Pub Date : 2024-09-18DOI: 10.1038/s43246-024-00636-8
Chunyang Zhang, Nam-Gyu Park
Although perovskite solar cells (PSCs) are promising next generation photovoltaics, the production of PSCs might be hampered by complex and inefficient procedures. This Review outlines important advances in materials and methods for the cost-effective manufacturing of PSCs, including precursor synthesis, selection criteria for precursors based on chemistry, additive engineering, and deposition techniques. The goal of these technologies is not only to improve the performance and stability of PSCs, but also to significantly reduce their manufacturing costs. These advances are critical to the commercialization of PSCs, in terms of making them viable and cost-effective. The scalable and cost-effective synthesis of perovskite solar cells is dependent on materials chemistry and the synthesis technique. This Review discusses these considerations, including selecting a suitable perovskite pre-cursor, additive engineering, and the deposition process.
{"title":"Materials and methods for cost-effective fabrication of perovskite photovoltaic devices","authors":"Chunyang Zhang, Nam-Gyu Park","doi":"10.1038/s43246-024-00636-8","DOIUrl":"10.1038/s43246-024-00636-8","url":null,"abstract":"Although perovskite solar cells (PSCs) are promising next generation photovoltaics, the production of PSCs might be hampered by complex and inefficient procedures. This Review outlines important advances in materials and methods for the cost-effective manufacturing of PSCs, including precursor synthesis, selection criteria for precursors based on chemistry, additive engineering, and deposition techniques. The goal of these technologies is not only to improve the performance and stability of PSCs, but also to significantly reduce their manufacturing costs. These advances are critical to the commercialization of PSCs, in terms of making them viable and cost-effective. The scalable and cost-effective synthesis of perovskite solar cells is dependent on materials chemistry and the synthesis technique. This Review discusses these considerations, including selecting a suitable perovskite pre-cursor, additive engineering, and the deposition process.","PeriodicalId":10589,"journal":{"name":"Communications Materials","volume":" ","pages":"1-13"},"PeriodicalIF":7.5,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s43246-024-00636-8.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142255332","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-18DOI: 10.1038/s43246-024-00629-7
Zainah A. AlDhawi, Ridha Hamdi, Mahmoud A. Abdulhamid
Photocatalytic degradation of organic pollutants is an essential technology for various environmental applications. However, the effectiveness of most photocatalysts is restricted to light. Herein, we report metal-free catalysts derived from intrinsically microporous polyimide for persistence in photocatalytic degradation of dyes. We systematically investigate the effect of porosity and functionality on photocatalytic efficiency. Both the pristine 4,4′-(hexafluoroisopropylidene)diphthalic anhydride-3,3′-dimethylnaphthidine and its thermally annealed counterpart at 530 °C exhibit high charge storage capabilities, enabling continuous photodegradation in the absence of light. The pre-irradiated catalyst exhibits an approximately 99% degradation of the dye, with a ~40% improvement relative to the non-pre-irradiated sample. We studied the influence of the chemical structure and porosity on the photocatalytic degradation efficiency in darkness by varying the polyimide chemical structure using different diamines. This research underscores the potential of polymers with intrinsic microporosity for application in the continuous degradation of dyes, contributing to the pursuit of cleaner water. Photodegradation of pollutants is important to produce clean water but their activities are restricted during nighttime. Here, metal-free catalysts derived from intrinsically microporous polyimide show efficient photocatalytic degradation activities of dyes under light and darkness.
