Materials Today Physics最新文献

{"title":"Diamond tin-vacancy centers: From synthesis and characterization to quantum photonic applications – a comprehensive review","authors":"Mariusz Banasiak,&nbsp;Mattia Pierpaoli,&nbsp;Robert Bogdanowicz","doi":"10.1016/j.mtphys.2026.102088","DOIUrl":"10.1016/j.mtphys.2026.102088","url":null,"abstract":"<div><div>The development of quantum information technologies relies critically on identifying solid-state platforms with controllable quantum states and coherent optical interfaces. Diamond color centers, particularly group-IV element-related defects, have emerged as promising candidates for quantum bit implementations and single-photon sources. Among these, tin-vacancy (SnV) centers have garnered significant attention due to their exceptional spectroscopic properties, including narrow emission linewidths, reduced phonon coupling, and operation at accessible cryogenic temperatures (∼4 K) compared to silicon-vacancy counterparts that require millikelvin cooling. This review provides a comprehensive analysis of SnV centers in diamond, elucidating formation mechanisms, electronic structure characteristics, and optoelectronic property modulation strategies. We examine various synthesis methodologies—high-pressure high-temperature (HPHT) growth, chemical vapor deposition (CVD), and ion implantation—critically evaluating their respective advantages and limitations for controlled SnV creation. The distinctive split-vacancy configuration, resulting from tin's large atomic radius, confers D_3d inversion symmetry, which provides intrinsic protection against electric field noise, enabling transform-limited optical linewidths. We also review SnV spectroscopic responses to external electromagnetic field perturbations, demonstrating that controlled Stark-effect tuning requires exceptionally high field strengths due to this symmetry protection, while magnetic fields induce complex Zeeman splitting for quantum state manipulation. The temporal dynamics parameters (T₁ optical and spin relaxation, T₂ spin coherence times) are systematically compared with other diamond color centers, establishing quantitative benchmarks for quantum information applications. Finally, we identify critical challenges and promising research directions for enhancing SnV center performance in next-generation quantum photonic devices.</div></div>","PeriodicalId":18253,"journal":{"name":"Materials Today Physics","volume":"63 ","pages":"Article 102088"},"PeriodicalIF":9.7,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147519140","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Charge relaxation and boundary reactions jointly drive ultralong cycle life in electric double-layer capacitors","authors":"Zeyu Song ,&nbsp;Kuan Sun ,&nbsp;Yongguang Tu ,&nbsp;Jihuai Wu","doi":"10.1016/j.mtphys.2026.102083","DOIUrl":"10.1016/j.mtphys.2026.102083","url":null,"abstract":"<div><div>Electric double-layer capacitors (EDLCs) exhibit ultralong cycle life (&gt;10,000 cycles) due to the chemical inertness of carbon electrodes. However, the fundamental mechanism governing their potential evolution during cycling remains poorly understood. Here, we establish a device charge-discharge model and monitor the potential changes of both positive and negative electrodes during cycling using an auxiliary voltage division system (AVDS). We demonstrate that, regardless of the initial electrode potential (−0.4 V, −0.6 V, or −0.8 V vs. Hg/HgO), the positive and negative electrode potentials spontaneously converge to stable values (V ⁺ _max ≈ −0.019 V, V⁻_min ≈ −1.019 V) within 10 cycles. This self-stabilization arises from the antagonistic interplay between the charge relaxation effect—which reduces the apparent specific capacitance by ∼23% compared to single-electrode measurements—and the boundary constraints imposed by irreversible oxidation-reduction reactions. Remarkably, stable cycling is achieved with Coulombic efficiency at ∼97%, challenging the conventional paradigm that 100% efficiency is necessary for long-term stability. Our findings provide quantitative design principles for optimizing long-life EDLC devices.