skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Reversible Modulation of the Electrostatic Potential of a Colloidal Quantum Dot through the Protonation Equilibrium of Its Ligands

Abstract

This Letter describes the reversible modulation of the electrostatic potential at the interface between a colloidal PbS quantum dot (QD) and solvent, through the protonation equilibrium of the QD’s histamine-derivatized dihydrolipoic acid (DHLA) ligand shell. The electrostatic potential is sensitively monitored by the yield of photoinduced electron transfer from the QD to a charged electron acceptor, 9,10-anthraquinone-2-sulfonate (AQ). The permeability of the DHLA coating to the AQ progressively increases as the average degree of protonation of the ligand shell increases from 0 to 92%, as quantified by 1H NMR, upon successive additions of p-toluenesulfonic acid; this increase results in a decrease in the photoluminescence (PL) intensity of the QDs by a factor of 6.7. The increase in permeability is attributable to favorable electrostatic interactions between the ligands and AQ. This work suggests the potential of the combination of near-IR-emitting QDs and molecular quenchers as robust local H+ sensors.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1];  [1]; ORCiD logo [1]
  1. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Bio-Inspired Energy Science (CBES)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1470005
Grant/Contract Number:  
SC0000989
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 8; Journal Issue: 20; Related Information: CBES partners with Northwestern University (lead); Harvard University; New York University; Pennsylvania State University; University of Michigan; University of Pittsburgh; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalysis (homogeneous); solar (photovoltaic); bio-inspired; charge transport; mesostructured materials; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly)

Citation Formats

He, Chen, Zhang, Zhengyi, Wang, Chen, Jiang, Yishu, and Weiss, Emily A. Reversible Modulation of the Electrostatic Potential of a Colloidal Quantum Dot through the Protonation Equilibrium of Its Ligands. United States: N. p., 2017. Web. doi:10.1021/acs.jpclett.7b02101.
He, Chen, Zhang, Zhengyi, Wang, Chen, Jiang, Yishu, & Weiss, Emily A. Reversible Modulation of the Electrostatic Potential of a Colloidal Quantum Dot through the Protonation Equilibrium of Its Ligands. United States. doi:10.1021/acs.jpclett.7b02101.
He, Chen, Zhang, Zhengyi, Wang, Chen, Jiang, Yishu, and Weiss, Emily A. Tue . "Reversible Modulation of the Electrostatic Potential of a Colloidal Quantum Dot through the Protonation Equilibrium of Its Ligands". United States. doi:10.1021/acs.jpclett.7b02101. https://www.osti.gov/servlets/purl/1470005.
@article{osti_1470005,
title = {Reversible Modulation of the Electrostatic Potential of a Colloidal Quantum Dot through the Protonation Equilibrium of Its Ligands},
author = {He, Chen and Zhang, Zhengyi and Wang, Chen and Jiang, Yishu and Weiss, Emily A.},
abstractNote = {This Letter describes the reversible modulation of the electrostatic potential at the interface between a colloidal PbS quantum dot (QD) and solvent, through the protonation equilibrium of the QD’s histamine-derivatized dihydrolipoic acid (DHLA) ligand shell. The electrostatic potential is sensitively monitored by the yield of photoinduced electron transfer from the QD to a charged electron acceptor, 9,10-anthraquinone-2-sulfonate (AQ). The permeability of the DHLA coating to the AQ progressively increases as the average degree of protonation of the ligand shell increases from 0 to 92%, as quantified by 1H NMR, upon successive additions of p-toluenesulfonic acid; this increase results in a decrease in the photoluminescence (PL) intensity of the QDs by a factor of 6.7. The increase in permeability is attributable to favorable electrostatic interactions between the ligands and AQ. This work suggests the potential of the combination of near-IR-emitting QDs and molecular quenchers as robust local H+ sensors.},
doi = {10.1021/acs.jpclett.7b02101},
journal = {Journal of Physical Chemistry Letters},
number = 20,
volume = 8,
place = {United States},
year = {2017},
month = {9}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 3 works
Citation information provided by
Web of Science

Save / Share: