Abstract:We have discovered a strong increase in the intensity of the chemiluminescence of a luminol flow and a dramatic modification of its spectral shape in the presence of metallic nanoparticles. We observed that pumping gold and silver nanoparticles into a microfluidic device fabricated in polydimethylsiloxane prolongs the glow time of luminol. We have demonstrated that the intensity of chemiluminescence in the presence of nanospheres depends on the position along the microfluidic serpentine channel. We show that the enhancement factors can be controlled by the nanoparticle size and material. Spectrally, the emission peak of luminol overlaps with the absorption band of the nanospheres, which maximizes the effect of confined plasmons on the optical density of states in the vicinity of the luminol emission peak. These observations, interpreted in terms of the Purcell effect mediated by nano-plasmons, form an essential step toward the development of microfluidic chips with gain media. Practical implementation of the discovered effect will include improving the detection limits of chemiluminescence for forensic science, research in biology and chemistry, and a number of commercial applications.
X Luís Deán-Ben,Gali Sela,Antonella Lauri,Moritz Kneipp,Vasilis Ntziachristos,Gil G Westmeyer,Shy Shoham,Daniel Razansky
Vol. 5, Issue 4, (2016) DOI: 10.1038/lsa.2016.201
Abstract:Non-invasive observation of spatiotemporal activity of large neural populations distributed over entire brains is a longstanding goal of neuroscience. We developed a volumetric multispectral optoacoustic tomography platform for imaging neural activation deep in scattering brains. It can record 100 volumetric frames per second across scalable fields of view ranging between 50 and 1000 mm3 with respective spatial resolution of 35–200 μm. Experiments performed in immobilized and freely swimming larvae and in adult zebrafish brains expressing the genetically encoded calcium indicator GCaMP5G demonstrate, for the first time, the fundamental ability to directly track neural dynamics using optoacoustics while overcoming the longstanding penetration barrier of optical imaging in scattering brains. The newly developed platform thus offers unprecedented capabilities for functional whole-brain observations of fast calcium dynamics; in combination with optoacoustics' well-established capacity for resolving vascular hemodynamics, it could open new vistas in the study of neural activity and neurovascular coupling in health and disease.
Marina Mariano,Gregory Kozyreff,Luis G Gerling,Pablo Romero-Gomez,Joaquim Puigdollers,Jorge Bravo-Abad,Jordi Martorell
Vol. 5, Issue 4, (2016) DOI: 10.1038/lsa.2016.216
Abstract:Extracting the light trapped in a waveguide, or the opposite effect of trapping light in a thin region and guiding it perpendicular to its incident propagation direction, is essential for optimal energetic performance in illumination, display or light harvesting devices. Here we demonstrate that the paradoxical goal of letting as much light in or out while maintaining the wave effectively trapped can be achieved with a periodic array of interpenetrated fibers forming a photonic fiber plate. Photons entering perpendicular to that plate may be trapped in an intermittent chaotic trajectory, leading to an optically ergodic system. We fabricated such a photonic fiber plate and showed that for a solar cell incorporated on one of the plate surfaces, light absorption is greatly enhanced. Confirming this, we found the unexpected result that a more chaotic photon trajectory reduces the production of photon scattering entropy.
Karl Zhanghao,Long Chen,Xu-San Yang,Miao-Yan Wang,Zhen-Li Jing,Hong-Bin Han,Michael Q Zhang,Dayong Jin,Jun-Tao Gao,Peng Xi
Vol. 5, Issue 4, (2016) DOI: 10.1038/lsa.2016.166
Abstract:Fluorescence polarization microscopy (FPM) aims to detect the dipole orientation of fluorophores and to resolve structural information for labeled organelles via wide-field or confocal microscopy. Conventional FPM often suffers from the presence of a large number of molecules within the diffraction-limited volume, with averaged fluorescence polarization collected from a group of dipoles with different orientations. Here, we apply sparse deconvolution and least-squares estimation to fluorescence polarization modulation data and demonstrate a super-resolution dipole orientation mapping (SDOM) method that resolves the effective dipole orientation from a much smaller number of fluorescent molecules within a sub-diffraction focal area. We further apply this method to resolve structural details in both fixed and live cells. For the first time, we show that different borders of a dendritic spine neck exhibit a heterogeneous distribution of dipole orientation. Furthermore, we illustrate that the dipole is always perpendicular to the direction of actin filaments in mammalian kidney cells and radially distributed in the hourglass structure of the septin protein under specific labelling. The accuracy of the dipole orientation can be further mapped using the orientation uniform factor, which shows the superiority of SDOM compared with its wide-field counterpart as the number of molecules is decreased within the smaller focal area. Using the inherent feature of the orientation dipole, the SDOM technique, with its fast imaging speed (at sub-second scale), can be applied to a broad range of fluorescently labeled biological systems to simultaneously resolve the valuable dipole orientation information with super-resolution imaging.
