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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Restriction-In-Motion of Surface Ligands Enhances Photoluminescence of Quantum Dots - Experiment and Theory

Here the relationship between emission and ligand restriction of a series of ZnSe/ZnS quantum dots (QDs) encapsulated in nanoparticles is investigated systematically via experiments and quantum theory. The QDs have a ZnSe core and a ZnS shell, capped with hydrophobic ligands (triotylphosphine oxide/hexadecylamine), allowing them to be entrapped in a model biomembrane, bicelle, made of zwitterionic dipalmitoyl and dihexanoyl phosphatidylcholines and charged dipalmitoyl phosphatidylglycerol. Enhanced photoluminescence is observed upon encapsulation, depending on the QD-to-lipid ratio. Transmission electron microscopy and small-angle X-ray scattering confirm that QDs are preferably situated at the rim of bicellar discs. A simplified quantum dissipation heat-bath theory is proposed to correlate the enhancement with slower nonradiative processes caused by the restriction-in-motion (RIM) of the surface ligands. However, Fõrster resonance energy transfer due to QD aggregation counteracts the effect.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Zero Crossing Steps and Anomalous Shapiro Maps in Graphene Josephson Junctions

The AC Josephson effect manifests itself in the form of “Shapiro steps” of quantized voltage in Josephson junctions subject to radio frequency (RF) radiation. This effect presents an early example of a driven–dissipative quantum phenomenon and is presently utilized in primary voltage standards. Shapiro steps have also become one of the standard tools to probe junctions made in a variety of novel materials. Here we study Shapiro steps in a widely tunable graphene-based Josephson junction in which the high- frequency dynamics is determined by the on-chip environment. We investigate the variety of patterns that can be obtained in this well-understood system depending on the carrier density, temperature, RF frequency, and magnetic field. Although the patterns of Shapiro steps can change drastically when just one parameter is varied, the overall trends can be understood and the behaviors straightforwardly simulated, showing some key differences from the conventional RCSJ model. The resulting understanding may help interpret similar measurements in more complex materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Tunable Ferromagnetism in LaCoO 3 Epitaxial Thin Films

We report ferromagnetic insulators play a crucial role in the development of low-dissipation quantum magnetic devices for spintronics. Epitaxial LaCoO 3 thin film is a prominent ferromagnetic insulator, in which the robust ferromagnetic ordering emerges owing to epitaxial strain. Whereas it is evident that strong spin-lattice coupling induces ferromagnetism, the reported ferromagnetic properties of epitaxially strained LaCoO 3 thin films are highly consistent. For example, even under largely modulated degree of strain, the reported Curie temperatures of epitaxially strained LaCoO 3 thin films lie in a narrow range of 80–85 K, without much deviation. In this study, substantial enhancement (≈18%) in the Curie temperature of epitaxial LaCoO 3 thin films is demonstrated via crystallographic orientation dependence. By changing the crystallographic orientation of the films from (111) to (110), the crystal-field energy is reduced and the charge transfer between the Co and O orbitals is enhanced. These modifications lead to a considerable enhancement of the ferromagnetic properties (including the Curie temperature and magnetization), despite the identical nominal degree of epitaxial strain. The findings of this study provide insights into facile tunability of ferromagnetic properties via structural symmetry control in LaCoO 3 .

36 MATERIALS SCIENCE↗
DOE OSTI2021

Influence of solution phase environmental heterogeneity and fluctuations on vibronic spectra: Perylene diimide molecular chromophore complexes in solution

Ensembles of ab initio parameterized Frenkel-exciton model Hamiltonians for different perylene diimide dimer systems are used, together with various dissipative quantum dynamics approaches, to study the influence of the solvation environment and fluctuations in chromophore relative orientation and packing on the vibronic spectra of two different dimer systems: a π-stacked dimer in aqueous solution in which the relative chromophore geometry is strongly confined by a phosphate bridge and a side-by-side dimer in dichloromethane involving a more flexible alkyne bridge that allows quasi-free rotation of the chromophores relative to one another. These entirely first-principles calculations are found to accurately reproduce the main features of the experimental absorption spectra, providing a detailed mechanistic understanding of how the structural fluctuations and environmental interactions influence the vibronic dynamics and spectroscopy of solutions of these multi-chromophore complexes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Excitons: Energetics and spatiotemporal dynamics

