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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 91 records · Page 5

Electrochemically Induced Strain Evolution in Pt–Ni Alloy Nanoparticles Observed by Bragg Coherent Diffraction Imaging

Strain is known to enhance the activity of the oxygen reduction reaction in catalytic platinum alloy nanoparticles, whose inactivity is the primary impediment to efficient fuel cells and metal–air batteries. Here, Bragg coherent diffraction imaging (BCDI) was employed to reveal the strain evolution during the voltammetric cycling in Pt–Ni alloy nanoparticles composed of Pt 2 Ni 3 , Pt 1 Ni 1 , and Pt 3 Ni 2 . Analysis of the 3D strain images using a core–shell model shows that the strain as large as 5% is induced on Pt-rich shells due to Ni dissolution. The composition dependency of the strain on the shells is in excellent agreement with that of the catalytic activity. The present study demonstrates that BCDI enables quantitative determination of the strain on alloy nanoparticles during electrochemical reactions, which provides a means to exploit surface strain to design a wide range of electrocatalysts.

36 MATERIALS SCIENCE↗

Retrieval of full angular- and energy-dependent complex transition dipoles in the molecular frame from laser-induced high-order harmonic signals with aligned molecules

High-order harmonic signals generated in molecules are the consequence of coherent summation of complex laser-induced transition dipoles $\textit{d}(θ, ω)$ with each fixed-in-space molecule; here $\theta$ is the angle of the molecular axis with respect to the laser polarization axis and $\omega$ is the harmonic energy. In the so-called rotational coherent spectroscopy, it is proposed to extract the fixed-in-space $\textit{d}(θ, ω)$ in the molecular frame by measuring harmonics generated by a probing laser from the rotational molecular wave packets that have been prepared by a prior pump laser. By varying the time delay between the two lasers, methods have been utilized to extract the $\theta$ dependence of both the amplitude and phase of each individual harmonic, but the relative phase between harmonics cannot be retrieved. Here we report that this limitation can be removed. It requires the additional measurement of harmonic spectra versus the pump-probe angles at one fixed time delay. The two-dimensional input harmonic data (time-delay and pump-probe angle) are then used to retrieve the full complex transition dipole $\textit{d}(θ, ω)$ using a retrieval method based on machine learning algorithms. Finally, we demonstrate this method on N 2 and CO 2 molecules.

74 ATOMIC AND MOLECULAR PHYSICS↗

Entangling-gate error from coherently displaced motional modes of trapped ions

Entangling gates in trapped-ion quantum computers are most often applied to stationary ions with initial motional distributions that are thermal and close to the ground state, while those demonstrations that involve transport generally use sympathetic cooling to reinitialize the motional state prior to applying a gate. Future systems with more ions, however, will face greater nonthermal excitation due to increased amounts of ion transport and exacerbated by longer operational times and variations over the trap array. In addition, pregate sympathetic cooling may be limited due to time costs and laser access constraints. In this paper, we analyze the impact of such coherent motional excitation on entangling-gate error by performing simulations of Mølmer-Sørenson (MS) gates on a pair of trapped-ion qubits with both thermal and coherent excitation present in a shared motional mode at the start of the gate. Here, we quantify how a small amount of coherent displacement erodes gate performance in the presence of experimental noise, and we demonstrate that adjusting the relative phase between the initial coherent displacement and the displacement induced by the gate or using Walsh modulation can suppress this error. We then use experimental data from transported ions to analyze the impact of coherent displacement on MS-gate error under realistic conditions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Coherent homodyne detection for amplified cross-beam electric-field induced second harmonic

The electric-field induced second harmonic (E-FISH) signal sensing is commonly used as a nonlinear optical technique to probe electric fields inside a plasma region. Cross-beam E-FISH is being investigated to improve spatial resolution by defining the interaction volume via a controlled geometry of two overlapping noncolinear optical beams. This drastic reduction in interaction length of the electric field and laser region results in a significant signal reduction. Here, to overcome this signal reduction, we introduce coherent amplification of the cross-beam E-FISH signal by mixing the low E-FISH signal with a phase-locked bright local oscillator. We demonstrate enhancement of the signal. By introducing a local oscillator we can now derive the polarity of the measured electric field through the phase of the homodyne signal. To illustrate the technique, we, for the first time, to the best of our knowledge, measure the magnitude and the direction of the electric field in a cold atmospheric pressure plasma jet, which dynamically follows the profile of the applied bias current.

