Phase-resolved attosecond near-threshold photoionization of molecular nitrogen
Stefan Haessler,Baptiste Fabre,J. Higuet,J. Caillat,Thierry Ruchon,Pierre Breger,Bertrand Carré,Eric Constant,Alfred Maquet,Eric Mével,Pascal Salières,Richard Taïeb,Yann Mairesse +12 more
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In this paper, the phase shift for the electrons produced in the ionization channels leading to the X 2 ⌺ g +, v ǫ = 1, and vǫ Á = 2 states was observed for different states of the ion.Abstract:
We photoionize nitrogen molecules with a train of extreme ultraviolet attosecond pulses together with a weak infrared field We measure the phase of the two-color two-photon ionization transition molecular phase for different states of the ion We observe a 09 shift for the electrons produced in the ionization channels leading to the X 2 ⌺ g + , vЈ = 1, and vЈ = 2 states We relate this phase shift to the presence of a complex resonance in the continuum By providing both a high spectral and temporal resolution, this general approach gives access to the evolution of extremely short-lived states, which is often not accessible otherwise DOI: 101103/PhysRevA80011404 PACS numbers: 3380Eh, 3360ϩq, 4265Ky, 8253Kp Ionization of atoms and molecules by absorption of ul-trashort extreme ultraviolet xuv radiation provides rich structural information on the considered species The ioniza-tion process releases an electron wave packet, which can be described as a coherent superposition of partial waves The relative contributions and phases of the partial waves can be extracted from photoelectron angular distributions at a given energy 1 However, the temporal structure of the ejected wave packet, which is imposed by the phase relation between different energy components, is not accessible with such experiments To access this phase, one needs to couple two energy components of the electron wave packet and record the resulting interference This can be achieved by absorption of high-order harmonics of an infrared laser pulse in the presence of the fundamental field An intense laser pulse propagating in a gas jet produces coherent xuv radiation constituted of odd harmonics 2q +1 0 of the fundamental frequency 0 These harmonics are all approximately phase locked with the fundamental and form an attosecond pulse train APT 2 In photoionization experiments with high harmonics, the photoelectron spectrum exhibits equidistant lines resulting from single-photon ionization Fig 1a If an additional laser field with frequency 0 is added, two-photon ionization can occur: absorption of a harmonic photon accompanied by either absorption or stimulated emission of one photon 0 New lines sidebands appear in the spectrum, in between the harmonics Fig 1a Since two coherent quantum paths lead to the same sideband, interferences occur They are observed in an oscillation of the sideband amplitude as the delay between the probe ir and harmonic fields is scanned 2,3 This is the basis of the reconstruction of attosecond beating by interference of two-photon transitions RABBITT technique The phase of the oscillation is determined by the phase difference between consecutive harmonics phase locking and by additional phase characteristics of the ionization process The same process can be described in the time domain The APT creates a train of attosecond electron wave packets The additional laser field acts as an optical gate on the electrons , which can be used to retrieve the temporal profile of the electron wave packets 4,5 This temporal structure is set by the temporal shape of the APT but also by the photoion-ization process Thus, RABBITT measurements with a well-characterized APT give access to the spectral phase of the photoionization 6,7, ie, the temporal dynamics of photo-ionization Recently Cavalieri et al 8 reported a time-resolved measurement of photoionization of a solid target by a single attosecond pulse Conceptually this is close to RABBITT 4,5 but using of an APT rather than a single pulse has major advantages: i the production of APT is much less demanding; ii the spectrum of APT is a comb of narrow harmonics that can be used to identify different photoioniza-tion channels; iii the intensity of the ir beam must be of Ϸ10 11 W cm −2 for RABBITT and about 10 13 W cm −2 with single pulses 9, which can perturb the system Here we study the photoionization of nitrogen molecules with an APT and characterize the outgoing electron wave packets using the RABBITT technique We probe the region just above the ionization threshold of N 2 , which is spectro-scopically very rich 10–12 We show that the " complex resonance " at 723 nm 10,12,13 induces a Ϸ phase change in the molecular phase This effect strongly dependsread more
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Attosecond imaging of molecular electronic wavepackets
Stefan Haessler,J. Caillat,Willem Boutu,C Giovanetti-Teixeira,Thierry Ruchon,Thierry Auguste,Z. Diveki,Pierre Breger,Alfred Maquet,Bertrand Carré,Richard Taïeb,Pascal Salières +11 more
TL;DR: In this paper, the attosecond contributions of the two highest occupied molecular orbitals are analyzed and the conditions where they are disentangled in real and imaginary parts of the emission dipole moment are determined.
