Jindou Shi, Zeyu Wang, Luxia Xu, Junnan Wang, Zheyuan Da, Chen Zhang, Yongqiang Ji, Qing Yao, Youlong Xu, Nikolai V. Gaponenko, Jinshou Tian, Minqiang Wang
Pb‐free double‐perovskite (DP) scintillators are highly promising candidates for X‐ray imaging because of their superior optoelectronic properties, low toxicity, and high stability. However, practical applications require Pb‐free DP crystals to be ground and mixed with polymers to produce scintillator films. Grinding can compromise film uniformity and optical properties, thereby affecting imaging resolution. In this study, an in situ fabrication strategy is proposed to facilitate the crystalline growth of Pb‐free Cs2AgInxBi1‐xCl6 micron sheets in polymethyl methacrylate in a single step. By adjusting the In3+/Bi3+ ratio, Cs2AgIn0.9Bi0.1Cl6/PMMA composite films (CFs) with excellent scintillation properties are obtained, including a light yield of up to 32000 photons per MeV and an X‐ray detection limit of 87 nGyairs−1. This strategy also enabled the production of large Cs2AgIn0.9Bi0.1Cl6/PMMA CFs, which demonstrated favorable flexibility and stability, fabricating products with advanced eligibility for commercial applications. The CFs exhibited outstanding performances in X‐ray imaging, producing high‐resolution structures and providing a new avenue for the development of Pb‐free DP materials in fields such as medical imaging and safety detection.
{"title":"In Situ Growth of Lead‐Free Double Perovskite Micron Sheets in Polymethyl Methacrylate for X‐Ray Imaging","authors":"Jindou Shi, Zeyu Wang, Luxia Xu, Junnan Wang, Zheyuan Da, Chen Zhang, Yongqiang Ji, Qing Yao, Youlong Xu, Nikolai V. Gaponenko, Jinshou Tian, Minqiang Wang","doi":"10.1002/adom.202400691","DOIUrl":"https://doi.org/10.1002/adom.202400691","url":null,"abstract":"Pb‐free double‐perovskite (DP) scintillators are highly promising candidates for X‐ray imaging because of their superior optoelectronic properties, low toxicity, and high stability. However, practical applications require Pb‐free DP crystals to be ground and mixed with polymers to produce scintillator films. Grinding can compromise film uniformity and optical properties, thereby affecting imaging resolution. In this study, an in situ fabrication strategy is proposed to facilitate the crystalline growth of Pb‐free Cs<jats:sub>2</jats:sub>AgIn<jats:sub>x</jats:sub>Bi<jats:sub>1‐x</jats:sub>Cl<jats:sub>6</jats:sub> micron sheets in polymethyl methacrylate in a single step. By adjusting the In<jats:sup>3+</jats:sup>/Bi<jats:sup>3+</jats:sup> ratio, Cs<jats:sub>2</jats:sub>AgIn<jats:sub>0.9</jats:sub>Bi<jats:sub>0.1</jats:sub>Cl<jats:sub>6</jats:sub>/PMMA composite films (CFs) with excellent scintillation properties are obtained, including a light yield of up to 32000 photons per MeV and an X‐ray detection limit of 87 nGy<jats:sub>air</jats:sub>s<jats:sup>−1</jats:sup>. This strategy also enabled the production of large Cs<jats:sub>2</jats:sub>AgIn<jats:sub>0.9</jats:sub>Bi<jats:sub>0.1</jats:sub>Cl<jats:sub>6</jats:sub>/PMMA CFs, which demonstrated favorable flexibility and stability, fabricating products with advanced eligibility for commercial applications. The CFs exhibited outstanding performances in X‐ray imaging, producing high‐resolution structures and providing a new avenue for the development of Pb‐free DP materials in fields such as medical imaging and safety detection.","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":null,"pages":null},"PeriodicalIF":9.0,"publicationDate":"2024-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141511782","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}
Ultrafast vortex beams have significant scientific and practical value because of their unique phase properties in both the longitudinal and transverse modes, enabling multi‐dimensional quantum control of light fields. Directly generating watt‐level ultrafast vortex beams with large angular momentum has remained a major challenge due to the limitations of mode‐locked materials and existing spatiotemporal mode‐locking generation methods. In this study, quasi‐2D PEA2(CsPbBr3)n‐1PbBr4 perovskite films are prepared by an anti‐solvent method and employed for the first time in a mode‐locked resonator operating in free space. Utilizing the angle‐based non‐collinear pumping and frequency doubling techniques, the second‐order ultrafast green vortex beams with a power of up to 1.05 W and a duration of 373 ps are generated. Experimental findings demonstrate the strong nonlinear saturable absorption properties of quasi‐2D PEA2(CsPbBr3)n‐1PbBr4 perovskite films at high power levels, highlighting their considerable potential in ultrafast laser technology and nonlinear optics.
