Growth of Highly Conductive PtSe2 Films Controlled by Raman Metrics for High-Frequency Photodetectors and Optoelectronic Mixers at 1.55 {\mu}m

Two-dimensional PtSe2 exhibits outstanding intrinsic properties such as high carrier mobility, tunable bandgap, broadband absorption and air stability, making it ideal for (opto)electronic applications. In particular, thick PtSe2 is semimetallic and well suited for ultrafast optoelectronics in the infrared domain. However, achieving PtSe2 films of high crystalline quality with controlled properties on low-cost and insulating substrates remains challenging. Here, highly crystalline semimetallic PtSe2 films are grown by molecular beam epitaxy on sapphire substrates. It is shown how an optimized post-growth annealing remarkably improves the out-of-plane crystallinity and leads to record sheet conductances, up to 1.6 mS. In-depth structural analyses reveal the strong influence of the domain arrangement within the films on their electrical properties. Films that are mainly composed of vertically single crystalline domains exhibit high sheet conductance (1.1 - 1.6 mS), whereas films that contain superimposed twisted domains present low sheet conductance (0.5 - 0.6 mS). Moreover, it is demonstrated that the A1g Raman peak width, in addition to the commonly used Eg peak width, are both effective metrics for evaluating the quality of PtSe2: films with narrower Eg and A1g peaks exhibit higher in-plane and out-of-plane crystalline quality, respectively, as well as higher sheet conductance. Finally, coplanar waveguides integrating a semimetallic PtSe2 channel are fabricated on a 2-inch sapphire substrate to demonstrate optoelectronic devices operating at the 1.55 {\mu}m telecom wavelength. This includes photodetectors with a record 60 GHz bandwidth and the first PtSe2-based optoelectronic mixer with a bandwidth above 30 GHz.