10,901 research outputs found
Non-Thermal Optical Engineering of Strongly-Correlated Quantum Materials
This thesis develops multiple optical engineering mechanisms to modulate the electronic, magnetic, and optical properties of strongly-correlated quantum materials, including polar metals, transition metal trichalcogenides, and copper oxides. We established the mechanisms of Floquet engineering and magnon bath engineering, and used optical probes, especially optical nonlinearity, to study the dynamics of these quantum systems.
Strongly-correlated quantum materials host complex interactions between different degrees of freedom, offering a rich phase diagram to explore both in and out of equilibrium. While static tuning methods of the phases have witnessed great success, the emerging optical engineering methods have provided a more versatile platform. For optical engineering, the key to success lies in achieving the desired tuning while suppressing other unwanted effects, such as laser heating.
We used sub-gap optical driving in order to avoid electronic excitation. Therefore, we managed to directly couple to low-energy excitation, or to induce coherent light-matter interactions. In order to elucidate the exact microscopic mechanisms of the optical engineering effects, we performed photon energy-dependent measurements and thorough theoretical analysis. To experimentally access the engineered quantum states, we leveraged various probe techniques, including the symmetry-sensitive optical second harmonic generation (SHG), and performed pump-probe type experiments to study the dynamics of quantum materials.
I will first introduce the background and the motivation of this thesis, with an emphasis on the principles of optical engineering within the big picture of achieving quantum material properties on demand (Chapter I). I will then continue to introduce the main probe technique used in this thesis: SHG. I will also introduce the experimental setups which we developed and where we conducted the works contained in this thesis (Chapter II). In Chapter III, I will introduce an often overlooked aspect of SHG studies -- using SHG to study short-range structural correlations. Chapter IV will contain the theoretical analysis and experimental realizations of using sub-gap and resonant optical driving to tune electronic and optical properties of MnPS₃. The main tuning mechanism used in this chapter is Floquet engineering, where light modulates material properties without being absorbed. In Chapter V, I will turn to another useful material property: magnetism. First I will describe the extension of the Floquet mechanism to the renormalization of spin exchange interaction. Then I will switch gears and describe the demagnetization in Sr₂Cu₃O₄Cl₂ by resonant coupling between photons and magnons. I will end the thesis with a brief closing remark (Chapter VI).</p
Towards A Graphene Chip System For Blood Clotting Disease Diagnostics
Point of care diagnostics (POCD) allows the rapid, accurate measurement of analytes near to a patient. This enables faster clinical decision making and can lead to earlier diagnosis and better patient monitoring and treatment. However, despite many prospective POCD devices being developed for a wide range of diseases this promised technology is yet to be translated to a clinical setting due to the lack of a cost-effective biosensing platform.This thesis focuses on the development of a highly sensitive, low cost and scalable biosensor platform that combines graphene with semiconductor fabrication tech-niques to create graphene field-effect transistors biosensor. The key challenges of designing and fabricating a graphene-based biosensor are addressed. This work fo-cuses on a specific platform for blood clotting disease diagnostics, but the platform has the capability of being applied to any disease with a detectable biomarker.Multiple sensor designs were tested during this work that maximised sensor ef-ficiency and costs for different applications. The multiplex design enabled different graphene channels on the same chip to be functionalised with unique chemistry. The Inverted MOSFET design was created, which allows for back gated measurements to be performed whilst keeping the graphene channel open for functionalisation. The Shared Source and Matrix design maximises the total number of sensing channels per chip, resulting in the most cost-effective fabrication approach for a graphene-based sensor (decreasing cost per channel from £9.72 to £4.11).The challenge of integrating graphene into a semiconductor fabrication process is also addressed through the development of a novel vacuum transfer method-ology that allows photoresist free transfer. The two main fabrication processes; graphene supplied on the wafer “Pre-Transfer” and graphene transferred after met-allisation “Post-Transfer” were compared in terms of graphene channel resistance and graphene end quality (defect density and photoresist). The Post-Transfer pro-cess higher quality (less damage, residue and doping, confirmed by Raman spec-troscopy).Following sensor fabrication, the next stages of creating a sensor platform involve the