Jadupati Nag, Saugata Sarker, Safdar Imam, Abishek Iyer, Michael J. Waters, Albert Suceava, James M. Rondinelli, Mercouri G. Kanatzidis, Venkatraman Gopalan
{"title":"Large Non-Resonant Infrared Optical Second Harmonic Generation in Bulk Crystals of Van der Waals Semiconductor, SnP2Se6","authors":"Jadupati Nag, Saugata Sarker, Safdar Imam, Abishek Iyer, Michael J. Waters, Albert Suceava, James M. Rondinelli, Mercouri G. Kanatzidis, Venkatraman Gopalan","doi":"10.1002/adom.202402649","DOIUrl":"https://doi.org/10.1002/adom.202402649","url":null,"abstract":"<p>2D van der Waals (vdW) materials have emerged as a highly promising candidates for nonlinear optical (NLO) applications. This study presents the synthesis, comprehensive linear optical, and optical second harmonic generation (SHG) characterization of a novel 2D vdW semiconductor SnP<sub>2</sub>Se<sub>6</sub> in its bulk single crystal form. It exhibits an indirect bandgap of ≈1.47 eV and an exceptional non-resonant SHG coefficient of <i>d</i><sub>33</sub> ∼ −222 ± 30 pm V<sup>−1</sup> at a fundamental wavelength of 2 µm, which is ≈7 times larger than that of the commercial AgGaSe<sub>2</sub> with a comparable bandgap. Density functional theory (DFT) calculations of the linear and nonlinear optical properties exhibit reasonable agreement with the experimental measurements, revealing the chemical origin of the enhanced properties. Moreover, SnP<sub>2</sub>Se<sub>6</sub> can exhibit both type-I and type-II phase matching over a wide spectral range, fulfilling one of the key criteria for an ideal NLO crystal. These exceptional properties position SnP<sub>2</sub>Se<sub>6</sub> as a highly promising candidate for NLO applications.</p>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"13 9","pages":""},"PeriodicalIF":8.0,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/adom.202402649","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143688686","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Dmitrii Belogolovskii, Md Masudur Rahman, Karl Johnson, Vladimir Fedorov, Andrew Grieco, Nikola Alic, Abdoulaye Ndao, Paul K. L. Yu, Yeshaiahu Fainman
{"title":"Large Bidirectional Refractive Index Change in Silicon-rich Nitride via Visible Light Trimming","authors":"Dmitrii Belogolovskii, Md Masudur Rahman, Karl Johnson, Vladimir Fedorov, Andrew Grieco, Nikola Alic, Abdoulaye Ndao, Paul K. L. Yu, Yeshaiahu Fainman","doi":"10.1002/adom.202403420","DOIUrl":"https://doi.org/10.1002/adom.202403420","url":null,"abstract":"<p>Phase-sensitive integrated photonic devices are highly susceptible to minor manufacturing deviations, resulting in significant performance inconsistencies. This variability has limited the scalability and widespread adoption of these devices. Here, a major advancement is achieved through continuous-wave (CW) visible light (405 and 520 nm) trimming of plasma-enhanced chemical vapor deposition (PECVD) silicon-rich nitride (SRN) waveguides. The demonstrated method achieves precise, bidirectional refractive index tuning with a single laser source in CMOS-compatible SRN samples with refractive indices of 2.4 and 2.9 (measured at 1550 nm). By utilizing a cost-effective setup for real-time resonance tracking in micro-ring resonators, the resonant wavelength shifts as fine as 10 pm are attained. Additionally, a record red shift of 49.1 nm and a substantial blue shift of 10.6 nm are demonstrated, corresponding to refractive index changes of approximately 0.11 and −2 × 10<sup>−2</sup>. The blue and red shifts are both conclusively attributed to thermal annealing. These results highlight SRN's exceptional capability for permanent optical tuning, establishing a foundation for stable, precisely controlled performance in phase-sensitive integrated photonic devices.</p>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"13 14","pages":""},"PeriodicalIF":8.0,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/adom.202403420","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144074599","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sihui Deng, Jiahui Wang, Junhui Miao, Jun Ma, Junli Hu, Jun Liu
