Predicting Spin-Dependent Phonon Band Structures of HKUST-1 Using Density Functional Theory and Machine-Learned Interatomic Potentials.

The present study focuses on the spin-dependent vibrational properties of HKUST-1, a metal-organic framework with potential applications in gas storage and separation. Employing density functional theory (DFT), we explore the consequences of spin couplings in the copper paddle wheels (as the secondary building units of HKUST-1) on the material's vibrational properties. By systematically screening the impact of the spin state on the phonon bands and densities of states in the various frequency regions, we identify asymmetric -COO- stretching vibrations as being most affected by different types of magnetic couplings. Notably, we also show that the DFT-derived insights can be quantitatively reproduced employing suitably parametrized, state-of-the-art machine-learned classical potentials with root-mean-square deviations from the DFT results between 3 cm-1 and 7 cm-1. This demonstrates the potential of machine-learned classical force fields for predicting the spin-dependent properties of complex materials, even when explicitly considering spins only for the generation of the reference data used in the force-field parametrization process.

Classification of cancer cells at the sub-cellular level by phonon microscopy using deep learning.

There is a consensus about the strong correlation between the elasticity of cells and tissue and their normal, dysplastic, and cancerous states. However, developments in cell mechanics have not seen significant progress in clinical applications. In this work, we explore the possibility of using phonon acoustics for this purpose. We used phonon microscopy to obtain a measure of the elastic properties between cancerous and normal breast cells. Utilising the raw time-resolved phonon-derived data (300 k individual inputs), we employed a deep learning technique to differentiate between MDA-MB-231 and MCF10a cell lines. We achieved a 93% accuracy using a single phonon measurement in a volume of approximately 2.5 µm3. We also investigated means for classification based on a physical model that suggest the presence of unidentified mechanical markers. We have successfully created a compact sensor design as a proof of principle, demonstrating its compatibility for use with needles and endoscopes, opening up exciting possibilities for future applications.

Hyperbolic polaritonic crystals with configurable low-symmetry Bloch modes.

Photonic crystals (PhCs) are a kind of artificial structures that can mold the flow of light at will. Polaritonic crystals (PoCs) made from polaritonic media offer a promising route to controlling nano-light at the subwavelength scale. Conventional bulk PhCs and recent van der Waals PoCs mainly show highly symmetric excitation of Bloch modes that closely rely on lattice orders. Here, we experimentally demonstrate a type of hyperbolic PoCs with configurable and low-symmetry deep-subwavelength Bloch modes that are robust against lattice rearrangement in certain directions. This is achieved by periodically perforating a natural crystal α-MoO3 that hosts in-plane hyperbolic phonon polaritons. The mode excitation and symmetry are controlled by the momentum matching between reciprocal lattice vectors and hyperbolic dispersions. We show that the Bloch modes and Bragg resonances of hyperbolic PoCs can be tuned through lattice scales and orientations while exhibiting robust properties immune to lattice rearrangement in the hyperbolic forbidden directions. Our findings provide insights into the physics of hyperbolic PoCs and expand the categories of PhCs, with potential applications in waveguiding, energy transfer, biosensing and quantum nano-optics.

Influence of CoFeB layer thickness on elastic parameters in CoFeB/MgO heterostructures.

The surface acoustic waves, i.e., surface phonons may have huge potential for future spintronic devices, if coupled to other waves (e.g., spin waves) or quasiparticles. In order to understand the coupling of acoustic phonons with the spin degree of freedom, especially in magnetic thin film-based heterostructures, one needs to investigate the properties of phonons in those heterostructures. This also allows us to determine the elastic properties of individual magnetic layers and the effective elastic parameters of the whole stacks. Here, we study frequency versus wavevector dispersion of thermally excited SAWs in CoFeB/MgO heterostructures with varying CoFeB thickness by employing Brillouin light spectroscopy. The experimental results are corroborated by finite element method-based simulations. From the best agreement of simulation results with the experiments, we find out the elastic tensor parameters for CoFeB layer. Additionally, we estimate the effective elastic parameters (elastic tensors, Young's modulus, Poisson's ratio) of the whole stacks for varying CoFeB thickness. Interestingly, the simulation results, either considering elastic parameters of individual layers or considering effective elastic parameters of whole stacks, show good agreement with the experimental results. These extracted elastic parameters will be very useful to understand the interaction of phonons with other quasiparticles.

