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Conference on Lasers and Electro-Optics

Attosecond Two-photon Atomic Transitions Containing Autoionizing States

Álvaro Jiménez-Galán, Luca Argenti, Fernando Martı́n

Published Jun 21, 2015• 0 citations
OpenAlex

Abstract

Attosecond light sources have provided the possibility to obtain a time-resolved picture of electron motion in atoms, thus allowing for the extraction of both the intensities and phases of electronic transitions. In particular, attosecond pump-probe experiments are ideally suited to investigate the role of autoionizing states in continuum atomic transitions since one can map their evolution on a time scale smaller than their lifetime.

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Using attosecond light pulses to doubly ionize a coherent doubly excited state, we show that the time-resolved correlated motion can be probed directly from the measured electron angular distributions.

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Attosecond Pump Probe: Exploring Ultrafast Electron Motion inside an Atom

S. X. Hu, Lee A. Collins

The attosecond pump probe, in close analogy to the standard femtosecond probing technique, has been proposed and theoretically demonstrated with its application to explore ultrafast electron motions inside atoms. We have performed realistic modeling for the full dynamics of both the femtosecond pumping and the attosecond probing processes. Our simulations have illustrated that an ultrashort oscillation period of 2.0 fs can be mapped out for a wave packet in low-lying excited states of the helium atom. This opens the prospect of a wealth of similar pump probe experiments to examine ultrafast electronic or atomic motions.

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This report presents the first real-time observation of electron tunnelling and multi-electron dynamics in atoms exposed to intense light. The observed sub-femtosecond ionization steps provide a powerful means of probing the transient population of short-lived valence electronic states in excited atoms offering direct, time-domain access to a wide range of multi-electron dynamics unfolding on an attosecond to femtosecond time scale. The results of pump-probe measurements are in good agreement with the predictions of the theory Keldysh put forward four decades ago.

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Strong-field control and attosecond probing of multielectron dynamics

Zengxiu Zhao

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.

Chinese Science Bulletin (Chinese Version)•Jun 5, 2020•2 citations

Photoabsorption of attosecond XUV light pulses by two strongly laser-coupled autoionizing states

Wei-Chun Chu, C. D. Lin

We study theoretically the photoabsorption spectra of an attosecond extreme ultraviolet (XUV) pulse by a laser-dressed atomic system. A weak XUV excites an autoionizing state which is strongly coupled to another autoionizing state by a laser. The theory was applied to explain two recent experiments [Loh, Greene, and Leone, Chem. Phys. 350, 7 (2008); Wang, Chini, Chen, Zhang, Cheng, He, Cheng, Wu, Thumm, and Chang, Phys. Rev. Lett. 105, 143002 (2010)] where the absorption spectra of the XUV lights were measured against the time delay between the laser and the XUV. In another example, we study an attosecond pulse exciting the $2s2p{(}^{1}\phantom{\rule{-0.16em}{0ex}}P)$ resonance of helium which is resonantly coupled to the $2{s}^{2}{(}^{1}\phantom{\rule{-0.16em}{0ex}}S)$ resonance by a moderately intense 540-nm laser. The relation between the photoabsorption spectra and the photoelectron spectra and the modification of the transmitted lights in such an experiment are analyzed. The role of Rabi flopping between the two autoionizing states within their lifetimes is investigated with respect to the laser intensity and detuning.

arXiv:1205.4766•Physical Review A•Jan 11, 2012•45 citations

Laser-assisted-autoionization dynamics of helium resonances with single attosecond pulses

Wei-Chun Chu, Song-Feng Zhao, C. D. Lin

The strong coupling between two autoionizing states in helium is studied theoretically with the pump-probe scheme. An isolated 100-as XUV pulse is used to excite helium near the $2s2p{(}^{1}\phantom{\rule{0.16em}{0ex}}P)$ resonance state in the presence of an intense infrared (IR) laser. The laser field introduces strong coupling between $2s2p{(}^{1}\phantom{\rule{0.16em}{0ex}}P)$ and $2{p}^{2}{(}^{1}\phantom{\rule{0.16em}{0ex}}S)$ states. The IR also can ionize helium from both autoionizing states. By changing the time delay between the XUV and the IR pulses, we investigated the photoelectron spectra near the two resonances. The results are used to explain the recent experiment by Gilbertson et al. [Phys. Rev. Lett. 105, 263003 (2010)]. Using the same isolated attosecond pulse and a 540-nm laser, we also investigate the strong coupling between $2s2p{(}^{1}\phantom{\rule{0.16em}{0ex}}P)$ and $2{s}^{2}{(}^{1}\phantom{\rule{0.16em}{0ex}}S)$ by examining how the photoelectron spectra are modified versus the time delay and the possibility of observing Autler-Townes doublet in such experiments.

