Disclosing intrinsic molecular dynamics on the 1-fs scale through extreme-ultraviolet pump-probe measurements

Carpeggiani, Paolo; Tzallas, P.; Palacios, Alicia; Gray, David; Martín, Fernando; Charalambidis, D.

doi:10.1103/physreva.89.023420

Cited by 57 publications

(49 citation statements)

References 32 publications

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“…Coherences between continuum states of different energies present in the wavepacket are now in reach and manifest themselves by "quantum beats" with frequencies | ′ − | (see e.g., Yudin et al, 2005Yudin et al, , 2006Hu and Collins, 2006;Morishita et al, 2007;Kazansky et al, 2008;Mauritsson et al, 2010;Argenti and Lindroth, 2010;Tzallas et al, 2011;Pabst et al, 2011;Feist et al, 2011;Bian and Bandrauk, 2012;Klünder et al, 2013;Wirth et al, 2013;Argenti et al, 2013;Carpeggiani et al, 2014;Chini et al, 2014;Ott et al, 2014). Comparison between Eqs.…”

Section: )mentioning

confidence: 99%

“…The time encoded in the wavepacket of the receding electron carries information on the initial localization within the molecule as well on the near-field of neighboring atomic constituents. The simplest prototypical case is the photoionization of a diatomic molecule (Fernández et al, 2007;Hu et al, 2009;Guan et al, 2011;Ivanov et al, 2012;Bian and Bandrauk, 2012;Serov et al, 2013;Carpeggiani et al, 2014;Ning et al, 2014;Chacon et al, 2014). Among the fundamental questions to be addressed are: Does it take a longer time for the electron to escape from the multicenter molecular core than from the one-center atomic core?…”

Section: Time-resolved Photoionization Of Moleculesmentioning

confidence: 99%

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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: )mentioning

confidence: 99%

Section: Time-resolved Photoionization Of Moleculesmentioning

confidence: 99%

Attosecond chronoscopy of photoemission

2015

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“…In a work by Ranitovic et al [23], VUV attosecond coherent control methods were used to excite and steer the dynamics of highly excited electronic states in a D 2 * molecule on an attosecond time scale. In another pump-probe experiment, short VUV-or-XUV pulses were used to excite a broad range of neutral states in the D 2 molecule that were subsequently ionized by a second XUV pulse [24].…”

Section: Introductionmentioning

confidence: 99%

Mapping and controlling ultrafast dynamics of highly excited H2 molecules by VUV-IR pump-probe schemes

et al. 2017

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We used ultrashort femtosecond vacuum ultraviolet (VUV) and infrared (IR) pulses in a pump-probe scheme to map the dynamics and nonequilibrium dissociation channels of excited neutral H 2 molecules. A nuclear wave packet is created in the B 1 + u state of the neutral H 2 molecule by absorption of the ninth harmonic of the driving infrared laser field. Due to the large stretching amplitude of the molecule excited in the B 1 + u electronic state, the effective H 2 + ionization potential changes significantly as the nuclear wave packet vibrates in the bound, highly electronically and vibrationally excited B potential-energy curve. We probed such dynamics by ionizing the excited neutral molecule using time-delayed VUV-or-IR radiation. We identified the nonequilibrium dissociation channels by utilizing three-dimensional momentum imaging of the ion fragments. We found that different dissociation channels can be controlled, to some extent, by changing the IR laser intensity and by choosing the wavelength of the probe laser light. Furthermore, we concluded that even in a benchmark molecular system such as H 2 *, the interpretation of the nonequilibrium multiphoton and multicolor ionization processes is still a challenging task, requiring intricate theoretical analysis.

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“…It has been found that the intensities of the XUV pulses in the interaction area can be up to 10 14 W/cm 2 [48], while their durations can be obtained by means of 2-IVAC measurements in case the CEP of the driving field is stabilized or measured and tagging approaches are applied [48,156]. These pulses were used for the observation of two-XUV-photon double ionization in Xenon gas (which has been placed in T-GJ) [48], for time-resolved XUV spectroscopy studies [157] and XUV-XUV pump-probe measurements of~1 fs scale dynamics in atoms [48] and molecules [158]. The temporal characterization of asec pulses generated in gas-phase media will be described in Section 4.…”

Section: Asec Beam Lines For Gas Phase Mediamentioning

confidence: 99%

“…While XUV-pump-XUV-probe experiments have been performed in the~1 fs time scale [48,158,180] it is not rigorously proven that they were using pulses of asec duration. The importance of XUV-pump-XUV-probe experiments has been stressed in a recent publication [181] highlighting the fact that XUV-IR pump-probe experiments might suffer from distortions of the system under instigation due to in some cases high intensity IR pulses are unavoidable.…”

Section: Conclusion and Ongoing Development On Gas-phase And Solid-smentioning

confidence: 99%

Generation of Attosecond Light Pulses from Gas and Solid State Media

et al. 2017

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Real-time observation of ultrafast dynamics in the microcosm is a fundamental approach for understanding the internal evolution of physical, chemical and biological systems. Tools for tracing such dynamics are flashes of light with duration comparable to or shorter than the characteristic evolution times of the system under investigation. While femtosecond (fs) pulses are successfully used to investigate vibrational dynamics in molecular systems, real time observation of electron motion in all states of matter requires temporal resolution in the attosecond (1 attosecond (asec) = 10 −18 s) time scale. During the last decades, continuous efforts in ultra-short pulse engineering led to the development of table-top sources which can produce asec pulses. These pulses have been synthesized by using broadband coherent radiation in the extreme ultraviolet (XUV) spectral region generated by the interaction of matter with intense fs pulses. Here, we will review asec pulses generated by the interaction of gas phase media and solid surfaces with intense fs IR laser fields. After a brief overview of the fundamental process underlying the XUV emission form these media, we will review the current technology, specifications and the ongoing developments of such asec sources.

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Disclosing intrinsic molecular dynamics on the 1-fs scale through extreme-ultraviolet pump-probe measurements

Cited by 57 publications

References 32 publications

Attosecond chronoscopy of photoemission

Attosecond chronoscopy of photoemission

Mapping and controlling ultrafast dynamics of highly excited H2 molecules by VUV-IR pump-probe schemes

Generation of Attosecond Light Pulses from Gas and Solid State Media

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