publication testing
2025 |
Elahi, Ehsan; Ahsan, Umer; Khan, Muhammad Farooq; Aziz, Jamal; Chauhan, Payal; Michalowski, Pawel Piotr; Chen, Yuan; Eda, Goki; Loula, Martin; Sarkar, Kalyan Jyoti; Sofer, Zdenek Electrical Transport of Nb-Doped MoS2 Homojunction P-N Diode: Investigating NDR and Avalanche Effect Journal Article SMALL, 2025, ISSN: 1613-6810. @article{ISI:001645762300001, title = {Electrical Transport of Nb-Doped MoS2 Homojunction P-N Diode: Investigating NDR and Avalanche Effect}, author = {Ehsan Elahi and Umer Ahsan and Muhammad Farooq Khan and Jamal Aziz and Payal Chauhan and Pawel Piotr Michalowski and Yuan Chen and Goki Eda and Martin Loula and Kalyan Jyoti Sarkar and Zdenek Sofer}, doi = {10.1002/smll.202509043}, times_cited = {0}, issn = {1613-6810}, year = {2025}, date = {2025-12-24}, journal = {SMALL}, publisher = {WILEY-V C H VERLAG GMBH}, address = {POSTFACH 101161, 69451 WEINHEIM, GERMANY}, abstract = {2D transition metal dichalcogenides (TMDCs) are promising candidates for next-generation nanoelectronics and optoelectronics. Yet, controlling layer number, stacking angle, and interfacial quality in van der Waals (vdW) heterostructures remains challenging, often limiting device performance and reproducibility. Homojunctions formed within a single 2D material can circumvent these issues, but their reliable fabrication and systematic exploration of exotic quantum phenomena remain elusive. Here, we report the fabrication and characterization of a thickness-modulated lateral p-n homojunction from a single flake of Nb-doped MoS2. This configuration suppresses interface traps without external interface engineering, enabling excellent and highly stable device performance. The diodes exhibit strong rectifying behavior with a rectification ratio of approximate to 10(4) and a remarkably low ideality factor (eta = 1.23). Notably, we observe field-dependent negative differential resistance (NDR) at low temperatures, offering unique prospects for unconventional electronic applications. The devices also achieve high photoresponsivity (1.09 x 103 A W-1), external quantum efficiency (2.16 x 10(5)%), and detectivity (7.5 x 1010 Jones). Furthermore, electrical breakdown studies reveal avalanche multiplication at relatively low voltages, enabling high-performance avalanche photodetectors. Overall, our results demonstrate a simple yet robust approach for probing carrier multiplication in 2D homojunction p-n diodes, underlining the broad potential of TMDCs in advanced optoelectronic and quantum device applications.}, keywords = {}, pubstate = {published}, tppubtype = {article} } 2D transition metal dichalcogenides (TMDCs) are promising candidates for next-generation nanoelectronics and optoelectronics. Yet, controlling layer number, stacking angle, and interfacial quality in van der Waals (vdW) heterostructures remains challenging, often limiting device performance and reproducibility. Homojunctions formed within a single 2D material can circumvent these issues, but their reliable fabrication and systematic exploration of exotic quantum phenomena remain elusive. Here, we report the fabrication and characterization of a thickness-modulated lateral p-n homojunction from a single flake of Nb-doped MoS2. This configuration suppresses interface traps without external interface engineering, enabling excellent and highly stable device performance. The diodes exhibit strong rectifying behavior with a rectification ratio of approximate to 10(4) and a remarkably low ideality factor (eta = 1.23). Notably, we observe field-dependent negative differential resistance (NDR) at low temperatures, offering unique prospects for unconventional electronic applications. The devices also achieve high photoresponsivity (1.09 x 103 A W-1), external quantum efficiency (2.16 x 10(5)%), and detectivity (7.5 x 1010 Jones). Furthermore, electrical breakdown studies reveal avalanche multiplication at relatively low voltages, enabling high-performance avalanche photodetectors. Overall, our results demonstrate a simple yet robust approach for probing carrier multiplication in 2D homojunction p-n diodes, underlining the broad potential of TMDCs in advanced optoelectronic and quantum device applications. |
Zhu, Bin; Tang, Jiulin; Cao, Qichao; Zhang, Nan; Yu, Xiaoan; Zhang, Kaisheng; Du, Hui; Li, Zhuo; Peng, Yanhua; Gao, Ruitong; Cai, Haoyuan; Yu, Xue-fang; Cheng, Jianbo; Yang, Xiaolong CHEMICAL ENGINEERING JOURNAL, 525 , 2025, ISSN: 1385-8947. @article{ISI:001641335200012, title = {Photothermal synergistic catalysis on Zr-doped ZnIn2S4 for mild alcoholysis of epoxides: Atomic-level acidity-basicity modulation and carrier dynamics steering}, author = {Bin Zhu and Jiulin Tang and Qichao Cao and Nan Zhang and Xiaoan Yu and Kaisheng Zhang and Hui Du and Zhuo Li and Yanhua Peng and Ruitong Gao and Haoyuan Cai and Xue-fang Yu and Jianbo Cheng and Xiaolong Yang}, doi = {10.1016/j.cej.2025.170765}, times_cited = {0}, issn = {1385-8947}, year = {2025}, date = {2025-12-01}, journal = {CHEMICAL ENGINEERING JOURNAL}, volume = {525}, publisher = {ELSEVIER SCIENCE SA}, address = {PO BOX 564, 1001 LAUSANNE, SWITZERLAND}, abstract = {The conventional nucleophilic addition of alcohols to epoxides for producing valuable beta-alkoxy alcohols typically requires strong acids and harsh conditions, hindering green synthesis under mild alternatives. Inspired by recent advances in photo-thermal-synergistic systems for energy and environmental applications, this work synthesized Zr-doped ZnIn2S4 (Zr-ZnIn2S4) nanosheets as a novel photothermal catalyst for the mild alcoholysis of epoxides. Remarkably, the optimal 2 % Zr-ZnIn2S4 catalyst achieved a 98.9 % yield for styrene oxide alcoholysis with isopropanol under blue light illumination at 80 degrees C. Structural characterization revealed that Zr doping modulated the electronic structure of ZnIn2S4, significantly enhancing surface acidity and basicity while simultaneously suppressing photogenerated carrier recombination through shallow-trap defects. The abundant exposed Zn/Zr sites functioned as acidic centers, facilitating the adsorption and polarization of epoxides-identified as the rate-determining step for pristine ZnIn2S4. Ultimately, the efficient separation of photogenerated carriers cooperatively promoted the nucleophilic addition reactions (SN1 and SN2) between the epoxide (styrene oxide or epichlorohydrin) and alcohol. This study provides deep insights into the atomic-level site design of Zr-Zn-In-S photothermal catalysts for achieving photothermal synergistic-driven organic transformations via photo-redox catalysis.