{"title":"Watt‐Level Second‐Order Topological Charge Ultrafast Green Vortex Laser with Quasi ‐2D PEA2(CsPbBr3)n‐1PbBr4 Perovskite Films Saturable Absorber","authors":"Zehua Liu, Jingzhen Li, Ling Zhang, Yu Zhang, Song Yang, Zhenxu Bai, Yulei Wang, Zhiwei Lu, Dapeng Yan, Yaoyao Qi, XingWang Zhang","doi":"10.1002/adom.202401165","DOIUrl":"https://doi.org/10.1002/adom.202401165","url":null,"abstract":"Ultrafast vortex beams have significant scientific and practical value because of their unique phase properties in both the longitudinal and transverse modes, enabling multi‐dimensional quantum control of light fields. Directly generating watt‐level ultrafast vortex beams with large angular momentum has remained a major challenge due to the limitations of mode‐locked materials and existing spatiotemporal mode‐locking generation methods. In this study, quasi‐2D PEA<jats:sub>2</jats:sub>(CsPbBr<jats:sub>3</jats:sub>)<jats:sub>n‐1</jats:sub>PbBr<jats:sub>4</jats:sub> perovskite films are prepared by an anti‐solvent method and employed for the first time in a mode‐locked resonator operating in free space. Utilizing the angle‐based non‐collinear pumping and frequency doubling techniques, the second‐order ultrafast green vortex beams with a power of up to 1.05 W and a duration of 373 ps are generated. Experimental findings demonstrate the strong nonlinear saturable absorption properties of quasi‐2D PEA<jats:sub>2</jats:sub>(CsPbBr<jats:sub>3</jats:sub>)<jats:sub>n‐1</jats:sub>PbBr<jats:sub>4</jats:sub> perovskite films at high power levels, highlighting their considerable potential in ultrafast laser technology and nonlinear optics.","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":null,"pages":null},"PeriodicalIF":9.0,"publicationDate":"2024-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141511726","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}
Cristina V. Manzano, Alba Díaz‐Lobo, Marta Gil‐García, Óscar Rodríguez de la Fuente, Ángel Morales‐Sabio, Marisol Martin‐Gonzalez
All‐day passive daytime radiative coolers (PDRC) offer a promising solution for energy‐free cooling of buildings and devices. This study investigates the use of various cellulose‐derivative networks to achieve optimal and stable cooling performance. These results showed that the mixed cellulose ester network has a maximum solar reflectance of 97%. While cellulose acetate network has a maximum infrared emissivity of 96% in the atmospheric transparency window band, which is a near‐perfect infrared emitter, the nitrocellulose network shows the highest cooling temperature, with a significant reduction of 14 °C from the ambient temperature and a power of 124 W·m−2 during the daytime and at night of 7.7 °C and 72.8 W·m−2. This study also analyzes the dampness's effect on the cooling performance of cellulose‐derivative networks. The cooling performance of the nitrocellulose network drops ≈ 3 °C (from 14 to 11.3 °C) when the relative humidity of the day exceeds ≈ 30% is observed. These findings indicate that the capacity of a material to absorb water from the surrounding air significantly influences its performance as a passive cooler, primarily due to changes in its optical properties. This is an important insight, as it highlights the need to consider environmental factors like relative humidity and sample hydrophobicity for PDRC systems.
