ACS PhotonicsPub Date : 2024-11-20DOI: 10.1021/acsphotonics.4c01852
Hui Chen, Zhenxu Bai, Junhong Chen, Xiaowei Li, Zhi-Han Zhu, Yulei Wang, Takashige Omatsu, Richard P. Mildren, Zhiwei Lu
{"title":"Diamond Raman Vortex Lasers","authors":"Hui Chen, Zhenxu Bai, Junhong Chen, Xiaowei Li, Zhi-Han Zhu, Yulei Wang, Takashige Omatsu, Richard P. Mildren, Zhiwei Lu","doi":"10.1021/acsphotonics.4c01852","DOIUrl":"https://doi.org/10.1021/acsphotonics.4c01852","url":null,"abstract":"For the first time, a cascaded diamond Raman vortex laser directly emitting within the cavity has been reported. Employing a two-mirror structured diamond Raman oscillator pumped by a 1064 nm Gaussian laser, first- and second-order Raman transitions yielded outputs at 1240 and 1485 nm, respectively. By incorporating the off-axis rotation of cavity mirrors, both wavelength bands produced spatially symmetrical distributions of Hermite–Gaussian (HG) and Laguerre–Gaussian (LG) vortex beams. The achieved maximum output powers for the first and second Stokes vortex lasers were 42 and 22 W, respectively, corresponding to conversion efficiencies of 15.3% and 5.8%. Benefiting from diamond’s exceptional thermal properties, no saturation or decline in the Raman vortex output power was observed within the experimental pump power range. The straightforward off-axis adjustment methodology introduced into a diamond Raman cavity with superior optical and thermal characteristics enables direct dual-wavelength vortex emission, validating diamond Raman oscillators as an effective means of expanding the wavelength of the vortex laser. This breakthrough holds significant implications for expanding the working wavelengths and output powers of vortex beams.","PeriodicalId":23,"journal":{"name":"ACS Photonics","volume":"4 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678790","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS PhotonicsPub Date : 2024-11-20DOI: 10.1021/acsphotonics.4c0211510.1021/acsphotonics.4c02115
Otto Cranwell Schaeper, Lesley Spencer, Dominic Scognamiglio, Waleed El-Sayed, Benjamin Whitefield, Jake Horder, Nathan Coste, Paul Barclay, Milos Toth, Anastasiia Zalogina* and Igor Aharonovich*,
{"title":"Double Etch Method for the Fabrication of Nanophotonic Devices from van der Waals Materials","authors":"Otto Cranwell Schaeper, Lesley Spencer, Dominic Scognamiglio, Waleed El-Sayed, Benjamin Whitefield, Jake Horder, Nathan Coste, Paul Barclay, Milos Toth, Anastasiia Zalogina* and Igor Aharonovich*, ","doi":"10.1021/acsphotonics.4c0211510.1021/acsphotonics.4c02115","DOIUrl":"https://doi.org/10.1021/acsphotonics.4c02115https://doi.org/10.1021/acsphotonics.4c02115","url":null,"abstract":"<p >The integration of van der Waals (vdW) materials into photonic devices has laid out a foundation for many new quantum and optoelectronic applications. Despite tremendous progress in the nanofabrication of photonic building blocks from vdW crystals, there are still limitations, specifically with large-area devices and masking. Here, we focus on hexagonal boron nitride (hBN) as a vdW material and present a double etch method that overcomes problems associated with methods that employ metallic films and resist-based films for masking. Efficacy of the developed protocol is demonstrated by designing and fabricating a set of functional photonic components─including waveguides, ring resonators, and photonic crystal cavities. The functionality of the fabricated structures is demonstrated through optical characterization over several key spectral ranges. These include the near-infrared and blue ranges, where the hBN boron vacancy (V<sub>B</sub><sup>–</sup>) spin defects and the coherent B center quantum emitters emit, respectively. The double etch method enables fabrication of high-quality factor optical cavities and constitutes a promising pathway toward on-chip integration of vdW materials.</p>","PeriodicalId":23,"journal":{"name":"ACS Photonics","volume":"11 12","pages":"5446–5452 5446–5452"},"PeriodicalIF":6.5,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142850580","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS PhotonicsPub Date : 2024-11-20DOI: 10.1021/acsphotonics.4c02115
Otto Cranwell Schaeper, Lesley Spencer, Dominic Scognamiglio, Waleed El-Sayed, Benjamin Whitefield, Jake Horder, Nathan Coste, Paul Barclay, Milos Toth, Anastasiia Zalogina, Igor Aharonovich
