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Field effect transistors based on 2D layered material have gained significant potential in emerging technologies, such as neuromorphic computing and ultrafast memory response for artificial intelligence applications. This study proposes a facile approach to fabricate an optoelectronic artificial synapse for neuromorphic computing and light‐decoding information system by utilizing the 2D heterostructure of CrSBr/PtS2 to overcome circuit complexity. The CrSBr layer serves as a trapping layer, while PtS2, mounted on top of CrSBr, acts as a channel layer. PtS2 exhibits n‐type semiconductor behavior with a hysteresis that varies with the thickness of the underlying CrSBr layer. The heterostructure device, featuring a 96.3 nm thick CrSBr layer, exhibited a large memory window of 11.9 V when the gate voltage is swept from −10 V to +10 V. Various synaptic behaviors are effectively demonstrated, including paired‐pulse facilitation, excitatory postsynaptic current, optical spike number and intensity‐dependent plasticity using laser light at a wavelength of 365 nm. The device achieves 26 distinct output signals depending on the intensity of the incident laser light, ranging from 10 to 385 mW cm−2, enabling its applications for light‐decoded information security systems. Thus, the investigation presents a unique approach to artificial intelligence and cybersecurity systems. [ABSTRACT FROM AUTHOR]

2D van der Waals (vdW) layered materials exhibit significant exciton binding energy and versatile stacking options, making them ideal for room‐temperature exciton‐polariton devices used in low‐threshold lasing, nonlinear optical switching, and quantum computing. However, most existing systems depend on external optical microcavities coupled with single monolayers, leading to limited controllability and increased costs. Here, external cavity‐free vdW magnet CrSBr crystals are presented that feature magnetically controllable self‐hybridized exciton‐polaritons that remain stable up to room temperature. The ultrastrong exciton‐photon coupling suppresses donor‐, phonon‐, and defect‐related emissions. Furthermore, the exciton‐polariton dispersion and emission spectra can be effectively controlled by adjusting the magnetic field, temperature, and CrSBr thickness. This vdW exciton‐polariton material platform, demonstrating remarkable magnetic responsiveness in open cavity configurations under ambient conditions, paves the way for the development of compact, fast, and low‐loss spin, quantum, and magneto‐photonic devices. [ABSTRACT FROM AUTHOR]

The layered metamagnet CrSBr offers a rich interplay between magnetic, optical, and electrical properties that can be extended down to the two‐dimensional (2D) limit. Despite the extensive research regarding the long‐range magnetic order in magnetic van der Waals materials, short‐range correlations have been loosely investigated. By using small‐angle neutron scattering (SANS) the formation of short‐range magnetic regions in CrSBr with correlation lengths that increase upon cooling up to ≈3 nm at the antiferromagnetic ordering temperature (TN ≈ 140 K) is shown. Interestingly, these ferromagnetic correlations start developing below 200 K, i.e., well above TN. Below TN, these correlations rapidly decrease and are negligible at low‐temperatures. The experimental results are well‐reproduced by an effective spin Hamiltonian, which pinpoints that the short‐range correlations in CrSBr are intrinsic to the monolayer limit, and discard the appearance of any frustrated phase in CrSBr at low‐temperatures within the experimental window between 2 and 200 nm. Overall, the obtained results are compatible with a spin freezing scenario of the magnetic fluctuations in CrSBr and highlight SANS as a powerful technique for characterizing the rich physical phenomenology beyond the long‐range order paradigm offered by van der Waals magnets. [ABSTRACT FROM AUTHOR]