}, keywords = {}, pubstate = {published}, tppubtype = {article} } The conventional nucleophilic addition of alcohols to epoxides for producing valuable beta-alkoxy alcohols typically requires strong acids and harsh conditions, hindering green synthesis under mild alternatives. Inspired by recent advances in photo-thermal-synergistic systems for energy and environmental applications, this work synthesized Zr-doped ZnIn2S4 (Zr-ZnIn2S4) nanosheets as a novel photothermal catalyst for the mild alcoholysis of epoxides. Remarkably, the optimal 2 % Zr-ZnIn2S4 catalyst achieved a 98.9 % yield for styrene oxide alcoholysis with isopropanol under blue light illumination at 80 degrees C. Structural characterization revealed that Zr doping modulated the electronic structure of ZnIn2S4, significantly enhancing surface acidity and basicity while simultaneously suppressing photogenerated carrier recombination through shallow-trap defects. The abundant exposed Zn/Zr sites functioned as acidic centers, facilitating the adsorption and polarization of epoxides-identified as the rate-determining step for pristine ZnIn2S4. Ultimately, the efficient separation of photogenerated carriers cooperatively promoted the nucleophilic addition reactions (SN1 and SN2) between the epoxide (styrene oxide or epichlorohydrin) and alcohol. This study provides deep insights into the atomic-level site design of Zr-Zn-In-S photothermal catalysts for achieving photothermal synergistic-driven organic transformations via photo-redox catalysis. |
Liu, Matthew W -J; Ulman, Kanchan Ajit; Zheng, Boyang; Jain, Arpit; Heintzelman, Daniel J; Wang, Ke; He, Wen; Dong, Chengye; Lu, Li-Syuan; Crespi, Vincent H; Quek, Su Ying; Robinson, Joshua A; Jr, Kenneth Knappenberger L Structure-Dependent Electronic Relaxation Dynamics of Two-Dimensional Silver Monolayers Journal Article NANO LETTERS, 25 (49), pp. 17145-17151, 2025, ISSN: 1530-6984. @article{ISI:001629007700001, title = {Structure-Dependent Electronic Relaxation Dynamics of Two-Dimensional Silver Monolayers}, author = {Matthew W -J Liu and Kanchan Ajit Ulman and Boyang Zheng and Arpit Jain and Daniel J Heintzelman and Ke Wang and Wen He and Chengye Dong and Li-Syuan Lu and Vincent H Crespi and Su Ying Quek and Joshua A Robinson and Kenneth Knappenberger L Jr}, doi = {10.1021/acs.nanolett.5c04723}, times_cited = {0}, issn = {1530-6984}, year = {2025}, date = {2025-12-01}, journal = {NANO LETTERS}, volume = {25}, number = {49}, pages = {17145-17151}, publisher = {AMER CHEMICAL SOC}, address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA}, abstract = {The electronic relaxation dynamics of two-dimensional silver polar metal heterostructures (2D-PMets), isolated with two different Ag lattice structures, were studied with femtosecond transient absorption (fs-TA) spectroscopy. The two 2D Ag phases, called Ag-(1) and Ag-(2), differ in atomic packing density, which leads to phase-specific ultralow frequency (ULF) phonon modes and visible electronic absorption transitions. Time-resolved kinetic traces for both phases were fit to a biexponential decay function, with the first decay component pertaining to ultrafast electronic relaxation and the second corresponding to carrier-phonon scattering. The first decay time constant tau(1) is <400 fs for both phases. In contrast, carrier-phonon scattering exhibited lattice-specific and excitation wavelength-independent relaxation time constants; tau(2) similar to 2 ps for Ag-(1) and similar to 1 ps for Ag-(2). The shorter tau(2) in Ag-(2) is attributed to increased carrier-phonon scattering probability in more close-packed lateral structures. The results indicate that atomic-level structure controls energy flow in spatially confined 2D materials.}, keywords = {}, pubstate = {published}, tppubtype = {article} } The electronic relaxation dynamics of two-dimensional silver polar metal heterostructures (2D-PMets), isolated with two different Ag lattice structures, were studied with femtosecond transient absorption (fs-TA) spectroscopy. The two 2D Ag phases, called Ag-(1) and Ag-(2), differ in atomic packing density, which leads to phase-specific ultralow frequency (ULF) phonon modes and visible electronic absorption transitions. Time-resolved kinetic traces for both phases were fit to a biexponential decay function, with the first decay component pertaining to ultrafast electronic relaxation and the second corresponding to carrier-phonon scattering. The first decay time constant tau(1) is <400 fs for both phases. In contrast, carrier-phonon scattering exhibited lattice-specific and excitation wavelength-independent relaxation time constants; tau(2) similar to 2 ps for Ag-(1) and similar to 1 ps for Ag-(2). The shorter tau(2) in Ag-(2) is attributed to increased carrier-phonon scattering probability in more close-packed lateral structures. The results indicate that atomic-level structure controls energy flow in spatially confined 2D materials. |
Shi, Lu; Zhang, Hanning; Grebenko, Artem K; Yamaletdinov, Ruslan; Rejaul, S K; Shivajirao, Ranjith; Tong, Zheng Jue; Luchkin, Sergey; Zhang, Hongji; Iakoubovskii, Konstantin V; Alekseeva, Alena A; Starkov, Andrei; Orofeo, Carlo M; Lin, Junhao; Suenaga, Kazutomo; Toh, Chee-Tat; Mahfouz, Remi; Tayeb, Talah M; Qari, Nada; Adams, Stefan; Weber, Bent; Yazyev, Oleg V; Ozyilmaz, Barbaros Monolayer Amorphous Carbon: Unlocking Disorder-Induced Lithiophilicity Journal Article ADVANCED SCIENCE, 2025. @article{ISI:001622287600001, title = {Monolayer Amorphous Carbon: Unlocking Disorder-Induced Lithiophilicity}, author = {Lu Shi and Hanning Zhang and Artem K Grebenko and Ruslan Yamaletdinov and S K Rejaul and Ranjith Shivajirao and Zheng Jue Tong and Sergey Luchkin and Hongji Zhang and Konstantin V Iakoubovskii and Alena A Alekseeva and Andrei Starkov and Carlo M Orofeo and Junhao Lin and Kazutomo Suenaga and Chee-Tat Toh and Remi Mahfouz and Talah M Tayeb and Nada Qari and Stefan Adams and Bent Weber and Oleg V Yazyev and Barbaros Ozyilmaz}, doi = {10.1002/advs.202516490}, times_cited = {0}, year = {2025}, date = {2025-11-25}, journal = {ADVANCED SCIENCE}, publisher = {WILEY}, address = {111 RIVER ST, HOBOKEN 07030-5774, NJ USA}, abstract = {Dendritic lithium growth on the current collector remains a major obstacle to developing anode-less batteries, arising from inhomogeneous lithium nucleation and uneven surface lithiophilicity. Existing approaches, such as metallic or carbonaceous interlayers, often fail to stabilize lithium deposition due to mechanical degradation or spatial variations in lithium affinity. Here, we demonstrate that a monolayer amorphous carbon (MAC) film-a single-atom-thick disordered sp2 network grown directly on copper-can fundamentally alter lithium nucleation behavior. The topological disorder of MAC produces a dense distribution of electron-rich sites that uniformly strengthen lithium binding. As a result, the MAC surface exhibits a lithium contact angle of 31 +/- 5 degrees, four times lower than that of graphene and nearly three times lower than that of bare copper, leading to homogeneous wetting and deposition. Electrochemical tests reveal a reduced nucleation overpotential of 28.9 mV at 0.5 mA cm-2. Density functional theory and scanning tunneling microscopy confirm that disorder-induced localization of states near the Fermi level enhances electronegativity and forms continuous lithium-binding sites. These findings establish intrinsic structural disorder, rather than chemical doping, as an effective route to designing uniformly lithiophilic current collectors for next-generation anode-less batteries.