Observation of stabilized negative capacitance effect in hafnium-based ferroic films

Leilei Qiao; Ruiting Zhao; Cheng Song; Yongjian Zhou; Qian Wang; Tian-Ling Ren; Feng Pan

doi:10.1088/2752-5724/ad0524

Volume 3 Issue 1

March 2024

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Article Contents

Leilei Qiao, Ruiting Zhao, Cheng Song, Yongjian Zhou, Qian Wang, Tian-Ling Ren, Feng Pan. Observation of stabilized negative capacitance effect in hafnium-based ferroic films[J]. Materials Futures, 2024, 3(1): 011001. doi: 10.1088/2752-5724/ad0524

Citation:

Leilei Qiao, Ruiting Zhao, Cheng Song, Yongjian Zhou, Qian Wang, Tian-Ling Ren, Feng Pan. Observation of stabilized negative capacitance effect in hafnium-based ferroic films[J]. Materials Futures, 2024, 3(1): 011001. doi: 10.1088/2752-5724/ad0524

Citation:

Leilei Qiao, Ruiting Zhao, Cheng Song, Yongjian Zhou, Qian Wang, Tian-Ling Ren, Feng Pan. Observation of stabilized negative capacitance effect in hafnium-based ferroic films[J]. Materials Futures, 2024, 3(1): 011001. doi: 10.1088/2752-5724/ad0524

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Letter •

OPEN ACCESS

Observation of stabilized negative capacitance effect in hafnium-based ferroic films

Materials Futures, Volume 3, Number 1

Received Date: 2023-06-23
Accepted Date: 2023-10-19
Rev Recd Date: 2023-09-26
Publish Date: 2024-01-03

Article information

doi: 10.1088/2752-5724/ad0524

1.
Key Laboratory of Advanced Materials (MOE), School of Materials Science and Engineering, Tsinghua University, Beijing 100084, People’s Republic of China
2.
Institute of Microelectronics & Beijing National Research Center for Information Science and Technology (BNRist), Tsinghua University, Beijing 100084, People’s Republic of China
Authors to whom any correspondence should be addressed.

More Information

Corresponding author: E-mail: songcheng@mail.tsinghua.edu.cn; E-mail: panf@mail.tsinghua.edu.cn

Abstract

Abstract

A negative capacitance (NC) effect has been proposed as a critical pathway to overcome the Boltzmann tyranny’ of electrons, achieve the steep slope operation of transistors and reduce the power dissipation of current semiconductor devices. In particular, the ferroic property in hafnium-based films with fluorite structure provides an opportunity for the application of the NC effect in electronic devices. However, to date, only a transient NC effect has been confirmed in hafnium-based ferroic materials, which is usually accompanied by hysteresis and is detrimental to low-power transistor operations. The stabilized NC effect enables hysteresis-free and low-power transistors but is difficult to observe and demonstrate in hafnium-based films. This difficulty is closely related to the polycrystalline and multi-phase structure of hafnium-based films fabricated by atomic layer deposition or chemical solution deposition. Here, we prepare epitaxial ferroelectric Hf_0.5Zr_0.5O₂ and antiferroelectric ZrO₂ films with single-phase structure and observe the capacitance enhancement effect of Hf_0.5Zr_0.5O₂/Al₂O₃ and ZrO₂/Al₂O₃ capacitors compared to that of the isolated Al₂O₃ capacitor, verifying the stabilized NC effect. The capacitance of Hf_0.5Zr_0.5O₂ and ZrO₂ is evaluated as -17.41 and -27.64 pF, respectively. The observation of the stabilized NC effect in hafnium-based films sheds light on NC studies and paves the way for low-power transistors.
- negative capacitance effect,
- fluorite structure,
- hafnium-based ferroelectrics,
- antiferroelectric

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Conflict of interest

The author declare no conflicts of interests.

Authors’ contributions

F Pan, C Song and L Qiao conceived and supervised the project. L Qiao and R Zhao deposited the films and fabricated the devices. L Qiao and Y Zhou L Qiao and Y Zhou performed the electrical measurements. F Pan, C Song, L Qiao, R Zhao, Y Zhou and Q Wang performed the data analysis and co-wrote the manuscript. All the authors discussed the results and revised the manuscript.