passivation and packaging of the sensor chip. Different approaches using dielec-tric deposition approaches are compared for passivation. Molecular Vapour Deposi-tion (MVD) deposited Al2O3 was shown to produce graphene channels with lower damage than unprocessed graphene, and also improves graphene doping bringing the Dirac point of the graphene close to 0 V. The packaging integration of microfluidics is investigated comparing traditional soft lithography approaches and the new 3D printed microfluidic approach. Specific microfluidic packaging for blood separation towards a blood sampling point of care sensor is examined to identify the laminar approach for lower blood cell count, as a method of pre-processing the blood sample before sensing.To test the sensitivity of the Post-Transfer MVD passivated graphene sensor de-veloped in this work, real-time IV measurements were performed to identify throm-bin protein binding in real-time on the graphene surface. The sensor was function-alised using a thrombin specific aptamer solution and real-time IV measurements were performed on the functionalised graphene sensor with a range of biologically relevant protein concentrations. The resulting sensitivity of the graphene sensor was in the 1-100 pg/ml concentration range, producing a resistance change of 0.2% per pg/ml. Specificity was confirmed using a non-thrombin specific aptamer as the neg-ative control. These results indicate that the graphene sensor platform developed in this thesis has the potential as a highly sensitive POCD. The processes developed here can be used to develop graphene sensors for multiple biomarkers in the future
A suite of quantum algorithms for the shortestvector problem
Crytography has come to be an essential part of the cybersecurity infrastructure that provides a safe environment for communications in an increasingly connected world. The advent of quantum computing poses a threat to the foundations of the current widely-used cryptographic model, due to the breaking of most of the cryptographic algorithms used to provide confidentiality, authenticity, and more. Consequently a new set of cryptographic protocols have been designed to be secure against quantum computers, and are collectively known as post-quantum cryptography (PQC). A forerunner among PQC is lattice-based cryptography, whose security relies upon the hardness of a number of closely related mathematical problems, one of which is known as the shortest vector problem (SVP).
In this thesis I describe a suite of quantum algorithms that utilize the energy minimization principle to attack the shortest vector problem. The algorithms outlined span the gate-model and continuous time quantum computing, and explore methods of parameter optimization via variational methods, which are thought to be effective on near-term quantum computers. The performance of the algorithms are analyzed numerically, analytically, and on quantum hardware where possible. I explain how the results obtained in the pursuit of solving SVP apply more broadly to quantum algorithms seeking to solve general real-world problems; minimize the effect of noise on imperfect hardware; and improve efficiency of parameter optimization.Open Acces
The Adirondack Chronology
The Adirondack Chronology is intended to be a useful resource for researchers and others interested in the Adirondacks and Adirondack history.https://digitalworks.union.edu/arlpublications/1000/thumbnail.jp
Physical phenomena controlling quiescent flame spread in porous wildland fuel beds
Despite well-developed solid surface flame spread theories, we still lack a coherent theory to describe flame spread through porous wildland fuel beds. This porosity results in additional complexity, reducing the thermal conductivity of the fuel bed, but allowing in-bed radiative and convective heat transfer to occur. While previous studies have explored the effect of fuel bed structure on the overall fire behaviour, there remains a need for further investigation of the effect of fuel structure on the underlying physical phenomena controlling flame spread. Through an extensive series of laboratory-based experiments, this thesis provides detailed, physics-based insights for quiescent flame spread through natural porous beds, across a range of structural conditions.
Measurements are presented for fuel beds representative of natural field conditions within an area of the fire-prone New Jersey Pinelands National Reserve, which compliment a related series of field experiments conducted as part of a wider research project. Additional systematic investigation across a wider range of fuel conditions identified independent effects of fuel loading and bulk density on the spread rate, flame height and heat release rate. However, neither fuel loading nor bulk density alone provided adequate prediction of the resulting fire behaviour. Drawing on existing structural descriptors (for both natural and engineered fuel beds) an alternative parameter ασδ was proposed. This parameter (incorporating the fuel bed porosity (α), fuel element surface-to-volume ratio (σ), and the fuel bed height (δ)) was strongly correlated with the spread rate.
