Pressure-Stabilized MnSb2 with Complex Incommensurate Magnetic Order

Pressure-Stabilized MnSb2 with Complex Incommensurate Magnetic Order | 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 Pressure-Stabilized MnSb 2 with Complex Incommensurate Magnetic Order Mingyu Xu, Matt Boswell, Danielle Yahne, Qing-Ping Ding, Peng Cheng, and 7 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-8980468/v1 This work is licensed under a CC BY 4.0 License Status: Under Review Version 1 posted 10 You are reading this latest preprint version Abstract Marcasite-type compounds have been proposed as promising hosts of exotic magnetic quantum states, yet experimental realizations in stoichiometric, disorder-free systems remain limited. Here, we report the high-pressure stabilization and magnetic characterization of MnSb 2 , a marcasite-type compound that is thermodynamically metastable under ambient pressure. Single crystals were synthesized using a cubic multi-anvil press, and powder and single-crystal X-ray diffraction confirm the orthorhombic Pnnm structure. These crystals are stable at ambient pressure for a long time up to between 450–500 K. Heat-capacity measurements reveal phase transitions at approximately 220 K and 118 K. Neutron diffraction uncovers an unconventional magnetic ground state below 220 K. Magnetic powder neutron diffraction refinements reveal possible multiple magnetic configurations that provide comparably acceptable fits to the experimental data. While most solutions are consistent with a spin-density-wave (SDW) description, helical models systematically yield inferior agreement factors. Across a broad range of models, the Mn ordered moment reaches a maximum value of approximately 2 µ B and remains predominantly collinear, with minimal canting along the c -axis. At 200 K, the magnetic propagation vector is q = (0, 0.3975, 0.3783); upon cooling, the b component increases toward 0.5, reflecting a temperature-dependent evolution of the modulation. The need for modification of the magnetic model between high and low temperatures further highlights the complex and strongly temperature-dependent nature of the magnetic order in this system. These results establish MnSb 2 as a pressure-stabilized marcasite magnet with a highly tunable, complex magnetic ground state and a compelling stoichiometric platform for exploring unconventional magnetic behavior, including potential altermagnetism. Physical sciences/Materials science Physical sciences/Physics Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Introduction When magnetism intertwines with band topology in quantum materials, it can, in some cases, give rise to a recently identified class of magnetic systems characterized by collinear spin arrangements with zero net magnetization, exhibiting time-reversal-symmetry-breaking responses 1 – 8 and spin-split electronic band structures 9 – 16 . These properties, referred to as altermagnetism, combine zero-net-moment magnetic order with symmetry-allowed spin splitting relevant for spintronic applications and have motivated intense theoretical and experimental interest in identifying chemically clean material platforms that realize this magnetic phase 8 , 17 – 31 . Marcasite-type compounds, in particular, have emerged as promising candidates due to their low crystal symmetry and symmetry-allowed spin splitting in antiferromagnetic states. FeSb 2 is a narrow-gap, strongly correlated semiconductor 32 – 36 that has been theoretically predicted to host a collinear altermagnetic state upon Co substitution or hole doping 37 . Experimentally, however, FeSb 2 exhibits no long-range magnetic order between 1.8 and 300 K. Stabilizing magnetic order in FeSb 2 therefore requires deliberate tuning of its electronic structure. While chemical substitution and external pressure are widely used to modify band filling and band width, substitution often introduces chemical disorder that complicates interpretation, and pressure-dependent magnetic measurements are experimentally nontrivial, especially for antiferromagnetism. This all motivates the search for chemically clean routes to stabilize magnetic order in the FeSb 2 structure class. A promising route to this goal is provided by MnSb 2 , a high-pressure marcasite-type compound that shares the same orthorhombic structure as FeSb 2 but incorporates Mn with a larger, and often more robust, local magnetic moment and intrinsic hole doping 38 (relative to FeSb 2 ). Whereas MnSb 2 does not form at ambient pressure, it can be synthesized under high-pressure conditions and quenched into a metastable form at ambient pressure 39 . Across the marcasite family, CrSb 2 exhibits robust antiferromagnetic order with a Néel temperature near 273 K 40 , whereas FeSb₂ remains nonmagnetic, suggesting that magnetic order emerges through band filling by hole doping. By analogy, MnSb₂ represents a chemically ordered, stoichiometric platform in which unconventional states may be realized. Results and Discussion MnSb 2 was synthesized at 3.3 GPa pressure and 490 °C using a Rockland Research cubic multi-anvil press. After maintaining this temperature for 24 hours, a high-quality MnSb 2 product, with more than half of the final material consisting of sub-millimeter-sized MnSb 2 single crystals that can be easily separated mechanically from the surrounding MnSb 2 polycrystalline matrix, was obtained. (See the Experimental Method section for further details.) The single-crystal X-ray diffraction (SCXRD) analysis of MnSb 2 , summarized in Tables S1 and S2 , illustrates the crystal structure of MnSb 2 shown in the right inset of Fig. 1 , which adopts the orthorhombic Pnnm space group and features edge-sharing MnSb 6 octahedra. The unit cell contains two crystallographically distinct atomic sites: Mn atoms occupy the 2 a Wyckoff position, while Sb atoms reside at the 4 g positions. Vacancies and site mixing were considered during the refinement, but no structural disorder or clear vacancies were detected. To assess the phase purity of samples synthesized under high-pressure conditions, powder X-ray diffraction (PXRD) measurements were performed using a bulk sample with single crystals in the polycrystalline matrix, as shown in Fig. 1 . The experimental data (red circles) were analyzed by Rietveld refinement (black line) using the GSAS-II software package 41 , and the difference between the observed and calculated patterns is shown by the blue line. The minor phase of elemental Sb is observed. The PXRD results are consistent with single-crystal X-ray diffraction measurements and with the previous report. 39 The left inset of Fig. 1 shows representative as-grown crystals, which display metallic luster and well-defined faceted morphologies, consistent with high crystallinity. To determine the thermal stability range of MnSb 2 at ambient pressure, temperature-dependent magnetization measurements were performed under both field-warming (FW) and field-cooling (FC) conditions, as shown in Fig. 2 a . Below 450 K, the magnetization curves exhibit no significant difference between the FW and FC protocols, indicating thermal and magnetic stability within this temperature range. However, above 450 K, a pronounced increase in magnetic moment is observed, suggesting the onset of decomposition and the formation of Mn 1.1 Sb, a known ferromagnetic impurity phase. This observation is corroborated by powder X-ray diffraction data collected before and after the magnetization measurements. As shown in Fig. 2 b , additional reflections corresponding to Mn 1.1 Sb emerge, and the intensity of the Sb peak increases significantly after heating above 500 K, confirming the partial decomposition of MnSb 2 . These results indicate that while MnSb 2 is metastable at ambient pressure, it remains structurally and magnetically stable at temperatures up to ~450 K, enabling long-term low-temperature studies without phase transformation. Moreover, within the temperature range of 1.8 K to 300 K, magnetization measurements (see Fig. 5 ) show no signatures of ferromagnetic or other phase transitions in MnSb 2 . The field-dependent magnetization displays predominant paramagnetic behavior with minor ferromagnetic contributions attributable to trace Mn 1.1 Sb impurities. Collectively, these results confirm that MnSb 2 is suitable for extended investigations at low temperatures under ambient conditions, without undergoing structural or magnetic phase transitions. To probe the magnetic and electronic properties of MnSb 2 , temperature-dependent electrical resistance measurements were performed on single-crystalline samples upon cooling from 300 K to 1.8 K and during subsequent warming, as shown in Fig. 3 a . The resistance curves from the cooling and warming cycles overlap closely, indicating negligible thermal hysteresis. The residual resistance ratio (RRR), defined as R(300K)/R(1.8K), is approximately 60. The inset of Fig. 3 a displays the temperature derivative of the resistance (d R /d T ). There are two clear breaks in slope visible in the raw data and two broad steps in d R /d T around 125 K and 220 K, as indicated with the arrows in Fig. 3 a and the inset. Complementary thermodynamic information is provided by temperature-dependent specific heat measurements on polycrystalline MnSb 2 performed at zero magnetic field. As shown in Fig. 3 b , three reproducible anomalies are observed at approximately 118 K ( T 0 ), 219 K ( T ₁), and 231 K ( T ₂). These features are independently confirmed using an alternative measurement protocol over a different temperature range. Notably, the application of a magnetic field of 90 kOe produces negligible changes