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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 559 records · Page 31

X-ray dichroism as a probe of orbital quenching and unquenching induced by optically excited Jahn-Teller modes

The use of soft-X-ray spectroscopy to probe changes in the ground-state due to vibronic excitations is studied. The changes in L-edge X-ray absorption on divalent cobalt in the presence of a vibrating Jahn-Teller distortion are calculated. For linear dichroism, a strong dependence on the distortion is obtained reflecting the change in the local quadrupole moment due to the changes in the xy versus yz/zx hole densities during the oscillation. Here, in the presence of a magnetic moment, significant variations in the circular dichroic signal are obtained related to the quenching and unquenching of the orbital angular momentum.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Dynamic near-field optical interaction between oscillating nanomechanical structures

Near-field optical techniques exploit light-matter interactions at small length scales for mechanical sensing and actuation of nanomechanical structures. Here, we study the optical interaction between two mechanical oscillators—a plasmonic nanofocusing probe-tip supported by a low frequency cantilever, and a high frequency nanomechanical resonator—and leverage their interaction for local detection of mechanical vibrations. The plasmonic nanofocusing probe provides a confined optical source to enhance the interaction between the two oscillators. Dynamic perturbation of the optical cavity between the probe-tip and the resonator leads to nonlinear modulation of the scattered light intensity at the sum and difference of their frequencies. This double-frequency demodulation scheme is explored to suppress unwanted background and to detect mechanical vibrations with a minimum detectable displacement sensitivity of 0.45pm/Hz 1/2 , which is limited by shot noise and electrical noise. We explore the demodulation scheme for imaging the bending vibration mode shape of the resonator with a lateral spatial resolution of 20nm. We also demonstrate the time-resolved aspect of the local optical interaction by recording the ring-down vibrations of the resonator at frequencies of up to 129MHz. The near-field optical technique is promising for studying dynamic mechanical processes in individual nanostructures.

36 MATERIALS SCIENCE↗

The hemisphere-cylinder at an angle of attack

The investigation of the flow over a cylinder with a hemispherical nose at an angle of attack is presented. Experiments were conducted in a 6 ft x 6 ft low-turbulence tunnel. The focus of this research is the separated region as well as the evaluation and testing of a new diagnostic tool, a fiber-optic laser-Doppler probe. A two-fold contribution is offered. On one hand, pressure distributions are provided along a fine grid over the body. On the other hand, a feasibility study is presented on the use of a fiber-optic LDV probe which can obtain data from inside the model.

Telionis, D. P.↗

Covert laser remote sensing and vibrometry

Designs of single-beam laser vibrometry systems and methods. For example, a method for detecting vibrations of a target based on optical sensing is provided to include operating a laser to produce a laser probe beam at a laser frequency and modulated at a modulation frequency onto a target; collecting light at or near the laser to collect light from the target while the target is being illuminated by the laser probe beam through an optical receiver aperture; using a narrow-band optical filter centered at the laser frequency to filter light collected from the optical receiver aperture to transmit light at the laser frequency while blocking light at other frequencies; using an optical detector to convert filtered light from the narrow-band optical filter to produce a receiver electrical signal; using a lock-in amplifier to detect and amplify the receiver electrical signal at the modulation frequency while rejecting signal components at other frequencies to produce an amplified receiver electrical signal; processing the amplified receiver electrical signal to extract information on vibrations of the target carried by reflected laser probe beam in the collected light; and controlling optical power of the laser probe beam at the target to follow optical power of background illumination at the target.

Maleki, Lutfollah↗

Time and frequency resolved transient-absorption and stimulated-Raman signals of stochastic light

Covariance spectroscopy signals based on the transmission of broadband stochastic probe light undergoing a nonlinear optical process with matter are studied. The resulting signal depends on intensity correlation functions of the probe pulse. Application is made to transient absorption and stimulated Raman signals, where an ultraviolet pump and a delayed stochastically modulated infrared or optical Raman probe are used for monitoring vibrational excitations. We show that the stochastic properties of light can be exploited to circumvent the limitations on the joint temporal and spectral resolution of the signal. We study a model system with a time-dependent frequency and show that the dynamical information can be fully extracted from the covariance signal. Finally, this information is heavily suppressed upon averaging of noisy signals and practically inaccessible in conventional stimulated Raman measurements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Observation of light-driven band structure via multiband high-harmonic spectroscopy

