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- Genre: Academic theses
- Creators: Goryll, Michael
Description
In the last few years, significant advances in nanofabrication have allowed tailoring of structures and materials at a molecular level enabling nanofabrication with precise control of dimensions and organization at molecular length scales, a development leading to significant advances in nanoscale systems. Although, the direction of progress seems to follow the path of microelectronics, the fundamental physics in a nanoscale system changes more rapidly compared to microelectronics, as the size scale is decreased. The changes in length, area, and volume ratios due to reduction in size alter the relative influence of various physical effects determining the overall operation of a system in unexpected ways. One such category of nanofluidic structures demonstrating unique ionic and molecular transport characteristics are nanopores. Nanopores derive their unique transport characteristics from the electrostatic interaction of nanopore surface charge with aqueous ionic solutions. In this doctoral research cylindrical nanopores, in single and array configuration, were fabricated in silicon-on-insulator (SOI) using a combination of electron beam lithography (EBL) and reactive ion etching (RIE). The fabrication method presented is compatible with standard semiconductor foundries and allows fabrication of nanopores with desired geometries and precise dimensional control, providing near ideal and isolated physical modeling systems to study ion transport at the nanometer level. Ion transport through nanopores was characterized by measuring ionic conductances of arrays of nanopores of various diameters for a wide range of concentration of aqueous hydrochloric acid (HCl) ionic solutions. Measured ionic conductances demonstrated two distinct regimes based on surface charge interactions at low ionic concentrations and nanopore geometry at high ionic concentrations. Field effect modulation of ion transport through nanopore arrays, in a fashion similar to semiconductor transistors, was also studied. Using ionic conductance measurements, it was shown that the concentration of ions in the nanopore volume was significantly changed when a gate voltage on nanopore arrays was applied, hence controlling their transport. Based on the ion transport results, single nanopores were used to demonstrate their application as nanoscale particle counters by using polystyrene nanobeads, monodispersed in aqueous HCl solutions of different molarities. Effects of field effect modulation on particle transition events were also demonstrated.
ContributorsJoshi, Punarvasu (Author) / Thornton, Trevor J (Thesis advisor) / Goryll, Michael (Thesis advisor) / Spanias, Andreas (Committee member) / Saraniti, Marco (Committee member) / Arizona State University (Publisher)
Created2011
Description
Solid-state nanopore research, used in the field of biomolecule detection and separation, has developed rapidly during the last decade. An electric field generated from the nanopore membrane to the aperture surface by a bias voltage can be used to electrostatically control the transport of charges. This results in ionic current rectification that can be used for applications such as biomolecule filtration and DNA sequencing.
In this doctoral research, a voltage bias was applied on the device silicon layer of Silicon-on-Insulator (SOI) cylindrical single nanopore to analyze how the perpendicular gate electrical field affected the ionic current through the pore. The nanopore was fabricated using electron beam lithography (EBL) and reactive ion etching (RIE) which are standard CMOS processes and can be integrated into any electronic circuit with massive production. The long cylindrical pore shape provides a larger surface area inside the aperture compared to other nanopores whose surface charge is of vital importance to ion transport.
Ionic transport through the nanopore was characterized by measuring the ionic conductance of the nanopore in aqueous hydrochloric acid and potassium chloride solutions under field effect modulation. The nanopores were separately coated with negatively charged thermal silicon oxide and positively charged aluminum oxide using Atomic Layer Deposition. Both layers worked as electrical insulation layers preventing leakage current once the substrate bias was applied. Different surface charges also provided different counterion-coion configurations. The transverse conductance of the nanopore at low electrolyte concentrations (<10-4 M) changed with voltage bias when the Debye length was comparable to the dimensions of the nanopore.
Ionic transport through nanopores coated with polyelectrolyte (PE) brushes were also investigated in ionic solutions with various pH values using Electrochemical Impedance spectroscopy (EIS). The pH sensitive poly[2–(dimethylamino) ethyl methacrylate] (PDMAEMA) PE brushes were integrated on the inner walls as well as the surface of the thermal oxidized SOI cylindrical nanopore using surface-initiated atom transfer radical polymerization (SI-ATRP). An equivalent circuit model was developed to extract conductive and resistive values of the nanopore in ionic solutions. The ionic conductance of PE coated nanopore was effectively rectified by varying the pH and gate bias.
In this doctoral research, a voltage bias was applied on the device silicon layer of Silicon-on-Insulator (SOI) cylindrical single nanopore to analyze how the perpendicular gate electrical field affected the ionic current through the pore. The nanopore was fabricated using electron beam lithography (EBL) and reactive ion etching (RIE) which are standard CMOS processes and can be integrated into any electronic circuit with massive production. The long cylindrical pore shape provides a larger surface area inside the aperture compared to other nanopores whose surface charge is of vital importance to ion transport.
