Strategies for efficient field-free molecular alignment and its control

Guérin, S.

doi:10.1080/09500340802428306

Cited by 3 publications

References 19 publications

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Laser-Induced Alignment of Molecules in Helium Nanodroplets

Nielsen

Pentlehner

Christiansen

et al. 2022

Topics in Applied Physics

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Moderately intense, nonresonant laser pulses can be used to accurately control how gas phase molecules are oriented in space. This topic, driven by intense experimental and theoretical efforts, has been ever growing and developed for more than 20 years, and laser-induced alignment methods are used routinely in a number of applications in physics and chemistry. Starting in 2013, we have demonstrated that laser-induced alignment also applies to molecules dissolved in helium nanodroplets. Here we present an overview of this new work discussing alignment in both the nonadiabatic (short-pulse) and adiabatic (long-pulse) limit. We show how femtosecond or picosecond pulses can set molecules into coherent rotation that lasts for a long time and reflects the rotational structure of the helium-solvated molecules, provided the pulses are weak or, conversely, results in desolvation of the molecules when the pulses are strong. For long pulses we show that the 0.4 K temperature of the droplets, shared with the molecules or molecular complexes, leads to exceptionally high degrees of alignment. Upon rapid truncation of the laser pulse, the strong alignment can be made effectively field-free, lasting for about 10 ps thanks to slowing of molecular rotation by the helium environment. Finally, we discuss how the combination of strongly aligned molecular dimers and laser-induced Coulomb explosion imaging enables determination of the structure of the dimers. As a background and reference point, the first third of the article introduces some of the central concepts of laser-induced alignment for isolated molecules, illustrated by numerical and experimental examples.

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Laser-Induced Alignment of Molecules in Helium Nanodroplets

Nielsen

Pentlehner

Christiansen

et al. 2022

Topics in Applied Physics

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Laser-induced alignment dynamics of gas phase CS₂ dimers

Chatterley

Baatrup

Schouder

et al. 2020

Phys. Chem. Chem. Phys.

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Communication: Switched wave packets with spectrally truncated chirped pulses

Chatterley

Karamatskos

Schouder

et al. 2018

The Journal of Chemical Physics

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A new technique for obtaining switched wave packets using spectrally truncated chirped laser pulses is demonstrated experimentally and numerically by one-dimensional alignment of both linear and asymmetric top molecules. Using a simple long-pass transmission filter, a pulse with a slow turn-on and a rapid turn-off is produced. The degree of alignment, characterized by cos 2 θ 2D , rises along with the pulse intensity and reaches a maximum at the peak of the pulse. After truncation, cos 2 θ 2D drops sharply but exhibits pronounced half and full revivals. The experimental alignment dynamics trace agrees very well with a numerically calculated trace based on the solution of the time-dependent Schrödinger equation. However, the extended periods of field-free alignment of asymmetric tops following pulse truncation reported previously are not reproduced in our work. Published by AIP Publishing. https://doi

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Strategies for efficient field-free molecular alignment and its control

Abstract: Strategies using shaped laser fields to produce and control efficient field-free alignment are analyzed and compared. It is in particular shown that the strategy recently proposed using a shaped laser field combining an adiabatic ramp with a kick is superior to the bipulse strategy.

Cited by 3 publications

References 19 publications

Laser-Induced Alignment of Molecules in Helium Nanodroplets

Laser-Induced Alignment of Molecules in Helium Nanodroplets

Laser-induced alignment dynamics of gas phase CS₂ dimers

Communication: Switched wave packets with spectrally truncated chirped pulses

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Strategies for efficient field-free molecular alignment and its control

Abstract: Strategies using shaped laser fields to produce and control efficient field-free alignment are analyzed and compared. It is in particular shown that the strategy recently proposed using a shaped laser field combining an adiabatic ramp with a kick is superior to the bipulse strategy.

Cited by 3 publications

References 19 publications

Laser-Induced Alignment of Molecules in Helium Nanodroplets

Laser-Induced Alignment of Molecules in Helium Nanodroplets

Laser-induced alignment dynamics of gas phase CS2 dimers

Communication: Switched wave packets with spectrally truncated chirped pulses

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Laser-induced alignment dynamics of gas phase CS₂ dimers