Broadband-absorbing structurally distorted cocrystal with enhanced nonradiative decay for solar interfacial water evaporation

• • NMTQ cocrystal achieves broadband absorption from 220 to 2000 nm, covering UV to NIR-II, enabling efficient solar harvesting across the full spectrum; this eliminates the need for complex multi-component systems and reduces material cost for photothermal applications. • • The non-planar butterfly-like conformation yields higher non-adiabatic couplings (NACs) and lower spatial overlap integral (Sr), enhancing non-radiative decay pathways; this structural distortion increases photothermal conversion efficiency by promoting vibrational relaxation, as validated by quantum chemical calculations. • • Interfacial solar evaporation system delivers an evaporation rate of 2.158 kg m−2 h−1 with 94.96% solar-to-vapor conversion efficiency under 1 Sun irradiation; this performance exceeds many reported systems and approaches the theoretical limit, offering a viable route for energy-efficient desalination and wastewater treatment. • • The photothermal platform simultaneously removes contaminants, integrating water purification with evaporation; this multifunctionality reduces operational complexity and cost, providing a sustainable solution for clean water production in off-grid or resource-limited settings.