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Updated: Mar 14, 2026
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Electrostatic Control of Excitonic Energies and Dynamics in a CdS Quantum Dot through Reversible Protonation of Its
Christopher M Thompson1, Mohamad Kodaimati1, Dana Westmoreland1
1Department of Chemistry, Northwestern University , 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States.
Abstract:
This paper describes the pH dependence of the excitonic energies and dynamics of CdS quantum dots (QDs) capped with phosphonopropionate (PPA) in water. QDs capped with PPA carry a negative charge on their surfaces upon deprotonation of PPA above pH ∼ 8.5; the resultant electric field induces large changes in the QD's optical properties. Between pH 5.6 and 12.0, an increase in pH is accompanied by a 47-meV bathochromic shift in the bandgap of the QDs and a decrease in the Stokes shift by ∼4.3 meV/pH unit. An increase in the radiative recombination rate by a factor of 20.9 occurs on increasing the pH from 5.6 to 9.4. These observations are attributed to a shifting of the energy levels within the first exciton manifold, and are simulated using time-dependent density functional theory calculations on model Cd29S29 clusters surrounded by point charges.
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