Intrinsic defects in primary halide perovskites: A first-principles study of the thermodynamic trends
نویسندگان
چکیده
Defects in halide perovskites play an essential role determining the efficiency and stability of optoelectronic devices based on these materials. We present a systematic study intrinsic point defects six primary metal perovskites, ${\mathrm{MAPbI}}_{3}, {\mathrm{MAPbBr}}_{3}, {\mathrm{MAPbCl}}_{3}, {\mathrm{FAPbI}}_{3}, {\mathrm{CsPbI}}_{3}$, ${\mathrm{MASnI}}_{3}$ (where MA denotes methylammonium FA formamidinium), upon density functional theory calculations. Within single computational scheme, using $\text{SCAN}+\text{rVV10}$ functional, we compare impact changing anions cations defect formation energies charge state transition levels compounds, identify physical origins underlying observed trends. Dominant lead iodide compounds are ${A}^{+}$ cation interstitials ($A=\text{Cs}$, MA, FA), charge-compensated by ${\mathrm{I}}^{\ensuremath{-}}$ or $(2\ensuremath{-})$ vacancies. In bromide chloride most prominent, for ${\mathrm{MAPbCl}}_{3}$, chlorine vacancy also becomes important. These trends can be explained terms changes electrostatic interactions chemical bonding replacing anions. Defect physics is strongly dominated tin vacancies, promoted easy oxidation tin. Intrinsically, all mildly $p$ doped, except ${\mathrm{MASnI}}_{3}$, which doped. All acceptor created shallow. Some defects, vacancies Pb Sn particular, create deep donor traps. Although such traps might hamper electronic behavior bromine- iodine-based their equilibrium concentrations too small to affect materials' properties.
منابع مشابه
Atomic structure of metal-halide perovskites from first principles
Powered by TCPDF (www.tcpdf.org) This material is protected by copyright and other intellectual property rights, and duplication or sale of all or part of any of the repository collections is not permitted, except that material may be duplicated by you for your research use or educational purposes in electronic or print form. You must obtain permission for any other use. Electronic or print cop...
متن کاملIntrinsic defects and dopants in LiNH2: a first-principles study.
The lithium amide (LiNH(2)) + lithium hydride (LiH) system is one of the most attractive light-weight materials options for hydrogen storage. Its dehydrogenation involves mass transport in the bulk (amide) crystal through lattice defects. We present a first-principles study of native point defects and dopants in LiNH(2) using density functional theory. We find that both Li-related defects (the ...
متن کاملFirst-principles thermodynamic modeling of lanthanum chromate perovskites
Tendencies toward local atomic ordering in (A,A′)(B,B′)O3−δ mixed composition perovskites are modeled to explore their influence on thermodynamic, transport, and electronic properties. In particular, dopants and defects within lanthanum chromate perovskites are studied under various simulated redox environments. (La1−x ,Srx)(Cr1−y ,Fey)O3−δ (LSCF) and (La1−x ,Srx)(Cr1−y ,Ruy)O3−δ (LSCR) are mod...
متن کاملFirst-principles study of structural instabilities in halide-based perovskites: Competition between ferroelectricity and ferroelasticity.
متن کامل
Thermodynamic origin of instability in hybrid halide perovskites
Degradation of hybrid halide perovskites under the influence of environmental factors impairs future prospects of using these materials as absorbers in solar cells. First principle calculations can be used as a guideline in search of new materials, provided we can rely on their predictive capabilities. We show that the instability of perovskites can be captured using ab initio total energy calc...
متن کاملذخیره در منابع من
با ذخیره ی این منبع در منابع من، دسترسی به آن را برای استفاده های بعدی آسان تر کنید
ژورنال
عنوان ژورنال: Physical Review Materials
سال: 2022
ISSN: ['2476-0455', '2475-9953']
DOI: https://doi.org/10.1103/physrevmaterials.6.055402