High Performance Nuclear Magnetic Resonance Imaging Using Magnetic Resonance Force Microscopy

DTIC Science & Technology

2013-12-12

Micron- Size Ferromagnet . Physical Review Letters, 92(3) 037205 (2004) [22] A. Z. Genack and A. G. Redeld. Theory of nuclear spin diusion in a...perform spatially resolved scanned probe studies of spin dynamics in nanoscale ensembles of few electron spins of varying size . Our research culminated...perform spatially resolved scanned probe studies of spin dynamics in nanoscale ensembles of few electron spins of varying size . Our research culminated

Spin resolved electronic transport through N@C20 fullerene molecule between Au electrodes: A first principles study

NASA Astrophysics Data System (ADS)

Caliskan, Serkan

2018-05-01

Using first principles study, through Density Functional Theory combined with Non Equilibrium Green's Function Formalism, electronic properties of endohedral N@C20 fullerene molecule joining Au electrodes (Au-N@C20) was addressed in the presence of spin property. The electronic transport behavior across the Au-N@C20 molecular junction was investigated by spin resolved transmission, density of states, molecular orbitals, differential conductance and current-voltage (I-V) characteristics. Spin asymmetric variation was clearly observed in the results due to single N atom encapsulated in the C20 fullerene cage, where the N atom played an essential role in the electronic behavior of Au-N@C20. This N@C20 based molecular bridge, exhibiting a spin dependent I-V variation, revealed a metallic behavior within the bias range from -1 V to 1 V. The induced magnetic moment, spin polarization and other relevant quantities associated with the spin resolved transport were elucidated.

Spin-resolved band structure of a densely packed Pb monolayer on Si(111)

NASA Astrophysics Data System (ADS)

Brand, C.; Muff, S.; Fanciulli, M.; Pfnür, H.; Tringides, M. C.; Dil, J. H.; Tegenkamp, C.

2017-07-01

Monolayer structures of Pb on Si(111) attracted recently considerable interest as superconductivity was found in these truly two-dimensional (2D) structures. In this study, we analyzed the electronic surface band structure of the so-called striped incommensurate Pb phase with 4/3 ML coverage by means of spin-resolved photoemission spectroscopy. Our results fully agree with density functional theory calculations done by Ren et al. [Phys. Rev. B 94, 075436 (2016), 10.1103/PhysRevB.94.075436]. We observe a local Zeeman-type splitting of a fully occupied and spin-polarized surface band at the K¯√{3} points. The growth of this densely packed Pb structure results in the formation of imbalanced rotational domains, which triggered the detection of C3 v symmetry forbidden spin components for surface states around the Fermi energy. Moreover, the Fermi surface of the metallic surface state of this phase is Rashba spin split and revealed a pronounced warping. However, the 2D nesting vectors are incommensurate with the atomic structure, thus keeping this system rather immune against charge density wave formation and possibly enabling a superconducting behavior.

Magneto-electronic properties and spin-resolved I-V curves of a Co/GeSe heterojunction diode: an ab initio study

NASA Astrophysics Data System (ADS)

Makinistian, Leonardo; Albanesi, Eduardo A.

2013-06-01

We present ab initio calculations of magnetoelectronic and transport properties of the interface of hcp Cobalt (001) and the intrinsic narrow-gap semiconductor germanium selenide (GeSe). Using a norm-conserving pseudopotentials scheme within DFT, we first model the interface with a supercell approach and focus on the spin-resolved densities of states and the magnetic moment (spin and orbital components) at the different atomic layers that form the device. We also report a series of cuts (perpendicular to the plane of the heterojunction) of the electronic and spin densities showing a slight magnetization of the first layers of the semiconductor. Finally, we model the device with a different scheme: using semiinfinite electrodes connected to the heterojunction. These latter calculations are based upon a nonequilibrium Green's function approach that allows us to explore the spin-resolved electronic transport under a bias voltage (spin-resolved I-V curves), revealing features of potential applicability in spintronics.

Trigonal warping induced unusual spin texture and strong spin polarization in graphene with the Rashba effect

NASA Astrophysics Data System (ADS)

Ma, Da-Shuai; Yu, Zhi-Ming; Pan, Hui; Yao, Yugui

2018-02-01

We study the electronic and scattering properties of graphene with moderate Rashba spin-orbit coupling (SOC). The Rashba SOC in graphene tends to distort the band structure and gives rise to a trigonally warped Fermi surface. For electrons at a pronouncedly warped Fermi surface, the spin direction exhibits a staircase profile as a function of the momentum, making an unusual spin texture. We also study the spin-resolved scattering on a Rashba barrier and find that the trigonal warping is essential for producing spin polarization of the transmitted current. Particularly, both the direction and strength of the spin polarization can be controlled by kinds of electric methods. Our work unveils that not only SOC but also the geometry of the Fermi surface is important for generating spin polarization.

Electrically tunable spin filtering for electron tunneling between spin-resolved quantum Hall edge states and a quantum dot

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kiyama, H., E-mail: kiyama@meso.t.u-tokyo.ac.jp; Fujita, T.; Teraoka, S.

2014-06-30

Spin filtering with electrically tunable efficiency is achieved for electron tunneling between a quantum dot and spin-resolved quantum Hall edge states by locally gating the two-dimensional electron gas (2DEG) leads near the tunnel junction to the dot. The local gating can change the potential gradient in the 2DEG and consequently the edge state separation. We use this technique to electrically control the ratio of the dot–edge state tunnel coupling between opposite spins and finally increase spin filtering efficiency up to 91%, the highest ever reported, by optimizing the local gating.

Femtosecond manipulation of spins, charges, and ions in nanostructures, thin films, and surfaces

PubMed Central

Carbone, F.; Hengsberger, M.; Castiglioni, L.; Osterwalder, J.

2017-01-01

Modern ultrafast techniques provide new insights into the dynamics of ions, charges, and spins in photoexcited nanostructures. In this review, we describe the use of time-resolved electron-based methods to address specific questions such as the ordering properties of self-assembled nanoparticles supracrystals, the interplay between electronic and structural dynamics in surfaces and adsorbate layers, the light-induced control of collective electronic modes in nanowires and thin films, and the real-space/real-time evolution of the skyrmion lattice in topological magnets. PMID:29308416

Magnetic tunnel spin injectors for spintronics

NASA Astrophysics Data System (ADS)

Wang, Roger

Research in spin-based electronics, or "spintronics", has a universal goal to develop applications for electron spin in a broad range of electronics and strives to produce low power nanoscale devices. Spin injection into semiconductors is an important initial step in the development of spintronic devices, with the goal to create a highly spin polarized population of electrons inside a semiconductor at room temperature for study, characterization, and manipulation. This dissertation investigates magnetic tunnel spin injectors that aim to meet the spin injection requirements needed for potential spintronic devices. Magnetism and spin are inherently related, and chapter 1 provides an introduction on magnetic tunneling and spintronics. Chapter 2 then describes the fabrication of the spin injector structures studied in this dissertation, and also illustrates the optical spin detection technique that correlates the measured electroluminescence polarization from quantum wells to the electron spin polarization inside the semiconductor. Chapter 3 reports the spin injection from the magnetic tunnel transistor (MTT) spin injector, which is capable of producing highly spin polarized tunneling currents by spin selective scattering in its multilayer structure. The MTT achieves ˜10% lower bound injected spin polarization in GaAs at 1.4 K. Chapter 4 reports the spin injection from CoFe-MgO(100) tunnel spin injectors, where spin dependent tunneling through MgO(100) produces highly spin polarized tunneling currents. These structures achieve lower bound spin polarizations exceeding 50% at 100 K and 30% in GaAs at 290 K. The CoFe-MgO spin injectors also demonstrate excellent thermal stability, maintaining high injection efficiencies even after exposure to temperatures of up to 400 C. Bias voltage and temperature dependent studies on these structures indicate a significant dependence of the electroluminescence polarization on the spin and carrier recombination lifetimes inside the semiconductor. Chapter 5 investigates these spin and carrier lifetime effects on the electroluminescence polarization using time resolved optical techniques. These studies suggest that a peak in the carrier lifetime with temperature is responsible for the nonmonotonic temperature dependence observed in the electroluminescence polarization, and that the initially injected spin polarization from CoFe-MgO spin injectors is a nearly temperature independent ˜70% from 10 K up to room temperature.

Gapped electronic structure of epitaxial stanene on InSb(111)

DOE PAGES

Xu, Cai-Zhi; Chan, Yang-Hao; Chen, Peng; ...

2018-01-11

We report that stanene (single-layer gray tin), with an electronic structure akin to that of graphene but exhibiting a much larger spin-orbit gap, offers a promising platform for room-temperature electronics based on the quantum spin Hall (QSH) effect. This material has received much theoretical attention, but a suitable substrate for stanene growth that results in an overall gapped electronic structure has been elusive; a sizable gap is necessary for room-temperature applications. Here, we report a study of stanene, epitaxially grown on the (111)B-face of indium antimonide (InSb). Angle-resolved photoemission spectroscopy measurements reveal a gap of 0.44 eV, in agreement withmore » our first-principles calculations. Lastly, the results indicate that stanene on InSb(111) is a strong contender for electronic QSH applications.« less

Gapped electronic structure of epitaxial stanene on InSb(111)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Xu, Cai-Zhi; Chan, Yang-Hao; Chen, Peng

We report that stanene (single-layer gray tin), with an electronic structure akin to that of graphene but exhibiting a much larger spin-orbit gap, offers a promising platform for room-temperature electronics based on the quantum spin Hall (QSH) effect. This material has received much theoretical attention, but a suitable substrate for stanene growth that results in an overall gapped electronic structure has been elusive; a sizable gap is necessary for room-temperature applications. Here, we report a study of stanene, epitaxially grown on the (111)B-face of indium antimonide (InSb). Angle-resolved photoemission spectroscopy measurements reveal a gap of 0.44 eV, in agreement withmore » our first-principles calculations. Lastly, the results indicate that stanene on InSb(111) is a strong contender for electronic QSH applications.« less

Study on spin and optical polarization in a coupled InGaN/GaN quantum well and quantum dots structure.

PubMed

Yu, Jiadong; Wang, Lai; Di Yang; Zheng, Jiyuan; Xing, Yuchen; Hao, Zhibiao; Luo, Yi; Sun, Changzheng; Han, Yanjun; Xiong, Bing; Wang, Jian; Li, Hongtao

2016-10-19

The spin and optical polarization based on a coupled InGaN/GaN quantum well (QW) and quantum dots (QDs) structure is investigated. In this structure, spin-electrons can be temporarily stored in QW, and spin injection from the QW into QDs via spin-conserved tunneling is enabled. Spin relaxation can be suppressed owing to the small energy difference between the initial state in the QW and the final states in the QDs. Photoluminescence (PL) and time-resolved photoluminescence (TRPL) measurements are carried out on optical spin-injection and -detection. Owing to the coupled structure, spin-conserved tunneling mechanism plays a significant role in preventing spin relaxation process. As a result, a higher circular polarization degree (CPD) (~49.1%) is achieved compared with conventional single layer of QDs structure. Moreover, spin relaxation time is also extended to about 2.43 ns due to the weaker state-filling effect. This coupled structure is believed an appropriate candidate for realization of spin-polarized light source.

Direct observation of spin-resolved full and empty electron states in ferromagnetic surfaces

DOE Office of Scientific and Technical Information (OSTI.GOV)

Berti, G., E-mail: giulia.berti@polimi.it; Calloni, A.; Brambilla, A.

2014-07-15

We present a versatile apparatus for the study of ferromagnetic surfaces, which combines spin-polarized photoemission and inverse photoemission spectroscopies. Samples can be grown by molecular beam epitaxy and analyzed in situ. Spin-resolved photoemission spectroscopy analysis is done with a hemispherical electron analyzer coupled to a 25 kV-Mott detector. Inverse photoemission spectroscopy experiments are performed with GaAs crystals as spin-polarized electron sources and a UV bandpass photon detector. As an example, measurements on the oxygen passivated Fe(100)-p(1×1)O surface are presented.

Quasi 2D electronic states with high spin-polarization in centrosymmetric MoS2 bulk crystals

NASA Astrophysics Data System (ADS)

Gehlmann, Mathias; Aguilera, Irene; Bihlmayer, Gustav; Młyńczak, Ewa; Eschbach, Markus; Döring, Sven; Gospodarič, Pika; Cramm, Stefan; Kardynał, Beata; Plucinski, Lukasz; Blügel, Stefan; Schneider, Claus M.

2016-06-01

Time reversal dictates that nonmagnetic, centrosymmetric crystals cannot be spin-polarized as a whole. However, it has been recently shown that the electronic structure in these crystals can in fact show regions of high spin-polarization, as long as it is probed locally in real and in reciprocal space. In this article we present the first observation of this type of compensated polarization in MoS2 bulk crystals. Using spin- and angle-resolved photoemission spectroscopy (ARPES), we directly observed a spin-polarization of more than 65% for distinct valleys in the electronic band structure. By additionally evaluating the probing depth of our method, we find that these valence band states at the point in the Brillouin zone are close to fully polarized for the individual atomic trilayers of MoS2, which is confirmed by our density functional theory calculations. Furthermore, we show that this spin-layer locking leads to the observation of highly spin-polarized bands in ARPES since these states are almost completely confined within two dimensions. Our findings prove that these highly desired properties of MoS2 can be accessed without thinning it down to the monolayer limit.

Electronic structure reconstruction across the antiferromagnetic transition in TaFe₁̣₂₃Te₃ spin ladder

DOE PAGES

Xu, Min; Wang, Li -Min; Peng, Rui; ...

2015-02-01

With angle-resolved photoemission spectroscopy, we studied the electronic structure of TaFe₁̣₂₃Te₃, a two-leg spin ladder compound with a novel antiferromagnetic ground state. Quasi-two-dimensional Fermi surface is observed, with sizable inter-ladder hopping. Moreover, instead of observing an energy gap at the Fermi surface in the antiferromagnetic state, we observed the shifts of various bands. Combining these observations with density-functional-theory calculations, we propose that the large scale reconstruction of the electronic structure, caused by the interactions between coexisting itinerant electrons and local moments, is most likely the driving force of the magnetic transition. Thus TaFe₁̣₂₃Te₃ serves as a simpler platform that containsmore » similar ingredients as the parent compounds of iron-based superconductors.« less

Insight into spin transport in oxide heterostructures from interface-resolved magnetic mapping

DOE PAGES

Bruno, F. Y.; Grisolia, M. N.; Visani, C.; ...

2015-02-17

At interfaces between complex oxides, electronic, orbital and magnetic reconstructions may produce states of matter absent from the materials involved, offering novel possibilities for electronic and spintronic devices. Here we show that magnetic reconstruction has a strong influence on the interfacial spin selectivity, a key parameter controlling spin transport in magnetic tunnel junctions. In epitaxial heterostructures combining layers of antiferromagnetic LaFeO 3 (LFO) and ferromagnetic La 0.7Sr 0.3MnO 3 (LSMO), we find that a net magnetic moment is induced in the first few unit planes of LFO near the interface with LSMO. Using X-ray photoemission electron microscopy, we show thatmore » the ferromagnetic domain structure of the manganite electrodes is imprinted into the antiferromagnetic tunnel barrier, endowing it with spin selectivity. Finally, we find that the spin arrangement resulting from coexisting ferromagnetic and antiferromagnetic interactions strongly influences the tunnel magnetoresistance of LSMO/LFO/LSMO junctions through competing spin-polarization and spin-filtering effects.« less

Microscopic description of orbital-selective spin ordering in BaMn2As2

NASA Astrophysics Data System (ADS)

Craco, L.; Carara, S. S.

2018-05-01

Using generalized gradient approximation+dynamical mean-field theory, we provide a microscopic description of orbital-selective spin ordering in the tetragonal manganese pnictide BaMn2As2 . We demonstrate the coexistence of local moments and small band-gap electronic states in the parent compound. We also explore the role played by electron/hole doping, showing that the Mott insulating state is rather robust to small removal of electron charge carriers similar to cuprate oxide superconductors. Good qualitative accord between theory and angle-resolved photoemission as well as electrical transport provides support to our view of orbital-selective spin ordering in BaMn2As2 . Our proposal is expected to be an important step to understanding the emergent correlated electronic structure of materials with persisting ordered localized moments coexisting with Coulomb reconstructed nonmagnetic electronic states.

Confinement and Diffusion Effects in Dynamical Nuclear Polarization in Low Dimensional Nanostructures

NASA Astrophysics Data System (ADS)

Henriksen, Dan; Tifrea, Ionel

2012-02-01

We investigate the dynamic nuclear polarization as it results from the hyperfine coupling between nonequilibrium electronic spins and nuclear spins in semiconductor nanostructures. The natural confinement provided by low dimensional nanostructures is responsible for an efficient nuclear spin - electron spin hyperfine coupling [1] and for a reduced value of the nuclear spin diffusion constant [2]. In the case of optical pumping, the induced nuclear spin polarization is position dependent even in the presence of nuclear spin diffusion. This effect should be measurable via optically induced nuclear magnetic resonance or time-resolved Faraday rotation experiments. We discuss the implications of our calculations for the case of GaAs quantum well structures.[4pt] [1] I. Tifrea and M. E. Flatt'e, Phys. Rev. B 84, 155319 (2011).[0pt] [2] A. Malinowski and R. T. Harley, Solid State Commun. 114, 419 (2000).

Time-resolved inner-shell photoelectron spectroscopy: From a bound molecule to an isolated atom

NASA Astrophysics Data System (ADS)

Brauße, Felix; Goldsztejn, Gildas; Amini, Kasra; Boll, Rebecca; Bari, Sadia; Bomme, Cédric; Brouard, Mark; Burt, Michael; de Miranda, Barbara Cunha; Düsterer, Stefan; Erk, Benjamin; Géléoc, Marie; Geneaux, Romain; Gentleman, Alexander S.; Guillemin, Renaud; Ismail, Iyas; Johnsson, Per; Journel, Loïc; Kierspel, Thomas; Köckert, Hansjochen; Küpper, Jochen; Lablanquie, Pascal; Lahl, Jan; Lee, Jason W. L.; Mackenzie, Stuart R.; Maclot, Sylvain; Manschwetus, Bastian; Mereshchenko, Andrey S.; Mullins, Terence; Olshin, Pavel K.; Palaudoux, Jérôme; Patchkovskii, Serguei; Penent, Francis; Piancastelli, Maria Novella; Rompotis, Dimitrios; Ruchon, Thierry; Rudenko, Artem; Savelyev, Evgeny; Schirmel, Nora; Techert, Simone; Travnikova, Oksana; Trippel, Sebastian; Underwood, Jonathan G.; Vallance, Claire; Wiese, Joss; Simon, Marc; Holland, David M. P.; Marchenko, Tatiana; Rouzée, Arnaud; Rolles, Daniel

2018-04-01

Due to its element and site specificity, inner-shell photoelectron spectroscopy is a widely used technique to probe the chemical structure of matter. Here, we show that time-resolved inner-shell photoelectron spectroscopy can be employed to observe ultrafast chemical reactions and the electronic response to the nuclear motion with high sensitivity. The ultraviolet dissociation of iodomethane (CH3I ) is investigated by ionization above the iodine 4 d edge, using time-resolved inner-shell photoelectron and photoion spectroscopy. The dynamics observed in the photoelectron spectra appear earlier and are faster than those seen in the iodine fragments. The experimental results are interpreted using crystal-field and spin-orbit configuration interaction calculations, and demonstrate that time-resolved inner-shell photoelectron spectroscopy is a powerful tool to directly track ultrafast structural and electronic transformations in gas-phase molecules.

Fine- and hyperfine-structure effects in molecular photoionization. I. General theory and direct photoionization.

PubMed

Germann, Matthias; Willitsch, Stefan

2016-07-28

We develop a model for predicting fine- and hyperfine intensities in the direct photoionization of molecules based on the separability of electron and nuclear spin states from vibrational-electronic states. Using spherical tensor algebra, we derive highly symmetrized forms of the squared photoionization dipole matrix elements from which we derive the salient selection and propensity rules for fine- and hyperfine resolved photoionizing transitions. Our theoretical results are validated by the analysis of the fine-structure resolved photoelectron spectrum of O2 reported by Palm and Merkt [Phys. Rev. Lett. 81, 1385 (1998)] and are used for predicting hyperfine populations of molecular ions produced by photoionization.

Valence-band structure of organic radical p-CF3PNN investigated by angle-resolved photoemission spectroscopy

NASA Astrophysics Data System (ADS)

Anzai, Hiroaki; Takakura, Ryosuke; Ono, Yusuke; Ishihara, Suzuna; Sato, Hitoshi; Namatame, Hirofumi; Taniguchi, Masaki; Matsui, Toshiyuki; Noguchi, Satoru; Hosokoshi, Yuko

2018-05-01

We study the electronic structure of p-trifluoromethylphenyl nitronyl nitroxide (p-CF3PNN), which forms a one-dimensional alternating antiferromagnetic chain of molecules, using angle-resolved photoemission spectroscopy. A singly occupied molecular orbital (SOMO) is observed clearly at ∼ 2 eV in the valence-band spectra. The small band gap and the overlap between the SOMO orbitals in the NO groups are associated with the antiferromagnetic interaction between neighboring spins.

Experimental bandstructure of the 5 d transition metal oxide IrO2

NASA Astrophysics Data System (ADS)

Kawasaki, Jason; Nie, Yuefeng; Uchida, Masaki; Schlom, Darrell; Shen, Kyle

2015-03-01

In the 5 d iridium oxides the close energy scales of spin-orbit coupling and electron-electron correlations lead to emergent quantum phenomena. Much research has focused on the ternary iridium oxides, e.g. the Ruddlesden-Poppers An + 1BnO3 n + 1 , which exhibit behavior from metal to antiferromagnetic insulator ground states, share common features with the cuprates, and may host a number of topological phases. The binary rutile IrO2 is another important 5 d oxide, which has technological importance for spintronics due to its large spin Hall effect and also applications in catalysis. IrO2 is expected to share similar physics as its perovskite-based cousins; however, due to bond-length distortions of the IrO6 octahedra in the rutile structure, the extent of similarities remains an open question. Here we use angle-resolved photoemission spectroscopy to perform momentum-resolved measurements of the electronic structure of IrO2 . IrO2 thin films were grown by molecular beam epitaxy on TiO2 (110) substrates using an Ir e-beam source and distilled ozone. Films were subsequently transferred through ultrahigh vacuum to a connected ARPES system. Combined with first-principles calculations we explore the interplay of spin-orbit coupling and correlations in IrO2 .

Ultrafast Study of Dynamic Exchange Coupling in Ferromagnet/Oxide/Semiconductor Heterostructures

NASA Astrophysics Data System (ADS)

Ou, Yu-Sheng

Spintronics is the area of research that aims at utilizing the quantum mechanical spin degree of freedom of electrons in solid-state materials for information processing and data storage application. Since the discovery of the giant magnetoresistance, the field of spintronics has attracted lots of attention for its numerous potential advantages over contemporary electronics, such as less power consumption, high integration density and non-volatility. The realization of a spin battery, defined by the ability to create spin current without associated charge current, has been a long-standing goal in the field of spintronics. The demonstration of pure spin current in ferromagnet/nonmagnetic material hybrid structures by ferromagnetic resonance spin pumping has defined a thrilling direction for this field. As such, this dissertation targets at exploring the spin and magnetization dynamics in ferromagnet/oxide/semiconductor heterostructures (Fe/MgO/GaAs) using time-resolved optical pump-probe spectroscopy with the long-range goal of understanding the fundamentals of FMR-driven spin pumping. Fe/GaAs heterostructures are complex systems that contain multiple spin species, including paramagnetic spins (GaAs electrons), nuclear spins (Ga and As nuclei) and ferromagnetic spins (Fe). Optical pump-probe studies on their interplay have revealed a number of novel phenomena that has not been explored before. As such they will be the major focus of this dissertation. First, I will discuss the effect of interfacial exchange coupling on the GaAs free-carrier spin relaxation. Temperature- and field-dependent spin-resolved pump-probe studies reveal a strong correlation of the electron spin relaxation with carrier freeze-out, in quantitative agreement with a theoretical interpretation that at low temperatures the free-carrier spin lifetime is dominated by inhomogeneity in the local hyperfine field due to carrier localization. Second, we investigate the impact of tunnel barrier thickness on GaAs electron spin dynamics in Fe/MgO/GaAs heterostructures. Comparison of the Larmor frequency between samples with thick and thin MgO barriers reveals a four-fold variation in exchange coupling strength, and investigation of the spin lifetimes argues that inhomogeneity in the local hyperfine field dominates free-carrier spin relaxation across the entire range of barrier thickness. These results provide additional evidence to support the theory of hyperfine-dominated spin relaxation in GaAs. Third, we investigated the origin and dynamics of an emergent spin population by pump power and magnetic field dependent spin-resolved pump-probe studies. Power dependent study confirms its origin to be filling of electronic states in GaAs, and further field dependent studies reveal the impact of contact hyperfine coupling on the dynamics of electron spins occupying distinct electronic states. Beyond above works, we also pursue optical detection of dynamic spin pumping in Fe/MgO/GaAs heterostructures in parallel. I will discuss the development and progress that we have made toward this goal. This project can be simply divided into two phases. In the first phase, we focused on microwave excitation and optical detection of spin pumping. In the second phase, we focused on all-optical excitation and detection of spin pumping. A number of measurement strategies have been developed and executed in both stages to hunt for a spin pumping signal. I will discuss the preliminary data based upon them.

Anomalous High-Energy Waterfall-Like Electronic Structure in 5 d Transition Metal Oxide Sr2IrO4 with a Strong Spin-Orbit Coupling

NASA Astrophysics Data System (ADS)

Liu, Yan; Yu, Li; Jia, Xiaowen; Zhao, Jianzhou; Weng, Hongming; Peng, Yingying; Chen, Chaoyu; Xie, Zhuojin; Mou, Daixiang; He, Junfeng; Liu, Xu; Feng, Ya; Yi, Hemian; Zhao, Lin; Liu, Guodong; He, Shaolong; Dong, Xiaoli; Zhang, Jun; Xu, Zuyan; Chen, Chuangtian; Cao, Gang; Dai, Xi; Fang, Zhong; Zhou, X. J.

2015-08-01

The low energy electronic structure of Sr2IrO4 has been well studied and understood in terms of an effective Jeff = 1/2 Mott insulator model. However, little work has been done in studying its high energy electronic behaviors. Here we report a new observation of the anomalous high energy electronic structure in Sr2IrO4. By taking high-resolution angle-resolved photoemission measurements on Sr2IrO4 over a wide energy range, we have revealed for the first time that the high energy electronic structures show unusual nearly-vertical bands that extend over a large energy range. Such anomalous high energy behaviors resemble the high energy waterfall features observed in the cuprate superconductors. While strong electron correlation plays an important role in producing high energy waterfall features in the cuprate superconductors, the revelation of the high energy anomalies in Sr2IrO4, which exhibits strong spin-orbit coupling and a moderate electron correlation, points to an unknown and novel route in generating exotic electronic excitations.

Anomalous High-Energy Waterfall-Like Electronic Structure in 5 d Transition Metal Oxide Sr2IrO4 with a Strong Spin-Orbit Coupling.

PubMed

Liu, Yan; Yu, Li; Jia, Xiaowen; Zhao, Jianzhou; Weng, Hongming; Peng, Yingying; Chen, Chaoyu; Xie, Zhuojin; Mou, Daixiang; He, Junfeng; Liu, Xu; Feng, Ya; Yi, Hemian; Zhao, Lin; Liu, Guodong; He, Shaolong; Dong, Xiaoli; Zhang, Jun; Xu, Zuyan; Chen, Chuangtian; Cao, Gang; Dai, Xi; Fang, Zhong; Zhou, X J

2015-08-12

The low energy electronic structure of Sr2IrO4 has been well studied and understood in terms of an effective Jeff = 1/2 Mott insulator model. However, little work has been done in studying its high energy electronic behaviors. Here we report a new observation of the anomalous high energy electronic structure in Sr2IrO4. By taking high-resolution angle-resolved photoemission measurements on Sr2IrO4 over a wide energy range, we have revealed for the first time that the high energy electronic structures show unusual nearly-vertical bands that extend over a large energy range. Such anomalous high energy behaviors resemble the high energy waterfall features observed in the cuprate superconductors. While strong electron correlation plays an important role in producing high energy waterfall features in the cuprate superconductors, the revelation of the high energy anomalies in Sr2IrO4, which exhibits strong spin-orbit coupling and a moderate electron correlation, points to an unknown and novel route in generating exotic electronic excitations.

Effect of spin fluctuations on the electronic structure in iron-based superconductors

NASA Astrophysics Data System (ADS)

Heimes, Andreas; Grein, Roland; Eschrig, Matthias

2012-08-01

Magnetic inelastic neutron scattering studies of iron-based superconductors reveal a strongly temperature-dependent spin-fluctuation spectrum in the normal conducting state, which develops a prominent low-energy resonance feature when entering the superconducting state. Angle-resolved photoemission spectroscopy (ARPES) and scanning tunneling spectroscopy (STS) allow us to study the fingerprints of fluctuation modes via their interactions with electronic quasiparticles. We calculate such fingerprints in 122 iron pnictides using an experimentally motivated spin-fluctuation spectrum and make a number of predictions that can be tested in ARPES and STS experiments. This includes discussions of the quasiparticle scattering rate and the superconducting order parameter. In quantitative agreement with experiment we reproduce the quasiparticle dispersions obtained from momentum distribution curves as well as energy distribution curves. We discuss the relevance of the coupling between spin fluctuations and electronic excitations for the superconducting mechanism.

Spin-resolved inelastic mean free path of slow electrons in Fe.

PubMed

Zdyb, R; Bauer, E

2013-07-10

The spin-dependent reflectivity of slow electrons from ultrathin Fe films on W(110) has been measured with spin polarized low energy electron microscopy. From the amplitude of the quantum size oscillations observed in the reflectivity curves the spin-dependent inelastic mean free path (IMFP) of electrons in Fe has been determined in the energy range from 5 to 16 eV above the vacuum level. The resulting IMFP values for the spin-up electrons are clearly larger than those for the spin-down electrons and the difference between the two values decreases with increasing electron energy in agreement with theoretical predictions.

Weak-coupling superconductivity in a strongly correlated iron pnictide

PubMed Central

Charnukha, A.; Post, K. W.; Thirupathaiah, S.; Pröpper, D.; Wurmehl, S.; Roslova, M.; Morozov, I.; Büchner, B.; Yaresko, A. N.; Boris, A. V.; Borisenko, S. V.; Basov, D. N.

2016-01-01

Iron-based superconductors have been found to exhibit an intimate interplay of orbital, spin, and lattice degrees of freedom, dramatically affecting their low-energy electronic properties, including superconductivity. Albeit the precise pairing mechanism remains unidentified, several candidate interactions have been suggested to mediate the superconducting pairing, both in the orbital and in the spin channel. Here, we employ optical spectroscopy (OS), angle-resolved photoemission spectroscopy (ARPES), ab initio band-structure, and Eliashberg calculations to show that nearly optimally doped NaFe0.978Co0.022As exhibits some of the strongest orbitally selective electronic correlations in the family of iron pnictides. Unexpectedly, we find that the mass enhancement of itinerant charge carriers in the strongly correlated band is dramatically reduced near the Γ point and attribute this effect to orbital mixing induced by pronounced spin-orbit coupling. Embracing the true band structure allows us to describe all low-energy electronic properties obtained in our experiments with remarkable consistency and demonstrate that superconductivity in this material is rather weak and mediated by spin fluctuations. PMID:26729630

Coexistence of ferromagnetism and superconductivity in iron based pnictides: a time resolved magnetooptical study.

PubMed

Pogrebna, A; Mertelj, T; Vujičić, N; Cao, G; Xu, Z A; Mihailovic, D

2015-01-13

Ferromagnetism and superconductivity are antagonistic phenomena. Their coexistence implies either a modulated ferromagnetic order parameter on a lengthscale shorter than the superconducting coherence length or a weak exchange coupling between the itinerant superconducting electrons and the localized ordered spins. In some iron based pnictide superconductors the coexistence of ferromagnetism and superconductivity has been clearly demonstrated. The nature of the coexistence, however, remains elusive since no clear understanding of the spin structure in the superconducting state has been reached and the reports on the coupling strength are controversial. We show, by a direct optical pump-probe experiment, that the coupling is weak, since the transfer of the excess energy from the itinerant electrons to ordered localized spins is much slower than the electron-phonon relaxation, implying the coexistence without the short-lengthscale ferromagnetic order parameter modulation. Remarkably, the polarization analysis of the coherently excited spin wave response points towards a simple ferromagnetic ordering of spins with two distinct types of ferromagnetic domains.

Improper magnetic ferroelectricity of nearly pure electronic nature in helicoidal spiral CaMn7O12

NASA Astrophysics Data System (ADS)

Lim, Jin Soo; Saldana-Greco, Diomedes; Rappe, Andrew M.

2018-01-01

Helicoidal magnetic order breaks inversion symmetry in quadruple perovskite CaMn7O12 , generating one of the largest spin-induced ferroelectric polarizations measured to date. Here, the microscopic origin of the polarization, including exchange interactions, coupling to the spin helicity, and charge density redistribution, is explored via first-principles calculations. The B -site Mn4 + (Mn3) spin adopts a noncentrosymmetric configuration, stabilized not only by spin-orbit coupling (SOC), but also by the fully anisotropic Hubbard J parameter in the absence of SOC, to break inversion symmetry and generate polarization. Berry phase computed polarization (Pelec=2169 μ C /m2 ) exhibits nearly pure electronic behavior, with negligible Mn displacements (≈0.7 m Å ). Orbital-resolved density of states shows that p -d orbital mixing is microscopically driven by nonrelativistic exchange striction within the commensurate ionic structure. Persistent electronic polarization induced by helical spin order in the nearly inversion-symmetric ionic crystal lattice suggests opportunities for ultrafast magnetoelectric response.

Ultrafast Time-Resolved Hard X-Ray Emission Spectroscopy on a Tabletop

NASA Astrophysics Data System (ADS)

Miaja-Avila, Luis; O'Neil, Galen C.; Joe, Young I.; Alpert, Bradley K.; Damrauer, Niels H.; Doriese, William B.; Fatur, Steven M.; Fowler, Joseph W.; Hilton, Gene C.; Jimenez, Ralph; Reintsema, Carl D.; Schmidt, Daniel R.; Silverman, Kevin L.; Swetz, Daniel S.; Tatsuno, Hideyuki; Ullom, Joel N.

2016-07-01

Experimental tools capable of monitoring both atomic and electronic structure on ultrafast (femtosecond to picosecond) time scales are needed for investigating photophysical processes fundamental to light harvesting, photocatalysis, energy and data storage, and optical display technologies. Time-resolved hard x-ray (>3 keV ) spectroscopies have proven valuable for these measurements due to their elemental specificity and sensitivity to geometric and electronic structures. Here, we present the first tabletop apparatus capable of performing time-resolved x-ray emission spectroscopy. The time resolution of the apparatus is better than 6 ps. By combining a compact laser-driven plasma source with a highly efficient array of microcalorimeter x-ray detectors, we are able to observe photoinduced spin changes in an archetypal polypyridyl iron complex [Fe (2 ,2'-bipyridine)3]2 + and accurately measure the lifetime of the quintet spin state. Our results demonstrate that ultrafast hard x-ray emission spectroscopy is no longer confined to large facilities and now can be performed in conventional laboratories with 10 times better time resolution than at synchrotrons. Our results are enabled, in part, by a 100- to 1000-fold increase in x-ray collection efficiency compared to current techniques.

Fine- and hyperfine-structure effects in molecular photoionization. I. General theory and direct photoionization

DOE Office of Scientific and Technical Information (OSTI.GOV)

Germann, Matthias; Willitsch, Stefan, E-mail: stefan.willitsch@unibas.ch

2016-07-28

We develop a model for predicting fine- and hyperfine intensities in the direct photoionization of molecules based on the separability of electron and nuclear spin states from vibrational-electronic states. Using spherical tensor algebra, we derive highly symmetrized forms of the squared photoionization dipole matrix elements from which we derive the salient selection and propensity rules for fine- and hyperfine resolved photoionizing transitions. Our theoretical results are validated by the analysis of the fine-structure resolved photoelectron spectrum of O{sub 2} reported by Palm and Merkt [Phys. Rev. Lett. 81, 1385 (1998)] and are used for predicting hyperfine populations of molecular ionsmore » produced by photoionization.« less

Dependence of spin dephasing on initial spin polarization in a high-mobility two-dimensional electron system

NASA Astrophysics Data System (ADS)

Stich, D.; Zhou, J.; Korn, T.; Schulz, R.; Schuh, D.; Wegscheider, W.; Wu, M. W.; Schüller, C.

2007-11-01

We have studied the spin dynamics of a high-mobility two-dimensional electron system in a GaAs/Al0.3Ga0.7As single quantum well by time-resolved Faraday rotation and time-resolved Kerr rotation in dependence on the initial degree of spin polarization, P , of the electrons. By increasing the initial spin polarization from the low- P regime to a significant P of several percent, we find that the spin dephasing time, T2* , increases from about 20to200ps . Moreover, T2* increases with temperature at small spin polarization but decreases with temperature at large spin polarization. All these features are in good agreement with theoretical predictions by Weng and Wu [Phys. Rev. B 68, 075312 (2003)]. Measurements as a function of spin polarization at fixed electron density are performed to further confirm the theory. A fully microscopic calculation is performed by setting up and numerically solving the kinetic spin Bloch equations, including the D’yakonov-Perel’ and the Bir-Aronov-Pikus mechanisms, with all the scattering explicitly included. We reproduce all principal features of the experiments, i.e., a dramatic decrease of spin dephasing with increasing P and the temperature dependences at different spin polarizations.

Electron spin resonance identification di-carbon-related centers in irradiated silicon

NASA Astrophysics Data System (ADS)

Hayashi, S.; Saito, H.; Itoh, K. M.; Vlasenko, M. P.; Vlasenko, L. S.

2018-04-01

A previously unreported electron spin resonance (ESR) spectrum was found in γ-ray irradiated silicon by the detection of the change in microwave photoconductivity arising from spin-dependent recombination (SDR). In the specially prepared silicon crystals doped by 13C isotope, a well resolved hyperfine structure of SDR-ESR lines due to the interaction between electrons and two equivalent carbon atoms having nuclear spin I = 1/2 was observed. The Si-KU4 spectrum is described by spin Hamiltonian for spin S = 1 and of g and D tensors of orthorhombic symmetry with principal values g1 = 2.008, g2 = 2.002, and g3 =2.007; and D1 = ± 103 MHz, D2 = ∓170 MHz, and D3 = ± 67 MHz where axes 1, 2, and 3 are parallel to the [1 1 ¯ 0 ], [110], and [001] crystal axes, respectively. The hyperfine splitting arising from 13C nuclei is about 0.35 mT. A possible microstructure of the detect leading to the Si-KU4 spectrum is discussed.

The adsorption, stability and properties of Mn6Cr Single-Molecule-Magnets studied by means of nc-AFM, STM, XAS and Spin-resolved Photoelectron Spectroscopy

NASA Astrophysics Data System (ADS)

Heinzmann, U.; Gryzia, A.; Helmstedt, A.; Dohmeier, N.; Predatsch, H.; Brechling, A.; Müller, N.; Sacher, M.; Hoeke, V.; Krickemeyer, E.; Glaser, T.; Bouvron, S.; Fonin, M.; Neumann, M.

2012-11-01

The ionic single-molecule-magnet [MnIII6CrIII]3 with corresponding three counterions has been deposited on different surfaces and studied with respect to its structure and its electronic and magnetic properties. This is the first time that spin polarization of photoelectrons ejected by means of circularly polarized synchrotron radiation has been measured in a single-molecule-magnet.

Anomalous High-Energy Waterfall-Like Electronic Structure in 5 d Transition Metal Oxide Sr2IrO4 with a Strong Spin-Orbit Coupling

PubMed Central

Liu, Yan; Yu, Li; Jia, Xiaowen; Zhao, Jianzhou; Weng, Hongming; Peng, Yingying; Chen, Chaoyu; Xie, Zhuojin; Mou, Daixiang; He, Junfeng; Liu, Xu; Feng, Ya; Yi, Hemian; Zhao, Lin; Liu, Guodong; He, Shaolong; Dong, Xiaoli; Zhang, Jun; Xu, Zuyan; Chen, Chuangtian; Cao, Gang; Dai, Xi; Fang, Zhong; Zhou, X. J.

2015-01-01

The low energy electronic structure of Sr2IrO4 has been well studied and understood in terms of an effective Jeff = 1/2 Mott insulator model. However, little work has been done in studying its high energy electronic behaviors. Here we report a new observation of the anomalous high energy electronic structure in Sr2IrO4. By taking high-resolution angle-resolved photoemission measurements on Sr2IrO4 over a wide energy range, we have revealed for the first time that the high energy electronic structures show unusual nearly-vertical bands that extend over a large energy range. Such anomalous high energy behaviors resemble the high energy waterfall features observed in the cuprate superconductors. While strong electron correlation plays an important role in producing high energy waterfall features in the cuprate superconductors, the revelation of the high energy anomalies in Sr2IrO4, which exhibits strong spin-orbit coupling and a moderate electron correlation, points to an unknown and novel route in generating exotic electronic excitations. PMID:26267653

Electron spin dynamics and optical orientation of Mn2+ ions in GaAs

NASA Astrophysics Data System (ADS)

Akimov, I. A.; Dzhioev, R. I.; Korenev, V. L.; Kusrayev, Yu. G.; Sapega, V. F.; Yakovlev, D. R.; Bayer, M.

2013-04-01

We present an overview of spin-related phenomena in GaAs doped with low concentration of Mn-acceptors (below 1018 cm-3). We use the combination of different experimental techniques such as spin-flip Raman scattering and time-resolved photoluminescence. This allows to evaluate the time evolution of both electron and Mn spins. We show that optical orientation of Mn ions is possible under application of weak magnetic field, which is required to suppress the manganese spin relaxation. The optically oriented Mn2+ ions maintain the spin and return part of the polarization back to the electron spin system providing a long-lived electron spin memory. This leads to a bunch of spectacular effects such as non-exponential electron spin decay and spin precession in the effective exchange fields.

Spin polarized and density modulated phases in symmetric electron-electron and electron-hole bilayers.

PubMed

Kumar, Krishan; Moudgil, R K

2012-10-17

We have studied symmetric electron-electron and electron-hole bilayers to explore the stable homogeneous spin phase and the feasibility of inhomogeneous charge-/spin-density ground states. The former is resolved by comparing the ground-state energies in states of different spin polarizations, while the latter is resolved by searching for a divergence in the wavevector-dependent static charge/spin susceptibility. For this endeavour, we have used the dielectric approach within the self-consistent mean-field theory of Singwi et al. We find that the inter-layer interactions tend to change an abrupt spin-polarization transition of an isolated layer into a nearly gradual one, even though the partially spin-polarized phases are not clearly stable within the accuracy of our calculation. The transition density is seen to decrease with a reduction in layer spacing, implying a suppression of spin polarization by inter-layer interactions. Indeed, the suppression shows up distinctly in the spin susceptibility computed from the spin-polarization dependence of the ground-state energy. However, below a critical layer spacing, the unpolarized liquid becomes unstable against a charge-density-wave (CDW) ground state at a density preceding full spin polarization, with the transition density for the CDW state increasing on further reduction in the layer spacing. Due to attractive e-h correlations, the CDW state is found to be more pronounced in the e-h bilayer. On the other hand, the static spin susceptibility diverges only in the long-wavelength limit, which simply represents a transition to the homogeneous spin-polarized phase.

First-principles calculation of the structure and electronic properties of Fe-substituted Bi2Ti2O7

NASA Astrophysics Data System (ADS)

Huang, Jin-Dou; Zhang, Zhenyi; Lin, Feng; Dong, Bin

2017-12-01

We performed first-principles calculations to investigate the formation energy, geometry structure, and electronic property of Fe-doped Bi2Ti2O7 systems with different Fe doping content. The calculated formation energies indicate that the substitutional configurations of Fe-doping Bi2Ti2O7 are easy to obtain under O-rich growth condition, but their thermodynamic stability decreases with the increase of Fe content. The calculated spin-resolved density of states and band structures indicate that the introduction of Fe into Bi2Ti2O7 brings high spin polarization. The spin-down impurity levels in Fe x Bi2-x Ti2O7 and spin-up impurity levels in Fe x Bi2Ti2-x O7 systems locate in the bottom of conduction band and narrow the band gap significantly, thus leading to the absorption of visible light. Interestingly, the impurity states in Fe x Bi2-x Ti2O7 are the efficient separation center of photogenerated electron and hole, and less affected by Fe doping content, in comparison, the levels of impurity band in Fe x Bi2Ti2-x O7 systems are largely effected by the Fe doping content, and high Fe doping content is the key factor to improve the separating rate of photogenerated electron and hole.

Sub-Doppler infrared spectroscopy of propargyl radical (H{sub 2}CCCH) in a slit supersonic expansion

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chang, Chih-Hsuan; Nesbitt, David J.

The acetylenic CH stretch mode (ν{sub 1}) of propargyl (H{sub 2}CCCH) radical has been studied at sub-Doppler resolution (∼60 MHz) via infrared laser absorption spectroscopy in a supersonic slit-jet discharge expansion, where low rotational temperatures (T{sub rot} = 13.5(4) K) and lack of spectral congestion permit improved determination of band origin and rotational constants for the excited state. For the lowest J states primarily populated in the slit jet cooled expansion, fine structure due to the unpaired electron spin is resolved completely, which permits accurate analysis of electron spin-rotation interactions in the vibrationally excited states (ε{sub aa} = − 518.1(1.8),more » ε{sub bb} = − 13.0(3), ε{sub cc} = − 1.8(3) MHz). In addition, hyperfine broadening in substantial excess of the sub-Doppler experimental linewidths is observed due to nuclear spin–electron spin contributions at the methylenic (—CH{sub 2}) and acetylenic (—CH) positions, which permits detailed modeling of the fine/hyperfine structure line contours. The results are consistent with a delocalized radical spin density extending over both methylenic and acetylenic C atoms, in excellent agreement with simple resonance structures as well as ab initio theoretical calculations.« less

Activation of coherent lattice phonon following ultrafast molecular spin-state photo-switching: A molecule-to-lattice energy transfer

PubMed Central

Marino, A.; Cammarata, M.; Matar, S. F.; Létard, J.-F.; Chastanet, G.; Chollet, M.; Glownia, J. M.; Lemke, H. T.; Collet, E.

2015-01-01

We combine ultrafast optical spectroscopy with femtosecond X-ray absorption to study the photo-switching dynamics of the [Fe(PM-AzA)2(NCS)2] spin-crossover molecular solid. The light-induced excited spin-state trapping process switches the molecules from low spin to high spin (HS) states on the sub-picosecond timescale. The change of the electronic state (<50 fs) induces a structural reorganization of the molecule within 160 fs. This transformation is accompanied by coherent molecular vibrations in the HS potential and especially a rapidly damped Fe-ligand breathing mode. The time-resolved studies evidence a delayed activation of coherent optical phonons of the lattice surrounding the photoexcited molecules. PMID:26798836

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chen, S. L., E-mail: shuch@ist.hokudai.ac.jp; Takayama, J.; Murayama, A.

Power-dependent time-resolved optical spin orientation measurements were performed on In{sub 0.1}Ga{sub 0.9}As quantum well (QW) and In{sub 0.5}Ga{sub 0.5}As quantum dot (QD) tunnel-coupled structures with an 8-nm-thick GaAs barrier. A fast transient increase of electron spin polarization was observed at the QW ground state after circular-polarized pulse excitation. The temporal maximum of polarization increased with increasing pumping fluence owing to enhanced spin blocking in the QDs, yielding a highest amplification of 174% with respect to the initial spin polarization. Further elevation of the laser power gradually quenched the polarization dynamics, which was induced by saturated spin filling of both themore » QDs and the QW phase spaces.« less

Spin resolved photoelectron spectroscopy of [Mn6IIICrIII]3 + single-molecule magnets and of manganese compounds as reference layers

NASA Astrophysics Data System (ADS)

Helmstedt, Andreas; Müller, Norbert; Gryzia, Aaron; Dohmeier, Niklas; Brechling, Armin; Sacher, Marc D.; Heinzmann, Ulrich; Hoeke, Veronika; Krickemeyer, Erich; Glaser, Thorsten; Bouvron, Samuel; Fonin, Mikhail; Neumann, Manfred

2011-07-01

Properties of the manganese-based single-molecule magnet [\\mathbf {Mn}^{\\mathbf {I}\\mathbf {I}\\mathbf {I}}_{\\mathbf {6}} \\mathbf {Cr}^{\\mathbf {I}\\mathbf {I}\\mathbf {I}}]^{\\mathbf {3} \\boldsymbol {+}} are studied. It contains six MnIII ions arranged in two bowl-shaped trinuclear triplesalen building blocks linked by a hexacyanochromate and exhibits a large spin ground state of St = 21/2. The dominant structures in the electron emission spectra of [\\mathbf {Mn}^{\\mathbf {I}\\mathbf {I}\\mathbf {I}}_{\\mathbf {6}}\\mathbf {Cr}^{\\mathbf {I}\\mathbf {I}\\mathbf {I}}]^{\\mathbf {3} \\boldsymbol {+}} resonantly excited at the L3-edge are the L3M2, 3M2, 3, L3M2, 3V and L3VV Auger emission groups following the decay of the primary p3/2 core hole state. Significant differences of the Auger spectra from intact and degraded [\\mathbf {Mn}^{\\mathbf {I}\\mathbf {I}\\mathbf {I}}_{\\mathbf {6}}\\mathbf {Cr}^{\\mathbf {I}\\mathbf {I}\\mathbf {I}}]^{\\mathbf {3} \\boldsymbol {+}} show up. First measurements of the electron spin polarization in the L3M2, 3V and L3VV Auger emission peaks from the manganese constituents in [\\mathbf {Mn}^{\\mathbf {I}\\mathbf {I}\\mathbf {I}}_{\\mathbf {6}} \\mathbf {Cr}^{\\mathbf {I}\\mathbf {I}\\mathbf {I}}]^{\\mathbf {3} \\boldsymbol {+}} resonantly excited at the L3-edge near 640 eV by circularly polarized synchrotron radiation are reported. In addition spin resolved Auger electron spectra of the reference substances MnO, Mn2O3 and MnII(acetate)2·4H2O are given. The applicability of spin resolved electron spectroscopy for characterizing magnetic states of constituent atoms compared to magnetic circular dichroism (MCD) is verified: the spin polarization obtained from MnII(acetate)2·4H2O at room temperature in the paramagnetic state compares to the MCD asymmetry revealed for a star-shaped molecule with a Mn4IIO6 core at 5 K in an external magnetic field of 5 T.

Electronic and spin structure of the wide-band-gap topological insulator: Nearly stoichiometric Bi2Te2S

NASA Astrophysics Data System (ADS)

Annese, E.; Okuda, T.; Schwier, E. F.; Iwasawa, H.; Shimada, K.; Natamane, M.; Taniguchi, M.; Rusinov, I. P.; Eremeev, S. V.; Kokh, K. A.; Golyashov, V. A.; Tereshchenko, O. E.; Chulkov, E. V.; Kimura, A.

2018-05-01

We have grown the phase-homogeneous ternary compound with composition Bi2Te1.85S1.15 very close to the stoichiometric Bi2Te2S . The measurements performed with spin- and angle-resolved photoelectron spectroscopy as well as density functional theory and G W calculations revealed a wide-band-gap three-dimensional topological insulator phase. The surface electronic spectrum is characterized by the topological surface state (TSS) with Dirac point located above the valence band and Fermi level lying in the band gap. TSS band dispersion and constant energy contour manifest a weak warping effect near the Fermi level along with in-plane and out-of-plane spin polarization along the Γ ¯-K ¯ line. We identified four additional states at deeper binding energies with high in-plane spin polarization.

Julius Edgar Lilienfeld Prize Talk: Quantum spintronics: abandoning perfection for new technologies

NASA Astrophysics Data System (ADS)

Awschalom, David D.

2015-03-01

There is a growing interest in exploiting the quantum properties of electronic and nuclear spins for the manipulation and storage of information in the solid state. Such schemes offer qualitatively new scientific and technological opportunities by leveraging elements of standard electronics to precisely control coherent interactions between electrons, nuclei, and electromagnetic fields. We provide an overview of the field, including a discussion of temporally- and spatially-resolved magneto-optical measurements designed for probing local moment dynamics in electrically and magnetically doped semiconductor nanostructures. These early studies provided a surprising proof-of-concept that quantum spin states can be created and controlled with high-speed optoelectronic techniques. However, as electronic structures approach the atomic scale, small amounts of disorder begin to have outsized negative effects. An intriguing solution to this conundrum is emerging from recent efforts to embrace semiconductor defects themselves as a route towards quantum machines. Individual defects in carbon-based materials possess an electronic spin state that can be employed as a solid state quantum bit at and above room temperature. Developments at the frontier of this field include gigahertz coherent control, nanofabricated spin arrays, nuclear spin quantum memories, and nanometer-scale sensing. We will describe advances towards quantum information processing driven by both physics and materials science to explore electronic, photonic, and magnetic control of spin. Work supported by the AFOSR, ARO, DARPA, NSF, and ONR.

Electronic Structure, Optical and Transport Properties of Double Perovskite La2NbMnO6: A Theoretical Understanding from DFT Calculations

NASA Astrophysics Data System (ADS)

Parrey, Khursheed Ahmad; Khandy, Shakeel Ahmad; Islam, Ishtihadah; Laref, Amel; Gupta, Dinesh C.; Niazi, Asad; Aziz, Anver; Ansari, S. G.; Khenata, R.; Rubab, Seemin

2018-03-01

Double perovskite La2NbMnO6 was systematically studied using the first-principles calculations. The structural, electronic, optical and transport properties of this compound were calculated. Spin resolved band structure predicted this material as a half-metal with an energy gap of 3.75 eV in spin down state. The optical coefficients including optical conductivity, reflectivity and electron energy loss are calculated for photon energy up to 30.00 eV to understand the optical response of this perovskite. The strong absorption of all the ultraviolet and infrared frequencies of the spectrum by this material may suggest the potential application of this material for the optoelectronic devices in ultraviolet and infra-red region. Also, the thermoelectric properties with a speculation from the half-metallic electronic structure are reported. Subsequently, the Seebeck coefficient, electrical and thermal conductivity coefficients are calculated to predict the thermoelectric figure of merit (zT), the maximum of which is found out to be 0.14 at 800 K.

Detailed Characterization of a Nanosecond-Lived Excited State: X-ray and Theoretical Investigation of the Quintet State in Photoexcited [Fe(terpy)2]2+

PubMed Central

2015-01-01

Theoretical predictions show that depending on the populations of the Fe 3dxy, 3dxz, and 3dyz orbitals two possible quintet states can exist for the high-spin state of the photoswitchable model system [Fe(terpy)2]2+. The differences in the structure and molecular properties of these 5B2 and 5E quintets are very small and pose a substantial challenge for experiments to resolve them. Yet for a better understanding of the physics of this system, which can lead to the design of novel molecules with enhanced photoswitching performance, it is vital to determine which high-spin state is reached in the transitions that follow the light excitation. The quintet state can be prepared with a short laser pulse and can be studied with cutting-edge time-resolved X-ray techniques. Here we report on the application of an extended set of X-ray spectroscopy and scattering techniques applied to investigate the quintet state of [Fe(terpy)2]2+ 80 ps after light excitation. High-quality X-ray absorption, nonresonant emission, and resonant emission spectra as well as X-ray diffuse scattering data clearly reflect the formation of the high-spin state of the [Fe(terpy)2]2+ molecule; moreover, extended X-ray absorption fine structure spectroscopy resolves the Fe–ligand bond-length variations with unprecedented bond-length accuracy in time-resolved experiments. With ab initio calculations we determine why, in contrast to most related systems, one configurational mode is insufficient for the description of the low-spin (LS)–high-spin (HS) transition. We identify the electronic structure origin of the differences between the two possible quintet modes, and finally, we unambiguously identify the formed quintet state as 5E, in agreement with our theoretical expectations. PMID:25838847

Detailed Characterization of a Nanosecond-Lived Excited State: X-ray and Theoretical Investigation of the Quintet State in Photoexcited [Fe(terpy) 2 ] 2+

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vankó, György; Bordage, Amélie; Pápai, Mátyás

2015-03-19

Theoretical predictions show that depending on the populations of the Fe 3dxy, 3dxz, and 3dyz orbitals two possible quintet states can exist for the high-spin state of the photoswitchable model system [Fe(terpy)2]2+. The differences in the structure and molecular properties of these 5B2 and 5E quintets are very small and pose a substantial challenge for experiments to resolve them. Yet for a better understanding of the physics of this system, which can lead to the design of novel molecules with enhanced photoswitching performance, it is vital to determine which high-spin state is reached in the transitions that follow the lightmore » excitation. The quintet state can be prepared with a short laser pulse and can be studied with cutting-edge time-resolved X-ray techniques. Here we report on the application of an extended set of X-ray spectroscopy and scattering techniques applied to investigate the quintet state of [Fe(terpy)2]2+ 80 ps after light excitation. High-quality X-ray absorption, nonresonant emission, and resonant emission spectra as well as X-ray diffuse scattering data clearly reflect the formation of the high-spin state of the [Fe(terpy)2]2+ molecule; moreover, extended X-ray absorption fine structure spectroscopy resolves the Fe-ligand bond-length variations with unprecedented bondlength accuracy in time-resolved experiments. With ab initio calculations we determine why, in contrast to most related systems, one configurational mode is insufficient for the description of the low-spin (LS)-high-spin (HS) transition. We identify the electronic structure origin of the differences between the two possible quintet modes, and finally, we unambiguously identify the formed quintet state as 5E, in agreement with our theoretical expectations.« less

Detailed Characterization of a Nanosecond-Lived Excited State: X-ray and Theoretical Investigation of the Quintet State in Photoexcited [Fe(terpy) 2 ] 2+

DOE PAGES

Vanko, Gyorgy; Bordage, Amelie; Papai, Matyas; ...

2015-03-19

Theoretical predictions show that depending on the populations of the Fe 3d xy, 3d xz, and 3d yz orbitals two possible quintet states can exist for the high-spin state of the photoswitchable model system [Fe(terpy) 2] 2+. The differences in the structure and molecular properties of these 5B2 and 5E quintets are very small and pose a substantial challenge for experiments to resolve them. Yet for a better understanding of the physics of this system, which can lead to the design of novel molecules with enhanced photoswitching performance, it is vital to determine which high-spin state is reached in themore » transitions that follow the light excitation. The quintet state can be prepared with a short laser pulse and can be studied with cutting-edge time-resolved X-ray techniques. Here we report on the application of an extended set of X-ray spectroscopy and scattering techniques applied to investigate the quintet state of [Fe(terpy) 2] 2+ 80 ps after light excitation. High-quality X-ray absorption, nonresonant emission, and resonant emission spectra as well as X-ray diffuse scattering data clearly reflect the formation of the high-spin state of the [Fe(terpy) 2] 2+ molecule; moreover, extended X-ray absorption fine structure spectroscopy resolves the Fe–ligand bond-length variations with unprecedented bond-length accuracy in time-resolved experiments. With ab initio calculations we determine why, in contrast to most related systems, one configurational mode is insufficient for the description of the low-spin (LS)–high-spin (HS) transition. We identify the electronic structure origin of the differences between the two possible quintet modes, and finally, we unambiguously identify the formed quintet state as 5E, in agreement with our theoretical expectations.« less

Optical Orientation of Mn2+ Ions in GaAs in Weak Longitudinal Magnetic Fields

NASA Astrophysics Data System (ADS)

Akimov, I. A.; Dzhioev, R. I.; Korenev, V. L.; Kusrayev, Yu. G.; Sapega, V. F.; Yakovlev, D. R.; Bayer, M.

2011-04-01

We report on optical orientation of Mn2+ ions in bulk GaAs subject to weak longitudinal magnetic fields (B≤100mT). A manganese spin polarization of 25% is directly evaluated by using spin-flip Raman scattering. The dynamical Mn2+ polarization occurs due to the s-d exchange interaction with optically oriented conduction band electrons. Time-resolved photoluminescence reveals a nontrivial electron spin dynamics, where the oriented Mn2+ ions tend to stabilize the electron spins.

Optical orientation of Mn2+ ions in GaAs in weak longitudinal magnetic fields.

PubMed

Akimov, I A; Dzhioev, R I; Korenev, V L; Kusrayev, Yu G; Sapega, V F; Yakovlev, D R; Bayer, M

2011-04-08

We report on optical orientation of Mn2+ ions in bulk GaAs subject to weak longitudinal magnetic fields (B≤100  mT). A manganese spin polarization of 25% is directly evaluated by using spin-flip Raman scattering. The dynamical Mn2+ polarization occurs due to the s-d exchange interaction with optically oriented conduction band electrons. Time-resolved photoluminescence reveals a nontrivial electron spin dynamics, where the oriented Mn2+ ions tend to stabilize the electron spins.

Electron spin polarization (CIDEP) investigation of the interaction of reactive free radicals with polynitroxyl stable free radicals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Turro, N.J.; Khudyakov, I.V.; Dwyer, D.W.

1993-10-14

Time-resolved electron spin resonance (TR ESR) was employed to investigate the polarized ESR (CIDEP) spectra produced by interaction of mono- and polynitroxyls with reactive free radicals (r[sup [number sign

Theoretical study of dynamic electron-spin-polarization via the doublet-quartet quantum-mixed state and time-resolved ESR spectra of the quartet high-spin state.

PubMed

Teki, Yoshio; Matsumoto, Takafumi

2011-04-07

The mechanism of the unique dynamic electron polarization of the quartet (S = 3/2) high-spin state via a doublet-quartet quantum-mixed state and detail theoretical calculations of the population transfer are reported. By the photo-induced electron transfer, the quantum-mixed charge-separate state is generated in acceptor-donor-radical triad (A-D-R). This mechanism explains well the unique dynamic electron polarization of the quartet state of A-D-R. The generation of the selectively populated quantum-mixed state and its transfer to the strongly coupled pure quartet and doublet states have been treated both by a perturbation approach and by exact numerical calculations. The analytical solutions show that generation of the quantum-mixed states with the selective populations after de-coherence and/or accompanying the (complete) dephasing during the charge-recombination are essential for the unique dynamic electron polarization. Thus, the elimination of the quantum coherence (loss of the quantum information) is the key process for the population transfer from the quantum-mixed state to the quartet state. The generation of high-field polarization on the strongly coupled quartet state by the charge-recombination process can be explained by a polarization transfer from the quantum-mixed charge-separate state. Typical time-resolved ESR patterns of the quantum-mixed state and of the strongly coupled quartet state are simulated based on the generation mechanism of the dynamic electron polarization. The dependence of the spectral pattern of the quartet high-spin state has been clarified for the fine-structure tensor and the exchange interaction of the quantum-mixed state. The spectral pattern of the quartet state is not sensitive towards the fine-structure tensor of the quantum-mixed state, because this tensor contributes only as a perturbation in the population transfer to the spin-sublevels of the quartet state. Based on the stochastic Liouville equation, it is also discussed why the selective population in the quantum-mixed state is generated for the "finite field" spin-sublevels. The numerical calculations of the elimination of the quantum coherence (de-coherence and/or dephasing) are demonstrated. A new possibility of the enhanced intersystem crossing pathway in solution is also proposed.

Spin-orbit-driven magnetic structure and excitation in the 5d pyrochlore Cd 2Os 2O 7

DOE PAGES

Calder, Stuart A; Vale, James G.; Bogdanov, Nikolay; ...

2016-06-07

Here, much consideration has been given to the role of spin-orbit coupling (SOC) in 5d oxides, particularly on the formation of novel electronic states and manifested metal-insulator transitions (MITs). SOC plays a dominant role in 5d 5 iridates (Ir 4+), undergoing MITs both concurrent (pyrochlores) and separated (perovskites) from the onset of magnetic order. However, the role of SOC for other 5d configurations is less clear. For example, 5d 3 (Os 5+) systems are expected to have an orbital singlet with reduced effective SOC. The pyrochlore Cd 2Os 2O 7 nonetheless exhibits a MIT entwined with magnetic order phenomenologically similarmore » to pyrochlore iridates. Here, we resolve the magnetic structure in Cd 2Os 2O 7 with neutron diffraction and then via resonant inelastic X-ray scattering determine the salient electronic and magnetic energy scales controlling the MIT. In particular, SOC plays a subtle role in creating the electronic ground state but drives the magnetic order and emergence of a multiple spin-flip magnetic excitation.« less

Generalized GW+Boltzmann Approach for the Description of Ultrafast Electron Dynamics in Topological Insulators.

PubMed

Battiato, Marco; Aguilera, Irene; Sánchez-Barriga, Jaime

2017-07-17

Quantum-phase transitions between trivial insulators and topological insulators differ from ordinary metal-insulator transitions in that they arise from the inversion of the bulk band structure due to strong spin-orbit coupling. Such topological phase transitions are unique in nature as they lead to the emergence of topological surface states which are characterized by a peculiar spin texture that is believed to play a central role in the generation and manipulation of dissipationless surface spin currents on ultrafast timescales. Here, we provide a generalized G W +Boltzmann approach for the description of ultrafast dynamics in topological insulators driven by electron-electron and electron-phonon scatterings. Taking the prototypical insulator Bi 2 Te 3 as an example, we test the robustness of our approach by comparing the theoretical prediction to results of time- and angle-resolved photoemission experiments. From this comparison, we are able to demonstrate the crucial role of the excited spin texture in the subpicosecond relaxation of transient electrons, as well as to accurately obtain the magnitude and strength of electron-electron and electron-phonon couplings. Our approach could be used as a generalized theory for three-dimensional topological insulators in the bulk-conducting transport regime, paving the way for the realization of a unified theory of ultrafast dynamics in topological materials.

