金属－半導体周期構造によるプラズモン誘起電荷分離と光機能デバイスへの応用

本文主要研究了SiO2@TiO2核壳胶体晶体上二维有序互联的金半壳阵列。(1)不同尺寸Au半壳的光电化学性质通过将Au蒸发到不同SiO2核的SiO2@TiO2胶体晶体上，得到了不同尺寸的Au半壳阵列。本文从实验和计算两方面研究了金半壳阵列的光学性质。采用金半壳阵列的电极在300 ~ 1000 nm范围内具有较宽的吸收。结果表明，直径为374nm的中等尺寸SiO2芯的光电极具有最高的光电电流响应。根据时域有限差分模拟结果，高响应可以用电极处的高电场强度来解释。(2)金、银、铜半壳阵列光伏电池利用金属半壳阵列的二维结构开发了固态电池，它既可以吸收光又可以集流。在可见光照射下，所有电池在透明掺氟氧化锡电极和金属半壳阵列电极之间产生光电压。比较了Ag半壳电池与Au和Cu半壳电池的光伏性能。Ag半壳电池比Au和Cu半壳电池具有更高的光伏性能，实现了固态PICS器件中最高的功率转换效率（PCE）。

This study was focused on two dimensionally ordered and interconnected Au halfshell arrays on SiO2@TiO2 core-shell colloidal crystals.(1) Photoelectrochemical properties of Au Halfshells with Different SizesAu halfshell arrays with different sizes were obtained by evaporating Au onto the SiO2@TiO2 colloidal crystals with various SiO2 cores. The optical properties of the Au halfshell arrays are studied both experimentally and computationally. The electrodes with Au halfshell arrays showed broad absorption in the range examined (300-1000 nm). It was found that the photoelectrode with the middle-sized SiO2 cores of 374 nm diameter shows the highest PICS-based photocurrent responses. According to the FDTD simulated results, the high responses can be explained in terms of the high electric field intensity at the electrode.(2) Photovoltaic Cells with Gold, Silver, and Copper Halfshell ArraysSolid-state cells were developed by taking advantage of the two-dimensional structure of the metal halfshell array, which serves both as a light absorber and a current collector. Under visible light irradiation, all the cells generated photovoltage between the transparent fluorine-doped tin oxide electrode and the metal halfshell array electrode. The photovoltaic properties of Ag halfshell cells were compared with those of Au and Cu halfshell cells. The Ag halfshell cells had higher photovoltaic performance than Au and Cu halfshell cells, achieving the highest power conversion efficiency (PCE) among the solid-state PICS devices.