The interlayer twist effectively regulates interlayer excitons in InSe/Sb van der Waals heterostructure

The interlayer twist effectively regulates interlayer excitons in InSe/Sb van der Waals heterostructure | 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 The interlayer twist effectively regulates interlayer excitons in InSe/Sb van der Waals heterostructure Xianghong Niu, Anqi Shi, Ruilin Guan, Zifan Niu, Wenxia Zhang, and 4 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-4161258/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 26 Aug, 2024 Read the published version in npj Computational Materials → Version 1 posted 9 You are reading this latest preprint version Abstract The interlayer twist angle endows a new degree of freedom to manipulate the spatially separated interlayer excitons in van der Waals (vdWs) heterostructures. Herein, we find that the band-edge Γ-Γ interlayer excitation directly forms interlayer exciton in InSe/Sb heterostructure, different from that of transition metal dichalcogenides (TMDs) heterostructures in two-step processes by intralayer excitation and transfer. By tuning the interlayer coupling and breathing vibrational modes associated with the Γ-Γ photoexcitation, the interlayer twist can significantly adjust the excitation peak position and lifetime of recombination. The interlayer excitation peak in InSe/Sb heterostructure can shift ~ 400 meV, and the interlayer exciton lifetime varies in hundreds of nanoseconds as a periodic function of the twist angle (0°-60°). This work enriches the understanding of interlayer exciton formation and facilitates the artificial excitonic engineering of vdWs heterostructures. Physical sciences/Materials science/Nanoscale materials/Two-dimensional materials Physical sciences/Materials science/Nanoscale materials/Electronic properties and materials interlayer exciton vdW heterostructure twist angle first-principles excited state dynamics Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Introduction For 2D semiconductors, the absence of dangling bonds, short of electron and hole migration paths and superior mobility at atomic layer thickness are very beneficial to provide the long-lived photogenerated carriers compared with traditional bulk materials. 1, 2 The long-lived photogenerated electrons and holes are critical for a broad range of applications in optoelectronics, photovoltaics, photocatalysis, sensors and biomedicine. 3, 4 Moreover, the rational design and synthesis of 2D heterojunctions is an important strategy to further improve the lifetime of photogenerated carriers. The rapidly separating photogenerated electron holes into different sublayers have a chance to form interlayer exciton. 5–7 The long-lived interlayer excitons possess great potential to pave the way in realistically exploring Bose-Einstein condensation 8 , temperature superfluidity 9 and light-induced exciton spin Hall effect 10 new physical phenomena. Therefore, in-depth understanding and regulation of interlayer excitons in 2D heterojunctions plays an essential role in various of application of 2D semiconductor devices. Inspired by stacking two graphene at a specific angle to present some unexpected properties, such as superconductor or insulator, 11, 12 the interlayer twist endows a new degree of freedom to flexibly engineer the electronic structures and interlayer excitons. 13 To date, artificially twisted 2D semiconductor heterostructures are mainly focused on transition-metal dichalcogenides (TMDs), which can indirectly form interlayer excitons in two steps, namely, photoexcitation forming intralayer exciton and then the photogenerated electron or hole transfer into the opposite sublayers. 7, 14–19 It is extremely complex to the formation dynamics and corresponding regulation of the interlayer excitons induced by two-step processes . 20 Since the interlayer photoexcitation probability is two orders of magnitude smaller than that of intralayer excitation in TMDs 2D heterostructures, 21–23 the formation of interlayer exciton is mainly explored from indirect photoluminescence rather than direct photoabsorption. 7 Simultaneously, although the time scale of transfer process from intralayer to interlayer exciton can be detected by using femtosecond pump-probe spectroscopy and phase-locked electromagnetic pulses, 24 a comprehensive understanding of photogenerated carriers transfer is still very difficult due to the complex momentum-space indirect intervalley transfer, such as Q-Γ, Q-K, K-Γ excitons. 17, 25, 26 It is also unclear whether intralayer photogenerated carriers are transferred into interlayer in the form of free or bound carriers. 27, 28 Therefore, to practical applications of interlayer exciton on specific devices, it is still necessary to increase the understanding of the interlayer exciton formation and regulation. In this work, we systematically investigate the formation and regulation of interlayer exciton based on first-principles and nonadiabatic molecular dynamics (NAMD) simulations. The interlayer exciton can be directly formed by interlayer photoexcitation in 2D indium selenide/antimonene (InSe/Sb) heterostructure. The interface atoms of Sb and InSe sublayers contribute the valence band maximum (VBM) and conduction band minimum (CBM) of heterostructure at Γ point, respectively, which forms an interlayer Γ-Γ transition channel due to the strong interlayer coupling and short spatial distance. By uniformly taking seven twist angles in the 0°-60° range, the interlayer twist can directly affect the interlayer interaction and change the electronic structure of band edge. Then, the interlayer exciton's lifetime and peak position can be regulated on a large scale. Results and discussion The interlayer exciton in TMDs heterostructures is formed in indirect two-step processes; that is, the intralayer exciton is firstly formed in one sublayer, and then the photogenerated electrons transfer into the other sublayer as shown in Fig. 1 a ① and ② processes. The process has been confirmed by many experimental and theoretical studies. 7, 14, 24, 26, 28 In fact, the formation mode can be clearly illustrated from the geometry and electronic structure of the TMDs. Taking MoS 2 as an example (see Fig. 1 b), monolayer MoS 2 is a sandwich structure with the middle Mo atom layer surrounded by two outer S atomic layers. The intermediate Mo atom layer mainly contributes to valence and conduct band edges. Hence, after forming type II TMDs heterostructures, the direct interlayer photoexcitation at band edges (see Fig. 1 a, the ③ process) will be difficult due to the large spatial distance between the two Mo atomic layers. Therefore, interlayer exciton in TMDs heterostructures can only be formed in intralayer excitation and interlayer transfer mechanism. To improve the probability of interlayer photoexcitation at band edges, the band edge components should be mainly composed of interface atoms. This can reduce the photoexcitation spatial distance of carriers. InSe, possessing high electron mobility (10 3 -10 4 cm 2 V − 1 s − 1 ), on/off ratio (~ 10 8 ), quantum Hall effect, and anomalous optical response 29, 30 , has attracted widespread attention in electronic and photoelectric applications. More fortunately, the p z orbital of surface Se atoms mainly contribute to its band edge states (see Fig. 1 c). This can reduce the spatial distance of photoexcitation channel after forming a vertical heterojunction with the other 2D semiconductor. 2D Sb semiconductor, a group-VA material, has been successfully prepared by various methods, such as liquid or mechanical exfoliation, 31–33 vdW epitaxy growth. 34 As a potential 2D photoelectric material, it not only has good photoresponse property 33, 35 , but also possesses high environmental stability. 