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Thomas Goldstein

Publications and source records attributed to Thomas Goldstein.

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Tight Second-Order Certificates for Randomized Smoothing

Randomized smoothing is a popular way of providing robustness guarantees against adversarial attacks: randomly-smoothed functions have a universal Lipschitz-like bound, allowing for robustness certificates to be easily computed. In this work, we show that there also exists a universal curvature-like bound for Gaussian random smoothing: given the exact value and gradient of a smoothed function, we compute a lower bound on the distance of a point to its closest adversarial example, called the Second-order Smoothing (SoS) robustness certificate. In addition to proving the correctness of this novel certificate, we show that SoS certificates are realizable and therefore tight. Interestingly, we show that the maximum achievable benefits, in terms of certified robustness, from using the additional information of the gradient norm are relatively small: because our bounds are tight, this is a fundamental negative result. The gain of SoS certificates further diminishes if we consider the estimation error of the gradient norms, for which we have developed an estimator. We therefore additionally develop a variant of Gaussian smoothing, called Gaussian dipole smoothing, which provides similar bounds to randomized smoothing with gradient information, but with much-improved sample efficiency. This allows us to achieve (marginally) improved robustness certificates on high-dimensional datasets such as CIFAR-10 and ImageNet. Code is available at https://github.com/alevine0/smoothing_second_order.

cs.LG

Ground and Excited Exciton Polarons in Monolayer MoSe2

Monolayer transition metal dichalcogenide semiconductors, with versatile experimentally accessible exciton species, offer an interesting platform for investigating the interaction between excitons and a Fermi sea of charges. Using hexagonal boron nitride encapsulated monolayer MoSe2, we study the impact of charge density tuning on the ground and excited Rydberg states in the atomic layer. Consistent excitonpolaron behavior is revealed in both photoluminescence and reflection spectra of the A exciton 1s (A:1s) Rydberg state, in contrast to previous studies. The A:2s Rydberg state provides an opportunity to understand such interactions with greatly reduced exciton binding energy. We found that the impact of the Fermi sea becomes much more dramatic. With a photoluminescence upconversion technique, we further verify the 2s polaron-like behavior for the repulsive branch of B:2s exciton whose energy is well above the bare bandgap. Our studies show that the polaron-like interaction features are quite generic and highly robust, offering key insights into the dressed manybody state in a Fermi sea.

cond-mat.mes-hall

The range of non-Kitaev terms and fractional particles in RuCl$_3$

Significant efforts have focused on the magnetic excitations of relativistic Mott insulators, predicted to realize the Kitaev quantum spin liquid (QSL). This exactly solvable model involves a highly entangled state resulting from bond-dependent Ising interactions that produce excitations which are non-local in terms of spin flips. A key challenge in real materials is identifying the relative size of the non-Kitaev terms and their role in the emergence or suppression of fractional excitations. Here, we identify the energy and temperature boundaries of non-Kitaev interactions by direct comparison of the Raman susceptibility of RuCl3 with quantum Monte Carlo (QMC) results for the Kitaev QSLs. Moreover, we further confirm the fractional nature of the magnetic excitations, which is given by creating a pair of fermionic quasiparticles. Interestingly, this fermionic response remains valid in the non-Kitaev range. Our results and focus on the use of the Raman susceptibility provide a stringent new test for future theoretical and experimental studies of QSLs.

cond-mat.str-el

Direct Evidence for Fermi Statistics from Proximity to the Kitaev Spin Liquid in RuCl3

A key characteristic of quantum spin liquids(QSL) is the presence of fractional excitations related to their entanglement properties, yet experimental verification of their statistics is missing. For example, in the potential Kitaev spin liquid, RuCl3 experiments uncovered signs of fractional particles, though not their Fermi statistics. Here we employ Raman scattering to reveal the true nature of the magnetic excitations, using improved experimental methods and analysis to remove the influence of laser heating and thermal fluctuations. Via the energy loss and gain spectra, we extract the energy and temperature dependence of the Raman susceptibility to prove RuCl3's magnetic response is given by pair creation of fermionic excitations. Furthermore, by comparing with quantum Monte Carlo (QMC) results for the exact Kitaev limit, we are able to discern the energy and temperature range where additional interaction terms are important. Our results open new directions in QSL research by providing a new way to investigate fractional excitations and the importance of terms causing spinon confinement.

cond-mat.str-el

Luminescent emission of excited Rydberg excitons from monolayer WSe2

We report the experimental observation of radiative recombination from Rydberg excitons in a two-dimensional semiconductor, monolayer WSe2, encapsulated in hexagonal boron nitride. Excitonic emission up to the 4s excited state is directly observed in photoluminescence spectroscopy in an out-of-plane magnetic field up to 31 Tesla. We confirm the progressively larger exciton size for higher energy excited states through diamagnetic shift measurements. This also enables us to estimate the 1s exciton binding energy to be about 170 meV, which is significantly smaller than most previous reports. The Zeeman shift of the 1s to 3s states, from both luminescence and absorption measurements, exhibits a monotonic increase of g-factor, reflecting nontrivial magnetic-dipole-moment differences between ground and excited exciton states. This systematic evolution of magnetic dipole moments is theoretically explained from the spreading of the Rydberg states in momentum space.

