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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 307 records · Page 17

Probing nanoparticle substrate interactions with synchrotron infrared nanospectroscopy: Coupling gold nanorod Fabry-Pérot resonances with SiO 2 and $h$-BN phonons

Spectroscopic interrogation of materials in the midinfrared with nanometer spatial resolution is inherently difficult due to the long wavelengths involved, reduced detector efficiencies, and limited availability of spectrally bright, coherent light sources. Technological advances are driving techniques that overcome these challenges, enabling material characterization in this relatively unexplored spectral regime. Synchrotron infrared nanospectroscopy (SINS) is an imaging technique that provides local sample information of nanoscale target specimens in an experimental energy window between 330 and 5000 cm -1 . Here, using SINS, we analyzed a series of individual gold nanorods patterned on a SiO 2 substrate and on a flake of hexagonal boron nitride. The SINS spectra reveal interactions between the nanorod photonic Fabry-Pérot resonances and the surface phonon polaritons of each substrate, which are characterized as avoided crossings. A coupled oscillator model of the hybrid system provides a deeper understanding of the coupling and provides a theoretical framework for future exploration.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Insights into the laser-assisted photoelectric effect from solid-state surfaces

Photoemission from a solid surface provides a wealth of information about its electronic structure and dynamic evolution. Ultrafast pump-probe experiments offer real-time access to photon-surface interactions and the resulting electron dynamics. Here, we present a femtosecond time-resolved photoelectron spectroscopy study of laser-assisted photoemission (LAPE) from two different metal surfaces, tungsten and platinum. Utilizing synchronized IR laser and x-ray pulses, photoelectron sideband generation up to the sixth order is observed. A significant material-dependent variation of the LAPE response has not been predicted by previous theoretical models, to the best of our knowledge. The observed phenomena are semiquantitatively reproduced by considering distinct dynamic dielectric responses of the two materials. In conclusion, these findings provide a deeper understanding of the LAPE process and insights into the dynamic interplay between optical laser fields and metal surfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Near-Field Radiative Heat Transfer Eigenmodes

The near-field electromagnetic interaction between nanoscale objects produces enhanced radiative heat transfer that can greatly surpass the limits established by far-field blackbody radiation. Here, we present a theoretical framework to describe the temporal dynamics of the radiative heat transfer in ensembles of nanostructures, which is based on the use of an eigenmode expansion of the equations that govern this process. Using this formalism, we identify the fundamental principles that determine the thermalization of collections of nanostructures, revealing general but often unintuitive dynamics. Overall, our results provide an elegant and precise approach to efficiently analyze the temporal dynamics of the near-field radiative heat transfer in systems containing a large number of nanoparticles.

74 ATOMIC AND MOLECULAR PHYSICS↗

Synthesis of inter‐lanthanide sesquioxides LnLn'O 3 by polymeric steric entrapment

Lanthanide oxides are well known in the fields of optical, electronic, and magnetic materials. Even so, there are many application spaces yet to be explored. Previous modeling of inter-lanthanide sesquioxides, in which the compound contains two lanthanide cations, predicts the lowest level energy structure as a function of chemistry, which this work seeks to verify. Three materials of interest, ErLuO 3 , LaLuO 3 , and SmLuO 3 , were synthesized for the first time by the polymeric steric entrapment (PSE) method. X-ray diffraction confirms the stable state predictions of ErLuO 3 and SmLuO 3 forming a bixbyite type structure and LaLuO 3 forming a perovskite type structure. This work demonstrates PSE as a viable and reliable route toward the synthesis of these unique materials.

36 MATERIALS SCIENCE↗

Attosecond probing and control of charge migration in carbon-chain molecule

In quantum mechanics, when an electron is quickly ripped off from a molecule, a superposition of new eigenstates of the cation creates an electron wave packet that governs the charge flow inside, which has been called charge migration (CM). Experimentally, extracting such dynamics at its natural (attosecond) timescale is quite difficult. We report the first such experiment in a linear carbon-chain molecule, butadiyne (C 4 H 2 ), via high-harmonic spectroscopy (HHS). By employing advanced theoretical and computational tools, we showed that the wave packet and the CM of a single molecule are reconstructed from the harmonic spectra for each fixed-in-space angle of the molecule. For this one-dimensional molecule, we calculate the center of charge $\langle$ x $\rangle$ ( t ) to obtain v cm , to quantify the migration speed and how it depends on the orientation angle. The findings also uncover how the electron dynamics at the first few tens to hundreds of attoseconds depends on molecular structure. The method can be extended to other molecules where the HHS technique can be employed.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Building epsilon near zero materials from layered uniaxial metamaterials

