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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 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Attosecond XUV probing of vibronic quantum superpositions in Br 2 +

Ultrafast laser excitation can create coherent superpositions of electronic states in molecules and trigger ultrafast flow of electron density on a few femtosecond timescale. While recent attosecond experiments have addressed real-time observation of these primary photochemical processes, the underlying roles of simultaneous nuclear motions and how they modify and disturb the valence electronic motion remain uncertain. In this work, we investigate coherent electronic-vibrational dynamics induced among multiple vibronic levels of ionic bromine (Br 2 + ), including both spin-orbit (X 2 Π 3/2,g – X 2 Π 1/2,g ) and valence (A 2 Π 3/2,u – 4 Σ 3/2,u ) electronic superpositions, using attosecond transient absorption spectroscopy. Decay, revival, and apparent frequency shifts of electronic coherences are measured via characteristic quantum beats on the Br-3d core-level absorption signals. Quantum-mechanical simulations attribute the observed electronic decoherence to broadened phase distributions of nuclear wave packets on anharmonic potentials. Molecular vibronic structure is further revealed to be imprinted as discrete progressions in electronic beat frequencies. These results provide a future basis to interpret complex charge-migration dynamics in polyatomic systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Robust Millisecond Coherence Times of Erbium Electron Spins

Erbium doped solids are prime candidates for quantum memories in optical quantum networks given their telecom-compatible photon emission. An electron spin of erbium with millisecond coherence time is desirable for generating remote entanglement between adjacent quantum network nodes. Here, in this study, we report GHz-range electron spin transitions of 167 Er 3+ in yttrium oxide (Y 2 O 3 ) matrix with coherence times that are consistently longer than a millisecond. By polarizing para magnetic impurity spins we achieve a spin T 2 up to 1.46 ms, and up to 7.1 ms after dynamical decoupling. These coherence lifetimes are among the longest found for erbium in crystalline matrices despite the presence of host nuclear spins. We further enhance the coherence time beyond conventional dynamical decoupling, using customized sequences to simultaneously mitigate spectral diffusion and dipolar interactions. Our study not only establishes 167 Er 3+ : Y 2 O 3 as a significant quantum memory platform but also provides a guideline for engineering long-lived erbium spins in a variety of host materials for quantum technologies.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Coherent high-power RF wakefield generation by electron bunch trains in a metamaterial structure

In this paper, we present an experimental study of coherent high-power wakefield generation in a metamaterial (MTM) structure at 11.7 GHz by 65 MeV electron bunch trains at the Argonne Wakefield Accelerator (AWA), following a previous experiment, the Stage-I experiment, at the AWA. Both the Stage-II experiment, reported in this paper, and the Stage-I experiment were conducted using MTM structures, which are all-metal periodic structures with the period being much smaller than the wavelength. Differences between the two experiments include (1) structure length (Stage-I 8 cm and Stage-II 20 cm); (2) number of bunches used to excite the structure (Stage-I with two bunches, up to 85 nC of total charge; Stage-II with eight bunches, up to 224 nC of total charge); and (3) highest peak power measured (Stage-I 80 MW in a 2 ns pulse and Stage-II 380 MW in a 10 ns pulse). High-power radio frequency pulses were generated by reversed Cherenkov radiation of the electron beam due to the negative group velocity in the MTM structures. Because the radiation is coherent, a train of bunches with a proper spacing can build up to achieve a high peak power. The observed output power levels are very promising for future applications in direct collinear wakefield acceleration or in transfer to a second accelerator for two-beam acceleration.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Revealing Defect-Seeded and Interfacial Generation Mechanisms of Photoinduced Coherent Phonons with 4D Ultrafast Electron Microscopy

Ultrafast photoexcitation of coherent phonons is driven by an impulsive, collective displacement of constituent atoms from their average equilibrium lattice positions [1]. Models describing the generation of coherent acoustic modes typically invoke the creation of an anisotropic strain profile arising from the relatively instantaneous absorption of an ultrafast laser pulse [2]. If the skin depth is shallow relative to the specimen thickness, a steep tensile strain gradient perpendicular to the surface ($\frac{∂ε}{∂z}$) results. Initial relaxation occurs via rapid contraction of the surface layers followed by subsequent coherent oscillations of the lattice and launch of a train of coherent elastic strain waves [i.e., coherent acoustic phonons (CAPs)]. Macroscopically, responses are generally well-described by constitutive relations as gleaned from data gathered using ultrasonic methods or ultrafast spectroscopies. Furthermore, at the atomic to nanoscale level, individual lattice discontinuities and their impact on CAP behaviors can be modeled using multiscale methods [3,4]. Further, average unit-cell level responses on ultrafast timescales can be probed using femtosecond electron and X-ray scattering [5,6].

