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arXiv:1702.04319 · Optica

Superresolution via structured illumination quantum correlation microscopy

Anton Classen, Joachim von Zanthier, Marlan O. Scully, G. S. Agarwal

Published May 25, 2017• 83 citations
arXivHTMLPDF

Abstract

We propose to use intensity correlation microscopy in combination with structured illumination to image quantum emitters that exhibit antibunching with a spatial resolution reaching far beyond the Rayleigh limit. Combining intensity measurements and intensity auto correlations up to order $m$ creates an effective PSF with FWHM shrunk by the factor $\sqrt{m}$. Structured Illumination microscopy on the other hand introduces a resolution improvement of factor 2 by use of the principle of moiré fringes. Here, we show that for linear low-intensity excitation and linear optical detection the simultaneous use of both techniques leads to an in theory unlimited resolution power with the improvement scaling favorably as $m + \sqrt{m}$ in dependence of the correlation order $m$. Hence, yielding this technique to be of interest in microscopy for imaging a variety of samples including biological ones. We present the underlying theory and simulations demonstrating the highly increased spatial superresolution, and point out requirements for an experimental implementation.

DOI
10.1364/optica.4.000580

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We propose to use intensity correlation microscopy in combination with structured illumination to image quantum emitters that exhibit antibunching with a spatial resolution reaching far beyond the Rayleigh limit. Combining intensity measurements and intensity auto correlations up to order mmm creates an effective PSF with FWHM shrunk by the factor m\sqrt{m}m​. Structured Illumination microscopy on the other hand introduces a resolution improvement of factor 2 by use of the principle of moiré fringes. Here, we show that for linear low-intensity excitation and linear optical detection the simultaneous use of both techniques leads to an in theory unlimited resolution power with the improvement scaling favorably as m+mm + \sqrt{m}m+m​ in dependence of the correlation order mmm. Hence, yielding this technique to be of interest in microscopy for imaging a variety of samples including biological ones. We present the underlying theory and simulations demonstrating the highly increased spatial superresolution, and point out requirements for an experimental implementation.
We propose to use intensity correlation microscopy in combination with structured illumination to image quantum emitters that exhibit antibunching with a spatial resolution reaching far into the sub-classical regime. Combining intensity measurements and intensity auto correlations up to order m creates an effective PSF with FWHM shrunk by the factor p m. Structured Illumination microscopy on the other hand introduces a resolution improvement of factor 2 by use of the principle of moiré fringes. Here, we show that for linear low-intensity excitation and linear optical detection the simultaneous use of both techniques leads to an in theory unlimited resolution power with the improvement scaling favorably as m+sqrt m in dependence of the correlation order m. Hence, yielding this technique to be of the utmost interest for biological imaging. We present the underlying theory and simulations demonstrating the highly increased spatial superresolution, and point out requirements for an experimental implementation.
Intensity correlation microscopy (ICM), which is prominently known through antibunching microscopy or super-resolution optical fluctuation imaging (SOFI), provides super-resolution through a correlation analysis of antibunching of independent quantum emitters or temporal fluctuations of blinking fluorophores. For correlation order m the PSF in the signal is effectively taken to the mth power, and is thus directly shrunk by the factor m. Combined with deconvolution, a close to linear resolution improvement of factor m can be obtained. Yet, analysis of high correlation orders is challenging, which limits the achievable resolutions. Here we propose to use three dimensional structured illumination along with mth-order correlation analysis to obtain an enhanced scaling of up to m + m = 2m. Including the stokes shift or plasmonic sub-wavelength illumination enhancements beyond 2m can be achieved. Hence, resolutions far below the diffraction limit in full 3D imaging and with already low correlation orders, can potentially be achieved. Since ICM operates in the linear regime our approach may be particularly promising for enhancing the resolution in biological imaging at low illumination levels.
