Atomic, Molecular and Optical Physics Commons^™

Resonant Photoemission Of Rare Earth Doped Gan Thin Films, S. R. Mchale, J. W. Mcclory, J. C. Petrosky, J. Wu, R. Palai, Yaroslav B. Losovyj, Peter A. Dowben

Peter Dowben Publications

The 4d → 4f Fano resonances for various rare earth doped GaN thin films (RE = Gd, Er, Yb) were investigated using synchrotron photoemission spectroscopy. The resonant photoemission Fano profiles show that the major Gd and Er rare earth 4f weight is at about 5–6 eV below the valence band maximum, similar to the 4f weights in the valence band of many other rare earth doped semiconductors. For Yb, there is very little resonant enhancement of the valence band of Yb doped GaN, consistent with a largely 4f¹⁴ occupancy.

Optical Properties Of Quasi-Tetragonal Bifeo3 Thin Films, P. Chen, N. J. Podraza, X. S. Xu, A. Melville, E. Vlahos, V. Gopalan, R. Ramesh, D. G. Schlom, J. L. Musfeldt

Xiaoshan Xu Papers

Optical transmission spectroscopy and spectroscopic ellipsometry were used to extract the optical properties of an epitaxially grown quasi-tetragonal BiFeO₃ thin film in the near infrared to near ultraviolet range. The absorption spectrum is overall blue shifted compared with that of rhombohedral BiFeO₃, with an absorption onset near 2.25 eV, a direct 3.1 eV band gap, and charge transfer excitations that are ~0.4 eV higher than those of the rhombohedral counterpart. We interpret these results in terms of structural strain and local symmetry breaking.

Adsorption-Controlled Growth Of Bimno3 Films By Molecular-Beam Epitaxy, J. H. Lee, X. Ke, R. Misra, J. F. Ihlefeld, X. S. Xu, Z. G. Mei, T. Heeg, M. Roeckerath, J. Schubert, Z. K. Liu, J. L. Musfeldt, P. Schiffer, D. G. Schlom

Xiaoshan Xu Papers

We have developed the means to grow BiMnO₃ thin films with unparalleled structural perfection by reactive molecular-beam epitaxy and determined its band gap. Film growth occurs in an adsorption-controlled growth regime. Within this growth window bounded by oxygen pressure and substrate temperature at a fixed bismuth overpressure, single-phase films of the metastable perovskite BiMnO₃ may be grown by epitaxial stabilization. X-ray diffraction reveals phase-pure and epitaxial films with w rocking curve full width at half maximum values as narrow as 11 arc sec (0.003°). Optical absorption measurements reveal that BiMnO₃ has a direct band gap of 1.1±0.1 …

Dynamical Theory Calculations Of Spin-Echo Resolved Grazing-Incidence Scattering From A Diffraction Grating, Rana Ashkar, P. Stonaha, A. L. Washington, V. R. Shah, M. R. Fitzsimmons, B. Maranville, C. F. Majkrzak, W. T. Lee, W. L. Schaich, Roger Pynn

Nebraska Center for Materials and Nanoscience: Faculty Publications

Neutrons scattered or reflected from a diffraction grating are subject to a periodic potential analogous to the potential experienced by electrons within a crystal. Hence, the wavefunction of the neutrons can be expanded in terms of Bloch waves and a dynamical theory can be applied to interpret the scattering phenomenon. In this paper, a dynamical theory is used to calculate the results of neutron spin-echo resolved grazing-incidence scattering (SERGIS) from a silicon diffraction grating with a rectangular profile. The calculations are compared with SERGIS measurements made on the same grating at two neutron sources: a pulsed source and a continuous …

Lattice Dynamical Probe Of Charge Order And Antipolar Bilayer Stacking In Lufe2o4, X. S. Xu, J. De Groot, Q.-C. Sun, B. C. Sales, D. Mandrus, M. Angst, A. P. Litvinchuk, J. L. Musfeldt

Xiaoshan Xu Papers

We investigated the infrared response of LuFe₂O₄ through the series of charge, magnetic, and structural transitions. All vibrational modes couple strongly to the charge order, whereas the LuO zone-folding modes are also sensitive to magnetic order and structural distortion. The dramatic splitting of the LuO₂ layer mode is attributed to charge-rich/poor proximity effects and its temperature dependence reveals the antipolar nature of the W layer pattern.

