Publications
2026 |
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 RENEWABLE & SUSTAINABLE ENERGY REVIEWS, 226 (E), 2026, DOI: 10.1016/j.rser.2025.116443. @article{WOS: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 = {2026}, date = {2026-01-01}, journal = {RENEWABLE & SUSTAINABLE ENERGY REVIEWS}, volume = {226}, number = {E}, 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.
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2025 |
Tummala, Pinaka Pani; Afanas'ev, Valeri; Ferrini, Gabriele; Alia, Mario; Serafini, Andrea; Targa, Paolo; Codegoni, Davide; Martella, Christian; Molle, Alessandro; Lamperti, Alessio Experimental electron band alignment of 1T'and 2H MoTe2/SiO2 interface using internal photoemission spectroscopy JOURNAL OF ELECTRON SPECTROSCOPY AND RELATED PHENOMENA, 283 , 2025, DOI: 10.1016/j.elspec.2025.147575. @article{WOS:001612700500001, title = {Experimental electron band alignment of 1T'and 2H MoTe2/SiO2 interface using internal photoemission spectroscopy}, author = {Pinaka Pani Tummala and Valeri Afanas'ev and Gabriele Ferrini and Mario Alia and Andrea Serafini and Paolo Targa and Davide Codegoni and Christian Martella and Alessandro Molle and Alessio Lamperti}, doi = {10.1016/j.elspec.2025.147575}, times_cited = {0}, issn = {0368-2048}, year = {2025}, date = {2025-12-01}, journal = {JOURNAL OF ELECTRON SPECTROSCOPY AND RELATED PHENOMENA}, volume = {283}, publisher = {ELSEVIER}, address = {RADARWEG 29, 1043 NX AMSTERDAM, NETHERLANDS}, abstract = {Unlike other two-dimensional (2D) transition metal dichalcogenides, molybdenum ditelluride (MoTe2) displays a stable biphasic character in artificially synthesizable 2H and 1T' state. While these phases are inherently distinguished in their electronic band character (semiconducting and metallic, respectively), it is not clear how they electronically interface with technology relevant substrate where to engineer an electronic device layout. In this study, we experimentally determine the electron band alignment at interfaces between SiO2 and 1T'/2H of MoTe2 few-layers ultrathin films grown by chemical vapor deposition. We use internal photoemission spectroscopy to determine the energy barrier height between the 1T'/2H-MoTe2 Fermi level and the oxide conduction band (CB) bottom. This observation indicates the band gap opening in 2H-MoTe2 and provides an estimate of the barrier height for holes at the polytypic 1T'/2H-MoTe2 interface. In particular, by comparing the Fermi level energy in single-phase 1 T'-MoTe2 with the VB energy in 2H-MoTe2, we reveal a approximate to 0.4 eV difference, suggesting that the low Schottky barrier observed at the 1T'/2H interface results from Fermi level pinning, which is independent of interface defects and unaffected by the VdW gap. Our findings can be exploited for optimizing charge transport and device performance, facilitating the development of next-generation electronic and optoelectronic devices that harness the unique properties of both phases in MoTe2.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Unlike other two-dimensional (2D) transition metal dichalcogenides, molybdenum ditelluride (MoTe2) displays a stable biphasic character in artificially synthesizable 2H and 1T' state. While these phases are inherently distinguished in their electronic band character (semiconducting and metallic, respectively), it is not clear how they electronically interface with technology relevant substrate where to engineer an electronic device layout. In this study, we experimentally determine the electron band alignment at interfaces between SiO2 and 1T'/2H of MoTe2 few-layers ultrathin films grown by chemical vapor deposition. We use internal photoemission spectroscopy to determine the energy barrier height between the 1T'/2H-MoTe2 Fermi level and the oxide conduction band (CB) bottom. This observation indicates the band gap opening in 2H-MoTe2 and provides an estimate of the barrier height for holes at the polytypic 1T'/2H-MoTe2 interface. In particular, by comparing the Fermi level energy in single-phase 1 T'-MoTe2 with the VB energy in 2H-MoTe2, we reveal a approximate to 0.4 eV difference, suggesting that the low Schottky barrier observed at the 1T'/2H interface results from Fermi level pinning, which is independent of interface defects and unaffected by the VdW gap. Our findings can be exploited for optimizing charge transport and device performance, facilitating the development of next-generation electronic and optoelectronic devices that harness the unique properties of both phases in MoTe2.
