Pub Date : 2025-04-24DOI: 10.1016/j.actamat.2025.121042
Abdelrahman Hussein, Margo Cauwels, Lisa Claeys, Tom Depover, Kim Verbeken
We present a fully kinetic, full-field model for hydrogen diffusion and trapping in two-phase microstructures. Trapping is described by a flux directed toward the center of trapping sites, spatially and temporally resolving the trapping kinetics. The model is used to analyze thermal desorption spectroscopy (TDS) in duplex stainless steel (DSS) under different charging times, showing good agreement with experimental results. We found that the charging time has a substantial effect on the shape of TDS curves and the underlying desorption kinetics. The 1-day charging condition resulted in accumulation of hydrogen at the edges compared to the bulk. The TDS curve for this condition is characterized by a main peak followed by a high-temperature tail. Analyzing the simulation results showed that the majority of the hydrogen accumulated at the edges desorbed, creating the main peak. The remaining fraction of this hydrogen diffused inward toward the center before desorbing, generating the tail. The 15-day charging and fully saturated conditions resulted in a shoulder preceding the main peak. Our analysis showed that in the low-temperature range of the TDS curve, fast desorption from the ferrite phase creates the shoulder. At higher temperatures, diffusion in the austenite phase accelerates, increasing the overall desorption rate and resulting in the main peak. The study concludes that the diffusion-based description provided by the presented model offers key details on desorption kinetics, particularly when the trapping phase is governed by diffusion, as in the case of DSS.
{"title":"A full-field model for hydrogen diffusion and trapping in two-phase microstructures: Application to thermal desorption spectroscopy of duplex stainless steel","authors":"Abdelrahman Hussein, Margo Cauwels, Lisa Claeys, Tom Depover, Kim Verbeken","doi":"10.1016/j.actamat.2025.121042","DOIUrl":"https://doi.org/10.1016/j.actamat.2025.121042","url":null,"abstract":"We present a fully kinetic, full-field model for hydrogen diffusion and trapping in two-phase microstructures. Trapping is described by a flux directed toward the center of trapping sites, spatially and temporally resolving the trapping kinetics. The model is used to analyze thermal desorption spectroscopy (TDS) in duplex stainless steel (DSS) under different charging times, showing good agreement with experimental results. We found that the charging time has a substantial effect on the shape of TDS curves and the underlying desorption kinetics. The 1-day charging condition resulted in accumulation of hydrogen at the edges compared to the bulk. The TDS curve for this condition is characterized by a main peak followed by a high-temperature tail. Analyzing the simulation results showed that the majority of the hydrogen accumulated at the edges desorbed, creating the main peak. The remaining fraction of this hydrogen diffused inward toward the center before desorbing, generating the tail. The 15-day charging and fully saturated conditions resulted in a shoulder preceding the main peak. Our analysis showed that in the low-temperature range of the TDS curve, fast desorption from the ferrite phase creates the shoulder. At higher temperatures, diffusion in the austenite phase accelerates, increasing the overall desorption rate and resulting in the main peak. The study concludes that the diffusion-based description provided by the presented model offers key details on desorption kinetics, particularly when the trapping phase is governed by diffusion, as in the case of DSS.","PeriodicalId":238,"journal":{"name":"Acta Materialia","volume":"20 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866273","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Rajwali Khan, Naveed Ur Rahman, Sujith Kalluri, Sundaravadivel Elumalai, Saritha Appukkuttan, Muhammad Fakhar E Alam, Muhammad Ikram, Sherzod Shukhratovich Abdullaev, Nasir Rahman, Sambasivam Sangaraju
The potential of two-dimensional (2D) transition metal dichalcogenides (TMDs), especially molybdenum telluride (MoTe₂), in sophisticated electrical and low-energy neuromorphic applications, has attracted a lot of interest. The creation, characteristics, and uses of MoTe₂-based memristive devices are summarized in this review paper, with an emphasis on their potential as artificial synapses for neuromorphic computing. We thoroughly examine the special properties of MoTe₂, such as its remarkable resistance switching response, excellent linearity in synaptic potentiation, and customizable phase states. These characteristics make it possible to implement basic computational functions with minimal energy consumption, including decimal arithmetic operations and the commutative principles