ACS Applied Optical Materials最新文献

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Optically Pumped Terahertz Amplitude Modulation in Type-II Ge QD/Si Heterostructures Grown via Molecular Beam Epitaxy 通过分子束外延生长的 II 型 Ge QD/Si 异质结构中的光泵浦太赫兹振幅调制
ACS Applied Optical Materials Pub Date : 2024-10-03 DOI: 10.1021/acsaom.4c0029810.1021/acsaom.4c00298
Suprovat Ghosh, Abir Mukherjee, Sudarshan Singh, Samit K Ray, Ananjan Basu, Santanu Manna and Samaresh Das*, 
{"title":"Optically Pumped Terahertz Amplitude Modulation in Type-II Ge QD/Si Heterostructures Grown via Molecular Beam Epitaxy","authors":"Suprovat Ghosh,&nbsp;Abir Mukherjee,&nbsp;Sudarshan Singh,&nbsp;Samit K Ray,&nbsp;Ananjan Basu,&nbsp;Santanu Manna and Samaresh Das*,&nbsp;","doi":"10.1021/acsaom.4c0029810.1021/acsaom.4c00298","DOIUrl":"https://doi.org/10.1021/acsaom.4c00298https://doi.org/10.1021/acsaom.4c00298","url":null,"abstract":"<p >This article explores group-IV germanium (Ge) quantum dots (QDs) on silicon-on-insulator (SOI) grown by molecular beam epitaxy (MBE) in order to explore their optical behavior in the terahertz (THz) regime. In this work, Ge QDs, pumped by an above bandgap near–infrared wavelength, exhibit THz amplitude modulation in the frequency range of 0.1–1.0 THz. The epitaxial Ge QDs outperform the reference SOI (170 nm top Si) substrate in THz amplitude modulation due to higher carrier generation in weakly confined dots compared to their bulk counterpart. This is further corroborated using a theoretical model based on the nonequilibrium Green’s function (NEGF) method. This model enables the calculation of photocarrier generated (PCG) and their confinement in the Ge QD region. Our model also reroutes the calculation from PCG to the corresponding plasma frequency and hence to refractive index and THz photoconductivity. Moreover, the photogenerated confined holes’ accumulation at the Ge QDs/Si interface is elevated after optical illumination, leading to decreased THz photoconductivity. This augmentation in THz photoconductivity contributes to a significant enhancement of THz modulation depth of ∼77% at Ge QDs/Si interfaces compared to bare SOI at 0.1 THz.</p>","PeriodicalId":29803,"journal":{"name":"ACS Applied Optical Materials","volume":"2 10","pages":"2085–2091 2085–2091"},"PeriodicalIF":0.0,"publicationDate":"2024-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142516877","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Phototransistors of Engineered InGaZnO Channel for Specific Molecular Detection in the Visible Range 用于可见光范围内特定分子检测的工程 InGaZnO 沟道光电晶体管
ACS Applied Optical Materials Pub Date : 2024-10-03 DOI: 10.1021/acsaom.4c0031010.1021/acsaom.4c00310
Yupeng Yang, Mohammad Hadi Khaksaran, Jong Bin An, Sujin Lee, Hyun Jae Kim, Ted Johansson, Xi Lu, Ilya Sychugov, Apurba Dev and Shi-Li Zhang*, 
{"title":"Phototransistors of Engineered InGaZnO Channel for Specific Molecular Detection in the Visible Range","authors":"Yupeng Yang,&nbsp;Mohammad Hadi Khaksaran,&nbsp;Jong Bin An,&nbsp;Sujin Lee,&nbsp;Hyun Jae Kim,&nbsp;Ted Johansson,&nbsp;Xi Lu,&nbsp;Ilya Sychugov,&nbsp;Apurba Dev and Shi-Li Zhang*,&nbsp;","doi":"10.1021/acsaom.4c0031010.1021/acsaom.4c00310","DOIUrl":"https://doi.org/10.1021/acsaom.4c00310https://doi.org/10.1021/acsaom.4c00310","url":null,"abstract":"<p >Fluorescence-based single-molecule detection has been widely investigated and applied in biosensing and bioimaging due to its ultrahigh sensitivity and specificity. However, bulky and expensive commercial fluorescence microscopes are usually required. The Stokes shift property of most commonly used fluorophores requires optical sets such as dichroic mirrors and specific filters in the optical pathway before a photodetector to eliminate excitation and scattering lights from the fluorescence signals. The fluorescence signal collected by an objective is further unavoidably attenuated, and the optical resolution is diffraction-limited. Herein, a proof of concept of a lab-on-a-chip compatible molecular sensor is shown by integrating upconversion nanoparticles (UCNPs) and amorphous