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Journal of Physics B Atomic Molecular and Optical Physics

Attosecond delays in photoionization: timeandquantum mechanics

A. Maquet, Jérémie Caillat, Richard Taïeb

Published Oct 8, 2014• 83 citations
Publisher

Abstract

This article addresses topics regarding time measurements performed on quantum systems. The motivation is linked to the advent of 'attophysics' which makes feasible to follow the motion of electrons in atoms and molecules, with time resolution at the attosecond (1 as = 10 −18 s) level, i.e. at the natural scale for electronic processes in these systems. In this context, attosecond 'time-delays' have been recently measured in experiments on photoionization and the question arises if such advances could cast a new light on the still active discussion on the status of the time variable in quantum mechanics. One issue still debatable is how to decide whether one can define a quantum time operator with eigenvalues associated to measurable 'time-delays', or time is a parameter, as it is implicit in the Newtonian classical mechanics. One objective of this paper is to investigate if the recent attophysics-based measurements could shed light on this parameter-operator conundrum. To this end, we present here the main features of the theory background, followed by an analysis of the experimental schemes that have been used to evidence attosecond 'time-delays' in photoionization. Our conclusion is that these results reinforce the view that time is a parameter which cannot be defined without reference to classical mechanics.

DOI
10.1088/0953-4075/47/20/204004

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Chinese Science Bulletin (Chinese Version)•Jun 5, 2020•2 citations
This article addresses topics regarding time measurements performed on quantum systems. The motivation is linked to the advent of 'attophysics' which makes feasible to follow the motion of electrons in atoms and molecules, with time resolution at the attosecond (1 as = 10 −18 s) level, i.e. at the natural scale for electronic processes in these systems. In this context, attosecond 'time-delays' have been recently measured in experiments on photoionization and the question arises if such advances could cast a new light on the still active discussion on the status of the time variable in quantum mechanics. One issue still debatable is how to decide whether one can define a quantum time operator with eigenvalues associated to measurable 'time-delays', or time is a parameter, as it is implicit in the Newtonian classical mechanics. One objective of this paper is to investigate if the recent attophysics-based measurements could shed light on this parameter-operator conundrum. To this end, we present here the main features of the theory background, followed by an analysis of the experimental schemes that have been used to evidence attosecond 'time-delays' in photoionization. Our conclusion is that these results reinforce the view that time is a parameter which cannot be defined without reference to classical mechanics.
The conundrum parameter-operator of time in quantum mechanics, as well as the time-energy uncertainty relation and the tunneling delay time, have recently been addressed in attosecond optical ionization experiments. Dirac's formulation of the electron's relativistic quantum mechanics (RQM) allows the introduction of a dynamical self-adjoint time operator, representing an internal time of the system. Its relation to the parametric (laboratory) time is derived. Its relevance to the tunneling measurements in these experiments is exhibited, namely, as the time it takes the wave packet to cross the exit point of the barrier, thus justifying considering this time operator an additional observable in RQM.
We theoretically study time-resolved photoemission in atoms as probed by attosecond streaking. We review recent advances in the study of the photoelectric efect in the time domain and show that the experimentally accessible time shifts can be decomposed into distinct contributions that stem from the feld-free photoionization process itself and from probe-field induced corrections. We perform accurate quantum-mechanical as well as classical simulations of attosecond streaking for efective one-electron systems and determine all relevant contributions to the time delay with attosecond precision. In particular, we investigate the properties and limitations of attosecond streaking for the transition from short-ranged potentials (photodetachment) to long-ranged Coulomb potentials (photoionization). As an example for a more complex system, we study time-resolved photoionization for endohedral fullerenes A @C 60 and discuss how streaking time shifts are modifed due to the interaction of the C 60 cage with the probing infrared streaking field.
Attosecond chronoscopy enables the exploration of correlated electron dynamics in real time. One key observable of attosecond physics is the determination of "time zero" of photoionization, the time delay with which the wave packet of the ionized electron departs from the ionic core. This observable has become accessible by experimental advances in attosecond streaking and reconstruction of attosecond beating by interference of two-photon transitions (RABBIT) techniques. In this Letter, we explore photoionization time delays by strong extreme ultraviolet fields beyond the linear-response limit. We identify novel signatures in time delays signifying strong coupling between atoms and light fields and the light-field dressing of the ion. As a prototypical case, we study the interelectronic coherence and entanglement in helium driven by a strong extreme ultraviolet field. By the numerical solution of the time-dependent Schrödinger equation in its full dimensionality, we show that the time delay of the photoionized electron allows one to monitor the ultrafast variations of coherence dynamics and entanglement in real time.
Tunneling and tunneling time are hot debated and very interesting issues because of their fundamental role in the quantum mechanics. The measurement of the tunneling time in today's attosecond and strong field (low-frequency) experiments, despite its controversial discussion offers a fruitful opportunity to understand the time measurement and the role of time in quantum mechanics. In previous work Kullie (2015 Phys. Rev. A 92 , 052118), we suggested a model and derived a simple relation to calculate the tunneling time, which showed a good agreement with the experimental result for He-atom. In the present work we analyze and discuss our model considering the experimental result for H-atom, which is obtained recently by Satya Sainadh et al (2017 arXiv: 1707.05445 ). In the tunneling region, we find that our model shows a good agreement with their experimental result (similar to the He-atom in our previous work), and with the accompanied time-dependent Schrödiger equation simulations. However, Sainadh et al use a different picture of the tunneling, in which tunneling time becomes an imaginary quantity. Whereas our model represents a real tunneling time picture, precisely a delay time with respect to the ionization time at the atomic field strength. Moreover, even though the above-threshold-ionization is beyond the tunneling regime, we still see that the actual ionization time is related to our model. However, crucial points arise and keep some questions open especially on the experimental side.
Abstract Tunneling time in attosecond and strong-field experiments is one of the most controversial issues in current research, because of its importance to the theory of time, the time operator and the time–energy uncertainty relation in quantum mechanics. In Kullie (2015 Phys. Rev. A 92 052118 ) we derived an estimation of the (real) tunneling time, which shows an excellent agreement with the time measured in attosecond experiments, our derivation is found by utilizing the time–energy uncertainty relation, and it represents a quantum clock. In this work, we show different aspects of the tunneling time in attosecond experiments, we discuss and compare the different views and approaches, which are used to calculate the tunneling time, i.e. Keldysh time (as a real or imaginary quantity), Mandelstam–Tamm time, the classical view of the time measurement and our tunneling time relation(s). We draw some conclusions concerning the validity and the relation between the different types of the tunneling time with the hope that they will help to answer the question put forward by Orlando et al (2014 J. Phys. B 47 204002 , 2014 Phys. Rev. A 89 014102 ): tunneling time, what does it mean? However, as we will see, the important question is a more general one: how to understand the time and the measurement of the time of a quantum system? In respect to our result, the time in quantum mechanics can be, in more general fashion, classified in two types, intrinsic dynamically connected, and external dynamically not connected to the system, and consequently (perhaps only) classical Newtonian time remains as a parametric type of time.
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.