{"title":"Double Etch Method for the Fabrication of Nanophotonic Devices from van der Waals Materials","authors":"Otto Cranwell Schaeper, Lesley Spencer, Dominic Scognamiglio, Waleed El-Sayed, Benjamin Whitefield, Jake Horder, Nathan Coste, Paul Barclay, Milos Toth, Anastasiia Zalogina, Igor Aharonovich","doi":"10.1021/acsphotonics.4c02115","DOIUrl":"https://doi.org/10.1021/acsphotonics.4c02115","url":null,"abstract":"The integration of van der Waals (vdW) materials into photonic devices has laid out a foundation for many new quantum and optoelectronic applications. Despite tremendous progress in the nanofabrication of photonic building blocks from vdW crystals, there are still limitations, specifically with large-area devices and masking. Here, we focus on hexagonal boron nitride (hBN) as a vdW material and present a double etch method that overcomes problems associated with methods that employ metallic films and resist-based films for masking. Efficacy of the developed protocol is demonstrated by designing and fabricating a set of functional photonic components─including waveguides, ring resonators, and photonic crystal cavities. The functionality of the fabricated structures is demonstrated through optical characterization over several key spectral ranges. These include the near-infrared and blue ranges, where the hBN boron vacancy (V<sub>B</sub><sup>–</sup>) spin defects and the coherent B center quantum emitters emit, respectively. The double etch method enables fabrication of high-quality factor optical cavities and constitutes a promising pathway toward on-chip integration of vdW materials.","PeriodicalId":23,"journal":{"name":"ACS Photonics","volume":"14 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142672936","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Advanced Image Classification Using a Differential Diffractive Network with “Learned” Structured Illumination","authors":"Jiajun Zhang, Shuyan Zhang, Weijie Shi, Yong Hu, Zheng-Gao Dong, Jiaqi Li, Weibing Lu","doi":"10.1021/acsphotonics.4c01511","DOIUrl":"https://doi.org/10.1021/acsphotonics.4c01511","url":null,"abstract":"As a new optical machine learning framework, the diffractive deep neural network (D<sup>2</sup>NN) has attracted much attention due to its advantages such as low power consumption, parallel computing, and fast execution speed. Here, we demonstrate a new optical neural network design of a differential D<sup>2</sup>NN with structured illumination. In this scheme, the illumination patterns participate in the training process of the network and are optimized by an end-to-end technique. With the application of differential detection, the non-negativity constraint in a diffractive neural network can be alleviated. The test results show that this network architecture can achieve 97.63 and 88.10% classification accuracies on the MNIST and Fashion-MNIST data sets using only one diffractive layer, which exceeds the effect achieved by the five-layer traditional D<sup>2</sup>NN. Moreover, this network architecture can achieve a comprehensive improvement over a traditional D<sup>2</sup>NN in the challenging classification problems of tiny samples and samples blocked by occlusions. Compared with the traditional D<sup>2</sup>NN, this scheme innovatively uses the illumination patterns as new degrees of freedom in system design, which can effectively improve classification ability and reduce the space complexity of the optical neural network.","PeriodicalId":23,"journal":{"name":"ACS Photonics","volume":"57 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678824","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Ultrasensitive Solar-Blind Phototransistor Based on ZnO/β-Ga2O3 Heterojunctions Fabricated Via Zinc-Induced Low-Temperature Dual-Crystallization","authors":"Guanghai Shi, Qiming Zhuang, Yuhang Liu, Jiao Xu, Teng Yun, Dengji Guo, Xujin Wang, Sudong Wu","doi":"10.1021/acsphotonics.4c01487","DOIUrl":"https://doi.org/10.1021/acsphotonics.4c01487","url":null,"abstract":"Crystalline Ga<sub>2</sub>O<sub>3</sub> is a desirable candidate for high-performance solar-blind photodetectors (SBPDs) owing to its intrinsic merits, such as an ultrawide bandgap (∼4.9 eV) and high chemical stability. However, Ga<sub>2</sub>O<sub>3</sub>-based