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    Vol. 6 , Issue 4 , 2017

      Original Articles

    • Tong Yang,Guo-Fan Jin,Jun Zhu
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.81
      Abstract:The automated design of imaging systems involving no or minimal human effort has always been the expectation of scientists, researchers and optical engineers. In addition, it is challenging to choose an appropriate starting point for an optical system design. In this paper, we present a novel design framework based on a point-by-point design process that can automatically obtain high-performance freeform systems. This framework only requires a combination of planes as the input based on the configuration requirements or the prior knowledge of designers. This point-by-point design framework is different from the decades-long tradition of optimizing surface coefficients. Compared with the traditional design method, whereby the selection of the starting point and the optimization process are independent of each other and require extensive amount of human effort, there are no obvious differences between these two processes in our design framework, and the entire design process is mostly automated. This automated design process significantly reduces the amount of human effort required and does not rely on advanced design skills and experience. To demonstrate the feasibility of the proposed design framework, we successfully designed two high-performance systems as examples. This point-by-point design framework opens up new possibilities for automated optical design and can be used to develop automated optical design in the areas of remote sensing, telescopy, microscopy, spectroscopy, virtual reality and augmented reality.  
      Keywords:automated design;construction and iteration;freeform imaging system;point-by-point   
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      Published:2024-09-18
    • Wenxuan Liang,Gunnsteinn Hall,Bernhard Messerschmidt,Ming-Jun Li,Xingde Li
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.82
      Abstract:This manuscript reports on the first two-photon, label-free, metabolic imaging of biological tissues in vivo at histological resolution on an extremely compact, fiber-optic endomicroscopy platform. This system provides new opportunities for performing non-invasive and functional histological imaging of internal organs in vivo, in situ and in real time. As a routine clinical procedure, traditional histology has made significant impacts on medicine. However, the procedure is invasive and time consuming, suffers random sampling errors, and cannot provide in vivo functional information. The technology reported here features an extremely compact and flexible fiber-optic probe ~2 mm in diameter, enabling direct access to internal organs. Unprecedented two-photon imaging quality comparable to a large bench-top laser scanning microscope was achieved through technological innovations in double-clad fiber optics and miniature objective lenses (among many others). In addition to real-time label-free visualization of biological tissues in situ with subcellular histological detail, we demonstrated for the first time in vivo two-photon endomicroscopic metabolic imaging on a functioning mouse kidney model. Such breakthroughs in nonlinear endoscopic imaging capability present numerous promising opportunities for paradigm-shifting applications in both clinical diagnosis and basic research.  
      Keywords:functional histology in vivo;label-free imaging;nonlinear endomicroscopy;two-photon metabolic imaging   
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      Published:2024-09-18
    • Lei Wang,Qi-Dai Chen,Xiao-Wen Cao,Ričardas Buividas,Xuewen Wang,Saulius Juodkazis,Hong-Bo Sun
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.112
      Abstract:The lossy nature of plasmonic wave due to absorption is shown to become an advantage for scaling-up a large area surface nanotexturing of transparent dielectrics and semiconductors by a self-organized sub-wavelength energy deposition leading to an ablation pattern—ripples—using this plasmonic nano-printing. Irreversible nanoscale modifications are delivered by surface plasmon polariton (SPP) using: (ⅰ) fast scan and (ⅱ) cylindrical focusing of femtosecond laser pulses for a high patterning throughput. The mechanism of ripple formation on ZnS dielectric is experimentally proven to occur via surface wave at the substrate–plasma interface. The line focusing increase the ordering quality of ripples and facilitates fabrication over wafer-sized areas within a practical time span. Nanoprinting using SPP is expected to open new applications in photo-catalysis, tribology, and solar light harvesting via localized energy deposition rather scattering used in photonic and sensing applications based on re-scattering of SPP modes into far-field modes.  