hydrogen-doped InGaZnO (InGaZnO:H) thin-film phototransistor (IGZO:H TFTs) aiming to alleviate those issues. Upon illumination with a 980 nm infrared light, the phototransistor shows no photocurrent without UCNPs but yields a high photocurrent with UV–visible fluorescent light emitted from the UCNPs. The molecular detection is enabled by further involving the Förster resonance energy transfer (FRET) mechanism, with the UCNPs as donors. The photocurrent falls back to its original low level when biotinylated gold nanoparticles are added to selectively bind and quench the UCNPs via biotin–streptavidin coupling. Each UCNP shows an estimated photocurrent-to-dark current ratio of 10<sup>3</sup> and each biotinylated gold nanoparticle causes at least 1 order of magnitude decrease of the photocurrent. Our integrated setup presents a promising platform for further development toward an optoelectronic biosensor capable of single-molecule detection.</p>","PeriodicalId":29803,"journal":{"name":"ACS Applied Optical Materials","volume":"2 10","pages":"2092–2100 2092–2100"},"PeriodicalIF":0.0,"publicationDate":"2024-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsaom.4c00310","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142517088","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Fluorescent Chemosensor for Pyrophosphate via Aggregation-Induced Emission and Principal Component Analysis 通过聚合诱导发射和主成分分析检测焦磷酸的荧光化学传感器
ACS Applied Optical Materials Pub Date : 2024-10-02 DOI: 10.1021/acsaom.4c0035210.1021/acsaom.4c00352
Tanjila Islam, Yan Zhao, Fatma Nur Arslan, Ziqi Yu and Kirk Schanze*, 
{"title":"Fluorescent Chemosensor for Pyrophosphate via Aggregation-Induced Emission and Principal Component Analysis","authors":"Tanjila Islam,&nbsp;Yan Zhao,&nbsp;Fatma Nur Arslan,&nbsp;Ziqi Yu and Kirk Schanze*,&nbsp;","doi":"10.1021/acsaom.4c0035210.1021/acsaom.4c00352","DOIUrl":"https://doi.org/10.1021/acsaom.4c00352https://doi.org/10.1021/acsaom.4c00352","url":null,"abstract":"<p >The fluorescent chemosensor <b>TPE-NH</b><sub><b>3</b></sub>, a derivative of tetraphenylethylene (TPE), substituted with four cationic ammonium groups, was developed for the selective detection of pyrophosphate (PPi) anion. With inherent aggregation-induced emission (AIE) characteristics, <b>TPE-NH</b><sub><b>3</b></sub> displays strong fluorescence enhancement accompanied by a blue shift upon interacting with PPi. The probe exhibits good selectivity toward PPi over ten other anions that were tested. The interactions between <b>TPE-NH</b><sub><b>3</b></sub> and PPi were investigated using Job plot analysis and molecular dynamics simulations. Dynamic light scattering measurements demonstrated a 4.5-fold increase in particle size of the aggregates after the addition of PPi. The morphology of these aggregates has been investigated using transmission electron microscopy and confocal fluorescence lifetime imaging microscopy analyses. Principal component analysis (PCA) was applied to quantify the PPi concentration in unknown samples, giving good accuracy and precision with a relatively low limit of detection (77 nM) and respectable error margins (0.06–8.96%). This combined AIE-based sensing and PCA approach provides a robust, sensitive method for selective PPi detection with significant potential for biomedical and environmental applications.</p>","PeriodicalId":29803,"journal":{"name":"ACS Applied Optical Materials","volume":"2 10","pages":"2208–2219 2208–2219"},"PeriodicalIF":0.0,"publicationDate":"2024-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142517362","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
PbS/CdS Core/Shell Quantum Dots Designed to Enable Efficient Photon Upconversion for Solar Energy Applications 设计用于太阳能应用的高效光子上转换的 PbS/CdS 核/壳量子点
ACS Applied Optical Materials Pub Date : 2024-09-28 DOI: 10.1021/acsaom.4c0034010.1021/acsaom.4c00340
Tory A. Welsch,  and , Matthew F. Doty*, 