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Rybin, M G; Guberna, E A; Kamynin, V A; Nguen, Van Chuc; Obraztsova, E D Modification of electrical characteristics of CVD- graphene by Joule heating CARBON TRENDS, 21 , 2025, DOI: 10.1016/j.cartre.2025.100577. @article{WOS:001591485000001, title = {Modification of electrical characteristics of CVD- graphene by Joule heating}, author = {M G Rybin and E A Guberna and V A Kamynin and Van Chuc Nguen and E D Obraztsova}, doi = {10.1016/j.cartre.2025.100577}, times_cited = {0}, issn = {2667-0569}, year = {2025}, date = {2025-12-01}, journal = {CARBON TRENDS}, volume = {21}, publisher = {ELSEVIER}, address = {RADARWEG 29, 1043 NX AMSTERDAM, NETHERLANDS}, abstract = {This paper presents an approach for enhancing the electrical characteristics of graphene synthesized by chemical vapor deposition (CVD), through a direct resistive heating of the graphene channel by an electric current. This method efficiently purifies graphene of impurities and restores the material ideal structure through the desorption of adsorbed molecules. A graphene field-effect transistor was employed to characterize the graphene, specifically - to assess the mobility and concentration of charge carriers. The study investigates the impact of annealing temperature on both the concentration and type of charge carriers. It was found that CVD-synthesized graphene exhibits p-type conductivity, with the charge neutrality point (CNP) positioned above 80 Volts gate voltage at a 300 nm thickness of SiO2. Annealing at 200 degrees C shifted this neutrality point to 0 Volts, switching the graphene to electrical neutrality. At higher annealing temperatures, n-type conductivity was achieved. Additionally, during the annealing process with current flow, there was a significant enhancement of the charge carriers mobility in graphene: for holes, mobility increased from 1000 cm2/(V center dot s) to 1800 cm2/(V center dot s), and for electrons - from 600 cm2/(V center dot s) to 1200 cm2/(V center dot s). Thus, the study reveals the effective method for removing impurities appeared after transfer of CVD graphene from copper foil to a dielectric substrate. This approach may be utilized in preparing samples for applications in microelectronics, optoelectronics, and related fields.}, keywords = {}, pubstate = {published}, tppubtype = {article} } This paper presents an approach for enhancing the electrical characteristics of graphene synthesized by chemical vapor deposition (CVD), through a direct resistive heating of the graphene channel by an electric current. This method efficiently purifies graphene of impurities and restores the material ideal structure through the desorption of adsorbed molecules. A graphene field-effect transistor was employed to characterize the graphene, specifically - to assess the mobility and concentration of charge carriers. The study investigates the impact of annealing temperature on both the concentration and type of charge carriers. It was found that CVD-synthesized graphene exhibits p-type conductivity, with the charge neutrality point (CNP) positioned above 80 Volts gate voltage at a 300 nm thickness of SiO2. Annealing at 200 degrees C shifted this neutrality point to 0 Volts, switching the graphene to electrical neutrality. At higher annealing temperatures, n-type conductivity was achieved. Additionally, during the annealing process with current flow, there was a significant enhancement of the charge carriers mobility in graphene: for holes, mobility increased from 1000 cm2/(V center dot s) to 1800 cm2/(V center dot s), and for electrons - from 600 cm2/(V center dot s) to 1200 cm2/(V center dot s). Thus, the study reveals the effective method for removing impurities appeared after transfer of CVD graphene from copper foil to a dielectric substrate. This approach may be utilized in preparing samples for applications in microelectronics, optoelectronics, and related fields.
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Yin, Yueming; Fu, Afu; Wang, Lipo Gaps between medical biology and AI drug discovery DRUG DISCOVERY TODAY, 30 (12), 2025, DOI: 10.1016/j.drudis.2025.104512. @article{WOS:001614334500001, title = {Gaps between medical biology and AI drug discovery}, author = {Yueming Yin and Afu Fu and Lipo Wang}, doi = {10.1016/j.drudis.2025.104512}, times_cited = {0}, issn = {1359-6446}, year = {2025}, date = {2025-12-01}, journal = {DRUG DISCOVERY TODAY}, volume = {30}, number = {12}, publisher = {ELSEVIER SCI LTD}, address = {125 London Wall, London, ENGLAND}, abstract = {Drug discovery is a complex, iterative process spanning biology, chemistry, pharmacology, and computational sciences. Artificial intelligence (AI) can accelerate this process but often misaligns with biological realities. Here, we highlight three crucial gaps in AI-driven drug discovery. First, conflating binding affinity with bioactivity ignores distinct experimental setups. Second, reliance on simplified bioactivity metrics limits the ability of AI models to capture richer biological contexts. Third, AI applications remain fragmented, addressing isolated tasks rather than integrating insights across pipeline stages. To bridge these gaps, we propose a biologically contextualized AI framework and provide guidelines for researchers in both medical biology and AI drug discovery.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Drug discovery is a complex, iterative process spanning biology, chemistry, pharmacology, and computational sciences. Artificial intelligence (AI) can accelerate this process but often misaligns with biological realities. Here, we highlight three crucial gaps in AI-driven drug discovery. First, conflating binding affinity with bioactivity ignores distinct experimental setups. Second, reliance on simplified bioactivity metrics limits the ability of AI models to capture richer biological contexts. Third, AI applications remain fragmented, addressing isolated tasks rather than integrating insights across pipeline stages. To bridge these gaps, we propose a biologically contextualized AI framework and provide guidelines for researchers in both medical biology and AI drug discovery.
