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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
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Ultrafast Carrier and Lattice Dynamics in Plasmonic Nanocrystalline Copper Sulfide Films

Excited carrier dynamics in plasmonic nanostructures determines many important optical properties such as nonlinear optical response and photocatalytic activity. Here it is shown that mesoscopic plasmonic covellite nanocrystals with low free-carrier concentration exhibit a much faster carrier relaxation than in traditional plasmonic materials. A nonequilibrium hot-carrier population thermalizes within first 20 fs after photoexcitation. A decreased thermalization time in nanocrystals compared to a bulk covellite is consistent with the reduced Coulomb screening in ultrathin films. The subsequent relaxation of thermalized, equilibrium electron gas is faster than in traditional plasmonic metals due to the lower carrier concentration and agrees well with that in a bulk covellite showing no evidence of quantum confinement or hot-hole trapping at the surface states. The excitation of coherent optical phonon modes in a covellite is also demonstrated, revealing coherent lattice dynamics in plasmonic materials, which until now was mainly limited to dielectrics, semiconductors, and semimetals. These findings show advantages of this new mesoscopic plasmonic material for active control of optical processes.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Modeling the electron cyclotron emission radiation signature from suprathermal electrons in a tokamak

An Electron Cyclotron Emission (ECE) modeling code has been developed to model ECE radiation with an arbitrary electron momentum distribution, a small oblique angle, both ordinary (O-mode) and extraordinary polarizations (X-mode), and multiple cyclotron frequency harmonics. The emission and absorption coefficients are calculated using the Poynting theorem from the cold plasma dispersion and the electron–microwave interaction from the full anti-Hermitian tensor. The modeling shows several ECE radiation signatures that can be used to diagnose the population of suprathermal electrons in a tokamak. First, in an n = 2 X-mode (X2) optically thick plasma and oblique ECE view, the modeling shows that only suprathermal electrons, which reside in a finite region of the velocity and space domains, can effectively generate cyclotron emissions to the ECE receiver. The code also finds that the O1 mode is sensitive to suprathermal electrons of both a high v ⊥ and v || , while the X2 mode is dominantly sensitive to suprathermal electrons of a high v ⊥ . Finally, the modeling shows that an oblique ECE system with both X/O polarization and a broad frequency coverage can be used to effectively yield information of the suprathermal electron population in a tokamak.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
NASA NTRS2003

Parametric optics with whispering-gallery modes

We propose to fabricate a dielectric cavity sustaining high-Q whispering gallery modes from a periodically poled material possessing a quadratic nonlinearity to achieve an efficient interaction among the modes. We show that the periodical poling allows for compensation of both the material and the cavity dispersions that prohibits the nonlinear interaction otherwise. Such a cavity might be a basics element of a family of efficient nonlinear devices operating at a broad range of optical wavelengths.

Maleki, Lute↗
DOE OSTI2020

Low-frequency Raman spectrum of 2D layered perovskites: Local atomistic motion or superlattice modes?

We report the low-frequency Raman spectrum (ω = 10 cm -1 –150 cm -1 ) of a wide variety of alkylammonium iodide based 2D lead halide perovskites (2D LHPs) as a function of A-site cation (MA = methylammonium and FA = formamidinium), octahedral layer thickness (n = 2–4), organic spacer chain length (butyl-, pentyl-, hexyl-), and sample temperature (T = 77 K–293 K). Using density functional theory calculations under the harmonic approximation for n = 2 BA:MAPbI, we assign several longitudinal/transverse optical phonon modes between 30 cm -1 and 100 cm -1 , the eigen displacements of which are analogous to that observed previously for octahedral twists/distortions in bulk MAPbI. Additionally, we propose an alternative assignment for low-frequency modes below this band (<30 cm -1 ) as zone-folded longitudinal acoustic phonons corresponding to the periodicity of the entire layered structure. Furthermore, we compare measured spectra to predictions of the Rytov elastic continuum model for zone-folded dispersion in layered structures. Our results are consistent across the various 2D LHPs studied herein, with energetic shifts of optical phonons corresponding to microscopic structural differences between materials and energetic shifts of acoustic phonons according to changes in the periodicity and elastic properties of the perovskite/organic subphases. This study highlights the importance of both the local atomic order and the superlattice structure on the vibrational properties of layered 2D materials.

