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Title: Super-resolution imaging of non-fluorescent reactions via competition

Abstract

Super-resolved fluorescence microscopy techniques have enabled substantial advances in the chemical and biological sciences. However, they can only interrogate entities that fluoresce, and most chemical or biological processes do not involve fluorescent species. Here we report a competition-enabled imaging technique with super-resolution (COMPEITS) (a COMPetition-Enabled Imaging Technique with Super-resolution) that enables quantitative super-resolution imaging of non-fluorescent processes. It is based on the incorporation of competition into a single-molecule fluorescence-detection scheme. We demonstrate COMPEITS by investigating a photoelectrocatalytic reaction; we map, with nanometre precision, a non-fluorescent surface reaction that is important for water decontamination on single photocatalyst particles. The subparticle-level quantitative information of reactant adsorption affinities unambiguously decouples size- and shape-scaling laws on specific particle facets and uncovers a surprising biphasic shape dependence, leading to catalyst design principles for optimal reactant adsorption efficacy. With its ability to provide spatially resolved information on the behaviours of unlabelled, non-fluorescent entities under operando conditions, COMPEITS could interrogate a variety of surface processes in fields ranging from heterogeneous catalysis and materials engineering to nanotechnology and energy sciences.

Authors:
 [1];  [1];  [1];  [1]; ORCiD logo [1]
  1. Cornell Univ., Ithaca, NY (United States). Dept. of Chemistry and Chemical Biology
Publication Date:
Research Org.:
Cornell Univ., Ithaca, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; US Army Research Office (ARO); NSF MRSEC Program
OSTI Identifier:
1593523
Grant/Contract Number:  
SC0004911; W911NF-17-1-0590; W911NF-18-1-0217; DMR-1719875
Resource Type:
Accepted Manuscript
Journal Name:
Nature Chemistry
Additional Journal Information:
Journal Volume: 11; Journal Issue: 8; Journal ID: ISSN 1755-4330
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Mao, Xianwen, Liu, Chunming, Hesari, Mahdi, Zou, Ningmu, and Chen, Peng. Super-resolution imaging of non-fluorescent reactions via competition. United States: N. p., 2019. Web. doi:10.1038/s41557-019-0288-8.
Mao, Xianwen, Liu, Chunming, Hesari, Mahdi, Zou, Ningmu, & Chen, Peng. Super-resolution imaging of non-fluorescent reactions via competition. United States. doi:10.1038/s41557-019-0288-8.
Mao, Xianwen, Liu, Chunming, Hesari, Mahdi, Zou, Ningmu, and Chen, Peng. Mon . "Super-resolution imaging of non-fluorescent reactions via competition". United States. doi:10.1038/s41557-019-0288-8.
@article{osti_1593523,
title = {Super-resolution imaging of non-fluorescent reactions via competition},
author = {Mao, Xianwen and Liu, Chunming and Hesari, Mahdi and Zou, Ningmu and Chen, Peng},
abstractNote = {Super-resolved fluorescence microscopy techniques have enabled substantial advances in the chemical and biological sciences. However, they can only interrogate entities that fluoresce, and most chemical or biological processes do not involve fluorescent species. Here we report a competition-enabled imaging technique with super-resolution (COMPEITS) (a COMPetition-Enabled Imaging Technique with Super-resolution) that enables quantitative super-resolution imaging of non-fluorescent processes. It is based on the incorporation of competition into a single-molecule fluorescence-detection scheme. We demonstrate COMPEITS by investigating a photoelectrocatalytic reaction; we map, with nanometre precision, a non-fluorescent surface reaction that is important for water decontamination on single photocatalyst particles. The subparticle-level quantitative information of reactant adsorption affinities unambiguously decouples size- and shape-scaling laws on specific particle facets and uncovers a surprising biphasic shape dependence, leading to catalyst design principles for optimal reactant adsorption efficacy. With its ability to provide spatially resolved information on the behaviours of unlabelled, non-fluorescent entities under operando conditions, COMPEITS could interrogate a variety of surface processes in fields ranging from heterogeneous catalysis and materials engineering to nanotechnology and energy sciences.},
doi = {10.1038/s41557-019-0288-8},
journal = {Nature Chemistry},
number = 8,
volume = 11,
place = {United States},
year = {2019},
month = {7}
}

