Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 151, Issue 14, Pages -Publisher
AMER INST PHYSICS
DOI: 10.1063/1.5118669
Keywords
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Funding
- U.S. Department of Energy, Office of Science, Basic Energy Sciences, CPIMS Program [DE-339SC0016534]
- Robert A. Welch Foundation [C-340 1787, C-1664]
- Smalley-Curl Institute at Rice University through a Carl and Lillian Illig Fellowship
- National Defense Science and Engineering Graduate Fellowship
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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. Published under license by AIP Publishing.
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