{"title":"Semifluoroalkyl n-Type Conjugated Polymers: Novel Cathode Interlayers for Air-Stable Organic Photodetectors","authors":"Sihui Deng, Jiahui Wang, Junhui Miao, Jun Ma, Junli Hu, Jun Liu","doi":"10.1002/adom.202403477","DOIUrl":"https://doi.org/10.1002/adom.202403477","url":null,"abstract":"<p>Typical organic cathode interlayer (CIL) materials for solution-processed organic optoelectronic devices usually have polar side chains or polar/ionic groups, making them hydrophilic and thus limiting device stability. This manuscript reports a novel CIL material based on an n-type polythiophene backbone with semifluoroalkyl side chains (n-PT11) for developing high-performance organic photodetectors (OPDs) with excellent device stability. The n-type polythiophene backbone of n-PT11 has a low-lying LUMO/HOMO energy level of −4.27 eV/−6.21 eV, suppressing reversed hole injection. The semifluoroalkyl side chains enable n-PT11 processing with 1,1,1,3,3,3-hexafluoro-2-propanol (HFIP) for fabricating multilayer OPDs and exhibit low trap density for suppressing dark current density (<i>J</i><sub>d</sub>). As a result, n-PT11-based near-infrared (NIR) OPDs exhibit an ultra-low <i>J</i><sub>d</sub> of 1.00 × 10<sup>−9</sup> A cm<sup>−2</sup> and a high specific detectivity (<i>D<sup>*</sup></i>) of 3.06 × 10<sup>12</sup> cm Hz<sup>1/2</sup> W<sup>−1</sup> at −1 V, which is among the highest <i>D<sup>*</sup></i> values reported so far for NIR OPDs. Most importantly, the hydrophobicity of n-PT11 allows the OPD unprecedented air stability, with unencapsulated OPDs retaining 94% of their initial responsiveness after 2000 h in ambient conditions. To the best knowledge, this is the first report of conjugated polymers with semifluoroalkyl side chains as CILs in OPDs.</p>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"13 14","pages":""},"PeriodicalIF":8.0,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144074299","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}
{"title":"Machine Learning Enabled LED Lighting Using Scattering Optics","authors":"Gangyi Li, Yuan Liu, Hao Liang, Xihua Wang","doi":"10.1002/adom.202402788","DOIUrl":"https://doi.org/10.1002/adom.202402788","url":null,"abstract":"<p>Illumination receives a great deal of attention as white light-emitting diodes become energy-efficient light sources in households and commercial buildings, on streets and highways, and at stadiums and construction sites. In general, lenses and mirrors are used to control the spatial distribution of white LED (WLED) light. Here, it is proposed to use an optical diffuser, the key device in scattering optics, to achieve a pre-defined WLED brightness distribution by nanocrystals and machine learning. Optical diffusers are typically used to create soft light (similar brightness from any angle of view), however, here the concentration of nanocrystals in a nanocomposite film (optical diffuser) to tune its optical property at different regions is altered. Machine learning is employed to achieve the inverse design of the optical diffuser pattern controlling the WLED brightness distribution, and this design task is beyond human capacities which are carried out using the brute force approach. In the end, several pre-defined WLED brightness distributions are demonstrated for showing the success of this efforts.</p>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"13 9","pages":""},"PeriodicalIF":8.0,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/adom.202402788","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143688654","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pablo B. Pinto, Pedro W. Matrone, Flávia S. Ferreira, Paulo V. Santos, Fernando A. Sigoli, Odilon D. D. Couto Jr.
