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 framework for the interpretation of UEDS signals, ultimately extracting the phonon mode occupancies across the entire Brillouin zone. These transient populations are then used to extract momentum- and mode-dependent electron-phonon and phonon-phonon coupling constants. Results of this analysis are presented for graphite, which provides complete information on the phonon-branch occupations and a determination of the $A_1'$ phonon mode-projected electron-phonon coupling strength $\langle g_{e,A_1'}^2 \rangle = 0.035 \pm 0.001$ eV$^2$ that is in agreement with other measurement techniques and simulations.
Time-domain femtosecond laser spectroscopic measurements of the ultrafast lattice dynamics in 2H-MoTe2 bulk crystals were carried out to understand the carrier-phonon interactions that govern electronic transport properties. An unusually long lifetime coherent A1g phonon mode was observed even in the presence of very large density of photo-excited carriers at room temperature. The decay rate was observed to decrease with increasing excitation laser fluence. Based on the laser fluence dependence including the inducement of significant phonon softening and a peculiar decrease in phonon decay rat…
Ultrafast dynamics of graphite is investigated by time-resolved photoemission spectroscopy. We observe spectral features of direct photoexcitations, non-thermal electron distributions, and recovery dynamics occurring with two time scales having distinct pump-power dependences. Additionally, we find an anomalous increase of the spectral intensity around the Fermi level, and we attribute this to spectral broadenings due to coupled optical phonons in the transient. The fingerprints of the coupled optical phonons occur from the temporal region where the electronic temperature is still not definabl…
We describe an ultrafast coherent control of the transient structural distortion arising from nonlinear phononics in ErFeO$_3$. Using density functional theory, we calculate the structural properties as input to an anharmonic phonon model that describes the response of the system to a pulsed optical excitation. We find that the trilinear coupling of two orthogonal infrared-active phonons to a Raman-active phonon causes a transient distortion of the lattice. The direction of the distortion is determined by the polarization of the exciting light, suggesting a route to nonlinear phononic lattice …
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 …
The magnetization response of bulk ferromagnets after excitation by an ultrashort optical pulse is calculated using a dynamical model of the Elliott-Yafet type that includes the effects of the spin-orbit interaction in the ab-initio ferromagnetic band structure, the electron-phonon interaction at the level of Boltzmann scattering integrals, and dynamical changes in the temperature of the phonon bath. Using realistic parameters for the ultrashort optical pulse, the computed maximum magnetization quenching achievable with electron-phonon scattering in a fixed band structure is much smaller than …
NaOH-reacted graphite oxide film was prepared by decomposing epoxy groups in graphite oxide into hydroxyl and -ONa groups with NaOH solution. Ultrafast carrier dynamics of the sample were studied by time-resolved transient differential reflection (\DeltaR/R). The data show two exponential relaxation processes. The slow relaxation process (\sim2ps) is ascribed to low energy acoustic phonon mediated scattering. The electron-phonon coupling and first-principles calculation results demonstrate that - OH and -ONa groups in the sample are strongly coupled. Thus, we attribute the fast relaxation proc…
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…
Despite their fundamental role in determining material properties, detailed momentum-dependent information on the strength of electron-phonon and phonon-phonon coupling (EPC and PPC, respectively) across the entire Brillouin zone (BZ) has proved difficult to obtain. Here we demonstrate that ultrafast electron diffuse scattering (UEDS) directly provides such information. By exploiting symmetry-based selection rules and time-resolution, scattering from different phonon branches can be distinguished even without energy resolution. Using graphite as a model system, we show that UEDS patterns map t…
We theoretically investigate spin-dependent carrier dynamics due to the electron-phonon interaction after ultrafast optical excitation in ferromagnetic metals. We calculate the electron-phonon matrix elements including the spin-orbit interaction in the electronic wave functions and the interaction potential. Using the matrix elements in Boltzmann scattering integrals, the momentum-resolved carrier distributions are obtained by solving their equation of motion numerically. We find that the optical excitation with realistic laser intensities alone leads to a negligible magnetization change, and …
