1 Supplemental Materials 2 3 4 All-Solid-State Electric-Double-Layer Transistor Based On Oxide Ion Migration in Gd-Doped CeO2 on SrTiO3 Single Crystal 5 6 Takashi Tsuchiya, Kazuya Terabe, and Masakazu Aono 7 8 9 WPI Center for Materials Nanoarchitechtectonics, National Institute for Materials Science,1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan 10 11 15 Supplement 1. Vgs dependencies of two-dimensional carrier density and field-effect mobility The Vgs dependencies of two-dimensional carrier density, n2D, and field-effect mobility, , are shown in Sup. 1. The n2D was calculated using the specific capacitance obtained from ac impedance spectroscopy. The was estimated by application of eq. 16 (2) to the ids vs. Vgs characteristic in the first half of the voltage sweep. 12 13 14 17 18 19 20 21 22 Supplement 2. Temperature dependency of ids Supplement 2 shows ids measured at various temperatures with Vgs of 3 V and Vds of 0.5 V. It shows a metallic temperature dependency with a small decrease in ids, namely 20 %, from room temperature to 473 K. 23 24 25 26 27 28 29 30 31 32 33 34 35 36 Supplement 3. Sample preparation The STO-Pt cell containing layered thin films was fabricated on 0.5 wt% Nb doped STO by PLD and radio-frequency (RF) sputtering (schematically shown in Sup. 3(a)). A 400-nm-thick GDC thin film is deposited on 0.5 wt% Nb-doped STO by PLD under the same conditions as for the STO-based EDLT, followed by deposition of a 20-nm-thick top platinum electrode with dimensions of 1 × 1 mm. The Pt-Pt cell containig layered thin films was fabricated on a Pt/Ti/SiO2/Si substrate by PLD and RF sputtering (schematically shown in Sup. 3(b)). A 400-nm-thick GDC thin film was deposited on a Pt/Ti/SiO2/Si substrate, which had been RF sputtered, by PLD under the same condition as for the STO-based EDLT, followed by deposition of a 20-nm-thick top platinum electrode with dimensions of 1 × 1 mm. In contrast to the (001) oriented GDC layer deposited on the STO, the one deposited on 1 1 2 the Pt thin film exhibited a poly-crystalline structure with preferential growth parallel to the (111) direction, as shown in Sups. 3 (c) and (d). 3 4 5 6 7 8 9 10 11 Supplement 4. AC impedance spectroscopy AC impedance spectroscopy of both STO-Pt and Pt-Pt cells was conducted with a typical frequency range of 1 MHz to 1 mHz and an ac bias voltage of 30 mV at various temperature from 300 to 523 K in air. The impedance spectra of the STO-Pt and Pt-Pt cells, measured at 473 and 430 K, and a bode plot of the Pt-Pt cell are shown in Sups. 4 (a-c). In the analysis of the impedance spectra, the best fit to the experimental data is made by the least square fitting method by assuming the equivalent circuit. 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 2 1 Captions 2 3 4 Sup. 1 5 mobility (μ). Vgs dependency of two-dimensional carrier density (n2D) and field-effect 6 7 8 Sup. 2 Temperature dependency of ids measured at temperatures of 473, 400, 360, and 300 K with Vgs of 3 V and Vds of 0.5 V. 9 10 11 12 Sup. 3 Schematic illustrations of (a) STO-Pt and (b) Pt-Pt two-terminal cells for ac impedance spectroscopy. (c) HR-TEM image of GDC/Pt interface of Pt-Pt cell. (d) X-ray diffraction pattern of Pt-Pt cell. 13 14 15 16 Sup. 4 Cole-Cole plot of (a) STO-Pt and (b) Pt-Pt two terminal cells measured at 430 K in air. Insets show magnified view of high-frequency region of spectra. (c) Bode plot of ac impedance spectroscopy results for Pt-Pt cell and diagram of equivalent circuit. 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 3 1 Figures 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 Sup. 1 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 Sup. 2 36 4 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 Sup. 3(a) Sup. 3(b) 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 Sup. 3(c) 34 35 36 5 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 Sup. 3(d) 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 6 1 2 3 4 5 6 7 8 9 10 11 12 13 14 Sup. 4(a) 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 Sup. 4(b) 34 35 36 7 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 Sup. 4(c) 18 19 20 21 8