42 ENGINEERING↗

Hard jet substructure in a multistage approach

We present predictions and postdictions for a wide variety of hard jet-substructure observables using a multistage model within the framework. The details of the multistage model and the various parameter choices are described in []. A novel feature of this model is the presence of two stages of jet modification: a high-virtuality phase [modeled using the modular all twist transverse-scattering elastic-drag and radiation model ()], where modified coherence effects diminish medium-induced radiation, and a lower virtuality phase [modeled using the linear Boltzmann transport model ()], where parton splits are fully resolved by the medium as they endure multiple scattering induced energy loss. Energy-loss calculations are carried out on event-by-event viscous fluid dynamic backgrounds constrained by experimental data. The uniform and consistent descriptions of multiple experimental observables demonstrate the essential role of modified coherence effects and the multistage modeling of jet evolution. Using the best choice of parameters from [], and with no further tuning, we present calculations for the medium modified jet fragmentation function, the groomed jet momentum fraction z g and angular separation r g distributions, as well as the nuclear modification factor of groomed jets. These calculations provide accurate descriptions of published data from experiments at the Large Hadron Collider. Furthermore, we provide predictions from the multistage model for future measurements at the BNL Relativistic Heavy Ion Collider. Published by the American Physical Society 2024

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Coherent microwave scattering from resonance enhanced multi-photon ionization (Radar REMPI): A review

Coherent microwave scattering from laser-induced plasmas, including weakly ionized plasma, laser sparks, Multiphoton Ionization (MPI), and Resonance Enhanced Multi-Photon Ionizations (Radar REMPI) has achieved much successes in plasma, reactive and nonreactive flow diagnostics. Under illumination of microwaves (Radar), electrons inside the laser-induced plasma oscillate with the electric field of the microwave and re-radiate from the electrons forming coherent scattering. In the far-field approximation, the microwave scattering from the small volume plasma reflects the generation and evolution of unbounded electrons inside the plasma, when the microwave wavelength is much greater than the size of the plasma and the skin layer depth at the microwave frequency is larger than the size of the plasma. Laser excitation schemes, microwave detection methods, calibration of microwave scattering, and the novel applications of the technique have been significantly expanded and improved. Furthermore, this review paper summarizes physical principles, various REMPI excitation schemes for atomic and molecular species, and temperature measurements in plasma and reactive flows. Discussions on new research directions and applications are given at the end.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

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↗

Mechanisms Underlying a Quantum Superposition Microscope Based on THz-Driven Coherent Oscillations in a Two-Level Molecular Sensor

Here we report pump-probe measurements of a hydrogen molecule (H 2 ) in the tunnel junction of a scanning tunneling microscope (STM) coupled to ultrashort terahertz (THz) pulses. The coherent oscillation of the THz induced DC tunneling current at a frequency of ~0.5 THz fingerprints the absorption by H 2 as a two-level system (TLS). Two components of the oscillatory signal are observed and point to both photon and field aspects of the THz pulses. A few loosely bound states with similar energies for the upper state of the TLS are evidenced by the coherent revival of oscillatory signal. Furthermore, the comparison of spectroscopic features of H 2 with different tips provides an understanding of the TLS for H 2 .

36 MATERIALS SCIENCE↗

Impact of moderate pump–Stokes chirp on femtosecond coherent anti-Stokes Raman scattering spectra

The effects of inducing moderate chirp in the pump and Stokes beams in chirped-probe-pulse femtosecond coherent anti-Stokes Raman scattering (CARS) spectroscopy are discussed. This is an important issue for measurements in high-pressure systems where the CARS beams must be transmitted through glass of significant thickness to reach the probe volume of interest. The effects were investigated both experimentally, by inserting disks of SF-11 glass into the pump and Stokes beam paths, and theoretically, by incorporating pulse chirp into our time-dependent density matrix (TDDM) simulations. Experimentally, we found that inducing moderate pump and Stokes chirp produced significant spectral narrowing of the nonresonant four-wave mixing contribution to the CARS signal, and this allowed us to control the resonant excitation bandwidth to eliminate interferences from neighboring species. The temperature measurement accuracy and precision were essentially unchanged with respect to the unchirped pump and Stokes case. The effect of moderate pump and Stokes chirp on the narrowing of the Raman excitation efficiency envelope was investigated by solving the full set of TDDM through direct numerical integration. The numerical efficiency of the solutions was enhanced dramatically by developing a parallel version of the TDDM code. The calculated Raman excitation efficiency profile was incorporated in our phenomenological spectral fitting codes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

All-optical seeding of a light-induced phase transition with correlated disorder

Ultrafast manipulation of vibrational coherence is an emergent route to control the structure of solids. However, this strategy can only induce long-range correlations and cannot modify atomic structure locally, which is required in many technologically-relevant phase transitions. Here, we demonstrate that ultrafast lasers can generate incoherent structural fluctuations which are more efficient for material control than coherent vibrations, extending optical control to a wider range of materials. We observe that local, non-equilibrium lattice distortions generated by a weak laser pulse reduce the energy barrier to switch between insulating and metallic states in vanadium dioxide by 6%. In conclusion, seeding inhomogeneous structural-fluctuations presents an alternative, more energy efficient, route for controlling materials that may be applicable to all solids, including those used in data and energy storage devices.

