Article(id=1319726472412123280, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1319726426404803327, articleNumber=null, orderNo=null, doi=10.14062/j.issn.0454-5648.20240814, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1734883200000, receivedDateStr=2024-12-23, revisedDate=1741968000000, revisedDateStr=2025-03-15, acceptedDate=null, acceptedDateStr=null, onlineDate=1792576910354, onlineDateStr=2026-10-21, pubDate=1766160000000, pubDateStr=2025-12-20, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1792576910354, onlineIssueDateStr=2026-10-21, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1792576910354, creator=13701087609, updateTime=1792576910354, updator=13701087609, issue=Issue{id=1319726426404803327, tenantId=1146029695717560320, journalId=1263187385517883426, year='2025', volume='53', issue='12', pageStart='3433', pageEnd='3832', issueExtLink='null', onlineDate='null', pubDate='1766160000000', pubDateStr='2025-12-20', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1792576899386, creator='13701087609', updateTime=1792577516933, updator='13701087609', preIssue=null, nextIssue=null, articleTotal=null, ext={EN=IssueExt(id=1319729016953749818, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1319726426404803327, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1319729016953749819, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1319726426404803327, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null, downloadFileDto=null}, startPage=3729, endPage=3739, ext={EN=ArticleExt(id=1319726474224062609, articleId=1319726472412123280, tenantId=1146029695717560320, journalId=1263187385517883426, language=EN, title=Photoelectric Properties of Lead Iodine-Based Perovskite Doped with Methylammonium/Formamidinium/Cesium, columnId=1319726165087077079, journalTitle=Journal of the Chinese Ceramic Society, columnName=Research Article, runingTitle=null, highlight=null, articleAbstract=
Introduction Building a clean, low-carbon, safe, and efficient energy system and implementing renewable energy substitution actions become important issues to promote sustainable energy utilization. As a representative of clean and sustainable energy, the use of solar energy can greatly reduce carbon emissions, while meeting the growing demand for energy consumption. Since 2009, CH3NH3PbI3 perovskite has been used as a light absorbing layer, achieving a photoelectric conversion efficiency of 3.8%. The organic-inorganic hybrid perovskite material has attracted much attention as a solar cell light absorbing material. However, lead halide perovskite materials are highly susceptible to various external environmental factors such as dopants, heat, light, humidity, etc., which can cause failures in the chemical or physical structure during their application, greatly restricting the commercial application of the devices. It is thus of great significance for the practical application of lead halide based perovskite devices to investigate the intrinsic relationship among the structure, properties and stability. This study employed methylammonium (CH3NH3+, MA), formamidinium (CH (NH2)2+, FA), and Cesium (Cs) as A-site ions to construct three perovskite configurations (i.e., MA1-xFAxPbI3, MA1-xCsxPbI3, and Cs1-xF AxPbI3). The structure, stability, electronic and optical properties were investigated, and the theoretical basis for further experimental optimization and exploration of efficient and stable perovskite solar cell materials was also discussed.
Methods The structure and optoelectronic properties of A-site modified lead halide A'1-XA''XPbI3 (where A' and A'' are any of MA, FA, and Cs) perovskite configurations were investigated based on density functional theory by using CASTEP module under the Perdew Burke Ernzerhof exchange correlation functional of generalized gradient approximation via optimizing the structure and calculating the formation energy, band structure, density of states and absorption coefficient. After structural convergence testing, the energy cutoff of the plane wave was selected as 600 eV, and the Monkhorst-Pack scheme was used to mark the Brillouin zone by using a 2×3×2 k-point grid. The energy convergence standard of the system was set at 10-5 eV/atom. The maximum force was limited to 0.03 eV/Å with the maximum stress of 0.05 GPa, and the maximum displacement of 0.01 Å.
