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Multiplexed Near-IR Detection of Single-Molecule Fluorescence Fluctuations Using a Single Superconducting Nanowire Single-Photon Detector
IF 7 1区 物理与天体物理 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-03-28 DOI: 10.1021/acsphotonics.5c00224
Abhilash Kulkarni, Niusha Bagheri, Jerker Widengren
Fluorescence-based single-molecule and fluctuation spectroscopy in the near-IR can open avenues for biomolecular dynamic studies in biological media with suppressed autofluorescence and scattering background. However, further implementation is limited by the lower brightness of NIR fluorophores and available single-photon detector technologies that are still to be explored and adapted. Superconducting nanowire single-photon detectors (snSPDs) have found increasing use in quantum optics and optical communication applications thanks to high sensitivity in the near-infraed (NIR), low dark-counts, no after-pulsing, and high time resolution. Here, we present characterization of fluorescence intensity fluctuations from single vesicles and NIR fluorophores based on fluorescence correlation spectroscopy (FCS), specifically taking advantage of these snSPD properties. We present a concept allowing multiplexed readouts based on only one snSPD, in which the emitted photons are separated by their emission wavelength into different optical paths, thereby translating the emission wavelengths into different arrival times onto the snSPD. This concept allows one-laser-one-detector, dual-color fluorescence cross-correlation spectroscopy (FCCS) measurements, with fluorescence intensity fluctuations of two fluorophore species separately analyzed and cross-correlated. It is shown how two fluorophore species in a sample can be distinguished by their different blinking kinetics, fluorescence lifetimes, and/or diffusion properties. Apart from differences in emission spectra, the presented concept for multiplexing using a single detector can also be applied to distinguish emitters by properties such as polarization, coherence lengths, and fluorescence bunching and antibunching signatures. It can also be generalized to other modalities than FCS, including single-molecule detection, confocal microscopy, and imaging.
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引用次数: 0
Multiplexed Near-IR Detection of Single-Molecule Fluorescence Fluctuations Using a Single Superconducting Nanowire Single-Photon Detector
IF 6.5 1区 物理与天体物理 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-03-28 DOI: 10.1021/acsphotonics.5c0022410.1021/acsphotonics.5c00224
Abhilash Kulkarni, Niusha Bagheri and Jerker Widengren*, 

Fluorescence-based single-molecule and fluctuation spectroscopy in the near-IR can open avenues for biomolecular dynamic studies in biological media with suppressed autofluorescence and scattering background. However, further implementation is limited by the lower brightness of NIR fluorophores and available single-photon detector technologies that are still to be explored and adapted. Superconducting nanowire single-photon detectors (snSPDs) have found increasing use in quantum optics and optical communication applications thanks to high sensitivity in the near-infraed (NIR), low dark-counts, no after-pulsing, and high time resolution. Here, we present characterization of fluorescence intensity fluctuations from single vesicles and NIR fluorophores based on fluorescence correlation spectroscopy (FCS), specifically taking advantage of these snSPD properties. We present a concept allowing multiplexed readouts based on only one snSPD, in which the emitted photons are separated by their emission wavelength into different optical paths, thereby translating the emission wavelengths into different arrival times onto the snSPD. This concept allows one-laser-one-detector, dual-color fluorescence cross-correlation spectroscopy (FCCS) measurements, with fluorescence intensity fluctuations of two fluorophore species separately analyzed and cross-correlated. It is shown how two fluorophore species in a sample can be distinguished by their different blinking kinetics, fluorescence lifetimes, and/or diffusion properties. Apart from differences in emission spectra, the presented concept for multiplexing using a single detector can also be applied to distinguish emitters by properties such as polarization, coherence lengths, and fluorescence bunching and antibunching signatures. It can also be generalized to other modalities than FCS, including single-molecule detection, confocal microscopy, and imaging.

