TY - JOUR
T1 - Nanoelectrode-emitter spectral overlap amplifies surface enhanced electrogenerated chemiluminescence
AU - Heiderscheit, Thomas S.
AU - Gallagher, Miranda J.
AU - Baiyasi, Rashad
AU - Collins, Sean S.E.
AU - Hosseini Jebeli, Seyyed Ali
AU - Scarabelli, Leonardo
AU - Al-Zubeidi, Alexander
AU - Flatebo, Charlotte
AU - Chang, Wei Shun
AU - Landes, Christy F.
AU - Link, Stephan
N1 - This work was primarily supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, CPIMS Program under Award No. DE-339SC0016534. We also acknowledge funding from the Robert A. Welch Foundation (Grant No. C-340 1787 to C.F.L., Grant No. C-1664 to S.L.). S.S.E.C. acknowledges support from the Smalley-Curl Institute at Rice University through a Carl and Lillian Illig Fellowship. C.F. acknowledges support from a National Defense Science and Engineering Graduate Fellowship. This work was conducted in part using resources of the Shared Equipment Authority at Rice University.
PY - 2019/10/14
Y1 - 2019/10/14
N2 - Electrogenerated chemiluminescence (ECL) is a promising technique for low concentration molecular detection. To improve the detection limit, plasmonic nanoparticles have been proposed as signal boosting antennas to amplify ECL. Previous ensemble studies have hinted that spectral overlap between the nanoparticle antenna and the ECL emitter may play a role in signal enhancement. Ensemble spectroscopy, however, cannot resolve heterogeneities arising from colloidal nanoparticle size and shape distributions, leading to an incomplete picture of the impact of spectral overlap. Here, we isolate the effect of nanoparticle-emitter spectral overlap for a model ECL system, coreaction of tris(2,2′-bipyridyl)dichlororuthenium(ii) hexahydrate and tripropylamine, at the single-particle level while minimizing other factors influencing ECL intensities. We found a 10-fold enhancement of ECL among 952 gold nanoparticles. This signal enhancement is attributed exclusively to spectral overlap between the nanoparticle and the emitter. Our study provides new mechanistic insight into plasmonic enhancement of ECL, creating opportunities for low concentration ECL sensing.
AB - Electrogenerated chemiluminescence (ECL) is a promising technique for low concentration molecular detection. To improve the detection limit, plasmonic nanoparticles have been proposed as signal boosting antennas to amplify ECL. Previous ensemble studies have hinted that spectral overlap between the nanoparticle antenna and the ECL emitter may play a role in signal enhancement. Ensemble spectroscopy, however, cannot resolve heterogeneities arising from colloidal nanoparticle size and shape distributions, leading to an incomplete picture of the impact of spectral overlap. Here, we isolate the effect of nanoparticle-emitter spectral overlap for a model ECL system, coreaction of tris(2,2′-bipyridyl)dichlororuthenium(ii) hexahydrate and tripropylamine, at the single-particle level while minimizing other factors influencing ECL intensities. We found a 10-fold enhancement of ECL among 952 gold nanoparticles. This signal enhancement is attributed exclusively to spectral overlap between the nanoparticle and the emitter. Our study provides new mechanistic insight into plasmonic enhancement of ECL, creating opportunities for low concentration ECL sensing.
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U2 - 10.1063/1.5118669
DO - 10.1063/1.5118669
M3 - Article
C2 - 31615232
AN - SCOPUS:85073448985
SN - 0021-9606
VL - 151
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
IS - 14
M1 - 144712
ER -