Marcelo L. Pereira, Emanuel J. A. dos Santos, Luiz A. Ribeiro and Douglas S. Galvão
The recent synthesis of goldene, a 2D atomic monolayer of gold, has opened new avenues in exploring novel materials. However, the question of when multilayer goldene transitions into bulk gold remains unresolved. This study used density functional theory calculations to address this fundamental question. Our findings reveal that multilayer goldene retains an AA-like stacking configuration of up to six layers, with no observation of Bernal-like stacking as seen in graphene. Goldene spontaneously transitions to a bulk-like gold structure at seven layers, adopting a rhombohedral (ABC-like) stacking characteristic of bulk face-centered cubic (FCC) gold. The atomic arrangement converges entirely to the bulk gold lattice for more than ten layers. Quantum confinement significantly impacts the electronic properties, with monolayer and bulk goldene exhibiting levels with linear dispersion at the X-point of the Brillouin zone. In contrast, multilayer goldene shows levels with linear dispersions at the X- and Y-points. Monolayer goldene exhibits anisotropic optical absorption, which is absent in bulk gold. This study provides a deeper understanding of multilayer goldene's structural and electronic properties and stacked 2D materials in general.
{"title":"How does goldene stack?†","authors":"Marcelo L. Pereira, Emanuel J. A. dos Santos, Luiz A. Ribeiro and Douglas S. Galvão","doi":"10.1039/D4MH01319K","DOIUrl":"10.1039/D4MH01319K","url":null,"abstract":"<p >The recent synthesis of goldene, a 2D atomic monolayer of gold, has opened new avenues in exploring novel materials. However, the question of when multilayer goldene transitions into bulk gold remains unresolved. This study used density functional theory calculations to address this fundamental question. Our findings reveal that multilayer goldene retains an AA-like stacking configuration of up to six layers, with no observation of Bernal-like stacking as seen in graphene. Goldene spontaneously transitions to a bulk-like gold structure at seven layers, adopting a rhombohedral (ABC-like) stacking characteristic of bulk face-centered cubic (FCC) gold. The atomic arrangement converges entirely to the bulk gold lattice for more than ten layers. Quantum confinement significantly impacts the electronic properties, with monolayer and bulk goldene exhibiting levels with linear dispersion at the <em>X</em>-point of the Brillouin zone. In contrast, multilayer goldene shows levels with linear dispersions at the <em>X</em>- and <em>Y</em>-points. Monolayer goldene exhibits anisotropic optical absorption, which is absent in bulk gold. This study provides a deeper understanding of multilayer goldene's structural and electronic properties and stacked 2D materials in general.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" 4","pages":" 1144-1154"},"PeriodicalIF":12.2,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143021313","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}
Hardware neural networks could perform certain computational tasks orders of magnitude more energy-efficiently than conventional computers. Artificial neurons are a key component of these networks and are currently implemented with electronic circuits based on capacitors and transistors. However, artificial neurons based on memristive devices are a promising alternative, owing to their potentially smaller size and inherent stochasticity. But despite their promise, demonstrations of memristive artificial neurons have so far been limited. Here we demonstrate a fully on-chip artificial neuron based on microscale electrodes and halide perovskite semiconductors as the active layer. By connecting a halide perovskite memristive device in series with a capacitor, the device demonstrates stochastic leaky integrate-and-fire behavior, with an energy consumption of 20 to 60 pJ per spike, lower than that of a biological neuron. We simulate populations of our neuron and show that the stochastic firing allows the detection of sub-threshold inputs. The neuron can easily be integrated with previously-demonstrated halide perovskite artificial synapses in energy-efficient neural networks.
