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<journal-meta>
<journal-id journal-id-type="publisher-id">Front. Mater.</journal-id>
<journal-title-group>
<journal-title>Frontiers in Materials</journal-title>
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<issn pub-type="epub">2296-8016</issn>
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<article-id pub-id-type="publisher-id">1735405</article-id>
<article-id pub-id-type="doi">10.3389/fmats.2025.1735405</article-id>
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<subj-group subj-group-type="heading">
<subject>Original Research</subject>
</subj-group>
</article-categories>
<title-group>
<article-title>Enhanced electrical stability of IGZO thin-film transistors using atomic layer deposited Al<sub>2</sub>O<sub>3</sub>/HfO<sub>2</sub> dual-layer gate insulator</article-title>
<alt-title alt-title-type="left-running-head">Lv et al.</alt-title>
<alt-title alt-title-type="right-running-head">
<ext-link ext-link-type="uri" xlink:href="https://doi.org/10.3389/fmats.2025.1735405">10.3389/fmats.2025.1735405</ext-link>
</alt-title>
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<contrib-group>
<contrib contrib-type="author">
<name>
<surname>Lv</surname>
<given-names>Shaocong</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
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<name>
<surname>Wang</surname>
<given-names>Weilin</given-names>
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<sup>1</sup>
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<name>
<surname>Zheng</surname>
<given-names>Shuaiying</given-names>
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<sup>1</sup>
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<given-names>Qian</given-names>
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<sup>1</sup>
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<surname>Li</surname>
<given-names>Yuxiang</given-names>
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<sup>1</sup>
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<surname>Song</surname>
<given-names>Aimin</given-names>
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<sup>2</sup>
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<xref ref-type="aff" rid="aff3">
<sup>3</sup>
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<surname>Kim</surname>
<given-names>Jaekyun</given-names>
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<sup>4</sup>
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<sup>4</sup>
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<surname>Zhang</surname>
<given-names>Jiawei</given-names>
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<aff id="aff1">
<label>1</label>
<institution>Shandong Technology Center of Nanodevices and Integration, School of Integrated Circuit, Shandong University</institution>, <city>Jinan</city>, <country country="CN">China</country>
</aff>
<aff id="aff2">
<label>2</label>
<institution>Institute of Nanoscience and Applications, Southern University of Science and Technology</institution>, <city>Shenzhen</city>, <country country="CN">China</country>
</aff>
<aff id="aff3">
<label>3</label>
<institution>Department of Electrical and Electronic Engineering, University of Manchester</institution>, <city>Manchester</city>, <country country="GB">United Kingdom</country>
</aff>
<aff id="aff4">
<label>4</label>
<institution>Department of Photonics and Nanoelectronics, Hanyang University</institution>, <city>Ansan</city>, <country country="KR">Republic of Korea</country>
</aff>
<author-notes>
<corresp id="c001">
<label>&#x2a;</label>Correspondence: Jidong Jin, <email xlink:href="mailto:jinjidong@hanyang.ac.kr">jinjidong@hanyang.ac.kr</email>; Jiawei Zhang, <email xlink:href="mailto:Jiawei.Zhang@email.sdu.edu.cn">Jiawei.Zhang@email.sdu.edu.cn</email>
</corresp>
</author-notes>
<pub-date publication-format="electronic" date-type="pub" iso-8601-date="2025-12-12">
<day>12</day>
<month>12</month>
<year>2025</year>
</pub-date>
<pub-date publication-format="electronic" date-type="collection">
<year>2025</year>
</pub-date>
<volume>12</volume>
<elocation-id>1735405</elocation-id>
<history>
<date date-type="received">
<day>30</day>
<month>10</month>
<year>2025</year>
</date>
<date date-type="rev-recd">
<day>25</day>
<month>11</month>
<year>2025</year>
</date>
<date date-type="accepted">
<day>02</day>
<month>12</month>
<year>2025</year>
</date>
</history>
<permissions>
<copyright-statement>Copyright &#xa9; 2025 Lv, Wang, Zheng, Wang, Xin, Li, Song, Kim, Jin and Zhang.</copyright-statement>
<copyright-year>2025</copyright-year>
<copyright-holder>Lv, Wang, Zheng, Wang, Xin, Li, Song, Kim, Jin and Zhang</copyright-holder>
<license>