{"title":"Performance and Relative Humidity Impact of Cellulose‐Derivative Networks in All‐Day Passive Radiative Cooling","authors":"Cristina V. Manzano, Alba Díaz‐Lobo, Marta Gil‐García, Óscar Rodríguez de la Fuente, Ángel Morales‐Sabio, Marisol Martin‐Gonzalez","doi":"10.1002/adom.202400551","DOIUrl":"https://doi.org/10.1002/adom.202400551","url":null,"abstract":"All‐day passive daytime radiative coolers (PDRC) offer a promising solution for energy‐free cooling of buildings and devices. This study investigates the use of various cellulose‐derivative networks to achieve optimal and stable cooling performance. These results showed that the mixed cellulose ester network has a maximum solar reflectance of 97%. While cellulose acetate network has a maximum infrared emissivity of 96% in the atmospheric transparency window band, which is a near‐perfect infrared emitter, the nitrocellulose network shows the highest cooling temperature, with a significant reduction of 14 °C from the ambient temperature and a power of 124 W·m<jats:sup>−2</jats:sup> during the daytime and at night of 7.7 °C and 72.8 W·m<jats:sup>−2</jats:sup>. This study also analyzes the dampness's effect on the cooling performance of cellulose‐derivative networks. The cooling performance of the nitrocellulose network drops ≈ 3 °C (from 14 to 11.3 °C) when the relative humidity of the day exceeds ≈ 30% is observed. These findings indicate that the capacity of a material to absorb water from the surrounding air significantly influences its performance as a passive cooler, primarily due to changes in its optical properties. This is an important insight, as it highlights the need to consider environmental factors like relative humidity and sample hydrophobicity for PDRC systems.","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":null,"pages":null},"PeriodicalIF":9.0,"publicationDate":"2024-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141511780","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}
Photodetectors with good polarization detection ability are promising in many applications, such as remote sensing imaging and environmental monitoring. However, the traditional polarization detection systems fall short in meeting integration demands of the integrated‐circuits field due to additional optical elements. The emerging 2D materials with in‐plane anisotropic structures provide a possible method to fabricate remarkable polarization detectors. Modulating the band structure by gate voltage is an important strategy for developing optoelectronic devices. Herein, a polarized photodetector based on PdSe2/MoS2 out‐of‐plane heterojunction is fabricated. Due to its unique out‐of‐plane heterostructure, the device exhibits excellent photoresponse characteristics and polarization sensitivity, including an excellent responsivity of 10.19A/W, an extremely high external quantum efficiency of 2429%, a fast rise/decay time of 68/192 µs, and a high photocurrent anisotropy ratio of 3.09. Based on the adjustment of the built‐in electric field through gate voltage, the performance of the device can be accordingly modulated. As the gate voltage increases from −30 to 30 V, the responsivity gradually increases from 7.5 to 13A/W and the detectivity increases from 1.53 to 2.63 × 109Jones. Finally, its olarization imaging ability is demonstrated at different polarization angles. The findings indicate that PdSe2/MoS2 devices exhibit significant potential for polarized photoelectric detection.
