ACS Photonics最新文献

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Short-Wave Infrared Optoelectronics with Colloidal CdHgSe/ZnCdS Core/Shell Nanoplatelets
IF 7 1区 物理与天体物理
ACS Photonics Pub Date : 2024-12-19 DOI: 10.1021/acsphotonics.4c01944
Hossein Roshan, Anatol Prudnikau, Jinfei Dai, Matilde Cirignano, Francesco De Boni, Mirko Prato, Fabian Paulus, Vladimir Lesnyak, Francesco Di Stasio
{"title":"Short-Wave Infrared Optoelectronics with Colloidal CdHgSe/ZnCdS Core/Shell Nanoplatelets","authors":"Hossein Roshan, Anatol Prudnikau, Jinfei Dai, Matilde Cirignano, Francesco De Boni, Mirko Prato, Fabian Paulus, Vladimir Lesnyak, Francesco Di Stasio","doi":"10.1021/acsphotonics.4c01944","DOIUrl":"https://doi.org/10.1021/acsphotonics.4c01944","url":null,"abstract":"Colloidal semiconductor nanocrystals (NCs) are an efficient and cost-effective class of nanomaterials for optoelectronic applications. Advancements in NC-based optoelectronic devices have resulted from progress in synthetic chemistry, adjustable surface properties, and optimized device architectures. Semiconductor nanoplatelets (NPLs) stand out among other NCs due to their precise growth control, yielding uniform thickness with submonolayer roughness. In this study, we demonstrate the versatility of core/shell Cd<sub><i>x</i></sub>Hg<sub>1–<i>x</i></sub>Se/Zn<sub><i>y</i></sub>Cd<sub>1–<i>y</i></sub>S NPLs for optoelectronic applications in the short-wave infrared (SWIR) spectral range. We employed the very same core/shell NPLs for the fabrication of light-emitting diodes and photodetectors alike, achieving significant performance in both electroluminescence (external quantum efficiency ranging from 7.5% at 1280 nm to 3.8% at 1550 nm) and detection (responsivity of 0.24 A W<sup>–1</sup> at 1200 nm).","PeriodicalId":23,"journal":{"name":"ACS Photonics","volume":"23 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142857647","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}
引用次数: 0
Chip-Scale Single-Beam Atomic Magnetometer Enabled by Spin-Selective Interference Meta-Optics
IF 7 1区 物理与天体物理
ACS Photonics Pub Date : 2024-12-19 DOI: 10.1021/acsphotonics.4c01638
Jinsheng Hu, Zihua Liang, Peng Zhou, Lu Liu, Gen Hu, Mao Ye
{"title":"Chip-Scale Single-Beam Atomic Magnetometer Enabled by Spin-Selective Interference Meta-Optics","authors":"Jinsheng Hu, Zihua Liang, Peng Zhou, Lu Liu, Gen Hu, Mao Ye","doi":"10.1021/acsphotonics.4c01638","DOIUrl":"https://doi.org/10.1021/acsphotonics.4c01638","url":null,"abstract":"Emerging atomic magnetometers (AMs) are among the most advanced sensors for detecting and characterizing magnetic fields. Recently, there has been growing interest in the miniaturization and integration of AMs due to the urgent demand for portability and compactness in various fields such as biomagnetism imaging. While conventional AMs require a bulky setup of optical devices for the pumping and optical readout of atomic spin, here, a novel chip-scale single-beam AM scheme is proposed by leveraging extreme transmissive circular polarization dichroism (TCPD) and geometric phase manipulation of spin-selective interference meta-optics. This is achieved through silicon-based metasurfaces that enable the realization of arbitrary-to-circular polarization conversion and wavefront modulation within a monolithic chip at Rb D1 transition wavelength (λ = 795 nm). Two spin-selective interference metasurfaces, i.e., meta-circular-polarizer (MCP) and meta-circular-polarizer-lens (MCPL), are fabricated and characterized, with a measured TCPD of 0.68 for the MCP as well as focusing efficiency and TCPD of around 70.67% and 0.69 for the MCPL, respectively. As a proof of concept, a 4 × 4 × 4 mm<sup>3</sup> Rb vapor cell is combined with our metasurface to construct a miniaturized single-beam AM. The sensitivity of our compact metasurface-based system is about 15 fT/Hz<sup>1/2</sup>, with a dynamic range near zero-field of ± 2.2 nT. We envision that this work could facilitate the development of burgeoning chip-scale quantum sensors, which hold great potential for high-spatial-resolution biomagnetic imaging, on-chip nuclear magnetic resonance, and so forth.","PeriodicalId":23,"journal":{"name":"ACS Photonics","volume":"28 9 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142857644","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}
