Van Der Waals Epitaxy Research Articles

Scalable approach for growing hexagonal boron nitride on silicon and its role in III-nitride van der Waals epitaxy

Hexagonal boron nitride (h-BN) stands out among 2D materials for its insulating properties, making it promising for the integration of 2D and 3D materials. However, achieving wafer-scale growth on silicon substrates remains a significant challenge. In this study, growth strategies for depositing h-BN on Si substrates are explored utilizing the wafer scalable metalorganic chemical vapor deposition. Our investigations reveal that employing a pulsed flow mode scheme is preferable over the conventional continuous flow mode scheme in growing h-BN thin films on 150 mm Si substrates. The as-grown h-BN film on Si exhibits uniform coverage with h-BN[0001]//Si[111]. With the successful wafer-scale growth of h-BN on Si, its role in aiding the van der Waals epitaxy of III-nitrides on Si substrates and subsequent epitaxial lift-off (ELO) of III-nitrides is further exemplified. An optimized h-BN thickness for the ELO process is also determined.

High-κ monocrystalline dielectrics for low-power two-dimensional electronics.

The downscaling of complementary metal-oxide-semiconductor technology has produced breakthroughs in electronics, but more extreme scaling has hit a wall of device performance degradation. One key challenge is the development of insulators with high dielectric constant, wide bandgap and high tunnel masses. Here, we show that two-dimensional monocrystalline gadolinium pentoxide, which is devised through combining particle swarm optimization algorithm and theoretical calculations and synthesized via van der Waals epitaxy, could exhibit a high dielectric constant of ~25.5 and a wide bandgap simultaneously. A desirable equivalent oxide thickness down to 1 nm with an ultralow leakage current of ~10-4 A cm-2 even at 5 MV cm-1 is achieved. The molybdenum disulfide transistors gated by gadolinium pentoxide exhibit high on/off ratios over 108 and near-Boltzmann-limit subthreshold swing at an operation voltage of 0.5 V. We also constructed inverter circuits with high gain and nanowatt power consumption. This reliable approach to integrating ultrathin monocrystalline insulators paves the way to future nanoelectronics.

Transferrable GaN-based Micro-LED heterostructures grown on h-BN for optogenetic applications

Individually transferrable GaN-based MQWs micro-LED structures grown on two-dimensional (2D) hexagonal boron nitride (h-BN) have been demonstrated. Different sizes (60 × 30 µm, 60 × 60 µm, 90 × 60 µm and 90 × 90 µm) of GaN-based LED heterostructures on layered h-BN were grown on dielectric SiN patterned sapphire substrates using Metal Organic Vapor Phase Epitaxy (MOVPE). Scanning electron microscope (SEM) images show micro-LEDs were grown with high selectivity within the mask opening areas. Consistent MQWs emission from micro-LEDs was observed at 452 ± 2 nm by cathodoluminescence (CL) spectroscopy for all micro-LED sizes. The structural and optical quality were similar to the GaN-based-LEDs grown on unpatterned substrates. In addition, we have successfully demonstrated the lift-off and transfer of individual micro-LEDs to arbitrary flexible templates using a transfer printing machine, which can be addressed by full front-end process. These studies highlight the role of combination of van der Waals (vdW) epitaxy and selective area growth (SAG) in facilitating the direct realization of dimensionally defined III-Nitride micro-LED structures and the mechanical release and transfer of these micro-LEDs to templates suitable for flexible display and optogenetics applications.

Conventional epitaxy of NiO thin films on muscovite mica and c-Al2O3 substrates

Fiber-textured and epitaxial NiO thin films were deposited on Si(100), c-Al2O3, and muscovite mica(001) substrates using reactive magnetron sputtering at substrate temperatures of 300°C and 400°C, to investigate the effect of film thickness and substrate temperature on epitaxial growth of NiO films. The as-deposited films exhibited a face-centered cubic structure with a larger lattice constant, attributed to strain induced during the sputtering process. With an increase in substrate temperature to 400°C, the d-spacing decreased due to strain release, approaching the NiO bulk value for the thickest film. The NiO film grown on Si(100) displayed fiber texture. On c-plane sapphire, NiO thin films exhibited twin domains and three-fold symmetry, consistent with expected crystallographic orientation relationship for NaCl-structured materials on sapphire:(111)NiO∥(0001)Al2O3and[01¯1]NiO∥[1¯010]Al2O3, [011¯]NiO∥[101¯0]Al2O3. On muscovite mica(001) substrates, the observed epitaxial shows that the mechanism is conventional epitaxy, rather than van der Waals epitaxy, consistent with the epitaxial growth of the non-layered non-van-der-Waals compound NiO. The epitaxial relationship was identified as of (111)NiO∥(001)Mica and [01¯1]NiO∥[010]Mica, [011¯]NiO∥[01¯0]Mica.

