interactions and reveals their effective impacts on valley manipulation of ML TMD via TMD/AFM heterostructure stacking, paving the way for a novel approach to manipulating quantum information in non-magnetic semiconductors. Results Spectral characteristics of MoSe 2 /CrSBr ML MoSe 2 and CrSBr flake were obtained by mechanical exfoliation, and the heterostructure was assembled using dry-transfer technique, followed by high-vacuum annealing at 200°C to improve interface contact (see Methods for detailed fabrication information). Figure 1 b shows the predicted type-III band alignment of the heterostructure 25 , 31 – 33 , where electrons in the valence band of MoSe 2 transfer to the conduction band of CrSBr upon contact. The efficient charge transfer results in p-doping of the MoSe 2 layer and a significant reduction in PL intensity 25 , 26 (see Supplementary Note 2). Under laser illumination, discrete band bending at the heterojunction prevents photogenerated carriers from transferring between the two materials, with electrons (holes) in MoSe 2 (or CrSBr) dragged out of the junction region back into their respective layers 34 . The normalized PL spectra of MoSe 2 /SiO 2 and the MoSe 2 /CrSBr heterostructure at low temperatures are shown in Fig. 1 c. Unless otherwise specified, all measurements were conducted at 15 K using continuous-wave excitation at 715 nm. Exciton (X) and trion (T) emission in MoSe 2 /SiO 2 are assigned at1.655 eV and 1.627 eV, respectively. In MoSe 2 /CrSBr, the peaks X * and T * exhibit significant blueshifts of ~ 16 meV and ~ 14 meV in contrast to the peaks X and T, respectively. Furthermore, a new peak (M * ) emerges on the low-energy side of the trion (T * ) in MoSe 2 /CrSBr, located at 1.620 eV. The energy differences between M * and T * and between M * and X * are ~ 21 meV and ~ 51 meV, respectively. To reveal the origin of the three peaks in MoSe 2 /CrSBr heterostructure, we conducted the power dependent PL measurement. The PL intensities of three peaks show linear dependence on the excitation power and do not saturate even at high excitation power (Fig. 1 d), indicating their exciton and trion characteristics and excludes the possibilities of biexcitons, localized excitons, or moiré excitons 24 . To further assign the three peaks’ origination, we consider the effects that may arise from the contact between ML MoSe 2 and CrSBr, as well as the subsequent laser irradiation, including variation of the dielectric environment, interlayer charge transfer, MEF induced by the MPE of CrSBr, and interlayer particle interactions. The effect of dielectric environment cannot result in such substantial temperature-dependent blueshift (see below). Interlayer charge transfer can also be excluded to cause the emergence of the three peaks, since no energy shift occurs in this mechanism 35 – 38 . Although an in-plane MEF may lead to a new emission peak via brightening dark excitons, the splitting energy between bright excitons and brightened dark excitons is only 1 ~ 2 meV 39 , 40 , which contradicts our experimental results. Hence, MEF is not the source that contributes to the occurrence of X * , T * and M * . Detailed discussions can be found in the Supplementary Note 3. Therefore, we suggest that the energy blueshift of X * and T * , as well as the emergence of M * , origin from the interlayer particle interactions between ML MoSe 2 and CrSBr, specifically, the interaction between the excitons in MoSe 2 and the magnons in CrSBr. Interfacial magnon-exciton interactions in MoSe/CrSBr To confirm the IMEI in the MoSe 2 /CrSBr heterostructure, we measured the temperature dependence of PL spectra for MoSe 2 /SiO 2 and MoSe 2 /CrSBr (Fig. 2a). Exciton peak energies are extracted and plotted as a function of temperature, as shown in Fig. 2b. We observed that the peak energy of X * in the heterostructure exhibits a significant blueshift compared to the exciton X in ML MoSe 2 . Furthermore, this blueshift energy features not a monotonic decrease with temperature, but shows an increase trend below ~ 70 K, then decreases monotonically, and finally achieves a constant (~ 7.5 meV) above T N of CrSBr. This constant energy difference is attributed to the variation of dielectric environment 21 – 24 . A similar non-monotonic temperature dependence of the blue-shifted energy was also observed in WSe 2 /CrSBr (see Supplementary Note 6), with the same transition temperature of ~ 70 K. The correlation between the energy blueshift of the exciton peak and the antiferromagnetic ordering in CrSBr indicates the existence of IMEI in the MoSe 2 /CrSBr below T N . Figure 2c shows the temperature dependence of the integrated PL intensity of M * . It is evident that the intensity of M * rapidly decreases as the temperature increases and vanishes around 80 K. This process can be described by the Arrhenius Eq. 2 4,41 : $$\:I\left(T\right)=\frac{{I}_{0}}{1+A\bullet\:\text{exp}\left(-\frac{{E}_{\text{a}}}{{k}_{\text{B}}T}\right)},$$ 1 where, I ( T ) represents the integrated intensity at temperature T , I 0 is the integrated intensity at 0 K, A is a constant related to the radiative and non-radiative decay rates, E a denotes the activation energy, and k B is the Boltzmann constant. By fitting the data, the activation energy of M * was determined to be ~ 42 meV, which is close to the energy difference between M * and X (~ 35 meV), considering the blueshift of ~ 7.5 meV induced by the variation of dielectric environment. More importantly, this energy difference (~ 42.5 meV) matches the energy 42 – 44 (~ 45 meV) of a high-energy magnon near the Γ point of the CrSBr Brillouin zone. Since energy splitting of the bright and dark excitons in MoSe 2 is tiny (~ -1.5 meV), it indicates that the emission of M * results from the interaction between bright/dark excitons in MoSe 2 and magnons in CrSBr. We suggest that X * and T * in MoSe 2 /CrSBr as manifestations of MES, while M * originates from MADER, which we identify as a complex of magnons and dark excitons. MADER can be analogous to the interaction between phonons and excitons 38 , 45 , 46 (this possibility can be excluded due to the mismatch between phonon energy 47 and spectral energy shift). Under the incidence of photons carrying zero momentum, magnons (~ 45 meV) near the Γ point in the Brillouin zone are typically excited 14 . From momentum and angular momentum conservation, Γ-point magnons can induce the intravalley spin-flip relaxation of electrons, enabling dark excitons to undergo radiative recombination by emitting magnons (Fig. 2d). This process reduces the dark exciton emission energy by one magnon energy and causes the spectral broadening due to the dispersion of magnons 45 . These assertions are supported by our results that M * exhibits a relatively broad linewidth (~ 41 meV) and a g -factor (-8.75, see Fig. 4 a, with detailed discussion in the Supplementary Note 3) similar to that of intravalley dark exciton recombination 37 , 38 , 48 . Similar results were also observed in the WSe 2 /CrSBr heterostructure (see Supplementary Note 4). Regarding the assignment of X * and T * in the MoSe 2 /CrSBr heterostructure, their energy shift (~ 8.5 meV) is smaller than the energy of a single magnon, and their g -factors reflect the characteristics of excitons and trions (-3.04 and − 4.12, respectively, see Fig. 4 a). Thus, we attribute them to the exciton states in MoSe 2 after elastic or inelastic scattering with the magnon states in CrSBr. In this process (Fig. 2e), the energy and momentum between excitons and magnons are redistributed 49 – 52 , leading to the energy shift of X and T, which correspond to the energy variation of magnons. We further demonstrate that the interlayer exchange coupling, as a short-range interaction, is the requisite to the formation of IMEI in MoSe 2 /CrSBr heterostructures by performing the same experiments in unannealed heterostructures and observing no EMC or MADER. Valley polarization enhanced by MES To investigate the effect of magnons on valley properties of MoSe 2 , we conducted the polarized PL spectra of heterostructure and compared them with ML MoSe 2 , as shown in Fig. 3 a. For easier identification, the PL intensity of MoSe 2 /CrSBr has been normalized to the co-polarized intensity of MoSe 2 /SiO 2 . The co-polarized and cross-polarized trion peaks of heterostructure exhibit an intensity discrepancy, which can be quantitatively evaluated using the VP. For σ + excitation, the VP can be estimated by the formula: P c ( σ + ) = ( I σ ⁺ σ ⁺ - I σ ⁺ σ ⁻ )/( I σ ⁺ σ ⁺ + I σ ⁺ σ ⁻ ), where I σ ⁺ σ ⁺ and I σ ⁺ σ ⁻ are the PL intensities under σ + excitation with co-polarized ( σ + excitation, σ + detection) and cross-polarized ( σ + excitation, σ ⁻ detection) configurations, respectively. For both σ + and σ ⁻ excitation, we obtained ~ 8% and 0% trion VP in MoSe 2 /CrSBr and MoSe 2 /SiO 2 , respectively (Fig. 3 b at B = 0 T). This differs from VP enhancement caused by MEF or the application of an out-of-plane magnetic field, which enhances the polarization for one helicity of excitation while suppressing it for the opposite helicity. More importantly, all PL peaks in MoSe 2 /CrSBr exhibited enhanced VP at 0 T (Fig. 3 a), indicating a breakthrough of zero VP in ML MoSe 2 , while it is challenging to increase VP by conventional methods (e.g., charge transfer 9 , doping 53 , and MEF 12 ) due to the fast valley depolarization rate caused by electron–hole exchange interaction. To understand the zero-field VP enhancement in the heterostructure, we measured VP dependence on an out-of-plane magnetic field (Fig. 3 b). It shows obviously linear variations of VP with the magnetic field in MoSe 2 /CrSBr, with rates of ~ 2.4%/T and ~ -2.2%/T for σ ± excitation, respectively. This linear dependence indicates that the zero-field VP enhancement is not determined by the spin orientation of CrSBr. Otherwise, the VP would display a larger tunability below the saturation field H s ( ~ ± 2 T) 54 in contrast to above H s , due to the combined effect of the external magnetic field and the spin-dependent interlayer charge transfer or effective magnetic field induced by the spin reorientation of CrSBr 9 , 10 . Besides, the intervalley charge transfer can be also excluded as the origin of the VP enhancement, as it would lead to an increase in trion VP and a decrease in exciton VP. This contradicts our results, which show an enhancement of exciton VP by ~ 16% in the heterostructure (see Supplementary Note 5 and 6). To find out the origin of the zero-field VP enhancement in MoSe 2 /CrSBr, we conducted the temperature dependence of the VP in the heterostructure. As shown in Fig. 3 c, the VP enhancement of trions in MoSe 2 /CrSBr decreases with temperature increasing and disappears around 130 K, which is close to the T N of CrSBr, indicating the association between the VP enhancement and the magnetism of CrSBr. We suggest that the zero-field enhancement of VP results from the MES of MoSe 2 /CrSBr heterostructure. This interaction weakens the electron-hole exchange interaction, resulting in the VP increasing. Specifically, the electron-hole exchange interaction in ML TMDs acts as an effective in-plane magnetic field B eff , which depends on the center-of-mass momentum k of excitons and drives the precession of valley pseudospin 55 , as illustrated in Fig. 3 d. Whenever a scattering event occurs, the direction of the exciton's center-of-mass momentum changes randomly, causing the B eff direction changing as well 55 . Since spin precession occurs between two scattering events, more frequent scattering result in more frequent changes in the direction of B eff . This reduces the mean free time of excitonic states, thereby decreasing the time-averaged B eff experienced by excitonic states 55 , leading to the weakening of intervalley relaxation and an increase in VP of excitonic states. In our work, magnons in CrSBr carry a transient magnetization with the oscillating direction along the c-axis 15 , 56 , 57 . These magnons provide a THz-frequency oscillating magnetic field and interact with excitonic states in MoSe 2 . The oscillating magnetic field of the magnons, along with the MES, reduces the time-averaged B eff by causing more frequent changes in B eff , leading to a weakened electron-hole exchange interaction and an increase in VP of excitonic states. Valley properties of magnon-exciton complex We investigated the valley properties of M * and its magnetic response under an out-of-plane magnetic field B . First, we extracted the g -factor by measuring polarized PL spectra with g = Δ E / µ B B , where Δ E = E σ ⁺ σ ⁺ - E σ ⁻ σ ⁻ , and E σ ⁺ σ ⁺( σ ⁻ σ ⁻) represents co-polarized PL peak energy under σ + ( σ ⁻) excitation, and µ B is the Bohr magneton, as shown in Fig. 4 a. The g -factor of M * is ~ -8.75, which is similar to the g -factor of intravalley dark exciton recombination, supporting the assignment of M * as the magnon-assisted radiative recombination of dark excitons. The g -factors of T * (~ -4.12) and X * (~ -3.04) keep the characteristics of trions and excitons. Then, we focus on the dependence of the VP of M * on the external out-of-plane magnetic field. We observe an asymmetric V-shaped pattern (Fig. 4 b), which is different from the linear dependence of T * and T in Fig. 3 b. We suggest that this asymmetry originates from the combined effects of Zeeman effect and electron-hole exchange interactions. Although both Zeeman effect and exchange interactions influence the VP, they respond differently to the out-of-plane magnetic field. In absence of magnetic field, valley degeneracy is preserved. When a positive magnetic field is exerted, Zeeman effect causes the energy of the K (-K) valley downshift (upshift), leading to more carriers relaxing into K (-K) valley. Thus, Zeeman splitting enhances (reduces) the VP for σ + excitation