scholarly journals Single-molecule spectroelectrochemical cross-correlation during redox cycling in recessed dual ring electrode zero-mode waveguides

2017 ◽  
Vol 8 (8) ◽  
pp. 5345-5355 ◽  
Author(s):  
Donghoon Han ◽  
Garrison M. Crouch ◽  
Kaiyu Fu ◽  
Lawrence P. Zaino III ◽  
Paul W Bohn

The ability of zero-mode waveguides (ZMW) to guide light into subwavelength-diameter nanoapertures has been exploited for studying electron transfer dynamics in zeptoliter-volume nanopores under single-molecule occupancy conditions.

2016 ◽  
Vol 120 (37) ◽  
pp. 20634-20641 ◽  
Author(s):  
Donghoon Han ◽  
Lawrence P. Zaino ◽  
Kaiyu Fu ◽  
Paul W. Bohn

2017 ◽  
Vol 137 (6) ◽  
pp. 159-164
Author(s):  
Kazuya Fujimoto ◽  
Yuki Morita ◽  
Ryota Iino ◽  
Michio Tomishige ◽  
Hirofumi Shintaku ◽  
...  
Keyword(s):  

2021 ◽  
Vol 125 (7) ◽  
pp. 1735-1745 ◽  
Author(s):  
Amanda S. Harper-Leatherman ◽  
Jean Marie Wallace ◽  
Jeffrey W. Long ◽  
Christopher P. Rhodes ◽  
Molly E. Graffam ◽  
...  

ACS Nano ◽  
2013 ◽  
Vol 7 (6) ◽  
pp. 5391-5401 ◽  
Author(s):  
Emil Wierzbinski ◽  
Ravindra Venkatramani ◽  
Kathryn L. Davis ◽  
Silvia Bezer ◽  
Jing Kong ◽  
...  

2004 ◽  
Vol 43 (45) ◽  
pp. 6116-6120 ◽  
Author(s):  
Mircea Cotlet ◽  
Sadahiro Masuo ◽  
Marc Lor ◽  
Eduard Fron ◽  
Mark Van der Auweraer ◽  
...  

2016 ◽  
Author(s):  
Changbong Hyeon ◽  
D. Thirumalai

AbstractUsing force as a probe to map the folding landscapes of RNA molecules has become a reality thanks to major advances in single molecule pulling experiments. Although the unfolding pathways under tension are complicated to predict studies in the context of proteins have shown that topology plays is the major determinant of the unfolding landscapes. By building on this finding we study the responses of RNA molecules to force by adapting Gaussian network model (GNM) that represents RNAs using a bead-spring network with isotropic interactions. Cross-correlation matrices of residue fluctuations, which are analytically calculated using GNM even upon application of mechanical force, show distinct allosteric communication as RNAs rupture. The model is used to calculate the force-extension curves at full thermodynamic equilibrium, and the corresponding unfolding pathways of four RNA molecules subject to a quasi-statically increased force. Our study finds that the analysis using GNM captures qualitatively the unfolding pathway of T. ribozyme elucidated by the optical tweezers measurement. However, the simple model is not sufficient to capture subtle features, such as bifurcation in the unfolding pathways or the ion effects, in the forced-unfolding of RNAs.


2015 ◽  
Vol 184 ◽  
pp. 101-115 ◽  
Author(s):  
Lawrence P. Zaino ◽  
Dane A. Grismer ◽  
Donghoon Han ◽  
Garrison M. Crouch ◽  
Paul W. Bohn

Zero-mode waveguides (ZMW) have the potential to be powerful confinement tools for studying electron transfer dynamics at single molecule occupancy conditions. Flavin mononucleotide contains an isoalloxazine chromophore, which is fluorescent in the oxidized state (FMN) while the reduced state (FMNH2) exhibits dramatically lower light emission, i.e. a dark-state. This allows fluorescence emission to report the redox state of single FMN molecules, an observation that has been used previously to study single electron transfer events in surface-immobilized flavins and flavoenzymes, e.g. sarcosine oxidase, by direct wide-field imaging of ZMW arrays. Single molecule electron transfer dynamics have now been extended to the study of freely diffusing molecules using fluorescence measurements of Au ZMWs under single occupancy conditions. The Au in the ZMW serves both as an optical cladding layer and as the working electrode for potential control, thereby accessing single molecule electron transfer dynamics at μM concentrations. Consistent with expectations, the probability of observing single reduced molecules increases as the potential is scanned negative, Eappl < Eeq, and the probability of observing emitting oxidized molecules increases at Eappl > Eeq. Different single molecules exhibit different electron transfer properties as reflected in the position of Eeq and the distribution of Eeq among a population of FMN molecules. Two types of actively-controlled electroluminescence experiments were used: chronofluorometry experiments, in which the potential is alternately stepped between oxidizing and reducing potentials, and cyclic potential sweep fluorescence experiments, analogous to cyclic voltammetry, these latter experiments exhibiting a dramatic scan rate dependence with the slowest scan rates showing distinct intermediate states that are stable over a range of potentials. These states are assigned to flavosemiquinone species that are stabilized in the special environment of the ZMW nanopore.


2013 ◽  
Vol 117 (42) ◽  
pp. 13015-13028 ◽  
Author(s):  
Dominik Haenni ◽  
Franziska Zosel ◽  
Luc Reymond ◽  
Daniel Nettels ◽  
Benjamin Schuler

Nanoscale ◽  
2018 ◽  
Vol 10 (36) ◽  
pp. 17362-17369 ◽  
Author(s):  
Paolo Ponzellini ◽  
Xavier Zambrana-Puyalto ◽  
Nicolò Maccaferri ◽  
Luca Lanzanò ◽  
Francesco De Angelis ◽  
...  

Experimental verification of a plasmonic zero mode waveguide able to enhance fluorescence from a single molecule in a confined volume.


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