Phonon Wave Packets Research Articles

Picosecond Ultrasonics in Magnetic Topological Insulator MnBi2Te4.

MnBi2Te4 is a magnetic topological insulator with layered A-type antiferromagnetic order. It exhibits a rich layer- and magnetic-state dependent topological phase diagram; however, much about the coupling between spin, charge, and lattice remains to be explored. In this work, we report that MnBi2Te4 is an excellent acoustic phonon cavity by realizing phonon frequency combs using picosecond ultrasonics. With the generated acoustic phonon wavepackets, we demonstrate that the timing and phase of acoustic echoes can be used to detect the presence of stacking faults between van der Waals layers buried deep within the crystal. Furthermore, by implementing this nondestructive ultrafast optical measurement in conjunction with time-resolved magneto-optical Kerr effect experiments, we uncover that out-of-plane vibrations in MnBi2Te4 do not couple to the magnetic order, i.e. there is no appreciable magnetostriction. Our work points out how a well-developed technique can probe the structural defects and phonon pulse engineering in layered topological insulators.

Atomistic wave packet investigation of phonon scattering at rough surfaces

Investigating the phonon-surface scattering mechanism is essential for the evaluation of thermal transport in nanostructures. The theoretical description to quantify this mechanism remains to be developed at the atomic scale. This work presents a phonon wave packet method to study the phonon-surface scattering behavior at rough surfaces. We obtain the specularity distribution dependent on phonon polarization, wavelength, and surface roughness. The reflection of the diffuse wave packet is primarily attributed to the surface shadowing effect at a higher incident angle, surface disorder, and surface-induced localized modes. Taking the wavevector-dependent specularity data as input, the thermal conductivity of silicon nanowires is calculated based on the Boltzmann Transport Equation. Our specularity model provides an accurate evaluation for predicting thermal conductivity. This work offers an atomic-level analysis for phonon-surface interaction, which is helpful for the understanding of thermal transport in nanostructures.

On-chip phonon-magnon reservoir for neuromorphic computing

Reservoir computing is a concept involving mapping signals onto a high-dimensional phase space of a dynamical system called “reservoir” for subsequent recognition by an artificial neural network. We implement this concept in a nanodevice consisting of a sandwich of a semiconductor phonon waveguide and a patterned ferromagnetic layer. A pulsed write-laser encodes input signals into propagating phonon wavepackets, interacting with ferromagnetic magnons. The second laser reads the output signal reflecting a phase-sensitive mix of phonon and magnon modes, whose content is highly sensitive to the write- and read-laser positions. The reservoir efficiently separates the visual shapes drawn by the write-laser beam on the nanodevice surface in an area with a size comparable to a single pixel of a modern digital camera. Our finding suggests the phonon-magnon interaction as a promising hardware basis for realizing on-chip reservoir computing in future neuromorphic architectures.

Phonon Focusing Effect in an Atomic Level Triangular Structure

The rise of artificial microstructures has made it possible to modulate propagation of various kinds of waves, such as light, sound and heat. Among them, the focusing effect is a modulation function of particular interest. We propose an atomic level triangular structure to realize the phonon focusing effect in single-layer graphene. In the positive incident direction, our phonon wave packet simulation results confirm that multiple features related to the phonon focusing effect can be controlled by adjusting the height of the triangular structure. More interestingly, a completed different focusing pattern and an enhanced energy transmission coefficient are found in the reverse incident direction. The detailed mode conversion physics is discussed based on the Fourier transform analysis on the spatial distribution of the phonon wave packet. Our study provides physical insights to achieving phonon focusing effect by designing atomic level microstructures.

