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At least 685 records · Page 38
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Perspective—Emergent Phases in Rare Earth Nickelate Heterostructure

The prediction of high T c superconductivity in layers of LaNiO 3 through orbital engineering has led to extensive research efforts over the last fifteen years. During this period, a plethora of thin films and heterostructures based rare-earth nickelate family with perovskite structure has been synthesized and explored. Here, in this short perspective, we briefly review the complexity of bulk RENiO 3 , spotlighting several recent findings of emergent phenomena in heterostructures containing the interface between RENiO 3 and another transition metal oxide. Finally, we outline potentially interesting future directions linked to time-domain dynamics to harness new Mott and topological phases in artificial structures of RENiO 3 .

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

Non-classical ion-indiffusion processes in quasi-one-dimensional ionic conductor KTiOPO4

Developments in coercive field engineering and waveguide writing via ion-exchange in the ferroelectric ionic-conductor KTiOPO4 (KTP) have led to breakthroughs within the field of nonlinear optics and quantum photonics. However, the microscopic diffusion dynamics of ion-exchange in KTP are poorly understood and show signs of non-classical diffusion dynamics. The precise control of ion-exchange gradients is critical for developing KTP into a mature, integrated nonlinear optical material but requires a level of control that, in turn, demands a deeper understanding of the ion-exchange process. We employ direct ToF-SIMS mapping to untangle the complex diffusion dynamics of the commonly used ion-exchange dopant ions: Rb, Ba, and K. We map periodic diffusion gradients of two exchanges, one dominated by Rb-ions and the other by Ba-ions. For the first time, we show the interdependent nature of the Ba- and Rb ion in the ion-exchange diffusion gradient. The low incorporation of the Ba ion is mapped and quantified, and dopant–crystal interactions are identified. This work highlights the complex diffusion dynamics of dopants in the KTP structure and lays the foundation for deterministic control of diffusion gradients for the next generation of integrated nonlinear and quantum photonic devices.

Barrett, Laura [ORNL]↗
DOE OSTI2022

Active and tunable nanophotonic metamaterials

Abstract Metamaterials enable subwavelength tailoring of light–matter interactions, driving fundamental discoveries which fuel novel applications in areas ranging from compressed sensing to quantum engineering. Importantly, the metallic and dielectric resonators from which static metamaterials are comprised present an open architecture amenable to materials integration. Thus, incorporating responsive materials such as semiconductors, liquid crystals, phase-change materials, or quantum materials (e.g., superconductors, 2D materials, etc.) imbue metamaterials with dynamic properties, facilitating the development of active and tunable devices harboring enhanced or even entirely novel electromagnetic functionality. Ultimately, active control derives from the ability to craft the local electromagnetic fields; accomplished using a host of external stimuli to modify the electronic or optical properties of the responsive materials embedded into the active regions of the subwavelength resonators. We provide a broad overview of this frontier area of metamaterials research, introducing fundamental concepts and presenting control strategies that include electronic, optical, mechanical, thermal, and magnetic stimuli. The examples presented range from microwave to visible wavelengths, utilizing a wide range of materials to realize spatial light modulators, effective nonlinear media, on-demand optics, and polarimetric imaging as but a few examples. Often, active and tunable nanophotonic metamaterials yield an emergent electromagnetic response that is more than the sum of the parts, providing reconfigurable or real-time control of the amplitude, phase, wavevector, polarization, and frequency of light. The examples to date are impressive, setting the stage for future advances that are likely to impact holography, beyond 5G communications, imaging, and quantum sensing and transduction.

36 MATERIALS SCIENCE↗
DOE OSTI2020

From magnetic order to quantum disorder in the Zn-barlowite series of S = 1/2 kagomé antiferromagnets

