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234 records · Page 13

High-luminosity meV-resolution single-shot hard X-ray spectrograph for cavity-based X-ray free-electron lasers

Cavity-based X-ray free-electron lasers (CBXFELs) represent a possible realization of fully coherent hard X-ray sources having high spectral brilliance along with a narrow spectral bandwidth of ∼1–50 meV, a high repetition pulse rate of ∼1 MHz, and good stability. A diagnostic tool is required to measure CBXFEL spectra with meV resolution and high luminosity on a shot-to-shot basis. We have designed a high-luminosity single-shot hard X-ray spectrograph that images 9.831 keV X-rays in a ∼200 meV spectral window with a spectral resolution of a few meV. The spectrograph is designed around angular dispersion of X-rays in Bragg diffraction from crystals. It operates close to design specifications, exhibiting a linear dispersion rate of ∼1.4 µm meV −1 and a ∼200 meV window of high-fidelity spectral imaging. The experimentally demonstrated spectral resolution is ∼20 meV; this resolution is twice as low as expected from theory primarily because the spectrograph is highly sensitive to crystal angular instabilities. The experiment was performed at the bending magnet X-ray optics testing beamline 1-BM at the Advanced Photon Source.

Bragg diffraction↗

The Future of Exoplanet Direct Detection

Diffraction fundamentally limits our ability to image and characterize exoplanets. Currant and planned coronagraphic searches for exoplanets are making incredible strides but are fundamentally limited by the inner working angle of a few λ/D. Some crucial topics, such as demographics of exoplanets within the first 50 Myr and the infrared characterization of terrestrial planets, are beyond the reach of the single aperture angular resolution for the foreseeable future. Interferometry offers some advantages in exoplanet detection and characterization and we explore in this white paper some of the potential scientific breakthroughs possible. We demonstrate here that investments in "exoplanet interferometry" could open up new possibilities for speckle suppression through spatial coherence, a giant boost in astrometric precision for determining exoplanet orbits, ability to take a census of young giant exoplanets (clusters <50 Myr age), and an unrivaled potential for infrared nulling from space to detect terrestrial planets and search for atmospheric biomarkers. All signs point to an exciting future for exoplanets and interferometers, albeit a promise that will take decades to fulfill.

John Monnier↗

Holographic Optical Data Storage

Although the basic idea may be traced back to the earlier X-ray diffraction studies of Sir W. L. Bragg, the holographic method as we know it was invented by D. Gabor in 1948 as a two-step lensless imaging technique to enhance the resolution of electron microscopy, for which he received the 1971 Nobel Prize in physics. The distinctive feature of holography is the recording of the object phase variations that carry the depth information, which is lost in conventional photography where only the intensity (= squared amplitude) distribution of an object is captured. Since all photosensitive media necessarily respond to the intensity incident upon them, an ingenious way had to be found to convert object phase into intensity variations, and Gabor achieved this by introducing a coherent reference wave along with the object wave during exposure. Gabor's in-line recording scheme, however, required the object in question to be largely transmissive, and could provide only marginal image quality due to unwanted terms simultaneously reconstructed along with the desired wavefront. Further handicapped by the lack of a strong coherent light source, optical holography thus seemed fated to remain just another scientific curiosity, until the field was revolutionized in the early 1960s by some major breakthroughs: the proposition and demonstration of the laser principle, the introduction of off-axis holography, and the invention of volume holography. Consequently, the remainder of that decade saw an exponential growth in research on theory, practice, and applications of holography. Today, holography not only boasts a wide variety of scientific and technical applications (e.g., holographic interferometry for strain, vibration, and flow analysis, microscopy and high-resolution imagery, imaging through distorting media, optical interconnects, holographic optical elements, optical neural networks, three-dimensional displays, data storage, etc.), but has become a prominent am advertising, and security medium as well. The evolution of holographic optical memories has followed a path not altogether different from holography itself, with several cycles of alternating interest over the past four decades. P. J. van Heerden is widely credited for being the first to elucidate the principles behind holographic data storage in a 1963 paper, predicting bit storage densities on the order of 1/lambda(sup 3) with source wavelength lambda - a fantastic capacity of nearly 1 TB/cu cm for visible light! The science and engineering of such a storage paradigm was heavily pursued thereafter, resulting in many novel hologram multiplexing techniques for dense data storage, as well as important advances in holographic recording materials. Ultimately, however, the lack of such enabling technologies as compact laser sources and high performance optical data I/O devices dampened the hopes for the development of a commercial product. After a period of relative dormancy, successful applications of holography in other arenas sparked a renewed interest in holographic data storage in the late 1980s and the early 1990s. Currently, with most of the critical optoelectronic device technologies in place and the quest for an ideal holographic recording medium intensified, holography is once again considered as one of several future data storage paradigms that may answer our constantly growing need for higher-capacity and faster-access memories.

