Tracking ultrafast solid-state dynamics using high harmonic spectroscopy
Mina R. Bionta, Elissa Haddad, Adrien Leblanc, Vincent Gruson, Philippe Lassonde, Heide Ibrahim, Jérémie Chaillou, Nicolas Émond, Martin R. Otto, Bradley J. Siw… 展开作者
Mina R. Bionta, Elissa Haddad, Adrien Leblanc, Vincent Gruson, Philippe Lassonde, Heide Ibrahim, Jérémie Chaillou, Nicolas Émond, Martin R. Otto, Bradley J. Siwick, Mohamed Chaker, François Légaré
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20 pages and 4 figures main text, 8 pages and 4 figures supplementary information
We establish time-resolved high harmonic generation (tr-HHG) as a powerful spectroscopy for photoinduced dynamics in strongly correlated materials through a detailed investigation of the insulator-to-metal transitions in vanadium dioxide. We benchmark our technique by comparing our measurements to established momentum-resolved ultrafast electron diffraction, and theoretical density functional calculations. Tr-HHG allows distinguishing of individual dynamic channels, including a transition to a thermodynamically hidden phase. In addition, the HHG yield is shown to be modulated at a frequency characteristic of a coherent phonon in the equilibrium monoclinic phase over a wide range of excitation fluences. These results demonstrate that tr-HHG is capable of tracking complex dynamics in solids through its sensitivity to the band structure.
Ultrafast light-matter interaction is a powerful tool for the study of solids. Upon laser excitation, carrier multiplication and lattice acceleration beyond thermal velocity can occur, as a result of far-from-equilibrium carrier relaxation. The roles of electron-electron and electron-phonon scatterings are identified by first-principles dynamic simulations, from which a unified phase diagram emerges. It not only explains the experimentally-observed "inertial" melting but also predicts abnormal damping by Pauli Exclusion Principle with a new perspective on ultrahigh-intensity laser applications…
We introduce a new method for performing ultrafast imaging and tracking of surface plasmon wave packets that propagate on metal films. We demonstrate the efficiency of leakage radiation microscopy implemented in the time domain for measuring both group and phase velocities of near-field pulses with a high level of precision. The versatility of our far-field imaging method is particularly appealing in the context of ultrafast near-field optics.
Here we report on a novel High Harmonic Generation (HHG) light source designed for space charge free ultrafast photoelectron spectroscopy (PES) on solids. The ultimate overall energy resolution achieved on a polycrystalline Au sample is ~22 meV at 40 K. These results have been obtained at a photon energy of 16.9 eV with a pulse bandwidth of ~19 meV, by varying, up to 200 kHz, the photon pulses repetition rate and the photon fluence on the sample. These features set a new benchmark for tunable narrowband HHG sources. By comparing the PES energy resolution and the photon pulse bandwidth with a p…
The ultrafast response of metals to light is governed by intriguing non-equilibrium dynamics involving the interplay of excited electrons and phonons. The coupling between them gives rise to nonlinear diffusion behavior on ultrashort timescales. Here, we use scanning ultrafast thermo-modulation microscopy to image the spatio-temporal hot-electron diffusion in a thin gold film. By tracking local transient reflectivity with 20 nm and 0.25 ps resolution, we reveal two distinct diffusion regimes, consisting of an initial rapid diffusion during the first few picoseconds after optical excitation, fo…
We predict a strong-field ultrafast optical Faraday effect, where a circularly polarized ultrashort optical pulse induces transient chirality in an achiral transparent dielectric. This effect is attractive for time-resolved measurements because it gives access to the non-instantaneity of the nonlinear medium response, and also because it represents relaxation of time-reversal symmetry by all-optical means. We propose probing the induced transient chirality with a weak linearly polarized ultraviolet pulse that is shorter than the near-infrared pump pulse. The predicted effects are ultrafast: th…
The ultrafast optical Kerr effect (OKE) is widely used to investigate the structural dynamics and interactions of liquids, solutions and solids by observing their intrinsic nonlinear temporal responses through nearly-collinear four-wave mixing (FWM). Non-degenerate mixing schemes allow for background free detection and can provide information on the interplay between a material's internal degrees of freedom. Here we show a source of temporal dynamics in the OKE signal that is not reflective of the intrinsic nonlinear response but arises from group index and momentum mismatch. It is observed in…
We present a theoretical description of resonant radiofrequency (RF) deflecting cavities in TM$_{110}$ mode as dynamic optical elements for ultrafast electron microscopy. We first derive the optical transfer matrix of an ideal pillbox cavity and use a Courant-Snyder formalism to calculate the 6D phase space propagation of a Gaussian electron distribution through the cavity. We derive closed, analytic expressions for the increase in transverse emittance and energy spread of the electron distribution. We demonstrate that for the special case of a beam focused in the center of the cavity, the low…