<ali:license_ref start_date="2025-12-12">https://creativecommons.org/licenses/by/4.0/</ali:license_ref>
<license-p>This is an open-access article distributed under the terms of the <ext-link ext-link-type="uri" xlink:href="https://creativecommons.org/licenses/by/4.0/">Creative Commons Attribution License (CC BY)</ext-link>. The use, distribution or reproduction in other forums is permitted, provided the original author(s) and the copyright owner(s) are credited and that the original publication in this journal is cited, in accordance with accepted academic practice. No use, distribution or reproduction is permitted which does not comply with these terms.</license-p>
</license>
</permissions>
<abstract>
<p>This study investigates the stability of positive bias temperature stress (PBTS) in bottom-gate indium-gallium-zinc-oxide (IGZO) thin-film transistors (TFTs) incorporating atomic layer deposited Al<sub>2</sub>O<sub>3</sub>/HfO<sub>2</sub> dual-layer gate insulators (GIs). By optimizing the thicknesses of the Al<sub>2</sub>O<sub>3</sub> and HfO<sub>2</sub>, hydrogen diffusion from the GI into the IGZO layer is effectively controlled and electron traps at the IGZO/GI interface are mitigated. The optimal dual-layer GI configuration for IGZO TFTs is identified as 15 nm Al<sub>2</sub>O<sub>3</sub> on 5 nm HfO<sub>2</sub>, resulting in an exceptionally low threshold voltage shift of &#x2212;0.02 V under PBTS at 125 &#xb0;C for 10<sup>4</sup> s. Additionally, the device exhibits excellent electrical performance, with a saturation mobility of 11.61 cm<sup>2</sup>/Vs, a subthreshold swing of 114 mV/dec, and a threshold voltage of &#x2212;0.23 V. These results highlight the potential of IGZO TFTs with dual-layer GIs for advanced integrated circuit applications.</p>
</abstract>
<kwd-group>
<kwd>IGZO</kwd>
<kwd>thin-film transistor</kwd>
<kwd>PBTs</kwd>
<kwd>high-k</kwd>
<kwd>dual-layer gate insulator</kwd>
</kwd-group>
<funding-group>
<funding-statement>The author(s) declared that financial support was received for this work and/or its publication. This work was supported by the National Key Research and Development Program of China (Grant No. 2016YFA0301200), the Natural Science Foundation of Shandong Province (Grant No. ZR2022ZD04), the National Natural Science Foundation of China (Grant No. 62204143), and the Korea Basic Science Institute (National Research Facilities and Equipment Center), grant funded by the Ministry of Education (Grant No. 2021R1C101A405).</funding-statement>
</funding-group>
<counts>
<fig-count count="7"/>
<table-count count="1"/>
<equation-count count="3"/>
<ref-count count="26"/>
<page-count count="10"/>
</counts>
<custom-meta-group>
<custom-meta>
<meta-name>section-in-acceptance</meta-name>
<meta-value>Semiconducting Materials and Devices</meta-value>
</custom-meta>
</custom-meta-group>
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</front>
<body>
<sec sec-type="intro" id="s1">
<label>1</label>
<title>Introduction</title>
<p>Indium-gallium-zinc-oxide (IGZO) thin-film transistors (TFTs) have attracted significant attention for various display applications due to their high carrier mobility, large-area uniformity and low-temperature processability (<xref ref-type="bibr" rid="B8">Ide et al., 2019</xref>; <xref ref-type="bibr" rid="B25">Shim et al., 2020</xref>; <xref ref-type="bibr" rid="B24">Shi et al., 2021</xref>; <xref ref-type="bibr" rid="B7">Geng et al., 2023</xref>; <xref ref-type="bibr" rid="B2">&#xc7;eliker et al., 2024</xref>; <xref ref-type="bibr" rid="B1">Bao et al., 2025</xref>). Furthermore, IGZO TFTs have demonstrated compatibility with back-end-of-line (BEOL) processes, making them suitable for integration into complex integrated circuits (<xref ref-type="bibr" rid="B3">Chi et al., 2016</xref>; <xref ref-type="bibr" rid="B26">Yu et al., 2016</xref>; <xref ref-type="bibr" rid="B5">Duan et al., 2022</xref>; <xref ref-type="bibr" rid="B9">Izukashi et al., 2025</xref>).</p>
<p>High-k dielectric materials, such as Al<sub>2</sub>O<sub>3</sub> (<xref ref-type="bibr" rid="B22">Ma et al., 2018a</xref>), HfO<sub>2</sub> (<xref ref-type="bibr" rid="B23">Ma et al., 2018b</xref>), Ta<sub>2</sub>O<sub>5</sub> (<xref ref-type="bibr" rid="B4">Chiu et al., 2010</xref>) and ZrO<sub>2</sub> (<xref ref-type="bibr" rid="B14">Lee et al., 2010</xref>) have been employed as gate insulators (GIs) to enable low-voltage operation in IGZO TFTs while maintaining good device performance. The choice of high-k dielectrics significantly impacts the electrical performance of IGZO TFTs, particularly in terms of leakage currents, interface quality and driving current capability (<xref ref-type="bibr" rid="B15">Lee et al., 2013</xref>; <xref ref-type="bibr" rid="B6">Geng et al., 2014</xref>; <xref ref-type="bibr" rid="B17">Li et al., 2022</xref>). In addition to the impact of high-k dielectrics on electrical characteristics, device reliability under bias stress must be rigorously evaluated. For BEOL compatible IGZO TFTs in integrated circuit applications, positive bias temperature stress (PBTS) is a critical metric for assessing device reliability (<xref ref-type="bibr" rid="B11">Kim et al., 2023</xref>; <xref ref-type="bibr" rid="B12">Kim et al., 2024</xref>). Therefore, ensuring high PBTS stability is essential for the development of robust and efficient integrated circuit technologies.</p>
