Sub-femtosecond stark control of molecular photoexcitation with near single-cycle pulses

Benoit Mignolet; Basile F.E. Curchod; Francoise Remacle; Todd J. Martínez

doi:10.1021/acs.jpclett.8b03814

Sub-femtosecond stark control of molecular photoexcitation with near single-cycle pulses

Benoit Mignolet^*, Basile F.E. Curchod, Francoise Remacle, Todd J. Martínez

^*Corresponding author for this work

School of Chemistry

Research output: Contribution to journal › Article (Academic Journal) › peer-review

10 Citations (Scopus)

Abstract

Electric fields can tailor molecular potential energy surfaces by interaction with the electronic state-dependent molecular dipole moment. Recent developments in optics have enabled the creation of ultrashort few-cycle optical pulses with precise control of the carrier envelope phase (CEP) that determines the offset of the maxima in the field and the pulse envelope. This opens news ways of controlling ultrafast molecular dynamics by exploiting the CEP. In this work, we show that the photoabsorption efficiency of oriented H ₂ CSO (sulfine) can be controlled by tuning the CEP. We further show that this control emanates from a resonance condition related to Stark shifting of the electronic energy levels.

Original language	English
Pages (from-to)	742-747
Number of pages	6
Journal	Journal of Physical Chemistry Letters
Volume	10
Issue number	4
DOIs	https://doi.org/10.1021/acs.jpclett.8b03814
Publication status	Published - 21 Feb 2019

Bibliographical note

Funding Information:
This work was supported by the AMOS program within the Chemical Sciences, Geosciences and Biosciences Division of the Office of Basic Energy Sciences, Office of Science, US Department of Energy. F.R. and B.M. acknowledge support from the Fonds National de la Recherche Scientifique, Belgium (F.R.S.-FNRS) and from the F.R.S.-FNRS research grants T.0132.16 and J.0012.18. Computational resources have been provided by the Consortium des Equipements de Calcul Intensif (CECI), funded by the F.R.S.-FNRS under Grant No. 2.5020.11. This work also made use of the facilities of the Hamilton HPC Service of Durham University and the XStream computational resource supported by the NSF MRI Program (Grant No. ACI-1429830).

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© 2019 American Chemical Society.

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title = "Sub-femtosecond stark control of molecular photoexcitation with near single-cycle pulses",

abstract = " Electric fields can tailor molecular potential energy surfaces by interaction with the electronic state-dependent molecular dipole moment. Recent developments in optics have enabled the creation of ultrashort few-cycle optical pulses with precise control of the carrier envelope phase (CEP) that determines the offset of the maxima in the field and the pulse envelope. This opens news ways of controlling ultrafast molecular dynamics by exploiting the CEP. In this work, we show that the photoabsorption efficiency of oriented H 2 CSO (sulfine) can be controlled by tuning the CEP. We further show that this control emanates from a resonance condition related to Stark shifting of the electronic energy levels. ",

author = "Benoit Mignolet and Curchod, \{Basile F.E.\} and Francoise Remacle and Mart{\'i}nez, \{Todd J.\}",

note = "Funding Information: This work was supported by the AMOS program within the Chemical Sciences, Geosciences and Biosciences Division of the Office of Basic Energy Sciences, Office of Science, US Department of Energy. F.R. and B.M. acknowledge support from the Fonds National de la Recherche Scientifique, Belgium (F.R.S.-FNRS) and from the F.R.S.-FNRS research grants T.0132.16 and J.0012.18. Computational resources have been provided by the Consortium des Equipements de Calcul Intensif (CECI), funded by the F.R.S.-FNRS under Grant No. 2.5020.11. This work also made use of the facilities of the Hamilton HPC Service of Durham University and the XStream computational resource supported by the NSF MRI Program (Grant No. ACI-1429830). Publisher Copyright: {\textcopyright} 2019 American Chemical Society.",

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T1 - Sub-femtosecond stark control of molecular photoexcitation with near single-cycle pulses

AU - Mignolet, Benoit

AU - Curchod, Basile F.E.

AU - Remacle, Francoise

AU - Martínez, Todd J.

N1 - Funding Information: This work was supported by the AMOS program within the Chemical Sciences, Geosciences and Biosciences Division of the Office of Basic Energy Sciences, Office of Science, US Department of Energy. F.R. and B.M. acknowledge support from the Fonds National de la Recherche Scientifique, Belgium (F.R.S.-FNRS) and from the F.R.S.-FNRS research grants T.0132.16 and J.0012.18. Computational resources have been provided by the Consortium des Equipements de Calcul Intensif (CECI), funded by the F.R.S.-FNRS under Grant No. 2.5020.11. This work also made use of the facilities of the Hamilton HPC Service of Durham University and the XStream computational resource supported by the NSF MRI Program (Grant No. ACI-1429830). Publisher Copyright: © 2019 American Chemical Society.

PY - 2019/2/21

Y1 - 2019/2/21

N2 - Electric fields can tailor molecular potential energy surfaces by interaction with the electronic state-dependent molecular dipole moment. Recent developments in optics have enabled the creation of ultrashort few-cycle optical pulses with precise control of the carrier envelope phase (CEP) that determines the offset of the maxima in the field and the pulse envelope. This opens news ways of controlling ultrafast molecular dynamics by exploiting the CEP. In this work, we show that the photoabsorption efficiency of oriented H 2 CSO (sulfine) can be controlled by tuning the CEP. We further show that this control emanates from a resonance condition related to Stark shifting of the electronic energy levels.

AB - Electric fields can tailor molecular potential energy surfaces by interaction with the electronic state-dependent molecular dipole moment. Recent developments in optics have enabled the creation of ultrashort few-cycle optical pulses with precise control of the carrier envelope phase (CEP) that determines the offset of the maxima in the field and the pulse envelope. This opens news ways of controlling ultrafast molecular dynamics by exploiting the CEP. In this work, we show that the photoabsorption efficiency of oriented H 2 CSO (sulfine) can be controlled by tuning the CEP. We further show that this control emanates from a resonance condition related to Stark shifting of the electronic energy levels.

UR - https://www.scopus.com/pages/publications/85061962308

U2 - 10.1021/acs.jpclett.8b03814

DO - 10.1021/acs.jpclett.8b03814

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JO - Journal of Physical Chemistry Letters

JF - Journal of Physical Chemistry Letters

IS - 4

ER -

Sub-femtosecond stark control of molecular photoexcitation with near single-cycle pulses

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