{"title":"PbS/CdS Core/Shell Quantum Dots Designed to Enable Efficient Photon Upconversion for Solar Energy Applications","authors":"Tory A. Welsch,&nbsp; and ,&nbsp;Matthew F. Doty*,&nbsp;","doi":"10.1021/acsaom.4c0034010.1021/acsaom.4c00340","DOIUrl":"https://doi.org/10.1021/acsaom.4c00340https://doi.org/10.1021/acsaom.4c00340","url":null,"abstract":"<p >Colloidal semiconductor quantum dot heterostructures are an attractive platform for photon upconversion in solar energy applications due to their wide absorption bandwidths and highly tunable optical properties. NIR-to-visible photon upconversion has been previously demonstrated in PbS/CdS/CdSe core/multishell heterostructures, but their reported upconversion efficiencies are low. The upconversion performance could be significantly improved by engineering the PbS/CdS core/shell intermediate structure to achieve the quasi-type II band structure and carrier separation behavior known to promote the upconversion process. Here we address two critical challenges to realizing an optimized PbS/CdS intermediate structure that could enable efficient upconversion in full PbS/CdS/CdSe structures. We first use computational simulations to predict the band alignment and carrier behavior in PbS/CdS and PbS/CdS/CdSe as a function of PbS core size and CdS shell thickness. We use the results to develop synthesis targets for PbS/CdS predicted to achieve effective carrier separation and improved upconversion performance. Next, we synthesize a library of PbS/CdS quantum dots via cation exchange across three particle sizes. We analyze the reaction products using absorbance, PL, and transmission electron microscopy to create a framework for the predictive synthesis of PbS/CdS with the target core and shell dimensions. Finally, we combine our computational and experimental findings to identify and understand a trade-off in design and synthetic factors required to realize PbS/CdS structures that provide a foundation for efficient NIR-to-visible upconversion.</p>","PeriodicalId":29803,"journal":{"name":"ACS Applied Optical Materials","volume":"2 10","pages":"2184–2195 2184–2195"},"PeriodicalIF":0.0,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142517752","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Upconversion Optical Materials 上转换光学材料
ACS Applied Optical Materials Pub Date : 2024-09-27 DOI: 10.1021/acsaom.4c0034310.1021/acsaom.4c00343
Felix N. Castellano, 
{"title":"Upconversion Optical Materials","authors":"Felix N. Castellano,&nbsp;","doi":"10.1021/acsaom.4c0034310.1021/acsaom.4c00343","DOIUrl":"https://doi.org/10.1021/acsaom.4c00343https://doi.org/10.1021/acsaom.4c00343","url":null,"abstract":"","PeriodicalId":29803,"journal":{"name":"ACS Applied Optical Materials","volume":"2 9","pages":"1731–1732 1731–1732"},"PeriodicalIF":0.0,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142326161","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Mixed Chalcogenides Nanoflakes’ Infrared Cutting Effect: Utilization in Thermal Soothing Electrochromic Goggles 混合钙钛矿纳米片的红外切割效应:在热舒缓电致变色护目镜中的应用
ACS Applied Optical Materials Pub Date : 2024-09-26 DOI: 10.1021/acsaom.4c0032510.1021/acsaom.4c00325
Bhumika Sahu, Love Bansal, Nikita Ahlawat, Anjali Ghanghass, Deb Kumar Rath, Subin Kaladi Chondath, Suchita Kandpal, Ravi Bhatia, Ivaturi Sameera* and Rajesh Kumar*, 
{"title":"Mixed Chalcogenides Nanoflakes’ Infrared Cutting Effect: Utilization in Thermal Soothing Electrochromic Goggles","authors":"Bhumika Sahu,&nbsp;Love Bansal,&nbsp;Nikita Ahlawat,&nbsp;Anjali Ghanghass,&nbsp;Deb Kumar Rath,&nbsp;Subin Kaladi Chondath,&nbsp;Suchita Kandpal,&nbsp;Ravi Bhatia,&nbsp;Ivaturi Sameera* and Rajesh Kumar*,&nbsp;","doi":"10.1021/acsaom.4c0032510.1021/acsaom.4c00325","DOIUrl":"https://doi.org/10.1021/acsaom.4c00325https://doi.org/10.1021/acsaom.4c00325","url":null,"abstract":"<p >A highly flexible prototype goggle with heat filtering capabilities has been built and demonstrated to have a heat soothing effect achieved through electrochromic modulation in the near-infrared (NIR) region. A flexible electrochromic device is designed by the doping of a WS<sub>2</sub>/WO<sub>3</sub> mixture, in P3HT-EV-based electrochromic active materials, which makes the devices