Polyoxometalate nanoscale electronic devices

Abstract

Electronic memories play a crucial role in our ever more digital world. Traditional tech-
nologies are reaching their limits as new computing paradigms continue to increase
their demand for computing power, efficiency, and miniaturisation. Resistive random
access memories (RRAM) have emerged as promising candidates to solve these issues.
Specifically, polyoxometalate (POM) -based devices show particular potential due to
their rich redox properties.
This thesis explores the development of POM-based nanoscale electronic devices for
next-generation memory applications and neuromorphic computing. Throughout this
work, I show that the phosphomolybdate POM, H3PMo12O40 is promising: it demon-
strates rich redox activity especially when carefully deposited in nanogap separated
Al/Au asymmetric coplanar electrodes. By adding a thin poly(methyl methacrylate)
(PMMA) layer between the metal electrodes and the POM film, device performance
can be enhanced, while addressing challenges such as device-to-device and cycle-to-
cycle variations. My analysis reveals that a complex combination of factors explains
the switching mechanism of these devices including: the POM redox reactions, envi-
ronmental factors such as moisture, and device structure-related effects.
I showcase the ability of these devices to mimic some operation of the biological brain
and specific neural responses such as nociception, opening new possibilities for artifi-
cial neural network technologies.
This work advances the field of nanoelectronics by optimising both device architecture
and material selection. My findings pave the way for the development of more effi-
cient and tuneable bio-inspired computing systems. These POM-based devices offer
solutions to overcome current technology limitations, potentially shaping future elec-
tronic systems.

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Identifiers

ORCID for Emilie Anne Gerouville: orcid.org/0000-0003-2569-5198

ORCID for Dimitra Georgiadou: orcid.org/0000-0002-2620-3346

ORCID for Nicholas Harris: orcid.org/0000-0003-4122-2219

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