Valery N Konopsky,Elena V Alieva,Sergey Yu Alyatkin,Alexey A Melnikov,Sergey V Chekalin,Vladimir M Agranovich
Vol. 5, Issue 4, (2016) DOI: 10.1038/lsa.2016.168
Abstract:Efficient nonlinear conversion requires that interacting optical waves maintain a consistent phase relationship when traveling in a medium despite its dispersion. Birefringent phase-matching, which is often used to compensate for the dispersion, is not applicable to optically isotropic nonlinear materials. Here, we present a one-dimensional photonic crystal structure that allows the propagation of optical surface waves, both at the fundamental and third-harmonic frequencies, as an efficient medium for phase-matched third-harmonic generation. A unique advantage of this structure is that the effective refractive indices for the surface waves are similar to the refractive index of air at both frequencies. This allows phase-matching between the first and third harmonics, and a visible collinear beam of the third harmonic is produced at the prism-coupled output. Moreover, these optical surface waves propagate over long distances even if a lossy nonlinear nanofilm is deposited onto the photonic crystal surface. We provide experimental results for third-harmonic generation at a wavelength of 410 nm for a bare dielectric Ta2O5/SiO2 multilayer structure and for the same structure coated with a 15-nm GaAs film.
Rajendran Rajeev,Johannes Hellwagner,Anne Schumacher,Inga Jordan,Martin Huppert,Andres Tehlar,Bhargava Ram Niraghatam,Denitsa Baykusheva,Nan Lin,Aaron von Conta,Hans Jakob Wörner
Vol. 5, Issue 4, (2016) DOI: 10.1038/lsa.2016.170
Abstract:Monochromatization of high-harmonic sources has opened fascinating perspectives regarding time-resolved photoemission from all phases of matter. Such studies have invariably involved the use of spectral filters or spectrally dispersive optical components that are inherently lossy and technically complex. Here we present a new technique for the spectral selection of near-threshold harmonics and their spatial separation from the driving beams without any optical elements. We discover the existence of a narrow phase-matching gate resulting from the combination of the non-collinear generation geometry in an extended medium, atomic resonances and absorption. Our technique offers a filter contrast of up to 104 for the selected harmonics against the adjacent ones and offers multiple temporally synchronized beamlets in a single unified scheme. We demonstrate the selective generation of 133, 80 or 56 nm femtosecond pulses from a 400-nm driver, which is specific to the target gas. These results open new pathways towards phase-sensitive multi-pulse spectroscopy in the vacuum- and extreme-ultraviolet, and frequency-selective output coupling from enhancement cavities.
Abstract:Because of their exceptional capability to tailor the effective medium parameters, metamaterials have been widely used to control electromagnetic waves, which has led to the observation of many interesting phenomena, for example, negative refraction, invisibility cloaking, and anomalous reflections and transmissions. However, the studies of metamaterials or metasurfaces are mainly limited to their physical features; currently, there is a lack of viewpoints on metamaterials and metasurfaces from the information perspective. Here we propose to measure the information of a coding metasurface using Shannon entropy. We establish an analytical connection between the coding pattern of an arbitrary coding metasurface and its far-field pattern. We introduce geometrical entropy to describe the information of the coding pattern (or coding sequence) and physical entropy to describe the information of the far-field pattern of the metasurface. The coding metasurface is demonstrated to enhance the information in transmitting messages, and the amount of enhanced information can be manipulated by designing the coding pattern with different information entropies. The proposed concepts and entropy control method will be helpful in new information systems (for example, communication, radar and imaging) that are based on the coding metasurfaces.