引用次数: 0
Probing Nanogap-Dependent Plasmonic Coupling in Gold Nanoparticle Superlattices by Scanning Tunneling Microscopy Induced Light Emission 通过扫描隧道显微镜诱导光发射探测金纳米粒子超晶格中依赖于纳米间隙的等离子耦合
IF 7 1区 物理与天体物理
ACS Photonics Pub Date : 2024-12-19 DOI: 10.1021/acsphotonics.4c01408
Yalan Ma, Bin Lu, Olivier J. F. Martin, Andreas Stemmer
{"title":"Probing Nanogap-Dependent Plasmonic Coupling in Gold Nanoparticle Superlattices by Scanning Tunneling Microscopy Induced Light Emission","authors":"Yalan Ma, Bin Lu, Olivier J. F. Martin, Andreas Stemmer","doi":"10.1021/acsphotonics.4c01408","DOIUrl":"https://doi.org/10.1021/acsphotonics.4c01408","url":null,"abstract":"Plasmonic nanogaps can support confined and enhanced electromagnetic fields. In this work, we use scanning tunneling microscopy-induced light emission (STM-LE) to study the localized surface plasmon resonance of gold nanoparticle superlattices, which consist of high-density nanogaps of tunable sizes (from 0.1 to 2.3 nm). By analyzing the far-field light emission, we discover that two distinct plasmon modes, i.e., the transverse dipolar plasmon mode (TDP) and bonding dipolar plasmon (BDP) mode, can be selectively excited depending on the location of the STM tip. As the interparticle gap distance decreases, the BDP mode excited at the plasmonic nanogaps shows a monotonous red-shift and broadening, indicating continuously enhanced interparticle plasmonic coupling. Moreover, we observe a stronger radiative strength of the BDP mode compared to the TDP mode excited at the nanoparticles, demonstrating that the plasmonic nanogaps act as electromagnetic hot spots. The intensity ratio of the BDP mode to the TDP mode is enhanced with decreased gap size down to the unprecedent 0.1 nm, revealing the extreme field confinement that can be achieved in plasmonic superlattices. Our results advance the understanding of near-field enhancement in subnanometer plasmonic gaps and shall benefit the design of plasmonic structures for applications in many fields, including surface enhance Raman spectroscopy, photocatalysis, and optoelectronics.","PeriodicalId":23,"journal":{"name":"ACS Photonics","volume":"53 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849296","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}
引用次数: 0
Nanoscale Vectorial Electric and Magnetic Field Measurement 纳米级矢量电场和磁场测量
IF 7 1区 物理与天体物理
ACS Photonics Pub Date : 2024-12-19 DOI: 10.1021/acsphotonics.4c01831
Jörg S. Eismann, Peter Banzer
{"title":"Nanoscale Vectorial Electric and Magnetic Field Measurement","authors":"Jörg S. Eismann, Peter Banzer","doi":"10.1021/acsphotonics.4c01831","DOIUrl":"https://doi.org/10.1021/acsphotonics.4c01831","url":null,"abstract":"In technology, old or new, from basic imaging through a camera lens to advanced applications such as fluorescence microscopy and optical lithography, there are countless examples that would be inconceivable without the utilization of focused light. As technology evolves, the demands on spatially confined light fields grow but so do the challenges of accurately characterizing these complex fields. This study introduces a technique to measure the full vectorial nature of light, reaching sub/wavelength spatial resolution while capturing the 3D amplitude and phase for both electric and magnetic fields. This is achieved based on a polarization-resolved far-field analysis of light scattered by a single spherical nanoparticle acting as a local probe. For experimental verification, the method is applied to tightly focused light fields under various input scenarios. Offering high resolution, precision, and flexibility, this technique shows great promise for both fundamental research and applications in technologies relying on highly localized light fields.","PeriodicalId":23,"journal":{"name":"ACS Photonics","volume":"23 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849302","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}
引用次数: 0
Anisotropic Photophysical Properties of Plexcitons in Strongly Coupled Metal–Organic Thin Films 强耦合金属有机薄膜中的各向异性丛生子光物理性质
IF 7 1区 物理与天体物理
ACS Photonics Pub Date : 2024-12-19 DOI: 10.1021/acsphotonics.4c01219
Maximilian Rödel, Luca Nils Philipp, Jin Hong Kim, Matthias Lehmann, Matthias Stolte, Roland Mitric, Frank Würthner, Jens Pflaum
