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2. High-throughput Computational Study of Halide Double Perovskite Inorganic Compounds

Author

Cai, Yao, Xie, Wei, Teng, Yin Ting, Harikesh, PC, Ghosh, Biplab, Huck, Patrick, Persson, Kristin A, Mathews, Nripan, Mhaisalkar, Subodh G, Sherburne, Matthew, and Asta, Mark

Subjects
Macromolecular and Materials Chemistry, Chemical Sciences, Physical Chemistry, Engineering, Materials, Chemical sciences
Abstract

Double perovskite halides are a class of materials with diverse chemistries that are amenable to solution-based synthesis routes, and display a range of properties for a variety of potential applications. Starting from a consideration of the octahedral and tolerance factors of ∼2000 candidate double perovskite compounds, we compute structural, electronic, and transport properties of ∼1000 using first-principles calculations based on density-functional-theory methods. The computational results have been assembled in a database that is accessible through the Materials Project online. As one potential application, double perovskites are candidates in the search for lead-free halide photovoltaic absorbers. We present the application of our database to aid the discovery of new double perovskite halide photovoltaic materials, by combining the results with optical absorption and phonon stability calculations. From three distinct classes of chemistries, 11 compounds were identified as promising solar absorbers and the complex chemical trends for band gap within each of these are analyzed, to provide guidelines for the use of substitutional alloying as a means of further tuning the electronic structure. Other possible applications of the database are also discussed.

Published
2019

3. Computational Study of Halide Perovskite-Derived A$_2$BX$_6$ Inorganic Compounds: Chemical Trends in Electronic Structure and Structural Stability

Author

Cai, Yao, Xie, Wei, Ding, Hong, Chen, Yan, Krishnamoorthy, Thirumal, Wong, Lydia H., Mathews, Nripan, Mhaisalkar, Subodh G., Sherburne, Matthew, and Asta, Mark

Subjects
Condensed Matter - Materials Science
Abstract

The electronic structure and energetic stability of A$_2$BX$_6$ halide compounds with the cubic and tetragonal variants of the perovskite-derived K$_2$PtCl$_6$ prototype structure are investigated computationally within the frameworks of density-functional-theory (DFT) and hybrid (HSE06) functionals. The HSE06 calculations are undertaken for seven known A$_2$BX$_6$ compounds with A = K, Rb and Cs, and B = Sn, Pd, Pt, Te, and X = I. Trends in band gaps and energetic stability are identified, which are explored further employing DFT calculations over a larger range of chemistries, characterized by A = K, Rb, Cs, B = Si, Ge, Sn, Pb, Ni, Pd, Pt, Se and Te and X = Cl, Br, I. For the systems investigated in this work, the band gap increases from iodide to bromide to chloride. Further, variations in the A site cation influences the band gap as well as the preferred degree of tetragonal distortion. Smaller A site cations such as K and Rb favor tetragonal structural distortions, resulting in a slightly larger band gap. For variations in the B site in the (Ni, Pd, Pt) group and the (Se, Te) group, the band gap increases with increasing cation size. However, no observed chemical trend with respect to cation size for band gap was found for the (Si, Sn, Ge, Pb) group. The findings in this work provide guidelines for the design of halide A$_2$BX$_6$ compounds for potential photovoltaic applications.

Published
2017

6. Weakly Confined Organic–Inorganic Halide Perovskite Quantum Dots as High-Purity Room-Temperature Single Photon Sources

Author

Wang, Bo, primary, Lim, Jia Wei Melvin, additional, Loh, Siow Mean, additional, Mayengbam, Rishikanta, additional, Ye, Senyun, additional, Feng, Minjun, additional, He, Huajun, additional, Liang, Xiao, additional, Cai, Rui, additional, Zhang, Qiannan, additional, Kwek, Leong-Chuan, additional, Demir, Hilmi Volkan, additional, Mhaisalkar, Subodh G., additional, Blundell, Steven A., additional, and Chien Sum, Tze, additional

Published
2024
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8. Recent advancements and perspectives on light management and high performance in perovskite light-emitting diodes

Author

Kar Shaoni, Jamaludin Nur Fadilah, Yantara Natalia, Mhaisalkar Subodh G., and Leong Wei Lin

Subjects
light emission, light-emitting diode, light outcoupling, perovskite, Physics, QC1-999
Abstract