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引用次数: 0
Anisotropic Excitonic Photoluminescence Observed on Artificial Bilayer MoS2 with Heterostrain
IF 6.5 1区 物理与天体物理 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-03-27 DOI: 10.1021/acsphotonics.4c0253910.1021/acsphotonics.4c02539
Xiaoan Jiang, Xiaoxu Zhao, Weitao Su*, Fei Chen, Senjiang Yu, Yijie Zeng, Hong-Wei Lu and Peiqing Chen, 

In a moiré structure formed by isotropic semiconducting transition metal dichalcogenide (TMD), tuning the isotropic excitons to be anisotropic is quite challenging. Herein, by introducing controllable in-plane interlayer uniaxial strain to a MoS2 monolayer (ML) and stacking it to another unstrained ML MoS2, we successfully prepared an artificial bilayer (BL) moiré structure with heterostrain. The intralayer direct and indirect excitons within this structure demonstrate pronounced anisotropic photoluminescence (PL) emissions at both ambient and low temperatures. At 80 K, the PL anisotropic ratios of indirect and direct excitons can be enhanced to 1.45 and 1.31, respectively, in samples subjected to tensile heterostrain. These findings significantly advance our understanding of the anisotropic optical behaviors exhibited by moiré excitons of TMD materials, potentially paving the way for the design of future anisotropic twistronic devices.

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引用次数: 0
Anisotropic Excitonic Photoluminescence Observed on Artificial Bilayer MoS2 with Heterostrain
IF 7 1区 物理与天体物理 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-03-27 DOI: 10.1021/acsphotonics.4c02539
Xiaoan Jiang, Xiaoxu Zhao, Weitao Su, Fei Chen, Senjiang Yu, Yijie Zeng, Hong-Wei Lu, Peiqing Chen
In a moiré structure formed by isotropic semiconducting transition metal dichalcogenide (TMD), tuning the isotropic excitons to be anisotropic is quite challenging. Herein, by introducing controllable in-plane interlayer uniaxial strain to a MoS2 monolayer (ML) and stacking it to another unstrained ML MoS2, we successfully prepared an artificial bilayer (BL) moiré structure with heterostrain. The intralayer direct and indirect excitons within this structure demonstrate pronounced anisotropic photoluminescence (PL) emissions at both ambient and low temperatures. At 80 K, the PL anisotropic ratios of indirect and direct excitons can be enhanced to 1.45 and 1.31, respectively, in samples subjected to tensile heterostrain. These findings significantly advance our understanding of the anisotropic optical behaviors exhibited by moiré excitons of TMD materials, potentially paving the way for the design of future anisotropic twistronic devices.
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引用次数: 0
Intrinsic Optical Response of Levitating Upconverting Single Particles
IF 6.5 1区 物理与天体物理 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-03-27 DOI: 10.1021/acsphotonics.4c0202410.1021/acsphotonics.4c02024
Laura Martinez Maestro, Miguel A. Antón, Eduardo Cabrera-Granado, Rosa Weigand and Javier Hernandez-Rueda*, 

Today, upconverting luminescent particles are routinely used as accurate and reliable probes to remotely measure the temperature of minute volumes of matter on the order of attoliters. Lanthanide-doped particles exhibit adaptability as optical nanothermometers within biological systems, aiding the understanding of cellular dynamics, pathology, and physiology. Herein, we investigate the intrinsic optical response of Er/Yb-doped single particles levitating in a vacuum and compare it with the collective response of ensembles of particles embedded in application-relevant wet and dry environments. We make use of a quadrupole Paul trap that employs a time-varying electric field to confine single Er/Yb-doped particles in a vacuum and a thermal bath module to study particles in the above-mentioned environments. Both subsystems use twin-excitation/detection setups that allow us to record luminescence spectra, covering 4 orders of magnitude in laser intensity (e.g., 10–1–103 W/cm2 at 980 nm) and temperatures from 20 up to 200 °C. We revisit the well-established reliability of ratiometric measurements to accurately measure temperature. We find an almost perfect overlap of the experimental Boltzmann factor as a function of temperature for water, ethanol, and air–substrate environments, which is then used to retrieve the temperature of particles levitating in vacuum. We also explored the influence of the surrounding environment for increasing laser intensities by numerically and experimentally examining the balance among relevant emission bands. Our simulations qualitatively reproduce the experimentally measured luminescence in different environments, yielding a single model to simultaneously explain the laser intensity dependence of UV–NIR transitions for both the low and strong laser excitation regimes. Our findings hold great potential to expand the range of applicability of upconverting particles as dual sensors of temperature and laser intensity in different media relevant to biological and nanophotonic applications.

