1 02 Zn-doped Silicon Dioxide Resistance Random Access Memory Resistance Random Access Memory : RRAM RRAM SiO 2 IC SiO 2 SiO 2 S

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1 1 02 Zn-doped Silicon Dioxide Resistance Random Access Memory Resistance Random Access Memory : RRAM RRAM SiO 2 IC SiO 2 SiO 2 SiO 2 IC IC Abstract Among the next-generation memory devices, resistance random access memory (RRAM) is a promising candidate for the applications on digital storage system due to its simple cell structure, low power consumption, high operating speed, and nondestructive readout. Therefore, the research of RRAM devices is a hot topic in the academia. Because the underlying mechanism of resistive switching behavior is still not understood clearly, many researches of RRAM focus on the physical models of resistive switching behaviors and its reliability and feasibility of nonvolatile memory properties for various

2 NANO COMMUNICATION 20 No.1 03 materials. Silicon dioxide is a promising material for integrated circuits (IC) process due to its great chemical stability. In thisstudy, although the pure SiO 2 material didn t reveal the resistive switching behaviors, the bipolar switching characteristics of silicon based material can be obtained through light metal doped in the SiO2 by co-sputtering technology. Therefore, the research using silicon-based oxide as the resistance-switching layer was worthy of investigation due to its high compatibility in IC fabrication for semiconductor industries. In addition, we proposed a novel supercritical CO 2 fluid (SCCO 2 ) treatment method on the silicon based Zn-doped (Zn:SiO 2 ) RRAM for the application in back-end of line (BEOL) of IC process. It was found that the operation current of Zn:SiO 2 RRAM can be reduced to decrease the power consumption and heating degradation of RRAM devices through the SCCO 2 treatment technology. We believe that the method is useful to raise device density of IC product. Keywords RRAMSiO 2 RRAM Nonvolatile Silicon Oxide Resistive Switching SCCO 2 PCRAM RRAM RRAM ns DRAM SRAM Flash 3C Volatile Non-volatile μa Retention Endurance RRAM Metal-Insulator-Metal MIM RRAM RRAM DRAM Flash Flash Flash DRAM DRAM FeRAM MRAM Memory Non-volatile Memory, NVM

3 1 04 SRAM DRAM Flash Read Only Memory, ROM Flash Floating gate Flash MP3 USB Endurance [1] 1T1R 1D1R MIM 1D1R [2-6] SiO 2 - based RRAM MIM SiO 2 CMOS RRAM COMS RRAM [7-9] SiO COMS Multi-target Sputter Metal-doped SiO 2 Thin-film Supercritical CO 2 Fluid, SCCO Filament RRAM 1 FTIR XPS 2 2 RRAM 2 3 Endurance > 10 7, Retentio > 10 4 RRAM

4 NANO COMMUNICATION 20 No.1 05 RRAM 4 Poole-frenkel 5 1 FTIR Zn SiO x XPS Zn 2

5 1 06 [10] 3.2 Supercritical CO 2 Fluid, SCCO 2 RRAM IC 3 Endurance R H / R L = Retention R H / R L >

6 NANO COMMUNICATION 20 No Pt / Zn:SiO x / TiN RRAM 400 o C 120 o C 6 TEM [11] Thermal Budget HfOx TEM

7 1 08 Threshold Voltage on Current Sub-threshold Slope [12] HfOx Traps [13] 7 8(a) RRAM 8(a) HRS Poole-frenkel Schottky 8(b) 9 RRAM LRS Ohmic Conduction 9 (c) Hopping Conduction 3-9 (b) 10 FTIR [14] 7 HfOx 8 SCCO 2 RRAM HRS LRS HRS Poole-frenkel Schottky

8 NANO COMMUNICATION 20 No.1 09 SiO 2 RRAM RRAM RRAM [15-18] NSC M NSC E SCCO 2 RRAM LRS Ohmic Hopping 10 (a) SCCO 2 FTIR (b) SCCO 2 Si-O-Zn (c) SCCO 2 Si-O-Si

