Translational and rotational diffusion coefficients of gold nanorods functionalized with a high molecular weight, thermoresponsive ligand: a depolarized dynamic light scattering study

Feller, Déborah; Otten, Marius; Hildebrandt, Marco; Krüsmann, Marcel; Bryant, Gary; Karg, Matthias

doi:10.1039/d1sm00077b

Cited by 14 publications

(15 citation statements)

References 25 publications

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“…For spherical colloids, their dynamic behavior is well understood, and a very good agreement has been established between theory, simulations, and experiments [4][5][6]. For anisotropic particles, well established theory and predictions can be found for dilute systems [7][8][9][10], which also have been successfully compared with experiments for both translational and rotational motions [11][12][13][14][15][16] mainly using dynamic light scattering (DLS) and depolarized dynamic light scattering (DDLS) [17]. DDLS is the most useful tool for characterizing nonspherical particles, and thus has been applied to optically anisotropic particles such as the tobacco mosaic virus [18], gold nanorods [19], spheres with internal optical anisotropy [20][21][22][23], carbon nanotubes [24], claylike particles [12,25] and cellulose nanocrystals [26].…”

Section: Introductionmentioning

confidence: 74%

Extending depolarized DLS measurements to turbid samples

Pal¹,

Holmqvist²,

Vaccaro³

et al. 2022

Preprint

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The application of dynamic light scattering to soft matter systems has strongly profited from advanced approaches such as the so-called modulated 3D cross correlation technique (mod3D-DLS) that suppress contributions from multiple scattering, and can therefore be used for the characterization of turbid samples. Here we now extend the possibilities of this technique to allow for depolarized light scattering (Mod3D-DDLS) and thus obtain information on both translational and rotational diffusion, which is important for the characterization of anisotropic particles. We describe the required optical design and test the performance of the approach for increasingly turbid samples using well defined anisotropic colloidal models systems. Our measurements demonstrate that 3D-DDLS experiments can be performed successfully for samples with a reduced transmission due to multiple scattering as low as 1%. We compare the results from this approach with those obtained by standard DDLS experiments, and point out the importance of using an appropriate optical design when performing depolarized dynamic light scattering experiments with turbid systems.

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Section: Introductionmentioning

confidence: 74%

Extending depolarized DLS measurements to turbid samples

Pal¹,

Holmqvist²,

Vaccaro³

et al. 2022

Preprint

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“…As both rotational and translational diffusion of rod-shaped nanoparticles contributed to the autocorrelation function for DLS, the average sizes of GNRs and p(DMAEMA- b -NIPAM)-GNRs seemed to be greater than their actual dimensions. 30 The small peaks represent the rotational diffusion of the non-spherical GNRs depending on the aspect ratio of GNRs, and their relative peak intensity distribution would be increased with a higher aspect ratio. 31 Furthermore, the aspect ratio of the GNRs would be estimated by the relative amplitude ratio of two relaxation modes in correlation function of the scattered intensity ascribed from translational and rotational diffusion.…”

Section: Resultsmentioning

confidence: 99%

Stimuli-responsive plasmonic core–satellite hybrid nanostructures with tunable nanogaps

et al. 2023

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“…It is important to note that the DLS cumulant fit assumes isotropic scatterers and, in the case of the expanded nanohybrids, is likely a reasonable approximation of the size, especially when compared with the dimensions extracted from the SEM micrographs. However, in the case of the collapsed nanohybrids, the shell thickness is at least 82% smaller than the longest dimension of the core, resulting in anisotropic scatterers that require applying theoretical models to depolarized DLS to extract the precise dimensions. , Thus, our DLS measurements serve as an initial verification and qualitative approximation of the temperature-induced VPT rather than to determine the absolute sizes. The similar diameters measured at 50 °C for the two AuNR@pNIPAM samples may be the result of the much thinner, collapsed polymer shells, and, therefore, the AuNR core size dominated the overall hydrodynamic dimensions.…”

Section: Results and Discussionmentioning

confidence: 99%

Heterogeneity and Hysteresis in the Polymer Collapse of Single Core–Shell Stimuli-Responsive Plasmonic Nanohybrids

et al. 2021

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Broad application of polymeric stimuli-responsive smart nanohybrids requires understanding the mechanisms governing active control. Ensemble techniques have identified inhomogeneous polymer collapse in microgels that potentially arise from heterogeneous interchain interactions and differences in core size. A single-particle examination would establish the influence of core size and internal polymer network heterogeneity on local interactions that contribute to the observed inhomogeneous polymer collapse dynamics of nanohybrids. Using single-particle dark-field spectroscopy, we investigated the complex polymer collapse profiles of core–shell plasmonic nanohybrids comprising thermoresponsive poly(N-isopropylacrylamide) (pNIPAM)-encapsulated gold nanorods (AuNRs). We report that the polymer collapse behavior was independent of the core size. For thinner polymer shells, we observed hysteresis in the collapse of AuNR@pNIPAMs, likely related to local pNIPAM aggregation due to interchain hydrogen bonding. For thicker polymer shells, we observed a broad polymer collapse distribution that we attributed to a two-step phase transition that arises from a polymer network density gradient. Our single-particle approach relates the internal heterogeneity of the polymer network of nanohybrids to the mechanisms underlying heterogeneous phase transitions that traditional, ensemble-averaged approaches are unable to discern.

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Translational and rotational diffusion coefficients of gold nanorods functionalized with a high molecular weight, thermoresponsive ligand: a depolarized dynamic light scattering study

Abstract: Probing the rotational and translational diffusion and colloidal stability of nanorods is of significant fundamental interest with implications for many different applications. Recently R. Nixon-Luke and G. Bryant presented a...

Cited by 14 publications

References 25 publications

Extending depolarized DLS measurements to turbid samples

Extending depolarized DLS measurements to turbid samples

Stimuli-responsive plasmonic core–satellite hybrid nanostructures with tunable nanogaps

Heterogeneity and Hysteresis in the Polymer Collapse of Single Core–Shell Stimuli-Responsive Plasmonic Nanohybrids

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