Understanding the stability limitations and defect formation mechanisms in 2D magnets is essential for their utilization in spintronic and memory technologies. Here, defects in monoto multilayer CrSBr are correlated with structural, vibrational, and magnetic properties. Resonant Raman scattering is used to reveal distinct vibrational defect signatures. In pristine CrSBr, it is shown that bromine atoms mediate vibrational interlayer coupling, allowing for distinguishing between surface and bulk defect modes. Environmental exposure is shown to cause drastic degradation in monolayers, with the formation of intralayer defects. This is in contrast to multilayers that predominantly show bromine surface defects. Through deliberate ion irradiation, the formation of defect modes is tuned: these are strongly polarized and resonantly enhanced, reflecting the quasi--1D electronic character of CrSBr. Strikingly, pronounced signatures of spin-phonon coupling ofthe intrinsic phonon modes and the ion beam-induced defect modes are observed throughout the magnetic transition temperature. Overall, defect engineering of magnetic properties is possible, with resonant Raman spectroscopy serving as a direct fingerprint of magnetic phases and defects in CrSBr. [ABSTRACT FROM AUTHOR]

CrSBr is a recently developed 2D van der Waals (vdW) magnet. However, this development is still in its infancy, and hence, there has been limited relevant research so far. In this study, ultrathin CrSBr is first prepared via blue‐tape‐based mechanical exfoliation. Subsequently, Raman and X‐ray photoelectron spectroscopy analyses are performed to obtain detailed information on the chemical structure. The thickness of most exfoliated samples measured using atomic force microscopy (AFM) is ≈1.6–6.5 nm corresponding to 2–8 layers. Notably, high‐resolution images of CrSBr atomic structures are seldom observed using transmission electron microscopy (TEM). Atomic‐thick CrSBr is extremely beam‐sensitive, and hence, it is easily damaged under e‐beam irradiation. Nevertheless, e‐beam damage provides an opportunity to study the structural properties of CrSBr. Different types of knock‐on effects are recorded and further analyzed using atomic‐scale imaging. Furthermore, the high‐resolution TEM images show that the unique atomic stepped boundary is consistent with the orthorhombic slip system. The recrystallization process of CrSBr and the formation/refilling of the nanoholes are recorded via in situ TEM. These findings deepen the understanding of the fundamental insight into 2D vdW magnetic semiconductors and pave the way for next‐generation spin‐based electronics. [ABSTRACT FROM AUTHOR]

Collective excitations of bound electron-hole pairs, i.e., excitons, are ubiquitous in condensed matter systems, and it has been shown that they can strongly couple to other degrees of freedom, such as spin, orbital, and lattice. Among van der Waals materials with pronounced excitonic responses, CrSBr has attracted significant interest due to a very large energy shift of its fundamental bright exciton (at 1.36 eV) under an external magnetic field. This effect has been associated with an increased interlayer electronic hopping when the magnetic order is switched from antiferromagnetic to ferromagnetic by an external magnetic field, enabling its optical detection. In this work, we report the observation of a second bright excitonic resonance (at 1.76 eV), displaying a 5-fold enhancement of the magnetically induced energy shift to ∼100 meV, which we associate to a decreased spatial localization and increased interband nature compared to the fundamental exciton. Moreover, we show how the light-matter interaction reaches the ultrastrong regime where this exciton hybridizes with the cavity modes of photons confined to CrSBr flakes, forming polaritons with a Rabi splitting of ℏ Ω R ≃ 372 meV, of the same order of magnitude as the one reported for the first exciton. These results expand the understanding of the relationship between the optical response and band structure of CrSBr and clarify the essential ingredients for optimizing magneto-electronic coupling for applications.

Abstract CrSBr is a recently developed 2D van der Waals (vdW) magnet. However, this development is still in its infancy, and hence, there has been limited relevant research so far. In this study, ultrathin CrSBr is first prepared via blue‐tape‐based mechanical exfoliation. Subsequently, Raman and X‐ray photoelectron spectroscopy analyses are performed to obtain detailed information on the chemical structure. The thickness of most exfoliated samples measured using atomic force microscopy (AFM) is ≈1.6–6.5 nm corresponding to 2–8 layers. Notably, high‐resolution images of CrSBr atomic structures are seldom observed using transmission electron microscopy (TEM). Atomic‐thick CrSBr is extremely beam‐sensitive, and hence, it is easily damaged under e‐beam irradiation. Nevertheless, e‐beam damage provides an opportunity to study the structural properties of CrSBr. Different types of knock‐on effects are recorded and further analyzed using atomic‐scale imaging. Furthermore, the high‐resolution TEM images show that the unique atomic stepped boundary is consistent with the orthorhombic slip system. The recrystallization process of CrSBr and the formation/refilling of the nanoholes are recorded via in situ TEM. These findings deepen the understanding of the fundamental insight into 2D vdW magnetic semiconductors and pave the way for next‐generation spin‐based electronics.

