Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Acta Physica Sinica

Research progress of the control and measurement of the atomic and molecular ultrafast electron dynamics using two-color field

Liu Can-Dong, Jia Zheng-Mao, Zheng Ying-Hui, Ge Xiao-Chun, Zeng Zhi-Nan, Ruxin Li

Published Jan 1, 2016• 1 citation
Publisher

Abstract

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.

DOI
10.7498/aps.65.223206

Related papers

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

Ultrafast quantum control of ionization dynamics in krypton

Konrad Hütten, Michael Mittermair, Sebastian O. Stock +11 more

Ultrafast spectroscopy with attosecond resolution has enabled the real time observation of ultrafast electron dynamics in atoms, molecules and solids. These experiments employ attosecond pulses or pulse trains and explore dynamical processes in a pump-probe scheme that is selectively sensitive to electronic state of matter via photoelectron or XUV absorption spectroscopy or that includes changes of the ionic state detected via photo-ion mass spectrometry. Here, we demonstrate how the implementation of combined photo-ion and absorption spectroscopy with attosecond resolution enables tracking the complex multidimensional excitation and decay cascade of an Auger auto-ionization process of a few femtoseconds in highly excited krypton. In tandem with theory, our study reveals the role of intermediate electronic states in the formation of multiply charged ions. Amplitude tuning of a dressing laser field addresses different groups of decay channels and allows exerting temporal and quantitative control over the ionization dynamics in rare gas atoms.

Nature Communications•Feb 13, 2018•41 citations

Strong-field response time and its implications on attosecond measurement

Chao Chen, Jiayin Che, Xuejiao Xie +3 more

To measure and control the electron motion in atoms and molecules by the strong laser field on the attosecond time scale is one of the research frontiers of atomic and molecular photophysics. It involves many new phenomena and processes and raises a series of questions of concepts, theories, and methods. Recent studies show that the Coulomb potential can cause the ionization time lag (about 100 attoseconds) between instants of the field maximum and the ionization-rate maximum. This lag can be understood as the response time of the electronic wave function to the strong-field-induced ionization event. It has a profound influence on the subsequent ultrafast dynamics of the ionized electron and can significantly change the time–frequency properties of electron trajectory (an important theoretical tool for attosecond measurement). Here, the research progress of response time and its implications on attosecond measurement are briefly introduced.

arXiv:2104.05511•Chinese Physics B•Sep 24, 2021•1 citation

Measuring and controlling the birth of quantum attosecond pulses

Matan Even Tzur, Chen Mor, Noa Yaffe +8 more

The generation and control of extreme ultraviolet (XUV) radiation by high harmonic generation (HHG) have advanced ultrafast science, providing direct insights into electron dynamics on their natural time scale. Attosecond science has established the capability to resolve ultrafast quantum phenomena in matter by characterizing and controlling the classical properties of the high harmonics. Recent theoretical proposals have introduced novel schemes for generating and manipulating XUV HHG with distinct quantum features, paving the way to attosecond quantum optics. In this work, we transfer fundamental concepts in quantum optics into attosecond science. By driving the HHG process with a combination of an infrared bright squeezed vacuum (BSV, a non-classical state of light), and a strong coherent field, we imprint the quantum correlations of the input BSV onto both the ultrafast electron wavefunction and the harmonics' field. Performing in-situ HHG interferometry provides an insight into the underlying sub-cycle dynamics, revealing squeezing in the statistical properties of one of the most fundamental strong-field phenomena -- field induced tunneling. Our measurement allows the reconstruction of the quantum state of the harmonics through homodyne-like tomography, resolving correlated fluctuations in the harmonic field that mirror those of the input BSV. By controlling the delay between the two driving fields, we manipulate the photon statistics of the emitted attosecond pulses with sub-cycle accuracy. The ability to measure and control quantum correlations in both electrons and XUV attosecond pulses establishes a foundation for attosecond electrodynamics, manipulating the quantum state of electrons and photons with sub-cycle precision.

arXiv:2502.09427•Feb 13, 2025•0 citations

Attosecond timing the ultrafast charge-transfer process in atomic collisions

S. X. Hu

By solving the three-dimensional, time-dependent Schr\"odinger equation, we have demonstrated that the ultrafast charge-transfer process in ion-atom collisions can be mapped out with attosecond extreme uv (xuv) pulses. During the dynamic-charge transfer from the target atom to the projectile ion, the electron coherently populates the two sites of both nuclei, which can be viewed as a ``short-lived'' molecular state. A probing attosecond xuv pulse can instantly unleash the delocalized electron from such a ``transient molecule,'' so that the resulting photoelectron may exhibit a ``double-slit'' interference. On the contrary, either reduced or no photoelectron interference will occur if the attosecond xuv pulse strikes well before or after the collision. Therefore, by monitoring the photoelectron interference visibility, one can precisely time the ultrafast charge-transfer process in atomic collisions with time-delayed attosecond xuv pulses.

