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EuCd_{2}As_{2} has attracted considerable interest as one of the few magnetic Weyl semimetal candidate materials, although recently there have been emerging reports that claim it to have a semiconducting electronic structure. To resolve this debate, we established the growth of n-type EuCd_{2}As_{2} crystals, to directly visualize the nature of the conduction band using angle resolve photoemission spectroscopy (ARPES). We show that La-doping leads to n-type transport signatures in both the thermopower and Hall effect measurements, in crystals with doping levels at 2 - 6 x 10^{17} e^{-} cm^{-3}. Both p-type and n-type doped samples exhibit antiferromagnetic ordering at 9 K. ARPES experiments at 6 K clearly show the presence of the conduction band minimum at 0.8 eV above the valence band maximum, which is further corroborated by the observation of a 0.71 - 0.72 eV band gap in room temperature diffuse reflectance absorbance measurements. Together these findings unambiguously show that EuCd_{2}As_{2} is indeed a semiconductor with a substantial band gap and not a topological semimetal.

The unique optical properties of graphene, with broadband absorption and ultrafast response, make it a critical component of optoelectronic and spintronic devices. Using time-resolved momentum microscopy with high data rate and high dynamic range, we report momentum-space measurements of electrons promoted to the graphene conduction band with visible light, and their subsequent relaxation. We observe a pronounced non-thermal distribution of nascent photoexcited electrons with lattice pseudospin polarization in remarkable agreement with results of simple tight-binding theory. By varying the excitation fluence, we vary the relative importance of electron-electron vs. electron-phonon scattering in the relaxation of the initial distribution. Increasing the excitation fluence results in increased noncollinear electron-electron scattering and reduced pseudospin polarization, although up-scattered electrons retain a degree of polarization. These detailed momentum-resolved electron dynamics in graphene demonstrate the capabilities of high-performance time-resolved momentum microscopy in the study of 2D materials and can inform the design of graphene devices., Comment: 19 pages, 5 figures

Kagome lattices have garnered substantial interest because their band structure consists of topological flat bands and Dirac cones. The RMn$_6$Sn$_6$ (R = rare earth) compounds are particularly interesting because of the existence of large intrinsic anomalous Hall effect (AHE) which originates from the gapped Dirac cones near the Fermi level. This makes RMn$_6$Sn$_6$ an outstanding candidate for realizing the high-temperature quantum anomalous Hall effect. The growth of RMn$_6$Sn$_6$ thin films is beneficial for both fundamental research and potential applications. However, most of the studies on RMn$_6$Sn$_6$ have focused on bulk crystals so far, and the synthesis of RMn$_6$Sn$_6$ thin films has not been reported so far. Here we report the atomic layer molecular beam epitaxy growth, structural and magnetic characterizations, and transport properties of ErMn$_6$Sn$_6$ and TbMn$_6$Sn$_6$ thin films. It is especially noteworthy that TbMn$_6$Sn$_6$ thin films have out-of-plane magnetic anisotropy, which is important for realizing the quantum anomalous Hall effect. Our work paves the avenue toward the control of the AHE using devices patterned from RMn$_6$Sn$_6$ thin films., Comment: 7 pages, 4 figures

Heterostructures of two-dimensional (2D) van der Waals (vdW) magnets and topological insulators (TI) are of substantial interest as candidate materials for efficient spin-torque switching, quantum anomalous Hall effect, and chiral spin textures. However, since many of the vdW magnets have Curie temperatures below room temperature, we want to understand how materials can be modified to stabilize their magnetic ordering to higher temperatures. In this work, we utilize molecular beam epitaxy to systematically tune the Curie temperature ($T_C$) in thin film Fe$_3$GeTe$_2$/Bi$_2$Te$_3$ from bulk-like values ($\sim$220 K) to above room temperature by increasing the growth temperature from 300 $^\circ$C to 375 $^\circ$C. For samples grown at 375 $^\circ$C, cross-sectional scanning transmission electron microscopy (STEM) reveals the spontaneous formation of different Fe$_m$Ge$_n$Te$_2$ compositions (e.g. Fe$_5$Ge$_2$Te$_2$ and Fe$_7$Ge$_6$Te$_2$) as well as intercalation in the vdW gaps, which are possible origins of the enhanced Curie temperature. This observation paves the way for developing various Fe$_m$Ge$_n$Te$_2$/TI heterostructures with novel properties., Comment: 8 pages, 4 figures