36 More interesting, Sb is suitable for constructing heterojunction with InSe to explore interlayer excitation (see Fig. 1 d). First of all, the VBM of Sb is located at the Γ point (see Fig. 1 g), which is in agreement with the CBM of InSe. Secondly, 2D Sb is a buckled honeycomb structure, and each Sb atom is bonded to three neighboring Sb atoms. Then, the nonbonding lone pair electrons are left at the surface, which can increase the interlayer coupling after forming a vertical heterojunction. And lastly, the lattice constants of Sb (4.12 Å) and InSe (4.07 Å) are very well matched with each other. Then, by adjusting the twist angles (see Fig. 1 e), the interlayer interaction can be periodically regulated, and the superlattice pattern can appear simultaneously. Therefore, the InSe/Sb heterojunction will be a suitable system to explore the direct formation of interlayer excitons and the interlayer twist regulation of interlayer excitons. We define a highly symmetrical structure as the 0° twist angle structure as shown in Figure S1 . The Sb and Se atoms at the interface of heterostructure are staggered arrangement forming strong interlayer coupling. Since 2D InSe and Sb are hexagonal lattice, after twisting 60° for one sublayer, the heterostructure can form a new highly symmetrical structure. Therefore, we evenly take seven twist angles from 0° to 60° (that is, 0.0°, 10.9°, 19.1°, 30.0°, 40.9°, 49.1° and 60.0°, see Figure S1 -S8) to investigate the formation and regulation of interlayer exciton in InSe/Sb heterostructure. According to the previously widely studied twist stacking preparation strategy for 2D materials, such as graphene, hexagonal boron nitride, TMDs, the InSe/Sb heterostructures with different twist angles have the opportunity to be prepared by using the stamping dry-transfer method. 19, 37, 38 As expected, InSe/Sb heterostructure is a type II heterojunction (see Fig. 2 a). The VBM and CBM are located at Γ point, which are contributed by Sb and InSe sublayers, respectively. The band gap of InSe/Sb heterostructure can be significantly adjusted from 0.63 to 0.91 eV by the different twist angles (see Fig. 2 a- 2 g). As presented in Fig. 2 h, the highly symmetrical structures possess stronger binding energy (around − 45 meV per atom) than asymmetric structures (around − 35 meV per atom). It's worth noting that even for asymmetric structures, the interlayer interactions are much stronger than typical 2D vdW interaction, such as bilayer MoS 2 or graphene/MoS 2 heterojunctions (around − 20 meV per atom). The strong interlayer interaction of InSe/Sb heterostructure will facilitate direct interlayer photoexcitation. As exhibited in Fig. 2 i, the photoexcitation threshold of the InSe/Sb heterostructures (around 0.6 -1.0 eV) is obviously smaller than that of isolated 2D InSe and Sb layers (larger than 1.5 eV). That is, the intralayer photoexcitation cannot contribute to the first photoabsorption peak of InSe/Sb heterostructures. Simultaneously, the electronic band gap of these heterostructures is also in the range from ~ 0.6 to ~ 1.0 eV. Therefore, the first photoabsorption peak should derive from the direct interlayer photoexcitation at band edges of heterostructures. Specifically, for the interlayer photoexcitation at around Γ point, the square of the transition dipole moments ( P 2 : see Fig. 2 j). reaches up to ~ 300–500 Debye 2 , which has similar transition strength with the intralayer photoexcitation of isolated 2D InSe and Sb layers. Therefore, the direct interlayer bright photoexcitation can occur in InSe/Sb heterostructures. Note that, for InSe/Sb heterostructure with 0.0°, 10.9°, 30.0°, 49.1° and 60.0° twist angles, the first photoexcitation is bright excitation from VBM to CBM. For InSe/Sb heterostructure with 19.1° and 40.9° twist angles, the first bright excitation arises from the transition channel from VBM-4 to CBM, and VBM-3 to CBM, respectively. Therefore, the bandgap value is smaller than the first peak position for InSe/Sb heterostructure with 19.1° and 40.9° twist angles. For the calculation of transition dipole moment, we use the sum of transition between the first four valence bands and one conduction band for InSe/Sb heterostructure with 19.1° and 40.9° twist angles, The interlayer twist can shift the peak position up to ~ 400 meV. In previous researches, the shifted range of the first photoluminescence peak is ~ 60 meV in twisted MoSe 2 /WS 2 heterostructure,) 16 , ~ 90 meV in MoS 2 /WSe 2 heterostructure 39 and ~ 100 meV in WS 2 bilayer 38 . Interesting, for InSe/Sb heterostructure, MoSe 2 /WS 2 heterostructure and WS 2 bilayer, although their shifted range of the first peak varies widely, the trend is consistent with each other. That is, for the highly symmetrical interlayer stacking heterostructure with twist angle near 0° or 60°, the energy of peak is small, while for the low symmetrical interlayer stacking heterostructures, the energy of peak is gradually increasing. the highly symmetrical interlayer stacking mode increases interlayer interaction and promotes the wavefunction coupling of band edge electronic states. this can be further confirmed by the transition probability between band edges (seeing Fig. 2 j). for highly symmetrical interlayer stacking heterostructures (0° and 60°), the Γ-Γ interlayer photoexcitation possesses a larger transition probability ( P 2 : >500 Debye 2 ) compared with that of other heterostructures ( P 2 : 300–400 Debye 2 ) . As presented in Fig. 3 a, after forming heterojunction, the InSe and Sb sublayer all contribute electrons to the interface central region, which is different common phenomenon of charge transfer from one sublayer to the other. 40, 41 Then, the stacked charge wavefunction distribution in the interface region can provide a buffer to increase the wavefunction overlap of interlayer transition channel, thereby in turn enhancing the transition probability of direct interlayer excitation. The interlayer twist obviously changes the distribution of charge density difference. As shown in Fig. 3 and S9-S15, for the highly symmetrical interlayer stacking heterostructures with 0° and 60° twist angles, there accumulates more charges at interface central region compared with that of the low symmetrical modes. This further indicates that the interlayer excitation of the highly symmetrical stacked structures has a greater transition probability, consistent with the result of the transition dipole moment in Fig. 2 j. Since the lattice parameter of InSe and Sb sublayer is similar to each other, for the low symmetrical modes, these heterostructures form a superlattice pattern (see Fig. 3 ). According to the different superlattice patterns of sectional charge distribution, the various interlayer twist angles indeed bring about different regulatory effects for electronic structure and interlayer photoexcitation properties. After interlayer photoexcitation, the photogenerated electron and hole are localized in InSe and Sb sublayer, respectively. The lifetime of photogenerated carriers plays an essential role in various applications, such as optoelectronics, photovoltaics, and sensors. We perform the NAMD simulation by initiating the photogenerated electron at the conduction band edge of heterojunction (see Fig. 4 b- 4 h). After the photogenerated electron recombines with the hole located in the valance band edge, the time interval is defined as the lifetime of photogenerated carriers. For the InSe/Sb heterojunctions with different twist angles, we find that only less than 6% of photogenerated carriers recombine in 5 ns simulating time (see Fig. 4 a). Although the precise lifetime is hard to obtain based on the current simulation period, we can estimate the timescale by fitting an exponential function: P(t) = exp(-t/τ). As presented in Fig. 4 b- 4 h, for different twist angle structures, the lifetime of photogenerated carriers is as high as 96.2 to 1181.9 ns. That is, the interlayer exciton can be adjusted over a wide range by interlayer twist. Generally, the photogenerated carrier hopping probability between two electronic states inversely depends on the square of nonadiabatic coupling (NAC) based on Fermi's golden rule. As exhibited in Fig. 5 a, the largest value of NAC is less than 2.5 meV for all InSe/Sb heterojunctions with different twist angles. Such a small NAC value ensures the long-lived photogenerated carrier lifetimes. Moreover, compared with the highly symmetrical structures, the low symmetrical structures generally have a smaller NAC coefficient. To facilitate comparison, we present the averaged absolute value of NAC between the adjacent 10 band edge states in Fig. 5 b- 5 h. The InSe/Sb heterojunction with 60° (40°) twist angle possesses the largest (smallest) NAC coefficient between VBM and CBM electronic states, which is in agreement with the longest (shortest) lifetime of InSe/Sb heterojunctions. That