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Layered ternary type‐II Weyl semimetals demonstrate promising applications in high‐performance and broadband optoelectronics, therefore it is crucial to gain insights into their photocarriers' dynamics. In this work, the probing polarization dependence of non‐equilibrium dynamics in NbIrTe4 is investigated by using transient reflectivity spectroscopy. Following photoexcitation at 3.18 eV, the dynamical response of 1.59 eV probe pulse exhibits a strong dependence on probe polarization. The relaxation comprises two components: a rapid recovery of ≈0.6 ps attributed to the electron–phonon scattering, and an anomalous slow recovery spanning hundreds of picoseconds attributed to the photoinduced quasi‐particle. The polarization dependence of rapid relaxation time τ is indicative of the in‐plane anisotropy of electron–phonon coupling in NbIrTe4. The slow relaxation modulated by a latest reported 16 cm−1 coherent phonon also shows strong probing polarization dependence, further revealing the anisotropic nature of electron–phonon coupling and the possibility of anisotropic lattice distortion, as well as photoinduced polaron, under ultrafast photoexcitation in NbIrTe4. The dynamical anisotropy in NbIrTe4 has provided valuable guidance for the application of NbIrTe4 in polarization‐sensitive nonlinear optics or optoelectronic devices and offers insights into the unique carrier transport as well as phonon transport properties of this newly established topological material. [ABSTRACT FROM AUTHOR]

Layered ternary type‐II Weyl semimetals demonstrate promising applications in high‐performance and broadband optoelectronics, therefore it is crucial to gain insights into their photocarriers' dynamics. In this work, the probing polarization dependence of non‐equilibrium dynamics in NbIrTe4 is investigated by using transient reflectivity spectroscopy. Following photoexcitation at 3.18 eV, the dynamical response of 1.59 eV probe pulse exhibits a strong dependence on probe polarization. The relaxation comprises two components: a rapid recovery of ≈0.6 ps attributed to the electron–phonon scattering, and an anomalous slow recovery spanning hundreds of picoseconds attributed to the photoinduced quasi‐particle. The polarization dependence of rapid relaxation time τ is indicative of the in‐plane anisotropy of electron–phonon coupling in NbIrTe4. The slow relaxation modulated by a latest reported 16 cm−1 coherent phonon also shows strong probing polarization dependence, further revealing the anisotropic nature of electron–phonon coupling and the possibility of anisotropic lattice distortion, as well as photoinduced polaron, under ultrafast photoexcitation in NbIrTe4. The dynamical anisotropy in NbIrTe4 has provided valuable guidance for the application of NbIrTe4 in polarization‐sensitive nonlinear optics or optoelectronic devices and offers insights into the unique carrier transport as well as phonon transport properties of this newly established topological material. [ABSTRACT FROM AUTHOR]

In this article, we investigate the coherent A1g phonon mode in bismuth crystal using transient reflectivity measurements, focusing on two distinct crystallographic orientations: one with the principal axis ((1 1 1)-direction in the trigonal cell representation) perpendicular to the sample surface, and the other with the principal axis parallel to the surface. Our results demonstrate significant variations in the amplitude, frequency, and lifetime of the coherent phonon mode between these two orientations, even when identical pumping and probing conditions are applied. We attribute these differences to the anisotropy of the electron effective mass, which influences electron mobility and, in turn, affects the phonon dynamics in bismuth. [ABSTRACT FROM AUTHOR]

Organic-inorganic layered perovskites, or Ruddlesden-Popper perovskites, are two-dimensional quantum wells with layers of lead-halide octahedra stacked between organic ligand barriers. The combination of their dielectric confinement and ionic sublattice results in excitonic excitations with substantial binding energies that are strongly coupled to the surrounding soft, polar lattice. However, the ligand environment in layered perovskites can significantly alter their optical properties due to the complex dynamic disorder of the soft perovskite lattice. Here, we infer dynamic disorder through phonon dephasing lifetimes initiated by resonant impulsive stimulated Raman photoexcitation followed by transient absorption probing for a variety of ligand substitutions. We demonstrate that vibrational relaxation in layered perovskite formed from flexible alkyl-amines as organic barriers is fast and relatively independent of the lattice temperature. Relaxation in layered perovskites spaced by aromatic amines is slower, although still fast relative to bulk inorganic lead bromide lattices, with a rate that is temperature dependent. Using molecular dynamics simulations, we explain the fast rates of relaxation by quantifying the large anharmonic coupling of the optical modes with the ligand layers and rationalize the temperature independence due to their amorphous packing. This work provides a molecular and time-domain depiction of the relaxation of nascent optical excitations and opens opportunities to understand how they couple to the complex layered perovskite lattice, elucidating design principles for optoelectronic devices.