Funding sources

The National Key R&D Program of China (Grant No. 2021YFB3601301), the National Natural Science Foundation of China (Grant No. 52225106 and 12241404) and the Natural Science Foundation of Beijing, China (Grant No. JQ20010).

References(62)

References

[1]	Theis T N, Solomon P M 2010 It’s time to reinvent the transistor! Science 327 1600 doi: 10.1126/science.1187597
[2]	Salahuddin S, Datta S 2008 Use of negative capacitance to provide voltage amplification for low power nanoscale devices Nano Lett. 8 405-10 doi: 10.1021/nl071804g
[3]	Salvatore G A, Bouvet D, Ionescu A M 2008 Demonstration of subthreshold swing smaller than 60 mV/decade in Fe-FET with P(VDF-TrFE)/SiO₂ gate stack IEEE Int. Electron Devices Meeting (IEDM) 167-7010.1109/IEDM.2008.4796642
[4]	Qiao L, Song C, Sun Y, Fayaz M U, Lu T, Yin S, Chen C, Xu H, Ren T-L, Pan F 2021 Observation of negative capacitance in antiferroelectric PbZrO₃ films Nat. Commun. 12 4215 doi: 10.1038/s41467-021-24530-w
[5]	Mller J, et al 2013 Ferroelectric hafnium oxide: a CMOS-compatible and highly scalable approach to future ferroelectric memories IEEE Int. Electron Devices Meeting 10.8.1-410.1109/IEDM.2013.6724605
[6]	Lee H-J, Lee M, Lee K, Jo J, Yang H, Kim Y, Chae S C, Waghmare U, Lee J H 2020 Scale-free ferroelectricity induced by flat phonon bands in HfO₂ Science 369 6509 doi: 10.1126/science.aba0067
[7]	Cheema S S, et al 2020 Enhanced ferroelectricity in ultrathin films grown directly on silicon Nature 580 478-82 doi: 10.1038/s41586-020-2208-x
[8]	Park M H, Kim H J, Kim Y J, Lee W, Kim H K, Hwang S C 2013 Effect of forming gas annealing on the ferroelectric properties of Hf_0.5Zr_0.5O₂ thin films with and without Pt electrodes Appl. Phys. Lett. 102 112914 doi: 10.1063/1.4798265
[9]	Schroeder U, Park M H, Mikolajick T, Hwang C S 2022 The fundamentals and applications of ferroelectric HfO₂ Nat. Rev. Mater. 7 653-69 doi: 10.1038/s41578-022-00431-2
[10]	Hoffmann M, Slesazeck S, Mikolajick T, Hwang C S 2019 Ferroelectricity in Doped Hafnium Oxide DuxfordWoodhead Publishing p 473
[11]	Khan A I, Chatterjee K, Brian W, Drapcho S, You L, Serrao C, Bakaul S R, Ramesh R, Salahuddin S 2015 Negative capacitance in a ferroelectric capacitor Nat. Mater. 14 5 doi: 10.1038/nmat4148
[12]	Hoffmann M, Pei M, Chatterjee K, Khan A I, Salahuddin S, Slesazeck S, Schroeder U, Mikolajick T 2016 Direct observation of negative capacitance in polycrystalline ferroelectric HfO₂ Adv. Funct. Mater. 26 8643-9 doi: 10.1002/adfm.201602869
[13]	Saha A K, Datta S, Gupta S K 2018 Negative capacitance in resistor-ferroelectric and ferroelectric-dielectric networks: apparent or intrinsic? J. Appl. Phys. 123 105102 doi: 10.1063/1.5016152
[14]	Hoffmann M, Khan A I, Serrao C, Lu Z, Salahuddin S, Pei M, Slesazeck S, Schroeder U, Mikolajick T 2018 Ferroelectric negative capacitance domain dynamics J. Appl. Phys. 123 184101 doi: 10.1063/1.5030072
[15]	Chen J-D, Han W-H, Yang C, Zhao X-S, Guo Y-Y, Zhang X-D, Yang F-H 2020 Recent research progress of ferroelectric negative capacitance field effect transistors Acta Phys. Sin. 69 137701 doi: 10.7498/aps.69.20200354
