• Schrader, Paul
• Cole-Filipiak, Neil
• Talin, Albert Alec
• Krishnakumar, Raga
• Spataru, Catalin D.
• Bhandarkar, Austin
• Bennett, Christopher H.
• Foster, Michael E.
• Robinson, Donald A.
• Ramasesha, Krupa
• Fuller, Elliot J.
• Stavila, Vitalie
• Allendorf, Mark D.

Abstract

This project was broadly motivated by the need for new hardware that can process information such as images and sounds right at the point of where the information is sensed (e.g. edge computing). The project was further motivated by recent discoveries by group demonstrating that while certain organic polymer blends can be used to fabricate elements of such hardware, the need to mix ionic and electronic conducting phases imposed limits on performance, dimensional scalability and the degree of fundamental understanding of how such devices operated. As an alternative to blended polymers containing distinct ionic and electronic conducting phases, in this LDRD project we have discovered that a family of mixed valence coordination compounds called Prussian blue analogue (PBAs), with an open framework structure and ability to conduct both ionic and electronic charge, can be used for inkjet-printed flexible artificial synapses that reversibly switch conductance by more than four orders of magnitude based on electrochemically tunable oxidation state. Retention of programmed states is improved by nearly two orders of magnitude compared to the extensively studied organic polymers, thus enabling in-memory compute and avoiding energy costly off-chip access during training. We demonstrate dopamine detection using PBA synapses and biocompatibility with living neurons, evoking prospective application for brain - computer interfacing. By application of electron transfer theory to in-situ spectroscopic probing of intervalence charge transfer, we elucidate a switching mechanism whereby the degree of mixed valency between N-coordinated Ru sites controls the carrier concentration and mobility, as supported by density functional theory (DFT) .

Topics

• density
• impedance spectroscopy
• compound
• phase
• mobility
• theory
• density functional theory
• biocompatibility
• polymer blend