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Description
Human breath is a concoction of thousands of compounds having in it a breath-print of physiological processes in the body. Though breath provides a non-invasive and easy to handle biological fluid, its analysis for clinical diagnosis is not very common. Partly the reason for this absence is unavailability of cost effective and convenient tools for such analysis. Scientific literature is full of novel sensor ideas but it is challenging to develop a working device, which are few. These challenges include trace level detection, presence of hundreds of interfering compounds, excessive humidity, different sampling regulations and personal variability. To meet these challenges as well as deliver a low cost solution, optical sensors based on specific colorimetric chemical reactions on mesoporous membranes have been developed. Sensor hardware utilizing cost effective and ubiquitously available light source (LED) and detector (webcam/photo diodes) has been developed and optimized for sensitive detection. Sample conditioning mouthpiece suitable for portable sensors is developed and integrated. The sensors are capable of communication with mobile phones realizing the idea of m-health for easy personal health monitoring in free living conditions. Nitric oxide and Acetone are chosen as analytes of interest. Nitric oxide levels in the breath correlate with lung inflammation which makes it useful for asthma management. Acetone levels increase during ketosis resulting from fat metabolism in the body. Monitoring breath acetone thus provides useful information to people with type1 diabetes, epileptic children on ketogenic diets and people following fitness plans for weight loss.
ContributorsPrabhakar, Amlendu (Author) / Tao, Nongjian (Thesis advisor) / Forzani, Erica (Committee member) / Lindsay, Stuart (Committee member) / Arizona State University (Publisher)
Created2013
Description
Measurements of the response of superconducting nanowire single photon detector (SNSPD) devices to changes in various forms of input power can be used for characterization of the devices and for probing device-level physics. Two niobium nitride (NbN) superconducting nanowires developed for use as SNSPD devices are embedded as the inductive (L) component in resonant inductor/capacitor (LC) circuits coupled to a microwave transmission line. The capacitors are low loss commercial chip capacitors which limit the internal quality factor of the resonators to approximately $Qi = 170$. The resonator quality factor, approximately $Qr = 23$, is dominated by the coupling to the feedline and limits the detection bandwidth to on the order of 1MHz. In our experiments with this first generation device, we measure the response of the SNSPD devices to changes in thermal and optical power in both the time domain and the frequency domain. Additionally, we explore the non-linear response of the devices to an applied bias current. For these nanowires, we find that the band-gap energy is $\Delta_0 \approx 1.1$meV and that the density of states at the Fermi energy is $N_0 \sim 10^{10}$/eV/$\mu$m$^3$.
We present the results of experimentation with a superconducting nanowire that can be operated in two detection modes: i) as a kinetic inductance detector (KID) or ii) as a single photon detector (SPD). When operated as a KID mode in linear mode, the detectors are AC-biased with tones at their resonant frequencies of 45.85 and 91.81MHz. When operated as an SPD in Geiger mode, the resonators are DC biased through cryogenic bias tees and each photon produces a sharp voltage step followed by a ringdown signal at the resonant frequency of the detector. We show that a high AC bias in KID mode is inferior for photon counting experiments compared to operation in a DC-biased SPD mode due to the small fraction of time spent near the critical current with an AC bias. We find a photon count rate of $\Gamma_{KID} = 150~$photons/s/mA in a critically biased KID mode and a photon count rate of $\Gamma_{SPD} = 10^6~$photons/s/mA in SPD mode.
This dissertation additionally presents simulations of a DC-biased, frequency-multiplexed readout of SNSPD devices in Advanced Design System (ADS), LTspice, and Sonnet. A multiplexing factor of 100 is achievable with a total count rate of $>5$MHz. This readout could enable a 10000-pixel array for astronomy or quantum communications. Finally, we present a prototype array design based on lumped element components. An early implementation of the array is presented with 16 pixels in the frequency range of 74.9 to 161MHz. We find good agreement between simulation and experimental data in both the time domain and the frequency domain and present modifications for future versions of the array.
We present the results of experimentation with a superconducting nanowire that can be operated in two detection modes: i) as a kinetic inductance detector (KID) or ii) as a single photon detector (SPD). When operated as a KID mode in linear mode, the detectors are AC-biased with tones at their resonant frequencies of 45.85 and 91.81MHz. When operated as an SPD in Geiger mode, the resonators are DC biased through cryogenic bias tees and each photon produces a sharp voltage step followed by a ringdown signal at the resonant frequency of the detector. We show that a high AC bias in KID mode is inferior for photon counting experiments compared to operation in a DC-biased SPD mode due to the small fraction of time spent near the critical current with an AC bias. We find a photon count rate of $\Gamma_{KID} = 150~$photons/s/mA in a critically biased KID mode and a photon count rate of $\Gamma_{SPD} = 10^6~$photons/s/mA in SPD mode.
