Electrical doping of metal halide perovskites (MPHs) is a key step towards the use of this efficient and cost-effective semiconductor class in modern electronics. In this work, we demonstrate n-type doping of methylammonium lead iodide (CH3NH3PbI3) by the post-fabrication introduction of Sm2+. The ionic radius of the latter is similar to that of Pb2+ and can replace it without altering the perovskite crystal lattice. It is demonstrated that once incorporated, Sm2+ can act as a dopant by undergoing oxidation to Sm3+. This results in the release of a negative charge that n-dopes the material, resulting in an increase of conductivity of almost 3 orders of magnitude. Unlike substitution doping with heterovalent ions, furtive dopants do not require counterions to maintain charge neutrality with respect to the ions they replace and are thus more likely to be incorporated into the crystalline structure. The incorporation of the dopant throughout the material is evidenced by XPS and ToF-SIMS, while the XRD pattern shows no phase separation at low and medium doping concentrations. A shift of the Fermi level towards a conduction energy of 0.52 eV confirms the doping to be n-type with a charge carrier density, calculated using the Mott-Schottky method, estimated to be nearly 1017 cm-3 for the most conductive samples. Variable-temperature conductivity experiments show that the dopant is only partially ionized at room temperature due to dopant freeze-out.
Materials horizons. 2023 Jul 31;10(8):2845-2853. doi: 10.1039/d3mh00663h Q110.72025
Redox-active ions unlock substitutional doping in halide perovskites
可还原离子解锁卤化物钙钛矿的固溶体杂质掺杂效应 翻译改进
作者单位 +展开
作者单位
DOI: 10.1039/d3mh00663h PMID: 37439828
摘要 Ai翻译
相关内容
-
From Large to Small Polarons in Lead, Tin, and Mixed Lead-Tin Halide Perovskites
从铅、锡及其固溶体卤化物钙钛矿中的大极化子到小极化子
The journal of physical chemistry letters. 2019 Apr 18;10(8):1790-1798.
-
Halide perovskites enable polaritonic XY spin Hamiltonian at room temperature
卤化物钙钛矿在室温下实现极子XY自旋哈密顿量
Nature materials. 2022 Jul;21(7):761-766.
-
Compositional gradient engineering and applications in halide perovskites
构成化梯度工程在卤化物钙钛矿材料中的应用研究
Chemical communications (Cambridge, England). 2023 Apr 27;59(35):5156-5173.
-
A study on theoretical models for investigating time-resolved photoluminescence in halide perovskites
卤化物钙钛矿中时间分辨光致发光的理论模型研究
Physical chemistry chemical physics : PCCP. 2023 Mar 15;25(11):7574-7588.
-
Indirect tail states formation by thermal-induced polar fluctuations in halide perovskites
卤化物钙钛矿中由热诱导的极化波动形成的间接能带尾态
Nature communications. 2019 Jan 29;10(1):484.
-
Piezoelectric Charge Coefficient of Halide Perovskites
卤化物钙钛矿的压电荷系数
Materials (Basel, Switzerland). 2024 Jun 23;17(13):3083.
-
Radiative Recombination Processes in Halide Perovskites Observed by Light Emission Voltage Modulated Spectroscopy
卤化物钙钛矿中通过发光电压调制光谱观测到的辐射复合过程
Advanced materials (Deerfield Beach, Fla.). 2023 Mar;35(11):e2207993.
-
Spatial Localization of Defects in Halide Perovskites Using Photothermal Deflection Spectroscopy
使用光电热偏转光谱法对卤化物钙钛矿中缺陷的空间定位
The journal of physical chemistry letters. 2024 Feb 8;15(5):1273-1278.