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    Works referencing / citing this record:

    A Smart Nanoprobe Based On Fluorescence-Quenching PEGylated Nanogels Containing Gold Nanoparticles for Monitoring the Response to Cancer Therapy
    journal, March 2009

    • Oishi, Motoi; Tamura, Atsushi; Nakamura, Takahito
    • Advanced Functional Materials, Vol. 19, Issue 6
    • DOI: 10.1002/adfm.200801164

    Correlative Super-Resolution Microscopy: New Dimensions and New Opportunities
    journal, January 2017


    Three-Dimensional Localization of Single Molecules for Super-Resolution Imaging and Single-Particle Tracking
    journal, February 2017


    Optical Super-Resolution Imaging of Surface Reactions
    journal, March 2017


    Superresolution Imaging of Biological Systems Using Photoactivated Localization Microscopy
    journal, January 2014

    • Sengupta, Prabuddha; van Engelenburg, Schuyler B.; Lippincott-Schwartz, Jennifer
    • Chemical Reviews, Vol. 114, Issue 6
    • DOI: 10.1021/cr400614m

    Size-Dependent Catalytic Activity and Dynamics of Gold Nanoparticles at the Single-Molecule Level
    journal, January 2010

    • Zhou, Xiaochun; Xu, Weilin; Liu, Guokun
    • Journal of the American Chemical Society, Vol. 132, Issue 1
    • DOI: 10.1021/ja904307n

    Single-Molecule Investigation of Initiation Dynamics of an Organometallic Catalyst
    journal, March 2016

    • Ng, James D.; Upadhyay, Sunil P.; Marquard, Angela N.
    • Journal of the American Chemical Society, Vol. 138, Issue 11
    • DOI: 10.1021/jacs.6b00357

    Single Molecule Nanospectroscopy Visualizes Proton-Transfer Processes within a Zeolite Crystal
    journal, October 2016

    • Ristanović, Zoran; Kubarev, Alexey V.; Hofkens, Johan
    • Journal of the American Chemical Society, Vol. 138, Issue 41
    • DOI: 10.1021/jacs.6b06083

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    • Nature, Vol. 439, Issue 7076
    • DOI: 10.1038/nature04502

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    • DOI: 10.1038/nature06599

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    Sub-particle reaction and photocurrent mapping to optimize catalyst-modified photoanodes
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    • DOI: 10.1038/nature16534

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    • Wu, Chung-Yeh; Wolf, William J.; Levartovsky, Yehonatan
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    Nanoparticles with photoinduced precipitation for the extraction of pollutants from water and soil
    journal, July 2015

    • Brandl, Ferdinand; Bertrand, Nicolas; Lima, Eliana Martins
    • Nature Communications, Vol. 6, Issue 1
    • DOI: 10.1038/ncomms8765

    Single-molecule nanocatalysis reveals heterogeneous reaction pathways and catalytic dynamics
    journal, November 2008

    • Xu, Weilin; Kong, Jason S.; Yeh, Yun-Ting E.
    • Nature Materials, Vol. 7, Issue 12
    • DOI: 10.1038/nmat2319

    Fluorescence nanoscopy by ground-state depletion and single-molecule return
    journal, September 2008

    • Fölling, Jonas; Bossi, Mariano; Bock, Hannes
    • Nature Methods, Vol. 5, Issue 11
    • DOI: 10.1038/nmeth.1257

    Genetically encoded biosensors for visualizing live-cell biochemical activity at super-resolution
    journal, March 2017

    • Mo, Gary C. H.; Ross, Brian; Hertel, Fabian
    • Nature Methods, Vol. 14, Issue 4
    • DOI: 10.1038/nmeth.4221

