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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
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Abstract Harvesting waste heat for useful purposes is an essential component of improving the efficiency of primary energy utilization. Today, approaches such as pyroelectric energy conversion are receiving renewed interest for their ability to turn wasted energy back into useful energy. From this perspective, the need for these approaches, the basic mechanisms and processes underlying their operation, and the material and device requirements behind pyroelectric energy conversion are reviewed, and the potential for advances in this area is also discussed.more » « less
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Abstract The hafnate perovskites PbHfO3(antiferroelectric) and SrHfO3(“potential” ferroelectric) are studied as epitaxial thin films on SrTiO3(001) substrates with the added opportunity of observing a morphotropic phase boundary (MPB) in the Pb1−xSrxHfO3system. The resulting (240)‐oriented PbHfO3(Pba2) films exhibited antiferroelectric switching with a saturation polarization ≈53 µC cm−2at 1.6 MV cm−1, weak‐field dielectric constant ≈186 at 298 K, and an antiferroelectric‐to‐paraelectric phase transition at ≈518 K. (002)‐oriented SrHfO3films exhibited neither ferroelectric behavior nor evidence of a polarP4mmphase . Instead, the SrHfO3films exhibited a weak‐field dielectric constant ≈25 at 298 K and no signs of a structural transition to a polar phase as a function of temperature (77–623 K) and electric field (–3 to 3 MV cm−1). While the lack of ferroelectric order in SrHfO3removes the potential for MPB, structural and property evolution of the Pb1−xSrxHfO3(0 ≤x < 1) system is explored. Strontium alloying increased the electric‐breakdown strength (EB) and decreased hysteresis loss, thus enhancing the capacitive energy storage density (Ur) and efficiency (η). The composition, Pb0.5Sr0.5HfO3produced the best combination ofEB = 5.12 ± 0.5 MV cm−1,Ur = 77 ± 5 J cm−3, and η = 97 ± 2%, well out‐performing PbHfO3and other antiferroelectric oxides.more » « less