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Results for “collective electron dynamics”

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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2014

Electron Dynamics in Nanostructures in Strong Laser Fields

The goal of our research was to gain deeper insight into the collective electron dynamics in nanosystems in strong, ultrashort laser fields. The laser field strengths will be strong enough to extract and accelerate electrons from the nanoparticles and to transiently modify the materials electronic properties. We aimed to observe, with sub-cycle resolution reaching the attosecond time domain, how collective electronic excitations in nanoparticles are formed, how the strong field influences the optical and electrical properties of the nanomaterial, and how the excitations in the presence of strong fields decay.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Measurement of the dynamic charge susceptibility near the charge density wave transition in ErTe 3

A charge density wave (CDW) is a phase of matter characterized by a periodic modulation of valence electron density coupled with lattice distortion. Its formation is closely tied to the dynamical charge susceptibility, χ(q, ω) , which reflects the collective electron dynamics of the material. Despite decades of study, χ(q, ω) near a CDW transition has never been measured at nonzero momentum, q, with meV energy resolution. Here, we investigate the canonical CDW transition in ErTe 3 using momentum-resolved electron energy loss spectroscopy, a technique uniquely sensitive to valence band charge excitations. Unlike phonons, which soften via the Kohn anomaly, we find the electronic excitations exhibit purely relaxational dynamics well described by a diffusive model, with the diffusivity peaking just below the critical temperature, T C1 . Additionally, we report for the first time a divergence in the real part of χ(q, ω) in the static limit (ω → 0), a long-predicted hallmark of CDWs. Unexpectedly, this divergence occurs as T → 0, with only a weak thermodynamic signature at T = T C1 . Our study necessitates a reexamination of the traditional description of CDW formation in quantum materials.

M-EELS↗
DOE OSTI2012

Enhanced collective focusing of intense neutralized ion beam pulses in the presence of weak solenoidal magnetic fields

In this study, the design of ion drivers for warm dense matter and high energy density physics applications and heavy ion fusion involves transverse focusing and longitudinal compression of intense ion beams to a small spot size on the target. To facilitate the process, the compression occurs in a long drift section filled with a dense background plasma, which neutralizes the intense beam self-fields. Typically, the ion bunch charge is better neutralized than its current, and as a result a net self-pinching (magnetic) force is produced. The self-pinching effect is of particular practical importance, and is used in various ion driver designs in order to control the transverse beam envelope. In the present work we demonstrate that this radial self-focusing force can be significantly enhanced if a weak (B~100 G) solenoidal magnetic field is applied inside the neutralized drift section, thus allowing for substantially improved transport. It is shown that in contrast to magnetic self-pinching, the enhanced collective self-focusing has a radial electric field component and occurs as a result of the overcompensation of the beam charge by plasmaelectrons, whereas the beam current becomes well-neutralized. As the beam leaves the neutralizing drift section, additional transverse focusing can be applied. For instance, in the neutralized drift compression experiments (NDCX) a strong (several Tesla) final focus solenoid is used for this purpose. In the present analysis we propose that the tight final focus in the NDCX experiments may possibly be achieved by using a much weaker (few hundred Gauss) magnetic lens, provided the ion beam carries an equal amount of co-moving neutralizing electrons from the preceding drift section into the lens. In this case the enhanced focusing is provided by the collective electrondynamics strongly affected by a weak applied magnetic field.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2014

Radiative damping and synchronization in a graphene-based terahertz emitter

We investigate the collective electron dynamics in a recently proposed graphene-based terahertz emitter under the influence of the radiative damping effect, which is included self-consistently in a molecular dynamics approach. We show that under appropriate conditions synchronization of the dynamics of single electrons takes place, leading to a rise of the oscillating component of the charge current. The synchronization time depends dramatically on the applied dc electric field and electron scattering rate and is roughly inversely proportional to the radiative damping rate that is determined by the carrier concentration and the geometrical parameters of the device. The emission spectra in the synchronized state, determined by the oscillating current component, are analyzed. The effective generation of higher harmonics for large values of the radiative damping strength is demonstrated.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2016

Retrieving plasmonic near-field information: A quantum-mechanical model for streaking photoelectron spectroscopy of gold nanospheres