Spin-phonon coupling in a double-stranded model of DNA.

We address the electron-spin-phonon coupling in an effective model Hamiltonian for DNA to assess its role in spin transfer involved in the Chiral-Induced Spin Selectivity (CISS) effect. The envelope function approach is used to describe semiclassical electron transfer in a tight-binding model of DNA at half filling in the presence of intrinsic spin-orbit coupling. Spin-phonon coupling arises from the orbital-configuration dependence of the spin-orbit interaction. We find spin-phonon coupling only for the acoustic modes, while the optical modes exhibit electron-phonon interaction without coupling to spin. We derive an effective Hamiltonian whose eigenstates carry spin currents that are protected by spin-inactive stretching optical modes. As optical phonons interact more strongly than acoustic phonons, side buckling and tilting optical base modes will be more strongly associated with decoherence, which allows for the two terminal spin filtering effects found in CISS.

Probing Enhanced Electron-Phonon Coupling in Graphene by Infrared Resonance Raman Spectroscopy.

We report on resonance Raman spectroscopy measurements with excitation photon energy down to 1.16 eV on graphene, to study how low-energy carriers interact with lattice vibrations. Thanks to the excitation energy close to the Dirac point at K, we unveil a giant increase of the intensity ratio between the double-resonant 2D and 2D^{'} peaks with respect to that measured in graphite. Comparing with fully ab initio theoretical calculations, we conclude that the observation is explained by an enhanced, momentum-dependent coupling between electrons and Brillouin zone-boundary optical phonons. This finding applies to two-dimensional Dirac systems and has important consequences for the modeling of transport in graphene devices operating at room temperature.

M-plane GaN terahertz quantum cascade laser structure design and doping effect for resonant-phonon and phonon-scattering-injection schemes.

Non-polar m-plane GaN terahertz quantum cascade laser (THz-QCL) structures have been studied. One is traditional three-well resonant-phonon (RP) design scheme. The other is two-well phonon scattering injection (PSI) design scheme. The peak gains of 41.8 and 44.2 cm-1 have been obtained at 8.2 and 7.7 THz respectively at 300 K according to the self-consistent non-equilibrium Green's function calculation. Different from the usual GaAs two-well design, the upper and lower lasing levels are both ground states in the GaN quantum wells for the PSI scheme, mitigating the severe broadening effect for the excited states in GaN. To guide the fabrication of such devices, the doping effect on the peak gain has been analyzed. The two designs have demonstrated distinct doping density dependence and it is mainly attributed to the very different doping dependent broadening behaviors. The results reveal the possibility of GaN based THz-QCL lasing at room temperature.

Temperature effects on the calculation of the functional derivative of Tc with respect to α2F(ω).

The functional derivative of the superconducting transition temperature Tc with respect to the electron-phonon coupling function [Formula: see text] permits identifying the frequency regions where phonons are most effective in raising Tc. This work presents an analysis of temperature effects on the calculation of the δTc/δα2F(ω) and µ* parameters. The results may permit establishing that the variation of the temperature in the δTc/δα2F(ω) and µ* parameter allows establishing patterns and conditions that are possibly related to the physical conditions in the superconducting state, with implications on the theoretical estimation of the Tc.

Spin current driven by ultrafast magnetization of FeRh.

Laser-induced ultrafast demagnetization is an important phenomenon that probes arguably the ultimate limits of the angular momentum dynamics in solid. Unfortunately, many aspects of the dynamics remain unclear except that the demagnetization transfers the angular momentum eventually to the lattice. In particular, the role and origin of electron-carried spin currents in the demagnetization process are debated. Here we experimentally probe the spin current in the opposite phenomenon, i.e., laser-induced ultrafast magnetization of FeRh, where the laser pump pulse initiates the angular momentum build-up rather than its dissipation. Using the time-resolved magneto-optical Kerr effect, we directly measure the ultrafast-magnetization-driven spin current in a FeRh/Cu heterostructure. A strong correlation between the spin current and the magnetization dynamics of FeRh is found even though the spin filter effect is negligible in this opposite process. This result implies that the angular momentum build-up is achieved by an angular momentum transfer from the electron bath (supplier) to the magnon bath (receiver) and followed by the spatial transport of angular momentum (spin current) and dissipation of angular momentum to the phonon bath (spin relaxation).

