The response time of the electron to light in photoemission is difficult to define and measure. The tunneling ionization of atoms and molecules in a strong laser field is a type of strong field-induced photoelectric effect. In this process, the electron response time will change the time of high-order harmonic generation (HHG), which will have a fundamental influence on the reconstruction of electron attosecond dynamics through HHG. We propose a simple theory to resolve the response time problem in strong field atomic tunneling ionization. The response time corresponds to the strong interaction time of three bodies i.e. Coulomb, electron and laser field, which can be determined at the quantum-classical boundary. The observable directly obtained through response time can quantitatively reproduce a series of attoclock experimental curves and provide consistent explanations for these experimental phenomena. This work introduces the main conclusions of response time theory and summarizes in detail the research progress of this theory. Firstly, this theory can be applied to the orthogonal two-color laser field to quantitatively explain the main characteristic structures of photoelectron momentum distribution (PMD). Besides, with this response time theory, the scaling law of the observable in attoclock experiment can be obtained. The proposal of scaling law is expected to provide a systematical theoretical guide for better understanding the applicability or feasibility of the attoclock under different conditions. In addition, based on the atomic response time theory, we further consider the property of multi-center Coulomb potential of molecular and develop a response time theory suitable for molecular system. Subsequently, we further apply the response time theory to polar molecules, by utilizing the asymmetry of PMD closely related to response time to recognize the permanent dipole (PD) effect within the laser sub-cycle. In the end, we discuss the prospects for research on response time. Firstly, it is envisioned to further apply response time theory to weak light and single photon transition to detect the response time of related processes. Besides, considering the significant influence of response time on the property of time-domain of HHG electron trajectories, the recombination (re-scattering) effect based on the current strong field tunneling ionization response time theory can be further investigated, thus extending this theory to describing HHG and above threshold ionization (ATI) processes. Furthermore, designing the “re-scattering electron trajectories” reconstruction scheme based on the electron trajectories with response time correction will provide important suggestions for HHG spectroscopic experiments. Finally, considering the asymmetric ionization caused by the PD effect of polar molecules, if the net ionization yield of adjacent sub-cycles is used as the current indicator, polar molecules can be used as a “micro diode” to study a type of attosecond response switching device. Polar molecular diodes emit electrons through tunneling ionization in laser field. According to the response time theory, tunneling occurs almost instantaneously, and response time needs considering only at the tunneling exit. Based on this, by searching for suitable materials (such as two-dimensional materials), it is possible to design a type of semi-classical diode (which can utilize tunneling) with femtosecond or even sub-femtosecond response time. The response time theory can provide a convenient theoretical tool for designing of such tunneling diodes.
The response time of the electron to light in photoemission is difficult to define and measure. The tunneling ionization of atoms and molecules in a strong laser field is a type of strong field-induced photoelectric effect. In this process, the electron response time will change the time of high-order harmonic generation (HHG), which will have a fundamental influence on the reconstruction of electron attosecond dynamics through HHG. We propose a simple theory to resolve the response time problem in strong field atomic tunneling ionization. The response time corresponds to the strong interaction time of three bodies i.e. Coulomb, electron and laser field, which can be determined at the quantum-classical boundary. The observable directly obtained through response time can quantitatively reproduce a series of attoclock experimental curves and provide consistent explanations for these experimental phenomena. This work introduces the main conclusions of response time theory and summarizes in detail the research progress of this theory. Firstly, this theory can be applied to the orthogonal two-color laser field to quantitatively explain the main characteristic structures of photoelectron momentum distribution (PMD). Besides, with this response time theory, the scaling law of the observable in attoclock experiment can be obtained. The proposal of scaling law is expected to provide a systematical theoretical guide for better understanding the applicability or feasibility of the attoclock under different conditions. In addition, based on the atomic response time theory, we further consider the property of multi-center Coulomb potential of molecular and develop a response time theory suitable for molecular system. Subsequently, we further apply the response time theory to polar molecules, by utilizing the asymmetry of PMD closely related to response time to recognize the permanent dipole (PD) effect within the laser sub-cycle. In the end, we discuss the prospects for research on response time. Firstly, it is envisioned to further apply response time theory to weak light and single photon transition to detect the response time of related processes. Besides, considering the significant influence of response time on the property of time-domain of HHG electron trajectories, the recombination (re-scattering) effect based on the current strong field tunneling ionization response time theory can be further investigated, thus extending this theory to describing HHG and above threshold ionization (ATI) processes. Furthermore, designing the “re-scattering electron trajectories” reconstruction scheme based on the electron trajectories with response time correction will provide important suggestions for HHG spectroscopic experiments. Finally, considering the asymmetric ionization caused by the PD effect of polar molecules, if the net ionization yield of adjacent sub-cycles is used as the current indicator, polar molecules can be used as a “micro diode” to study a type of attosecond response switching device. Polar molecular diodes emit electrons through tunneling ionization in laser field. According to the response time theory, tunneling occurs almost instantaneously, and response time needs considering only at the tunneling exit. Based on this, by searching for suitable materials (such as two-dimensional materials), it is possible to design a type of semi-classical diode (which can utilize tunneling) with femtosecond or even sub-femtosecond response time. The response time theory can provide a convenient theoretical tool for designing of such tunneling diodes.
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 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.
