Optics Commons^™

Single‐Molecule 3d Orientation Imaging Reveals Nanoscale Compositional Heterogeneity In Lipid Membranes, Jin Lu, Hesam Mazidi, Tianben Ding, Oumeng Zhang, Matthew D. Lew

Electrical & Systems Engineering Publications and Presentations

In soft matter, thermal energy causes molecules to continuously translate and rotate, even in crowded environments, thereby impacting the spatial organization and function of most molecular assemblies, such as lipid membranes. Directly measuring the orientation and spatial organization of large collections (>3000 molecules μm⁻²) of single molecules with nanoscale resolution remains elusive. In this paper, we utilize SMOLM, single‐molecule orientation localization microscopy, to directly measure the orientation spectra (3D orientation plus “wobble”) of lipophilic probes transiently bound to lipid membranes, revealing that Nile red's (NR) orientation spectra are extremely sensitive to membrane chemical composition. SMOLM images resolve …

Structural Organization And Chemical Activity Revealed By New Developments In Single-Molecule Fluorescence And Orientation Imaging, Tianben Ding

McKelvey School of Engineering Graduate Student Theses & Dissertations

Single-molecule (SM) fluorescence and its localization are important and versatile tools for understanding and quantifying dynamical nanoscale behavior of nanoparticles and biological systems. By actively controlling the concentration of fluorescent molecules and precisely localizing individual single molecules, it is possible to overcome the classical diffraction limit and achieve 'super-resolution' with image resolution on the order of 10 nanometers.

Single molecules also can be considered as nanoscale sensors since their fluorescence changes in response to their local nanoenvironment. This dissertation discusses extending this SM approach to resolve heterogeneity and dynamics of nanoscale materials and biophysical structures by using positions and orientations …

Designing A Reactor Chamber For Hot Electron Chemistry On Bimetallic Plasmonic Nanoparticles, Bryn Merrill, Bingjie Zhang, Jerry Larue

SURF Posters and Papers

Catalysis provides pathways for efficient and selective chemical reactions by lowering the energy barriers for desired products. Gold nanoparticles (AuNPs) show excellent promise as plasmonic catalysts. Plasmonic materials have localized surface plasmon resonances, oscillations of the electron bath at the surface of a nanoparticle, that generate energetically intense electric fields which rapidly decay into energetically excited electrons. The excited electrons have the potential to destabilize atoms strongly bound to the catalysts through occupation of antibonding orbitals. Tuning the antibonding orbitals to make them accessible for occupancy by electrons is achieved by coating the AuNP in a thin layer of another …

Monitoring And Identifying The Rhodamine 6g-Hydroxide Ion Reaction Using In-Situ, Surface-Enhanced Raman Spectroscopy, Ryan Lamb

Masters Theses & Specialist Projects

An effective method for monitoring chemical reactions is necessary to better understand their mechanisms and kinetics. Effective reaction monitoring requires a spectroscopy technique with fast data acquisition, high sensitivity, structure-to-spectrum correlation, and low solvent interference. Surface-enhanced Raman spectroscopy (SERS) provides these features, which makes it a valuable tool for monitoring reactions. To obtain the Raman enhancement, metallic nanostructures typically made of silver or gold are aggregated using a salt. The nanoparticles aggregates must then be stabilized using a surfactant to use this method in situ due to eventual nanoparticle precipitation. In this study, gold nanoparticles stabilized with sodium dodecyl sulfate …

Nanoscale Colocalization Of Fluorogenic Probes Reveals The Role Of Oxygen Vacancies In The Photocatalytic Activity Of Tungsten Oxide Nanowires, Meikun Shen, Tianben Ding, Steven T. Hartman, Fudong Wang, Christina Krucylak, Zheyu Wang, Che Tan, Bo Yin, Rohan Mishra, Matthew D. Lew, Bryce Sadtler

