Revealing the Cooper minimum of<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:msub><mml:mi mathvariant="bold">N</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:math>by Molecular Frame High-Harmonic Spectroscopy

Bertrand, J. B.; Wörner, Hans Jakob; Hockett, Paul; Villeneuve, D. M.; Corkum, P. B.

doi:10.1103/physrevlett.109.143001

Cited by 68 publications

(65 citation statements)

References 39 publications

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“…[10,30]), irrespective of orientation and laser intensity. The two-center interference minimum of concern should not be confused with the Cooper minimum, which appears at ∼ 38 eV [23,26]. The latter minimum is related to scattering properties of the molecular potential [40] and is not considered in the present work, where we focus at larger energies, where the approach treating the continuum states as Volkov waves is reasonably accurate.…”

Section: Resultsmentioning

confidence: 99%

“…Yet the two-center interference minimum, though theoretically predicted [28,29], has never been observed experimentally [10,23,30]. We explain the lack of a two-center interference minimum in terms of laser-induced orbital distortion.…”

Section: Introductionmentioning

confidence: 81%

“…Accounting for the effects of orbital distortion allows us to resolve a long-disputed puzzle in N 2 : Both experimental and theoretical works have proven the existence of Cooper minima [19][20][21][22][23]26] and the role of multiple molecular orbital contributions in HHG spectra [27]. Yet the two-center interference minimum, though theoretically predicted [28,29], has never been observed experimentally [10,23,30].…”

Section: Introductionmentioning

confidence: 99%

“…Such a minimum may have different origin depending on the target and laser parameters, but it always carries important information about the target. For example, a Cooper minimum holds information about the electronic structure of the target [19][20][21][22][23]. Participation of multiple orbitals in the HHG process gives rise to a so-called dynamic minimum which allows elucidation of the interplay between the HOMO and lower-lying orbitals in the HHG process [24,25].…”

Section: Introductionmentioning

confidence: 99%

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High-order-harmonic generation from field-distorted orbitals

2013

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We investigate the effect on high-order harmonic generation of the distortion of molecular orbitals by the driving laser field. Calculations for high-order harmonic generation including orbital distortion are performed for N2. Our results allow us to suggest that field-distortion is the reason why the two-center interference minimum has never been observed experimentally in N2. We propose experimental parameters which should allow an observation of the two-center interference minimum.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 81%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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High-order-harmonic generation from field-distorted orbitals

2013

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“…Meanwhile, related studies were discussing the lack of experimental data for real two-center interferences in this low photon energy range to support corresponding calculations [12,13]. Effects that possibly mask the pure Young-type interference patterns are the scattering of the photoelectron on the neighboring atomic sites [4,5,12], molecular shape resonances [14,15], Cooper minima [16,17], Rydberg enhanced resonances [18], and excitation of doubly excited valence-like states [14,18]. All of them are located in the photon energy range below 100 eV.…”

