Department of Chemistry, Indian Institute of Science Education and Research (IISER), Pune, 411008, India.
Nanoscale. 2015 May 28;7(20):9204-14. doi: 10.1039/c5nr01016k. Epub 2015 Apr 30.
Electronic grade semiconductor films have been obtained via the sintering of solution processed PbS and PbSe nanocrystals at room temperature. Prior attempts to achieve similar films required the sintering of nanocrystals at higher temperatures (>350 °C), which inhibits the processing of such films on a flexible polymer substrate, and it is also expensive. We reduced the sintering temperature by employing two important strategies: (i) use of ligand-free nanocrystals and (ii) oriented attachment of nanocrystals. Colloidal ligand-free PbS and PbSe nanocrystals were synthesized at 70 °C with high yield (∼70%). However, these nanocrystals start to agglomerate with time in formamide, and upon the removal of the solvation energy, nanocrystals undergo oriented attachment, forming larger elongated crystals. PbS and PbSe nanocrystal films made on both glass and flexible substrates at room temperature exhibit Ohmic behavior with optimum DC conductivities of 0.03 S m(-1) and 0.08 S m(-1), respectively. Mild annealing of the films at 150 °C increases the conductivity values to 1.1 S m(-1) and 137 S m(-1) for PbS and PbSe nanocrystal films, respectively. AC impedance was measured to distinguish the contributions from grain and grain boundaries to the charge transport mechanism. Charge transport properties remain similar after the repeated bending of the film on a flexible polymer substrate. Reasonably high thermoelectric Seebeck coefficients of 600 μV K(-1) and 335 μV K(-1) for PbS and PbSe nanocrystal pellets, respectively, were obtained at room temperature.
通过室温下溶液处理的 PbS 和 PbSe 纳米晶的烧结,获得了电子级半导体薄膜。先前尝试获得类似的薄膜需要在较高温度(>350°C)下烧结纳米晶,这会抑制此类薄膜在柔性聚合物衬底上的加工,并且成本也很高。我们通过采用两种重要策略降低了烧结温度:(i)使用无配体的纳米晶,(ii)纳米晶的取向附生。在 70°C 下以高产率(约 70%)合成了胶体无配体的 PbS 和 PbSe 纳米晶。然而,这些纳米晶在甲酰胺中会随着时间的推移开始团聚,并且在去除溶剂化能时,纳米晶会发生取向附生,形成更大的拉长晶体。在室温下,在玻璃和柔性衬底上制备的 PbS 和 PbSe 纳米晶薄膜表现出欧姆行为,最佳直流电导率分别为 0.03 S m(-1) 和 0.08 S m(-1)。将薄膜在 150°C 下轻度退火会将电导率值分别提高到 1.1 S m(-1)和 137 S m(-1)。交流阻抗测量用于区分晶粒和晶界对电荷输运机制的贡献。在柔性聚合物衬底上反复弯曲后,电荷输运性能保持相似。在室温下,PbS 和 PbSe 纳米晶颗粒分别获得了 600 μV K(-1)和 335 μV K(-1)的合理高热电塞贝克系数。