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Results for “Optical phonons”

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 505 records · Page 28
All sourcesNASA NTRSDOE OSTI
NASA NTRS1981

Intraband optical conductivity sigma/omega,T/ of Cu, Ag, and Au - Contribution from electron-electron scattering

The frequency and temperature dependence of the intraband optical conductivity of the noble metals Cu, Ag and Au is measured and contributions of electron-electron scattering are assessed. Optical measurements were performed at temperatures of 77, 295 and 425 K to obtain values of the Drude electron scattering rate with a linear dependence on temperature which may be attributed to electron-phonon scattering, and a quadratic dependence on photon energy, which is suggestive of electron-electron scattering but is a factor of two to three times greater than would be expected. Comparison of the optical data with dc electrical and thermal resistivity data which also show behavior attributed to electron-electron scattering reveals discrepancies of up to an order of magnitude. Other possible mechanisms for the frequency dependence, including absorptance, electron-surface plasmon interactions, a two-carrier model, and a structure dependence are considered, and it is concluded that the frequency dependence in the Drude scattering rates of the noble metals is not yet quantitatively understood

Parkins, G. R.↗
DOE OSTI2023

Ultrafast Switching of Interfacial Thermal Conductance

Dynamical control of thermal transport at the nanoscale provides a time-domain strategy for optimizing thermal management in nanoelectronics, magnetic devices, and thermoelectric devices. However, the rate of change available for thermal switches and regulators is limited to millisecond time scales, calling for a faster modulation speed. Here, in this work, time-resolved X-ray diffraction measurements and thermal transport modeling reveal an ultrafast modulation of the interfacial thermal conductance of an FeRh/MgO heterostructure as a result of a structural phase transition driven by optical excitation. Within 90 ps after optical excitation, the interfacial thermal conductance is reduced by a factor of 5 and lasts for a few nanoseconds, in comparison to the value at the equilibrium FeRh/MgO interface. The experimental results combined with thermal transport calculations suggest that the reduced interfacial thermal conductance results from enhanced phonon scattering at the interface where the lattice experiences transient in-plane biaxial stress due to the structural phase transition of FeRh. Our results suggest that optically driven phase transitions can be utilized for ultrafast nanoscale thermal switches for device application.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Narrow-band high-lying excitons with negative-mass electrons in monolayer WSe2

Monolayer transition-metal dichalcogenides (TMDCs) show a wealth of exciton physics. Here, we report the existence of a new excitonic species, the high-lying exciton (HX), in single-layer WSe 2 with an energy of ~3.4 eV, almost twice the band-edge A-exciton energy, with a linewidth as narrow as 5.8 meV. The HX is populated through momentum-selective optical excitation in the K-valleys and is identified in upconverted photoluminescence (UPL) in the UV spectral region. Strong electron-phonon coupling results in a cascaded phonon progression with equidistant peaks in the luminescence spectrum, resolvable to ninth order. Ab initio GW-BSE calculations with full electron-hole correlations explain HX formation and unmask the admixture of upper conduction-band states to this complex many-body excitation. These calculations suggest that the HX is comprised of electrons of negative mass. The coincidence of such high-lying excitonic species at around twice the energy of band-edge excitons rationalizes the excitonic quantum-interference phenomenon recently discovered in optical second-harmonic generation (SHG) and explains the efficient Auger-like annihilation of band-edge excitons.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Coherent helicity-dependent spin-phonon oscillations in the ferromagnetic van der Waals crystal CrI3

Abstract The discovery of two-dimensional systems hosting intrinsic magnetic order represents a seminal addition to the rich landscape of van der Waals materials. CrI 3 is an archetypal example, where the interdependence of structure and magnetism, along with strong light-matter interactions, provides a new platform to explore the optical control of magnetic and vibrational degrees of freedom at the nanoscale. However, the nature of magneto-structural coupling on its intrinsic ultrafast timescale remains a crucial open question. Here, we probe magnetic and vibrational dynamics in bulk CrI 3 using ultrafast optical spectroscopy, revealing spin-flip scattering-driven demagnetization and strong transient exchange-mediated interactions between lattice vibrations and spin oscillations. The latter yields a coherent spin-coupled phonon mode that is highly sensitive to the driving pulse’s helicity in the magnetically ordered phase. Our results elucidate the nature of ultrafast spin-lattice coupling in CrI 3 and highlight its potential for applications requiring high-speed control of magnetism at the nanoscale.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Optical and Plasmonic Properties of High-Electron-Density Epitaxial and Oxidative Controlled Titanium Nitride Thin Films

