Diffraction-limited Size Research Articles

Manufacturability-based optical design optimization for advanced Kirkpatrick–Baez X-ray focusing mirrors

The advanced Kirkpatrick–Baez (AKB) mirror setup is an effective and compelling solution to provide stable X-ray nano-focusing for synchrotron radiation or free-electron laser beamlines. We propose an AKB mirror design optimization approach to mitigate the difficulties associated with mirror fabrication by minimizing the total slope ranges of the four curved mirrors while achieving the expected focusing performance. In the optimization, we have considered geometry constraints to ensure the beam acceptance with the required clear aperture, the diffraction-limited focal size with the adequate numerical aperture, and the desired mirror gaps for adjustment and the necessary working distance for the sample stage. Additionally, practical constraints linked to mirror metrology and fabrication, such as mirror length limits and curvature uncertainty in measurement, are taken into account. Furthermore, progressive objective optimization eliminates the need for any initial guess, fully automating the AKB optimization process. This approach facilitates the development of an elegant Wolter-I or Wolter-III type AKB design solution that satisfies these multiple constraints. In cases where constraints cannot be simultaneously satisfied, the optimization results provide valuable insights into areas where trade-offs need to be considered. Simulations with ray tracing and wavefront propagation validate the optimized AKB design showing high tolerance to the beam incident angle.

(Invited) Direct Laser Induced Gold Wiring of 2D Materials with Sub-Μm Resolution

One of the most influential technologies of our modern world are integrated electronics. Almost all parts of our daily life include some bearing with any kind of electrical technologies. The fabrication methods itself, for integrated miniatured electrical devices have had not much innovation in terms of production. Several processing steps still mainly consist of different kinds of lithography. This situation may change with new challenges on the production of smaller quantities with specialized functions, or the use of temperature critical or atomically thin surfaces, where the thermal evaporation of metals damages the sample.For some decades now, printing of all types of electronics have gained great attraction. While lithography is a time-consuming multi-step process (including resist preparation, illuminating, developing, evaporation and lift-off) with expensive and harmful photoresists and harsh environmental conditions (high-vacuum and thermal treatments), ink printing allows for direct and simple application of the desired structures [1]. Two main types of inks are typically applied: colloidal solutions of metal nanoparticles [2, 3] or metal-organic precursor solutions [4]. In both cases, thermal curing after deposition is required to achieve metallic conduction. To this end, laser writing is often advantageous over thermal sintering due to the overall lower thermal stress applied to the material, particularly on flexible, thermally sensitive substrates [5] whereas metal nanoparticles suffer from a relatively high photothermal stability and the need for a large laser power to achieve sufficient sintering [3]. In contrast, metal-organic precursor solutions feature a relatively low metal content (≤34 wt-%)10, and undergo large volume contractions during laser writing. These challenges have so far prevented the definition of metallic gold contacts with diffraction-limited feature sizes by ink printing and laser writing.Here, we introduce atomically-precise, metalloid Au32(nBuP12Cl8) nanoclusters (Au32NCs) [6] as an ink for resistless, direct laser writing of metallic gold micro- and nanostructures. The unique advantages of this ink over Au nanoparticles or typical metal-organic Au precursors are their high photosensitivity in combination with a large gold content of 70 wt-%. This allows for writing gold structures with feature sizes of 250 nm and line spacings < 200 nm using 1.86 mW laser power at 488 nm with a scan speed of 0.1 mm/s. We apply this method on a wide range of substrates, including flexible polymer membranes, find metallic conductance with conductivities ~ 1 × 106 S/m and demonstrate that defining such Au contacts on two-dimensional semiconductors results in fully functional optical switches and field effect transistors made out from 2D materials.[1] Raut NC. et al., Jour. Mat. Chem. C 2018, 6(7): 1618-1641.[2] Ko E. et al., Nanotechnology 2007, 18(34): 345202.[3] Hong S. et al., ACS Nano 2013, 7(6): 5024-5031.[4] Schoner C et al., Thin Solid Films 2013, 531: 147-151.[5] Skylar-Scott MA et al., PNAS 2016, 113(22): 6137-6142.[6] Kenzler S et al., Angew. Chem. Int. Ed. 2019, 58(18): 5902-5905. Figure 1

High-throughput screening to identify modulators of membrane protein raft affinity in giant plasma membrane vesicles.