This dissertation additionally presents simulations of a DC-biased, frequency-multiplexed readout of SNSPD devices in Advanced Design System (ADS), LTspice, and Sonnet. A multiplexing factor of 100 is achievable with a total count rate of $>5$MHz. This readout could enable a 10000-pixel array for astronomy or quantum communications. Finally, we present a prototype array design based on lumped element components. An early implementation of the array is presented with 16 pixels in the frequency range of 74.9 to 161MHz. We find good agreement between simulation and experimental data in both the time domain and the frequency domain and present modifications for future versions of the array.
ContributorsSchroeder, Edward, Ph.D (Author) / Mauskopf, Philip (Thesis advisor) / Chamberlin, Ralph (Committee member) / Lindsay, Stuart (Committee member) / Newman, Nathan (Committee member) / Easson, Damien (Committee member) / Arizona State University (Publisher)
Created2018
Description
Charge transport in molecular systems, including DNA (Deoxyribonucleic acid), is involved in many basic chemical and biological processes. Studying their charge transport properties can help developing DNA based electronic devices with many tunable functionalities. This thesis investigates the electric properties of double-stranded DNA, DNA G-quadruplex and dsDNA with modified base.
First, double-stranded DNA with alternating GC sequence and stacked GC sequence were measured with respect to length. The resistance of DNA sequences increases linearly with length, indicating a hopping transport mechanism. However, for DNA sequences with stacked GC, a periodic oscillation is superimposed on the linear length dependence, indicating a partial coherent transport. The result is supported by the finding of delocalization of the highest occupied molecular orbitals of Guanines from theoretical simulation and by fitting based on the Büttiker’s theory.
Then, a DNA G4-duplex structures with a G-quadruplex as the core and DNA duplexes as the arms were studied. Similar conductance values were observed by varying the linker positions, thus a charge splitter is developed. The conductance of the DNA G-tetrads structures was found to be sensitive to the π-stacking at the interface between the G-quadruplex and DNA duplexes by observing a higher conductance value when one duplex was removed and a polyethylene glycol (PEG) linker was added into the interface. This was further supported by molecular dynamic simulations.
Finally, a double-stranded DNA with one of the bases replaced by an anthraquinone group was studied via electrochemical STM break junction technique. Anthraquinone can be reversibly switched into the oxidized state or reduced state, to give a low conductance or high conductance respectively. Furthermore, the thermodynamics and kinetics properties of the switching were systematically studied. Theoretical simulation shows that the difference between the two states is due to a difference in the energy alignment with neighboring Guanine bases.
First, double-stranded DNA with alternating GC sequence and stacked GC sequence were measured with respect to length. The resistance of DNA sequences increases linearly with length, indicating a hopping transport mechanism. However, for DNA sequences with stacked GC, a periodic oscillation is superimposed on the linear length dependence, indicating a partial coherent transport. The result is supported by the finding of delocalization of the highest occupied molecular orbitals of Guanines from theoretical simulation and by fitting based on the Büttiker’s theory.
Then, a DNA G4-duplex structures with a G-quadruplex as the core and DNA duplexes as the arms were studied. Similar conductance values were observed by varying the linker positions, thus a charge splitter is developed. The conductance of the DNA G-tetrads structures was found to be sensitive to the π-stacking at the interface between the G-quadruplex and DNA duplexes by observing a higher conductance value when one duplex was removed and a polyethylene glycol (PEG) linker was added into the interface. This was further supported by molecular dynamic simulations.
Finally, a double-stranded DNA with one of the bases replaced by an anthraquinone group was studied via electrochemical STM break junction technique. Anthraquinone can be reversibly switched into the oxidized state or reduced state, to give a low conductance or high conductance respectively. Furthermore, the thermodynamics and kinetics properties of the switching were systematically studied. Theoretical simulation shows that the difference between the two states is due to a difference in the energy alignment with neighboring Guanine bases.
