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Title: Mechanically Activated Molecular Switch through Single-Molecule Pulling

Abstract

We investigate a prototypical single-molecule switch marrying force spectroscopy and molecular electronics far from the thermodynamic limit. We use molecular dynamics to simulate a conducting atomic force microscope mechanically manipulating a molecule bound to a surface between a folded state and an unfolded state while monitoring the conductance. Both the complexity and the unique phenomenology of single-molecule experiments are evident in this system. As the molecule unfolds/refolds, the average conductance reversibly changes over 3 orders of magnitude; however, throughout the simulation the transmission fluctuates considerably, illustrating the need for statistical sampling in these systems. We predict that emergent single-molecule signatures will still be evident with conductance blinking, correlated with force blinking, being observable in a region of dynamic bistability. Finally, we illustrate some of the structure-function relationships in this system, mapping the dominant interactions in the molecule for mediating charge transport throughout the pulling simulation.

Authors:
; ; ; ;
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC); Center for Bio-Inspired Energy Science (CBES)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1065455
DOE Contract Number:  
SC0000989
Resource Type:
Journal Article
Resource Relation:
Journal Name: J. Am. Chem. Soc.; Journal Volume: 133 (7); Related Information: CBES partners with Northwestern University (lead); Harvard University; New York University; Pennsylvania State University; University of Michigan; University of Pittsburgh
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; catalysis (homogeneous), solar (photovoltaic), bio-inspired, charge transport, mesostructured materials, materials and chemistry by design, synthesis (novel materials), synthesis (self-assembly)

Citation Formats

Franco, Ignacio, George, Christopher B., Solomon, G.C., Schatz, George C., and Ratner, Mark A.. Mechanically Activated Molecular Switch through Single-Molecule Pulling. United States: N. p., 2011. Web. doi:10.1021/ja1095396.
Franco, Ignacio, George, Christopher B., Solomon, G.C., Schatz, George C., & Ratner, Mark A.. Mechanically Activated Molecular Switch through Single-Molecule Pulling. United States. doi:10.1021/ja1095396.
Franco, Ignacio, George, Christopher B., Solomon, G.C., Schatz, George C., and Ratner, Mark A.. Wed . "Mechanically Activated Molecular Switch through Single-Molecule Pulling". United States. doi:10.1021/ja1095396.
@article{osti_1065455,
title = {Mechanically Activated Molecular Switch through Single-Molecule Pulling},
author = {Franco, Ignacio and George, Christopher B. and Solomon, G.C. and Schatz, George C. and Ratner, Mark A.},
abstractNote = {We investigate a prototypical single-molecule switch marrying force spectroscopy and molecular electronics far from the thermodynamic limit. We use molecular dynamics to simulate a conducting atomic force microscope mechanically manipulating a molecule bound to a surface between a folded state and an unfolded state while monitoring the conductance. Both the complexity and the unique phenomenology of single-molecule experiments are evident in this system. As the molecule unfolds/refolds, the average conductance reversibly changes over 3 orders of magnitude; however, throughout the simulation the transmission fluctuates considerably, illustrating the need for statistical sampling in these systems. We predict that emergent single-molecule signatures will still be evident with conductance blinking, correlated with force blinking, being observable in a region of dynamic bistability. Finally, we illustrate some of the structure-function relationships in this system, mapping the dominant interactions in the molecule for mediating charge transport throughout the pulling simulation.},
doi = {10.1021/ja1095396},
journal = {J. Am. Chem. Soc.},
number = ,
volume = 133 (7),
place = {United States},
year = {Wed Feb 23 00:00:00 EST 2011},
month = {Wed Feb 23 00:00:00 EST 2011}
}