Advanced Functional Materials最新文献

{"title":"Multibit Ferroelectric HfZrO Memcapacitor for Non-Volatile Analogue Memory and Reconfigurable Electronics","authors":"Deepika Yadav, Spyros Stathopoulos, Patrick Foster, Andreas Tsiamis, Mohamed Awadein, Hannah Levene, Themis Prodromakis","doi":"10.1002/adfm.202531011","DOIUrl":"https://doi.org/10.1002/adfm.202531011","url":null,"abstract":"Tunable capacitors are essential for adaptive and reconfigurable electronics, yet most existing implementations rely on continuous biasing or mechanical actuation. In this context, ferroelectric memcapacitors have emerged as promising non-volatile tuning elements for analogue, RF, and neuromorphic computing applications. While multilevel capacitance has been demonstrated in recent reports, a systematic understanding of switching behavior, stability, and circuit-level implications remains limited. Here, we present a voltage-programmable (<span data-altimg=\"/cms/asset/dcc2dc97-a57a-48e9-9985-72d7671a1094/adfm74384-math-0001.png\"></span><math altimg=\"urn:x-wiley:1616301X:media:adfm74384:adfm74384-math-0001\" display=\"inline\" location=\"graphic/adfm74384-math-0001.png\">\u0000<semantics>\u0000<mo>±</mo>\u0000$pm$</annotation>\u0000</semantics></math>3 V) ferroelectric memcapacitor based on a simple TiN/HfZrO/TiN stack that achieves more than eight stable capacitive states within a competitive memory window of <span data-altimg=\"/cms/asset/85383981-f2f9-423c-ac68-79bc6c7a451c/adfm74384-math-0002.png\"></span><math altimg=\"urn:x-wiley:1616301X:media:adfm74384:adfm74384-math-0002\" display=\"inline\" location=\"graphic/adfm74384-math-0002.png\">\u0000<semantics>\u0000<mo>∼</mo>\u0000$sim$</annotation>\u0000</semantics></math>24 pF in compact <span data-altimg=\"/cms/asset/40b45f38-694d-43c9-80c9-d4093f9105aa/adfm74384-math-0003.png\"></span><math altimg=\"urn:x-wiley:1616301X:media:adfm74384:adfm74384-math-0003\" display=\"inline\" location=\"graphic/adfm74384-math-0003.png\">\u0000<semantics>\u0000<mrow>\u0000<mn>60</mn>\u0000<mo>×</mo>\u0000<mn>60</mn>\u0000<mspace width=\"3.33333pt\"></mspace>\u0000<mi>μ</mi>\u0000<msup>\u0000<mi mathvariant=\"normal\">m</mi>\u0000<mn>2</mn>\u0000</msup>\u0000</mrow>\u0000$60 times 60nobreakspace umu{rm m}^2$</annotation>\u0000</semantics></math> devices, exhibiting synaptic-like switching behavior. The devices show endurance up to <span data-altimg=\"/cms/asset/e3fd1e82-91d2-4ccc-a4de-4b97fd97f089/adfm74384-math-0004.png\"></span><math altimg=\"urn:x-wiley:1616301X:media:adfm74384:adfm74384-math-0004\" display=\"inline\" location=\"graphic/adfm74384-math-0004.png\">\u0000<semantics>\u0000<msup>\u0000<mn>10</mn>\u0000<mn>6</mn>\u0000</msup>\u0000$10^{6}$</annotation>\u0000</semantics></math> cycles and state retention beyond <span data-altimg=\"/cms/asset/056f3cf3-50c5-47cf-af0b-75baab91c371/adfm74384-math-0005.png\"></span><math altimg=\"urn:x-wiley:1616301X:media:adfm74384:adfm74384-math-0005\" display=\"inline\" location=\"graphic/adfm74384-math-0005.png\">\u0000<semantics>\u0000<msup>\u0000<mn>10</mn>\u0000<mn>5</mn>\u0000</msup>\u0000$10^{5}$</annotation>\u0000</semantics></math> s without extrapolation. Systematic area scaling from <span data-altimg=\"/cms/asset/71198647-cc0c-4560-ab83-c6474ceddb42/adfm74384-math-0006.png\"></span><math altimg=\"urn:x-wiley:1616301X:media:adfm74384:adfm74384-math-0006\" display=\"inline\" location=\"graphic/adfm74384-math-0006.png\">\u0000<semantics>\u0000<mrow>\u0000<mn>2</mn>\u0000<mo>×</mo>\u0000<mn>2</mn>\u0000</mrow>\u0000$2 times 2$</annotation>\u0000</semantics></math> to <span data-altimg=\"/cms/asset/7a2a02ff-e285-4977-9716-62c47","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"9 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146116072","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Universal Integration of 2D Organic Single Crystals With Fluorinated Polymer Dielectrics for High-Performance Transistors and Single-Pixel Imaging Applications","authors":"Huchao Li, Shuchao Qin, Wen Xu, Guofeng Tian, Yunfeng Deng, Zhixin Hu, Xin Ye, Hui Yang, Lang Jiang, Deyang Ji, Wenping Hu","doi":"10.1002/adfm.74393","DOIUrl":"https://doi.org/10.1002/adfm.74393","url":null,"abstract":"Organic single-crystal field-effect transistors (OSCFETs) are regarded as an ideal platform for investigating intrinsic charge transport behaviors and developing high-performance organic electronic devices, thanks to their ordered molecular