Australian Journal of Chemistry Australian Journal of Chemistry Society
An international journal for chemical science
RESEARCH FRONT

Redox-Executed Logic Operations through the Reversible Voltammetric Response Characteristics of Electroactive Self-Assembled Monolayers

Ganga Periyasamy A , R. D. Levine B C D and F. Remacle A D
+ Author Affiliations
- Author Affiliations

A Department of Chemistry, B6c, University of Liège, B4000 Liège, Belgium.

B The Fritz Haber Research Center for Molecular Dynamics, The Hebrew University of Jerusalem, Jerusalem 91904, Israel.

C Department of Chemistry and Biochemistry, Crump Institute for Molecular Imaging and Department of Molecular and Medical Pharmacology, The University of California Los Angeles, Los Angeles, CA 90095, USA.

D Corresponding authors. Email: fremacle@ulg.ac.be; rafi@fh.huji.ac.il

Australian Journal of Chemistry 63(2) 173-183 https://doi.org/10.1071/CH09504
Submitted: 19 September 2009  Accepted: 13 January 2010   Published: 26 February 2010

Abstract

We propose charge quantization in electrochemical oxidation–reduction (redox) systems as a route to performing logical operations efficiently and reversibly. The theory is based on the interfacial potential distribution for electrodes coated with electroactive self-assembled molecular films. We monitor the change in the oxidation number by studying the current as a function of the working and reference electrode potentials and of the temperature. Diamond-shaped regions can be defined that delineate the stability of a given redox species as a function of the applied and reference potentials. Using these electrochemical Coulomb diamonds, we then show the principles for the design of a complete set of binary gates and a finite-state set–reset machine. We demonstrate the analogies between these redox systems and nanoscale solid-state systems where the charging energy is finite. Redox systems allow simple logic operations at room temperature because typically the standard potential is higher than the thermal energy.


Acknowledgements

Our work is supported by the FET-Proactive STREP FP7 project MOLOC. G.P. is supported by a post-doctoral fellowship of the Inter-University Attraction Pole (IAP) project ‘Cluster and Nanowires’ of the Belgian Federal Government.


References


[1]   Bard A. J., Faulkner L. R., Electrochemical Methods: Fundamentals and Applications 2001 (Wiley: New York, NY).

[2]   Brett C. M. A., Brett A. M. O., Electrochemistry: Principles, Methods and Applications 1993 (Oxford University Press: Oxford).

[3]   L. E. Brus, J. Chem. Phys. 1983, 79,  5566.
        | CrossRef |   

[4]   R. C. Ashoori, Nature 1996, 379,  413.
        | CrossRef |   

[5]   M. A. Kastner, Phys. Today 1993, 46,  24.
        | CrossRef |   

[6]   A. P. Alivisatos, Science 1996, 271,  933.
        | CrossRef |   

[7]   U. Banin, Y. W. Cao, D. Katz, O. Millo, Nature 1999, 400,  542.
        | CrossRef |   

[8]   S. Chen, R. S. Ingram, M. J. Hostetler, J. J. Pietron, R. W. Murray, T. G. Schaaff, J. T. Khoury, M. M. Alvarez, R. L. Whetten, Science 1998, 280,  2098.
        | CrossRef |   

[9]   G. Markovich, C. P. Collier, S. E. Henrichs, F. Remacle, R. D. Levine, J. R. Heath, Acc. Chem. Res. 1999, 32,  415.
        | CrossRef |   

[10]   F. Remacle, R. D. Levine, ChemPhysChem 2001, 2,  20.
        | CrossRef |   

[11]   L. Brus, J. Phys. Chem. 1986, 90,  2555.
        | CrossRef |   

[12]   G. J. Iafrate, K. Hess, J. B. Krieger, M. Maccuci, Phys. Rev. B 1995, 52,  10737.
        | CrossRef |   

[13]   Imry Y., Introduction to Mesoscopic Physics 2002 (Oxford University Press: Oxford).

[14]   B. M. Quinn, P. Liljeroth, V. Ruiz, T. Laaksonen, K. Kontturi, J. Am. Chem. Soc. 2003, 125,  6644.
        | CrossRef |   

[15]   E. Katz, O. Lioubashevski, I. Willner, Chem. Comm. 2006,  1109.
         