Spintronic, spin caloritronic, and magnonic phenomena arise from complex interactions between charge, spin, and structural degrees of freedom that are challenging to model and even more difficult to predict. This situation is compounded by the relative scarcity of magnetically-ordered materials with relevant functionality, leaving the field strongly constrained to work with a handful of well-studied systems that do not encompass the full phase space of phenomenology predicted by fundamental theory. Here we present an important advance in this coupled theory-experiment challenge, wherein we extend existing theories of the spin Seebeck effect (SSE) to explicitly include the temperature-dependence of magnon non-conserving processes. This expanded theory quantitatively describes the low-temperature behavior of SSE signals previously measured in the mainstay material yttrium iron garnet (YIG) and predicts a new regime for magnonic and spintronic materials that have low saturation magnetization, $M_S$, and ultra-low damping. Finally, we validate this prediction by directly observing the spin Seebeck resistance (SSR) in the molecule-based ferrimagnetic semiconductor vanadium tetracyanoethylene (V[TCNE]$_x$, $x \sim 2$). These results validate the expanded theory, yielding SSR signals comparable in magnitude to YIG and extracted magnon diffusion length ($\lambda_m>1$ $\mu$ m) and magnon lifetime for V[TCNE]$_x$ ($\tau_{th}\approx 1-10$ $\mu$ s) exceeding YIG ($\tau_{th}\sim 10$ ns). Surprisingly, these properties persist to room temperature despite relatively low spin wave stiffness (exchange). This identification of a new regime for highly efficient SSE-active materials opens the door to a new class of magnetic materials for spintronic and magnonic applications.

Systems with flat bands are ideal for studying strongly correlated electronic states and related phenomena. Among them, kagome-structured metals such as CoSn have been recognized as promising candidates due to the proximity between the flat bands and the Fermi level. A key next step will be to realize epitaxial kagome thin films with flat bands to enable tuning of the flat bands across the Fermi level via electrostatic gating or strain. Here we report the band structures of epitaxial CoSn thin films grown directly on insulating substrates. Flat bands are observed using synchrotron-based angle-resolved photoemission spectroscopy (ARPES). The band structure is consistent with density functional theory (DFT) calculations, and the transport properties are quantitatively explained by the band structure and semiclassical transport theory. Our work paves the way to realize flat band-induced phenomena through fine-tuning of flat bands in kagome materials., Comment: 30 pages, 12 figures

Magnetic multilayers are a promising platform for storage and logic devices based on skyrmion spin textures, due to the large materials phase space for tuning properties. Epitaxial superlattice structures of [Pt/Co/Cu]n thin films were grown by molecular beam epitaxy at room temperature. Spin-polarized scanning tunneling microscopy (SP-STM) of these samples was used to probe the connection between surface structure and skyrmion morphology with nanoscale spatial resolution. Irregular-shaped skyrmion bubbles were observed, with effective diameters from 20-200 nm that are much larger than the nanoscale grain structure of the surface topography. Nucleation, annihilation, and motion of skyrmion bubbles could be driven using the stray field of the ferromagnetic tip in repeated imaging, and spin-polarized current/voltage pulses. Our detailed comparison of STM topography and differential conductance images shows that there are no surface defects or inhomogeneities at length scales that could account for the range in skyrmion bubble size or shape observed in the measurements., Comment: 11 pages, 5 figures

Creating materials that do not exist in nature can lead to breakthroughs in science and technology. Magnetic skyrmions are topological excitations that have attracted great attention recently for their potential applications in low power, ultrahigh density memory. A major challenge has been to find materials that meet the dual requirement of small skyrmions stable at room temperature. Here we meet both these goals by developing epitaxial FeGe films with excess Fe using atomic layer molecular beam epitaxy (MBE) far from thermal equilibrium. Our novel atomic layer design permits the incorporation of 20% excess Fe while maintaining a non-centrosymmetric crystal structure supported by theoretical calculations and necessary for stabilizing skyrmions. We show that the Curie temperature is well above room temperature, and that the skyrmions probed by topological Hall effect have sizes down to 15 nm as imaged by Lorentz transmission electron microscopy (LTEM) and magnetic force microscopy (MFM). Our results illustrate new avenues for creating artificial materials tailored at the atomic scale that can impact nanotechnology., Comment: 22 figures, 34 pages

