The photothermoelectric effect, directly converting light energy into electrical energy, shows promising prospects in self-powered broad-band optical detection, which can extend to various applications, such as sensing, optoelectronic communications, and wide-temperature-range measurements. However, the low photosensitivity, narrow-band response, and rapid performance degeneration under continuous illumination restrict its broad application. Herein, we propose a simple bottom-up strategy to manipulate nanowires (NWs) into a well-defined multilayer Te-Ag 2 Te-Ag NW film, resulting in a high-performance photothermoelectric photodetector with a broad-band responsivity (4.1 V/W), large detectivity (944 MHz 1/2 W −1 ), and fast response speed (0.4− 0.7 s from 365 to 1200 nm). In addition, the ultrathin structure endows this device with slow and weak transverse heat conduction, enabling a stable voltage without an obvious degeneration over 1500 s. The highly anisotropic arrangement of NWs gives this device a prominent polarization sensitivity. Prospectively, this hierarchically designed nanowire film provides a promising pathway toward engineering photodetectors with high performance.

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