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Register a new user6 nm super-resolution optical transmission and scattering spectroscopic imaging of carbon nanotubes using a nanometer-scale white light source
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Optical hyperspectral imaging based on absorption and scattering of photons at the visible and adjacent frequencies denotes one of the most informative and inclusive characterization methods in material research. Unfortunately, restricted by the diffraction limit of light, it is unable to resolve the nanoscale inhomogeneity in light-matter interactions, which is diagnostic of the local modulation in material structure and properties. Moreover, many nanomaterials have highly anisotropic optical properties that are outstandingly appealing yet hard to characterize through conventional optical methods. Therefore, there has been a pressing demand in the diverse fields including electronics, photonics, physics, and materials science to extend the optical hyperspectral imaging into the nanometer length scale. In this work, we report a super-resolution hyperspectral imaging technique that simultaneously measures optical absorption and scattering spectra with the illumination from a tungsten-halogen lamp. We demonstrated sub-5 nm spatial resolution in both visible and near-infrared wavelengths (415 to 980 nm) for the hyperspectral imaging of strained single-walled carbon nanotubes (SWNT) and reconstructed true-color images to reveal the longitudinal and transverse optical transition-induced light absorption and scattering in the SWNTs. This is the first time transverse optical absorption in SWNTs were clearly observed experimentally. The new technique provides rich near-field spectroscopic information that had made it possible to analyze the spatial modulation of band-structure along a single SWNT induced through strain engineering.
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Highly efficient exciton-exciton annihilation process unique to one-dimensional systems is utilized for super-resolution imaging of air-suspended carbon nanotubes. Through the comparison of fluorescence signals in linear and sublinear regimes at different excitation powers, we extract the efficiency of the annihilation processes using conventional confocal microscopy. Spatial images of the annihilation rate of the excitons have resolution beyond the diffraction limit. We investigate excitation power dependence of the annihilation processes by experiment and Monte Carlo simulation, and the resolution improvement of the annihilation images can be quantitatively explained by the superlinearity of the annihilation process. We have also developed another method in which the cubic dependence of the annihilation rate on exciton density is utilized to achieve further sharpening of single nanotube images.
Super-resolution imaging with advanced optical systems has been revolutionizing technical analysis in various fields from biological to physical sciences. However, many objects are hidden by strongly scattering media such as rough wall corners or biological tissues that scramble light paths, create speckle patterns and hinder objects visualization, let alone super-resolution imaging. Here, we realize a method to do non-invasive super-resolution imaging through scattering media based on stochastic optical scattering localization imaging (SOSLI) technique. Simply by capturing multiple speckle patterns of photo-switchable emitters in our demonstration, the stochastic approach utilizes the speckle correlation properties of scattering media to retrieve an image with more than five-fold resolution enhancement compared to the diffraction limit, while posing no fundamental limit in achieving higher spatial resolution. More importantly, we demonstrate our SOSLI to do non-invasive super-resolution imaging through not only optical diffusers, i.e. static scattering media, but also biological tissues, i.e. dynamic scattering media with decorrelation of up to 80%. Our approach paves the way to non-invasively visualize various samples behind scattering media at unprecedented levels of detail.
Atomic resolution imaging in transmission electron microscopy (TEM) and scanning TEM (STEM) of light elements in electron-transparent materials has long been a challenge. Biomolecular materials, for example, are rapidly altered when illuminated with electrons. These issues have driven the development of TEM and STEM techniques that enable the structural analysis of electron beam-sensitive and weakly scattering nano-materials. Here, we demonstrate such a technique, STEM holography, capable of absolute phase and amplitude object wave measurement with respect to a vacuum reference wave. We use an amplitude-dividing nanofabricated grating to prepare multiple spatially separated electron diffraction probe beams focused at the sample plane, such that one beam transmits through the specimen while the others pass through vacuum. We raster-scan the diffracted probes over the region of interest. We configure the post specimen imaging system of the microscope to diffraction mode, overlapping the probes to form an interference pattern at the detector. Using a fast-readout, direct electron detector, we record and analyze the interference fringes at each position in a 2D raster scan to reconstruct the complex transfer function of the specimen, t(x). We apply this technique to image a standard target specimen consisting of gold nanoparticles on a thin amorphous carbon substrate, and demonstrate 2.4 angstrom resolution phase images. We find that STEM holography offers higher phase-contrast of the amorphous material while maintaining Au atomic lattice resolution when compared with high angle annular dark field STEM.
Extending super-resolution imaging techniques to objects hidden in strongly scattering media potentially revolutionize the technical analysis for much broader categories of samples, such as biological tissues. The main challenge is the medias inhomogeneous structures which scramble the light path and create noise-like speckle patterns, hindering the objects visualization even at a low-resolution level. Here, we propose a computational method relying on the objects spatial and temporal fluctuation to visualize nanoscale objects through scattering media non-invasively. The fluctuating object can be achieved by random speckle illumination, illuminating through dynamic scattering media, or flickering emitters. The optical memory effect allows us to derive the object at diffraction limit resolution and estimate the point spreading function (PSF). Multiple images of the fluctuating object are obtained by deconvolution, then super-resolution images are achieved by computing the high order cumulants. Non-linearity of high order cumulant significantly suppresses the noise and artifacts in the resulting images and enhances the resolution by a factor of $sqrt{N}$, where $N$ is the cumulant order. Our non-invasive super-resolution speckle fluctuation imaging (NISFFI) presents a nanoscopy technique with very simple hardware to visualize samples behind scattering media.
Chip-based Evanescent Light Scattering (cELS) utilizes the multiple modes of a high-index contrast optical waveguide to provide a near-field illumination for unlabeled samples. The scattered light off the sample is engineered to have random phase differences within the integration time of the camera to mitigate the coherent speckle noise, thus enabling label-free superior-contrast imaging of weakly scattering nanosized specimens such as extra-cellular vesicles (EVs) and liposomes, dynamics of living HeLa cells etc. The article explains and validates experimentally the physics behind cELS, by demonstrating a wide highly multi-moded straight waveguide as a partially coherent light source. Next, to circumvent the diffraction-limit in cELS, intensity-fluctuation based algorithms are employed with spatially incoherent light engineered via multiple-arms waveguide chip. The proof-of-concept results are demonstrated on 100 nm polystyrene beads. We believe cELS will further propel the nascent field of label-free super-resolution microscopy finding applications in cell biology.
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