under positive (negative) magnetic fields, resulting in a linear dependence of VP with the magnetic field. In contrast, the electron-hole exchange interaction is weakened by an out-of-plane magnetic field in either direction due to the lifting of valley degeneracy 58 , which suppresses intervalley relaxation. Stronger magnetic field results in greater suppression. Consequently, VP manifests a symmetric V-shaped dependence on the magnetic field under the electron-hole exchange interaction mechanism. We established a theoretical model of VP contributed by both the Zeeman effect and electron-hole exchange interaction, using a four-level system (details in the Supplementary Note 8). This model well fits the experimental results and allows for the separation of the contributions of two mechanisms to the VP, as shown in Fig. 4 c. Based on the fitting parameters, the zero-field intervalley relaxation rate resulting from the electron-hole exchange interaction is ~ 42.5 times larger than that caused by the Zeeman effect, revealing that the electron-hole exchange interaction dominates zero-field VP of M * . Under the framework of this model, we can interpret the linear dependence of VP on the magnetic field for T * and T in Fig. 3 b as predominated by the mechanism of Zeeman effect. Finally, we discuss the impact of CrSBr spin orientation on the valley properties of M * , which can be estimated by the valley contrasting circular dichroism (VCCD) between two valleys with ρ = ( I σ ⁺ σ ⁺ - I σ ⁻ σ ⁻ )/( I σ ⁺ σ ⁺ + I σ ⁻ σ ⁻ ). Figure 4 d shows the VCCD of T * , T, and M * dependence on the out-of-plane magnetic field. It can be observed that the VCCDs of T * and T show a linear variation with the magnetic field, with a slope of ~ 2.4%/T. In contrast, VCCD of M * exhibits an S-shaped variation, with a sharp changing rate (~ 2.2%/T) within H s of CrSBr and a slower rate (~ 0.1%/T) beyond H s . This S-shaped behavior suggests that, the VCCD of M * is also modulated by the spin orientation of CrSBr in addition to the direct effect of the magnetic field. In the absence of magnetic field, the energy band preserve spin degenerate in CrSBr due to the anti-parallel spin orientation of adjacent layers along the b-axis, resulting in an equal population of magnons with the angular momentum of -1 and + 1. Thus, the impact of magnons in CrSBr on the VCCD is balanced, as shown in Fig. 4 e. When we applied a positive (negative) out-of-plane magnetic field lower than H s of CrSBr, the spin orientation gradually canted towards + c (-c) axis as the magnetic field increase, breaking the spin degeneracy, and the population of magnons with angular momentum of -1 (+ 1) exceeded that with angular momentum of + 1 (-1), as shown in Fig. 4 f. Since the M * emission with photon angular momentum of + 1 (-1) occurs via magnons with − 1 (+ 1) angular momentum coupling with dark excitons in K (-K) valley, the M * emission in K (-K) valley enhanced, resulting in a rapid increase of VCCD with the magnetic field. When B = H s ( B = - H s ), magnetization along the + c (-c) axis reaches saturation. There are only magnons with angular momentum of -1 (+ 1). Thus, the contribution of the spin orientation to the VCCD would no longer increases as the magnetic field increases, leading to a slower changing rate of VCCD with the magnetic field. We notice a slight tunability of VCCD when the magnetic field exceeds H s , that is, when the slope of VCCD is solely influenced by the magnetic field. This suggests that the intervalley scattering of M * is less affected by Zeeman effect, which is in line with the above discussion on the VP of M * . The S-shaped variation of VCCD with the magnetic field cannot attributed to the MEF or spin-dependent interlayer charge transfer induced by the spin orientation of CrSBr, as no additional energy splitting within H s was observed in Fig. 4 a, and no S-shaped VCCD was observed in T * . We note that our finding can be well reproduced in WSe 2 /CrSBr heterostructure system (see Supplementary Note 7), demonstrating the IMEI widely exist in TMD/CrSBr heterostructures. In summary, we have demonstrated the existence of two types of IMEI, MES and MADER, in TMD/CrSBr systems and thoroughly investigated their impacts on the excitonic states and valley properties of ML TMDs. MES induces a blueshift in the excitonic states of ML TMDs in the TMD/CrSBr heterostructure below the T N of CrSBr and enhances the VP of all emission peaks under both σ ⁺ and σ + excitations. The latter can be attributed to the suppression of intervalley electron-hole exchange interactions by magnons. More importantly, MES offers an effective and field-free method to enhance a completely quenched VP of ML MoSe 2 , which is challenging to achieve through other methods such as doping, MEF, or charge transfer. On the other hand, MADER leads to the formation of dark exciton-magnon complexes, which can be observed in PL spectra. The complexes exhibit g -factors similar to that of their original dark excitons, and display asymmetric V-shaped VP and S-shaped VCCD variations with magnetic field, which respectively indicate a valley depolarization mechanism dominated by intervalley electron-hole exchange interactions and valley selectivity enhanced by magnons. Our findings provide a new platform for manipulating the excitonic and valley properties of non-magnetic semiconductors, highlighting the critical role of hybridized quasiparticles in TMD/AFM heterostructures and opening up exciting opportunities in the fields of quantum information science, opto-spintronics and valleytronics. Methods Sample preparation. A few layer CrSBr flake is mechanically exfoliated from bulk CrSBr crystals by scotch tape (3M Scotch), and then are transferred on a clean SiO 2 /Si substrate. The thickness of SiO 2 is about 285 nm. The CrSBr flake was then thermally annealed at 250°C for 2h in a high vacuum (~ 10 − 6 mbar) atmosphere. ML MoSe 2 exfoliated from bulk crystals (HQ Graphene) is transferred on the top of CrSBr flake using the dry-transfer technique and polydimethylsiloxane (PDMS) substrate. Next, the device is thermally annealed at 200°C for 2h in a high vacuum (~ 10 − 6 mbar) atmosphere to improve the interface contact. Magneto-optical spectroscopy. PL spectroscopy were performed by a lab-built confocal microscope system. The sample was mounted in a close-cycle cryostat (Opticool, Quantum Design) with a piezo-units (attocube system, ANPx101, ANPx101, and ANPz102). The temperature was set to T = 15 K, and the magnetic field was up to ± 7 T. We focused the laser beam onto the sample using an objective lens (Nikon, 50×, N.A. = 0.6), with a spot diameter of 1 µm. PL spectra with 715 nm excitation were obtained with a Ti:sapphire laser (TiF-100ST-F10-AU, Avesta) in continuous wave mode, and rotating 750 nm short-pass (FESH0750, Thorlabs) and long-pass (FELH0750, Thorlabs) filters were used to remove the laser line. For PL spectra with 670 nm excitation, a picosecond laser diode (PLDD-20M, ALPHALAS GmbH) was used in continuous wave mode, and 700 nm short-pass (FESH0700, Thorlabs) and long-pass (FELH0700, Thorlabs) filters were used to remove the laser line. Both excitation and detection were circularly polarized, with the polarization of the excitation light initialized by a vertically oriented polarizer and controlled by a half-wave plate (AHWP05M-600, Thorlabs) and a quarter-wave plate (AQWP05M-600, Thorlabs). The optical system in the collection path was similar to the excitation optical system. The waveplates were mounted on a motorized rotary stage to automate the experiment. The signal was analyzed using a spectrometer (Shamrock 500i, Oxford Instruments) with a CCD camera (iDus CCD 420). Declarations Author contributions H.L. and Z.S. synthesized CrSBr crystals. X.Z., H.M., and C.J. designed the research. X.Z. performed sample preparation with the assistance of Y.Z., R.M., and Z.Y. X.Z. performed optical measurements with the assistance of X.D., R.Z., and Y.T. X.Z. performed data processing with the assistance of R.B. and C.J. X.Z., H.M., and C.J. analyzed and discussed the data. X.Z., H.M., and C.J. wrote the paper. All authors commented on the manuscript. Competing interests The authors declare no competing interest. Acknowledgements This work was supported by the National Natural Science Foundation of China (62374095, 61974075, and 61704121), the National Key Technologies R&D Program of China (2022YFB2803900), the Natural Science Foundation of Tianjin City (19JCQNJC00700 and 22JCZDJC00460), the Scientific Research Project of Tianjin Municipal Education Commission (2019KJ028), and the Fundamental Research Funds for the Central Universities of Nankai University (22JCZDJC00460). C.J. acknowledges the Tianjin Key Laboratory of Efficient Utilization of Solar Energy and the Engineering Research Center of Thin Film Optoelectronics Technology, Ministry of Education of China. Z.S. was supported by ERC-CZ program (project LL2101) from Ministry of Education Youth and Sports (MEYS) and by the project Advanced Functional Nanorobots (reg. No. CZ.02.1.01/0.0/0.0/15_003/0000444 financed by the EFRR). References Regan, E. C. et al. Emerging exciton physics in transition metal dichalcogenide heterobilayers. Nature Reviews Materials 7 , 778-795 (2022). Li, W., Lu, X., Wu, J. & Srivastava, A. Optical control of the valley Zeeman effect through many-exciton interactions. Nature Nanotechnology 16 , 148-152 (2021). Geim, A. K. & Grigorieva, I. V. Van der Waals heterostructures. Nature 499 , 419-425 (2013). Novoselov, K. S., Mishchenko, A., Carvalho, A. & Castro Neto, A. H. 2D materials and van der Waals heterostructures. Science 353 , aac9439 (2016). Norden, T. et al. Giant valley splitting in monolayer WS 2 by magnetic proximity effect. Nature Communications 10 , 4163 (2019). Huang, B. et al. Emergent phenomena and proximity effects in two-dimensional magnets and heterostructures. Nature Materials 19 , 1276-1289 (2020). Mak, K. F., Shan, J. & Ralph, D. C. Probing and controlling magnetic states in 2D layered magnetic materials. Nature Reviews Physics 1 , 646-661 (2019). Choi, J., Lane, C., Zhu, J.-X. & Crooker, S. A. Asymmetric magnetic proximity interactions in MoSe 2 /CrBr 3 van der Waals heterostructures. Nature Materials 22 , 305-310 (2023). Lyons, T. P. et al. Interplay between spin proximity effect and charge-dependent exciton dynamics in MoSe 2 /CrBr 3 van der Waals heterostructures. Nature Communications 11 , 6021 (2020). Zhong, D. et al. Van der Waals engineering of ferromagnetic semiconductor heterostructures for spin and valleytronics. Science Advances 3 , e1603113. Zhao, C. et al. Enhanced valley splitting in monolayer WSe 2 due to magnetic exchange field. Nature Nanotechnology 12 , 757-762 (2017). Zhang, T. et al. Electrically and Magnetically Tunable Valley Polarization in Monolayer MoSe 2 Proximitized by a 2D Ferromagnetic Semiconductor. Advanced Functional Materials 32 , 2204779 (2022). Zheng, H. et al. Enhanced valley polarization in WSe 2 /YIG heterostructures via interfacial magnetic exchange effect. Nano Research 16 , 10580-10586 (2023). Bae, Y. J. et al. Exciton-coupled coherent magnons in a 2D semiconductor. Nature 609 , 282-286 (2022). Sun, Y. et al. Dipolar spin wave packet transport in a van der Waals antiferromagnet. Nature Physics 20 , 794-800 (2024). Cenker, J. et al. Direct observation of two-dimensional magnons in atomically thin CrI 3 . Nature Physics 17 , 20-25 (2021). Liu, S. et al. Direct Observation of Magnon-Phonon Strong Coupling in Two-Dimensional Antiferromagnet at High Magnetic Fields. Physical Review Letters 127 , 097401 (2021). Dirnberger, F. et al. Magneto-optics in a van der Waals magnet tuned by self-hybridized polaritons. Nature 620 , 533-537 (2023). Lin, K. et al. Strong Exciton–Phonon Coupling as a Fingerprint of Magnetic Ordering in van der Waals Layered CrSBr. ACS Nano 18 , 2898-2905 (2024). Cui, J. et al. Chirality selective magnon-phonon hybridization and magnon-induced chiral phonons in a layered zigzag antiferromagnet. Nature Communications 14 , 3396 (2023). Onga, M. et al. Antiferromagnet–Semiconductor Van Der Waals Heterostructures: Interlayer Interplay of Exciton with Magnetic Ordering. Nano Letters 20 , 4625-4630 (2020). Liu, C. et al. Probing the Néel-Type Antiferromagnetic Order and Coherent Magnon–Exciton Coupling in Van Der Waals VPS 3 . Advanced Materials 35 , 2300247 (2023). Zhao, S.-X. et al. Interlayer Interaction of Excitons and Magnons in Graphene/WS 2 /Néel-Type Manganese Phosphorus Trichalcogenide Heterostructures. Advanced Functional Materials 34 , 2405882 (2024). Zhang, Y. et al. Magnon-Coupled Intralayer Moiré Trion in Monolayer Semiconductor–Antiferromagnet Heterostructures. Advanced Materials 34 , 2200301 (2022). Serati de Brito, C. et al. Charge Transfer and Asymmetric Coupling of MoSe 2 Valleys to the Magnetic Order of CrSBr. Nano Letters 23 , 11073-11081 (2023). Beer, A. et al. Proximity-Induced Exchange Interaction and Prolonged Valley Lifetime in MoSe 2 /CrSBr Van-Der-Waals Heterostructure with Orthogonal Spin Textures. ACS Nano 18 , 31044-31054 (2024). Wilson, N. P. et al. Interlayer electronic coupling on demand in a 2D magnetic semiconductor. Nature Materials 20 , 1657-1662 (2021). Brennan, N. J., Noble, C. A., Tang, J., Ziebel, M. E. & Bae, Y. J. Important Elements of Spin-Exciton and Magnon-Exciton Coupling. ACS Physical Chemistry Au 4 , 322-327 (2024). Candido, D. R., Fuchs, G. D., Johnston-Halperin, E. & Flatté, M. E. Predicted strong coupling of solid-state spins via a single magnon mode. Materials for Quantum Technology 1 , 011001 (2021). Lee, K. et al. Magnetic Order and Symmetry in the 2D Semiconductor CrSBr. Nano Letters 21 , 3511-3517 (2021). Wang, C. et al. A family of high-temperature ferromagnetic monolayers with locked spin-dichroism-mobility anisotropy: MnNX and CrCX (X = Cl, Br, I; C = S, Se, Te). Science Bulletin 64 , 293-300 (2019). Gao, Y., Liu, Q., Zhu, Y., Jiang, X. & Zhao, J. Magnetic field modulated photoelectric devices in ferromagnetic semiconductor CrXh (X = S/Se, h = Cl/Br/I) van der Waals heterojunctions. Applied Physics Letters 119 , 032103 (2021). Durán Retamal, J. R., Periyanagounder, D., Ke, J.