stacking and minimal grain boundary defects. However, conventional integration methods frequently introduce impurities that induce interface defects or crystal damage, significantly impairing charge transport efficiency-a long-standing limitation plaguing diverse organic semiconductors. To address this critical challenge, we propose a universal strategy for the integration of two-dimensional (2D) organic single crystals with fluorinated polymer dielectrics. This approach synergistically combines an in-house microspacing in-air sublimation (MAS) growth technique with a gentle, damage-free transfer process, effectively eliminating interfacial imperfections. The resulting high-quality crystal-dielectric interfaces enable OSCFETs to achieve exceptional comprehensive performance: a record-high mobility of 18.9 cm² V⁻¹ s⁻¹, ultralow operating voltage of −5 V, ultrafast photoresponse of 30 µs, outstanding high-speed image acquisition capability, and robust dual-mode driving performance for organic light-emitting diodes (OLED). This work establishes a universal method for constructing high-quality single crystals on polymer dielectrics, which holds broad implications for advancing high-speed sensing, imaging technologies, flexible displays, and integrated logic circuits.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"9 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146116254","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Epoxy Network Hosts Confine Small Molecule Guests for Enhancing Phosphorescence Through F-π and π-π Synergistic Interactions","authors":"Xinyue Xu, Yanji Zhu, Xuewei Jiao, Haonan Liu, Haodong Hu, Yue Zhang, Junqi Ning, Huaiyuan Wang","doi":"10.1002/adfm.202530467","DOIUrl":"https://doi.org/10.1002/adfm.202530467","url":null,"abstract":"Organic room-temperature phosphorescent (RTP) materials have attracted significant interest in information security and anti-counterfeiting due to their unique afterglow properties. However, the role of non-covalent interactions in enhancing phosphorescence remains insufficiently explored. Herein, we report a composite coating based on the synergistic effects of F-π and π-π stacking interactions within a dual-phase 3D covalently cross-linked network, by confining small molecular guests within an epoxy network host. The coating exhibits an ultra-long room-temperature phosphorescence (URTP) lifetime of up to 5.40 s, representing the longest lifetime reported in an epoxy resin system. The coating also displays switchable URTP and excellent surface characteristics, enabling the creation of rewritable anti-counterfeiting labels through light-activated printing and thermal erasure. Its low surface energy (15.85 mN·m⁻¹) and self-cleaning ability ensure the long-term stability and concealment of encoded information. This work highlights the efficacy of engineering non-covalent interactions for the development of high-performance, erasable organic phosphorescent materials in anti-counterfeiting applications.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"302 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122406","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Carbon Nanotubes Assembled Ordered Macro-Microporous Superstructure as Bifunctional Oxygen Electrocatalyst for Long-Life Rechargeable Zn–Air Batteries","authors":"Shilong Wen, Ke Ma, Yongfang Zhang, Ying Wang, Wenjie Yu, Liyang Shao, Xue Yang, Yanchao Zhao, Cong Han, Rutao Wang, Jianxing Shen, Enyan Guo, Liting Yan, Lili Han, Xuebo Zhao, Lianzhou Wang","doi":"10.1002/adfm.202531733","DOIUrl":"https://doi.org/10.1002/adfm.202531733","url":null,"abstract":"Achieving precise fabrication of ordered superstructures with multifunctional catalytic activity is fascinating but elusive due to uncontrollable interfacial energy and growth kinetics at the material surface. Herein, we develop a facile strategy for oriented formation of carbon nanotubes (CNT) anchored on three-dimensionally ordered macro-microporous (3DOM) superstructure derived from a Co-based 3DOM metal-organic framework (3DOM-MOF). Mechanism studies based on density functional theory (DFT) calculations and in situ spectroscopy reveal that the synergistic coupling of curved CNTs supports and Co nanoparticles in the as-prepared Co-based porous superstructures CNTs catalysts (Co-HOPS-CNTs_20D) can regulate the electronic structure of the isolated Co-N₄ sites, thus optimizing the binding strength of the oxygenated intermediates and facilitating intrinsic catalyst activity. The unique feature of the superstructure is validated using 3D transmission electron microscopy tomography, and the corresponding finite element analysis (FEA) simulations prove enhanced conductivity of Co-HOPS-CNTs_20D superstructure, which facilitates transfer efficiency of electrons and improves catalytic activity. As a result, the Co-HOPS-CNTs_20D exhibits a low overpotential of 287 mV at 10 mA cm⁻² for OER and a high ORR half-wave potential of 0.863 V. The zinc-air battery incorporating Co-HOPS-CNTs_20D demonstrates efficient and stable operation over a period of 160 h.