We report on the dynamics of coherent phonons in semimetal 1T'-MoTe2 using femtosecond pump-probe spectroscopy. On an ultrafast sub-picosecond time scale at room temperature, a low frequency and long-lifetime shear phonon mode was observed at 0.39 THz, which was previously reported in the form of a characteristic phonon only in the low temperature Td-MoTe2 phase. Unlike the other optical phonon modes, the shear phonon mode was found to strongly couple with photoexcited carriers. Moreover, the amplitude of the shear mode surprisingly decreased with increasing excitation density, a phenomenon which can be attributed to be a consequence of the lattice temperature rising after excitation. These results provide useful physical information on ultrafast lattice symmetry switching between the normal semimetal 1T' and the lattice inversion symmetry breaking Type-II Weyl semimetal Td phases.
$\mathrm{MoTe_2}$ has recently been shown to realize in its low-temperature phase the type-II Weyl semimetal (WSM). We investigated by time- and angle- resolved photoelectron spectroscopy (tr-ARPES) the possible influence of the Weyl points in the electron dynamics above the Fermi level $\mathrm{E_F}$, by comparing the ultrafast response of $\mathrm{MoTe_2}$ in the trivial and topological phases. In the low-temperature WSM phase, we report an enhanced relaxation rate of electrons optically excited to the conduction band, which we interpret as a fingerprint of the local gap closure when Weyl po…
A Weyl semimetal is a new type of topological quantum phase with intriguing physics near the Weyl nodes. Although the equilibrium state of Weyl semimetals has been investigated, the ultrafast dynamics near the Weyl node in the nonequilibrium state is still missing. Here by performing time and angle resolved photoemission spectroscopy on type-II Weyl semimetal MoTe$_2$, we reveal the dispersion of the unoccupied states and identify the Weyl node at 70 meV above E$_F$. Moreover, by tracking the ultrafast relaxation dynamics near the Weyl node upon photo-excitation with energy, momentum and tempo…
By using constrained density functional theory modeling, we demonstrate that ultrafast optical pumping unveils hidden charge orders in group VI monolayer transition metal ditellurides. We show that irradiation of the insulating 2H phases stabilizes multiple transient charge density wave orders with light-tunable distortion, periodicity, electronic structure and bandgap. Moreover, optical pumping of the semimetallic 1T' phases generates a transient charge ordered metallic phase composed of 2D diamond clusters. For each transient phase we identify the critical fluence at which it is observed and…
The dynamics of band-gap renormalization and gain build-up in monolayer MoTe$_2$ is investigated by evaluating the non-equilibrium Dirac-Bloch equations with the incoherent carrier-carrier and carrier-phonon scattering treated via quantum-Boltzmann type scattering equations. For the case where an approximately $300$ fs-long high intensity optical pulse generates charge-carrier densities in the gain regime, the strong Coulomb coupling leads to a relaxation of excited carriers on a few fs time scale. The pump-pulse generation of excited carriers induces a large band-gap renormalization during th…
Recent development of ultrashort laser pulses allows for optical control of structural and electronic properties of complex quantum materials. The layered transition metal dichalcogenide MoTe2, which can crystalize into several different structures with distinct topological and electronic properties, provides possibilities to control or switch between different phases. In this study we report a photo-induced sub-picosecond structural transition between the type-II Weyl semimetal phase and normal semimetal phase in bulk crystalline MoTe2 by using ultrafast pump-probe and time-resolved second ha…
Photo-induced phase transitions (PIPTs) provide an ultrafast, energy-efficient way for precisely manipulating the topological properties of transition-metal ditellurides, and can be used to stabilize a topological phase in an otherwise semiconducting material. Using first-principles calculations, we demonstrate that the PIPT in monolayer MoTe$_2$ from the semiconducting 2H phase to the topological 1T$'$ phase can be triggered purely by electronic excitations that soften multiple lattice vibrational modes. These softenings, driven by a Peierls-like mechanism within the conduction bands, lead to…
We report on time-resolved broadband transient reflectivity (tr-bb-TR) measurements performed on a bulk single crystal of T$_d$-MoTe$_2$ as a function of the incident pump fluence (F). Tr-bb-TR data unveil photoinduced electronic changes progressing on the sub-picosecond timescale as well as the dynamics of the coherent low-frequency $^1A_1$ interlayer shear phonon. Our results indicate a gradual evolution of both the TR and the $^1A_1$ Fourier intensity spectra as a function of F, ruling out the threshold-like change that has been associated with the ultrafast photoinduced $T_d \to 1T'$ phase…