in specific heat ( Fig. S3 a ), demonstrating that the transition is largely insensitive to external magnetic fields. Integration of the excess specific heat yields a total magnetic entropy change of approximately ( Fig. S3 b ) using the reference of FeSb 2 specific heat, which is close to the Mn high-spin state. Curiously, the weak field dependence of the upper specific heat feature might suggest an antiferromagnetic transition that couples only weakly to uniform magnetic fields. To assess the uniform magnetic response of MnSb 2 and the presence of any net magnetic moment, magnetic susceptibility and field-dependent magnetization measurements were performed. Fig. 3 a shows the field-dependent magnetization of polycrystalline MnSb 2 measured up to 70 kOe at selected temperatures. The magnetization exhibits only weak temperature dependence, remains unsaturated over the entire field range, and displays a very small net moment. A weak ferromagnetic contribution is observed and attributed to trace amounts (<1%) of the Mn 1.1 Sb impurity, which is below the detection limit of X-ray diffraction but was detected by NMR measurements ( Fig. S5 ). The inset shows representative M ( H ) curves measured at 300 K in five quadrants, confirming the absence of intrinsic ferromagnetic hysteresis. Fig. 3 b presents the temperature-dependent magnetization of polycrystalline MnSb 2 measured under a 10 kOe applied field. There are two anomalies between 2 K and 300 K, T 0 = 122 K and T ’ 1 = 226 K, indicated by the black arrows. This observation is consistent with electric transport and the heat-capacity measurements. The inset displays the temperature derivative of MT , which shows two anomalies. This behavior is consistent with an amplitude-modulated antiferromagnetic ground state and highlights the limited sensitivity of uniform magnetization measurements to this type of magnetic order as well as a relatively large contribution to M ( T ) from a ferromagnetic impurity. To elucidate the microscopic origin of this magnetic transition, we next turn to neutron scattering measurements, which directly probe the magnetic ordering wave vector and spatial distribution of the ordered moments. Powder neutron diffraction measurements on MnSb 2 were carried out between 308 K and 4 K ( Fig. 4 ). Upon cooling below ~200 K, well below the ~220 K upper magnetic transitions, additional Bragg reflections (shown in the red arrows) of magnetic origin emerge ( Fig. 4 a ). Similar magnetic peaks are found at 150 K and new peaks (shown in the black arrows) at 100K and 4 K, temperatures below the lower magnetic transition. Refinements of diffraction patterns collected above ( Figs. 4 b ) and below ( Fig. 4 c ) the show that orthorhombic MnSb 2 develops a complex magnetic ground state that evolves with temperature. Two irreducible representations can be utilized to analyze the structure that is related by symmetry. The magnetic powder refinement allows many magnetic structures to fit reasonably well. Although most structures are aligned with a spin density wave formation, trying a helical magnetic structure overall results in a lower quality of fit. The multiple models that can describe this system make it challenging to determine the direction of the spin density wave specifically and require polarized neutrons to better understand the structure. However, in many models, the Mn moment reaches a maximum of 2 μ B and tends to be collinear with little orientation along the c- axis. The propagation vector q is (0, 0.3975, 0.3783) at 200 K, and the b component of the propagation vector increases as temperature decreases, and the value approaches 0.5. With the changing temperature, the modulation of the spin wave changes and typically requires changing the model from high to low temperatures, further highlighting the complexity of the magnetic order within the system. The magnetic ground state of orthorhombic MnSb 2 is fundamentally distinct from both conventional helical magnets and simple spin-density-wave (SDW) systems. Importantly, the strictly collinear antiferromagnetic order with zero net magnetization, combined with sublattice-dependent anisotropy and broken spin degeneracy at finite wave vector, places MnSb 2 in close proximity to the emerging class of altermagnetic materials. To evaluate the magnetic ground state of MnSb 2 , first-principles calculations were performed using the experimentally determined single-crystal structure, considering non-magnetic (NM), ferromagnetic (FM), and a simple collinear antiferromagnetic (AFM) configurations with antiparallel Mn moments in the primitive cell. Although neutron diffraction reveals a considerably more complex magnetic structure, calculations with a simple collinear AFM configuration provide a useful reference for evaluating the magnetic instability of the electronic structure. In addition, the limited experimental constraints on the full magnetic structure from unpolarized neutron diffraction and the computational cost of large magnetic supercells make such simplified calculations a practical first step. The calculated total energies ( Table S3 ) show that the AFM state is the most stable, lying 80.79 meV below the NM configuration, while the FM state is also energetically favored (69.68 meV below NM), indicating close energetic competition among magnetic states. In the AFM configuration, the calculated local magnetic moment on Mn is 2.81 μ B . The calculated electronic band structures are shown in Fig. 5 . In the NM state ( Fig. 5 a ), a flat band appears near the Fermi level, producing a pronounced peak in the density of states and signaling electronic instability. Although MnSb 2 shares the same nominal valence electron count as FeSb 2 , the partial occupation of states at the Fermi level confirms metallic behavior rather than the insulating ground state of FeSb 2 . Upon inclusion of spin polarization in the AFM state ( Fig. 5 b ), the flat band shifts below the Fermi level, and the density of states at the Fermi level is strongly reduced, leading to the formation of a pseudogap and a more stable electronic structure. Importantly, the AFM state breaks time-reversal symmetry while preserving a net zero magnetization, a symmetry condition that can allow momentum-dependent spin splitting of electronic bands in low-symmetry crystals. This symmetry condition is consistent with the collinear, finite- antiferromagnetic order and orthogonal sublattice anisotropy resolved by neutron diffraction, although a detailed analysis of altermagnetic band splitting is beyond the scope of the present calculations. Together, these results indicate that MnSb 2 satisfies the essential energetic and symmetrical prerequisites for altermagnetic behavior, motivating future momentum-resolved experimental and theoretical studies. In summary, altermagnets have recently emerged as a distinct class of magnetic materials that combine collinear antiferromagnetic order with spin-split electronic band structures and zero net magnetization, offering new opportunities for quantum and spintronic functionalities. In this work, we establish MnSb 2 as a chemically clean, pressure-stabilized marcasite-type compound hosting an unconventional magnetic ground state. Using high-pressure synthesis, thermodynamic measurements, neutron diffraction, and first-principles calculations, we show that MnSb 2 does not develop a single, rigid magnetic order below a well-defined T N . Instead, magnetic entropy begins to be released near ~230 K, accompanied by the appearance of incommensurate magnetic Bragg reflections below ~ 200 K. A second thermodynamic anomaly near ~ 118 K coincides with the emergence of additional magnetic peaks, indicating a reconstruction of the ordered state. Remarkably, specific heat and neutron refinements reveal that the magnetic structure continues to evolve throughout the ordered regime: the propagation vector shifts systematically with temperature (with the b -component trending toward 0.5). The relating ground state is described as a complex SDW with the available data do not uniquely determine the modulation direction, and polarized neutron experiments will be required for definitive resolution. These findings establish MnSb 2 as a rare stoichiometric platform in which an incommensurate SDW remains highly tunable at low temperature, highlighting an unusual interplay between anisotropy, competing exchange interactions, and the underlying electronic structure. Experimental Methods High-Pressure Synthesis: MnSb 2 was synthesized using a two-step method, which is different from the reference 39 (lower pressure and temperature used in this experiment), involving (i) the preparation of a finely mixed Mn–Sb precursor and (ii) a subsequent high-pressure, high-temperature reaction. In the first step, manganese metal (CZ-1-110) and antimony shot (99.999%) were combined in a 1:2 molar ratio and loaded into a 1.7 mL fritted alumina Canfield Crucible Set (CCS, LSP Industrial Ceramics, Inc.). 