Phonon Properties of Bulk Violet Phosphorus Single Crystals: Temperature and Pressure Evolution
Explore the source record for details and available documents.
Zhang, Lihui↗
SEARCH · Search NASA
Results for “phononics”
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.
Exciton-phonon coupling and phonon-assisted exciton relaxation dynamics in In1-xGaxP quantum dots
Not Available
Li, Beiye C. (ORCID:0000000267174318)↗
Helicity-Dependent Coherent Spin-Phonon Oscillations in the Ferromagnetic van der Waals Crystal CrI3
Explore the source record for details and available documents.
Material Science↗
Raman scattering by phonons and magnons and phonon-magnon interactions in NiO.
Explore the source record for details and available documents.
Perry, C. H.↗
Effect of interfacial structures on phonon transport across atomically precise Si/Al heterojunctions
Phonons are important carriers of energy and information in many cryogenic devices used for quantum information science and in fundamental physics experiments such as dark matter detectors. In these systems phonon behavior can be dominated by interfaces, hence there is increasing demand for a more detailed understanding of interfacial phonon transport in relevant material systems. Previous studies have focused on understanding thermal transport over the entire phonon spectrum at and above room temperature. At ultra-low temperatures, however, knowledge is missing regarding athermal phonon behavior due to the challenge in modeling the extreme conditions in micro-scale, heterogeneous cryogenic systems, as well as extracting single-phonon information from a large ensemble. In this work, we delineate interfacial phonon transport using a combination of classical molecular dynamics (MD) and phonon wave packet simulations, to illustrate the consistency and differences between the ensemble- and single-phonon dynamics. We consider three single-crystal Si surface reconstructions --- (1×1), (v3×v3) and (7×7) --- and model both experimentally observed Si(1×1)/Al interfaces and hypothesized Si(v3×v3)/Al and Si(7×7)/Al interfaces. The overall interfacial thermal conductance calculated from non-equilibrium MD shows that for the Si(1×1)/Al system, the presence of Al twin grain boundaries can hinder phonon transport and reduce thermal conductance by 2--12% relative to single-crystal Al; whereas the Si (v3×v3) and (7×7) reconstructions can enhance it by 6--19%. Normal mode decomposition reveals that both the increase and decrease in conductance are related to inelastic phonon scattering. Single-phonon wave packet simulations show results consistent with NEMD, while further suggesting that phonon polarization conversion is significant even when elastic transmission dominates, and that the interfacial structures have anisotropic impacts on atomic vibrations along different lattice directions. Our findings suggest alternative perspectives in achieving selective phonon transport through controlling interfacial structures of materials with atomically-precise fabrication techniques, and that the phonon wave packet formalism is a potentially powerful method for developing a detailed understanding of non-equilibrium phenomena in the low-temperature limit.
Lu, Zexi↗
Lattice anharmonicity effects in fluorite oxide single crystals and anomalous increase in phonon lifetime in ceria at elevated temperature
Here, we investigate the temperature dependence of the frequency and linewidth of the triply degenerate T 2g zone-centered optical phonon in flux-grown ceria and hydrothermally synthesized thoria single crystals from room temperature to 1273 K using Raman spectroscopy. Both crystals exhibit an expected increase in the phonon linewidth with temperature due to enhanced phonon–phonon scattering. However, ceria displays an anomalous linewidth reduction in the temperature range of 1023–1123 K. First-principles phonon linewidth calculations considering cubic and quartic phonon interactions within temperature-independent phonon dispersion fail to describe this anomaly. A parameterization of the temperature-dependent second-order interatomic force constants based on previously reported phonon dispersion measured at room and high temperatures predicts a deviation from the monotonic linewidth increase, albeit at temperatures lower than those observed experimentally for ceria. The qualitative agreement in the trend of temperature-dependent linewidth suggests that lattice anharmonicity-induced phonon renormalization plays a role in phonon lifetime. Specifically, a change in the overlap between softened acoustic and optical branches in the dispersion curve reduces the available phonon scattering phase space of the Raman-active mode at the zone center, leading to an increased phonon lifetime within a narrow temperature interval. These findings provide insights into higher-order anharmonic interactions in ceria and thoria, motivating further investigations into the role of anharmonicity-induced phonon renormalization on phonon lifetimes at high temperatures.
