Slippery covalently‐attached liquid surfaces (SCALS) with low contact angle hysteresis (CAH, <5◦) and nanoscale thickness display impressive anti‐adhesive properties, similar to lubricant‐infused surfaces. Their efficacy is generally attributed to the
liquid‐like mobility of the constituent tethered chains. However, the precise physico‐chemical properties that facilitate this mobility are
unknown, hindering rational design.
This work quantifies the chain length, grafting density, and microviscosity of a range of polydimethylsiloxane (PDMS) SCALS, elucidating
the nanostructure responsible for their properties. Three prominent methods are used to produce SCALS, with characterization
carried out via single‐molecule force measurements, neutron reflectometry, and fluorescence correlation spectroscopy. CO2 snow‐jet
cleaning was also shown to reduce the CAH of SCALS via a modification of their grafting density. SCALS behavior can be predicted
by reduced grafting density, Σ, with the lowest water CAH achieved at Σ ≈ 2. This study provides the first direct examination of
SCALS grafting density, chain length, and microviscosity and supports the hypothesis that SCALS properties stem from a balance of
layer uniformity and mobility.