arXiv subjects

Stephen K. Gray

Publications and source records attributed to Stephen K. Gray.

At least 37 records · Page 2Linked to original sources

arXiv2021

Quantum Krylov subspace algorithms for ground and excited state energy estimation

Quantum Krylov subspace diagonalization (QKSD) algorithms provide a low-cost alternative to the conventional quantum phase estimation algorithm for estimating the ground and excited-state energies of a quantum many-body system. While QKSD algorithms typically rely on using the Hadamard test for estimating Krylov subspace matrix elements of the form, $\langle ϕ_i|e^{-i\hat{H}τ}|ϕ_j \rangle$, the associated quantum circuits require an ancilla qubit with controlled multi-qubit gates that can be quite costly for near-term quantum hardware. In this work, we show that a wide class of Hamiltonians relevant to condensed matter physics and quantum chemistry contain symmetries that can be exploited to avoid the use of the Hadamard test. We propose a multi-fidelity estimation protocol that can be used to compute such quantities showing that our approach, when combined with efficient single-fidelity estimation protocols, provides a substantial reduction in circuit depth. In addition, we develop a unified theory of quantum Krylov subspace algorithms and present three new quantum-classical algorithms for the ground and excited-state energy estimation problems, where each new algorithm provides various advantages and disadvantages in terms of total number of calls to the quantum computer, gate depth, classical complexity, and stability of the generalized eigenvalue problem within the Krylov subspace.

quant-ph↗

arXiv2021

Sample-efficient adaptive calibration of quantum networks using Bayesian optimization

Indistinguishable photons are imperative for advanced quantum communication networks. Indistinguishability is difficult to obtain because of environment-induced photon transformations and loss imparted by communication channels, especially in noisy scenarios. Strategies to mitigate these transformations often require hardware or software overhead that is restrictive (e.g. adding noise), infeasible (e.g. on a satellite), or time-consuming for deployed networks. Here we propose and develop resource-efficient Bayesian optimization techniques to rapidly and adaptively calibrate the indistinguishability of individual photons for quantum networks using only information derived from their measurement. To experimentally validate our approach, we demonstrate the optimization of Hong-Ou-Mandel interference between two photons -- a central task in quantum networking -- finding rapid, efficient, and reliable convergence towards maximal photon indistinguishability in the presence of high loss and shot noise. We expect our resource-optimized and experimentally friendly methodology will allow fast and reliable calibration of indistinguishable quanta, a necessary task in distributed quantum computing, communications, and sensing, as well as for fundamental investigations.

quant-ph↗

arXiv2021

Giant Optomechanical Coupling in the Charge Density Wave State of Tantalum Disulfide

We study the coupling of light and the structural order parameter in the charge density wave (CDW) state of the layered transition-metal dichalcogenide, Tantalum Disulfide ($1T-\mathrm{TaS_2}$). Using time-dependent density functional theory calculations of the dielectric properties along the distortions coordinates, we show that $1T-\mathrm{TaS_2}$ displays very large change in its dielectric function along the amplitude (Higgs) mode due to the coupling of the periodic lattice distortion with an in-plane metal-insulator transition, leading to optomechanical coupling coefficients two orders of magnitude larger than the ones of diamond and ErFeO$_3$. In addition, we derive an effective model of the light-induced dynamics, which is in quantitative agreement with experimental observations in $1T-\mathrm{TaS_2}$. We show that light-induced dynamics of the structural order parameter in $1T-\mathrm{TaS_2}$ can be deterministically controlled to engineer large third-order non-linear optical susceptibilities. Our findings suggest that CDW materials are promising active materials for non-linear optics.