Imaging and controlling coherent phonon wave packets in single graphene nanoribbons

The motion of atoms is at the heart of any chemical or structural transformation in molecules and materials. Upon activation of this motion by an external source, several (usually many) vibrational modes can be coherently coupled, thus facilitating the chemical or structural phase transformation. These coherent dynamics occur on the ultrafast timescale, as revealed, e.g., by nonlocal ultrafast vibrational spectroscopic measurements in bulk molecular ensembles and solids. Tracking and controlling vibrational coherences locally at the atomic and molecular scales is, however, much more challenging and in fact has remained elusive so far. Here, we demonstrate that the vibrational coherences induced by broadband laser pulses on a single graphene nanoribbon (GNR) can be probed by femtosecond coherent anti-Stokes Raman spectroscopy (CARS) when performed in a scanning tunnelling microscope (STM). In addition to determining dephasing (~440 fs) and population decay times (~1.8 ps) of the generated phonon wave packets, we are able to track and control the corresponding quantum coherences, which we show to evolve on time scales as short as ~70 fs. We demonstrate that a two-dimensional frequency correlation spectrum unequivocally reveals the quantum couplings between different phonon modes in the GNR.

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 equationsis 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.

Coherent-Phonon-Driven Hot-Carrier Effect in a Superlattice Solar Cell

Carrier thermalization in a superlattice solar cell made of polar semiconductors is studied theoretically by considering a minimal model where electron-phonon scattering is the principal channel of carrier energy loss. Importantly, the effect of an intrinsic quantum mechanical property; the phonon coherence, on carrier thermalization is investigated, within semiclassical picture in terms of phonon wave packet. It turns out that coherent longitudinal optical (LO) phonons weaken the effective electron-phonon coupling, thus supposedly lowering the carrier energy loss rate in solar cell. The resulting thermalization power is indeed significantly reduced by the coherent phonons, resulting in enhanced hot carrier effect, particularly for thin enough well layer where carrier confinement is also strong. A recent experiment on superlattice solar cell prototype is shown to manifest the coherent phonons-driven phenomenon. Our results demonstrate the practical implications of the fundamental quantum coherence property of phonons in semiconductors for improving superlattice solar cell performance, via hot carrier effect.

Impact of interfacial compositional diffusion on interfacial phonon scattering and transmission in GaN/AlN heterostructure

Compositional diffusion at interfaces often occurs during the synthesis of heterostructures, which poses a significant challenge to the reliability and performance of heterostructure-based electronic devices. In this study, the effect of interfacial compositional diffusion on the interfacial phonon transport in GaN/AlN heterostructures has been explored using molecular dynamics and phonon dynamics simulations. It is found the compositional diffusion results in a remarkable reduction in the interfacial thermal conductance (ITC) of the heterostructures, which can be modulated by tuning the compositional diffusion thickness. Phonon wave packet simulations further revealed that the energy transmission coefficient across the interface is strongly phonon frequency-dependent and interfacial morphology-dependent, which is consistent well with the calculated ITC of the structures. The phonon mode conversion and phonon localization are observed at the region of interfaces. Furthermore, it is found that the longitudinal acoustic phonons are more sensitive to the compositional diffusion interface than transverse-acoustic phonons do. However, it is interesting to find that the energy transmission coefficients of transverse-acoustic phonons with a high frequency (above 3.6 THz) across the compositional interface are abnormally higher than those across the sharp interface due to the stronger phonon mode conversion in the compositional diffusion region, which provides additional pathways for energy transmission. Our findings provide a deeper insight into the interfacial phonon scattering and transmission under the coupling effect of interfacial morphology and compositional diffusion.

