Diffraction Limit Of Light Research Articles

Coupled-Dipole Modeling and Experimental Characterization of Geometry-Dependent Trochoidal Dichroism in Nanorod Trimers

Noble metal nanoparticles host surface plasmon resonances that confine electromagnetic waves below the diffraction limit of light, making them effective building blocks for near-field optical anten...

Subwavelength optical localization with toroidal excitations in plasmonic and Mie metamaterials

AbstractSince the performance of electronic circuits is becoming rather limited in face of intensively increasing of amount of information and related operations, all‐optical processing offers a promising strategy for future information system. It would benefit a great deal if the all‐optical processing could be implemented within the developed electronic chips of nanoscale structures. In that it is highly desirable to break the diffraction limit of light for achieving effective light manipulations with deep subwavelength structures compatible with the state‐of‐the‐art nanofabrication processes. It is of fundamental importance to get subwavelength optical localization, that is, squeeze light wave into subwavelength space for achieving freely manipulating of light fields. This review summarizes the development in realizing subwavelength optical localization by exciting toroidal mode in photonic metamaterials. The toroidal excitations in plasmonic metamaterials and Mie resonant metamaterials, in 3D structures and planar metamaterials, with single or few layers in spectral regime from microwave to optical frequencies are surveyed. Based on the discussion on the configurations of toroidal excitations, the recent development on toroidal‐related optical scattering control actively manipulates the toroidal excitations, and promising applications are further investigated and highlighted.image

Nanocomposite Interfaces: Resolving Nanocomposite Interfaces via Simultaneous Submicrometer Optical‐Photothermal Infrared‐Raman Microspectroscopy (Adv. Mater. Interfaces 5/2021)

Conventional Fourier-transform infrared (FTIR) and quantum cascade laser IR microspectroscopies are limited in spatial resolution by the diffraction limit of IR light. The optical-photothermal infrared (O-PTIR) technique with simultaneous Raman microspectroscopy (O-PTIR+R) described in this work affords wavelength independent position-specific IR spectra with submicron spatial resolution, demonstrating unprecedented spatial resolution of nanocarbon-based polymer nanocomposite interphases with chemical exactitude. More details can be found in article number 2001720 by Alexander J. Wang and co-workers.

An Estimation Algorithm for General Linear Single Particle Tracking Models with Time-Varying Parameters.

Single Particle Tracking (SPT) is a powerful class of methods for studying the dynamics of biomolecules inside living cells. The techniques reveal the trajectories of individual particles, with a resolution well below the diffraction limit of light, and from them the parameters defining the motion model, such as diffusion coefficients and confinement lengths. Most existing algorithms assume these parameters are constant throughout an experiment. However, it has been demonstrated that they often vary with time as the tracked particles move through different regions in the cell or as conditions inside the cell change in response to stimuli. In this work, we propose an estimation algorithm to determine time-varying parameters of systems that discretely switch between different linear models of motion with Gaussian noise statistics, covering dynamics such as diffusion, directed motion, and Ornstein–Uhlenbeck dynamics. Our algorithm consists of three stages. In the first stage, we use a sliding window approach, combined with Expectation Maximization (EM) to determine maximum likelihood estimates of the parameters as a function of time. These results are only used to roughly estimate the number of model switches that occur in the data to guide the selection of algorithm parameters in the second stage. In the second stage, we use Change Detection (CD) techniques to identify where the models switch, taking advantage of the off-line nature of the analysis of SPT data to create non-causal algorithms with better precision than a purely causal approach. Finally, we apply EM to each set of data between the change points to determine final parameter estimates. We demonstrate our approach using experimental data generated in the lab under controlled conditions.

