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All sources NASA NTRS DOE OSTI

DOE OSTI2020

Visualizing conical intersection passages via vibronic coherence maps generated by stimulated ultrafast X-ray Raman signals

Significance The capabilities of modern X-ray sources have substantially increased the temporal and spectral resolutions for the observation of elementary molecular events. Theoretically, it has been shown that these unique features can be exploited to probe vibronic coherences that emerge when molecules pass through conical intersections. Here, we demonstrate this technique for the photorelaxation of the RNA-nucleobase uracil after UV excitation. The generated coherence maps reveal the path of the nuclear wavepacket on the excited-state surface in the vicinity of the conical intersection. This information is directly accessible from the spectroscopically recorded signal. Being transferrable to other molecules, these coherence maps will provide detailed visualizations of other nonadiabatic passages in the future.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1980

Evidence for globally coherent variability in solar magnetic flux emergence

We examine the large-scale spatial and temporal variations in the emergence of X-ray bright points on the sun, in order to study the global properties of magnetic flux emergence. Major variations in the rate of flux emergence are observed at all solar latitudes, on a time scale of 3-5 months. The most economical explanation of the observations is that the full sun participated in a single large eruptive event during the available 8 month observing period from Skylab in 1973. The peak of this global event corresponds in time to the eruption of a major complex of activity. Moreover, it appears that the only portion of the solar surface which deviates from the above pattern of behavior is the low latitude region in the vicinity of the AR complex; this area shows a temporary depletion immediately following the AR outburst. The high-latitude regions in both hemispheres show the same variation and appear to lead the low-latitude emergence by approximately 1 month.

Golub, L.↗

DOE OSTI2021

Imaging conical intersection dynamics during azobenzene photoisomerization by ultrafast X-ray diffraction

Significance Vibronic coherences are unique features that emerge in the decisive moments of photochemistry and photophysics. Here we demonstrate how X-ray diffraction can access fundamental information about these coherences. This is enabled by recent developments at free-electron lasers, working toward temporal resolution and single-molecule accessibility of scattering-based measurements. Time-resolved diffraction patterns of the isomerization of azobenzene are simulated. The process is monitored in time via the momentum-space signal, with a special focus on the mixed elastic/inelastic scattering from coherences. We give practical ideas on how this relatively weak contribution to the signal can potentially be retrieved. A direct connection to the real-space movie of the conical intersection dynamics is made, enabling the observation of quantum coherences that direct chemical processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Pushing the Boundaries of Coherence in Superconducting Quantum Systems at the SQMS Center for Computing, Sensing, and Metrology

This talk will highlight recent advances at the SQMS Center in understanding and mitigating decoherence in superconducting quantum systems, focusing on both transmon qubits and 3D superconducting cavities. I will present results from systematic studies of materials and devices, aimed at identifying key sources of loss: including two-level systems (TLS), quasiparticles, and other noise mechanisms. These studies span microwave loss characterization in materials such as niobium, tantalum, aluminum, and their native oxides, as well as substrate losses in silicon and sapphire. Using both qubits and cavities, we disentangle subsystem contributions to loss and develop a hierarchy of mitigation strategies. Through these efforts, we have achieved transmon coherence times exceeding one millisecond. I will also present investigations into quasiparticle dynamics, including bursts observed in qubits located above ground and in the Gran Sasso underground laboratory. Additional studies explore temperature dependence to distinguish between TLS and quasiparticle losses, and reveal that applying a magnetic field can reduce temporal T1 fluctuations in transmons. Building on these results, we demonstrate a record-coherence two-cell cavity-qudit system with coherence times exceeding 20 milliseconds. By leveraging sideband interactions and error-resilient protocols including measurement-based correction and post-selection, we achieve high-fidelity quantum state control. This includes preparation of Fock states up to N = 20 with fidelities over 95%, and two-mode entanglement with coherence-limited fidelities reaching 99.9% after post-selection. These achievements position the SQMS platform as a powerful foundation for scalable quantum information processing and high-dimensional qudit encodings. Finally, I will discuss how these ultra-coherent systems are being deployed in emerging quantum sensing applications, including dark matter searches and gravitational wave detection.