Roman Gansch,Stefan Kalchmair,Patrice Genevet,Tobias Zederbauer,Hermann Detz,Aaron M Andrews,Werner Schrenk,Federico Capasso,Marko Lončar,Gottfried Strasser
Vol. 5, Issue 4, (2016) DOI: 10.1038/lsa.2016.147
Abstract:We directly measure optical bound states in the continuum (BICs) by embedding a photodetector into a photonic crystal slab. The BICs observed in our experiment are the result of accidental phase matching between incident, reflected and in-plane waves at seemingly random wave vectors in the photonic band structure. Our measurements were confirmed through a rigorously coupled-wave analysis simulation in conjunction with temporal coupled mode theory. Polarization mixing between photonic crystal slab modes was observed and described using a plane wave expansion simulation. The ability to probe the field intensity inside the photonic crystal and thereby to directly measure BICs represents a milestone in the development of integrated opto-electronic devices based on BICs.
Xue-Yu Zhang,Shi-Han Sun,Xiao-Juan Sun,Yan-Rong Zhao,Li Chen,Yue Yang,Wei Lü,Da-Bing Li
Vol. 5, Issue 4, (2016) DOI: 10.1038/lsa.2016.130
Abstract:Commonly used energy storage devices include stacked layers of active materials on two-dimensional sheets, and the limited specific surface area restricts the further development of energy storage. Three-dimensional (3D) structures with high specific surface areas would improve device performance. Herein, we present a novel procedure to fabricate macroscopic, high-quality, nitrogen-doped, 3D graphene/nanoparticle aerogels. The procedure includes vacuum filtration, freeze-drying, and plasma treatment, which can be further expanded for large-scale production of nitrogen-doped, graphene-based aerogels. The behavior of the supercapacitor is investigated using a typical nitrogen-doped graphene/Fe3O4 nanoparticle 3D structure (NG/Fe3O4). Compared with 3D graphene/Fe3O4 structures prepared by the traditional hydrothermal method, the NG/Fe3O4 supercapacitor prepared by the present method has a 153% improvement in specific capacitance, and there is no obvious decrease in specific capacitance after 1000 cycles. The present work provides a new and facile method to produce large-scale, 3D, graphene-based materials with high specific capacitance for energy storage.
Abstract:Color rendition, luminous efficacy and reliability are three key technical parameters for white light-emitting diodes (wLEDs) that are dominantly determined by down-conversion phosphors. However, there is usually an inevitable trade-off between color rendition and luminescence efficacy because the spectrum of red phosphor (that is, spectral broadness and position) cannot satisfy them simultaneously. In this work, we report a very promising red phosphor that can minimize the aforementioned trade-off via structure and band-gap engineering, achieved by introducing isostructural LiSi2N3 into CaAlSiN3: Eu2+. The solid solution phosphors show both substantial spectra broadening (88→117 nm) and blueshift (652→642 nm), along with a significant improvement in thermal quenching (only a 6% reduction at 150 ℃), which are strongly associated with electronic and crystal structure evolutions. The broadband and robust red phosphor thus enables fabrication of super-high color rendering wLEDs (Ra=95 and R9=96) concurrently with the maintenance of a high-luminous efficacy (101 lm W−1), validating its superiority in high-performance solid state lightings over currently used red phosphors.
Mark Jayson Villangca,Darwin Palima,Andrew Rafael Bañas,Jesper Glückstad
Vol. 5, Issue 4, (2016) DOI: 10.1038/lsa.2016.148
Abstract:Leveraging developments in microfabrication open new possibilities for optical manipulation. With the structural design freedom from three-dimensional printing capabilities of two-photon polymerization, we are starting to see the emergence of cleverly shaped 'light robots' or optically actuated micro-tools that closely resemble their macroscopic counterparts in function and sometimes even in form. In this work, we have fabricated a new type of light robot that is capable of loading and unloading cargo using photothermally induced convection currents within the body of the tool. We have demonstrated this using silica and polystyrene beads as cargo. The flow speeds of the cargo during loading and unloading are significantly larger than when using optical forces alone. This new type of light robot presents a mode of material transport that may have a significant impact on targeted drug delivery and nanofluidics injection.
