Nanoscience and Nanotechnology Commons^™

Sensing Negative-Cone Rotational Diffusion Of Dipole-Like Emitters, Yuanxin Qiu, Kaizhi A. Nie, Matthew D. Lew

Electrical & Systems Engineering Publications and Presentations

Fluorescence anisotropy and single-molecule orientation-localization microscopy (SMOLM) are powerful techniques that quantify the rotational diffusion of dipole-like emitters, which is important for sensing molecular interactions and chemical environments at the nanoscale. Numerous theoretical and experimental studies have thoroughly characterized single-molecule rotations even when those rotations are much faster than the detector integration time. Here, we extend the theory of measuring rotational diffusion to situations where a single dipole rotates uniformly everywhere outside of an isotropic cone of a certain size, termed a negative cone. This scenario corresponds to negative fluorescence anisotropy 𝑟 and has been observed in emitters exhibiting strong …

Single-Molecule Orientation And Localization Microscopy, Sophie Brasselet, Matthew D. Lew

Electrical & Systems Engineering Publications and Presentations

Single-molecule localization microscopy (SMLM) offers enhanced spatial resolution in optical microscopy, providing detailed insights into the spatial organization of proteins in cells at the nanoscale. Over the past decade, SMLM has progressively incorporated the capability to retrieve the orientations of single molecules using their polarized dipolar emission pattern. Here we explore recent advancements in single-molecule orientation and localization microscopy (SMOLM), which yields super-resolved images of molecular three-dimensional (3D) orientations, wobble and 3D positions. This advancement opens possibilities to explore the nanoscale organization and conformation of biological molecules as well as to monitor and design local 3D optical fields in nanophotonics. …

Functional Devices Based On Freestanding 2d Materials, Shijue Xu

McKelvey School of Engineering Graduate Student Theses & Dissertations

Two-dimensional (2D) materials have attracted extensive attention in the field of nanoelectronics due to their atomic-scale thickness, high surface-to-volume ratio, tunable electronic properties, and compatibility with low-temperature processing. These characteristics make them highly suitable for the construction of emerging device architectures, particularly in both ionic and electronic devices.

In this work, we investigate the application of 2D materials in two distinct classes of devices: ionically-driven memristors and electronically-dominated metal–semiconductor contacts. For the memristor study, we fabricate heterostructure-based resistive switching devices using h-BN and WSe₂ as active layers. These 2D material-based memristors exhibit stable power consumption loops and high linearity …

Josephson Junctions: Fabrication And Applications For The Axion Dark Matter Experiment, Jonah M. Sachs

Senior Honors Papers / Undergraduate Theses

The observation of axions could revolutionize the world of physics. Through microwave frequency cavity readout of the photons associated with these axions, the ADMX project at WashU utilizes multiple different forms of the Josephson junction (JJ), a superconductive circuit element. The physics behind the JJ are essential to understanding its operation for resonant cavity readout in addition to parametric amplification. Parametric amplifiers produced using JJs can approach the signal-to-noise ratio set by quantum mechanics, and prove essential for the amplification chain used by the ADMX experiment for axionic detection. The limits of these amplifiers are set by the noise tuning …

Single-Molecule Orientation Imaging Reveals The Nano-Architecture Of Amyloid Fibrils Undergoing Growth And Decay, Brian Sun, Tianben Ding, Weiyan Zhou, Tara S. Porter, Matthew D. Lew

Electrical & Systems Engineering Publications and Presentations

Amyloid-beta (Aβ42) aggregates are characteristic Alzheimer’s disease signatures, but probing how their nanoscale architectures influence their growth and decay remains challenging using current technologies. Here, we apply time-lapse single-molecule orientation-localization microscopy (SMOLM) to measure the orientations and rotational “wobble” of Nile blue (NB) molecules transiently binding to Aβ42 fibrils. We correlate fibril architectures measured by SMOLM with their growth and decay over the course of 5 to 20 min visualized by single-molecule localization microscopy (SMLM). We discover that stable Aβ42 fibrils tend to be well-ordered and signified by well-aligned NB orientations and small wobble. SMOLM also shows that increasing order …