Counting Fluorophores and Finding Potentials from FRET, Bayesian Nonparametrics for Challenging Problems in Biophysics

Fluorescence spectroscopy is a great way to reveal complex interactions at the molecular level, but because fluorophores are much smaller than the diffraction limit of light, one bright spot may contain many fluorescently labeled biomolecules. One technique to quantify the number of molecules within a diffraction limited spot is to illuminate the spot, putting the fluorophores into their fluorescently active bright states, then to watch for steplike brightness drops as the fluorophores photobleach one-by-one. This analysis is impeded by detector noise, shot noise, and by the fact that fluorophores can have dark states and multiple bright states. Furthermore, because the number of fluorophores is unknown, we cannot utilize traditional Bayesian methods to count and we must invoke new methods to solve the problem. Here we use Bayesian nonparametric (BNP) tools, that are necessary as the number of fluorophores is unknown, to solve the counting problem. We conclude that our method allows us to count upwards of 100 fluorophores. Single molecule Forster resonance energy transfer (FRET) based fluorescence experiments are a useful way to probe configuration dynamics of molecules based on the distance between donor and acceptor labels. Here we show that we can use single photon information to extract potential profiles from molecules of interest. We do so using Gaussian processes, a powerful tool within BNPs

Scaling of metal-clad InP nanodisk lasers: optical performance and thermal effects.

A key component for optical on-chip communication is an efficient light source. However, to enable low energy per bit communication and local integration with Si CMOS, devices need to be further scaled down. In this work, we fabricate micro- and nanolasers of different shapes in InP by direct wafer bonding on Si. Metal-clad cavities have been proposed as means to scale dimensions beyond the diffraction limit of light by exploiting hybrid photonic-plasmonic modes. Here, we explore the size scalability of whispering-gallery mode light sources by cladding the sidewalls of the device with Au. We demonstrate room temperature lasing upon optical excitation for Au-clad devices with InP diameters down to 300 nm, while the purely photonic counterparts show lasing only down to 500 nm. Numerical thermal simulations support the experimental findings and confirm an improved heat-sinking capability of the Au-clad devices, suggesting a reduction in device temperature of 450 - 500 K for the metal-clad InP nanodisk laser, compared to the one without Au. This would provide substantial performance benefits even in the absence of a plasmonic mode. These results give an insight into the benefits of metal-clad designs to downscale integrated lasers on Si.

Super-Resolution Live Cell Imaging of Subcellular Structures.

There has long been a crucial tradeoff between spatial and temporal resolution in imaging. Imaging beyond the diffraction limit of light has traditionally been restricted to be used only on fixed samples or live cells outside of tissue labeled with strong fluorescent signal. Current super-resolution live cell imaging techniques require the use of special fluorescence probes, high illumination, multiple image acquisitions with post-acquisition processing, or often a combination of these processes. These prerequisites significantly limit the biological samples and contexts that this technique can be applied to. Here we describe a method to perform super-resolution (~140 nm XY-resolution) time-lapse fluorescence live cell imaging in situ. This technique is also compatible with low fluorescent intensity, for example, EGFP or mCherry endogenously tagged at lowly expressed genes. As a proof-of-principle, we have used this method to visualize multiple subcellular structures in the Drosophila testis. During tissue preparation, both the cellular structure and tissue morphology are maintained within the dissected testis. Here, we use this technique to image microtubule dynamics, the interactions between microtubules and the nuclear membrane, as well as the attachment of microtubules to centromeres. This technique requires special procedures in sample preparation, sample mounting and immobilizing of specimens. Additionally, the specimens must be maintained for several hours after dissection without compromising cellular function and activity. While we have optimized the conditions for live super-resolution imaging specifically in Drosophila male germline stem cells (GSCs) and progenitor germ cells in dissected testis tissue, this technique is broadly applicable to a variety of different cell types. The ability to observe cells under their physiological conditions without sacrificing either spatial or temporal resolution will serve as an invaluable tool to researchers seeking to address crucial questions in cell biology.

