Quantum acoustics unravels Planckian resistivity.

Strange metals exhibit universal linear-in-temperature resistivity described by a Planckian scattering rate, the origin of which remains elusive. By employing an approach inspired by quantum optics, we arrive at the coherent state representation of lattice vibrations: quantum acoustics. Utilizing this nonperturbative framework, we demonstrate that lattice vibrations could serve as active drivers in the Planckian resistivity phenomenon, challenging prevailing theories. By treating charge carriers as quantum wave packets negotiating the dynamic acoustic field, we find that a competition ensues between localization and delocalization giving rise to the previously conjectured universal quantum bound of diffusion, [Formula: see text], independent of temperature or any other material parameters. This leads to the enigmatic T-linear resistivity over hundreds of degrees, except at very low temperatures. Quantum diffusion also explains why strange metals have much higher electrical resistivity than typical metals. Our work elucidates the critical role of phonons in Planckian resistivity from a unique perspective and reconsiders their significance in the transport properties of strange metals.

Phonon screening and dissociation of excitons at finite temperatures from first principles.

The properties of excitons, or correlated electron-hole pairs, are of paramount importance to optoelectronic applications of materials. A central component of exciton physics is the electron-hole interaction, which is commonly treated as screened solely by electrons within a material. However, nuclear motion can screen this Coulomb interaction as well, with several recent studies developing model approaches for approximating the phonon screening of excitonic properties. While these model approaches tend to improve agreement with experiment, they rely on several approximations that restrict their applicability to a wide range of materials, and thus far they have neglected the effect of finite temperatures. Here, we develop a fully first-principles, parameter-free approach to compute the temperature-dependent effects of phonon screening within the ab initio [Formula: see text]-Bethe-Salpeter equation framework. We recover previously proposed models of phonon screening as well-defined limits of our general framework, and discuss their validity by comparing them against our first-principles results. We develop an efficient computational workflow and apply it to a diverse set of semiconductors, specifically AlN, CdS, GaN, MgO, and [Formula: see text]. We demonstrate under different physical scenarios how excitons may be screened by multiple polar optical or acoustic phonons, how their binding energies can exhibit strong temperature dependence, and the ultrafast timescales on which they dissociate into free electron-hole pairs.

Superradiant Thomson scattering from graphite in the extreme ultraviolet.

We study the Thomson scattering from highly oriented pyrolitic graphite excited by the extreme ultraviolet, coherent pulses of FERMI free electron laser (FEL). An apparent nonlinear behavior is observed and fully described in terms of the coherent nature of both exciting FEL beam and scattered radiation, producing an intensity-dependent enhancement of the Thomson scattering cross-section. The process resembles Dicke's superradiant phenomenon and is thus interpreted as the observation of superradiant Thomson scattering. The process also triggers the creation of coherent, low-q ([Formula: see text] 0.3 Å[Formula: see text]), low energy phonons. The experimental data and analysis provide quantitative information on the sample characteristics, absorption, scattering factor, and coherent phonon energies and populations and open the route for the investigation of the deep nature of complex materials.

Chemical bonding dictates drastic critical temperature difference in two seemingly identical superconductors.

Though YB6 and LaB6 share the same crystal structure, atomic valence electron configuration, and phonon modes, they exhibit drastically different phonon-mediated superconductivity. YB6 superconducts below 8.4 K, giving it the second-highest critical temperature of known borides, second only to MgB2. LaB6 does not superconduct until near-absolute zero temperatures (below 0.45 K), however. Though previous studies have quantified the canonical superconductivity descriptors of YB6's greater Fermi-level (Ef) density of states and higher electron-phonon coupling (EPC), the root of this difference has not been assessed with full detail of the electronic structure. Through chemical bonding, we determine low-lying, unoccupied 4f atomic orbitals in lanthanum to be the key difference between these superconductors. These orbitals, which are not accessible in YB6, hybridize with π B-B bonds and bring this π-system lower in energy than the σ B-B bonds otherwise at Ef. This inversion of bands is crucial: the optical phonon modes we show responsible for superconductivity cause the σ-orbitals of YB6 to change drastically in overlap, but couple weakly to the π-orbitals of LaB6. These phonons in YB6 even access a crossing of electronic states, indicating strong EPC. No such crossing in LaB6 is observed. Finally, a supercell (the M k-point) is shown to undergo Peierls-like effects in YB6, introducing additional EPC from both softened acoustic phonons and the same electron-coupled optical modes as in the unit cell. Overall, we find that LaB6 and YB6 have fundamentally different mechanisms of superconductivity, despite their otherwise near-identity.

