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We describe strategies to estimate the upper limits of the efficiency ofphoton energy harvesting via hot electron extraction from gapless absorbers.Gapless materials such as noble metals can be used for harvesting the wholesolar spectrum, including visible and near-infrared light. The energy ofphoto-generated non-equilibrium or hot charge carriers can be harvested beforethey thermalize with the crystal lattice via the process of their internalphoto-emission (IPE) through the rectifying Schottky junction with asemiconductor. However, the low efficiency and the high cost of noble metalsnecessitates the search for cheaper abundant alternative materials, and we showhere that carbon can serve as a promising IPE material candidate. We comparethe upper limits of performance of IPE photon energy-harvesting platforms,which incorporate either gold or carbon as the photoactive material where hotelectrons are generated. Through a combination of density functional theory,joint electron density of states calculations, and Schottky diode efficiencymodeling, we show that the material electron band structure imposes a strictupper limit on the achievable efficiency of the IPE devices. Our calculationsreveal that graphite is a good material candidate for the IPE absorber forharvesting visible and near-infrared photons. Graphite electron density ofstates yields a sizeable population of hot electrons with energies high enoughto be collected across the potential barrier. We also discuss the mechanismsthat prevent the IPE device efficiency from reaching the upper limits imposedby their material electron band structures. The proposed approach is generaland allows for efficient pre-screening of materials for their potential use inIPE energy converters and photodetectors within application-specific spectralwindows.

Efficiency Limits of Solar Energy Harvesting via Internal Photoemission in Carbon Materials