Tunable Band Gap In Bi(Fe1−Xmnx)O3 Films, X. S. Xu, J. F. Ihlefeld, J. H. Lee, O. K. Ezekoye, E. Vlahos, R. Ramesh, V. Gopalan, X. Q. Pan, D. G. Schlom, J. L. Musfeldt

Xiaoshan Xu Papers

In order to investigate band gap tunability in polar oxides, we measured the optical properties of a series of Bi(Fe_1−xMn_x)O₃ thin films. The absorption response of the mixed metal solid solutions is approximately a linear combination of the characteristics of the two end members, a result that demonstrates straightforward band gap tunability in this system.

Magnetodielectric Coupling Of Infrared Phonons In Single-Crystal Cu2oseo3, K. H. Miller, X. S. Xu, H. Berger, E. S. Knowles, D. J. Arenas, M. W. Meisel, D. B. Tanner

Xiaoshan Xu Papers

Reflection and transmission as a function of temperature (5–300 K) have been measured on a single crystal of the magnetoelectric ferrimagnetic compound Cu₂OSeO₃ utilizing light spanning the far infrared to the visible portions of the electromagnetic spectrum. The complex dielectric function and optical properties were obtained via Kramers-Kronig analysis and by fits to a Drude-Lortentz model. The fits of the infrared phonons show a magnetodielectric effect near the transition temperature (T_c~60 K). Assignments to strong far-infrared phonon modes have been made, especially those exhibiting anomalous behavior around the transition temperature.

Deposition Of High-Quality Hfo2 On Graphene And The Effect Of Remote Oxide Phonon Scattering, K. Zou, X. Hong, D. Keefer, J. Zhu

Xia Hong Publications

We demonstrate atomic layer deposition of high-quality dielectric HfO₂ films on graphene and determine the magnitude of remote oxide surface phonon scattering in dual-oxide structures. The carrier mobility in these HfO₂-covered graphene samples reaches 20 000 cm²/Vs at low temperature. Distinct contributions to the resistivity from surface optical phonons in the SiO₂ substrate and the HfO₂ overlayer are isolated. At 300 K, surface phonon modes of the HfO₂ film centered at 54 meV limit the mobility to approximately 20 000 cm²/Vs.

Unusual Resistance Hysteresis In N-Layer Graphene Field Effect Transistors Fabricated On Ferroelectric Pb(Zr0.2Ti0.8)O3, X. Hong, J. Hoffman, A. Posadas, K. Zou, C. H. Ahn, J. Zhu

Xia Hong Publications

We have fabricated n-layer graphene field effect transistors on epitaxial ferroelectric Pb(Zr_0.2Ti_0.8)O₃ (PZT) thin films. At low gate voltages, PZT behaves as a high-k dielectric with k up to 100. An unusual resistance hysteresis occurs in gate sweeps at high voltages, with its direction opposite to that expected from the polarization switching of PZT. The relaxation of the metastable state is thermally activated, with an activation barrier of 50–110 meV and a time constant of 6 h at 300 K. We attribute its origin to the slow dissociation/recombination dynamics of water molecules adsorbed at …

Robust Isothermal Electric Control Of Exchange Bias At Room Temperature, Xi He, Ning Wu, Anthony N. Caruso, Elio Vescovo, Kirill D. Belashchenko, Peter A. Dowben, Christian Binek

Kirill Belashchenko Publications

Voltage-controlled spin electronics is crucial for continued progress in information technology. It aims at reduced power consumption, increased integration density and enhanced functionality where non-volatile memory is combined with highspeed logical processing. Promising spintronic device concepts use the electric control of interface and surface magnetization. From the combination of magnetometry, spin-polarized photoemission spectroscopy, symmetry arguments and first-principles calculations, we show that the (0001) surface of magnetoelectric Cr₂O₃ has a roughness-insensitive, electrically switchable magnetization. Using a ferromagnetic Pd/Co multilayer deposited on the (0001) surface of a Cr₂O₃ single crystal, we achieve reversible, room-temperature isothermal switching …