switch in ∼1 s, making it one of the fastest devices in the family. The fully flexible NIR cutting electrochromic device (flex-NIR cutting-ECD) shows high NIR shielding by maintaining a temperature difference of up to 6 °C and cuts more than 15% of the heat when in the ON state. The device shows an optical modulation of up to 60% and a photopic coloration effeciency of 34 cm<sup>2</sup>/C along with a cyclic staibility of more than 100 toggles. The real world applicability has been demonstrated by making mini-goggles which change color between blue and magenta and cut heat making a way for a heat-calming eye-care gadget with bendable and twistable properties.</p>","PeriodicalId":29803,"journal":{"name":"ACS Applied Optical Materials","volume":"2 10","pages":"2128–2136 2128–2136"},"PeriodicalIF":0.0,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142555528","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Enhancing the X-ray Sensitivity of Cs2AgBiBr6 Double Perovskite Single Crystals through Cation Engineering. 通过阳离子工程提高 Cs2AgBiBr6 双包晶单晶的 X 射线灵敏度
ACS Applied Optical Materials Pub Date : 2024-09-26 eCollection Date: 2024-10-25 DOI: 10.1021/acsaom.4c00265
Donato Valli, Heng Zhang, Marián Betušiak, Giacomo Romolini, Arne Meulemans, Daniel Escudero, Sudipta Seth, Qing Zhao, Zonglong Zhu, Mischa Bonn, Eduard Belas, Roman Grill, Hai Wang, Johan Hofkens, Elke Debroye
{"title":"Enhancing the X-ray Sensitivity of Cs<sub>2</sub>AgBiBr<sub>6</sub> Double Perovskite Single Crystals through Cation Engineering.","authors":"Donato Valli, Heng Zhang, Marián Betušiak, Giacomo Romolini, Arne Meulemans, Daniel Escudero, Sudipta Seth, Qing Zhao, Zonglong Zhu, Mischa Bonn, Eduard Belas, Roman Grill, Hai Wang, Johan Hofkens, Elke Debroye","doi":"10.1021/acsaom.4c00265","DOIUrl":"10.1021/acsaom.4c00265","url":null,"abstract":"<p><p>Owing to their outstanding optoelectronic properties, halide perovskite (HP) materials have been employed in a wide range of applications, including solar cells, light-emitting devices, and X-ray detectors. Among them, lead-free double HPs are characterized by enhanced stability and reduced toxicity compared with lead-based alternatives. Cs<sub>2</sub>AgBiBr<sub>6</sub>, in particular, has emerged as a promising candidate for direct X-ray detection. The detection sensitivity, on the other hand, cannot yet compete with that of lead-containing perovskites. Developing schemes to improve X-ray detection efficiency is critical for reducing radiation exposure in medical imaging applications. Here, we investigate the potential of controlled doping and cation substitution with either lanthanides or small organic cations to improve the X-ray detection performance of Cs<sub>2</sub>AgBiBr<sub>6</sub>. Our findings reveal that by growing the perovskite in a slightly Bi-poor and Eu-rich environment, the X-ray sensitivity significantly increases 7-fold (from 17 to 120 μC Gy<sub>air</sub> <sup>-1</sup> cm<sup>-2</sup>) and simultaneously improves the phototo-dark current ratio (from 2.5 to 29). Additionally, Cs-site substitution with imidazolium remarkably enhances the sensitivity over 10-fold (180 μC Gy<sub>air</sub> <sup>-1</sup> cm<sup>-2</sup>), and ammonium enhances the phototo-dark current ratio to 37. Terahertz photoconductivity measurements reveal a positive correlation between enhanced X-ray sensitivity and improved charge transport properties (e.g., increased scattering time and, thus, carrier mobility) by doping. This study outlines straightforward strategies for boosting X-ray detection and fundamental photoconductivity in lead-free double HP, with potential implications for broader optoelectronic applications.</p>","PeriodicalId":29803,"journal":{"name":"ACS Applied Optical Materials","volume":"2 10","pages":"2075-2084"},"PeriodicalIF":0.0,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11519909/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142547979","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Single Particle Insights into the Thermal Sensing of Conjugated Polyelectrolyte–Nanoparticle Assemblies 对共轭聚电解质-纳米粒子组合热感应的单粒子洞察
