CdSe quantum dots have tuneable electronic properties and are sensitive to diffused light, making them appealing candidates for light harvesting. They also offer the enticing possibility of harvesting hot electrons, but in reality, their performance is often limited because excess energy above the band gap is dissipated faster than charge separation. This process is known as hot carrier cooling. We investigate hot carrier cooling by application of electronic structure calculations to a series of model ammonia-passivated CdSe nanoparticles. We demonstrate that this process is mediated by a cascade of conical intersections between electronic excited states. Analysis of these intersections indicates that energy is deposited into a complex combination of modes involving the surface atoms and ligands.

Hot carrier cooling in quantum dots via a cascade of conical intersections

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ACS Fall 2022

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.