11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Monte-Carlo modeling of phonon thermal transport using DFT-based anisotropic dispersion relations over the full Brillouin zone
In this work, we present a Monte Carlo (MC) approach to solve the phonon Boltzmann transport equation (BTE) in which the anisotropic phonon dispersion relations over the full Brillouin zone (BZ) are used. In this approach, the discretization of the BZ used to compute the phonon relaxation time places constraints on the direction of scattered phonons in the real-space simulation domain. The phonon dispersion and phonon relaxation times are calculated using the density functional theory (DFT) approach. The modified MC approach is validated by a close examination of its ability to simulate phonon transport in both the ballistic and diffusive regimes for multiple materials including GaAs, InAs, ThO 2 , and α-U. In doing so, the phonon thermal conductivities from 100 K to 1000 K are calculated and compared with traditional non-transport solution of the phonon BTE. It is found that the phonon thermal conductivities of α-U and ThO 2 obtained from MC simulations using isotropic dispersion are larger than the values obtained using anisotropic phonon dispersion relations over the full BZ. The effect of phonon-defect scattering on the thermal conductivity of ThO 2 is also studied as an application of the current MC approach and found to agree with previously computed values in the literature. The MC solver developed here has been parallelized as a step to demonstrate its potential to solving computationally intensive phonon thermal transport problems at the mesoscale.
36 MATERIALS SCIENCE↗
A First Principles Approach to Spectral Phonon Transport in Heterostructures
Understanding thermal transport across interfaces which give rise to a thermal resistance (also known as Kapitza resistance) is a critical issue affecting the development of nanotechnologies. Much modern and emergent nanotechnology consist of adjacent materials, and phonon mediated heat transfer governs thermal behavior across internal interfaces in these devices. The physics of thermal transport in solids are governed both by phenomena occurring at the atomic scale and interactions with the material's microstructure. The forecasting of fundamental quantities such as temperature, heat flux and thermal conductivity typically employs the semi-classical Boltzmann transport equation to predict the macroscopic behavior of materials in terms of the microscopic dynamics of its heat carriers. Kapitza resistance was first discovered in liquid helium experiments and has led to a fundamental research thrust in micro and nano-scale heat transport, the behavior of thermal carriers across internal interfaces. Thermal interfacial resistance (TIR) is a widely studied phenomenon, first engaged by Swartz and Pohl through their development of the acoustic and diffuse mismatch methods, then continued through myriad efforts with varying methods and approaches in an attempt to resolve carrier behavior at thermal interfaces. Many of the fundamental approaches to TIR have been at the nanoscale, and research is conducted with molecular dynamics (MD) and density functional theory (DFT) methods. The limitations of these methods is system size; atomistic methods tend to be limited to system sizes of 100,000 atoms or less. Larger length-scale methods have also been pursued, based on the principles of acoustic or diffuse mismatch, but not all include simulation of TIR using a full phonon band spectrum, or temperature dependent methods. Our approach to enabling phonon transport in layered materials draws upon our previous work of demonstrating spectrally coupled phonon transport in homogeneous and heterogeneous materials. We use a semi-analytical approach in which the Bose-Einstein (B-E) statistics set the strength of the phonon radiance in a frequency group, but the B-E statistics are informed with information from the transport system. The B-E statistics in a single frequency group feels the influence of all the groups through the spatial temperature. We also include a new field term which is an indicator of the amount of non-equilibrium behavior of the phonon spectrum---this is added to the phonon source term in all groups to ensure closure and conservation of energy, as the phonon groups in the transport system and the analytical systems are coupled. This work builds upon our previous approach by adding a phonon coupling term at an internal interface, using the principles of the DMM through transmission and reflection coefficients. In this work, the coefficients are determined through computing a common temperature at the interface, influenced by the phonon band structure of both materials, in effect, providing