Phase behavior of a deionized binary mixture of charged spheres in the presence of gravity

TL;DR

This study explores the complex phase behavior of a binary charged sphere suspension under deionized conditions, revealing regions of crystal stability, coexistence, and potential eutectic formation influenced by composition and gravity.

Contribution

It provides the first detailed phase diagram of a deionized binary charged sphere mixture, highlighting the effects of composition and gravity on crystallization and phase stability.

Findings

Dominance of bcc crystal formation without compositional order.

Identification of a stability minimum at p ≈ 0.8 and a stability peak at p ≈ 0.4.

Evidence of eutectic coexistence and compound formation.

Abstract

We report on the phase behavior of an aqueous binary charged sphere suspension under exhaustively deionized conditions as a function of number fraction of small particles p and total number density n. The mixture of size ratio 0.557 displays a complex phase diagram. Formation of bcc crystals with no compositional order dominates. We observe a region of drastically decreased crystal stability at 0.55 < p < 0.95 with the minimum located at p = 0.8 +/- 0.05 at densities above n = 26um-3. A peaked region of enhanced stability is observed at p = 0.4. Further light scattering experiments were conducted to characterize the crystallization time scales, the density profiles and the composition of formed phases. For 0.82 > p > 0.95 crystal formation is partially assisted by gravity, i.e. gravitational separation of the two species precedes crystal formation samples in the coexistence range. In the composition range corresponding to the decreased crystal stability only lower bounds of the freezing and melting line are obtained, but the general shape of the phase diagram is retained. At p = 0.93 and n = 43um-3 two different crystalline phases coexist in the bulk, while at p = 0.4 additional Bragg peaks appear in the static light scattering experiments. This strongly suggests that we observe a eutectic in the region of decreased stability, while the enhanced stability at p = 0.4 seems to correlate with compound formation.