{"title":"Gate‐Modulated and Polarization‐Sensitive Photodetector Based on the MoS2/PdSe2 Out‐Of‐Plane Van Der Waals Heterostructure","authors":"Chengdong Yin, Sixian He, Xiaofeng Fan, Yuke Xiao, Liancheng Zhao, Liming Gao","doi":"10.1002/adom.202401122","DOIUrl":"https://doi.org/10.1002/adom.202401122","url":null,"abstract":"Photodetectors with good polarization detection ability are promising in many applications, such as remote sensing imaging and environmental monitoring. However, the traditional polarization detection systems fall short in meeting integration demands of the integrated‐circuits field due to additional optical elements. The emerging 2D materials with in‐plane anisotropic structures provide a possible method to fabricate remarkable polarization detectors. Modulating the band structure by gate voltage is an important strategy for developing optoelectronic devices. Herein, a polarized photodetector based on PdSe<jats:sub>2</jats:sub>/MoS<jats:sub>2</jats:sub> out‐of‐plane heterojunction is fabricated. Due to its unique out‐of‐plane heterostructure, the device exhibits excellent photoresponse characteristics and polarization sensitivity, including an excellent responsivity of 10.19A/W, an extremely high external quantum efficiency of 2429%, a fast rise/decay time of 68/192 µs, and a high photocurrent anisotropy ratio of 3.09. Based on the adjustment of the built‐in electric field through gate voltage, the performance of the device can be accordingly modulated. As the gate voltage increases from −30 to 30 V, the responsivity gradually increases from 7.5 to 13A/W and the detectivity increases from 1.53 to 2.63 × 10<jats:sup>9</jats:sup>Jones. Finally, its olarization imaging ability is demonstrated at different polarization angles. The findings indicate that PdSe<jats:sub>2</jats:sub>/MoS<jats:sub>2</jats:sub> devices exhibit significant potential for polarized photoelectric detection.","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":null,"pages":null},"PeriodicalIF":9.0,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141511786","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}
Chiral self‐discrimination plays a critical role in supramolecular chemistry and materials science. However, an ideal strategy for achieving chiral self‐discrimination remains elusive due to the inevitable nonspecific binding of incorrect enantiomers, and insufficient intrinsic optical activity of chiral molecules. Herein, a novel 1,1′‐binaphthol (BINOL) derivative with an imide group fused at the peri‐position of one naphthol scaffold is developed, which combines the dual functionalities of aggregation‐induced emission characteristic of BINOLs, and high emission of 1,8‐naphthalimides. The multiple molecular recognition between two hydroxyl groups in BINOL units and two carbonyl groups in 1,8‐naphthalimide moieties endows the precise chiral self‐discrimination behaviors. As expected, the homochiral aggregates exhibit reversible phase transitions, switching from non‐emission to bright green emission upon absorption and desorption of methanol vapor. In contrast, the heterochiral conglomerates exhibit irreversible yellow emission changes due to the impact of chiral self‐discrimination. Such chiral self‐discrimination‐induced luminescence vapochromism can be further applied to high‐level anti‐counterfeiting and data encryption. This work provides a new perspective on smart chiral organic materials based on chiral self‐discrimination.
{"title":"Chiral Self‐Discrimination Induced Luminescence Vapochromism of Binaphthol Imides for Anti‐Counterfeiting and Data Encryption","authors":"Yang Zhang, Hong‐Ming Chen, Mei‐Jin Lin","doi":"10.1002/adom.202400898","DOIUrl":"https://doi.org/10.1002/adom.202400898","url":null,"abstract":"Chiral self‐discrimination plays a critical role in supramolecular chemistry and materials science. However, an ideal strategy for achieving chiral self‐discrimination remains elusive due to the inevitable nonspecific binding of incorrect enantiomers, and insufficient intrinsic optical activity of chiral molecules. Herein, a novel 1,1′‐binaphthol (BINOL) derivative with an imide group fused at the <jats:italic>peri</jats:italic>‐position of one naphthol scaffold is developed, which combines the dual functionalities of aggregation‐induced emission characteristic of BINOLs, and high emission of 1,8‐naphthalimides. The multiple molecular recognition between two hydroxyl groups in BINOL units and two carbonyl groups in 1,8‐naphthalimide moieties endows the precise chiral self‐discrimination behaviors. As expected, the homochiral aggregates exhibit reversible phase transitions, switching from non‐emission to bright green emission upon absorption and desorption of methanol vapor. In contrast, the heterochiral conglomerates exhibit irreversible yellow emission changes due to the impact of chiral self‐discrimination. Such