Pengwei Wang, Zhiping Hu, Peixi Cong, Fengxian Zhou, Qi Yue, Zixiao Xue, Chenfang Lin, Ying Jiang, Juan Du, Anlian Pan, Long Zhang, Jiabin Cui, Jin He
Nano‐confined synthesis of perovskite quantum dots (QDs) in solid matrix is emerging as a promising route to solve their long‐standing stability problem. Utilizing sol‐gel derived nanoporous glass as matrix that has high flexibility in chemical composition and pore size, a novel spatial and chemical dual nano‐confined strategy is presented for the synthesis of ultrastable perovskite QDs with tunable composition and bandgap in glass. The findings reveal that the Pb─O bonding is formed at perovskite QDs/glass interface during a nano‐confined chemical vapor deposition (CVD) reaction. In particular, the presence of interfacial chemical bonding is discovered to be critical for passivating surface traps and stabilizing the perovskite QDs during the final densification process (related photoluminescence intensity maintained ≈100% after immersed in aqueous solution for 30 days). Series optical spectroscopy unravels the exciton modulation (80 meV) of perovskite QDs in nanoporous and densified glass related to the unique combination of dual physical and chemistry nano‐confined effect. By shedding light on the nano‐confined growth of functional nanocrystals, the research offers the key paths for fabricating high‐performance perovskite devices.
{"title":"Spatial and Chemical Dual Nano‐Confined Ultrastable Perovskite Quantum Dots Glass Manifesting Exciton Modulation","authors":"Pengwei Wang, Zhiping Hu, Peixi Cong, Fengxian Zhou, Qi Yue, Zixiao Xue, Chenfang Lin, Ying Jiang, Juan Du, Anlian Pan, Long Zhang, Jiabin Cui, Jin He","doi":"10.1002/adom.202400630","DOIUrl":"https://doi.org/10.1002/adom.202400630","url":null,"abstract":"Nano‐confined synthesis of perovskite quantum dots (QDs) in solid matrix is emerging as a promising route to solve their long‐standing stability problem. Utilizing sol‐gel derived nanoporous glass as matrix that has high flexibility in chemical composition and pore size, a novel spatial and chemical dual nano‐confined strategy is presented for the synthesis of ultrastable perovskite QDs with tunable composition and bandgap in glass. The findings reveal that the Pb─O bonding is formed at perovskite QDs/glass interface during a nano‐confined chemical vapor deposition (CVD) reaction. In particular, the presence of interfacial chemical bonding is discovered to be critical for passivating surface traps and stabilizing the perovskite QDs during the final densification process (related photoluminescence intensity maintained ≈100% after immersed in aqueous solution for 30 days). Series optical spectroscopy unravels the exciton modulation (80 meV) of perovskite QDs in nanoporous and densified glass related to the unique combination of dual physical and chemistry nano‐confined effect. By shedding light on the nano‐confined growth of functional nanocrystals, the research offers the key paths for fabricating high‐performance perovskite devices.","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":null,"pages":null},"PeriodicalIF":9.0,"publicationDate":"2024-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141355075","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}
Metal nanoclusters with aggregation‐induced emission (AIE) characteristics are potential nanomaterial candidates for a wide array of advanced optical applications. In this study, a novel self‐assembly enhanced AIE strategy utilizing 6‐thioguanine (TG)‐protected gold nanoclusters (AuNCs) is fabricated with dual‐stimuli responsive modes of excitation wavelength‐dependent (Ex‐De) emission and mechanochromic properties. The sheetlike structures of AuNCs self‐assembly (AuNC sheets) with typical AIE characteristics are generated in bad solvent owing to the intermolecular hydrogen‐bonds interaction among guanine‐rich moieties of TG ligand. Interestingly, the maximum emission peaks of AuNC sheets are red‐shifted with the increased excitation wavelengths, indicating Ex‐De emission behavior. This phenomenon enables the achievement of wide‐range tunable photoluminescence (PL). In addition, the emission peak of AuNC sheets powders before and after grinding displays the bathochromic shift of 110 nm. The “off–on” switch of Ex‐De emission behavior in AuNC sheets can be manipulated by changing mechanical pressure. It is speculated that the tunable PL behavior of AuNC sheets originates from multiple excited states due to the existence of different Au(I)···Au(I) distances. The self‐assembly‐driven AIE strategy of AuNCs with stimuli‐responsive allochroic modes will facilitate the recording of rewritable information, opening up a new avenue for high‐throughput and multi‐dimensional optical security.