{"title":"Integrated artificial neurons from metal halide perovskites.","authors":"Jeroen J de Boer, Bruno Ehrler","doi":"10.1039/d4mh01729c","DOIUrl":"10.1039/d4mh01729c","url":null,"abstract":"<p><p>Hardware neural networks could perform certain computational tasks orders of magnitude more energy-efficiently than conventional computers. Artificial neurons are a key component of these networks and are currently implemented with electronic circuits based on capacitors and transistors. However, artificial neurons based on memristive devices are a promising alternative, owing to their potentially smaller size and inherent stochasticity. But despite their promise, demonstrations of memristive artificial neurons have so far been limited. Here we demonstrate a fully on-chip artificial neuron based on microscale electrodes and halide perovskite semiconductors as the active layer. By connecting a halide perovskite memristive device in series with a capacitor, the device demonstrates stochastic leaky integrate-and-fire behavior, with an energy consumption of 20 to 60 pJ per spike, lower than that of a biological neuron. We simulate populations of our neuron and show that the stochastic firing allows the detection of sub-threshold inputs. The neuron can easily be integrated with previously-demonstrated halide perovskite artificial synapses in energy-efficient neural networks.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":12.2,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11745301/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142996530","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}
Conductive hydrogels with stable sensing performance are highly required in soft electronic devices. However, these hydrogels tend to solidify and experience structural damage at sub-zero temperatures, leading to material breakdown and device malfunction. The main challenge lies in effectively designing the micro/nano-structure to enhance mechanical properties and stable strain sensing while preventing freezing in hydrogels. Here, we present a rapid strategy for developing a MXene bridging double-network structure-based strain sensor using polyacrylamide and agar hydrogels that can maintain stable functionality even at an extremely low temperature of -30 °C. By incorporating MXenes as a catalyst to expedite free radical polymerization, we achieve outstanding mechanical and strain sensing properties at room temperature (a high response range of 1000%, a response signal linearity of 0.998, and a gauge factor (GF) value of 1.41). This sensing performance surpasses those reported for many other hydrogels. Importantly, we also observe that the stable micro-nanostructure in the hydrogel at an extreme temperature of approximately -30 °C results in exceptional strain-detection performance (a stable response range of up to 250%) with a linearity of 0.995 and a GF value of 1.25 due to its remarkably low freezing point (<-80 °C). These findings highlight the application of our hydrogel-based tactile sensor in low-temperature environments.
{"title":"Anti-freezing conductive hydrogels with exceptional mechanical properties and stable sensing performance at -30 °C.","authors":"Yunfei Yu, Shuo Wang, Huitao Yu, Xiaojian Liao, Wei Feng","doi":"10.1039/d4mh01115e","DOIUrl":"https://doi.org/10.1039/d4mh01115e","url":null,"abstract":"<p><p>Conductive hydrogels with stable sensing performance are highly required in soft electronic devices. However, these hydrogels tend to solidify and experience structural damage at sub-zero temperatures, leading to material breakdown and device malfunction. The main challenge lies in effectively designing the micro/nano-structure to enhance mechanical properties and stable strain sensing while preventing freezing in hydrogels. Here, we present a rapid strategy for developing a MXene bridging double-network structure-based strain sensor using polyacrylamide and agar hydrogels that can maintain stable functionality even at an extremely low temperature of -30 °C. By incorporating MXenes as a catalyst to expedite free radical polymerization, we achieve outstanding mechanical and strain sensing properties at room temperature (a high response range of 1000%, a response signal linearity of 0.998, and a gauge factor (GF) value of 1.41). This sensing performance surpasses those reported for many other hydrogels. Importantly, we also observe that the stable micro-nanostructure in the hydrogel at an extreme temperature of approximately -30 °C results in exceptional strain-detection performance (a stable response range of up to 250%) with a linearity of 0.995 and a GF value of 1.25 due to its remarkably low freezing point (<-80 °C). These findings highlight the application of our hydrogel-based tactile sensor in low-temperature environments.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":12.2,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142996523","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}
Realizing spin-orbit torque (SOT)-driven magnetization switching offers promising opportunities for the advancement of next-generation spintronics. However, the relatively low charge-spin conversion efficiency accompanied by an ultrahigh critical switching current density (Jc) remains a significant obstacle to the further development of SOT-based storage elements. Herein, spin absorption engineering at the ferromagnet/nonmagnet interface is firstly proposed to achieve high SOT efficiency in Pt/Co/Ir trilayers. The Jc value was significantly decreased to 7.5 × 106 A cm-2, achieving a maximum reduction of 58% when a 4.0-nm Gd layer was inserted into the Co/Ir interface. A similar trend was observed in the trilayers with various rare metal insertions, suggesting the universality of this approach. Simultaneously, the highest effective spin Hall angle of 0.29 was obtained in the Pt/Co/Gd (4.0 nm)/Ir multilayers, which was approximately three times greater than that obtained in the Pt/Co/Ir trilayer. First-principles calculations together with polarized neutron reflectivity results revealed that spin mixed conductivity can be significantly enhanced due to a spontaneous interfacial CoGd alloy, which is critical for high SOT efficiency. In addition, the deterministic field-free switching polarity can be tuned by introducing Gd insertion. These findings provide a promising pathway for deeply understanding the spin-charge conversion mechanism, and further enable the design of low-consumption spintronic circuits.
