J. Semicond. > 2021, Volume 42 > Issue 5 > 050203
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RESEARCH HIGHLIGHTS

Defect engineering on all-inorganic perovskite solar cells for high efficiency

Bingcheng Yu1, 4, Chuantian Zuo2, Jiangjian Shi1, Qingbo Meng1, 3, 5, and Liming Ding2,

+ Author Affiliations

 Corresponding author: Qingbo Meng, qbmeng@iphy.ac.cn; Liming Ding, ding@nanoctr.cn

DOI: 10.1088/1674-4926/42/5/050203

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Perovskite solar cells based on organic–inorganic hybrid perovskite materials have become a research hotspot in photovoltaics field due to their outstanding power conversion efficiency (PCE)[1]. Nonetheless, the organic cations are volatile and have rotation freedom, which is not good for photo- and thermal-stability of the devices. Fortunately, these issues can be solved by all-inorganic perovskites, which consist of Cs, Pb and I (or Br)[2, 3]. Moreover, the all-inorganic perovskites, such as CsPbI3, are excellent candidates as top-cell absorbers in tandem solar cells because of their suitable bandgaps and high stability. All-inorganic perovskites were first used as light absorbers in solar cells in 2015[4, 5]. All-inorganic perovskite solar cells experienced rapid development in last few years, and the PCE reaches 20.4% at the end of 2020[6]. Most recently, Meng et al. pushed the PCE to >21.0% (unpublished). Despite these advances, we should recognize that there still remains a big gap between the PCEs for all-inorganic perovskite solar cells and hybrid perovskite solar cells (Fig. 1(a))[7, 8]. The PCE for hybrid cells has reached 80% of the theoretical limit, while the PCE for all-inorganic cells is still below 70% of the theoretical limit[9]. A detailed analysis on performance parameters of these cells suggests that the PCE for all-inorganic cells is mainly limited by the open-circuit voltage (Voc) and fill factor (FF) (Fig. 1(b)). In solar cells, these two parameters correlate to non-radiative charge loss caused by defects[10]. Therefore, defect engineering is the most critical approach for achieving higher PCE for all-inorganic perovskite solar cells.

Figure  1.  (Color online) (a) Efficiency evolution of organic–inorganic hybrid perovskite solar cells and all-inorganic perovskite solar cells. (b) Performance parameters of the current record-efficiency cells in comparison with Shockley-Queisser detailed-balance limit. (c) The defect transition levels of CsPbI3. Reproduced with permission[11], Copyright 2017, AIP publishing. (d) Effect of NH4I on the crystallization of CsPbI3. Reproduced with permission[13], Copyright 2021, WILEY-VCH. (e) Illustration of Mn2+ doping in CsPbBrI2. Reproduced with permission[15], Copyright 2018, American Chemical Society. (f) Illustration of the passivation effect of PN4N and PDCBT. Reproduced with permission[20], Copyright 2019, WILEY-VCH.
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Though CsPbI3 has similar bulk defects to that of hybrid perovskites (Fig. 1(c))[11], it presents more charge recombination and much shorter carrier lifetime. All-inorganic perovskites might have a higher degree of atom (or lattice) disorder and defect distribution because the crystals experience complicated phase transformation processes under relatively high temperature. Thus, improving the crystallization of all-inorganic perovskites is an effective approach to reduce the defects[6, 12, 13]. Recently, Seok et al. controlled the intermediate stages during the crystallization process by adding methyl ammonium chloride[6]. CsPbI3 films showed high crystallinity and good surface morphology. Thermally stimulated current test indicated that the defect density decreased from 3.947 × 1016 to 2.803 × 1016 cm–3. With surface passivation, CsPbI3 solar cells gave a PCE of 20.37%. At the same time, Meng et al. added NH4I into perovskite precursor solution to adjust the nucleation and crystallization, thus reducing the defects (Fig. 1(d))[13]. Thermal admittance spectroscopy showed that the charge capture in crossing the perovskite was reduced by about one order of magnitude. Recently, Meng et al. controlled perovskite crystallization by using coordination-active additives or synergistic additives, and the solar cells delivered a PCE of over 21.0%.