Roy, Tanay [Fermilab]↗

DOE OSTI2024

Intermittent cluster dynamics and temporal fractional diffusion in a bulk metallic glass

Glassy solids evolve towards lower-energy structural states by physical aging. This can be characterized by structural relaxation times, the assessment of which is essential for understanding the glass’ time-dependent property changes. Conducted over short times, a continuous increase of relaxation times with time is seen, suggesting a time-dependent dissipative transport mechanism. By focusing on micro-structural rearrangements at the atomic-scale, we demonstrate the emergence of sub-diffusive anomalous transport and therefore temporal fractional diffusion in a metallic glass, which we track via coherent x-ray scattering conducted over more than 300,000 s. At the longest probed decorrelation times, a transition from classical stretched exponential to a power-law behavior occurs, which in concert with atomistic simulations reveals collective and intermittent atomic motion. Our observations give a physical basis for classical stretched exponential relaxation behavior, uncover a new power-law governed collective transport regime for metallic glasses at long and practically relevant time-scales, and demonstrate a rich and highly non-monotonous aging response in a glassy solid, thereby challenging the common framework of homogeneous aging and atomic scale diffusion.

42 ENGINEERING↗

DOE OSTI2024

Light-wave-controlled Haldane model in monolayer hexagonal boron nitride

In recent years, the stacking and twisting of atom-thin structures with matching crystal symmetry has provided a unique way to create new superlattice structures in which new properties emerge. In parallel, control over the temporal characteristics of strong light fields has allowed researchers to manipulate coherent electron transport in such atom-thin structures on sublaser-cycle timescales. Here we demonstrate a tailored light-wave-driven analogue to twisted layer stacking. Tailoring the spatial symmetry of the light waveform to that of the lattice of a hexagonal boron nitride monolayer and then twisting this waveform result in optical control of time-reversal symmetry breaking and the realization of the topological Haldane model in a laser-dressed two-dimensional insulating crystal. Further, the parameters of the effective Haldane-type Hamiltonian can be controlled by rotating the light waveform, thus enabling ultrafast switching between band structure configurations and allowing unprecedented control over the magnitude, location and curvature of the bandgap. This results in an asymmetric population between complementary quantum valleys that leads to a measurable valley Hall current, which can be detected by optical harmonic polarimetry. The universality and robustness of our scheme paves the way to valley-selective bandgap engineering on the fly and unlocks the possibility of creating few-femtosecond switches with quantum degrees of freedom.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

The MOSAiC Distributed Network: Observing the coupled Arctic system with multidisciplinary, coordinated platforms

Central Arctic properties and processes are important to the regional and global coupled climate system. The Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) Distributed Network (DN) of autonomous ice-tethered systems aimed to bridge gaps in our understanding of temporal and spatial scales, in particular with respect to the resolution of Earth system models. By characterizing variability around local measurements made at a Central Observatory, the DN covers both the coupled system interactions involving the ocean-ice-atmosphere interfaces as well as three-dimensional processes in the ocean, sea ice, and atmosphere. The more than 200 autonomous instruments (“buoys”) were of varying complexity and set up at different sites mostly within 50 km of the Central Observatory. During an exemplary midwinter month, the DN observations captured the spatial variability of atmospheric processes on sub-monthly time scales, but less so for monthly means. They show significant variability in snow depth and ice thickness, and provide a temporally and spatially resolved characterization of ice motion and deformation, showing coherency at the DN scale but less at smaller spatial scales. Ocean data show the background gradient across the DN as well as spatially dependent time variability due to local mixed layer sub-mesoscale and mesoscale processes, influenced by a variable ice cover. The second case (May–June 2020) illustrates the utility of the DN during the absence of manually obtained data by providing continuity of physical and biological observations during this key transitional period. We show examples of synergies between the extensive MOSAiC remote sensing observations and numerical modeling, such as estimating the skill of ice drift forecasts and evaluating coupled system modeling. The MOSAiC DN has been proven to enable analysis of local to mesoscale processes in the coupled atmosphere-ice-ocean system and has the potential to improve model parameterizations of important, unresolved processes in the future.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1987

Gyroresonant pitch angle scattering by coherent and incoherent whistler mode waves in the magnetosphere

A test particle approach is used to compare gyroresonant pitch angle scattering of energetic electrons by coherent versus incoherent whistler mode waves, for the case in which the coherent wave amplitude is below the nonlinear phase trapping threshold. Wave packets of 400 ms duration propagating along the magnetic field at L = 4 within the plasmasphere are considered, and the wave-induced pitch angle scattering along the propagation path from one hemisphere to the other and the resulting precipitation flux are computed. An incoherent wave spectrum is simulated by random modulation of the wave frequency at intervals of 1 ms, thereby generating signals with nearly constant power spectral density over a bandwidth of 2 kHz centered at 5.5 kHz. The associated pitch angle scattering is compared with that of a monochromatic 5.5-kHz signal of 400 ms duration. Results of the test particle analysis are compared with those expected on the basis of a classical diffusion treatment, and an expression is derived for an effective “diffusion” coefficient for pitch angle scattering by coherent waves. The trajectory followed by a particle when interacting with incoherent waves essentially represents a random walk in velocity space, while for coherent waves the pitch angle of the particle varies in a well-defined manner. In spite of the fact that individual particle scatterings are typically larger for coherent waves, the peak precipitation fluxes induced by incoherent waves are found to be approximately the same as those for coherent waves having the same total power. This results from the fact that incoherent waves interact with particles over a wider range of energies. As a consequence, the energy spectrum and the temporal extent of transient precipitation pulses due to incoherent wave packets are broader than those for equivalent coherent ones.