Flannigan, David J. [University of Minnesota, Minn↗
DOE OSTI2026

Bootstrap embedding for interacting electrons in phonon coherent-state mean field

Here, we develop a Fermi–Bose bootstrap embedding framework for the ground state of interacting electrons coupled to a phonon mean field. The method combines bootstrap embedding for correlated electrons with a self-consistent coherent-state mean-field treatment for phonons. This method models the interacting electron–phonon problem as a system of correlated electrons traveling in a self-consistently specified potential landscape, allowing for efficient treatment of large lattice systems. Convergence of the methods for fragment size and total system size is demonstrated for the one-dimensional Hubbard–Holstein model for up to 350 sites. Finite-size scaling is performed to extrapolate to the infinite system size. Benchmarking against the density matrix renormalization group for a small 8-site system at half- and quarter-filling shows an orders-of-magnitude runtime advantage. The comparison further reveals that the method performs best in regimes dominated by localization, such as the Mott insulating phase and the strong-coupling tiny polaron regime, where the local embedding ansatz is still valid. However, due to the mean-field treatment for phonons, we find limitations of our methods in the weakly coupled delocalized region and at the Peierls transition, where quantum phonon fluctuations and long-range kinetic correlations become substantial.

Islam, Shariful [North Carolina State University, ↗
DOE OSTI2023

Incoherent nonadiabatic to coherent adiabatic transition of electron transfer in colloidal quantum dot molecules

Electron transfer is a fundamental process in chemistry, biology, and physics. One of the most intriguing questions concerns the realization of the transitions between nonadiabatic and adiabatic regimes of electron transfer. Using colloidal quantum dot molecules, we computationally demonstrate how the hybridization energy (electronic coupling) can be tuned by changing the neck dimensions and/or the quantum dot sizes. This provides a handle to tune the electron transfer from the incoherent nonadiabatic regime to the coherent adiabatic regime in a single system. We develop an atomistic model to account for several states and couplings to the lattice vibrations and utilize the mean-field mixed quantum-classical method to describe the charge transfer dynamics. Here, we show that charge transfer rates increase by several orders of magnitude as the system is driven to the coherent, adiabatic limit, even at elevated temperatures, and delineate the inter-dot and torsional acoustic modes that couple most strongly to the charge transfer dynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1994

Coherent-phase or random-phase acceleration of electron beams in solar flares

Time structures of electron beam signatures at radio wavelengths are investigated to probe correlated versus random behavior in solar flares. In particular we address the issue whether acceleration and injection of electron beams is coherently modulated by a single source, or whether the injection is driven by a stochastic (possibly spatially fragmented) process. We analyze a total of approximately = 6000 type III bursts observed by Ikarus (Zurich) in the frequency range of 100-500 MHz, during 359 solar flares with simultaneous greater than or = 25 keV hard X-ray emission, in the years 1890-1983. In 155 flares we find a total of 260 continuous type III groups, with an average number of 13 +/- 9 bursts per group, a mean duration of D = 12 +/- 14 s, a mean period of P = 2.0 +/- 1.2 s, with the highest burst rate at a frequency of nu = 310 +/- 120 MHz. Pulse periods have been measured between 0.5 and 10 s, and can be described by an exponential distribution, i.e., N(P) varies as e (exp -P/1.0s). The period shows a frequency dependence of P(nu)=46(exp-0.6)(sub MHz)s for different flares, but is invariant during a particular flare. We measure the mean period P and its standard deviation sigma (sub p) in each type III group, and quantify the degree of periodicity (or phase-coherence) by the dimensionless parameter sigma (sub p)P. The representative sample of 260 type III burst groups shows a mean periodicity of sigma (sub p/P) = 0.37 +/- 0.12, while Monte Carlo simulations of an equivalent set of truly random time series show a distinctly different value of sigma (sub p)P = 0.93 +/- 0.26. This result indicates that the injection of electron beams is coherently modulated by a particle acceleration source which is either compact or has a global organization on a timescale of seconds, in contrast to an incoherent acceleration source, which is stochastic either in time or space. We discuss the constraints on the size of the acceleration region resulting from electron beam propagation delays and from Alfvenic synchronization during a pulse period. We discuss two periodic preocesses in flares, which potentially control quasi-periodic particle acceleration: (1) MHD oscillations, and (2) current sheets with oscillatory dynamics.