The present paper reports on the fabrication, detailed structural characterizations, and theoretical modeling of titanium nitride (TiN) and its isostructural oxide derivative, titanium oxynitride (TiNO) thin films that have excellent plasmonic properties and that also have the potential to overcome the limitation of noble metal and refractory metals. The TiNO films deposited at 700 °C in high vacuum conditions have the highest reflectance (R = ~ 95%), largest negative dielectric constant (ε 1 = –161), and maximal plasmonic figure of merit (FoM = –ε 1 /ε 2 ) of 1.2, followed by the 600 °C samples deposited in a vacuum (R = ~ 85%, ε 1 = –145, FoM = 0.8) and 700 °C–5 mTorr sample (R = ~ 82%, ε 1 = –8, FoM = 0.3). To corroborate our experimental observations, we calculated the phonon dispersions and Raman active modes of TiNO by using the virtual crystal approximation. From the experimental and theoretical studies, a multilayer optical model has been proposed for the TiN/TiNO epitaxial thin films for obtaining individual complex dielectric functions from which many other optical parameters can be calculated. The advantages of oxide derivatives of TiN are the continuation of similar free electron density as in TiN and the acquisition of additional features such as oxygen-dependent semiconductivity with a tunable bandgap.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Superconducting dome in ferroelectric-type materials from soft mode instability

Here we present a minimal theory of superconductivity enhancement in ferroelectric-type materials. Simple expressions for the optical mode responsible for the soft mode transition are assumed. A key role is played by the anharmonic phonon damping which is modulated by an external control parameter (electron doping or mechanical strain) causing the appearance of the soft mode. It is shown that the enhancement in the superconducting critical temperature T c upon approaching the ferroelectric transition from either side is due to the Stokes electron-phonon scattering processes promoted by strong phonon damping effects.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Nonlinear propagating modes beyond the phonons in fluorite-structured crystals

The vibrational energy of crystals is known to propagate in a fixed number of phonon branches allowed by symmetry. In the realm of nonlinear dynamics, however, additional nonlinear propagating modes are possible. Nonlinear propagating modes have unique properties that are important in many disciplines including optical communications, conducting polymers, biology, magnetism, and nuclear physics. Yet, despite the crucial importance of crystal lattice vibrations in fundamental and applied science, such additional propagating modes have not been observed in ordinary crystals. Here, we show that propagating modes exist beyond the phonons in fluorite-structured thoria, urania, and natural calcium fluoride using neutron scattering and first-principles calculations. These modes are observed at temperatures ranging from 5 K up to 1200 K, extend to frequencies 30–40% higher than the maximum phonon frequency, and travel at velocities comparable to or higher than the fastest phonon. The nonlinear origin of the modes is explained in part via perturbation theory, which approximately accounts for nonlinearity. Given that these modes are still clearly observed at 5 K, they are likely an inherent feature of the quantum ground state. The existence of these waves in three-dimensional crystals may have ramifications for material properties.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Continuous and Time-Domain Coherent Signal Conversion between Optical and Microwave Frequencies

A quantum network consisting of computational nodes connected by high-fidelity communication channels could expand information-processing capabilities significantly beyond those of classical networks. Superconducting qubits hold promise for scalable and high-fidelity quantum computation at microwave frequencies but must operate in an isolated cryogenic environment, obviating the potential for practical long-range communication. Quantum communication has, however, been demonstrated with optical photons. A fast efficient quantum-coherent interface between superconducting qubits and optical photons would provide a key resource for a large-scale quantum network or distributed quantum computer. Here, we describe the design and experimental operation of a device incorporating a silicon optomechanical nanobeam combined with an aluminum-nitride-based electromechanical transducer. We experimentally demonstrate classical continuous-wave operation of this device at room temperature with external conversion efficiencies of (2.5 +/- 0.4) x 10 -5 (microwave to optical) and (3.8 +/- 0.4) x 10 -5 (optical to microwave), corresponding to internal efficiencies of 2.4% and 3.7%, respectively. Finally, this device also has a larger bandwidth than previous efficient microwave-optical transducers, allowing us to operate in the time domain with 20-ns pulses.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Effect of CO{sub 2}-laser power density on the absorption coefficient of polycrystalline CVD diamonds

The effect of 1-s irradiation of an uncooled polycrystalline CVD diamond plate by a focused cw CO{sub 2} laser beam with a power density of 300 – 800 kW cm{sup −2} is investigated. The absorption coefficient of the sample at a power density of 800 kW cm{sup −2} is found to be 0.035 cm{sup −1} larger as compared with that at 300 kW cm{sup −2}, which is related to the temperature dependence of its phonon-induced absorption with a change in temperature from 44 to 100 °C. It is shown that polycrystalline diamond, in contrast to other optical materials, does not exhibit nonlinear (avalanche-like) rise in absorption at high CO{sub 2}-laser power densities, at least up to 800 kW cm{sup −2}. (paper)