Intense light–matter interactions have revolutionized our ability to probe and manipulate quantum systems at sub-femtosecond timescales, opening routes to the all-optical control of electronic currents in solids at petahertz rates. Such control typically requires electric-field amplitudes in the range of almost volts per angstrom, when the voltage drop across a lattice site becomes comparable to the characteristic bandgap energies. In this regime, intense light–matter interaction induces notable modifications to the electronic and optical properties, dramatically modifying the crystal band structure. Yet, identifying and characterizing such modifications remain an outstanding problem. As the oscillating electric field changes within the driving field’s cycle, does the band structure follow and how can it be defined? Here we address this fundamental question, proposing all-optical spectroscopy to probe the laser-induced closing of the bandgap between adjacent conduction bands. Our work reveals the link between nonlinear light–matter interactions in strongly driven crystals and the sub-cycle modifications in their effective band structure.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Kramers–Kronig relation in attosecond transient absorption spectroscopy

The Kramers–Kronig relation (KKR) has a wide range of applications in extreme ultraviolet (XUV) and x-ray spectroscopy. However, the validity of KKR for many of these applications has not been systematically studied, while it is known to require careful attention in nonlinear and pump–probe experiments in optical domain spectroscopy. Here, we study the validity of KKR in XUV attosecond transient absorption spectroscopy pump–probe measurements both experimentally and theoretically using argon Fano resonances as a case study. Experiments are enabled by a phase-resolved method dubbed Complex Attosecond Transient-absorption Spectroscopy (CATS). Although the estimations based on the rotating-wave approximation suggest that KKR violation could be expected in the studied case, our results validate KKR and provide a solid basis for its application in a broad range of attosecond spectroscopy experiments.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Ab initio phonon coupling and optical response of hot electrons in plasmonic metals

Ultrafast laser measurements probe the nonequilibrium dynamics of excited electrons in metals with increasing temporal resolution. Electronic structure calculations can provide a detailed microscopic understanding of hot electron dynamics, but a parameter-free description of pump-probe measurements has not yet been possible, despite intensive research, because of the phenomenological treatment of electron-phonon interactions. As such, we present ab initio predictions of the electron-temperature dependent heat capacities and electron-phonon coupling coefficients of plasmonic metals. We find substantial differences from free-electron and semiempirical estimates, especially in noble metals above transient electron temperatures of 2000 K, because of the previously neglected strong dependence of electron-phonon matrix elements on electron energy. We also present first-principles calculations of the electron-temperature dependent dielectric response of hot electrons in plasmonic metals, including direct interband and phonon-assisted intraband transitions, facilitating complete theoretical predictions of the time-resolved optical probe signatures in ultrafast laser experiments.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

In Situ UV–vis Quantification of Chlorobasicity in Binary Molten Chlorides

Optical basicity measurements provide a basis for determining the relative chlorobasicity of a given molten salt composition. This study uses Bi3+ as a spectroscopic probe to investigate optical basicity across three binary molten chloride systems (LiCl-KCl, MgCl2–KCl, and ZnCl2–KCl) through in situ UV–vis spectroscopy measurements of the 1S0→3P1 transition. LiCl-KCl systems exhibit the highest optical basicity with minimal compositional dependence, while both divalent systems show stronger, yet nonlinear, dependence that is reminiscent of acid–base titration curves. The influence of cation electronegativity and polarizing power (Li+ < Mg2+ < Zn2+) directly reflects the basicity curves, with ZnCl2–KCl displaying the steepest gradients and lowest basicity values. Nonlinear dependencies in divalent systems indicate formation of chloride-bridged network structures with coordination states dictated by the amount of KCl in a salt composition, which was further investigated and validated by molecular dynamics simulations of polymeric structures formed in ZnCl2 and MgCl2-based salts using machine learning force fields. The temperature dependence of chlorobasicity in terms of optical basicity was investigated, and a loose, positive correlation between the two was revealed. These findings establish Bi3+ as a sensitive probe for understanding electronic environments in molten chloride systems and provide insights for predicting the chemical behavior of molten salts for use in high-temperature environments.

