First-Principles and BoltzTraP approach to the optoelectronic design of CuMCl3 (M = Ge, Sn) halide perovskites for Future energy devices
Source abstract
Abstract
Lead-free halide perovskites are emerging as sustainable alternatives to toxic Pb-based materials for energy conversion technologies. In this study, a comprehensive first-principles investigation combining density functional theory (DFT) and Boltzmann transport theory (BoltzTraP2) is employed to explore the structural, electronic, optical, and thermoelectric properties of novel Cu-based perovskites CuMCl 3 (M = Ge, Sn). Both compounds crystallise in a stable cubic phase (Pm-3 m) with negative formation energies (−2.96 and − 2.87 eV/atom) and exhibit ductile mechanical behaviour. Electronic calculations reveal direct band gaps of 0.70 eV (CuGeCl 3 ) and 0.91 eV (CuSnCl 3 ), confirming their suitability for optoelectronic applications. CuGeCl 3 exhibits a stronger optical response with a higher dielectric constant ( ( ) = 5.12) and absorption, whereas CuSnCl 3 displays lower reflectivity and a higher exciton binding energy (0.099 eV), making it suitable for LED and coating applications. Thermoelectric analysis identifies both materials as n -type semiconductors, with Seebeck coefficients around − 225 μV/K and maximum ZT values of 2.50 (CuGeCl 3 ) and 2.99 (CuSnCl 3 ) at 900 K, surpassing conventional thermoelectric benchmarks. These findings highlight CuGeCl 3 as a promising optoelectronic absorber and CuSnCl 3 as an efficient high-temperature thermoelectric material, offering multifunctional potential for next-generation energy and photonic devices.
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: Perovskite Materials and Applications · Thermal Expansion and Ionic Conductivity · Heusler alloys: electronic and magnetic properties
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (86)
Show source-provided references
1. Nazir, Abrar, Ejaz Ahmad Khera, Mumtaz Manzoor, Bandar Ali Al-Asbahi, Yedluri Anil Kumar, and Ramesh Sharma. “A Density Functional Theory Study of the Structural, Mechanical, Optoelectronics and Thermoelectric Properties of InGeX3 (X= F, Cl) Perovskites.” Polyhedron 257 (2024): 117009.10.1016/j.poly.2024.117009 ↗
2. Chu, Liang, Waqar Ahmad, Wei Liu, Jian Yang, Rui Zhang, Yan Sun, Jianping Yang, and Xing’ao Li. “Lead-Free Halide Double Perovskite Materials: A New Superstar toward Green and Stable Optoelectronic Applications.” Nano-Micro Letters 11, No. 1 (2019): 16.10.1007/s40820-019-0244-6 ↗
3. Yang, Woon Seok, Byung-Wook Park, Eui Hyuk Jung, Nam Joong Jeon, Young Chan Kim, Dong Uk Lee, Seong Sik Shin et al. “Iodide Management in Formamidinium-Lead-Halide–Based Perovskite Layers for Efficient Solar Cells.” Science 356, No. 6345 (2017): 1376-1379.10.1126/science.aan2301 ↗
4. Xing, Guichuan, Nripan Mathews, Shuangyong Sun, Swee Sien Lim, Yeng Ming Lam, Michael Grätzel, Subodh Mhaisalkar, and Tze Chien Sum. “Long-Range Balanced Electron-and Hole-Transport Lengths in Organic-Inorganic CH3NH3PbI3.” Science 342, No. 6156 (2013): 344-347.10.1126/science.1243167 ↗