One effect of the fuel bed structure is to influence the heat transfer mechanisms both above and within the porous fuel bed. Existing descriptions of radiation transport through porous fuel beds are often predicated on the assumption of an isotropic fuel bed. However, given their preferential angle of inclination, the pine needle beds in this study may not exhibit isotropic behaviour.
Regardless, for the structural conditions investigated, horizontal heat transfer through the fuel bed was identified as the dominant heating mechanism within this quiescent flame spread scenario. However, the significance of heat transfer contributions from the above-bed flame generally increased with increasing ασδ value of the fuel bed. Using direct measurements of the heat flux magnitude and effective heating distance, close agreement was observed between experimentally observed spread rates and a simple thermal model considering only radiative heat transfer through the fuel bed, particularly at lower values of ασδ. Over-predictions occurred at higher ασδ values, or where other heat transfer terms were incorporated, which may highlight the need to include additional heat loss terms.
A significant effect of fuel structure on the primary flow regimes, both within and above these porous fuel beds, was also observed, with important implications for the heat transfer and oxygen supply within the fuel bed. Independent effects of fuel loading and bulk density on both the buoyant and buoyancy-driven entrainment flow were observed, with a complex feedback cycle occurring between Heat Release Rate (HRR) and combustion behaviour. Generally, increases in fuel loading resulted in increased HRR, and therefore increased buoyant flow velocity, along with an increase in the velocity of flow entrained towards the combustion region.
The complex effects of fuel structure in both the flaming and smouldering combustion phases may necessitate modifications to other common modelling approaches. The widely used Rothermel model under-predicted spread rate for higher bulk density and lower ασδ fuel beds. As previously suggested, an over-sensitivity to fuel bed height was observed, with experimental comparison indicating an under-prediction of reaction intensity at lower fuel heights. These findings have important implications particularly given the continuing widespread use of the Rothermel model, which continues to underpin elements of the BehavePlus fire modelling system and the US National Fire Danger Rating System.
The physical insights, and modelling approaches, developed for this low-intensity, quiescent flame spread scenario, are applicable to common prescribed fire activities. It is hoped that this work (alongside complimentary laboratory and field experiments conducted by various authors as part of a wider multi-agency project (SERDP-RC2641)) will contribute to the emerging field of prescribed fire science, and help to address the pressing need for further development of fire prediction and modelling tools
Optimising acoustic cavitation for industrial application
The ultrasonic horn is one of the most commonly used acoustic devices in laboratories and industry. For its efficient application to cavitation mediated process, the cavitation generated at its tip as a function of its tip-vibration amplitudes still needed to be studied in detail. High-speed imaging and acoustic detection are used to investigate the cavitation generated at the tip of an ultrasonic horn, operating at a fundamental frequency, f0, of 20 kHz. Tip-vibration amplitudes are sampled at fine increments across the range of input powers available. The primary bubble cluster under the tip is found to undergo subharmonic periodic collapse, with concurrent shock wave emission, at frequencies of f0/m, with m increasing through integer values with increasing tip-vibration amplitude. The contribution of periodic shock waves to the noise spectra of the acoustic emissions is confirmed. Transitional input powers for which the value of m is indistinct, and shock wave emission irregular and inconsistent, are identified through Vrms of the acoustic detector output. For cavitation applications mediated by bubble collapse, sonications at transitional powers may lead to inefficient processing. The ultrasonic horn is also deployed to investigate the role of shock waves in the fragmentation of intermetallic crystals, nominally for ultrasonic treatment of Aluminium melt, and in a novel two-horn configuration for potential cavitation enhancement effects. An experiment investigating