Streaked photoemission from nanostructures is characterized by size- and material-dependent nanometer-scale variations of the induced nanoplasmonic response to the electronic field of the streaking pulse and thus holds promise of allowing photoelectron imaging with both subfemtosecond temporal and nanometer spatial resolution. In order to scrutinize the driven collective electronic dynamics in 10–200-nm-diameter gold nanospheres, we calculated the plasmonic field induced by streaking pulses in the infrared and visible spectral range and developed a quantum-mechanical model for streaked photoemission by extreme ultraviolet pulses. Overall, our simulated photoelectron spectra reveal a significant amplitude enhancement and phase shift of the photoelectron streaking trace relative to calculations that exclude the induced plasmonic field. Both are most pronounced for streaking pulses tuned to the plasmon frequency and retrace the plasmonic electromagnetic field enhancement and phase shift near the nanosphere surface.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Correlation-driven attosecond photoemission delay in the plasmonic excitation of C60 fullerene

Extreme light confinement in plasmonic nanosystems enables novel applications in photonics, sensor technology, energy harvesting, biology, and quantum information processing. Fullerenes represent an extreme case for nanoplasmonics: they are sub-nanometer carbon- based molecules showing high-energy and ultrabroad plasmon resonances, however the fundamental mechanisms driving the plasmonic response and the corresponding collective electron dynamics are still elusive. Here, we uncover the dominant role of electron correlations in the dynamics of the giant plasmon resonance (GPR) of the sub-nanometer system C60 by employing attosecond photoemission chronoscopy. We find a characteristic photoemission delay of up to about 300 attoseconds that is purely induced by coherent large-scale electron correlations in the plasmonic potential. These results provide novel insights into the nature of the plasmon resonances in sub-nanometer systems and open new perspectives for advancing nanoplasmonic applications.

Biswas, Shubhadeep [SLAC National Accelerator Labo↗
DOE OSTI2015

Theoretical investigation of polarization effects in solution: Importance of solvent collective motions

Recent theoretical studies on interesting topics related to polarization effects in solutions are presented. As one of interesting topics, ionic liquids (ILs) solvents are focused on. The collective dynamics of electronic polarizability through interionic dynamics and the effect of polarization in ILs, 1-butyl-3-methylimidazolium hexafluorophosphate ([BMIm][PF{sub 6}]), are studied with molecular dynamics simulation. Also, the time-dependent polarization effect on the probe betaine dye molecule, pyridinium N-phenoxide, in water is investigated by a time-dependent reference interaction site model self-consistent field (time-dependent RISM-SCF) approach. The importance of considering polarization effects on solution systems related to solvent collective motions is shown.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2026

Single-shot imaging with randomized structured illumination at a free electron laser

Stroboscopic nanoscale imaging with free electron laser light is revolutionizing our understanding of fast dynamics in heterogeneous systems. The short wavelength of X-ray and extreme ultraviolet radiation makes it possible to achieve nanoscale resolution, while resonance with atomic transitions gives access to electronic and magnetic degrees of freedom. Here, we report on our implementation of a recently developed imaging method, randomized probe imaging, at a free electron laser. The advantage of randomized probe imaging over existing methods is its compatibility with extended and strongly scattering samples. Our implementation delivers robust single-shot reconstructions at up to a full-pitch resolution of 400 nm over a field of view with a 40 µm diameter. We also demonstrate single-shot imaging of magnetic domain structures using circular dichroism at resonance, paving the way to future time-resolved studies of magnetic dynamics, shock physics, and the dynamics of collective electronic phases.

