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

详细信息    查看全文

• 作者：Sandeep Ghosh ; Tommaso Avellini ; Alessia Petrelli ; Ilka Kriegel ; Roberto Gaspari ; Guilherme Almeida ; Giovanni Bertoni ; Andrea Cavalli ; Francesco Scotognella ; Teresa Pellegrino ; Liberato Manna
• 刊名：Chemistry of Materials
• 出版年：2016
• 出版时间：July 12, 2016
• 年：2016
• 卷：28
• 期：13
• 页码：4848-4858
• 全文大小：564K
• 年卷期：0
• ISSN：1520-5002

文摘

We describe the colloidal hot-injection synthesis of phase-pure nanocrystals (NCs) of a highly abundant mineral, chalcopyrite (CuFeS₂). Absorption bands centered at around 480 and 950 nm, spanning almost the entire visible and near-infrared regions, encompass their optical extinction characteristics. These peaks are ascribable to electronic transitions from the valence band (VB) to the empty intermediate band (IB), located in the fundamental gap and mainly composed of Fe 3d orbitals. Laser-irradiation (at 808 nm) of an aqueous suspension of CuFeS₂ NCs exhibited significant heating, with a photothermal conversion efficiency of 49%. Such efficient heating is ascribable to the carrier relaxation within the broad IB band (owing to the indirect VB–IB gap), as corroborated by transient absorption measurements. The intense absorption and high photothermal transduction efficiency (PTE) of these NCs in the so-called biological window (650–900 nm) make them suitable for photothermal therapy as demonstrated by tumor cell annihilation upon laser irradiation. The otherwise harmless nature of these NCs in dark conditions was confirmed by in vitro toxicity tests on two different cell lines. The presence of the deep Fe levels constituting the IB is the origin of such enhanced PTE, which can be used to design other high performing NC photothermal agents.