Perovskite semiconductors have experienced meteoric rise in a variety of optoelectronic applications. With a strong foothold on photovoltaics, much focus now lies on their light emission applications. Rapid progress in materials engineering have led to the demonstration of external quantum efficiencies that surpass the previously established theoretical limits. However, there remains much scope to further optimize the light propagation inside the device stack through careful tailoring of the optical processes that take place at the bulk and interface levels. Photon recycling in the emitter material followed by efficient outcoupling can result in boosting external efficiencies up to 100%. In addition, the poor ambient and operational stability of these materials and devices restrict further commercialization efforts. With best operational lifetimes of only a few hours reported, there is a long way to go before perovskite LEDs can be perceived as reliable alternatives to more established technologies like organic or quantum dot-based LED devices. This review article starts with the discussions of the mechanism of luminescence in these perovskite materials and factors impacting it. It then looks at the possible routes to achieve efficient outcoupling through nanostructuring of the emitter and the substrate. Next, we analyse the instability issues of perovskite-based LEDs from a photophysical standpoint, taking into consideration the underlying phenomena pertaining to defects, and summarize recent advances in mitigating the same. Finally, we provide an outlook on the possible routes forward for the field and propose new avenues to maximally exploit the excellent light-emitting capabilities of this family of semiconductors.

Published
2021
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11. Enhancing FAPbI3 perovskite solar cell performance with a methanesulfonate-based additive

Author

Foong, Japheth Joseph Yeow Wan, primary, Dewi, Herlina Arianita, additional, Zhumekenov, Ayan A., additional, Febriansyah, Benny, additional, Bruno, Annalisa, additional, Salim, Teddy, additional, Tay, Darrell Jun Jie, additional, Abuzeid, Hesham R., additional, Koh, Teck Ming, additional, Mhaisalkar, Subodh G., additional, and Mathews, Nripan, additional

Published
2024
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12. Solution‐Processed, Highly Crystalline and Oriented MAPbI3 Thin Films by Engineering Crystal Growth Kinetics

Author

Ahmad, Riyas, primary, Buenconsejo, Pio John S., additional, Lim, Ming Pin Alan, additional, Harikesh, P.C., additional, Sugathan, Vipinraj, additional, Haselsberger, Reinhard, additional, Koh, Teck Ming, additional, Leong, Wei Lin, additional, Mathews, Nripan, additional, Bruno, Annalisa, additional, Michel-Beyerle, Maria-Elisabeth, additional, and Mhaisalkar, Subodh G., additional

Published
2023
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18. Solution-Processed, Highly Crystalline, and Oriented MAPbI3 Thin Films by Engineering Crystal-Growth Kinetics.

Author

Ahmad, Riyas, Buenconsejo, Pio John S., Alan Lim, Ming Pin, Harikesh, Padinhare Cholakkal, Sugathan, Vipinraj, Haselsberger, Reinhard, Koh, Teck Ming, Wei Lin Leong, Mathews, Nripan, Bruno, Annalisa, Michel-Beyerle, Maria-Elisabeth, and Mhaisalkar, Subodh G.

Subjects
THIN films, PHOTOVOLTAIC cells, OPTOELECTRONIC devices, EPITAXY, LEAD halides, SOLAR cells
Abstract

Growing oriented and monocrystalline layers of lead halide perovskites over device substrates helps to harness their outstanding optoelectronic properties. Epitaxial growth of lead halide perovskites for device fabrication is limited by the lack of lattice-matched substrates and the requirement of compact pinhole-free films. Most optoelectronic devices use amorphous substrates, hindering oriented epitaxial growth. Herein, highly crystalline methylammonium lead iodide (MAPbI3) thin films over amorphous substrates are demonstrated by meticulously optimizing the nucleation and growth kinetics in spin-coating. The "epitaxial-like" films enable large-area crystalline layer fabrication, with larger than 100 μm spherulitic grains oriented along [200] and [224] planes. The compact, highly crystalline, and oriented films of MAPbI3 formed over indium tin oxide/SnO2 are used to fabricate perovskite solar cells (PSCs) with an area of 1 cm². Despite the perovskite films being highly oriented and crystalline, the PSCs' performances highlight the critical role the interfaces play in photovoltaic cells. [ABSTRACT FROM AUTHOR]

Published
2024
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19. Molecular Locking with All‐Organic Surface Modifiers Enables Stable and Efficient Slot‐Die Coated Methyl‐Ammonium‐Free Perovskite Solar Modules

