Structured water in polyelectrolyte dendrimers: Understanding small angle neutron scattering results through atomistic simulation

Wu, Bin; Kerkeni, Boutheïna; Egami, Takeshi; Do, Changwoo; Liu, Yun; Wang, Yongmei; Porcar, Lionel; Hong, Kunlun; Smith, Sean C.; Liu, Emily L.; Smith, Gregory S.; Chen, Wei-Ren

doi:10.1063/1.3697479

Structured water in polyelectrolyte dendrimers: Understanding small angle neutron scattering results through atomistic simulation

Journal Article · Sat Apr 14 04:00:00 EDT 2012 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.3697479· OSTI ID:1042880

Wu, Bin; Kerkeni, Boutheïna; Egami, Takeshi; Do, Changwoo; Liu, Yun; Wang, Yongmei; Porcar, Lionel; Hong, Kunlun; Smith, Sean C.; Liu, Emily L.; Smith, Gregory S.; Chen, Wei-Ren

Based on atomistic molecular dynamics (MD) simulations, the small angle neutron scattering (SANS) intensity behavior of a single generation-4 (G4) polyelectrolyte polyamidoamine (PAMAM) starburst dendrimer is investigated at different levels of molecular protonation. The SANS form factor, P(Q), and Debye autocorrelation function, γ(r), are calculated from the equilibrium MD trajectory based on a mathematical approach proposed in this work which provides a link between the neutron scattering experiment and MD computation. The simulations enable scattering calculations of not only the hydrocarbons, but also the contribution to the scattering length density fluctuations caused by structured, confined water within the dendrimer. Based on our computational results, we question the validity of using radius of gyration RG for microstructure characterization of a polyelectrolyte dendrimer from the scattering perspective.

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-00OR22725

OSTI ID:: 1042880

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 14 Vol. 136; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)

Country of Publication:: United States

Language:: English

References (59)