Fluorescence Polarization Of Atomic, Dissociated Atomic, And Molecular Transitions Induced By Spin-Polarized Electron Impact, Jack W. Maseberg

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

Excitation of atoms by spin-polarized electron impact yields fluorescence that can generally exhibit both linear and circular polarization. For experiments where the scattered electrons are not detected, symmetry requires that the electron beam be spin polarized in order for non-zero circular polarization to be observed. Extensive theoretical and experimental investigations have been performed regarding fluorescence polarizations (Stokes parameters) resulting from spin-polarized electron impact excitation of atoms. Measurement of fluorescence polarization provides insight into the angular momentum coupling that exists in the atomic state of interest. It also enables the measurement of electron spin polarization and experimental benchmarking of theoretical atomic …

Optical Properties And Magnetochromism In Multiferroic Bifeo3, X. S. Xu, T. V. Brinzari, S. Lee, Y. H. Chu, L. W. Martin, A. Kumar, S. Mcgill, R. C. Rai, R. Ramesh, V. Gopalan, S. W. Cheong, J. L. Musfeldt

Xiaoshan Xu Papers

In order to investigate spin-charge coupling in multiferroic oxides, we measured the optical properties of BiFeO₃. Although the direct 300 K charge gap is observed at 2.67 eV, absorption onset actually occurs at much lower energy with Fe³⁺ excitations at 1.41 and 1.90 eV. Temperature and magnetic-field-induced spectral changes reveal complex interactions between on-site crystal-field and magnetic excitations in the form of magnon sidebands. We employ the sensitivity of these magnon sidebands to map out the magnetic-fieldtemperature phase diagram which demonstrates optical evidence for spin spiral quenching above 20 T and suggests a spin domain reorientation near …

Magnon Sidebands And Spin-Charge Coupling In Bismuth Ferrite Probed By Nonlinear Optical Spectroscopy, M. O. Ramirez, A. Kumar, S. A. Denev, N. J. Podraza, X. S. Xu, R. C. Rai, Y. H. Chu, J. Seidel, L. W. Martin, S. -Y. Yang, E. Saiz, J. F. Ihlefeld, S. Lee, J. Klug, S. W. Cheong, M. J. Bedzyk, O. Auciello, D. G. Schlom, R. Ramesh, J. Orenstein, J. L. Musfeldt, V. Gopalan

Xiaoshan Xu Papers

The interplay between spin waves (magnons) and electronic structure in materials leads to the creation of additional bands associated with electronic energy levels which are called magnon sidebands. The large difference in the energy scales between magnons (meV) and electronic levels (eV) makes this direct interaction weak and hence makes magnon sidebands difficult to probe. Linear light absorption and scattering techniques at low temperatures are traditionally used to probe these sidebands. Here we show that optical secondharmonic generation, as the lowest-order nonlinear process, can successfully probe the magnon sidebands at room temperature and up to 723 K in bismuth ferrite, …

Electron Attachment To Trans-Azobenzene, Alberto Modelli, Paul Burrow

Paul Burrow Publications

The temporary anion states of gas-phase trans-azobenzene are characterized by means of electron transmission spectroscopy (ETS) in the 0–6 eV range. The measured energies of vertical electron attachment are compared with the energies of the π* virtual orbitals of the neutral molecule supplied by HF (at MP2 optimized geometries) and B3LYP calculations. The calculated energies, scaled with empirical equations, reproduce quantitatively the energies of the corresponding spectral features and predict a positive vertical electron affinity of 0.83 eV.