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…
We systematically study the high-resolution and polarized Raman spectra of multilayer (ML) MoTe2. The layer-breathing (LB) and shear (C) modes are observed in the ultralow-frequency region, which are used to quantitatively evaluate the interlayer coupling in ML MoTe2 based on the linear chain model, in which only the nearest interlayer coupling is considered. The Raman spectra on three different substrates verify the negligible substrate effect on the phonon frequencies of ML MoTe2. Ten excitation energies are used to measure the high-frequency modes of N-layer MoTe2 (NL MoTe2; N is an integer…
We report on room-temperature Raman scattering measurements in few-layer crystals of exfoliated molybdenum ditelluride (MoTe$_{2}$) performed with the use of 632.8 nm (1.96 eV) laser light excitation. In agreement with recent study reported by G. Froehlicher et al, (2015 $Nano$ $Lett.$ 15 6481) we observe a complex structure of the out-of-plane vibrational modes (A$_{1g}$/A$^{'}_{1}$), which can be explained in terms of interlayer interactions between single atomic planes of MoTe$_{2}$. In the case of low-energy shear and breathing modes of rigid interlayer vibrations it is shown that their en…
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…
Phonon-modulated Kerr nonlinearity in ultrathin 2H-MoTe2
Max Planck Institute for Solid State Research（马克斯·普朗克固体研究所）；Tsientang Institute for Advanced Study（紫江高等研究院）；Hefei National Laboratory, University of Science and Technology of China（合肥国家实验室，中国科学技术大学）；Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences（北京凝聚态物理国家实验室，中国科学院物理研究所）；School of Physical Sciences, University of Chinese Academy of Sciences（中国科学院大学物理科学学院）；Indian Institute of Science Education and Research（印度科学教育与研究机构）
Laser excitation has emerged as a means to expose hidden states of matter and promote phase transitions on demand. Such laser induced transformations are often rendered possible owing to the delivery of spatially and/or temporally manipulated light, carrying energy quanta well above the thermal background. Here, we report time-resolved broadband femtosecond (fs) transient absorption measurements on thin flakes of Weyl semimetal candidate $T_d$-MoTe$_2$ subjected to various levels and schemes of fs-photoexcitation. Our results reveal that impulsive fs-laser irradiation alters the interlayer beh…
Measurements of Ag radiotracer diffusion in shear bands of deformed bulk metallic glass, Pd40Ni40P20, [Joachim Bokeloh, Sergiy V. Divinski, Gerrit Reglitz, and Gerhard Wilde, Phys. Rev. Lett. 107, 235503 (2011).] have found a colossal enhancement of diffusion coefficient by more than eight orders of magnitude than in undeformed Pd40Ni40P20. Suggestion was made by Bokeloh et al. that enhanced diffusion occurs in high-mobility pathways originating from some excess free volume distribution inside the shear bands. Although plausible, this qualitative suggestion does not allow quantitative calculat…
Enabling the light-control of complex systems on ultra-short timescales gives rise to rich physics with promising applications. While crucial, the quantitative determination of both the longitudinal and shear photo-induced strains still remains challenging. Here, by scrutinizing asymmetric Bragg peaks pairs $(\pm h01)$ using picosecond time-resolved X-ray diffraction experiments in BiFeO$_3$, we simultaneously determine the longitudinal and shear strains. The relative amplitude of those strains can be explained only if both thermal and non-thermal processes contribute to the acoustic phonon ph…
Using femtosecond time-resolved X-ray diffraction, we investigated optically excited coherent acoustic phonons in the Weyl semimetal TaAs. The low symmetry of the (112) surface probed in our experiment enables the simultaneous excitation of longitudinal and shear acoustic modes, whose dispersion closely matches our simulations. We observed an asymmetry in the spectral lineshape of the longitudinal mode that is notably absent from the shear mode, suggesting a time-dependent frequency chirp that is likely driven by photoinduced carrier diffusion. We argue on the basis of symmetry that these acou…
$N$-layer transition metal dichalcogenides provide a unique platform to investigate the evolution of the physical properties between the bulk (three dimensional) and monolayer (quasi two-dimensional) limits. Here, using high-resolution micro-Raman spectroscopy, we report a unified experimental description of the $Γ$-point optical phonons in $N$-layer $2H$-molybdenum ditelluride (MoTe$_2$). We observe a series of $N$-dependent low-frequency interlayer shear and breathing modes (below $40~\rm cm^{-1}$, denoted LSM and LBM) and well-defined Davydov splittings of the mid-frequency modes (in the ra…
