Single-Particle Photoluminescence and Dark-Field Scattering during Charge Density Tuning

Emily K. Searles; Eric Gomez; Stephen Lee; Behnaz Ostovar; Stephan Link; Christy F. Landes

doi:10.1021/acs.jpclett.2c03566

Single-Particle Photoluminescence and Dark-Field Scattering during Charge Density Tuning

Emily K. Searles, Eric Gomez, Stephen Lee, Behnaz Ostovar, Stephan Link, Christy F. Landes

Research output: Contribution to journal › Article › peer-review

Abstract

Single-particle spectroelectrochemistry provides optical insight into understanding physical and chemical changes occurring on the nanoscale. While changes in dark-field scattering during electrochemical charging are well understood, changes to the photoluminescence of plasmonic nanoparticles under similar conditions are less studied. Here, we use correlated single-particle photoluminescence and dark-field scattering to compare their plasmon modulation at applied potentials. We find that changes in the emission of a single gold nanorod during charge density tuning of intraband photoluminescence can be attributed to changes in the Purcell factor and absorption cross section. Finally, modulation of interband photoluminescence provides an additional constructive observable, giving promise for establishing dual channel sensing in spectroelectrochemical measurements.

Original language	English (US)
Pages (from-to)	318-325
Number of pages	8
Journal	Journal of Physical Chemistry Letters
Volume	14
Issue number	2
DOIs	https://doi.org/10.1021/acs.jpclett.2c03566
State	Published - Jan 19 2023
Externally published	Yes

ASJC Scopus subject areas

General Materials Science
Physical and Theoretical Chemistry

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10.1021/acs.jpclett.2c03566

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title = "Single-Particle Photoluminescence and Dark-Field Scattering during Charge Density Tuning",

abstract = "Single-particle spectroelectrochemistry provides optical insight into understanding physical and chemical changes occurring on the nanoscale. While changes in dark-field scattering during electrochemical charging are well understood, changes to the photoluminescence of plasmonic nanoparticles under similar conditions are less studied. Here, we use correlated single-particle photoluminescence and dark-field scattering to compare their plasmon modulation at applied potentials. We find that changes in the emission of a single gold nanorod during charge density tuning of intraband photoluminescence can be attributed to changes in the Purcell factor and absorption cross section. Finally, modulation of interband photoluminescence provides an additional constructive observable, giving promise for establishing dual channel sensing in spectroelectrochemical measurements.",

author = "Searles, {Emily K.} and Eric Gomez and Stephen Lee and Behnaz Ostovar and Stephan Link and Landes, {Christy F.}",

note = "Funding Information: This work was primarily supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, CPIMS Program, under Award DE-SC0016534. Funding for this work was in part provided by the ACS Petroleum Research Fund No. 62665-ND6. The work was conducted, in part, using resources of the Shared Equipment Authority (SEA) at Rice University. C.F.L. acknowledges the Kenneth S. Pitzer-Schlumberger Chair in Chemistry. S.L. thanks the Robert A. Welch Foundation for support through the Charles W. Duncan, Jr.-Welch Chair in Chemistry (C-0002). Publisher Copyright: {\textcopyright} 2023 American Chemical Society.",

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doi = "10.1021/acs.jpclett.2c03566",

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AU - Lee, Stephen

AU - Ostovar, Behnaz

AU - Link, Stephan

AU - Landes, Christy F.

N1 - Funding Information: This work was primarily supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, CPIMS Program, under Award DE-SC0016534. Funding for this work was in part provided by the ACS Petroleum Research Fund No. 62665-ND6. The work was conducted, in part, using resources of the Shared Equipment Authority (SEA) at Rice University. C.F.L. acknowledges the Kenneth S. Pitzer-Schlumberger Chair in Chemistry. S.L. thanks the Robert A. Welch Foundation for support through the Charles W. Duncan, Jr.-Welch Chair in Chemistry (C-0002). Publisher Copyright: © 2023 American Chemical Society.

PY - 2023/1/19

Y1 - 2023/1/19

N2 - Single-particle spectroelectrochemistry provides optical insight into understanding physical and chemical changes occurring on the nanoscale. While changes in dark-field scattering during electrochemical charging are well understood, changes to the photoluminescence of plasmonic nanoparticles under similar conditions are less studied. Here, we use correlated single-particle photoluminescence and dark-field scattering to compare their plasmon modulation at applied potentials. We find that changes in the emission of a single gold nanorod during charge density tuning of intraband photoluminescence can be attributed to changes in the Purcell factor and absorption cross section. Finally, modulation of interband photoluminescence provides an additional constructive observable, giving promise for establishing dual channel sensing in spectroelectrochemical measurements.

AB - Single-particle spectroelectrochemistry provides optical insight into understanding physical and chemical changes occurring on the nanoscale. While changes in dark-field scattering during electrochemical charging are well understood, changes to the photoluminescence of plasmonic nanoparticles under similar conditions are less studied. Here, we use correlated single-particle photoluminescence and dark-field scattering to compare their plasmon modulation at applied potentials. We find that changes in the emission of a single gold nanorod during charge density tuning of intraband photoluminescence can be attributed to changes in the Purcell factor and absorption cross section. Finally, modulation of interband photoluminescence provides an additional constructive observable, giving promise for establishing dual channel sensing in spectroelectrochemical measurements.

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Single-Particle Photoluminescence and Dark-Field Scattering during Charge Density Tuning

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