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…
Ultrafast two-color pump-probe measurements, involving coherent acoustic phonon (CAP) waves, have provided information simultaneously on the mechanical properties and on the electronic structure of ferromagnetic GaMnAs. The elastic constant C11 of Ga1-xMnxAs (0.03<x<0.07) are observed to be systematically smaller than those of GaAs. Both C11 and Vs of GaMnAs are found to increase with temperature (78 K<T<295 K), again in contrast to the opposite behavior in GaAs. In addition, the fundamental bandgap (at E0 critical point) of Ga1-xMnxAs is found to shift slightly to higher energies with Mn conc…
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…
Ultrafast lattice dynamics of few quintuple layers of topological insulator (TI) Bi$_2$Te$_3$ is studied with time-resolved optical pump-probe spectroscopy. Both optical and acoustic phonons are photogenerated and detected. Here, in order to get new insights on the out-of-equilibrium electron-phonon coupling and phonons dynamics in confined TI, different nanostructures have been investigated (single or polycrystalline QLs assemblies and nano-crystallized islands). Contrary to previous literature claims, we show that even for nanostructures containing only 10 quintuple layers (QLs), the symmetr…
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…
Ultrafast optical excitation of gold-cobalt bilayers triggers the nontrivial interplay between the electronic, acoustic, and magnetic degrees of freedom. Laser-heated electrons generated at the gold-air interface diffuse through the layer of gold and strongly overheat the lattice in cobalt resulting in the emission of ultrashort acoustic pulses and generation of exchange-coupled magnons. Time-resolved optical measurements allow for extracting the thermal boundary (Kapitza) resistances at metal/metal interfaces and the hot electron diffusion length in ferromagnetic materials. Both the experimen…
We report the ultrafast dynamics of the 47.4 THz coherent phonons of graphite interacting with a photoinduced non-equilibrium electron-hole plasma. Unlike conventional materials, upon photoexcitation the phonon frequency of graphite upshifts, and within a few picoseconds relaxes to the stationary value. Our first-principles density functional calculations demonstrate that the phonon stiffening stems from the light-induced decoupling of the non-adiabatic electron-phonon interaction by creating the non-equilibrium electron-hole plasma. Time-resolved vibrational spectroscopy provides a window on …
The temperature evolution of GdFeCo electrons following optical heating plays a key role in all optical switching of GdFeCo and is primarily governed by the strength of coupling between electrons and phonons. Typically, the strength of electron-phonon coupling in a metal is deduced by monitoring changes in reflectance following optical heating and then analyzing the transient reflectance with a simple two-temperature thermal model. In a magnetic metal, the change in reflectance cannot be assumed to depend only the electron and phonon temperatures because a metal's reflectance also depends on t…
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 c…
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…
Radio-frequency compressed ultrafast electron diffraction has been used to probe the coherent and incoherent coupling of impulsive electronic excitation at 1.55 eV (800 nm) to optical and acoustic phonon modes directly from the perspective of the lattice degrees of freedom. A bi-exponential suppression of diffracted intensity due to relaxation of the electronic system into incoherent phonons is observed, with the 250 fs fast contribution dominated by coupling to the $E_{2g2}$ optical phonon mode at the $Γ$-point ($Γ-E_{2g2}$) and $A_1^{'}$ optical phonon mode at the $K$-point ($K-A_1^{'}$). Bo…
Ultrafast laser excitation of a metal causes correlated, highly nonequilibrium dynamics of electronic and ionic degrees of freedom, which are however only poorly captured by the widely-used two-temperature model. Here we develop an out-of-equilibrium theory that captures the full dynamic evolution of the electronic and phononic populations and provides a microscopic description of the transfer of energy delivered optically into electrons to the lattice. All essential nonequilibrium energy processes, such as electron-phonon and phonon-phonon interactions are taken into account. Moreover, as all…
We report femtosecond time-resolved reflectivity measurements of coherent phonons in tellurium performed over a wide range of temperatures (3K to 296K) and pump laser intensities. A totally symmetric A$_{1}$ coherent phonon at 3.6 THz responsible for the oscillations in the reflectivity data is observed to be strongly positively chirped (i.e, phonon time period decreases at longer pump-probe delay times) with increasing photoexcited carrier density, more so at lower temperatures. We show for the first time that the temperature dependence of the coherent phonon frequency is anomalous (i.e, incr…
