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用于在复杂生物流体中增强质子化的双偏置金属氧化物电解质门控薄膜晶体管。

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

作者信息

Hwang Chuljin, Song Yoonseok, Baek Seokhyeon, Choi Jun-Gyu, Park Sungjun

机构信息

Department of Electrical and Computer Engineering, Ajou University, Suwon, 16499, Republic of Korea.

Department of Intelligence Semiconductor Engineering, Ajou University, Suwon, 16499, Republic of Korea.

出版信息

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.

摘要

pH传感技术对于监测水生生态系统和诊断人类健康状况至关重要。铟镓锌氧化物电解质门控薄膜晶体管(IGZO EGTFT)因其传感膜的pH依赖性表面化学性质而被高度视为离子传感设备。然而,由于离子干扰以及受能斯特极限限制的固有低灵敏度,将基于EGTFT的pH传感器应用于含有多种带电物质的复杂生物流体中存在挑战。在此,我们提出了一种双偏置(DB)EGTFT pH传感平台,在半导体 - 生物流体界面实现背栅辅助的灵敏度增强和可循环的氧化还原耦合质子化。一种溶液处理的非晶IGZO薄膜用作质子敏感膜,确保了在6英寸晶圆上的可扩展均匀性。当浸入pH值为4和8的溶液中时,这些器件在数小时内表现出优异的pH抗性。深入的电化学研究表明,背栅偏置显著提高了灵敏度,超过了能斯特极限,达到85 mV/pH。这种提高是由于沟道中额外的电荷积累,从而扩大了传感窗口。作为概念验证,我们观察到在重复的pH循环中,不仅在标准溶液中,而且在生理电解质如磷酸盐缓冲盐水(PBS)和人工尿液中,阈值电压都有一致的变化,证实了在复杂生物环境中可靠运行的潜力。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f52e/11680892/7d6bde2b11a8/41598_2024_80005_Fig1_HTML.jpg

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