      Keywords:deep-subwavelength structures;laser induced periodic structures;large-area fabrication;plasmonic;subwavelength structures   
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      Published:2024-09-18
    • Fuxing Gu,Fuming Xie,Xing Lin,Shuangyi Linghu,Wei Fang,Heping Zeng,Limin Tong,Songlin Zhuang
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.61
      Abstract:Single-mode lasing in whispering-gallery mode (WGM) microresonators is challenging to achieve. In bottle microresonators, the highly non-degenerated WGMs are spatially well-separated along the long-axis direction and provide mode-selection capability. In this work, by engineering the pump intensity to modify the spatial gain profiles of bottle microresonators, we demonstrate a simple and general approach to realizing single-mode WGM lasing in polymer bottle microresonators. The pump intensity is engineered into an interference distribution on the bottle microresonator surface. By tuning the spacing between axial positions of the interference pump patterns, the mode intensity profiles of single-bottle WGMs can be spatially overlapped with the interference stripes, intrinsically enabling single-mode lasing and selection. Attractive advantages of the system, including high side-mode suppression factors > 20 dB, large spectral tunability > 8 nm, low-lasing threshold and reversible control, are presented. Our demonstrated approach may have a variety of promising applications, ranging from tunable single-mode lasing and sensing to nonlinear optics.  
      Keywords:bottle microresonators;polymer;single-mode lasing;spatial pump engineering;whispering-gallery modes   
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      Published:2024-09-18
    • Ze-Bo Zheng,Jun-Tao Li,Teng Ma,Han-Lin Fang,Wen-Cai Ren,Jun Chen,Jun-Cong She,Yu Zhang,Fei Liu,Huan-Jun Chen,Shao-Zhi Deng,Ning-Sheng Xu
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.57
      Abstract:Graphene has great potential for enhancing light−matter interactions in a two-dimensional regime due to surface plasmons with low loss and strong light confinement. Further utilization of graphene in nanophotonics relies on the precise control of light localization properties. Here, we demonstrate the tailoring of electromagnetic field localizations in the mid-infrared region by precisely shaping the graphene into nanostructures with different geometries. We generalize the phenomenological cavity model and employ nanoimaging techniques to quantitatively calculate and experimentally visualize the two-dimensional electromagnetic field distributions within the nanostructures, which indicate that the electromagnetic field can be shaped into specific patterns depending on the shapes and sizes of the nanostructures. Furthermore, we show that the light localization performance can be further improved by reducing the sizes of the nanostructures, where a lateral confinement of λ0/180 of the incidence light can be achieved. The electromagnetic field localizations within a nanostructure with a specific geometry can also be modulated by chemical doping. Our strategies can, in principle, be generalized to other two-dimensional materials, therefore providing new degrees of freedom for designing nanophotonic components capable of tailoring two-dimensional light confinement over a broad wavelength range.  
      Keywords:chemical doping;electromagnetic field localizations;graphene;graphene nanostructures;graphene plasmons   
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      Published:2024-09-18
    • Diana Serrano,Stefan Seeger
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.66
      Abstract:Raman scattering microscopy is a versatile tool for label-free imaging and molecular fingerprint analysis. Here, we provide the first demonstration that the selective collection of scattered signals exceeding the critical angle for total internal reflection enables surface-confined spontaneous Raman investigations at nanometre resolution. This high-axial selectivity leads to improved signal-to-background ratios, thus making this technique an excellent probe for surface-related molecular specimens. The richness of the spectroscopic information obtained through the supercritical angle Raman (SAR) collection path was proven by comparing its output with that of a parallel far-field collection path. Furthermore, we demonstrated that the proposed SAR technique is a versatile microscopy approach that can be used alone or in combination with amplified Raman modalities such as surface-enhanced resonance Raman scattering.  