Author

Rana, Prem Jyoti Singh, primary, Febriansyah, Benny, additional, Koh, Teck Ming, additional, Kanwat, Anil, additional, Xia, Junmin, additional, Salim, Teddy, additional, Hooper, Thomas J. N., additional, Kovalev, Mikhail, additional, Giovanni, David, additional, Aw, Yeow Chong, additional, Chaudhary, Bhumika, additional, Cai, Yongqing, additional, Xing, Guichuan, additional, Sum, Tze Chien, additional, Ager, Joel W., additional, Mhaisalkar, Subodh G., additional, and Mathews, Nripan, additional

Published
2023
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20. Inorganic frameworks of low-dimensional perovskites dictate the performance and stability of mixed-dimensional perovskite solar cells

Author

Febriansyah, Benny, primary, Li, Yongxin, additional, Giovanni, David, additional, Salim, Teddy, additional, Hooper, Thomas J. N., additional, Sim, Ying, additional, Ma, Daphne, additional, Laxmi, Shoba, additional, Lekina, Yulia, additional, Koh, Teck Ming, additional, Shen, Ze Xiang, additional, Pullarkat, Sumod A., additional, Sum, Tze Chien, additional, Mhaisalkar, Subodh G., additional, Ager, Joel W., additional, and Mathews, Nripan, additional

Published
2023
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27. Alkali Additives Enable Efficient Large Area (>55 cm 2 ) Slot‐Die Coated Perovskite Solar Modules

Author

Rana, Prem Jyoti Singh, primary, Febriansyah, Benny, additional, Koh, Teck Ming, additional, Muhammad, Bening Tirta, additional, Salim, Teddy, additional, Hooper, Thomas J. N., additional, Kanwat, Anil, additional, Ghosh, Biplab, additional, Kajal, Priyanka, additional, Lew, Jia Haur, additional, Aw, Yeow Chong, additional, Yantara, Natalia, additional, Bruno, Annalisa, additional, Pullarkat, Sumod A., additional, Ager, Joel W., additional, Leong, Wei Lin, additional, Mhaisalkar, Subodh G., additional, and Mathews, Nripan, additional

Published
2022
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28. Ultrafast THz photophysics of solvent engineered triple-cation halide perovskites.

Author

Kumar, Abhishek, Priyadarshi, Anish, Shukla, Sudhanshu, Manjappa, Manukumara, Haur, Lew Jia, Mhaisalkar, Subodh G., and Singh, Ranjan

Subjects
THIN films, PEROVSKITE, SOLAR cells, METHYLAMMONIUM, CESIUM compounds
Abstract

Solution processed thin film organic-inorganic perovskites are key to the large scale manufacturing of next generation wafer scale solar cell devices. The high efficiency of the hybrid perovskite solar cells is derived mainly from the large carrier mobility and the charge dynamics of films, which heavily depend on the type of solvent used for the material preparation. Here, we investigate the nature of conduction and charge carrier dynamics of mixed organic-inorganic cations [methylammonium (MA), formamidinium (FA), and cesium (Cs)] along with the mixed halides [iodine (I) and bromine (Br)] perovskite material [Cs0.05(MA0.17FA0.83)0.95Pb(I0.83Br0.17)3] synthesized in different solvents using optical pump terahertz probe (OPTP) spectroscopy. Our findings reveal that carrier mobilities and diffusion lengths strongly depend on the type of solvent used for the preparation of the mixed cation perovskite film. The mixed cation perovskite film prepared using dimethylformamide/dimethylsulfoxide solvent shows greater mobility and diffusion length compared to γ-butyrolactone solvent. Our findings provide valuable insights to improve the charge carrier transport in mixed cation perovskites through solvent engineering. [ABSTRACT FROM AUTHOR]

Published
2018
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30. Reversible Photochromism in ⟨110⟩ Oriented Layered Halide Perovskite

Author

Kanwat, Anil, primary, Ghosh, Biplab, additional, Ng, Si En, additional, Rana, Prem J. S., additional, Lekina, Yulia, additional, Hooper, Thomas J. N., additional, Yantara, Natalia, additional, Kovalev, Mikhail, additional, Chaudhary, Bhumika, additional, Kajal, Priyanka, additional, Febriansyah, Benny, additional, Tan, Qi Ying, additional, Klein, Maciej, additional, Shen, Ze Xiang, additional, Ager, Joel W., additional, Mhaisalkar, Subodh G., additional, and Mathews, Nripan, additional

Published
2022
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33. One-Pot Synthesis and Structural Evolution of Colloidal Cesium Lead Halide–Lead Sulfide Heterostructure Nanocrystals for Optoelectronic Applications

