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Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC)

Attosecond Chronoscopy of Many-Body Correlations between Bloch Electrons

Josef Freudenstein, Markus Borsch, Manuel Meierhofer, D. Afanasiev, Christoph P. Schmid, Fabian Sandner, Marlene Liebich, Anna Girnghuber, Matthias Knorr, M. Kira, R. Huber

Published Jun 26, 2023• 0 citations
Publisher

Abstract

Correlations between delocalized Bloch electrons are the driving force behind key properties of solids as well as intriguing phase transitions [1]; to directly follow how many-body interactions affect intrinsic electron motion, sub-femtosecond$(1\ \text{fs}=10^{-15}\mathrm{s})$temporal resolution is desirable [2]. Multi-terahertz (THz) photon energies are perfectly matched to resonantly probe millielectronvolt (meV) correlation-induced excitations [3]. Yet, resolving the influence of correlations on the trajectories of delocalized Bloch electrons has remained an open challenge.

DOI
10.1109/cleo/europe-eqec57999.2023.10231482

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Acta Physica Sinica•Jan 1, 2016•1 citation
Correlations between delocalized Bloch electrons are the driving force behind key properties of solids as well as intriguing phase transitions [1]; to directly follow how many-body interactions affect intrinsic electron motion, sub-femtosecond(1 fs=10−15s)(1\ \text{fs}=10^{-15}\mathrm{s})(1 fs=10−15s)temporal resolution is desirable [2]. Multi-terahertz (THz) photon energies are perfectly matched to resonantly probe millielectronvolt (meV) correlation-induced excitations [3]. Yet, resolving the influence of correlations on the trajectories of delocalized Bloch electrons has remained an open challenge.
The past thirty years witnessed rapid developing of strong field physics that leads to the first generation of attosecond (10−18 s) pulses. The duration of available pulses has recently been reduced to less than 100 as, approaching the Kepler period of a classical electron revolving around the nucleus. For the first time, electron motions inside atoms, molecules and solids can be traced, probed and even steered in real time. It pushed the study on ultrafast dynamic processes into a new frontier, giving birth to attosecond physics. The development of attosecond pulses provides unprecedented coherent ultrashort XUV (extreme ultra-violet) of soft X-ray sources that enable imaging the atomic structure and resolving the related quantum dynamics for matter science. In particular, it allows the probing and monitoring of electron dynamics in the natural time scale of attoseconds with atomic spatial resolution. The generation and applications of attosecond pulses are directly related to the control and manipulation of the sub-cycle electron dynamics. Recent studies on the correlated multielectron dynamics have provided insight into the optical and dynamical properties of matter in the perspectives of time, phase and entanglement. It deepens our understanding on some of the fundamental questions, e.g., how the single or multiple photons are absorbed and how short are the quantum processes such as photoionization, tunneling ionization and charge migration. Although currently attosecond pulses are limited by the flux and pulse duration, the combination of attosecond pulses with intense infrared laser pulses paves new ways of controlling and probing electron dynamics in the domains of energy, time and space that lays the foundation for petahertz optoelectronics and attosecond pulse based transient spectroscopy. In this review, we will first briefly summarize the advancement of strong field and ultrafast physics including the relevant experimental findings, the theoretical explorations, the related technologies and the possible applications. Then we focus on the sub-cycle electron or multielectron dynamics and their manifestation on the ionization and coherent radiation properties. We start with the time behavior of Fano resonance and how it can be probed in time domain. In section 2, the correlated electron dynamics is discussed in term of anti-screening effect and Pauli effect that influence strong field ionization and high harmonic generation processes. In section 3, the coherent emission with frequency from terahertz to soft XUV and their joint measurement are discussed by emphasizing the generation mechanism of terahertz wave in two-color laser pulses. The developed high-harmonic and terahertz wave spectroscopy (HATS) is shown capable of imaging the molecular structure and dynamics. In section 4, the time-resolving of electron and hole dynamics and their coherence is proposed based on attosecond transient absorption technique. The coherence of ionization and the correlated electron dynamics is hinted crucial for electron-hole interaction. The topics are very limited and mainly selected from the perspectives of our group.
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The advent of the ultrafast laser pulse provides the powerful and efficient tool for probing the ultrafast electron dynamics in atoms and molecules. The various nonlinear process induced by the laser-matter interaction allows one to obtain the electron motion information on the sub-femtosecond time scale. A series of the ultrafast spectroscopic technique, such as attosecond streak camera, attosecond transient absorption spectrum, and etc., have been successfully applied to the probe of electron dynamics in atoms, molecules, and solids. Using two-color field is one of the significant methods to achieve the coherent control and exploring of the electron motion. This paper summarizes recent research activities in the field of the atomic and molecular ultrafast process investigated in State Key Laboratory of High Field Laser Physics, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, including the detection of the electron dynamics of the multi-bound states, measurement of the carrier envelope phase (CEP) and the phase of the attosecond pulse, and the ultrafast electron control with the THz/UV and MIR/IR field. To measure the dynamics of the multi-bound states, a broadband attosecond pulse can be used to ionize the electrons after it is excited by the pump laser. By changing the delay between the pump laser and the attosecond pulse, the measured electrons ionized by the broadband xuv attosecond pulse can present the multi-bound states dynamics simultaneously. The XUV/IR scheme is popularly used in attosecond dynamics measurement. But usually, the IR field is not very strong. We find that, if the IR field is strong enough to induce the above threshold ionization (ATI), the interference between the ATI electron and the electron from XUV pulse can be used to measure the CEP of the attosecond XUV pulse. Besides, if the electron ionized by attosecond pulse can be pushed back to the nuclei, the emission from the recombination can be used to determine the spectral phase of the attosecond pulse, which is an all-optical measurement. We also investigate the two color scheme of THz/UV and MIR/IR fields. With THz/UV two color scheme, very high electron localization can be achieved duration molecular dissociation when we use the UV pulse to excite the electron and the THz pulse to control the following electron movement. When we use the MIR/IR field to control the electron motion during the high harmonic generation, the recollision can be greatly decreased and the single attosecond pulse can be produced with multi-cycle MIR laser field.