Investigation of ligand effects on exciton recombination in PbS nanoparticles
Multiple exciton generation (MEG) and exciton recombination were studied by femtosecond transient absorption spectroscopy in PbS nanoparticles (NPs) capped with oleic acid (PbS–OLA) and 2,3-dimercaptopropane sulfonate (PbS–DMPS) ligands. Analysis of the transient absorption data showed that the PbS–DMPS nanoparticles exhibit increased rates of multi- and single-exciton recombination compared with the PbS–OLA nanoparticles; however, the MEG yield for both sets of particles was the same within experimental error. The origin of the differences in the exciton recombination decay rates is unknown, but it is speculated that it may be due to the ionic functionality of DMPS or to the different ligating atoms of the OLA and DMPS ligands. The PbS–DMPS nanoparticles were highly sensitive to the presence of oxygen, which caused a dramatic increase in nonradiative decay pathways, which can be mistaken for multiexciton absorbance and decay. Removal of oxygen eliminated the nonradiative decay pathways. Overall, this study showed that the dynamics of MEG can be modified by changing the NP ligand shell, a result that may be useful in the development of NP-based thin-film solar devices.