chiral self‐discrimination‐induced luminescence vapochromism can be further applied to high‐level anti‐counterfeiting and data encryption. This work provides a new perspective on smart chiral organic materials based on chiral self‐discrimination.","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":null,"pages":null},"PeriodicalIF":9.0,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141511791","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 charge‐transfer (CT) co‐crystals have demonstrated remarkable physical properties and have found applications in numerous fields. Yet their utility as a Surface‐Enhanced Raman Spectroscopy (SERS) substrate, a powerful and versatile analytical tool, has never been explored. Herein, three twisted molecular donors are synthesized, that exhibit well‐controlled switchable optical properties including aggregation‐induced emission (AIE), mechanochromic luminescence (MCL), and color‐specific polymorphism. Rapid production of charge‐transfer co‐crystals is also established with a π‐acceptor TCNQ and utilized conceptually as a SERS substrate for methylene blue (MB) detection, exhibiting a very high enhancement factor of 109 and limit of detection of 10−13m, respectively, due to the presence of low‐lying excited state, exhibit an 80% CT character, originating from the HOMO of the co‐crystal and interacting with the LUMO of the MB molecule. This approach using CT co‐crystals as a SERS substrate presents newer frontiers that require minuscule levels of rapid detection and impact allied areas, helping us understand and optimize the fascinating properties of such multicomponent materials for newer technologies.
{"title":"Engineering Single Component Luminogens to Multicomponent Charge‐transfer Co‐crystal Substrate as New Frontiers for Sensitive SERS Detection","authors":"Debika Barman, Debasish Barman, Kalishankar Bhattacharyya, Parameswar Krishnan Iyer","doi":"10.1002/adom.202401352","DOIUrl":"https://doi.org/10.1002/adom.202401352","url":null,"abstract":"Organic charge‐transfer (CT) co‐crystals have demonstrated remarkable physical properties and have found applications in numerous fields. Yet their utility as a Surface‐Enhanced Raman Spectroscopy (SERS) substrate, a powerful and versatile analytical tool, has never been explored. Herein, three twisted molecular donors are synthesized, that exhibit well‐controlled switchable optical properties including aggregation‐induced emission (AIE), mechanochromic luminescence (MCL), and color‐specific polymorphism. Rapid production of charge‐transfer co‐crystals is also established with a π‐acceptor TCNQ and utilized conceptually as a SERS substrate for methylene blue (MB) detection, exhibiting a very high enhancement factor of 10<jats:sup>9</jats:sup> and limit of detection of 10<jats:sup>−13</jats:sup> <jats:sc>m,</jats:sc> respectively, due to the presence of low‐lying excited state, exhibit an 80% CT character, originating from the HOMO of the co‐crystal and interacting with the LUMO of the MB molecule. This approach using CT co‐crystals as a SERS substrate presents newer frontiers that require minuscule levels of rapid detection and impact allied areas, helping us understand and optimize the fascinating properties of such multicomponent materials for newer technologies.","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":null,"pages":null},"PeriodicalIF":9.0,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141511785","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}
Yao Zhao, Yawen Zhang, Jie Yang, Yi Chen, Guqiang Pu, Yunsheng Wang, Dan Li, Wei Fan, Manman Fang, Jishan Wu, Zhen Li
Donor–acceptor (D–A) structure with charge transfer (CT) effect is widely utilized in the construction of organic luminescent materials. The adjustment of their CT effect and related luminescent property usually relies on the changes of molecular structure with different D or A moieties, which will lead to some uncertainties in structure‐property relationship. With the aim to explore the clear inherent luminescent mechanism for D–A molecule with CT effect, it is ideal that the regulation of intramolecular charge transfer in one same D–A molecule can be realized. Accordingly, three D–A type organic phosphorescence luminogens are designed and synthesized. Once being doped into different polymer matrixes, disparate charge transfer effects and related room temperature phosphorescence (RTP) properties can be achieved for a single molecule. Subsequent experiments confirm that different distributions of molecules with locally excited (LE) state and CT state are mainly responsible for their distinct RTP behaviors, exhibiting the well‐clarified structure‐property relationship of D–A type phosphorescence luminogens. Furthermore, the transition from CT to LE state can even be realized through chemical reaction, leading to the activated RTP effect for practical applications.