36 MATERIALS SCIENCE↗
DOE OSTI2024

Efficient simulations of charge density waves in the transition metal Dichalcogenide TiSe 2

Charge density waves (CDWs) in transition metal dichalcogenides are the subject of growing scientific interest due to their rich interplay with exotic phases of matter and their potential technological applications. Here, using density functional theory with advanced meta-generalized gradient approximations (meta-GGAs) and linear response time-dependent density functional theory (TDDFT) with state-of-the-art exchange-correlation kernels, we investigate the electronic, vibrational, and optical properties in 1T-TiSe 2 with and without CDW. In both bulk and monolayer TiSe 2 , the electronic bands and phonon dispersions in either normal or CDW (semiconducting) phase are described well via meta-GGAs, which separate the valence and conduction bands just as HSE06 does but with significantly more computational feasibility. The experimentally observed humps of electron energy loss spectroscopy are successfully reproduced in TDDFT. Our work opens the door to simulating these complexities in CDW compounds from first principles by revealing meta-GGAs as an accurate low-cost alternative to HSE06.

Electronic properties and materials↗
DOE OSTI2026

Defect in diamond with millisecond-scale spin relaxation time at room temperature

Spin defects in diamond are promising platforms for quantum sensing. The longest electron spin relaxation times (T1) at room temperature for solid-state defects are observed in nitrogen vacancy centers in diamond, which can reach 6.67 ms [1], and substitutional nitrogen (“P1 centers”) in diamond, which exhibit a T1 of 2 ms [2]. No other solid-state defect has exhibited millisecond-scale spin relaxation times at room temperature thus far. Here, we characterize the spin properties of the WAR5 defect in diamond [3] with pulsed electron spin resonance. The observed T1 is one of the longest for solid-state spin defects: 0.97(27) ms at room temperature and 14.38(19) min at 4 K. The observed coherence time (T2) is 246(7) µs, which can be extended to 6.49(34) ms at 4 K with dynamical decoupling. Finally, we demonstrate optical spin polarization with a range of wavelengths from 405 nm to 500 nm and propose potential zero-phonon line candidates.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Ab initio evaluation of the electronic and optical properties of V B C B defect in wurtzite boron nitride as promising single-photon emitter

Single-photon emitters (SPEs) in the near-infrared (NIR) range with sharp and intense zero-phonon lines (ZPLs) of emission are critical for quantum communications. Certain local defects in wide-bandgap semiconductors create isolated occupied and unoccupied states within the bandgap of the host semiconductor and thus exhibit sharp ZPLs of emission. We designed and studied a defect in the wurtzite boron nitride as a potential SPE. It consists of a boron vacancy and a carbon atom substituting another boron atom (V B C B defect). The density of states is obtained within the GW method to identify favorable local defect states that may dominate optical transitions. The dielectric function and oscillator strength of the V B C B defect are obtained using the Bethe-Salpeter equation method to identify the optical excitations of the V B C B defect, from which we conclude that the defect could be a source of NIR emission with a narrow bright ZPL peak, thus an efficient SPE.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Dipole-Phonon Quantum Logic with Trapped Polar Molecular Ions

The interaction between the electric dipole moment of a trapped molecular ion and the phonon modes of the confined Coulomb crystal couples the orientation of the molecule to its motion. We consider the practical feasibility of harnessing this interaction to initialize, process, and read out quantum information encoded in molecular ion qubits without ever optically illuminating the molecules. We present two schemes wherein a molecular ion can be entangled with a cotrapped atomic ion qubit, providing, among other things, a means for molecular state preparation and measurement. Here, we also show that virtual phonon exchange can significantly boost the range of the intermolecular dipole-dipole interaction, allowing strong coupling between widely separated molecular ion qubits.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Paratellurite Nanowires as a Versatile Material for THz Phonon Polaritons

Polaritons, i.e., hybrid quasi-particles of light and matter resonances, have been extensively investigated due to their potential to enhance light-matter interactions. Although polaritonic applications thrive in the mid-infrared range, their extension to the terahertz (THz) range remains limited. Here, we present paratellurite (α-TeO 2 ) nanowires, a versatile material acting as a platform for different types of phonon polaritons. Utilizing synchrotron infrared nanospectroscopy from 10 to 24 THz, we uncover the polaritonic properties of α-TeO 2 nanowires, showcasing their dual functionality as both a Fabry-Pérot cavity and a waveguide for surface phonon polaritons. Furthermore, near-field measurements with a free-electron laser as a THz source reveal a localized optical contrast down to 5.5 THz, an indication of hyperbolic bands. In conclusion, our findings complement the repertoire of polaritonic materials, with significant implications for advancing THz technologies.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Plasmon coupling in topological insulator multilayers

