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We describe the colloidal hot-injection synthesis of phase-pure nanocrystals(NCs) of a highly abundant mineral, chalcopyrite (CuFeS2). Absorption bandscentered at around 480 and 950 nm, spanning almost the entire visible and nearinfrared regions, encompass their optical extinction characteristics. Thesepeaks are ascribable to electronic transitions from the valence band (VB) tothe empty intermediate band (IB), located in the fundamental gap and mainlycomposed of Fe 3d orbitals. Laser-irradiation (at 808 nm) of an aqueoussuspension of CuFeS2 NCs exhibited significant heating, with a photothermalconversion efficiency of 49%. Such efficient heating is ascribable to thecarrier relaxation within the broad IB band (owing to the indirect VB-IB gap),as corroborated by transient absorption measurements. The intense absorptionand high photothermal transduction efficiency (PTE) of these NCs in theso-called biological window (650-900 nm) makes them suitable for photothermaltherapy as demonstrated by tumor cell annihilation upon laser irradiation. Theotherwise harmless nature of these NCs in dark conditions was confirmed by invitro toxicity tests on two different cell lines. The presence of the deep Felevels constituting the IB is the origin of such enhanced PTE, which can beused to design other high performing NC photothermal agents.

Colloidal CuFeS2 Nanocrystals: Intermediate Fe d-Band Leads to High Photothermal Conversion Efficiency