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"89 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122408","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Heterogeneous Coherent Interface Enabling Nonstochastic Crystallization for Phase-Change Memory","authors":"Tian-Yu Zhao, Jiahao Li, Nian-Ke Chen, Bai-Qian Wang, Xiaomin Cheng, Shun-Yao Qin, Huan-Ran Ding, Shengbai Zhang, Hong-Bo Sun, Xiangshui Miao, Xian-Bin Li","doi":"10.1002/adfm.202523223","DOIUrl":"https://doi.org/10.1002/adfm.202523223","url":null,"abstract":"Phase-change memory (PCM) displays great promise for the storage-class memory (SCM) technology due to its combination of fast speed of dynamic random-access memory and nonvolatility of Flash. Yet, to meet the high industrial requirement of write/erase speed for the SCM application, robust strategies for further accelerating phase transition, particularly from amorphous to crystalline PCM materials, are urgently needed. In this work, we propose a unique strategy of coherent-interface induced ultrafast crystallization in PCM materials. Employing rock-salt YAs/Ge₂Sb₂Te₅ as a prototype, systematic first-principles molecular dynamics demonstrate that rapid nonstochastic crystallization behaviors can be achieved by the rock-salt-lattice-matching and high-temperature-resistant heterogeneous interface attached to the popular PCM material Ge₂Sb₂Te₅ (GST). Further experiment shows that the YAs-incorporated GST device has a faster SET process compared with the pure GST device. Finally, to extend the strategy in the family of inorganic materials, high-throughput screening from over 150 000 structures discovers as many as 71 candidates for coherent interfaces with PCM GST. The present study establishes a promising strategy to overcome the speed bottleneck of PCM through atomic-scale interface design for future storage-class memory implementation.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"87 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146116073","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Diethyl Sulfide as a Multifunctional Electrolyte Additive for Enhancing Electrochemical Performance of Lithium Metal Batteries","authors":"Wenjie Zhang, Xiaosong Xiong, Run Xu, Guangyao Xiang, Tao Wang, Xu Liu, Yong Wang, Lili Liu, Yuping Wu","doi":"10.1002/adfm.202529688","DOIUrl":"https://doi.org/10.1002/adfm.202529688","url":null,"abstract":"With the increasing demand for energy storage devices with higher energy density, lithium metal anode (LMA) has emerged as promising candidate due to ultra-high theoretical specific capacity (3860 mAh g⁻¹) and the lowest reduction potential (-3.04 V vs. S.H.E.). However, the practical application of LMA is still restricted by notorious active lithium loss and lithium dendrite growth, which cause low Coulombic efficiency, poor cycling life, and even potential safety hazards. In this study, a multifunctional diethyl sulfide electrolyte additive is proposed to synergistically construct a stable Li₂S-rich solid electrolyte interphase (SEI) and Li₂S/Li₂SO₄/Li₂SO₃-rich cathode electrolyte interphases (CEI), which could accelerate Li ions (Li⁺) transport kinetics and enhance the interfacial stability during long-term cycling. Moreover, the sulfur-rich composite in electrolyte interface could reduce the energy barrier for Li⁺ desolvation and thereby enhance interface dynamics. Based on these merits, the introduction of 2.0 vol.% diethyl sulfide into a carbonate electrolyte (without FEC) enables the lithium anode to achieve a 7-fold enhancement in long-term cycling performance. More impressively, the Li||LiFePO₄ (LFP) pouch cell with the modified electrolyte achieves an outstanding capacity retention of 98.75% after 200 cycles at 0.1 C. The multifunctional diethyl sulfide additive paves the way for high-performance LMBs for practical applications.