-J., Tsai, M.-L. & He, J.-H. Charge carrier injection and transport engineering in two-dimensional transition metal dichalcogenides. Chemical Science 9 , 7727-7745 (2018). Lee, J. et al. Modulation of Junction Modes in SnSe 2 /MoTe 2 Broken-Gap van der Waals Heterostructure for Multifunctional Devices. Nano Letters 20 , 2370-2377 (2020). Jiang, Y., Chen, S., Zheng, W., Zheng, B. & Pan, A. Interlayer exciton formation, relaxation, and transport in TMD van der Waals heterostructures. Light: Science & Applications 10 , 72 (2021). Le, C. T. et al. Negative Valley Polarization of the Intralayer Exciton via One-Step Growth of H-Type Heterobilayer WS 2 /MoS 2 . ACS Nano 17 , 2629-2638 (2023). Yang, M. et al. Relaxation and darkening of excitonic complexes in electrostatically doped monolayer WSe 2 : Roles of exciton-electron and trion-electron interactions. Physical Review B 105 , 085302 (2022). He, M. et al. Valley phonons and exciton complexes in a monolayer semiconductor. Nature Communications 11 , 618 (2020). Robert, C. et al. Measurement of the spin-forbidden dark excitons in MoS 2 and MoSe 2 monolayers. Nature Communications 11 , 4037 (2020). Robert, C. et al. Fine structure and lifetime of dark excitons in transition metal dichalcogenide monolayers. Physical Review B 96 , 155423 (2017). Huang, J., Hoang, T. B. & Mikkelsen, M. H. Probing the origin of excitonic states in monolayer WSe 2 . Scientific Reports 6 , 22414 (2016). Scheie, A. et al. Spin Waves and Magnetic Exchange Hamiltonian in CrSBr. Advanced Science 9 , 2202467 (2022). Pawbake, A. et al. Magneto-Optical Sensing of the Pressure Driven Magnetic Ground States in Bulk CrSBr. Nano Letters 23 , 9587-9593 (2023). Uykur, E. et al. Phonon and magnon dynamics across antiferromagnetic transition in 2D layered van der Waals material CrSBr. Preprint at https://arxiv.org/abs/2405.07853 (2024). Kudlacik, D. et al. Exciton and exciton-magnon photoluminescence in the antiferromagnet CuB 2 O 4 . Physical Review B 102 , 035128 (2020). Liu, E. et al. Valley-selective chiral phonon replicas of dark excitons and trions in monolayer WSe 2 . Physical Review Research 1 , 032007 (2019). Lee, D. H., Choi, S.-J., Kim, H., Kim, Y.-S. & Jung, S. Direct probing of phonon mode specific electron–phonon scatterings in two-dimensional semiconductor transition metal dichalcogenides. Nature Communications 12 , 4520 (2021). Li, Z. et al. Phonon-exciton Interactions in WSe 2 under a quantizing magnetic field. Nature Communications 11 , 3104 (2020). Eremenko, V., Kachur, I., Novikov, V., Shapiro, V. J. S. J. o. E. & Physics, T. Scattering of excitons by long-wavelength magnons in the quasi-one-dimensional antiferromagnet CsMnCI 3 .2H 2 O. 67 , 1862 (1988). Cornelissen, L. J., Peters, K. J. H., Bauer, G. E. W., Duine, R. A. & van Wees, B. J. Magnon spin transport driven by the magnon chemical potential in a magnetic insulator. Physical Review B 94 , 014412 (2016). Olsson, K. S. et al. Pure Spin Current and Magnon Chemical Potential in a Nonequilibrium Magnetic Insulator. Physical Review X 10 , 021029 (2020). Streib, S., Vidal-Silva, N., Shen, K. & Bauer, G. E. W. Magnon-phonon interactions in magnetic insulators. Physical Review B 99 , 184442 (2019). Shinokita, K. et al. Continuous Control and Enhancement of Excitonic Valley Polarization in Monolayer WSe 2 by Electrostatic Doping. Advanced Functional Materials 29 , 1900260 (2019). López-Paz, S. A. et al. Dynamic magnetic crossover at the origin of the hidden-order in van der Waals antiferromagnet CrSBr. Nature Communications 13 , 4745 (2022). Hao, K. et al. Direct measurement of exciton valley coherence in monolayer WSe 2 . Nature Physics 12 , 677-682 (2016). Cham, T. M. J. et al. Anisotropic Gigahertz Antiferromagnetic Resonances of the Easy-Axis van der Waals Antiferromagnet CrSBr. Nano Letters 22 , 6716-6723 (2022). Kamimaki, A., Iihama, S., Suzuki, K. Z., Yoshinaga, N. & Mizukami, S. Parametric Amplification of Magnons in Synthetic Antiferromagnets. Physical Review Applied 13 , 044036 (2020). Surrente, A. et al. Intervalley Scattering of Interlayer Excitons in a MoS 2 /MoSe 2 /MoS 2 Heterostructure in High Magnetic Field. Nano Letters 18 , 3994-4000 (2018). Additional Declarations There is NO Competing Interest. Supplementary Files SupplementaryInformation.docx Cite Share Download PDF Status: Posted Version 1 posted You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. 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Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-5909229","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":414974012,"identity":"f60b35a5-59f2-4a19-a7f7-c6f924919fdf","order_by":0,"name":"Chongyun Jiang","email":"data:image/png;base64,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","orcid":"https://orcid.org/0000-0002-6496-2191","institution":"Nankai University","correspondingAuthor":true,"prefix":"","firstName":"Chongyun","middleName":"","lastName":"Jiang","suffix":""},{"id":414974015,"identity":"99ee3809-8949-43a8-8135-145cee65fafc","order_by":1,"name":"Xilin Zhang","email":"","orcid":"","institution":"Nankai University","correspondingAuthor":false,"prefix":"","firstName":"Xilin","middleName":"","lastName":"Zhang","suffix":""},{"id":414974017,"identity":"2176968a-b74f-4af5-b1eb-80050e4c28a8","order_by":2,"name":"Yaojie Zhu","email":"","orcid":"","institution":"Tiangong University","correspondingAuthor":false,"prefix":"","firstName":"Yaojie","middleName":"","lastName":"Zhu","suffix":""},{"id":414974019,"identity":"5f865af7-b73b-4cff-b393-e047b39e7650","order_by":3,"name":"Ruixue Bai","email":"","orcid":"","institution":"Nankai University","correspondingAuthor":false,"prefix":"","firstName":"Ruixue","middleName":"","lastName":"Bai","suffix":""},{"id":414974020,"identity":"fcd8f1df-0387-445a-af0f-c40c24c05864","order_by":4,"name":"Runcheng Mao","email":"","orcid":"","institution":"Nankai University","correspondingAuthor":false,"prefix":"","firstName":"Runcheng","middleName":"","lastName":"Mao","suffix":""},{"id":414974021,"identity":"533c8d61-57f7-45e6-bfb3-37e6ce81b811","order_by":5,"name":"Zuowei Yan","email":"","orcid":"","institution":"Nankai University","correspondingAuthor":false,"prefix":"","firstName":"Zuowei","middleName":"","lastName":"Yan","suffix":""},{"id":414974022,"identity":"5f93e20c-e3a9-4855-8d83-97db0a0e8ee4","order_by":6,"name":"Xiaoshan Du","email":"","orcid":"","institution":"Nankai University","correspondingAuthor":false,"prefix":"","firstName":"Xiaoshan","middleName":"","lastName":"Du","suffix":""},{"id":414974023,"identity":"b8eb80b8-a3f9-454b-95fe-ea223e1f4eb0","order_by":7,"name":"Rui Zhou","email":"","orcid":"","institution":"Tiangong University","correspondingAuthor":false,"prefix":"","firstName":"Rui","middleName":"","lastName":"Zhou","suffix":""},{"id":414974024,"identity":"697130a3-344f-457e-8842-54006943ac47","order_by":8,"name":"Yisen Tang","email":"","orcid":"","institution":"Tiangong University","correspondingAuthor":false,"prefix":"","firstName":"Yisen","middleName":"","lastName":"Tang","suffix":""},{"id":414974025,"identity":"835d8cb2-3950-431b-83a5-82ffe68900c9","order_by":9,"name":"Hui Ma","email":"","orcid":"","institution":"Tiangong University","correspondingAuthor":false,"prefix":"","firstName":"Hui","middleName":"","lastName":"Ma","suffix":""},{"id":414974026,"identity":"f1a96144-88b0-4181-898c-db6b7915ddd2","order_by":10,"name":"Heng Li","email":"","orcid":"","institution":"University of Chemistry and Technology Prague","correspondingAuthor":false,"prefix":"","firstName":"Heng","middleName":"","lastName":"Li","suffix":""},{"id":414974027,"identity":"1982c4ab-d0c0-4261-a38c-ac66c6b5f12b","order_by":11,"name":"Zdenek Sofer","email":"","orcid":"https://orcid.org/0000-0002-1391-4448","institution":"University of Chemistry and Technology Prague","correspondingAuthor":false,"prefix":"","firstName":"Zdenek","middleName":"","lastName":"Sofer","suffix":""}],"badges":[],"createdAt":"2025-01-27 04:15:11","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-5909229/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-5909229/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":78652292,"identity":"f6ac5470-558f-4786-894c-a425e71e0ac2","added_by":"auto","created_at":"2025-03-17 08:41:50","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":2675067,"visible":true,"origin":"","legend":"\u003cp\u003eSample structure and PL Spectra of MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr heterostructure. (a) Schematic diagram of the MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr heterostructure. Grey arrows in CrSBr represent the spin orientation. (b) Band alignment of MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr and the transfer of photogenerated carriers under laser irradiation. The transfer of photogenerated carriers in MoSe\u003csub\u003e2\u003c/sub\u003e and CrSBr are shown in orange and purple curved arrows, respectively. (c) Normalized PL spectra and fitting results of MoSe\u003csub\u003e2\u003c/sub\u003e/SiO\u003csub\u003e2\u003c/sub\u003e and MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr at 15 K under excitation of 715 nm. (d) Excitation power (\u003cem\u003eP\u003c/em\u003e) dependence of the integrated PL intensity (\u003cem\u003eI\u003c/em\u003e) of M\u003csup\u003e*\u003c/sup\u003e, T\u003csup\u003e*\u003c/sup\u003e, and X\u003csup\u003e*\u003c/sup\u003e peaks in MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr. Solid curves show \u003cem\u003eI\u003c/em\u003e ∝ \u003cem\u003eP\u003c/em\u003e\u003csup\u003e\u003cem\u003eα\u003c/em\u003e\u003c/sup\u003e fitting, along with their \u003cem\u003eα\u003c/em\u003e value.\u003c/p\u003e","description":"","filename":"floatimage1.png","url":"https://assets-eu.researchsquare.com/files/rs-5909229/v1/b1ad67af2d900cfd55e00a35.png"},{"id":78651184,"identity":"6a635581-1c72-4d63-b2cb-f9f5776aff50","added_by":"auto","created_at":"2025-03-17 08:33:50","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":1506686,"visible":true,"origin":"","legend":"\u003cp\u003eTemperature dependence of PL. (a) Normalized PL spectra of MoSe\u003csub\u003e2\u003c/sub\u003e/SiO\u003csub\u003e2\u003c/sub\u003e (blue) and MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr (red) at different temperatures. X and X\u003csup\u003e* \u003c/sup\u003epeaks are marked by blue and red triangles, respectively. (b) Temperature dependence of the exciton energy in MoSe\u003csub\u003e2\u003c/sub\u003e/SiO\u003csub\u003e2\u003c/sub\u003e (X) and MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr (X\u003csup\u003e*\u003c/sup\u003e), with the energy difference between X\u003csup\u003e*\u003c/sup\u003e and X shown on the right axis. The solid green line is the guide line. (c) Temperature dependence of PL intensity of M\u003csup\u003e*\u003c/sup\u003e in MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr. Activation energy (\u003cem\u003eE\u003c/em\u003e\u003csub\u003ea\u003c/sub\u003e) are obtained by fitting with Eq. (1) (solid curve). (d) Schematic diagram of MADER process. Red (blue) solid lines represent spin-up (down) band-edge states. The dark exciton decay in the K valley is accompanied by the emission of a left-handed (|L⟩) magnon and a right-handed (|R⟩) photon. This process reduces the dark exciton emission energy by one magnon energy (from the spin-down conduction band in the K valley to the black dashed line). (e) Schematic diagram of MES process, energy (\u003cem\u003eω\u003c/em\u003e) and momentum (\u003cem\u003ek\u003c/em\u003e) redistributed between excitons and magnons.\u003c/p\u003e","description":"","filename":"floatimage2.png","url":"https://assets-eu.researchsquare.com/files/rs-5909229/v1/412486860e85bab80e8495df.png"},{"id":78652295,"identity":"711d442c-9d69-4b4d-919a-5f687126ce25","added_by":"auto","created_at":"2025-03-17 08:41:50","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":5174532,"visible":true,"origin":"","legend":"\u003cp\u003eVP dependence on out-of-plane magnetic field and temperature. (a) Normalized co- and cross-polarized PL spectra of MoSe\u003csub\u003e2\u003c/sub\u003e/SiO\u003csub\u003e2\u003c/sub\u003e and MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr under \u003cem\u003eσ\u003c/em\u003e\u003csup\u003e+\u003c/sup\u003e excitation. VP are extracted and shown with green and purple curves. (b) VP of trions (T, T\u003csup\u003e*\u003c/sup\u003e) as a function of out-of-plane magnetic field under \u003cem\u003eσ\u003c/em\u003e\u003csup\u003e+\u003c/sup\u003e (solid symbols) and \u003cem\u003eσ\u003c/em\u003e\u003csup\u003e-\u003c/sup\u003e excitation (empty symbols) in MoSe\u003csub\u003e2\u003c/sub\u003e/SiO\u003csub\u003e2\u003c/sub\u003e and MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr. Solid and dashed lines are linear fitting results. (c) Temperature dependence of trions VP in MoSe\u003csub\u003e2\u003c/sub\u003e/SiO\u003csub\u003e2\u003c/sub\u003e and MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr. The solid lines are the guide lines. (d) Schematic diagram of magnon-enhanced VP via weakening the electron-hole exchange interaction. The up panel describes the VP evolving with time, which is divided into three stages, free of magnon scattering (I and Ⅲ) and exciton-magnon scattering (Ⅱ). The down panel shows the physical process. The electron-hole exchange interaction acts as an effective in-plane magnetic field \u003cem\u003e\u003cstrong\u003eB\u003c/strong\u003e\u003c/em\u003e\u003csub\u003eeff\u003c/sub\u003e (yellow arrows), which drives the precession of exciton valley pseudospin (red arrows), resulting in VP decreasing. The out-of-phase precession of the sublattice spins\u003cem\u003e \u003c/em\u003e\u003cem\u003e\u003cstrong\u003eS\u003c/strong\u003e\u003c/em\u003e\u003csub\u003e1\u003c/sub\u003e and \u003cem\u003e\u003cstrong\u003eS\u003c/strong\u003e\u003c/em\u003e\u003csub\u003e2\u003c/sub\u003e (blue arrows) leads to a net magnetization \u003cem\u003e\u003cstrong\u003eM\u003c/strong\u003e\u003c/em\u003e\u003csub\u003ez\u003c/sub\u003e with amplitude oscillation along out-of-plane direction. The oscillation amplitude of \u003cem\u003e\u003cstrong\u003eM\u003c/strong\u003e\u003c/em\u003e\u003csub\u003ez\u003c/sub\u003e is denoted as Δ\u003cem\u003e\u003cstrong\u003eM\u003c/strong\u003e\u003c/em\u003e\u003csub\u003ez\u003c/sub\u003e (purple arrow). When excitons are scattered by magnons (orange arrow), the spin precession is prohibited, which suppresses VP decreasing.