of addition and multiplication. In addition to simulating intricate synaptic processes such as long-term potentiation (LTP), long-term depression (LTD), and spike-timing-dependent plasticity (STDP), the article emphasizes experimental performances of MoTe₂ memristors, which include their capacity to execute exact decimal arithmetic operations. The demonstration of centimeter-scale 2D MoTe₂ film-based memristor arrays attaining over 90% recognition accuracy in handwritten digit identification tests further demonstrates the devices great scalability, stability, and incorporation capabilities. Notwithstanding these developments, issues such poor environmental robustness, phase transition sensitivity, and low thermal stability still exist. The creation of hybrid or composite materials, doping, and structural alteration are some of the methods to get beyond these obstacles that are covered in the paper. The need for scalable, economical synthesis techniques and a better comprehension of the materials mechanical, optical, and electrical properties through modeling and experiments are emphasized.
{"title":"2D Material-Based Memristors for Low Energy Consumption Artificial Synapses for Neuromorphic Responses","authors":"Rajwali Khan, Naveed Ur Rahman, Sujith Kalluri, Sundaravadivel Elumalai, Saritha Appukkuttan, Muhammad Fakhar E Alam, Muhammad Ikram, Sherzod Shukhratovich Abdullaev, Nasir Rahman, Sambasivam Sangaraju","doi":"10.1039/d5nr01509j","DOIUrl":"https://doi.org/10.1039/d5nr01509j","url":null,"abstract":"The potential of two-dimensional (2D) transition metal dichalcogenides (TMDs), especially molybdenum telluride (MoTe₂), in sophisticated electrical and low-energy neuromorphic applications, has attracted a lot of interest. The creation, characteristics, and uses of MoTe₂-based memristive devices are summarized in this review paper, with an emphasis on their potential as artificial synapses for neuromorphic computing. We thoroughly examine the special properties of MoTe₂, such as its remarkable resistance switching response, excellent linearity in synaptic potentiation, and customizable phase states. These characteristics make it possible to implement basic computational functions with minimal energy consumption, including decimal arithmetic operations and the commutative principles of addition and multiplication. In addition to simulating intricate synaptic processes such as long-term potentiation (LTP), long-term depression (LTD), and spike-timing-dependent plasticity (STDP), the article emphasizes experimental performances of MoTe₂ memristors, which include their capacity to execute exact decimal arithmetic operations. The demonstration of centimeter-scale 2D MoTe₂ film-based memristor arrays attaining over 90% recognition accuracy in handwritten digit identification tests further demonstrates the devices great scalability, stability, and incorporation capabilities. Notwithstanding these developments, issues such poor environmental robustness, phase transition sensitivity, and low thermal stability still exist. The creation of hybrid or composite materials, doping, and structural alteration are some of the methods to get beyond these obstacles that are covered in the paper. The need for scalable, economical synthesis techniques and a better comprehension of the materials mechanical, optical, and electrical properties through modeling and experiments are emphasized.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"6 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866369","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jia Cao, Xiongyi Liang, Wei Gao, Di Yin, Xiuming Bu, Siwei Yang, Chuqian Xiao, Shaoyan Wang, Xiao-Cheng Zeng, Johnny C Ho, Xianying Wang
A stable and efficient RuO2-based electrocatalyst for the acidic oxygen evolution reaction (OER) is essential to replace the current IrO2 anode in proton-exchange membrane water electrolysis (PEMWE). In this research, we introduce RuO2 catalysts designed with coexisting oxygen and ruthenium vacancies using a metal-organic pyrolysis method. Our experimental and theoretical analyses indicate that the OER pathway varies with different facets. Oxygen vacancies are crucial as they elevate the energy barrier for additional Ru vacancy formation during the in-situ surface reconstruction, thus stabilizing the (110) and (101) facets. Notably, Ru vacancies in the (101) facet activate lattice oxygen, allowing rapid replenishment of depleted lattice oxygen and enabling a reversible lattice oxygen participation (LOM) cycling process. As a result, the catalyst, mainly exposing the (101) facet, exhibits outstanding stability, operating continuously in custom-assembled PEMWEs at 100 mA cm-2 for 200 hours via the LOM pathway. This advancement opens the door to more robust and efficient catalysts for water electrolysis applications.