{"title":"Assembly‐Driven Aggregation‐Induced Emission of Gold Nanoclusters with Excitation Wavelength‐Dependent Emission and Mechanochromic Property","authors":"Yuanyuan Huang, Xiaofei Han, Li Wang, Renjun Pei","doi":"10.1002/adom.202400078","DOIUrl":"https://doi.org/10.1002/adom.202400078","url":null,"abstract":"Metal nanoclusters with aggregation‐induced emission (AIE) characteristics are potential nanomaterial candidates for a wide array of advanced optical applications. In this study, a novel self‐assembly enhanced AIE strategy utilizing 6‐thioguanine (TG)‐protected gold nanoclusters (AuNCs) is fabricated with dual‐stimuli responsive modes of excitation wavelength‐dependent (Ex‐De) emission and mechanochromic properties. The sheetlike structures of AuNCs self‐assembly (AuNC sheets) with typical AIE characteristics are generated in bad solvent owing to the intermolecular hydrogen‐bonds interaction among guanine‐rich moieties of TG ligand. Interestingly, the maximum emission peaks of AuNC sheets are red‐shifted with the increased excitation wavelengths, indicating Ex‐De emission behavior. This phenomenon enables the achievement of wide‐range tunable photoluminescence (PL). In addition, the emission peak of AuNC sheets powders before and after grinding displays the bathochromic shift of 110 nm. The “off–on” switch of Ex‐De emission behavior in AuNC sheets can be manipulated by changing mechanical pressure. It is speculated that the tunable PL behavior of AuNC sheets originates from multiple excited states due to the existence of different Au(I)···Au(I) distances. The self‐assembly‐driven AIE strategy of AuNCs with stimuli‐responsive allochroic modes will facilitate the recording of rewritable information, opening up a new avenue for high‐throughput and multi‐dimensional optical security.","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":null,"pages":null},"PeriodicalIF":9.0,"publicationDate":"2024-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141357359","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}
Chenyang Zhan, Haomiao Zhu, Sisi Liang, Wendong Nie, Zihao Wang, Maochun Hong
Transition metal ions, such as Cr3+, Fe3+, and Ni2+, are widely recognized activators for efficient broadband near‐infrared (NIR) phosphors. However, the potential of Mn2+ ions as NIR‐emitting activators is relatively overlooked due to their typically narrowband emission in the visible spectral region and relatively weak absorption. Herein, a heavy Mn2+‐doped Zn1‐xAl2O4: xMn2+ (ZAO: xMn2+) phosphor is presented that exhibits a single NIR emission band peaked at 830 nm with a bandwidth of 135 nm under excitation at 450 nm. Through comprehensive structural and spectral analysis, this NIR band is attributed to the emission originating from Mn2+ ions within the MnO6 octahedra. Importantly, the formation of Mn2+–Mn2+ dimers breaks the spin‐forbidden rule and significantly enhances the transition probability, as supported by the excited state dynamic analysis. Consequently, the optimal ZAO: 0.70Mn2+ sample shows high internal/external photoluminescence quantum yields of 85.8%/36.9%, along with good thermal stability demonstrated by the emission intensity at 423 K retains 60% of that at 298 K. Finally, a prototype NIR pc‐LED device is fabricated by combining ZAO: 0.70Mn2+ phosphor with a 450 nm blue diode chip, generating an NIR output power of 28.84 mW at 100 mA. This study provides novel insights into high‐performance Mn2+‐activated NIR phosphors.