\u003c/p\u003e","description":"","filename":"floatimage3.png","url":"https://assets-eu.researchsquare.com/files/rs-5909229/v1/d46ce76a0561311d860da1b7.png"},{"id":78651183,"identity":"2576b92c-5cfd-4662-9ad5-e709b1ef62a8","added_by":"auto","created_at":"2025-03-17 08:33:50","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":1737773,"visible":true,"origin":"","legend":"\u003cp\u003eValley properties of exciton-magnon complexes (M*) in MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr. (a) Valley splitting Δ\u003cem\u003eE\u003c/em\u003e of the M\u003csup\u003e*\u003c/sup\u003e, T\u003csup\u003e*\u003c/sup\u003e, and X\u003csup\u003e*\u003c/sup\u003e. The solid lines represent linear fits results. (b) VP of M\u003csup\u003e*\u003c/sup\u003e dependence on magnetic field under \u003cem\u003eσ\u003c/em\u003e\u003csup\u003e+ \u003c/sup\u003eand \u003cem\u003eσ\u003c/em\u003e⁻ excitation. Solid lines are guide lines. (c) Fitting of VP under \u003cem\u003eσ\u003c/em\u003e\u003csup\u003e+ \u003c/sup\u003eexcitation with a theoretical model contributed by Zeeman effect and electron-hole exchange interaction. (d) Magnetic field dependence of VCCD of M\u003csup\u003e*\u003c/sup\u003e, T\u003csup\u003e*\u003c/sup\u003e, and T. Dashed black lines indicate ±\u003cem\u003eH\u003c/em\u003e\u003csub\u003es\u003c/sub\u003e, solid green line is the guide line, while blue and orange dashed lines are the linear fittings of T\u003csup\u003e*\u003c/sup\u003e and T, respectively. (e-f) Schematic diagram of MADER process at \u003cem\u003eB\u003c/em\u003e = 0 (e) and 0 \u0026lt; \u003cem\u003eB\u003c/em\u003e \u0026lt; \u003cem\u003eH\u003c/em\u003e\u003csub\u003es\u003c/sub\u003e (f). Red (blue) solid lines represent spin-up (down) band-edge states, while red and blue solid circles represent electrons with spin-up and spin-down, respectively. Spin-up and spin-down electrons in CrSBr are allowed to form magnons with angular momentum of -1 (green wavy arrow) and +1 (orange wavy arrow), respectively, which are allowed to couple with dark excitons in the K and -K valleys, respectively. When the energy band of CrSBr is spin-degenerate at \u003cem\u003eB\u003c/em\u003e = 0 (e), the population of spin-up and spin-down electrons equals, and the influence of magnons on valley contrasting is balanced. When the spin-degeneracy is broken at 0 \u0026lt; B \u0026lt; \u003cem\u003eH\u003c/em\u003e\u003csub\u003es\u003c/sub\u003e (f), more spin-up electrons in CrSBr leads to stronger MADER emission from the K valley.\u003c/p\u003e","description":"","filename":"floatimage4.png","url":"https://assets-eu.researchsquare.com/files/rs-5909229/v1/a4aa2b36e9a05d553976a6da.png"},{"id":99307407,"identity":"e7a698e7-4a7f-4e76-94cc-8dcf736f130a","added_by":"auto","created_at":"2025-12-31 16:06:13","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":11306172,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-5909229/v1/84378863-da9f-4af4-b7f9-ab038e9a9a33.pdf"},{"id":78652298,"identity":"4ba1b326-93b4-433b-86e9-2d5dc9b15aa2","added_by":"auto","created_at":"2025-03-17 08:41:50","extension":"docx","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":16596794,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cbr\u003e\u003c/p\u003e","description":"","filename":"SupplementaryInformation.docx","url":"https://assets-eu.researchsquare.com/files/rs-5909229/v1/200442f46725d242326ec41a.docx"}],"financialInterests":"There is \u003cb\u003eNO\u003c/b\u003e Competing Interest.","formattedTitle":"Valley Selectivity Manipulation via Interfacial Magnon-Exciton Interactions in TMD/CrSBr Antiferromagnetic van der Waals Heterostructures","fulltext":[{"header":"Introduction","content":"\u003cp\u003eTMDs exhibit a number of unique optical features, including strong excitonic effects and valley-contrasting exciton selection rules, making them a promising platform for quantum optics and nanophotonics\u003csup\u003e\u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e,\u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e\u003c/sup\u003e. VdW heterostructures, offering the advantage of freely constructing preferred 2D materials independently of their crystal structure, provide new avenues for achieving novel physical properties at their interfaces\u003csup\u003e\u003cspan citationid=\"CR3\" class=\"CitationRef\"\u003e3\u003c/span\u003e,\u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e4\u003c/span\u003e\u003c/sup\u003e. Heterostructures that integrate ML TMDs with 2D magnetic materials are anticipated to effectively manipulate the valley properties of ML TMDs via magnetic proximity effects (MPE)\u003csup\u003e\u003cspan additionalcitationids=\"CR6\" citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e\u003c/sup\u003e. Recent reports have demonstrated spontaneous valley splitting and enhanced VP in heterostructures such as MoSe\u003csub\u003e2\u003c/sub\u003e/CrBr\u003csub\u003e3\u003c/sub\u003e\u003csup\u003e8,9\u003c/sup\u003e, WSe\u003csub\u003e2\u003c/sub\u003e/CrI\u003csub\u003e3\u003c/sub\u003e\u003csup\u003e10\u003c/sup\u003e, WSe\u003csub\u003e2\u003c/sub\u003e/EuS\u003csup\u003e11\u003c/sup\u003e, MoSe\u003csub\u003e2\u003c/sub\u003e/Cr\u003csub\u003e2\u003c/sub\u003eGe\u003csub\u003e2\u003c/sub\u003eTe\u003csub\u003e6\u003c/sub\u003e\u003csup\u003e12\u003c/sup\u003e, WSe\u003csub\u003e2\u003c/sub\u003e/YIG\u003csup\u003e13\u003c/sup\u003e. However, previous studies have primarily focused on the vdW heterointerfaces consisting of the ferromagnetic layers, and the impact of antiferromagnets (AFMs) on the TMD valley properties in AFM/TMD vdW heterostructures remains elusive.\u003c/p\u003e \u003cp\u003eAFMs are magnetically ordered, yet with zero net magnetization, which makes them less susceptible to external field perturbation. More importantly, AFMs have high-frequency spin dynamics up to the terahertz (THz) range\u003csup\u003e\u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e\u003c/sup\u003e, which are generally two or three orders of magnitude higher than ferromagnets, along with long-lived coherent magnons\u003csup\u003e\u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e15\u003c/span\u003e\u003c/sup\u003e, leading to the prominent magnon effect\u003csup\u003e\u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e\u003c/sup\u003e. The hybridization of magnons with other quasiparticles provides potential avenues for the investigation and manipulation of other quasiparticles in TMD/AFM vdW heterostructures\u003csup\u003e\u003cspan additionalcitationids=\"CR18 CR19\" citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e\u003c/sup\u003e. One example is the IMEI, which have been demonstrated in the heterostructures formed by ML TMDs and N\u0026eacute;el-type AFMs\u003csup\u003e\u003cspan additionalcitationids=\"CR22 CR23\" citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e\u003c/sup\u003e. However, researches on IMEI in TMD/AFM vdW heterostructures are still in its infancy, with studies have primarily revealed the spectral signature and offering limited attention to the process involved in IMEI. In addition, investigations of IMEI remain confined to the vdW heterostructures integrated with TMDs and N\u0026eacute;el-type AFMs, which are expected to extend to other types of AFMs, such as the A-type AFM CrSBr\u003csup\u003e\u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e,\u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e\u003c/sup\u003e, recently reported to possess strong magnon effect\u003csup\u003e\u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e27\u003c/span\u003e,\u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e28\u003c/span\u003e\u003c/sup\u003e, enabling a more comprehensive understanding of IMEI involving various magnetic orderings. Furthermore, magnons hold magnetic dipole moments, which enable them directly couple to spin-based qubits through magnetic dipolar coupling\u003csup\u003e\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e\u003c/sup\u003e. This feature of magnons provides a promising way to manipulate the valley selection properties of TMD via heterointerface exciton-magnon coupling, which, however, remains elusive.\u003c/p\u003e \u003cp\u003eIn this work, we choose the A-type AFM CrSBr to vertically stack with ML MoSe\u003csub\u003e2\u003c/sub\u003e. The CrSBr crystal is composed of layers with rectangular unit cells in the a-b plane, and stacked along the c axis to produce an orthorhombic structure\u003csup\u003e\u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e\u003c/sup\u003e (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ea). Spins within each layer are ferromagnetically align along the crystal b axis, while the interlayer coupling is antiferromagnetic. The in-plane magnetization of CrSBr is misaligned with the out-of-plane spin texture of K (-K) valleys in ML MoSe\u003csub\u003e2\u003c/sub\u003e, which suppresses the impact of spin-dependent charge transfer in MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr heterostructures, and facilitates the investigation of IMEI and their impact on valley selectivity of ML MoSe\u003csub\u003e2\u003c/sub\u003e. In MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr heterostructures, we observed a blueshift of MoSe\u003csub\u003e2\u003c/sub\u003e excitonic states (excitons and trions) in the photoluminescence (PL) spectra below the N\u0026eacute;el temperature (\u003cem\u003eT\u003c/em\u003e\u003csub\u003eN\u003c/sub\u003e ~ 132 K)\u003csup\u003e\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e\u003c/sup\u003e of CrSBr, along with the emergency of a magnon-exciton complex on the low-energy side below 80 K. These phenomena cannot be explained by the magnetic exchange fields (MEF) as observed in ferromagnetic vdW interfaces. Instead, they indicate the existence of IMEI. Based on the exciton g-factors in the ML TMDs and heterostructures, and the comparison of exciton energy shift with magnon energy, we suggest two mechanisms of IMEI: MES and MADER, which result in the blueshift of excitonic states and the formation of magnon-exciton complexes, respectively. We found that MES remarkably enhances the complete quenched zero-field VP of the excitonic states in MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr, regardless of left-handed (\u003cem\u003eσ\u003c/em\u003e⁻) or right-handed (\u003cem\u003eσ\u003c/em\u003e\u003csup\u003e+\u003c/sup\u003e) circular polarized excitations. The valley-contrasting circular dichroism of magnon-exciton complexes can be increased by switching the spin orientation of CrSBr from in-plane to out-of-plane. Our work sheds light on the process of heterointerface exciton-magnon interactions and reveals their effective impacts on valley manipulation of ML TMD via TMD/AFM heterostructure stacking, paving the way for a novel approach to manipulating quantum information in non-magnetic semiconductors.\u003c/p\u003e"},{"header":"Results","content":"\u003cdiv id=\"Sec3\" class=\"Section2\"\u003e\n \u003ch2\u003eSpectral characteristics of MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr\u003c/h2\u003e\n \u003cp\u003eML MoSe\u003csub\u003e2\u003c/sub\u003e and CrSBr flake were obtained by mechanical exfoliation, and the heterostructure was assembled using dry-transfer technique, followed by high-vacuum annealing at 200\u0026deg;C to improve interface contact (see Methods for detailed fabrication information). Figure \u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003eb shows the predicted type-III band alignment of the heterostructure\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e25\u003c/span\u003e,\u003cspan class=\"CitationRef\"\u003e31\u003c/span\u003e\u0026ndash;\u003cspan class=\"CitationRef\"\u003e33\u003c/span\u003e\u003c/sup\u003e, where electrons in the valence band of MoSe\u003csub\u003e2\u003c/sub\u003e transfer to the conduction band of CrSBr upon contact. The efficient charge transfer results in p-doping of the MoSe\u003csub\u003e2\u003c/sub\u003e layer and a significant reduction in PL intensity\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e25\u003c/span\u003e,\u003cspan class=\"CitationRef\"\u003e26\u003c/span\u003e\u003c/sup\u003e (see Supplementary Note 2). Under laser illumination, discrete band bending at the heterojunction prevents photogenerated carriers from transferring between the two materials, with electrons (holes) in MoSe\u003csub\u003e2\u003c/sub\u003e (or CrSBr) dragged out of the junction region back into their respective layers\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e34\u003c/span\u003e\u003c/sup\u003e. The normalized PL spectra of MoSe\u003csub\u003e2\u003c/sub\u003e/SiO\u003csub\u003e2\u003c/sub\u003e and the MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr heterostructure at low temperatures are shown in Fig. \u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003ec. Unless otherwise specified, all measurements were conducted at 15 K using continuous-wave excitation at 715 nm. Exciton (X) and trion (T) emission in MoSe\u003csub\u003e2\u003c/sub\u003e/SiO\u003csub\u003e2\u003c/sub\u003e are assigned at1.655 eV and 1.627 eV, respectively. In MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr, the peaks X\u003csup\u003e*\u003c/sup\u003e and T\u003csup\u003e*\u003c/sup\u003e exhibit significant blueshifts of ~\u0026thinsp;16 meV and ~\u0026thinsp;14 meV in contrast to the peaks X and T, respectively. Furthermore, a new peak (M\u003csup\u003e*\u003c/sup\u003e) emerges on the low-energy side of the trion (T\u003csup\u003e*\u003c/sup\u003e) in MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr, located at 1.620 eV. The energy differences between M\u003csup\u003e*\u003c/sup\u003e and T\u003csup\u003e*\u003c/sup\u003e and between M\u003csup\u003e*\u003c/sup\u003e and X\u003csup\u003e*\u003c/sup\u003e are ~\u0026thinsp;21 meV and ~\u0026thinsp;51 meV, respectively.