scholarly journals Slowing down of dynamics and orientational order preceding crystallization in hard-sphere systems

2020 ◽  
Vol 6 (43) ◽  
pp. eabc5916
Author(s):  
Felix Lehmkühler ◽  
Birgit Hankiewicz ◽  
Martin A. Schroer ◽  
Leonard Müller ◽  
Beatrice Ruta ◽  
...  

Despite intensive studies in the past decades, the local structure of disordered matter remains widely unknown. We show the results of a coherent x-ray scattering study revealing higher-order correlations in dense colloidal hard-sphere systems in the vicinity of their crystallization and glass transition. With increasing volume fraction, we observe a strong increase in correlations at both medium-range and next-neighbor distances in the supercooled state, both invisible to conventional scattering techniques. Next-neighbor correlations are indicative of ordered precursor clusters preceding crystallization. Furthermore, the increase in such correlations is accompanied by a marked slowing down of the dynamics, proving experimentally a direct relation between orientational order and sample dynamics in a soft matter system. In contrast, correlations continuously increase for nonequilibrated, glassy samples, suggesting that orientational order is reached before the sample slows down to reach (quasi-)equilibrium.


1999 ◽  
Vol 32 (3) ◽  
pp. 426-435 ◽  
Author(s):  
Cheng-Si Tsao ◽  
Tsang-Lang Lin

An improved method for small-angle X-ray scattering (SAXS) data analysis is developed to reconstruct the free-form particle size distribution of δ′ precipitation in an Al–Li alloy. This improved method consists of four iterative steps; the interparticle interference is also included. The indirect transform method (ITM) plus a hard-sphere (HS) model which considers the depleted zones are used in the analysis of δ′ precipitation in an Al–Li alloy. Two parameters, namely the hard-sphere volume fraction, ηHS, and the ratio of hard-sphere radius to the particle radius,RHS/R, which determine the structure factor of the interparticle effect, are iteratively calculated using the monodisperse assumption and Gaussian size distribution. These two parameters are finally used in reconstructing the particle size distribution by the ITM + HS method. This method is tested by analysing simulated SAXS data and shows a better agreement than found in similar studies. This improved method is applied to analyse a set of experimental SAXS intensities from δ′ (Al3Li particles) precipitation in an Al–9.7 at.% Li alloy. The monodisperse results are compared with the polydisperse ITM + HS results. The current ITM + HS method fits the SAXS data better than the other methods. The variations of average radii with aging time were found to follow the kinetic power law. The SAXS results are used to investigate the theoretical kinetic model of the volume-fraction effect on late-stage coarsening (Ostwald ripening). By comparing both experimentally obtained asymptotic size distributions of δ′ particles as well as coarsening rate constants with those predicted by the various kinetic models, the modified Lifshitz–Slyozov–Wagner (MLSW) theory is found to be in better agreement with the experimental results than the other theories.





2012 ◽  
Vol 45 (6) ◽  
pp. 1208-1218 ◽  
Author(s):  
Frédéric De Geuser ◽  
Françoise Bley ◽  
Alexis Deschamps

A methodology is presented for extracting the thickness and length of plate-like precipitates from streaking that appears in the small-angle scattering pattern of moderately textured polycrystalline samples. This methodology builds upon existing work on single crystals but is extended to polycrystals through a modeling of the streaking misalignment distribution. It is also shown that it is essential to take into account the Ewald sphere curvature. The protocol is applied to anin situsmall-angle X-ray scattering study of the transition between θ′ andT1in an Al–Li–Cu system, where the contributions of both phases are well separated, and the size, volume fraction and number density are monitored.



2019 ◽  
Vol 116 (16) ◽  
pp. 7766-7771 ◽  
Author(s):  
Ha Seong Kim ◽  
Nesrin Şenbil ◽  
Chi Zhang ◽  
Frank Scheffold ◽  
Thomas G. Mason

Motivated by improvements in diffusing wave spectroscopy (DWS) for nonergodic, highly optically scattering soft matter and by cursory treatment of collective scattering effects in prior DWS microrheology experiments, we investigate the low-frequency plateau elastic shear moduli Gp′ of concentrated, monodisperse, disordered oil-in-water emulsions as droplets jam. In such experiments, the droplets play dual roles both as optical probes and as the jammed objects that impart shear elasticity. Here, we demonstrate that collective scattering significantly affects DWS mean-square displacements (MSDs) in dense colloidal emulsions. By measuring and analyzing the scattering mean free path as a function of droplet volume fraction φ, we obtain a φ-dependent average structure factor. We use this to correct DWS MSDs by up to a factor of 4 and then calculate Gp′ predicted by the generalized Stokes–Einstein relation. We show that DWS-microrheological Gp′(φ) agrees well with mechanically measured Gp′(φ) over about three orders of magnitude when droplets are jammed but only weakly deformed. Moreover, both of these measurements are consistent with predictions of an entropic–electrostatic–interfacial (EEI) model, based on quasi-equilibrium free-energy minimization of disordered, screened-charge–stabilized, deformable droplets, which accurately describes prior mechanical measurements of Gp′(φ) made on similar disordered monodisperse emulsions over a wide range of droplet radii and φ. This very good quantitative agreement between DWS microrheology, mechanical rheometry, and the EEI model provides a comprehensive and self-consistent view of weakly jammed emulsions. Extensions of this approach may improve DWS microrheology on other systems of dense, jammed colloids that are highly scattering.



2015 ◽  
Vol 610 (1) ◽  
pp. 44-50 ◽  
Author(s):  
M. R. Thomas ◽  
J. E. Hallett ◽  
S. Klein ◽  
S. Mann ◽  
A. W. Perriman ◽  
...  




2010 ◽  
Vol 114 (49) ◽  
pp. 16347-16355 ◽  
Author(s):  
Isabelle Bihannic ◽  
Christophe Baravian ◽  
Jérôme F. L. Duval ◽  
Erwan Paineau ◽  
Florian Meneau ◽  
...  


1996 ◽  
Vol 6 (8) ◽  
pp. 1085-1094 ◽  
Author(s):  
A. Gibaud ◽  
J. Wang ◽  
M. Tolan ◽  
G. Vignaud ◽  
S. K. Sinha




Author(s):  
Ilya V. Roslyakov ◽  
Andrei P. Chumakov ◽  
Andrei A. Eliseev ◽  
Alexey P. Leontiev ◽  
Oleg V. Konovalov ◽  
...  


Sign in / Sign up

Export Citation Format

Share Document