42 The crucible was sealed in a silica ampoule under an argon atmosphere (~1/3 atm). Silica wool was packed above and below the CCS to stabilize the crucible during centrifugation and to contain any escaped liquid. The ampoule was heated in a box furnace to 760 °C over two hours, held at this temperature for 10 hours, and then rapidly centrifuged to separate the molten and non-molten phases. The solid residue retained on the frit disc appeared as a black solid, likely a minor oxide crust, while the solidified, decanted melt was collected, ground into a fine powder, and pressed into a pellet using a die press. In the second step, the pellet was loaded into a boron nitride (BN) crucible (7 mm length, 5.7 mm inner diameter), with any remaining void space filled with BN powder. The assembly was subjected to 3.3 GPa pressure at room temperature using a Rockland Research cubic multi-anvil press (~20mm anvil size) and then heated to 490 °C. This temperature was selected as the maximum before the Mn-Sb mix begins to melt, determined using the sample current (power) as a function of temperature curve, as shown in Fig. S7 c . The reason to prevent the mixture from melting during the experiment is to avoid a large amount of Mn 1.1 Sb impurity from incongruent melting, as shown in Figs. S7 b and d . After maintaining this temperature for 24 hours, the sample was quenched to room temperature before slowly releasing the pressure. This two-step process yields a high-quality MnSb 2 product, with more than half of the final material consisting of sub-millimeter-sized single crystals that can be easily separated from the surrounding polycrystalline matrix. Single Crystal X-ray diffraction: To determine the crystal structure of the obtained single crystal, the sample with dimensions 0.218 × 0.158 × 0.138 mm³ was picked up, mounted on a nylon loop with Paratone oil, and measured using an XtalLAB Synergy, Dualflex, Hypix single crystal X-ray diffractometer with an Oxford Cryosystems 800 low-temperature device. Data were collected using ω scans with Mo Kα radiation (λ = 0.71073 Å). The total number of runs and images was based on the strategy calculation from the program CrysAlisPro 1.171.43.92a (Rigaku OD, 2023). Data reduction was performed with correction for Lorentz polarization. The integration of the data using an orthorhombic unit cell yielded a total of 3540 reflections to a maximum θ angle of 40.13° (0.55 Å resolution), of which 478 were independent (average redundancy 7.406, completeness = 98.8%, Rint = 5.61%). A numerical absorption correction was applied based on Gaussian integration over a multifaceted crystal model 43 . Empirical absorption correction used spherical harmonics, implemented in the SCALE3 ABSPACK scaling algorithm. 44 The structure was solved and refined using the SHELXTL Software Package 45,46 . Powder X-ray diffraction: To examine the phase information, the powder X-ray diffraction (PXRD) analysis was performed subsequent to the synthesis process. The crystals were ground using an agate mortar and pestle to achieve a homogeneous powder. This powdered sample was then uniformly distributed on a single crystalline silicon sample holder, designed for zero background measurements, with a minimal application of vacuum grease to secure the powder in place. The PXRD data acquisition spanned a 2θ range from 15° to 80°, utilizing incremental steps of 0.01° and a fixed dwell time of 3 seconds per step. These measurements were conducted using a Rigaku MiniFlex II powder diffractometer, employing Bragg-Brentano geometry coupled with Cu Kα radiation (λ = 1.5406 Å). The refinement of the powder X-ray data was executed using the GSAS-II software suite 47 . Physical Properties Measurements: Temperature-, magnetic-field-dependent DC magnetization data and resistance measurements were collected using Quantum Design (QD), Magnetic Property Measurement Systems (MPMS and MPMS3), and Physical Property Measurement Systems (PPMS). During the measurements of single crystals, the field is along a random direction of the crystals due to the poorly defined facets and the small size of the crystal. The samples are placed between two collapsed plastic straws, with the third uncollapsed straw providing support as a sheath on the outside or a quartz sample holder. Samples were fixed on the straw or quartz sample holder with GE-7031-varnish. AC electrical resistance measurements were performed in a standard four-contact geometry using the ACT option of the PPMS, with a 3-mA current and a frequency of 17 Hz. 50µm diameter Pt wires were bonded to the samples with silver paint (DuPont 4929N) with contact resistance values of about 2-3 Ohms. Temperature-dependent specific heat measurements on the MnSb 2 in a mass of about 6 mg polycrystalline sample were carried out using a Quantum Design, Physical Property Measurement System (PPMS DynaCool) in the temperature range of 200-280 K ( H grease), 150 K- 280 K (N grease with addenda measurement points that are the same as the sample measurement), 107 K-127 K( N grease), and 4 K- 200 K (N grease). Neutron Powder Diffraction: To determine whether magnetic ordering exists, neutron powder diffraction (NPD) measurements were performed using a time-of-flight powder diffractometer, POWGEN, at the Spallation Neutron Source at Oak Ridge National Laboratory. Approximately 2.6 g of samples were prepared after grinding several single crystals to a fine powder and passing them through a 45µm mesh sieve. Diffraction patterns were collected at 308 K for 2 hours 36 minutes using a neutron beam with a center wavelength of 1.5. Rietveld refinements using GSAS-II software 47 and Fullprof suite 48 were performed to determine the crystal and magnetic structures, respectively. Determination of the magnetic structure was performed on HB-2A POWDER beamline at the High-Flux Isotope Reactor (HFIR) located at Oak Ridge National Lab (ORNL). Roughly 1 g of MnSb 2 was loaded into an aluminum can backfilled with He. Diffraction patterns were measured with a vertically focused Ge monochromator to select the 2.41 Å wavelength while a collimation of open-open-12 was used. Magnetic structure analysis was performed with SARAh Representation Analysis and SARAh Refine and refined with the Fullprof suite software 49 . Nuclear Magnetic Resonance: Nuclear magnetic resonance (NMR) measurements of 55 Mn (nuclear spin I = 5/2, gyromagnetic ratio g N /2p = 10.50 MHz/T), 121 Sb ( I = 5/2, g N /2p =10.189 MHz/T), and 123 Sb ( I = 7/2, g N /2p =5.517 MHz/T) nuclei were conducted using a laboratory-built phase-coherent spin-echo pulse spectrometer on polycrystalline powder samples. The NMR spectrum was obtained under magnetic fields by sweeping the magnetic field at a fixed NMR frequency of 67 MHz, while the zero magnetic field NMR spectrum was measured by plotting spin-echo intensity as a function of NMR frequency. DFT Calculation: Density Functional Theory (DFT) calculations were carried out using version 7.3.1 of the Quantum ESPRESSO package to evaluate the total energies of MnSb 2 in non-magnetic, ferromagnetic, and antiferromagnetic configurations. 50 The calculations employed ultrasoft pseudopotentials and the Perdew-Burke-Ernzerhof (PBE) exchange-correlation functional within the generalized gradient approximation (GGA). 51–53 A plane-wave kinetic energy cutoff of 300 Ry was used, with a charge density cutoff set to 3600 Ry (12 times the wavefunction cutoff). Brillouin zone integration was performed using a 7×7×13 Monkhorst-Pack k-point grid. 54 Total energy convergence was ensured with a threshold of less than 1 meV per atom. The electronic self-consistency was achieved using the Davidson diagonalization algorithm, with a convergence criterion of 10 -9 Ry. 55 High-symmetrical k -point paths for band structure calculations were generated using the Spglib library. 56,57 Declarations Author Contributions W.X. conceived the research idea. M.X. carried out experimental synthesis and physical property characterization. M.B., Q.Z., and D.Y. performed neutron scattering experiments and analysis. Q.-P.D. and Y.F. conducted solid-state NMR measurements and analysis. P.C. performed the simulations. A.S., S.B., and R.R. contributed to physical property measurements, data analysis, and manuscript preparation. W.X. and P.C. supervised the project. All authors discussed the results and contributed to the final manuscript. Funding This work was primarily supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award DE-SC-0023648 (Michigan State University) to Weiwei Xie. Work carried out at Ames National Laboratory was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. Ames National Laboratory is operated for the U.S. Department of Energy by Iowa State University under Contract DE-AC02-07CH11358 to Paul Canfield. C.P. in the Weiwei Xie group was supported by the National Science Foundation under Grant NSF-DMR-2422361 (to Weiwei Xie). A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by Oak Ridge National Laboratory. M. B. in the Weiwei Xie group was supported by the DOE Office of Science Graduate Student Research Program, administered by the Oak Ridge Institute for Science and Education (ORISE) for the U.S. Department of Energy. ORISE is managed by Oak Ridge Associated Universities under Contract DE-SC0014664. 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Spglib: A Software Library for Crystal Symmetry Search. Science and Technology of Advanced Materials: Methods 2024 , 4 (1). https://doi.org/10.1080/27660400.2024.2384822. Additional Declarations No competing interests reported. Supplementary Files MnSb2v16SI.docx Cite Share Download PDF Status: Under Review Version 1 posted Reviewers agreed at journal 18 May, 2026 Reviewers agreed at journal 18 May, 2026 Reviews received at journal 10 Apr, 2026 Reviewers agreed at journal 23 Mar, 2026 Reviewers agreed at journal 21 Mar, 2026 Reviewers agreed at journal 21 Mar, 2026 Reviewers invited by journal 16 Mar, 2026 Editor assigned by journal 11 Mar, 2026 Submission checks completed at journal 10 Mar, 2026 First submitted to journal 26 Feb, 2026 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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Red circles indicate experimental data, the black line the calculated pattern, and the blue line the difference curve. The main phase is indexed to MnSb\u003csub\u003e2\u003c/sub\u003e, with a minor impurity phase identified as elemental Sb (about 1% by weight). \u003cem\u003eRight inset\u003c/em\u003e: crystal structure of MnSb\u003csub\u003e2\u003c/sub\u003e. \u003cem\u003eLeft inset\u003c/em\u003e: optical image of representative single crystals; grid spacing is 1 mm.