is, the interlayer twist has a strong regulatory effect on the photogenerated carrier lifetime. Simultaneously, the average NAC between other neighboring states is larger than that of VBM and CBM. This also facilitates the other photogenerated carriers transferring into the VBM and CBM band edge states, forming the Γ-Γ interlayer exciton. The NAC element is dependent on the energy gap difference of hopping channel ( \({\epsilon }_{k}-{\epsilon }_{j}\) ), the electron-phonon coupling ( \(\langle {\phi _j}|{\nabla _R}H|{\phi _k}\rangle\) ) and nuclear velocity ( Ṙ I ) describing as follows: \({d_{jk}}=\langle {\phi _j}|\frac{\partial }{{\partial t}}|{\phi _k}\rangle =\sum\limits_{I} {\frac{{\langle {\phi _j}|{\nabla _R}H|{\phi _k}\rangle }}{{{\varepsilon _k} - {\varepsilon _j}}}\mathop {{R_I}}\limits^{ \bullet } }\) Where H is the Kohn-Sham Hamiltonian, \({\phi _k}\) , \({\phi _j}\) , \({\epsilon }_{j}\) , \({\epsilon }_{k}\) are the wave-functions and corresponding eigenvalues for j and k electronic states, respectively, and Ṙ I is velocity of the nuclei. For InSe/Sb heterojunctions with different twist angles, since the elements and the temperature are the same with each other, the difference in NAC should derive from the energy gap difference and electron-phonon coupling term. As discussed above, the band gap of InSe/Sb heterojunctions can be gradually adjusted from 0.63 to 0.91 eV with the change of twist angle. That is, the small energy gap difference will increase the carrier hopping probability, which is consistent with the trend of photo-generated carrier lifetime with the change of twist angle. For the electron-phonon coupling term, its strength can be reflected by the energy fluctuation of involved electronic states. As shown in Fig. 4 b- 4 h, the fluctuation of VBM with the time evolution is stronger than that of CBM. Hence, the vibration of Sb sublayer will play a more critical role in lifetime. To visualize the phonon modes dominating the fluctuation, the Fourier transforms (FT) of the autocorrelation functions are calculated to the time-dependent evolution of the band edges energy difference (Fig. 5 i). For all InSe/Sb heterojunctions, the vibrational peaks are mainly concentrated around 50 and 200 cm − 1 , attributed to the interlayer breathing mode, A 1g mode of InSe 42 and Sb 34 sublayer, respectively. Clearly, the phonon spectral density changes from high to low as the different twist angle structures from high to low symmetric stacking mode. This is also consistent with the trend of photogenerated carrier lifetime. Moreover, the pure-dephasing time between initial and final electronic states, similar to Huang-Rhys factor and Frank-Condon factor, is also associated with the lifetime of nonradiative recombination. The fast loss of quantum coherence can suppress the hopping rate. As presented in Fig. 5 j, for all InSe/Sb heterojunctions, the range of pure dephasing time is from 10 to 27 fs by Gaussian fitting, exp(-0.5(t/τ)). This is obviously smaller than that of MoS 2 /WS 2 heterojunctions with different twist angles from 37 to 58 fs. 18 Hence, the small pure dephasing time also contributes to the long lifetime of photogenerated carriers for InSe/Sb heterojunctions. For 2D materials, the excitonic effect is of significance due to the enhanced Coulomb interactions. Unfortunately, for InSe/Sb heterojunctions with various twist angles, it is not yet feasible because of excessive computational expense associated with NAMD involving thousands of electronic structure calculations. Although the single-particle picture cannot accurately obtain the lifetime of photogenerated electron and hole recombination, the change trends of lifetime should be reliable as the twist angle changes. In previous researches, Zhu et al. have studied the effect of twist angle on the photogenerated electron and hole recombination in MoS 2 /WS 2 heterostructure and WS 2 bilayer 17 based on single-particle picture. They found that the larger bandgaps or smaller nonadiabatic couplings make the slower electron and hole recombination in twisted than high-symmetry structures. The trend of their results is consistent with the experiments 19, 38 . Conclusions Combining fist-principles and nonadiabatic molecular dynamics simulations, we find that the InSe/Sb heterojunction can form interlayer excitons in one-step interlayer photoexcitation, and the photo-response range and lifetime can be significantly modulated by interlayer twist. the interlayer twist can periodically regulate the interlayer coupling. Then, the band edge states, contributed by interface atoms, can be directly affected by different twist angles. This induces the large range of regulation for the interlayer excitation peak and photogenerated carrier lifetime. This study enriches the understanding and engineering the interlayer exciton in artificial 2D vdW heterostructure materials. Declarations Author contributions X. N. and A. S. conceived the project. A. S., R. G. and Z. N carried out DFT and NAMD calculations. W. Z., X. Z., and S. W. carried out twist model constructing and DFT calculations. A. S., X. N., J. L. and B. W. co-wrote the paper with all authors contributing to the discussion and preparation of the manuscript. Acknowledgements This work is supported by China Postdoctoral Science Foundation (Grant No. 2022M711691), National Natural Science Foundation of China (Grant No. 12104130), Natural Science Foundation of Shanxi province (Grant No. 20210302123336), Six talent peaks project in Jiangsu Province (Grant No. XCL-104), Jiangsu Innovation Projects for Graduate Student (Grant Nos. 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ACS Nano 2021, 15 , 14394-14403. Yan, W.; Meng, L.; Meng, Z.; Weng, Y.; Kang, L.; Li, X.-a., Probing Angle-Dependent Interlayer Coupling in Twisted Bilayer Ws2. J. Phys. Chem. C 2019, 123 , 30684-30688. Kim, J.; Ko, E.; Jo, J.; Kim, M.; Yoo, H.; Son, Y.-W.; Cheong, H., Anomalous Optical Excitations from Arrays of Whirlpooled Lattice Distortions in Moiré Superlattices. Nat. Mater. 2022, 21 , 890-895. Niu, X.; Li, Y.; Shu, H.; Yao, X.; Wang, J., Efficient Carrier Separation in Graphitic Zinc Oxide and Blue Phosphorus Van Der Waals Heterostructure. J. Phys. Chem. C 2017, 121 , 3648-3653. Niu, X.; Bai, X.; Zhou, Z.; Wang, J., Rational Design and Characterization of Direct Z-Scheme Photocatalyst for Overall Water Splitting from Excited State Dynamics Simulations. ACS Catal. 2020, 10 , 1976-1983. Ahmad, W.; Liu, J.; Jiang, J.; Hao, Q.; Wu, D.; Ke, Y.; Gan, H.; Laxmi, V.; Ouyang, Z.; Ouyang, F.; Wang, Z.; Liu, F.; Qi, D.; Zhang, W., Strong Interlayer Transition in Few‐Layer Inse/Pdse2 Van Der Waals Heterostructure for near‐Infrared Photodetection. Adv. Funct. Mater. 2021, 31 , 2104143. Additional Declarations (Not answered) Supplementary Files supportinginformation.docx Supporting Information Schematic diagram of the twist supercell in hexagonal lattice with different twist angles; the top and side view for supercell structure of InSe/Sb heterostructure; and the charge density difference and photo-absorption of InSe/Sb heterostructures. (PDF) Cite Share Download PDF Status: Published Journal Publication published 26 Aug, 2024 Read the published version in npj Computational Materials → Version 1 posted Editorial decision: revise 10 Jun, 2024 Review # 2 received at journal 08 Jun, 2024 Review # 1 received at journal 23 May, 2024 Reviewer # 2 agreed at journal 14 May, 2024 Reviewer # 1 agreed at journal 25 Apr, 2024 Reviewers invited by journal 24 Apr, 2024 Submission checks completed at journal 27 Mar, 2024 Editor assigned by journal 25 Mar, 2024 First submitted to journal 25 Mar, 2024 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. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. 