Electrical properties of self-assembled metal-molecular networks: modelling, experiment and applications

dc.contributor.authorAmadi, Eberechukwu Victoria
dc.contributor.supervisorPapadopoulos, Christo
dc.date.accessioned2021-10-01T22:57:14Z
dc.date.available2021-10-01T22:57:14Z
dc.date.copyright2021en_US
dc.date.issued2021-10-01
dc.degree.departmentDepartment of Electrical and Computer Engineeringen_US
dc.degree.levelMaster of Applied Science M.A.Sc.en_US
dc.description.abstractComplementing electronic components with molecular analogs is a promising alternative to further miniaturization of conventional silicon electronic devices in the quest to achieve functional molecular nanoscale circuit elements. To this end, molecular units have been widely investigated to evaluate their suitability for future nanoelectronic circuit applications. Previous work has typically either focused on tightly packed layers of dithiol molecule-encapsulated gold nanoparticles or small oligomeric structures comprised of nanoparticles linked by a few dithiol molecules. In this thesis, we study the electrical and electronic properties of metal-molecular networks having an intermediate number of dithiol molecules both theoretically and experimentally. Electronic transport through self-assembled networks with tunable thiol molecule: gold nanoparticle ratios (ranging from 1:1 to 50:1) is studied using two-terminal electrical characterization techniques. The tunability of the electrical properties (e.g., resistance, current etc.) of the molecular networks on modifying the thiol molecule: gold nanoparticle ratios and/or type of molecule used was observed. Specifically, the current in the molecular networks studied typically decreased with increasing molecule: AuNP. For example, in gold-benzenedithiol molecular networks with approximately the same length-to-width ratios, current at low bias, 0.3 V, was found to decrease from the μA range in 1:1 ratio samples to the nA range in 50:1 samples. Additionally, many gold-benzenedithiol molecular networks which had linear I-V characteristics at low biases displayed nonlinearities in their I-Vs at higher biases. In such cases, the nonlinearities in the I-Vs at higher biases became more pronounced with increasing molecule: AuNP ratio. For example, in a control sample, consisting of only gold nanoparticles, linear I-V behaviour was observed, while the 50:1 gold-benzenedithiol molecular network displayed NDR with a measured peak-to-valley ratio of approximately 1.52. A linear resistor circuit model provided accurate approximations of the low bias I-V behaviour of the molecular networks. Experimental studies were complemented with first principles density functional theory-based simulations of the molecular networks. Linear chains and branched networks of interconnected benzenedithiol molecules and Au6 clusters were the systems of interest in this study. Calculated current-voltage characteristics of the metal-molecular networks exhibited nonlinearities and rectification with negative differential resistance (NDR) peaks that became more pronounced with increasing chain length of the linear chains. Peak-to-valley current NDR ratios as large as ~ 500 and rectification ratios of ~ 10 (0.25 V) were shown for linear and branched circuit elements, respectively, illustrating how charge transport through molecular-scale devices could be controlled with precision by modifying the structure and geometry of molecule-nanoparticle networks. Observed nonlinearities (e.g., NDR, hysteresis, and rectification) in the I-Vs of the self-assembled metal-molecular networks studied highlight their potential for application as circuit elements in future nanoelectronic devices and circuits, including memory, logic, switching and sensing. Additionally, the device level physical randomness and imperfections induced during fabrication of the metal-molecular networks, as well as the variability of the resistance of the networks on modifying the molecule: gold nanoparticle ratios can be applied for generating random binary sequences.en_US
dc.description.scholarlevelGraduateen_US
dc.identifier.bibliographicCitationA. Venkataraman, E. V. Amadi, T. S. M. Zaborniak, P. Zhang and C. Papadopoulos, "Negative Differential Resistance and Hysteresis in Self-Assembled Nanoscale Networks with Tunable Molecule-to-Nanoparticle Ratios," physica status solidi (b), vol. 257, p. 2000019, 2020.en_US
dc.identifier.bibliographicCitationE. Amadi, V. Anusha, T. Zaborniak and C. Papadopoulos, "Nanoelectronic circuit elements based on metal-molecular networks," in ACS Spring Meeting 2021, 2021.en_US
dc.identifier.bibliographicCitationA. Venkataraman, E. Amadi, P. Zhang and C. Papadopoulos, "Random key generation using self-assembled nanoparticle-molecular networks," in ACS Spring Meeting 2021, 2021.en_US
dc.identifier.bibliographicCitationE. V. Amadi, A. Venkataraman, T. S. M. Zaborniak and C. Papadopoulos, "Nanoelectronic Circuit Elements Based on Nanoscale Metal-Molecular Networks," Journal of Computational Electronics, 2021.en_US
dc.identifier.bibliographicCitationA. Venkataraman, E. V. Amadi and C. Papadopoulos, "Hardware security using self-assembled nanoelectronic networks," Small, 2021.en_US
dc.identifier.bibliographicCitationA. Venkataraman, E. V. Amadi, Y. Chen and C. Papadopoulos, "Carbon Nanotube Assembly and Integration for Applications," Nanoscale research letters, vol. 14, pp. 220-220, 2019.en_US
dc.identifier.bibliographicCitationA. Venkataraman, E. V. Amadi and C. Papadopoulos, "Nanoscale self-assembly : concepts, applications, and challenges," IOP Publishing, 2021.en_US
dc.identifier.urihttp://hdl.handle.net/1828/13438
dc.languageEnglisheng
dc.language.isoenen_US
dc.rightsAvailable to the World Wide Weben_US
dc.subjectself-assemblyen_US
dc.subjectmetal-molecular networksen_US
dc.subjectmolecular electronicsen_US
dc.subjectnegative differential resistanceen_US
dc.subjectdensity functional theoryen_US
dc.titleElectrical properties of self-assembled metal-molecular networks: modelling, experiment and applicationsen_US
dc.typeThesisen_US

Files

Original bundle
Now showing 1 - 1 of 1
Loading...
Thumbnail Image
Name:
Amadi_Eberechukwu_MASc_2021.pdf
Size:
5.32 MB
Format:
Adobe Portable Document Format
Description:
License bundle
Now showing 1 - 1 of 1
No Thumbnail Available
Name:
license.txt
Size:
2 KB
Format:
Item-specific license agreed upon to submission
Description: