Search NASA⌕ Search

SEARCH · Search NASA

Results for “Phonon scattering”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 307 records · Page 17
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Phonon-engineered extreme thermal conductivity materials

Materials with ultrahigh or low thermal conductivity are desirable for many technological applications, such as thermal management of electronic and photonic devices, heat exchangers, energy converters and thermal insulation. Recent advances in simulation tools (first principles, the atomistic Green’s function and molecular dynamics) and experimental techniques (pump–probe techniques and microfabricated platforms) have led to new insights on phonon transport and scattering in materials and the discovery of new thermal materials, and are enabling the engineering of phonons towards desired thermal properties. Here, we review recent discoveries of both inorganic and organic materials with ultrahigh and low thermal conductivity, highlighting heat-conduction physics, strategies used to change thermal conductivity, and future directions to achieve extreme thermal conductivities in solid-state materials.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Effects of anisotropy and disorder on the superconducting properties of niobium

We report results for the superconducting transition temperature and anisotropic energy gap for pure niobium based on Eliashberg’s equations and electron and phonon band structures computed from density functional theory. The electronic band structure is used to construct the Fermi surface and calculate the Fermi velocity at each point on the Fermi surface. The phonon bands are in excellent agreement with inelastic neutron scattering data. The corresponding phonon density of states and electron–phonon coupling define the electron–phonon spectral function, α 2 F(p, p'; ω), and the corresponding electron–phonon pairing interaction, which is the basis for computing the superconducting properties. The electron–phonon spectral function is in good agreement with existing tunneling spectroscopy data except for the spectral weight of the longitudinal phonon peak at ℏω LO = 23 meV. We obtain an electron–phonon coupling constant of λ = 1.057, renormalized Coulomb interaction μ* = 0.218, and transition temperature T c = 9.33 K. The corresponding strong-coupling gap at T = 0 is modestly enhanced, Δ 0 = 1.55 meV, compared to the weak-coupling BCS value $Δ^{\text {wc}}_{0}$ = 1.78 k B T c = 1.43 meV. The superconducting gap function exhibits substantial anisotropy on the Fermi surface. We analyze the distribution of gap anisotropy and compute the suppression of the superconducting transition temperature using a self-consistent T-matrix theory for quasiparticle-impurity scattering to describe niobium doped with non-magnetic impurities. We compare these results with experimental results on niobium SRF cavities doped with nitrogen impurities.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Thermal expansion and phonon anharmonicity of cuprite studied by inelastic neutron scattering and ab initio calculations

Inelastic neutron scattering measurements were performed with a time-of-flight chopper spectrometer to observe phonons in all parts of the Brillouin zone of a single crystal of cuprite Cu 2 O. We reduced the experimental data to phonon dispersions in the high-symmetry directions, and changes between 10 and 300 K are reported. In this paper, we show ab initio quasiharmonic (QH) and anharmonic (AH) calculations of phonon dispersions. We performed all AH calculations with a temperature-dependent effective potential method. Both QH and AH calculations account for the small negative thermal expansion of cuprite at low temperatures. However, the measured temperature-dependent phonon behavior was predicted more accurately with the AH calculations than the QH ones. Nevertheless, at 300 K, the cubic AH used in this paper did not entirely account for the experimental phonon dispersions in cuprite.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Phonon-mediated ultrafast dynamics in self-assembled monolayers of 4-mercaptobenzoic acid on gold