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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-4161258","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":295142370,"identity":"c75ecf74-57ac-4ede-89dd-84723a2d9158","order_by":0,"name":"Xianghong Niu","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAAy0lEQVRIie3RrwvCQBTA8TcOZtlcvRX/hgdGwb9lsGBZHgbDLEuKdeDYn2HeeGCS5cEuaDEZFi2C+2WT7WyG+6Z7cB9eeAAq1T/GAVJYA+smXZpcGsJ+IKCFzUuWYLnPyEzEBMtDCpVPYB2DYWLHuUPm6c5QEGhRTsBFOkws7mFNiGHhAjNDAuTOMNFbEvfkJUO6LUFPNBliRx5m8ZmYLQizXb4yeDFCsPDm1WND7rTc3q5PfzGzohHyye1uCmDI/a9btjdVqVQq1bfeQz5Cu+tRe3IAAAAASUVORK5CYII=","orcid":"","institution":"Nanjing University of Posts \u0026 Telecommunications","correspondingAuthor":true,"prefix":"","firstName":"Xianghong","middleName":"","lastName":"Niu","suffix":""},{"id":295142371,"identity":"a53438e0-7ffb-4a87-b382-8a3e5ff66223","order_by":1,"name":"Anqi Shi","email":"","orcid":"","institution":"Nanjing University of Posts \u0026 Telecommunications","correspondingAuthor":false,"prefix":"","firstName":"Anqi","middleName":"","lastName":"Shi","suffix":""},{"id":295142372,"identity":"cbc276bd-bf0c-4d5e-af89-6f36b5969f3d","order_by":2,"name":"Ruilin Guan","email":"","orcid":"","institution":"Nanjing University of Posts \u0026 Telecommunications","correspondingAuthor":false,"prefix":"","firstName":"Ruilin","middleName":"","lastName":"Guan","suffix":""},{"id":295142373,"identity":"29bbb1b0-e551-469b-a699-0a413f9ce3f2","order_by":3,"name":"Zifan Niu","email":"","orcid":"","institution":"Nanjing University of Posts \u0026 Telecommunications","correspondingAuthor":false,"prefix":"","firstName":"Zifan","middleName":"","lastName":"Niu","suffix":""},{"id":295142374,"identity":"45ef919f-dc4b-4e5e-9fce-c99e3c0e96b2","order_by":4,"name":"Wenxia Zhang","email":"","orcid":"","institution":"Chongqing University of Posts and Telecommunications","correspondingAuthor":false,"prefix":"","firstName":"Wenxia","middleName":"","lastName":"Zhang","suffix":""},{"id":295142375,"identity":"4d471cdb-cb45-4630-b7dd-4e384e8edcf1","order_by":5,"name":"Xiuyun Zhang","email":"","orcid":"","institution":"Yangzhou University","correspondingAuthor":false,"prefix":"","firstName":"Xiuyun","middleName":"","lastName":"Zhang","suffix":""},{"id":295142376,"identity":"0c776587-0fb7-4714-a101-38ce5f7a5270","order_by":6,"name":"Shiyan Wang","email":"","orcid":"","institution":"Nanjing University of Posts \u0026 Telecommunications","correspondingAuthor":false,"prefix":"","firstName":"Shiyan","middleName":"","lastName":"Wang","suffix":""},{"id":295142377,"identity":"58a8c9ca-19af-4474-960f-954988ca3e54","order_by":7,"name":"Bing Wang","email":"","orcid":"https://orcid.org/0000-0003-2537-5805","institution":"Henan University","correspondingAuthor":false,"prefix":"","firstName":"Bing","middleName":"","lastName":"Wang","suffix":""},{"id":295142378,"identity":"4ffb9b91-8181-4d67-91ad-5a1f104fdef0","order_by":8,"name":"Jin Lv","email":"","orcid":"","institution":"Shanxi Normal University","correspondingAuthor":false,"prefix":"","firstName":"Jin","middleName":"","lastName":"Lv","suffix":""}],"badges":[],"createdAt":"2024-03-25 07:00:44","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-4161258/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-4161258/v1","draftVersion":[],"editorialEvents":[{"content":"https://doi.org/10.1038/s41524-024-01384-6","type":"published","date":"2024-08-26T04:00:00+00:00"}],"editorialNote":"","failedWorkflow":false,"files":[{"id":55561494,"identity":"53cc0f16-c68c-459c-91ca-2e763ca39d7f","added_by":"auto","created_at":"2024-04-30 02:55:02","extension":"jpg","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":675541,"visible":true,"origin":"","legend":"\u003cp\u003e(a) The schematic diagram of intralayer and interlayer excitons in 2D heterostructures and the indirect (① and ②) and direct (③) formation processes for interlayer excitons. (b, c) Projection-resolved band structures for 3×3 supercell of MoS\u003csub\u003e2\u003c/sub\u003e and InSe monolayers. The illustration is a side view of MoS\u003csub\u003e2\u003c/sub\u003e and InSe monolayers. (d) The diagrammatic process of directly forming interlayer excitons in InSe/Sb heterostructure. (e) the diagram of twist angle for InSe/Sb heterostructure. (f, g) Projection-resolved band structures for 3×3 supercell of InSe and Sb monolayers. The gray region at valence and conduct band edge of sublayers may form a direct interlayer photoexcitation channel after constructing InSe/Sb heterostructure. Fermi level is set to 0 eV.\u003c/p\u003e","description":"","filename":"floatimage1.jpg","url":"https://assets-eu.researchsquare.com/files/rs-4161258/v1/fc588ba0039f9a305179f261.jpg"},{"id":55562140,"identity":"4a7a0344-4b41-4a0c-a93b-9437f9431171","added_by":"auto","created_at":"2024-04-30 03:03:02","extension":"jpg","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":636043,"visible":true,"origin":"","legend":"\u003cp\u003e(a-g) Projection-resolved band structures for the InSe/Sb heterostructures with different interlayer twist angle. The red and blue dots represent as the contributions of Sb and InSe sublayers, respectively. The inserted value is the band gap. Fermi level is set to 0 eV. (h) the average binding energy per atom of InSe/Sb heterostructures with different interlayer twist angle and other corresponding heterostructures. (i) Photoabsorption of the isolated InSe and Sb layers, and InSe/Sb heterostructures with different twist angles. The absorption spectrum in light green area refers to the interlayer photoexcitation. (j) The square of the transition dipole moment between valence and conduct band edges for the isolated InSe and Sb monolayers, and InSe/Sb heterostructures with different twist angles.\u003c/p\u003e","description":"","filename":"floatimage2.jpg","url":"https://assets-eu.researchsquare.com/files/rs-4161258/v1/2ac9202572fa3d9277e24c6e.jpg"},{"id":55561495,"identity":"79b39fc4-e100-4094-8b99-1aba823bd9b4","added_by":"auto","created_at":"2024-04-30 02:55:02","extension":"jpg","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":505785,"visible":true,"origin":"","legend":"\u003cp\u003e(a) The charge density difference of InSe/Sb heterostructure with 0° twist angle. The yellow and cyan regions refer to distribution of positive and negative charges, respectively. (b-g) The top view of the sectional distribution of charge density difference in the interface central area for InSe/Sb heterostructure with other twist angle. The unit of the color scale is the e bohr\u003csup\u003e-3\u003c/sup\u003e.\u003c/p\u003e","description":"","filename":"floatimage3.jpg","url":"https://assets-eu.researchsquare.com/files/rs-4161258/v1/6f722e7fb7616858f7b02cdd.jpg"},{"id":55561498,"identity":"5f6c042a-7e1d-4f81-b31f-f10353d5167b","added_by":"auto","created_at":"2024-04-30 02:55:02","extension":"jpg","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":370435,"visible":true,"origin":"","legend":"\u003cp\u003e(a) The averaged photogenerated electron and hole nonradiative recombination dynamics in InSe/Sb heterojunctions with different twist angles. (b-h) Time-dependent evolution of the band edges and its adjacent electronic states of InSe/Sb heterojunctions with different twist angles. The blue and red lines denote the conduct and valence band edges, respectively. Fermi level is set to 0 eV. The temperature is set to 300 K. The insert values are the averaged photogenerated electron and hole nonradiative recombination lifetime.\u003c/p\u003e","description":"","filename":"floatimage4.jpg","url":"https://assets-eu.researchsquare.com/files/rs-4161258/v1/d7fbc94f7c2e60dbffe89827.jpg"},{"id":55561497,"identity":"13cc114b-9a7d-4fa9-8ffc-2c774e09697a","added_by":"auto","created_at":"2024-04-30 02:55:02","extension":"jpg","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":380253,"visible":true,"origin":"","legend":"\u003cp\u003e(a) The Time-dependent evolution of absolute value of NAC between VBM and CBM for InSe/Sb heterojunctions with different twist angles. (b-h) The averaged absolute value of NAC between the adjacent 10 band edge states for InSe/Sb heterojunctions with different twist angles. The temperature is set to 300 K. The inset value is the averaged absolute value of NAC between VBM and CBM. (i) Fourier transforms of the autocorrelation functions for the fluctuations of time evolution of bandgap between VBM and CBM of InSe/Sb heterojunctions with different twist angles. (j) Pure-dephasing functions between VBM and CBM of InSe/Sb heterojunctions with different twist angles.