Lipid rafts remain an active area of membrane biophysics research. Due to their diffraction-limited size and transient nature direct studies of rafts and their resident proteins in cells remains intractable. The lack of tools to manipulate raft-resident proteins has also stymied our ability to study raft function and raft partitioning of proteins. Giant plasma membrane vesicles (GPMVs), which spontaneously separate into ordered (raft) and disordered (non-raft) phases, are a practical a tool for studying rafts in biological membranes. We recently developed a high-throughput screening pipeline combining high-content imaging with a custom image-analysis software package, VesA, to identify small molecule modulators of phase separation in GPMVs. Using this approach, we are conducting an on-going screen 20,000 of small molecules from the Vanderbilt University Discover collection to find compounds that alter the phase partitioning of the peripheral myelin protein 22 (PMP22). PMP22, a major component of myelin in Schwann cells of the peripheral nervous system, shows a high affinity for ordered phases of GPMVs. Disease causing mutations in PMP22 exhibit both varying degrees of misfolding and decreased raft partitioning which strongly correlate to disease severity. We hypothesize that PMP22 fold stability is necessary for both raft partitioning and trafficking to the plasma membrane. From the screen, we are identifying hits that we sort into different categories based on their effects on (1) PMP22 raft partitioning (2) GPMV phase composition and (3) raft partitioning of other proteins. Identification of small molecules that non-specifically alter raft affinity will be useful tools for dissecting how and why proteins prefer rafts. The identification of small molecules that selectively bind to PMP22 and alter its phase partitioning will be crucial to investigating the relationship between PMP22 structure, raft affinity, and trafficking.

Direct Heat-Induced Patterning of Inorganic Nanomaterials.

Patterning functional inorganic nanomaterials is an important process for advanced manufacturing of quantum dot (QD) electronic and optoelectronic devices. This is typically achieved by inkjet printing, microcontact printing, and photo- and e-beam lithography. Here, we investigate a different patterning approach that utilizes local heating, which can be generated by various sources, such as UV-, visible-, and IR-illumination, or by proximity heat transfer. This direct thermal lithography method, termed here heat-induced patterning of inorganic nanomaterials (HIPIN), uses colloidal nanomaterials with thermally unstable surface ligands. We designed several families of such ligands and investigated their chemical and physical transformations responsible for heat-induced changes of nanocrystal solubility. Compared to traditional photolithography using photochemical surface reactions, HIPIN extends the scope of direct optical lithography toward longer wavelengths of visible (532 nm) and infrared (10.6 μm) radiation, which is necessary for patterning optically thick layers (e.g., 1.2 μm) of light-absorbing nanomaterials. HIPIN enables patterning of features defined by the diffraction-limited beam size. Our approach can be used for direct patterning of metal, semiconductor, and dielectric nanomaterials. Patterned semiconductor QDs retain the majority of their as-synthesized photoluminescence quantum yield. This work demonstrates the generality of thermal patterning of nanomaterials and provides a new path for additive device manufacturing using diverse colloidal nanoscale building blocks.

Wide-Field Super-Resolution Optical Fluctuation Imaging through Dynamic Near-Field Speckle Illumination.

Stochastic optical fluctuation imaging (SOFI) generates super-resolution fluorescence images by emphasizing the positions of fluorescent emitters via statistical analysis of their on-and-off blinking dynamics. In SOFI with speckle illumination (S-SOFI), the diffraction-limited grain size of the far-field speckles prevents independent blinking of closely located emitters, becoming a hurdle to realize the full super-resolution granted by SOFI processing. Here, we present a surface-sensitive super-resolution technique exploiting dynamic near-field speckle illumination to bring forth the full super-resolving power of SOFI without blinking fluorophores. With our near-field S-SOFI technique, up to 2.8- and 2.3-fold enhancements in lateral spatial resolution are demonstrated with computational and experimental fluorescent test targets labeled with conventional fluorophores, respectively. Fluorescent beads separated by 175 nm are also super-resolved by near-field speckles of 150 nm grain size, promising sub-100 nm resolution with speckle patterns of much smaller grain size.

Realization of Curved Circular Nanotubes Using In Situ Monitored Self-Assembly.

Curved fluidic channels with a circular cross-section play an important role in biology, chemistry, and medicine. However, in nanofluidics, a problem that is largely unsolved is the lack of an effective fabrication method for curved circular nanotubes (10-1000 nm). In this work, an electron-beam-induced self-assembly process was applied to achieve fine curved nanostructures for the realization of nanofluidic devices. The diameter of the tube could be precisely controlled by an atomic layer deposition process. Fluid transported through the nanochannels was verified and characterized using a dark-field microscope under an optical diffraction limit size. The fluid flow demonstrates that the liquid's evaporation (vapor diffusion) in the nanochannel generates compressed vapor, which pumps the liquid and pushes it forward, resulting in a directional flow behavior in the ∼100 nm radius of tubes. This phenomenon could provide a useful platform for the development of diverse nanofluidic devices.

