Molecular internal dynamics studied by quantum path interferences in high order harmonic generation

Zaïr, A.; Siegel, Thomas; Sukiasyan, Suren; Risoud, François; Brugnera, Leonardo; Hutchison, C.; Divéki, Zsolt; Auguste, T.; Tisch, J. W. G.; Salières, P.; Ivanov, Misha; Marangos, Jonathan P.

doi:10.1016/j.chemphys.2012.12.022

Cited by 29 publications

(32 citation statements)

References 30 publications

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“…The revival-like feature also appears to be associated with a 0.8π phase jump of the autocorrelation function ( Figure 3), providing a signature that should be clearly visible in quantum-path interference experiments. 23 We note that the population of the B 2g adiabatic surfaces appears to reach a minimum at t ≈ 1.4 fs, nearly simultaneously with the beginning of the phase jump. Because an identical minimum in the autocorrelation function appears in single-surface simulations (see below), the population minimum is likely coincidental.…”

Section: ■ Results and Discussionmentioning

confidence: 64%

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Short-Time Dynamics at a Conical Intersection in High-Harmonic Spectroscopy

Patchkovskii

Schuurman

2014

J. Phys. Chem. A

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Vous avez des questions? Nous pouvons vous aider. Pour communiquer directement avec un auteur, consultez la première page de la revue dans laquelle son article a été publié afin de trouver ses coordonnées. Si vous n'arrivez pas à les repérer, communiquez avec nous à PublicationsArchive-ArchivesPublications@nrc-cnrc.gc.ca. Questions? Contact the NRC Publications Archive team atPublicationsArchive-ArchivesPublications@nrc-cnrc.gc.ca. If you wish to email the authors directly, please see the first page of the publication for their contact information. NRC Publications Archive Archives des publications du CNRCThis publication could be one of several versions: author's original, accepted manuscript or the publisher's version. / La version de cette publication peut être l'une des suivantes : la version prépublication de l'auteur, la version acceptée du manuscrit ou la version de l'éditeur.Access and use of this website and the material on it are subject to the Terms and Conditions set forth at Short-time dynamics at a conical intersection in high-harmonic spectroscopy Patchkovskii, Serguei; Schuurman, Michael S.http://nparc.cisti-icist.nrc-cnrc.gc.ca/fra/droits L'accès à ce site Web et l'utilisation de son contenu sont assujettis aux conditions présentées dans le site LISEZ CES CONDITIONS ATTENTIVEMENT AVANT D'UTILISER CE SITE WEB. NRC Publications Record / Notice d'Archives des publications de CNRC:http://nparc.cisti-icist.nrc-cnrc.gc.ca/eng/view/object/?id=aad3fd82-4d1b-46b5-8a04-31cbd7427a52 http://nparc.cisti-icist.nrc-cnrc.gc.ca/fra/voir/objet/?id=aad3fd82-4d1b-46b5-8a04-31cbd7427a52 ABSTRACT: High-harmonic spectroscopy probes molecular dynamics using electrons liberated from the same molecule earlier in the laser cycle. It affords sub-Ångstrom spatial and subfemtosecond temporal resolution. Nuclear dynamics in the intermediate cation influence the spectrum of the emitted high-harmonic photons through an autocorrelation function. Here, we develop an analytical approach for computing short-time nuclear autocorrelation functions in the vicinity of conical intersections, including laser-induced and nonadiabatic coupling between the surfaces. We apply the technique to two molecules of current experimental interest, C 6 H 6 and C 6 H 5 F. In both molecules, high-harmonics generated within the same electronic channel are not sensitive to nonadiabatic dynamics, even in the presence of substantial population transfer. Calculated autocorrelation functions exhibit significant deviations from the expected Gaussian decay and may undergo revivals at short (∼1.5 fs) times. The associated phase of the nuclear wavepacket provides a possible experimental signature.

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Section: ■ Results and Discussionmentioning

confidence: 64%

“…19−22 Quantum-path interference can be used to observe coherent nuclear motion in the intermediate cations even in the absence of isotopic substitution. 23 To a first approximation, the harmonic intensity is proportional to the square modulus of the nuclear autocorrelation function η …”

Section: ■ Introductionmentioning

confidence: 99%

Short-Time Dynamics at a Conical Intersection in High-Harmonic Spectroscopy

Patchkovskii

Schuurman

2014

J. Phys. Chem. A

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“…In practice, the influence of the electron dynamics on the structural interference could be observed by following the phase difference between the short/long trajectory contributions when varying the laser intensity, e.g., by recording the Quantum Path Interferences in the total harmonic dipole 34,35 .…”

Section: Introductionmentioning

confidence: 99%

Laser-induced blurring of molecular structure information in high harmonic spectroscopy

Risoud

Lévêque

Labeye

et al. 2017

Sci Rep

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High harmonic spectroscopy gives access to molecular structure with Angström resolution. Such information is encoded in the destructive interferences occurring between the harmonic emissions from the different parts of the molecule. By solving the time-dependent Schrödinger equation, either numerically or with the molecular strong-field approximation, we show that the electron dynamics in the emission process generally results in a strong spectral smoothing of the interferences, blurring the structural information. However we identify specific generation conditions where they are unaffected. These findings have important consequences for molecular imaging and orbital tomography using high harmonic spectroscopy.

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“…Combining to such a technique an attosecond time resolution will open a new route to explore ultrafast inner-shell charge dynamics in molecular systems. One example of this is the emergence of attosecond spectroscopy where the high harmonic generation process itself is used to probe ultrafast intracation dynamics in aligned molecules [3,4]. The high harmonic generation (HHG) process allowed a time-frequency mapping due to the attosecond chirp; therefore, the intracation dynamics is encoded in the harmonic spectra.…”

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confidence: 99%

Beyond CarbonK-Edge Harmonic Emission Using a Spatial and Temporal Synthesized Laser Field

et al. 2013

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We present numerical simulations of high-order harmonic generation in helium using a temporally synthesized and spatially nonhomogeneous strong laser field. The combination of temporal and spatial laser field synthesis results in a dramatic cutoff extension far beyond the usual semiclassical limit. Our predictions are based on the convergence of three complementary approaches: resolution of the three dimensional time dependent Schrödinger equation, time-frequency analysis of the resulting dipole moment, and classical trajectory extraction. A laser field synthesized both spatially and temporally has been proven capable of generating coherent extreme ultraviolet photons beyond the carbon K edge, an energy region of high interest as it can be used to initiate inner-shell dynamics and study time-resolved intramolecular attosecond spectroscopy.

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Molecular internal dynamics studied by quantum path interferences in high order harmonic generation

Cited by 29 publications

References 30 publications

Short-Time Dynamics at a Conical Intersection in High-Harmonic Spectroscopy

Short-Time Dynamics at a Conical Intersection in High-Harmonic Spectroscopy

Laser-induced blurring of molecular structure information in high harmonic spectroscopy

Beyond CarbonK-Edge Harmonic Emission Using a Spatial and Temporal Synthesized Laser Field

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