</div></div>","PeriodicalId":18253,"journal":{"name":"Materials Today Physics","volume":"63 ","pages":"Article 102083"},"PeriodicalIF":9.7,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147524013","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Nanofiber yarn strain sensor with interpenetrating 3D MXene network via conjugated electrospinning and deep deposition","authors":"Binghui Wang ,&nbsp;Zhiye Qiu ,&nbsp;Yuxin Wei ,&nbsp;Mengzheng Wang ,&nbsp;Tianming Lu ,&nbsp;Liuxie Huang ,&nbsp;Qiaoqing Hu ,&nbsp;Jindan Wu","doi":"10.1016/j.mtphys.2026.102086","DOIUrl":"10.1016/j.mtphys.2026.102086","url":null,"abstract":"<div><div>Driven by the growing demand for human-machine interaction and smart health monitoring, one-dimensional flexible strain sensors have attracted considerable interest due to their excellent flexibility and compatibility with textile integration. However, conventional sensors based on surface conductive coatings are often hindered by poor interfacial adhesion, inadequate environmental stability, and slow response dynamics. To address these challenges, this study proposes a “deep deposition” strategy to construct polyamide/polyvinyl alcohol (PA/PVA) nanofiber yarns (MPPY) featuring an internal three-dimensional interconnected conductive network via conjugated electrospinning. By precisely tuning the PA/PVA flow ratio, the yarn composition and porosity were tailored, while the intrinsic hydrophilicity of PVA facilitated full cross-sectional infiltration of MXene nanosheets. Subsequent twisting and plying further enhanced mechanical robustness and conductivity uniformity, yielding a three-ply yarn that was then incorporated into elastic fabrics via embroidery for customizable patterning. The resulting yarns exhibited an ultrafast response time (58 ± 2 ms at 10% strain) and demonstrated remarkable sensitivity across multiple strain regimes, with gauge factor values of 1.82 (0–50% strain), 9.71 (50–80% strain), and 22.93 (100% strain), while maintaining a coefficient (R²) above 0.98 throughout. The yarn-integrated textile demonstrated outstanding durability, withstanding over 6000 stretching-releasing cycles at 50% strain, along with excellent washability, and resistance to corrosion in artificial sweat. By implementing patterned configurations (e.g., straight-line and serpentine-line), the fabric sensor facilitated real-time and precise monitoring of multi-joint human motions, including those of the neck, wrist, spine, and knee. This study provides a novel design pathway toward next-generation wearable electronic textiles with high reliability, fast response, and practical versatility.</div></div>","PeriodicalId":18253,"journal":{"name":"Materials Today Physics","volume":"63 ","pages":"Article 102086"},"PeriodicalIF":9.7,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147524014","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"High-performance SnTe-based thermoelectric materials driven by band convergence and lattice softening via CuSbS2 alloying and Cd doping","authors":"Chenyue Sun ,&nbsp;Jinbo Li ,&nbsp;Pengyuan Zhang ,&nbsp;Donglin Yuan ,&nbsp;Meichen Tian ,&nbsp;Hong Chen ,&nbsp;Muchun Guo ,&nbsp;Qinyong Zhang ,&nbsp;Yuke Zhu ,&nbsp;Ming Liu ,&nbsp;Jiehe Sui","doi":"10.1016/j.mtphys.2026.102093","DOIUrl":"10.1016/j.mtphys.2026.102093","url":null,"abstract":"<div><div>SnTe, as a lead-free analog of thermoelectric material PbTe, has garnered extensive attention for medium-temperature thermoelectric applications, yet its thermoelectric performance is severely hindered by high intrinsic carrier concentration, narrow band gap, and large lattice thermal conductivity. Herein, we report a two-step optimization strategy for SnTe, combining CuSbS₂ alloying and Cd doping to synergistically modulate its electronic and phonon transport properties. Electrically, CuSbS₂ alloying facilitates band convergence, which contributes to an enhanced density-of-states effective mass. Thermally, alloying weakens chemical bonding and induces ferroelectric instability, strengthening acoustic-optical phonon coupling and intensifying phonon scattering, thereby effectively suppressing the lattice thermal conductivity. Subsequent Cd doping further tailors the band structure, optimizes carrier concentration, and introduces additional point defects to enhance phonon scattering. As a result, the Sn_0.81Te_0.9Cd_0.09(CuSbS₂)_0.1 sample achieves a peak <em>ZT</em> of 1.0 at 773 K. This work highlights the critical role of chemical bond softening and ferroelectric instability induction in suppressing lattice thermal conductivity of chalcogenides.