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DOE OSTI2025

Listening for Neutrinos with Quantum Acoustics

Many low-threshold superconducting detectors rely on athermal phonon sensing, in which meV-scale phonons from a DM scatter are sensed via their ability to break Cooper pairs in superconducting films. While detectors based on such pairbreaking sensors are highly advantageous and scalable, their sensor threshold is ultimately limited by the energy needed to break a Cooper pair, 2Δ. We present a novel detector architecture for single phonon detection at the O(10μeV) scale, the qubit-coupled hBAR, that does not share this limitation. This architecture, composed of a superconducting qubit piezoelectrically coupled to a high-overtone bulk acoustic resonator, was originally developed in the context of the quantum acoustics community and has a sensor threshold ultimately limited by thermal noise. Such ultra-low-threshold detectors have a wide range of fundamental science applications, including reactor monitoring via neutrinos.

Baxter, Daniel Stephen [Fermilab] (ORCID:000000030↗

DOE OSTI2022

Kohn anomaly and elastic softening in body-centered cubic molybdenum at high pressure

Transition metals in body-centered cubic (bcc) structures under compression can display several novel physical properties because of their complex electronic structures and electron-phonon interactions. Here, we used inelastic x-ray scattering experiments in a diamond-anvil cell up to ∼45 GPa and density-functional theory calculations up to 210 GPa to investigate the phonon dispersions, and electronic and elastic properties of single-crystal molybdenum (Mo). Our results show a pressure-induced Kohn anomaly at 𝑞∼0.5 along the [ξ00] direction in the longitudinal acoustic mode at ∼45 GPa; this anomaly is triggered by the pressure-enhanced Fermi-surface nesting effect. Theoretical calculations show that electron redistributions in the 𝑠-to-𝑑 orbitals of bcc-Mo contribute to the shear modulus anomaly at ∼50 GPa. In contrast, the Young's modulus anomaly in bcc-Mo at ∼210 GPa results from a Lifshitz-type electronic topological transition. In conclusion, our results shed light on the complex electronic behaviors that are associated with macroscopic elastic properties in typical bcc 𝑑-block transition metals under compression.

3-dimensional systems↗

DOE OSTI2024

Phonon modal analysis of thermal transport in ThO 2 with point defects using equilibrium molecular dynamics

Defects can significantly degrade the thermal conductivity of ThO 2 , an advanced nuclear fuel material as well as a surrogate for other fluorite-structured materials. Here, we investigate how point defects in ThO 2 impact phonon mode-resolved thermal transport. By incorporating phonon modes from lattice dynamics, we decompose the trajectory and heat flux to phonon normal mode space and extract key phonon properties, including phonon relaxation times and their contributions to thermal conductivity. We implement two methods. The first method is based on the Green Kubo formalism to resolve the contribution of each phonon mode to thermal conductivity. The second resolves the lifetime of individual phonon modes and the thermal conductivity is calculated using the Boltzmann transport equation within relaxation time approximation. Notably, a lower contribution of acoustic modes is revealed compared to perturbative approaches considering only three-phonon scattering processes. The effects of four types of point defects are evaluated. The strongest impact on a reduction in thermal conductivity is from Th interstitials, followed by Th vacancies. O interstitials/vacancies have a similar impact, albeit smaller than defects on the thorium sublattice. These observations are consistent with previous studies.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2024

A GHz-frequency multistrip acoustic beam splitter for quantum applications

Here we demonstrate a microwave-frequency, two-track acoustic beam splitter, based on a multistrip coupler design matched to four unidirectional transducers, two on each of the two acoustic tracks that make up the device. We explain the device design and its experimental implementation, showing good agreement between our model and the measured device scattering spectra. The beam splitter regime, dividing an input signal at port 1 into closely equal outputs at ports 2 and 3, is reached over a 94.7 MHz bandwidth centered at 4.79 GHz, with an output power division ratio |S 21 /S 31 | 2 = 1.1 ± 0.2. The measured bandwidth of the device is limited by the bandwidth of the transducers, rather than that of the multistrip coupler.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

Giant phonon anomalies in the proximate Kitaev quantum spin liquid α-RuCl 3

The Kitaev quantum spin liquid epitomizes an entangled topological state, for which two flavors of fractionalized low-energy excitations are predicted: the itinerant Majorana fermion and the Z 2 gauge flux. Here, it was proposed recently that fingerprints of fractional excitations are encoded in the phonon spectra of Kitaev quantum spin liquids through a novel fractional-excitation-phonon coupling. Here, we detect anomalous phonon effects in α-RuCl 3 using inelastic X-ray scattering with meV resolution. At high temperature, we discover interlaced optical phonons intercepting a transverse acoustic phonon between 3 and 7 meV. Upon decreasing temperature, the optical phonons display a large intensity enhancement near the Kitaev energy, J K ~8 meV, that coincides with a giant acoustic phonon softening near the Z 2 gauge flux energy scale. These phonon anomalies signify the coupling of phonon and Kitaev magnetic excitations in α-RuCl 3 and demonstrates a proof-of-principle method to detect anomalous excitations in topological quantum materials.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Nonlinear coupling of electromagnetic and electron acoustic waves in multi-species degenerate astrophysical plasma

