Présentation du LADIR > Dynamique du proton dans les solides
 

Dynamique du proton dans les solides

François Fillaux, DR-CNRS

 

Dans les solides l'atome d'hydrogène peut participer à des liaisons chimiques variées. Il peut également exister sous forme isolée, neutre ou ionique. En raison de sa faible masse cet atome peut effectuer des mouvements de grande amplitude qui ne peuvent être décrits dans le cadre de la mécanique quantique qu'avec des outils théoriques appropriés. C'est en raison de ces caractéristiques que l'atome d'hydrogène contribue de façon spécifique à certaines propriétés des solides : liaisons hydrogène, transfert du proton, transitions de phase, conduction protonique, corrélations quantiques...

La spectroscopie de vibration est la seule technique permettant d'observer la dynamique des atomes d'hydrogène dans le régime quantique. De plus, la diffusion des neutrons apporte des informations supplémentaires, inaccessibles avec l'infrarouge ou le Raman.



 Cours du 13 décembre 2004                                                                                                            Contact

 

 Quelques résultats marquants : 


Les corrélations quantiques des protons dans les cristaux

  • Where are protons and deuterons in KHpD1-pCO3? A neutron diffraction study,
    F. Fillaux and A. Cousson, Z. Phys. Chem. 222 (2008) 1279-1290.(pdf)
    Oldenbourg Wissenschaftsverlag, München


  • Nonlocal protons and deuterons opposed to disorder: a single-crystal neutron diffraction study of KH0.76D0.24CO3 and a theoretical framework,
    F. Fillaux and A. Cousson, J. Phys.:Condens. Matter 20 (2008) 252202.(pdf)


  • A neutron diffraction study of macroscopically entangled proton states in the high temperature phase of the KHCO3 crystal at 340 K,
    F. Fillaux, A. Cousson and M. J Gutmann, J. Phys.:Condensed Matter, 20 (2008) 015225. (pdf)


  • Proton tranfer in the KHCO3 and benzoin acid crystals : a quantum view,
    F. Fillaux, J. Mol. Struct. 38, (2007), 308-318.(pdf)


  • Proton transfer across hydrogen bonds: From reaction path to Schrödinger's Cat,
    F. Fillaux, A. Cousson and M. J. Gutmann, Pure Applied Chemistry 79, (2007), 1023-1039.(pdf)


  • Macroscopic quantum tunnelling of protons in the KHCO3 crystal,
    F. Fillaux, A. Cousson, M. J. Gutmann, J. Mol. Struct. 790 (2006) 122-126.(pdf)


  • Macroscopic quantum entanglement and 'super-rigidity' of protons in the KHCO3 crystal from 30 to 300 K
    F. Fillaux, A. Cousson and M. J. Gutmann, J. Phys.: Cond. Matter, 18 (2006) 3229-3249.(pdf)


  • Comment on: "Quantum correlation between protons in potassium bicarbonate" 
    by D. A. Keen and S. W. Lovesey, J. Phys.: Cond. Matter, 15 (2003) 4937-4946. 
    F. Fillaux and A. Cousson, J. Phys.: Cond. Matter, 16 (2004) 1007-1010.(pdf)


  • Observation of the Dynamical Structure Arising from Spatially Extended Quantum Entanglement and Long-Lived Quantum Coherence in the KHCO3 Crystal.
    F. Fillaux, A. Cousson and D. Keen, Phys. Rev. B, 67 (2003) 054301.(pdf)

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  • Incoherent elastic neutron scattering study of the vibrational dynamics and spin-related symmetry of protons in the KHCO3 crystal.
    S. Ikeda and F. Fillaux, Phys. Rev. B, 59 (1999) 4134.(pdf)


  • The Pauli principle and the vibrational dynamics of protons in solids : a new spin related symmetry.
    F. Fillaux, Physica D, 113 (1998) 172.(pdf)


Dynamiques des liaisons hydrogène

  • A neutron scattering study of strong-symmetric hydrogen bonds in potassium and cesium hydrogen bistrifluoroacetates: Determination of the crystal structures and of the single-well potentials for protons.
    F. Fillaux, A. Cousson, J. F. R. Archilla and J. Tomkinson, J. Chem. Phys. 128 (2008), 204502.(pdf)


  • Vibrational Spectroscopy and Quantum Localization, F. Fillaux in Energy Localization and Transfer. Editors T. Dauxois, A. Litvak-Hinenzon, R. MacKay and A. Spanoudaki. Advanced series in nonlinear dynamics, Vol 22 (World Scientific Publishing Co. Pte Ltd., 2004) p.73-148.(pdf)


  • Inelastic neutron scattering study of the localized dynamics of protons in KHCO3 single crystals.
    S. Ikeda, S. Kashida, H. Sugimoto, Y. Yamada, S. M. Bennington and F. Fillaux, Phys. Rev. B, 66 (2002) 184302.(pdf)


  • New proton dynamics in solids revealed by vibrational spectroscopy with neutrons.
    F. Fillaux, J. Mol. Struct., 511-512 (1999) 35.(pdf)


Transferts de protons le long des liaisons hydrogène

  • Extended tunnelling states in the benzoic acid crystal : Infrared and Raman spectra of the OH and OD stretching modes, F. Fillaux, F. Romain, M-H Limage and N. Leygue, Phys. Chem. Chem. Phys., 2006, 4327-4336.(pdf)

 