5. Zhu, Haiming, Yongping Fu, Fei Meng, Xiaoxi Wu, Zizhou Gong, Qi Ding, Martin V. Gustafsson, M. Tuan Trinh, Song Jin, and X. Y. Zhu. “Lead Halide Perovskite Nanowire Lasers with Low Lasing Thresholds and High Quality Factors.” Nature Materials 14, No. 6 (2015): 636-642.10.1038/nmat4271 ↗
6. Cho, Himchan, Su-Hun Jeong, Min-Ho Park, Young-Hoon Kim, Christoph Wolf, Chang-Lyoul Lee, Jin Hyuck Heo et al. “Overcoming the Electroluminescence Efficiency Limitations of Perovskite Light-Emitting Diodes.” Science 350, No. 6265 (2015): 1222-1225.10.1126/science.aad1818 ↗
7. Chu, Liang, Ruiyuan Hu, Wei Liu, Yuhui Ma, Rui Zhang, Jian Yang, and Xing’ao Li. “Screen Printing Large-Area Organometal Halide Perovskite Thin Films for Efficient Photodetectors.” Materials Research Bulletin 98 (2018): 322-327.10.1016/j.materresbull.2017.10.039 ↗
8. Formamidinium Lead Bromide (FAPbBr3) Perovskite Microcrystals for Sensitive and Fast Photodetectors10.1007/s40820-018-0196-2 ↗
9. Chen, Qiushui, Jing Wu, Xiangyu Ou, Bolong Huang, Jawaher Almutlaq, Ayan A. Zhumekenov, Xinwei Guan et al. “All-Inorganic Perovskite Nanocrystal Scintillators.” Nature 561, No. 7721 (2018): 88-93.10.1038/s41586-018-0451-1 ↗
10. Make Perovskite Solar Cells Stable10.1038/544155a ↗
11. Bandgap‐tunable Cesium Lead Halide Perovskites with High thermal Stability for Efficient Solar Cells10.1002/aenm.201502458 ↗
12. Organometal Halide Perovskites as Visible-Light Sensitizers for Photovoltaic Cells10.1021/ja809598r ↗
13. Identifying Defect-Tolerant Semiconductors with High Minority-Carrier Lifetimes: beyond Hybrid Lead Halide Perovskites10.1557/mrc.2015.26 ↗
14. Sequential Deposition as a Route to High-Performance Perovskite-Sensitized Solar Cells10.1038/nature12340 ↗
15. High Efficiency Perovskite Solar Cells: from complex Nanostructure to Planar Heterojunction10.1039/C3TA14160H ↗
16. Semiconducting Tin and Lead Iodide Perovskites with Organic Cations: phase Transitions, High Mobilities, and near-Infrared Photoluminescent Properties10.1021/ic401215x ↗
17. Shi, Dong, Valerio Adinolfi, Riccardo Comin, Mingjian Yuan, Erkki Alarousu, Andrei Buin, Yin Chen et al. “Low Trap-State Density and Long Carrier Diffusion in Organolead Trihalide Perovskite Single Crystals.” Science 347, No. 6221 (2015): 519-522.10.1126/science.aaa2725 ↗
18. Tuning of the Thermoelectric figure of Merit of CH3NH3MI3 (M Pb, Sn) Photovoltaic Perovskites10.1021/acs.jpcc.5b03939 ↗
19. Toxicity of Organometal Halide Perovskite Solar Cells10.1038/nmat4572 ↗
20. Lead-Free Germanium Iodide Perovskite Materials for Photovoltaic Application10.1039/C5TA05741H ↗
21. Hall Mobility in Tin Iodide Perovskite CH3NH3SnI3: evidence for a Doped Semiconductor10.1016/j.jssc.2013.07.008 ↗
22. A DFT Study of Electronic, Optical and Thermoelectric Properties of Ge-Halide Perovskites CsGeX3 (X= F, Cl and Br)10.1016/j.cocom.2022.e00663 ↗
23. Electronic Band Structure, Phonons, and Exciton Binding Energies of Halide Perovskites CsSnCl3, CsSnBr3, and CsSnI3. Physical Review B—Condensed Matter and Materials
24. Electronic Structure of TlGeI3, TlSnI3, and TlPbI3: potential use for Spectroscopic Radiation Detection
25. CsSnI3: Semiconductor or Metal? High Electrical Conductivity and strong near-Infrared Photoluminescence from a Single Material. High Hole Mobility and Phase-Transitions10.1021/ja301539s ↗