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Dendritic lithium growth on the current collector remains a major obstacle to developing anode-less batteries, arising from inhomogeneous lithium nucleation and uneven surface lithiophilicity. Existing approaches, such as metallic or carbonaceous interlayers, often fail to stabilize lithium deposition due to mechanical degradation or spatial variations in lithium affinity. Here, we demonstrate that a monolayer amorphous carbon (MAC) film-a single-atom-thick disordered sp2 network grown directly on copper-can fundamentally alter lithium nucleation behavior. The topological disorder of MAC produces a dense distribution of electron-rich sites that uniformly strengthen lithium binding. As a result, the MAC surface exhibits a lithium contact angle of 31 +/- 5 degrees, four times lower than that of graphene and nearly three times lower than that of bare copper, leading to homogeneous wetting and deposition. Electrochemical tests reveal a reduced nucleation overpotential of 28.9 mV at 0.5 mA cm-2. Density functional theory and scanning tunneling microscopy confirm that disorder-induced localization of states near the Fermi level enhances electronegativity and forms continuous lithium-binding sites. These findings establish intrinsic structural disorder, rather than chemical doping, as an effective route to designing uniformly lithiophilic current collectors for next-generation anode-less batteries. |
Fu, Deyi; Liu, Jiawei; Hou, Fuchen; Chang, Xiao; Qu, Tingyu; Felisaz, Johan; Krishnaswamy, Gunasheel Kauwtilyaa; Grebenchuk, Sergey; Jie, Yuang; Watanabe, Kenji; Taniguchi, Takashi; Pereira, Vitor M; Novoselov, Kostya S; Koperski, Maciej; Yakovlev, Nikolai L; Soumyanarayanan, Anjan; Avsar, Ahmet; Yazyev, Oleg V; Lin, Junhao; Ozyilmaz, Barbaros Electric field-tunable ferromagnetism in a van der Waals semiconductor up to room temperature Journal Article NATURE COMMUNICATIONS, 16 (1), 2025. @article{ISI:001620530800035, title = {Electric field-tunable ferromagnetism in a van der Waals semiconductor up to room temperature}, author = {Deyi Fu and Jiawei Liu and Fuchen Hou and Xiao Chang and Tingyu Qu and Johan Felisaz and Gunasheel Kauwtilyaa Krishnaswamy and Sergey Grebenchuk and Yuang Jie and Kenji Watanabe and Takashi Taniguchi and Vitor M Pereira and Kostya S Novoselov and Maciej Koperski and Nikolai L Yakovlev and Anjan Soumyanarayanan and Ahmet Avsar and Oleg V Yazyev and Junhao Lin and Barbaros Ozyilmaz}, doi = {10.1038/s41467-025-59961-2}, times_cited = {0}, year = {2025}, date = {2025-11-20}, journal = {NATURE COMMUNICATIONS}, volume = {16}, number = {1}, publisher = {NATURE PORTFOLIO}, address = {HEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY}, abstract = {Ferromagnetic semiconductors, coupling charge transport and magnetism via electrical means, show great promise for spin-based logic devices. Despite decades of efforts to achieve such co-functionality, maintaining ferromagnetic order at room temperature remains elusive. Here, we address this long-standing challenge by implanting dilute Co atoms into few-layer black phosphorus through atomically-thin boron nitride diffusion barrier. Our Co-doped black phosphorus-based devices exhibit ferromagnetism up to room temperature while preserving its high mobility (similar to 1000cm(2)V(-1)s(-1)) and semiconducting characteristics. By incorporating ferromagnetic Co-doped black phosphorus into magnetic tunnel junction devices, we demonstrate a large tunnelling magnetoresistance that extends up to room temperature. This study presents a new approach to engineering ferromagnetic ordering in otherwise nonmagnetic materials, thereby expanding the repertoire and applications of magnetic semiconductors envisioned thus far.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Ferromagnetic semiconductors, coupling charge transport and magnetism via electrical means, show great promise for spin-based logic devices. Despite decades of efforts to achieve such co-functionality, maintaining ferromagnetic order at room temperature remains elusive. Here, we address this long-standing challenge by implanting dilute Co atoms into few-layer black phosphorus through atomically-thin boron nitride diffusion barrier. Our Co-doped black phosphorus-based devices exhibit ferromagnetism up to room temperature while preserving its high mobility (similar to 1000cm(2)V(-1)s(-1)) and semiconducting characteristics. By incorporating ferromagnetic Co-doped black phosphorus into magnetic tunnel junction devices, we demonstrate a large tunnelling magnetoresistance that extends up to room temperature. This study presents a new approach to engineering ferromagnetic ordering in otherwise nonmagnetic materials, thereby expanding the repertoire and applications of magnetic semiconductors envisioned thus far. |
Zhang, Deqiang; Yeo, Jing Ying; Zhang, Hanning; Yamaletdinov, Ruslan; Yang, Qian; Zhan, Yufeng; Martin-Fernandez, Inigo; Yazyev, Oleg V; Toh, Chee-Tat; Ozyilmaz, Barbaros Dry Transfer of CVD Graphene Film Using Adhesion Switchable Ferroelectric Polymers Journal Article ADVANCED MATERIALS, 37 (50), 2025, ISSN: 0935-9648. @article{ISI:001618079400001, title = {Dry Transfer of CVD Graphene Film Using Adhesion Switchable Ferroelectric Polymers}, author = {Deqiang Zhang and Jing Ying Yeo and Hanning Zhang and Ruslan Yamaletdinov and Qian Yang and Yufeng Zhan and Inigo Martin-Fernandez and Oleg V Yazyev and Chee-Tat Toh and Barbaros Ozyilmaz}, doi = {10.1002/adma.202510545}, times_cited = {0}, issn = {0935-9648}, year = {2025}, date = {2025-11-19}, journal = {ADVANCED MATERIALS}, volume = {37}, number = {50}, publisher = {WILEY-V C H VERLAG GMBH}, address = {POSTFACH 101161, 69451 WEINHEIM, GERMANY}, abstract = {Although chemical vapor deposition (CVD) produces meter-scale, high-quality graphene (Gr) on copper (Cu) foils, its practical integration is hampered by challenges in the transfer process. Conventional wet transfers are slow, produce chemical waste, and lack scalability, whereas existing dry