\u003c/p\u003e","description":"","filename":"floatimage5.jpg","url":"https://assets-eu.researchsquare.com/files/rs-4161258/v1/e537dcc3150a086842d29965.jpg"},{"id":63345805,"identity":"ba37835c-3560-4e1f-8361-5b27e86cce90","added_by":"auto","created_at":"2024-08-27 07:24:50","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":3016859,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-4161258/v1/6abf073b-a097-4df2-8b22-966d08857676.pdf"},{"id":55561499,"identity":"e522a3de-00ac-466d-b1a3-6890b355d644","added_by":"auto","created_at":"2024-04-30 02:55:03","extension":"docx","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":7915897,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eSupporting Information\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eSchematic diagram of the twist supercell in hexagonal lattice with different twist angles; the top and side view for supercell structure of InSe/Sb heterostructure; and the charge density difference and photo-absorption of InSe/Sb heterostructures. (PDF)\u003c/p\u003e","description":"","filename":"supportinginformation.docx","url":"https://assets-eu.researchsquare.com/files/rs-4161258/v1/737c485d701e51e4bbaa3e73.docx"}],"financialInterests":"(Not answered)","formattedTitle":"The interlayer twist effectively regulates interlayer excitons in InSe/Sb van der Waals heterostructure","fulltext":[{"header":"Introduction","content":"\u003cp\u003eFor 2D semiconductors, the absence of dangling bonds, short of electron and hole migration paths and superior mobility at atomic layer thickness are very beneficial to provide the long-lived photogenerated carriers compared with traditional bulk materials.\u003csup\u003e1, 2\u003c/sup\u003e The long-lived photogenerated electrons and holes are critical for a broad range of applications in optoelectronics, photovoltaics, photocatalysis, sensors and biomedicine.\u003csup\u003e3, 4\u003c/sup\u003e Moreover, the rational design and synthesis of 2D heterojunctions is an important strategy to further improve the lifetime of photogenerated carriers. The rapidly separating photogenerated electron holes into different sublayers have a chance to form interlayer exciton.\u003csup\u003e5\u0026ndash;7\u003c/sup\u003e The long-lived interlayer excitons possess great potential to pave the way in realistically exploring Bose-Einstein condensation\u003csup\u003e8\u003c/sup\u003e, temperature superfluidity\u003csup\u003e9\u003c/sup\u003e and light-induced exciton spin Hall effect\u003csup\u003e10\u003c/sup\u003e new physical phenomena. Therefore, in-depth understanding and regulation of interlayer excitons in 2D heterojunctions plays an essential role in various of application of 2D semiconductor devices.\u003c/p\u003e \u003cp\u003eInspired by stacking two graphene at a specific angle to present some unexpected properties, such as superconductor or insulator,\u003csup\u003e11, 12\u003c/sup\u003e the interlayer twist endows a new degree of freedom to flexibly engineer the electronic structures and interlayer excitons.\u003csup\u003e13\u003c/sup\u003e To date, artificially twisted 2D semiconductor heterostructures are mainly focused on transition-metal dichalcogenides (TMDs), which can indirectly form interlayer excitons in two steps, namely, photoexcitation forming intralayer exciton and then the photogenerated electron or hole transfer into the opposite sublayers.\u003csup\u003e7, 14\u0026ndash;19\u003c/sup\u003e It is extremely complex to the formation dynamics and corresponding regulation of the interlayer excitons induced by two-step processes .\u003csup\u003e20\u003c/sup\u003e Since the interlayer photoexcitation probability is two orders of magnitude smaller than that of intralayer excitation in TMDs 2D heterostructures,\u003csup\u003e21\u0026ndash;23\u003c/sup\u003e the formation of interlayer exciton is mainly explored from indirect photoluminescence rather than direct photoabsorption.\u003csup\u003e7\u003c/sup\u003e Simultaneously, although the time scale of transfer process from intralayer to interlayer exciton can be detected by using femtosecond pump-probe spectroscopy and phase-locked electromagnetic pulses,\u003csup\u003e24\u003c/sup\u003e a comprehensive understanding of photogenerated carriers transfer is still very difficult due to the complex momentum-space indirect intervalley transfer, such as Q-Γ, Q-K, K-Γ excitons.\u003csup\u003e17, 25, 26\u003c/sup\u003e It is also unclear whether intralayer photogenerated carriers are transferred into interlayer in the form of free or bound carriers.\u003csup\u003e27, 28\u003c/sup\u003e Therefore, to practical applications of interlayer exciton on specific devices, it is still necessary to increase the understanding of the interlayer exciton formation and regulation.\u003c/p\u003e \u003cp\u003eIn this work, we systematically investigate the formation and regulation of interlayer exciton based on first-principles and nonadiabatic molecular dynamics (NAMD) simulations. The interlayer exciton can be directly formed by interlayer photoexcitation in 2D indium selenide/antimonene (InSe/Sb) heterostructure. The interface atoms of Sb and InSe sublayers contribute the valence band maximum (VBM) and conduction band minimum (CBM) of heterostructure at Γ point, respectively, which forms an interlayer Γ-Γ transition channel due to the strong interlayer coupling and short spatial distance. By uniformly taking seven twist angles in the 0\u0026deg;-60\u0026deg; range, the interlayer twist can directly affect the interlayer interaction and change the electronic structure of band edge. Then, the interlayer exciton's lifetime and peak position can be regulated on a large scale.\u003c/p\u003e"},{"header":"Results and discussion","content":"\u003cp\u003eThe interlayer exciton in TMDs heterostructures is formed in indirect two-step processes; that is, the intralayer exciton is firstly formed in one sublayer, and then the photogenerated electrons transfer into the other sublayer as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ea ① and ② processes. The process has been confirmed by many experimental and theoretical studies.\u003csup\u003e7, 14, 24, 26, 28\u003c/sup\u003e In fact, the formation mode can be clearly illustrated from the geometry and electronic structure of the TMDs. Taking MoS\u003csub\u003e2\u003c/sub\u003e as an example (see Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003eb), monolayer MoS\u003csub\u003e2\u003c/sub\u003e is a sandwich structure with the middle Mo atom layer surrounded by two outer S atomic layers. The intermediate Mo atom layer mainly contributes to valence and conduct band edges. Hence, after forming type II TMDs heterostructures, the direct interlayer photoexcitation at band edges (see Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ea, the ③ process) will be difficult due to the large spatial distance between the two Mo atomic layers. Therefore, interlayer exciton in TMDs heterostructures can only be formed in intralayer excitation and interlayer transfer mechanism.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eTo improve the probability of interlayer photoexcitation at band edges, the band edge components should be mainly composed of interface atoms. This can reduce the photoexcitation spatial distance of carriers. InSe, possessing high electron mobility (10\u003csup\u003e3\u003c/sup\u003e-10\u003csup\u003e4\u003c/sup\u003e cm\u003csup\u003e2\u003c/sup\u003eV\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003es\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e), on/off ratio (~\u0026thinsp;10\u003csup\u003e8\u003c/sup\u003e), quantum Hall effect, and anomalous optical response \u003csup\u003e29, 30\u003c/sup\u003e, has attracted widespread attention in electronic and photoelectric applications. More fortunately, the \u003cem\u003ep\u003c/em\u003e\u003csub\u003ez\u003c/sub\u003e orbital of surface Se atoms mainly contribute to its band edge states (see Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ec). This can reduce the spatial distance of photoexcitation channel after forming a vertical heterojunction with the other 2D semiconductor.\u003c/p\u003e \u003cp\u003e2D Sb semiconductor, a group-VA material, has been successfully prepared by various methods, such as liquid or mechanical exfoliation,\u003csup\u003e31\u0026ndash;33\u003c/sup\u003e vdW epitaxy growth.