Article
Chemistry, Multidisciplinary
Lucy D. Whalley, Puck van Gerwen, Jarvist M. Frost, Sunghyun Kim, Samantha N. Hood, Aron Walsh
Summary: The study found that the neutral iodine interstitial plays a role in fast and irreversible electron capture, affecting the optoelectronic performance of halide perovskite semiconductors. The localization of phonon modes is associated with electron capture by the neutral iodine interstitial. Suppressing octahedral rotations is a key factor in enhancing defect tolerance.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Bo Li, Zhen Li, Danpeng Gao, Xin Wu, Xintong Li, Chunlei Zhang, Shuai Li, Jianqiu Gong, Dong Zhang, Xiangfan Xie, Shuang Xiao, Haipeng Lu, Mingjie Li, Zonglong Zhu
Summary: By designing long-chain alkylamines as crystallization buffer molecules, the residual strain in tin perovskite films was released, thus improving the photovoltaic performance and stability of lead-stabilized tin perovskite solar cells (TPSCs).
MATERIALS CHEMISTRY FRONTIERS
(2023)
Article
Chemistry, Physical
Yunjuan Niu, Yaole Peng, Xianxi Zhang, Yingke Ren, Rahim Ghadari, Jun Zhu, Gavin Tulloch, Hong Zhang, Polycarpos Falaras, Linhua Hu
Summary: The energy level alignment at interfaces is crucial for the efficiency and stability of perovskite solar cells. In this study, an innovative interface engineering approach using an ortho-squaraine derivative was proposed to change the charge state of the perovskite surface and tune the energy level structure. The results showed that this approach greatly improved the efficiency and stability of the perovskite solar cells.
ACS ENERGY LETTERS
(2022)
Review
Chemistry, Physical
Jingru Zhang, Wangen Zhao, Selina Olthof, Shengzhong (Frank) Liu
Summary: The rapid development of inorganic metal perovskite materials, such as CsPbX3, shows great potential for top-cells in tandem junctions due to their thermal stability and adjustable band gap. However, the efficiency of CsPbX3 perovskite solar cells still needs improvement due to defects. Research on defect passivation in CsPbX3 PSCs is summarized, including discussions on defect physics, tolerance, self-healing, and techniques for defect identification and manipulation for enhancing photoelectric properties.
Article
Chemistry, Physical
Jialong Duan, Meng Wang, Yingli Wang, Junshuai Zhang, Qiyao Guo, Qiaoyu Zhang, Yanyan Duan, Qunwei Tang
Summary: This study demonstrates the importance of regulating the side group of a dipole molecule for interfacial passivation and surface energy level reconstruction of CsPbBr3 perovskite films to achieve efficient hole extraction and improve power conversion efficiency.
ACS ENERGY LETTERS
(2021)
Article
Chemistry, Physical
Jiuyao Du, Jifeng Yuan, Jiahao Xi, Fei Huang, Jianjun Tian
Summary: In this study, 1-ethyl-3-methylimidazolium acetate ([EMIM]Ac) ionic liquid was introduced to passivate the surface defects of perovskite films, improving the performance and stability of metal halide perovskite solar cells. The carbonyl groups of [EMIM]Ac coordinate with the uncoordinated lead ions on the perovskite surface, reducing nonradiative recombination and improving working stability. The power conversion efficiency of the solar cell increased from 16.95% to 19.29% with [EMIM]Ac treatment. This surface passivation method using an ionic liquid may have significant implications for the development and practical application of perovskite solar cells.
JOURNAL OF ALLOYS AND COMPOUNDS
(2023)
Review
Chemistry, Physical
Pei-Ying Lin, Aswaghosh Loganathan, Itaru Raifuku, Ming-Hsien Li, Yueh-Ya Chiu, Shao-Tung Chang, Azhar Fakharuddin, Chen-Fu Lin, Tzung-Fang Guo, Lukas Schmidt-Mende, Peter Chen
Summary: Perovskite solar cells have achieved high power conversion efficiency, but the intrinsic instability of perovskite materials remains a key issue. Studies have shown that mixed-halide perovskites and other negative monovalent ions can improve stability. This review presents the evolution and applications of pseudo-halide perovskite solar cells.