Controlling photons by phonons via giant atom in a waveguide QED setup.

We investigate the single photon scattering in a phonon-photon hybrid system in the waveguide quantum electrodynamics (QED) scheme. In our consideration, an artificial giant atom, which is dressed by the phonons in a surface acoustic wave resonator, interacts with a coupled resonator waveguide (CRW) nonlocally via two connecting sites. Together with the interference effect by the nonlocal coupling, the phonon serves as a controller to the transport of the photon in the waveguide. On the one hand, the coupling strength between the giant atom and the surface acoustic wave resonator modulates the width of the transmission valley or window in the near resonant regime. On the other hand, the two reflective peaks induced by the Rabi splitting degrade into a single one when the giant atom is large detuned from the surface acoustic resonator, which implies an effective dispersive coupling. Our study paves the way for the potential application of giant atoms in the hybrid system.

Laser2: A two-domain photon-phonon laser.

The laser is one of the greatest inventions in history. Because of its ubiquitous applications and profound societal impact, the concept of the laser has been extended to other physical domains including phonon lasers and atom lasers. Quite often, a laser in one physical domain is pumped by energy in another. However, all lasers demonstrated so far have only lased in one physical domain. We have experimentally demonstrated simultaneous photon and phonon lasing in a two-mode silica fiber ring cavity via forward intermodal stimulated Brillouin scattering (SBS) mediated by long-lived flexural acoustic waves. This two-domain laser may find potential applications in optical/acoustic tweezers, optomechanical sensing, microwave generation, and quantum information processing. Furthermore, we believe that this demonstration will usher in other multidomain lasers and related applications.

Ultrafast imaging of polariton propagation and interactions.

Semiconductor excitations can hybridize with cavity photons to form exciton-polaritons (EPs) with remarkable properties, including light-like energy flow combined with matter-like interactions. To fully harness these properties, EPs must retain ballistic, coherent transport despite matter-mediated interactions with lattice phonons. Here we develop a nonlinear momentum-resolved optical approach that directly images EPs in real space on femtosecond scales in a range of polaritonic architectures. We focus our analysis on EP propagation in layered halide perovskite microcavities. We reveal that EP-phonon interactions lead to a large renormalization of EP velocities at high excitonic fractions at room temperature. Despite these strong EP-phonon interactions, ballistic transport is maintained for up to half-exciton EPs, in agreement with quantum simulations of dynamic disorder shielding through light-matter hybridization. Above 50% excitonic character, rapid decoherence leads to diffusive transport. Our work provides a general framework to precisely balance EP coherence, velocity, and nonlinear interactions.

Effects of nonlinearity and a new nonlinear resonance in two-path phonon transmittance in lattices with two-dimensional arrays of atomic defects.