实现自旋轨道转矩(SOT)驱动的磁化开关为下一代自旋电子学的发展提供了很好的机会。然而,相对较低的电荷自旋转换效率和超高的临界开关电流密度(Jc)仍然是制约sot存储元件进一步发展的一个重要障碍。本文首次提出了铁磁体/非磁体界面的自旋吸收工程,以实现Pt/Co/Ir三层薄膜的高SOT效率。当在Co/Ir界面中插入4.0 nm的Gd层时,Jc值显著降低至7.5 × 106 A cm-2,最大降幅达58%。在各种稀有金属插入的三层中观察到类似的趋势,表明该方法的普遍性。同时,Pt/Co/Gd (4.0 nm)/Ir多层膜的有效自旋霍尔角为0.29,约为Pt/Co/Ir多层膜的3倍。第一性原理计算和极化中子反射率结果表明,自发界面CoGd合金可以显著提高自旋混合电导率,这是提高SOT效率的关键。此外,可以通过引入Gd插入来调节确定性的无场开关极性。这些发现为深入理解自旋-电荷转换机制,进一步实现低功耗自旋电子电路的设计提供了一条有希望的途径。
{"title":"High spin-orbit torque efficiency induced by engineering spin absorption for fully electric-driven magnetization switching.","authors":"Pengwei Dou, Jingyan Zhang, Tao Zhu, Peng Kang, Xiao Deng, Yuanbo Wang, Quangao Qiu, Liangyu Feng, Jinhu Hu, Jianxin Shen, Xiao Wang, He Huang, Xinqi Zheng, Shiming Zhou, Baogen Shen, Shouguo Wang","doi":"10.1039/d4mh01628a","DOIUrl":"https://doi.org/10.1039/d4mh01628a","url":null,"abstract":"<p><p>Realizing spin-orbit torque (SOT)-driven magnetization switching offers promising opportunities for the advancement of next-generation spintronics. However, the relatively low charge-spin conversion efficiency accompanied by an ultrahigh critical switching current density (<i>J</i><sub>c</sub>) remains a significant obstacle to the further development of SOT-based storage elements. Herein, spin absorption engineering at the ferromagnet/nonmagnet interface is firstly proposed to achieve high SOT efficiency in Pt/Co/Ir trilayers. The <i>J</i><sub>c</sub> value was significantly decreased to 7.5 × 10<sup>6</sup> A cm<sup>-2</sup>, achieving a maximum reduction of 58% when a 4.0-nm Gd layer was inserted into the Co/Ir interface. A similar trend was observed in the trilayers with various rare metal insertions, suggesting the universality of this approach. Simultaneously, the highest effective spin Hall angle of 0.29 was obtained in the Pt/Co/Gd (4.0 nm)/Ir multilayers, which was approximately three times greater than that obtained in the Pt/Co/Ir trilayer. First-principles calculations together with polarized neutron reflectivity results revealed that spin mixed conductivity can be significantly enhanced due to a spontaneous interfacial CoGd alloy, which is critical for high SOT efficiency. In addition, the deterministic field-free switching polarity can be tuned by introducing Gd insertion. These findings provide a promising pathway for deeply understanding the spin-charge conversion mechanism, and further enable the design of low-consumption spintronic circuits.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":12.2,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142996526","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}
This study focuses on fabricating photonic crystals (PCs) by surfactant-based particle capture at the gas-liquid interface of evaporating sessile droplets. The captured particles form interfacial films, resulting in ordered monolayer depositions manifesting iridescent structural colors. The particle dynamics behind the ordered arrangement is delineated. This arrangement is influenced by the alteration in particles' hydrophobicity, charge, and internal flow introduced by the surfactant addition. The influence of surfactant and particle concentrations on the phenomenon is also investigated. The work demonstrates a drop-by-drop technique to scale up the formation of PCs. Furthermore, the work is extended towards demonstrating the utilization of this mechanism to fabricate arbitrary PCs efficiently by direct writing technique. The particle coverage in directly written patterns is influenced by printing speed and particle concentration, which are adjusted to achieve covert photonic patterns. Finally, the replication of colloidal PC onto a flexible polymer with minimal colloid transfer is demonstrated using soft lithography.