cond-mat.mes-hall

Asymmetric Two-Terminal Graphene Detector for Broadband Radiofrequency Heterodyne- and Self-Mixing

Graphene, a single atomic layer of covalently bonded carbon atoms, has been investigated intensively for optoelectronics and represents a promising candidate for high-speed electronics. Here we present a microwave mixer constructed as an asymmetrically-contacted two-terminal graphene device based on the thermoelectric effect. We report a 50 GHz (minimum) mixer bandwidth as well as 130 V/W (163 mA/W) extrinsic direct-detection responsivity. Anomalous second-harmonic generation due to self-mixing in our graphene detector is also observed. Careful investigation of the responsivity from four different approaches gives consistent results, confirming the exceptional performance of our zero-bias device operating at room temperature. The 50 GHz bandwidth indicates an extremely fast response time and our experimental results represent an encouraging advance towards practical graphene microwave devices, with anticipated future applications extended through millimeter wave and terahertz frequencies.

physics.app-ph

Coulomb-bound four- and five-particle valleytronic states in an atomically-thin semiconductor

As hosts for tightly-bound electron-hole pairs carrying quantized angular momentum, atomically-thin semiconductors of transition metal dichalcogenides provide an appealing platform for optically addressing the valley degree of freedom. In particular, the valleytronic properties of neutral and charged excitons in these systems have been widely investigated. Meanwhile, correlated quantum states involving more particles are so far elusive and controversial. Here we present experimental evidence for valleytronic four-particle biexcitons and five-particle exciton-trions in high-quality monolayer tungsten diselenide samples. Through charge doping, thermal activation, and magnetic-field tuning measurements, we determined that the biexciton and exciton-trion optical emissions are bound with respect to the bright exciton and the trion respectively. Further, both the biexciton and the exciton-trion are intervalley bound states involving dark excitons, giving rise to emissions with large, negative valley polarizations in contrast to that of the well-known two-particle excitons. Our studies provide new opportunities for building valleytronic quantum devices harnessing high-order excitations.

cond-mat.mes-hall

Superior valley polarization and coherence of 2s excitons in monolayer WSe2

We report experimental observation of 2s exciton radiative emission from monolayer tungsten diselenide, enabled by hexagonal boron nitride protected high-quality samples. The 2s luminescence is highly robust and persists up to 150K, offering a new quantum entity for manipulating the valley degree of freedom. Remarkably, the 2s exciton displays superior valley polarization and coherence than 1s under similar experimental conditions. This observation provides evidence that the Coulomb-exchange-interaction-driven valley-depolarization process, the Maialle-Silva-Sham mechanism, plays an important role in valley excitons of monolayer transition metal dichalcogenides.

cond-mat.mes-hall

Intrinsic Phonon Bands in High-Quality Monolayer T' Molybdenum Ditelluride

The topologically nontrivial and chemically functional distorted octahedral (T') transition metal dichalcogenides (TMDCs) are a type of layered semimetal that has attracted significant recent attention. However, the properties of monolayer (1L) T'-TMDC, a fundamental unit of the system, is still largely unknown due to rapid sample degradation in air. Here we report that well-protected 1L CVD T'-MoTe2 exhibits sharp and robust intrinsic Raman bands, with intensities about one order of magnitude stronger than those from bulk T'-MoTe2. The high-quality samples enabled us to reveal the set of all nine even-parity zone-center optical phonons, providing reliable fingerprints for the previously elusive crystal. By performing light polarization and crystal orientation resolved scattering analysis, we can effectively distinguish the intrinsic modes from Te-metalloid-like modes A (~122 cm-1) and B (~141 cm-1) which are related to the sample degradation. Our studies offer a powerful non-destructive method for assessing sample quality and for monitoring sample degradation in situ, representing a solid advance in understanding the fundamental properties of 1L-T'-TMDCs.

cond-mat.mtrl-sci

Activation of new Raman modes by inversion symmetry breaking in type II Weyl semimetal candidate T'-MoTe2

We synthesized distorted octahedral(T') molybdenum ditelluride (MoTe2) and investigated its vibrational properties with Raman spectroscopy, density functional theory and symmetry analysis. Compared to the results from high temperature centrosymmetric monoclinic (T'mo) phase, four new Raman bands emerge in the low temperature orthorhombic (T'or) phase, which was recently predicted to be a type II Weyl semimetal. Crystal-angle-dependent, light-polarization-resolved measurements indicate that all the observed Raman peaks belong to two categories: those vibrating along the zigzag Mo atomic chain (z-mode) and those vibrating in the mirror plane (m-mode) perpendicular to the zigzag chain. Interestingly the low energy shear z-mode and shear m-mode, absent from the T'mo spectra, become activated when sample cooling induces a phase transition to the T'or crystal structure. We interpret this observation as a consequence of inversion-symmetry breaking, which is crucial for the existence of Weyl fermions in the layered crystal. Our temperature dependent Raman measurements further show that both the high energy m-mode at 130 cm-1 and the low energy shear m-mode at 12 cm-1 provide useful gauges for monitoring the broken inversion symmetry in the crystal.