Dynamics and Structure of Hydration Water on Rutile and Cassiterite Nanopowders Studied by Quasielastic Neutron Scattering and Molecular Dynamics Simulations Mamontov, E.; Vlcek, L.; Wesolowski, D. J. The Journal of Physical Chemistry C, Vol. 111, Issue 11 https://doi.org/10.1021/jp067242r	journal	February 2007
Automatic atom type and bond type perception in molecular mechanical calculations Wang, Junmei; Wang, Wei; Kollman, Peter A. Journal of Molecular Graphics and Modelling, Vol. 25, Issue 2 https://doi.org/10.1016/j.jmgm.2005.12.005	journal	October 2006
A modified TIP3P water potential for simulation with Ewald summation Price, Daniel J.; Brooks, Charles L. The Journal of Chemical Physics, Vol. 121, Issue 20 https://doi.org/10.1063/1.1808117	journal	November 2004
Intramolecular Structural Change of PAMAM Dendrimers in Aqueous Solutions Revealed by Small-Angle Neutron Scattering Porcar, Lionel; Hong, Kunlun; Butler, Paul D. The Journal of Physical Chemistry B, Vol. 114, Issue 5 https://doi.org/10.1021/jp9064455	journal	February 2010
Effect of counterion valence on the pH responsiveness of polyamidoamine dendrimer structure Liu, Yun; Porcar, Lionel; Hong, Kunlun The Journal of Chemical Physics, Vol. 132, Issue 12 https://doi.org/10.1063/1.3358349	journal	March 2010
VMD: Visual molecular dynamics Humphrey, William; Dalke, Andrew; Schulten, Klaus Journal of Molecular Graphics, Vol. 14, Issue 1 https://doi.org/10.1016/0263-7855(96)00018-5	journal	February 1996
Quantum and statistical mechanical studies of liquids. 10. Transferable intermolecular potential functions for water, alcohols, and ethers. Application to liquid water Jorgensen, William L. Journal of the American Chemical Society, Vol. 103, Issue 2 https://doi.org/10.1021/ja00392a016	journal	January 1981
Effect of physical state (solid vs. liquid) of lipid core on the rate of transport of oxygen and free radicals in solid lipid nanoparticles and emulsion Tikekar, Rohan V.; Nitin, N. Soft Matter, Vol. 7, Issue 18 https://doi.org/10.1039/c1sm05031a	journal	January 2011
Properties of Dendrimers with Flexible Spacer-Chains: A Monte Carlo Study Kłos, J. S.; Sommer, J. -U. Macromolecules, Vol. 42, Issue 13 https://doi.org/10.1021/ma900479y	journal	July 2009
Conformations of high-generation dendritic polyelectrolytes Huißmann, Sebastian; Likos, Christos N.; Blaak, Ronald Journal of Materials Chemistry, Vol. 20, Issue 46 https://doi.org/10.1039/c0jm01584a	journal	January 2010
Integral expressions of the derivatives of the small‐angle scattering correlation function Ciccariello, S. Journal of Mathematical Physics, Vol. 36, Issue 1 https://doi.org/10.1063/1.531303	journal	January 1995
The effects of pH, salt and bond stiffness on charged dendrimers Huißmann, Sebastian; Wynveen, Aaron; Likos, Christos N. Journal of Physics: Condensed Matter, Vol. 22, Issue 23 https://doi.org/10.1088/0953-8984/22/23/232101	journal	April 2010
Self-Organization in Dendrimer Polyelectrolytes Karatasos, K. Macromolecules, Vol. 41, Issue 3 https://doi.org/10.1021/ma7019489	journal	February 2008
Molecular Dynamics Studies of the Size, Shape, and Internal Structure of 0% and 90% Acetylated Fifth-Generation Polyamidoamine Dendrimers in Water and Methanol Lee, Hwankyu; Baker,, James R.; Larson, Ronald G. The Journal of Physical Chemistry B, Vol. 110, Issue 9 https://doi.org/10.1021/jp056148s	journal	March 2006
Computer Simulation of the Dynamics of Neutral and Charged Dendrimers Lyulin, Sergey V.; Darinskii, Anatolij A.; Lyulin, Alexey V. Macromolecules, Vol. 37, Issue 12 https://doi.org/10.1021/ma0357927	journal	June 2004
Experimental Study of Solvation Forces Horn, R. G.; Ninham, B. W. Micellar Solutions and Microemulsions https://doi.org/10.1007/978-1-4613-8938-5_5	book	January 1990
Structure and Dynamics of DNA−Dendrimer Complexation: Role of Counterions, Water, and Base Pair Sequence Maiti, Prabal K.; Bagchi, Biman Nano Letters, Vol. 6, Issue 11 https://doi.org/10.1021/nl061609m	journal	November 2006
Small Angle Neutron Scattering Studies of the Structure and Interaction in Micellar and Microemulsion Systems Chen, S. H. Annual Review of Physical Chemistry, Vol. 37, Issue 1 https://doi.org/10.1146/annurev.pc.37.100186.002031	journal	October 1986
Effects of PEGylation on the Size and Internal Structure of Dendrimers: Self-Penetration of Long PEG Chains into the Dendrimer Core Lee, Hwankyu; Larson, Ronald G. Macromolecules, Vol. 44, Issue 7 https://doi.org/10.1021/ma102482u	journal	April 2011