cond-mat.mtrl-sci↗

arXiv2021

Ab Initio Molecular Dynamics on Quantum Computers

Ab initio molecular dynamics (AIMD) is a valuable technique for studying molecules and materials at finite temperatures where the nuclei evolve on potential energy surfaces obtained from accurate electronic structure calculations. In this work, a quantum computer-based AIMD method is presented. The electronic energies are calculated on a quantum computer using the variational quantum eigensolver (VQE) method. We compute the energy gradients numerically using the Hellmann-Feynman theorem, finite differences, and a correlated sampling technique. Our method only requires additional classical calculations of electron integrals for each degree of freedom, without any additional computations on a quantum computer beyond the initial VQE run. To achieve comparable accuracy, our gradient calculation method requires three to five orders of magnitude fewer measurements than other brute force methods without correlated sampling. As a proof of concept, AIMD dynamics simulations are demonstrated for the H2 molecule on IBM quantum devices. To the best of our knowledge, it is the first successful attempt to run AIMD on quantum devices for a chemical system. In addition, we demonstrate the validity of the method for larger molecules using full configuration interaction (FCI) wave functions. As quantum hardware and noise mitigation techniques continue to improve, the method can be utilized for studying larger molecular and material systems.

physics.chem-ph↗

arXiv2020

Momentum-resolved surface enhanced Raman scattering from a nanowire-nanoparticle junction cavity

Herein we report experimental evidence of directional SERS from molecules situated inside a single nanowire-nanoparticle junction cavity. The emission was confined to a narrow range of wavevectors perpendicular to the axis of the cavity. In addition to this, the molecules excite multiple guided modes of the nanowire which were imaged using leakage radiation Fourier microscopy. We further characterize the emission wavevectors as a function of output polarization. The excited guided modes of the wire show interesting polarization signatures. All the results were corroborated using finite element method based numerical simulations. Essentially, we provide an important connection between gap-cavity enhanced Raman scattering and its directionality of emission. The results may be of relevance in understanding the cavity electrodynamics at the nanoscale and molecular coupling to extremely small gaps between a one dimensional and a zero-dimensional plasmonic nanostructure.

physics.optics↗

arXiv2020

Accelerating quantum optics experiments with statistical learning

Quantum optics experiments, involving the measurement of low-probability photon events, are known to be extremely time-consuming. We present a new methodology for accelerating such experiments using physically-motivated ansatzes together with simple statistical learning techniques such as Bayesian maximum a posteriori estimation based on few-shot data. We show that it is possible to reconstruct time-dependent data using a small number of detected photons, allowing for fast estimates in under a minute and providing a one-to-two order of magnitude speed up in data acquisition time. We test our approach using real experimental data to retrieve the second order intensity correlation function, $G^{(2)}(τ)$, as a function of time delay $τ$ between detector counts, for thermal light as well as anti-bunched light emitted by a quantum dot driven by periodic laser pulses. The proposed methodology has a wide range of applicability and has the potential to impact the scientific discovery process across a multitude of domains.

quant-ph↗

arXiv2020

Accelerating ultrafast spectroscopy with compressive sensing

Ultrafast spectroscopy is an important tool for studying photoinduced dynamical processes in atoms, molecules, and nanostructures. Typically, the time to perform these experiments ranges from several minutes to hours depending on the choice of spectroscopic method. It is desirable to reduce this time overhead to not only to shorten time and laboratory resources, but also to make it possible to examine fragile specimens which quickly degrade during long experiments. In this article, we motivate using compressive sensing to significantly shorten data acquisition time by reducing the total number of measurements in ultrafast spectroscopy. We apply this technique to experimental data from ultrafast transient absorption spectroscopy and ultrafast terahertz spectroscopy and show that good estimates can be obtained with as low as 15% of the total measurements, implying a 6-fold reduction in data acquisition time.