cond-mat.mes-hall

ShapeFit and ShapeKick for Robust, Scalable Structure from Motion

We introduce a new method for location recovery from pair-wise directions that leverages an efficient convex program that comes with exact recovery guarantees, even in the presence of adversarial outliers. When pairwise directions represent scaled relative positions between pairs of views (estimated for instance with epipolar geometry) our method can be used for location recovery, that is the determination of relative pose up to a single unknown scale. For this task, our method yields performance comparable to the state-of-the-art with an order of magnitude speed-up. Our proposed numerical framework is flexible in that it accommodates other approaches to location recovery and can be used to speed up other methods. These properties are demonstrated by extensively testing against state-of-the-art methods for location recovery on 13 large, irregular collections of images of real scenes in addition to simulated data with ground truth.

cs.CV

Raman scattering and anomalous Stokes anti-Stokes ratio in MoTe2 atomic layers

Stokes and anti-Stokes Raman scattering are performed on atomic layers of hexagonal molybdenum ditelluride (MoTe2), a prototypical transition metal dichalcogenide (TMDC) semiconductor. The data reveal all six types of zone center optical phonons, along with their corresponding Davydov splittings, which have been challenging to see in other TMDCs. We discover that the anti-Stokes Raman intensity of the low energy layer-breathing mode becomes more intense than the Stokes peak under certain experimental conditions, and find the effect to be tunable by excitation frequency and number of atomic layers. These observations are interpreted as a result of resonance effects arising from the C excitons in the vicinity of the Brillouin zone center in the photon-electron-phonon interaction process.

cond-mat.mtrl-sci

Inversion-symmetry-breaking-activated shear Raman bands in $T'$-MoTe$_2$

Type-II Weyl fermion nodes, located at the touching points between electron and hole pockets, have been recently predicted to occur in distorted octahedral ($T'$) transition metal dichalcogenide semimetals, contingent upon the condition that the layered crystal has the noncentrosymmetric orthorhombic ($T'_{or}$) stacking. Here, we report on the emergence of two shear Raman bands activated by inversion symmetry breaking in $T'$-MoTe$_2$ due to sample cooling. Polarization and crystal orientation resolved measurements further point to a phase transition from the monoclinic ($T'_{mo}$) structure to the desired $T'_{or}$ lattice. These results provide spectroscopic evidence that low-temperature $T'$-MoTe$_2$ is suitable for probing type-II Weyl physics.

cond-mat.mes-hall

Layer-Specific Adaptive Learning Rates for Deep Networks

The increasing complexity of deep learning architectures is resulting in training time requiring weeks or even months. This slow training is due in part to vanishing gradients, in which the gradients used by back-propagation are extremely large for weights connecting deep layers (layers near the output layer), and extremely small for shallow layers (near the input layer); this results in slow learning in the shallow layers. Additionally, it has also been shown that in highly non-convex problems, such as deep neural networks, there is a proliferation of high-error low curvature saddle points, which slows down learning dramatically. In this paper, we attempt to overcome the two above problems by proposing an optimization method for training deep neural networks which uses learning rates which are both specific to each layer in the network and adaptive to the curvature of the function, increasing the learning rate at low curvature points. This enables us to speed up learning in the shallow layers of the network and quickly escape high-error low curvature saddle points. We test our method on standard image classification datasets such as MNIST, CIFAR10 and ImageNet, and demonstrate that our method increases accuracy as well as reduces the required training time over standard algorithms.

cs.CV

Fast Sublinear Sparse Representation using Shallow Tree Matching Pursuit

Sparse approximations using highly over-complete dictionaries is a state-of-the-art tool for many imaging applications including denoising, super-resolution, compressive sensing, light-field analysis, and object recognition. Unfortunately, the applicability of such methods is severely hampered by the computational burden of sparse approximation: these algorithms are linear or super-linear in both the data dimensionality and size of the dictionary. We propose a framework for learning the hierarchical structure of over-complete dictionaries that enables fast computation of sparse representations. Our method builds on tree-based strategies for nearest neighbor matching, and presents domain-specific enhancements that are highly efficient for the analysis of image patches. Contrary to most popular methods for building spatial data structures, out methods rely on shallow, balanced trees with relatively few layers. We show an extensive array of experiments on several applications such as image denoising/superresolution, compressive video/light-field sensing where we practically achieve 100-1000x speedup (with a less than 1dB loss in accuracy).

cs.CV