Xinyang Zhang, Xinyang Ge, Jingya You, Yipu Wang, Qiang Huang and Li Wan
{"title":"Emerging chiral molecular carbon materials for chiroptoelectronic applications","authors":"Xinyang Zhang, Xinyang Ge, Jingya You, Yipu Wang, Qiang Huang and Li Wan","doi":"10.1039/D5TC02532J","DOIUrl":"https://doi.org/10.1039/D5TC02532J","url":null,"abstract":"<p >Chirality is a ubiquitous phenomenon in nature and continues to inspire modern materials science. Among various chiral systems, chiral carbon materials have been extensively developed, with their chirality flexibly tuned through molecular-level chemical design and further amplified by solid-state intermolecular assembly. By incorporating different functional groups, these carbon materials can be tailored to exhibit excellent light-emitting and light-absorbing properties, making their chiral forms suitable for emitting or detecting circularly polarized light. In this review, we first introduce the basic concepts of chiral materials and spectroscopic chiroptical responses, and explain how chirality is introduced into molecular carbon systems through chemical design. We then systematically summarize recent research progress in chiral optoelectronic (chiroptoelectronic) applications that incorporate chiral carbon materials. Furthermore, we analyze the dissymmetry factors of each system and offer perspectives on strategies to enhance performance. We believe that this review will attract broad attention from interdisciplinary researchers working on carbon materials, chirality science, and optoelectronics.</p>","PeriodicalId":84,"journal":{"name":"Journal of Materials Chemistry C","volume":" 40","pages":" 20444-20462"},"PeriodicalIF":5.1,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/tc/d5tc02532j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145315566","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Nathan Yee, Tyler Davidson-Hall, Neil Graddage, Barbara Martin, Jianying Ouyang, Philippe Berrouard and Jianping Lu
{"title":"Low bandgap conjugated polymers based on thiadiazoloquinoxaline for high performance shortwave infrared photodetection","authors":"Nathan Yee, Tyler Davidson-Hall, Neil Graddage, Barbara Martin, Jianying Ouyang, Philippe Berrouard and Jianping Lu","doi":"10.1039/D5TC02404H","DOIUrl":"https://doi.org/10.1039/D5TC02404H","url":null,"abstract":"<p >The detection of light in the second near-infrared (NIR-II) region of the electromagnetic spectrum is critical for various applications such as bioimaging, environmental sensing and health monitoring. However, the narrow band gaps of organic semiconductors required for NIR-II photodetection increase the probability of charge injection under bias voltages and bulk thermal charge generation in the active layer, leading to a large dark current and low external quantum efficiency which results in poor detectivity. In this study, we introduce a series of low band-gap donor–acceptor type alternating conjugated polymers using thiadiazoloquinoxaline (TQ) as electron-withdrawing units and indacenodithiophene (<strong>P1</strong> and <strong>P2</strong>) or propylenedioxythiophene as electron-donating units (<strong>P3–P5</strong>) for NIR-II photodetection. Polymers <strong>P3–P5</strong> have much lower band gaps than <strong>P1</strong> and <strong>P2</strong> due to the stronger intrachain D–A interaction in the former. <strong>P3</strong> and <strong>P5</strong> have excellent solubility in a variety of organic solvents even at room temperature, which greatly facilitates the device fabrication process. The photodiode device based on <strong>P5</strong> exhibited the highest specific detectivity of 2.0 × 10<small><sup>10</sup></small> Jones at 1200 nm under −1 V bias owing to the significantly low dark current.</p>","PeriodicalId":84,"journal":{"name":"Journal of Materials Chemistry C","volume":" 40","pages":" 20760-20768"},"PeriodicalIF":5.1,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/tc/d5tc02404h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145315611","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Kamila Lupinska, Kinga E. Szkaradek, Kacper Parafiniuk, Robert Góra, Piotr Fita, Yann Bretonnière, Chantal Andraud and Lech Sznitko
