Here we show how time-resolved broadband optical spectroscopy can be used to quantify, with femtometer resolution, the oscillation amplitudes of coherent phonons through a displacive model without free tuning parameters, except an overall scaling factor determined by comparison between experimental data and density functional theory calculations. $WTe_2$ is used to benchmark this approach. In this semimetal, the response is anisotropic and provides the spectral fingerprints of two $A_1$ optical phonons at $\sim$8 and $\sim$80 $cm^-$$^1$. In principle, this methodology can be extended to any material in which an ultrafast excitation triggers coherent lattice modes modulating the high-energy optical properties.
By using constrained density functional theory modeling, we demonstrate that ultrafast optical pumping unveils hidden charge orders in group VI monolayer transition metal ditellurides. We show that irradiation of the insulating 2H phases stabilizes multiple transient charge density wave orders with light-tunable distortion, periodicity, electronic structure and bandgap. Moreover, optical pumping of the semimetallic 1T' phases generates a transient charge ordered metallic phase composed of 2D diamond clusters. For each transient phase we identify the critical fluence at which it is observed and…
Weyl Fermions (WFs) in the type-II Weyl Semimetal (WSM) WTe$_2$ are difficult to resolve experimentally because the Weyl bands disperse in an extremely narrow region of the (E-k) space. Here, by using DFT-assisted high-resolution $^{125}$Te solid-state NMR (ssNMR) in the temperature range $50$K - $700$K, we succeeded in detecting low energy WF excitations and monitor their evolution with temperature. Remarkably, WFs appear to emerge at T$\sim 120$K; at lower temperatures WTe$_2$ behaves as a metal. This intriguing metal-to-WSM phase transition is shown to be induced by the rapid raise of the F…
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…
The electromagnetic response of Dirac semimetals in the infrared and terahertz frequency ranges is attracting growing interest for potential applications in optoelectronics and nonlinear optics. The interplay between the free-carrier response and interband transitions in the gapless, linear dispersion relation plays a key role in enabling novel functionalities. Here we investigate ultrafast dynamics in thin films of a photoexcited Dirac semimetal Cd$_3$As$_2$ by probing the broadband response functions as complex quantities in the multiterahertz region (10-45 THz, 40-180 meV, or 7-30 $μ$m), wh…
Intense, few-cycle pulses in the terahertz frequency range have strong potential for schemes of control over vibrational modes in solid-state materials in the electronic ground-state. Here we report an experiment using single cycle terahertz pulses to directly excite lattice vibrations in the ferroelectric material $\mathrm{Sn_2P_2S_6}$ and ultrafast x-ray diffraction to quantify the resulting structural dynamics. A model of a damped harmonic oscillator driven by the transient electric field of the terahertz pulses describes well the movement of the Sn$^{2+}$ ion along the ferroelectric soft m…
Probing sliding ferroelectricity in bilayer T$_\mathrm{d}$-WTe$_2$ with high-harmonic generation
TU Graz（格拉茨工业大学）；Max Planck Institute for the Structure and Dynamics of Matter（马普物质结构与动力学研究所）；Flatiron Institute（平顿研究所）；Universidad del País Vasco UPV/EHU（巴斯克大学）
Terahertz spin waves could be generated on-demand via all-optical manipulation of magnetization by femtosecond laser pulse. Here, we present an energy balance model, which explains the energy transfer rates from laser pulse to electron bath coupled with phonon, spin, and magnetization of five different magnetic metallic thin films: Iron, Cobalt, Nickel, Gadolinium and Ni$_{2}$MnSn Heusler alloy. Two types of transient magnetization dynamics emerge in metallic magnetic thin films based on their Curie temperatures (T$_{C}$): type I (Fe, Co, and Ni with T$_{C}$ > room temperature, RT) and type II…
$\mathrm{MoTe_2}$ 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…
Competition between the Pseudogap and Superconducting States of Bi$_{2}$Sr$_{2}$Ca$_{0.92}$Y$_{0.08}$Cu$_{2}$O$_{8+δ}$ Single Crystals Revealed by Ultrafast Broadband Optical Reflectivity