{"title":"Anisotropic Photophysical Properties of Plexcitons in Strongly Coupled Metal–Organic Thin Films","authors":"Maximilian Rödel, Luca Nils Philipp, Jin Hong Kim, Matthias Lehmann, Matthias Stolte, Roland Mitric, Frank Würthner, Jens Pflaum","doi":"10.1021/acsphotonics.4c01219","DOIUrl":"https://doi.org/10.1021/acsphotonics.4c01219","url":null,"abstract":"Exciton–plasmon polaritons have gained increasing interest over recent years due to their versatile properties emerging by the underlying light–matter coupling and making them potential candidates for new photonic applications. We have advanced this concept by studying thin films of laterally aligned J-aggregates of self-assembled tetra-bay phenoxy-dendronized perylene bisimide (PBI) molecules, arranged in a helical manner of three slip-stacked strands on a silver surface. As a result of the interaction between the uniformly aligned dipole moments and the surface plasmons of a thin silver layer underneath, the excitonic state at 1.94 eV evolves into dispersions in absorption and emission, both characterized by distinct anisotropy. The coupling constant defined by the scalar product of the transition dipole moment μ⃗ and the surface plasmon wavevector <i>k⃗</i><sub><i>x</i></sub> shows a pronounced 2-fold rotational symmetry with values between almost 0 and 29.5 meV. Complementary time-dependent density functional theory (TD-DFT) calculations of the angular-dependent absorption and photoluminescence (PL) provide insights in the coherent energy exchange between the excitonic and plasmonic subsystems. Additionally, power-dependent PL studies yield first evidence that the diffusion length of the coupled exciton–plasmon polaritons exceeds that of the mere Frenkel state in neat PBI-based J-aggregates by at least 1 order of magnitude. Our results not only demonstrate the possibility to control the photophysical properties of strongly coupled states by their spatially anisotropic light–matter interaction but also reveal innovative strategies to influence optoelectronic device operation by the directional transport of hybrid-state energy.","PeriodicalId":23,"journal":{"name":"ACS Photonics","volume":"4 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849294","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}
引用次数: 0
Fast and Efficient Sub-Band Gap Photodetection in Al:ZnO/Si Heterojunction by Enhanced Photoexcited Hole Transport via Interfacial Defect States
IF 7 1区 物理与天体物理
ACS Photonics Pub Date : 2024-12-18 DOI: 10.1021/acsphotonics.4c01057
Geunpil Kim, Byung Chul Lee, Jongbum Kim
{"title":"Fast and Efficient Sub-Band Gap Photodetection in Al:ZnO/Si Heterojunction by Enhanced Photoexcited Hole Transport via Interfacial Defect States","authors":"Geunpil Kim, Byung Chul Lee, Jongbum Kim","doi":"10.1021/acsphotonics.4c01057","DOIUrl":"https://doi.org/10.1021/acsphotonics.4c01057","url":null,"abstract":"This study focuses on sub-band gap photodetection in n<sup>+</sup>-Al:ZnO/n-Si isotype heterojunction-based photodiodes via interfacial defects induced by metal oxide films. Through comparative studies on the photoresponse of Schottky junction-based photodiodes with the modified electronic band structure by controlling the structural and electrical properties of Al:ZnO films, as well as the Si substrate’s doping level, we investigate the underlying mechanisms of interfacial defect states for sub-band gap photodetection in Si. Our analysis suggests that these interfacial defects not only act as additional sources for photoexcited carrier generations but also serve as pathways for photogenerated holes in the Si valence band, enabling their flow into the Al:ZnO film and improving the operating speed. Time-resolved photocurrent measurements under near-infrared illumination illustrate an enhancement in photocurrent with lower oxygen partial pressures (0 mTorr) attributed to alterations in the energy band structure caused by interfacial defect states. Significantly, the Al:ZnO/Si photodiode fabricated under optimized conditions exhibits a photoresponse of 2.48 mA/W at 1310 nm with fast rise/fall times of 5.5/5.25 μs at 1 kHz and a 3 dB bandwidth of approximately 150 kHz, without introducing additional bulk trap states in Si. In light of these findings, the combination of simple fabrication and excellent switching speed of interfacial defect-mediated Si photodiodes has the potential to significantly impact the technologies of Si photonics and advanced Si-based photoelectric devices.","PeriodicalId":23,"journal":{"name":"ACS Photonics","volume":"48 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841677","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}