{"title":"Thermal Dynamics Induced by Surface Acoustic Waves in Lanthanide-Doped Core@Multishell Nanoparticles","authors":"Pablo B. Pinto, Pedro W. Matrone, Flávia S. Ferreira, Paulo V. Santos, Fernando A. Sigoli, Odilon D. D. Couto Jr.","doi":"10.1002/adom.202403497","DOIUrl":"https://doi.org/10.1002/adom.202403497","url":null,"abstract":"<p>Accurate local temperature readout in integrated nanoscaled devices driven by high-frequency surface acoustic waves (SAWs) has a strong technological interest. The optical response of lanthanide (Ln)-doped NaLnF<sub>4</sub> core@multishell nanoparticles inserted into SAW delay lines is reported. The recombination dynamics between the <sup>2</sup><i>H</i><sub>11/2</sub> and <sup>4</sup><i>S</i><sub>3/2</sub> to the <sup>4</sup><i>I</i><sub>15/2</sub> states of Er<sup>3+</sup> is probed under SAWs modulation at 5, 225, and 290 K. It is shown that the spectral weight of the upconverted individual Stark levels of the <sup>4</sup><i>S</i><sub>3/2</sub> band changes with the SAW and that their recombination lifetimes decrease as the SAW power is increased. By monitoring the luminescence intensity ratio (LIR), it is shown that such dynamics is consistent with a temperature increase and a carrier repopulation process across the <sup>4</sup><i>S</i><sub>3/2</sub> Stark levels induced by Joule heating, which can reach up to 47 K at cryogenic temperatures. These effects, however, can be strongly suppressed by reducing the SAW duty cycle during the optical measurements. The results demonstrate that heating of nanoscopic systems integrated into SAW devices can be quite pronounced and that, since they do not interact with the SAW strain or piezoelectric field, these NaLnF<sub>4</sub> nanoparticles can be effectively employed as nanoscale in-situ and in-operando thermometers in such kind of application.</p>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"13 14","pages":""},"PeriodicalIF":8.0,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/adom.202403497","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144074370","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Diffractive Metasurface-Enabled Single-Shot Characterization of Hybrid-Order Poincaré Beams","authors":"Xiaoxin Li, Bojian Shi, Qi Jia, Yanxia Zhang, Yanyu Gao, Wenya Gao, Donghua Tang, Yongyin Cao, Fangkui Sun, Rui Feng, Weiqiang Ding","doi":"10.1002/adom.202403405","DOIUrl":"https://doi.org/10.1002/adom.202403405","url":null,"abstract":"<p>Hybrid-order Poincaré beams (HyOPBs) with complex transverse polarization states hold significant potential in optical communication and quantum information. Fully characterizing the Poincaré parameters of HyOPBs is a key task to accelerate applications. Conventional methods typically require mapping in multiple polarization states and reconstructing point by point, creating a fundamental bottleneck for fast measurement and real-time monitoring of Poincaré parameters. In this work, a single-shot and real-time characterization scheme for HyOPBs is demonstrated by applying diffractive neural networks to a system of cascaded diffractive metasurfaces. The designed diffractive metasurfaces essentially function as an optical processor, efficiently extracting high-dimensional spatial modes and complex amplitude information. Whereafter, the Poincaré parameters are accurately predicted, and the HyOPBs are correctly reconstructed with the help of electronic deep neural networks. This innovative approach is validated through a series of simulation studies with average reconstruction errors of <2.68% for σ and 1.84% for θ, respectively. The work provides an effective strategy for precise, compact, and real-time detection of HyOPBs, paving the way for their application in the next generation of high-capacity optical communication systems.</p>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"13 13","pages":""},"PeriodicalIF":8.0,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143904958","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}
