n-Doping of Quantum Dots by Lithium Ion Intercalation.

The optical properties of colloidal quantum dots (QDs) are sensitive to introduction of excess electrons or holes into their delocalized bands. Crucial to robust and energy-efficient electronic doping of QDs is suitable charge compensation. Compensation by surface modification and substitutional impurities are however not sufficiently controllable to enable effective doping of QDs. This manuscript describes electrochemical n-type doping of CdSe QDs where injected electrons are compensated by interstitial Li+ to form LixCdSe, x ≤ 0.3. n-type degenerate doping reversibly decreases absorption into the lowest-energy excitonic state of the QD, activates intraband optical transitions, and shifts the photoluminescence of the QD to higher energy. This work establishes electrochemical interstitial doping as a reversible and highly controllable method for tuning the optical properties of colloidal QDs.