{"title":"Surfactant-based interface capture towards the development of 2D-printed photonic structures.","authors":"Appurva Tiwari, Seong Jae Lee, Ashish Kumar Thokchom","doi":"10.1039/d4mh01560f","DOIUrl":"https://doi.org/10.1039/d4mh01560f","url":null,"abstract":"<p><p>This study focuses on fabricating photonic crystals (PCs) by surfactant-based particle capture at the gas-liquid interface of evaporating sessile droplets. The captured particles form interfacial films, resulting in ordered monolayer depositions manifesting iridescent structural colors. The particle dynamics behind the ordered arrangement is delineated. This arrangement is influenced by the alteration in particles' hydrophobicity, charge, and internal flow introduced by the surfactant addition. The influence of surfactant and particle concentrations on the phenomenon is also investigated. The work demonstrates a drop-by-drop technique to scale up the formation of PCs. Furthermore, the work is extended towards demonstrating the utilization of this mechanism to fabricate arbitrary PCs efficiently by direct writing technique. The particle coverage in directly written patterns is influenced by printing speed and particle concentration, which are adjusted to achieve covert photonic patterns. Finally, the replication of colloidal PC onto a flexible polymer with minimal colloid transfer is demonstrated using soft lithography.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":12.2,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142996546","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}
Recent advances in interfacial solar steam generation have made direct solar desalination a promising approach for providing cost-effective and environmentally friendly clean water solutions. However, developing highly effective, salt-resistant solar absorbers for long-term desalination at high efficiencies and evaporation rates remains a significant challenge. We present a Janus hydrogel-based absorber featuring a surface modified with thermo-responsive hydroxypropyl cellulose (HPC) and a hydrogel matrix containing photothermal conversion units, MXene, specifically designed for long-term seawater desalination. At the lower critical solution temperature, HPC undergoes phase separation, which results in the formation of a rough hydrophobic surface. This process creates a Janus evaporator structure that exhibits a high evaporation rate, excellent salt resistance, and long-term stability. Consequently, the hydrogel absorbers achieve an impressive evaporation rate (3.11 kg m-2 h-1) under one-sun irradiation. Salt residues are deposited only at the edges of the super-hydrophilic bottom. This process ensures long-term evaporator stability for continuous solar evaporation (>30 hours) in simulated seawater at an average evaporation rate of ∼2.58 kg m-2 h-1. With its unique structural design, achieved via a straightforward design process, the flexible Janus absorber serves as an efficient, salt-resistant, and stable solar steam generator for direct solar desalination.