Electrical control of flying spin precession in chiral 1D edge states

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nakajima, Takashi; Komiyama, Susumu; Lin, Kuan-Ting

2013-12-04

Electrical control and detection of spin precession are experimentally demonstrated by using spin-resolved edge states in the integer quantum Hall regime. Spin precession is triggered at a corner of a biased metal gate, where electron orbital motion makes a sharp turn leading to a nonadiabatic change in the effective magnetic field via spin-orbit interaction. The phase of precession is controlled by the group velocity of edge-state electrons tuned by gate bias voltage: Spin-FET-like coherent control of spin precession is thus realized by all-electrical means.

Anisotropy of magnetic interactions and spin filter behavior in hexagonal (Ga,Mn)As nanoribbons

NASA Astrophysics Data System (ADS)

Nie, Ya; Lan, Mu; Zhang, Xi; Xiang, Gang

2017-09-01

The electronic and magnetic properties of Mn doped hexagonal GaAs nanoribbons ((Ga,Mn)As NRs) have been investigated using spin-polarized density functional theory (DFT), and the spin-resolved transport behaviors of (Ga,Mn)As NRs have also been studied with non-equilibrium Green function theory. The calculations show that every Mn dopant brings 4 Bohr magneton (μB) magnetic moment and the ground states of (Ga,Mn)As NRs are ferromagnetic (FM). The investigation of magnetic anisotropies shows that magnetic interactions are dependent on both the distribution directions of Mn atoms and the edge effect of the NRs. The studies of electronic structures and transport properties show that incorporation of Mn atom turns GaAs NR from semiconducting to half-metallic, which significantly enhances the spin-up conductivity and strongly weakens the spin-down conductivity, resulting in non-monatomic variations of spin-dependent conductivities. The nearly 100% spin polarization shown in (Ga,Mn)As NR may be used for low dimensional spin filters, even with as large a bias as 0.9 V. Also, (Ga,Mn)As NR can be used to generate a relatively stable spin-polarized current in a wide bias interval.

Rabi oscillation and electron-spin-echo envelope modulation of the photoexcited triplet spin system in silicon

NASA Astrophysics Data System (ADS)

Akhtar, Waseem; Sekiguchi, Takeharu; Itahashi, Tatsumasa; Filidou, Vasileia; Morton, John J. L.; Vlasenko, Leonid; Itoh, Kohei M.

2012-09-01

We report on a pulsed electron paramagnetic resonance (EPR) study of the photoexcited triplet state (S=1) of oxygen-vacancy centers in silicon. Rabi oscillations between the triplet sublevels are observed using coherent manipulation with a resonant microwave pulse. The Hahn echo and stimulated echo decay profiles are superimposed with strong modulations known as electron-spin-echo envelope modulation (ESEEM). The ESEEM spectra reveal a weak but anisotropic hyperfine coupling between the triplet electron spin and a 29Si nuclear spin (I=1/2) residing at a nearby lattice site, that cannot be resolved in conventional field-swept EPR spectra.

Impact of stoichiometry and disorder on the electronic structure of the PbBi2Te4 -xSex topological insulator

NASA Astrophysics Data System (ADS)

Shvets, I. A.; Klimovskikh, I. I.; Aliev, Z. S.; Babanly, M. B.; Sánchez-Barriga, J.; Krivenkov, M.; Shikin, A. M.; Chulkov, E. V.

2017-12-01

Detailed comparative theoretical and experimental study of electronic properties and spin structure was carried out for a series of Pb-based quaternary compounds PbBi2Te4 -xSex . For all values of x , these compounds are theoretically predicted to be topological insulators, possessing at high Se content a remarkably large band gap and a Dirac point isolated from bulk states. Using spin- and angle-resolved photoemission spectroscopy, it was shown that the PbBi2Te2Se2 and PbBi2Te1.4Se2.6 compounds are characterized by well-defined spin-polarized topological surface state in the bulk gap. To define the probable distribution of atoms over the atomic sites for these samples, we performed ab initio calculations in ordered and disordered configurations of the unit cell. We found that theoretical calculations better reproduce photoemission data when Te atoms are placed in the outermost layers of the septuple layer block.

Electronic structure of BaNi2As2

NASA Astrophysics Data System (ADS)

Zhou, Bo; Xu, Min; Zhang, Yan; Xu, Gang; He, Cheng; Yang, L. X.; Chen, Fei; Xie, B. P.; Cui, Xiao-Yu; Arita, Masashi; Shimada, Kenya; Namatame, Hirofumi; Taniguchi, Masaki; Dai, X.; Feng, D. L.

2011-01-01

BaNi2As2, with a first-order phase transition around 131 K, is studied by the angle-resolved photoemission spectroscopy. The measured electronic structure is compared to the local-density approximation calculations, revealing similar large electronlike bands around M¯ and differences along Γ¯-X¯. We further show that the electronic structure of BaNi2As2 is distinct from that of the sibling iron pnictides. Particularly, there is no signature of band folding, indicating no collinear spin-density-wave-related magnetic ordering. Moreover, across the strong first-order phase transition, the band shift exhibits a hysteresis, which is directly related to the significant lattice distortion in BaNi2As2.

High quality atomically thin PtSe2 films grown by molecular beam epitaxy

NASA Astrophysics Data System (ADS)

Yan, Mingzhe; Wang, Eryin; Zhou, Xue; Zhang, Guangqi; Zhang, Hongyun; Zhang, Kenan; Yao, Wei; Lu, Nianpeng; Yang, Shuzhen; Wu, Shilong; Yoshikawa, Tomoki; Miyamoto, Koji; Okuda, Taichi; Wu, Yang; Yu, Pu; Duan, Wenhui; Zhou, Shuyun

2017-12-01

Atomically thin PtSe2 films have attracted extensive research interests for potential applications in high-speed electronics, spintronics and photodetectors. Obtaining high quality thin films with large size and controlled thickness is critical. Here we report the first successful epitaxial growth of high quality PtSe2 films by molecular beam epitaxy. Atomically thin films from 1 ML to 22 ML have been grown and characterized by low-energy electron diffraction, Raman spectroscopy and x-ray photoemission spectroscopy. Moreover, a systematic thickness dependent study of the electronic structure is revealed by angle-resolved photoemission spectroscopy (ARPES), and helical spin texture is revealed by spin-ARPES. Our work provides new opportunities for growing large size single crystalline films to investigate the physical properties and potential applications of PtSe2.

orbital selective correlation reduce in collapse tetragonal phase of CaFe2(As0.935P0.065)2 and electronic structure reconstruction studied by angel resolved photoemission spectroscopy

NASA Astrophysics Data System (ADS)

Zeng, Lingkun

We performed an angle-resolved photoemission spectroscopy (ARPES) study of the CaFe2(As0.935P0.065)2 in the collapse tetragonal(CT) phase and uncollapse tetragonal(UCT) phase. We find in the CT phase the electronic correlation dramatically reduces respective to UCT phase. Meanwhile, the reduction of correlation in CT phase show an orbital selective effect: correlation in dxy reduces the most, and then dxz/yz, while the one in dz2-r2 almost keeps the same. In CT phase, almost all bands sink downwards to higher binding energy, leading to the hole like bands around Brillouin zone(BZ) center sink below EF compared with UCT phase. However, the electron pocket around Brillouin Zone(BZ) corner(M) in UCT phase, forms a hole pocket around BZ center(Z point) in CT phase. Moreover, the dxy exhibits larger movement down to higher binding energy, resulting in farther away from dyz/xz and closer to dxy.We propose the electron filling ,namely high spin state in UCT phase to low spin state in CT phase(due to competing between crystal structure field and Hund's coupling), other than the Fermi surface nesting might be responsible for the absent of magnetic ordering.

Quasiparticle dynamics and spin-orbital texture of the SrTiO3 two-dimensional electron gas.

PubMed

King, P D C; McKeown Walker, S; Tamai, A; de la Torre, A; Eknapakul, T; Buaphet, P; Mo, S-K; Meevasana, W; Bahramy, M S; Baumberger, F

2014-02-27

Two-dimensional electron gases (2DEGs) in SrTiO3 have become model systems for engineering emergent behaviour in complex transition metal oxides. Understanding the collective interactions that enable this, however, has thus far proved elusive. Here we demonstrate that angle-resolved photoemission can directly image the quasiparticle dynamics of the d-electron subband ladder of this complex-oxide 2DEG. Combined with realistic tight-binding supercell calculations, we uncover how quantum confinement and inversion symmetry breaking collectively tune the delicate interplay of charge, spin, orbital and lattice degrees of freedom in this system. We reveal how they lead to pronounced orbital ordering, mediate an orbitally enhanced Rashba splitting with complex subband-dependent spin-orbital textures and markedly change the character of electron-phonon coupling, co-operatively shaping the low-energy electronic structure of the 2DEG. Our results allow for a unified understanding of spectroscopic and transport measurements across different classes of SrTiO3-based 2DEGs, and yield new microscopic insights on their functional properties.

Charge and spin in low-dimensional cuprates

NASA Astrophysics Data System (ADS)

Maekawa, Sadamichi; Tohyama, Takami

2001-03-01

One of the central issues in the study of high-temperature superconducting cuprates which are composed of two-dimensional (2D) CuO2 planes is whether the 2D systems with strong electron correlation behave as a Fermi liquid or a non-Fermi-liquid-like one-dimensional (1D) system with electron correlation. In this article, we start with the detailed examination of the electronic structure in cuprates and study theoretically the spin and charge dynamics in 1D and 2D cuprates. The theoretical background of spin-charge separation in the 1D model systems including the Hubbard and t-J models is presented. The first direct observation of collective modes of spin and charge excitations in a 1D cuprate, which are called spinons and holons respectively, in angle-resolved photoemission spectroscopy (ARPES) experiments is reviewed in the light of the theoretical results based on the numerically exact-diagonalization method. The charge and spin dynamics in 1D insulating cuprates is also discussed in connection with the spin-charge separation. The arguments are extended to the 2D cuprates, and the unique aspects of the electronic properties of high-temperature superconductors are discussed. Special emphasis is placed on the d-wave-like excitations in insulating 2D cuprates observed in ARPES experiments. We explain how the excitations are caused by the spin-charge separation. The charge stripes observed in the underdoped cuprates are examined in connection with spin-charge separation in real space.

Time-resolved lateral spin-caloric transport of optically generated spin packets in n-GaAs

NASA Astrophysics Data System (ADS)

Göbbels, Stefan; Güntherodt, Gernot; Beschoten, Bernd

2018-05-01

We report on lateral spin-caloric transport (LSCT) of electron spin packets which are optically generated by ps laser pulses in the non-magnetic semiconductor n-GaAs at K. LSCT is driven by a local temperature gradient induced by an additional cw heating laser. The spatio-temporal evolution of the spin packets is probed using time-resolved Faraday rotation. We demonstrate that the local temperature-gradient induced spin diffusion is solely driven by a non-equilibrium hot spin distribution, i.e. without involvement of phonon drag effects. Additional electric field-driven spin drift experiments are used to verify directly the validity of the non-classical Einstein relation for moderately doped semiconductors at low temperatures for near band-gap excitation.

Mims electron-nuclear double resonance in LiYF4:Ce3+ crystal

NASA Astrophysics Data System (ADS)

Gafurov, M.; Mamin, G.; Kurkin, I.; Orlinskii, S.

2018-05-01

We report the observation of the pulsed electron-nuclear double resonance (ENDOR) spectra from 19F and 7Li nuclei on impurity Ce3+ ions in LiYF4 crystal. The resolved structure from the nearby and remote nuclei in spectra is observed. The outcome shows that LiYF4:Ce3+ system can be exploited as a convenient matrix for performing spin manipulations and adjusting quantum computation protocols while ENDOR technique is usable for the investigation of electron-nuclear interaction with all the nuclei of the system.

Photoemission study of electronic structure of the half-metallic ferromagnet Co3Sn2S2

NASA Astrophysics Data System (ADS)

Holder, M.; Dedkov, Yu. S.; Kade, A.; Rosner, H.; Schnelle, W.; Leithe-Jasper, A.; Weihrich, R.; Molodtsov, S. L.

2009-05-01

Surface electronic structure of polycrystalline and single-crystalline samples of the half-metallic ferromagnet Co3Sn2S2 was studied by means of angle-resolved and core-level photoemissions. The experiments were performed in temperature regimes both above and below a Curie temperature of 176.9 K. The spectroscopic results are compared to local-spin density approximation band-structure calculations for the bulk samples. It is found that the surface sensitive experimental data are generally reproduced by the bulk computation suggesting that the theoretically predicted half-metallic properties of Co3Sn2S2 are retained at the surface.

Time-resolved x-ray absorption spectroscopy: Watching atoms dance

NASA Astrophysics Data System (ADS)

Milne, Chris J.; Pham, Van-Thai; Gawelda, Wojciech; van der Veen, Renske M.; El Nahhas, Amal; Johnson, Steven L.; Beaud, Paul; Ingold, Gerhard; Lima, Frederico; Vithanage, Dimali A.; Benfatto, Maurizio; Grolimund, Daniel; Borca, Camelia; Kaiser, Maik; Hauser, Andreas; Abela, Rafael; Bressler, Christian; Chergui, Majed

2009-11-01

The introduction of pump-probe techniques to the field of x-ray absorption spectroscopy (XAS) has allowed the monitoring of both structural and electronic dynamics of disordered systems in the condensed phase with unprecedented accuracy, both in time and in space. We present results on the electronically excited high-spin state structure of an Fe(II) molecular species, [FeII(bpy)3]2+, in aqueous solution, resolving the Fe-N bond distance elongation as 0.2 Å. In addition an analysis technique using the reduced χ2 goodness of fit between FEFF EXAFS simulations and the experimental transient absorption signal in energy space has been successfully tested as a function of excited state population and chemical shift, demonstrating its applicability in situations where the fractional excited state population cannot be determined through other measurements. Finally by using a novel ultrafast hard x-ray 'slicing' source the question of how the molecule relaxes after optical excitation has been successfully resolved using femtosecond XANES.

Electron Spin Resonance Studies of Carbonic Anhydrase: Transition Metal Ions and Spin-Labeled Sulfonamides*

PubMed Central

Taylor, June S.; Mushak, Paul; Coleman, Joseph E.

1970-01-01

Electron spin resonance (esr) spectra of Cu(II) and Co(II) carbonic anhydrase, and a spin-labeled sulfonamide complex of the Zn(II) enzyme, are reported. The coordination geometry of Cu(II) bound in the enzyme appears to have approximately axial symmetry. Esr spectra of enzyme complexes with metal-binding anions also show axial symmetry and greater covalency, in the order ethoxzolamide < SH- < N3- ≤ CN-. Well-resolved superhyperfine structure in the spectrum of the cyanide complex suggests the presence of two, and probably three, equivalent nitrogen ligands from the protein. Esr spectra of the Co(II) enzyme and its complexes show two types of Co(II) environment, one typical of the native enzyme and the 1:1 CN- complex, and one typical of a 2:1 CN- complex. Co(II) in the 2:1 complex appears to be low-spin and probably has a coordination number of 5. Binding of a spin-labeled sulfonamide to the active center immobilizes the free radical. The similarity of the esr spectra of spin-labeled Zn(II) and Co(II) carbonic anhydrases suggests that the conformation at the active center is similar in the two metal derivatives. PMID:4320976

Spin-orbit-coupled fermions in an optical lattice clock

NASA Astrophysics Data System (ADS)

Kolkowitz, S.; Bromley, S. L.; Bothwell, T.; Wall, M. L.; Marti, G. E.; Koller, A. P.; Zhang, X.; Rey, A. M.; Ye, J.

2017-02-01

Engineered spin-orbit coupling (SOC) in cold-atom systems can enable the study of new synthetic materials and complex condensed matter phenomena. However, spontaneous emission in alkali-atom spin-orbit-coupled systems is hindered by heating, limiting the observation of many-body effects and motivating research into potential alternatives. Here we demonstrate that spin-orbit-coupled fermions can be engineered to occur naturally in a one-dimensional optical lattice clock. In contrast to previous SOC experiments, here the SOC is both generated and probed using a direct ultra-narrow optical clock transition between two electronic orbital states in 87Sr atoms. We use clock spectroscopy to prepare lattice band populations, internal electronic states and quasi-momenta, and to produce spin-orbit-coupled dynamics. The exceptionally long lifetime of the excited clock state (160 seconds) eliminates decoherence and atom loss from spontaneous emission at all relevant experimental timescales, allowing subsequent momentum- and spin-resolved in situ probing of the SOC band structure and eigenstates. We use these capabilities to study Bloch oscillations, spin-momentum locking and Van Hove singularities in the transition density of states. Our results lay the groundwork for using fermionic optical lattice clocks to probe new phases of matter.

Orbital-occupancy versus charge ordering and the strength of electron correlations in electron-doped CaMnO3.

PubMed

Luo, Weidong; Franceschetti, Alberto; Varela, Maria; Tao, Jing; Pennycook, Stephen J; Pantelides, Sokrates T

2007-07-20

The structural, electronic, and magnetic properties of mixed-valence compounds are believed to be governed by strong electron correlations. Here we report benchmark density-functional calculations in the spin-polarized generalized-gradient approximation (GGA) for the ground-state properties of doped CaMnO(3). We find excellent agreement with all available data, while inclusion of strong correlations in the GGA+U scheme impairs this agreement. We demonstrate that formal oxidation states reflect only orbital occupancies, not charge transfer, and resolve outstanding controversies about charge ordering.

Orbital-Occupancy versus Charge Ordering and the Strength of Electron Correlations in Electron-Doped CaMnO3

NASA Astrophysics Data System (ADS)

Luo, Weidong; Franceschetti, Alberto; Varela, Maria; Tao, Jing; Pennycook, Stephen J.; Pantelides, Sokrates T.

2007-07-01

The structural, electronic, and magnetic properties of mixed-valence compounds are believed to be governed by strong electron correlations. Here we report benchmark density-functional calculations in the spin-polarized generalized-gradient approximation (GGA) for the ground-state properties of doped CaMnO3. We find excellent agreement with all available data, while inclusion of strong correlations in the GGA+U scheme impairs this agreement. We demonstrate that formal oxidation states reflect only orbital occupancies, not charge transfer, and resolve outstanding controversies about charge ordering.

Two-Dimensional Superconductor with a Giant Rashba Effect: One-Atom-Layer Tl-Pb Compound on Si(111).

PubMed

Matetskiy, A V; Ichinokura, S; Bondarenko, L V; Tupchaya, A Y; Gruznev, D V; Zotov, A V; Saranin, A A; Hobara, R; Takayama, A; Hasegawa, S

2015-10-02

A one-atom-layer compound made of one monolayer of Tl and one-third monolayer of Pb on a Si(111) surface having √3×√3 periodicity was found to exhibit a giant Rashba-type spin splitting of metallic surface-state bands together with two-dimensional superconducting transport properties. Temperature-dependent angle-resolved photoelectron spectroscopy revealed an enhanced electron-phonon coupling for one of the spin-split bands. In situ micro-four-point-probe conductivity measurements with and without magnetic field demonstrated that the (Tl, Pb)/Si(111) system transformed into the superconducting state at 2.25 K, followed by the Berezinskii-Kosterlitz-Thouless mechanism. The 2D Tl-Pb compound on Si(111) is believed to be the prototypical object for prospective studies of intriguing properties of the superconducting 2D system with lifted spin degeneracy, bearing in mind that its composition, atomic and electron band structures, and spin texture are already well established.

A theory for bioinorganic chemical reactivity of oxometal complexes and analogous oxidants: the exchange and orbital-selection rules.

PubMed

Usharani, Dandamudi; Janardanan, Deepa; Li, Chunsen; Shaik, Sason

2013-02-19

Over the past decades metalloenzymes and their synthetic models have emerged as an area of increasing research interest. The metalloenzymes and their synthetic models oxidize organic molecules using oxometal complexes (OMCs), especially oxoiron(IV)-based ones. Theoretical studies have helped researchers to characterize the active species and to resolve mechanistic issues. This activity has generated massive amounts of data on the relationship between the reactivity of OMCs and the transition metal's identity, oxidation state, ligand sphere, and spin state. Theoretical studies have also produced information on transition state (TS) structures, reaction intermediates, barriers, and rate-equilibrium relationships. For example, the experimental-theoretical interplay has revealed that nonheme enzymes carry out H-abstraction from strong C-H bonds using high-spin (S = 2) oxoiron(IV) species with four unpaired electrons on the iron center. However, other reagents with higher spin states and more unpaired electrons on the metal are not as reactive. Still other reagents carry out these transformations using lower spin states with fewer unpaired electrons on the metal. The TS structures for these reactions exhibit structural selectivity depending on the reactive spin states. The barriers and thermodynamic driving forces of the reactions also depend on the spin state. H-Abstraction is preferred over the thermodynamically more favorable concerted insertion into C-H bonds. Currently, there is no unified theoretical framework that explains the totality of these fascinating trends. This Account aims to unify this rich chemistry and understand the role of unpaired electrons on chemical reactivity. We show that during an oxidative step the d-orbital block of the transition metal is enriched by one electron through proton-coupled electron transfer (PCET). That single electron elicits variable exchange interactions on the metal, which in turn depend critically on the number of unpaired electrons on the metal center. Thus, we introduce the exchange-enhanced reactivity (EER) principle, which predicts the preferred spin state during oxidation reactions, the dependence of the barrier on the number of unpaired electrons in the TS, and the dependence of the deformation energy of the reactants on the spin state. We complement EER with orbital-selection rules, which predict the structure of the preferred TS and provide a handy theory of bioinorganic oxidative reactions. These rules show how EER provides a Hund's Rule for chemical reactivity: EER controls the reactivity landscape for a great variety of transition-metal complexes and substrates. Among many reactivity patterns explained, EER rationalizes the abundance of high-spin oxoiron(IV) complexes in enzymes that carry out bond activation of the strongest bonds. The concepts used in this Account might also be applicable in other areas such as in f-block chemistry and excited-state reactivity of 4d and 5d OMCs.

Correlating nuclear frequencies by two-dimensional ELDOR-detected NMR spectroscopy.

PubMed

Kaminker, Ilia; Wilson, Tiffany D; Savelieff, Masha G; Hovav, Yonatan; Zimmermann, Herbert; Lu, Yi; Goldfarb, Daniella

2014-03-01

ELDOR (Electron Double Resonance)-detected NMR (EDNMR) is a pulse EPR experiment that is used to measure the transition frequencies of nuclear spins coupled to electron spins. These frequencies are further used to determine hyperfine and quadrupolar couplings, which are signatures of the electronic and spatial structures of paramagnetic centers. In recent years, EDNMR has been shown to be particularly useful at high fields/high frequencies, such as W-band (∼95 GHz, ∼3.5 T), for low γ quadrupolar nuclei. Although at high fields the nuclear Larmor frequencies are usually well resolved, the limited resolution of EDNMR still remains a major concern. In this work we introduce a two dimensional, triple resonance, correlation experiment based on the EDNMR pulse sequence, which we term 2D-EDNMR. This experiment allows circumventing the resolution limitation by spreading the signals in two dimensions and the observed correlations help in the assignment of the signals. First we demonstrate the utility of the 2D-EDNMR experiment on a nitroxide spin label, where we observe correlations between (14)N nuclear frequencies. Negative cross-peaks appear between lines belonging to different MS electron spin manifolds. We resolved two independent correlation patterns for nuclear frequencies arising from the EPR transitions corresponding to the (14)N mI=0 and mI=-1 nuclear spin states, which severely overlap in the one dimensional EDNMR spectrum. The observed correlations could be accounted for by considering changes in the populations of energy levels that S=1/2, I=1 spin systems undergo during the pulse sequence. In addition to these negative cross-peaks, positive cross-peaks appear as well. We present a theoretical model based on the Liouville equation and use it to calculate the time evolution of populations of the various energy levels during the 2D-EDNMR experiment and generated simulated 2D-EDMR spectra. These calculations show that the positive cross-peaks appear due to off resonance effects and/or nuclear relaxation effects. These results suggest that the 2D-EDNMR experiment can be also useful for relaxation pathway studies. Finally we present preliminary results demonstrating that 2D-EDNMR can resolve overlapping (33)S and (14)N signals of type 1 Cu(II) center in (33)S enriched Azurin. Copyright © 2014 Elsevier Inc. All rights reserved.

The ground state infrared spectrum of the MnH radical ( 7Σ) from diode laser spectroscopy

NASA Astrophysics Data System (ADS)

Urban, Rolf-Dieter; Jones, Harold

1989-11-01

The infrared spectrum of the manganese hydride radical ( 55MnH) in its ground electronic state ( 7Σ) has been observed using a diode laser spectrometer. The wavenumbers of twelve transitions of the v=1→0 band, five of the v=2→1 band and seven of the v=3→2 band have been measured with a nominal accuracy of ±0.001 cm -1. Coupling between the electronic spin ( S=3) and the overall molecular rotation causes each ro-vibrational transition with N>3 to be split (γ splitting) into seven components each separated by a few hundredths of a wavenumber. In most cases the complete structure was resolved. Correction terms arising from spin-spin coupling had to be included in the analysis. This work has produced the most accurate set of ground-state parameters available for MnH.

Hierarchy of Modes in an Interacting One-Dimensional System

NASA Astrophysics Data System (ADS)

Tsyplyatyev, O.; Schofield, A. J.; Jin, Y.; Moreno, M.; Tan, W. K.; Ford, C. J. B.; Griffiths, J. P.; Farrer, I.; Jones, G. A. C.; Ritchie, D. A.

2015-05-01

Studying interacting fermions in one dimension at high energy, we find a hierarchy in the spectral weights of the excitations theoretically, and we observe evidence for second-level excitations experimentally. Diagonalizing a model of fermions (without spin), we show that levels of the hierarchy are separated by powers of R2/L2, where R is a length scale related to interactions and L is the system length. The first-level (strongest) excitations form a mode with parabolic dispersion, like that of a renormalized single particle. The second-level excitations produce a singular power-law line shape to the first-level mode and multiple power laws at the spectral edge. We measure momentum-resolved tunneling of electrons (fermions with spin) from or to a wire formed within a GaAs heterostructure, which shows parabolic dispersion of the first-level mode and well-resolved spin-charge separation at low energy with appreciable interaction strength. We find structure resembling the second-level excitations, which dies away quite rapidly at high momentum.

Observation of a hierarchy of modes in an interacting one-dimensional system

NASA Astrophysics Data System (ADS)

Ford, Christopher; Moreno, Maria; Jin, Yiqing; Tan, Wooi Kiat; Griffiths, Jon; Farrer, Ian; Jones, Geb; Anthore, Anne; Ritchie, David; Tsyplyatyev, Oleksandr; Schofield, Andrew

2015-03-01

Studying interacting fermions in 1D at high energy, we find a hierarchy in the spectral weights of the excitations theoretically and we observe evidence for second-level excitations experimentally. Diagonalising a model of fermions (without spin), we show that levels of the hierarchy are separated by powers of 2 /L2 , where  is a length-scale related to interactions and L is the system length. The first-level (strongest) excitations form a mode with parabolic dispersion, like that of a renormalised single particle. The second-level excitations produce a singular power-law line shape to the first-level mode and multiple power-laws at the spectral edge. We measure momentum-resolved tunneling of electrons (fermions with spin) from/to a wire formed within a GaAs heterostructure, which shows parabolic dispersion of the first-level mode and well-resolved spin-charge separation at low energy with appreciable interaction strength. We find structure resembling the second-level excitations, which dies away quite rapidly at high momentum.

Theoretical Modeling of Various Spectroscopies for Cuprates and Topological Insulators

NASA Astrophysics Data System (ADS)

Basak, Susmita

Spectroscopies resolved highly in momentum, energy and/or spatial dimensions are playing an important role in unraveling key properties of wide classes of novel materials. However, spectroscopies do not usually provide a direct map of the underlying electronic spectrum, but act as a complex 'filter' to produce a 'mapping' of the underlying energy levels, Fermi surfaces (FSs) and excitation spectra. The connection between the electronic spectrum and the measured spectra is described as a generalized 'matrix element effect'. The nature of the matrix element involved differs greatly between different spectroscopies. For example, in angle-resolved photoemission (ARPES) an incoming photon knocks out an electron from the sample and the energy and momentum of the photoemitted electron is measured. This is quite different from what happens in K-edge resonant inelastic X-ray scattering (RIXS), where an X-ray photon is scattered after inducing electronic transitions near the Fermi energy through an indirect second order process, or in Compton scattering where the incident X-ray photon is scattered inelastically from an electron transferring energy and momentum to the scattering electron. For any given spectroscopy, the matrix element is, in general, a complex function of the phase space of the experiment, e.g. energy/polarization of the incoming photon and the energy/momentum/spin of the photoemitted electron in the case of ARPES. The matrix element can enhance or suppress signals from specific states, or merge signals of groups of states, making a good understanding of the matrix element effects important for not only a robust interpretation of the spectra, but also for ascertaining optimal regions of the experimental phase space for zooming in on states of the greatest interest. In this thesis I discuss a comprehensive scheme for modeling various highly resolved spectroscopies of the cuprates and topological insulators (TIs) where effects of matrix element, crystal structure, strong electron correlations (for cuprates) and spin-orbit coupling (for TIs) are included realistically in material-specific detail. Turning to the cuprates, in order to obtain a realistic description of various spectroscopies, one must include not only the effects of the matrix elements and the complexity of the crystal structure, but also of strong electronic correlations beyond the local density approximation (LDA)-based conventional picture, so that the physics of kinks, pseudogaps and superconductivity can be taken into account properly. In this connection, a self-consistent, intermediate coupling scheme informed by material-specific, first-principles band structures has been developed, where electron correlation effects beyond the LDA are incorporated via appropriate self-energy corrections to the electron and hole one-particle Green's functions. Here the antiferromagnetic (AFM) order is used as the simplest model of a competing order. A number of salient features of the resulting electronic spectrum and its energy, momentum and doping dependencies are in accord with experimental observations in electron as well as hole doped cuprates. This scheme thus provides a reasonable basis for undertaking a comprehensive, beyond-LDA level of modeling of various spectroscopies. The specific topics considered here are: (i) Origin of high-energy kink or the waterfall effect found in ARPES; (ii) Identification of the three energy scales observed in RIXS spectra as the pseudogap, charge transfer gap, and Mott gap; (iii) Evolution of the electron momentum densities with holedoping as seen in Compton scattering experiments. For three dimensional topological insulators, the ARPES and scanning tunneling microscopy (STM) spectra has been analyzed using a tight-binding model as well as a k · p model. The spin-orbit coupling, which is essential to produce the characteristic features of the surface states of a TI, is included realistically in the above models. In our generalized k · p model Dresselhaus spin-orbit coupling term extends up to fifth order to reproduce the correct spin-polarization of the surface electrons. These model calculations explain a number of important features associated with the energy and spins of the surface electrons of the first and second generations of TIs. The specific issues addressed in this article are: (i) Non-orthogonality between spin and momentum of the surface electrons; (ii) Electron dynamics at the TI-metal interface; (iii) Origin of the broken time-reversal symmetry observed in the Fourier transform scanning tunneling spectroscopy.

Growth and Electronic Structure of Heusler Compounds for Use in Electron Spin Based Devices

NASA Astrophysics Data System (ADS)

Patel, Sahil Jaykumar

Spintronic devices, where information is carried by the quantum spin state of the electron instead of purely its charge, have gained considerable interest for their use in future computing technologies. For optimal performance, a pure spin current, where all electrons have aligned spins, must be generated and transmitted across many interfaces and through many types of materials. While conventional spin sources have historically been elemental ferromagnets, like Fe or Co, these materials pro duce only partially spin polarized currents. To increase the spin polarization of the current, materials like half-metallic ferromagnets, where there is a gap in the minority spin density of states around the Fermi level, or topological insulators, where the current transport is dominated by spin-locked surface states, show promise. A class of materials called Heusler compounds, with electronic structures that range from normal metals, to half metallic ferromagnets, semiconductors, superconductors and even topological insulators, interfaces well with existing device technologies, and through the use of molecular beam epitaxy (MBE) high quality heterostructures and films can be grown. This dissertation examines the electronic structure of surfaces and interfaces of both topological insulator (PtLuSb-- and PtLuBi--) and half-metallic ferromagnet (Co2MnSi-- and Co2FeSi--) III-V semiconductor heterostructures. PtLuSb and PtLuBi growth by MBE was demonstrated on Alx In1--xSb (001) ternaries. PtLuSb (001) surfaces were observed to reconstruct with either (1x3) or c(2x2) unit cells depending on Sb overpressure and substrate temperature. viii The electronic structure of these films was studied by scanning tunneling microscopy/spectroscopy (STM/STS) and photoemission spectroscopy. STS measurements as well as angle resolved photoemission spectropscopy (ARPES) suggest that PtLuSb has a zero-gap or semimetallic band structure. Additionally, the observation of linearly dispersing surface states, with an approximate crossing point 240meV above the Fermi level, suggests that PtLuSb (001) films are topologically non-trivial. PtLuBi films also display a Fermi level position approximately 500meV below the valence band maximum. Co2MnSi and Co2FeSi were also grown by MBE on GaAs (001) for use as spin injectors into GaAs lateral spin valve devices. By the growth of the quaternary alloy Co2FexMn1-- xSi and varying x, electron doping of the full Heusler compound was demonstrated by observation of a crossover from a majority spin polarization of Co2MnSi to a minority spin polarization in Co2FeSi. Co2MnSi films were studied as a function of the nucleation sequence, using either Co-- or MnSi-- initiated films on c(4x4) GaAs. Studies using x-ray photoemission spectroscopy (XPS), STM/STS, and transmission electron microscopy (TEM) suggest that the bulk of the Co2MnSi films and the interfacial structure between Co 2MnSi and GaAs is not modified by the nucleation sequence, but a change in spin transport characteristics suggests a modification of semiconductor band structure at the Co2MnSi/GaAs interface due to diffusion of Mn leading to compensation of the Schottky barrier contact. Diffusion of Mn into the GaAs was confirmed by secondary ion mass spectrometry (SIMS) measurements. The proposed mechanism for the modified spin transport characteristics for MnSi initiated films is that additional diffusion of Mn into the GaAs, widens the Schottky barrier contact region. These studies suggest that the ideal initiation sequence for Co2MnSi/GaAs (001) lateral spin valve devices is achieved by deposition of Co first.

Reduced interface spin polarization by antiferromagnetically coupled Mn segregated to the C o2MnSi /GaAs (001) interface

NASA Astrophysics Data System (ADS)

Rath, Ashutosh; Sivakumar, Chockalingam; Sun, C.; Patel, Sahil J.; Jeong, Jong Seok; Feng, J.; Stecklein, G.; Crowell, Paul A.; Palmstrøm, Chris J.; Butler, William H.; Voyles, Paul M.

2018-01-01

We have investigated the interfacial structure and its correlation with the calculated spin polarization in C o2MnSi /GaAs(001) lateral spin valves. C o2MnSi (CMS) films were grown on As-terminated c(4 ×4 ) GaAs(100) by molecular beam epitaxy using different first atomic layers: MnSi, Co, and Mn. Atomically resolved Z -contrast scanning transmission electron microscopy (STEM) imaging and electron energy loss spectroscopy (EELS) were used to develop atomic structural models of the CMS/GaAs interfaces that were used as inputs for first-principles calculations to understand the magnetic and electronic properties of the interface. First-principles structures were relaxed and then validated by comparing experimental and simulated high-resolution STEM images. STEM-EELS results show that all three films have similar six atomic layer thick, Mn- and As-rich multilayer interfaces. However, the Co-initiated interface contains a M n2As -like layer, which is antiferromagnetic, and which is not present in the other two interfaces. Density functional theory calculations show a higher degree of interface spin polarization in the Mn- and MnSi-initiated cases, compared to the Co-initiated case, although none of the interfaces are half-metallic. The loss of half-metallicity is attributed, at least in part, to the segregation of Mn at the interface, which leads to the formation of interface states. The implications for the performance of lateral spin valves based on these interfaces are discussed briefly.

Giant spin-splitting and gap renormalization driven by trions in single-layer WS2/h-BN heterostructures

NASA Astrophysics Data System (ADS)

Katoch, Jyoti; Ulstrup, Søren; Koch, Roland J.; Moser, Simon; McCreary, Kathleen M.; Singh, Simranjeet; Xu, Jinsong; Jonker, Berend T.; Kawakami, Roland K.; Bostwick, Aaron; Rotenberg, Eli; Jozwiak, Chris

2018-04-01

In two-dimensional (2D) semiconducting transition metal dichalcogenides (TMDs), new electronic phenomena such as tunable bandgaps1-3 and strongly bound excitons and trions emerge from strong many-body effects4-6, beyond the spin and valley degrees of freedom induced by spin-orbit coupling and by lattice symmetry7. Combining single-layer TMDs with other 2D materials in van der Waals heterostructures offers an intriguing means of controlling the electronic properties through these many-body effects, by means of engineered interlayer interactions8-10. Here, we use micro-focused angle-resolved photoemission spectroscopy (microARPES) and in situ surface doping to manipulate the electronic structure of single-layer WS2 on hexagonal boron nitride (WS2/h-BN). Upon electron doping, we observe an unexpected giant renormalization of the spin-orbit splitting of the single-layer WS2 valence band, from 430 meV to 660 meV, together with a bandgap reduction of at least 325 meV, attributed to the formation of trionic quasiparticles. These findings suggest that the electronic, spintronic and excitonic properties are widely tunable in 2D TMD/h-BN heterostructures, as these are intimately linked to the quasiparticle dynamics of the materials11-13.

Ab initio study on rare-earth iron-pnictides RFeAsO (R = Pr, Nd, Sm, Gd) in low-temperature Cmma phase

NASA Astrophysics Data System (ADS)

Eryigit, Resul; Gurel, Tanju; Erturk, Esra; Lukoyanov, A. V.; Akcay, Guven; Anisimov, V. I.

2014-03-01

We present density functional theory calculations on iron-based pnictides RFeAsO (R = Pr, Nd, Sm, Gd). The calculations have been carried out using plane-waves and projector augmented wave (PAW) pseudopotential approach. Structural, magnetic and electronic properties are studied within generalized gradient approximation (GGA) and also within GGA+U in order to investigate the influence of electron correlation effects. Low-temperature Cmma structure is fully optimized by GGA considering both non-magnetic and magnetic cells. We have found that spin-polarized structure improves the agreement with experiments on equilibrium lattice parameters, particularly c lattice parameter and Fe-As bond-lengths. Electronic band structure, total density of states, and spin-dependent orbital-resolved density of states are also analyzed in the frameworks of GGA and GGA+U and discussed. For all materials, by including on-site Coulomb correction, rare earth 4f states move away from the Fermi level and the Fermi level features of the systems are found to be mostly defined by the 3d electron-electron correlations in Fe. This work was supported by the Scientific and Technological Research Council of Turkey (TUBITAK Project No. TBAG-111T796) and the Russian Foundation for Basic Research (Project No. 12-02-91371-CT_a).

Theoretical study of charge and spin-resolved quantum transport in III-V semiconductor nanostructures

NASA Astrophysics Data System (ADS)

Botha, Andre Erasmus

2003-07-01

This thesis is a theoretical investigation into the spin-resolved transport properties of III-V semiconductor quantum wells. Based on a modified 8 x 8 k · p matrix Hamiltonian, a theory is developed to study the recombination rate in type-II semi metallic quantum wells. The non-parabolicity of the energy band structure and its anisotropy is included via the interband matrix elements and the addition of an anisotropic crystal field potential (parameterized by delta). The effects of externally applied electric and magnetic fields are incorporated into the theory. The electric field is incorporated using a WKB-type approximation. In order to study the anisotropy, the magnetic field is incorporated so that it can be applied at an arbitrary angle theta, with respect to the crystallographic direction c[001]. The case of oblique tunneling (k|| ≠ 0), is also considered. Several interesting results, from calculations of the transmission coefficient, recombination rate, and electron-spin polarization, are presented and discussed for both n-type and p-type single and double quantum wells made from clean InAs and GaSb. For example, in the case of a 150 A wide GaSb/InAs/GaSb quantum well, with B = 4 T, and theta = pi/8, the two maxima in the electron-spin polarization, from the ground and first excited resonant states, are found to be approximately 75%, and 35%, respectively. As theta is varied, a maximum polarization is achieved for a given magnetic field, and this maximum depends on the value of the anisotropy parameter, delta. By using a more sophisticated 14 x 14 band k · p formalism, which explicitly takes into account the coupling between higher bands ( Gc15-Gu 15,Gc1-G u15 , and Gc1-Gc15 ), a theory is developed for the total zero-field spin-splitting and resulting electron-spin polarization in symmetric and asymmetric type-II quantum wells. This theory includes the non-parabolicity, non sphericity, and anisotropy of the energy band structure. The anisotropy in the band structure is introduced via the addition of an anisotropic crystal potential. In the case of an asymmetric GaSb/InAs/GaSb quantum well, it is predicted that the two contributions to the total spin-splitting will be roughly of equal importance. It is also shown that the polarization maxima and minima, for a given resonance state, may not be equal in magnitude. If the resonant state lies close to the forbidden energy gap, the transmission peaks for spin-up and spin-down are skewed. This feature may have potential applications in the design of spintronic filtering and switching devices, in which it is desirable to filter unpolarized electrons (with respect to energy and spin) in order to produce highly polarized, adjustable low-energy beams.

Strain Coupling of a Nitrogen-Vacancy Center Spin to a Diamond Mechanical Oscillator

NASA Astrophysics Data System (ADS)

Teissier, J.; Barfuss, A.; Appel, P.; Neu, E.; Maletinsky, P.

2014-07-01

We report on single electronic spins coupled to the motion of mechanical resonators by a novel mechanism based on crystal strain. Our device consists of single-crystal diamond cantilevers with embedded nitrogen-vacancy center spins. Using optically detected electron spin resonance, we determine the unknown spin-strain coupling constants and demonstrate that our system resides well within the resolved sideband regime. We realize coupling strengths exceeding 10 MHz under mechanical driving and show that our system has the potential to reach strong coupling. Our novel hybrid system forms a resource for future experiments on spin-based cantilever cooling and coherent spin-oscillator coupling.

Spin-resolved electron waiting times in a quantum-dot spin valve

NASA Astrophysics Data System (ADS)

Tang, Gaomin; Xu, Fuming; Mi, Shuo; Wang, Jian

2018-04-01

We study the electronic waiting-time distributions (WTDs) in a noninteracting quantum-dot spin valve by varying spin polarization and the noncollinear angle between the magnetizations of the leads using the scattering matrix approach. Since the quantum-dot spin valve involves two channels (spin up and down) in both the incoming and outgoing channels, we study three different kinds of WTDs, which are two-channel WTD, spin-resolved single-channel WTD, and cross-channel WTD. We analyze the behaviors of WTDs in short times, correlated with the current behaviors for different spin polarizations and noncollinear angles. Cross-channel WTD reflects the correlation between two spin channels and can be used to characterize the spin-transfer torque process. We study the influence of the earlier detection on the subsequent detection from the perspective of cross-channel WTD, and define the influence degree quantity as the cumulative absolute difference between cross-channel WTDs and first-passage time distributions to quantitatively characterize the spin-flip process. We observe that influence degree versus spin-transfer torque for different noncollinear angles as well as different polarizations collapse into a single curve showing universal behaviors. This demonstrates that cross-channel WTDs can be a pathway to characterize spin correlation in spintronics system.

Direct evidence of hidden local spin polarization in a centrosymmetric superconductor LaO0.55 F0.45BiS2.

PubMed

Wu, Shi-Long; Sumida, Kazuki; Miyamoto, Koji; Taguchi, Kazuaki; Yoshikawa, Tomoki; Kimura, Akio; Ueda, Yoshifumi; Arita, Masashi; Nagao, Masanori; Watauchi, Satoshi; Tanaka, Isao; Okuda, Taichi

2017-12-04

Conventional Rashba spin polarization is caused by the combination of strong spin-orbit interaction and spatial inversion asymmetry. However, Rashba-Dresselhaus-type spin-split states are predicted in the centrosymmetric LaOBiS 2 system by recent theory, which stem from the local inversion asymmetry of active BiS 2 layer. By performing high-resolution spin- and angle-resolved photoemission spectroscopy, we have investigated the electronic band structure and spin texture of superconductor LaO 0.55 F 0.45 BiS 2 . Here we present direct spectroscopic evidence for the local spin polarization of both the valence band and the conduction band. In particular, the coexistence of Rashba-like and Dresselhaus-like spin textures has been observed in the conduction band. The finding is of key importance for fabrication of proposed dual-gated spin-field effect transistor. Moreover, the spin-split band leads to a spin-momentum locking Fermi surface from which superconductivity emerges. Our demonstration not only expands the scope of spintronic materials but also enhances the understanding of spin-orbit interaction-related superconductivity.

Observation of the spin-polarized surface state in a noncentrosymmetric superconductor BiPd

DOE Office of Scientific and Technical Information (OSTI.GOV)

Neupane, Madhab; Alidoust, Nasser; Hosen, M. Mofazzel

Recently, noncentrosymmetric superconductor BiPd has attracted considerable research interest due to the possibility of hosting topological superconductivity. Here in this paper we report a systematic high-resolution angle-resolved photoemission spectroscopy (ARPES) and spin-resolved ARPES study of the normal state electronic and spin properties of BiPd. Our experimental results show the presence of a surface state at higher-binding energy with the location of Dirac point at around 700 meV below the Fermi level. The detailed photon energy, temperature-dependent and spin-resolved ARPES measurements complemented by our first-principles calculations demonstrate the existence of the spin-polarized surface states at high-binding energy. The absence of suchmore » spin-polarized surface states near the Fermi level negates the possibility of a topological superconducting behaviour on the surface. Our direct experimental observation of spin-polarized surface states in BiPd provides critical information that will guide the future search for topological superconductivity in noncentrosymmetric materials.« less

Observation of the spin-polarized surface state in a noncentrosymmetric superconductor BiPd

DOE PAGES

Neupane, Madhab; Alidoust, Nasser; Hosen, M. Mofazzel; ...

2016-11-07

Recently, noncentrosymmetric superconductor BiPd has attracted considerable research interest due to the possibility of hosting topological superconductivity. Here in this paper we report a systematic high-resolution angle-resolved photoemission spectroscopy (ARPES) and spin-resolved ARPES study of the normal state electronic and spin properties of BiPd. Our experimental results show the presence of a surface state at higher-binding energy with the location of Dirac point at around 700 meV below the Fermi level. The detailed photon energy, temperature-dependent and spin-resolved ARPES measurements complemented by our first-principles calculations demonstrate the existence of the spin-polarized surface states at high-binding energy. The absence of suchmore » spin-polarized surface states near the Fermi level negates the possibility of a topological superconducting behaviour on the surface. Our direct experimental observation of spin-polarized surface states in BiPd provides critical information that will guide the future search for topological superconductivity in noncentrosymmetric materials.« less

Widespread spin polarization effects in photoemission from topological insulators

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jozwiak, C.; Chen, Y. L.; Fedorov, A. V.

2011-06-22

High-resolution spin- and angle-resolved photoemission spectroscopy (spin-ARPES) was performed on the three-dimensional topological insulator Bi{sub 2}Se{sub 3} using a recently developed high-efficiency spectrometer. The topological surface state's helical spin structure is observed, in agreement with theoretical prediction. Spin textures of both chiralities, at energies above and below the Dirac point, are observed, and the spin structure is found to persist at room temperature. The measurements reveal additional unexpected spin polarization effects, which also originate from the spin-orbit interaction, but are well differentiated from topological physics by contrasting momentum and photon energy and polarization dependencies. These observations demonstrate significant deviations ofmore » photoelectron and quasiparticle spin polarizations. Our findings illustrate the inherent complexity of spin-resolved ARPES and demonstrate key considerations for interpreting experimental results.« less

Highly Efficient Room Temperature Spin Injection Using Spin Filtering in MgO

NASA Astrophysics Data System (ADS)

Jiang, Xin

2007-03-01

Efficient electrical spin injection into GaAs/AlGaAs quantum well structures was demonstrated using CoFe/MgO tunnel spin injectors at room temperature. The spin polarization of the injected electron current was inferred from the circular polarization of electroluminescence from the quantum well. Polarization values as high as 57% at 100 K and 47% at 290 K were obtained in a perpendicular magnetic field of 5 Tesla. The interface between the tunnel spin injector and the GaAs interface remained stable even after thermal annealing at 400 ^oC. The temperature dependence of the electron-hole recombination time and the electron spin relaxation time in the quantum well was measured using time-resolved optical techniques. By taking into account of these properties of the quantum well, the intrinsic spin injection efficiency can be deduced. We conclude that the efficiency of spin injection from a CoFe/MgO spin injector is nearly independent of temperature and, moreover, is highly efficient with an efficiency of ˜ 70% for the temperature range studied (10 K to room temperature). Tunnel spin injectors are thus highly promising components of future semiconductor spintronic devices. Collaborators: Roger Wang^1, 3, Gian Salis^2, Robert Shelby^1, Roger Macfarlane^1, Seth Bank^3, Glenn Solomon^3, James Harris^3, Stuart S. P. Parkin^1 ^1 IBM Almaden Research Center, San Jose, CA 95120 ^2 IBM Zurich Research Laboratory, S"aumerstrasse 4, 8803 R"uschlikon, Switzerland ^3 Solid States and Photonics Laboratory, Stanford University, Stanford, CA 94305

Study of MoNbO(y) (y = 2-5) anion and neutral clusters using photoelectron spectroscopy and density functional theory calculations: impact of spin contamination on single point calculations.

PubMed

Waller, Sarah E; Mann, Jennifer E; Rothgeb, David W; Jarrold, Caroline C

2012-10-04

Results of a study combining anion photoelectron spectroscopy and density functional theory calculations on the heteronuclear MoNbO(y)(-) (y = 2-5) transition metal suboxide cluster series are reported and analyzed. The photoelectron spectra, which exhibit broad electronic bands with partially resolved vibrational structure, were compared to spectral simulations generated from calculated spectroscopic parameters for all computationally determined energetically competitive structures. Although computational results on the less oxidized clusters could not be satisfactorily reconciled with experimental spectra, possibly because of heavy spin contamination found in a large portion of the computational results, the results suggest that (1) neutral cluster electron affinity is a strong indicator of whether O-atoms are bound in M-O-M bridge positions or M═O terminal positions, (2) MoNbO(y) anions and neutrals have structures that can be described as intermediate with respect to the unary (homonuclear) Mo(2)O(y) and Nb(2)O(y) clusters, and (3) structures in which O-atoms preferentially bind to the Nb center are slightly more stable than alternative structures. Several challenges associated with the calculations are considered, including spin contamination, which appears to cause spurious single point calculations used to determine vertical detachment energies.

Evolution of the Valley Position in Bulk Transition-Metal Chalcogenides and Their Monolayer Limit.

PubMed

Yuan, Hongtao; Liu, Zhongkai; Xu, Gang; Zhou, Bo; Wu, Sanfeng; Dumcenco, Dumitru; Yan, Kai; Zhang, Yi; Mo, Sung-Kwan; Dudin, Pavel; Kandyba, Victor; Yablonskikh, Mikhail; Barinov, Alexei; Shen, Zhixun; Zhang, Shoucheng; Huang, Yingsheng; Xu, Xiaodong; Hussain, Zahid; Hwang, Harold Y; Cui, Yi; Chen, Yulin

2016-08-10

Layered transition metal chalcogenides with large spin orbit coupling have recently sparked much interest due to their potential applications for electronic, optoelectronic, spintronics, and valleytronics. However, most current understanding of the electronic structure near band valleys in momentum space is based on either theoretical investigations or optical measurements, leaving the detailed band structure elusive. For example, the exact position of the conduction band valley of bulk MoS2 remains controversial. Here, using angle-resolved photoemission spectroscopy with submicron spatial resolution (micro-ARPES), we systematically imaged the conduction/valence band structure evolution across representative chalcogenides MoS2, WS2, and WSe2, as well as the thickness dependent electronic structure from bulk to the monolayer limit. These results establish a solid basis to understand the underlying valley physics of these materials, and also provide a link between chalcogenide electronic band structure and their physical properties for potential valleytronics applications.

Logical spin-filtering in a triangular network of quantum nanorings with a Rashba spin-orbit interaction

NASA Astrophysics Data System (ADS)

Dehghan, E.; Sanavi Khoshnoud, D.; Naeimi, A. S.

2018-01-01

The spin-resolved electron transport through a triangular network of quantum nanorings is studied in the presence of Rashba spin-orbit interaction (RSOI) and a magnetic flux using quantum waveguide theory. This study illustrates that, by tuning Rashba constant, magnetic flux and incoming electron energy, the triangular network of quantum rings can act as a perfect logical spin-filtering with high efficiency. By changing in the energy of incoming electron, at a proper value of the Rashba constant and magnetic flux, a reverse in the direction of spin can take place in the triangular network of quantum nanorings. Furthermore, the triangular network of quantum nanorings can be designed as a device and shows several simultaneous spintronic properties such as spin-splitter and spin-inverter. This spin-splitting is dependent on the energy of the incoming electron. Additionally, different polarizations can be achieved in the two outgoing leads from an originally incoming spin state that simulates a Stern-Gerlach apparatus.

Electrical controllable spin pump based on a zigzag silicene nanoribbon junction.

PubMed

Zhang, Lin; Tong, Peiqing

2017-12-13

We propose a possible electrical controllable spin pump based on a zigzag silicene nanoribbon ferromagnetic junction by applying two time-dependent perpendicular electric fields. By using the Keldysh Green's function method, we derive the analytic expression of the spin-resolved current at the adiabatic approximation and demonstrate that two asymmetric spin up and spin down currents can be pumped out in the device without an external bias. The pumped currents mainly come from the interplay between the photon-assisted spin pump effect and the electrically-modulated energy band structure of the tunneling junction. The spin valve phenomena are not only related to the energy gap opened by two perpendicular staggered potentials, but also dependent on the system parameters such as the pumping frequency, the pumping phase difference, the spin-orbit coupling and the Fermi level, which can be tuned by the electrical methods. The proposed device can also be used to produce a pure spin current and a 100% polarized spin current through the photon-assisted pumping process. Our investigations may provide an electrical manipulation of spin-polarized electrons in graphene-like pumping devices.

Quantum spin Hall state in monolayer 1T '-WTe 2

DOE PAGES

Tang, Shujie; Zhang, Chaofan; Wong, Dillon; ...

2017-06-26

A quantum spin Hall (QSH) insulator is a novel two-dimensional quantum state of matter that features quantized Hall conductance in the absence of a magnetic field, resulting from topologically protected dissipationless edge states that bridge the energy gap opened by band inversion and strong spin–orbit coupling. By investigating the electronic structure of epitaxially grown monolayer 1T '-WTe 2 using angle-resolved photoemission (ARPES) and first-principles calculations, we observe clear signatures of topological band inversion and bandgap opening, which are the hallmarks of a QSH state. Scanning tunnelling microscopy measurements further confirm the correct crystal structure and the existence of a bulkmore » bandgap, and provide evidence for a modified electronic structure near the edge that is consistent with the expectations for a QSH insulator. Our results establish monolayer 1T '-WTe 2 as a new class of QSH insulator with large band gap in a robust two-dimensional materials family of transition metal dichalcogenides (TMDCs).« less

Quantum spin Hall state in monolayer 1T '-WTe 2

DOE PAGES

Tang, Shujie; Zhang, Chaofan; Wong, Dillon; ...

2017-06-26

A quantum spin Hall (QSH) insulator is a novel two-dimensional quantum state of matter that features quantized Hall conductance in the absence of a magnetic field, resulting from topologically protected dissipationless edge states that bridge the energy gap opened by band inversion and strong spin–orbit coupling. By investigating the electronic structure of epitaxially grown monolayer 1T '-WTe 2 using angle-resolved photoemission (ARPES) and first-principles calculations, we observe clear signatures of topological band inversion and bandgap opening, which are the hallmarks of a QSH state. Scanning tunnelling microscopy measurements further confirm the correct crystal structure and the existence of a bulkmore » bandgap, and provide evidence for a modified electronic structure near the edge that is consistent with the expectations for a QSH insulator. Finally, our results establish monolayer 1T '-WTe 2 as a new class of QSH insulator with large band gap in a robust two-dimensional materials family of transition metal dichalcogenides (TMDCs).« less

Topological surface state of α -Sn on InSb(001) as studied by photoemission

NASA Astrophysics Data System (ADS)

Scholz, M. R.; Rogalev, V. A.; Dudy, L.; Reis, F.; Adler, F.; Aulbach, J.; Collins-McIntyre, L. J.; Duffy, L. B.; Yang, H. F.; Chen, Y. L.; Hesjedal, T.; Liu, Z. K.; Hoesch, M.; Muff, S.; Dil, J. H.; Schäfer, J.; Claessen, R.

2018-02-01

We report on the electronic structure of the elemental topological semimetal α -Sn on InSb(001). High-resolution angle-resolved photoemission data allow us to observe the topological surface state (TSS) that is degenerate with the bulk band structure and show that the former is unaffected by different surface reconstructions. An unintentional p -type doping of the as-grown films was compensated by deposition of potassium or tellurium after the growth, thereby shifting the Dirac point of the surface state below the Fermi level. We show that, while having the potential to break time-reversal symmetry, iron impurities with a coverage of up to 0.25 monolayers do not have any further impact on the surface state beyond that of K or Te. Furthermore, we have measured the spin-momentum locking of electrons from the TSS by means of spin-resolved photoemission. Our results show that the spin vector lies fully in-plane, but it also has a finite radial component. Finally, we analyze the decay of photoholes introduced in the photoemission process, and by this gain insight into the many-body interactions in the system. Surprisingly, we extract quasiparticle lifetimes comparable to other topological materials where the TSS is located within a bulk band gap. We argue that the main decay of photoholes is caused by intraband scattering, while scattering into bulk states is suppressed due to different orbital symmetries of bulk and surface states.

State-Resolved Metal Nanoparticle Dynamics Viewed through the Combined Lenses of Ultrafast and Magneto-optical Spectroscopies.

PubMed

Zhao, Tian; Herbert, Patrick J; Zheng, Hongjun; Knappenberger, Kenneth L

2018-06-19

Electronic carrier dynamics play pivotal roles in the functional properties of nanomaterials. For colloidal metals, the mechanisms and influences of these dynamics are structure dependent. The coherent carrier dynamics of collective plasmon modes for nanoparticles (approximately 2 nm and larger) determine optical amplification factors that are important to applied spectroscopy techniques. In the nanocluster domain (sub-2 nm), carrier coupling to vibrational modes affects photoluminescence yields. The performance of photocatalytic materials featuring both nanoparticles and nanoclusters also depends on the relaxation dynamics of nonequilibrium charge carriers. The challenges for developing comprehensive descriptions of carrier dynamics spanning both domains are multifold. Plasmon coherences are short-lived, persisting for only tens of femtoseconds. Nanoclusters exhibit discrete carrier dynamics that can persist for microseconds in some cases. On this time scale, many state-dependent processes, including vibrational relaxation, charge transfer, and spin conversion, affect carrier dynamics in ways that are nonscalable but, rather, structure specific. Hence, state-resolved spectroscopy methods are needed for understanding carrier dynamics in the nanocluster domain. Based on these considerations, a detailed understanding of structure-dependent carrier dynamics across length scales requires an appropriate combination of spectroscopic methods. Plasmon mode-specific dynamics can be obtained through ultrafast correlated light and electron microscopy (UCLEM), which pairs interferometric nonlinear optical (INLO) with electron imaging methods. INLO yields nanostructure spectral resonance responses, which capture the system's homogeneous line width and coherence dynamics. State-resolved nanocluster dynamics can be obtained by pairing ultrafast with magnetic-optical spectroscopy methods. In particular, variable-temperature variable-field (VTVH) spectroscopies allow quantification of transient, excited states, providing quantification of important parameters such as spin and orbital angular momenta as well as the energy gaps that separate electronic fine structure states. Ultrafast two-dimensional electronic spectroscopy (2DES) can be used to understand how these details influence state-to-state carrier dynamics. In combination, VTVH and 2DES methods can provide chemists with detailed information regarding the structure-dependent and state-specific flow of energy through metal nanoclusters. In this Account, we highlight recent advances toward understanding structure-dependent carrier dynamics for metals spanning the sub-nanometer to tens of nanometers length scale. We demonstrate the use of UCLEM methods for arresting interband scattering effects. For sub-nanometer thiol-protected nanoclusters, we discuss the effectiveness of VTVH for distinguishing state-specific radiative recombination originating from a gold core versus organometallic protecting layers. This state specificity is refined further using femtosecond 2DES and two-color methods to isolate so-called superatom state dynamics and vibrationally mediated spin-conversion and emission processes. Finally, we discuss prospects for merging VTVH and 2DES methods into a single platform.

Direct measurement of discrete valley and orbital quantum numbers in bilayer graphene.

PubMed

Hunt, B M; Li, J I A; Zibrov, A A; Wang, L; Taniguchi, T; Watanabe, K; Hone, J; Dean, C R; Zaletel, M; Ashoori, R C; Young, A F

2017-10-16

The high magnetic field electronic structure of bilayer graphene is enhanced by the spin, valley isospin, and an accidental orbital degeneracy, leading to a complex phase diagram of broken symmetry states. Here, we present a technique for measuring the layer-resolved charge density, from which we directly determine the valley and orbital polarization within the zero energy Landau level. Layer polarization evolves in discrete steps across 32 electric field-tuned phase transitions between states of different valley, spin, and orbital order, including previously unobserved orbitally polarized states stabilized by skew interlayer hopping. We fit our data to a model that captures both single-particle and interaction-induced anisotropies, providing a complete picture of this correlated electron system. The resulting roadmap to symmetry breaking paves the way for deterministic engineering of fractional quantum Hall states, while our layer-resolved technique is readily extendable to other two-dimensional materials where layer polarization maps to the valley or spin quantum numbers.The phase diagram of bilayer graphene at high magnetic fields has been an outstanding question, with orders possibly between multiple internal quantum degrees of freedom. Here, Hunt et al. report the measurement of the valley and orbital order, allowing them to directly reconstruct the phase diagram.

Probing temperature-driven flow lines in a gated two-dimensional electron gas with tunable spin-splitting.

PubMed

Wang, Yi-Ting; Kim, Gil-Ho; Huang, C F; Lo, Shun-Tsung; Chen, Wei-Jen; Nicholls, J T; Lin, Li-Hung; Ritchie, D A; Chang, Y H; Liang, C-T; Dolan, B P

2012-10-10

We study the temperature flow of conductivities in a gated GaAs two-dimensional electron gas (2DEG) containing self-assembled InAs dots and compare the results with recent theoretical predictions. By changing the gate voltage, we are able to tune the 2DEG density and thus vary disorder and spin-splitting. Data for both the spin-resolved and spin-degenerate phase transitions are presented, the former collapsing to the latter with decreasing gate voltage and/or decreasing spin-splitting. The experimental results support a recent theory, based on modular symmetry, which predicts how the critical Hall conductivity varies with spin-splitting.

Time-resolved scanning electron microscopy with polarization analysis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Frömter, Robert, E-mail: rfroemte@physik.uni-hamburg.de; Oepen, Hans Peter; The Hamburg Centre for Ultrafast Imaging, Luruper Chaussee 149, 22761 Hamburg

2016-04-04

We demonstrate the feasibility of investigating periodically driven magnetization dynamics in a scanning electron microscope with polarization analysis based on spin-polarized low-energy electron diffraction. With the present setup, analyzing the time structure of the scattering events, we obtain a temporal resolution of 700 ps, which is demonstrated by means of imaging the field-driven 100 MHz gyration of the vortex in a soft-magnetic FeCoSiB square. Owing to the efficient intrinsic timing scheme, high-quality movies, giving two components of the magnetization simultaneously, can be recorded on the time scale of hours.

Electronic structure of YbB 6 : Is it a topological insulator or not?

DOE PAGES

Kang, Chang -Jong; Denlinger, J. D.; Allen, J. W.; ...

2016-03-17

Here, to finally resolve the controversial issue of whether or not the electronic structure of YbB6 is nontrivially topological, we have made a combined study using angle-resolved photoemission spectroscopy (ARPES) of the nonpolar (110) surface and density functional theory (DFT). The flat-band conditions of the (110) ARPES avoid the strong band bending effects of the polar (001) surface and definitively show that YbB 6 has a topologically trivial B 2p–Yb 5d semiconductor band gap of ~0.3 eV. Accurate determination of the low energy band topology in DFT requires the use of a modified Becke-Johnson exchange potential incorporating spin-orbit coupling andmore » an on-site Yb 4f Coulomb interaction U as large as 7 eV. The DFT result, confirmed by a more precise GW band calculation, is similar to that of a small gap non-Kondo nontopological semiconductor. Additionally, the pressure-dependent electronic structure of YbB 6 is investigated theoretically and found to transform into a p–d overlap semimetal with small Yb mixed valency.« less

Fermiology and Superconductivity of Topological Surface States in PdTe2

NASA Astrophysics Data System (ADS)

Clark, O. J.; Neat, M. J.; Okawa, K.; Bawden, L.; Marković, I.; Mazzola, F.; Feng, J.; Sunko, V.; Riley, J. M.; Meevasana, W.; Fujii, J.; Vobornik, I.; Kim, T. K.; Hoesch, M.; Sasagawa, T.; Wahl, P.; Bahramy, M. S.; King, P. D. C.

