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Polarizability of molecular clusters as calculated by a dipole interaction model

J. Chem. Phys. 116, 4001 (2002); doi:10.1063/1.1433747

Issue Date: 8 March 2002

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Lasse Jensen
Theoretical Chemistry, Material Science Centre, Rijksuniversiteit Groningen, Nijenborgh 4, 9747 AG Groningen, The Netherlands

Per-Olof Åstrand
Materials Research Department, Risø National Laboratory, DK-4000 Roskilde, Denmark
Department of Chemistry, H. C. Ørsted Institute, University of Copenhagen, DK-2100 Copenhagen Ø, Denmark

Anders Osted, Jacob Kongsted, and Kurt V. Mikkelsen
Department of Chemistry, H. C. Ørsted Institute, University of Copenhagen, DK-2100 Copenhagen Ø, Denmark
We have developed and investigated a dipole interaction model for calculating the polarizability of molecular clusters. The model has been parametrized from the frequency-dependent molecular polarizability as obtained from quantum chemical calculations for a series of 184 aliphatic, aromatic, and heterocyclic compounds. A damping of the interatomic interaction at short distances is introduced in such a way as to retain a traceless interaction tensor and a good description of the damping over a wide range of interatomic distances. By adopting atomic polarizabilities in addition to atom-type parameters describing the damping and the frequency dependence, respectively, the model is found to reproduce the molecular frequency-dependent polarizability tensor calculated with ab initio methods. A study of the polarizability of four dimers has been carried out: the hydrogen fluoride, methane, benzene, and urea dimers. We find in general good agreement between the model and the quantum chemical results over a wide range of intermolecular distances. To demonstrate the power of the model, the polarizability has been calculated for a linear chain of urea molecules with up to 300 molecules and one- and two-dimensional clusters of C60 with up to 25 molecules. Substantial intermolecular contributions are found for the polarizability anisotropy, whereas the effects are small for the mean polarizability. For the mean polarizability of C60, we find good agreement between the model and experiments both in the case of an isolated molecule and in a comparison of a planar cluster of 25 C60 molecules with experimental results on thin films. ©2002 American Institute of Physics.
History: Received 20 June 2001; accepted 15 November 2001
Permalink: http://link.aip.org/link/?JCPSA6/116/4001/1
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KEYWORDS and PACS

Keywords
PACS
  • 36.40.Cg
    Exotic atoms and molecules; macromolecules; clusters Atomic and molecular clusters Electronic and magnetic properties of clusters
  • 36.40.Sx
    Exotic atoms and molecules; macromolecules; clusters Atomic and molecular clusters Diffusion and dynamics of clusters
  • 33.15.Kr
    Molecular properties and interactions with photons Properties of molecules Electric and magnetic moments (and derivatives), polarizability, and magnetic susceptibility
  • 31.15.Ar
    Electronic structure of atoms and molecules: theory Calculations and mathematical techniques in atomic and molecular physics (excluding electron correlation calculations) Ab initio calculations
  • 33.15.Dj
    Molecular properties and interactions with photons Properties of molecules Interatomic distances and angles
  • 34.20.Gj
    Atomic and molecular collision processes and interactions Interatomic and intermolecular potentials and forces, potential energy surfaces for collisions Intermolecular and atom–molecule potentials and forces
  • YEAR: 2002

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0021-9606 (print)   1089-7690 (online)
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REFERENCES (83)
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For access to fully linked references, you need to log in. For access to fully linked references, you need to Log in.
  1. P. N. Prasad and D. J. Williams, Introduction to Nonlinear Optical Effects in Molecules and Polymers (Wiley, New York, 1991).