Abstract:We introduce an extremely simple and highly stable system for stimulated Raman scattering (SRS) microscopy. An 8-W, 450-fs Yb: KGW bulk oscillator with 41 MHz repetition rate pumps an optical parametric amplifier, which is seeded by a cw tunable external cavity diode laser. The output radiation is frequency doubled in a long PPLN crystal and generates 1.5-ps long narrowband pump pulses that are tunable between 760 and 820 nm with > 50 mW average power. Part of the oscillator output is sent through an etalon and creates Stokes pulses with 100 mW average power and 1.7 ps duration. We demonstrate SRS microscopy at a 30-μs pixel dwell time with high chemical contrast, signal-to-noise ratio in excess of 45 and no need for balanced detection, thanks to the favorable noise properties of the bulk solid-state system. Cw seeding intrinsically ensures low spectral drift. We discuss its application to chemical contrast microscopy of freshly prepared plant tissue sections at different vibrational bands.
Otto L Muskens,Luca Bergamini,Yudong Wang,Jeffrey M Gaskell,Nerea Zabala,CH de Groot,David W Sheel,Javier Aizpurua
Vol. 5, Issue 4, (2016) DOI: 10.1038/lsa.2016.173
Abstract:Nanoscale devices in which the interaction with light can be configured using external control signals hold great interest for next-generation optoelectronic circuits. Materials exhibiting a structural or electronic phase transition offer a large modulation contrast with multi-level optical switching and memory functionalities. In addition, plasmonic nanoantennas can provide an efficient enhancement mechanism for both the optically induced excitation and the readout of materials strategically positioned in their local environment. Here, we demonstrate picosecond all-optical switching of the local phase transition in plasmonic antenna-vanadium dioxide (VO2) hybrids, exploiting strong resonant field enhancement and selective optical pumping in plasmonic hotspots. Polarization- and wavelength-dependent pump–probe spectroscopy of multifrequency crossed antenna arrays shows that nanoscale optical switching in plasmonic hotspots does not affect neighboring antennas placed within 100 nm of the excited antennas. The antenna-assisted pumping mechanism is confirmed by numerical model calculations of the resonant, antenna-mediated local heating on a picosecond time scale. The hybrid, nanoscale excitation mechanism results in 20 times reduced switching energies and 5 times faster recovery times than a VO2 film without antennas, enabling fully reversible switching at over two million cycles per second and at local switching energies in the picojoule range. The hybrid solution of antennas and VO2 provides a conceptual framework to merge the field localization and phase-transition response, enabling precise, nanoscale optical memory functionalities.
Yu-Chao Li,Hong-Bao Xin,Hong-Xiang Lei,Lin-Lin Liu,Yan-Ze Li,Yao Zhang,Bao-Jun Li
Vol. 5, Issue 4, (2016) DOI: 10.1038/lsa.2016.176
Abstract:Optical methods to manipulate and detect nanoscale objects are highly desired in both nanomaterials and molecular biology fields. Optical tweezers have been used to manipulate objects that range in size from a few hundred nanometres to several micrometres. The emergence of near-field methods that overcome the diffraction limit has enabled the manipulation of objects below 100 nm. A highly free manipulation with signal-enhanced real-time detection, however, remains a challenge for single sub-100-nm nanoparticles or biomolecules. Here we show an approach that uses a photonic nanojet to perform the manipulation and detection of single sub-100-nm objects. With the photonic nanojet generated by a dielectric microlens bound to an optical fibre probe, three-dimensional manipulations were achieved for a single 85-nm fluorescent polystyrene nanoparticle as well as for a plasmid DNA molecule. Backscattering and fluorescent signals were detected with the enhancement factors up to ~103 and ~30, respectively. The demonstrated approach provides a potentially powerful tool for nanostructure assembly, biosensing and single-biomolecule studies.
