Impulsive alignment in dense molecular gasses : high temperatures and new directions

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Abstract/Contents

Abstract
A molecular ensemble which is aligned to a laboratory-fixed axis can be useful in any number of structure determination experiments including spectroscopy, x-ray scattering, and high harmonic generation. To date, the majority of techniques aimed at achieving and measuring alignment have been developed for low-density ensembles commonly found in vacuum chambers. In this work, I explore the application of one technique, impulsive alignment, in particular, to samples at densities and pressures approaching one atmosphere. This regime is shown to represent opportunities for new measurement techniques based on optical absorption and measurements of refractive index. Specific experimental demonstrations covered within this work include alignment of a sample of molecular iodine at 425 degrees Kelvin in which centrifugal distortion and vibrational population are shown to have a significant effect on alignment. The creation and measurement of a wavepacket exhibiting both transient and static alignment along the axis of beam propagation is demonstrated as well, allowing for alignment of a symmetric top molecule along all three lab-fixed axes. Measurement techniques developed and discussed in this work include forms of both spectroscopy and interferometry. Herein, spectroscopic detection methods are demonstrated to be effective at measuring alignment at near-atmospheric densities, while revealing additional effects of driving fields, such as ionization and dissociation. A novel interferometric measurement technique is also explored and shown to be effective for nonresonant measurements of alignment. It is additionally useful in that it is capable of measuring the temporally changing refractive index of an impulsively aligned ensemble without the need for an associated birefringence.

Description

Type of resource text
Form electronic; electronic resource; remote
Extent 1 online resource.
Publication date 2013
Issuance monographic
Language English

Creators/Contributors

Associated with Broege, Douglas W
Associated with Stanford University, Department of Applied Physics.
Primary advisor Bucksbaum, Philip H
Thesis advisor Bucksbaum, Philip H
Thesis advisor Fayer, Michael D
Thesis advisor Kasevich, Mark A
Advisor Fayer, Michael D
Advisor Kasevich, Mark A

Subjects

Genre Theses

Bibliographic information

Statement of responsibility Douglas W. Broege.
Note Submitted to the Department of Applied Physics.
Thesis Thesis (Ph.D.)--Stanford University, 2013.
Location electronic resource

Access conditions

Copyright
© 2013 by Douglas Wallace Broege
License
This work is licensed under a Creative Commons Attribution Non Commercial 3.0 Unported license (CC BY-NC).

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