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State-to-state rate coefficients for NH3–NH3 collisions from pump–probe chirped pulse experiments

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Endres,  Christian P.
Center for Astrochemical Studies at MPE, MPI for Extraterrestrial Physics, Max Planck Society;

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Caselli,  Paola
Center for Astrochemical Studies at MPE, MPI for Extraterrestrial Physics, Max Planck Society;

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Endres, C. P., Caselli, P., & Schlemmer, S. (2019). State-to-state rate coefficients for NH3–NH3 collisions from pump–probe chirped pulse experiments. The Journal of Physical Chemistry Letters, 10(17), 4836-4841. doi:10.1021/acs.jpclett.9b01653.


Cite as: http://hdl.handle.net/21.11116/0000-0005-45DA-8
Abstract
The kinetics of rotational inelastic NH3–NH3 collisions are recorded using pump–probe experiments, carried out with a K-band waveguide chirped pulse Fourier transform microwave spectrometer, in which the population of one inversion doublet is altered by the pump pulse. Due to self-collisions, the resulting deviation from equilibrium propagates to other states and, thus, can be interrogated by probe pulses as a function of the pump–probe delay time. A clear hierarchy of the state-to-state collision processes is found and subsequently translated into propensity rules. State-to-state rate coefficients are estimated, first via an analysis of the kinetics, and then more robustly and accurately derived from the pressure-dependent measurements using a global fitting procedure.