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High mechanical strength Si anode synthesis with interlayer bonded expanded graphite structure for lithium-ion batteries
Authors:
Wenhui Lai,
Jong Hak Lee,
Lu Shi,
Yuqing Liu,
Yanhui Pu,
Yong Kang Ong,
Carlos Limpo,
Ting Xiong,
Yifan Rao,
Chorng Haur Sow,
Barbaros Özyilmaz
Abstract:
Despite advancements in silicon-based anodes for high-capacity lithium-ion batteries, their widespread commercial adoption is still hindered by significant volume expansion during cycling, especially at high active mass loadings crucial for practical use. The root of these challenges lies in the mechanical instability of the material, which subsequently leads to the structural failure of the elect…
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Despite advancements in silicon-based anodes for high-capacity lithium-ion batteries, their widespread commercial adoption is still hindered by significant volume expansion during cycling, especially at high active mass loadings crucial for practical use. The root of these challenges lies in the mechanical instability of the material, which subsequently leads to the structural failure of the electrode. Here, we present a novel synthesis of a composite combining expanded graphite and silicon nanoparticles. This composite features a unique interlayer-bonded graphite structure, achieved through the application of a modified spark plasma sintering method. Notably, this innovative structure not only facilitates efficient ion and electron transport but also provides exceptional mechanical strength (Vickers hardness: up to 658 MPa, Young's modulus: 11.6 GPa). This strength effectively accommodates silicon expansion, resulting in an impressive areal capacity of 2.9 mA h cm-2 (736 mA h g-1) and a steady cycle life (93% after 100 cycles). Such outstanding performance is paired with features appropriate for large-scale industrial production of silicon batteries, such as active mass loading of at least 3.9 mg cm-2, a high-tap density electrode material of 1.68 g cm-3 (secondary clusters: 1.12 g cm-3), and a production yield of up to 1 kg per day.
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Submitted 25 June, 2025;
originally announced June 2025.
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Enabling microrobotic chemotaxis via reset-free hierarchical reinforcement learning
Authors:
Tongzhao Xiong,
Zhaorong Liu,
Chong Jin Ong,
Lailai Zhu
Abstract:
Microorganisms have evolved diverse strategies to propel in viscous fluids, navigate complex environments, and exhibit taxis in response to stimuli. This has inspired the development of synthetic microrobots, where machine learning (ML) is playing an increasingly important role. Can ML endow these robots with intelligence resembling that developed by their natural counterparts over evolutionary ti…
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Microorganisms have evolved diverse strategies to propel in viscous fluids, navigate complex environments, and exhibit taxis in response to stimuli. This has inspired the development of synthetic microrobots, where machine learning (ML) is playing an increasingly important role. Can ML endow these robots with intelligence resembling that developed by their natural counterparts over evolutionary timelines? Here, we demonstrate chemotactic navigation of a multi-link articulated microrobot using two-level hierarchical reinforcement learning (RL). The lower-level RL allows the robot -- featuring either a chain or ring topology -- to acquire topology-specific swimming gaits: wave propagation characteristic of flagella or body oscillation akin to an ameboid. Such flagellar and ameboid microswimmers, further enabled by the higher-level RL, accomplish chemotactic navigation in prototypical biologically-relevant scenarios that feature conflicting chemoattractants, pursuing a swimming bacterial mimic, steering in vortical flows, and squeezing through tight constrictions. Additionally, we achieve reset-free, partially observable RL, where the robot observes only its joint angles and local scalar quantities. This advancement illuminates solutions for overcoming the persistent challenges of manual resets and partial observability in real-world microrobotic RL.
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Submitted 14 August, 2024;
originally announced August 2024.
