System for Ultrahigh Density Storage Supporting. Information. and James M. Tour,ǁ, *

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1 Three-Dimensional Networked Nanoporous Ta 2 O 5-x Memory System for Ultrahigh Density Storage Supporting Information Gunuk Wang,, Jae-Hwang Lee, Yang Yang, Gedeng Ruan, Nam Dong Kim, Yongsung Ji, and James M. Tour,ǁ, * Department of Chemistry, ǁ Department of Materials Science and NanoEngineering, The Richard E. Smalley Institute of Nanoscale Science & Technology, Rice University 6100 Main Street, Houston, Texas 77005, USA. KU-KIST Graduate School of Converging Science & Technology. Korea University, 145, Anam-ro, Seongbuk-gu, Seoul , Republic of Korea. Department of Mechanical and Industrial Engineering, University of Massachusetts, Amherst, Massachusetts 01003, USA. * tour@rice.edu 1. The oxygen ratio of Ta 2 O 5-x (Figure S1). 2. Readout margin of a NP Ta 2 O 5-x memory device (Figure S2). 3. Switching properties of a NP Ta 2 O 5-x memory device with various set voltages (Figure S3). 4. The I-V plot of a NP Ta 2 O 5-x memory device (Figure S4). 5. Summary of the resistances and the readout margin for various integration architectures (Table S1). 6. Supporting Movie M1 and Supporting Movie M2 S1

2 1. The oxygen ratio of Ta 2 O 5-x Figure S1. The plot of the x of the NP Ta 2 O 5-x film as a function of its depth, which can be estimated from Ta and O atomic concentrations. S2

3 2. Modelling: Readout margin of a NP Ta 2 O 5-x memory device Figure S2. Calculated readout margin V/V pu as a function word/bit lines for a NP Ta 2 O 5-x memory device under V r /3 scheme. All resistance values are calculated from the linear fit of the I-V data (Figure 2a). We assumed a worst-case scenario, the one bit-line pull-up (One BLPU). S3

4 3. Switching properties of a NP Ta 2 O 5-x memory device with various set voltages Figure S3. (a) The representative I-V characteristics of the NP Ta 2 O 5-x device with different set voltages (8 and 14 V). (b) The ON/OFF ratio and ON power as a function of different set voltages. S4

5 4. The I-V plot of a NP Ta 2 O 5-x memory device Figure S4. The I-V characteristic of the NP Ta 2 O 5-x device with highest non-linearity. The nonlinearity is ~ S5

6 5. Summary of the resistances and the readout margin for various integration architectures Table S1. Summary of switching parameters for various integration architectures such as 1D-1R, 1S-1R, CRS, and selector-less memory. The resistances for ON, OFF, and sneak and the maximum readout margin for each architecture are summarized. 6. Supporting Movie M1 and Supporting Movie M2 S6

7 Focused ion beam (FIB) tomography was performed by milling out the junction with slice thicknesses of 30 to 50 nm and taking cross-sectional SEM images at every milling step; Supporting Movie M1 is a sequence of the images. Supporting Movie M2 is a rotating 3D reconstructed topology of NP Ta 2 O 5-x junction structure, by the cross-sectional SEM images. References 1. Kim, G. H.; Lee, J. H.; Ahn, Y.; Jeon, W.; Song, S. J.; Seok, J. Y.; Yoon, J. H.; Yoon, K. J.; Park, T. J.; Hwang, C. S. Adv. Funct. Mater. 2013, 23, Wang, G.; Lauchner, A. C.; Lin, J.; Natelson, D.; Palem, K. V.; Tour, J. M. Adv. Mater. 2013, 25, Lee, M. J.; Seo, S.; Kim, D. C.; Ahn, S. E.; Seo, D. H.; Yoo, I. K.; Baek, I. G.; Kim, D. S.; Byun, I. S.; Kim, S. H.; Hwang, I. R.; Kim, J. S.; Jeon, S. H.; Park, B. H. Adv. Mater. 2007, 19, Seo, J. W.; Baik, S. J.; Kang, S. J.; Hong, Y. H.; Yang, J. H.; Lim, K. S. Appl. Phys. Lett. 2011, 98, Liu, Z.-J.; Gan, J.-Y.; Yew, T.-R. Appl. Phys. Lett. 2012, 100, Jiun-Jia, H.; Tuo-Hung, H.; Chung-Wei, H.; Yi-Ming, T.; Wen-Hsiung, C.; Wen-Yueh, J.; Chen-Hsi, L. Jpn. J. Appl. Phys. 2012, 51, 04DD Li, Y.; Lv, H.; Liu, Q.; Long, S.; Wang, M.; Xie, H.; Zhang, K.; Huo, Z.; Liu, M. Nanoscale 2013, 5, Ji, Y.; Zeigler, D. F.; Lee, D. S.; Choi, H.; Jen, A. K. Y.; Ko, H. C.; Kim, T.-W. Nat. Commun. 2013, 4:2707 doi: /ncomms Lee, M.-J.; Kim, S. I.; Lee, C. B.; Yin, H.; Ahn, S.-E.; Kang, B. S.; Kim, K. H.; Park, J. S7