\u003csup\u003e34\u003c/sup\u003e As a potential 2D photoelectric material, it not only has good photoresponse property\u003csup\u003e33, 35\u003c/sup\u003e, but also possesses high environmental stability. \u003csup\u003e36\u003c/sup\u003e More interesting, Sb is suitable for constructing heterojunction with InSe to explore interlayer excitation (see Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ed). First of all, the VBM of Sb is located at the Γ point (see Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003eg), which is in agreement with the CBM of InSe. Secondly, 2D Sb is a buckled honeycomb structure, and each Sb atom is bonded to three neighboring Sb atoms. Then, the nonbonding lone pair electrons are left at the surface, which can increase the interlayer coupling after forming a vertical heterojunction. And lastly, the lattice constants of Sb (4.12 \u0026Aring;) and InSe (4.07 \u0026Aring;) are very well matched with each other. Then, by adjusting the twist angles (see Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ee), the interlayer interaction can be periodically regulated, and the superlattice pattern can appear simultaneously. Therefore, the InSe/Sb heterojunction will be a suitable system to explore the direct formation of interlayer excitons and the interlayer twist regulation of interlayer excitons.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eWe define a highly symmetrical structure as the 0\u0026deg; twist angle structure as shown in Figure \u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003e. The Sb and Se atoms at the interface of heterostructure are staggered arrangement forming strong interlayer coupling. Since 2D InSe and Sb are hexagonal lattice, after twisting 60\u0026deg; for one sublayer, the heterostructure can form a new highly symmetrical structure. Therefore, we evenly take seven twist angles from 0\u0026deg; to 60\u0026deg; (that is, 0.0\u0026deg;, 10.9\u0026deg;, 19.1\u0026deg;, 30.0\u0026deg;, 40.9\u0026deg;, 49.1\u0026deg; and 60.0\u0026deg;, see Figure \u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003e-S8) to investigate the formation and regulation of interlayer exciton in InSe/Sb heterostructure. According to the previously widely studied twist stacking preparation strategy for 2D materials, such as graphene, hexagonal boron nitride, TMDs, the InSe/Sb heterostructures with different twist angles have the opportunity to be prepared by using the stamping dry-transfer method.\u003csup\u003e19, 37, 38\u003c/sup\u003e\u003c/p\u003e \u003cp\u003eAs expected, InSe/Sb heterostructure is a type II heterojunction (see Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ea). The VBM and CBM are located at Γ point, which are contributed by Sb and InSe sublayers, respectively. The band gap of InSe/Sb heterostructure can be significantly adjusted from 0.63 to 0.91 eV by the different twist angles (see Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ea-\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eg). As presented in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eh, the highly symmetrical structures possess stronger binding energy (around \u0026minus;\u0026thinsp;45 meV per atom) than asymmetric structures (around \u0026minus;\u0026thinsp;35 meV per atom). It's worth noting that even for asymmetric structures, the interlayer interactions are much stronger than typical 2D vdW interaction, such as bilayer MoS\u003csub\u003e2\u003c/sub\u003e or graphene/MoS\u003csub\u003e2\u003c/sub\u003e heterojunctions (around \u0026minus;\u0026thinsp;20 meV per atom). The strong interlayer interaction of InSe/Sb heterostructure will facilitate direct interlayer photoexcitation.\u003c/p\u003e \u003cp\u003eAs exhibited in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ei, the photoexcitation threshold of the InSe/Sb heterostructures (around 0.6 -1.0 eV) is obviously smaller than that of isolated 2D InSe and Sb layers (larger than 1.5 eV). That is, the intralayer photoexcitation cannot contribute to the first photoabsorption peak of InSe/Sb heterostructures. Simultaneously, the electronic band gap of these heterostructures is also in the range from ~\u0026thinsp;0.6 to ~\u0026thinsp;1.0 eV. Therefore, the first photoabsorption peak should derive from the direct interlayer photoexcitation at band edges of heterostructures. Specifically, for the interlayer photoexcitation at around Γ point, the square of the transition dipole moments (\u003cem\u003eP\u003c/em\u003e\u003csup\u003e2\u003c/sup\u003e: see Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ej). reaches up to ~\u0026thinsp;300\u0026ndash;500 Debye\u003csup\u003e2\u003c/sup\u003e, which has similar transition strength with the intralayer photoexcitation of isolated 2D InSe and Sb layers. Therefore, the direct interlayer bright photoexcitation can occur in InSe/Sb heterostructures. Note that, for InSe/Sb heterostructure with 0.0\u0026deg;, 10.9\u0026deg;, 30.0\u0026deg;, 49.1\u0026deg; and 60.0\u0026deg; twist angles, the first photoexcitation is bright excitation from VBM to CBM. For InSe/Sb heterostructure with 19.1\u0026deg; and 40.9\u0026deg; twist angles, the first bright excitation arises from the transition channel from VBM-4 to CBM, and VBM-3 to CBM, respectively. Therefore, the bandgap value is smaller than the first peak position for InSe/Sb heterostructure with 19.1\u0026deg; and 40.9\u0026deg; twist angles. For the calculation of transition dipole moment, we use the sum of transition between the first four valence bands and one conduction band for InSe/Sb heterostructure with 19.1\u0026deg; and 40.9\u0026deg; twist angles,\u003c/p\u003e \u003cp\u003eThe interlayer twist can shift the peak position up to ~\u0026thinsp;400 meV. In previous researches, the shifted range of the first photoluminescence peak is ~\u0026thinsp;60 meV in twisted MoSe\u003csub\u003e2\u003c/sub\u003e/WS\u003csub\u003e2\u003c/sub\u003e heterostructure,)\u003csup\u003e16\u003c/sup\u003e, ~ 90 meV in MoS\u003csub\u003e2\u003c/sub\u003e/WSe\u003csub\u003e2\u003c/sub\u003e heterostructure\u003csup\u003e39\u003c/sup\u003e and ~\u0026thinsp;100 meV in WS\u003csub\u003e2\u003c/sub\u003e bilayer\u003csup\u003e38\u003c/sup\u003e. Interesting, for InSe/Sb heterostructure, MoSe\u003csub\u003e2\u003c/sub\u003e/WS\u003csub\u003e2\u003c/sub\u003e heterostructure and WS\u003csub\u003e2\u003c/sub\u003e bilayer, although their shifted range of the first peak varies widely, the trend is consistent with each other. That is, for the highly symmetrical interlayer stacking heterostructure with twist angle near 0\u0026deg; or 60\u0026deg;, the energy of peak is small, while for the low symmetrical interlayer stacking heterostructures, the energy of peak is gradually increasing. the highly symmetrical interlayer stacking mode increases interlayer interaction and promotes the wavefunction coupling of band edge electronic states. this can be further confirmed by the transition probability between band edges (seeing Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ej). for highly symmetrical interlayer stacking heterostructures (0\u0026deg; and 60\u0026deg;), the Γ-Γ interlayer photoexcitation possesses a larger transition probability (\u003cem\u003eP\u003c/em\u003e\u003csup\u003e2\u003c/sup\u003e: \u0026gt;500 Debye\u003csup\u003e2\u003c/sup\u003e) compared with that of other heterostructures (\u003cem\u003eP\u003c/em\u003e\u003csup\u003e2\u003c/sup\u003e: 300\u0026ndash;400 Debye\u003csup\u003e2\u003c/sup\u003e) .\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eAs presented in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ea, after forming heterojunction, the InSe and Sb sublayer all contribute electrons to the interface central region, which is different common phenomenon of charge transfer from one sublayer to the other.\u003csup\u003e40, 41\u003c/sup\u003e Then, the stacked charge wavefunction distribution in the interface region can provide a buffer to increase the wavefunction overlap of interlayer transition channel, thereby in turn enhancing the transition probability of direct interlayer excitation.\u003c/p\u003e \u003cp\u003eThe interlayer twist obviously changes the distribution of charge density difference. