A non-invasive method to quantify the stress distribution in polymer-based materials is presented through the piezospectroscopic calibration of alumina-epoxy nanocomposites. Three different alumina volume fraction nanocomposites were created and loaded under uniaxial compression in order to determine the relationship between applied stress and the frequency shift of the R-lines produced by alumina under excitation. Quantitative values for six piezospectroscopic coefficients were obtained which represent the stress-sensing property of the nanocomposites. The results were applied to an alumina-filled adhesive in a single lap shear configuration demonstrating the capability of the technique to monitor R-line peak positions with high spatial resolution and assess the stress distribution within the material prior to failure. Additionally, particle dispersion and volume fraction were confirmed with spectral intensities, introducing a novel experimental method for the assessment of quality in manufacturing of such nanocomposites. Results were further used to initiate studies in determining the load transfer to the nanoparticles and assessing the fundamental driving mechanisms.

Volumetric optical microscopy has the advantages of quantitative and global measurement of three-dimensional (3D) biological specimens with high spatial resolution and minimum invasion. However, current volumetric imaging technologies based on light transmission, scattering or fluorescence cannot reveal specimen’s chemical distribution that brings insights to study the chemical events in organisms and their metabolism, functionality, and development. Stimulated Raman scattering (SRS) microscopy allowing visualization of chemical contents based on their intrinsic molecular vibrations is an emerging imaging technology to provide rapid label-free volumetric chemical imaging. This dissertation describes three methodologies for developing advanced volumetric SRS imaging technologies to address the challenges of imaging in vivo samples, imaging speed, and axial resolution. In the first methodology, SRS volumetric imaging is enabled by axially scanning the laser foci for sectioning different depth layers. In Chapter 2, we utilize a piezo objective positioner to drive the objective. Combining with the tissue clearance technique, we realize volumetric SRS imaging up to 500 µm depth in brain tissues showing the potential for 3D staining-free histology. The limitations of piezo scanning are slow speed and disturbance to in vivo samples while rapidly scanning the objective. To tackle the limitations, in Chapter 3, we develop a remote-focusing volumetric SRS microscope based on a deformable mirror and adaptive optics optimization, allowing focal scanning without physically moving the objective or sample. We demonstrate in vivo monitoring of chemical penetration in human sweat pores. In the second methodology, instead of axially scanning the laser foci, the SRS volumetric imaging is enabled by projection imaging with extended depth-of-focus (DOF) beams such as Bessel beams and low numerical-aperture beams. The extended DOF beams integrate SRS signals along the propagation direction to form projection images; thus, a single lateral scan obtains the volumetric chemical information, significantly increasing the volumetric imaging speed for measuring chemical content over a large volume. In Chapter 4, we describe a stimulated Raman projection microscope for fast quantitation of chemicals in a 3D volume. However, projection imaging intrinsically loses axial resolution. We addressed the limitation by developing SRS projection tomography. Mimicking computed tomography, the axial information is reconstructed by angle-dependent projection images obtained by sequentially rotating the sample in a capillary glass tube within the SRS focus. Nevertheless, sample rotation is complicated and not compatible with in vivo samples. To address the difficulty, in Chapter 5, we develop tilted-angle-illuminated stimulated Raman projection tomography which utilizes tilted-angle beams with a tilted angle respected to the optical axis of the objective to obtain angle-dependent projections. This scheme is free of sample rotation and enables fast projection scanning for pushing the imaging speed. The calibration approach and vector-field back-projection algorithm are developed for the multi-view tomographic reconstruction. In the third methodology, we improve the spatial resolution in miniature volumetric SRS imaging via the innovation of metasurface photonics. In developing an SRS endoscope for volumetric chemical imaging inside the human body, the axial resolution deteriorates due to chromatic and monochromatic aberrations induced by poorly made miniature objective lenses. In Chapter 6, we develop a silicon metasurface tailored for compensating the phase errors between the pump and Stokes wavelengths of a singlet refractive lens. Integrating the metasurface with the refractive lens, the hybrid achromatic metalens is compact and provides nearly diffraction-limit resolution, demonstrating a way for developing high resolution chemical imaging endoscopy.