Nonlinear wave-coupling is studied in a multispecies degenerate astrophysical plasma consisting of two electron species (at different temperatures): a highly degenerate main component plus a smaller classical relativistic flow immersed in a static neutralizing ion background. It is shown that the high frequency electromagnetic waves through their strong nonlinear interactions with the electron-acoustic waves [sustained by a multielectron component (degenerate) plasma surrounding a compact astrophysical object] can scatter to lower frequencies so that the radiation observed faraway will be spectrally shifted downward. It is also shown that, under definite conditions, the electromagnetic waves could settle into stationary solitonic states. It is expected that the effects of such structures may persist as detectable signatures in forms of modulated micropulses in the radiation observed far away from the accreting compact object. Both these effects will advance our abilities to interpret the radiation coming out of the compact objects.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

Photoacoustic 3-D imaging of polycrystalline microstructure improved with transverse acoustic waves

Non-invasive fast imaging of grain microstructure of polycrystalline ceria with sub-micrometric spatial resolution is performed via time-domain Brillouin scattering. The propagation of a nanoacoustic pulse is monitored down to 8 µm deep in a 30 × 30 µm2 area. Grains boundaries are reconstructed in three-dimensions via a twostep processing method, relying on the wavelet synchro-squeezed transform and the alpha shape algorithm. Imaging contrast is improved by taking advantage of stronger sensitivity to anisotropy of transverse acoustic waves, compared with longitudinal waves. Utilization of transverse waves in the image processing reveals additional boundaries that are not discerned using longitudinal waves, confirmed by an electron backscattering diffraction pattern. A buried inclined interface between differently oriented grains is identified by monitoring changes in amplitude (phase) of the portion of the signal associated with transverse (longitudinal) waves. Estimates of the inclination angle of this interface prove the sensitivity of our laser ultrasonic method to image inclined boundaries.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Block orbital-selective Mott insulators: A spin excitation analysis

We present a comprehensive study of the spin excitations—as measured by the dynamical spin structure factor S(q,ω)—of the so-called block-magnetic state of low-dimensional orbital-selective Mott insulators. We realize this state via both a multi-orbital Hubbard model and a generalized Kondo-Heisenberg Hamiltonian. Due to various competing energy scales present in the models, the system develops periodic ferromagnetic islands of various shapes and sizes, which are antiferromagnetically coupled. The 2×2 particular case was already found experimentally in the ladder material BaFe2Se3 that becomes superconducting under pressure. Here we discuss the electronic density as well as Hubbard and Hund coupling dependence of S(q,ω) using density matrix renormalization group method. Several interesting features were identified: (1) An acoustic (dispersive spin-wave) mode develops. (2) The spin-wave bandwidth establishes a new energy scale that is strongly dependent on the size of the magnetic island and becomes abnormally small for large clusters. (3) Optical (dispersionless spin excitation) modes are present for all block states studied here. In addition, a variety of phenomenological spin Hamiltonians have been investigated but none matches entirely our results that were obtained primarily at intermediate Hubbard U strengths. Our comprehensive analysis provides theoretical guidance and motivation to crystal growers to search for appropriate candidate materials to realize the block states, and to neutron scattering experimentalists to confirm the exotic dynamical magnetic properties unveiled here, with a rich mixture of acoustic and optical features.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2026

Phononic Casimir Effect in Planar Materials

The phononic Casimir effect between planar objects is investigated by deriving a formalism from the quantum partition function of the system following multiscattering approach. This fluctuation-induced coupling is mediated by phonons modeled as an effective elastic medium. We find that excitations with three types of polarizations arise from the resolved boundary conditions, however the coupling is dominated by only one of these degrees of freedom due to exponential suppression effects in the other two. Here, the obtained scaling laws and dependence on materials properties and temperature suggest effective pathways of interaction control. Scenarios of materials combinations are envisioned where the phononic Casimir effect is of similar order as the standard Casimir interaction mediated by electromagnetic fluctuations.