\u003c/p\u003e","description":"","filename":"1.png","url":"https://assets-eu.researchsquare.com/files/rs-8980468/v1/a85ca5097e7338d40b1c6f7f.png"},{"id":105034057,"identity":"dd6ea0f0-7298-4408-8f47-3b006b403afb","added_by":"auto","created_at":"2026-03-20 07:22:33","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":126402,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003e(\u003c/strong\u003e\u003cem\u003e\u003cstrong\u003ea\u003c/strong\u003e\u003c/em\u003e\u003cstrong\u003e)\u003c/strong\u003e Temperature-dependent magnetization of MnSb\u003csub\u003e2\u003c/sub\u003e measured under field-cooling (FC) and field-warming (FW) across different temperature ranges: 300-350 K (black), 300-400 K (blue), 300-450 K (yellow), and 300-500 K (red). A significant increase in magnetization above 450 K indicates the onset of decomposition. \u003cstrong\u003e(\u003c/strong\u003e\u003cem\u003e\u003cstrong\u003eb\u003c/strong\u003e\u003c/em\u003e\u003cstrong\u003e)\u003c/strong\u003e Powder X-ray diffraction patterns collected before and after the magnetization measurements are shown in \u003cstrong\u003e(\u003c/strong\u003e\u003cem\u003e\u003cstrong\u003ea\u003c/strong\u003e\u003c/em\u003e\u003cstrong\u003e)\u003c/strong\u003e. The emergence of Mn\u003csub\u003e1.1\u003c/sub\u003eSb reflections and an increase in Sb peak intensity after heating above 500 K confirm the thermal decomposition of MnSb\u003csub\u003e2\u003c/sub\u003e.\u003c/p\u003e","description":"","filename":"2.png","url":"https://assets-eu.researchsquare.com/files/rs-8980468/v1/ba780f6a184044461eff3010.png"},{"id":104898072,"identity":"89faddde-11d2-4ea1-ad42-ac9a72a6a5f9","added_by":"auto","created_at":"2026-03-18 12:34:00","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":285120,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eElectrical transport, specific heat, and magnetization of MnSb\u003c/strong\u003e\u003csub\u003e\u003cstrong\u003e2\u003c/strong\u003e\u003c/sub\u003e\u003cstrong\u003e. (\u003c/strong\u003e\u003cem\u003e\u003cstrong\u003ea\u003c/strong\u003e\u003c/em\u003e\u003cstrong\u003e)\u003c/strong\u003e Electrical resistance of single-crystalline MnSb\u003csub\u003e2\u003c/sub\u003e measured upon cooling (black) and warming (red) between 300 K and 1.8 K, showing negligible thermal hysteresis. \u003cem\u003eInset\u003c/em\u003e: Temperature derivative \u003cem\u003ed\u003c/em\u003eR/\u003cem\u003ed\u003c/em\u003eT with two anomalies. \u003cstrong\u003e(\u003c/strong\u003e\u003cem\u003e\u003cstrong\u003eb\u003c/strong\u003e\u003c/em\u003e\u003cstrong\u003e)\u003c/strong\u003e Temperature-dependent specific heat showing three anomalies at \u003cem\u003eT\u003c/em\u003e\u003csub\u003e0\u003c/sub\u003e, \u003cem\u003eT\u003c/em\u003e\u003csub\u003e1,\u003c/sub\u003e and \u003cem\u003eT\u003c/em\u003e\u003csub\u003e2\u003c/sub\u003e, defined by the midpoint between onset and offset temperatures, shown in the right insets. Data from 200-280 K are obtained by point-by-point background subtraction of N-grease measurements. The temperature range is from 4K -280 K. The left inset shows a comparison of H-grease and N-grease measurements. \u003cem\u003eT\u003c/em\u003e\u003csub\u003e1,\u003c/sub\u003e and \u003cem\u003eT\u003c/em\u003e\u003csub\u003e2\u003c/sub\u003e anomalies are clearly shown in both measurements. \u003cstrong\u003e(\u003c/strong\u003e\u003cem\u003e\u003cstrong\u003ec\u003c/strong\u003e\u003c/em\u003e\u003cstrong\u003e) \u003c/strong\u003eField-dependent magnetization (\u003cem\u003eM\u003c/em\u003e-\u003cem\u003eH\u003c/em\u003e) of polycrystalline MnSb\u003csub\u003e2\u003c/sub\u003e measured at selected temperatures. Inset: representative \u003cem\u003eM\u003c/em\u003e-\u003cem\u003eH\u003c/em\u003e curves at 300 K.\u003cstrong\u003e (\u003c/strong\u003e\u003cem\u003e\u003cstrong\u003ed\u003c/strong\u003e\u003c/em\u003e\u003cstrong\u003e) \u003c/strong\u003eTemperature-dependent magnetization (\u003cem\u003eM\u003c/em\u003e-\u003cem\u003eT\u003c/em\u003e) of polycrystalline MnSb\u003csub\u003e2\u003c/sub\u003e measured under applied magnetic fields. \u003cem\u003eInset\u003c/em\u003e: temperature derivative of \u003cem\u003eMT\u003c/em\u003e, showing two anomalies between 1.8 K and 300 K. The black arrow indicates the anomalies shown in the measurement and the criteria of anomalies’ temperature and width.\u003c/p\u003e\n\u003cp\u003e\u0026nbsp;\u003c/p\u003e","description":"","filename":"3.png","url":"https://assets-eu.researchsquare.com/files/rs-8980468/v1/54910bd973899f1e9818bd6b.png"},{"id":105034441,"identity":"789fc201-3cd0-496c-bd9d-379415f0009c","added_by":"auto","created_at":"2026-03-20 07:23:18","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":220489,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eNeutron diffraction and magnetic structure of MnSb\u003c/strong\u003e\u003csub\u003e\u003cstrong\u003e2\u003c/strong\u003e\u003c/sub\u003e\u003cstrong\u003e. (\u003c/strong\u003e\u003cem\u003e\u003cstrong\u003ea\u003c/strong\u003e\u003c/em\u003e\u003cstrong\u003e) \u003c/strong\u003ePowder neutron diffraction patterns of MnSb\u003csub\u003e2\u003c/sub\u003e collected at 308, 250, 200, 150, 100, and 4 K (logarithmic intensity scale).\u003cbr\u003e\n\u003cstrong\u003e(\u003c/strong\u003e\u003cem\u003e\u003cstrong\u003eb\u003c/strong\u003e\u003c/em\u003e\u003cstrong\u003e,\u003c/strong\u003e\u003cem\u003e\u003cstrong\u003e c\u003c/strong\u003e\u003c/em\u003e\u003cstrong\u003e) \u003c/strong\u003eRietveld refinements of the powder neutron diffraction data collected at 308 K(an aluminum can contributes the impurity peaks of Al in \u003cstrong\u003eFig\u003c/strong\u003e. \u003cstrong\u003e4\u003c/strong\u003e\u003cem\u003e\u003cstrong\u003eb\u003c/strong\u003e\u003c/em\u003e), 200 K, and 4 K, illustrating the emergence of magnetic reflections upon cooling.\u003c/p\u003e","description":"","filename":"4.png","url":"https://assets-eu.researchsquare.com/files/rs-8980468/v1/0005e64f10ba13980b60dba9.png"},{"id":105034496,"identity":"8bb1e3cc-04d6-45a7-a8d4-ce786e9389cf","added_by":"auto","created_at":"2026-03-20 07:23:25","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":363735,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eCalculated electronic band structure of MnSb\u003c/strong\u003e\u003csub\u003e\u003cstrong\u003e2\u003c/strong\u003e\u003c/sub\u003e\u003cstrong\u003e. (\u003c/strong\u003e\u003cem\u003e\u003cstrong\u003ea\u003c/strong\u003e\u003c/em\u003e\u003cstrong\u003e) \u003c/strong\u003eNon-magnetic (spin-unpolarized) state. \u003cstrong\u003e(\u003c/strong\u003e\u003cem\u003e\u003cstrong\u003eb\u003c/strong\u003e\u003c/em\u003e\u003cstrong\u003e)\u003c/strong\u003e Antiferromagnetic state.\u003c/p\u003e","description":"","filename":"5.png","url":"https://assets-eu.researchsquare.com/files/rs-8980468/v1/1f89878a00b69e48ce5dd625.png"},{"id":105036669,"identity":"b693ab6a-b487-4297-b0f0-329642573563","added_by":"auto","created_at":"2026-03-20 07:35:05","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":2058962,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-8980468/v1/a6bedff5-67fc-468d-9897-ad6a88073c78.pdf"},{"id":104898074,"identity":"1d0eec23-74d1-4706-a77b-d14e4180db82","added_by":"auto","created_at":"2026-03-18 12:34:00","extension":"docx","order_by":0,"title":"","display":"","copyAsset":false,"role":"supplement","size":1560184,"visible":true,"origin":"","legend":"","description":"","filename":"MnSb2v16SI.docx","url":"https://assets-eu.researchsquare.com/files/rs-8980468/v1/d3ca54adbeccbbafa4ae711f.docx"}],"financialInterests":"No competing interests reported.","formattedTitle":"\u003cp\u003e\u003cstrong\u003ePressure-Stabilized MnSb\u003c/strong\u003e\u003csub\u003e\u003cstrong\u003e2\u003c/strong\u003e\u003c/sub\u003e\u003cstrong\u003e with Complex Incommensurate Magnetic Order\u003c/strong\u003e\u003c/p\u003e","fulltext":[{"header":"Introduction","content":"\u003cp\u003eWhen magnetism intertwines with band topology in quantum materials, it can, in some cases, give rise to a recently identified class of magnetic systems characterized by collinear spin arrangements with zero net magnetization, exhibiting time-reversal-symmetry-breaking responses\u003csup\u003e\u003cspan additionalcitationids=\"CR2 CR3 CR4 CR5 CR6 CR7\" citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e\u003c/sup\u003e and spin-split electronic band structures \u003csup\u003e\u003cspan additionalcitationids=\"CR10 CR11 CR12 CR13 CR14 CR15\" citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e\u003c/sup\u003e. These properties, referred to as altermagnetism, combine zero-net-moment magnetic order with symmetry-allowed spin splitting relevant for spintronic applications and have motivated intense theoretical and experimental interest in identifying chemically clean material platforms that realize this magnetic phase\u003csup\u003e\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e,\u003cspan additionalcitationids=\"CR18 CR19 CR20 CR21 CR22 CR23 CR24 CR25 CR26 CR27 CR28 CR29 CR30\" citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e31\u003c/span\u003e\u003c/sup\u003e. Marcasite-type compounds, in particular, have emerged as promising candidates due to their low crystal symmetry and symmetry-allowed spin splitting in antiferromagnetic states. FeSb\u003csub\u003e2\u003c/sub\u003e is a narrow-gap, strongly correlated semiconductor\u003csup\u003e\u003cspan additionalcitationids=\"CR33 CR34 CR35\" citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR36\" class=\"CitationRef\"\u003e36\u003c/span\u003e\u003c/sup\u003e that has been theoretically predicted to host a collinear altermagnetic state upon Co substitution or hole doping\u003csup\u003e\u003cspan citationid=\"CR37\" class=\"CitationRef\"\u003e37\u003c/span\u003e\u003c/sup\u003e. Experimentally, however, FeSb\u003csub\u003e2\u003c/sub\u003e exhibits no long-range magnetic order between 1.8 and 300 K. Stabilizing magnetic order in FeSb\u003csub\u003e2\u003c/sub\u003e therefore requires deliberate tuning of its electronic structure. While chemical substitution and external pressure are widely used to modify band filling and band width, substitution often introduces chemical disorder that complicates interpretation, and pressure-dependent magnetic measurements are experimentally nontrivial, especially for antiferromagnetism. This all motivates the search for chemically clean routes to stabilize magnetic order in the FeSb\u003csub\u003e2\u003c/sub\u003e structure class.