ADVANCED ENERGY MATERIALS
(2021)
Article
Nanoscience & Nanotechnology
Shaocong Duan, Qing Sun, Gang Liu, Jianguo Deng, Xiangxin Meng, Bo Shen, Die Hu, Bonan Kang, S. Ravi P. Silva
Summary: Organic-inorganic hybrid perovskite solar cells with high-quality perovskite thin films passivated by an ionic liquid (DADA) exhibit improved device performance, including increased power conversion efficiency and enhanced stability. The DADA treatment reduces surface defects and improves film morphology, leading to reduced charged defects and prolonged carrier lifetime. The increase in work function and passivation of ion defects contribute to better carrier transport.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Japheth Joseph Yeow Wan Foong, Benny Febriansyah, Prem Jyoti Singh Rana, Teck Ming Koh, Darrell Jun Jie Tay, Annalisa Bruno, Subodh Mhaisalkar, Nripan Mathews
Summary: Passivation with alkylammonium alkanoate can significantly reduce recombination losses and improve open-circuit voltage, leading to higher power conversion efficiencies. The unencapsulated device retains 85% of its initial PCE after treatment, while the standard 3D perovskite device loses 50% of its original PCE after exposure to ambient environment for 1500 hours.
Review
Energy & Fuels
Mahdi Malekshahi Byranvand, Michael Saliba
Summary: Perovskite solar cells have attracted attention for their low-cost processing, abundant raw materials, and high efficiency, but defects within the films can lead to reduced efficiency and stability. Different passivation methods, including bulk and surface treatments, can help minimize defects and improve performance. Understanding defect sources and utilizing passivation agents are crucial for enhancing the efficiency and stability of perovskite photovoltaics.
Article
Multidisciplinary Sciences
Zaiwei Wang, Lewei Zeng, Tong Zhu, Hao Chen, Bin Chen, Dominik J. Kubicki, Adam Balvanz, Chongwen Li, Aidan Maxwell, Esma Ugur, Roberto dos Reis, Matthew Cheng, Guang Yang, Biwas Subedi, Deying Luo, Juntao Hu, Junke Wang, Sam Teale, Suhas Mahesh, Sasa Wang, Shuangyan Hu, Eui Dae Jung, Mingyang Wei, So Min Park, Luke Grater, Erkan Aydin, Zhaoning Song, Nikolas J. Podraza, Zheng-Hong Lu, Jinsong Huang, Vinayak P. Dravid, Stefaan De Wolf, Yanfa Yan, Michael Gratzel, Merx G. Kanatzidis, Edward H. Sargent
Summary: Researchers have discovered that lattice distortion in iodide/bromide mixed perovskites can suppress phase segregation, leading to increased ion-migration energy barrier. By using an approximately 2.0-electron-volt rubidium/caesium mixed-cation inorganic perovskite with large lattice distortion, they achieved an efficiency of 24.3% in all-perovskite triple-junction solar cells. This is the first reported certified efficiency for perovskite-based triple-junction solar cells.
Article
Multidisciplinary Sciences
Matteo Degani, Qingzhi An, Miguel Albaladejo-Siguan, Yvonne J. Hofstetter, Changsoon Cho, Fabian Paulus, Giulia Grancini, Yana Vaynzof
Summary: This study presents a dual interfacial modification approach by incorporating large organic cations at both the bottom and top interfaces of the perovskite active layer, leading to simultaneous improvement in both open-circuit voltage and fill factor of the devices, reaching a champion device efficiency of 23.7%. This dual interfacial modification is fully compatible with bulk modification of the perovskite active layer by ionic liquids, resulting in efficient and stable inverted architecture devices.
Article
Chemistry, Physical
Qi Chen, Yang Bai, Qizhen Song
Summary: This article introduces the application of Bayesian Optimization algorithm in the field of perovskite solar cells. Perovskite solar cells have made significant progress due to their unique optoelectronic properties. However, they still face some challenges in practical applications. The Bayesian Optimization algorithm can accelerate the development of processing chemistry and has great potential for solving problems in the field of perovskite solar cells.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Multidisciplinary
Baoning Wang, Na Li, Lin Yang, Chunxiang Dall'Agnese, Ajay Kumar Jena, Tsutomu Miyasaka, Xiao-Feng Wang
Summary: The photovoltaic performance of Cs2AgBiBr6 perovskite was improved by introducing indoline dyes, leading to higher power conversion efficiencies and short-circuit current densities in the hybrid cells. The double perovskite functioned as a p-type interlayer to enhance overall performance.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Engineering, Environmental
Yali Liu, Wanchun Xiang, Shaiqiang Mou, Hao Zhang, Shengzhong Liu
Summary: Passivating ionic defects on the surface of inorganic perovskite films using DADA significantly reduces defect density and extends the lifetime of charge carriers within the film. Additionally, DADA treatment induces an upward shift of the energy band edge of the perovskite layer, potentially facilitating hole extraction at the interface.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Olha Aftenieva, Julius Brunner, Mohammad Adnan, Swagato Sarkar, Andreas Fery, Yana Vaynzof, Tobias A. F. Koenig
Summary: We use a simple grating configuration to direct and amplify the omnidirectional emission of perovskite nanocrystals. By using a soft lithographic printing process, we can reliably structure perovskite nanocrystals into light-emitting metasurfaces with high contrast on a large area. Our self-assembly process allows for scalable fabrication of gratings with predefined periodicities and tunable optical properties.
