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  Suppression of spontaneous emission in the optical pumping of molecules: Pump-dump-sweep-probe.

Bartels, N., Krüger, B. C., Meyer, S., Wodtke, A. M., & Schäfer, T. (2013). Suppression of spontaneous emission in the optical pumping of molecules: Pump-dump-sweep-probe. The Journal of Physical Chemistry Letters, 4(14), 2367-2370. doi:10.1021/jz401266m.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-0014-4CA9-6 Version Permalink: http://hdl.handle.net/11858/00-001M-0000-0028-56E0-7
Genre: Journal Article

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http://pubs.acs.org/doi/pdf/10.1021/jz401266m (Publisher version)
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 Creators:
Bartels, N., Author
Krüger, B. C., Author
Meyer, S., Author
Wodtke, A. M.1, Author              
Schäfer, T.1, Author              
Affiliations:
1Department of Dynamics at Surfaces, MPI for biophysical chemistry, Max Planck Society, ou_578600              

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 Abstract: Optical pumping experiments on molecules are often complicated by spontaneous emission, which competes with stimulated absorption and emission processes. One well-known example is stimulated emission pumping (SEP), an optical pumping method relying on a A-transition via an excited electronic state to produce highly vibrationally excited molecules in their ground electronic state. Here, spontaneous emission populates a host of untargeted vibrational states in the optical pumping. In this Letter, we report a novel approach to suppressing spontaneous emission and show its application by preparing NO molecules in X-2 Pi(v = 16) via the transient A(2)Sigma(+)(v = 2) state. Subsequent to nanosecond time scale optical pumping, we depopulate the upper state in the A-transition by selective resonant excitation to rapidly dissociating states. We demonstrate reduction in the spontaneous emission from the A(2)Sigma(+)(v = 2) state by more than 90%. Because this method employs pulsed lasers, it is easily implemented in the ultraviolet.

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Language(s): eng - English
 Dates: 2013-07-01
 Publication Status: Published online
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 Rev. Method: Peer
 Identifiers: DOI: 10.1021/jz401266m
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Title: The Journal of Physical Chemistry Letters
Source Genre: Journal
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Pages: - Volume / Issue: 4 (14) Sequence Number: - Start / End Page: 2367 - 2370 Identifier: ISSN: 1948-7185