{"title":"Mn2+–Mn2+ Dimers Induced Robust Light Absorption in Heavy Mn2+ Doped ZnAl2O4 Near‐Infrared Phosphor with an Excellent Photoluminescence Quantum Yield and Thermal Stability","authors":"Chenyang Zhan, Haomiao Zhu, Sisi Liang, Wendong Nie, Zihao Wang, Maochun Hong","doi":"10.1002/adom.202400574","DOIUrl":"https://doi.org/10.1002/adom.202400574","url":null,"abstract":"Transition metal ions, such as Cr3+, Fe3+, and Ni2+, are widely recognized activators for efficient broadband near‐infrared (NIR) phosphors. However, the potential of Mn2+ ions as NIR‐emitting activators is relatively overlooked due to their typically narrowband emission in the visible spectral region and relatively weak absorption. Herein, a heavy Mn2+‐doped Zn1‐xAl2O4: xMn2+ (ZAO: xMn2+) phosphor is presented that exhibits a single NIR emission band peaked at 830 nm with a bandwidth of 135 nm under excitation at 450 nm. Through comprehensive structural and spectral analysis, this NIR band is attributed to the emission originating from Mn2+ ions within the MnO6 octahedra. Importantly, the formation of Mn2+–Mn2+ dimers breaks the spin‐forbidden rule and significantly enhances the transition probability, as supported by the excited state dynamic analysis. Consequently, the optimal ZAO: 0.70Mn2+ sample shows high internal/external photoluminescence quantum yields of 85.8%/36.9%, along with good thermal stability demonstrated by the emission intensity at 423 K retains 60% of that at 298 K. Finally, a prototype NIR pc‐LED device is fabricated by combining ZAO: 0.70Mn2+ phosphor with a 450 nm blue diode chip, generating an NIR output power of 28.84 mW at 100 mA. This study provides novel insights into high‐performance Mn2+‐activated NIR phosphors.","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":null,"pages":null},"PeriodicalIF":9.0,"publicationDate":"2024-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141356078","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}
Chaojun Yang, Xiangdan Tian, Guangguang Huang, Xinyang Xiong, Kaiwei Sun, Bo Zhang, Shujie Wang, Zuliang Du
Cesium zirconium halide (e.g., Cs2ZrCl6:Te or CZCT) perovskites have garnered significant interest due to their unique optical properties. However, there have been no reports of CZCT perovskite nanoparticles (PNPs) that simultaneously offer high efficiency and thermal stability. Here, a comprehensive defect suppression strategy is reported to achieve CZCT PNPs with these attributes. First, the inner defects of CZCT perovskite microcrystals (PMCs) are minimized by controlling crystallization kinetics precisely. Second, the PNPs are obtained from PMCs via top‐down fabrication, and the surface defects of PNPs are passivated via the hydroxyl groups of alkyl‐terminated silica‐oligomer shell (ASO). The resulting CZCT@ASO PNPs show the highest photoluminescence quantum yield (PLQY) of 96% and high thermal stability among the reported conventional CZCT emitters. Finally, white light‐emitting diodes (WLEDs) are integrated by using CZCT@ASO PNPs as the down‐color converters, achieving a color coordinate of (0.31, 0.33) and a color rendering index of 86. These results demonstrate that core/shell CZCT@ASO PNPs have great potential as phosphors for lighting applications.