  2. P. Ball, Made to Measure, New Materials for the 21st Century (Princeton University Press, Princeton, NJ, 1997).
  3. Molecular Electronics, edited by J. Jortner and M. Ratner (Blackwell Science, Oxford, 1997).
  4. D. P. Shelton and J. E. Rice, Chem. Rev. 94, 3 (1994).
  5. D. R. Kanis, M. A. Ratner, and T. J. Marks, Chem. Rev. 94, 195 (1994).
  6. D. M. Bishop, Adv. Quantum Chem. 25, 1 (1994).
  7. Y. Luo, H. Ågren, P. Jørgensen, and K. V. Mikkelsen, Adv. Quantum Chem. 26, 165 (1995).
  8. I. D. L. Albert, T. J. Marks, and M. A. Ratner, J. Phys. Chem. 100, 9714 (1996).
  9. S. P. Karna, J. Phys. Chem. A 104, 4671 (2000).
  10. J. Olsen and P. Jørgensen, J. Chem. Phys. 82, 3235 (1985).
  11. B. Champagne, E. A. Perpéte, S. J. A. van Gisbergen, E.-J. Baerends, J. G. Snijders, C. Soubra-Ghaoui, K. A. Robins, and B. Kirtman, J. Chem. Phys. 109, 10489 (1998).
  12. S. J. A. van Gisbergen, P. R. T. Schipper, O. V. Gritsenko, E. J. Baerends, J. G. Snijders, B. Champagne, and B. Kirtman, Phys. Rev. Lett. 83, 694 (1999).
  13. L. Silberstein, Philos. Mag. 33, 92 (1917).
  14. K. G. Denbigh, Trans. Faraday Soc. 36, 936 (1940).
  15. B. C. Vickery and K. G. Denbigh, Trans. Faraday Soc. 45, 61 (1949).
  16. K. J. Miller and J. A. Savchik, J. Am. Chem. Soc. 101, 7206 (1979).
  17. Y. K. Kang and M. S. Jhon, Theor. Chim. Acta 61, 41 (1982).
  18. K. J. Miller, J. Am. Chem. Soc. 112, 8533 (1990).
  19. J. M. Stout and C. E. Dykstra, J. Am. Chem. Soc. 117, 5127 (1995).
  20. J. M. Stout and C. E. Dykstra, J. Phys. Chem. A 102, 1576 (1998).
  21. K. O. Sylvester-Hvid, P.-O. Åstrand, M. A. Ratner, and K. V. Mikkelsen, J. Phys. Chem. A 103, 1818 (1999).
  22. J. Applequist, J. R. Carl, and K. F. Fung, J. Am. Chem. Soc. 94, 2952 (1972).
  23. J. Applequist, Acc. Chem. Res. 10, 79 (1977).
  24. K. A. Bode and J. Applequist, J. Phys. Chem. 100, 17820 (1996).
  25. L. Silberstein, Philos. Mag. 33, 215 (1917).
  26. L. Silberstein, Philos. Mag. 33, 521 (1917).
  27. R. R. Birge, J. Chem. Phys. 72, 5312 (1980).
  28. B. T. Thole, Chem. Phys. 59, 341 (1981).
  29. R. R. Birge, G. A. Schick, and D. F. Bocian, J. Chem. Phys. 79, 2256 (1983).
  30. A. H. de Vries, P. T. van Duijnen, R. W. J. Zijlstra, and M. Swart, J. Electron Spectrosc. Relat. Phenom. 86, 49 (1997).