</div></div>","PeriodicalId":18253,"journal":{"name":"Materials Today Physics","volume":"63 ","pages":"Article 102093"},"PeriodicalIF":9.7,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147598071","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Ambient-pressure superconductivity in a hard ternary nitride VMgN2 achieved via element substitution","authors":"Lei Chen ,&nbsp;Mengyi Yun ,&nbsp;Hongbo Wen ,&nbsp;Tianyu Zhai ,&nbsp;Meiyan Li ,&nbsp;Zhenyi Jiang ,&nbsp;Junlian Xu ,&nbsp;Meiguang Zhang","doi":"10.1016/j.mtphys.2026.102090","DOIUrl":"10.1016/j.mtphys.2026.102090","url":null,"abstract":"<div><div>The exploration of ambient-pressure superconductors that simultaneously exhibit high critical temperatures (<em>T</em>_c) and high hardness is a fascinating topic in fundamental and experimental physics. In this work, through first-principles calculations combined with structure searches and elemental substitution, we predict a novel ternary hexagonal VMgN₂, which exhibits robust thermodynamic and dynamical stability up to 2000 K, a greatly boosted superconducting <em>T</em>_c of around 41 K at ambient pressure (compared to 7.5 K of binary VN), a high Vickers hardness of about 18 GPa. Substituting V for W in isostructural WMgN₂ induces a semiconductor-to-superconductor transition, mediated by a valence electron reduction that brings a van Hove singularity (VHS) near the Fermi level (<em>E</em>_F). Flat bands, primarily derived from V-<em>d</em> orbitals, together with Fermi surface nesting, give rise to a high density of states (DOS), which significantly enhances the electron-phonon coupling (EPC) strength between V-<em>d</em> orbitals and low-frequency phonon modes. Based on the Migdal–Eliashberg formalism, the calculated superconducting gap vanishes at 41 K under ambient pressure. Furthermore, electronic localization function (ELF) calculations confirm the presence of excess electrons localized in interstitial regions in WMgN₂, characteristic of an electride with interstitial anionic electrons (IAEs). In contrast, V-for-W substitution leads to the dissipation of these IAEs, indicating enhanced electron delocalization which thus likely underpins the emergent metallic behavior and superconductivity. <em>Ab initio</em> molecular dynamics (AIMD) simulations verify the thermal and dynamical stability of VMgN₂ at finite temperatures, demonstrating that its structure remains stable up to 2000 K. Owing to strong <em>p</em>-<em>d</em> and <em>p</em>-<em>p</em> hybridizations from V-N and Mg-N bonds, VMgN₂ also exhibits high Vickers hardness (18 GPa) and an ideal tensile strength exceeding 31.6 GPa. These results offer valuable insights into the coexistence mechanisms of superconductivity and superior mechanical properties of this newly discovered class of superconductors.</div></div>","PeriodicalId":18253,"journal":{"name":"Materials Today Physics","volume":"63 ","pages":"Article 102090"},"PeriodicalIF":9.7,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147598078","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Tuning of wide bandgap in Cs1-nFAnPbI2+xBr1-x perovskites via antisolvent free and dry processing approach for efficient and stable perovskite solar cells","authors":"Jyoti V. Patil ,&nbsp;Sawanta S. Mali ,&nbsp;Chang Kook Hong","doi":"10.1016/j.mtphys.2026.102078","DOIUrl":"10.1016/j.mtphys.2026.102078","url":null,"abstract":"<div><div>Wide bandgap (WBG) perovskites are crucial for tandem solar cell applications, where efficient light harvesting and thermal stability are essential. In this work, we present a novel strategy for tuning of WBG in Cs_1-nFA_nPbI_2+xBr_1-x perovskite by combining an antisolvent free hot air and a dry process method. Here, the bottom layer of the CsPbI₂Br is deposited using an antisolvent free hot air method, enabling uniform, thick films with followed by a dry processed FAPbI₃ top layer to modulate the halide and A-site cation composition, forming a compositionally tuned mixed WBG perovskite. The resulting mixed perovskite films through different film thickness of FAPbI₃ layer exhibit a tunable WBG in the range of ∼1.74 to 1.83 eV, which would be suitable for tandem solar cells fabrication. This mixed Cs_1-nFA_nPbI_2+xBr_1-x perovskite (target) device showed notable improvement in power conversion efficiency (PCE) of 18.26% and long-term operational stability compared to control CsPbI₂Br-based (13.15%) devices. This work highlights an alternative route for fine tuning of WBG perovskites with high performance and durability.