{"title":"Comprehensive Defect Suppression in Te‐Doped Cs2ZrCl6 Perovskite Nanoparticles for Highly Efficient and Thermally Stable White Light‐Emitting Diodes","authors":"Chaojun Yang, Xiangdan Tian, Guangguang Huang, Xinyang Xiong, Kaiwei Sun, Bo Zhang, Shujie Wang, Zuliang Du","doi":"10.1002/adom.202303079","DOIUrl":"https://doi.org/10.1002/adom.202303079","url":null,"abstract":"Cesium zirconium halide (e.g., Cs2ZrCl6:Te or CZCT) perovskites have garnered significant interest due to their unique optical properties. However, there have been no reports of CZCT perovskite nanoparticles (PNPs) that simultaneously offer high efficiency and thermal stability. Here, a comprehensive defect suppression strategy is reported to achieve CZCT PNPs with these attributes. First, the inner defects of CZCT perovskite microcrystals (PMCs) are minimized by controlling crystallization kinetics precisely. Second, the PNPs are obtained from PMCs via top‐down fabrication, and the surface defects of PNPs are passivated via the hydroxyl groups of alkyl‐terminated silica‐oligomer shell (ASO). The resulting CZCT@ASO PNPs show the highest photoluminescence quantum yield (PLQY) of 96% and high thermal stability among the reported conventional CZCT emitters. Finally, white light‐emitting diodes (WLEDs) are integrated by using CZCT@ASO PNPs as the down‐color converters, achieving a color coordinate of (0.31, 0.33) and a color rendering index of 86. These results demonstrate that core/shell CZCT@ASO PNPs have great potential as phosphors for lighting applications.","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":null,"pages":null},"PeriodicalIF":9.0,"publicationDate":"2024-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141358572","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}
The design of near‐infrared photosensitizers with high photodynamic and photothermal synergistic therapeutic properties is of great significance for tumor therapy. In this study, An‐cyclic‐BDP with excellent near‐infrared absorption (ε = 1.94 × 105 m−1 cm−1 at 804 nm) is prepared using a dual strategy of twisted π‐conjugated system induction (T‐π‐CSI) and spin‐orbit charge transfer (SOCT). Theoretical calculations, steady‐state and transient absorption spectra are used to investigate the intrinsic regulatory mechanisms between molecular structure and intersystem crossing (ISC) capacity. The results indicate that the application of the T‐π‐CSI and SOCT approach can be superimposed to increase ISC capacity and the triplet lifetime of An‐cyclic‐BDP (τ = 2961 ps). Electron paramagnetic resonance (EPR) results confirm that An‐cyclic‐BDP has the ability to generate hydroxyl radical (·OH) and singlet oxygen (1O2). Furthermore, the calculated 1O2 yield of An‐cyclic‐BDP is found to be 13%. The experimental results of the photothermal conversion indicates that An‐cyclic‐BDP exhibits a photothermal conversion efficiency of up to 48%. In vitro cell experiments demonstrate that An‐cyclic‐BDP‐NPs, constructed by encapsulating An‐cyclic‐BDP with DSPE‐mPEG2000, exhibit excellent biocompatibility and tumor cell‐killing ability. Therefore, the strong near‐IR absorption photosensitizer prepared in this study exhibits significant potential for application in the area of photodynamic and photothermal synergistic therapy.
{"title":"Construction and Properties of Strong Near‐IR Absorption Photosensitizers","authors":"Fei Cheng, Taotao Qiang, Tony D. James","doi":"10.1002/adom.202401012","DOIUrl":"https://doi.org/10.1002/adom.202401012","url":null,"abstract":"The design of near‐infrared photosensitizers with high photodynamic and photothermal synergistic therapeutic properties is of great significance for tumor therapy. In this study, An‐cyclic‐BDP with excellent near‐infrared absorption (ε = 1.94 × 105 m−1 cm−1 at 804 nm) is prepared using a dual strategy of twisted π‐conjugated system induction (T‐π‐CSI) and spin‐orbit charge transfer (SOCT). Theoretical calculations, steady‐state and transient absorption spectra are used to investigate the intrinsic regulatory mechanisms between molecular structure and intersystem crossing (ISC) capacity. The results indicate that the application of the T‐π‐CSI and SOCT approach can be superimposed to increase ISC capacity and the triplet lifetime of An‐cyclic‐BDP (τ = 2961 ps). Electron paramagnetic resonance (EPR) results confirm that