physics.optics↗

arXiv2020

Ground-state cooling enabled by critical coupling and dark entangled states

We analyze the cooling of a mechanical resonator coupled to an ensemble of interacting two-level systems via an open quantum systems approach. Using an exact analytical result, we find optimal cooling occurs when the phonon mode is critically coupled ($γ\sim g$) to the two-level system ensemble. Typical systems operate in sub-optimal cooling regimes due to the intrinsic parameter mismatch ($γ\gg g$) between the dissipative decay rate $γ$ and the coupling factor $g$. To overcome this obstacle, we show that carefully engineering the coupling parameters through the strain profile of the mechanical resonator allows phonon cooling to proceed through the dark (subradiant) entangled states of an \emph{interacting} ensemble, thereby resulting in optimal phonon cooling. Our results provide a new avenue for ground-state cooling and should be accessible for experimental demonstrations.

quant-ph↗

arXiv2019

Coherent photon coincidence spectroscopy of single quantum systems

Non-equilibrium photon correlations of coherently excited single quantum systems can reveal their internal quantum dynamics and provide spectroscopic access. Here we propose and discuss the fundamentals of a coherent photon coincidence spectroscopy based on the application of laser pulses with variable delay and the detection of an time-averaged two-photon coincidence rate. For demonstration, two simple but important cases, i.e., an exciton - biexciton in a quantum dot and two coupled quantum emitters, are investigated based on quantum dynamics simulations demonstrating that this nonlinear spectroscopy reveals information specific to the particular single quantum system.

quant-ph↗

arXiv2019

Non-Hermitian approach for quantum plasmonics

We examine the limits of applicability of a simple non-Hermitian model for exciton/plasmon interactions in the presence of dissipation and dephasing. The model can be used as an alternative to the more complete Lindblad density matrix approach and is computationally and conceptually simpler. We find that optical spectra in the linear regime can be adequately described by this approach. The model can fail, however, under continuous optical driving in some circumstances. In the case of two quantum dots or excitons interacting with a plasmon, the model can also describe coherences and entanglement qualitatively when both dissipation and dephasing are present, and quantitatively in the limit with no dephasing. The model can also be extended to the case of many quantum dots interacting with a plasmon and results, within the single-excitation manifold, are presented for the fifty quantum dot case.

quant-ph↗

arXiv2019

Noise-Resilient Quantum Dynamics Using Symmetry-Preserving Ansatzes

We describe and demonstrate a method for the computation of quantum dynamics on small, noisy universal quantum computers. This method relies on the idea of `restarting' the dynamics; at least one approximate time step is taken on the quantum computer and then a parameterized quantum circuit ansatz is optimized to produce a state that well approximates the time-stepped results. The simulation is then restarted from the optimized state. By encoding knowledge of the form of the solution in the ansatz, such as ensuring that the ansatz has the appropriate symmetries of the Hamiltonian, the optimized ansatz can recover from the effects of decoherence. This allows for the quantum dynamics to proceed far beyond the standard gate depth limits of the underlying hardware, albeit incurring some error from the optimization, the quality of the ansatz, and the typical time step error. We demonstrate this methods on the Aubry-André model with interactions at half-filling, which shows interesting many-body localization effects in the long time limit. Our method is capable of performing high-fidelity Hamiltonian simulation hundred of time steps longer than the standard Trotter approach. These results demonstrate a path towards using small, lossy devices to calculate quantum dynamics.

quant-ph↗

arXiv2018

Comparing optimization strategies for force field parameterization

Classical molecular dynamics (MD) simulations enable modeling of materials and examination of microscopic details that are not accessible experimentally. The predictive capability of MD relies on the force field (FF) used to describe interatomic interactions. FF parameters are typically determined to reproduce selected material properties computed from density functional theory (DFT) and/or measured experimentally. A common practice in parameterizing FFs is to use least-squares local minimization algorithms. Genetic algorithms (GAs) have also been demonstrated as a viable global optimization approach, even for complex FFs. However, an understanding of the relative effectiveness and efficiency of different optimization techniques for the determination of FF parameters is still lacking. In this work, we evaluate various FF parameter optimization schemes, using as example a training data set calculated from DFT for different polymorphs of Ir$O_2$. The Morse functional form is chosen for the pairwise interactions and the optimization of the parameters against the training data is carried out using (1) multi-start local optimization algorithms: Simplex, Levenberg-Marquardt, and POUNDERS, (2) single-objective GA, and (3) multi-objective GA. Using random search as a baseline, we compare the algorithms in terms of reaching the lowest error, and number of function evaluations. We also compare the effectiveness of different approaches for FF parameterization using a test data set with known ground truth (i.e generated from a specific Morse FF). We find that the performance of optimization approaches differs when using the Test data vs. the DFT data. Overall, this study provides insight for selecting a suitable optimization method for FF parameterization, which in turn can enable more accurate prediction of material properties and chemical phenomena.