{"title":"Reversible Lattice Oxygen Participation in Ru1-xO2-x for Superior Acidic Oxygen Evolution Reaction","authors":"Jia Cao, Xiongyi Liang, Wei Gao, Di Yin, Xiuming Bu, Siwei Yang, Chuqian Xiao, Shaoyan Wang, Xiao-Cheng Zeng, Johnny C Ho, Xianying Wang","doi":"10.1039/d5ta01484k","DOIUrl":"https://doi.org/10.1039/d5ta01484k","url":null,"abstract":"A stable and efficient RuO2-based electrocatalyst for the acidic oxygen evolution reaction (OER) is essential to replace the current IrO2 anode in proton-exchange membrane water electrolysis (PEMWE). In this research, we introduce RuO<small><sub>2</sub></small> catalysts designed with coexisting oxygen and ruthenium vacancies using a metal-organic pyrolysis method. Our experimental and theoretical analyses indicate that the OER pathway varies with different facets. Oxygen vacancies are crucial as they elevate the energy barrier for additional Ru vacancy formation during the in-situ surface reconstruction, thus stabilizing the (110) and (101) facets. Notably, Ru vacancies in the (101) facet activate lattice oxygen, allowing rapid replenishment of depleted lattice oxygen and enabling a reversible lattice oxygen participation (LOM) cycling process. As a result, the catalyst, mainly exposing the (101) facet, exhibits outstanding stability, operating continuously in custom-assembled PEMWEs at 100 mA cm<small><sup>-2</sup></small> for 200 hours via the LOM pathway. This advancement opens the door to more robust and efficient catalysts for water electrolysis applications.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"35 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866542","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zhichao Yu, Lun Li, Keyu An, Hongling Liu, Xingshuai Lv, Weng Fai Ip, Hui Pan
The search for efficient Haber–Bosch catalysts toward ammonia production under mild conditions is never-ending, which is greatly limited by the Brønsted–Evans–Polanyi (BEP) relationship. Great efforts have been put into optimizing the BEP relations and achieving the Sabatier optimum, which requires a balance between the dissociation and hydrogenation of nitrogen. However, challenges in this field inspire us to believe that completely breaking the linear BEP relations is indeed the final target although out of sight in such a holy grail reaction. Here, based on the first-principles calculations, we discover inverted trends of BEP relation of N2 dissociation to approach the kinetic optimum of ammonia synthesis on Fe-based single-atom alloys. It is found that the adsorption characteristic of N–N transition states follows the 10-electron count rule, while that of the final states mimics the d-band model, which accounts for the inversion. Crystal orbital Hamiltonian populations (COHP) and Bader charge analysis further corroborate that a bonding-dependent adsorption mechanism lies at the root of the inverted trends of the BEP relation. Our finding not only paves the way for the milder Haber–Bosch process but also promotes explorations of breaking the linear BEP relations of the critical steps in various chemical reactions.