Non-equilibrium interactions between plasmonic metals and adsorbed molecules lie at the heart of emerging applications such as plasmonic photocatalysis and sensing, though the ultrafast charge and energy transfer mechanisms arising from these interactions are not well understood. Herein, we investigate the ultrafast dynamics of Au nano-islands tethered with a self-assembled monolayer (SAM) of electron-withdrawing 4-mercaptobenzoic acid (4MBA) molecules. Ultrafast UV-visible transient absorption spectroscopy following excitation of the interband transition in Au reveals three well-known, characteristic time constants that quantify electron–electron (el–el), electron–phonon (el–ph) and phonon–phonon (ph–ph) scattering lifetimes. When comparing the dynamics of bare Au and 4MBA-Au, we find that the el–ph and ph–ph scattering lifetimes are notably longer in 4MBA-Au. Density functional perturbation theory calculations ascribe the elongation in el–ph lifetimes in 4MBA-Au to the significant coupling of acoustic phonon modes of Au with certain molecular vibrations of 4MBA, leading to decreased spatial overlap between carrier electronic states and the acoustic modes. We speculate that the elongation of ph–ph scattering lifetimes in 4MBA-Au arises due to poor thermal conductivity of the SAM which disrupts efficient energy dissipation from Au to the environment, thus slowing down the thermalization of phonons. This work provides a glimpse into how molecular adsorbates modify the charge carrier and phonon dynamics of Au and sets the stage for further systematic exploration of plasmonic metal–molecule interactions.

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

Matryoshka phonon twinning in α-GaN

Understanding lattice dynamics is crucial for effective thermal management in electronic devices because phonons dominate thermal transport in most semiconductors. α -GaN has become a focus of interest as one of the most important third-generation power semiconductors, however, the knowledge on its phonon dynamics remains limited. Here we show a Matryoshka phonon dispersion of α -GaN with the complementary inelastic X-ray and neutron scattering techniques and the first-principles calculations. Such Matryoshka twinning throughout the basal plane of the reciprocal space is demonstrated to amplify the anharmonicity of the related phonons through creating abundant three-phonon scattering channels and cutting the lifetime of affected modes by more than 50%. Such phonon topology contributes to reducing the in-plane thermal transport, thus the anisotropic thermal conductivity of α -GaN. The results not only have implications for engineering the thermal performance of α -GaN, but also offer valuable insights on the role of anomalous phonon topology in thermal transport of other technically semiconductors.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2021

Generation and detection of 50 GHz surface acoustic waves by extreme ultraviolet pulses

In this work, we use femtosecond extreme ultraviolet pulses derived from a free electron laser to excite and probe surface acoustic waves (SAWs) on the (001) surface of single crystal SrTiO 3 . SAWs are generated by a pair of 39.9 nm pulses crossed at the sample with the crossing angle defining the SAW wavelength at 84 nm. Detection of SAWs is performed via diffraction of a time-delayed 13.3 nm probe pulse by SAW-induced surface ripples. Despite the low reflectivity of the sample in the extreme ultraviolet range, the reflection mode detection is found to be efficient because of an increase in the diffraction efficiency for shorter wavelengths. We describe a methodology for extracting the SAW attenuation in the presence of a thermal grating, which is based on measuring the decay of oscillations at twice the SAW frequency. The proposed approach can be used to study ultrahigh frequency SAWs in a broad range of materials and will bridge the wave vector gap in surface phonon spectroscopy between Brillouin scattering and He atom scattering.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Unraveling the Origin of Glassy Thermal Transport in Medium-Entropy Semiconductors: From Nanoscale Phase Segregation to Atomic-Scale Lattice Distortion

Thermoelectric (TE) materials can directly and reversibly convert heat into electricity, offering a promising pathway for reshaping the global energy landscape. The performance of thermoelectric materials is evaluated using the figure of merit, zT = S 2 σT/κ, which can be optimized by improving Seebeck coefficient (S) and electrical conductivity (σ) while suppressing the thermal conductivity (κ) at the operating temperature (T). Here, we introduce a medium-entropy metal chalcogenide that exhibits phonon-glass electron-crystal behavior. The conventional perspective hypothesizes that the suppression of thermal transport arises solely from disordered atomic occupation, which enhances alloy scattering mechanisms for phonon transport. However, emerging evidence suggests the presence of structural and chemical inhomogeneity at multiple length scales in entropy-engineered materials, a phenomenon that has rarely been investigated in detail.

