Mode-Selective Laser Control of Palladium Catalyst Decomposition,The Journal of Physical Chemistry Letters

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Mode-Selective Laser Control of Palladium Catalyst Decomposition
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2017-12-21 00:00:00 , DOI: 10.1021/acs.jpclett.7b03030
Patrick J. J. Carr ₁ , Michael J. Lecours ₁ , Michael J. Burt ₁ , Rick A. Marta ₁ , Vincent Steinmetz ₂ , Eric Fillion ₁ , W. Scott Hopkins ₁

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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.

中文翻译：

钯催化剂分解的模式选择激光控制

通常假设分子在化学反应过程中具有人体工程学的特性，也就是说，反应性仅取决于总能量含量，而不取决于分子的初始状态。虽然在少数（通常是电子激发的）物种中有一些非遍历行为的例子，但迄今为止，还没有关于由几十个原子组成的较大的共价结合物种中这种行为的报道。在这里，我们展示了一系列钯催化剂中的振动模式选择性行为。当我们使用红外激光激发溶剂标记的气相Pd催化剂时，可以将其调谐为与特定的分子振动共振，具体取决于我们激发的振动，我们可以选择不同的反应途径。我们还证明可以通过化学取代来“关闭”这种行为。

更新日期：2017-12-21

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