如今,上转换发光粒子已被常规用作精确可靠的探针,用于远程测量微小体积物质的温度,其量级为阿托立特(attoliters)。掺杂镧系元素的颗粒作为光学纳米温度计在生物系统中表现出良好的适应性,有助于了解细胞动力学、病理学和生理学。在此,我们研究了悬浮在真空中的掺铒/掺镱单颗粒的内在光学响应,并将其与嵌入应用相关干湿环境中的颗粒集合体的集体响应进行了比较。我们利用一个四极保罗陷阱(采用时变电场将掺铒/掺镱单粒子限制在真空中)和一个热浴模块来研究上述环境中的粒子。这两个子系统都使用双激发/检测装置,使我们能够记录发光光谱,激光强度覆盖 4 个数量级(例如,980 纳米波长 10-1-103 W/cm2),温度范围从 20 到 200 °C。我们重新审视了比率测量法在精确测量温度方面公认的可靠性。我们发现,在水、乙醇和空气-基底环境中,实验波尔兹曼因子与温度函数几乎完全重合,然后用它来检索真空中悬浮粒子的温度。我们还通过数值和实验研究了相关发射带之间的平衡,从而探索了周围环境对激光强度增加的影响。我们的模拟定性地再现了在不同环境中实验测量到的发光,产生了一个单一的模型,可以同时解释低激光激发和强激光激发下紫外-近红外跃迁的激光强度依赖性。我们的研究结果极有可能扩大上转换粒子的应用范围,使其成为生物和纳米光子应用相关的不同介质中温度和激光强度的双重传感器。
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引用次数: 0
Retina-Inspired Dual-Mode Photodetector with Spectral-Tunable Memory Switching for Neuromorphic Visual Systems
IF 6.5 1区 物理与天体物理 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-03-27 DOI: 10.1021/acsphotonics.5c0003610.1021/acsphotonics.5c00036
Chao Han, Jiayue Han, Lei Guo, Xingwei Han, Meiyu He, Yurong Zhang, Zhiming Wu, He Yu, Jun Gou and Jun Wang*, 

The development of multifunctional photodetectors that integrate sensing, storage, and computing to mimic the human visual system for efficient image processing is a key area of research. In particular, retina-inspired optoelectronic devices with multispectral information preprocessing capabilities are critical for constructing neuromorphic visual systems; however, achieving this in traditional photodetectors is challenging due to the lack of suitable photoresponse modes. Herein, a graphene/organic photodetector (GOP) with a spectral-tunable photoresponse memory mode switching feature is demonstrated. Benefiting from the unique photogenerated charge transfer and trapping behavior in the heterojunction, the device exhibits memory-free (with recovery times of a few milliseconds) and long-memory (with recovery times of several hundred seconds) photoresponse modes under long-wavelength (650–1064 nm) and short-wavelength (370–520 nm) light stimulation, respectively. Furthermore, the device supports spectral-tunable dual-mode switching between photosynaptic and photodetection under multiple light pulse stimulations, enabling real-time preprocessing of images with mixed green and red dual-wavelength information using a GOP-based 3 × 3-pixel image sensor. We also demonstrate a GOP-constructed neuromorphic visual system for efficient image processing, where the front-end GOP-based image sensor filters out background noise in the input images, significantly improving the image recognition accuracy of the back-end GOP-connected artificial neural network (from 40 to 93%).