The paper is devoted to analytical and numerical studies of the effects of nonlinearity on the two-path phonon interference in the transmission through two-dimensional arrays of atomic defects embedded in a lattice. The emergence of transmission antiresonance (transmission node) in the two-path system is demonstrated for the few-particle nanostructures, which allow us to model both linear and nonlinear phonon transmission antiresonances. The universality of destructive-interference origin of transmission antiresonances of waves of different nature, such as phonons, photons, and electrons, in two-path nanostructures and metamaterials is emphasized. Generation of the higher harmonics as a result of the interaction of lattice waves with nonlinear two-path atomic defects is considered, and the full system of nonlinear algebraic equations is obtained to describe the transmission through nonlinear two-path atomic defects with an account for the generation of second and third harmonics. Expressions for the coefficients of lattice energy transmission through and reflection from the embedded nonlinear atomic systems are derived. It is shown that the quartic interatomic nonlinearity shifts the antiresonance frequency in the direction determined by the sign of the nonlinear coefficient and enhances in general the transmission of high-frequency phonons due to third harmonic generation and propagation. The effects of the quartic nonlinearity on phonon transmission are described for the two-path atomic defects with a different topology. Transmission through the nonlinear two-path atomic defects is also modeled with the simulation of the phonon wave packet, for which the proper amplitude normalization is proposed and implemented. It is shown that the cubic interatomic nonlinearity red shifts in general the antiresonance frequency for longitudinal phonons independently of the sign of the nonlinear coefficient, and the equilibrium interatomic distances (bond lengths) in the atomic defects are changed by the incident phonon due to cubic interatomic nonlinearity. For longitudinal phonons incident on a system with the cubic nonlinearity, the new narrow transmission resonance on the background of a broad antiresonance is predicted to emerge, which we relate to the opening of the additional transmission channel for the phonon second harmonic through the nonlinear defect atoms. Conditions of the existence of the new nonlinear transmission resonance are determined and demonstrated for different two-path nonlinear atomic defects. A two-dimensional array of embedded three-path defects with an additional weak transmission channel, in which a linear analog of the nonlinear narrow transmission resonance on the background of a broad antiresonance is realized, is proposed and modeled. The presented results provide better understanding and detailed description of the interplay between the interference and nonlinearity in phonon propagation through and scattering in two-dimensional arrays of two-path anharmonic atomic defects with a different topology.

Phonon transport along long polymer chains with varying configurations: Effects of phonon scattering.

Following recent molecular dynamic simulations [M. Dinpajooh and A. Nitzan, J. Chem. Phys. 153, 164903 (2020)], we theoretically analyze how the phonon heat transport along a single polymer chain may be affected by varying the chain configuration. We suggest that phonon scattering controls the phonon heat conduction in strongly compressed (and tangled) chain when multiple random bends act as scattering centers for vibrational phonon modes, which results in the diffusive character of heat transport. As the chain is straightening up, the number of scatterers decreases, and the heat transport acquires nearly ballistic character. To analyze these effects, we introduce a model of a long atomic chain made out of identical atoms where some atoms are put in contact with scatterers and treat the phonon heat transfer through such a system as a multichannel scattering problem. We simulate the changes in the chain configurations by varying the number of the scatterers and mimic a gradual straightening of the chain by a gradual reducing of the number of scatterers attached to the chain atoms. It is demonstrated, in agreement with recently published simulation results, that the phonon thermal conductance shows a threshold-like transition from the limit where nearly all atoms are attached to the scatterers to the opposite limit where the scatterers vanish, which corresponds to a transition from the diffusive to the ballistic phonon transport.

Evaluating strain and doping of Janus MoSSe from phonon mode shifts supported by ab initio DFT calculations.

With the study of Janus monolayer transition metal dichalcogenides, in which one of the two chalcogen layers is replaced by another type of chalcogen atom, research on two-dimensional materials is advancing into new areas. Yet only little is known about this new kind of material class, mainly due to the difficult synthesis. In this work, we synthesize MoSSe monolayers from exfoliated samples and compare their Raman signatures with density functional theory calculations of phonon modes that depend in a nontrivial way on doping and strain. With this as a tool, we can infer limits for the possible combinations of strain and doping levels. This reference data can be applied to all MoSSe Janus samples in order to quickly estimate their strain and doping, providing a reliable tool for future work. In order to narrow down the results for our samples further, we analyze the temperature-dependent photoluminescence spectra and time-correlated single-photon counting measurements. The lifetime of Janus MoSSe monolayers exhibits two decay processes with an average total lifetime of 1.57 ns. Moreover, we find a strong trion contribution to the photoluminescence spectra at low temperature which we attribute to excess charge carriers, corroborating our ab initio calculations.

Gate-Tunable Phonon Magnetic Moment in Bilayer Graphene.

We develop a first-principles quantum scheme to calculate the phonon magnetic moment in solids. As a showcase example, we apply our method to study gated bilayer graphene, a material with strong covalent bonds. According to the classical theory based on the Born effective charge, the phonon magnetic moment in this system should vanish, yet our quantum mechanical calculations find significant phonon magnetic moments. Furthermore, the magnetic moment is highly tunable by changing the gate voltage. Our results firmly establish the necessity of the quantum mechanical treatment, and identify small-gap covalent materials as a promising platform for studying tunable phonon magnetic moment.

