Condensed Matter Physics Commons^™

Magnetic Anisotropy And Exchange In (001) Textured Fept-Based Nanostructures, Tom George

Department of Physics and Astronomy: Dissertations, Theses, and Student Research

Hard-magnetic L1₀ phase FePt has been demonstrated as a promising candidate for future nanomagnetic applications, especially magnetic recording at areal densities approaching 10 Tb/in². Realization of FePt’s potential in recording media requires control of grain size and intergranular exchange interactions in films with high degrees of L1₀ order and (001) crystalline texture, including high perpendicular magnetic anisotropy. Furthermore, a write-assist mechanism must be employed to overcome the high coercivity of L1₀ FePt nanograins. The research described in this dissertation examines potential solutions to the aforementioned problems. Specifically, a nonepitaxial method of fabricating highly (001) textured …

Interface States In Cofe2O4 Spin-Filter Tunnel Junctions, Pavel V. Lukashev, John D. Burton, Alexander Smogunov, Julian P. Velev, Evgeny Y. Tsymbal

Evgeny Tsymbal Publications

Spin-filter tunneling is a promising way to generate highly spin-polarized current, a key component for spintronics applications. In this paper we explore the tunneling conductance across the spin-filter material CoFe₂O₄ interfaced with Au electrodes, a geometry which provides nearly perfect lattice matching at the CoFe₂O₄/Au(001) interface. Using density functional theory calculations we demonstrate that interface states play a decisive role in controlling the transport spin polarization in this tunnel junction. For a realistic CoFe₂O₄ barrier thickness, we predict a tunneling spin polarization of about −60%. We show that this value …

Polarization-Controlled Ohmic To Schottky Transition At A Metal/Ferroelectric Interface, Xiaohui Liu, Yong Wang, John D. Burton, Evgeny Y. Tsymbal

Evgeny Tsymbal Publications

Ferroelectric polar displacements have recently been observed in conducting electron-doped BaTiO₃ (n-BTO). The coexistence of a ferroelectric phase and conductivity opens the door to new functionalities that may provide a unique route for novel device applications. Using first-principles methods and electrostatic modeling, we explore the effect that the switchable polarization of n-BTO has on the electronic properties of the SrRuO₃/n-BTO (001) interface. Ferroelectric polarization controls the accumulation or depletion of electron charge at the interface, and the associated bending of the n-BTO conduction band determines the transport regime across the interface. The …

Polarization Discontinuity Induced Two-Dimensional Electron Gas At Zno/Zn(Mg)O Interfaces: A First-Principles Study, Jesuan Betancourt, J. J. Saavedra-Arias, John D. Burton, Yasuyuki Ishikawa, Evgeny Y. Tsymbal, Julian P. Velev

Evgeny Tsymbal Publications

The discovery of a high-mobility two-dimensional electron gas (2DEG) in wurtzite ZnO/Zn(Mg)O heterostructures is promising for applications due to the high mobility of the carriers. In this paper, we study the formation and properties of the 2DEG at ZnO/Zn(Mg)O interfaces using first-principles calculations based on hybrid density functional theory. The 2DEG arises from the polarization discontinuity at the interface between the two materials. The uncompensated bound charge at the interface gives rise to an electric field in the bulk of ZnO which confines free carriers close to the interface. We find that the type of the confined carriers is determined …

Ferroelectric And Dielectric Properties Of Electroactive Oligomers And Nanocomposites, Kristin Leigh Kraemer

Department of Physics and Astronomy: Dissertations, Theses, and Student Research

Polyvinylidene fluoride (PVDF) and its copolymers have been well established as ferroelectric polymers. The dielectric and ferroelectric properties for vinylidene fluoride (VDF) oligomer thin films were investigated. By synthesizing oligomers instead of long polymer chains, films with higher crystalinity can be formed and the locations of oligomers can be controlled for applications such as molecular electronics.

Evidence of ferroelectricity was observed in oligomer thin films evaporated onto room temperature substrates and by Langmuir-Blodgett (LB) deposition. Voltage and frequency dependence of the capacitance was measured. Oligomers functionalized with phosphonic acid formed self-assembled monolayers (SAM) on aluminum and mica substrates. Film thickness …

Use Of Zwitterionic Molecules For Forming A Hole Or Electron Transport Layer, Bernard Doudin, Pierre Braunstein, Lucie Routaboul, Guillaume Dalmas, Zhengzheng Zhang, Peter Dowben

Peter Dowben Publications

The invention relates to the use of zwitterionic molecules for forming a hole or electron transport layer. The preferred zwitterionic molecules of the invention are derivatives of p-benzoquinonemonoimines. The invention is useful in the field of electronic devices in particular.

