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Multiferroic materials host both ferroelectricity and magnetism, offering potential for magnetic memory and spin transistor applications. Here, we report a multiferroic chalcogenide semiconductor Cu1−xMn1+ySiTe3(0.04 ≤x≤ 0.26; 0.03 ≤y≤ 0.15), which crystallizes in a polar monoclinic structure (Pmspace group). It exhibits a canted antiferromagnetic state below 35 kelvin, with magnetic hysteresis and remanent magnetization under 15 kelvin. We demonstrate multiferroicity and strong magnetoelectric coupling through magnetodielectric and magnetocurrent measurements. At 10 kelvin, the magnetically induced electric polarization reaches ~0.8 microcoulombs per square centimeter, comparable to the highest value in oxide multiferroics. We also observe possible room-temperature ferroelectricity. Given that multiferroicity is very rare among transition metal chalcogenides, our finding sets up a unique materials platform for designing multiferroic chalcogenides.more » « less
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Abstract Optical second harmonic generation (SHG) is a nonlinear optical effect widely used for nonlinear optical microscopy and laser frequency conversion. Closed-form analytical solution of the nonlinear optical responses is essential for evaluating materials whose optical properties are unknown a priori. A recent open-source code, ♯SHAARP.si, can provide such closed form solutions for crystals with arbitrary symmetries, orientations, and anisotropic properties at asingleinterface. However, optical components are often in the form of slabs, thin films on substrates, and multilayer heterostructures with multiple reflections of both the fundamental and up to ten different SHG waves at each interface, adding significant complexity. Many approximations have therefore been employed in the existing analytical approaches, such as slowly varying approximation, weak reflection of the nonlinear polarization, transparent medium, high crystallographic symmetry, Kleinman symmetry, easy crystal orientation along a high-symmetry direction, phase matching conditions and negligible interference among nonlinear waves, which may lead to large errors in the reported material properties. To avoid these approximations, we have developed an open-source package named Second Harmonic Analysis of Anisotropic Rotational Polarimetry in Multilayers (♯SHAARP.ml). The reliability and accuracy are established by experimentally benchmarking with both the SHG polarimetry and Maker fringes using standard and commonly used nonlinear optical materials as well as twisted 2-dimensional heterostructures.more » « less
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Liu, Zhiwen; Psaltis, Demetri; Shi, Kebin (Ed.)Optical Second Harmonic Generation (SHG) is a nonlinear optical effect widely used for nonlinear optical microscopy and laser frequency conversion. The closed-form analytical solution of the nonlinear optical responses is essential for evaluating the optical responses of new materials whose optical properties are unknown a priori. Many approximations have therefore been employed in the existing analytical approaches, such as slowly varying approximation, weak reflection of the nonlinear polarization, transparent medium, high crystallographic symmetry, Kleinman symmetry, easy crystal orientation along a high-symmetry direction, phase matching conditions and negligible interference among nonlinear waves, which may lead to large errors in the reported material properties. To avoid these approximations, we have developed an open-source package named Second Harmonic Analysis of Anisotropic Rotational Polarimetry (♯SHAARP) for single interface (si) and in multilayers (ml) for homogeneous crystals. The reliability and accuracy are established by experimentally benchmarking with both the SHG polarimetry and Maker fringes predicted from the package using standard materials. SHAARP.si and SHAARP.ml are available through GitHub https://github.com/Rui-Zu/SHAARP and https://github.com/bzw133/SHAARP.ml, respectively.more » « less
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The growth of layered 2D compounds is a key ingredient in finding new phenomena in quantum materials, optoelectronics, and energy conversion. Here, we report SnP2Se6, a van der Waals chiral (R3 space group) semiconductor with an indirect bandgap of 1.36 to 1.41 electron volts. Exfoliated SnP2Se6flakes are integrated into high-performance field-effect transistors with electron mobilities >100 cm2/Vs and on/off ratios >106at room temperature. Upon excitation at a wavelength of 515.6 nanometer, SnP2Se6phototransistors show high gain (>4 × 104) at low intensity (≈10−6W/cm2) and fast photoresponse (< 5 microsecond) with concurrent gain of ≈52.9 at high intensity (≈56.6 mW/cm2) at a gate voltage of 60 V across 300-nm-thick SiO2dielectric layer. The combination of high carrier mobility and the non-centrosymmetric crystal structure results in a strong intrinsic bulk photovoltaic effect; under local excitation at normal incidence at 532 nm, short circuit currents exceed 8 mA/cm2at 20.6 W/cm2.more » « less
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Nonlinear optical (NLO) crystals with superior properties are significant for advancing laser technologies and applications. Introducing rare earth metals to borates is a promising and effective way to modify the electronic structure of a crystal to improve its optical properties in the visible and ultraviolet range. In this work, we computationally discover inversion symmetry breaking in EuBa3(B3O6)3, which was previously identified as centric, and demonstrate noncentrosymmetry via synthesizing single crystals for the first time by the floating zone method. We determine the correct space group to beP6¯. The material has a large direct bandgap of 5.56 eV and is transparent down to 250 nm. The complete anisotropic linear and nonlinear optical properties were also investigated with ad11of ∼0.52 pm/V for optical second harmonic generation. Further, it is Type I and Type II phase matchable. This work suggests that rare earth metal borates are an excellent crystal family for exploring future deep ultraviolet (DUV) NLO crystals. It also highlights how first principles computations combined with experiments can be used to identify noncentrosymmetric materials that have been wrongly assigned to be centrosymmetric.more » « less
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Abstract Magnetic topological materials have recently emerged as a promising platform for studying quantum geometry by the nonlinear transport in thin film devices. In this work, an antiferromagnetic (AFM) semiconductor EuSc₂Te₄ as the first bulk crystal that exhibits quantum geometry‐driven nonlinear transport is reported. This material crystallizes into an orthorhombic lattice with AFM order below 5.2 K and a bandgap of less than 50 meV. The calculated band structure aligns with the angle‐resolved photoemission spectroscopy spectrum. The AFM order preserves combined space‐time inversion symmetry but breaks both spatial inversion and time‐reversal symmetry, leading to the nonlinear Hall effect (NLHE). Nonlinear Hall voltage measured in bulk crystals appears at zero field, peaks near the spin‐flop transition as the field increases, and then diminishes as the spin moments align into a ferromagnetic order. This field dependence, along with the scaling analysis of the nonlinear Hall conductivity, suggests that the NLHE of EuSc₂Te₄ involves contributions from quantum metric, in addition to extrinsic contributions, such as spin scattering and junction effects. Furthermore, this NLHE is found to have the functionality of broadband frequency mixing, indicating its potential applications in electronics. This work reveals a new avenue for studying magnetism‐induced nonlinear transport in magnetic materials.more » « less
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