Thermal Transport Study in a Strained Carbon Nanotube and Graphene Junction Using Phonon Wavepacket Analysis

This study investigates single-mode phonon scattering from a junction structure consisting of a (6,6) single-walled carbon nanotube (SWCNT) and graphene, subject to mechanical deformation, using phonon wavepacket analysis. Results show that longitudinal acoustic (LA) and transverse acoustic (TA) phonons at low frequencies are transmitted more effectively through the SWCNT–graphene junction when the junction is deformed. As low-frequency phonons in LA and TA modes are major energy carriers, it is expected that thermal transport across the SWCNT–graphene junction will be more efficient when the junction is deformed. Interfacial thermal resistance across the SWCNT-graphene junction was calculated using reverse nonequilibrium molecular dynamics (RNEMD). The RNEMD results show that the interfacial thermal resistance decreases when the structure is elongated, deforming the junction between the SWCNT and graphene. However, there was no notable difference in the transmission of twisting (TW) and flexural (FO) phonons when the junction was deformed. The study also showed that the transmission of phonon energy through the SWCNT–graphene junction has a slight dependence on the group velocity of phonons, with phonons having higher group velocities transmitting the junction more effectively. The findings of this research will play a significant role in advancing the development of futuristic electronics by providing a tool for developing 3D carbon nanostructures with high thermal performance under mechanical deformation.

Observation of kinked soliton structure in realistic materials through wave packet simulations

In this work, we report the observation of a kinked structure in single-layer graphene through phonon wave packet simulations. The observed kinked structure agrees very well with the tanh-form solution of the soliton wave, and its group velocity increases with increasing kink amplitude, which suggests that the kinked structure has a soliton nature. This conclusion is further supported by the separate soliton wave packet simulations, in which consistent results with the phonon wave packet simulations are obtained. Our study provides a useful platform to study the soliton wave transport in realistic materials.

Launching Coherent Acoustic Phonon Wave Packets with Local Femtosecond Coulomb Forces.

Generation and manipulation of coherent acoustic phonons enables ultrafast control of solids and has been exploited for applications in various acoustic devices. We show that localized coherent acoustic phonon wave packets can be launched by ultrafast Coulomb forces in a scanning tunneling microscope (STM) using tip-enhanced terahertz electric fields. The wave packets propagate at the speed of the longitudinal acoustic phonon, creating standing waves up to 0.26THz for a 6.4nm thin Au film on mica. The ultrafast lattice displacement can be as large as 5pm and is precisely controlled by varying the tip-sample distance. This nonthermal femtosecond Coulomb-force-based excitation mechanism is applicable in nano-optomechanics for advanced terahertz engineering and opens new perspectives in exploiting coherent phonons at the atomic scale.

Femtosecond x-ray diffraction study of multi-THz coherent phonons in SrTiO3

We report generation of ultra-broadband longitudinal acoustic coherent phonon wavepackets in SrTiO3 (STO) with frequency components extending throughout the first Brillouin zone. The wavepackets are efficiently generated in STO using femtosecond infrared laser excitation of an atomically flat 1.6 nm-thick epitaxial SrRuO3 film. We use femtosecond x-ray diffraction at the European X-Ray Free Electron Laser Facility to study the dispersion and damping of phonon wavepackets. The experimentally determined damping constants for multi-THz frequency phonons compare favorably to the extrapolation of a simple ultrasound damping model over several orders of magnitude.

Resonant and phonon-assisted ultrafast coherent control of a single hBN color center

Single-photon emitters in solid-state systems are important building blocks for scalable quantum technologies. Recently, quantum light emitters have been discovered in the wide-gap van der Waals insulator hexagonal boron nitride (hBN). These color centers have attracted considerable attention due to their quantum performance at elevated temperatures and wide range of transition energies. Here, we demonstrate coherent state manipulation of a single hBN color center with ultrafast laser pulses and investigate in our joint experiment–theory study the coupling between the electronic system and phonons. We demonstrate that coherent control can be performed not only resonantly on the optical transition giving access to the decoherence but also phonon-assisted, which reveals the internal phonon quantum dynamics. In the case of optical phonons, we measure their decoherence, stemming in part from their anharmonic decay. Dephasing induced by the creation of acoustic phonons manifests as a rapid decrease in the coherent control signal when traveling phonon wave packets are emitted. Furthermore, we demonstrate that the quantum superposition between a phonon-assisted process and resonant excitation causes ultrafast oscillations of the coherent control signal. Our results pave the way for ultrafast phonon quantum state control on the nanoscale and open up a new promising perspective for hybrid quantum technologies.