physics.comp-ph↗

arXiv2018

Reactive optical matter: light-induced motility in electrodynamically asymmetric nano-scale scatterers

From Newtons third law, the principle of actio et reactio, we expect the forces between interacting particles to be equal and opposite. However, non-reciprocal forces can arise. Specifically, this has recently been shown theoretically in the interaction between dissimilar optically trapped particles mediated by an external field. As a result, despite the incident external field not having a transverse component of momentum, the particle pair experiences a force in a direction transverse to the light propagation direction. In this letter, we directly measure the net non-reciprocal force in electrodynamically interacting nanoparticle dimers illuminated by plane waves and confined to pseudo one-dimensional geometries. We show by electrodynamic theory and simulations that inter-particle interactions cause asymmetric scattering from heterodimers and therefore, the non-reciprocal forces are a consequence of momentum conservation. Finally, we demonstrate experimentally that non-reciprocal dynamics occur generally for illuminated asymmetric scatterers.

physics.optics↗

arXiv2017

Evolutionary optimization of a charge transfer ionic potential model for Ta/Ta-oxide hetero-interfaces

Tantalum, tantalum oxide and their hetero-interfaces are of tremendous technological interest in several applications spanning electronics, thermal management, catalysis and biochemistry. For example, local oxygen stoichiometry variation in TaOx memristors comprising of metallic (Ta) and insulating oxide (Ta2O5) have been shown to result in fast switching on the sub-nanosecond timescale over a billion cycles, relevant to neuromorphic computation. Despite its broad importance, an atomistic scale understanding of oxygen stoichiometry variation across Ta/TaOx hetero-interfaces, such as during early stages of oxidation and oxide growth, is not well understood. This is mainly due to the lack of a variable charge interatomic potential model for tantalum oxides that can accurately describe the ionic interactions in the metallic (Ta) and oxide (TaOx) environment as well as at their interfaces. To address this challenge, we introduce a charge transfer ionic potential (CTIP) model for Ta/Ta-oxide system by training against lattice parameters, cohesive energies, equations of state, and elastic properties of various experimentally observed Ta2O5 polymorphs. The best set of CTIP parameters are determined by employing a single-objective global optimization scheme driven by genetic algorithms followed by local Simplex optimization. Our newly developed CTIP potential accurately predicts structure, thermodynamics, energetic ordering of polymorphs, as well as elastic and surface properties of both Ta and Ta2O5, in excellent agreement with DFT calculations and experiments. We employ our newly parameterized CTIP potential to investigate the early stages of oxidation of Ta at different temperatures and atomic/molecular nature of the oxidizing species.

cond-mat.mtrl-sci↗

arXiv2016

Unraveling the Planar-Globular Transition in Gold Nanoclusters through Evolutionary Search

Au nanoclusters are of technological relevance for catalysis, photonics, sensors, and of fundamental scientific interest owing to planar to globular structural transformation at an anomalously high number of atoms i.e. in the range 12-14. The nature and causes of this transition remain a mystery. In order to unravel this conundrum, high throughput density functional theory (DFT) calculations, coupled with a global structural optimization scheme based on a modified genetic algorithm (GA) are conducted. More than 20,000 Au$_{12}$, Au$_{13}$, and Au$_{14}$ nanoclusters are evaluated. With any DFT functional, globular and planar structures coexist across the size range of interest. The planar-globular transition is gradual at room temperature rather than a sharp transition as previously believed. The effects of anionicity, $\textit{s-d}$ band hybridization and long range interactions on the dimensional transition are quantified by using the structures adjacent to minima. Anionicity marginally changes the relative stability of the clusters. The degree of $\textit{s-d}$ hybridization is varied via changing the Hubbard U value which corroborate that $\textit{s-d}$ hybridization alone does not stabilize planar structures. van der Waals interactions, on the other hand, stabilize globular structures. These results elucidate the balance between the different reasons of the dimensional transition in gold nanoclusters.

