Determining Orientations of Optical Transition Dipole Moments Using Ultrafast X-ray Scattering

Haiwang Yong; Nikola Zotev; Brian Stankus; Jennifer M. Ruddock; Darren Bellshaw; Sébastien Boutet; Thomas J. Lane; Mengning Liang; Sergio Carbajo; Joseph S. Robinson; Wenpeng Du; Nathan Goff; Yu Chang; Jason E. Koglin; Max D. J. Waters; Theis I. Sølling; Michael P. Minitti; Adam Kirrander; Peter M. Weber

doi:10.1021/acs.jpclett.8b02773

Determining Orientations of Optical Transition Dipole Moments Using Ultrafast X-ray Scattering

Haiwang Yong, Nikola Zotev, Brian Stankus, Jennifer M. Ruddock, Darren Bellshaw, Sébastien Boutet, Thomas J. Lane, Mengning Liang, Sergio Carbajo, Joseph S. Robinson, Wenpeng Du, Nathan Goff, Yu Chang, Jason E. Koglin, Max D. J. Waters, Theis I. Sølling, Michael P. Minitti, Adam Kirrander, Peter M. Weber

Department of Chemistry

21 Citations (Scopus)

Abstract

Identification of the initially prepared, optically active state remains a challenging problem in many studies of ultrafast photoinduced processes. We show that the initially excited electronic state can be determined using the anisotropic component of ultrafast time-resolved X-ray scattering signals. The concept is demonstrated using the time-dependent X-ray scattering of N-methyl morpholine in the gas phase upon excitation by a 200 nm linearly polarized optical pulse. Analysis of the angular dependence of the scattering signal near time zero renders the orientation of the transition dipole moment in the molecular frame and identifies the initially excited state as the 3p_z Rydberg state, thus bypassing the need for further experimental studies to determine the starting point of the photoinduced dynamics and clarifying inconsistent computational results.

Original language	English
Journal	The Journal of Physical Chemistry Letters
Volume	9
Issue number	22
Pages (from-to)	6556-6562
Number of pages	7
ISSN	1948-7185
DOIs	https://doi.org/10.1021/acs.jpclett.8b02773
Publication status	Published - 15 Nov 2018

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Yong, H., Zotev, N., Stankus, B., Ruddock, J. M., Bellshaw, D., Boutet, S., Lane, T. J., Liang, M., Carbajo, S., Robinson, J. S., Du, W., Goff, N., Chang, Y., Koglin, J. E., Waters, M. D. J., Sølling, T. I., Minitti, M. P., Kirrander, A., & Weber, P. M. (2018). Determining Orientations of Optical Transition Dipole Moments Using Ultrafast X-ray Scattering. The Journal of Physical Chemistry Letters, 9(22), 6556-6562. https://doi.org/10.1021/acs.jpclett.8b02773

Yong, H, Zotev, N, Stankus, B, Ruddock, JM, Bellshaw, D, Boutet, S, Lane, TJ, Liang, M, Carbajo, S, Robinson, JS, Du, W, Goff, N, Chang, Y, Koglin, JE, Waters, MDJ, Sølling, TI, Minitti, MP, Kirrander, A & Weber, PM 2018, 'Determining Orientations of Optical Transition Dipole Moments Using Ultrafast X-ray Scattering', The Journal of Physical Chemistry Letters, vol. 9, no. 22, pp. 6556-6562. https://doi.org/10.1021/acs.jpclett.8b02773

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title = "Determining Orientations of Optical Transition Dipole Moments Using Ultrafast X-ray Scattering",

abstract = "Identification of the initially prepared, optically active state remains a challenging problem in many studies of ultrafast photoinduced processes. We show that the initially excited electronic state can be determined using the anisotropic component of ultrafast time-resolved X-ray scattering signals. The concept is demonstrated using the time-dependent X-ray scattering of N-methyl morpholine in the gas phase upon excitation by a 200 nm linearly polarized optical pulse. Analysis of the angular dependence of the scattering signal near time zero renders the orientation of the transition dipole moment in the molecular frame and identifies the initially excited state as the 3pz Rydberg state, thus bypassing the need for further experimental studies to determine the starting point of the photoinduced dynamics and clarifying inconsistent computational results.",

author = "Haiwang Yong and Nikola Zotev and Brian Stankus and Ruddock, {Jennifer M.} and Darren Bellshaw and S{\'e}bastien Boutet and Lane, {Thomas J.} and Mengning Liang and Sergio Carbajo and Robinson, {Joseph S.} and Wenpeng Du and Nathan Goff and Yu Chang and Koglin, {Jason E.} and Waters, {Max D. J.} and S{\o}lling, {Theis I.} and Minitti, {Michael P.} and Adam Kirrander and Weber, {Peter M.}",

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doi = "10.1021/acs.jpclett.8b02773",

language = "English",

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journal = "The Journal of Physical Chemistry Letters",

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T1 - Determining Orientations of Optical Transition Dipole Moments Using Ultrafast X-ray Scattering

AU - Yong, Haiwang

AU - Zotev, Nikola

AU - Stankus, Brian

AU - Ruddock, Jennifer M.

AU - Bellshaw, Darren

AU - Boutet, Sébastien

AU - Lane, Thomas J.

AU - Liang, Mengning

AU - Carbajo, Sergio

AU - Robinson, Joseph S.

AU - Du, Wenpeng

AU - Goff, Nathan

AU - Chang, Yu

AU - Koglin, Jason E.

AU - Waters, Max D. J.

AU - Sølling, Theis I.

AU - Minitti, Michael P.

AU - Kirrander, Adam

AU - Weber, Peter M.

PY - 2018/11/15

Y1 - 2018/11/15

N2 - Identification of the initially prepared, optically active state remains a challenging problem in many studies of ultrafast photoinduced processes. We show that the initially excited electronic state can be determined using the anisotropic component of ultrafast time-resolved X-ray scattering signals. The concept is demonstrated using the time-dependent X-ray scattering of N-methyl morpholine in the gas phase upon excitation by a 200 nm linearly polarized optical pulse. Analysis of the angular dependence of the scattering signal near time zero renders the orientation of the transition dipole moment in the molecular frame and identifies the initially excited state as the 3pz Rydberg state, thus bypassing the need for further experimental studies to determine the starting point of the photoinduced dynamics and clarifying inconsistent computational results.

AB - Identification of the initially prepared, optically active state remains a challenging problem in many studies of ultrafast photoinduced processes. We show that the initially excited electronic state can be determined using the anisotropic component of ultrafast time-resolved X-ray scattering signals. The concept is demonstrated using the time-dependent X-ray scattering of N-methyl morpholine in the gas phase upon excitation by a 200 nm linearly polarized optical pulse. Analysis of the angular dependence of the scattering signal near time zero renders the orientation of the transition dipole moment in the molecular frame and identifies the initially excited state as the 3pz Rydberg state, thus bypassing the need for further experimental studies to determine the starting point of the photoinduced dynamics and clarifying inconsistent computational results.

U2 - 10.1021/acs.jpclett.8b02773

DO - 10.1021/acs.jpclett.8b02773

M3 - Journal article

C2 - 30380873

SN - 1948-7185

VL - 9

SP - 6556

EP - 6562

JO - The Journal of Physical Chemistry Letters

JF - The Journal of Physical Chemistry Letters

IS - 22

ER -

Determining Orientations of Optical Transition Dipole Moments Using Ultrafast X-ray Scattering

Abstract

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