  31. P. T. van Duijnen and M. Swart, J. Phys. Chem. 102, 2399 (1998).
  32. A. A. Chialvo and P. T. Cummings, Fluid Phase Equilib. 150-151, 73 (1998).
  33. C. J. Burnham, J. Li, S. S. Xantheas, and M. Leslie, J. Chem. Phys. 110, 4566 (1999).
  34. L. Jensen, P.-O. Åstrand, K. O. Sylvester-Hvid, and K. V. Mikkelsen, J. Phys. Chem. A 104, 1563 (2000).
  35. L. Jensen, O. H. Schmidt, K. V. Mikkelsen, and P.-O. Åstrand, J. Phys. Chem. B 104, 10462 (2000).
  36. D. M. Bishop, Rev. Mod. Phys. 62, 343 (1990).
  37. D. M. Bishop, Adv. Chem. Phys. 104, 1 (1998).
  38. B. Champagne, Int. J. Quantum Chem. 65, 689 (1997).
  39. J. Kongsted, A. Osted, L. Jensen, P.-O. Åstrand, and K. V. Mikkelsen, J. Phys. Chem. B 105, 10243 (2001).
  40. A. D. Buckingham, Adv. Chem. Phys. 12, 107 (1967).
  41. A. D. Buckingham, E. P. Concannon, and I. D. Hands, J. Phys. Chem. 98, 10455 (1994).
  42. M. J. Gunning and R. E. Raab, Mol. Phys. 91, 589 (1997).
  43. S. F. Boys, Proc. R. Soc. London 200, 542 (1950).
  44. T. Helgaker, P. Jørgensen, and J. Olsen, Molecular Electronic-Structure Theory (Wiley, Chichester, 2000).
  45. G. A. van der Velde, CECAM Workshop Report, 1972, edited by H. J. C. Berendsen.
  46. T. Helgaker, H. J. Aa. Jensen, P. Jørgensen et al., DALTON, an electronic structure program, Release 1.0 http://www.kjemi.uio.no/software/dalton, 1997.
  47. H. J. Aa. Jensen, H. Koch, P. Jørgensen, and J. Olsen, Chem. Phys. 119, 297 (1988).
  48. H. J. Aa. Jensen, P. Jørgensen, and J. Olsen, J. Chem. Phys. 89, 3654 (1988).
  49. A. J. Sadlej, Collect. Czech. Chem. Commun. 53, 1995 (1988).
  50. The 74 molecules are: borazine, 1,2-dichloro-borazine, 2,4-dichloro-borazine, 1,2-difluoro-borazine, 1,4-difluoro-borazine, 2,4-difluoro-borazine, 1-amino-4-nitro-borazine, 2-amino-1-nitro-borazine, 2-amino-4-nitro-borazine, 4-amino-1-nitro-borazine, 1,3,5-triborane, 1,3-difluoro-1,3,5-triborane, 1-amino-3-nitro-1,3,5-triborane, 2-amino-4-nitro-1,3,5-triborane, cis-2,4-dichloro-1,3,5-triborane, cis-2,4-difluoro-1,3,5-triborane, trans-2,4-dichloro-1,3,5-triborane, trans-2,4-difluoro-1,3,5-triborane, 1,2-dichloro-1,3,5-triborane, 1,2-difluoro-1,3,5-triborane, 1-amino-2-nitro-1,3,5-triborane, 1,4-dichloro-1,3,5-triborane, 1,4-difluoro-1,3,5-triborane, 1-nitro-2-amino-1,3,5-triborane, 1-nitro-4-amino-1,3,5-triborane, 