Designing dendrimers for biological applications Lee, Cameron C.; MacKay, John A.; Fréchet, Jean M. J. Nature Biotechnology, Vol. 23, Issue 12 https://doi.org/10.1038/nbt1171	journal	December 2005
Direct measurement of temperature-dependent solvation forces between DNA double helices Rau, D. C.; Parsegian, V. A. Biophysical Journal, Vol. 61, Issue 1 https://doi.org/10.1016/S0006-3495(92)81832-5	journal	January 1992
Assess the Intramolecular Cavity of a PAMAM Dendrimer in Aqueous Solution by Small-Angle Neutron Scattering Li, Tianfu; Hong, Kunlun; Porcar, Lionel Macromolecules, Vol. 41, Issue 22 https://doi.org/10.1021/ma801555j	journal	November 2008
A smooth particle mesh Ewald method Essmann, Ulrich; Perera, Lalith; Berkowitz, Max L. The Journal of Chemical Physics, Vol. 103, Issue 19 https://doi.org/10.1063/1.470117	journal	November 1995
Simulation of a Symmetric Binary Mixture of Charged Dendrimers Under Varying Electrostatic Interactions: Static and Dynamic Aspects Karatasos, K.; Tanis, I. Macromolecules, Vol. 44, Issue 16 https://doi.org/10.1021/ma2013282	journal	August 2011
Direct measurement of forces between linear polysaccharides xanthan and schizophyllan Rau, D.; Parsegian, V. Science, Vol. 249, Issue 4974 https://doi.org/10.1126/science.2144663	journal	September 1990
Are Polyelectrolyte Dendrimers Stimuli Responsive? Giupponi, Giovanni; Buzza, D. Martin A.; Adolf, Dave B. Macromolecules, Vol. 40, Issue 16 https://doi.org/10.1021/ma070609l	journal	August 2007
Simulations of Dendrimers with Flexible Spacer Chains and Explicit Counterions under Low and Neutral pH Conditions Kłos, J. S.; Sommer, J. -U. Macromolecules, Vol. 43, Issue 24 https://doi.org/10.1021/ma102055w	journal	December 2010
Structure of poly(propyl ether imine) dendrimer from fully atomistic molecular dynamics simulation and by small angle x-ray scattering Jana, Chandan; Jayamurugan, G.; Ganapathy, Rajesh The Journal of Chemical Physics, Vol. 124, Issue 20 https://doi.org/10.1063/1.2194538	journal	May 2006
Simulations of Terminally Charged Dendrimers with Flexible Spacer Chains and Explicit Counterions Kłos, J. S.; Sommer, J. -U. Macromolecules, Vol. 43, Issue 9 https://doi.org/10.1021/ma1003997	journal	May 2010
Molecular Dynamics Simulations of a Charged Dendrimer in Multivalent Salt Solution Tian, Wen-de; Ma, Yu-qiang The Journal of Physical Chemistry B, Vol. 113, Issue 40 https://doi.org/10.1021/jp906449g	journal	October 2009
Spatial distribution of intra-molecular water and polymeric components in polyelectrolyte dendrimers revealed by small angle scattering investigations Wu, Bin; Li, Xin; Do, Changwoo The Journal of Chemical Physics, Vol. 135, Issue 14 https://doi.org/10.1063/1.3651364	journal	October 2011
Association of a Weakly Acidic Anti-Inflammatory Drug (Ibuprofen) with a Poly(Amidoamine) Dendrimer as Studied by Molecular Dynamics Simulations Tanis, I.; Karatasos, K. The Journal of Physical Chemistry B, Vol. 113, Issue 31 https://doi.org/10.1021/jp9039176	journal	August 2009
Electrostatic Swelling and Conformational Variation Observed in High-Generation Polyelectrolyte Dendrimers Liu, Yun; Chen, Chun-Yu; Chen, Hsin-Lung The Journal of Physical Chemistry Letters, Vol. 1, Issue 13 https://doi.org/10.1021/jz1006143	journal	June 2010
Tuning the Density Profile of Dendritic Polyelectrolytes Welch, P.; Muthukumar, M. Macromolecules, Vol. 31, Issue 17 https://doi.org/10.1021/ma980198w	journal	August 1998
Dendrimers in Solution: Insight from Theory and Simulation Ballauff, Matthias; Likos, Christos N. Angewandte Chemie International Edition, Vol. 43, Issue 23 https://doi.org/10.1002/anie.200300602	journal	June 2004
Structural response of polyelectrolyte dendrimer towards molecular protonation: the inconsistency revealed by SANS and NMR Hong, Kunlun; Liu, Yun; Porcar, Lionel Journal of Physics: Condensed Matter, Vol. 24, Issue 6 https://doi.org/10.1088/0953-8984/24/6/064116	journal	January 2012
pH Responsiveness of polyelectrolyte dendrimers: a dynamical perspective Li, Xin; Zamponi, Michaela; Hong, Kunlun Soft Matter, Vol. 7, Issue 2 https://doi.org/10.1039/c0sm00671h	journal	January 2011
Charge-Induced Conformational Changes of Dendrimers Blaak, Ronald; Lehmann, Swen; Likos, Christos N. Macromolecules, Vol. 41, Issue 12 https://doi.org/10.1021/ma800283z	journal	June 2008
Solvent Quality Changes the Structure of G8 PAMAM Dendrimer, a Disagreement with Some Experimental Interpretations Maiti, Prabal K.; Goddard, William A. The Journal of Physical Chemistry B, Vol. 110, Issue 51 https://doi.org/10.1021/jp0622684	journal	December 2006