光催化降解有机污染物是各种环境应用中的一项重要技术。然而，大多数光催化剂的功效仅限于光。在此，我们报告了由固有微孔聚酰亚胺衍生的无金属催化剂在光催化降解染料中的持久性。我们系统地研究了多孔性和功能性对光催化效率的影响。原始的 4,4′-(六氟异亚丙基)二邻苯二甲酸酐-3,3′-二甲基萘啶及其在 530 °C 下热退火的对应物都表现出很高的电荷储存能力，能在无光条件下持续光降解。预辐照催化剂的染料降解率约为 99%，与未经预辐照的样品相比提高了约 40%。我们通过使用不同的二胺改变聚酰亚胺的化学结构，研究了化学结构和孔隙率对黑暗中光催化降解效率的影响。这项研究强调了具有固有微孔的聚合物在持续降解染料方面的应用潜力，有助于实现更清洁的水质。
{"title":"Intrinsically microporous polyimide-based metal-free catalysts for round-the-clock photodegradation of organic pollutants","authors":"Zainah A. AlDhawi, Ridha Hamdi, Mahmoud A. Abdulhamid","doi":"10.1038/s43246-024-00629-7","DOIUrl":"10.1038/s43246-024-00629-7","url":null,"abstract":"Photocatalytic degradation of organic pollutants is an essential technology for various environmental applications. However, the effectiveness of most photocatalysts is restricted to light. Herein, we report metal-free catalysts derived from intrinsically microporous polyimide for persistence in photocatalytic degradation of dyes. We systematically investigate the effect of porosity and functionality on photocatalytic efficiency. Both the pristine 4,4′-(hexafluoroisopropylidene)diphthalic anhydride-3,3′-dimethylnaphthidine and its thermally annealed counterpart at 530 °C exhibit high charge storage capabilities, enabling continuous photodegradation in the absence of light. The pre-irradiated catalyst exhibits an approximately 99% degradation of the dye, with a ~40% improvement relative to the non-pre-irradiated sample. We studied the influence of the chemical structure and porosity on the photocatalytic degradation efficiency in darkness by varying the polyimide chemical structure using different diamines. This research underscores the potential of polymers with intrinsic microporosity for application in the continuous degradation of dyes, contributing to the pursuit of cleaner water. Photodegradation of pollutants is important to produce clean water but their activities are restricted during nighttime. Here, metal-free catalysts derived from intrinsically microporous polyimide show efficient photocatalytic degradation activities of dyes under light and darkness.","PeriodicalId":10589,"journal":{"name":"Communications Materials","volume":" ","pages":"1-12"},"PeriodicalIF":7.5,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s43246-024-00629-7.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142255335","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-18DOI: 10.1038/s43246-024-00634-w
Seong-Hoon Jang, Yukitoshi Motome
The Kitaev honeycomb model plays a pivotal role in the quest for quantum spin liquids, in which fractional quasiparticles would provide applications in decoherence-free topological quantum computing. The key ingredient is the bond-dependent Ising-type interactions, dubbed the Kitaev interactions, which require strong entanglement between spin and orbital degrees of freedom. Here we investigate the identification and design of rare-earth materials displaying robust Kitaev interactions. We scrutinize all possible 4f electron configurations, which require up to 6+ million intermediate states in the perturbation processes, by developing a parallel computational program designed for massive-scale calculations. Our analysis reveals a predominant interplay between the isotropic Heisenberg J and anisotropic Kitaev K interactions across all realizations of the Kramers doublets. Remarkably, instances featuring 4f3 and 4f11 configurations showcase the prevalence of K over J, presenting unexpected prospects for exploring the Kitaev quantum spin liquids in compounds, including Nd3+ and Er3+, respectively. Kitaev magnets are interesting as they can host quantum spin liquid phases and fractional quasiparticles for decoherence-free topological quantum computing. Here, a parallel computational program explores all possible 4f electron configurations of rare-earth Kitaev materials, identifying those configurations, such as 4f3 and 4f11 in Nd3+ and Er3+ compounds, where anisotropic Kitaev interactions prevail over isotropic Heisenberg exchange.