Aschwanden, Markus J.↗
DOE OSTI2022

Connection between coherent phonons and electron-phonon coupling in Sb (111)

We report time- and angle-resolved photoemission spectroscopy (trARPES) measurements on the Sb(111) surface. We observe band- and momentum-dependent binding-energy oscillations in the bulk and surface bands driven by $A_{1g}$ and $E_{g}$ coherent phonons. While the bulk band shows simultaneous $A_{1g}$ and $E_{g}$ oscillations, the surface bands show either $A_{1g}$ or $E_{g}$ oscillations. The observed behavior is reproduced by frozen-phonon calculations based on density-functional theory. Furthermore, this evidences the connection between electron-phonon coupling and coherent binding energy dynamics tied to lattice vibration and confirms that band-, momentum-, and mode-dependent electron-phonon coupling can indeed be probed by trARPES in the low fluence limit.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Establishing coherent momentum-space electronic states in locally ordered materials

Rich momentum-dependent electronic structure naturally arises in solids with long-range crystalline symmetry. Reliable and scalable quantum technologies rely on materials that are either not perfect crystals or non-crystalline, breaking translational symmetry. This poses the fundamental questions of whether coherent momentum-dependent electronic states can arise without long-range order, and how they can be characterized. Here we investigate Bi 2 Se 3 , which exists in crystalline, nanocrystalline, and amorphous forms, allowing direct comparisons between varying degrees of spatial ordering. Through angle-resolved photoemission spectroscopy, we show for the first time momentum-dependent band structure with Fermi surface repetitions in an amorphous solid. The experimental data is complemented by a model that accurately reproduces the vertical, dispersive features as well as the replication at higher momenta in the amorphous form. These results reveal that well-defined real-space length scales are sufficient to produce dispersive band structures, and that photoemission can expose the imprint of these length scales on the electronic structure.

36 MATERIALS SCIENCE↗
NASA NTRS1987

Resonance between coherent whistler mode waves and electrons in the topside ionosphere

Landau resonance and cyclotron resonance of coherent whistler mode waves and energetic electrons are explored for magnetoplasmas with appreciable gradients in the plasma density and magnetic field strength. It is shown that in the topside ionosphere of the earth near the ion transition height the gradients in plasma density and magnetic field strength along a magnetic field line may match in a way which enhances both Landau and cyclotron interactions between waves and electrons at the loss cone pitch angle. The pitch angle scattering induced by a signal from a ground-based VLF transmitter in the ionosphere above the transmitter has been estimated and compared to the pitch angle scattering induced by naturally occurring ELF hiss through cyclotron resonance. It is found that the expected scattering due to plasmapheric hiss is an order of magnitude larger than that due to Landau resonance in the topside ionosphere. Pitch angle scattering due to cyclotron resonance in the topside ionosphere, however, may be larger by a factor of 2. It is suggested that the 'fast Trimpi' effect may be caused by a cyclotron resonance interaction in the topside ionosphere.

Neubert, T.↗
DOE OSTI2025

Electron beam characterization via quantum coherent electric field imaging

We demonstrate an all-optical, minimally invasive electron beam (𝑒−beam) characterization using Rydberg electrometry. An 𝑒-beam passes through a localized detector volume containing thermal Rb atoms that are optically excited in a quantum superposition of ground and Rydberg states. The 𝑒-beam's electric field perturbs atomic coherence and modifies resonance fluorescence in a narrow spectral region near the two-photon optical transition. Imaging Rb fluorescence provides a map of the electric field from the 𝑒-beam via Rydberg state Stark shifts and allows us to reconstruct the 𝑒-beam width, centroid position, and current. For an 𝑒-beam of 20 keV and electron currents of 20–40 µ⁢A, we measured the centroid position with an accuracy of ≤ 8 µ⁢m and width to within 100 µ⁢m, limited by the experimental sensitivity of electric field reconstruction of ∼0.02 V/cm. This method is suitable for a wide range of electron energies and currents, and can be adopted for nuclear and high-energy experiments for minimally invasive real-time diagnostics and profiling of charged particle beams.

Behary, Rob [College of William and Mary, Williams↗
DOE OSTI2020

Coherent Manipulation of Single Electrons with Optical Photons in Condensed Helium-4

Single electrons are one of the simplest quantum objects in nature. In free space or conventional materials, single electrons hardly interact with optical (ultraviolet-visible-infrared) photons, so their quantum states cannot be easily manipulated by optics. Here, a notable exception is is theoretically demonstrated: A single electron in condensed helium-4 can be self-confined in a nanometric bubble of 1 to 2 nm radius and resonantly interact with mid-infrared photons of 3 to 12 μm wavelength. A femtosecond laser can drive the electron into Rabi oscillations and prepare it onto arbitrary superposition states between the ground and excited states. After the laser pulse, the electron bubble can exhibit remarkable nonequilibrium quantum dynamics and evolve toward various final states with various lifetimes. These processes are accompanied with intense phonon radiation.

36 MATERIALS SCIENCE↗