47 OTHER INSTRUMENTATION↗
DOE OSTI2019

Atomic and Molecular Physics in Strong Fields

In this project, we have investigated a broad range of atomic, molecular, and optical (AMO) processes of current significance in strong-field and ultrafast science and technology. The main goals are to develop new theoretical formalisms and accurate computational methods for ab initio and in-depth non-perturbative study of time-resolved multiphoton quantum dynamics and spectroscopy, very-high-order harmonic generation, optimal control of ultrafast attosecond pulse generation, and resonance-enhanced below threshold harmonics in intense ultrashort laser fields. We have worked on the following projects and we have published 20 top 15 % SCI journal articles during the last 3.5 years (Jan. 1, 2016 to June 30, 2019), including one article in top raking Physical Review Letters, and 3 articles in top ranking (Nature) Scientific Reports, and one Physical Review A article was chosen as Editors’ suggestion paper, etc. (a) Development of new time-dependent methods for accurate and efficient solution of multi-dimensional time-dependent Schrödinger equation and time-dependent density functional theory. (b) Non-perturbative treatment of very-high order (1000th – 5000th order) harmonic generation and broadband supercontinuum spectra from XUV to soft x-ray regime. (c) Development of synchrosqueezing transform (SST) for precision time-frequency analysis of electron multi-rescattering dynamics. (d) Exploration of the dynamical origin of resonance-enhanced near- and below-threshold harmonics. (e) Probing the high-order harmonics generation in disordered semiconductor. (f) Multiphoton ionization of one-electron relativistic diatomic quasi-molecules in strong laser fields. and, (g) New development of non-adiabatic density functional theory. The theoretical and simulation projects we have pursued are closely related to the ongoing experimental researches in several leading laboratories in the US and Europe, etc. It is expected that the outcome of this project will provide timely and significant new information and insight for the advancement of strong-field atomic and molecular physics and ultrafast science and technology.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2019

Collective charge and spin dynamics in low-dimensional itinerant electron systems with spin-orbit coupling

This research project in theoretical condensed-matter physics aims to study the collective charge and spin excitations of itinerant quasi-two-dimensional electronic systems such as doped semiconductor nanostructures and carbon-based materials, in the presence of impurities and spin-orbit coupling. In previous work under DOE support, we had discovered an interesting interplay between many-body effects and Rashba and Dresselhaus spin-orbit interactions: contrary to many situation in spintronics where spin-orbit interactions lead to loss of spin coherence, collective spin modes are robust against such coherence losses, and behave as macroscopic quantum objects with a collective magnetic moment precessing about an effective spin-orbit magnetic field. Experimental data for GaAs and CdMnTe quantum wells, obtained by our collaborators at the University Pierre et Marie Curie in Paris, confirmed our predictions and suggested that the observed effect is universal. However, a full theoretical explanation of the effect is still missing, and a wealth of new experimental data remains to be analyzed. We therefore plan to address the following three interrelated objectives: 1. Theory of collective modes in chiral systems. We will explore the various ways in which spin-orbit interactions affect collective spin-density and spin-flip excitations in semiconductor quantum wells. The goal will be to develop a universal formalism for chiral collective modes, with a particular emphasis on analytic results for dispersion relations, which will be compared with experimental results from inelastic light scattering. We will calculate the linewidths of spin plasmons and spin-flip waves due to impurity scattering and spin Coulomb drag from first principles. 2.Many-body effects in noncollinear magnetism. We will describe electronic many-body effects using time-dependent density-functional theory (TDDFT) in the linear-response regime. Quantum wells with spin-orbit coupling are noncollinear itinerant magnetic systems at the crossover between two and three dimensions, which poses subtle challenges for standard exchange-correlation (xc) functionals such as the local-density approximation (LDA). We will develop new orbital-dependent xc functionals for noncollinear magnetic systems by generalizing the so-called STLS approach. 3. Beyond single semiconductor quantum wells. We will consider quantum well bilayer or multilayer systems with spin-orbit coupling, where the coupling between the quasi-2D electron systems leads to acoustic and optical modes (in phase and out of phase). How are these modes affected if the two layers have the same or different chirality? Plasmon modes have been widely studied in graphene and other topological materials, and we will study collective spin excitations in graphene and other carbon-based materials in the presence of spin-orbit coupling and magnetic fields. The potential impact of the proposed research will be both on a fundamental and a practical level. A universal theory of chiral collective modes will advance our understanding of the interplay between many-body effects and spin-orbit interactions in a wide variety of materials and systems. A generalized STLS approach for noncollinear magnetism will be of wide interest beyond the systems studied here. This work may also point towards new ways of manipulating and controlling spin waves in low-dimensional itinerant electron systems: this could be used to encode, transport and process information, which would be of interest to the field of magnon spintronics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Time-resolved K α spectroscopy measurements of hot-electron equilibration dynamics in thin-foil solid targets: Collisional and collective effects