2018-04-01

We study the low-energy surface electronic structure of the transition-metal dichalcogenide superconductor PdTe2 by spin- and angle-resolved photoemission, scanning tunneling microscopy, and density-functional theory-based supercell calculations. Comparing PdTe2 with its sister compound PtSe2 , we demonstrate how enhanced interlayer hopping in the Te-based material drives a band inversion within the antibonding p -orbital manifold well above the Fermi level. We show how this mediates spin-polarized topological surface states which form rich multivalley Fermi surfaces with complex spin textures. Scanning tunneling spectroscopy reveals type-II superconductivity at the surface, and moreover shows no evidence for an unconventional component of its superconducting order parameter, despite the presence of topological surface states.

Spatially resolved nuclear spin relaxation, electron spin relaxation and light absorption in swift heavy ion irradiated LiF crystals.

PubMed

Stork, H; Dinse, K-P; Ditter, M; Fujara, F; Masierak, W; Neumann, R; Schuster, B; Schwartz, K; Trautmann, C

2010-05-12

Spatially resolved (19)F and (7)Li spin-lattice relaxation rates are measured for LiF single crystals after irradiation with two kinds of swift heavy ions ((12)C of 133 MeV and (208)Pb of 1.78 GeV incident energy). Like in earlier studies on (130)Xe and (238)U irradiated LiF crystals, we found a strong enhancement of the nuclear spin-lattice relaxation rate within the ion penetration depth and a slight--but still significant--enhancement beyond. By evaluating the nuclear relaxation rate enhancement within the ion range after irradiation with different projectiles, a universal relationship between the spin-lattice relaxation rate and the dose is deduced. The results of accompanying X-band electron paramagnetic resonance relaxation measurements and optical absorption spectroscopy are included in a physical interpretation of this relationship. Also the reason for the enhanced relaxation rate beyond the ion range is further discussed.

Delayed entanglement echo for individual control of a large number of nuclear spins

PubMed Central

Wang, Zhen-Yu; Casanova, Jorge; Plenio, Martin B.

2017-01-01

Methods to selectively detect and manipulate nuclear spins by single electrons of solid-state defects play a central role for quantum information processing and nanoscale nuclear magnetic resonance (NMR). However, with standard techniques, no more than eight nuclear spins have been resolved by a single defect centre. Here we develop a method that improves significantly the ability to detect, address and manipulate nuclear spins unambiguously and individually in a broad frequency band by using a nitrogen-vacancy (NV) centre as model system. On the basis of delayed entanglement control, a technique combining microwave and radio frequency fields, our method allows to selectively perform robust high-fidelity entangling gates between hardly resolved nuclear spins and the NV electron. Long-lived qubit memories can be naturally incorporated to our method for improved performance. The application of our ideas will increase the number of useful register qubits accessible to a defect centre and improve the signal of nanoscale NMR. PMID:28256508

Delayed entanglement echo for individual control of a large number of nuclear spins.

PubMed

Wang, Zhen-Yu; Casanova, Jorge; Plenio, Martin B

2017-03-03

Methods to selectively detect and manipulate nuclear spins by single electrons of solid-state defects play a central role for quantum information processing and nanoscale nuclear magnetic resonance (NMR). However, with standard techniques, no more than eight nuclear spins have been resolved by a single defect centre. Here we develop a method that improves significantly the ability to detect, address and manipulate nuclear spins unambiguously and individually in a broad frequency band by using a nitrogen-vacancy (NV) centre as model system. On the basis of delayed entanglement control, a technique combining microwave and radio frequency fields, our method allows to selectively perform robust high-fidelity entangling gates between hardly resolved nuclear spins and the NV electron. Long-lived qubit memories can be naturally incorporated to our method for improved performance. The application of our ideas will increase the number of useful register qubits accessible to a defect centre and improve the signal of nanoscale NMR.

Spin-resolved correlations in the warm-dense homogeneous electron gas

NASA Astrophysics Data System (ADS)

Arora, Priya; Kumar, Krishan; Moudgil, R. K.

2017-04-01

We have studied spin-resolved correlations in the warm-dense homogeneous electron gas by determining the linear density and spin-density response functions, within the dynamical self-consistent mean-field theory of Singwi et al. The calculated spin-resolved pair-correlation function gσσ'(r) is compared with the recent restricted path-integral Monte Carlo (RPIMC) simulations due to Brown et al. [Phys. Rev. Lett. 110, 146405 (2013)], while interaction energy Eint and exchange-correlation free energy Fxc with the RPIMC and very recent ab initio quantum Monte Carlo (QMC) simulations by Dornheim et al. [Phys. Rev. Lett. 117, 156403 (2016)]. g↑↓(r) is found to be in good agreement with the RPIMC data, while a mismatch is seen in g↑↑(r) at small r where it becomes somewhat negative. As an interesting result, it is deduced that a non-monotonic T-dependence of g(0) is driven primarily by g↑↓(0). Our results of Eint and Fxc exhibit an excellent agreement with the QMC study due to Dornheim et al., which deals with the finite-size correction quite accurately. We observe, however, a visible deviation of Eint from the RPIMC data for high densities ( 8% at rs = 1). Further, we have extended our study to the fully spin-polarized phase. Again, with the exception of high density region, we find a good agreement of Eint with the RPIMC data. This points to the need of settling the problem of finite-size correction in the spin-polarized phase also. Interestingly, we also find that the thermal effects tend to oppose spatial localization as well as spin polarization of electrons. Supplementary material in the form of one zip file available from the Journal web page at http://https://doi.org/10.1140/epjb/e2017-70532-y

Design and commissioning of an aberration-corrected ultrafast spin-polarized low energy electron microscope with multiple electron sources.

PubMed

Wan, Weishi; Yu, Lei; Zhu, Lin; Yang, Xiaodong; Wei, Zheng; Liu, Jefferson Zhe; Feng, Jun; Kunze, Kai; Schaff, Oliver; Tromp, Ruud; Tang, Wen-Xin

2017-03-01

We describe the design and commissioning of a novel aberration-corrected low energy electron microscope (AC-LEEM). A third magnetic prism array (MPA) is added to the standard AC-LEEM with two prism arrays, allowing the incorporation of an ultrafast spin-polarized electron source alongside the standard cold field emission electron source, without degrading spatial resolution. The high degree of symmetries of the AC-LEEM are utilized while we design the electron optics of the ultrafast spin-polarized electron source, so as to minimize the deleterious effect of time broadening, while maintaining full control of electron spin. A spatial resolution of 2nm and temporal resolution of 10ps (ps) are expected in the future time resolved aberration-corrected spin-polarized LEEM (TR-AC-SPLEEM). The commissioning of the three-prism AC-LEEM has been successfully finished with the cold field emission source, with a spatial resolution below 2nm. Copyright © 2017 Elsevier B.V. All rights reserved.

Termination of the spin-resolved integer quantum Hall effect

NASA Astrophysics Data System (ADS)

Wong, L. W.; Jiang, H. W.; Palm, E.; Schaff, W. J.

1997-03-01

We report a magnetotransport study of the termination of the spin-resolved integer quantum Hall effect by controlled disorder in a gated GaAs/AlxGa1-xAs heterostructure. We have found that, for a given Nth Landau level, the difference in filling factors of a pair of spin-split resistivity peaks δνN=\\|νN↑-νN↓\\| changes rapidly from one to zero near a critical density nc. Scaling analysis shows that δνN collapses onto a single curve independent of N when plotted against the parameter (n-nc)/nc for five Landau levels. The effect of increasing the Zeeman energy is also examined by tilting the direction of magnetic field relative to the plane of the two-dimensional electron gas. Our experiment suggests the termination of the spin-resolved quantum Hall effect is a phase transition.

Spin coherence and dephasing of localized electrons in monolayer MoS 2

DOE PAGES

Yang, Luyi; Chen, Weibing; McCreary, Kathleen M.; ...

2015-11-10

Here, we report a systematic study of coherent spin precession and spin dephasing in electron-doped monolayer MoS 2. Using time-resolved Kerr rotation spectroscopy and applied in-plane magnetic fields, a nanosecond time scale Larmor spin precession signal commensurate with g-factor |g 0| ≃ 1.86 is observed in several different MoS 2 samples grown by chemical vapor deposition. The dephasing rate of this oscillatory signal increases linearly with magnetic field, suggesting that the coherence arises from a subensemble of localized electron spins having an inhomogeneously broadened distribution of g-factors, g 0 + Δg. In contrast to g 0, Δg is sample-dependent andmore » ranges from 0.042 to 0.115.« less

Quantitative analysis of magnetic spin and orbital moments from an oxidized iron (1 1 0) surface using electron magnetic circular dichroism.

PubMed

Thersleff, Thomas; Rusz, Jan; Rubino, Stefano; Hjörvarsson, Björgvin; Ito, Yasuo; J Zaluzec, Nestor; Leifer, Klaus

2015-08-17

Understanding the ramifications of reduced crystalline symmetry on magnetic behavior is a critical step in improving our understanding of nanoscale and interfacial magnetism. However, investigations of such effects are often controversial largely due to the challenges inherent in directly correlating nanoscale stoichiometry and structure to magnetic behavior. Here, we describe how to use Transmission Electron Microscope (TEM) to obtain Electron Magnetic Circular Dichroism (EMCD) signals as a function of scattering angle to locally probe the magnetic behavior of thin oxide layers grown on an Fe (1 1 0) surface. Experiments and simulations both reveal a strong dependence of the magnetic orbital to spin ratio on its scattering vector in reciprocal space. We exploit this variation to extract the magnetic properties of the oxide cladding layer, showing that it locally may exhibit an enhanced orbital to spin moment ratio. This finding is supported here by both spatially and angularly resolved EMCD measurements, opening up the way for compelling investigations into how magnetic properties are affected by nanoscale features.

Quantitative analysis of magnetic spin and orbital moments from an oxidized iron (1 1 0) surface using electron magnetic circular dichroism

DOE PAGES

Thersleff, Thomas; Rusz, Jan; Rubino, Stefano; ...

2015-08-17

Understanding the ramifications of reduced crystalline symmetry on magnetic behavior is a critical step in improving our understanding of nanoscale and interfacial magnetism. However, investigations of such effects are often controversial largely due to the challenges inherent in directly correlating nanoscale stoichiometry and structure to magnetic behavior. Here, we describe how to use Transmission Electron Microscope (TEM) to obtain Electron Magnetic Circular Dichroism (EMCD) signals as a function of scattering angle to locally probe the magnetic behavior of thin oxide layers grown on an Fe (1 1 0) surface. Experiments and simulations both reveal a strong dependence of the magneticmore » orbital to spin ratio on its scattering vector in reciprocal space. We exploit this variation to extract the magnetic properties of the oxide cladding layer, showing that it locally may exhibit an enhanced orbital to spin moment ratio. This finding is supported here by both spatially and angularly resolved EMCD measurements, opening up the way for compelling investigations into how magnetic properties are affected by nanoscale features.« less

Electronic structure of monolayer 1T'-MoTe2 grown by molecular beam epitaxy

NASA Astrophysics Data System (ADS)

Tang, Shujie; Zhang, Chaofan; Jia, Chunjing; Ryu, Hyejin; Hwang, Choongyu; Hashimoto, Makoto; Lu, Donghui; Liu, Zhi; Devereaux, Thomas P.; Shen, Zhi-Xun; Mo, Sung-Kwan

2018-02-01

Monolayer transition metal dichalcogenides (TMDCs) in the 1T' structural phase have drawn a great deal of attention due to the prediction of quantum spin Hall insulator states. The band inversion and the concomitant changes in the band topology induced by the structural distortion from 1T to 1T' phases are well established. However, the bandgap opening due to the strong spin-orbit coupling (SOC) is only verified for 1T'-WTe2 recently and still debated for other TMDCs. Here we report a successful growth of high-quality monolayer 1T'-MoTe2 on a bilayer graphene substrate through molecular beam epitaxy. Using in situ angle-resolved photoemission spectroscopy (ARPES), we have investigated the low-energy electronic structure and Fermi surface topology. The SOC-induced breaking of the band degeneracy points between the valence and conduction bands is clearly observed by ARPES. However, the strength of SOC is found to be insufficient to open a bandgap, which makes monolayer 1T'-MoTe2 on bilayer graphene a semimetal.

Electronic structure of monolayer 1T'-MoTe 2 grown by molecular beam epitaxy

DOE PAGES

Tang, Shujie; Zhang, Chaofan; Jia, Chunjing; ...

2017-11-14

Monolayer transition metal dichalcogenides (TMDCs) in the 1T' structural phase have drawn a great deal of attention due to the prediction of quantum spin Hall insulator states. The band inversion and the concomitant changes in the band topology induced by the structural distortion from 1T to 1T' phases are well established. However, the bandgap opening due to the strong spin-orbit coupling (SOC) is only verified for 1T'-WTe 2 recently and still debated for other TMDCs. Here we report a successful growth of high-quality monolayer 1T'-MoTe 2 on a bilayer graphene substrate through molecular beam epitaxy. Using in situ angle-resolved photoemissionmore » spectroscopy (ARPES), we have investigated the low-energy electronic structure and Fermi surface topology. The SOC-induced breaking of the band degeneracy points between the valence and conduction bands is clearly observed by ARPES. However, the strength of SOC is found to be insufficient to open a bandgap, which makes monolayer 1T'-MoTe 2 on bilayer graphene a semimetal.« less

Rapid high-resolution spin- and angle-resolved photoemission spectroscopy with pulsed laser source and time-of-flight spectrometer

NASA Astrophysics Data System (ADS)

Gotlieb, K.; Hussain, Z.; Bostwick, A.; Lanzara, A.; Jozwiak, C.

2013-09-01

A high-efficiency spin- and angle-resolved photoemission spectroscopy (spin-ARPES) spectrometer is coupled with a laboratory-based laser for rapid high-resolution measurements. The spectrometer combines time-of-flight (TOF) energy measurements with low-energy exchange scattering spin polarimetry for high detection efficiencies. Samples are irradiated with fourth harmonic photons generated from a cavity-dumped Ti:sapphire laser that provides high photon flux in a narrow bandwidth, with a pulse timing structure ideally matched to the needs of the TOF spectrometer. The overall efficiency of the combined system results in near-EF spin-resolved ARPES measurements with an unprecedented combination of energy resolution and acquisition speed. This allows high-resolution spin measurements with a large number of data points spanning multiple dimensions of interest (energy, momentum, photon polarization, etc.) and thus enables experiments not otherwise possible. The system is demonstrated with spin-resolved energy and momentum mapping of the L-gap Au(111) surface states, a prototypical Rashba system. The successful integration of the spectrometer with the pulsed laser system demonstrates its potential for simultaneous spin- and time-resolved ARPES with pump-probe based measurements.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tayebjee, Murad J. Y.; Sanders, Samuel N.; Kumarasamy, Elango

Singlet fission, in which two triplet excitons are generated from a single absorbed photon, is a key third-generation solar cell concept. Conservation of angular momentum requires that singlet fission populates correlated multiexciton states, which can subsequently dissociate to generate free triplets. However, little is known about electronic and spin correlations in these systems since, due to its typically short lifetime, the multiexciton state is challenging to isolate and study. Here, we use bridged pentacene dimers, which undergo intramolecular singlet fission while isolated in solution and in solid matrices, as a unimolecular model system that can trap long-lived multiexciton states. Wemore » also combine transient absorption and time-resolved electron spin resonance spectroscopies to show that spin correlations in the multiexciton state persist for hundreds of nanoseconds. Furthermore, we confirm long-standing predictions that singlet fission produces triplet pair states of quintet character. Finally, we compare two different pentacene–bridge–pentacene chromophores, systematically tuning the coupling between the pentacenes to understand how differences in molecular structure affect the population and dissociation of multiexciton quintet states.« less

Synthesis, characterization, and modeling of new molecule-based magnets

NASA Astrophysics Data System (ADS)

Olson, Christopher Samuel

The chemical bond and its role as a mediator of magnetic exchange interaction remains an important aspect in the study of magnetic insulators and semiconductors. The M[TCNE] (M = transition metal, TCNE = tetracyanoethylene) class of organic-based magnets has attracted considerable interest since V II[TCNE]x (x ˜ 2) exhibits one of the highest critical temperatures for its class -- Tc ˜ 400 K -- in addition to highly spin-polarized conduction and valance bands (Eg ˜ 0.5 eV), thus foreseeing potential spintronic application. The magneto-structural factors underlying this exceptional behavior remain elusive, however, due to the amorphous nature of the material. To address this, a novel synthetic route was utilized to produce new polycrystalline M[TCNE] solids (whose crystal structures have been resolved) with varying transition metal centers (Ni, Mn, Fe) and lattice dimensionality (2D-3D), exhibiting a wide range of Tc (40-170 K). Spectroscopic and magnetometric studies were performed and demonstrate that in 2D [M II(TCNE)(NCMe)2]X structures (M = Ni, Mn, Fe; X = diamagnetic anion), strong ligand-to-metal transfer of electron density from the organic TCNE radical plays a significant role in the formation of magnetic exchange pathways, while single-ion anisotropy strongly influences the critical temperature and below-Tc spin disorder for magnets in this material class. Additionally, using quantum-computational modeling, magnetic spin-density transfer trends, spin-polarized electronic structures, and electronic exchange coupling constants have been identified and interpreted in terms of 3d-orbital filling and dimensionality of magnetic interaction. These findings offer new perspectives on the stabilization of magnetic order in M[TCNE] solids.

When combined X-ray and polarized neutron diffraction data challenge high-level calculations: spin-resolved electron density of an organic radical.

PubMed

Voufack, Ariste Bolivard; Claiser, Nicolas; Lecomte, Claude; Pillet, Sébastien; Pontillon, Yves; Gillon, Béatrice; Yan, Zeyin; Gillet, Jean Michel; Marazzi, Marco; Genoni, Alessandro; Souhassou, Mohamed

2017-08-01

Joint refinement of X-ray and polarized neutron diffraction data has been carried out in order to determine charge and spin density distributions simultaneously in the nitronyl nitroxide (NN) free radical Nit(SMe)Ph. For comparison purposes, density functional theory (DFT) and complete active-space self-consistent field (CASSCF) theoretical calculations were also performed. Experimentally derived charge and spin densities show significant differences between the two NO groups of the NN function that are not observed from DFT theoretical calculations. On the contrary, CASSCF calculations exhibit the same fine details as observed in spin-resolved joint refinement and a clear asymmetry between the two NO groups.

High-Resolution Two-Dimensional Optical Spectroscopy of Electron Spins

NASA Astrophysics Data System (ADS)

Salewski, M.; Poltavtsev, S. V.; Yugova, I. A.; Karczewski, G.; Wiater, M.; Wojtowicz, T.; Yakovlev, D. R.; Akimov, I. A.; Meier, T.; Bayer, M.

2017-07-01

Multidimensional coherent optical spectroscopy is one of the most powerful tools for investigating complex quantum mechanical systems. While it was conceived decades ago in magnetic resonance spectroscopy using microwaves and radio waves, it has recently been extended into the visible and UV spectral range. However, resolving MHz energy splittings with ultrashort laser pulses still remains a challenge. Here, we analyze two-dimensional Fourier spectra for resonant optical excitation of resident electrons to localized trions or donor-bound excitons in semiconductor nanostructures subject to a transverse magnetic field. Particular attention is devoted to Raman coherence spectra, which allow one to accurately evaluate tiny splittings of the electron ground state and to determine the relaxation times in the electron spin ensemble. A stimulated steplike Raman process induced by a sequence of two laser pulses creates a coherent superposition of the ground-state doublet which can be retrieved only optically because of selective excitation of the same subensemble with a third pulse. This provides the unique opportunity to distinguish between different complexes that are closely spaced in energy in an ensemble. The related experimental demonstration is based on photon-echo measurements in an n -type CdTe /(Cd ,Mg )Te quantum-well structure detected by a heterodyne technique. The difference in the sub-μ eV range between the Zeeman splittings of donor-bound electrons and electrons localized at potential fluctuations can be resolved even though the homogeneous linewidth of the optical transitions is larger by 2 orders of magnitude.

Spin-dependent electron many-body effects in GaAs

NASA Astrophysics Data System (ADS)

Nemec, P.; Kerachian, Y.; van Driel, H. M.; Smirl, Arthur L.

2005-12-01

Time- and polarization-resolved differential transmission measurements employing same and oppositely circularly polarized 150fs optical pulses are used to investigate spin characteristics of conduction band electrons in bulk GaAs at 295K . Electrons and holes with densities in the 2×1016cm-3-1018cm-3 range are generated and probed with pulses whose center wavelength is between 865 and 775nm . The transmissivity results can be explained in terms of the spin sensitivity of both phase-space filling and many-body effects (band-gap renormalization and screening of the Coulomb enhancement factor). For excitation and probing at 865nm , just above the band-gap edge, the transmissivity changes mainly reflect spin-dependent phase-space filling which is dominated by the electron Fermi factors. However, for 775nm probing, the influence of many-body effects on the induced transmission change are comparable with those from reduced phase space filling, exposing the spin dependence of the many-body effects. If one does not take account of these spin-dependent effects one can misinterpret both the magnitude and time evolution of the electron spin polarization. For suitable measurements we find that the electron spin relaxation time is 130ps .

Femtosecond optical reflectivity measurements of lattice-mediated spin repulsions in photoexcited LaCoO3 thin films

NASA Astrophysics Data System (ADS)

Bielecki, J.; Rata, A. D.; Börjesson, L.

2014-01-01

We present results on the temperature dependence of ultrafast electron and lattice dynamics, measured with pump-probe transient reflectivity experiments, of an epitaxially grown LaCoO3 thin film under tensile strain. Probing spin-polarized transitions into the antibonding eg band provides a measure of the low-spin fraction, both as a function of temperature and time after photoexcitation. It is observed that femtosecond laser pulses destabilize the constant low-spin fraction (˜63%-64%) in equilibrium into a thermally activated state, driven by a subpicosecond change in spin gap Δ. From the time evolution of the low-spin fraction, it is possible to disentangle the thermal and lattice contributions to the spin state. A lattice mediated spin repulsion, identified as the governing factor determining the equilibrium spin state in thin-film LaCoO3, is observed. These results suggests that time-resolved spectroscopy is a sensitive probe of the spin state in LaCoO3 thin films, with the potential to bring forward quantitative insight into the complicated interplay between structure and spin state in LaCoO3.

Appearance of the minority dz2 surface state and disappearance of the image-potential state: Criteria for clean Fe(001)

NASA Astrophysics Data System (ADS)

Eibl, Christian; Schmidt, Anke B.; Donath, Markus

2012-10-01

The unoccupied surface electronic structure of clean and oxidized Fe(001) was studied with spin-resolved inverse photoemission and target current spectroscopy. For the clean surface, we detected a dz2 surface state with minority spin character just above the Fermi level, while the image-potential surface state disappears. The opposite is observed for the ordered p(1×1)O/Fe(001) surface: the dz2-type surface state is quenched, while the image-potential state shows up as a pronounced feature. This behavior indicates enhanced surface reflectivity at the oxidized surface. The appearance and disappearance of specific unoccupied surface states prove to be decisive criteria for a clean Fe(001) surface. In addition, enhanced spin asymmetry in the unoccupied states is observed for the oxidized surface. Our results have implications for the use of clean and oxidized Fe(001) films as spin-polarization detectors.

Direct Observation of Very Large Zero-Field Splitting in a Tetrahedral Ni(II)Se4 Coordination Complex.

PubMed

Jiang, Shang-Da; Maganas, Dimitrios; Levesanos, Nikolaos; Ferentinos, Eleftherios; Haas, Sabrina; Thirunavukkuarasu, Komalavalli; Krzystek, J; Dressel, Martin; Bogani, Lapo; Neese, Frank; Kyritsis, Panayotis

2015-10-14

The high-spin (S = 1) tetrahedral Ni(II) complex [Ni{(i)Pr2P(Se)NP(Se)(i)Pr2}2] was investigated by magnetometry, spectroscopic, and quantum chemical methods. Angle-resolved magnetometry studies revealed the orientation of the magnetization principal axes. The very large zero-field splitting (zfs), D = 45.40(2) cm(-1), E = 1.91(2) cm(-1), of the complex was accurately determined by far-infrared magnetic spectroscopy, directly observing transitions between the spin sublevels of the triplet ground state. These are the largest zfs values ever determined--directly--for a high-spin Ni(II) complex. Ab initio calculations further probed the electronic structure of the system, elucidating the factors controlling the sign and magnitude of D. The latter is dominated by spin-orbit coupling contributions of the Ni ions, whereas the corresponding effects of the Se atoms are remarkably smaller.

Topological Insulators: A New Platform for Fundamental Science and Applications

NASA Astrophysics Data System (ADS)

Bansil, Arun

2013-03-01

Topological insulators constitute a new phase of quantum matter whose recent discovery has focused world-wide attention on wide-ranging phenomena in materials driven by spin-orbit coupling effects well beyond their traditional role in determining magnetic properties. I will discuss how by exploiting electronic structure techniques we have been able to predict and understand the characteristics of many new classes of binary, ternary and quaternary topologically interesting systems. The flexibility of chemical, structural and magnetic parameters so obtained is the key ingredient for exploring fundamental science questions, including novel spin-textures and exotic superconducting states, as well as for the realization of multi-functional topological devices for thermoelectric, spintronics, information processing and other applications. I will also highlight new insights that have been enabled through our material-specific modeling of angle-resolved photoemission (ARPES) and scanning tunneling (STS) spectroscopies of topological surface states, including effects of the photoemission and tunneling matrix element, which is well-known to be important for a robust interpretation of various highly resolved spectroscopies. Work supported by the Materials Science & Engineering Division, Basic Energy Sciences, U. S. D. O. E.

Fermiology of the strongly spin-orbit coupled superconductor Sn(1-x)In(x)Te: implications for topological superconductivity.

PubMed

Sato, T; Tanaka, Y; Nakayama, K; Souma, S; Takahashi, T; Sasaki, S; Ren, Z; Taskin, A A; Segawa, Kouji; Ando, Yoichi

2013-05-17

We have performed angle-resolved photoemission spectroscopy on the strongly spin-orbit coupled low-carrier density superconductor Sn(1-x)In(x)Te (x = 0.045) to elucidate the electronic states relevant to the possible occurrence of topological superconductivity, as recently reported for this compound based on point-contact spectroscopy. The obtained energy-band structure reveals a small holelike Fermi surface centered at the L point of the bulk Brillouin zone, together with a signature of a topological surface state, indicating that this material is a doped topological crystalline insulator characterized by band inversion and mirror symmetry. A comparison of the electronic states with a band-noninverted superconductor possessing a similar Fermi surface structure, Pb(1-x)Tl(x)Te, suggests that the anomalous behavior in the superconducting state of Sn(1-x)In(x)Te is related to the peculiar orbital characteristics of the bulk valence band and/or the presence of a topological surface state.

Imaging Magnetization Structure and Dynamics in Ultrathin Y3Fe5O12/Pt Bilayers with High Sensitivity Using the Time-Resolved Longitudinal Spin Seebeck Effect

NASA Astrophysics Data System (ADS)

Bartell, Jason M.; Jermain, Colin L.; Aradhya, Sriharsha V.; Brangham, Jack T.; Yang, Fengyuan; Ralph, Daniel C.; Fuchs, Gregory D.

2017-04-01

We demonstrate an instrument for time-resolved magnetic imaging that is highly sensitive to the in-plane magnetization state and dynamics of thin-film bilayers of yttrium iron garnet [Y3Fe5O12(YIG )]/Pt : the time-resolved longitudinal spin Seebeck (TRLSSE) effect microscope. We detect the local in-plane magnetic orientation within the YIG by focusing a picosecond laser to generate thermally driven spin current from the YIG into the Pt by the spin Seebeck effect and then use the inverse spin Hall effect in the Pt to transduce this spin current to an output voltage. To establish the time resolution of TRLSSE, we show that pulsed optical heating of patterned YIG (20 nm )/Pt (6 nm )/Ru (2 nm ) wires generates a magnetization-dependent voltage pulse of less than 100 ps. We demonstrate TRLSSE microscopy to image both static magnetic structure and gigahertz-frequency magnetic resonance dynamics with submicron spatial resolution and a sensitivity to magnetic orientation below 0.3 °/√{H z } in ultrathin YIG.

Hyperfine rather than spin splittings dominate the fine structure of the B (4)Σ(-)-X (4)Σ(-) bands of AlC.

PubMed

Clouthier, Dennis J; Kalume, Aimable

2016-01-21

Laser-induced fluorescence and wavelength resolved emission spectra of the B (4)Σ(-)-X (4)Σ(-) band system of the gas phase cold aluminum carbide free radical have been obtained using the pulsed discharge jet technique. The radical was produced by electron bombardment of a precursor mixture of trimethylaluminum in high pressure argon. High resolution spectra show that each rotational line of the 0-0 and 1-1 bands of AlC is split into at least three components, with very similar splittings and intensities in both the P- and R-branches. The observed structure was reproduced by assuming bβS magnetic hyperfine coupling in the excited state, due to a substantial Fermi contact interaction of the unpaired electron in the aluminum 3s orbital. Rotational analysis has yielded ground and excited state equilibrium bond lengths in good agreement with the literature and our own ab initio values. Small discrepancies in the calculated intensities of the hyperfine lines suggest that the upper state spin-spin constant λ' is of the order of ≈ 0.025-0.030 cm(-1).

Ultrafast Imaging of Chiral Surface Plasmon by Photoemission Electron Microscopy

NASA Astrophysics Data System (ADS)

Dai, Yanan; Dabrowski, Maciej; Petek, Hrvoje

We employ Time-Resolved Photoemission Electron Microscopy (TR-PEEM) to study surface plasmon polariton (SPP) wave packet dynamics launched by tunable (VIS-UV) femtosecond pulses of various linear and circular polarizations. The plasmonic structures are micron size single-crystalline Ag islands grown in situ on Si surfaces and characterized by Low Energy Electron Microscopy (LEEM). The local fields of plasmonic modes enhance two and three photon photoemission (2PP and 3PP) at the regions of strong field enhancement. Imaging of the photoemission signal with PEEM electron optics thus images the plasmonic fields excited in the samples. The observed PEEM images with left and right circularly polarized light show chiral images, which is a consequence of the transverse spin momentum of surface plasmon. By changing incident light polarization, the plasmon interference pattern shifts with light ellipticity indicating a polarization dependent excitation phase of SPP. In addition, interferometric-time resolved measurements record the asymmetric SPP wave packet motion in order to characterize the dynamical properties of chiral SPP wave packets.

Spin-resolved inelastic electron scattering by spin waves in noncollinear magnets

NASA Astrophysics Data System (ADS)

dos Santos, Flaviano José; dos Santos Dias, Manuel; Guimarães, Filipe Souza Mendes; Bouaziz, Juba; Lounis, Samir

2018-01-01

Topological noncollinear magnetic phases of matter are at the heart of many proposals for future information nanotechnology, with novel device concepts based on ultrathin films and nanowires. Their operation requires understanding and control of the underlying dynamics, including excitations such as spin waves. So far, no experimental technique has attempted to probe large wave-vector spin waves in noncollinear low-dimensional systems. In this paper, we explain how inelastic electron scattering, being suitable for investigations of surfaces and thin films, can detect the collective spin-excitation spectra of noncollinear magnets. To reveal the particularities of spin waves in such noncollinear samples, we propose the usage of spin-polarized electron-energy-loss spectroscopy augmented with a spin analyzer. With the spin analyzer detecting the polarization of the scattered electrons, four spin-dependent scattering channels are defined, which allow us to filter and select specific spin-wave modes. We take as examples a topological nontrivial skyrmion lattice, a spin-spiral phase, and the conventional ferromagnet. Then we demonstrate that, counterintuitively and in contrast to the ferromagnetic case, even non-spin-flip processes can generate spin waves in noncollinear substrates. The measured dispersion and lifetime of the excitation modes permit us to fingerprint the magnetic nature of the substrate.

Determination of the band parameters of bulk 2H-MX2 (M = Mo, W; X = S, Se) by angle-resolved photoemission spectroscopy

PubMed Central

Kim, Beom Seo; Rhim, Jun-Won; Kim, Beomyoung; Kim, Changyoung; Park, Seung Ryong

2016-01-01

Monolayer MX2 (M = Mo, W; X = S, Se) has recently been drawn much attention due to their application possibility as well as the novel valley physics. On the other hand, it is also important to understand the electronic structures of bulk MX2 for material applications since it is very challenging to grow large size uniform and sustainable monolayer MX2. We performed angle-resolved photoemission spectroscopy and tight binding calculations to investigate the electronic structures of bulk 2H-MX2. We could extract all the important electronic band parameters for bulk 2H-MX2, including the band gap, direct band gap size at K (-K) point and spin splitting size. Upon comparing the parameters for bulk 2H-MX2 (our work) with mono- and multi-layer MX2 (published), we found that stacked layers, substrates for thin films, and carrier concentration significantly affect the parameters, especially the band gap size. The origin of such effect is discussed in terms of the screening effect. PMID:27805019

Dynamic spin injection into a quantum well coupled to a spin-split bound state

NASA Astrophysics Data System (ADS)

Maslova, N. S.; Rozhansky, I. V.; Mantsevich, V. N.; Arseyev, P. I.; Averkiev, N. S.; Lähderanta, E.

2018-05-01

We present a theoretical analysis of dynamic spin injection due to spin-dependent tunneling between a quantum well (QW) and a bound state split in spin projection due to an exchange interaction or external magnetic field. We focus on the impact of Coulomb correlations at the bound state on spin polarization and sheet density kinetics of the charge carriers in the QW. The theoretical approach is based on kinetic equations for the electron occupation numbers taking into account high order correlation functions for the bound state electrons. It is shown that the on-site Coulomb repulsion leads to an enhanced dynamic spin polarization of the electrons in the QW and a delay in the carriers tunneling into the bound state. The interplay of these two effects leads to nontrivial dependence of the spin polarization degree, which can be probed experimentally using time-resolved photoluminescence experiments. It is demonstrated that the influence of the Coulomb interactions can be controlled by adjusting the relaxation rates. These findings open a new way of studying the Hubbard-like electron interactions experimentally.

Dynamical control of Mn spin-system cooling by photogenerated carriers in a (Zn,Mn)Se/BeTe heterostructure

NASA Astrophysics Data System (ADS)

Debus, J.; Maksimov, A. A.; Dunker, D.; Yakovlev, D. R.; Tartakovskii, I. I.; Waag, A.; Bayer, M.

2010-08-01

The magnetization dynamics of the Mn spin system in an undoped (Zn,Mn)Se/BeTe type-II quantum well was studied by a time-resolved pump-probe photoluminescence technique. The Mn spin temperature was evaluated from the giant Zeeman shift of the exciton line in an external magnetic field of 3 T. The relaxation dynamics of the Mn spin temperature to the equilibrium temperature of the phonon bath after the pump-laser-pulse heating can be accelerated by the presence of free electrons. These electrons, generated by a control laser pulse, mediate the spin and energy transfer from the Mn spin system to the lattice and bypass the relatively slow direct spin-lattice relaxation of the Mn ions.

Ultrafast magnon generation in an Fe film on Cu(100).

PubMed

Schmidt, A B; Pickel, M; Donath, M; Buczek, P; Ernst, A; Zhukov, V P; Echenique, P M; Sandratskii, L M; Chulkov, E V; Weinelt, M

2010-11-05

We report on a combined experimental and theoretical study of the spin-dependent relaxation processes in the electron system of an iron film on Cu(100). Spin-, time-, energy- and angle-resolved two-photon photoemission shows a strong characteristic dependence of the lifetime of photoexcited electrons on their spin and energy. Ab initio calculations as well as a many-body treatment corroborate that the observed properties are determined by relaxation processes involving magnon emission. Thereby we demonstrate that magnon emission by hot electrons occurs on the femtosecond time scale and thus provides a significant source of ultrafast spin-flip processes. Furthermore, engineering of the magnon spectrum paves the way for tuning the dynamic properties of magnetic materials.

Inhomogeneous nuclear spin polarization induced by helicity-modulated optical excitation of fluorine-bound electron spins in ZnSe

NASA Astrophysics Data System (ADS)

Heisterkamp, F.; Greilich, A.; Zhukov, E. A.; Kirstein, E.; Kazimierczuk, T.; Korenev, V. L.; Yugova, I. A.; Yakovlev, D. R.; Pawlis, A.; Bayer, M.

2015-12-01

Optically induced nuclear spin polarization in a fluorine-doped ZnSe epilayer is studied by time-resolved Kerr rotation using resonant excitation of donor-bound excitons. Excitation with helicity-modulated laser pulses results in a transverse nuclear spin polarization, which is detected as a change of the Larmor precession frequency of the donor-bound electron spins. The frequency shift in dependence on the transverse magnetic field exhibits a pronounced dispersion-like shape with resonances at the fields of nuclear magnetic resonance of the constituent zinc and selenium isotopes. It is studied as a function of external parameters, particularly of constant and radio frequency external magnetic fields. The width of the resonance and its shape indicate a strong spatial inhomogeneity of the nuclear spin polarization in the vicinity of a fluorine donor. A mechanism of optically induced nuclear spin polarization is suggested based on the concept of resonant nuclear spin cooling driven by the inhomogeneous Knight field of the donor-bound electron.

Transient radical pairs studied by time-resolved EPR.

PubMed

Bittl, Robert; Weber, Stefan

2005-02-25

Photogenerated short-lived radical pairs (RP) are common in biological photoprocesses such as photosynthesis and enzymatic DNA repair. They can be favorably probed by time-resolved electron paramagnetic resonance (EPR) methods with adequate time resolution. Two EPR techniques have proven to be particularly useful to extract information on the working states of photoinduced biological processes that is only difficult or sometimes even impossible to obtain by other types of spectroscopy. Firstly, transient EPR yields crucial information on the chemical nature and the geometry of the individual RP halves in a doublet-spin pair generated by a short laser pulse. This time-resolved method is applicable in all magnetic field/microwave frequency regimes that are used for continuous-wave EPR, and is nowadays routinely utilized with a time resolution reaching about 10 ns. Secondly, a pulsed EPR method named out-of-phase electron spin echo envelope modulation (OOP-ESEEM) is increasingly becoming popular. By this pulsed technique, the mutual spin-spin interaction between the RP halves in a doublet-spin pair manifests itself as an echo modulation detected as a function of the microwave-pulse spacing of a two-pulse echo sequence subsequent to a laser pulse. From the dipolar coupling, the distance between the radicals is readily derived. Since the spin-spin interaction parameters are typically not observable by transient EPR, the two techniques complement each other favorably. Both EPR methods have recently been applied to a variety of light-induced RPs in photobiology. This review summarizes the results obtained from such studies in the fields of plant and bacterial photosynthesis and DNA repair mediated by the enzyme DNA photolyase.

In-situ spectro-microscopy on organic films: Mn-Phthalocyanine on Ag(100)

NASA Astrophysics Data System (ADS)

Al-Mahboob, Abdullah; Sadowski, Jerzy T.; Vescovo, Elio

2013-03-01

Metal phthalocyanines are attracting significant attention, owing to their potential for applications in chemical sensors, solar cells and organic magnets. As the electronic properties of molecular films are determined by their crystallinity and molecular packing, the optimization of film quality is important for improving the performance of organic devices. Here, we present the results of in situ low-energy electron microscopy / photoemission electron microscopy (LEEM/PEEM) studies of incorporation-limited growth of manganese-phthalocyanine (MnPc) on Ag(100) surfaces. MnPc thin films were grown on both, bulk Ag(100) surface and thin Ag(100)/Fe(100) films, where substrate spin-polarized electronic states can be modified through tuning the thickness of the Ag film. We also discuss the electronic structure and magnetic ordering in MnPc thin films, investigated by angle- and spin-resolved photoemission spectroscopy. Research carried out at the Center for Functional Nanomaterials and National Synchrotron Light Source, Brookhaven National Laboratory, which are supported by the U.S. Dept. of Energy, Office of Basic Energy Sciences, under Contract No. DE-AC02-98CH10886.

The electronic structure of iron in rhyolitic and basaltic glasses at high pressure

NASA Astrophysics Data System (ADS)

Solomatova, N. V.; Jackson, J. M.; Sturhahn, W.; Roskosz, M.

2016-12-01

The physical properties of silicate melts within the Earth's mantle affect the chemical and thermal evolution of the Earth's interior. To understand melting processes within the Earth, it is imperative to determine the structure of silicate melts at high pressure. It has been proposed that iron-bearing silicate melts may exist in the lower mantle just above the core-mantle boundary [1]. The behavior of iron in mantle melts is poorly understood, but can be experimentally approximated by iron-bearing silicate glasses. Previous studies have conflicting conclusions on whether iron in lower mantle silicate melts goes through a high-spin to low-spin transition [2-4]. Additionally, the average coordination environment of iron in glasses is poorly constrained. XANES experiments on basaltic glasses have demonstrated that both four and six-fold coordinated iron may exist in significant amounts regardless of oxidation state [5] while conventional Mössbauer experiments have observed five-fold coordinated Fe2+ with small amounts of four and six-fold coordinated Fe2+ [6]. In an attempt to resolve these discrepancies, we have measured the hyperfine parameters of iron-bearing rhyolitic glass up to 115 GPa and basaltic glass up to 92 GPa in a neon pressure medium using time-resolved synchrotron Mössbauer spectroscopy at the Advanced Photon Source (Argonne National Laboratory, IL). We observed changes in the hyperfine parameters likely due to coordination changes as a result of increasing pressure. Our results indicate that iron does not undergo a high-spin to low-spin transition within the pressure range investigated. Changes in the electronic configuration, such as the spin state of iron affects the compressibility and thermal properties of melts. With the assumption that silica glasses can be used to model structural behavior in silicate melts, our study predicts that iron in chemically-complex silica-rich melts in the lower mantle likely exists in a high-spin state. Select references: [1] Williams and Garnero, Science 273, 1528-1530 (1996). [2] Nomura et al., Nature 473, 199-202 (2011). [3] Gu et al., Geophys. Res. Lett. 39 (2012). [4] Mao et al., Am. Mineral. 99, 415-423 (2014). [5] Wilke et al., Chem. Geology 220, 143-161 (2005). [6] Cottrell and Kelley Earth Planet. Sci. Lett. 305, 270-282 (2011).

Circular polarization in a non-magnetic resonant tunneling device.

PubMed

Dos Santos, Lara F; Gobato, Yara Galvão; Teodoro, Márcio D; Lopez-Richard, Victor; Marques, Gilmar E; Brasil, Maria Jsp; Orlita, Milan; Kunc, Jan; Maude, Duncan K; Henini, Mohamed; Airey, Robert J

2011-01-25

We have investigated the polarization-resolved photoluminescence (PL) in an asymmetric n-type GaAs/AlAs/GaAlAs resonant tunneling diode under magnetic field parallel to the tunnel current. The quantum well (QW) PL presents strong circular polarization (values up to -70% at 19 T). The optical emission from GaAs contact layers shows evidence of highly spin-polarized two-dimensional electron and hole gases which affects the spin polarization of carriers in the QW. However, the circular polarization degree in the QW also depends on various other parameters, including the g-factors of the different layers, the density of carriers along the structure, and the Zeeman and Rashba effects.

Circular polarization in a non-magnetic resonant tunneling device

PubMed Central

2011-01-01

We have investigated the polarization-resolved photoluminescence (PL) in an asymmetric n-type GaAs/AlAs/GaAlAs resonant tunneling diode under magnetic field parallel to the tunnel current. The quantum well (QW) PL presents strong circular polarization (values up to -70% at 19 T). The optical emission from GaAs contact layers shows evidence of highly spin-polarized two-dimensional electron and hole gases which affects the spin polarization of carriers in the QW. However, the circular polarization degree in the QW also depends on various other parameters, including the g-factors of the different layers, the density of carriers along the structure, and the Zeeman and Rashba effects. PMID:21711613

New Measurement of the Electron Magnetic Moment and the Fine Structure Constant: A First Application of a One-Electron Quantum Cyclotron

ScienceCinema

Gabrielse, Gerald

2018-05-22

Remarkably, the famous UW measurement of the electron magnetic moment has stood since 1987. With QED theory, this measurement has determined the accepted value of the fine structure constant. This colloquium is about a new Harvard measurement of these fundamental constants. The new measurement has an uncertainty that is about six times smaller, and it shifts the values by 1.7 standard deviations. One electron suspended in a Penning trap is used for the new measurement, like in the old measurement. What is different is that the lowest quantum levels of the spin and cyclotron motion are resolved, and the cyclotron as well as spin frequencies are determined using quantum jump spectroscopy. In addition, a 0.1 mK Penning trap that is also a cylindrical microwave cavity is used to control the radiation field, to suppress spontaneous emission by more than a factor of 100, to control cavity shifts, and to eliminate the blackbody photons that otherwise stimulate excitations from the cyclotron ground state. Finally, great signal-to-noise for one-quantum transitions is obtained using electronic feedback to realize the first one-particle self-excited oscillator. The new methods may also allow a million times improved measurement of the 500 times small antiproton magnetic moment.

Chemical disorder in topological insulators: A route to magnetism tolerant topological surface states

DOE PAGES

Martínez-Velarte, M. Carmen; Kretz, Bernhard; Moro-Lagares, Maria; ...

2017-06-13

Here, we show that the chemical inhomogeneity in ternary three-dimensional topological insulators preserves the topological spin texture of their surface states against a net surface magnetization. The spin texture is that of a Dirac cone with helical spin structure in the reciprocal space, which gives rise to spin-polarized and dissipation-less charge currents. Thanks to the nontrivial topology of the bulk electronic structure, this spin texture is robust against most types of surface defects. However, magnetic perturbations break the time-reversal symmetry, enabling magnetic scattering and loss of spin coherence of the charge carriers. This intrinsic incompatibility precludes the design of magnetoelectronicmore » devices based on the coupling between magnetic materials and topological surface states. We demonstrate that the magnetization coming from individual Co atoms deposited on the surface can disrupt the spin coherence of the carriers in the archetypal topological insulator Bi 2Te 3, while in Bi 2Se 2Te the spin texture remains unperturbed. This is concluded from the observation of elastic backscattering events in quasiparticle interference patterns obtained by scanning tunneling spectroscopy. The mechanism responsible for the protection is investigated by energy resolved spectroscopy and ab initio calculations, and it is ascribed to the distorted adsorption geometry of localized magnetic moments due to Se–Te disorder, which suppresses the Co hybridization with the surface states.« less

Chemical disorder in topological insulators: A route to magnetism tolerant topological surface states

DOE Office of Scientific and Technical Information (OSTI.GOV)

Martínez-Velarte, M. Carmen; Kretz, Bernhard; Moro-Lagares, Maria

Here, we show that the chemical inhomogeneity in ternary three-dimensional topological insulators preserves the topological spin texture of their surface states against a net surface magnetization. The spin texture is that of a Dirac cone with helical spin structure in the reciprocal space, which gives rise to spin-polarized and dissipation-less charge currents. Thanks to the nontrivial topology of the bulk electronic structure, this spin texture is robust against most types of surface defects. However, magnetic perturbations break the time-reversal symmetry, enabling magnetic scattering and loss of spin coherence of the charge carriers. This intrinsic incompatibility precludes the design of magnetoelectronicmore » devices based on the coupling between magnetic materials and topological surface states. We demonstrate that the magnetization coming from individual Co atoms deposited on the surface can disrupt the spin coherence of the carriers in the archetypal topological insulator Bi 2Te 3, while in Bi 2Se 2Te the spin texture remains unperturbed. This is concluded from the observation of elastic backscattering events in quasiparticle interference patterns obtained by scanning tunneling spectroscopy. The mechanism responsible for the protection is investigated by energy resolved spectroscopy and ab initio calculations, and it is ascribed to the distorted adsorption geometry of localized magnetic moments due to Se–Te disorder, which suppresses the Co hybridization with the surface states.« less

Manipulating charge transfer excited state relaxation and spin crossover in iron coordination complexes with ligand substitution

DOE PAGES

Zhang, Wenkai; Kjaer, Kasper S.; Alonso-Mori, Roberto; ...

2016-08-25

Developing light-harvesting and photocatalytic molecules made with iron could provide a cost effective, scalable, and environmentally benign path for solar energy conversion. To date these developments have been limited by the sub-picosecond metal-to-ligand charge transfer (MLCT) electronic excited state lifetime of iron based complexes due to spin crossover – the extremely fast intersystem crossing and internal conversion to high spin metal-centered excited states. We revitalize a 30 year old synthetic strategy for extending the MLCT excited state lifetimes of iron complexes by making mixed ligand iron complexes with four cyanide (CN –) ligands and one 2,2'-bipyridine (bpy) ligand. This enablesmore » MLCT excited state and metal-centered excited state energies to be manipulated with partial independence and provides a path to suppressing spin crossover. We have combined X-ray Free-Electron Laser (XFEL) Kβ hard X-ray fluorescence spectroscopy with femtosecond time-resolved UV-visible absorption spectroscopy to characterize the electronic excited state dynamics initiated by MLCT excitation of [Fe(CN) 4(bpy)] 2–. The two experimental techniques are highly complementary; the time-resolved UV-visible measurement probes allowed electronic transitions between valence states making it sensitive to ligand-centered electronic states such as MLCT states, whereas the Kβ fluorescence spectroscopy provides a sensitive measure of changes in the Fe spin state characteristic of metal-centered excited states. Here, we conclude that the MLCT excited state of [Fe(CN) 4(bpy)] 2– decays with roughly a 20 ps lifetime without undergoing spin crossover, exceeding the MLCT excited state lifetime of [Fe(2,2'-bipyridine) 3] 2+ by more than two orders of magnitude.« less

Anisotropic interactions of a single spin and dark-spin spectroscopy in diamond

NASA Astrophysics Data System (ADS)

Epstein, R. J.; Mendoza, F. M.; Kato, Y. K.; Awschalom, D. D.

2005-11-01

Experiments on single nitrogen-vacancy (N-V) centres in diamond, which include electron spin resonance, Rabi oscillations, single-shot spin readout and two-qubit operations with a nearby13C nuclear spin, show the potential of this spin system for solid-state quantum information processing. Moreover, N-V centre ensembles can have spin-coherence times exceeding 50 μs at room temperature. We have developed an angle-resolved magneto-photoluminescence microscope apparatus to investigate the anisotropic electron-spin interactions of single N-V centres at room temperature. We observe negative peaks in the photoluminescence as a function of both magnetic-field magnitude and angle that are explained by coherent spin precession and anisotropic relaxation at spin-level anti-crossings. In addition, precise field alignment unmasks the resonant coupling to neighbouring `dark' nitrogen spins, otherwise undetected by photoluminescence. These results demonstrate the capability of our spectroscopic technique for measuring small numbers of dark spins by means of a single bright spin under ambient conditions.

Superconductivity switch from spin-singlet to -triplet pairing in a topological superconducting junction.

PubMed

Tao, Ze; Chen, F J; Zhou, L Y; Li, Bin; Tao, Y C; Wang, J

2018-06-06

The interedge coupling is the cardinal characteristic of the narrow quantum spin Hall (QSH) insulator, and thus could bring about exotic transport phenomena. Herein, we present a theoretical investigation of the spin-resolved Andreev reflection (AR) in a QSH insulator strip touching on two neighbouring ferromagnetic insulators and one s-wave superconductor. It is demonstrated that, due to the interplay of the interedge coupling and ferromagnetic configuration, there could be not only usual local ARs leading to the spin-singlet pairing with the incident electron and Andreev-reflected hole from different spin subbands, but also novel local ARs giving rise to the spin-triplet pairing from the same spin subband. However, only the latter exists in the absence of the interedge coupling, and therefore the two pairings in turn testify the helical spin texture of the edge states. By proper tuning of the band structures of the ferromagnetic layers, under the resonance bias voltage, the usual and novel local ARs of [Formula: see text] can be all exhibited, resulting in fully spin-polarized pure spin-singlet superconductivity and pure spin-triplet superconductivity, respectively, which suggests a superconductivity switch from spin-singlet to -triplet pairing by electrical control. The results can be experimentally confirmed by the tunneling conductance and the noise power.

Superconductivity switch from spin-singlet to -triplet pairing in a topological superconducting junction

NASA Astrophysics Data System (ADS)

Tao, Ze; Chen, F. J.; Zhou, L. Y.; Li, Bin; Tao, Y. C.; Wang, J.

2018-06-01

The interedge coupling is the cardinal characteristic of the narrow quantum spin Hall (QSH) insulator, and thus could bring about exotic transport phenomena. Herein, we present a theoretical investigation of the spin-resolved Andreev reflection (AR) in a QSH insulator strip touching on two neighbouring ferromagnetic insulators and one s-wave superconductor. It is demonstrated that, due to the interplay of the interedge coupling and ferromagnetic configuration, there could be not only usual local ARs leading to the spin-singlet pairing with the incident electron and Andreev-reflected hole from different spin subbands, but also novel local ARs giving rise to the spin-triplet pairing from the same spin subband. However, only the latter exists in the absence of the interedge coupling, and therefore the two pairings in turn testify the helical spin texture of the edge states. By proper tuning of the band structures of the ferromagnetic layers, under the resonance bias voltage, the usual and novel local ARs of can be all exhibited, resulting in fully spin-polarized pure spin-singlet superconductivity and pure spin-triplet superconductivity, respectively, which suggests a superconductivity switch from spin-singlet to -triplet pairing by electrical control. The results can be experimentally confirmed by the tunneling conductance and the noise power.

Maximal Rashba-like spin splitting via kinetic-energy-coupled inversion-symmetry breaking.

PubMed

Sunko, Veronika; Rosner, H; Kushwaha, P; Khim, S; Mazzola, F; Bawden, L; Clark, O J; Riley, J M; Kasinathan, D; Haverkort, M W; Kim, T K; Hoesch, M; Fujii, J; Vobornik, I; Mackenzie, A P; King, P D C

2017-09-27

Engineering and enhancing the breaking of inversion symmetry in solids-that is, allowing electrons to differentiate between 'up' and 'down'-is a key goal in condensed-matter physics and materials science because it can be used to stabilize states that are of fundamental interest and also have potential practical applications. Examples include improved ferroelectrics for memory devices and materials that host Majorana zero modes for quantum computing. Although inversion symmetry is naturally broken in several crystalline environments, such as at surfaces and interfaces, maximizing the influence of this effect on the electronic states of interest remains a challenge. Here we present a mechanism for realizing a much larger coupling of inversion-symmetry breaking to itinerant surface electrons than is typically achieved. The key element is a pronounced asymmetry of surface hopping energies-that is, a kinetic-energy-coupled inversion-symmetry breaking, the energy scale of which is a substantial fraction of the bandwidth. Using spin- and angle-resolved photoemission spectroscopy, we demonstrate that such a strong inversion-symmetry breaking, when combined with spin-orbit interactions, can mediate Rashba-like spin splittings that are much larger than would typically be expected. The energy scale of the inversion-symmetry breaking that we achieve is so large that the spin splitting in the CoO 2 - and RhO 2 -derived surface states of delafossite oxides becomes controlled by the full atomic spin-orbit coupling of the 3d and 4d transition metals, resulting in some of the largest known Rashba-like spin splittings. The core structural building blocks that facilitate the bandwidth-scaled inversion-symmetry breaking are common to numerous materials. Our findings therefore provide opportunities for creating spin-textured states and suggest routes to interfacial control of inversion-symmetry breaking in designer heterostructures of oxides and other material classes.

The extraction of the spin structure function, g2 (and g1) at low Bjorken x

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ndukum, Luwani Z.

2015-08-01

The Spin Asymmetries of the Nucleon Experiment (SANE) used the Continuous Electron Beam Accelerator Facility at Jefferson Laboratory in Newport News, VA to investigate the spin structure of the proton. The experiment measured inclusive double polarization electron asymmetries using a polarized electron beam, scattered off a solid polarized ammonia target with target polarization aligned longitudinal and near transverse to the electron beam, allowing the extraction of the spin asymmetries A1 and A2, and spin structure functions g1 and g2. Polarized electrons of energies of 4.7 and 5.9 GeV were used. The scattered electrons were detected by a novel, non-magnetic arraymore » of detectors observing a four-momentum transfer range of 2.5 to 6.5 GeV*V. This document addresses the extraction of the spin asymmetries and spin structure functions, with a focus on spin structure function, g2 (and g1) at low Bjorken x. The spin structure functions were measured as a function of x and W in four Q square bins. A full understanding of the low x region is necessary to get clean results for SANE and extend our understanding of the kinematic region at low x.« less

Local self-energies for V and Pd emergent from a nonlocal LDA+FLEX implementation

NASA Astrophysics Data System (ADS)

Savrasov, Sergey Y.; Resta, Giacomo; Wan, Xiangang

2018-04-01

In the spirit of recently developed LDA+U and LDA+DMFT methods, we implement a combination of density functional theory in its local density approximation (LDA) with a k - and ω -dependent self-energy found from diagrammatic fluctuational exchange (FLEX) approximation. The active Hilbert space here is described by the correlated subset of electrons which allows one to tremendously reduce the sizes of the matrices needed to represent charge and spin susceptibilities. The method is perturbative in nature but accounts for both bubble and ladder diagrams and accumulates the physics of momentum-resolved spin fluctuations missing in such popular approach as GW. As an application, we study correlation effects on band structures in V and Pd. The d -electron self-energies emergent from this calculation are found to be remarkably k independent. However, when we compare our calculated electronic mass enhancements against LDA+DMFT, we find that for the longstanding problem of spin fluctuations in Pd, LDA+FLEX delivers a better agreement with experiment, although this conclusion depends on a particular value of the Hubbard U used in the simulation. We also discuss outcomes of a recently proposed combination of k -dependent FLEX with dynamical mean-field theory (DMFT).

Exact-exchange spin-density functional theory of Wigner localization and phase transitions in quantum rings

NASA Astrophysics Data System (ADS)

Arnold, Thorsten; Siegmund, Marc; Pankratov, Oleg

2011-08-01

We apply exact-exchange spin-density functional theory in the Krieger-Li-Iafrate approximation to interacting electrons in quantum rings of different widths. The rings are threaded by a magnetic flux that induces a persistent current. A weak space and spin symmetry breaking potential is introduced to allow for localized solutions. As the electron-electron interaction strength described by the dimensionless parameter rS is increased, we observe—at a fixed spin magnetic moment—the subsequent transition of both spin sub-systems from the Fermi liquid to the Wigner crystal state. A dramatic signature of Wigner crystallization is that the persistent current drops sharply with increasing rS. We observe simultaneously the emergence of pronounced oscillations in the spin-resolved densities and in the electron localization functions indicating a spatial electron localization showing ferrimagnetic order after both spin sub-systems have undergone the Wigner crystallization. The critical rSc at the transition point is substantially smaller than in a fully spin-polarized system and decreases further with decreasing ring width. Relaxing the constraint of a fixed spin magnetic moment, we find that on increasing rS the stable phase changes from an unpolarized Fermi liquid to an antiferromagnetic Wigner crystal and finally to a fully polarized Fermi liquid.

Exact-exchange spin-density functional theory of Wigner localization and phase transitions in quantum rings.

PubMed

Arnold, Thorsten; Siegmund, Marc; Pankratov, Oleg

2011-08-24

We apply exact-exchange spin-density functional theory in the Krieger-Li-Iafrate approximation to interacting electrons in quantum rings of different widths. The rings are threaded by a magnetic flux that induces a persistent current. A weak space and spin symmetry breaking potential is introduced to allow for localized solutions. As the electron-electron interaction strength described by the dimensionless parameter r(S) is increased, we observe-at a fixed spin magnetic moment-the subsequent transition of both spin sub-systems from the Fermi liquid to the Wigner crystal state. A dramatic signature of Wigner crystallization is that the persistent current drops sharply with increasing r(S). We observe simultaneously the emergence of pronounced oscillations in the spin-resolved densities and in the electron localization functions indicating a spatial electron localization showing ferrimagnetic order after both spin sub-systems have undergone the Wigner crystallization. The critical r(S)(c) at the transition point is substantially smaller than in a fully spin-polarized system and decreases further with decreasing ring width. Relaxing the constraint of a fixed spin magnetic moment, we find that on increasing r(S) the stable phase changes from an unpolarized Fermi liquid to an antiferromagnetic Wigner crystal and finally to a fully polarized Fermi liquid. © 2011 IOP Publishing Ltd

Generalized GW+Boltzmann Approach for the Description of Ultrafast Electron Dynamics in Topological Insulators

PubMed Central

Battiato, Marco; Sánchez-Barriga, Jaime

2017-01-01

Quantum-phase transitions between trivial insulators and topological insulators differ from ordinary metal-insulator transitions in that they arise from the inversion of the bulk band structure due to strong spin–orbit coupling. Such topological phase transitions are unique in nature as they lead to the emergence of topological surface states which are characterized by a peculiar spin texture that is believed to play a central role in the generation and manipulation of dissipationless surface spin currents on ultrafast timescales. Here, we provide a generalized GW+Boltzmann approach for the description of ultrafast dynamics in topological insulators driven by electron–electron and electron–phonon scatterings. Taking the prototypical insulator Bi2Te3 as an example, we test the robustness of our approach by comparing the theoretical prediction to results of time- and angle-resolved photoemission experiments. From this comparison, we are able to demonstrate the crucial role of the excited spin texture in the subpicosecond relaxation of transient electrons, as well as to accurately obtain the magnitude and strength of electron–electron and electron–phonon couplings. Our approach could be used as a generalized theory for three-dimensional topological insulators in the bulk-conducting transport regime, paving the way for the realization of a unified theory of ultrafast dynamics in topological materials. PMID:28773171

Photodissociation spectroscopy and ab initio calculations for the Sr +-N 2 complex

NASA Astrophysics Data System (ADS)

Massaouti, Maria; Fanourgakis, George S.; Velegrakis, Michalis

2010-04-01

Electronic vibrationally resolved spectra of the Sr +-N 2 complex have been recorded in two energy regions 20 284-22 988 cm -1 and 15 576-16 380 cm -1. In the high energy region, two progressions are present and they are attributed to the (2) 2Π 3/2,1/2 ← X2Σ+ transitions assuming a linear molecule. This linear configuration is supported from the observed spin-orbit splitting of these excited states as well as from electronic structure calculations. The lower energy spectrum shows a structure, which ends up to a continuum. Considering the complex as an anharmonic oscillator, the spectroscopic constants and the dissociation energies of the corresponding states are determined.

Quintet multiexciton dynamics in singlet fission

DOE PAGES

Tayebjee, Murad J. Y.; Sanders, Samuel N.; Kumarasamy, Elango; ...

2016-10-17

Singlet fission, in which two triplet excitons are generated from a single absorbed photon, is a key third-generation solar cell concept. Conservation of angular momentum requires that singlet fission populates correlated multiexciton states, which can subsequently dissociate to generate free triplets. However, little is known about electronic and spin correlations in these systems since, due to its typically short lifetime, the multiexciton state is challenging to isolate and study. Here, we use bridged pentacene dimers, which undergo intramolecular singlet fission while isolated in solution and in solid matrices, as a unimolecular model system that can trap long-lived multiexciton states. Wemore » also combine transient absorption and time-resolved electron spin resonance spectroscopies to show that spin correlations in the multiexciton state persist for hundreds of nanoseconds. Furthermore, we confirm long-standing predictions that singlet fission produces triplet pair states of quintet character. Finally, we compare two different pentacene–bridge–pentacene chromophores, systematically tuning the coupling between the pentacenes to understand how differences in molecular structure affect the population and dissociation of multiexciton quintet states.« less

Magnetic coupling of Fe-porphyrin molecules adsorbed on clean and c(2×2) oxygen-reconstructed Co(100) investigated by spin-polarized photoemission spectroscopy

NASA Astrophysics Data System (ADS)

Weber, A. P.; Caruso, A. N.; Vescovo, E.; Ali, Md. E.; Tarafder, K.; Janjua, S. Z.; Sadowski, J. T.; Oppeneer, P. M.

2013-05-01

The spin-polarized electronic structure of iron octaethylporphyrin (FeOEP) molecules adsorbed on a pristine and on a c(2×2) oxygen-reconstructed Co(100) surface has been analyzed by means of spin-polarized photoemission spectroscopy (SPPES) and first-principles density functional theory with the on-site Coulomb repulsion U term (DFT+U) calculations with and without Van der Waals corrections. The aim is to examine the magnetic exchange mechanism between the FeOEP molecules and the Co(100) substrate in the presence or absence of the oxygen mediator. The results demonstrate that the magnetic coupling from the ferromagnetic substrate to the adsorbed FeOEP molecules is ferromagnetic, whereas, the coupling is antiferromagnetic for the FeOEP on the c(2×2)O/Co(100) system. Spin-resolved partial densities of states extracted from ab initio DFT+U modeling are in fairly good comparison with the electronic spectral densities seen in angle-integrated SPPES energy dispersion curves for submonolayer coverages of FeOEP. Through combined analysis of these spectra and theoretical results, we determine that hybridization of 2p orbitals of N and O with Co 3d orbitals facilitates indirect magnetic exchange interactions between Fe and Co, whereas, a direct Fe-Co interaction involving the Fe dz2 orbital is also found for FeOEP on Co. It is observed through SPPES that the spin polarization of the photoemission-visible molecular overlayers decreases to zero as coverage is increased beyond the submonolayer regime, indicating that only interfacial magnetic coupling is at work. Microspot low-energy electron diffraction and low-energy electron microscopy were performed to characterize the physical order of the molecular coverage, revealing that FeOEP structural domains are orders of magnitude greater in size on c(2×2)O/Co(100) than on clean Co(100), which coincides with reduced scattering from the disorder and sharper features seen in SPPES.

Quasiparticle interference in unconventional 2D systems.