Liquid crystals have been a major subject of research for the past decades. Aside from the variety of structures they can form, they exhibit a vast range of optical phenomena. Many of these phenomena found applications in technology and became an essential part of it. In this dissertation thesis we continue the line to propose a number of new applications of optical effects in liquid crystals and develop their theoretical framework. One such application is the possibility of beam combining using Orientational Stimulated Scattering in a nematic liquid crystal cell. Our numerical study of the OSS process shows that normally this possibility does not exist. However, we found that if a number of special conditions is satisfied efficient beam combining with OSS can be done. These conditions require a combination of special geometric arrangement of incident beams, their profiles, nematic material, and more. When these conditions are fulfilled, power of the beamlets can be coherently combined into a single beam, with high conversion efficiency while the shape and wave-front of the output beam are still of good quality. We also studied the dynamics of the OSS process itself and observed (in a numerical model) a number of notorious instabilities caused by effects of back-conversion iv process. Additionally, there was found a numerical solitary-wave solution associated with this back-conversion process. As a liquid crystal display application, we consider a nematic liquid crystal layer with the anisotropy axis modulated at a fixed rate in the transverse direction with respect to light propagation direction. If the layer locally constitutes a half-wave plate, then the thinscreen approximation predicts 100% -efficient diffraction of normal incident wave. If this diffracted light is blocked by an aperture only transmitting the zero-th order, the cell is in dark state. If now the periodic structure is washed out by applying voltage across the cell and light passes through the cell undiffracted, the light will pass through the aperture as well and the cell will be in its bright state. Such properties of this periodically aligned nematic layer suggest it as a candidate element in projection display cells. We studied the possibility to implement such layer through anchoring at both surfaces of the cell. It was found that each cell has a thickness threshold for which the periodic structure can exist. The anchored periodic structure cannot exist if thickness of the cell exceeds this threshold. For the case when the periodic structure exists, we found the structure distortion in comparison with the preferable ideal sinusoidal profile. To complete description of the electromechanical properties of the periodic cell, we studied its behavior at Freedericksz transition. Optical performance was successfully described with the coupled-mode theory. While influence of director distortion is shown to be negligibly small, the walk-off effects appear to be larger. In summary, there are good prospects for use of this periodically v aligned cell as a pixel in projection displays but experimental study and optimization need to be performed. In the next part we discuss another modulated liquid crystal structure in which the director periodically swings in the direction of light propagation. The main characteristic of such structure is the presence of bandgap. Cholesteric liquid crystals are known to possess bandgap for one of two circular polarizations of light. However, unlike the cholesterics the bandgap of the proposed structure is independent of polarization of normally incident light. This means that no preparation of light is needed in order for the structure to work in, for example, liquid crystal displays. The polarization universality comes at the cost of bandgap size, whose maximum possible value ∆ωPTN compared to that of cholesterics ∆ωCh is approximately twice smaller: ∆ωPTN ≈ 0.58∆ωCh if modulation profile is sinusoidal, and ∆ωPTN ≈ 0.64∆ωCh if it is rectangular. This structure has not yet been experimentally demonstrated, and we discuss possible ways to make it.