8 C.; Kim, C. J.; Song, I.; Kim, S. W.; Stefanovich, G.; Lee, J. H.; Chung, S. J.; Kim, Y. H.; Park, Y. Adv. Funct. Mater. 2009, 19, Lee, D.-Y.; Tsai, T.-L.; Tseng, T.-Y. Appl. Phys. Lett. 2013, 103, Jiun-Jia, H.; Yi-Ming, T.; Wun-Cheng, L.; Chung-Wei, H.; Tuo-Hung, H. IEEE International Electron Devices Meeting (IEDM). 2011, Lee, W.; Park, J.; Kim, S.; Woo, J.; Shin, J.; Choi, G.; Park, S.; Lee, D.; Cha, E.; Lee, B. H.; Hwang, H. ACS Nano 2012, 6, Lee, M.-J.; Lee, D.; Cho, S.-H.; Hur, J.-H.; Lee, S.-M.; Seo, D. H.; Kim, D.-S.; Yang, M.-S.; Lee, S.; Hwang, E.; Uddin, M. R.; Kim, H.; Chung, U. I.; Park, Y.; Yoo, I.-K. Nat. Commun. 2013, 4:2629 doi: /ncomms Shin, J.; Choi, G.; Woo, J.; Park, J.; Park, S.; Lee, W.; Kim, S.; Son, M.; Hwang, H. Microelectronic Engineering 2012, 93, Myungwoo, S.; Joonmyoung, L.; Jubong, P.; Jungho, S.; Godeuni, C.; Seungjae, J.; Wootae, L.; Seonghyun, K.; Sangsu, P.; Hyunsang, H. IEEE Elect. Dev. Lett. 2011, 32, Lee, M.-J.; Lee, C. B.; Lee, D.; Lee, S. R.; Chang, M.; Hur, J. H.; Kim, Y.-B.; Kim, C.- J.; Seo, D. H.; Seo, S.; Chung, U. I.; Yoo, I.-K.; Kim, K. Nat. Mater. 2011, 10, Lee, A. R.; Bae, Y. C.; Im, H. S.; Hong, J. P. App. Surf. Sci. 2013, 274, Xinjun, L.; Sadaf, S. M.; Sangsu, P.; Seonghyun, K.; Euijun, C.; Daeseok, L.; Gun- Young, J.; Hyunsang, H. IEEE Elec. Dev. Lett. 2013, 34, Bae, Y. C.; Lee, A. R.; Lee, J. B.; Koo, J. H.; Kwon, K. C.; Park, J. G.; Im, H. S.; Hong, J. P. Adv. Funct. Mater. 2012, 22, Yang, C.; Yi, W.; Takei, K.; Hong-Yu, C.; Shimeng, Y.; Chan, P. C. H.; Javey, A.; Wong, S8

9 H. S. P. IEEE Trans. Electron Devices, 2011, 58, Woo, J.; Lee, D.; Choi, G.; Cha, E.; Kim, S.; Lee, W.; Park, S.; Hwang, H. Microelectronic Engineering 2013, 109, Joonmyoung, L.; Jungho, S.; Daeseok, L.; Wootae, L.; Seungjae, J.; Minseok, J.; Jubong, P.; Biju, K. P.; Seonghyun, K.; Sangsu, P.; Hyunsang, H. IEEE International Electron Devices Meeting (IEDM). 2010, Kim, K.-H.; Jo, S. H.; Gaba, S.; Lu, W. Appl. Phys. Lett. 2010, 96, Yang, Y.; Lee, J.; Lee, S.; Liu, C.-H.; Zhong, Z.; Lu, W. Adv. Mater. 2014, 26, Chang, S. H.; Lee, S. B.; Jeon, D. Y.; Park, S. J.; Kim, G. T.; Yang, S. M.; Chae, S. C.; Yoo, H. K.; Kang, B. S.; Lee, M. J.; Noh, T. W. Adv. Mater. 2011, 23, S9

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