We report a comprehensive muon spectroscopy study of the Zn-barlowite series of $S=\frac{1}{2}$ kagomé antiferromagnets, Zn x Cu 4-x (OH) 6 FBr, for x= 0.00 to 0.99(1). By combining muon spin relaxation and rotation measurements with state-of-the-art density-functional theory muon-site calculations, we observe the formation of both μ–F and μ–OH complexes in Zn-barlowite. From these stopping sites, implanted muon spins reveal the suppression of long-range magnetic order into a possible quantum spin liquid state upon the increasing concentration of Zn-substitution. In the parent compound (x = 0), static long-range magnetic order below T N = 5 K manifests itself in the form of spontaneous oscillations in the time-dependent muon asymmetry signal consistent with the dipolar fields expected from the calculated muon stopping sites and the previously determined magnetic structure of barlowite. Meanwhile, in the x = 1.0 end-member of the series—in which antiferromagnetic kagomé layers of Cu 2+ $S=\frac{1}{2}$ moments are decoupled by diamagnetic Zn 2+ ions—we observe that dynamic magnetic moment fluctuations persist down to at least 50 mK, indicative of a quantum disordered ground state. We demonstrate that this crossover from a static to dynamic magnetic ground state occurs for compositions of Zn-barlowite with x > 0.5, which bears resemblance to the dynamical behaviour of the widely studied Zn-paratacamite series that contains the quantum spin liquid candidate herbertsmithite.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Mixed gauge-global symmetries, elliptic modes, and black hole thermodynamics in Hořava-Lifshitz gravity

In Hořava-Lifshitz gravity, a putative consistent theory of quantum gravity for which there is evidence for both black hole thermodynamics and a holographic construction, spacetime is endowed with a preferred dynamical spacelike foliation. The theory has a leaf reparameterization symmetry that is neither global nor local gauge, hyperbolic and elliptic equations of motion, a lack of splittability, and universal horizon black hole solutions. The reparameterization symmetry is “mixed”: it is a local symmetry in one coordinate yet global on each leaf. More broadly it is an example of both unfree and projectable gauge symmetries. The mixed symmetry and associated charge has not yet been accounted for in calculations of universal horizon thermodynamics in Hořava-Lifshitz gravity. This has led to problems, in particular the failure of the first law in a class of asymptotically AdS solutions where the normal to the leaves of the foliation is not aligned with the time translation Killing vector at infinity. We show how the dynamics of the charge corresponding to this symmetry coupled with the other features above resolves this issue. We then briefly comment how this mixed symmetry, the corresponding charge, and the elliptic equations of motion also conspire to evade recent holographic arguments for only local gauge fields in consistent theories of quantum gravity due to the lack of splittability of the elliptic equation and associated mode.

Global Symmetries↗
DOE OSTI2022

Nonlinear Anti-(Parity-Time) Symmetric Dimer

In the present work we propose a nonlinear anti- P T -symmetric dimer, that at the linear level has been experimentally created in the realm of electric circuit resonators. We find four families of solutions, the so-called upper and lower branches, both in a symmetric and in an asymmetric (symmetry-broken) form. We unveil analytically and confirm numerically the critical thresholds for the existence of such branches and explore the bifurcations (such as saddle-node ones) that delimit their existence, as well as transcritical ones that lead to their potential exchange of stability. We find that out of the four relevant branches, only one, the upper symmetric branch, corresponds to a spectrally and dynamically robust solution. We subsequently leverage detailed direct numerical computations in order to explore the dynamics of the different states, corroborating our spectral analysis results.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRSDate not supplied

Dynamical Decoupling of Crosstalk on Superconducting Qubit Devices

Current NISQ devices are prone to errors. In order to be used for practical applications or achieve fault-tolerant thresholds, strategies to suppress error rates will be needed to maximize the potential of noisy devices. Dynamical decoupling (DD) is one such strategy for suppressing — or at least alleviating — the effects of decoherence, in which sequences of pulses are applied to qubits to decouple their interaction with the environment. Through experimental runs performed on several Rigetti quantum computing units (QPUs), we first demonstrate that DD is capable of improving coherence times for isolated qubits, as well as suppressing errors caused by the ZZ coupling between pairs of qubits. Extending this framework to cycles containing2-qubit gates, we show that DD can be inserted to decouple qubits from crosstalk occurring during neighboring 2-qubit gates, and demonstrate the efficacy of this procedure on quantum approximate optimization algorithm (QAOA) circuits. We also explore the usage of tailored DD sequences for the suppression of characterized error channels. We are grateful for support from the NASA Ames Research Center and from the DARPA ONISQ program under interagency agreement IAA 8839,Annex 114. HYH is supported by the USRA Feynman QuantumAcademy funded by the NAMS R&D Student Program and a UCHellman Fellowship. JS, ZGI and ZW are supported by USRA NASAAcademic Mission Service (NNA16BD14C).