Phonon Wave Packet Emission during State Preparation of a Semiconductor Quantum Dot using Different Schemes

The carrier–phonon interaction in semiconductor quantum dots (QDs) can greatly affect the optical preparation of the excited state. For resonant excitation used in the Rabi preparation scheme, the polaron is formed accompanied by the emission of a phonon wave packet, leading to a degradation of preparation fidelity. In this article, phonon wave packets for different coherent excitation schemes are analyzed. One example is the adiabatic rapid passage scheme relying on a chirped excitation. Herein, also a phonon wave packet is emitted, but the preparation fidelity can still be approximately unity. A focus is on the phonon impact on a recently proposed swing‐up scheme, induced by two detuned pulses. Similar to the Rabi scheme, a degradation and a phonon wave packet emission are found, despite the detuning. If the swing‐up frequency coincides with the maximum of the phonon spectral density, a series of wave packets is emitted yielding an even stronger degradation. The insight gained from our results further helps in designing an optimal preparation scheme for QDs.

Structure and lattice thermal conductivity of grain boundaries in silicon by using machine learning potential and molecular dynamics

In silicon, lattice thermal conductivity plays an important role in a wide range of applications such as thermoelectric and microelectronic devices. Grain boundaries (GBs) in polycrystalline silicon can significantly reduce lattice thermal conductivity, but the impact of GB atomic structures on it remains to be elucidated. This study demonstrates accurate predictions of the GB structures, GB energies, and GB phonon properties in silicon using machine learning potentials (MLPs). The results indicate that the MLPs enable robust GB structure searches owing to the fact that the MLPs were developed from a training dataset covering a wide variety of structures. We also investigate lattice thermal conduction at four GB atomic structures using large-scale perturbed molecular dynamics and phonon wave-packet simulations. The comparison of these results indicates that the GB structure dependence of thermal conductivity stems from anharmonic vibrations at GBs rather than from the phonon transmission behavior at GBs. The advantages of the MLPs compared with a typical empirical potential of silicon are also thoroughly investigated.

Moving window techniques to model shock wave propagation using the concurrent atomistic–continuum method

Atomistic methods have successfully modeled different aspects of shock wave propagation in materials over the past several decades, but they suffer from limitations which restrict the total runtime and system size. Multiscale methods have been able to increase the length and time scales that can be modeled but employing such schemes to simulate wave propagation and evolution through engineering-scale domains is an active area of research. In this work, we develop two distinct moving window approaches within a Concurrent Atomistic–Continuum (CAC) framework to model shock wave propagation through a one-dimensional monatomic chain. In the first method, the entire CAC system travels with the shock in a conveyor fashion and maintains the shock front in the middle of the overall domain. In the second method, the atomistic region follows the shock by the simultaneous coarsening and refinement of the continuum regions. The CAC and moving window frameworks are verified through dispersion relation studies and phonon wave packet tests. We achieve good agreement between the simulated shock velocities and the values obtained from theory with the conveyor technique, while the coarsen-refine technique allows us to follow the propagating wave front through a large-scale domain. This work showcases the ability of the CAC method to accurately simulate propagating shocks and also demonstrates how a moving window technique can be used in a multiscale framework to study highly nonlinear, transient phenomena.

Evidence of phonon Anderson localization on the thermal properties of disordered atomic systems

Localization is a well-known wave phenomenon that significantly impedes transport, as uncovered by a pioneering work of Anderson. The localization of thermal phonons based on the phonon wave nature is widely represented in disordered atomic systems. Compared with electron and photon localization, the observations of phonon localization are much rarer, owning to the broadband nature of phonon thermal transport. In this Perspective, we summarize the experimental and theoretical evidences of phonon Anderson localization in disordered atomic systems from the aspects of vibrational spectroscopy, thermal conductivity measurement, phonon transmission, phonon wave packet, phonon participation ratio, and energy distribution.