Phonon stability boundary and deep elastic strain engineering of lattice thermal conductivity.

Recent studies have reported the experimental discovery that nanoscale specimens of even a natural material, such as diamond, can be deformed elastically to as much as 10% tensile elastic strain at room temperature without the onset of permanent damage or fracture. Computational work combining ab initio calculations and machine learning (ML) algorithms has further demonstrated that the bandgap of diamond can be altered significantly purely by reversible elastic straining. These findings open up unprecedented possibilities for designing materials and devices with extreme physical properties and performance characteristics for a variety of technological applications. However, a general scientific framework to guide the design of engineering materials through such elastic strain engineering (ESE) has not yet been developed. By combining first-principles calculations with ML, we present here a general approach to map out the entire phonon stability boundary in six-dimensional strain space, which can guide the ESE of a material without phase transitions. We focus on ESE of vibrational properties, including harmonic phonon dispersions, nonlinear phonon scattering, and thermal conductivity. While the framework presented here can be applied to any material, we show as an example demonstration that the room-temperature lattice thermal conductivity of diamond can be increased by more than 100% or reduced by more than 95% purely by ESE, without triggering phonon instabilities. Such a framework opens the door for tailoring of thermal-barrier, thermoelectric, and electro-optical properties of materials and devices through the purposeful design of homogeneous or inhomogeneous strains.

Coherent detection of hidden spin-lattice coupling in a van der Waals antiferromagnet.

Strong interactions between different degrees of freedom lead to exotic phases of matter with complex order parameters and emergent collective excitations. Conventional techniques, such as scattering and transport, probe the amplitudes of these excitations, but they are typically insensitive to phase. Therefore, novel methods with phase sensitivity are required to understand ground states with phase modulations and interactions that couple to the phase of collective modes. Here, by performing phase-resolved coherent phonon spectroscopy (CPS), we reveal a hidden spin-lattice coupling in a vdW antiferromagnet FePS3 that eluded other phase-insensitive conventional probes, such as Raman and X-ray scattering. With comparative analysis and analytical calculations, we directly show that the magnetic order in FePS3 selectively couples to the trigonal distortions through partially filled t2g orbitals. This magnetoelastic coupling is linear in magnetic order and lattice parameters, rendering these distortions inaccessible to inelastic scattering techniques. Our results not only capture the elusive spin-lattice coupling in FePS3 but also establish phase-resolved CPS as a tool to investigate hidden interactions.

A stability bound on the [Formula: see text]-linear resistivity of conventional metals.

Perturbative considerations account for the properties of conventional metals, including the range of temperatures where the transport scattering rate is 1/τtr = 2πλT, where λ is a dimensionless strength of the electron-phonon coupling. The fact that measured values satisfy λ ≲ 1 has been noted in the context of a possible "Planckian" bound on transport. However, since the electron-phonon scattering is quasielastic in this regime, no such Planckian considerations can be relevant. We present and analyze Monte Carlo results on the Holstein model which show that a different sort of bound is at play: a "stability" bound on λ consistent with metallic transport. We conjecture that a qualitatively similar bound on the strength of residual interactions, which is often stronger than Planckian, may apply to metals more generally.

Ubiquitous coexisting electron-mode couplings in high-temperature cuprate superconductors.

In conventional superconductors, electron-phonon coupling plays a dominant role in generating superconductivity. In high-temperature cuprate superconductors, the existence of electron coupling with phonons and other boson modes and its role in producing high-temperature superconductivity remain unclear. The evidence of electron-boson coupling mainly comes from angle-resolved photoemission (ARPES) observations of [Formula: see text]70-meV nodal dispersion kink and [Formula: see text]40-meV antinodal kink. However, the reported results are sporadic and the nature of the involved bosons is still under debate. Here we report findings of ubiquitous two coexisting electron-mode couplings in cuprate superconductors. By taking ultrahigh-resolution laser-based ARPES measurements, we found that the electrons are coupled simultaneously with two sharp modes at [Formula: see text]70meV and [Formula: see text]40meV in different superconductors with different dopings, over the entire momentum space and at different temperatures above and below the superconducting transition temperature. These observations favor phonons as the origin of the modes coupled with electrons and the observed electron-mode couplings are unusual because the associated energy scales do not exhibit an obvious energy shift across the superconducting transition. We further find that the well-known "peak-dip-hump" structure, which has long been considered a hallmark of superconductivity, is also omnipresent and consists of "peak-double dip-double hump" finer structures that originate from electron coupling with two sharp modes. These results provide a unified picture for the [Formula: see text]70-meV and [Formula: see text]40-meV energy scales and their evolutions with momentum, doping and temperature. They provide key information to understand the origin of these energy scales and their role in generating anomalous normal state and high-temperature superconductivity.