Magnetic Interactions In Low-Dimensional Iron Nanostructures, Rui Zhang

Department of Physics and Astronomy: Dissertations, Theses, and Student Research

Three systems involving low-dimensional magnetic nanostructures, namely the Kondo Effect in Isolated Cu(Fe) Clusters, Magnetization Reversal in Transition-Metal/Fe:SiO₂ Thin Films, and Anisotropy and Micromagnetism of Fe/CrPt Bilayers, have been investigated to understand the magnetic interactions in iron nanostructures.

Kondo Effect in Isolated Cu(Fe) Clusters —Iron impurities were added into copper clusters embedded in an insulating matrix to ensure that the Kondo effect is strictly confined by the size of the cluster. The Kondo temperature of our naoscale system is 0.7 K, which is greatly suppressed from its bulk value of 29 K and is consistent with our theory prediction. …

Anomalous And Spin Hall Effects In A Magnetic Tunnel Junction With Rashba Spin-Orbit Coupling, A. V. Vedyayev, M. S. Titova, N. V. Ryzhanova, M. Ye. Zhuravlev, Evgeny Y. Tsymbal

Evgeny Tsymbal Publications

Anomalous and spin Hall effects are investigated theoretically for a magnetic tunnel junction where the applied voltage produces a Rashba spin-orbit coupling within the tunneling barrier layer. The ferromagnetic electrodes are the source of the spin-polarized current. The tunneling electrons experience a spin-orbit coupling inside the barrier due to the applied electrical field. Charge and spin Hall currents are calculated as functions of the position inside the barrier and the angle between the magnetizations of the electrodes. We find that both charge and spin Hall currents are located inside the barrier near the interfaces. The dependence of the currents on …

Ab-Initio And Model Studies Of Spin Fluctuation Effects In Transport And Thermodynamics Of Magnetic Metals, James K. Glasbrenner

Department of Physics and Astronomy: Dissertations, Theses, and Student Research

Magnetic materials are vital to many devices and the manipulation of spins is central to the operation of novel devices such as spin transistors. It is important to understand the effect of spin fluctuations on such systems. In this dissertation, first-principles calculations and models further the understanding of spin fluctuation effects in the transport and thermodynamics of magnetic metals.

A simple classical spin-fluctuation Hamiltonian with a single itinerancy parameter is studied using the mean-field approximation, Monte Carlo simulations, and a generalized Onsager cavity field method. The results of these different methods are in agreement. It is found that the thermodynamics …

Hydroxyl-Decorated Graphene Systems As Candidates For Organic Metal-Free Ferroelectrics, Multiferroics, And High-Performance Proton Battery Cathode Materials, Menghao Wu, John D. Burton, Evgeny Y. Tsymbal, Xiao Cheng Zeng, Purusottam Jena

Evgeny Tsymbal Publications

Using a first-principles method we show that graphene based materials, functionalized with hydroxyl groups, constitute a class of multifunctional, lightweight, and nontoxic organic materials with functional properties such as ferroelectricity, multiferroicity, and can be used as proton battery cathode materials. For example, the polarizations of semihydroxylized graphane and graphone, as well as fully hydroxylized graphane, are much higher than any organic ferroelectric materials known to date. Further, hydroxylized graphene nanoribbons with proton vacancies at the end can have much larger dipole moments. They may also be applied as high-capacity cathode materials with a specific capacity that is six times larger …

Strain-Mediated Elastic Coupling In Magnetoelectric Nickel/Barium-Titanate Heterostructures, Robert Streubel, Denny Köhler, Rudolf Schäfer, Lukas M. Eng