Van der Waals epitaxial growth of single-crystal molecular film.

Epitaxy is the cornerstone of semiconductor technology, enabling the fabrication of single-crystal film. Recent advancements in van der Waals (vdW) epitaxy have opened new avenues for producing wafer-scale single-crystal 2D atomic crystals. However, when it comes to molecular crystals, the overall weak vdW force means that it is a significant challenge for small molecules to form a well-ordered structure during epitaxy. Here we demonstrate that the vdW epitaxy of Sb2O3 molecular crystal, where the whole growth process is governed by vdW interactions, can be precisely controlled. The nucleation is deterministically modulated by epilayer-substrate interactions and unidirectional nuclei are realized through designing the lattice and symmetry matching between epilayer and substrate. Moreover, the growth and coalescence of nuclei as well as the layer-by-layer growth mode are kinetically realized via tackling the Schwoebel-Ehrlich barrier. Such precise control of vdW epitaxy enables the growth of single-crystal Sb2O3 molecular film with desirable thickness. Using the ultrathin highly oriented Sb2O3 film as a gate dielectric, we fabricated MoS2-based field-effect transistors that exhibit superior device performance. The results substantiate the viability of precisely managing molecule alignment in vdW epitaxy, paving the way for large-scale synthesis of single-crystal 2D molecular crystals.

Mechanisms of Controllable Growth and Ohmic Contact of Two-Dimensional Molybdenum Disulfide: Insight from Atomistic Simulations.

ConspectusTwo-dimensional (2D) semiconducting transition metal dichalcogenides (TMDs), in particular molybdenum disulfide (MoS2), have recently attracted huge interest due to their proper bandgap, high mobility at 2D limit, and easy-to-integrate planar structure, which are very promising for extending Moore's law in postsilicon electronics technology. Great effort has been devoted toward such a goal since the demonstration of protype MoS2 devices with high room-temperature on/off current ratios, ultralow standby power consumption, and atomic level scaling capacity down to sub-1-nm technology node. However, there are still several key challenges that need to be addressed prior to the real application of MoS2-based electronics technology. The controllable growth of wafer-scale single-crystal MoS2 on industry-compatible insulating substrates is the prerequisite of application while the currently synthesized MoS2 films mostly are polycrystalline with limited sizes of single-crystal domains and may involve metal substrates. The precise layer-control is also very important for MoS2 growth since its electronic properties are layer-dependent, whereas the layer-by-layer growth of multilayer MoS2 dominated by the van der Waals (vdW) epitaxy leads to poor thickness uniformity and noncontinuously distributed domains. High density up to 1013 cm-2 of sulfur vacancies (SVs) in grown MoS2 can cause unfavorable carrier scatting and electronic properties variations and will inevitably disturb the device performance. The dangling-bond-free surface of MoS2 gives rise to an inherent vdW gap at metal-semiconductor (M-S) contact, which leads to high electrical resistance and poor current-delivery capability at the contact interface and thereby substantially limits the performances of MoS2 devices.In this Account, we briefly review recent experimental and theoretical attempts for addressing the aforementioned challenges and present our own insights from atomistic simulations. We theoretically revealed the vital role of substrate steps for guiding unidirectional nucleation of monolayer MoS2 and uniform nucleation and edge-aligned growth of bilayer MoS2 by advanced simulations. The established thermodynamic mechanisms have successfully directed the experimental works on the controllable growth of 2 in. single-crystal monolayer and centimeter-scale uniform bilayer MoS2. The postgrowth repair mechanism of SV defect in MoS2 via thiol chemistry treatment has been theoretically explored with the consideration of side reaction of surface functionalization to help experimentally reduce SV defect density by 75%. Beyond the atomic level understanding, theoretical simulations proposed the electronic states hybridization mechanism across the semimetal-MoS2 vdW interface, thereby guiding experimental effort for realizing Ohmic contact at the MoS2-Sb(0112) vdW interface with record-low contact resistance.These advances provide a sound basis with an atomic-level understanding for addressing the related issues. However, there are still notable gaps in terms of system size and time scale of dynamics between atomistic simulations and experimental observations for the studies of MoS2 growth and interfaces. The combination of multiscale simulations and artificial intelligence technology is expected to narrow these gaps and provide a more insightful understanding of the controllable growth and interfacial properties modulation of MoS2. We conclude the Account with the standing challenges and outlook on future research directions from the theoretical perspective.