Another defect suppression strategy is element doping at the Pb site in perovskite. The 6s and 6p orbitals of Pb2+ significantly contribute to the energy band of CsPbX3 (X = Cl, Br and I) perovskites, and using divalent metal ions (i.e. Cu2+, Mn2+ and Sn2+) doping or alloying Pb sites will affect the defect tolerance[14]. Recently, Liu et al. found that Mn2+ incorporation could passivate the defects at the grain boundary and surface, thus reducing carrier recombination (Fig. 1(e))[15].

Surface passivation is widely used for enhancing the performance of all-inorganic perovskite solar cells[16]. Bulky organic ammonium halides, such as quaternary ammonium salt, were used to passivate the defects in hybrid perovskites. This method can also be used to passivate the surface defects of all-inorganic perovskites. In 2018, Zhao et al. treated CsPbI3 film with choline iodide to reduce surface defects[17]. Phenyltrimethylammonium halides and 3,3-diphenylpropylamine were used for surface passivation, accelerating the development of all-inorganic perovskite solar cells[18, 19]. The recently reported high PCE of 20.37% benefited from the surface passivation by octylammonium iodide[6]. Organic materials having Coulombic interaction with the terminal atoms of perovskites can be applied for surface or interface passivation. Ye et al. theoretically and experimentally proved that an amino-functionalized polymer and a dopant-free hole-transporting polymer can help passivating both the top and the bottom surface of CsPbI2Br films (Fig. 1(f))[20]. The numerous organic ligands synthesized for enhancing the luminescence of all-inorganic perovskite nanocrystals may be suitable for passivating perovskite surface and grain boundaries[21, 22].

In summary, all-inorganic perovskites have a complicated formation process and large lattice distortion caused by phase competition. Besides the top surface, more attention should be paid to passivating the defects at bottom surface and inside the bulk. Interface materials which can withstand high temperature should be developed to buffer the energy level mismatch, lattice mismatch, and interface stress between inorganic charge-transport layers and all-inorganic perovskites.

This work was supported by the National Natural Science Foundation of China (51872321, 11874402, 52072402, 51627803) and the National Key Research and Development Program of China (2018YFB1500101). L. Ding thanks the National Key Research and Development Program of China (2017YFA0206600) and the National Natural Science Foundation of China (51773045, 21772030, 51922032, 21961160720) for financial support.