Robert Streubel Papers

Multiferroic nanomaterials bear the potential for assembling a manifold of novel and smart devices. For room temperature (RT) applications, however, only the BiFeO3 single-phase perovskites are potential candidates to date. Nevertheless, vertical heterostructures separating magnetic and ferroelectric functionality into different layers are now widely proposed to circumvent this lack in materials' availability. We show here that the second approach is very profitable as illustrated by the strain-mediated coupling between such two layers, i.e., a ferroelectric barium titanate single-crystal (BTO) and a magnetostrictive nickel (Ni) thin film. Applying an electric field across the BTO substrate forces the magnetic easy axis in …

Adherent Cells Avoid Polarization Gradients On Periodically Poled Litao3 Ferroelectrics, Christof Christophis, Elisabetta Ada Cavalcanti-Adam, Maximilian Hanke, Kenji Kitamura, Alexei Gruverman, Michael Grunze, Peter A. Dowben, Axel Rosenhahn

Peter Dowben Publications

The response of fibroblast cells to periodically poled LiTaO₃ ferroelectric crystals has been studied. While fibroblast cells do not show morphological differences on the two polarization directions, they show a tendency to avoid the field gradients that occur between polarization domains of the ferroelectric. The response to the field gradients is fully established after one hour, a time at which fibroblasts form their first focal contacts. If suspension cells, with a lower tendency to establish strong surface contacts are used, no influence of the field gradients is observed.

Proton Transfer In Surface-Stabilized Chiral Motifs Of Croconic Acid, Donna A. Kunkel, James Hooper, Scott Simpson, Geoffrey Rojas, Stephen Ducharme, Timothy Usher, Eva Zurek, Axel Enders

Stephen Ducharme Publications

The structure and cooperative proton ordering of two-dimensional sheets of croconic acid were studied with scanning tunneling microscopy and first-principles calculations. Unlike in the crystalline form, which exhibits a pleated, densely packed polar sheet structure, the confinement of the molecules to the surface results in hydrogenbonded chiral clusters and networks. First-principles calculations suggest that the surface stabilizes networks of configurational isomers, which arise from direct hydrogen transfer between their constituent croconic acid monomers. Some of these configurations have a net polarization. It is demonstrated through constrained molecular dynamics simulations that simultaneous proton transfer between any two molecules can occur spontaneously. …

Infrared Phonon Modes In Multiferroic Single-Crystal Fete2o5br, K. H. Miller, X. S. Xu, H. Berger, V. Cracium, Xiaoxiang Xi, C. Martin, G. L. Carr, D. B. Tanner

Xiaoshan Xu Papers

Reflection and transmission as a function of temperature (7–300 K and 5–300 K respectively) have been measured on single crystals of the multiferroic compound FeTe₂O₅Br utilizing light spanning from the far infrared to the visible. The complex dielectric function and other optical properties were obtained via Kramers-Kronig analysis and by fits to a Drude-Lortentz model. Analysis of the anisotropic excitation spectra via Drude-Lorentz fitting and lattice dynamical calculations have led to the observation of 43 of the 53 modes predicted along the b axis of the monoclinic cell. The phonon response parallel to the a and …

Growth Diagram Of La0.7sr0.3mno3 Thin Films Using Pulsed Laser Deposition, Hangwen Guo, Dali Sun, Wenbin Wang, Zheng Gai, Ivan Kravchenko, Jian Shao, Lu Jiang, Thomas Z. Ward, Paul C. Snijders, Lifeng Yin, Jian Shao, Xiaoshan Xu

Xiaoshan Xu Papers

An experimental study was conducted on controlling the growth mode of La_0.7Sr_0.3MnO₃ thin films on SrTiO₃ substrates using pulsed laser deposition (PLD) by tuning growth temperature, pressure, and laser fluence. Different thin film morphology, crystallinity, and stoichiometry have been observed depending on growth parameters. To understand the microscopic origin, the adatom nucleation, step advance processes, and their relationship to film growth were theoretically analyzed and a growth diagram was constructed. Three boundaries between highly and poorly crystallized growth, 2D and 3D growth, stoichiometric and non-stoichiometric growth were identified in the growth diagram. A good …

Room-Temperature Multiferroic Hexagonal Lufeo3 Films, Wenbin Wang, Jun Zhao, Wenbo Wang, Zheng Gai, Nina Balke, Miaofang Chi, Ho Nyung Lee, Wei Tian, Leyi Zhu, Xuemei Cheng, David J. Keavney, Jieyu Yi, Thomas Z. Ward, Paul C. Snijders, Hans M. Christen, Weida Wu, Jian Shen, Xiaoshan Xu

