Annealing Temperature-Dependent Terahertz Thermal–Electrical Conversion Characteristics of Three-Dimensional Microporous Graphene

Three-dimensional microporous graphene (3DMG) possesses ultrahigh photon absorptivity and excellent photothermal conversion ability and shows great potential in energy storage and photodetection, especially for the not well-explored terahertz (THz) frequency range. Here, we report on the characterization of the THz thermal-electrical conversion properties of 3DMG with different annealing treatments. We observe distinct behavior of bolometric and photothermoelectric responses varying with annealing temperature. Resistance-temperature characteristics and thermoelectric power measurements reveal that marked charge carrier reversal occurs in 3DMG as the annealing temperature changes between 600 and 800 °C, which can be well explained by Fermi-level tuning associated with oxygen functional group evolution. Benefiting from the large specific surface area of 3DMG, it has an extraordinary capability of reaching thermal equilibrium quickly and exhibits a fast photothermal conversion with a time constant of 23 ms. In addition, 3DMG can serve as an ideal absorber to improve the sensitivity of THz detectors and we demonstrate that the responsivity of a carbon nanotube device could be enhanced by 12 times through 3DMG. Our work provides new insight into the physical characteristics of carrier transport and THz thermal-electrical conversion in 3DMG controlled by annealing temperature and opens an avenue for the development of highly efficient graphene-based THz devices.