Electrical & Systems Engineering Publications and Presentations

Defect engineering is a strategy that has been widely used to design active semiconductor photocatalysts. However, understanding the role of defects, such as oxygen vacancies, in controlling photocatalytic activity remains a challenge. Here, we report the use of chemically triggered fluorogenic probes to study the spatial distribution of active regions in individual tungsten oxide nanowires using super-resolution fluorescence microscopy. The nanowires show significant heterogeneity along their lengths for the photocatalytic generation of hydroxyl radicals. Through quantitative, coordinate-based colocalization of multiple probe molecules activated by the same nanowires, we demonstrate that the nanoscale regions most active for the photocatalytic generation of …

Gravity-Drawing Flexible Silicone Filaments As Fiber Optics And Model Foldamers, Katherine Snell

CMC Senior Theses

Here, we present a method of gravity-drawing polydimethylsiloxane (PDMS) silicone fibers with application as fiber optics and as model foldamers. Beginning as a viscous liquid, PDMS is cured using heat until its measured viscosity reaches 4000 mPa•s. The semi-cured elastomer is then extruded through a tube furnace to produce thin (diameters on the order of hundred micrometers) filaments with scalable lengths. PDMS is biocompatible, gas-permeable, flexible, and hydrophobic. Additionally, the PDMS surface hydrophobicity can be modified via UV exposure, O2 plasma, and corona discharge. We demonstrate the patternibility (i.e patterns of hydrophobicity) of PDMS fibers, adding complexity to potential foldamer …

Studying Near-Critical And Super-Critical Fluids In Reduced Gravity, Christian Hawkins, Ana Oprisan, Carole Lecoutre-Chabot, Yves Garrabos, Daniel Beysens

Journal of the South Carolina Academy of Science

Critical and supercritical fluids have a variety of applications, from use as machine lubricants in high pressure or high temperature environments to the manufacturing of materials such as aerogel. The optical properties of fluids undergo rapid changes near the critical point resulting in a rapid increase in turbidity known as critical opalescence. These optical changes can be used to probe the universality of critical behavior. As a fluid approaches the critical point, the compressibility rapidly increases. In a gravitational field, this increase in compressibility leads to near-critical fluids stratifying by phase and density, making it difficult to observe the optical …

Erratum: "Imaging The Three‐Dimensional Orientation And Rotational Mobility Of Fluorescent Emitters Using The Tri‐Spot Point Spread Function", Oumeng Zhang, Jin Lu, Tianben Ding, Matthew D. Lew

Electrical & Systems Engineering Publications and Presentations

In the original paper, a calibration error exists in the image-formation model used to analyze experimental images taken by our microscope, causing a bias in the orientation measurements in Figs. 2 and 3. The updated measurements are shown in Fig. E1. We have also updated the supplementary material for the original article to discuss the revised PSF model and estimation algorithms (supplementary material 2) and show the revised model and measurements (Figs. S1, S3, S7, S8, and S10–S13).

Development Of A Ground-Based Aerial-Tracking Instrument For Open-Path Spectroscopy To Monitor Atmospheric Constituents, Haden Hodges

Civil Engineering Undergraduate Honors Theses

A ground-based aerial-tracking instrument, known as the Ground Tracker, designed to provide spectral data to quantify greenhouse gases is under development. The Ground Tracker includes an Optical System including a high power rifle scope, video camera, and spectrometer used to locate an active light source from the Emitter, and collect spectral data by utilizing an actuating mirror. The implementation of this instrument could be made low cost by utilizing existing weather balloon infrastructure to allow the Emitter to be placed into the lower stratosphere. The recovery of the emitter will be possible by tracking the GPS coordinates. Weather balloon instrument …

The Development Of An Integrated Simulation Model On Understandings On The Interaction Between Electromagnetic Waves And Nanoparticles, Xiaojin Wang

Masters Theses & Specialist Projects

To investigate the interaction between nanoparticles and electromagnetic waves, a numerical simulation model based on FEM was built in this thesis. Numerical simulation is an important auxiliary research method besides experiments. The optical properties of nanoparticles consist of scattering, absorption, and extinction, and in the case of nanoparticle suspension, the transmission is also involved. This thesis addressed two typical applications based on the established model, one was regarding the nanofluids for solar energy harvesting, and the other was regarding the optical properties of atmospheric soot. In the case of the nanofluids solar energy harvesting, the established model provided a convenient …

