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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. 

Abstract Dirac and Weyl semimetals are a central topic of contemporary condensed matter physics, and the discovery of new compounds with Dirac/Weyl electronic states is crucial to the advancement of topological materials and quantum technologies. Here we show a widely applicable strategy that uses high configuration entropy to engineer relativistic electronic states. We take theAMnSb₂(A= Ba, Sr, Ca, Eu, and Yb) Dirac material family as an example and demonstrate that mixing of Ba, Sr, Ca, Eu and Yb at theAsite generates the compound (Ba_0.38Sr_0.14Ca_0.16Eu_0.16Yb_0.16)MnSb₂(denoted asA⁵MnSb₂), giving access to a polar structure with a space group that is not present in any of the parent compounds.A⁵MnSb₂is an entropy-stabilized phase that preserves its linear band dispersion despite considerable lattice disorder. Although bothA⁵MnSb₂andAMnSb₂have quasi-two-dimensional crystal structures, the two-dimensional Dirac states in the pristineAMnSb₂evolve into a highly anisotropic quasi-three-dimensional Dirac state triggered by local structure distortions in the high-entropy phase, which is revealed by Shubnikov–de Haas oscillations measurements. 

Abstract Strong coupling between polarization (P) and strain (ɛ) in ferroelectric complex oxides offers unique opportunities to dramatically tune their properties. Here colossal strain tuning of ferroelectricity in epitaxial KNbO₃thin films grown by sub‐oxide molecular beam epitaxy is demonstrated. While bulk KNbO₃exhibits three ferroelectric transitions and a Curie temperature (T_c) of ≈676 K, phase‐field modeling predicts that a biaxial strain of as little as −0.6% pushes itsT_c> 975 K, its decomposition temperature in air, and for −1.4% strain, toT_c> 1325 K, its melting point. Furthermore, a strain of −1.5% can stabilize a single phase throughout the entire temperature range of its stability. A combination of temperature‐dependent second harmonic generation measurements, synchrotron‐based X‐ray reciprocal space mapping, ferroelectric measurements, and transmission electron microscopy reveal a single tetragonal phase from 10 K to 975 K, an enhancement of ≈46% in the tetragonal phase remanent polarization (P_r), and a ≈200% enhancement in its optical second harmonic generation coefficients over bulk values. These properties in a lead‐free system, but with properties comparable or superior to lead‐based systems, make it an attractive candidate for applications ranging from high‐temperature ferroelectric memory to cryogenic temperature quantum computing. 

Abstract Discovery of new materials with enhanced optical properties in the visible and UV‐C range can impact applications in lasers, nonlinear optics, and quantum optics. Here, the optical floating zone growth of a family of rare earth borates,RBa₃(B₃O₆)₃(R= Nd, Sm, Tb, Dy, and Er), with promising linear and nonlinear optical (NLO) properties is reported. Although previously identified to be centrosymmetric, the X‐ray analysis combined with optical second harmonic generation (SHG) assigns the noncentrosymmetricPspace group to these crystals. Characterization of linear optical properties reveals a direct bandgap of ≈5.61–5.72 eV and strong photoluminescence in both the visible and mid‐IR regions. Anisotropic linear and nonlinear optical characterization reveals both Type‐I and Type‐II SHG phase matchability, with the highest effective phase‐matched SHG coefficient of 1.2 pm V⁻¹at 800‐nm fundamental wavelength (for DyBa₃(B₃O₆)₃), comparable to β‐BaB₂O₄(phase‐matchedd₂₂≈ 1.9 pm V⁻¹). Laser‐induced surface damage threshold for these environmentally stable crystals is 650–900 GW cm⁻², which is four to five times higher than that of β‐BaB₂O₄, thus providing an opportunity to pump with significantly higher power to generate about six to seven times stronger SHG light. Since the SHG arises from disorder on the Ba‐site, significantly larger SHG coefficients may be realized by “poling” the crystals to align the Ba displacements. These properties motivate further development of this crystal family for laser and wide bandgap NLO applications. 

