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Bi(Te, Se)-based compounds have attracted lots of attention for nearly two centuries as one of the most successful commercial thermoelectric (TE) materials due to their high performance at near room temperature. Compared with 3D bulks, 2D thin films are more compatible with modern semiconductor technology and have unique advantages in the construction of micro- and nano-devices. For device applications, high average TE performance over the entire operating temperature range is critical. Herein, highly c-axis-oriented N-type Bi(Te, Se) epitaxial thin films have been successfully prepared using the pulsed laser deposition technology by adjusting the deposition temperature. The film deposited at ~260 ℃ demonstrate a remarkable average power factor (PFave) of ~24.4 μW·cm−1·K−2 over the temperature range of 305–470 K, higher than most of the state-of-the-art Bi(Te, Se)-based films. Moreover, the estimated average zT value of the film is as high as ~0.81. We then constructed thin-film TE devices by using the above oriented Bi(Te, Se) films, and the maximum output power density of the device can reach up to ~30.1 W/m2 under the temperature difference of 40 K. Predictably, the outstanding average TE performance of the highly oriented Bi(Te, Se) thin films will have an excellent panorama of applications in semiconductor cooling and power generation.
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