4.5 Article

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

Journal

JOURNAL OF PHYSICAL CHEMISTRY B
Volume 117, Issue 49, Pages 15651-15658

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/jp406323f

Keywords

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Funding

  1. CFI
  2. NSERC
  3. FQRNT
  4. McGill University
  5. NSF [CHE-1112192]
  6. Division Of Chemistry
  7. Direct For Mathematical & Physical Scien [1112192] Funding Source: National Science Foundation

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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.

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