Ab initio study of antiferroelectric PbZrO3 (001) surfaces

Pilania, Ghanshyam; Cao, Yang; Venkataramani, Venkat; Chen, Q.; Ramprasad, Rampi

doi:10.1007/s10853-009-3465-0

Cited by 19 publications

(12 citation statements)

References 23 publications

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“…The reciprocal space integration was performed by sampling the Brillouin zone of the five-atom cubic unit cell with the 5 × 5 × 1 Pack-Monkhorst net [35], that provides the balanced summation in direct and reciprocal spaces. To achieve high accuracy, large enough tolerances of 7,8,7,7,14 were chosen for the Coulomb overlap, Coulomb penetration, exchange overlap, the first exchange pseudo-overlap, and for the second exchange pseudo-overlap, respectively [28].…”

Section: Methodsmentioning

confidence: 99%

“…Although experimental studies dealing with the SrZrO 3 (001) surface are still missing, the temperature dependence of the ferroelectric hysteresis and capacitance in PbZrO 3 epitaxial films has been investigated in the 4.2-400 K temperature range [5]. SrZrO 3 and PbZrO 3 (001) surfaces have recently been studied theoretically by means of ab initio methods [6][7][8][9][10].…”

Section: Introductionmentioning

confidence: 99%

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First-principles calculations of the atomic and electronic structure of SrZrO₃and PbZrO₃(001) and (011) surfaces

Eglitis

Rohlfing

2010

J. Phys.: Condens. Matter

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We present the results of calculations of surface relaxations, rumplings, energetics, optical band gaps, and charge distribution for the SrZrO(3) and PbZrO(3) (001) and (011) surfaces using the ab initio code CRYSTAL and a hybrid description of exchange and correlation. We consider both SrO(PbO) and ZrO(2) terminations of the (001) surface and Sr(Pb), ZrO, and O terminations of the polar SrZrO(3) and PbZrO(3) (011) surfaces. On the (001) surfaces, we find that all upper and third layer atoms relax inward, while outward relaxations of all atoms in the second layer are found with the sole exception of the SrO-terminated SrZrO(3) (001) surface second layer O atom. Between all (001) and (011) surfaces the largest relaxations, more than 15% of the bulk lattice constant, are for the Sr- and Pb-terminated SrZrO(3) and PbZrO(3) (011) surface upper layer Sr and Pb atoms. Our calculated surface rumpling for the SrO- and PbO-terminated SrZrO(3) and PbZrO(3) (001) surfaces (6.77 and 3.32% of a(0)) are by a factor of ten larger than the surface rumpling for the ZrO(2)-terminated (001) surfaces (-0.72 and 0.38% of a(0), respectively). In contrast to the surface rumpling, the (001) surface energies are comparable and in the energy range from 0.93 eV/cell for the ZrO(2)-terminated PbZrO(3) surface to 1.24 eV/cell for the ZrO(2)-terminated SrZrO(3) surface. In contrast to the (001) surface, different terminations of the SrZrO(3) and PbZrO(3) (011) surfaces lead to very different surface energies ranging from 1.74 eV/cell for the Pb-terminated PbZrO(3) (011) surface to 3.61 eV/cell for the ZrO-terminated SrZrO(3) (011) surface. All our calculated (011) surface energies are considerably larger than the (001) surface energies. Our calculated optical band gap for the SrZrO(3) bulk, 5.31 eV, is in fair agreement with the experimental value of 5.6 eV. All our calculated optical band gaps for the SrZrO(3) and PbZrO(3) (001) and (011) surfaces are reduced with respect to the bulk. We predict a considerable increase in the Zr-O chemical bond covalency near the SrZrO(3) and PbZrO(3) (011) surfaces as compared both to the bulk and to the (001) surface.

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Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

First-principles calculations of the atomic and electronic structure of SrZrO₃and PbZrO₃(001) and (011) surfaces

Eglitis

Rohlfing

2010

J. Phys.: Condens. Matter

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“…It was demonstrated that a cleaner nanoparticle surface results in a higher breakdown strength . According to theoretical calculations, while clean surfaces retain bulk‐like behavior, hydroxyl adsorbates induce substantial changes in the surface geometry and introduce electronic states into the bandgap, thereby possibly rendering the surfaces metallic ( Figure ) . The oxygen octahedral configuration is distorted, thereby resulting in a surface state for electrons (directly above the valence band), which has severe implications for nanoparticle synthesis and their impact on the dielectric properties of the nanocomposite.…”

Section: Nanodielectric Materials Explorationmentioning

confidence: 99%

Section: Nanodielectric Materials Explorationmentioning

confidence: 99%

Review of Polymer‐Based Nanodielectric Exploration and Film Scale‐Up for Advanced Capacitors

