| Abstract Scope |
Combining data-driven approaches with static and time-dependent density functional theories and nonadiabatic molecular dynamics simulations, we predict more than a dozen of high-performance photoabsorber materials from a family of known quaternary semiconductors. These compounds possess mixed tetrahedral and octahedral coordination environments with covalent and ionic bonding, respectively. Such bonding features suggest that these materials may possesses properties complementary to the known high-performance photo-absorber materials with either tetrahedral (e.g., Si, GaAs, CdTe) or octahedral (e.g., methylammonium lead iodide) coordination chemistries. The calculated optical absorption coefficient and photo-conversion efficiency for these compounds are very high and the calculated exciton binding energies are relatively small (30-32 meV). Investigations of photoexcited carrier dynamics reveal a relatively long carrier lifetime (∼ 30-40 ns), signifying suppressed nonradiative recombination. Calculations of the defect formation energies showed the absence of midgap states, making them non-detrimental to carrier recombination. |