Revisiting the Epitaxial Growth Mechanism of 2D TMDC Single Crystals.

Epitaxial growth of 2D transition metal dichalcogenides (TMDCs) on sapphire substrates has been recognized as a pivotal method for producing wafer-scale single-crystal films. Both step-edges and symmetry of substrate surfaces have been proposed as controlling factors. However, the underlying fundamental still remains elusive. In this work, through the molybdenum disulfide (MoS2) growth on C/M sapphire, it is demonstrated that controlling the sulfur evaporation rate is crucial for dictating the switch between atomic-edge guided epitaxy and van der Waals epitaxy. Low-concentration sulfur condition preserves O/Al-terminated step edges, fostering atomic-edge epitaxy, while high-concentration sulfur leads to S-terminated edges, preferring van der Waals epitaxy. These experiments reveal that on a 2 in. wafer, the van der Waals epitaxy mechanism achieves better control in MoS2 alignment (≈99%) compared to the step edge mechanism (<85%). These findings shed light on the nuanced role of atomic-level thermodynamics in controlling nucleation modes of TMDCs, thereby providing a pathway for the precise fabrication of single-crystal 2D materials on a wafer scale.

Cold Seeded Epitaxy and Flexomagnetism in GdAuGe Membranes Exfoliated From Graphene/Ge(111).

Remote and van der Waals epitaxy are promising approaches for synthesizing single crystalline membranes for flexible electronics and discovery of new properties via extreme strain; however, a fundamental challenge is that most materials do not wet the graphene surface. We develop a cold seed approach for synthesizing smooth intermetallic films on graphene that can be exfoliated to form few nanometer thick single crystalline membranes. Our seeded GdAuGe films have narrow X-ray rocking curve widths of 9-24 arc seconds, which is 2 orders of magnitude lower than their counterparts grown by typical high temperature methods, and have atomically sharp interfaces observed by transmission electron microscopy. Upon exfoliation and rippling, strain gradients in GdAuGe membranes induce an antiferromagnetic to ferri/ferromagnetic transition. Our smooth, ultrathin membranes provide a clean platform for discovering new flexomagnetic effects in quantum materials.

(Invited) Phase Engineering for Enhanced Stability of Perovskite Nanowire Optoelectronics

The crystallization of halide perovskites (HPs) into one-dimensional structures has generated considerable research interest for their promising prospects in studying electron transport characteristics and multifunctional nanoscale devices. Various strategies have been developed to achieve in-plane growth of one-dimensional (1D) structures, including epitaxy, capillary-bridge-manipulated graphoepitaxy, and van der Waals epitaxy. Typically, the VLS growth mode, which involves the initial seeding of metallic catalytic nanoparticles to facilitate the process, has realized the out-of-plane and bottom-up synthesis route, opening up a new pathway for the one-dimensional perovskite electronics and optoelectronics.Among many recent advances, Zinc (Zn) has become a significant suppressor of vacancy formation in halide perovskites, establishing its pivotal role in defect engineering for these materials. Herein, we report the Zn-catalyzed vapor-liquid-solid (VLS) route to render black-phase CsPbI3 nanowires operationally stable at room temperature. Based on first-principle calculations, the doped Zn2+ can not only lead to the partial crystal lattice distortion but also reduce the formation energy value from the black phase to the yellow phase, improving the stability of the desired black phase. A series of contrast tests further confirm the stabilization effect of the Zn-doped strategy. Besides, the polarization-sensitive characteristics of black phase CsPbI3 nanowires were revealed. Our work highlights the importance of phase stabilization engineering for CsPbI3 nanowires and their potential applications in anisotropic optoelectronics.

Advancements and Challenges in the Integration of Indium Arsenide and Van der Waals Heterostructures.