{"title":"Exploring rare-earth Kitaev magnets by massive-scale computational analysis","authors":"Seong-Hoon Jang, Yukitoshi Motome","doi":"10.1038/s43246-024-00634-w","DOIUrl":"10.1038/s43246-024-00634-w","url":null,"abstract":"The Kitaev honeycomb model plays a pivotal role in the quest for quantum spin liquids, in which fractional quasiparticles would provide applications in decoherence-free topological quantum computing. The key ingredient is the bond-dependent Ising-type interactions, dubbed the Kitaev interactions, which require strong entanglement between spin and orbital degrees of freedom. Here we investigate the identification and design of rare-earth materials displaying robust Kitaev interactions. We scrutinize all possible 4f electron configurations, which require up to 6+ million intermediate states in the perturbation processes, by developing a parallel computational program designed for massive-scale calculations. Our analysis reveals a predominant interplay between the isotropic Heisenberg J and anisotropic Kitaev K interactions across all realizations of the Kramers doublets. Remarkably, instances featuring 4f3 and 4f11 configurations showcase the prevalence of K over J, presenting unexpected prospects for exploring the Kitaev quantum spin liquids in compounds, including Nd3+ and Er3+, respectively. Kitaev magnets are interesting as they can host quantum spin liquid phases and fractional quasiparticles for decoherence-free topological quantum computing. Here, a parallel computational program explores all possible 4f electron configurations of rare-earth Kitaev materials, identifying those configurations, such as 4f3 and 4f11 in Nd3+ and Er3+ compounds, where anisotropic Kitaev interactions prevail over isotropic Heisenberg exchange.","PeriodicalId":10589,"journal":{"name":"Communications Materials","volume":" ","pages":"1-8"},"PeriodicalIF":7.5,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s43246-024-00634-w.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142255248","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-17DOI: 10.1038/s43246-024-00626-w
Michael J. Caplan, Richard Baldwin, Xiangyun Yin, Alexander Grishin, Stephanie Eisenbarth, Hugh A. Sampson, Kim Bottomly, Robert K. Prud’homme
Immune modulation and desensitization is a growing field of research and clinical investigation that requires precise delivery of antigens to immune system cells. Nanoparticles (NPs) have emerged as excellent candidates for antigen delivery, particularly in immune desensitization applications. NP-encapsulated protein antigens enable the delivery of protein and co-encapsulated adjuvant to antigen-presenting cells without systemic exposure and allergic response. Here, we show a method for producing poly(lactide-co-glycolide) (PLG) NPs in an efficient, high-yield, and large-scale inhomogeneous precipitation process. The process enables the production of compositionally complex PLG NPs containing protein while also incorporating DNA and E. coli phospholipids as integral adjuvants in the NP vehicle. Orally delivered PLG NPs activate the murine immune system, and encapsulated peanut allergen protein elicits approximately 10-fold lower levels of basophil activation than does unencapsulated protein in basophils isolated from peanut-allergic patients. This efficacy and safety evidence makes these PLG NPs excellent candidates for clinical applications. Protein-loaded nanoparticles are important for immunomodulatory applications. Here, an efficient method for producing protein-containing nanoparticles at large scale is developed which overcomes prior limitations on the use of poly(lactide-co-glycolide) nanoparticles.
{"title":"Scaleable production of highly loaded protein nanoparticles for immune modulation","authors":"Michael J. Caplan, Richard Baldwin, Xiangyun Yin, Alexander Grishin, Stephanie Eisenbarth, Hugh A. Sampson, Kim Bottomly, Robert K. Prud’homme","doi":"10.1038/s43246-024-00626-w","DOIUrl":"10.1038/s43246-024-00626-w","url":null,"abstract":"Immune modulation and desensitization is a growing field of research and clinical investigation that requires precise delivery of antigens to immune system cells. Nanoparticles (NPs) have emerged as excellent candidates for antigen delivery, particularly in immune desensitization applications. NP-encapsulated protein antigens enable the delivery of protein and co-encapsulated adjuvant to antigen-presenting cells without systemic exposure and allergic response. Here, we show a method for producing poly(lactide-co-glycolide) (PLG) NPs in an efficient, high-yield, and large-scale inhomogeneous precipitation process. The process enables the production of compositionally complex PLG NPs containing protein while also incorporating DNA and E. coli phospholipids as integral adjuvants in the NP vehicle. Orally delivered PLG NPs activate the murine immune system, and encapsulated peanut allergen protein elicits approximately 10-fold lower levels of basophil activation than does unencapsulated protein in basophils isolated from peanut-allergic patients. This efficacy and safety evidence makes these PLG NPs excellent candidates for clinical applications. Protein-loaded nanoparticles are important for immunomodulatory applications. Here, an efficient method for producing protein-containing nanoparticles at large scale is developed which overcomes prior limitations on the use of poly(lactide-co-glycolide) nanoparticles.","PeriodicalId":10589,"journal":{"name":"Communications Materials","volume":" ","pages":"1-11"},"PeriodicalIF":7.5,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s43246-024-00626-w.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142255249","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-16DOI: 10.1038/s43246-024-00632-y
Manisha Rajput, Sameer Kumar Mallik, Sagnik Chatterjee, Ashutosh Shukla, Sooyeon Hwang, Satyaprakash Sahoo, G. V. Pavan Kumar, Atikur Rahman
Two-dimensional transition metal dichalcogenides (TMDs)-based memristors are promising candidates for realizing artificial synapses in next-generation computing. However, practical implementation faces several challenges, such as high non-linearity and asymmetry in synaptic weight updates, limited dynamic range, and cycle-to-cycle variability. Here, utilizing optimal-power argon plasma treatment, we significantly enhance the performance matrix of memristors fabricated from monolayer MoS2. Our approach not only improves linearity and symmetry in synaptic weight updates but also increases the number of available synaptic weight updates and enhances Spike-Time Dependent Plasticity. Notably, it broadens the switching ratio by two orders, minimizes cycle-to-cycle variability, reduces non-linear factors, and achieves an energy consumption of ~30 fJ per synaptic event. Implementation of these enhancements is demonstrated through Artificial Neural Network simulations, yielding a learning accuracy of ~97% on the MNIST hand-written digits dataset. Our findings underscore the significance of defect engineering as a powerful tool in advancing the synaptic functionality of memristors. Memristors based on 2D materials are promising candidates for realizing artificial synapses in next-generation computing. Here, utilizing optimal-power argon plasma treatment, the authors enhance the performance of memristors fabricated from monolayer MoS2, reducing non-linearity and asymmetry in synaptic weight updates and minimizing cycle-to-cycle variability.