\u003c/p\u003e \u003cp\u003eA promising route to this goal is provided by MnSb\u003csub\u003e2\u003c/sub\u003e, a high-pressure marcasite-type compound that shares the same orthorhombic structure as FeSb\u003csub\u003e2\u003c/sub\u003e but incorporates Mn with a larger, and often more robust, local magnetic moment and intrinsic hole doping\u003csup\u003e\u003cspan citationid=\"CR38\" class=\"CitationRef\"\u003e38\u003c/span\u003e\u003c/sup\u003e(relative to FeSb\u003csub\u003e2\u003c/sub\u003e). Whereas MnSb\u003csub\u003e2\u003c/sub\u003e does not form at ambient pressure, it can be synthesized under high-pressure conditions and quenched into a metastable form at ambient pressure\u003csup\u003e\u003cspan citationid=\"CR39\" class=\"CitationRef\"\u003e39\u003c/span\u003e\u003c/sup\u003e. Across the marcasite family, CrSb\u003csub\u003e2\u003c/sub\u003e exhibits robust antiferromagnetic order with a N\u0026eacute;el temperature near 273 K\u003csup\u003e40\u003c/sup\u003e, whereas FeSb₂ remains nonmagnetic, suggesting that magnetic order emerges through band filling by hole doping. By analogy, MnSb₂ represents a chemically ordered, stoichiometric platform in which unconventional states may be realized.\u003c/p\u003e"},{"header":"Results and Discussion","content":"\u003cp\u003eMnSb\u003csub\u003e2\u003c/sub\u003e was synthesized at 3.3 GPa pressure and 490 \u0026deg;C using a Rockland Research cubic multi-anvil press. After maintaining this temperature for 24 hours, a high-quality MnSb\u003csub\u003e2\u003c/sub\u003e product, with more than half of the final material consisting of sub-millimeter-sized MnSb\u003csub\u003e2\u0026nbsp;\u003c/sub\u003esingle crystals that can be easily separated mechanically from the surrounding MnSb\u003csub\u003e2\u0026nbsp;\u003c/sub\u003epolycrystalline matrix, was obtained. (See the Experimental Method section for further details.) The single-crystal X-ray diffraction (SCXRD) analysis of MnSb\u003csub\u003e2\u003c/sub\u003e, summarized in \u003cstrong\u003eTables S1\u003c/strong\u003e and \u003cstrong\u003eS2\u003c/strong\u003e, illustrates the crystal structure of MnSb\u003csub\u003e2\u003c/sub\u003e shown in the right inset of \u003cstrong\u003eFig. 1\u003c/strong\u003e, which adopts the orthorhombic \u003cem\u003ePnnm\u003c/em\u003e space group and features edge-sharing MnSb\u003csub\u003e6\u003c/sub\u003e octahedra. The unit cell contains two crystallographically distinct atomic sites: Mn atoms occupy the 2\u003cem\u003ea\u003c/em\u003e Wyckoff position, while Sb atoms reside at the 4\u003cem\u003eg\u003c/em\u003e positions. Vacancies and site mixing were considered during the refinement, but no structural disorder or clear vacancies were detected.\u003c/p\u003e\n\u003cp\u003eTo assess the phase purity of samples synthesized under high-pressure conditions, powder X-ray diffraction (PXRD) measurements were performed using a bulk sample with single crystals in the polycrystalline matrix, as shown in \u003cstrong\u003eFig. 1\u003c/strong\u003e. The experimental data (red circles) were analyzed by Rietveld refinement (black line) using the GSAS-II software package\u003csup\u003e41\u003c/sup\u003e, and the difference between the observed and calculated patterns is shown by the blue line. The minor phase of elemental Sb is observed. The PXRD results are consistent with single-crystal X-ray diffraction measurements and with the previous report.\u003csup\u003e39\u003c/sup\u003e The left inset of \u003cstrong\u003eFig. 1\u003c/strong\u003e shows representative as-grown crystals, which display metallic luster and well-defined faceted morphologies, consistent with high crystallinity.\u003c/p\u003e\n\u003cp\u003eTo determine the thermal stability range of MnSb\u003csub\u003e2\u003c/sub\u003e at ambient pressure, temperature-dependent magnetization measurements were performed under both field-warming (FW) and field-cooling (FC) conditions, as shown in \u003cstrong\u003eFig. 2\u003cem\u003ea\u003c/em\u003e\u003c/strong\u003e. Below 450 K, the magnetization curves exhibit no significant difference between the FW and FC protocols, indicating thermal and magnetic stability within this temperature range. However, above 450 K, a pronounced increase in magnetic moment is observed, suggesting the onset of decomposition and the formation of Mn\u003csub\u003e1.1\u003c/sub\u003eSb, a known ferromagnetic impurity phase. This observation is corroborated by powder X-ray diffraction data collected before and after the magnetization measurements. As shown in \u003cstrong\u003eFig. 2\u003cem\u003eb\u003c/em\u003e\u003c/strong\u003e, additional reflections corresponding to Mn\u003csub\u003e1.1\u003c/sub\u003eSb emerge, and the intensity of the Sb peak increases significantly after heating above 500 K, confirming the partial decomposition of MnSb\u003csub\u003e2\u003c/sub\u003e. These results indicate that while MnSb\u003csub\u003e2\u003c/sub\u003e is metastable at ambient pressure, it remains structurally and magnetically stable at temperatures up to ~450 K, enabling long-term low-temperature studies without phase transformation. Moreover, within the temperature range of 1.8 K to 300 K, magnetization measurements (see \u003cstrong\u003eFig. 5\u003c/strong\u003e) show no signatures of ferromagnetic or other phase transitions in MnSb\u003csub\u003e2\u003c/sub\u003e. The field-dependent magnetization displays predominant paramagnetic behavior with minor ferromagnetic contributions attributable to trace Mn\u003csub\u003e1.1\u003c/sub\u003eSb impurities. Collectively, these results confirm that MnSb\u003csub\u003e2\u003c/sub\u003e is suitable for extended investigations at low temperatures under ambient conditions, without undergoing structural or magnetic phase transitions.\u003c/p\u003e\n\u003cp\u003eTo probe the magnetic and electronic properties of MnSb\u003csub\u003e2\u003c/sub\u003e, temperature-dependent electrical resistance measurements were performed on single-crystalline samples upon cooling from 300 K to 1.8 K and during subsequent warming, as shown in \u003cstrong\u003eFig. 3\u003cem\u003ea\u003c/em\u003e\u003c/strong\u003e. The resistance curves from the cooling and warming cycles overlap closely, indicating negligible thermal hysteresis. The residual resistance ratio (RRR), defined as R(300K)/R(1.8K), is approximately 60. The inset of \u003cstrong\u003eFig. 3\u003cem\u003ea\u003c/em\u003e\u003c/strong\u003e displays the temperature derivative of the resistance (d\u003cem\u003eR\u003c/em\u003e/d\u003cem\u003eT\u003c/em\u003e). There are two clear breaks in slope visible in the raw data and two broad steps in d\u003cem\u003eR\u003c/em\u003e/d\u003cem\u003eT\u003c/em\u003e around 125 K and 220 K, as indicated with the arrows in \u003cstrong\u003eFig. 3\u003cem\u003ea\u003c/em\u003e\u003c/strong\u003e and the inset. Complementary thermodynamic information is provided by temperature-dependent specific heat measurements on polycrystalline MnSb\u003csub\u003e2\u003c/sub\u003e performed at zero magnetic field. As shown in \u003cstrong\u003eFig. 3\u003cem\u003eb\u003c/em\u003e\u003c/strong\u003e, three reproducible anomalies are observed at approximately 118 K (\u003cem\u003eT\u003c/em\u003e\u003csub\u003e0\u003c/sub\u003e), 219 K (\u003cem\u003eT\u003c/em\u003e₁), and 231 K (\u003cem\u003eT\u003c/em\u003e₂). These features are independently confirmed using an alternative measurement protocol over a different temperature range. Notably, the application of a magnetic field of 90 kOe produces negligible changes in specific heat (\u003cstrong\u003eFig. S3\u003cem\u003ea\u003c/em\u003e\u003c/strong\u003e), demonstrating that the transition is largely insensitive to external magnetic fields. Integration of the excess specific heat yields a total magnetic entropy change of approximately \u0026nbsp; (\u003cstrong\u003eFig. S3\u003cem\u003eb\u003c/em\u003e\u003c/strong\u003e) using the reference of FeSb\u003csub\u003e2\u003c/sub\u003e specific heat, which is close to the Mn high-spin state. Curiously, the weak field dependence of the upper specific heat feature might suggest an antiferromagnetic transition that couples only weakly to uniform magnetic fields. To assess the uniform magnetic response of MnSb\u003csub\u003e2\u003c/sub\u003e and the presence of any net magnetic moment, magnetic susceptibility and field-dependent magnetization measurements were performed. \u003cstrong\u003eFig. 