26. Kaewmeechai, Chaiyawat, Yongyut Laosiritaworn, and Atchara Punya Jaroenjittichai. “Electronic Structure of Nontoxic-Inorganic Perovskite: CsMgBr3 Using DFT Calculation.” In Journal of Physics: Conference Series, Vol. 1380, No. 1, p. 012112. IOP Publishing, 2019.10.1088/1742-6596/1380/1/012112 ↗
27. Nanostructured Bi2Se3 Films and their Thermoelectric Transport Properties
28. Simultaneous Enhancement of Thermoelectric Performance and Mechanical Properties in Bi2Te3 via Ru Compositing10.1016/j.cej.2020.126407 ↗
29. Poudel, Bed, Qing Hao, Yi Ma, Yucheng Lan, Austin Minnich, Bo Yu, Xiao Yan et al. “High-Thermoelectric Performance of Nanostructured Bismuth Antimony Telluride Bulk Alloys.” Science 320, No. 5876 (2008): 634-638.10.1126/science.1156446 ↗
30. Cubic PbGeO3 Perovskite Oxide: a compound with striking Electronic, Thermoelectric and Optical Properties, Explored using DFT Studies10.1016/j.cocom.2020.e00532 ↗
31. Study of Optoelectronic and Thermoelectric Properties of BaSiO3 Perovskite under Moderate pressure for Energy Renewable Devices applications10.1016/j.jpcs.2018.04.024 ↗
32. The First-Principle Study of Mechanical, Optical and Thermoelectric Properties of SnZrO3 and SnHfO3 for Renewable Energy applications10.1016/j.ssc.2019.01.011 ↗
33. First Principle Studies on Structural, Electronic, Elastic, Optical, and Thermoelectric Properties of XGeCl3 (X= Rb/Cs): Promising Compounds for Green Energy Application10.1002/qua.27342 ↗
34. Nazir, Abrar, Refka Ghodhbani, Ejaz Ahmad Khera, Mumtaz Manzoor, Sabirov Sardor, Abdulla Hayitov, Ramesh Sharma, and Imed Boukhris. “Probing the Physical Attributes of Calcium-Based Perovskites for ACaI3 (A= Li and Na) Perovskites for next-Generation Renewable Energy Devices via TB-mBJ Approach.” Journal of Electroceramics (2025): 1-19.10.1007/s10832-025-00415-y ↗
35. Chen, Haijie, Joao M. Pina, Fanglong Yuan, Andrew Johnston, Dongxin Ma, Bin Chen, Ziliang Li et al. “Multiple Self-Trapped Emissions in the Lead-Free Halide Cs3Cu2I5.” The Journal of Physical Chemistry Letters 11, No. 11 (2020): 4326-4330.10.1021/acs.jpclett.0c01166 ↗
36. Strongly Emissive Lead‐free 0D Cs3Cu2I5 Perovskites Synthesized by a Room Temperature Solvent Evaporation Crystallization for Down‐conversion Light‐emitting Devices and Fluorescent Inks10.1002/adom.201901723 ↗
37. Li, Ying, Zhifeng Shi, Wenqing Liang, Lintao Wang, Sen Li, Fei Zhang, Zhuangzhuang Ma et al. “Highly Stable and Spectrum-Selective Ultraviolet Photodetectors Based on Lead-Free Copper-Based Perovskites.” Materials Horizons 7, No. 2 (2020): 530-540.10.1039/C9MH01371G ↗
38. Opportunity of the Lead-Free All-Inorganic Cs3Cu2I5 Perovskite Film for Memristor and Neuromorphic Computing applications10.1021/acsami.0c03106 ↗
39. Xu, Qiang, Juan Wang, Qindong Zhang, Xiao Ouyang, Maheng Ye, Weiting Xie, Xuewen Yan et al. “Solution-Processed Lead-Free Bulk 0D Cs3Cu2I5 Single Crystal for Indirect Gamma-Ray Spectroscopy Application.” Photonics Research 9, No. 3 (2021): 351-356.10.1364/PRJ.412959 ↗