PubMed

Chen, Lan; Cheng, Peng; Wu, Kehui

2017-03-15

At present, research of 2D systems mainly focuses on two kinds of materials: graphene-like materials and transition-metal dichalcogenides (TMDs). Both of them host unconventional 2D electronic properties: pseudospin and the associated chirality of electrons in graphene-like materials, and spin-valley-coupled electronic structures in the TMDs. These exotic electronic properties have attracted tremendous interest for possible applications in nanodevices in the future. Investigation on the quasiparticle interference (QPI) in 2D systems is an effective way to uncover these properties. In this review, we will begin with a brief introduction to 2D systems, including their atomic structures and electronic bands. Then, we will discuss the formation of Friedel oscillation due to QPI in constant energy contours of electron bands, and show the basic concept of Fourier-transform scanning tunneling microscopy/spectroscopy (FT-STM/STS), which can resolve Friedel oscillation patterns in real space and consequently obtain the QPI patterns in reciprocal space. In the next two parts, we will summarize some pivotal results in the investigation of QPI in graphene and silicene, in which systems the low-energy quasiparticles are described by the massless Dirac equation. The FT-STM experiments show there are two different interference channels (intervalley and intravalley scattering) and backscattering suppression, which associate with the Dirac cones and the chirality of quasiparticles. The monolayer and bilayer graphene on different substrates (SiC and metal surfaces), and the monolayer and multilayer silicene on a Ag(1 1 1) surface will be addressed. The fifth part will introduce the FT-STM research on QPI in TMDs (monolayer and bilayer of WSe 2 ), which allow us to infer the spin texture of both conduction and valence bands, and present spin-valley coupling by tracking allowed and forbidden scattering channels.

High-resolution magnetic resonance spectroscopy using a solid-state spin sensor

NASA Astrophysics Data System (ADS)

Glenn, David R.; Bucher, Dominik B.; Lee, Junghyun; Lukin, Mikhail D.; Park, Hongkun; Walsworth, Ronald L.

2018-03-01

Quantum systems that consist of solid-state electronic spins can be sensitive detectors of nuclear magnetic resonance (NMR) signals, particularly from very small samples. For example, nitrogen–vacancy centres in diamond have been used to record NMR signals from nanometre-scale samples, with sensitivity sufficient to detect the magnetic field produced by a single protein. However, the best reported spectral resolution for NMR of molecules using nitrogen–vacancy centres is about 100 hertz. This is insufficient to resolve the key spectral identifiers of molecular structure that are critical to NMR applications in chemistry, structural biology and materials research, such as scalar couplings (which require a resolution of less than ten hertz) and small chemical shifts (which require a resolution of around one part per million of the nuclear Larmor frequency). Conventional, inductively detected NMR can provide the necessary high spectral resolution, but its limited sensitivity typically requires millimetre-scale samples, precluding applications that involve smaller samples, such as picolitre-volume chemical analysis or correlated optical and NMR microscopy. Here we demonstrate a measurement technique that uses a solid-state spin sensor (a magnetometer) consisting of an ensemble of nitrogen–vacancy centres in combination with a narrowband synchronized readout protocol to obtain NMR spectral resolution of about one hertz. We use this technique to observe NMR scalar couplings in a micrometre-scale sample volume of approximately ten picolitres. We also use the ensemble of nitrogen–vacancy centres to apply NMR to thermally polarized nuclear spins and resolve chemical-shift spectra from small molecules. Our technique enables analytical NMR spectroscopy at the scale of single cells.

Investigation of charge injection and transport behavior in multilayer structure consisted of ferromagnetic metal and organic polymer under external fields

NASA Astrophysics Data System (ADS)

Zhao, Hua; Meng, Wei-Feng

2017-10-01

In this paper a five layer organic electronic device with alternately placed ferromagnetic metals and organic polymers: ferromagnetic metal/organic layer/ferromagnetic metal/organic layer/ferromagnetic metal, which is injected a spin-polarized electron from outsides, is studied theoretically using one-dimensional tight binding model Hamiltonian. We calculated equilibrium state behavior after an electron with spin is injected into the organic layer of this structure, charge density distribution and spin polarization density distribution of this injected spin-polarized electron, and mainly studied possible transport behavior of the injected spin polarized electron in this multilayer structure under different external electric fields. We analyze the physical process of the injected electron in this multilayer system. It is found by our calculation that the injected spin polarized electron exists as an electron-polaron state with spin polarization in the organic layer and it can pass through the middle ferromagnetic layer from the right-hand organic layer to the left-hand organic layer by the action of increasing external electric fields, which indicates that this structure may be used as a possible spin-polarized charge electronic device and also may provide a theoretical base for the organic electronic devices and it is also found that in the boundaries between the ferromagnetic layer and the organic layer there exist induced interface local dipoles due to the external electric fields.

Ultrafast spintronics roadmap: from femtosecond spin current pulses to terahertz non-uniform spin dynamics via nano-confined spin transfer torques (Conference Presentation)

NASA Astrophysics Data System (ADS)

Melnikov, Alexey; Razdolski, Ilya; Alekhin, Alexandr; Ilin, Nikita; Meyburg, Jan; Diesing, Detlef; Roddatis, Vladimir; Rungger, Ivan; Stamenova, Maria; Sanvito, Stefano; Bovensiepen, Uwe

2016-10-01

Further development of spintronics requires miniaturization and reduction of characteristic timescales of spin dynamics combining the nanometer spatial and femtosecond temporal ranges. These demands shift the focus of interest towards the fundamental open question of the interaction of femtosecond spin current (SC) pulses with a ferromagnet (FM). The spatio-temporal properties of the spin transfer torque (STT) exerted by ultrashort SC pulses on the FM open the time domain for studying STT fingerprint on spatially non-uniform magnetization dynamics. Using the sensitivity of magneto-induced second harmonic generation to SC, we develop technique for SC monitoring. With 20 fs resolution, we demonstrate the generation of 250 fs-long SC pulses in Fe/Au/Fe/MgO(001) structures. Their temporal profile indicates (i) nearly-ballistic hot electron transport in Au and (ii) that the pulse duration is primarily determined by the thermalization time of laser-excited hot carriers in Fe. Together with strongly spin-dependent Fe/Au interface transmission calculated for these carriers, this suggests the non-thermal spin-dependent Seebeck effect dominating the generation of ultrashort SC pulses. The analysis of SC transmission/reflection at the Au/Fe interface shows that hot electron spins orthogonal to the Fe magnetization rotate gaining huge parallel (anti-parallel) projection in transmitted (reflected) SC. This is accompanied by a STT-induced perturbation of the magnetization localized at the interface, which excites the inhomogeneous high-frequency spin dynamics in the FM. Time-resolved magneto-optical studies reveal the excitation of several standing spin wave modes in the Fe film with their spectrum extending up to 0.6 THz and indicating the STT spatial confinement to 2 nm.

Chemical modulation of electronic structure at the excited state

NASA Astrophysics Data System (ADS)

Li, F.; Song, C.; Gu, Y. D.; Saleem, M. S.; Pan, F.

2017-12-01

Spin-polarized electronic structures are the cornerstone of spintronics, and have thus attracted a significant amount of interest; in particular, researchers are looking into how to modulate the electronic structure to enable multifunctional spintronics applications, especially in half-metallic systems. However, the control of the spin polarization has only been predicted in limited two-dimensional systems with spin-polarized Dirac structures and is difficult to achieve experimentally. Here, we report the modulation of the electronic structure in the light-induced excited state in a typical half-metal, L a1 /2S r1 /2Mn O3 -δ . According to the spin-transport measurements, there appears a light-induced increase in magnetoresistance due to the enhanced spin scattering, which is closely associated with the excited spin polarization. Strikingly, the light-induced variation can be enhanced via alcohol processing and reduced by oxygen annealing. X-ray photoelectron spectroscopy measurements show that in the chemical process, a redox reaction occurs with a change in the valence of Mn. Furthermore, first-principles calculations reveal that the change in the valence of Mn alters the electronic structure and consequently modulates the spin polarization in the excited state. Our findings thus report a chemically tunable electronic structure, demonstrating interesting physics and the potential for multifunctional applications and ultrafast spintronics.

Femtosecond time-resolved optical and Raman spectroscopy of photoinduced spin crossover: temporal resolution of low-to-high spin optical switching.

PubMed

Smeigh, Amanda L; Creelman, Mark; Mathies, Richard A; McCusker, James K

2008-10-29

A combination of femtosecond electronic absorption and stimulated Raman spectroscopies has been employed to determine the kinetics associated with low-spin to high-spin conversion following charge-transfer excitation of a FeII spin-crossover system in solution. A time constant of tau = 190 +/- 50 fs for the formation of the 5T2 ligand-field state was assigned based on the establishment of two isosbestic points in the ultraviolet in conjunction with changes in ligand stretching frequencies and Raman scattering amplitudes; additional dynamics observed in both the electronic and vibrational spectra further indicate that vibrational relaxation in the high-spin state occurs with a time constant of ca. 10 ps. The results set an important precedent for extremely rapid, formally forbidden (DeltaS = 2) nonradiative relaxation as well as defining the time scale for intramolecular optical switching between two electronic states possessing vastly different spectroscopic, geometric, and magnetic properties.

High-pressure studies with x-rays using diamond anvil cells

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shen, Guoyin; Mao, Ho Kwang

2016-11-22

Pressure profoundly alters all states of matter. The symbiotic development of ultrahigh-pressure diamond anvil cells, to compress samples to sustainable multi-megabar pressures; and synchrotron x-ray techniques, to probe materials' properties in situ, has enabled the exploration of rich high-pressure (HP) science. In this article, we first introduce the essential concept of diamond anvil cell technology, together with recent developments and its integration with other extreme environments. We then provide an overview of the latest developments in HP synchrotron techniques, their applications, and current problems, followed by a discussion of HP scientific studies using x-rays in the key multidisciplinary fields. Thesemore » HP studies include: HP x-ray emission spectroscopy, which provides information on the filled electronic states of HP samples; HP x-ray Raman spectroscopy, which probes the HP chemical bonding changes of light elements; HP electronic inelastic x-ray scattering spectroscopy, which accesses high energy electronic phenomena, including electronic band structure, Fermi surface, excitons, plasmons, and their dispersions; HP resonant inelastic x-ray scattering spectroscopy, which probes shallow core excitations, multiplet structures, and spin-resolved electronic structure; HP nuclear resonant x-ray spectroscopy, which provides phonon densities of state and time-resolved Mössbauer information; HP x-ray imaging, which provides information on hierarchical structures, dynamic processes, and internal strains; HP x-ray diffraction, which determines the fundamental structures and densities of single-crystal, polycrystalline, nanocrystalline, and non-crystalline materials; and HP radial x-ray diffraction, which yields deviatoric, elastic and rheological information. Integrating these tools with hydrostatic or uniaxial pressure media, laser and resistive heating, and cryogenic cooling, has enabled investigations of the structural, vibrational, electronic, and magnetic properties of materials over a wide range of pressure-temperature conditions.« less

High-pressure studies with x-rays using diamond anvil cells

NASA Astrophysics Data System (ADS)

Shen, Guoyin; Mao, Ho Kwang

2017-01-01

Pressure profoundly alters all states of matter. The symbiotic development of ultrahigh-pressure diamond anvil cells, to compress samples to sustainable multi-megabar pressures; and synchrotron x-ray techniques, to probe materials’ properties in situ, has enabled the exploration of rich high-pressure (HP) science. In this article, we first introduce the essential concept of diamond anvil cell technology, together with recent developments and its integration with other extreme environments. We then provide an overview of the latest developments in HP synchrotron techniques, their applications, and current problems, followed by a discussion of HP scientific studies using x-rays in the key multidisciplinary fields. These HP studies include: HP x-ray emission spectroscopy, which provides information on the filled electronic states of HP samples; HP x-ray Raman spectroscopy, which probes the HP chemical bonding changes of light elements; HP electronic inelastic x-ray scattering spectroscopy, which accesses high energy electronic phenomena, including electronic band structure, Fermi surface, excitons, plasmons, and their dispersions; HP resonant inelastic x-ray scattering spectroscopy, which probes shallow core excitations, multiplet structures, and spin-resolved electronic structure; HP nuclear resonant x-ray spectroscopy, which provides phonon densities of state and time-resolved Mössbauer information; HP x-ray imaging, which provides information on hierarchical structures, dynamic processes, and internal strains; HP x-ray diffraction, which determines the fundamental structures and densities of single-crystal, polycrystalline, nanocrystalline, and non-crystalline materials; and HP radial x-ray diffraction, which yields deviatoric, elastic and rheological information. Integrating these tools with hydrostatic or uniaxial pressure media, laser and resistive heating, and cryogenic cooling, has enabled investigations of the structural, vibrational, electronic, and magnetic properties of materials over a wide range of pressure-temperature conditions.

Conventional electron paramagnetic resonance of Mn2+ in synthetic hydroxyapatite at different concentrations of the doped manganese

NASA Astrophysics Data System (ADS)

Murzakhanov, F.; Mamin, G.; Voloshin, A.; Klimashina, E.; Putlyaev, V.; Doronin, V.; Bakhteev, S.; Yusupov, R.; Gafurov, M.; Orlinskii, S.

2018-05-01

Powders of synthetic hydroxyapatite doped with Mn2+ ions in concentrations from 0.05 till 5 wt. % were investigated by conventional electron paramagnetic resonance (EPR). The parameters of the spin-Hamiltonian are derived. Partially resolved hyperfine structure in the magnetic fields corresponding to g ≈ 4.3 and g ≈ 9.4 is observed. The narrowing of the central peak with concentration is reported. A possibility to use the linewidth and intensity of the central peak for concentration measurements are discussed. The results could be used for the identification and qualification of Mn2+ in oil, mining and ore formations.

Calculation of the spin-polarized electronic structure of an interstitial iron impurity in silicon

NASA Astrophysics Data System (ADS)

Katayama-Yoshida, H.; Zunger, Alex

1985-06-01

We apply our self-consistent, all-electron, spin-polarized Green's-function method within an impurity-centered, dynamic basis set to study the interstitial iron impurity in silicon. We use two different formulations of the interelectron interactions: the local-spin-density (LSD) formalism and the self-interaction-corrected (SIC) local-spin-density (SIC-LSD) formalism. We find that the SIC-LSD approach is needed to obtain the correct high-spin ground state of Si:Fe+. We propose a quantitative explanation to the observed donor ionization energy and the high-spin ground states for Si:Fe+ within the SIC-LSD approach. For both Si:Fe0 and Si:Fe+, this approach leads to a hyperfine field, contact spin density, and ionization energy in better agreement with experiments than the simple LSD approach. The apparent dichotomy between the covalently delocalized nature of Si:Fe as suggested on the one hand by its reduced hyperfine field (relative to the free atom) and extended spin density and by the occurrence of two closely spaced, stable charge states (within 0.4 eV) and on the other hand by the atomically localized picture (suggested, for example, by the stability of a high-spin, ground-state configuration) is resolved. We find a large reduction in the hyperfine field and contact spin density due to the covalent hybridization between the impurity 3d orbitals and the tails of the delocalized sp3 hybrid orbitals of the surrounding silicon atoms. Using the calculated results, we discuss (i) the underlying mechanism for the stability and plurality of charged states, (ii) the covalent reduction in the hyperfine field, (iii) the remarkable constancy of the impurity Mössbauer isomer shift for different charged states, (iv) comparison with the multiple charged states in ionic crystals, and (v) some related speculation about the mechanism of (Fe2+/Fe3+) oxidation-reduction ionizations in heme proteins and electron-transporting biological systems.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chen, S. L., E-mail: shuch@ist.hokudai.ac.jp; Takayama, J.; Murayama, A.

Time-resolved optical spin orientation spectroscopy was employed to investigate the temperature-dependent electron spin injection in In{sub 0.1}Ga{sub 0.9}As quantum well (QW) and In{sub 0.5}Ga{sub 0.5}As quantum dots (QDs) tunnel-coupled nanostructures with 4, 6, and 8 nm-thick GaAs barriers. The fast picosecond-ranged spin injection from QW to QD excited states (ES) was observed to speed up with temperature, as induced by pronounced longitudinal-optical (LO)-phonon-involved multiple scattering process, which contributes to a thermally stable and almost fully spin-conserving injection within 5–180 K. The LO-phonon coupling was also found to cause accelerated electron spin relaxation of QD ES at elevated temperature, mainly via hyperfine interactionmore » with random nuclear field.« less

Self-consistent electronic structure of disordered Fe/sub 0. 65/Ni/sub 0. 35/

DOE Office of Scientific and Technical Information (OSTI.GOV)

Johnson, D.D.; Pinski, F.J.; Stocks, G.M.

1985-04-15

We present the results of the first ab initio calculation of the electronic structure of the disordered alloy Fe/sub 0.65/Ni/sub 0.35/. The calculation is based on the multiple-scattering coherent-potential approach (KKR-CPA) and is fully self-consistent and spin polarized. Magnetic effects are included within local-spin-density functional theory using the exchange-correlation function of Vosko--Wilk--Nusair. The most striking feature of the calculation is that electrons of different spins experience different degrees of disorder. The minority spin electrons see a very large disorder, whereas the majority spin electrons see little disorder. Consequently, the minority spin density of states is smooth compared to the verymore » structured majority spin density of states. This difference is due to a subtle balance between exchange splitting and charge neutrality.« less

Self-consistent electronic structure of disordered Fe/sub 0/ /sub 65/Ni/sub 0/ /sub 35/

DOE Office of Scientific and Technical Information (OSTI.GOV)

Johnson, D.D.; Pinski, F.J.; Stocks, G.M.

1984-01-01

We present the results of the first ab-initio calculation of the electronic structure of a disordered Fe/sub 0/ /sub 65/Ni/sub 0/ /sub 35/ alloy. The calculation is based on the multiple-scattering coherent-potential approach (KKR-CPA) and is fully self-consistent and spin-polarized. Magnetic effects are included within local-spin-density functional theory using the exchange-correlation function of Vosko-Wilk-Nusair. The most striking feature of the calculation is that electrons of different spins experience different degrees of disorder. The minority spin electrons see a very large disorder; whereas, the majority spin electrons see little disorder. Consequently, the minority spin density of states is smooth compared tomore » the very structured majority spin density of states. This difference is due to a subtle balance between exchange-splitting and charge neutrality. 15 references, 2 figures.« less

Electron spin relaxation in two polymorphic structures of GaN

NASA Astrophysics Data System (ADS)

Kang, Nam Lyong

2015-03-01

The relaxation process of electron spin in systems of electrons interacting with piezoelectric deformation phonons that are mediated through spin-orbit interactions was interpreted from a microscopic point of view using the formula for the electron spin relaxation times derived by a projection-reduction method. The electron spin relaxation times in two polymorphic structures of GaN were calculated. The piezoelectric material constant for the wurtzite structure obtained by a comparison with a previously reported experimental result was {{P}pe}=1.5 × {{10}29} eV {{m}-1}. The temperature and magnetic field dependence of the relaxation times for both wurtzite and zinc-blende structures were similar, but the relaxation times in zinc-blende GaN were smaller and decreased more rapidly with increasing temperature and magnetic field than that in wurtzite GaN. This study also showed that the electron spin relaxation for wurtzite GaN at low density could be explained by the Elliot-Yafet process but not for zinc-blende GaN in the metallic regime.

Non-Markovian spin-resolved counting statistics and an anomalous relation between autocorrelations and cross correlations in a three-terminal quantum dot

NASA Astrophysics Data System (ADS)

Luo, JunYan; Yan, Yiying; Huang, Yixiao; Yu, Li; He, Xiao-Ling; Jiao, HuJun

2017-01-01

We investigate the noise correlations of spin and charge currents through an electron spin resonance (ESR)-pumped quantum dot, which is tunnel coupled to three electrodes maintained at an equivalent chemical potential. A recursive scheme is employed with inclusion of the spin degrees of freedom to account for the spin-resolved counting statistics in the presence of non-Markovian effects due to coupling with a dissipative heat bath. For symmetric spin-up and spin-down tunneling rates, an ESR-induced spin flip mechanism generates a pure spin current without an accompanying net charge current. The stochastic tunneling of spin carriers, however, produces universal shot noises of both charge and spin currents, revealing the effective charge and spin units of quasiparticles in transport. In the case of very asymmetric tunneling rates for opposite spins, an anomalous relationship between noise autocorrelations and cross correlations is revealed, where super-Poissonian autocorrelation is observed in spite of a negative cross correlation. Remarkably, with strong dissipation strength, non-Markovian memory effects give rise to a positive cross correlation of the charge current in the absence of a super-Poissonian autocorrelation. These unique noise features may offer essential methods for exploiting internal spin dynamics and various quasiparticle tunneling processes in mesoscopic transport.

Spin-vibronic quantum dynamics for ultrafast excited-state processes.

PubMed

Eng, Julien; Gourlaouen, Christophe; Gindensperger, Etienne; Daniel, Chantal

2015-03-17

Ultrafast intersystem crossing (ISC) processes coupled to nuclear relaxation and solvation dynamics play a central role in the photophysics and photochemistry of a wide range of transition metal complexes. These phenomena occurring within a few hundred femtoseconds are investigated experimentally by ultrafast picosecond and femtosecond transient absorption or luminescence spectroscopies, and optical laser pump-X-ray probe techniques using picosecond and femtosecond X-ray pulses. The interpretation of ultrafast structural changes, time-resolved spectra, quantum yields, and time scales of elementary processes or transient lifetimes needs robust theoretical tools combining state-of-the-art quantum chemistry and developments in quantum dynamics for solving the electronic and nuclear problems. Multimode molecular dynamics beyond the Born-Oppenheimer approximation has been successfully applied to many small polyatomic systems. Its application to large molecules containing a transition metal atom is still a challenge because of the nuclear dimensionality of the problem, the high density of electronic excited states, and the spin-orbit coupling effects. Rhenium(I) α-diimine carbonyl complexes, [Re(L)(CO)3(N,N)](n+) are thermally and photochemically robust and highly flexible synthetically. Structural variations of the N,N and L ligands affect the spectroscopy, the photophysics, and the photochemistry of these chromophores easily incorporated into a complex environment. Visible light absorption opens the route to a wide range of applications such as sensors, probes, or emissive labels for imaging biomolecules. Halide complexes [Re(X)(CO)3(bpy)] (X = Cl, Br, or I; bpy = 2,2'-bipyridine) exhibit complex electronic structure and large spin-orbit effects that do not correlate with the heavy atom effects. Indeed, the (1)MLCT → (3)MLCT intersystem crossing (ISC) kinetics is slower than in [Ru(bpy)3](2+) or [Fe(bpy)3](2+) despite the presence of a third-row transition metal. Counterintuitively, singlet excited-state lifetime increases on going from Cl (85 fs) to Br (128 fs) and to I (152 fs). Moreover, correlation between the Re-X stretching mode and the rate of ISC is observed. In this Account, we emphasize on the role of spin-vibronic coupling on the mechanism of ultrafast ISC put in evidence in [Re(Br)(CO)3(bpy)]. For this purpose, we have developed a model Hamiltonian for solving an 11 electronic excited states multimode problem including vibronic and SO coupling within the linear vibronic coupling (LVC) approximation and the assumption of harmonic potentials. The presence of a central metal atom coupled to rigid ligands, such as α-diimine, ensures nuclear motion of small amplitudes and a priori justifies the use of the LVC model. The simulation of the ultrafast dynamics by wavepacket propagations using the multiconfiguration time-dependent Hartree (MCTDH) method is based on density functional theory (DFT), and its time-dependent extension to excited states (TD-DFT) electronic structure data. We believe that the interplay between time-resolved experiments and these pioneering simulations covering the first picoseconds and including spin-vibronic coupling will promote a number of quantum dynamical studies that will contribute to a better understanding of ultrafast processes in a wide range of organic and inorganic chromophores easily incorporated in biosystems or supramolecular devices for specific functions.

Spin-orbit coupling, electron transport and pairing instabilities in two-dimensional square structures

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kocharian, Armen N.; Fernando, Gayanath W.; Fang, Kun

Rashba spin-orbit effects and electron correlations in the two-dimensional cylindrical lattices of square geometries are assessed using mesoscopic two-, three- and four-leg ladder structures. Here the electron transport properties are systematically calculated by including the spin-orbit coupling in tight binding and Hubbard models threaded by a magnetic flux. These results highlight important aspects of possible symmetry breaking mechanisms in square ladder geometries driven by the combined effect of a magnetic gauge field spin-orbit interaction and temperature. The observed persistent current, spin and charge polarizations in the presence of spin-orbit coupling are driven by separation of electron and hole charges andmore » opposite spins in real-space. The modeled spin-flip processes on the pairing mechanism induced by the spin-orbit coupling in assembled nanostructures (as arrays of clusters) engineered in various two-dimensional multi-leg structures provide an ideal playground for understanding spatial charge and spin density inhomogeneities leading to electron pairing and spontaneous phase separation instabilities in unconventional superconductors. Such studies also fall under the scope of current challenging problems in superconductivity and magnetism, topological insulators and spin dependent transport associated with numerous interfaces and heterostructures.« less

Spin-resolved photoemission study of epitaxially grown MoSe 2 and WSe 2 thin films

DOE PAGES

Mo, Sung-Kwan; Hwang, Choongyu; Zhang, Yi; ...

2016-09-12

Few-layer thick MoSe 2 and WSe 2 possess non-trivial spin textures with sizable spin splitting due to the inversion symmetry breaking embedded in the crystal structure and strong spin–orbit coupling. Here, we report a spin-resolved photoemission study of MoSe 2 and WSe 2 thin film samples epitaxially grown on a bilayer graphene substrate. Furthermore, we only found spin polarization in the single- and trilayer samples—not in the bilayer sample—mostly along the out-of-plane direction of the sample surface. The measured spin polarization is found to be strongly dependent on the light polarization as well as the measurement geometry, which reveals intricatemore » coupling between the spin and orbital degrees of freedom in this class of material.« less

Quantum interference measurement of spin interactions in a bio-organic/semiconductor device structure

DOE PAGES

Deo, Vincent; Zhang, Yao; Soghomonian, Victoria; ...

2015-03-30

Quantum interference is used to measure the spin interactions between an InAs surface electron system and the iron center in the biomolecule hemin in nanometer proximity in a bio-organic/semiconductor device structure. The interference quantifies the influence of hemin on the spin decoherence properties of the surface electrons. The decoherence times of the electrons serve to characterize the biomolecule, in an electronic complement to the use of spin decoherence times in magnetic resonance. Hemin, prototypical for the heme group in hemoglobin, is used to demonstrate the method, as a representative biomolecule where the spin state of a metal ion affects biologicalmore » functions. The electronic determination of spin decoherence properties relies on the quantum correction of antilocalization, a result of quantum interference in the electron system. Spin-flip scattering is found to increase with temperature due to hemin, signifying a spin exchange between the iron center and the electrons, thus implying interactions between a biomolecule and a solid-state system in the hemin/InAs hybrid structure. The results also indicate the feasibility of artificial bioinspired materials using tunable carrier systems to mediate interactions between biological entities.« less

Low-lying vibronic level structure of the ground state of the methoxy radical: Slow electron velocity-map imaging (SEVI) spectra and Köppel-Domcke-Cederbaum (KDC) vibronic Hamiltonian calculations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Weichman, Marissa L.; Cheng, Lan; Kim, Jongjin B.

A joint experimental and theoretical study is reported on the low-lying vibronic level structure of the ground state of the methoxy radical using slow photoelectron velocity-map imaging spectroscopy of cryogenically cooled, mass-selected anions (cryo-SEVI) and Köppel-Domcke-Cederbaum (KDC) vibronic Hamiltonian calculations. The KDC vibronic model Hamiltonian in the present study was parametrized using high-level quantum chemistry, allowing the assignment of the cryo-SEVI spectra for vibronic levels of CH 3O up to 2000 cm –1 and of CD 3O up to 1500 cm –1 above the vibrational origin, using calculated vibronic wave functions. The adiabatic electron affinities of CH 3O and CDmore » 3O are determined from the cryo-SEVI spectra to be 1.5689 ± 0.0007 eV and 1.5548 ± 0.0007 eV, respectively, demonstrating improved precision compared to previous work. Experimental peak splittings of <10 cm –1 are resolved between the e 1/2 and e 3/2 components of the 6 1 and 5 1 vibronic levels. A pair of spin-vibronic levels at 1638 and 1677 cm –1 were predicted in the calculation as the e 1/2 and e 3/2 components of 6 2 levels and experimentally resolved for the first time. The strong variation of the spin-orbit splittings with a vibrational quantum number is in excellent agreement between theory and experiment. In conclusion, the observation of signals from nominally forbidden a 1 vibronic levels in the cryo-SEVI spectra also provides direct evidence of vibronic coupling between ground and electronically excited states of methoxy.« less

Low-lying vibronic level structure of the ground state of the methoxy radical: Slow electron velocity-map imaging (SEVI) spectra and Köppel-Domcke-Cederbaum (KDC) vibronic Hamiltonian calculations

DOE PAGES

Weichman, Marissa L.; Cheng, Lan; Kim, Jongjin B.; ...

2017-06-12

A joint experimental and theoretical study is reported on the low-lying vibronic level structure of the ground state of the methoxy radical using slow photoelectron velocity-map imaging spectroscopy of cryogenically cooled, mass-selected anions (cryo-SEVI) and Köppel-Domcke-Cederbaum (KDC) vibronic Hamiltonian calculations. The KDC vibronic model Hamiltonian in the present study was parametrized using high-level quantum chemistry, allowing the assignment of the cryo-SEVI spectra for vibronic levels of CH 3O up to 2000 cm –1 and of CD 3O up to 1500 cm –1 above the vibrational origin, using calculated vibronic wave functions. The adiabatic electron affinities of CH 3O and CDmore » 3O are determined from the cryo-SEVI spectra to be 1.5689 ± 0.0007 eV and 1.5548 ± 0.0007 eV, respectively, demonstrating improved precision compared to previous work. Experimental peak splittings of <10 cm –1 are resolved between the e 1/2 and e 3/2 components of the 6 1 and 5 1 vibronic levels. A pair of spin-vibronic levels at 1638 and 1677 cm –1 were predicted in the calculation as the e 1/2 and e 3/2 components of 6 2 levels and experimentally resolved for the first time. The strong variation of the spin-orbit splittings with a vibrational quantum number is in excellent agreement between theory and experiment. In conclusion, the observation of signals from nominally forbidden a 1 vibronic levels in the cryo-SEVI spectra also provides direct evidence of vibronic coupling between ground and electronically excited states of methoxy.« less

A single-atom quantum memory in silicon

DOE Office of Scientific and Technical Information (OSTI.GOV)

Freer, Solomon; Simmons, Stephanie; Laucht, Arne

Long coherence times and fast gate operations are desirable but often conflicting requirements for physical qubits. This conflict can be resolved by resorting to fast qubits for operations, and by storing their state in a ‘quantum memory’ while idle. The 31P donor in silicon comes naturally equipped with a fast qubit (the electron spin) and a long-lived qubit (the 31P nuclear spin), coexisting in a bound state at cryogenic temperatures. Here, we demonstrate storage and retrieval of quantum information from a single donor electron spin to its host phosphorus nucleus in isotopically-enriched 28Si. The fidelity of the memory process ismore » characterised via both state and process tomography. We report an overall process fidelity Fp ! 81%, a memory fidelity Fm ! 92%, and memory storage times up to 80 ms. These values are limited by a transient shift of the electron spin resonance frequency following highpower radiofrequency pulses.« less

A single-atom quantum memory in silicon

DOE PAGES

Freer, Solomon; Simmons, Stephanie; Laucht, Arne; ...

2017-03-20

Long coherence times and fast gate operations are desirable but often conflicting requirements for physical qubits. This conflict can be resolved by resorting to fast qubits for operations, and by storing their state in a ‘quantum memory’ while idle. The 31P donor in silicon comes naturally equipped with a fast qubit (the electron spin) and a long-lived qubit (the 31P nuclear spin), coexisting in a bound state at cryogenic temperatures. Here, we demonstrate storage and retrieval of quantum information from a single donor electron spin to its host phosphorus nucleus in isotopically-enriched 28Si. The fidelity of the memory process ismore » characterised via both state and process tomography. We report an overall process fidelity Fp ! 81%, a memory fidelity Fm ! 92%, and memory storage times up to 80 ms. These values are limited by a transient shift of the electron spin resonance frequency following highpower radiofrequency pulses.« less

New developments in laser-based photoemission spectroscopy and its scientific applications: a key issues review

NASA Astrophysics Data System (ADS)

Zhou, Xingjiang; He, Shaolong; Liu, Guodong; Zhao, Lin; Yu, Li; Zhang, Wentao

2018-06-01

The significant progress in angle-resolved photoemission spectroscopy (ARPES) in last three decades has elevated it from a traditional band mapping tool to a precise probe of many-body interactions and dynamics of quasiparticles in complex quantum systems. The recent developments of deep ultraviolet (DUV, including ultraviolet and vacuum ultraviolet) laser-based ARPES have further pushed this technique to a new level. In this paper, we review some latest developments in DUV laser-based photoemission systems, including the super-high energy and momentum resolution ARPES, the spin-resolved ARPES, the time-of-flight ARPES, and the time-resolved ARPES. We also highlight some scientific applications in the study of electronic structure in unconventional superconductors and topological materials using these state-of-the-art DUV laser-based ARPES. Finally we provide our perspectives on the future directions in the development of laser-based photoemission systems.

Modeling of the N-terminal Section and the Lumenal Loop of Trimeric Light Harvesting Complex II (LHCII) by Using EPR*

PubMed Central

Fehr, Niklas; Dietz, Carsten; Polyhach, Yevhen; von Hagens, Tona; Jeschke, Gunnar; Paulsen, Harald

2015-01-01

The major light harvesting complex II (LHCII) of green plants plays a key role in the absorption of sunlight, the regulation of photosynthesis, and in preventing photodamage by excess light. The latter two functions are thought to involve the lumenal loop and the N-terminal domain. Their structure and mobility in an aqueous environment are only partially known. Electron paramagnetic resonance (EPR) has been used to measure the structure of these hydrophilic protein domains in detergent-solubilized LHCII. A new technique is introduced to prepare LHCII trimers in which only one monomer is spin-labeled. These heterogeneous trimers allow to measure intra-molecular distances within one LHCII monomer in the context of a trimer by using double electron-electron resonance (DEER). These data together with data from electron spin echo envelope modulation (ESEEM) allowed to model the N-terminal protein section, which has not been resolved in current crystal structures, and the lumenal loop domain. The N-terminal domain covers only a restricted area above the superhelix in LHCII, which is consistent with the “Velcro” hypothesis to explain thylakoid grana stacking (Standfuss, J., van Terwisscha Scheltinga, A. C., Lamborghini, M., and Kühlbrandt, W. (2005) EMBO J. 24, 919–928). The conformation of the lumenal loop domain is surprisingly different between LHCII monomers and trimers but not between complexes with and without neoxanthin bound. PMID:26316535

Spectroscopic characterization of III-V semiconductor nanomaterials

NASA Astrophysics Data System (ADS)

Crankshaw, Shanna Marie

III-V semiconductor materials form a broad basis for optoelectronic applications, including the broad basis of the telecom industry as well as smaller markets for high-mobility transistors. In a somewhat analogous manner as the traditional silicon logic industry has so heavily depended upon process manufacturing development, optoelectronics often relies instead on materials innovations. This thesis focuses particularly on III-V semiconductor nanomaterials, detailed characterization of which is invaluable for translating the exhibited behavior into useful applications. Specifically, the original research described in these thesis chapters is an investigation of semiconductors at a fundamental materials level, because the nanostructures in which they appear crystallize in quite atypical forms for the given semiconductors. Rather than restricting the experimental approaches to any one particular technique, many different types of optical spectroscopies are developed and applied where relevant to elucidate the connection between the crystalline structure and exhibited properties. In the first chapters, for example, a wurtzite crystalline form of the prototypical zincblende III-V binary semiconductor, GaAs, is explored through polarization-dependent Raman spectroscopy and temperature-dependent photoluminescence, as well as second-harmonic generation (SHG). The altered symmetry properties of the wurtzite crystalline structure are particularly evident in the Raman and SHG polarization dependences, all within a bulk material realm. A rather different but deeply elegant aspect of crystalline symmetry in GaAs is explored in a separate study on zincblende GaAs samples quantum-confined in one direction, i.e. quantum well structures, whose quantization direction corresponds to the (110) direction. The (110) orientation modifies the low-temperature electron spin relaxation mechanisms available compared to the usual (001) samples, leading to altered spin coherence times explored through a novel spectroscopic technique first formulated for the rather different purpose of dispersion engineering for slow-light schemes. The frequency-resolved technique combined with the unusual (110) quantum wells in a furthermore atypical waveguide experimental geometry has revealed fascinating behavior of electron spin splitting which points to the possibility of optically orienting electron spins with linearly polarized light---an experimental result supporting a theoretical description of the phenomenon itself only a few years old. Lastly, to explore a space of further-restricted dimensionality, the final chapters describe InP semiconductor nanowires with dimensions small enough to be considered truly one-dimensional. Like the bulk GaAs of the first few chapters, the InP nanowires here crystallize in a wurtzite structure. In the InP nanowire case, though, the experimental techniques explored for characterization are temperature-dependent time-integrated photoluminescence at the single-wire level (including samples with InAsP insertions) and time-resolved photoluminescence at the ensemble level. The carrier dynamics revealed through these time-resolved studies are the first of their kind for wurtzite InP nanowires. The chapters are thus ordered as a progression from three (bulk), to two (quantum well), to one (nanowire), to zero dimensions (axially-structured nanowire), with the uniting theme the emphasis on connecting the semiconductor nanomaterials' crystallinity to its exhibited properties by relevant experimental spectroscopic techniques, whether these are standard methods or effectively invented for the case at hand.

Equal-Spin Andreev Reflection on Junctions of Spin-Resolved Quantum Hall Bulk State and Spin-Singlet Superconductor.

PubMed

Matsuo, Sadashige; Ueda, Kento; Baba, Shoji; Kamata, Hiroshi; Tateno, Mizuki; Shabani, Javad; Palmstrøm, Christopher J; Tarucha, Seigo

2018-02-22

The recent development of superconducting spintronics has revealed the spin-triplet superconducting proximity effect from a spin-singlet superconductor into a spin-polarized normal metal. In addition recently superconducting junctions using semiconductors are in demand for highly controlled experiments to engineer topological superconductivity. Here we report experimental observation of Andreev reflection in junctions of spin-resolved quantum Hall (QH) states in an InAs quantum well and the spin-singlet superconductor NbTi. The measured conductance indicates a sub-gap feature and two peaks on the outer side of the sub-gap feature in the QH plateau-transition regime increases. The observed structures can be explained by considering transport with Andreev reflection from two channels, one originating from equal-spin Andreev reflection intermediated by spin-flip processes and second arising from normal Andreev reflection. This result indicates the possibility to induce the superconducting proximity gap in the the QH bulk state, and the possibility for the development of superconducting spintronics in semiconductor devices.

Hallmarks of Hunds coupling in the Mott insulator Ca2RuO4

PubMed Central

Sutter, D.; Fatuzzo, C. G.; Moser, S.; Kim, M.; Fittipaldi, R.; Vecchione, A.; Granata, V.; Sassa, Y.; Cossalter, F.; Gatti, G.; Grioni, M.; Rønnow, H. M.; Plumb, N. C.; Matt, C. E.; Shi, M.; Hoesch, M.; Kim, T. K.; Chang, T-R; Jeng, H-T; Jozwiak, C.; Bostwick, A.; Rotenberg, E.; Georges, A.; Neupert, T.; Chang, J.

2017-01-01

A paradigmatic case of multi-band Mott physics including spin-orbit and Hund's coupling is realized in Ca2RuO4. Progress in understanding the nature of this Mott insulating phase has been impeded by the lack of knowledge about the low-energy electronic structure. Here we provide—using angle-resolved photoemission electron spectroscopy—the band structure of the paramagnetic insulating phase of Ca2RuO4 and show how it features several distinct energy scales. Comparison to a simple analysis of atomic multiplets provides a quantitative estimate of the Hund's coupling J=0.4 eV. Furthermore, the experimental spectra are in good agreement with electronic structure calculations performed with Dynamical Mean-Field Theory. The crystal field stabilization of the dxy orbital due to c-axis contraction is shown to be essential to explain the insulating phase. These results underscore the importance of multi-band physics, Coulomb interaction and Hund's coupling that together generate the Mott insulating state of Ca2RuO4. PMID:28474681

The millimeter and submillimeter rotational spectrum of the MgCN radical (X (sup 2) Sigma(+))

NASA Technical Reports Server (NTRS)

Anderson, M. A.; Steimle, T. C.; Ziurys, L. M.

1994-01-01

The pure rotational spectrum of the MgCN radical has been recorded in the laboratory using millimeter/submillimeter direct absorption spectroscopy. Twenty-seven rotational transitions of the species were observed in the range 101-376 GHz and indicate that the molecule is linear with a (sup 2)Sigma(+) ground electronic state, as predicted by theory. Spin rotation interactions were resolved in the spectra, but no hyperfine splittings were observed, which would originate with the nitrogen nuclear spin. The rotational and fine-structure constants were determined for this radical from a nonlinear least-squares fit to the data using a (sup 2)Sigma Hamiltonian. MgCN is of astrophysical interest because it is the metastable isomer of MgNC, which recently has been detected toward IRC +10216

Laser angle-resolved photoemission as a probe of initial state k z dispersion, final-state band gaps, and spin texture of Dirac states in the Bi 2Te 3 topological insulator

DOE PAGES

Ärrälä, Minna; Hafiz, Hasnain; Mou, Daixiang; ...

2016-10-27

Here, we have obtained angle-resolved photoemission (ARPES) spectra from single crystals of the topological insulator material Bi 2Te 3 using tunable laser spectrometer. The spectra were collected for eleven different photon energies ranging from 5.57 to 6.70 eV for incident light polarized linearly along two different in-plane directions. Parallel first-principles, fully relativistic computations of photo-intensities were carried out using the experimental geometry within the framework of the one-step model of photoemission. Good overall accord between theory and experiment is used to gain insight into how properties of the initial and final state band structures as well as those of themore » topological surface states and their spin-textures are reflected in the laser-ARPES spectra. In conclusion, our analysis reveals that laser-ARPES is sensitive to both the initial state k z dispersion and the presence of delicate gaps in the final state electronic spectrum.« less

Maximal Rashba-like spin splitting via kinetic-energy-coupled inversion-symmetry breaking

NASA Astrophysics Data System (ADS)

Sunko, Veronika; Rosner, H.; Kushwaha, P.; Khim, S.; Mazzola, F.; Bawden, L.; Clark, O. J.; Riley, J. M.; Kasinathan, D.; Haverkort, M. W.; Kim, T. K.; Hoesch, M.; Fujii, J.; Vobornik, I.; MacKenzie, A. P.; King, P. D. C.

2017-09-01

Engineering and enhancing the breaking of inversion symmetry in solids—that is, allowing electrons to differentiate between ‘up’ and ‘down’—is a key goal in condensed-matter physics and materials science because it can be used to stabilize states that are of fundamental interest and also have potential practical applications. Examples include improved ferroelectrics for memory devices and materials that host Majorana zero modes for quantum computing. Although inversion symmetry is naturally broken in several crystalline environments, such as at surfaces and interfaces, maximizing the influence of this effect on the electronic states of interest remains a challenge. Here we present a mechanism for realizing a much larger coupling of inversion-symmetry breaking to itinerant surface electrons than is typically achieved. The key element is a pronounced asymmetry of surface hopping energies—that is, a kinetic-energy-coupled inversion-symmetry breaking, the energy scale of which is a substantial fraction of the bandwidth. Using spin- and angle-resolved photoemission spectroscopy, we demonstrate that such a strong inversion-symmetry breaking, when combined with spin-orbit interactions, can mediate Rashba-like spin splittings that are much larger than would typically be expected. The energy scale of the inversion-symmetry breaking that we achieve is so large that the spin splitting in the CoO2- and RhO2-derived surface states of delafossite oxides becomes controlled by the full atomic spin-orbit coupling of the 3d and 4d transition metals, resulting in some of the largest known Rashba-like spin splittings. The core structural building blocks that facilitate the bandwidth-scaled inversion-symmetry breaking are common to numerous materials. Our findings therefore provide opportunities for creating spin-textured states and suggest routes to interfacial control of inversion-symmetry breaking in designer heterostructures of oxides and other material classes.

Interaction of proflavin with aromatic amines in homogeneous and micellar media: Photoinduced electron transfer probed by magnetic field effect

NASA Astrophysics Data System (ADS)

Chakraborty, Brotati; Basu, Samita

2010-02-01

Photoinduced electron transfer (PET) between proflavin (PF +) and two aromatic amines viz., dimethylaniline (DMA) and 4,4'-bis(dimethylamino)diphenylmethane (DMDPM) is studied in homogeneous and heterogeneous media using steady-state as well as time-resolved fluorescence spectroscopy and laser flash photolysis with an associated magnetic field. Ionic micelles have been used to study the effect of charge of proflavin on PET with amines. Magnetic field effect on PET reactions reveals that the parent spin-state of precursors of PET for DMA-PF + system is singlet while for DMDPM-PF + system is triplet, implying that the dynamics of PET is influenced by the structure of the donor.

Persistent Charge-Density-Wave Order in Single-Layer TaSe2.

PubMed

Ryu, Hyejin; Chen, Yi; Kim, Heejung; Tsai, Hsin-Zon; Tang, Shujie; Jiang, Juan; Liou, Franklin; Kahn, Salman; Jia, Caihong; Omrani, Arash A; Shim, Ji Hoon; Hussain, Zahid; Shen, Zhi-Xun; Kim, Kyoo; Min, Byung Il; Hwang, Choongyu; Crommie, Michael F; Mo, Sung-Kwan

2018-02-14

We present the electronic characterization of single-layer 1H-TaSe 2 grown by molecular beam epitaxy using a combined angle-resolved photoemission spectroscopy, scanning tunneling microscopy/spectroscopy, and density functional theory calculations. We demonstrate that 3 × 3 charge-density-wave (CDW) order persists despite distinct changes in the low energy electronic structure highlighted by the reduction in the number of bands crossing the Fermi energy and the corresponding modification of Fermi surface topology. Enhanced spin-orbit coupling and lattice distortion in the single-layer play a crucial role in the formation of CDW order. Our findings provide a deeper understanding of the nature of CDW order in the two-dimensional limit.

Imaging of surface spin textures on bulk crystals by scanning electron microscopy

NASA Astrophysics Data System (ADS)

Akamine, Hiroshi; Okumura, So; Farjami, Sahar; Murakami, Yasukazu; Nishida, Minoru

2016-11-01

Direct observation of magnetic microstructures is vital for advancing spintronics and other technologies. Here we report a method for imaging surface domain structures on bulk samples by scanning electron microscopy (SEM). Complex magnetic domains, referred to as the maze state in CoPt/FePt alloys, were observed at a spatial resolution of less than 100 nm by using an in-lens annular detector. The method allows for imaging almost all the domain walls in the mazy structure, whereas the visualisation of the domain walls with the classical SEM method was limited. Our method provides a simple way to analyse surface domain structures in the bulk state that can be used in combination with SEM functions such as orientation or composition analysis. Thus, the method extends applications of SEM-based magnetic imaging, and is promising for resolving various problems at the forefront of fields including physics, magnetics, materials science, engineering, and chemistry.

Angle-resolved photoemission spectroscopy studies of metallic surface and interface states of oxide insulators

NASA Astrophysics Data System (ADS)

Plumb, Nicholas C.; Radović, Milan

2017-11-01

Over the last decade, conducting states embedded in insulating transition metal oxides (TMOs) have served as gateways to discovering and probing surprising phenomena that can emerge in complex oxides, while also opening opportunities for engineering advanced devices. These states are commonly realized at thin film interfaces, such as the well-known case of LaAlO3 (LAO) grown on SrTiO3 (STO). In recent years, the use of angle-resolved photoemission spectroscopy (ARPES) to investigate the k-space electronic structure of such materials led to the discovery that metallic states can also be formed on the bare surfaces of certain TMOs. In this topical review, we report on recent studies of low-dimensional metallic states confined at insulating oxide surfaces and interfaces as seen from the perspective of ARPES, which provides a direct view of the occupied band structure. While offering a fairly broad survey of progress in the field, we draw particular attention to STO, whose surface is so far the best-studied, and whose electronic structure is probably of the most immediate interest, given the ubiquitous use of STO substrates as the basis for conducting oxide interfaces. The ARPES studies provide crucial insights into the electronic band structure, orbital character, dimensionality/confinement, spin structure, and collective excitations in STO surfaces and related oxide surface/interface systems. The obtained knowledge increases our understanding of these complex materials and gives new perspectives on how to manipulate their properties.

Direct measurement of ferromagnetic ordering in biaxially strained LaCoO3 thin films

NASA Astrophysics Data System (ADS)

Klie, R. F.; Yuan, T.; Tanase, M.; Yang, G.; Ramasse, Q.

2010-02-01

LaCoO3 undergoes a transition from a nonmagnetic to a paramagnetic semiconductor at 80 K, associated with a spin-state transition of the Co3+ ions. It was proposed that the temperature of the spin-state transition depends strongly on the LaCoO3 lattice parameter, suggesting that strain can stabilize different spin states at different temperatures. By combining atomic-resolution Z-contrast imaging, electron diffraction, and angular-resolved electron energy-loss spectroscopy (EELS) with in situ cooling experiments, we show that epitaxially strained LaCoO3 (001) thin films grown on LaAlO3 (001) do not undergo a low temperature spin-state transition. Our EELS study explores the origins of the ferromagnetic ordering in strained LaCoO3 films.

The pure rotational spectrum of TiF (X 4Φr): 3d transition metal fluorides revisited

NASA Astrophysics Data System (ADS)

Sheridan, P. M.; McLamarrah, S. K.; Ziurys, L. M.

2003-11-01

The pure rotational spectrum of TiF in its X 4Φr (v=0) ground state has been measured using millimeter/sub-millimeter wave direct absorption techniques in the range 140-530 GHz. In ten out of the twelve rotational transitions recorded, all four spin-orbit components were observed, confirming the 4Φr ground state assignment. Additional small splittings were resolved in several of the spin components in lower J transitions, which appear to arise from magnetic hyperfine interactions of the 19F nucleus. In contrast, no evidence for Λ-doubling was seen in the data. The rotational transitions of TiF were analyzed using a case (a) Hamiltonian, resulting in the determination of rotational and fine structure constants, as well as hyperfine parameters for the fluorine nucleus. The data were readily fit in a case (a) basis, indicating strong first order spin-orbit coupling and minimal second-order effects, as also evidenced by the small value of λ, the spin-spin parameter. Moreover, only one higher order term, η, the spin-orbit/spin-spin interaction term, was needed in the analysis, again suggesting limited perturbations in the ground state. The relative values of the a, b, and c hyperfine constants indicate that the three unpaired electrons in this radical lie in orbitals primarily located on the titanium atom and support the molecular orbital picture of TiF with a σ1δ1π1 single electron configuration. The bond length of TiF (1.8342 Å) is significantly longer than that of TiO, suggesting that there are differences in the bonding between 3d transition metal fluorides and oxides.

Momentum space view of the ultrafast dynamics of surface photocurrents on topological insulators

NASA Astrophysics Data System (ADS)

Kuroda, K.; Reimann, J.; Güdde, J.; Höfer, U.

2017-02-01

The Dirac-cone surface states of topological insulators are characterized by a chiral spin texture in k-space with the electron spin locked to its parallel momentum. Mid-infrared pump pulses can induce spin-polarized photocurrents in such a topological surface state by optical transitions between the occupied and unoccupied part of the Dirac cone. We monitor the ultrafast dynamics of the corresponding asymmetric electron population in momentum space directly by time- and angle-resolved two-photon photoemission (2PPE). The elastic scattering times of 2.5 ps deduced for Sb2Te3 corresponds to a mean-fee path of 0.75 μm in real space.

(Charge separation in photoredox reactions). Informal annual technical progress report, October 1, 1981-October 1, 1982. [N,N,N',N'tetramethylbenzidine

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kevan, L.

1982-10-21

During this period work has focused on the structural aspects of photoinduced charge separation in micellar media with initial forays into vesicular media. The primary techniques utilized are electron spin resonance and electron spin echo spectrometry. The analysis of electron spin echo modulation gives a unique handle on very weak hyperfine interactions thus providing a new structural tool for this general problem. Electron spin resonance and electron spin echo studies of the photoionization of N,N,N',N'tetramethylbenzidine (TMB) to give the cation radical have been carried out in anionic, cationic and nonionic micellar solutions frozen to 77/sup 0/K. The photoionization efficiency ofmore » TMB has also been studied in micelles with varying alkyl chain lengths of the surfactant. Stearic acid nitroxide spin probes have also been used to determine some structural aspects of the location of the neutral TMB molecule in anionic micelles before photoionization. The nitroxide work in which the nitroxide is acting as an electron acceptor also shows that a suitable electron acceptor can be located within the micellar structure. The effect of inorganic solutes on the efficiency of the photoionization of TMB in frozen micelles has also been studied. A series of electron scavenger studies have been initiated to study the effect on TMB photoionization efficiency. Electron spin echo detection of laser photogenerated TMB cation in liquid sodium dodecyl sulfate solutions at room temperature has recently been observed.« less

Adiabatic quantum computing with spin qubits hosted by molecules.

PubMed

Yamamoto, Satoru; Nakazawa, Shigeaki; Sugisaki, Kenji; Sato, Kazunobu; Toyota, Kazuo; Shiomi, Daisuke; Takui, Takeji

2015-01-28

A molecular spin quantum computer (MSQC) requires electron spin qubits, which pulse-based electron spin/magnetic resonance (ESR/MR) techniques can afford to manipulate for implementing quantum gate operations in open shell molecular entities. Importantly, nuclear spins, which are topologically connected, particularly in organic molecular spin systems, are client qubits, while electron spins play a role of bus qubits. Here, we introduce the implementation for an adiabatic quantum algorithm, suggesting the possible utilization of molecular spins with optimized spin structures for MSQCs. We exemplify the utilization of an adiabatic factorization problem of 21, compared with the corresponding nuclear magnetic resonance (NMR) case. Two molecular spins are selected: one is a molecular spin composed of three exchange-coupled electrons as electron-only qubits and the other an electron-bus qubit with two client nuclear spin qubits. Their electronic spin structures are well characterized in terms of the quantum mechanical behaviour in the spin Hamiltonian. The implementation of adiabatic quantum computing/computation (AQC) has, for the first time, been achieved by establishing ESR/MR pulse sequences for effective spin Hamiltonians in a fully controlled manner of spin manipulation. The conquered pulse sequences have been compared with the NMR experiments and shown much faster CPU times corresponding to the interaction strength between the spins. Significant differences are shown in rotational operations and pulse intervals for ESR/MR operations. As a result, we suggest the advantages and possible utilization of the time-evolution based AQC approach for molecular spin quantum computers and molecular spin quantum simulators underlain by sophisticated ESR/MR pulsed spin technology.

The Electronic Structure Signature of the Spin Cross-Over Transition of [Co(dpzca)2

NASA Astrophysics Data System (ADS)

Zhang, Xin; Mu, Sai; Liu, Yang; Luo, Jian; Zhang, Jian; N'Diaye, Alpha T.; Enders, Axel; Dowben, Peter A.

2018-05-01

The unoccupied electronic structure of the spin crossover molecule cobalt (II) N-(2-pyrazylcarbonyl)-2-pyrazinecarboxamide, [Co(dpzca)2] was investigated, using X-ray absorption spectroscopy (XAS) and compared with magnetometry (SQUID) measurements. The temperature dependence of the XAS and molecular magnetic susceptibility χmT are in general agreement for [Co(dpzca)2], and consistent with density functional theory (DFT). This agreement of magnetic susceptibility and X-ray absorption spectroscopy provides strong evidence that the changes in magnetic moment can be ascribed to changes in electronic structure. Calculations show the choice of Coulomb correlation energy U has a profound effect on the electronic structure of the low spin state, but has little influence on the electronic structure of the high spin state. In the temperature dependence of the XAS, there is also evidence of an X-ray induced excited state trapping for [Co(dpzca)2] at 15 K.

The electron-spin--nuclear-spin interaction studied by polarized neutron scattering.

PubMed

Stuhrmann, Heinrich B

2007-11-01

Dynamic nuclear spin polarization (DNP) is mediated by the dipolar interaction of paramagnetic centres with nuclear spins. This process is most likely to occur near paramagnetic centres at an angle close to 45 degrees with respect to the direction of the external magnetic field. The resulting distribution of polarized nuclear spins leads to an anisotropy of the polarized neutron scattering pattern, even with randomly oriented radical molecules. The corresponding cross section of polarized coherent neutron scattering in terms of a multipole expansion is derived for radical molecules in solution. An application using data of time-resolved polarized neutron scattering from an organic chromium(V) molecule is tested.

Spin-resolved conductance of Dirac electrons through multibarrier arrays

NASA Astrophysics Data System (ADS)

Dahal, Dipendra; Gumbs, Godfrey; Iurov, Andrii

We use a transfer matrix method to calculate the transmission coefficient of Dirac electrons through an arbitrary number of square potential barrier in gapped monolayer graphene(MLG) and bilayer graphene (BLG). The widths of barriers may not be chosen equal. The shift in the angle of incidence and the width of the barrier required for resonance are investigated numerically for both MLG and BLG. We compare the effects due to energy gap on these two transmission coefficient for each of these two structures (MLG and BLG). We present our results as functions of barrier width, height as well as incoming electron energy as well as band gap and examine the conditions for which perfect reflection or transmission occurs. Our transmission data are further used to calculate conductivity.

Anisotropic in-plane spin splitting in an asymmetric (001) GaAs/AlGaAs quantum well

PubMed Central

2011-01-01

The in-plane spin splitting of conduction-band electron has been investigated in an asymmetric (001) GaAs/AlxGa1-xAs quantum well by time-resolved Kerr rotation technique under a transverse magnetic field. The distinctive anisotropy of the spin splitting was observed while the temperature is below approximately 200 K. This anisotropy emerges from the combined effect of Dresselhaus spin-orbit coupling plus asymmetric potential gradients. We also exploit the temperature dependence of spin-splitting energy. Both the anisotropy of spin splitting and the in-plane effective g-factor decrease with increasing temperature. PACS: 78.47.jm, 71.70.Ej, 75.75.+a, 72.25.Fe, PMID:21888636

Increasing the efficiency and accuracy of time-resolved electronic spectra calculations with on-the-fly ab initio quantum dynamics methods

NASA Astrophysics Data System (ADS)

Vanicek, Jiri

2014-03-01

Rigorous quantum-mechanical calculations of coherent ultrafast electronic spectra remain difficult. I will present several approaches developed in our group that increase the efficiency and accuracy of such calculations: First, we justified the feasibility of evaluating time-resolved spectra of large systems by proving that the number of trajectories needed for convergence of the semiclassical dephasing representation/phase averaging is independent of dimensionality. Recently, we further accelerated this approximation with a cellular scheme employing inverse Weierstrass transform and optimal scaling of the cell size. The accuracy of potential energy surfaces was increased by combining the dephasing representation with accurate on-the-fly ab initio electronic structure calculations, including nonadiabatic and spin-orbit couplings. Finally, the inherent semiclassical approximation was removed in the exact quantum Gaussian dephasing representation, in which semiclassical trajectories are replaced by communicating frozen Gaussian basis functions evolving classically with an average Hamiltonian. Among other examples I will present an on-the-fly ab initio semiclassical dynamics calculation of the dispersed time-resolved stimulated emission spectrum of the 54-dimensional azulene. This research was supported by EPFL and by the Swiss National Science Foundation NCCR MUST (Molecular Ultrafast Science and Technology) and Grant No. 200021124936/1.

Quasi-Particle Relaxation and Quantum Femtosecond Magnetism in Non-Equilibrium Phases of Insulating Manganites

NASA Astrophysics Data System (ADS)

Perakis, Ilias; Kapetanakis, Myron; Lingos, Panagiotis; Barmparis, George; Patz, A.; Li, T.; Wang, Jigang

We study the role of spin quantum fluctuations driven by photoelectrons during 100fs photo-excitation of colossal magneto-resistive manganites in anti-ferromagnetic (AFM) charge-ordered insulating states with Jahn-Teller distortions. Our mean-field calculation of composite fermion excitations demonstrates that spin fluctuations reduce the energy gap by quasi-instantaneously deforming the AFM background, thus opening a conductive electronic pathway via FM correlation. We obtain two quasi-particle bands with distinct spin-charge dynamics and dependence on lattice distortions. To connect with fs-resolved spectroscopy experiments, we note the emergence of fs magnetization in the low-temperature magneto-optical signal, with threshold dependence on laser intensity characteristic of a photo-induced phase transition. Simultaneously, the differential reflectivity shows bi-exponential relaxation, with fs component, small at low intensity, exceeding ps component above threshold for fs AFM-to-FM switching. This suggests the emergence of a non-equilibrium metallic FM phase prior to establishment of a new lattice structure, linked with quantum magnetism via spin/charge/lattice couplings for weak magnetic fields.

Charge and spin control of ultrafast electron and hole dynamics in single CdSe/ZnSe quantum dots

NASA Astrophysics Data System (ADS)

Hinz, C.; Gumbsheimer, P.; Traum, C.; Holtkemper, M.; Bauer, B.; Haase, J.; Mahapatra, S.; Frey, A.; Brunner, K.; Reiter, D. E.; Kuhn, T.; Seletskiy, D. V.; Leitenstorfer, A.

2018-01-01

We study the dynamics of photoexcited electrons and holes in single negatively charged CdSe/ZnSe quantum dots with two-color femtosecond pump-probe spectroscopy. An initial characterization of the energy level structure is performed at low temperatures and magnetic fields of up to 5 T. Emission and absorption resonances are assigned to specific transitions between few-fermion states by a theoretical model based on a configuration interaction approach. To analyze the dynamics of individual charge carriers, we initialize the quantum system into excited trion states with defined energy and spin. Subsequently, the time-dependent occupation of the trion ground state is monitored by spectrally resolved differential transmission measurements. We observe subpicosecond dynamics for a hole excited to the D shell. The energy dependence of this D -to-S shell intraband transition is investigated in quantum dots of varying size. Excitation of an electron-hole pair in the respective p shells leads to the formation of singlet and triplet spin configurations. Relaxation of the p -shell singlet is observed to occur on a time scale of a few picoseconds. Pumping of p -shell triplet transitions opens up two pathways with distinctly different scattering times. These processes are shown to be governed by the mixing of singlet and triplet states due to exchange interactions enabling simultaneous electron and hole spin flips. To isolate the relaxation channels, we align the spin of the residual electron by a magnetic field and employ laser pulses of defined helicity. This step provides ultrafast preparation of a fully inverted trion ground state of the quantum dot with near unity probability, enabling deterministic addition of a single photon to the probe pulse. Therefore our experiments represent a significant step towards using single quantum emitters with well-controled inversion to manipulate the photon statistics of ultrafast light pulses.

Spin-orbit excitations and electronic structure of the putative Kitaev magnet α -RuCl3

NASA Astrophysics Data System (ADS)

Sandilands, Luke J.; Tian, Yao; Reijnders, Anjan A.; Kim, Heung-Sik; Plumb, K. W.; Kim, Young-June; Kee, Hae-Young; Burch, Kenneth S.

2016-02-01

Mott insulators with strong spin-orbit coupling have been proposed to host unconventional magnetic states, including the Kitaev quantum spin liquid. The 4 d system α -RuCl3 has recently come into view as a candidate Kitaev system, with evidence for unusual spin excitations in magnetic scattering experiments. We apply a combination of optical spectroscopy and Raman scattering to study the electronic structure of this material. Our measurements reveal a series of orbital excitations involving localized total angular momentum states of the Ru ion, implying that strong spin-orbit coupling and electron-electron interactions coexist in this material. Analysis of these features allows us to estimate the spin-orbit coupling strength, as well as other parameters describing the local electronic structure, revealing a well-defined hierarchy of energy scales within the Ru d states. By comparing our experimental results with density functional theory calculations, we also clarify the overall features of the optical response. Our results demonstrate that α -RuCl3 is an ideal material system to study spin-orbit coupled magnetism on the honeycomb lattice.

Interdependence of spin structure, anion height and electronic structure of BaFe{sub 2}As{sub 2}

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sen, Smritijit, E-mail: smritijit.sen@gmail.com; Ghosh, Haranath, E-mail: hng@rrcat.gov.in; Homi Bhabha National Institute, Anushaktinagar, Mumbai, 400094

2016-05-06

Superconducting as well as other electronic properties of Fe-based superconductors are quite sensitive to the structural parameters specially, on anion height which is intimately related to z{sub As}, the fractional z co-ordinate of As atom. Due to presence of strong magnetic fluctuation in these Fe-based superconductors, optimized structural parameters (lattice parameters a, b, c) including z{sub As} using density functional theory (DFT) under generalized gradient approximation (GGA) does not match experimental values accurately. In this work, we show that the optimized value of z{sub As} is strongly influenced by the spin structures in the orthorhombic phase of BaFe{sub 2}As{sub 2}more » system. We take all possible spin structures for the orthorhombic BaFe{sub 2}As{sub 2} system and then optimize z{sub As}. Using these optimized structures we calculate electronic structures like density of states, band structures etc., for each spin configurations. From these studies we show that the electronic structure, orbital order which is responsible for structural as well as related to nematic transition, are significantly influenced by the spin structures.« less

A Perspective on the Application of Spatially Resolved ARPES for 2D Materials

PubMed Central

Cattelan, Mattia

2018-01-01

In this paper, a perspective on the application of Spatially- and Angle-Resolved PhotoEmission Spectroscopy (ARPES) for the study of two-dimensional (2D) materials is presented. ARPES allows the direct measurement of the electronic band structure of materials generating extremely useful insights into their electronic properties. The possibility to apply this technique to 2D materials is of paramount importance because these ultrathin layers are considered fundamental for future electronic, photonic and spintronic devices. In this review an overview of the technical aspects of spatially localized ARPES is given along with a description of the most advanced setups for laboratory and synchrotron-based equipment. This technique is sensitive to the lateral dimensions of the sample. Therefore, a discussion on the preparation methods of 2D material is presented. Some of the most interesting results obtained by ARPES are reported in three sections including: graphene, transition metal dichalcogenides (TMDCs) and 2D heterostructures. Graphene has played a key role in ARPES studies because it inspired the use of this technique with other 2D materials. TMDCs are presented for their peculiar transport, optical and spin properties. Finally, the section featuring heterostructures highlights a future direction for research into 2D material structures. PMID:29702567

A Perspective on the Application of Spatially Resolved ARPES for 2D Materials.