nitrogen fixation via cavitation generated by focused ultrasound exposures is also described. Vrms from the acoustic detector is again used to quantify the acoustic emissions for comparison to the sonochemical nitrite yield and for optimisation of sonication protocols at constant input energy. The findings revealed that the acoustic cavitation could be enhanced at constant input energy through optimisation of the pulse duration and pulse interval. Anomalous results may be due to inadequate assessment for the nitrate generated. The studies presented in this thesis have illustrated means of improving the cavitation efficiency of the used acoustic devices, which may be important to some selected industrial processes
Optical coherence tomography methods using 2-D detector arrays
Optical coherence tomography (OCT) is a non-invasive, non-contact optical technique that allows cross-section imaging of biological tissues with high spatial resolution, high sensitivity and high dynamic range. Standard OCT uses a focused beam to illuminate a point on the target and detects the signal using a single photodetector. To acquire transverse information, transversal scanning of the illumination point is required. Alternatively, multiple OCT channels can be operated in parallel simultaneously; parallel OCT signals are recorded by a two-dimensional (2D) detector array. This approach is known as Parallel-detection OCT. In this thesis, methods, experiments and results using three parallel OCT techniques, including full -field (time-domain) OCT (FF-OCT), full-field swept-source OCT (FF-SS-OCT) and line-field Fourier-domain OCT (LF-FD-OCT), are presented. Several 2D digital cameras of different formats have been used and evaluated in the experiments of different methods. With the LF-FD-OCT method, photography equipment, such as flashtubes and commercial DSLR cameras have been equipped and tested for OCT imaging. The techniques used in FF-OCT and FF-SS-OCT are employed in a novel wavefront sensing technique, which combines OCT methods with a Shack-Hartmann wavefront sensor (SH-WFS). This combination technique is demonstrated capable of measuring depth-resolved wavefront aberrations, which has the potential to extend the applications of SH-WFS in wavefront-guided biomedical imaging techniques
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Novel delivery and sample mixing for synchrotron diffraction experiments using acoustic levitation with multi-transducer arrays
Acoustic levitation may utilise standing waves at ultrasonic frequencies to manipulate suspended substances and small objects in a contactless manner. These materials may be levitated in the positions in which the nodes are located, corresponding to positions of low acoustic pressure. In recent years, off the shelf transducer based acoustic levitators have been used for contactless manipulation of liquids. These systems benefit from requiring low power and low-cost components making acoustic levitation more accessible to the masses. Such a system was investigated in this work for presenting protein crystals, within their mother liquor, to the I24 beamline at Diamond Light Source for x-ray diffraction experiments. It was found that the crystals tended to sediment toward the bottom of the droplets, which were oblate in shape. The droplets which were levitated often became unstable and fell from their suspended position, or they would not detach from the pipette tip when they were being injected. To rectify this, a coating of silicone oil was added allowing the droplets to remain stable as well as limit the evaporation of the droplet whilst it was manually inserted and the area cleared of personnel before the x-ray beam was engaged. This silicone oil coating is non-crystalline and thus did not invalidate the results collected which showed the lysozyme crystal structure with a resolution of 1.69 A, confirming acoustic levitation as a good sample presentation method for these types of experiments. To remove the requirement for the silicone oil, a bespoke system was created named the DLS-Lev that allowed top-loading of the sample. The droplets of mother liquor which contained protein crystals were easily detached from the pipette tip into the traps within the DLS-Lev system owing to the increased strength of the traps in the modified design. This system, paired with an automated pipette, facilitated sample mixing experiments whilst the x-ray beam was engaged. The further development of the pipetting system was halted due to the COVID-19 pandemic. However, future work should see the permanent installation of these systems at the I24 beamline at Diamond Light Source, as well as additional bespoke acoustic levitators designed for the other beamlines specialising in the research of protein structure via x-ray scattering techniques