Laser-induced electron tunneling ionization from atoms and molecules plays as the trigger for a broad class of interesting strong-field phenomena in attosecond community. Understanding the time of electron tunneling ionization is vital to achieving the ultimate accuracy in attosecond metrology. We propose a novel attosecond photoelectron interferometer, which is based on the interference of the direct and near-forward rescattering electron wave packets, to determine the time information characterizing the tunneling process. Adding a weak perturbation in orthogonal to the strong fundamental field, the phases of the direct and the near-forward rescattering electron wave packets are modified, leading to the shift of the interferogram in the photoelectron momentum distributions. By analyzing the response of the interferogram to the perturbation, the real part of the ionization time, which denotes the instant when the electron exits the potential barrier, and the associated rescattering time are precisely retrieved. Moreover, the imaginary part of the ionization time, which has been interpreted as a quantity related to electron motion under the potential barrier, is also unambiguously determined.
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.
When matter is exposed to strong fields, electrons are ionized and a number of processes such as high harmonic generation (HHG), above threshold ionization (ATI), non-sequential ionization happen. These processes are usually investigated semiclassically, i.e. matter is treated by quantum mechanics, and radiation is treated classically. In particular HHG which is the generation of ultrashort coherent extreme ultraviolet (XUV) pulses, has enabled a wealth of novel ultrashort spectroscopic methods in atomic, molecular, and condensed matter physics. Further, ionization has applications in micro-machining. Strong field physics continues to have numerous open questions. As an illustration, the mechanisms underlying dominant HHG pathways in solids remain insufficiently understood. It is not clear which mechanism dominates HHG in various materials. Possible pathways are the interband and intraband contributions. Furthermore, many of these processes in strong field physics have been described by single active electron (SAE) approximation. This approach relies on the assumption that the interaction between a single electron and the intense laser field dominates all other interactions. However, this is clearly not the case especially in solids where interactions with the lattice and other electrons can be important. In addition, quantum optical aspects of strong field physics have generated increasing interest, yet they remain partially explored. This chapter involves treating electromagnetic fields using the formalism of second quantization. Quantum optical properties, such as squeezing, entanglement and the negativity of the Wigner function, are of fundamental importance for the field of quantum information and quantum computation. The central theme of my thesis is the development of quantum optical and statistical theoretical frameworks for describing intense laser field processes such as ionization and HHG in atomic and molecular gases and in solids. The second chapter focuses on gaining a detailed understanding of the mathematical steps involved in the Keldysh theory of ionization to establish a solid theoretical foundation. Through this analysis we identified an additional factor of two compared to Keldysh’s original derivation of atomic ionization rates. The third chapter addresses the inadequately understood mechanisms that govern dominant high harmonic generation (HHG) pathways in solids. One approach to clarify these mechanisms involves introducing real (resonant) and virtual processes. We developed the strong field adiabatic following (SFAF) formalism which is based on Dyson expansion using the von-Neumann equation of density matrix. Using SFAF a diagnostic method is obtained to separate virtual and resonant channels. Through this separation, and by comparing with experimental results, we identified the need to incorporate many-body effects. The fourth chapter explores the fact that a solid is a complex many body system in which the SAE approximation is very crude. The electron interacts with holes, other electrons, collective excitations such as plasmons, and phonons. Our work is based on the idea that all theses effects can be treated as a quantum statistical heat bath of bosonic harmonic oscillators. We apply this to our SFAF formalism. In the ionization case, this work has settled a long standing issue which is the fact that simple phenomenological approaches such as the relaxation time approximation 𝑇2 result in nonphysical enhancement of ionization. In chapter five, we have investigated ways to transfer quantum optical properties on the otherwise classical high harmonic radiation. The goal is to use HHG to scale quantum sources to smaller wavelengths. Quantum properties can be imprinted by perturbing HHG with a quantum field, such as bright squeezed vacuum (BSV). In this chapter, the theory of quantum sideband high harmonic generation (QSHHG) in atoms and solids is derived to find ways by which to transfer quantum properties from the perturbative BSV to the harmonic sideband. The theoretical framework is a quantum generalization of the semi-classical Lewenstein model of HHG. It gives closed-form solutions for the HHG and QSHHG wavefunctions. Knowing the wavefunction, we can identify the quantum properties of QSHHG. The additional photons absorbed and emitted from the quantum perturbation, here BSV, create entanglement between individual harmonic sidebands and between the harmonic sidebands and the BSV. We show how this entanglement can be used to create a variety of non-classical states commonly used in quantum information science, such as high-purity single-photon states, Schrödinger cat states, and photon-added squeezed vacuum states. Some of these non-Gaussian states with negative Wigner functions have been shown to provide a quantum computational advantage over their Gaussian counterparts. Additionally, they play a significant role in quantum metrology, enhancing precision measurements beyond classical limits. This chapter has opened a path to quantum engineering of HHG.
Strong-field tunneling ionization is the initial step for various ultrafast dynamics in intense laser-atom and/or molecule interactions. Time-resolving tunneling ionization is of crucial importance for accurately understanding these ultrafast processes. In our previous work [Phys. Rev. Lett. 121, 253203 (2018).], we proposed an attosecond photoelectron interferometer based on strong-field photoelectron holography to resolve the tunneling ionization. Here, we show more details about how the complex ionization time of tunneling is retrieved with our scheme. We demonstrate that the Coulomb interaction, which is a tedious and complex problem in dealing with photoelectron interference in strong-field ionization, can be safely canceled in our scheme. This is further confirmed by performing our scheme for both the model atoms with short-range and Coulomb potentials. Additionally, the validity and accuracy of our scheme are confirmed by its application in different targets and different laser parameters. Our scheme provides a reliable and versatile method to resolve the time information of strong-field tunneling ionization.