Self-healing low molecular weight supramolecular gels (SMGs) represent an emerging class of smart materials, which can closely mimic the complex biological healing process, such as blood clotting, bone repair or wound healing. However, a lack of understanding of the structure-function correlation in the self-assembly process limits their molecular design and subsequent property tuning. The indispensability of a rheological study on supramolecular gels lies in direct transcription of the assembly property to the viscoelastic behavior of the material. This is similarly relevant to healable and non-healable systems. Thus, using rheology as a tool for elucidating structure-function relationships in self-assembled systems has huge potential. This review article will depict a general introduction of rheology in the field of soft matter including SMGs, followed by representative studies with interpretations, and discussion on future challenges. Altogether, this would be an effort, where an in-depth rheological study complemented with a real-time visualization with the help of microscopy, and introduction of other sophisticated real-time experiments, could be a step forward to capture the mystery of self-assembly process.

Thermodynamic versus kinetic control: Small‐angle neutron scattering (SANS) and single‐crystal X‐ray diffraction data have been used to elucidate the effect of temperature, solvent, and metal identity on the formation of dimeric or hexameric metal‐seamed pyrogallol[4]arene capsules. Higher temperatures, methanol solution, and the use of nickel metal favor dimer formation (see scheme).

Lateral slicing of micron length carbon nanotubes (CNTs) is effective on laser irradiation of the materials suspended within dynamic liquid thin films in a microfluidic vortex fluidic device (VFD). The method produces sliced CNTs with minimal defects in the absence of any chemical stabilizers, having broad length distributions centred at ca 190, 160 nm and 171 nm for single, double and multi walled CNTs respectively, as established using atomic force microscopy and supported by small angle neutron scattering solution data. Molecular dynamics simulations on a bent single walled carbon nanotube (SWCNT) with a radius of curvature of order 10 nm results in tearing across the tube upon heating, highlighting the role of shear forces which bend the tube forming strained bonds which are ruptured by the laser irradiation. CNT slicing occurs with the VFD operating in both the confined mode for a finite volume of liquid and continuous flow for scalability purposes.