Fabrication Of Two-Dimensional Material-Based Nano-Capacitors Using Bismuth Selenite (Bi2seo5) To Study Its Dielectric Properties, Major Kc

McKelvey School of Engineering Graduate Student Theses & Dissertations

In recent years, the demand for high-performance micro and nanodevices has surged, necessitating the exploration of novel dielectric materials to replace conventional silicon dioxide. Following the continuation of the Moorse law, as device dimensions reduce to nanoscale levels, the properties of silicon dioxide can degrade, leading to issues such as increased leakage current and reduced gate control. Materials with superior electrical properties, such as higher dielectric constant, lower leakage current, and better thermal stability allowing for the development of faster, more efficient, and more reliable devices are in higher demand than ever. Two-dimensional layered semiconductor nanomaterials represented by compounds such …

6d Single-Fluorogen Orientation-Localization Microscopy For Elucidating The Architecture Of Beta-Sheet Assemblies And Biomolecular Condensates, Tingting Wu, Weiyan Zhou, Jai S. Rudra, Rohit V. Pappu, Matthew D. Lew

Electrical & Systems Engineering Publications and Presentations

We develop six-dimensional single-molecule orientation-localization microscopy (SMOLM) to measure the 3D positions and 3D orientations simultaneously of single fluorophores. We show how careful optimization of phase and polarization modulation components can encode phase, polarization, and angular spectrum information from each fluorescence photon into a microscope’s dipole-spread function. We used the transient binding and blinking of Nile red (NR) to characterize the helical structure of fibrils formed by designed amphipathic peptides, KFE8^L and KFE8^D, and the pathological amyloid-beta peptide Aβ42. We also deployed merocyanine 540 to uncover the interfacial architectures of biomolecular condensates.

Analytical And Experimental Investigation Of Interphase And Dispersion Effects On The Mechanical Stiffness Of Cellulose Nanocomposites, Will Goldberg

McKelvey School of Engineering Graduate Student Theses & Dissertations

The effect of dispersion and interphase properties on the elastic behavior of cellulose nanocomposites was investigated using a number of composite models, experimental data and a thorough literature review. Cellulose nanocomposites consisting of soy protein isolate (SPI) and cellulose nanocrystals (CNC) or polydopamine coated cellulose nanocrystals (PD-CNC) were prepared via solution casting method and tested for mechanical stiffness. These outcomes were compared to standard composite models as well as novel methods adapted from the literature that incorporate data regarding dispersion quality and interphase properties. The literature review verified that both dispersion and interphase properties are highly dependent on interfacial chemistry …

Six-Dimensional Single-Molecule Imaging With Isotropic Resolution Using A Multi-View Reflector Microscope, Oumeng Zhang, Zijian Guo, Yuanyuan He, Tingting Wu, Michael D. Vahey, Matthew D. Lew

Electrical & Systems Engineering Publications and Presentations

Imaging of both the positions and orientations of single fluorophores, termed single-molecule orientation-localization microscopy, is a powerful tool for the study of biochemical processes. However, the limited photon budget associated with single-molecule fluorescence makes high-dimensional imaging with isotropic, nanoscale spatial resolution a formidable challenge. Here we realize a radially and azimuthally polarized multi-view reflector (raMVR) microscope for the imaging of the three-dimensional (3D) positions and 3D orientations of single molecules, with precisions of 10.9 nm and 2.0° over a 1.5-μm depth range. The raMVR microscope achieves 6D super-resolution imaging of Nile red molecules transiently bound to lipid-coated spheres, accurately resolving …

Synthesis And Consolidation Of Metal Oxide Nanocrystals Via Nonthermal Plasma, Austin Cendejas