Flexographic printed nanogranular LBZA derived ZnO gas sensors: Synthesis, printing and processing
Within this document, investigations of the processes towards the production of a flexographic printed ZnO gas sensor for breath H2 analysis are presented. Initially, a hexamethylenetetramine (HMTA) based, microwave assisted, synthesis method of layered basic zinc acetate (LBZA) nanomaterials was investigated. Using the synthesised LBZA, a dropcast nanogranular ZnO gas sensor was produced. The testing of the sensor showed high sensitivity towards hydrogen with response (Resistanceair/ Resistancegas) to 200 ppm H2 at 328 °C of 7.27. The sensor is highly competitive with non-catalyst surface decorated sensors and sensitive enough to measure current H2 guideline thresholds for carbohydrate malabsorption (Positive test threshold: 20 ppm H2, Predicted response: 1.34). Secondly, a novel LBZA synthesis method was developed, replacing the HMTA by NaOH. This resulted in a large yield improvement, from a [OH-] conversion of 4.08 at% to 71.2 at%. The effects of [OH-]/[Zn2+] ratio, microwave exposure and transport to nucleation rate ratio on purity, length, aspect ratio and polydispersity were investigated in detail. Using classical nucleation theory, analysis of the basal layer charge symmetries, and oriented attachment theory, a dipole-oriented attachment reaction mechanism is presented. The mechanism is the first theory in literature capable of describing all observed morphological features along length scales. The importance of transport to nucleation rate ratio as the defining property that controls purity and polydispersity is then shown. Using the NaOH derived LBZA, a flexographic printing ink was developed, and proof-of-concept sensors printed. Gas sensing results showed a high response to 200 ppm H2 at 300 °C of 60.2. Through IV measurements and SEM analysis this was shown to be a result of transfer of silver between the electrode and the sensing layer during the printing process. Finally, Investigations into the intense pulsed light treatment of LBZA were conducted. The results show that dehydration at 150 °C prior to exposure is a requirement for successful calcination, producing ZnO quantum dots (QDs) in the process. SEM measurements show mean radii of 1.77-2.02 nm. The QDs show size confinement effects with the exciton blue shifting by 0.105 eV, and exceptionally low defect emission in photoluminescence spectra, indicative of high crystalline quality, and high conductivity. Due to the high crystalline quality and amenity to printing, the IPL ZnO QDs have numerous potential uses ranging from sensing to opto-electronic devices
Fotónica aplicada a la monitorización de procesos y al desarrollo de sensores en la industria agroalimentaria
Tesis por compendio[ES] El objetivo de la presente tesis es el de desarrollar y utilizar técnicas basadas en la fotónica de baja frecuencia, como la radiofrecuencia, las microondas y los infrarrojos, para monitorizar de forma no destructiva procesos utilizados en la industria agroalimentaria, desde el punto de vista de la termodinámica irreversible. Estudiar los distintos fenómenos que ocurren durante la operación de deshidratación de patata mediante el secado con aire caliente combinado con microondas, utilizando la termografía infrarroja para monitorizar los perfiles de temperatura superficial que presenta la muestra, la espectrofotometría en el rango de las microondas y la termodinámica irreversible para modelizar el proceso. Desarrollar un sistema de monitorización de la congelación de la carne de pollo, que permita obtener datos del proceso a tiempo real y de forma no invasiva mediante la espectrofotometría en el rango de la radiofrecuencia y la termografía infrarroja. A su vez, con esos datos se modelizará el comportamiento del producto a lo largo del proceso de congelación, utilizando los principios de la termodinámica irreversible para estimar los distintos fenómenos que ocurren. Desarrollar una herramienta de predicción de los distintos estados del agua y la sacarosa durante el proceso de caramelizado de manzanas, basada en las propiedades dieléctricas obtenidas mediante la espectrofotometría en el rango de las microondas. Diseñar y desarrollar un sensor basado en las propiedades dieléctricas en el rango de la radiofrecuencia, capaz de monitorizar en tiempo real y de forma no invasiva con el medio las cinéticas de liberación de compuestos encapsulados en matrices de alginato en un medio líquido. Utilizando este nuevo sensor se pueden modelizar y estudiar las cinéticas de liberación y utilizarse para diseñar la encapsulación de compuestos.