40. Air-Stable Bulk Halide Single-Crystal Scintillator Cs3Cu2I5 by Melt Growth: Intrinsic and Tl Doped with High Light Yield10.1021/acsami.0c09047 ↗
41. Mn2+ Induced significant Improvement and Robust Stability of Radioluminescence in Cs3Cu2I5 for High-Performance Nuclear Battery10.1038/s41467-021-24185-7 ↗
42. Asker, Ceyla, Candida Pipitone, Federica Ursi, Kan Chen, Antonio Gaetano Ricciardulli, Eugenio S. Suena Galindez, Sally Luong et al. “Doping and Thermoelectric Properties of the Zero-Dimensional Inorganic Halide Perovskite Derivative, Cs3Cu2I5.” Journal of Materials Chemistry A 13, No. 31 (2025): 26009-26018.10.1039/D5TA02695D ↗
43. Systematic Study of Spin Dependent Electronic, Mechanical, Optoelectronic and Thermoelectric Properties of Halide double Perovskites K2CuCrZ6 (Z= Cl, Br): DFT-Calculations10.1016/j.jpcs.2024.112474 ↗
44. DFT-Based Modelling of Optoelectronic, Thermodynamic and Thermoelectric Properties in Copper-based Perovskites CuMCl3 (M: Ca and Sr) for Thermoelectric applications10.1142/S0129183127500045 ↗
45. Blaha · “Wien2k”. an Augmented Plane Wave+ Local Orbitals Program for Calculating Crystal Properties · 2001 · 60 · 155
46. “Improving the Modified Becke-Johnson Exchange potential.” Physical Review B—Condensed Matter and Materials
47. Segall, M. D., Philip JD Lindan, MJ al Probert, Christopher James Pickard, Philip James Hasnip, S. J. Clark, and M. C. Payne. “First-Principles Simulation: Ideas, Illustrations and the CASTEPcode.” Journal of Physics: Condensed Matter 14, No. 11 (2002): 2717.10.1088/0953-8984/14/11/301 ↗
48. The Elastic Behaviour of a Crystalline Aggregate10.1088/0370-1298/65/5/307 ↗
49. Cesium-based Perovskite Hydrides: a Theoretical Insight into Hydrogen Storage and Optoelectronic Characteristics
50. Elastic Constants versus Melting Temperature in Metals10.1016/0036-9748(84)90267-9 ↗
51. The thermal Conductivity of Nonmetallic Crystals10.1016/S0081-1947(08)60359-8 ↗
52. AbstAb-Initio Insights into the Elastic, Bonding, Phonon, Optoelectronic and Thermophysical Properties of SnTaS2
53. Theory of Heat Conduction in Rare-Gas Crystals10.1103/PhysRev.137.A128 ↗
54. Materials selection guidelines for Low thermal Conductivity thermal Barrier Coatings
55. Ali, Farooq, Mazia Asghar, Hafiza Sumaira Waheed, Hamid Ullah, M. Junaid Iqbal Khan, Ghiyas Anwar, Mehran Amin, Saikh Mohammad Wabaidur, and Young-Han Shin. “Optoelectronic and Thermoelectric Response of Lead Free Halide Double Perovskites Rb2AgPX6 (X= Cl, Br, I) for Energy Storage Applications.” Optical and Quantum Electronics 56, No. 7 (2024): 1094.10.1007/s11082-024-07005-2 ↗
56. Scheidemantel, T. J., C. Ambrosch-Draxl, Timo Thonhauser, J. V. Badding, and Jorge O. Sofo. “Transport Coefficients from First-Principles Calculations.” Physical Review B 68, No. 12 (2003): 125210.10.1103/PhysRevB.68.125210 ↗
57. VESTA 3 for Three-Dimensional Visualization of Crystal, Volumetric and Morphology Data10.1107/S0021889811038970 ↗
58. Structural, Electronic and Optical Properties of CsPbX3 (X= Cl, Br, I) for Energy Storage and Hybrid Solar Cell applications10.1016/j.jallcom.2017.02.147 ↗
59. Md Saiduzzaman, and Minhajul Islam. “Tailoring the Physical Properties of InSnX3 (X= F, Cl) Perovskites via pressure: a Path toward Sustainable Optoelectronics.10.1016/j.chemphys.2025.112635 ↗