开发集传感、存储和计算于一体的多功能光电探测器,模仿人类视觉系统进行高效图像处理,是一个关键的研究领域。特别是,具有多光谱信息预处理能力的视网膜启发光电器件对于构建神经形态视觉系统至关重要;然而,由于缺乏合适的光响应模式,在传统光电探测器中实现这一目标具有挑战性。本文展示了一种具有光谱可调光响应记忆模式切换功能的石墨烯/有机光电探测器(GOP)。受益于异质结中独特的光生电荷转移和捕获行为,该器件在长波长(650-1064 nm)和短波长(370-520 nm)光刺激下分别表现出无记忆(恢复时间为几毫秒)和长记忆(恢复时间为几百秒)光响应模式。此外,该器件还支持在多个光脉冲刺激下,在光突触和光检测之间进行光谱可调的双模式切换,从而能够使用基于 GOP 的 3 × 3 像素图像传感器,对包含绿色和红色混合双波长信息的图像进行实时预处理。我们还展示了一种用于高效图像处理的 GOP 构建的神经形态视觉系统,其中基于 GOP 的前端图像传感器可过滤掉输入图像中的背景噪声,从而显著提高后端 GOP 连接的人工神经网络的图像识别准确率(从 40% 提高到 93%)。
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引用次数: 0
Intrinsic Optical Response of Levitating Upconverting Single Particles
IF 7 1区 物理与天体物理 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-03-27 DOI: 10.1021/acsphotonics.4c02024
Laura Martinez Maestro, Miguel A. Antón, Eduardo Cabrera-Granado, Rosa Weigand, Javier Hernandez-Rueda
Today, upconverting luminescent particles are routinely used as accurate and reliable probes to remotely measure the temperature of minute volumes of matter on the order of attoliters. Lanthanide-doped particles exhibit adaptability as optical nanothermometers within biological systems, aiding the understanding of cellular dynamics, pathology, and physiology. Herein, we investigate the intrinsic optical response of Er/Yb-doped single particles levitating in a vacuum and compare it with the collective response of ensembles of particles embedded in application-relevant wet and dry environments. We make use of a quadrupole Paul trap that employs a time-varying electric field to confine single Er/Yb-doped particles in a vacuum and a thermal bath module to study particles in the above-mentioned environments. Both subsystems use twin-excitation/detection setups that allow us to record luminescence spectra, covering 4 orders of magnitude in laser intensity (e.g., 10–1–103 W/cm2 at 980 nm) and temperatures from 20 up to 200 °C. We revisit the well-established reliability of ratiometric measurements to accurately measure temperature. We find an almost perfect overlap of the experimental Boltzmann factor as a function of temperature for water, ethanol, and air–substrate environments, which is then used to retrieve the temperature of particles levitating in vacuum. We also explored the influence of the surrounding environment for increasing laser intensities by numerically and experimentally examining the balance among relevant emission bands. Our simulations qualitatively reproduce the experimentally measured luminescence in different environments, yielding a single model to simultaneously explain the laser intensity dependence of UV–NIR transitions for both the low and strong laser excitation regimes. Our findings hold great potential to expand the range of applicability of upconverting particles as dual sensors of temperature and laser intensity in different media relevant to biological and nanophotonic applications.
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引用次数: 0
Retina-Inspired Dual-Mode Photodetector with Spectral-Tunable Memory Switching for Neuromorphic Visual Systems
IF 7 1区 物理与天体物理 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-03-27 DOI: 10.1021/acsphotonics.5c00036
Chao Han, Jiayue Han, Lei Guo, Xingwei Han, Meiyu He, Yurong Zhang, Zhiming Wu, He Yu, Jun Gou, Jun Wang
The development of multifunctional photodetectors that integrate sensing, storage, and computing to mimic the human visual system for efficient image processing is a key area of research. In particular, retina-inspired optoelectronic devices with multispectral information preprocessing capabilities are critical for constructing neuromorphic visual systems; however, achieving this in traditional photodetectors is challenging due to the lack of suitable photoresponse modes. Herein, a graphene/organic photodetector (GOP) with a spectral-tunable photoresponse memory mode switching feature is demonstrated. Benefiting from the unique photogenerated charge transfer and trapping behavior in the heterojunction, the device exhibits memory-free (with recovery times of a few milliseconds) and long-memory (with recovery times of several hundred seconds) photoresponse modes under long-wavelength (650–1064 nm) and short-wavelength (370–520 nm) light stimulation, respectively. Furthermore, the device supports spectral-tunable dual-mode switching between photosynaptic and photodetection under multiple light pulse stimulations, enabling real-time preprocessing of images with mixed green and red dual-wavelength information using a GOP-based 3 × 3-pixel image sensor. We also demonstrate a GOP-constructed neuromorphic visual system for efficient image processing, where the front-end GOP-based image sensor filters out background noise in the input images, significantly improving the image recognition accuracy of the back-end GOP-connected artificial neural network (from 40 to 93%).
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引用次数: 0
Efficient Finite Element Modeling of Light Scattering in Symmetric Structures: A Nondegenerate Case
IF 6.5 1区 物理与天体物理 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-03-26 DOI: 10.1021/acsphotonics.4c0247410.1021/acsphotonics.4c02474
Jingwei Wang, Lida Liu, Yuhao Jing, Zhongfei Xiong*, Dominik Kowal and Yuntian Chen*, 