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Distinguishing the importance of different charge trapping centers in CaF2-based 2D material MOSFETs
Authors:
Zhe Zhao,
Tao Xiong,
Jian Gong,
Yue-Yang Liu
Abstract:
Crystalline CaF2 is drawing huge attentions due to its great potential of being the gate dielectric of two-dimensional (2D) material MOSFETs. It is deemed to be much superior than boron nitride and traditional SiO2 because of its larger dielectric constant, wider band gap, and lower defect density. Nevertheless, the CaF2-based MOSFETs fabricated in experiment still present notable reliability issu…
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Crystalline CaF2 is drawing huge attentions due to its great potential of being the gate dielectric of two-dimensional (2D) material MOSFETs. It is deemed to be much superior than boron nitride and traditional SiO2 because of its larger dielectric constant, wider band gap, and lower defect density. Nevertheless, the CaF2-based MOSFETs fabricated in experiment still present notable reliability issues, and the underlying reason remains unclear. Here we studied the various intrinsic defects and adsorbates in CaF2/MoS2 and CaF2/MoSi2N4 interface systems to reveal the most active charge trapping centers in CaF2-based 2D material MOSFETs. An elaborate Table that comparing the importance of different defects in both n-type and p-type device is provided. Most impressively, the oxygen molecules adsorbed at the interface or surface, which are inevitable in experiments, are as active as the intrinsic defects in channel materials, and they can even change the MoSi2N4 to p-type spontaneously. These results mean that it is necessary to develop high vacuum packaging process as well as preparing high-quality 2D materials for better device performance.
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Submitted 12 September, 2023;
originally announced September 2023.
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Nanoconfinement of Tetraphenylethylene in Zeolitic Metal-Organic Framework for Turn-on Mechanofluorochromic Stress Sensing
Authors:
Yang Zhang,
Tao Xiong,
Annika F. Möslein,
Samraj Mollick,
Vishal Kachwal,
Arun Singh Babal,
Jin-Chong Tan
Abstract:
Mechanofluorochromic materials are of great significance for the fabrication of innovative sensors and optoelectronics. However, efficient mechanofluorochromic materials are rarely explored due to the deficiency of existing design strategies. Here, we demonstrate the incarceration of aggregation-induced emission (AIE) materials within metal-organic framework (MOF) single crystals to construct a co…
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Mechanofluorochromic materials are of great significance for the fabrication of innovative sensors and optoelectronics. However, efficient mechanofluorochromic materials are rarely explored due to the deficiency of existing design strategies. Here, we demonstrate the incarceration of aggregation-induced emission (AIE) materials within metal-organic framework (MOF) single crystals to construct a composite system with turn-on mechanofluorochromism. A new type of AIE@MOF material was designed: integrating a zeolitic MOF (ZIF-71) and tetraphenylethylene (TPE, a topical AIE material) to generate a TPE@ZIF-71 system with exceptional turn-on type mechanofluorochromism. Using terahertz vibrational spectroscopy, we show the unique fluorochromism emanates from the enhanced nanoconfinement effect exerted by ZIF-71 host on TPE guest under pressure and its permanent fluorescence after stress release. Compared with pure TPE, we demonstrate the nanoconfinement in AIE@MOF not only changes the TPE's turn-off type sensing behavior to a turn-on type, but boosts the original sensitivity markedly by tenfold. Significantly, because ZIF-71 prevents the spontaneous recrystallization of TPE upon unloading, this allows TPE@ZIF-71 to record the stress history. This is the first demonstration of the Guest@MOF system combining the concepts of AIE and MOF; its promising properties and potential engineering applications will stimulate new directions pertaining to luminescent stress sensors and smart optics.
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Submitted 21 November, 2021;
originally announced November 2021.