{"title":"Inverted Trends of the Brønsted–Evans–Polanyi Relation in N2 Dissociation Originated from a Bonding-Dependent Adsorption Mechanism","authors":"Zhichao Yu, Lun Li, Keyu An, Hongling Liu, Xingshuai Lv, Weng Fai Ip, Hui Pan","doi":"10.1021/acsami.4c21214","DOIUrl":"https://doi.org/10.1021/acsami.4c21214","url":null,"abstract":"The search for efficient Haber–Bosch catalysts toward ammonia production under mild conditions is never-ending, which is greatly limited by the Brønsted–Evans–Polanyi (BEP) relationship. Great efforts have been put into optimizing the BEP relations and achieving the Sabatier optimum, which requires a balance between the dissociation and hydrogenation of nitrogen. However, challenges in this field inspire us to believe that completely breaking the linear BEP relations is indeed the final target although out of sight in such a holy grail reaction. Here, based on the first-principles calculations, we discover inverted trends of BEP relation of N<sub>2</sub> dissociation to approach the kinetic optimum of ammonia synthesis on Fe-based single-atom alloys. It is found that the adsorption characteristic of N–N transition states follows the 10-electron count rule, while that of the final states mimics the d-band model, which accounts for the inversion. Crystal orbital Hamiltonian populations (COHP) and Bader charge analysis further corroborate that a bonding-dependent adsorption mechanism lies at the root of the inverted trends of the BEP relation. Our finding not only paves the way for the milder Haber–Bosch process but also promotes explorations of breaking the linear BEP relations of the critical steps in various chemical reactions.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"261 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866579","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Repair and regeneration of oral and maxillofacial tissue defects remain significant challenges, mainly due to the limitations of existing treatment approaches. Conventional methods such as transplantation, tissue scaffolds, growth factors, and stem cell therapies often face obstacles, including donor shortages, insufficient vascularization, and safety concerns. There is an urgent need for innovative therapeutic strategies to effectively promote vascular regeneration while minimizing complications. Black phosphorus nanosheets (BPNSs) and hydrogels present significant advantages and broad application potential as tissue regeneration carriers due to their biocompatibility, degradability, and controlled drug release properties. By combining various characterization techniques and detection methods, we conducted a thorough analysis of BPNSs and gelatin methacryloyl (GelMA) scaffolds loaded with BPNSs (BP-GelMA). The results indicate that this study successfully prepared BPNSs with uniform size, good dispersion, and intact structure. Moreover, the BP-GelMA composite demonstrated excellent swelling behavior and structural stability while effectively enabling the controlled release of BPNSs. This study investigated the angiogenic effects of BP-GelMA at concentrations of 0, 12.5, and 25.0 μg/mL. In vitro experiments showed that BP-GelMA significantly enhanced endothelial cell proliferation, migration, and tube formation. In vivo results demonstrated that 12.5 μg/mL and 25.0 μg/mL BP-GelMA did not induce significant developmental toxicity in zebrafish and effectively promoted neovascularization. RNA-Seq analysis revealed that BP-GelMA activates angiogenesis-related biological processes. Mechanistic studies identified PEAK1 as a central regulator, driving vascular formation through activation of the MAPK signaling pathway. These findings highlight the potential of BP-GelMA as a therapeutic strategy for promoting angiogenesis and underscore the importance of optimizing BP-GelMA concentrations to achieve maximum therapeutic efficacy and safety in clinical applications.