1-amino-4-nitro-1,3,5-triborane, hexahydro-1,3,5-triazine, 1,3-dichloro-tetrahydro-1,3,5-triazine, 1,3-difluoro-tetrahydro-1,3,5-triazine, 2-amino-4-nitro-tetrahydro-1,3,5-triazine, cis-2,4-dichloro-tetrahydro-1,3,5-triazine, cis-2,4-difluoro-tetrahydro-1,3,5-triazine, trans-2,4-dichloro-tetrahydro-1,3,5-triazine, trans-2,4-difluoro-tetrahydro-1,3,5-triazine, 1,2-dichloro-tetrahydro-1,3,5-triazine, 1-amino-2-nitro-tetrahydro-1,3,5-triazine, 2-amino-1-nitro-tetrahydro-1,3,5-triazine, 1,4-dichloro-tetrahydro-1,3,5-triazine, 1-amino-4-nitro-tetrahydro-1,3,5-triazine, 4-amino-1-nitro-tetrahydro-1,3,5-triazine, hexahydro-1,4-dibora-2,5-diazine, 1,3-dichloro-tetrahydro-1,4-dibora-2,5-diazine, 1,5-dichloro-tetrahydro-1,4-dibora-2,5-diazine, 3,5-dichloro-tetrahydro-1,4-dibora-2,5-diazine, 1,3-difluoro-tetrahydro-1,4-dibora-2,5-diazine, 1,5-difluoro-tetrahydro-1,4-dibora-2,5-diazine, 3,5-difluoro-tetrahydro-1,4-dibora-2,5-diazine, 1-amino-3-nitro-tetrahydro-1,4-dibora-2,5-diazine, 3-amino-1-nitro-tetrahydro-1,4-dibora-2,5-diazine, 1-amino-5-nitro-tetrahydro-1,4-dibora-2,5-diazine, 4-amino-2-nitro-tetrahydro-1,4-dibora-2,5-diazine, 2-amino-6-nitro-tetrahydro-1,4-dibora-2,5-diazine, 3-amino-5-nitro-tetrahydro-1,4-dibora-2,5-diazine, 1,2-dichloro-tetrahydro-1,4-dibora-2,5-diazine, 1,6-dichloro-tetrahydro-1,4-dibora-2,5-diazine, 1,2-difluoro-tetrahydro-1,4-dibora-2,5-diazine, 1,6-difluoro-tetrahydro-1,4-dibora-2,5-diazine, 2,3-difluoro-tetrahydro-1,4-dibora-2,5-diazine, 1-amino-2-nitro-tetrahydro-1,4-dibora-2,5-diazine, 1-amino-6-nitro-tetrahydro-1,4-dibora-2,5-diazine, 2-amino-1-nitro-tetrahydro-1,4-dibora-2,5-diazine, 3-amino-2-nitro-tetrahydro-1,4-dibora-2,5-diazine, 3-amino-4-nitro-tetrahydro-1,4-dibora-2,5-diazine, 1,4-dichloro-tetrahydro-1,4-dibora-2,5-diazine, 2,5-dichloro-tetrahydro-1,4-dibora-2,5-diazine, cis-3,6-dichloro-tetrahydro-1,4-dibora-2,5-diazine, trans-3,6-dichloro-tetrahydro-1,4-dibora-2,5-diazine, 1,4-difluoro-tetrahydro-1,4-dibora-2,5-diazine, 2,5-difluoro-tetrahydro-1,4-dibora-2,5-diazine, cis-3,6-difluoro-tetrahydro-1,4-dibora-2,5-diazine, trans-3,6-difluoro-tetrahydro-1,4-dibora-2,5-diazine, 2-amino-5-nitro-tetrahydro-1,4-dibora-2,5-diazine, trans-3-amino-6-nitro-tetrahydro-1,4-dibora-2,5-diazine, 3-nitro-2-amino-tetrahydro-1,4-dibora-2,5-diazine.
