Department of Chemistry, Kyoto University, Kyoto, 606-8502, Japan.
Nano Lett. 2011 Apr 13;11(4):1845-50. doi: 10.1021/nl200651p. Epub 2011 Mar 31.
We developed time-domain ab initio simulation of Auger phenomena, including multiple exciton generation (MEG) and recombination (MER). It is the first approach describing phonon-assisted processes and early dynamics. MEG starts below the electronic threshold, strongly accelerating with energy. Ligands are particularly important to phonon-assisted MEG, which therefore can be probed with infrared spectroscopy. Short-time gaussian component gives 5-10% of MEG, justifying rate theories that assume exponential dynamics. MER is preceded by electron-phonon relaxation to low energies.
我们开发了包括多激子产生（MEG）和复合（MER）在内的俄歇现象的时域从头算模拟。这是第一个描述声子辅助过程和早期动力学的方法。MEG 在电子阈值以下开始，随着能量的增加而强烈加速。配体对声子辅助 MEG 特别重要，因此可以用红外光谱进行探测。短时高斯分量给出了 5-10%的 MEG，这证明了假设指数动力学的速率理论是正确的。MER 之前是电子-声子弛豫到低能态。
