Nonadiabatic Laser-Induced Alignment Dynamics of Molecules on a Surface

Lorenz Kranabetter; Henrik H Kristensen; Areg Ghazaryan; Constant A Schouder; Adam S Chatterley; Paul Janssen; Frank Jensen; Robert E Zillich; Mikhail Lemeshko; Henrik Stapelfeldt

doi:10.1103/PhysRevLett.131.053201

Nonadiabatic Laser-Induced Alignment Dynamics of Molecules on a Surface

Lorenz Kranabetter, Henrik H Kristensen, Areg Ghazaryan, Constant A Schouder, Adam S Chatterley, Paul Janssen, Frank Jensen, Robert E Zillich, Mikhail Lemeshko, Henrik Stapelfeldt^*

^*Corresponding author for this work

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaper › Journal article › Research › peer-review

10 Citations (Scopus)

Abstract

We demonstrate that a sodium dimer, Na2(1ςu+3), residing on the surface of a helium nanodroplet, can be set into rotation by a nonresonant 1.0 ps infrared laser pulse. The time-dependent degree of alignment measured, exhibits a periodic, gradually decreasing structure that deviates qualitatively from that expected for gas-phase dimers. Comparison to alignment dynamics calculated from the time-dependent rotational Schrödinger equation shows that the deviation is due to the alignment dependent interaction between the dimer and the droplet surface. This interaction confines the dimer to the tangential plane of the droplet surface at the point where it resides and is the reason that the observed alignment dynamics is also well described by a 2D quantum rotor model.

Original language	English
Article number	053201
Journal	Physical Review Letters
Volume	131
Issue	5
Number of pages	6
ISSN	0031-9007
DOIs	https://doi.org/10.1103/PhysRevLett.131.053201
Publication status	Published - 4 Aug 2023

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10.1103/PhysRevLett.131.053201

https://arxiv.org/pdf/2308.15247

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title = "Nonadiabatic Laser-Induced Alignment Dynamics of Molecules on a Surface",

abstract = "We demonstrate that a sodium dimer, Na2(1ςu+3), residing on the surface of a helium nanodroplet, can be set into rotation by a nonresonant 1.0 ps infrared laser pulse. The time-dependent degree of alignment measured, exhibits a periodic, gradually decreasing structure that deviates qualitatively from that expected for gas-phase dimers. Comparison to alignment dynamics calculated from the time-dependent rotational Schr{\"o}dinger equation shows that the deviation is due to the alignment dependent interaction between the dimer and the droplet surface. This interaction confines the dimer to the tangential plane of the droplet surface at the point where it resides and is the reason that the observed alignment dynamics is also well described by a 2D quantum rotor model.",

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doi = "10.1103/PhysRevLett.131.053201",

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T1 - Nonadiabatic Laser-Induced Alignment Dynamics of Molecules on a Surface

AU - Kranabetter, Lorenz

AU - Kristensen, Henrik H

AU - Ghazaryan, Areg

AU - Schouder, Constant A

AU - Chatterley, Adam S

AU - Janssen, Paul

AU - Jensen, Frank

AU - Zillich, Robert E

AU - Lemeshko, Mikhail

AU - Stapelfeldt, Henrik

PY - 2023/8/4

Y1 - 2023/8/4

N2 - We demonstrate that a sodium dimer, Na2(1ςu+3), residing on the surface of a helium nanodroplet, can be set into rotation by a nonresonant 1.0 ps infrared laser pulse. The time-dependent degree of alignment measured, exhibits a periodic, gradually decreasing structure that deviates qualitatively from that expected for gas-phase dimers. Comparison to alignment dynamics calculated from the time-dependent rotational Schrödinger equation shows that the deviation is due to the alignment dependent interaction between the dimer and the droplet surface. This interaction confines the dimer to the tangential plane of the droplet surface at the point where it resides and is the reason that the observed alignment dynamics is also well described by a 2D quantum rotor model.

AB - We demonstrate that a sodium dimer, Na2(1ςu+3), residing on the surface of a helium nanodroplet, can be set into rotation by a nonresonant 1.0 ps infrared laser pulse. The time-dependent degree of alignment measured, exhibits a periodic, gradually decreasing structure that deviates qualitatively from that expected for gas-phase dimers. Comparison to alignment dynamics calculated from the time-dependent rotational Schrödinger equation shows that the deviation is due to the alignment dependent interaction between the dimer and the droplet surface. This interaction confines the dimer to the tangential plane of the droplet surface at the point where it resides and is the reason that the observed alignment dynamics is also well described by a 2D quantum rotor model.

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U2 - 10.1103/PhysRevLett.131.053201

DO - 10.1103/PhysRevLett.131.053201

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VL - 131

JO - Physical Review Letters

JF - Physical Review Letters

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Nonadiabatic Laser-Induced Alignment Dynamics of Molecules on a Surface

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