Data for: Air Exposure Oxidation and Photooxidation of Solution-Phase Treated PbS Quantum Dot Thin Films and Solar Cells
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Figure 1. a) X-ray diffraction pattern of the synthesized particles is consistent with the standard pattern of rock-salt PbS, b) TEM image and the size distribution histogram indicate that the synthesized QDs are monodispersed and have an average diameter of 3 nm with a standard deviation of 9.43%, c) the emission and absorption spectra of the colloidal QDs. Figure 2. AFM images (ARA AFM instrument, Ara research, Iran) of PbS QDs thin films prepared by different methods: a) LBL process consisting 13 times repetition of QDs deposition, solid-state ligand exchange with MPA, and washing steps, b) single-step deposition of MPA-treated QDs, c) single-step deposition of MAI-treated QDs. Figure 3. PL spectra of colloidal and thin films of PbS QDs treated with different ligands: a) OA, b) BA, c) MPA, d) TBAI, e) MAI, f) MAPbI3. Figure 4. Effect of air exposure times on the PL spectra of PbS QD thin films treated with different ligands: a) OA, b) BA, c) MPA, d) TBAI, e) MAI, f) MAPbI3. Figure 5. Variations of PL peak shifts of the different surface treated PbS QDs thin films over the long terms of air exposure. Figure 6. The XPS full scan (a) and XPS Pb 4f (b) spectra of the OA-capped PbS QDs thin film before and after 10 days of air exposure. Deconvolution of XPS Pb 4f spectra of air-free (c) and air-exposed (d) OA-capped PbS QDs thin films to their chemical components. Figure 7. a) Atomistic model of 3 nm PbS QDs with a truncated octahedron morphology. Schematic of ligands coverage and oxygen penetration pathways to the surface of PbS QDs treated with OA (b), TBAI (c), MAI (d), BA (e), MPA (f), and MAPbI3 (g) ligands. Figure 8. The XPS full scan (a) and XPS I 3d (b) spectra of the PbS QDs thin film before and after the TBAI ligand exchange. Deconvolution of XPS Pb 4f spectra of air-free (c) and air-exposed (d) iodide-capped PbS QDs thin films to their chemical components. Figure 9. XPS spectra of PbS QD thin films before and after the MAPbI3 ligand exchange: a) the XPS full scan, b) XPS I 3d spectrum, c) XPS N 1s spectrum, and d) XPS Pb 4f spectrum. Figure 10. XPS spectra of MAPbI3-treated PbS QDs thin films before and after 10 days of air storage: a) the XPS full scan, b) XPS I 3d spectrum, c) XPS Pb 4f spectrum, d) deconvolution of XPS Pb 4f spectra of the air-exposed thin film to its chemical components. Figure 11. Time-resolved PL signals of PbS QD thin films treated with different ligands, under two different cycles of continuous and intermittent laser illumination (λ= 1064 nm). Figure 12. PCE variations of p-n (a) and p-i-n (b) QDSCs at different air storage times (Background: schematic structure of the fabricated devices).
图1。a) 合成颗粒的X射线衍射（X-ray diffraction, XRD）图谱与岩盐结构硫化铅（PbS）的标准衍射图谱一致；b) 透射电子显微镜（Transmission Electron Microscopy, TEM）图像及粒径分布直方图显示，所合成的量子点（Quantum Dots, QDs）单分散性良好，平均粒径为3 nm，标准偏差为9.43%；c) 该胶体量子点的发射光谱与吸收光谱。图2。采用不同方法制备的硫化铅（PbS）量子点薄膜的原子力显微镜（Atomic Force Microscopy, AFM）图像（测试仪器为ARA AFM，由伊朗Ara研究公司生产）：a) 经13次量子点沉积、巯基丙酸（Mercaptopropionic Acid, MPA）固相配体交换及清洗工序的层叠（Layer-by-Layer, LBL）组装工艺制备样品；b) 经MPA处理的量子点一步沉积制备样品；c) 经甲胺碘（Methylammonium Iodide, MAI）处理的量子点一步沉积制备样品。图3。经不同配体处理的硫化铅胶体量子点及其薄膜的光致发光（Photoluminescence, PL）光谱：a) 油酸（Oleic Acid, OA）配体，b) 正丁酸（Butyric Acid, BA）配体，c) 巯基丙酸（Mercaptopropionic Acid, MPA）配体，d) 四丁基碘化铵（Tetrabutylammonium Iodide, TBAI）配体，e) 甲胺碘（Methylammonium Iodide, MAI）配体，f) 甲胺碘化铅（Methylammonium Lead Triiodide, MAPbI3）配体。图4。空气暴露时长对经不同配体处理的硫化铅量子点薄膜光致发光光谱的影响：a) OA配体，b) BA配体，c) MPA配体，d) TBAI配体，e) MAI配体，f) MAPbI3配体。图5。不同表面修饰的硫化铅量子点薄膜在长期空气暴露过程中的光致发光峰位偏移变化。图6。OA封端的硫化铅量子点薄膜在空气暴露10天前后的X射线光电子能谱（X-ray Photoelectron Spectroscopy, XPS）全扫描谱(a)与Pb 4f高分辨谱(b)；将无空气暴露(c)与经空气暴露(d)的OA封端硫化铅量子点薄膜的Pb 4f高分辨谱分峰拟合为其化学组分。图7。a) 具有截角八面体形貌的3 nm硫化铅量子点原子级模型；配体覆盖情况及氧气渗透至经不同配体处理的硫化铅量子点表面的路径示意图：b) OA配体，c) TBAI配体，d) MAI配体，e) BA配体，f) MPA配体，g) MAPbI3配体。图8。经TBAI配体交换处理的硫化铅量子点薄膜在处理前后的XPS全扫描谱(a)与I 3d高分辨谱(b)；将无空气暴露(c)与经空气暴露(d)的碘封端硫化铅量子点薄膜的Pb 4f高分辨谱分峰拟合为其化学组分。图9。经MAPbI3配体交换处理的硫化铅量子点薄膜的XPS谱图：a) XPS全扫描谱，b) I 3d高分辨谱，c) N 1s高分辨谱，d) Pb 4f高分辨谱。图10。经MAPbI3处理的硫化铅量子点薄膜在空气储存10天前后的XPS谱图：a) XPS全扫描谱，b) I 3d高分辨谱，c) Pb 4f高分辨谱，d) 经空气暴露的薄膜的Pb 4f高分辨谱分峰拟合结果。图11。不同配体修饰的硫化铅量子点薄膜在连续与间歇两种激光照明循环下的时间分辨光致发光信号（激发波长λ=1064 nm）。图12。不同空气储存时长下p-n型(a)与p-i-n型(b)量子点太阳能电池（Quantum Dot Solar Cells, QDSCs）的光电转换效率（Power Conversion Efficiency, PCE）变化（背景：所制备器件的结构示意图）。
