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Designing High-Performance CdSe Nanocrystal Thin-Film Transistors Based on Solution Process of Simultaneous Ligand Exchange, Trap Passivation, and Doping
Chemistry of Materials ( IF 7.2 ) Pub Date : 2019-11-07 , DOI: 10.1021/acs.chemmater.9b02965 Woo Seok Lee , Yoon Gu Kang 1 , Ho Kun Woo , Junhyuk Ahn , Haneun Kim , Donggyu Kim , Sanghyun Jeon , Myung Joon Han 1 , Ji-Hyuk Choi 2 , Soong Ju Oh
Chemistry of Materials ( IF 7.2 ) Pub Date : 2019-11-07 , DOI: 10.1021/acs.chemmater.9b02965 Woo Seok Lee , Yoon Gu Kang 1 , Ho Kun Woo , Junhyuk Ahn , Haneun Kim , Donggyu Kim , Sanghyun Jeon , Myung Joon Han 1 , Ji-Hyuk Choi 2 , Soong Ju Oh
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We report a simple, solution-based, and postsynthetic process for simultaneous ligand exchange, surface passivation, and doping of CdSe nanocrystals (NCs) for the design of high-performance field-effect transistors (FETs). Strong electronic coupling, effective surface trap passivation, and n-type doping of the NCs could be achieved by simply immersing the as-synthesized CdSe NC thin films into InX3 (X = Cl, Br, I) solution. The optical, chemical, and structural properties of these CdSe NC thin films were analyzed, revealing successful ligand exchange and In doping. It is demonstrated that the doping level could be precisely controlled from lightly doped films to degenerately doped films by adjusting the type and concentration of halogen used in the ligand exchange solution. Ultraviolet photoelectron spectroscopy, first-principles calculation, and temperature-dependent electrical characterization of the InX3-treated CdSe NC FETs were performed to fundamentally understand their electronic structure and charge transport behavior. Combinational studies show that halides, as well as In, significantly affect the charge transport behavior in terms of halide-induced trap states as well as both tunneling and hopping transport mechanisms. It is demonstrated that Cl induces strong electronic coupling, effective trap passivation, and moderate In doping, resulting in optimized FETs with a mobility of over 10 cm2 V–1 s–1, ION/IOFF of over 107, and low activation energy of around 1 meV or even band-like transport behavior. This work provides a novel technological strategy and fundamental information on nanoscience for the design of cost-efficient, high-performance NC-based electronic, and optoelectronic devices.
中文翻译：
基于同时交换配体，陷阱钝化和掺杂的溶液工艺设计高性能CdSe纳米晶体薄膜晶体管
我们报告了一种简单的，基于溶液的合成后过程，用于同时配体交换，表面钝化和CdSe纳米晶体（NCs）掺杂，用于设计高性能场效应晶体管（FET）。只需将合成后的CdSe NC薄膜浸入InX 3中，即可实现强电子耦合，有效的表面陷阱钝化和NC的n型掺杂。（X = Cl，Br，I）溶液。分析了这些CdSe NC薄膜的光学，化学和结构性质，揭示了成功的配体交换和In掺杂。结果表明，通过调节配体交换溶液中所用卤素的类型和浓度，可以从轻掺杂薄膜到简并掺杂薄膜精确地控制掺杂水平。InX 3的紫外光电子能谱，第一性原理计算和与温度有关的电特性对经过处理的CdSe NC FET进行了研究，以从根本上了解其电子结构和电荷传输行为。组合研究表明，卤化物以及In会显着影响卤化物诱导的陷阱态以及隧穿和跳跃传输机制中的电荷传输行为。结果表明，Cl诱导了强电子耦合，有效的陷阱钝化和中等的In掺杂，从而产生了迁移率超过10 cm 2 V –1 s –1，I ON / I OFF超过10 7的优化FET。，并且活化能低，约为1 meV，甚至具有带状的传输行为。这项工作为设计具有成本效益的高性能基于NC的电子和光电设备提供了有关纳米科学的新颖技术策略和基本信息。
更新日期：2019-11-08
中文翻译：
基于同时交换配体，陷阱钝化和掺杂的溶液工艺设计高性能CdSe纳米晶体薄膜晶体管
我们报告了一种简单的，基于溶液的合成后过程，用于同时配体交换，表面钝化和CdSe纳米晶体（NCs）掺杂，用于设计高性能场效应晶体管（FET）。只需将合成后的CdSe NC薄膜浸入InX 3中，即可实现强电子耦合，有效的表面陷阱钝化和NC的n型掺杂。（X = Cl，Br，I）溶液。分析了这些CdSe NC薄膜的光学，化学和结构性质，揭示了成功的配体交换和In掺杂。结果表明，通过调节配体交换溶液中所用卤素的类型和浓度，可以从轻掺杂薄膜到简并掺杂薄膜精确地控制掺杂水平。InX 3的紫外光电子能谱，第一性原理计算和与温度有关的电特性对经过处理的CdSe NC FET进行了研究，以从根本上了解其电子结构和电荷传输行为。组合研究表明，卤化物以及In会显着影响卤化物诱导的陷阱态以及隧穿和跳跃传输机制中的电荷传输行为。结果表明，Cl诱导了强电子耦合，有效的陷阱钝化和中等的In掺杂，从而产生了迁移率超过10 cm 2 V –1 s –1，I ON / I OFF超过10 7的优化FET。，并且活化能低，约为1 meV，甚至具有带状的传输行为。这项工作为设计具有成本效益的高性能基于NC的电子和光电设备提供了有关纳米科学的新颖技术策略和基本信息。
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