Abstract
| Original language | English |
|---|---|
| Journal | Journal of Chemical Physics |
| Volume | 119 |
| Issue number | 5 |
| Pages (from-to) | 2569-2576 |
| ISSN | 0021-9606 |
| DOIs | |
| Publication status | Published - 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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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 journal › Journal article › Research › peer-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 -