The strategic integration of low-dimensional InAs-based materials and emerging van der Waals systems is advancing in various scientific fields, including electronics, optics, and magnetics. With their unique properties, these InAs-based van der Waals materials and devices promise further miniaturization of semiconductor devices in line with Moore's Law. However, progress in this area lags behind other 2D materials like graphene and boron nitride. Challenges include synthesizing pure crystalline phase InAs nanostructures and single-atomic-layer 2D InAs films, both vital for advanced van der Waals heterostructures. Also, diverse surface state effects on InAs-based van der Waals devices complicate their performance evaluation. This review discusses the experimental advances in the van der Waals epitaxy of InAs-based materials and the working principles of InAs-based van der Waals devices. Theoretical achievements in understanding and guiding the design of InAs-based van der Waals systems are highlighted. Focusing on advancing novel selective area growth and remote epitaxy, exploring multi-functional applications, and incorporating deep learning into first-principles calculations are proposed. These initiatives aim to overcome existing bottlenecks and accelerate transformative advancements in integrating InAs and van der Waals heterostructures.

MoS2-assisted growth of highly-oriented AlN thin films by low-temperature van der Waals epitaxy

Aluminum nitride (AlN) is a wide bandgap material used in acoustic devices, piezo- micro-electromechanical system and is promising for other electronic applications. However, for most applications, the AlN crystalline quality obtained by PVD or MOCVD is insufficient, and suitable growth substrates providing an adapted lattice match and coefficient of thermal expansion are limited. Alternatively, monocrystalline AlN wafers are not yet available in 200/300 mm sizes and suffer from high costs and quality issues. Here, we propose a novel approach involving a two-dimensional transition metal dichalcogenide (TMD) material as a seed layer, which displays an excellent lattice matching with AlN (&amp;gt;98%) allowing a strong enhancement in the c axis texture of sputtered AlN layers on Si(100)/SiO2 thermal oxide (500 nm) substrates. We have successfully demonstrated an eightfold improvement of the AlN (002) rocking curve compared to reference samples grown on thermal SiO2, thus providing a relevant and cost-effective process for the large-scale deployment of high-quality III-N materials on silicon-based substrates.

Realization of monolayer ZrTe5 topological insulators with wide band gaps

Two-dimensional topological insulators hosting the quantum spin Hall effect have application potential in dissipationless electronics. To observe the quantum spin Hall effect at elevated temperatures, a wide band gap is indispensable to efficiently suppress bulk conduction. Yet, most candidate materials exhibit narrow or even negative band gaps. Here, via elegant control of van der Waals epitaxy, we have successfully grown monolayer ZrTe5 on a bilayer graphene/SiC substrate. The epitaxial ZrTe5 monolayer crystalizes in two allotrope isomers with different intralayer alignments of ZrTe3 prisms. Our scanning tunneling microscopy/spectroscopy characterization unveils an intrinsic full band gap as large as 254 meV and one-dimensional edge states localized along the periphery of the ZrTe5 monolayer. First-principles calculations further confirm that the large band gap originates from strong spin−orbit coupling, and the edge states are topologically nontrivial. These findings thus provide a highly desirable material platform for the exploration of the high-temperature quantum spin Hall effect.

Van der Waals Epitaxial Growth of Ultrathin Indium Antimonide on Arbitrary Substrates through Low-Thermal Budget.

III-V semiconductors possess high mobility, high frequency response, and detection sensitivity, making them potentially attractive for beyond-silicon electronics applications. However, the traditional heteroepitaxy of III-V semiconductors is impeded by a significant lattice mismatch and the necessity for extreme vacuum and high temperature conditions, thereby impeding their in situ compatibility with flexible substrates and silicon-based circuits. In this study, a novel approach is presented for fabricating ultrathin InSb single-crystal nanosheets on arbitrary substrates with a thickness as thin as 2.4nm using low-thermal-budget van der Waals (vdW) epitaxy through chemical vapor deposition (CVD). In particular, in situ growth has been successfully achieved on both silicon-based substrates and flexible polyimide (PI) substrates. Notably, the growth temperature required for InSb nanosheets (240°C) is significantly lower than that employed in back-end-of-line processes (400°C). The field effect transistor devices based on fabricated ultrathin InSb nanosheets exhibit ultra-high on-off ratio exceeding 108 and demonstrate minimal gate leakage currents. Furthermore, these ultrathin InSb nanosheets display p-type characteristics with hole mobilities reaching up to 203 cm2 V-1 s-1 at room temperatures. This study paves the way for achieving heterogeneous integration of III-V semiconductors and facilitating their application in flexible electronics.

Epitaxial Growth of GaN Films on Chemical-Vapor-Deposited 2D MoS2 Layers by Plasma-Assisted Molecular Beam Epitaxy.