Buttice, Kailee [Department of Nuclear Engineering↗

Perfect Coulomb drag and exciton transport in an excitonic insulator

Strongly coupled electron-hole bilayers can host quantum states of interlayer excitons, such as high-temperature exciton condensates at zero magnetic field. This state is predicted to feature perfect Coulomb drag, where a current in one layer is accompanied by an equal but opposite current in the other. We used an optical technique to probe the electrical transport of correlated electron-hole bilayers based on MoSe2/hBN/WSe2 heterostructures. We observed perfect Coulomb drag in the excitonic insulator phase at low temperatures; the counterflow resistance of interlayer excitons remained finite. These results indicate the formation of an exciton gas that does not condense into a superfluid. Our work demonstrates that dynamic optical spectroscopy provides a powerful tool for probing exciton transport behavior in correlated electron-hole fluids.

Qi, Ruishi↗

Identification of spin, valley and moiré quasi-angular momentum of interlayer excitons

Moiré superlattices provide a powerful way to engineer properties of electrons and excitons in two-dimensional van der Waals heterostructures. The moir\'e effect can be especially strong for interlayer excitons, where electrons and holes reside in different layers and can be addressed separately. In particular, it was recently proposed that the moiré superlattice potential not only localizes interlayer exciton states at different superlattice positions, but also hosts an emerging moiré quasi-angular momentum (QAM) that periodically switches the optical selection rules for interlayer excitons at different moiré sites. Here we report the observation of multiple interlayer exciton states coexisting in a WSe 2 /WS 2 moiré superlattice and unambiguously determine their spin, valley, and moiré QAM through novel resonant optical pump-probe spectroscopy and photoluminescence excitation spectroscopy. We demonstrate that interlayer excitons localized at different moiré sites can exhibit opposite optical selection rules due to the spatially-varying moiré QAM. Finally, our observation reveals new opportunities to engineer interlayer exciton states and valley physics with moiré superlattices for optoelectronic and valleytronic applications.

74 ATOMIC AND MOLECULAR PHYSICS↗

Optical conductivity of the type-II Weyl semimetal TaIrTe 4

TaIrTe4 is an example of a candidate Weyl type-II semimetal with a minimal possible number of Weyl nodes. Four nodes are reported to exist a single plane in k-space. The existence of a conical dispersion linked to Weyl nodes has yet to be shown experimentally. Here we use optical spectroscopy as a probe of the band structure on a low-energy scale. Studying optical conductivity allows us to probe intraband and interband transitions with zero momentum. In TaIrTe 4 , we observe a narrow Drude contribution and an interband conductivity that may be consistent with a tilted linear band dispersion up to 40 meV. The interband conductivity allows us to establish the effective parameters of the conical dispersion; effective velocity v = 1.1 · 10 4 m/s and tilt γ = 0.37. The transport data, Seebeck and Hall coefficients, are qualitatively consistent with conical features in the band structure. Quantitative disagreement may be linked to the multiband nature of TaIrTe 4 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Anomalous behavior of nonequilibrium excitations in U O 2

Ultrafast optical pump-probe studies of uranium dioxide (UO 2 ) under pressure were performed in order to better understand the material's response to ionizing radiation. Photoexcitation generates oscillations in the time-resolved reflectivity at two distinct GHz-scale frequencies. The higher-frequency mode is attributed to a coherent longitudinal acoustic mode. The lower-frequency mode does not correspond to any known excitation under equilibrium conditions. The frequency and lifetime of the low-frequency mode are studied as a function of pressure. Abrupt changes in the pressure-dependent slopes of these attributes are observed at ~10 GPa, which correlates with an electronic transition in UO 2 . Variation of probe wavelength reveals that the low- k dispersion of the low-frequency mode does not fit into either an optical or acoustic framework. Rather, we propose that this mode is related to the dynamical magnetic structure of UO 2 . As a result, the implications of these results help account for the anomalously small volume of damage known to be caused by ionizing radiation in UO 2 ; we propose that the existence of the low-frequency mode enhances the material's transient thermal conductivity, while its long lifetime lengthens the timescale over which energy is dissipated. Both mechanisms enhance damage recovery.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

A multi-probe thermophoretic soot sampling system for high-pressure diffusion flames