Abstract Multifunctionality as a paradigm requires materials exhibiting multiple superior properties. Integrating second‐order optical nonlinearity and large bandgap with piezoelectricity can, for example, enable broadband, strain‐tunable photonics. Though very different phenomena at distinct frequencies, both second‐order optical nonlinearity and piezoelectricity are third‐rank polar tensors present only in acentric crystal structures. However, simultaneously enhancing both phenomena is highly challenging since it involves competing effects with tradeoffs. Recently, a large switchable ferroelectric polarization of ≈80 μC cm⁻²was reported in Zn_1‐xMg_xO films. Here, ferroelectric Zn_1‐xMg_xO is demonstrated to be a platform that hosts simultaneously a 30% increase in the electronic bandgap, a 50% enhancement in the second harmonic generation (SHG) coefficients, and a near 200% improvement in the piezoelectric coefficients over pure ZnO. These enhancements are shown to be due to a 400% increase in the electronic anharmonicity and a ≈200% decrease in the ionic anharmonicity with Mg substitution. Precisely controllable periodic ferroelectric domain gratings are demonstrated down to 800 nm domain width, enabling ultraviolet quasi‐phase‐matched optical harmonic generation as well as domain‐engineered piezoelectric devices. 

Abstract Superior infrared nonlinear optical (NLO) crystals are in urgent demand in the development of lasers and optical technologies for communications and computing. The critical challenge is to find a crystal with large non‐resonant phase‐matchable NLO coefficients and high laser damage threshold (LDTs) simultaneously, which however scale inversely. This work reports such a material, MgSiP_2,that exhibits a large second harmonic generation (SHG) coefficient ofd₁₄≈d₃₆= 89 ± 5 pm V⁻¹at 1550 nm fundamental wavelength, surpassing the commercial NLO crystals AgGaS₂, AgGaSe₂, and ZnGeP₂. First principles theory reveals the polarizability and geometric arrangement of the [SiP₄] tetrahedral units as the origin of this large nonlinear response. Remarkably, it also exhibits a high LDT value of 684 GW cm⁻², which is six times larger than ZnGeP₂and three times larger than CdSiP₂. It has a wide transparency window of 0.53–10.35 µm, allowing broadband tunability. Further, it is Type I and Type II phase‐matchable with large effective SHG coefficients ofd_eff,I≈80.2 pm V⁻¹andd_eff,II≈73.4 pm V⁻¹. The outstanding properties of MgSiP₂make it a highly attractive candidate for optical frequency conversion in the infrared. 

Abstract Recent advances in 2D magnetism have heightened interest in layered magnetic materials due to their potential for spintronics. In particular, layered semiconducting antiferromagnets exhibit intriguing low‐dimensional semiconducting behavior with both charge and spin as carrier controls. However, synthesis of these compounds is challenging and remains rare. Here, first‐principles based high‐throughput search is conducted to screen potentially stable mixed metal phosphorous trichalcogenides (MM^′P₂X₆, where M and M^′are transition metals and X is a chalcogenide) that have a wide range of tunable bandgaps and interesting magnetic properties. Among the potential candidates, a stable semiconducting layered magnetic material, CdFeP₂Se₆, that exhibits a short‐range antiferromagnetic order atT_N = 21 K with an indirect bandgap of 2.23 eV is successfully synthesized . This work suggests that high‐throughput screening assisted synthesis can be an effective method for layered magnetic materials discovery. 

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. 

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. 

The melting behavior of Ruddlesden-Popper type hybrid improper ferroelectric Sr3Zr2O7 phase in the ZrO2–SrO pseudo-binary system was investigated, and its single crystals were successfully grown. A series of the slowcooling floating zone experiments revealed that Sr3Zr2O7 melts incongruently into SrZrO3 phase and a liquid and that the compositional range where Sr3Zr2O7 and a liquid coexist is located around 70 mol% SrO composition. Based on the results, we attempted to grow Sr3Zr2O7 single crystals by the traveling solvent floating zone method using SrO-excess solvent and feed. Consequently, many small single crystals of Sr3Zr2O7 phase with several millimeters in size were discovered in the as-grown boules covered with SrO phase. The phase transition behavior of the grown crystals was investigated by differential thermal analysis with polarizing optical microscopy as well as by optical second harmonic generation measurements. We directly observed a reconstruction of orthorhombic twin domains in Sr3Zr2O7 single crystals accompanied by the first-order ferroelectric transition at about 410 ◦C.