Unprecedented Improvement of Near-Infrared Photothermal Conversion Efficiency to 87.2% by Ultrafast Non-radiative Decay of Excited States of Self-Assembly Cocrystal.Near-infrared (NIR) photothermal conversion is of great interest in many fields.  Here, a self-assembly organic cocrystal (N,N,N',N'-tetramethyl-p-phenylenediamine (TMPD) and pyromellitic dianhydride (PMDA)) with strong absorption in NIR range is constructed, with widespread absorption (200-1500 nm) and very high NIR photothermal conversion efficiency (87.2%).  Strong intermolecular interactions enable the cocrystal to have dense electronic energy levels, leading to a high proportion (94.4%) vibrational cooling and internal conversion processes with ultrafast excited-state relaxation (0.12 ps), which contributes to high NIR photothermal conversion efficiency.  Furthermore, the cocrystal has exhibited capable ability for being an excellent candidate for a NIR photothermal therapy agent.
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