\u003c/p\u003e\n \u003cp\u003eTo reveal the origin of the three peaks in MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr heterostructure, we conducted the power dependent PL measurement. The PL intensities of three peaks show linear dependence on the excitation power and do not saturate even at high excitation power (Fig. \u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003ed), indicating their exciton and trion characteristics and excludes the possibilities of biexcitons, localized excitons, or moir\u0026eacute; excitons\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e24\u003c/span\u003e\u003c/sup\u003e. To further assign the three peaks\u0026rsquo; origination, we consider the effects that may arise from the contact between ML MoSe\u003csub\u003e2\u003c/sub\u003e and CrSBr, as well as the subsequent laser irradiation, including variation of the dielectric environment, interlayer charge transfer, MEF induced by the MPE of CrSBr, and interlayer particle interactions. The effect of dielectric environment cannot result in such substantial temperature-dependent blueshift (see below). Interlayer charge transfer can also be excluded to cause the emergence of the three peaks, since no energy shift occurs in this mechanism\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e35\u003c/span\u003e\u0026ndash;\u003cspan class=\"CitationRef\"\u003e38\u003c/span\u003e\u003c/sup\u003e. Although an in-plane MEF may lead to a new emission peak via brightening dark excitons, the splitting energy between bright excitons and brightened dark excitons is only 1\u0026thinsp;~\u0026thinsp;2 meV\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e39\u003c/span\u003e,\u003cspan class=\"CitationRef\"\u003e40\u003c/span\u003e\u003c/sup\u003e, which contradicts our experimental results. Hence, MEF is not the source that contributes to the occurrence of X\u003csup\u003e*\u003c/sup\u003e, T\u003csup\u003e*\u003c/sup\u003e and M\u003csup\u003e*\u003c/sup\u003e. Detailed discussions can be found in the Supplementary Note 3. Therefore, we suggest that the energy blueshift of X\u003csup\u003e*\u003c/sup\u003e and T\u003csup\u003e*\u003c/sup\u003e, as well as the emergence of M\u003csup\u003e*\u003c/sup\u003e, origin from the interlayer particle interactions between ML MoSe\u003csub\u003e2\u003c/sub\u003e and CrSBr, specifically, the interaction between the excitons in MoSe\u003csub\u003e2\u003c/sub\u003e and the magnons in CrSBr.\u003c/p\u003e\n\u003c/div\u003e\n\u003ch3\u003eInterfacial magnon-exciton interactions in MoSe/CrSBr\u003c/h3\u003e\n\u003cp\u003eTo confirm the IMEI in the MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr heterostructure, we measured the temperature dependence of PL spectra for MoSe\u003csub\u003e2\u003c/sub\u003e/SiO\u003csub\u003e2\u003c/sub\u003e and MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr (Fig.\u0026nbsp;2a). Exciton peak energies are extracted and plotted as a function of temperature, as shown in Fig.\u0026nbsp;2b. We observed that the peak energy of X\u003csup\u003e*\u003c/sup\u003e in the heterostructure exhibits a significant blueshift compared to the exciton X in ML MoSe\u003csub\u003e2\u003c/sub\u003e. Furthermore, this blueshift energy features not a monotonic decrease with temperature, but shows an increase trend below ~\u0026thinsp;70 K, then decreases monotonically, and finally achieves a constant (~\u0026thinsp;7.5 meV) above \u003cem\u003eT\u003c/em\u003e\u003csub\u003eN\u003c/sub\u003e of CrSBr. This constant energy difference is attributed to the variation of dielectric environment\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e21\u003c/span\u003e\u0026ndash;\u003cspan class=\"CitationRef\"\u003e24\u003c/span\u003e\u003c/sup\u003e. A similar non-monotonic temperature dependence of the blue-shifted energy was also observed in WSe\u003csub\u003e2\u003c/sub\u003e/CrSBr (see Supplementary Note 6), with the same transition temperature of ~\u0026thinsp;70 K. The correlation between the energy blueshift of the exciton peak and the antiferromagnetic ordering in CrSBr indicates the existence of IMEI in the MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr below \u003cem\u003eT\u003c/em\u003e\u003csub\u003eN\u003c/sub\u003e.\u003c/p\u003e\n\u003cp\u003eFigure 2c shows the temperature dependence of the integrated PL intensity of M\u003csup\u003e*\u003c/sup\u003e. It is evident that the intensity of M\u003csup\u003e*\u003c/sup\u003e rapidly decreases as the temperature increases and vanishes around 80 K. This process can be described by the Arrhenius Eq. 2\u003csup\u003e4,41\u003c/sup\u003e:\u003c/p\u003e\n\u003cdiv id=\"Equ1\" class=\"Equation\"\u003e\n \u003cdiv class=\"mathdisplay\" id=\"FileID_Equ1\" name=\"EquationSource\"\u003e$$\\:I\\left(T\\right)=\\frac{{I}_{0}}{1+A\\bullet\\:\\text{exp}\\left(-\\frac{{E}_{\\text{a}}}{{k}_{\\text{B}}T}\\right)},$$\u003c/div\u003e\n \u003cdiv class=\"EquationNumber\"\u003e1\u003c/div\u003e\n\u003c/div\u003e\n\u003cp\u003ewhere, \u003cem\u003eI\u003c/em\u003e(\u003cem\u003eT\u003c/em\u003e) represents the integrated intensity at temperature \u003cem\u003eT\u003c/em\u003e, \u003cem\u003eI\u003c/em\u003e\u003csub\u003e0\u003c/sub\u003e is the integrated intensity at 0 K, \u003cem\u003eA\u003c/em\u003e is a constant related to the radiative and non-radiative decay rates, \u003cem\u003eE\u003c/em\u003e\u003csub\u003ea\u003c/sub\u003e denotes the activation energy, and \u003cem\u003ek\u003c/em\u003e\u003csub\u003eB\u003c/sub\u003e is the Boltzmann constant. By fitting the data, the activation energy of M\u003csup\u003e*\u003c/sup\u003e was determined to be ~\u0026thinsp;42 meV, which is close to the energy difference between M\u003csup\u003e*\u003c/sup\u003e and X (~\u0026thinsp;35 meV), considering the blueshift of ~\u0026thinsp;7.5 meV induced by the variation of dielectric environment. More importantly, this energy difference (~\u0026thinsp;42.5 meV) matches the energy\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e42\u003c/span\u003e\u0026ndash;\u003cspan class=\"CitationRef\"\u003e44\u003c/span\u003e\u003c/sup\u003e (~\u0026thinsp;45 meV) of a high-energy magnon near the \u0026Gamma; point of the CrSBr Brillouin zone. Since energy splitting of the bright and dark excitons in MoSe\u003csub\u003e2\u003c/sub\u003e is tiny (~ -1.5 meV), it indicates that the emission of M\u003csup\u003e*\u003c/sup\u003e results from the interaction between bright/dark excitons in MoSe\u003csub\u003e2\u003c/sub\u003e and magnons in CrSBr.\u003c/p\u003e\n\u003cp\u003eWe suggest that X\u003csup\u003e*\u003c/sup\u003e and T\u003csup\u003e*\u003c/sup\u003e in MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr as manifestations of MES, while M\u003csup\u003e*\u003c/sup\u003e originates from MADER, which we identify as a complex of magnons and dark excitons. MADER can be analogous to the interaction between phonons and excitons\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e38\u003c/span\u003e,\u003cspan class=\"CitationRef\"\u003e45\u003c/span\u003e,\u003cspan class=\"CitationRef\"\u003e46\u003c/span\u003e\u003c/sup\u003e (this possibility can be excluded due to the mismatch between phonon energy\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e47\u003c/span\u003e\u003c/sup\u003e and spectral energy shift). Under the incidence of photons carrying zero momentum, magnons (~\u0026thinsp;45 meV) near the \u0026Gamma; point in the Brillouin zone are typically excited\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e14\u003c/span\u003e\u003c/sup\u003e. From momentum and angular momentum conservation, \u0026Gamma;-point magnons can induce the intravalley spin-flip relaxation of electrons, enabling dark excitons to undergo radiative recombination by emitting magnons (Fig.\u0026nbsp;2d). This process reduces the dark exciton emission energy by one magnon energy and causes the spectral broadening due to the dispersion of magnons\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e45\u003c/span\u003e\u003c/sup\u003e. These assertions are supported by our results that M\u003csup\u003e*\u003c/sup\u003e exhibits a relatively broad linewidth (~\u0026thinsp;41 meV) and a \u003cem\u003eg\u003c/em\u003e-factor (-8.75, see Fig. \u003cspan class=\"InternalRef\"\u003e4\u003c/span\u003ea, with detailed discussion in the Supplementary Note 3) similar to that of intravalley dark exciton recombination\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e37\u003c/span\u003e,\u003cspan class=\"CitationRef\"\u003e38\u003c/span\u003e,\u003cspan class=\"CitationRef\"\u003e48\u003c/span\u003e\u003c/sup\u003e. Similar results were also observed in the WSe\u003csub\u003e2\u003c/sub\u003e/CrSBr heterostructure (see Supplementary Note 4). Regarding the assignment of X\u003csup\u003e*\u003c/sup\u003e and T\u003csup\u003e*\u003c/sup\u003e in the MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr heterostructure, their energy shift (~\u0026thinsp;8.5 meV) is smaller than the energy of a single magnon, and their \u003cem\u003eg\u003c/em\u003e-factors reflect the characteristics of excitons and trions (-3.04 and \u0026minus;\u0026thinsp;4.12, respectively, see Fig. \u003cspan class=\"InternalRef\"\u003e4\u003c/span\u003ea). Thus, we attribute them to the exciton states in MoSe\u003csub\u003e2\u003c/sub\u003e after elastic or inelastic scattering with the magnon states in CrSBr. In this process (Fig. 2e), the energy and momentum between excitons and magnons are redistributed\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e49\u003c/span\u003e\u0026ndash;\u003cspan class=\"CitationRef\"\u003e52\u003c/span\u003e\u003c/sup\u003e, leading to the energy shift of X and T, which correspond to the energy variation of magnons. We further demonstrate that the interlayer exchange coupling, as a short-range interaction, is the requisite to the formation of IMEI in MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr heterostructures by performing the same experiments in unannealed heterostructures and observing no EMC or MADER.\u003c/p\u003e\n\u003ch3\u003eValley polarization enhanced by MES\u003c/h3\u003e\n\u003cp\u003eTo investigate the effect of magnons on valley properties of MoSe\u003csub\u003e2\u003c/sub\u003e, we conducted the polarized PL spectra of heterostructure and compared them with ML MoSe\u003csub\u003e2\u003c/sub\u003e, as shown in Fig. \u003cspan class=\"InternalRef\"\u003e3\u003c/span\u003ea. For easier identification, the PL intensity of MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr has been normalized to the co-polarized intensity of MoSe\u003csub\u003e2\u003c/sub\u003e/SiO\u003csub\u003e2\u003c/sub\u003e. The co-polarized and cross-polarized trion peaks of heterostructure exhibit an intensity discrepancy, which can be quantitatively evaluated using the VP. For \u003cem\u003e\u0026sigma;\u003c/em\u003e\u003csup\u003e+\u003c/sup\u003e excitation, the VP can be estimated by the formula: \u003cem\u003eP\u003c/em\u003e\u003csub\u003ec\u003c/sub\u003e (\u003cem\u003e\u0026sigma;\u003c/em\u003e\u003csup\u003e+\u003c/sup\u003e) = (\u003cem\u003eI\u003c/em\u003e\u003csub\u003e\u003cem\u003e\u0026sigma;\u003c/em\u003e⁺\u003cem\u003e\u0026sigma;\u003c/em\u003e⁺\u003c/sub\u003e - \u003cem\u003eI\u003c/em\u003e\u003csub\u003e\u003cem\u003e\u0026sigma;\u003c/em\u003e⁺\u003cem\u003e\u0026sigma;\u003c/em\u003e⁻\u003c/sub\u003e)/(\u003cem\u003eI\u003c/em\u003e\u003csub\u003e\u003cem\u003e\u0026sigma;\u003c/em\u003e⁺\u003cem\u003e\u0026sigma;\u003c/em\u003e⁺\u003c/sub\u003e + \u003cem\u003eI\u003c/em\u003e\u003csub\u003e\u003cem\u003e\u0026sigma;\u003c/em\u003e⁺\u003cem\u003e\u0026sigma;\u003c/em\u003e⁻\u003c/sub\u003e), where \u003cem\u003eI\u003c/em\u003e\u003csub\u003e\u003cem\u003e\u0026sigma;\u003c/em\u003e⁺\u003cem\u003e\u0026sigma;\u003c/em\u003e⁺\u003c/sub\u003e and \u003cem\u003eI\u003c/em\u003e\u003csub\u003e\u003cem\u003e\u0026sigma;\u003c/em\u003e⁺\u003cem\u003e\u0026sigma;\u003c/em\u003e⁻\u003c/sub\u003e are the PL intensities under \u003cem\u003e\u0026sigma;\u003c/em\u003e\u003csup\u003e+\u003c/sup\u003e excitation with co-polarized (\u003cem\u003e\u0026sigma;\u003c/em\u003e\u003csup\u003e+\u003c/sup\u003e excitation, \u003cem\u003e\u0026sigma;\u003c/em\u003e\u003csup\u003e+\u003c/sup\u003e detection) and cross-polarized (\u003cem\u003e\u0026sigma;\u003c/em\u003e\u003csup\u003e+\u003c/sup\u003e excitation, \u003cem\u003e\u0026sigma;\u003c/em\u003e⁻ detection) configurations, respectively. For both \u003cem\u003e\u0026sigma;\u003c/em\u003e\u003csup\u003e+\u003c/sup\u003e and \u003cem\u003e\u0026sigma;\u003c/em\u003e⁻ excitation, we obtained\u0026thinsp;~\u0026thinsp;8% and 0% trion VP in MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr and MoSe\u003csub\u003e2\u003c/sub\u003e/SiO\u003csub\u003e2\u003c/sub\u003e, respectively (Fig. \u003cspan class=\"InternalRef\"\u003e3\u003c/span\u003eb at B\u0026thinsp;=\u0026thinsp;0 T). This differs from VP enhancement caused by MEF or the application of an out-of-plane magnetic field, which enhances the polarization for one helicity of excitation while suppressing it for the opposite helicity. More importantly, all PL peaks in MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr exhibited enhanced VP at 0 T (Fig. \u003cspan class=\"InternalRef\"\u003e3\u003c/span\u003ea), indicating a breakthrough of zero VP in ML MoSe\u003csub\u003e2\u003c/sub\u003e, while it is challenging to increase VP by conventional methods (e.g., charge transfer\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e9\u003c/span\u003e\u003c/sup\u003e, doping\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e53\u003c/span\u003e\u003c/sup\u003e, and MEF\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e12\u003c/span\u003e\u003c/sup\u003e) due to the fast valley depolarization rate caused by electron\u0026ndash;hole exchange interaction.