Mutual spin-phonon driving effects and phonon eigenvector renormalization in nickel (II) oxide.

The physics of mutual interaction of phonon quasiparticles with electronic spin degrees of freedom, leading to unusual transport phenomena of spin and heat, has been a subject of continuing interests for decades. Despite its pivotal role in transport processes, the effect of spin-phonon coupling on the phonon system, especially acoustic phonon properties, has so far been elusive. By means of inelastic neutron scattering and first-principles calculations, anomalous scattering spectral intensity from acoustic phonons was identified in the exemplary collinear antiferromagnetic nickel (II) oxide, unveiling strong spin-lattice correlations that renormalize the polarization of acoustic phonon. In particular, a clear magnetic scattering signature of the measured neutron scattering intensity from acoustic phonons is demonstrated by its momentum transfer and temperature dependences. The anomalous scattering intensity is successfully modeled with a modified magneto-vibrational scattering cross-section, suggesting the presence of spin precession driven by phonon. The renormalization of phonon eigenvector is indicated by the observed "geometry-forbidden" neutron scattering intensity from transverse acoustic phonon. Importantly, the eigenvector renormalization cannot be explained by magnetostriction but instead, it could result from the coupling between phonon and local magnetization of ions.

Direct visualization of polaron formation in the thermoelectric SnSe.

SnSe is a layered material that currently holds the record for bulk thermoelectric efficiency. The primary determinant of this high efficiency is thought to be the anomalously low thermal conductivity resulting from strong anharmonic coupling within the phonon system. Here we show that the nature of the carrier system in SnSe is also determined by strong coupling to phonons by directly visualizing polaron formation in the material. We employ ultrafast electron diffraction and diffuse scattering to track the response of phonons in both momentum and time to the photodoping of free carriers across the bandgap, observing the bimodal and anisotropic lattice distortions that drive carrier localization. Relatively large (18.7 Å), quasi-one-dimensional (1D) polarons are formed on the 300-fs timescale with smaller (4.2 Å) 3D polarons taking an order of magnitude longer (4 ps) to form. This difference appears to be a consequence of the profoundly anisotropic electron-phonon coupling in SnSe, with strong Fröhlich coupling only to zone-center polar optical phonons. These results demonstrate a high density of polarons in SnSe at optimal doping levels. Strong electron-phonon coupling is critical to the thermoelectric performance of this benchmark material and, potentially, high performance thermoelectrics more generally.

Dissipative coupling-induced phonon lasing.

Phonon lasers, as the counterpart of photonic lasers, have been intensively studied in a large variety of systems; however, (all) most of them are based on the directly coherent pumping. Intuitively, dissipation is unfavorable for lasing. Here, we experimentally demonstrate a mechanism of generating phonon lasing from the dissipative coupling in a multimode optomechanical system. By precisely engineering the dissipations of two membranes and tuning the intensity modulation of the cavity light, the two-membrane-in-the-middle system exhibits non-Hermitian characteristics and the cavity-mediated interaction between two nanomechanical resonators becomes purely dissipative. The level attraction and damping repulsion are clearly exhibited as the signature of dissipative coupling. After the exceptional point, a non-Hermitian phase transition, where eigenvalues and the corresponding eigenmodes coalesce, two phonon modes are simultaneously excited into the self-sustained oscillation regime by increasing the interaction strength over a critical value (threshold). In distinct contrast to conventional phonon lasers, the measurement of the second-order phonon correlation reveals the oscillatory and biexponential phases in the nonlasing regime as well as the coherence phase in the lasing regime. Our study provides a method to study phonon lasers in a non-Hermitian open system and could be applied to a wide range of disciplines, including optics, acoustics, and quantum many-body physics.

Phonon drag thermal Hall effect in metallic strontium titanate.

