Abstract
In order to develop an alternate high-k and low-loss dielectric material for high density energy storage and gate oxide applications and to address the leakage current issues in single layer oxide thin films, nano-stacked devices with the active oxide layer sandwiched between higher bandgap barrier layers have recently been extensively explored. Here, we report the fabrication of Al2O3/TiO2 (20 nm)/Al2O3 (ATA) nano-stacks using an optimized atomic layer deposition technique, where the effect of the Al2O3 barrier layer thickness on leakage and dielectric properties was thoroughly explored. The high dielectric loss (> 1) and leakage current values (> 10−4 A/cm2) exhibited by ~ 20 nm TiO2 thin film was reduced significantly by encapsulating with Al2O3 barrier layer. Introducing barrier layer thickness from 1 to 5 nm, the leakage paths are substantially reduced and the charge carriers are effectively trapped at the interfaces, leading to a significant improvement in leakage current density (reduction from ~ 7.47 × 10−7 to 1.21 × 10−9 A/cm2 at 1 V applied bias), breakdown field (increase from 0.8 to 1.75 MV/cm) and dielectric loss (reduction from 0.1 to 0.06). Furthermore, the capacitance density of a particular ATA structure was found to be invariant with applied bias voltage (− 1 V to + 1 V) and frequency (10 kHz to 1 MHz), demonstrating its potential in various high frequency capacitive circuit applications. Notably, the ATA structure having barrier layer thickness of ~ 1 nm, demonstrated a significantly high capacitance density (~ 13.2 fF/µm2), low dielectric loss (~ 0.1) and low leakage current density (~ 7.47 × 10−7 A/cm2 @1 V bias), making this ATA stack a promising material for high-density energy storage and gate dielectric applications.
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs10854-023-10615-3/MediaObjects/10854_2023_10615_Fig1_HTML.png)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs10854-023-10615-3/MediaObjects/10854_2023_10615_Fig2_HTML.png)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs10854-023-10615-3/MediaObjects/10854_2023_10615_Fig3_HTML.png)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs10854-023-10615-3/MediaObjects/10854_2023_10615_Fig4_HTML.png)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs10854-023-10615-3/MediaObjects/10854_2023_10615_Fig5_HTML.png)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs10854-023-10615-3/MediaObjects/10854_2023_10615_Fig6_HTML.png)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs10854-023-10615-3/MediaObjects/10854_2023_10615_Fig7_HTML.png)
Similar content being viewed by others
Data availability
The data underlying this article are available in the article. The datasets generated during and/or analysed during the current study can be made available from the corresponding author on reasonable request.
Code availability
Not applicable.
References
J.R. Miller, P. Simon, Science 321, 651–652 (2008)
B. Kang, G. Ceder, Nature 458, 190–193 (2009)
B. Zhu, X. Wu, W.-J. Liu, S.-J. Ding, D.W. Zhang, Z. Fan, Nanoscale Res. Lett. 14(1), 1–6 (2019)
C.H. Chen, C.S. Change, C.P. Chao, J.F. Kuan, C.L. Chang, IEEE International Electron Devices Meeting 2003, Washington, DC, pp. 2.5.1–2.5.4 (2003).