Umran S Inan↗

NASA NTRS2001

Stochastic Modeling and Generation of Partially Polarized or Partially Coherent Electromagnetic Waves

Many new Earth remote-sensing instruments are embracing both the advantages and added complexity that result from interferometric or fully polarimetric operation. To increase instrument understanding and functionality a model of the signals these instruments measure is presented. A stochastic model is used as it recognizes the non-deterministic nature of any real-world measurements while also providing a tractable mathematical framework. A stationary, Gaussian-distributed model structure is proposed. Temporal and spectral correlation measures provide a statistical description of the physical properties of coherence and polarization-state. From this relationship the model is mathematically defined. The model is shown to be unique for any set of physical parameters. A method of realizing the model (necessary for applications such as synthetic calibration-signal generation) is given and computer simulation results are presented. The signals are constructed using the output of a multi-input multi-output linear filter system, driven with white noise.

Davis, Brynmor↗

NASA NTRSDate not supplied

Coherence Analysis of the Space Launch System using Unsteady Pressure Sensitive Paint

Transonic buffet during atmospheric ascent is a major source of unsteady loading on launch vehicles that, in the past, has led to structural failures. Thus, determining accurate buffet forcing functions (BFFs) to properly predict the vehicle response to buffet is of vital importance in launch vehicle design. The state of the art for obtaining the BFFs relies on wind-tunnel tests where the fluctuating pressures are measured by pressure transducers (PTs) at sparse locations on a rigid, geometrically-scaled buffet model. To compute the BFFs, the outer mold line (OML) of the vehicle is mapped onto contiguous panels centered at the location of the PTs and the measured fluctuating pressures are integrated over the panels’ areas. To mitigate conservatism due to the assumption that the measured buffet pressures act in phase across each panel, coherence factors are applied, effectively reducing the integration areas and, therefore, the buffet forces. For coherence factors to provide the proper level of BFF attenuation, accurate knowledge of the spatial and temporal correlation of the buffet pressures is paramount. Unfortunately, even with hundreds of unsteady pressure transducers instrumenting the models, compromises must be made on the spatial resolution of the PTs. Typically, the PT layout aims at resolving the pressure correlation along the longitudinal axis of the vehicle, assuming that coherent structures propagate mostly in the longitudinal direction. As a result, the distribution of azimuthal/cross-stream correlation is not well known and its impact on the estimated BFFs is often neglected. To fill this and other knowledge gaps, extremely high spatial-resolution uPSP data were collected for three different production-design configurations of the Space Launch System in the NASA Ames Research Center Unitary Plan Wind Tunnel 11-Foot Transonic Wind Tunnel. Specifically, two cargo configurations, the Block 1 and Block 1B, and one crew configuration, the Block 1B crew, were surveyed at resolutions ranging from 600,000 to over 1 million uPSP measurement locations. To shed light on the temporal and spectral behavior of are presented. Several OML regions and flow features of interest are investigated, from theexpansion/shock on the Orion Multi-Purpose Crew Vehicle, to the terminal shock environment on the core stage, and the Strouhal shedding behind the boosters forward attach. The sensitivity of these environments to the vehicle attitude is examined. Furthermore, for selected panels,coherence factors that accurately capture the azimuthal coherence distribution of the buffetpressures are derived and their impact on the estimated BFFs is discussed. Finally, distributions of the local convection velocity and cross spectrum phase are presented.

buffet↗

NASA NTRS2014

Application of Spectral Analysis Techniques in the Intercomparison of Aerosol Data. Part II: Using Maximum Covariance Analysis to Effectively Compare Spatiotemporal Variability of Satellite and AERONET Measured Aerosol Optical Depth