Time-resolved K α spectroscopy measurements from high-intensity laser interactions with thin-foil solid targets are reviewed. Thin Cu foils were irradiated with 1- to 10-J, 1-ps pulses at focused intensities from 10 18 to 10 19 W/cm 2 . The experimental data show K α -emission pulse widths from 3 to 6 ps, increasing with laser intensity. The time-resolved K α -emission data are compared to a hot-electron transport and K α -production model that includes collisional electron-energy coupling, resistive heating, and electromagnetic field effects. The experimental data show good agreement with the model when a reduced ponderomotive scaling is used to describe the initial mean hot-electron energy over the relevant intensity range.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2019

Tomographic Dynamics and Scale-Dependent Viscosity in 2D Electron Systems

Fermi gases in two dimensions display collective dynamics originating from head-on collisions, a collinear carrier scattering process that dominates angular relaxation at not-too-high temperatures T<< TF. In this regime, a large family of excitations emerges, with an odd-parity angular structure of momentum distribution and exceptionally long lifetimes. This leads to “tomographic” dynamics: fast 1D spatial diffusion along the unchanging velocity direction accompanied by a slow angular dynamics that gradually randomizes velocity orientation. Here, the tomographic regime features an unusual hierarchy of timescales and scale-dependent transport coefficients with nontrivial fractional scaling dimensions, leading to fractional-power current flow profiles and unusual conductance scaling versus sample width.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Intersubband plasmons in the quantum limit in gated and aligned carbon nanotubes

Confined electrons collectively oscillate in response to light, resulting in a plasmon resonance whose frequency is determined by the electron density and the size and shape of the confinement structure. Plasmons in metallic particles typically occur in the classical regime where the characteristic quantum level spacing is negligibly small compared to the plasma frequency. In doped semiconductor quantum wells, quantum plasmon excitations can be observed, where the quantization energy exceeds the plasma frequency. Such intersubband plasmons occur in the mid- and far-infrared ranges and exhibit a variety of dynamic manybody effects. Here, we report the observation of intersubband plasmons in carbon nanotubes, where both the quantization and plasma frequencies are larger than those of typical quantum wells by three orders of magnitude. As a result, we observed a pronounced absorption peak in the near-infrared. Specifically, we observed the near-infrared plasmon peak in gated films of aligned single-wall carbon nanotubes only for probe light polarized perpendicular to the nanotube axis and only when carriers are present either in the conduction or valence band. Both the intensity and frequency of the peak were found to increase with the carrier density, consistent with the plasmonic nature of the resonance. With this being said, our observation of gate-controlled quantum plasmons in aligned carbon nanotubes will not only pave the way for the development of carbon-based near-infrared optoelectronic devices but also allow us to study the collective dynamic response of interacting electrons in one dimension.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2018

Development of formalisms based on locally coupled open subsystems for calculations in molecular electronic structure and dynamics

Quantum embedding theories model a collection of interacting molecules as a set of subsystems, where each can be treated with a particular electronic structure method (wave function or density functional theory, for example); these theories can lead to computationally efficient and accurate algorithms. Motivated by challenges in the field, we previously described a formalism (that models two subsystems), which we call “locally coupled open subsystems” (LCOS), for the computation of ground-state energies, fractional electron-occupation numbers of the subsystems, and the size-consistent limit of subsystem dissociation. In this work we present the full (nonrelativistic) LCOS theory and the following extensions of our previous work: (i) the framework to study systems composed of multiple subsystems and a procedure to spin-adapt the auxiliary wave function that describes the partitioned system, so that its spin state matches that of the real system of interest; (ii) potential functionals and ideas to employ machine learning for the computation of ground-state densities and energies; (iii) formulation of two LCOS ground-state approaches where the fragments are assigned Kohn-Sham wave functions; and (iv) a time-dependent (TD) extension of these two ground-state formalisms in which the state of the subsystems evolves according to a unitary propagation; from this evolution we can extract TD electron populations of the fragments, for instance. We also discuss potential applications of the TD LCOS theory to linear photoabsorption and Raman spectroscopy. As a result, the developments presented in this work can lead to ground-state and TD electronic structure calculations where the computational scaling can be controlled, depending on the level of theory and the accuracy desired to model each one of the subsystems and their coupling.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Electronic superradiance mediated by nuclear dynamics

