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Nonlinear optical colloidal metacrystals 非线性光学胶体元晶体
IF 35 1区 物理与天体物理 Q1 OPTICS Pub Date : 2024-10-31 DOI: 10.1038/s41566-024-01558-0
Ye Zhang, David D. Xu, Ibrahim Tanriover, Wenjie Zhou, Yuanwei Li, Rafael López-Arteaga, Koray Aydin, Chad A. Mirkin

Atomic and molecular structure inversion symmetry breaking in naturally occurring crystals dictate their physical properties including nonlinear optical (NLO) effects, piezo- or ferroelectricity, and non-reciprocal charge transport behaviour. With metamaterials composed of nanoscale building blocks (that is, meta-atoms), the spatial inversion symmetry violation on planar surfaces leads to spin-controlled photonics as well as NLO metasurfaces. Synthetically, low-symmetry 3D metacrystals can be synthesized, but NLO behaviour has not been identified so far (for example, harmonic generations). Herein we show how DNA-mediated assembly of octahedron-shaped plasmonic gold nanocrystals can be used to design and deliberately synthesize non-centrosymmetric and centrosymmetric colloidal crystals. Importantly, while the centrosymmetric structures do not exhibit substantial second-harmonic generation, the non-centrosymmetric crystals do—a consequence of the asymmetric distribution of localized electric fields in plasmonic hotspots. Moreover, this non-centrosymmetric NLO metacrystal represents a 3D NLO metamaterial being developed via a bottom-up approach, exhibiting a maximum second-harmonic generation conversion efficiency of 10−9 to surpass the efficiencies observed in the majority of plasmonic 2D metasurfaces. Finally, the DNA-loading density on the particle building blocks can be used to toggle between the centrosymmetric and non-centrosymmetric phases.