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Attosecond Electron Dynamics in Molecules.
TL;DR: This review will concentrate on the application of attosecond methods to the investigation of ultrafast processes in molecules, with emphasis in molecules of chemical and biological interest.
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Introduction to attosecond delays in photoionization
TL;DR: In this article, the authors present an introduction to the interaction of light and matter on the attosecond timescale and the theoretical description of ultra-short time delays and relate these to the phase of extreme ultraviolet (XUV) light pulses and to the asymptotic phaseshifts of photoelectron wave packets.
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A table-top ultrashort light source in the extreme ultraviolet for circular dichroism experiments
A. Ferré,C. Handschin,Mathieu Dumergue,Frédéric Burgy,Antoine Comby,Dominique Descamps,Baptiste Fabre,Gustavo A. Garcia,Romain Géneaux,L. Merceron,Eric Mével,Laurent Nahon,Stéphane Petit,Bernard Pons,David Staedter,Sébastien J. Weber,Thierry Ruchon,Valérie Blanchet,Yann Mairesse +18 more
TL;DR: In this article, a resonant high-order harmonic generation of an elliptical laser pulse was proposed to measure photoelectron circular dichroism on chiral molecules, opening the route to table-top time-resolved femtosecond and attosecond chiroptical experiments.
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Attosecond science: recent highlights and future trends.
TL;DR: The first ten years of attosecond science is reviewed with a selection of recent highlights and trends, and the main spectroscopic tools are introduced and recent examples of representative experiments employing them are given.
References
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Observation of a Train of Attosecond Pulses from High Harmonic Generation
TL;DR: It is found that the harmonics are locked in phase and form a train of 250-attosecond pulses in the time domain, suggesting that Harmonic generation may be a promising source for attosecond time-resolved measurements.
Journal ArticleDOI
The spectrum of molecular nitrogen
Alf Lofthus,Paul H. Krupenie +1 more
TL;DR: In this paper, a critical review and compilation of the observed and predicted spectroscopic data on the molecule N2 and its ions N2, N2−, n2−+, n 2−, N 2−+, N2++, N 2´2´−, and N2´2`− is presented, along with potential energy curves, as well as radiative lifetimes.
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Atomic transient recorder
Reinhard Kienberger,Eleftherios Goulielmakis,M. Uiberacker,Andrius Baltuška,Vladislav S. Yakovlev,F. Bammer,Armin Scrinzi,T. Westerwalbesloh,Ulf Kleineberg,Ulrich Heinzmann,Markus Drescher,Ferenc Krausz +11 more
TL;DR: With the current ∼750-nm laser probe and ∼100-eV excitation, the transient recorder is capable of resolving atomic electron dynamics within the Bohr orbit time.
Journal ArticleDOI
Attosecond spectroscopy in condensed matter
A. L. Cavalieri,Norbert Müller,Thorsten Uphues,Vladislav S. Yakovlev,Andrius Baltuška,Balint Horvath,B. E. Schmidt,L. Blumel,Ronald Holzwarth,Stefan Hendel,Markus Drescher,Ulf Kleineberg,Pedro M. Echenique,Reinhard Kienberger,Ferenc Krausz,Ulrich Heinzmann +15 more
TL;DR: The ability to obtain direct time-domain access to charge dynamics with attosecond resolution by probing photoelectron emission from single-crystal tungsten is demonstrated and illustrates thatAttosecond metrology constitutes a powerful tool for exploring not only gas-phase systems, but also fundamental electronic processes occurring on the attose Cond timescale in condensed-matter systems and on surfaces.
Journal ArticleDOI
Attosecond Synchronization of High-Harmonic Soft X-rays
Yann Mairesse,A de Bohan,Leszek J. Frasinski,Hamed Merdji,L. C. Dinu,P. Monchicourt,Pierre Breger,Milutin Kovacev,Richard Taïeb,Bertrand Carré,H. G. Muller,Pierre Agostini,Pascal Salières +12 more
TL;DR: It is shown that the synchronization could be improved considerably by controlling the underlying ultrafast electron dynamics, to provide pulses of 130 attoseconds in duration, which would allow us to track fast electron processes in matter.
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