Xiaoshan Xu Papers

The crystal and magnetic structures of single-crystalline hexagonal LuFeO₃ films have been studied using x-ray, electron, and neutron diffraction methods. The polar structure of these films are found to persist up to 1050 K; and the switchability of the polar behavior is observed at room temperature, indicating ferroelectricity. An antiferromagnetic order was shown to occur below 440 K, followed by a spin reorientation resulting in a weak ferromagnetic order below 130 K. This observation of coexisting multiple ferroic orders demonstrates that hexagonal LuFeO₃ films are room-temperature multiferroics.

Stacking Principle And Magic Sizes Of Transition Metal Nanoclusters Based On Generalized Wulff Construction, S. F. Li, X. J. Zhao, X. S. Xu, Y. F. Gao, Zhenyu Zhang

Xiaoshan Xu Papers

Nanoclusters with extra stability at certain cluster sizes are known as magic clusters with exotic properties. The classic Wulff construction principle, which stipulates that the preferred structure of a cluster should minimize its total surface energy, is often invoked in determining the cluster magicity, resulting in close-shelled Mackay icosahedronal clusters with odd-numbered magic sizes of 13, 55, 147, etc. Here we use transition metal clusters around size 55 as prototypical examples to demonstrate that, in the nanometer regime, the classic Wulff construction principle needs to be generalized to primarily emphasize the edge atom effect instead of the surface energy. Specifically, …

Infrared Dielectric Anisotropy And Phonon Modes Of Rutile Tio2, Rafal Korlacki, Stefan Schöche, Tino Hofmann, Tom E. Tiwald, Mathias Schubert

Department of Electrical and Computer Engineering: Faculty Publications

Spectroscopic ellipsometry in the mid-infrared and far-infrared spectral range and generalized ellipsometry in the mid-infrared spectral range are used to investigate the anisotropic dielectric response of rutile TiO₂. The ordinary and extraordinary dielectric function tensor components and all infrared active phonon mode parameters of single crystalline rutile TiO₂ are determined with high accuracy for wavelengths from 3 μm to 83 μm. The data were acquired from samples of (001), (100), and (111) surfaces cut from bulk single crystals. A factorized model dielectric function is employed in order to determine the frequencies and damping parameters of the transverse …

Domain Wall Roughness And Creep In Nanoscale Crystalline Ferroelectric Polymers, Zhengguo Xiao, Shashi Poddar, Stephen Ducharme, X. Hong

Stephen Ducharme Publications

We report piezo-response force microscopy studies of the static and dynamic properties of domain walls (DWs) in 11 to 36 nm thick films of crystalline ferroelectric poly(vinylidene-fluoride-trifluorethylene). The DW roughness exponent ζ ranges from 0.39 to 0.48 and the DW creep exponent µ varies from 0.20 to 0.28, revealing an unexpected effective dimensionality of ~1.5 that is independent of film thickness. Our results suggest predominantly 2D ferroelectricity in the layered polymer and we attribute the fractal dimensionality to DW deroughening due to the correlations between the in-plane and out-of-plane polarization, an effect that can be exploited to achieve high lateral …

Induced Magneto-Electric Coupling In Ferroelectric/Ferromagnetic Heterostructures, Jeffery Carvell, Ruihua Cheng, Peter A. Dowben, Q Yang

Peter Dowben Publications

Using an external magnetic field, we have demonstrated room temperature control of the electric polarization of a ferroelectric polymer, polyvinylidene fluoride (PVDF), in an artificial multiferroic structure. For ferroelectric PVDF polymer thin films in an iron-PVDF-iron heterostructure, both the ferroelectric coercivity and polarization display a hysteresis dependence on the external magnetic field. We also find that the thickness of the PVDF layer has an effect on the magnetoelectric coupling in our samples. We observe a giant magnetoelectric coupling with values as large as 3700 V/cm Oe to 41700 V/cm Oe.