An In-Situ Study Of The Aqueous Speciation Of Uranium (Vi) Under Hydrothermal Conditions, Diwash Dhakal

Graduate Theses/Dissertations

Rigorous study of the speciation distribution of uranyl-chloride bearing solutions under hydrothermal conditions is important to understand the transport mechanism of uranium underground, which is of uttermost interest to parties studying the geological uranium deposits and those studying the possibilities of geological repositories for spent nuclear waste. I report an in-situ Raman spectroscopic study of the speciation distribution of aqueous uranyl-chloride complexes upto 500°C conducted using a HDAC as the high PT spectroscopic cell. The samples studied contained the species UO₂²⁺, UO₂Cl⁺, UO₂Cl₂⁰ and UO₂Cl₃^{- …}

Application Of X-Ray Grating Interferometry To Polymer/Flame Retardant Blends In Additive Manufacturing, Omoefe Joy Kio

LSU Doctoral Dissertations

X-ray grating interferometry is a nondestructive tool for visualizing the internal structures of samples. Image contrast can be generated from the absorption of X-rays, the change in phase of the beam and small-angle X-ray scattering (dark-field). The attenuation and differential phase data obtained complement each other to give the internal composition of a material and large-scale structural information. The dark-field signal reveals sub-pixel structural detail usually invisible to the attenuation and phase probe, with the potential to highlight size distribution detail in a fashion faster than conventional small-angle scattering techniques. This work applies X-ray grating interferometry to the study of …

Fundamental Limits Of Measuring Single-Molecule Rotational Mobility, Oumeng Zhang, Matthew D. Lew

Electrical & Systems Engineering Publications and Presentations

Various methods exist for measuring molecular orientation, thereby providing insight into biochemical activities at nanoscale. Since fluorescence intensity and not electric field is detected, these methods are limited to measuring even-order moments of molecular orientation. However, any measurement noise, for example photon shot noise, will result in nonzero measurements of any of these even-order moments, thereby causing rotationally-free molecules to appear to be partially constrained. Here, we build a model to quantify measurement errors in rotational mobility. Our theoretical framework enables scientists to choose the optimal single-molecule orientation measurement technique for any desired measurement accuracy and photon budget.

Energy Transfer Between Eu2+ And Mn2+ For Na(Sr,Ba)Po4 And Ba2mg(Bo3)2, Kevin Bertschinger

Dissertations, Master's Theses and Master's Reports

There is no debate of the affect that solid-state lighting has had on the world we live in. Throughout the centuries, lighting has continued to improve from kerosene lanterns to white light emitting diodes. Even though lighting today is sufficient there is still much room to improve color rendering index and efficiency. An active area of research to improve today's lighting technology is by doping inorganic phosphors with luminescent ion centers. There have been numerous reports of inorganic phosphors showing a variety of emission color and luminescence. In this thesis we discuss two new inorganic phosphors codoped with Eu^{2+ …}

A System For Conducting Laser-Induced Fluorescence Measurements On Gas Mixtures Exposed To Alpha Radiation, Patrick Ables

Master's Theses

This paper documents modifications to an existing vacuum system to allow laser-induced fluorescence spectroscopy measurements within simulated atmospheres under a variety of conditions. This added capability will expand the laboratory’s ability to experimentally validate a computational model that calculates the effects of radiation within the atmosphere. The computational model could reveal radiation-induced chemical products that can be used to develop an alternative detection method that can be implemented from a safe distance. The selection of molecules for experimental validation has been limited to those which can be detected utilizing cavity ringdown spectroscopy. The current model indicates nitric oxide and ozone …

Nanostructured Fibers As A Versatile Photonic Platform: Radiative Cooling And Waveguiding Through Transverse Anderson Localization, Norman Nan Shi, Cheng-Chia Tsai, Michael J. Carter, Jyotirmoy Mandal, Adam C. Overvig, Matthew Y. Sfeir, Ming Lu, Catherine L. Craig, Gary D. Bernard, Yuan Yang, Nanfang Yu