The unique functionalities of antiferromagnets offer promising routes to advance information technology. Their compensated magnetic order leads to spin resonances in the THz-regime, which suggest the possibility to coherently control antiferromagnetic (AFM) devices orders of magnitude faster than traditional electronics. However, the required time resolution, complex sublattice interations and the relative inaccessibility of the AFM order parameter pose serious challenges to studying AFM spin dynamics. Here, we reveal the temporal evolution of an AFM order parameter directly in the time domain…
Sculpting ultrafast mid-infrared light for solid-state high harmonic generation
Eastern Institute of Technology（东方理工学院）；ELI-ALPS, ELI-Hu Non-Profit Ltd.（极强光激光科学研究所有限公司）；Laboratoire Photonique Numérique et Nanosciences (LP2N), UMR 5298, CNRS-IOGS-Université Bordeaux（波尔多大学光子学与纳米科学实验室）；Theoretisch-Physikalisches Institut, Friedrich-Schiller-Universität Jena（耶拿大学理论物理研究所）；Centro de Investigaciones en Óptica, A.C.（光学研究中心）；School of Optical-Electrical and Computer Engineering, University of Shanghai for Science and Technology（上海理工大学光电信息与计算机工程学院）；Zhejiang Key Laboratory of 3D Micro/Nano Fabrication and Characterization, Department of Electronic and Information Engineering, School of Engineering, Westlake University（西湖大学工学院电子与信息工程系三维微纳加工与表征浙江省重点实验室）；Helmholtz-Institut Jena（耶拿亥姆霍兹研究所）；GSI Helmholtzzentrum für Schwerionenforschung GmbH（达姆施塔特重离子研究中心）
Strong-field methods in solids enable new strategies for ultrafast nonlinear spectroscopy and provide all-optical insights into the electronic properties of condensed matter in reciprocal and real space. Additionally, solid-state media offers unprecedented possibilities to control high-harmonic generation using modified targets or tailored excitation fields. Here we merge these important points and demonstrate circularly-polarized high-harmonic generation with polarization-matched excitation fields for spectroscopy of chiral electronic properties at surfaces. The sensitivity of our approach is…
Ultrafast electronic dynamics in solids lies at the core of modern condensed matter and materials physics. To build up a practical ab initio method for studying solids under photoexcitation, we develop a momentum-resolved real-time time dependent density functional theory (rt-TDDFT)algorithm using numerical atomic basis, together with the implementation of both the length and vector gauge of the electromagnetic field. When applied to simulate elementary excitations in two-dimensional materials such as graphene, different excitation modes, only distinguishable in momentum space, are observed. T…
The first step to gain optical control over the ultrafast processes initiated by light in solids is a correct identification of the physical mechanisms at play. Among them, exciton formation has been identified as a crucial phenomenon which deeply affects the electro-optical properties of most semiconductors and insulators of technological interest. While recent experiments based on attosecond spectroscopy techniques have demonstrated the possibility to observe the early-stage exciton dynamics, the description of the underlying exciton properties remains non-trivial. In this work we propose a …
We have developed a single-shot imaging technique that can capture ultrafast events occurring on femtosecond to picosecond time scales. The technique is based on an optical pump-probe method, in which multiple time-delayed femtosecond pulses simultaneously probe a pump-excited sample. Here we use two sets of 2-by-2 mirror arrays for spatial/temporal division and routing of multiple probe pulses. This single-shot scheme is successfully applied to capture femtosecond ionization fronts propagating at the speed of light in air, as well as laser-induced ablation of solid targets.
We report a 2μm ultrafast solid-state Tm:Lu2O3 laser, mode-locked by single-layer graphene, generating transform-limited~410fs pulses, with a spectral width~11.1nm at 2067nm. The maximum average output power is 270mW, at a pulse repetition frequency of 110MHz. This is a convenient high-power transform-limited laser at 2μm for various applications, such as laser surgery and material processing.
Approaching energy coupling in laser-irradiated metals, we point out the role of electron-electron collision as an efficient control factor for ultrafast optical absorption. The high degree of laser-induced electron-ion nonequilibrium drives a complex absorption pattern with consequences on the transient optical properties. Consequently, high electronic temperatures determine largely the collision frequency and establish a transition between absorptive regimes in solid and plasma phases. In particular, taking into account umklapp electron-electron collisions, we performed hydrodynamic simulati…
Broadband ultrafast optical spectroscopy methods, such as transient absorption spectroscopy and 2D spectroscopy, are widely used to study molecular dynamics. However, these techniques are typically restricted to optically thick samples, such as solids and liquid solutions. In this article we discuss a cavity-enhanced ultrafast transient absorption spectrometer covering almost the entire visible range with a detection limit of $Δ$OD $ < 1 \times 10^{-9}$, extending broadband all-optical ultrafast spectroscopy techniques to dilute beams of gas-phase molecules and clusters. We describe the techni…
The Keldysh theory of photoionization in a solid dielectric is generalized to the case of arbitrarily short driving pulses of arbitrary pulse shape. We derive a closed-form solution for the nonadiabatic ionization rate in a transparent solid with a periodic dispersion relation, which reveals ultrafast ionization dynamics within the field cycle and recovers the key results of the Keldysh theory in the appropriate limiting regimes.
