In view of their exciting optoelectronic light− matter interaction properties, plasmonic−hot-electron devices have attracted significant attention during the last few years as a novel route for photodetection and light-energy harvesting. Herein we report the use of quasi-3D large-area plasmonic crystals (PC) for hot-electron photodetection, with a tunable response across the visible and near-infrared. The strong interplay between the different PC modes gives access to intense electric fields and hot-carrier generation confined to the metal− semiconductor interface, maximizing injection efficiencies with responsivities up to 70 mA/W. Our approach, compatible with large-scale manufacturing, paves the way for the practical implementation of plasmonic−hot-electron optoelectronic devices. KEYWORDS: hot carriers, plasmonic crystal, photodetectors, soft nanoimprint lithography, internal photoemission T he unique light−matter interaction properties endowed by the plasmonic character of free electrons in metallic nanostructures have motivated vivid research that during the last few decades found applications in a variety of fields such as biology, 1 chemistry, 2 medicine, 3 information theory, and quantum optics 4−6 or energy harvesting and photodetection.
7−9These plasmonic resonances give rise to photocurrent generation by decaying into highly energetic electrons, socalled "hot electrons", which are then emitted from the metal before thermalization and collected at the electrodes on the basis of the principle of internal photoemission. 10,11 The field of hot-electron plasmonics has rapidly developed during the last years, 11−33 led by the interest in active optoelectronic devices with functionalities that emanate from their plasmonic character, such as a tailored spectral response, which are especially appealing for solar-energy harvesting, 11−19 and subband-gap visible or infrared detection.20−27 The increase in hot-electron-based devices has also been fostered by the advances in associated nanofabrication technologies. Electron or ion-beam lithographies are currently used to fabricate prototypes that exploit the spectral tunability of plasmonic architectures. These devices have relied on nanoparticles, 11,22 nanoantennas, 12,20,26 or gratings 24 to excite individually either localized plasmons or surface plasmon polaritons, whose relaxation eventually leads to the creation of hot carriers. This nanostructuring, required to address the spectral tunability in these devices, has hitherto relied on low-throughput, costly, and time-consuming lithographic processes. This may seriously limit the future potential of plasmonic−hot-electron optoelectronics because large-area and high-throughput manufacturing are requisites for energy-harvesting and large-area optoelectronic applications. 34 Here we report the implementation of plasmonic crystals (PC) as a novel platform for hot-electron generation. 35,36 PCs, similar to their dielectric counterparts (photonic crystals), are periodically organized metallic architectur...