{"title":"Efficient optical photoswitching of benzyloxy-substituted TCF-based D–π–A molecules","authors":"Kamila Lupinska, Kinga E. Szkaradek, Kacper Parafiniuk, Robert Góra, Piotr Fita, Yann Bretonnière, Chantal Andraud and Lech Sznitko","doi":"10.1039/D5TC02366A","DOIUrl":"https://doi.org/10.1039/D5TC02366A","url":null,"abstract":"<p >Molecules exhibiting photo-switching behavior are essential for the development of various photonic and optoelectronic devices. In this study, we report the synthesis of five novel donor–π–acceptor organic dyes, in which a stilbene moiety serves as a π-linker between the electron-donating and electron-withdrawing units. To address the challenge of developing photo-switchable molecules responsive to visible light, we performed fundamental optical characterization in both solution and solid state. The photoisomerization capability was confirmed for all compounds through real-time absorption measurements, enabling the calculation of <em>E</em> → <em>Z</em> isomerization kinetics. The presence of both isomeric forms was further validated by <small><sup>1</sup></small>H NMR spectroscopy. These experimental findings were supported by quantum chemical calculations, which identified the most stable conformers and accurately predicted their spectral properties. Moreover, pump–probe experiments demonstrated that irradiation with linearly polarized light efficiently triggers photo-induced birefringence in dye-doped polymer systems, with a notable “memory effect” observed for all studied compounds. Remarkably, the dyes are highly sensitive to light, and the birefringence saturation can be achieved at light intensities comparable to natural daylight, highlighting their broad potential application in optoelectronic devices.</p>","PeriodicalId":84,"journal":{"name":"Journal of Materials Chemistry C","volume":" 40","pages":" 20519-20530"},"PeriodicalIF":5.1,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/tc/d5tc02366a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145315583","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Material-engineered self-compliant memristor enabling multibit synaptic learning and in-memory computing","authors":"Minseo Noh and Sungjun Kim","doi":"10.1039/D5TC02402A","DOIUrl":"https://doi.org/10.1039/D5TC02402A","url":null,"abstract":"<p >To improve the integration density of memristor-based crossbar arrays, we present a self-compliant RRAM device that eliminates the need for external current-limiting transistors. Additionally, an Al<small><sub>2</sub></small>O<small><sub>3</sub></small> layer enhances switching uniformity by stabilizing the filament path, while an AlN layer acts as an oxygen barrier to improve retention. A thin SiO<small><sub>2</sub></small> tunnel barrier is also introduced to modulate oxygen ion migration, which localized the formation of conductive filaments and significantly improved endurance by reducing cycle-to-cycle variation. This material-engineered architecture enables stable and repeatable resistive switching with low variability and high endurance. Neuromorphic characteristics were evaluated by applying pulse-based electrical stimuli to emulate biological synaptic behaviors such as long-term potentiation (LTP), long-term depression (LTD), and spike-timing-dependent plasticity (STDP), enabling analog synaptic weight updates. The multibit capabilities of the device were systematically investigated by modulating voltage amplitudes and applying incremental step pulse with verify algorithm (ISPVA) scheme, demonstrating reliable conductance tuning up to 8-bit resolution. Furthermore, the device was integrated into a memristor-based pattern recognition system for edge-computing-oriented neuromorphic inference, where externally controlled conductance states were used to emulate synaptic weights during digit classification. These results highlight the potential of the proposed memristor array as a scalable and energy-efficient platform for on-device learning and in-memory computing applications in edge environments.</p>","PeriodicalId":84,"journal":{"name":"Journal of Materials Chemistry C","volume":" 40","pages":" 20675-20689"},"PeriodicalIF":5.1,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145315626","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}
Jingyu Du, Daohai Zhang, Yuhuan Xu, Xiao Zhan and Shuhao Qin