Liu, Yukun [Northwestern Univ]↗
DOE OSTI2023

Probing Defects and Spin‐Phonon Coupling in CrSBr via Resonant Raman Scattering

Abstract Understanding the stability limitations and defect formation mechanisms in 2D magnets is essential for their utilization in spintronic and memory technologies. Here, defects in mono‐ to multilayer CrSBr are correlated with structural, vibrational, and magnetic properties. Resonant Raman scattering is used to reveal distinct vibrational defect signatures. In pristine CrSBr, it is shown that bromine atoms mediate vibrational interlayer coupling, allowing for distinguishing between surface and bulk defect modes. Environmental exposure is shown to cause drastic degradation in monolayers, with the formation of intralayer defects. This is in contrast to multilayers that predominantly show bromine surface defects. Through deliberate ion irradiation, the formation of defect modes is tuned: these are strongly polarized and resonantly enhanced, reflecting the quasi‐‐1D electronic character of CrSBr. Strikingly, pronounced signatures of spin‐phonon coupling of the intrinsic phonon modes and the ion beam‐induced defect modes are observed throughout the magnetic transition temperature. Overall, defect engineering of magnetic properties is possible, with resonant Raman spectroscopy serving as a direct fingerprint of magnetic phases and defects in CrSBr.

2D magnetic semiconductors↗
DOE OSTI2025

Experimental confirmation of first-principles thermal conductivity in Zirconium-doped ThO 2

The degradation of thermal conductivity in advanced nuclear fuels due to the accumulation of fission products and irradiation-induced defects is inevitable, and must be considered as part of safety and efficiency analyses of nuclear reactors. Here, this study examines the thermal conductivity of a zirconium-doped ThO 2 crystal, synthesized via the hydrothermal method using a spatial domain thermoreflectance technique. Zirconium is one of the soluble fission products in oxide fuels that can effectively scatter heat-carrying phonons in the crystalline lattice of fuel. Thus, thermal property measurements of zirconium-doped ThO 2 single crystals provide insights into the effects of substitutional zirconium doping, isolated from extrinsic factors such as grain boundary scattering. The experimental results are compared with first-principles calculations of the lattice thermal conductivity of ThO 2 , employing an iterative solution of the Peierls-Boltzmann transport equation. Additionally, the non-perturbative Green's function methodology is utilized to compute phonon-point defect scattering rates, accounting for local distortions around point defects, including mass difference changes, interatomic force constants, and structural relaxation. The congruence between the predicted results from first-principles calculations and the measured temperature-dependent thermal conductivity validates the computational methodology. Furthermore, the methodologies employed in this study enable systematic investigations of thermal conductivity reduction by fission products, potentially leading to the development of more accurate fuel performance codes.

36 - MATERIALS SCIENCE↗
DOE OSTI2026

Experimental Quantification of Spin–Phonon Coupling in Molecular Qubits Using Inelastic Neutron Scattering

Electronic spin superposition states enable nanoscale sensing through their sensitivity to the local environment, yet their sensitivity to vibrational motion also limits their coherence times. In molecular spin systems, chemical tunability and atomicscale resolution are accompanied by a dense, thermally accessible phonon spectrum that introduces efficient spin relaxation pathways. Despite extensive theoretical work, there is little experimental consensus on which vibrational energies dominate spin relaxation or how molecular structure controls spin−phonon coupling (SPC). We present a fully experimental method to quantify SPC coefficients by combining temperature-dependent vibrational spectra from inelastic neutron scattering with spin relaxation rates measured by electron paramagnetic resonance. We apply this framework to two model S = 1/2 systems, copper(II) phthalocyanine (CuPc) and copper(II) octaethylporphyrin (CuOEP). Two distinct relaxation regimes emerge: below 40 K, weakly coupled lattice modes below 50 cm −1 dominate, whereas above 40 K, optical phonons above ∼185 cm −1 become thermally populated and drive relaxation with SPC coefficients nearly 3 orders of magnitude larger. Structural distortions in CuOEP that break planar symmetry soften the crystal lattice and enhance anharmonic scattering but also raise the energy of stretching modes at the molecular core where the spins reside. This redistributes vibrational energy toward the molecular periphery and out of plane, ultimately reducing SPC relative to CuPc and enabling room-temperature spin coherence in CuOEP. Although our method does not provide mode-specific SPC coefficients, it quantifies contributions from distinct spectral regions and establishes a broadly applicable, fully experimental link between crystal structure, lattice dynamics, and spin relaxation.