SBPDs fabricated using conventional methods often suffer from high crystallization temperatures exceeding 750 °C. Herein, we propose a zinc-induced low-temperature dual-crystallization method for facile fabrication of high-performance n-ZnO/n-β-Ga<sub>2</sub>O<sub>3</sub> heterostructures by annealing a sputtered Zn/a-Ga<sub>2</sub>O<sub>3</sub> bilayer (5 nm/15 nm) at 500 °C in air. The structural evolution and crystallization mechanism of n–n heterojunctions were explored using cross-sectional high-resolution transmission electron microscopy and X-ray photoelectron spectroscopy. Benefiting synergistically from the significantly reduced oxygen vacancies as well as the high mobility of the n-ZnO derived from zinc oxidation, the back-gated phototransistors based on this heterojunction exhibited outstanding and balanced optoelectronic performance, with an ultrahigh responsivity of 7.4 × 10<sup>4</sup> A/W, an ultrafast rise time of 8.0 ms, a photo-to-dark current ratio of 2.4 × 10<sup>7</sup>, and a detectivity of 2.8 × 10<sup>15</sup> Jones. This study presents a novel approach for low-cost fabrication of high-quality ZnO/Ga<sub>2</sub>O<sub>3</sub> heterojunctions, revealing a promising pathway for achieving high-performance heterojunction optoelectronic devices.","PeriodicalId":23,"journal":{"name":"ACS Photonics","volume":"22 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142672935","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"2.46 MHz Ultranarrow Line Width Vertical-Cavity Surface-Emitting Lasers with Cholesteric Liquid Crystals Coupled Cavity","authors":"Ning Cui, Chen Zhang, Huihui Wang, Lishan Fu, Feng Zhang, Yudong Liu, Baolu Guan","doi":"10.1021/acsphotonics.4c01640","DOIUrl":"https://doi.org/10.1021/acsphotonics.4c01640","url":null,"abstract":"Due to their high level of integration, vertical-cavity surface-emitting lasers (VCSELs) are promising candidates for applications in quantum communication and sub-Doppler atomic microsystems. However, there is an urgent need to develop narrow line width, high-quality VCSELs that provide stable and reliable emission to meet commercial demands. Here, we demonstrate a novel coupled-cavity VCSEL integrated with a cholesteric liquid crystal (CLC) film to develop high-performance ultranarrow line width VCSELs. The CLC film can be flexibly integrated onto the surface of the VCSEL and applies weak light feedback which enhances the coherent superposition and compresses the line width of the VCSEL. It has been shown that when the length of the coupled cavity is less than 150 μm, it can suppress the higher-order modes and significantly reduce the threshold current of VCSEL. Furthermore, the CLC-VCSEL exhibits circular polarization output and an impressive line width of 2.46 MHz, which is the narrowest micron-scale integration VCSEL as reported, comparable to the line width of distributed Bragg reflection and distributed feedback semiconductor lasers. Compared with recently reported high-performance VCSELs and semiconductor lasers, the CLC-VCSELs achieve a lower threshold current and an enhanced beam quality. This micrometer-scale coupled cavity VCSEL will provide more possibilities for the development of next-generation VCSELs and integrated packages for CLC modulation. Moreover, the CLC optical feedback technique is not exclusive to VCSEL and can also be applied to other optoelectronic devices, such as low-power edge-emitting lasers, quantum dot lasers, and so forth.","PeriodicalId":23,"journal":{"name":"ACS Photonics","volume":"63 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678704","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS PhotonicsPub Date : 2024-11-20DOI: 10.1021/acsphotonics.4c0148710.1021/acsphotonics.4c01487
Guanghai Shi, Qiming Zhuang, Yuhang Liu, Jiao Xu*, Teng Yun, Dengji Guo, Xujin Wang and Sudong Wu,
