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The rheology of molecular brushes remains challenging to control due to themultiple length scales and relaxation processes involved and the lack of directobservation of molecular conformation during flow. We use molecular dynamicssimulations to determine the shear thinning of unentangled bottlebrush polymerswith varying architecture, from linear chains to combs, to densely graftedbottlebrushes, to star-like and star polymers. We find shear thinning exponentsin line with theoretical and experimental results and characterize the shapeand orientation of bottlebrushes in steady-state flow. Many shape parametersderived from the gyration tensor show molecular alignment with the flow for allsystems. Yet, the orientation of individual bonds is what most stronglycorrelates with the architecture-dependent shear-thinning exponents. In denselygrafted bottlebrushes, the packing of side chains prevents alignment with theflow, causing a reduction in shear thinning. The molecular insight from oursimulations is useful to tune the architecture of bottlebrushes to controltheir rheology.

Shear Thinning from Bond Orientation in Model Unentangled Bottlebrush Polymer Melts