Physical Review A•Apr 14, 2011•7 citations

Attosecond-resolved quantum fluctuations of light and matter

Matan Even Tzur, Chen Mor, Noa Yaffe +10 more

Until recently, attosecond optical spectroscopy and quantum optics evolved along non-overlapping directions. In attosecond science, attosecond pulses have been regarded as classical waves, applied to probe electron dynamics on their natural time scale. Here, we transfer fundamental concepts of quantum optics into attosecond physics, enabling control of both the properties of the XUV attosecond pulses and the quantum fluctuations of matter on attosecond time scales. By combining bright squeezed vacuum (BSV) with a strong laser field to drive high-harmonic generation, we transfer the quantum properties of the BSV onto the resulting XUV attosecond pulses. Applying advanced attosecond interferometry, we reconstruct the quantum state of the XUV high harmonics and their associated attosecond pulses with attosecond precision. Finally, we resolve the squeezing of the electron's wavepacket during one of the most fundamental strong-field phenomena - field induced tunneling. The ability to measure and control quantum correlations in both electrons and XUV attosecond pulses establishes a foundation for attosecond quantum electrodynamics, manipulating the quantum state of electrons and photons with sub-cycle precision.

physics.opticsCross-listedarXiv:2511.18362•Nov 25, 2025•2 citations
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.
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.
Ultrafast spectroscopy with attosecond resolution has enabled the real time observation of ultrafast electron dynamics in atoms, molecules and solids. These experiments employ attosecond pulses or pulse trains and explore dynamical processes in a pump-probe scheme that is selectively sensitive to electronic state of matter via photoelectron or XUV absorption spectroscopy or that includes changes of the ionic state detected via photo-ion mass spectrometry. Here, we demonstrate how the implementation of combined photo-ion and absorption spectroscopy with attosecond resolution enables tracking the complex multidimensional excitation and decay cascade of an Auger auto-ionization process of a few femtoseconds in highly excited krypton. In tandem with theory, our study reveals the role of intermediate electronic states in the formation of multiply charged ions. Amplitude tuning of a dressing laser field addresses different groups of decay channels and allows exerting temporal and quantitative control over the ionization dynamics in rare gas atoms.
To measure and control the electron motion in atoms and molecules by the strong laser field on the attosecond time scale is one of the research frontiers of atomic and molecular photophysics. It involves many new phenomena and processes and raises a series of questions of concepts, theories, and methods. Recent studies show that the Coulomb potential can cause the ionization time lag (about 100 attoseconds) between instants of the field maximum and the ionization-rate maximum. This lag can be understood as the response time of the electronic wave function to the strong-field-induced ionization event. It has a profound influence on the subsequent ultrafast dynamics of the ionized electron and can significantly change the time–frequency properties of electron trajectory (an important theoretical tool for attosecond measurement). Here, the research progress of response time and its implications on attosecond measurement are briefly introduced.
The generation and control of extreme ultraviolet (XUV) radiation by high harmonic generation (HHG) have advanced ultrafast science, providing direct insights into electron dynamics on their natural time scale. Attosecond science has established the capability to resolve ultrafast quantum phenomena in matter by characterizing and controlling the classical properties of the high harmonics. Recent theoretical proposals have introduced novel schemes for generating and manipulating XUV HHG with distinct quantum features, paving the way to attosecond quantum optics. In this work, we transfer fundamental concepts in quantum optics into attosecond science. By driving the HHG process with a combination of an infrared bright squeezed vacuum (BSV, a non-classical state of light), and a strong coherent field, we imprint the quantum correlations of the input BSV onto both the ultrafast electron wavefunction and the harmonics' field. Performing in-situ HHG interferometry provides an insight into the underlying sub-cycle dynamics, revealing squeezing in the statistical properties of one of the most fundamental strong-field phenomena -- field induced tunneling. Our measurement allows the reconstruction of the quantum state of the harmonics through homodyne-like tomography, resolving correlated fluctuations in the harmonic field that mirror those of the input BSV. By controlling the delay between the two driving fields, we manipulate the photon statistics of the emitted attosecond pulses with sub-cycle accuracy. The ability to measure and control quantum correlations in both electrons and XUV attosecond pulses establishes a foundation for attosecond electrodynamics, manipulating the quantum state of electrons and photons with sub-cycle precision.
By solving the three-dimensional, time-dependent Schr\"odinger equation, we have demonstrated that the ultrafast charge-transfer process in ion-atom collisions can be mapped out with attosecond extreme uv (xuv) pulses. During the dynamic-charge transfer from the target atom to the projectile ion, the electron coherently populates the two sites of both nuclei, which can be viewed as a ``short-lived'' molecular state. A probing attosecond xuv pulse can instantly unleash the delocalized electron from such a ``transient molecule,'' so that the resulting photoelectron may exhibit a ``double-slit'' interference. On the contrary, either reduced or no photoelectron interference will occur if the attosecond xuv pulse strikes well before or after the collision. Therefore, by monitoring the photoelectron interference visibility, one can precisely time the ultrafast charge-transfer process in atomic collisions with time-delayed attosecond xuv pulses.
Until recently, attosecond optical spectroscopy and quantum optics evolved along non-overlapping directions. In attosecond science, attosecond pulses have been regarded as classical waves, applied to probe electron dynamics on their natural time scale. Here, we transfer fundamental concepts of quantum optics into attosecond physics, enabling control of both the properties of the XUV attosecond pulses and the quantum fluctuations of matter on attosecond time scales. By combining bright squeezed vacuum (BSV) with a strong laser field to drive high-harmonic generation, we transfer the quantum properties of the BSV onto the resulting XUV attosecond pulses. Applying advanced attosecond interferometry, we reconstruct the quantum state of the XUV high harmonics and their associated attosecond pulses with attosecond precision. Finally, we resolve the squeezing of the electron's wavepacket during one of the most fundamental strong-field phenomena - field induced tunneling. The ability to measure and control quantum correlations in both electrons and XUV attosecond pulses establishes a foundation for attosecond quantum electrodynamics, manipulating the quantum state of electrons and photons with sub-cycle precision.