Xu Kang, Pagliero Daniela, López-Morales Gabriel I, Flick Johannes, Wolcott Abraham, Meriles Carlos A
Department of Physics, CUNY-City College of New York, New York, New York 10031, United States.
CUNY-The Graduate Center, New York, New York 10016, United States.
ACS Appl Mater Interfaces. 2024 Jul 17;16(28):37226-37233. doi: 10.1021/acsami.4c06298. Epub 2024 Jul 8.
Thanks to its low or negative surface electron affinity and chemical inertness, diamond is attracting broad attention as a source material of solvated electrons produced by optical excitation of the solid-liquid interface. Unfortunately, its wide bandgap typically imposes the use of wavelengths in the ultraviolet range, hence complicating practical applications. Here, we probe the photocurrent response of water surrounded by single-crystal diamond surfaces engineered to host shallow nitrogen-vacancy (NV) centers. We observe clear signatures of diamond-induced photocurrent generation throughout the visible range and for wavelengths reaching up to 594 nm. Experiments as a function of laser power suggest that NV centers and other coexisting defects─likely in the form of surface traps─contribute to carrier injection, though we find that NVs dominate the system response in the limit of high illumination intensities. Given our growing understanding of near-surface NV centers and adjacent point defects, these results open new perspectives in the application of diamond-liquid interfaces to photocarrier-initiated chemical and spin processes in fluids.
由于其低或负的表面电子亲和力以及化学惰性,金刚石作为通过固液界面光激发产生溶剂化电子的源材料正受到广泛关注。不幸的是,其宽带隙通常要求使用紫外波段的波长,这使得实际应用变得复杂。在此,我们探测了由设计用于容纳浅氮空位(NV)中心的单晶金刚石表面所包围的水的光电流响应。我们在整个可见光范围内以及波长高达594 nm时都观察到了金刚石诱导光电流产生的明显特征。作为激光功率函数的实验表明,NV中心和其他共存缺陷(可能以表面陷阱的形式)有助于载流子注入,不过我们发现在高光照强度极限下NV主导了系统响应。鉴于我们对近表面NV中心和相邻点缺陷的认识不断加深,这些结果为金刚石 - 液体界面在流体中光载流子引发的化学和自旋过程中的应用开辟了新的前景。