Two-photon absorption (2PA) has been used for a number of scientific and technological applications, exploiting the fact that the 2PA probability is directly proportional to the square of the incident light intensity (while one-photon absorption bears a linear relation to the incident light intensity). This intrinsic property of 2PA leads to 3D spatial localization, important in fields such as optical data storage, fluorescence microscopy, and 3D microfabrication. The spatial confinement that 2PA enables has been used to induce photochemical and photophysical events in increasingly smaller volumes and allowed nonlinear, 2PA-based, technologies to reach sub-diffraction limit resolutions. The primary focus of this dissertation is the development of novel, efficient 2PA, fluorene-based molecules to be used either as photoacid generators (PAGs) or fluorophores. A second aim is to develop more effective methods of synthesizing these compounds. As a third and final objective, the new molecules were used to develop a write-once-read many (WORM) optical data storage system, and stimulated emission depletion probes for bioimaging. In Chapter I, the microwave-assisted synthesis of triarylsulfonium salt photoacid generators (PAGs) from their diphenyliodonium counterparts is reported. The microwave-assisted synthesis of these novel sulfonium salts afforded reaction times 90 to 420 times faster than conventional thermal conditions, with photoacid quantum yields of new sulfonium PAGs ranging from 0.01 to 0.4. These PAGs were used to develop a fluorescence readout-based, nonlinear three-dimensional (3D) optical data storage system (Chapter II). In this system, writing was achieved by acid generation upon two-photon absorption (2PA) of a PAG (at 710 or 730 nm). Readout was then performed by interrogating two-photon absorbing dyes, after protonation, at 860 nm. Two-photon recording and readout of voxels was demonstrated in five and eight consecutive, crosstalk-free layers within a polymer matrix, generating a data storage capacity of up to 1.8 x 1013 bits/cm3. The possibility of using these PAGs in microfabrication is described in Chapter III, where two-photon induced cationic ring-opening polymerization (CROP) crosslinking of an SU8 resin is employed to produce free-standing microstructures. Chapter IV describes the investigation of one- and two-photon stimulated emission transitions by the fluorescence quenching of a sulfonyl-containing fluorene compound in solution at room temperate using a picosecond pump-probe technique. The nature of stimulated transitions under various fluorescence excitation and quenching conditions were analyzed theoretically, and good agreement with experimental data was demonstrated. Two-photon stimulated transitions S1 to S0 were shown at 1064 nm. The two-photon stimulated emission cross section of the sulfonyl fluorophore was estimated as aproximately 240 - 280 GM, making this compound a good candidate for use in two-photon stimulated emission depletion (STED) microscopy.

Cutaneous lupus erythematosus (CLE) is an autoimmune disease that resolves with or without permanent scars depending on the subtype. Interferons (IFNs), including the skin specific IFNλ mainly activate STAT1, which results in inflammation in CLE and may play a significant role in scar formation in chronic discoid CLE. IL-22 activates STAT3 and it is emerging as a mediator with significant impact on normal wound repair, epidermal hyperproliferation and prevention of fibrosis. This work focussed on understanding the regulation and functional impact of IL-22 and IFNλ on skin cells. The counter-regulatory effect of IL-22 on the activities of IFNλ was assessed through downstream interferon stimulated genes (ISGs) expression in healthy and CLE keratinocytes. Cell proliferation and gap closure were investigated in skin resident cells using cell trace dye and scratch assay. Dermal fibroblasts were assessed for the presence of IFNλR1 and IL-22R1, downstream activities of the receptors. Results showed that IL-22 accelerated “scratch” closure in keratinocytes while IFNλ caused a delay in closure. IL-22 significantly downregulated IFNλ-induced chemokines expression in healthy, but not CLE keratinocytes. Reduced IL-22R1 expression and “STAT3 signature genes” was observed in CLE keratinocytes. A key finding of this project is that dermal fibroblasts respond to both IFNλ and IL-22. This work shows that IL-22 can reduce the damaging effect of IFNs in inflamed skin and also identifies dermal fibroblasts as important cells in skin immune responses. In conclusion, IL-10 family members can have both beneficial and destructive effects on the skin organ depending on the micro milieu and cell-type involved. Manipulating the balance of IL-10 family members in the skin may offer new therapeutic approach for both psoriasis and CLE. / University of Bradford and Centre for Skin Sciences