2D materials↗
DOE OSTI2023

The Role of Optical Phonon Confinement in the Infrared Dielectric Response of III–V Superlattices

Polar dielectrics are key materials of interest for infrared (IR) nanophotonic applications due to their ability to host phonon-polaritons that allow for low-loss, subdiffractional control of light. The properties of phonon-polaritons are limited by the characteristics of optical phonons, which are nominally fixed for most “bulk” materials. Superlattices composed of alternating atomically thin materials offer control over crystal anisotropy through changes in composition, optical phonon confinement, and the emergence of new modes. In particular, the modified optical phonons in superlattices offer the potential for so-called crystalline hybrids whose IR properties cannot be described as a simple mixture of the bulk constituents. To date, however, studies have primarily focused on identifying the presence of new or modified optical phonon modes rather than assessing their impact on the IR response. Here, this study focuses on assessing the impact of confined optical phonon modes on the hybrid IR dielectric function in superlattices of GaSb and AlSb. Using a combination of first principles theory, Raman, FTIR, and spectroscopic ellipsometry, the hybrid dielectric function is found to track the confinement of optical phonons, leading to optical phonon spectral shifts of up to 20 cm -1 . These results provide an alternative pathway toward designer IR optical materials.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Superconductivity from the Slater mode: Application to KTaO 3 heterostructures

Superconductivity has been observed for the 2D electron gas (2DEG) at the interface of KTaO 3 with other oxides, with a transition temperature about an order of magnitude higher than its 3⁢𝑑 cousin SrTiO 3 . Here, the superconducting transition temperature is strongly dependent on the orientation of the interface. Motivated by this observation, we study pairing due to the exchange of the soft transverse optic phonon mode characteristic of quantum paraelectrics and use the resulting theory to comment on the nature of superconductivity of this 2DEG. We find (1) an orientation dependence consistent with experiment along with an anisotropic gap function, but (2) a BCS coupling constant that is smaller than needed and so must be augmented by contributions from other phonons to be consistent with the observed values of 𝑇 𝑐 .

Norman, M. R. [Argonne National Laboratory (ANL), ↗
DOE OSTI2014

Experimental setup for investigation of nanoclusters at cryogenic temperatures by electron spin resonance and optical spectroscopies

We present the design and performance of an experimental setup for simultaneous electron spin resonance (ESR) and optical studies of nanoclusters with stabilized free radicals at cryogenic temperatures. A gas mixture of impurities and helium after passing through a RF discharge for dissociation of molecules is directed onto the surface of superfluid helium to form the nanoclusters of impurities. A specially designed ESR cavity operated in the TE{sub 011} mode allows optical access to the sample. The cavity is incorporated into a homemade insert which is placed inside a variable temperature insert of a Janis {sup 4}He cryostat. The temperature range for sample investigation is 1.25–300 K. A Bruker EPR 300E and Andor 500i optical spectrograph incorporated with a Newton EMCCD camera are used for ESR and optical registration, respectively. The current experimental system makes it possible to study the ESR and optical spectra of impurity-helium condensates simultaneously. The setup allows a broad range of research at low temperatures including optically detected magnetic resonance, studies of chemical processes of the active species produced by photolysis in solid matrices, and investigations of nanoclusters produced by laser ablation in superfluid helium.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2018

Electronic, Vibrational, and Elastic Properties of Zn{sub 2}SeTe Crystals with Antihalcopirite Structure

Using the capabilities of the CRYSTAL14 code, the parameters of an equilibrium crystal lattice are obtained and the electronic and vibrational structures of a new chalcopyrite-like Zn{sub 2}SeTe crystal are studied. The energy band structure, long-wave vibrational frequencies at the point Г, and elastic moduli are calculated. The dependence of the contributions from the vibrations of individual atoms to the vibrational modes of a crystal caused by filling the cationic or anionic sublattices in the chalcopyrite structure is established.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

III-Nitride Nanowire Lasers

In recent years there has been a tremendous interest in nanoscale optoelectronic devices. Among these devices are semiconductor nanowires whose diameters range from 10-100 nm. To date, nanowires have been grown using many semiconducting material systems and have been utilized as light emitting diodes, photodetectors, and solar cells. Nanowires possess a relatively large index contrast relative to their dielectric environment and can be used as lasers. A key gure of merit that allows for nanowire lasing is the relatively high optical con nement factor. In this work, I discuss the optical characterization of 3 types of III-nitride nanowire laser devices. Two devices were designed to reduce the number of lasing modes to achieve singlemode operation. The third device implements low-group velocity mode lasing with a photonic crystal constructed of an array of nanowires. Single-mode operation is necessary in any application where high beam quality and single frequency operation is required. III-Nitride nanowire lasers typically operate in a combined multi-longitudinal and multi-transverse mode state. Two schemes are introduced here for controlling the optical modes and achieving single-mode op eration. The rst method involves reducing the diameter of individual nanowires to the cut-o condition, where only one optical mode propagates in the wire. The second method employs distributed feedback (DFB) to achieve single-mode lasing by placing individual GaN nanowires onto substrates with etched gratings. The nanowire-grating substrate acted as a distributed feedback mirror producing single mode operation at 370 nm with a mode suppression ratio (MSR) of 17 dB. The usage of lasers for solid state lighting has the potential to further reduce U.S. lighting energy usage through an increase in emitter e ciency. Advances in nanowire fabrication, speci cally a two-step top-down approach, have allowed for the demonstration of a multi-color array of lasers on a single chip that emit vertically. By tuning the geometrical properties of the individual lasers across the array, each individual nanowire laser produced a di erent emission wavelength yielding a near continuum of laser wavelengths. I successfully fabricated an array of emitters spanning a bandwidth of 60 nm on a single chip. This was achieved in the blue-violet using III-nitride photonic crystal nanowire lasers.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2014