Moderate Resolution Imaging SpectroRadiometer (MODIS) and Multi-angle Imaging Spectroradiomater (MISR) provide regular aerosol observations with global coverage. It is essential to examine the coherency between space- and ground-measured aerosol parameters in representing aerosol spatial and temporal variability, especially in the climate forcing and model validation context. In this paper, we introduce Maximum Covariance Analysis (MCA), also known as Singular Value Decomposition analysis as an effective way to compare correlated aerosol spatial and temporal patterns between satellite measurements and AERONET data. This technique not only successfully extracts the variability of major aerosol regimes but also allows the simultaneous examination of the aerosol variability both spatially and temporally. More importantly, it well accommodates the sparsely distributed AERONET data, for which other spectral decomposition methods, such as Principal Component Analysis, do not yield satisfactory results. The comparison shows overall good agreement between MODIS/MISR and AERONET AOD variability. The correlations between the first three modes of MCA results for both MODIS/AERONET and MISR/ AERONET are above 0.8 for the full data set and above 0.75 for the AOD anomaly data. The correlations between MODIS and MISR modes are also quite high (greater than 0.9). We also examine the extent of spatial agreement between satellite and AERONET AOD data at the selected stations. Some sites with disagreements in the MCA results, such as Kanpur, also have low spatial coherency. This should be associated partly with high AOD spatial variability and partly with uncertainties in satellite retrievals due to the seasonally varying aerosol types and surface properties.

aerosols↗

NASA NTRS1985

Coherent structures in a turbulent mixing layer - A comparison between direct numerical simulations and experiments

An eduction scheme has been developed in an attempt to determine the characteristics of large-scale vortical structures in a turbulent mixing layer. This analysis scheme has been applied to a set of experimental data taken in a new, larger mixing layer facility designed to minimize boundary and resonance effects. A similar scheme has been developed to apply to the results of a direct numerical simulation of a temporally growing mixing layer. A comparison of the two approaches shows important similarities in the coherent structures. The numerical simulations indicate that low levels of coherent forcing can dramatically change the evolution of the mixing layer. In the absence of such forcing, the numerical simulations and experiments show a lack of regularity in the transverse position, spacing, amplitude, shape and spanwise coherence of the large-scale vortical structures.

Metcalfe, R. W.↗

DOE OSTI2024

Mapping the nonequilibrium order parameter of a quasi-two dimensional charge density wave system

The driving force of a charge density wave (CDW) transition in quasi-two dimensional systems is still debated, while being crucial in understanding electronic correlation in such materials. Here we use femtosecond time- and angle-resolved photoemission spectroscopy combined with computational methods to investigate the coherent lattice dynamics of a prototypical CDW system. The photo-induced temporal evolution of the periodic lattice distortion associated with the amplitude mode reveals the dynamics of the free energy functional governing the order parameter. Our approach establishes that optically-induced screening rather than CDW melting at the electronic level leads to a transiently modified potential which explains the anharmonic behaviour of the amplitude mode and discloses the structural origin of the symmetry-breaking phase transition.

electronic properties and materials↗

DOE OSTI2023

Invited article: X-ray phase contrast imaging in inertial confinement fusion and high energy density research

X-ray phase contrast imaging (XPCI) provides enhanced image contrast beyond absorption-based x-ray imaging alone due to refraction and diffraction from gradients in the object material density. It is sensitive to small variations in density, such as internal voids, cracks, grains, defects, and material flow, as well as to stronger density variations such as from a shock wave. Beyond its initial use in biology and materials science, XPCI is now routinely used in inertial confinement fusion (ICF) and high energy density (HED) research, first to characterize ICF capsules and targets, and later applied in dynamic experiments, where coherent x-ray sources, ultrafast x-ray pulses, and high temporal and spatial resolution are required. In this Review article, XPCI image formation theory is presented, its diverse use in ICF and HED research is discussed, the unique requirements for ultrafast XPCI imaging are given, as well as current challenges and issues in its use.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2024

Quantifying the thermal effect and methyl radical production in nanosecond repetitively pulsed glow discharges applied to a methane-air flame