Structure Analysis by Small-Angle X-Ray and Neutron Scattering Feigin, L. A.; Svergun, D. I. https://doi.org/10.1007/978-1-4757-6624-0	book	January 1987
Soft matter with soft particles Likos, Christos N. Soft Matter, Vol. 2, Issue 6 https://doi.org/10.1039/b601916c	journal	January 2006
Development and testing of a general amber force field Wang, Junmei; Wolf, Romain M.; Caldwell, James W. Journal of Computational Chemistry, Vol. 25, Issue 9 https://doi.org/10.1002/jcc.20035	journal	January 2004
Effects of valences of salt ions at various concentrations on charged dendrimers Tian, Wen-de; Ma, Yu-qiang Soft Matter, Vol. 6, Issue 6 https://doi.org/10.1039/b923960j	journal	January 2010
Diffusion of flexible, charged, nanoscopic molecules in solution: Size and pH dependence for PAMAM dendrimer Maiti, Prabal K.; Bagchi, Biman The Journal of Chemical Physics, Vol. 131, Issue 21 https://doi.org/10.1063/1.3266512	journal	December 2009
Dendrimers Designed for Functions: From Physical, Photophysical, and Supramolecular Properties to Applications in Sensing, Catalysis, Molecular Electronics, Photonics, and Nanomedicine Astruc, Didier; Boisselier, Elodie; Ornelas, Cátia Chemical Reviews, Vol. 110, Issue 4 https://doi.org/10.1021/cr900327d	journal	April 2010
Evidence for Non-DLVO Hydration Interactions in Solutions of the Protein Apoferritin Petsev, Dimiter N.; Vekilov, Peter G. Physical Review Letters, Vol. 84, Issue 6 https://doi.org/10.1103/PhysRevLett.84.1339	journal	February 2000
Effect of Solvent and pH on the Structure of PAMAM Dendrimers Maiti, Prabal K.; Çaǧın, Tahir; Lin, Shiang-Tai Macromolecules, Vol. 38, Issue 3 https://doi.org/10.1021/ma049168l	journal	February 2005
An analysis of the accuracy of Langevin and molecular dynamics algorithms Pastor, Richard W.; Brooks, Bernard R.; Szabo, Attila Molecular Physics, Vol. 65, Issue 6 https://doi.org/10.1080/00268978800101881	journal	December 1988
Structural Investigation of PAMAM Dendrimers in Aqueous Solutions Using Small-Angle Neutron Scattering: Effect of Generation Porcar, Lionel; Liu, Yun; Verduzco, Rafael The Journal of Physical Chemistry B, Vol. 112, Issue 47 https://doi.org/10.1021/jp805297a	journal	November 2008
Analysis of Surface Structure and Hydrogen/Deuterium Exchange of Colloidal Silica Suspension by Contrast-Variation Small-Angle Neutron Scattering Suzuki, Takuya; Endo, Hitoshi; Shibayama, Mitsuhiro Langmuir, Vol. 24, Issue 9 https://doi.org/10.1021/la7039515	journal	May 2008
Numerical integration of the cartesian equations of motion of a system with constraints: molecular dynamics of n-alkanes Ryckaert, Jean-Paul; Ciccotti, Giovanni; Berendsen, Herman J. C. Journal of Computational Physics, Vol. 23, Issue 3 https://doi.org/10.1016/0021-9991(77)90098-5	journal	March 1977
Structural investigations of poly(amido amine) dendrimers in methanol using molecular dynamics Opitz, Armin W.; Wagner, Norman J. Journal of Polymer Science Part B: Polymer Physics, Vol. 44, Issue 21 https://doi.org/10.1002/polb.20949	journal	January 2006
Structural Molecular Dynamics Studies on Polyamidoamine Dendrimers for a Therapeutic Application: Effects of pH and Generation Lee, Inhan; Athey, Brian D.; Wetzel, Arthur W. Macromolecules, Vol. 35, Issue 11 https://doi.org/10.1021/ma010354q	journal	May 2002
Chord length distributions and small-angle scattering Gille, W. The European Physical Journal B, Vol. 17, Issue 3 https://doi.org/10.1007/s100510070116	journal	October 2000
PAMAM Dendrimers Undergo pH Responsive Conformational Changes without Swelling Liu, Yi; Bryantsev, Vyacheslav S.; Diallo, Mamadou S. Journal of the American Chemical Society, Vol. 131, Issue 8 https://doi.org/10.1021/ja8100227	journal	March 2009
Realistic numerical simulations of dendrimer molecules Freire, Juan J. Soft Matter, Vol. 4, Issue 11 https://doi.org/10.1039/b804687e	journal	January 2008
Scattering by an Inhomogeneous Solid Debye, P.; Bueche, A. M. Journal of Applied Physics, Vol. 20, Issue 6 https://doi.org/10.1063/1.1698419	journal	June 1949
Colloidal interactions Belloni, Luc Journal of Physics: Condensed Matter, Vol. 12, Issue 46 https://doi.org/10.1088/0953-8984/12/46/201	journal	October 2000
Small Angle Neutron Scattering Studies of the Counterion Effects on the Molecular Conformation and Structure of Charged G4 PAMAM Dendrimers in Aqueous Solutions Chen, Wei-Ren; Porcar, Lionel; Liu, Yun Macromolecules, Vol. 40, Issue 16 https://doi.org/10.1021/ma0626564	journal	August 2007