\u003c/p\u003e\n\u003cp\u003eTo understand the zero-field VP enhancement in the heterostructure, we measured VP dependence on an out-of-plane magnetic field (Fig. \u003cspan class=\"InternalRef\"\u003e3\u003c/span\u003eb). It shows obviously linear variations of VP with the magnetic field in MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr, with rates of ~\u0026thinsp;2.4%/T and ~ -2.2%/T for \u003cem\u003e\u0026sigma;\u003c/em\u003e\u003csup\u003e\u0026plusmn;\u003c/sup\u003e excitation, respectively. This linear dependence indicates that the zero-field VP enhancement is not determined by the spin orientation of CrSBr. Otherwise, the VP would display a larger tunability below the saturation field \u003cem\u003eH\u003c/em\u003e\u003csub\u003es\u003c/sub\u003e (\u0026thinsp;~\u0026thinsp;\u0026plusmn;\u0026thinsp;2 T)\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e54\u003c/span\u003e\u003c/sup\u003e in contrast to above \u003cem\u003eH\u003c/em\u003e\u003csub\u003es\u003c/sub\u003e, due to the combined effect of the external magnetic field and the spin-dependent interlayer charge transfer or effective magnetic field induced by the spin reorientation of CrSBr\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e9\u003c/span\u003e,\u003cspan class=\"CitationRef\"\u003e10\u003c/span\u003e\u003c/sup\u003e. Besides, the intervalley charge transfer can be also excluded as the origin of the VP enhancement, as it would lead to an increase in trion VP and a decrease in exciton VP. This contradicts our results, which show an enhancement of exciton VP by ~\u0026thinsp;16% in the heterostructure (see Supplementary Note 5 and 6).\u003c/p\u003e\n\u003cp\u003eTo find out the origin of the zero-field VP enhancement in MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr, we conducted the temperature dependence of the VP in the heterostructure. As shown in Fig. \u003cspan class=\"InternalRef\"\u003e3\u003c/span\u003ec, the VP enhancement of trions in MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr decreases with temperature increasing and disappears around 130 K, which is close to the \u003cem\u003eT\u003c/em\u003e\u003csub\u003eN\u003c/sub\u003e of CrSBr, indicating the association between the VP enhancement and the magnetism of CrSBr. We suggest that the zero-field enhancement of VP results from the MES of MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr heterostructure. This interaction weakens the electron-hole exchange interaction, resulting in the VP increasing. Specifically, the electron-hole exchange interaction in ML TMDs acts as an effective in-plane magnetic field \u003cem\u003eB\u003c/em\u003e\u003csub\u003eeff\u003c/sub\u003e, which depends on the center-of-mass momentum k of excitons and drives the precession of valley pseudospin\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e55\u003c/span\u003e\u003c/sup\u003e, as illustrated in Fig. \u003cspan class=\"InternalRef\"\u003e3\u003c/span\u003ed. Whenever a scattering event occurs, the direction of the exciton\u0026apos;s center-of-mass momentum changes randomly, causing the \u003cem\u003eB\u003c/em\u003e\u003csub\u003eeff\u003c/sub\u003e direction changing as well\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e55\u003c/span\u003e\u003c/sup\u003e. Since spin precession occurs between two scattering events, more frequent scattering result in more frequent changes in the direction of \u003cem\u003eB\u003c/em\u003e\u003csub\u003eeff\u003c/sub\u003e. This reduces the mean free time of excitonic states, thereby decreasing the time-averaged \u003cem\u003eB\u003c/em\u003e\u003csub\u003eeff\u003c/sub\u003e experienced by excitonic states\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e55\u003c/span\u003e\u003c/sup\u003e, leading to the weakening of intervalley relaxation and an increase in VP of excitonic states. In our work, magnons in CrSBr carry a transient magnetization with the oscillating direction along the c-axis\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e15\u003c/span\u003e,\u003cspan class=\"CitationRef\"\u003e56\u003c/span\u003e,\u003cspan class=\"CitationRef\"\u003e57\u003c/span\u003e\u003c/sup\u003e. These magnons provide a THz-frequency oscillating magnetic field and interact with excitonic states in MoSe\u003csub\u003e2\u003c/sub\u003e. The oscillating magnetic field of the magnons, along with the MES, reduces the time-averaged \u003cem\u003eB\u003c/em\u003e\u003csub\u003eeff\u003c/sub\u003e by causing more frequent changes in \u003cem\u003eB\u003c/em\u003e\u003csub\u003eeff\u003c/sub\u003e, leading to a weakened electron-hole exchange interaction and an increase in VP of excitonic states.\u003c/p\u003e\n\u003ch3\u003eValley properties of magnon-exciton complex\u003c/h3\u003e\n\u003cp\u003eWe investigated the valley properties of M\u003csup\u003e*\u003c/sup\u003e and its magnetic response under an out-of-plane magnetic field \u003cem\u003eB\u003c/em\u003e. First, we extracted the \u003cem\u003eg\u003c/em\u003e-factor by measuring polarized PL spectra with \u003cem\u003eg\u003c/em\u003e\u0026thinsp;=\u0026thinsp;\u0026Delta;\u003cem\u003eE\u003c/em\u003e /\u003cem\u003e\u0026micro;\u003c/em\u003e\u003csub\u003eB\u003c/sub\u003e\u003cem\u003eB\u003c/em\u003e, where \u0026Delta;\u003cem\u003eE\u003c/em\u003e\u0026thinsp;=\u0026thinsp;\u003cem\u003eE\u003c/em\u003e\u003csub\u003e\u003cem\u003e\u0026sigma;\u003c/em\u003e⁺\u003cem\u003e\u0026sigma;\u003c/em\u003e⁺\u003c/sub\u003e - \u003cem\u003eE\u003c/em\u003e\u003csub\u003e\u003cem\u003e\u0026sigma;\u003c/em\u003e⁻\u003cem\u003e\u0026sigma;\u003c/em\u003e⁻\u003c/sub\u003e, and \u003cem\u003eE\u003c/em\u003e\u003csub\u003e\u003cem\u003e\u0026sigma;\u003c/em\u003e⁺\u003cem\u003e\u0026sigma;\u003c/em\u003e⁺(\u003cem\u003e\u0026sigma;\u003c/em\u003e⁻\u003cem\u003e\u0026sigma;\u003c/em\u003e⁻)\u003c/sub\u003e represents co-polarized PL peak energy under \u003cem\u003e\u0026sigma;\u003c/em\u003e\u003csup\u003e+\u003c/sup\u003e (\u003cem\u003e\u0026sigma;\u003c/em\u003e⁻) excitation, and \u003cem\u003e\u0026micro;\u003c/em\u003e\u003csub\u003eB\u003c/sub\u003e is the Bohr magneton, as shown in Fig. \u003cspan class=\"InternalRef\"\u003e4\u003c/span\u003ea. The \u003cem\u003eg\u003c/em\u003e-factor of M\u003csup\u003e*\u003c/sup\u003e is ~ -8.75, which is similar to the \u003cem\u003eg\u003c/em\u003e-factor of intravalley dark exciton recombination, supporting the assignment of M\u003csup\u003e*\u003c/sup\u003e as the magnon-assisted radiative recombination of dark excitons. The \u003cem\u003eg\u003c/em\u003e-factors of T\u003csup\u003e*\u003c/sup\u003e (~ -4.12) and X\u003csup\u003e*\u003c/sup\u003e(~ -3.04) keep the characteristics of trions and excitons.\u003c/p\u003e\n\u003cp\u003eThen, we focus on the dependence of the VP of M\u003csup\u003e*\u003c/sup\u003e on the external out-of-plane magnetic field. We observe an asymmetric V-shaped pattern (Fig. \u003cspan class=\"InternalRef\"\u003e4\u003c/span\u003eb), which is different from the linear dependence of T\u003csup\u003e*\u003c/sup\u003e and T in Fig. \u003cspan class=\"InternalRef\"\u003e3\u003c/span\u003eb. We suggest that this asymmetry originates from the combined effects of Zeeman effect and electron-hole exchange interactions. Although both Zeeman effect and exchange interactions influence the VP, they respond differently to the out-of-plane magnetic field. In absence of magnetic field, valley degeneracy is preserved. When a positive magnetic field is exerted, Zeeman effect causes the energy of the K (-K) valley downshift (upshift), leading to more carriers relaxing into K (-K) valley. Thus, Zeeman splitting enhances (reduces) the VP for \u003cem\u003e\u0026sigma;\u003c/em\u003e\u003csup\u003e+\u003c/sup\u003e excitation under positive (negative) magnetic fields, resulting in a linear dependence of VP with the magnetic field. In contrast, the electron-hole exchange interaction is weakened by an out-of-plane magnetic field in either direction due to the lifting of valley degeneracy\u003csup\u003e\u003cspan class=\"CitationRef\"\u003e58\u003c/span\u003e\u003c/sup\u003e, which suppresses intervalley relaxation. Stronger magnetic field results in greater suppression. Consequently, VP manifests a symmetric V-shaped dependence on the magnetic field under the electron-hole exchange interaction mechanism.\u003c/p\u003e\n\u003cp\u003eWe established a theoretical model of VP contributed by both the Zeeman effect and electron-hole exchange interaction, using a four-level system (details in the Supplementary Note 8). This model well fits the experimental results and allows for the separation of the contributions of two mechanisms to the VP, as shown in Fig. \u003cspan class=\"InternalRef\"\u003e4\u003c/span\u003ec. Based on the fitting parameters, the zero-field intervalley relaxation rate resulting from the electron-hole exchange interaction is ~\u0026thinsp;42.5 times larger than that caused by the Zeeman effect, revealing that the electron-hole exchange interaction dominates zero-field VP of M\u003csup\u003e*\u003c/sup\u003e. Under the framework of this model, we can interpret the linear dependence of VP on the magnetic field for T\u003csup\u003e*\u003c/sup\u003e and T in Fig. \u003cspan class=\"InternalRef\"\u003e3\u003c/span\u003eb as predominated by the mechanism of Zeeman effect.\u003c/p\u003e\n\u003cp\u003eFinally, we discuss the impact of CrSBr spin orientation on the valley properties of M\u003csup\u003e*\u003c/sup\u003e, which can be estimated by the valley contrasting circular dichroism (VCCD) between two valleys with \u003cem\u003e\u0026rho;\u003c/em\u003e = (\u003cem\u003eI\u003c/em\u003e\u003csub\u003e\u003cem\u003e\u0026sigma;\u003c/em\u003e⁺\u003cem\u003e\u0026sigma;\u003c/em\u003e⁺\u003c/sub\u003e - \u003cem\u003eI\u003c/em\u003e\u003csub\u003e\u003cem\u003e\u0026sigma;\u003c/em\u003e⁻\u003cem\u003e\u0026sigma;\u003c/em\u003e⁻\u003c/sub\u003e)/(\u003cem\u003eI\u003c/em\u003e\u003csub\u003e\u003cem\u003e\u0026sigma;\u003c/em\u003e⁺\u003cem\u003e\u0026sigma;\u003c/em\u003e⁺\u003c/sub\u003e + \u003cem\u003eI\u003c/em\u003e\u003csub\u003e\u003cem\u003e\u0026sigma;\u003c/em\u003e⁻\u003cem\u003e\u0026sigma;\u003c/em\u003e⁻\u003c/sub\u003e). Figure \u003cspan class=\"InternalRef\"\u003e4\u003c/span\u003ed shows the VCCD of T\u003csup\u003e*\u003c/sup\u003e, T, and M\u003csup\u003e*\u003c/sup\u003e dependence on the out-of-plane magnetic field. It can be observed that the VCCDs of T\u003csup\u003e*\u003c/sup\u003e and T show a linear variation with the magnetic field, with a slope of ~\u0026thinsp;2.4%/T. In contrast, VCCD of M\u003csup\u003e*\u003c/sup\u003e exhibits an S-shaped variation, with a sharp changing rate (~\u0026thinsp;2.2%/T) within \u003cem\u003eH\u003c/em\u003e\u003csub\u003es\u003c/sub\u003e of CrSBr and a slower rate (~\u0026thinsp;0.1%/T) beyond \u003cem\u003eH\u003c/em\u003e\u003csub\u003es\u003c/sub\u003e. This S-shaped behavior suggests that, the VCCD of M\u003csup\u003e*\u003c/sup\u003e is also modulated by the spin orientation of CrSBr in addition to the direct effect of the magnetic field.\u003c/p\u003e\n\u003cp\u003eIn the absence of magnetic field, the energy band preserve spin degenerate in CrSBr due to the anti-parallel spin orientation of adjacent layers along the b-axis, resulting in an equal population of magnons with the angular momentum of -1 and +\u0026thinsp;1. Thus, the impact of magnons in CrSBr on the VCCD is balanced, as shown in Fig. \u003cspan class=\"InternalRef\"\u003e4\u003c/span\u003ee. When we applied a positive (negative) out-of-plane magnetic field lower than \u003cem\u003eH\u003c/em\u003e\u003csub\u003es\u003c/sub\u003e of CrSBr, the spin orientation gradually canted towards +\u0026thinsp;c (-c) axis as the magnetic field increase, breaking the spin degeneracy, and the population of magnons with angular momentum of -1 (+\u0026thinsp;1) exceeded that with angular momentum of +\u0026thinsp;1 (-1), as shown in Fig. \u003cspan class=\"InternalRef\"\u003e4\u003c/span\u003ef. Since the M\u003csup\u003e*\u003c/sup\u003e emission with photon angular momentum of +\u0026thinsp;1 (-1) occurs via magnons with \u0026minus;\u0026thinsp;1 (+\u0026thinsp;1) angular momentum coupling with dark excitons in K (-K) valley, the M\u003csup\u003e*\u003c/sup\u003e emission in K (-K) valley enhanced, resulting in a rapid increase of VCCD with the magnetic field. When \u003cem\u003eB\u003c/em\u003e\u0026thinsp;=\u0026thinsp;\u003cem\u003eH\u003c/em\u003e\u003csub\u003es\u003c/sub\u003e (\u003cem\u003eB\u003c/em\u003e = -\u003cem\u003eH\u003c/em\u003e\u003csub\u003es\u003c/sub\u003e), magnetization along the +\u0026thinsp;c (-c) axis reaches saturation. There are only magnons with angular momentum of -1 (+\u0026thinsp;1). Thus, the contribution of the spin orientation to the VCCD would no longer increases as the magnetic field increases, leading to a slower changing rate of VCCD with the magnetic field. We notice a slight tunability of VCCD when the magnetic field exceeds \u003cem\u003eH\u003c/em\u003e\u003csub\u003es\u003c/sub\u003e, that is, when the slope of VCCD is solely influenced by the magnetic field. This suggests that the intervalley scattering of M\u003csup\u003e*\u003c/sup\u003e is less affected by Zeeman effect, which is in line with the above discussion on the VP of M\u003csup\u003e*\u003c/sup\u003e. The S-shaped variation of VCCD with the magnetic field cannot attributed to the MEF or spin-dependent interlayer charge transfer induced by the spin orientation of CrSBr, as no additional energy splitting within \u003cem\u003eH\u003c/em\u003e\u003csub\u003es\u003c/sub\u003e was observed in Fig. \u003cspan class=\"InternalRef\"\u003e4\u003c/span\u003ea, and no S-shaped VCCD was observed in T\u003csup\u003e*\u003c/sup\u003e.