Timucin, Dogan A.↗

Attosecond light science and its application for probing quantum materials

In this paper, we review the development and application of coherent short wavelength light sources implemented using the high harmonic generation (HHG) process. The physics underlying HHG brought quantum physics into the domain of attosecond time-scales for the first time. Here, the observation and manipulation of electron dynamics on such short time-scales—a capability not conceived—of just a few decades ago—is becoming both more-and-more sophisticated and useful as a route to achieve exquisite control over short wavelength light. New experimental techniques are enabling HHG light sources to provide new insights into fundamental quantum interactions in materials, making it possible for the first time to capture the fastest charge, spin, photon and phonon interactions and to achieve diffraction-limited imaging at short wavelengths.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Atomic-Scale Structure and Non-Stoichiometry of Meteoritic Hibonite: A Transmission Electron Microscope Study

Hibonite (CaAl_12O_19) is a common refractory mineral in Ca-Al-rich inclusions (CAIs) in primitive meteorites. Transmission electron microscope (TEM) studies have identified enigmatic planar defects in different occurrences of hibonite in the Allende meteorite that give rise to strong streaking along c* in electron diffraction patterns. Atomic resolution high-angle annular dark-field (HAADF) imaging and energy-dispersive X-ray (EDX) analyses were used to determine the nature and origin of these planar features. HAADF images of hibonite grains reveal lamellar intergrowths of common 1.6 nm spacing, and less commonly 2.0 and 2.5 nm spacings, interspersed in stoichiometric hibonite showing 1.1 nm (002) spacing. Stoichiometric hibonite consists of alternating Ca-containing (“R”) and spinel-structured (“S”) blocks stacked in a sequence RS. In contrast, the 1.6 nm layers result from a doubled S block such that the stacking sequence is RSS, while in the widest defect observed, the stacking sequence is RSSSS. These intergrowths are epitaxial and have coherent, low-strain boundaries with the host hibonite Meteoritic hibonite shows common Ti and Mg substitution for Al in its structure. Atomic-resolution EDX maps of hibonite grains in the Allende CAI confirm the preferred site occupancy of Mg on tetragonal M3 sites in S blocks and of Ti on trigonal bipyramidal M2 and octahedral M4 sites in R blocks. Mg is highly concentrated, but Ti is absent in the planar defects where wider S blocks show Al-rich compositions compared to stoichiometric MgAl_2O_4 spinel. Therefore, Mg likely played the major role in the formation and metastability of planar defects in hibonite. Electron energy loss spectroscopy data from the Ti L_2,3 edge show the presence of mixed Ti oxidation states with ~ 15–20% of Ti as Ti^(3+) in hibonite, suggesting a direct substitution of Ti^(3+) ↔ Al^(3+) in hibonite. The remaining ~ 80–85% of Ti is present as Ti^(4+) and corresponding EDX analyses are consistent with the well-known coupled substitution 2Al^(3+) ↔ Ti^(4+) + Mg^(2+) being the major mechanism for Ti and Mg substitution in hibonite. The formation of planar defects in hibonite occurred during high-temperature nebular condensation or melting/crystallization processes. The occurrence of non-stoichiometric hibonite in the Allende CAI deviates from the mineral formation sequence predicted from equilibrium condensation models. Overall, our atomic resolution TEM observations signify non-equilibrium, kinetic-controlled crystal growth during the high-temperature formation of refractory solids in the early solar nebula.

hibonite↗

Unusual Breathing Behavior of Optically Excited Barium Titanate Nanocrystals

Coherent X-ray diffraction patterns were recorded by using an X-ray free-electron laser to illuminate barium titanate nanocrystals as a function of time delay after laser excitation. Rather than seeing any significant thermal expansion effects, the diffraction peaks were found to move perpendicular to the momentum transfer direction. This suggests a laser driven rotation of the crystal lattice, which is delayed by the aggregated state of the crystals. Internal deformations associated with crystal contacts were also observed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Rapid 3D nanoscale coherent imaging via physics-aware deep learning

