What will it take to observe processes in 'real time'?

Leone, Stephen R.; McCurdy, C. William; Burgdörfer, Joachim; Cederbaum, Lorenz S.; Chang, Zenghu; Dudovich, Nirit; Feist, Johannes; Greene, Chris H.; Ivanov, Misha; Kienberger, Reinhard; Keller, U.; Kling, Matthias F.; Loh, Zhi-Heng; Pfeifer, Thomas; Pfeiffer, Adrian N.; Santra, Robin; Schafer, Kenneth J.; Stolow, Albert; Thumm, Uwe; Vrakking, Marc J. J.

doi:10.1038/nphoton.2014.48

Cited by 245 publications

(182 citation statements)

References 26 publications

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“…Time-resolved electronic dynamics holds the promise to eventually go beyond observing and clocking the temporal evolution. The ultimate goal will be to actively control and manipulate electrons on the attosecond time and Ångstrom length scale (Leone et al, 2014). Realization of such a vision, dubbed "light-field electronics" (Goulielmakis et al, 2007;Schultze et al, 2012;Schiffrin et al, 2012), remains a challenge.…”

Section: Discussionmentioning

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: Discussionmentioning

confidence: 99%

Attosecond chronoscopy of photoemission

2015

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“…While streaked photoemission spectra have been recorded and modeled in many experiments [3,7,16] and theoretical investigations [16,17] for gaseous atomic targets, comparatively few time-resolved experimental [8,18,19] and theoretical [20,21] studies were carried out for solid targets [22]. This is attributable to both, experimental challenges in preparing clean and atomically flat solid surfaces and the more complicated nature of photoemission from complex targets.…”

Section: Introductionmentioning

confidence: 99%

Comparative time-resolved photoemission from the Cu(100) and Cu(111) surfaces

Ambrosio

Thumm

2016

Phys. Rev. A

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Motivated by the striking dependence of the valence electronic structure of transition metal surfaces on their crystallographic orientation, and by emerging experiments on laser-assisted extended ultraviolet (XUV) photoemission from solid surfaces, we calculate photoemission spectra from Cu(100) and Cu(111) surfaces as a function of the photoelectron final kinetic energy and the delay between the ionizing attosecond XUV pulse train and assisting infrared (IR) laser pulse. Our numerical simulations predict distinct differences in delaydependent photoelectron energy distributions and photoemission time delays for Cu(100) and Cu(111) surfaces. These differences can be scrutinized experimentally with existing technology in a suggested in situ comparative RABBITT (reconstruction of attosecond beating by interference of two-photon transitions) configuration by placing the two surfaces on a sliding platform while keeping all optical components and pathlengths fixed. Our calculations also show that the inclusion of the Fresnel-reflected incident IR pulse at the metal-vacuum interface modifies photoelectron spectra and photoemission time delays in a characteristic way that reveals the degree of spatial location of the initial electronic states.

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“…In light of the availability of attosecond pulses, the detection and experimental investigation of correlation-driven electron dynamics can be anticipated for the near future. However, even for simple systems, the interpretation of attosecond experiments is usually complicated [10]. Therefore, the tracing of correlated electron dynamics in molecules appears currently still an outstanding problem.…”

Section: Introductionmentioning

confidence: 99%

Correlation-driven charge migration following double ionization and attosecond transient absorption spectroscopy

2017

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We theoretically investigate charge migration following prompt double ionization. Thereby, we extend the concept of correlation-driven charge migration, which was introduced by Cederbaum and coworkers for single ionization [Chem. Phys. Lett. 307, 205 (1999)], to doubly ionized molecules. This allows us to demonstrate that compared to singly ionized molecules, in multiply ionized molecules, electron dynamics originating from electronic relaxation and correlation are particularly prominent. In addition, we also discuss how these correlationdriven electron dynamics might be evidenced and traced experimentally using attosecond transient absorption spectroscopy. For this purpose, we determine the time-resolved absorption cross section and find that the correlated electron dynamics discussed are reflected in it with exceptionally great detail. Strikingly, we find that features in the cross section can be traced back to electron hole populations and time-dependent partial charges and hence, can be interpreted with surprising ease. By taking advantage of element-specific core-to-valence transitions even atomic spatial resolution can be achieved. Thus, with the theoretical considerations presented, not only do we predict particularly diverse and correlated electron dynamics in molecules to follow prompt multiple ionization but we also identify a promising route towards their experimental investigation.

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What will it take to observe processes in 'real time'?

Abstract: Even for simple systems, the interpretations of new attosecond measurements are complicated and provide only a glimpse of their potential. Nonetheless, the lasting impact will be the revelation of how short-time dynamics can determine the electronic properties of more complex systems.

Cited by 245 publications

References 26 publications

Attosecond chronoscopy of photoemission

Attosecond chronoscopy of photoemission

Comparative time-resolved photoemission from the Cu(100) and Cu(111) surfaces

Correlation-driven charge migration following double ionization and attosecond transient absorption spectroscopy

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