Superradiance, in which the collective behavior of emitters can generate enhanced radiative decay, was first predicted by a model, now known as the Dicke model, that contains a collection of two-level systems (the emitters) all interacting with the same photonic mode. In this article, we extend the original Dicke model to elucidate the influence of nuclear motion on superradiant emission. Our dynamical simulations of the combined electronic, nuclear, and photonic system reveal a new time scale attributed to the population leakage of the dark, subradiant states. Furthermore, this dark-state emission pathway can be controlled by tuning the nuclear potential energy landscape. These findings impact how superradiant states and molecular degrees of freedom can be leveraged and utilized in quantum optical systems. Published by the American Physical Society 2025

Tao, Xuecheng (ORCID:0000000329073839)↗
DOE OSTI2014

Synchronized charge oscillations in correlated electron systems

Strongly correlated phases exhibit collective carrier dynamics that if properly harnessed can enable novel functionalities and applications. In this article, we investigate the phenomenon of electrical oscillations in a prototypical MIT system, vanadium dioxide (VO 2 ). We show that the key to such oscillatory behaviour is the ability to induce and stabilize a non-hysteretic and spontaneously reversible phase transition using a negative feedback mechanism. Further, we investigate the synchronization and coupling dynamics of such VO 2 based relaxation oscillators and show, via experiment and simulation, that this coupled oscillator system exhibits rich non-linear dynamics including charge oscillations that are synchronized in both frequency and phase. Our approach of harnessing a non-hysteretic reversible phase transition region is applicable to other correlated systems exhibiting metal-insulator transitions and can be a potential candidate for oscillator based non-Boolean computing.

42 ENGINEERING↗
DOE OSTI2019

Orientational Dependence of Cofacial Porphyrin–Quinone Electronic Interactions within the Strong Coupling Regime

We examine the relative magnitudes of electronic coupling HDA in two face-to-face rigid and diastereomeric (porphinato)zinc(II)–quinone (PZn–Q) as-semblies, 1β-ZnA and 1β-ZnB, in which the six quinonyl carbon atoms lie in virtually identical arrangements relative to the PZn plane at sub-van der Waals donor–acceptor (D–A) interplanar separations. Steady-state and time-resolved transient optical data and computational studies show that minor differences in relative D–A cofacial orientation give rise to disparate H DA magnitudes for both photoinduced charge separation (CS) and thermal charge recombination (CR). Here, time-dependent density functional theory (TDDFT) computations illuminate the nature of direct charge transfer states and the electronic structural factors that give rise to these differential H DA s. These data show more extensive mixing of locally excited (LE) and CS states in 1β-ZnA relative to 1β-ZnB and that these H DA differences track the magnitudes of electronic coupling matrix elements determined from steady-state electronic spectral data and thermal CR rate constants measured via pump–probe spectroscopy. Collectively, this work shows that electron transfer dynamics may be manipulated in cofacial D–A systems, even at sub-van der Waals contact, provided that conformational rigidity precludes structural fluctuations that modulate D–A interactions on the charge transfer time scale.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

The beat in laser-accelerated ion beams

Regular modulation in the ion velocity distribution becomes detectable if intense femtosecond laser pulses with very high temporal contrast are used for target normal sheath acceleration of ions. Analytical and numerical analysis of the experimental observation associates the modulation with the half-cycle of the driving laser field period. In processes like ion acceleration, the collective and laser-frequency determined electron dynamics creates strong fields in plasma to accelerate the ions. Even the oscillatory motion of electrons and its influence on the acceleration field can dominate over smoothing effects in plasma if a high temporal contrast of the driving laser pulse is given. Acceleration parameters can be directly concluded out of the experimentally observed modulation period in ion velocity spectra. The appearance of the phenomenon at a temporal contrast of ten orders between the intensity of the pulse peak and the spontaneous amplified emission background as well as remaining intensity wings at picosecond time-scale might trigger further parameter studies with even higher contrast.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