\u003c/p\u003e\n\u003cp\u003eWe note that our finding can be well reproduced in WSe\u003csub\u003e2\u003c/sub\u003e/CrSBr heterostructure system (see Supplementary Note 7), demonstrating the IMEI widely exist in TMD/CrSBr heterostructures.\u003c/p\u003e\n\u003cp\u003eIn summary, we have demonstrated the existence of two types of IMEI, MES and MADER, in TMD/CrSBr systems and thoroughly investigated their impacts on the excitonic states and valley properties of ML TMDs. MES induces a blueshift in the excitonic states of ML TMDs in the TMD/CrSBr heterostructure below the \u003cem\u003eT\u003c/em\u003e\u003csub\u003eN\u003c/sub\u003e of CrSBr and enhances the VP of all emission peaks under both \u003cem\u003e\u0026sigma;\u003c/em\u003e⁺ and \u003cem\u003e\u0026sigma;\u003c/em\u003e\u003csup\u003e+\u003c/sup\u003e excitations. The latter can be attributed to the suppression of intervalley electron-hole exchange interactions by magnons. More importantly, MES offers an effective and field-free method to enhance a completely quenched VP of ML MoSe\u003csub\u003e2\u003c/sub\u003e, which is challenging to achieve through other methods such as doping, MEF, or charge transfer. On the other hand, MADER leads to the formation of dark exciton-magnon complexes, which can be observed in PL spectra. The complexes exhibit \u003cem\u003eg\u003c/em\u003e-factors similar to that of their original dark excitons, and display asymmetric V-shaped VP and S-shaped VCCD variations with magnetic field, which respectively indicate a valley depolarization mechanism dominated by intervalley electron-hole exchange interactions and valley selectivity enhanced by magnons. Our findings provide a new platform for manipulating the excitonic and valley properties of non-magnetic semiconductors, highlighting the critical role of hybridized quasiparticles in TMD/AFM heterostructures and opening up exciting opportunities in the fields of quantum information science, opto-spintronics and valleytronics.\u003c/p\u003e"},{"header":"Methods","content":"\u003cp\u003e \u003cb\u003eSample preparation.\u003c/b\u003e A few layer CrSBr flake is mechanically exfoliated from bulk CrSBr crystals by scotch tape (3M Scotch), and then are transferred on a clean SiO\u003csub\u003e2\u003c/sub\u003e/Si substrate. The thickness of SiO\u003csub\u003e2\u003c/sub\u003e is about 285 nm. The CrSBr flake was then thermally annealed at 250\u0026deg;C for 2h in a high vacuum (~\u0026thinsp;10\u003csup\u003e\u0026minus;\u0026thinsp;6\u003c/sup\u003e mbar) atmosphere. ML MoSe\u003csub\u003e2\u003c/sub\u003e exfoliated from bulk crystals (HQ Graphene) is transferred on the top of CrSBr flake using the dry-transfer technique and polydimethylsiloxane (PDMS) substrate. Next, the device is thermally annealed at 200\u0026deg;C for 2h in a high vacuum (~\u0026thinsp;10\u003csup\u003e\u0026minus;\u0026thinsp;6\u003c/sup\u003e mbar) atmosphere to improve the interface contact.\u003c/p\u003e \u003cp\u003e \u003cb\u003eMagneto-optical spectroscopy.\u003c/b\u003e PL spectroscopy were performed by a lab-built confocal microscope system. The sample was mounted in a close-cycle cryostat (Opticool, Quantum Design) with a piezo-units (attocube system, ANPx101, ANPx101, and ANPz102). The temperature was set to \u003cem\u003eT\u003c/em\u003e\u0026thinsp;=\u0026thinsp;15 K, and the magnetic field was up to \u0026plusmn;\u0026thinsp;7 T. We focused the laser beam onto the sample using an objective lens (Nikon, 50\u0026times;, N.A. = 0.6), with a spot diameter of 1 \u0026micro;m. PL spectra with 715 nm excitation were obtained with a Ti:sapphire laser (TiF-100ST-F10-AU, Avesta) in continuous wave mode, and rotating 750 nm short-pass (FESH0750, Thorlabs) and long-pass (FELH0750, Thorlabs) filters were used to remove the laser line. For PL spectra with 670 nm excitation, a picosecond laser diode (PLDD-20M, ALPHALAS GmbH) was used in continuous wave mode, and 700 nm short-pass (FESH0700, Thorlabs) and long-pass (FELH0700, Thorlabs) filters were used to remove the laser line. Both excitation and detection were circularly polarized, with the polarization of the excitation light initialized by a vertically oriented polarizer and controlled by a half-wave plate (AHWP05M-600, Thorlabs) and a quarter-wave plate (AQWP05M-600, Thorlabs). The optical system in the collection path was similar to the excitation optical system. The waveplates were mounted on a motorized rotary stage to automate the experiment. The signal was analyzed using a spectrometer (Shamrock 500i, Oxford Instruments) with a CCD camera (iDus CCD 420).\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e\u003cstrong\u003eAuthor contributions\u003c/strong\u003e\u003cbr\u003e\u0026nbsp;H.L. and Z.S. synthesized CrSBr crystals. X.Z., H.M., and C.J. designed the research. X.Z. performed sample preparation with the assistance of Y.Z., R.M., and Z.Y. X.Z. performed optical measurements with the assistance of X.D., R.Z., and Y.T. X.Z. performed data processing with the assistance of R.B. and C.J. X.Z., H.M., and C.J. analyzed and discussed the data. X.Z., H.M., and C.J. wrote the paper. All authors commented on the manuscript.\u003c/p\u003e\n\u003cp\u003eCompeting interests\u003c/p\u003e\n\u003cp\u003eThe authors declare no competing interest.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAcknowledgements\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThis work was supported by the National Natural Science Foundation of China (62374095, 61974075, and 61704121), the National Key Technologies R\u0026amp;D Program of China (2022YFB2803900), the Natural Science Foundation of Tianjin City (19JCQNJC00700 and 22JCZDJC00460), the Scientific Research Project of Tianjin Municipal Education Commission (2019KJ028), and the Fundamental Research Funds for the Central Universities of Nankai University (22JCZDJC00460). C.J. acknowledges the Tianjin Key Laboratory of Efficient Utilization of Solar Energy and the Engineering Research Center of Thin Film Optoelectronics Technology, Ministry of Education of China.\u003c/p\u003e\n\u003cp\u003eZ.S. was supported by ERC-CZ program (project LL2101) from Ministry of Education Youth and Sports (MEYS) and by the project Advanced Functional Nanorobots (reg. No. CZ.02.1.01/0.0/0.0/15_003/0000444 financed by the EFRR).\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\n\u003cli\u003eRegan, E. C.\u003cem\u003e et al.\u003c/em\u003e Emerging exciton physics in transition metal dichalcogenide heterobilayers. \u003cem\u003eNature Reviews Materials\u003c/em\u003e \u003cstrong\u003e7\u003c/strong\u003e, 778-795 (2022).\u003c/li\u003e\n\u003cli\u003eLi, W., Lu, X., Wu, J. \u0026amp; Srivastava, A. Optical control of the valley Zeeman effect through many-exciton interactions. \u003cem\u003eNature Nanotechnology\u003c/em\u003e \u003cstrong\u003e16\u003c/strong\u003e, 148-152 (2021).\u003c/li\u003e\n\u003cli\u003eGeim, A. K. \u0026amp; Grigorieva, I. V. Van der Waals heterostructures. \u003cem\u003eNature\u003c/em\u003e \u003cstrong\u003e499\u003c/strong\u003e, 419-425 (2013).\u003c/li\u003e\n\u003cli\u003eNovoselov, K. S., Mishchenko, A., Carvalho, A. \u0026amp; Castro Neto, A. H. 2D materials and van der Waals heterostructures. \u003cem\u003eScience\u003c/em\u003e \u003cstrong\u003e353\u003c/strong\u003e, aac9439 (2016).\u003c/li\u003e\n\u003cli\u003eNorden, T.\u003cem\u003e et al.\u003c/em\u003e Giant valley splitting in monolayer WS\u003csub\u003e2\u003c/sub\u003e by magnetic proximity effect. \u003cem\u003eNature Communications\u003c/em\u003e \u003cstrong\u003e10\u003c/strong\u003e, 4163 (2019).\u003c/li\u003e\n\u003cli\u003eHuang, B.\u003cem\u003e et al.\u003c/em\u003e Emergent phenomena and proximity effects in two-dimensional magnets and heterostructures. \u003cem\u003eNature Materials\u003c/em\u003e \u003cstrong\u003e19\u003c/strong\u003e, 1276-1289 (2020).\u003c/li\u003e\n\u003cli\u003eMak, K. F., Shan, J. \u0026amp; Ralph, D. C. Probing and controlling magnetic states in 2D layered magnetic materials. \u003cem\u003eNature Reviews Physics\u003c/em\u003e \u003cstrong\u003e1\u003c/strong\u003e, 646-661 (2019).\u003c/li\u003e\n\u003cli\u003eChoi, J., Lane, C., Zhu, J.-X. \u0026amp; Crooker, S. A. Asymmetric magnetic proximity interactions in MoSe\u003csub\u003e2\u003c/sub\u003e/CrBr\u003csub\u003e3\u003c/sub\u003e van der Waals heterostructures. \u003cem\u003eNature Materials\u003c/em\u003e \u003cstrong\u003e22\u003c/strong\u003e, 305-310 (2023).\u003c/li\u003e\n\u003cli\u003eLyons, T. P.\u003cem\u003e et al.\u003c/em\u003e Interplay between spin proximity effect and charge-dependent exciton dynamics in MoSe\u003csub\u003e2\u003c/sub\u003e/CrBr\u003csub\u003e3\u003c/sub\u003e van der Waals heterostructures. \u003cem\u003eNature Communications\u003c/em\u003e \u003cstrong\u003e11\u003c/strong\u003e, 6021 (2020).\u003c/li\u003e\n\u003cli\u003eZhong, D.\u003cem\u003e et al.\u003c/em\u003e Van der Waals engineering of ferromagnetic semiconductor heterostructures for spin and valleytronics. \u003cem\u003eScience Advances\u003c/em\u003e \u003cstrong\u003e3\u003c/strong\u003e, e1603113.\u003c/li\u003e\n\u003cli\u003eZhao, C.\u003cem\u003e et al.\u003c/em\u003e Enhanced valley splitting in monolayer WSe\u003csub\u003e2\u003c/sub\u003e due to magnetic exchange field. \u003cem\u003eNature Nanotechnology\u003c/em\u003e \u003cstrong\u003e12\u003c/strong\u003e, 757-762 (2017).\u003c/li\u003e\n\u003cli\u003eZhang, T.\u003cem\u003e et al.\u003c/em\u003e Electrically and Magnetically Tunable Valley Polarization in Monolayer MoSe\u003csub\u003e2\u003c/sub\u003e Proximitized by a 2D Ferromagnetic Semiconductor. \u003cem\u003eAdvanced Functional Materials\u003c/em\u003e \u003cstrong\u003e32\u003c/strong\u003e, 2204779 (2022).\u003c/li\u003e\n\u003cli\u003eZheng, H.\u003cem\u003e et al.\u003c/em\u003e Enhanced valley polarization in WSe\u003csub\u003e2\u003c/sub\u003e/YIG heterostructures via interfacial magnetic exchange effect. \u003cem\u003eNano Research\u003c/em\u003e \u003cstrong\u003e16\u003c/strong\u003e, 10580-10586 (2023).\u003c/li\u003e\n\u003cli\u003eBae, Y. J.\u003cem\u003e et al.\u003c/em\u003e Exciton-coupled coherent magnons in a 2D semiconductor. \u003cem\u003eNature\u003c/em\u003e \u003cstrong\u003e609\u003c/strong\u003e, 282-286 (2022).\u003c/li\u003e\n\u003cli\u003eSun, Y.\u003cem\u003e et al.\u003c/em\u003e Dipolar spin wave packet transport in a van der Waals antiferromagnet. \u003cem\u003eNature Physics\u003c/em\u003e \u003cstrong\u003e20\u003c/strong\u003e, 794-800 (2024).\u003c/li\u003e\n\u003cli\u003eCenker, J.\u003cem\u003e et al.\u003c/em\u003e Direct observation of two-dimensional magnons in atomically thin CrI\u003csub\u003e3\u003c/sub\u003e. \u003cem\u003eNature Physics\u003c/em\u003e \u003cstrong\u003e17\u003c/strong\u003e, 20-25 (2021).\u003c/li\u003e\n\u003cli\u003eLiu, S.\u003cem\u003e et al.\u003c/em\u003e Direct Observation of Magnon-Phonon Strong Coupling in Two-Dimensional Antiferromagnet at High Magnetic Fields. \u003cem\u003ePhysical Review Letters\u003c/em\u003e \u003cstrong\u003e127\u003c/strong\u003e, 097401 (2021).\u003c/li\u003e\n\u003cli\u003eDirnberger, F.\u003cem\u003e et al.\u003c/em\u003e Magneto-optics in a van der Waals magnet tuned by self-hybridized polaritons. \u003cem\u003eNature\u003c/em\u003e \u003cstrong\u003e620\u003c/strong\u003e, 533-537 (2023).\u003c/li\u003e\n\u003cli\u003eLin, K.\u003cem\u003e et al.\u003c/em\u003e Strong Exciton\u0026ndash;Phonon Coupling as a Fingerprint of Magnetic Ordering in van der Waals Layered CrSBr. \u003cem\u003eACS Nano\u003c/em\u003e \u003cstrong\u003e18\u003c/strong\u003e, 2898-2905 (2024).\u003c/li\u003e\n\u003cli\u003eCui, J.\u003cem\u003e et al.\u003c/em\u003e Chirality selective magnon-phonon hybridization and magnon-induced chiral phonons in a layered zigzag antiferromagnet. \u003cem\u003eNature Communications\u003c/em\u003e \u003cstrong\u003e14\u003c/strong\u003e, 3396 (2023).\u003c/li\u003e\n\u003cli\u003eOnga, M.\u003cem\u003e et al.\u003c/em\u003e Antiferromagnet\u0026ndash;Semiconductor Van Der Waals Heterostructures: Interlayer Interplay of Exciton with Magnetic Ordering. \u003cem\u003eNano Letters\u003c/em\u003e \u003cstrong\u003e20\u003c/strong\u003e, 4625-4630 (2020).\u003c/li\u003e\n\u003cli\u003eLiu, C.\u003cem\u003e et al.\u003c/em\u003e Probing the N\u0026eacute;el-Type Antiferromagnetic Order and Coherent Magnon\u0026ndash;Exciton Coupling in Van Der Waals VPS\u003csub\u003e3\u003c/sub\u003e. \u003cem\u003eAdvanced Materials\u003c/em\u003e \u003cstrong\u003e35\u003c/strong\u003e, 2300247 (2023).\u003c/li\u003e\n\u003cli\u003eZhao, S.-X.\u003cem\u003e et al.\u003c/em\u003e Interlayer Interaction of Excitons and Magnons in Graphene/WS\u003csub\u003e2\u003c/sub\u003e/N\u0026eacute;el-Type Manganese Phosphorus Trichalcogenide Heterostructures. \u003cem\u003eAdvanced Functional Materials\u003c/em\u003e \u003cstrong\u003e34\u003c/strong\u003e, 2405882 (2024).