{"title":"","authors":"Wen Xie, Qian Wu and Zhichuan J. Xu*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 6","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":14.0,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/accountsmr.5c00092","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144489194","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}
Hengrui Zhang, Alexandru B. Georgescu, Suraj Yerramilli, Christopher Karpovich, Daniel W. Apley, Elsa A. Olivetti, James M. Rondinelli* and Wei Chen*,
{"title":"","authors":"Hengrui Zhang, Alexandru B. Georgescu, Suraj Yerramilli, Christopher Karpovich, Daniel W. Apley, Elsa A. Olivetti, James M. Rondinelli* and Wei Chen*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 6","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":14.0,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/accountsmr.5c00011","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144489193","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 : 2025-06-07DOI: 10.1021/accountsmr.5c00113
Yang Cao*, Nobukiyo Kobayashi, Hanae Kijima-Aoki, Jun Zhang and Hiroshi Masumoto*,
<p >Magnetic granular nanocomposites, consisting of magnetic nanogranules dispersed within a host matrix, represent a versatile class of functional materials that enable control over electrical, magnetic, and thermal properties at the nanoscale. Over the past decade, by leveraging electrons as carriers of spin, charge, and heat, these features have enabled the discovery of a family of tunnel related phenomena: tunnel magnetoresistance (TMR), tunnel magneto-Seebeck (TMS), tunnel magnetodielectric (TMD), and most recently tunnel magneto-optical (TMO) effects. Their structural features allow for tuning of granular size, distribution, and intergranular spacing, positioning these materials as promising candidates for miniaturized magnetic field sensors, antennas, microwave devices, and spintronic components.</p><p >In this Account, we summarize our recent advances in understanding TMD effects in complex granular nanocomposites over the past decade. We begin by illustrating how key structural parameters, including intergranular spacing, granule distribution, and magnetic granule composition, govern dielectric variations. From a theoretical standpoint, we derive a formula that predicts the maximum achievable dielectric change. Experimentally, we show that introducing small amounts of ferromagnetic species to balance the ferromagnetic and superparamagnetic components in a nanogranular composite greatly enhances low-field sensitivity. Moreover, by integrating silicon into the films to improve interfaces, the TMD response (i.e., the maximum dielectric variation) reaches a record 8.5% under a 10 kOe magnetic field. We also investigate the heterostructures, such as gradient and multilayer architectures, which effectively broaden the TMD frequency range. Based on the established mechanism of spin-dependent charge oscillations, we demonstrate that optical transmittance in these nanocomposites can be regulated via an external magnetic field (the TMO effect). Transparent FeCo–AlF<sub>3</sub> films exhibit magneto-tunable transmittance across the visible-NIR range, while fluoride- and nitride-based nanogranular films yield giant Faraday rotations, which is more than 40 times greater than that of Bisubstituted yttrium iron garnet. Additionally, we have introduced our recent discovery in granular nanocomposites, including giant Faraday rotation as well as electrically tunable dielectric properties. We demonstrate electric-field control of dielectric relaxation in Co–MgF<sub>2</sub>, enabling MHz-range tunable capacitors driven by a DC bias.</p><p >Finally, we outline the key challenges and future directions in TMD research. Further progress will rely on continued exploration of novel material combinations, including the design of compositionally graded multilayers and heterostructures that couple TMD-active layers with magnonic or photonic elements. Integrating nanogranular films into CMOS-compatible platforms and silicon photonic circuits may open pathways toward
{"title":"Multifunctional Spin-Dependent Tunneling: From Tunnel Magnetodielectric to Magneto-Optic and Faraday Effects","authors":"Yang Cao*, Nobukiyo Kobayashi, Hanae Kijima-Aoki, Jun Zhang and Hiroshi Masumoto*, ","doi":"10.1021/accountsmr.5c00113","DOIUrl":"10.1021/accountsmr.5c00113","url":null,"abstract":"<p >Magnetic granular nanocomposites, consisting of magnetic nanogranules dispersed within a host matrix, represent a versatile class of functional materials that enable control over electrical, magnetic, and thermal properties at the nanoscale. Over the past decade, by leveraging electrons as carriers of spin, charge, and heat, these features have enabled the discovery of a family of tunnel related phenomena: tunnel magnetoresistance (TMR), tunnel magneto-Seebeck (TMS), tunnel magnetodielectric (TMD), and most recently tunnel magneto-optical (TMO) effects. Their structural features allow for tuning of granular size, distribution, and intergranular spacing, positioning these materials as promising candidates for miniaturized magnetic field sensors, antennas, microwave devices, and spintronic components.