Ionic Liquid Gating Enhanced Photothermoelectric Conversion in Three-Dimensional Microporous Graphene

The photothermoelectric (PTE) effect can effectively convert light into electricity through photothermal and thermoelectric processes and has great potential applications in light energy harvesting and bandgap-independent photodetection. It is particularly applicable for the terahertz (THz) range featuring low photon energy but has not been well established due to lack of high-performance PTE materials in this range. Three-dimensional microporous graphene (3DMG) foam possesses ultrahigh THz absorptivity and outstanding photothermal conversion and can serve as a promising candidate. Here, enhancement of the THz PTE response of 3DMG foam by fine-tuning its thermoelectric properties using the ionic liquid electric double layer (EDL) technique was demonstrated. Continuous and reversible control of the Seebeck coefficient of 3DMG highlights the effectiveness of EDL gating in manipulating the electronic structures of such bulk and porous material. An approximate 1 order of magnitude enhancement in the Seebeck coefficient as well as the PTE responsivity was observed. In addition, a double-cell 3DMG EDL device with a p–n junction like channel configuration enabled further improvement of the photoresponse. This work opens a new avenue to optimize the PTE performance of 2D nanosheet-assembled 3D porous materials for highly efficient energy harvesting and detection of THz radiation.