界面太阳能蒸汽产生的最新进展使直接太阳能脱盐成为一种有前途的方法,可以提供具有成本效益和环境友好的清洁水解决方案。然而,开发高效、耐盐的太阳能吸收器,以高效率和高蒸发速率长期淡化海水,仍然是一个重大挑战。我们提出了一种Janus水凝胶基吸收剂,其表面用热响应性羟丙基纤维素(HPC)修饰,水凝胶基质含有光热转换单元MXene,专门用于长期海水淡化。在较低的临界溶液温度下,HPC发生相分离,形成粗糙的疏水表面。这一过程创造了Janus蒸发器结构,具有高蒸发速率,优异的耐盐性和长期稳定性。因此,水凝胶吸收剂在一次太阳照射下实现了令人印象深刻的蒸发速率(3.11 kg m-2 h-1)。盐残只沉积在超亲水底的边缘。该过程确保蒸发器在模拟海水中以平均蒸发速率约2.58 kg m-2 h-1连续太阳蒸发(bbb30小时)的长期稳定性。凭借其独特的结构设计,通过简单的设计过程实现,灵活的Janus吸收器可作为高效,耐盐和稳定的太阳能蒸汽发生器,用于直接太阳能脱盐。
{"title":"Highly salt-resistant and efficient dynamic Janus absorber based on thermo-responsive hydroxypropyl cellulose.","authors":"Jianfeng Gu, Zhaohui Luan, Xinmin Zhang, Huihui Wang, Xu Cai, Weiqing Zhan, Xinyi Ji, Jiajie Liang","doi":"10.1039/d4mh01699h","DOIUrl":"https://doi.org/10.1039/d4mh01699h","url":null,"abstract":"<p><p>Recent advances in interfacial solar steam generation have made direct solar desalination a promising approach for providing cost-effective and environmentally friendly clean water solutions. However, developing highly effective, salt-resistant solar absorbers for long-term desalination at high efficiencies and evaporation rates remains a significant challenge. We present a Janus hydrogel-based absorber featuring a surface modified with thermo-responsive hydroxypropyl cellulose (HPC) and a hydrogel matrix containing photothermal conversion units, MXene, specifically designed for long-term seawater desalination. At the lower critical solution temperature, HPC undergoes phase separation, which results in the formation of a rough hydrophobic surface. This process creates a Janus evaporator structure that exhibits a high evaporation rate, excellent salt resistance, and long-term stability. Consequently, the hydrogel absorbers achieve an impressive evaporation rate (3.11 kg m<sup>-2</sup> h<sup>-1</sup>) under one-sun irradiation. Salt residues are deposited only at the edges of the super-hydrophilic bottom. This process ensures long-term evaporator stability for continuous solar evaporation (>30 hours) in simulated seawater at an average evaporation rate of ∼2.58 kg m<sup>-2</sup> h<sup>-1</sup>. With its unique structural design, achieved <i>via</i> a straightforward design process, the flexible Janus absorber serves as an efficient, salt-resistant, and stable solar steam generator for direct solar desalination.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":12.2,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142996529","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}
Meidan Que, Yuan Xu, Qizhao Wu, Jin Chen, Lili Gao, Shengzhong Frank Liu
Quantum dots have garnered significant interest in perovskite solar cells (PSCs) due to their stable chemical properties, high carrier mobility, and unique features such as multiple exciton generation and excellent optoelectronic characteristics resulting from quantum confinement effects. This review explores quantum dot properties and their applications in photoelectronic devices, including their synthesis and deposition processes. This sets the stage for discussing their diverse roles in the carrier transport, absorber, and interfacial layers of PSCs. We thoroughly examine advances in defect passivation, energy band alignment, perovskite crystallinity, device stability, and broader light absorption. In particular, novel approaches to enhance the photoelectric conversion efficiency (PCE) of quantum dot-enhanced perovskite solar cells are highlighted. Lastly, based on a comprehensive overview, we provide a forward-looking outlook on advanced quantum dot fabrication and its impact on enhancing the photovoltaic performance of solar cells. This review offers insights into fundamental mechanisms that endorse quantum dots for improved PSC performance, paving the way for further development of quantum dot-integrated PSCs.
