Author(s) Carr, P.J.J.; Lecours, M.J.; Burt, M.; Marta, R.A.; Steinmetz, V.; Fillion, E.; Hopkins, S.
Journal J Phys Chem Lett
Date Published 2017 Dec 15

It is generally assumed that molecules behave ergodically during chemical reactions, that is, reactivities depend only on the total energy content, and not on the initial state of the molecule. While there are a few examples of non-ergodic behavior in small (usually electronically excited) species, to date there have been no reports of such behavior in larger covalently-bound species composed of several 10s of atoms. Here, we demonstrate vibrational mode-selective behavior in a series of palladium catalysts. When we excite solvent-tagged gas-phase Pd-catalysts with an infrared laser that is tuned to be resonant with specific molecular vibrations, depending on which vibration we excite, we can select different reaction pathways. We also demonstrate that this behavior can be "turned off" via chemical substitution.

DOI 10.1021/acs.jpclett.7b03030
ISSN 1948-7185
Citation Carr PJ, Lecours MJ, Burt M, Marta RA, Steinmetz V, Fillion E, et al. Mode-Selective Laser-Control of Palladium Catalyst Decomposition. J Phys Chem Lett. 2017.

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