Current driven magnetization dynamics of a self-polarised synthetic ferrimagnet

Spin torque driven excitations in spin valves and tunnel junctions are often investigated for a two magnetic layer system for which a polarizer (fixed magnetization) and a free layer can be distinguished. In the search for improved microwave properties and to understand the role of different coupling mechanisms between the magnetic layers, here, the excitation spectrum of an exchange coupled two layer synthetic ferrimagnet (SyF) system is investigated numerically with spin momentum transfer acting on both layers simultaneously. This self-polarised two layer system does not contain an external polarizer, and excitation of coupled modes arises due to the mutual spin transfer torque and the Ruderman-Kittel-Kasuya-Yosida interlayer exchange coupling. The current-field state diagrams of static and dynamic states are reported as a function of the interlayer exchange coupling strength. The numerically determined critical boundaries are well reproduced by an analytical stability analysis. The dynamic steady states reveal an optic-like mode at low magnetic fields, which becomes progressively acoustic-like for increased magnetic fields and currents. The frequency of these modes can be tuned by the film thickness and the strength of the interlayer exchange interaction. The results presented here will provide an important guide for designing spin torque oscillators that exploit the dynamic coupling between layers and, furthermore, they will provide a basis to test analytical models of spin torque driven coupled excitations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Mode Purity of Electron Cyclotron Waves after Their Passage through the Peripheral Plasma in the Large Helical Device

Plasma heating and current drive with Electron Cyclotron Waves (ECWs) require precise control over the polarization state of ECWs to ensure that the entire input power is deposited where intended. However, due to the magnetic shear in the peripheral plasma, the polarization state can change. This effect is particularly pronounced in the Large Helical Device (LHD), where the magnetic field is sheared strongly. Here, we present a new code PARADE (PAraxial RAy DEscription) that can simulate the evolution of the polarization state along the beam propagation without resorting to full-wave modeling. We apply PARADE to the LHD plasma and simulate the evolution of the beam transverse structure, including the local amplitudes of the two electromagnetic eigenmodes. Here, the results surpass those yielded by the code LHDGauss used in the past. Based on these new results, we discuss how to improve the mode purity of ECWs by controlling the initial polarization state. A remarkable improvement is predicted numerically.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2016

Anharmonicity in light scattering by optical phonons in GaAs 1- x Bi x

We present a Raman spectroscopic study of GaAs 1-x Bi x epilayers grown by molecular beam epitaxy. We have investigated the anharmonic effect on the GaAs-like longitudinal optical phonon mode (LO' GaAs ) of GaAs 1-x Bi x for different Bi concentrations at various temperatures. The results are analyzed in terms of the anharmonic damping effect induced by thermal and compositional disorder. We have observed that the anharmonicity increases with Bi concentration in GaAs 1-x Bi x as evident from the increase in the anharmonicity constants. Additionally, the anharmonic lifetime of the optical phonon decreases with increasing Bi concentration in GaAs 1-x Bi x .

36 MATERIALS SCIENCE↗
DOE OSTI2024

Phonon modes and electron–phonon coupling at the FeSe/SrTiO 3 interface

The remarkable increase in superconducting transition temperature (T c ) observed at the interface of one-unit-cell FeSe films on SrTiO3 substrates (1 uc FeSe/STO) has attracted considerable research into the interface effects. Although this high T c is thought to be associated with electron-phonon coupling (EPC), the microscopic coupling mechanism and its role in the superconductivity remain elusive. Here we use momentum-selective high-resolution electron energy loss spectroscopy to atomically resolve the phonons at the FeSe/STO interface. We uncover new optical phonon modes, coupling strongly with electrons, in the energy range of 75-99 meV. These modes are characterized by out-of-plane vibrations of oxygen atoms in the interfacial double-TiO x layer and the apical oxygens in STO. Our results also demonstrate that the EPC strength and superconducting gap of 1 uc FeSe/STO are closely related to the interlayer spacing between FeSe and the TiOx terminated STO. These findings shed light on the microscopic origin of the interfacial EPC and provide insights into achieving large and consistent T c enhancement in FeSe/STO and potentially other superconducting systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Phonovoltaic. III. Electron-phonon coupling and figure of merit of graphene:BN