Topological insulators (TIs) house two-dimensional Dirac plasmons on their surfaces. In TI thin films, plasmons on the top and bottom surfaces couple electrostatically, giving rise to an acoustic and an optical plasmon mode. By extension, a superlattice comprising TI layers and trivially-insulating layers could house multiple complex plasmon modes which could be used to create a new type of Dirac metamaterial. In this paper, we synthesize TI superlattices, fabricate them into stripe arrays, characterize their optical and plasmonic properties, and model the samples using transfer matrices. Furthermore, we excite plasmon modes that couple to the phonons in the superlattice, resulting in hybrid plasmon phonon polaritons. These modes are modeled using an analytical Fano resonance model and the extracted resonant positions are reproduced by transfer matrix modeling. We also excite an epsilon-near-zero mode in the top dielectric material (Bi 0.5 In 0.5 ) 2 Se 3 . Understanding the behavior of the polariton modes in this complex system will lend insight into the many-body interaction in low-dimensional systems.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Extended anharmonic collapse of phonon dispersions in SnS and SnSe

The lattice dynamics and high-temperature structural transition in SnS and SnSe are investigated via inelastic neutron scattering, high-resolution Raman spectroscopy and anharmonic first-principles simulations. We uncover a spectacular, extreme softening and reconstruction of an entire manifold of low-energy acoustic and optic branches across a structural transition, reflecting strong directionality in bonding strength and anharmonicity. Further, our results solve a prior controversy by revealing the soft-mode mechanism of the phase transition that impacts thermal transport and thermoelectric efficiency. Our simulations of anharmonic phonon renormalization go beyond low-order perturbation theory and capture these striking effects, showing that the large phonon shifts directly affect the thermal conductivity by altering both the phonon scattering phase space and the group velocities. These results provide a detailed microscopic understanding of phase stability and thermal transport in technologically important materials, providing further insights on ways to control phonon propagation in thermoelectrics, photovoltaics, and other materials requiring thermal management.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Ab initio electron-two-phonon scattering in GaAs from next-to-leading order perturbation theory

Electron-phonon (e–ph) interactions are usually treated in the lowest order of perturbation theory. Here we derive next-to-leading order e–ph interactions, and compute from first principles the associated electron-two-phonon (2ph) scattering rates. The derivations involve Matsubara sums of two-loop Feynman diagrams, and the numerical calculations are challenging as they involve Brillouin zone integrals over two crystal momenta and depend critically on the intermediate state lifetimes. Using Monte Carlo integration together with a self-consistent update of the intermediate state lifetimes, we compute and converge the 2ph scattering rates, and analyze their energy and temperature dependence. We apply our method to GaAs, a weakly polar semiconductor with dominant optical-mode long-range e–ph interactions. We find that the 2ph scattering rates are as large as nearly half the value of the one-phonon rates, and that including the 2ph processes is necessary to accurately predict the electron mobility in GaAs from first principles.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Atomically Resolved Acoustic Dynamics Coupled with Magnetic Order in a Van der Waals Antiferromagnet

Magnetoelastic coupling in van der Waals (vdW) magnetic materials enables a unique interplay between the spin and lattice degrees of freedom. Characterizing the elastic responses with atomic and femtosecond resolution across the magnetic transition is essential for guiding the design of magnetically tunable actuators and strain-mediated spintronic devices. Here, ultrafast X-ray diffraction employed at a free-electron laser reveals that the atomic displacements, wave vectors, and dispersion relations of acoustic phonon modes in a vdW antiferromagnet FePS3 are coupled with the magnetic order, by tracking both in-plane and out-of-plane Bragg peaks upon optical excitation across the Néel temperature (TN). One transverse mode shows that a quasi-out-of-plane atomic displacement undergoes a significant directional change across TN. Its quasi-in-plane wave vector is derived by comparing the measured sound velocity and the first-principles calculations. The other transverse mode is an interlayer shear acoustic mode whose amplitude is strongly enhanced in the antiferromagnetic phase, exhibiting eight times stronger amplitude than the longitudinal acoustic mode below TN. The atomically resolved characterization of acoustic phonon dynamics that couple with magnetic ordering opens opportunities for harnessing unique magnetoelastic coupling in vdW magnets on ultrafast timescales.

coherent acoustic phonons↗