Tan

2019

Adv Funct Materials

326

166

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The uprising demands for electrical power and electrification requires advanced dielectric functionalities including high capacitance density, high energy density, high current handling capability, high voltage, high temperature, high thermal conductivity, light weight, and environmental reliability. Nanodielectric engineering emerges and attracts extensive efforts from many countries as a result. Unlike prior reviews focusing on lab scale nanocomposite study, this review focuses on recent innovations in polymerbased nanodielectric design on a large scale and their film scale-up efforts for advanced capacitors. The unconventional polymer-nanofiller engineering and their process in the last two decades are discussed. The nanofunctionalized polymers on a molecular level for high dielectric constants and high dielectric strength are briefly described. The challenge associated with film scale-up and retention of nanodielectric properties are then pointed out to be crucial toward a transfer of dielectric and capacitor technology. Several important attempts at scaling up dielectric films and capacitors recently supported by the US government and industry are reviewed. An alternative strategic approach to achieving high performance polymer films is introduced by leveraging 2D surface coating on commercially mature large-scale polymer films. Future pathways for high quality scalable dielectric films exhibiting desirable dielectric properties and feasibility for capacitor manufacturing are suggested.to develop a more compact pulse-forming network for a pulsed high power microwave (HPM), a laser source, aircraft ignition systems, and high-power electrical systems. [1] The US NAVY strove to develop an all-electric warship for advancing its future combat capability (lethality and survivability). This warship required high-power weapons such as electromagnetic railguns for obtaining pin-point accuracy at a very long range electromagnetic launch systems for rapid aircraft and missile deployment and higher-power radar and sonar systems for "seeing" farther through both air and water. The US Army funded the development of the high-energy-density biaxially oriented polypropylene (BOPP) capacitor and the high-temperature polyetherimide dielectric for ground vehicles to realize better serviceability, higher power, and lower mass of the equipment that ground troops carry. [2,3] Although the energy density has been improved up to 3 J cm −3 via metallization control, the performance, and lifetime of BOPP capacitors degrade rapidly with increasing temperature (the ripple current handing capability decreases as the temperature increases from 85 to 105 °C).Improvements in the fault resistance and the reliability of dielectric materials will enable capacitors to withstand higher electrical current and heat without being excessively derated under extreme stress conditions. A large gap remains between the technology availability and the desired properties, such as combined high temperature and energy density and a low dissipation factor. Fa...

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“…Wang provides a detailed account of the application of phase-field approaches to the study of ferroelectric phase transformations and domain mechanisms [19]. First-principles calculations are carried out to predict hypertoroidal electric moments in ferroelectric nanostructures [20] and to describe the antiferroelectric behavior of PbZrO 3 [21]. The effect of external stresses on the electromechanical properties is treated using a microscopic model [22].…”

mentioning

confidence: 99%

Recent developments in ferroelectric nanostructures and multilayers

2009

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The property of ferroelectricity was first reported in 1921 in Rochelle salt (sodium potassium tartrate). Once considered a rare phenomenon limited to a comparatively small class of crystals, the discovery of ferroelectricity in the binary oxide compound barium titanate (BaTiO 3 ) in the mid-1940s paved the way for rapid advances in the search of new materials. Since that time, a great many other ferroelectric compounds and solid solutions have been found and there has been broad interest in ferroelectric materials that has continued essentially uninterrupted until the present time. Ferroelectric materials remain subjects of intensive investigation today for three principal reasons. First, the unique dielectric, pyroelectric, piezoelectric, and electro-optic properties exhibited by ferroelectric crystals, ceramics, composites, and thin films can be exploited in great many devices of commercial importance. Second, apart from their many technological applications, ferroelectric materials as a class exhibit a great diversity of phase transitions that make them ideal objects for scientific investigations into the origins and mechanisms of a wide range of structural transformation phenomena. Finally, advances in thin-film deposition and nanoscale fabrication techniques made over the past two decades have created new possibilities for the integration of these materials into the ever expanding array of microelectronic devices.Ferroelectrics form a sub-group of functional (or smart) materials whose physical properties are sensitive to changes in external conditions such as temperature, pressure, and electric fields. Below some critical temperature T C , the dielectric displacement (electric polarization) spontaneously assumes non-zero values in the absence of any externally applied force. The transition between non-ferroelectric and ferroelectric phases is accompanied by a loss of symmetry, characterized by double-well minima below the transition temperature, resulting in a switchable polarization that is accompanied by a hysteresis in the electric field-dielectric displacement response. As a class of materials, ferroelectrics also exhibit unusually large and nonlinear generalized susceptibilities; their dielectric, piezoelectric, elastic, and other properties display critical behavior near the ferroelectric phase transformation temperature. Ferroelectrics may be regarded as high energydensity materials as well that can be configured to store, release or interconvert electrical and mechanical energy in a well-controlled manner. Their exceptionally large piezoelectric compliances, pyroelectric coefficients, and dielectric susceptibilities can be exploited in a variety of microelectronic devices. Important examples of these include piezoelectric sensors and actuators, pyroelectric thermal imaging devices, high-dielectric constant capacitors, electro-optic light valves, and thin-film memories. Because of their strongly non-linear dielectric response ferroelectrics can be utilized in applications such as frequency-agile pha...

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Ab initio study of antiferroelectric PbZrO3 (001) surfaces

Cited by 19 publications

References 23 publications

First-principles calculations of the atomic and electronic structure of SrZrO₃and PbZrO₃(001) and (011) surfaces

First-principles calculations of the atomic and electronic structure of SrZrO₃and PbZrO₃(001) and (011) surfaces

Review of Polymer‐Based Nanodielectric Exploration and Film Scale‐Up for Advanced Capacitors

Recent developments in ferroelectric nanostructures and multilayers

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Ab initio study of antiferroelectric PbZrO3 (001) surfaces

Cited by 19 publications

References 23 publications

First-principles calculations of the atomic and electronic structure of SrZrO3and PbZrO3(001) and (011) surfaces

First-principles calculations of the atomic and electronic structure of SrZrO3and PbZrO3(001) and (011) surfaces

Review of Polymer‐Based Nanodielectric Exploration and Film Scale‐Up for Advanced Capacitors

Recent developments in ferroelectric nanostructures and multilayers

Contact Info

Product

Resources

About

First-principles calculations of the atomic and electronic structure of SrZrO₃and PbZrO₃(001) and (011) surfaces

First-principles calculations of the atomic and electronic structure of SrZrO₃and PbZrO₃(001) and (011) surfaces