Acoustic phonons↗

DOE OSTI2021

Direct Imaging of Resonant Phonon-Magnon Coupling

Detection of phonons is critical for research on the interconversion between resonantly coupled magnons and phonons. Here we report the direct visualization of the resonant coupling of magnons and phonons by microfocused Brillouin light scattering on the Ni/Li Nb O 3 hybrid heterostructure. The static patterns of surface acoustic wave phonons, originating from the interference between the incident wave ψ 0 (A 0 , k, φ 0 ) and reflected wave ψ 1 (A 1 , - k, φ 1 ), can be modulated by magnetic field due to the magnon-phonon coupling. By analyzing the information of phonons obtained from Brillouin spectroscopy, the properties of the magnon system (Ni film), e.g., ferromagnetic resonance field and resonance linewidth, can be determined. The results provide spatially resolved information about phonon manipulation and detection in a coupled magnon-phonon system.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2021

The damping of terahertz acoustic modes in aqueous nanoparticle suspensions

In this work, we investigate the possibility of controlling the acoustic damping in a liquid when nanoparticles are suspended in it. To shed light on this topic, we performed Inelastic X-Ray Scattering (IXS) measurements of the terahertz collective dynamics of aqueous suspensions of nanospheres of various materials, size, and relative concentration, either charged or neutral. A Bayesian analysis of measured spectra indicates that the damping of the two acoustic modes of water increases upon nanoparticle immersion. This effect seems particularly pronounced for the longitudinal acoustic mode, which, whenever visible at all, rapidly damps off when increasing the exchanged wavevector. Results also indicate that the observed effect strongly depends on the material the immersed nanoparticles are made of.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Imaging phonon dynamics with ultrafast electron microscopy: Kinematical and dynamical simulations

Ultrafast x-ray and electron scattering techniques have proven to be useful for probing the transient elastic lattice deformations associated with photoexcited coherent acoustic phonons. Indeed, femtosecond electron imaging using an ultrafast electron microscope (UEM) has been used to directly image the influence of nanoscale structural and morphological discontinuities on the emergence, propagation, dispersion, and decay behaviors in a variety of materials. Here, we describe our progress toward the development of methods ultimately aimed at quantifying acoustic-phonon properties from real-space UEM images via conventional image simulation methods extended to the associated strain-wave lattice deformation symmetries and extents. Using a model system consisting of pristine single-crystal Ge and a single, symmetric Lamb-type guided-wave mode, we calculate the transient strain profiles excited in a wedge specimen and then apply both kinematical- and dynamical-scattering methods to simulate the resulting UEM bright-field images. While measurable contrast strengths arising from the phonon wavetrains are found for optimally oriented specimens using both approaches, incorporation of dynamical scattering effects via a multi-slice method returns better qualitative agreement with experimental observations. Contrast strengths arising solely from phonon-induced local lattice deformations are increased by nearly an order of magnitude when incorporating multiple electron scattering effects. We also explicitly demonstrate the effects of changes in global specimen orientation on the observed contrast strength, and we discuss the implications for increasing the sophistication of the model with respect to quantification of phonon properties from UEM images.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Low spontaneous Brillouin scattering in anti-resonant hollow-core fibers in GHz frequency range

Brillouin light scattering (BLS) is a powerful experimental tool that can be used to gain insights into the fundamental and applied properties of matter, like dispersions of quasiparticles in a solid, as well as their spatiotemporal dynamics. Many applications of light scattering favor the use of optical fibers in place of free-space optics. In this study, we compare the performance of anti-resonant hollow core fibers to that of conventional solid core fused silica fibers for BLS experiments in the GHz frequency range. Conventional fibers are barely suitable for low-noise measurements because of the spontaneous scattering of photons on various phononic modes present in the core and cladding. In the case of the hollow-core fiber, we identify a range of discrete phononic modes and associate them with the various acoustic modes of the structure surrounding the hollow core using finite-element numerical simulations. The measured relative intensity of the spontaneous BLS signal from these modes is orders of magnitude smaller than that of a solid-core fiber, making anti-resonant hollow-core fibers one of the best solutions for the single-mode light guidance for BLS and potentially other low-noise photonic experiments.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Anharmonic lattice dynamics and superionic transition in AgCrSe 2

Intrinsically low lattice thermal conductivity ( κ l a t ) in superionic conductors is of great interest for energy conversion applications in thermoelectrics. Yet, the complex atomic dynamics leading to superionicity and ultralow thermal conductivity remain poorly understood. Here, we report a comprehensive study of the lattice dynamics and superionic diffusion in A g C r S e 2 from energy- and momentum-resolved neutron and X-ray scattering techniques, combined with first-principles calculations. Our results settle unresolved questions about the lattice dynamics and thermal conduction mechanism in A g C r S e 2 . We find that the heat-carrying long-wavelength transverse acoustic (TA) phonons coexist with the ultrafast diffusion of Ag ions in the superionic phase, while the short-wavelength nondispersive TA phonons break down. Strong scattering of phonon quasiparticles by anharmonicity and Ag disorder are the origin of intrinsically low κ l a t . The breakdown of short-wavelength TA phonons is directly related to the Ag diffusion, with the vibrational spectral weight associated to Ag oscillations evolving into stochastic decaying fluctuations. Furthermore, the origin of fast ionic diffusion is shown to arise from extended flat basins in the energy landscape and collective hopping behavior facilitated by strong repulsion between Ag ions. These results provide fundamental insights into the complex atomic dynamics of superionic conductors.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Effect of a Fine-Scale Layered Structure of the Atmosphere on Infrasound Signals from Fragmenting Meteoroids

