Simulation of mesogenic diruthenium tetracarboxylates: Development of a force field for coordination polymers of the MMX type

A classical molecular mechanics force field, able to simulate coordination polymers (CP) based on ruthenium carboxylates (Ru2(O2CReq)4Lax) (eq = equatorial group containing aliphatic chains, Lax= axial ligand), has been developed. New parameters extracted from experimental data and quantum calculations on short aliphatic chains model systems were included in the generalized AMBER force field. The proposed parametrization was evaluated using model systems with known structure, containing either short or long aliphatic chains; experimental results were reproduced satisfactorily. This modified force field, although in a preliminary stage, could then be applied to long chain liquid crystalline compounds. The resulting atomistic simulations allowed assessing the relative influence of the factors determining the CP conformation, determinant for the physical properties of these materials. © 2013 Wiley Periodicals, Inc.

[1]  D. Guillon,et al.  Liquid-crystalline materials based on rhodium carboxylate coordination polymers: Synthesis, characterization and mesomorphic properties of tetra(alkoxybenzoato)dirhodium(II) complexes and their pyrazine adducts , 2002 .

[2]  M. Handa,et al.  Magnetic interactions in one-, two-, and three-dimensional assemblies of dinuclear ruthenium carboxylates , 2006 .

[3]  J. Gómez‐Herrero,et al.  Time-dependence structures of coordination network wires in solution. , 2008, ACS nano.

[4]  R. Clark,et al.  RESONANCE RAMAN, EXCITATION PROFILE AND ELECTRONIC STRUCTURAL STUDIES OF DIRUTHENIUM TETRACARBOXYLATE COMPLEXES , 1981 .

[5]  C. Massobrio,et al.  Advances in the Atomic-Scale Modeling of Nanosystems and Nanostructured Materials , 2010 .

[6]  P. Maldivi,et al.  Structural study of crystalline and columnar copper (II) soaps , 1992 .

[7]  R. Swendsen,et al.  THE weighted histogram analysis method for free‐energy calculations on biomolecules. I. The method , 1992 .

[8]  A. Becke.  A New Mixing of Hartree-Fock and Local Density-Functional Theories , 1993 .

[9]  E. Sileo,et al.  Thermal stability of mixed-valent diruthenium (II,III) carboxylates , 2003 .

[10]  A. Calzolari,et al.  Highly conductive self-assembled nanoribbons of coordination polymers. , 2010, Nature nanotechnology.

[11]  P. Maldivi,et al.  Columnar liquid crystals derived from long-chain carboxylates of transition metal ions , 1990, Philosophical Transactions of the Royal Society of London. Series A, Mathematical and Physical Sciences.

[12]  G. Torrie,et al.  Monte Carlo free energy estimates using non-Boltzmann sampling: Application to the sub-critical Lennard-Jones fluid , 1974 .

[13]  Kenneth M Merz,et al.  Structural Survey of Zinc Containing Proteins and the Development of the Zinc AMBER Force Field (ZAFF). , 2010, Journal of chemical theory and computation.

[14]  P. Strevens.  Iii , 1985 .

[15]  J. Perdew,et al.  Density-functional approximation for the correlation energy of the inhomogeneous electron gas. , 1986, Physical review. B, Condensed matter.

[16]  Y. Kitagawa,et al.  Theoretical studies on relation among structures, electric structures and magnetic interactions in MMX complexes , 2007 .

[17]  R. Templer,et al.  Copper(II) pentacosadiynoate: a discotic mesogen with unusual liquid-crystalline and solid-state ultrastructures , 1993 .

[18]  Masahiro Yamamoto,et al.  Charge Ordering with Lattice Distortions in a Conductive MMX-Chain Complex, Pt2(dta)4I (dta = CH3CS2-) , 1999 .

[19]  G. G. Stokes.  "J." , 1890, The New Yale Book of Quotations.

[20]  B. Heinrich,et al.  Supramolecular architecture elucidation of the room temperature columnar mesophases exhibited by mixed-valent diruthenium alkoxybenzoates , 2009 .