<p>Both electron trapping at the IGZO/GI interface and hydrogen (H) diffusion from the GI into the IGZO channel strongly influence device reliability of IGZO TFTs under PBTS (<xref ref-type="bibr" rid="B11">Kim et al., 2023</xref>; <xref ref-type="bibr" rid="B12">Kim et al., 2024</xref>; <xref ref-type="bibr" rid="B20">Liu et al., 2024b</xref>). Notably, the H content in the GI critically affects PBTS stability (<xref ref-type="bibr" rid="B12">Kim et al., 2024</xref>; <xref ref-type="bibr" rid="B18">Lin et al., 2024</xref>; <xref ref-type="bibr" rid="B19">Liu et al., 2024a</xref>; <xref ref-type="bibr" rid="B20">Liu et al., 2024b</xref>; <xref ref-type="bibr" rid="B21">Lv et al., 2025</xref>). Under PBTS, it should be noted that high H content in the GI can diffuse into the IGZO channel and form donor-like states (<xref ref-type="bibr" rid="B12">Kim et al., 2024</xref>; <xref ref-type="bibr" rid="B20">Liu et al., 2024b</xref>). These states increase free electron density and passivate IGZO/GI interface defects, leading to negative threshold voltage shifts (&#x394;V<sub>TH</sub>) (<xref ref-type="bibr" rid="B12">Kim et al., 2024</xref>; <xref ref-type="bibr" rid="B20">Liu et al., 2024b</xref>; <xref ref-type="bibr" rid="B21">Lv et al., 2025</xref>). In contrast, low H content in the GI may leave IGZO/GI interface traps unpassivated under PBTS, resulting in positive &#x394;V<sub>TH</sub> (<xref ref-type="bibr" rid="B12">Kim et al., 2024</xref>; <xref ref-type="bibr" rid="B21">Lv et al., 2025</xref>). Therefore, precise control of H concentration in the GI is essential for achieving reliable PBTS stability with minimal &#x394;V<sub>TH</sub>.</p>
<p>In this study, we introduce a H-regulated GI strategy for IGZO TFTs, enabled by an engineered Al<sub>2</sub>O<sub>3</sub>/HfO<sub>2</sub> dual-layer stack that precisely modulates H diffusion and electron trapping dynamics. The H content in the GI was controlled by adjusting the thickness of HfO<sub>2</sub> and Al<sub>2</sub>O<sub>3</sub> during the atomic layer deposition (ALD) process. Through combined PBTS measurements, X-ray photoelectron spectroscopy (XPS) and time-of-flight secondary ion mass spectrometry (TOF-SIMS) analyses, we identified H concentration and transport pathways within the GI as the primary factors governing the direction and magnitude of &#x394;V<sub>TH</sub> for IGZO TFTs under PBTS. It was found that the device based on a 15 nm Al<sub>2</sub>O<sub>3</sub>/5 nm HfO<sub>2</sub> dual-layer GI effectively passivate electron traps at the IGZO/GI interface without inducing significant H diffusion under PBTS. As a result, the device demonstrates excellent PBTS stability with a &#x394;V<sub>TH</sub> of &#x2212;0.02 V at 125 &#xb0;C for 10<sup>4</sup> s. Furthermore, the device demonstrated excellent electrical performance. These characteristics demonstrate that this approach offers a promising pathway toward IGZO TFTs with both high stability and excellent electrical performance for display and integrated circuit technologies.</p>
</sec>
<sec id="s2">
<label>2</label>
<title>Experimental section</title>
<p>
<xref ref-type="fig" rid="F1">Figure 1a</xref> illustrates the schematic diagram of bottom-gate IGZO TFTs with different GIs: 20 nm Al<sub>2</sub>O<sub>3</sub> (Device 1), 20 nm HfO<sub>2</sub> (Device 2), 10 nm Al<sub>2</sub>O<sub>3</sub>/10 nm HfO<sub>2</sub> (Device 3), and 15 nm Al<sub>2</sub>O<sub>3</sub>/5 nm HfO<sub>2</sub> (Device 4). Initially, a 50-nm-thick W gate electrode was deposited on the SiO<sub>2</sub>/Si substrate by radio-frequency (RF) sputtering at room temperature in an Ar atmosphere. Then, ALD was employed to deposit the GI materials at 200 &#xb0;C. Trimethylaluminum (TMA) and tetrakis(dimethylamido)hafnium (TDMAH) served as the precursors for Al<sub>2</sub>O<sub>3</sub> and HfO<sub>2</sub> respectively, with H<sub>2</sub>O used as the oxidant. Following the GI deposition, a 12 nm IGZO active channel layer was deposited by RF sputtering using an IGZO target with an In:Ga:Zn ratio of 2:2:1 at room temperature in Ar. Subsequently, the GI and IGZO channel layers were annealed at 400 &#xb0;C for 1 h in O<sub>2</sub>. A 100 nm SiO<sub>2</sub> passivation layer was then deposited by plasma-enhanced chemical vapor deposition (PECVD), and the source/drain regions were defined by reactive ion etching. The source and drain electrodes, consisting of 10 nm indium tin oxide and 100 nm tungsten, were deposited by RF sputtering. Finally, the IGZO TFTs underwent a post-deposition annealing at 400 &#xb0;C for 1 h in O<sub>2</sub>. The channel width and length of the TFTs were 35 &#x3bc;m and 5 &#x3bc;m, respectively.</p>
