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Fulfilling the potential of the colloidal semiconductor quantum dots (QDs) inelectrically driven applications remains a challenge largely since operation ofsuch devices involves charged QDs with drastically different photo-physicalproperties compared to their well-studied neutral counterparts. In this work,the full picture of excited state dynamics in charged CdSe QDs at varioustime-scales has been revealed via transient absorption spectroscopy combinedwith electrochemistry as direct manipulation tool to control the negativecharging of CdSe QDs. In trions, excited states of single charged QDs, theadditional electron in the conduction band speeds up the hot electron coolingby enhanced electron-electron scattering followed by charge redistribution andpolaron formation in picoseconds timescale. The trions are finally decayed byAuger process in 500 ps timescale. Double charging in QDs, on the other hand,decelerates the polaron formation process while accelerates the following Augerdecay. Our work demonstrates the potential of photo-electrochemistry as aplatform for ultrafast spectroscopy of charged species and paves a way forfurther studies to develop comprehensive knowledge of the photophysicalprocesses in charged QDs more than the well-known Auger decay preparing theiruse in future optoelectronic applications.

Photo-Excitation Dynamics in Electrochemically Charged CdSe Quantum Dots: from Hot Carrier Cooling to Auger Recombination of Negative Trions