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Register a new userDemonstration of variable angle Super-Heterodyne Dynamic Light Scattering for measuring colloidal dynamics
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We demonstrate a prototype light scattering instrument combining a frequency domain approach to the intermediate scattering function from Super-Heterodyning Doppler Velocimetry with the versatility of a standard homodyne Dynamic Light Scattering goniometer setup for investigations over a large range of scattering vectors. Comparing to reference experiments in correlation-time domain, we show that the novel approach can determine diffusion constants and hence hydrodynamic radii with high precision and accuracy. Possible future applications are discussed shortly.
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In soft matter structure couples to flow and vice versa. Complementary to structural investigations, we here are interested in the determination of particle velocities of charged colloidal suspensions of different structure under flow. In a combined effort of theory and experiment we determine the Fourier transform of the super-heterodyne field auto-correlation function (power spectrum) which in frequency space is found to be well separated from homodyne contributions and low frequency noise. Under certain conditions the power spectrum is dominated by incoherently scattered light, originating from the unavoidable size polydispersity of colloidal particles. A simple approximate form for the low-wavenumber self-intermediate scattering function is proposed, reminiscent to the case of non-interacting particles. We experimentally scrutinize the range of applicability of these simplified calculations on employing a parabolic electro-osmotic flow profile. Both for non-interacting and strongly interacting fluid particle systems, the spectra are well described as diffusion-broadened velocity distributions comprising an osmotic flow-averaged superposition of Lorentzians at distinct locations. We discuss the performance and scope of this approach with particular focus on moderately strong interactions and on multiphase flow. In addition, we point to some remaining theoretical challenges in connection to the observed linear increase of the effective diffusion constant and the integrated spectral power with increasing electric field strength.
Frequency domain super-heterodyne laser light scattering is utilized in a low angle integral measurement configuration to determine flow and diffusion in charged sphere suspensions showing moderate to strong multiple scattering. We introduce an empirical correction to subtract the multiple scattering background and isolate the singly scattered light. We demonstrate the excellent feasibility of this simple approach for turbid suspensions of transmittance T>0.4. We study the particle concentration dependence of the electro-kinetic mobility in low salt aqueous suspension over an extended concentration regime and observe a maximum at intermediate concentrations. We further use our scheme for measurements of the self-diffusion coefficients in the fluid samples in the absence or presence of shear, as well as in polycrystalline samples during crystallization and coarsening. We discuss the scope and limits of our approach as well as possible future applications.
Intermediate Scattering Functions (ISFs) are measured for colloidal hard sphere systems using both Dynamic Light Scattering (DLS) and X-ray Photon Correlation Spectroscopy (XPCS). We compare the techniques, and discuss the advantages and disadvantages of each. Both techniques agree in the overlapping range of scattering vectors. We investigate the scaling behaviour found by Segre and Pusey [1] but challenged by Lurio et al. [2]. We observe a scaling behaviour over several decades in time but not in the long time regime. Moreover, we do not observe long time diffusive regimes at scattering vectors away from the peak of the structure factor and so question the existence of a long time diffusion coefficients at these scattering vectors.
The Dynamic Monte Carlo (DMC) method is an established molecular simulation technique for the analysis of the dynamics in colloidal suspensions. An excellent alternative to Brownian Dynamics or Molecular Dynamics simulation, DMC is applicable to systems of spherical and/or anisotropic particles and to equilibrium or out-of-equilibrium processes. In this work, we present a theoretical and methodological framework to extend DMC to the study of heterogeneous systems, where the presence of an interface between coexisting phases introduces an additional element of complexity in determining the dynamic properties. In particular, we simulate a Lennard-Jones fluid at the liquid-vapor equilibrium and determine the diffusion coefficients in the bulk of each phase and across the interface. To test the validity of our DMC results, we also perform Brownian Dynamics simulations and unveil an excellent quantitative agreement between the two simulation techniques.
Understanding the rheology of colloidal suspensions is crucial in the formulation of a wide selection of industry-relevant products. To characterise the viscoelastic behaviour of these soft materials, one can analyse the microscopic dynamics of colloidal tracers diffusing through the host fluid and generating local deformations and stresses. This technique, referred to as microrheology, links the bulk rheology of fluids to the microscopic dynamics at the particle scale. If tracers are subjected to external forces, rather than freely diffusing, it is called active microrheology. Motivated by the impact of microrheology in providing information on local structure in complex systems such as colloidal glasses, active matter or biological systems, we have extended the dynamic Monte Carlo (DMC) technique to investigate active microrheology in colloids. The original DMC framework, able to accurately describe the Brownian dynamics of colloids at equilibrium, is here reconsidered and expanded to describe the effects of an external force pulling a tracer embedded in isotropic colloidal suspensions at different densities. To this end, we studied the dynamics of a spherical tracer dragged by a constant external force through a bath of spherical and rod-like particles of comparable size. We could extract valuable details on its effective friction coefficient, being constant at small and large values of the external force, but otherwise displaying a nonlinear behaviour that indicates the occurrence of a force-thinning regime. Our DMC simulation results are in excellent quantitative agreement with past Langevin dynamics simulations and theoretical works for the bath of spherical colloids. The bath of rod-like particles is studied in the isotropic phase, and displays an example where DMC is more convenient than Brownian or Langevin dynamics, in this case in dealing with particle rotation.
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