Localized coherent phonon generation in monolayer MoSe2 from ultrafast exciton trapping at shallow traps

We report spectroscopic evidence for the ultrafast trapping of band edge excitons at defects and the subsequent generation of defect-localized coherent phonons (CPs) in monolayer MoSe2. While the photoluminescence measurement provides signals of exciton recombination at both shallow and deep traps, our time-resolved pump-probe spectroscopy on the sub-picosecond time scale detects localized CPs only from the ultrafast exciton trapping at shallow traps. Based on occupation-constrained density functional calculations, we identify the Se vacancy and the oxygen molecule adsorbed on a Se vacancy as the atomistic origins of deep and shallow traps, respectively. Establishing the correlations between the defect-induced ultrafast exciton trapping and the generation of defect-localized CPs, our work could open up new avenues to engineer photoexcited carriers through lattice defects in two-dimensional materials.

Automated summary

We present spectroscopic evidence for the ultrafast trapping of band edge excitons at defects and the subsequent generation of defect-localized coherent phonons (CPs) in monolayer MoSe2. Our time-resolved pump-probe spectroscopy on the sub-picosecond time scale detects localized CPs only from the ultrafast exciton trapping at shallow traps. Based on density functional calculations, we identify the origins of deep and shallow traps as Se vacancy and oxygen molecule adsorbed on a Se vacancy, respectively. Our work establishes the correlations between defect-induced ultrafast exciton trapping and the generation of defect-localized CPs, providing new opportunities for engineering photoexcited carriers in two-dimensional materials through lattice defects.