Magnetic skyrmions are promising for next-generation information storage and processing owing to their potential advantages in data storage density, robustness, and energy efficiency. The magnetic multilayers consisting of Pt, Co, and a third metal element $X$ provide an ideal platform to study the skyrmions due to their highly tunable magnetic properties. Here, we report the observation of room-temperature bubble-like N\'eel skyrmions in epitaxial Pt/Co/Cu multilayers in samples with multidomain states in zero field. The magneto-optic Kerr effect (MOKE) and superconducting quantum interference device (SQUID) magnetometry are applied to investigate the shapes of the hysteresis loops, the magnetic anisotropy, and the saturation magnetization. By tuning the Co thickness and the number of periods, we achieve perpendicular and in-plane magnetized states and multidomain states that are identified by a wasp-waisted hysteresis loop. Skyrmions are directly imaged by magnetic force microscopy (MFM) and Lorentz transmission electron microscopy (LTEM). The development of room-temperature skyrmions in Pt/Co/Cu multilayers may lead to advances in skyrmion-related research and applications., Comment: 11 pages, 6 Figures

Magnetic materials with kagome crystal structure exhibit rich physics such as frustrated magnetism, skyrmion formation, topological flat bands, and Dirac/Weyl points. Until recently, most studies on kagome magnets have been performed on bulk crystals or polycrystalline films. Here we report the atomic layer molecular beam epitaxy synthesis of high-quality thin films of topological kagome magnet Fe${_3}$Sn${_2}$. Structural and magnetic characterization of Fe${_3}$Sn${_2}$ on epitaxial Pt(111) identifies highly ordered films with c-plane orientation and an in-plane magnetic easy axis. Studies of the local magnetic structure by anomalous Nernst effect imaging reveals in-plane oriented micrometer size domains. Superlattice structures consisting of Fe${_3}$Sn${_2}$ and Fe${_3}$Sn are also synthesized by atomic layer molecular beam epitaxy, demonstrating the ability to modulate the sample structure at the atomic level. The realization of high-quality films by atomic layer molecular beam epitaxy opens the door to explore the rich physics of this system and investigate novel spintronic phenomena by interfacing Fe${_3}$Sn${_2}$ with other materials., Comment: 8 pages, 5 figures. arXiv admin note: substantial text overlap with arXiv:2105.12203

Adversarial attacks have been extensively studied in recent years since they can identify the vulnerability of deep learning models before deployed. In this paper, we consider the black-box adversarial setting, where the adversary needs to craft adversarial examples without access to the gradients of a target model. Previous methods attempted to approximate the true gradient either by using the transfer gradient of a surrogate white-box model or based on the feedback of model queries. However, the existing methods inevitably suffer from low attack success rates or poor query efficiency since it is difficult to estimate the gradient in a high-dimensional input space with limited information. To address these problems and improve black-box attacks, we propose two prior-guided random gradient-free (PRGF) algorithms based on biased sampling and gradient averaging, respectively. Our methods can take the advantage of a transfer-based prior given by the gradient of a surrogate model and the query information simultaneously. Through theoretical analyses, the transfer-based prior is appropriately integrated with model queries by an optimal coefficient in each method. Extensive experiments demonstrate that, in comparison with the alternative state-of-the-arts, both of our methods require much fewer queries to attack black-box models with higher success rates., Comment: Accepted by IEEE Transactions on Pattern Recognition and Machine Intelligence (TPAMI). The official version is at https://ieeexplore.ieee.org/document/9609659