Results and discussion The optimized crystal structures of MA1-xCsxPbI3, MA1-xFAxPbI3 and Cs1-xFAxPbI3 (x=0.125, 0.250, 0.500) perovskite configurations show that the cell volume of Cs1-xFAxPbI3 and MA1-xFAxPbI3 increases while MA1-xCsxPbI3 decreases with increasing the doping content due to the atomic distance of FA group with 3.996 A, MA group with 3.009 A and the radius of Cs+ only 1.88 A. Meanwhile, the doping ions at A-site can cause the distortion of Pb-I octahedron, resulting in variations on bond length, bond angle and torsion of octahedron, and MA0.875FA0.125PbI3 demonstrates a slight distortion. The formation energy of MA1-xCsxPbI3, MA1-xFAxPbI3 and Cs1-xFAxPbI3 configurations is negative. As the Cs/MA, FA/MA, and FA/Cs ratios increase, the formation energy becomes more negative, indicating the doped groups can enter the lattice spontaneously and smoothly. The formation energy of MA1-xFAxPbI3 is minimum (i.e., -521.77, -1042.79 eV and -1824.49 eV correspond to x=0.125, 0.250 and 0.500), compared to that of MA1-xCsxPbI3 (i.e., -492.58, -984.86 eV and -1722.95 eV) and Cs1-xFAxPbI3 (-28.87, -57.79 eV and -101.61 eV), due to the large energy difference in MA and FA groups and the resulting strong force between atomic groups. This indicates that FA groups can enter MAPbI3 lattice more easily and form a more stable structure. The energy band structure calculated shows that the conduction band minimum (CBM) and valance band maximum (VBM) of MA1-xCsxPbI3, MA1-xFAxPbI3 and Cs1-xFAxPbI3 are located at the same high symmetric point G(0, 0, 0), thus determining direct band gap semiconductors. Furthermore, Pb 6p orbital and I 5p orbital dominate in CBM and VBM, respectively. Except that, the electron orbital of FA contributes to CBM significantly, mainly situating at 3.33 eV. The contribution of MA and Cs is primarily at -4.60 eV and 5.35 eV away from the Fermi surface, hence leading to a relatively large band gap in MA1-xCsxPbI3. As for Cs1-xFAxPbI3, Cs and FA orbital overlap at the conduction band (CB, 2.0-4.0 eV), and a great covalent bond can be formed between C-Cs, which facilitates the new energy orbital formed and thus more stronger orbital hybridization with Pb and I, and eventually in turn causes CB to shift upward and the band gap increases. However, compared with Cs, the interaction of MA and FA electron orbital at CB reduces, and MA1-xFAxPbI3 shows a relatively small band gap. MA0.875FA0.125PbI3 exhibits a decent band gap and a decreased energy band dispersion at CBM, promoting the transition of charge carriers and improving light absorption. Also, the real part of the dielectric functions ε1(ω) peak for MA0.875FA0.125PbI3 demonstrates a red shift from 533 nm to 572 nm, and ε1(ω) is optimal with the increase of wavelength. The widened wavelength response range and high ε1(ω) endow MA0.875FA0.125PbI3 with an optimal light absorption capacity in the visible light range of 380-780 nm.
Conclusions The optoelectronic properties of lead iodide-based perovskite A'1-XA''XPbI3 were predicted by using first-principles via the structural optimization and the calculation of formation energy, band structure, density of states, absorption coefficient. The results indicated that MA, FA groups, and Cs ions could spontaneously enter the A-site of lead iodide A'1-XA''XPbI3 perovskite to form a stable structure. Compared with MA1-xCsxPbI3 and Cs1-xFAxPbI3, MA1-xFAxPbI3 configuration displayed a minimum distortion of Pb-I octahedral and a more stable structure. In addition to the contribution of I 5p orbitals to VBM and Pb 6p orbitals to CBM, the electronic orbitals of FA in the CBM resulted in a dramatical decrease in band dispersion, which was conducive to light absorption. The absorption peak of MA0.875FA0.125PbI3 at 500nm showed a significant red shift. The widened wavelength response range and increased light absorption coefficient endowed MA0.875FA0.125PbI3 with an optimal light absorption ability in the visible light range, making it a promising solar cell photovoltaic material.
, authors=Zhuo LI, Nannan LEI, Dingjie LONG, authorsList=Zhuo LI, Nannan LEI, Dingjie LONG, authorCompany=null, correspAuthors=null, authorNote=
LI Zhuo (1982-), female, Ph.D., Associate Professor. E-mail: Lzhysgc@126.com
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作为太阳能电池热点材料之一的铅卤基钙钛矿，近年来得到了广泛关注。采用第一性原理预测了A位甲氨基（CH3NH3+，MA）、甲脒基［CH（NH2）2+，FA］和铯（Cs）改性铅碘基MA1-xCsxPbI3、MA1-xFAxPbI3和Cs1-xFAxPbI3（x=0.125，0.250，0.500）3种钙钛矿构型的光电性能，通过结构优化、掺杂元素形成能、能带结构、态密度和吸收系数的计算，研究了微观构型对光电特性的影响。结果表明，MA、FA基团和Cs离子均可自发进入A'1-XA''XPbI3铅碘基钙钛矿A位形成稳定结构，相对于MA1-xCsxPbI3和Cs1-xFAxPbI3，MA1-xFAxPbI3体系Pb-I八面体畸变程度最小且结构最稳定。由态密度分析可知MA1-xFAxPbI3的价带顶（VBM）主要由I 5p轨道构成，而Pb 6p轨道和FA的电子轨道主要对导带底（CBM）贡献，FA的少量加入使MA0.875FA0.125PbI3的带隙从MAPbI3的1.771 eV微增至1.797 eV，但导带底能带色散变小，其对光的吸收有明显作用。光学性能的计算表明：MA0.875FA0.125PbI3在533 nm处的吸收峰发生了明显的红移，增加的波长响应范围及随波长而增大的ε1（ω）赋予MA0.875FA0.125PbI3在可见光范围内最佳的光吸收能力，是一种非常有前途的太阳能电池光电转换材料。
, authors=李卓, 雷楠楠, 龙定杰, authorsList=李卓, 雷楠楠, 龙定杰, authorCompany=null, correspAuthors=null, authorNote=
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李卓（1982—），女，博士，副教授。
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