2D magnets represent material systems in which magnetic order and topological phase transitions can be observed. Based on these phenomena, novel types of computing architectures and magnetoelectronic devices can be envisaged. Unlike conventional magnetic films, their magnetism is independent of the substrate and interface qualities, and 2D magnetic properties manifest even in formally bulk single crystals. However, 2D magnetism in layered materials is rarely reported often due to weak exchange interactions and magnetic anisotropy, and low magnetic transition temperatures. Here, the electron spin resonance (ESR) properties of a layered antiferromagnetic CrSBr single crystal are reported. The W‐like shape angular dependence of the ESR linewidth provides a signature for room temperature spin–spin correlations and for the XY spin model. By approaching the Néel temperature the arising of competing intralayer ferromagnetic and interlayer antiferromagnetic interactions might lead to the formation of vortex and antivortex pairs. This argument is inferred by modeling the temperature dependence of the ESR linewidth with the topological Berezinskii‐Kosterlitz‐Thouless phase transition. These findings together with the chemical stability and semiconducting properties, make CrSBr a promising layered magnet for future magneto‐ and topological‐electronics. [ABSTRACT FROM AUTHOR]

Two-dimensional materials are extraordinarily sensitive to external stimuli, making them ideal for studying fundamental properties and for engineering devices with new functionalities. One such stimulus, strain, affects the magnetic properties of the layered magnetic semiconductor CrSBr to such a degree that it can induce a reversible antiferromagnetic-to-ferromagnetic phase transition. Using scanning SQUID-on-lever microscopy, we directly image the effects of spatially inhomogeneous strain on the magnetization of layered CrSBr, as it is polarized by a field applied along its easy axis. The evolution of this magnetization and the formation of domains is reproduced by a micromagnetic model, which incorporates the spatially varying strain and the corresponding changes in the local interlayer exchange stiffness. The observed sensitivity to small strain gradients along with similar images of a nominally unstrained CrSBr sample suggest that unintentional strain inhomogeneity influences the magnetic behavior of exfoliated samples.

Heat-to-charge conversion efficiency of thermoelectric materials is closely linked to the entropy per charge carrier. Thus, magnetic materials are promising building blocks for highly efficient energy harvesters as their carrier entropy is boosted by a spin degree of freedom. In this work, we investigate how this spin-entropy impacts heat-to-charge conversion in the A-type antiferromagnet CrSBr. We perform simultaneous measurements of electrical conductance and thermocurrent while changing magnetic order using the temperature and magnetic field as tuning parameters. We find a strong enhancement of the thermoelectric power factor at around the Néel temperature. We further reveal that the power factor at low temperatures can be increased by up to 600% upon applying a magnetic field. Our results demonstrate that the thermoelectric properties of 2D magnets can be optimized by exploiting the sizable impact of spin-entropy and confirm thermoelectric measurements as a sensitive tool to investigate subtle magnetic phase transitions in low-dimensional magnets.

van der Waals magnets are emerging as a promising material platform for electric field control of magnetism, offering a pathway toward the elimination of external magnetic fields from spintronic devices. A further step is the integration of such magnets with electrical gating components that would enable nonvolatile control of magnetic states. However, this approach remains unexplored for antiferromagnets, despite their growing significance in spintronics. Here, we demonstrate nonvolatile electric field control of magnetoelectric characteristics in van der Waals antiferromagnet CrSBr. We integrate a CrSBr channel in a flash-memory architecture featuring charge trapping graphene multilayers. The electrical gate operation triggers a nonvolatile 200% change in the antiferromagnetic state of CrSBr resistance by manipulating electron accumulation/depletion. Moreover, the nonvolatile gate modulates the metamagnetic transition field of CrSBr and the magnitude of magnetoresistance. Our findings highlight the potential of manipulating magnetic properties of antiferromagnetic semiconductors in a nonvolatile way.