Dynamical decoupling↗
DOE OSTI2025

Enhanced quasiparticle relaxation in a superconductor via the proximity effect

Quasiparticle dynamics have been identified as an important factor in the operational performance of superconductors in quantum computing and sensing applications. In order to study such dynamics, we performed measurements of quasiparticle transport in a superconductor engineered to enhance quasiparticle relaxation. We found that a thin, highly disordered normal metal layer can be used to greatly reduce the relaxation time of quasiparticles in a superconductor, as seen by a large reduction in the quasiparticle charge imbalance in a fully proximitized Cu/Al bilayer wire, without significantly affecting the properties of the superconductor. The enhanced relaxation is likely due to an increased electron–electron scattering rate in the disordered normal metal. Our results provide a positive indication that quasiparticle relaxation can be substantially enhanced via a simple and technologically viable method, and demonstrate that direct measurement of quasiparticle imbalance can be a useful tool for the assessment and engineering of superconductors in various applications at mK temperatures.

Ryan, Kevin M. [Northwestern U.] (ORCID:0000000293↗
DOE OSTI2022

Sensitivity of time-dependent density functional theory to initial conditions

Time-dependent density-functional theory is mathematically formulated through nonlinear coupled time-dependent three-dimensional partial differential equations, and it is natural to expect a strong sensitivity of its solutions to variations of the initial conditions, akin to the butterfly effect ubiquitous in classical dynamics. Since the Schrödinger equation for an interacting many-body system is, however, linear and mathematically the exact equations of the density-functional theory reproduce the corresponding one-body properties, it would follow that the Lyapunov exponents are also vanishing within a density-functional theory framework. Whether for realistic implementations of the time-dependent density-functional theory the question of the absence of the butterfly effect and whether the dynamics provided is indeed a predictable theory was never discussed. At the same time, since the time-dependent density-functional theory is a unique tool allowing us to study the nonequilibrium dynamics of strongly interacting many-fermion systems, the question of predictability of this theoretical framework is of paramount importance. Here our analysis, for a number of quantum superfluid many-body systems (unitary Fermi gas, nuclear fission, and heavy-ion collisions) with a classical equivalent number of degrees of freedom O(10 10 ) and larger, suggests that its maximum Lyapunov exponents are negligible for all practical purposes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Distributed Quantum Learning with co-Management in a Multi-tenant Quantum System

The rapid advancement of quantum computing has pushed classical designs into the quantum domain, breaking physical boundaries for computing-intensive and data-hungry applications with the hope that some systems may provide a quantum speedup. For example, variational quantum algorithms have been proposed for quantum neural networks to train deep learning models on qubits, achieving promising results. Existing quantum learning architectures and systems rely on single, monolithic quantum machines with abundant and stable resources, such as qubits. However, fabricating a large, monolithic quantum device is considerably more challenging than producing an array of smaller devices. In this paper, we investigate a distributed quantum system that combines multiple quantum machines into a unified system. We propose DQuLearn, which divides a quantum learning task into multiple subtasks. Each subtask can be executed distributively on individual quantum machines, with the results looping back to classical machines for subsequent training iterations. Additionally, our system supports multiple concurrent clients and dynamically manages their circuits according to the runtime status of quantum workers. Through extensive experiments, we demonstrate that DQuLearn achieves similar accuracies with significant runtime reduction, by up to 68.7% and an increase per-second circuit processing speed, by up to 3.99 times, in a 4-worker multi-tenant setting.

quantum computing↗
DOE OSTI2022

On the use of vibronic coherence to identify reaction coordinates for ultrafast excited-state dynamics of transition metal-based chromophores

In this study, the question of whether one can use information from quantum coherence as a means of identifying vibrational degrees of freedom that are active along an excited-state reaction coordinate is discussed. Specifically, we are exploring the notion of whether quantum oscillations observed in single-wavelength kinetics data exhibiting coherence dephasing times that are intermediate between that expected for either pure electronic or pure vibrational dephasing are vibronic in nature and therefore may be coupled to electronic state-to-state evolution. In the case of a previously published Fe(ιι) polypyridyl complex, coherences observed subsequent to 1 A 1 → 1 MLCT excitation were linked to large-amplitude motion of a portion of the ligand framework; dephasing times on the order of 200–300 fs suggested that these degrees of freedom could be associated with ultrafast (~100 fs) conversion from the initially formed MLCT excited state to lower-energy, metal-centered ligand-field excited state(s) of the compound. Incorporation of an electronically benign but sterically restrictive Cu(ι) ion into the superstructure designed to interfere with this motion yielded a compound exhibiting a ~25-fold increase in the compound’s MLCT lifetime, a result that was interpreted as confirmation of the initial hypothesis. However, new data acquired on a different chemical system – Cr(acac') 3 (where acac' represents various derivatives of acetylacetonate) – yielded results that call into question this same hypothesis. Coherences observed subsequent to 4 A 2 → 4 T 2 ligand-field excitation on a series of molecules implicated similar vibrational degrees of freedom across the series, but exhibited dephasing times ranging from 340 fs to 2.5 ps without any clear correlation to the dynamics of excited-state evolution in the system. Taken together, the results obtained on both of these chemical platforms suggest that while identification of coherences can indeed point to degrees of freedom that should be considered as candidate modes for defining reaction trajectories, our understanding of the factors that determine the interplay across coherences, dephasing times, and electronic and geometric structure is insufficient at the present time to view this parameter as a robust metric for differentiating active versus spectator modes for ultrafast dynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Quantum dynamics of non-Hermitian many-body Landau-Zener systems