Optical diagnostics and physical probing of the soot processes in high pressure combustion pose challenges that are not faced in atmospheric flames. One of the preferred methods of studying soot in atmospheric flames is in situ thermophoretic sampling followed by transmission electron microscopy imaging and analysis for soot sizing and morphology. The application of this method of sampling to high pressures has been held back by various operational and mechanical problems. In this work, we describe a rotating disk multi-probe thermophoretic soot sampling system, driven by a microstepping stepper motor, fitted into a high-pressure chamber capable of producing sooting laminar diffusion flames up to 100 atm. Innovative aspects of the sampling system design include an easy and precise control of the sampling time down to 2.6 ms, avoidance of the drawbacks of the pneumatic drivers used in conventional thermophoretic sampling systems, and the capability to collect ten consecutive samples in a single experimental run. Proof of principle experiments were performed using this system in a laminar diffusion flame of methane, and primary soot diameter distributions at various pressures up to 10 atm were determined. High-speed images of the flame during thermophoretic sampling were recorded to assess the influence of probe intrusion on the flow field of the flame.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

A Fluorescence Spectrum Analyzer Based on a Fiber-Optic Y-Circulator

We consider a method of probe analysis employing fiber-optic a composite Y-circulator design for the implementation of laser-induced fluorescence (LIF) spectroscopy diagnostics. The proposed principle of the LIF analyzer is based on spatially separated directed optical beams of excitation and fluorescence radiations. Conditions of the effective Y-circulator operation as a passive fiber-optic switch are determined. Experimental investigation of the switched radiation losses is performed. An example of using the proposed analyzer for LIF diagnostics of biological media is presented.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Attosecond Optical Orientation

Circularly polarized light offers opportunities to probe symmetry-dependent properties of matter such as chirality and spin. Circular-dichroic measurements typically require further intrinsic or extrinsic breaking of symmetry by, e.g., enantiomeric excess, orientation, magnetic fields, or direction-sensitive detectors. Here we introduce circular-dichroic attosecond transient absorption spectroscopy by leveraging the angular momentum of two circularly polarized pulses, both pump and probe, in an isotropic medium, optically orienting the angular momentum of excited states on an attosecond timescale. We investigate a circular-dichroic measurement of the attosecond transient absorption of He Rydberg states. By limiting the allowed pathways via dipole selection rules for co- and counterrotating circularly polarized near-infrared and extreme ultraviolet (XUV) pulses, different spectral reshapings of the XUV transient absorption due to the AC Stark effect are observed. Furthermore, paired with time-dependent Schrödinger equation calculations, the results show the role of selection and propensity rules and open up new opportunities to study coupling pathways of excited states as well as spin-dependent dynamics in atoms and beyond via attosecond optical orientation.

Angular momentum of light↗

Disentangling electronic, lattice, and spin dynamics in the chiral helimagnet Cr 1/3 NbS 2

We investigate the static and ultrafast magneto-optical response of the hexagonal chiral helimagnet Cr 1/3 NbS 2 above and below the helimagnetic ordering temperature. The presence of a magnetic easy plane contained within the crystallographic $ab$-plane is confirmed, while degenerate optical pump-probe experiments reveal significant differences in the dynamic between the parent, NbS 2 , and Cr-intercalated compounds. Time-resolved magneto-optical Kerr effect measurements show a two-step demagnetization process, where an initial, subpicosecond relaxation and subsequent buildup (τ > 50ps) in the demagnetization dynamic scale similarly with increasing pump fluence. Despite theoretical evidence for partial gapping of the minority spin channel, suggestive of possible half-metallicity in Cr 1/3 NbS 2 , such a long demagnetization dynamic likely results from spin-lattice relaxation as opposed to minority state blocking. However, comparison of the two-step demagnetization process in Cr 1/3 NbS 2 with other 3d intercalated transition metal dichalcogenides reveals a behavior that is unexpected from conventional spin-lattice relaxation, and may be attributed to the complicated interaction of local moments with itinerant electrons in this material system.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Investigation of the effect of a power feed vacuum gap in solid liner experiments at 1 MA

We present an experimental study of plasma initiation of a solid metal liner at the 1 MA level. In contrast to previous work, we introduce a vacuum gap at one of the liner connections to the power feed to investigate how this affects plasma initiation and to infer how this may affect the symmetry of the liner in compression experiments. We observed that the vacuum gap causes non-uniform plasma initiation both azimuthally and axially in liners, diagnosed by gated optical imaging. Using magnetic field probes external to the liner, we also determined that the optical emission is strongly linked to the current distribution in the liner. The apparent persistent of azimuthal non-uniformities may have implications for fusion-scale liner experiments.

Bott-Suzuki, S. C.↗