\u003c/li\u003e\n\u003cli\u003eZhang, Y.\u003cem\u003e et al.\u003c/em\u003e Magnon-Coupled Intralayer Moir\u0026eacute; Trion in Monolayer Semiconductor\u0026ndash;Antiferromagnet Heterostructures. \u003cem\u003eAdvanced Materials\u003c/em\u003e \u003cstrong\u003e34\u003c/strong\u003e, 2200301 (2022).\u003c/li\u003e\n\u003cli\u003eSerati de Brito, C.\u003cem\u003e et al.\u003c/em\u003e Charge Transfer and Asymmetric Coupling of MoSe\u003csub\u003e2\u003c/sub\u003e Valleys to the Magnetic Order of CrSBr. \u003cem\u003eNano Letters\u003c/em\u003e \u003cstrong\u003e23\u003c/strong\u003e, 11073-11081 (2023).\u003c/li\u003e\n\u003cli\u003eBeer, A.\u003cem\u003e et al.\u003c/em\u003e Proximity-Induced Exchange Interaction and Prolonged Valley Lifetime in MoSe\u003csub\u003e2\u003c/sub\u003e/CrSBr Van-Der-Waals Heterostructure with Orthogonal Spin Textures. \u003cem\u003eACS Nano\u003c/em\u003e \u003cstrong\u003e18\u003c/strong\u003e, 31044-31054 (2024).\u003c/li\u003e\n\u003cli\u003eWilson, N. P.\u003cem\u003e et al.\u003c/em\u003e Interlayer electronic coupling on demand in a 2D magnetic semiconductor. \u003cem\u003eNature Materials\u003c/em\u003e \u003cstrong\u003e20\u003c/strong\u003e, 1657-1662 (2021).\u003c/li\u003e\n\u003cli\u003eBrennan, N. J., Noble, C. A., Tang, J., Ziebel, M. E. \u0026amp; Bae, Y. J. Important Elements of Spin-Exciton and Magnon-Exciton Coupling. \u003cem\u003eACS Physical Chemistry Au\u003c/em\u003e \u003cstrong\u003e4\u003c/strong\u003e, 322-327 (2024).\u003c/li\u003e\n\u003cli\u003eCandido, D. R., Fuchs, G. D., Johnston-Halperin, E. \u0026amp; Flatt\u0026eacute;, M. E. Predicted strong coupling of solid-state spins via a single magnon mode. \u003cem\u003eMaterials for Quantum Technology\u003c/em\u003e \u003cstrong\u003e1\u003c/strong\u003e, 011001 (2021).\u003c/li\u003e\n\u003cli\u003eLee, K.\u003cem\u003e et al.\u003c/em\u003e Magnetic Order and Symmetry in the 2D Semiconductor CrSBr. \u003cem\u003eNano Letters\u003c/em\u003e \u003cstrong\u003e21\u003c/strong\u003e, 3511-3517 (2021).\u003c/li\u003e\n\u003cli\u003eWang, C.\u003cem\u003e et al.\u003c/em\u003e A family of high-temperature ferromagnetic monolayers with locked spin-dichroism-mobility anisotropy: MnNX and CrCX (X = Cl, Br, I; C = S, Se, Te). \u003cem\u003eScience Bulletin\u003c/em\u003e \u003cstrong\u003e64\u003c/strong\u003e, 293-300 (2019).\u003c/li\u003e\n\u003cli\u003eGao, Y., Liu, Q., Zhu, Y., Jiang, X. \u0026amp; Zhao, J. Magnetic field modulated photoelectric devices in ferromagnetic semiconductor CrXh (X = S/Se, h = Cl/Br/I) van der Waals heterojunctions. \u003cem\u003eApplied Physics Letters\u003c/em\u003e \u003cstrong\u003e119\u003c/strong\u003e, 032103 (2021).\u003c/li\u003e\n\u003cli\u003eDur\u0026aacute;n Retamal, J. R., Periyanagounder, D., Ke, J.-J., Tsai, M.-L. \u0026amp; He, J.-H. Charge carrier injection and transport engineering in two-dimensional transition metal dichalcogenides. \u003cem\u003eChemical Science\u003c/em\u003e \u003cstrong\u003e9\u003c/strong\u003e, 7727-7745 (2018).\u003c/li\u003e\n\u003cli\u003eLee, J.\u003cem\u003e et al.\u003c/em\u003e Modulation of Junction Modes in SnSe\u003csub\u003e2\u003c/sub\u003e/MoTe\u003csub\u003e2\u003c/sub\u003e Broken-Gap van der Waals Heterostructure for Multifunctional Devices. \u003cem\u003eNano Letters\u003c/em\u003e \u003cstrong\u003e20\u003c/strong\u003e, 2370-2377 (2020).\u003c/li\u003e\n\u003cli\u003eJiang, Y., Chen, S., Zheng, W., Zheng, B. \u0026amp; Pan, A. Interlayer exciton formation, relaxation, and transport in TMD van der Waals heterostructures. \u003cem\u003eLight: Science \u0026amp; Applications\u003c/em\u003e \u003cstrong\u003e10\u003c/strong\u003e, 72 (2021).\u003c/li\u003e\n\u003cli\u003eLe, C. T.\u003cem\u003e et al.\u003c/em\u003e Negative Valley Polarization of the Intralayer Exciton via One-Step Growth of H-Type Heterobilayer WS\u003csub\u003e2\u003c/sub\u003e/MoS\u003csub\u003e2\u003c/sub\u003e. \u003cem\u003eACS Nano\u003c/em\u003e \u003cstrong\u003e17\u003c/strong\u003e, 2629-2638 (2023).\u003c/li\u003e\n\u003cli\u003eYang, M.\u003cem\u003e et al.\u003c/em\u003e Relaxation and darkening of excitonic complexes in electrostatically doped monolayer WSe\u003csub\u003e2\u003c/sub\u003e: Roles of exciton-electron and trion-electron interactions. \u003cem\u003ePhysical Review B\u003c/em\u003e \u003cstrong\u003e105\u003c/strong\u003e, 085302 (2022).\u003c/li\u003e\n\u003cli\u003eHe, M.\u003cem\u003e et al.\u003c/em\u003e Valley phonons and exciton complexes in a monolayer semiconductor. \u003cem\u003eNature Communications\u003c/em\u003e \u003cstrong\u003e11\u003c/strong\u003e, 618 (2020).\u003c/li\u003e\n\u003cli\u003eRobert, C.\u003cem\u003e et al.\u003c/em\u003e Measurement of the spin-forbidden dark excitons in MoS\u003csub\u003e2\u003c/sub\u003e and MoSe\u003csub\u003e2\u003c/sub\u003e monolayers. \u003cem\u003eNature Communications\u003c/em\u003e \u003cstrong\u003e11\u003c/strong\u003e, 4037 (2020).\u003c/li\u003e\n\u003cli\u003eRobert, C.\u003cem\u003e et al.\u003c/em\u003e Fine structure and lifetime of dark excitons in transition metal dichalcogenide monolayers. \u003cem\u003ePhysical Review B\u003c/em\u003e \u003cstrong\u003e96\u003c/strong\u003e, 155423 (2017).\u003c/li\u003e\n\u003cli\u003eHuang, J., Hoang, T. B. \u0026amp; Mikkelsen, M. H. Probing the origin of excitonic states in monolayer WSe\u003csub\u003e2\u003c/sub\u003e. \u003cem\u003eScientific Reports\u003c/em\u003e \u003cstrong\u003e6\u003c/strong\u003e, 22414 (2016).\u003c/li\u003e\n\u003cli\u003eScheie, A.\u003cem\u003e et al.\u003c/em\u003e Spin Waves and Magnetic Exchange Hamiltonian in CrSBr. \u003cem\u003eAdvanced Science\u003c/em\u003e \u003cstrong\u003e9\u003c/strong\u003e, 2202467 (2022).\u003c/li\u003e\n\u003cli\u003ePawbake, A.\u003cem\u003e et al.\u003c/em\u003e Magneto-Optical Sensing of the Pressure Driven Magnetic Ground States in Bulk CrSBr. \u003cem\u003eNano Letters\u003c/em\u003e \u003cstrong\u003e23\u003c/strong\u003e, 9587-9593 (2023).\u003c/li\u003e\n\u003cli\u003eUykur, E.\u003cem\u003e et al.\u003c/em\u003e Phonon and magnon dynamics across antiferromagnetic transition in 2D layered van der Waals material CrSBr. Preprint at https://arxiv.org/abs/2405.07853 (2024).\u003c/li\u003e\n\u003cli\u003eKudlacik, D.\u003cem\u003e et al.\u003c/em\u003e Exciton and exciton-magnon photoluminescence in the antiferromagnet CuB\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e. \u003cem\u003ePhysical Review B\u003c/em\u003e \u003cstrong\u003e102\u003c/strong\u003e, 035128 (2020).\u003c/li\u003e\n\u003cli\u003eLiu, E.\u003cem\u003e et al.\u003c/em\u003e Valley-selective chiral phonon replicas of dark excitons and trions in monolayer WSe\u003csub\u003e2\u003c/sub\u003e. \u003cem\u003ePhysical Review Research\u003c/em\u003e \u003cstrong\u003e1\u003c/strong\u003e, 032007 (2019).\u003c/li\u003e\n\u003cli\u003eLee, D. H., Choi, S.-J., Kim, H., Kim, Y.-S. \u0026amp; Jung, S. Direct probing of phonon mode specific electron\u0026ndash;phonon scatterings in two-dimensional semiconductor transition metal dichalcogenides. \u003cem\u003eNature Communications\u003c/em\u003e \u003cstrong\u003e12\u003c/strong\u003e, 4520 (2021).\u003c/li\u003e\n\u003cli\u003eLi, Z.\u003cem\u003e et al.\u003c/em\u003e Phonon-exciton Interactions in WSe\u003csub\u003e2\u003c/sub\u003e under a quantizing magnetic field. \u003cem\u003eNature Communications\u003c/em\u003e \u003cstrong\u003e11\u003c/strong\u003e, 3104 (2020).\u003c/li\u003e\n\u003cli\u003eEremenko, V., Kachur, I., Novikov, V., Shapiro, V. J. S. J. o. E. \u0026amp; Physics, T. Scattering of excitons by long-wavelength magnons in the quasi-one-dimensional antiferromagnet CsMnCI\u003csub\u003e3\u003c/sub\u003e.2H\u003csub\u003e2\u003c/sub\u003eO. \u003cstrong\u003e67\u003c/strong\u003e, 1862 (1988).\u003c/li\u003e\n\u003cli\u003eCornelissen, L. J., Peters, K. J. H., Bauer, G. E. W., Duine, R. A. \u0026amp; van Wees, B. J. Magnon spin transport driven by the magnon chemical potential in a magnetic insulator. \u003cem\u003ePhysical Review B\u003c/em\u003e \u003cstrong\u003e94\u003c/strong\u003e, 014412 (2016).\u003c/li\u003e\n\u003cli\u003eOlsson, K. S.\u003cem\u003e et al.\u003c/em\u003e Pure Spin Current and Magnon Chemical Potential in a Nonequilibrium Magnetic Insulator. \u003cem\u003ePhysical Review X\u003c/em\u003e \u003cstrong\u003e10\u003c/strong\u003e, 021029 (2020).\u003c/li\u003e\n\u003cli\u003eStreib, S., Vidal-Silva, N., Shen, K. \u0026amp; Bauer, G. E. W. Magnon-phonon interactions in magnetic insulators. \u003cem\u003ePhysical Review B\u003c/em\u003e \u003cstrong\u003e99\u003c/strong\u003e, 184442 (2019).\u003c/li\u003e\n\u003cli\u003eShinokita, K.\u003cem\u003e et al.\u003c/em\u003e Continuous Control and Enhancement of Excitonic Valley Polarization in Monolayer WSe\u003csub\u003e2\u003c/sub\u003e by Electrostatic Doping. \u003cem\u003eAdvanced Functional Materials\u003c/em\u003e \u003cstrong\u003e29\u003c/strong\u003e, 1900260 (2019).\u003c/li\u003e\n\u003cli\u003eL\u0026oacute;pez-Paz, S. A.\u003cem\u003e et al.\u003c/em\u003e Dynamic magnetic crossover at the origin of the hidden-order in van der Waals antiferromagnet CrSBr. \u003cem\u003eNature Communications\u003c/em\u003e \u003cstrong\u003e13\u003c/strong\u003e, 4745 (2022).\u003c/li\u003e\n\u003cli\u003eHao, K.\u003cem\u003e et al.\u003c/em\u003e Direct measurement of exciton valley coherence in monolayer WSe\u003csub\u003e2\u003c/sub\u003e. \u003cem\u003eNature Physics\u003c/em\u003e \u003cstrong\u003e12\u003c/strong\u003e, 677-682 (2016).\u003c/li\u003e\n\u003cli\u003eCham, T. M. J.\u003cem\u003e et al.\u003c/em\u003e Anisotropic Gigahertz Antiferromagnetic Resonances of the Easy-Axis van der Waals Antiferromagnet CrSBr. \u003cem\u003eNano Letters\u003c/em\u003e \u003cstrong\u003e22\u003c/strong\u003e, 6716-6723 (2022).\u003c/li\u003e\n\u003cli\u003eKamimaki, A., Iihama, S., Suzuki, K. Z., Yoshinaga, N. \u0026amp; Mizukami, S. Parametric Amplification of Magnons in Synthetic Antiferromagnets. \u003cem\u003ePhysical Review Applied\u003c/em\u003e \u003cstrong\u003e13\u003c/strong\u003e, 044036 (2020).\u003c/li\u003e\n\u003cli\u003eSurrente, A.\u003cem\u003e et al.\u003c/em\u003e Intervalley Scattering of Interlayer Excitons in a MoS\u003csub\u003e2\u003c/sub\u003e/MoSe\u003csub\u003e2\u003c/sub\u003e/MoS\u003csub\u003e2\u003c/sub\u003e Heterostructure in High Magnetic Field. \u003cem\u003eNano Letters\u003c/em\u003e \u003cstrong\u003e18\u003c/strong\u003e, 3994-4000 (2018).\u003c/li\u003e\n\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":true,"hideJournal":true,"highlight":"","institution":"","isAcceptedByJournal":false,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true},"keywords":"valley selectivity manipulation, interfacial magnon-exciton interaction, van der Waals heterostructure, antiferromagnet, transition metal dichalcogenides","lastPublishedDoi":"10.21203/rs.3.rs-5909229/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-5909229/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eValley properties of monolayer (ML) transition metal dichalcogenide (TMDs) can be effectively manipulated via magnetic proximity effects in van der Waals (vdW) heterostructures (HS) stacked with 2D ferromagnetic materials and ML TMDs. Antiferromagnetic materials with high-frequency and long-lived coherent magnons, allowing interactions between distinct excitations at the heterointerface, potentially serve as an alternative to valley manipulation via heterostructure constructions, however this remains elusive. Here, we demonstrated the existence of interfacial magnon-exciton interaction (IMEI) in the vdW heterostructure composed of ML MoSe\u003csub\u003e2\u003c/sub\u003e and A-type antiferromagnetic CrSBr with in-plane magnetization. We proposed two mechanisms of IMEI, i.e., magnon-exciton scattering (MES), which induces the blueshift of excitonic states of MoSe\u003csub\u003e2\u003c/sub\u003e below the N\u0026eacute;el temperature of CrSBr, and magnon-assisting dark exciton recombination (MADER), which leads to the formation of magnon-exciton complexes. We found that MES induces a remarkable valley polarization (VP) enhancement of excitonic states from a completely quenched level, and the magnon-exciton complexes exhibit an increase in valley-contrasting circular dichroism when the spin orientation of CrSBr switched from in-plane to out-of-plane. Our work provides a new platform for manipulating excitonic and valley properties in non-magnetic semiconductors without external fields, opening up fresh opportunities of hybridized quasiparticles in quantum interconnects and opto-spintronics.\u003c/p\u003e","manuscriptTitle":"Valley Selectivity Manipulation via Interfacial Magnon-Exciton Interactions in TMD/CrSBr Antiferromagnetic van der Waals Heterostructures","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-03-17 08:33:45","doi":"10.21203/rs.3.rs-5909229/v1","editorialEvents":[{"type":"communityComments","content":0}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"a9516fd1-fcf8-4753-809e-7dbdf912c6e0","owner":[],"postedDate":"March 17th, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"posted","subjectAreas":[{"id":44251811,"name":"Physical sciences/Physics/Electronics, photonics and device physics/Electronic and spintronic devices"},{"id":44251812,"name":"Physical sciences/Physics/Optical physics/Magneto-optics"},{"id":44251813,"name":"Physical sciences/Nanoscience and technology/Nanoscale materials/Two-dimensional materials"}],"tags":[],"updatedAt":"2025-12-22T15:43:39+00:00","versionOfRecord":[],"versionCreatedAt":"2025-03-17 08:33:45","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-5909229","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-5909229","identity":"rs-5909229","version":["v1"]},"buildId":"8U1c8b4HqxoKbykW_rLl7","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}