Resolving Nanocomposite Interfaces via Simultaneous Submicrometer Optical‐Photothermal Infrared‐Raman Microspectroscopy

AbstractNanocomposite materials are assuming increasingly important roles across contemporary materials science. Analytical characterizations and visualizations of nanoscale interphases/interfaces are critical to development of novel multiphase nanostructures and nanoscale systems. While conventional vibrational spectroscopies are indispensable physicochemical characterization tools, standard techniques such as Fourier‐transform and quantum cascade laser infrared (IR) microspectroscopies are intrinsically limited in spatial resolution by the wavelength‐dependent diffraction limit of IR light (≈5–12 µm). Optical‐photothermal infrared (O‐PTIR) with simultaneous hyperspectral Raman microspectroscopy (O‐PTIR+R) is a novel all‐optical technique that circumvents such diffraction limits, yielding position‐specific IR spectra with sub‐micrometer wavelength‐independent resolution across the mid‐IR. This work implements single‐frequency O‐PTIR with concomitant hyperspectral Raman microspectroscopy to resolve interfacial regions in a poly(octadecyl acrylate)‐grafted‐multiwall carbon nanotube (PODA‐g‐MWCNT) nanocomposite for wearable temperature sensors and highlights how the O‐PTIR+R technique can be used for analytical characterization and visualization of other nanocomposite systems below resolution limitations of conventional IR spectroscopies.

Expansion microscopy of the mitotic spindle.

The mitotic spindle is a dynamic and complex cellular structure made of microtubules and associated proteins. Although the general localization of most proteins has been identified, the arrangement of the microtubules in the mitotic spindle and precise localization of various proteins are still under intensive research. However, techniques used previously to decipher such puzzles are resolution limited or require complex microscopy systems. On the other hand, expansion microscopy is a novel super-resolution microscopy technique that uses physical expansion of fixed specimens to allow features closer than the diffraction limit of light (~250nm) to become resolvable in the expanded specimen on a conventional confocal microscope. This chapter focuses on expansion microscopy of the mitotic spindle, specifically using tubulin labeling to visualize all microtubule subpopulations within the spindle. Furthermore, we discuss a protocol for expansion of GFP-tagged proteins, such as protein regulator of cytokinesis 1 (PRC1). We also discuss various approaches for image analysis pointing out main advantages of expansion microscopy when compared to previously used techniques. This approach is currently used in our laboratory to study the architecture of the microtubules in the mitotic spindle after perturbations of various proteins important for the structural and dynamical properties of the mitotic spindle.

Expansion STED microscopy (ExSTED).

The recently developed expansion microscopy method (ExM) allows for the resolution of structures below the diffraction limit of light not by sophisticated instrumentation, but rather by physically expanding the molecular structure of cells. This happens by crosslinking the protein in the sample to a hydrogel that is polymerized in situ and subsequently expanded, tearing the proteins apart in a nearly isotropic manner. In the resulting, larger facsimile of the original sample, the fluorescence-labeled molecules of interest can be optically separated by conventional fluorescence microscopy since the intermolecular distances are enlarged by a factor ranging from ~4 to 20 depending on the chemistry used for the hydrogel. The achieved improvement in resolution thus corresponds to the expansion factor. Further increase in resolution beyond this value may be achieved by combining ExM with established super-resolution microscopy methods. Indeed, this is possible using structured illumination microscopy (SIM) (Halpern et al., 2017; Wang et al., 2018), single molecule localization microscopy (SMLM) (Zwettler et al., 2020) and stimulated emission depletion (STED), as we and others have shown recently (Gambarotto et al., 2019; Gao et al., 2018; Kim, Kim, Lee, & Shim, 2019; Unnersjö-Jess et al., 2016). Here, we provide a protocol, for our method, called ExSTED, which enabled us to achieve an increase in resolution of up to 30-fold compared to conventional microscopy, well beyond what is possible with conventional STED microscopy. Our protocol includes a strategy to achieve very high intensity fluorescence labeling, which is essential for optimal signal retention during the expansion process for ExSTED.

A Novel Method to Map Small RNAs with High Resolution.

Analyzing cellular structures and the relative location of molecules is essential for addressing biological questions. Super-resolution microscopy techniques that bypass the light diffraction limit have become increasingly popular to study cellular molecule dynamics in situ. However, the application of super-resolution imaging techniques to detect small RNAs (sRNAs) is limited by the choice of proper fluorophores, autofluorescence of samples, and failure to multiplex. Here, we describe an sRNA-PAINT protocol for the detection of sRNAs at nanometer resolution. The method combines the specificity of locked nucleic acid probes and the low background, precise quantitation, and multiplexable characteristics of DNA Point Accumulation for Imaging in Nanoscale Topography (DNA-PAINT). Using this method, we successfully located sRNA targets that are important for development in maize anthers at sub-20 nm resolution and quantitated their exact copy numbers. Graphic abstract: Multiplexed sRNA-PAINT. Multiple Vetting and Analysis of RNA for In Situ Hybridization (VARNISH) probes with different docking strands (i.e., a, b, …) will be hybridized to samples. The first probe will be imaged with the a* imager. The a* imager will be washed off with buffer C, and then the sample will be imaged with b* imager. The wash and image steps can be repeated sequentially for multiplexing.