transfer methods struggle with mechanical damage and residues due to strong Gr-Cu adhesion and the difficulty in precisely tuning interfacial forces. Here, a fully dry, industrially compatible transfer platform utilizing a ferroelectric poly(vinylidene-fluoride-trifluoroethylene) (P(VDF-TrFE)) film with electrostatically switchable adhesion, serving as both a mechanical support and a transfer layer, is demonstrated. Negative Corona poling of P(VDF-TrFE) induces p-type doping in graphene. Density Functional Theory calculations confirm that this simultaneously reduces Gr-Cu adhesion while increasing P(VDF-TrFE)-Gr adhesion, enabling clean, large-scale graphene delamination from Cu foils with >99% coverage. Subsequent thermal annealing above P(VDF-TrFE)'s Curie temperature (approximate to 135 degrees C) depolarizes the film, neutralizing the interfacial charge for a clean release. The versatility of this method is shown for other two-dimensional (2D) materials, including molybdenum disulfide and hexagonal boron nitride. Crucially, the process has been validated on cm-scale samples using a fully automated system with a transfer time of <5 min, highlighting a viable path toward industrial-scale production of high-quality 2D material films.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Although chemical vapor deposition (CVD) produces meter-scale, high-quality graphene (Gr) on copper (Cu) foils, its practical integration is hampered by challenges in the transfer process. Conventional wet transfers are slow, produce chemical waste, and lack scalability, whereas existing dry transfer methods struggle with mechanical damage and residues due to strong Gr-Cu adhesion and the difficulty in precisely tuning interfacial forces. Here, a fully dry, industrially compatible transfer platform utilizing a ferroelectric poly(vinylidene-fluoride-trifluoroethylene) (P(VDF-TrFE)) film with electrostatically switchable adhesion, serving as both a mechanical support and a transfer layer, is demonstrated. Negative Corona poling of P(VDF-TrFE) induces p-type doping in graphene. Density Functional Theory calculations confirm that this simultaneously reduces Gr-Cu adhesion while increasing P(VDF-TrFE)-Gr adhesion, enabling clean, large-scale graphene delamination from Cu foils with >99% coverage. Subsequent thermal annealing above P(VDF-TrFE)'s Curie temperature (approximate to 135 degrees C) depolarizes the film, neutralizing the interfacial charge for a clean release. The versatility of this method is shown for other two-dimensional (2D) materials, including molybdenum disulfide and hexagonal boron nitride. Crucially, the process has been validated on cm-scale samples using a fully automated system with a transfer time of <5 min, highlighting a viable path toward industrial-scale production of high-quality 2D material films. |
Li, Huanxin; Chen, Haotian; Pang, Boyi; Zhang, Jincan; Luo, Bingcheng; Silva, Ravi S P; Wang, Yi-Chi; Zhao, Siyu; Shearing, Paul R; Robinson, James B; Novoselov, Kostya S textitVan-textitder-textitWaals-textitforces-modulated graphene-P-phenyl-graphene carbon allotropes Journal Article NATURE COMMUNICATIONS, 16 (1), 2025. @article{ISI:001616374600008, title = {textitVan-textitder-textitWaals-textitforces-modulated graphene-P-phenyl-graphene carbon allotropes}, author = {Huanxin Li and Haotian Chen and Boyi Pang and Jincan Zhang and Bingcheng Luo and Ravi S P Silva and Yi-Chi Wang and Siyu Zhao and Paul R Shearing and James B Robinson and Kostya S Novoselov}, doi = {10.1038/s41467-025-64971-1}, times_cited = {0}, year = {2025}, date = {2025-11-14}, journal = {NATURE COMMUNICATIONS}, volume = {16}, number = {1}, publisher = {NATURE PORTFOLIO}, address = {HEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY}, abstract = {Graphene has received much attention due to its monoatomic, unique two-dimensional structure, which results in remarkable mechanical, physical, and electrical properties. However, synthesizing high-quality graphene-based composites with high conductivity and ionic mobility remains challenging. Here, we report an allotrope to the nanocarbon family, Graphene-P-phenyl-Graphene, synthesized by inserting pi-pi-conjugated p-phenyls between graphene layers and connecting them via C-C sigma bonds. Graphene-P-phenyl-Graphene is thermally and dynamically stable, as verified by density functional theory and molecular dynamics, and can be produced at kilogram scale. The p-phenyl bridges swell the layer spacing from similar to 0.34 to similar to 0.56 nm, reducing van der Waals forces and enhancing electron delocalization. Electrons in these separated graphene layers benefit from low mass and efficient 3D screening of charge scattering, resulting in high Hall mobility (10,000-13,000 cm(2) V-1 s(-1)) in freestanding films. The expanded spacing also enables decoupling of layer electrons and rapid ion storage and transport-even for large ions. For example, potassium-ion batteries using Graphene-P-phenyl-Graphene exhibit high reversible capacity, long-term stability, and high charge-discharge rates. Graphene-P-phenyl-Graphene holds promise for large-scale, portable, high-performance electronics with energy storage capabilities.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Graphene has received much attention due to its monoatomic, unique two-dimensional structure, which results in remarkable mechanical, physical, and electrical properties. However, synthesizing high-quality graphene-based composites with high conductivity and ionic mobility remains challenging. Here, we report an allotrope to the nanocarbon family, Graphene-P-phenyl-Graphene, synthesized by inserting pi-pi-conjugated p-phenyls between graphene layers and connecting them via C-C sigma bonds. Graphene-P-phenyl-Graphene is thermally and dynamically stable, as verified by density functional theory and molecular dynamics, and can be produced at kilogram scale. The p-phenyl bridges swell the layer spacing from similar to 0.34 to similar to 0.56 nm, reducing van der Waals forces and enhancing electron delocalization. Electrons in these separated graphene layers benefit from low mass and efficient 3D screening of charge scattering, resulting in high Hall mobility (10,000-13,000 cm(2) V-1 s(-1)) in freestanding films. The expanded spacing also enables decoupling of layer electrons and rapid ion storage and transport-even for large ions. For example, potassium-ion batteries using Graphene-P-phenyl-Graphene exhibit high reversible capacity, long-term stability, and high charge-discharge rates. Graphene-P-phenyl-Graphene holds promise for large-scale, portable, high-performance electronics with energy storage capabilities. |