{"title":"Application of advanced quantum dots in perovskite solar cells: synthesis, characterization, mechanism, and performance enhancement.","authors":"Meidan Que, Yuan Xu, Qizhao Wu, Jin Chen, Lili Gao, Shengzhong Frank Liu","doi":"10.1039/d4mh01478b","DOIUrl":"https://doi.org/10.1039/d4mh01478b","url":null,"abstract":"<p><p>Quantum dots have garnered significant interest in perovskite solar cells (PSCs) due to their stable chemical properties, high carrier mobility, and unique features such as multiple exciton generation and excellent optoelectronic characteristics resulting from quantum confinement effects. This review explores quantum dot properties and their applications in photoelectronic devices, including their synthesis and deposition processes. This sets the stage for discussing their diverse roles in the carrier transport, absorber, and interfacial layers of PSCs. We thoroughly examine advances in defect passivation, energy band alignment, perovskite crystallinity, device stability, and broader light absorption. In particular, novel approaches to enhance the photoelectric conversion efficiency (PCE) of quantum dot-enhanced perovskite solar cells are highlighted. Lastly, based on a comprehensive overview, we provide a forward-looking outlook on advanced quantum dot fabrication and its impact on enhancing the photovoltaic performance of solar cells. This review offers insights into fundamental mechanisms that endorse quantum dots for improved PSC performance, paving the way for further development of quantum dot-integrated PSCs.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":12.2,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142996524","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}
Sreelakshmi Chandrabose, Ana M Valencia, Meysam Raoufi, Nisreen Alshehri, Tracey M Clarke, Frédéric Laquai, Caterina Cocchi, Dieter Neher
Two-dimensional transition metal dichalcogenides (2D TMDCs) can be combined with organic semiconductors to form hybrid van der Waals heterostructures. Specially, non-fullerene acceptors (NFAs) stand out due to their excellent absorption and exciton diffusion properties. Here, we couple monolayer tungsten diselenide (ML-WSe2) with two well performing NFAs, ITIC, and IT-4F (fluorinated ITIC) to achieve hybrid architectures. Using steady state and time resolved spectroscopic techniques, we reveal sub-picosecond free charge generation in the heterostructure of ML-WSe2 with ITIC, where however, bimolecular recombination of spin uncorrelated charge carriers with possible contributions from geminate charge recombination cause rapid formation of low-lying triplet (T1) states in ITIC. Importantly, this unwanted process is effectively suppressed when the fluorinated derivative of ITIC, IT-4F, is deposited on ML-WSe2. We observe a similar scenario when replacing the ML-TMDC with copper thiocyanate (CuSCN) as the hole acceptor meaning that triplet state formation is not driven by the spin-orbit coupling of ML-WSe2. From ab initio calculations based on density functional theory, we interpret the high triplet formation in the ML-WSe2/ITIC hybrid bilayer due to changes in the nature and energies of the interfacial charge transfer (CT) levels. Our results highlight the delicate balance between excitons and charges in such inorganic/NFA heterostructures.
