Ultrafast charge transfer coupled to quantum proton motion at molecule/metal oxide interface
Ultrafast charge transfer coupled to quantum proton motion at molecule/metal oxide interface
复制标题
分子/金属氧化物界面处与量子质子运动耦合的超快电荷转移
DOI：
10.1126/sciadv.abo2675
复制
发表时间：
2022-06-17
期刊：
影响因子：
13.6
通讯作者：
Zhao, Jin
中科院分区：
文献类型：
--
作者：
Chu, Weibin;Tan, Shijing;Zhao, Jin
理解氢键(H键)网络中的核量子效应(NQE)如何影响半导体/分子界面的光激电荷转移是一个具有挑战性的问题。通过在从头算水平上结合两种新兴的分子动力学方法，即基于路径积分的分子动力学和含时非绝热分子动力学，并选择CH3OH/Ti02作为原型系统进行研究，我们发现氢键网络中的量子质子运动与界面上的超快光激发电荷动力学是强耦合的。吸附的甲醇分子的空穴捕获能力被NQE显著增强，因此，它对二氧化钛具有空穴清除剂的作用。紫外光照射下的原位扫描隧道显微镜测量证实了氢键网络的关键作用。得出结论：氢键网络中的量子质子运动对基于光激发的能量转换效率起着至关重要的作用。
Understanding how the nuclear quantum effects (NQEs) in the hydrogen bond (H-bond) network influence the photoexcited charge transfer at semiconductor/molecule interface is a challenging problem. By combining two kinds of emerging molecular dynamics methods at the ab initio level, the path integral-based molecular dynamics and time-dependent nonadiabatic molecular dynamics, and choosing CH3OH/TiO2 as a prototypical system to study, we find that the quantum proton motion in the H-bond network is strongly coupled with the ultrafast photoexcited charge dynamics at the interface. The hole trapping ability of the adsorbed methanol molecule is notably enhanced by the NQEs, and thus, it behaves as a hole scavenger on titanium dioxide. The critical role of the H-bond network is confirmed by in situ scanning tunneling microscope measurements with ultraviolet light illumination. It is concluded the quantum proton motion in the H-bond network plays a critical role in influencing the energy conversion efficiency based on photoexcitation.