Phase retrieval, the problem of recovering lost phase information from measured intensity alone, is an inverse problem that is widely faced in various imaging modalities ranging from astronomy to nanoscale imaging. The current process of phase recovery is iterative in nature. As a result, the image formation is time consuming and computationally expensive, precluding real-time imaging. Here, we use 3D nanoscale X-ray imaging as a representative example to develop a deep learning model to address this phase retrieval problem. We introduce 3D-CDI-NN, a deep convolutional neural network and differential programing framework trained to predict 3D structure and strain, solely from input 3D X-ray coherent scattering data. Our networks are designed to be “physics-aware” in multiple aspects; in that the physics of the X-ray scattering process is explicitly enforced in the training of the network, and the training data are drawn from atomistic simulations that are representative of the physics of the material. We further refine the neural network prediction through a physics-based optimization procedure to enable maximum accuracy at lowest computational cost. 3D-CDI-NN can invert a 3D coherent diffraction pattern to real-space structure and strain hundreds of times faster than traditional iterative phase retrieval methods. Our integrated machine learning and differential programing solution to the phase retrieval problem is broadly applicable across inverse problems in other application areas.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

NASA Tech Briefs, May 2009

Topics covered include: Valve-"Health"-Monitoring System; Microstrip Antenna for Remote Sensing of Soil Moisture and Sea Surface Salinity; Biomedical Wireless Ambulatory Crew Monitor; Wireless Avionics Packet to Support Fault Tolerance for Flight Applications; Aerobot Autonomy Architecture; Submillimeter Confocal Imaging Active Module; Traveling-Wave Maser for 32 GHz; System Synchronizes Recordings from Separated Video Cameras; Piecewise-Planar Parabolic Reflectarray Antenna; Reducing Interference in ATC Voice Communication; EOS MLS Level 1B Data Processing, Version 2.2; Auto-Generated Semantic Processing Services; Geospatial Authentication; Maneuver Automation Software; Event Driven Messaging with Role-Based Subscriptions; Estimating Relative Positions of Outer-Space Structures; Fabricating PFPE Membranes for Capillary Electrophoresis; Linear Actuator Has Long Stroke and High Resolution; Installing a Test Tap on a Metal Battery Case; Fabricating PFPE Membranes for Microfluidic Valves and Pumps; Room-Temperature-Cured Copolymers for Lithium Battery Gel Electrolytes; Catalysts for Efficient Production of Carbon Nanotubes; Amorphous Silk Fibroin Membranes for Separation of CO2; "Zero-Mass" Noninvasive Pressure Transducers; Radial-Electric-Field Piezoelectric Diaphragm Pumps; Ejector-Enhanced, Pulsed, Pressure-Gain Combustor; Suppressing Ghost Diffraction in E-Beam-Written Gratings; Target-Tracking Camera for a Metrology System; Polarimetric Imaging using Two Photoelastic Modulators; Miniature Wide-Angle Lens for Small-Pixel Electronic Camera; Modal Filters for Infrared Interferometry; Mo(3)Sb(7-x)Te(x) for Thermoelectric Power Generation; Two-Dimensional Quantum Model of a Nanotransistor; Scanning Miniature Microscopes without Lenses; Manipulating Neutral Atoms in Chip-Based Magnetic Traps; Expansion Compression Contacts for Thermoelectric Legs; Processing Electromyographic Signals to Recognize Words; Physical Principle for Generation of Randomness; DSN Beowulf Cluster-Based VLBI Correlator; Hybrid NN/SVM Computational System for Optimizing Designs; Criteria for Modeling in LES of Multicomponent Fuel Flow; Computerized Machine for Cutting Space Shuttle Thermal Tiles; Orbiting Depot and Reusable Lander for Lunar Transportation; FPGA-Based Networked Phasemeter for a Heterodyne Interferometer; Aquarius Digital Processing Unit; Three-Dimensional Optical Coherence Tomography; Benchtop Antigen Detection Technique using Nanofiltration and Fluorescent Dyes; Isolation of Precursor Cells from Waste Solid Fat Tissue; Identification of Bacteria and Determination of Biological Indicators; Further Development of Scaffolds for Regeneration of Nerves; Chemically Assisted Photocatalytic Oxidation System; Use of Atomic Oxygen for Increased Water Contact Angles of Various Polymers for Biomedical Applications; Crashworthy Seats Would Afford Superior Protection; Open-Access, Low-Magnetic-Field MRI System for Lung Research; Microfluidic Mixing Technology for a Universal Health Sensor; Microfluidic Extraction of Biomarkers using Water as Solvent; Microwell Arrays for Studying Many Individual Cells; Droplet-Based Production of Liposomes; and Identifying and Inactivating Bacterial Spores

