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Nanoscale phase management of the 2d/3d heterostructure toward efficient perovskite solar cells

Science Bulletin 2024年第18期69卷 2853-2861页

作者： Hao Gu Annan Zhu Junmin Xia Wang Li Jiahao Zheng Tao Yang Shengwen Li Nan Zhang Shiliang Mei Yongqing Cai Shi Chen Chao Liang Guichuan Xing Joint Key Laboratory of the Ministry of Education Institute of Applied Physics and Materials EngineeringUniversity of MacaoMacao 999078China State Key Laboratory of Organic Electronics and Information Displays&Institute of Advanced Materials(IAM) Jiangsu National Synergetic Innovation Center for Advanced Materials(SICAM)Nanjing University of Posts&Telecommunications(NUPT)Nanjing 210023China MOE Key Laboratory for Nonequilibrium Synthesis and Modulation of Condensed Matter School of PhysicsNational Innovation Platform(Center)for Industry-Education Integration of Energy Storage TechnologyXi’an Jiaotong UniversityXi’an 710049China Ministry of Industry and Information Technology Key Lab of Micro-Nano Optoelectronic Information System Guangdong Provincial Key Laboratory of Semiconductor Optoelectronic Materials and Intelligent Photonic SystemsHarbin Institute of TechnologyShenzhen 518055China Institute for Electric Light Sources School of Information Science and TechnologyFudan UniversityShanghai 200433China

The stabilization of the formamidinium lead iodide(FAPbI_(3))structure is pivotal for the development of efficient photovoltaic *** two-dimensional(2d)layers to passivate the threedimensional(3d)perovskite is essential for maintaining the a-phase of FAPbI_(3) and enhancing the power conversion efficiency(PCE)of perovskite solar cells(PSCs).However,the role of bulky ligands in the phase management of 2d perovskites,crucial for the stabilization of FAPbI_(3),has not yet been *** this study,we synthesized nanoscale 2d perovskite capping crusts with=1 and 2 Ruddlesden-Popper(RP)perovskite layers,respectively,which form a type-Ⅱ 2d/3d *** heterostructure stabilizes the a-phase of FAPbI_(3),and facilitates ultrafast carrier extraction from the 3d perovskite network to transport contact *** introduced tri-fluorinated ligands to mitigate defects caused by the halide vacancies and uncoordinated Pb^(2+)ions,thereby reducing nonradiative carrier recombination and extending carrier *** films produced were incorporated into PSCs that not only achieved a PCE of 25.39%but also maintained 95%of their initial efficiency after 2000 h of continuous light exposure without *** findings underscore the effectiveness of a phase-pure 2d/3d heterostructure-terminated film in inhibiting phase transitions passivating the iodide anion vacancy defects,facilitating the charge carrier extraction,and boosting the performance of optoelectronic devices.

关键词： Phase-pure 2d perovskite 2d/3d heterostructure Type-II energy alignment Carrier dynamic FAPbI_(3)

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Ordered crystal growth of 2d Ruddlesden-Popper perovskites via synergistic fluorination and chlorination for efficient and stable 2d/3d heterostructure perovskite solar cells

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CHEMICAL ENGINEERING JOURNAL 2025年 512卷

作者： du, Shitong Yang, Wenbin Hao, Wending Liu, Tao Hou, Meichen Wang, Ning Hainan Univ State Key Lab Marine Resource Utilizat South China Haikou 570228 Peoples R China