      Keywords:near-field optics;Raman scattering;supercritical microscopy;surface science   
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      Published:2024-09-18
    • Luca Masini,Alessandro Pitanti,Lorenzo Baldacci,Miriam S Vitiello,Riccardo Degl'Innocenti,Harvey E Beere,David A Ritchie,Alessandro Tredicucci
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.54
      Abstract:Resonators and the way they couple to external radiation rely on very different concepts if one considers devices belonging to the photonic and electronic worlds. The terahertz frequency range, however, provides intriguing possibilities for the development of hybrid technologies that merge ideas from both fields in novel functional designs. In this paper, we show that high-quality, subwavelength, whispering-gallery lasers can be combined to form a linear dipole antenna, which creates a very efficient, low-threshold laser emission in a collimated beam pattern. For this purpose, we employ a terahertz quantum-cascade active region patterned into two 19-μm-radius microdisks coupled by a suspended metallic bridge, which simultaneously acts as an inductive antenna and produces the dipole symmetry of the lasing mode. Continuous-wave vertical emission is demonstrated at approximately 3.5 THz in a very regular, low-divergence (±10°) beam, with a high slope efficiency of at least 160 mW A−1 and a mere 6 mA of threshold current, which is ensured by the ultra-small resonator size (VRES/λ3≈10−2). The extremely low power consumption and the superior beam brightness make this concept very promising for the development of miniaturized and portable THz sources to be used in the field for imaging and sensing applications as well as for exploring novel optomechanical intracavity effects.  
      Keywords:microresonators;optical antennas;quantum cascade laser;terahertz;whispering-gallery   
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      Published:2024-09-18
    • Haitao Chen,Vincent Corboliou,Alexander S Solntsev,Duk-Yong Choi,Maria A Vincenti,Domenico de Ceglia,Costantino de Angelis,Yuerui Lu,Dragomir N Neshev
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.60
      Abstract:Two-dimensional transition-metal dichalcogenides (TMDCs) with intrinsically broken crystal inversion symmetry and large second-order nonlinear responses have shown great promise for future nonlinear light sources. However, the sub-nanometer monolayer thickness of such materials limits the length of their nonlinear interaction with light. Here, we experimentally demonstrate the enhancement of the second-harmonic generation from monolayer MoSe2 by its integration onto a 220-nm-thick silicon waveguide. Such on-chip integration allows for a marked increase in the interaction length between the MoSe2 and the waveguide mode, further enabling phase matching of the nonlinear process. The demonstrated TMDC–silicon photonic hybrid integration opens the door to second-order nonlinear effects within the silicon photonic platform, including efficient frequency conversion, parametric amplification and the generation of entangled photon pairs.  
      Keywords:2D material;MoSe2;SHG;waveguide   
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      Published:2024-09-18
    • Martina Barbiero,Stefania Castelletto,Xiaosong Gan,Min Gu
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.85
      Abstract:Due to their exceptional optical and magnetic properties, negatively charged nitrogen-vacancy (NV−) centers in nanodiamonds (NDs) have been identified as an indispensable tool for imaging, sensing and quantum bit manipulation. The investigation of the emission behaviors of single NV− centers at the nanoscale is of paramount importance and underpins their use in applications ranging from quantum computation to super-resolution imaging. Here, we report on a spin-manipulated nanoscopy method for nanoscale resolutions of the collectively blinking NV− centers confined within the diffraction-limited region. Using wide-field localization microscopy combined with nanoscale spin manipulation and the assistance of a microwave source tuned to the optically detected magnetic resonance (ODMR) frequency, we discovered that two collectively blinking NV− centers can be resolved. Furthermore, when the collective emitters possess the same ground state spin transition frequency, the proposed method allows the resolving of each single NV− center via an external magnetic field used to split the resonant dips. In spin manipulation, the three-level blinking dynamics provide the means to resolve two NV− centers separated by distances of 23 nm. The method presented here offers a new platform for studying and imaging spin-related quantum interactions at the nanoscale with super-resolution techniques.  