天然晶体中的原子和分子结构反转对称性破坏决定了它们的物理特性,包括非线性光学(NLO)效应、压电性或铁电性以及非互易电荷传输行为。对于由纳米级构件(即元原子)组成的超材料,平面上的空间反转对称性违反会导致自旋控制光子学和 NLO 超表面。低对称性三维元晶体可以合成,但至今尚未发现 NLO 行为(例如谐波发生)。在此,我们展示了如何利用 DNA 介导的八面体形质子金纳米晶体组装来设计和有意合成非中心对称和中心对称胶体晶体。重要的是,虽然中心对称结构不会产生大量二次谐波,但非中心对称晶体却能产生二次谐波--这是等离子热点局部电场分布不对称的结果。此外,这种非中心对称 NLO 超晶体代表了一种通过自下而上方法开发的三维 NLO 超材料,其最大二次谐波发生转换效率为 10-9,超过了在大多数等离子体二维超表面中观察到的效率。最后,粒子构件上的 DNA 负载密度可用于在中心对称和非中心对称相之间切换。
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引用次数: 0
Light–matter interactions driven by lasers at highest intensities 最高强度激光驱动的光物质相互作用
IF 32.3 1区 物理与天体物理 Q1 OPTICS Pub Date : 2024-10-31 DOI: 10.1038/s41566-024-01554-4
Stepan Bulanov
The interaction of electrons and photons lies at the very foundation of quantum electrodynamics. However, if an electron is able to scatter off several hundred photons, provided by a high-power laser, new physical phenomena come into play. This might pave a way for future light sources and photon–photon colliders.
电子与光子的相互作用是量子电动力学的基础。然而,如果一个电子能够散射由高功率激光器提供的几百个光子,新的物理现象就会出现。这可能会为未来的光源和光子-光子对撞机铺平道路。
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引用次数: 0
Twisted topological light illuminates molecular chirality 扭曲拓扑光照亮分子手性
IF 32.3 1区 物理与天体物理 Q1 OPTICS Pub Date : 2024-10-31 DOI: 10.1038/s41566-024-01553-5
Daria Smirnova, Alexander B. Khanikaev
A nonlinear optical response to a new form of light, dubbed chiral topological light owing to its local chirality and global topological characteristics, is enabling unprecedented enantiosensitivity and robustness of chiro-optical spectroscopies as a result of structured light–matter interactions at deep subwavelength scales.
由于其局部手性和全局拓扑特性,一种被称为手性拓扑光的新型光的非线性光学响应,在深亚波长尺度的结构化光-物质相互作用下,实现了前所未有的对映灵敏度和坚固耐用的气光学光谱。
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引用次数: 0
Photon-trapping detector 光子捕获探测器
IF 32.3 1区 物理与天体物理 Q1 OPTICS Pub Date : 2024-10-31 DOI: 10.1038/s41566-024-01560-6
Noriaki Horiuchi
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引用次数: 0
Fundamental scaling laws of water-window X-rays from free-electron-driven van der Waals structures 自由电子驱动范德瓦耳斯结构的水窗 X 射线基本缩放定律
IF 32.3 1区 物理与天体物理 Q1 OPTICS Pub Date : 2024-10-28 DOI: 10.1038/s41566-024-01547-3
Nikhil Pramanik, Sunchao Huang, Ruihuan Duan, Qingwei Zhai, Michael Go, Chris Boothroyd, Zheng Liu, Liang Jie Wong
Water-window X-rays are crucial in medical and biological applications, enabling the natural-contrast imaging of biological cells without external staining. However, water-window X-ray sources with bespoke photon energies—needed in high-contrast imaging—remain challenging to obtain, except at large synchrotron facilities. Here we address this challenge by demonstrating tabletop, water-window X-ray generation from free-electron-driven van der Waals materials, enabling the continuous tuning of photon energies across the entire water-window regime. Additionally, we present a truly predictive theoretical framework combining first-principles electromagnetism with Monte Carlo simulations to accurately predict the photon flux and brightness in absolute quantities. We obtain fundamental scaling laws for the tunable photon flux, matching the experimental results and providing a way to design powerful emitters based on free-electron-driven quantum materials. We show that we can potentially achieve photon fluxes needed for imaging and spectroscopy applications (over 108 photons s–1 on the sample—verified by our framework based on our experimentally achieved fluxes of about 103 photons s–1 using ~50 nA current). Importantly, our theory highlights the critical role played by the large mean free paths and interlayer atomic spacings unique to van der Waals structures, showing the latter’s advantages over other materials in generating water-window X-rays. Tabletop, water-window X-rays are generated using free-electron-driven van der Waals materials. The X-ray energy from the source can be tuned across the water window, and the established fundamental scaling laws for the tunable photon flux may enable the design of powerful emitters based on free-electron-driven quantum materials.
水窗 X 射线在医疗和生物应用中至关重要,它可以在不进行外部染色的情况下对生物细胞进行自然对比成像。然而,除了大型同步加速器设施外,要获得高对比度成像所需的定制光子能量的水窗 X 射线源仍然很困难。为了应对这一挑战,我们在这里展示了由自由电子驱动的范德瓦耳斯材料产生的台式水窗 X 射线,从而实现了在整个水窗系统中对光子能量的持续调整。此外,我们还提出了一个真正具有预测性的理论框架,将第一原理电磁学与蒙特卡罗模拟相结合,以准确预测光子通量和亮度的绝对量。我们获得了可调光子通量的基本缩放定律,与实验结果相吻合,为设计基于自由电子驱动量子材料的强大发射器提供了方法。我们的研究表明,我们有可能实现成像和光谱学应用所需的光子通量(在样品上超过 108 光子 s-1--我们的框架根据使用 ~50 nA 电流实现的约 103 光子 s-1 的实验通量进行了验证)。重要的是,我们的理论强调了范德华结构特有的大平均自由路径和层间原子间距所发挥的关键作用,显示了后者在产生水窗 X 射线方面优于其他材料的优势。
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引用次数: 0
Advances in inverted perovskite solar cells 倒置型过氧化物太阳能电池的进展
IF 35 1区 物理与天体物理 Q1 OPTICS Pub Date : 2024-10-28 DOI: 10.1038/s41566-024-01541-9
Xin Zhang, Shengfan Wu, Hong Zhang, Alex K. Y. Jen, Yiqiang Zhan, Junhao Chu

Considerable efforts are being made to advance inverted (p–i–n) perovskite solar cells (PSCs). Several passivation and insulation strategies have effectively been applied to reduce non-radiative recombination, a notorious issue for PSCs. Consequently, the performance of inverted PSCs has begun to rival those of regular (n–i–p) PSCs, with power conversion efficiency (PCE) values above 26%. The efficiency of tandem solar cells containing an inverted PSC as a subcell has also grown rapidly, reaching >33%. This Review discusses the origin of non-radiative recombinations in PSCs and recent progress in reducing them. We review how innovative device configurations, perovskite composition and interfacial engineering contribute to the high efficiency and long-term operational stability of inverted PSCs. We aim to provide readers with important insights into materials chemistry, physical processing and device configurations to further improve perovskite-based photovoltaics.