The total anion current at the walls of the collision chamber and the mass-selected molecular anion current are also reported as …

Absence Of Spin Liquid Behavior In Nd3ga5sio14 Using Magneto-Optical Spectroscopy, X. S. Xu, T. V. Brinzari, S. Mcgill, H. D. Zhou, C. R. Wiebe, J. L. Musfeldt

Xiaoshan Xu Papers

We measured the low-lying crystal field levels of Nd³⁺ in Nd₃Ga₅SiO₁₄ via magneto-optical spectroscopy and employed the extracted energies, magnetic moments, and symmetries to analyze the magnetic properties and test the spin liquid candidacy of this material. The exchange interaction is surprisingly small, a discovery that places severe constraints on models used to describe the ground state of this system. Further, it demonstrates the value of local-probe photophysical techniques for rare-earthcontaining materials where bulk property measurements can be skewed by low-lying electronic structure.

Anisotropic Magnetoresistance And Planar Hall Effect In Epitaxial Films Of La0.7Ca0.3Mno3, N. Naftalis, Y. Bason, J. Hoffman, X. Hong, C. H. Ahn, L. Klein

Xia Hong Publications

We measured the anisotropic magnetoresistance (AMR) and the planar Hall effect (PHE) in a [001] oriented epitaxial thin film of La_0.7Ca_0.3MnO₃ (LCMO) as a function of magnetic field, temperature, and current direction relative to the crystal axes. We find that both AMR and PHE in LCMO depend strongly on the current orientation relative to the crystal axes, and we demonstrate the applicability of AMR and PHE equations based on a fourth order magnetoresistance tensor consistent with the film symmetry.

High-Mobility Few-Layer Graphene Field Effect Transistors Fabricated On Epitaxial Ferroelectric Gate Oxides, X. Hong, A. Posadas, K. Zou, C. H. Ahn, J. Zhu

Xia Hong Publications

The carrier mobility μ of few-layer graphene (FLG) field-effect transistors increases tenfold when the SiO₂ substrate is replaced by single-crystal epitaxial Pb(Zr_0.2Ti_0:8)O₃ (PZT). In the electron-only regime of the FLG, μ reaches 7 X 10⁴ cm² / Vs at 300 K for n = 2.4 X 10¹²=cm², 70% of the intrinsic limit set by longitudinal acoustic (LA) phonons; it increases to 1.4 X 10⁵ cm² / Vs at low temperature. The temperature-dependent resistivity p(T) reveals a clear signature of LA phonon scattering, yielding …

Quantum Scattering Time And Its Implications On Scattering Sources In Graphene, X. Hong, K. Zou, J. Zhu

Xia Hong Publications

We determine the quantum scattering time T_q in six graphene samples with mobility of 4 400<μ <17 000 cm² /V s over a wide range of carrier density (1.2<n<6X10¹²/cm2). T_q derived from Shubnikov–de Haas oscillation ranges ~25–74 fs, corresponding to a single-particle level broadening of 4.5–13 meV. The ratio of the transport to quantum scattering time T_t /T_q spans 1.5–5.1 in these samples, which can be quantitatively understood combining scattering from short-ranged centers and charged impurities located within 2 nm of the graphene sheet. Our results suggest that charges residing on the SiO …

Photoconductivity In Bifeo3 Thin Films, S. R. Basu, L. W. Martin, Y. H. Chu, M. Gajek, R. Ramesh, R. C. Rai, X. S. Xu, J. L. Musfeldt

Xiaoshan Xu Papers

The optical properties of epitaxial BiFeO₃ thin films have been characterized in the visible range. Variable temperature spectra show an absorption onset near 2.17 eV, a direct gap (2.667±0.005 eV at 300 K), and charge transfer excitations at higher energy. Additionally, we report photoconductivity in BiFeO₃ films under illumination from a 100 mW/cm² white light source. A direct correlation is observed between the magnitude of the photoconductivity and postgrowth cooling pressure. Dark conductivities increased by an order of magnitude when comparing films cooled in 760 and 0.1 Torr. Large increases in photoconductivity are observed in light.

