Giant energy storage and power density negative capacitance superlattices

• 成果类型: Article
• 署名作者: Cheema, Suraj S.; Shanker, Nirmaan; Hsu, Shang-Lin; Schaadt, Joseph; Ellis, Nathan M.; Cook, Matthew; Rastogi, Ravi; Pilawa-Podgurski, Robert C. N.; Ciston, Jim; Mohamed, Mohamed; Salahuddin, Sayeef
• 署名单位: University of California System; University of California Berkeley; University of California System; University of California Berkeley; Lincoln Laboratory; Massachusetts Institute of Technology (MIT); United States Department of Energy (DOE); Lawrence Berkeley National Laboratory; United States Department of Energy (DOE); Lawrence Berkeley National Laboratory; Massachusetts Institute of Technology (MIT)
• 刊物名称: Nature
• ISSN/ISSBN: 0028-6050
• DOI: 10.1038/s41586-024-07365-5
• 发表日期: 2024-05-23
• 关键词: oxide-films; ferroelectricity; supercapacitors; breakdown; zirconia; science; FUTURE; robots; oxygen; layer

摘要

Dielectric electrostatic capacitors(1), because of their ultrafast charge-discharge, are desirable for high-power energy storage applications. Along with ultrafast operation, on-chip integration can enable miniaturized energy storage devices for emerging autonomous microelectronics and microsystems(2-5). Moreover, state-of-the-art miniaturized electrochemical energy storage systems-microsupercapacitors and microbatteries-currently face safety, packaging, materials and microfabrication challenges preventing on-chip technological readiness(2,3,6), leaving an opportunity for electrostatic microcapacitors. Here we report record-high electrostatic energy storage density (ESD) and power density, to our knowledge, in HfO2-ZrO2-based thin film microcapacitors integrated into silicon, through a three-pronged approach. First, to increase intrinsic energy storage, atomic-layer-deposited antiferroelectric HfO2-ZrO2 films are engineered near a field-driven ferroelectric phase transition to exhibit amplified charge storage by the negative capacitance effect(7-12), which enhances volumetric ESD beyond the best-known back-end-of-the-line-compatible dielectrics (115 J cm(-3)) (ref.13). Second, to increase total energy storage, antiferroelectric superlattice engineering(14) scales the energy storage performance beyond the conventional thickness limitations of HfO2-ZrO2-based (anti)ferroelectricity(15) (100-nm regime). Third, to increase the storage per footprint, the superlattices are conformally integrated into three-dimensional capacitors, which boosts the areal ESD nine times and the areal power density 170 times that of the best-known electrostatic capacitors: 80 mJ cm(-2) and 300 kW cm(-2), respectively. This simultaneous demonstration of ultrahigh energy density and power density overcomes the traditional capacity-speed trade-off across the electrostatic-electrochemical energy storage hierarchy(1,16). Furthermore, the integration of ultrahigh-density and ultrafast-charging thin films within a back-end-of-the-line-compatible process enables monolithic integration of on-chip microcapacitors(5), which can unlock substantial energy storage and power delivery performance for electronic microsystems(17-19).