Zhang Chongjian, Fan Yunyan, Huang Xiaochun, Zhang Kelvin H L, Beard Matthew C, Yang Ye
State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
Chemistry and Nanoscience Center, National Renewable Energy Laboratory, Golden, Colorado 80401, USA.
J Chem Phys. 2020 Apr 14;152(14):144705. doi: 10.1063/5.0005881.
Interfacial charge transfer from silicon to heterogeneous catalysts plays a key role in silicon-based photoelectrochemical systems. In general, prior to interfacial charge transfer, carriers that are generated by photons with energies above the bandgap dissipate the excess kinetic energy via hot-carrier cooling, and such energy loss limits the maximum power conversion efficiency. The excess energy of hot-carriers, however, could be utilized through hot-carrier transfer from silicon to the catalysts, but such hot-carrier extraction has not yet been demonstrated. Here, we exploit transient reflection spectroscopy to interrogate charge transfer at the interface between silicon and platinum. Quantitative modeling of the surface carrier kinetics indicates that the velocity of charge transfer from silicon to platinum exceeds 2.6 × 10 cm s, corresponding to an average carrier temperature of extracted carriers of ∼600 K, two times higher than the lattice temperature. The charge transfer velocity can be controllably reduced by inserting silica spacing layers between silicon and platinum.
从硅到异质催化剂的界面电荷转移在硅基光电化学系统中起着关键作用。一般来说,在界面电荷转移之前,由能量高于带隙的光子产生的载流子通过热载流子冷却耗散多余的动能,这种能量损失限制了最大功率转换效率。然而,热载流子的多余能量可以通过从硅到催化剂的热载流子转移来利用,但这种热载流子提取尚未得到证实。在这里,我们利用瞬态反射光谱来研究硅和铂之间界面处的电荷转移。表面载流子动力学的定量模型表明,从硅到铂的电荷转移速度超过2.6×10厘米/秒,对应于提取载流子的平均载流子温度约为600 K,比晶格温度高两倍。通过在硅和铂之间插入二氧化硅间隔层,可以可控地降低电荷转移速度。