{"title":"Ultrasensitive Solar-Blind Phototransistor Based on ZnO/β-Ga2O3 Heterojunctions Fabricated Via Zinc-Induced Low-Temperature Dual-Crystallization","authors":"Guanghai Shi, Qiming Zhuang, Yuhang Liu, Jiao Xu*, Teng Yun, Dengji Guo, Xujin Wang and Sudong Wu, ","doi":"10.1021/acsphotonics.4c0148710.1021/acsphotonics.4c01487","DOIUrl":"https://doi.org/10.1021/acsphotonics.4c01487https://doi.org/10.1021/acsphotonics.4c01487","url":null,"abstract":"<p >Crystalline Ga<sub>2</sub>O<sub>3</sub> is a desirable candidate for high-performance solar-blind photodetectors (SBPDs) owing to its intrinsic merits, such as an ultrawide bandgap (∼4.9 eV) and high chemical stability. However, Ga<sub>2</sub>O<sub>3</sub>-based SBPDs fabricated using conventional methods often suffer from high crystallization temperatures exceeding 750 °C. Herein, we propose a zinc-induced low-temperature dual-crystallization method for facile fabrication of high-performance n-ZnO/n-β-Ga<sub>2</sub>O<sub>3</sub> heterostructures by annealing a sputtered Zn/a-Ga<sub>2</sub>O<sub>3</sub> bilayer (5 nm/15 nm) at 500 °C in air. The structural evolution and crystallization mechanism of n–n heterojunctions were explored using cross-sectional high-resolution transmission electron microscopy and X-ray photoelectron spectroscopy. Benefiting synergistically from the significantly reduced oxygen vacancies as well as the high mobility of the n-ZnO derived from zinc oxidation, the back-gated phototransistors based on this heterojunction exhibited outstanding and balanced optoelectronic performance, with an ultrahigh responsivity of 7.4 × 10<sup>4</sup> A/W, an ultrafast rise time of 8.0 ms, a photo-to-dark current ratio of 2.4 × 10<sup>7</sup>, and a detectivity of 2.8 × 10<sup>15</sup> Jones. This study presents a novel approach for low-cost fabrication of high-quality ZnO/Ga<sub>2</sub>O<sub>3</sub> heterojunctions, revealing a promising pathway for achieving high-performance heterojunction optoelectronic devices.</p>","PeriodicalId":23,"journal":{"name":"ACS Photonics","volume":"11 12","pages":"5251–5259 5251–5259"},"PeriodicalIF":6.5,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842951","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Multifunctional Ionic Liquid Enables the Grain Coarsening and Defect Passivation of CsPbBr3 Films to Enhance the Performance of Perovskite Solar Cells","authors":"Xiaobing Cao, Zhaoqi Zhang, Jian Zhou, Qingshuo Zhang, Jinquan Wei","doi":"10.1021/acsphotonics.4c01827","DOIUrl":"https://doi.org/10.1021/acsphotonics.4c01827","url":null,"abstract":"CsPbBr<sub>3</sub>-based perovskite solar cells (PSCs) have attracted increasing attention owing to their superhigh stability, ease of fabrication process, and compatibility with the simplified device structure. It is a golden rule to promote the efficiency of PSCs to approach their theoretical efficiency limit through fabrication of CsPbBr<sub>3</sub> films with large grains and low defects. Herein, an ionic liquid of 1-ethyl-3-methylimidazoliumiodide (EMI) is introduced into a CsBr/H<sub>2</sub>O solution, and it is then spin-coated onto PbBr<sub>2</sub> films to fabricate high-quality CsPbBr<sub>3</sub> films. After optimizing the concentration of EMI in the CsBr/H<sub>2</sub>O solution, it can produce a significant grain coarsening effect, which is evidenced by the increase in mean grain size from 607 to 1070 nm under the assistance of EMI. On this foundation, EMI is also deposited onto the optimized CsPbBr<sub>3</sub> films so as to passivate the surface defects. After optimizing the grain size and the surface defects by EMI, it suppresses the nonradiative recombination owing to the passivation effects of EMI, which is achieved through forming an interaction between the uncoordinated ions (Cs<sup>+</sup> and Pb<sup>2+</sup>) and EMI. As a result, the power conversion efficiency of solar cells increases from 7.16% to 9.78% based on the simplified device structure of FTO/TiO<sub>2</sub>/CsPbBr<sub>3</sub>/Carbon, and it exhibits high stability in open air conditions. This work provides a feasible approach to improve the quality of CsPbBr<sub>3</sub> films and their performance in solar cells, and it enriches the strategies to obtain highly efficient CsPbBr<sub>3</sub> solar cells.","PeriodicalId":23,"journal":{"name":"ACS Photonics","volume":"6 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142672937","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS PhotonicsPub Date : 2024-11-19DOI: 10.1021/acsphotonics.4c01901
Chen Shen, Zhuo Xue, Wang Li, Wei Zeng, Jingyi Zhu, Zhen-Long Dou, Li Zhou, Xudong Xiao, Junbo Gong, Sheng Wang