<fig id="F1" position="float">
<label>FIGURE 1</label>
<caption>
<p>
<bold>(a)</bold> Schematic of IGZO TFTs with different dielectric layers. <bold>(b)</bold> Cross-sectional TEM image and <bold>(c)</bold> EDS image of Device 4.</p>
</caption>
<graphic xlink:href="fmats-12-1735405-g001.tif">
<alt-text content-type="machine-generated">Diagram (a) shows a layered structure of a transistor with labeled components: source, drain, gate, substrate, SiO&#x2082;, IGZO, and GI. Each layer is associated with various devices showing different compositions and thicknesses of Al&#x2082;O&#x2083; and HfO&#x2082;. Image (b) is a cross-sectional electron microscope view of the transistor highlighting layers of SiO&#x2082;, IGZO, Al&#x2082;O&#x2083;, HfO&#x2082;, WO&#x2093;, and W. Image (c) displays an elemental map of the transistor layers, indicating presence of tungsten, hafnium, aluminum, indium, gallium, zinc, silicon, and oxygen.</alt-text>
</graphic>
</fig>
<p>Electrical characteristics were measured using a Keysight B2902A semiconductor parameter analyzer. PBTS tests were conducted in a chamber probe station with a hot chuck at both 25 &#xb0;C and 125 &#xb0;C. XPS spectra were recorded using a ThermoFisher ESCALAB 250Xi system. The spatial distribution of H was determined by TOF-SIMS depth profiling using an ION TOF-SIMS 5 instrument. The cross-sectional transmission electron microscopy (TEM) image and energy dispersive spectroscopy (EDS) elemental line scans were obtained using a high-resolution TEM (HRTEM, Talos F200X, Thermo Fisher Scientific).</p>
</sec>
<sec sec-type="results|discussion" id="s3">
<label>3</label>
<title>Results and discussion</title>
<p>
<xref ref-type="fig" rid="F1">Figure 1b</xref> shows the cross-sectional TEM image of Device 4, revealing uniform, well-defined interfaces between all layers. <xref ref-type="fig" rid="F1">Figure 1c</xref> shows EDS mapping of W, Hf, Al, In, Ga, Zn, Si, and O for Device 4, confirming uniform growth and distribution of all elements.</p>
<p>
<xref ref-type="fig" rid="F2">Figure 2a</xref> shows the capacitance densities of various dielectric materials measured using a metal-insulator-metal (MIM) device structure. The capacitance densities for 20 nm Al<sub>2</sub>O<sub>3</sub>, 20 nm HfO<sub>2</sub>, 10 nm Al<sub>2</sub>O<sub>3</sub>/10 nm HfO<sub>2</sub>, and 15 nm Al<sub>2</sub>O<sub>3</sub>/5 nm HfO<sub>2</sub> are 334.16, 873.18, 483.34, and 395.14 nF/cm<sup>2</sup>, respectively. <xref ref-type="fig" rid="F2">Figure 2b</xref> presents the transfer curves of the IGZO TFTs with different GIs, while <xref ref-type="fig" rid="F2">Figures 2c&#x2013;f</xref> show the corresponding output curves. Key device parameters, including threshold voltage (V<sub>TH</sub>), subthreshold swing (SS), field-effect saturation mobility (&#x3bc;<sub>sat</sub>), and interface trap density (D<sub>it</sub>), were extracted from the transfer curves and are summarized in <xref ref-type="table" rid="T1">Table 1</xref>. The &#x3bc;<sub>sat</sub> and SS were calculated using the following <xref ref-type="disp-formula" rid="e1">Equations 1</xref>, <xref ref-type="disp-formula" rid="e2">2</xref> (<xref ref-type="bibr" rid="B13">Lee and Chung, 2023</xref>):<disp-formula id="e1">
<mml:math id="m1">
<mml:mrow>
<mml:msub>
<mml:mi mathvariant="normal">&#x3bc;</mml:mi>
<mml:mtext>sat</mml:mtext>
</mml:msub>
<mml:mo>&#x3d;</mml:mo>
<mml:mfrac>
<mml:mrow>
<mml:mn>2</mml:mn>
<mml:mi mathvariant="normal">L</mml:mi>
</mml:mrow>
<mml:mrow>
<mml:mi mathvariant="normal">W</mml:mi>
<mml:msub>
<mml:mi mathvariant="normal">C</mml:mi>
<mml:mtext>ox</mml:mtext>
</mml:msub>
</mml:mrow>
</mml:mfrac>
<mml:msup>
<mml:mrow>
<mml:mfenced open="(" close=")" separators="&#x7c;">
<mml:mrow>
<mml:mfrac>
<mml:mrow>
<mml:mi mathvariant="normal">d</mml:mi>
<mml:msqrt>
<mml:msub>
<mml:mi mathvariant="normal">I</mml:mi>
<mml:mi mathvariant="normal">D</mml:mi>
</mml:msub>
</mml:msqrt>
</mml:mrow>
<mml:mrow>
<mml:mi mathvariant="normal">d</mml:mi>
<mml:msub>
<mml:mi mathvariant="normal">V</mml:mi>
<mml:mi mathvariant="normal">G</mml:mi>
</mml:msub>
</mml:mrow>
</mml:mfrac>
</mml:mrow>
</mml:mfenced>
</mml:mrow>
<mml:mn>2</mml:mn>
</mml:msup>
</mml:mrow>
</mml:math>
<label>(1)</label>
</disp-formula>
<disp-formula id="e2">