The van der Waals epitaxy of wafer-scale GaN on 2D MoS2 and the integration of GaN/MoS2 heterostructures were investigated in this report. GaN films have been successfully grown on 2D MoS2 layers using three different Ga fluxes via a plasma-assisted molecular beam epitaxy (PA-MBE) system. The substrate for the growth was a few-layer 2D MoS2 deposited on sapphire using chemical vapor deposition (CVD). Three different Ga fluxes were provided by the gallium source of the K-cell at temperatures of 825, 875, and 925 °C, respectively. After the growth, RHEED, HR-XRD, and TEM were conducted to study the crystal structure of GaN films. The surface morphology was obtained using FE-SEM and AFM. Chemical composition was confirmed by XPS and EDS. Raman and PL spectra were carried out to investigate the optical properties of GaN films. According to the characterizations of GaN films, the van der Waals epitaxial growth mechanism of GaN films changed from 3D to 2D with the increase in Ga flux, provided by higher temperatures of the K-cell. GaN films grown at 750 °C for 3 h with a K-cell temperature of 925 °C demonstrated the greatest crystal quality, chemical composition, and optical properties. The heterostructure of 3D GaN on 2D MoS2 was integrated successfully using the low-temperature PA-MBE technique, which could be applied to novel electronics and optoelectronics.

Stabilizing Phosphorene‐Like Group IV–VI Compounds via van der Waals Imprinting for Multistate Ferroelectricity and Tunable Spin Transport

AbstractLayered group IV–VI compounds (i.e., SnSe, SnS, GeSe, and GeS) in the puckered structure resembling black‐phosphorene (BlackP) have attracted increasing interest because of their intriguing ferroic orders and outstanding thermoelectric properties. By invoking the guiding principles of isovalency and isomorphism for promoting van der Waals epitaxy, and based on comprehensive first‐principles calculations, here it is shown that the typically metastable BlackP‐like GeTe can be readily stabilized on the (001) surface of isostructural SnSe. Importantly, the ferroelectricity of such a BlackP‐like GeTe monolayer can be substantially enhanced compared to the freestanding state, due to the substrate enlarged in‐plane polar displacements. The GeTe/SnSe heterobilayer exhibits multiple ferroelectric/ferrielectric polarization states, which can be exploited for high‐density memory devices. These mutually switchable polarization states are also shown to be internally locked with the spin polarization of the valence/conduction bands with pronounced Rashba spin‐orbit splitting and Berry curvature dipole. These findings highlight the intuitive yet enabling power of van der Waals imprinting in growing novel 2D materials for enriched functionalities.

Quasi van der Waals Epitaxy of Single Crystalline GaN on Amorphous SiO2/Si(100) for Monolithic Optoelectronic Integration.

The realization of high quality (0001) GaN on Si(100) is paramount importance for the monolithic integration of Si-based integrated circuits and GaN-enabled optoelectronic devices. Nevertheless, thorny issues including large thermal mismatch and distinct crystal symmetries typically bring about uncontrollable polycrystalline GaN formation with considerable surface roughness on standard Si(100). Here a breakthrough of high-quality single-crystalline GaN film on polycrystalline SiO2/Si(100) is presented by quasi van der Waals epitaxy and fabricate the monolithically integrated photonic chips. The in-plane orientation of epilayer is aligned throughout a slip and rotation of high density AlN nuclei due to weak interfacial forces, while the out-of-plane orientation of GaN can be guided by multi-step growth on transfer-free graphene. For the first time, the monolithic integration of light-emitting diode (LED) and photodetector (PD) devices are accomplished on CMOS-compatible SiO2/Si(100). Remarkably, the self-powered PD affords a rapid response below 250µs under adjacent LED radiation, demonstrating the responsivity and detectivity of 2.01×105 A/W and 4.64×1013Jones, respectively. This work breaks a bottleneck of synthesizing large area single-crystal GaN on Si(100), which is anticipated to motivate the disruptive developments in Si-integrated optoelectronic devices.

