Plasmon-Enhanced Single-Molecule Enzymology

ACS Photonics
Yuyang Wang, Peter Zijlstra

Abstract

We present a numerical study on plasmon-enhanced single-molecule enzymology. We combine Brownian dynamics and electromagnetic simulations to calculate the enhancement of fluorescence signals of fluorogenic substrate converted by an enzyme conjugated to a plasmonic particle. We simulate the Brownian motion of a fluorescent product away from the active site of the enzyme, and calculate the photon detection rate taking into account modifications of the excitation and emission processes by coupling to the plasmon. We show that plasmon enhancement can boost the signal-to-noise ratio (SNR) of single turnovers by up to 100 fold compared to confocal microscopy. This enhancement factor is a trade-off between the reduced residence time in the near-field of the particle, and the enhanced emission intensity due to coupling to the plasmon. The enhancement depends on the size, shape and material of the particle and the photophysical properties of the fluorescent product. Our study provides guidelines on how to enhance the SNR of single-molecule enzyme studies and may aid in further understanding and quantifying static and dynamic heterogeneity.

References

Dec 4, 1998·Science·H P LuX S Xie
Aug 5, 1997·Chemical Reviews·Andrew D. Robertson, Kenneth P. Murphy
Feb 28, 2002·Physical Review Letters·C SönnichsenP Mulvaney
Nov 13, 2003·Journal of the American Chemical Society·K K CaswellCatherine J Murphy
Dec 25, 2004·Angewandte Chemie·Kelly VeloniaFrans C de Schryver
Feb 8, 2005·Proceedings of the National Academy of Sciences of the United States of America·Ophir FlomenbomJoseph Klafter
Feb 22, 2005·Nature Biotechnology·Yannick RondelezHiroyuki Noji
Mar 15, 2005·Biophysical Journal·Alan I Lee, James P Brody
Jan 18, 2006·Nature Chemical Biology·Brian P EnglishX Sunney Xie
Jan 30, 2007·Nano Letters·Felicia TamNaomi J Halas
Nov 23, 2007·Journal of the American Chemical Society·Gert De CremerDirk E De Vos
Feb 21, 2009·Biotechnology Journal·Kerstin BlankJohan Hofkens
Aug 20, 2009·Chemical Society Reviews·Qi ChenG Julius Vancso
Dec 3, 2011·ACS Nano·Tatyana G TerentyevaKerstin Blank
Mar 13, 2012·Annual Review of Physical Chemistry·Taekjip Ha, Philip Tinnefeld
Dec 12, 2012·Angewandte Chemie·Haifeng YuanMichel Orrit
Jan 15, 2013·The Journal of Physical Chemistry. B·Tatyana G TerentyevaChun-Biu Li
Jul 23, 2013·FEBS Letters·L Michaelis, Miss Maud L Menten
Jul 1, 2014·Optics Express·Lutz Langguth, A Femius Koenderink
Jul 11, 2014·Annual Review of Statistics and Its Application·Hong Qian, S C Kou
Sep 10, 2014·Physical Chemistry Chemical Physics : PCCP·Saumyakanti KhatuaMichel Orrit
Feb 11, 2015·Physics of Life Reviews·Warren Colomb, Susanta K Sarkar
Apr 16, 2016·The Journal of Physical Chemistry Letters·Emilie WientjesNiek F van Hulst
Feb 10, 2017·Nano Letters·Valentin FlauraudJürgen Brugger
Jun 9, 2017·Langmuir : the ACS Journal of Surfaces and Colloids·Pedro M R PauloSílvia M B Costa
Aug 2, 2017·ACS Sensors·Adam B Taylor, Peter Zijlstra
Nov 9, 2017·Langmuir : the ACS Journal of Surfaces and Colloids·James Nicholas VranishIgor L Medintz
Jan 23, 2018·ACS Photonics·A Femius Koenderink

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Citations

Sep 24, 2019·Langmuir : the ACS Journal of Surfaces and Colloids·Yuyang WangPeter Zijlstra

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Methods Mentioned

BETA
confocal microscopy
fluorescence correlation spectroscopy
fluorescence-correlation spectroscopy
PCR

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