McKelvey School of Engineering Graduate Student Theses & Dissertations

Nonthermal plasmas offer a unique nonequilibrium environment that has been leveraged in a wide variety of applications in the fields of material processing, lighting, and waste management to name a few. In all of these cases, the plasma serves as a source of high energy electrons, ions, reactive gas species, and radicals that interact in several ways with surfaces brought into contact with the plasma. Specifically, nonthermal plasmas have been shown to be very successful in achieving continuous, high-throughput, monodisperse nanocrystals of a wide variety of materials. The crystallinity of nanoparticles synthesized in nonthermal plasmas can be attributed to the …

Nano-Bio Interactions: Implications And Applications, Anushree Ghosh

McKelvey School of Engineering Graduate Student Theses & Dissertations

Rapid expansion of technology development at the nanoscale has underpinned a promising industry. Towards this, there remain significant information gaps which are critical with regard to decision making processes and ultimate industrial sustainability. From an implication point of view, understanding how common biological macromolecules, including glycolipids and/or biopolymers produced by bacteria and fungi, which are ubiquitous in the environment, is fundamental to predicting the behavior of released/produced nanoparticles. Conversely, other bio-based tailored macromolecules, including mussel foot protein (MFP), have significant potential as functional material coatings for advanced applications.This PhD thesis is focused on interfacial processes related to superparamagnetic iron oxide …

Multifunctional Polydopamine Nanomaterials For Biomedical And Environmental Applications, Hamed Gholami Derami

McKelvey School of Engineering Graduate Student Theses & Dissertations

Polydopamine (PDA), a synthetic and organic material, has emerged as a promising materialplatform for various applications in energy, environmental, and biomedical fields. PDA, formed by self-polymerization of dopamine, is rich in catechol and amine groups, which facilitate covalent conjugation and/or other non-covalent interactions with organic and inorganic materials. It is highly biocompatible, biodegradable, has broadband light absorption spectrum and excellent light-to-heat conversion efficiency. Also, it is easy to synthesize and functionalize. The combination of excellent characteristics of polydopamine-based nanomaterials, make them a promising adsorbent agent for environmental wastewater treatment and photothermal agent for biomedical applications. In the first half of …

Growth Of Small Particles In Nonequilibrium Plasmas, Necip Berker Üner

McKelvey School of Engineering Graduate Student Theses & Dissertations

Nonequilibrium plasma (NEP) is an extraordinary environment for material synthesis. NEP is comprised of hot electrons with temperatures greater than 10000 K and of cold ions and neutrals that are usually at few hundred kelvins above room temperature. Due to this large difference in species’ temperatures, the assumption of local thermal equilibrium does not hold in NEP. Therefore, NEP can act as a unique processor of mass, and it can transform materials along pathways that are not accessible by methods wherein local thermal equilibrium is valid. For decades, NEPs have been employed in the semiconductor industry to manufacture many thin …

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 …

Defect Chemistry And Ion Intercalation During The Growth And Solid-State Transformation Of Metal Halide Nanocrystals, Bo Yin

McKelvey School of Engineering Graduate Student Theses & Dissertations

Abstract of the Dissertation

Defect Chemistry and Ion Intercalation During the Growth and Solid-State Transformation of Metal Halide Nanocrystals

Semiconductor metal halides as light-sensitive materials have applications in multiple areas, such as photographic film, antibacterial agents and photocatalysts. One focus of this dissertation is to achieve novel morphologies of ternary silver bromoiodide (AgBr1-xIx, 0

For the silver halide system, we demonstrate that the anion composition of AgBr1-xIx nanocrystals determines their shape through the introduction of twin defects as the nanocrystals are made more iodide-rich. AgBr1-xIx nanocrystals grow as single-phase, solid solutions with the rock salt crystal structure for anions compositions …

Towards Engineering Advanced Nanomaterials: Elucidating Fundamental Particle Behavior In Water And Critical Sorption Dynamics, Changwoo Kim