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e and S9-S15, for the highly symmetrical interlayer stacking heterostructures with 0\u0026deg; and 60\u0026deg; twist angles, there accumulates more charges at interface central region compared with that of the low symmetrical modes. This further indicates that the interlayer excitation of the highly symmetrical stacked structures has a greater transition probability, consistent with the result of the transition dipole moment in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ej. Since the lattice parameter of InSe and Sb sublayer is similar to each other, for the low symmetrical modes, these heterostructures form a superlattice pattern (see Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e). According to the different superlattice patterns of sectional charge distribution, the various interlayer twist angles indeed bring about different regulatory effects for electronic structure and interlayer photoexcitation properties.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eAfter interlayer photoexcitation, the photogenerated electron and hole are localized in InSe and Sb sublayer, respectively. The lifetime of photogenerated carriers plays an essential role in various applications, such as optoelectronics, photovoltaics, and sensors. We perform the NAMD simulation by initiating the photogenerated electron at the conduction band edge of heterojunction (see Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eb-\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eh). After the photogenerated electron recombines with the hole located in the valance band edge, the time interval is defined as the lifetime of photogenerated carriers.\u003c/p\u003e \u003cp\u003eFor the InSe/Sb heterojunctions with different twist angles, we find that only less than 6% of photogenerated carriers recombine in 5 ns simulating time (see Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ea). Although the precise lifetime is hard to obtain based on the current simulation period, we can estimate the timescale by fitting an exponential function: P(t)\u0026thinsp;=\u0026thinsp;exp(-t/τ). As presented in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eb-\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eh, for different twist angle structures, the lifetime of photogenerated carriers is as high as 96.2 to 1181.9 ns. That is, the interlayer exciton can be adjusted over a wide range by interlayer twist.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eGenerally, the photogenerated carrier hopping probability between two electronic states inversely depends on the square of nonadiabatic coupling (NAC) based on Fermi's golden rule. As exhibited in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ea, the largest value of NAC is less than 2.5 meV for all InSe/Sb heterojunctions with different twist angles. Such a small NAC value ensures the long-lived photogenerated carrier lifetimes. Moreover, compared with the highly symmetrical structures, the low symmetrical structures generally have a smaller NAC coefficient. To facilitate comparison, we present the averaged absolute value of NAC between the adjacent 10 band edge states in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eb-\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eh. The InSe/Sb heterojunction with 60\u0026deg; (40\u0026deg;) twist angle possesses the largest (smallest) NAC coefficient between VBM and CBM electronic states, which is in agreement with the longest (shortest) lifetime of InSe/Sb heterojunctions. That is, the interlayer twist has a strong regulatory effect on the photogenerated carrier lifetime. Simultaneously, the average NAC between other neighboring states is larger than that of VBM and CBM. This also facilitates the other photogenerated carriers transferring into the VBM and CBM band edge states, forming the Γ-Γ interlayer exciton.\u003c/p\u003e \u003cp\u003eThe NAC element is dependent on the energy gap difference of hopping channel (\u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\({\\epsilon }_{k}-{\\epsilon }_{j}\\)\u003c/span\u003e\u003c/span\u003e), the electron-phonon coupling (\u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(\\langle {\\phi _j}|{\\nabla _R}H|{\\phi _k}\\rangle\\)\u003c/span\u003e\u003c/span\u003e) and nuclear velocity (\u003cem\u003eṘ\u003c/em\u003e\u003csub\u003e\u003cem\u003eI\u003c/em\u003e\u003c/sub\u003e) describing as follows:\u003c/p\u003e \u003cp\u003e \u003cspan class=\"InlineEquation\"\u003e \u003cspan class=\"mathinline\"\u003e\\({d_{jk}}=\\langle {\\phi _j}|\\frac{\\partial }{{\\partial t}}|{\\phi _k}\\rangle =\\sum\\limits_{I} {\\frac{{\\langle {\\phi _j}|{\\nabla _R}H|{\\phi _k}\\rangle }}{{{\\varepsilon _k} - {\\varepsilon _j}}}\\mathop {{R_I}}\\limits^{ \\bullet } }\\)\u003c/span\u003e \u003c/span\u003e \u003c/p\u003e \u003cp\u003eWhere H is the Kohn-Sham Hamiltonian,\u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\({\\phi _k}\\)\u003c/span\u003e\u003c/span\u003e,\u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\({\\phi _j}\\)\u003c/span\u003e\u003c/span\u003e,\u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\({\\epsilon }_{j}\\)\u003c/span\u003e\u003c/span\u003e,\u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\({\\epsilon }_{k}\\)\u003c/span\u003e\u003c/span\u003e are the wave-functions and corresponding eigenvalues for j and k electronic states, respectively, and \u003cem\u003eṘ\u003c/em\u003e\u003csub\u003e\u003cem\u003eI\u003c/em\u003e\u003c/sub\u003e is velocity of the nuclei. For InSe/Sb heterojunctions with different twist angles, since the elements and the temperature are the same with each other, the difference in NAC should derive from the energy gap difference and electron-phonon coupling term.\u003c/p\u003e \u003cp\u003eAs discussed above, the band gap of InSe/Sb heterojunctions can be gradually adjusted from 0.63 to 0.91 eV with the change of twist angle. That is, the small energy gap difference will increase the carrier hopping probability, which is consistent with the trend of photo-generated carrier lifetime with the change of twist angle.\u003c/p\u003e \u003cp\u003eFor the electron-phonon coupling term, its strength can be reflected by the energy fluctuation of involved electronic states. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eb-\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eh, the fluctuation of VBM with the time evolution is stronger than that of CBM. Hence, the vibration of Sb sublayer will play a more critical role in lifetime. To visualize the phonon modes dominating the fluctuation, the Fourier transforms (FT) of the autocorrelation functions are calculated to the time-dependent evolution of the band edges energy difference (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ei). For all InSe/Sb heterojunctions, the vibrational peaks are mainly concentrated around 50 and 200 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, attributed to the interlayer breathing mode, \u003cem\u003eA\u003c/em\u003e\u003csub\u003e1g\u003c/sub\u003e mode of InSe\u003csup\u003e42\u003c/sup\u003e and Sb \u003csup\u003e34\u003c/sup\u003esublayer, respectively. Clearly, the phonon spectral density changes from high to low as the different twist angle structures from high to low symmetric stacking mode. This is also consistent with the trend of photogenerated carrier lifetime.\u003c/p\u003e \u003cp\u003eMoreover, the pure-dephasing time between initial and final electronic states, similar to Huang-Rhys factor and Frank-Condon factor, is also associated with the lifetime of nonradiative recombination. The fast loss of quantum coherence can suppress the hopping rate. As presented in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ej, for all InSe/Sb heterojunctions, the range of pure dephasing time is from 10 to 27 fs by Gaussian fitting, exp(-0.5(t/τ)). This is obviously smaller than that of MoS\u003csub\u003e2\u003c/sub\u003e/WS\u003csub\u003e2\u003c/sub\u003e heterojunctions with different twist angles from 37 to 58 fs.\u003csup\u003e18\u003c/sup\u003e Hence, the small pure dephasing time also contributes to the long lifetime of photogenerated carriers for InSe/Sb heterojunctions.\u003c/p\u003e \u003cp\u003eFor 2D materials, the excitonic effect is of significance due to the enhanced Coulomb interactions. Unfortunately, for InSe/Sb heterojunctions with various twist angles, it is not yet feasible because of excessive computational expense associated with NAMD involving thousands of electronic structure calculations. Although the single-particle picture cannot accurately obtain the lifetime of photogenerated electron and hole recombination, the change trends of lifetime should be reliable as the twist angle changes. In previous researches, Zhu et al. have studied the effect of twist angle on the photogenerated electron and hole recombination in MoS\u003csub\u003e2\u003c/sub\u003e/WS\u003csub\u003e2\u003c/sub\u003e heterostructure and WS\u003csub\u003e2\u003c/sub\u003e bilayer\u003csup\u003e17\u003c/sup\u003e based on single-particle picture. They found that the larger bandgaps or smaller nonadiabatic couplings make the slower electron and hole recombination in twisted than high-symmetry structures. The trend of their results is consistent with the experiments\u003csup\u003e19, 38\u003c/sup\u003e.