Based on epitaxial growth theory, a highly ordered 2d perovskite is necessary to boost the photoelectric performance of 2d/3d perovskite heterostructures. The strong NH...I hydrogen-bonding interaction between spacer cations and inorganic frameworks could be built by widely used dipolar aromatic amine spacer cations with single halogen (F or Cl) substitution, which is crucial to the stabilization of 2d perovskites. However, the effect of synergistic fluorination and chlorination on the octahedral tilt of 2d perovskites is relatively unexplored. Herein, halogen substituted meta, para-aniline iodide (3,4-AnI) salts, including 3-F-4-ClAnI, 3,4-FAnI, 3,4-ClAnI, and 3Cl-4-FAnI, were respectively added into 3d perovskite precursor solution. By contrast, the 3-F-4-ClAnI-treated n = 2 2d Ruddlesden-Popper (RP) perovskite exhibits the highest ordered crystalline structure. We find that 3-F-4ClAn+ spacer cations have both strong NH...I hydrogen interaction and Pb-halide interaction with [PbI6]4octahedron cages. Both are favorable for the stability of 2d perovskites and subsequent orientation growth of 3d perovskite crystals, thereby leading to reduced stack defects as well as improved carrier transport. Consequently, the optimized perovskite solar cell (PSC) with 3-F-4-ClAnI-treated 2d/3d Cs0.05MA0.16FA0.79Pb(I0.83Br0.17)3 perovskite yields a high power conversion efficiency (PCE) of 22.73 % compared with the control device without 2d perovskite (19.54 %). A higher PCE of 24.74 % is delivered for the device assembled with 3-F-4-ClAnI-treated 2d/3d FAPbI3 perovskite. The experimental results are of certain significance in guiding the design of the highly orientated 2d/3d perovskites.

关键词： 3-Fluoro-4-chloroaniline iodine salt NH...I hydrogen bond Pb-halide interaction Orientation order 2d/3d heterostructure Perovskite solar cells

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Efficient and Stable CsPbI2Br Perovskite Solar Cells Based on In-situ Formation of 2d/3d heterostructure

Efficient and Stable CsPbI2Br Perovskite Solar Cells Based o...

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第九届新型太阳能材料科学与技术学术研讨会

作者： Xuanling Liu Meiqian Tai Hong Lin School of Materials Science and Engineering Tsinghua University

Mixed halide inorganic perovskite CsPbI2 Br has been considered as promising absorber due to its improved phase stability and reasonable bandgap(1.92 eV). However, the instability of CsPbI2 Br solar cells in humidity environment hampers its further development. In order to prepare efficient and stable CsPbI2 Br solar cells, our group used carbon nanotube(CNT) sheets as an evaporator to prepare CsPbI2 Br thin films by Flash-evaporation printing(FEP) at high temperature without solvent and anti-solvent, demonstrating a method that can prepare compact and uniform thin films with high reproducibility and it's also suitable for preparing insoluble materials. Solar cells based on these CsPbI2 Br thin films exhibited a champion power conversion efficiency of 12.2%. To further improve the humidity stability, we next reported an in-situ growth method to prepare 2 d/3 d heterostructure for CsPbI2 Br solar cells with the help of solvent, which overcome difficulties of constructing 2 d perovskite for Cs-based perovskite through simple cation-exchange because of reaction resistance. As a result, the Type Ⅱ heterostructure was constructed between the 2 d capping layer and 3 d perovskite, which facilitated hole extraction and suppressed the carrier recombination at the perovskite/hole transport layer interface. The optimized CsPbI2 Br solar cells based on 2 d/3 d heterostructure exhibited power conversion efficiencies of 14.5% with improved humidity stability. To further increase the device stability, vertically-aligned quasi-2 d CsPbI3 solar cells were prepared by controlling the crystallization kinetics, and the variation law of phase purity, film morphology, and crystal orientation was revealed.

