电子隧道电流对化学反应的非平衡催化作用
Out-of-equilibrium catalysis of chemical reactions by electronic tunnel currents
摘要：
我们提出了电流诱导化学反应的逃逸率理论。我们使用Keldysh非平衡格林函数导出反应坐标的Langevin方程。由于平衡态电子自由度的存在，朗之万方程中的摩擦、噪声和有效温度局部依赖于反应坐标。作为一个例子，我们考虑的解离双原子分子诱导的电子电流从扫描隧道显微镜针尖。在共振隧穿机制中，分子解离涉及两个相互关联的过程：势能势垒的改变和分子的加热。伴随着有效的、反应坐标依赖的温度的出现的分子势垒的降低（即电流诱导的势垒的催化还原）是电流诱导的化学反应的另一种机制，其明显不同于通常的泵浦振动自由度的范例。
英文摘要：
We present an escape rate theory for current-induced chemical reactions. We use Keldysh nonequilibrium Green's functions to derive a Langevin equation for the reaction coordinate. Due to the out of equilibrium electronic degrees of freedom, the friction, noise, and effective temperature in the Langevin equation depend locally on the reaction coordinate. As an example, we consider the dissociation of diatomic molecules induced by the electronic current from a scanning tunnelling microscope tip. In the resonant tunnelling regime, the molecular dissociation involves two processes which are intricately interconnected: a modification of the potential energy barrier and heating of the molecule. The decrease of the molecular barrier (i.e. the current induced catalytic reduction of the barrier) accompanied by the appearance of the effective, reaction-coordinate-dependent temperature is an alternative mechanism for current-induced chemical reactions, which is distinctly different from the usual paradigm of pumping vibrational degrees of freedom.
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