{"title":"A high strength and dendrite free low-temperature nanocellulose composite PVA gel electrolyte for zinc ion batteries","authors":"Jingyu Du, Daohai Zhang, Yuhuan Xu, Xiao Zhan and Shuhao Qin","doi":"10.1039/D5TC01464F","DOIUrl":"https://doi.org/10.1039/D5TC01464F","url":null,"abstract":"<p >With the increasing global energy demand, water-based zinc ion batteries have received widespread attention. However, the growth of zinc dendrites and the occurrence of side reactions on the surface of zinc electrodes can affect the capacity of zinc ion batteries, hindering their practical application. This study reports a multifunctional dendrite-free gel electrolyte prepared by introducing carboxyl modified nanocellulose (C-CNFs) into a polyvinyl alcohol (PVA) based gel electrolyte. At the same time, we also add the antifreeze agent dimethyl sulfoxide (DMSO) to it, which greatly improves the low-temperature performance of gel electrolytes. The rich functional groups on the surface of C-CNFs can effectively adjust the continuous movement of PVA and improve the mechanical strength of the gel electrolyte, and at the same time, they can effectively absorb zinc ions, enable uniform distribution of zinc ions in the electrolyte, reduce the interface concentration gradient, and reduce the occurrence of side reactions, so that the zinc ion deposition is more uniform, and dendrite free deposition is achieved. The polyaniline zinc ion battery assembled with this electrolyte can stably cycle over 3000 times at room temperature, with a capacity retention rate of 83.23%. At −20 °C, the capacity retention rate reaches 60% after 1200 cycles.</p>","PeriodicalId":84,"journal":{"name":"Journal of Materials Chemistry C","volume":" 40","pages":" 20531-20539"},"PeriodicalIF":5.1,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145315584","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}
Yanran Liu, Allen Jian Yang, Shanhu Wang, Huiping Han, Jiayi Qin, Zhiwei Li, Tianli Jin, Josephine Si Yu See, Liang Wu and X. Renshaw Wang
{"title":"Stable operation of two-dimensional field-effect transistors with van der Waals integrated SrTiO3 top-gate dielectrics","authors":"Yanran Liu, Allen Jian Yang, Shanhu Wang, Huiping Han, Jiayi Qin, Zhiwei Li, Tianli Jin, Josephine Si Yu See, Liang Wu and X. Renshaw Wang","doi":"10.1039/D5TC02024G","DOIUrl":"https://doi.org/10.1039/D5TC02024G","url":null,"abstract":"<p >The ultra-thin atomic layer structure of two-dimensional (2D) materials confers potential capabilities that extend and transcend Moore's law, while rendering them highly susceptible to environmental factors such as temperature fluctuations, adsorbates, and trap charges in adjacent dielectric materials. Consequently, the stability of 2D material-based devices has become critically important for the fabrication of low-power field-effect transistors (FETs). In this work, we constructed top-gated 2D FETs using monolayer MoS<small><sub>2</sub></small> and SrTiO<small><sub>3</sub></small> (STO) as the channel and dielectrics, respectively. We systematically investigated their temperature stability, electrical hysteresis and long-term stability under ambient conditions. Experimental results demonstrate that STO top-gated MoS<small><sub>2</sub></small> FETs exhibit remarkable stability, maintaining performance after one month of ambient exposure and showing no irreversible degradation under thermal (100 °C) and electrical stress conditions. This study provides valuable reference for enhancing the stability of low dimensional devices and for developing 2D devices with complex functionalities.</p>","PeriodicalId":84,"journal":{"name":"Journal of Materials Chemistry C","volume":" 39","pages":" 20056-20064"},"PeriodicalIF":5.1,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145248110","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}
Jiao Liu, Qiangqiang Wen, Jianwei Cao, Yuwei Ma, Weixiang Shang, Gaofei Pan, Hongxia Li, Fei Ruan, Qingchun Wang and Jinxiao Bao
{"title":"Photochromic and photoluminescence modulation properties of Zr6Nb2O17 ceramics doped with a variety of rare earth ions","authors":"Jiao Liu, Qiangqiang Wen, Jianwei Cao, Yuwei Ma, Weixiang Shang, Gaofei Pan, Hongxia Li, Fei Ruan, Qingchun Wang and Jinxiao Bao","doi":"10.1039/D5TC02458G","DOIUrl":"https://doi.org/10.1039/D5TC02458G","url":null,"abstract":"<p >Inorganic photochromic (PC) materials are increasingly recognized as promising candidates for anti-counterfeiting technologies and optical storage applications. To enhance their practical value, integrating superior mechanical properties can improve durability, ensuring stable performance over extended periods of use. In this study, we synthesized Zr<small><sub>6</sub></small>Nb<small><sub>2</sub></small>O<small><sub>17</sub></small>-based structural–functional integrated ceramics doped with rare earth ions (Sm<small><sup>3+</sup></small>, Eu<small><sup>3+</sup></small>, Dy<small><sup>3+</sup></small>, and Ho<small><sup>3+</sup></small>) using the high-temperature solid-state reaction