cond-mat.mtrl-sci↗

arXiv2015

Describing the diverse geometries of gold from nanoclusters to bulk-- a first-principles based hybrid bond order potential

Molecular dynamics simulations using empirical force fields (EFFs) are crucial for gaining fundamental insights into atomic structure and long timescale dynamics of Au nanoclusters with far-reaching applications in energy and devices. This approach is thwarted by the failure of currently available EFFs in describing the size-dependent dimensionality and diverse geometries exhibited by Au clusters (e.g., planar, hollow cages, pyramids). Owing to their ability to account for bond directionality, bond-order based EFFs, such as the Tersoff-type Bond Order Potential (BOP), are well suited for such a description. Nevertheless, the predictive power of existing BOP parameters is severely limited in the nm length scale owing to the predominance of bulk Au properties used to train them. Here, we mitigate this issue by introducing a new hybrid bond order potential (HyBOP), which account for (a) short-range interactions via Tersoff-type BOP terms and (b) long-range effects by a scaled LJ term whose contribution depends on the local atomic density. We optimized the independent parameters for our HyBOP using a global optimization scheme driven by genetic algorithms. Moreover, to ensure good transferability of these parameters across different length scales, we used an extensive training dataset encompasses structural and energetic properties of a thousand 13-atom Au clusters, surface energies, as well as bulk polymorphs, obtained from density functional theory (DFT) calculations. Our newly developed HyBOP has been found to accurately describe (a) global minimum energy configurations at different clusters sizes, (b) critical size of transition from planar to globular clusters, (c) evolution of structural motifs with cluster size, and (d) thermodynamics, structure, elastic properties of bulk polymorphs as well as surfaces, in excellent agreement with DFT calculations and spectroscopic experiments.

cond-mat.mtrl-sci↗

arXiv2013

The refraction of surface plasmon polaritons

We show how a complex Snell's law can be used to describe the refraction of surface plasmon polaritons (SPPs) at an interface between two metals, validating its predictions with 3-D electrodynamics simulations. Refraction gives rise to peculiar SPP features including inhomogeneities in the waveform and dispersion relations that depend on the incident wave and associated material. These features make it possible to generate SPPs propagating away from the interface with significant confinement normal to the propagation direction. We also show that it is possible to encode optical properties of the incident material into the refracted SPP. These consequences of metal-metal SPP refraction provide new avenues for the design of plasmonics-based devices.

cond-mat.mes-hall↗

arXiv2013

Ultrafast Reversal of a Fano Resonance in a Plasmon-Exciton System

When a two-level quantum dot and a plasmonic metal nanoantenna are resonantly coupled by the electromagnetic near field, the system can exhibit a Fano resonance, resulting in a transparency dip in the optical spectrum of the coupled system. We calculate the nonlinear response of such a system, for illumination both by continuous-wave and ultrafast pulsed lasers, using both a cavity quantum electrodynamics and a semiclassical coupled-oscillator model. For the experimentally relevant case of meV thermal broadening of the quantum-dot transition, we predict that femtosecond pulsed illumination can lead to a reversal of the Fano resonance, with the induced transparency changing into a superscattering spike in the spectrum. This ultrafast reversal is due to a transient change in the phase relationship between the dipoles of the plasmon and the quantum dot. It thus represents a new approach to dynamically control the collective optical properties and coherence of coupled nanoparticle systems.

cond-mat.mes-hall↗