ESR, OSL and TT-OSL dating methods were applied to samples collected from six of the Ancient Coastal Deposits (ACDs) along the southern Georgia Coastline. Samples were collected from the Princess Anne (the youngest and most seaward ACD), Pamlico, Talbot, Penholoway, Wicomico, and Okefenokee ACDs with the goal of determining the age of formation of these features. Ground Penetrating Radar (GPR) was used to determine the subsurface morphology and target lithologies for age determination. OSL and TT-OSL dating was attempted on samples collected from the youngest two ACDs, the Pamlico and Princess Anne, at McMaster Universities AGE Lab. ESR samples collected from all of the ACDs studied were measured at Florida State University as well as Osaka University. ESR analysis measured the Al signal, the Ti-Li signal, measured using two different methods, as well as the Ti-H signal. A number of low additive dose points were added to the ESR dose plan to attempt to create a better dose response curve for the low saturating Ti-H signal in attempt to better utilize the signal. While the geochronological methodology did not prove useful for determining the age of all of the ACDs it did result in depositional age estimates for the Cypresshead Formation at 433-2978 ka and Satilla Formations at 243-417 ka using the Ti-Li ESR signal as a maximum age estimate. The GPR, ESR, and core data all point to the conclusion that the ACDs of the Georgia Coast are geomorphic modifications and not the result of a unique depositional process. Based on the discrepancy between the depositional age of the Cypresshead and Satilla Formations as determined by ESR in this study and the ages of the ACDs published by others from Georgia (Markewich et.al., 2013) or other areas of the Atlantic Coast (Wehmiller, 2004; Willis, 2006) it can be concluded that paleo sea-levels modified the Cypresshead and Satilla Formations in to the morphology seen today at some point after their initial deposition. / Dissertation / Doctor of Philosophy (PhD) / ESR, OSL and TT-OSL dating methods were applied to samples collected from six of the Ancient Coastal Deposits (ACDs) along the southern Georgia Coastline with the goal of determining the age of formation of these features. Ground Penetrating Radar (GPR) was used to determine the subsurface morphology and target lithologies for age determination. A number of low additive dose points were added to the ESR dose plan to attempt to create a better dose response curve for the low-dose saturation of the Ti-H signal in attempt to better utilize the signal. While the geochronological methodology did not prove useful for determining the age of all of the ACDs, it did result in depositional age estimates for the Cypresshead Formation at 433-2978 ka and Satilla Formations at 243-417 ka. The GPR, ESR, and core data all point to the conclusion that the ACDs of the Georgia Coast are geomorphic features without unique depositional events.

Quantum and classical frameworks form two perspectives for describing physical systems. Their formulation also presents interesting isomorphism: for example, the Schrodinger equation can find its classical correspondence in the paraxial Helmholtz equation, and coherent atomic population transfers is analogous to coupling dynamics in waveguides. In classical coupled mode systems, quantum notion can be manifested in the following ways: (1) adiabatic (i.e., sufficiently slow) evolution of the Hamiltonian enables robust mode conversion and light transfer, where the dynamics is carried out in predominantly one eigenmode; (2) non-Hermitian Hamiltonians give rise to peculiar singularities known as exceptional points (EPs), associated with not only degenerate eigenvalues but coalescent eigenvectors. In this dissertation, we explore the above principles in light manipulation, sensing, and photonic emulation. First, we numerically demonstrate two examples of photonic devices based on adiabatic evolution engineering. We present a coupled waveguide system analogous to the atomic physics process of stimulated Raman adiabatic passage, where the principle of adiabaticity not only allows high-extinction polarization mode splitting, but also counterintuitively mitigates the losses from the plasmonic structure involved. We show a modal hybridization effect in rib waveguide geometry that allows the mode to adiabatically evolve from one polarization to its orthogonal state upon electro-optic modulation in thin film lithium niobate, enabling an actively switchable polarization converter. We propose a generic EP emulator based on programmable photonics to tackle the challenging implementation of EP. Our approach combines on-chip operations of coupling, loss and detuning based on generic photonic modules (Mach-Zehnder interferometers), and a discrete scheme for mapping Hamiltonians to common mesh architecture. We demonstrate multiple exemplary EP functionalities, including loss-induced transparency, encircling second-order EPs in the PT and anti-PT symmetry picture, and a third-order EP. The proposed EP emulator marks a new paradigm for discrete, \textit{in situ} programming of EPs and multi-functional, repurposable EP devices. We also present our preliminary work on NV center-induced EPs. In contrast to conventional fluorescence-based schemes for addressing NV centers, we leverage NV centers' absorption to bring a coupled ring resonator system to an EP and numerically demonstrate the emerging dynamics. Our primary numerical results promise proof-of-concept magnetometry, combining NV centers' response to magnetic and microwave fields with the sensitivity enhancing nature of EP. This dissertation sheds light on unconventional photonics inspired by quantum-like principles. / 2025-08-29T00:00:00Z

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