Author

Jagadeeswararao, Metikoti, primary, Vashishtha, Parth, additional, Hooper, Thomas J. N., additional, Kanwat, Anil, additional, Lim, Jia Wei Melvin, additional, Vishwanath, Sujaya Kumar, additional, Yantara, Natalia, additional, Park, Taewook, additional, Sum, Tze Chien, additional, Chung, Dae Sung, additional, Mhaisalkar, Subodh G., additional, and Mathews, Nripan, additional

Published
2021
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34. Slot-die coated methylammonium-free perovskite solar cells with 18% efficiency

Author

Fievez, Mathilde, primary, Singh Rana, Prem Jyoti, additional, Koh, Teck Ming, additional, Manceau, Matthieu, additional, Lew, Jia Haur, additional, Jamaludin, Nur Fadilah, additional, Ghosh, Biplab, additional, Bruno, Annalisa, additional, Cros, Stéphane, additional, Berson, Solenn, additional, Mhaisalkar, Subodh G., additional, and Leong, Wei Lin, additional

Published
2021
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35. Dual Role of Cu‐Chalcogenide as Hole‐Transporting Layer and Interface Passivator for p–i–n Architecture Perovskite Solar Cell (Adv. Funct. Mater. 38/2021)

Author

Sadhu, Anupam, primary, Rai, Monika, additional, Salim, Teddy, additional, Jin, Xin, additional, Tan, Joel Ming Rui, additional, Leow, Shin Woei, additional, Ahmed, Mahmoud G., additional, Magdassi, Shlomo, additional, Mhaisalkar, Subodh G., additional, and Wong, Lydia Helena, additional

Published
2021
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38. Alkali Additives Enable Efficient Large Area (>55 cm2) Slot‐Die Coated Perovskite Solar Modules.

Author

Rana, Prem Jyoti Singh, Febriansyah, Benny, Koh, Teck Ming, Muhammad, Bening Tirta, Salim, Teddy, Hooper, Thomas J. N., Kanwat, Anil, Ghosh, Biplab, Kajal, Priyanka, Lew, Jia Haur, Aw, Yeow Chong, Yantara, Natalia, Bruno, Annalisa, Pullarkat, Sumod A., Ager, Joel W., Leong, Wei Lin, Mhaisalkar, Subodh G., and Mathews, Nripan

Subjects
PEROVSKITE, X-ray photoelectron spectroscopy, POTASSIUM ions, SOLAR cells, ALKALIES
Abstract

Typical fabrication methods for laboratory‐scale (<1 cm2) perovskite solar cells (PSCs) are undeniably not scalable and the control of crystallization of large‐area perovskite layer for commercial sized modules is also particularly challenging. Here, a seed‐assisted crystallization approach is demonstrated through addition of alkali salts, CsPbBr3 and KPb2Br5, to the perovskite precursor ink for enabling homogeneous and highly crystalline large‐area Cs0.15FA0.85Pb(I0.83Br0.17)3 (CsFA) perovskite films via scalable slot‐die coating technique. X‐ray photoelectron spectroscopy analysis reveals the segregation of potassium ions at SnO2/perovskite interface which serve as nucleation sites for the crystallization of perovskite layer. The uniformly slot‐die coated CsFA films (100 cm2) from the additives containing precursor inks possess larger grains with enhanced optoelectronic properties and the corresponding devices display higher reproducibility and consistency. A champion device efficiency of 18.94% under 1 sun illumination for slot‐die coated PSCs in n‐type/intrinsic/p‐type structure is demonstrated with improved stability with 82% of its initial efficiency tested at 65 °C for 1150 h. The slot‐die coated methylammonium‐free perovskite module with an active area of 57.5 cm2 shows an efficiency of 16.22% and retains 82% of its initial efficiency after 4800 h under 30% relative humidity without encapsulation. [ABSTRACT FROM AUTHOR]

Published
2022
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40. Precise Control of CsPbBr3 Perovskite Nanocrystal Growth at Room Temperature: Size Tunability and Synthetic Insights

Author

Brown, Alasdair A. M., primary, Vashishtha, Parth, additional, Hooper, Thomas J. N., additional, Ng, Yan Fong, additional, Nutan, Gautam V., additional, Fang, Yanan, additional, Giovanni, David, additional, Tey, Ju Nie, additional, Jiang, Liudi, additional, Damodaran, Bahulayan, additional, Sum, Tze Chien, additional, Pu, Suan Hui, additional, Mhaisalkar, Subodh G., additional, and Mathews, Nripan, additional

Published
2021
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