Accounts of materials research最新文献

{"title":"C–H σ-Dopants Mediated n-Doping of Conjugated Polymers: Mutual Designs and Multiscale Characteristics","authors":"Yuan-He Li, Jie-Yu Wang and Jian Pei*, ","doi":"10.1021/accountsmr.4c0013410.1021/accountsmr.4c00134","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00134https://doi.org/10.1021/accountsmr.4c00134","url":null,"abstract":"<p >Conjugated polymers have gained significant interest in recent decades, offering complementary advantages over traditional inorganic electronic materials in ways such as solution processability, mechanical flexibility, and structural diversity afforded via bottom-up organic synthesis. Doping is a crucial aspect for advancing these materials as it adjusts the energies, spatial distributions, and occupancies of the orbitals, affecting the carrier density and mobility. Compared to their p-doping counterparts, n-doping strategies lag behind in their performances. The combination of p-type and n-type polymers is essential for many organic optoelectronic applications, which signified the importance of developing novel n-doping solutions. Traditional electron transfer-type n-dopants, which rely on a low ionization potential for their reactivity, face challenges in processability, reversibility, and sensitivity to ambient conditions. In contrast, C–H σ-dopants operate through different mechanisms. This could open up new avenues to reconcile these conflicts.</p><p >In this Account, we present our recent efforts to establish a multiscale model for understanding the determinants of n-doping conjugated polymers with C–H σ-dopants. Central to the doping process are the molecular structures of the dopant and the polymer repeating unit, as their interactions dictate reaction kinetics and lay the foundation for the electronic structures of the doped polymers. Backbone conformation is pivotal for orbital delocalization and π–π stacking, affecting the intrachain charge transport process and interactions between polymer backbones. Beyond single-molecule behaviors, achieving ordered polymer–polymer stacking structures is crucial for enhanced electrical performance. This requirement coexists with the need for solubility and efficient doping, influenced by polymer-dopant or polymer–solvent interactions. Fine-tuning these interactions involves considerations of the polymer conformation, side-chain structure, dopant design, and solvent selection. Induced disorders in the side-chain packing region can accommodate the orderly arrangement of polymer backbones, while tolerating dopant molecules, preventing phase segregation, and reducing the tendency for the cationic dopant byproducts to interact with the oppositely charged polymer backbones. We also demonstrated that polarized side chains could minimize transport barriers caused by electrostatic interactions and reduce the impact of dopant cations on backbone packing. Finally, we explored the effects of polymer microstructures including phase segregation and crystallization behaviors. The practical importance of considering these multifaceted factors is illustrated through the construction of some of the best-performing flexible thermoelectric generators. From theories and molecular designs to characterizations and applications, this Account provides a comprehensive framework for further exploration in the field of n-d","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"5 9","pages":"1059–1071 1059–1071"},"PeriodicalIF":14.0,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325958","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}

{"title":"C–H σ-Dopants Mediated n-Doping of Conjugated Polymers: Mutual Designs and Multiscale Characteristics","authors":"Yuan-He Li, Jie-Yu Wang, Jian Pei","doi":"10.1021/accountsmr.4c00134","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00134","url":null,"abstract":"Conjugated polymers have gained significant interest in recent decades, offering complementary advantages over traditional inorganic electronic materials in ways such as solution processability, mechanical flexibility, and structural diversity afforded via bottom-up organic synthesis. Doping is a crucial aspect for advancing these materials as it adjusts the energies, spatial distributions, and occupancies of the orbitals, affecting the carrier density and mobility. Compared to their p-doping counterparts, n-doping strategies lag behind in their performances. The combination of p-type and n-type polymers is essential for many organic optoelectronic applications, which signified the importance of developing novel n-doping solutions. Traditional electron transfer-type n-dopants, which rely on a low ionization potential for their reactivity, face challenges in processability, reversibility, and sensitivity to ambient conditions. In contrast, C–H σ-dopants operate through different mechanisms. This could open up new avenues to reconcile these conflicts.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"39 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141877769","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}