用超快宽带瞬态反射率实验研究了Bi $_{2}$ Sr $_{2}$ Ca $_{0.92}$ Y $_{0.08}$ Cu $_{2}$ O $_{8+δ}$中赝能隙的非平衡动力学与超导相的相互作用.一旦建立了超导电性，赝能隙的弛豫速度就会比正常状态快2倍，而相应的瞬态反射率变化在$\sim$ 0.5 ps后改变符号。$\sim$。结果可以用一组耦合的赝能隙和超导序参量的微分方程来描述。耦合项的符号和强度表明两相之间的竞争非常弱，允许它们共存。
Transition metal nitrides have recently gained attention in the fields of plasmonics, plasmon-enhanced photocatalysis, photothermal applications, and nonlinear optics because of their suitable optical properties, refractory nature, and large laser damage thresholds. This work reports comparative studies of the transient response of films of titanium nitride, zirconium nitride, and Au under femtosecond excitation. Broadband transient optical characterization helps to adjudicate earlier, somewhat inconsistent reports regarding hot electron lifetimes based upon single wavelength measurements. The…
The availability of high-frequency pulsed emitters in the $2-2.5\,μ$m wavelength range paved the way for a wealth of new applications in ultrafast spectroscopy, free-space and fiber-optical communications, surveillance and recognition, artificial intelligence, and medical imaging. However, developing these emerging technologies and their large-scale use depend on the availability of high-speed, low-noise, and cost-effective photodetectors. With this perspective, here we demonstrate GeSn photodiodes grown on silicon wafers featuring a high broadband operation covering the extended-SWIR range wi…
Transient Pauli blocking in a InN film as a mechanism for broadband ultrafast optical switching
Global Center for Science and Engineering (GCSE), Faculty of Science and Engineering, Waseda University（早稻田大学理工学部）；Graduate School of Advanced Science and Engineering, Waseda University（早稻田大学先进理工学研究科）；Graduate School of Science and Engineering, Aoyama Gakuin University（青山学院大学理工学府）；Institute for Molecular Science（分子科学研究所）；The Graduate University for Advanced Studies (SOKENDAI)（综合研究大学院大学）；National Metrology Institute of Japan (NMIJ), National Institute of Advanced Industrial Science and Technology (AIST)（产业技术综合研究所国家计量标准研究所）
Multi-temperature models are nowadays often used to quantify the ultrafast electron-phonon (boson) relaxations and coupling strengths in advanced quantum solids. To test their applicability we study the time evolution of the electron distribution function, f(E), in Cu over large range of excitation densities using broadband time-resolved optical spectroscopy. Following intraband optical excitation, f(E) is found to be athermal over several 100 fs, while substantial part of the absorbed energy already being transferred to the lattice. We show, however, that the electron-phonon coupling constant…
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…
Metal-oxide-semiconductor junctions are central to most electronic and optoelectronic devices. Here, the element-specificity of broadband extreme ultraviolet (XUV) ultrafast pulses is used to measure the charge transport and recombination kinetics in each layer of a Ni-TiO2-Si junction. After photoexcitation of silicon, holes are inferred to transport from Si to Ni ballistically in ~100 fs, resulting in spectral shifts in the Ni M2,3 XUV edge that are characteristic of holes and the absence of holes initially in TiO2. Meanwhile, the electrons are observed to remain on Si. After picoseconds, th…
Strong light-matter interactions in layered transition metal dichalcogenides (TMDs) open up vivid possibilities for novel exciton-based devices. The optical properties of TMDs are dominated mostly by the tightly bound excitons and more complex quasiparticles, the biexcitons. Instead of physically exfoliated monolayers, the solvent-mediated chemical exfoliation of these 2D crystals is a cost-effective, large-scale production method suitable for real device applications. We explore the ultrafast excitonic processes in WS$_{2}$ dispersion using broadband femtosecond pump-probe spectroscopy at roo…
Recently, the switching between the different charge-ordered phases of 1T-TaS2 has been probed by ultrafast techniques, revealing unexpected phenomena such as "hidden" metastable states and peculiar photoexcited charge patterns. Here, we apply broadband pump-probe spectroscopy with varying excitation energy to study the ultrafast optical properties of 1T-TaS2 in the visible regime. By scanning the excitation energy in the near-IR region we unravel the coupling between different charge excitations and the low-lying charge-density wave state. We find that the amplitude mode of the charge-density…