</div></div>","PeriodicalId":18253,"journal":{"name":"Materials Today Physics","volume":"63 ","pages":"Article 102078"},"PeriodicalIF":9.7,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147506803","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Coexistence of analog and digital in MoS2-based memristor for memory and synaptic performance","authors":"Xiaoyi Lei ,&nbsp;Pengsheng Tian ,&nbsp;Chenghao Yang ,&nbsp;Jing Wang ,&nbsp;Jiahao Xue ,&nbsp;Xiaozhen Liang ,&nbsp;Wu Zhao","doi":"10.1016/j.mtphys.2026.102084","DOIUrl":"10.1016/j.mtphys.2026.102084","url":null,"abstract":"<div><div>Memristor is a prominent candidate for high-density digital data storage and analog neuromorphic computing. However, different application scenarios impose distinct requirements on device characteristics. In this work, we report the digital-to-analog conversion resistive switching behavior of Cu/MoS₂/ITO memristor under various forming stimuli. The mechanisms underlying the controllable coexistence of digital and analog modes in the device were investigated through electrical property analyses and temperature-dependent measurements. The synergistic regulation of Cu metallic filaments and sulfur vacancies governs the digital mode resistive switching. In contrast, the analog switching mode exhibits volatile semiconductor-like conductive properties, primarily dominated by variations in the MoS₂/ITO interface Schottky barrier. Furthermore, based on the digital switching characteristics of the device, we achieved five stable multi-level resistance states by adjusting the compliance current, thereby validating the multi-level storage capability of the device in digital mode. Additionally, by exploiting the analog switching properties of the Cu/MoS₂/ITO device, we explored its potential applications in optical and electrical synapses, as well as neural network computing, confirming the promising prospects of MoS₂-based memristor for in-memory computing architectures and the synaptic simulation field.</div></div>","PeriodicalId":18253,"journal":{"name":"Materials Today Physics","volume":"63 ","pages":"Article 102084"},"PeriodicalIF":9.7,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147524016","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Interface design of ZnO/Ti3C2Tx composite and study on its ammonia performance at room temperature","authors":"Zhipeng Li ,&nbsp;Xudong Li ,&nbsp;Hongyan Zhang ,&nbsp;Jie Ai ,&nbsp;Haiyang Zhang ,&nbsp;Chu Chen ,&nbsp;Ling Zhang","doi":"10.1016/j.mtphys.2026.102056","DOIUrl":"10.1016/j.mtphys.2026.102056","url":null,"abstract":"<div><div>A high-performance ammonia (NH₃) gas sensor based on ZnO/Ti₃C₂T_x composites was fabricated using the hydrothermal method. The gas sensitivity test results show that the composite of Ti₃C₂T_x and ZnO improves the sensing performance of Ti₃C₂T_x-based NH₃ sensor at room temperature. The response of ZnO/Ti₃C₂T_x to 200 ppm NH₃ is 158.7 and the response/recovery time is 3.6 s/0.9 s. Additionally, the sensor demonstrated excellent humidity resistance and long-term stability. This improvement is attributed to the introduction of additional free oxygen species and oxygen vacancies on the Ti₃C₂T_x surface by ZnO, exposing more active metallic Ti sites. Simultaneously, reducing the number of -OH groups increases the number of -F groups and enhances the polarity of the -OH groups. DFT studies indicate that higher surface oxygen vacancy density promotes the formation of highly active and unsaturated Ti sites, thereby enhancing strong chemical adsorption of NH₃. Concurrently, the reduction in -OH groups increases the polarity of -OH, thereby improving the adsorption efficiency of NH₃ molecules. Thus, modulating the Ti₃C₂T_x surface with metal oxides to reduce hydroxyl groups and increase oxygen vacancies promotes the formation of Ti metal sites, offering a novel approach for developing high-performance room-temperature NH₃ gas sensors based on Ti₃C₂T_x.