Bin Zheng,Hamza Ahmad Madni,Ran Hao,Xianmin Zhang,Xu Liu,Erping Li,Hongsheng Chen
Vol. 5, Issue 4, (2016) DOI: 10.1038/lsa.2016.177
Abstract:An invisibility cloak that can hide an arbitrary object external to the cloak itself has not been devised before. In this Letter, we introduce a novel way to design a remote cloaking device that makes any object located at a certain distance invisible. This is accomplished using multi-folded transformation optics to remotely generate a hidden region around the object that no field can penetrate and that does not disturb the far-field scattering electromagnetic field. As a result, any object in the hidden region can stay in position or move freely within that region and remain invisible. Our idea is further extended in order to design a remote illusion optics that can transform any arbitrary object into another one. Unlike other cloaking methods, this method would require no knowledge of the details of the object itself. The proposed multi-folded transformation optics will be crucial in the design of remote devices in a variety of contexts.
Abstract:The paper addresses the creation of circular optical properties from a femtosecond laser light beam with a linear polarization in an achiral material (glass) under an orthogonal incidence. In this situation, all aspects of the experiment are achiral and therefore should not give rise to chiral property creation. From that observation, we propose an interpretation that involves the action of a light-induced torque on the matter carrying a light-induced dielectric moment. We found that a direct current (DC) electric field could be produced in the lattice by the femtosecond laser in our conditions and that a non-collinear dielectric moment is created by a nonlinear effect between the DC electric field and the stress field due to the transformation of the material. We reveal that it is possible to break the chiral symmetry of glass using an intense, ultrashort laser light pulse.
Xi Wang,Yang Deng,Qitong Li,Yijing Huang,Zilun Gong,Kyle B Tom,Jie Yao
Vol. 5, Issue 4, (2016) DOI: 10.1038/lsa.2016.179
Abstract:Accompanied by the rise of plasmonic materials beyond those based on noble metals and the development of advanced materials processing techniques, it is important to understand the plasmonic behavior of materials with large-scale inhomogeneity (such as gradient permittivity materials) because they cannot be modeled simply as scatterers. In this paper, we theoretically analyze the excitation and propagation of surface plasmon polaritons (SPPs) on a planar interface between a homogeneous dielectric and a material with a gradient of negative permittivity. We demonstrate the following: (ⅰ) free-space propagating waves and surface waves can be coupled by a gradient negative-permittivity material and (ⅱ) the coupling can be enhanced if the material permittivity variation is suitably designed. This theory is then verified by numerical simulations. A direct application of this theory, 'rainbow trapping', is also proposed, considering a realistic design based on doped indium antimonide. This theory may lead to various applications, such as ultracompact spectroscopy and dynamically controllable generation of SPPs.
Abstract:Two parallel optical surfaces often exhibit colorful fringes along the lines of equal thickness because of the interference of light. This simple phenomenon allows one to observe subwavelength corrugations on a reflective surface by simply placing on it a flat reference dielectric surface, a so-called optical flat, and inspecting the resultant interference pattern. In this work, we extend this principle from dielectric surfaces to two-dimensional plasmonic nanostructures. Optical couplings between an Au nanodisk array and an Au thin film were measured quantitatively using two different techniques, namely, the classical Newton's rings method and a closed-loop nano-positioning system. Extremely high spectral sensitivity to the inter-surface distance was observed in the near-field coupling regime, where a 1-nm change in distance could alter the resonance wavelength by almost 10 nm, > 40 times greater than the variation in the case without near-field coupling. With the help of a numerical fitting technique, the resonance wavelength could be determined with a precision of 0.03 nm, corresponding to a distance precision as high as 0.003 nm. Utilizing this effect, we demonstrated that a plasmonic nanodisk array can be utilized as a plasmonic optical flat, with which nanometer-deep grooves can be directly visualized using a low-cost microscope.