{"title":"Black Phosphorus-Loaded Gelatin Methacryloyl Hydrogels Enhance Angiogenesis via Activation of the PEAK1–MAPK Pathway","authors":"Ruoting Xian, Hongyi Xian, Hao Dong, Jiating Lin, Xianxian Zhuang, Yue Zou, Qinkai Xie, Youde Liang, Shaobing Li","doi":"10.1021/acsami.5c02054","DOIUrl":"https://doi.org/10.1021/acsami.5c02054","url":null,"abstract":"Repair and regeneration of oral and maxillofacial tissue defects remain significant challenges, mainly due to the limitations of existing treatment approaches. Conventional methods such as transplantation, tissue scaffolds, growth factors, and stem cell therapies often face obstacles, including donor shortages, insufficient vascularization, and safety concerns. There is an urgent need for innovative therapeutic strategies to effectively promote vascular regeneration while minimizing complications. Black phosphorus nanosheets (BPNSs) and hydrogels present significant advantages and broad application potential as tissue regeneration carriers due to their biocompatibility, degradability, and controlled drug release properties. By combining various characterization techniques and detection methods, we conducted a thorough analysis of BPNSs and gelatin methacryloyl (GelMA) scaffolds loaded with BPNSs (BP-GelMA). The results indicate that this study successfully prepared BPNSs with uniform size, good dispersion, and intact structure. Moreover, the BP-GelMA composite demonstrated excellent swelling behavior and structural stability while effectively enabling the controlled release of BPNSs. This study investigated the angiogenic effects of BP-GelMA at concentrations of 0, 12.5, and 25.0 μg/mL. <i>In vitro</i> experiments showed that BP-GelMA significantly enhanced endothelial cell proliferation, migration, and tube formation. <i>In vivo</i> results demonstrated that 12.5 μg/mL and 25.0 μg/mL BP-GelMA did not induce significant developmental toxicity in zebrafish and effectively promoted neovascularization. RNA-Seq analysis revealed that BP-GelMA activates angiogenesis-related biological processes. Mechanistic studies identified PEAK1 as a central regulator, driving vascular formation through activation of the MAPK signaling pathway. These findings highlight the potential of BP-GelMA as a therapeutic strategy for promoting angiogenesis and underscore the importance of optimizing BP-GelMA concentrations to achieve maximum therapeutic efficacy and safety in clinical applications.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"138 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866589","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Distinct clinical phenotypes of periodontitis are associated with specific microbiome profiles and diverse inflammatory conditions. Current drug delivery systems face challenges in precisely modulating this dynamic microenvironment. Effective inhibition of bone resorption can only be achieved through a strategic response to bacterial infections and inflammation within the periodontal pocket, followed by prompt treatment tailored to disease severity. In this study, tannic acid (TA) is loaded into hollow mesoporous silica nanoparticles (HMSNs) that are functionalized with positively charged polyarginines (R8) and negatively charged human serum albumin (HSA). These HMSNs‐R8@TA‐HSA (HRT) nanoparticles are then encapsulated within an injectable Nap‐Gly‐Phe‐Phe‐Tyr‐OH (NapGFFY) hydrogel (NHRT). The intermediate linker R8 can interact with both arginine gingipain A (RgpA) and reactive oxygen species (ROS), which serve as markers of bacterial infections and inflammation, respectively. HSA, arginine, TA, and nitric oxide are differentially released from the hydrogel in response to varying concentrations of RgpA and ROS, demonstrating excellent antibacterial, antioxidant, and anti‐inflammatory properties. This smart RgpA/ROS dual‐responsive and injectable hydrogel with multifunctional therapy provides new prospects for the management of periodontitis.