An‐cyclic‐BDP has the ability to generate hydroxyl radical (·OH) and singlet oxygen (1O2). Furthermore, the calculated 1O2 yield of An‐cyclic‐BDP is found to be 13%. The experimental results of the photothermal conversion indicates that An‐cyclic‐BDP exhibits a photothermal conversion efficiency of up to 48%. In vitro cell experiments demonstrate that An‐cyclic‐BDP‐NPs, constructed by encapsulating An‐cyclic‐BDP with DSPE‐mPEG2000, exhibit excellent biocompatibility and tumor cell‐killing ability. Therefore, the strong near‐IR absorption photosensitizer prepared in this study exhibits significant potential for application in the area of photodynamic and photothermal synergistic therapy.","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":null,"pages":null},"PeriodicalIF":9.0,"publicationDate":"2024-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141359953","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}
Juri Kim, Hyejeong Yeon, Hye‐Ryung Choi, Soon Mo Park, Chang-Hun Huh, Kyung Cheol Choi, D. Yoon
Herein, an organic light–emitting diode (OLED) is fabricated with increased luminous efficiency and biocompatibility by topographic DNA film. In addition to the natural abundance and biocompatibility of DNA, its semi‐flexible characteristics facilitated the emergence of the liquid crystal phase, allowing the formation of a periodic wavy undulation structure by applying shear force. The resultant zigzag structure possesses sufficient periodicity and roughness, enhancing the effective scattering of emitted light. Furthermore, the DNA‐coated red OLED demonstrates cell proliferative effects and exhibits high electrical and thermal stability even in a bent state, suggesting its potential application in attachable OLED‐based light therapy.
在此，我们利用拓扑 DNA 薄膜制造出了发光效率更高、生物相容性更好的有机发光二极管（OLED）。除了 DNA 的天然丰富性和生物兼容性之外，其半柔性的特性还有助于液晶相的出现，从而可以通过施加剪切力形成周期性的波浪起伏结构。由此形成的 "之 "字形结构具有足够的周期性和粗糙度，从而增强了对发射光的有效散射。此外，DNA 涂层红色 OLED 还具有细胞增殖效应，即使在弯曲状态下也表现出很高的电稳定性和热稳定性，这表明它有望应用于基于可附着 OLED 的光疗。
{"title":"Highly Efficient Organic Light–Emitting Diode Using DNA as Scattering Layer","authors":"Juri Kim, Hyejeong Yeon, Hye‐Ryung Choi, Soon Mo Park, Chang-Hun Huh, Kyung Cheol Choi, D. Yoon","doi":"10.1002/adom.202400702","DOIUrl":"https://doi.org/10.1002/adom.202400702","url":null,"abstract":"Herein, an organic light–emitting diode (OLED) is fabricated with increased luminous efficiency and biocompatibility by topographic DNA film. In addition to the natural abundance and biocompatibility of DNA, its semi‐flexible characteristics facilitated the emergence of the liquid crystal phase, allowing the formation of a periodic wavy undulation structure by applying shear force. The resultant zigzag structure possesses sufficient periodicity and roughness, enhancing the effective scattering of emitted light. Furthermore, the DNA‐coated red OLED demonstrates cell proliferative effects and exhibits high electrical and thermal stability even in a bent state, suggesting its potential application in attachable OLED‐based light therapy.","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":null,"pages":null},"PeriodicalIF":9.0,"publicationDate":"2024-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141357320","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 demonstrates effective manipulation of exciton spin dynamics in a prototypical chiral inorganic nanosystem, i.e., cadmium selenide (CdSe) nanosheets capped with chiral cysteine ligands in aqueous solution, via facile pH‐regulation that can directly modify the electronic coupling between CdSe and cysteine's thiol group through Cd─S bonding. The comparative scrutiny by using transient circular dichroism spectroscopy enables to decipher the pertinent mechanisms behind the pH‐regulated spin‐flip dynamics. The hole‐trapping interaction between the valence‐band heavy‐hole spin state of CdSe and the cysteine‐induced “extrinsic” surface state is found to play a dominant role in prolonging the hole spin relaxation lifetime (by more than threefold). This study also demonstrates a relevant application in modulating the sensitivity of circularly polarized light detection. This work sets a paradigm for harnessing the elusive interactions in chiral inorganic nanosystems to achieve desired spin‐polarization regulation, refreshing the fundamental understanding about the mechanisms of spin dynamics involved therein.