mixing between the two material systems and using the common temperature to set the strength of the phonon radiance at the boundaries on either side of the interface. Our approach uses material properties computed along various crystallographic orientations, and while some isotropy is built into the interface condition, the material properties weight the phonon distributions in the proper crystalline direction. Greater resolution of phonon behavior in proximity to an interface, and more accurate predictions of TIR are obtained. While it is true the assumption of diffuse mismatch can yield inconsistent results compared to experiment especially at low temperatures, this work focuses on room temperature and beyond effects, for future applications in nuclear fuel, or thermoelectric devices; a modified mismatch approach may be feasible if applied properly. Additionally, our methods focus on bridging mesoscale to engineering scale
36 MATERIALS SCIENCE↗
Phonon-mediated lipid raft formation in biological membranes
Short-wavelength collective molecular motions, also known as phonons, have recently attracted much interest in revealing dynamic properties of biological membranes through the use of neutron and x-ray scattering, infrared and Raman spectroscopies, and molecular dynamics simulations. Experimentally detecting unique vibrational patterns such as, shear phonon excitations, viscoelastic crossovers, transverse acoustic phonon gaps, and continuous and truncated optical phonon modes in cellular membranes, to name a few, has proven non-trivial. Here, we review recent advances in liquid thermodynamics that have resulted in the development of the phonon theory of 1 liquids. The theory has important predictions regarding the shear vibrational spectra of fluids, namely the emergence of viscoelastic crossovers and transverse acoustic phonon gaps. Furthermore, we show that these vibrational patterns are common in soft (non-crystalline) materials, including, but not limited to liquids, colloids, liquid crystals (mesogens), block copolymers, and biological membranes. The existence of viscoelastic crossovers and acoustic phonon gaps define the self-diffusion properties of cellular membranes and provide a molecular picture of the transient nature of lipid rafts.1 Importantly, the timescales (picoseconds) for the formation and dissolution of transient lipid rafts match the lifetime of the formation and breakdown of interfacial water hydrogen bonds. Apart from acoustic propagating phonon modes, biological membranes can also support more energetic non-propagating optical phonon excitations, also known as standing waves or breathing modes. Importantly, optical phonons can be truncated due to the existence of finite size nanodomains made up of strongly correlated lipid-cholesterol molecular pairs. These strongly coupled molecular pairs can serve as nucleation centers for the formation of stable rafts at larger length scales, due to correlations of spontaneous fluctuations (Onsager’s regression hypothesis). Finally and importantly, molecular level viscoelastic crossovers, acoustic phonon gaps, and continuous and truncated optical phonon modes may offer insights as to how lipid-lipid and lipid-protein interactions enable biological function.
59 BASIC BIOLOGICAL SCIENCES↗
Reverse phonon thermal flux from an applied electric field
In the phenomenon known as electron drag, a phonon thermal flux is established in a conducting crystal by an electric field applied under isothermal conditions through directed transfer of quasimomentum from the electronic charge current to the phonon subsystem. Prior understanding of this phenomenon involves a thermal current composed of low-frequency acoustic phonons that is in the same direction as the charge current. This results in an increase of the Peltier thermopower. Here, we show that it is also possible to establish a phonon thermal current that is in the opposite direction to the charge current, which we refer to as a reverse phonon thermal flux. We demonstrate this behavior both through a simple qualitative model and through first-principles calculations performed for three materials: p-type 𝜃-TaN, n-type BAs, and n-type Si. The reverse phonon flux is shown to arise through intervalley electron-phonon scattering processes involving high-frequency acoustic phonons. Unlike n-BAs and n-Si, the combined features in the band structure and phonon dispersions of p-type 𝜃-TaN promote a particularly large reverse phonon thermal flux comparable in magnitude to the oppositely directed thermal flux from low-frequency phonons. Finally, this work highlights a previously unrecognized behavior in the coupled electron-phonon system and advances our understanding of the rich physics of transport in solids.
