Phonon-Mediated Ultrafast Hole Transfer from Photoexcited CdSe Quantum Dots to Black Dye

Cui, Peng; Jabed, Mohammed; Vogel, Dayton Jon; Kilina, Svetlana

doi:10.1021/bk-2019-1331.ch006

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Title: Phonon-Mediated Ultrafast Hole Transfer from Photoexcited CdSe Quantum Dots to Black Dye

Journal Article · 10 December 2019 · ACS Symposium Series

DOI: https://doi.org/10.1021/bk-2019-1331.ch006 · OSTI ID:1573807

Cui, Peng ^[1]; Jabed, Mohammed ^[2]; Vogel, Dayton Jon ^[2];

^[2]

North Dakota State Univ., Fargo, ND (United States); North Dakota State University
North Dakota State Univ., Fargo, ND (United States)

We have applied non-adiabatic molecular dynamics (NAMD) and Fewest Switching surface hopping (FSSH) method to simulate the energy dissipation and charge transfer processes in the CdSe quantum dot (QD) functionalized by the Black dye. Our calculations reveal ultrafast hole transfer from the photoexcited QD to the dye, despite a significant energy splitting between QD’s and dye’s occupied states. The mechanism of such ultrafast QD-to-dye hole transfer is rationalized by strong non-adiabatic couplings between the delocalized surface orbitals of the QD and the high-frequency vibrations of isothiocyanate ligands of the Black dye. Here, this mechanism is also confirmed by a very rapid lose of coherency of the excitation due to strong electronic couplings with vibrational modes of the dye.

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Research Organization:: North Dakota State University, Fargo, ND (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: SC0008446

OSTI ID:: 1573807

Journal Information:: ACS Symposium Series, Journal Name: ACS Symposium Series Vol. 1331; ISSN 0097-6156

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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