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confidence: 99%

Angular Momentum Sensitive Two-Center Interference

et al. 2014

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In quantum mechanics the Young-type double-slit experiment can be performed with electrons either traveling through a double slit or being coherently emitted from two inversion symmetric molecular sites. In the latter one the valence photoionization cross sections of homonuclear diatomic molecules were predicted to oscillate over kinetic energy almost 50 years ago. Beyond the direct proof of the oscillatory behavior of these photoionization cross sections σ, we show that the angular distribution of the emitted electrons reveals hitherto unexplored information on the relative phase shift between the corresponding partial waves through two-center interference patterns. The Young-type double-slit experiment with nonzero mass quantum objects provides a very direct view on wave-particle duality. One way to observe the fundamental quantum nature is provided by electrons being coherently emitted from two inversion symmetric molecular sites. This highly debated molecular double-slit experiment is based on the assumption that coherent electron emission from homonuclear diatomic molecules such as H 2 , N 2 , and O 2 leads to observable interference phenomena in the photoionization cross section of these molecules [1]. Here, the slit distance and the wavelength of Young's classical experiment with photons correspond to the bond length and the de Broglie wavelength of the electron partial wave, respectively. It is the absence of "which-way information" that allows for interference. Therefore, most of the existing related studies focus on the inner shells of homonuclear diatomic molecules [2][3][4][5][6][7] to exploit the chemically localized but quantum mechanically nonlocalized character of the core electrons. The nonlocalization allows coherent electron emission from two slits which are fixed and spatially well defined. However, the fundamental formalism describing the molecular double slit [1] was discussed for the chemically highly delocalized valence states of N 2 and O 2 [1,8]. The basic physics of that work and the numerous K-shell studies are similar for the prediction of the oscillatory behavior of the photoionization partial cross sections σ, which is described in the following equation:Here, σ are the total and partial cross sections for which the angular momentum l denotes the individual angular momentum, Z Ã is the atomic number, k is the electron wave number, R the molecular bond length, and S is the overlap integral for the electrons localized at each site of the molecule. The equation implies that the molecular system absorbs a photon from both possible sites of electron excitation. Recent studies of the molecular double-slit phenomenon in the vibrational branching ratios of molecular photoionization gave the first experimental evidence that the basic model of Cohen and Fano is indeed valid for the valence states [9][10][11]. However, the oscillation of the partial cross sections was never directly observed. In fact, the difference between almost unexplored valence and well studied K-shell double-slit experi...

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Perspektiven für das Verständnis fundamentaler Elektronenkorrelationen durch Attosekundenspektroskopie

Kraus

Wörner

2018

Angewandte Chemie

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Zusammenfassung Molekülorbitale sind ein sehr erfolgreiches Konzept in der Chemie zur Beschreibung der elektronischen Struktur von Molekülen. Diese Beschreibung ist jedoch unzureichend, wenn die Elektronen in Molekülen stark korreliert sind und nicht als unabhängige Teilchen behandelt werden können. Die Auswirkungen solcher Elektronenkorrelationen sind allgegenwärtig in der Spektroskopie innerer Valenzelektronen durch Ultraviolet-und Röntgenstrahlen, ausserdem können Elektronenkorrelationen Ladungswanderungen in Molekülen vorantreiben und sind verantwortlich für viele exotische Eigenschaften stark korrelierter Materialien. Zeitaufgelöste Spektroskopie mit Attosekundenzeitauösung kann im Allgemeinen Elektronendynamik in Echtzeit verfolgen und kann dadurch einen experimentellen Zugang zu Phänomenen erönen, welche durch Elektronenkorrelation vorangetrieben werden. Die Spektroskopie hoher Harmonischer im Speziellen verwendet die präzise zeitabgestimmte Rekollision von laser-beschleunigten Elektronen, um die elektronische Struktur und Dynamik des untersuchten Systems auf einer sub-Femtosekunden Zeitskala zu messen. In diesem Übersichtsartikel diskutieren wir die Möglichkeiten der Spektroskopie hoher Harmonischer, um Elektronendynamik in Molekülen zu verfolgen. Wir besprechen, wie die Spektroskopie hoher Harmonischer auf qualitative und quantitative Weise analysiert werden kann, um die detaillierte Elektronendynamik in Molekülen nach Ionisierung zu verfolgen. Diese Fortschritte machen die Spektroskopie hoher Harmonischer zu einer vielversprechenden Methode, um fundamentale Elektronenkorrelationen aufzudecken und experimentelle Daten zu komplexen Elektronendynamiken bereitzustellen. * peter.kraus@berkeley.edu † hwoerner@ethz.ch; www.atto.ethz.ch 1

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Revealing the Cooper minimum ofN2by Molecular Frame High-Harmonic Spectroscopy

Abstract: /npsi/ctrl?lang=en http://nparc.cisti-icist.nrc-cnrc.gc.ca/npsi/ctrl?lang=fr Access and use of this website and the material on it are subject to the Terms and Conditions set forth at

Cited by 68 publications

References 39 publications

High-order-harmonic generation from field-distorted orbitals

High-order-harmonic generation from field-distorted orbitals

Angular Momentum Sensitive Two-Center Interference

Perspektiven für das Verständnis fundamentaler Elektronenkorrelationen durch Attosekundenspektroskopie

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