McKelvey School of Engineering Graduate Student Theses & Dissertations

As advanced nanomaterials, inorganic-organic nano composites have received great interest as potential platform (nano) structures for sensor, catalyst, sorbent, and environmental applications. Here, my Ph.D. research has focused on the design, synthesis, and characterization of advanced water-stable engineered metal-oxide nanoparticles functionalized by organic frames for environmental applications. For the environmental applications, I have evaluated particleoptimized sorption processes for the remediation and separation of arsenic, chromium, and uranium under environmentally relevant conditions. More specifically, I have explored the critical role of organic coating on sorption mechanisms and performances using engineered iron oxide -based, manganese oxide -based, and manganese ferrite -based (core) …

Development And Evaluation Of Biocompatible Engineered Nanoparticles For Use In Ophthalmology, Bedia Begum Karakocak

McKelvey School of Engineering Graduate Student Theses & Dissertations

The synthesis and design of biocompatible nanoparticles for targeted drug delivery and bioimaging requires knowledge of both their potential toxicity and their transport. For both practical and ethical reasons, evaluating exposure via cell studies is a logical precursor to in vivo tests. As a step towards clinical trials, this work extensively investigated the toxicity of gold nanoparticles (Au NPs) and carbon dot (CD) nanoparticles as a prelude to their in vivo application, focusing specifically on ocular cells. As a further step, it also evaluated their whole-body transport in mice. The research pursued two approaches in assessing the toxicity of engineered …

Increasing Ph In Cancer: Enabling A New Therapeutic Paradigm Using Novel Carbonate Nanoparticles, Avik Som

McKelvey School of Engineering Graduate Student Theses & Dissertations

Enormous progress has been made to treat cancer, and yet the mortality rate of cancer remains unacceptably high. High clinical resistance to molecularly targeted therapeutics has pushed interest again towards inhibiting universal biochemical hallmarks of cancer. Recent evidence suggests that malignant tumors acidify the local extracellular environment to activate proteases for degrading the tumor matrix, which facilitates metastasis, and explains why more aggressive tumors are more acidic. Current therapies have only focused on using the low pH for enhancing drug release in tumors, thereby still relying on the traditional paradigm of intracellular inhibition of pathways, a method that continues to …

Functional Bio-Nano Hybrids Through A Precise Control Of Interfacial Interactions At The Nanoscale, Sirimuvva Tadepalli

McKelvey School of Engineering Graduate Student Theses & Dissertations

During the course of evolution, proteins have evolved to perform exquisite functions including structural support, signal transduction, actuation, sensing, catalysis, trafficking, gating, light-harvesting, charge transfer, molecular recognition, self-assembly, self-organization, or combinations of two or more of these functions. A precise control and manipulation of the structure and function of proteins is conceivable with the advent of nanotechnology, which has facilitated the integration of nanomaterials with functional biomolecules to realize bio-nano hybrids with synergistically enhanced functionalities.

At the genesis of bionanotechnology, a paucity in the fundamental understanding of the bio-nano interfaces is a grave impediment to the progress of the field. …

Activity Preservation Of Plasmonic Biosensors With A Metal-Organic Framework, Lu Wang

McKelvey School of Engineering Graduate Student Theses & Dissertations

Antibody-antigen recognition enables antibody-conjugated nanostructures to serve as plasmonic biosensors with tunable specificity. However due to the instability of antibodies, these biosensors are susceptible to changes in the environment such as heat and aridity, leading to constraints on the transportation and handling of these sensors. Here we establish a method using a metal-organic framework crystal to preserve biosensor activity under severe environmental conditions, including exposure to high temperatures, an organic solvent and a proteolytic agent. After zeolitic imidazolate framework-8 (ZIF-8) crystals formed for 12 hours on a biosensor of gold nanorods conjugated with a model antibody, rabbit IgG, 80% of …

Development And Evaluation Of A Near-Infrared (1047 Nm) Photoacoustic-Nephelometer Spectrometer For Detection And Optical Characterization Of Black Carbon Aerosol, Yang Yu