引用次数: 0
Confocal Raman Microscopy with Adaptive Optics
IF 7 1区 物理与天体物理
ACS Photonics Pub Date : 2024-12-18 DOI: 10.1021/acsphotonics.4c01432
Juan David Muñoz-Bolaños, Pouya Rajaeipour, Kai Kummer, Michaela Kress, Çag̃lar Ataman, Monika Ritsch-Marte, Alexander Jesacher
{"title":"Confocal Raman Microscopy with Adaptive Optics","authors":"Juan David Muñoz-Bolaños, Pouya Rajaeipour, Kai Kummer, Michaela Kress, Çag̃lar Ataman, Monika Ritsch-Marte, Alexander Jesacher","doi":"10.1021/acsphotonics.4c01432","DOIUrl":"https://doi.org/10.1021/acsphotonics.4c01432","url":null,"abstract":"Confocal Raman microscopy, a highly specific and label-free technique for the microscale study of thick samples, often presents difficulties due to weak Raman signals. Inhomogeneous samples introduce wavefront aberrations that further reduce these signals, requiring even longer acquisition times. In this study, we introduce Adaptive Optics to confocal Raman microscopy for the first time to counteract such aberrations, significantly increasing the Raman signal and image quality. The method is designed to integrate seamlessly with existing commercial microscopes without hardware modifications. It uses a wavefront sensorless approach to measure aberrations using an optofluidic, transmissive spatial light modulator that can be attached to the microscope nosepiece. Our experimental results demonstrate the compensation of aberrations caused by artificial scatterers and mouse brain tissue, improving spatial resolution and achieving up to 3.5-fold signal enhancements. Our results provide a basis for the molecular label-free study of biological systems at greater imaging depths.","PeriodicalId":23,"journal":{"name":"ACS Photonics","volume":"56 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841679","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}
引用次数: 0
Photonic Thermal Switch with Positive Differential Emissivity 具有正差分发射率的光子热开关
IF 7 1区 物理与天体物理
ACS Photonics Pub Date : 2024-12-18 DOI: 10.1021/acsphotonics.4c01696
Guillaume Boudan, Etienne Eustache, Laurent Divay, Dominique Carisetti, Riccardo Messina, Philippe Ben-Abdallah
{"title":"Photonic Thermal Switch with Positive Differential Emissivity","authors":"Guillaume Boudan, Etienne Eustache, Laurent Divay, Dominique Carisetti, Riccardo Messina, Philippe Ben-Abdallah","doi":"10.1021/acsphotonics.4c01696","DOIUrl":"https://doi.org/10.1021/acsphotonics.4c01696","url":null,"abstract":"Controlling temperature in solid-state devices is crucial as high temperatures can negatively impact their functionality, efficiency, speed, reliability, and lifespan. One way to manage this is by adjusting their radiative surface emission properties. Metal–insulator transition (MIT) materials, which have a critical temperature (<i>T</i><sub>c</sub>), have been proposed for thermal switches that drastically change their radiative properties around <i>T</i><sub>c</sub>. Typically, MIT materials become less emitting at high temperatures (negative differential emitter). This study introduces a broadband thermal switch with positive differential emitter behavior. Using a genetic algorithm, a composite multilayer structure based on vanadium dioxide (VO<sub>2</sub>) (an MIT material with a phase transition at <i>T</i><sub>c</sub> = 68 °C) films has been designed. The analysis of local losses within the switch reveals that its behavior is related to the soft metallic behavior of VO<sub>2</sub> films in the infrared spectrum beyond <i>T</i><sub>c</sub>, reducing electric field screening. The developed switch emits a heat flux of 59 W m<sup>–2</sup> below <i>T</i><sub>c</sub> and about six times more just above this temperature, which is 60% of the blackbody emission.","PeriodicalId":23,"journal":{"name":"ACS Photonics","volume":"22 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849297","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}
引用次数: 0
High-Sensitivity Detection of Chiro-Optical Effects in Single Nanoparticles by Four-Wave Mixing Interferometry 利用四波混合干涉测量法高灵敏度检测单个纳米粒子的奇光效应
