A comprehensive study on the structural evolution of HfO2 thin films doped with various dopants

Park, Min Hyuk; Schenk, Tony; Fancher, Christopher M.; Grimley, Everett D.; Zhou, Chuanzhen; Richter, Claudia; LeBeau, James M.; Jones, Jacob L.; Mikolajick, Thomas; Schroeder, Uwe

doi:10.1039/C7TC01200D

Title: A comprehensive study on the structural evolution of HfO₂ thin films doped with various dopants

Journal Article · Wed Apr 19 00:00:00 EDT 2017 · Journal of Materials Chemistry C

DOI:https://doi.org/10.1039/C7TC01200D· OSTI ID:1357985

Park, Min Hyuk ^[1]; Schenk, Tony ^[1]; Fancher, Christopher M. ^[2]; Grimley, Everett D. ^[3]; Zhou, Chuanzhen ^[3]; Richter, Claudia ^[1]; LeBeau, James M. ^[3]; Jones, Jacob L. ^[3]; Mikolajick, Thomas ^[1]; Schroeder, Uwe ^[1]

NaMLab gGmbH, Dresden (Germany)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
North Carolina State Univ., Raleigh, NC (United States)

The origin of the unexpected ferroelectricity in doped HfO₂ thin films is now considered to be the formation of a non-centrosymmetric Pca2₁ orthorhombic phase. Due to the polycrystalline nature of the films as well as their extremely small thickness (~10 nm) and mixed orientation and phase composition, structural analysis of doped HfO₂ thin films remains a challenging task. As a further complication, the structural similarities of the orthorhombic and tetragonal phase are difficult to distinguish by typical structural analysis techniques such as X-ray diffraction. To resolve this issue, the changes in the grazing incidence X-ray diffraction (GIXRD) patterns of HfO₂ films doped with Si, Al, and Gd are systematically examined. For all dopants, the shift of o111/t101 diffraction peak is observed with increasing atomic layer deposition (ALD) cycle ratio, and this shift is thought to originate from the orthorhombic to P4₂/nmc tetragonal phase transition with decreasing aspect ratio (2a/(b + c) for orthorhombic and c/a for the tetragonal phase). For quantitative phase analysis, Rietveld refinement is applied to the GIXRD patterns. A progressive phase transition from P2₁/c monoclinic to orthorhombic to tetragonal is confirmed for all dopants, and a strong relationship between orthorhombic phase fraction and remanent polarization value is uniquely demonstrated. The concentration range for the ferroelectric properties was the narrowest for the Si-doped HfO₂ films. As a result, the dopant size is believed to strongly affect the concentration range for the ferroelectric phase stabilization, since small dopants can strongly decrease the free energy of the tetragonal phase due to their shorter metal–oxygen bonds.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1357985

Journal Information:: Journal of Materials Chemistry C, Vol. 5, Issue 19; ISSN 2050-7526

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 196 works

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Formation of the orthorhombic phase in CeO ₂ -HfO ₂ solid solution epitaxial thin films and their ferroelectric properties Shiraishi, T.; Choi, S.; Kiguchi, T. Applied Physics Letters, Vol. 114, Issue 23 https://doi.org/10.1063/1.5097980	journal	June 2019
Structure of HfO ₂ modified with Y, Gd, and Zr at ambient conditions and high pressures Johnson, Brienne; Fancher, Chris M.; Hou, Dong Journal of Applied Physics, Vol. 126, Issue 20 https://doi.org/10.1063/1.5121024	journal	November 2019
Evolution of crystallographic structure and ferroelectricity of Hf _0.5 Zr _0.5 O ₂ films with different deposition rate Kim, Taeho; An, Minho; Jeon, Sanghun AIP Advances, Vol. 10, Issue 1 https://doi.org/10.1063/1.5121454	journal	January 2020
Fluorite-structure antiferroelectrics Park, Min Hyuk; Hwang, Cheol Seong Reports on Progress in Physics, Vol. 82, Issue 12 https://doi.org/10.1088/1361-6633/ab49d6	journal	November 2019
Origin of Pyroelectricity in Ferroelectric HfO ₂ Liu, J.; Liu, S.; Liu, L. H. Physical Review Applied, Vol. 12, Issue 3 https://doi.org/10.1103/physrevapplied.12.034032	journal	September 2019
Atomic Layer Deposition and Properties of HfO ₂ -Al ₂ O ₃ Nanolaminates Kukli, Kaupo; Kemell, Marianna; Castán, Helena ECS Journal of Solid State Science and Technology, Vol. 7, Issue 9 https://doi.org/10.1149/2.0261809jss	journal	January 2018
Ferroelectric hafnium oxide for ferroelectric random-access memories and ferroelectric field-effect transistors Mikolajick, Thomas; Slesazeck, Stefan; Park, Min Hyuk MRS Bulletin, Vol. 43, Issue 5 https://doi.org/10.1557/mrs.2018.92	journal	May 2018
Bulk Depolarization Fields as a Major Contributor to the Ferroelectric Reliability Performance in Lanthanum Doped Hf _0.5 Zr _0.5 O ₂ Capacitors Mehmood, Furqan; Hoffmann, Michael; Lomenzo, Patrick D. Advanced Materials Interfaces, Vol. 6, Issue 21 https://doi.org/10.1002/admi.201901180	journal	August 2019
Crystal Phase Distribution and Ferroelectricity in Ultrathin HfO ₂ –ZrO ₂ Bilayers McBriarty, Martin E.; Narasimhan, Vijay K.; Weeks, Stephen L. physica status solidi (b), Vol. 257, Issue 1 https://doi.org/10.1002/pssb.201900285	journal	September 2019
Microstructural and Thermomechanical Comparison of Ni-Rich and Ni-Lean NiTi-20 at.% Hf High Temperature Shape Memory Alloy Wires Young, A. W.; Wheeler, R. W.; Ley, N. A. Shape Memory and Superelasticity, Vol. 5, Issue 4 https://doi.org/10.1007/s40830-019-00255-0	journal	December 2019
Ferroelectric and pyroelectric properties of polycrystalline La-doped HfO ₂ thin films Mart, C.; Kühnel, K.; Kämpfe, T. Applied Physics Letters, Vol. 114, Issue 10 https://doi.org/10.1063/1.5089821	journal	March 2019
Observing large ferroelectric polarization in top-electrode-free Al:HfO ₂ thin films with Al-rich strip structures Liu, Xin; Yao, Lulu; Cheng, Yonghong Applied Physics Letters, Vol. 115, Issue 15 https://doi.org/10.1063/1.5110668	journal	October 2019
Epitaxial ferroelectric Hf _0.5 Zr _0.5 O ₂ thin film on a buffered YSZ substrate through interface reaction Li, Tao; Zhang, Nian; Sun, Zhenzhong Journal of Materials Chemistry C, Vol. 6, Issue 34 https://doi.org/10.1039/c8tc02941e	journal	January 2018

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