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Phys Rev E. 2019 May;99(5-1):052504. doi: 10.1103/PhysRevE.99.052504.

Model-free description of polymer-coated gold nanoparticle dynamics in aqueous solutions obtained by Bayesian analysis of neutron spin echo data.

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Consiglio Nazionale delle Ricerche, Istituto Officina dei Materiali c/o OGG Grenoble, France.
Dipartimento di Economia e Diritto, Università di Macerata, Via Crescimbeni 20, 62100 Macerata, Italy.
Department of Chemistry, McGill University, Sherbrooke St. West, Montreal, Canada.
Dipartimento di Fisica e Astronomia, Università di Firenze, via G. Sansone 1, I-50019 Sesto Fiorentino, Italy.
Consiglio Nazionale delle Ricerche, Istituto di Fisica Applicata "Nello Carrara", via Madonna del Piano 10, I-50019 Sesto Fiorentino, Italy.
Institut Laue-Langevin, Grenoble, France.
Université Grenoble Alpes-Laboratoire TIMC/IMAG UMR CNRS 5525 Grenoble, France.


We present a neutron spin echo study of the nanosecond dynamics of polyethylene glycol (PEG) functionalized nanosized gold particles dissolved in D_{2}O at two temperatures and two different PEG molecular weights (400D and 2000D). The analysis of the neutron spin echo data was performed by applying a Bayesian approach to the description of time correlation function decays in terms of exponential terms, recently proved to be theoretically rigorous. This approach, which addresses in a direct way the fundamental issue of model choice in any dynamical analysis, provides here a guide to the most statistically supported way to follow the decay of the intermediate scattering functions I(Q,t) by basing on statistical grounds the choice of the number of terms required for the description of the nanosecond dynamics of the studied systems. Then, the presented analysis avoids from the start resorting to a preselected framework and can be considered as model free. By comparing the results of PEG-coated nanoparticles with those obtained in PEG2000 solutions, we were able to disentangle the translational diffusion of the nanoparticles from the internal dynamics of the polymer grafted to them, and to show that the polymer corona relaxation follows a pure exponential decay in agreement with the behavior predicted by coarse grained molecular dynamics simulations and theoretical models. This methodology has one further advantage: in the presence of a complex dynamical scenario, I(Q,t) is often described in terms of the Kohlrausch-Williams-Watts function that can implicitly represent a distribution of relaxation times. By choosing to describe the I(Q,t) as a sum of exponential functions and with the support of the Bayesian approach, we can explicitly determine when a finer-structure analysis of the dynamical complexity of the system exists according to the available data without the risk of overparametrization. The approach presented here is an effective tool that can be used in general to provide an unbiased interpretation of neutron spin echo data or whenever spectroscopy techniques yield time relaxation data curves.


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