Fundamental Efficiency Limits of Transition-Metal Dichalcogenide Solar Cells with Carrier Multiplication and Hot-Carrier Effects.
basic_science · Level V
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- Record sourced from PubMed, PMID 42208055.
- Also identified by DOI 10.1021/acs.nanolett.6c02055.
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Abstract
Detailed-balance limits for transition-metal dichalcogenide (TMD) solar cells have been reported, but a unified treatment of thickness-dependent optics, carrier multiplication (CM), hot-carrier (HC) extraction, and finite cooling leakage has been lacking. Here, we develop a generalized detailed-balance upper-bound framework that combines energy- and thickness-dependent absorptance, exciton-resolved monolayer absorbance, an experimental CM-yield limit (η<sub>CM</sub> ≤ 0.97), and an endoreversible HC engine with a finite cooling coefficient κ. For optically thick absorbers under AM1.5G, the Shockley-Queisser optimum near <i>E</i><sub><i>g</i></sub> ≃ 1.3 eV shifts toward ∼1.0 eV, with reversible efficiencies above 50%. CM does not raise the reversible HC limit; at finite κ, it only redistributes part of the same excess photon energy into collected current. Monolayer TMDs show negligible CM benefit, whereas bulk-like TMDs can exhibit large HC gains only when electron-phonon cooling is strongly suppressed. These results identify narrow-bandgap, optically strong TMDs as the more plausible beyond-SQ route.