Source record↗

Multiscale Imaging of Nuclear Deformation at the Electron-Ion Collider

We show within the Color Glass Condensate framework that exclusive vector meson production at high energy is sensitive to the geometric deformation of the target nucleus at multiple length scales. Studying e+U collisions and varying the deformation of the uranium target, we demonstrate that larger deformations result in enhanced incoherent vector meson production cross sections. Further, different multipole deformation parameters affect different regions of transverse momentum transfer. Employing JIMWLK evolution to study the Bjorken-x dependence of our results, we find that the ratio of incoherent to coherent cross sections decreases with decreasing x, largely independently of the quadrupole deformation of the target. Comparing results for the same process using 20 Ne targets with 16 O targets, we find that differences in deformation are clearly visible in the incoherent cross section. These findings show that certain observables at the Electron-Ion Collider are very sensitive to nuclear structure. Consequently, deformations need to be taken into account when interpreting experimental results. More importantly, this also means that |t|-differential diffractive vector meson production could become a powerful tool, enabling the most direct measurements of nuclear structure at different length scales, ranging from nuclear deformation at low |t| to nucleon and subnucleon-size scales at higher |t|.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Soft x-ray high-harmonic generation in an anti-resonant hollow core fiber driven by a 3 μ m ultrafast laser

High-harmonic upconversion driven by a mid-infrared femtosecond laser can generate coherent soft x-ray beams in a tabletop-scale setup. Here, we report on a compact ytterbium-pumped optical parametric chirped pulse amplifier (OPCPA) laser system seeded by an all-fiber front-end and employing periodically poled lithium niobate (PPLN) nonlinear media operated near the pulse fluence limits of current commercially available PPLN crystals. The OPCPA delivers 3 µm wavelength pulses with 775 µJ energy at 1 kHz repetition rate, with transform-limited 120 fs pulse duration, diffraction-limited beam quality, and ultrahigh 0.33% rms energy stability over >18 h. Using this laser, we generate soft x-ray high harmonics (HHG) in argon gas by focusing into a low-loss, high-pressure gas-filled anti-resonant hollow core fiber (ARHCF), generating coherent light at photon energies up to the argon L-edge (250 eV) and carbon K-edge (284 eV), with high beam quality and ∼1% rms energy stability. This work demonstrates soft x-ray HHG in a high-efficiency guided-wave phase matched geometry, overcoming the high losses inherent to mid-IR propagation in unstructured waveguides, or the short interaction lengths of gas cells or jets. The ARHCF can operate in the long term without damage and with the repetition rate, stability, and robustness required for demanding applications in spectromicroscopy and imaging. Finally, we discuss routes for further optimizing the soft x-ray HHG flux by driving He at higher laser intensities using either the signal (1.5 μm) or idler wavelengths (3 μm).

Femtosecond lasers↗

Universal linear intensity transformations using spatially incoherent diffractive processors

Abstract Under spatially coherent light, a diffractive optical network composed of structured surfaces can be designed to perform any arbitrary complex-valued linear transformation between its input and output fields-of-view (FOVs) if the total number ( N ) of optimizable phase-only diffractive features is ≥~2 N i N o , where N i and N o refer to the number of useful pixels at the input and the output FOVs, respectively. Here we report the design of a spatially incoherent diffractive optical processor that can approximate any arbitrary linear transformation in time-averaged intensity between its input and output FOVs. Under spatially incoherent monochromatic light, the spatially varying intensity point spread function ( H ) of a diffractive network, corresponding to a given, arbitrarily-selected linear intensity transformation, can be written as H ( m , n ; m ′, n ′) = | h ( m , n ; m ′, n ′)| 2 , where h is the spatially coherent point spread function of the same diffractive network, and ( m , n ) and ( m ′, n ′) define the coordinates of the output and input FOVs, respectively. Using numerical simulations and deep learning, supervised through examples of input-output profiles, we demonstrate that a spatially incoherent diffractive network can be trained to all-optically perform any arbitrary linear intensity transformation between its input and output if N ≥ ~2 N i N o . We also report the design of spatially incoherent diffractive networks for linear processing of intensity information at multiple illumination wavelengths, operating simultaneously. Finally, we numerically demonstrate a diffractive network design that performs all-optical classification of handwritten digits under spatially incoherent illumination, achieving a test accuracy of >95%. Spatially incoherent diffractive networks will be broadly useful for designing all-optical visual processors that can work under natural light.