{"title":"A Smart Injectable Hydrogel with Dual Responsivity to Arginine Gingipain A and Reactive Oxygen Species for Multifunctional Therapy of Periodontitis","authors":"Xuejing Li, Zhanwei Zhang, Jian Xie, Bangping Cao, Xin Wang, Yiqiang Yu, Jiansheng Su","doi":"10.1002/smll.202408034","DOIUrl":"https://doi.org/10.1002/smll.202408034","url":null,"abstract":"Distinct clinical phenotypes of periodontitis are associated with specific microbiome profiles and diverse inflammatory conditions. Current drug delivery systems face challenges in precisely modulating this dynamic microenvironment. Effective inhibition of bone resorption can only be achieved through a strategic response to bacterial infections and inflammation within the periodontal pocket, followed by prompt treatment tailored to disease severity. In this study, tannic acid (TA) is loaded into hollow mesoporous silica nanoparticles (HMSNs) that are functionalized with positively charged polyarginines (R8) and negatively charged human serum albumin (HSA). These HMSNs‐R8@TA‐HSA (HRT) nanoparticles are then encapsulated within an injectable Nap‐Gly‐Phe‐Phe‐Tyr‐OH (NapGFFY) hydrogel (NHRT). The intermediate linker R8 can interact with both arginine gingipain A (RgpA) and reactive oxygen species (ROS), which serve as markers of bacterial infections and inflammation, respectively. HSA, arginine, TA, and nitric oxide are differentially released from the hydrogel in response to varying concentrations of RgpA and ROS, demonstrating excellent antibacterial, antioxidant, and anti‐inflammatory properties. This smart RgpA/ROS dual‐responsive and injectable hydrogel with multifunctional therapy provides new prospects for the management of periodontitis.","PeriodicalId":228,"journal":{"name":"Small","volume":"6 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866651","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
José Manuel Ramón, José G. Sánchez, Miriam Más‐Montoya, Wenhui Li, Eugenia Martínez‐Ferrero, Emilio Palomares, David Curiel
The application of self‐assembled molecules (SAMs) as selective charge transport layers in inverted perovskite solar cells (iPSCs) has attracted significant interest because of their ability to provide high‐efficiency and stable devices. In this work, four dipodal SAMs are reported based on π‐expanded indolo[2,3‐a]carbazole, incorporated as hole‐selective contacts in iPSCs. The presence of methoxy substituents and the spacer length in SAMs are modified to assess their influence on the device performance. For that, the ITO/SAM and ITO/SAM/PSCs interfaces are characterized in detail, including theoretical studies and analysis of the complete device performance. These results demonstrate the multifactorial effect that SAMs have on the growth of crystalline perovskite and the charge dynamics in the devices. The resulting iPSCs show power conversion efficiency (PCE) between 19.76% and 22.20% with fill factors exceeding 82% in all cases and good stability under continuous illumination. Notably, SAM combining unsubstituted indolocarbazole and longer pentyl spacer (5CPICZ) shows the highest PCE of 22.20%. In contrast, analogous SAMs with propyl spacers (3CPICZ) achiev a PCE of 22.01%. The experimental results reveal that the improved PCE reached with unsubstituted indolocarbazole SAMs is attributed to reduced charge recombination and longer carrier lifetime owing to effective perovskite surface passivation.
{"title":"Revealing the Role of Spacer Length and Methoxy Substitution of Dipodal Indolocarbazole‐based SAMs on the Performance of Inverted Perovskite Solar Cells","authors":"José Manuel Ramón, José G. Sánchez, Miriam Más‐Montoya, Wenhui Li, Eugenia Martínez‐Ferrero, Emilio Palomares, David Curiel","doi":"10.1002/smll.202500067","DOIUrl":"https://doi.org/10.1002/smll.202500067","url":null,"abstract":"The application of self‐assembled molecules (SAMs) as selective charge transport layers in inverted perovskite solar cells (iPSCs) has attracted significant interest because of their ability to provide high‐efficiency and stable devices. In this work, four dipodal SAMs are reported based on π‐expanded indolo[2,3‐<jats:italic>a</jats:italic>]carbazole, incorporated as hole‐selective contacts in iPSCs. The presence of methoxy substituents and the spacer length in SAMs are modified to assess their influence on the device performance. For that, the ITO/SAM and ITO/SAM/PSCs interfaces are characterized in detail, including theoretical studies and analysis of the complete device performance. These results demonstrate the multifactorial effect that SAMs have on the growth of crystalline perovskite and the charge dynamics in the devices. The resulting iPSCs show power conversion efficiency (PCE) between 19.76% and 22.20% with fill