Quantum Zeno Effect Rationalizes the Phonon Bottleneck in Semiconductor Quantum Dots

Svetlana V. Kilina, Amanda J. Neukirch, Bradley F. Habenicht, Dmitri S. Kilin, and Oleg V. Prezhdo

Phys. Rev. Lett. 110, 180404 – Published 2 May 2013

Abstract

Quantum confinement can dramatically slow down electron-phonon relaxation in nanoclusters. Known as the phonon bottleneck, the effect remains elusive. Using a state-of-the-art time-domain ab initio approach, we model the observed bottleneck in CdSe quantum dots and show that it occurs under quantum Zeno conditions. Decoherence in the electronic subsystem, induced by elastic electron-phonon scattering, should be significantly faster than inelastic scattering. Achieved with multiphonon relaxation, the phonon bottleneck is broken by Auger processes and structural defects, rationalizing experimental difficulties.

Received 8 December 2012

DOI:https://doi.org/10.1103/PhysRevLett.110.180404

Authors & Affiliations

Svetlana V. Kilina¹, Amanda J. Neukirch², Bradley F. Habenicht³, Dmitri S. Kilin⁴, and Oleg V. Prezhdo⁵

¹Department of Chemistry and Biochemistry, North Dakota State University, Fargo, North Dakota 58108, USA
²Department of Physics and Astronomy, University of Rochester, Rochester, New York 14627, USA
³Center for Nanophase Materials Science, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, USA
⁴Department of Chemistry, University of South Dakota, Vermillion, South Dakota 57069, USA
⁵Department of Chemistry, University of Rochester, Rochester, New York 14627, USA