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Ghods, Soheil; Jang, Ho-Chan; Choi, Jun-Hui; Kim, Min Woo; Lee, Hyunjin; Kim, Tae-Hoon; Heo, Keun; Kwun, Hyung Jun; Lee, Taehun; Lee, Yoon Kyeung; Lee, Sang Hoon; Kim, Seung-Il; Baek, Woonhyuk; Bae, Sukang; Moon, Ji-Yun; Lee, Jae-Hyun Selective Charge Injection via Topological van der Waals Contacts for Barrier-Free p-Type TMD Transistors ADVANCED FUNCTIONAL MATERIALS, 2025, DOI: 10.1002/adfm.202520506. @article{WOS:001610168200001, title = {Selective Charge Injection via Topological van der Waals Contacts for Barrier-Free p-Type TMD Transistors}, author = {Soheil Ghods and Ho-Chan Jang and Jun-Hui Choi and Min Woo Kim and Hyunjin Lee and Tae-Hoon Kim and Keun Heo and Hyung Jun Kwun and Taehun Lee and Yoon Kyeung Lee and Sang Hoon Lee and Seung-Il Kim and Woonhyuk Baek and Sukang Bae and Ji-Yun Moon and Jae-Hyun Lee}, doi = {10.1002/adfm.202520506}, times_cited = {0}, issn = {1616-301X}, year = {2025}, date = {2025-11-01}, journal = {ADVANCED FUNCTIONAL MATERIALS}, publisher = {WILEY-V C H VERLAG GMBH}, address = {POSTFACH 101161, 69451 WEINHEIM, GERMANY}, abstract = {The continued miniaturization of electronic and optoelectronic devices places stringent demands on contact engineering for 2D semiconductors, particularly for p-type materials, where achieving low-resistance contacts remains a critical challenge. While van der Waals (vdW) contacts offer a promising route for next-generation electronics, the impact of microscopic interfacial phenomena on device performance remains insufficiently understood. Here, how selective charge injection is revealed to be governed by key interfacial parameters between WTe2, a topological vdW contact, and both Se- and S-based transition metal dichalcogenide (TMD) channel materials. Through device measurements and first-principles simulations, it is shown that WTe2 forms an exceptional vdW contact with p-type MoSe2, exhibiting an ultralow Schottky barrier height (approximate to 7 meV), low contact resistance (approximate to 0.47 k Omega mu m), and high carrier mobility (373 cm2 V-1 s-1). This selective charge injection is attributed to a larger interlayer distance in WTe2/Se-based TMDs, which suppresses orbital overlap and preserves interface quality. These microscopic descriptors serve as essential design principles for future 2D electronic and optoelectronic systems.}, keywords = {}, pubstate = {published}, tppubtype = {article} } The continued miniaturization of electronic and optoelectronic devices places stringent demands on contact engineering for 2D semiconductors, particularly for p-type materials, where achieving low-resistance contacts remains a critical challenge. While van der Waals (vdW) contacts offer a promising route for next-generation electronics, the impact of microscopic interfacial phenomena on device performance remains insufficiently understood. Here, how selective charge injection is revealed to be governed by key interfacial parameters between WTe2, a topological vdW contact, and both Se- and S-based transition metal dichalcogenide (TMD) channel materials. Through device measurements and first-principles simulations, it is shown that WTe2 forms an exceptional vdW contact with p-type MoSe2, exhibiting an ultralow Schottky barrier height (approximate to 7 meV), low contact resistance (approximate to 0.47 k Omega mu m), and high carrier mobility (373 cm2 V-1 s-1). This selective charge injection is attributed to a larger interlayer distance in WTe2/Se-based TMDs, which suppresses orbital overlap and preserves interface quality. These microscopic descriptors serve as essential design principles for future 2D electronic and optoelectronic systems.
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Fu, Xinliang; Guo, Xiangyu; Shi, Pengyu; Frauenheim, Thomas; Novoselov, Kostya S; Yuan, Mingjian; Wang, Mei Control of CO2 Electrocatalysis via Modularly Customizable Graphdiyne JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 147 (46), pp. 42394-42405, 2025, DOI: 10.1021/jacs.5c11774. @article{WOS:001608563200001, title = {Control of CO2 Electrocatalysis via Modularly Customizable Graphdiyne}, author = {Xinliang Fu and Xiangyu Guo and Pengyu Shi and Thomas Frauenheim and Kostya S Novoselov and Mingjian Yuan and Mei Wang}, doi = {10.1021/jacs.5c11774}, times_cited = {0}, issn = {0002-7863}, year = {2025}, date = {2025-11-01}, journal = {JOURNAL OF THE AMERICAN CHEMICAL SOCIETY}, volume = {147}, number = {46}, pages = {42394-42405}, publisher = {AMER CHEMICAL SOC}, address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA}, abstract = {On-demand customization of materials with tailored structures and properties is a long-standing goal in materials science. Yet conventional materials often exhibit complex configurations, hindering unified design principles and limiting performance optimization. Here, utilizing modular graphdiyne (GDY) as a configurable platform, we present a chemically guided molecular design framework to achieve atomic-level precision control over catalytic behaviors. By combining density functional theory (DFT) with experimental validation, we systematically introduced electron-donating and electron-withdrawing groups to construct 13 organic molecular units, yielding modularly customizable GDYs with predetermined structures, enabling us to disentangle the interplay between structure and catalytic function. We identified a volcano-shaped correlation, linking the oxidation state of the active alkyne carbons to CO2 reduction (CO2RR) activity. Furthermore, we established that this oxidation state is directly correlated with intrinsic electronic descriptors, including work function, VBM, and Fermi level (E-f)-constructing a predictive framework. In particular, by precisely tuning the oxidation state of sp-hybridized carbons, we showed that GDYs can rationally optimize intermediate binding energies and effectively resolve the conventional trade-off between the CO2RR activity and HER suppression. This mechanistic approach enables systematic control of the CO/H-2 ratio from 1:10 to 13:1. Notably, the fluorinated GDY (3FGDY) achieves a remarkable 93% CO Faradaic efficiency with sustained stability over 90 h. These findings establish a direct atomic-level structure-performance relationship and provide a robust proof-of-concept for modular materials design, with promising implications for syngas production and sustainable energy conversion.