factors exceeding 82% in all cases and good stability under continuous illumination. Notably, SAM combining unsubstituted indolocarbazole and longer pentyl spacer (5CPICZ) shows the highest PCE of 22.20%. In contrast, analogous SAMs with propyl spacers (3CPICZ) achiev a PCE of 22.01%. The experimental results reveal that the improved PCE reached with unsubstituted indolocarbazole SAMs is attributed to reduced charge recombination and longer carrier lifetime owing to effective perovskite surface passivation.","PeriodicalId":228,"journal":{"name":"Small","volume":"24 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866652","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Alvin Joseph, Anitha B. Pillai, Muthukrishnan Sundaram, Birabar Ranjit Kumar Nanda, Manoj A. G. Namboothiry
The reliability of performance metrics in organic photodiodes (OPDs) is a fundamental factor for their efficacy in real‐time applications. Among these metrics, the dark current density stands out for its direct impact on the sensitivity of the detectors. In this study, an anomalous illumination‐sensitive variation in dark current is observed in fabricated near‐infrared OPDs, which undermines the device reliability. The systematic investigation reveals that this behavior stems from the photocatalytic nature of zinc oxide (ZnO), the electron transport layer used in the OPD. The photocatalytic nature of ZnO detrimentally affects the stability of the active material, particularly the nonfullerene acceptor employed in this study. Through robust interface engineering approach, which involves modifying the interface between ZnO and the active layer, the anomalies in the dark current are successfully mitigated, enhancing the consistency and reliability of the OPDs. In addition to reducing the dark current, this interface engineering strategy improves the overall performance and operational stability of the OPDs, especially under ultraviolet exposure.
{"title":"Mitigation of Illumination Sensitive Dark Current in Broadband Organic Photodiode Enabled by Robust Interface Engineering","authors":"Alvin Joseph, Anitha B. Pillai, Muthukrishnan Sundaram, Birabar Ranjit Kumar Nanda, Manoj A. G. Namboothiry","doi":"10.1002/aenm.202500748","DOIUrl":"https://doi.org/10.1002/aenm.202500748","url":null,"abstract":"The reliability of performance metrics in organic photodiodes (OPDs) is a fundamental factor for their efficacy in real‐time applications. Among these metrics, the dark current density stands out for its direct impact on the sensitivity of the detectors. In this study, an anomalous illumination‐sensitive variation in dark current is observed in fabricated near‐infrared OPDs, which undermines the device reliability. The systematic investigation reveals that this behavior stems from the photocatalytic nature of zinc oxide (ZnO), the electron transport layer used in the OPD. The photocatalytic nature of ZnO detrimentally affects the stability of the active material, particularly the nonfullerene acceptor employed in this study. Through robust interface engineering approach, which involves modifying the interface between ZnO and the active layer, the anomalies in the dark current are successfully mitigated, enhancing the consistency and reliability of the OPDs. In addition to reducing the dark current, this interface engineering strategy improves the overall performance and operational stability of the OPDs, especially under ultraviolet exposure.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"68 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866657","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-24DOI: 10.1038/s41524-025-01572-y
Jenna A. Bilbrey, Jesun S. Firoz, Mal-Soon Lee, Sutanay Choudhury
For neural network potentials (NNPs) to gain widespread use, researchers must be able to trust model outputs. However, the blackbox nature of neural networks and their inherent stochasticity are often deterrents, especially for foundation models trained over broad swaths of chemical space. Uncertainty information provided at the time of prediction can help reduce aversion to NNPs. In this work, we detail two uncertainty quantification (UQ) methods. Readout ensembling, by finetuning the readout layers of an ensemble of foundation models, provides information about model uncertainty, while quantile regression, by replacing point predictions with distributional predictions, provides information about uncertainty within the underlying training data. We demonstrate our approach with the MACE-MP-0 model, applying UQ to the foundation model and a series of finetuned models. The uncertainties produced by the readout ensemble and quantile methods are demonstrated to be distinct measures by which the quality of the NNP output can be judged.