{"title":"Manipulation and Mechanistic Understanding of Exciton Spin Dynamics in a Chiral Inorganic Nanosystem via Facile pH‐Regulation","authors":"Qinglong Wu, Shenlong Jiang, Qun Zhang, Yi Luo","doi":"10.1002/adom.202400583","DOIUrl":"https://doi.org/10.1002/adom.202400583","url":null,"abstract":"This study demonstrates effective manipulation of exciton spin dynamics in a prototypical chiral inorganic nanosystem, i.e., cadmium selenide (CdSe) nanosheets capped with chiral cysteine ligands in aqueous solution, via facile pH‐regulation that can directly modify the electronic coupling between CdSe and cysteine's thiol group through Cd─S bonding. The comparative scrutiny by using transient circular dichroism spectroscopy enables to decipher the pertinent mechanisms behind the pH‐regulated spin‐flip dynamics. The hole‐trapping interaction between the valence‐band heavy‐hole spin state of CdSe and the cysteine‐induced “extrinsic” surface state is found to play a dominant role in prolonging the hole spin relaxation lifetime (by more than threefold). This study also demonstrates a relevant application in modulating the sensitivity of circularly polarized light detection. This work sets a paradigm for harnessing the elusive interactions in chiral inorganic nanosystems to achieve desired spin‐polarization regulation, refreshing the fundamental understanding about the mechanisms of spin dynamics involved therein.","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":null,"pages":null},"PeriodicalIF":9.0,"publicationDate":"2024-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141356332","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}
To boost the power conversion efficiency of silicon/perovskite tandem solar cells, pyramid‐textured structures have been investigated and introduced into devices. However, high‐quality pyramid‐shaped single crystal preparation is an obstacle in tandem device development. Perovskite crystals obtained using general methods are cubic because of their structural symmetry and rapid growth rate. In this study, based on mass transfer boundary layer theory, a pyramid‐shaped perovskite single crystal is successfully obtained using an asymmetrically spatial confinement‐induced crystallization method. The synthesized pyramid crystals exhibited high crystallinity and enhanced optical absorption. A photodetector constructed using the as‐grown crystal exhibited high‐performance properties, including a responsivity of 9.4 A W−1, photo‐to‐dark current ratio of 2.3 × 104, and detectivity of 2.1 × 1011 Jones. Its unique insensitivity to the incident photon direction is also characterized. The flexible photodetector also exhibited excellent responsivity under different bending curvature radii. Additionally, the light‐trapping effect and absorption superiority of pyramid crystals over cuboid crystals are well established based on a semi‐empirical analytical model. This breakthrough in pyramid‐shaped perovskite crystal preparation provides a promising approach for the development of novel tandem solar cells and other optoelectronic devices.