}, keywords = {}, pubstate = {published}, tppubtype = {article} } On-demand customization of materials with tailored structures and properties is a long-standing goal in materials science. Yet conventional materials often exhibit complex configurations, hindering unified design principles and limiting performance optimization. Here, utilizing modular graphdiyne (GDY) as a configurable platform, we present a chemically guided molecular design framework to achieve atomic-level precision control over catalytic behaviors. By combining density functional theory (DFT) with experimental validation, we systematically introduced electron-donating and electron-withdrawing groups to construct 13 organic molecular units, yielding modularly customizable GDYs with predetermined structures, enabling us to disentangle the interplay between structure and catalytic function. We identified a volcano-shaped correlation, linking the oxidation state of the active alkyne carbons to CO2 reduction (CO2RR) activity. Furthermore, we established that this oxidation state is directly correlated with intrinsic electronic descriptors, including work function, VBM, and Fermi level (E-f)-constructing a predictive framework. In particular, by precisely tuning the oxidation state of sp-hybridized carbons, we showed that GDYs can rationally optimize intermediate binding energies and effectively resolve the conventional trade-off between the CO2RR activity and HER suppression. This mechanistic approach enables systematic control of the CO/H-2 ratio from 1:10 to 13:1. Notably, the fluorinated GDY (3FGDY) achieves a remarkable 93% CO Faradaic efficiency with sustained stability over 90 h. These findings establish a direct atomic-level structure-performance relationship and provide a robust proof-of-concept for modular materials design, with promising implications for syngas production and sustainable energy conversion.
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Jana, Dipankar; Acharya, Swagata; Orlita, Milan; Faugeras, Clement; Pashov, Dimitar; Schilfgaarde, Mark Van; Potemski, Marek; Koperski, Maciej Deconstruction of the Anisotropic Magnetic Interactions from Spin-Entangled Optical Excitations in van der Waals Antiferromagnets ADVANCED SCIENCE, 2025, DOI: 10.1002/advs.202505834. @article{WOS:001610214800001, title = {Deconstruction of the Anisotropic Magnetic Interactions from Spin-Entangled Optical Excitations in van der Waals Antiferromagnets}, author = {Dipankar Jana and Swagata Acharya and Milan Orlita and Clement Faugeras and Dimitar Pashov and Mark Van Schilfgaarde and Marek Potemski and Maciej Koperski}, doi = {10.1002/advs.202505834}, times_cited = {0}, year = {2025}, date = {2025-11-01}, journal = {ADVANCED SCIENCE}, publisher = {WILEY}, address = {111 RIVER ST, HOBOKEN 07030-5774, NJ USA}, abstract = {Magneto-optical excitations in antiferromagnetic d systems can originate from a multiplicity of light-spin and spin-spin interactions, as the light and spin degrees of freedom can be entangled. This is exemplified in van der Waals systems with attendant strong anisotropy between in-plane and out-of-plane directions, such as and films studied here. The rich interplay between the magnetic ordering and sub-bandgap optical transitions poses a challenge to resolve the mechanisms driving spin-entangled optical transitions, as well as the single-particle bandgap itself. Here, a high-fidelity ab initio theory is applied to find a realistic estimation of the bandgap by elucidating the atom- and orbital-resolved contributions to the fundamental sub-bands. It is further demonstrated that the spin-entangled excitations, observable as photoluminescence and absorption resonances, originate from an on-site spin-flip transition confined to a magnetic atom (Mn or Ni). The evolution of the spin-flip transition in a magnetic field is used to deduce the effective exchange coupling and anisotropy constants.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Magneto-optical excitations in antiferromagnetic d systems can originate from a multiplicity of light-spin and spin-spin interactions, as the light and spin degrees of freedom can be entangled. This is exemplified in van der Waals systems with attendant strong anisotropy between in-plane and out-of-plane directions, such as and films studied here. The rich interplay between the magnetic ordering and sub-bandgap optical transitions poses a challenge to resolve the mechanisms driving spin-entangled optical transitions, as well as the single-particle bandgap itself. Here, a high-fidelity ab initio theory is applied to find a realistic estimation of the bandgap by elucidating the atom- and orbital-resolved contributions to the fundamental sub-bands. It is further demonstrated that the spin-entangled excitations, observable as photoluminescence and absorption resonances, originate from an on-site spin-flip transition confined to a magnetic atom (Mn or Ni). The evolution of the spin-flip transition in a magnetic field is used to deduce the effective exchange coupling and anisotropy constants.