</div></div>","PeriodicalId":18253,"journal":{"name":"Materials Today Physics","volume":"62 ","pages":"Article 102056"},"PeriodicalIF":9.7,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146778091","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Interfacial engineering of ultrathin π-π stacked conjugated coordination polymer/graphene heterostructures for nonlinear optics and ultrafast photonics","authors":"Yixin Ding ,&nbsp;Yue Kuai ,&nbsp;Heng Liu ,&nbsp;Caiyang Wang ,&nbsp;Yingtian Xu ,&nbsp;He Zhang ,&nbsp;Yunping Lan","doi":"10.1016/j.mtphys.2026.102065","DOIUrl":"10.1016/j.mtphys.2026.102065","url":null,"abstract":"<div><div>Two-dimensional (2D) π-conjugated coordination polymers (CCP) are of significant interest in various fields because of their excellent electrical conductivity, abundant active sites and porous structures. Nevertheless, their applications for ultrafast photonics and nonlinear optics still need to be further explored. The preparation of atomic-scale high-quality ultrathin CCP nanostructures remains a great challenge. Moreover, 2D van der Waals heterostructures (vdWhs) have attracted considerable attention owing to their unique photoelectric characteristics. Based on this, herein, two types of ultrathin CCP nanosheets of CuHHBNs and Cu₃(BHT)Ns (HHB = 1,2,3,4,5,6-hexahydroxy benzene, BHT = hexahydrophobic benzene) with the thickness of 4-6 nm are prepared via surfactant-assisted synthesis strategy. Then, the desirable π-π stacked ultrathin Cu₃(BHT)Ns/graphene and Cu-HHBNs/graphene organic-inorganic vdWhs (Cu₃(BHT)G-VHS and CuHHBG-VHS) are synthesized by ultrasonic-assisted method. Based on characterization analyses and theoretical simulations, because of the π-π stacking interactions between graphene and CCP, these ultrathin vdWhs display noticeable electron cloud extension, interfacial charge transfer and improved nonlinear optical (NLO) property. Ultimately, CuHHBG-VHS and Cu₃(BHT)G-VHS saturable absorbers reveal remarkable performance in ultrafast fiber laser. CuHHBG-VHS attains femtosecond fundamental mode-locking (FML) pulses and 14-order harmonic mode-locking (HML). Cu₃(BHT)G-VHS attains FML with pulse duration as short as 567 fs, and 48-order stabilized HML with GHz repetition frequency. The preferable performance of Cu₃(BHT)G-VHS is due to the larger π-conjugated system within Cu₃(BHT) structure, which may lead to stronger electron cloud extension and more charge transfer. This work offers new pathways toward CCP-based high-performance optoelectronic systems and ultrafast photonic applications.</div></div>","PeriodicalId":18253,"journal":{"name":"Materials Today Physics","volume":"62 ","pages":"Article 102065"},"PeriodicalIF":9.7,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147392480","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Mixed-alkali ion-exchange engineering enables fast-ion transport in Na1.5K1.5V2(PO4)2F3 fluorophosphate as a high-voltage cathode material for Na/K-ion batteries","authors":"Abdelghani Bensassi ,&nbsp;Abdelfattah Mahmoud ,&nbsp;Abdallah El Kenz ,&nbsp;Abdelilah Benyoussef ,&nbsp;Omar Mounkachi","doi":"10.1016/j.mtphys.2026.102059","DOIUrl":"10.1016/j.mtphys.2026.102059","url":null,"abstract":"<div><div>Mixed-alkali engineering offers a powerful strategy for enhancing the electrochemical performance of polyanionic cathodes in Na- and K-ion batteries. Here, we deliver a comprehensive multiscale computational investigation of Na₃V₂(PO₄)₂F₃ and its ion-exchanged mixed-alkali analogue Na_1.5K_1.5V₂(PO₄)₂F₃, revealing fundamental structure–property relationships that govern their electrochemical performance. The most stable phase configuration of Na_1.5K_1.5V₂(PO₄)₂F₃ emerges as the thermodynamic ground state, stabilizing an expanded yet mechanically robust NASICON-like VO₄/F₂–PO₄ lattice. K⁺ incorporation markedly narrows the band gap, enhancing electronic transport, while climbing-image nudged elastic band (CI-NEB) calculations show ultralow in-plane migration barriers of 0.211 eV (Na⁺) and 0.243 eV (K⁺), enabling diffusion coefficients near 10⁻⁷ cm² s⁻¹. Thermodynamic analysis uncovers a sequence of stable intermediate phases governing selective and dual-ion de-intercalation, giving rise to distinct voltage plateaus with average operating voltages of 3.22 V (Na⁺), 3.68 V (K⁺), and 4.17 V (Na⁺/K⁺). Notably, simultaneous Na⁺/K⁺ extraction leads to the achievement of a high theoretical capacity of 182 mAh g⁻¹ and an energy density of 759 Wh kg⁻¹ while maintaining small structural expansion. ab initio molecular dynamics (AIMD) simulations confirm exceptional thermal resilience across all charged states. These insights position ion-exchanged Na_1.5K_1.5V₂(PO₄)₂F₃ as a highly stable, high-voltage, and fast-ion-conducting mixed-alkali platform, advancing the design of next-generation Na-ion, K-ion, and hybrid Na/K-ion battery cathodes.</div></div>","PeriodicalId":18253,"journal":{"name":"Materials Today Physics","volume":"62 ","pages":"Article 102059"},"PeriodicalIF":9.7,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147278284","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}