Enhancing High-Order Harmonic Generation in Light Molecules by Using Chirped Pulses

Lara-Astiaso, Manuel; Silva, R.E.F.; Gubaydullin, A. R.; Rivière, P.; Meier, Christoph; Martı́n, Fernando

doi:10.1103/physrevlett.117.093003

Cited by 64 publications

(27 citation statements)

References 54 publications

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“…In the calculations the pump pulse was optimized in order to create a coherent superposition of three states: the ground state and two low excited states, the states 2A and 1E shown if A number of issues have been subsequently explored in glycine. 380 The rst is the role and time scale of coherences between the photoelectron and the remaining cation, which was totally neglected in the previous study, as in most other treatments. Computing time dependent one particle density matrices both for the N -electron system including the photoelectron, and the (N − 1)-electron cation, as previously done, the evolution of the charge density after the pulse was compared.…”

Section: Experimental Ndingsmentioning

confidence: 99%

Attosecond Electron Dynamics in Molecules

et al. 2017

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Advances in attosecond science have led to a wealth of important discoveries in atomic, molecular, and solid-state physics and are progressively directing their footsteps toward problems of chemical interest. Relevant technical achievements in the generation and application of extreme-ultraviolet subfemtosecond pulses, the introduction of experimental techniques able to follow in time the electron dynamics in quantum systems, and the development of sophisticated theoretical methods for the interpretation of the outcomes of such experiments have raised a continuous growing interest in attosecond phenomena, as demonstrated by the vast literature on the subject. In this review, after introducing the physical mechanisms at the basis of attosecond pulse generation and attosecond technology and describing the theoretical tools that complement experimental research in this field, we 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. The measurement and control of electronic motion in complex molecular structures is a formidable challenge, for both theory and experiment, but will indubitably have a tremendous impact on chemistry in the years to come.

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Section: Experimental Ndingsmentioning

confidence: 99%

Attosecond Electron Dynamics in Molecules

et al. 2017

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“…1(c). This causes the ionization potential smaller [35] and ionization rate bigger [5]. Besides, we find that redshifts in the high energy region (inset at the top-right corner in Fig.…”

Section: Methodsmentioning

confidence: 64%

Alignment dependent ultrafast electron-nuclear dynamics in molecular high-order harmonic generation

Jia

Bian

2017

The Journal of Chemical Physics

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We investigated the high-order harmonic generation (HHG) process of diatomic molecular ion H + 2 in non-Born-Oppenheimer approximations. The corresponding three-dimensional time-dependent Schrödinger equation is solved with arbitrary alignment angles. It is found that the nuclear motion can lead to spectral modulation of HHG. Redshifts are unique in molecular HHG which decrease with the increase of alignment angles of the molecules and are sensitive to the initial vibrational states. It can be used to extract the ultrafast electron-nuclear dynamics and image molecular structure.

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“…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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Enhancing High-Order Harmonic Generation in Light Molecules by Using Chirped Pulses

Cited by 64 publications

References 54 publications

Attosecond Electron Dynamics in Molecules

Attosecond Electron Dynamics in Molecules

Alignment dependent ultrafast electron-nuclear dynamics in molecular high-order harmonic generation

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

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