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Zhang, Zhi; Zhang, Yuwei; Lu, Kangjun; Zhang, Jun-Jie; Zhang, Nannan; Feng, Rui; Ye, Haoran; Zhou, Xiaoli; Li, Linglong; Wan, Dongyang; Lu, Junpeng; Ni, Zhenhua; Wang, Jinlan; Chen, Qian; Lu, Jiong; Li, Zejun Near-100% spontaneous rolling up of polar van der Waals materials NATURE MATERIALS, 24 (11), 2025, DOI: 10.1038/s41563-025-02357-w. @article{WOS:001592760400001, title = {Near-100% spontaneous rolling up of polar van der Waals materials}, author = {Zhi Zhang and Yuwei Zhang and Kangjun Lu and Jun-Jie Zhang and Nannan Zhang and Rui Feng and Haoran Ye and Xiaoli Zhou and Linglong Li and Dongyang Wan and Junpeng Lu and Zhenhua Ni and Jinlan Wang and Qian Chen and Jiong Lu and Zejun Li}, doi = {10.1038/s41563-025-02357-w}, times_cited = {0}, issn = {1476-1122}, year = {2025}, date = {2025-11-01}, journal = {NATURE MATERIALS}, volume = {24}, number = {11}, publisher = {NATURE PORTFOLIO}, address = {HEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY}, abstract = {Rolling two-dimensional materials into one-dimensional nanoscrolls introduces curvature, chirality and symmetry breaking, enabling emergent properties. Conventional methods relying on external driving forces, however, exhibit poor control, low yield and limited reproducibility. Here we report spontaneous scrolling in polar van der Waals materials via an electrochemical intercalation/exfoliation process, enabling scalable nanoscroll production. This self-rolling is driven intrinsically by out-of-plane electric polarization (P-perpendicular to), where the magnitude of P-perpendicular to is modulated by the intercalant size. Validated across eight polar materials, this approach achieves virtually 100% yield and reproducibility with defined scrolling direction, surpassing external driving force limitations. The nanoscrolls exhibit layer-independent inversion symmetry breaking and coherently enhanced second-harmonic generation, exceeding two-dimensional flakes by similar to 100-fold and rivalling leading two-dimensional nonlinear materials. Electrochemical initiation further facilitates metal-ion co-intercalation, yielding ten hybrid nanoscroll architectures. These findings establish a scalable route to create one-dimensional nanostructures and hybrid heterostructures, paving the way for designer quantum solids and van der Waals superlattices in quantum nanodevices.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Rolling two-dimensional materials into one-dimensional nanoscrolls introduces curvature, chirality and symmetry breaking, enabling emergent properties. Conventional methods relying on external driving forces, however, exhibit poor control, low yield and limited reproducibility. Here we report spontaneous scrolling in polar van der Waals materials via an electrochemical intercalation/exfoliation process, enabling scalable nanoscroll production. This self-rolling is driven intrinsically by out-of-plane electric polarization (P-perpendicular to), where the magnitude of P-perpendicular to is modulated by the intercalant size. Validated across eight polar materials, this approach achieves virtually 100% yield and reproducibility with defined scrolling direction, surpassing external driving force limitations. The nanoscrolls exhibit layer-independent inversion symmetry breaking and coherently enhanced second-harmonic generation, exceeding two-dimensional flakes by similar to 100-fold and rivalling leading two-dimensional nonlinear materials. Electrochemical initiation further facilitates metal-ion co-intercalation, yielding ten hybrid nanoscroll architectures. These findings establish a scalable route to create one-dimensional nanostructures and hybrid heterostructures, paving the way for designer quantum solids and van der Waals superlattices in quantum nanodevices.
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Xuan, Dalong; Wu, Di'an; Geng, Xiaobin; Li, Sihao; Wu, Xianglong; Wang, Yu; Zhang, Xue Quantum coherence and relaxation of single spins on surfaces probed by ESR-STM NANOSCALE, 17 (45), pp. 26024-26032, 2025, DOI: 10.1039/d5nr03773e. @article{WOS:001607645200001, title = {Quantum coherence and relaxation of single spins on surfaces probed by ESR-STM}, author = {Dalong Xuan and Di'an Wu and Xiaobin Geng and Sihao Li and Xianglong Wu and Yu Wang and Xue Zhang}, doi = {10.1039/d5nr03773e}, times_cited = {0}, issn = {2040-3364}, year = {2025}, date = {2025-11-01}, journal = {NANOSCALE}, volume = {17}, number = {45}, pages = {26024-26032}, publisher = {ROYAL SOC CHEMISTRY}, address = {THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND}, abstract = {The miniaturization of modern devices to the nanoscale has inspired the development of quantum information processing, in which quantum coherence is of vital importance for both fundamental research and applications. The integration of electron spin resonance with scanning tunneling microscopy (ESR-STM) has emerged as a powerful platform for atomic-scale quantum sensing, simulation and qubit operations on surfaces. However, the qubit lifetime faces significant challenges due to environmental perturbations in STM circuits, whose underlying mechanisms require a deep and comprehensive understanding. This minireview summarizes recent advances in studying spin coherence using ESR-STM, focusing on the fundamental decoherence pathways including scattering and tunneling electrons and magnetic perturbations near the tunnel junction. By elucidating the microscopic origins of decoherence in atomic and molecular spin systems on surfaces, we provide a framework for developing targeted strategies to enhance the quantum coherence of spin qubits on surfaces.}, keywords = {}, pubstate = {published}, tppubtype = {article} } The miniaturization of modern devices to the nanoscale has inspired the development of quantum information processing, in which quantum coherence is of vital importance for both fundamental research and applications. The integration of electron spin resonance with scanning tunneling microscopy (ESR-STM) has emerged as a powerful platform for atomic-scale quantum sensing, simulation and qubit operations on surfaces. However, the qubit lifetime faces significant challenges due to environmental perturbations in STM circuits, whose underlying mechanisms require a deep and comprehensive understanding. This minireview summarizes recent advances in studying spin coherence using ESR-STM, focusing on the fundamental decoherence pathways including scattering and tunneling electrons and magnetic perturbations near the tunnel junction. By elucidating the microscopic origins of decoherence in atomic and molecular spin systems on surfaces, we provide a framework for developing targeted strategies to enhance the quantum coherence of spin qubits on surfaces.