{"title":"The Role of Locally Excited State and Charge Transfer State in Organic Room Temperature Phosphorescence and Corresponding Applications","authors":"Yao Zhao, Yawen Zhang, Jie Yang, Yi Chen, Guqiang Pu, Yunsheng Wang, Dan Li, Wei Fan, Manman Fang, Jishan Wu, Zhen Li","doi":"10.1002/adom.202400980","DOIUrl":"https://doi.org/10.1002/adom.202400980","url":null,"abstract":"Donor–acceptor (D–A) structure with charge transfer (CT) effect is widely utilized in the construction of organic luminescent materials. The adjustment of their CT effect and related luminescent property usually relies on the changes of molecular structure with different D or A moieties, which will lead to some uncertainties in structure‐property relationship. With the aim to explore the clear inherent luminescent mechanism for D–A molecule with CT effect, it is ideal that the regulation of intramolecular charge transfer in one same D–A molecule can be realized. Accordingly, three D–A type organic phosphorescence luminogens are designed and synthesized. Once being doped into different polymer matrixes, disparate charge transfer effects and related room temperature phosphorescence (RTP) properties can be achieved for a single molecule. Subsequent experiments confirm that different distributions of molecules with locally excited (LE) state and CT state are mainly responsible for their distinct RTP behaviors, exhibiting the well‐clarified structure‐property relationship of D–A type phosphorescence luminogens. Furthermore, the transition from CT to LE state can even be realized through chemical reaction, leading to the activated RTP effect for practical applications.","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":null,"pages":null},"PeriodicalIF":9.0,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141511784","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}
Anna‐Lena Hofmann, Jakob Wolansky, Mike Hambsch, Felix Talnack, Eva Bittrich, Lucy Winkler, Max Herzog, Tianyi Zhang, Tobias Antrack, L. Conrad Winkler, Jonas Schröder, Moritz Riede, Stefan C.B. Mannsfeld, Johannes Benduhn, Karl Leo
Organic semiconductors still lag behind their inorganic counterparts in terms of mobility due to their lower structural order, in particular in thin films. Here, the highly ordered phase of triclinic rubrene – characterized by high vertical hole mobility – grown from a vacuum‐deposited thin film is used by post‐annealing and implemented into organic photodetectors. Since the triclinic rubrene exhibits a high roughness with a peak‐to‐valley value of 250 nm, which is detrimental to the dark current, strategies to control the crystal growth are developed. These investigations show that a suppression layer of 20 nm C60 is the most promising approach to successfully reduce the surface roughness while maintaining the triclinic phase, proven by grazing‐incidence wide‐angle X‐ray scattering (GIWAXS). With the smoothened active layer, the dark current density is reduced by three orders of magnitude compared to the neat rubrene layer. It is as low as 2.5 × 10−10 A cm−2 at −0.1 V bias, reflected in an overall specific detectivity of 6 × 1011 Jones at zero bias (based on noise measurements) and a high linear dynamic range of 170 dB. This strategy using a suppression layer thus proves successful and is very promising to be applied to other crystalline materials.