Publications and Research

Broadband high reflectance in nature is often the result of randomly, three-dimensionally structured materials. This study explores unique optical properties associated with one-dimensional nanostructures discovered in silk cocoon fibers of the comet moth, Argema mittrei. The fibers are populated with a high density of air voids randomly distributed across the fiber cross-section but are invariant along the fiber. These filamentary air voids strongly scatter light in the solar spectrum. A single silk fiber measuring ~50 μm thick can reflect 66% of incoming solar radiation, and this, together with the fibers' high emissivity of 0.88 in the mid-infrared range, allows …

Super‐Resolution Imaging Of Amyloid Structures Over Extended Times By Using Transient Binding Of Single Thioflavin T Molecules, Kevin Spehar, Tianben Ding, Yuanzi Sun, Niraja Kedia, Jin Lu, George R. Nahass, Matthew D. Lew, Jan Bieschke

Electrical & Systems Engineering Publications and Presentations

Oligomeric amyloid structures are crucial therapeutic targets in Alzheimer's and other amyloid diseases. However, these oligomers are too small to be resolved by standard light microscopy. We have developed a simple and versatile tool to image amyloid structures by using thioflavin T without the need for covalent labeling or immunostaining. The dynamic binding of single dye molecules generates photon bursts that are used for fluorophore localization on a nanometer scale. Thus, photobleaching cannot degrade image quality, allowing for extended observation times. Super‐resolution transient amyloid binding microscopy promises to directly image native amyloid by using standard probes and record amyloid dynamics …

Investigation Of Temperature Response Of Photopolymer Material Used For Holographic Sensor, Muhammad Irfan, Tatsiana Mikulchyk, Suzanne Martin, Izabela Naydenova

Conference Papers

Recently, functionalised photopolymer has emerged as a versatile recording material in the field of optical holography due to its novel characteristics and potential use in the development of holographic based sensors, and optical elements. This work describes the temperature response of a newly developed photopolymer, containing of a monomer Nisopropylacrylamide (NIPA) which under photopolymerisation forms a temperature sensitive polymer - Poly(Nisopropylacrylamide) (PNIPA). The photonic sensor was developed by holographic recording of volume phase transmission gratings in a self-processing NIPA-based polymer with a 532 nm laser beam. A 633 nm probe beam was used to monitor real time diffraction efficiency (DE) …

Investigation Of Temperature Response Of Photopolymer Material Used For Holographic Sensor, Muhammad Irfan Dr, Tatsiana Mikulchyk Dr, Suzanne Martin Dr, Izabela Naydenova Prof

Articles

Recently, functionalised photopolymer has emerged as a versatile recording material in the field of optical holography due to its novel characteristics and potential use in the development of holographic based sensors, and optical elements. This work describes the temperature response of a newly developed photopolymer, containing of a monomer Nisopropylacrylamide (NIPA) which under photopolymerisation forms a temperature sensitive polymer - Poly(Nisopropylacrylamide) (PNIPA). The photonic sensor was developed by holographic recording of volume phase transmission gratings in a self-processing NIPA-based polymer with a 532 nm laser beam. A 633 nm probe beam was used to monitor real time diffraction efficiency (DE) …

Analysis Of The Red And Green Optical Absorption Spectrum Of Gas Phase Ammonia, Nikolai F. Zobov, Phillip A. Coles, Roman I. Ovsyannikov, Aleksandra A. Kyuberis, Robert J. Hargreaves, Peter F. Bernath, Jonathan Tennyson, Sergei N. Yurchenko, Oleg L. Polyansky

Chemistry & Biochemistry Faculty Publications

Room temperature NH₃ absorption spectra recorded at the Kitt Peak National Solar Observatory in 1980 are analyzed. The spectra cover two regions in the visible: 15,200 - 15,700 cm^-1 and 17,950 - 18,250 cm^-1. These high overtone rotation-vibration spectra are analyzed using both combination differences and variational line lists. Two variational line lists were computed using the TROVE nuclear motion program: one is based on an ab initio potential energy surface (PES) while the other used a semi-empirical PES. Ab initio dipole moment surfaces are used in both cases. 95 energy levels with J = 1 …