      Keywords:nanodiamonds;nanoscale microscopy;nitrogen-vacancy color centers;optically detected magnetic resonance   
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      Published:2024-09-18
    • Andreas Döpp,Benoit Mahieu,Agustin Lifschitz,Cedric Thaury,Antoine Doche,Emilien Guillaume,Gabriele Grittani,Olle Lundh,Martin Hansson,Julien Gautier,Michaela Kozlova,Jean Philippe Goddet,Pascal Rousseau,Amar Tafzi,Victor Malka,Antoine Rousse,Sebastien Corde,Kim Ta Phuoc
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.86
      Abstract:Technology based on high-peak-power lasers has the potential to provide compact and intense radiation sources for a wide range of innovative applications. In particular, electrons that are accelerated in the wakefield of an intense laser pulse oscillate around the propagation axis and emit X-rays. This betatron source, which essentially reproduces the principle of a synchrotron at the millimeter scale, provides bright radiation with femtosecond duration and high spatial coherence. However, despite its unique features, the usability of the betatron source has been constrained by its poor control and stability. In this article, we demonstrate the reliable production of X-ray beams with tunable polarization. Using ionization-induced injection in a gas mixture, the orbits of the relativistic electrons emitting the radiation are reproducible and controlled. We observe that both the signal and beam profile fluctuations are significantly reduced and that the beam pointing varies by less than a tenth of the beam divergence. The polarization ratio reaches 80%, and the polarization axis can easily be rotated. We anticipate a broad impact of the source, as its unprecedented performance opens the way for new applications.  
      Keywords:laser-plasma interaction;laser-wakefield acceleration;synchrotron light sources   
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      Published:2024-09-18
    • Fei Guo,Andre Karl,Qi-Fan Xue,Kai Cheong Tam,Karen Forberich,Christoph J Brabec
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.94
      Abstract:Electroluminescent devices based on organic semiconductors have attracted significant attention owing to their promising applications in flat-panel displays. The conventional display pixel consisting of side-by-side arrayed red, green and blue subpixels represents the mature technology but bears an intrinsic deficiency of a low pixel density. Constructing an individual color-tunable pixel that comprises vertically stacked subpixels is considered an advanced technology. Although color-tunable organic light-emitting diodes (OLEDs) have been fabricated using the vacuum deposition of small molecules, the solution processing of conjugated polymers would enable a much simpler and inexpensive manufacturing process. Here we present the all-solution processing of color-tunable OLEDs comprising two vertically stacked polymer emitters. A thin layer of highly conducting and transparent silver nanowires is introduced as the intermediate charge injection contact, which allows the emission spectrum and intensity of the tandem devices to be seamlessly manipulated. To demonstrate a viable application of this technology, a 4-by-4 pixelated matrix color-tunable display was fabricated.  
      Keywords:color tunable;OLED display;organic light-emitting diode;silver nanowires;solution processing;tandem   
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      Published:2024-09-18
    • Hadas Frostig,Tim Bayer,Yonina C Eldar,Yaron Silberberg
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.115
      Abstract:Two-dimensional (2D) spectroscopy is used to study the interactions between energy levels in both the field of optics and nuclear magnetic resonance (NMR). Conventionally, the strength of interaction between two levels is inferred from the value of their common off-diagonal peak in the 2D spectrum, which is termed the cross peak. However, stronger diagonal peaks often have long tails that extend into the locations of the cross peaks and alter their values. Here, we introduce a method for retrieving the true interaction strengths by using sparse signal recovery techniques and apply our method in 2D Raman spectroscopy experiments.  
      Keywords:multidimensional spectroscopy;nonlinear optics;sparsity-based algorithms   
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      Published:2024-09-18
    • Evan P Perillo,Jeremy W Jarrett,Yen-Liang Liu,Ahmed Hassan,Daniel C Fernée,John R Goldak,Andrei Bonteanu,David J Spence,Hsin-Chih Yeh,Andrew K Dunn
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.95
      Abstract:Two-color multiphoton microscopy through wavelength mixing of synchronized lasers has been shown to increase the spectral window of excitable fluorophores without the need for wavelength tuning. However, most currently available dual output laser sources rely on the costly and complicated optical parametric generation approach. In this report, we detail a relatively simple and low cost diamond Raman laser pumped by a ytterbium fiber amplifier emitting at 1055 nm, which generates a first Stokes emission centered at 1240 nm with a pulse width of 100 fs. The two excitation wavelengths of 1055 and 1240 nm, along with the effective two-color excitation wavelength of 1140 nm, provide an almost complete coverage of fluorophores excitable within the range of 1000–1300 nm. When compared with 1055 nm excitation, two-color excitation at 1140 nm offers a 90% increase in signal for many far-red emitting fluorescent proteins (for example, tdKatushka2). We demonstrate multicolor imaging of tdKatushka2 and Hoechst 33342 via simultaneous two-color two-photon, and two-color three-photon microscopy in engineered 3D multicellular spheroids. We further discuss potential benefits and applications for two-color three-photon excitation. In addition, we show that this laser system is capable of in vivo imaging in mouse cortex to nearly 1 mm in depth with two-color excitation.  