lattice dynamics↗
Oscillate and renormalize: Fast phonons reshape the Kondo effect in flat-band systems
Here, we examine the interplay between electron correlations and phonons in an Anderson-Holstein impurity model with an Einstein phonon. When the phonons are slow compared to charge fluctuations (frequency 𝜔 0 ≪ 𝑈/2, the onsite Coulomb scale 𝑈/2), we demonstrate analytically that the expected phonon-mediated reduction of interactions is completely suppressed, even in the strong-coupling regime. This suppression arises from the oscillator's inability to respond to rapid charge fluctuations, manifested as a compensation effect between the polaronic cloud and the excited-state phonons associated with valence fluctuations. We identify a frozen mixed valence phase, above a threshold dimensionless electron-phonon coupling 𝛼* when the phonons are slow, where the static phonon cloud locks the impurity into specific valence configurations, potentially explaining the puzzling coexistence of mixed valence behavior and insulating properties in materials like rust. Conversely, when the phonon is fast (𝜔 0 ≳ 𝑈/2), the system exhibits conventional polaronic behavior with renormalized onsite interactions effectively 𝑈 eff due to phonon-mediated attraction, with additional satellite features in the local spectral function due to phonon excitations. Using numerical renormalization group calculations, a fully dynamic renormalization technique, we confirm these behaviors in both regimes. These findings have important implications for strongly correlated systems where phonon energy scales may be comparable to the Coulomb scale, such as in twisted bilayer graphene, necessitating careful consideration of interaction renormalizations in theoretical models.
Anderson impurity model↗
Direct observation of strong momentum-dependent electron-phonon coupling in a metal
Phonon scattering in metals is one of the most fundamental processes in materials science. However, understanding such processes has remained challenging and requires detailed information on interactions between phonons and electrons. We use an ultrafast electron diffuse scattering technique to resolve the nonequilibrium phonon dynamics in femtosecond–laser-excited tungsten in both time and momentum. We determine transient populations of phonon modes which show strong momentum dependence initiated by electron-phonon coupling. For phonons near Brillouin zone border, we observe a transient rise in their population on a timescale of approximately 1 picosecond driven by the strong electron-phonon coupling, followed by a slow decay on a timescale of approximately 8 picosecond governed by the weaker phonon-phonon relaxation process. We find that the exceptional harmonicity of tungsten is needed for isolating the two processes, resulting in long-lived nonequilibrium phonons in a pure metal. Our finding highlights that electron-phonon scattering can be the determinant factor in the phonon thermal transport of metals.
36 MATERIALS SCIENCE↗
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↗
Strong Surface-Enhanced Coherent Phonon Generation in van der Waals Materials
Terahertz (THz) coherent phonons have emerged as promising candidates for the next generation of high-speed, low-energy information carriers in atomically thin phononic or phonon-integrated on-chip devices. However, effectively manipulating THz coherent phonons remains a significant challenge. Here, in this study, we investigated THz coherent phonon generation in exfoliated van der Waals (vdW) flakes of Fe 3 GeTe 2 , Fe 5 GeTe 2 , and FePS 3 . We successfully generated the THz A 1g coherent phonon mode in these vdW flakes. An innovative approach involved partially exfoliating vdW flakes on a gold substrate and partially on a silicon (Si) substrate to compare the THz coherent phonon generation between both sides. Interestingly, we observed a significantly enhanced THz coherent phonon in the vdW/gold area compared with that in the vdW/Si area. Frequency-domain Raman mapping across the vdW flakes corroborated these findings. Numerical simulations further indicated a stronger enhanced surface field in vdW/gold structures than in vdW/Si structures. Consequently, we attribute the observed enhancement in THz coherent phonon generation to the increased surface field on the gold substrate. This enhancement was consistent across the three different vdW materials studied, suggesting the universality of this strategy. Our results hold promise for advancing the design of THz phononic and phonon-integrated devices.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Anharmonic phonon behavior via irreducible derivatives: Self-consistent perturbation theory and molecular dynamics
