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Results for “Quantum transition rate”

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 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
NASA NTRS1981

Long wavelength carbonyl sulfide photodissociation

The aeronomic implications of a preliminary observation of weak OCS photoabsorption above 270 nm are investigated. It is argued that the measured cross section is consistent with a forbidden transition in this wavelength region. Model calculations are made for the OCS photodissociation rates in daylight, the OCS and SO2 distributions in the upper atmosphere, and the budgets of sulfur in the stratosphere and OCS in the troposphere, assuming various extrapolations of the measured OCS absorption cross sections and quantum yields to longer wavelengths. It is shown that weak OCS absorption above 300 nm can have important consequences for all of these quantities. Laboratory and field experiments are identified which might lead to a better understanding of the atmospheric OCS cycle.

Turco, R. P.↗
DOE OSTI2025

Dependence of Exciton Spin Dynamics on Quantum Confinement Dimensionality in CsPbBr 3 Nanocrystals

Semiconductor nanomaterials offer a promising platform to produce optically addressable spins for use in quantum technologies. Here, in this study, we examine CsPbBr 3 nanospheres, cubes, and rods spanning the zero-dimensional (0D) to three-dimensional (3D) transition to investigate the influence of dimensionality and shape on exciton spin decoherence. Using circularly polarized transient absorption spectroscopy, we find that the spin relaxation rate is independent of the surface to volume ratio and instead follows a dependence on the length of the shortest dimension. Additionally, differences in surface quality and termination appear to have no effect on the spin relaxation rate for measured materials, and instead the spin relaxation rate is most clearly correlated with the exciton binding energy. Finally, decreasing the dimensionality of the nanomaterials decreases the influence of multiexciton interactions on the spin relaxation rate.

CsPbBr3 nanocrystals↗
DOE OSTI2025

Quantifying Trapped Magnetic Vortex Losses in Niobium Resonators at mK Temperatures

Trapped magnetic vortices in niobium introduce microwave losses that degrade the performance of superconducting resonators. While such losses have been extensively studied above 1 K, we report here their direct quantification in the millikelvin and low-photon regime relevant to quantum devices. Using a high-quality factor 3D niobium cavity cooled through its superconducting transition in controlled magnetic fields, we isolate vortex-induced losses and find the resistive component of the sensitivity to trapped flux S to be approximately 2 nOhm/mG at 10 mK and 6 GHz. The decay rate is initially dominated by two-level system (TLS) losses from the native niobium pentoxide, with vortex-induced degradation of T1 occurring above Btrap~50 mG. In the absence of the oxide, even 10 mG of trapped flux limits performance, Q0 ~ 1010, or T1 ~350 ms, underscoring the need for stringent magnetic shielding. The resistive sensitivity, S, decreases with temperature and remains largely field-independent, whereas the reactive component, S , exhibits a maximum near 0.8 K. These behaviors are well modeled within the Coffey Clem framework in the zero-creep limit, under the assumption that vortex pinning is enhanced by thermally activated processes. Our results suggest that niobium-based transmon qubits can tolerate vortex-induced dissipation at trapped field levels up to several hundred mG, but achieving long coherence times still requires careful magnetic shielding to suppress lower-field losses from other mechanisms

Bafia, Daniel P. [Fermilab]↗
DOE OSTI2020

Mixed quantum–classical approach to model non-adiabatic electron–nuclear dynamics: Detailed balance and improved surface hopping method

We develop a density matrix formalism to describe coupled electron–nuclear dynamics. To this end, we introduce an effective Hamiltonian formalism that describes electronic transitions and small (quantum) nuclear fluctuations along a classical trajectory of the nuclei. Using this Hamiltonian, we derive equations of motion for the electronic occupation numbers and for the nuclear coordinates and momenta. We show that, in the limit, when the number of nuclear degrees of freedom coupled to a given electronic transition is sufficiently high (i.e., the strong decoherence limit), the equations of motion for the electronic occupation numbers become Markovian. Furthermore, the transition rates in these (rate) equations are asymmetric with respect to the lower-to-higher energy transitions and vice versa. In thermal equilibrium, such asymmetry corresponds to the detailed balance condition. We also study the equations for the electronic occupations in the non-Markovian regime and develop a surface hopping algorithm based on our formalism. To treat the decoherence effects, we introduce additional “virtual” nuclear wave packets whose interference with the “real” (physical) wave packets leads to the reduction in coupling between the electronic states (i.e., decoherence) as well as to the phase shifts that improve the accuracy of the numerical approach. Remarkably, the same phase shifts lead to the detailed balance condition in the strong decoherence limit.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

