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  1. Abstract

    Thin ferroelectric materials hold great promise for compact nonvolatile memory and nonlinear optical and optoelectronic devices. Herein, an ultrathin in‐plane ferroelectric material that exhibits a giant nonlinear optical effect, group‐IV monochalcogenide SnSe, is reported. Nanometer‐scale ferroelectric domains with ≈90°/270° twin boundaries or ≈180° domain walls are revealed in physical‐vapor‐deposited SnSe by lateral piezoresponse force microscopy. Atomic structure characterization reveals both parallel and antiparallel stacking of neighboring van der Waals ferroelectric layers, leading to ferroelectric or antiferroelectric ordering. Ferroelectric domains exhibit giant nonlinear optical activity due to coherent enhancement of second‐harmonic fields and the as‐resulted second‐harmonic generation was observed to be 100 times more intense than monolayer WS2. This work demonstrates in‐plane ferroelectric ordering and giant nonlinear optical activity in SnSe, which paves the way for applications in on‐chip nonlinear optical components and nonvolatile memory devices.

     
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  2. Abstract

    Nonlinear light–matter interaction, as the core of ultrafast optics, bulk photovoltaics, nonlinear optical sensing and imaging, and efficient generation of entangled photons, has been traditionally studied by first-principles theoretical methods with the sum-over-states approach. However, this indirect method often suffers from the divergence at band degeneracy and optical zeros as well as convergence issues and high computation costs when summing over the states. Here, using shift vector and shift current conductivity tensor as an example, we present a gauge-invariant generalized approach for efficient and direct calculations of nonlinear optical responses by representing interband Berry curvature, quantum metric, and shift vector in a generalized Wilson loop. This generalized Wilson loop method avoids the above cumbersome challenges and allows for easy implementation and efficient calculations. More importantly, the Wilson loop representation provides a succinct geometric interpretation of nonlinear optical processes and responses based on quantum geometric tensors and quantum geometric potentials and can be readily applied to studying other excited-state responses.

     
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  3. Abstract

    Nonlinear photocurrent in time-reversal invariant noncentrosymmetric systems such as ferroelectric semimetals sparked tremendous interest of utilizing nonlinear optics to characterize condensed matter with exotic phases. Here we provide a microscopic theory of two types of second-order nonlinear direct photocurrents, magnetic shift photocurrent (MSC) and magnetic injection photocurrent (MIC), as the counterparts of normal shift current (NSC) and normal injection current (NIC) in time-reversal symmetry and inversion symmetry broken systems. We show that MSC is mainly governed by shift vector and interband Berry curvature, and MIC is dominated by absorption strength and asymmetry of the group velocity difference at time-reversed ±kpoints. Taking$${\cal{P}}{\cal{T}}$$PT-symmetric magnetic topological quantum material bilayer antiferromagnetic (AFM) MnBi2Te4as an example, we predict the presence of large MIC in the terahertz (THz) frequency regime which can be switched between two AFM states with time-reversed spin orderings upon magnetic transition. In addition, external electric field breaks$${\cal{P}}{\cal{T}}$$PTsymmetry and enables large NSC response in bilayer AFM MnBi2Te4, which can be switched by external electric field. Remarkably, both MIC and NSC are highly tunable under varying electric field due to the field-induced large Rashba and Zeeman splitting, resulting in large nonlinear photocurrent response down to a few THz regime, suggesting bilayer AFM-zMnBi2Te4as a tunable platform with rich THz and magneto-optoelectronic applications. Our results reveal that nonlinear photocurrent responses governed by NSC, NIC, MSC, and MIC provide a powerful tool for deciphering magnetic structures and interactions which could be particularly fruitful for probing and understanding magnetic topological quantum materials.