The concept of an exciton as a quasiparticle that represents collective excited states was originally adapted from solid-state physics and has been successfully applied to molecular aggregates by relying on the well-established limits of the Wannier exciton and the Frenkel exciton. However, the study of excitons in more complex chemical systems and solid materials over the past two decades has made it clear that simple concepts based on Wannier or Frenkel excitons are not sufficient to describe detailed excitonic behavior, especially in nano-structured solid materials, multichromophoric macromolecules, and complex molecular aggregates. In addition, important effects such as vibronic coupling, the influence of charge-transfer (CT) components, spin-state interconversion, and electronic correlation, which had long been studied but not fully understood, have turned out to play a central role in many systems. This has motivated new experimental approaches and theoretical studies of increasing sophistication. This article provides an overview of works addressing these issues that were published for A Special Topic of the Journal of Chemical Physics on ``Excitons: Energetics and spatio-temporal dynamics" and discusses their implications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Dynamics of photosynthetic light harvesting systems interacting with N-photon Fock states

Here, we develop a method to simulate the excitonic dynamics of realistic photosynthetic light harvesting systems, including non-Markovian coupling to phonon degrees of freedom, under excitation by N-photon Fock state pulses. This method combines the input–output and the hierarchical equations of motion formalisms into a double hierarchy of density matrix equations. We show analytically that under weak field excitation relevant to natural photosynthesis conditions, an N-photon Fock state input and a corresponding coherent state input give rise to equal density matrices in the excited manifold. However, an N-photon Fock state input induces no off-diagonal coherence between the ground and excited subspaces, in contrast with the coherences created by a coherent state input. We derive expressions for the probability to absorb a single Fock state photon with or without the influence of phonons. For short pulses (or, equivalently, wide bandwidth pulses), we show that the absorption probability has a universal behavior that depends only upon a system-dependent effective energy spread parameter Δ and an exciton–light coupling constant Γ. This holds for a broad range of chromophore systems and for a variety of pulse shapes. We also analyze the absorption probability in the opposite long pulse (narrow bandwidth) regime. We then derive an expression for the long time emission rate in the presence of phonons and use it to study the difference between collective vs independent emission. Finally, we present a numerical simulation for the LHCII monomer (14-mer) system under single photon excitation that illustrates the use of the double hierarchy equations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Zero-cost corrections to influence functional coefficients from bath response functions

Recent work has shown that it is possible to circumvent the calculation of the spectral density and directly generate the coefficients of the discretized influence functionals using data from classical trajectory simulations. However, the accuracy of this procedure depends on the validity of the high temperature approximation. In this work, an alternative derivation based on the Kubo formalism is provided. This enables the calculation of additional correction terms that increases the range of applicability of the procedure to lower temperatures. Because it is based on the Kubo-transformed correlation function, this approach allows the direct use of correlation functions obtained from methods such as ring-polymer molecular dynamics and centroid molecular dynamics in determining the influence functional coefficients for subsequent system-solvent simulations. The accuracy of the original procedure and the corrected procedure is investigated across a range of parameters. It is interesting that the correction term comes at zero additional cost. Furthermore, it is possible to improve upon the correction using zero-cost physical intuition and heuristics making the method even more accurate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Non-equilibrium rate theory for polariton relaxation dynamics

We derive an analytic expression of the non-equilibrium Fermi’s golden rule (NE-FGR) expression for a Holstein–Tavis–Cumming Hamiltonian, a universal model for many molecules collectively coupled to the optical cavity. These NE-FGR expressions capture the full-time-dependent behavior of the rate constant for transitions from polariton states to dark states. The rate is shown to be reduced to the well-known frequency domain-based equilibrium Fermi’s golden rule (E-FGR) expression in the equilibrium and collective limit and is shown to retain the same scaling with the number of sites in non-equilibrium and non-collective cases. We use these NE-FGR to perform population dynamics with a time-non-local and time-local quantum master equation and obtain accurate population dynamics from the initially occupied upper or lower polariton states. Furthermore, NE-FGR significantly improves the accuracy of the population dynamics when starting from the lower polariton compared to the E-FGR theory, highlighting the importance of the non-Markovian behavior and the short-time transient behavior in the transition rate constant.