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[6]
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Green M, Dunlop E, Hohl-Ebinger J, et al. Solar cell efficiency tables (version 57). Prog Photovolt Res Appl, 2021, 29, 3 doi: 10.1002/pip.3371
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Polman A, Knight M, Garnett E C, et al. Photovoltaic materials: present efficiencies and future challenges. Science, 2016, 352, aad4424 doi: 10.1126/science.aad4424
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Li Y, Zhang C, Zhang X, et al. Intrinsic point defects in inorganic perovskite CsPbI3 from first-principles prediction. Appl Phys Lett, 2017, 111, 162106 doi: 10.1063/1.5001535
[12]
Shang Y, Fang Z, Hu W, et al. Efficient and photostable CsPbI2Br solar cells realized by adding PMMA. J Semicond, 2021, 42, 050501 doi: 10.1088/1674-4926/42/5050501
[13]
Tan S, Shi J, Yu B, et al. Inorganic ammonium halide additive strategy for highly efficient and stable CsPbI3 perovskite solar cells. doi: 10.1002/adfm.202010813
[14]
Swarnkar A, Mir W J, Nag A. Can B-Site doping or alloying improve thermal- and phase-stability of all-Inorganic CsPbX3 (X = Cl, Br, I) perovskites. ACS Energy Lett, 2018, 3, 286 doi: 10.1021/acsenergylett.7b01197
[15]
Bai D, Zhang J, Jin Z, et al. Interstitial Mn2+-driven high-aspect-ratio grain growth for low-trap-density microcrystalline films for record efficiency CsPbI2Br solar cells. ACS Energy Lett, 2018, 3, 970 doi: 10.1021/acsenergylett.8b00270
[16]
Fang Z, Meng X, Zuo C, et al. Interface engineering gifts CsPbI2.25Br0.75 solar cells high performance. Sci Bull, 2019, 64, 1743 doi: 10.1016/j.scib.2019.09.023
[17]
Wang Y, Dar M I, Ono L K, et al. Thermodynamically stabilized β-CsPbI3-based perovskite solar cells with efficiencies > 18%. Science, 2019, 365, 591 doi: 10.1126/science.aav8680
[18]
Wang Y, Liu X, Zhang T, et al. The role of dimethylammonium iodine in CsPbI3 perovskite fabrication: additive or dopant. Angew Chem Int Ed, 2019, 58, 16691 doi: 10.1002/anie.201910800
[19]
Fang Z, Liu L, Zhang Z, et al. CsPbI2.25Br0.75 solar cells with 15.9% efficiency. Sci Bull, 2019, 64, 507 doi: 10.1016/j.scib.2019.04.013
[20]
Tian J, Xue Q, Tang X, et al. Dual interfacial design for efficient CsPbI2Br perovskite solar cells with improved photostability. Adv Mater, 2019, 31, 1901152 doi: 10.1002/adma.201901152
[21]
He X, Qiu Y, Yang S. Fully-inorganic trihalide perovskite nanocrystals: a new research frontier of optoelectronic materials. Adv Mater, 2017, 29, 1700775 doi: 10.1002/adma.201700775
[22]
Yang D, Li X, Zhou W, et al. CsPbBr3 quantum dots 2.0: benzenesulfonic acid equivalent ligand awakens complete purification. Adv Mater, 2019, 31, 1900767 doi: 10.1002/adma.201900767
Fig. 1.  (Color online) (a) Efficiency evolution of organic–inorganic hybrid perovskite solar cells and all-inorganic perovskite solar cells. (b) Performance parameters of the current record-efficiency cells in comparison with Shockley-Queisser detailed-balance limit. (c) The defect transition levels of CsPbI3. Reproduced with permission[11], Copyright 2017, AIP publishing. (d) Effect of NH4I on the crystallization of CsPbI3. Reproduced with permission[13], Copyright 2021, WILEY-VCH. (e) Illustration of Mn2+ doping in CsPbBrI2. Reproduced with permission[15], Copyright 2018, American Chemical Society. (f) Illustration of the passivation effect of PN4N and PDCBT. Reproduced with permission[20], Copyright 2019, WILEY-VCH.