Jiang, Yingying; Lin, Guoming; Mirsaidov, Utkur Nucleation and crystallization of metal oxides from carbonates Journal Article NANOSCALE, 17 (45), pp. 26194-26202, 2025, ISSN: 2040-3364. @article{ISI:001608691200001, title = {Nucleation and crystallization of metal oxides from carbonates}, author = {Yingying Jiang and Guoming Lin and Utkur Mirsaidov}, doi = {10.1039/d5nr01525a}, times_cited = {0}, issn = {2040-3364}, year = {2025}, date = {2025-11-06}, journal = {NANOSCALE}, volume = {17}, number = {45}, pages = {26194-26202}, publisher = {ROYAL SOC CHEMISTRY}, address = {THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND}, abstract = {Metal oxides play an important role in catalysis, integrated circuit fabrication, and optical coatings. A common approach for obtaining these oxides is the thermal decomposition of solid precursor templates, among which metal carbonates are the most widely used ones. Despite the importance of the process, the atomic-scale mechanisms governing the transformation of such templates into oxides remain insufficiently understood. Using in situ transmission electron microscopy (TEM), we show that La2(CO3)3 keywords = {}, pubstate = {published}, tppubtype = {article} } Metal oxides play an important role in catalysis, integrated circuit fabrication, and optical coatings. A common approach for obtaining these oxides is the thermal decomposition of solid precursor templates, among which metal carbonates are the most widely used ones. Despite the importance of the process, the atomic-scale mechanisms governing the transformation of such templates into oxides remain insufficiently understood. Using in situ transmission electron microscopy (TEM), we show that La2(CO3)3<middle dot>8H2O and Ce2(CO3)3<middle dot>8H2O undergo a multistep transformation: (i) dehydrogenation, (ii) decarbonization, and (iii) crystallization. Our observations reveal concurrent compositional and structural changes within the precursor templates during their conversion to oxides. These findings offer valuable insights into the crystallization of metal oxides, providing a basis for optimizing their properties for diverse technological applications. |
Tewari, Chetna; Rawat, Kundan Singh; Kim, Youngnam; Arya, Tanuja; Dhali, Sunil; Rana, Sravendra; Andreeva, Daria V; Ozyilmaz, Barbaros; Mahfouz, Remi; Qari, Nada; Jung, Yong Chae; Sahoo, Nanda Gopal; Novoselov, Kostya S Functional nanocarbons from waste plastics for energy storage applications Journal Article RENEWABLE & SUSTAINABLE ENERGY REVIEWS, 226 , 2025, ISSN: 1364-0321. @article{ISI:001614303300001, title = {Functional nanocarbons from waste plastics for energy storage applications}, author = {Chetna Tewari and Kundan Singh Rawat and Youngnam Kim and Tanuja Arya and Sunil Dhali and Sravendra Rana and Daria V Andreeva and Barbaros Ozyilmaz and Remi Mahfouz and Nada Qari and Yong Chae Jung and Nanda Gopal Sahoo and Kostya S Novoselov}, doi = {10.1016/j.rser.2025.116443}, times_cited = {0}, issn = {1364-0321}, year = {2025}, date = {2025-11-05}, journal = {RENEWABLE & SUSTAINABLE ENERGY REVIEWS}, volume = {226}, publisher = {PERGAMON-ELSEVIER SCIENCE LTD}, address = {THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND}, abstract = {The mismanagement of waste plastic could lead to significant environmental challenge, underscoring the urgent need for adopting innovative strategies that will address its management and utilization. At the same time, the growing demand for sustainable energy storage materials necessitates the exploration of resourceful solutions including advanced plastic-based materials. Addressing these dual concerns, this review examines the transformation of waste plastics into functional nanocarbons (FNCs) for energy-related applications. This review provides a comprehensive analysis of zero-to-three-dimensional FNCs derived from waste plastics, detailing synthesis techniques such as chemical vapor deposition, pyrolysis/catalytic pyrolysis, and hydrothermal carbonization, along with the underlying mechanisms. Key factors influencing the conversion process-including pressure, temperature, and catalytic systems-are thoroughly examined. Discussions on morphology and surface chemistry shed light on strategies to optimize material properties for specific applications. Special attention is given to the performance of FNCs in supercapacitors and batteries, using benchmarks such as electrical conductivity, specific surface area, and cycling stability to evaluate their suitability for energy storage. Additionally, the review incorporates a circular economic perspective, offering insights into how upcycling waste plastics into FNCs can contribute to a more sustainable future. It identifies critical research gaps, evaluates the environmental impacts of these processes, and highlights promising opportunities for innovation. By fostering interdisciplinary collaboration and bridging knowledge gaps, this review aims to inspire advancements in both waste plastic upcycling and energy technologies, ultimately contributing to sustainable solutions for urgent environmental and energy challenges.}, keywords = {}, pubstate = {published}, tppubtype = {article} } The mismanagement of waste plastic could lead to significant environmental challenge, underscoring the urgent need for adopting innovative strategies that will address its management and utilization. At the same time, the growing demand for sustainable energy storage materials necessitates the exploration of resourceful solutions including advanced plastic-based materials. Addressing these dual concerns, this review examines the transformation of waste plastics into functional nanocarbons (FNCs) for energy-related applications. This review provides a comprehensive analysis of zero-to-three-dimensional FNCs derived from waste plastics, detailing synthesis techniques such as chemical vapor deposition, pyrolysis/catalytic pyrolysis, and hydrothermal carbonization, along with the underlying mechanisms. Key factors influencing the conversion process-including pressure, temperature, and catalytic systems-are thoroughly examined. Discussions on morphology and surface chemistry shed light on strategies to optimize material properties for specific applications. Special attention is given to the performance of FNCs in supercapacitors and batteries, using benchmarks such as electrical conductivity, specific surface area, and cycling stability to evaluate their suitability for energy storage. Additionally, the review incorporates a circular economic perspective, offering insights into how upcycling waste plastics into FNCs can contribute to a more sustainable future. It identifies critical research gaps, evaluates the environmental impacts of these processes, and highlights promising opportunities for innovation. By fostering interdisciplinary collaboration and bridging knowledge gaps, this review aims to inspire advancements in both waste plastic upcycling and energy technologies, ultimately contributing to sustainable solutions for urgent environmental and energy challenges. |