Recently, there has been an explosion of activity in the fields of optics and photonics with the advent of fabrication techniques which enable the design of metamaterials which possess properties not encountered in the natural world. In this work, we are concerned with zero permittivity materials and a new scheme to design metamaterials for which all components of the dielectric tensor are approximately zero. Our approach involves the alternate layering of many, very thin, slices of two constituent metamaterials, a uniaxial layered medium and a uniaxial nanowire array. With a simple optimization strategy we demonstrate a candidate configuration which very nearly satisfies our design goal of zero permittivity.

Gray, Stephen K. [Argonne National Laboratory (ANL↗

Monolithic Spatial Heterodyne Raman Spectrometers (mSHRS): Toward highly miniature chemical sensors for deployment on moving platforms (Final Report, Phase I)

This report covers phase 1 (year 1) of the mSHRS project. Our ultimate long-term goal is to develop highly miniature Raman analyzers, known as spatial heterodyne Raman spectrometers (SHRS), that are deployable as in-situ chemical sensors on moving platforms. During Phase I (FY19/20) funding, our team focused our efforts solely on the key innovation needed toward realizing that goal: the development of the monolithic interferometer comprising the beam splitter and gratings with the appropriate design parameters and tolerances to enable Raman interferometry. We successfully developed and characterized the performance of the first monolithic SHRS devices including a monolithic version that incorporates field-widened optics. Our solid-state design approach integrated all optical components as a single monolithic unit for maintaining precise optical alignment during sensor operation, a requirement for operating in a vibration prone environment. This project has two principle activities: (1) Design and fabricate monolithic SHRS devices (i.e. monolithic device task) and (2) characterize the mSHRS devices in terms of performance (i.e. the Monolithic SHRS characterization task).

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Synthetic Aperture Radar Height of Focus

Synthetic Aperture Radar (SAR) projects a 3-D scene’s reflectivity into a 2-D image. In doing so, it generally focusses the image to a surface, usually a ground plane. Consequently, scatterers above or below the focal/ground plane typically exhibit some degree of distortion manifesting as a geometric distortion and misfocusing or smearing. Limits to acceptable misfocusing define a Height of Focus (HOF), analogous to Depth of Field in optical systems. This may be exacerbated by the radar’s flightpath during the synthetic aperture data collection. It might also be exploited for target height estimation and offer insight to other height estimation techniques.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Growth and characterization of ferromagnetic Ga 2 O 3 :(Cr, Mn)

The goal of this Exploratory Express project was to explore the possibility of tunable ferromagnetism in Mn or Cr incorporated epitaxial Ga 2 O 3 films. Tunability of magnetic properties can enable novel applications in spintronics, quantum computing, and magnetism-based logics by allowing control of magnetism down to the nanoscale. Carriers (electrons or holes) mediated ferromagnetic ordering in semiconductor can lead to tunable ferromagnetism by leveraging the tunability of carrier density with doping level, gate electric field, or optical pumping of the carriers. The magnetic ions (Cr or Mn) in Ga 2 O 3 act as localized spin centers which can potentially be magnetically coupled through conduction electrons to enable ferromagnetic ordering. Here we investigated tunable ferromagnetism in beta Ga 2 O 3 semiconductor host with various n-doping levels by incorporating 2.4 atomic percent Mn or Cr. The R&D approach involved growth of epitaxial Ga 2 O 3 film on sapphire or Ga 2 O 3 substrate, implantation of Mn or Cr ions, annealing of the samples post implantation, and magnetic measurements. We studied magnetic behavior of Mn:Ga 2 O 3 as a function of different n-doping levels and various annealing temperatures. The vibrating sample magnetometry (VSM) measurement exhibited strong ferromagnetic signals from the annealed Mn:Ga 2 O 3 sample with n-doping level of 5E19 cm -3 . This ferromagnetic behavior disappears from Mn:Ga 2 O 3 when the n-doping level is reduced to 5E16 cm -3 . Although these results are to be further verified by other measurement schemes due to the observation of background ferromagnetism from the growth substrate, these results indicate the possibility of tunable ferromagnetism in Mn:Ga 2 O 3 mediated by conduction electrons.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Analysis of Near-Field Magnetic Responses on ZrTe 5 through Cryogenic Magneto-THz Nano-Imaging

