Nonempirical hybrid functionals for band gaps of inorganic metal-halide perovskites

被引:50
作者
Bischoff, Thomas [1 ]
Wiktor, Julia [1 ,2 ]
Chen, Wei [3 ]
Pasquarello, Alfredo [1 ]
机构
[1] Ecole Polytech Fed Lausanne, CSEA, CH-1015 Lausanne, Switzerland
[2] Chalmers Univ Technol, Dept Phys, SE-41296 Gothenburg, Sweden
[3] Catholic Univ Louvain, Inst Condensed Matter & Nanosci IMCN, B-1348 Louvain La Neuve, Belgium
基金
瑞士国家科学基金会;
关键词
DIELECTRIC-CONSTANT; EXCHANGE; PHOTOLUMINESCENCE; FOCK; TIN;
D O I
10.1103/PhysRevMaterials.3.123802
中图分类号
T [工业技术];
学科分类号
08 ;
摘要
Nonempirical hybrid functionals are investigated for band-gap predictions of inorganic metal-halide perovskites belonging to the class CsBX3, with B = Ge, Sn, Pb and X = Cl, Br, I. We consider both global and range-separated hybrid functionals and determine the parameters through two different schemes. The first scheme is based on the static screening response of the material and thus yields dielectric-dependent hybrid functionals. The second scheme defines the hybrid functionals through the enforcement of Koopmans' condition for localized defect states. We also carry out quasiparticle self-consistent GW calculations with vertex corrections to establish state-of-the-art references. For the investigated class of materials, dielectric-dependent functionals and those fulfilling Koopmans' condition yield band gaps of comparable accuracy (similar to 0.2 eV), but the former only require calculations for the primitive unit cell and are less subject to the specifics of the material.
引用
收藏
页数:9
相关论文
共 71 条
[1]   QUANTUM THEORY OF DIELECTRIC CONSTANT IN REAL SOLIDS [J].
ADLER, SL .
PHYSICAL REVIEW, 1962, 126 (02) :413-+
[2]   Defect levels through hybrid density functionals: Insights and applications [J].
Alkauskas, Audrius ;
Broqvist, Peter ;
Pasquarello, Alfredo .
PHYSICA STATUS SOLIDI B-BASIC SOLID STATE PHYSICS, 2011, 248 (04) :775-789
[3]   DENSITY-FUNCTIONAL THERMOCHEMISTRY .3. THE ROLE OF EXACT EXCHANGE [J].
BECKE, AD .
JOURNAL OF CHEMICAL PHYSICS, 1993, 98 (07) :5648-5652
[4]   Adjustable potential probes for band-gap predictions of extended systems through nonempirical hybrid functionals [J].
Bischoff, Thomas ;
Reshetnyak, Igor ;
Pasquarello, Alfredo .
PHYSICAL REVIEW B, 2019, 99 (20)
[5]   Sequential deposition as a route to high-performance perovskite-sensitized solar cells [J].
Burschka, Julian ;
Pellet, Norman ;
Moon, Soo-Jin ;
Humphry-Baker, Robin ;
Gao, Peng ;
Nazeeruddin, Mohammad K. ;
Graetzel, Michael .
NATURE, 2013, 499 (7458) :316-+
[6]   Bandgap calculations and trends of organometal halide perovskites [J].
Castelli, Ivano E. ;
Garcia-Lastra, Juan Maria ;
Thygesen, Kristian S. ;
Jacobsen, Karsten W. .
APL MATERIALS, 2014, 2 (08)
[7]   Nonempirical dielectric-dependent hybrid functional with range separation for semiconductors and insulators [J].
Chen, Wei ;
Miceli, Giacomo ;
Rignanese, Gian-Marco ;
Pasquarello, Alfredo .
PHYSICAL REVIEW MATERIALS, 2018, 2 (07)
[8]   Accurate band gaps of extended systems via efficient vertex corrections in GW [J].
Chen, Wei ;
Pasquarello, Alfredo .
PHYSICAL REVIEW B, 2015, 92 (04)
[9]   First-principles determination of defect energy levels through hybrid density functionals and GW [J].
Chen, Wei ;
Pasquarello, Alfredo .
JOURNAL OF PHYSICS-CONDENSED MATTER, 2015, 27 (13)
[10]   Band-edge positions in GW: Effects of starting point and self-consistency [J].
Chen, Wei ;
Pasquarello, Alfredo .
PHYSICAL REVIEW B, 2014, 90 (16)