      Keywords:microscopy;nonlinear processes;three-dimensional imaging;ultrafast lasers   
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      Published:2024-09-18
    • Song Jiang,Xianbiao Zhang,Yao Zhang,Chunrui Hu,Rui Zhang,Yang Zhang,Yuan Liao,Zachary J Smith,Zhenchao Dong,J G Hou
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.98
      Abstract:Tip-enhanced Raman spectroscopy (TERS) is a powerful surface analysis technique that can provide subnanometer-resolved images of nanostructures with site-specific chemical fingerprints. However, due to the limitation of weak Raman signals and the resultant difficulty in achieving TERS imaging with good signal-to-noise ratios (SNRs), the conventional single-peak analysis is unsuitable for distinguishing complex molecular architectures at the subnanometer scale. Here we demonstrate that the combination of subnanometer-resolved TERS imaging and advanced multivariate analysis can provide an unbiased panoramic view of the chemical identity and spatial distribution of different molecules on surfaces, yielding high-quality chemical images despite limited SNRs in individual pixel-level spectra. This methodology allows us to exploit the full power of TERS imaging and unambiguously distinguish between adjacent molecules with a resolution of ~0.4 nm, as well as to resolve submolecular features and the differences in molecular adsorption configurations. Our results provide a promising methodology that promotes TERS imaging as a routine analytical technique for the analysis of complex nanostructures on surfaces.  
      Keywords:chemical imaging;hyperspectral imaging;multivariate analysis;nanoimaging;tip-enhanced Raman spectroscopy   
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      Published:2024-09-18
    • Rudrakant Sollapur,Daniil Kartashov,Michael Zürch,Andreas Hoffmann,Teodora Grigorova,Gregor Sauer,Alexander Hartung,Anka Schwuchow,Joerg Bierlich,Jens Kobelke,Mario Chemnitz,A Schmidt Markus,Christian Spielmann
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.124
      Abstract:Ultrafast supercontinuum generation in gas-filled waveguides is an enabling technology for many intriguing applications ranging from attosecond metrology towards biophotonics, with the amount of spectral broadening crucially depending on the pulse dispersion of the propagating mode. In this study, we show that structural resonances in a gas-filled antiresonant hollow core optical fiber provide an additional degree of freedom in dispersion engineering, which enables the generation of more than three octaves of broadband light that ranges from deep UV wavelengths to near infrared. Our observation relies on the introduction of a geometric-induced resonance in the spectral vicinity of the ultrafast pump laser, outperforming gas dispersion and yielding a unique dispersion profile independent of core size, which is highly relevant for scaling input powers. Using a krypton-filled fiber, we observe spectral broadening from 200 nm to 1.7 μm at an output energy of ~ 23 μJ within a single optical mode across the entire spectral bandwidth. Simulations show that the frequency generation results from an accelerated fission process of soliton-like waveforms in a non-adiabatic dispersion regime associated with the emission of multiple phase-matched Cherenkov radiations on both sides of the resonance. This effect, along with the dispersion tuning and scaling capabilities of the fiber geometry, enables coherent ultra-broadband and high-energy sources, which range from the UV to the mid‐infrared spectral range.  