Interaction-driven transport of dark excitons in 2D semiconductors with phonon-mediated optical readout.

The growing field of quantum information technology requires propagation of information over long distances with efficient readout mechanisms. Excitonic quantum fluids have emerged as a powerful platform for this task due to their straightforward electro-optical conversion. In two-dimensional transition metal dichalcogenides, the coupling between spin and valley provides exciting opportunities for harnessing, manipulating, and storing bits of information. However, the large inhomogeneity of single layers cannot be overcome by the properties of bright excitons, hindering spin-valley transport. Nonetheless, the rich band structure supports dark excitonic states with strong binding energy and longer lifetime, ideally suited for long-range transport. Here we show that dark excitons can diffuse over several micrometers and prove that this repulsion-driven propagation is robust across non-uniform samples. The long-range propagation of dark states with an optical readout mediated by chiral phonons provides a new concept of excitonic devices for applications in both classical and quantum information technology.

Chirality selective magnon-phonon hybridization and magnon-induced chiral phonons in a layered zigzag antiferromagnet.

Two-dimensional (2D) magnetic systems possess versatile magnetic order and can host tunable magnons carrying spin angular momenta. Recent advances show angular momentum can also be carried by lattice vibrations in the form of chiral phonons. However, the interplay between magnons and chiral phonons as well as the details of chiral phonon formation in a magnetic system are yet to be explored. Here, we report the observation of magnon-induced chiral phonons and chirality selective magnon-phonon hybridization in a layered zigzag antiferromagnet (AFM) FePSe3. With a combination of magneto-infrared and magneto-Raman spectroscopy, we observe chiral magnon polarons (chiMP), the new hybridized quasiparticles, at zero magnetic field. The hybridization gap reaches 0.25 meV and survives down to the quadrilayer limit. Via first principle calculations, we uncover a coherent coupling between AFM magnons and chiral phonons with parallel angular momenta, which arises from the underlying phonon and space group symmetries. This coupling lifts the chiral phonon degeneracy and gives rise to an unusual Raman circular polarization of the chiMP branches. The observation of coherent chiral spin-lattice excitations at zero magnetic field paves the way for angular momentum-based hybrid phononic and magnonic devices.

Nonlinear optical phonon spectroscopy revealing polaronic signatures of the LaAlO3/SrTiO3 interface.

We report the direct observation of lattice phonons confined at LaAlO3/SrTiO3 (LAO/STO) interfaces and STO surfaces using the sum-frequency phonon spectroscopy. This interface-specific nonlinear optical technique unveiled phonon modes localized within a few monolayers at the interface, with inherent sensitivity to the coupling between lattice and charge degrees of freedom. Spectral evolution across the insulator-to-metal transition at LAO/STO interface revealed an electronic reconstruction at the subcritical LAO thickness, as well as strong polaronic signatures upon formation of the two-dimensional electron gas. We further discovered a characteristic lattice mode from interfacial oxygen vacancies, enabling us to probe such important structural defects in situ. Our study provides a unique perspective on many-body interactions at the correlated oxide interfaces.

Verwey transition as evolution from electronic nematicity to trimerons via electron-phonon coupling.

Understanding the driving mechanisms behind metal-insulator transitions (MITs) is a critical step toward controlling material's properties. Since the proposal of charge order-induced MIT in magnetite Fe3O4 in 1939 by Verwey, the nature of the charge order and its role in the transition have remained elusive. Recently, a trimeron order was found in the low-temperature structure of Fe3O4; however, the expected transition entropy change in forming trimeron is greater than the observed value, which arises a reexamination of the ground state in the high-temperature phase. Here, we use electron diffraction to unveil that a nematic charge order on particular Fe sites emerges in the high-temperature structure of bulk Fe3O4 and that, upon cooling, a competitive intertwining of charge and lattice orders arouses the Verwey transition. Our findings discover an unconventional type of electronic nematicity in correlated materials and offer innovative insights into the transition mechanism in Fe3O4 via the electron-phonon coupling.