Deciphering Structural and Ferroelectric behaviour in Hf_1-xZr_xO₂ Thin Films through Chemical Beam Vapor Deposition

Author(s)

Abstract
The discovery of ferroelectricity (FE) in hafnium-based thin film system has opened a new avenue of research, where HfO2 is considered a suitable replacement for Si-based electronic devices. However, the occurence of FE and its underlying physical mechanism is not well understood. In this paper, we report the synergistic role of defect dipoles on the structure, electrical, and ferroelectric behavior of Hf0.7Zr0.3O2 (Hf-rich), Hf0.5Zr0.5O2 (50-50), Hf0.3Zr0.7O2 (Zr-rich) thin films grown on TiO2: Nb substrate using Chemical Beam Vapor deposition (CBVD) technique. Grazing angle incidence X-ray diffraction (GIXRD) and Raman measurements confirm the coexistence of the monoclinic and orthorhombic phases in the films. Detailed X-ray Photoelectron Spectroscopy (XPS) analysis showed the coexistence of metallic and oxide cationic forms of Hf, which ratify the presence of defect dipoles. These defect dipoles significantly affect the electrical and ferroelectric behavior of the films. A lossy polarization behavior was observed for 50/50 and Zr-rich films. The negative shift of polarization loops a supports the antistites disordering in the systems. A maximum dielectric constant of ~16 and a minimum value of ~7 was recorded for Hf-rich and Zr-rich films at 100Hz frequency.

Keywords
Hf1-xZrxO2; Thin Film; Chemical Beam Vapor deposition; Ferroelectricity; Defect Dipoles.

Cite this paper
Md Kashif Shamim, William Maudez, Estelle Wagner, Digvijay Narayan Singh, Seema Sharma, Giacomo Benvenuti, Rashmi Rani, Deciphering Structural and Ferroelectric behaviour in Hf_1-xZr_xO₂ Thin Films through Chemical Beam Vapor Deposition , International Journal of Materials Science and Technology. Volume 1, Issue 1, January 2023 | PP. 1-13. 10.54647/ijmst6101002

