Multiple Exciton Generation in Semiconductor Quantum Dots.

Multiple exciton generation in quantum dots (QDs) has been intensively studied as a way to enhance solar energy conversion by utilizing the excess energy in the absorbed photons. Among other useful properties, quantum confinement can both increase Coulomb interactions that drive the MEG process and decrease the electron-phonon coupling that cools hot excitons in bulk semiconductors. However, variations in the reported enhanced quantum yields (QYs) have led to disagreements over the role that quantum confinement plays. The enhanced yield of excitons per absorbed photon is deduced from a dynamical signature in the transient absorption or transient photoluminescence and is ascribed to the creation of biexcitons. Extraneous effects such as photocharging are partially responsible for the observed variations. When these extraneous effects are reduced, the MEG efficiency, defined in terms of the number of additional electron-hole pairs produced per additional band gap of photon excitation, is about two times better in PbSe QDs than that in bulk PbSe. Thin films of electronically coupled QDs have shown promise in simple photon-to-electron conversion architectures. If the MEG efficiency can be further enhanced and charge separation and transport can be optimized within QD films, then QD solar cells can lead to third-generation solar energy conversion technologies.