method. By controlling the excitation energy of luminescent centers, we regulated the photochromic contrast and photoluminescence modulation ratio of the materials. The results showed that, upon irradiation with 365 nm UV light, all prepared ceramic samples exhibited a significant deepening in color. The photochromic contrasts of the four types of rare earth ion-doped Zr<small><sub>6</sub></small>Nb<small><sub>2</sub></small>O<small><sub>17</sub></small> ceramics were 20.4% (Sm<small><sup>3+</sup></small>), 20.3% (Eu<small><sup>3+</sup></small>), 19.5% (Dy<small><sup>3+</sup></small>), and 20.0% (Ho<small><sup>3+</sup></small>), significantly higher than the undoped matrix's contrast of 12.4%. After heating at 350 °C, the colors of the ceramics were restored. Even after eight coloring–bleaching cycles, the color-changing performance remained stable, demonstrating excellent cycling stability and reversibility. Fluorescence modulation based on photochromic reactions effectively controlled the luminescence intensity of the rare earth ions, with luminescence modulation ratios of 39.7% (Sm<small><sub>2</sub></small>O<small><sub>3</sub></small>), 62.9% (Eu<small><sub>2</sub></small>O<small><sub>3</sub></small>), 61.2% (Dy<small><sub>2</sub></small>O<small><sub>3</sub></small>), and 41.3% (Ho<small><sub>2</sub></small>O<small><sub>3</sub></small>). The Vickers hardness values of different compositions ranged from 14.66 to 15.90 GPa, while the fracture toughness values ranged between 4.66 and 4.98 MPa m<small><sup>1/2</sup></small>. All ceramic materials exhibited excellent cycling stability, reversibility, and rapid photoresponse times, indicating significant potential for applications in optical information storage.</p>","PeriodicalId":84,"journal":{"name":"Journal of Materials Chemistry C","volume":" 39","pages":" 20289-20301"},"PeriodicalIF":5.1,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145248131","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":"Evolution of color-tunable TADF emitters in OLEDs: from design strategies to color modulation","authors":"Tapashi Sarmah, Chakali Srinivas, Debika Barman, Rajdikshit Gogoi, Retwik Parui, Kavita Narang, Himangshu Baishya and Parameswar Krishan Iyer","doi":"10.1039/D5TC02697K","DOIUrl":"https://doi.org/10.1039/D5TC02697K","url":null,"abstract":"<p >Organic thermally activated delayed fluorescence (TADF) materials have gained considerable attention in recent times, specifically in advancing organic light-emitting diodes (OLEDs) due to the possibility of achieving 100% EQE and the ability to tune their emission color. This review highlights the evolution of molecular design strategies that enable precise control of the singlet–triplet energy gap (Δ<em>E</em><small><sub>ST</sub></small>) and reverse intersystem crossing (RISC), thereby advancing device efficiency and color purity. We discuss the progression from early donor–acceptor systems to more advanced methodologies, including π-conjugation tuning and steric and substituent engineering, through-space charge transfer (TSCT), multi-resonance (MR) TADF, and circularly polarized luminescence (CPL)-active TADF emitters. In the later sections, we summarize the progression from the early conceptual development to the recent emergence of blue, green, red, and white TADF OLEDs and their operation mechanism. Thus, the objective of this review is to connect molecular design strategies with the development of next-generation TADF materials for high-performance, color-tunable OLEDs.</p>","PeriodicalId":84,"journal":{"name":"Journal of Materials Chemistry C","volume":" 40","pages":" 20367-20423"},"PeriodicalIF":5.1,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145315565","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}
Yonglin Yang, Xiao Fu, Honglong Ning, Zhihao Liang, Weixin Cheng, Junxiong Luo, Han He, Weiguang Xie, Rihui Yao and Junbiao Peng