36 MATERIALS SCIENCE↗

Symmetry Protected Two-Photon Coherence Time

We report the observation of symmetry protected two-photon coherence time of biphotons generated from backward spontaneous four-wave mixing in laser-cooled 87 Rb atoms. When biphotons are nondegenerate, nonsymmetric photonic absorption loss results in exponential decay of the temporal waveform of the two-photon joint probability amplitude, leading to shortened coherence time. In contrast, in the case of degenerate biphotons, when both paired photons propagate with the same group velocity and absorption coefficient, the two-photon coherence time, protected by space-time symmetry, remains unaffected by medium absorptive losses. Furthermore, our experimental results validate these theoretical predictions. This outcome highlights the pivotal role of symmetry in manipulating and controlling photonic quantum states.

74 ATOMIC AND MOLECULAR PHYSICS↗

Spectral proper orthogonal decomposition of active wake mixing dynamics in a stable atmospheric boundary layer

Recent advancements in the use of active wake mixing (AWM) to reduce wake effects on downstream turbines open new avenues for increasing power generation in wind farms. However, a better understanding of the fluid dynamics underlying AWM is still needed to make wake mixing a reliable strategy for wind farm flow control. In this work, a spectral proper orthogonal decomposition (SPOD) is used to analyze the dynamics of coherent flow structures that are induced in the wake through blade pitch actuation. The data are generated using the ExaWind software suite to perform large eddy simulations of an NREL 2.8 MW turbine operating in a stable atmospheric boundary layer. SPOD tracks the modal behavior of flow structures from their generation in the turbine induction field through their growth in the near-wake region and to their subsequent evolution and energy transfers in the far wake. SPOD is shown to be a useful tool in the context of AWM because it translates the wavenumber and frequency inputs to the turbine controller to structures in the wake. A decomposition of the radial shear stress flux in the wake is also developed using SPOD to measure the contribution of coherent flow structures to mean flow turbulent entrainment and wake recovery. The effectiveness of AWM is connected to its ability to excite inherent structures in the wake of the turbine that arise using baseline controls. The effects of AWM on blade loading are also analyzed by connecting the axial force along the blade to the SPOD analysis of the turbine induction field. Lastly, the performance of different AWM strategies is demonstrated in a two-turbine array.

17 WIND ENERGY↗

Monitoring aromatic ring-currents in Mg-porphyrin by time-resolved circular dichroism

We report time-resolved circular dichroism signals (TRCD) in the X-ray regime can directly probe the magnitude and the direction of ring currents in molecules. The electronic ring currents in Mg-porphyrin, generated by a coherent superposition of electronic states induced by a circularly polarized UV pulse, are tracked by a time-delayed circularly polarized attosecond X-ray pulse. The signals are calculated using the minimal coupling Hamiltonian, which directly makes use of transition current densities. The TRCD signals obtained from the left and right circularly polarized light pump have opposite signs, revealing the direction of the ring current. Molecular aromaticity and its role in photochemical reactions such as ring opening or closure can be studied using this technique.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Bragg Coherent Imaging of Fluctuating Domains

This review presents two examples of domain dynamics in crystalline solid state samples which were imaged recently with synchrotron X-rays by Bragg Coherent Diffraction methods. Domains are associated with sub-atomic phase shifts in the structure which are revealed by the strong phase contrast associated with Bragg diffraction. At low temperatures, La2-xSrxNiO4 has an antiferromagnetic spin-ordered phase with correlation lengths of 200 nm; its domains are imaged with magnetic Bragg Ptychography to visualize their slow fluctuations. Hydrothermally synthesized nanocrystalline BaTiO3 is found to be made up of ~50 nm domains using Bragg Coherent Diffraction Imaging; electric field induced movement of its internal domain walls is a likely explanation of the nano-material's anomalously large dielectric constant, which is used in the manufacture of multilayer ceramic capacitors

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Evaluating radiation impact on transmon qubits in above and underground facilities