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Yu, Wen; Xia, Shengpeng; Zhang, Miaomiao; Gao, Zhiqiang; Lv, Fengting; Huang, Yiming; Bai, Haotian; Bazan, Guillermo C; Wang, Shu Recent Advances of Conjugated Polymers-Based Biohybrid Systems for the Synthesis of Value-Added Chemicals CCS CHEMISTRY, 2025, DOI: 10.31635/ccschem.025.202506431. @article{WOS:001611972700001, title = {Recent Advances of Conjugated Polymers-Based Biohybrid Systems for the Synthesis of Value-Added Chemicals}, author = {Wen Yu and Shengpeng Xia and Miaomiao Zhang and Zhiqiang Gao and Fengting Lv and Yiming Huang and Haotian Bai and Guillermo C Bazan and Shu Wang}, doi = {10.31635/ccschem.025.202506431}, times_cited = {0}, year = {2025}, date = {2025-11-01}, journal = {CCS CHEMISTRY}, publisher = {CHINESE CHEMICAL SOC}, address = {C/O DEPT INT AFFAIRS, SECRETARY OF CHEM SOC, PO BOX 2709, BEIJING 100080, PEOPLES R CHINA}, abstract = {Conjugated polymers (CPs) have garnered considerable attention for biohybrid systems due to their intrinsic biocompatibility, superior light-harvesting and charge-separation capabilities, and tunable bioconductivity. This review outlines recent breakthroughs and emerging paradigms in CP-based biohybrid systems, specifically in the field of biosynthesis, which harness optical and electrical energy to generate chemical energy. We begin by surveying photosynthetic biohybrid system constructs that couple CPs with living microorganisms. In these systems, CPs generate photoactive electrons as ``light-trapping antennas'' to drive microbial synthetic pathways. Such platforms empower microorganisms to valorize CO2, N-2, and other simple substrates into renewable energy fuels and chemicals by utilizing light energy. Beyond solar-driven processes, electrosynthesis biohybrids offer an orthogonal yet equally sustainable strategy by leveraging renewable electricity. In electro-synthetic biohybrid systems, CPs act as electronic bridges that interface with electroactive microorganisms, significantly enhancing the interfacial electron transfer rate at the material-biological interface and thus boosting the efficiency of electricity-chemical conversion. In summary, these advances not only expand the functional repertoire of CP-based biohybrid systems but also inform rational design principles aimed at realizing scalable, sustainable, and programmable biosynthetic platforms ideas to promote their industrial synthesis of chemicals powered by solar and electrical inputs.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Conjugated polymers (CPs) have garnered considerable attention for biohybrid systems due to their intrinsic biocompatibility, superior light-harvesting and charge-separation capabilities, and tunable bioconductivity. This review outlines recent breakthroughs and emerging paradigms in CP-based biohybrid systems, specifically in the field of biosynthesis, which harness optical and electrical energy to generate chemical energy. We begin by surveying photosynthetic biohybrid system constructs that couple CPs with living microorganisms. In these systems, CPs generate photoactive electrons as ``light-trapping antennas'' to drive microbial synthetic pathways. Such platforms empower microorganisms to valorize CO2, N-2, and other simple substrates into renewable energy fuels and chemicals by utilizing light energy. Beyond solar-driven processes, electrosynthesis biohybrids offer an orthogonal yet equally sustainable strategy by leveraging renewable electricity. In electro-synthetic biohybrid systems, CPs act as electronic bridges that interface with electroactive microorganisms, significantly enhancing the interfacial electron transfer rate at the material-biological interface and thus boosting the efficiency of electricity-chemical conversion. In summary, these advances not only expand the functional repertoire of CP-based biohybrid systems but also inform rational design principles aimed at realizing scalable, sustainable, and programmable biosynthetic platforms ideas to promote their industrial synthesis of chemicals powered by solar and electrical inputs.
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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 ACS NANO, 19 (43), pp. 38040-38052, 2025, DOI: 10.1021/acsnano.5c13278. @article{WOS: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 = {2025-11-01}, 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.