<mml:math id="m2">
<mml:mrow>
<mml:mtext>SS</mml:mtext>
<mml:mo>&#x3d;</mml:mo>
<mml:msup>
<mml:mrow>
<mml:mfenced open="(" close=")" separators="&#x7c;">
<mml:mrow>
<mml:mfrac>
<mml:mrow>
<mml:mi mathvariant="normal">d</mml:mi>
<mml:mo>&#x2061;</mml:mo>
<mml:mi>log</mml:mi>
<mml:mrow>
<mml:mfenced open="(" close=")" separators="&#x7c;">
<mml:mrow>
<mml:msub>
<mml:mi mathvariant="normal">I</mml:mi>
<mml:mi mathvariant="normal">D</mml:mi>
</mml:msub>
</mml:mrow>
</mml:mfenced>
</mml:mrow>
</mml:mrow>
<mml:mrow>
<mml:mi mathvariant="normal">d</mml:mi>
<mml:msub>
<mml:mi mathvariant="normal">V</mml:mi>
<mml:mi mathvariant="normal">G</mml:mi>
</mml:msub>
</mml:mrow>
</mml:mfrac>
<mml:msub>
<mml:mo>&#x7c;</mml:mo>
<mml:mi>max</mml:mi>
</mml:msub>
</mml:mrow>
</mml:mfenced>
</mml:mrow>
<mml:mrow>
<mml:mo>&#x2010;</mml:mo>
<mml:mn>1</mml:mn>
</mml:mrow>
</mml:msup>
</mml:mrow>
</mml:math>
<label>(2)</label>
</disp-formula>where L is the channel length, W is the channel width, C<sub>ox</sub> is the gate capacitance per unit area, I<sub>D</sub> and V<sub>G</sub> are the drain current and gate voltage, respectively. The V<sub>TH</sub> was defined at a drain current of (W/L) &#xd7; 10 nA. The D<sub>it</sub> can be estimated using the following <xref ref-type="disp-formula" rid="e3">Equation 3</xref> (<xref ref-type="bibr" rid="B10">Jin et al., 2023</xref>):<disp-formula id="e3">
<mml:math id="m3">
<mml:mrow>
<mml:msub>
<mml:mi mathvariant="normal">D</mml:mi>
<mml:mtext>it</mml:mtext>
</mml:msub>
<mml:mo>&#x3d;</mml:mo>
<mml:mrow>
<mml:mfenced open="(" close=")" separators="&#x7c;">
<mml:mrow>
<mml:mfrac>
<mml:mrow>
<mml:mtext>SSlog</mml:mtext>
<mml:mrow>
<mml:mfenced open="(" close=")" separators="&#x7c;">
<mml:mrow>
<mml:mi mathvariant="normal">e</mml:mi>
</mml:mrow>
</mml:mfenced>
</mml:mrow>
</mml:mrow>
<mml:mrow>
<mml:mtext>kT</mml:mtext>
<mml:mo>/</mml:mo>
<mml:mi mathvariant="normal">q</mml:mi>
</mml:mrow>
</mml:mfrac>
<mml:mo>&#x2010;</mml:mo>
<mml:mn>1</mml:mn>
</mml:mrow>
</mml:mfenced>
</mml:mrow>
<mml:mfrac>
<mml:mrow>
<mml:msub>
<mml:mi mathvariant="normal">C</mml:mi>
<mml:mtext>ox</mml:mtext>
</mml:msub>
</mml:mrow>
<mml:mrow>
<mml:msup>
<mml:mi mathvariant="normal">q</mml:mi>
<mml:mn>2</mml:mn>
</mml:msup>
</mml:mrow>
</mml:mfrac>
</mml:mrow>
</mml:math>
<label>(3)</label>
</disp-formula>where k is the Boltzmann constant, T is temperature, and q is the elementary charge. When comparing single-GI devices, Device 2 (20 nm HfO<sub>2</sub>) shows a more positive V<sub>TH</sub> (&#x2212;0.10 V) and higher D<sub>it</sub> (4.22 &#xd7; 10<sup>12</sup> cm<sup>-2</sup>/eV) than Device 1 (20 nm Al<sub>2</sub>O<sub>3</sub>), while its &#x3bc;<sub>sat</sub> is slightly reduced due to the higher D<sub>it</sub>. Devices 3 and 4, which employ Al<sub>2</sub>O<sub>3</sub>/HfO<sub>2</sub> bilayer GIs, exhibit intermediate V<sub>TH</sub> and SS values, while maintaining high &#x3bc;<sub>sat</sub> (&#x223c;11.6 cm<sup>2</sup>/Vs) and relatively low D<sub>it</sub> (&#x223c;2.2 &#xd7; 10<sup>12</sup> cm<sup>-2</sup>/eV), demonstrating that bilayer GIs can effectively balance V<sub>TH</sub> control, SS, and interface quality. To assess reproducibility, 5 additional devices of each type were tested, and the results are summarized in <xref ref-type="fig" rid="F3">Figure 3</xref>, showing consistent device performance across samples.</p>
<fig id="F2" position="float">
<label>FIGURE 2</label>
<caption>
<p>
<bold>(a)</bold> Capacitance-voltage characteristics of MIM devices with different insulators. <bold>(b)</bold> Transfer characteristics of IGZO TFTs. Output characteristics of. <bold>(c)</bold> Device 1, <bold>(d)</bold> Device 2, <bold>(e)</bold> Device 3 and <bold>(f)</bold> Device 4.</p>
</caption>
<graphic xlink:href="fmats-12-1735405-g002.tif">
<alt-text content-type="machine-generated">Six graphs display electrical characteristics of different devices. (a) Capacitance vs. applied voltage for five dielectric stacks, with consistent capacitance from -2 to 4 V. (b) Drain current \(I_D\) vs. gate voltage \(V_G\) at \(V_D &#x3d; 3.3\) V for four devices, showing varying thresholds. (c)-(f) Output characteristics for Devices 1 to 4, respectively, with \(I_D\) vs. drain voltage \(V_D\) at \(V_G\) from -0.2 to 3.3 V in steps of 0.5 V. Each device graph shows current increasing with higher gate voltage.</alt-text>
</graphic>
</fig>
<table-wrap id="T1" position="float">
<label>TABLE 1</label>
<caption>
<p>Electrical characteristics of IGZO TFTs with different GIs.</p>
</caption>
<table>
<thead valign="top">
<tr>
<th align="center">IGZO TFT</th>
<th align="center">Al<sub>2</sub>O<sub>3</sub>/HfO<sub>2</sub> (nm)</th>
<th align="center">V<sub>TH</sub> (V)</th>
<th align="center">SS (mV/dec)</th>
