Wavelength domain spatial frequency modulation imaging: enabling fiber optic delivery and detection.

Spatial frequency modulation imaging (SPIFI) provides a simple architecture for modulating an extended illumination source that is compatible with single pixel imaging. We demonstrate wavelength domain SPIFI (WD-SPIFI) by encoding time-varying spatial frequencies in the spectral domain that can produce enhanced resolution images, like its spatial domain counterpart, spatial domain (SD) SPIFI. However, contrary to SD-SPIFI, WD-SPIFI enables remote delivery by single mode fiber, which can be attractive for applications where free-space imaging is not practical. Finally, we demonstrate a cascaded system incorporating WD-SPIFI in-line with SD-SPIFI enabling single pixel 2D imaging without any beam or sample scanning.

Cascaded domain multiphoton spatial frequency modulation imaging.

Significance: Multiphoton microscopy is a powerful imaging tool for biomedical applications. A variety of techniques and respective benefits exist for multiphoton microscopy, but an enhanced resolution is especially desired. Additionally multiphoton microscopy requires ultrafast pulses for excitation, so optimization of the pulse duration at the sample is critical for strong signals. Aim: We aim to perform enhanced resolution imaging that is robust to scattering using a structured illumination technique while also providing a rapid and easily repeatable means to optimize group delay dispersion (GDD) compensation through to the sample. Approach: Spatial frequency modulation imaging (SPIFI) is used in two domains: the spatial domain (SD) and the wavelength domain (WD). The WD-SPIFI system is an in-line tool enabling GDD optimization that considers all material through to the sample. The SD-SPIFI system follows and enables enhanced resolution imaging. Results: The WD-SPIFI dispersion optimization performance is confirmed with independent pulse characterization, enabling rapid optimization of pulses for imaging with the SD-SPIFI system. The SD-SPIFI system demonstrates enhanced resolution imaging without the use of photon counting enabled by signal to noise improvements due to the WD-SPIFI system. Conclusions: Implementing SPIFI in-line in two domains enables full-path dispersion compensation optimization through to the sample for enhanced resolution multiphoton microscopy.

Design and analysis of polygonal mirror-based scan engines for improved spatial frequency modulation imaging.

Spatial frequency modulation imaging (SPIFI) is a structured illumination single pixel imaging technique that is most often achieved via a rotating modulation disk. This implementation produces line images with exposure times on the order of tens of milliseconds. Here, we present a new architecture for SPIFI using a polygonal scan mirror with the following advances: (1) reducing SPIFI line image exposure times by 2 orders of magnitude, (2) facet-to-facet measurement and correction for polygonal scan design, and (3) a new anamorphic magnification scheme that improves resolution for long working distance optics.

Super-resolution computational saturated absorption microscopy.

Imaging beyond the diffraction limit barrier has attracted wide attention due to the ability to resolve previously hidden image features. Of the various super-resolution microscopy techniques available, a particularly simple method called saturated excitation microscopy (SAX) requires only simple modification of a laser scanning microscope: The illumination beam power is sinusoidally modulated and driven into saturation. SAX images are extracted from the harmonics of the modulation frequency and exhibit improved spatial resolution. Unfortunately, this elegant strategy is hindered by the incursion of shot noise that prevents high-resolution imaging in many realistic scenarios. Here, we demonstrate a technique for super-resolution imaging that we call computational saturated absorption (CSA) in which a joint deconvolution is applied to a set of images with diversity in spatial frequency support among the point spread functions (PSFs) used in the image formation with saturated laser scanning fluorescence microscopy. CSA microscopy allows access to the high spatial frequency diversity in a set of saturated effective PSFs, while avoiding image degradation from shot noise.

Single-shot spatial frequency modulation for imaging.

Spatial frequency modulation for imaging (SPIFI) has traditionally employed a time-varying spatial modulation of the excitation beam. Here, for the first time to our knowledge, we introduce single-shot SPIFI, where the spatial frequency modulation is imposed across the entire spatial bandwidth of the optical system simultaneously enabling single-shot operation.