      Keywords:antiresonant hollow core fiber;dispersion design;nonlinear optics;soliton dynamics;supercontinuum generation   
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      Published:2024-09-18
    • Yanjun Bao,Qiao Jiang,Yimin Kang,Xing Zhu,Zheyu Fang
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.71
      Abstract:A multifocal metalens, which focuses incident light at multiple foci, has many applications in imaging systems and optical communications. However, the traditional design strategy of a multifocal metalens combines several lenses that have different focal points into a planar integrated unit, resulting in low imaging quality because of the high background noise. Here we show that the defects of the traditional method can be overcome by designing a metalens with conic shapes (the ellipse and the hyperbola); this approach could improve the imaging performance and substantially decrease the background noise of multifocal metalenses. These benefits arise from the intrinsic properties of the two conic curves, which can focus incident light constructively at all of the foci of the metalens. We further demonstrate that the proposed conic-shaped metalens can function well within a broadband operation wavelength that ranges from 600 to 900 nm with the dual polarity actively controlled by the incident circular polarized light. The great agreement between the experimental and simulation results demonstrates that our proposed metalens has significant potential for use in future integrated nanophotonic devices.  
      Keywords:conic shape;metasurface;multifocal metalens;optical performance   
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      Published:2024-09-18
    • Basudeb Sain,Roy Kaner,Yehiam Prior
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.72
      Abstract:Directional emission of electromagnetic radiation can be achieved using a properly shaped single antenna or a phased array of individual antennas. Control of the individual phases within an array enables scanning or other manipulations of the emission, and it is this property of phased arrays that makes them attractive in modern systems. Likewise, the propagation of surface plasmons at the interface between metal films and dielectric materials can be determined by shaping the individual surface nanostructures or via the phase control of individual elements in an array of such structures. Here, we demonstrate control of the propagation of surface plasmons within a linear array of nanostructures. The generic situation of plasmonic surface propagation that is different on both sides of a metal film provides a unique opportunity for such control: plasmons propagating on the slower side feed into the side with the faster propagation, creating a phased array of interfering antennas and thus controlling the directionality of the wake fields. We further show that by shaping the individual nanoantennas, we can generate an asymmetric propagation geometry.  
      Keywords:FDTD;NSOM;phased array;plasmonic wakes;surface plasmons   
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      Published:2024-09-18
    • Germann Hergert,Jan Vogelsang,Felix Schwarz,Dong Wang,Heiko Kollmann,Petra Groß,Christoph Lienau,Erich Runge,Peter Schaaf
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.75
      Abstract:We report long-lived, highly spatially localized plasmon states on the surface of nanoporous gold nanoparticles—nanosponges—with high excitation efficiency. It is well known that disorder on the nanometer scale, particularly in two-dimensional systems, can lead to plasmon localization and large field enhancements, which can, in turn, be used to enhance nonlinear optical effects and to study and exploit quantum optical processes. Here, we introduce promising, three-dimensional model systems for light capture and plasmon localization as gold nanosponges that are formed by the dewetting of gold/silver bilayers and dealloying. We study light-induced electron emission from single nanosponges, a nonlinear process with exponents of n≈5...7, using ultrashort laser pulse excitation to achieve femtosecond time resolution. The long-lived electron emission process proves, in combination with optical extinction measurements and finite-difference time-domain calculations, the existence of localized modes with lifetimes of more than 20 fs. These electrons couple efficiently to the dipole antenna mode of each individual nanosponge, which in turn couples to the far-field. Thus, individual gold nanosponges are cheap and robust disordered nanoantennas with strong local resonances, and an ensemble of nanosponges constitutes a meta material with a strong polarization independent, nonlinear response over a wide frequency range.  
      Keywords:disorder-induced plasmon localization;nanoantennas;nanoporous gold nanoparticles;ultrafast photoemission spectroscopy   
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      Published:2024-09-18
    • Ming Yan,Pei-Ling Luo,Kana Iwakuni,Guy Millot,Theodor W Hänsch,Nathalie Picqué
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.76
      Abstract:Absorption spectroscopy of fundamental ro-vibrational transitions in the mid-infrared region provides a powerful tool for studying the structure and dynamics of molecules in the gas phase and for sensitive and quantitative gas sensing. Laser frequency combs permit novel approaches to perform broadband molecular spectroscopy. Multiplex dual-comb spectroscopy without moving parts can achieve particularly high speed, sensitivity and resolution. However, achieving Doppler-limited resolution in the mid-infrared still requires overcoming instrumental challenges. Here we demonstrate a new approach based on difference-frequency generation of frequency-agile near-infrared frequency combs that are produced using electro-optic modulators. The combs have a remarkably flat intensity distribution, and their positions and line spacings can be freely selected by simply dialing a knob. Using the proposed technique, we record, in the 3-μm region, Doppler-limited absorption spectra with resolved comb lines within milliseconds, and precise molecular line parameters are retrieved. Our technique holds promise for fast and sensitive time-resolved studies of, for example, trace gases.  