{"title":"Defect-engineered monolayer MoS2 with enhanced memristive and synaptic functionality for neuromorphic computing","authors":"Manisha Rajput, Sameer Kumar Mallik, Sagnik Chatterjee, Ashutosh Shukla, Sooyeon Hwang, Satyaprakash Sahoo, G. V. Pavan Kumar, Atikur Rahman","doi":"10.1038/s43246-024-00632-y","DOIUrl":"10.1038/s43246-024-00632-y","url":null,"abstract":"Two-dimensional transition metal dichalcogenides (TMDs)-based memristors are promising candidates for realizing artificial synapses in next-generation computing. However, practical implementation faces several challenges, such as high non-linearity and asymmetry in synaptic weight updates, limited dynamic range, and cycle-to-cycle variability. Here, utilizing optimal-power argon plasma treatment, we significantly enhance the performance matrix of memristors fabricated from monolayer MoS2. Our approach not only improves linearity and symmetry in synaptic weight updates but also increases the number of available synaptic weight updates and enhances Spike-Time Dependent Plasticity. Notably, it broadens the switching ratio by two orders, minimizes cycle-to-cycle variability, reduces non-linear factors, and achieves an energy consumption of ~30 fJ per synaptic event. Implementation of these enhancements is demonstrated through Artificial Neural Network simulations, yielding a learning accuracy of ~97% on the MNIST hand-written digits dataset. Our findings underscore the significance of defect engineering as a powerful tool in advancing the synaptic functionality of memristors. Memristors based on 2D materials are promising candidates for realizing artificial synapses in next-generation computing. Here, utilizing optimal-power argon plasma treatment, the authors enhance the performance of memristors fabricated from monolayer MoS2, reducing non-linearity and asymmetry in synaptic weight updates and minimizing cycle-to-cycle variability.","PeriodicalId":10589,"journal":{"name":"Communications Materials","volume":" ","pages":"1-14"},"PeriodicalIF":7.5,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s43246-024-00632-y.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142234031","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-14DOI: 10.1038/s43246-024-00633-x
Oleg Makarovsky, Richard J. A. Hill, Tin S. Cheng, Alex Summerfield, Takeshi Taniguchi, Kenji Watanabe, Christopher J. Mellor, Amalia Patanè, Laurence Eaves, Sergei V. Novikov, Peter H. Beton
Graphene placed on hexagonal boron nitride (hBN) has received significant interest due to its excellent electrical performance and physics phenomena, such as superlattice Dirac points. Direct molecular beam epitaxy growth of graphene on hBN offers an alternative fabrication route for hBN/graphene devices. Here, we investigate the electronic transport of moiré field effect transistors (FETs) in which the conducting channel is monolayer graphene grown on hexagonal boron nitride by high temperature molecular beam epitaxy (HT-MBE). Alignment between hBN and HT-MBE graphene crystal lattices gives rise to a moiré-fringed hexagonal superlattice pattern. Its electronic band structure takes the form of a “Hofstadter butterfly”. When a strong magnetic field B is applied perpendicular to the graphene layer, the electrical conductance displays magneto-oscillations, periodic in B−1, over a wide range of gate voltages and temperatures up to 350 K. We attribute this behaviour to the quantisation of electronic charge and magnetic flux within each unit cell of the superlattice, which gives rise to so-called Brown-Zak oscillations, previously reported only in high-mobility exfoliated graphene. Thus, this HT-MBE graphene/hBN heterostructure provides a platform for observation of room temperature quantum effects and device applications. Moiré field-effect transistors based on graphene/hexagonal boron nitride heterostructures are promising for their high room-temperature carrier mobilities and magnetotransport properties. Here, high-temperature molecular beam epitaxy growth of graphene/hBN gives rise to a moiré-fringed hexagonal superlattice with Hofstadter butterfly electronic band structure and quantum magneto-oscillations above room temperature.