Wavelength-multiplexed single-shot ptychography.

We present the first experimental demonstration of wavelength-multiplexing in single-shot ptychography. Specifically, we experimentally reconstruct the complex transmission profile of a wavelength-independent and wavelength-dependent object simultaneously for 532 nm and 633 nm probing wavelengths. In addition, we discuss the advantages of a more general approach to detector segmentation in single-shot ptychography. A minimization to correct for uncertainties in a priori information that is required for single-shot geometries is presented along with a novel probe constraint. Furthermore, this technique is complementary to dual-wavelength interferometry without the need for an external reference. This work is enabling to imaging technologies and applications such as broadband single-shot ptychography, time-resolved imaging by multiplexed ptychography, real-time inspection for laser micro-machining, and plasma imaging.

Investigating low salinity waterflooding via glass micromodels with triangular pore-throat architectures.

Glass micromodels have been extensively used to simulate and investigate crude oil, brine, and surface interactions due to their homogeneous wettability, rigidity, and ability to precisely capture a reservoir's areal heterogeneity. Most micromodels are fabricated via two-dimensional patterning, implying that feature depths are constant despite varying width, which sub-optimally describes a three-dimensional porous architecture. We have successfully fabricated micromodels with arbitrary triangular cross sections via femtosecond pulsed laser direct writing resulting in depth-dependent channel width. As such, we have achieved arbitrary geometric control over device fabrication and thus a more accurate recapitulation of a geological porous media. With this fabrication technique, we are now able to directly observe pore-level, depth-dependent multiphase flow phenomena. This platform was used to study the low salinity effect (LSE) by simulating waterflooding processes using various brine solutions that differ in cation type and salinity. Patterned pore-throat structures were created to investigate displacement behavior during waterflooding. Real-time monitoring of the displacement processes, combined with a comparison of the brine chemistry before and after waterflooding provides an insight into realistic interactions occurring between crude oil and brine. The results indicate that produced emulsions were prone to coalesce in the presence of lower salinity brine. Combined with previous work, the LSE was interpreted as favored coalescence and resisted breakup that resulting in a more continuous aqueous phase during waterflooding therefore improving the displacement efficiency.

Fabrication of sealed sapphire microfluidic devices using femtosecond laser micromachining.

Due to its hardness, strength, and transparency, sapphire is an attractive material for the construction of microfluidic devices intended for high-pressure applications, but its physiochemical properties resist traditional microfabrication and bonding techniques. Here a femtosecond pulsed laser was used to directly machine fluidic channels within sapphire substrates and to form bonds between machined and flat sapphire windows, resulting in the creation of sealed microfluidic devices. Sapphire-sapphire bond strength was determined by destructive mechanical testing, and the integrity of the bond was verified by the capillary filling of the channel with air and ethanol. This combination of optical micromachining and bonding establishes a fully integrated approach to the fabrication of sapphire-based microfluidic systems.

Two-dimensional random access multiphoton spatial frequency modulated imaging.

Spatial frequency modulated imaging (SPIFI) enables the use of an extended excitation source for linear and nonlinear imaging with single element detection. To date, SPIFI has only been used with fixed excitation source geometries. Here, we explore the potential for the SPIFI method when a spatial light modulator (SLM) is used to program the excitation source, opening the door to a more versatile, random access imaging environment. In addition, an in-line, quantitative pulse compensation and measurement scheme is demonstrated using a new technique, spectral phase and amplitude retrieval and compensation (SPARC). This enables full characterization of the light exposure conditions at the focal plane of the random access imaging system, an important metric for optimizing, and reporting imaging conditions within specimens.

Single-pixel fluorescent diffraction tomography.