Birefringence, which modulates the polarization of electromagnetic wave, has been commercially developed and widely used in modern photonics. Fostered by high-frequency signal processing and communications, feasible birefringence technologies operating in gigahertz (GHz) range are highly desired. Here, a coherent phonon-induced GHz optical birefringence and its manipulation in SrTiO3 (STO) crystals are demonsrated. With ultrafast laser pumping, the coherent acoustic phonons with low damping are created in the transducer/STO structures. A series of transducer layers are examined and the optimized one with relatively high photon-phonon conversion efficiency, i.e., semiconducting LaRhO3 film, is obtained. The most intriguing finding here is that, by virtue of high sensitivity to strain perturbation of STO, GHz optical birefringence can be induced by the coherent acoustic phonons and the birefringent amplitudes possess crystal orientation dependence. Optical manipulation of both coherent phonons and its induced GHz birefringence by double pump technique are also realized. These findings reveal an alternative mechanism of ultrafast optical birefringence control, and offer prospects for applications in high-frequency acoustic-optics devices. [ABSTRACT FROM AUTHOR]

Birefringence, which modulates the polarization of electromagnetic wave, has been commercially developed and widely used in modern photonics. Fostered by high-frequency signal processing and communications, feasible birefringence technologies operating in gigahertz (GHz) range are highly desired. Here, a coherent phonon-induced GHz optical birefringence and its manipulation in SrTiO3 (STO) crystals are demonsrated. With ultrafast laser pumping, the coherent acoustic phonons with low damping are created in the transducer/STO structures. A series of transducer layers are examined and the optimized one with relatively high photon-phonon conversion efficiency, i.e., semiconducting LaRhO3 film, is obtained. The most intriguing finding here is that, by virtue of high sensitivity to strain perturbation of STO, GHz optical birefringence can be induced by the coherent acoustic phonons and the birefringent amplitudes possess crystal orientation dependence. Optical manipulation of both coherent phonons and its induced GHz birefringence by double pump technique are also realized. These findings reveal an alternative mechanism of ultrafast optical birefringence control, and offer prospects for applications in high-frequency acoustic-optics devices. [ABSTRACT FROM AUTHOR]

We briefly review a few recent progresses of the ultrafast generation and detection of coherent phonons in various types of quantum materials. Both the shared properties and unique aspects of coherent phonons are addressed, followed by concrete examples, including some recent works from our group. Perspectives on the mechanism of coherent phonons are introduced, along with experimental details, tricks, and innovations. The main focus of this review is to reveal what one can obtain from the studies of coherent phonons, thus guiding the further investigations. Particularly, we show that various interactions among different degrees of freedom can be unveiled, telling the legends of the hidden secrets in many quantum materials. The content is intended to be intriguing to non-ultrafast spectroscopy experts as well. [ABSTRACT FROM AUTHOR]

We have investigated the dependence of terahertz wave emissions on the internal electric field in undoped GaAs/ n -type GaAs epitaxial structures irradiated by ultrashort laser pulses. The undoped layer has an electric field, the strength of which was controlled by the temperature in addition to the undoped layer thickness. We observed the electric field dependence of the terahertz waveform, and the results were explained by the calculation of the transient dynamics of electrons and phonons under electric fields. Furthermore, we indicated that the terahertz amplitude can be linearly controlled by the electric field strength in a wide electric field range. [ABSTRACT FROM AUTHOR]

