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

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

doi:10.1063/1.3697479

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

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

SANS & Spin Echo

Research output: Contribution to journal › Article › peer-review

23 Scopus citations

Abstract

Based on atomistic molecular dynamics (MD) simulations, the small angle neutron scattering (SANS) intensity behavior of a single generation-4 polyelectrolyte polyamidoamine 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. The consistency found in comparison against previously published experimental findings (W.-R. Chen, L. Porcar, Y. Liu, P. D. Butler, and L. J. Magid, Macromolecules 40, 5887 (2007)) leads to a link between the neutron scattering experiment and MD computation, and fresh perspectives. The simulations enable scattering calculations of not only the hydrocarbons but also the contribution from the scattering length density fluctuations caused by structured, confined water within the dendrimer. Based on our computational results, we explore the validity of using radius of gyration RG for microstructure characterization of a polyelectrolyte dendrimer from the scattering perspective.

Original language	English
Article number	144901
Journal	Journal of Chemical Physics
Volume	136
Issue number	14
DOIs	https://doi.org/10.1063/1.3697479
State	Published - Apr 14 2012

Funding

This Research at Oak Ridge National Laboratory's Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. We thank the ORNL Institutional Cluster (OIC) for the computational support.

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title = "Structured water in polyelectrolyte dendrimers: Understanding small angle neutron scattering results through atomistic simulation",

abstract = "Based on atomistic molecular dynamics (MD) simulations, the small angle neutron scattering (SANS) intensity behavior of a single generation-4 polyelectrolyte polyamidoamine 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. The consistency found in comparison against previously published experimental findings (W.-R. Chen, L. Porcar, Y. Liu, P. D. Butler, and L. J. Magid, Macromolecules 40, 5887 (2007)) leads to a link between the neutron scattering experiment and MD computation, and fresh perspectives. The simulations enable scattering calculations of not only the hydrocarbons but also the contribution from the scattering length density fluctuations caused by structured, confined water within the dendrimer. Based on our computational results, we explore the validity of using radius of gyration RG for microstructure characterization of a polyelectrolyte dendrimer from the scattering perspective.",

author = "Bin Wu and Bouthe{\"i}na Kerkeni and Takeshi Egami and Changwoo Do and Yun Liu and Yongmei Wang and Lionel Porcar and Kunlun Hong and Smith, {Sean C.} and Liu, {Emily L.} and Smith, {Gregory S.} and Chen, {Wei Ren}",

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doi = "10.1063/1.3697479",

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AU - Kerkeni, Boutheïna

AU - Egami, Takeshi

AU - Do, Changwoo

AU - Liu, Yun

AU - Wang, Yongmei

AU - Porcar, Lionel

AU - Hong, Kunlun

AU - Smith, Sean C.

AU - Liu, Emily L.

AU - Smith, Gregory S.

AU - Chen, Wei Ren

PY - 2012/4/14

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N2 - Based on atomistic molecular dynamics (MD) simulations, the small angle neutron scattering (SANS) intensity behavior of a single generation-4 polyelectrolyte polyamidoamine 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. The consistency found in comparison against previously published experimental findings (W.-R. Chen, L. Porcar, Y. Liu, P. D. Butler, and L. J. Magid, Macromolecules 40, 5887 (2007)) leads to a link between the neutron scattering experiment and MD computation, and fresh perspectives. The simulations enable scattering calculations of not only the hydrocarbons but also the contribution from the scattering length density fluctuations caused by structured, confined water within the dendrimer. Based on our computational results, we explore the validity of using radius of gyration RG for microstructure characterization of a polyelectrolyte dendrimer from the scattering perspective.

AB - Based on atomistic molecular dynamics (MD) simulations, the small angle neutron scattering (SANS) intensity behavior of a single generation-4 polyelectrolyte polyamidoamine 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. The consistency found in comparison against previously published experimental findings (W.-R. Chen, L. Porcar, Y. Liu, P. D. Butler, and L. J. Magid, Macromolecules 40, 5887 (2007)) leads to a link between the neutron scattering experiment and MD computation, and fresh perspectives. The simulations enable scattering calculations of not only the hydrocarbons but also the contribution from the scattering length density fluctuations caused by structured, confined water within the dendrimer. Based on our computational results, we explore the validity of using radius of gyration RG for microstructure characterization of a polyelectrolyte dendrimer from the scattering perspective.

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

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