Optical Band Gap Of Bifeo3 Grown By Molecular-Beam Epitaxy, J. F. Ihlefeld, N. J. Podraza, Z. K. Liu, R. C. Rai, X. Xu, T. Heeg, Y. B. Chen, J. Li, R. W. Collins, J. L. Musfeldt, X. Q. Pan, J. Schubert, R. Ramesh, D. G. Schlom

Xiaoshan Xu Papers

BiFeO₃ thin films have been deposited on (001) SrTiO₃ substrates by adsorption-controlled reactive molecular-beam epitaxy. For a given bismuth overpressure and oxygen activity, single-phase BiFeO₃ films can be grown over a range of deposition temperatures in accordance with thermodynamic calculations. Four-circle x-ray diffraction reveals phase-pure, epitaxial films with w rocking curve full width at half maximum values as narrow as 29 arc sec (0.008°). Multiple-angle spectroscopic ellipsometry reveals a direct optical band gap at 2.74 eV for stoichiometric as well as 5% bismuth-deficient single-phase BiFeO₃ films.

Charge Order, Dynamics, And Magnetostructural Transition In Multiferroic Lufe2o4, X. S. Xu, M. Angst, T. V. Brinzari, R. P. Hermann, J. L. Musfeldt, A. D. Christianson, D. Mandrus, B. C. Sales, S. Mcgill, J. -W. Kim, Z. Islam

Xiaoshan Xu Papers

We investigated the series of temperature and field-driven transitions in LuFe₂O₄ by optical and Mossbauer spectroscopies, magnetization, and x-ray scattering in order to understand the interplay between charge, structure, and magnetism in this multiferroic material. We demonstrate that charge fluctuation has an onset well below the charge ordering transition, supporting the ‘‘order by fluctuation’’ mechanism for the development of charge order superstructure. Bragg splitting and large magneto-optical contrast suggest a low-temperature monoclinic distortion that can be driven by both temperature and magnetic field.

Unoccupied Orbital Energies Of 1,4-Benzenedithiol And The Homo–Lumo Gap, Adam M. Scheer, Gordon A. Gallup, Paul Burrow

Paul Burrow Publications

The energies of the temporary anion states of 1,4-benzenedithiol (BDT) are determined by electron scattering and compared with those computed by density functional theory (DFT) and Hartree–Fock (HF) methods. Using semi-empirical scalings derived from the ionization energies and electron affinities of a series of phenyl–ethynyl compounds, we compute the HOMO–LUMO energy gap of BDT. We show that without such scalings the gap is substantially underestimated using DFT and overestimated using HF methods. Scaled gaps are also determined for several related compounds and compared with experimental measurements in the literature.

Are There Π* Shape Resonances In Electron Scattering From Phosphate Groups?, Paul Burrow, Gordon A. Gallup, Alberto Modelli

Paul Burrow Publications

The temporary anion states of trimethyl phosphate and several compounds bearing the P=O group were explored using electron transmission spectroscopy and ab initio calculations to determine if these states have the characteristics of the π* resonances usually associated with multiple bonds. No evidence was found for this in (CH₃O)₃PO and, by extension, we do not expect them to appear in the phosphate group of DNA. Cl₃PO, however, does display such characteristics to some extent, and we show that they arise from the spatial properties of the π* (P-Cl) orbitals rather than from multiple PO …

Anisotropic Magnetoresistance In Colossal Magnetoresistive La1−XsrXMno3 Thin Films, Jeng-Bang Yau, X. Hong, A. Posadas, C. H. Ahn, W. Gao, E. Altman, Y. Bason, L. Klein, M. Sidorov, Z. Krivokapic

Xia Hong Publications

We report on magnetic field and temperature-dependent measurements of the anisotropic magnetoresistance (AMR) in epitaxial La_1−xSr_xMnO₃ (LSMO) thin films. While in 3d ferromagnetic alloys increasing the magnetization, either by reducing the temperature or increasing the magnetic field, increases the AMR, we find that in LSMO films the AMR dependence on magnetization displays nonmonotonic behavior which becomes particularly pronounced in lightly doped compounds. We believe that this behavior is related to the inhomogeneity exhibited by these materials.