Demonstration of ultrafast coherent sub-picosecond magnon pulses
Charles University（查理大学）；Czech Academy of Sciences（捷克科学院）；Walther-Meissner-Institut, Bayerische Akademie der Wissenschaften（瓦尔特·迈斯纳研究所，巴伐利亚科学院）；Technical University of Munich（慕尼黑工业大学）；Freie Universität Berlin（柏林自由大学）；University of Nottingham（诺丁汉大学）；Tohoku University（东北大学）
Oscillator-driven broadband femtosecond transient microspectroscopy with supercontinuum probes generated in a photonic crystal fiber
Osaka Metropolitan University（大阪公立大学）；Institute for Molecular Science, National Institutes of Natural Sciences（国立自然科学研究所分子科学研究所）；Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC)（马德里材料科学研究所）
In order to determine the role of non-thermal transport of hot carriers which is decisive for the dissipation of energy in condensed matter we performed time-resolved broadband femtosecond transient reflectivity measurements on $7-197 \mathrm{nm}$ thick Bi(111) films epitaxially grown on Si(111). We monitored the behavior of the Fourier amplitude and the central frequency of the coherent $A_\mathrm{1g}$ phonon mode as function of the incident fluence, film thickness, and probe wavelength in the range of $580 -700 \mathrm{nm}$. The frequency redshift that follows photoexcitation was used as a r…
Ultrafast THz radiation generation from ferromagnetic/nonmagnetic bilayer heterostructure-based spintronic emitters generally exploits the conversion from spin- to charge-current within the nonmagnetic layer and its interface with the ferromagnetic layer. Various possible sub-contributions to the underlying mechanism of inverse spin Hall effect for the THz emission from such structures, need to be exploited for not only investigating the intricacies at the fundamental level in the material properties themselves but also for improving their performance for broadband and high-power THz emission.…
The ultrafast polarization response to incident light and ensuing exciton/carrier generation are essential to outstanding optoelectronic properties of lead halide perovskites (LHPs). A large number of mechanistic studies in the LHP field to date have focused on contributions to polarizability from organic cations and the highly polarizable inorganic lattice. For a comprehensive understanding of the ultrafast polarization response, we must additionally account for the nearly instantaneous hyperpolarizability response to the propagating light field itself. While light propagation is pivotal to o…
Transition metal dichalcogenides (TMDs) are emerging as promising two-dimensional (2d) semiconductors for optoelectronic and flexible devices. However, a microscopic explanation of their photophysics -- of pivotal importance for the understanding and optimization of device operation -- is still lacking. Here we use femtosecond transient absorption spectroscopy, with pump pulse tunability and broadband probing, to monitor the relaxation dynamics of single-layer MoS2 over the entire visible range, upon photoexcitation of different excitonic transitions. We find that, irrespective of excitation p…
Point defects in crystalline materials often occur in multiple charge states. Although many experimental methods to study and explore point defects are available, techniques to explore the non-equilibrium dynamics of the charge states of these defects at ultrafast (sub-nanosecond) time scales have not been discussed before. We present results from ultrafast optical-pump supercontinuum-probe spectroscopy measurements on $β$-Ga$_2$O$_3$. The study of point defects in $β$-Ga$_2$O$_3$ is essential for its establishment as a material platform for high-power electronics and deep-UV optoelectronics. …
Integrating femtosecond (fs) lasers to electron microscopies has enabled direct imaging of transient structures and morphologies of materials in real time and space, namely, ultrafast electron microscopy (UEM). Here we report the development of a laser-free UEM offering the same capability of real-time imaging with high spatiotemporal resolutions but without requiring expensive fs lasers and intricate instrumental modifications. We create picosecond electron pulses for probing dynamic events by chopping a continuous beam with a radiofrequency (RF)-driven pulser, where the repetition rate of th…