In this study, we employ the atomistic wave-packet method to directly simulate coherent phonon transport and scattering dynamics in an aperiodic superlattice structure with aperiodically arranged interfaces. Our investigation reveals that interference dynamics, contingent upon the relative magnitudes of phonon wavelength, spatial coherence length, and average interface spacing, profoundly influence transmission spectra and mode-conversion behavior. Particularly, longer-wavelength phonons possessing larger coherence lengths exhibit more pronounced destructive interference and mode-conversion, leading to generally lower transmission. The insights gained into coherent phonon wave physics from this study can significantly augment the analysis and design of phononic devices. • Phonon interference changes with both wavelength and spatial coherence length. • The impact of coherence length on transport lessens with decreasing wavelength. • Greater spatial coherence leads to reduced transmission in aperiodic superlattice. • Reduced transmission explains lower thermal conductivity at low temperatures. [ABSTRACT FROM AUTHOR]

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 _1 _g 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 that the phonon relaxation dynamics are not simply governed by alloy scattering, but are significantly modified by anharmonic phonon–phonon scattering with implied minor contributions from electron–phonon scattering in a Weyl-semimetal phase.

Coherent phonons can be launched in materials upon localized pulsed optical excitation, and be subsequently followed in time-domain, with a sub-picosecond resolution, using a time-delayed pulsed probe. This technique yields characterization of mechanical, optical, and electronic properties at the nanoscale, and is taken advantage of for investigations in material science, physics, chemistry, and biology. Here we review the use of this experimental method applied to the emerging field of homo- and heterostructures of van der Waals materials. Their unique structure corresponding to non-covalently stacked atomically thin layers allows for the study of original structural configurations, down to one-atom-thin films free of interface defect. The generation and relaxation of coherent optical phonons, as well as propagative and resonant breathing acoustic phonons, are comprehensively discussed. This approach opens new avenues for the in situ characterization of these novel materials, the observation and modulation of exotic phenomena, and advances in the field of acoustics microscopy.

The implementation of thermal barriers in thermoelectric materials improves their power conversion rates effectively. For this purpose, material boundaries are utilized and manipulated to affect phonon transmissivity. Specifically, interface intermixing and topography represents a useful but complex parameter for thermal transport modification. This study investigates epitaxial thin film multilayers, so called superlattices (SL), of TiNiSn/HfNiSn, both with pristine and purposefully deteriorated interfaces. High-resolution transmission electron microscopy and X-ray diffractometry are used to characterize their structural properties in detail. A differential 3 ω -method probes their thermal resistivity. The thermal resistivity reaches a maximum for an intermediate interface quality and decreases again for higher boundary layer intermixing. For boundaries with the lowest interface quality, the interface thermal resistance is reduced by 23% compared to a pristine SL. While an uptake of diffuse scattering likely explains the initial deterioration of thermal transport, we propose a phonon bridge interpretation for the lowered thermal resistivity of the interfaces beyond a critical intermixing. In this picture, the locally reduced acoustic contrast of the less defined boundary acts as a mediator that promotes phonon transition.

Applying high pressure to effectively modulate the electronic and lattice structures of materials could unravel various physical properties associated with phase transitions. In this work, high-pressure-compatible femtosecond pump-probe microscopy was constructed to study the pressure-dependent ultrafast dynamics in black phosphorus (BP) thin films. We observed pressure-driven evolution of the electronic topological transition and three structural phases as the pressure reached ∼22 GPa, which could be clearly differentiated in the transient absorption images containing spatially resolved ultrafast carrier and coherent phonon dynamics. Surprisingly, an anomalous coherent acoustic phonon mode with pressure softening behavior was observed within the range of ∼3-8 GPa, showing distinct laser power and time dependences. Density functional theory calculations show that this mode, identified as the shear mode along the armchair orientation, gains significant electron-phonon coupling strength from out-of-plane compression that leads to decreased phonon frequency. Our results provide insights into the structure evolution of BP with pressure and hold potential for applications in microelectromechanical devices.

