Anisotropy control in photoelectron spectra: A coherent two-pulse interference strategy

Chamakhi, R.; Telmini, M.; Atabek, O.; Charron, Eric

doi:10.1103/physreva.100.033402

Cited by 7 publications

(3 citation statements)

References 42 publications

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“…( 26) is between the transition amplitudes T 1 , with a controlled delay τ . Such interference mechanisms have already been recently exploited in the control of rotational anisotropy [43]. A physical understanding of the mechanism can be obtained by considering the vibrational wavepacket back and forth oscillations in the excited states potentials.…”

Section: Coherent Control Strategiesmentioning

confidence: 99%

Laser control strategies in full dimensional funneling dynamics: The case of pyrazine

Mainali¹,

Gatti²,

Atabek³

2022

Preprint

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Motivated by the major role funneling dynamics plays in light-harvesting processes, we built some laser control strategies inspired from basic mechanisms such as interference and kicks, and apply them to the case of pyrazine. We are studying the internal conversion between the two excited states, the highest and directly reachable from the initial ground state being considered as a donor, and the lowest as an acceptor. The ultimate control objective is the maximum population deposit in the otherwise dark acceptor, from a two-step process: radiative excitation of the donor, followed by a conical-intersection-mediated funneling towards the acceptor. The overall idea is to first obtain the control field parameters (individual pulses leading frequency and intensity, duration and inter-pulse time delay) for tractable reduced dimensional models basically describing the conical intersection branching space. Once these parameters are optimized, they are fixed and used in full dimensional dynamics describing the electronic population transfer. In the case of pyrazine, the reduced model is 4 dimensional, whereas the full dynamics involve 24 vibrational modes. Within experimentally achievable electromagnetic field requirements, we obtain a robust control with about 60% of the ground state population deposited in the acceptor state, while about 16% remains in the donor. Moreover, we anticipate a possible transposition to the control of even larger molecular systems, for which only a small number of normal modes are active, among all the others acting as spectators in the dynamics.

show abstract

Section: Coherent Control Strategiesmentioning

confidence: 99%

Laser control strategies in full dimensional funneling dynamics: The case of pyrazine

Mainali¹,

Gatti²,

Atabek³

2022

Preprint

View full text Add to dashboard Cite

show abstract

“…( 30) is between the transition amplitudes T 1 , with a controlled delay τ. Such interference mechanisms have already been recently exploited in the control of rotational anisotropy [44] . A physical understanding of the mechanism can be obtained by considering the vibrational wavepacket back and forth oscillations in the excited states potentials.…”

Section: Coherent Control Strategiesmentioning

confidence: 99%

Laser control strategies in full-dimensional funneling dynamics: the case of pyrazine [Invited]

2022

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Motivated by the major role funneling dynamics plays in light-harvesting processes, we built some laser control strategies inspired from basic mechanisms such as interference and kicks, and applied them to the case of pyrazine. We are studying the internal conversion between the two excited states, the highest and directly reachable from the initial ground state being considered as a donor and the lowest as an acceptor. The ultimate control objective is the maximum population deposit in the otherwise dark acceptor from a two-step process: radiative excitation of the donor, followed by a conical-intersection-mediated funneling towards the acceptor. The overall idea is to first obtain the control field parameters (individual pulses leading frequency and intensity, duration, and inter-pulse time delay) for tractable reduced dimensional models basically describing the conical intersection branching space. Once these parameters are optimized, they are fixed and used in full-dimensional dynamics describing the electronic population transfer. In the case of pyrazine, the reduced model is four-dimensional, whereas the full dynamics involves 24 vibrational modes. Within experimentally achievable electromagnetic field requirements, we obtain a robust control with about 60% of the ground state population deposited in the acceptor state, while about 16% remains in the donor. Moreover, we anticipate a possible transposition to the control of even larger molecular systems, for which only a small number of normal modes are active, among all the others acting as spectators in the dynamics.

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“…Under resonant excitation, the interference asymmetry is also shown to be sensitive to pulse intensities [33]. Interference effects among ion rotational channels during photoionization have been exploited to control the asymmetry of photoelectron angular distributions at specific photoelectron energies [34]. In addition, interference effects of electronic states on vibrationally resolved photoionization in molecules have been studied [35,36].…”

Section: Introductionmentioning

confidence: 99%

Asymmetry of molecular frame photoelectron angular distributions in ${{\rm{H}}}_{2}^{+}$ by intense two-color attosecond pulses: coherent excitation and charge migration effects

Yuan

Bandrauk

2020

J. Phys. B: At. Mol. Opt. Phys.

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Molecular frame photoelectron angular distributions (MFPADs) are theoretically studied by intense two-color attosecond linearly polarized laser pulses. Simulations are performed on aligned from numerical solutions of corresponding time-dependent Schrödinger equations. Asymmetric MFPADs are produced by a time-delayed soft x-ray attosecond pulse in the presence of an extreme ultraviolet (XUV) pump pulse. We present the dependence of the asymmetry ratio Γ of the MFPADs on the laser parameters of the pump-probe pulses. The asymmetry ratio Γ varies with the time delay, illustrating the coherent superposition of electronic states. Altering the phase, intensity and duration of the pump pulse gives rise to a modulation of the asymmetry ratio Γ as well. Moreover, the asymmetry of the MFPADs disappears in the case of long duration probe pulses, illustrating the coherent charge migration dynamics on the attosecond time scale.

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Anisotropy control in photoelectron spectra: A coherent two-pulse interference strategy

Cited by 7 publications

References 42 publications

Laser control strategies in full dimensional funneling dynamics: The case of pyrazine

Laser control strategies in full dimensional funneling dynamics: The case of pyrazine

Laser control strategies in full-dimensional funneling dynamics: the case of pyrazine [Invited]

Asymmetry of molecular frame photoelectron angular distributions in ${{\rm{H}}}_{2}^{+}$ by intense two-color attosecond pulses: coherent excitation and charge migration effects

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