Here, we develop a framework to solve a large class of linearly driven non-Hermitian quantum systems. Such a class of models in the Hermitian scenario is commonly known as multistate Landau-Zener models. The non-Hermiticity is due to the anti-Hermitian couplings between the diabatic levels. We find that there exists a conservation law, unique to this class of models, that describes the simultaneous growth of the unnormalized wave functions. These models have practical applications in Bose-Einstein condensates, and they can describe the dynamics of multispecies bosonic systems. The conservation law relates to a pair-production mechanism that explains the dissociation of diatomic molecules into atoms. We provide a general framework for both solvable and semiclassically solvable non-Hermitian Landau-Zener models. Our findings will open alternative avenues for a number of diverse emergent phenomena in explicitly time-dependent non-Hermitian quantum systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Frontier nonequilibrium materials science enabled by ultrafast electron methods

Most innovation in materials science and engineering resides in our ability to understand and control the intimate relationship between the structure of materials and their properties. Conventionally, the only route to discovering innovative new material properties has been to explore the structural and compositional phase space that is accessible at (or near) thermodynamic equilibrium. The characterization, manipulation and, ultimately, control of material properties far from equilibrium offers almost completely untapped possibilities for uncovering novel states and phases of materials. Investigations of materials far from equilibrium require the development of new techniques, which are capable of following dynamic processes in materials with extreme spatiotemporal resolution. Thus, ultrafast electron-based methods have become a major new frontier in materials science due to the capability of following dynamics on time scales as short as femtoseconds with the high spatial resolution and sensitivity afforded by electrons. The articles in this issue provide an exciting cross section of the novel research directions that have been enabled at this frontier. Imaging on ultrafast time scales carries critical information on phase transitions, fundamental processes involved in light-harvesting, magnetic, and plasmonic dynamics, the coupling of electronic and nuclear degrees of freedom in materials and has revealed previously hidden, nonequilibrium metastable states of matter that have no equilibrium analog.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Enhancing Coherence Limits in Superconducting Quantum Systems for Computing and Sensing

This talk will highlight recent efforts at the SQMS Center to develop qudit-based quantum computing architectures using superconducting three-dimensional (3D) cavities, as well as the use of these ultra-coherent cavities for quantum sensing. I will present systematic studies of materials and devices aimed at identifying and mitigating the dominant sources of decoherence—including two-level systems (TLS), quasiparticles, and other noise mechanisms—in both transmons and 3D cavities. These investigations include microwave loss characterization of niobium, tantalum, aluminum, their native oxides, and substrate materials such as silicon and sapphire. By combining measurements on qubits and cavities, we disentangle subsystem-specific loss mechanisms and establish a hierarchy of mitigation strategies, leading to transmon coherence times exceeding one millisecond. I will also discuss studies of quasiparticle dynamics, including quasiparticle bursts observed in qubits operated both above ground and at the Gran Sasso underground laboratory, and the observation that applied magnetic fields can suppress temporal T₁ fluctuations. Building on these advances, we demonstrate a record-coherence two-cell cavity-qudit system with coherence times exceeding 20 milliseconds. Leveraging tunable sideband interactions together with error-resilient protocols, including measurement-based error correction and post-selection, we achieve high-fidelity quantum state control, including the preparation of Fock states up to N=20 with fidelities above 95% and the generation of high-fidelity two-mode entangled states. Finally, I will discuss how these ultra-coherent quantum systems are enabling emerging quantum sensing applications, including searches for dark matter and gravitational waves.