Similar Records

Molecular dynamics and neutron scattering study of the dependence of polyelectrolyte dendrimer conformation on counterion behavior

Journal Article · Tue Jul 31 20:00:00 EDT 2012 · The Journal of Chemical Physics · OSTI ID:1048155

The Effect of Counterion Valence on the pH Responsiveness of Polyelectrolyte Dendrimer Structure: A Small Angle Neutron Scattering Study

Journal Article · Sun Feb 28 23:00:00 EST 2010 · The Journal of Chemical Physics · OSTI ID:984767

Intra-molecular Structural Change of PAMAM Dendrimers in Aqueous Solutions Revealed by Small Angle Neutron Scattering

Journal Article · Thu Dec 31 23:00:00 EST 2009 · Journal of Physical Chemistry B · OSTI ID:979183

Related Subjects

75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
ELECTROLYTES
FLUCTUATIONS
FORM FACTORS
HYDROCARBONS
MICROSTRUCTURE
MOLECULAR DYNAMICS METHOD
NEUTRON DIFFRACTION
SCATTERING LENGTHS
SIMULATION
SMALL ANGLE SCATTERING
WATER

Structured water in polyelectrolyte dendrimers: Understanding small angle neutron scattering results through atomistic simulation

Citation Formats

References (59)

Similar Records

Related Subjects