This paper reviews our recent study on a coherent optical phonon in a hexagonal YMnO3 thin film together with related optical studies in hexagonal RMnO3 (R = Y, Lu, Ho) compounds. Coherent phonons have been observed in RMnO3 compounds by pump-probe spectroscopy with subpicosecond laser pulses, whereas the observation of coherent optical phonons was reported only in LuMnO3. Recently, we succeeded in the observation of the coherent optical phonon in a YMnO3 thin film. The generation process of the coherent optical phonon is assigned to a displacive mechanism, which is identical to that in LuMnO3. The coherent optical phonon is observed in the temperature range from 10 K to room temperature, while the oscillation intensity strongly decreases as the temperature increases to the Néel temperature of ~70 K from a lower temperature range. It is interesting that the temperature dependence is largely different from that in LuMnO3. We describe that the result can be qualitatively explained by the property of an isostructural transition around the Néel temperature in RMnO3 compounds. In addition, we briefly discuss ultrafast incoherent responses of excited electronic states from the viewpoint of the excitation photon energy of laser pulses. [ABSTRACT FROM AUTHOR]

Black phosphorus is a layered semiconducting material, demonstrating strong layer-dependent optical and electronic properties. Probing the photophysical properties on ultrafast time scales is of central importance in understanding many-body interactions and nonequilibrium quasiparticle dynamics. Here, we applied temporally, spectrally, and spatially resolved pump–probe microscopy to study the transient optical responses of mechanically exfoliated few-layer black phosphorus, with layer numbers ranging from 2 to 9. We have observed layer-dependent resonant transient absorption spectra with both photobleaching and red-shifted photoinduced absorption features, which could be attributed to band gap renormalization of higher subband transitions. Surprisingly, coherent phonon oscillations with unprecedented intensities were observed when the probe photons were in resonance with the optical transitions, which correspond to the low-frequency layer-breathing mode. Our results reveal strong Coulomb interactions and electron–phonon couplings in photoexcited black phosphorus, providing important insights into the ultrafast optical, nanomechanical, and optoelectronic properties of this novel two-dimensional material. [ABSTRACT FROM AUTHOR]

Plasmon hybridization theory, inspired by molecular orbital theory, has been extremely successful in describing the near-field coupling in clusters of plasmonic nanoparticles, also known as plasmonic molecules. However, the vibrational modes of plasmonic molecules have been virtually unexplored. By designing precisely configured plasmonic molecules of varying complexity and probing them at the individual plasmonic molecule level, intramolecular coupling of acoustic modes, mediated by the underlying substrate, is observed. The strength of this coupling can be manipulated through the configuration of the plasmonic molecules. Surprisingly, classical continuum elastic theory fails to account for the experimental trends, which are well described by a simple coupled oscillator picture that assumes the vibrational coupling is mediated by coherent phonons with low energies. These findings provide a route to the systematic optical control of the gigahertz response of metallic nanostructures, opening the door to new optomechanical device strategies. [ABSTRACT FROM AUTHOR]

This paper describes the dynamics of three-component superlattices consisting of non-ferroelectric and anti-ferromagnetic NdMnO/SrMnO/LaMnO layers. Using a femtosecond pump-probe method, two acoustic phonons are observed at frequencies of 49 and 19 GHz, respectively. The temperature dependence of the acoustic phonon follows a similar trend to that of the magnetic phase transition. Surprisingly, one phonon responds strongly to an external magnetic field. The results support the existence of magneto-electric coupling in the superlattice induced by interfacial effects between the non-ferroelectric and anti-ferromagnetic layers and suggest the possible development of ultrafast magneto-tunable devices. [ABSTRACT FROM AUTHOR]

Methods that allow versatile manipulation of metastable centers in semiconductors are highly important owing to their potential for quantum information processing and computations. In this study, we demonstrate that the electron-phonon interaction enables phonon participation to promote relaxation of metastable centers in ZnO, which is known for its persistent photoconductivity (PPC) effect. Experimentally, we show that continuous infrared (IR) radiation (1064 nm, ∼30 mW/cm 2 ) promotes longitudinal optical phonons via the Fröhlich interaction and increases the PPC relaxation rate by ∼4 folds. More importantly, we discover that coherent phonons activated by an ultrashort pulse IR laser of the same power increased the relaxation rate by ∼1200-fold, as confirmed by ultrafast transient spectroscopy to be correlated to the excitation of coherent acoustic phonons via the inverse piezoelectric effect. We expect this study to provide valuable guidance for the development of novel quantum and photoactive devices.