SrTiO3, a quantum paralectric, displays a detectable phonon thermal Hall effect (THE). Here, we show that the amplitude of the THE is extremely sensitive to stoichiometry. It drastically decreases upon substitution of a tiny fraction of Sr atoms with Ca, which stabilizes the ferroelectric order. It drastically increases by an even lower density of oxygen vacancies, which turn the system to a dilute metal. The enhancement in the metallic state exceeds by far the sum of the electronic and the phononic contributions. We explain this observation as an outcome of three features: 1) Heat is mostly transported by phonons; 2) the electronic Hall angle is extremely large; and 3) there is substantial momentum exchange between electrons and phonons. Starting from Herring's picture of phonon drag, we arrive to a quantitative account of the enhanced THE. Thus, phonon drag, hitherto detected as an amplifier of thermoelectric coefficients, can generate a purely thermal transverse response in a dilute metal with a large Hall angle. Our results reveal a hitherto-unknown consequence of momentum-conserving collisions between electrons and phonons.

Influence of nuclear quantum effects on the electronic properties of amorphous carbon.

We carry out quantum simulations to study the physical properties of diamond-like amorphous carbon by coupling first-principles molecular dynamics with a quantum thermostat, and we analyze multiple samples representative of different defective sites present in the disordered network. We show that quantum vibronic coupling is critical in determining the electronic properties of the system, in particular its electronic and mobility gaps, while it has a moderate influence on the structural properties. We find that despite localized electronic states near the Fermi level, the quantum nature of the nuclear motion leads to a renormalization of the electronic gap surprisingly similar to that found in crystalline diamond. We also discuss the notable influence of nuclear quantum effects on band-like and variable-hopping mechanisms contributing to electrical conduction. Our calculations indicate that methods often used to evaluate electron-phonon coupling in ordered solids are inaccurate to study the electronic and transport properties of amorphous semiconductors composed of light atoms.

Phonon signatures for polaron formation in an anharmonic semiconductor.

Mechanistic studies on lead halide perovskites (LHPs) in recent years have suggested charge carrier screening as partially responsible for long carrier diffusion lengths and lifetimes that are key to superior optoelectronic properties. These findings have led to the ferroelectric large polaron proposal, which attributes efficient charge carrier screening to the extended ordering of dipoles from symmetry-breaking unit cells that undergo local structural distortion and break inversion symmetry. It remains an open question whether this proposal applies in general to semiconductors with LHP-like anharmonic and dynamically disordered phonons. Here, we study electron-phonon coupling in Bi2O2Se, a semiconductor which bears resemblance to LHPs in ionic bonding, spin-orbit coupling, band transport with long carrier diffusion lengths and lifetimes, and phonon disorder as revealed by temperature-dependent Raman spectroscopy. Using coherent phonon spectroscopy, we show the strong coupling of an anharmonic phonon mode at 1.50 THz to photo-excited charge carriers, while the Raman excitation of this mode is symmetry-forbidden in the ground-state. Density functional theory calculations show that this mode, originating from the A1g phonon of out-of-plane Bi/Se motion, gains oscillator strength from symmetry-lowering in polaron formation. Specifically, lattice distortion upon ultrafast charge localization results in extended ordering of symmetry-breaking unit cells and a planar polaron wavefunction, namely a two-dimensional polaron in a three-dimensional lattice. This study provides experimental and theoretical insights into charge interaction with anharmonic phonons in Bi2O2Se and suggests ferroelectric polaron formation may be a general principle for efficient charge carrier screening and for defect-tolerant semiconductors.

Chiral Phonons: Prediction, Verification, and Application.

Chirality as an asymmetric property is prevalent in nature. In physics, the chirality of the elementary particles that make up matter has been widely studied and discussed, and nowadays, the concept has developed into the field of phonons. As an important fundamental excitation in condensed matter physics, phonons are traditionally considered to be linearly polarized and nonchiral. However, in recent years, the chirality of phonons has been revealed and further experimentally verified. The discovery has triggered a series of new explorations and developments in phonon-related physical processes. This Mini-Review provides an overview of the theoretical prediction of chiral phonons and multiple experimental detection methods and highlights the current key issues in the application of chiral phonons in different fields.

Modulating Thermal Conductivity via Targeted Phonon Excitation.

