Mode-Selective Laser Control of Palladium Catalyst Decomposition
| Autor: | Michael J. Burt, W. Scott Hopkins, Vincent Steinmetz, Rick A. Marta, Michael J. Lecours, Eric Fillion, Patrick J. J. Carr |
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| Rok vydání: | 2017 |
| Předmět: |
Materials science
010405 organic chemistry Far-infrared laser chemistry.chemical_element 010402 general chemistry Laser 01 natural sciences Chemical reaction 0104 chemical sciences Catalysis law.invention chemistry Chemical physics law Molecular vibration Excited state Molecule General Materials Science Physics::Chemical Physics Physical and Theoretical Chemistry Palladium |
| Zdroj: | The journal of physical chemistry letters. 9(1) |
| ISSN: | 1948-7185 |
| Popis: | 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 nonergodic 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 tens 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. |
| Databáze: | OpenAIRE |
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