Document Type

Dissertation

Degree

Doctor of Philosophy (PhD)

Major/Program

Physics

First Advisor's Name

Jin He

First Advisor's Committee Title

Committee chair

Second Advisor's Name

Prem P. Chapagain

Second Advisor's Committee Title

Committee member

Third Advisor's Name

Xuewen Wang

Third Advisor's Committee Title

Committee member

Fourth Advisor's Name

Chunlei Wang

Fourth Advisor's Committee Title

Committee member

Keywords

Nanoelelctrode collisions, Analytical methods, Nanopores, Single-entity analysis, Potential sensing, Nanotechnology, Nanopipette

Date of Defense

6-26-2020

Abstract

Complex biological processes occur in the nanoscale (1-100 nm) regime. ‘DNA’ which is just 2 nm in dimension is a fundamental building block of all life. ‘Hemoglobin’, a blood protein that transports oxygen throughout our body is only 5 nm in diameter. Importantly, the structure, composition, and dynamics of these nanoscale entities determine their biological function. A slight alteration in the structure and composition can lead to the malfunction of the protein which is key to various diseases including cancer. Therefore, the single-molecule measurement approach is essential to characterize both the average properties and the rare and dynamic changes of these nanoscale entities. This dissertation focused on the development of a novel single-entity method by fabricating nanopore and nanoelectrode integrated nanopipette for multi-mode electroanalytical detection of individual nanoparticles (NPs) and biomolecules.

The multifunctional nanopipette was fabricated, characterized, and initially used to study model NPs. First, polystyrene (PS) NPs was studied as it mimics the dielectric nature of the biomolecules. Hybrid dielectrophoretic (DEP) method was developed to efficiently preconcentrate the PS NPs to form large assemblies outside the nanopipette tip, for high-throughput single-NP detection and analysis. Second, a highly effective and facile electroanalytical method was developed to differentiate metallic NPs and dielectric NPs in solution based on their polarizability by implementing single-NP collision events at the nanoelectrode (‘nanoimpact’). Third, the multifunctional nanopipette was used to probe magneto-electric NPs (MENPs) composed of a piezoelectric shell and a ferromagnetic core. For the first time, the nanopipette based electrochemical single-entity approach was used to probe AC B-field induced strain mediated surface potential enhancement on a MENP surface via “nanoimpact’. The results confirmed that the AC B-field stimulation caused localized surface potential enhancement of MENP. This observation is associated with the presence of a piezoelectric shell whereas magnetic NPs were found unaffected under the identical stimulation. Finally, the nanopipette was used to probe proteins at the single-molecule level. We demonstrated a facile yet highly sensitive ‘nanoimpact’ based potentiometric method of detecting electrochemically inactive bio-macromolecules, by sensing open circuit potential (OCP) change when they approach towards and/or collides with and/or scatter away from the nanoelectrode of the nanopipette.

In summary, this dissertation presents the fabrication, development, and optimization of multifunctional nanopipette based electroanalytical biosensing platforms. First, it presents a systematic study using model NPs and later expands its use for biomolecule studies. With both experimental and simulation results, this dissertation announces a facile, cost-effective, versatile, sensitive, easy integration with scanning probe technique, robust and label-free electroanalytical sensing method to study individual NPs including biomolecules based on a charge sensing mechanism. The nanopipette based multi-mode biosensing platform developed in this project has great potential to be used as a smart sensor for various biomedical applications, health monitoring, quality control, and environmental sensing.

Identifier

FIDC009024

ORCID

0000-0002-1899-3480

Previously Published In

1. Pandey, P.; Panday, N.; Chang, S.; Pang, P.; Garcia, J.; Wang, X.; Fu, Q.; He, J., Probing Dynamic Events of Dielectric Nanoparticles by a Nanoelectrode-Nanopore Nanopipette. ChemElectroChem 2018, 5 (20), 3102-3112.

2. Pandey, P.; Garcia, J.; Guo, J.; Wang, X.; Yang, D.; He, J., Differentiation of metallic and dielectric nanoparticles in solution by single nanoparticle collision events at the nanoelectrode. Nanotechnology 2019, 31 (1), 015503.

3. Panday, N.; Qian, G.; Wang, X.; Chang, S.; Pandey, P.; He, J., Simultaneous Ionic Current and Potential Detection of Nanoparticles by a Multifunctional Nanopipette. ACS Nano 2016, 10 (12), 11237-11248.

4. Pandey, P., et al., Single-entity approach to investigate surface charge enhancement in magnetoelectric nanoparticles induced by AC magnetic field stimulation. ACS Sensors, 2020.

Available for download on Sunday, June 05, 2022

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