{"title":"Light-Controlled Macrocyclic Supramolecular Assemblies and Luminescent Behaviors","authors":"Shuangqi Song, Hengzhi Zhang, Yu Liu","doi":"10.1021/accountsmr.4c00157","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00157","url":null,"abstract":"Intelligent supramolecular assemblies can respond well to external stimuli such as pH, temperature, light, electricity, magnetism, and enzymes to achieve not only reversible topological morphology changes and assembly/disassembly processes but also special physical and chemical properties, which are successfully applied to biological imaging, cancer treatment, luminescent materials, anticounterfeiting, sensing, molecular switch in chemical, materials, as well as biological research fields. Among all stimuli-responsive supramolecular assemblies, light-controlled supramolecular assemblies have always attracted intense attention because light is a kind of clean and eco-friendly energy. In this Account, we focus on light-controlled supramolecular assemblies formed by four types of photoresponsive molecules and macrocyclic hosts such as cucurbit[n]urils, cyclodextrins, and crown ethers, and their regulations in luminescent materials and bioimaging. The assemblies and cascade assemblies between photoisomerization or photoreaction molecules and macrocyclic hosts mainly include: 1) light-controlled supramolecular assemblies based on macrocycles and diarylethene. As molecular switches, the open-ring and closed-ring configurations of diarylethenes can be reversibly controlled to achieve tunable fluorescence resonance energy transfer (<b>FRET</b>) process and further regulate luminescent behaviors to construct intelligent response cell-imaging, anticounterfeiting, and multicolor luminescence systems. 2) Light-controlled supramolecular assemblies based on macrocycles and spiropyran. Different from the diarylethenes, spiropyran can converse between positive charges in the ring-open merocyanie (<b>MC</b>) state, which is amphiphilic and easy to bond with macrocycles like cucurbit[n]urils, and neutral/negative charges in the ring-closed spiropyran (<b>SP</b>) state, which is more likely to self-assemble. Therefore, the differentiation of bonding affinities with macrocycles between <b>MC</b> and <b>SP</b> can achieve light-driven molecular machines. 3) Light-controlled supramolecular assemblies between macrocycles and azobenzene, whether azobenzene is modified to the macrocyclic hosts or functional guests, supramolecular assemblies are formed through host–guest interactions, and the topological morphology and luminescence behavior of the assemblies can be regulated by photoisomerization to apply in catalytic activity modulation, induction of microtubule (<b>MT</b>) assembly/disassembly, drug delivery, and others. 4) Light-controlled supramolecular assemblies based on macrocycles and anthracene, in which different bonding affinities between anthracene before and after photooxidation and macrocyclic hosts, as well as reversible dimerization, not only change the topological morphologies but also drive fluorescence phosphorescence dual imaging and the construction of photostimuli-driven luminescent lanthanide molecular switch. With the creation of macrocycles with n","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"181 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141877771","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}

{"title":"Light-Controlled Macrocyclic Supramolecular Assemblies and Luminescent Behaviors","authors":"Shuangqi Song, Hengzhi Zhang and Yu Liu*, ","doi":"10.1021/accountsmr.4c0015710.1021/accountsmr.4c00157","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00157https://doi.org/10.1021/accountsmr.4c00157","url":null,"abstract":"<p >Intelligent supramolecular assemblies can respond well to external stimuli such as pH, temperature, light, electricity, magnetism, and enzymes to achieve not only reversible topological morphology changes and assembly/disassembly processes but also special physical and chemical properties, which are successfully applied to biological imaging, cancer treatment, luminescent materials, anticounterfeiting, sensing, molecular switch in chemical, materials, as well as biological research fields. Among all stimuli-responsive supramolecular assemblies, light-controlled supramolecular assemblies have always attracted intense attention because light is a kind of clean and eco-friendly energy. In this Account, we focus on light-controlled supramolecular assemblies formed by four types of photoresponsive molecules and macrocyclic hosts such as cucurbit[n]urils, cyclodextrins, and crown ethers, and their regulations in luminescent materials and bioimaging. The assemblies and cascade assemblies between photoisomerization or photoreaction molecules and macrocyclic hosts mainly include: 1) light-controlled supramolecular assemblies based on macrocycles and diarylethene. As molecular switches, the open-ring and closed-ring configurations of diarylethenes can be reversibly controlled to achieve tunable fluorescence resonance energy transfer (<b>FRET</b>) process and further regulate luminescent behaviors to construct intelligent response cell-imaging, anticounterfeiting, and multicolor luminescence systems. 