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Creators/Authors contains: "Mao, Zhiqiang"

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  1. Excitation of coherent phonons has the potential to dramatically alter the electronic structure of Dirac and Weyl semimetals, enabling sub-picosecond control of their optical and electronic properties. The Dirac semimetal SrMnSb2 is a candidate for such control, with a coherent-phonon mode that is predicted to close and reopen a gap at the Dirac node. Here, through a series of ultrafast pump-probe experiments, we establish suitable samples and conditions for driving the coherent phonon to high amplitude and attempting to observe the gap’s closure. Films of SrMnSb2 grown by molecular-beam epitaxy are shown to have phononic properties matching those of bulk crystals. We find that the phonon can be strongly excited by pump pulses with wavelength near 1500 nm, which will excite a 30-nm film almost uniformly and will penetrate the arsenic capping layers that protect the films. We find that samples withstand pump pulses of fluence up to 20 mJ/cm2, and we demonstrate the potential for sequences of pulses to amplify the oscillation while suppressing other phonon modes. Armed with our new knowledge of the conditions for exciting the desired coherent phonon, future experiments will be well prepared to measure its motion and to observe phononic control of the Dirac-point gap. 
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  2. 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. 
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  3. Abstract Rare-earth monopnictides are a family of materials simultaneously displaying complex magnetism, strong electronic correlation, and topological band structure. The recently discovered emergent arc-like surface states in these materials have been attributed to the multi-wave-vector antiferromagnetic order, yet the direct experimental evidence has been elusive. Here we report observation of non-collinear antiferromagnetic order with multiple modulations using spin-polarized scanning tunneling microscopy. Moreover, we discover a hidden spin-rotation transition of single-to-multiple modulations 2 K below the Néel temperature. The hidden transition coincides with the onset of the surface states splitting observed by our angle-resolved photoemission spectroscopy measurements. Single modulation gives rise to a band inversion with induced topological surface states in a local momentum region while the full Brillouin zone carries trivial topological indices, and multiple modulation further splits the surface bands via non-collinear spin tilting, as revealed by our calculations. The direct evidence of the non-collinear spin order in NdSb not only clarifies the mechanism of the emergent topological surface states, but also opens up a new paradigm of control and manipulation of band topology with magnetism. 
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  4. 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. 
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  5. Abstract Achieving spin-pinning at the interface of hetero-bilayer ferromagnet/antiferromagnet structures in conventional exchange bias systems can be challenging due to difficulties in interface control and the weakening of spin-pinning caused by poor interface quality. In this work, we propose an alternative approach to stabilize the exchange interaction at the interface of an uncompensated antiferromagnet by utilizing a gradient of interlayer exchange coupling. We demonstrate this exchange interaction through a designed field training protocol in the odd-layer topological antiferromagnet MnBi2Te4. Our results reveal a remarkable field-trained exchange bias of up to ~ 400 mT, which exhibits high repeatability and can be easily reset by a large training field. Notably, this field-trained exchange bias effect persists even with zero-field initialization, presenting a stark contrast to the traditional field-cooled exchange bias. The highly tunable exchange bias observed in this single antiferromagnet compound, without the need for an additional magnetic layer, provides valuable insight into the exchange interaction mechanism. These findings pave the way for the systematic design of topological antiferromagnetic spintronics. 
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  6. Abstract Effective control of magnetic phases in two-dimensional magnets would constitute crucial progress in spintronics, holding great potential for future computing technologies. Here, we report a new approach of leveraging tunneling current as a tool for controlling spin states in CrI3. We reveal that a tunneling current can deterministically switch between spin-parallel and spin-antiparallel states in few-layer CrI3, depending on the polarity and amplitude of the current. We propose a mechanism involving nonequilibrium spin accumulation in the graphene electrodes in contact with the CrI3layers. We further demonstrate tunneling current-tunable stochastic switching between multiple spin states of the CrI3tunnel devices, which goes beyond conventional bi-stable stochastic magnetic tunnel junctions and has not been documented in two-dimensional magnets. Our findings not only address the existing knowledge gap concerning the influence of tunneling currents in controlling the magnetism in two-dimensional magnets, but also unlock possibilities for energy-efficient probabilistic and neuromorphic computing. 
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