Editorial Material
Chemistry, Physical
Nicholas M. Twyman, Aron Walsh, Tonio Buonassisi
CHEMISTRY OF MATERIALS
(2023)
Editorial Material
Materials Science, Multidisciplinary
Zhuoying Chen, Dinesh Kabra, Yana Vaynzof
JOURNAL OF MATERIALS CHEMISTRY C
(2023)
Article
Chemistry, Physical
Kazuki Morita, Matthias J. Golomb, Miguel Rivera, Aron Walsh
Summary: Polarons are localized excess charge in materials, especially transition metal oxides, which are of fundamental interest for photochemical and electrochemical reactions. This study focuses on the model system rutile TiO2 and investigates the effect of impurity doping on polaron formation. Additionally, two metal-organic frameworks (MOFs), MIL-125 and ACM-1, are compared to TiO2, demonstrating the influence of ligands and connectivity on polaron mobility.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Kasper Tolborg, Aron Walsh
Summary: The researchers investigated the tetragonal-to-cubic phase transition of ZrO2 at high temperatures using anharmonic lattice dynamics and molecular dynamics simulations. They found that the stability of cubic zirconia cannot be solely explained by anharmonic stabilization, but may also involve spontaneous defect formation and entropic stabilization, which is responsible for its superionic conductivity at elevated temperatures.
CRYSTAL GROWTH & DESIGN
(2023)
Article
Chemistry, Physical
Zhenzhu Li, Ji-Sang Park, Alex M. M. Ganose, Aron Walsh
Summary: Polytypes formed during the growth of metal halide perovskites can affect the formation of face-sharing sequences in corner-sharing octahedral networks. The electronic properties of these structures, such as the 6H and 12R phases, are related to the fraction and stacking order of the face-sharing layers. The bandgaps of the polytypes change from indirect to direct as they evolve from pure hexagonal (2H) to cubic (3C) phases. The large band gap bowing in the CsPbI3 family is attributed to long-range electronic interactions between octahedral building blocks rather than orbital mixing at the atomic level. Carrier velocity remains high, but Fermi surface analysis shows a decrease in dimensionality from 3D to 2D in commonly observed polytypes, indicating a blocking effect and anisotropic transport, which has implications for solar cells and other optoelectronic devices.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Seung-Jae Shin, Jamie W. W. Gittins, Matthias J. J. Golomb, Alexander C. C. Forse, Aron Walsh
Summary: The electrochemical interface of Cu-3(HHTP)(2) with an organic electrolyte was investigated using simulations and experimental measurements. The excess charges mainly formed on the organic ligand, and cation-dominated charging mechanisms led to greater capacitance. By changing the ligand, the spatially confined electric double-layer structure and self-diffusion coefficients of in-pore electrolytes were improved. The performance of MOF-based supercapacitors can be controlled by modifying the ligating group.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Adair Nicolson, Joachim Breternitz, Sean R. Kavanagh, Yvonne Tomm, Kazuki Morita, Alexander G. Squires, Michael Tovar, Aron Walsh, Susan Schorr, David O. Scanlon
Summary: Researchers predict and confirm a disordered room-temperature structure of the mixed-anion crystal Sn2SbS2I3 using a first-principles cluster expansion approach and single-crystal X-ray diffraction. The disorder reduces the bandgap from 1.8 eV at low temperature to 1.5 eV at a specific annealing temperature. Tailoring the cation disorder allows for targeted bandgap engineering, making this crystal useful for optoelectronic applications, including graded solar cells. Further investigation into the material properties associated with defect and disorder tolerance is encouraged.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Miguel Albaladejo-Siguan, Anatol Prudnikau, Alina Senina, Elizabeth C. Baird, Yvonne J. Hofstetter, Julius Brunner, Juanzi Shi, Yana Vaynzof, Fabian Paulus
Summary: The synthesis of metal sulfide nanocrystals is essential for quantum dot (QD) photovoltaics. The control over QD size allows for precise tuning of optical and electronic properties, making them suitable for various electronic applications. A new air-stable sulfur precursor, bis(stearoyl) sulfide (St(2)S), is introduced for sulfide-based QD synthesis, resulting in uniform and stable nanocrystals. Photovoltaic devices based on St(2)S-synthesized QDs exhibit comparable efficiency to those using the toxic, air- and moisture-sensitive sulfur source (TMS)(2)S, but have improved operational stability.