置于六方氮化硼（hBN）上的石墨烯因其优异的电气性能和超晶格狄拉克点等物理现象而备受关注。石墨烯在六方氮化硼上的直接分子束外延生长为六方氮化硼/石墨烯器件的制造提供了另一种途径。在这里，我们研究了摩尔场效应晶体管（FET）的电子传输，其中导电通道是通过高温分子束外延（HT-MBE）生长在六方氮化硼上的单层石墨烯。氮化硼和 HT-MBE 石墨烯晶格之间的排列产生了摩尔边六边形超晶格图案。其电子能带结构呈 "霍夫斯塔特蝴蝶 "状。当施加垂直于石墨烯层的强磁场 B 时，电导率在广泛的栅极电压和高达 350 K 的温度范围内显示出以 B-1 为周期的磁振荡。我们将这种行为归因于超晶格每个单元格内的电子电荷和磁通量的量化，从而产生了所谓的布朗-扎克振荡，这种振荡以前只在高迁移率剥离石墨烯中报道过。因此，这种 HT-MBE 石墨烯/hBN 异质结构为观察室温量子效应和器件应用提供了一个平台。基于石墨烯/六方氮化硼异质结构的莫伊里场效应晶体管具有很高的室温载流子迁移率和磁传输特性，因此前景广阔。在这里，石墨烯/六方氮化硼的高温分子束外延生长产生了具有霍夫施塔特蝶形电子能带结构和室温以上量子磁振荡的摩尔边六方超晶格。
{"title":"High-temperature Brown-Zak oscillations in graphene/hBN moiré field effect transistor fabricated using molecular beam epitaxy","authors":"Oleg Makarovsky, Richard J. A. Hill, Tin S. Cheng, Alex Summerfield, Takeshi Taniguchi, Kenji Watanabe, Christopher J. Mellor, Amalia Patanè, Laurence Eaves, Sergei V. Novikov, Peter H. Beton","doi":"10.1038/s43246-024-00633-x","DOIUrl":"10.1038/s43246-024-00633-x","url":null,"abstract":"Graphene placed on hexagonal boron nitride (hBN) has received significant interest due to its excellent electrical performance and physics phenomena, such as superlattice Dirac points. Direct molecular beam epitaxy growth of graphene on hBN offers an alternative fabrication route for hBN/graphene devices. Here, we investigate the electronic transport of moiré field effect transistors (FETs) in which the conducting channel is monolayer graphene grown on hexagonal boron nitride by high temperature molecular beam epitaxy (HT-MBE). Alignment between hBN and HT-MBE graphene crystal lattices gives rise to a moiré-fringed hexagonal superlattice pattern. Its electronic band structure takes the form of a “Hofstadter butterfly”. When a strong magnetic field B is applied perpendicular to the graphene layer, the electrical conductance displays magneto-oscillations, periodic in B−1, over a wide range of gate voltages and temperatures up to 350 K. We attribute this behaviour to the quantisation of electronic charge and magnetic flux within each unit cell of the superlattice, which gives rise to so-called Brown-Zak oscillations, previously reported only in high-mobility exfoliated graphene. Thus, this HT-MBE graphene/hBN heterostructure provides a platform for observation of room temperature quantum effects and device applications. Moiré field-effect transistors based on graphene/hexagonal boron nitride heterostructures are promising for their high room-temperature carrier mobilities and magnetotransport properties. Here, high-temperature molecular beam epitaxy growth of graphene/hBN gives rise to a moiré-fringed hexagonal superlattice with Hofstadter butterfly electronic band structure and quantum magneto-oscillations above room temperature.","PeriodicalId":10589,"journal":{"name":"Communications Materials","volume":" ","pages":"1-6"},"PeriodicalIF":7.5,"publicationDate":"2024-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s43246-024-00633-x.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142234035","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Most of the van der Waals homo- and hetero-junctions of group VIB two-dimensional (2D) transition-metal dichalcogenides (TMDs; MoS2, WS2, MoSe2, and WSe2) show indirect energy band gaps which hinders some of their applications especially in optoelectronics. In the current work, we demonstrate that most of the bilayers and even few-layers consisting of group VIB TMDs can have direct gaps by efficient weakening of their interlayer interactions via real and/or energy spaces tuning, which is based on insights from quantitative analyses of interlayer electronic hybridizations. Real space tuning here means introducing large-angle rotational misalignment between layers, which has been realized in a very recent experiment; and, energy space tuning means introducing energy mismatch between layers which can be introduced efficiently by different means thanks to the small vertical dielectric constant of 2D semiconducting TMDs. The efficient tuning in both real and energy spaces proposed here paves an avenue for indirect-direct gap regulation of homo- and hetero-junctions of TMDs and other 2D semiconductors. Notably, both tuning can be permanently preserved and hence our work is of great significance for the diverse applications of 2D semiconductors. Most van der Waals homo- and hetero-junctions of 2D transition-metal dichalcogenides of group VIB have indirect bandgaps. Here, the authors demonstrate a way of inducing direct gaps in these systems by tuning interlayer interactions via rotational misalignment or energy mismatch between layers.
