Lee Hyunhwa, Song Kyoungjae, Lee Moonsang, Park Jeong Young
Department of Chemistry Korea Advanced Institute of Science and Technology (KAIST) Daejeon 34133 Republic of Korea.
Center for Nanomaterials and Chemical Reactions Institute for Basic Science (IBS) Daejeon 31414 Republic of Korea.
Adv Sci (Weinh). 2020 Aug 6;7(20):2001148. doi: 10.1002/advs.202001148. eCollection 2020 Oct.
Nonradiative surface plasmon decay produces highly energetic electron-hole pairs with desirable characteristics, but the measurement and harvesting of nonequilibrium hot holes remain challenging due to ultrashort lifetime and diffusion length. Here, the direct observation of LSPR-driven hot holes created in a Au nanoprism/p-GaN platform using photoconductive atomic force microscopy (pc-AFM) is demonstrated. Significant enhancement of photocurrent in the plasmonic platforms under light irradiation is revealed, providing direct evidence of plasmonic hot hole generation. Experimental and numerical analysis verify that a confined ||-field surrounding a single Au nanoprism spurs resonant coupling between localized surface plasmon resonance (LSPR) and surface charges, thus boosting hot hole generation. Furthermore, geometrical and size dependence on the extraction of LSPR-driven hot holes suggests an optimized pathway for their efficient utilization. The direct visualization of hot hole flow at the nanoscale provides significant opportunities for harnessing the underlying nature and potential of plasmonic hot holes.
非辐射表面等离子体激元衰变产生具有理想特性的高能电子 - 空穴对,但由于非平衡热空穴的超短寿命和扩散长度,对其进行测量和收集仍然具有挑战性。在此,展示了使用光电导原子力显微镜(pc - AFM)对在金纳米棱镜/p - 氮化镓平台中产生的局域表面等离子体共振(LSPR)驱动的热空穴进行直接观测。揭示了在光照射下等离子体平台中光电流的显著增强,为等离子体热空穴的产生提供了直接证据。实验和数值分析证实,单个金纳米棱镜周围受限的||场激发了局域表面等离子体共振(LSPR)与表面电荷之间的共振耦合,从而促进了热空穴的产生。此外,LSPR驱动的热空穴提取对几何形状和尺寸的依赖性为其有效利用提供了一条优化途径。纳米尺度下热空穴流动的直接可视化,为利用等离子体热空穴的潜在本质和潜力提供了重要机会。