36 MATERIALS SCIENCE↗

Extending the Takagi-Taupin equations for x-ray nanobeam Bragg coherent diffraction

We present an approach for simulating x-ray nanobeam Bragg coherent diffraction patterns based on the Takagi-Taupin equations. Compared to conventional methods, the current approach can be universally applied to any weakly strained system including semi-infinite crystals that diffract dynamically. It addresses issues such as the curved wave front and redivergence of the focused incident beam. In conclusion, we show excellent agreement with experimental data for a strained La 0.7 ⁢Sr 0.3⁢ MnO 3 thin film on a SrTiO 3 substrate and a path to extracting physical information using automatic differentiation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Theoretical and experimental analysis of the modulated phase grating X-ray interferometer

X-ray grating interferometry allows for the simultaneous acquisition of attenuation, differential-phase contrast, and dark-field images, resulting from X-ray attenuation, refraction, and small-angle scattering, respectively. The modulated phase grating (MPG) interferometer is a recently developed grating interferometry system capable of generating a directly resolvable interference pattern using a relatively large period grating envelope function that is sampled at a pitch that is small enough that X-ray spatial coherence can be achieved by using a microfocus X-ray source or G0 grating. We present the theory of the MPG interferometry system for a 2-dimensional staggered grating, derived using Fourier optics, and we compare the theoretical predictions with experiments we have performed with a microfocus X-ray system at Pennington Biomedical Research Center, LSU. The theoretical and experimental fringe visibility is evaluated as a function of grating-to-detector distance. Additionally, quantitative experiments are performed with porous carbon and alumina compounds, and the mean normalized dark-field signal is compared with independent porosimetry measurements. Qualitative analysis of attenuation and dark-field images of a dried anchovy are shown.

47 OTHER INSTRUMENTATION↗

Speckle contrast of interfering fluorescence X-rays

With the development of X-ray free-electron lasers (XFELs), producing pulses of femtosecond durations comparable with the coherence times of X-ray fluorescence, it has become possible to observe intensity–intensity correlations due to the interference of emission from independent atoms. This has been used to compare durations of X-ray pulses and to measure the size of a focused X-ray beam, for example. Here it is shown that it is also possible to observe the interference of fluorescence photons through the measurement of the speckle contrast of angle-resolved fluorescence patterns. Speckle contrast is often used as a measure of the degree of coherence of the incident beam or the fluctuations of the illuminated sample as determined from X-ray diffraction patterns formed by elastic scattering, rather than from fluorescence patterns as addressed here. Commonly used approaches to estimate speckle contrast were found to suffer when applied to XFEL-generated fluorescence patterns due to low photon counts and a significant variation of the excitation pulse energy from shot to shot. A new method to reliably estimate speckle contrast under such conditions, using a weighting scheme, is introduced. The method is demonstrated by comparing the speckle contrast of fluorescence observed with pulses of 3 fs to 15 fs duration.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Imaging plasma formation in isolated nanoparticles with ultrafast resonant scattering

We have recorded the diffraction patterns from individual xenon clusters irradiated with intense extreme ultraviolet pulses to investigate the influence of light-induced electronic changes on the scattering response. The clusters were irradiated with short wavelength pulses in the wavelength regime of different 4d inner-shell resonances of neutral and ionic xenon, resulting in distinctly different optical properties from areas in the clusters with lower or higher charge states. The data show the emergence of a transient structure with a spatial extension of tens of nanometers within the otherwise homogeneous sample. Simulations indicate that ionization and nanoplasma formation result in a light-induced outer shell in the cluster with a strongly altered refractive index. The presented resonant scattering approach enables imaging of ultrafast electron dynamics on their natural timescale.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Laser Light Scattering by Shock Waves