In recent years, advancements in optical scattering of nanostructures have significantly driven the development of telecommunications, medical imaging, detection, and novel light sources. However, due to the structural complexity of nanostructures, particularly metasurfaces and metamaterials, traditional methods of full-wave modeling for simulating optical scattering face substantial challenges due to increased degrees of freedom. In this work, we propose a symmetry-adapted finite element method to reduce the computational domain and enhance the efficiency of optical scattering simulations. By introducing the concepts of symmetry group and projection operator, we offer a formal and rigorous framework for decomposing the original problem, i.e., the incident condition, boundary constraints, and the finite element method implementation in decoupled subtasks. To demonstrate its broad applicability, we present three numerical examples: the enhancement of light confinement via quasi-bound states in the continuum in a photonic crystal slab, the scattering cross sections of incident configurations, and the calculation of transmission spectra in the metasurface. These examples illustrate the use of the symmetry finite element method under different symmetry conditions, including mirror symmetry, rotational symmetry, and the combination of Bloch’s theorem. Our method significantly reduces computation time and memory usage, thereby greatly improving the computational efficiency. Given the universality of symmetry principles, our method has important applications in the optical analysis and design of symmetric photonic devices, especially for symmetric yet large-sized optical structures.

近年来,纳米结构光散射的进步极大地推动了电信、医学成像、检测和新型光源的发展。然而,由于纳米结构(尤其是超表面和超材料)结构复杂,用于模拟光散射的传统全波建模方法因自由度增加而面临巨大挑战。在这项工作中,我们提出了一种对称适配有限元方法,以缩小计算域并提高光散射模拟的效率。通过引入对称组和投影算子的概念,我们提供了一个正式而严谨的框架来分解原始问题,即入射条件、边界约束和有限元方法实施中的解耦子任务。为了证明其广泛的适用性,我们介绍了三个数值示例:通过光子晶体板中连续体的准约束态增强光约束、入射配置的散射截面以及元表面的透射光谱计算。这些例子说明了对称有限元法在不同对称条件下的应用,包括镜像对称、旋转对称和布洛赫定理的组合。我们的方法大大减少了计算时间和内存用量,从而极大地提高了计算效率。鉴于对称原理的普遍性,我们的方法在对称光子器件的光学分析和设计中具有重要的应用价值,特别是对于对称但尺寸较大的光学结构。
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引用次数: 0
Efficient Finite Element Modeling of Light Scattering in Symmetric Structures: A Nondegenerate Case
IF 7 1区 物理与天体物理 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-03-26 DOI: 10.1021/acsphotonics.4c02474
Jingwei Wang, Lida Liu, Yuhao Jing, Zhongfei Xiong, Dominik Kowal, Yuntian Chen
In recent years, advancements in optical scattering of nanostructures have significantly driven the development of telecommunications, medical imaging, detection, and novel light sources. However, due to the structural complexity of nanostructures, particularly metasurfaces and metamaterials, traditional methods of full-wave modeling for simulating optical scattering face substantial challenges due to increased degrees of freedom. In this work, we propose a symmetry-adapted finite element method to reduce the computational domain and enhance the efficiency of optical scattering simulations. By introducing the concepts of symmetry group and projection operator, we offer a formal and rigorous framework for decomposing the original problem, i.e., the incident condition, boundary constraints, and the finite element method implementation in decoupled subtasks. To demonstrate its broad applicability, we present three numerical examples: the enhancement of light confinement via quasi-bound states in the continuum in a photonic crystal slab, the scattering cross sections of incident configurations, and the calculation of transmission spectra in the metasurface. These examples illustrate the use of the symmetry finite element method under different symmetry conditions, including mirror symmetry, rotational symmetry, and the combination of Bloch’s theorem. Our method significantly reduces computation time and memory usage, thereby greatly improving the computational efficiency. Given the universality of symmetry principles, our method has important applications in the optical analysis and design of symmetric photonic devices, especially for symmetric yet large-sized optical structures.
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引用次数: 0
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ACS Photonics
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