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Zhou, Shengmin; Liu, Jiaxi; Xia, Yongpeng; Chu, Hailiang; Pan, Hongge; Xu, Fen; Sun, Lixian; Novoselov, Kostya S; Huang, Pengru Size effects in close-to-atomic scale synthesis of NaBH4 and NaBO2 nanoparticles for reversible hydrogen storage JOURNAL OF ALLOYS AND COMPOUNDS, 1046 , 2025, DOI: 10.1016/j.jallcom.2025.184727. @article{WOS:001616125900022, title = {Size effects in close-to-atomic scale synthesis of NaBH4 and NaBO2 nanoparticles for reversible hydrogen storage}, author = {Shengmin Zhou and Jiaxi Liu and Yongpeng Xia and Hailiang Chu and Hongge Pan and Fen Xu and Lixian Sun and Kostya S Novoselov and Pengru Huang}, doi = {10.1016/j.jallcom.2025.184727}, times_cited = {0}, issn = {0925-8388}, year = {2025}, date = {2025-11-01}, journal = {JOURNAL OF ALLOYS AND COMPOUNDS}, volume = {1046}, publisher = {ELSEVIER SCIENCE SA}, address = {PO BOX 564, 1001 LAUSANNE, SWITZERLAND}, abstract = {Sodium borohydride (NaBH4) is a promising solid-state hydrogen storage material for portable applications due to its reversible hydrogen release and uptake. However, its practical deployment is limited by low hydrogen generation yields and the high cost of regeneration. Nanoscale synthesis has emerged as an effective approach to increase surface-to-volume ratios and exploit size-dependent effects, thereby lowering thermodynamic and kinetic barriers and enhancing reversibility. In this study, we systematically investigate the size effects of both NaBH4 and its hydrolysis product, sodium metaborate (NaBO2). Thickness-dependent stabilities, electronic structures, and hydrogenation/dehydrogenation behaviors are examined in detail. Our results reveal an intrinsic dilemma: nanosizing significantly reduces the thermodynamic barrier for NaBH4 oxidation and NaBO2 reduction, thereby facilitating reversible hydrogen cycling, but simultaneously destabilizes the nanosheets, posing challenges for their synthesis. By interfacing nanosheets with metal substrates, we show that the improved thermodynamic properties can be retained while stability is markedly enhanced. These findings provide fundamental insights and design principles for nanoscale engineering of reversible hydrogen storage materials.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Sodium borohydride (NaBH4) is a promising solid-state hydrogen storage material for portable applications due to its reversible hydrogen release and uptake. However, its practical deployment is limited by low hydrogen generation yields and the high cost of regeneration. Nanoscale synthesis has emerged as an effective approach to increase surface-to-volume ratios and exploit size-dependent effects, thereby lowering thermodynamic and kinetic barriers and enhancing reversibility. In this study, we systematically investigate the size effects of both NaBH4 and its hydrolysis product, sodium metaborate (NaBO2). Thickness-dependent stabilities, electronic structures, and hydrogenation/dehydrogenation behaviors are examined in detail. Our results reveal an intrinsic dilemma: nanosizing significantly reduces the thermodynamic barrier for NaBH4 oxidation and NaBO2 reduction, thereby facilitating reversible hydrogen cycling, but simultaneously destabilizes the nanosheets, posing challenges for their synthesis. By interfacing nanosheets with metal substrates, we show that the improved thermodynamic properties can be retained while stability is markedly enhanced. These findings provide fundamental insights and design principles for nanoscale engineering of reversible hydrogen storage materials.
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Mylnikov, Dmitry A; Safonov, Ilya V; Kashchenko, Mikhail A; Novoselov, Kostya S; Bandurin, Denis A; Chernov, Alexander I; Svintsov, Dmitry A Hysteresis-controlled Van der Waals tunneling infrared detector enabled by selective layer heating NPJ 2D MATERIALS AND APPLICATIONS, 9 (1), 2025, DOI: 10.1038/s41699-025-00612-x. @article{WOS:001613817900003, title = {Hysteresis-controlled Van der Waals tunneling infrared detector enabled by selective layer heating}, author = {Dmitry A Mylnikov and Ilya V Safonov and Mikhail A Kashchenko and Kostya S Novoselov and Denis A Bandurin and Alexander I Chernov and Dmitry A Svintsov}, doi = {10.1038/s41699-025-00612-x}, times_cited = {0}, year = {2025}, date = {2025-11-01}, journal = {NPJ 2D MATERIALS AND APPLICATIONS}, volume = {9}, number = {1}, publisher = {NATURE PORTFOLIO}, address = {HEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY}, abstract = {Mid-infrared (mid-IR) photodetectors play a crucial role in various applications, including the development of biomimetic vision systems that emulate neuronal function. In this work, we demonstrate a new infrared photodetector based on graphene/boron nitride/graphene tunneling heterostructure combining perception and memory functions. The detection principle is based on the shift of the N-shaped tunneling resonant feature in the I-V-curve upon infrared illumination. In the current-biased mode, such a shift results in a strong voltage ``jump'' (0.05-1 V) to another branch of the I-V-characteristic that persists after switching the radiation off. As a result, the structure can be considered as a visual neuron that combines perception and memory functions. More interestingly, the direction of voltage switching depends on laser beam position, adding extra recognition functionality to our perception device. The observed phenomena are explained within the theory of selective light-induced heating of electrons in the graphene layers, and the tunneling of hot carriers.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Mid-infrared (mid-IR) photodetectors play a crucial role in various applications, including the development of biomimetic vision systems that emulate neuronal function. In this work, we demonstrate a new infrared photodetector based on graphene/boron nitride/graphene tunneling heterostructure combining perception and memory functions. The detection principle is based on the shift of the N-shaped tunneling resonant feature in the I-V-curve upon infrared illumination. In the current-biased mode, such a shift results in a strong voltage ``jump'' (0.05-1 V) to another branch of the I-V-characteristic that persists after switching the radiation off. As a result, the structure can be considered as a visual neuron that combines perception and memory functions. More interestingly, the direction of voltage switching depends on laser beam position, adding extra recognition functionality to our perception device. The observed phenomena are explained within the theory of selective light-induced heating of electrons in the graphene layers, and the tunneling of hot carriers.