ADVANCED ENERGY MATERIALS
(2023)
Article
Nanoscience & Nanotechnology
Jing Li, Rene Huebner, Marielle Deconinck, Ankita Bora, Markus Goebel, Dana Schwarz, Guangbo Chen, Guangzhao Wang, Shengyuan A. Yang, Yana Vaynzof, Vladimir Lesnyak
Summary: In this study, a method for efficiently synthesizing alloyed Re x Mo1-x S2 nanoflakes with enlarged interlayer distance was reported, among which Re0.55Mo0.45S2 exhibited excellent catalytic performance. Density functional theory calculations proved that enlarging the distance between layers in the Re x Mo1-x S2 alloy can greatly improve its catalytic performance. This research paves the way for designing advanced transition metal dichalcogenide-based catalysts for hydrogen evolution and promoting their large-scale practical application.
ACS APPLIED NANO MATERIALS
(2023)
Article
Chemistry, Physical
Kanta Ogawa, Hajime Suzuki, Aron Walsh, Ryu Abe
Summary: Three novel bismuth-based layered oxyiodides with increased water oxidation activity under visible light were reported. The electronic structure of these compounds is controlled by the Bi-Bi interaction, resulting in enhanced photoabsorption and reduced band gap. This research not only provided new photocatalysts for water splitting, but also offered a pathway to control the optoelectronic properties of lone-pair semiconductors.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Shanti M. Liga, Sean R. Kavanagh, Aron Walsh, David O. Scanlon, Gerasimos Konstantatos
Summary: Lead toxicity and poor stability hinder the commercialization of metal-halide perovskite solar cells. This study explores the use of Ti(IV) and Sn(IV) as alternatives to replace Pb(II), with Ti(IV) perovskites being unstable in air and Sn(IV) perovskites showing good stability in ambient conditions. The research focuses on mixed titanium-tin bromide and iodide double perovskites, finding that these mixtures exhibit higher stability at high percentages of Sn, with bromide compositions demonstrating greater stability compared to iodides.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Xia Liang, Johan Klarbring, William J. Baldwin, Zhenzhu Li, Gabor Csanyi, Aron Walsh
Summary: Metal halide perovskites are classified as soft semiconductors with flexible corner-sharing octahedral networks and polymorphous nature. A quantitative analysis of structural dynamics in perovskite crystals is achieved through molecular dynamics simulations. A machine learning force field is trained for methylammonium lead bromide and used to reproduce stable phases and identify symmetry-breaking effects. The structural dynamics descriptors and Python toolkit can be applied to perovskites and complex compositions.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Materials Science, Multidisciplinary
Lucas Scalon, Julius Brunner, Maria Gabriella Detone Guaita, Rodrigo Szostak, Miguel Albaladejo-Siguan, Tim Kodalle, L. Andres Guerrero-Leon, Carolin M. Sutter-Fella, Caio C. Oliveira, Yana Vaynzof, Ana Flavia Nogueira
Summary: The introduction of chiral organic spacers in low-dimensional metal-halide perovskites leads to chiroptical activity, which is attractive for spintronic applications. However, there is still a lack of comprehensive understanding regarding the formation of structure and the ability to control phase purity in such materials. This study explores the impact of processing conditions on the phase purity, microstructure, and chiroptical properties of chiral 2D perovskites. The anisotropic emergence of a 1D perovskite inside the 2D matrix and its dependence on the organic cation chirality, solvent, and thermal annealing conditions are demonstrated.
ADVANCED OPTICAL MATERIALS
(2023)
Article
Materials Science, Multidisciplinary
Shraddha M. Rao, Alexander Kiligaridis, Aymen Yangui, Qingzhi An, Yana Vaynzof, Ivan G. Scheblykin
Summary: Defects in metal halide perovskites (MHP) exhibit photosensitivity, causing the observer effect in laser spectroscopy. The creation and healing of defects lead to transient phenomena such as photoluminescence (PL) bleaching and enhancement. The use of the dependence of PL quantum yield (PLQY) on laser pulse repetition rate and pulse fluence as a unique fingerprint of charge carrier dynamics and defect evolution is demonstrated. Automatic PLQY mapping can be used as a universal method for assessing the quality of perovskite samples.
ADVANCED OPTICAL MATERIALS
(2023)