The phonovoltaic cell harvests optical phonons like a photovoltaic harvests photons, that is, a nonequilibrium (hot) population of optical phonons (at temperature $T$ p,O ) more energetic than the band gap produces electron-hole pairs in a $p$-$n$ junction, which separates these pairs to produce power. A phonovoltaic material requires an optical phonon mode more energetic than its band gap and much more energetic than the thermal energy ($E$ p,O $ΔE$ e,g ≫ $k$ B $T$ ) , which relaxes by generating electrons and power (at rate $\dot{γ}$ e-p ) rather than acoustic phonons and heat (at rate $\dot{γ}$ p-p ). Graphene (h-C) is the most promising material candidate: when its band gap is tuned to its optical phonon energy without greatly reducing the electron-phonon (e-p) coupling, it reaches a substantial figure of merit [ $Z$ pV = $ΔE$ e,g $\dot{γ}$ e-p / $E$ p,O ($\dot{γ}$ e-p + $\dot{γ}$ p-p ) ≈ 0.8 ] . A simple tight-binding (TB) model presented here predicts that lifting the sublattice symmetry of graphene in order to open a band gap proscribes the e-p interaction at the band edge, such that $\dot{γ}$ e-p → 0 as $ΔE$ e,g → $E$ p,O . However, ab initio (DFT-LDA) simulations of layered h-C/BN and substitutional h-C:BN reveal that the e-p coupling remains substantial in these asymmetric crystals. Indeed, h-C:BN achieves a high figure of merit ( $Z$ pV ≈ 0.6 ) . At 300 K and for a Carnot limit of 0.5 ( $T$ p,O = 600 K ) , a h-C:BN phonovoltaic can reach an efficiency of η pV ≈ 0.2 , double the thermoelectric efficiency ( $ZT$ ≈ 1) under similar conditions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Exciton dynamics in a site-controlled quantum dot coupled to a photonic crystal cavity

Exciton and cavity mode (CM) dynamics in site-controlled pyramidal quantum dots (QDs), integrated with linear photonic crystal membrane cavities, are investigated for a range of temperatures and photo-excitation power levels. The absence of spurious multi-excitonic effects, normally observed in similar structures based on self-assembled QDs, permits the observation of effects intrinsic to two-level systems embedded in a solid state matrix and interacting with optical cavity modes. The coupled exciton and CM dynamics follow the same trend, indicating that the CM is fed only by the exciton transition. The Purcell reduction of the QD and CM decay times is reproduced well by a theoretical model that includes exciton linewidth broadening and temperature dependent non-radiative processes, from which we extract a Purcell factor of 17 ± 5. For excitation powers above QD saturation, we show the influence of quantum wire barrier states at short delay time, and demonstrate the absence of multiexcitonic background emission.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Energy relaxation dynamics in a nodal-line semimetal

Here we study the temperature relaxation dynamics of nodal-line semimetals after a sudden excitation in the presence of acoustic and optical phonon modes. We find that the nodal line constrains the electron momenta in scattering processes, and as a result, the temperature relaxation due to acoustic phonons is exponential as a function of time. However, depending on initial conditions, other functional forms are possible. In typical pump-probe experiments, the temperature relaxation is linear due to acoustic phonons with rates that vary as ~n 1/2 with density. The temperature relaxation due to optical phonons is also linear with rates ~n -1/2 or ~n .

36 MATERIALS SCIENCE↗
DOE OSTI2013

Theoretical analysis of phase locking in an array of globally coupled lasers

A model of an array of globally coupled fibre lasers, with the same fraction of the total output beam power injected into each laser, is considered. Phase self-locking of the laser array makes it possible to increase the brightness of the total output beam without any devices for controlling the phases of output beams, which significantly complicate the laser system. The spread of the laser optical lengths is several hundreds of wavelengths (or even more); within the theory of hollow cavities, this spread should lead to a fast decrease in the total power with an increase in the number of lasers. The presence of the active medium may reduce this drop to a great extent due to the self-tuning of the laser array radiation wavelength to a value providing a maximum gain for the array lasing mode. The optical length of each element is assumed to be random. The increase in the phase-locking efficiency due to the gain saturation is explained based on the probabilistic approach. An iterative procedure is developed to find the array output power in the presence of steady-state phase locking. Calculations for different values of small-signal gain and the output-power fraction spent on global coupling are performed. It is shown that, when this fraction amounts to ∼20 % – 30 %, phase locking of up to 20 fibre lasers can be implemented with an efficiency as high as 70 %. (control of laser radiation parameters)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