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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 ADVANCED MATERIALS, 2025, DOI: 10.1002/adma.202510545. @article{WOS: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 = {2025-11-01}, journal = {ADVANCED MATERIALS}, 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.
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Liu, Yuqing; Dale, Stephen G; Sow, Chorng Haur; Gupta, Puneet; Lim, Sharon Xiaodai Constructing high-ionic-conductivity solid-state electrolytes with improved interface stability by rapid laser processing JOURNAL OF ENERGY CHEMISTRY, 110 , pp. 712-727, 2025, DOI: 10.1016/j.jechem.2025.06.062. @article{WOS:001543719900002, title = {Constructing high-ionic-conductivity solid-state electrolytes with improved interface stability by rapid laser processing}, author = {Yuqing Liu and Stephen G Dale and Chorng Haur Sow and Puneet Gupta and Sharon Xiaodai Lim}, doi = {10.1016/j.jechem.2025.06.062}, times_cited = {0}, issn = {2095-4956}, year = {2025}, date = {2025-11-01}, journal = {JOURNAL OF ENERGY CHEMISTRY}, volume = {110}, pages = {712-727}, publisher = {ELSEVIER}, address = {RADARWEG 29, 1043 NX AMSTERDAM, NETHERLANDS}, abstract = {All-solid-state batteries (ASSBs) with Li or Si anodes promise enhanced safety and high energy densities but face challenges with complex fabrication, stringent storage requirements, and pressure-dependent operation. Polyethylene oxide (PEO)-based composite solid electrolytes (CSEs) enable easy processing and flexible interfaces, supporting pressure-free operation and reducing costs. However, their low ionic conductivity remains a key limitation. Here, we present a rapid (similar to 5 min) and eco-friendly laser modification strategy for post-synthesized PEO CSEs, achieving enhanced ionic conductivity while retaining the attributes of simple fabrication and compatibility with Li and Si anodes under pressure-free operation. Laser engineering reduces PEO crystallinity, introduces additional Li* coordination sites, and improves interfacial stability through tailored solid electrolyte interphases. The laser-modified electrolyte enables LiFePO4//Li cells to retain 142.4 mAh g-1 after 800 cycles with 99.8 % Coulombic efficiency at 1 C and 60 degrees C. Moreover, without stack pressure, a Si anode paired with the laser-modified electrolyte delivers a high capacity of 1710.3 mAh g-1 with 56 % retention at 0.5 A g-1 after 50 cycles at 60 degrees C. Beyond performance enhancements, this work establishes a link between fluorescence emission and Li* transport in CSEs. Specifically, fluorescence shifts to shorter wavelengths correspond to shorter molecular chain lengths and lower coordination bonds, supported by time-dependent density functional theory calculations. These factors give rise to improved Li* transport. This optical probe offers a non-destructive approach for rapidly assessing electrolyte properties and enriching electrolyte design. Overall, this work demonstrates laser engineering as a practical post-synthetic strategy and highlights fluorescence as a practical indicator for advancing next-generation ASSBs. (c) 2025 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.}, keywords = {}, pubstate = {published}, tppubtype = {article} } All-solid-state batteries (ASSBs) with Li or Si anodes promise enhanced safety and high energy densities but face challenges with complex fabrication, stringent storage requirements, and pressure-dependent operation. Polyethylene oxide (PEO)-based composite solid electrolytes (CSEs) enable easy processing and flexible interfaces, supporting pressure-free operation and reducing costs. However, their low ionic conductivity remains a key limitation. Here, we present a rapid (similar to 5 min) and eco-friendly laser modification strategy for post-synthesized PEO CSEs, achieving enhanced ionic conductivity while retaining the attributes of simple fabrication and compatibility with Li and Si anodes under pressure-free operation. Laser engineering reduces PEO crystallinity, introduces additional Li* coordination sites, and improves interfacial stability through tailored solid electrolyte interphases. The laser-modified electrolyte enables LiFePO4//Li cells to retain 142.4 mAh g-1 after 800 cycles with 99.8 % Coulombic efficiency at 1 C and 60 degrees C. Moreover, without stack pressure, a Si anode paired with the laser-modified electrolyte delivers a high capacity of 1710.3 mAh g-1 with 56 % retention at 0.5 A g-1 after 50 cycles at 60 degrees C. Beyond performance enhancements, this work establishes a link between fluorescence emission and Li* transport in CSEs. Specifically, fluorescence shifts to shorter wavelengths correspond to shorter molecular chain lengths and lower coordination bonds, supported by time-dependent density functional theory calculations. These factors give rise to improved Li* transport. This optical probe offers a non-destructive approach for rapidly assessing electrolyte properties and enriching electrolyte design. Overall, this work demonstrates laser engineering as a practical post-synthetic strategy and highlights fluorescence as a practical indicator for advancing next-generation ASSBs. (c) 2025 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
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