    Sub-diffraction-limit imaging by stochastic optical reconstruction microscopy (STORM)
    journal, August 2006

    • Rust, Michael J.; Bates, Mark; Zhuang, Xiaowei
    • Nature Methods, Vol. 3, Issue 10
    • DOI: 10.1038/nmeth929

    Quantitative super-resolution imaging uncovers reactivity patterns on single nanocatalysts
    journal, February 2012

    • Zhou, Xiaochun; Andoy, Nesha May; Liu, Guokun
    • Nature Nanotechnology, Vol. 7, Issue 4
    • DOI: 10.1038/nnano.2012.18

    3D single-molecule super-resolution microscopy with a tilted light sheet
    journal, January 2018

    • Gustavsson, Anna-Karin; Petrov, Petar N.; Lee, Maurice Y.
    • Nature Communications, Vol. 9, Issue 1
    • DOI: 10.1038/s41467-017-02563-4

    99TcO4− remediation by a cationic polymeric network
    journal, August 2018


    Two-dimensional Na–Cl crystals of unconventional stoichiometries on graphene surface from dilute solution at ambient conditions
    journal, May 2018


    Emerging opportunities for nanotechnology to enhance water security
    journal, August 2018

    • Alvarez, Pedro J. J.; Chan, Candace K.; Elimelech, Menachem
    • Nature Nanotechnology, Vol. 13, Issue 8
    • DOI: 10.1038/s41565-018-0203-2

    Electron ptychography of 2D materials to deep sub-ångström resolution
    journal, July 2018


    X-ray and cryo-EM structures of the mitochondrial calcium uniporter
    journal, July 2018


    Adsorption of organic molecules on rutile TiO2 and anatase TiO2 single crystal surfaces
    journal, January 2012

    • Thomas, Andrew G.; Syres, Karen L.
    • Chemical Society Reviews, Vol. 41, Issue 11
    • DOI: 10.1039/c2cs35057b

    Superresolution fluorescence mapping of single-nanoparticle catalysts reveals spatiotemporal variations in surface reactivity
    journal, July 2015

    • Zhang, Yuwei; Lucas, J. Matthew; Song, Ping
    • Proceedings of the National Academy of Sciences, Vol. 112, Issue 29
    • DOI: 10.1073/pnas.1502005112

    Intermittent photocatalytic activity of single CdS nanoparticles
    journal, September 2017

    • Fang, Yimin; Li, Zhimin; Jiang, Yingyan
    • Proceedings of the National Academy of Sciences, Vol. 114, Issue 40
    • DOI: 10.1073/pnas.1708617114

    The Challenge of Micropollutants in Aquatic Systems
    journal, August 2006


    Imaging Intracellular Fluorescent Proteins at Nanometer Resolution
    journal, September 2006


    Identification of Active Edge Sites for Electrochemical H2 Evolution from MoS2 Nanocatalysts
    journal, July 2007

    • Jaramillo, T. F.; Jorgensen, K. P.; Bonde, J.
    • Science, Vol. 317, Issue 5834, p. 100-102
    • DOI: 10.1126/science.1141483

    Break-Up of Stepped Platinum Catalyst Surfaces by High CO Coverage
    journal, February 2010


    Room-Temperature Detection of a Single Molecule's Absorption by Photothermal Contrast
    journal, October 2010


    Nanoporous BiVO4 Photoanodes with Dual-Layer Oxygen Evolution Catalysts for Solar Water Splitting
    journal, February 2014


    Increased spatiotemporal resolution reveals highly dynamic dense tubular matrices in the peripheral ER
    journal, October 2016


    Nanometer resolution imaging and tracking of fluorescent molecules with minimal photon fluxes
    journal, December 2016


    Hydrolytically stable fluorinated metal-organic frameworks for energy-efficient dehydration
    journal, May 2017


    Super-resolution chromatin tracing reveals domains and cooperative interactions in single cells
    journal, October 2018