Ionic transport through the nanopore was characterized by measuring the ionic conductance of the nanopore in aqueous hydrochloric acid and potassium chloride solutions under field effect modulation. The nanopores were separately coated with negatively charged thermal silicon oxide and positively charged aluminum oxide using Atomic Layer Deposition. Both layers worked as electrical insulation layers preventing leakage current once the substrate bias was applied. Different surface charges also provided different counterion-coion configurations. The transverse conductance of the nanopore at low electrolyte concentrations (<10-4 M) changed with voltage bias when the Debye length was comparable to the dimensions of the nanopore.
Ionic transport through nanopores coated with polyelectrolyte (PE) brushes were also investigated in ionic solutions with various pH values using Electrochemical Impedance spectroscopy (EIS). The pH sensitive poly[2–(dimethylamino) ethyl methacrylate] (PDMAEMA) PE brushes were integrated on the inner walls as well as the surface of the thermal oxidized SOI cylindrical nanopore using surface-initiated atom transfer radical polymerization (SI-ATRP). An equivalent circuit model was developed to extract conductive and resistive values of the nanopore in ionic solutions. The ionic conductance of PE coated nanopore was effectively rectified by varying the pH and gate bias.
ContributorsWang, Xiaofeng (Author) / Goryll, Michael (Thesis advisor) / Thornton, Trevor J (Committee member) / Christen, Jennifer M (Committee member) / Yu, Hongbin (Committee member) / Arizona State University (Publisher)
Created2015
Description
Engineered nanoporous substrates made using materials such as silicon nitride or silica have been demonstrated to work as particle counters or as hosts for nano-lipid bilayer membrane formation. These mechanically fabricated porous structures have thicknesses of several hundred nanometers up to several micrometers to ensure mechanical stability of the membrane. However, it is desirable to have a three-dimensional structure to ensure increased mechanical stability. In this study, circular silica shells used from Coscinodiscus wailesii, a species of diatoms (unicellular marine algae) were immobilized on a silicon chip with a micrometer-sized aperture using a UV curable polyurethane adhesive. The current conducted by a single nanopore of 40 nm diameter and 50 nm length, during the translocation of a 27 nm polystyrene sphere was simulated using COMSOL multiphysics and tested experimentally. The current conducted by a single 40 nm diameter nanopore of the diatom shell during the translocation of a 27 nm polystyrene sphere was simulated using COMSOL Multiphysics (28.36 pA) and was compared to the experimental measurement (28.69 pA) and Coulter Counting theory (29.95 pA).In addition, a mobility of 1.11 x 10-8 m2s-1V-1 for the 27 nm polystyrene spheres was used to convert the simulated current from spatial dependence to time dependence.
To achieve a sensing diameter of 1-2 nanometers, the diatom shells were used as substrates to perform ion-channel reconstitution experiments. The immobilized diatom shell was functionalized using silane chemistry and lipid bilayer membranes were formed. Functionalization of the diatom shell surface improves bilayer formation probability from 1 out of 10 to 10 out of 10 as monitored by impedance spectroscopy. Self-insertion of outer membrane protein OmpF of E.Coli into the lipid membranes could be confirmed using single channel recordings, indicating that nano-BLMs had formed which allow for fully functional porin activity. The results indicate that biogenic silica nanoporous substrates can be simulated using a simplified two dimensional geometry to predict the current when a nanoparticle translocates through a single aperture. With their tiered three-dimensional structure, diatom shells can be used in to form nano-lipid bilayer membranes and can be used in ion-channel reconstitution experiments similar to synthetic nanoporous membranes.
To achieve a sensing diameter of 1-2 nanometers, the diatom shells were used as substrates to perform ion-channel reconstitution experiments. The immobilized diatom shell was functionalized using silane chemistry and lipid bilayer membranes were formed. Functionalization of the diatom shell surface improves bilayer formation probability from 1 out of 10 to 10 out of 10 as monitored by impedance spectroscopy. Self-insertion of outer membrane protein OmpF of E.Coli into the lipid membranes could be confirmed using single channel recordings, indicating that nano-BLMs had formed which allow for fully functional porin activity. The results indicate that biogenic silica nanoporous substrates can be simulated using a simplified two dimensional geometry to predict the current when a nanoparticle translocates through a single aperture. With their tiered three-dimensional structure, diatom shells can be used in to form nano-lipid bilayer membranes and can be used in ion-channel reconstitution experiments similar to synthetic nanoporous membranes.
ContributorsRamakrishnan, Shankar (Author) / Goryll, Michael (Thesis advisor) / Blain Christen, Jennifer (Committee member) / Dey, Sandwip (Committee member) / Thornton, Trevor (Committee member) / Arizona State University (Publisher)
Created2015