In the past decade, the advent of time-resolved spectroscopic tools has provided a new ground to explore fundamental interactions in solids and to disentangle degrees of freedom whose coupling leads to broad structures in the frequency domain. Time- and angle-resolved photoemission spectroscopy (tr-ARPES) has been utilized to directly study the relaxation dynamics of a metal in the presence of electron-phonon coupling. The effect of photo-excitations on the real and imaginary part of the self-energy as well as the time scale associated with different recombination processes are discussed. In contrast to a theoretical model, the phonon energy does not set a clear scale governing quasiparticle dynamics, which is also different from the results observed in a superconducting material. These results point to the need for a more complete theoretical framework to understand electron-phonon interaction in a photo-excited state.
Identifying an efficient pathway to change the order parameter via a subtle excitation of the coupled high-frequency mode is the ultimate goal of the field of ultrafast phase transitions. This is an especially interesting research direction in magnetism, where the coupling between spin and lattice excitations is required for magnetization reversal. Despite several attempts however, the switching between magnetic states via resonant pumping of phonon modes has not yet been demonstrated. Here we show how an ultrafast resonant excitation of the longitudinal optical phonon modes in magnetic garnet…
We investigate ultrafast phonon dynamics in the Bi$_{1-x}$Sb$_{x}$ alloy system for various compositions $x$ using a reflective femtosecond pump-probe technique. The coherent optical phonons corresponding to the A$_{1g}$ local vibrational modes of Bi-Bi, Bi-Sb, and Sb-Sb are generated and observed in the time domain with a few picoseconds dephasing time. The frequencies of the coherent optical phonons were found to change as the Sb composition $x$ was varied, and more importantly, the relaxation time of those phonon modes was dramatically reduced for $x$ values in the range 0.5--0.8. We argue …
Despite intense experimental effort, theoretical proposals and modeling approaches, a lack of consensus exists about the intrinsic mechanisms driving ultrafast magnetization dynamics in 3$d$ ferromagnets. In this work, we find evidence of electron-phonon mediated spin-flip as the driving mechanism for the ultrafast magnetization dynamics in all three 3$d$ ferromagnets; nickel, iron and cobalt. We use a microscopic three temperature model with parameters calculated from first-principles, which has been validated by direct comparison to the electron and lattice dynamics extracted from previous e…
We use theory and first-principles calculations to investigate how structural changes induced by ultrafast optical excitation of infrared-active phonons change with hydrostatic pressure in LaAlO$_3$. Our calculations show that the observed structural changes are sensitive to pressure, with the largest changes occurring at pressures near the boundary between the cubic perovskite and rhombohedral phases. We rationalize our findings by defining a figure of merit that depends only on intrinsic materials quantities, and show that the peak response near the phase boundary is dictated by different mi…
One central challenge in understanding phonon thermal transport is a lack of experimental tools to investigate mode-based transport information. Although recent advances in computation lead to mode-based information, it is hindered by unknown defects in bulk region and at interfaces. Here we present a framework that can reveal microscopic phonon transport information in heterostructures, integrating state-of-the-art ultrafast electron diffraction (UED) with advanced scientific machine learning. Taking advantage of the dual temporal and reciprocal-space resolution in UED, we are able to reliabl…
Chiral Phonons Enable Ultrafast Magnetization Switching via Magnetoelastic Coupling
Nanjing University of Aeronautics and Astronautics (NUAA)（南京航空航天大学）；Instituto de Ciencia de Materiales de Madrid (ICMM), CSIC（马德里材料科学研究所，西班牙国家科学研究委员会）；The University of Manchester（曼彻斯特大学）；University of York（约克大学）
The out-of-equilibrium dynamics of electrons and phonons upon laser excitation are often described by the two-temperature model, which assumes that both subsystems are separately in thermal equilibrium. However, recent experiments show that this description is not sufficient to describe the out-of-equilibrium dynamics on ultrashort timescales. Here, we extend and apply a parameter-free microscopic out-of-equilibrium model to describe the ultrafast laser-induced system dynamics of archetypical metallic systems such as gold, aluminum, iron, nickel, and cobalt. We report strong deviations from th…
The interaction between lattice and spins is at the heart of an extremely intriguing ultrafast dynamics in magnetic materials. In this work we formulate a general non-equilibrium theory that disentangles the complex interplay between them in a THz laser-excited antiferromagnetic insulator. The theory provides a quantitative description of the transient energy flow between the spin and lattice sub-systems, subject to magnon-phonon and phonon-phonon scatterings, giving rise to finite life-times of the quasiparticles and to the equilibration time of the system. We predict a novel kind of scatteri…