为了提高硅/透闪石串联太阳能电池的功率转换效率，人们对金字塔纹理结构进行了研究，并将其引入到设备中。然而，高质量金字塔形单晶的制备是串联设备开发的一个障碍。采用一般方法获得的包光体晶体为立方体，因为其结构对称且生长速度快。本研究基于传质边界层理论，采用非对称空间约束诱导结晶方法，成功获得了金字塔形的透辉石单晶。合成的金字塔晶体具有很高的结晶度和更强的光吸收能力。利用该晶体生长的光电探测器表现出高性能特性，包括 9.4 A W-1、2.3 × 104 的光暗电流比和 2.1 × 1011 Jones 的检测率。此外，它还具有对入射光子方向不敏感的独特特性。这种柔性光电探测器在不同的弯曲曲率半径下也表现出卓越的响应性。此外，基于半经验分析模型，金字塔晶体的光捕获效应和吸收能力优于立方体晶体。金字塔形包晶石晶体制备技术的这一突破为新型串联太阳能电池和其他光电器件的开发提供了一种前景广阔的方法。
{"title":"Pyramid‐Shaped Perovskite Single‐Crystal Growth and Application for High‐Performance Photodetector","authors":"Xiaoyan Li, Chen Shao, Yipeng Zhao, Gang Ouyang, Wei Hu, Jianfa Zhang","doi":"10.1002/adom.202400329","DOIUrl":"https://doi.org/10.1002/adom.202400329","url":null,"abstract":"To boost the power conversion efficiency of silicon/perovskite tandem solar cells, pyramid‐textured structures have been investigated and introduced into devices. However, high‐quality pyramid‐shaped single crystal preparation is an obstacle in tandem device development. Perovskite crystals obtained using general methods are cubic because of their structural symmetry and rapid growth rate. In this study, based on mass transfer boundary layer theory, a pyramid‐shaped perovskite single crystal is successfully obtained using an asymmetrically spatial confinement‐induced crystallization method. The synthesized pyramid crystals exhibited high crystallinity and enhanced optical absorption. A photodetector constructed using the as‐grown crystal exhibited high‐performance properties, including a responsivity of 9.4 A W−1, photo‐to‐dark current ratio of 2.3 × 104, and detectivity of 2.1 × 1011 Jones. Its unique insensitivity to the incident photon direction is also characterized. The flexible photodetector also exhibited excellent responsivity under different bending curvature radii. Additionally, the light‐trapping effect and absorption superiority of pyramid crystals over cuboid crystals are well established based on a semi‐empirical analytical model. This breakthrough in pyramid‐shaped perovskite crystal preparation provides a promising approach for the development of novel tandem solar cells and other optoelectronic devices.","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":null,"pages":null},"PeriodicalIF":9.0,"publicationDate":"2024-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141360744","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}
Tuhin Samanta, Amar Nath Yadav, Joo Hyeong Han, Minji Kim, Sung Woo Jang, N. Viswanath, Won Bin Im
Recently, lanthanide‐based 0D metal halides have garnered considerable attention owing to their applications in light–emitting diodes (LEDs), X‐ray imaging, and photodetectors. Among these materials, 0D Cs3TbCl6 (CTC) nanocrystals (NCs) have demonstrated promising performance in X‐ray imaging and light‐emitting diodes. However, a considerable drawback of CTC NCs is their limited absorption coefficient in the UV‐A region (315–380 nm). To address this limitation and enhance the absorption coefficient in the UV‐A region, Ce3+ is incorporated into CTC NCs—advantageous owing to the high absorption coefficient of Ce3+ in the UV‐A region, attributed to—4f‐5d orbital coupling. In addition, Ce3+ ions sensitize the luminescence of CTC NCs and enhance the photoluminescence quantum yield from 75% to 87%. Energy transfer from Ce3+ to Tb3+ is investigated at different dopant ratios. Furthermore, Cs3CeTbCl6 (CCTC) NCs have been utilized in white LED devices. Understanding such competitive energy transfer in lanthanide‐based perovskite‐inspired metal halides will facilitate the development of novel luminescent metal halides for lighting applications.