Modeling of Radiative Emission from Shallow Color Centers in Single Crystalline Diamond

Optically active defects in diamond are widely used as bright single-photon sources for quantum sensing, computing, and communication. For many applications, it is useful to place the emitter close to the diamond surface, where the radiative properties of the emitter are strongly modified by its dielectric environment. It is well-known that the radiative power from an electric dipole decreases as the emitter approaches an interface with a lower-index dielectric, leading to an increase in the radiative lifetime. For emitters in crystalline solids, modeling of this effect needs to take into account the crystal orientation and direction of the surface cut, which can greatly impact the emission characteristics. In this paper, a framework for analyzing the emission rates of shallow (<100 nm) defects is provided, in which optical transitions are derived from electric dipoles in a plane perpendicular to their spin axis. The calculations for the depth-dependent radiative lifetime for color centers in (100)-, (110)-, and (111)-cut diamond are presented, which can be extended to other vacancy defects in diamond.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS2003

Collective Excitations in InAs Well Intersubband Transitions

Intersubband transitions in semiconductor quantum well are studied using a density matrix theory that goes beyond the Hartree-Fock approximation by including the full second order electron-electron scattering terms in the polarization equation for the first time. Even though the spectral features remain qualitatively similar to the results obtained with dephasing rate approximation, significant quantitative changes result from such a more detailed treatment of dephasing. More specifically, we show how the interplay of the two fundamental collective excitations, the Fermi-edge singularity and the intersubband plasmon, leads to significant changes in lineshape as the electron density varies.

Li, Jian-Zhong↗
DOE OSTI2020

Varying Quantum Degeneracy in Plasmas Created at the National Ignition Facility [Slides]

Physically realized electron gas systems usually reside in either the quantum non-degenerate or fully degenerate limit, where the average de Broglie wavelength of the thermal electrons becomes comparable with the interparticle distance between electrons. A few systems, such as young brown dwarfs and the cold dense fuels created in imploded cryogenic capsules at the National Ignition Facility, lie between these two limits and are partially degenerate. The National Ignition Facility has the unique capability of varying the electron quantum degeneracy by adjusting the laser drive used to implode the capsules. This allows experimental studies of the effects of the degeneracy level on plasma transport properties. By measuring rare nuclear reactions in these cold dense fuels, we show that the electron stopping power, which is the rate of energy loss per unit distance travelled by a charged particle, changes with increasing electron density. We observe a quantum-induced shift in the peak of the stopping power using diagnostics that measure above and below this peak. The observed changes in the stopping power are shown to be unique to the transition region between non-degenerate and degenerate plasmas. Our results support the screening models applied to partially degenerate astrophysical systems such as young brown dwarfs.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
NASA NTRS1996

Technology Directions for the 21st Century, volume 1

For several decades, semiconductor device density and performance have been doubling about every 18 months (Moore's Law). With present photolithography techniques, this rate can continue for only about another 10 years. Continued improvement will need to rely on newer technologies. Transition from the current micron range for transistor size to the nanometer range will permit Moore's Law to operate well beyond 10 years. The technologies that will enable this extension include: single-electron transistors; quantum well devices; spin transistors; and nanotechnology and molecular engineering. Continuation of Moore's Law will rely on huge capital investments for manufacture as well as on new technologies. Much will depend on the fortunes of Intel, the premier chip manufacturer, which, in turn, depend on the development of mass-market applications and volume sales for chips of higher and higher density. The technology drivers are seen by different forecasters to include video/multimedia applications, digital signal processing, and business automation. Moore's Law will affect NASA in the areas of communications and space technology by reducing size and power requirements for data processing and data fusion functions to be performed onboard spacecraft. In addition, NASA will have the opportunity to be a pioneering contributor to nanotechnology research without incurring huge expenses.

