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Volumn 126, Issue 44, 2004, Pages 14620-14630

Interfacial electron-transfer kinetics of ferrocene through oligophenyleneethynylene bridges attached to gold electrodes as constituents of self-assembled monolayers: Observation of a nonmonotonic distance dependence

Author keywords

[No Author keywords available]

Indexed keywords

ELECTRODES; MOLECULAR STRUCTURE; REACTION KINETICS; SUBSTRATES; THERMAL EFFECTS;

EID: 7744244037     PISSN: 00027863     EISSN: None     Source Type: Journal    
DOI: 10.1021/ja047458b     Document Type: Article
Times cited : (118)

References (119)
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    • Ph.D. Thesis, Stanford University, Stanford, CA
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    • (2000)
    • Sachs, S.B.1
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    • note
    • n,NA in eq 6 omits a factor of order unity.20,26
  • 78
    • 11944257247 scopus 로고
    • Chidsey, C. E. D.; Bertozzi, C. R.; Putvinski, T. M.; Mujsce, A. M. J. Am. Chem. Soc. 1990, 112, 4301-4306. See Figure 2 in this reference for examples of cyclic voltammograms of mixed alkanethiol SAMs in which the ferrocene redox moieties are not isolated and, therefore, not identical.
    • (1990) J. Am. Chem. Soc. , vol.112 , pp. 4301-4306
    • Chidsey, C.E.D.1    Bertozzi, C.R.2    Putvinski, T.M.3    Mujsce, A.M.4
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    • note
    • A,n (see eq 10 in ref 26).67
  • 82
    • 7744223646 scopus 로고    scopus 로고
    • note
    • In agreement with the CV results discussed previously, these diagnostic checks also confirm that the ferrocene redox moieties are identical and isolated.
  • 88
    • 7744222205 scopus 로고    scopus 로고
    • note
    • n,app for electroactive compound I, therefore, is not an artifact of our measurements.2,26
  • 89
    • 7744223042 scopus 로고    scopus 로고
    • note
    • 4) eV (including the data determined in the present study).20,26,13
  • 91
  • 92
    • 7744232370 scopus 로고    scopus 로고
    • note
    • This result does not contradict either the observations or the conclusions presented in ref 36.
  • 100
    • 7744224221 scopus 로고    scopus 로고
    • note
    • A,n are consistent with Marcus theory requires that the enthalpy changes associated with these equilibria be negligible.35, 37
  • 101
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    • note
    • i.
  • 102
    • 7744242902 scopus 로고    scopus 로고
    • note
    • ab,n (a reduction of less than 10% for n = 3) and β was found to be minor.81
  • 106
    • 7744231203 scopus 로고    scopus 로고
    • note
    • n OH (diluents 1, 3, and 7 in Chart 2), L = 4.06 Å + 1.09 Å(n); for diluent number 8 in Chart 2, L = 21.63 Å; for diluent number 2 in Chart 2, L = 6.85 Å; for diluents numbers 5 and 11 in Chart 2, L= 11.78 and 18.67 Å, respectively; and for diluent number 9 in Chart 2, L = 20.70 Å (average of the values for diluents numbers 6 and 7). Note that all of these values of L include the diameter of the adsorbed sulfur atom.
  • 108
    • 7744236497 scopus 로고    scopus 로고
    • note
    • n versus l data that includes the unsubstituted data at n = 2 and n = 4 as well as the substituted data (see the black dotted line in Figure 7). However, the choice of such a subset is ad hoc and unnecessary for the present rough calculation.
  • 109
    • 7744246831 scopus 로고    scopus 로고
    • note
    • For example, all of the other (nonreactive) conformations could be in equilibrium with the reactive, optimal conformations.82
  • 111
    • 7744246527 scopus 로고    scopus 로고
    • note
    • M = 0.75, 0.41, and 0.24 V, respectively. The good fits to eqs 3-5 (such as those shown in Figure 4) also demonstrate that changing the potential drop through the monolayer by as much as an additional ±0.15 V has no effect on the rate of electron transfer through OPE bridges. However, the distributions of electrostatic potential along the lengths of these bridges are unknown.13,33,94
  • 115
    • 7744245925 scopus 로고    scopus 로고
    • note
    • We should emphasize that, even though there are significant potential changes across the Au-bridge-Fc junctions effected by the SAMs employed in the present study,92 the electron-transfer reaction in an ILIT experiment is driven by a free energy change that is always less than a few millielectronvolts (see, for example, the data in Figures 2 and 3).
  • 116
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    • Xu, B.; Tao, N. J. Science 2003, 301, 1221-1223.
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    • Xu, B.1    Tao, N.J.2
  • 117
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    • note
    • A calculated52 conductance based upon the model presented in ref 13 also is in excellent agreement with the measured conductance reported in ref 52. However, we should point out that the authors of ref 52 assume that their measured conductance is effected by a "hopping" mechanism while the model presented in ref 13 is a only valid for a (nonresonant) tunneling mechanism.


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