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 behaviors can be dominated by interfaces and their atomic structures; 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 ultralow temperatures, however, knowledge is missing regarding athermal phonon behavior due to the challenge in modeling the extreme conditions in microscale, heterogeneous cryogenic systems, as well as extracting single-phonon information from a large ensemble. In this paper, we delineate the effects of interfacial atomic structures on 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---$(1\ifmmode\times\else\texttimes\fi{}1), (\sqrt{3}\ifmmode\times\else\texttimes\fi{}\sqrt{3})$ and $(7\ifmmode\times\else\texttimes\fi{}7)$---and model both experimentally observed $\mathrm{Si}(1\ifmmode\times\else\texttimes\fi{}1)/\mathrm{Al}$ interfaces and hypothesized $\mathrm{Si}(\sqrt{3}\ifmmode\times\else\texttimes\fi{}\sqrt{3})$/Al and $\mathrm{Si}(7\ifmmode\times\else\texttimes\fi{}7)/\mathrm{Al}$ interfaces. The overall interfacial thermal conductance calculated from non-equilibrium MD shows that for the $\mathrm{Si}(1\ifmmode\times\else\texttimes\fi{}1)/\mathrm{Al}$ system, the presence of Al twin boundaries can hinder phonon transport and reduce thermal conductance by 2--12% relative to single-crystal Al; whereas the Si $(\sqrt{3}\ifmmode\times\else\texttimes\fi{}\sqrt{3})$ and $(7\ifmmode\times\else\texttimes\fi{}7)$ 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 predict phonon transport properties consistent with non-equilibrium MD, 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 avenues for achieving selective phonon transport via controlling interfacial structures of materials using 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.

Coherent phonon detection gated by transient spin-polarized electrons

Manipulating electron spins on ultrashort timescales shows promise in the field of data processing. Because of the direct electron-photon coupling, photons have been widely used for such studies, but not phonons. Here we tie coherent phonon detection to transient spin populations. We optically excite gigahertz picosecond phonon wave packets in a metal-coated GaAs slab containing $\mathrm{GaAs}\text{/}{\mathrm{Al}}_{0.4}{\mathrm{Ga}}_{0.6}\mathrm{As}$ multiple quantum wells on the opposite side. Before the phonon wave-packet arrival, circularly polarized light induces a transient spin polarization. Phonon-induced ultrafast polarization rotation and reflectivity changes contingent on the transient spin population are detected by a heterodyne modulation technique. With an analytical model, we posit the presence of significant second-order interactions, enabled by spins, in the coherent-phonon optical detection. Applications include transient spin population monitoring and novel spintronic nanodevices.

Phonon wave-packet simulations using the quantized definition of energy and a temperature-dependent phonon dispersion relation and phonon density of states.

Wave-packet simulations, regarded as phonon dynamics in the literature, have been used to explore interface conductance problems and to study the frequency-based dynamics of systems of particles. In this work we introduce an extension of the method to improve the postsimulation analysis and to add an energy aspect to the definition of a wave packet. In a wave-packet simulation the most populated frequency activated with the wave packet is known through knowledge of the wave number implemented in the atom displacement equation. The one-to-one correspondence of wave number and frequency is known through the phonon dispersion relation (PDR). We add the temperature dependence of this one-to-one correspondence to the analysis of wave packets through consideration of a temperature-dependent PDR and showed the importance of the temperature-dependent PDR in the wave-packet definition by presenting results considering and neglecting the phenomenon. In addition, the temperature-dependent PDR and the density of states provide us the chance to change the nature of the atomic displacement amplitude as an arbitrary parameter to a tuning knob for the amount of energy it carries and utilize the chance to provide a quantitative measure for the validity of molecular-dynamics simulations considering their classical nature in comparison with the quantum particle picture of phonons.