{"title":"Toward direct band gaps in typical 2D transition-metal dichalcogenides junctions via real and energy spaces tuning","authors":"Mei-Yan Tian, Yu-Meng Gao, Yue-Jiao Zhang, Meng-Xue Ren, Xiao-Huan Lv, Ke-Xin Hou, Chen-Dong Jin, Hu Zhang, Ru-Qian Lian, Peng-Lai Gong, Rui-Ning Wang, Jiang-Long Wang, Xing-Qiang Shi","doi":"10.1038/s43246-024-00631-z","DOIUrl":"10.1038/s43246-024-00631-z","url":null,"abstract":"Most of the van der Waals homo- and hetero-junctions of group VIB two-dimensional (2D) transition-metal dichalcogenides (TMDs; MoS2, WS2, MoSe2, and WSe2) show indirect energy band gaps which hinders some of their applications especially in optoelectronics. In the current work, we demonstrate that most of the bilayers and even few-layers consisting of group VIB TMDs can have direct gaps by efficient weakening of their interlayer interactions via real and/or energy spaces tuning, which is based on insights from quantitative analyses of interlayer electronic hybridizations. Real space tuning here means introducing large-angle rotational misalignment between layers, which has been realized in a very recent experiment; and, energy space tuning means introducing energy mismatch between layers which can be introduced efficiently by different means thanks to the small vertical dielectric constant of 2D semiconducting TMDs. The efficient tuning in both real and energy spaces proposed here paves an avenue for indirect-direct gap regulation of homo- and hetero-junctions of TMDs and other 2D semiconductors. Notably, both tuning can be permanently preserved and hence our work is of great significance for the diverse applications of 2D semiconductors. Most van der Waals homo- and hetero-junctions of 2D transition-metal dichalcogenides of group VIB have indirect bandgaps. Here, the authors demonstrate a way of inducing direct gaps in these systems by tuning interlayer interactions via rotational misalignment or energy mismatch between layers.","PeriodicalId":10589,"journal":{"name":"Communications Materials","volume":" ","pages":"1-9"},"PeriodicalIF":7.5,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s43246-024-00631-z.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142234042","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-12DOI: 10.1038/s43246-024-00624-y
Ani Vardanyan, Guojun Zhou, Nayoung Kim, Tetyana M. Budnyak, Vadim G. Kessler, Insung S. Choi, Zhehao Huang, Gulaim A. Seisenbaeva
Metal-organic frameworks (MOFs) have emerged as highly promising materials for hosting functional biomolecules. Here, a 1,2,4-benzenetricarboxylate ligand with a flat asymmetric shape is applied to infuse an unusual behavior to a 3D europium MOF (SLU-1). Solvent addition results in the 3D MOF splitting into a 2D one (SLU-2), and in the presence of excess water, gets cross-linked into a different 3D MOF (SLU-3) prone to spontaneous exfoliation. SLU-3 features a combination of highly hydrophilic and hydrophobic spots and serves as an attractive host for incorporating large active species. As a representative demonstration, horseradish peroxidase (HRP) is incorporated into the exfoliated 3D-layered structure by simple mixing, and secured by an outer silica layer in the form of core-shell structures. The resulting HRP-based biocatalyst exhibited enhanced stability and reusability, effectively degrading phenol. This work showcases the potential of reconfigurable MOFs, offering upheld applications through the controlled uptake and retention of biocatalytic agents. Metal-organic frameworks are promising materials for hosting functional biomolecules. Here, a 3D europium metal-organic framework could split into a 2D one upon solvent addition and re-cross-link to 3D with excess solvent which can host enzymes as a biocatalyst.