{"title":"Mitigating triplet loss in 2D WSe<sub>2</sub>/non-fullerene heterostructures using halogenated acceptors.","authors":"Sreelakshmi Chandrabose, Ana M Valencia, Meysam Raoufi, Nisreen Alshehri, Tracey M Clarke, Frédéric Laquai, Caterina Cocchi, Dieter Neher","doi":"10.1039/d4mh00894d","DOIUrl":"https://doi.org/10.1039/d4mh00894d","url":null,"abstract":"<p><p>Two-dimensional transition metal dichalcogenides (2D TMDCs) can be combined with organic semiconductors to form hybrid van der Waals heterostructures. Specially, non-fullerene acceptors (NFAs) stand out due to their excellent absorption and exciton diffusion properties. Here, we couple monolayer tungsten diselenide (ML-WSe<sub>2</sub>) with two well performing NFAs, ITIC, and IT-4F (fluorinated ITIC) to achieve hybrid architectures. Using steady state and time resolved spectroscopic techniques, we reveal sub-picosecond free charge generation in the heterostructure of ML-WSe<sub>2</sub> with ITIC, where however, bimolecular recombination of spin uncorrelated charge carriers with possible contributions from geminate charge recombination cause rapid formation of low-lying triplet (T<sub>1</sub>) states in ITIC. Importantly, this unwanted process is effectively suppressed when the fluorinated derivative of ITIC, IT-4F, is deposited on ML-WSe<sub>2</sub>. We observe a similar scenario when replacing the ML-TMDC with copper thiocyanate (CuSCN) as the hole acceptor meaning that triplet state formation is not driven by the spin-orbit coupling of ML-WSe<sub>2</sub>. From <i>ab initio</i> calculations based on density functional theory, we interpret the high triplet formation in the ML-WSe<sub>2</sub>/ITIC hybrid bilayer due to changes in the nature and energies of the interfacial charge transfer (CT) levels. Our results highlight the delicate balance between excitons and charges in such inorganic/NFA heterostructures.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":12.2,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142996539","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}
Baoqi Li, Mingcong Xu, Bang An, Wenye Sun, Rui Teng, Sha Luo, Chunhui Ma, Zhijun Chen, Jian Li, Wei Li, Shouxin Liu
Dynamic responsive structural colored materials have drawn increased consideration in a wide range of applications, such as colorimetric sensors and high-safety tags. However, the sophisticated interactions among the individual responsive parts restrict the advanced design of multimodal responsive photonic materials. Inspired by stimuli-responsive color change in chameleon skin, a simple and effective photo-crosslinking strategy is proposed to construct hydroxypropyl cellulose (HPC) based hydrogels with multiple responsive structured colors. By controlling UV exposure time, the structural color of HPC hydrogels can be effectively controlled in a full-color spectrum. At the same time, HPC hydrogels showcase temperature and mechanical dual-responsive structural colors. In particular, the microstructure of HPC hydrogels undergoes a transition from the chiral nematic phase to the nematic phase under the action of external stretching, leading to a significant reflection of circularly polarized light (CPL) to linearly polarized light (LPL). Given the diverse responsiveness exhibited by HPC hydrogels and their unique structural transition properties under external forces, we have explored their potential applications as dynamic anti-counterfeiting labels and optical skins. This work reveals the great possibility of using structural colored cellulose hydrogels in multi-sensing and optical displays, opening up a new path for the exploration of next-generation flexible photonic devices.