60. Dynamic Tuning of Optoelectronic and Mechanical Properties in TlMCl3 (M= Ge, Sn) under Pressure-Induced phase transition10.1016/j.heliyon.2025.e42603 ↗
61. Rehman, Jalil Ur, Muhammad Usman, Sana Amjid, Muhammad Sagir, M. Bilal Tahir, Abid Hussain, Iftikhar Alam et al. “First-Principles Calculations to Investigate Structural, Electronics, Optical and Elastic Properties of Sn-Based Inorganic Halide-Perovskites CsSnX3 (X= I, Br, Cl) for Solar Cell Applications.” Computational and Theoretical Chemistry 1209 (2022): 113624.10.1016/j.comptc.2022.113624 ↗
62. Rony, Jahid Kabir, Minhajul Islam, Md Saiduzzaman, Khandaker Monower Hossain, Safin Alam, Arpon Biswas, M. H. Mia, Sohail Ahmad, and S. K. Mitro. “TlBX3 (B= Ge, Sn; X= Cl, Br, I): Promising Non-Toxic Metal Halide Perovskites for Scalable and Affordable Optoelectronics.” Journal of Materials Research and Technology 29 (2024): 897-909.10.1016/j.jmrt.2024.01.093 ↗
63. Nature of the Band Gap of Halide Perovskites ABX3 (A= CH3NH3, Cs; B= Sn, Pb; X= Cl, Br, I): First-Principles Calculations10.1088/1674-1056/24/11/116302 ↗
64. The Mössbauer effect in Tin (II) Compounds. Part XI. the Spectra of Cubic Trihalogenostannates (II)10.1039/J19710003105 ↗
65. Chiarella, Fabio, Andrea Zappettini, Francesca Licci, Ivo Borriello, Giovanni Cantele, Domenico Ninno, Antonio Cassinese, and Ruggero Vaglio. “Combined Experimental and Theoretical Investigation of Optical, Structural, and Electronic Properties of CH3NH3SnX3 Thin Films (X= Cl, Br).” Physical Review B—Condensed Matter and Materials Physics 77, No. 4 (2008): 045129.10.1103/PhysRevB.77.045129 ↗
66. Ti2PTe2 Chalcogenide: a Comprehensive DFT Study on Physical Properties10.1016/j.nxmate.2024.100434 ↗
67. First-Principle Insights of Electronic and Optical Properties of Cubic Organic–Inorganic Mage x Pb(1–x) I3 Perovskites for Photovoltaic applications10.1021/acs.jpcc.8b08436 ↗
68. Necessary and Sufficient Elastic Stability Conditions in Various Crystal Systems10.1103/PhysRevB.90.224104 ↗
69. Shakoor, Abdul, Bakhtiar Ul Haq, Sikandar Azam, Fakhra Ghafoor, Muhammad Saqib, Muhammad Waqas, H. W. Seo, and Muhammad Jawad. “DFT Investigation of Structural, Electronic, Optical, Mechanical, and Thermoelectric Properties of Halide Perovskites XZnCl3 (X= Ag, Au, Cu).” Physica B: Condensed Matter (2025): 417309.10.1016/j.physb.2025.417309 ↗
70. Huang, Tengcheng, Zheyu Zhang, Baoyun Liang, Ang Li, Xin Xu, Yujia Gao, Zhuxia Wu et al. “The Stability of CsGeX3 (X= I, Br, Cl) Selectively Tuned by the Crystal Structures and Halide Ions as Inferred from the Calculated Phonon Spectrum.” Physical Chemistry Chemical Physics 27, No. 1 (2025): 232-239.10.1039/D4CP02988G ↗
71. Wave-Number-Dependent Dielectric Function of Semiconductors10.1103/PhysRev.128.2093 ↗
72. Narrowing Bandgap and Enhanced Mechanical and Optoelectronic Properties of Perovskite Halides: Effects of Metal Doping
73. Md Rasidul Islam, and Md Masud Rana. “a DFT and AIMD Study on the Physical and Optoelectronic Properties of Novel A3PF3 (A= Ca, Sr, and Ba) Perovskites for Energy Harvesting applications.