Magnetic Enhancement In Cobalt-Manganese Alloy Clusters, Shuangye Yin, Ramiro Moro, Xiaoshan Xu, Walter A. De Heer

Xiaoshan Xu Papers

Magnetic moments of Co_NMn_M and Co_NV_M clusters (N ≤ 60; M ≤ N/3) are measured in molecular beams using the Stern-Gerlach deflection method. Surprisingly, the per atom average moments of Co_NMn_M clusters are found to increase with Mn concentration, in contrast to bulk CoMn. The enhancement with Mn doping is found to be independent of cluster size and composition in the size range studied. Meanwhile, Co_NV_M clusters show reduction of average moments with increasing V doping, consistent with what is expected in bulk CoV. The results are …

A Relation Between Energies Of The Short-Lived Negative Ion States And Energies Of Unfilled Molecular Orbitals For A Series Of Bromoalkanes, S. A. Pshenichnyuk, N. L. Asfandiarov, Paul Burrow

Paul Burrow Publications

A series of bromoalkanes was investigated by means of electron transmission spectroscopy in the gas phase. Experimental values of vertical electron affinities associated with occupation of the LUMO by an incoming electron were assigned using ab initio quantum chemical calculations. The predicted vertical electron affinity values differ from measured ones by at most ±0.2 eV.

Planar Hall Effect In Epitaxial Thin Films Of Magnetite, Y. Bason, L. Klein, H. Q. Wang, J. Hoffman, X. Hong, V. E. Henrich, C. H. Ahn

Xia Hong Publications

We measured the planar Hall effect (PHE) of magnetite (Fe₃O₄) films between 150 and 350 K. The PHE was measured both with a constant magnetic field rotating in the plane of the sample and in a remanent state after applying a field in specific directions. The PHE amplitude decreases with temperature; however, it changes little between 300 and 350 K. The remanent PHE signal is as high as 10 V/A, larger than previously observed in manganite films. We also measured the PHE in the remanent state and found that its magnitude and stability make it a …

Low-Energy Electron Capture By 6-Aza-2-Thiothymine: Investigations By Electron Attachment And Electron Transmission Spectroscopies, Stanislav A. Pshenichnyuk, Gordon A. Gallup, Paul Burrow

Paul Burrow Publications

The interaction of low-energy (0-10 eV) electrons with 6-aza-2-thiothymine is investigated in the gas phase by studies of sharp structure in the total electron scattering cross section and by mass analysis of the stable or long-lived negative ions produced by electron attachment. The most efficient fragmentation process, occurring at 0.15 eV, involves the ejection of a closed-shell neutral molecule (CH₃CN). Ab initio calculations support our proposal that this process leads to ring closure to form a stable four-member heterocyclic anion. A long-lived parent anion with an approximate lifetime of 75 microseconds is observed near zero electron energy, and …

Planar Hall-Effect Magnetic Random Access Memory, Y. Bason, L. Klein, J.-B. Yau, X. Hong, J. Hoffman, C. H. Ahn

Xia Hong Publications

We suggest a type of magnetic random access memory (MRAM) that is based on the phenomenon of the planar Hall effect (PHE) in magnetic films, and we demonstrate this idea with manganite films. The PHE-MRAM is structurally simpler than the currently developed MRAM that is based on magnetoresistance tunnel junctions, with the tunnel junction structure being replaced by a single-layer film.

Ferromagnetism And Structure Of Epitaxial Cr-Doped Anatase Tio2 Thin Films, T. C. Kaspar, T. Droubay, V. Shutthanandan, S. M. Heald, C. M. Wang, D. E. Mccready, S. Thevuthasan, J. D. Bryan, D. R. Gamelin, A. J. Kellock, M. F. Toney, X. Hong, C. H. Ahn, S. A. Chambers

Xia Hong Publications

The materials and magnetic properties of Cr-doped anatase TiO₂ thin films deposited on LaAlO₃(001) and SrTiO₃(001) substrates by oxygen-plasma-assisted molecular beam epitaxy have been studied in detail to elucidate the origin of ferromagnetic ordering. Cr substitution for Ti in the anatase lattice, with no evidence of Cr interstitials, segregation, or secondary phases, was independently confirmed by transmission electron microscopy with energy dispersive x-ray spectroscopy, extended x-ray absorption fine structure, and Rutherford backscattering spectrometry in the channeling geometry. Epitaxial films deposited at ~0.1 Å/ s were found to have a highly defected crystalline structure, as quantified …