arXiv:1205.4775•Physical Review A•Sep 29, 2011•40 citations
Attosecond light sources have provided the possibility to obtain a time-resolved picture of electron motion in atoms, thus allowing for the extraction of both the intensities and phases of electronic transitions. In particular, attosecond pump-probe experiments are ideally suited to investigate the role of autoionizing states in continuum atomic transitions since one can map their evolution on a time scale smaller than their lifetime.
The attosecond pump probe, in close analogy to the standard femtosecond probing technique, has been proposed and theoretically demonstrated with its application to explore ultrafast electron motions inside atoms. We have performed realistic modeling for the full dynamics of both the femtosecond pumping and the attosecond probing processes. Our simulations have illustrated that an ultrashort oscillation period of 2.0 fs can be mapped out for a wave packet in low-lying excited states of the helium atom. This opens the prospect of a wealth of similar pump probe experiments to examine ultrafast electronic or atomic motions.
This report presents the first real-time observation of electron tunnelling and multi-electron dynamics in atoms exposed to intense light. The observed sub-femtosecond ionization steps provide a powerful means of probing the transient population of short-lived valence electronic states in excited atoms offering direct, time-domain access to a wide range of multi-electron dynamics unfolding on an attosecond to femtosecond time scale. The results of pump-probe measurements are in good agreement with the predictions of the theory Keldysh put forward four decades ago.
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.
We study theoretically the photoabsorption spectra of an attosecond extreme ultraviolet (XUV) pulse by a laser-dressed atomic system. A weak XUV excites an autoionizing state which is strongly coupled to another autoionizing state by a laser. The theory was applied to explain two recent experiments [Loh, Greene, and Leone, Chem. Phys. 350, 7 (2008); Wang, Chini, Chen, Zhang, Cheng, He, Cheng, Wu, Thumm, and Chang, Phys. Rev. Lett. 105, 143002 (2010)] where the absorption spectra of the XUV lights were measured against the time delay between the laser and the XUV. In another example, we study an attosecond pulse exciting the 2s2p(1P)2s2p{(}^{1}\phantom{\rule{-0.16em}{0ex}}P)2s2p(1P) resonance of helium which is resonantly coupled to the 2s2(1S)2{s}^{2}{(}^{1}\phantom{\rule{-0.16em}{0ex}}S)2s2(1S) resonance by a moderately intense 540-nm laser. The relation between the photoabsorption spectra and the photoelectron spectra and the modification of the transmitted lights in such an experiment are analyzed. The role of Rabi flopping between the two autoionizing states within their lifetimes is investigated with respect to the laser intensity and detuning.
The strong coupling between two autoionizing states in helium is studied theoretically with the pump-probe scheme. An isolated 100-as XUV pulse is used to excite helium near the 2s2p(1P)2s2p{(}^{1}\phantom{\rule{0.16em}{0ex}}P)2s2p(1P) resonance state in the presence of an intense infrared (IR) laser. The laser field introduces strong coupling between 2s2p(1P)2s2p{(}^{1}\phantom{\rule{0.16em}{0ex}}P)2s2p(1P) and 2p2(1S)2{p}^{2}{(}^{1}\phantom{\rule{0.16em}{0ex}}S)2p2(1S) states. The IR also can ionize helium from both autoionizing states. By changing the time delay between the XUV and the IR pulses, we investigated the photoelectron spectra near the two resonances. The results are used to explain the recent experiment by Gilbertson et al. [Phys. Rev. Lett. 105, 263003 (2010)]. Using the same isolated attosecond pulse and a 540-nm laser, we also investigate the strong coupling between 2s2p(1P)2s2p{(}^{1}\phantom{\rule{0.16em}{0ex}}P)2s2p(1P) and 2s2(1S)2{s}^{2}{(}^{1}\phantom{\rule{0.16em}{0ex}}S)2s2(1S) by examining how the photoelectron spectra are modified versus the time delay and the possibility of observing Autler-Townes doublet in such experiments.