{"title":"Uncertainty quantification for neural network potential foundation models","authors":"Jenna A. Bilbrey, Jesun S. Firoz, Mal-Soon Lee, Sutanay Choudhury","doi":"10.1038/s41524-025-01572-y","DOIUrl":"https://doi.org/10.1038/s41524-025-01572-y","url":null,"abstract":"<p>For neural network potentials (NNPs) to gain widespread use, researchers must be able to trust model outputs. However, the blackbox nature of neural networks and their inherent stochasticity are often deterrents, especially for foundation models trained over broad swaths of chemical space. Uncertainty information provided at the time of prediction can help reduce aversion to NNPs. In this work, we detail two uncertainty quantification (UQ) methods. Readout ensembling, by finetuning the readout layers of an ensemble of foundation models, provides information about model uncertainty, while quantile regression, by replacing point predictions with distributional predictions, provides information about uncertainty within the underlying training data. We demonstrate our approach with the MACE-MP-0 model, applying UQ to the foundation model and a series of finetuned models. The uncertainties produced by the readout ensemble and quantile methods are demonstrated to be distinct measures by which the quality of the NNP output can be judged.</p>","PeriodicalId":19342,"journal":{"name":"npj Computational Materials","volume":"69 1","pages":""},"PeriodicalIF":9.7,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866932","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yajing Miao, Anatoli Kurkin, Pengfei Wang, Lin Ye, Xin Zhang
The demand for lightweight and high-performance multifunctional composite materials is becoming increasingly widespread nowadays. This study investigates the impact-resistance and force-sensing capabilities of polyborosiloxane (PBS) integrated within carbon fiber. Two types of PBS are synthesized with different crosslinking densities, focusing on their rheological and mechanical properties under various strain rates and impact conditions. The results show that peak force is highly correlated with impact energy, rather than velocity, when PBS is in its rubbery state. Interestingly, with the dynamic compression of a high strain rate, PBS produces a yielding stage and then a strengthening stage. Compared to traditional epoxy/carbon laminates, PBS65/Carbon composites exhibited superior impact energy absorption, withstanding up to seven repeated impacts due to the brittle cracking of PBS and its stiffening transition and the self-healing function. Moreover, the addition of carbon nanotubes to the PBS matrix enabled the development of a force-sensing composite, which can detect and measure impact forces. The PBS/Carbon laminates also exhibited enhanced flexibility, making them suitable for advanced protective applications requiring repeated impact-resistance and real-time force monitoring.
{"title":"Flexible Carbon Fiber Composite with Enhanced Durable Impact-Resistance and Sensing Capability Based on Polyborosiloxane Network","authors":"Yajing Miao, Anatoli Kurkin, Pengfei Wang, Lin Ye, Xin Zhang","doi":"10.1002/adfm.202503952","DOIUrl":"https://doi.org/10.1002/adfm.202503952","url":null,"abstract":"The demand for lightweight and high-performance multifunctional composite materials is becoming increasingly widespread nowadays. This study investigates the impact-resistance and force-sensing capabilities of polyborosiloxane (PBS) integrated within carbon fiber. Two types of PBS are synthesized with different crosslinking densities, focusing on their rheological and mechanical properties under various strain rates and impact conditions. The results show that peak force is highly correlated with impact energy, rather than velocity, when PBS is in its rubbery state. Interestingly, with the dynamic compression of a high strain rate, PBS produces a yielding stage and then a strengthening stage. Compared to traditional epoxy/carbon laminates, PBS65/Carbon composites exhibited superior impact energy absorption, withstanding up to seven repeated impacts due to the brittle cracking of PBS and its stiffening transition and the self-healing function. Moreover, the addition of carbon nanotubes to the PBS matrix enabled the development of a force-sensing composite, which can detect and measure impact forces. The PBS/Carbon laminates also exhibited enhanced flexibility, making them suitable for advanced protective applications requiring repeated impact-resistance and real-time force monitoring.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"14 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143867116","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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