Coupling between exciton states across the Brillouin zone in monolayer transition metal dichalcogenides can lead to ultrafast valley depolarization. Using time- and angle-resolved photoemission, we present momentum- and energy-resolved measurements of exciton coupling in monolayer WS$_2$. By comparing full 4D ($k_x, k_y, E, t$) data sets after both linearly and circularly polarized excitation, we are able to disentangle intervalley and intravalley exciton coupling dynamics. Recording in the exciton binding energy basis instead of excitation energy, we observe strong mixing between the B$_{1s}$ exciton and A$_{n>1}$ states. The photoelectron energy and momentum distributions observed from excitons populated via intervalley coupling (e.g. K$^-$ $\rightarrow$ K$^+$) indicate that the dominant valley depolarization mechanism conserves the exciton binding energy and center-of-mass momentum, consistent with intervalley Coulomb exchange. On longer timescales, exciton relaxation is accompanied by contraction of the momentum space distribution., Comment: 16 pages: 8 pages main text with 5 figures, 8 pages SI with 6 figures

Zeroth-order (ZO) optimization is widely used to handle challenging tasks, such as query-based black-box adversarial attacks and reinforcement learning. Various attempts have been made to integrate prior information into the gradient estimation procedure based on finite differences, with promising empirical results. However, their convergence properties are not well understood. This paper makes an attempt to fill up this gap by analyzing the convergence of prior-guided ZO algorithms under a greedy descent framework with various gradient estimators. We provide a convergence guarantee for the prior-guided random gradient-free (PRGF) algorithms. Moreover, to further accelerate over greedy descent methods, we present a new accelerated random search (ARS) algorithm that incorporates prior information, together with a convergence analysis. Finally, our theoretical results are confirmed by experiments on several numerical benchmarks as well as adversarial attacks., Comment: NeurIPS 2021; code available at https://github.com/csy530216/pg-zoo

Magnetic materials with kagome crystal structure exhibit rich physics such as frustrated magnetism, skyrmion formation, topological flat bands, and Dirac/Weyl points. Until recently, most studies on kagome magnets have been performed on bulk crystals or polycrystalline films. Here we report the synthesis of high-quality epitaxial films of topological kagome magnet Fe$_3$Sn$_2$ by atomic layer molecular beam epitaxy. Structural and magnetic characterization of Fe$_3$Sn$_2$ on epitaxial Pt(111) identifies highly ordered films with c-plane orientation and an in-plane magnetic easy axis. Studies of the local magnetic structure by anomalous Nernst effect imaging reveals in-plane oriented micrometer size domains. The realization of high-quality films by atomic layer molecular beam epitaxy opens the door to explore the rich physics of this system and investigate novel spintronic phenomena by interfacing Fe$_3$Sn$_2$ with other materials., Comment: 6 pages, 5 figures

We propose a simple and highly query-efficient black-box adversarial attack named SWITCH, which has a state-of-the-art performance in the score-based setting. SWITCH features a highly efficient and effective utilization of the gradient of a surrogate model $\hat{\mathbf{g}}$ w.r.t. the input image, i.e., the transferable gradient. In each iteration, SWITCH first tries to update the current sample along the direction of $\hat{\mathbf{g}}$, but considers switching to its opposite direction $-\hat{\mathbf{g}}$ if our algorithm detects that it does not increase the value of the attack objective function. We justify the choice of switching to the opposite direction by a local approximate linearity assumption. In SWITCH, only one or two queries are needed per iteration, but it is still effective due to the rich information provided by the transferable gradient, thereby resulting in unprecedented query efficiency. To improve the robustness of SWITCH, we further propose SWITCH$_\text{RGF}$ in which the update follows the direction of a random gradient-free (RGF) estimate when neither $\hat{\mathbf{g}}$ nor its opposite direction can increase the objective, while maintaining the advantage of SWITCH in terms of query efficiency. Experimental results conducted on CIFAR-10, CIFAR-100 and TinyImageNet show that compared with other methods, SWITCH achieves a satisfactory attack success rate using much fewer queries, and SWITCH$_\text{RGF}$ achieves the state-of-the-art attack success rate with fewer queries overall. Our approach can serve as a strong baseline for future black-box attacks because of its simplicity. The PyTorch source code is released on https://github.com/machanic/SWITCH., Comment: 18 pages, including the supplementary material after the reference section