McKelvey School of Engineering Graduate Student Theses & Dissertations

Black carbon (BC) aerosol are aggregates of small carbon spherules of <10 nm to approximately 50 nm in diameter. They are characterized by their strong visible light absorption property with a mass absorption cross-section (MAC) value above 5 m² g ⁻¹ at a wavelength λ = 550 nm, which increases inversely with wavelengths from near-infrared (≈1 µm) to ultraviolet with a power law of one. The absorbing nature of BC aerosol has been implicated in regional atmospheric warming, changing of monsoon patterns, and accelerated melting of the glaciers. The BC radiative effects over earth is currently estimated within a factor of four, resulting in one of the largest uncertainties in climate modeling. This uncertainty results from our inadequate knowledge about regional BC emission rates, and associated aerosol …

Contact Radius And Insulator-Metal Transition In Films Comprised Of Touching Semiconductor Nanocrystals, Deanna M. Lanigan

McKelvey School of Engineering Graduate Student Theses & Dissertations

Nanocrystal assemblies are being explored for a number of optoelectronic applications such as transparent conductors, photovoltaic solar cells, and electrochromic windows. Majority carrier transport is important for these applications, yet it remains relatively poorly understood in films comprised of touching nanocrystals. Specifically, the underlying structural parameters expected to determine the transport mechanism have not been fully elucidated. In this report, we demonstrate experimentally that the contact radius, between touching heavily doped ZnO nanocrystals, controls the electron transport mechanism. Spherical nanocrystals are considered, which are connected by a circular area. The radius of this circular area is the contact radius. For …

Feed-Forward Inhibitory Circuits In Hippocampus And Their Computational Role In Fragile X Syndrome, Sarah Lauren Wahlstrom Helgren

McKelvey School of Engineering Graduate Student Theses & Dissertations

Feed-forward inhibitory (FFI) circuits are canonical neural microcircuits. They are unique in that they are comprised of excitation rapidly followed by a time-locked inhibition. This sequence provides for a powerful computational tool, but also a challenge in the analysis and study of these circuits. In this work, mechanisms and computations of two hippocampal FFI circuits have been examined. Specifically, the modulation of synaptic strength of the excitation and the inhibition is studied during constant-frequency and naturalistic stimulus patterns to reveal how FFI circuit properties and operations are dynamically modulated during ongoing activity. In the first part, the FFI circuit dysfunction …

Entry Flow And Heat Transfer Of Laminar And Turbulent Forced Convection Of Nanofluids In A Pipe And A Channel, Yihe Huang

McKelvey School of Engineering Graduate Student Theses & Dissertations

This thesis presents a numerical investigation of laminar and turbulent fluid flow and convective heat transfer of nanofluids in the entrance and fully developed regions of flow in a channel and a pipe. In recent years, nanofluids have attracted attention as promising heat transfer fluids in many industrial processes due to their high thermal conductivity. Nanofluids consist of a suspension of nanometer-sized particles of higher thermal conductivity in a liquid such as water. The thermal conductivity of nanoparticles is typically an order-of-magnitude higher than the base liquid, which results in a significant increase in the thermal performance of the nanofluid …

Optical Resonators And Fiber Tapers As Transducers For Detection Of Nanoparticles And Bio-Molecules, Huzeyfe Yilmaz

McKelvey School of Engineering Graduate Student Theses & Dissertations

In recent years, detection of biological interactions on single molecule level has aspired many researchers to investigate several optical, chemical, electrical and mechanical sensing tools. Among these tools, toroidal optical resonators lead the way in detection of the smallest particle/molecule with the real time measurements. In this work, bio-sensing capabilities of toroidal optical resonators are investigated. Bio-sensing is realized via measuring the analyte-antigen interaction while the antigen is immobilized through a novel functionalization method.

Not long ago, detection of single nanoparticles using optical resonators has been accomplished however the need for cost-effective and practical transducers demands simpler tools. A tapered …