[16]	Hoffmann M, Slesazeck S, Mikolajick T 2021 Progress and future prospects of negative capacitance electronics: a materials perspective APL Mater. 9 020902 doi: 10.1063/5.0032954
[17]	Wang Y, et al 2020 Record-low subthreshold-swing negative-capacitance 2D field-effect transistors Adv. Mater. 32 2005353 doi: 10.1002/adma.202005353
[18]	Hoffmann M, Fengler F P G, Herzig M, Mittmann T, Max B, Schroeder U, Negrea R, Lucian P, Slesazeck S, Mikolajick T 2019 Unveiling the double-well energy landscape in a ferroelectric layer Nature 565 464-7 doi: 10.1038/s41586-018-0854-z
[19]	Rollo T, Blanchini F, Giordano G, Specogna R, Esseni D 2019 Revised analysis of negative capacitance in ferroelectric-insulator capacitors: analytical and numerical results, physical insight, comparison to experiments IEEE Annual Inter. Electron Devices Meeting 10.1109/IEDM19573.2019.8993436
[20]	Esseni D, Fontanini R 2021 Macroscopic and microscopic picture of negative capacitance operation in ferroelectric capacitors Nanoscale 13 9641-50 doi: 10.1039/D0NR06886A
[21]	Cheema S S, et al 2022 Ultrathin ferroic HfO₂-ZrO₂ superlattice gate stack for advanced transistors Nature 604 65-71 doi: 10.1038/s41586-022-04425-6
[22]	Jo S, et al 2023 Negative differential capacitance in ultrathin ferroelectric Hafnia Nat. Electron. 6 390-7 doi: 10.1038/s41928-023-00959-3
[23]	Park M H, Kim H J, Kim Y J, Lee W, Moon T, Hwang C S 2013 Evolution of phases and ferroelectric properties of thin Hf_0.5Zr_0.5O₂ films according to the thickness and annealing temperature Appl. Phys. Lett. 102 242905 doi: 10.1063/1.4811483
[24]	Ohtaka O, Fukui H, Kunisada T, Fujisawa T O 2004 Phase relations and volume changes of hafnia under high pressure J. Am. Ceram. Soc. 84 5 doi: 10.1111/j.1151-2916.2001.tb00843.x
[25]	Starschich S, Griesche D, Schneller T, Waser R, Bottger U 2014 Chemical solution deposition of ferroelectric yttrium-doped hafnium oxide films on platinum electrode Appl. Phys. Lett. 104 202903 doi: 10.1063/1.4879283
[26]	Hsain H A, Lee Y, Materano M, Mittmann T, Payne A, Mikolajick T, Schroeder U, Parsons G N, Jones J L 2022 Many routes to ferroelectric HfO₂: a review of current deposition methods J. Vac. Sci. Technol. A 40 010803 doi: 10.1116/6.0001317
[27]	Pujar P, Cho H, Gandla S, Naqi M, Hong S, Kim S 2021 Sub-thermionic negative capacitance field effect transistors with solution combustion-derived Hf_0.5Zr_0.5O₂ Adv. Funct. Mater. 31 2103748 doi: 10.1002/adfm.202103748
[28]	Song J, Qi Y, Xiao Z, Wang K, Li D, Kim S-H, Kingon A I, Rappe A M, Hong X 2022 Domain wall enabled steep slope switching in MoS₂ transistors towards hysteresis-free operation npj 2D Mater. Appl. 6 77 doi: 10.1038/s41699-022-00353-1
[29]	Park H W, Oh M, Hwang C S 2022 Negative capacitance from the inhomogenous stray field in a ferroelectric-dielectric structure Adv. Funct. Mater. 32 2200389 doi: 10.1002/adfm.202200389
[30]	Cho H W, Pujar P, Choi M, Kang S, Hong S, Park J, Baek S, Kim Y, Lee J, Kim S 2021 Direct growth of orthorhombic Hf_0.5Zr_0.5O₂ thin films for hysteresis-free MoS₂ negative capacitance field-effect transistors npj 2D Mater. Appl. 5 1-8 doi: 10.1038/s41699-021-00229-w
[31]	Cho H, Pujar P, Choi M, Naqi M, Cho Y, Rho H Y, Lee J, Kim S 2021 Expeditiously crystallized pure orthorhombic-Hf_0.5Zr_0.5O₂ for negative capacitance field effect transistors ACS Appl. Mater. Interfaces 13 60250-60 doi: 10.1021/acsami.1c21387
