Instantaneous nonvertical electronic transitions with shaped femtosecond laser pulses: Is it possible?

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Abstract

In molecular electronic transitions, a vertical transition can be induced by an ultrashort laser pulse. That is, a replica of the initial nuclear state-times the transition dipole moment of the electronic transition-can be created instantaneously (on the time scale of nuclear motion) in the excited electronic state. Now, applying pulse shaping via the modulation of the phases of each spectral component of an ultrashort pulse, it is tempting to ask whether it is also possible to induce instantaneous nonvertical transitions to bound electronic states, provided that the phases of each spectral component of the pulse are set to appropriate values at the discrete frequencies corresponding to the energy levels of the potential. We analyze the problem in the weak-field limit, and show that such a phase requirement cannot be encoded into an ultrashort pulse. This result is equivalent to the statement that it is not possible to move matter faster than the time associated with the natural (field-free) dynamics of the system.
Original languageEnglish
JournalJournal of Chemical Physics
Volume119
Issue number5
Pages (from-to)2569-2576
ISSN0021-9606
DOIs
Publication statusPublished - 2003

Bibliographical note

Copyright (2003) American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the American Institute of Physics.

Keywords

  • DYNAMICS
  • QUANTUM CONTROL
  • CHEMICAL-REACTIONS

Cite this

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title = "Instantaneous nonvertical electronic transitions with shaped femtosecond laser pulses: Is it possible?",
abstract = "In molecular electronic transitions, a vertical transition can be induced by an ultrashort laser pulse. That is, a replica of the initial nuclear state-times the transition dipole moment of the electronic transition-can be created instantaneously (on the time scale of nuclear motion) in the excited electronic state. Now, applying pulse shaping via the modulation of the phases of each spectral component of an ultrashort pulse, it is tempting to ask whether it is also possible to induce instantaneous nonvertical transitions to bound electronic states, provided that the phases of each spectral component of the pulse are set to appropriate values at the discrete frequencies corresponding to the energy levels of the potential. We analyze the problem in the weak-field limit, and show that such a phase requirement cannot be encoded into an ultrashort pulse. This result is equivalent to the statement that it is not possible to move matter faster than the time associated with the natural (field-free) dynamics of the system.",
keywords = "DYNAMICS, QUANTUM CONTROL, CHEMICAL-REACTIONS",
author = "Henriksen, {Niels Engholm} and M{\o}ller, {Klaus Braagaard}",
note = "Copyright (2003) American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the American Institute of Physics.",
year = "2003",
doi = "10.1063/1.1586701",
language = "English",
volume = "119",
pages = "2569--2576",
journal = "Journal of Chemical Physics",
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publisher = "American Institute of Physics",
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Instantaneous nonvertical electronic transitions with shaped femtosecond laser pulses: Is it possible? / Henriksen, Niels Engholm; Møller, Klaus Braagaard.

In: Journal of Chemical Physics, Vol. 119, No. 5, 2003, p. 2569-2576.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Instantaneous nonvertical electronic transitions with shaped femtosecond laser pulses: Is it possible?

AU - Henriksen, Niels Engholm

AU - Møller, Klaus Braagaard

N1 - Copyright (2003) American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the American Institute of Physics.

PY - 2003

Y1 - 2003

N2 - In molecular electronic transitions, a vertical transition can be induced by an ultrashort laser pulse. That is, a replica of the initial nuclear state-times the transition dipole moment of the electronic transition-can be created instantaneously (on the time scale of nuclear motion) in the excited electronic state. Now, applying pulse shaping via the modulation of the phases of each spectral component of an ultrashort pulse, it is tempting to ask whether it is also possible to induce instantaneous nonvertical transitions to bound electronic states, provided that the phases of each spectral component of the pulse are set to appropriate values at the discrete frequencies corresponding to the energy levels of the potential. We analyze the problem in the weak-field limit, and show that such a phase requirement cannot be encoded into an ultrashort pulse. This result is equivalent to the statement that it is not possible to move matter faster than the time associated with the natural (field-free) dynamics of the system.

AB - In molecular electronic transitions, a vertical transition can be induced by an ultrashort laser pulse. That is, a replica of the initial nuclear state-times the transition dipole moment of the electronic transition-can be created instantaneously (on the time scale of nuclear motion) in the excited electronic state. Now, applying pulse shaping via the modulation of the phases of each spectral component of an ultrashort pulse, it is tempting to ask whether it is also possible to induce instantaneous nonvertical transitions to bound electronic states, provided that the phases of each spectral component of the pulse are set to appropriate values at the discrete frequencies corresponding to the energy levels of the potential. We analyze the problem in the weak-field limit, and show that such a phase requirement cannot be encoded into an ultrashort pulse. This result is equivalent to the statement that it is not possible to move matter faster than the time associated with the natural (field-free) dynamics of the system.

KW - DYNAMICS

KW - QUANTUM CONTROL

KW - CHEMICAL-REACTIONS

U2 - 10.1063/1.1586701

DO - 10.1063/1.1586701

M3 - Journal article

VL - 119

SP - 2569

EP - 2576

JO - Journal of Chemical Physics

JF - Journal of Chemical Physics

SN - 0021-9606

IS - 5

ER -