Scaling Of The Coercive Field In Ferroelectrics At The Nanoscale, R. V. Gaynutdinov, M. Minnekaev, S. Mitko, A. L. Tolstikhina, A. Zenkevich, Stephen Ducharme, Vladimir M. Fridkin

Stephen Ducharme Publications

The scaling of the coercive field in ferroelectric films at the nanoscale is investigated experimentally. The scaling in the films of copolymer vinylidene fluoride and BaTiO3 with thickness equal by the order of value to the critical domain nucleus size 1–10 nm reveals deviation from the well-known Kay–Dunn law. At this thickness region coercive field does not depend on thickness and coincides with Landau–Ginzburg–Devonshire value.

Rhodizonic Acid On Noble Metals: Surface Reactivity And Coordination Chemistry, Donna A. Kunkel, James Hooper, Scott Simpson, Sumit Beniwal, Katie L. Morrow, Douglas C. Smith, Kimberly Cousins, Stephen Ducharme, Eva Zurek, Axel Enders

Stephen Ducharme Publications

A study of the two-dimensional crystallization of rhodizonic acid on the crystalline surfaces of gold and copper is presented. Rhodizonic acid, a cyclic oxocarbon related to the ferroelectric croconic acid and the antiferroelectric squaric acid, has not been synthesized in bulk crystalline form yet. Capitalizing on surface-assisted molecular self-assembly, a two-dimensional analogue to the well-known solution-based coordination chemistry, two-dimensional structures of rhodizonic acid were stabilized under ultrahigh vacuum on Au(111) and Cu(111) surfaces. Scanning tunneling microscopy, coupled with first-principles calculations, reveals that on the less reactive Au surface, extended two-dimensional islands of rhodizonic acid are formed, in which the molecules …

Changing Molecular Band Offsets In Polymer Blends Of (P3ht/P(Vdf–Trfe)) Poly(3-Hexylthiophene) And Poly(Vinylidene Fluoride With Trifluoroethylene) Due To Ferroelectric Poling, Freddy Wong, Godohaldo Perez, Manuel Bonilla, Juan A. Colon-Santana, Xin Zhang, Pankaj Sharma, Alexei Gruverman, Peter A. Dowben, Luis G. Rosa

Peter Dowben Publications

Photoelectron emission and inverse photoemission spectroscopy studies of polymer blends of poly(vinylidene fluoride (70%) – trifluoroethylene (30%)) P(VDF–TrFE 70 : 30) and regio-regular poly(3- hexylthiophene) (P3HT) provide evidence of changes in the molecular band offsets as a result of changes in the ferroelectric polarization in P(VDF–TrFE). Investigation of the blends with higher concentrations of the semiconducting P3HT component revealed that the organic semiconductor component of the blend dominates the electronic structure in the vicinity of the chemical potential. Specifically, the states of P3HT at the conduction band minimum and valence band maximum fall within the HOMO–LUMO gap of the dielectric …

Magnetoelectric Coupling At The Euo/Batio3 Interface, Shi Cao, P Liu, Jinke Tang, Haidong Lu, C W. Bark, Sangjin Ryu, Chang-Beom Eom, Alexei Gruverman, Peter A. Dowben

Peter Dowben Publications

Magnetization modulation by ferroelectric polarization switching is reported for the ferromagnetic-ferroelectric EuO/BaTiO₃heterostructure. The value of the magnetization critical exponent β is consistent with the expected Heisenberg-like ferromagnetism of EuO and reported Curie temperature. The critical exponent is seen to decrease with increased magnetic coupling. The results are discussed in the context of data obtained earlier for epitaxial La_0.67Sr_0.33MnO₃/BaTiO₃ heterostructures, where magnetization increases and critical exponent b also declines with ferroelectric polarization pointing away from ferromagnetic layer. The observed similarity between two systems illustrates an importance of charge doping in magnetoelectric coupling, …

Adsorption Of Tcnqh-Functionalized Quinonoid Zwitterions On Gold And Graphene: Evidence For Dominant Intermolecular Interactions+, Lingmei Kong, Lucie Routaboul, Pierre Braunstein, Hong-Gi Park, Jaewu Choi, John P. Colon Cordova, E Vega, Luis G. Rosa, Bernard Doudin, Peter A. Dowben

Peter Dowben Publications

We experimentally investigate the electronic structure of the strongly dipolar, quinonoid-type molecule obtained by TCNQH-functionalization (TCNQH = (NC)₂CC₆H₄CH(CN)₂) of (6Z)-4-(butylamino)-6-(butyliminio)- 3-oxocyclohexa-1,4-dien-1-olate C₆H₂(...NHR)₂(...O)₂ (where R = n-C₄H₉) to be very similar after deposition from solution on either graphene or gold substrates. These zwitterion adsorbate thin films form structures that are distinct from those formed by related quinonoid molecules previously studied. We argue that adsorbate–adsorbate interactions dominate and lead to a Stranski–Krastanov ‘island growth’ mechanism.

