Improved Ferroelectric Switching Endurance of La-Doped Hf0.5Zr0

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Improved ferroelectric switching endurance of La-doped Hf0.5Zr0.5O2 thin films Anna G Chernikova, Maxim G Kozodaev, Dmitry V Negrov, Evgeny V Korostylev, Min Hyuk Park, Uwe Schroeder, Cheol Seong Hwang, and Andrey M. Markeev ACS Appl. Mater. Interfaces, Just Accepted Manuscript • DOI: 10.1021/acsami.7b15110 • Publication Date (Web): 28 Dec 2017 Downloaded from http://pubs.acs.org on December 29, 2017

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ACS Applied Materials & Interfaces

Improved ferroelectric switching endurance of La-doped Hf0.5Zr0.5O2 thin films Anna G. Chernikova1, Maxim G. Kozodaev1, Dmitry V. Negrov1, Evgeny V. Korostylev1, Min Hyuk Park2, Uwe Schroeder2, Cheol Seong Hwang1,3 and Andrey M. Markeev1* 1

Moscow Institute of Physics and Technology, Institutskii per. 9, 141700 Dolgoprudny, Moscow region, Russia 2 3

NaMLab gGmbH/TU Dresden, Noethnitzer Strasse 64, 01187 Dresden, Germany

Department of Materials Science and Engineering and Inter-University Semiconductor Research Center, Seoul National University, Seoul 08826, Republic of Korea

*Corresponding author: [email protected]

ABSTRACT Hf0.5Zr0.5O2 thin films are one of the most appealing HfO2-based ferroelectric thin films, which have been researched extensively for their applications in ferroelectric memory devices. In this work, a 1 mol. % La-doped Hf0.5Zr0.5O2 thin film was grown by a plasma-assisted atomic layer deposition and annealed at temperatures of 450 and 500 °C to crystallize the film into the desired orthorhombic phase. Despite the use of a lower temperature than in previous reports, the film showed highly promising ferroelectric properties – a remnant polarization of ~19 µC/cm2 and switching cycle endurance up to 4·1010. The performance was much better than that of undoped Hf0.5Zr0.5O2 thin films, demonstrating the positive influence of La doping. Such improvements were mainly attributed to the decreased coercive field (by ~30% compared to the undoped film), which allowed for use of a lower applied field to drive the cycling tests while keeping a high polarization value. La doping also decreased the leakage current by ~3 orders of magnitude compared to the undoped film, which also contributed to the strongly improved endurance. Nonetheless, the La-doped film required a larger number of wake-up cycles (~106 cycles) to reach a saturated remnant polarization value. This behaviour might be explained by the increased generation of oxygen vacancies and slower migration of these vacancies from the interface to the bulk region. However, the maximum number of wake-up cycle was less than 1 ACS Paragon Plus Environment

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0.01% of the total possible cycles, and therefore, initializing the film to the maximum performance state would not be a serious burden.

Keywords: hafnium oxide, multicomponent oxide, thin films, ferroelectricity, non-volatile memory, atomic layer deposition

INTRODUCTION Hf0.5Zr0.5O2 (HZO) thin films are the leading candidate material among the various cationdoped HfO2-based ferroelectric (FE) thin films for semiconductor memory applications. This is mainly due to the lower processing temperature in the film deposition and annealing of the material (less than 500 °C for annealing is required for crystallization1-3) compared to other films, such as Si- or Al-doped HfO2 films, which require at least ~ 800 °C for sufficient crystallization4-6. The most feasible film deposition method is atomic layer deposition (ALD), which offers high reproducibility, precise thickness control, and conformal coverage over extreme three-dimensional structures. Moreover, it can be applied not only for growth of functional ferroelectric layers, but also for CMOS-compatible electrodes, including TiN, Ru, Ir, etc7,8. ZrO2 thin films have a lower crystallization temperature compared to HfO2, making the crystallization of HZO films feasible at such a low temperature. The low processing temperature is critical for integrating the metal-ferroelectric-metal (MFM) structure, where the typical electrode metal is TiN, into the back-end-of-line (BEOL) process, which requires a low temperature (preferably 1010), and therefore, wake-up can be quickly performed before actual device use.

CONFLICTS OF INTERESTS There are no conflicts of interest to declare.

ACKNOWLEDGMENTS ALD growth of the HZLO and HZO films and their electrical property investigations were supported by Russian Science Foundation (Project. No 14-19-01645-P) using equipment at the MIPT Shared Facilities Center supported from the Ministry of Education and Science of Russian Federation (Grant No. RFMEFI59417X0014). Structural investigations of the mentioned films were supported by Moscow Institute of Physics and Technology and Russian Academic Excellence Project 5-100 (Contract № 19VP/2017).

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Improved Ferroelectric Switching Endurance of La-Doped Hf0.5Zr0

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