ACS Applied Optical Materials Pub Date : 2024-09-26 DOI: 10.1021/acsaom.4c0032110.1021/acsaom.4c00321
Kareem Alhafi, Nour Merhi and Pierre Karam*, 
{"title":"Single Particle Insights into the Thermal Sensing of Conjugated Polyelectrolyte–Nanoparticle Assemblies","authors":"Kareem Alhafi,&nbsp;Nour Merhi and Pierre Karam*,&nbsp;","doi":"10.1021/acsaom.4c0032110.1021/acsaom.4c00321","DOIUrl":"https://doi.org/10.1021/acsaom.4c00321https://doi.org/10.1021/acsaom.4c00321","url":null,"abstract":"<p >Developing sensitive temperature sensors for nano- and microscale applications has become critical in many fields. In this work, we report on the use of anionic poly[5-methoxy-2-(3-sulfopropoxy)-1,4-phenylenevinylene] conjugated polyelectrolyte (CPE) as a thermal sensor upon its interaction with poly(1-vinylpyrrolidone-<i>co</i>-styrene) (PVP-<i>co</i>-PS) nanoparticles. The concentration of CPE was optimized to adopt a collapsed state at room temperature when assembled onto the PVP-<i>co</i>-PS nanoparticles with the ability to extend its backbone upon heating. This configuration allowed for the observation of fluorescence enhancement at higher temperatures. The relative sensitivity of the sensor was calculated to be equal to 1.57% at 40 °C with a linear range between 20 and 90 °C. The photophysical properties of the thermal nanoparticles’ sensor were studied at the single-particle level. Intensity-time traces and emission spectra collected from single nanoparticles validated the structural–spectroscopic correlation with the observed thermal response, which we believe can be generalized to many similar conjugated polyelectrolyte systems.</p>","PeriodicalId":29803,"journal":{"name":"ACS Applied Optical Materials","volume":"2 10","pages":"2118–2127 2118–2127"},"PeriodicalIF":0.0,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsaom.4c00321","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142517621","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Enhancing the X-ray Sensitivity of Cs2AgBiBr6 Double Perovskite Single Crystals through Cation Engineering 通过阳离子工程提高 Cs2AgBiBr6 双包晶石单晶的 X 射线灵敏度
ACS Applied Optical Materials Pub Date : 2024-09-26 DOI: 10.1021/acsaom.4c0026510.1021/acsaom.4c00265
Donato Valli, Heng Zhang, Marián Betušiak, Giacomo Romolini, Arne Meulemans, Daniel Escudero, Sudipta Seth, Qing Zhao, Zonglong Zhu, Mischa Bonn, Eduard Belas, Roman Grill, Hai Wang, Johan Hofkens and Elke Debroye*, 
{"title":"Enhancing the X-ray Sensitivity of Cs2AgBiBr6 Double Perovskite Single Crystals through Cation Engineering","authors":"Donato Valli,&nbsp;Heng Zhang,&nbsp;Marián Betušiak,&nbsp;Giacomo Romolini,&nbsp;Arne Meulemans,&nbsp;Daniel Escudero,&nbsp;Sudipta Seth,&nbsp;Qing Zhao,&nbsp;Zonglong Zhu,&nbsp;Mischa Bonn,&nbsp;Eduard Belas,&nbsp;Roman Grill,&nbsp;Hai Wang,&nbsp;Johan Hofkens and Elke Debroye*,&nbsp;","doi":"10.1021/acsaom.4c0026510.1021/acsaom.4c00265","DOIUrl":"https://doi.org/10.1021/acsaom.4c00265https://doi.org/10.1021/acsaom.4c00265","url":null,"abstract":"<p >Owing to their outstanding optoelectronic properties, halide perovskite (HP) materials have been employed in a wide range of applications, including solar cells, light-emitting devices, and X-ray detectors. Among them, lead-free double HPs are characterized by enhanced stability and reduced toxicity compared with lead-based alternatives. Cs<sub>2</sub>AgBiBr<sub>6</sub>, in particular, has emerged as a promising candidate for direct X-ray detection. The detection sensitivity, on the other hand, cannot yet compete with that of lead-containing perovskites. Developing schemes to improve X-ray detection efficiency is critical for reducing radiation exposure in medical imaging applications. Here, we investigate the potential of controlled doping and cation substitution with either lanthanides or small organic cations to improve the X-ray detection performance of Cs<sub>2</sub>AgBiBr<sub>6</sub>. Our findings reveal that by growing the perovskite in a slightly Bi-poor and Eu-rich environment, the X-ray sensitivity significantly