Axis-dependence of molecular high harmonic emission in three dimensions

Limor S. Spector; Maxim Artamonov; Shungo Miyabe; Todd Martinez; Tamar Seideman; Markus Guehr; Philip H. Bucksbaum

doi:10.1038/ncomms4190

Axis-dependence of molecular high harmonic emission in three dimensions

Limor S. Spector^*, Maxim Artamonov, Shungo Miyabe, Todd Martinez, Tamar Seideman, Markus Guehr, Philip H. Bucksbaum

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

15 Scopus citations

Abstract

High-order harmonic generation in an atomic or molecular gas is a promising source of sub-femtosecond vacuum ultraviolet coherent radiation for transient scattering, absorption, metrology and imaging applications. High harmonic spectra are sensitive to Ångstrom-scale structure and motion of laser-driven molecules, but interference from radiation produced by random molecular orientations obscures this in all but the simplest cases, such as linear molecules. Here we show how to extract full body-frame high harmonic generation information for molecules with more complicated geometries by utilizing the methods of coherent transient rotational spectroscopy. To demonstrate this approach, we obtain the relative strength of harmonic emission along the three principal axes in the asymmetric-top sulphur dioxide. This greatly simplifies the analysis task of high harmonic spectroscopy and extends its usefulness to more complex molecules.

Original language	English (US)
Article number	3190
Journal	Nature communications
Volume	5
DOIs	https://doi.org/10.1038/ncomms4190
State	Published - Feb 7 2014

ASJC Scopus subject areas

Chemistry(all)
Biochemistry, Genetics and Molecular Biology(all)
Physics and Astronomy(all)

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title = "Axis-dependence of molecular high harmonic emission in three dimensions",

abstract = "High-order harmonic generation in an atomic or molecular gas is a promising source of sub-femtosecond vacuum ultraviolet coherent radiation for transient scattering, absorption, metrology and imaging applications. High harmonic spectra are sensitive to {\AA}ngstrom-scale structure and motion of laser-driven molecules, but interference from radiation produced by random molecular orientations obscures this in all but the simplest cases, such as linear molecules. Here we show how to extract full body-frame high harmonic generation information for molecules with more complicated geometries by utilizing the methods of coherent transient rotational spectroscopy. To demonstrate this approach, we obtain the relative strength of harmonic emission along the three principal axes in the asymmetric-top sulphur dioxide. This greatly simplifies the analysis task of high harmonic spectroscopy and extends its usefulness to more complex molecules.",

author = "Spector, {Limor S.} and Maxim Artamonov and Shungo Miyabe and Todd Martinez and Tamar Seideman and Markus Guehr and Bucksbaum, {Philip H.}",

note = "Funding Information: We would like to acknowledge fruitful discussions with Varun Makhija, Xiaoming Ren, Adi Natan, Brian K. McFarland, Song Wang and Joseph P. Farrell. This research is supported through the Chemical Sciences Division of the SLAC National Accelerator Laboratory by the US Department of Energy, Office of Basic Energy Sciences and by a US Department of Energy award (Grant No. DE-FG02-04ER15612). We acknowledge support from a National Defense Science and Engineering Graduate Fellowship (L.S.S.), a Stanford Diversifying Academia, Recruiting Excellence Graduate Fellowship (L.S.S.) and an Office of Science Early Career Research Program Grant (M.G.). Publisher Copyright: {\textcopyright} 2014 Macmillan Publishers Limited. All rights reserved.",

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doi = "10.1038/ncomms4190",

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AU - Spector, Limor S.

AU - Artamonov, Maxim

AU - Miyabe, Shungo

AU - Martinez, Todd

AU - Seideman, Tamar

AU - Guehr, Markus

AU - Bucksbaum, Philip H.

N1 - Funding Information: We would like to acknowledge fruitful discussions with Varun Makhija, Xiaoming Ren, Adi Natan, Brian K. McFarland, Song Wang and Joseph P. Farrell. This research is supported through the Chemical Sciences Division of the SLAC National Accelerator Laboratory by the US Department of Energy, Office of Basic Energy Sciences and by a US Department of Energy award (Grant No. DE-FG02-04ER15612). We acknowledge support from a National Defense Science and Engineering Graduate Fellowship (L.S.S.), a Stanford Diversifying Academia, Recruiting Excellence Graduate Fellowship (L.S.S.) and an Office of Science Early Career Research Program Grant (M.G.). Publisher Copyright: © 2014 Macmillan Publishers Limited. All rights reserved.

PY - 2014/2/7

Y1 - 2014/2/7

N2 - High-order harmonic generation in an atomic or molecular gas is a promising source of sub-femtosecond vacuum ultraviolet coherent radiation for transient scattering, absorption, metrology and imaging applications. High harmonic spectra are sensitive to Ångstrom-scale structure and motion of laser-driven molecules, but interference from radiation produced by random molecular orientations obscures this in all but the simplest cases, such as linear molecules. Here we show how to extract full body-frame high harmonic generation information for molecules with more complicated geometries by utilizing the methods of coherent transient rotational spectroscopy. To demonstrate this approach, we obtain the relative strength of harmonic emission along the three principal axes in the asymmetric-top sulphur dioxide. This greatly simplifies the analysis task of high harmonic spectroscopy and extends its usefulness to more complex molecules.

AB - High-order harmonic generation in an atomic or molecular gas is a promising source of sub-femtosecond vacuum ultraviolet coherent radiation for transient scattering, absorption, metrology and imaging applications. High harmonic spectra are sensitive to Ångstrom-scale structure and motion of laser-driven molecules, but interference from radiation produced by random molecular orientations obscures this in all but the simplest cases, such as linear molecules. Here we show how to extract full body-frame high harmonic generation information for molecules with more complicated geometries by utilizing the methods of coherent transient rotational spectroscopy. To demonstrate this approach, we obtain the relative strength of harmonic emission along the three principal axes in the asymmetric-top sulphur dioxide. This greatly simplifies the analysis task of high harmonic spectroscopy and extends its usefulness to more complex molecules.

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Axis-dependence of molecular high harmonic emission in three dimensions

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