      Keywords:Fourier transform spectroscopy;frequency comb;mid-infrared;molecular spectroscopy   
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      Published:2024-09-18
    • Seunghyun Lee,Owoong Kwon,Mansik Jeon,Jaejung Song,Seungjun Shin,HyeMi Kim,Minguk Jo,Taiuk Rim,Junsang Doh,Sungjee Kim,Junwoo Son,Yunseok Kim,Chulhong Kim
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.80
      Abstract:Imaging the intrinsic optical absorption properties of nanomaterials with optical microscopy (OM) is hindered by the optical diffraction limit and intrinsically poor sensitivity. Thus, expensive and destructive electron microscopy (EM) has been commonly used to examine the morphologies of nanostructures. Further, while nanoscale fluorescence OM has become crucial for investigating the morphologies and functions of intracellular specimens, this modality is not suitable for imaging optical absorption and requires the use of possibly undesirable exogenous fluorescent molecules for biological samples. Here we demonstrate super-resolution visible photoactivated atomic force microscopy (pAFM), which can sense intrinsic optical absorption with ~8 nm resolution. Thus, the resolution can be improved down to ~8 nm. This system can detect not only the first harmonic response, but also the higher harmonic response using the nonlinear effect. The thermoelastic effects induced by pulsed laser irradiation allow us to obtain visible pAFM images of single gold nanospheres, various nanowires, and biological cells, all with nanoscale resolution. Unlike expensive EM, the visible pAFM system can be simply implemented by adding an optical excitation sub-system to a commercial atomic force microscope.  
      Keywords:Arabidopsis imaging;gold nanoparticle imaging;melanoma cell imaging;nanowire imaging;super-resolution optical microscopy   
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    • Malcolm C Finlay,Charles A Mosse,Richard J Colchester,Sacha Noimark,Edward Z Zhang,Sebastien Ourselin,Paul C Beard,Richard J Schilling,Ivan P Parkin,Ioannis Papakonstantinou,Adrien E Desjardins
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.103
      Abstract:High-frequency ultrasound imaging can provide exquisite visualizations of tissue to guide minimally invasive procedures. Here, we demonstrate that an all-optical ultrasound transducer, through which light guided by optical fibers is used to generate and receive ultrasound, is suitable for real-time invasive medical imaging in vivo. Broad-bandwidth ultrasound generation was achieved through the photoacoustic excitation of a multiwalled carbon nanotube-polydimethylsiloxane composite coating on the distal end of a 300-μm multi-mode optical fiber by a pulsed laser. The interrogation of a high-finesse Fabry–Pérot cavity on a single-mode optical fiber by a wavelength-tunable continuous-wave laser was applied for ultrasound reception. This transducer was integrated within a custom inner transseptal needle (diameter 1.08 mm; length 78 cm) that included a metallic septum to acoustically isolate the two optical fibers. The use of this needle within the beating heart of a pig provided unprecedented real-time views (50 Hz scan rate) of cardiac tissue (depth: 2.5 cm; axial resolution: 64 μm) and revealed the critical anatomical structures required to safely perform a transseptal crossing: the right and left atrial walls, the right atrial appendage, and the limbus fossae ovalis. This new paradigm will allow ultrasound imaging to be integrated into a broad range of minimally invasive devices in different clinical contexts.  