In this work, we investigated non-equilibrium plasma produced by nanosecond repetitively pulsed glow discharges applied across a lean premixed methane-air flame. The flame is stationary, axisymmetric, and laminar. The discharges are applied on the symmetry axis crossing the reactant gases, flame front, and product gases, allowing phase-locked averaged measurements and comparisons with axisymmetric numerical simulations. The thermal effect and methyl radical production are quantified in the discharge in the reactant gas region. One-dimensional, two-beam, hybrid, femtosecond-picosecond, coherent anti-Stokes Raman scattering is used to acquire spatial and temporal profiles of temperature and oxygen-to-nitrogen concentration ratio. Photo-fragmentation laser-induced fluorescence is used to acquire quantitative two-dimensional profiles of methyl radicals in the discharge providing the first quantitative imaging of methyl produced ahead of a flame by plasma-induced methane dissociation. The spatial profiles of temperature and oxygen-to-nitrogen concentration ratio are in steady state, indicating that individual discharges have an insignificant heating effect. Upper and lower bounds of the produced mole fraction of methyl radicals in the plasma are obtained due to uncertainties in the collisional quenching rates of excited state methylidyne radicals in the plasma. The discharges produce a maximum of 600–1100 ppm of methyl radicals upstream of the flame front within 25 ns. This amount is similar to the predicted methyl mole fraction for the flame without plasma and thus represents a significant chemical perturbation to the reactants upstream of the flame front. The produced methyl follows an exponential decay in the first microsecond after the discharge with a decay constant of 8 µs close to the flame, and 0.8 µs further from the flame. The decay then deviates from the exponential curve and the methyl persists for tens of microseconds. The results suggest that for the tested configuration, the thermal effect of individual discharges through fast gas heating is negligible, while active chemical species are produced in large quantities in the reactant gases, upstream of the flame front.

hybrid fs-ps CARS↗

NASA NTRS2003

A Self-Contained Mapping Closure Approximation for Scalar Mixing

Scalar turbulence exhibits interplays of coherent structures and random fluctuations over a broad range of spatial and temporal scales. This feature necessitates a probabilistic description of the scalar dynamics, which can be achieved comprehensively by using probability density functions (PDFs). Therefore, the challenge is to obtain the scalar PDFs (Lundgren 1967; Dopazo 1979). Generally, the evolution of a scalar is governed by three dynamical processes: advection, diffusion and reaction. In a PDF approach (Pope 1985), the advection and reaction can be treated exactly but the effect of molecular diffusion has to be modeled. It has been shown (Pope 1985) that the effect of molecular diffusion can be expressed as conditional dissipation rates or conditional diffusions. The currently used models for the conditional dissipation rates and conditional diffusions (Pope 1991) have resisted deduction from the fundamental equations and are unable to yield satisfactory results for the basic test cases of decaying scalars in isotropic turbulence, although they have achieved some success in a variety of individual cases. The recently developed mapping closure approach (Pope 1991; Chen, Chen & Kraichnan 1989; Kraichnan 1990; Klimenko & Pope 2003) provides a deductive method for conditional dissipation rates and conditional di usions, and the models obtained can successfully describe the shape relaxation of the scalar PDF from an initial double delta distribution to a Gaussian one. However, the mapping closure approach is not able to provide the rate at which the scalar evolves. The evolution rate has to be modeled. Therefore, the mapping closure approach is not closed. In this letter, we will address this problem.

He, Guo-Wei↗

NASA NTRS2014

Double Bright Band Observations with High-Resolution Vertically Pointing Radar, Lidar, and Profiles

On 11 May 2010, an elevated temperature inversion associated with an approaching warm front produced two melting layers simultaneously, which resulted in two distinct bright bands as viewed from the ER-2 Doppler radar system, a vertically pointing, coherent X band radar located in Greenbelt, MD. Due to the high temporal resolution of this radar system, an increase in altitude of the melting layer of approximately 1.2 km in the time span of 4 min was captured. The double bright band feature remained evident for approximately 17 min, until the lower atmosphere warmed enough to dissipate the lower melting layer. This case shows the relatively rapid evolution of freezing levels in response to an advancing warm front over a 2 h time period and the descent of an elevated warm air mass with time. Although observations of double bright bands are somewhat rare, the ability to identify this phenomenon is important for rainfall estimation from spaceborne sensors because algorithms employing the restriction of a radar bright band to a constant height, especially when sampling across frontal systems, will limit the ability to accurately estimate rainfall.

ER-2 Doppler radar↗

DOE OSTI2020

Floquet Cavity Electromagnonics

Hybrid magnonics has recently attracted intensive attention as a promising platform for coherent information processing. In spite of its rapid development, on-demand control over the interaction of magnons with other information carriers, in particular, microwave photons in electromagnonic systems, has been long missing, significantly limiting the potential broad applications of hybrid magnonics. Here, we show that, by introducing Floquet engineering into cavity electromagnonics, coherent control on the magnon-microwave photon coupling can be realized. Leveraging the periodic temporal modulation from a Floquet drive, our first-of-its-kind Floquet cavity electromagnonic system enables the manipulation of the interaction between hybridized cavity electromagnonic modes. Moreover, we have achieved a new coupling regime in such systems: the Floquet ultrastrong coupling, where the Floquet splitting is comparable with or even larger than the level spacing of the two interacting modes, beyond the conventional rotating-wave picture. As a result, our findings open up new directions for magnon-based coherent signal processing.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