Relations between absorption, emission, and excited state chemical potentials from nanocrystal 2D spectra
Ryu, Jisu ; Park, Samuel D. ; Baranov, Dmitry LU
; Rreza, Iva
; Owen, Jonathan S.
and Jonas, David M.
(2021)
In Science Advances
7(22).
- Abstract
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... (More)
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.
(Less)
- author
- Ryu, Jisu
; Park, Samuel D.
; Baranov, Dmitry
LU
; Rreza, Iva
; Owen, Jonathan S.
and Jonas, David M.
- publishing date
- 2021-05
- type
- Contribution to journal
- publication status
- published
- in
- Science Advances
- volume
- 7
- issue
- 22
- article number
- eabf4741
- pages
- 14 pages
- publisher
- American Association for the Advancement of Science (AAAS)
- external identifiers
-
- pmid:34049871
- scopus:85106973422
- ISSN
- 2375-2548
- DOI
- 10.1126/sciadv.abf4741
- language
- English
- LU publication?
- no
- additional info
- Publisher Copyright: Copyright © 2021 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).
- id
- 7e2bf6d3-b956-4193-9038-d0c382157bf9
- date added to LUP
- 2023-01-17 11:54:14
- date last changed
- 2024-07-11 15:58:01
@article{7e2bf6d3-b956-4193-9038-d0c382157bf9,
abstract = {{<p>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.</p>}},
author = {{Ryu, Jisu and Park, Samuel D. and Baranov, Dmitry and Rreza, Iva and Owen, Jonathan S. and Jonas, David M.}},
issn = {{2375-2548}},
language = {{eng}},
number = {{22}},
publisher = {{American Association for the Advancement of Science (AAAS)}},
series = {{Science Advances}},
title = {{Relations between absorption, emission, and excited state chemical potentials from nanocrystal 2D spectra}},
url = {{http://dx.doi.org/10.1126/sciadv.abf4741}},
doi = {{10.1126/sciadv.abf4741}},
volume = {{7}},
year = {{2021}},
}