Direct-focusing surface-emitting laser.

Focusing is a fundamental optical technique that has been widely implemented via lenses. Here, we demonstrate direct focusing from a band-edge surface-emitting laser, whose emission area is 200 µm × 200 µm, without any lenses. To achieve this, a phase-modulating layer is incorporated into the laser cavity. This layer acts simultaneously as a lasing cavity similar to that of a photonic crystal laser and as a holographic spatial-phase modulator, which transforms the output beam into a focusing beam by slightly shifting the positions of holes from a periodic square lattice. Beam profiles along the surface normal clearly show that direct focusing occurs with a focal length and focal spot size of 310 µm and 6.1 µm, respectively. The focal length agrees well with the theoretical value, and the focal spot size is 2.0 times the diffraction-limited size, which indicates that the higher transverse modes are sufficiently suppressed. In addition, the power density at the focus is 540 times higher than that at the near-field plane. Interestingly, a focus pattern is also observed in the opposite direction at the near-field plane, which indicates that a converging beam and a diverging beam are simultaneously emitted because of the nature of the in-plane band-edge laser. The conventional beam patterns of semiconductor laser cavities are limited to the regime of two-dimensional projection based on a Fourier hologram. In contrast, we demonstrate the simplest form of a three-dimensional point cloud based on a Fresnel hologram, which is quite useful for micro-sensing applications such as microfluidics, flow cytometry, blood sensors, and endoscopy.

Single-Molecule Fluorescence Spectroscopy of Phase-Separated 10,12-Pentacosadynoic Acid Films.

Phase-separated monolayers of 10,12-pentacosadiynoic acid and perfluorotetradecanoic acid can be photopolymerized to produce micrometer-sized, fluorescent polydiacetylene fibers at the air-solid interface. The photopolymer fibers were not uniformly fluorescent but rather showed a series of fluorescent spots along their lengths. The spots exhibited the classic properties of single-molecule fluorescence emission, including diffraction-limited size and fluorescence intermittency ("on-off blinking"). We have analyzed the fluorescence blinking dynamics of these spots using a variety of single-molecule analysis approaches, including fluorescence intensity histograms, autocorrelation analysis, as well as cross-correlation analysis as a function of distance between individual transition dipole moments, and propose a simple physical model for the fiber structure based on the observed blinking dynamics, in which the polymer fibers contain numerous structural defects. The model was supported by grazing incidence X-ray diffraction measurements of the mixed monolayer films at the air-water interface, in which it was observed that the presence of perfluorocarbon in the mixed monolayers significantly inhibited the ability of the 10,12-pentacosadiynoic acid to polymerize.

Parallel Polarization Illumination with a Multifocal Axicon Metalens for Improved Polarization Imaging.

Polarization imaging is an important branch of the microscopy technique that can provide additional information and enhanced contrast. The illumination system of a polarization microscope enables many different polarizations but makes the setup bulky, complicated, and slow. Here, we design and fabricate an ultrathin planar axicon metalens that also enables parallel illumination with different polarizations. Our results reveal a diffraction-limited size and high degree of linear polarization. To verify our approach, we accurately map the polarization angle of an aluminum grating, which is used as a polarizer. Furthermore, we demonstrate that elliptical polarization can be generated without additional design. A single metalens has the same capabilities as a conventional illumination module containing a polarizer, compensator, and rotation-stage/optical modulator. In addition, our device has the potential to enable rapid super-resolution polarization imaging. The new method could be useful in many applications and areas, including, e.g., materials research and biomedicine.

Focusing Surface-Acoustic-Wave Microcavities on GaAs

Focusing microcavities for surface acoustic waves (SAWs) produce highly localized strain and piezoelectric fields that can dynamically control excitations in nanostructures. Focusing transducers (FIDTs) that generate SAW beams that match nanostructure dimensions require pattern correction due to diffraction and wave-velocity anisotropy. The anisotropy correction is normally implemented by adding a quadratic term to the dependence of the wave velocity on the propagation angle. We show that a SAW focusing to a diffraction-limited size in $\mathrm{Ga}\mathrm{As}$ requires corrections that more closely follow the group-velocity wave front, which is not a quadratic function. Optical interferometric mapping of the resultant SAW displacement field reveals tightly focused SAW beams on $\mathrm{Ga}\mathrm{As}$ with a minimal beam waist. An additional set of Gouy-phase--corrected passive fingers creates an acoustic microcavity in the focal region with a small volume and a high quality factor. Our ${\ensuremath{\lambda}}_{\mathrm{SAW}}=5.6\phantom{\rule{0.2em}{0ex}}\ensuremath{\mu}\mathrm{m}$ FIDTs are expected to scale well to the approximately 500-nm wavelength regime needed to study strong coupling between vibrations and electrons in electrostatic $\mathrm{Ga}\mathrm{As}$ quantum dots.