9 1 10 [1] T. C. Chang, F. Y. Jian, S. C. Chen and Y. T. Tsai, Developments in Nanocrystal Memory, Mater. Today, vol. 14 (12), pp. 608, 2011 [2] R. Sohal, C. Walczyk, P. Zaumseil, D. Wolansky, A. Fox, B. Tillack, H. J. Mussig, T. Schroeder, Thermal Oxidation of Chemical Vapour Deposited Tungsten Layers on Silicon Substrates for Embedded Non-volatile Memory Application, Thin Solid Films, vol. 517(16), pp , [3] H. Y. Jeong, S. K. Kim, J. Y. Lee, S. Y. Choi, Role of Interface Reaction on Resistive Switching of Metal/ Amorphous TiO 2 /Al RRAM Devices, J. Electrochem. Soc., vol. 158 (10), pp , [4] L. Zhao, J. Zhang, Y. He, X. Guan, H. Qian, and Z. Yu, Dynamic Modeling and Atomistic Simulations of SET and RESET Operations in TiO 2 -Based Unipolar Resistive Memory, IEEE Electron Device Lett., vol. 32(5), pp , [5] Y. L. Chung, P. Y. Lai, Y. C. Chen, and J. S. Chen, Schottky Barrier Mediated Single-Polarity Resistive Switching in Pt Layer - Included TiOx Memory Device, ACS Appl. Mater. Interfaces, vol. 3(6), pp , [6] Z. Fang, H. Y. Yu, X. Li, N. Singh, G. Q. Lo, D. L. Kwong, HfO x /TiO x /HfO x /TiO x Multilayer-Based Forming- Free RRAM Devices With Excellent Uniformity, IEEE Electron Device Lett., vol. 32 (4), pp , [7] M. N. Kozicki, C. Gopalan, M. Balakrishnan, M. Mitkova, A Low-power Nonvolatile Switching Element Based on Copper-tungsten Oxide Solid Electrolyte, IEEE Trans. Nanotechnol., vol. 5, pp , [8] L. Zhang, R. Huang, Albert Wang, D. Wu, R. Wang, Y. Kuang, The Parasitic Effects Induced by the Contact in RRAM with MIM Structure, Proc. IEEE ICSICT, pp , [9] C. Schindler, S. C. P. Thermadam, R. Waser, M. N. Kozicki, Bipolar and Unipolar Resistive Switching in Cudoped SiO 2, IEEE Trans. Electron Devices, vol. 54, pp , [10] K. C. Chang, T. M. Tsai, T. C. Chang, H. H. Wu, J. H. Chen, Y. E. Syu, G. W. Chang, T. J. Chu, G. R. Liu, Y. T. Su, M. C. Chen, J. H. Pan, J. Y. Chen, C. W. Tung, H. C. Huang, Y. H. Tai, D. S. Gan, and Simon M. Sze, Characteristics and Mechanisms of Silicon Oxide Based Resistance Random Access Memory, has been accepted by IEEE Electron Device Lett., [11] C. H. Chen, T. C. Chang, I. H. Liao, P. B. Xi, C. T. Tsai, P. Y. Yang, J. Hsieh, J. Chen, U. S. Chen, and J. R. Chen, Tungsten Nanocrystal Memory Devices Improved by Supercritical Fluid Treatment, Appl. Phys. Lett., vol. 91 (23), pp , [12] M. C. Chen, T. C. Chang, S. Y. Huang, K. C. Chang, H. W. Li, S. C. Chen, J. Lu, and Y. Shi, A low-temperature Method for Improving the Performance of Sputterdeposited ZnO Thin-film-transistors with Supercritical Fluid, Appl. Phys. Lett., vol. 94, p , [13] C. T. Tsai, T. C. Chang, P. T. Liu, P. Y. Yang, Y. C. Kuo, K. T. Kin, P. L. Chang, and F. S. Huang, Low-temperature Method for Enhancing Sputter-deposited HfO 2 Films with Complete Oxidization, Appl. Phys. Lett., vol., 91 (1), pp , [14] K. C. Chang, T. M. Tsai, T. C. Chang, H. H. Wu, K. H. Chen, J. H. Chen, T. F. Young, T. J. Chu, J. Y. Chen, C. H. Pan, Y. T. Su, Y. E. Syu, C. W. Tung, G. W. Chang, M. C. Chen, H. C. Huang, Y. H. Tai, D. S. Gan, J. J. Wu, and Simon M. Sze, Low Temperature Improvement Method on Zn:SiOx Resistive Random Access Memory Devices, has been accepted by IEEE Electron Device Lett., [15] T. M. Tsai, K. C. Chang, T. C. Chang, Y. E. Syu, S. L. Chuang, G. W. Chang, G. R. Liu, M. C. Chen, H. C. Huang, S. K. Liu, Y. H. Tai, D. S. Gan, Y. L. Yang, T. F. Young, B. H. Tseng, K. H. Chen, M. J. Tsai, and S. M. Sze, Bipolar Resistive RAM Characteristics Induced by Nickel Incorporated into Silicon Oxide Dielectrics for IC Applications, IEEE Electron Device Lett., vol. 33 (12), pp , 2012.

10 NANO COMMUNICATION 20 No.1 11 [16] K. C. Chang, T. M. Tsai, T. C. Chang, Y. E. Syu, S. L. Chuang, C. H. Li, D. S. Gan, S. M. Sze, The Effect of Silicon Oxide Based RRAM with Tin Doping, Electrochem. Solid State Lett., vol. 15(3), pp. H65-H68, [17] T. M. Tsai, K. C. Chang, T. C. Chang, G. W. Chang, Y. E. Syu, Y. T. Su, G. R. Liu, K. H. Liao, M. C. Chen, H. C. Huang, Y. H. Tai, D. S. Gan, and S. M. Sze, Origin of Hopping Conduction in Sn-doped Silicon Oxide RRAM with Supercritical CO 2 fluid treatment, IEEE Electron Device Lett., vol. 33 (12), pp , [18] K. C. Chang, T. M. Tsai, T. C. Chang, Y. E. Syu, C. C. Wang, S. L. Chuang, C. H. Li, D. S. Gan, and S. M. Sze, Reducing Operation Current of Ni-doped Silicon Oxide Resistance Random Access Memory by Supercritical CO 2 Fluid Treatment, Appl. Phys. Lett., vol. 99, pp , 2011.

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24-2_cover_OK 2 08 Flexible All Solid State Thin Film Li-ion Battery 1 1 2 1 1 2 ( 300Wh/kg) (3.4~3.8 V) ( 1000 cycles) (LiCoO 2 ) (LiPON) (Mica) 26mAhcm -2 mm -1 30 85% LED Abstract With the ever-changing technology,