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Tunable Fluorescein-Encapsulated Zeolitic Imidazolate Framework-8 Nanoparticles for Solid-State Lighting
Authors:
Tao Xiong,
Yang Zhang,
Lorenzo Donà,
Mario Gutiérrez,
Annika F. Möslein,
Arun S. Babal,
Nader Amin,
Bartolomeo Civalleri,
Jin-Chong Tan
Abstract:
A series of fluorescein-encapsulated zeolitic imidazolate framework-8 (fluorescein@ZIF-8) luminescent nanoparticles with a scalable guest loading has been fabricated and characterized. The successful encapsulation of the organic dye (fluorescein) is supported by both experimental evidence and theoretical simulations. The measured optical band gap is found to be comparable with the computed values…
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A series of fluorescein-encapsulated zeolitic imidazolate framework-8 (fluorescein@ZIF-8) luminescent nanoparticles with a scalable guest loading has been fabricated and characterized. The successful encapsulation of the organic dye (fluorescein) is supported by both experimental evidence and theoretical simulations. The measured optical band gap is found to be comparable with the computed values of a hypothetical guest-host system. Isolated monomers and aggregates species of fluorescein confined in ZIF-8 nanocrystals have been systematically investigated through fluorescence lifetime spectroscopy. The quantum yield (QY) of the obtained solid-state materials is particularly high (QY~98%), especially when the concentration of the fluorescein guest is low. Combining a blue LED chip and a thin photoactive film of fluorescein@ZIF-8, we demonstrate a device with good optical tunability for multicolor and white light emissions. Additionally, we show that the fluorescein@ZIF-8 nanoparticles exhibit an improved photostability due to the shielding effect conferred by the nanoconfinement of host framework, making them promising candidates for practical applications such as solid-state lighting, photonics, and optical communications.
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Submitted 24 September, 2021;
originally announced September 2021.
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Characterizing Random-singlet State in Two-dimensional Frustrated Quantum Magnets and Implications for the Double Perovskite Sr$_2$CuTe$_{1-x}$W$_{x}$O$_6$
Authors:
Huan-Da Ren,
Tian-Yu Xiong,
Han-Qing Wu,
D. N. Sheng,
Shou-Shu Gong
Abstract:
Motivated by experimental observation of the non-magnetic phase in the compounds with frustration and disorder, we study the ground state of the spin-$1/2$ square-lattice Heisenberg model with randomly distributed nearest-neighbor $J_1$ and next-nearest-neighbor $J_2$ couplings. By using the density matrix renormalization group (DMRG) calculation on cylinder system with circumference up to $10$ la…
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Motivated by experimental observation of the non-magnetic phase in the compounds with frustration and disorder, we study the ground state of the spin-$1/2$ square-lattice Heisenberg model with randomly distributed nearest-neighbor $J_1$ and next-nearest-neighbor $J_2$ couplings. By using the density matrix renormalization group (DMRG) calculation on cylinder system with circumference up to $10$ lattice sites, we identify a disordered phase between the Néel and stripe magnetic phase with growing $J_2 / J_1$ in the presence of strong bond randomness. The vanished spin-freezing parameter indicates the absence of spin glass order. The large-scale DMRG results unveil the size-scaling behaviors of the spin-freezing parameter, the power-law decay of the average spin correlation, and the exponential decay of the typical spin correlation, which all agree with the corresponding behavior in the one-dimensional random singlet (RS) state and characterize the RS nature of this disordered phase. The DMRG simulation also provides insights and opportunities for characterizing a class of non-magnetic states in two-dimensional frustrated magnets with disorder. We also compare with existing experiments and suggest more measurements for understanding the spin-liquid-like behaviors in the double perovskite Sr$_2$CuTe$_{1-x}$W$_{x}$O$_6$.
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Submitted 20 January, 2023; v1 submitted 5 April, 2020;
originally announced April 2020.
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Floquet engineering to exotic topological phases in systems of cold atoms
Authors:
Hui Liu,
Tian-Shi Xiong,
Wei Zhang,
Jun-Hong An
Abstract:
Topological phases with a widely tunable number of edge modes have been extensively studied as a typical class of exotic states of matter with potentially important applications. Although several models have been shown to support such phases, they are not easy to realize in solid-state systems due to the complexity of various intervening factors. Inspired by the realization of synthetic spin-orbit…
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Topological phases with a widely tunable number of edge modes have been extensively studied as a typical class of exotic states of matter with potentially important applications. Although several models have been shown to support such phases, they are not easy to realize in solid-state systems due to the complexity of various intervening factors. Inspired by the realization of synthetic spin-orbit coupling in a cold-atom system [Z. Wu {\it et al.}, Science \textbf{354}, 83 (2016)], we propose a periodic quenching scheme to realize large-topological-number phases with multiple edge modes in optical lattices. Via introducing the periodic quenching to the Raman lattice, it is found that a large number of edge modes can be induced in a controllable manner from the static topologically trivial system. Our result provides an experimentally accessible method to artificially synthesize and manipulate exotic topological phases with large topological numbers and multiple edge modes.