关键词： Perovskite solar cells 2d/3d heterostructure Stability CsPbI2Br perovskite Flash-evaporation printing

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In-situ fabrication of novel BiOCl/Bi5O7I 2d/3d heterostructures with enhanced photocatalytic activity

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JOURNAL OF ALLOYS ANd COMPOUNdS 2022年第Part2期895卷 162669-162669页

作者： Huang, Wendi Xiao, Xinyan Lu, Mingli Xiao, Yu South China Univ Technol Guangdong Prov Key Lab Green Chem Prod Technol Sch Chem & Chem Engn Guangzhou 510640 Peoples R China Univ Manitoba Dept Mech Engn Winnipeg MB R3T 2N2 Canada

A novel BiOCl/Bi5O7I (BOC-BOI) heterojunction was prepared by growing ultrathin 2d BiOCl nanosheets in situ on the surface of 3d Bi5O7I microspheres. The 2d/3d heterostructure of BOC-BOI composites inhibited the agglomeration of BiOCl nanosheets, and benefited the multiple reflection and refraction of light, which greatly enhanced the absorption and utilization of light. The 50-BOC-BOI composite showed 97.7% de-gradation efficiency of rhodamine B (RhB) after 70 min Xe light irradiation. And its apparent degradation rate constant (k) was 0.0377 min(-1), being 4.9 and 15.1 times than that of pristine BiOCl (0.0077 min(-1)) and Bi5O7I (0.0025 min(-1)), respectively. The enhanced photocatalytic activity of BOC-BOI composites was attributed to stronger light capture ability, more abundant active sites and higher charge carrier separation efficiency, confirmed by UV-Vis dRS, SEM, TEM, BET, Zeta potential and electrochemical characterizations. The free radical capture experiments showed that the main active species in this system were holes (h(+)) and superoxide free radicals (center dot O-2(-)). Combining the results of UV-Vis dRS and Mott-Schottky test, a reasonable type II heterojunction mechanism was proposed. (C) 2021 Elsevier B.V. All rights reserved.

关键词： Ultrathin BiOCl Bi5O7I 2d/3d heterostructure In-situ growth method Type II heterojunction

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Semiconductor-Semimetal 2d/3d MoS2/SrRuO3(111) TMd/TMO Heterojunction-Based ReRAM devices

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ACS APPLIEd ELECTRONIC MATERIALS 2023年第10期5卷 5588-5597页

作者： Parmar, Swati Panchal, Suresh datar, Suwarna Ogale, Satishchandra Def Inst Adv Technol Pune 411025 Maharashtra India Indian Inst Sci Educ & Res IISER Pune Dept Phys Pune 411008 Maharashtra India Indian Inst Sci Educ & Res IISER Pune Ctr Energy Sci Pune 411008 Maharashtra India Res Inst Sustainable Energy TCG Ctr Res & Educ Sci & Technol Kolkata 700091 India Savitribai Phule Pune Univ Dept Technol Pune 411007 Maharashtra India

We have designed and grown MoS2/SrRuO3(111) (MoS2/SRO(111)) semiconductor (SC)/semimetal (SM) heterostructures involving transition-metal dichalcogenide (TMd) and transition-metal oxide (TMO) partners for TMd-based electronic device application. MoS2 is directly grown on a polar SrRuO3(111)/c-Al2O3 substrate by pulsed laser deposition (PLd). A comparative evaluation of few-layer (FL) versus bulk (BL) MoS2 on polar SRO(111) was performed by using several chemical and physical characterizations. Raman spectroscopy and X-ray photoelectron spectroscopy (XPS) confirm the degenerate states in strained MoS2 caused by polar SRO(111). In-plane room-temperature resistivity of 1.83 and 1.39 mu Omega-cm is obtained for FL and BL MoS2/SRO, respectively. Conducting atomic force microscopy (CAFM) was used to elucidate the distribution of in-plane conductive components. The electrical current across the CAFM-tip/MoS2/SRO(111) is primarily controlled by MoS2 and its interfaces with the tip metal on one side and the oxide semimetal on the other. We find an impressive ReRAM unipolar linear I-V characteristic in the case of FL MoS2/SRO (a sharp jump by a factor of 12), while in the BL MoS2/SRO (thicker overlayer) case, only a negligible effect is noted. Studies of the work function and Schottky barrier height (SBH) modulation due to the thickness variation of the semiconductor MoS2 at the SC/SM heterojunction are performed by the electrostatic force microscopy (EFM) to unveil the mechanism of the memristor-type I-V characteristics.