The intrinsic magnetic topological insulators MnBi$_2$X$_4$ (X = Se, Te) are promising candidates in realizing various novel topological states related to symmetry breaking by magnetic order. Although much progress had been made in MnBi$_2$Te$_4$, the study of MnBi$_2$Se$_4$ has been lacking due to the difficulty of material synthesis of the desired trigonal phase. Here, we report the synthesis of multilayer trigonal MnBi$_2$Se$_4$ with alternating-layer molecular beam epitaxy. Atomic-resolution scanning transmission electron microscopy (STEM) and scanning tunneling microscopy (STM) identify a well-ordered multilayer van der Waals (vdW) crystal with septuple-layer base units in agreement with the trigonal structure. Systematic thickness-dependent magnetometry studies illustrate the layered antiferromagnetic ordering as predicted by theory. Angle-resolved photoemission spectroscopy (ARPES) reveals the gapless Dirac-like surface state of MnBi$_2$Se$_4$, which demonstrates that MnBi$_2$Se$_4$ is a topological insulator above the magnetic ordering temperature. These systematic studies show that MnBi$_2$Se$_4$ is a promising candidate for exploring the rich topological phases of layered antiferromagnetic topological insulators., Comment: 20 pages, 9 figures

Score matching provides an effective approach to learning flexible unnormalized models, but its scalability is limited by the need to evaluate a second-order derivative. In this paper, we present a scalable approximation to a general family of learning objectives including score matching, by observing a new connection between these objectives and Wasserstein gradient flows. We present applications with promise in learning neural density estimators on manifolds, and training implicit variational and Wasserstein auto-encoders with a manifold-valued prior., Comment: AISTATS 2020

We report the crystal and electronic structures of a non-centrosymmetric quasi-two-dimensional (2D), candidate of topological semimetal AuTe2Br. The Fermi surface of this layered compound consists of 2D-like, topological trivial electron and non-trivial hole pockets which host a Dirac cone along the kz direction. Our transport measurements on the single crystals show highly anisotropic, compensated low-density electrons and holes, both of which exhibit ultrahigh mobility at a level of 10^5cm^2V^-1s^-1 at low temperature. The highly mobile, compensated carriers lead a non-saturated, parabolic magnetoresistance as large as 3*10^5 in single-crystalline AuTe2Br in a magnetic field up to 58 T., Comment: 8 pages, 5 figures

We consider the black-box adversarial setting, where the adversary has to generate adversarial perturbations without access to the target models to compute gradients. Previous methods tried to approximate the gradient either by using a transfer gradient of a surrogate white-box model, or based on the query feedback. However, these methods often suffer from low attack success rates or poor query efficiency since it is non-trivial to estimate the gradient in a high-dimensional space with limited information. To address these problems, we propose a prior-guided random gradient-free (P-RGF) method to improve black-box adversarial attacks, which takes the advantage of a transfer-based prior and the query information simultaneously. The transfer-based prior given by the gradient of a surrogate model is appropriately integrated into our algorithm by an optimal coefficient derived by a theoretical analysis. Extensive experiments demonstrate that our method requires much fewer queries to attack black-box models with higher success rates compared with the alternative state-of-the-art methods., Comment: NeurIPS 2019; Code available at https://github.com/thu-ml/Prior-Guided-RGF

Gradient-based Monte Carlo sampling algorithms, like Langevin dynamics and Hamiltonian Monte Carlo, are important methods for Bayesian inference. In large-scale settings, full-gradients are not affordable and thus stochastic gradients evaluated on mini-batches are used as a replacement. In order to reduce the high variance of noisy stochastic gradients, Dubey et al. [2016] applied the standard variance reduction technique on stochastic gradient Langevin dynamics and obtained both theoretical and experimental improvements. In this paper, we apply the variance reduction tricks on Hamiltonian Monte Carlo and achieve better theoretical convergence results compared with the variance-reduced Langevin dynamics. Moreover, we apply the symmetric splitting scheme in our variance-reduced Hamiltonian Monte Carlo algorithms to further improve the theoretical results. The experimental results are also consistent with the theoretical results. As our experiment shows, variance-reduced Hamiltonian Monte Carlo demonstrates better performance than variance-reduced Langevin dynamics in Bayesian regression and classification tasks on real-world datasets., Comment: 25 pages