PubMed

Cattelan, Mattia; Fox, Neil A

2018-04-27

In this paper, a perspective on the application of Spatially- and Angle-Resolved PhotoEmission Spectroscopy (ARPES) for the study of two-dimensional (2D) materials is presented. ARPES allows the direct measurement of the electronic band structure of materials generating extremely useful insights into their electronic properties. The possibility to apply this technique to 2D materials is of paramount importance because these ultrathin layers are considered fundamental for future electronic, photonic and spintronic devices. In this review an overview of the technical aspects of spatially localized ARPES is given along with a description of the most advanced setups for laboratory and synchrotron-based equipment. This technique is sensitive to the lateral dimensions of the sample. Therefore, a discussion on the preparation methods of 2D material is presented. Some of the most interesting results obtained by ARPES are reported in three sections including: graphene, transition metal dichalcogenides (TMDCs) and 2D heterostructures. Graphene has played a key role in ARPES studies because it inspired the use of this technique with other 2D materials. TMDCs are presented for their peculiar transport, optical and spin properties. Finally, the section featuring heterostructures highlights a future direction for research into 2D material structures.

Defect Induced Electronic Structure of Uranofullerene

PubMed Central

Dai, Xing; Cheng, Cheng; Zhang, Wei; Xin, Minsi; Huai, Ping; Zhang, Ruiqin; Wang, Zhigang

2013-01-01

The interaction between the inner atoms/cluster and the outer fullerene cage is the source of various novel properties of endohedral metallofullerenes. Herein, we introduce an adatom-type spin polarization defect on the surface of a typical endohedral stable U2@C60 to predict the associated structure and electronic properties of U2@C61 based on the density functional theory method. We found that defect induces obvious changes in the electronic structure of this metallofullerene. More interestingly, the ground state of U2@C61 is nonet spin in contrast to the septet of U2@C60. Electronic structure analysis shows that the inner U atoms and the C ad-atom on the surface of the cage contribute together to this spin state, which is brought about by a ferromagnetic coupling between the spin of the unpaired electrons of the U atoms and the C ad-atom. This discovery may provide a possible approach to adapt the electronic structure properties of endohedral metallofullerenes. PMID:23439318

Dynamic generation of spin-wave currents in hybrid structures

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lyapilin, I. I.; Okorokov, M. S., E-mail: Okorokovmike@gmail.com

2016-11-15

Spin transport through the interface in a semiconductor/ferromagnetic insulator hybrid structure is studied by the nonequilibrium statistical operator method under conditions of the spin Seebeck effect. The effective parameter approach in which each examined subsystem (conduction electrons, magnons, phonons) is characterized by its specific effective temperature is considered. The effect of the resonant (electric dipole) excitation of the spin electronic subsystem of conduction electrons on spin-wave current excitation in a ferromagnetic insulator is considered. The macroscopic equations describing the spin-wave current caused by both resonant excitation of the spin system of conduction electrons and the presence of a nonuniform temperaturemore » field in the ferromagnetic insulator are derived taking into account both the resonance-diffusion propagation of magnons and their relaxation processes. It is shown that spin-wave current excitation is also of resonant nature under the given conditions.« less

Reduced-Density-Matrix Description of Decoherence and Relaxation Processes for Electron-Spin Systems

NASA Astrophysics Data System (ADS)

Jacobs, Verne

2017-04-01

Electron-spin systems are investigated using a reduced-density-matrix description. Applications of interest include trapped atomic systems in optical lattices, semiconductor quantum dots, and vacancy defect centers in solids. Complimentary time-domain (equation-of-motion) and frequency-domain (resolvent-operator) formulations are self-consistently developed. The general non-perturbative and non-Markovian formulations provide a fundamental framework for systematic evaluations of corrections to the standard Born (lowest-order-perturbation) and Markov (short-memory-time) approximations. Particular attention is given to decoherence and relaxation processes, as well as spectral-line broadening phenomena, that are induced by interactions with photons, phonons, nuclear spins, and external electric and magnetic fields. These processes are treated either as coherent interactions or as environmental interactions. The environmental interactions are incorporated by means of the general expressions derived for the time-domain and frequency-domain Liouville-space self-energy operators, for which the tetradic-matrix elements are explicitly evaluated in the diagonal-resolvent, lowest-order, and Markov (short-memory time) approximations. Work supported by the Office of Naval Research through the Basic Research Program at The Naval Research Laboratory.

Gigantic 2D laser-induced photovoltaic effect in magnetically doped topological insulators for surface zero-bias spin-polarized current generation

NASA Astrophysics Data System (ADS)

Shikin, A. M.; Voroshin, V. Yu; Rybkin, A. G.; Kokh, K. A.; Tereshchenko, O. E.; Ishida, Y.; Kimura, A.

2018-01-01

A new kind of 2D photovoltaic effect (PVE) with the generation of anomalously large surface photovoltage up to 210 meV in magnetically doped topological insulators (TIs) has been studied by the laser time-resolved pump-probe angle-resolved photoelectron spectroscopy. The PVE has maximal efficiency for TIs with high occupation of the upper Dirac cone (DC) states and the Dirac point located inside the fundamental energy gap. For TIs with low occupation of the upper DC states and the Dirac point located inside the valence band the generated surface photovoltage is significantly reduced. We have shown that the observed giant PVE is related to the laser-generated electron-hole asymmetry followed by accumulation of the photoexcited electrons at the surface. It is accompanied by the 2D relaxation process with the generation of zero-bias spin-polarized currents flowing along the topological surface states (TSSs) outside the laser beam spot. As a result, the spin-polarized current generates an effective in-plane magnetic field that is experimentally confirmed by the k II-shift of the DC relative to the bottom non-spin-polarized conduction band states. The realized 2D PVE can be considered as a source for the generation of zero-bias surface spin-polarized currents and the laser-induced local surface magnetization developed in such kind 2D TSS materials.

Laser Spectroscopy and AB Initio Calculations on the TaF Molecule

NASA Astrophysics Data System (ADS)

Ng, Kiu Fung; Zou, Wenli; Liu, Wenjian; Cheung, Allan S. C.

2016-06-01

Electronic transition spectrum of the tantalum monoflouride (TaF) molecule in the spectral region between 448 and 520 nm has been studied using the technique of laser-ablation/reaction free jet expansion and laser induced fluorescence spectroscopy. TaF molecule was produced by reacting laser-ablated tantalum atoms with sulfur hexafluoride gas seeded in argon. Sixteen vibrational bands with resolved rotational structure have been recorded and analyzed, which were organized into six electronic transition systems and the ground state has been identified to be the X3Σ-(0+) state with bond length, ro, and equilibrium vibrational frequency, ωe, determined to be 1.8209 Å and 700.1 wn respectively. In addition, four vibrational bands belong to another transition system involving lower state with Ω = 2 component has also been analyzed. All observed transitions are with ΔΩ = 0. Least-squares fit of the measured line positions yielded molecular constants for the electronic states involved. The Λ-S and Ω states of TaF were calculated at the state-averaged complete active space self-consistent field (SA-CASSCF) and the subsequent internally contracted multi-reference configuration interaction with singles and doubles and Davidson's cluster correction (MRCISD+Q) levels of theory with the active space of 4 electrons in 6 orbitals, that is, the molecular orbitals corresponding to Ta 5d6s are active. The spin-orbit coupling (SOC) is calculated by the state-interaction approach at the SA-CASSCF level via the relativistic effective core potentials (RECPs) spin-orbit operator, where the diagonal elements of the spin-orbit matrix are replaced by the above MRCISD+Q energies. The spectroscopic properties of the ground and many low-lying electronic states of the TaF molecule will be reported. With respect to the observed electronic states in this work, the calculated results are in good agreement with our experimental determinations. This work represents the first experimental investigation of the molecular structure of the TaF molecule.

Spin-dependent dwell times of electron tunneling through double- and triple-barrier structures

NASA Astrophysics Data System (ADS)

Erić, Marko; Radovanović, Jelena; Milanović, Vitomir; Ikonić, Zoran; Indjin, Dragan

2008-04-01

We have analyzed the influence of Dresselhaus and Rashba spin-orbit couplings (caused by the bulk inversion asymmetry and the structural asymmetry, respectively) on electron tunneling through a double- and triple-barrier structures, with and without an externally applied electric field. The results indicate that the degree of structural asymmetry and external electric field can greatly affect the dwell times of electrons with opposite spin orientation. This opens up the possibilities of obtaining efficient spin separation in the time domain. The material system of choice is AlxGa1-xSb, and the presented model takes into account the position dependence of material parameters, as well as the effects of band nonparabolicity.

Gate-Controlled Spin-Valley Locking of Resident Carriers in WSe2 Monolayers

NASA Astrophysics Data System (ADS)

Dey, P.; Yang, Luyi; Robert, C.; Wang, G.; Urbaszek, B.; Marie, X.; Crooker, S. A.

2017-09-01

Using time-resolved Kerr rotation, we measure the spin-valley dynamics of resident electrons and holes in single charge-tunable monolayers of the archetypal transition-metal dichalcogenide (TMD) semiconductor WSe2 . In the n -type regime, we observe long (˜130 ns ) polarization relaxation of electrons that is sensitive to in-plane magnetic fields By, indicating spin relaxation. In marked contrast, extraordinarily long (˜2 μ s ) polarization relaxation of holes is revealed in the p -type regime, which is unaffected by By, directly confirming long-standing expectations of strong spin-valley locking of holes in the valence band of monolayer TMDs. Supported by continuous-wave Kerr spectroscopy and Hanle measurements, these studies provide a unified picture of carrier polarization dynamics in monolayer TMDs, which can guide design principles for future valleytronic devices.

Controlling entangled spin-orbit coupling of 5 d states with interfacial heterostructure engineering

NASA Astrophysics Data System (ADS)

Kim, J.-W.; Choi, Y.; Chun, S. H.; Haskel, D.; Yi, D.; Ramesh, R.; Liu, J.; Ryan, P. J.

2018-03-01

The combination of strong electron correlations in 3 d transition-metal oxides and spin-orbit interactions in the 5 d counterpart can give rise to exotic electronic and magnetic properties. Here, the nature of emerging phenomena at the interface between SrIr O3 (SIO) and L a2 /3S r1 /3Mn O3 (LSMO) is presented. Nominally, SIO with strong spin-orbit interaction is metallic and nonmagnetic on the verge of a metal-insulator transition, whereas LSMO is metallic and ferromagnetic with itinerant character and high spin polarization. In the 1:1 LSMO/SIO superlattice, we observe ferromagnetic Mn moments with an insulating behavior, accompanied by antiferromagnetic ordering in SIO. Element-resolved x-ray magnetic circular dichroism proves that there is a weak net ferromagnetic Ir moment aligned antiparallel to the Mn counterpart. The branching ratio shows the formation of molecular orbitals between the Mn and Ir layers modifying the Ir 5 d electronic configuration through the mixture of t2 g and eg states, resulting in a deviation from Jeff=1 /2 . This result demonstrates a pathway to manipulate the spin-orbit entanglement in 5 d states with two-dimensional 3 d spin-polarized electrons through heterostructure design.

Determining the nature of excitonic dephasing in high-quality GaN/AlGaN quantum wells through time-resolved and spectrally resolved four-wave mixing spectroscopy

NASA Astrophysics Data System (ADS)

Gallart, M.; Ziegler, M.; Crégut, O.; Feltin, E.; Carlin, J.-F.; Butté, R.; Grandjean, N.; Hönerlage, B.; Gilliot, P.

2017-07-01

Applying four-wave mixing spectroscopy to a high-quality GaN/AlGaN single quantum well, we report on the experimental determination of excitonic dephasing times at different temperatures and exciton densities in III-nitride heterostructures. By comparing the evolution with the temperature of the dephasing and the spin-relaxation rate, we conclude that both processes are related to the rate of excitonic collisions. When spin relaxation occurs in the motional-narrowing regime, it remains constant over a large temperature range as the spin-precession frequency increases linearly with temperature, hence compensating for the observed decrease in the dephasing time. From those measurements, a value of the electron-hole exchange interaction strength of 0.45 meV at T =10 K is inferred.

Gd(III) complexes as paramagnetic tags: Evaluation of the spin delocalization over the nuclei of the ligand

NASA Astrophysics Data System (ADS)

Collauto, A.; Feintuch, A.; Qi, M.; Godt, A.; Meade, T.; Goldfarb, D.

2016-02-01

Complexes of the Gd(III) ion are currently being established as spin labels for distance determination in biomolecules by pulse dipolar spectroscopy. Because Gd(III) is an f ion, one expects electron spin density to be localized on the Gd(III) ion - an important feature for the mentioned application. Most of the complex ligands have nitrogens as Gd(III) coordinating atoms. Therefore, measurement of the 14N hyperfine coupling gives access to information on the localization of the electron spin on the Gd(III) ion. We carried out W-band, 1D and 2D 14N and 1H ENDOR measurements on the Gd(III) complexes Gd-DOTA, Gd-538, Gd-595, and Gd-PyMTA that serve as spin labels for Gd-Gd distance measurements. The obtained 14N spectra are particularly well resolved, revealing both the hyperfine and nuclear quadrupole splittings, which were assigned using 2D Mims ENDOR experiments. Additionally, the spectral contributions of the two different types of nitrogen atoms of Gd-PyMTA, the aliphatic N atom and the pyridine N atom, were distinguishable. The 14N hyperfine interaction was found to have a very small isotropic hyperfine component of -0.25 to -0.37 MHz. Furthermore, the anisotropic hyperfine interactions with the 14N nuclei and with the non-exchangeable protons of the ligands are well described by the point-dipole approximation using distances derived from the crystal structures. We therefore conclude that the spin density is fully localized on the Gd(III) ion and that the spin density distribution over the nuclei of the ligands is rightfully ignored when analyzing distance measurements.

Diode laser spectroscopy of the MnD radical ( 7Σ) and the determination of mass-independent parameters

NASA Astrophysics Data System (ADS)

Urban, Rolf-Dieter; Jones, Harold

1991-03-01

The infrared spectrum of the manganese deuteride radical has been observed in its ground electronic state ( 7Σ) using a diode-laser spectrometer. The hyperfine structure of a number of infrared transitions in the bands ν=1←0, ν=2←1 and ν=3←2 were measured with a nominal accuracy of ±0.001 cm -1. In all cases, the complete structure was easily resolved. Dunham parameters, spin—rotation and spin—spin coupling parameters were determined from the MnD data. A simultaneous fit of these data with those determined previously for MnH was carried out to determine mass-independent parameters and mass-scaling coefficients.

Atomic-scale understanding of high thermal stability of the Mo/CoFeB/MgO spin injector for spin-injection in remanence.

PubMed

Tao, Bingshan; Barate, Philippe; Devaux, Xavier; Renucci, Pierre; Frougier, Julien; Djeffal, Abdelhak; Liang, Shiheng; Xu, Bo; Hehn, Michel; Jaffrès, Henri; George, Jean-Marie; Marie, Xavier; Mangin, Stéphane; Han, Xiufeng; Wang, Zhanguo; Lu, Yuan

2018-05-31

Remanent spin injection into a spin light emitting diode (spin-LED) at zero magnetic field is a prerequisite for future application of spin optoelectronics. Here, we demonstrate the remanent spin injection into GaAs based LEDs with a thermally stable Mo/CoFeB/MgO spin injector. A systematic study of magnetic properties, polarization-resolved electroluminescence (EL) and atomic-scale interfacial structures has been performed in comparison with the Ta/CoFeB/MgO spin injector. The perpendicular magnetic anisotropy (PMA) of the Mo/CoFeB/MgO injector shows more advanced thermal stability than that of the Ta/CoFeB/MgO injector and robust PMA can be maintained up to 400 °C annealing. The remanent circular polarization (PC) of EL from the Mo capped spin-LED reaches a maximum value of 10% after 300 °C annealing, and even remains at 4% after 400 °C annealing. In contrast, the Ta capped spin-LED almost completely loses the remanent PC under 400 °C annealing. Combined advanced electron microscopy and spectroscopy studies reveal that a large amount of Ta diffuses into the MgO tunneling barrier through the CoFeB layer after 400 °C annealing. However, the diffusion of Mo into CoFeB is limited and never reaches the MgO barrier. These findings afford a comprehensive perspective to use the highly thermally stable Mo/CoFeB/MgO spin injector for efficient electrical spin injection in remanence.

Coherent manipulation of spin correlations in the Hubbard model

NASA Astrophysics Data System (ADS)

Wurz, N.; Chan, C. F.; Gall, M.; Drewes, J. H.; Cocchi, E.; Miller, L. A.; Pertot, D.; Brennecke, F.; Köhl, M.

2018-05-01

We coherently manipulate spin correlations in a two-component atomic Fermi gas loaded into an optical lattice using spatially and time-resolved Ramsey spectroscopy combined with high-resolution in situ imaging. This technique allows us not only to imprint spin patterns but also to probe the static magnetic structure factor at an arbitrary wave vector, in particular, the staggered structure factor. From a measurement along the diagonal of the first Brillouin zone of the optical lattice, we determine the magnetic correlation length and the individual spatial spin correlators. At half filling, the staggered magnetic structure factor serves as a sensitive thermometer, which we employ to study the equilibration in the spin and density sector during a slow quench of the lattice depth.

Electronic Structure, Surface Doping, and Optical Response in Epitaxial WSe2 Thin Films.

PubMed

Zhang, Yi; Ugeda, Miguel M; Jin, Chenhao; Shi, Su-Fei; Bradley, Aaron J; Martín-Recio, Ana; Ryu, Hyejin; Kim, Jonghwan; Tang, Shujie; Kim, Yeongkwan; Zhou, Bo; Hwang, Choongyu; Chen, Yulin; Wang, Feng; Crommie, Michael F; Hussain, Zahid; Shen, Zhi-Xun; Mo, Sung-Kwan

2016-04-13

High quality WSe2 films have been grown on bilayer graphene (BLG) with layer-by-layer control of thickness using molecular beam epitaxy. The combination of angle-resolved photoemission, scanning tunneling microscopy/spectroscopy, and optical absorption measurements reveal the atomic and electronic structures evolution and optical response of WSe2/BLG. We observe that a bilayer of WSe2 is a direct bandgap semiconductor, when integrated in a BLG-based heterostructure, thus shifting the direct-indirect band gap crossover to trilayer WSe2. In the monolayer limit, WSe2 shows a spin-splitting of 475 meV in the valence band at the K point, the largest value observed among all the MX2 (M = Mo, W; X = S, Se) materials. The exciton binding energy of monolayer-WSe2/BLG is found to be 0.21 eV, a value that is orders of magnitude larger than that of conventional three-dimensional semiconductors, yet small as compared to other two-dimensional transition metal dichalcogennides (TMDCs) semiconductors. Finally, our finding regarding the overall modification of the electronic structure by an alkali metal surface electron doping opens a route to further control the electronic properties of TMDCs.

Electronic structure, surface doping, and optical response in epitaxial WSe 2 thin films

DOE PAGES

Zhang, Yi; Ugeda, Miguel M.; Jin, Chenhao; ...

2016-03-14

High quality WSe 2 films have been grown on bilayer graphene (BLG) with layer-by-layer control of thickness using molecular beam epitaxy. The combination of angle-resolved photoemission, scanning tunneling microscopy/spectroscopy, and optical absorption measurements reveal the atomic and electronic structures evolution and optical response of WSe 2/BLG. We observe that a bilayer of WSe 2 is a direct bandgap semiconductor, when integrated in a BLG-based heterostructure, thus shifting the direct–indirect band gap crossover to trilayer WSe 2. In the monolayer limit, WSe 2 shows a spin-splitting of 475 meV in the valence band at the K point, the largest value observedmore » among all the MX 2 (M = Mo, W; X = S, Se) materials. The exciton binding energy of monolayer-WSe 2/BLG is found to be 0.21 eV, a value that is orders of magnitude larger than that of conventional three-dimensional semiconductors, yet small as compared to other two-dimensional transition metal dichalcogennides (TMDCs) semiconductors. Lastly, our finding regarding the overall modification of the electronic structure by an alkali metal surface electron doping opens a route to further control the electronic properties of TMDCs.« less

Fingerprints of entangled spin and orbital physics in itinerant ferromagnets via angle-resolved resonant photoemission

NASA Astrophysics Data System (ADS)

Da Pieve, F.

2016-01-01

A method for mapping the local spin and orbital nature of the ground state of a system via corresponding flip excitations is proposed based on angle-resolved resonant photoemission and related diffraction patterns, obtained here via an ab initio modified one-step theory of photoemission. The analysis is done on the paradigmatic weak itinerant ferromagnet bcc Fe, whose magnetism, a correlation phenomenon given by the coexistence of localized moments and itinerant electrons, and the observed non-Fermi-Liquid behavior at extreme conditions both remain unclear. The combined analysis of energy spectra and diffraction patterns offers a mapping of local pure spin-flip, entangled spin-flip-orbital-flip excitations and chiral transitions with vortexlike wave fronts of photoelectrons, depending on the valence orbital symmetry and the direction of the local magnetic moment. Such effects, mediated by the hole polarization, make resonant photoemission a promising tool to perform a full tomography of the local magnetic properties even in itinerant ferromagnets or macroscopically nonmagnetic systems.

Doping-dependent correlation effects in (Sr1-xLax) 3Ir2O7

NASA Astrophysics Data System (ADS)

Affeldt, Gregory; Hogan, Tom; Denlinger, Jonathan D.; Vishwanath, Ashvin; Wilson, Stephen D.; Lanzara, Alessandra

2018-03-01

We have measured the signatures of electronic energy scales and their doping evolution in the band structure of (Sr1-xLax) 3Ir2O7 using angle-resolved photoemission spectroscopy. While band splittings and positions corresponding to the bilayer splitting and spin-orbit coupling undergo only small changes, the Mott gap and effective mass of both the lower Hubbard band and conduction band exhibit strong variations with doping. These changes correspond to similar observations in the cuprate superconductors, and are likely connected to the changing effective Coulomb interaction upon addition of itinerant carriers.

Enhancing coherence in molecular spin qubits via atomic clock transitions

NASA Astrophysics Data System (ADS)

Shiddiq, Muhandis; Komijani, Dorsa; Duan, Yan; Gaita-Ariño, Alejandro; Coronado, Eugenio; Hill, Stephen

2016-03-01

Quantum computing is an emerging area within the information sciences revolving around the concept of quantum bits (qubits). A major obstacle is the extreme fragility of these qubits due to interactions with their environment that destroy their quantumness. This phenomenon, known as decoherence, is of fundamental interest. There are many competing candidates for qubits, including superconducting circuits, quantum optical cavities, ultracold atoms and spin qubits, and each has its strengths and weaknesses. When dealing with spin qubits, the strongest source of decoherence is the magnetic dipolar interaction. To minimize it, spins are typically diluted in a diamagnetic matrix. For example, this dilution can be taken to the extreme of a single phosphorus atom in silicon, whereas in molecular matrices a typical ratio is one magnetic molecule per 10,000 matrix molecules. However, there is a fundamental contradiction between reducing decoherence by dilution and allowing quantum operations via the interaction between spin qubits. To resolve this contradiction, the design and engineering of quantum hardware can benefit from a ‘bottom-up’ approach whereby the electronic structure of magnetic molecules is chemically tailored to give the desired physical behaviour. Here we present a way of enhancing coherence in solid-state molecular spin qubits without resorting to extreme dilution. It is based on the design of molecular structures with crystal field ground states possessing large tunnelling gaps that give rise to optimal operating points, or atomic clock transitions, at which the quantum spin dynamics become protected against dipolar decoherence. This approach is illustrated with a holmium molecular nanomagnet in which long coherence times (up to 8.4 microseconds at 5 kelvin) are obtained at unusually high concentrations. This finding opens new avenues for quantum computing based on molecular spin qubits.

Experimental and ab initio characterization of HC3N+ vibronic structure. II. High-resolution VUV PFI-ZEKE spectroscopy.

PubMed

Gans, Bérenger; Lamarre, Nicolas; Broquier, Michel; Liévin, Jacques; Boyé-Péronne, Séverine

2016-12-21

Vacuum-ultraviolet pulsed-field-ionization zero-kinetic-energy photoelectron spectra of X + Π2←XΣ+1 and B + Π2←XΣ+1 transitions of the HC 3 14 N and HC 3 15 N isotopologues of cyanoacetylene have been recorded. The resolution of the photoelectron spectra allowed us to resolve the vibrational structures and the spin-orbit splittings in the cation. Accurate values of the adiabatic ionization potentials of the two isotopologues (E I /hc(HC 3 14 N)=93 909(2) cm -1 and E I /hc(HC 3 15 N)=93 912(2) cm -1 ), the vibrational frequencies of the ν 2 , ν 6 , and ν 7 vibrational modes, and the spin-orbit coupling constant (A SO = -44(2) cm -1 ) of the X + Π2 cationic ground state have been derived from the measurements. Using ab initio calculations, the unexpected structure of the B + Π2←XΣ+1 transition is tentatively attributed to a conical intersection between the A + and B + electronic states of the cation.

Atomic-scale observation of structural and electronic orders in the layered compound α-RuCl3

NASA Astrophysics Data System (ADS)

Ziatdinov, M.; Banerjee, A.; Maksov, A.; Berlijn, T.; Zhou, W.; Cao, H. B.; Yan, J.-Q.; Bridges, C. A.; Mandrus, D. G.; Nagler, S. E.; Baddorf, A. P.; Kalinin, S. V.

2016-12-01

A pseudospin-1/2 Mott phase on a honeycomb lattice is proposed to host the celebrated two-dimensional Kitaev model which has an elusive quantum spin liquid ground state, and fascinating physics relevant to the development of future templates towards topological quantum bits. Here we report a comprehensive, atomically resolved real-space study by scanning transmission electron and scanning tunnelling microscopies on a novel layered material displaying Kitaev physics, α-RuCl3. Our local crystallography analysis reveals considerable variations in the geometry of the ligand sublattice in thin films of α-RuCl3 that opens a way to realization of a spatially inhomogeneous magnetic ground state at the nanometre length scale. Using scanning tunnelling techniques, we observe the electronic energy gap of ~0.25 eV and intra-unit cell symmetry breaking of charge distribution in individual α-RuCl3 surface layer. The corresponding charge-ordered pattern has a fine structure associated with two different types of charge disproportionation at Cl-terminated surface.

Periodicity, Electronic Structures, and Bonding of Gold Tetrahalides [AuX4](-) (X = F, CI, Br, I, At, Uus)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Li, Wan-Lu; Li, Yong; Xu, Congqiao

2015-12-07

Systematic theoretical and experimental investigations have been performed to understand the periodicity and electronic structures of trivalent-gold halides using gold tetrahalides [AuX4]⁻ anions (X = F, Cl, Br, I, At, Uus). The [AuX4]⁻ (X = Cl, Br, I) anions were produced in gas phase and their negative-ion photoelectron spectra were obtained, which exhibited rich and well-resolved spectral peaks. We calculated the adiabatic as well as vertical electron detachment energies using density functional methods with scalar and spin-orbit coupling relativistic effects. The simulated photoelectron spectra based on these calculations are in good agreement with the experimental spectra. Our results show thatmore » the trivalent Au(III) oxidation state becomes progressively less stable while Au(I) is preferred when the halides become heavier along the Period Table. This trend reveals that the oxidation state of metals in complexes can be manipulated through ligand design« less

Ultrafast observation of critical nematic fluctuations and giant magnetoelastic coupling in iron pnictides

NASA Astrophysics Data System (ADS)

Patz, Aaron; Li, Tianqi; Ran, Sheng; Fernandes, Rafael M.; Schmalian, Joerg; Bud'Ko, Sergey L.; Canfield, Paul C.; Perakis, Ilias E.; Wang, Jigang

2014-02-01

Many of the iron pnictides have strongly anisotropic normal-state characteristics, important for the exotic magnetic and superconducting behaviour these materials exhibit. Yet, the origin of the observed anisotropy is unclear. Electronically driven nematicity has been suggested, but distinguishing this as an independent degree of freedom from magnetic and structural orders is difficult, as these couple together to break the same tetragonal symmetry. Here we use time-resolved polarimetry to reveal critical nematic fluctuations in unstrained Ba(Fe1-xCox)2As2. The femtosecond anisotropic response, which arises from the two-fold in-plane anisotropy of the complex refractive index, displays a characteristic two-step recovery absent in the isotropic response. The fast recovery appears only in the magnetically ordered state, whereas the slow one persists in the paramagnetic phase with a critical divergence approaching the structural transition temperature. The dynamics also reveal a gigantic magnetoelastic coupling that far exceeds electron-spin and electron-phonon couplings, opposite to conventional magnetic metals.

A parity-breaking electronic nematic phase transition in the spin-orbit coupled metal Cd 2Re 2O 7

DOE Office of Scientific and Technical Information (OSTI.GOV)

Harter, J. W.; Zhao, Z. Y.; Yan, J. -Q.

Strong electron interactions can drive metallic systems toward a variety of well-known symmetry-broken phases, but the instabilities of correlated metals with strong spin-orbit coupling have only recently begun to be explored. We uncovered a multipolar nematic phase of matter in the metallic pyrochlore Cd 2Re 2O 7 using spatially resolved second-harmonic optical anisotropy measurements. Like previously discovered electronic nematic phases, this multipolar phase spontaneously breaks rotational symmetry while preserving translational invariance. However, it has the distinguishing property of being odd under spatial inversion, which is allowed only in the presence of spin-orbit coupling. By examining the critical behavior of themore » multipolar nematic order parameter, we show that it drives the thermal phase transition near 200 kelvin in Cd 2Re 2O 7 and induces a parity-breaking lattice distortion as a secondary order.« less

A parity-breaking electronic nematic phase transition in the spin-orbit coupled metal Cd2Re2O7

NASA Astrophysics Data System (ADS)

Harter, J. W.; Zhao, Z. Y.; Yan, J.-Q.; Mandrus, D. G.; Hsieh, D.

2017-04-01

Strong electron interactions can drive metallic systems toward a variety of well-known symmetry-broken phases, but the instabilities of correlated metals with strong spin-orbit coupling have only recently begun to be explored. We uncovered a multipolar nematic phase of matter in the metallic pyrochlore Cd2Re2O7 using spatially resolved second-harmonic optical anisotropy measurements. Like previously discovered electronic nematic phases, this multipolar phase spontaneously breaks rotational symmetry while preserving translational invariance. However, it has the distinguishing property of being odd under spatial inversion, which is allowed only in the presence of spin-orbit coupling. By examining the critical behavior of the multipolar nematic order parameter, we show that it drives the thermal phase transition near 200 kelvin in Cd2Re2O7 and induces a parity-breaking lattice distortion as a secondary order.

A parity-breaking electronic nematic phase transition in the spin-orbit coupled metal Cd 2Re 2O 7

DOE PAGES

Harter, J. W.; Zhao, Z. Y.; Yan, J. -Q.; ...

2017-04-21

Strong electron interactions can drive metallic systems toward a variety of well-known symmetry-broken phases, but the instabilities of correlated metals with strong spin-orbit coupling have only recently begun to be explored. We uncovered a multipolar nematic phase of matter in the metallic pyrochlore Cd 2Re 2O 7 using spatially resolved second-harmonic optical anisotropy measurements. Like previously discovered electronic nematic phases, this multipolar phase spontaneously breaks rotational symmetry while preserving translational invariance. However, it has the distinguishing property of being odd under spatial inversion, which is allowed only in the presence of spin-orbit coupling. By examining the critical behavior of themore » multipolar nematic order parameter, we show that it drives the thermal phase transition near 200 kelvin in Cd 2Re 2O 7 and induces a parity-breaking lattice distortion as a secondary order.« less

Multinuclear Detection of Nuclear Spin Optical Rotation at Low Field.

PubMed

Zhu, Yue; Gao, Yuheng; Rodocker, Shane; Savukov, Igor; Hilty, Christian

2018-06-06

We describe the multinuclear detection of nuclear spin optical rotation (NSOR), an effect dependent on the hyperfine interaction between nuclear spins and electrons. Signals of 1 H and 19 F are discriminated by frequency in a single spectrum acquired at sub-millitesla field. The simultaneously acquired optical signal along with the nuclear magnetic resonance signal allows the calculation of the relative magnitude of the NSOR constants corresponding to different nuclei within the sample molecules. This is illustrated by a larger NSOR signal measured at the 19 F frequency despite a smaller corresponding spin concentration. Second, it is shown that heteronuclear J-coupling is observable in the NSOR signal, which can be used to retrieve chemical information. Multinuclear frequency and J resolution can localize optical signals in the molecule. Properties of electronic states at multiple sites in a molecule may therefore ultimately be determined by frequency-resolved NSOR spectroscopy at low field.

Ballistic Electron Emission Microscopy Studies of Ferromagnet - Semiconductor Interfaces

NASA Astrophysics Data System (ADS)

Mather, P. G.; Perrella, A. C.; Yurtsever, A.; Buhrman, R. A.

2004-03-01

Devices that employ spin as well as charge effects have been the subjects of extensive study recently. The magnetic tunneling transistor (1) is one important device that demonstrates an electrical means of injecting spin-polarized electrons into a semiconductor. A Schottky barrier lies at the heart of the device, and a high quality spatially homogenous and uniform barrier formed on GaAs is highly desirable. We have used ballistic electron emission microscopy (BEEM) to study CoFe, Fe and permalloy deposited on a GaAs substrate to give nanometer resolved evaluation of hot electron transport through the films and across the Schottky barrier. All films give a homogenous, uniform barrier as compared with evaporated Au/GaAs and Ag/GaAs interfaces. We will report on BEEM measurements of the hot electron transfer ratio across the Schottky barrier for the different ferromagnetic materials, and on the energy and spin-dependent hot electron attenuation lengths of the CoFe, Fe, and permalloy films. (1) Sebastiaan van Dijken, Xin Jiang, Stuart S. P. Parkin, APL, 80, 3364.

The local magnetic properties of [MnIII6 CrIII]3+ and [FeIII6 CrIII]3+ single-molecule magnets deposited on surfaces studied by spin-polarized photoemission and XMCD with circularly polarized synchrotron radiation

NASA Astrophysics Data System (ADS)

Heinzmann, U.; Helmstedt, A.; Dohmeier, N.; Müller, N.; Gryzia, A.; Brechling, A.; Hoeke, V.; Krickemeyer, E.; Glaser, T.; Fonin, M.; Bouvron, S.; Leicht, P.; Tietze, T.; Goering, E.; Kuepper, K.

2014-04-01

It is demonstrated that local magnetic moments of single molecule magnets (SMM) normally studied by XMCD at very low temperatures and high magnetic fields can be measured by means of spin-resolved electron emission in the paramagnetic phase at room temperature by use of circularly polarized radiation.

EDITORIAL: Ultrafast magnetization processes

NASA Astrophysics Data System (ADS)

Hillebrands, Burkard

2008-09-01

This Cluster Issue of Journal of Physics D: Applied Physics is devoted to ultrafast magnetization processes. It reports on the scientific yield of the Priority Programme 1133 'Ultrafast Magnetization Processes' which was funded by the Deutsche Forschungsgemeinschaft in the period 2002-2008 in three successive two-year funding periods, supporting research of 17-18 groups in Germany. Now, at the end of this Priority Programme, the members feel that the achievements made in the course of the programme merit communication to the international scientific community in a concerted way. Therefore, each of the projects of the last funding period presents a key result in a published contribution to this Cluster Issue. The purpose of the funding by a Priority Programme is to advance knowledge in an emerging field of research through collaborative networked support over several locations. Priority Programmes are characterized by their enhanced quality of research through the use of new methods and forms of collaboration in emerging fields, by added value through interdisciplinary cooperation, and by networking. The aim of the Priority Programme 1133 'Ultrafast Magnetization Processes' may be well characterized by the call for projects in June 2001 after the programme was approved by the Deutsche Forschungsgemeinschaft: 'The aim of the priority programme is the achievement of a basic understanding of the temporal evolution of fast magnetization processes in magnetically ordered films, multilayers and micro-structured systems. The challenge lies in the advancement of the field of ultrafast magnetization processes into the regime of a few femtoseconds to nanoseconds, a topic not yet well explored. A general aim is to understand the fundamental mechanisms needed for applications in ultrafast magneto-electronic devices. The fundamental topic to be addressed is the response of the magnetization of small structures upon the application of pulsed magnetic fields, laser pulses or injected spin-polarized electron pulses on short time scales, ranging from a small disturbance of the system up to the reversal of the magnetization direction.' Now, seven years later, the subject of ultrafast magnetization processes has grown into a mainstream research direction in modern magnetism. The major international conferences on magnetism, such as the Annual Conference on Magnetism and Magnetic Materials (MMM), the INTERMAG, the International Conference of Magnetism, as well as many regional conferences, schedule dedicated sessions to ultrafast magnetization processes, very often several of them. The large share in research in this field from German scientists has been made possible by this Priority Programme. Since its beginning, new developments have been picked up by the Priority Programme 1133 and addressed by projects. Spin torque phenomena in spin dynamics, although foreseen at the time of establishing the Priority Programme, have been taken up. The field of dissipation has been addressed and extended by several groups, with contributions both from theoretical and experimental groups. A first set of contributions addresses ultrafast dynamics and materials. T Roth et al [article 164001] in this issue] study the dynamics of coercivity in ultrafast pump-probe experiments on the femtosecond time scale. They show that an all optical pump-probe technique is, in general, not suitable for gaining access to the time-dependent behaviour of the coercivity, since the switching in a fixed external field is an irreversible process. They comment on the possible mechanisms leading to the observed reduction of the coercivity with increasing pump power and propose a potential solution to clarify the origin of such a behaviour. B Heitkamp et al [164002] discuss the femtosecond spin dynamics of ferromagnetic CoPt thin films and nanodots, which they probe using spin-polarized photoemission electron microscopy. They show by photoelectron spin analysis, that enhanced optical near fields can be used to induce a local demagnetization of the sample following femtosecond laser excitation. A B Schmidt et al [164003] report a new access to the surface electronic structure of fcc Co films combining spin-resolved one- and two-photon photoemission. The knowledge of surface states is important for interpreting time-resolved measurements of ultrafast magnetization dynamics in this material. An extension of ultrafast dynamics has been made by several groups. A Melnikov et al [164004] report on the ultrafast dynamics at lanthanide surfaces such as Gd(0001) and Tb(0001) using time-resolved second-harmonic generation and photoelectron spectroscopy. These surfaces exhibit a rich dynamics including a collective response of the crystal lattice and the magnetization. Effects of phonon-magnon scattering are discussed. M Fiebig et al [164005] report on experiments of ultrafast magnetization dynamics in antiferromagnetic compounds, and show that the magnetization dynamics in these systems differs noticeably from that of ferromagnetic compounds. They use optical second-harmonic generation and linear reflection to monitor the evolution of the antiferromagnetic order parameter subsequent to an intense optical excitation. In a theory paper, the local light-induced spin manipulation in two-magnetic-centre metallic chains is studied by T Hardenstein et al [164006] using highly correlational ab initio calculations. They show that, as an example of local spin manipulation, the spin on the iron side of a Co-Na-Fe cluster can be switched. S Halm et al [164007] present evidence to manipulate spin states in a diluted magnetic semiconductor on a submicrometer length scale via the magnetic fringe fields of micro-structured magnets. By optically switching the magnetization of the ferromagnet, the magnetization in the semiconductor is manipulated and the limits of a dynamical interaction between the spin states in the ferromagnet and the magnetic semiconductor are discussed. A second set of contributions addresses the field of spin waves and dynamic spin torque phenomena. C W Sandweg et al [164008] discuss the modification of the thermal spin wave spectrum by a domain wall in a narrow stripe and report the observation of a localized mode near the domain wall using the new technique of Brillouin light scattering microscopy. Time-resolved measurements are often made using a stroboscopic approach, thus missing non-periodic responses. P Möhrke et al [164009] report single-shot Kerr magnetometer measurements to observe the real time-domain wall motion in permalloy nanowires. The dynamics in magnetic disks is studied by I Neudecker et al [164010] using in-plane magnetic microwave fields for excitation. The effect of current-induced magnetization dynamics in single and double layer magnetic nanopillars is reported by N Müsgens et al [164011]. A spin-polarized charge current can modify the damping properties of spin waves in magnetic nanostructures. This is reported by V E Demidov et al [164012] using space-resolved Brillouin light scattering. They also present results regarding nonlinear spin-wave propagation and mode coupling in magnetic stripes and squares. D V Berkov and N L Gorn [164013] report on their results of nonlinear magnetization dynamics in nanodevices induced by a spin-polarized current using micromagnetic simulation. A third set of contributions focuses on dissipation phenomena ranging from a phenomenological description to the investigation of the microscopic origin(s). In a theory paper, M Fähnle et al [164014] revisit the Gilbert equation and discuss anisotropic and non-local damping of the magnetization dynamics. They derive their results by a combination of the breathing Fermi surface model with a variant of the ab initio density functional electron theory given by the magnetic force theorem. On the experimental side, S Serrano-Guisan et al [164015] address Gilbert damping in Ni81Fe19 thin films and microstructures using anisotropic magnetoresistance and pulsed inductive microwave magnetometry to measure the time-resolved precessional magnetization dynamics. The intrinsic and non-local Gilbert damping in polycrystalline Ni films is also addressed by J Walowski et al [164016] using femtosecond laser pulses. Several spin-wave modes are observed and their dissipation is studied. Non-local damping by spin currents emitted into a non-magnetic metallic layer of either vanadium, palladium or dysprosium is studied. Dissipation in small magnetic Ni81Fe19 rings is studied using Brillouin light scattering microscopy by H Schultheiss et al [164017]. They investigate the spatial profiles and the decay constants of spin-wave quasi-eigenmodes. We hope that this cluster of papers will help to stimulate and advance a better understanding of this very interesting field of ultrafast magnetization processes.

Polaron pair mediated triplet generation in polymer/fullerene blends

PubMed Central

Dimitrov, Stoichko D.; Wheeler, Scot; Niedzialek, Dorota; Schroeder, Bob C.; Utzat, Hendrik; Frost, Jarvist M.; Yao, Jizhong; Gillett, Alexander; Tuladhar, Pabitra S.; McCulloch, Iain; Nelson, Jenny; Durrant, James R.

2015-01-01

Electron spin is a key consideration for the function of organic semiconductors in light-emitting diodes and solar cells, as well as spintronic applications relying on organic magnetoresistance. A mechanism for triplet excited state generation in such systems is by recombination of electron-hole pairs. However, the exact charge recombination mechanism, whether geminate or nongeminate and whether it involves spin-state mixing is not well understood. In this work, the dynamics of free charge separation competing with recombination to polymer triplet states is studied in two closely related polymer-fullerene blends with differing polymer fluorination and photovoltaic performance. Using time-resolved laser spectroscopic techniques and quantum chemical calculations, we show that lower charge separation in the fluorinated system is associated with the formation of bound electron-hole pairs, which undergo spin-state mixing on the nanosecond timescale and subsequent geminate recombination to triplet excitons. We find that these bound electron-hole pairs can be dissociated by electric fields. PMID:25735188

Spin structure of electron subbands in (110)-grown quantum wells

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nestoklon, M. O.; Tarasenko, S. A.; Jancu, J.-M.

We present the theory of fine structure of electron states in symmetric and asymmetric zinc-blende-type quantum wells with the (110) crystallographic orientation. By combining the symmetry analysis, sp{sup 3}d{sup 5}s* tight-binding method, and envelope-function approach we obtain quantitative description of in-plane wave vector, well width and applied electric field dependencies of the zero-magnetic-field spin splitting of electron subbands and extract spin-orbit-coupling parameters.

Probing the electronic and spintronic properties of buried interfaces by extremely low energy photoemission spectroscopy

PubMed Central

Fetzer, Roman; Stadtmüller, Benjamin; Ohdaira, Yusuke; Naganuma, Hiroshi; Oogane, Mikihiko; Ando, Yasuo; Taira, Tomoyuki; Uemura, Tetsuya; Yamamoto, Masafumi; Aeschlimann, Martin; Cinchetti, Mirko

2015-01-01

Ultraviolet photoemission spectroscopy (UPS) is a powerful tool to study the electronic spin and symmetry features at both surfaces and interfaces to ultrathin top layers. However, the very low mean free path of the photoelectrons usually prevents a direct access to the properties of buried interfaces. The latter are of particular interest since they crucially influence the performance of spintronic devices like magnetic tunnel junctions (MTJs). Here, we introduce spin-resolved extremely low energy photoemission spectroscopy (ELEPS) to provide a powerful way for overcoming this limitation. We apply ELEPS to the interface formed between the half-metallic Heusler compound Co2MnSi and the insulator MgO, prepared as in state-of-the-art Co2MnSi/MgO-based MTJs. The high accordance between the spintronic fingerprint of the free Co2MnSi surface and the Co2MnSi/MgO interface buried below up to 4 nm MgO provides clear evidence for the high interface sensitivity of ELEPS to buried interfaces. Although the absolute values of the interface spin polarization are well below 100%, the now accessible spin- and symmetry-resolved wave functions are in line with the predicted existence of non-collinear spin moments at the Co2MnSi/MgO interface, one of the mechanisms evoked to explain the controversially discussed performance loss of Heusler-based MTJs at room temperature. PMID:25702631

Breaking Symmetry in Time-Dependent Electronic Structure Theory to Describe Spectroscopic Properties of Non-Collinear and Chiral Molecules

NASA Astrophysics Data System (ADS)

Goings, Joshua James

Time-dependent electronic structure theory has the power to predict and probe the ways electron dynamics leads to useful phenomena and spectroscopic data. Here we report several advances and extensions of broken-symmetry time-dependent electronic structure theory in order to capture the flexibility required to describe non-equilibrium spin dynamics, as well as electron dynamics for chiroptical properties and vibrational effects. In the first half, we begin by discussing the generalization of self-consistent field methods to the so-called two-component structure in order to capture non-collinear spin states. This means that individual electrons are allowed to take a superposition of spin-1/2 projection states, instead of being constrained to either spin-up or spin-down. The system is no longer a spin eigenfunction, and is known a a spin-symmetry broken wave function. This flexibility to break spin symmetry may lead to variational instabilities in the approximate wave function, and we discuss how these may be overcome. With a stable non-collinear wave function in hand, we then discuss how to obtain electronic excited states from the non-collinear reference, along with associated challenges in their physical interpretation. Finally, we extend the two-component methods to relativistic Hamiltonians, which is the proper setting for describing spin-orbit driven phenomena. We describe the first implementation of the explicit time propagation of relativistic two-component methods and how this may be used to capture spin-forbidden states in electronic absorption spectra. In the second half, we describe the extension of explicitly time-propagated wave functions to the simulation of chiroptical properties, namely circular dichroism (CD) spectra of chiral molecules. Natural circular dichroism, that is, CD in the absence of magnetic fields, originates in the broken parity symmetry of chiral molecules. This proves to be an efficient method for computing circular dichroism spectra for high density-of-states chiral molecules. Next, we explore the impact of allowing nuclear motion on electronic absorption spectra within the context of mixed quantum-classical dynamics. We show that nuclear motion modulates the electronic response, and this gives rise to infrared absorption as well as Raman scattering phenomena in the computed dynamic polarizability. Finally, we explore the accuracy of several perturbative approximations to the equation-of-motion coupled-cluster methods for the efficient and accurate prediction of electronic absorption spectra.

Magic angle spinning NMR with metallized rotors as cylindrical microwave resonators.

PubMed

Scott, Faith J; Sesti, Erika L; Choi, Eric J; Laut, Alexander J; Sirigiri, Jagadishwar R; Barnes, Alexander B

2018-04-19

We introduce a novel design for millimeter wave electromagnetic structures within magic angle spinning (MAS) rotors. In this demonstration, a copper coating is vacuum deposited onto the outside surface of a sapphire rotor at a thickness of 50 nm. This thickness is sufficient to reflect 197-GHz microwaves, yet not too thick as to interfere with radiofrequency fields at 300 MHz or prevent sample spinning due to eddy currents. Electromagnetic simulations of an idealized rotor geometry show a microwave quality factor of 148. MAS experiments with sample rotation frequencies of ω r /2π = 5.4 kHz demonstrate that the drag force due to eddy currents within the copper does not prevent sample spinning. Spectra of sodium acetate show resolved 13 C J-couplings of 60 Hz and no appreciable broadening between coated and uncoated sapphire rotors, demonstrating that the copper coating does not prevent shimming and high-resolution nuclear magnetic resonance spectroscopy. Additionally, 13 C Rabi nutation curves of ω 1 /2π = 103 kHz for both coated and uncoated rotors indicate no detrimental impact of the copper coating on radio frequency coupling of the nuclear spins to the sample coil. We present this metal coated rotor as a first step towards an MAS resonator. MAS resonators are expected to have a significant impact on developments in electron decoupling, pulsed dynamic nuclear polarization (DNP), room temperature DNP, DNP with low-power microwave sources, and electron paramagnetic resonance detection. Copyright © 2018 John Wiley & Sons, Ltd.

Do Gluons Carry Proton Spin? - Toward Resolving the Spin Crisis (445th Brookhaven Lecture)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bazilevsky, Alexander

2009-01-21

Just as Earth and other planets spin within the solar system, subatomic quark and gluon particles spin within the protons and neutrons that spin within the nucleus of an atom. Quantum Chromodynamics (QCD) is a theory that describes interactions between subatomic particles and it has played a defining role in understanding the spin of protons and neutrons, which make up most of the visible mass in the universe. Experiments first completed at CERN and furthered at several other laboratories around the world revealed that surprisingly, quarks and their partnering anti-quarks are responsible for only 20 to 30 percent of protonmore » spin. These findings pointed to what would become known as "spin crisis." More recent experiments at BNL's Relativistic Heavy Ion Collider (RHIC), the first collider to smash protons that are "polarized," or made to spin in the same orientation, have helped to isolate the role of the gluon's spin within the spinning proton in hopes of resolving this crisis. In his lecture, Bazilevsky will explain how data from RHIC's PHENIX and STAR detectors help to reveal the role of gluons in the proton's spin. Bazilevsky will also discuss long- and short-term plans to attain a deeper look into the proton spin structure, utilizing RHIC and its future upgrades« less

The short-lived signaling state of the photoactive yellow protein photoreceptor revealed by combined structural probes.

PubMed

Ramachandran, Pradeep L; Lovett, Janet E; Carl, Patrick J; Cammarata, Marco; Lee, Jae Hyuk; Jung, Yang Ouk; Ihee, Hyotcherl; Timmel, Christiane R; van Thor, Jasper J

2011-06-22

The signaling state of the photoactive yellow protein (PYP) photoreceptor is transiently developed via isomerization of its blue-light-absorbing chromophore. The associated structural rearrangements have large amplitude but, due to its transient nature and chemical exchange reactions that complicate NMR detection, its accurate three-dimensional structure in solution has been elusive. Here we report on direct structural observation of the transient signaling state by combining double electron electron resonance spectroscopy (DEER), NMR, and time-resolved pump-probe X-ray solution scattering (TR-SAXS/WAXS). Measurement of distance distributions for doubly spin-labeled photoreceptor constructs using DEER spectroscopy suggests that the signaling state is well ordered and shows that interspin-label distances change reversibly up to 19 Å upon illumination. The SAXS/WAXS difference signal for the signaling state relative to the ground state indicates the transient formation of an ordered and rearranged conformation, which has an increased radius of gyration, an increased maximum dimension, and a reduced excluded volume. Dynamical annealing calculations using the DEER derived long-range distance restraints in combination with short-range distance information from (1)H-(15)N HSQC perturbation spectroscopy give strong indication for a rearrangement that places part of the N-terminal domain in contact with the exposed chromophore binding cleft while the terminal residues extend away from the core. Time-resolved global structural information from pump-probe TR-SAXS/WAXS data supports this conformation and allows subsequent structural refinement that includes the combined energy terms from DEER, NMR, and SAXS/WAXS together. The resulting ensemble simultaneously satisfies all restraints, and the inclusion of TR-SAXS/WAXS effectively reduces the uncertainty arising from the possible spin-label orientations. The observations are essentially compatible with reduced folding of the I(2)' state (also referred to as the 'pB' state) that is widely reported, but indicates it to be relatively ordered and rearranged. Furthermore, there is direct evidence for the repositioning of the N-terminal region in the I(2)' state, which is structurally modeled by dynamical annealing and refinement calculations.

Velocity barrier-controlled of spin-valley polarized transport in monolayer WSe2 junction

NASA Astrophysics Data System (ADS)

Qiu, Xuejun; Lv, Qiang; Cao, Zhenzhou

2018-05-01

In this work, we have theoretically investigated the influence of velocity barrier on the spin-valley polarized transport in monolayer (ML) WSe2 junction with a large spin-orbit coupling (SOC). Both the spin-valley resolved transmission probabilities and conductance are strong dependent on the velocity barrier, as the velocity barrier decreases to 0.06, a spin-valley polarization of exceeding 90% is observed, which is distinct from the ML MoS2 owing to incommensurable SOC. In addition, the spin-valley polarization is further increased above 95% in a ML WSe2 superlattice, in particular, it's found many extraordinary velocity barrier-dependent transport gaps for multiple barrier due to evanescent tunneling. Our results may open an avenue for the velocity barrier-controlled high-efficiency spin and valley polarizations in ML WSe2-based electronic devices.

Control of Spin Wave Dynamics in Spatially Twisted Magnetic Structures

DTIC Science & Technology

2017-06-27

realize high-performance spintronic and magnetic storage devices. 15. SUBJECT TERMS nano- electronics , spin, wave, magnetic, multi-functional, device 16... electronics has required us to develop high-performance and multi-functional electronic devices driven with extremely low power consumption...Spintronics”, simultaneously utilizing the charge and the spin of electrons , provides us with solutions to essential problems for semiconductor-based

Weakly-Correlated Nature of Ferromagnetism in Nonsymmorphic CrO2 Revealed by Bulk-Sensitive Soft-X-Ray ARPES

NASA Astrophysics Data System (ADS)

Bisti, F.; Rogalev, V. A.; Karolak, M.; Paul, S.; Gupta, A.; Schmitt, T.; Güntherodt, G.; Eyert, V.; Sangiovanni, G.; Profeta, G.; Strocov, V. N.

2017-10-01

Chromium dioxide CrO2 belongs to a class of materials called ferromagnetic half-metals, whose peculiar aspect is that they act as a metal in one spin orientation and as a semiconductor or insulator in the opposite one. Despite numerous experimental and theoretical studies motivated by technologically important applications of this material in spintronics, its fundamental properties such as momentum-resolved electron dispersions and the Fermi surface have so far remained experimentally inaccessible because of metastability of its surface, which instantly reduces to amorphous Cr2O3 . In this work, we demonstrate that direct access to the native electronic structure of CrO2 can be achieved with soft-x-ray angle-resolved photoemission spectroscopy whose large probing depth penetrates through the Cr2O3 layer. For the first time, the electronic dispersions and Fermi surface of CrO2 are measured, which are fundamental prerequisites to solve the long debate on the nature of electronic correlations in this material. Since density functional theory augmented by a relatively weak local Coulomb repulsion gives an exhaustive description of our spectroscopic data, we rule out strong-coupling theories of CrO2 . Crucial for the correct interpretation of our experimental data in terms of the valence-band dispersions is the understanding of a nontrivial spectral response of CrO2 caused by interference effects in the photoemission process originating from the nonsymmorphic space group of the rutile crystal structure of CrO2 .

Resonant optical spectroscopy and coherent control of Cr4+ spin ensembles in SiC and GaN

NASA Astrophysics Data System (ADS)

Koehl, William

Spins bound to point defects have emerged as an important resource in quantum information and spintronic technologies, especially as new materials systems have been developed that enable robust and precise quantum state control via optical, electronic, or mechanical degrees of freedom. In an effort to broaden the range of materials platforms available to such defect-based quantum technologies, we have recently begun exploring optically active transition metal ion spins doped into common wide-bandgap semiconductors. The spins of such ions are derived in part from unpaired d orbital electron states, suggesting in some cases that they may be portable across multiple materials systems. This in contrast to many vacancy-related defect spins such as the diamond nitrogen vacancy center or silicon carbide divacancy, which are formed primarily from the dangling bond states of the host. Here we demonstrate ensemble optical spin polarization and time-resolved optically detected magnetic resonance (ODMR) of the S = 1 electronic ground state of chromium (Cr4+) impurities in silicon carbide (SiC) and gallium nitride (GaN). We find that these impurities possess narrow optical linewidths (<8.5 GHz at cryogenic temperatures) that allow us to optically resolve the magnetic sublevels of the spins even when probing a large ensemble of many ions simultaneously. This enables us to directly polarize and probe the Cr4+ spins using straightforward optical techniques, which we then combine with coherent microwave excitation in order to characterize the dynamical properties of the ensemble. Significantly, these near-infrared emitters also possess exceptionally weak phonon sidebands, ensuring that >73% of the overall optical emission is contained within the defects' zero-phonon lines. These characteristics make the Cr4+ ion system a promising target for further study in the ongoing effort to integrate optically active quantum states within common optoelectronic materials. In collaboration with B. Diler, S. J. Whiteley, A. Bourassa, N. T. Son, E. Janzén, and D. D. Awschalom. This work supported by AFOSR, ARO, NSF MRSEC, the Argonne LDRD Program, LiLi-NFM, and the Knut and Alice Wallenberg Foundation.

Anisotropic spin-density distribution and magnetic anisotropy of strained La1-xSrxMnO3 thin films: angle-dependent x-ray magnetic circular dichroism

NASA Astrophysics Data System (ADS)

Shibata, Goro; Kitamura, Miho; Minohara, Makoto; Yoshimatsu, Kohei; Kadono, Toshiharu; Ishigami, Keisuke; Harano, Takayuki; Takahashi, Yukio; Sakamoto, Shoya; Nonaka, Yosuke; Ikeda, Keisuke; Chi, Zhendong; Furuse, Mitsuho; Fuchino, Shuichiro; Okano, Makoto; Fujihira, Jun-ichi; Uchida, Akira; Watanabe, Kazunori; Fujihira, Hideyuki; Fujihira, Seiichi; Tanaka, Arata; Kumigashira, Hiroshi; Koide, Tsuneharu; Fujimori, Atsushi

2018-01-01

Magnetic anisotropies of ferromagnetic thin films are induced by epitaxial strain from the substrate via strain-induced anisotropy in the orbital magnetic moment and that in the spatial distribution of spin-polarized electrons. However, the preferential orbital occupation in ferromagnetic metallic La1-xSrxMnO3 (LSMO) thin films studied by x-ray linear dichroism (XLD) has always been found out-of-plane for both tensile and compressive epitaxial strain and hence irrespective of the magnetic anisotropy. In order to resolve this mystery, we directly probed the preferential orbital occupation of spin-polarized electrons in LSMO thin films under strain by angle-dependent x-ray magnetic circular dichroism (XMCD). Anisotropy of the spin-density distribution was found to be in-plane for the tensile strain and out-of-plane for the compressive strain, consistent with the observed magnetic anisotropy. The ubiquitous out-of-plane preferential orbital occupation seen by XLD is attributed to the occupation of both spin-up and spin-down out-of-plane orbitals in the surface magnetic dead layer.

Majorana surface modes of nodal topological pairings in spin-3/2 semimetals

NASA Astrophysics Data System (ADS)

Yang, Wang; Xiang, Tao; Wu, Congjun

2017-10-01

When solid state systems possess active orbital-band structures subject to spin-orbit coupling, their multicomponent electronic structures are often described in terms of effective large-spin fermion models. Their topological structures of superconductivity are beyond the framework of spin singlet and triplet Cooper pairings for spin-1/2 systems. Examples include the half-Heusler compound series of RPtBi, where R stands for a rare-earth element. Their spin-orbit coupled electronic structures are described by the Luttinger-Kohn model with effective spin-3/2 fermions and are characterized by band inversion. Recent experiments provide evidence to unconventional superconductivity in the YPtBi material with nodal spin-septet pairing. We systematically study topological pairing structures in spin-3/2 systems with the cubic group symmetries and calculate the surface Majorana spectra, which exhibit zero energy flat bands, or, cubic dispersion depending on the specific symmetry of the superconducting gap functions. The signatures of these surface states in the quasiparticle interference patterns of tunneling spectroscopy are studied, which can be tested in future experiments.

Coherent spin transfer between molecularly bridged quantum dots.

PubMed

Ouyang, Min; Awschalom, David D

2003-08-22

Femtosecond time-resolved Faraday rotation spectroscopy reveals the instantaneous transfer of spin coherence through conjugated molecular bridges spanning quantum dots of different size over a broad range of temperature. The room-temperature spin-transfer efficiency is approximately 20%, showing that conjugated molecules can be used not only as interconnections for the hierarchical assembly of functional networks but also as efficient spin channels. The results suggest that this class of structures may be useful as two-spin quantum devices operating at ambient temperatures and may offer promising opportunities for future versatile molecule-based spintronic technologies.

Layered Chalcogenides beyond Graphene: from Electronic Structure Evolution to the Spin Transport

NASA Astrophysics Data System (ADS)

Yuan, Hongtao

2014-03-01

Recent efforts on graphene-like atomic layer materials, aiming at novel electronic properties and quantum phenomena beyond graphene, have attracted much attention for potential electronics/spintronics applications. Compared to the weak spin-orbit-interaction (SOI) in graphene, metal chalcogenides MX2 have heavy 4d/5d elements with strong atomic SOI, providing a unique way for generating spin polarization based on valleytronics physics. Indeed, such a spin-polarized band structure has been demonstrated theoretically and supported by optical investigations. However, despite these exciting progresses, following two important issues in MX2 community remain elusive: 1. the quantitative band structure of MX2 compounds (where are the valleys -band maxima/minima- locating in the BZ) have not been experimentally confirmed. Especially for those cleaved ultrathin mono- and bi-layer flakes hosting most of recently-reported exotic phenomena at the 2D limit, the direct detection for band dispersion becomes of great importance for valleytronics. 2. Spin transports have seldom been reported even though such a strong SOI system can serve as an ideal platform for the spin polarization and spin transport. In this work, we started from the basic electronic structures of representative MX2, obtained by ARPES, and investigated both the band variation between these compounds and their band evolution from bulk to the monolayer limit. After having a systematic understanding on band structures, we reported a giant Zeeman-type spin-polarization generated and modulated by an external electric field in WSe2 electric-double-layer transistors. The non-magnetic approach for realizing such an intriguing spin splitting not only keeps the system time-reversally invariant but also suggests a new paradigm for manipulating the spin-degrees of freedom of electrons. Acknowledge the support from DoE, BES, Division of MSE under contract DE-AC02-76SF00515.

Persistent spin helix manipulation by optical doping of a CdTe quantum well

NASA Astrophysics Data System (ADS)

Passmann, F.; Anghel, S.; Tischler, T.; Poshakinskiy, A. V.; Tarasenko, S. A.; Karczewski, G.; Wojtowicz, T.; Bristow, A. D.; Betz, M.

2018-05-01

Time-resolved Kerr-rotation microscopy explores the influence of optical doping on the persistent spin helix in a [001]-grown CdTe quantum well at cryogenic temperatures. Electron spin-diffusion dynamics reveal a momentum-dependent effective magnetic field providing SU(2) spin-rotation symmetry, consistent with kinetic theory. The Dresselhaus and Rashba spin-orbit coupling parameters are extracted independently from rotating the spin helix with external magnetic fields applied parallel and perpendicular to the effective magnetic field. Most importantly, a nonuniform spatiotemporal precession pattern is observed. The kinetic-theory framework of spin diffusion allows for modeling of this finding by incorporating the photocarrier density into the Rashba (α) and the Dresselhaus (β3) parameters. Corresponding calculations are further validated by an excitation-density-dependent measurement. This work shows universality of the persistent spin helix by its observation in a II-VI compound and the ability to fine-tune it by optical doping.

Surface analytical characterization of Streptavidin/poly(3-hexylthiophene) bilayers for bio-electronic applications

NASA Astrophysics Data System (ADS)

Sportelli, M. C.; Picca, R. A.; Manoli, K.; Re, M.; Pesce, E.; Tapfer, L.; Di Franco, C.; Cioffi, N.; Torsi, L.

2017-10-01

The analytical performance of bioelectronic devices is highly influenced by their fabrication methods. In particular, the final architecture of field-effect transistor biosensors combining spin-cast poly(3-hexylthiophene) (P3HT) film and a biomolecule interlayer deposited on a SiO2/Si substrate can lead to the development of highly performing sensing systems, such as for the case of streptavidin (SA) used for biotin sensing. To gain a better understanding of the quality of the interfacial area, critical is the assessment of the morphological features characteristic of the adopted biolayer deposition protocol, namely: the layer-by-layer (LbL) approach and the spin coating technique. The present study relies on a combined surface spectroscopic and morphological characterization. Specifically, X-ray photoelectron spectroscopy operated in the parallel angle-resolved mode allowed the non-destructive investigation of the in-depth chemical composition of the SA film, alone or in the presence of the P3HT overlayer. Spectroscopic data were supported and corroborated by the results obtained with a Scanning Electron and a Helium Ion microscope investigation performed on the SA layer that provided relevant information on the protein structural arrangement or on its surface morphology. Clear differences emerged between the SA layers prepared by the two approaches, with the layer-by-layer deposition resulting in a smoother and better defined bio-electronic interface. Such findings support the superior analytical performance shown by bioelectronic devices based on LbL-deposited protein layers over spin coated ones.