</p><p >In this Account, we summarize our recent advances in understanding TMD effects in complex granular nanocomposites over the past decade. We begin by illustrating how key structural parameters, including intergranular spacing, granule distribution, and magnetic granule composition, govern dielectric variations. From a theoretical standpoint, we derive a formula that predicts the maximum achievable dielectric change. Experimentally, we show that introducing small amounts of ferromagnetic species to balance the ferromagnetic and superparamagnetic components in a nanogranular composite greatly enhances low-field sensitivity. Moreover, by integrating silicon into the films to improve interfaces, the TMD response (i.e., the maximum dielectric variation) reaches a record 8.5% under a 10 kOe magnetic field. We also investigate the heterostructures, such as gradient and multilayer architectures, which effectively broaden the TMD frequency range. Based on the established mechanism of spin-dependent charge oscillations, we demonstrate that optical transmittance in these nanocomposites can be regulated via an external magnetic field (the TMO effect). Transparent FeCo–AlF<sub>3</sub> films exhibit magneto-tunable transmittance across the visible-NIR range, while fluoride- and nitride-based nanogranular films yield giant Faraday rotations, which is more than 40 times greater than that of Bisubstituted yttrium iron garnet. Additionally, we have introduced our recent discovery in granular nanocomposites, including giant Faraday rotation as well as electrically tunable dielectric properties. We demonstrate electric-field control of dielectric relaxation in Co–MgF<sub>2</sub>, enabling MHz-range tunable capacitors driven by a DC bias.</p><p >Finally, we outline the key challenges and future directions in TMD research. Further progress will rely on continued exploration of novel material combinations, including the design of compositionally graded multilayers and heterostructures that couple TMD-active layers with magnonic or photonic elements. Integrating nanogranular films into CMOS-compatible platforms and silicon photonic circuits may open pathways toward ","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 8","pages":"979–990"},"PeriodicalIF":14.7,"publicationDate":"2025-06-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144237478","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
<p >With the rapid advancement of energy storage technologies, lithium-ion batteries (LIBs) based on graphite anodes and liquid organic electrolytes have achieved remarkable progress. Nevertheless, the limited specific capacity of graphite anodes and the safety concerns associated with organic electrolytes hinder further enhancement of LIBs. In pursuit of higher energy density and improved safety, solid-state Li metal batteries (SSLMBs) have drawn significant attention. Furthermore, anode-free solid-state batteries (AFSSBs), as a particularly promising innovation in the field of energy storage, have gained increasing interest in recent years. With increasing research investment and continuous technological optimization, AFSSBs hold great potential for widespread applications including electric vehicles, grid energy storage, and beyond.</p><p >Central to AFSSBs, solid-state electrolytes (SSEs) are crucial for achieving high energy density and performance. Among the various SSEs, garnet-type oxide SSEs stand out as one of the most promising systems due to their favorable thermodynamic stability with Li metal anodes, excellent ionic conductivity (∼10<sup>–3</sup> S cm<sup>–1</sup>), and wide electrochemical window (>6 V). However, poor solid–solid interface contact and the growth of Li dendrite have led to sluggish interfacial ion and electron transfer kinetics, thereby impeding the commercialization of garnet-based AFSSBs. Although previous reviews have highlighted interfacial challenges and summarized corresponding mitigation strategies, specific case studies remain scarce and a comprehensive understanding of interfacial dynamics in garnet-based AFSSBs has not yet been established.</p><p >In this Account, we critically evaluate the unique advantages of garnet-based AFSSBs, including their enhanced energy density and improved safety, compared to conventional battery technologies. Additionally, we summarize current understanding primarily from the perspective of interfacial dynamics, covering Li nucleation and growth mechanisms, interfacial evolution at the garnet/current collector interface during Li deposition, and dendrite growth behaviors, aiming to provide deeper insights into interfacial dynamics. Building upon this, we summarize the major interfacial challenges in garnet-based AFSSBs that significantly hinder the interfacial ion and electron transport. In order to enhance the interfacial charge transfer kinetics, we discuss critical parameters, including the properties of the garnet electrolyte and current collector as well as the interfacial wettability at the Li/garnet and Li/current collector interface. Furthermore, we present an overview of our innovative strategy designed to improve interfacial contact and Li-ion transport between the garnet electrolyte and current collector. Finally, we summarize the progress and provide an outlook for garnet-based AFSSBs, exploring their future improvements and development directions toward practica