{"title":"Enhanced charge trapping effect in PVA/PbI2 synaptic transistors achieved through integrated UV irradiation and thermal annealing treatments","authors":"Yonglin Yang, Xiao Fu, Honglong Ning, Zhihao Liang, Weixin Cheng, Junxiong Luo, Han He, Weiguang Xie, Rihui Yao and Junbiao Peng","doi":"10.1039/D5TC01587A","DOIUrl":"https://doi.org/10.1039/D5TC01587A","url":null,"abstract":"<p >Charge-trapping synaptic transistors, owing to their excellent non-volatility, controllable channel conductance, and switching performance, have garnered widespread attention as promising candidates for neuromorphic devices. In this study, the underlying PVA film can smooth the surface of the PbI<small><sub>2</sub></small> film, thus decreasing its surface roughness and alleviating the charge trapping phenomenon at the PbI<small><sub>2</sub></small>/IGZO heterojunction. The PVA/PbI<small><sub>2</sub></small> charge-trapping synaptic transistors exhibit progressively enhanced charge-trapping capacity with increasing PbI<small><sub>2</sub></small> thickness, attributed to the elevated concentration of iodine vacancies (V<small><sub>I</sub></small>) within the PbI<small><sub>2</sub></small> layer. Moreover, the synergistic combination of UV irradiation and thermal annealing can significantly enhance the charge trapping capability of PVA/PbI<small><sub>2</sub></small> synaptic transistors because it induces the decomposition of PbI<small><sub>2</sub></small> and the formation of PbO, thus modulating the concentration of V<small><sub>I</sub></small>. At a lower UV irradiation intensity of 87.5 mW cm<small><sup>−2</sup></small>, the hysteresis window of the devices initially increases, then decreases with increasing temperature. In contrast, when the UV irradiation intensity is elevated to 122.5 mW cm<small><sup>−2</sup></small>, the hysteresis window shows a monotonic decrease with increasing temperature. When the UV irradiation intensity was maintained at 87.5 mW cm<small><sup>−2</sup></small> and the thermal annealing temperature at 150 °C, the device demonstrated a substantial hysteresis window of 8.56 ± 0.34 V (<em>V</em><small><sub>G</sub></small>: −10–10 V). Finally, the PVA/PbI<small><sub>2</sub></small> charge-trapping synaptic transistor manifested typical synaptic characteristics. The image recognition accuracy reached as high as 90.1% after 40 training epochs. This suggests that PVA/PbI<small><sub>2</sub></small> synaptic transistors hold considerable promise in the fields of neuromorphic computing and artificial intelligence (AI).</p>","PeriodicalId":84,"journal":{"name":"Journal of Materials Chemistry C","volume":" 39","pages":" 20169-20181"},"PeriodicalIF":5.1,"publicationDate":"2025-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145248118","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}
Yu Liu, ShuaiYu Wang, Dan Jiang, Lei Wang and Fengyu Li
{"title":"Janus S-XSSe: a new family of 2D polar half-metals with stacking-engineered magnetism and antiferromagnetic spin splitting","authors":"Yu Liu, ShuaiYu Wang, Dan Jiang, Lei Wang and Fengyu Li","doi":"10.1039/D5TC01948F","DOIUrl":"https://doi.org/10.1039/D5TC01948F","url":null,"abstract":"<p >The quest for materials uniting polarity with metallicity or half-metallicity is pivotal for next-generation multifunctional devices, yet their realization, particularly with robust magnetism, remains a formidable challenge. Here, we unveil a new family of two-dimensional (2D) Janus <em>S</em>-XSSe (X = Re, Os, V, Cr and Mo) monolayers as intrinsically polar metals/half-metals, exhibiting substantial out-of-plane polarization (2.56–4.00 pC m<small><sup>−1</sup></small>) and excellent structural stability. We demonstrate that <em>S</em>-VSSe, <em>S</em>-CrSSe and <em>S</em>-MoSSe are polar half-metals, where the distinct origins of polarity (S–Se electronegativity difference) and half-metallicity (transition metal d-orbitals) enable their robust coexistence. Furthermore, intriguing anisotropic Rashba effects have been observed in polarized metallic <em>S</em>-ReSSe and <em>S</em>-OsSSe monolayers. In addition, we identify a viable polarization switching pathway, whose energy barrier can be effectively tuned by biaxial strain. Moreover, bilayer <em>S</em>-XSSe systems exhibit enhanced magnetic transition temperature and stacking-dependent magnetism, elucidated <em>via</em> spin Hamiltonian analysis and interlayer electron hopping. Remarkably, an interlayer antiferromagnetic <em>S</em>-VSSe bilayer with parallel polar stacking exhibits significant spin splitting alongside nontrivial topological characteristics, a direct consequence of the built-in electric field breaking inversion symmetry. This discovery of a novel class of polar metals/half-metals, particularly the emergent antiferromagnetic spintronic phenomena in bilayers, paves the way for innovative spintronic and multifunctional electronic applications.</p>","PeriodicalId":84,"journal":{"name":"Journal of Materials Chemistry C","volume":" 40","pages":" 20482-20490"},"PeriodicalIF":5.1,"publicationDate":"2025-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145315551","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}