3\u003cem\u003ea\u003c/em\u003e\u003c/strong\u003e shows the field-dependent magnetization of polycrystalline MnSb\u003csub\u003e2\u003c/sub\u003e measured up to 70 kOe at selected temperatures. The magnetization exhibits only weak temperature dependence, remains unsaturated over the entire field range, and displays a very small net moment. A weak ferromagnetic contribution is observed and attributed to trace amounts (\u0026lt;1%) of the Mn\u003csub\u003e1.1\u003c/sub\u003eSb impurity, which is below the detection limit of X-ray diffraction but was detected by NMR measurements (\u003cstrong\u003eFig. S5\u003c/strong\u003e). The inset shows representative \u003cem\u003eM\u003c/em\u003e(\u003cem\u003eH\u003c/em\u003e) curves measured at 300 K in five quadrants, confirming the absence of intrinsic ferromagnetic hysteresis. \u003cstrong\u003eFig. 3\u003cem\u003eb\u003c/em\u003e\u003c/strong\u003e presents the temperature-dependent magnetization of polycrystalline MnSb\u003csub\u003e2\u003c/sub\u003e measured under a 10 kOe applied field. There are two anomalies between 2 K and 300 K, \u003cem\u003eT\u003c/em\u003e\u003csub\u003e0\u003c/sub\u003e = 122 K and \u003cem\u003eT\u003c/em\u003e\u0026rsquo;\u003csub\u003e1\u003c/sub\u003e = 226 K, indicated by the black arrows. This observation is consistent with electric transport and the heat-capacity measurements. The inset displays the temperature derivative of \u003cem\u003eMT\u003c/em\u003e, which shows two anomalies. This behavior is consistent with an amplitude-modulated antiferromagnetic ground state and highlights the limited sensitivity of uniform magnetization measurements to this type of magnetic order as well as a relatively large contribution to \u003cem\u003eM\u003c/em\u003e(\u003cem\u003eT\u003c/em\u003e) from a ferromagnetic impurity. To elucidate the microscopic origin of this magnetic transition, we next turn to neutron scattering measurements, which directly probe the magnetic ordering wave vector and spatial distribution of the ordered moments.\u003c/p\u003e\n\u003cp\u003ePowder neutron diffraction measurements on MnSb\u003csub\u003e2\u003c/sub\u003e were carried out between 308 K and 4 K (\u003cstrong\u003eFig. 4\u003c/strong\u003e). Upon cooling below ~200 K, well below the ~220 K upper magnetic transitions, additional Bragg reflections (shown in the red arrows) of magnetic origin emerge (\u003cstrong\u003eFig. 4\u003cem\u003ea\u003c/em\u003e\u003c/strong\u003e). Similar magnetic peaks are found at 150 K and new peaks (shown in the black arrows) at 100K and 4 K, temperatures below the lower magnetic transition. \u0026nbsp; Refinements of diffraction patterns collected above (\u003cstrong\u003eFigs. 4\u003cem\u003eb\u003c/em\u003e\u003c/strong\u003e) and below (\u003cstrong\u003eFig. 4\u003cem\u003ec\u003c/em\u003e\u003c/strong\u003e) the show that orthorhombic MnSb\u003csub\u003e2\u003c/sub\u003e develops a complex magnetic ground state that evolves with temperature. Two irreducible representations can be utilized to analyze the structure that is related by symmetry. \u0026nbsp;\u003c/p\u003e\n\u003cp\u003eThe magnetic powder refinement allows many magnetic structures to fit reasonably well. Although most structures are aligned with a spin density wave formation, trying a helical magnetic structure overall results in a lower quality of fit. The multiple models that can describe this system make it challenging to determine the direction of the spin density wave specifically and require polarized neutrons to better understand the structure. However, in many models, the Mn moment reaches a maximum of 2 \u0026mu;\u003csub\u003eB\u003c/sub\u003e\u003csub\u003e\u0026nbsp;\u003c/sub\u003eand tends to be collinear with little orientation along the \u003cem\u003ec-\u003c/em\u003eaxis. The propagation vector \u003cem\u003eq\u003c/em\u003e is (0, 0.3975, 0.3783) at 200 K, and the \u003cem\u003eb\u003c/em\u003e component of the propagation vector increases as temperature decreases, and the value approaches 0.5. With the changing temperature, the modulation of the spin wave changes and typically requires changing the model from high to low temperatures, further highlighting the complexity of the magnetic order within the system.\u003c/p\u003e\n\u003cp\u003eThe magnetic ground state of orthorhombic MnSb\u003csub\u003e2\u003c/sub\u003e is fundamentally distinct from both conventional helical magnets and simple spin-density-wave (SDW) systems. \u0026nbsp;Importantly, the strictly collinear antiferromagnetic order with zero net magnetization, combined with sublattice-dependent anisotropy and broken spin degeneracy at finite wave vector, places MnSb\u003csub\u003e2\u003c/sub\u003e in close proximity to the emerging class of altermagnetic materials.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eTo evaluate the magnetic ground state of MnSb\u003csub\u003e2\u003c/sub\u003e, first-principles calculations were performed using the experimentally determined single-crystal structure, considering non-magnetic (NM), ferromagnetic (FM), and a simple collinear antiferromagnetic (AFM) configurations with antiparallel Mn moments in the primitive cell. Although neutron diffraction reveals a considerably more complex magnetic structure, calculations with a simple collinear AFM configuration provide a useful reference for evaluating the magnetic instability of the electronic structure. In addition, the limited experimental constraints on the full magnetic structure from unpolarized neutron diffraction and the computational cost of large magnetic supercells make such simplified calculations a practical first step. The calculated total energies (\u003cstrong\u003eTable S3\u003c/strong\u003e) show that the AFM state is the most stable, lying 80.79 meV below the NM configuration, while the FM state is also energetically favored (69.68 meV below NM), indicating close energetic competition among magnetic states. In the AFM configuration, the calculated local magnetic moment on Mn is 2.81 \u0026mu;\u003csub\u003eB\u003c/sub\u003e. The calculated electronic band structures are shown in \u003cstrong\u003eFig. 5\u003c/strong\u003e. In the NM state (\u003cstrong\u003eFig. 5\u003cem\u003ea\u003c/em\u003e\u003c/strong\u003e), a flat band appears near the Fermi level, producing a pronounced peak in the density of states and signaling electronic instability. Although MnSb\u003csub\u003e2\u003c/sub\u003e shares the same nominal valence electron count as FeSb\u003csub\u003e2\u003c/sub\u003e, the partial occupation of states at the Fermi level confirms metallic behavior rather than the insulating ground state of FeSb\u003csub\u003e2\u003c/sub\u003e. Upon inclusion of spin polarization in the AFM state (\u003cstrong\u003eFig. 5\u003cem\u003eb\u003c/em\u003e\u003c/strong\u003e), the flat band shifts below the Fermi level, and the density of states at the Fermi level is strongly reduced, leading to the formation of a pseudogap and a more stable electronic structure. Importantly, the AFM state breaks time-reversal symmetry while preserving a net zero magnetization, a symmetry condition that can allow momentum-dependent spin splitting of electronic bands in low-symmetry crystals. This symmetry condition is consistent with the collinear, finite- \u0026nbsp;antiferromagnetic order and orthogonal sublattice anisotropy resolved by neutron diffraction, although a detailed analysis of altermagnetic band splitting is beyond the scope of the present calculations. Together, these results indicate that MnSb\u003csub\u003e2\u003c/sub\u003e satisfies the essential energetic and symmetrical prerequisites for altermagnetic behavior, motivating future momentum-resolved experimental and theoretical studies.\u003c/p\u003e\n\u003cp\u003eIn summary, altermagnets have recently emerged as a distinct class of magnetic materials that combine collinear antiferromagnetic order with spin-split electronic band structures and zero net magnetization, offering new opportunities for quantum and spintronic functionalities. In this work, we establish MnSb\u003csub\u003e2\u003c/sub\u003e as a chemically clean, pressure-stabilized marcasite-type compound hosting an unconventional magnetic ground state. Using high-pressure synthesis, thermodynamic measurements, neutron diffraction, and first-principles calculations, we show that MnSb\u003csub\u003e2\u003c/sub\u003e does not develop a single, rigid magnetic order below a well-defined \u003cem\u003eT\u003c/em\u003e\u003csub\u003eN\u003c/sub\u003e. Instead, magnetic entropy begins to be released near ~230 K, accompanied by the appearance of incommensurate magnetic Bragg reflections below ~ 200 K. A second thermodynamic anomaly near ~ 118 K coincides with the emergence of additional magnetic peaks, indicating a reconstruction of the ordered state. Remarkably, specific heat and neutron refinements reveal that the magnetic structure continues to evolve throughout the ordered regime: the propagation vector shifts systematically with temperature (with the \u003cem\u003eb\u003c/em\u003e-component trending toward 0.5). The relating ground state is described as a complex SDW with the available data do not uniquely determine the modulation direction, and polarized neutron experiments will be required for definitive resolution. \u0026nbsp;These findings establish MnSb\u003csub\u003e2\u003c/sub\u003e as a rare stoichiometric platform in which an incommensurate SDW remains highly tunable at low temperature, highlighting an unusual interplay between anisotropy, competing exchange interactions, and the underlying electronic structure.