74. Brinkmann, Matthias, Joseph Hayden, Martin Letz, Steffen Reichel, Carol Click, Wolfgang Mannstadt, Bianca Schreder et al. “Optical Materials and Their Properties.” In Springer Handbook of Lasers and Optics, Pp. 249-372. Springer, New York, NY, 2007.10.1007/978-0-387-30420-5_5 ↗
75. Tuning of Direct Bandgap of Rb2ScTlX6 (X= Cl, Br, I) double Perovskites through Halide Ion Substitution for Solar Cell Devices10.1016/j.jmrt.2022.05.082 ↗
76. Hasan, Md Mehedi, Md Amran Sarker, Md Rabbi Talukder, Moshina Binte Mansur, Md Rasidul Islam, and Sohail Ahmad. “Exploring Pressure-Driven Semiconducting to Metallic Phase Transition in Lead-Free InGeX3 (X= F, Cl) Perovskites with Tunable Optoelectronic and Mechanical Properties via DFT.” Physica B: Condensed Matter 705 (2025): 417083.10.1016/j.physb.2025.417083 ↗
77. Density Functional Study of Cubic, Tetragonal, and Orthorhombic CsPbBr3 Perovskite10.1021/acsomega.0c00197 ↗
78. Influence of Halide Composition on the Structural, Electronic, and Optical Properties of mixed CH3NH3Pb(I 1–x Br x)3 Perovskites calculated using the Virtual Crystal Approximation Method10.1103/PhysRevB.94.125139 ↗
79. Advancements in Perovskite Solar Cells: Photophysics behind the Photovoltaics10.1039/C4EE00673A ↗
80. An Introduction to the Theory of the Boltzmann Equation
81. BoltzTraP2, a program for Interpolating Band Structures and calculating Semi-Classical Transport Coefficients10.1016/j.cpc.2018.05.010 ↗
82. A Review on Fundamentals, Design and Optimization to High ZT of Thermoelectric Materials for Application to Thermoelectric Technology10.1007/s11664-021-09153-7 ↗
83. Thermoelectric Properties of KCaF310.1016/j.physb.2019.04.019 ↗
84. A DFT Manifestation of the Physical, Thermodynamic and Thermoelectric Properties in Sn-based Halide Perovskites10.1016/j.inoche.2024.113573 ↗
85. The Optoelectronic and Thermoelectric Properties of PrTl2InX4 (X= Se, Te) Chalcogenides: for Energy Harvesting applications10.1016/j.inoche.2025.115406 ↗
86. Alharbi, Safia Abdullah R., Banat Gul, Muhammad Salman Khan, and Siti Maisarah Aziz. “Li-Based Ternary Semiconductors: Probing Electronic, Mechanical, Optical, and Transport Nature from First Principles Study.” Micro and Nanostructures (2025): 208357.10.1016/j.micrna.2025.208357 ↗