[CA] L'objectiu de la present tesi és el de desenvolupar i utilitzar tècniques basades en la fotònica de baixa freqüència, com ara la radiofreqüència, les microones i els infrarojos, per monitoritzar de forma no destructiva processos utilitzats a la indústria agroalimentària, des del punt de vista de la termodinàmica irreversible. Estudiar els diferents fenòmens que ocorren durant l'operació de deshidratació de patata mitjançant l'assecat amb aire calent combinat amb microones, utilitzant la termografia infraroja per monitoritzar els perfils de temperatura superficial que presenta la mostra, l'espectrofotometria al rang de les microones i la termodinàmica irreversible per modelitzar el procés. Desenvolupar un sistema de monitorització de la congelació de la carn de pollastre, que permeti obtenir dades del procés a temps real i de manera no invasiva mitjançant l'espectrofotometria al rang de la radiofreqüència i la termografia infraroja. Alhora, amb aquestes dades es modelitzarà el comportament del producte al llarg del procés de congelació, utilitzant els principis de la termodinàmica irreversible per estimar els diferents fenòmens que ocorren. Desenvolupar una eina de predicció dels diferents estats de l'aigua i la sacarosa durant el procés de caramel·litzat de pomes, basada en les propietats dielèctrics obtingudes mitjançant l'espectrofotometria al rang de les microones. Dissenyar i desenvolupar un sensor basat en les propietats dielèctrics al rang de la radiofreqüència, capaç de monitoritzar en temps real i de forma no invasiva amb el medi les cinètiques d'alliberament de compostos encapsulats en matrius d'alginat en un medi líquid. Utilitzant aquest sensor nou es poden modelitzar i estudiar les cinètiques d'alliberament i utilitzar-se per dissenyar l'encapsulació de compostos.[EN] The objective of this thesis is to develop and use techniques based on low-frequency photonics, such as radiofrequency, microwaves and infrared, to non-destructively monitor processes used in the agri-food industry, from the point of view of irreversible thermodynamics. To study the different phenomena that occur during the potato dehydration operation by drying with hot air combined with microwaves, using infrared thermography to monitor the surface temperature profiles of the sample, spectrophotometry in the microwave range and thermodynamics. irreversible to model the process. Develop a monitoring system for the freezing of chicken meat, which allows data to be obtained from the process in real time and non-invasively through spectrophotometry in the radiofrequency range and infrared thermography. In turn, with these data, the behavior of the product will be modeled throughout the freezing process, using the principles of irreversible thermodynamics to estimate the different phenomena that occur. To develop a prediction tool for the different states of water and sucrose during the candying process of apples, based on the dielectric properties obtained by spectrophotometry in the microwave range. Design and develop a sensor based on dielectric properties in the radiofrequency range, capable of monitoring in real time and non-invasively with the medium the release kinetics of compounds encapsulated in alginate matrices in a liquid medium. Using this new sensor, release kinetics can be modeled and studied and used to design the encapsulation of compounds.The authors acknowledge the financial support from THE SPANISH
MINISTERIO DE ECONOMÍA, INDUSTRIA Y COMPETITIVIDAD,
Programa Estatal de I+D+i orientada a los Retos de la Sociedad AGL2016-
80643-R, Agencia Estatal de Investigación (AEI) and Fondo Europeo de
Desarrollo Regional (FEDER). Juan Ángel Tomás-Egea wants to thank the FPI Predoctoral Program of the Universitat Politècnica de València for its support. This paper is part of the I+D+i PID2020-116816RB-I00 project,
funded by MCIN/ AEI/10.13039/501100011033.Tomás Egea, JÁ. (2022). Fotónica aplicada a la monitorización de procesos y al desarrollo de sensores en la industria agroalimentaria [Tesis doctoral]. Universitat Politècnica de València. https://doi.org/10.4995/Thesis/10251/182292TESISCompendi
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