Carrier Multiplication in Transition Metal Dichalcogenides Beyond Threshold Limit

Abstract Carrier multiplication (CM), multiexciton generation by absorbing a single photon, enables disruptive improvements in photovoltaic conversion efficiency. However, energy conservation constrains the threshold energy to at least twice bandgap (2). Here, a below threshold limit CM in monolayer transition metal dichalcogenides (TMDCs) is reported. Surprisingly, CM is observed with excitation energy of only 1.75 due to lattice vibrations. Electron–phonon coupling (EPC) results in significant changes in electronic structures, which favors CM. Indeed, the strongest EPC in monolayer MoS₂ leads to the most efficient CM among the studied TMDCs. For practical applications, chalcogen vacancies can further lower the threshold by introducing defect states within bandgap. In particular, for monolayer WS₂, CM occurs with excitation energy as low as 1.51 . The results identify TMDCs as attractive candidate materials for efficient optoelectronic devices with the advantages of high photoconductivity and efficient CM.