{"title":"Promise and Perspectives of Garnet-Based Anode-Free Solid-State Batteries","authors":"Jiayun Wen, Yiming Dai, Qian Yu, Zhiyuan Ouyang, Wei Luo* and Yunhui Huang*, ","doi":"10.1021/accountsmr.4c00129","DOIUrl":"10.1021/accountsmr.4c00129","url":null,"abstract":"<p >With the rapid advancement of energy storage technologies, lithium-ion batteries (LIBs) based on graphite anodes and liquid organic electrolytes have achieved remarkable progress. Nevertheless, the limited specific capacity of graphite anodes and the safety concerns associated with organic electrolytes hinder further enhancement of LIBs. In pursuit of higher energy density and improved safety, solid-state Li metal batteries (SSLMBs) have drawn significant attention. Furthermore, anode-free solid-state batteries (AFSSBs), as a particularly promising innovation in the field of energy storage, have gained increasing interest in recent years. With increasing research investment and continuous technological optimization, AFSSBs hold great potential for widespread applications including electric vehicles, grid energy storage, and beyond.</p><p >Central to AFSSBs, solid-state electrolytes (SSEs) are crucial for achieving high energy density and performance. Among the various SSEs, garnet-type oxide SSEs stand out as one of the most promising systems due to their favorable thermodynamic stability with Li metal anodes, excellent ionic conductivity (∼10<sup>–3</sup> S cm<sup>–1</sup>), and wide electrochemical window (>6 V). However, poor solid–solid interface contact and the growth of Li dendrite have led to sluggish interfacial ion and electron transfer kinetics, thereby impeding the commercialization of garnet-based AFSSBs. Although previous reviews have highlighted interfacial challenges and summarized corresponding mitigation strategies, specific case studies remain scarce and a comprehensive understanding of interfacial dynamics in garnet-based AFSSBs has not yet been established.</p><p >In this Account, we critically evaluate the unique advantages of garnet-based AFSSBs, including their enhanced energy density and improved safety, compared to conventional battery technologies. Additionally, we summarize current understanding primarily from the perspective of interfacial dynamics, covering Li nucleation and growth mechanisms, interfacial evolution at the garnet/current collector interface during Li deposition, and dendrite growth behaviors, aiming to provide deeper insights into interfacial dynamics. Building upon this, we summarize the major interfacial challenges in garnet-based AFSSBs that significantly hinder the interfacial ion and electron transport. In order to enhance the interfacial charge transfer kinetics, we discuss critical parameters, including the properties of the garnet electrolyte and current collector as well as the interfacial wettability at the Li/garnet and Li/current collector interface. Furthermore, we present an overview of our innovative strategy designed to improve interfacial contact and Li-ion transport between the garnet electrolyte and current collector. Finally, we summarize the progress and provide an outlook for garnet-based AFSSBs, exploring their future improvements and development directions toward practica","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 7","pages":"902–913"},"PeriodicalIF":14.7,"publicationDate":"2025-06-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144237479","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-06-04DOI: 10.1021/accountsmr.5c00076
Haodi Zeng, Chunxia Gao*, Yuanyuan Yu, Mengjin Jiang, Tingyin Deng and Jiadeng Zhu*,
<p >Poly(3,4-ethylenedioxythiophene): poly(styrenesulfonate) (PEDOT:PSS) is a derivative of polythiophene and an intrinsically conductive polymer (CP). Due to its excellent conductivity, processability, and biocompatibility, it has received widespread attention in the past decade and has become a popular material for wearable electronic devices. Thin films and fibers are the two primary dimensions that PEDOT:PSS has been made into. Compared with two-dimensional (2D) thin films, 1D fibers have natural advantages in integration and structural design, remarkably accelerating practical applications.</p><p >Wet spinning has been considered the primary method to fabricate 1D PEDOT:PSS fibers, which can continuously produce fibers on a large scale with the outstanding capability of fine-tuning the compositions and morphologies to achieve the desired properties. For example, untreated wet-spun PEDOT:PSS fibers generally have relatively lower conductivity (0.1 S·cm<sup>–1</sup>), while the coagulation bath obtained by mixing acetone and isopropanol significantly increases the conductivity (310 S·cm<sup>–1</sup>), which has become a classic combination. Nevertheless, the extensive use of such solvents does not meet the requirements of environmental friendliness, and researchers have been searching for suitable alternatives. Even though the coagulation bath composed of ethanol, water, and metal salts compensates for improving that, the performance needs further enhancement, including conductivity, elongation at break, and capacitance. Thus, intensive efforts have been taken to boost the performance of PEDOT:PSS by changing the formula of the coagulation bath, blending other additives with the starting materials, and secondary treatment for the obtained fibers. In addition to ethanol and water, other coagulation baths are also being developed, such as sulfuric acid, N, N-dimethylacetamide, etc., which play a critical role in the above solutions due to the excellent performance of the resultant fibers.