\u003c/p\u003e"},{"header":"Experimental Methods","content":"\u003cp\u003e\u003cstrong\u003eHigh-Pressure Synthesis:\u003c/strong\u003e MnSb\u003csub\u003e2\u003c/sub\u003e was synthesized using a two-step method, which is different from the reference\u003csup\u003e39\u003c/sup\u003e(lower pressure and temperature used in this experiment), involving (i) the preparation of a finely mixed Mn\u0026ndash;Sb precursor and (ii) a subsequent high-pressure, high-temperature reaction. In the first step, manganese metal (CZ-1-110) and antimony shot (99.999%) were combined in a 1:2 molar ratio and loaded into a 1.7 mL fritted alumina Canfield Crucible Set (CCS, LSP Industrial Ceramics, Inc.).\u003csup\u003e42\u003c/sup\u003e The crucible was sealed in a silica ampoule under an argon atmosphere (~1/3 atm). Silica wool was packed above and below the CCS to stabilize the crucible during centrifugation and to contain any escaped liquid. The ampoule was heated in a box furnace to 760 \u0026deg;C over two hours, held at this temperature for 10 hours, and then rapidly centrifuged to separate the molten and non-molten phases. The solid residue retained on the frit disc appeared as a black solid, likely a minor oxide crust, while the solidified, decanted melt was collected, ground into a fine powder, and pressed into a pellet using a die press. In the second step, the pellet was loaded into a boron nitride (BN) crucible (7 mm length, 5.7 mm inner diameter), with any remaining void space filled with BN powder. The assembly was subjected to 3.3 GPa pressure at room temperature using a Rockland Research cubic multi-anvil press (~20mm anvil size) and then heated to 490 \u0026deg;C. This temperature was selected as the maximum before the Mn-Sb mix begins to melt, determined using the sample current (power) as a function of temperature curve, as shown in\u0026nbsp;\u003cstrong\u003eFig. S7\u003cem\u003ec\u003c/em\u003e\u003c/strong\u003e. The reason to prevent the mixture from melting during the experiment is to avoid a large amount of Mn\u003csub\u003e1.1\u003c/sub\u003eSb impurity from incongruent melting, as shown in\u0026nbsp;\u003cstrong\u003eFigs. S7\u003cem\u003eb\u003c/em\u003e\u003c/strong\u003e and\u0026nbsp;\u003cstrong\u003e\u003cem\u003ed\u003c/em\u003e\u003c/strong\u003e. After maintaining this temperature for 24 hours, the sample was quenched to room temperature before slowly releasing the pressure. This two-step process yields a high-quality MnSb\u003csub\u003e2\u003c/sub\u003e product, with more than half of the final material consisting of sub-millimeter-sized single crystals that can be easily separated from the surrounding polycrystalline matrix.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eSingle Crystal X-ray diffraction:\u003c/strong\u003e To determine the crystal structure of the obtained single crystal, the sample with dimensions 0.218 \u0026times; 0.158 \u0026times; 0.138 mm\u0026sup3; was picked up, mounted on a nylon loop with Paratone oil, and measured using an XtalLAB Synergy, Dualflex, Hypix single crystal X-ray diffractometer with an Oxford Cryosystems 800 low-temperature device. Data were collected using \u0026omega; scans with Mo K\u0026alpha; radiation (\u0026lambda; = 0.71073 \u0026Aring;). The total number of runs and images was based on the strategy calculation from the program CrysAlisPro 1.171.43.92a (Rigaku OD, 2023). Data reduction was performed with correction for Lorentz polarization. The integration of the data using an orthorhombic unit cell yielded a total of 3540 reflections to a maximum \u0026theta; angle of 40.13\u0026deg; (0.55 \u0026Aring; resolution), of which 478 were independent (average redundancy 7.406, completeness = 98.8%, Rint = 5.61%). A numerical absorption correction was applied based on Gaussian integration over a multifaceted crystal model\u003csup\u003e43\u003c/sup\u003e. Empirical absorption correction used spherical harmonics, implemented in the SCALE3 ABSPACK scaling algorithm.\u003csup\u003e44\u003c/sup\u003e The structure was solved and refined using the SHELXTL Software Package\u003csup\u003e45,46\u003c/sup\u003e.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003ePowder X-ray diffraction:\u003c/strong\u003e To examine the phase information, the powder X-ray diffraction (PXRD) analysis was performed subsequent to the synthesis process. The crystals were ground using an agate mortar and pestle to achieve a homogeneous powder. This powdered sample was then uniformly distributed on a single crystalline silicon sample holder, designed for zero background measurements, with a minimal application of vacuum grease to secure the powder in place. The PXRD data acquisition spanned a 2\u0026theta; range from 15\u0026deg; to 80\u0026deg;, utilizing incremental steps of 0.01\u0026deg; and a fixed dwell time of 3 seconds per step. These measurements were conducted using a Rigaku MiniFlex II powder diffractometer, employing Bragg-Brentano geometry coupled with Cu K\u0026alpha; radiation (\u0026lambda; = 1.5406 \u0026Aring;). The refinement of the powder X-ray data was executed using the GSAS-II software suite\u003csup\u003e47\u003c/sup\u003e.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003ePhysical Properties Measurements:\u003c/strong\u003e Temperature-, magnetic-field-dependent DC magnetization data and resistance measurements were collected using Quantum Design (QD), Magnetic Property Measurement Systems (MPMS and MPMS3), and Physical Property Measurement Systems (PPMS). During the measurements of single crystals, the field is along a random direction of the crystals due to the poorly defined facets and the small size of the crystal. The samples are placed between two collapsed plastic straws, with the third uncollapsed straw providing support as a sheath on the outside or a quartz sample holder. Samples were fixed on the straw or quartz sample holder with GE-7031-varnish. AC electrical resistance measurements were performed in a standard four-contact geometry using the ACT option of the PPMS, with a 3-mA current and a frequency of 17 Hz. 50\u0026micro;m diameter Pt wires were bonded to the samples with silver paint (DuPont 4929N) with contact resistance values of about 2-3 Ohms. Temperature-dependent specific heat measurements on the MnSb\u003csub\u003e2\u003c/sub\u003e in a mass of about 6 mg polycrystalline sample were carried out using a Quantum Design, Physical Property Measurement System (PPMS DynaCool) in the temperature range of 200-280 K ( H grease), 150 K- 280 K (N grease with addenda measurement points that are the same as the sample measurement), 107 K-127 K( N grease), and 4 K- 200 K (N grease).\u0026nbsp;\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eNeutron Powder Diffraction:\u003c/strong\u003e To determine whether magnetic ordering exists, neutron powder diffraction (NPD) measurements were performed using a time-of-flight powder diffractometer, POWGEN, at the Spallation Neutron Source at Oak Ridge National Laboratory. Approximately 2.6 g of samples were prepared after grinding several single crystals to a fine powder and passing them through a 45\u0026micro;m mesh sieve. Diffraction patterns were collected at 308 K for 2 hours 36 minutes using a neutron beam with a center wavelength of 1.5. Rietveld refinements using GSAS-II software\u003csup\u003e47\u003c/sup\u003e and Fullprof suite\u003csup\u003e48\u0026nbsp;\u003c/sup\u003ewere performed to determine the crystal and magnetic structures, respectively. Determination of the magnetic structure was performed on HB-2A POWDER beamline at the High-Flux Isotope Reactor (HFIR) located at Oak Ridge National Lab (ORNL). Roughly 1 g of MnSb\u003csub\u003e2\u003c/sub\u003e was loaded into an aluminum can backfilled with He. Diffraction patterns were measured with a vertically focused Ge monochromator to select the 2.41 \u0026Aring; wavelength while a collimation of open-open-12 was used. Magnetic structure analysis was performed with SARAh Representation Analysis and SARAh Refine and refined with the Fullprof suite software\u003csup\u003e49\u003c/sup\u003e.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eNuclear Magnetic Resonance:\u003c/strong\u003e Nuclear magnetic resonance (NMR) measurements of \u003csup\u003e55\u003c/sup\u003eMn (nuclear spin \u003cem\u003eI\u003c/em\u003e = 5/2, gyromagnetic ratio\u0026nbsp;g\u003csub\u003eN\u003c/sub\u003e/2p\u0026nbsp;=\u0026nbsp;10.50\u0026nbsp;MHz/T), \u003csup\u003e121\u003c/sup\u003eSb (\u003cem\u003eI\u003c/em\u003e = 5/2,\u0026nbsp;g\u003csub\u003eN\u003c/sub\u003e/2p\u0026nbsp;=10.189\u0026nbsp;MHz/T), \u0026nbsp;and \u003csup\u003e123\u003c/sup\u003eSb (\u003cem\u003eI\u003c/em\u003e = 7/2,\u0026nbsp;g\u003csub\u003eN\u003c/sub\u003e/2p\u0026nbsp;=5.517\u0026nbsp;MHz/T) \u0026nbsp;nuclei were conducted using a laboratory-built phase-coherent spin-echo pulse spectrometer on polycrystalline powder samples. The NMR spectrum was obtained under magnetic fields by sweeping the magnetic field at a fixed NMR frequency of 67 MHz, while the zero magnetic field NMR spectrum was measured by plotting spin-echo intensity as a function of NMR frequency.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eDFT Calculation:\u003c/strong\u003e Density Functional Theory (DFT) calculations were carried out using version 7.3.1 of the Quantum ESPRESSO package to evaluate the total energies of MnSb\u003csub\u003e2\u003c/sub\u003e in non-magnetic, ferromagnetic, and antiferromagnetic configurations.\u003csup\u003e50\u003c/sup\u003e The calculations employed ultrasoft pseudopotentials and the Perdew-Burke-Ernzerhof (PBE) exchange-correlation functional within the generalized gradient approximation (GGA).