Phase-only laser control in the weak-field limit: Two-pulse control of IBr photofragmentation revisited

Ashwani Kumar Tiwari, Niels Engholm Henriksen

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Abstract

We demonstrate theoretically that laser-induced coherent quantum interference control of asymptotic states of dissociating molecules is possible, starting from a single vibrational eigenstate, after the interaction with two laser pulses-at a fixed time delay-both operating in the weak-field limit. Thus, phase dependence in the interaction with the second fixed-energy phase-modulated pulse persists after the pulse is over. This is illustrated for the nonadiabatic process: I + Br*←IBr → I + Br, where the relative yield of excited Br* can be changed by pure phase modulation. Furthermore, a strong frequency dependence of the branching ratio is observed and related to the re-crossing dynamics of the avoided crossing in the above-mentioned process.
Original languageEnglish
Article number014306
JournalJournal of Chemical Physics
Volume144
Issue number1
Number of pages5
ISSN0021-9606
DOIs
Publication statusPublished - 2016

Keywords

  • Chirping
  • Phase modulation
  • Dissociation energies
  • Excitation energies

Cite this

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title = "Phase-only laser control in the weak-field limit: Two-pulse control of IBr photofragmentation revisited",
abstract = "We demonstrate theoretically that laser-induced coherent quantum interference control of asymptotic states of dissociating molecules is possible, starting from a single vibrational eigenstate, after the interaction with two laser pulses-at a fixed time delay-both operating in the weak-field limit. Thus, phase dependence in the interaction with the second fixed-energy phase-modulated pulse persists after the pulse is over. This is illustrated for the nonadiabatic process: I + Br*←IBr → I + Br, where the relative yield of excited Br* can be changed by pure phase modulation. Furthermore, a strong frequency dependence of the branching ratio is observed and related to the re-crossing dynamics of the avoided crossing in the above-mentioned process.",
keywords = "Chirping, Phase modulation, Dissociation energies, Excitation energies",
author = "Tiwari, {Ashwani Kumar} and Henriksen, {Niels Engholm}",
year = "2016",
doi = "10.1063/1.4939247",
language = "English",
volume = "144",
journal = "Journal of Chemical Physics",
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Phase-only laser control in the weak-field limit: Two-pulse control of IBr photofragmentation revisited. / Tiwari, Ashwani Kumar; Henriksen, Niels Engholm.

In: Journal of Chemical Physics, Vol. 144, No. 1, 014306, 2016.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Phase-only laser control in the weak-field limit: Two-pulse control of IBr photofragmentation revisited

AU - Tiwari, Ashwani Kumar

AU - Henriksen, Niels Engholm

PY - 2016

Y1 - 2016

N2 - We demonstrate theoretically that laser-induced coherent quantum interference control of asymptotic states of dissociating molecules is possible, starting from a single vibrational eigenstate, after the interaction with two laser pulses-at a fixed time delay-both operating in the weak-field limit. Thus, phase dependence in the interaction with the second fixed-energy phase-modulated pulse persists after the pulse is over. This is illustrated for the nonadiabatic process: I + Br*←IBr → I + Br, where the relative yield of excited Br* can be changed by pure phase modulation. Furthermore, a strong frequency dependence of the branching ratio is observed and related to the re-crossing dynamics of the avoided crossing in the above-mentioned process.

AB - We demonstrate theoretically that laser-induced coherent quantum interference control of asymptotic states of dissociating molecules is possible, starting from a single vibrational eigenstate, after the interaction with two laser pulses-at a fixed time delay-both operating in the weak-field limit. Thus, phase dependence in the interaction with the second fixed-energy phase-modulated pulse persists after the pulse is over. This is illustrated for the nonadiabatic process: I + Br*←IBr → I + Br, where the relative yield of excited Br* can be changed by pure phase modulation. Furthermore, a strong frequency dependence of the branching ratio is observed and related to the re-crossing dynamics of the avoided crossing in the above-mentioned process.

KW - Chirping

KW - Phase modulation

KW - Dissociation energies

KW - Excitation energies

U2 - 10.1063/1.4939247

DO - 10.1063/1.4939247

M3 - Journal article

VL - 144

JO - Journal of Chemical Physics

JF - Journal of Chemical Physics

SN - 0021-9606

IS - 1

M1 - 014306

ER -