Dual-biased metal oxide electrolyte-gated thin-film transistors for enhanced protonation in complex biofluids

Sci Rep. 2024 Dec 28;14(1):30772. doi: 10.1038/s41598-024-80005-0.

Abstract

pH sensing technology is pivotal for monitoring aquatic ecosystems and diagnosing human health conditions. Indium-gallium-zinc oxide electrolyte-gated thin-film transistors (IGZO EGTFTs) are highly regarded as ion-sensing devices due to the pH-dependent surface chemistry of their sensing membranes. However, applying EGTFT-based pH sensors in complex biofluids containing diverse charged species poses challenges due to ion interference and inherently low sensitivity constrained by the Nernst limit. Here, we propose a dual-biased (DB) EGTFT pH sensing platform, acquiring back-gate-assisted sensitivity enhancement and recyclable redox-coupled protonation at the semiconductor-biofluid interface. A solution-processed amorphous IGZO film, used as the proton-sensitive membrane, ensures scalable uniformity across a 6-inch wafer. These devices demonstrate exceptional pH resistivity over several hours when submerged in solutions with pH levels of 4 and 8. In-depth electrochemical investigations reveal that back-gate bias significantly enhances sensitivity beyond the Nernst limit, reaching 85 mV/pH. This improvement is due to additional charge accumulation in the channel, which expands the sensing window. As a proof of concept, we observe consistent variations in threshold voltage during repeated pH cycles, not only in standard solutions but also in physiological electrolytes such as phosphate-buffered saline (PBS) and artificial urine, confirming the potential for reliable operation in complex biological environments.

Keywords: Back-gate effect; Biofluids; Dual-biased electrolyte-gated thin-film transistors; Oxide semiconductor; pH sensor.

MeSH terms

  • Biosensing Techniques / instrumentation
  • Biosensing Techniques / methods
  • Body Fluids / chemistry
  • Body Fluids / metabolism
  • Electrochemical Techniques / methods
  • Electrolytes* / chemistry
  • Gallium / chemistry
  • Humans
  • Hydrogen-Ion Concentration
  • Indium* / chemistry
  • Oxides / chemistry
  • Protons*
  • Transistors, Electronic*
  • Zinc Oxide / chemistry

Substances

  • Protons
  • Indium
  • Electrolytes
  • Gallium
  • Zinc Oxide
  • gallium oxide
  • Oxides
  • indium oxide