Wang, Wenhui; Zhu, Mingyun; Erofeev, Ivan; Lin, Guoming; Yin, Kuibo; Sun, Litao; Mirsaidov, Utkur Size-Focusing of Au Nanoparticles through Dissolution-Renucleation Process Imaged with In Situ TEM Journal Article SMALL METHODS, 9 (11), 2025, ISSN: 2366-9608. @article{ISI:001597531200001, title = {Size-Focusing of Au Nanoparticles through Dissolution-Renucleation Process Imaged with In Situ TEM}, author = {Wenhui Wang and Mingyun Zhu and Ivan Erofeev and Guoming Lin and Kuibo Yin and Litao Sun and Utkur Mirsaidov}, doi = {10.1002/smtd.202501033}, times_cited = {0}, issn = {2366-9608}, year = {2025}, date = {2025-10-22}, journal = {SMALL METHODS}, volume = {9}, number = {11}, publisher = {WILEY-V C H VERLAG GMBH}, address = {POSTFACH 101161, 69451 WEINHEIM, GERMANY}, abstract = {The transformation of large polydisperse nanoparticles (NPs) into small monodisperse ones by adding ligands is an important and powerful post-synthesis method for tuning the size and morphology of NPs. However, the mechanism of this widely used process is not well understood. Here, using in situ liquid-phase transmission electron microscopy (TEM), we show that the steps of this transformation are a complete dissolution of the original NPs and a subsequent renucleation and growth of new, smaller, uniformly-sized NPs. This work offers mechanistic insights into the synthesis of monodisperse NPs and highlights the importance of direct imaging in identifying the physical and chemical details of nanoscale processes that occur in a liquid phase.}, keywords = {}, pubstate = {published}, tppubtype = {article} } The transformation of large polydisperse nanoparticles (NPs) into small monodisperse ones by adding ligands is an important and powerful post-synthesis method for tuning the size and morphology of NPs. However, the mechanism of this widely used process is not well understood. Here, using in situ liquid-phase transmission electron microscopy (TEM), we show that the steps of this transformation are a complete dissolution of the original NPs and a subsequent renucleation and growth of new, smaller, uniformly-sized NPs. This work offers mechanistic insights into the synthesis of monodisperse NPs and highlights the importance of direct imaging in identifying the physical and chemical details of nanoscale processes that occur in a liquid phase. |
Lai, Wenhui; Lee, Jong Hak; Yeo, Zhen Yuan; Yuan, Yue; Liu, Yuqing; Shi, Lu; Pu, Yanhui; Ong, Yong Kang; Limpo, Carlos Maria Alava; Rao, Yifan; Xiong, Ting; Lanza, Mario; Loh, Duane N; Ozyilmaz, Barbaros Robust Silicon-Based Anode with High Energy Density upon Dual Welding Encapsulation Journal Article ACS NANO, 19 (43), pp. 38040-38052, 2025, ISSN: 1936-0851. @article{ISI:001598368000001, title = {Robust Silicon-Based Anode with High Energy Density upon Dual Welding Encapsulation}, author = {Wenhui Lai and Jong Hak Lee and Zhen Yuan Yeo and Yue Yuan and Yuqing Liu and Lu Shi and Yanhui Pu and Yong Kang Ong and Carlos Maria Alava Limpo and Yifan Rao and Ting Xiong and Mario Lanza and Duane N Loh and Barbaros Ozyilmaz}, doi = {10.1021/acsnano.5c13278}, times_cited = {0}, issn = {1936-0851}, year = {2025}, date = {2025-10-22}, journal = {ACS NANO}, volume = {19}, number = {43}, pages = {38040-38052}, publisher = {AMER CHEMICAL SOC}, address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA}, abstract = {Silicon has long been considered one of the most promising anode materials for high-performance lithium-ion batteries due to its high theoretical capacity. However, a significant challenge that restricts its practical application is the persistent issue of weak interfacial contact in the silicon anode, which leads to structural instability during lithiation/delithiation processes due to large volume expansion. In this work, we develop a dual welding encapsulation strategy by constructing Si-C chemical bonding between the silicon and conductive covering shells and establishing C-C interlayer bonding connections among the covering shells. By directly examining the interface of silicon-based composites, we identify the types of compounds and hybrid orbital structures from their spatial distribution using machine-learning-enhanced transmission electron microscopy analysis techniques. This dual welding mechanism not only enhances the mechanical strength of the protective carbon shell but also ensures sustained electrical connection between the core and shell through the Si-C bonds. The robust heterogeneous structure effectively mitigates interfacial instability within the silicon anode, suppressing volume expansion below 12% after 300 cycles. Thus, the full-cell with the composite anode and LiNi0.8Co0.1Mn0.1O2 cathode performs a high energy density of 576 Wh kg-1 and stable cycling, inspiring the construction of commercial silicon batteries.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Silicon has long been considered one of the most promising anode materials for high-performance lithium-ion batteries due to its high theoretical capacity. However, a significant challenge that restricts its practical application is the persistent issue of weak interfacial contact in the silicon anode, which leads to structural instability during lithiation/delithiation processes due to large volume expansion. In this work, we develop a dual welding encapsulation strategy by constructing Si-C chemical bonding between the silicon and conductive covering shells and establishing C-C interlayer bonding connections among the covering shells. By directly examining the interface of silicon-based composites, we identify the types of compounds and hybrid orbital structures from their spatial distribution using machine-learning-enhanced transmission electron microscopy analysis techniques. This dual welding mechanism not only enhances the mechanical strength of the protective carbon shell but also ensures sustained electrical connection between the core and shell through the Si-C bonds. The robust heterogeneous structure effectively mitigates interfacial instability within the silicon anode, suppressing volume expansion below 12% after 300 cycles. Thus, the full-cell with the composite anode and LiNi0.8Co0.1Mn0.1O2 cathode performs a high energy density of 576 Wh kg-1 and stable cycling, inspiring the construction of commercial silicon batteries. |