Lohaus, Stefan H. [California Institute of Technol↗
DOE OSTI2025

Origin of Large Effective Phonon Magnetic Moments in Monolayer MoS 2

Recent helicity-resolved magneto-Raman spectroscopy measurement demonstrates large effective phonon magnetic moments of ~2.5 μ B in monolayer MoS 2 , highlighting resonant excitation of bright excitons as a feasible route to activate Γ-point circularly polarized phonons in transition metal dichalcogenides. However, a microscopic picture of this intriguing phenomenon remains lacking. In this work, we show that an orbital transition between the split conduction bands (Δ 0 = 4 meV) of MoS 2 couples to the doubly degenerate E" phonon mode (Ω 0 = 33 meV), forming two hybridized states. Our phononic and electronic Raman scattering measurements capture these two states: (i) one with predominantly phonon contribution in the helicity-switched channels and (ii) one with primarily orbital contribution in the helicity-conserved channels. An orbital-phonon coupling model successfully reproduces the large effective magnetic moments of the circularly polarized phonons and explains their thermodynamic properties. Strikingly, the Raman mode from the orbital transition is superimposed on a strong quasi-elastic scattering background, indicating the presence of spin fluctuations. As a result, the electrons excited to the conduction bands through the exciton exhibit paramagnetic behavior although MoS 2 is generally considered as a nonmagnetic material. By depositing nanometer-thickness nickel thin films on monolayer MoS 2 , we tune the electronic structure so that the A exciton perfectly overlaps with the 633 nm laser. The optimization of resonance excitation leads to pronounced tunability of the orbital-phonon hybridized states. Our results generalize the orbital-phonon coupling model of effective phonon magnetic moments to material systems beyond the paramagnets and magnets.

2D transition metal dichalcogenide↗
DOE OSTI2020

Strained bilayer WSe 2 with reduced exciton-phonon coupling

We explore excitonic absorption and emission in bilayer WSe 2 under tensile strain. We observe a redshift of 110 meV in the energy of the A exciton absorption peak (at the direct gap at the K point in the Brillouin zone) under 2.1% uniaxial tensile strain. In addition, under the same strain, the spectral linewidth of the A exciton at room temperature decreases by a factor of 2, from 70 to 36 meV. We show that this decrease is a result of suppression of phonon-mediated exciton scattering channels. This suppression is associated with the relative upshift under strain of the Q valley in the conduction band (involved in the indirect exciton emission), which is nearly degenerate with the K valley (involved in the A exciton). We analyze the strain-dependent absorption and photoluminescence spectra to determine the relative positions of these valleys and to infer intervalley scattering rates. Our model describes well the decrease and the distinct trends in the A exciton linewidth of monolayer and bilayer WSe 2 under strain. The findings show that strain can be used to tune, as well as to probe, the relative energies of band extrema and exciton scattering channels in two-dimensional semiconductors.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Single crystal growth and thermoelectric properties of Nowotny chimney-ladder compound Fe 2 Ge 3