Plasmon-Enhanced Optical Sensing By Engineering Metallic Nanostructures, Peng Zheng

Graduate Theses, Dissertations, and Problem Reports (ETD)

The world’s booming population projected to reach 10 billion by 2050 causes enormous stresses on environmental safety, food supply, and healthcare, which in return threatens human civilizations. One of the most promising solutions lies at innovating point-of-care (POC) sensing technologies to conduct detection of environmental hazards, monitoring of food safety, and early diagnosis of diseases in a timely and accurate manner. The discovery of surface-enhanced spectroscopy in the 1970s has significantly stimulated research on light-matter interaction which gives rise to enhanced optical phenomena such as surface-enhanced Raman scattering (SERS), plasmon-enhanced fluorescence (PEF), and particularly, they have found enormous applications in …

Raman Spectroscopy Of Oxygen Evolution Catalysts And Psii Manganese Model Compounds, Sergei Shmakov, Daniel A. Hartzler, Alireza Karbakhsh Ravari, Yulia Pushkar

The Summer Undergraduate Research Fellowship (SURF) Symposium

Photosynthesis is the basis of life on earth, and oxygen evolution catalysts are key components of this complicated, yet not fully understood process. Photosystem II, a large membrane bound pigment-protein complex, is the key system that facilitates oxygenic photosynthesis via the oxygen evolving complex (a natural oxygen evolving catalyst). It is a key component in oxygen producing catalysts, which can be used in fields such as energy production and biomimetic catalysts. The oxygen evolution cycle, or Kok cycle going within it is still not studied completely. In this project, we were studying the vibrational (and structural) state of a Manganese …

Using Low-Coherence Interferometry To Monitor Cell Invasion In An In-Vitro Model System, Behnaz Davoudi Nasab

Honors Undergraduate Theses

In an optically random system, such as naturally occurring and man-made media, light undergoes pronounced multiple scattering. This phenomenon has shown a remarkable potential in characterizing complex materials. In this regime, scattering occurs from each individual center of the scattering and independent scattering events lead to multiple light scattering. This phenomenon is often described as a random walk of photons and can be modeled in terms of a diffusion equation based on the radiative transfer theory. In this thesis, we used optical path-length spectroscopy (OPS), which is an experimental method to obtain the path-length probability density of the propagating light …

Micro-Spectroscopy Of Bio-Assemblies At The Single Cell Level, Jeslin Kera

Honors Undergraduate Theses

In this thesis, we investigate biological molecules on a micron scale in the ultraviolet spectral region through the non-destructive confocal absorption microscopy. The setup involves a combination of confocal microscope with a UV light excitation beam to measure the optical absorption spectra with spatial resolution of 1.4 μm in the lateral and 3.6 μm in the axial direction. Confocal absorption microscopy has the benefits of requiring no labels and only low light intensity for excitation while providing a strong signal from the contrast generated by the attenuation of propagating light due to absorption. This enables spatially resolved measurements of single …

New And Improved Infra-Red Absorption Cross Sections And Ace-Fts Retrievals Of Carbon Tetrachloride (Ccl4), Jeremy J. Harrison, Christopher D. Boone, Peter F. Bernath

Chemistry & Biochemistry Faculty Publications

Carbon tetrachloride (CCl₄) is one of the species regulated by the Montreal Protocol on account of its ability to deplete stratospheric ozone. As such, the inconsistency between observations of its abundance and estimated sources and sinks is an important problem requiring urgent attention (Carpenter et al., 2014) [5]. Satellite remote-sensing has a role to play, particularly limb sounders which can provide vertical profiles into the stratosphere and therefore validate stratospheric loss rates in atmospheric models. This work is in two parts. The first describes new and improved high-resolution infra-red absorption cross sections of carbon tetrachloride/dry synthetic air over …

The Hitran2016 Molecular Spectroscopic Database, I. E. Gordon, L. S. Rothman, C. Hill, R. V. Kochanov, Y. Tan, P. F. Bernath, M. Birk, V. Boudon, A. Campargue, K. V. Chance