[32]	Khan A I, Keshavarzi A, Datta S 2020 The future of ferroelectric field-effect transistor technology Nat. Electron. 3 588-97 doi: 10.1038/s41928-020-00492-7
[33]	Zhang Z, Su M, Li G, Wang J, Zhang X, Ho J C, Wang C, Wan D, Liu X, Liao L 2020 Stable hysteresis-free MoS₂ transistors with low-k/high/k bilayer gate dielectrics IEEE Electron. Device Lett. 41 1036-9 doi: 10.1109/LED.2020.3000259
[34]	Zubko P, Wojde J C, Hadjimichael M, Fernandez-Pena S, Sen A, Luk’yanchuk I, Triscone J-M, iguez J 2016 Negative capacitance in multidomain ferroelectric superlattices Nature 534 15 doi: 10.1038/nature17659
[35]	Yadav A K, et al 2019 Spatially resolved steady-state negative capacitance Nature 565 468-71 doi: 10.1038/s41586-018-0855-y
[36]	Park M H, Lee Y H, Hwang C S 2019 Understanding ferroelectric phase formation in doped HfO₂ thin films based on classical nucleation theory Nanoscale 11 19477-87 doi: 10.1039/C9NR05768D
[37]	Park M H, Lee Y H, Mikolajick T, Schroeder U, Hwang C S 2019 Thermodynamic and kinetic origins of ferroelectricity in fluorite structure oxides Adv. Electron. Mater. 5 1800522 doi: 10.1002/aelm.201800522
[38]	Zhao D, Lenz T, Gelinck G H, Groen P, Damjanovic D, de Leeuw D M, Katsouras I 2019 Depolarization of multidomain ferroelectric materials Nat. Commun. 10 2547 doi: 10.1038/s41467-019-10530-4
[39]	Luk’yanchuk I, Tikhonov Y, Sen A, Razumnaya A, Vinokur V M 2019 Harnessing ferroelectric domains for negative capacitance Commun. Phys. 2 22 doi: 10.1038/s42005-019-0121-0
[40]	Park H W, Roh J, Lee Y B, Hwang C S 2019 Modeling of negative capacitance in ferroelectric thin films Adv. Mater. 31 1805266 doi: 10.1002/adma.201805266
[41]	Wei Y, et al 2018 A rhombohedral ferroelectric phase in epitaxially strained Hf_0.5Zr_0.5O₂ thin films Nat. Mater. 17 1095-100 doi: 10.1038/s41563-018-0196-0
[42]	Yoong H Y, et al 2018 Epitaxial ferroelectric Hf_0.5Zr_0.5O₂ thin films and their implementations in memristors for brain-inspired computing Adv. Funct. Mater. 28 1806037 doi: 10.1002/adfm.201806037
[43]	Estanda S, Dix N, Gazquez J, Fina I, Lyu J, Chisholm M F, Fontcuberta J, Snchez F 2019 Engineering ferroelectric Hf_0.5Zr_0.5O₂ thin films by epitaxial stress ACS Appl. Electron. Mater. 1 1449-57 doi: 10.1021/acsaelm.9b00256
[44]	Pintilie L, Lisca M, Alexe M 2005 Polarization reversal and capacitance-voltage characteristic of epitaxial Pb(Zr,Ti)O₃ layers Appl. Phys. Lett. 86 192902 doi: 10.1063/1.1926403
[45]	Luo Q, et al 2020 A highly CMOS compatible hafnia-based ferroelectric diode Nat. Commun. 11 1391 doi: 10.1038/s41467-020-15159-2
[46]	Catalan G, O’Neill D, Bowman R M, Gregg J M 2000 Relaxor features in ferroelectric superlattices: a maxwell-wagner approach Appl. Phys. Lett. 77 3078-80 doi: 10.1063/1.1324729
[47]	Zhang Z, et al 2022 Flexible polystyrene/graphene composites with epsilon-near-zero properties Adv. Compos. Hybrid Mater. 5 1054-66 doi: 10.1007/s42114-022-00486-3
[48]	Xie P, et al 2022 Recent advances in radio-frequency negative dielectric metamaterials by designing heterogeneous composites Adv. Compos. Hybrid Mater. 5 679-95 doi: 10.1007/s42114-022-00479-2