{"title":"Transformation of europium metal-organic framework from 3D via 2D into exfoliating 3D for enzyme immobilization","authors":"Ani Vardanyan, Guojun Zhou, Nayoung Kim, Tetyana M. Budnyak, Vadim G. Kessler, Insung S. Choi, Zhehao Huang, Gulaim A. Seisenbaeva","doi":"10.1038/s43246-024-00624-y","DOIUrl":"10.1038/s43246-024-00624-y","url":null,"abstract":"Metal-organic frameworks (MOFs) have emerged as highly promising materials for hosting functional biomolecules. Here, a 1,2,4-benzenetricarboxylate ligand with a flat asymmetric shape is applied to infuse an unusual behavior to a 3D europium MOF (SLU-1). Solvent addition results in the 3D MOF splitting into a 2D one (SLU-2), and in the presence of excess water, gets cross-linked into a different 3D MOF (SLU-3) prone to spontaneous exfoliation. SLU-3 features a combination of highly hydrophilic and hydrophobic spots and serves as an attractive host for incorporating large active species. As a representative demonstration, horseradish peroxidase (HRP) is incorporated into the exfoliated 3D-layered structure by simple mixing, and secured by an outer silica layer in the form of core-shell structures. The resulting HRP-based biocatalyst exhibited enhanced stability and reusability, effectively degrading phenol. This work showcases the potential of reconfigurable MOFs, offering upheld applications through the controlled uptake and retention of biocatalytic agents. Metal-organic frameworks are promising materials for hosting functional biomolecules. Here, a 3D europium metal-organic framework could split into a 2D one upon solvent addition and re-cross-link to 3D with excess solvent which can host enzymes as a biocatalyst.","PeriodicalId":10589,"journal":{"name":"Communications Materials","volume":" ","pages":"1-10"},"PeriodicalIF":7.5,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s43246-024-00624-y.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142206413","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-12DOI: 10.1038/s43246-024-00576-3
Farshad Jafarzadeh, Luigi Angelo Castriotta, Emanuele Calabrò, Pierpaolo Spinelli, Amanda Generosi, Barbara Paci, David Becerril Rodriguez, Marco Luce, Antonio Cricenti, Francesco Di Giacomo, Fabio Matteocci, Francesca Brunetti, Aldo Di Carlo
Perovskite solar cells have rapidly advanced, achieving over 26% power conversion efficiency on the laboratory scale. However, transitioning to large-scale production remains a challenge due to limitations in conventional fabrication methods like spin coating. Here, we introduce an optimized blade coating process for the scalable fabrication of large-area (15 cm × 15 cm) perovskite solar modules with a nickel oxide hole transport layer, performed in ambient air and utilizing a non-toxic solvent system. Self-assembled monolayers between the nickel oxide and perovskite layer improve the uniformity and morphology of the perovskite film. Perovskite solar modules with a 110 cm2 active area achieve a power conversion efficiency of 12.6%. Moreover, encapsulated modules retained 84% of their initial efficiency after 1,000 hours at 85 °C in air (ISOS-T-1). This study demonstrates progress in the large-scale production of perovskite solar cells that combine efficiency with long-term stability. Perovskite solar cells and have shown great promise on the lab scale, but work is needed to scale-up their fabrication. Here, blade coating is used to fabricate 15 cm×15 cm perovskite modules with a nickel oxide hole transport layer, achieving high power conversion efficiency and stability.