关键词： 2d materials semimetal thin films memory device 2d/3d heterostructure

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2d/3d Hybrid of MoS₂/GaN for a High-Performance Broadband Photodetector

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ACS APPLIEd ELECTRONIC MATERIALS 2021年第5期3卷 2407-2414页

作者： Jain, Shubhendra Kumar Low, Mei Xian Taylor, Patrick d. Tawfik, Sherif Abdulkader Spencer, Michelle J. S. Kuriakose, Sruthi Arash, Aram Xu, Chenglong Sriram, Sharath Gupta, Govind Bhaskaran, Madhu Walia, Sumeet RMIT Univ Funct Mat & Microsyst Res Grp Melbourne Vic 3000 Australia RMIT Univ Micro Nano Res Facil Melbourne Vic 3000 Australia CSIR Sensor Devices & Metrol Grp Natl Phys Lab CSIR NPL New Delhi 110012 India Acad Sci & Innovat Res AcSIR Ghaziabad 201002 Uttar Pradesh India RMIT Univ Sch Sci Melbourne Vic 3001 Australia RMIT Univ ARC Ctr Excellence Future Low Energy Elect Techno Sch Sci Melbourne Vic 3001 Australia RMIT Univ Micro Nano Res Facil Melbourne Vic 3001 Australia RMIT Univ Sch Engn Melbourne Vic 3001 Australia

Narrow spectral sensitivity in materials is one of the crucial challenges to develop high-performance broadband photodetectors. Here, we design a heterostructure of two-dimensional molybdenum disulfide (MoS2) and epitaxial gallium nitride (GaN) films to create an enhanced spectral absorption profile. This combination utilizes complementary optical absorption of MoS2 (visible) and GaN (UV) driven by type II band alignment at their interface to showcase highly sensitive photodetectors spanning across the UV-NIR regime. Concurrently, the heterostructure exhibits significantly enhanced responsivity (order of 10(4) A/W) and external quantum efficiency that are 500% higher than the bare GaN photodetectors. Given the available scalable synthesis approaches that have now been designed by the research community for both constituent materials, the demonstration of this heterostructure as a broadband photodetector with high figures-of-merit opens opportunities in designing efficient optoelectronic junctions and imaging applications.

关键词： 2d/3d heterostructure type II band structure broadband photodetector gallium nitride molybdenum disulfide

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MoS_(2)/Si tunnel diodes based on comprehensive transfer technique

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Chinese Physics B 2023年第1期32卷 106-112页

作者：朱翊吕红亮张玉明贾紫骥孙佳乐吕智军芦宾 School of Microelectronics Xidian UniversityThe State Key Discipline Laboratory of Wide Band Gap Semiconductor TechnologyXi'an 710071China Department of Integrated Circuit Design Institute of Microelectronics TechnologyXi'an 710071China School of Physics and Information Engineering Shanxi Normal UniversityTaiyuan 030031China

due to the pristine interface of the 2d/3d face-tunneling heterostructure with an ultra-sharp doping profile, the 2d/3d tunneling field-effect transistor(TFET) is considered as one of the most promising low-power devices that can simultaneously obtain low off-state current(IOFF), high on-state current(ION) and steep subthreshold swing(SS). As a key element for the 2d/3d TFET, the intensive exploration of the tunnel diode based on the 2d/3d heterostructure is in urgent *** transfer technique composed of the exfoliation and the release process is currently the most common approach to fabricating the 2d/3d heterostructures. However, the well-established transfer technique of the 2d materials is still *** a small part of the irregular films can usually be obtained by mechanical exfoliation, while the choice of the chemical exfoliation may lead to the contamination of the 2d material films by the ions in the chemical etchants. Moreover, the deformation of the 2d material in the transfer process due to its soft nature also leads to the nonuniformity of the transferred film,which is one of the main reasons for the presence of the wrinkles and the stacks in the transferred film. Thus, the large-scale fabrication of the high-quality 2d/3d tunnel diodes is limited. In this article, a comprehensive transfer technique that can mend up the shortages mentioned above with the aid of the water and the thermal release tape(TRT) is proposed. Based on the method we proposed, the MoS_(2)/Si tunnel diode is experimentally demonstrated and the transferred monolayer MoS_(2) film with the relatively high crystal quality is confirmed by atomic force microscopy(AFM), scanning electron microscopy(SEM), and Raman characterizations. Besides, the prominent negative differential resistance(NdR) effect is observed at room temperature, which verifies the relatively high quality of the MoS_(2)/Si heterojunction. The bilayer MoS_(2)/Si tunnel diode is also experimentally fabricated