  51. IUPAC, Nomenclature of Organic Chemistry. Sections A, B, C, D, E, F and H (Pergamon, Oxford, 1979).
  52. M. J. Frisch, G. W. Trucks, H. B. Schlegel et al., GAUSSIAN 94, Revision B.3, Gaussian, Inc., Pittsburgh, PA, 1995.
  53. Handbook of Chemistry and Physics, edited by R. C. Weast, 62nd ed. (CRC Press, Boca Raton, FL, 1981).
  54. J. A. Pople and M. Gordon, J. Am. Chem. Soc. 89, 4253 (1967).
  55. M. L. Olson and K. R. Sundberg, J. Chem. Phys. 69, 5400 (1978).
  56. J. Applequist, J. Phys. Chem. 97, 6016 (1993).
  57. L. Jensen, P.-O. Åstrand, and K. V. Mikkelsen, Int. J. Quantum Chem. 84, 513 (2001).
  58. J. Applequist and C. O. Quicksall, J. Chem. Phys. 66, 3455 (1977).
  59. S. F. Boys and F. Bernardi, Mol. Phys. 19, 553 (1970).
  60. E. R. Andrew and D. Hyndman, Discuss. Faraday Soc. 19, 195 (1955).
  61. P.-O. Åstrand, A. Wallqvist, and G. Karlström, J. Chem. Phys. 100, 1262 (1994).
  62. P. A. Heiney, J. E. Fischer, A. R. McGhie, W. J. Romanow, A. M. Denenstein, J. P. McCauley, Jr., A. B. Smith III, and D. E. Cox, Phys. Rev. Lett. 66, 2911 (1991).
  63. D. M. Bishop and M. Dupuis, Mol. Phys. 88, 887 (1996).
  64. C. E. Dykstra and S.-Y. Liu, J. Mol. Struct.: THEOCHEM 135, 357 (1986).
  65. J. D. Augspurger and C. E. Dykstra, Int. J. Quantum Chem. 43, 135 (1992).
  66. M. Nakano, S. Yamada, S. Kiribayashi, and K. Yamaguchi, Synth. Met. 102, 1542 (1999).
  67. G. Maroulis, J. Chem. Phys. 113, 1813 (2000).
  68. J. Perez and M. Dupuis, J. Phys. Chem. 95, 6525 (1991).
  69. S. Chen and H. A. Kurtz, J. Mol. Struct.: THEOCHEM 388, 79 (1996).
  70. B. Kirtman, C. E. Dykstra, and B. Champagne, Chem. Phys. Lett. 305, 132 (1999).
  71. E. K. Dalskov, J. Oddershede, and D. M. Bishop, J. Chem. Phys. 108, 2152 (1998).
  72. R. Antoine, Ph. Dugourd, D. Rayane, E. Benichou, F. Chandezon, M. Broyer, and C. Guet, J. Chem. Phys. 110, 9771 (1999).
  73. K. Ruud, D. Jonsson, and P. R. Taylor, J. Chem. Phys. 114, 4331 (2001).
  74. W. Krätschmer, L. D. Lamb, K. Fostiropoulos, and D. R. Huffman, Nature (London) 347, 354 (1990).
  75. A. F. Hebard, R. C. Haddon, R. M. Fleming, and A. R. Kortan, Appl. Phys. Lett. 59, 2109 (1991).
  76. Z. H. Kafafi, J. R. Lindle, R. G. S. Pong, F. J. Bartoli, L. J. Lingg, and J. Milliken, Chem. Phys. Lett. 188, 492 (1992).
  77. S. L. Ren, K. A. Wang, P. Zhou, Y. Wang, A. M. Rao, M. S. Meier, J. P. Selegue, and P. C. Eklund, Appl. Phys. Lett. 61, 124 (1992).
  78. A. Ritcher and J. Sturm, Appl. Phys. A: Mater. Sci. Process. 61, 163 (1995).
  79. P. C. Eklund, A. M. Rao, Y. Wang, K. A. Zhou, P. Wang, J. M. Holden, M. S. Dresselhaus, and G. Dresselhaus, Thin Solid Films 257, 211 (1995).
  80. M. P. Hodges, A. J. Stone, and E. C. Lago, J. Phys. Chem. A 102, 2455 (1998).
  81. R. L. Rowley and T. Pakkanen, J. Chem. Phys. 110, 3368 (1999).
  82. R. L. Jaffe and G. D. Smith, J. Chem. Phys. 105, 2780 (1996).
  83. See EPAPS Document No. E-JCPSA6-116-518206 for Cartesian coordinates and quantum chemical molecular polarizability tensors for the 184 aliphatic, aromatic and heterocyclic compounds used as training set. This document may be retrieved via the EPAPS homepage (http://www.aip.org/pubservs/epaps.html) or from ftp.aip.org in the directory /epaps/. See the EPAPS homepage for more information. [EPAPS]

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