Cubic phonon interactions are now regularly computed from first principles, and the quartic interactions have begun to receive more attention. Given this realistic anharmonic vibrational Hamiltonian, the classical phonon Green's function can be precisely measured using molecular dynamics, which can then be used to rigorously assess the range of validity for self-consistent diagrammatic approaches in the classical limit. Here we use the bundled irreducible derivative approach to efficiently and precisely compute the cubic and quartic phonon interactions of CaF 2 , systematically obtaining the vibrational Hamiltonian purely in terms of irreducible derivatives. We demonstrate that the 4-phonon sunset diagram has an important contribution to the optical phonon linewidths beyond T = 500 K. Reasonable results are obtained even at T = 900 K when performing self-consistency using the 4-phonon loop diagram and evaluating the 3-phonon bubble and 4-phonon sunset diagrams post-self-consistency. Further improvements are obtained by performing quasiparticle perturbation theory, where both the 4-phonon loop and the real part of the 3-phonon bubble are employed during self-consistency. Finally, our irreducible derivative approach to self-consistent perturbation theory is a robust tool for studying anharmonic phonons in both the quantum and classical regimes.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Cavity-Assisted Coherent Phonon Generation and Control in a WSe 2 /Au Structure
Coherent phonons in the Terahertz (THz) regime have gained attention as potential candidates for next-generation high-speed, low-energy information carriers in atomically thin phononic or phonon-integrated on-chip devices. Nevertheless, achieving efficient control over THz coherent phonons continues to pose a considerable challenge. In this work, we explore THz coherent phonon generation in exfoliated van der Waals (vdW) flakes of WSe 2 on Au (WSe 2 /Au) and Si (WSe 2 /Si) using time-resolved pump-probe spectroscopy. The generation of THz coherent phonons was studied as a function of WSe 2 layer thickness and laser wavelength. Notably, a significant enhancement in THz coherent phonon generation was observed in the WSe 2 /Au structure, but only within specific ranges of WSe 2 thickness and laser wavelength. Further, the results from numerical simulations, which consider a self-hybridized optical cavity depending on WSe 2 thickness, along with optical reflectance and Raman spectroscopy measurements, aligned well with the time-domain observations of THz coherent phonon generation. We propose that the observed enhancement in THz coherent phonon generation is strongly influenced by light-matter interaction in the WSe 2 cavity, a mechanism that may be applicable to a broader range of vdW materials. These findings offer promising insights for the development of THz phononic or phonon-integrated devices.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Unravelling ultralow thermal conductivity in perovskite Cs2AgBiBr6: dominant wave-like phonon tunnelling and strong anharmonicity
Abstract Understanding the lattice dynamics and heat transport physics in the lead-free halide double perovskites remains an outstanding challenge due to their lattice dynamical instability and strong anharmonicity. In this work, we investigate the microscopic mechanisms of anharmonic lattice dynamics and thermal transport in lead-free halide double perovskite Cs 2 AgBiBr 6 from first principles. We combine self-consistent phonon calculations with bubble diagram correction and a unified theory of lattice thermal transport that considers both the particle-like phonon propagation and wave-like tunnelling of phonons. An ultra-low thermal conductivity at room temperature (~0.21 Wm −1 K −1 ) is predicted with weak temperature dependence( ~ T −0.34 ), in sharp contrast to the conventional ~T −1 dependence. Particularly, the vibrational properties of Cs 2 AgBiBr 6 are featured by strong anharmonicity and wave-like tunnelling of phonons. Anharmonic phonon renormalization from both the cubic and quartic anharmonicities are found essential in precisely predicting the phase transition temperature in Cs 2 AgBiBr 6 while the negative phonon energy shifts induced by cubic anharmonicity has a significant influence on particle-like phonon propagation. Further, the contribution of the wave-like tunnelling to the total thermal conductivity surpasses that of the particle-like propagation above around 310 K, indicating the breakdown of the phonon gas picture conventionally used in the Peierls-Boltzmann Transport Equation. Importantly, further including four-phonon scatterings is required in achieving the dominance of wave-like tunnelling, as compared to the dominant particle-like propagation channel when considering only three-phonon scatterings. Our work highlights the importance of lattice anharmonicity and wave-like tunnelling of phonons in the thermal transport in lead-free halide double perovskites.
Chemistry↗