ContributorsXiang, Liming (Author) / Tao, Nongjian (Thesis advisor) / Lindsay, Stuart (Committee member) / Gould, Ian (Committee member) / Arizona State University (Publisher)
Created2016
Description
Single molecule identification is one essential application area of nanotechnology. The application areas including DNA sequencing, peptide sequencing, early disease detection and other industrial applications such as quantitative and quantitative analysis of impurities, etc. The recognition tunneling technique we have developed shows that after functionalization of the probe and substrate of a conventional Scanning Tunneling Microscope with recognition molecules ("tethered molecule-pair" configuration), analyte molecules trapped in the gap that is formed by probe and substrate will bond with the reagent molecules. The stochastic bond formation/breakage fluctuations give insight into the nature of the intermolecular bonding at a single molecule-pair level. The distinct time domain and frequency domain features of tunneling signals were extracted from raw signals of analytes such as amino acids and their enantiomers. The Support Vector Machine (a machine-learning method) was used to do classification and predication based on the signal features generated by analytes, giving over 90% accuracy of separation of up to seven analytes. This opens up a new interface between chemistry and electronics with immediate implications for rapid Peptide/DNA sequencing and molecule identification at single molecule level.
ContributorsZhao, Yanan, 1986- (Author) / Lindsay, Stuart (Thesis advisor) / Nemanich, Robert (Committee member) / Qing, Quan (Committee member) / Ros, Robert (Committee member) / Zhang, Peiming (Committee member) / Arizona State University (Publisher)
Created2014
Description
Understanding the interplay between the electrical and mechanical properties of single molecules is of fundamental importance for molecular electronics. The sensitivity of charge transport to mechanical fluctuations is a key problem in developing long lasting molecular devices. Furthermore, harnessing this response to mechanical perturbation, molecular devices which can be mechanically gated can be developed. This thesis demonstrates three examples of the unique electromechanical properties of single molecules.
First, the electromechanical properties of 1,4-benzenedithiol molecular junctions are investigate. Counterintuitively, the conductance of this molecule is found to increase by more than an order of magnitude when stretched. This conductance increase is found to be reversible when the molecular junction is compressed. The current-voltage, conductance-voltage and inelastic electron tunneling spectroscopy characteristics are used to attribute the conductance increase to a strain-induced shift in the frontier molecular orbital relative to the electrode Fermi level, leading to resonant enhancement in the conductance.
Next, the effect of stretching-induced structural changes on charge transport in DNA molecules is studied. The conductance of single DNA molecules with lengths varying from 6 to 26 base pairs is measured and found to follow a hopping transport mechanism. The conductance of DNA molecules is highly sensitive to mechanical stretching, showing an abrupt decrease in conductance at surprisingly short stretching distances, with weak dependence on DNA length. This abrupt conductance decrease is attributed to force-induced breaking of hydrogen bonds in the base pairs at the end of the DNA sequence.
Finally, the effect of small mechanical modulation of the base separation on DNA conductance is investigated. The sensitivity of conductance to mechanical modulation is studied for molecules of different sequence and length. Sequences with purine-purine stacking are found to be more responsive to modulation than purine-pyrimidine sequences. This sensitivity is attributed to the perturbation of &pi-&pi stacking interactions and resulting effects on the activation energy and electronic coupling for the end base pairs.
First, the electromechanical properties of 1,4-benzenedithiol molecular junctions are investigate. Counterintuitively, the conductance of this molecule is found to increase by more than an order of magnitude when stretched. This conductance increase is found to be reversible when the molecular junction is compressed. The current-voltage, conductance-voltage and inelastic electron tunneling spectroscopy characteristics are used to attribute the conductance increase to a strain-induced shift in the frontier molecular orbital relative to the electrode Fermi level, leading to resonant enhancement in the conductance.
Next, the effect of stretching-induced structural changes on charge transport in DNA molecules is studied. The conductance of single DNA molecules with lengths varying from 6 to 26 base pairs is measured and found to follow a hopping transport mechanism. The conductance of DNA molecules is highly sensitive to mechanical stretching, showing an abrupt decrease in conductance at surprisingly short stretching distances, with weak dependence on DNA length. This abrupt conductance decrease is attributed to force-induced breaking of hydrogen bonds in the base pairs at the end of the DNA sequence.
Finally, the effect of small mechanical modulation of the base separation on DNA conductance is investigated. The sensitivity of conductance to mechanical modulation is studied for molecules of different sequence and length. Sequences with purine-purine stacking are found to be more responsive to modulation than purine-pyrimidine sequences. This sensitivity is attributed to the perturbation of &pi-&pi stacking interactions and resulting effects on the activation energy and electronic coupling for the end base pairs.
ContributorsBruot, Christopher, 1986- (Author) / Tao, Nongjian (Thesis advisor) / Lindsay, Stuart (Committee member) / Mujica, Vladimiro (Committee member) / Ferry, David (Committee member) / Arizona State University (Publisher)
Created2014