Evidence of an Improper Displacive Phase Transition in Cd2 Re2 O7 via Time-Resolved Coherent Phonon Spectroscopy

NASA Astrophysics Data System (ADS)

Harter, J. W.; Kennes, D. M.; Chu, H.; de la Torre, A.; Zhao, Z. Y.; Yan, J.-Q.; Mandrus, D. G.; Millis, A. J.; Hsieh, D.

2018-01-01

We have used a combination of ultrafast coherent phonon spectroscopy, ultrafast thermometry, and time-dependent Landau theory to study the inversion symmetry breaking phase transition at Tc=200 K in the strongly spin-orbit coupled correlated metal Cd2 Re2 O7 . We establish that the structural distortion at Tc is a secondary effect through the absence of any softening of its associated phonon mode, which supports a purely electronically driven mechanism. However, the phonon lifetime exhibits an anomalously strong temperature dependence that decreases linearly to zero near Tc. We show that this behavior naturally explains the spurious appearance of phonon softening in previous Raman spectroscopy experiments and should be a prevalent feature of correlated electron systems with linearly coupled order parameters.

Direct characterization of photoinduced lattice dynamics in BaFe 2As 2

DOE PAGES

Gerber, S.; Kim, K. W.; Zhang, Y.; ...

2015-06-08

Ultrafast light pulses can modify electronic properties of quantum materials by perturbing the underlying, intertwined degrees of freedom. In particular, iron-based superconductors exhibit a strong coupling among electronic nematic fluctuations, spins and the lattice, serving as a playground for ultrafast manipulation. Here we use time-resolved X-ray scattering to measure the lattice dynamics of photoexcited BaFe 2As 2. On optical excitation, no signature of an ultrafast change of the crystal symmetry is observed, but the lattice oscillates rapidly in time due to the coherent excitation of an A1g mode that modulates the Fe–As–Fe bond angle. We directly quantify the coherent latticemore » dynamics and show that even a small photoinduced lattice distortion can induce notable changes in the electronic and magnetic properties. Our analysis implies that transient structural modification can be an effective tool for manipulating the electronic properties of multi-orbital systems, where electronic instabilities are sensitive to the orbital character of bands.« less

Direct characterization of photoinduced lattice dynamics in BaFe2As2

PubMed Central

Gerber, S.; Kim, K. W.; Zhang, Y.; Zhu, D.; Plonka, N.; Yi, M.; Dakovski, G. L.; Leuenberger, D.; Kirchmann, P.S.; Moore, R. G.; Chollet, M.; Glownia, J. M.; Feng, Y.; Lee, J.-S.; Mehta, A.; Kemper, A. F.; Wolf, T.; Chuang, Y.-D.; Hussain, Z.; Kao, C.-C.; Moritz, B.; Shen, Z.-X.; Devereaux, T. P.; Lee, W.-S.

2015-01-01

Ultrafast light pulses can modify electronic properties of quantum materials by perturbing the underlying, intertwined degrees of freedom. In particular, iron-based superconductors exhibit a strong coupling among electronic nematic fluctuations, spins and the lattice, serving as a playground for ultrafast manipulation. Here we use time-resolved X-ray scattering to measure the lattice dynamics of photoexcited BaFe2As2. On optical excitation, no signature of an ultrafast change of the crystal symmetry is observed, but the lattice oscillates rapidly in time due to the coherent excitation of an A1g mode that modulates the Fe–As–Fe bond angle. We directly quantify the coherent lattice dynamics and show that even a small photoinduced lattice distortion can induce notable changes in the electronic and magnetic properties. Our analysis implies that transient structural modification can be an effective tool for manipulating the electronic properties of multi-orbital systems, where electronic instabilities are sensitive to the orbital character of bands. PMID:26051704

Antisymmetric Spin-Orbit Coupling in a d-p Model on a Zigzag Chain

DOE PAGES

Sugita, Yusuke; Hayami, Satoru; Motome, Yukitoshi

2015-12-29

In this paper, we theoretically investigate how an antisymmetric spin-orbit coupling emerges in electrons moving on lattice structures which are centrosymmetric but break the spatial inversion symme- try at atomic positions. We construct an effective d-p model on the simplest lattice structure, a zigzag chain of edge-sharing octahedra, with taking into account the crystalline electric field, the spin-orbit coupling, and on-site and inter-site d-p hybridizations. We show that an effective antisymmetric spin-orbit coupling arises in the sublattice-dependent form, which results in a hidden spin polarization in the band structure. Finally, we explicitly derive the effective antisymmetric spin-orbit coupling for dmore » electrons, which not only explains the hidden spin polarization but also indicates how to enhance it.« less

Antisymmetric Spin-Orbit Coupling in a d-p Model on a Zigzag Chain

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sugita, Yusuke; Hayami, Satoru; Motome, Yukitoshi

In this paper, we theoretically investigate how an antisymmetric spin-orbit coupling emerges in electrons moving on lattice structures which are centrosymmetric but break the spatial inversion symme- try at atomic positions. We construct an effective d-p model on the simplest lattice structure, a zigzag chain of edge-sharing octahedra, with taking into account the crystalline electric field, the spin-orbit coupling, and on-site and inter-site d-p hybridizations. We show that an effective antisymmetric spin-orbit coupling arises in the sublattice-dependent form, which results in a hidden spin polarization in the band structure. Finally, we explicitly derive the effective antisymmetric spin-orbit coupling for dmore » electrons, which not only explains the hidden spin polarization but also indicates how to enhance it.« less

Optically programmable electron spin memory using semiconductor quantum dots.

PubMed

Kroutvar, Miro; Ducommun, Yann; Heiss, Dominik; Bichler, Max; Schuh, Dieter; Abstreiter, Gerhard; Finley, Jonathan J

2004-11-04

The spin of a single electron subject to a static magnetic field provides a natural two-level system that is suitable for use as a quantum bit, the fundamental logical unit in a quantum computer. Semiconductor quantum dots fabricated by strain driven self-assembly are particularly attractive for the realization of spin quantum bits, as they can be controllably positioned, electronically coupled and embedded into active devices. It has been predicted that the atomic-like electronic structure of such quantum dots suppresses coupling of the spin to the solid-state quantum dot environment, thus protecting the 'spin' quantum information against decoherence. Here we demonstrate a single electron spin memory device in which the electron spin can be programmed by frequency selective optical excitation. We use the device to prepare single electron spins in semiconductor quantum dots with a well defined orientation, and directly measure the intrinsic spin flip time and its dependence on magnetic field. A very long spin lifetime is obtained, with a lower limit of about 20 milliseconds at a magnetic field of 4 tesla and at 1 kelvin.

Identification of a new low energy 1u state in dicopper with resonant four-wave mixing.

PubMed

Visser, B; Beck, M; Bornhauser, P; Knopp, G; van Bokhoven, J A; Marquardt, R; Gourlaouen, C; Radi, P P

2017-12-07

The low energy electronic structure of the copper dimer has been re-investigated using non-linear four-wave mixing spectroscopy and high level ab initio calculations. In addition to the measurement of the previously reported A, B, and C electronic states, a new state denoted A' is identified with T 0 = 20 100.4090(16) cm -1 ( 63 Cu 2 ). Rotational analysis of the A'-X (0,0) and (1,0) transitions leads to the assignment of A' 1 u . Ab initio calculations present the first theoretical description of the low energy states of the copper dimer in Hund's case (c) and confirm the experimental assignment. The discovery of this new low energy excited state emphasizes that spin-orbit coupling is significant in states with d-hole electronic configurations and resolves a decades-long mystery in the initial assignment of the A state.

Ultrafast Multi-Level Logic Gates with Spin-Valley Coupled Polarization Anisotropy in Monolayer MoS2

PubMed Central

Wang, Yu-Ting; Luo, Chih-Wei; Yabushita, Atsushi; Wu, Kaung-Hsiung; Kobayashi, Takayoshi; Chen, Chang-Hsiao; Li, Lain-Jong

2015-01-01

The inherent valley-contrasting optical selection rules for interband transitions at the K and K′ valleys in monolayer MoS2 have attracted extensive interest. Carriers in these two valleys can be selectively excited by circularly polarized optical fields. The comprehensive dynamics of spin valley coupled polarization and polarized exciton are completely resolved in this work. Here, we present a systematic study of the ultrafast dynamics of monolayer MoS2 including spin randomization, exciton dissociation, free carrier relaxation, and electron-hole recombination by helicity- and photon energy-resolved transient spectroscopy. The time constants for these processes are 60 fs, 1 ps, 25 ps, and ~300 ps, respectively. The ultrafast dynamics of spin polarization, valley population, and exciton dissociation provides the desired information about the mechanism of radiationless transitions in various applications of 2D transition metal dichalcogenides. For example, spin valley coupled polarization provides a promising way to build optically selective-driven ultrafast valleytronics at room temperature. Therefore, a full understanding of the ultrafast dynamics in MoS2 is expected to provide important fundamental and technological perspectives. PMID:25656222

Microscopic theory for coupled atomistic magnetization and lattice dynamics

NASA Astrophysics Data System (ADS)

Fransson, J.; Thonig, D.; Bessarab, P. F.; Bhattacharjee, S.; Hellsvik, J.; Nordström, L.

2017-12-01

A coupled atomistic spin and lattice dynamics approach is developed which merges the dynamics of these two degrees of freedom into a single set of coupled equations of motion. The underlying microscopic model comprises local exchange interactions between the electron spin and magnetic moment and the local couplings between the electronic charge and lattice displacements. An effective action for the spin and lattice variables is constructed in which the interactions among the spin and lattice components are determined by the underlying electronic structure. In this way, expressions are obtained for the electronically mediated couplings between the spin and lattice degrees of freedom, besides the well known interatomic force constants and spin-spin interactions. These former susceptibilities provide an atomistic ab initio description for the coupled spin and lattice dynamics. It is important to notice that this theory is strictly bilinear in the spin and lattice variables and provides a minimal model for the coupled dynamics of these subsystems and that the two subsystems are treated on the same footing. Questions concerning time-reversal and inversion symmetry are rigorously addressed and it is shown how these aspects are absorbed in the tensor structure of the interaction fields. By means of these results regarding the spin-lattice coupling, simple explanations of ionic dimerization in double-antiferromagnetic materials, as well as charge density waves induced by a nonuniform spin structure, are given. In the final parts, coupled equations of motion for the combined spin and lattice dynamics are constructed, which subsequently can be reduced to a form which is analogous to the Landau-Lifshitz-Gilbert equations for spin dynamics and a damped driven mechanical oscillator for the ionic motion. It is important to notice, however, that these equations comprise contributions that couple these descriptions into one unified formulation. Finally, Kubo-like expressions for the discussed exchanges in terms of integrals over the electronic structure and, moreover, analogous expressions for the damping within and between the subsystems are provided. The proposed formalism and types of couplings enable a step forward in the microscopic first principles modeling of coupled spin and lattice quantities in a consistent format.

Magnetoelectroluminescence of organic heterostructures: Analytical theory and spectrally resolved measurements

NASA Astrophysics Data System (ADS)

Liu, Feilong; Kelley, Megan R.; Crooker, Scott A.; Nie, Wanyi; Mohite, Aditya D.; Ruden, P. Paul; Smith, Darryl L.

2014-12-01

The effect of a magnetic field on the electroluminescence of organic light emitting devices originates from the hyperfine interaction between the electron/hole polarons and the hydrogen nuclei of the host molecules. In this paper, we present an analytical theory of magnetoelectroluminescence for organic semiconductors. To be specific, we focus on bilayer heterostructure devices. In the case we are considering, light generation at the interface of the donor and acceptor layers results from the formation and recombination of exciplexes. The spin physics is described by a stochastic Liouville equation for the electron/hole spin density matrix. By finding the steady-state analytical solution using Bloch-Wangsness-Redfield theory, we explore how the singlet/triplet exciplex ratio is affected by the hyperfine interaction strength and by the external magnetic field. To validate the theory, spectrally resolved electroluminescence experiments on BPhen/m-MTDATA devices are analyzed. With increasing emission wavelength, the width of the magnetic field modulation curve of the electroluminescence increases while its depth decreases. These observations are consistent with the model.

Spin-dependent delay time in ferromagnet/insulator/ferromagnet heterostructures

DOE Office of Scientific and Technical Information (OSTI.GOV)

Xie, ZhengWei; Zheng Shi, De; Lv, HouXiang

2014-07-07

We study theoretically spin-dependent group delay and dwell time in ferromagnet/insulator/ferromagnet (FM/I/FM) heterostructure. The results indicate that, when the electrons with different spin orientations tunnel through the FM/I/FM junction, the spin-up process and the spin-down process are separated on the time scales. As the self-interference delay has the spin-dependent features, the variations of spin-dependent dwell-time and spin-dependent group-delay time with the structure parameters appear different features, especially, in low incident energy range. These different features show up as that the group delay times for the spin-up electrons are always longer than those for spin-down electrons when the barrier height ormore » incident energy increase. In contrast, the dwell times for the spin-up electrons are longer (shorter) than those for spin-down electrons when the barrier heights (the incident energy) are under a certain value. When the barrier heights (the incident energy) exceed a certain value, the dwell times for the spin-up electrons turn out to be shorter (longer) than those for spin-down electrons. In addition, the group delay time and the dwell time for spin-up and down electrons also relies on the comparative direction of magnetization in two FM layers and tends to saturation with the thickness of the barrier.« less

Gate tunable spin transport in graphene with Rashba spin-orbit coupling

NASA Astrophysics Data System (ADS)

Tan, Xiao-Dong; Liao, Xiao-Ping; Sun, Litao

2016-10-01

Recently, it attracts much attention to study spin-resolved transport properties in graphene with Rashba spin-orbit coupling (RSOC). One remarkable finding is that Klein tunneling in single layer graphene (SLG) with RSOC (SLG + R for short below) behaves as in bi-layer graphene (BLG). Based on the effective Dirac theory, we reconsider this tunneling problem and derive the analytical solution for the transmission coefficients. Our result shows that Klein tunneling in SLG + R and BLG exhibits completely different behaviors. More importantly, we find two new transmission selection rules in SLG + R, i.e., the single band to single band (S → S) and the single band to multiple bands (S → M) transmission regimes, which strongly depend on the relative height among Fermi level, RSOC, and potential barrier. Interestingly, in the S → S transmission regime, only normally incident electrons have capacity to pass through the barrier, while in the S → M transmission regime the angle-dependent tunneling becomes very prominent. Using the transmission coefficients, we also derive spin-resolved conductance analytically, and conductance oscillation with the increasing barrier height and zero conductance gap are found in SLG + R. The present study offers new insights and opportunities for developing graphene-based spin devices.

The spin-temperature theory of dynamic nuclear polarization and nuclear spin-lattice relaxation

NASA Technical Reports Server (NTRS)

Byvik, C. E.; Wollan, D. S.

1974-01-01

A detailed derivation of the equations governing dynamic nuclear polarization (DNP) and nuclear spin lattice relaxation by use of the spin temperature theory has been carried to second order in a perturbation expansion of the density matrix. Nuclear spin diffusion in the rapid diffusion limit and the effects of the coupling of the electron dipole-dipole reservoir (EDDR) with the nuclear spins are incorporated. The complete expression for the dynamic nuclear polarization has been derived and then examined in detail for the limit of well resolved solid effect transitions. Exactly at the solid effect transition peaks, the conventional solid-effect DNP results are obtained, but with EDDR effects on the nuclear relaxation and DNP leakage factor included. Explicit EDDR contributions to DNP are discussed, and a new DNP effect is predicted.

Effect of thermal annealing on carrier localization and efficiency of spin detection in GaAsSb epilayers grown on InP

NASA Astrophysics Data System (ADS)

Zhang, Bin; Chen, Cheng; Han, Junbo; Jin, Chuan; Chen, Jianxin; Wang, Xingjun

2018-04-01

The effect of the thermal annealing on the optical and spin properties in GaAs0.44Sb0.56 epilayers grown on InP was investigated via photoreflectance, power-dependent and time-resolved photoluminescence spectroscopy as well as optical orientation measurement. The carrier's localization and the optical spin detection efficiency increase with an increase of annealing temperature up to 600 °C. The enhancement of the spin detection efficiency is attributed to both the shortening of the electron lifetime and the prolonging of the spin lifetime as a result of the enhanced carriers' localization induced by the annealing process. Our results provided an approach to enhance spin detection efficiency of GaAsSb with its PL emission in the 1.55 μm region.

Unique spin-polarized transmission effects in a QD ring structure

NASA Astrophysics Data System (ADS)

Hedin, Eric; Joe, Yong

2010-10-01

Spintronics is an emerging field in which the spin of the electron is used for switching purposes and to communicate information. In order to obtain spin-polarized electron transmission, the Zeeman effect is employed to produce spin-split energy states in quantum dots which are embedded in the arms of a mesoscopic Aharonov-Bohm (AB) ring heterostructure. The Zeeman splitting of the QD energy levels can be induced by a parallel magnetic field, or by a perpendicular field which also produces AB-effects. The combination of these effects on the transmission resonances of the structure is studied analytically and several parameter regimes are identified which produce a high degree of spin-polarized output. Contour and line plots of the weighted spin polarization as a function of electron energy and magnetic field are presented to visualize the degree of spin-polarization. Taking advantage of these unique parameter regimes shows the potential promise of such devices for producing spin-polarized currents.

Resonant Tunneling Spin Pump

NASA Technical Reports Server (NTRS)

Ting, David Z.

2007-01-01

The resonant tunneling spin pump is a proposed semiconductor device that would generate spin-polarized electron currents. The resonant tunneling spin pump would be a purely electrical device in the sense that it would not contain any magnetic material and would not rely on an applied magnetic field. Also, unlike prior sources of spin-polarized electron currents, the proposed device would not depend on a source of circularly polarized light. The proposed semiconductor electron-spin filters would exploit the Rashba effect, which can induce energy splitting in what would otherwise be degenerate quantum states, caused by a spin-orbit interaction in conjunction with a structural-inversion asymmetry in the presence of interfacial electric fields in a semiconductor heterostructure. The magnitude of the energy split is proportional to the electron wave number. Theoretical studies have suggested the possibility of devices in which electron energy states would be split by the Rashba effect and spin-polarized currents would be extracted by resonant quantum-mechanical tunneling.

Ultrafast demagnetization enhancement in CoFeB/MgO/CoFeB magnetic tunneling junction driven by spin tunneling current.

PubMed

He, Wei; Zhu, Tao; Zhang, Xiang-Qun; Yang, Hai-Tao; Cheng, Zhao-Hua

2013-10-07

The laser-induced ultrafast demagnetization of CoFeB/MgO/CoFeB magnetic tunneling junction is exploited by time-resolved magneto-optical Kerr effect (TRMOKE) for both the parallel state (P state) and the antiparallel state (AP state) of the magnetizations between two magnetic layers. It was observed that the demagnetization time is shorter and the magnitude of demagnetization is larger in the AP state than those in the P state. These behaviors are attributed to the ultrafast spin transfer between two CoFeB layers via the tunneling of hot electrons through the MgO barrier. Our observation indicates that ultrafast demagnetization can be engineered by the hot electrons tunneling current. It opens the door to manipulate the ultrafast spin current in magnetic tunneling junctions.

DFT calculations of strain and interface effects on electronic structures and magnetic properties of L10-FePt/Ag heterojunction of GMR applications

NASA Astrophysics Data System (ADS)

Pramchu, Sittichain; Jaroenjittichai, Atchara Punya; Laosiritaworn, Yongyut

2018-03-01

In this work, density functional theory (DFT) was employed to investigate the effect of strain and interface on electronic structures and magnetic properties of L10-FePt/Ag heterojunction. Two possible interface structures of L10-FePt(001)/Ag(001), that is, interface between Fe and Ag layers (Fe/Ag) and between Pt and Ag layers (Pt/Ag), were inspected. It was found that Pt/Ag interface is more stable than Fe/Ag interface due to its lower formation energy. Further, under the lattice mismatch induced tensile strain, the enhancement of magnetism for both Fe/Ag and Pt/Ag interface structures has been found to have progressed, though the magnetic moments of "interfacial" Fe and Pt atoms have been found to have decreased. To explain this further, the local density of states (LDOS) analysis suggests that interaction between Fe (Pt) and Ag near Fe/Ag (Pt/Ag) interface leads to spin symmetry breaking of the Ag atom and hence induces magnetism magnitude. In contrast, the magnetic moments of interfacial Fe and Pt atoms reduce because of the increase in the electronic states near the Fermi level of the minority-spin electrons. In addition, the significant enhancements of the LDOS near the Fermi levels of the minority-spin electrons signify the boosting of the transport properties of the minority-spin electrons and hence the spin-dependent electron transport at this ferromagnet/metal interface. From this work, it is expected that this clarification of the interfacial magnetism may inspire new innovation on how to improve spin-dependent electron transport for enhancing the giant magnetoresistance (GMR) ratio of potential GMR-based spintronic devices.

Spin polarized surface resonance bands in single layer Bi on Ge(1 1 1)

NASA Astrophysics Data System (ADS)

Bottegoni, F.; Calloni, A.; Bussetti, G.; Camera, A.; Zucchetti, C.; Finazzi, M.; Duò, L.; Ciccacci, F.

2016-05-01

The spin features of surface resonance bands in single layer Bi on Ge(1 1 1) are studied by means of spin- and angle-resolved photoemission spectroscopy and inverse photoemission spectroscopy. We characterize the occupied and empty surface states of Ge(1 1 1) and show that the deposition of one monolayer of Bi on Ge(1 1 1) leads to the appearance of spin-polarized surface resonance bands. In particular, the C 3v symmetry, which Bi adatoms adopt on Ge(1 1 1), allows for the presence of Rashba-like occupied and unoccupied electronic states around the \\overline{\\text{M}} point of the Bi surface Brillouin zone with a giant spin-orbit constant |{α\\text{R}}| =≤ft(1.4+/- 0.1\\right) eV · Å.

Spin- and Valley-Dependent Electronic Structure in Silicene Under Periodic Potentials

NASA Astrophysics Data System (ADS)

Lu, Wei-Tao; Li, Yun-Fang; Tian, Hong-Yu

2018-03-01

We study the spin- and valley-dependent energy band and transport property of silicene under a periodic potential, where both spin and valley degeneracies are lifted. It is found that the Dirac point, miniband, band gap, anisotropic velocity, and conductance strongly depend on the spin and valley indices. The extra Dirac points appear as the voltage potential increases, the critical values of which are different for electron with different spins and valleys. Interestingly, the velocity is greatly suppressed due to the electric field and exchange field, other than the gapless graphene. It is possible to achieve an excellent collimation effect for a specific spin near a specific valley. The spin- and valley-dependent band structure can be used to adjust the transport, and perfect transmissions are observed at Dirac points. Therefore, a remarkable spin and valley polarization is achieved which can be switched effectively by the structural parameters. Importantly, the spin and valley polarizations are greatly enhanced by the disorder of the periodic potential.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mankey, G J; Morton, S A; Tobin, J G

A spin- and angle-resolved x-ray photoelectron spectrometer for the study of magnetic materials will be discussed. It consists of a turntable with electron lenses connected to a large hemispherical analyzer. A mini-Mott spin detector is fitted to the output of the hemispherical analyzer. This system, when coupled to a synchrotron radiation source will allow determination of a complete set of quantum numbers of a photoelectron. This instrument will be used to study ferromagnetic, antiferromagnetic and nonmagnetic materials. Some prototypical materials systems to be studied with this instrument system will be proposed.

Towards the Rational Design of MRI Contrast Agents: Electron Spin Relaxation Is Largely Unaffected by the Coordination Geometry of Gadolinium(III)–DOTA-Type Complexes

PubMed Central

Bean, Jonathan F.; Clarkson, Robert B.; Helm, Lothar; Moriggi, Loïck; Sherry, A. Dean

2009-01-01

Electron-spin relaxation is one of the determining factors in the efficacy of MRI contrast agents. Of all the parameters involved in determining relaxivity it remains the least well understood, particularly as it relates to the structure of the complex. One of the reasons for the poor understanding of electron-spin relaxation is that it is closely related to the ligand-field parameters of the Gd3+ ion that forms the basis of MRI contrast agents and these complexes generally exhibit a structural isomerism that inherently complicates the study of electron spin relaxation. We have recently shown that two DOTA-type ligands could be synthesised that, when coordinated to Gd3+, would adopt well defined coordination geometries and are not subject to the problems of intramolecular motion of other complexes. The EPR properties of these two chelates were studied and the results examined with theory to probe their electron-spin relaxation properties. PMID:18283704

Spin waves in micro-structured yttrium iron garnet nanometer-thick films

DOE PAGES

Jungfleisch, Matthias B.; Zhang, Wei; Jiang, Wanjun; ...

2015-03-24

Here, we investigated the spin-wave propagation in a micro-structured yttrium iron garnet waveguide of 40 nm thickness. Utilizing spatially-resolved Brillouin light scattering microscopy, an exponential decay of the spinwave amplitude of 10 μm was observed. This leads to an estimated Gilbert damping constant of α = (8.79 ± 0.73) x 10 $-$4, which is larger than damping values obtained through ferromagnetic resonance measurements in unstructured films. Furthermore, we compared the theoretically calculated spatial interference of waveguide modes to the spin-wave pattern observed experimentally by means of Brillouin light scattering spectroscopy.

A Two-Dimensional Manganese Gallium Nitride Surface Structure Showing Ferromagnetism at Room Temperature.

PubMed

Ma, Yingqiao; Chinchore, Abhijit V; Smith, Arthur R; Barral, María Andrea; Ferrari, Valeria

2018-01-10

Practical applications of semiconductor spintronic devices necessitate ferromagnetic behavior at or above room temperature. In this paper, we demonstrate a two-dimensional manganese gallium nitride surface structure (MnGaN-2D) which is atomically thin and shows ferromagnetic domain structure at room temperature as measured by spin-resolved scanning tunneling microscopy and spectroscopy. Application of small magnetic fields proves that the observed magnetic domains follow a hysteretic behavior. Two initially oppositely oriented MnGaN-2D domains are rotated into alignment with only 120 mT and remain mostly in alignment at remanence. The measurements are further supported by first-principles theoretical calculations which reveal highly spin-polarized and spin-split surface states with spin polarization of up to 95% for manganese local density of states.

Spin Polarization Transfer from a Photogenerated Radical Ion Pair to a Stable Radical Controlled by Charge Recombination.

PubMed

Horwitz, Noah E; Phelan, Brian T; Nelson, Jordan N; Mauck, Catherine M; Krzyaniak, Matthew D; Wasielewski, Michael R

2017-06-15

Photoexcitation of electron donor-acceptor molecules frequently produces radical ion pairs with well-defined initial spin-polarized states that have attracted significant interest for spintronics. Transfer of this initial spin polarization to a stable radical is predicted to depend on the rates of the radical ion pair recombination reactions, but this prediction has not been tested experimentally. In this study, a stable radical/electron donor/chromophore/electron acceptor molecule, BDPA • -mPD-ANI-NDI, where BDPA • is α,γ-bisdiphenylene-β-phenylallyl, mPD is m-phenylenediamine, ANI is 4-aminonaphthalene-1,8-dicarboximide, and NDI is naphthalene-1,4:5,8-bis(dicarboximide), was synthesized. Photoexcitation of ANI produces the triradical BDPA • -mPD +• -ANI-NDI -• in which the mPD +• -ANI-NDI -• radical ion pair is spin coupled to the BDPA • stable radical. BDPA • -mPD +• -ANI-NDI -• and its counterpart lacking the stable radical are found to exhibit spin-selective charge recombination in which the triplet radical ion pair 3 (mPD +• -ANI-NDI -• ) is in equilibrium with the 3 *NDI charge recombination product. Time-resolved EPR measurements show that this process is associated with an inversion of the sign of the polarization transferred to BDPA • over time. The polarization transfer rates are found to be strongly solvent dependent, as shifts in this equilibrium affect the spin dynamics. These results demonstrate that even small changes in electron transfer dynamics can have a large effect on the spin dynamics of photogenerated multispin systems.

VizieR Online Data Catalog: Rotational frequencies of TiO isotopologues (Lincowski+, 2016)

NASA Astrophysics Data System (ADS)

Lincowski, A. P.; Halfen, D. T.; Ziurys, L. M.

2017-03-01

Pure rotational spectra of the rare isotopologues of titanium oxide, 46TiO, 47TiO, 49TiO, and 50TiO, have been recorded using a combination of Fourier transform millimeter-wave (FTmmW) and millimeter/submillimeter direct absorption techniques in the frequency range 62-538GHz. This study is the first complete spectroscopic characterization of these species in their X3Δr ground electronic states. The isotopologues were created by the reaction of N2O or O2 and titanium vapor, produced either by laser ablation or in a Broida-type oven, and observed in the natural Ti isotopic abundances. Between 10 and 11 rotational transitions J+1<->J were measured for each species, typically in all 3 spin-orbit ladders Ω=1, 2, and 3. For 47TiO and 49TiO, hyperfine structure was resolved, originating from the titanium-47 and titanium-49 nuclear spins of I=5/2 and 7/2, respectively. For the Ω=1 and 3 components, the hyperfine structure was found to follow a classic Lande pattern, while that for Ω=2 appeared to be perturbed, likely a result of mixing with the nearby isoconfigurational a1Δ state. The spectra were analyzed with a case (a) Hamiltonian, and rotational, spin-orbit, and spin-spin parameters were determined for each species, as well as magnetic hyperfine and electric quadrupole constants for the two molecules with nuclear spins. The most abundant species, 48TiO, has been detected in circumstellar envelopes. These measurements will enable other titanium isotopologues to be studied at millimeter wavelengths, providing Ti isotope ratios that can test models of nucleosynthesis. (1 data file).

Millimeter/Submillimeter Spectroscopy of TiO (X3Δr): The Rare Titanium Isotopologues

NASA Astrophysics Data System (ADS)

Lincowski, A. P.; Halfen, D. T.; Ziurys, L. M.

2016-12-01

Pure rotational spectra of the rare isotopologues of titanium oxide, 46TiO, 47TiO, 49TiO, and 50TiO, have been recorded using a combination of Fourier transform millimeter-wave (FTmmW) and millimeter/submillimeter direct absorption techniques in the frequency range 62-538 GHz. This study is the first complete spectroscopic characterization of these species in their X 3Δ r ground electronic states. The isotopologues were created by the reaction of N2O or O2 and titanium vapor, produced either by laser ablation or in a Broida-type oven, and observed in the natural Ti isotopic abundances. Between 10 and 11 rotational transitions J + 1 ≤ftrightarrow J were measured for each species, typically in all 3 spin-orbit ladders Ω = 1, 2, and 3. For 47TiO and 49TiO, hyperfine structure was resolved, originating from the titanium-47 and titanium-49 nuclear spins of I = 5/2 and 7/2, respectively. For the Ω = 1 and 3 components, the hyperfine structure was found to follow a classic Landé pattern, while that for Ω = 2 appeared to be perturbed, likely a result of mixing with the nearby isoconfigurational a 1Δ state. The spectra were analyzed with a case (a) Hamiltonian, and rotational, spin-orbit, and spin-spin parameters were determined for each species, as well as magnetic hyperfine and electric quadrupole constants for the two molecules with nuclear spins. The most abundant species, 48TiO, has been detected in circumstellar envelopes. These measurements will enable other titanium isotopologues to be studied at millimeter wavelengths, providing Ti isotope ratios that can test models of nucleosynthesis.

Density functional perturbational orbital theory of spin polarization in electronic systems. II. Transition metal dimer complexes.

PubMed

Seo, Dong-Kyun

2007-11-14

We present a theoretical scheme for a semiquantitative analysis of electronic structures of magnetic transition metal dimer complexes within spin density functional theory (DFT). Based on the spin polarization perturbational orbital theory [D.-K. Seo, J. Chem. Phys. 125, 154105 (2006)], explicit spin-dependent expressions of the spin orbital energies and coefficients are derived, which allows to understand how spin orbitals form and change their energies and shapes when two magnetic sites are coupled either ferromagnetically or antiferromagnetically. Upon employment of the concept of magnetic orbitals in the active-electron approximation, a general mathematical formula is obtained for the magnetic coupling constant J from the analytical expression for the electronic energy difference between low-spin broken-symmetry and high-spin states. The origin of the potential exchange and kinetic exchange terms based on the one-electron picture is also elucidated. In addition, we provide a general account of the DFT analysis of the magnetic exchange interactions in compounds for which the active-electron approximation is not appropriate.

The excited spin-triplet state of a charged exciton in quantum dots.

PubMed

Molas, M R; Nicolet, A A L; Piętka, B; Babiński, A; Potemski, M

2016-09-14

We report on spectroscopic studies of resonances related to ladder of states of a charged exciton in single GaAlAs/AlAs quantum dot structures. Polarization-resolved photoluminescence, photoluminescence excitation and photon-correlation measurements were performed at low (T  =  4.2 K) temperature also in magnetic field applied in Faraday configuration. The investigated resonances are assigned to three different configurations of a positively charged exciton. Together with a singlet ground state and a conventional triplet state (involving an electron from the ground state electronic s-shell), an excited triplet state, which involved an electron from the excited electronic p-shell was identified in single dots. The appearance of an emission line related to the latter complex is due to a partially suppressed electron relaxation in the investigated dots. An analysis of this emission line allows us to scrupulously determine properties of the excited triplet state and compare them with those of the conventional triplet state. Both triplets exhibit similar patterns of anisotropic fine structure and Zeeman splitting, however their amplitudes significantly differ for those two states. Presented results emphasize the role of the symmetry of the electronic state on the properties of the triplet states of two holes  +  electron excitonic complex.

Magnetic Control of the Charge-Separated State Lifetime Realized by Covalent Attachment of a Platinum Complex.

PubMed

Miura, Tomoaki; Fujiwara, Dai; Akiyama, Kimio; Horikoshi, Takafumi; Suzuki, Shuichi; Kozaki, Masatoshi; Okada, Keiji; Ikoma, Tadaaki

2017-02-02

Dynamics of the photogenerated charge-separated (CS) state is studied for a newly synthesized molecular triad, in which the donor (D) dimethoxytriphenylamine, 1,3-bis(2-pyridylimino)isoindolate platinum (BPIPt), and the acceptor (A) naphthaldiimide are linked with a triethynylbenzene unit (BPIPt-DA). Photoexcitation of BPIPt gives rise to generation of a long-lived (∼4 μs) CS state BPIPt-D + A - , of which the lifetime is considerably increased by an applied magnetic field of 270 mT. The positive magnetic field effect (MFE) is in contrast to the negative MFE for the reference DA molecule, which indicates successful switching of the initial spin state of the CS state from singlet to triplet. Simulations of the MFE and time-resolved electron paramagnetic resonance show that spin-selective charge recombination and spin relaxation are unaffected by attachment of BPIPt. The minimum impact of heavy atom substitution on the electronic and magnetic properties has been realized by the small electronic coupling mediated by the rigid meta-triethynylbenzene.

Controlling the orientation of spin-correlated radical pairs by covalent linkage to nanoporous anodic aluminum oxide membranes.

PubMed

Chen, Hsiao-Fan; Gardner, Daniel M; Carmieli, Raanan; Wasielewski, Michael R

2013-10-07

Ordered multi-spin assemblies are required for developing solid-state molecule-based spintronics. A linear donor-chromophore-acceptor (D-C-A) molecule was covalently attached inside the 150 nm diam. nanopores of an anodic aluminum oxide (AAO) membrane. Photoexcitation of D-C-A in a 343 mT magnetic field results in sub-nanosecond, two-step electron transfer to yield the spin-correlated radical ion pair (SCRP) (1)(D(+)˙-C-A(-)˙), which then undergoes radical pair intersystem crossing (RP-ISC) to yield (3)(D(+)˙-C-A(-)˙). RP-ISC results in S-T0 mixing to selectively populate the coherent superposition states |S'> and |T'>. Microwave-induced transitions between these states and the unpopulated |T(+1)> and |T(-1)> states result in spin-polarized time-resolved EPR (TREPR) spectra. The dependence of the electron spin polarization (ESP) phase of the TREPR spectra on the orientation of the AAO membrane pores relative to the externally applied magnetic field is used to determine the overall orientation of the SCRPs within the pores at room temperature.

Silicene on Ag(1 1 1): Geometric and electronic structures of a new honeycomb material of Si

NASA Astrophysics Data System (ADS)

Takagi, Noriaki; Lin, Chun-Liang; Kawahara, Kazuaki; Minamitani, Emi; Tsukahara, Noriyuki; Kawai, Maki; Arafune, Ryuichi

2015-02-01

Silicene, a two-dimensional honeycomb sheet consisting of Si atoms, has attracted much attention as a new low-dimensional material because it gains various fascinating characteristics originating from the combination of Dirac fermion features with spin-orbit coupling. The novel properties such as the quantum spin Hall effect and the compatibility with the current Si device technologies have fueled competition to realize the silicene. This review article focuses on the geometric and electronic structures of silicene grown on Ag(1 1 1) investigated by scanning tunneling microcopy (STM), low energy electron diffraction (LEED) and density functional theory (DFT) calculations. The silicene on Ag(1 1 1) takes locally-buckled structure in which the Si atoms are displaced perpendicularly to the basal plane. As a result, several superstructures such as 4 × 4,√{ 13 } ×√{ 13 } R 13.9 °, 4 /√{ 3 } × 4 /√{ 3 } , and etc. emerge. The atomic arrangement of the 4 × 4 silicene has been determined by STM, DFT calculations and LEED dynamical analysis, while the other superstructures remain to be fully-resolved. In the 4 × 4 silicene, Si atoms are arranged to form a buckled honeycomb structure where six Si atoms of 18 Si atoms in the unit cell are displaced vertically. The displacements lead to the vertical shift of the substrate Ag atoms, indicating the non-negligible coupling at the interface between the silicene layer and the substrate. The interface coupling significantly modifies the electronic structure of the 4 × 4 silicene. No Landau level sequences were observed by scanning tunneling spectroscopy (STS) with magnetic fields applied perpendicularly to the sample surface. The DFT calculations showed that the π and π∗ bands derived from the Si 3pz are hybridized with the Ag electronic states, leading to the drastic modification in the band structure and then the absence of Dirac fermion features together with the two-dimensionality in the electronic states. These findings demonstrate that the strong coupling at the interface causes the symmetry breaking for the 4 × 4 silicene and as a result the disappearance of Dirac fermion features. The geometric and electronic structures of other superstructures are also discussed.

Layer-dependent quantum cooperation of electron and hole states in the anomalous semimetal WTe 2

DOE PAGES

Das, Pranab Kumar; Di Sante, D.; Vobornik, I.; ...

2016-02-29

The behaviour of electrons and holes in a crystal lattice is a fundamental quantum phenomenon, accounting for a rich variety of material properties. Boosted by the remarkable electronic and physical properties of two-dimensional materials such as graphene and topological insulators, transition metal dichalcogenides have recently received renewed attention. In this context, the anomalous bulk properties of semimetallic WTe 2 have attracted considerable interest. We report angle- and spin-resolved photoemission spectroscopy of WTe 2 single crystals, through which we disentangle the role of W and Te atoms in the formation of the band structure and identify the interplay of charge, spinmore » and orbital degrees of freedom. Supported by first-principles calculations and high-resolution surface topography, we also reveal the existence of a layer-dependent behaviour. The balance of electron and hole states is found only when considering at least three Te–W–Te layers, showing that the behaviour of WTe 2 is not strictly two dimensional.« less

Miniature Magnet for Electron Spin Resonance Experiments

ERIC Educational Resources Information Center

Rupp, L. W.; And Others

1976-01-01

Describes commercially available permanent magnets that have been incorporated in a compact and inexpensive structure providing both field sweep and modulation suitable for electron spin resonance at microwave frequencies. (MLH)

Hot Electron Injection into Uniaxially Strained Silicon

NASA Astrophysics Data System (ADS)

Kim, Hyun Soo

In semiconductor spintronics, silicon attracts great attention due to the long electron spin lifetime. Silicon is also one of the most commonly used semiconductor in microelectronics industry. The spin relaxation process of diamond crystal structure such as silicon is dominant by Elliot-Yafet mechanism. Yafet shows that intravalley scattering process is dominant. The conduction electron spin lifetime measured by electron spin resonance measurement and electronic measurement using ballistic hot electron method well agrees with Yafet's theory. However, the recent theory predicts a strong contribution of intervalley scattering process such as f-process in silicon. The conduction band minimum is close the Brillouin zone edge, X point which causes strong spin mixing at the conduction band. A recent experiment of electric field-induced hot electron spin relaxation also shows the strong effect of f-process in silicon. In uniaxially strained silicon along crystal axis [100], the suppression of f-process is predicted which leads to enhance electron spin lifetime. By inducing a change in crystal structure due to uniaxial strain, the six fold degeneracy becomes two fold degeneracy, which is valley splitting. As the valley splitting increases, intervalley scattering is reduced. A recent theory predicts 4 times longer electron spin lifetime in 0.5% uniaxially strained silicon. In this thesis, we demonstrate ballistic hot electron injection into silicon under various uniaxial strain. Spin polarized hot electron injection under strain is experimentally one of the most challenging part to measure conduction electron spin lifetime in silicon. Hot electron injection adopts tunnel junction which is a thin oxide layer between two conducting materials. Tunnel barrier, which is an oxide layer, is only 4 ˜ 5 nm thick. Also, two conducting materials are only tens of nanometer. Therefore, under high pressure to apply 0.5% strain on silicon, thin films on silicon substrate can be easily destroyed. In order to confirm the performance of tunnel junction, we use tunnel magnetoresistance(TMR). TMR consists of two kinds of ferromagnetic materials and an oxide layer as tunnel barrier in order to measure spin valve effect. Using silicon as a collector with Schottky barrier interface between metal and silicon, ballistic hot spin polarized electron injection into silicon is demonstrated. We also observed change of coercive field and magnetoresistance due to modification of local states in ferromagnetic materials and surface states at the interface between metal and silicon due to strain.

Pentacene appended to a TEMPO stable free radical: the effect of magnetic exchange coupling on photoexcited pentacene.

PubMed

Chernick, Erin T; Casillas, Rubén; Zirzlmeier, Johannes; Gardner, Daniel M; Gruber, Marco; Kropp, Henning; Meyer, Karsten; Wasielewski, Michael R; Guldi, Dirk M; Tykwinski, Rik R

2015-01-21

Understanding the fundamental spin dynamics of photoexcited pentacene derivatives is important in order to maximize their potential for optoelectronic applications. Herein, we report on the synthesis of two pentacene derivatives that are functionalized with the [(2,2,6,6-tetramethylpiperidin-1-yl)oxy] (TEMPO) stable free radical. The presence of TEMPO does not quench the pentacene singlet excited state, but does quench the photoexcited triplet excited state as a function of TEMPO-to-pentacene distance. Time-resolved electron paramagnetic resonance experiments confirm that triplet quenching is accompanied by electron spin polarization transfer from the pentacene excited state to the TEMPO doublet state in the weak coupling regime.

Atomic-scale observation of structural and electronic orders in the layered compound α-RuCl3

PubMed Central

Ziatdinov, M.; Banerjee, A.; Maksov, A.; Berlijn, T.; Zhou, W.; Cao, H. B.; Yan, J.-Q.; Bridges, C. A.; Mandrus, D. G.; Nagler, S. E.; Baddorf, A. P.; Kalinin, S. V.

2016-01-01

A pseudospin-1/2 Mott phase on a honeycomb lattice is proposed to host the celebrated two-dimensional Kitaev model which has an elusive quantum spin liquid ground state, and fascinating physics relevant to the development of future templates towards topological quantum bits. Here we report a comprehensive, atomically resolved real-space study by scanning transmission electron and scanning tunnelling microscopies on a novel layered material displaying Kitaev physics, α-RuCl3. Our local crystallography analysis reveals considerable variations in the geometry of the ligand sublattice in thin films of α-RuCl3 that opens a way to realization of a spatially inhomogeneous magnetic ground state at the nanometre length scale. Using scanning tunnelling techniques, we observe the electronic energy gap of ≈0.25 eV and intra-unit cell symmetry breaking of charge distribution in individual α-RuCl3 surface layer. The corresponding charge-ordered pattern has a fine structure associated with two different types of charge disproportionation at Cl-terminated surface. PMID:27941761

Atomic-scale observation of structural and electronic orders in the layered compound α-RuCl3.

PubMed

Ziatdinov, M; Banerjee, A; Maksov, A; Berlijn, T; Zhou, W; Cao, H B; Yan, J-Q; Bridges, C A; Mandrus, D G; Nagler, S E; Baddorf, A P; Kalinin, S V

2016-12-12

A pseudospin-1/2 Mott phase on a honeycomb lattice is proposed to host the celebrated two-dimensional Kitaev model which has an elusive quantum spin liquid ground state, and fascinating physics relevant to the development of future templates towards topological quantum bits. Here we report a comprehensive, atomically resolved real-space study by scanning transmission electron and scanning tunnelling microscopies on a novel layered material displaying Kitaev physics, α-RuCl 3 . Our local crystallography analysis reveals considerable variations in the geometry of the ligand sublattice in thin films of α-RuCl 3 that opens a way to realization of a spatially inhomogeneous magnetic ground state at the nanometre length scale. Using scanning tunnelling techniques, we observe the electronic energy gap of ≈0.25 eV and intra-unit cell symmetry breaking of charge distribution in individual α-RuCl 3 surface layer. The corresponding charge-ordered pattern has a fine structure associated with two different types of charge disproportionation at Cl-terminated surface.

Atomic-scale observation of structural and electronic orders in the layered compound α-RuCl 3

DOE PAGES

Ziatdinov, Maxim A.; Banerjee, Arnab; Maksov, Artem B.; ...

2016-12-12

A pseudospin-1/2 Mott phase on a honeycomb lattice is proposed to host the celebrated two-dimensional Kitaev model which has an elusive quantum spin liquid ground state, and fascinating physics relevant to the development of future templates towards topological quantum bits. Here we report a comprehensive, atomically resolved real-space study by scanning transmission electron and scanning tunnelling microscopies on a novel layered material displaying Kitaev physics, -RuCl3. Our local crystallography analysis reveals considerable variations in the geometry of the ligand sublattice in thin films of -RuCl3 that opens a way to realization of a spatially inhomogeneous magnetic ground state at themore » nanometre length scale. Using scanning tunnelling techniques, we observe the electronic energy gap of 0.25 eV and intra-unit cell symmetry breaking of charge distribution in individual -RuCl3 surface layer. The corresponding charge-ordered pattern has a fine structure associated with two different types of charge disproportionation at Cl-terminated surface.« less

Electronic transitions of tantalum monofluoride

NASA Astrophysics Data System (ADS)

Ng, K. F.; Zou, Wenli; Liu, Wenjian; Cheung, A. S.-C.

2017-03-01

The electronic transition spectrum of the tantalum monofluoride (TaF) molecule in the spectral region between 448 and 560 nm has been studied using the technique of laser-ablation/reaction free jet expansion and laser induced fluorescence spectroscopy. The TaF molecule was produced by reacting laser-ablated tantalum atoms with sulfur hexafluoride gas seeded in argon. Twenty-two vibrational bands with resolved rotational structure have been recorded and analyzed, which were organized into seven electronic transitions. The X3Σ-(0+) state has been identified to be the ground state and the determined equilibrium bond length, re, and vibrational frequency, ωe, are 1.8184 Å and 700.1 cm-1, respectively. The low-lying Λ-S states and Ω sub-states of TaF were also theoretically studied at the MRCISD+Q level of theory with spin-orbit coupling. The Ω = 0+ and 2 sub-states from the -3Σ and 3Φ state have been found to be the ground and the first excited states, respectively, which agrees well with our experimental determinations. This work represents the first experimental investigation of the molecular structure of the TaF molecule.

Controlling Spin Coherence with Semiconductor Nanostructures

NASA Astrophysics Data System (ADS)

Awschalom, David D.

We present two emerging opportunities for manipulating and communicating coherent spin states in semiconductors. First, we show that semiconductor microcavities offer unique means of controlling light-matter interactions in confined geometries, resulting in a wide range of applications in optical communications and inspiring proposals for quantum information processing and computational schemes. Studies of spin dynamics in microcavities — a new and promising research field — have revealed novel effects such as polarization beats, stimulated spin scattering, and giant Faraday rotation. Here, we study the electron spin dynamics in optically-pumped GaAs microdisk lasers with quantum wells and interface-fluctuation quantum dots in the active region. In particular, we examine how the electron spin dynamics are modified by the stimulated emission in the disks, and observe an enhancement of the spin coherence time when the optical excitation is in resonance with a high quality (Q ~ 5000) lasing mode.1 This resonant enhancement, contrary to expectations from the observed trend in the carrier recombination time, is then manipulated by altering the cavity design and dimensions. In analogy to devices based on excitonic coherence, this ability to engineer coherent interactions between electron spins and photons may provide novel pathways towards spin dependent quantum optoelectronics. In a second example, the nitrogen-vacancy (N-V) center in diamond has garnered interest as a room-temperature solid-state system not only for exploring electronic and nuclear spin phenomena but also as a candidate for spin-based quantum information processing. Spin coherence times of up to 50 microseconds have been reported for ensembles of N-V centers and a two-qubit gate utilizing the electron spin of a N-V center and the nuclear spin of a nearby C-13 atom has been demonstrated. Here, we present experiments using angle-resolved magneto-photoluminescence microscopy to investigate anisotropic spin interactions of single N-V centers in diamond at room temperature.2 Negative peaks in the photoluminescence intensity are observed as a function of both magnetic field magnitude and angle, and can be explained by coherent spin precession and anisotropic relaxation at spin-level anticrossings. Additionally, precise field alignment with the symmetry axis of a single N-V center reveals the resonant magnetic dipolar coupling of a single "bright" electron spin of an N-V center to small numbers of "dark" spins of nitrogen defects in its immediate vicinity, which are otherwise undetected by photoluminescence. Most recently, we are exploring the possibility of utilizing this magnetic dipole coupling between bright and dark spins to couple two spatially separated single N-V center spins by means of intermediate nitrogen spins. Note from Publisher: This article contains the abstract only.

Time-resolved nonlinear optics in strongly correlated insulators

NASA Astrophysics Data System (ADS)

Dodge, J. Steven

2000-03-01

Transition metal oxides form the basis for much of our understanding of Mott insulators, and have enjoyed a renaissance of interest since the discovery of high temperature superconductivity in the cuprates. They are characterized by complex interactions among spin, lattice, orbital and charge degrees of freedom, which lead to dynamical behavior on time scales ranging from femtoseconds to microseconds. We have applied time resolved nonlinear optical spectroscopy to probe these dynamics. In one well-studied antiferromagnetic insulator, Cr_2O_3, we observed spin-wave dynamics on a picosecond time scale by performing pump-probe spectroscopy of the exciton-magnon transition(J. S. Dodge, et al.), Phys. Rev. Lett. 83, 4650 (1999).. At excitation densities ~ 10-3/Cr, a lineshape associated with the exciton-magnon absorption appears in the pump-probe spectrum. We assign this nonlinearity to a time-dependent renormalization of the magnon band structure, which in turn modifies the lineshape of the exciton-magnon transition. At long time delays, this assignment agrees semiquantitatively with calculations based on spin-wave theory. However, the initial population at the zone-boundary induces surprisingly little renormalization effect, indicating that spin-wave theory is insufficient to describe our observations in this regime. The renormalization lineshape grows on a time scale of ~ 50 ps, which we associate with the decay of the photoexcited, nonequilibrium population of zone-boundary spin-waves into a thermalized population of zone-center spin-waves. We have also performed a study of the linear and nonlinear optical properties of Sr_2CuO_2Cl_2, an insulating, two-dimensional cuprate. In the nonlinear optical experiments, we have performed pump-probe spectroscopy over a 1 eV spectral range, varying both the pump and the probe energy. We observe a pump-probe lineshape which varies considerably as a function of pump energy and temperature, and which differs sharply from those typically observed in band insulators. At low-temperatures, in particular, we observe an overall increase of spectral weight in our probe range, indicating that states are shifting over an energy scale larger than 1 eV. We attribute this behavior to the strongly correlated nature of the electronic structure in this material. Studies of the elementary excitations in other magnetic oxides, currently in progress, will be discussed.

Roles of nonlocal conductivity on spin Hall angle measurement

NASA Astrophysics Data System (ADS)

Chen, Kai; Zhang, Shufeng

2017-10-01

Spin Hall angle characterizes the rate of spin-charge current conversion and it has become one of the most important material parameters for spintronics physics and device application. A long-standing controversy is that the spin Hall angles for a given material measured by spin pumping and by spin Hall torque experiments are inconsistent and they could differ by as much as an order of magnitude. By using the linear response spin transport theory, we explicitly formulate the relation between the spin Hall angle and measured variables in different experiments. We find that the nonlocal conductivity inherited in the layered structure plays a key role to resolve conflicting values of the spin Hall angle. We provide a generalized scheme for extracting spin transport coefficients from experimental data.

Magnetization reversal of the domain structure in the anti-perovskite nitride Co{sub 3}FeN investigated by high-resolution X-ray microscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hajiri, T., E-mail: t.hajiri@numse.nagoya-u.ac.jp; Kuroki, Y.; Ando, H.

2016-05-14

We performed X-ray magnetic circular dichroism (XMCD) photoemission electron microscopy imaging to reveal the magnetic domain structure of anti-perovskite nitride Co{sub 3}FeN exhibiting a negative spin polarization. In square and disc patterns, we systematically and quantitatively determined the statistics of the stable states as a function of geometry. By direct imaging during the application of a magnetic field, we revealed the magnetic reversal process in a spatially resolved manner. We compared the hysteresis on the continuous area and the square patterns from the magnetic field-dependent XMCD ratio, which can be explained as resulting from the effect of the shape anisotropy,more » present in nanostructured thin films.« less

Rashba-type spin splitting and the electronic structure of ultrathin Pb/MoTe2 heterostructure

NASA Astrophysics Data System (ADS)

Du, X.; Wang, Z. Y.; Huang, G. Q.

2016-11-01

The spin-polarized band structures of the Pb(111)/MoTe2 heterostructure are studied by the first-principles calculations. Due to strong spin-orbit coupling and space inversion asymmetry, large Rashba spin splitting of electronic bands appears in this hybrid system. The spin splitting is completely out-of-plane and opposite at \\bar{K} and {\\bar{K}}\\prime points. Rashba spin splitting also appears along the in-plane momentum direction around the \\bar{{{Γ }}} point due to the existence of surface potential gradient induced by charge transfer at interface. Furthermore, our calculations show that the spin-polarized bands closely approach the Fermi level in Pb/MoTe2 heterostructure, showing that this heterostructure may be a good candidate in valleytronics or spintronics.

Electron refrigeration in hybrid structures with spin-split superconductors

NASA Astrophysics Data System (ADS)

Rouco, M.; Heikkilä, T. T.; Bergeret, F. S.

2018-01-01

Electron tunneling between superconductors and normal metals has been used for an efficient refrigeration of electrons in the latter. Such cooling is a nonlinear effect and usually requires a large voltage. Here we study the electron cooling in heterostructures based on superconductors with a spin-splitting field coupled to normal metals via spin-filtering barriers. The cooling power shows a linear term in the applied voltage. This improves the coefficient of performance of electron refrigeration in the normal metal by shifting its optimum cooling to lower voltage, and also allows for cooling the spin-split superconductor by reverting the sign of the voltage. We also show how tunnel coupling spin-split superconductors with regular ones allows for a highly efficient refrigeration of the latter.

Asymmetrical edges induced strong current-polarization in embedded graphene nanoribbons

NASA Astrophysics Data System (ADS)

Li, Kuanhong; Zhang, Xiang-Hua

2018-05-01

We investigate the electronic structures and transport properties of the embedded zigzag graphene nanoribbon (E-ZGNR) in hexagonal boron nitride trenches, which are achievable in recent experiments. Our first principles results show that the E-ZGNR has a significant enhanced conductivity relative to common ZGNRs due to the existence of asymmetrical edge structures. Moreover, only one spin-orientation electrons possess a widely opened band gap at the magnetic ground state with anti-ferromagnetic configuration, resulting in a full current-polarization at low bias region. Our findings indicate that the state-of-the-art embedding technology is quite useful for tuning the electronic structure of ZGNR and building possible spin injection and spin filter devices in spintronics.

Probing Chemical Bonding and Electronic Structures in ThO- by Anion Photoelectron Imaging and Theoretical Calculations.

PubMed

Li, Yanli; Zou, Jinghan; Xiong, Xiao-Gen; Su, Jing; Xie, Hua; Fei, Zejie; Tang, Zichao; Liu, Hongtao

2017-03-16

Because of renewed research on thorium-based molten salt reactors, there is growing demand and interest in enhancing the knowledge of thorium chemistry both experimentally and theoretically. Compared with uranium, thorium has few chemical studies reported up to the present. Here we report the vibrationally resolved photoelectron imaging of the thorium monoxide anion. The electron affinity of ThO is first reported to be 0.707 ± 0.020 eV. Vibrational frequencies of the ThO molecule and its anion are determined from Franck-Condon simulation. Spectroscopic evidence is obtained for the two-electron transition in ThO - , indicating the strong electron correlation among the (7s σ ) 2 (6d δ ) 1 electrons in ThO - and the (7s σ ) 2 electrons in ThO. These findings are explained by using quantum-chemical calculations including spin-orbit coupling, and the chemical bonding of gaseous ThO molecules is analyzed. The present work will enrich our understanding of bonding capacities with the 6d valence shell.

Spin-polarization dependent carrier recombination dynamics and spin relaxation mechanism in asymmetrically doped (110) n-GaAs quantum wells

NASA Astrophysics Data System (ADS)

Teng, Lihua; Jiang, Tianran; Wang, Xia; Lai, Tianshu

2018-05-01

Carrier recombination and electron spin relaxation dynamics in asymmetric n-doped (110) GaAs/AlGaAs quantum wells are investigated with time-resolved pump-probe spectroscopy. The experiment results reveal that the measured carrier recombination time depends strongly on the polarization of pump pulse. With the same pump photon flux densities, the recombination time of spin-polarized carriers is always longer than that of the spin-balanced carriers except at low pump photon flux densities, this anomaly originates from the polarization-sensitive nonlinear absorption effect. Differing from the traditional views, in the low carrier density regime, the D'yakonov-Perel' (DP) mechanism can be more important than the Bir-Aronov-Pikus (BAP) mechanism, since the DP mechanism takes effect, the spin relaxation time in (110) GaAs QWs is shortened obviously via asymmetric doping.

Dual nature of 3 d electrons in YbT 2 Zn 20 (T = Co; Fe) evidenced by electron spin resonance

DOE PAGES

Ivanshin, V. A.; Litvinova, T. O.; Gimranova, K.; ...

2015-03-18

The electron spin resonance experiments were carried out in the single crystals YbFe 2Zn 20. The observed spin dynamics is compared with that in YbCo 2Zn 20 and Yb 2Co 12P 7 as well as with the data of inelastic neutron scattering and electronic band structure calculations. Our results provide direct evidence that 3d electrons are itinerant in YbFe 2Zn 20 and localized in YbCo 2Zn 20. Possible connection between spin paramagnetism of dense heavy fermion systems, quantum criticality effects, and ESR spectra is discussed.

Diradicals acting through diamagnetic phenylene vinylene bridges: Raman spectroscopy as a probe to characterize spin delocalization

DOE Office of Scientific and Technical Information (OSTI.GOV)

González, Sandra Rodríguez; Nieto-Ortega, Belén; González Cano, Rafael C.

2014-04-28

We present a complete Raman spectroscopic study in two structurally well-defined diradical species of different lengths incorporating oligo p-phenylene vinylene bridges between two polychlorinated triphenylmethyl radical units, a disposition that allows sizeable conjugation between the two radicals through and with the bridge. The spectroscopic data are interpreted and supported by quantum chemical calculations. We focus the attention on the Raman frequency changes, interpretable in terms of: (i) bridge length (conjugation length); (ii) bridge conformational structure; and (iii) electronic coupling between the terminal radical units with the bridge and through the bridge, which could delineate through-bond spin polarization, or spin delocalization.more » These items are addressed by using the “oligomer approach” in conjunction with pressure and temperature dependent Raman spectroscopic data. In summary, we have attempted to translate the well-known strategy to study the electron (charge) structure of π−conjugated molecules by Raman spectroscopy to the case of electron (spin) interactions via the spin delocalization mechanism.« less

Geometric phase effects in the ultracold D + HD $$ \\rightarrow $$ D + HD and D + HD $$\\leftrightarrow $$ H + D 2 reactions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kendrick, Brian Kent; Hazra, Jisha; Balakrishnan, Naduvaluth

The results of accurate quantum reactive scattering calculations for the D + HD(v = 4, j = 0)more » $$\\to $$ D + HD($$v^{\\prime} $$, $$j^{\\prime} $$), D + HD(v = 4, j = 0) $$\\to $$ H + D2($$v^{\\prime} $$, $$j^{\\prime} $$) and H + D2(v = 4, j = 0) $$\\to $$ D + HD($$v^{\\prime} $$, $$j^{\\prime} $$) reactions are presented for collision energies between $$1\\,\\mu {\\rm{K}}$$ and $$100\\,{\\rm{K}}$$. The ab initio BKMP2 PES for the ground electronic state of H3 is used and all values of total angular momentum between $J=0-4$ are included. The general vector potential approach is used to include the geometric phase. The rotationally resolved, vibrationally resolved, and total reaction rate coefficients are reported as a function of collision energy. Rotationally resolved differential cross sections are also reported as a function of collision energy and scattering angle. Large geometric phase effects appear in the ultracold reaction rate coefficients which result in a significant enhancement or suppression of the rate coefficient (up to 3 orders of magnitude) relative to calculations which ignore the geometric phase. The results are interpreted using a new quantum interference mechanism which is unique to ultracold collisions. Significant effects of the geometric phase also appear in the rotationally resolved differential cross sections which lead to a very different oscillatory structure in both energy and scattering angle. Several shape resonances occur in the 1–$$10\\,{\\rm{K}}$$ energy range and the geometric phase is shown to significantly alter the predicted resonance spectrum. The geometric phase effects and ultracold rate coefficients depend sensitively on the nuclear spin. Furthermore, experimentalists may be able to control the reaction by the selection of a particular nuclear spin state.« less

Geometric phase effects in the ultracold D + HD $$ \\rightarrow $$ D + HD and D + HD $$\\leftrightarrow $$ H + D 2 reactions

DOE PAGES

Kendrick, Brian Kent; Hazra, Jisha; Balakrishnan, Naduvaluth

2016-12-15

The results of accurate quantum reactive scattering calculations for the D + HD(v = 4, j = 0)more » $$\\to $$ D + HD($$v^{\\prime} $$, $$j^{\\prime} $$), D + HD(v = 4, j = 0) $$\\to $$ H + D2($$v^{\\prime} $$, $$j^{\\prime} $$) and H + D2(v = 4, j = 0) $$\\to $$ D + HD($$v^{\\prime} $$, $$j^{\\prime} $$) reactions are presented for collision energies between $$1\\,\\mu {\\rm{K}}$$ and $$100\\,{\\rm{K}}$$. The ab initio BKMP2 PES for the ground electronic state of H3 is used and all values of total angular momentum between $J=0-4$ are included. The general vector potential approach is used to include the geometric phase. The rotationally resolved, vibrationally resolved, and total reaction rate coefficients are reported as a function of collision energy. Rotationally resolved differential cross sections are also reported as a function of collision energy and scattering angle. Large geometric phase effects appear in the ultracold reaction rate coefficients which result in a significant enhancement or suppression of the rate coefficient (up to 3 orders of magnitude) relative to calculations which ignore the geometric phase. The results are interpreted using a new quantum interference mechanism which is unique to ultracold collisions. Significant effects of the geometric phase also appear in the rotationally resolved differential cross sections which lead to a very different oscillatory structure in both energy and scattering angle. Several shape resonances occur in the 1–$$10\\,{\\rm{K}}$$ energy range and the geometric phase is shown to significantly alter the predicted resonance spectrum. The geometric phase effects and ultracold rate coefficients depend sensitively on the nuclear spin. Furthermore, experimentalists may be able to control the reaction by the selection of a particular nuclear spin state.« less

A Ku band pulsed electron paramagnetic resonance spectrometer using an arbitrary waveform generator for quantum control experiments at millikelvin temperatures

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yap, Yung Szen, E-mail: yungszen@utm.my; Faculty of Science, Universiti Teknologi Malaysia, 81310 UTM Johor Bahru, Johor; Tabuchi, Yutaka

2015-06-15

We present a 17 GHz (Ku band) arbitrary waveform pulsed electron paramagnetic resonance spectrometer for experiments down to millikelvin temperatures. The spectrometer is located at room temperature, while the resonator is placed either in a room temperature magnet or inside a cryogen-free dilution refrigerator; the operating temperature range of the dilution unit is from ca. 10 mK to 8 K. This combination provides the opportunity to perform quantum control experiments on electron spins in the pure-state regime. At 0.6 T, spin echo experiments were carried out using γ-irradiated quartz glass from 1 K to 12.3 mK. With decreasing temperatures, wemore » observed an increase in spin echo signal intensities due to increasing spin polarizations, in accordance with theoretical predictions. Through experimental data fitting, thermal spin polarization at 100 mK was estimated to be at least 99%, which was almost pure state. Next, to demonstrate the ability to create arbitrary waveform pulses, we generate a shaped pulse by superposing three Gaussian pulses of different frequencies. The resulting pulse was able to selectively and coherently excite three different spin packets simultaneously—a useful ability for analyzing multi-spin system and for controlling a multi-qubit quantum computer. By applying this pulse to the inhomogeneously broadened sample, we obtain three well-resolved excitations at 8 K, 1 K, and 14 mK.« less

Focus: Two-dimensional electron-electron double resonance and molecular motions: The challenge of higher frequencies.