\u003csup\u003e51\u0026ndash;53\u003c/sup\u003e A plane-wave kinetic energy cutoff of 300 Ry was used, with a charge density cutoff set to 3600 Ry (12 times the wavefunction cutoff). Brillouin zone integration was performed using a 7\u0026times;7\u0026times;13 Monkhorst-Pack k-point grid.\u003csup\u003e54\u003c/sup\u003e Total energy convergence was ensured with a threshold of less than 1 meV per atom. The electronic self-consistency was achieved using the Davidson diagonalization algorithm, with a convergence criterion of 10\u003csup\u003e-9\u003c/sup\u003e Ry.\u003csup\u003e55\u003c/sup\u003e High-symmetrical \u003cem\u003ek\u003c/em\u003e-point paths for band structure calculations were generated using the Spglib library.\u003csup\u003e56,57\u003c/sup\u003e\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e\u003cstrong\u003eAuthor Contributions\u003c/strong\u003e \u0026nbsp;\u003c/p\u003e\n\u003cp\u003eW.X. conceived the research idea. M.X. carried out experimental synthesis and physical property characterization. M.B., Q.Z., and D.Y. performed neutron scattering experiments and analysis. Q.-P.D. and Y.F. conducted solid-state NMR measurements and analysis. P.C. performed the simulations. A.S., S.B., and R.R. contributed to physical property measurements, data analysis, and manuscript preparation. W.X. and P.C. supervised the project. All authors discussed the results and contributed to the final manuscript.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eFunding\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThis work was primarily supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award DE-SC-0023648 (Michigan State University) to Weiwei Xie. Work carried out at Ames National Laboratory was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. Ames National Laboratory is operated for the U.S. Department of Energy by Iowa State University under Contract DE-AC02-07CH11358 to Paul Canfield. C.P. in the Weiwei Xie group was supported by the National Science Foundation under Grant NSF-DMR-2422361 (to Weiwei Xie). A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by Oak Ridge National Laboratory. M. B. in the Weiwei Xie group was supported by the DOE Office of Science Graduate Student Research Program, administered by the Oak Ridge Institute for Science and Education (ORISE) for the U.S. Department of Energy. ORISE is managed by Oak Ridge Associated Universities under Contract DE-SC0014664. The views expressed in this work are those of the authors and do not necessarily reflect the policies of the U.S. Department of Energy, ORAU, or ORISE. No animals were used in this research.\u003cstrong\u003e\u0026nbsp;\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eConflict of Interest\u003c/strong\u003e\u003cstrong\u003es\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe authors have no relevant financial or non‐financial interests to disclose.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\n\u003cli\u003e\u0026Scaron;mejkal, L.; Sinova, J.; Jungwirth, T. Beyond Conventional Ferromagnetism and Antiferromagnetism: A Phase with Nonrelativistic Spin and Crystal Rotation Symmetry. \u003cem\u003ePhys. Rev. X\u003c/em\u003e \u003cstrong\u003e2022\u003c/strong\u003e, \u003cem\u003e12\u003c/em\u003e (3), 031042. https://doi.org/10.1103/PhysRevX.12.031042.\u003c/li\u003e\n\u003cli\u003eMa, H.-Y.; Hu, M.; Li, N.; Liu, J.; Yao, W.; Jia, J.-F.; Liu, J. Multifunctional Antiferromagnetic Materials with Giant Piezomagnetism and Noncollinear Spin Current. \u003cem\u003eNat. 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Spglib: A Software Library for Crystal Symmetry Search. \u003cem\u003eScience and Technology of Advanced Materials: Methods\u003c/em\u003e \u003cstrong\u003e2024\u003c/strong\u003e, \u003cem\u003e4\u003c/em\u003e (1). https://doi.org/10.1080/27660400.2024.2384822.\u003c/li\u003e\n\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":false,"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":"npj-quantum-materials","isNatureJournal":false,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"npjquantmats","sideBox":"Learn more about [npj Quantum Materials](http://www.nature.com/npjquantmats/)","snPcode":"41535","submissionUrl":"https://mts-npjquantmats.nature.com/cgi-bin/main.plex","title":"npj Quantum Materials","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"ejp","reportingPortfolio":"NPJ","inReviewEnabled":true,"inReviewRevisionsEnabled":true},"keywords":"","lastPublishedDoi":"10.21203/rs.3.rs-8980468/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-8980468/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eMarcasite-type compounds have been proposed as promising hosts of exotic magnetic quantum states, yet experimental realizations in stoichiometric, disorder-free systems remain limited. Here, we report the high-pressure stabilization and magnetic characterization of MnSb\u003csub\u003e2\u003c/sub\u003e, a marcasite-type compound that is thermodynamically metastable under ambient pressure. Single crystals were synthesized using a cubic multi-anvil press, and powder and single-crystal X-ray diffraction confirm the orthorhombic \u003cem\u003ePnnm\u003c/em\u003e structure. These crystals are stable at ambient pressure for a long time up to between 450\u0026ndash;500 K. Heat-capacity measurements reveal phase transitions at approximately 220 K and 118 K. Neutron diffraction uncovers an unconventional magnetic ground state below 220 K. Magnetic powder neutron diffraction refinements reveal possible multiple magnetic configurations that provide comparably acceptable fits to the experimental data. While most solutions are consistent with a spin-density-wave (SDW) description, helical models systematically yield inferior agreement factors. Across a broad range of models, the Mn ordered moment reaches a maximum value of approximately 2 \u0026micro;\u003csub\u003eB\u003c/sub\u003e and remains predominantly collinear, with minimal canting along the \u003cem\u003ec\u003c/em\u003e-axis. At 200 K, the magnetic propagation vector is \u003cem\u003eq\u003c/em\u003e = (0, 0.3975, 0.3783); upon cooling, the \u003cem\u003eb\u003c/em\u003e component increases toward 0.5, reflecting a temperature-dependent evolution of the modulation. The need for modification of the magnetic model between high and low temperatures further highlights the complex and strongly temperature-dependent nature of the magnetic order in this system. These results establish MnSb\u003csub\u003e2\u003c/sub\u003e as a pressure-stabilized marcasite magnet with a highly tunable, complex magnetic ground state and a compelling stoichiometric platform for exploring unconventional magnetic behavior, including potential altermagnetism.\u003c/p\u003e","manuscriptTitle":"Pressure-Stabilized MnSb2 with Complex Incommensurate Magnetic Order","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2026-03-18 12:33:55","doi":"10.21203/rs.3.rs-8980468/v1","editorialEvents":[{"type":"communityComments","content":0},{"type":"reviewerAgreed","content":"200531492779814649643180988095151110077","date":"2026-05-18T12:19:15+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"333620623914391275207146142110999250830","date":"2026-05-18T07:37:10+00:00","index":"hide","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2026-04-10T18:08:01+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"248506564538084566267591026639431567924","date":"2026-03-23T15:40:24+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"109525674665451842394135204051713886309","date":"2026-03-21T13:34:13+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"234650925967064124410423613894092730735","date":"2026-03-21T07:22:40+00:00","index":"hide","fulltext":""},{"type":"reviewersInvited","content":"","date":"2026-03-16T05:45:23+00:00","index":"","fulltext":""},{"type":"editorAssigned","content":"","date":"2026-03-12T03:32:22+00:00","index":"","fulltext":""},{"type":"checksComplete","content":"","date":"2026-03-11T03:28:59+00:00","index":"","fulltext":""},{"type":"submitted","content":"npj Quantum Materials","date":"2026-02-26T17:27:27+00:00","index":"","fulltext":""}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"npj-quantum-materials","isNatureJournal":false,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"npjquantmats","sideBox":"Learn more about [npj Quantum Materials](http://www.nature.com/npjquantmats/)","snPcode":"41535","submissionUrl":"https://mts-npjquantmats.nature.com/cgi-bin/main.plex","title":"npj Quantum Materials","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"ejp","reportingPortfolio":"NPJ","inReviewEnabled":true,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"add7dab2-e1ae-4415-8edf-f60e8664a156","owner":[],"postedDate":"March 18th, 2026","published":true,"recentEditorialEvents":[{"type":"reviewerAgreed","content":"200531492779814649643180988095151110077","date":"2026-05-18T12:19:15+00:00","index":27,"fulltext":""},{"type":"reviewerAgreed","content":"333620623914391275207146142110999250830","date":"2026-05-18T07:37:10+00:00","index":26,"fulltext":""}],"rejectedJournal":[],"revision":"","amendment":"","status":"under-review","subjectAreas":[{"id":64723863,"name":"Physical sciences/Materials science"},{"id":64723864,"name":"Physical sciences/Physics"}],"tags":[],"updatedAt":"2026-03-18T12:33:55+00:00","versionOfRecord":[],"versionCreatedAt":"2026-03-18 12:33:55","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-8980468","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-8980468","identity":"rs-8980468","version":["v1"]},"buildId":"XKTyCvWXoU3ODBz1xrDgd","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}