<th align="center">&#x3bc;<sub>sat</sub> (cm<sup>2</sup>/Vs)</th>
<th align="center">D<sub>it</sub> (cm<sup>&#x2212;2</sup>/eV)</th>
</tr>
</thead>
<tbody valign="top">
<tr>
<td align="center">Device 1</td>
<td align="center">20/0</td>
<td align="center">&#x2212;0.33</td>
<td align="center">128</td>
<td align="center">11.64</td>
<td align="center">2.31 &#xd7; 10<sup>12</sup>
</td>
</tr>
<tr>
<td align="center">Device 2</td>
<td align="center">0/20</td>
<td align="center">&#x2212;0.10</td>
<td align="center">105</td>
<td align="center">11.14</td>
<td align="center">4.22 &#xd7; 10<sup>12</sup>
</td>
</tr>
<tr>
<td align="center">Device 3</td>
<td align="center">10/10</td>
<td align="center">&#x2212;0.16</td>
<td align="center">106</td>
<td align="center">11.66</td>
<td align="center">2.21 &#xd7; 10<sup>12</sup>
</td>
</tr>
<tr>
<td align="center">Device 4</td>
<td align="center">15/5</td>
<td align="center">&#x2212;0.23</td>
<td align="center">114</td>
<td align="center">11.61</td>
<td align="center">2.23 &#xd7; 10<sup>12</sup>
</td>
</tr>
</tbody>
</table>
</table-wrap>
<fig id="F3" position="float">
<label>FIGURE 3</label>
<caption>
<p>Statistical data of &#x3bc;<sub>sat</sub>, V<sub>TH</sub>, and SS of IGZO TFTs.</p>
</caption>
<graphic xlink:href="fmats-12-1735405-g003.tif">
<alt-text content-type="machine-generated">Scatter plot comparing four devices on three metrics: saturation mobility (\( \mu_{sat} \), black, left axis), threshold voltage (\( V_{TH} \), red, right axis), and subthreshold swing (SS, blue, right axis). Each device shows different values and error bars for each metric.</alt-text>
</graphic>
</fig>
<p>In addition to electrical performance, the reliability of these devices under PBTS was further evaluated, revealing distinct behaviors depending on the GI configuration, with Device 4 exhibiting the highest PBTS stability. The PBTS test results are shown in <xref ref-type="fig" rid="F4">Figures 4a&#x2013;d</xref>. During the PBTS measurements, a gate-stress voltage, V<sub>G</sub> (stress) &#x3d; V<sub>TH</sub> &#x2b; 2 V, was applied for 10<sup>4</sup> s under vacuum conditions at both 25 &#xb0;C and 125 &#xb0;C. The transfer curves were measured at V<sub>D</sub> &#x3d; 0.05 V. The devices exhibit distinct behaviors under PBTS conditions, depending on the type of GI. Device 1 shows a positive &#x394;V<sub>TH</sub> of &#x2b;0.1 V at 125 &#xb0;C, indicating that electron trapping at the IGZO/Al<sub>2</sub>O<sub>3</sub> interface or within the Al<sub>2</sub>O<sub>3</sub> layer is the dominant degradation mechanism (<xref ref-type="bibr" rid="B11">Kim et al., 2023</xref>). In contrast, Device 2 exhibits a negative &#x394;V<sub>TH</sub> of &#x2212;0.2 V under identical conditions due to excessive free carrier generation in IGZO, likely caused by H diffusion from the HfO<sub>2</sub> GI (<xref ref-type="bibr" rid="B16">Lee et al., 2023</xref>). In Devices 3 and 4, which utilize a dual-layer GI, lower &#x394;V<sub>TH</sub> values were observed under PBTS at 125 &#xb0;C for 10<sup>4</sup> s. Device 3 exhibits a &#x394;V<sub>TH</sub> of &#x2212;0.07 V, while Device 4 exhibits a &#x394;V<sub>TH</sub> of &#x2212;0.02 V. These enhanced PBTS stabilities suggest that the implementation of a dual-layer GI can effectively mitigate electron trapping at the IGZO/GI interface through H diffusion. For effective H diffusion, the H content must differ significantly between the two layers of the dual-layer GI. The variations in &#x394;V<sub>TH</sub> for IGZO TFTs with different GIs under PBTS at 125 &#xb0;C are presented in <xref ref-type="fig" rid="F4">Figure 4e</xref>. Clearly, Device 4 shows the best PBTS stability. <xref ref-type="fig" rid="F4">Figure 4f</xref> illustrates the &#x394;V<sub>TH</sub> values measured at both 25 &#xb0;C and 125 &#xb0;C for IGZO TFTs with different GIs subjected to PBTS for 10<sup>4</sup> s, with Device 4 exhibiting the smallest variation in &#x394;V<sub>TH</sub>.</p>
<fig id="F4" position="float">
<label>FIGURE 4</label>
<caption>
<p>Variations in transfer curves with the evolution of stress time for <bold>(a)</bold> Device 1, <bold>(b)</bold> Device 2, <bold>(c)</bold> Device 3 and <bold>(d)</bold> Device 4 under PBTS (125 &#xb0;C). Summary of <bold>(e)</bold> stress-time-dependent variations in &#x394;V<sub>TH</sub> and <bold>(f)</bold> &#x394;V<sub>TH</sub> at 10<sup>4</sup> s under 25 &#xb0;C and 125 &#xb0;C.</p>
</caption>
<graphic xlink:href="fmats-12-1735405-g004.tif">
<alt-text content-type="machine-generated">Graphs showing electrical behavior of four devices at 125&#xB0;C. Graphs (a) to (d) display current (I\_D) vs. gate voltage (V\_G) with stress times. Device 1 shows &#x394;V\_TH &#x3d; &#x2b;0.1V, Device 2 &#x394;V\_TH &#x3d; -0.2V, Device 3 &#x394;V\_TH &#x3d; -0.07V, and Device 4 &#x394;V\_TH &#x3d; -0.02V. Graph (e) plots threshold voltage shift (&#x394;V\_TH) against stress time, comparing all devices. Graph (f) compares &#x394;V\_TH for two temperatures (25&#xB0;C and 125&#xB0;C) across devices.</alt-text>