Thermal conductivity is a critical material property in numerous applications, such as those related to thermoelectric devices and heat dissipation. Effectively modulating thermal conductivity has become a great concern in the field of heat conduction. Here, a quantum modulation strategy is proposed to modulate the thermal conductivity/heat flux by exciting targeted phonons. It shows that the thermal conductivity of graphene can be tailored in the range of 1559 W m-1 K-1 (decreased to 49%) to 4093 W m-1 K-1 (increased to 128%), compared with the intrinsic value of 3189 W m-1 K-1. The effects are also observed for graphene nanoribbons and bulk silicon. The results are obtained through both density functional theory calculations and molecular dynamics simulations. This novel modulation strategy may pave the way for quantum heat conduction.

Modulating Carrier Dynamics in PdSe2: The Role of Pressure in Electronic and Phononic Interactions.

PdSe2 is a puckered transition metal dichalcogenide that has been reported to undergo a two-dimensional to three-dimensional structural transition under pressure. Here, we investigated the electronic and phononic evolution of PdSe2 under high pressure using pump-probe spectroscopy. We observed the electronic intraband and interband transitions occurring in the d orbitals of Pd, revealing the disappearance of the Jahn-Teller effect under high pressure. Furthermore, we found that the decay rates of interband recombination and intraband relaxation lifetimes change at 3 and 7 GPa, respectively. First-principles calculations suggest that the bandgap closure slows the decay rate of interband recombination after 3 GPa, while the saturation of phonon-phonon scattering is the main reason for the relatively constant intraband relaxation lifetime. Our work provides a novel perspective for understanding the evolution of the electron and modulation of the carrier dynamics by phonons under pressure.

Electron Drag Effect on Thermal Conductivity in Two-Dimensional Semiconductors.

Two-dimensional (2D) materials have shown great potential in applications as transistors, where thermal dissipation becomes crucial because of the increasing energy density. Although the thermal conductivity of 2D materials has been extensively studied, interactions between nonequilibrium electrons and phonons, which can be strong when high electric fields and heat current coexist, are not considered. In this work, we systematically study the electron drag effect, where nonequilibrium electrons impart momenta to phonons and influence the thermal conductivity, in 2D semiconductors using ab initio simulations. We find that, at room temperature, electron drag can significantly increase thermal conductivity by decreasing phonon-electron scattering in 2D semiconductors while its impact in three-dimensional semiconductors is negligible. We attribute this difference to the large electron-phonon scattering phase space and larger contribution to thermal conductivity by drag-active phonons. Our work elucidates the fundamental physics underlying coupled electron-phonon transport in materials of various dimensionalities.

Hole Relaxation Bottlenecks in CdSe/CdTe/CdSe Lateral Heterostructures Lead to Bicolor Emission.

Concentric lateral CdSe/CdTe/CdSe heterostructures show bicolor photoluminescence from both a red charge transfer band of the CdSe/CdTe interface and a green fluorescence from CdSe. This work uses visible and near-infrared transient spectroscopy measurements to demonstrate that the deviation from Kasha's rule arises from a hole relaxation bottleneck from CdSe to CdTe. Hole transfer can take up to 1 ns, which permits radiative relaxation of excitons remaining in CdSe. Simulations indicate that the hole relaxation bottleneck arises due to the sparse density of states and poor spatial overlap of hole states at energies near the CdSe band edge. The divergent kinetics of transfer for band edge and hot holes is exploited to vary the ratio of green and red photoluminescence with excitation wavelength, providing another knob to control emission color. These findings support the use of lateral heterojunctions as a method for slowing carrier relaxation in two-dimensional materials.

Infrared Resonance Raman of Bilayer Graphene: Signatures of Massive Fermions and Band Structure on the 2D Peak.

Few-layer graphene possesses low-energy carriers that behave as massive Fermions, exhibiting intriguing properties in both transport and light scattering experiments. Lowering the excitation energy of resonance Raman spectroscopy down to 1.17 eV, we target these massive quasiparticles in the split bands close to the K point. The low excitation energy weakens some of the Raman processes that are resonant in the visible, and induces a clearer frequency-separation of the substructures of the resonance 2D peak in bi- and trilayer samples. We follow the excitation-energy dependence of the intensity of each substructure, and comparing experimental measurements on bilayer graphene with ab initio theoretical calculations, we trace back such modifications on the joint effects of probing the electronic dispersion close to the band splitting and enhancement of electron-phonon matrix elements.