We report the lattice dynamics of transition metal thin films by using the ultrafast electron diffraction. We observe a suppression of the diffraction intensity in a few picosecond after the photoexcitation, which is directly interpreted as the lattice heating via the electron-phonon interaction. The electron-phonon coupling constants for Au, Cu and Mo are quantitatively evaluated by employing the two-temperature model, which are consistent with those obtained by optical pump-probe methods. The variation in the lattice dynamics of the transition metals are systematically explained by the stren…
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…
Cold neutron scattering experiments have been performed to explore the energy, temperature, and wave-vector dependence of the diffuse scattering and the transverse acoustic (TA) phonons in the relaxor PbMg(1/3)Nb(2/3)O3. We have observed a weak, but definitive, diffuse scattering cross section above the Burns temperature T_d ~ 600 K. This cross section, which is most likely caused by chemical short-range order, persists down to 100 K, and coexists with the much stronger diffuse scattering that is attributed to the polar nanoregions. A systematic study of the TA phonon around (1, 1, 0) has also…
With the rapid advances in the development of nanotechnology, nowadays, the sizes of elementary unit, i.e. transistor, of micro- and nanoelectronic devices are well deep into nanoscale. For the pursuit of cheaper and faster nanoscale electronic devices, the size of transistors keeps scaling down. As the miniaturization of the nanoelectronic devices, the electrical resistivity increases dramatically, resulting rapid growth in the heat generation. The heat generation and limited thermal dissipation in nanoscale materials have become a critical problem in the development of the next generation na…
We investigate ultrafast demagnetization due to electron-phonon interaction in a model band-ferromagnet. We show that the microscopic mechanism behind the spin dynamics due to electron-phonon interaction is the interplay of scattering and the precession around momentum-dependent effective internal spin-orbit magnetic fields. The resulting magnetization dynamics can only be mimicked by spin-flip transitions if the spin precession around the internal fields is sufficiently fast (compared to the scattering time) so that it averages out the transverse spin components.
We analyze the effect of electron-phonon coupling on photoemission properties and ultrafast response of doped monolayer MoS2. The analysis is based on combined DFT and many-body (Eliashberg theory) approaches. In particular, we have calculated the electronic and phonon spectra, the electron-phonon coupling and the electronic spectral function of the system at different values of doping. We have also analyzed the emissive properties and the response of the system to femtosecond (fs) laser pulses. It is shown that position of the emission peak of undoped system is in agreement with the experimen…
We synthesize sub-THz longitudinal quasi-monochromatic acoustic phonons in a SrTiO$_3$ single crystal using a SrRuO$_3$/SrTiO$_3$ superlattice as an optical-acoustic transducer. The generated acoustic phonon spectrum is determined using ultrafast X-ray diffraction. The analysis of the generated phonon spectrum in the time domain reveals a k-vector dependent phonon lifetime. It is observed that even at sub-THz frequencies the phonon lifetime agrees with the 1/$ω^2$ power law known from Akhiezer's model for hyper sound attenuation. The observed shift of the synthesized spectrum to the higher $q$…
Time-resolved diffuse scattering experiments have gained increasing attention due to their potential to reveal non-equilibrium dynamics of crystal lattice vibrations with full momentum resolution. Although progress has been made in interpreting experimental data on the basis of one-phonon scattering, understanding the role of individual phonons can be sometimes hindered by multi-phonon excitations. In Ref. [{\it arXiv:2103.10108}] we have introduced a rigorous approach for the calculation of the all-phonon inelastic scattering intensity of solids from first-principles. In the present work, we …
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…
Raman scattering in relaxor ferroelectric PbMg1/3Ta2/3O3 (PMT) was investigated in the single crystalline form in the temperature range of 20 - 295 K. Anomalous temperature dependence of the integrated intensity and the Raman line contours were found at the diffuse phase transition. A correlation between the anomalies in the integrated intensities and the dispersion of the dielectric response was observed. The distortions of Raman lines with decreasing temperature are discussed.