IF 7 1区 物理与天体物理
ACS Photonics Pub Date : 2024-12-18 DOI: 10.1021/acsphotonics.4c01782
Paola Borri, Lukas Payne, Francesco Masia, Marco Esposito, Vittorianna Tasco, Adriana Passaseo, Wolfgang Langbein
{"title":"High-Sensitivity Detection of Chiro-Optical Effects in Single Nanoparticles by Four-Wave Mixing Interferometry","authors":"Paola Borri, Lukas Payne, Francesco Masia, Marco Esposito, Vittorianna Tasco, Adriana Passaseo, Wolfgang Langbein","doi":"10.1021/acsphotonics.4c01782","DOIUrl":"https://doi.org/10.1021/acsphotonics.4c01782","url":null,"abstract":"The field of chiral nanoparticles is rapidly expanding, yet measuring the chirality of single nano-objects remains a challenging endeavor. Here, we report a technique to detect chiro-optical effects in single plasmonic nanoparticles by means of phase-sensitive polarization-resolved four-wave mixing interferometric microscopy. Beyond conventional circular dichroism, the method is sensitive to the particle polarizability, in amplitude and phase. First, we demonstrate its application on single chiral nanohelices fabricated by focused ion beam induced deposition. We examined the combination of detected fields, which measures the particle polarizability, and showed that this is a sensitive reporter of chirality, providing dissymmetry factors (<i>g</i><sub>α</sub>) impressively approaching unity. We then applied the method to a set of individual small gold nanoparticles near the dipole limit (60 nm nominal size), having correspondingly small chiral effects from the intrinsic lattice defects and nonperfectly spherical shape. We find that <i>g</i><sub>α</sub> is randomly distributed in the population, consistent with its nondeterministic origin, but again exhibits remarkably high values, an order of magnitude higher than those obtained using conventional light absorption. Considering the importance of chiral plasmonic nanoparticles in fields ranging from catalysis to metamaterials, this technique offers a powerful way to quantify chiro-optical effects at the single particle level with unprecedented sensitivity.","PeriodicalId":23,"journal":{"name":"ACS Photonics","volume":"12 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849300","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}
引用次数: 0
Polaritonic Bright and Dark States Collectively Affect the Reactivity of a Hydrolysis Reaction
IF 7 1区 物理与天体物理
ACS Photonics Pub Date : 2024-12-17 DOI: 10.1021/acsphotonics.4c01630
Yulei Wang, Daniel Rosenmann, John V. Muntean, Xuedan Ma
{"title":"Polaritonic Bright and Dark States Collectively Affect the Reactivity of a Hydrolysis Reaction","authors":"Yulei Wang, Daniel Rosenmann, John V. Muntean, Xuedan Ma","doi":"10.1021/acsphotonics.4c01630","DOIUrl":"https://doi.org/10.1021/acsphotonics.4c01630","url":null,"abstract":"Vibrational strong coupling (VSC) has emerged as a means for modifying chemical reactivity. Despite the intriguing discoveries and progresses in the field, the precise mechanisms that govern polaritonic chemistry still deserve further interrogation. Herein, we use the hydrolysis of ammonia borane in D<sub>2</sub>O as an exemplary reaction and systematically investigate the influence of VSC on its reactivity. Experimental evidence of the coexistence of a resonant effect and reaction acceleration is observed in this system. In particular, we find that when the O–D stretching mode of D<sub>2</sub>O is strongly coupled to a cavity mode, reaction acceleration is observed. The reaction rate acceleration factor, μ, is consistently observed to be dependent on the coupling conditions between the vibrational and cavity modes, and reaches a minimum at zero mode detuning, suggesting that a resonant effect is likely in play. In addition, we find that μ decreases with an increasing Rabi splitting. Based on these experimental findings, we propose that the overall influence of VSC on this reaction is likely determined collectively by the polaritonic bright and dark states. These findings could help shed new light on the intricate effects of VSC on ground-state reaction landscapes.","PeriodicalId":23,"journal":{"name":"ACS Photonics","volume":"1 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832667","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}
引用次数: 0
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