Superconducting qubits can be sensitive to energy deposits caused by cosmic rays and ambient radioactivity. While previous studies have explored correlated effects in time and space due to cosmic ray interactions, we present the first direct comparison of a transmon qubit’s performance measured at two distinct sites: the above-ground SQMS facility (Fermilab, US) and the deep-underground Gran Sasso Laboratory (Italy). Despite the stark difference in radiation levels, we observe a similar average qubit relaxation time of approximately 80 microseconds at both locations. To investigate radiation-induced events, we employ a fast decay detection protocol, comparing the relative rates of events between the two environments. Although intrinsic noise remains the dominant source of errors in superconducting qubits, our analysis revealed a significant excess of radiation-induced events for high-coherence transmon qubits operated above-ground. Finally, using γ-ray sources with increasing activity levels, we evaluate the qubit response in a controlled low-background environment.

De Dominicis, Francesco [GSSI, Aquila; INFN, LNS]↗

Power output of turbines mounted on tension-leg platforms subjected to fully developed ocean gravity waves

A concern in the deployment of large wind turbines on ocean floating platforms is the effect of floating-platform motions on their electrical power generation. Further, it is not clear how floating motions influence waking, which might affect the combined power generation of collections of turbines. We examine the average power output of a single and a collection of NREL 5 MW wind turbines mounted on a tension-leg platform (TLP) under the action of fully developed ocean wave motions, coupling floating motions with the large-eddy simulation (LES) of atmospheric and rotor dynamics. The ocean dynamics enter as fully developed waves derived from the Pierson–Moskowitz spectrum. To assess the influence of ocean motions, we performed simulations over the full range of wind speeds in the operational range of the turbine, reporting comparisons of average power output when the platforms are allowed to move to when they are held rigidly in place. In all simulations, we find that the effects of the TLP floating-platform's induced motions have a minor effect on single and multiple turbine power production and wake deficits. Even when using coherent and large amplitude harmonic-floating-induced perturbations, any significant wake modifications from floating motions are confined to the near-wake region, where downstream turbines are unlikely to be located. The relatively small amplitude of TLP motions relative to pre-existing turbulent fluctuations are the primary reason for low wake and power modifications downstream.

Restrepo, Juan [ORNL] (ORCID:0000000326092882)↗

Selective bond formation triggered by short optical pulses: quantum dynamics of a four-center ring closure

Here we report bond formation induced by an ultrashort UV pulse. The photochemical process is described by quantum dynamics as coherent electronic and nuclear motions during the ultrashort pulse induced ring closure of norbornadiene to quadricyclane. Norbornadiene consists of two ethylene moieties connected by a rigid (CH 2 ) 3 bridge. Upon photoexcitation, two new sigma bonds are formed, resulting in the closure of a four-atom ring. As a medium-sized polyatomic molecule, norbornadiene exhibits a high density of strongly coupled electronic states from about 6 eV above the ground state. We report on inducing the formation of the new bonds using a short femtosecond UV pulse to pump a non-equilibrium electronic density in the open form that evolves towards the closed ring form. As the coherent electronic-nuclear coupled dynamics unfold, the excited states change character through non-adiabatic interactions and become valence states for the two new C–C bonds of quadricyclane. Our three-dimensional fully quantum dynamical grid simulations during the first 200 fs show that short UV pulses of different polarization initiate markedly different initial non-equilibrium electronic densities that follow different dynamical paths to the S 0 /S 1 conical intersection. They lead to different initial relative yields of quadricyclane, thereby opening the way to controlling bond-making with attopulses.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Raman spectroscopy of neutron irradiated silicon carbide

The effects of neutron irradiation on microstructural evolution and the resultant changes in physical and mechanical properties are of critical importance for the development of silicon carbide (SiC) materials for nuclear applications. This study neutron-irradiated βSiC under a wide range of conditions at temperatures between 235 and 750°C and neutron doses of 0.01–11.8 displacements per atom, and then evaluated the effects on the SiC structure using Raman spectroscopy. The SiC optical phonon lines were shifted to lower wavenumbers by irradiation. Correlations were found among the wavenumber of the longitudinal optical phonon line, irradiation-induced swelling, and irradiation temperature. The peak shift also correlated indirectly with decreasing thermal conductivity of irradiated SiC. The irradiation-induced peak shift is explained by combinations of lattice strain, reduction of the elastic modulus, and other factors including decreasing coherent domain size. These findings bridge irradiation-induced microstructural changes and property changes and illustrate how Raman spectroscopy is a useful tool for nondestructively assessing irradiated SiC materials for nuclear applications.

Koyanagi, T.↗