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Out-of-equilibrium catalysis of chemical reactions by electronic tunnel currents
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10.1063/1.4797495
/content/aip/journal/jcp/138/13/10.1063/1.4797495
http://aip.metastore.ingenta.com/content/aip/journal/jcp/138/13/10.1063/1.4797495

Figures

Image of FIG. 1.
FIG. 1.

(Upper part) Possible experimental setup. The STM tip is positioned above a molecule (represented as a sphere). An electron coming from the tip onto the molecule then tunnel into the conducting surface. A gate electrode is used to tune the molecular energy level(s), and to control the current flow between the STM tip and the conducting surface. (Lower part) Schematic illustration of the model. By varying the gate voltage, the molecular energy level can be shifted near the chemical potential of the electrodes. The molecular orbital energy ɛ(x) and electron-electron interaction energy U C(x) depend on the bond length x.

Image of FIG. 2.
FIG. 2.

Effective single particle energy level ɛeff(x) and population n(x) as a function of the reaction coordinate x for different values of the asymmetry coefficient g = Γ L R and applied voltage V. We chose ɛeff(x min) = −9.8 eV, where x min = 1.66 a.u. corresponds to the minimum of the equilibrium potential energy of the molecule. The Fermi energies of the electrodes are set to zero.

Image of FIG. 3.
FIG. 3.

Friction coefficient ξ(x) and noise intensity D(x) as a function of the reaction coordinate x. All the parameters are the same as those in Fig. 2 .

Image of FIG. 4.
FIG. 4.

(Upper panels) Effective temperature T eff as a function of the reaction coordinate x for two values of the applied voltage x. (Lower panels) Effective temperature T eff as a function of the applied voltage V for two values of the reaction coordinate x. All the parameters are the same as those in Fig. 2 .

Image of FIG. 5.
FIG. 5.

Effective nonequilibrium potential U eff(x) as a function of the reaction coordinate x for two values of the applied voltage V. The panels correspond to different positions of the effective molecular orbital energy relative to the electrode Fermi energy εeff(x min) = −9.8 eV + V g . All other parameters are the same as those in Fig. 2 .

Image of FIG. 6.
FIG. 6.

Escape time computed for various values of the asymmetry coefficient g as a function of the applied voltage. The left and right panels correspond to different positions of the effective molecular orbital energy relative to the electrode Fermi energy εeff(x min) = −9.8 eV + V g . All other parameters are the same as those in Fig. 2 .

Image of FIG. 7.
FIG. 7.

Reaction rate for the molecule dissociation computed at the fixed applied voltage as a function of the electric current. The left and right panels correspond to different positions of the effective molecular orbital energy relative to the electrode Fermi energy εeff(x min) = −9.8 eV + V g . In our calculations we choose the right coupling fixed, Γ R = 1.36 eV, and vary the left coupling to change the current at constant applied voltage. All other parameters are the same as those in Fig. 2 .

Tables

Generic image for table
Table I.

The period of motion (Eq. (19) , a.u. of time) in the nonequilibrium effective potential (the bias voltage V = 1.36 eV) for different values of the asymmetry coefficient g and the gate voltage V g . The parameter k defines the energy, k = (EE min)/(E maxE min). All other parameters are the same as those in Fig. 2 .

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/content/aip/journal/jcp/138/13/10.1063/1.4797495
2013-04-01
2014-04-19
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Out-of-equilibrium catalysis of chemical reactions by electronic tunnel currents
http://aip.metastore.ingenta.com/content/aip/journal/jcp/138/13/10.1063/1.4797495
10.1063/1.4797495
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