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"88 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146116251","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"An All-in-One DNA Nanodevice as a Programmed Theranostic Platform for Intelligent Cancer Cell Identification and On-Site Drug Release","authors":"Yi Yuan, Qiufeng Song, Linwen Lan, Xuefen Chen, Jiangchuan Du, Linjun Zhang, Nan Chen, Zhifa Shen, Chang Xue","doi":"10.1002/adfm.202531762","DOIUrl":"https://doi.org/10.1002/adfm.202531762","url":null,"abstract":"Chemotherapy remains the cornerstone of malignant tumor treatment; however, off-target effects and severe systemic toxicity limit its efficacy. Here, we developed a programmable theranostic platform based on an all-in-one smart DNA nanodevice (SND) that integrates a programmable cancer-cell classifier (PCC) with a responsive delivery system (RDS). By employing a modular design that permits the customization of aptamer combinations for specific cancer cell types, the platform achieves accurate tumor recognition and spatially controlled drug release. Functioning as a dual-aptamer molecular guide, the PCC utilizes an interlocked configuration to identify cell-surface biomarkers in a stepwise manner, thereby ensuring highly specific target cell recognition. The RDS is constructed from a 1D central trunk flanked by double-stranded drug-loading units, a structure that confers high payload capacity and nuclease-enhanced resistance. These peripheral units also function as recognition elements for endogenous stimuli; upon activation, they trigger conformational changes that facilitate efficient intracellular drug release. In vivo studies in tumor-bearing mice demonstrate that this programmable theranostic platform selectively accumulates in tumor tissues, leading to marked inhibition of tumor growth and a substantial reduction in systemic toxicity. By integrating programmable molecular recognition with stimulus-responsive drug delivery, our theranostic platform offers a promising strategy for advancing targeted cancer therapy.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"38 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122276","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Laser Engineering of HfN-Based Nanoparticles for Safe NIR-I Photothermal and X-ray Enhancing Cancer Therapies","authors":"Julia S. Babkova, Ivan V. Zelepukin, Lyubov V. Gorelik, Anton L. Popov, Andrei I. Pastukhov, Gleb V. Tikhonowski, Maxim S. Savinov, Danil D. Kolmanovich, Nikita A. Pivovarov, Alina Yu. Kapitannikova, Anton A. Popov, Anna S. Sogomonyan, Vsevolod A. Skribitsky, Aziz B. Mirkasymov, Andrei V. Kabashin, Sergey M. Deyev","doi":"10.1002/adfm.202529532","DOIUrl":"https://doi.org/10.1002/adfm.202529532","url":null,"abstract":"Transition metal nitrides are robust alternatives to noble metals in plasmonics, offering strong NIR absorption, high melting points, and chemical stability. Hafnium nitride (HfN) nanoparticles are especially promising owing to the high atomic number of hafnium, which could provide X-ray-based theranostic functionalities in addition to the prominent plasmonic properties. However, their biomedical potential has remained unexplored due to difficulties in synthesis of pure water-dispersible nanostructures. Here, we use femtosecond laser ablation in acetone to produce HfN-based nanoparticles exhibiting a red-shifted plasmon resonance spanning both the NIR-I and NIR-II windows. We then present the first in vivo assessment of the biocompatibility, photothermal performance, and radiosensitizing capacity of HfN-based nanomaterials. We show that PEGylated HfN nanoparticles exhibit negligible cytotoxicity across three cancer cell lines in vitro and no significant long-term adverse effects in healthy mice following intravenous administration. NIR-I photothermal therapy of 4T1 tumor-bearing mice after systemic nanoparticle administration leads to a 2.4-fold suppression of tumor growth and a significant extension of survival. The multimodal therapeutic potential of HfN is demonstrated by the enhanced efficacy of X-ray radiotherapy after local administration of nanoparticles. Laser ablated engineering of hafnium nitrides establishes this nanomaterial as a promising candidate for multimodal optical and radiosensitizing theranostics.