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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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 Urheber:
Bartels, N., Autor
Krüger, B. C., Autor
Meyer, S., Autor
Wodtke, A. M.1, Autor           
Schäfer, T.1, Autor           
Affiliations:
1Department of Dynamics at Surfaces, MPI for biophysical chemistry, Max Planck Society, ou_578600              

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 Zusammenfassung: 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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Sprache(n): eng - English
 Datum: 2013-07-01
 Publikationsstatus: Online veröffentlicht
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 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1021/jz401266m
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Titel: The Journal of Physical Chemistry Letters
Genre der Quelle: Zeitschrift
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Seiten: - Band / Heft: 4 (14) Artikelnummer: - Start- / Endseite: 2367 - 2370 Identifikator: ISSN: 1948-7185