Optical diffraction tomography (ODT) is an indispensable tool for studying objects in three dimensions. Until now, ODT has been limited to coherent light because spatial phase information is required to solve the inverse scattering problem. We introduce a method that enables ODT to be applied to imaging incoherent contrast mechanisms such as fluorescent emission. Our strategy mimics the coherent scattering process with two spatially coherent illumination beams. The interferometric illumination pattern encodes spatial phase in temporal variations of the fluorescent emission, thereby allowing incoherent fluorescent emission to mimic the behavior of coherent illumination. The temporal variations permit recovery of the spatial distribution of fluorescent emission with an inverse scattering model. Simulations and experiments demonstrate isotropic resolution in the 3D reconstruction of a fluorescent object.

Fluorescent coherent diffractive imaging with accelerating light sheets.

Fluorescence microscopy is a powerful method for producing high fidelity images with high spatial resolution, particularly in the biological sciences. We recently introduced coherent holographic image reconstruction by phase transfer (CHIRPT), a single-pixel imaging method that significantly improves the depth of field in fluorescence microscopy and enables holographic refocusing of fluorescent light. Here we demonstrate that by installing a confocal slit conjugate to the illuminating light sheets used in CHIRPT, out-of-focus light is rejected, thus improving lateral spatial resolution and rejecting noise from out-of-focus fluorescent light. Confocal CHIRPT is demonstrated and fully modeled. Finally, we explore the use of beam shaping and point-spread-function engineering to enable holographic single-lens light-sheet microscopy with single-pixel detection.

Spectral phase and amplitude retrieval and compensation technique for measurement of pulses.

In this Letter, an in-line, compact, and efficient quantitative pulse compensation and measurement scheme is demonstrated. This simple system can be readily deployed in multiphoton imaging systems and advanced manufacturing where multiphoton processes are exploited.

Fourier computed tomographic imaging of two dimensional fluorescent objects.

We introduce a new form of tomographic imaging that is particularly advantageous for a new class of super-resolution optical imaging methods. Our tomographic method, Fourier Computed Tomography (FCT), operates in a conjugate domain relative to conventional computed tomography techniques. FCT is the first optical tomography method that records complex projections of the object spatial frequency distribution. From these spatial frequency projections, the spatial slice theorem is derived, which is used to build a tomographic imaging reconstruction algorithm. FCT enables enhancement of spatial frequency support along a single spatial direction to be isotropic in the entire transverse spatial frequency domain.

Interferometric spatial frequency modulation imaging.

Interferometric spatial frequency modulation for imaging (I-SPIFI) is demonstrated for the first time, to our knowledge. Significantly, this imaging modality can be seamlessly combined with nonlinear SPIFI imaging and operates through single-element detection, making it compatible for use in scattering specimens. Imaging dynamic processes with submicrometer axial resolution through long working distance optics is shown, and high contrast images compared to traditional wide-field microscopy images. Finally, enhanced lateral resolution is achieved in I-SPIFI. To our knowledge, this is the first single platform that enables multimodal linear and nonlinear imaging, with enhanced resolution, all of which can be performed simultaneously.

Three-dimensional single-pixel imaging of incoherent light with spatiotemporally modulated illumination.

We derive analytic expressions for the three-dimensional coherent transfer function (CTF) and coherent spread function (CSF) for coherent holographic image reconstruction by phase transfer (CHIRPT) microscopy with monochromatic and broadband illumination sources. The 3D CSF and CTF were used to simulate CHIRPT images, and the results show excellent agreement with experimental data. Finally, we show that the formalism presented here for computing the CSF/CTF pair in CHIRPT microscopy can be readily extended to other forms of single-pixel imaging, such as spatial-frequency-modulated imaging.

Fabrication and characterization of modulation masks for multimodal spatial frequency modulated microscopy.

Spatial frequency modulated imaging (SPIFI) is a powerful imaging method that when used in conjunction with multiphoton contrast mechanisms has the potential to improve the spatial and temporal scales that can be explored within a single nonlinear optical microscope platform. Here we demonstrate, for the first time to our knowledge, that it is possible to fabricate inexpensive masks using femtosecond laser micromachining that can be readily deployed within the multiphoton microscope architecture to transform the system from a traditional point-scanning system to SPIFI and gain the inherent advantages that follow.