{"title":"Cerium‐Sensitized Highly Emissive 0D Cesium Cerium Terbium Chloride Alloy Nanocrystals for White Light Emission","authors":"Tuhin Samanta, Amar Nath Yadav, Joo Hyeong Han, Minji Kim, Sung Woo Jang, N. Viswanath, Won Bin Im","doi":"10.1002/adom.202400909","DOIUrl":"https://doi.org/10.1002/adom.202400909","url":null,"abstract":"Recently, lanthanide‐based 0D metal halides have garnered considerable attention owing to their applications in light–emitting diodes (LEDs), X‐ray imaging, and photodetectors. Among these materials, 0D Cs3TbCl6 (CTC) nanocrystals (NCs) have demonstrated promising performance in X‐ray imaging and light‐emitting diodes. However, a considerable drawback of CTC NCs is their limited absorption coefficient in the UV‐A region (315–380 nm). To address this limitation and enhance the absorption coefficient in the UV‐A region, Ce3+ is incorporated into CTC NCs—advantageous owing to the high absorption coefficient of Ce3+ in the UV‐A region, attributed to—4f‐5d orbital coupling. In addition, Ce3+ ions sensitize the luminescence of CTC NCs and enhance the photoluminescence quantum yield from 75% to 87%. Energy transfer from Ce3+ to Tb3+ is investigated at different dopant ratios. Furthermore, Cs3CeTbCl6 (CCTC) NCs have been utilized in white LED devices. Understanding such competitive energy transfer in lanthanide‐based perovskite‐inspired metal halides will facilitate the development of novel luminescent metal halides for lighting applications.","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":null,"pages":null},"PeriodicalIF":9.0,"publicationDate":"2024-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141356547","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}
Organic optical waveguide materials have attracted considerable attention for their promising applications in photonic and optoelectronic devices. However, for most materials, excellent light‐loss properties at high temperature cannot be obtained due to many factors. Consequently, realizing efficient optical waveguide materials that perform well at elevated temperatures remains a significant challenge. In this study, relying on the luminescent properties and self‐assembly properties of luminescent liquid crystals (LLCs), successfully fabricated materials are present for highly efficient active optical waveguides. A systematically synthesized set of LLCs with different structures is named according to the substituent type and the position of the cyano group, namely α‐DECN, α‐DEEOCN, β‐DECN, and β‐DEEOCN. Notably, α‐DECN and β‐DECN reveal hexagonal columnar phase, while α‐DEEOCN and β‐DEEOCN exhibit smectic phase. Optical waveguide experiments have revealed that the obtained LLCs showed highly efficient optical waveguide behavior, where the lowest light loss reached 0.15 dB mm−1 at room temperature. Remarkably, these LLCs show even lower light loss at high temperatures, with the light loss reaching 0.11 dB mm−1 as the lowest point. Further experimental results indicate that this phenomenon is attributed to the change in the dipole moment of these molecules. This research forms a significant groundwork for advanced exploration in optical waveguide material.
{"title":"Dynamic Dipole Moment of Luminescent Liquid Crystals Enabled Highly Efficient Active Waveguide Materials Design and Synthesis","authors":"Jin‐Kang Chen, Yu Cao, Akhila Joy, Jie Li, Tian‐Tian Hao, Jiang Huang, Xiao Li, Feng Liu, He‐Lou Xie","doi":"10.1002/adom.202400726","DOIUrl":"https://doi.org/10.1002/adom.202400726","url":null,"abstract":"Organic optical waveguide materials have attracted considerable attention for their promising applications in photonic and optoelectronic devices. However, for most materials, excellent light‐loss properties at high temperature cannot be obtained due to many factors. Consequently, realizing efficient optical waveguide materials that perform well at elevated temperatures remains a significant challenge. In this study, relying on the luminescent properties and self‐assembly properties of luminescent liquid crystals (LLCs), successfully fabricated materials are present for highly efficient active optical waveguides. A systematically synthesized set of LLCs with different structures is named according to the substituent type and the position of the cyano group, namely α‐DECN, α‐DEEOCN, β‐DECN, and β‐DEEOCN. Notably, α‐DECN and β‐DECN reveal hexagonal columnar phase, while α‐DEEOCN and β‐DEEOCN exhibit smectic phase. Optical waveguide experiments have revealed that the obtained LLCs showed highly efficient optical waveguide behavior, where the lowest light loss reached 0.15 dB mm−1 at room temperature. Remarkably, these LLCs show even lower light loss at high temperatures, with the light loss reaching 0.11 dB mm−1 as the lowest point. Further experimental results indicate that this phenomenon is attributed to the change in the dipole moment of these molecules. This research forms a significant groundwork for advanced exploration in optical waveguide material.","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":null,"pages":null},"PeriodicalIF":9.0,"publicationDate":"2024-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141363263","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}
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