关键词： 2d/3d heterostructure transfer technique tunnel diode MoS_(2)/Si

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diammonium-induced dion-Jacobson 2d/3d wide-bandgap perovskite solar cells with enhanced efficiency and stability

ECOMAT

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ECOMAT 2023年第1期5卷

作者： Yu, Yue Liu, Rui Xu, Maoxia Yu, Hua Southwest Petr Univ Inst Photovolta Chengdu Peoples R China

Surface passivation by two-dimensional (2d) organic spacers provides promising avenue to substantially enhance the photovoltaic performance and structural stability of perovskite solar cells (PSCs). Herein, a diammonium organic salt of 2,2 '-(Ethylenedioxy) diethyl ammonium diiodide (EdBEI2) is used to passivate surface defects with spontaneously established dion-Jacobson (dJ)-type two-dimensional/three-dimensional (2d/3d) perovskite structure. The 2d dJ perovskite (EdBEPbI4) is formed on the surface of 3d WBG film, which passivates surface defects and reduces non-radiation recombination with better-matched energy-level alignment. Consequently, the modified device shows an excellent power conversion efficiency of 18.85% with large open-circuit voltage of 1.28 V. Besides, such 2d/3d perovskite exhibits better stability, which maintains 89% of its original efficiency after 1000 h under a relative humidity of 30% for the unencapsulated EdBEI2-treated device. These results give a suggestive strategy to enhance the efficiency and stability of WBG PSCs, potentially, providing a feasible way for achieving the commercialization of perovskites.

关键词： 2d/3d heterostructure defect passivation dion-Jacobson stability wide-bandgap perovskite

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Unraveling Bulk versus Surface Passivation Effects in Highly Efficient p-i-n Perovskite Solar Cells Using Thiophene-Based Cations

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SOLAR RRL 2024年第9期8卷

作者： Pica, Giovanni Montecucco, Riccardo Zanetta, Andrea Oranskaia, Aleksandra Faini, Fabiola Pancini, Lorenzo Mrkyvkova, Nada Siffalovic, Peter dally, Pia Pirota, Valentina Ledinsky, Martin de Bastiani, Michele de Wolf, Stefaan doria, Filippo Schwingenschlogl, Udo Grancini, Giulia Univ Pavia Dept Chem Via T Taramelli 14 I-27100 Pavia Italy Univ Pavia INSTM Via T Taramelli 14 I-27100 Pavia Italy King Abdullah Univ Sci & Technol KAUST KAUST Solar Ctr KSC Phys Sci & Engn Div PSE Thuwal 239556900 Saudi Arabia Slovak Acad Sci Inst Phys Dubravska Cesta 9 Bratislava 84511 Slovakia Slovak Acad Sci CEMEA Dubravska Cesta 9 Bratislava 84511 Slovakia Inst Phys Czech Acad Sci Cukrovarnicka 10 Prague 16200 Czech Republic

defect passivation is nowadays considered a must-have route for high-efficiency perovskite solar cells. However, a general rule that correlates the choice of passivating agents with performance enhancements is still missing. Herein, two different thiophene salts that are used as passivating agents are compared, namely thiophene methylammonium chloride and thiophene ethylammonium chloride (TEACl), which are used for the passivation of bulk and surface defects in triple-cation-based metal halide perovskites. First, it is observed that the surface passivation method leads to better device performances reaching a power conversion efficiency of 23.56%, with reduced voltage losses and increased fill factor when compared with the reference. Second, it is demonstrated that the chemical structure of the cation dictates its capability either in passivating bulk defects effectively or to form a superficial two-dimensional/three-dimensional heterostructure, which happens only for the TEACl case. The chemical composition and the cation dimension are responsible for device performance enhancement as observed by a joint spectroscopic and density functional theory simulations study, providing rational guidelines for further smart device design.