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"288 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122316","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Accelerated Discovery of High Performance Ni3S4/Ni3Mo HER Catalysts via Bayesian Optimization","authors":"Namuersaihan Namuersaihan, Zhiqiang Zhao, Oliver J. Conquest, Ying Shu, Haoyue Sun, Chunjing Su, Qi Cheng, Aloysius Soon, Catherine Stampfl, Jun Huang","doi":"10.1002/adfm.202528363","DOIUrl":"https://doi.org/10.1002/adfm.202528363","url":null,"abstract":"The hydrogen evolution reaction (HER) in alkaline media is a promising strategy for sustainable hydrogen production, but the exploration of efficient and durable HER electrocatalysts is often hindered by the empirical and time-consuming nature of traditional synthesis. Herein, a machine learning (ML)–driven strategy combining Bayesian optimization is introduced to achieve the rational design of Ni₃S₄/Ni₃Mo heterostructures for alkaline HER. By coupling predictive modeling with experimental feedback, this approach efficiently navigated a complex synthesis space and identified conditions yielding a structurally and electronically optimized catalyst. The optimized Ni₃S₄/Ni₃Mo exhibits a vibrant morphological evolution—from compact buds to blooming petal-like structures—enabling enriched active sites and accelerated mass transport. Guided by Bayesian optimization, the optimized Ni₃S₄/Ni₃Mo achieves a 10.5-fold enhancement in <i>C</i>_dl and delivers an exceptionally low overpotential of 18.2 mV at 100 mA cm⁻², outperforming most reported transition-metal catalysts and even surpassing commercial Pt/C. Mechanistic insights from in situ Raman and DFT reveal that interfacial charge redistribution between Ni₃S₄ and Ni₃Mo optimizes H* adsorption (Δ<i>G</i>_H* ≈ 0.04 eV) and significantly reduces the water-dissociation barrier (0.08 eV), thereby accelerating reaction kinetics. This work demonstrates how the ML-guided optimization can synergistically couple morphology control, interfacial engineering with electronic tuning, offering a generalizable framework for intelligent catalyst discovery and mechanistic understanding in electrochemical energy conversion.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"47 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122403","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Beyond the Edge: Charge-Transfer Excitons in Organic Donor-Acceptor Cocrystals","authors":"Sebastian Anhäuser, Ana M. Valencia, Sergei I. Ivlev, Marc Zeplichal, Andreas Terfort, Caterina Cocchi, Gregor Witte","doi":"10.1002/adfm.202530499","DOIUrl":"https://doi.org/10.1002/adfm.202530499","url":null,"abstract":"Charge-transfer excitons (CTXs) at organic donor/acceptor interfaces are crucial intermediates for charge separation in photovoltaic devices. While blends used in real-world devices hamper detailed characterization of CTXs, atomistic models of cocrystals offer powerful alternatives for gaining microscopic insights. In this work, we investigate electronic and optical properties of acene-perfluoroacene cocrystals (anthracene, tetracene, and pentacene), combining experimental synthesis and characterization with first-principles calculations based on many-body theory. We prepare ultrathin cocrystals for polarization-resolved transmission-absorption spectroscopy, linking exciton polarization with molecular packing. Complementing this analysis, density-functional and many-body perturbation theory reveal complex excitonic landscapes that challenge several common assumptions about CTXs in weakly interacting donor-acceptor systems. For the studied cocrystals, we demonstrate that such CTXs are not limited to the absorption onset, but also occur at higher energy and produce sharp, intense absorption features. Adopting the intrinsic molecular coordinate system, we categorize the various excitons according to their polarization and show that the transition dipole moment of the lowest energy CTX is not necessarily aligned with the donor-acceptor stacking axis. We further characterize triplet excitons from first principles, which are only indirectly accessible experimentally. This work provides a deep understanding of CTXs in organic cocrystals, developing a refined conceptual framework that is crucial for future design of environmentally sustainable photoactive materials.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"12 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122404","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}