Non-Markovian Exciton-Phonon Interactions in Core-Shell Colloidal Quantum Dots at Femtosecond Timescales

Autor(es)

Liu, A. ^[1] ; Almeida, D. B. ^[1] ; Bae, W. K. ^[2] ; Padilha, L. A. ^[3] ; Cundiff, S. T. ^[1]

Afiliação do(s) autor(es)

^[1] Univ Michigan, Phys Dept, Ann Arbor, MI 48109 - USA

^[2] Sungkyunkwan Univ, SKKU Adv Inst Nano Technol, Gyeonggi 16419 - South Korea

^[3] Univ Estadual Campinas, Inst Fis Gleb Wataghin, BR-13083970 Campinas, SP - Brazil

• Tipo de documento: Artigo Científico
• Fonte: Physical Review Letters; v. 123, n. 5 AUG 2 2019.
• Citações Web of Science: 3

Resumo

We perform two-dimensional coherent spectroscopy on CdSe/CdZnS core-shell colloidal quantum dots at cryogenic temperatures. In the two-dimensional spectra, sidebands due to electronic coupling with CdSe lattice LO-phonon modes are observed to have evolutions deviating from the exponential dephasing expected from Markovian spectral diffusion, which is instantaneous and memoryless. Comparison to simulations provides evidence that LO-phonon coupling induces energy-gap fluctuations on the finite timescales of nuclear motion. The femtosecond resolution of our technique probes exciton dynamics directly on the timescales of phonon coupling in nanocrystals. (AU)

• Processo FAPESP: 13/16911-2 - Espectroscopia avançada em novos nanomateriais
• Beneficiário: Lázaro Aurélio Padilha Junior
• Modalidade de apoio: Auxílio à Pesquisa - Jovens Pesquisadores
• Processo FAPESP: 16/50011-7 - Two-dimensional spectroscopy of novel nanomaterials
• Beneficiário: Lázaro Aurélio Padilha Junior
• Modalidade de apoio: Auxílio à Pesquisa - Regular