Tracing and controlling electronic dynamics in atoms and molecules by attosecond pulses

Peng, Liang-You; Jiang, Wei-Chao; Geng, Jie; Xiong, Wei; Gong, Qihuang

doi:10.1016/j.physrep.2015.02.002

Cited by 118 publications

(61 citation statements)

References 679 publications

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“…While for resolving the atomic motion in molecules in time, for example, by creating and taking snapshots of a vibronic wavepacket, laser pulses with duration of several femtoseconds (10 −15 s) are sufficient, accomplishing a similar feat for the electronic motion in atoms, molecules, or condensed matter requires sub-femtosecond, that is attosecond (as), time resolution (1 as = 10 −18 s). Advances during the last decade in the development of phasecontrolled few-cycle infrared (IR) laser pulses (cycle period IR ≃ 2.7 fs at = 800 nm) and ∼ 100 attosecond XUV pulses, temporally well correlated with each other through the underlying high-harmonic generation (HHG) process Hentschel et al, 2001;Paul et al, 2001) have opened up the possibility to observe and to control electronic dynamics in matter in real time and has developed into a new field dubbed attosecond physics (see e.g., Agostini and Dimauro, 2004;Reider, 2004;Scrinzi et al, 2006;Corkum and Krausz, 2007;Bucksbaum, 2007;Kling and Vrakking, 2008;Krausz and Ivanov, 2009;Chang, 2011;Gallmann et al, 2012;Plaja et al, 2013;Schultz and Vrakking, 2013;Kim et al, 2014;Lepine et al, 2014;Krausz and Stockman, 2014;Peng et al, 2015, for reviews of the subject). Previously, time-resolved electronic dynamics was accessible only for high-lying excited states.…”

Section: Introductionmentioning

confidence: 99%

Attosecond chronoscopy of photoemission

2015

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Recent advances in the generation of well characterized sub-femtosecond laser pulses have opened up unpredicted opportunities for the real-time observation of ultrafast electronic dynamics in matter. Such attosecond chronoscopy allows a novel look at a wide range of fundamental photophysical and photochemical processes in the time domain, including Auger and autoionization processes, photoemission from atoms, molecules, and surfaces, complementing conventional energy-domain spectroscopy. Attosecond chronoscopy raises fundamental conceptual and theoretical questions as which novel information becomes accessible and which dynamical processes can be controlled and steered. These questions are currently a matter of lively debate which we address in this review. We will focus on one prototypical case, the chronoscopy of the photoelectric effect by attosecond streaking. Is photoionization instantaneous or is there a finite response time of the electronic wavefunction to the photoabsorption event? Answers to this question turn out to be far more complex and multi-faceted than initially thought. They touch upon fundamental issues of time and time delay as observables in quantum theory. We review recent progress of our understanding of time-resolved photoemission from atoms, molecules, and solids. We will highlight the unresolved and open questions and we point to future directions aiming at the observation and control of electronic motion in more complex nanoscale structures and in condensed matter.

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Section: Introductionmentioning

confidence: 99%

Attosecond chronoscopy of photoemission

2015

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“…The interaction of strong laser fields with atoms or molecules can lead to high-order harmonic generation(HHG), which can be applied as table-top coherent light sources in a wide frequency range [1][2][3][4]. Recently, much attention has been paid to the below or near-threshold harmonics because of its potential applications as coherent vacuum-ultraviolet light sources in different circumstances [5][6][7][8][9].…”

Section: Introductionmentioning

confidence: 99%

Half-cycle cutoff in near-threshold harmonic generation

et al. 2015

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A half-cycle cutoff is identified in the harmonic generation spectra near the ionization potential for short driving laser pulses. Unlike the half-cycle cutoff in the high-energy region, the newly found lowenergy cutoff is strongly affected by the ionic potential and multiple return trajectories. We show their contribution clearly in the observable harmonic spectrum based on the reference of this cutoff structure. Our results are calculated from a numerical solution to the 3D time-dependent Schrödinger equation and a classical trajectory Monte Carlo method. By comparing the results from both methods, we analyze the time-dependent sub-cycle electron dynamics and provide a transparent explanation to this half-cycle cutoff. We further investigate the low-energy harmonic yield as a function of CEP for different pulse durations. The modulation depth of this yield drops rapidly when the pulse duration is increased, which can explain the CEP-dependence recently observed in the experiment.

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“…Импульсы с длительностью порядка периода колебаний световой волны, безусловно, найдут многочисленные приме-нения в фундаментальных и прикладных исследованиях [1][2][3][4]. Эффективная генерация ПКИ позволила бы применять их для сверхбыстрого управления процессами в веществе, создавать новые типы ускорите-лей электронов и ионов.…”

Section: Introductionunclassified

“…В работах [9,10] была рассмотрена возможность генерации ПКИ непосредственно в лазере при условии когерентного взаимо-действия света с веществом, в режиме так называемой когерентной синхронизации мод. Когерентное взаимодействие света с веществом возникает, когда длительность импульса света τ p меньше времени релаксации поляризации среды 2 T , 2 τ p T  [15]. Наличие «фазовой памяти» 2 T меняет картину распро-странения света в резонансной среде.…”

Section: Introductionunclassified