Antiferroelectric (Pb0.87Sr0.05Ba0.05La0.02)(Zr0.52Sn0.40Ti0.08)O3 thin film capacitors were fabricated for dielectric energy storage. Thin films with excellent crystal quality (FWHM 0.021°) were prepared on (100) SrRuO3/SrTiO3 substrates by pulsed laser deposition. The out-of-plane lattice constant of the thin film was 4.110 ± 0.001 Å. An average maximum recoverable energy storage density, 88 ± 17 J cm−3 with an efficiency of 85% ± 6% at 1 kHz and 80 ± 15 J cm−3 with an efficiency of 91% ± 4% at 10 kHz, was achieved at room temperature. The capacitor was fatigue resistant up to 106 cycles at an applied electric field of 2 MV cm−1. These properties are linked to a low level of hysteresis and slow polarization saturation. PbZrO3-derived oxide thin film capacitors are promising for high efficiency and low loss dielectric energy storage applications.
more »
« less
Thermal stability of antiferroelectric-like Al:HfO 2 thin films with TiN or Pt electrodes
HfO 2 -based antiferroelectric-like thin films are increasingly being considered for commercial devices. However, even with initial promise, the temperature sensitivity of electrical properties such as loss tangent and leakage current remains unreported. 50 nm thick, 4 at. % Al-doped HfO 2 thin films were synthesized via atomic layer deposition with both top and bottom electrodes being TiN or Pt. A study of their capacitance vs temperature showed that the Pt/Al:HfO 2 /Pt had a relative dielectric permittivity of 23.30 ± 0.06 at room temperature with a temperature coefficient of capacitance (TCC) of 78 ± 86 ppm/°C, while the TiN/Al:HfO 2 /TiN had a relative dielectric permittivity of 32.28 ± 0.14 at room temperature with a TCC of 322 ± 41 ppm/°C. The capacitance of both devices varied less than 6% over 1 to 1000 kHz from −125 to 125 °C. Both capacitors maintained loss tangents under 0.03 and leakage current densities of 10 −9 –10 −7 A/cm 2 between −125 and 125 °C. The TiN/Al:HfO 2 /TiN capacitor maintained an energy storage density (ESD) of 18.17 ± 0.79 J/cm 3 at an efficiency of 51.79% ± 2.75% over the −125 to 125 °C range. The Pt/Al:HfO 2 /Pt capacitor also maintained a stable ESD of 9.83 ± 0.26 J/cm 3 with an efficiency of 62.87% ± 3.00% over the same temperature range. Such low losses in both capacitors along with their thermal stability make antiferroelectric-like, Al-doped HfO 2 thin films a promising material for temperature-stable microelectronics.
more »
« less
- PAR ID:
- 10352378
- Date Published:
- Journal Name:
- Applied Physics Letters
- Volume:
- 120
- Issue:
- 23
- ISSN:
- 0003-6951
- Page Range / eLocation ID:
- 232901
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
ABSTRACT This study explores the integration of atomic layer deposited (ALD) HfO2dielectric films with solution‐processed In2O3semiconductor channel, thin‐film transistors (TFTs) for a silicon chip‐free temperature sensor label. The inclusion of the HfO2high‐κ dielectric permits reduced voltage operation of the sensor label. HfO2films are deposited by atomic layer deposition (ALD) at three different hot source temperatures (80°C, 90°C, 100°C), with XPS revealing improved stoichiometry and O/Hf ratios of 1.75, 1.92, and 1.95, respectively, as temperature increases. MOSCAP measurements show improved oxide/semiconductor interface with higher deposition temperatures. The extracted dielectric constants (εr≈ 18.5–18.8) correspond to an equivalent oxide thickness (EOT) of about 3.1 nm, consistent with optimized high‐κ film formation. To enhance drain current, a reduced 7.5 nm HfO2film thickness is used, achieving higher current but reducing yield by 30% due to increased leakage probability in ultrathin films. A voltage divider circuit is developed to integrate an electrochemical thermal sensor, TFT, and an irreversible visual indicator (IVI), allowing for temperature monitoring with a resistivity change of three orders of magnitude at 8°C. The circuit is powered by a 60 mF supercapacitor array providing approximately 0.21 J of available energy, resulting in IVI activation within 40 min at measured activation currents of 20 µA. The system demonstrates potential for low‐voltage, energy‐efficient, silicon‐free sensor labels in applications such as food safety and healthcare monitoring.more » « less
