Multiple pulse coherent dynamics and wave packet control of the N2 a" 1 Σ$$^+_g$$ dark state by attosecond four-wave mixing
Abstract
Nonlinear multidimensional spectroscopy is ubiquitous in the optical and radio frequency regions as a powerful tool to access structure and dynamics. The extension of this technique into the extreme ultraviolet (XUV) region with attosecond pulses holds promise for probing electronic dynamics and correlations with unprecedented time and spatial resolution. In this work, we use noncollinear four-wave mixing of a weak XUV attosecond pulse train (11–17 eV) and few-femtosecond NIR pulses (800 nm) to spectroscopically and dynamically probe the dipole-forbidden double-well potential of the a" 1Σ+g electronic state of nitrogen. The results demonstrate optical coupling of the inner and outer limits of the initial XUV-prepared vibrational wave packet in the valence character b' 1Σ+u state to the inner and outer wells, respectively, of the a" 1Σ+g double well state by 800 nm light. Two four-wave mixing schemes with different pulse timing sequences and noncollinear beam geometries are used (one NIR pulse collinear and one NIR pulse noncollinear versus both NIR pulses noncollinear to the XUV beam) to measure the a" dark state energetic structure and to control the dynamical preparation and motion of a dark state wave packet by selective population of either the inner Rydberg or outer valence-character potential well.more »
- Authors:
-
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1580348
- Alternate Identifier(s):
- OSTI ID: 1471430
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Faraday Discussions
- Additional Journal Information:
- Journal Volume: 212; Journal Issue: 0; Journal ID: ISSN 1359-6640
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Warrick, Erika R., Fidler, Ashley P., Cao, Wei, Bloch, Etienne, Neumark, Daniel M., and Leone, Stephen R. Multiple pulse coherent dynamics and wave packet control of the N2 a" 1 Σ$^+_g$ dark state by attosecond four-wave mixing. United States: N. p., 2018.
Web. doi:10.1039/c8fd00074c.
Warrick, Erika R., Fidler, Ashley P., Cao, Wei, Bloch, Etienne, Neumark, Daniel M., & Leone, Stephen R. Multiple pulse coherent dynamics and wave packet control of the N2 a" 1 Σ$^+_g$ dark state by attosecond four-wave mixing. United States. https://doi.org/10.1039/c8fd00074c
Warrick, Erika R., Fidler, Ashley P., Cao, Wei, Bloch, Etienne, Neumark, Daniel M., and Leone, Stephen R. Tue .
"Multiple pulse coherent dynamics and wave packet control of the N2 a" 1 Σ$^+_g$ dark state by attosecond four-wave mixing". United States. https://doi.org/10.1039/c8fd00074c. https://www.osti.gov/servlets/purl/1580348.
@article{osti_1580348,
title = {Multiple pulse coherent dynamics and wave packet control of the N2 a" 1 Σ$^+_g$ dark state by attosecond four-wave mixing},
author = {Warrick, Erika R. and Fidler, Ashley P. and Cao, Wei and Bloch, Etienne and Neumark, Daniel M. and Leone, Stephen R.},
abstractNote = {Nonlinear multidimensional spectroscopy is ubiquitous in the optical and radio frequency regions as a powerful tool to access structure and dynamics. The extension of this technique into the extreme ultraviolet (XUV) region with attosecond pulses holds promise for probing electronic dynamics and correlations with unprecedented time and spatial resolution. In this work, we use noncollinear four-wave mixing of a weak XUV attosecond pulse train (11–17 eV) and few-femtosecond NIR pulses (800 nm) to spectroscopically and dynamically probe the dipole-forbidden double-well potential of the a" 1Σ+g electronic state of nitrogen. The results demonstrate optical coupling of the inner and outer limits of the initial XUV-prepared vibrational wave packet in the valence character b' 1Σ+u state to the inner and outer wells, respectively, of the a" 1Σ+g double well state by 800 nm light. Two four-wave mixing schemes with different pulse timing sequences and noncollinear beam geometries are used (one NIR pulse collinear and one NIR pulse noncollinear versus both NIR pulses noncollinear to the XUV beam) to measure the a" dark state energetic structure and to control the dynamical preparation and motion of a dark state wave packet by selective population of either the inner Rydberg or outer valence-character potential well. Finally, experimental measurements of the a" 1Σ+g outer well vibrational spacing and anharmonicity closely match the values theoretically predicted for this previously unobserved state.},
doi = {10.1039/c8fd00074c},
journal = {Faraday Discussions},
number = 0,
volume = 212,
place = {United States},
year = {Tue May 08 00:00:00 EDT 2018},
month = {Tue May 08 00:00:00 EDT 2018}
}
Web of Science
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Works referencing / citing this record:
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