We investigate the influence of a fine-scale (FS) layered structure in the atmosphere on the propagation of infrasound signals generated by fragmenting meteoroids. Using a pseudo-differential parabolic equation (PPE) approach, we model broadband acoustic signals from point sources at altitudes of 35–100 km. The presence of FS fluctuations in the stratosphere (37–45 km) and the lower thermosphere (100–120 km) modifies ray trajectories, causing multiple arrivals and prolonged signal durations at ground stations. In particular, meteoroids fragmenting at 80–100 km can produce two distinct thermospheric arrivals beyond 150 km range, while meteoroids descending to 50 km or below yield weak, long-lived arrivals within the acoustic shadow zone via antiguiding propagation and diffraction. Comparison with observed infrasound data confirms that FS-layered inhomogeneities can account for multi-arrival “N-waves,” broadening potential interpretations of meteoroid signals. The results also apply to other atmospheric-entry objects, such as sample return capsules, emphasizing how FS structure impacts shock wave propagation. In conclusion, our findings advance understanding of wavefield evolution in a layered atmosphere and have broad relevance for global infrasound monitoring of diverse phenomena (e.g., re-entry capsules, rocket launches, and large-scale explosions).

Aeroacoustics↗

DOE OSTI2020

Nematic Correlation Length in Iron-Based Superconductors Probed by Inelastic X-Ray Scattering

Nematicity is ubiquitous in electronic phases of high-T c superconductors, particularly in the Fe-based systems. We used inelastic x-ray scattering to extract the temperature-dependent nematic correlation length ξ from the anomalous softening of acoustic phonon modes in FeSe, underdoped Ba(Fe 0.97 Co 0.03 ) 2 As 2 , and optimally doped Ba(Fe 0.94 Co 0.06 ) 2 As 2 . In all cases, we find that. is well described by a power law (T - T 0 ) -1/2 extending over a wide temperature range. Combined with the previously reported Curie-Weiss behavior of the nematic susceptibility, these results point to the mean-field character of the nematic transition, which we attribute to a sizable nematoelastic coupling that is likely detrimental to superconductivity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Temperature-dependent elastic constants of thorium dioxide probed using time-domain Brillouin scattering

Herein we report the adiabatic elastic constants of single-crystal thorium dioxide over a temperature range of 77–350 K. Time-domain Brillouin scattering, an all-optical, non-contact picosecond ultrasonic technique, is used to generate and detect coherent acoustic phonons that propagate in the bulk perpendicular to the surface of the crystal. These coherent acoustic lattice vibrations have been monitored in two hydrothermally grown single-crystal thorium dioxide samples along the (100) and (311) crystallographic directions. The three independent elastic constants of the cubic crystal (C 11 , C 12 , and C 44 ) are determined from the measured bulk acoustic velocities. The longitudinal wave along the (100) orientation provided a direct measurement of C 11 . Measurement of C 44 and C 12 was achieved by enhancing the intensity of quasi-shear mode in a (311) oriented crystal by adjusting the polarization angle relative to the crystal axes. We find the magnitude of softening of the three elastic constants to be ~2.5% over the measured temperature range. Good agreement is found between the measured elastic constants with previously reported values at room temperature, and between the measured temperature-dependent bulk modulus with calculated values. We find that semi-empirical models capturing lattice anharmonicity adequately reproduce the observed trend. We also determine the acoustic Grüneisen anharmonicity parameter from the experimentally derived temperature-dependent bulk modulus and previously reported temperature-dependent values of volumetric thermal expansion coefficient and heat capacity. This work presents measurements of the temperature-dependent elasticity in single-crystal thorium dioxide at cryogenic temperature and provides a basis for testing ab initio theoretical models and evaluating the impact of anharmonicity on thermophysical properties.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Shaping the terahertz sound propagation in water under highly directional confinement

Here, we consider the possibility of shaping the high-frequency acoustic propagation in a liquid upon directional confinement. This hypothesis is investigated by inelastic x-ray scattering measurements on water confined in aligned multiwalled carbon nanotubes, in which the momentum transfer was either parallel or orthogonal to the confinement axis. The comparison between the spectra measured in these two scattering geometries highlights the anisotropic nature of the dynamic response of directionally confined water, thus potentially inspiring pathways to shape high-frequency sound propagation in isotropic systems. Finally, a Bayesian analysis of measured spectra unravels close similarities in the phonon dispersions of multiwalled nanotubes and graphite.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