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

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Wodtke,  A. M.
Department of Dynamics at Surfaces, MPI for biophysical chemistry, Max Planck Society;

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Schäfer,  T.
Department of Dynamics at Surfaces, MPI for biophysical chemistry, Max Planck Society;

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Citation

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.


Cite as: http://hdl.handle.net/11858/00-001M-0000-0014-4CA9-6
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.