     
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  4. Abstract

    Under broken time reversal symmetry such as in the presence of external magnetic field or internal magnetization, a transverse voltage can be established in materials perpendicular to both longitudinal current and applied magnetic field, known as classical Hall effect. However, this symmetry constraint can be relaxed in the nonlinear regime, thereby enabling nonlinear anomalous Hall current in time-reversal invariant materials – an underexplored realm with exciting new opportunities beyond classical linear Hall effect. Here, using group theory and first-principles theory, we demonstrate a remarkable ferroelectric nonlinear anomalous Hall effect in time-reversal invariant few-layer WTe2where nonlinear anomalous Hall current switches in odd-layer WTe2except 1T′ monolayer while remaining invariant in even-layer WTe2upon ferroelectric transition. This even-odd oscillation of ferroelectric nonlinear anomalous Hall effect was found to originate from the absence and presence of Berry curvature dipole reversal and shift dipole reversal due to distinct ferroelectric transformation in even and odd-layer WTe2. Our work not only treats Berry curvature dipole and shift dipole on an equal footing to account for intraband and interband contributions to nonlinear anomalous Hall effect, but also establishes Berry curvature dipole and shift dipole as new order parameters for noncentrosymmetric materials. The present findings suggest that ferroelectric metals and Weyl semimetals may offer unprecedented opportunities for the development of nonlinear quantum electronics.

     
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  5. Abstract

    Halide perovskites are revolutionizing the renewable energy sector owing to their high photovoltaic efficiency, low manufacturing cost, and flexibility. Their remarkable mobility and long carrier lifetime are also valuable for information technology, but fundamental challenges like poor stability under an electric field prevent realistic applications of halide perovskites in electronics. Here, it is discovered that valleytronics is a promising route to leverage the advantages of halide perovskites and derivatives for information storage and processing. The synthesized all‐inorganic lead‐free perovskite derivative, Cs3Bi2I9, exhibits strong light–matter interaction and parity‐dependent optically addressable valley degree of freedom. Robust optical helicity in all odd‐layer‐number crystals with inversion symmetry breaking is observed, indicating excitonic coherence extending well beyond 11 layers. The excellent optical and valley properties of Cs3Bi2I9arise from the unique parallel bands, according to first principles calculations. This discovery points to new materials design principles for scalable valleytronic devices and demonstrates the promise of perovskite derivatives beyond energy applications.

     
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  6. Strong coupling between light and mechanical strain forms the foundation for next-generation optical micro- and nano-electromechanical systems. Such optomechanical responses in two-dimensional materials present novel types of functionalities arising from the weak van der Waals bond between atomic layers. Here, by using structure-sensitive megaelectronvolt ultrafast electron diffraction, we report the experimental observation of optically driven ultrafast in-plane strain in the layered group IV monochalcogenide germanium sulfide (GeS). Surprisingly, the photoinduced structural deformation exhibits strain amplitudes of order 0.1% with a 10 ps fast response time and a significant in-plane anisotropy between zigzag and armchair crystallographic directions. Rather than arising due to heating, experimental and theoretical investigations suggest deformation potentials caused by electronic density redistribution and converse piezoelectric effects generated by photoinduced electric fields are the dominant contributors to the observed dynamic anisotropic strains. Our observations define new avenues for ultrafast optomechanical control and strain engineering within functional devices. 
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  7. null (Ed.)
    Antiferromagnets are interesting materials for spintronics because of their faster dynamics and robustness against perturbations from magnetic fields. Control of the antiferromagnetic order constitutes an important step towards applications, but has been limited to bulk materials so far. Here, using spatially resolved second-harmonic generation, we show direct evidence of long-range antiferromagnetic order and Ising-type Néel vector switching in monolayer MnPSe3 with large XY anisotropy. In additional to thermally induced switching, uniaxial strain can rotate the Néel vector, aligning it to a general in-plane direction irrespective of the crystal axes. A change of the universality class of the phase transition in the XY model under uniaxial strain causes this emergence of strain-controlled Ising order in the XY magnet MnPSe3. Our discovery is a further ingredient for compact antiferromagnetic spintronic devices in the two-dimensional limit. 
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