\u003c/p\u003e"},{"header":"Conclusions","content":"\u003cp\u003eCombining fist-principles and nonadiabatic molecular dynamics simulations, we find that the InSe/Sb heterojunction can form interlayer excitons in one-step interlayer photoexcitation, and the photo-response range and lifetime can be significantly modulated by interlayer twist. the interlayer twist can periodically regulate the interlayer coupling. Then, the band edge states, contributed by interface atoms, can be directly affected by different twist angles. This induces the large range of regulation for the interlayer excitation peak and photogenerated carrier lifetime. This study enriches the understanding and engineering the interlayer exciton in artificial 2D vdW heterostructure materials.\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e\u003cstrong\u003eAuthor contributions\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eX. N. and A. S. conceived the project. A. S., R. G. and Z. N carried out DFT and NAMD calculations. W. Z., X. Z., and S. W. carried out\u0026nbsp;twist\u0026nbsp;model constructing and DFT calculations. A. S., X. N., J. L. and B. W. co-wrote the paper with all authors contributing to the discussion and preparation of the manuscript.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAcknowledgements\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThis work is supported by China Postdoctoral Science Foundation (Grant No. 2022M711691), National Natural Science Foundation of China (Grant No. 12104130), Natural Science Foundation of Shanxi province (Grant No. 20210302123336), Six talent peaks project in Jiangsu Province (Grant No. XCL-104), Jiangsu Innovation Projects for Graduate Student (Grant Nos. KYCX22_0901, KYCX22_0991) and NUPTSF (Grant No. NY221102).\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eConflicts of interest\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe authors declare no competing financial interests.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\n\u003cli\u003eSu, T.; Shao, Q.; Qin, Z.; Guo, Z.; Wu, Z., Role of Interfaces in Two-Dimensional Photocatalyst for Water Splitting. \u003cem\u003eACS Catal. \u003c/em\u003e\u003cstrong\u003e2018,\u003c/strong\u003e \u003cem\u003e8\u003c/em\u003e, 2253-2276.\u003c/li\u003e\n\u003cli\u003eLiu, Y.; Duan, X.; Huang, Y.; Duan, X., Two-Dimensional Transistors Beyond Graphene and Tmdcs. \u003cem\u003eChem. Soc. Rev. \u003c/em\u003e\u003cstrong\u003e2018,\u003c/strong\u003e \u003cem\u003e47\u003c/em\u003e, 6388-6409.\u003c/li\u003e\n\u003cli\u003eFrisenda, R.; Navarro-Moratalla, E.; Gant, P.; Perez De Lara, D.; Jarillo-Herrero, P.; Gorbachev, R. 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Mater. \u003c/em\u003e\u003cstrong\u003e2021,\u003c/strong\u003e \u003cem\u003e31\u003c/em\u003e, 2104143.\u003c/li\u003e\n\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"npj-computational-materials","isNatureJournal":false,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"npjcompumats","sideBox":"Learn more about [npj Computational Materials](http://www.nature.com/npjcompumats/)","snPcode":"41524","submissionUrl":"https://mts-npjcompumats.nature.com/","title":"npj Computational Materials","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"ejp","reportingPortfolio":"NPJ","inReviewEnabled":true,"inReviewRevisionsEnabled":true},"keywords":"interlayer exciton, vdW heterostructure, twist angle, first-principles, excited state dynamics","lastPublishedDoi":"10.21203/rs.3.rs-4161258/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-4161258/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eThe interlayer twist angle endows a new degree of freedom to manipulate the spatially separated interlayer excitons in van der Waals (vdWs) heterostructures. Herein, we find that the band-edge Γ-Γ interlayer excitation directly forms interlayer exciton in InSe/Sb heterostructure, different from that of transition metal dichalcogenides (TMDs) heterostructures in two-step processes by intralayer excitation and transfer. By tuning the interlayer coupling and breathing vibrational modes associated with the Γ-Γ photoexcitation, the interlayer twist can significantly adjust the excitation peak position and lifetime of recombination. The interlayer excitation peak in InSe/Sb heterostructure can shift\u0026thinsp;~\u0026thinsp;400 meV, and the interlayer exciton lifetime varies in hundreds of nanoseconds as a periodic function of the twist angle (0\u0026deg;-60\u0026deg;). This work enriches the understanding of interlayer exciton formation and facilitates the artificial excitonic engineering of vdWs heterostructures.\u003c/p\u003e","manuscriptTitle":"The interlayer twist effectively regulates interlayer excitons in InSe/Sb van der Waals heterostructure","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2024-04-30 02:54:57","doi":"10.21203/rs.3.rs-4161258/v1","editorialEvents":[{"type":"communityComments","content":0},{"type":"decision","content":"revise","date":"2024-06-10T05:42:45+00:00","index":"","fulltext":""},{"type":"editorInvitedReview","content":"This content is not available.","date":"2024-06-08T15:11:54+00:00","index":2,"fulltext":"This content is not available."},{"type":"editorInvitedReview","content":"This content is not available.","date":"2024-05-24T00:25:40+00:00","index":1,"fulltext":"This content is not available."},{"type":"reviewerAgreed","content":"This content is not available.","date":"2024-05-14T08:19:05+00:00","index":2,"fulltext":"This content is not available."},{"type":"reviewerAgreed","content":"This content is not available.","date":"2024-04-25T12:05:32+00:00","index":1,"fulltext":"This content is not available."},{"type":"reviewersInvited","content":"","date":"2024-04-24T19:49:12+00:00","index":"","fulltext":""},{"type":"checksComplete","content":"","date":"2024-03-27T10:11:19+00:00","index":"","fulltext":""},{"type":"editorAssigned","content":"","date":"2024-03-25T07:00:03+00:00","index":"","fulltext":""},{"type":"submitted","content":"npj Computational Materials","date":"2024-03-25T07:00:02+00:00","index":"","fulltext":""}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"npj-computational-materials","isNatureJournal":false,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"npjcompumats","sideBox":"Learn more about [npj Computational Materials](http://www.nature.com/npjcompumats/)","snPcode":"41524","submissionUrl":"https://mts-npjcompumats.nature.com/","title":"npj Computational Materials","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"ejp","reportingPortfolio":"NPJ","inReviewEnabled":true,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"21a3d771-699c-47c7-b11d-b0c400b48bc1","owner":[],"postedDate":"April 30th, 2024","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"published-in-journal","subjectAreas":[{"id":31120543,"name":"Physical sciences/Materials science/Nanoscale materials/Two-dimensional materials"},{"id":31120544,"name":"Physical sciences/Materials science/Nanoscale materials/Electronic properties and materials"}],"tags":[],"updatedAt":"2024-08-27T07:24:44+00:00","versionOfRecord":{"articleIdentity":"rs-4161258","link":"https://doi.org/10.1038/s41524-024-01384-6","journal":{"identity":"npj-computational-materials","isVorOnly":false,"title":"npj Computational Materials"},"publishedOn":"2024-08-26 04:00:00","publishedOnDateReadable":"August 26th, 2024"},"versionCreatedAt":"2024-04-30 02:54:57","video":"","vorDoi":"10.1038/s41524-024-01384-6","vorDoiUrl":"https://doi.org/10.1038/s41524-024-01384-6","workflowStages":[]},"version":"v1","identity":"rs-4161258","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-4161258","identity":"rs-4161258","version":["v1"]},"buildId":"qtupq5eGEP_6zYnWcrvyt","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}