Ultrafast wide-field 3D topography with extended depth of field
Key Laboratory of Light Field Manipulation and Information Acquisition, Ministry of Industry and Information Technology, School of Physical Science and Technology, Northwestern Polytechnical University（西北工业大学）
Programmable high-harmonic emission in solids through photon pathways
Advanced Research Center for Nanolithography（先进纳米光刻研究中心）；Max-Born-Institute for Nonlinear Optics and Short Pulse Spectroscopy（马克斯·玻恩非线性光学与超短脉冲光谱研究所）；Instituto de Ciencia de Materiales de Madrid, Consejo Superior de Investigaciones Científicas（马德里材料科学研究所，西班牙高等科学研究委员会）；Department of Physics and Astronomy, and LaserLaB, Vrije Universiteit（自由大学物理与天文系及激光实验室）
Two-color harmonic spectroscopy of ultrafast Dirac electron dynamics
Technion – Israel Institute of Technology（以色列理工学院）；Guangdong Technion – Israel Institute of Technology（广东以色列理工学院）；Eastern Institute of Technology（东方理工）
State-of-the-art experiments employ strong ultrafast optical fields to study the nonlinear response of electrons in solids on an attosecond time-scale. Notably, a recent experiment retrieved a 3rd order nonlinear susceptibility by comparing the nonlinear response induced by a strong laser field to a linear response induced by the otherwise identical weak field. In parallel, experiments have demonstrated high harmonic generation (HHG) in solids, a highly nonlinear process that until recently had only been observed in gases. The highly nonlinear nature of HHG has the potential to extract even hi…
Probing of Core Excitons in Solid NaF with Polarization-Selective Attosecond Time-Resolved Four-Wave Mixing Spectroscopy
University of California, Berkeley（加州大学伯克利分校）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）；University of Regensburg（雷根斯堡大学）；Lund University（隆德大学）
"Single-shot" ultrafast spectroscopy based on the frequency encoding of transient absorbance kinetics using chirped probe pulses is analyzed theoretically. FDSS has an advantage over pump-probe spectroscopy in a situation where the "noise" is dominated by amplitude variations of the signal. Unlike "single-shot" techniques based on spatial encoding of the kinetics, no a priori knowledge of the excitation profile of the pump is needed. FDSS spectroscopy can be used for many types of samples, liquid or solid, including those comparable in thickness to the wavelength of the probe light. Another ad…
High harmonic generation in solids provides us compact and coherent UV sources. Our simulations illustrate abnormal harmonic yield dependence on the intensity of driving or pre-excitation pulses. A multielectron interference model is proposed to reveal the mechanism of the extreme nonlinear optical phenomena. We find that the $k$-resolved intraband harmonic demonstrates different symmetry, phase, and amplitude, which can be observed by using a resonant pre-excitation pulse. The position of the interference minimum obtained by solving the semiconductor Bloch equations agrees well with that obta…
We present a table-top extreme ultraviolet (XUV) beamline for measuring time- and frequency-resolved XUV excited optical luminescence (XEOL) with additional femtosecond-resolution XUV transient absorption spectroscopy functionality. XUV pulses are generated via high-harmonic generation using a near-infrared pulse in a noble gas medium, and focused to excite luminescence from a solid sample. The luminescence is collimated and guided into a streak camera, where its spectral components are temporally resolved with picosecond temporal resolution. We time-resolve XUV excited luminescence and compar…
We vary the time-frequency mode structure of ultrafast pulse-pumped modulational instability (MI) twin beams in an argon-filled hollow-core kagomé-style PCF by adjusting the pressure, pump pulse chirp, fiber length and parametric gain. Compared to solid-core systems, the pressure dependent dispersion landscape brings increased flexibility to the tailoring of frequency correlations and we demonstrate that the pump pulse chirp can be used to tune the joint spectrum of femtosecond-pumped sources. We also characterize the resulting mode content, not only by measuring the multimode second-order cor…
A femtosecond pump-probe setup is described that is optimised for broadband transient reflectivity experiments on solid samples over a wide range of temperatures. By combining a temporal resolution of 45 fs and a broad detection range between 1.75 and 2.85 eV, this apparatus can provide insightful information on the interplay between coherent collective modes and high-energy electronic excitations, which is one of the distinctive characteristics of strongly interacting and correlated quantum systems. The use of a single-shot readout CMOS array detector at frame rates up to 10 kHz allows to res…
Viscosity is an important property of out-of-equilibrium systems such as active biological materials and driven non-Newtonian fluids, and for fields ranging from biomaterials to geology, energy technologies and medicine. However, noninvasive viscosity measurements typically require integration times of seconds. Here we demonstrate a four orders-of-magnitude improvement in speed, down to twenty microseconds, with uncertainty dominated by fundamental thermal noise for the first time. We achieve this using the instantaneous velocity of a trapped particle in an optical tweezer. To resolve the inst…