由于结构有序性较低，有机半导体在迁移率方面仍然落后于无机半导体，尤其是在薄膜中。在这里，利用真空沉积薄膜生长出的高度有序的三菱红柱石相（具有高垂直空穴迁移率的特点）进行后退火，并将其应用到有机光电探测器中。由于三linic rubrene 具有峰谷值为 250 nm 的高粗糙度，不利于暗电流，因此开发了控制晶体生长的策略。通过掠入射广角 X 射线散射 (GIWAXS)，这些研究表明 20 nm C60 抑制层是在保持三菱相的同时成功降低表面粗糙度的最有前途的方法。与纯红宝石层相比，平滑活性层的暗电流密度降低了三个数量级。在 -0.1 V 偏压下，暗电流密度低至 2.5 × 10-10 A cm-2，这反映在零偏压下 6 × 1011 Jones 的总体特定检测率（基于噪声测量）和 170 dB 的高线性动态范围上。因此，这种使用抑制层的策略被证明是成功的，并有望应用于其他晶体材料。
{"title":"Strategies to Control Crystal Growth of Highly Ordered Rubrene Thin Films for Application in Organic Photodetectors","authors":"Anna‐Lena Hofmann, Jakob Wolansky, Mike Hambsch, Felix Talnack, Eva Bittrich, Lucy Winkler, Max Herzog, Tianyi Zhang, Tobias Antrack, L. Conrad Winkler, Jonas Schröder, Moritz Riede, Stefan C.B. Mannsfeld, Johannes Benduhn, Karl Leo","doi":"10.1002/adom.202401025","DOIUrl":"https://doi.org/10.1002/adom.202401025","url":null,"abstract":"Organic semiconductors still lag behind their inorganic counterparts in terms of mobility due to their lower structural order, in particular in thin films. Here, the highly ordered phase of triclinic rubrene – characterized by high vertical hole mobility – grown from a vacuum‐deposited thin film is used by post‐annealing and implemented into organic photodetectors. Since the triclinic rubrene exhibits a high roughness with a peak‐to‐valley value of 250 nm, which is detrimental to the dark current, strategies to control the crystal growth are developed. These investigations show that a suppression layer of 20 nm C<jats:sub>60</jats:sub> is the most promising approach to successfully reduce the surface roughness while maintaining the triclinic phase, proven by grazing‐incidence wide‐angle X‐ray scattering (GIWAXS). With the smoothened active layer, the dark current density is reduced by three orders of magnitude compared to the neat rubrene layer. It is as low as 2.5 × 10<jats:sup>−10 </jats:sup>A cm<jats:sup>−2</jats:sup> at −0.1 V bias, reflected in an overall specific detectivity of 6 × 10<jats:sup>11</jats:sup> Jones at zero bias (based on noise measurements) and a high linear dynamic range of 170 dB. This strategy using a suppression layer thus proves successful and is very promising to be applied to other crystalline materials.","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":null,"pages":null},"PeriodicalIF":9.0,"publicationDate":"2024-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141511787","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}
Stepan Ilin, Daria Khmelevskaia, Anna Nikolaeva, George M. Maragkakis, Sotiris Psilodimitrakopoulos, Leonidas Mouchliadis, Pavel M. Talianov, Soslan A. Khubezhov, Emmanuel Stratakis, Lev E. Zelenkov, Sergey V. Makarov
Lead‐free halide perovskites is a novel class of environment‐friendly nonlinear optical materials, that already demonstrate high potential for second harmonics generation (SHG). Here a synthesis protocol is optimized to create single‐crystal CsGeI3 nanoparticles (NPs) supporting optical Mie resonances that efficiently convert infrared light to visible both via lasing and SHG mechanisms. Such high‐quality resonant NPs allow us to achieve up‐conversion lasing in the broadband excitation wavelength (1200–1520 nm), which is accompanied by efficient spectrally tunable SHG with intensity comparable with that for lasing depending on temperature. Experimental and theoretical study of linear and nonlinear optical properties of CsGeI3 material in the form of high‐quality thin film and NPs of different sizes reveal that coupling incident light with a magnetic dipole resonance leads to a strong enhancement of SHG by one order of magnitude. As a result, the study provides a novel strategy where individual NPs can support both up‐conversion lasing and SHG in a broad range of excitation wavelengths.