目前正在大力推进反向(p-i-n)包晶石太阳能电池(PSCs)的发展。一些钝化和绝缘策略已得到有效应用,以减少非辐射重组,这是 PSCs 的一个臭名昭著的问题。因此,倒置型 PSC 的性能已开始与普通(n-i-p)PSC 相媲美,功率转换效率(PCE)值超过 26%。含有倒置 PSC 子电池的串联太阳能电池的效率也迅速提高,达到了 33%。本综述讨论了 PSC 中非辐射重组的起源以及在减少非辐射重组方面的最新进展。我们回顾了创新的器件配置、包晶石成分和界面工程如何有助于提高倒置式 PSCs 的效率和长期运行稳定性。我们旨在为读者提供有关材料化学、物理加工和器件配置的重要见解,以进一步改进基于包晶石的光伏技术。
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引用次数: 0
Integrated non-reciprocal magneto-optics with ultra-high endurance for photonic in-memory computing 用于光子内存计算的具有超高耐用性的集成非互易磁光学器件
IF 35 1区 物理与天体物理 Q1 OPTICS Pub Date : 2024-10-23 DOI: 10.1038/s41566-024-01549-1
Paolo Pintus, Mario Dumont, Vivswan Shah, Toshiya Murai, Yuya Shoji, Duanni Huang, Galan Moody, John E. Bowers, Nathan Youngblood

Processing information in the optical domain promises advantages in both speed and energy efficiency over existing digital hardware for a variety of emerging applications in artificial intelligence and machine learning. A typical approach to photonic processing is to multiply a rapidly changing optical input vector with a matrix of fixed optical weights. However, encoding these weights on-chip using an array of photonic memory cells is currently limited by a wide range of material- and device-level issues, such as the programming speed, extinction ratio and endurance, among others. Here we propose a new approach to encoding optical weights for in-memory photonic computing using magneto-optic memory cells comprising heterogeneously integrated cerium-substituted yttrium iron garnet (Ce:YIG) on silicon micro-ring resonators. We show that leveraging the non-reciprocal phase shift in such magneto-optic materials offers several key advantages over existing architectures, providing a fast (1 ns), efficient (143 fJ per bit) and robust (2.4 billion programming cycles) platform for on-chip optical processing.

对于人工智能和机器学习领域的各种新兴应用而言,与现有数字硬件相比,光域信息处理在速度和能效方面都具有优势。光子处理的典型方法是将快速变化的光输入向量与固定光权重矩阵相乘。然而,使用光子存储单元阵列在芯片上对这些权重进行编码,目前受到材料和设备层面的各种问题的限制,如编程速度、消光比和耐用性等。在这里,我们提出了一种为内存光子计算进行光权重编码的新方法,即在硅微环谐振器上使用由异质集成的铈取代钇铁石榴石(Ce:YIG)组成的磁光存储单元。我们的研究表明,与现有架构相比,利用这种磁光材料的非互易相移提供了几个关键优势,为片上光学处理提供了一个快速(1 ns)、高效(每比特 143 fJ)和稳健(24 亿编程周期)的平台。
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引用次数: 0
Near-petahertz fieldoscopy of liquid 液体的近派赫兹场镜检查
IF 35 1区 物理与天体物理 Q1 OPTICS Pub Date : 2024-10-21 DOI: 10.1038/s41566-024-01548-2
Anchit Srivastava, Andreas Herbst, Mahdi M. Bidhendi, Max Kieker, Francesco Tani, Hanieh Fattahi

Measuring transient optical fields is pivotal not only for understanding ultrafast phenomena but also for the quantitative detection of various molecular species in a sample. Here we demonstrate near-petahertz electric field detection of a few femtosecond pulses with 200 attosecond temporal resolution and subfemtojoule detection sensitivity. By field-resolved detection of the impulsively excited molecules in the liquid phase, termed femtosecond fieldoscopy, we demonstrate temporal isolation of the response of the target molecules from those of the environment and the excitation pulse. In a proof-of-concept analysis of aqueous and liquid samples, we demonstrate field-sensitive detection of combination bands of 4.13 μmol ethanol for the first time. This method expands the scope of aqueous sample analysis to higher detection sensitivity and dynamic range, while the simultaneous direct measurements of phase and intensity information pave the path towards high-resolution biological spectro-microscopy.