DownLoad: Full-Size Img PowerPoint
[1]
Huang J, Yuan Y, Shao Y, et al. Understanding the physical properties of hybrid perovskites for photovoltaic applications. Nat Rev Mater, 2017, 2, 17042 doi: 10.1038/natrevmats.2017.42
[2]
Faheem M B, Khan B, Feng C, et al. All-Inorganic perovskite solar cells: energetics, key challenges, and strategies toward commercialization. ACS Energy Lett, 2020, 5, 290 doi: 10.1021/acsenergylett.9b02338
[3]
Jia X, Zuo C, Tao S, et al. CsPb(IxBr1– x)3 solar cells. Sci Bull, 2019, 64, 1532 doi: 10.1016/j.scib.2019.08.017
[4]
Eperon G E, Paterno G M, Sutton R J, et al. Inorganic caesium lead iodide perovskite solar cells. J Mater Chem A, 2015, 3, 19688 doi: 10.1039/C5TA06398A
[5]
Kulbak M, Cahen D, Hodes G. How important is the organic part of lead halide perovskite photovoltaic cells? Efficient CsPbBr3 cells. J Phys Chem Lett, 2015, 6, 2452 doi: 10.1021/acs.jpclett.5b00968
[6]
Yoon S, Min H, Kim J, et al. Surface engineering of ambient-air-processed cesium lead triiodide layers for efficient solar cells. Joule, 2021, 5, 183 doi: 10.1016/j.joule.2020.11.020
[7]
Ho-Baillie A, Zhang M, Lau C F J, et al. Untapped potentials of inorganic metal halide perovskite solar cells. Joule, 2019, 3, 938 doi: 10.1016/j.joule.2019.02.002
[8]
Green M, Dunlop E, Hohl-Ebinger J, et al. Solar cell efficiency tables (version 57). Prog Photovolt Res Appl, 2021, 29, 3 doi: 10.1002/pip.3371
[9]
Shockley W, Queisser H J. Detailed balance limit of efficiency of p-n junction solar cells. J Appl Phys, 1961, 32, 510 doi: 10.1063/1.1736034
[10]
Polman A, Knight M, Garnett E C, et al. Photovoltaic materials: present efficiencies and future challenges. Science, 2016, 352, aad4424 doi: 10.1126/science.aad4424
[11]
Li Y, Zhang C, Zhang X, et al. Intrinsic point defects in inorganic perovskite CsPbI3 from first-principles prediction. Appl Phys Lett, 2017, 111, 162106 doi: 10.1063/1.5001535
[12]
Shang Y, Fang Z, Hu W, et al. Efficient and photostable CsPbI2Br solar cells realized by adding PMMA. J Semicond, 2021, 42, 050501 doi: 10.1088/1674-4926/42/5050501
[13]
Tan S, Shi J, Yu B, et al. Inorganic ammonium halide additive strategy for highly efficient and stable CsPbI3 perovskite solar cells. doi: 10.1002/adfm.202010813
[14]
Swarnkar A, Mir W J, Nag A. Can B-Site doping or alloying improve thermal- and phase-stability of all-Inorganic CsPbX3 (X = Cl, Br, I) perovskites. ACS Energy Lett, 2018, 3, 286 doi: 10.1021/acsenergylett.7b01197
[15]
Bai D, Zhang J, Jin Z, et al. Interstitial Mn2+-driven high-aspect-ratio grain growth for low-trap-density microcrystalline films for record efficiency CsPbI2Br solar cells. ACS Energy Lett, 2018, 3, 970 doi: 10.1021/acsenergylett.8b00270
[16]
Fang Z, Meng X, Zuo C, et al. Interface engineering gifts CsPbI2.25Br0.75 solar cells high performance. Sci Bull, 2019, 64, 1743 doi: 10.1016/j.scib.2019.09.023
[17]
Wang Y, Dar M I, Ono L K, et al. Thermodynamically stabilized β-CsPbI3-based perovskite solar cells with efficiencies > 18%. Science, 2019, 365, 591 doi: 10.1126/science.aav8680
[18]
Wang Y, Liu X, Zhang T, et al. The role of dimethylammonium iodine in CsPbI3 perovskite fabrication: additive or dopant. Angew Chem Int Ed, 2019, 58, 16691 doi: 10.1002/anie.201910800
[19]
Fang Z, Liu L, Zhang Z, et al. CsPbI2.25Br0.75 solar cells with 15.9% efficiency. Sci Bull, 2019, 64, 507 doi: 10.1016/j.scib.2019.04.013
[20]
Tian J, Xue Q, Tang X, et al. Dual interfacial design for efficient CsPbI2Br perovskite solar cells with improved photostability. Adv Mater, 2019, 31, 1901152 doi: 10.1002/adma.201901152
[21]
He X, Qiu Y, Yang S. Fully-inorganic trihalide perovskite nanocrystals: a new research frontier of optoelectronic materials. Adv Mater, 2017, 29, 1700775 doi: 10.1002/adma.201700775
[22]
Yang D, Li X, Zhou W, et al. CsPbBr3 quantum dots 2.0: benzenesulfonic acid equivalent ligand awakens complete purification. Adv Mater, 2019, 31, 1900767 doi: 10.1002/adma.201900767
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    Bingcheng Yu, Chuantian Zuo, Jiangjian Shi, Qingbo Meng, Liming Ding. Defect engineering on all-inorganic perovskite solar cells for high efficiency[J]. Journal of Semiconductors, 2021, 42(5): 050203. doi: 10.1088/1674-4926/42/5/050203
    B C Yu, C T Zuo, J J Shi, Q B Meng, L M Ding, Defect engineering on all-inorganic perovskite solar cells for high efficiency[J]. J. Semicond., 2021, 42(5): 050203. doi: 10.1088/1674-4926/42/5/050203.
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    Received: 15 March 2021 Revised: Online: Accepted Manuscript: 15 March 2021Uncorrected proof: 15 March 2021Published: 01 May 2021