{"title":"Mechanical and thermal responsive chiral photonic cellulose hydrogels for dynamic anti-counterfeiting and optical skin.","authors":"Baoqi Li, Mingcong Xu, Bang An, Wenye Sun, Rui Teng, Sha Luo, Chunhui Ma, Zhijun Chen, Jian Li, Wei Li, Shouxin Liu","doi":"10.1039/d4mh01646g","DOIUrl":"https://doi.org/10.1039/d4mh01646g","url":null,"abstract":"<p><p>Dynamic responsive structural colored materials have drawn increased consideration in a wide range of applications, such as colorimetric sensors and high-safety tags. However, the sophisticated interactions among the individual responsive parts restrict the advanced design of multimodal responsive photonic materials. Inspired by stimuli-responsive color change in chameleon skin, a simple and effective photo-crosslinking strategy is proposed to construct hydroxypropyl cellulose (HPC) based hydrogels with multiple responsive structured colors. By controlling UV exposure time, the structural color of HPC hydrogels can be effectively controlled in a full-color spectrum. At the same time, HPC hydrogels showcase temperature and mechanical dual-responsive structural colors. In particular, the microstructure of HPC hydrogels undergoes a transition from the chiral nematic phase to the nematic phase under the action of external stretching, leading to a significant reflection of circularly polarized light (CPL) to linearly polarized light (LPL). Given the diverse responsiveness exhibited by HPC hydrogels and their unique structural transition properties under external forces, we have explored their potential applications as dynamic anti-counterfeiting labels and optical skins. This work reveals the great possibility of using structural colored cellulose hydrogels in multi-sensing and optical displays, opening up a new path for the exploration of next-generation flexible photonic devices.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":12.2,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142996535","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}
Given that optical thermometers are widely used due to their unique advantages, this study aims to address critical challenges in existing technologies, such as insufficient sensitivity, limited temperature measurement ranges, and poor signal recognition capabilities. Herein, we develop a thermometer based on the fluorescence intensity ratio (FIR) of Sb-doped Cs2NaInCl6 (Cs2NaInCl6:Sb). As the temperature increases from 203 to 323 K, the thermally induced transition from triplet to singlet self-trapped excitons (STEs) leads to enhanced 455 nm photoluminescence (PL) from singlet STE recombination. Thus, the FIR monotonically depends on temperature, allowing for temperature sensing with a high absolute sensitivity (SA) of 0.0575 K-1 and the maximum relative sensitivity (SR) of 1.005% K-1. We demonstrate that spatial temperature distribution can be measured by mapping the PL spectra, even with a transparent medium screening the target. Furthermore, blue emissive Cs2NaInCl6:Sb is mixed with yellow emissive Cs2AgInCl6:Sb with a thermal quenching feature. The fluorescence color of the mixture dramatically depends on temperature, enabling a user-friendly colorimetric temperature sensing. Therefore, two operational modes are proposed to meet various practical application demands.
{"title":"Highly sensitive temperature sensors based on the fluorescence intensity ratio of dual-emissive lead-free metal halides.","authors":"Jianhui Zhao, Yunsong Di, Yuhang Sheng, Jiaxin Sui, Xingru Yang, Yi Zhang, Ying Wang, Haoyu Wang, Xiaowei Zhang, Liyan Yu, Zhihui Chen, Zhixing Gan","doi":"10.1039/d4mh01369g","DOIUrl":"https://doi.org/10.1039/d4mh01369g","url":null,"abstract":"<p><p>Given that optical thermometers are widely used due to their unique advantages, this study aims to address critical challenges in existing technologies, such as insufficient sensitivity, limited temperature measurement ranges, and poor signal recognition capabilities. Herein, we develop a thermometer based on the fluorescence intensity ratio (FIR) of Sb-doped Cs<sub>2</sub>NaInCl<sub>6</sub> (Cs<sub>2</sub>NaInCl<sub>6</sub>:Sb). As the temperature increases from 203 to 323 K, the thermally induced transition from triplet to singlet self-trapped excitons (STEs) leads to enhanced 455 nm photoluminescence (PL) from singlet STE recombination. Thus, the FIR monotonically depends on temperature, allowing for temperature sensing with a high absolute sensitivity (<i>S</i><sub>A</sub>) of 0.0575 K<sup>-1</sup> and the maximum relative sensitivity (<i>S</i><sub>R</sub>) of 1.005% K<sup>-1</sup>. We demonstrate that spatial temperature distribution can be measured by mapping the PL spectra, even with a transparent medium screening the target. Furthermore, blue emissive Cs<sub>2</sub>NaInCl<sub>6</sub>:Sb is mixed with yellow emissive Cs<sub>2</sub>AgInCl<sub>6</sub>:Sb with a thermal quenching feature. The fluorescence color of the mixture dramatically depends on temperature, enabling a user-friendly colorimetric temperature sensing. Therefore, two operational modes are proposed to meet various practical application demands.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":12.2,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142982155","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}