2) Light-controlled supramolecular assemblies based on macrocycles and spiropyran. Different from the diarylethenes, spiropyran can converse between positive charges in the ring-open merocyanie (<b>MC</b>) state, which is amphiphilic and easy to bond with macrocycles like cucurbit[n]urils, and neutral/negative charges in the ring-closed spiropyran (<b>SP</b>) state, which is more likely to self-assemble. Therefore, the differentiation of bonding affinities with macrocycles between <b>MC</b> and <b>SP</b> can achieve light-driven molecular machines. 3) Light-controlled supramolecular assemblies between macrocycles and azobenzene, whether azobenzene is modified to the macrocyclic hosts or functional guests, supramolecular assemblies are formed through host–guest interactions, and the topological morphology and luminescence behavior of the assemblies can be regulated by photoisomerization to apply in catalytic activity modulation, induction of microtubule (<b>MT</b>) assembly/disassembly, drug delivery, and others. 4) Light-controlled supramolecular assemblies based on macrocycles and anthracene, in which different bonding affinities between anthracene before and after photooxidation and macrocyclic hosts, as well as reversible dimerization, not only change the topological morphologies but also drive fluorescence phosphorescence dual imaging and the construction of photostimuli-driven luminescent lanthanide molecular switch. With the creation of macrocycles wi","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"5 9","pages":"1109–1120 1109–1120"},"PeriodicalIF":14.0,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325959","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}

{"title":"Low-Energy Dissipation Diamond MEMS","authors":"Guo Chen, Satoshi Koizumi, Yasuo Koide, Meiyong Liao","doi":"10.1021/accountsmr.4c00139","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00139","url":null,"abstract":"Microelectromechanical systems (MEMS) that integrate tiny mechanical devices with electronics on a semiconductor substate have experienced explosive growth over the past decades. MEMS have a range of wide applications from accelerometers and gyroscopes in automotive safety, to precise reference oscillators in consumer electrons to probes in atomic force microscopy and sensors for gravitational wave detection. The quality (<i>Q</i>)-factor is a fundamental parameter of a MEMS resonator that determines the sensitivity, noise level, energy efficiency, and stability of the device. MEMS with low energy dissipation have always been pursued. Despite the brilliant progress of silicon-based MEMS due to the mature technology in counterpart microelectronics, the intrinsic material properties limit the sensitivity and reliability, especially for the applications under extreme conditions. Diamond has emerged as the ideal semiconductor material for low-energy dissipation MEMS with high performance and high reliability, owing to its unparalleled material properties, such as extremely high mechanical strength, superelectrical properties, highest thermal conductivity, and chemical inertness. Diamond resonators are thus expected to exhibit high <i>Q</i>-factors, and high reliability, with low thermomechanical force noise and long coherence rate of mechanical quantum states, not only improving the performance of MEMS devices but also expanding to the quantum domain. Single-crystal diamond (SCD) is desirable to achieve the ultralow energy loss or high <i>Q</i>-factor MEMS resonator due to the nonexistence of grain boundaries and other carbon phases. However, micromachining for SCD is tough and heteroepitaxial growth of SCD on foreign substrates remains quite difficult.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"74 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141857996","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}

{"title":"Low-Energy Dissipation Diamond MEMS","authors":"Guo Chen,&nbsp;Satoshi Koizumi,&nbsp;Yasuo Koide and Meiyong Liao*,&nbsp;","doi":"10.1021/accountsmr.4c0013910.1021/accountsmr.4c00139","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00139https://doi.org/10.1021/accountsmr.4c00139","url":null,"abstract":"&lt;p &gt;Microelectromechanical systems (MEMS) that integrate tiny mechanical devices with electronics on a semiconductor substate have experienced explosive growth over the past decades. MEMS have a range of wide applications from accelerometers and gyroscopes in automotive safety, to precise reference oscillators in consumer electrons to probes in atomic force microscopy and sensors for gravitational wave detection. The quality (&lt;i&gt;Q&lt;/i&gt;)-factor is a fundamental parameter