Van der Waals epitaxy of CsPbBr3/WSe2 heterostructure and dynamics study of exciton recombination

Van der Waals heterostructures formed by inorganic perovskites and transition metal dichalcogenides (TMDCs) have promising applications in photonics and optoelectronics. However, there are few studies on the properties of CsPbBr3/TMDC at low temperatures. Here, we demonstrate van der Waals epitaxy of CsPbBr3 nanowires (NWs), nanoplates (NPs) and nanocones (NCs) on monolayer (ML) WSe2, and investigate the lattice dynamics of the heterostructure at low temperatures using temperature-dependent Raman spectroscopy. In addition, temperature-dependent photoluminescence (PL) spectroscopy shows that the type II band alignment between CsPbBr3 and ML WSe2 leads to a broad emission peak at the low-energy side of the ML WSe2 emission at low temperatures. Meanwhile, a high-energy peak appears near the CsPbBr3 emission below 133 K, which may be related to the phase transition of CsPbBr3 from the cubic to the orthorhombic phase. These findings are important for the development of van der Waals heterostructure based self-powered photodetector with high performance.

Self-Assembly of Organic Semiconductors on Strained Graphene under Strain-Induced Pseudo-Electric Fields.

Graphene is used as a growth template for van der Waals epitaxy of organic semiconductor (OSC) thin films. During the synthesis and transfer of chemical-vapor-deposited graphene on a target substrate, local inhomogeneities in the graphene-in particular, a nonuniform strain field in the graphene template-can easily form, causing poor morphology and crystallinity of the OSC thin films. Moreover, a strain field in graphene introduces a pseudo-electric field in the graphene. Here, the study investigates how the strain and strain-induced pseudo-electric field of a graphene template affect the self-assembly of π-conjugated organic molecules on it. Periodically strained graphene templates are fabricated by transferring graphene onto an array of nanospheres and then analyzed the growth and nucleation behavior of C60 thin films on the strained graphene templates. Both experiments and a numerical simulation demonstrated that strained graphene reduced the desorption energy between the graphene and the C60 molecules and thereby suppressed both nucleation and growth of the C60. A mechanism is proposed in which the strain-induced pseudo-electric field in graphene modulates the binding energy of organic molecules on the graphene.

Transfer of III-nitride epitaxial layers onto pre-patterned silicon substrates for the simple fabrication of free-standing MEMS

In recent years, the remarkable properties and potential applications of III-nitride (III-N) semiconductors have sparked a significant interest in the field of microelectromechanical systems (MEMS). Traditionally, III-N MEMS are fabricated through a process involving the epitaxial growth of III-N epilayers on a silicon substrate followed by etching the handle wafer to generate free-standing structures. In this study, we explore the potential of a relatively simple approach based on the two-dimensional (2D) material-based liftoff and transfer to fabricate III-N mechanical resonators. The methodology involves van der Waals epitaxy of III-N layers on 2D hexagonal-boron nitride (h-BN), which leverages the weak van der Waals adhesion between h-BN layers to lift off and transfer these layers from their original growth substrate to an alternative host substrate. The employed method is demonstrated by fabricating 600 nm thick GaN/AlGaN and 2.5 μm thick h-BN micro-resonators onto pre-patterned cavities etched in silicon substrates. These devices are characterized using laser Doppler vibrometry, enabling the observation of well-defined modes of vibration and resonant frequencies. Furthermore, finite element method simulations are performed to gain insights into the experimental observations and the mechanical properties of the transferred layers. This approach could be extended to transfer high-quality III-N MEMS devices onto various host substrates, including flexible substrates, and could be used to assess the mechanical properties of emerging III-N semiconductor materials.

Van der Waals Epitaxial Growth of One-Unit-Cell-Thick Ferroelectric CuCrS2 Nanosheets.

Ferroelectric two-dimensional (2D) materials with a high transition temperature are highly desirable for new physics and next-generation memory electronics. However, the long-range polar order of ferroelectrics will barely persist when the thickness reaches the nanoscale. In this work, we synthesized 2D CuCrS2 nanosheets with thicknesses down to one unit cell via van der Waals epitaxy in a chemical vapor deposition system. A combination of transmission electron microscopy, second-harmonic generation, and Raman spectroscopy measurements confirms the R3m space group and noncentrosymmetric structure. Switchable ferroelectric domains and obvious ferroelectric hysteresis loops were created and visualized by piezoresponse force microscopy. Theoretical calculation helps us understand the mechanism of ferroelectric switching in CuCrS2 nanosheets. Finally, we fabricated a ferroelectric memory device that achieves an on/off ratio of ∼102 and remains stable after 2000 s, indicating its applicability in novel nanoelectronics. Overall, 2D CuCrS2 nanosheets exhibit excellent ferroelectric properties at the nanoscale, showing great promise for next-generation devices.