One manifestation of light-Weyl fermion interaction is the emergence of chiral magnetic effects under magnetic fields. Probing real space magnetic responses at terahertz (THz) scales is challenging but highly desired, as the local responses are less affected by the topologically trivial inhomogeneity that is ubiquitous in spatially averaged measurements. Here, we implement a cryogenic THz microscopy instrument under a magnetic field environment—a task only recently achieved. We explore the technical approach of this system and characterize the magnetic field’s influence on our AFM operation by statistical noise analysis. We find evidence for local near-field spatial variations in the topological semimetal ZrTe 5 up to a 5-Tesla magnetic field and obtain near-field THz spectra to discuss their implications for future studies on the chiral magnetic effect.

36 MATERIALS SCIENCE↗

Volumetric carrier injection in InGaN quantum well light emitting diodes

InGaN/GaN quantum well (QW) light emitting diodes (LEDs) are essential components of solid-state lighting and displays. However, the efficiency of long wavelength (green to red) devices is inferior to that of blue LEDs. To a large degree, this occurs because the equilibration of injected holes between multiple QWs of the active region is hindered by GaN quantum confinement and polarization barriers. This drawback could be overcome by volumetric hole injection into all QWs through semipolar QWs present on the facets of V-defects that form at threading dislocations in polar GaN-based structures. In this work, we have tested the viability of this injection mechanism and studied its properties by time-resolved and near-field spectroscopy techniques. Here, we have found that indeed the hole injection via the V-defects does take place, the mechanism is fast, and the hole spread from the V-defect is substantial, making this type of injection feasible for efficient long wavelength GaN LEDs.

InGaN/GaN quantum wells↗

Efficient Measurement of Length Distribution of 1D Nanoparticles in Solution via Optical Polarimetry

The efficient measurement of the length distribution of nanotubes, nanowires, and other one-dimensional (1D) nanoparticles in solution is important to enable their incorporation into materials and devices and to optimize their processing for properties of interest, such as thermal/electrical conductivity or mechanical strength, in suspensions and composites. We report an electric-field (E-field)-assisted optical-polarimetry technique to measure the length distribution of ensembles of high-aspect-ratio particles in dilute suspension. The degree of alignment of polarizable 1D particles suspended in a fluid under Brownian motion explicitly depends on the E-field strength and the particle length. We show that it is possible to extract the length distribution of 1D nanoparticles suspended in an insulating fluid by applying a range of E-fields and using optical polarimetry to measure the corresponding alignment order parameter. Notably, the method is relatively insensitive to the diameter of the 1D particles, which can be poorly known or vary within a sample. The technique is validated with silver nanowires and carbon nanotubes of known lengths, as well as polymer-depletion-length-separated single-wall carbon nanotube samples with length distributions independently measured with analytical ultracentrifugation. Finally, we demonstrate the ability of the optical-polarimetry technique to quantify changes in the length distribution of ultranarrow, sub-nanometer-diameter single-wall carbon nanotubes under different types and durations of ultrasonication. Within its range of applicability (polarizable 1D nanoparticles in the 0.5 to 15 μm length range, constrained by the voltage stability of the media and the suspended particles), the E-field-assisted optical-polarimetry method is a particularly efficient and accurate method to measure the length distribution of nanowires and nanotubes in suspension.

1D nanoparticles↗

Characterization of a modified printed optical particle spectrometer for high-frequency and high-precision laboratory and field measurements