Doubling the resolution of a confocal spinning-disk microscope using image scanning microscopy

Fluorescence microscopy has become an indispensable tool for cell biology. Recently, super-resolution methods have been developed to overcome the diffraction limit of light and have shown living cells in unprecedented detail. Often, these methods come at a high cost and with complexity in terms of instrumentation and sample preparation, thus calling for the development of low-cost, more accessible methods. We previously developed image scanning microscopy (ISM), which uses structured illumination to double the resolution and quadruple the contrast of a confocal microscope. Implementing this technique into a confocal spinning-disk (CSD) microscope allows recording ISM images with up to ~1 frame per second, making it ideal for imaging dynamic biological processes. Here we present a step-by-step protocol describing how to convert any existing commercial CSD microscope into a CSD-ISM, with only moderate changes to the hardware and at low cost. Operation of the CSD-ISM is realized with a field programmable gate array using the software environment Micro-Manager, a popular open-source platform for microscopy. The provided software ( https://projects.gwdg.de/projects/csdism-2020 ) takes care of all algorithmic complexities and numerical workload of the CSD-ISM, including hardware synchronization and image reconstruction. The hardware modifications described here result in a theoretical maximum increase in resolution of √2 ≈ 1.41, which can be further improved by deconvolution to obtain a theoretical maximum twofold increase. An existing CSD setup can be upgraded in ~3 d by anyone with basic knowledge in optics, electronics and microscopy software.

(Invited) Enhancement of Plasmon-Induced Charge Separation through Plasmon Coupling

Plasmon-induced charge separation (PICS)1,2 involves electron transfer from plasmonic noble metal nanoparticles or compound nanoparticles to an n-type semiconductor such as TiO2. Oxidation reactions involved in PICS are based on a charge accumulation mechanism (Figure a) or a hole ejection mechanism (Figure b).3 The latter enables nanoscale local oxidation at relatively positive potentials.4-7 This can be applied to photoinduced nanofabrication beyond the diffraction limit of light. For instance, chiral plasmonic nanostructures can be prepared by PICS under right or left circularly polarized light (Figure c).8,9 Some other applications of the plasmonic hole ejection will also be mentioned. Enhancement of PICS with hole ejection through plasmon coupling10 and its application to photocatalysis will also be described.References Y. Tian and T. Tatsuma, J. Am. Chem. Soc., 127, 7632 (2005).T. Tatsuma, H. Nishi, and T. Ishida, Chem. Sci., 8, 3325 (2017) [review].T. Tatsuma and H. Nishi, Nanoscale Horiz., 5, 597-606 (2020) [review].E. Kazuma, N. Sakai, and T. Tatsuma, Chem. Commun., 47, 5777 (2011).I. Tanabe and T. Tatsuma, Nano Lett., 12, 5418 (2012).K. Saito, I. Tanabe, and T. Tatsuma, J. Phys. Chem. Lett., 7, 4363 (2016).H. Nishi, M. Sakamoto, and T. Tatsuma, Chem. Commun., 54, 11741 (2018).K. Saito and T. Tatsuma, Nano Lett., 18, 3209 (2018).K. Morisawa, T. Ishida, and T. Tatsuma, ACS Nano, 14, 3603 (2020).T. Ishida and T. Tatsuma, J. Phys. Chem. C, 122, 26153 (2018). Figure 1

Prospects and limitations of expansion microscopy in chromatin ultrastructure determination

