Manipulating Molecular Matter - Thesis Electronic Supplementary

Organisation. The deposit is grouped into three folders, one per thesis chapter. Files are named Ch_MovieS.mp4, matching the "Movie Sn" labels used in the thesis text.

Each folder carries a README.md describing its contents and acquisition conditions; a top-level README.md describes the deposit as a whole. Chapter 2 — A Supramolecular Zipping Engine (2 movies). Optical-tweezer manipulation of single supramolecular fibres held in a splayed "zipping" conformation.

Movie S1 shows repeated unzipping "ping-pong" cycles performed on a morphologically less pristine fibre docked on a glass needle. Movie S2 (15 Hz brightfield) shows a fibre in the aligned splayed conformation whose two ends spontaneously zip together upon approach and are subsequently unzipped under tension; this is the recording from which the zipping force F_zip = 1.41 ± 0.11 pN is determined. Chapter 3 — Emergence of Plasticity through Inter-Fibril Sliding (4 movies).

Movie S1: tensile strain applied to a bulk hydrogel (3.33 mM monomer, 1 M KCl), showing plastic deformation and fibre alignment; the material begins in the solution phase at 20 °C and is gelled at 37 °C, visible as a colour change. Movies S2–S4: correlated brightfield timelapses of optical-tweezer experiments — cyclic loading of a single fibre, cyclic loading of a hydrogel, and point-stress deformation of a hydrogel. Movies carry burnt-in scale bars.

Chapter 4 — Mechanochemistry inside Motile Marangoni Droplets (6 movies). Movie S1: motility assay covering the full kinetic sequence — non-motile lag phase, onset of motility with concurrent internal phase separation, acceleration, and the plateau regime in which polarised Janus droplets appear. Movies S2–S3: fluorescent bead tracking inside droplets under solution-phase and gelated conditions, showing uncorrelated versus strongly correlated inter-bead motion.

Movie S4: cross-polarised optical microscopy of a motile and a non-motile droplet above the LCST, showing birefringence only in the motile droplet. Movie S5: particle-tracking velocimetry of the internal flow field, revealing a toroidal vortex. Movie S6: cross-polarised videography of the monomer solution in a shear rheometer during a flow ramp (0.15–100 rad s⁻¹), showing shear-induced anisotropic structures.

Formats and size. Twelve MP4 (H.264) movies, approximately 775 MB in total, plus four Markdown README files. Chapters 1 (design principles for supramolecular machines) and 5 (encapsulation in giant unilamellar vesicles) have no associated movies and are not represented here.