Mechanically Activated Molecular Switch through Single-Molecule Pulling

Ignacio Franco; Christopher B. George; Gemma Clare Solomon; George C. Schatz; Mark A. Ratner

Mechanically Activated Molecular Switch through Single-Molecule Pulling

Ignacio Franco, Christopher B. George, Gemma Clare Solomon, George C. Schatz, Mark A. Ratner

Kemisk Institut

48 Citationer (Scopus)

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.

Originalsprog	Engelsk
Tidsskrift	Journal of the American Chemical Society
Vol/bind	133
Sider (fra-til)	2242-2249
ISSN	0002-7863
Status	Udgivet - 23 feb. 2011

Citationsformater

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T1 - Mechanically Activated Molecular Switch through Single-Molecule Pulling

AU - Franco, Ignacio

AU - George, Christopher B.

AU - Solomon, Gemma Clare

AU - Schatz, George C.

AU - Ratner, Mark A.

PY - 2011/2/23

Y1 - 2011/2/23

N2 - 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.

AB - 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.

M3 - Journal article

SN - 0002-7863

VL - 133

SP - 2242

EP - 2249

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

ER -

Mechanically Activated Molecular Switch through Single-Molecule Pulling

Abstract

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