of a MEMS resonator that determines the sensitivity, noise level, energy efficiency, and stability of the device. MEMS with low energy dissipation have always been pursued. Despite the brilliant progress of silicon-based MEMS due to the mature technology in counterpart microelectronics, the intrinsic material properties limit the sensitivity and reliability, especially for the applications under extreme conditions. Diamond has emerged as the ideal semiconductor material for low-energy dissipation MEMS with high performance and high reliability, owing to its unparalleled material properties, such as extremely high mechanical strength, superelectrical properties, highest thermal conductivity, and chemical inertness. Diamond resonators are thus expected to exhibit high &lt;i&gt;Q&lt;/i&gt;-factors, and high reliability, with low thermomechanical force noise and long coherence rate of mechanical quantum states, not only improving the performance of MEMS devices but also expanding to the quantum domain. Single-crystal diamond (SCD) is desirable to achieve the ultralow energy loss or high &lt;i&gt;Q&lt;/i&gt;-factor MEMS resonator due to the nonexistence of grain boundaries and other carbon phases. However, micromachining for SCD is tough and heteroepitaxial growth of SCD on foreign substrates remains quite difficult.&lt;/p&gt;&lt;p &gt;In this Account, we provide an overview of the recent research and strategies in SCD diamond MEMS for achieving high &lt;i&gt;Q&lt;/i&gt;-factors, focusing on those fabricated by the smart-cut method developed in our lab. We start with the concept of diamond MEMS, covering structure fabrication, fundamentals, and applications. A comprehensive discussion of the energy dissipation mechanisms on the &lt;i&gt;Q&lt;/i&gt;-factors in diamond MEMS resonators is provided. The approaches to enhance the &lt;i&gt;Q&lt;/i&gt;-factor of diamond resonators including (1) the growth of high crystal quality SCD epilayer on the ion-implanted substrate, (2) defects engineering, and (3) strain engineering by thinning the resonator to around 100 nm thick are presented. In the smart-cut method, the ∼100 nm thick defective layer contributes to the main intrinsic energy loss. By combing the growth of a high crystal quality diamond epilayer above the defective layer and the atomic scale etching of the defective layer, the &lt;i&gt;Q&lt;/i&gt;-factors could be improved from thousands to over one million at room temperature, the highest among all the semiconductors. The intrinsic high &lt;i&gt;Q&lt;/i&gt;-factors of SCD MEMS are also due to the well-controlled purity of the d","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"5 9","pages":"1087–1096 1087–1096"},"PeriodicalIF":14.0,"publicationDate":"2024-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142326314","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}

{"title":"Vascularization and Innervation for Bone Tissue Engineering","authors":"Shuo Chen, Xiaojun Zhou, Tao Li, Chuanglong He","doi":"10.1021/accountsmr.4c00165","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00165","url":null,"abstract":"In the rapidly evolving landscape of regenerative medicine, the field of bone tissue engineering stands as a beacon of innovative progress, pushing the boundaries of what is achievable in the realm of medical science. A pivotal leap forward in this domain involves the integration of vascularization and innervation into engineered bone tissues, propelling the field toward the realization of biomimetic and functionally superior bone constructs. In recent years, considerable significant progress has been made on this promising topic. Vascularization has been considered an essential strategy for bone regeneration. Meanwhile, innervation has emerged as a novel developmental trend in vascularized tissue engineered bone for the field of bone tissue engineering. The integration of vascularization and innervation in bone tissue engineering goes beyond merely replicating the structural aspects of native bone. It opens new possibilities for creating biohybrid constructs that not only restore bone function but also actively participate in the dynamic interplay of the musculoskeletal system. The vascularized and innervated scaffolds could potentially accelerate healing processes, respond to mechanical stimuli, and exhibit enhanced biological compatibility with the host organism, making them highly desirable for researchers in this field. The concept of vascularized and innervated biomaterials is fundamental and important. It is expected to be extensive future work based on this Account in generalizing the work to other regenerative medicines. Thus, to elucidate the effect and mechanism of vascularization and innervation of tissue engineered bone not only has important theoretical significance but also provides a new idea for the design of bone repair materials. In this Account, we present recent progress of our group on vascularized and innervated scaffolds for bone tissue engineering, including the