Broadband nano-focusing of high-order harmonics in soft X-ray region with ellipsoidal mirror

We demonstrate broadband focusing of multiple high-order harmonics of intense femtosecond laser pulses using an ellipsoidal mirror. The ellipsoidal mirror, with a high numerical aperture and a highly accurate surface, was fabricated using a replication process. The multiple high-order harmonics in the wavelength range between 10 and 20 nm were focused to the nearly diffraction-limited size of 350 × 380 nm2. According to Rayleigh's quarter wavelength criteria, the wavefront aberration of the focused beam was estimated to be less than 5 nm, which corresponds to a temporal dispersion of 16 as. The developed focusing system is suited for producing an intense attosecond laser field with negligible wavefront aberration, with which nonlinear light-matter interactions in the attosecond time domain can be explored.

Rocking curve and spatial coherence properties ofalong X-ray compound refractive lens.

Semi-analytical theory of a long set of X-ray compound refractive lenses (CRLs) based on recurrence relations is developed further. The geometrical aperture, angular divergence of incident radiation and source size were accurately taken into account. Using this theory it is possible to calculate the width of the rocking curve of a long (40.7 cm) Be CRL which coincides with experimental data obtained earlier. By this approach the transverse coherence length for the X-ray beam after passing a set of CRLs of arbitrary complexity has been estimated. It is shown that at the focus this coherence length is equal to a diffraction-limited beam size (beam size in the case of a point source) and has minimal difference with the real beam size.

Nearly diffraction-limited hard X-ray line focusing with hybrid adaptive X-ray mirror based on mechanical and piezo-driven deformation.

We have developed the new hybrid adaptive X-ray mirror based on mechanical and piezo-driven deformation to realize precise shape controllability on a long-length mirror. The mechanical bender approximately provides the required ellipse, while the piezoelectric actuators attached to the mirror correct very small residual errors to satisfy the diffraction-limited condition. The mechanical bender significantly reduces the role of the piezoelectric actuator, resulting in the suppression of accuracy degradation due to the drift and/or junction effect of the piezoelectric actuators. In addition, line focusing was demonstrated with two different numerical apertures at SPring-8, and the obtained beam sizes were 127 and 253 nm (FWHM), which agree well with the diffraction-limited sizes.

The impact of ELT distortions and instabilities on future astrometric observations

The paper discusses an assessment study about the impact of the distortions on the astrometric observations with the Extremely Large Telescope originated from the optics positioning errors and telescope instabilities. Optical simulations combined with Monte Carlo approach reproducing typical inferred opto-mechanical and dynamical instabilities, show RMS distortions between $\sim$ 0.1-5 mas over 1 arcmin field of view. Over minutes timescales the plate scale variations from ELT-M2 caused by wind disturbances and gravity flexures and the field rotation from ELT-M4-M5 induce distortions and PSF jitter at the edge of 1 arcmin FoV (radius 35 arcsec) up to $\sim$ 5 mas comparable to the diffraction-limited PSF size $FWHM_H = 8.5$ mas. The RMS distortions inherent to the ELT design are confined to the 1$^{st}$-3$^{rd}$ order and reduce to an astrometric RMS residual post fit of $\sim$ 10-20 $\mu as$ for higher order terms. In this paper, we study which calibration effort has to be undertaken to reach an astrometric stability close to this level of higher order residuals. The amplitude and timescales of the assumed telescope tolerances indicate the need for frequent on-sky calibrations and MCAO stabilization of the plate scale to enable astrometric observations with ELT at the level of $\leq 50 \mu as$, which is one of the core science missions for the ELT / MICADO instrument.

Radiating pattern of surge-current-induced THz light in near-field and far-field zone

We generate the THz wave on the surface of an unbiased GaAs crystal by illuminating femtosecond laser pulses with a 45° incidence angle, and investigate its propagation properties comprehensively both in a near-field and in a far-field zone by performing a knife-edge scan measurement. In the near-field zone, i.e. 540 μm away from the generation point, we found that the beam simply takes a Gaussian shape of which width follows well a behavior predicted by a paraxial wave equation. In the far-field zone, on the other hand, it takes a highly anisotropic shape; whereas the beam profile maintains a Gaussian shape along the normal to the plane of incidence, it takes satellite peak structures along the direction in parallel to the plane of incidence. From the comparison with simulation results obtained by using a dipole radiation model, we demonstrated that this irregular beam pattern is attributed to the combined effect of the position-dependent phase retardation of the THz waves and the diffraction-limited size of the initial beam which lead to the interference of the waves in the far-field zone. Also, we found that this consideration accounting for a crossover of THz beam profile to the anisotropic non-Gaussian beam in the far-field zone can be applied for a comprehensive understanding of several other THz beam profiles obtained previously in different configurations.