      Keywords:cardiac;medical devices;optoacoustic;photoacoustic;ultrasound   
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      Published:2024-09-18
    • Qi Yu,Pengli Gao,Kenneth Yin Zhang,Xiao Tong,Huiran Yang,Shujuan Liu,Jing Du,Qiang Zhao,Wei Huang
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.107
      Abstract:Gold nanoclusters (Au NCs) are promising luminescent nanomaterials due to their outstanding optical properties. However, their relatively low quantum yields and environment-dependent photoluminescence properties have limited their biological applications. To address these problems, we developed a novel strategy to prepare chitosan oligosaccharide lactate (Chi)-functionalized Au NCs (Au NCs@Chi), which exhibited emission with enhanced quantum yield and elongated emission lifetime as compared to the Au NCs, as well as exhibited environment-independent photoluminescence properties. In addition, utilizing the free amino groups of Chi onto Au NCs@Chi, we designed a FRET-based sensing platform for the detection of hydrogen sulfide (H2S). The Au NCs and the specific H2S-sensitive merocyanine compound were respectively employed as an energy donor and acceptor in the platform. The addition of H2S induced changes in the emission profile and luminescence lifetime of the platform with high sensitivity and selectivity. Utilization of the platform was demonstrated to detect exogenous and endogenous H2S in vitro and in vivo through wavelength-ratiometric and time-resolved luminescence imaging (TLI). Compared to previously reported luminescent molecules, the platform was less affected by experimental conditions and showed minimized autofluorescence interference and improved accuracy of detection.  
      Keywords:bioimaging;gold nanoclusters;hydrogen sulfide;luminescent sensors;photoluminescence   
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      Published:2024-09-18
    • Andrea Annoni,Emanuele Guglielmi,Marco Carminati,Giorgio Ferrari,Marco Sampietro,David AB Miller,Andrea Melloni,Francesco Morichetti
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.110
      Abstract:Propagation of light beams through scattering or multimode systems may lead to the randomization of the spatial coherence of the light. Although information is not lost, its recovery requires a coherent interferometric reconstruction of the original signals, which have been scrambled into the modes of the scattering system. Here we show that we can automatically unscramble optical beams that have been arbitrarily mixed in a multimode waveguide, undoing the scattering and mixing between the spatial modes through a mesh of silicon photonics tuneable beam splitters. Transparent light detectors integrated in a photonic chip are used to directly monitor the evolution of each mode along the mesh, allowing sequential tuning and adaptive individual feedback control of each beam splitter. The entire mesh self-configures automatically through a progressive tuning algorithm and resets itself after significantly perturbing the mixing, without turning off the beams. We demonstrate information recovery by the simultaneous unscrambling, sorting and tracking of four mixed modes, with residual cross-talk of −20 dB between the beams. Circuit partitioning assisted by transparent detectors enables scalability to meshes with a higher port count and to a higher number of modes without a proportionate increase in the control complexity. The principle of self-configuring and self-resetting in optical systems should be applicable in a wide range of optical applications.  
      Keywords:optical processing;photonic integrated circuits;silicon photonics;tuneable photonic devices   
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      Published:2024-09-18

      Review

    • Lucia Caspani,Chunle Xiong,Benjamin J Eggleton,Daniele Bajoni,Marco Liscidini,Matteo Galli,Roberto Morandotti,David J Moss
      Vol. 6, Issue 4, (2017) DOI: 10.1038/lsa.2017.100
      Abstract:The ability to generate complex optical photon states involving entanglement between multiple optical modes is not only critical to advancing our understanding of quantum mechanics but will play a key role in generating many applications in quantum technologies. These include quantum communications, computation, imaging, microscopy and many other novel technologies that are constantly being proposed. However, approaches to generating parallel multiple, customisable bi- and multi-entangled quantum bits (qubits) on a chip are still in the early stages of development. Here, we review recent advances in the realisation of integrated sources of photonic quantum states, focusing on approaches based on nonlinear optics that are compatible with contemporary optical fibre telecommunications and quantum memory platforms as well as with chip-scale semiconductor technology. These new and exciting platforms hold the promise of compact, low-cost, scalable and practical implementations of sources for the generation and manipulation of complex quantum optical states on a chip, which will play a major role in bringing quantum technologies out of the laboratory and into the real world.  
      Keywords:entanglement;integrated optics;nonlinear optics;photon pairs;quantum optics;quantum states   
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      Published:2024-09-18
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