designing principle, preparation method, and involved biological mechanism. First, we provide a brief introduction of basic concept and importance for vascularization and innervation. Then, we summarize the design principle for scaffolds favorable for vascularization and innervation in bone tissue engineering by focusing on several aspects including material types, microstructure construction, and drug delivery. Subsequently, the biological strategies for promoting vascularization and innervation are classified with the introduction of the underlying mechanism. Furthermore, we developed novel evaluation strategy of osteogenesis based on in vivo imaging, which provides a new idea for continuous monitoring of osteogenic in vivo. Finally, we conclude by offering our perspective on open challenges and future development trends of this rapidly evolving field. This Account highlighting the vascularized and innervated scaffolds not only provides interesting insights into strategies for bone regeneration but also provides a new perspective for design and processing of bio","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"30 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141754512","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}

{"title":"Vascularization and Innervation for Bone Tissue Engineering","authors":"Shuo Chen,&nbsp;Xiaojun Zhou,&nbsp;Tao Li and Chuanglong He*,&nbsp;","doi":"10.1021/accountsmr.4c0016510.1021/accountsmr.4c00165","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00165https://doi.org/10.1021/accountsmr.4c00165","url":null,"abstract":"&lt;p &gt;In the rapidly evolving landscape of regenerative medicine, the field of bone tissue engineering stands as a beacon of innovative progress, pushing the boundaries of what is achievable in the realm of medical science. A pivotal leap forward in this domain involves the integration of vascularization and innervation into engineered bone tissues, propelling the field toward the realization of biomimetic and functionally superior bone constructs. In recent years, considerable significant progress has been made on this promising topic. Vascularization has been considered an essential strategy for bone regeneration. Meanwhile, innervation has emerged as a novel developmental trend in vascularized tissue engineered bone for the field of bone tissue engineering. The integration of vascularization and innervation in bone tissue engineering goes beyond merely replicating the structural aspects of native bone. It opens new possibilities for creating biohybrid constructs that not only restore bone function but also actively participate in the dynamic interplay of the musculoskeletal system. The vascularized and innervated scaffolds could potentially accelerate healing processes, respond to mechanical stimuli, and exhibit enhanced biological compatibility with the host organism, making them highly desirable for researchers in this field. The concept of vascularized and innervated biomaterials is fundamental and important. It is expected to be extensive future work based on this Account in generalizing the work to other regenerative medicines. Thus, to elucidate the effect and mechanism of vascularization and innervation of tissue engineered bone not only has important theoretical significance but also provides a new idea for the design of bone repair materials. In this Account, we present recent progress of our group on vascularized and innervated scaffolds for bone tissue engineering, including the designing principle, preparation method, and involved biological mechanism. First, we provide a brief introduction of basic concept and importance for vascularization and innervation. Then, we summarize the design principle for scaffolds favorable for vascularization and innervation in bone tissue engineering by focusing on several aspects including material types, microstructure construction, and drug delivery. Subsequently, the biological strategies for promoting vascularization and innervation are classified with the introduction of the underlying mechanism. Furthermore, we developed novel evaluation strategy of osteogenesis based on in vivo imaging, which provides a new idea for continuous monitoring of osteogenic in vivo. Finally, we conclude by offering our perspective on open challenges and future development trends of this rapidly evolving field. This Account highlighting the vascularized and innervated scaffolds not only provides interesting insights into strategies for bone regeneration but also provides a new perspective for design and processing of","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"5 9","pages":"1121–1133 1121–1133"},"PeriodicalIF":14.0,"publicationDate":"2024-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142326313","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}