Fe 2 Ge 3 with an incommensurate Nowotny chimney-ladder (NCL) structure is a promising material for thermoelectric applications due to its low thermal conductivity. Previous experimental studies on Fe 2 Ge 3 have mainly focused on polycrystalline samples, resulting in a limited understanding of the material's intrinsic thermoelectric properties and the underlying causes of its low thermal conductivity. Here we report the synthesis and thermoelectric properties of single crystalline Fe 2 Ge 3 . Millimeter-sized Fe 2 Ge 3 single crystals grown by the chemical vapor transport method enable the study of the intrinsic thermoelectric properties. The Seebeck coefficient of Fe 2 Ge 3 is negative and its magnitude increases linearly with temperature, showing a degenerate n-type semiconductor behavior. Analysis of the electrical resistivity and specific heat data indicates the existence of an Einstein mode with a characteristic temperature of about 60 K, suggesting the presence of low-energy optical phonons. Further, the thermal conductivity of Fe 2 Ge 3 along the c axis is as low as 1.9Wm -1 K -1 at 300 K and exhibits a nearly temperature-independent characteristic, which is distinct from the previous theoretical calculations with a stronger temperature dependence. The low thermal conductivity may be attributed to the scattering of acoustic phonons by low-energy optical modes and the presence of non-extended diffuson modes, as reported in another NCL compound, MnSi 1.74 . This study provides valuable insights into the electrical and thermal properties of Fe 2 Ge 3 , which can open up possibilities for future advances in thermoelectric applications.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Origin of ultralow phonon transport and strong anharmonicity in lead-free halide perovskites

All-inorganic lead-free halide double perovskites offer a promising avenue toward non-toxic, stable optoelectronic materials, properties that are missing in their prominent lead-containing counterparts. Their large thermopowers and high carrier mobilities also make them promising for thermoelectric applications. Here, in this work, we present a first-principles study of the lattice vibrations and thermal transport behaviors of Cs 2 SnI 6 and γ-CsSnI 3 , two prototypical compounds in this materials class. We show that conventional static zero temperature density functional theory (DFT) calculations severely underestimate the lattice thermal conductivities (κ l ) of these compounds, indicating the importance of dynamical effects. By calculating anharmonic renormalized phonon dispersions, we show that some optic phonons significantly harden with increasing temperature (T), which reduces the scattering of heat carrying phonons and enhances calculated κ l values when compared with standard zero temperature DFT. Furthermore, we demonstrate that coherence contributions to κ l , arising from wave like phonon tunneling, are important in both compounds. Overall, calculated κ l with temperature-dependent interatomic force constants, built from particle and coherence contributions, are in good agreement with available measured data, for both magnitude and temperature dependence. Large anharmonicity combined with low phonon group velocities yield ultralow values, with room temperature values of 0.26 W/m-K and 0.72 W/m-K predicted for Cs 2 SnI 6 and γ-CsSnI 3 , respectively. We further show that the lattice dynamics of these compounds are highly anharmonic, largely mediated by rotation of the SnI6 octahedra and localized modes originating from Cs rattling motion. These thermal characteristics combined with their previously computed excellent electronic properties make these perovskites promising candidates for optoelectronic and room temperature thermoelectric applications.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Sound attenuation in the hyperhoneycomb Kitaev spin liquid

In recent years, it has been shown that the phonon dynamics may serve as an indirect probe of fractionalization of spin degrees of freedom. Furthermore we propose that the sound attenuation measurements allows for the characterization and identification of the Kitaev quantum spin liquid on the hyperhoneycomb lattice, which is particularly interesting since the strong Kitaev interaction was observed in the the hyperhoneycomb magnet β–Li 2 IrO 3 . To this end we consider the low-temperature scattering between acoustic phonons and gapless Majorana fermions with nodal-line band structure. Here, we find that the sound attenuation has a characteristic angular dependence, which is explicitly shown for the high-symmetry planes at temperatures below the flux energy gap.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Excitons in two-dimensional metal-halide perovskites