Abstract:Optical fibre sensors based on Brillouin scattering have been vigorously studied in the context of structural health monitoring on account of their capacity for distributed strain and temperature measurements. However, real-time distributed strain measurement has been achieved only for two-end-access systems; such systems reduce the degree of freedom in embedding the sensors into structures, and furthermore render the measurement no longer feasible when extremely high loss or breakage occurs at a point along the sensing fibre. Here, we demonstrate real-time distributed measurement with an intrinsically one-end-access reflectometry configuration by using a correlation-domain technique. In this method, the Brillouin gain spectrum is obtained at high speed using a voltage-controlled oscillator, and the Brillouin frequency shift is converted into a phase delay of a synchronous sinusoidal waveform; the phase delay is subsequently converted into a voltage, which can be directly measured. When a single-point measurement is performed at an arbitrary position, a strain sampling rate of up to 100 kHz is experimentally verified by detecting locally applied dynamic strain at 1 kHz. When distributed measurements are performed at 100 points with 10 times averaging, a repetition rate of 100 Hz is verified by tracking a mechanical wave propagating along the fibre. Some drawbacks of this ultrahigh-speed configuration, including the reduced measurement accuracy, lowered spatial resolution and limited strain dynamic range, are also discussed.
Keywords:Brillouin scattering;distributed strain and temperature sensing;high-speed measurement;nonlinear optics;optical fibre sensors
Abstract:Entangled quantum states in high-dimensional space show many advantages compared with entangled states in two-dimensional space. The former enable quantum communication with higher channel capacity, enable more efficient quantum-information processing and are more feasible for closing the detection loophole in Bell test experiments. Establishing high-dimensional entangled memories is essential for long-distance communication, but its experimental realization is lacking. We experimentally established high-dimensional entanglement in orbital angular momentum space between two atomic ensembles separated by 1 m. We reconstructed the density matrix for a three-dimensional entanglement and obtained an entanglement fidelity of (83.9±2.9)%. More importantly, we confirmed the successful preparation of a state entangled in more than three-dimensional space (up to seven-dimensional) using entanglement witnesses. Achieving high-dimensional entanglement represents a significant step toward a high-capacity quantum network.
Anna S Bezryadina,Daryl C Preece,Joseph C Chen,Zhigang Chen
Vol. 5, Issue 4, (2016) DOI: 10.1038/lsa.2016.158
Abstract:Bacterial biofilms underlie many persistent infections, posing major hurdles in antibiotic treatment. Here we design and demonstrate 'tug-of-war' optical tweezers that can facilitate the assessment of cell–cell adhesion—a key contributing factor to biofilm development, thanks to the combined actions of optical scattering and gradient forces. With a customized optical landscape distinct from that of conventional tweezers, not only can such 'tug-of-war' tweezers stably trap and stretch a rod-shaped bacterium in the observing plane, but, more importantly, they can also impose a tunable lateral force that pulls apart cellular clusters without any tethering or mechanical movement. As a proof of principle, we examined a Sinorhizobium meliloti strain that forms robust biofilms and found that the strength of intercellular adhesion depends on the growth medium. This technique may herald new photonic tools for optical manipulation and biofilm study, as well as other biological applications.
Yohannes Abate,Sampath Gamage,Zhen Li,Viktoriia Babicheva,Mohammad H Javani,Han Wang,Stephen B Cronin,Mark I Stockman
Vol. 5, Issue 4, (2016) DOI: 10.1038/lsa.2016.162
Abstract:Black phosphorus (BP) is an emerging two-dimensional material with intriguing physical properties. It is highly anisotropic and highly tunable by means of both the number of monolayers and surface doping. Here, we experimentally investigate and theoretically interpret the near-field properties of a-few-atomic-monolayer nanoflakes of BP. We discover near-field patterns of bright outside fringes and a high surface polarizability of nanofilm BP consistent with its surface-metallic, plasmonic behavior at mid-infrared frequencies < 1176 cm−1. We conclude that these fringes are caused by the formation of a highly polarizable layer at the BP surface. This layer has a thickness of ~1 nm and exhibits plasmonic behavior. We estimate that it contains free carriers in a concentration of n≈1.1 × 1020 cm−3. Surface plasmonic behavior is observed for 10–40 nm BP thicknesses but absent for a 4-nm BP thickness. This discovery opens up a new field of research and potential applications in nanoelectronics, plasmonics and optoelectronics.