{"title":"Stable and sustainable perovskite solar modules by optimizing blade coating nickel oxide deposition over 15 × 15 cm2 area","authors":"Farshad Jafarzadeh, Luigi Angelo Castriotta, Emanuele Calabrò, Pierpaolo Spinelli, Amanda Generosi, Barbara Paci, David Becerril Rodriguez, Marco Luce, Antonio Cricenti, Francesco Di Giacomo, Fabio Matteocci, Francesca Brunetti, Aldo Di Carlo","doi":"10.1038/s43246-024-00576-3","DOIUrl":"10.1038/s43246-024-00576-3","url":null,"abstract":"Perovskite solar cells have rapidly advanced, achieving over 26% power conversion efficiency on the laboratory scale. However, transitioning to large-scale production remains a challenge due to limitations in conventional fabrication methods like spin coating. Here, we introduce an optimized blade coating process for the scalable fabrication of large-area (15 cm × 15 cm) perovskite solar modules with a nickel oxide hole transport layer, performed in ambient air and utilizing a non-toxic solvent system. Self-assembled monolayers between the nickel oxide and perovskite layer improve the uniformity and morphology of the perovskite film. Perovskite solar modules with a 110 cm2 active area achieve a power conversion efficiency of 12.6%. Moreover, encapsulated modules retained 84% of their initial efficiency after 1,000 hours at 85 °C in air (ISOS-T-1). This study demonstrates progress in the large-scale production of perovskite solar cells that combine efficiency with long-term stability. Perovskite solar cells and have shown great promise on the lab scale, but work is needed to scale-up their fabrication. Here, blade coating is used to fabricate 15 cm×15 cm perovskite modules with a nickel oxide hole transport layer, achieving high power conversion efficiency and stability.","PeriodicalId":10589,"journal":{"name":"Communications Materials","volume":" ","pages":"1-9"},"PeriodicalIF":7.5,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s43246-024-00576-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142206414","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-12DOI: 10.1038/s43246-024-00611-3
Max L. Neveau, William R. Meier, Hyojin Park, Michael J. Thompson, Nitish Bibhanshu, Catrin Böcher, Tomer Fishman, David Weiss, Matthew F. Chisholm, Orlando Rios, Gerd Duscher
Alloying in metal castings is one of the principal methods of strengthening an alloy for various structural and functional applications, but very rarely does it modify an alloy’s elastic modulus. We report a methodology of combining isostructural Laves phases to form a multi-component, high symmetry, isotropic phase that was discovered to enhance the elastic modulus of a cast aluminum alloy to 91.5 ± 7.4 GPa. Flux grown single crystals of the rhombicuboctahedron phase (RCO), so named for the observed morphology, were used to enhance understanding of the structure and mechanical properties of the phase. The pure RCO phase’s structure and site occupancies were co-refined using x-ray and neutron diffraction. Dynamic nanomechanical testing of the cast alloy shows the primary RCO phase has a high, relatively isotropic, elastic modulus. This RCO containing aluminum alloy is found to have a specific modulus that exceeds that of the leading Al, Mg, Steel, and Ti alloys. The elastic properties of alloys are typically insensitive to changes in microstructure. Here, an as-cast Al-Ce alloy achieves a large Young’s modulus of approximately 92 GPa, due to the presence of isotropic, high symmetry secondary phase.
{"title":"Secondary phase increases the elastic modulus of a cast aluminum-cerium alloy","authors":"Max L. Neveau, William R. Meier, Hyojin Park, Michael J. Thompson, Nitish Bibhanshu, Catrin Böcher, Tomer Fishman, David Weiss, Matthew F. Chisholm, Orlando Rios, Gerd Duscher","doi":"10.1038/s43246-024-00611-3","DOIUrl":"10.1038/s43246-024-00611-3","url":null,"abstract":"Alloying in metal castings is one of the principal methods of strengthening an alloy for various structural and functional applications, but very rarely does it modify an alloy’s elastic modulus. We report a methodology of combining isostructural Laves phases to form a multi-component, high symmetry, isotropic phase that was discovered to enhance the elastic modulus of a cast aluminum alloy to 91.5 ± 7.4 GPa. Flux grown single crystals of the rhombicuboctahedron phase (RCO), so named for the observed morphology, were used to enhance understanding of the structure and mechanical properties of the phase. The pure RCO phase’s structure and site occupancies were co-refined using x-ray and neutron diffraction. Dynamic nanomechanical testing of the cast alloy shows the primary RCO phase has a high, relatively isotropic, elastic modulus. This RCO containing aluminum alloy is found to have a specific modulus that exceeds that of the leading Al, Mg, Steel, and Ti alloys. The elastic properties of alloys are typically insensitive to changes in microstructure. Here, an as-cast Al-Ce alloy achieves a large Young’s modulus of approximately 92 GPa, due to the presence of isotropic, high symmetry secondary phase.","PeriodicalId":10589,"journal":{"name":"Communications Materials","volume":" ","pages":"1-9"},"PeriodicalIF":7.5,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s43246-024-00611-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142206415","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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