Zhang, Jingda; Quek, Su Ying Quantum Defects in 2D Transition Metal Dichalcogenides for Terahertz Technologies Journal Article ACS NANO, 19 (41), pp. 36204-36214, 2025, ISSN: 1936-0851. @article{ISI:001588895100001, title = {Quantum Defects in 2D Transition Metal Dichalcogenides for Terahertz Technologies}, author = {Jingda Zhang and Su Ying Quek}, doi = {10.1021/acsnano.5c06007}, times_cited = {0}, issn = {1936-0851}, year = {2025}, date = {2025-10-07}, journal = {ACS NANO}, volume = {19}, number = {41}, pages = {36204-36214}, publisher = {AMER CHEMICAL SOC}, address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA}, abstract = {Substitutional transition metal (TM) point defects have recently been controllably introduced in two-dimensional (2D) transition metal dichalcogenides. We identify quantum defect candidates through a first-principles materials discovery approach with 25 TM elements substituting Mo and W in 2D MoS2 and WSe2, respectively. We elucidate trends in the charge transition levels for these 50 systems and report the existence of defects with spin-triplet ground states and a zero-field splitting (ZFS) in the terahertz (THz) regime, in contrast to typical gigahertz values. These defects can couple to resonant near-infrared radiation, providing a route to applications as high-fidelity qubits controlled by spin-dependent optical transitions. The THz ZFS implies that these high-fidelity operations can take place at higher temperatures compared to the case for GHz qubits. Our results also point toward the possibility of realizing a single-photon THz emitter. This work broadens the scope of quantum defects, highlighting the opportunities for next-generation THz quantum technologies-an area of growing interest given the rapid advancement in the development of THz sources and detectors.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Substitutional transition metal (TM) point defects have recently been controllably introduced in two-dimensional (2D) transition metal dichalcogenides. We identify quantum defect candidates through a first-principles materials discovery approach with 25 TM elements substituting Mo and W in 2D MoS2 and WSe2, respectively. We elucidate trends in the charge transition levels for these 50 systems and report the existence of defects with spin-triplet ground states and a zero-field splitting (ZFS) in the terahertz (THz) regime, in contrast to typical gigahertz values. These defects can couple to resonant near-infrared radiation, providing a route to applications as high-fidelity qubits controlled by spin-dependent optical transitions. The THz ZFS implies that these high-fidelity operations can take place at higher temperatures compared to the case for GHz qubits. Our results also point toward the possibility of realizing a single-photon THz emitter. This work broadens the scope of quantum defects, highlighting the opportunities for next-generation THz quantum technologies-an area of growing interest given the rapid advancement in the development of THz sources and detectors. |
Jie, Yuang; Cai, Xiaofan; Lin, Yijie; Watanabe, Kenji; Taniguchi, Takashi; Yan, Jiaqiang; Ovchinnikov, Dmitry; Avsar, Ahmet Reconfigurable Magnetotransport in MnBi2Te4 via Gate and Magnetic Field Tuning Journal Article ADVANCED MATERIALS, 37 (50), 2025, ISSN: 0935-9648. @article{ISI:001581804400001, title = {Reconfigurable Magnetotransport in MnBi2Te4 via Gate and Magnetic Field Tuning}, author = {Yuang Jie and Xiaofan Cai and Yijie Lin and Kenji Watanabe and Takashi Taniguchi and Jiaqiang Yan and Dmitry Ovchinnikov and Ahmet Avsar}, doi = {10.1002/adma.202510734}, times_cited = {0}, issn = {0935-9648}, year = {2025}, date = {2025-09-26}, journal = {ADVANCED MATERIALS}, volume = {37}, number = {50}, publisher = {WILEY-V C H VERLAG GMBH}, address = {POSTFACH 101161, 69451 WEINHEIM, GERMANY}, abstract = {The intrinsic magnetic topological insulator MnBi2Te4 is a promising platform for exploring quantum phases with nontrivial band topology and for enabling electrical control over coupled magnetic and electronic phase transitions. In-plane magnetic fields, in particular, offer a distinct means of tuning these properties by strengthening quantized Hall effects, enhancing surface energy gaps, and driving spin reorientation transitions. However, a systematic understanding of how such fields affect magnetotransport is limited. Here, the magnetotransport behavior of few-layer MnBi2Te4 as a function of gate voltage, temperature, and magnetic field angle, with a primary focus on in-plane field effects, are investigated. A gate-tunable crossover in magnetoresistance is observed from positive to negative values under in-plane magnetic fields as the gate voltage is swept below the charge neutrality point at temperatures below the N & eacute;el temperature. The in-plane field drives a transition from the antiferromagnetic ground state to a ferromagnetic configuration with spins aligned in-plane, while simultaneously altering the electronic structure, as revealed by gate-dependent transport features. The angle-dependent measurements reveal strongly gate-tunable magnetotransport anisotropy. These results establish in-plane magnetic fields as an effective tuning parameter for modulating spin and charge transport in MnBi2Te4, advancing prospects for reconfigurable spintronic and topological devices.}, keywords = {}, pubstate = {published}, tppubtype = {article} } The intrinsic magnetic topological insulator MnBi2Te4 is a promising platform for exploring quantum phases with nontrivial band topology and for enabling electrical control over coupled magnetic and electronic phase transitions. In-plane magnetic fields, in particular, offer a distinct means of tuning these properties by strengthening quantized Hall effects, enhancing surface energy gaps, and driving spin reorientation transitions. However, a systematic understanding of how such fields affect magnetotransport is limited. Here, the magnetotransport behavior of few-layer MnBi2Te4 as a function of gate voltage, temperature, and magnetic field angle, with a primary focus on in-plane field effects, are investigated. A gate-tunable crossover in magnetoresistance is observed from positive to negative values under in-plane magnetic fields as the gate voltage is swept below the charge neutrality point at temperatures below the N & eacute;el temperature. The in-plane field drives a transition from the antiferromagnetic ground state to a ferromagnetic configuration with spins aligned in-plane, while simultaneously altering the electronic structure, as revealed by gate-dependent transport features. The angle-dependent measurements reveal strongly gate-tunable magnetotransport anisotropy. These results establish in-plane magnetic fields as an effective tuning parameter for modulating spin and charge transport in MnBi2Te4, advancing prospects for reconfigurable spintronic and topological devices. |