Interactions between the lattice and charge carriers can drive the formation of phases and ordering phenomena that give rise to conventional superconductivity, insulator-to-metal transitions, and charge-density waves. These couplings also play a determining role in properties that include electric and thermal conductivity. Ultrafast electron diffuse scattering (UEDS) has recently become a viable laboratory-scale tool to track energy flow into and within the lattice system across the entire Brillouin zone, and deconvolves interactions in the time domain. Here, we present a detailed quantitative…
Generalized thermodynamic closure in ultrafast phonon dynamics
Max-Planck Institute for Polymer Research（马克斯·普朗克聚合物研究所）；Pohang University of Science and Technology（浦项科技大学）；Leiden University（莱顿大学）；Helmholtz-Zentrum Dresden-Rossendorf（德累斯顿-罗斯多夫亥姆霍兹中心）
This study investigates the ultrafast dynamics of coherent phonons and phonon-polaritons in lithium niobate (LiNbO$_{3}$) crystals using reflective pump-probe spectroscopy with 25-fs time resolution. In addition to several coherent optical phonon modes, the electro-optic sampling measurements explored the coexistence of phonon-polariton E-modes near 3.8 and 14.9 THz, which agrees considerably with the theoretical phonon-polariton dispersion curves. We also discovered that a time lag ($Δ$t $\approx$ 0.2 ps) between the coherent optical phonon and phonon-polariton originates from the coupling ti…
The ultrafast dynamics of magnetic order in a ferromagnet are governed by the interplay between electronic, magnetic and lattice degrees of freedom. In order to obtain a microscopic understanding of ultrafast demagnetization, information on the response of all three subsystems is required. A consistent description of demagnetization and microscopic energy flow, however, is still missing. Here, we combine a femtosecond electron diffraction study of the ultrafast lattice response of nickel to laser excitation with ab initio calculations of the electron-phonon interaction and energy-conserving at…
Electron-phonon interaction during optically induced ultrafast magnetization dynamics of Au/GdFeCo bilayers
光加热后GdFeCo电子的温度演化在GdFeCo的全光开关中起着关键作用，并且主要由电子和声子之间的耦合强度决定。通常，金属中的电子-声子耦合的强度是通过监测光加热后反射率的变化，然后用一个简单的双温度热模型分析瞬态反射率来推导的。在磁性金属中，不能假设反射率的变化仅取决于电子和声子温度，因为金属的反射率也取决于磁化强度。为了推导GdFeCo中的电子-声子耦合常数，我们分析了GdFeCo电子在光加热后Au和GdFeCo双层膜中的热输运。我们利用Au层的反射率来监测Au声子的温度演化。通过用热模型解释双层膜对加热的响应，我们确定GdFeCo中的电子-声子耦合常数为6 x 10^17 W/（m^3-K），对应于GdFeCo中的电子-声子弛豫时间约为150 fs。
We observe pronounced oscillations in differential reflectivity of 9 nm and 60 nm BaFe\textsubscript{2}As\textsubscript{2} (Ba-122) thin films using ultrafast optical spectroscopy. Our studies show that the oscillations result from propagating longitudinal acoustic (LA) phonon wave packets with strong thickness and temperature dependence. Particularly, the experimentally measured oscillation frequency approaches to 50 GHz for the ultra-thin film. Our calculations show that Young's modulus of 9 nm thin film is nearly four times as large as that of 60 nm thin film, consistent with the experiment…
Recent investigations have advanced the understanding of how structure-property relationships in ferromagnetic metal alloys affect the magnetization dynamics on nanosecond time-scales. A similar understanding for magnetization dynamics on femto- to pico-second time-scales does not yet exist. To address this, we perform time-resolved magneto optic Kerr effect (TRMOKE) measurements of magnetization dynamics in Co-Fe alloys on femto- to nano-second regimes. We show that Co-Fe compositions that exhibit low Gilbert damping parameters also feature prolonged ultrafast demagnetization upon photoexcita…
Our examination of the interplay of ultrafast charge dynamics and electron-phonon interaction in bilayer MoS2 provides a microscopic basis for understanding the features (two peaks) in the emission spectrum. We demonstrate that while the initial accumulation of excited charge occurs at and near the Q point of the two-dimensional Brillioun zone, emission takes place predominantly through two pathways: direct charge recombination at the K point and indirect phonon-assisted recombination of electrons at the K valley and holes at Γ hill of the Brillouin zone. Analysis of the wave vector dependenci…
The zone-center $E_{2g}$ modes play a crucial role in MgB$_2$, controlling the scattering mechanisms in the normal state as well the superconducting pairing. Here, we demonstrate via first-principles quantum-field theory calculations that, due to the anisotropic electron-phonon interaction, a $hot$-$phonon$ regime where the $E_{2g}$ phonons can achieve significantly larger effective populations than other modes, is triggered in MgB$_2$ by the interaction with an ultra-short laser pulse. Spectral signatures of this scenario in ultrafast pump-probe Raman spectroscopy are discussed in detail, rev…