{"title":"Two-Dimensional and Interface Superconductivity in Crystalline Systems","authors":"Haoran Ji, Yi Liu, Chengcheng Ji, Jian Wang","doi":"10.1021/accountsmr.4c00017","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00017","url":null,"abstract":"The investigations of crystalline two-dimensional (2D) superconducting systems have become a frontier of condensed matter physics and materials science due to the emergence of novel quantum phenomena. With the reduced dimensionality, the fluctuations, the disorder effect, and the intricate interactions between electrons, spins, and orbits may impose dramatic effects on the quantum behavior of 2D superconductors. This Account reviews the recent research progress in 2D crystalline superconducting films and interfacial superconducting systems, focusing on the quantum phase transitions, emergent quantum states, and unconventional superconductivity. Six topics are introduced, including quantum Griffiths singularity, anomalous metallic state, rotational-symmetry-broken superconducting state, Ising superconductivity, interfacial high-transition temperature superconductivity, and interface-induced superconductivity. As a paradigm of quantum phase transition in 2D superconductors, the superconductor–insulator/metal transition (SIT/SMT) has been intensively studied over the last three decades, which highlights the prominent effect of disorder and quantum fluctuations. The quantum Griffiths singularity (QGS) and the anomalous metallic state revealed recently go beyond the framework of the SIT/SMT at the zero-temperature limit. The QGS of SMT was first discovered in trilayer Ga films and subsequently confirmed in various 2D superconductors. The main characteristic of QGS is a divergent critical exponent, in stark contrast to a fixed critical exponent of the conventional SIT/SMT. The anomalous metallic state, characterized by a saturating resistance at ultralow temperatures, is detected as an intervening metallic ground state that disrupts the SIT/SMT. The charge-2&lt;i&gt;e&lt;/i&gt; quantum oscillations and the absence of the Hall effect indicate that the anomalous metallic states are dominated by the bosonic Cooper pairs instead of fermionic quasiparticles. Furthermore, the 2D systems could host various kinds of interactions and ordered states, which may be intertwined with the superconductivity. Originating from the interplay between multiple orders and strong electronic correlations, the rotational symmetry breakings are observed as in the infinite-layer nickelate superconductors, revealing the unconventional superconductivity. Arisen from the strong Zeeman-type spin–orbit coupling, the Ising superconductivity is discovered in diverse 2D superconducting systems, which features a large in-plane critical magnetic field exceeding the Pauli limit. Through interface engineering or heterostructure fabrication, the superconductivity, even high transition temperature (high-&lt;i&gt;T&lt;/i&gt;&lt;sub&gt;c&lt;/sub&gt;) superconductivity, could be achieved at the interfaces between different materials. Moreover, the interface effect and the nontrivial topology could be introduced through interface engineering or heterostructure fabrication incorporating superconductors, insulators, semiconductors, n","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"31 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141783090","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}

{"title":"Supramolecular-Based One-Pot Separation of Highly Pure Adsorbent-Free Semiconducting Single-Walled Carbon Nanotubes and Machine Learning-Based Nanotube Solubilization","authors":"Naotoshi Nakashima, Yoshiyuki Nonoguchi, Aleksandar Staykov","doi":"10.1021/accountsmr.4c00113","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00113","url":null,"abstract":"Carbon nanotubes are classified into single-walled carbon nanotubes (SWNTs), double-walled carbon nanotubes and multiwalled carbon nanotubes. Among these, SWNTs have remarkable electronic, mechanical, optical, chemical and thermal properties, which are derived from their one-dimensional extended π-conjugated structures, and thus, they demonstrate a high potential toward the development of the next-generation nanoelectronics, (nano)bio, and energy and environmental materials and devices. As-produced SWNTs are a mixture of semiconducting (sem-) and metallic (met-)-SWNTs; thus, chirality sorting is highly important. So far various methods have been presented for such a separation including (i) use of chemical adsorbents such as polyfluorenes (PFOs) and their analogues and (ii) physical methods including surfactant-aided density gradient ultracentrifugation (DGU), gel chromatography techniques, and the surfactant-aided aqueous two-phase extraction method. However, such methods are not simple, and the removal of the wrapped adsorbents on the SWNTs is very difficult. Thus, the development of a method to remove the adsorbent from the sorted SWNTs is highly important to obtain adsorbent-free pure sem-SWNTs.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"334 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141732744","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}