  • Proton transfer in maloaldehyde : From reaction path to Schrödinger's Cat
    F. Fillaux and B. Nicolaï, Chem. Phys. Letters 415 (2005) 357-361.(pdf)

 

  • Quantum entanglement and nonlocal proton transfer dynamics in dimers of formic acid and analogues.
    F. Fillaux, Chem. Phys. Letters, 408 (2005) 302-306.(pdf)


  • Comment on: 'A symmetric hydrogen bond revisited: potassium hydrogen maleate by variable temperature, variable pressure neutron diffraction and plane-wave DFT methods' [Chem. Phys. Lett. 381 (2003) 102],
    François Fillaux, A. Cousson and J. Tomkinson, Chem. Phys. Lett.,  399 (2004) 2891.(pdf)


  • Quantum proton transfer and orientational disorder in the benzoic acid crystal: vibrational spectra, mechanism and theory.
    F. Fillaux, M. -H. Limage and F. Romain, Chem. Phys., 276 (2002) 181-210.(pdf)


  • The impact of vibrational spectroscopy with neutrons on our view of quantum dynamics in hydrogen bonds and proton transfer.
    F. Fillaux, J. Mol. Struct., 615 (2002) 45-59.(pdf)


  • Hydrogen bonding and quantum dynamics in the solid state.
    F. Fillaux, International Review in Physical Chemistry, 19 (2000) 553.(pdf)


  • Hydrogen bonding. A historical perspective.
    F. Fillaux and J. P. Perchard, J. Chim. Phys., Hors série (2000) 91.


  • Structure and dynamics of the hydrogen bond in potassium hydrogen maleate: a neutron scattering study.
    F. Fillaux, N. Leygue, J. Tomkinson, A. Cousson and W. Paulus, Chem.Phys., 244 (1999) 387.(pdf)

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Effet tunnel rotationnel des groupements méthyles

  • Collective rotational tunnelling of methyl groups and quantum solitons in  4-methylpyridine: Neutron scattering studies of single crystals
    F. Fillaux, B. Nicolaï, W. Paulus, E. Kaiser-Morris and A. Cousson, Phys. Rev. B, 68 (2003) 224301.(pdf)


  • The effect of methyl deuteration on the crystalline structure in Lithium acetate dihydrate
    B. Nicolaï, A. Cousson and F. Fillaux, Chem. Phys., 290 (2003) 101-120.(pdf)


  • Experimental Studies and Theory of Nonlinear Rotational Dynamics in the Quantum Regime: the Interplay of Structure, Dynamics and Localization in Crystals.
    F. Fillaux, B. Nicolaï and A. Cousson (World Scientific, Publishing Co., Inc, 2003).(pdf)


  • Collective Rotational Tunnelling and Quantum sine-Gordon Solitons.
    F. Fillaux, (World Scientific, Publishing Co., Inc, 2003).(pdf)


  • Structure of manganese diacetate tetrahydrate and low-temperature methyl-group dynamics.
    B. Nicolaï, G. J. Kearley, A. Cousson, W. Paulus, F. Fillaux, F. Gentner, L. Schröder, and D. Watkin, Acta Cryst. B57 (2001) 36.


  • Crystal structure and low-temperature methyl-group dynamics of cobalt and nickel acetates.
    B. Nicolaï, G. J. Kearley, M. R. Johnson, F. Fillaux and E. Suard, J.Chem.Phys., 109 (1998) 9062.(pdf)


  • Inelastic neutron-scattering study of the sine-Gordon breather interactions in isotopic mixtures of 4-methyle-pyridine.
    F. Fillaux, C. J. Carlile and G. J. Kearley, Phys.Rev.B, 58 (1998) 11416.(pdf)


  • Inelastic neutron scattering study of methyl tunnelling in an oriented single-crystal of 2,6-dimethylpyrazine at low temperature and rotational potential calculations.
    B. Nicolaï, E. Kaiser, F. Fillaux, G. J. Kearley, A. Cousson and W. Paulus, Chem.Phys., 226 (1998) 1.(pdf)


Protons libres et conduction protonique

  • Inelastic neutron scattering studies of polypyrroles and partially deuterated analogues.
    F. Fillaux, S. F. Parker and L. T. Yu, Solid State Ionics, 14 (2001) 451-57.(pdf)


  • Inelastic neutron scattering study of the proton dynamics in Bi-dopped manganese oxides.
    F. Fillaux, C. Cachet, S. F. Parker, J. Tomkinson, A. Quivy, and L. T. Yu, J. Electrochem. Soc., 147 (2000) 4184.


  • New proton dynamics in solids revealed by vibrational spectroscopy with neutrons.
    F. Fillaux, Solid State Ionics, 125 (1999) 69.(pdf)


  • Inelastic neutron scattering study of the proton dynamics in HNO3 graphite intercalation compounds.
    F. Fillaux, S. Menu, J. Conard, H. Fuzellier, S. F. Parker, A. C. Hanon and J. Tomkinson, Chem.Phys., 242 (1999) 273.(pdf)


  • Inelastic neutron scattering studies of polyanilines and partially deuterated analogues.
    F. Fillaux, N. Leygue, R. Baddour-Hadjean, S. F. Parker, Ph. Colomban, A. Gruger, A. Régis and L.T.Yu, Chem.Phys., 216 (1997) 281.(pdf)


  • Inelastic neutron-scattering study of free proton dynamics in γ-MnO2.
    F. Fillaux, S. M. Bennington, J. Tomkinson and L. T. Yu, Chem.Phys., 209 (1996) 111.(pdf)

 

 

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