Abstract

We perform Brownian dynamics simulations of semiflexible colloidal sheets with hydrodynamic interactions and thermal fluctuations in shear flow. As a function of the ratio of bending rigidity to shear energy (a dimensionless quantity we denote S) and the ratio of bending rigidity to thermal energy, we observe a dynamical transition from stochastic flipping to crumpling and continuous tumbling. This dynamical transition is broadened by thermal fluctuations, and the value of S at which it occurs is consistent with the onset of chaotic dynamics found for athermal sheets. The effects of different dynamical conformations on rheological properties such as viscosity and normal stress differences are also quantified. Namely, the viscosity in a dilute dispersion of sheets is found to decrease with increasing shear rate (shear-thinning) up until the dynamical crumpling transition, at which point it increases again (shear-thickening), and non-zero first normal stress differences are found that exhibit a local maximum with respect to temperature at large S (small shear rate). These results shed light on the dynamical behavior of fluctuating 2D materials dispersed in fluids and should greatly inform the design of associated solution processing methods.

Highlights

  • Researchers are turning to solution processing methods for 2D materials,[1–15] yet fundamental knowledge of the dynamical behavior of 2D materials in flow and how such behavior correlates with macroscopic rheological properties and coupled fluid dynamical responses is still lacking

  • In previous work,[23] we studied the dynamical behavior of thin, athermal, semiflexible sheets in simple shear flow as a function of two dominant variables: the initial orientation of a flat sheet about the flow axis, f, and the dimensionless ratio of bending rigidity, k, to shear strength given by k

  • Numerical immersed boundary simulations of semiflexible sheets subjected to thermal fluctuations and ambient simple shear flow were conducted over a range of values for dimensionless bending rigidity, S = k/(pZg_L3), and dimensionless temperature, kBT/k

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Summary

Introduction

Researchers are turning to solution processing methods for 2D materials,[1–15] yet fundamental knowledge of the dynamical behavior of 2D materials in flow and how such behavior correlates with macroscopic rheological properties and coupled fluid dynamical responses is still lacking. In previous work,[23] we studied the dynamical behavior of thin, athermal, semiflexible sheets in simple shear flow as a function of two dominant variables: the initial orientation of a flat sheet about the flow axis, f, and the dimensionless ratio (denoted S) of bending rigidity, k, to shear strength given by k. We study the behavior of a thermalized ‘‘beadspring’’ sheet model immersed in a low-Reynolds-number simple shear flow. Such sheets can be considered asymptotically thin from the hydrodynamic point of view and are relatively inextensible compared to out-plane bending modes (i.e., they have large Foppl–von Karman numbers). Scaling predictions for flipping statistics (g_Dtflip B (kBT/k)À1/3SÀ1/3 and Var[g_Dtflip] B (kBT/k)À2/3SÀ2/3) are made with the aid of a first passage time model, and all are found to match simulation data well

Model and methods
Flipping behavior
Conformational behavior
Rheological properties
Conclusions
Findings
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