Harnessing work-function-driven rotational steering for quantum state control in HCl dissociation on bimetallic alloys

), which generates a non-monotonic orientation-dependent potential energy landscape. We further establish a quantitative, predictive design principle, where rotational efficacy scales primarily with the work function difference and is systematically modulated by surface strain, with the highest efficacy achieved when a large work function difference is combined with compressive strain. This multivariate framework resolves a long standing dichotomy by demonstrating that rotational effects depend decisively on the global topography of the potential energy surface (PES), a mechanism fundamentally distinct from the transition state (TS) localized picture of vibrational promotion. The resulting quantum state control window enables rotation to act as a precise external knob for steering reactivity, advancing a new paradigm for the design of catalysts with targeted, state selective function.