The International Technology Roadmap for Semiconductors (ITRS) (Semiconductor Industry Association, 2022). http://www.itrs2.net/2022-itrs.html for ITRS Roadmap (2022)
G.D. Wilk, R.M. Wallace, J.M. Anthony, J. Appl. Phys. 89, 5243–5275 (2001)
J. Robertson, Rep. Prog. Phys. 69, 327–396 (2006)
W. Li, O. Auciello, R.N. Premnath, B. Kabius, Appl. Phys. Lett. 96, 162907 (2010)
C.H. Cheng, S.H. Lin, K.Y. Jhou, C.P. Chou, F.S. Yeh, J. Hu, M. Hwang, T. Arikado, S.P. McAlister, IEEE Electron Device Lett. 29, 845 (2008)
M.T. Yu, K.Y. Chen, Y.H. Chen, RSC Adv. 5, 13550–13554 (2015)
J.H. Choi, Y. Mao, J.P. Chang, Mater. Sci. Eng. R Rep. 72, 97–136 (2011)
H.M. Kwon, I.S. Han, S.U. Park, J.D. Bok, Y.J. Jung, H.S. Shin, C.Y. Kang, B.H. Lee, R. Jammy, G.W. Lee, H.D. Lee, Jpn. J. Appl. Phys. 50, 04DD02 (2011)
T. Bertaud, C. Bermond, S. Blonkowski, C. Vallée, T. Lacrevaz, A. Farcy, M. Gros-Jean, B. Fléchet, IEEE Trans. Compon. Packag. Manuf. Technol. 2(3), 502–509 (2012)
S. Kumar, H. Kumar, S. Vura, A.S. Pratiyush, V.S. Charan, S.B. Dolmanan, S. Tripathy, R. Muralidharan, D.N. Nath, IEEE Trans. Electron Devices 66(3), 1230–1235 (2019)
P.S. Padhi, S.K. Rai, H. Srivastava, R.S. Ajimsha, A.K. Srivastava, P. Misra, A.C.S. Appl, Mater. Interfaces 14(10), 12873–12882 (2022)
B. Hudec, K. Husekova, E. Dobrocka, J. Aarik, R. Rammula, A. Kasikov, A. Tarre, A. Vincze, K. Fröhlich, J. Vac. Sci. Technol. B 29(1), 01AC09 (2011)
W. Weinreich, A. Shariq, K. Seidel, J. Sundqvist, A. Paskaleva, M. Lemberger, A.J. Bauer, J. Vac. Sci. Technol. B 31, 01A109 (2013)
S. Kim, S.H. Lee, I.H. Jo, J. Seo, Y.E. Yoo, J.H. Kim, Sci. Rep. 12, 5124 (2022)
X. Wang, H. Liu, L. Zhao, Y. Wang, S. Wang, J. Mater. Sci. Mater. Electron. 30, 12577–12583 (2019)
P.S. Padhi, R.S. Ajimsha, S.K. Chetia, A.K. Das, V.K. Sahu, P. Misra, AIP Conf. Proc. 2265(1), 030190 (2020)
D. Cao, F. Liu, X. Shi, H. Shi, L. Zheng, L. Shen, X. Cheng, Y. Yu, X. Li, W. Shi, J. Mater. Sci. Mater. Electron. 29, 7644–7650 (2018)
J.C. Woo, Y.S. Chun, Y.H. Joo, C.I. Kim, Appl. Phys. Lett. 100, 081101 (2012)
P.S. Padhi, R. S. Ajimsha, S. K. Rai, S. Bhartiya, A. Bose, B. Das, M. K. Tiwari, P. Misra, Precursor purge time dependent interface quality and interfacial polarization in Al2O3/TiO2 nanolaminates grown by atomic layer deposition. Physica E Low-Dimens. Syst. Nanostruct. (under review)
P.S. Padhi, R.S. Ajimsha, S.K. Rai, U.K. Goutam, A. Bose, S. Bhartiya, P. Misra, Process temperature dependent interface quality and Maxwell–Wagner interfacial polarization in atomic layer deposited Al2O3/TiO2 nanolaminates for energy storage application. Nanoscale Advance Article (2023).
O.M.E. Ylivaara, L. Kilpi, X. Liu, S. Sintonen, S. Ali, M. Laitinen, J. Julin, E. Haimi, T. Sajavaara, H. Lipsanen, S.P. Hannula, H. Ronkainen, R.L. Puurunen, J. Vac. Sci. Technol. A 35, 1105 (2017)
A.A. Chaaya, R. Viter, I. Baleviciute, M. Bechelany, A. Ramanavicius, Z. Gertnere, P. Miele, J. Phys. Chem. C 118(7), 3811–3819 (2014)
I. Iatsunskyi, M. Kempiński, M. Jancelewicz, K. Załęski, S. Jurga, V. Smyntyna, Vacuum 113, 52–58 (2015)
L. Yang, L. Jiang, W. Fu, A.W. Weimer, X. Hu, Y. Zhou, Appl. Phys. A 123, 1–6 (2017)
M. **e, X. Sun, C. Zhou, A.S. Cavanagh, H. Sun, T. Hu, S.M. George, J. Electrochem. Soc. 162(6), A974–A998 (2015)
A.H. Alshehri, K. Mistry, V.H. Nguyen, K.H. Ibrahim, D. Muñoz-Rojas, M. Yavuz, K.P. Musselman, Adv. Funct. Mater. 29, 1805533 (2018)
B. Bharti, S. Kumar, H.-N. Lee, R. Kumar, Sci. Rep. 6(1), 32355 (2016)