-
Dielectric capacitors are critical components in electronics and energy storage devices. The polymer-based dielectric capacitors have the advantages of device flexibility, fast charge–discharge rates, low loss, and graceful failure. Elevating the use of polymeric dielectric capacitors for advanced energy applications such as electric vehicles (EVs), however, requires significant enhancement of their energy densities. Here, we report a polymer thin film heterostructure-based capacitor of poly(vinylidene fluoride)/poly(methyl methacrylate) with stratified 2D nanofillers (Mica or h-BN nanosheets) (PVDF/PMMA-2D fillers/PVDF), that shows enhanced permittivity, high dielectric strength, and an ultrahigh energy density of ≈75 J/cm3 with efficiency over 79%. Density functional theory calculations verify the observed permittivity enhancement. This approach of using oriented 2D nanofillers-based polymer heterostructure composites is expected to be versatile for designing high energy density thin film polymeric dielectric capacitors for myriads of applications.more » « less
-
Abstract Hf 0.5 Zr 0.5 O 2 (HZO) thin films are promising candidates for non-volatile memory and other related applications due to their demonstrated ferroelectricity at the nanoscale and compatibility with Si processing. However, one reason that HZO has not been fully scaled into industrial applications is due to its deleterious wake-up and fatigue behavior which leads to an inconsistent remanent polarization during cycling. In this study, we explore an interfacial engineering strategy in which we insert 1 nm Al 2 O 3 interlayers at either the top or bottom HZO/TiN interface of sequentially deposited metal-ferroelectric-metal capacitors. By inserting an interfacial layer while limiting exposure to the ambient environment, we successfully introduce a protective passivating layer of Al 2 O 3 that provides excess oxygen to mitigate vacancy formation at the interface. We report that TiN/HZO/TiN capacitors with a 1 nm Al 2 O 3 at the top interface demonstrate a higher remanent polarization (2P r ∼ 42 μ C cm −2 ) and endurance limit beyond 10 8 cycles at a cycling field amplitude of 3.5 MV cm −1 . We use time-of-flight secondary ion mass spectrometry, energy dispersive spectroscopy, and grazing incidence x-ray diffraction to elucidate the origin of enhanced endurance and leakage properties in capacitors with an inserted 1 nm Al 2 O 3 layer. We demonstrate that the use of Al 2 O 3 as a passivating dielectric, coupled with sequential ALD fabrication, is an effective means of interfacial engineering and enhances the performance of ferroelectric HZO devices.more » « less
-
null (Ed.)A phase transition material, VO 2 , with a semiconductor-to-metal transition (SMT) near 341 K (68 °C) has attracted significant research interest because of drastic changes in its electrical resistivity and optical dielectric properties. To address its application needs at specific temperatures, tunable SMT temperatures are highly desired. In this work, effective transition temperature ( T c ) tuning of VO 2 has been demonstrated via a novel Pt : VO 2 nanocomposite design, i.e. , uniform Pt nanoparticles (NPs) embedded in the VO 2 matrix. Interestingly, a bidirectional tuning has been achieved, i.e. , the transition temperature can be systematically tuned to as low as 329.16 K or as high as 360.74 K, with the average diameter of Pt NPs increasing from 1.56 to 4.26 nm. Optical properties, including transmittance ( T %) and dielectric permittivity ( ε ′) were all effectively tuned accordingly. All Pt : VO 2 nanocomposite thin films maintain reasonable SMT properties, i.e. sharp phase transition and narrow width of thermal hysteresis. The bidirectional T c tuning is attributed to two factors: the reconstruction of the band structure at the Pt : VO 2 interface and the change of the Pt : VO 2 phase boundary density. This demonstration sheds light on phase transition tuning of VO 2 at both room temperature and high temperature, which provides a promising approach for VO 2 -based novel electronics and photonics operating under specific temperatures.more » « less
An official website of the United States government