Strain engineering has been extended recently to the ultrafast timescales, driving metal-insulator phase transitions and the propagation of ultrasonic demagnetization fronts. However, the non-linear lattice dynamics underpinning interfacial optoelectronic phase switching have not yet been addressed. Here we focus on the lattice dynamics initiated by impulsive resonant excitation of polar lattice vibrations in LaAlO$_3$ single crystals, one of the most widely utilized substrates for oxide electronics. We show that ionic Raman scattering drives coherent oxygen octahedra rotations around a high-s…
We investigate the interlayer phonon modes in $N$-layer rhenium diselenide (ReSe$_2$) and rhenium disulfide (ReS$_2$) by means of ultralow-frequency micro-Raman spectroscopy. These transition metal dichalcogenides exhibit a stable distorted octahedral (1T') phase with significant in-plane anisotropy, leading to sizable splitting of the (in-plane) layer shear modes. The fan-diagrams associated with the measured frequencies of the interlayer shear modes and the (out-of-plane) interlayer breathing modes are perfectly described by a finite linear chain model and allow the determination of the inte…
The control of optically driven high-frequency strain waves in nanostructured systems is an essential ingredient for the further development of nanophononics. However, broadly applicable experimental means to quantitatively map such structural distortion on their intrinsic ultrafast time and nanometer length scales are still lacking. Here, we introduce ultrafast convergent beam electron diffraction (U-CBED) with a nanoscale probe beam for the quantitative retrieval of the time-dependent local distortion tensor. We demonstrate its capabilities by investigating the ultrafast acoustic deformation…
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…
The selective excitation of coherent phonons provides unique capabilities to control fundamental properties of quantum materials on ultrafast time scales. For instance, in the presence of strong electron-phonon coupling, the electronic band structure can become substantially modulated. Recently, it was predicted that by this means even topologically protected states of matter can be manipulated and, ultimately, be destroyed: For the layered transition metal dichalcogenide Td-WTe$_2$, pairs of Weyl points are expected to annihilate as an interlayer shear mode drives the crystalline structure to…
Identifying and understanding the mechanisms behind strong phonon-phonon scattering in condensed matter systems is critical to maximizing the efficiency of thermoelectric devices. To date, the leading method to address this has been to meticulously survey the full phonon dispersion of the material in order to isolate modes with anomalously large linewidth and temperature-dependence. Here we combine quantitative MeV ultrafast electron diffraction (UED) analysis with Monte Carlo based dynamic diffraction simulation and first-principles calculations to directly unveil the soft, anharmonic lattice…
Trigonal tellurium (Te) is a chiral semiconductor that lacks both mirror and inversion symmetries, resulting in complex band structures with Weyl crossings and unique spin textures. Detailed time-resolved polarized reflectance spectroscopy is used to investigate its band structure and carrier dynamics. The polarized transient spectra reveal optical transitions between the uppermost spin-split H4 and H5 and the degenerate H6 valence bands (VB) and the lowest degenerate H6 conduction band (CB) as well as a higher energy transition at the L-point. Surprisingly, the degeneracy of the H6 CB (a prop…
Strain-induced Dynamic Spin-Phonon Coupling in Epitaxial RuO2 Films
Gwangju Institute of Science and Technology (GIST)（光州科学技术院）；University of Minnesota−Twin Cities（明尼苏达大学双城分校）；Hankuk University of Foreign Studies（韩国外国语大学）；Seoul National University（首尔大学）；Sejong University（世宗大学）
Atomically Resolved Acoustic Dynamics Coupled with Magnetic Order in a van der Waals Antiferromagnet
Materials Science Division, Argonne National Laboratory（阿贡国家实验室材料科学部）；Department of Physics, University of Washington（华盛顿大学物理系）；Center for Ultrafast Phase Transformation, Department of Physics, Sogang University（西江大学物理系超快相变中心）；Department of Materials Science and Engineering, University of Washington（华盛顿大学材料科学与工程系）；Pohang Accelerator Laboratory, POSTECH（韩国科学技术院浦项加速器实验室）；Institute for Condensed Matter and Complex Systems, School of Physics and Astronomy, The University of Edinburgh（爱丁堡大学物理与天文学学院凝聚态与复杂系统研究所）；Donostia International Physics Center（圣塞巴斯蒂安国际物理中心）；Department of Physics, Cambridge, Massachusetts Institute of Technology（麻省理工学院物理系）；Departments of Physics and Applied Physics, Stanford University（斯坦福大学物理与应用物理系）
Photo-induced phase transitions have been intensively studied owing to the ability to control a material of interest in the ultrafast manner, which can induce exotic phases unable to be attained at equilibrium. However, the key mechanisms are still under debate, and it has currently been a central issue how the couplings between the electron, lattice, and spin degrees of freedom are evolving during photo-induced phase transitions. Here, we develop a new analysis method, frequency-domain angle-resolved photoemission spectroscopy, to gain precise insight into electron-phonon couplings during pho…