PubMed

Franck, John M; Chandrasekaran, Siddarth; Dzikovski, Boris; Dunnam, Curt R; Freed, Jack H

2015-06-07

The development, applications, and current challenges of the pulsed ESR technique of two-dimensional Electron-Electron Double Resonance (2D ELDOR) are described. This is a three-pulse technique akin to 2D Exchange Nuclear Magnetic Resonance, but involving electron spins, usually in the form of spin-probes or spin-labels. As a result, it required the extension to much higher frequencies, i.e., microwaves, and much faster time scales, with π/2 pulses in the 2-3 ns range. It has proven very useful for studying molecular dynamics in complex fluids, and spectral results can be explained by fitting theoretical models (also described) that provide a detailed analysis of the molecular dynamics and structure. We discuss concepts that also appear in other forms of 2D spectroscopy but emphasize the unique advantages and difficulties that are intrinsic to ESR. Advantages include the ability to tune the resonance frequency, in order to probe different motional ranges, while challenges include the high ratio of the detection dead time vs. the relaxation times. We review several important 2D ELDOR studies of molecular dynamics. (1) The results from a spin probe dissolved in a liquid crystal are followed throughout the isotropic → nematic → liquid-like smectic → solid-like smectic → crystalline phases as the temperature is reduced and are interpreted in terms of the slowly relaxing local structure model. Here, the labeled molecule is undergoing overall motion in the macroscopically aligned sample, as well as responding to local site fluctuations. (2) Several examples involving model phospholipid membranes are provided, including the dynamic structural characterization of the boundary lipid that coats a transmembrane peptide dimer. Additionally, subtle differences can be elicited for the phospholipid membrane phases: liquid disordered, liquid ordered, and gel, and the subtle effects upon the membrane, of antigen cross-linking of receptors on the surface of plasma membrane, vesicles can be observed. These 2D ELDOR experiments are performed as a function of mixing time, Tm, i.e., the time between the second and third π/2 pulses, which provides a third dimension. In fact, a fourth dimension may be added by varying the ESR frequency/magnetic field combination. Therefore, (3) it is shown how continuous-wave multifrequency ESR studies enable the decomposition of complex dynamics of, e.g., proteins by virtue of their respective time scales. These studies motivate our current efforts that are directed to extend 2D ELDOR to higher frequencies, 95 GHz in particular (from 9 and 17 GHz), in order to enable multi-frequency 2D ELDOR. This required the development of quasi-optical methods for performing the mm-wave experiments, which are summarized. We demonstrate state-of-the-art 95 GHz 2D ELDOR spectroscopy through its ability to resolve the two signals from a spin probe dissolved in both the lipid phase and the coexisting aqueous phase. As current 95 GHz experiments are restricted by limited spectral coverage of the π/2 pulse, as well as the very short T2 relaxation times of the electron spins, we discuss how these limitations are being addressed.

Focus: Two-dimensional electron-electron double resonance and molecular motions: The challenge of higher frequencies

NASA Astrophysics Data System (ADS)

Franck, John M.; Chandrasekaran, Siddarth; Dzikovski, Boris; Dunnam, Curt R.; Freed, Jack H.

2015-06-01

The development, applications, and current challenges of the pulsed ESR technique of two-dimensional Electron-Electron Double Resonance (2D ELDOR) are described. This is a three-pulse technique akin to 2D Exchange Nuclear Magnetic Resonance, but involving electron spins, usually in the form of spin-probes or spin-labels. As a result, it required the extension to much higher frequencies, i.e., microwaves, and much faster time scales, with π/2 pulses in the 2-3 ns range. It has proven very useful for studying molecular dynamics in complex fluids, and spectral results can be explained by fitting theoretical models (also described) that provide a detailed analysis of the molecular dynamics and structure. We discuss concepts that also appear in other forms of 2D spectroscopy but emphasize the unique advantages and difficulties that are intrinsic to ESR. Advantages include the ability to tune the resonance frequency, in order to probe different motional ranges, while challenges include the high ratio of the detection dead time vs. the relaxation times. We review several important 2D ELDOR studies of molecular dynamics. (1) The results from a spin probe dissolved in a liquid crystal are followed throughout the isotropic → nematic → liquid-like smectic → solid-like smectic → crystalline phases as the temperature is reduced and are interpreted in terms of the slowly relaxing local structure model. Here, the labeled molecule is undergoing overall motion in the macroscopically aligned sample, as well as responding to local site fluctuations. (2) Several examples involving model phospholipid membranes are provided, including the dynamic structural characterization of the boundary lipid that coats a transmembrane peptide dimer. Additionally, subtle differences can be elicited for the phospholipid membrane phases: liquid disordered, liquid ordered, and gel, and the subtle effects upon the membrane, of antigen cross-linking of receptors on the surface of plasma membrane, vesicles can be observed. These 2D ELDOR experiments are performed as a function of mixing time, Tm, i.e., the time between the second and third π/2 pulses, which provides a third dimension. In fact, a fourth dimension may be added by varying the ESR frequency/magnetic field combination. Therefore, (3) it is shown how continuous-wave multifrequency ESR studies enable the decomposition of complex dynamics of, e.g., proteins by virtue of their respective time scales. These studies motivate our current efforts that are directed to extend 2D ELDOR to higher frequencies, 95 GHz in particular (from 9 and 17 GHz), in order to enable multi-frequency 2D ELDOR. This required the development of quasi-optical methods for performing the mm-wave experiments, which are summarized. We demonstrate state-of-the-art 95 GHz 2D ELDOR spectroscopy through its ability to resolve the two signals from a spin probe dissolved in both the lipid phase and the coexisting aqueous phase. As current 95 GHz experiments are restricted by limited spectral coverage of the π/2 pulse, as well as the very short T2 relaxation times of the electron spins, we discuss how these limitations are being addressed.

Coexistence of perfect spin filtering for entangled electron pairs and high magnetic storage efficiency in one setup.

PubMed

Ji, T T; Bu, N; Chen, F J; Tao, Y C; Wang, J

2016-04-14

For Entangled electron pairs superconducting spintronics, there exist two drawbacks in existing proposals of generating entangled electron pairs. One is that the two kinds of different spin entangled electron pairs mix with each other. And the other is a low efficiency of entanglement production. Herein, we report the spin entanglement state of the ferromagnetic insulator (FI)/s-wave superconductor/FI structure on a narrow quantum spin Hall insulator strip. It is shown that not only the high production of entangled electron pairs in wider energy range, but also the perfect spin filtering of entangled electron pairs in the context of no highly spin-polarized electrons, can be obtained. Moreover, the currents for the left and right leads in the antiferromagnetic alignment both can be zero, indicating 100% tunnelling magnetoresistance with highly magnetic storage efficiency. Therefore, the spin filtering for entangled electron pairs and magnetic storage with high efficiencies coexist in one setup. The results may be experimentally demonstrated by measuring the tunnelling conductance and the noise power.

Magnetic Excitations of Stripes

NASA Astrophysics Data System (ADS)

Yao, Daoxin; Carlson, Erica; Campbell, David

2005-03-01

Competing tendencies in electronic systems with strong correlations can lead to spontaneous nanoscale structure, pattern formation, and even long-range spatial order. There has been continued interest in various ``stripe'' phases of electrons, as well as more recent interest in possible ``checkerboard'' patterns. New experimental techniques allow for the extraction of detailed and reproducible neutron scattering spectra in copper oxide superconductors and related nickelate compounds. We discuss the magnetic excitations of well-ordered stripe phases, including the high energy magnetic excitations of recent interest and possible connections to the ``resonance peak'' in cuprate superconductors. Using a suitably parametrized Heisenberg model and spin wave theory, we study a variety of possible stripe configurations, including vertical, diagonal, staircase, and zigzag stripes. We calculate the expected neutron scattering intensities as a function of energy and momentum. Constant energy cuts at high energy often reveal a square-like scattering pattern, and occasionally a circular pattern. Bond-centered stripes have weight gathered near (pi,pi) at low energy, indicating that only part of the spin wave cone is expected to be resolvable experimentally. In addition, we present a litmus test for experimentally distinguishing bond-centered stripes from site-centered stripes using low energy data.

Local density of states in two-dimensional topological superconductors under a magnetic field: Signature of an exterior Majorana bound state

NASA Astrophysics Data System (ADS)

Suzuki, Shu-Ichiro; Kawaguchi, Yuki; Tanaka, Yukio

2018-04-01

We study quasiparticle states on a surface of a topological insulator (TI) with proximity-induced superconductivity under an external magnetic field. An applied magnetic field creates two Majorana bound states: a vortex Majorana state localized inside a vortex core and an exterior Majorana state localized along a circle centered at the vortex core. We calculate the spin-resolved local density of states (LDOS) and demonstrate that the shrinking of the radius of the exterior Majorana state, predicted in R. S. Akzyanov et al., Phys. Rev. B 94, 125428 (2016), 10.1103/PhysRevB.94.125428, under a strong magnetic field can be seen in LDOS without smeared out by nonzero-energy states. The spin-resolved LDOS further reveals that the spin of the exterior Majorana state is strongly spin-polarized. Accordingly, the induced odd-frequency spin-triplet pairs are found to be spin-polarized as well. In order to detect the exterior Majorana states, however, the Fermi energy should be closed to the Dirac point to avoid contributions from continuum levels. We also study a different two-dimensional topological-superconducting system where a two-dimensional electron gas with the spin-orbit coupling is sandwiched between an s -wave superconductor and a ferromagnetic insulator. We show that the radius of an exterior Majorana state can be tuned by an applied magnetic field. However, on the contrary to the results at a TI surface, neither the exterior Majorana state nor the induced odd-frequency spin-triplet pairs are spin-polarized. We conclude that the spin polarization of the Majorana state is attributed to the spin-polarized Landau level, which is characteristic for systems with the Dirac-like dispersion.

High resolution photoelectron imaging of UO(-) and UO2(-) and the low-lying electronic states and vibrational frequencies of UO and UO2.

PubMed

Czekner, Joseph; Lopez, Gary V; Wang, Lai-Sheng

2014-12-28

We report a study of the electronic and vibrational structures of the gaseous uranium monoxide and dioxide molecules using high-resolution photoelectron imaging. Vibrationally resolved photoelectron spectra are obtained for both UO(-) and UO2(-). The spectra for UO2(-) are consistent with, but much better resolved than a recent study using a magnetic-bottle photoelectron analyzer [W. L. Li et al., J. Chem. Phys. 140, 094306 (2014)]. The electron affinity (EA) of UO is reported for the first time as 1.1407(7) eV, whereas a much more accurate EA is obtained for UO2 as 1.1688(6) eV. The symmetric stretching modes for the neutral and anionic ground states, and two neutral excited states for UO2 are observed, as well as the bending mode for the neutral ground state. These vibrational frequencies are consistent with previous experimental and theoretical results. The stretching vibrational modes for the ground state and one excited state are observed for UO. The current results for UO and UO2 are compared with previous theoretical calculations including relativistic effects and spin-orbit coupling. The accurate experimental data reported here provide more stringent tests for future theoretical methods for actinide-containing species.

Imaging the Formation of High-Energy Dispersion Anomalies in the Actinide UCoGa5

NASA Astrophysics Data System (ADS)

Das, Tanmoy; Durakiewicz, Tomasz; Zhu, Jian-Xin; Joyce, John J.; Sarrao, John L.; Graf, Matthias J.

2012-10-01

We use angle-resolved photoemission spectroscopy to image the emergence of substantial dispersion and spectral-weight anomalies in the electronic renormalization of the actinide compound UCoGa5 that was presumed to belong to a conventional Fermi-liquid family. Kinks or abrupt breaks in the slope of the quasiparticle dispersion are detected both at low (approximately 130 meV) and high (approximately 1 eV) binding energies below the Fermi energy, ruling out any significant contribution of phonons. We perform numerical calculations to demonstrate that the anomalies are adequately described by coupling between itinerant fermions and spin fluctuations arising from the particle-hole continuum of the spin-orbit-split 5f states of uranium. These anomalies resemble the “waterfall” phenomenon of the high-temperature copper-oxide superconductors, suggesting that spin fluctuations are a generic route toward multiform electronic phases in correlated materials as different as high-temperature superconductors and actinides.

Nonlocal Polarization Feedback in a Fractional Quantum Hall Ferromagnet.

PubMed

Hennel, Szymon; Braem, Beat A; Baer, Stephan; Tiemann, Lars; Sohi, Pirouz; Wehrli, Dominik; Hofmann, Andrea; Reichl, Christian; Wegscheider, Werner; Rössler, Clemens; Ihn, Thomas; Ensslin, Klaus; Rudner, Mark S; Rosenow, Bernd

2016-04-01

In a quantum Hall ferromagnet, the spin polarization of the two-dimensional electron system can be dynamically transferred to nuclear spins in its vicinity through the hyperfine interaction. The resulting nuclear field typically acts back locally, modifying the local electronic Zeeman energy. Here we report a nonlocal effect arising from the interplay between nuclear polarization and the spatial structure of electronic domains in a ν=2/3 fractional quantum Hall state. In our experiments, we use a quantum point contact to locally control and probe the domain structure of different spin configurations emerging at the spin phase transition. Feedback between nuclear and electronic degrees of freedom gives rise to memristive behavior, where electronic transport through the quantum point contact depends on the history of current flow. We propose a model for this effect which suggests a novel route to studying edge states in fractional quantum Hall systems and may account for so-far unexplained oscillatory electronic-transport features observed in previous studies.

Spin injection and transport in semiconductor and metal nanostructures

NASA Astrophysics Data System (ADS)

Zhu, Lei

In this thesis we investigate spin injection and transport in semiconductor and metal nanostructures. To overcome the limitation imposed by the low efficiency of spin injection and extraction and strict requirements for retention of spin polarization within the semiconductor, novel device structures with additional logic functionality and optimized device performance have been developed. Weak localization/antilocalization measurements and analysis are used to assess the influence of surface treatments on elastic, inelastic and spin-orbit scatterings during the electron transport within the two-dimensional electron layer at the InAs surface. Furthermore, we have used spin-valve and scanned probe microscopy measurements to investigate the influence of sulfur-based surface treatments and electrically insulating barrier layers on spin injection into, and spin transport within, the two-dimensional electron layer at the surface of p-type InAs. We also demonstrate and analyze a three-terminal, all-electrical spintronic switching device, combining charge current cancellation by appropriate device biasing and ballistic electron transport. The device yields a robust, electrically amplified spin-dependent current signal despite modest efficiency in electrical injection of spin-polarized electrons. Detailed analyses provide insight into the advantages of ballistic, as opposed to diffusive, transport in device operation, as well as scalability to smaller dimensions, and allow us to eliminate the possibility of phenomena unrelated to spin transport contributing to the observed device functionality. The influence of the device geometry on magnetoresistance of nanoscale spin-valve structures is also demonstrated and discussed. Shortcomings of the simplified one-dimensional spin diffusion model for spin valve are elucidated, with comparison of the thickness and the spin diffusion length in the nonmagnetic channel as the criterion for validity of the 1D model. Our work contributes directly to the realization of spin valve and spin transistor devices based on III-V semiconductors, and offers new opportunities to engineer the behavior of spintronic devices at the nanoscale.

Symmetry properties of the electron density and following from it limits on the KS-DFT applications

NASA Astrophysics Data System (ADS)

Kaplan, Ilya G.

2018-03-01

At present, the Density Functional Theory (DFT) approach elaborated by Kohn with co-authors more than 50 years ago became the most widely used method for study molecules and solids. Using modern computation facilities, it can be applied to systems with million atoms. In the atmosphere of such great popularity, it is particularly important to know the limits of the applicability of DFT methods. In this report, I will discuss two cases when the conventional DFT approaches, using only electron density ρ and its gradients, cannot be applied (I will not consider the Ψ-versions of DFT). The first case is quite evident. In the degenerated states, the electron density may not be defined, since electronic and nuclear motions cannot be separated, the vibronic interaction mixed them. The second case is related to the spin of the state. As it was rigorously proved by group theoretical methods at the theorem level, the electron density does not depend on the total spin S of the arbitrary N-electron state. It means that the Kohn-Sham equations have the same form for states with different S. The critical survey of elaborated DFT procedures, taking into account spin, shows that they modified only exchange functionals, the correlation functionals do not correspond to the spin of the state. The point is that the conception of spin cannot be defined in the framework of the electron density formalism, which corresponds to the one-particle reduced density matrix. This is the main reason of the problems arising in the study by DFT of magnetic properties of the transition metals. The possible way of resolving these problems can be found in the two-particle reduced density matrix formulation of DFT.

Wide-band, time-resolved photoacoustic study of electron-transfer reactions. Photoexcited magnesium porphyrin and quinones

DOE Office of Scientific and Technical Information (OSTI.GOV)

Feitelson, J.; Mauzerall, D.C.

1993-08-12

Wide-band, time-resolved, pulsed photoacoustics has been employed to study the electron-transfer reaction between a triplet magnesium porphyrin and various quinones in polar and nonpolar solvents. The reaction rate constants are near encounter limited. The yield of triplet state is 70% in both solvents. The yield of ions is 85% in the former and zero in the latter, in agreement with spin dephasing time and escape times from the Coulomb wells in the two solvents. In methanol the plot of measured heat output versus quinone redox potential is linear. This implies that the entropy of electron transfer is constant through themore » series, but it may not be negligible. 16 refs., 2 figs., 1 tab.« less

Spin noise spectroscopy of donor-bound electrons in ZnO

NASA Astrophysics Data System (ADS)

Horn, H.; Balocchi, A.; Marie, X.; Bakin, A.; Waag, A.; Oestreich, M.; Hübner, J.

2013-01-01

We investigate the intrinsic spin dynamics of electrons bound to Al impurities in bulk ZnO by optical spin noise spectroscopy. Spin noise spectroscopy enables us to investigate the longitudinal and transverse spin relaxation time with respect to nuclear and external magnetic fields in a single spectrum. On one hand, the spin dynamic is dominated by the intrinsic hyperfine interaction with the nuclear spins of the naturally occurring 67Zn isotope. We measure a typical spin dephasing time of 23 ns, in agreement with the expected theoretical values. On the other hand, we measure a third, very high spin dephasing rate which is attributed to a high defect density of the investigated ZnO material. Measurements of the spin dynamics under the influence of transverse as well as longitudinal external magnetic fields unambiguously reveal the intriguing connections of the electron spin with its nuclear and structural environment.

Spin- and valley-dependent electronic band structure and electronic heat capacity of ferromagnetic silicene in the presence of strain, exchange field and Rashba spin-orbit coupling

NASA Astrophysics Data System (ADS)

Hoi, Bui Dinh; Yarmohammadi, Mohsen; Kazzaz, Houshang Araghi

2017-10-01

We studied how the strain, induced exchange field and extrinsic Rashba spin-orbit coupling (RSOC) enhance the electronic band structure (EBS) and electronic heat capacity (EHC) of ferromagnetic silicene in presence of external electric field (EF) by using the Kane-Mele Hamiltonian, Dirac cone approximation and the Green's function approach. Particular attention is paid to investigate the EHC of spin-up and spin-down bands at Dirac K and K‧ points. We have varied the EF, strain, exchange field and RSOC to tune the energy of inter-band transitions and consequently EHC, leading to very promising features for future applications. Evaluation of EF exhibits three phases: Topological insulator (TI), valley-spin polarized metal (VSPM) and band insulator (BI) at given aforementioned parameters. As a new finding, we have found a quantum anomalous Hall phase in BI regime at strong RSOCs. Interestingly, the effective mass of carriers changes with strain, resulting in EHC behaviors. Here, exchange field has the same behavior with EF. Finally, we have confirmed the reported and expected symmetry results for both Dirac points and spins with the study of valley-dependent EHC.

Electronic and transport properties of Cobalt-based valence tautomeric molecules and polymers

NASA Astrophysics Data System (ADS)

Chen, Yifeng; Calzolari, Arrigo; Buongiorno Nardelli, Marco

2011-03-01

The advancement of molecular spintronics requires further understandings of the fundamental electronic structures and transport properties of prototypical spintronics molecules and polymers. Here we present a density functional based theoretical study of the electronic structures of Cobalt-based valence tautomeric molecules Co III (SQ)(Cat)L Co II (SQ)2 L and their polymers, where SQ refers to the semiquinone ligand, and Cat the catecholate ligand, while L is a redox innocent backbone ligand. The conversion from low-spin Co III ground state to high-spin Co II excited state is realized by imposing an on-site potential U on the Co atom and elongating the Co-N bond. Transport properties are subsequently calculated by extracting electronic Wannier functions from these systems and computing the charge transport in the ballistic regime using a Non-Equilibrium Green's Function (NEGF) approach. Our transport results show distinct charge transport properties between low-spin ground state and high-spin excited state, hence suggesting potential spintronics devices from these molecules and polymers such as spin valves.

Using ultrashort terahertz pulses to directly probe spin dynamics in insulating antiferromagnets

NASA Astrophysics Data System (ADS)

Bowlan, P.; Trugman, S. A.; Yarotski, D. A.; Taylor, A. J.; Prasankumar, R. P.

2018-05-01

Terahertz pulses are a direct and general probe of ultrafast spin dynamics in insulating antiferromagnets (AFM). This is shown by using optical-pump, THz-probe spectroscopy to directly track AFM spin dynamics in the hexagonal multiferroic HoMnO3 and the orthorhombic multiferroic TbMnO3. Our studies show that despite the different structural and spin orders in these materials, THz pulses can unambiguously resolve spin dynamics after optical photoexcitation. We believe that this approach is quite general and can be applied to a broad range of materials with different AFM spin alignments, providing a novel non-contact approach for probing AFM order with femtosecond temporal resolution.

Quantum Conductance in Metal Nanowires

NASA Astrophysics Data System (ADS)

Ugarte, Daniel

2004-03-01

Quantum Conductance in Metal Nanowires D. Ugarte Brazilian National Synchrotron Light Laboratory C.P. 6192, 13084-971 Campinas SP, Brazil. Electrical transport properties of metallic nanowires (NWs) have received great attention due to their quantum conductance behavior. Atomic scale wires can be generated by stretching metal contacts; during the elongation and just before rupture, the NW conductance shows flat plateaus and abrupt jumps of approximately a conductance quantum. In this experiments, both the NW atomic arrangement and conductance change simultaneously, making difficult to discriminate electronic and structural effects. In this work, the atomic structure of NWs was studied by time-resolved in situ experiments in a high resolution transmission electron microscope, while their electrical properties using an UHV mechanically controllable break junction (MCBJ). From the analysis of numerous HRTEM images and videos, we have deduced that metal (Au, Ag, Pt, etc.) junctions generated by tensile deformation are crystalline and free of defects. The neck structure is strongly dependent on the surface properties of the analyzed metal, this was verified by comparing different metal NWs (Au, Ag, Cu), which have similar atomic structure (FCC), but show very different faceting patterns. The correlation between the observed structural and transport properties of NW points out that the quantum conductance behavior is defined by preferred atomic arrangement at the narrowest constriction. In the case of magnetic (ex. Fe,Co,Ni) or quasi-magnetic (ex. Pd) wires, we have observed that one-atom-thick structures show a conductance of half the quantum as expected for a fully spin polarized current. This phenomenon seems to occur spontaneously for magnetic suspended atom-chains in zero magnetic field and at room temperature. These results open new opportunities for spin control in nanostructures. Funded by FAPESP, LNLS and CNPq.

X-ray emission spectroscopy of biomimetic Mn coordination complexes

DOE PAGES

Jensen, Scott C.; Davis, Katherine M.; Sullivan,

2017-05-19

Understanding the function of Mn ions in biological and chemical redox catalysis requires precise knowledge of their electronic structure. X-ray emission spectroscopy (XES) is an emerging technique with a growing application to biological and biomimetic systems. Here, we report an improved, cost-effective spectrometer used to analyze two biomimetic coordination compounds, [Mn IV(OH) 2(Me 2EBC)] 2+ and [Mn IV(O)(OH)(Me 2EBC)] +, the second of which contains a key Mn IV=O structural fragment. Despite having the same formal oxidation state (Mn IV) and tetradentate ligands, XES spectra from these two compounds demonstrate different electronic structures. Experimental measurements and DFT calculations yield differentmore » localized spin densities for the two complexes resulting from Mn IV–OH conversion to Mn IV=O. The relevance of the observed spectroscopic changes is discussed for applications in analyzing complex biological systems such as photosystem II. In conclusion, a model of the S 3 intermediate state of photosystem II containing a Mn IV=O fragment is compared to recent time-resolved X-ray diffraction data of the same state.« less

X-ray Emission Spectroscopy of Biomimetic Mn Coordination Complexes.

PubMed

Jensen, Scott C; Davis, Katherine M; Sullivan, Brendan; Hartzler, Daniel A; Seidler, Gerald T; Casa, Diego M; Kasman, Elina; Colmer, Hannah E; Massie, Allyssa A; Jackson, Timothy A; Pushkar, Yulia

2017-06-15

Understanding the function of Mn ions in biological and chemical redox catalysis requires precise knowledge of their electronic structure. X-ray emission spectroscopy (XES) is an emerging technique with a growing application to biological and biomimetic systems. Here, we report an improved, cost-effective spectrometer used to analyze two biomimetic coordination compounds, [Mn IV (OH) 2 (Me 2 EBC)] 2+ and [Mn IV (O)(OH)(Me 2 EBC)] + , the second of which contains a key Mn IV ═O structural fragment. Despite having the same formal oxidation state (Mn IV ) and tetradentate ligands, XES spectra from these two compounds demonstrate different electronic structures. Experimental measurements and DFT calculations yield different localized spin densities for the two complexes resulting from Mn IV -OH conversion to Mn IV ═O. The relevance of the observed spectroscopic changes is discussed for applications in analyzing complex biological systems such as photosystem II. A model of the S 3 intermediate state of photosystem II containing a Mn IV ═O fragment is compared to recent time-resolved X-ray diffraction data of the same state.

Structure of spin excitations in heavily electron-doped Li 0.8Fe 0.2ODFeSe superconductors

DOE PAGES

Pan, Bingying; Shen, Yao; Hu, Die; ...

2017-07-25

Heavily electron-doped iron-selenide high-transition-temperature (high-T c) superconductors, which have no hole Fermi pockets, but have a notably high T c, have challenged the prevailing s± pairing scenario originally proposed for iron pnictides containing both electron and hole pockets. The microscopic mechanism underlying the enhanced superconductivity in heavily electron-doped iron-selenide remains unclear. Here, we used neutron scattering to study the spin excitations of the heavily electron-doped iron-selenide material Li 0.8Fe 0.2ODFeSe (T c = 41 K). Our data revealed nearly ring-shaped magnetic resonant excitations surrounding (π, π) at ~21 meV. As the energy increased, the spin excitations assumed a diamond shape,more » and they dispersed outward until the energy reached ~60 meV and then inward at higher energies. The observed energy-dependent momentum structure and twisted dispersion of spin excitations near (π, π) are analogous to those of hole-doped cuprates in several aspects, thus implying that such spin excitations are essential for the remarkably high T c in these materials.« less

Zero Quantum Coherence in a Series of Covalent Spin-Correlated Radical Pairs.

PubMed

Nelson, Jordan N; Krzyaniak, Matthew D; Horwitz, Noah E; Rugg, Brandon K; Phelan, Brian T; Wasielewski, Michael R

2017-03-23

Photoinitiated subnanosecond electron transfer within covalently linked electron donor-acceptor molecules can result in the formation of a spin-correlated radical pair (SCRP) with a well-defined initial singlet spin configuration. Subsequent coherent mixing between the SCRP singlet and triplet m s = 0 spin states, the so-called zero quantum coherence (ZQC), is of potential interest in quantum information processing applications because the ZQC can be probed using pulse electron paramagnetic resonance (pulse-EPR) techniques. Here, pulse-EPR spectroscopy is utilized to examine the ZQC oscillation frequencies and ZQC dephasing in three structurally well-defined D-A systems. While transitions between the singlet and triplet m s = 0 spin states are formally forbidden (Δm s = 0), they can be addressed using specific microwave pulse turning angles to map information from the ZQC onto observable single quantum coherences. In addition, by using structural variations to tune the singlet-triplet energy gap, the ZQC frequencies determined for this series of molecules indicate a stronger dependence on the electronic g-factor than on electron-nuclear hyperfine interactions.

A three-dimensional spin-diffusion model for micromagnetics

PubMed Central

Abert, Claas; Ruggeri, Michele; Bruckner, Florian; Vogler, Christoph; Hrkac, Gino; Praetorius, Dirk; Suess, Dieter

2015-01-01

We solve a time-dependent three-dimensional spin-diffusion model coupled to the Landau-Lifshitz-Gilbert equation numerically. The presented model is validated by comparison to two established spin-torque models: The model of Slonzewski that describes spin-torque in multi-layer structures in the presence of a fixed layer and the model of Zhang and Li that describes current driven domain-wall motion. It is shown that both models are incorporated by the spin-diffusion description, i.e., the nonlocal effects of the Slonzewski model are captured as well as the spin-accumulation due to magnetization gradients as described by the model of Zhang and Li. Moreover, the presented method is able to resolve the time dependency of the spin-accumulation. PMID:26442796

Velocity modulation spectroscopy of molecular ions II: The millimeter/submillimeter-wave spectrum of TiF + ( X3Φr)

NASA Astrophysics Data System (ADS)

Halfen, D. T.; Ziurys, L. M.

2006-11-01

The pure rotational spectrum of the molecular ion TiF + in its 3Φr ground state has been measured in the range 327-542 GHz using millimeter-wave direct absorption techniques combined with velocity modulation spectroscopy. TiF + was made in an AC discharge from a mixture of TiCl 4, F 2 in He, and argon. Ten transitions of this ion were recorded. In every transition, fluorine hyperfine interactions, as well as the fine structure splittings, were resolved. The fine structure pattern was found to be regular with almost equal spacing in frequency between the three spin components, in contrast to TiCl +, which is perturbed in the ground state. The data were fit with a case ( a) Hamiltonian and rotational, fine structure, and hyperfine constants were determined. The bond length established for TiF +, r0 = 1.7775 Å, was found to be shorter than that of TiF, r0 = 1.8342 Å—also established from mm-wave data. The hyperfine parameters determined are consistent with a δ1π1 electron configuration with the electrons primarily located on the titanium nucleus. The nuclear spin-orbit constant a indicates that the unpaired electrons are closer to the fluorine nucleus in TiF + relative to TiF, as expected with the decrease in bond length for the ion. The shorter bond distance is thought to arise from increased charge on the titanium nucleus as a result of a Ti 2+F - configuration. A similar decrease in bond length was found for TiCl + relative to TiCl.

Impact of methionine oxidation on calmodulin structural dynamics

DOE Office of Scientific and Technical Information (OSTI.GOV)

McCarthy, Megan R.; Thompson, Andrew R.; Nitu, Florentin

2015-01-09

Highlights: • We measured the distance distribution between two spin labels on calmodulin by DEER. • Two structural states, open and closed, were resolved at both low and high Ca. • Ca shifted the equilibrium toward the open state by a factor of 13. • Methionine oxidation, simulated by glutamine substitution, decreased the Ca effect. • These results have important implications for aging in muscle and other tissues. - Abstract: We have used electron paramagnetic resonance (EPR) to examine the structural impact of oxidizing specific methionine (M) side chains in calmodulin (CaM). It has been shown that oxidation of eithermore » M109 or M124 in CaM diminishes CaM regulation of the muscle calcium release channel, the ryanodine receptor (RyR), and that mutation of M to Q (glutamine) in either case produces functional effects identical to those of oxidation. Here we have used site-directed spin labeling and double electron–electron resonance (DEER), a pulsed EPR technique that measures distances between spin labels, to characterize the structural changes resulting from these mutations. Spin labels were attached to a pair of introduced cysteine residues, one in the C-lobe (T117C) and one in the N-lobe (T34C) of CaM, and DEER was used to determine the distribution of interspin distances. Ca binding induced a large increase in the mean distance, in concert with previous X-ray crystallography and NMR data, showing a closed structure in the absence of Ca and an open structure in the presence of Ca. DEER revealed additional information about CaM’s structural heterogeneity in solution: in both the presence and absence of Ca, CaM populates both structural states, one with probes separated by ∼4 nm (closed) and another at ∼6 nm (open). Ca shifts the structural equilibrium constant toward the open state by a factor of 13. DEER reveals the distribution of interprobe distances, showing that each of these states is itself partially disordered, with the width of each population ranging from 1 to 3 nm. Both mutations (M109Q and M124Q) decrease the effect of Ca on the structure of CaM, primarily by decreasing the closed-to-open equilibrium constant in the presence of Ca. We propose that Met oxidation alters CaM’s functional interaction with its target proteins by perturbing this Ca-dependent structural shift.« less

Effects of structural spin-orbit coupling in two dimensional electron and hole liquids

NASA Astrophysics Data System (ADS)

Chesi, Stefano

The recent interest in spin-dependent phenomena in semiconductor heterostructures motivates our detailed study of the structural spin-orbit coupling present in clean two-dimensional electron and hole liquids. Interesting polarization effects are produced in a system out of equilibrium, as when a finite current flows in the sample. In particular, the consequences of a lateral confinement creating a quasi one-dimensional wire are studied in detail, partially motivated by a recent experimental investigation of the point-contact transmission for two-dimensional holes. We also address the role of the electron-electron interaction in the presence of spin-orbit coupling, which has received little attention in the literature. We discuss the formulation of the Hartree-Fock approximation in the particular case of linear Rashba spin-orbit. We establish the form of the mean-field phase diagram in the homogeneous case, which shows a complex interplay between paramagnetic and ferromagnetic states. The latter can be polarized in the plane or in a transverse direction, and are characterized by a complex spin structure and nontrivial occupation. The generality of the Hartree-Fock method allows a simple treatment of the Pauli spin susceptibility, and the application to different forms of spin-orbit coupling. Correlation corrections can be obtained in an analytic form for particular asymptotic regimes. For linear Rashba spin-orbit we identified the relevance of the large spin-orbit limit, dominated by many-body effects, and explicitly treated the high density limit, in which the system is asymptotically noninteracting. As a special case, we derive a new exact formula for the polarization dependence of the ring-diagram correlation energy.

Rashba and Dresselhaus spin-orbit interactions effects on electronic features of a two dimensional elliptic quantum dot

NASA Astrophysics Data System (ADS)

Mokhtari, P.; Rezaei, G.; Zamani, A.

2017-06-01

In this paper, electronic structure of a two dimensional elliptic quantum dot under the influence of external electric and magnetic fields are studied in the presence of Rashba and Dresselhaus spin-orbit interactions. This investigation is done computationally and to do this, at first, the effective Hamiltonian of the system by considering the spin-orbit coupling is demonstrated in the presence of applied electric and magnetic fields and afterwards the Schrödinger equation is solved using the finite difference approach. Utilizing finite element method, eigenvalues and eigenstates of the system are calculated and the effect of the external fields, the size of the dot as well as the strength of Rashba spin-orbit interaction are studied. Our results indicate that, Spin-orbit interactions, external fields and the dot size have a great influence on the electronic structure of the system.

Unconventional magnetisation texture in graphene/cobalt hybrids

DOE PAGES

Vu, A. D.; Coraux, J.; Chen, G.; ...

2016-04-26

Magnetic domain structure and spin-dependent reflectivity measurements on cobalt thin films intercalated at the graphene/Ir(111) interface are investigated using spin-polarised low-energy electron microscopy. We find that graphene-covered cobalt films have surprising magnetic properties. Vectorial imaging of magnetic domains reveals an unusually gradual thickness-dependent spin reorientation transition, in which magnetisation rotates from out-of-the-film plane to the in-plane direction by less than 10° per cobalt monolayer. During this transition, cobalt films have a meandering spin texture, characterised by a complex, three-dimensional, wavy magnetisation pattern. In addition, spectroscopy measurements suggest that the electronic band structure of the unoccupied states is essentially spin-independent alreadymore » a few electron-Volts above the vacuum level. These properties strikingly differ from those of pristine cobalt films and could open new prospects in surface magnetism.« less

Magnetic edge states in Aharonov-Bohm graphene quantum rings

DOE Office of Scientific and Technical Information (OSTI.GOV)

Farghadan, R., E-mail: rfarghadan@kashanu.ac.ir; Heidari Semiromi, E.; Saffarzadeh, A.

2013-12-07

The effect of electron-electron interaction on the electronic structure of Aharonov-Bohm (AB) graphene quantum rings (GQRs) is explored theoretically using the single-band tight-binding Hamiltonian and the mean-field Hubbard model. The electronic states and magnetic properties of hexagonal, triangular, and circular GQRs with different sizes and zigzag edge terminations are studied. The results show that, although the AB oscillations in the all types of nanoring are affected by the interaction, the spin splitting in the AB oscillations strongly depends on the geometry and the size of graphene nanorings. We found that the total spin of hexagonal and circular rings is zeromore » and therefore, no spin splitting can be observed in the AB oscillations. However, the non-zero magnetization of the triangular rings breaks the degeneracy between spin-up and spin-down electrons, which produces spin-polarized AB oscillations.« less

Magnetoelectroluminescence of organic heterostructures: Analytical theory and spectrally resolved measurements

DOE PAGES

Liu, Feilong; Kelley, Megan R.; Crooker, Scott A.; ...

2014-12-22

The effect of a magnetic field on the electroluminescence of organic light emitting devices originates from the hyperfine interaction between the electron/hole polarons and the hydrogen nuclei of the host molecules. In this paper, we present an analytical theory of magnetoelectroluminescence for organic semiconductors. To be specific, we focus on bilayer heterostructure devices. In the case we are considering, light generation at the interface of the donor and acceptor layers results from the formation and recombination of exciplexes. The spin physics is described by a stochastic Liouville equation for the electron/hole spin density matrix. By finding the steady-state analytical solutionmore » using Bloch-Wangsness-Redfield theory, we explore how the singlet/triplet exciplex ratio is affected by the hyperfine interaction strength and by the external magnetic field. In order to validate the theory, spectrally resolved electroluminescence experiments on BPhen/m-MTDATA devices are analyzed. With increasing emission wavelength, the width of the magnetic field modulation curve of the electroluminescence increases while its depth decreases. Furthermore, these observations are consistent with the model.« less

Topologically nontrivial electronic bands and tunable Dirac cones in graphynes with spin-orbit coupling

NASA Astrophysics Data System (ADS)

Juricic, Vladimir; van Miert, Guido; Morais Smith, Cristiane

2015-03-01

Graphynes represent an emerging family of carbon allotropes that differ from graphene by the presence of the triple bonds (-C ≡C-) in their band structure. They have recently attracted much interest due to the tunability of the Dirac cones in the band structure. I will show that the spin-orbit coupling in β-graphyne could produce various effects related to the topological properties of its electronic bands. Intrinsic spin-orbit coupling yields high- and tunable Chern-number bands, which may host both topological and Chern insulators, in the presence and absence of time-reversal symmetry, respectively. Furthermore, Rashba spin-orbit coupling can be used to control the position and the number of Dirac cones in the Brillouin zone. Finally, I will also discuss the electronic properties of α - and γ - graphyne in the presence of the spin-orbit coupling within recently developed general theory of spin-orbit couplings in graphynes. Work supported by the Netherlands Organization for Scientific Research (NWO).

Observation of a topologically non-trivial surface state in half-Heusler PtLuSb (001) thin films

DOE PAGES

Logan, J. A.; Patel, S. J.; Harrington, S. D.; ...

2016-06-27

The discovery of topological insulators, materials with bulk band gaps and protected cross-gap surface states in compounds such as Bi 2Se 3, has generated much interest in identifying topological surface states (TSSs) in other classes of materials. In particular, recent theoretical calculations suggest that TSSs may be found in half-Heusler ternary compounds. If experimentally realizable, this would provide a materials platform for entirely new heterostructure spintronic devices that make use of the structurally identical but electronically varied nature of Heusler compounds. Here we show the presence of a TSS in epitaxially grown thin films of the half-Heusler compound PtLuSb. Spin-more » and angle-resolved photoemission spectroscopy, complemented by theoretical calculations, reveals a surface state with linear dispersion and a helical tangential spin texture consistent with previous predictions. As a result, this experimental verification of topological behavior is a significant step forward in establishing half-Heusler compounds as a viable material system for future spintronic devices.« less

Revealing the correlation between real-space structure and chiral magnetic order at the atomic scale

NASA Astrophysics Data System (ADS)

Hauptmann, Nadine; Dupé, Melanie; Hung, Tzu-Chao; Lemmens, Alexander K.; Wegner, Daniel; Dupé, Bertrand; Khajetoorians, Alexander A.

2018-03-01

We image simultaneously the geometric, the electronic, and the magnetic structures of a buckled iron bilayer film that exhibits chiral magnetic order. We achieve this by combining spin-polarized scanning tunneling microscopy and magnetic exchange force microscopy (SPEX) to independently characterize the geometric as well as the electronic and magnetic structures of nonflat surfaces. This new SPEX imaging technique reveals the geometric height corrugation of the reconstruction lines resulting from strong strain relaxation in the bilayer, enabling the decomposition of the real-space from the electronic structure at the atomic level and the correlation with the resultant spin-spiral ground state. By additionally utilizing adatom manipulation, we reveal the chiral magnetic ground state of portions of the unit cell that were not previously imaged with spin-polarized scanning tunneling microscopy alone. Using density functional theory, we investigate the structural and electronic properties of the reconstructed bilayer and identify the favorable stoichiometry regime in agreement with our experimental result.

Molecular Spintronics: Theory of Spin-Dependent Electron Transport in Fe/BDT/Fe Molecular Wire Systems

NASA Astrophysics Data System (ADS)

Dalgleish, Hugh; Kirczenow, George

2004-03-01

Metal/Molecule/Metal junction systems forming molecular wires are currently the focus of intense study. Recently, spin-dependent electron transport in molecular wires with magnetic Ni electrodes has been studied theoretically, and spin-valve effects have been predicted.* Here we explore theoretically another magnetic molecular wire system, namely, ferromagnetic Fe nano-contacts bridged with 1,4-benzene-dithiolate (BDT). We estimate the essential structural and electronic parameters for this system based on ab initio density functional calculations (DFT) for some simple model systems involving thiol groups and Fe clusters as well as semi-empirical considerations and the known electronic structure of bulk Fe. We then use Lippmann-Schwinger and Green's function techniques together with the Landauer formalism to study spin-dependent transport. *E. G. Emberly and G. Kirczenow, Chem. Phys. 281, 311 (2002); R. Pati, L. Senapati, P.M. Ajayan and S.K. Nayak, Phys. Rev. B68, 100407 (2003).

First principles calculation of the structural, electronic, and magnetic properties of Au-Pd atomic chains

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dave, Mudra R., E-mail: mdave-phy@yahoo.co.in; Sharma, A. C.

2015-06-24

The structural, electronic and magnetic properties of free standing Au-Pd bimetallic atomic chain is studied using ab-initio method. It is found that electronic and magnetic properties of chains depend on position of atoms and number of atoms. Spin polarization factor for different atomic configuration of atomic chain is calculated predicting a half metallic behavior. It suggests a total spin polarised transport in these chains.

Kohn-Sham Band Structure Benchmark Including Spin-Orbit Coupling for 2D and 3D Solids

NASA Astrophysics Data System (ADS)

Huhn, William; Blum, Volker

2015-03-01

Accurate electronic band structures serve as a primary indicator of the suitability of a material for a given application, e.g., as electronic or catalytic materials. Computed band structures, however, are subject to a host of approximations, some of which are more obvious (e.g., the treatment of the exchange-correlation of self-energy) and others less obvious (e.g., the treatment of core, semicore, or valence electrons, handling of relativistic effects, or the accuracy of the underlying basis set used). We here provide a set of accurate Kohn-Sham band structure benchmarks, using the numeric atom-centered all-electron electronic structure code FHI-aims combined with the ``traditional'' PBE functional and the hybrid HSE functional, to calculate core, valence, and low-lying conduction bands of a set of 2D and 3D materials. Benchmarks are provided with and without effects of spin-orbit coupling, using quasi-degenerate perturbation theory to predict spin-orbit splittings. This work is funded by Fritz-Haber-Institut der Max-Planck-Gesellschaft.

Spin-interaction effects for ultralong-range Rydberg molecules in a magnetic field

NASA Astrophysics Data System (ADS)

Hummel, Frederic; Fey, Christian; Schmelcher, Peter

2018-04-01

We investigate the fine and spin structure of ultralong-range Rydberg molecules exposed to a homogeneous magnetic field. Each molecule consists of a 87Rb Rydberg atom the outer electron of which interacts via spin-dependent s - and p -wave scattering with a polarizable 87Rb ground-state atom. Our model includes also the hyperfine structure of the ground-state atom as well as spin-orbit couplings of the Rydberg and ground-state atom. We focus on d -Rydberg states and principal quantum numbers n in the vicinity of 40. The electronic structure and vibrational states are determined in the framework of the Born-Oppenheimer approximation for varying field strengths ranging from a few up to hundred Gauss. The results show that the interplay between the scattering interactions and the spin couplings gives rise to a large variety of molecular states in different spin configurations as well as in different spatial arrangements that can be tuned by the magnetic field. This includes relatively regularly shaped energy surfaces in a regime where the Zeeman splitting is large compared to the scattering interaction but small compared to the Rydberg fine structure, as well as more complex structures for both weaker and stronger fields. We quantify the impact of spin couplings by comparing the extended theory to a spin-independent model.

Electronic structure and microscopic model of V(2)GeO(4)F(2)-a quantum spin system with S = 1.

PubMed

Rahaman, Badiur; Saha-Dasgupta, T

2007-07-25

We present first-principles density functional calculations and downfolding studies of the electronic and magnetic properties of the oxide-fluoride quantum spin system V(2)GeO(4)F(2). We discuss explicitly the nature of the exchange paths and provide quantitative estimates of magnetic exchange couplings. A microscopic modelling based on analysis of the electronic structure of this systems puts it in the interesting class of weakly coupled alternating chain S = 1 systems. Based on the microscopic model, we make inferrences about its spin excitation spectra, which needs to be tested by rigorous experimental study.

Probing ultrafast changes of spin and charge density profiles with resonant XUV magnetic reflectivity at the free-electron laser FERMI.

PubMed

Gutt, C; Sant, T; Ksenzov, D; Capotondi, F; Pedersoli, E; Raimondi, L; Nikolov, I P; Kiskinova, M; Jaiswal, S; Jakob, G; Kläui, M; Zabel, H; Pietsch, U

2017-09-01

We report the results of resonant magnetic XUV reflectivity experiments performed at the XUV free-electron laser FERMI. Circularly polarized XUV light with the photon energy tuned to the Fe M 2,3 edge is used to measure resonant magnetic reflectivities and the corresponding Q -resolved asymmetry of a Permalloy/Ta/Permalloy trilayer film. The asymmetry exhibits ultrafast changes on 240 fs time scales upon pumping with ultrashort IR laser pulses. Depending on the value of the wavevector transfer Q z , we observe both decreasing and increasing values of the asymmetry parameter, which is attributed to ultrafast changes in the vertical spin and charge density profiles of the trilayer film.

On the temperature-dependent exchange splitting in the quasiparticle bandstructure of Ni

NASA Astrophysics Data System (ADS)

Borgiel, W.; Nolting, W.; Donath, M.

1989-11-01

A theoretical model for the bandferromagnet Ni is proposed, which takes into account the intraatomic electron interactions within the d band complex. After introducing effective spin operators the model-Hamiltonian consists of a one-particle part, an intraband interaction of Hubbard-type, and an interband exchange, formally describing electron magnon scattering (s-f model). The one particle energies are taken from a realistic bandstructure calculation for paramagnetic Ni. We use a many body procedure for a detailed inspection of the quasiparticle bandstructure in KX and XW directions, present the corresponding spectral densities, and compare the temperature dependent exchange splittings near the X and W point with recent results from spin resolved photoemission (PE) - and inverse photoemission (IPE) - experiments.

Spin splitting in band structures of BiTeX (X=Cl, Br, I) monolayers

NASA Astrophysics Data System (ADS)

Hvazdouski, D. C.; Baranava, M. S.; Stempitsky, V. R.

2018-04-01

In systems with breaking of inversion symmetry a perpendicular electric field arises that interacts with the conduction electrons. It may give rise to electron state splitting even without influence of external magnetic field due to the spin-orbital interaction (SOI). Such a removal of the spin degeneracy is called the Rashba effect. Nanostructure with the Rashba effect can be part of a spin transistor. Spin degeneracy can be realized in a channel from a material of this type without additive of magnetic ions. Lack of additive increases the charge carrier mobility and reliability of the device. Ab initio simulations of BiTeX (X=Cl, Br, I) monolayers have been carried out using VASP wherein implemented DFT method. The study of this structures is of interest because such sort of structures can be used their as spin-orbitronics materials. The crystal parameters of BiTeCl, BiTeBr, BiTeI have been determined by the ionic relaxation and static calculations. It is necessary to note that splitting of energy bands occurs in case of SOI included. The values of the Rashba coefficient aR (in the range from 6.25 to 10.00 eV·Å) have high magnitudes for spintronics materials. Band structure of monolayers structures have ideal Rashba electron gas, i.e. there no other energy states near to Fermi level except Rashba states.

Correlation Effects and Hidden Spin-Orbit Entangled Electronic Order in Parent and Electron-Doped Iridates Sr2 IrO4

NASA Astrophysics Data System (ADS)

Zhou, Sen; Jiang, Kun; Chen, Hua; Wang, Ziqiang

2017-10-01

Analogs of the high-Tc cuprates have been long sought after in transition metal oxides. Because of the strong spin-orbit coupling, the 5 d perovskite iridates Sr2 IrO4 exhibit a low-energy electronic structure remarkably similar to the cuprates. Whether a superconducting state exists as in the cuprates requires understanding the correlated spin-orbit entangled electronic states. Recent experiments discovered hidden order in the parent and electron-doped iridates, some with striking analogies to the cuprates, including Fermi surface pockets, Fermi arcs, and pseudogap. Here, we study the correlation and disorder effects in a five-orbital model derived from the band theory. We find that the experimental observations are consistent with a d -wave spin-orbit density wave order that breaks the symmetry of a joint twofold spin-orbital rotation followed by a lattice translation. There is a Berry phase and a plaquette spin flux due to spin procession as electrons hop between Ir atoms, akin to the intersite spin-orbit coupling in quantum spin Hall insulators. The associated staggered circulating Jeff=1 /2 spin current can be probed by advanced techniques of spin-current detection in spintronics. This electronic order can emerge spontaneously from the intersite Coulomb interactions between the spatially extended iridium 5 d orbitals, turning the metallic state into an electron-doped quasi-2D Dirac semimetal with important implications on the possible superconducting state suggested by recent experiments.

Mapping of spin wave propagation in a one-dimensional magnonic crystal

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ordóñez-Romero, César L., E-mail: cloro@fisica.unam.mx; Lazcano-Ortiz, Zorayda; Aguilar-Huerta, Melisa

2016-07-28

The formation and evolution of spin wave band gaps in the transmission spectrum of a magnonic crystal have been studied. A time and space resolved magneto inductive probing system has been used to map the spin wave propagation and evolution in a geometrically structured yttrium iron garnet film. Experiments have been carried out using (1) a chemically etched magnonic crystal supporting the propagation of magnetostatic surface spin waves, (2) a short microwave pulsed excitation of the spin waves, and (3) direct spin wave detection using a movable magneto inductive probe connected to a synchronized fast oscilloscope. The results show thatmore » the periodic structure not only modifies the spectra of the transmitted spin waves but also influences the distribution of the spin wave energy inside the magnonic crystal as a function of the position and the transmitted frequency. These results comprise an experimental confirmation of Bloch′s theorem in a spin wave system and demonstrate good agreement with theoretical observations in analogue phononic and photonic systems. Theoretical prediction of the structured transmission spectra is achieved using a simple model based on microwave transmission lines theory. Here, a spin wave system illustrates in detail the evolution of a much more general physical concept: the band gap.« less

Electronic Structures of Anti-Ferromagnetic Tetraradicals: Ab Initio and Semi-Empirical Studies.

PubMed

Zhang, Dawei; Liu, Chungen

2016-04-12

The energy relationships and electronic structures of the lowest-lying spin states in several anti-ferromagnetic tetraradical model systems are studied with high-level ab initio and semi-empirical methods. The Full-CI method (FCI), the complete active space second-order perturbation theory (CASPT2), and the n-electron valence state perturbation theory (NEVPT2) are employed to obtain reference results. By comparing the energy relationships predicted from the Heisenberg and Hubbard models with ab initio benchmarks, the accuracy of the widely used Heisenberg model for anti-ferromagnetic spin-coupling in low-spin polyradicals is cautiously tested in this work. It is found that the strength of electron correlation (|U/t|) concerning anti-ferromagnetically coupled radical centers could range widely from strong to moderate correlation regimes and could become another degree of freedom besides the spin multiplicity. Accordingly, the Heisenberg-type model works well in the regime of strong correlation, which reproduces well the energy relationships along with the wave functions of all the spin states. In moderately spin-correlated tetraradicals, the results of the prototype Heisenberg model deviate severely from those of multi-reference electron correlation ab initio methods, while the extended Heisenberg model, containing four-body terms, can introduce reasonable corrections and maintains its accuracy in this condition. In the weak correlation regime, both the prototype Heisenberg model and its extended forms containing higher-order correction terms will encounter difficulties. Meanwhile, the Hubbard model shows balanced accuracy from strong to weak correlation cases and can reproduce qualitatively correct electronic structures, which makes it more suitable for the study of anti-ferromagnetic coupling in polyradical systems.

Re-Visiting the Electronic Energy Map of the Copper Dimer by Double-Resonant Four-Wave Mixing

NASA Astrophysics Data System (ADS)

Visser, Bradley; Bornhauser, Peter; Beck, Martin; Knopp, Gregor; Marquardt, Roberto; Gourlaouen, Christophe; van Bokhoven, Jeroen A.; Radi, Peter

2017-06-01

The copper dimer is one of the most studied transition metal (TM) diatomics due to its alkali-metal like electronic shell structure, strongly bound ground state and chemical reactivity. The high electronic promotion energy in the copper atom yields numerous low-lying electronic states compared to TM dimers with d)-hole electronic configurations. Thus, through extensive study the excited electronic structure of Cu_2 is relatively well known, however in practice few excited states have been investigated with rotational resolution or even assigned term symbols or dissociation limits. The spectroscopic methods that have been used to investigate the copper dimer until now have not possessed sufficient spectral selectivity, which has complicated the analysis of the often overlapping transitions. Resonant four-wave mixing is a non-linear absorption based spectroscopic method. In favorable cases, the two-color version (TC-RFWM) enables purely optical mass selective spectral measurements in a mixed molecular beam. Additionally, by labelling individual rotational levels in the common intermediate state the spectra are dramatically simplified. In this work, we report on the rotationally resolved characterization of low-lying electronic states of dicopper. Several term symbols have been assigned unambiguously. De-perturbation studies performed shed light on the complex electronic structure of the molecule. Furthermore, a new low-lying electronic state of Cu_2 is discovered and has important implications for the high-level theoretical structure calculations performed in parallel. In fact, the ab initio methods applied yield relative energies among the electronic levels that are almost quantitative and allow assignment of the newly observed state that is governed by spin-orbit interacting levels.

Bilinear magnetoelectric resistance as a probe of three-dimensional spin texture in topological surface states

NASA Astrophysics Data System (ADS)

He, Pan; Zhang, Steven S.-L.; Zhu, Dapeng; Liu, Yang; Wang, Yi; Yu, Jiawei; Vignale, Giovanni; Yang, Hyunsoo

2018-05-01

Surface states of three-dimensional topological insulators exhibit the phenomenon of spin-momentum locking, whereby the orientation of an electron spin is determined by its momentum. Probing the spin texture of these states is of critical importance for the realization of topological insulator devices, but the main technique currently available is spin- and angle-resolved photoemission spectroscopy. Here we reveal a close link between the spin texture and a new kind of magnetoresistance, which depends on the relative orientation of the current with respect to the magnetic field as well as the crystallographic axes, and scales linearly with both the applied electric and magnetic fields. This bilinear magnetoelectric resistance can be used to map the spin texture of topological surface states by simple transport measurements. For a prototypical Bi2Se3 single layer, we can map both the in-plane and out-of-plane components of the spin texture (the latter arising from hexagonal warping). Theoretical calculations suggest that the bilinear magnetoelectric resistance originates from conversion of a non-equilibrium spin current into a charge current under application of the external magnetic field.

X-ray imaging of spin currents and magnetisation dynamics at the nanoscale

NASA Astrophysics Data System (ADS)

Bonetti, Stefano

2017-04-01

Understanding how spins move in time and space is the aim of both fundamental and applied research in modern magnetism. Over the past three decades, research in this field has led to technological advances that have had a major impact on our society, while improving the understanding of the fundamentals of spin physics. However, important questions still remain unanswered, because it is experimentally challenging to directly observe spins and their motion with a combined high spatial and temporal resolution. In this article, we present an overview of the recent advances in x-ray microscopy that allow researchers to directly watch spins move in time and space at the microscopically relevant scales. We discuss scanning x-ray transmission microscopy (STXM) at resonant soft x-ray edges, which is available at most modern synchrotron light sources. This technique measures magnetic contrast through the x-ray magnetic circular dichroism (XMCD) effect at the resonant absorption edges, while focusing the x-ray radiation at the nanometre scale, and using the intrinsic pulsed structure of synchrotron-generated x-rays to create time-resolved images of magnetism at the nanoscale. In particular, we discuss how the presence of spin currents can be detected by imaging spin accumulation, and how the magnetisation dynamics in thin ferromagnetic films can be directly imaged. We discuss how a direct look at the phenomena allows for a deeper understanding of the the physics at play, that is not accessible to other, more indirect techniques. Finally, we present an overview of the exciting opportunities that lie ahead to further understand the fundamentals of novel spin physics, opportunities offered by the appearance of diffraction limited storage rings and free electron lasers.

X-ray imaging of spin currents and magnetisation dynamics at the nanoscale.

PubMed

Bonetti, Stefano

2017-04-05

Understanding how spins move in time and space is the aim of both fundamental and applied research in modern magnetism. Over the past three decades, research in this field has led to technological advances that have had a major impact on our society, while improving the understanding of the fundamentals of spin physics. However, important questions still remain unanswered, because it is experimentally challenging to directly observe spins and their motion with a combined high spatial and temporal resolution. In this article, we present an overview of the recent advances in x-ray microscopy that allow researchers to directly watch spins move in time and space at the microscopically relevant scales. We discuss scanning x-ray transmission microscopy (STXM) at resonant soft x-ray edges, which is available at most modern synchrotron light sources. This technique measures magnetic contrast through the x-ray magnetic circular dichroism (XMCD) effect at the resonant absorption edges, while focusing the x-ray radiation at the nanometre scale, and using the intrinsic pulsed structure of synchrotron-generated x-rays to create time-resolved images of magnetism at the nanoscale. In particular, we discuss how the presence of spin currents can be detected by imaging spin accumulation, and how the magnetisation dynamics in thin ferromagnetic films can be directly imaged. We discuss how a direct look at the phenomena allows for a deeper understanding of the the physics at play, that is not accessible to other, more indirect techniques. Finally, we present an overview of the exciting opportunities that lie ahead to further understand the fundamentals of novel spin physics, opportunities offered by the appearance of diffraction limited storage rings and free electron lasers.

Pulse Double-Resonance EPR Techniques for the Study of Metallobiomolecules.

PubMed

Cox, Nicholas; Nalepa, Anna; Pandelia, Maria-Eirini; Lubitz, Wolfgang; Savitsky, Anton

2015-01-01

Electron paramagnetic resonance (EPR) spectroscopy exploits an intrinsic property of matter, namely the electron spin and its related magnetic moment. This can be oriented in a magnetic field and thus, in the classical limit, acts like a little bar magnet. Its moment will align either parallel or antiparallel to the field, giving rise to different energies (termed Zeeman splitting). Transitions between these two quantized states can be driven by incident microwave frequency radiation, analogous to NMR experiments, where radiofrequency radiation is used. However, the electron Zeeman interaction alone provides only limited information. Instead, much of the usefulness of EPR is derived from the fact that the electron spin also interacts with its local magnetic environment and thus can be used to probe structure via detection of nearby spins, e.g., NMR-active magnetic nuclei and/or other electron spin(s). The latter is exploited in spin labeling techniques, an exciting new area in the development of noncrystallographic protein structure determination. Although these interactions are often smaller than the linewidth of the EPR experiment, sophisticated pulse EPR methods allow their detection. A number of such techniques are well established today and can be broadly described as double-resonance methods, in which the electron spin is used as a reporter. Below we give a brief description of pulse EPR methods, particularly their implementation at higher magnetic fields, and how to best exploit them for studying metallobiomolecules. © 2015 Elsevier Inc. All rights reserved.

First-principles study of low-spin LaCoO3 with structurally consistent Hubbard U

NASA Astrophysics Data System (ADS)

Hsu, H.; Umemoto, K.; Cococcioni, M.; Wentzcovitch, R.

2008-12-01

We use the local density approximation + Hubbard U (LDA+U) method to calculate the structural and electronic properties of low-spin LaCoO3. The Hubbard U is obtained by first principles and consistent with each fully-optimized atomic structure at different pressures. With structurally consistent U, the fully-optimized atomic structure agrees with experimental data better than the calculations with fixed or vanishing U. A discussion on how the Hubbard U affects the electronic and atomic structure of LaCoO3 is also given.

Hybrid-exchange density-functional theory study of the electronic structure of MnV2O4 : Exotic orbital ordering in the cubic structure

NASA Astrophysics Data System (ADS)

Wu, Wei

2015-05-01

The electronic structures of cubic and tetragonal MnV2O4 have been studied using hybrid-exchange density-functional theory. The computed electronic structure of the tetragonal phase shows an antiferro-orbital ordering on V sites and a ferrimagnetic ground state (the spins on V and Mn are antialigned). These results are in good agreement with the previous theoretical result obtained from the local-density approximation + U methods [S. Sarkar et al., Phys. Rev. Lett. 102, 216405 (2009), 10.1103/PhysRevLett.102.216405]. Moreover, the electronic structure, especially the projected density of states of the cubic phase, has been predicted with good agreement with the recent soft x-ray spectroscopy experiment. Similar to the tetragonal phase, the spins on V and Mn in the cubic structure favor a ferrimagnetic configuration. Most interesting is that the computed charge densities of the spin-carrying orbitals on V in the cubic phase show an exotic orbital ordering, i.e., a ferro-orbital ordering along [110] but an antiferro-orbital ordering along [1 ¯10 ] .

Spin relaxation in quantum dots due to electron exchange with leads.

PubMed

Vorontsov, A B; Vavilov, M G

2008-11-28

We calculate spin relaxation rates in lateral quantum dot systems due to electron exchange between dots and leads. Using rate equations, we develop a theoretical description of the experimentally observed electric current in the spin blockade regime of double quantum dots. A single expression fits the entire current profile and describes the structure of both the conduction peaks and the suppressed ("valley") region. Extrinsic rates calculated here have to be taken into account for accurate extraction of intrinsic relaxation rates due to the spin-orbit and hyperfine spin scattering mechanisms from spin blockade measurements.

Enhancing Spin Filters by Use of Bulk Inversion Asymmetry

NASA Technical Reports Server (NTRS)

Ting, David; Cartoixa,Xavier

2007-01-01

Theoretical calculations have shown that the degrees of spin polarization in proposed nonmagnetic semiconductor resonant tunneling spin filters could be increased through exploitation of bulk inversion asymmetry (BIA). These enhancements would be effected through suitable orientation of spin collectors (or spin-polarization- inducing lateral electric fields), as described below. Spin filters -- more precisely, sources of spin-polarized electron currents -- have been sought for research on, and development of, the emerging technological discipline of spintronics (spin-transport electronics). The proposed spin filters were to be based on the Rashba effect, which is an energy splitting of what would otherwise be degenerate quantum states, caused by a spinorbit interaction in conjunction with a structural-inversion asymmetry (SIA) in the presence of interfacial electric fields in a semiconductor heterostructure. The magnitude of the energy split is proportional to the electron wave number. In a spin filter, the spin-polarized currents produced by the Rashba effect would be extracted by quantum-mechanical resonant tunneling.

Effect of spin-orbit and on-site Coulomb interactions on the electronic structure and lattice dynamics of uranium monocarbide

NASA Astrophysics Data System (ADS)

Wdowik, U. D.; Piekarz, P.; Legut, D.; Jagło, G.

2016-08-01

Uranium monocarbide, a potential fuel material for the generation IV reactors, is investigated within density functional theory. Its electronic, magnetic, elastic, and phonon properties are analyzed and discussed in terms of spin-orbit interaction and localized versus itinerant behavior of the 5 f electrons. The localization of the 5 f states is tuned by varying the local Coulomb repulsion interaction parameter. We demonstrate that the theoretical electronic structure, elastic constants, phonon dispersions, and their densities of states can reproduce accurately the results of x-ray photoemission and bremsstrahlung isochromat measurements as well as inelastic neutron scattering experiments only when the 5 f states experience the spin-orbit interaction and simultaneously remain partially localized. The partial localization of the 5 f electrons could be represented by a moderate value of the on-site Coulomb interaction parameter of about 2 eV. The results of the present studies indicate that both strong electron correlations and spin-orbit effects are crucial for realistic theoretical description of the ground-state properties of uranium carbide.