测量瞬态光场不仅对理解超快现象至关重要,而且对定量检测样品中的各种分子物种也至关重要。在这里,我们展示了对几个飞秒脉冲的近太赫兹电场检测,其时间分辨率为 200 阿秒,检测灵敏度为亚飞秒焦耳。通过对液相中脉冲激发的分子进行场分辨检测(称为飞秒场镜),我们展示了目标分子的响应与环境和激发脉冲的响应之间的时间隔离。在对水和液体样品的概念验证分析中,我们首次展示了对 4.13 μmol 乙醇组合带的场敏检测。这种方法扩大了水样分析的范围,提高了检测灵敏度和动态范围,同时直接测量相位和强度信息,为实现高分辨率生物光谱显微镜铺平了道路。
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引用次数: 0
Semiconductor thermoradiative power conversion 半导体热辐射功率转换
IF 32.3 1区 物理与天体物理 Q1 OPTICS Pub Date : 2024-10-21 DOI: 10.1038/s41566-024-01537-5
Michael P. Nielsen, Andreas Pusch, Phoebe M. Pearce, Muhammad H. Sazzad, Peter J. Reece, Martin A. Green, Nicholas J. Ekins-Daukes
Power can be generated from radiative exchange between two bodies with different temperatures—from the radiative cooling of the Earth’s surface into space, for example. Thermoradiative diodes are low-bandgap optoelectronic devices in which the occupancies of the valence and conduction bands are established through radiative exchange with the external environment. A warm diode viewing cold surroundings will spontaneously develop a reverse electrical bias, which, combined with the recombination current from the radiative imbalance, generates electrical power. Here we review the operating principles of the thermoradiative diode in both the radiative limit and in the presence of non-radiative processes. We discuss some present limitations and opportunities for improved performance together with potential applications such as night-sky power generation and waste-heat recovery. This article reviews the concept of using thermoradiative diodes for power conversion, and discusses potential applications such as night-sky power generation and waste-heat recovery.
两个不同温度的物体之间的辐射交换--例如地球表面向太空的辐射冷却--可以产生能量。热辐射二极管是一种低带隙光电器件,其中价带和导带的占位是通过与外部环境的辐射交换来确定的。热二极管在观察冷环境时会自发产生反向电偏压,再加上辐射不平衡产生的重组电流,从而产生电能。在此,我们回顾了热辐射二极管在辐射极限和非辐射过程中的工作原理。我们讨论了目前的一些局限性和改进性能的机会,以及夜空发电和废热回收等潜在应用。
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引用次数: 0
Image-guided computational holographic wavefront shaping 图像引导的计算全息波前整形
IF 35 1区 物理与天体物理 Q1 OPTICS Pub Date : 2024-10-18 DOI: 10.1038/s41566-024-01544-6
Omri Haim, Jeremy Boger-Lombard, Ori Katz

Optical imaging through scattering media is important in a variety of fields ranging from microscopy to autonomous vehicles. Although advanced wavefront shaping techniques have offered several breakthroughs in the past decade, current techniques still require a known guide star and a high-resolution spatial light modulator or a very large number of measurements and are limited in their correction field of view. Here we introduce a guide-star-free, non-invasive approach that can correct more than 190,000 scattered modes using only 25 incoherently compounded, holographically measured, scattered light fields, obtained under unknown random illuminations. This is achieved by computationally emulating an image-guided wavefront shaping experiment, where several virtual spatial light modulators are simultaneously optimized to maximize the reconstructed image quality. Our method shifts the burden from the physical hardware to a digital, naturally parallelizable computational optimization, leveraging state-of-the-art automatic differentiation tools. We demonstrate the flexibility and generality of this framework by applying it to imaging through various complex samples and imaging modalities, including epi-illumination, anisoplanatic multi-conjugate correction of highly scattering layers, lensless endoscopy in multicore fibres and acousto-optic tomography. The presented approach offers high versatility, effectiveness and generality for fast, non-invasive imaging in diverse applications.

通过散射介质进行光学成像在从显微镜到自动驾驶汽车等多个领域都非常重要。尽管先进的波前整形技术在过去十年中取得了一些突破,但目前的技术仍然需要已知的导星和高分辨率空间光调制器或大量的测量,而且校正视野有限。在这里,我们介绍一种无需导星的非侵入式方法,只需使用 25 个非相干复合、全息测量的散射光场,就能校正 190,000 多种散射模式,这些散射光场是在未知的随机光照下获得的。这是通过计算模拟图像引导的波前整形实验实现的,在该实验中,多个虚拟空间光调制器同时进行优化,以最大限度地提高重建图像的质量。我们的方法利用最先进的自动微分工具,将物理硬件的负担转移到数字化、自然可并行的计算优化上。我们将这一框架应用于各种复杂样本和成像模式的成像,包括外延照明、高散射层的异平面多共轭校正、多芯光纤中的无镜头内窥镜和声光层析成像,从而展示了这一框架的灵活性和通用性。所提出的方法具有很高的通用性、有效性和通用性,可在各种应用中实现快速、无创成像。
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引用次数: 0
期刊
Nature Photonics
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