Chemical dynamics↗
DOE OSTI2025

Tree tensor network hierarchical equations of motion based on time-dependent variational principle for efficient open quantum dynamics in structured thermal environments

In this work, we introduce an efficient method, TTN-HEOM, for exactly calculating the open quantum dynamics for driven quantum systems interacting with highly structured bosonic baths by combining the tree tensor network (TTN) decomposition scheme with the bexcitonic generalization of the numerically exact hierarchical equations of motion (HEOM). The method yields a series of quantum master equations for all core tensors in the TTN that efficiently and accurately capture the open quantum dynamics for non-Markovian environments to all orders in the system–bath interaction. These master equations are constructed based on the time-dependent Dirac–Frenkel variational principle, which isolates the optimal dynamics for the core tensors given the TTN ansatz. The dynamics converges to the HEOM when increasing the rank of the core tensors, a limit in which the TTN ansatz becomes exact. We introduce TENSO, tensor equations for non-Markovian structured open systems, as a general-purpose Python code to propagate the TTN-HEOM dynamics. We implement three general propagators for the coupled master equations: two fixed-rank methods that require a constant memory footprint during the dynamics and one adaptive-rank method with a variable memory footprint controlled by the target level of computational error. We exemplify the utility of these methods by simulating a two-level system coupled to a structured bath containing one Drude–Lorentz component and eight Brownian oscillators, which is beyond what can presently be computed using the standard HEOM. Our results show that the TTN-HEOM is capable of simulating both dephasing and relaxation dynamics of driven quantum systems interacting with structured baths, even those of chemical complexity, with an affordable computational cost.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Ultrafast local demagnetization in 𝑑 6 systems via driven Jahn-Teller distortions

Ultrafast control of spin orientations without relying on highly nonequilibrium electron distributions offers a new pathway for femtosecond spintronics. It is shown that excitation of specific vibronic modes can drive a substantial demagnetization of a local moment relative to the magnetization axis, while preserving its total spin quantum number. Using a fully quantum many-body treatment of a local 𝑆=2 (𝑑 6 ) many-body spin coupled to a driven Jahn-Teller mode with quantum dissipation, we find that the projected spin can be strongly reduced via a Jahn-Teller-induced 𝑥⁢𝑦↑→𝑦⁢𝑧/𝑧⁢𝑥↓ transition, which occurs without additional Coulomb exchange cost. The excited state subsequently relaxes back to its original electronic configuration with a rotated spin direction, enabling spin reorientation without generating a large net angular momentum in the electronic subsystem.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Lifetime renormalization of driven weakly anharmonic superconducting qubits. II. The readout problem

Recent experiments in superconducting qubit systems have shown an unexpectedly strong dependence of the qubit relaxation rate on the readout drive power. This phenomenon limits the maximum measurement strength and thus the achievable readout speed and fidelity. We address this problem here and provide a plausible mechanism for drive-power dependence of relaxation rates. To this end we introduce a two-parameter perturbative expansion in qubit anharmonicity and the drive amplitude through a unitary transformation technique introduced in Part I. This approach naturally reveals number-nonconserving terms in the Josephson potential as a fundamental mechanism through which applied microwave drives can activate additional relaxation mechanisms. Here, we present our results in terms of an effective master equation with renormalized state- and drive-dependent transition frequency and relaxation rates. Comparison of numerical results from this effective master equation to those obtained from a Lindblad master equation which only includes number-conserving terms (i.e., Kerr interactions) shows that number-nonconserving terms can lead to significant drive-power dependence of the relaxation rates. The systematic expansion technique introduced here is of general applicability to obtaining effective master equations for driven-dissipative quantum systems that contain weakly nonlinear degrees of freedom.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Bulk dissipation in the quantum anomalous Hall effect

Even at the lowest accessible temperatures, measurements of the quantum anomalous Hall (QAH) effect have indicated the presence of parasitic dissipative conduction channels. There is no consensus whether parasitic conduction is related to processes in the bulk or along the edges. Here, we approach this problem by comparing transport measurements of Hall bar and Corbino geometry devices fabricated from Cr-doped (BiSb) 2 Te 3 . We identify bulk conduction as the dominant source of dissipation at all values of temperature and in-plane electric field. Furthermore, we observe identical breakdown phenomenology in both geometries, indicating that breakdown of the QAH phase is a bulk process. The methodology developed in this study could be used to identify dissipative conduction mechanisms in new QAH materials, ultimately guiding material development towards realization of the QAH effect at higher temperatures