{"title":"Revealing Different Types of Grain Boundaries in Perovskite Films by Intensity-dependent Fluorescence Lifetime Imaging Microscopy","authors":"Chen Shen, Zhuo Xue, Wang Li, Wei Zeng, Jingyi Zhu, Zhen-Long Dou, Li Zhou, Xudong Xiao, Junbo Gong, Sheng Wang","doi":"10.1021/acsphotonics.4c01901","DOIUrl":"https://doi.org/10.1021/acsphotonics.4c01901","url":null,"abstract":"Grain boundaries (GBs) in polycrystalline perovskite films play a crucial role in determining photogenerated carrier transport and recombination, thereby impacting both efficiency and stability of perovskite solar cells (PSCs). Despite extensive research into grain boundary engineering to optimize PSC performance, the specific mechanisms through which GBs influence carrier dynamics remain unclear and highly debated. Here, we employ high-resolution, intensity-dependent fluorescence lifetime imaging microscopy (FLIM) to systematically investigate the behaviors of different types of GBs in hybrid perovskite films under varying light conditions. Our analysis reveals three distinct categories of GBs: I-type, which remains invisible at low excitation intensities and exerts minimal influence on carrier transport; W-type, characterized by a W-shaped lifetime profile at high light intensities, suggesting significant carrier scattering at the boundary; and V-type, marked by a V-shaped lifetime profile, indicating a more specialized role in regulating carrier dynamics. These findings provide critical insights into how various GBs modulate photogenerated carrier behavior, offering a new framework for understanding their diverse impacts on the optoelectronic properties of perovskite films. Our results underscore the importance of targeted grain boundary engineering strategies to advance the design and optimization of next-generation perovskite-based photonic and optoelectronic devices.","PeriodicalId":23,"journal":{"name":"ACS Photonics","volume":"27 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142672938","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS PhotonicsPub Date : 2024-11-19DOI: 10.1021/acsphotonics.4c0190110.1021/acsphotonics.4c01901
Chen Shen, Zhuo Xue, Wang Li, Wei Zeng, Jingyi Zhu, Zhen-Long Dou, Li Zhou, Xudong Xiao*, Junbo Gong* and Sheng Wang*,
{"title":"Revealing Different Types of Grain Boundaries in Perovskite Films by Intensity-dependent Fluorescence Lifetime Imaging Microscopy","authors":"Chen Shen, Zhuo Xue, Wang Li, Wei Zeng, Jingyi Zhu, Zhen-Long Dou, Li Zhou, Xudong Xiao*, Junbo Gong* and Sheng Wang*, ","doi":"10.1021/acsphotonics.4c0190110.1021/acsphotonics.4c01901","DOIUrl":"https://doi.org/10.1021/acsphotonics.4c01901https://doi.org/10.1021/acsphotonics.4c01901","url":null,"abstract":"<p >Grain boundaries (GBs) in polycrystalline perovskite films play a crucial role in determining photogenerated carrier transport and recombination, thereby impacting both efficiency and stability of perovskite solar cells (PSCs). Despite extensive research into grain boundary engineering to optimize PSC performance, the specific mechanisms through which GBs influence carrier dynamics remain unclear and highly debated. Here, we employ high-resolution, intensity-dependent fluorescence lifetime imaging microscopy (FLIM) to systematically investigate the behaviors of different types of GBs in hybrid perovskite films under varying light conditions. Our analysis reveals three distinct categories of GBs: I-type, which remains invisible at low excitation intensities and exerts minimal influence on carrier transport; W-type, characterized by a W-shaped lifetime profile at high light intensities, suggesting significant carrier scattering at the boundary; and V-type, marked by a V-shaped lifetime profile, indicating a more specialized role in regulating carrier dynamics. These findings provide critical insights into how various GBs modulate photogenerated carrier behavior, offering a new framework for understanding their diverse impacts on the optoelectronic properties of perovskite films. Our results underscore the importance of targeted grain boundary engineering strategies to advance the design and optimization of next-generation perovskite-based photonic and optoelectronic devices.</p>","PeriodicalId":23,"journal":{"name":"ACS Photonics","volume":"11 12","pages":"5439–5445 5439–5445"},"PeriodicalIF":6.5,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142850867","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}