[16]   J. R. Tucker, J. Appl. Phys. 1992, 72,  4399.
        | CrossRef |   

[17]   D. V. Averin, A. N. Korotkov, K. K. Likharev, Phys. Rev. B 1991, 44,  6199.
        | CrossRef |   

[18]   Single Charge Tunneling (Eds H. Grabert, M. H. Devoret) 1992 (Plenum Press: New York, NY).

[19]   Kouwenhoven L. P., McEuen P. L., in Nanotechnology (Ed. G. Timp) 1999, pp. 475–536 (Springer Verlag: New York, NY).

[20]   K. K. Likharev, Proc. IEEE 1999, 87,  606.
        | CrossRef |   

[21]   Uchida K., in Nanoelectronics and Information Technology (Ed. R. Waser) 2003, pp. 426–443 (Wiley-VCH: Weinheim).

[22]   Y. Ono, A. Fujiwara, K. Nishiguchi, H. Inokawa, Y. Takahashi, J. Appl. Phys. 2005, 97,  031101.
        | CrossRef |   

[23]   R. Hanson, L. P. Kouwenhoven, J. R. Petha, S. Tarucha, L. M. K. Vandersypen, Rev. Mod. Phys. 2007, 79,  1217.
        | CrossRef |   

[24]   M. Klein, R. D. Levine, F. Remacle, J. Appl. Phys. 2008, 104,  044509.
        | CrossRef |   

[25]   M. Klein, G. P. Lansbergen, J. A. Mol, S. Rogge, R. D. Levine, F. Remacle, ChemPhysChem 2009, 10,  162.
        | CrossRef |   

[26]   F. Remacle, J. R. Heath, R. D. Levine, Proc. Natl. Acad. Sci. USA 2005, 102,  5653.
        | CrossRef |   

[27]   A. J. Houtepen, D. Vanmaekelbergh, J. Phys. Chem. B 2005, 109,  19634.
        | CrossRef |   

[28]   D. Vanmaekelbergh, A. J. Houtepen, J. J. Kelly, Electrochim. Acta 2007, 53,  1140.
        | CrossRef |   

[29]   C. P. Smith, H. S. White, Anal. Chem. 1992, 64,  2398.
        | CrossRef |   

[30]   M. Ohtani, Electrochem. Commun. 1999, 1,  488.
        | CrossRef |   

[31]   M. Ohtani, S. Kuwabata, H. Yoneyama, Anal. Chem. 1997, 69,  1045.
        | CrossRef |   

[32]   Mano M. M., Kime C. R., Logic and Computer Design Fundamentals 2000 (Prentice Hall: Upper Saddle River, NJ).

[33]   T. Albrecht, S. F. L. Mertens, J. Ulstrup, J. Am. Chem. Soc. 2007, 129,  9162.
        | CrossRef |   

[34]   U. Pischel, Angew. Chem. Int. Ed. 2007, 46,  4026.
        | CrossRef |   

[35]   A. P. de Silva, S. Uchiyama, Nat. Nanotechnol. 2007, 2,  399.
        | CrossRef |   

[36]   K. Szaciłowski, Chem. Rev. 2008, 108,  3481.
        | CrossRef |   

[37]   C. P. Collier, G. Mattersteig, E. W. Wong, Y. Luo, K. Beverly, J. Sampaio, F. M. Raymo, J. F. Stoddart, J. R. Heath, Science 2000, 289,  1172.
        | CrossRef |   

[38]   Y. Luo, C. P. Collier, J. O. Jeppesen, K. A. Nielsen, E. DeIonno, G. Ho, J. Perkins, H. R. Tseng, T. Yamamoto, J. F. Stoddart, J. R. Heath, ChemPhysChem 2002, 3,  519.
        | CrossRef |   

[39]   J. E. Green, J. W. Choi, A. Boukai, Y. Bunimovich, E. Johnston-Halperin, E. DeIonno, Y. Luo, B. A. Sheriff, K. Xu, Y. S. Shin, H. R. Tseng, J. F. Stoddart, J. R. Heath, Nature 2007, 445,  414.
        | CrossRef |   

[40]   G. Periyasamy, J.-P. Collin, J. P. Sauvage, R. D. Levine, F. Remacle, Chem. Eur. J. 2009, 15,  1310.
        | CrossRef |   

[41]   R. W. Murray, Chem. Rev. 2008, 108,  2688.
        | CrossRef |   

[42]   T. Gupta, M. E. van der Boom, Angew. Chem. Int. Ed. 2008, 47,  5322.
        | CrossRef |   