Mishra, Abhishek; Verzhbitskiy, Ivan A; Lee, Rainer; Rodin, Aleksandr; Zhang, Zhepeng; Das, Sarthak; Lau, Chit Siong; Huang, Ding; Eda, Goki; Goh, Kuan Eng Johnson Hopping conduction in quasi-1D titanium trisulfide layered nanoribbons Journal Article APPLIED PHYSICS LETTERS, 127 (11), 2025, ISSN: 0003-6951. @article{ISI:001572716900010, title = {Hopping conduction in quasi-1D titanium trisulfide layered nanoribbons}, author = {Abhishek Mishra and Ivan A Verzhbitskiy and Rainer Lee and Aleksandr Rodin and Zhepeng Zhang and Sarthak Das and Chit Siong Lau and Ding Huang and Goki Eda and Kuan Eng Johnson Goh}, doi = {10.1063/5.0281384}, times_cited = {0}, issn = {0003-6951}, year = {2025}, date = {2025-09-15}, journal = {APPLIED PHYSICS LETTERS}, volume = {127}, number = {11}, publisher = {AIP Publishing}, address = {1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA}, abstract = {Quasi-one-dimensional (quasi-1D) layered nanoribbons (NRs) are being extensively investigated for their potential applications in next-generation nanoelectronics and optoelectronics. Understanding electrical conduction in such NRs is essential for designing the devices. In this work, we provide insights into hopping conduction mechanisms in NR transistors based on titanium trisulfide (TiS3), a quasi-1D layered semiconductor with distinctive anisotropic properties. We report both linear and nonlinear current-voltage characteristics over a temperature range of 5-300 K. The thermal evolution of the nonlinear characteristics exhibits power-law scaling and collapses onto a single universal curve when scaled by temperature. Our findings suggest that the nonlinear conduction is dominated by rare-chain hopping, having its origins in the disorders in TiS3.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Quasi-one-dimensional (quasi-1D) layered nanoribbons (NRs) are being extensively investigated for their potential applications in next-generation nanoelectronics and optoelectronics. Understanding electrical conduction in such NRs is essential for designing the devices. In this work, we provide insights into hopping conduction mechanisms in NR transistors based on titanium trisulfide (TiS3), a quasi-1D layered semiconductor with distinctive anisotropic properties. We report both linear and nonlinear current-voltage characteristics over a temperature range of 5-300 K. The thermal evolution of the nonlinear characteristics exhibits power-law scaling and collapses onto a single universal curve when scaled by temperature. Our findings suggest that the nonlinear conduction is dominated by rare-chain hopping, having its origins in the disorders in TiS3. |
Rao, Yifan; Lee, Jong Hak; Pu, Yanhui; Ong, Yong Kang; Shi, Lu; Lai, Wenhui; Limpo, Carlos; Yuan, Yue; Xiong, Ting; Lanza, Mario; Ozyilmaz, Barbaros Reinforcement-free monolithic all-in-one structural supercapacitors Journal Article CHEMICAL ENGINEERING JOURNAL, 519 , 2025, ISSN: 1385-8947. @article{ISI:001532082000001, title = {Reinforcement-free monolithic all-in-one structural supercapacitors}, author = {Yifan Rao and Jong Hak Lee and Yanhui Pu and Yong Kang Ong and Lu Shi and Wenhui Lai and Carlos Limpo and Yue Yuan and Ting Xiong and Mario Lanza and Barbaros Ozyilmaz}, doi = {10.1016/j.cej.2025.165492}, times_cited = {0}, issn = {1385-8947}, year = {2025}, date = {2025-09-01}, journal = {CHEMICAL ENGINEERING JOURNAL}, volume = {519}, publisher = {ELSEVIER SCIENCE SA}, address = {PO BOX 564, 1001 LAUSANNE, SWITZERLAND}, abstract = {Structural supercapacitors, potential game-changers for various applications such as aerospace, automotive, and construction industries, offer a combination of energy storage and load-bearing functionalities. Conventional approaches, however, have been hindered by a significant decrease in overall energy storage performance due to the inherent separation of energy storage components and structural reinforcement elements. In this study, we report reinforcement-free all-in-one structural supercapacitors that tailor the conventional trade-off problem between energy capacity and mechanical strength by ensuring that the essential energy storage components possess high mechanical properties. This dual-functional structure ensures that it volumetrically constitutes nearly 90% of the cells excluding the packaging. Simultaneously, by employing interlocking interfacial engineering, we optimize the functionalities of these components, enhancing the overall robustness and energy capacity of the device. Consequently, our structural supercapacitor demonstrates good structural integrity, as evidenced by its flexural modulus of 8.34 GPa. Moreover, our supercapacitor stands out in terms of energy storage capacity, boasting a volumetric energy density of 45 Wh/L. This achievement, outperforming the current state-of-the-art by a staggering tenfold, significantly enhances multifunctionality, a critical index for evaluating structural energy devices, reaching a 9.95 rating. This novel strategy provides insight for other structural energy storage devices with higher multifunctional efficiency.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Structural supercapacitors, potential game-changers for various applications such as aerospace, automotive, and construction industries, offer a combination of energy storage and load-bearing functionalities. Conventional approaches, however, have been hindered by a significant decrease in overall energy storage performance due to the inherent separation of energy storage components and structural reinforcement elements. In this study, we report reinforcement-free all-in-one structural supercapacitors that tailor the conventional trade-off problem between energy capacity and mechanical strength by ensuring that the essential energy storage components possess high mechanical properties. This dual-functional structure ensures that it volumetrically constitutes nearly 90% of the cells excluding the packaging. Simultaneously, by employing interlocking interfacial engineering, we optimize the functionalities of these components, enhancing the overall robustness and energy capacity of the device. Consequently, our structural supercapacitor demonstrates good structural integrity, as evidenced by its flexural modulus of 8.34 GPa. Moreover, our supercapacitor stands out in terms of energy storage capacity, boasting a volumetric energy density of 45 Wh/L. This achievement, outperforming the current state-of-the-art by a staggering tenfold, significantly enhances multifunctionality, a critical index for evaluating structural energy devices, reaching a 9.95 rating. This novel strategy provides insight for other structural energy storage devices with higher multifunctional efficiency. |