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      Article Navigation >  Journal of Semiconductors  > 2021  >  42(5): 050203
      Bingcheng Yu, Chuantian Zuo, Jiangjian Shi, Qingbo Meng, Liming Ding. Defect engineering on all-inorganic perovskite solar cells for high efficiency[J]. Journal of Semiconductors, 2021, 42(5): 050203. doi: 10.1088/1674-4926/42/5/050203 ****B C Yu, C T Zuo, J J Shi, Q B Meng, L M Ding, Defect engineering on all-inorganic perovskite solar cells for high efficiency[J]. J. Semicond., 2021, 42(5): 050203. doi: 10.1088/1674-4926/42/5/050203.
      Citation:
      Bingcheng Yu, Chuantian Zuo, Jiangjian Shi, Qingbo Meng, Liming Ding. Defect engineering on all-inorganic perovskite solar cells for high efficiency[J]. Journal of Semiconductors, 2021, 42(5): 050203. doi: 10.1088/1674-4926/42/5/050203 ****
      B C Yu, C T Zuo, J J Shi, Q B Meng, L M Ding, Defect engineering on all-inorganic perovskite solar cells for high efficiency[J]. J. Semicond., 2021, 42(5): 050203. doi: 10.1088/1674-4926/42/5/050203.
      shu

      Defect engineering on all-inorganic perovskite solar cells for high efficiency

      DOI: 10.1088/1674-4926/42/5/050203
      • 1.

        Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China

      • 2.

        Center for Excellence in Nanoscience (CAS), Key Laboratory of Nanosystem and Hierarchical Fabrication (CAS), National Center for Nanoscience and Technology, Beijing 100190, China

      • 3.

        Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China

      • 4.

        School of Physical Sciences, University of Chinese Academy of Sciences, Beijing 100049, China

      • 5.

        Songshan Lake Materials Laboratory, Dongguan 523808, China

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      • Bingcheng Yu：got his BS in Materials Science and Engineering from Hunan University in 2016. He is now a PhD candidate in Condensed Matter Physics at Institute of Physics (CAS) under the supervision of Professor Qingbo Meng. His research focuses on developing highly efficient all-inorganic perovskite optoelectronic devices
      • Chuantian Zuo：received his PhD degree in 2018 from National Center for Nanoscience and Technology (CAS) under the supervision of Professor Liming Ding. Then he did postdoctoral research at CSIRO, Australia. Currently, he is an assistant professor in Liming Ding Group. His research focuses on innovative materials and devices
      • Jiangjian Shi：obtained his PhD degree from Institute of Physics (CAS) in 2017. Now he is an associate professor at Institute of Physics. His research interests include investigation on charge carrier dynamics, interfacial charge transfer and surface modification in new generation solar cells
      • Qingbo Meng：received his PhD from Changchun Institute of Applied Chemistry (CAS) in 1997. Now he is a professor at Institute of Physics (CAS). His research focuses on solar energy materials and technologies as well as the research on dynamics of electron diffusion and charge recombination in solar cells
      • Liming Ding：got his PhD from University of Science and Technology of China (was a joint student at Changchun Institute of Applied Chemistry, CAS). He started his research on OSCs and PLEDs in Olle Inganäs Lab in 1998. Later on, he worked at National Center for Polymer Research, Wright-Patterson Air Force Base and Argonne National Lab (USA). He joined Konarka as a Senior Scientist in 2008. In 2010, he joined National Center for Nanoscience and Technology as a full professor. His research focuses on functional materials and devices. He is RSC Fellow, the nominator for Xplorer Prize, and the Associate Editors for Science Bulletin and Journal of Semiconductors
      • Corresponding author: qbmeng@iphy.ac.cn; ding@nanoctr.cn
      • Received Date: 2021-03-15
      • Published Date: 2021-05-10

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