Mixed-Halide Perovskite Alloys CsPb(I1–xBrx)3 and CsPb(Br1–xClx)3: New Insight of Configurational Entropy Effect from First-Principles and Phase Diagrams
Source abstract
Abstract
Stability is one of the key issues in mixed-halide perovskite alloys that are promising in emergent optoelectronics. Previous density functional theory (DFT) and machine learning studies indicate that the formation-energy convex hulls of these materials are very shallow, and stable alloy compositions are rare. In this work, we revisit this problem using DFT, with a special focus on the effects of configurational and vibrational entropies. Allowed by the 20-atomic models for the C s P b ( I 1 − x B r x ) 3 and C s P b ( B r 1 − x C l x ) 3 series, the partition functions and therewith thermodynamic state functions are calculated by traversing all possible mixed-halide configurations. We can thus evaluate the temperature- and system-dependent configurational entropy, which largely corrects the conventional approach based on the ideal solution model. Finally, temperature–composition phase diagrams that include α, β, γ, and δ phases of both alloys are constructed based on the free energy data, for which the contribution of phonon vibrations is included.
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: Perovskite Materials and Applications · Thermal Expansion and Ionic Conductivity · Advanced Thermoelectric Materials and Devices
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
State Key Laboratory for Manufacturing Systems Engineering; Electronic Materials Research Laboratory, Key Laboratory of the Ministry of Education, School of Electronic Science and Engineering, Xi’an Jiaotong University, Xi’an 710049, China
Key Laboratory for Physical Electronics and Devices of the Ministry of Education and Shaanxi Key Lab of Information Photonic Technique, School of Electronic Science and Engineering, Xi’an Jiaotong University, Xi’an 710049, China
State Key Laboratory for Manufacturing Systems Engineering & International Joint Laboratory for Micro/Nano Manufacturing and Measurement Technology, Xi’an Jiaotong University, Xi’an 710049, China
Department of Chemistry and 4D LABORATORIES, Simon Fraser University, Burnaby, British Columbia V5A 1S6, Canada
MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, China
Funding
National Natural Science Foundation of China · Natural Science Foundation of Shaanxi Province
References (68)
Show source-provided references
1. National Renewable Energy Laboratory. Best Research-Cell Efficiency Chart. https://www.nrel.gov/pv/cell-efficiency.html (accessed Mar 29, 2024).
2. 10.1021/accountsmr.3c0006810.1021/accountsmr.3c00068 ↗
3. 10.1021/acsenergylett.3c0164910.1021/acsenergylett.3c01649 ↗
4. 10.1002/adfm.20190200810.1002/adfm.201902008 ↗
5. 10.1038/s41563-020-0784-710.1038/s41563-020-0784-7 ↗
6. 10.1038/s41928-022-00745-710.1038/s41928-022-00745-7 ↗
7. 10.1039/C7EE01674C10.1039/C7EE01674C ↗
8. 10.1039/C8EE03559H10.1039/C8EE03559H ↗
9. 10.1002/adma.20180533710.1002/adma.201805337 ↗
10. 10.1021/acsmaterialslett.1c0047410.1021/acsmaterialslett.1c00474 ↗
11. 10.1016/j.cej.2021.13270110.1016/j.cej.2021.132701 ↗
12. 10.1039/c6ee03397k10.1039/c6ee03397k ↗
13. 10.1126/science.aam632310.1126/science.aam6323 ↗
14. 10.1126/science.aah506510.1126/science.aah5065 ↗