Roy, Tanay [Fermilab] (ORCID:000000019442862X)↗
DOE OSTI2026

Quantum Routing and Entanglement Dynamics Through Bottlenecks

To implement arbitrary quantum circuits in architectures with restricted interactions, one may effectively simulate all-to-all connectivity by routing quantum information. We consider the entanglement dynamics and routing between two regions only connected through an intermediate “bottleneck” region with few qubits. In such systems, where the entanglement rate is restricted by a vertex boundary rather than an edge boundary of the underlying interaction graph, existing results such as the small incremental entangling theorem give only a trivial constant lower bound on the routing time (the minimum time to perform an arbitrary permutation). We significantly improve the lower bound on the routing time in systems with a vertex bottleneck. Specifically, for any system with two regions 𝐿,𝑅 with 𝑁 𝐿 ,𝑁 𝑅 qubits, respectively, coupled only through an intermediate region 𝐶 with 𝑁 𝐶 qubits, for any 𝛿 > 0 we show a lower bound of Ω⁢(𝑁$^{1−𝛿}_{𝑅}$/√𝑁 𝐿⁢ 𝑁 𝐶 ) on the Hamiltonian quantum routing time when using piecewise time-independent Hamiltonians, or time-dependent Hamiltonians subject to a smoothness condition. We also prove an upper bound on the average amount of bipartite entanglement between 𝐿 and 𝐶,𝑅 that can be generated in time 𝑡 by such architecture-respecting Hamiltonians in systems constrained by vertex bottlenecks, improving the scaling in the system size from 𝑂⁡(𝑁 𝐿⁢ 𝑡) to 𝑂⁡(√𝑁 𝐿⁢ 𝑡). As a special case, when applied to the star graph (i.e., one vertex connected to 𝑁 leaves), we obtain an Ω⁡(√𝑁 1−𝛿 ) lower bound on the routing time and on the time to prepare 𝑁/2 Bell pairs between the vertices. We also show that, in systems of free particles, we can route optimally on the star graph in time Θ⁡(√𝑁) using Hamiltonian quantum routing, obtaining a speedup over gate-based routing, which takes time Θ⁡(𝑁).

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2023

Extracting the Quantum Hall Conductance from a Single Bulk Wave Function

In this work, we propose a new formula that extracts the quantum Hall conductance from a single (2+1)⁢ D gapped wave function. The formula applies to general many-body systems that conserve particle number, and is based on the concept of modular flow, i.e., unitary dynamics generated from the entanglement structure of the wave function. The formula is shown to satisfy all formal properties of the Hall conductance: it is odd under time reversal and reflection, even under charge conjugation, universal and topologically rigid in the thermodynamic limit. Further evidence for relating the formula to the Hall conductance is obtained from conformal field theory arguments. Finally, we numerically check the formula by applying it to a noninteracting Chern band where excellent agreement is obtained.

2-dimensional systems↗
DOE OSTI2020

Uncovering the Role of Hole Traps in Promoting Hole Transfer from Multiexcitonic Quantum Dots to Molecular Acceptors

The understanding of electronic dynamics in multiexcitonic quantum dots (QDs) is important for designing efficient systems useful in high power scenarios, such as solar concentrators and multielectron charge transfer. The multiple charge carriers within a QD can undergo undesired Auger recombination events, which rapidly annihilate carriers on picosecond time scales and generate heat from absorbed photons instead of useful work. Compared to the transfer of multiple electrons, the transfer of multiple holes has proven to be more difficult due to slower hole transfer rates. To probe the competition between Auger recombination and hole transfer in CdSe, CdS, and CdSe/CdS QDs of varying sizes, we synthesized a phenothiazine derivative with optimized functionalities for binding to QDs as a hole accepting ligand and for spectroscopic observation of hole transfer. Transient absorption spectroscopy was used to monitor the photoinduced absorption features from both trapped holes and oxidized ligands under excitation fluences where the averaged initial number of excitons in a QD ranged from ~1 to 19. We observed fluence-dependent hole transfer kinetics that last around 100 ps longer than the predicted Auger recombination lifetimes, and the transfer of up to 3 holes per QD. Theoretical modeling of the kinetics suggests that binding of hole acceptors introduces trapping states significantly different from those in native QDs passivated with oleate ligands. Holes in these modified trap states have prolonged lifetimes, which promotes the hole transfer efficiency. These results highlight the beneficial role of hole-trapping states in devising hole transfer pathways in QD-based systems under multiexcitonic conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