Microscale optical cryptography using a subdiffraction-limit optical key

We present microscale optical cryptography using a subdiffraction-limit optical pattern, which is finer than the diffraction-limit size of the decrypting optical system, as a key and a substrate with a reflectance distribution as an encrypted image. Because of the subdiffraction-limit spatial coding, this method enables us to construct a secret image with the diffraction-limit resolution. Simulation and experimental results demonstrate, both qualitatively and quantitatively, that the secret image becomes recognizable when and only when the substrate is illuminated with the designed key pattern.

Two-photon deep-tissue spatially resolved mitochondrial imaging using membrane potential fluorescence fluctuations.

Cell metabolism and viability are directly reflected in their mitochondria. Imaging-based analysis of mitochondrial morphological structure, size and dynamic characteristics can therefore provide critical insight into cell function. However, mitochondria are often very abundant, and due to their close to diffraction-limit size, it is often non-trivial to distinguish a tubular or large mitochondrion from an ensemble of punctate mitochondria. In this paper, we use membrane potential dependent fluorescence fluctuations of individual mitochondria to resolve them using an approach similar to single molecule localization microscopy. We use 2-photon microscopy to image mitochondrial intensity fluctuations at 200 μm deep inside an intact in-vivo mouse soleus muscle. By analyzing the acquired images, we can reconstruct images with an extra layer of information about individual mitochondria, separated from their ensemble. Our analysis shows a factor of 14 improvement in detection of mitochondria.

Polarized Nonlinear Nanoscopy of Metal Nanostructures

Nonlinear signals from metal nanostructures are known to be highly polarization-dependent, due to the intrinsic vectorial nature of nonlinear optical coupling. Nonlinear optical polarization responses contain important information on the near-field properties of nanostructures; however, they remain complex to monitor and to model at the nanoscale. Polarization resolved nonlinear optical microscopy can potentially address this question; however, the recorded signals are generally averaged over the diffraction-limited size of a few hundreds of nanometers, thus, missing the spatial specificity of the nanostructure’s optical response. Here we present a form of polarization resolved microscopy, named polarization nonlinear nanoscopy, which reveals subdiffraction scale vectorial variations of electromagnetic fields, even though the intensity image is diffraction-limited. We show that by exploiting, at a single subdiffraction pixel level, the information gained by the polarization-induced modulation, it is possi...

Clean localization super-resolution microscopy for 3D biological imaging

We propose clean localization microscopy (a variant of fPALM) using a molecule filtering technique. Localization imaging involves acquiring a large number of images containing single molecule signatures followed by one-to-one mapping to render a super-resolution image. In principle, this process can be repeated for other z-planes to construct a 3D image. But, single molecules observed from off-focal planes result in false representation of their presence in the focal plane, resulting in incorrect quantification and analysis. We overcome this with a single molecule filtering technique that imposes constraints on the diffraction limited spot size of single molecules in the image plane. Calibration with sub-diffraction size beads puts a natural cutoff on the actual diffraction-limited size of single molecules in the focal plane. This helps in distinguishing beads present in the focal plane from those in the off-focal planes thereby providing an estimate of the single molecules in the focal plane. We study the distribution of actin (labeled with a photoactivatable CAGE 552 dye) in NIH 3T3 mouse fibroblast cells.

Generation of a spherical focal spot in a 4Pi focusing system through reversing the radiation of infinite biconical antenna

A method of generating spherical focal spot is demonstrated through reversely propagating and tightly focusing the electric field at the pupil plane radiated from an infinite biconical antenna centered at the foci of two confocal high numerical aperture aplanatic objective lenses. The required incident field distribution at the pupil plane is found by solving the inverse problem of radiation from an infinite biconical antenna using the Richards–Wolf vectorial diffraction theory. Numerical simulations show that a focal spot of excellent spherical symmetry along with extremely low sidelobe (~4.72% of the peak) and diffraction limited spot size of 0.432λ can be obtained in a 4Pi focusing system. It is also shown that the generated focal spot can be shifted along the optical axis while still maintaining its spherical shape and diffraction limited size through introducing a phase difference between the pupil illumination fields of the two objective lenses used in the 4Pi focusing system.