15. 10.1002/aenm.20180375410.1002/aenm.201803754 ↗
16. 10.1016/j.mattod.2017.03.02110.1016/j.mattod.2017.03.021 ↗
17. 10.1038/s41566-018-0260-y10.1038/s41566-018-0260-y ↗
18. 10.1002/adma.20180583610.1002/adma.201805836 ↗
19. 10.1063/1.514410110.1063/1.5144101 ↗
20. 10.1038/s41467-020-20582-610.1038/s41467-020-20582-6 ↗
21. 10.1016/j.matt.2021.01.00810.1016/j.matt.2021.01.008 ↗
22. 10.1063/1.173603410.1063/1.1736034 ↗
23. 10.1021/acsenergylett.7b0119710.1021/acsenergylett.7b01197 ↗
24. 10.1021/acsenergylett.1c0063610.1021/acsenergylett.1c00636 ↗
25. 10.1007/s11433-022-2020-510.1007/s11433-022-2020-5 ↗
26. 10.1016/j.matre.2021.10006410.1016/j.matre.2021.100064 ↗
27. 10.1021/acs.jpclett.8b0319410.1021/acs.jpclett.8b03194 ↗
28. 10.1021/jz501896w10.1021/jz501896w ↗
29. 10.1103/PhysRevMaterials.2.04540110.1103/PhysRevMaterials.2.045401 ↗
30. 10.1021/acs.chemmater.8b0532910.1021/acs.chemmater.8b05329 ↗
31. 10.1103/PhysRevMaterials.6.11380110.1103/PhysRevMaterials.6.113801 ↗
32. 10.1039/c5ee03255e10.1039/c5ee03255e ↗
33. 10.1039/C9CP03656C10.1039/C9CP03656C ↗
34. 10.1002/adma.20210364010.1002/adma.202103640 ↗
35. 10.1002/adma.20230216110.1002/adma.202302161 ↗
36. 10.1016/j.msea.2003.10.25710.1016/j.msea.2003.10.257 ↗
37. 10.1016/j.intermet.2014.06.00410.1016/j.intermet.2014.06.004 ↗
38. 10.1038/ncomms948510.1038/ncomms9485 ↗
39. 10.1038/s41586-023-06786-y10.1038/s41586-023-06786-y ↗
40. 10.1021/acs.jpclett.2c0118010.1021/acs.jpclett.2c01180 ↗
41. 10.1016/j.nanoen.2019.10424910.1016/j.nanoen.2019.104249 ↗
42. 10.1002/aenm.20200018310.1002/aenm.202000183 ↗
43. 10.1002/aenm.20220173310.1002/aenm.202201733 ↗
44. 10.1002/adfm.20230142510.1002/adfm.202301425 ↗
45. 10.1103/physrevb.99.10410510.1103/physrevb.99.104105 ↗
46. 10.1002/adfm.20210626410.1002/adfm.202106264 ↗
47. Li, J.; Pan, F.; Zhang, G.X.; Liu, Z.; Dong, H.; Wang, D.; Jiang, Z.; Ren, W.; Ye, Z.G.; Todorović, M.; Rinke, P. Structural Disorder by Octahedral Tilting in Inorganic Halide Perovskites: New Insight with Bayesian Optimization. 2023. arXiv.org Prepr, arXiv:2303.08426.
48. Marstrander A. · Mater. Fys. Medd. Dan. Vid. Selsk. · 1966 · 35 · 1
49. 10.1002/hlca.20200008010.1002/hlca.202000080 ↗
50. 10.1016/j.actamat.2022.11866110.1016/j.actamat.2022.118661 ↗
51. 10.1021/acs.jpclett.6b0000210.1021/acs.jpclett.6b00002 ↗
52. 10.1038/s41467-019-08610-610.1038/s41467-019-08610-6 ↗
53. 10.1103/PhysRevLett.100.13640610.1103/PhysRevLett.100.136406 ↗
54. 10.1016/j.cpc.2009.06.02210.1016/j.cpc.2009.06.022 ↗
55. 10.1016/j.jcp.2009.08.00810.1016/j.jcp.2009.08.008 ↗
56. 10.1088/1367-2630/14/5/05302010.1088/1367-2630/14/5/053020 ↗
57. 10.1016/j.cpc.2015.02.02110.1016/j.cpc.2015.02.021 ↗
58. 10.1021/acs.jpclett.7b0242310.1021/acs.jpclett.7b02423 ↗
59. 10.1103/PhysRevLett.119.14550110.1103/PhysRevLett.119.145501 ↗
60. 10.1063/5.003544810.1063/5.0035448 ↗
61. 10.1063/1.46605910.1063/1.466059 ↗
62. 10.1016/j.cpc.2015.01.00310.1016/j.cpc.2015.01.003 ↗
63. 10.1038/s41524-019-0175-210.1038/s41524-019-0175-2 ↗
64. 10.1016/j.scriptamat.2015.07.02110.1016/j.scriptamat.2015.07.021 ↗
65. 10.7566/JPSJ.92.01200110.7566/JPSJ.92.012001 ↗
66. 10.1002/advs.20190080810.1002/advs.201900808 ↗
67. 10.1038/s41524-017-0048-510.1038/s41524-017-0048-5 ↗
68. 10.1557/mrs.2018.20810.1557/mrs.2018.208 ↗