过渡金属配合物系间交叉的超快级联理论
Ultrafast Cascading Theory in Intersystem Crossings in Transition-Metal Complexes
摘要：
我们研究了过渡金属配合物中自旋轨道耦合介导的超快系间跃迁的级联衰变机制。光激发后发生的级联过程的量子力学描述。给出了超快级联的条件，并将级联过程中能级间的能量差与电子-声子自能联系起来。这些限制有助于确定级联路径。对于$Fe^{2+}$自旋交叉复合物，这导致的结论是，超快衰减主要发生在反键金属-配体电荷转移态的歧管。我们还解释了为什么一些中间状态被绕过。
英文摘要：
We investigate the cascade decay mechanism for ultrafast intersystem crossing mediated by the spin-orbit coupling in transition-metal complexes. A quantum-mechanical description of the cascading process that occurs after photoexcitation is presented. The conditions for ultrafast cascading are given, which relate the energy difference between the levels in the cascading process to the electron-phonon self energy. These limitations aid in the determination of the cascade path. For $Fe^{2+}$ spin-crossover complexes, this leads to the conclusion that the ultrafast decay primarily occurs in the manifold of antibonding metal-to-ligand charge-transfer states. We also give an interpretation why some intermediate states are bypassed.
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