36 MATERIALS SCIENCE↗
DOE OSTI2022

Distinguishing between Quantum and Classical Markovian Dephasing Dissipation

Understanding whether dissipation in an open quantum system is truly quantum is a question of both fundamental and practical interest. We consider n qubits subject to correlated Markovian dephasing and present a sufficient condition for when bath-induced dissipation can generate system entanglement and hence must be considered quantum. Surprisingly, we find that the presence or absence of time-reversal symmetry plays a crucial role: broken time-reversal symmetry is required for dissipative entanglement generation. Further, simply having nonzero bath susceptibilities is not enough for the dissipation to be quantum. We also present an explicit experimental protocol for identifying truly quantum dephasing dissipation and lay the groundwork for studying more complex dissipative systems and finding optimal noise mitigating strategies.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

General framework for quantifying dissipation pathways in open quantum systems. III. Off-diagonal subsystem–bath couplings

This paper extends the previously reported theory of dissipation pathways [C. W. Kim and I. Franco, J. Chem. Phys. 160, 214111 (2024)] to incorporate off-diagonal subsystem–bath coupling, which is often required to model molecular systems where the environment directly influences transitions and couplings between subsystem states. We systematically derive master equations for both population transfer and dissipation into individual bath components, for which we also rigorously prove energy conservation and detailed balance. The approach is based on second-order perturbation theory with respect to the subsystem–bath couplings, whose form is not limited to any specific model. The accuracy of the developed method is tested by applying it to diverse model Hamiltonians involving linearly coupled harmonic oscillator baths and comparing the outcomes against the hierarchical equations of motion (HEOM) method. Overall, our method accurately quantifies the contributions of specific bath components to the overall dissipation while significantly reducing the computational cost compared to numerically exact methods such as HEOM, thus offering a path to examine how vibronic interactions steer non-adiabatic processes in realistic chemical systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Singularities in nearly uniform one-dimensional condensates due to quantum diffusion

Dissipative systems often exhibit wavelength-dependent loss rates. One prominent example is Rydberg polaritons formed by electromagnetically induced transparency, which have long been a leading candidate for studying the physics of interacting photons and also hold promise as a platform for quantum information. In this system, dissipation is in the form of quantum diffusion, i.e., proportional to k 2 (k being the wavevector) and vanishing at long wavelengths as k→0. Here, we show that one-dimensional condensates subject to this type of loss are unstable to long-wavelength density fluctuations in an unusual manner: after a prolonged period in which the condensate appears to relax to a uniform state, local depleted regions quickly form and spread ballistically throughout the system. We connect this behavior to the leading-order equation for the nearly uniform condensate—a dispersive analog to the Kardar-Parisi-Zhang equation—which develops singularities in finite time. Furthermore, we show that the wavefronts of the depleted regions are described by purely dissipative solitons within a pair of hydrodynamic equations, with no counterpart in lossless condensates. We close by discussing conditions under which such singularities and the resulting solitons can be physically realized.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Fluctuation–dissipation relation for a quantum Brownian oscillator in a parametrically squeezed thermal field

In this paper we study the nonequilibrium evolution of a quantum Brownian oscillator, modeling the internal degree of freedom of a harmonic atom or an Unruh–DeWitt detector, coupled to a nonequilibrium and nonstationary quantum field bath and inquire whether a fluctuation–dissipation relation (FDR) can exist after/if it approaches equilibration. This is a nontrivial issue because a squeezed field bath cannot reach equilibration and yet, as this work shows, the system oscillator indeed can, which is a necessary condition for FDRs. We discuss three different settings: (A) The bath field essentially remains in a squeezed thermal state throughout, whose squeeze parameter is a mode- and time-independent constant. This situation is often encountered in quantum optics and quantum thermodynamics. (B) The bath field is initially in a thermal state, but is subjected to a parametric process leading to mode- and time-dependent squeezing. This scenario is encountered in cosmology and dynamical Casimir effects. The squeezing in the bath in both types of processes will affect the oscillator’s nonequilibrium evolution. We show that at late times it approaches equilibration and this stationarity condition warrants the existence of a FDR. The trait of squeezing is marked by the oscillator’s effective equilibrium temperature, and the proportionality factor in the FDR is only related to the stationary component of the noise kernel of the bath field. Setting (C) is more subtle: A finite system–bath coupling strength can set the oscillator in a squeezed state even though the bath field is stationary and does not engage in any parametric process. The squeezing of the system in this case is in general time-dependent but becomes constant when the internal dynamics is fully relaxed. We begin with comments on the broad range of physical processes involving squeezed thermal baths and end with some remarks on the significance of FDRs in capturing the essence of quantum backreaction in nonequilibrium and stochastic systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