Far-field optical microscopy beyond the Abbe diffraction limit, making use of nonlinear excitation (e.g. STED), or temporal fluctuations in fluorescence (PALM, STORM, SOFI) is already a reality. In contrast, overcoming the diffraction limit using non-classical properties of light is very difficult to achieve due to the fragility of quantum states of light. Here, we experimentally demonstrate superresolution microscopy based on quantum properties of light naturally emitted by fluorophores used as markers in fluorescence microscopy. Our approach is based on photon antibunching, the tendency of fluorophores to emit photons one by one rather than in bursts. Although a distinctively quantum phenomenon, antibunching is readily observed in most common fluorophores even at room temperature. This nonclassical resource can be utilized directly to enhance the imaging resolution, since the non-classical far-field intensity correlations induced by antibunching carry high spatial frequency information on the spatial distribution of emitters. Detecting photon statistics simultaneously in the entire field of view, we were able to detect non-classical correlations of the second and third order, and reconstructed images with resolution significantly beyond the diffraction limit. Alternatively, we demonstrate the utilization of antibunching for augmenting the capabilities of localization-based superresolution imaging in the presence of multiple emitters, using a novel detector comprised of an array of single photon detectors connected to a densely packed fiber bundle. These features allow us to enhance the spatial and temporal resolution with which multiple emitters can be imaged compared with other techniques that rely on CCD cameras.
Reaching high-resolution imaging of delicate samples at a low-intensity level is a major challenge in microscopy. Here, we present and experimentally implement an advanced quantum super-resolution imaging technique based on photon statistics measurement. Our reconstruction algorithm adapts to any kind of non-Poissonian emitters, outperforming the corresponding classical SOFI method, in particular in low-light conditions. It offers sub-diffraction resolution improvement that scales with the j , where j is the highest-order central moments of the photocounts. More remarkably, we show that in combination with structured illumination, an improvement of j + j can be reached, providing a promising avenue for non-invasive super-resolution microscopy.
The resolution of optical imaging devices is ultimately limited by the diffraction of light. To circumvent this limit, modern superresolution microscopy techniques employ active interaction with the object by exploiting its optical nonlinearities, nonclassical properties of the illumination beam, or near field probing. Thus, they are not applicable whenever such interaction is not possible, for example, in astronomy or noninvasive biological imaging. Far field, linear optical superresolution techniques based on passive analysis of light coming from the object would cover these gaps. In this Letter, we present the first proof-of-principle demonstration of such a technique for 2D imaging. It works by accessing information about spatial correlations of the image optical field and, hence, about the object itself via measuring projections onto Hermite-Gaussian transverse spatial modes. With a basis of 21 spatial modes in both transverse dimensions, we perform two-dimensional imaging with twofold resolution enhancement beyond the diffraction limit.
The resolution of imaging devices is ultimately limited by the diffraction of light. This limit can be circumvented by exploiting near-field phenomena, non-linearities of the sample or specific illumination schemes, which led to the recent explosion of optical super-resolution techniques. However, it would be desirable to reach the nanoscale in the most general way possible, with far-field linear imaging of uniformly illuminated samples. In the last few years, the answer to that came with the field of quantum-inspired super-resolution (QISR), where quantum metrological techniques were used to find novel measurement schemes that, beyond the conventional direct imaging of light, would achieve higher precisions. Interestingly, these ideas would always in some way or another involve transverse spatial modes of light. This thesis presents our work on the subject, with novel theoretical and experimental results. Firstly, we develop the traditional theory of QISR, with has mostly focused on either the estimation of separation of two point sources or on geometric moments of samples. Then, we introduce our own results on optical imaging of general distributions of point sources, in a step to take QISR from toy examples to real imaging scenarios. Secondly, we apply all the concepts studied on a experimental, proof-of-principle implementation of a QISR scheme dubbed Hermite-Gaussian Microscopy (HGM), which uses heterodyne detection with several Hermite-Gaussian modes as local oscillator in order to reconstruct the object sample and achieve super-resolution. We report the techniques necessary for the manipulation of spatial modes of light, as well as our results, where we demonstrated 2D imaging with twofold resolution enhancement beyond the diffraction limit.