Georgia Tech School of Chemistry and Biochemistry Special Summer Seminar Series, Prof Carlos Silva; While polarons --- charges bound to a lattice deformation induced by electron-phonon coupling --- are primary photoexcitations at room temperature in bulk metal-halide hybrid organic-inorganic perovskites (HOIP), excitons --- Coulomb-bound electron-hole pairs --- are the stable quasi-particles in their two-dimensional (2D) analogues. Here we address the fundamental question: are polaronic effects consequential for excitons in 2D-HIOPs? Based on our recent work, we argue that polaronic effects are manifested intrinsically in the exciton spectral structure, which is comprised of multiple non-degenerate resonances with constant inter-peak energy spacing. We highlight measurements of population and dephasing dynamics that point to the apparently deterministic role of polaronic effects in excitonic properties. We contend that an interplay of long-range and short-range exciton-lattice couplings give rise to exciton polarons, a character that fundamentally establishes their effective mass and radius, and consequently, their quantum dynamics. Given this complexity, a fundamentally far-reaching issue is how Coulomb-mediated many-body interactions---elastic scattering such as excitation-induced dephasing, inelastic exciton bimolecular scattering, and multi-exciton binding---depend upon the specific exciton-lattice coupling within the structured excitation lineshape. We measure the intrinsic and density-dependent exciton dephasing rates of the multiple excitons and their dependence on temperature by means of two-dimensional coherent excitation spectroscopy. We find that diverse excitons display distinct intrinsic dephasing rates mediated by phonon scattering involving different effective phonons, and contrasting rates of exciton-exciton elastic scattering. These findings establish specifically the consequence of distinct lattice dressing on exciton many-body quantum dynamics, which critically define fundamental optical properties that underpin photonics and quantum optoelectronics.

solar cells, metal-halide perovskites, excitons, p↗
DOE OSTI2025

Spontaneously formed phonon frequency combs in van der Waals solid CrGeTe 3 and CrSiTe 3

Optical phonon engineering through nonlinear effects has been utilized in ultrafast control of material properties. However, nonlinear optical phonons typically exhibit rapid decay due to strong mode-mode couplings, limiting their effectiveness in temperature or frequency sensitive applications. Here we report the observation of long-lived nonlinear optical phonons through the spontaneous formation of phonon frequency combs in the van der Waals material CrXTe 3 (X=Ge, Si) using high-resolution Raman scattering. Unlike conventional optical phonons, the highest A g mode in CrGeTe 3 splits into equidistant, sharp peaks forming a frequency comb that persists for hundreds of oscillations and survives up to 200K. These modes correspond to localized oscillations of Ge 2 Te 6 clusters, isolated from Cr hexagons, behaving as independent quantum oscillators. Introducing a cubic nonlinear term to the harmonic oscillator model, we simulate the phonon time evolution and successfully replicate the observed comb structure. Similar frequency comb behavior is observed in CrSiTe 3 , demonstrating the generalizability of this phenomenon. Our findings demonstrate that Raman scattering effectively probes high-frequency nonlinear phonon modes, offering insight into the generation of long-lived, tunable phonon frequency combs with potential applications in ultrafast material control and phonon-based technologies.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Phonon confinement and interface lattice dynamics of ultrathin high- k rare earth sesquioxide films: the case of Eu 2 O 3 on YSZ(001)

The spatial confinement of atoms at surfaces and interfaces significantly alters the lattice dynamics of thin films, heterostructures and multilayers. Ultrathin films with high dielectric constants (high-k) are of paramount interest for applications as gate layers in current and future integrated circuits. Here we report a lattice dynamics study of high-k Eu 2 O 3 films with thicknesses of 21.3, 2.2, 1.3, and 0.8 nm deposited on YSZ(001). The Eu-partial phonon density of states (PDOS), obtained from nuclear inelastic scattering, exhibits broadening of the phonon peaks accompanied by up to a four-fold enhancement of the number of low-energy states compared to the ab initio calculated PDOS of a perfect Eu 2 O 3 crystal. Our analysis demonstrates that while the former effect reflects the reduced phonon lifetimes observed in thin films due to scattering from lattice defects, the latter phenomenon arises from an ultrathin EuO layer formed between the thin Eu 2 O 3 film and the YSZ(001) substrate. Thus, our work uncovers another potential source of vibrational anomalies in thin films and multilayers, which has to be cautiously considered.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