T.J. Seok, Y. Liu, J.H. Choi, H.J. Kim, D.H. Kim, S.M. Kim, J.H. Jang, D.Y. Cho, S.W. Lee, T.J. Park, Chem. Mater. 32, 7662–7669 (2020)
C. Giovinazzo, C. Ricciardi, C.F. Pirri, A. Chiolerio, S. Porro, Appl. Phys. A 124(10), 1–8 (2018)
C.W. Wiegand, R. Faust, A. Meinhardt, R.H. Blick, R. Zierold, K. Nielsch, Chem. Mater. 30(6), 1971–1979 (2018)
X. Chen, J. Wan, L. Ji, J. Gao, H. Wu, C. Liu, Vacuum 200, 111022 (2022)
A.K. Jonscher, J. Mater. Sci. 16, 2037 (1981)
S.S. Batool, Z. Imran, K. Rasool, J. Ambreen, S. Hassan, S. Arif, M. Ahmad, M.A. Rafiq, Sci. Rep. 10(1), 1–10 (2020)
M.A. Fusco, C.J. Oldham, G.N. Parsons, Materials 12(4), 672 (2019)
M. Liu, Z. Wang, J. Wu, Q. Li, J. Alloys Compd. 652, 260–265 (2015)
W. Tang, J. Xuan, H. Wang, S. Zhao, H. Liu, J. Power Sources 384, 249–255 (2018)
N.D.M. Said, M.Z. Sahdan, A. Ahmad, I. Senain, A.S. Bakri, S.A. Abdullah, M.S. Rahim, AIP Conf. Proc. 1788, 030130 (2017)
F. Huang, Y.-B. Cheng, R.A. Caruso, Aust. J. Chem. 64, 1–4 (2011)
V. Mikhelashvili, G. Eisenstein, A. Lahav, Appl. Phys. Lett. 90, 013506 (2007)
I.S. Park, K.-M. Ryu, J. Jeong, J. Ahn, IEEE Electron. Device Lett. 34(1), 120–122 (2013)
B. Zhu, W. Liu, L. Wei, D.W. Zhang, A. Jiang, S.J. Ding, J. Appl. Phys. 118, 014501 (2015)
Y.H. Wu, C.K. Kao, B.Y. Chen, Y.S. Lin, M.Y. Li, H.C. Wu, Appl. Phys. Lett. 93, 033511 (2008)
S.R. Patil, V.N. Barhate, V.S. Patil, K.S. Agrawal, A.M. Mahajan, J. Mater. Sci. Mater. Electron. 33, 11227–11235 (2022)
Q.X. Zhang, B. Zhu, L.F. Zhang, S.J. Ding, Micro electron. Eng. 122, 1 (2014)
Acknowledgements
One of the authors (PSP) acknowledges HBNI, Mumbai, India, for financial support and is thankful to Amit Das, Vikas Sahu, and S. K. Chetia of ONEL lab, RRCAT for fruitful discussions. Authors are thankful to K. Rajiv from the Mechanical and Optical Support Section, RRCAT, Indore for help in Au thin film coating on silicon substrates, Sushmita Bhartiya from Laser Functional Materials Division, RRCAT, Indore for help in AFM measurements and U.K. Goutam from technical Physics Division, BARC, Mumbai for XPS measurements. Authors are also thankful to Mr. Rakesh Kaul, Head, Laser Materials Processing Division and Associate Director, Materials Science and Advanced Technology Group, RRCAT, Indore for his constant support and encouragement during this Work.
Funding
Information given in the Acknowledgments section.
Author information
Authors and Affiliations
Contributions
PSP: conceptualization, visualization, methodology, formal analysis, investigation, data curation, writing—original draft. RSA: methodology, writing—review and editing. SKR: conceptualization, methodology, formal analysis, writing—review and editing. AB: methodology, formal analysis, writing—review and editing. PM: supervision, project administration. Resources, writing—review and editing.
Corresponding authors
Ethics declarations
Conflict of interest
The authors have no relevant financial or non-financial interests to disclose. The authors declare that they have no conflict of interest.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
S.I. : Selected Papers from ISSMD 2022.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Padhi, P.S., Ajimsha, R.S., Rai, S.K. et al. Effect of Al2O3 layer thickness on leakage current and dielectric properties of atomic layer deposited Al2O3/TiO2/Al2O3 nano-stack. J Mater Sci: Mater Electron 34, 1160 (2023). https://doi.org/10.1007/s10854-023-10615-3
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s10854-023-10615-3