</graphic>
</fig>
<p>The chemical bonding states at the surfaces of HfO<sub>2</sub> and Al<sub>2</sub>O<sub>3</sub> gate dielectrics were examined using XPS. <xref ref-type="fig" rid="F5">Figure 5</xref> illustrates the O 1s core-level XPS spectra for both the HfO<sub>2</sub> and Al<sub>2</sub>O<sub>3</sub> films, where O<sub>I</sub> represents the metal&#x2013;O bond, while O<sub>II</sub> represents the metal&#x2013;OH bond. The area ratios of&#x2013;OH in the HfO<sub>2</sub> and Al<sub>2</sub>O<sub>3</sub> films are 22.5% and 7.9%, respectively, indicating a significantly higher H content in the HfO<sub>2</sub> film. <xref ref-type="fig" rid="F6">Figure 6</xref> presents TOF-SIMS analysis of the devices, revealing that the H intensity in HfO<sub>2</sub> reaches 1.69 &#xd7; 10<sup>3</sup> a.u., approximately four times higher than in Al<sub>2</sub>O<sub>3</sub>. For the devices with a dual-layer Al<sub>2</sub>O<sub>3</sub>/HfO<sub>2</sub> GI, a pronounced H gradient is clearly observed across the interface.</p>
<fig id="F5" position="float">
<label>FIGURE 5</label>
<caption>
<p>The XPS spectra of <bold>(a)</bold> Al<sub>2</sub>O<sub>3</sub> film and <bold>(b)</bold> HfO<sub>2</sub> film with a thickness of 20 nm.</p>
</caption>
<graphic xlink:href="fmats-12-1735405-g005.tif">
<alt-text content-type="machine-generated">X-ray photoelectron spectroscopy (XPS) spectra comparing aluminum oxide (Al&#x2082;O&#x2083;) and hafnium oxide (HfO&#x2082;). Graph (a) shows Al&#x2082;O&#x2083; with measured and fitted curves indicating 92.1% Al-O and 7.9% Al-OH binding. Graph (b) shows HfO&#x2082; with measured and fitted curves indicating 77.5% Hf-O and 22.5% Al-OH binding. Both graphs display intensity against binding energy in electron volts (eV).</alt-text>
</graphic>
</fig>
<fig id="F6" position="float">
<label>FIGURE 6</label>
<caption>
<p>TOF-SIMS depth profiles of the intensities of H across the samples with different GIs.</p>
</caption>
<graphic xlink:href="fmats-12-1735405-g006.tif">
<alt-text content-type="machine-generated">Graph depicting intensity versus sputtering time for four devices labeled in different colors: green (Device 1), blue (Device 2), red (Device 3), and gray (Device 4). Intensity is plotted on a logarithmic scale. The layers in the diagram, from left to right, are SiO2, IGZO, GI, and W. The graph shows varying intensity patterns across devices, with peaks near 100 seconds.</alt-text>
</graphic>
</fig>
<p>
<xref ref-type="fig" rid="F7">Figure 7</xref> presents the schematic energy band diagrams of IGZO TFTs incorporating different GI configurations under PBTS, constructed from the combined PBTS, XPS and TOF-SIMS analyses. The distinct PBTS behaviors observed across the devices can be directly attributed to differences in the H content of the Al<sub>2</sub>O<sub>3</sub> and HfO<sub>2</sub> layers. <xref ref-type="fig" rid="F7">Figure 7a</xref> represents Device 1 (single Al<sub>2</sub>O<sub>3</sub> GI) and indicates that the markedly low H concentration in the Al<sub>2</sub>O<sub>3</sub> GI suppresses H-related reactions (<xref ref-type="bibr" rid="B21">Lv et al., 2025</xref>). As a result, electron trapping at the IGZO/GI interface or within the GI becomes the dominant PBTS mechanism, yielding a positive &#x394;V<sub>TH</sub>. under PBTS (<xref ref-type="bibr" rid="B12">Kim et al., 2024</xref>; <xref ref-type="bibr" rid="B21">Lv et al., 2025</xref>). In <xref ref-type="fig" rid="F7">Figure 7b</xref>, representing Device 2 (single HfO<sub>2</sub> GI), the significantly higher H concentration in the HfO<sub>2</sub> GI promotes H diffusion from HfO<sub>2</sub> into the IGZO channel. This migrated H acts as a shallow donor and increases the free electron density (<xref ref-type="bibr" rid="B16">Lee et al., 2023</xref>), leading to donor-generation-dominated and a negative &#x394;V<sub>TH</sub>. <xref ref-type="fig" rid="F7">Figures 7c,d</xref> correspond to Devices 3 and 4, which employ dual-layer Al<sub>2</sub>O<sub>3</sub>/HfO<sub>2</sub> GIs. These stacked GIs provide enhanced PBTS stability by simultaneously moderating H diffusion and reducing interface-related electron trapping. Notably, Device 4, with its thinner HfO<sub>2</sub> layer, further restricts H diffusion into the IGZO channel. Such controlled H diffusion is unique to Device 4 and results in the most balanced and stable PBTS behavior among all devices examined.</p>
<fig id="F7" position="float">
<label>FIGURE 7</label>
<caption>
