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Title: Relations between absorption, emission, and excited state chemical potentials from nanocrystal 2D spectra
For quantum-confined nanomaterials, size dispersion causes a static broadening of spectra that has been difficult to measure and invalidates all-optical methods for determining the maximum photovoltage that an excited state can generate. Using femtosecond two-dimensional (2D) spectroscopy to separate size dispersion broadening of absorption and emission spectra allows a test of single-molecule generalized Einstein relations between such spectra for colloidal PbS quantum dots. We show that 2D spectra and these relations determine the thermodynamic standard chemical potential difference between the lowest excited and ground electronic states, which gives the maximum photovoltage. Further, we find that the static line broadening from many slightly different quantum dot structures allows single-molecule generalized Einstein relations to determine the average single-molecule linewidth from Stokes’ frequency shift between ensemble absorption and emission spectra.  more » « less
Award ID(s):
1800523
NSF-PAR ID:
10292106
Author(s) / Creator(s):
; ; ; ; ;
Date Published:
Journal Name:
Science Advances
Volume:
7
Issue:
22
ISSN:
2375-2548
Page Range / eLocation ID:
eabf4741
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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