Vibrational-state and isotope dependence of high-order harmonic generation in water molecules

Falge, Mirjam; Engel, Volker; Lein, Manfred

doi:10.1103/physreva.81.023412

Cited by 21 publications

(29 citation statements)

References 45 publications

(59 reference statements)

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“…Structural information can be extracted from the harmonic signal [16] with its climax in tomographic imaging of molecular orbitals [18,20,21]. Recently, attention turned toward HHG in water molecules [22][23][24][25][26], due to the fact that it is of nontrivial structure. Therein, the contributions of different molecular orbitals to the harmonic signal could be identified [27].…”

Section: Introductionmentioning

confidence: 99%

High-order-harmonic generation from dense water microdroplets

et al. 2013

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We report on high-order-harmonic generation from micrometer-sized liquid water droplets. In pump-probe experiments, the influence of the time delay onto the emission of harmonic radiation is systematically studied. Phase-matching aspects are observed by controlling the focal position and the intensity of the probe pulse. The spatiotemporal dynamics of the droplet during interaction with intense laser pulses are studied by controlling the intensity of the pump pulse. We find transient phase-matching conditions and the expansion dynamics of the droplet to be of major influence on the harmonic yield.

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Section: Introductionmentioning

confidence: 99%

High-order-harmonic generation from dense water microdroplets

et al. 2013

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“…However, the first half revival occurs at an earlier time, and has a substantially higher magnitude (CH 4 : 2.9/2.5% at 1.93/1.98 fs for ν 4 /ν 3 ; CD 4 : 2.8/2.7% at 2.23/2.25 fs for ν 4 /ν 3 respectively). The faster short-time dynamics of vibrationally excited states has been noted before [52,65,67,85,94]. This property will be important for understanding the HHG spectra at longer wavelengths (Sec.…”

Section: A Free-cation Dynamics and Autocorrelation Functionmentioning

confidence: 65%

“…Nonetheless, most of the non-BO numerical studies of HHG still concern the dynamics of simple, oneand two-electron diatomics (H 2 [65][66][67][68], H 2 + [64,66,[68][69][70][71][72][73][74][75][76][77][78][79][80], HeH 2+ [81]), usually with the additional approximations of the reduced dimensionality [66][67][68][69][70][71][72][73][74]77,80,81] or special field polarizations [64,75,76,78,79]. Some attempts at extending the theory of nuclear dynamics in HHG to more general non-BO systems have been reported in the literature [65,[82][83][84][85][86][87][88][89][90][91]…”

Section: Published By the American Physical Society Under The Terms Omentioning

confidence: 99%

Full-dimensional treatment of short-time vibronic dynamics in a molecular high-order-harmonic-generation process in methane

Patchkovskii

Schuurman

2017

Phys. Rev. A

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We present derivation and implementation of the multiconfigurational strong-field approximation with Gaussian nuclear wave packets (MC-SFA-GWP)-a version of the molecular strong-field approximation which treats all electronic and nuclear degrees of freedom, including their correlations, quantum mechanically. The technique allows realistic simulation of high-order-harmonic emission in polyatomic molecules without invoking reduced-dimensionality models for the nuclear motion or the electronic structure. We use MC-SFA-GWP to model isotope effects in high-order-harmonic-generation (HHG) spectroscopy of methane. The HHG emission in this molecule transiently involves the strongly vibronically coupled 2 F 2 electronic state of the CH 4 + cation. We show that the isotopic HHG ratio in methane contains signatures of (a) field-free vibronic dynamics at the conical intersection (CI); (b) resonant features in the recombination cross sections; (c) laser-driven bound-state dynamics; as well as (d) the well-known short-time Gaussian decay of the emission. We assign the intrinsic vibronic feature (a) to a relatively long-lived ( 4 fs) vibronic wave packet of the singly excited ν 4 (t 2 ) and ν 2 (e) vibrational modes, strongly coupled to the components of the 2 F 2 electronic state. We demonstrate that these physical effects differ in their dependence on the wavelength, intensity, and duration of the driving pulse, allowing them to be disentangled. We thus show that HHG spectroscopy provides a versatile tool for exploring both conical intersections and resonant features in photorecombination matrix elements in the regime not easily accessible with other techniques.

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“…This suggests that the state of the electrons adapts immediately to the changing distance of the nuclei and that the laser electric field has its most significant effect mainly on the electron dynamics. Although this is true if the laser pulse is short compared with the characteristic time scale of nuclear motion, for a long pulse the nuclear motion can become relevant and can induce significant modifications on the electron dynamics [3,6,[9][10][11][12][13][14][15][16][17][18]. In particular, for a short few-cycle pulse [less than 10 optical cycles (o.c.)…”

Section: Introductionmentioning

confidence: 99%

Pulse-duration dependence of the isotopic effect in simple molecular ions driven by strong laser fields

et al. 2011

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In this paper we discuss isotopic effects in simple molecular ions subjected to strong laser fields. We show that the intensity of the emitted spectra strongly depends upon both the nuclear mass of the molecular ions and the laser pulse duration. In particular, for short pulse duration [up to 8 optical cycles (o.c.)], we confirm the trend described in the most studied case in which the high-order harmonic generation is more efficient for heavier isotopes; in contrast, an interesting physical phenomenon is predicted for pulses longer than 16 o.c. characterized by an inverse effect in which lighter molecular species are responsible for higher-order harmonic emission.

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Vibrational-state and isotope dependence of high-order harmonic generation in water molecules

Cited by 21 publications

References 45 publications

High-order-harmonic generation from dense water microdroplets

High-order-harmonic generation from dense water microdroplets

Full-dimensional treatment of short-time vibronic dynamics in a molecular high-order-harmonic-generation process in methane

Pulse-duration dependence of the isotopic effect in simple molecular ions driven by strong laser fields

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