Magnetic van der Waals heterostructures provide a unique platform to study magnetism and spintronics device concepts in the 2D limit. Here, studies of exchange bias from the van der Waals antiferromagnet CrSBr acting on the van der Waals ferromagnet Fe 3 GeTe 2 (FGT) are reported. The orientation of the exchange bias is along the in-plane easy axis of CrSBr, perpendicular to the out-of-plane anisotropy of the FGT, inducing a strongly tilted magnetic configuration in the FGT. Furthermore, the in-plane exchange bias provides sufficient symmetry breaking to allow deterministic spin-orbit torque switching of the FGT in CrSBr/FGT/Pt samples at zero applied magnetic field. A minimum thickness of the CrSBr of >10 nm is needed to provide a non-zero exchange bias at 30 K., (© 2024 Wiley‐VCH GmbH.)

The layered, air-stable van der Waals antiferromagnetic compound CrSBr exhibits pronounced coupling among its optical, electronic, and magnetic properties. As an example, exciton dynamics can be significantly influenced by lattice vibrations through exciton-phonon coupling. Using low-temperature photoluminescence spectroscopy, we demonstrate the effective coupling between excitons and phonons in nanometer-thick CrSBr. By careful analysis, we identify that the satellite peaks predominantly arise from the interaction between the exciton and an optical phonon with a frequency of 118 cm -1 (∼14.6 meV) due to the out-of-plane vibration of Br atoms. Power-dependent and temperature-dependent photoluminescence measurements support exciton-phonon coupling and indicate a coupling between magnetic and optical properties, suggesting the possibility of carrier localization in the material. The presence of strong coupling between the exciton and the lattice may have important implications for the design of light-matter interactions in magnetic semiconductors and provide insights into the exciton dynamics in CrSBr. This highlights the potential for exploiting exciton-phonon coupling to control the optical properties of layered antiferromagnetic materials.

Recent progress in polarization-resolved photodetection based on low-symmetry 2D materials has formed the basis of cutting-edge optoelectronic devices, including quantum optical communication, 3D image processing, and sensing applications. Here, we report an optical polarization-resolving photodetector (PD) fabricated from multilayer semiconducting CrSBr single crystals with high structural anisotropy. We have demonstrated self-powered photodetection due to the formation of Schottky junctions at the Au-CrSBr interfaces, which also caused the photocurrent to display a position-sensitive and binary nature. The self-biased CrSBr PD showed a photoresponsivity of ∼0.26 mA/W with a detectivity of 3.4 × 10 8 Jones at 514 nm excitation of fluency (0.42 mW/cm 2 ) under ambient conditions. The optical polarization-induced photoresponse exhibits a large dichroic ratio of 3.4, while the polarization is set along the a- and the b -axes of single-crystalline CrSBr. The PD also showed excellent stability, retaining >95% of the initial photoresponsivity in ambient conditions for more than five months without encapsulation. Thus, we demonstrate CrSBr as a fascinating material for ultralow-powered optical polarization-resolving optoelectronic devices for cutting-edge technology.

Recent advancements in 2D materials have revealed the potential of van der Waals magnets, and specifically of their magnetic anisotropy that allows applications down to the 2D limit. Among these materials, CrSBr has emerged as a promising candidate, because its intriguing magnetic and electronic properties have appeal for both fundamental and applied research in spintronics or magnonics. In this work, nano-SQUID-on-tip (SOT) microscopy is used to obtain direct magnetic imaging of CrSBr flakes with thicknesses ranging from monolayer (N = 1) to few-layer (N = 5). The ferromagnetic order is preserved down to the monolayer, while the antiferromagnetic coupling of the layers starts from the bilayer case. For odd layers, at zero applied magnetic field, the stray field resulting from the uncompensated layer is directly imaged. The progressive spin reorientation along the out-of-plane direction (hard axis) is also measured with a finite applied magnetic field, allowing evaluation of the anisotropy constant, which remains stable down to the monolayer and is close to the bulk value. Finally, by selecting the applied magnetic field protocol, the formation of Néel magnetic domain walls is observed down to the single-layer limit., (© 2023 The Authors. Advanced Materials published by Wiley-VCH GmbH.)