Chemistry & Biochemistry Faculty Publications

This paper describes the contents of the 2016 edition of the HITRAN molecular spectroscopic compilation. The new edition replaces the previous HITRAN edition of 2012 and its updates during the intervening years. The HITRAN molecular absorption compilation is composed of five major components: the traditional line-by-line spectroscopic parameters required for high-resolution radiative-transfer codes, infrared absorption cross-sections for molecules not yet amenable to representation in a line-by-line form, collision-induced absorption data, aerosol indices of refraction, and general tables such as partition sums that apply globally to the data. The new HITRAN is greatly extended in terms of accuracy, spectral coverage, additional …

Molecular Sensitivity And Selectivity Of Metal Nanoparticles Decorated Graphene As ‘Smart’ Surface-Enhanced Raman Scattering (Sers) Platforms [Hybrid Poster 1-A], Alexander Banaszak, Tyler Smith

Posters-at-the-Capitol

Raman scattering signal enhancement that uses graphene as support, graphene-enhanced Raman scattering (GERS), is a recent phenomenon. It can produce clean and reproducible Raman signals of chemical molecules with significantly enhanced signal intensity in contrast to traditional surface- (SERS) and tip- enhanced Raman scattering (TERS) techniques. While enhancement in SERS and TERS arise due to the electromagnetic mechanism, GERS also relies on a chemical mechanism and therefore shows unique molecular sensitivity and selectivity. In this work, we developed graphene materials decorated with noble metal (silver and gold) nanoparticles for detection of different chemical molecules e.g. methylene blue (MB) and rhodamine …

Light-Activated Photocurrent Degradation And Self-Healing In Perovskite Solar Cells, Wanyi Nie, Jean-Christophe Blancon, Amanda J. Neukirch, Kannatassen Appavoo, Hsinhan Tsai, Manish Chhowalla, Muhammad A. Alam, Matthew Y. Sfeir, Claudine Katan, Jacky Even, Sergei Tretiak, Jared J. Crochet, Gautam Gupta, Aditya D. Mohite

Publications and Research

Solution-processed organometallic perovskite solar cells have emerged as one of the most promising thin-film photovoltaic technology. However, a key challenge is their lack of stability over prolonged solar irradiation. Few studies have investigated the effect of light soaking on hybrid perovskites and have attributed the degradation in the optoelectronic properties to photochemical or field-assisted ion migration. Here we show that the slow photocurrent degradation in thin-film photovoltaic devices is due to the formation of light-activated meta-stable deep-level trap states. However, the devices can self-heal completely by resting them in the dark for <1 min or the degradation can be completely prevented by operating the devices at 0°C. We investigate several physical mechanisms to explain the microscopic origin for the formation of these trap states, among which the creation of small polaronic states involving localized cooperative lattice strain and molecular orientations emerges as a credible microscopic mechanism requiring further detailed studies.

Ultrafast Spectroscopy And Energy Transfer In An Organic/Inorganic Composite Of Zinc Oxide And Graphite Oxide, Jeff A. Secor

Dissertations, Theses, and Capstone Projects

The energy transfers and nature of defect levels of an organic/inorganic composite of Zinc Oxide and Graphite are studied with multidimensional spectroscopy. The edge and surface states of each composite are uncovered using excitation emission experiments showing which defect states are mediating the energy transfer from the metal oxide to the graphite oxide. Multidimensional time resolved spectroscopy further describes the effect of the carbon phase on the energy transfer pathways in the material.

The Dawn Of New Quantum Dots: Synthesis And Characterization Of Ge1-Xsnx Nanocrystals For Tunable Bandgaps., Richard J. Esteves

Theses and Dissertations

Ge_1-xSn_x alloys are among a small class of benign semiconductors with composition tunable bandgaps in the near-infrared spectrum. As the amount of Sn is increased the band energy decreases and a transition from indirect to direct band structure occurs. Hence, they are prime candidates for fabrication of Si-compatible electronic and photonic devices, field effect transistors, and novel charge storage device applications. Success has been achieved with the growth of Ge_1-xSn_x thin film alloys with Sn compositions up to 34%. However, the synthesis of nanocrystalline alloys has proven difficult due to larger discrepancies (~14%) in …