<p>Energy band diagrams of <bold>(a)</bold> Device 1, <bold>(b)</bold> Device 2 <bold>(c)</bold> Device 3 and <bold>(d)</bold> Device 4 under PBTS.</p>
</caption>
<graphic xlink:href="fmats-12-1735405-g007.tif">
<alt-text content-type="machine-generated">Diagram with four panels (a-d) illustrating different devices with gate and channel configurations. (a) Device 1 uses Al&#x2082;O&#x2083;. (b) Device 2 features HfO&#x2082;. (c) Device 3 combines HfO&#x2082; and Al&#x2082;O&#x2083;. (d) Device 4 also uses HfO&#x2082; and Al&#x2082;O&#x2083;. Each device has a positive gate bias and shows electron flow with labeled energy levels E_C, E_F, and E_V.</alt-text>
</graphic>
</fig>
</sec>
<sec sec-type="conclusion" id="s4">
<label>4</label>
<title>Conclusion</title>
<p>In this work, we demonstrate a H-regulated GI design based on a Al<sub>2</sub>O<sub>3</sub>/HfO<sub>2</sub> stack that enables fine control over H diffusion and electron trapping in IGZO TFTs. XPS and TOF-SIMS analyses collectively reveal that H concentration and transport pathways within the GI critically determine the sign and magnitude of &#x394;V<sub>TH</sub> for IGZO TFTs under PBTS. The optimized IGZO TFT with 15 nm Al<sub>2</sub>O<sub>3</sub>/5 nm HfO<sub>2</sub> GI demonstrates an exceptionally low &#x394;V<sub>TH</sub> of &#x2212;0.02 V under PBTS at 125 &#xb0;C for 10<sup>4</sup> s. Moreover, the optimized TFT exhibits excellent electrical performance, featuring a &#x3bc;<sub>sat</sub> of 11.61 cm<sup>2</sup>/Vs, a SS of 114 mV/dec, and a V<sub>TH</sub> of &#x2212;0.23 V. These findings offer significant potential for integrated circuit applications, where excellent electrical performance and high stability are essential.</p>
</sec>
</body>
<back>
<sec sec-type="data-availability" id="s5">
<title>Data availability statement</title>
<p>The raw data supporting the conclusions of this article will be made available by the authors, without undue reservation.</p>
</sec>
<sec sec-type="author-contributions" id="s6">
<title>Author contributions</title>
<p>SL: Methodology, Software, Writing &#x2013; review and editing, Conceptualization, Writing &#x2013; original draft, Formal Analysis, Data curation. WW: Methodology, Writing &#x2013; original draft, Formal Analysis, Data curation. SZ: Software, Conceptualization, Methodology, Writing &#x2013; review and editing. CW: Writing &#x2013; review and editing. QX: Writing &#x2013; review and editing. YL: Writing &#x2013; review and editing. AS: Writing &#x2013; review and editing. JK: Writing &#x2013; review and editing. JJ: Methodology, Writing &#x2013; original draft, Data curation, Investigation, Writing &#x2013; review and editing. JZ: Conceptualization, Methodology, Supervision, Funding acquisition, Investigation, Writing &#x2013; review and editing, Formal Analysis, Project administration, Writing &#x2013; original draft, Data curation, Resources, Validation.</p>
</sec>
<sec sec-type="COI-statement" id="s8">
<title>Conflict of interest</title>
<p>The author(s) declared that this work was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest.</p>
</sec>
<sec sec-type="ai-statement" id="s9">
<title>Generative AI statement</title>
<p>The author(s) declared that generative AI was not used in the creation of this manuscript.</p>
<p>Any alternative text (alt text) provided alongside figures in this article has been generated by Frontiers with the support of artificial intelligence and reasonable efforts have been made to ensure accuracy, including review by the authors wherever possible. If you identify any issues, please contact us.</p>
</sec>
<sec sec-type="disclaimer" id="s10">
<title>Publisher&#x2019;s note</title>
<p>All claims expressed in this article are solely those of the authors and do not necessarily represent those of their affiliated organizations, or those of the publisher, the editors and the reviewers. Any product that may be evaluated in this article, or claim that may be made by its manufacturer, is not guaranteed or endorsed by the publisher.</p>
</sec>
<fn-group>
<fn fn-type="custom" custom-type="edited-by">
<p>
<bold>Edited by:</bold> <ext-link ext-link-type="uri" xlink:href="https://loop.frontiersin.org/people/2035443/overview">Tongbo Wei</ext-link>, Chinese Academy of Sciences (CAS), China</p>
</fn>
<fn fn-type="custom" custom-type="reviewed-by">
<p>
<bold>Reviewed by:</bold> <ext-link ext-link-type="uri" xlink:href="https://loop.frontiersin.org/people/1401848/overview">Yuyao Kuang</ext-link>, University of California, Irvine, United States</p>
<p>
<ext-link ext-link-type="uri" xlink:href="https://loop.frontiersin.org/people/3271511/overview">Li Xuyang</ext-link>, Xi&#x2019;an Technological University, China</p>
</fn>
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