Correlated quantum phenomena in one-dimensional (1D) systems that exhibit competing electronic and magnetic order are of strong interest for the study of fundamental interactions and excitations, such as Tomonaga-Luttinger liquids and topological orders and defects with properties completely different from the quasiparticles expected in their higher-dimensional counterparts. However, clean 1D electronic systems are difficult to realize experimentally, particularly for magnetically ordered systems. Here, we show that the van der Waals layered magnetic semiconductor CrSBr behaves like a quasi-1D material embedded in a magnetically ordered environment. The strong 1D electronic character originates from the Cr-S chains and the combination of weak interlayer hybridization and anisotropy in effective mass and dielectric screening, with an effective electron mass ratio of m X ∼ 50. This extreme anisotropy experimentally manifests in strong electron-phonon and exciton-phonon interactions, a Peierls-like structural instability, and a Fano resonance from a van Hove singularity of similar strength to that of metallic carbon nanotubes. Moreover, because of the reduced dimensionality and interlayer coupling, CrSBr hosts spectrally narrow (1 meV) excitons of high binding energy and oscillator strength that inherit the 1D character. Overall, CrSBr is best understood as a stack of weakly hybridized monolayers and appears to be an experimentally attractive candidate for the study of exotic exciton and 1D-correlated many-body physics in the presence of magnetic order.e / m Y e ∼ 50. This extreme anisotropy experimentally manifests in strong electron-phonon and exciton-phonon interactions, a Peierls-like structural instability, and a Fano resonance from a van Hove singularity of similar strength to that of metallic carbon nanotubes. Moreover, because of the reduced dimensionality and interlayer coupling, CrSBr hosts spectrally narrow (1 meV) excitons of high binding energy and oscillator strength that inherit the 1D character. Overall, CrSBr is best understood as a stack of weakly hybridized monolayers and appears to be an experimentally attractive candidate for the study of exotic exciton and 1D-correlated many-body physics in the presence of magnetic order.

Atomic-level defects in van der Waals (vdW) materials are essential building blocks for quantum technologies and quantum sensing applications. The layered magnetic semiconductor CrSBr is an outstanding candidate for exploring optically active defects because of a direct gap, in addition to a rich magnetic phase diagram, including a recently hypothesized defect-induced magnetic order at low temperature. Here, we show optically active defects in CrSBr that are probes of the local magnetic environment. We observe a spectrally narrow (1 meV) defect emission in CrSBr that is correlated with both the bulk magnetic order and an additional low-temperature, defect-induced magnetic order. We elucidate the origin of this magnetic order in the context of local and nonlocal exchange coupling effects. Our work establishes vdW magnets like CrSBr as an exceptional platform to optically study defects that are correlated with the magnetic lattice. We anticipate that controlled defect creation allows for tailor-made complex magnetic textures and phases with direct optical access.

Magnetic van der Waals (vdW) materials possess versatile spin configurations stabilized in reduced dimensions. One magnetic order is the interlayer antiferromagnetism in A-type vdW antiferromagnet, which may be effectively modified by the magnetic field, stacking order, and thickness scaling. However, atomically revealing the interlayer spin orientation in the vdW antiferromagnet is highly challenging, because most of the material candidates exhibit an insulating ground state or instability in ambient conditions. Here, we report the layer-dependent interlayer antiferromagnetic spin reorientation in air-stable semiconductor CrSBr using magnetotransport characterization and first-principles calculations. We reveal an odd-even layer effect of interlayer spin reorientation, which originates from the competitions among interlayer exchange, magnetic anisotropy energy, and extra Zeeman energy of uncompensated magnetization. Furthermore, we quantitatively constructed the layer-dependent magnetic phase diagram with the help of a linear-chain model. Our work uncovers the layer-dependent interlayer antiferromagnetic spin reorientation engineered by magnetic field in the air-stable semiconductor.