increases 7-fold (from 17 to 120 μC Gy<sub>air</sub><sup>–1</sup> cm<sup>–2</sup>) and simultaneously improves the phototo-dark current ratio (from 2.5 to 29). Additionally, Cs-site substitution with imidazolium remarkably enhances the sensitivity over 10-fold (180 μC Gy<sub>air</sub><sup>–1</sup> cm<sup>–2</sup>), and ammonium enhances the phototo-dark current ratio to 37. Terahertz photoconductivity measurements reveal a positive correlation between enhanced X-ray sensitivity and improved charge transport properties (e.g., increased scattering time and, thus, carrier mobility) by doping. This study outlines straightforward strategies for boosting X-ray detection and fundamental photoconductivity in lead-free double HP, with potential implications for broader optoelectronic applications.</p>","PeriodicalId":29803,"journal":{"name":"ACS Applied Optical Materials","volume":"2 10","pages":"2075–2084 2075–2084"},"PeriodicalIF":0.0,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsaom.4c00265","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142555529","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Enhanced Efficiency in Green PhOLEDs Using a Simplified Three-Layer Architecture with Bipolar Carbazole–Quinazolinone Hosts 利用具有双极咔唑-喹唑啉酮宿主的简化三层结构提高绿色 PhOLED 的效率
ACS Applied Optical Materials Pub Date : 2024-09-21 DOI: 10.1021/acsaom.4c0022810.1021/acsaom.4c00228
Hemant Keshari, Namira Ansari, Yi-Ting Chen, Yi-Qi Chao, Chih-Hao Chang*, Vipin Kumar, Prabhakar Chetti and Atul Chaskar*, 
{"title":"Enhanced Efficiency in Green PhOLEDs Using a Simplified Three-Layer Architecture with Bipolar Carbazole–Quinazolinone Hosts","authors":"Hemant Keshari,&nbsp;Namira Ansari,&nbsp;Yi-Ting Chen,&nbsp;Yi-Qi Chao,&nbsp;Chih-Hao Chang*,&nbsp;Vipin Kumar,&nbsp;Prabhakar Chetti and Atul Chaskar*,&nbsp;","doi":"10.1021/acsaom.4c0022810.1021/acsaom.4c00228","DOIUrl":"https://doi.org/10.1021/acsaom.4c00228https://doi.org/10.1021/acsaom.4c00228","url":null,"abstract":"<p >With an aim to provide a balanced charge flux for enhanced PhOLED device efficiency, two novel bipolar host materials, <b>3-CBZ-QZ</b> and <b>9-CBZ-QZ</b>, incorporating carbazole and quinazolinone as the electron donor and acceptor, respectively, have been synthesized, characterized, and used as efficient host materials for phosphorescent devices. Furthermore, their photophysical, thermal, and electrochemical properties have been investigated to shed the importance on the structure–performance relationship. <b>3-CBZ-QZ</b> and <b>9-CBZ-QZ</b> have high triplet energies of 3.09 and 2.54 eV, respectively, which make them suitable host materials for green emitters in the emissive layer (EML). DFT studies reveal high charge mobilities for both synthesized molecules based on electron and hole reorganization energy calculations. This balanced charge-carrying capacity prompted us to fabricate simple three-layer devices with a single hole and electron transport layer across the EML. The <b>3-CBZ-QZ</b>-based device resulted in a superior electroluminescent (EL) performance with a turn-on voltage of 2.6 V, a maximum luminance of 77973 cd/m<sup>2</sup>, a maximum power efficiency of 71.0 Im/W, and an EQE of 18.1%. Although devices with the <b>9-CBZ-QZ</b> host demonstrated a lower EQE of 16.0%, it showed a higher luminance value of 91111 cd/m<sup>2</sup> than <b>3-CBZ-QZ</b> with a significantly lower efficiency roll-off at a higher practical luminance of 100 cd/m<sup>2</sup>. The EL characteristics significantly varied with the positional changes in the donor–acceptor linkage. Moreover, these recorded performances demonstrate the promising advantage of the carbazole–quinoxaline-based compounds in developing host materials for realizing efficient PhOLEDs.</p>","PeriodicalId":29803,"journal":{"name":"ACS Applied Optical Materials","volume":"2 10","pages":"2039–2050 2039–2050"},"PeriodicalIF":0.0,"publicationDate":"2024-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142550524","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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