Abstract. The printed optical particle spectrometer (POPS) is a lightweight, low-cost instrument for measurements of aerosol number concentrations and size distributions. This work reports on modifications of the Handix Scientific commercial version of the POPS to facilitate its use in multi-instrument aerosol sampling systems. The flow system is modified by replacing the internal pump with a needle valve and a vacuum pump. The instrument is integrated into closed-flow systems by routing the sheath flow from filtered inlet air. A high-precision multichannel analyzer (MCA) card is added to sample the analog pulse signal. The MCA card is polled at 10 Hz frequency using an external data acquisition system and improves upon the count-rate limitation associated with the POPS internal data acquisition system. The times required to change the concentration between 90 % and 10 % and vice versa for a step change in concentration were measured to be 0.17 and 0.41 s at a flow rate of 5 cm3 s−1. This yields a sampling frequency of ∼ 1–2 Hz, below which the amplitude of measured fluctuations is captured with > 70 % efficiency. The modified POPS was integrated into the dual tandem differential mobility analyzer system to explore the coalescence of dimer particles. Results show that the pulse-height response increases upon dimer coalescence. The magnitude of the increase is broadly consistent with the change in light-scattering amplitude predicted by the T-matrix method. It is anticipated that this modified version of the POPS will extend the utilization of the technique for a range of field and laboratory applications.

54 ENVIRONMENTAL SCIENCES↗

Two-dimensional Thomson scattering measurements of misaligned electron density and temperature gradients and associated Biermann battery produced fields

We present optical Thomson scattering measurements of electron density and temperature in high Mach number laser-driven blast waves in homogeneous gases. Taylor–Sedov blast waves are launched in nitrogen (N2) or helium (He) at pressures between 0.4 mTorr and 10 Torr by ablating a solid plastic target with a high energy laser pulse (10 J, 1012 W/cm2). Experiments are performed at high repetition rate (1 Hz), which allows one-dimensional and two-dimensional Thomson scattering measurements over an area of several cm2 by automatically translating the scattering volume between shots. Electron temperature and density in the blast wave fronts were seen to increase with increasing background gas pressure. Measured electron density and temperature gradients were used to calculate ∂B/∂t∝∇Te×∇ne. The experimentally measured ∂B/∂t showed agreement with the magnetic field probe (B-dot) measurements, revealing that magnetic fields are generated in the observed blast waves via the Biermann battery effect. The results are compared to numerical three-dimensional collisional magnetohydrodynamic simulations performed with FLASH, and are discussed in the context of spontaneous magnetic field generation via the Biermann battery effect.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Ultrafast temporal phase-resolved nonlinear optical spectroscopy in the molecular frame

In an ultrafast nonlinear optical interaction, the electric field of the emitted nonlinear signal provides direct access to the induced nonlinear transient polarization or transient currents and thus carries signatures of ultrafast dynamics in a medium. Measurement of the electric field of such signals offers sensitive observables to track ultrafast electron dynamics in various systems. In this work, we resolve the real-time phase of the electric field of a femtosecond third-order nonlinear optical signal in the molecular frame. The electric field emitted from impulsively pre-aligned gas-phase molecules at room temperature, in a degenerate four-wave mixing scheme, is measured using a spectral interferometry technique. The nonlinear signal is measured around a rotational revival to extract its molecular-frame angle dependence from pump-probe time-delay scans. By comparing these measurements for two linear molecules, carbon dioxide and nitrogen, we show that the measured second-order phase parameter (temporal chirp) of the signal is sensitive to the valence electronic symmetry of the molecules, whereas the amplitude of the signal does not show such sensitivity. We compare measurements to theoretical calculations of the chirp observable in the molecular frame. This work is an important step towards using electric field measurements in nonlinear optical spectroscopy to study ultrafast dynamics of electronically excited molecules in the molecular frame.

47 OTHER INSTRUMENTATION↗

Optical-pump–terahertz-probe spectroscopy in high magnetic fields with kHz single-shot detection

We demonstrate optical pump–THz probe (OPTP) spectroscopy with a variable external magnetic field (0–9 T), in which the time-dependent THz signal is measured by echelon-based single-shot detection at a repetition rate of 1 kHz. The method reduces data acquisition times by more than an order of magnitude compared to conventional electro-optic sampling using a scanning delay stage. The approach illustrates the wide applicability of the single-shot measurement approach to non-equilibrium systems that are studied through OPTP spectroscopy, especially in cases where parameters such as magnetic field strength (B) or other experimental parameters are varied. We demonstrate the capabilities of our measurement by performing cyclotron resonance experiments in bulk silicon, where we observe B-field-dependent carrier relaxation and distinct relaxation rates for different carrier types. We use a pair of economical linear array detectors to measure 500 time points on each shot, offering an equivalent performance to camera-based detection with possibilities for higher repetition rates.

Instruments & Instrumentation↗