{"title":"Lead‐Free Halide Perovskite Nanoparticles for Up‐Conversion Lasing and Efficient Second Harmonic Generation","authors":"Stepan Ilin, Daria Khmelevskaia, Anna Nikolaeva, George M. Maragkakis, Sotiris Psilodimitrakopoulos, Leonidas Mouchliadis, Pavel M. Talianov, Soslan A. Khubezhov, Emmanuel Stratakis, Lev E. Zelenkov, Sergey V. Makarov","doi":"10.1002/adom.202400170","DOIUrl":"https://doi.org/10.1002/adom.202400170","url":null,"abstract":"Lead‐free halide perovskites is a novel class of environment‐friendly nonlinear optical materials, that already demonstrate high potential for second harmonics generation (SHG). Here a synthesis protocol is optimized to create single‐crystal CsGeI<jats:sub>3</jats:sub> nanoparticles (NPs) supporting optical Mie resonances that efficiently convert infrared light to visible both via lasing and SHG mechanisms. Such high‐quality resonant NPs allow us to achieve up‐conversion lasing in the broadband excitation wavelength (1200–1520 nm), which is accompanied by efficient spectrally tunable SHG with intensity comparable with that for lasing depending on temperature. Experimental and theoretical study of linear and nonlinear optical properties of CsGeI<jats:sub>3</jats:sub> material in the form of high‐quality thin film and NPs of different sizes reveal that coupling incident light with a magnetic dipole resonance leads to a strong enhancement of SHG by one order of magnitude. As a result, the study provides a novel strategy where individual NPs can support both up‐conversion lasing and SHG in a broad range of excitation wavelengths.","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":null,"pages":null},"PeriodicalIF":9.0,"publicationDate":"2024-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141511788","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}
Junwen Lai, Jie Zhan, Peitao Liu, Tomonori Shirakawa, Yunoki Seiji, Xing‐Qiu Chen, Yan Sun
Bulk photovoltaic effect, i.e. shift current, is a nonlinear second‐order optical response that can rectify an alternating current (AC) electric field into a direct current (DC). Depending on the wavelength of the incident light, shift current finds applications in various fields, including solar energy conversion and radiation detection. Its promising application in energy conversion and information processing has inspired investigations to uncover the relationship between shift current and electronic structures of materials. Despite numerous efforts dedicated to designing principles for strong bulk photovoltaic effect materials, the only widely accepted crucial parameter is the joint density of states (JDOS). In this study, employing effective model analysis and first‐principles calculations, an enhancement effect of bulk photovoltaic effect is found to arise from band hybridization that is typically along with anti‐crossing‐like electronic band structures, similar to the Berry curvature effects in intrinsic anomalous Hall conductivity. While this mechanism does not offer a comprehensive understanding of the relationship between electronic structure and the magnitude of bulk photovoltaic effect, it represents practical progress in the design of materials with strong bulk photovoltaic effect.
{"title":"Universal Enhancement Effect of Nonlinear Optical Response from Band Hybridization","authors":"Junwen Lai, Jie Zhan, Peitao Liu, Tomonori Shirakawa, Yunoki Seiji, Xing‐Qiu Chen, Yan Sun","doi":"10.1002/adom.202401143","DOIUrl":"https://doi.org/10.1002/adom.202401143","url":null,"abstract":"Bulk photovoltaic effect, i.e. shift current, is a nonlinear second‐order optical response that can rectify an alternating current (AC) electric field into a direct current (DC). Depending on the wavelength of the incident light, shift current finds applications in various fields, including solar energy conversion and radiation detection. Its promising application in energy conversion and information processing has inspired investigations to uncover the relationship between shift current and electronic structures of materials. Despite numerous efforts dedicated to designing principles for strong bulk photovoltaic effect materials, the only widely accepted crucial parameter is the joint density of states (JDOS). In this study, employing effective model analysis and first‐principles calculations, an enhancement effect of bulk photovoltaic effect is found to arise from band hybridization that is typically along with anti‐crossing‐like electronic band structures, similar to the Berry curvature effects in intrinsic anomalous Hall conductivity. While this mechanism does not offer a comprehensive understanding of the relationship between electronic structure and the magnitude of bulk photovoltaic effect, it represents practical progress in the design of materials with strong bulk photovoltaic effect.","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":null,"pages":null},"PeriodicalIF":9.0,"publicationDate":"2024-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141511795","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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