[21]  P. Maldivi,et al.  Mixed-Valent Diruthenium Long-Chain Carboxylates. 2. Magnetic Properties. , 1998, Inorganic chemistry.

[22]  J. Warman,et al.  Discotic Liquid Crystalline Semiconductors , 2003 .

[23]  Xiaozhen Yang,et al.  SPECTROSCOPIC CHARACTERIZATION OF MESOGEN ORDER IN DISCOTIC LIQUID-CRYSTAL , 1988 .

[24]  M. A. Aquino.  Diruthenium and diosmium tetracarboxylates: synthesis, physical properties and applications , 1998 .

[25]  W. R. Wadt,et al.  Ab initio effective core potentials for molecular calculations. Potentials for K to Au including the outermost core orbitals , 1985 .

[26]  H. Kitagawa,et al.  On the nature of the multiple ground states of the MMX mixed-valence chain compound, [Pt(II/III)2(n-PenCS2)4I]∞. , 2011, Inorganic chemistry.

[27]  B. Heinrich,et al.  Lyotropic Behavior of Diruthenium(II,III) Alkoxybenzoates in Dodecane , 2002 .

[28]  P. Maldivi,et al.  Side chain influence on mesomorphic properties: Low‐temperature melting of metal‐containing liquid crystals , 1993 .

[29]  O. Francescangeli,et al.  A2[MX4] Copper(II) Pyridinium Salts. From Ionic Liquids to Layered Solids to Liquid Crystals , 2001 .

[30]  J. Serrano,et al.  Silver pyrazolates as coordination-polymer luminescent metallomesogens. , 2010, Chemistry.

[31]  D. Guillon,et al.  Molecular Dynamics Simulations of Liquid-Crystalline Dendritic Architectures , 2010 .

[32]  R. Lemieux,et al.  Evidence for room temperature mesomorphism in a mixed-valent diruthenium(II,III) quintapalmitoleate polymer , 1998 .

[33]  W. R. Wadt,et al.  Ab initio effective core potentials for molecular calculations. Potentials for main group elements Na to Bi , 1985 .

[34]  W. R. Wadt,et al.  Ab initio effective core potentials for molecular calculations , 1984 .

[35]  Thomas J. Meyer,et al.  Comprehensive Coordination Chemistry II , 2004 .

[36]  F. Lelj,et al.  Atomistic simulation of discotic liquid crystals: transition from isotropic to columnar phase example. , 2007, The Journal of chemical physics.

[37]  Peter A. Kollman,et al.  Application of the RESP Methodology in the Parametrization of Organic Solvents , 1998 .

[38]  P. Maldivi,et al.  Mixed-Valent Diruthenium (II,III) Long-Chain Carboxylates. 1. Molecular Design of Columnar Liquid-Crystalline Order , 1998 .

[39]  N. Kimizuka,et al.  Controlled polymerization and self-assembly of halogen-bridged diruthenium complexes in organic media and their dielectrophoretic alignment. , 2012, Journal of the American Chemical Society.

[40]  Philip A. Gale,et al.  Supramolecular Chemistry: From Molecules to Nanomaterials , 2012 .

[41]  Colin Eaborn,et al.  Comprehensive Coordination Chemistry , 1988 .

[42]  Norman L. Allinger,et al.  Molecular mechanics parameters , 1994 .

[43]  Parr,et al.  Development of the Colle-Salvetti correlation-energy formula into a functional of the electron density. , 1988, Physical review. B, Condensed matter.

[44]  V. Miskowski,et al.  Electronic and vibrational spectra of Ru2(carboxylate)4+ complexes. Characterization of a high-spin metal-metal ground state , 1987 .

[45]  A. Becke.  A multicenter numerical integration scheme for polyatomic molecules , 1988 .

[46]  A. Roitberg,et al.  Theoretical and experimental studies of diruthenium tetracarboxylates structure, spectroscopy, and electrochemistry. , 2008, Inorganic chemistry.

[47]  J. Serrano,et al.  Rectangular and hexagonal columnar mesophases in dinuclear rhodium (II) (alkyloxy)benzoate complexes , 1992 .