[43]   D. A. Leigh, M. A. F. Morales, E. M. Perez, J. K. Y. Wong, C. G. Saiz, A. M. Z. Slawin, A. J. Carmichael, D. M. Haddleton, A. M. Brouwer, W. J. Buma, G. W. H. Wurpel, S. Leon, F. Zerbetto, Angew. Chem. Int. Ed. 2005, 44,  3062.
        | CrossRef |   

[44]   F. Remacle, I. Willner, R. D. Levine, ChemPhysChem 2005, 6,  1239.
        | CrossRef |   

[45]   R. Baron, A. Onopriyenko, E. Katz, O. Lioubashevski, I. Willner, W. Sheng, H. Tian, Chem. Commun. 2006,  2147.
        | CrossRef |   

[46]   G. d Ruiter, E. Tartakovsky, N. Oded, M. E. v. d. Boom, Angew. Chem. Int. Ed. 2009, 48,
        | CrossRef |   

[47]   Smith C. P., White H. S., in Microscopic Models of Electrode–Electrolyte Interfaces, Vol. 93 (Ed. J. W. Halley) 1993, p. 5 (Electrochemical Society: Princeton, NJ).

[48]   C. P. Smith, H. S. White, Langmuir 1993, 9,  1.
        | CrossRef |   

[49]   J. Park, A. N. Pasupathy, J. I. Goldsmith, C. Chang, Y. Yaish, J. R. Petta, M. Rinkoski, J. P. Sthena, H. D. Abruna, P. L. McEuen, D. C. Ralph, Nature 2002, 417,  722.
        | CrossRef |   

[50]   J. Zhang, A. L. Barker, D. Mandler, P. R. Unwin, J. Am. Chem. Soc. 2003, 125,  9312.
        | CrossRef |   

[51]   S. B. Cronin, R. Barnett, M. Tinkham, S. G. Chou, O. Rabin, M. S. Dresselhaus, A. K. Swan, M. S. Unlu, B. B. Goldberg, Appl. Phys. Lett. 2004, 84,  2052.
        | CrossRef |   

[52]   P. Liljeroth, D. Vanmaekelbergh, V. Ruiz, K. Kontturi, H. Jiang, E. Kauppinen, B. M. Quinn, J. Am. Chem. Soc. 2004, 126,  7126.
        | CrossRef |   

[53]   L. Larrimore, S. Nad, X. Zhou, H. Abruna, P. L. McEuen, Nano Lett. 2006, 6,  1329.
        | CrossRef |   

[54]   P. G. Nicholson, V. Ruiz, J. V. Macpherson, P. R. Unwin, Phys. Chem. Chem. Phys. 2006, 8,  5096.
        | CrossRef |   

[55]   J. Zhang, A. M. Kuznetsov, I. G. Medvedev, Q. Chi, T. Albrecht, P. S. Jensen, J. Ulstrup, Chem. Rev. 2008, 108,  2737.
        | CrossRef |   

[56]   P. Ahonen, V. Ruiz, K. Kontturi, P. Liljeroth, B. M. Quinn, J. Phys. Chem. C 2008, 112,  2724.
        | CrossRef |   

[57]   F. Chen, N. J. Tao, Acc. Chem. Res. 2009, 42,  429.
        | CrossRef |   

[58]   A. B. Kharitonov, A. N. Shipway, I. Willner, Anal. Chem. 1999, 71,  5441.
        | CrossRef |   

[59]   M. Motornov, R. Sheparovych, E. Katz, S. Minko, ACS Nano 2008, 2,  41.
        | CrossRef |   

[60]   J. F. Smalley, M. D. Newton, S. W. Feldberg, J. Electroanal. Chem. 2006, 589,  1.
        | CrossRef |   

[61]   M. R. Moncelli, L. Becucci, F. T. Buoninsegni, R. Guidelli, Biophys. J. 1998, 74,  2388.
        | CrossRef |   

[62]   M. Sano, H. Taube, J. Am. Chem. Soc. 1991, 113,  2327.
        | CrossRef |   

[63]   Kohavi Z., Switching and Finite Automata Theory 1999 (Tata McGraw-Hill: New Delhi).



Rent Article (via Deepdyve) Supplementary MaterialSupplementary Material (233 KB) Export Citation Cited By (6)