Scattering of coherent light as it propagates parallel to a shock wave, formed in front of a bluff cylindrical body placed in a supersonic stream, is studied experimentally and numerically. Two incident optical fields are considered. First, a large diameter collimated beam is allowed to pass through the shock containing flow. The light intensity distribution in the resultant shadowgraph image, measured by a low light CCD camera, shows well-defined fringes upstream and downstream of the shadow cast by the shock. In the second situation, a narrow laser beam is brought to a grazing incidence on the shock and the scattered light, which appears as a diverging sheet from the point of interaction, is visualized and measured on a screen placed normal to the laser path. Experiments are conducted on shocks formed at various free-stream Mach numbers, M, and total pressures, P(sub 0). It is found that the widths of the shock shadows in a shadowgraph image become independent of M and P(sub 0) when plotted against the jump in the refractive index, (Delta)n, created across the shock. The total scattered light measured from the narrow laser beam and shock interaction also follows the same trend. In the numerical part of the study, the shock is assumed to be a 'phase object', which introduces phase difference between the upstream and downstream propagating parts of the light disturbances. For a given shape and (Delta)n of the bow shock the phase and amplitude modulations are first calculated by ray tracing. The wave front is then propagated to the screen using the Fresnet diffraction equation. The calculated intensity distribution, for both of the incident optical fields, shows good agreement with the experimental data.

Panda, J.↗

White-Light Phase-Conjugate Mirrors as Distortion Correctors

White-light phase-conjugate mirrors would be incorporated into some optical systems, according to a proposal, as means of correcting for wavefront distortions caused by imperfections in large optical components. The proposal was given impetus by a recent demonstration that white, incoherent light can be made to undergo phase conjugation, whereas previously, only coherent light was known to undergo phase conjugation. This proposal, which is potentially applicable to almost any optical system, was motivated by a need to correct optical aberrations of the primary mirror of the Hubble Space telescope. It is difficult to fabricate large optical components like the Hubble primary mirror and to ensure the high precision typically required of such components. In most cases, despite best efforts, the components as fabricated have small imperfections that introduce optical aberrations that adversely affect imaging quality. Correcting for such aberrations is difficult and costly. The proposed use of white-light phase conjugate mirrors offers a relatively simple and inexpensive solution of the aberration-correction problem. Indeed, it should be possible to simplify the entire approach to making large optical components because there would be no need to fabricate those components with extremely high precision in the first place: A white-light phase-conjugate mirror could correct for all the distortions and aberrations in an optical system. The use of white-light phase-conjugate mirrors would be essential for ensuring high performance in optical systems containing lightweight membrane mirrors, which are highly deformable. As used here, "phase-conjugate mirror" signifies, more specifically, an optical component in which incident light undergoes time-reversal phase conjugation. In practice, a phase-conjugate mirror would typically be implemented by use of a suitably positioned and oriented photorefractive crystal. In the case of a telescope comprising a primary and secondary mirror (see figure) white light from a distant source would not be brought to initial focus on one or more imaging scientific instrument(s) as in customary practice. Instead, the light would be brought to initial focus on a phase-conjugate mirror. The phase-conjugate mirror would send a phase-conjugate image back, along the path of the incoming light, to the primary mirror. A transparent, highly efficient diffractive thin film deposited on the primary mirror would direct the phase-conjugate image to the imaging instrument(s).

Frazier, Donald↗

Localization of Nonblinking Point Sources Using Higher-Order-Mode Detection and Optical Heterodyning: Developing a Strategy for Extending the Scope of Molecular, Super-resolution Imaging

While the stochastic, “blinking” nature of fluorescent systems has enabled the super-resolution of their localization by the fitting of their point-spread functions (PSFs), this strategy cannot be exploited for similar resolution of “nonblinking” systems, such as those that might be encountered in a coherent Raman experiment. An alternative method for subdiffraction-limited imaging lies in the exploitation of optical heterodyning. For example, if a Gaussian PSF (a TEM00 mode) of a point emitter is displaced with respect to the origin of the optical system, photons in the higher-order TEM modes carry information about that displacement. Information concerning the displacement can be extracted from photons in these higher-order modes. These photons can be collected by optical heterodyning, which exploits the large gain in a detector’s response to an optical signal from an emitter coupled to a local oscillator, which is prepared in the TEM of interest, e.g., TEM10. We have generalized and developed the heterodyning technique to localize point emitters via the detection of higher-order spatial modes. We have developed a theoretical approach to find a practical estimation limit of the localization parameters using a realistic model that accounts for shot noise, background noise, and Gaussian noise. To demonstrate the applicability of the method, we designed experiments in which a laser is a surrogate for one and two point emitters. Using the Fisher information and its accompanying Cramér-Rao lower bound, we demonstrate super-resolution localization in these cases: we show that objects can be localized to roughly 2–3 orders of magnitude of their point-spread function’s size for a given optical system. Finally and most importantly, it is suggested that the results will ultimately be generalizable to multiple emitters and, most importantly, to “nonblinking” molecular systems, which will be essential for broadening the scope of super-resolution measurements beyond the limits of fluorescence-based techniques.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