Crimi, Giles F.↗
DOE OSTI2025

A Theory of Ultrafast Charge Transfer Relaxation with Non-Innocent Solvent Molecules

In this work we revisit the photodynamics of tetracyanoethylene-hexamethylbenzene (TCNE- HMB), the molecular complex studied by Hochstrasser et al. [J. Chem. Phys. 100, 4797–4810, 1994] that has long challenged the applicability of Marcus’s theory of elec- tron transfer for predicting photochemical reactions. Using a novel black-box electronic structure algorithm (time-dependent density functional theory with one double, TD- DFT-1D) to efficiently run molecular dynamics that can treat charge recombination, we run ab initio surface hopping molecular dynamics and confirm that, for a polar solvent, charge recombination rates can be incredibly fast (indeed faster than the sol- vent relaxation time); for non-polar solvents, the rate is much slower. We demonstrate that, although Marcus theory cannot be directly applied, these nonequilibrium (and sometimes incredibly fast) photoexcited dynamics can be effectively explained within a two-state model without any evidence of a transition through a conical intersection. Most importantly, for this paradigmatic model system, we are able to identify two nuclear coordinates of interest (rather than the single coordinate predicted by Marcus or a full set of internal quantum modes studied by Bixon and Jortner): the solvent relaxation in the first shell (that strongly modulates the energies of the charge trans- fer state and differentiates time scales for relaxation) and a nuclear displacement in the TCNE-HMB complex arising from a handful of vibrations that induces non-Born Oppenheimer motion and eventually facilitates an abrupt electronic transition to the ground state. Altogether, these findings suggest a tractable generalization of Marcus theory for future simulations of photochemistry with non-innocent solvent environ- ments in the spirit of a Hamiltonian suggested by Stuchebrukhov (J. Chem. Phys. 107, 3821, 1997).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Modeling Oxidative Dehydrogenation of Propane with Supported Vanadia Catalysts Using Multireference Methods

The oxidative dehydrogenation of propane over supported vanadium oxide catalysts poses significant computational challenges due to complex electronic structure changes along the reaction coordinate, driven primarily by changes in the oxidation states of vanadium. To address these challenges, we systematically test quantum chemical methods, including multireference (MR) approaches, domain-based local pair natural orbital coupled cluster theory (DLPNO-CCSD(T)), and density functional theory (DFT). The initial C–H bond-breaking transition state requires MR treatment due to its multireference character, while subsequent steps permit efficient single-reference calculations. For the rate-limiting C–H activation step mediated by the vanadyl moiety, complete 1 active space second-order perturbation theory (CASPT2) yields an apparent activation barrier (E app 600K ) of 138 kJ/mol, consistent with experimental values (134 ± 4 kJ/mol; Gruene et al. Catal. Today 2010, 157, 137). In contrast, DLPNO-CCSD(T) overestimates this barrier (198 kJ/mol), whereas DFT predictions span 125–150 kJ/mol, depending on the functional. Our multireference investigation of this transition metal oxide-catalyzed process demonstrates that an active space that incorporates the C–H σ and V=O σ/π bonding orbitals, oxygen lone pairs, and their antibonding counterparts adequately captures electronic structure changes along the chemical transformation. Furthermore, these findings provide a general strategy for active space selection in transition metal oxide-catalyzed C/O–H bond activation reactions. The reference dataset from this work, which includes MR calculations with manually selected active spaces for all intermediates and transition states in the propane ODH reaction network, will serve as a benchmark for automating active space selection in similar systems.

Catalysts↗
DOE OSTI2022

Exponential Escape Rate of Filamentary Incubation in Mott Spiking Neurons

Mott materials such as vanadium oxides, when subject to a strong applied voltage, present an inhomogeneous insulator-to-metal transition with formation of metallic filaments within the insulating bulk. This property is enabling the development of compact and power-efficient neuromorphic devices known as Mott neurons. However, the nature of the transition has not been fully understood yet, as it may be attributed to different effects, including Joule self-heating and hot-carrier injection. Moreover, the experimental determination of the threshold voltage needed to induce the transition has proven to be challenging, as the transition becomes increasingly unpredictable when the threshold is approached. The physical understanding of these issues would not only deepen our understanding of Mott insulators, but would also be an important step toward the realization of neuromorphic devices based on such materials. In this work we use numerical simulations based on the Mott resistor network model to study the nature of the filament incubation and formation process. Here, we show that both electronic and thermal effects, in the form of current density focusing and Joule self-heating, respectively, contribute to the filamentary incubation and growth. Remarkably, we find that the percolation of the metallic filaments near the threshold is intrinsically stochastic, qualitatively similar to the familiar Arrhenius activated behavior and to the stochastic firing of biological neurons. More precisely, we characterize the filament percolation as a Poisson point process, which has the same probability distribution as mathematical models of neuronal firing with an exponential escape rate. Finally, we support the numerical simulation results by performing experiments in VO 2 that are in agreement with the exponential escape rate behavior. Thus, we establish a functionality of Mott insulators that opens a path toward implementing neuromorphic hardware with quantum materials.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Chiral effective field theory calculations of weak transitions in light nuclei