[49]	Wu H, Zhong Y, Tang Y, Huang Y, Liu G, Sun W, Xie P, Pan D, Liu C, Guo Z 2022 Precise regulation of weekly negative permittivity in CaCu₃Ti₄O₁₂ metacomposites by synergistic effects of carbon nanotubes and grapheme Adv. Compos. Hybrid Mater. 5 419-30 doi: 10.1007/s42114-021-00378-y
[50]	Chang S C, et al 2021 FeRAM using anti-ferroelectric capacitors for high-speed and high-density embedded memory 2021 IEEE Inter. Electron Devices Meeting (IEDM) 33.2.1-410.1109/IEDM19574.2021.9720510
[51]	Yan X, et al 2019 Robust Ag/ZrO₂/WS₂/Pt memristor for neuromorphic computing ACS Appl. Mater. Interfaces 11 48029-38 doi: 10.1021/acsami.9b17160
[52]	Hoffmann M, et al 2022 Antiferroelectric negative capacitance from a structural phase transition in zirconia Nat. Commun. 13 1228 doi: 10.1038/s41467-022-28860-1
[53]	Ali F, Ali T, Lehninger D, Sunbul A, Viegas A, Sachdeva R, Abbas A, Czernohorsky M, Seidel K 2022 Fluorite-structured ferroelectric and antiferroelectric materials: a gateway of miniaturized electronic devices Adv. Funct. Mater. 32 2201737 doi: 10.1002/adfm.202201737
[54]	Cheema S S, et al 2022 Emergent ferroelectricity in subnanometer binary oxide films on silicon Science 5 376 doi: 10.1126/science.abm8642
[55]	Luo X, Toprasertpong K, Takenaka M, Takagi S 2021 Antiferroelectric properties of ZrO₂ ultra-thin films prepared by atomic layer deposition Appl. Phys. Lett. 118 232904 doi: 10.1063/5.0051068
[56]	Gao S, et al 2022 Highly transmitted silver nanowires-SWCNTs conductive flexible film by nested density structure and aluminum-doped zinc oxide capping layer for flexible amorphous silicon solar cells J. Mater. Sci. Technol. 126 152-60 doi: 10.1016/j.jmst.2022.03.012
[57]	Hou C, et al 2023 Boosted lithium storage performance by local build-in electric field derived by oxygen vacancies in 3D holey N-doped carbon structure decorated with molybdenum dioxide J. Mate. Sci. Technol. 142 185-95 doi: 10.1016/j.jmst.2022.10.007
[58]	Ma R, et al 2022 Enhanced energy storage of lead-free mixed oxide core double-shell barium strontium zirconate titanate@magnesium aluminate@zinc oxide-boron trioxide-silica ceramic nanocomposites Adv. Compos. Hybrid Mater. 5 1477-89 doi: 10.1007/s42114-022-00509-z
[59]	Wu N, Zhao B, Chen X, Hou C, Huang M, Alhadhrami A, Mersal G A M, Ibrahim M M, Tian J 2022 Dielectric properties and electromagnetic simulation of molybdenum disulfide and ferric oxide-modified Ti₃C₂T_X MXene hetero-structure for potential microwave absorption Adv. Compos. Hybrid Mater. 5 1548-56 doi: 10.1007/s42114-022-00490-7
[60]	Jiang X, et al 2022 Manipulation of current rectification in van der Waals ferroionic CuInP₂S₆ Nat. Commun. 13 574 doi: 10.1038/s41467-022-28235-6
[61]	Dai S, et al 2022 Robustly stable ferroelectric polarization states enable long-term nonvolatile storage against radiation in hfo2-based ferroelectric field-effect transistors ACS Adv. Appl. Mater. Interfaces 14 51459-67 doi: 10.1021/acsami.2c13392
[62]	Liao J, Dai S, Peng R-C, Yang J, Zeng B, Liao M, Zhou Y 2023 HfO₂-based ferroelectric thin film and memory device applications in the post-Moore era: a review Fundam. Res. 3 332-45 doi: 10.1016/j.fmre.2023.02.010