Expansion microscopy (ExM) is a method to magnify physically a specimen with preserved ultrastructure. It has the potential to explore structural features beyond the diffraction limit of light. The procedure has been successfully used for different animal species, from isolated macromolecular complexes through cells to tissue slices. Expansion of plant-derived samples is still at the beginning, and little is known, whether the chromatin ultrastructure becomes altered by physical expansion. In this study, we expanded isolated barley nuclei and compared whether ExM can provide a structural view of chromatin comparable with super-resolution microscopy. Different fixation and denaturation/digestion conditions were tested to maintain the chromatin ultrastructure. We achieved up to ~4.2-times physically expanded nuclei corresponding to a maximal resolution of ~50–60 nm when imaged by wild-field (WF) microscopy. By applying structured illumination microscopy (SIM, super-resolution) doubling the WF resolution, the chromatin structures were observed at a resolution of ~25–35 nm. WF microscopy showed a preserved nucleus shape and nucleoli. Moreover, we were able to detect chromatin domains, invisible in unexpanded nuclei. However, by applying SIM, we observed that the preservation of the chromatin ultrastructure after the expansion was not complete and that the majority of the tested conditions failed to keep the ultrastructure. Nevertheless, using expanded nuclei, we localized successfully centromere repeats by fluorescence in situ hybridization (FISH) and the centromere-specific histone H3 variant CENH3 by indirect immunolabelling. However, although these repeats and proteins were localized at the correct position within the nuclei (indicating a Rabl orientation), their ultrastructural arrangement was impaired.

Optical Fiber Technologies for Nanomanipulation and Biodetection: A Review

Optical manipulation and detection of nanoscale biospecimen such as organic nanoparticles, biomolecules, bacterial viruses, and subcellular nanostructures, is crucial in numerous biomedical and biological applications. Traditional lens-based free-space techniques for optical manipulation and detection are limited by their bulky systems and the inherent diffraction limit of light. Micro/nano optical fibers are promising candidates to overcome these issues because of their compact structure, flexibility, high sensitivity, and sub-diffraction-limit confinement. In this review, we focused on recent advances in nanoscale manipulation and biological detection using optical fibers, ranging from the fundamentals to applications for biological exploration, such as nanoparticle delivery and detection, single-molecule trapping and sensing, and single-cell manipulation and analysis. Different kinds of optical fibers were discussed in this review, including tapered fibers, plasmonic fibers, microlens-based fibers, nanofibers, and hollow fibers. We aim for this review to highlight current trends and future direction for applications of optical fibers for nanomanipulation and biodetection.

Methods to fabricate and recycle plasmonic probes for ultrahigh vacuum scanning tunneling microscopy‐based tip‐enhanced Raman spectroscopy

AbstractScanning tunneling microscopy‐based tip‐enhanced Raman spectroscopy (TERS) is a powerful analytical technique for surface characterization, providing both topological and chemical information with sub‐nm spatial resolution, well below the diffraction limit of light. In order to take advantage of plasmonic activity, it is necessary to use silver (Ag) probes due to their plasmonic range in the visible region. However, the Ag probe fabrication process remains challenging and is not yet standardized in practice, leading to inconsistent enhancements even for two similar types of tips prepared consecutively. In this work, we demonstrate an alternative way to reuse and recycle a plasmonic tip for distinct molecular systems inside an ultrahigh vacuum (UHV). We provide evidence of the ability to recycle tips without compromising the TERS experimental results. A long‐term preservation (>2 months) of plasmonically active probes inside UHV is demonstrated.

Lasing at the nanoscale: coherent emission of surface plasmons by an electrically driven nanolaser

Abstract Plasmonics offers a unique opportunity to break the diffraction limit of light and bring photonic devices to the nanoscale. As the most prominent example, an integrated nanolaser is a key to truly nanoscale photonic circuits required for optical communication, sensing applications and high-density data storage. Here, we develop a concept of an electrically driven subwavelength surface-plasmon-polariton nanolaser, which is based on a novel amplification scheme, with all linear dimensions smaller than the operational free-space wavelength λ and a mode volume of under λ 3/30. The proposed pumping approach is based on a double-heterostructure tunneling Schottky barrier diode and gives the possibility to reduce the physical size of the device and ensure in-plane emission so that the nanolaser output can be naturally coupled to a plasmonic or nanophotonic waveguide circuitry. With the high energy efficiency (8% at 300 K and 37% at 150 K), the output power of up to 100 μW and the ability to operate at room temperature, the proposed surface plasmon polariton nanolaser opens up new avenues in diverse application areas, ranging from ultrawideband optical communication on a chip to low-power nonlinear photonics, coherent nanospectroscopy, and single-molecule biosensing.