In this work, we report quantum Monte Carlo calculations of weak transitions in A≤10 nuclei, based on the Norfolk two- and three-nucleon chiral interactions, and associated one- and two-body axial currents. Furthermore, we find that the contribution from two-body currents is at the 2–3% level, with the exception of matrix elements entering the rates of 8Li, 8B, and 8He β decay. These matrix elements are suppressed in impulse approximation based on the (leading order) Gamow Teller transition operator alone; two-body currents provide a 20–30% correction, which is, however, insufficient to bring theory in agreement with experimental data. For the other transitions, the agreement with the data is satisfactory, and the results exhibit a negligible to mild model dependence when different combinations of Norfolk interactions are utilized to construct the nuclear wave functions. We report a complete study of two-body weak transition densities which reveals the expected universal behavior of two-body currents at short distances throughout the range of A=3 to A=10 systems considered here.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2026

Theory of quasiparticle generation by microwave drives in superconducting qubits

Microwave drives play a central role in the control of superconducting quantum circuits, enabling qubit gates, readout, and parametric interactions. As the drive frequencies are typically an order of magnitude smaller than (twice) the superconducting gap, it is generally assumed that such drives do not disturb the BCS ground state. However, sufficiently strong drives can activate multiphoton pair-breaking processes that generate quasiparticles (QPs) and result in qubit errors. In this work, we present a theoretical framework for calculating the rates of multiphoton-assisted pair-breaking transitions induced by charge- or flux-coupled microwave drives. Through illustrative examples, we show that photon-assisted QP generation may affect novel high-frequency dispersive readout architectures, as well as Floquet-engineered superconducting circuits operating under strong driving.

circuit quantum electrodynamics↗
DOE OSTI2020

Experimental and theoretical studies of the doubly substituted methyl-ethyl Criegee intermediate: Infrared action spectroscopy and unimolecular decay to OH radical products

In this work the infrared (IR) action spectrum of the doubly substituted methyl-ethyl Criegee intermediate (MECI) is observed in the CH stretch overtone region with detection of OH products. The MECI exhibits four conformers, all of which undergo unimolecular decay via a 1,4 H-atom transfer mechanism, followed by the rapid release of OH products. Conformers with different orientations of the carbonyl oxide group with respect to the methyl and ethyl substituents (i.e., anti and syn ) decay via distinct transition state barriers (16.1 kcal mol –1 and 15.4 kcal mol –1 , respectively). The observed IR action spectrum is in good agreement with the predicted anharmonic IR absorption spectrum, but exhibits significant congestion, which is attributed to couplings between spectroscopic bright states and nearby dark states. Energy-dependent OH appearance rates are measured upon IR excitation of the strongest features in the IR action spectrum and are found to be on the order of 10 6 –10 7 s –1 . The experimental rates are in good agreement with computed Rice–Ramsperger–Kassel–Marcus rates for the unimolecular decay of MECI at these energies, which incorporate quantum mechanical tunneling and sophisticated hindered rotor treatments, as well as high-level theoretical calculations of the TS barrier heights, rovibrational properties, and torsional barriers associated with the MECI conformers. Master equation modeling is used to predict thermal rates for the unimolecular decay of anti - and syn -MECI of 473 s –1 and 660 s –1 , respectively. Comparison with other previously studied Criegee intermediate systems provides insights into substituent effects on unimolecular decay under both energy-dependent and thermal conditions.