关键词： 2d/3d heterostructure bulk passivation perovskite solar cells surface passivation thiophene-based passivants

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Stabilization of Inorganic Perovskite Solar Cells with a 2d dion-Jacobson Passivating Layer

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AdVANCEd MATERIALS 2023年第42期35卷 2304150-2304150页

作者： Wu, Luyan Li, Guixiang Prashanthan, Karunanantharajah Musiienko, Artem Li, Jinzhao Gries, Thomas W. Zhang, Hao Koebler, Hans Janasik, Patryk Appiah, Augustine N. S. Paramasivam, Gopinath Sun, Tianxiao Li, Meng Marongiu, daniela Saba, Michele Abate, Antonio Univ Cagliari Dipartimento Fis I-09042 Monserrato CA Italy Helmholtz Zentrum Berlin Materialien & Energie Hahn-Meitner-Pl 1 D-14109 Berlin Germany Ecole Polytech Fed Lausanne EPFL Inst Chem Sci & Engn CH-1015 Lausanne Switzerland Univ Bielefeld Dept Chem Univ Str 25 D-33615 Bielefeld Germany Univ Jaffna Dept Phys Jaffna 40000 Sri Lanka Univ Bordeaux Lab Ondes & Matiere Aquitaine F-33405 Talence France CNRS F-33405 Talence France Silesian Tech Univ Dept Chem Strzody 9 PL-44100 Gliwice Poland Henan Univ Natl & Local Joint Engn Res Ctr Highefficiency Di Collaborat Innovat Ctr Nanofunctional Mat & Appli Key Lab Special Functional Mat Minist Educ Sch M Kaifeng 475004 Peoples R China

Inorganic metal halide perovskites such as CsPbI3 are promising for high-performance, reproducible, and robust solar cells. However, inorganic perovskites are sensitive to humidity, which causes the transformation from the black phase to the yellow & delta;, non-perovskite phase. Such phase instability has been a significant challenge to long-term operational stability. Here, a surface dimensionality reduction strategy is reported, using 2-(4-aminophenyl)ethylamine cation to construct a dion-Jacobson 2d phase that covers the surface of the 3d inorganic perovskite structure. The dion-Jacobson layer mainly grows at the grain boundaries of the perovskite, effectively passivating surface defects and providing favourable interfacial charge transfer. The resulting inorganic perovskite films exhibit excellent humidity resistance when submerged in an aqueous solution (isopropanol:water = 4:1 v/v) and exposed to a 50% humidity air atmosphere. The dion-Jacobson 2d/3d inorganic perovskite solar cell (PSC) achieves a power conversion efficiency (PCE) of 19.5% with a Voc of 1.197 eV. It retains 83% of its initial PCE after 1260 h of maximum power point tracking under 1.2 sun illumination. The work demonstrates an effective way for stabilizing efficient inorganic perovskite solar cells. CsPbI3 perovskites suffers fast transfer to non-perovskite phase, especially exposed to humidity. Using 2-(4-aminophenyl)ethylamine cation to construct a dion-Jacobson 2d phase that covers the 3d inorganic perovskite surface, the obtained 2d/3d perovskite films exhibit excellent humidity resistance and higher temperature stability, resulting in improved efficiency and operational stability in solar ***

关键词： 2d/3d heterostructure dion-Jacobson phase humidity stability inorganic perovskite solar cells

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