</p><p >In this <i>Account</i>, the efforts are mainly concentrated on the advancements and progress in achieving high-performance wet-spun PEDOT:PSS fibers, from coagulation bath regulation to secondary treatment of spinning solution blending. The fundamental electrochemistry and challenges of PEDOT:PSS fibers will also be discussed. It will then focus on the advantages and control mechanisms of preparing PEDOT:PSS fibers through wet spinning from three perspectives: (i) coagulation bath control; (ii) polymer blending; and (iii) post-treatment. For example, we will discuss: 1) how different additives in the coagulation bath regulate the structure and properties of PEDOT:PSS fibers; 2) how polymer blending can improve the stability and durability of PEDOT:PSS fibers; and 3) how post-treatment can endow PEDOT:PSS fibers with unique structures, enhancing their strength and conductivity. Finally, the key research directions required in this field and the remaining
{"title":"Wet Spinning Enabled Advanced PEDOT:PSS Composite Fibers for Smart Devices","authors":"Haodi Zeng, Chunxia Gao*, Yuanyuan Yu, Mengjin Jiang, Tingyin Deng and Jiadeng Zhu*, ","doi":"10.1021/accountsmr.5c00076","DOIUrl":"10.1021/accountsmr.5c00076","url":null,"abstract":"<p >Poly(3,4-ethylenedioxythiophene): poly(styrenesulfonate) (PEDOT:PSS) is a derivative of polythiophene and an intrinsically conductive polymer (CP). Due to its excellent conductivity, processability, and biocompatibility, it has received widespread attention in the past decade and has become a popular material for wearable electronic devices. Thin films and fibers are the two primary dimensions that PEDOT:PSS has been made into. Compared with two-dimensional (2D) thin films, 1D fibers have natural advantages in integration and structural design, remarkably accelerating practical applications.</p><p >Wet spinning has been considered the primary method to fabricate 1D PEDOT:PSS fibers, which can continuously produce fibers on a large scale with the outstanding capability of fine-tuning the compositions and morphologies to achieve the desired properties. For example, untreated wet-spun PEDOT:PSS fibers generally have relatively lower conductivity (0.1 S·cm<sup>–1</sup>), while the coagulation bath obtained by mixing acetone and isopropanol significantly increases the conductivity (310 S·cm<sup>–1</sup>), which has become a classic combination. Nevertheless, the extensive use of such solvents does not meet the requirements of environmental friendliness, and researchers have been searching for suitable alternatives. Even though the coagulation bath composed of ethanol, water, and metal salts compensates for improving that, the performance needs further enhancement, including conductivity, elongation at break, and capacitance. Thus, intensive efforts have been taken to boost the performance of PEDOT:PSS by changing the formula of the coagulation bath, blending other additives with the starting materials, and secondary treatment for the obtained fibers. In addition to ethanol and water, other coagulation baths are also being developed, such as sulfuric acid, N, N-dimethylacetamide, etc., which play a critical role in the above solutions due to the excellent performance of the resultant fibers.</p><p >In this <i>Account</i>, the efforts are mainly concentrated on the advancements and progress in achieving high-performance wet-spun PEDOT:PSS fibers, from coagulation bath regulation to secondary treatment of spinning solution blending. The fundamental electrochemistry and challenges of PEDOT:PSS fibers will also be discussed. It will then focus on the advantages and control mechanisms of preparing PEDOT:PSS fibers through wet spinning from three perspectives: (i) coagulation bath control; (ii) polymer blending; and (iii) post-treatment. For example, we will discuss: 1) how different additives in the coagulation bath regulate the structure and properties of PEDOT:PSS fibers; 2) how polymer blending can improve the stability and durability of PEDOT:PSS fibers; and 3) how post-treatment can endow PEDOT:PSS fibers with unique structures, enhancing their strength and conductivity. Finally, the key research directions required in this field and the remaining ","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 8","pages":"952–963"},"PeriodicalIF":14.7,"publicationDate":"2025-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144237481","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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