Ferroelectric Instability Under Screened Coulomb Interactions, Yong Wang, Xiaohui Liu, John D. Burton, Sitaram S. Jaswal, Evgeny Y. Tsymbal

Evgeny Tsymbal Publications

We explore the effect of charge carrier doping on ferroelectricity using density functional calculations and phenomenological modeling. By considering a prototypical ferroelectric material, BaTiO₃, we demonstrate that ferroelectric displacements are sustained up to the critical concentration of 0.11 electron per unit cell volume. This result is consistent with experimental observations and reveals that the ferroelectric phase and conductivity can coexist. Our investigations show that the ferroelectric instability requires only a short-range portion of the Coulomb force with an interaction range of the order of the lattice constant. These results provide a new insight into the origin of ferroelectricity …

Electron–Phonon Coupling And Structural Phase Transitions On Au/Mo(112), Keisuke Fukutani

Department of Physics and Astronomy: Dissertations, Theses, and Student Research

The electronic structures, many-body interactions and Fermi surface topologies of Au/Mo(112) were investigated in detail and were found to play important roles in the newly discovered order-disorder structural phase transition of the system. First, the high-resolution angle-resolved photoemission spectroscopy was utilized to characterize the electronic band structure of Mo(112) in far greater details than before. This elucidated the existence of several surface-derived states and their dispersion relations in high precisions near the Fermi level, as well as the symmetries of the bulk and surface electronic states, which are in good quantitative agreement with the ab-initio calculations. Such thorough understanding of …

Equilibrium Magnetic States In Individual Hemispherical Permalloy Caps, Robert Streubel, Volodymyr P. Kravchuk, Denis D. Sheka, Denys Makarov, Florian Kronast, Oliver G. Schmidt, Yuri Gaididei

Robert Streubel Papers

The magnetization distributions in individual soft magnetic permalloy caps on non-magnetic spherical particles with sizes ranging from 50 to 800nm are investigated. We experimentally visualize the magnetic structures at the resolution limit of the x-ray magnetic circular dichroism photoelectron emission microscopy (XMCD-PEEM). By analyzing the so-called tail contrast in XMCD-PEEM, the spatial resolution is significantly enhanced, which allowed us to explore magnetic vortices and their displacement on curved surfaces. Furthermore, cap nanostructures are modeled as extruded hemispheres to determine theoretically the phase diagram of equilibrium magnetic states. The calculated phase diagram agrees well with the experimental observations. © 2012 American …

Magnetic Vortices On Closely Packed Spherically Curved Surfaces, Robert Streubel, Denys Makarov, Florian Kronast, Volodymyr Kravchuk, Manfred Albrecht, Oliver G. Schmidt

Robert Streubel Papers

We investigate the change of magnetic vortex states driven by curvature. The equilibrium state and magnetization reversal of soft magnetic permalloy (Py, Ni ₈₀Fe ₂₀) caps on self-assembled spherical particles with diameters of 100, 330, and 800 nm are investigated, revealing the vortex ground state for individual caps and closely packed cap arrays. The magnetic coupling between vortices is substantially reduced due to the shape of the cap as apparent in a much weaker dependence of the magnetization reversal process on the separation distance. Interestingly, the remaining coupling is still sufficiently large to introduce chirality frustrated vortex states …

Out-Of-Surface Vortices In Spherical Shells, Volodymyr P. Kravchuk, Denis D. Sheka, Robert Streubel, Denys Makarov, Oliver G. Schmidt, Yuri Gaididei

Robert Streubel Papers

The interplay of topological defects with curvature is studied for out-of-surface magnetic vortices in thin spherical nanoshells. In the case of an easy-surface Heisenberg magnet it is shown that the curvature of the underlying surface leads to a coupling between the localized out-of-surface component of the vortex with its delocalized in-surface structure, i.e., polarity-chirality coupling. © 2012 American Physical Society.