Charge transfer between photoexcited quantum dots and molecular acceptors is one of the key limiting processes in most applications of colloidal nanostructures, most prominently in photovoltaics. An atomistic detailed description of this process would open new ways to optimize existing and create new structures with targeted properties. We achieve a one-to-one comparison between ab-initio non-adiabatic molecular dynamics calculations and transient absorption spectroscopy experiments, which allows us to draw a comprehensive atomistic picture of the charge transfer process, following the time ev…
Here we report an ultrafast optical spectroscopic study of the nodal-line semimetal ZrSiTe. Our measurements reveal that, converse to other compounds of the family, the sudden injection of electronic excitations results in a strongly coherent response of an $A_{1g}$ phonon mode which dynamically modifies the distance between Zr and Te atoms and Si layers. "Frozen phonon" DFT calculations, in which band structures are calculated as a function of nuclear position along the phonon mode coordinate, show that large displacements along this mode alter the material's electronic structure significantl…
Femtosecond laser excitation of solid-state systems creates non-equilibrium hot electrons that cool down by transferring their energy to other degrees of freedom and ultimately to lattice vibrations of the solid. By combining ab initio calculations with ultrafast diffuse electron scattering we gain a detailed understanding of the complex non-equilibrium energy transfer between electrons and phonons in laser-excited Ni metal. Our experimental results show that the wavevector resolved population dynamics of phonon modes is distinctly different throughout the Brillouin zone and are in remarkable …
Perturbo is a software package for first-principles calculations of charge transport and ultrafast carrier dynamics in materials. The current version focuses on electron-phonon interactions and can compute phonon-limited transport properties such as the conductivity, carrier mobility and Seebeck coefficient. It can also simulate the ultrafast nonequilibrium electron dynamics in the presence of electron-phonon scattering. Perturbo uses results from density functional theory and density functional perturbation theory calculations as input, and employs Wannier interpolation to reduce the computat…
High-resolution angle-resolved photoemission spectroscopy and ultrafast optical pump-probe spectroscopy were used to study semimetallic 1T - TiTe2 quasiparticle dispersion and dynamics. A kink and a flat band, having the same energy scale and temperature-dependent behaviors along the G-M direction, were detected. Both manifested at low temperatures but blurred as temperature increased. The kink was formed by an electron-phonon coupling. And the localized flat band might be closely related to an electron-phonon coupling. Ultrafast optical spectroscopy identified multiple distinct time scales in…
Ultrafast spectroscopies can access the dynamics of electrons and nuclei at short timescales, shedding light on nonequilibrium phenomena in materials. However, development of accurate calculations to interpret these experiments has lagged behind as widely adopted simulation schemes are limited to sub-picosecond timescales or employ simplified interactions lacking quantitative accuracy. Here we show a precise approach to obtain the time-dependent populations of nonequilibrium electrons and atomic vibrations (phonons) up to tens of picoseconds, with a femtosecond time resolution. Combining first…
Precision-controlled ultrafast electron microscope platforms. A case study: Multiple-order coherent phonon dynamics in 1T-TaSe$_2$ probed at 50 femtosecond - 10 femtometer scales
Quantitative knowledge of electron-phonon coupling is important for many applications as well as for the fundamental understanding of nonequilibrium relaxation processes. Time-resolved diffraction provides direct access to this knowledge through its sensitivity to laser-induced lattice dynamics. Here, we present an approach for analyzing time-resolved polycrystalline diffraction data. A two-step routine is used to minimize the number of time-dependent fit parameters. The lattice dynamics are extracted by finding the best fit to the full transient diffraction pattern rather than by analyzing tr…
Ultrafast optical control of ferroelectricity using intense terahertz fields has attracted significant interest. Here we show that the nonlinear interactions between two optical phonons in SnTe, a two-dimensional in-plane ferroelectric material, enables a dynamical amplification of the electric polarization within subpicoseconds time domain. Our first principles time dependent simulations show that the infrared-active out-of-plane phonon mode, pumped to nonlinear regimes, spontaneously generates in-plane motions, leading to rectified oscillations in the in-plane electric polarization. We sugge…
Exciton-phonon coupling induces new pathway for ultrafast intralayer-to-interlayer exciton transition and interlayer charge transfer in WS2-MoS2 heterostructure: a first-principles study