We report a novel phenomenon in carbon nanotube (CNT) based devices, the transphonon effects, which resemble the transonic effects in aerodynamics. It is caused by dissipative resonance of nanotube phonons similar to the radial breathing mode, and subsequent drastic surge of the dragging force on the sliding tube, and multiple phonon barriers are encountered as the intertube sliding velocity reaches critical values. It is found that the transphonon effects can be tuned by applying geometric constraints or varying chirality combinations of the nanotubes.
Diffuse scattering is a rich source of information about disorder in crystalline materials, which can be modelled using atomistic techniques such as Monte Carlo and molecular dynamics simulations. Modern X-ray and neutron scattering instruments can rapidly measure large volumes of diffuse-scattering data. Unfortunately, current algorithms for atomistic diffuse-scattering calculations are too slow to model large data sets completely, because the fast Fourier transform (FFT) algorithm has long been considered unsuitable for such calculations [Butler & Welberry, J. Appl. Cryst. 25, 391 (1992)]. H…
Impulsive optical excitation can generate both coherent and squeezed phonons. The expectation value of the phonon displacement $<u_q>$ oscillates at the mode frequency for the coherent state but remains zero for a pure squeezed state. In contrast, both show oscillations in $<|u_q|^2>$ at twice the mode frequency. Therefore it can be difficult to distinguish them in a second-order measurement of the displacements, such as in first-order x-ray diffuse scattering. Here we demonstrate a simple method to distinguish squeezed from coherent atomic motion by measurement of the diffuse scattering follo…
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…
Thermal diffuse scattering in TEM: complex absorptive potentials compared to the frozen phonon model
Institute of Physical Engineering, Brno University of Technology（Brno理工大学物理工程学院）；Department of Physics and Astronomy, Uppsala University（乌普萨拉大学物理与天文学系）
Using ultrafast optical pump-probe spectroscopy, we study the relaxation dynamics of hot optical phonons in few-layer and multi-layer graphene films grown by epitaxy on silicon carbide substrates and by chemical vapor deposition on nickel substrates. In the first few hundred femtoseconds after photoexcitation, the hot carriers lose most of their energy to the generation of hot optical phonons which then present the main bottleneck to subsequent carrier cooling. Optical phonon cooling on short time scales is found to be independent of the graphene growth technique, the number of layers, and the…
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
We report GHz longitudinal as well as shear acoustic phonons photoexcitation and photodetection using femtosecond laser pulses in a spin-crossover molecular crystal. From our experimental observation of time domain Brillouin scattering triggered by the photoexcitation of acoustic waves across the low-spin (LS) to high-spin (HS) thermal crossover, we reveal a link between molecular spin state and photoexcitation of coherent GHz acoustic phonons. In particular, we experimentally evidence an unconventional non-thermal pathway for the laser excitation of GHz phonons. We also provide experimental i…
We study the ultrafast dynamics of surface electromagnetic waves photogenerated on aluminum film perforated with subwavelength holes array by means of transient photomodulation with 100 fs time resolution. We observed a pronounced blueshift of the resonant transmission band that reveals the important role of plasma attenuation in the dynamics and that is inconsistent with plasmon-polariton mechanism of extraordinary transmission. The transient photomodulation spectra were successfully modeled within the Boltzmann equation approach for the electron-phonon relaxation dynamics, involving non-equi…