References

[ 1 ]	G D Wilk, J Appl. Phys. 89, 5243 (2001)
[ 2 ]	G D Wilk, R M Wallace, J M Anthony, J Appl. Phys. 87, 484 (2000)
[ 3 ]	J A Eastman, Nature 21, 838 (2022)
[ 4 ]	T S Boscke, J Muller, D Brauhaus, U Schroder and U Bottger, Appl. Phys. Lett 99, 102903 (2011)
[ 5 ]	N V Nguyen, Albert, V Davyadov, D Chandler-Horowitz; Appl. Phys. Lett. 87, 192903 (2005)
[ 6 ]	K D Kim, M H Park, H J Kim, Y J Kim, T Moon, Y H Lee, S D Hyun, T Gwon, and C S Wang, J Mat Chem C, 4, 6864 (2016)
[ 7 ]	K D Kim, M H Park, H J Kim, Y J Kim, T Moon, Y H Lee, S D Hyun, T Gwon, and C S Wang, J Mat Chem C, 4, 6864 (2016)
[ 8 ]	X. Sang, E. D. Grimley, T. Schenk, U. Schroeder, James M. LeBeau, Appl. Phys. Lett. 106, 162905 (2015)
[ 9 ]	S Mueller, J Mueller, A Singh, S Riedel, J Sundqvist, W Schroeder and Thomas Milkolajick, Adv. Funct. Mat. 22, 2412 (2012)
[ 10 ]	A Chernikova,D S Kuzmichev, D V Negrov, M G Kozodeav, S N Polyakov and A M Markeev, Appl. Phys. Lett. 108 242905 (2016)
[ 11 ]	J Müller, T S. Böscke, U Schröder, S Mueller, D Bräuhaus, U Böttger, L Frey, and T Mikolajick, Nano Lett. 12, 4318 (2012)
[ 12 ]	M. Hoffmann, U. Schroeder, T. Schenk, T. Shimizu, H. Funakubo, O. Sakata, D. Pohl, M. Drescher, C. Adelmann, R. Materlik, A. Kersch, and T. Mikolajick, J Appl. Phys. 118, 072006 (2015)
[ 13 ]	T Schenk, S Mueller, U Schroder, R Materlik, A Kresch, M Popovici, C Adelmann, S V Elshocht, T Mikalojick, Proceedings of the European Solid-State Device Research Conference (ESSDERC), Bucharest, Romania, B6L-C Emerging memories II, 260, (2013)
[ 14 ]	T Shimizu, K Katayama, T Kiguchi, A Akama, T J. Konno, O Sakata & H Funakubo, Sc. Reports. 6, 32931 (2016)
[ 15 ]	M H Park, H J Kim, Y J Kim, T Moon, and C S Hwang, Appl. Phys. Lett. 104, 072901 (2014)
[ 16 ]	M H Park, H J Kim, Y J Kim, W Lee, H K Kim, and C S Hwang, Appl. Phys. Lett. 102, 112914 (2013)
[ 17 ]	Y Wei, S Matzen, T Maroutian, G Agnus, M Salverda, P Nukala, Q Chen, J Ye, P Lecoeur, and B Noheda, Phys. Rev. Appl. 12, 031001 (2019)
[ 18 ]	T Shimizu, T Yokouchi, T Shiraishi, T Oikawa, P. S. Sankara Rama Krishnan and H Funakubo, Jpn. J. Appl. Phys. 53 09PA04 (2014)
[ 19 ]	P Nukala, J A -Lleonart, Y Wei, L Yedra, B Dkhil, and B Noheda, ACS Appl. Elec. Mater.1, 2585 (2019)
[ 20 ]	L B-Lours, M Mulder, P Nukala, S de Graaf, Y A. Birkhölzer, B Kooi, B Noheda, G Koster, and G Rijnders, Phys. Rev. Materials 4, 043401 (2020)
[ 21 ]	J. Zhu, L. Chen, J. Jiang, X. Lu, L. Yang, B. Hou, M. Liao, Y. Zhou, X. Ma, and Y. Hao, IEEE Electron Device Lett. 39, 79 (2018)
[ 22 ]	R Rani, W Maudez, R Sayal, R Rai, S Kumar, Md K Shamim, E Wagner, S Sharma and G Benvenuti, Phys. B: Cond. Mat. 650, 414541 (2023)
[ 23 ]	R Rani, Md K Shamim, W Maudez, , E Wagner, R Rai, S Sharma and G Benvenuti, Thin Solid Films. 778, 139883 (2023)
[ 24 ]	S Starschich, D Griesche, T Schneller, U Bottger, ECS J Sol. St. Tech. 3, P419 (2015)
[ 25 ]	M Pesic, M Hoffman, C Richter, T Mikolajick, U Schroeder, Adv Func Mater. 26, 7489 (2016)
[ 26 ]	J Lyu, I Fina, J Fontcuberta, F Sanchez ACS Appl. Mater. Interfaces 11, 6224 (2019)
[ 27 ]	C Zacharaki, P Tsipas, S Chaitoglou, S Fragkos, M Axiotis, A Lagoyiannis, RNegrea, L Pintilie, A Dimoulas, Appl. Phys. Lett. 114, 112901 (2019)
[ 28 ]	B Zhou,H Shi,X D Zhang, Q Su, and ZY Jiang, J Phys. D Appl. Phys. 47, 115502 (2014)
[ 29 ]	X Zhao, and D Vanderbilt, Phys Rev B 65, 233106 (2002)
[ 30 ]	M N Lee, Y.-T. Wei, C. Liu, J.-J. Huang, M Tang, Y-L Chueh, K.-Y. Chu, M-J Chen, H-Y Lee, Y-S Chen, L-H Lee, and M-J Tsai, J Eel. Dev. 3, 377 (2015)
[ 31 ]	T Minmura, T Shimizu, H Uchida, H Funakubo, Appl. Phys. Lett. 116, 062901 (2020)
[ 32 ]	T Kiguchi, S Nakamura, A A Kama, T Shiraishi and T J. Konno; J Ceram. Soc. Japan 124, 689 (2016)