Near-field Terahertz Sensing of HeLa Cells and Pseudomonas Based on Monolithic Integrated Metamaterials with a Spintronic Terahertz Emitter.

Label-free biosensors operating within the terahertz (THz) spectra have helped to unlock a myriad of potential THz applications, ranging from biomaterial detection to point-of-care diagnostics. However, the THz wave diffraction limit and the lack of emitter-integrated THz biosensors hinder the proliferation of high-resolution near-field label-free THz biosensing. Here, a monolithic THz emission biosensor (TEB) is achieved for the first time by integrating asymmetric double-split ring resonator metamaterials with a ferromagnetic heterojunction spintronic THz emitter. This device exhibits an electromagnetically induced transparency window with a resonance frequency of 1.02 THz and a spintronic THz radiation source with a bandwidth of 900 GHz, which are integrated on a fused silica substrate monolithically for the first time. It was observed that the resonance frequency experienced a red-shift behavior with increasing concentration of HeLa cells and Pseudomonas because of the strong interaction between the spintronic THz radiation and the biological samples on the metamaterials. The spatial frequency red-shift resolution is ∼0.01 THz with a Pseudomonas concentration increase from ∼0.5 × 104 to ∼1 × 104/mL. The monolithic THz biosensor is also sensitive to the sample concentration distribution with a 15.68 sensitivity under a spatial resolution of 500 μm, which is determined by the infrared pump light diffraction limit. This TEB shows great potential for high-resolution near-field biosensing applications of trace biological samples.

Tunable Plasmonic Quantum Light Source with Silver Nanoclusters on a Silver Surface

Scanning tunneling luminescence (STL) can be used to investigate the optical properties of nanostructures with high spatial resolution beyond the diffraction limit of light. To get appropriate STL spectra, one needs to modify the tip repeatedly. However, such irreversible tip modification often leads to very unstable tips. Here, by using a scanning tunneling microscope (STM) tip, we demonstrate that STL spectra are tunable via silver nanocluster arrays fabricated directly on a silver surface. The silver nanoclusters are created by transferring silver atoms from the silver tip to the silver surface under STM. We found that the STL spectra were enhanced (suppressed) at higher (lower) energy on the clusters and that they showed opposite behaviors between the nanoclusters. Without relying on the irreversible tip shape modification, our findings indicate that we can tune the STL spectra simply by moving the STM tip over the nanoclusters. Our method can be used to provide a tunable light source for systematic nano-optical experiments and for nanoscale optical devices.

Hybrid Electro-Optical Pumping of Active Plasmonic Nanostructures.

Surface plasmon polaritons (SPPs) offer a unique opportunity to overcome the diffraction limit of light. However, this opportunity comes at the cost of the strong absorption of the SPP field in a metal, which unavoidably limits the SPP propagation length to a few tens of micrometers in nanostructures with deep-subwavelength mode confinement. The only possibility to avoid the propagation losses is to compensate for them by optical gain in the adjacent active medium. Different approaches for surface plasmon amplification by stimulated emission of radiation have been proposed based on either optical or electrical pumping. However, each has its own disadvantages caused by the selected type of pumping scheme. Here, we study, for the first time, hybrid electro-optical pumping of active plasmonic waveguide structures, and by using comprehensive self-consistent numerical simulations, demonstrate that this hybrid approach can outperform both pure electrical pumping and pure optical pumping. The SPP modal gain is higher than under pure optical pumping, while one can precisely and locally adjust it by tuning the electric current, which allows the reduction of amplification noise and provides additional functionalities. We believe that our findings lay a solid foundation for the development of a new generation of active plasmonic devices and stimulate further research in this area.