{"title":"Exploring the Mystery of “Negative Thermal Quenching” in Cs3Cu2I5 Single-Crystal","authors":"Yusheng Ma, Haohang Song, Qian Yao, Xin Guan, Yanqi Zhang, Mingkang Yang, Xuesong Li, Xutang Tao","doi":"10.1002/adom.202403194","DOIUrl":"https://doi.org/10.1002/adom.202403194","url":null,"abstract":"<p>As a high-interest emerging effect, negative thermal quenching (NTQ) may bring revolutionary advances in luminescence. However, the reason for NTQ is still unclear, making it challenging to target design materials with such unique properties. Interestingly, it is found that the Cs<sub>3</sub>Cu<sub>2</sub>I<sub>5</sub> single-crystals grown using the Bridgman and antisolvent methods exhibit the conventional thermal quenching, while the single-crystal grown by the aqueous solution method yet has the NTQ. This suggests that a specific structural change in the single crystals can be induced to produce NTQ, harboring the secrets of NTQs. It is found that the Cs<sub>3</sub>Cu<sub>2</sub>I<sub>5</sub> single-crystal from the aqueous solution method has a more compact crystal structure, smaller Huang–Rhys factor, and a more considerable exciton binding energy than other methods. In this case, the structural distortion of Cs<sub>3</sub>Cu<sub>2</sub>I<sub>5</sub> single-crystal after photoexcitation is limited at low temperatures, and consequently, the self-trapped exciton (STE) energy levels are incompletely formed. As the temperature increases, the STE energy levels gradually become fully formed, and their ability to trap electrons improves, resulting in the marvelous phenomenon of NTQ. This work provides a plausible mechanism for the mysterious NTQ and will guide the future design of NTQ materials.</p>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"13 12","pages":""},"PeriodicalIF":8.0,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143861442","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}
{"title":"Dual-Wavelength Photosensitizer Based on Phthalocyanine Nanodots for Multifunctional Composites with Enhanced Photodynamic Antibacterial, Photothermal Performance, and UV Protection","authors":"Meng Ju, Changwu Zheng, Aiqin Hou, Kongliang Xie, Xiaoyue Han, Aiqin Gao","doi":"10.1002/adom.202403212","DOIUrl":"https://doi.org/10.1002/adom.202403212","url":null,"abstract":"<p>Designing efficient near-infrared photosensitive molecules and excellent photosensitive materials is a major challenge in the fields of photodynamic antibacterial and photothermal energy conversion. The Förster resonance energy transfer shows much promise for enhancing the photodynamic antibacterial property and photothermal performance. Herein, a novel water-soluble dual-band enhanced naphthylimide functionalized phthalocyanine photosensitizer is designed and synthesized. The designed dual-band enhanced photosensitizer, 2,9(10),16(17),23(24)-Tetrakis[N-Benzyl-N,N'-dimethyl-1-propanaminium-4-(N-hydroxyethyl)-1,8-naphthylimino] phthalocyanine Zinc(II) (NAPc-N), can self-assemble by the <i>π–π</i> stacking interactions to form nanodots with a size of ≈40–50 nm. Nanodot composites prepared using waterborne polyurethane (WPU), exhibit dual-wavelength photodynamic antibacterial at 440 and 680 nm irradiations, efficiently photothermal conversion, and excellent UV protection (UPF) performances. The produced singlet oxygen amount by NAPc-N shows tremendous enhancement in dual-wavelength irradiations. After 30 min under the blue and infrared lights, the antibacterial rate of NAPc-N against <i>Staphylococcus aureus</i> and <i>Escherichia coli</i> reaches 99.99%. The temperature of the NAPc-N composite can be heated up to 60 °C and the UPF value can be up to 128.23. These dual-wavelength enhanced photosensitizer nanodots hold significant potential for advanced photodynamic materials and biomaterials applications.</p>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"13 12","pages":""},"PeriodicalIF":8.0,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143861499","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}
Paolo Franceschini, Andrea Tognazzi, Virginia Maria Demartis, Luca Carletti, Evgenii Menshikov, Ivano Alessandri, Alfonso Carmelo Cino, Fabrizio Torricelli, Costantino De Angelis, Maria Antonietta Vincenti
{"title":"Iontronically Tunable Broadband Graded Index Films (Advanced Optical Materials 7/2025)","authors":"Paolo Franceschini, Andrea Tognazzi, Virginia Maria Demartis, Luca Carletti, Evgenii Menshikov, Ivano Alessandri, Alfonso Carmelo Cino, Fabrizio Torricelli, Costantino De Angelis, Maria Antonietta Vincenti","doi":"10.1002/adom.202570064","DOIUrl":"https://doi.org/10.1002/adom.202570064","url":null,"abstract":"<p><b>Tunable Optical Devices</b></p><p>Laser light is deflected thanks to the spatial modulation of the bulk electronic conductance of a PEDOT:PSS layer arranged in an organic electrochemical transistor configuration. More details can be found in article 2402410 by Maria Antonietta Vincenti and co-workers.\u0000\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"13 7","pages":""},"PeriodicalIF":8.0,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/adom.202570064","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143554675","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}