Two-phase displacements in microchannels of triangular cross-section.

Varying microfluidic channel cross-sectional geometry can dramatically alter fluid flow behavior, particularly for capillary-driven flow. Most fabrication techniques, however, are planar and therefore incapable of providing depth-dependent variations in width. We introduce an ultrafast laser ablation technique that enables the fabrication of microchannels with arbitrary triangular cross sectional geometry. Triangular channels were fabricated with widths ranging from 45 to 116µm and aspect ratios between 0.7 and 1.9. This experimental platform was utilized to observe two-phase flow and evaluate the capillary pressures required to initiate flow within triangular capillaries. Applying Mayer, Stowe and Princen (MS-P) theory, critical drainage capillary pressures were predicted for varying cross sections and compared to experimental observations. Results indicate the capability to predict capillary pressures inside triangular channels with perfectly water wet surfaces, providing the first instance of experimental validation of the theory for arbitrary triangular cross sections. This work was extended to intermediate wet conditions, which provides an insight into the prediction of capillary pressure under more realistic conditions. The fabrication techniques and validation of predictive frameworks presented here provide an approach to microfluidic experimental design that will impact a wide range of fundamental and applied technology areas.

Plasmon-less surface enhanced Raman spectra induced by self-organized networks of silica nanoparticles produced by femtosecond lasers.

Raman spectroscopy is the workhorse for label-free analysis of molecules. It relies on the inelastic scattering of incoming monochromatic light impinging molecules of interest. This effect leads to a very weak emission of light spectrum that provides a signature of the molecules being observed. Considerable efforts have been made over the last decades, in particular with the development of Surface Enhanced Raman Spectroscopy (SERS), to enhance the intensity of the emitted signal so that ultimately, traces of molecules can be detected. Here, we show that dense self-organized networks of quasi-monodisperse nanoparticles redepositing during femtosecond laser ablation of trenches in fused silica can lead to a significant field enhancement effect, enabling the Raman detection of a single-molecule layer deposited on the surface (so called monolayer). Unlike previously reported for SERS experiments, here, there is no metal layer promoting plasmonics effects causing localized field enhancement. The method for producing SERS substrates is therefore quite straightforward and low cost.

Superresolved multiphoton microscopy with spatial frequency-modulated imaging.

Superresolved far-field microscopy has emerged as a powerful tool for investigating the structure of objects with resolution well below the diffraction limit of light. Nearly all superresolution imaging techniques reported to date rely on real energy states of fluorescent molecules to circumvent the diffraction limit, preventing superresolved imaging with contrast mechanisms that occur via virtual energy states, including harmonic generation (HG). We report a superresolution technique based on spatial frequency-modulated imaging (SPIFI) that permits superresolved nonlinear microscopy with any contrast mechanism and with single-pixel detection. We show multimodal superresolved images with two-photon excited fluorescence (TPEF) and second-harmonic generation (SHG) from biological and inorganic media. Multiphoton SPIFI (MP-SPIFI) provides spatial resolution up to 2η below the diffraction limit, where η is the highest power of the nonlinear intensity response. MP-SPIFI can be used to provide enhanced resolution in optically thin media and may provide a solution for superresolved imaging deep in scattering media.

Simultaneous spatial frequency modulation imaging and micromachining with a femtosecond laser.

A Ti:Al2O3 chirped-pulse amplification system is used to simultaneously image and machine. By combining simultaneous spatial and temporal focusing (SSTF) with spatial frequency modulation for imaging (SPIFI), we are able to decouple the imaging and cutting beams to attain a resolution and a field-of-view that is independent of the cutting beam, while maintaining single-element detection. This setup allows for real-time feedback with the potential for simultaneous nonlinear imaging and imaging through scattering media. The novel SSTF machining platform uses refractive optics that, in general, are prohibitive for energetic, amplified pulses that might otherwise compromise the integrity of the focus as a result of nonlinear effects.