Control of Phonons in Semiconductor Nanocrystals via Femtosecond Pulse Chirp-Influenced Wavepacket Dynamics and Polarization

Autor: Brenna R. Walsh, Jonathan I. Saari, Patanjali Kambhampati, Anne Myers Kelley, Jonathan Mooney, Michael M. Krause
Rok vydání: 2013
Předmět:
Zdroj: The Journal of Physical Chemistry B. 117:15651-15658
ISSN: 1520-5207
1520-6106
DOI: 10.1021/jp406323f
Popis: The realistic electronic structure of semiconductor nanocrystals is characterized by excitonic fine structure and atomistic symmetry breakings that are challenging to resolve experimentally. Exciton-phonon coupling is one of the most sensitive measures of the excitonic wave functions of the nanocrystals. Here, we exploit this sensitivity via chirped pulse and polarization resolved femtosecond pump/probe spectroscopy of colloidal CdSe nanocrystals. Pulse chirp measurements and simulations are used to explore the contributions of excited- and ground-state vibrational wavepackets to the observed coherent phonons in the pump/probe signals. Polarization resolved pump/probe spectroscopy is used to explore electronic and vibrational polarization anisotropies. We find no electronic polarization anisotropy, whereas vibrational anisotropy is preserved.
Databáze: OpenAIRE