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Submitted 26 August, 2019; v1 submitted 31 March, 2019;
originally announced April 2019.
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Effect of aging-induced disorder on the quantum transport properties of atomically thin WTe$_{2}$
Authors:
W. L. Liu,
M. L. Chen,
X. X. Li,
S. Dubey,
T. Xiong,
Z. M. Dai,
J. Yin,
W. L. Guo,
J. L. Ma,
Y. N. Chen,
J. Tan,
D. Li,
Z. H. Wang,
W. Li,
V. Bouchiat,
D. M. Sun,
Z. Han,
Z. D. Zhang
Abstract:
Atomically thin layers of transition-metal dicalcogenides (TMDCs) are often known to be metastable in the ambient atmosphere. Understanding the mechanism of degradation is essential for their future applications in nanoelectronics, and thus has attracted intensive interest recently. Here, we demonstrate a systematic study of atomically thin WTe$_{2}$ in its low temperature quantum electronic trans…
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Atomically thin layers of transition-metal dicalcogenides (TMDCs) are often known to be metastable in the ambient atmosphere. Understanding the mechanism of degradation is essential for their future applications in nanoelectronics, and thus has attracted intensive interest recently. Here, we demonstrate a systematic study of atomically thin WTe$_{2}$ in its low temperature quantum electronic transport properties. Strikingly, while the temperature dependence of few layered WTe$_{2}$ showed clear metallic tendency in the fresh state, degraded devices first exhibited a re-entrant insulating behavior, and finally entered a fully insulating state. Correspondingly, a crossover from parabolic to linear magnetoresistance, and finally to weak anti-localization was seen. Real-time Raman scattering measurement, together with transmission electron microscopy studies done before and after air degradation of atomically thin WTe$_{2}$ further confirmed that the material gradually form amorphous islands. It thus leads to localized electronic states and explains the low temperature Coulomb gap observed in transport measurements. Our study reveals for the first time the correlation between the unusual magnetotransport and disorder in few-layered WTe$_{2}$, which is indispensable in providing guidance on its future devices application.
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Submitted 16 August, 2016;
originally announced August 2016.
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Towards large-Chern-number topological phases by periodic quenching
Authors:
Tian-Shi Xiong,
Jiangbin Gong,
Jun-Hong An
Abstract:
Topological phases with large Chern numbers have important implications. They were previously predicted to exist by considering fabricated long-range interactions or multi-layered materials. Stimulated by recent wide interests in Floquet topological phases, here we propose a scheme to engineer large-Chern-number phases with ease by periodic quenching. Using a two-band system as an example, we theo…
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Topological phases with large Chern numbers have important implications. They were previously predicted to exist by considering fabricated long-range interactions or multi-layered materials. Stimulated by recent wide interests in Floquet topological phases, here we propose a scheme to engineer large-Chern-number phases with ease by periodic quenching. Using a two-band system as an example, we theoretically show how a variety of topological phases with widely tunable Chern numbers can be generated by periodic quenching between two simple Hamiltonians that otherwise give low Chern numbers. The obtained large Chern numbers are explained through the emergence of multiple Dirac cones in the Floquet spectra. The transition lines between different topological phases in the two-band model are also explicitly found, thus establishing a class of easily solvable but very rich systems useful for further understandings and applications of topological phases in periodically driven systems.
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Submitted 31 May, 2016; v1 submitted 18 January, 2016;
originally announced January 2016.