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

Nonlinear dynamics and quantum chaos of a family of kicked p -spin models

Herein we introduce kicked p-spin models describing a family of transverse Ising-like models for an ensemble of spin-1/2 particles with all-to-all p-body interaction terms occurring periodically in time as delta-kicks. This is the natural generalization of the well-studied quantum kicked top (p = 2) [Haake, Kus', and Scharf, Z. Phys. B 65, 381 (1987)]. We fully characterize the classical nonlinear dynamics of these models, including the transition to global Hamiltonian chaos. The classical analysis allows us to build a classification for this family of models, distinguishing between p = 2 and p > 2, and between models with odd and even p's. Quantum chaos in these models is characterized in both kinematic and dynamic signatures. For the latter, we show numerically that the growth rate of the out-of-time-order correlator is dictated by the classical Lyapunov exponent. Finally, we argue that the classification of these models constructed in the classical system applies to the quantum system as well.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS1995

Theoretical study of hole initiated impact ionization in bulk silicon and GaAs using a wave-vector-dependent numerical transition rate formulation within an ensemble Monte Carlo calculation

In this paper, calculations of the hole initiated interband impact ionization rate in bulk silicon and GaAs are presented based on an ensemble Monte Carlo simulation with the inclusion of a wave-vector-dependent numerical transition rate formulation. The ionization transition rate is determined for each of the three valence bands, heavy, light, and split-off, using Fermi's golden rule with a two-body, screened Coulomb interaction. The dielectric function used within the calculation is assumed to be wave-vector-dependent. Calculations of the field-dependent impact ionization rate as well as the quantum yield are presented. It is found from both the quantum yield results and examination of the hole distribution function that the effective threshold energy for hole initiated impact ionization is relatively soft, similar to that predicted for the corresponding electron initiated ionization events occur more frequently than either heavy or split-offf initiated ionization events in bulk silicon over the applied electric field strengths examined here, 250-500 kV/cm. Conversely,in GaAs, the vast majority of hole initated ionization events originate from holes within the split-off band.

Oguzman, Ismail H.↗
DOE OSTI2025

Stabilizing Non-Abelian Topological Order Against Heralded Noise via Local Lindbladian Dynamics

An important open question for the current generation of highly controllable quantum devices is understanding which phases can be realized as stable steady states under local quantum dynamics. In this work, we show how robust steady-state phases with both Abelian and non-Abelian mixed-state topological order can be stabilized, in two spatial dimensions, against generic “heralded” noise using active dynamics that incorporate measurement and feedback, modeled as a fully local Lindblad master equation. These topologically ordered steady states are two-way connected to pure topologically ordered ground states using local quantum channels, and preserve quantum information for a time that is exponentially large in the system size. Specifically, we present explicit constructions of families of local Lindbladians for both Abelian (ℤ 2 ) and non-Abelian (𝐷 4 ) topological order whose steady states host mixed-state topological order when the noise is below a threshold strength. As the noise strength is increased, these models exhibit first-order transitions to intermediate mixed-state phases where they encode robust classical memories, followed by (first-order) transitions to a trivial steady state at high noise rates. When the noise is imperfectly heralded, steady-state order disappears but our active dynamics significantly enhances the lifetime of the encoded logical information. To carry out the numerical simulations for the non-Abelian 𝐷 4 case, we introduce a generalized stabilizer tableau formalism that permits efficient simulation of the non-Abelian Lindbladian dynamics.

Monte Carlo methods↗
DOE OSTI2022

Topological order and entanglement dynamics in the measurement-only XZZX quantum code

We examine the dynamics of a ( 1 + 1 ) -dimensional measurement-only circuit defined by the stabilizers of the [[5,1,3]] quantum error correcting code interrupted by single-qubit Pauli measurements. The code corrects arbitrary single-qubit errors and it stabilizes an area law entangled state with a D 2 = Z 2 × Z 2 symmetry protected topological (SPT) order, as well as a symmetry breaking (SB) order from a twofold bulk degeneracy. The Pauli measurements break the topological order and induce a phase transition into a trivial area law phase. Allowing more than one type of Pauli measurement increases the measurement-induced frustration and the SPT and SB order can be broken either simultaneously or separately at nonzero measurement rate. This yields a rich phase diagram and unanticipated critical behavior at the phase transitions. Although the correlation length exponent ν = 4 3 and the dynamical critical exponent z = 1 are consistent with bond percolation, the prefactor of the logarithmic entanglement growth may take noninteger multiples of the percolation value. Remarkably, we identify a robust transient scaling regime for the purification dynamics of L qubits. It reveals a modified dynamical critical exponent z * ≠ z , which is observable up to times t ~ L z * and is reminiscent of the relaxation of critical systems into a prethermal state.

36 MATERIALS SCIENCE↗