Cold denaturation induces inversion of dipole and spin transfer in chiral peptide monolayers

PubMed Central

Eckshtain-Levi, Meital; Capua, Eyal; Refaely-Abramson, Sivan; Sarkar, Soumyajit; Gavrilov, Yulian; Mathew, Shinto P.; Paltiel, Yossi; Levy, Yaakov; Kronik, Leeor; Naaman, Ron

2016-01-01

Chirality-induced spin selectivity is a recently-discovered effect, which results in spin selectivity for electrons transmitted through chiral peptide monolayers. Here, we use this spin selectivity to probe the organization of self-assembled α-helix peptide monolayers and examine the relation between structural and spin transfer phenomena. We show that the α-helix structure of oligopeptides based on alanine and aminoisobutyric acid is transformed to a more linear one upon cooling. This process is similar to the known cold denaturation in peptides, but here the self-assembled monolayer plays the role of the solvent. The structural change results in a flip in the direction of the electrical dipole moment of the adsorbed molecules. The dipole flip is accompanied by a concomitant change in the spin that is preferred in electron transfer through the molecules, observed via a new solid-state hybrid organic–inorganic device that is based on the Hall effect, but operates with no external magnetic field or magnetic material. PMID:26916536

Cold denaturation induces inversion of dipole and spin transfer in chiral peptide monolayers

NASA Astrophysics Data System (ADS)

Eckshtain-Levi, Meital; Capua, Eyal; Refaely-Abramson, Sivan; Sarkar, Soumyajit; Gavrilov, Yulian; Mathew, Shinto P.; Paltiel, Yossi; Levy, Yaakov; Kronik, Leeor; Naaman, Ron

2016-02-01

Chirality-induced spin selectivity is a recently-discovered effect, which results in spin selectivity for electrons transmitted through chiral peptide monolayers. Here, we use this spin selectivity to probe the organization of self-assembled α-helix peptide monolayers and examine the relation between structural and spin transfer phenomena. We show that the α-helix structure of oligopeptides based on alanine and aminoisobutyric acid is transformed to a more linear one upon cooling. This process is similar to the known cold denaturation in peptides, but here the self-assembled monolayer plays the role of the solvent. The structural change results in a flip in the direction of the electrical dipole moment of the adsorbed molecules. The dipole flip is accompanied by a concomitant change in the spin that is preferred in electron transfer through the molecules, observed via a new solid-state hybrid organic-inorganic device that is based on the Hall effect, but operates with no external magnetic field or magnetic material.

Electronic properties of novel topological quantum materials studied by angle-resolved photoemission spectroscopy (ARPES)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wu, Yun

The discovery of quantum Hall e ect has motivated the use of topology instead of broken symmetry to classify the states of matter. Quantum spin Hall e ect has been proposed to have a separation of spin currents as an analogue of the charge currents separation in quantum Hall e ect, leading us to the era of topological insulators. Three-dimensional analogue of the Dirac state in graphene has brought us the three-dimensional Dirac states. Materials with three-dimensional Dirac states could potentially be the parent compounds for Weyl semimetals and topological insulators when time-reversal or space inversion symmetry is broken. Inmore » addition to the single Dirac point linking the two dispersion cones in the Dirac/Weyl semimetals, Dirac points can form a line in the momentum space, resulting in a topological node line semimetal. These fascinating novel topological quantum materials could provide us platforms for studying the relativistic physics in condensed matter systems and potentially lead to design of new electronic devices that run faster and consume less power than traditional, silicon based transistors. In this thesis, we present the electronic properties of novel topological quantum materials studied by angle-resolved photoemission spectroscopy (ARPES).« less

Spin Coherence in Silicon-based Quantum Structures and Devices

DTIC Science & Technology

2017-08-31

Using electron spin resonance (ESR) to measure the den- sity of shallow traps, we find that the two sets of devices are nearly identical , indicating...experiments which cannot utilize a clock transition or a field-cancelling decoherence-free subspace. Our approach was to lock the microwave source driving...the electron spins to a strong nuclear spin signal. In our initial experiments we locked to the proton signal in a water cell. However, the noise in

Voltage-induced Interface Reconstruction and Electrical Instability of the Ferromagnet-Semiconductor Device.

PubMed

Chang, Shu-Jui; Chang, Po-Chun; Lin, Wen-Chin; Lo, Shao-Hua; Chang, Liang-Chun; Lee, Shang-Fan; Tseng, Yuan-Chieh

2017-03-23

Using x-ray magnetic spectroscopy with in-situ electrical characterizations, we investigated the effects of external voltage on the spin-electronic and transport properties at the interface of a Fe/ZnO device. Layer-, element-, and spin-resolved information of the device was obtained by cross-tuning of the x-ray mode and photon energy, when voltage was applied. At the early stage of the operation, the device exhibited a low-resistance state featuring robust Fe-O bonds. However, the Fe-O bonds were broken with increasing voltage. Breaking of the Fe-O bonds caused the formation of oxygen vacancies and resulted in a high-resistance state. Such interface reconstruction was coupled to a charge-transfer effect via Fe-O hybridization, which suppressed/enhanced the magnetization/coercivity of Fe electronically. Nevertheless, the interface became stabilized with the metallic phase if the device was continuously polarized. During this stage, the spin-polarization of Fe was enhanced whereas the coercivity was lowered by voltage, but changes of both characteristics were reversible. This stage is desirable for spintronic device applications, owing to a different voltage-induced electronic transition compared to the first stage. The study enabled a straightforward detection of the spin-electronic state at the ferromagnet-semiconductor interface in relation to the transport and reversal properties during operation process of the device.

Electron paramagnetic resonance of a 10B-containing heterocyclic radical

NASA Astrophysics Data System (ADS)

Eaton, Sandra S.; Ngendahimana, Thacien; Eaton, Gareth R.; Jupp, Andrew R.; Stephan, Douglas W.

2018-05-01

Electron paramagnetic resonance measurements for a 10B-containing heterocyclic phenanthrenedione radical, (C6F5)2B(O2C14H8), were made at X-band in 9:1 toluene:dichloromethane from 10 to 293 K and in toluene from 180 to 293 K. In well-deoxygenated 0.1 mM toluene solution at room temperature hyperfine couplings to 10B, four pairs of protons and five pairs of fluorines contribute to a continuous wave spectrum with many resolved lines. Hyperfine couplings were adjusted to provide the best fit for spectra of the radical enriched in 10B and the analogous radical synthesized with 10,11B in natural abundance, resulting in small refinements of the hyperfine coupling constants previously reported for the natural abundance sample. Electron spin relaxation rates at temperatures between 15 and 293 K were similar for samples containing 10B and natural isotope abundance. Analysis of electron spin echo envelope modulation and hyperfine correlation spectroscopy data at 80 K found Axx = -7.5 ± 0.3, Ayy = -8.5 ± 0.3, and Azz = -10.8 ± 0.3 MHz for 11B, which indicates small spin density on the boron. The spin echo and hyperfine spectroscopy data for the 10B -containing radical are consistent with the factor of 2.99 smaller hyperfine values for 10B than for 11B.

Magnetic and structural X-ray dichroïsms of metallic multilayers

NASA Astrophysics Data System (ADS)

Pizzini, Stefania; Fontaine, A.; Baudelet, F.; Minr, S.; Giorgetti, C.; Dartyge, E.; Bobo, J. F.; Piecuch, M.

1995-05-01

Fe/Cu and Co/Cu multilayers are intensively studied because of their exceptional magnetic properties, i.e., their giant magnetoresistance and the oscillations of the magnetic coupling between magnetic layers as a function of the thickness of the copper spacer [S.S. Parkin et al., Phys. Rev. Lett. 66 (1991) 2152; F. Petroff et al., Phys. Rev. B 44 (1991) 5355]. Spectroscopic approaches to the understanding of the coupling of ferromagnetic layers through a noble metal layer have been recently introduced, in particular spin-resolved photoemission [N.B. Brookes et al., Phys. Rev. Lett. 67 (1991) 354; C. Carbone et al., PRL 71 (1993) 2805] inverse photoemission [J.E. Ortega et al., Phys. Rev. Lett. 69 (1992) 844; Phys. Rev. B 47 (1993) 1540] and magnetic circular dichroism [S. Pizzini et al., MRS Symp. Proc., vol. 313 (1993); M.G. Samant et al. Phys. Rev. Lett. 72 (1994) 2152; S. Pizzini et al., Phys. Rev. Lett. 74 (1995) 1470]. X-ray absorption spectroscopy appears to be effective both for determination of the local structure, specific to the bidimensionality of the system but also for the electron symmetry-dependent evaluation of the spin polarisation of the noble metal as well as the magnetic element.

Magneto-optical studies of quantum dots

NASA Astrophysics Data System (ADS)

Russ, Andreas Hans

Significant effort in condensed matter physics has recently been devoted to the field of "spintronics" which seeks to utilize the spin degree of freedom of electrons. Unlike conventional electronics that rely on the electron charge, devices exploiting their spin have the potential to yield new and novel technological applications, including spin transistors, spin filters, and spin-based memory devices. Any such application has the following essential requirements: 1) Efficient electrical injection of spin-polarized carriers; 2) Long spin lifetimes; 3) Ability to control and manipulate electron spins; 4) Effective detection of spin-polarized carriers. Recent work has demonstrated efficient electrical injection from ferromagnetic contacts such as Fe and MnAs, utilizing a spin-Light Emitting Diode (spin-LED) as a method of detection. Semiconductor quantum dots (QDs) are attractive candidates for satisfying requirements 2 and 3 as their zero dimensionality significantly suppresses many spin-flip mechanisms leading to long spin coherence times, as well as enabling the localization and manipulation of a controlled number of electrons and holes. This thesis is composed of three projects that are all based on the optical properties of QD structures including: I) Intershell exchange between spin-polarized electrons occupying adjacent shells in InAs QDs; II) Spin-polarized multiexitons in InAs QDs in the presence of spin-orbit interactions; III) The optical Aharonov-Bohm effect in AlxGa1-xAs/AlyGa1-yAs quantum wells (QWs). In the following we introduce some of the basic optical properties of quantum dots, describe the main tool (spin-LED) employed in this thesis to inject and detect spins in these QDs, and conclude with the optical Aharonov-Bohm effect (OAB) in type-II QDs.

Structure of MQ-NMR spin spaces under higher Sn- and ( Sn)↓ G symmetries. II. Γ/ overlineΓ ( S6)↓ O subduced irreps for sixfold spin clusters pertaining to the molecular cage ion, [ 11BH] 62-

NASA Astrophysics Data System (ADS)

Colpa, J. P.; Temme, F. P.

1991-06-01

The structures of higher n-fold spin cluster systems as irreps under the S6/( S6)↓ O groups are derived using combinatorial techniques over permutational fields, namely that of generalized wordlengths (GWL), to generate the invariance and irrep sets over the M ( q) subspaces for the [ A] 6( Ii) clusters, i.e. those derived from sets of identical nuclear spins I i whose magnitude lies between 1/2 ⩽ I i ⩽ 3/2. The partitions and invariance properties of such monoclusters provide the background to an investigation of the structure of bicluster spin problems over both Hilbert and Liouville spaces. Hence, the [λ], [ overlineλ] ( Sn) partitional aspects of the NMR of the borohydride molecular cage-ion, [ 11BH] 62-, arise from the form of GWLs for specific primes ( p) (i.e. in Sn theory sense of an index denoting the number of subfields) and the use of invariance hierarchies under the direct product group of the subduced spin symmetries. Such ( Sn)↓ G spin symmetries have been presented in discussions of the symmetry of many-electron spin systems, e.g. as outlined in the seminal work of Kaplan (1975). Attention is drawn to the role of Sn-inner tensor products and Cayley algebra in explicitly resolving certain problems connected with the non-simple reducibility pertaining to ( M1- M n ( S6) fields once p exceeds 2 (i.e. for clusters of identical higher spins). By partitioning Liouville space derived from the density operator σ(SO (3) × S6) and its analogues under subduced spin symmetries this paper extends both the formalism and practical application of various recent multiquantum techniques to experimental NMR. The present semitheoretical "tool" to factor << kqv | CL(SO (3) × [ overline6]) | k' q' v'>> and matrix representation of the Liouville operator for the subduced direct product symmetry of the total bicluster problem emphasizes Pines' 1988 argument [in Proc. C-th E. Fermi Physics Institute] that sets of selective subproblems exist which are ameniable to analysis of their information content without the need to treat the full problem; he focusses on selective q processes from an experimental viewpoint whereas we emphasize all q, [λ] forms of factoring in the analysis of spin evolution. Finally, we stress the primary theoretical importance of scalar invariants in few- and many-body spin problems in the context of SU2 × Sn dual mappings and associated genealogies.

Homogeneous microwave field emitted propagating spin waves: Direct imaging and modeling

NASA Astrophysics Data System (ADS)

Lohman, Mathis; Mozooni, Babak; McCord, Jeffrey

2018-03-01

We explore the generation of propagating dipolar spin waves by homogeneous magnetic field excitation in the proximity of the boundaries of magnetic microstructures. Domain wall motion, precessional dynamics, and propagating spin waves are directly imaged by time-resolved wide-field magneto-optical Kerr effect microscopy. The aspects of spin wave generation are clarified by micromagnetic calculations matching the experimental results. The region of dipolar spin wave formation is confined to the local resonant excitation due to non-uniform internal demagnetization fields at the edges of the patterned sample. Magnetic domain walls act as a border for the propagation of plane and low damped spin waves, thus restraining the spin waves within the individual magnetic domains. The findings are of significance for the general understanding of structural and configurational magnetic boundaries for the creation, the propagation, and elimination of spin waves.

Ultrafast magnetodynamics with free-electron lasers

NASA Astrophysics Data System (ADS)

Malvestuto, Marco; Ciprian, Roberta; Caretta, Antonio; Casarin, Barbara; Parmigiani, Fulvio

2018-02-01

The study of ultrafast magnetodynamics has entered a new era thanks to the groundbreaking technological advances in free-electron laser (FEL) light sources. The advent of these light sources has made possible unprecedented experimental schemes for time-resolved x-ray magneto-optic spectroscopies, which are now paving the road for exploring the ultimate limits of out-of-equilibrium magnetic phenomena. In particular, these studies will provide insights into elementary mechanisms governing spin and orbital dynamics, therefore contributing to the development of ultrafast devices for relevant magnetic technologies. This topical review focuses on recent advancement in the study of non-equilibrium magnetic phenomena from the perspective of time-resolved extreme ultra violet (EUV) and soft x-ray spectroscopies at FELs with highlights of some important experimental results.

Decoherence and fluctuation dynamics of the quantum dot nuclear spin bath probed by nuclear magnetic resonance

NASA Astrophysics Data System (ADS)

Chekhovich, Evgeny A.

2017-06-01

Dynamics of nuclear spin decoherence and nuclear spin flip-flops in self-assembled InGaAs/GaAs quantum dots are studied experimentally using optically detected nuclear magnetic resonance (NMR). Nuclear spin-echo decay times are found to be in the range 1-4 ms. This is a factor of ~3 longer than in strain-free GaAs/AlGaAs structures and is shown to result from strain-induced quadrupolar effects that suppress nuclear spin flip-flops. The correlation times of the flip-flops are examined using a novel frequency-comb NMR technique and are found to exceed 1 s, a factor of ~1000 longer than in strain-free structures. These findings complement recent studies of electron spin coherence and reveal the paradoxical dual role of the quadrupolar effects in self-assembled quantum dots: large increase of the nuclear spin bath coherence and at the same time significant reduction of the electron spin-qubit coherence. Approaches to increasing electron spin coherence are discussed. In particular the nanohole filled GaAs/AlGaAs quantum dots are an attractive option: while their optical quality matches the self-assembled dots the quadrupolar effects measured in NMR spectra are a factor of 1000 smaller.

Measurement Of Molecular Mobilities Of Polymers

NASA Technical Reports Server (NTRS)

Kim, Soon Sam; Tsay, Fun-Dow

1989-01-01

New molecular-probe technique used to measure molecular mobility of polymer. Method based on use of time-resolved electron-spin resonance (ESR) spectroscopy to monitor decay of transient nutation amplitudes from photoexcited triplet states of probe molecules with which polymer is doped. The higher molecular mobility of polymer matrix, the faster nutation amplitudes of the probe molecules decay.

Two-dimensional electron gas in tricolor oxide interfaces

NASA Astrophysics Data System (ADS)

Cao, Yanwei; Kareev, Michael; Liu, Xiaoran; Middey, Srimanta; Meyers, Derek; Tchakhalian, Jak

2014-03-01

Understanding and manipulating spin of electrons in nanometer scale is the main challenge of current spintronics, recent emergent two-dimensional electron gas in oxide interface provides a good platform to investigate the spin behavior by covering an insulating magnetic oxide layer. In this work, take titanates as an example, ultra-thin tricolor (tri-compound) titanate superlattices ([LaTiO3/SrTiO3/YTiO3]) were grown in a layer-by-layer way by pulsed laser deposition. High sample quality and their electronic structures were characterized by the combination of in-situ photoelectron and ex-situ structure and surface morphology probes. Temperature-dependent sheet resistance indicates the presence of metallic interfaces in both [LaTiO3 /SrTiO3 ] and all the tricolor structures, whereas a [YTiO3 /SrTiO3] bi-layer shows insulating behavior. The tricolor titanate superlattices provide an opportunity to induce tunable spin-polarization into the two-dimensional electron gas (2DEG) with Mott carriers.

Probing the Impact of Solvation on Photoexcited Spin Crossover Complexes with High-Precision X-ray Transient Absorption Spectroscopy

DOE PAGES

Liu, Cunming; Zhang, Jianxin; Lawson Daku, Latevi M.; ...

2017-11-10

Investigating the photoinduced electronic and structural response of bistable molecular building blocks incorporating transition metals in solution phase constitutes a necessary stepping stone for steering their properties towards applications and perfomance optimizations. Here, this paper presents a detailed X-ray transient absorption (XTA) spectroscopy study of a prototypical spin crossover (SCO) complex [Fe II(mbpy) 3] 2+ (where mbpy=4,4’-dimethyl-2,2’-bipyridine) with a [Fe IIN 6] first coordination shell in water (H 2O) and acetonitrile (CH 3CN). The unprecedented data quality of the XTA spectra together with the direct fitting of the difference spectra in k space using a large number of scattering pathsmore » enables resolving the subtle difference in the photoexcited structures of an Fe II complex in two solvents for the first time. Also, compared to the low spin (LS) 1A 1 state, the average Fe-N bond elongations for the photoinduced high spin (HS) 5T 2 state are found to be 0.181 ± 0.003 Å in H 2O and 0.199 ± 0.003 Å in CH 3CN. This difference in structural response is attributed to ligand-solvent interactions that are stronger in H 2O than in CH 3CN for the HS excited state. Our studies demonstrate that, although the metal center of [Fe II(mbpy) 3] 2+ could have been expected to be rather shielded by the three bidentate ligands with quasi-octahedral-coordination, the ligand field strength in the HS excited state is nevertheless indirectly affected by solvation that modifies the charge distribution within the Fe-N covalent bonds. More generally, this work highlights the importance of including solvation effects in order to develop a generalized understanding of the spin-state switching at the atomic level.« less

Mechanism of spin crossover in LaCoO3 resolved by shape magnetostriction in pulsed magnetic fields.

PubMed

Rotter, M; Wang, Z-S; Boothroyd, A T; Prabhakaran, D; Tanaka, A; Doerr, M

2014-11-11

In the scientific description of unconventional transport properties of oxides (spin-dependent transport, superconductivity etc.), the spin-state degree of freedom plays a fundamental role. Because of this, temperature- or magnetic field-induced spin-state transitions are in the focus of solid-state physics. Cobaltites, e.g. LaCoO3, are prominent examples showing these spin transitions. However, the microscopic nature of the spontaneous spin crossover in LaCoO3 is still controversial. Here we report magnetostriction measurements on LaCoO3 in magnetic fields up to 70 T to study the sharp, field-induced transition at Hc ≈ 60 T. Measurements of both longitudinal and transversal magnetostriction allow us to separate magnetovolume and magnetodistortive changes. We find a large increase in volume, but only a very small increase in tetragonal distortion at Hc. The results, supported by electronic energy calculations by the configuration interaction cluster method, provide compelling evidence that above Hc LaCoO3 adopts a correlated low spin/high spin state.

Mechanism of spin crossover in LaCoO3 resolved by shape magnetostriction in pulsed magnetic fields

PubMed Central

Rotter, M.; Wang, Z.-S.; Boothroyd, A. T.; Prabhakaran, D.; Tanaka, A.; Doerr, M.

2014-01-01

In the scientific description of unconventional transport properties of oxides (spin-dependent transport, superconductivity etc.), the spin-state degree of freedom plays a fundamental role. Because of this, temperature- or magnetic field-induced spin-state transitions are in the focus of solid-state physics. Cobaltites, e.g. LaCoO3, are prominent examples showing these spin transitions. However, the microscopic nature of the spontaneous spin crossover in LaCoO3 is still controversial. Here we report magnetostriction measurements on LaCoO3 in magnetic fields up to 70 T to study the sharp, field-induced transition at Hc ≈ 60 T. Measurements of both longitudinal and transversal magnetostriction allow us to separate magnetovolume and magnetodistortive changes. We find a large increase in volume, but only a very small increase in tetragonal distortion at Hc. The results, supported by electronic energy calculations by the configuration interaction cluster method, provide compelling evidence that above Hc LaCoO3 adopts a correlated low spin/high spin state. PMID:25384532

Mechanism of spin crossover in LaCoO3 resolved by shape magnetostriction in pulsed magnetic fields

NASA Astrophysics Data System (ADS)

Rotter, M.; Wang, Z.-S.; Boothroyd, A. T.; Prabhakaran, D.; Tanaka, A.; Doerr, M.

2014-11-01

In the scientific description of unconventional transport properties of oxides (spin-dependent transport, superconductivity etc.), the spin-state degree of freedom plays a fundamental role. Because of this, temperature- or magnetic field-induced spin-state transitions are in the focus of solid-state physics. Cobaltites, e.g. LaCoO3, are prominent examples showing these spin transitions. However, the microscopic nature of the spontaneous spin crossover in LaCoO3 is still controversial. Here we report magnetostriction measurements on LaCoO3 in magnetic fields up to 70 T to study the sharp, field-induced transition at Hc ~ 60 T. Measurements of both longitudinal and transversal magnetostriction allow us to separate magnetovolume and magnetodistortive changes. We find a large increase in volume, but only a very small increase in tetragonal distortion at Hc. The results, supported by electronic energy calculations by the configuration interaction cluster method, provide compelling evidence that above Hc LaCoO3 adopts a correlated low spin/high spin state.

Electron spin resonance of an irradiated single crystal of potassium hydrogen maleate

DOE Office of Scientific and Technical Information (OSTI.GOV)

Iwasaki, Machio; Itoh, Koichi

1963-09-15

Electron spin resonance absorptions of x-irradiated single crystals of potassium hydrogen maleate and potassium deuterium maleate were observed. Both compounds gave the same hyperfine structures, although the slightly sharper line widths were observed for the deuterium exchanged compound.

Focus: Two-dimensional electron-electron double resonance and molecular motions: The challenge of higher frequencies

DOE Office of Scientific and Technical Information (OSTI.GOV)

Franck, John M.; Chandrasekaran, Siddarth; Dzikovski, Boris

2015-06-07

The development, applications, and current challenges of the pulsed ESR technique of two-dimensional Electron-Electron Double Resonance (2D ELDOR) are described. This is a three-pulse technique akin to 2D Exchange Nuclear Magnetic Resonance, but involving electron spins, usually in the form of spin-probes or spin-labels. As a result, it required the extension to much higher frequencies, i.e., microwaves, and much faster time scales, with π/2 pulses in the 2-3 ns range. It has proven very useful for studying molecular dynamics in complex fluids, and spectral results can be explained by fitting theoretical models (also described) that provide a detailed analysis ofmore » the molecular dynamics and structure. We discuss concepts that also appear in other forms of 2D spectroscopy but emphasize the unique advantages and difficulties that are intrinsic to ESR. Advantages include the ability to tune the resonance frequency, in order to probe different motional ranges, while challenges include the high ratio of the detection dead time vs. the relaxation times. We review several important 2D ELDOR studies of molecular dynamics. (1) The results from a spin probe dissolved in a liquid crystal are followed throughout the isotropic → nematic → liquid-like smectic → solid-like smectic → crystalline phases as the temperature is reduced and are interpreted in terms of the slowly relaxing local structure model. Here, the labeled molecule is undergoing overall motion in the macroscopically aligned sample, as well as responding to local site fluctuations. (2) Several examples involving model phospholipid membranes are provided, including the dynamic structural characterization of the boundary lipid that coats a transmembrane peptide dimer. Additionally, subtle differences can be elicited for the phospholipid membrane phases: liquid disordered, liquid ordered, and gel, and the subtle effects upon the membrane, of antigen cross-linking of receptors on the surface of plasma membrane, vesicles can be observed. These 2D ELDOR experiments are performed as a function of mixing time, T{sub m}, i.e., the time between the second and third π/2 pulses, which provides a third dimension. In fact, a fourth dimension may be added by varying the ESR frequency/magnetic field combination. Therefore, (3) it is shown how continuous-wave multifrequency ESR studies enable the decomposition of complex dynamics of, e.g., proteins by virtue of their respective time scales. These studies motivate our current efforts that are directed to extend 2D ELDOR to higher frequencies, 95 GHz in particular (from 9 and 17 GHz), in order to enable multi-frequency 2D ELDOR. This required the development of quasi-optical methods for performing the mm-wave experiments, which are summarized. We demonstrate state-of-the-art 95 GHz 2D ELDOR spectroscopy through its ability to resolve the two signals from a spin probe dissolved in both the lipid phase and the coexisting aqueous phase. As current 95 GHz experiments are restricted by limited spectral coverage of the π/2 pulse, as well as the very short T{sub 2} relaxation times of the electron spins, we discuss how these limitations are being addressed.« less

Spin coherence and 14N ESEEM effects of nitrogen-vacancy centers in diamond with X-band pulsed ESR

NASA Astrophysics Data System (ADS)

Rose, B. C.; Weis, C. D.; Tyryshkin, A. M.; Schenkel, T.; Lyon, S. A.

2017-02-01

Pulsed ESR experiments are reported for ensembles of negatively-charged nitrogen-vacancy centers (NV$^-$) in diamonds at X-band magnetic fields (280-400 mT) and low temperatures (2-70 K). The NV$^-$ centers in synthetic type IIb diamonds (nitrogen impurity concentration $<1$~ppm) are prepared with bulk concentrations of $2\\cdot 10^{13}$ cm$^{-3}$ to $4\\cdot 10^{14}$ cm$^{-3}$ by high-energy electron irradiation and subsequent annealing. We find that a proper post-radiation anneal (1000$^\\circ$C for 60 mins) is critically important to repair the radiation damage and to recover long electron spin coherence times for NV$^-$s. After the annealing, spin coherence times of T$_2 = 0.74$~ms at 5~K are achieved, being only limited by $^{13}$C nuclear spectral diffusion in natural abundance diamonds. At X-band magnetic fields, strong electron spin echo envelope modulation (ESEEM) is observed originating from the central $^{14}$N nucleus. The ESEEM spectral analysis allows for accurate determination of the $^{14}$N nuclear hypefine and quadrupole tensors. In addition, the ESEEM effects from two proximal $^{13}$C sites (second-nearest neighbor and fourth-nearest neighbor) are resolved and the respective $^{13}$C hyperfine coupling constants are extracted.

Theory versus experiment for a family of single-layer compounds with a similar atomic arrangement: (Tl,X )/Si(111 )√{3 }×√{3 }(X =Pb,Sn,Bi,Sb,Te,Se)

NASA Astrophysics Data System (ADS)

Matetskiy, A. V.; Kibirev, I. A.; Mihalyuk, A. N.; Eremeev, S. V.; Gruznev, D. V.; Bondarenko, L. V.; Tupchaya, A. Y.; Zotov, A. V.; Saranin, A. A.

2017-08-01

Two-dimensional compounds made of one monolayer of Tl and one-third monolayer of Pb, Bi, Te, or Se (but not of Sn or Sb) on Si(111) have been found to have a similar atomic arrangement which can be visualized as a √{3 }×√{3 } -periodic honeycomb network of chained Tl trimers with atoms of the second adsorbate occupying the centers of the honeycomb units. Structural and electronic properties of the compounds have been examined in detail theoretically using density functional theory (DFT) calculations and experimentally using low-energy electron diffraction (LEED), scanning tunneling microscopy (STM), and angle-resolved photoelectron spectroscopy (ARPES) observations. It has been found that though structural parameters of the compounds are very similar for all species, the only common feature of their band structure is a considerable spin-splitting of the surface-state bands, while other basic electronic properties vary greatly with a change of species. The Tl-Pb compound is strongly metallic with two metallic surface-state bands; the Tl-Bi compound is also metallic but with a single metallic band; the Tl-Te and Tl-Se compounds appear to be insulators.

A minimal model for the structural energetics of VO2

NASA Astrophysics Data System (ADS)

Kim, Chanul; Marianetti, Chris; The Marianetti Group Team

Resolving the structural, magnetic, and electronic structure of VO2 from the first-principles of quantum mechanics is still a forefront problem despite decades of attention. Hybrid functionals have been shown to qualitatively ruin the structural energetics. While density functional theory (DFT) combined with cluster extensions of dynamical mean-field theory (DMFT) have demonstrated promising results in terms of the electronic properties, structural phase stability has not yet been addressed. In order to capture the basic physics of the structural transition, we propose a minimal model of VO2 based on the one dimensional Peierls-Hubbard model and parameterize this based on DFT calculations of VO2. The total energy versus dimerization in the minimal mode is then solved numerically exactly using density matrix renormalization group (DMRG) and compared to the Hartree-Fock solution. We demonstrate that the Hartree-Fock solution exhibits the same pathologies as DFT+U, and spin density functional theory for that matter, while the DMRG solution is consistent with experimental observation. Our results demonstrate the critical role of non-locality in the total energy, and this will need to be accounted for to obtain a complete description of VO2 from first-principles. The authors acknowledge support from FAME, one of six centers of STARnet, a Semiconductor Research Corporation program sponsored by MARCO and DARPA.

Laser photoelectron spectroscopy of MnH - and FeH - : Electronic structures of the metal hydrides, identification of a low-spin excited state of MnH, and evidence for a low-spin ground state of FeH

NASA Astrophysics Data System (ADS)

Stevens, Amy E.; Feigerle, C. S.; Lineberger, W. C.

1983-05-01

The laser photoelectron spectra of MnH- and MnD-, and FeH- and FeD- are reported. A qualitative description of the electronic structure of the low-spin and high-spin states of the metal hydrides is developed, and used to interpret the spectra. A diagonal transition in the photodetachment to the known high-spin, 7Σ+, ground state of MnH is observed. An intense off-diagonal transition to a state of MnH, at 1725±50 cm-1 excitation energy, is attributed to loss of an antibonding electron from MnH-, to yield a low-spin quintet state of MnH. For FeH- the photodetachment to the ground state is an off-diagonal transition, attributed to loss of the antibonding electron from FeH-, to yield a low-spin quartet ground state of FeH. A diagonal transition results in an FeH state at 1945±55 cm-1; this state of FeH is assigned as the lowest-lying high-spin sextet state of FeH. An additional excited state of MnH and two other excited states of FeH are observed. Excitation energies for all the states are reported; vibrational frequencies and bond lengths for the ions and several states of the neutrals are also determined from the spectra. The electron affinity of MnH is found to be 0.869±0.010 eV; and the electron affinity of FeH is determined to be 0.934±0.011 eV. Spectroscopic constants for the various deuterides are also reported.

Fine structure and optical pumping of spins in individual semiconductor quantum dots

NASA Astrophysics Data System (ADS)

Bracker, Allan S.; Gammon, Daniel; Korenev, Vladimir L.

2008-11-01

We review spin properties of semiconductor quantum dots and their effect on optical spectra. Photoluminescence and other types of spectroscopy are used to probe neutral and charged excitons in individual quantum dots with high spectral and spatial resolution. Spectral fine structure and polarization reveal how quantum dot spins interact with each other and with their environment. By taking advantage of the selectivity of optical selection rules and spin relaxation, optical spin pumping of the ground state electron and nuclear spins is achieved. Through such mechanisms, light can be used to process spins for use as a carrier of information.

Resonant inelastic x-ray scattering probes the electron-phonon coupling in the spin liquid κ -(BEDT-TTF)2Cu2(CN) 3

NASA Astrophysics Data System (ADS)

Ilakovac, V.; Carniato, S.; Foury-Leylekian, P.; Tomić, S.; Pouget, J.-P.; Lazić, P.; Joly, Y.; Miyagawa, K.; Kanoda, K.; Nicolaou, A.

2017-11-01

Resonant inelastic x-ray scattering at the N K edge reveals clearly resolved harmonics of the anion plane vibrations in the κ -(BEDT-TTF) 2Cu2 (CN) 3 spin-liquid insulator. Tuning the incoming light energy at the K edge of two distinct N sites permits us to excite different sets of phonon modes. The cyanide (CN) stretching mode is selected at the edge of the ordered N sites which are more strongly connected to the bis(ethylenedithio)tetrathiafulvalene (BEDT-TTF) molecules, while positionally disordered N sites show multimode excitation. Combining measurements with calculations on an anion plane cluster permits us to estimate the site-dependent electron-phonon coupling of the modes related to nitrogen excitation.

2D layered transport properties from topological insulator Bi2Se3 single crystals and micro flakes

PubMed Central

Chiatti, Olivio; Riha, Christian; Lawrenz, Dominic; Busch, Marco; Dusari, Srujana; Sánchez-Barriga, Jaime; Mogilatenko, Anna; Yashina, Lada V.; Valencia, Sergio; Ünal, Akin A.; Rader, Oliver; Fischer, Saskia F.

2016-01-01

Low-field magnetotransport measurements of topological insulators such as Bi2Se3 are important for revealing the nature of topological surface states by quantum corrections to the conductivity, such as weak-antilocalization. Recently, a rich variety of high-field magnetotransport properties in the regime of high electron densities (∼1019 cm−3) were reported, which can be related to additional two-dimensional layered conductivity, hampering the identification of the topological surface states. Here, we report that quantum corrections to the electronic conduction are dominated by the surface states for a semiconducting case, which can be analyzed by the Hikami-Larkin-Nagaoka model for two coupled surfaces in the case of strong spin-orbit interaction. However, in the metallic-like case this analysis fails and additional two-dimensional contributions need to be accounted for. Shubnikov-de Haas oscillations and quantized Hall resistance prove as strong indications for the two-dimensional layered metallic behavior. Temperature-dependent magnetotransport properties of high-quality Bi2Se3 single crystalline exfoliated macro and micro flakes are combined with high resolution transmission electron microscopy and energy-dispersive x-ray spectroscopy, confirming the structure and stoichiometry. Angle-resolved photoemission spectroscopy proves a single-Dirac-cone surface state and a well-defined bulk band gap in topological insulating state. Spatially resolved core-level photoelectron microscopy demonstrates the surface stability. PMID:27270569

High resolution photoelectron imaging of UO{sup −} and UO{sub 2}{sup −} and the low-lying electronic states and vibrational frequencies of UO and UO{sub 2}

DOE Office of Scientific and Technical Information (OSTI.GOV)

Czekner, Joseph; Lopez, Gary V.; Wang, Lai-Sheng

2014-12-28

We report a study of the electronic and vibrational structures of the gaseous uranium monoxide and dioxide molecules using high-resolution photoelectron imaging. Vibrationally resolved photoelectron spectra are obtained for both UO{sup −} and UO{sub 2}{sup −}. The spectra for UO{sub 2}{sup −} are consistent with, but much better resolved than a recent study using a magnetic-bottle photoelectron analyzer [W. L. Li et al., J. Chem. Phys. 140, 094306 (2014)]. The electron affinity (EA) of UO is reported for the first time as 1.1407(7) eV, whereas a much more accurate EA is obtained for UO{sub 2} as 1.1688(6) eV. The symmetricmore » stretching modes for the neutral and anionic ground states, and two neutral excited states for UO{sub 2} are observed, as well as the bending mode for the neutral ground state. These vibrational frequencies are consistent with previous experimental and theoretical results. The stretching vibrational modes for the ground state and one excited state are observed for UO. The current results for UO and UO{sub 2} are compared with previous theoretical calculations including relativistic effects and spin-orbit coupling. The accurate experimental data reported here provide more stringent tests for future theoretical methods for actinide-containing species.« less

Structural Changes Correlated with Magnetic Spin State Isomorphism in the S2 State of the Mn4CaO5 Cluster in the Oxygen-Evolving Complex of Photosystem II

PubMed Central

Chatterjee, Ruchira; Han, Guangye; Kern, Jan; Gul, Sheraz; Fuller, Franklin D.; Garachtchenko, Anna; Young, Iris; Weng, Tsu-Chien; Nordlund, Dennis; Alonso-Mori, Roberto; Bergmann, Uwe; Sokaras, Dimosthenis; Hatakeyama, Makoto; Yachandra, Vittal K.; Yano, Junko

2016-01-01

The Mn4CaO5 cluster in Photosystem II catalyzes the four-electron redox reaction of water oxidation in natural photosynthesis. This catalytic reaction cycles through four intermediate states (Si, i = 0 to 4), involving changes in the redox state of the four Mn atoms in the cluster. Recent studies suggest the presence and importance of isomorphous structures within the same redox/intermediate S-state. It is highly likely that geometric and electronic structural flexibility play a role in the catalytic mechanism. Among the catalytic intermediates that have been identified experimentally thus far, there is clear evidence of such isomorphism in the S2 state, with a high-spin (5/2) (HS) and a low spin (1/2) (LS) form, identified and characterized by their distinct electron paramagnetic resonance (EPR spectroscopy) signals. We studied these two S2 isomers with Mn extended X-ray absorption fine structure (EXAFS) and absorption and emission spectroscopy (XANES/XES) to characterize the structural and electronic structural properties. The geometric and electronic structure of the HS and LS S2 states are different as determined using Mn EXAFS and XANES/XES, respectively. The Mn K-edge XANES and XES for the HS form are different from the LS and indicate a slightly lower positive charge on the Mn atoms compared to the LS form. Based on the EXAFS results which are clearly different, we propose possible structural differences between the two spin states. Such structural and magnetic redox-isomers if present at room temperature, will likely play a role in the mechanism for water-exchange/oxidation in photosynthesis. PMID:28044099

Structural changes correlated with magnetic spin state isomorphism in the S 2 state of the Mn 4CaO 5 cluster in the oxygen-evolving complex of photosystem II

DOE PAGES

Chatterjee, Ruchira; Han, Guangye; Kern, Jan; ...

2016-05-09

The Mn 4CaO 5 cluster in photosystem II catalyzes the four-electron redox reaction of water oxidation in natural photosynthesis. This catalytic reaction cycles through four intermediate states (S i, i = 0 to 4), involving changes in the redox state of the four Mn atoms in the cluster. Recent studies suggest the presence and importance of isomorphous structures within the same redox/intermediate S-state. It is highly likely that geometric and electronic structural flexibility play a role in the catalytic mechanism. Among the catalytic intermediates that have been identified experimentally thus far, there is clear evidence of such isomorphism in themore » S2 state, with a high-spin (5/2) (HS) and a low spin (1/2) (LS) form, identified and characterized by their distinct electron paramagnetic resonance (EPR spectroscopy) signals. We studied these two S2 isomers with Mn extended X-ray absorption fine structure (EXAFS) and absorption and emission spectroscopy (XANES/XES) to characterize the structural and electronic structural properties. The geometric and electronic structure of the HS and LS S2 states are different as determined using Mn EXAFS and XANES/XES, respectively. The Mn K-edge XANES and XES for the HS form are different from the LS and indicate a slightly lower positive charge on the Mn atoms compared to the LS form. Based on the EXAFS results which are clearly different, we propose possible structural differences between the two spin states. As a result, such structural and magnetic redox-isomers if present at room temperature, will likely play a role in the mechanism for water-exchange/oxidation in photosynthesis.« less

Effect of disorder on the magnetic and electronic structure of a prospective spin-gapless semiconductor MnCrVAl

DOE PAGES

Kharel, P.; Herran, J.; Lukashev, P.; ...

2016-12-19

Recent discovery of a new class of materials, spin-gapless semiconductors (SGS), has attracted considerable attention in the last few years, primarily due to potential applications in the emerging field of spin-based electronics (spintronics). Here, we investigate structural, electronic, and magnetic properties of one potential SGS compound, MnCrVAl, using various experimental and theoretical techniques. Our calculations show that this material exhibits ≈ 0.5 eV band gap for the majority-spin states, while for the minority-spin it is nearly gapless. The calculated magnetic moment for the completely ordered structure is 2.9 μB/f.u., which is different from our experimentally measured value of almost zero.more » Here, this discrepancy is explained by the structural disorder. In particular, A2 type disorder, where Mn or Cr atoms exchange their positions with Al atoms, results in induced antiferromagnetic exchange coupling, which, at a certain level of disorder, effectively reduces the total magnetic moment to zero. This is consistent with our x-ray diffraction measurements which indicate the presence of A2 disorder in all of our samples. In addition, we also show that B2 disorder does not result in antiferromagnetic exchange coupling and therefore does not significantly reduce the total magnetic moment.« less

Finger-gate manipulated quantum transport in Dirac materials

NASA Astrophysics Data System (ADS)

Kleftogiannis, Ioannis; Tang, Chi-Shung; Cheng, Shun-Jen

2015-05-01

We investigate the quantum transport properties of multichannel nanoribbons made of materials described by the Dirac equation, under an in-plane magnetic field. In the low energy regime, positive and negative finger-gate potentials allow the electrons to make intra-subband transitions via hole-like or electron-like quasibound states (QBS), respectively, resulting in dips in the conductance. In the high energy regime, double dip structures in the conductance are found, attributed to spin-flip or spin-nonflip inter-subband transitions through the QBSs. Inverting the finger-gate polarity offers the possibility to manipulate the spin polarized electronic transport to achieve a controlled spin-switch.

Structural, electronic and magnetic properties of metal thiophosphate InPS4

NASA Astrophysics Data System (ADS)

Rajpoot, Priyanka; Nayak, Vikas; Kumari, Meena; Yadav, Priya; Nautiyal, Shashank; Verma, U. P.

2017-05-01

The non-centrosymmetric crystal, InPS4, has been investigated by means of density functional theory (DFT). In this paper we have calculated the structural parameters, electronic band structures, density of states plot and magnetic properties using full potential linearized augmented plane wave (FP-LAPW) method. The exchange correlation has been solved employing the generalised gradient approximation due to Perdew-Burke-Ernzerhof. The calculations are performed both without spin as well as spin polarized. The results show that InPS4 is an indirect band gap semiconductor with (N-Г) energy gap of 2.32eV (without spin) and 1.86eV in spin up and down channels.The obtained lattice parameters and energy gap agree well with the experimental results. Our reported magnetic moment results show that the property of InPS4is nonmagnetic.

Analogies between Vanadoborates and Planar Aromatic Hydrocarbons: A High-Spin Analogue of Aromaticity.

PubMed

King, R Bruce

2017-12-23

The vanadium-vanadium interactions in the polygonal aggregates of d¹ vanadium(IV) atoms, with a total of 4 k + 2 vanadium electrons ( k an integer) imbedded in an electronically inactive borate matrix in certain vanadoborate structures are analogous to the ring carbon-carbon interactions in diamagnetic planar cyclic hydrocarbons. They thus represent a high-spin analogue of aromaticity. Thus, the vanadoborate anion [V₆B 20 O 50 H₈] 8- with six V(IV) electrons (i.e., 4 k + 2 for k = 1) contains a macrohexagon of d¹ V(IV) atoms with four unpaired electrons. This high-spin system is related to the low-spin aromaticity in the diamagnetic benzene having six π electrons. Similarly, the vanadoborate anion [V 10 B 28 O 74 H₈] 16- with ten V(IV) electrons (i.e., 4 k + 2 for k = 2) contains a macrodecagon of d¹ V(IV) atoms with eight unpaired electrons. Again, this high-spin system is related to the aromaticity in the diamagnetic 1,6-methanol[10]annulene, having ten π electrons.

Pulsed EPR measurements on reaction rate constants for addition of photo-generated radicals to double bonds of diethyl fumarate and diethyl maleate

NASA Astrophysics Data System (ADS)

Takahashi, Hirona; Hagiwara, Kenta; Kawai, Akio

2016-11-01

Addition reaction of photo-generated radicals to double bonds of diethyl fumarate (deF) and diethyl maleate (deM), which are geometrical isomers, was studied by means of time-resolved- (TR-) and pulsed-electron paramagnetic resonance (EPR). Analysis of TR-EPR spectra indicates that adduct radicals from deF and deM should have the same structure. The double bonds of these monomers are converted to single ones by addition reaction, which allows hindered internal rotation to give the same structure of adduct radical. The rate constants for addition reaction of photo-generated radicals were determined by Stern-Volmer analysis of the decay time of electron spin-echo intensity of these radicals measured by the pulsed EPR method. Rate constants for deF were found to be larger than those for deM. This relation is in good consistent with efficiency of polymerisation of deF and deM. Experimentally determined rate constants were evaluated by introducing the addition reaction model on the basis of two important factors enthalpy and polar effects.

Ultrafast optical excitation of magnetic skyrmions

NASA Astrophysics Data System (ADS)

Ogawa, N.; Seki, S.; Tokura, Y.

2015-04-01

Magnetic skyrmions in an insulating chiral magnet Cu2OSeO3 were studied by all-optical spin wave spectroscopy. The spins in the conical and skyrmion phases were excited by the impulsive magnetic field from the inverse-Faraday effect, and resultant spin dynamics were detected by using time-resolved magneto-optics. Clear dispersions of the helimagnon were observed, which is accompanied by a distinct transition into the skyrmion phase, by sweeping temperature and magnetic field. In addition to the collective excitations of skyrmions, i.e., rotation and breathing modes, several spin precession modes were identified, which would be specific to optical excitation. The ultrafast, nonthermal, and local excitation of the spin systems by photons would lead to the efficient manipulation of nano-magnetic structures.

Singlet and triplet trions in WS2 monolayer encapsulated in hexagonal boron nitride.

PubMed

Vaclavkova, D; Wyzula, J; Nogajewski, K; Bartos, M; Slobodeniuk, A O; Faugeras, C; Potemski, M; Molas, M R

2018-08-10

Embedding a WS 2 monolayer in flakes of hexagonal boron nitride allowed us to resolve and study the photoluminescence response due to both singlet and triplet states of negatively charged excitons (trions) in this atomically thin semiconductor. The energy separation between the singlet and triplet states has been found to be relatively small reflecting rather weak effects of the electron-electron exchange interaction for the trion triplet in a WS 2 monolayer, which involves two electrons with the same spin but from different valleys. Polarization-resolved experiments demonstrate that the helicity of the excitation light is better preserved in the emission spectrum of the triplet trion than in that of the singlet trion. Finally, the singlet (intravalley) trions are found to be observable even at ambient conditions whereas the emission due to the triplet (intervalley) trions is only efficient at low temperatures.

Spin quenching assisted by a strongly anisotropic compression behavior in MnP

NASA Astrophysics Data System (ADS)

Han, Fei; Wang, Di; Wang, Yonggang; Li, Nana; Bao, Jin-Ke; Li, Bing; Botana, Antia S.; Xiao, Yuming; Chow, Paul; Chung, Duck Young; Chen, Jiuhua; Wan, Xiangang; Kanatzidis, Mercouri G.; Yang, Wenge; Mao, Ho-Kwang

2018-02-01

We studied the crystal structure and spin state of MnP under high pressure with synchrotron x-ray diffraction and x-ray emission spectroscopy (XES). MnP has an exceedingly strong anisotropy in compressibility, with the primary compressible direction along the b axis of the Pnma structure. XES reveals a pressure-driven quenching of the spin state in MnP. First-principles calculations suggest that the strongly anisotropic compression behavior significantly enhances the dispersion of the Mn d-orbitals and the splitting of the d-orbital levels compared to the hypothetical isotropic compression behavior. Thus, we propose spin quenching results mainly from the significant enhancement of the itinerancy of d electrons and partly from spin rearrangement occurring in the split d-orbital levels near the Fermi level. This explains the fast suppression of magnetic ordering in MnP under high pressure. The spin quenching lags behind the occurrence of superconductivity at ˜8 GPa implying that spin fluctuations govern the electron pairing for superconductivity.

Spin quenching assisted by a strongly anisotropic compression behavior in MnP

DOE Office of Scientific and Technical Information (OSTI.GOV)

Han, Fei; Wang, Di; Wang, Yonggang

We studied the crystal structure and spin state of MnP under high pressure with synchrotron X-ray diffraction and X-ray emission spectroscopy. MnP has an exceedingly strong anisotropy in compressibility, with the primary compressible direction along the b axis of the Pnma structure. X-ray emission spectroscopy reveals a pressure-driven quenching of the spin state in MnP. First-principles calculations suggest that the strongly anisotropic compression behavior significantly enhances the dispersion of the Mn d-orbitals and the splitting of the d-orbital levels compared to the hypothetical isotropic compression behavior. Thus, we propose spin quenching results mainly from the significant enhancement of the itinerancymore » of d electrons and partly from spin rearrangement occurring in the split d-orbital levels near the Fermi level. This explains the fast suppression of magnetic ordering in MnP under high pressure. The spin quenching lags behind the occurrence of superconductivity at ~8 GPa implying that spin fluctuations govern the electron pairing for superconductivity.« less

Transient nutation electron spin resonance spectroscopy on spin-correlated radical pairs: A theoretical analysis on hyperfine-induced nuclear modulations

NASA Astrophysics Data System (ADS)

Weber, Stefan; Kothe, Gerd; Norris, James R.

1997-04-01

The influence of anisotropic hyperfine interaction on transient nutation electron paramagnetic resonance (EPR) of light-induced spin-correlated radical pairs is studied theoretically using the density operator formalism. Analytical expressions for the time evolution of the transient EPR signal during selective microwave excitation of single transitions are derived for a model system comprised of a weakly coupled radical pair and one hyperfine-coupled nucleus with I=1/2. Zero-quantum electron coherence and single-quantum nuclear coherence are created as a result of the sudden light-induced generation of the radical pair state from a singlet-state precursor. Depending on the relative sizes of the nuclear Zeeman frequency and the secular and pseudo-secular parts of the hyperfine coupling, transitions between levels with different nuclear spin orientations are predicted to modulate the time-dependent EPR signal. These modulations are in addition to the well-known transient nutations and electron zero-quantum precessions. Our calculations provide insight into the mechanism of recent experimental observations of coherent nuclear modulations in the time-resolved EPR signals of doublets and radical pairs. Two distinct mechanisms of the modulations are presented for various microwave magnetic field strengths. The first modulation scheme arises from electron and nuclear coherences initiated by the laser excitation pulse and is "read out" by the weak microwave magnetic field. While the relative modulation depth of these oscillations with respect to the signal intensity is independent of the Rabi frequency, ω1, the frequencies of this coherence phenomenon are modulated by the effective microwave amplitude and determined by the nuclear Zeeman interaction and hyperfine coupling constants as well as the electron-electron spin exchange and dipolar interactions between the two radical pair halves. In a second mechanism the modulations are both created and detected by the microwave radiation. Here, the laser pulse merely defines the beginning of the microwave-induced coherent time evolution. This second mechanism appears the most consistent with current experimental observations.

Electron Tunneling in Lithium Ammonia Solutions Probed by Frequency-Dependent Electron-Spin Relaxation Studies

PubMed Central

Maeda, Kiminori; Lodge, Matthew T.J.; Harmer, Jeffrey; Freed, Jack H.; Edwards, Peter P.

2012-01-01

Electron transfer or quantum tunneling dynamics for excess or solvated electrons in dilute lithium-ammonia solutions have been studied by pulse electron paramagnetic resonance (EPR) spectroscopy at both X- (9.7 GHz) and W-band (94 GHz) frequencies. The electron spin-lattice (T1) and spin-spin (T2) relaxation data indicate an extremely fast transfer or quantum tunneling rate of the solvated electron in these solutions which serves to modulate the hyperfine (Fermi-contact) interaction with nitrogen nuclei in the solvation shells of ammonia molecules surrounding the localized, solvated electron. The donor and acceptor states of the solvated electron in these solutions are the initial and final electron solvation sites found before, and after, the transfer or tunneling process. To interpret and model our electron spin relaxation data from the two observation EPR frequencies requires a consideration of a multi-exponential correlation function. The electron transfer or tunneling process that we monitor through the correlation time of the nitrogen Fermi-contact interaction has a time scale of (1–10)×10−12 s over a temperature range 230–290K in our most dilute solution of lithium in ammonia. Two types of electron-solvent interaction mechanisms are proposed to account for our experimental findings. The dominant electron spin relaxation mechanism results from an electron tunneling process characterized by a variable donor-acceptor distance or range (consistent with such a rapidly fluctuating liquid structure) in which the solvent shell that ultimately accepts the transferring electron is formed from random, thermal fluctuations of the liquid structure in, and around, a natural hole or Bjerrum-like defect vacancy in the liquid. Following transfer and capture of the tunneling electron, further solvent-cage relaxation with a timescale of ca. 10−13 s results in a minor contribution to the electron spin relaxation times. This investigation illustrates the great potential of multi-frequency EPR measurements to interrogate the microscopic nature and dynamics of ultra fast electron transfer or quantum-tunneling processes in liquids. Our results also impact on the universal issue of the role of a host solvent (or host matrix, e.g. a semiconductor) in mediating long-range electron transfer processes and we discuss the implications of our results with a range of other materials and systems exhibiting the phenomenon of electron transfer. PMID:22568866

Spin-polarized exciton quantum beating in hybrid organic-inorganic perovskites

NASA Astrophysics Data System (ADS)

Odenthal, Patrick; Talmadge, William; Gundlach, Nathan; Wang, Ruizhi; Zhang, Chuang; Sun, Dali; Yu, Zhi-Gang; Valy Vardeny, Z.; Li, Yan S.

2017-09-01

Hybrid organic-inorganic perovskites have emerged as a new class of semiconductors that exhibit excellent performance as active layers in photovoltaic solar cells. These compounds are also highly promising materials for the field of spintronics due to their large and tunable spin-orbit coupling, spin-dependent optical selection rules, and their predicted electrically tunable Rashba spin splitting. Here we demonstrate the optical orientation of excitons and optical detection of spin-polarized exciton quantum beating in polycrystalline films of the hybrid perovskite CH3NH3PbClxI3-x. Time-resolved Faraday rotation measurement in zero magnetic field reveals unexpectedly long spin lifetimes exceeding 1 ns at 4 K, despite the large spin-orbit couplings of the heavy lead and iodine atoms. The quantum beating of exciton states in transverse magnetic fields shows two distinct frequencies, corresponding to two g-factors of 2.63 and -0.33, which we assign to electrons and holes, respectively. These results provide a basic picture of the exciton states in hybrid perovskites, and suggest they hold potential for spintronic applications.

Development of structure in natural silk spinning and poly(vinyl alcohol) hydrogel formation

NASA Astrophysics Data System (ADS)

Willcox, Patricia Jeanene

This research involves the characterization of structure and structure formation in aqueous systems. Particularly, these studies investigate the effect of various processing variables on the structure formation that occurs upon conversion from aqueous solution to fiber or hydrogel. The two processes studied include natural silk fiber spinning and physical gelation of poly(vinyl alcohol), PVOH, in water. The techniques employed combine cryogenic technology for sample preparation and direct observation by transmission electron microscopy with electron diffraction, atomic force microscopy, optical rheometry, X-ray scattering and optical microscopy. In order to explore the full range of structure formation in natural silk spinning, studies are conducted in vivo and in vitro. In vivo structural investigations are accomplished through the cryogenic quenching and subsequent microtoming of live silk-spinning animals, Nephila clavipes (spider) and Bombyx mori (silkworm). Observations made using transmission electron microscopy, electron diffraction and atomic force microscopy indicate a cholesteric liquid crystalline mesophase of aqueous silk fibroin in both species. The mechanism of structure formation in solution is studied in vitro using optical rheometry on aqueous solutions made from regenerated Bombyx mori cocoon silk. Concentrated solutions exhibit birefringence under flow, with a wormlike conformation of the silk molecules in concentrated salt solution. Changes in salt concentration and pH of the aqueous silk solutions result in differing degrees of alignment and aggregation. These results suggest that structural control in the natural silk spinning process is accomplished by chemical manipulation of the electrostatic interactions and hydrogen bonding between chains. Application of cryogenic methods in transmission electron microscopy also provides a unique look at hydration-dependent structures in gels of poly(vinyl alcohol) produced by freeze-thaw processing. Morphologies ranging from circular pores to fibrillar networks are observed in gels formed from aqueous PVOH solutions subjected to cycles of freezing and thawing. These morphologies can be directly associated with the progressive nature of the mechanism of gelation as it proceeds from liquid-liquid phase separation to crystallization with increased cycling. A comparison of the structures produced by cycling and by aging suggests that there is a similarity in structural changes, but a superposition of the effects of cycling and aging is not possible.

Constraints on Exotic Spin-Dependent Interactions Between Matter and Antimatter from Antiprotonic Helium Spectroscopy

NASA Astrophysics Data System (ADS)

Ficek, Filip; Fadeev, Pavel; Flambaum, Victor V.; Jackson Kimball, Derek F.; Kozlov, Mikhail G.; Stadnik, Yevgeny V.; Budker, Dmitry

2018-05-01

Heretofore undiscovered spin-0 or spin-1 bosons can mediate exotic spin-dependent interactions between standard model particles. Here, we carry out the first search for semileptonic spin-dependent interactions between matter and antimatter. We compare theoretical calculations and spectroscopic measurements of the hyperfine structure of antiprotonic helium to constrain exotic spin- and velocity-dependent interactions between electrons and antiprotons.

Constraints on Exotic Spin-Dependent Interactions Between Matter and Antimatter from Antiprotonic Helium Spectroscopy.

PubMed

Ficek, Filip; Fadeev, Pavel; Flambaum, Victor V; Jackson Kimball, Derek F; Kozlov, Mikhail G; Stadnik, Yevgeny V; Budker, Dmitry

2018-05-04

Heretofore undiscovered spin-0 or spin-1 bosons can mediate exotic spin-dependent interactions between standard model particles. Here, we carry out the first search for semileptonic spin-dependent interactions between matter and antimatter. We compare theoretical calculations and spectroscopic measurements of the hyperfine structure of antiprotonic helium to constrain exotic spin- and velocity-dependent interactions between electrons and antiprotons.

Strain-induced phase transition and electron spin-polarization in graphene spirals

PubMed Central

Zhang, Xiaoming; Zhao, Mingwen

2014-01-01

Spin-polarized triangular graphene nanoflakes (t-GNFs) serve as ideal building blocks for the long-desired ferromagnetic graphene superlattices, but they are always assembled to planar structures which reduce its mechanical properties. Here, by joining t-GNFs in a spiral way, we propose one-dimensional graphene spirals (GSs) with superior mechanical properties and tunable electronic structures. We demonstrate theoretically the unique features of electron motion in the spiral lattice by means of first-principles calculations combined with a simple Hubbard model. Within a linear elastic deformation range, the GSs are nonmagnetic metals. When the axial tensile strain exceeds an ultimate strain, however, they convert to magnetic semiconductors with stable ferromagnetic ordering along the edges. Such strain-induced phase transition and tunable electron spin-polarization revealed in the GSs open a new avenue for spintronics devices. PMID:25027550

Strain-induced phase transition and electron spin-polarization in graphene spirals.

PubMed

Zhang, Xiaoming; Zhao, Mingwen

2014-07-16

Spin-polarized triangular graphene nanoflakes (t-GNFs) serve as ideal building blocks for the long-desired ferromagnetic graphene superlattices, but they are always assembled to planar structures which reduce its mechanical properties. Here, by joining t-GNFs in a spiral way, we propose one-dimensional graphene spirals (GSs) with superior mechanical properties and tunable electronic structures. We demonstrate theoretically the unique features of electron motion in the spiral lattice by means of first-principles calculations combined with a simple Hubbard model. Within a linear elastic deformation range, the GSs are nonmagnetic metals. When the axial tensile strain exceeds an ultimate strain, however, they convert to magnetic semiconductors with stable ferromagnetic ordering along the edges. Such strain-induced phase transition and tunable electron spin-polarization revealed in the GSs open a new avenue for spintronics devices.

Bilinear magnetoelectric resistance as a probe of three-dimensional spin texture in topological surface states

DOE PAGES

He, Pan; Zhang, Steven S. -L.; Zhu, Dapeng; ...

2018-02-05

Surface states of three-dimensional topological insulators exhibit the phenomenon of spin-momentum locking, whereby the orientation of an electron spin is determined by its momentum. Probing the spin texture of these states is of critical importance for the realization of topological insulator devices, but the main technique currently available is spin-and angle-resolved photoemission spectroscopy. Here in this paper we reveal a close link between the spin texture and a new kind of magnetoresistance, which depends on the relative orientation of the current with respect to the magnetic field as well as the crystallographic axes, and scales linearly with both the appliedmore » electric and magnetic fields. This bilinear magnetoelectric resistance can be used to map the spin texture of topological surface states by simple transport measurements. For a prototypical Bi 2Se 3 single layer, we can map both the in-plane and out-of-plane components of the spin texture (the latter arising from hexagonal warping). Theoretical calculations suggest that the bilinear magnetoelectric resistance originates from conversion of a non-equilibrium spin current into a charge current under application of the external magnetic field.« less

Bilinear magnetoelectric resistance as a probe of three-dimensional spin texture in topological surface states

DOE Office of Scientific and Technical Information (OSTI.GOV)

He, Pan; Zhang, Steven S. -L.; Zhu, Dapeng

Surface states of three-dimensional topological insulators exhibit the phenomenon of spin-momentum locking, whereby the orientation of an electron spin is determined by its momentum. Probing the spin texture of these states is of critical importance for the realization of topological insulator devices, but the main technique currently available is spin-and angle-resolved photoemission spectroscopy. Here in this paper we reveal a close link between the spin texture and a new kind of magnetoresistance, which depends on the relative orientation of the current with respect to the magnetic field as well as the crystallographic axes, and scales linearly with both the appliedmore » electric and magnetic fields. This bilinear magnetoelectric resistance can be used to map the spin texture of topological surface states by simple transport measurements. For a prototypical Bi 2Se 3 single layer, we can map both the in-plane and out-of-plane components of the spin texture (the latter arising from hexagonal warping). Theoretical calculations suggest that the bilinear magnetoelectric resistance originates from conversion of a non-equilibrium spin current into a charge current under application of the external magnetic field.« less

Femtosecond stimulated Raman evidence for charge-transfer character in pentacene singlet fission.

PubMed

Hart, Stephanie M; Silva, W Ruchira; Frontiera, Renee R

2018-02-07

Singlet fission is a spin-allowed process in which an excited singlet state evolves into two triplet states. We use femtosecond stimulated Raman spectroscopy, an ultrafast vibrational technique, to follow the molecular structural evolution during singlet fission in order to determine the mechanism of this process. In crystalline pentacene, we observe the formation of an intermediate characterized by pairs of excited state peaks that are red- and blue-shifted relative to the ground state features. We hypothesize that these features arise from the formation of cationic and anionic species due to partial transfer of electron density from one pentacene molecule to a neighboring molecule. These observations provide experimental evidence for the role of states with significant charge-transfer character which facilitate the singlet fission process in pentacene. Our work both provides new insight into the singlet fission mechanism in pentacene and demonstrates the utility of structurally-sensitive time-resolved spectroscopic techniques in monitoring ultrafast processes.

Electron Density Distribution Changes of Magnesiowüstite With Pressure

NASA Astrophysics Data System (ADS)

Diamond, M. R.; Popov, D.; Shen, G.; Jeanloz, R.

2017-12-01

Magnesiowüstite is one of the dominant minerals in the earth's lower mantle; its density and elasticity, substantially altered by its spin crossover, have direct consequence to interpreting deep-earth geophysical data. High-resolution single-crystal x-ray diffraction data can portray the 3-dimensional distribution of electron density through the Fourier transform of measured form factors. Here we present experimentally measured changes in electron density distribution of single-crystal (Mg.85,Fe.15)O as it goes through its iron(II) high-spin to low-spin electronic transition between about 40 and 60 GPa [Lin and Tsuchiya, 2008], in a diamond-anvil cell. As (Mg,Fe)O undergoes a pressure induced spin crossover (from high spin at low pressure to low spin at high pressure) due to overlap of its eg orbitals, the t2g orbitals become more pronounced to due a higher population of electrons, while the eg orbitals diminish. The spin splitting energy becomes increasingly unfavorable compared to the spin orbital pairing energy. By looking at the population of electrons at different directions in real space, we directly observe these changes in orbital occupation leading up to and during the spin crossover. Since high-Mg magnesiowüstite has a high symmetry structure at these pressure conditions, detecting relative changes in electron density distribution (comparing subsequent pressure steps) is feasible by collecting high resolution data offered by high-energy X rays and wide opening-angle diamond-anvil cells.

Analysis of Rotationally Resolved Spectra to Non-Degenerate (a''_1) Upper-State Vibronic Levels in the tilde{A} ^2E''-tilde{X}^2A^'_2 Electronic Transition of NO_3

NASA Astrophysics Data System (ADS)

Roudjane, Mourad; Codd, Terrance Joseph; Chen, Ming-Wei; Tran, Henry; Melnik, Dmitry G.; Miller, Terry A.; Stanton, John F.

2015-06-01

The vibronic structure of the tilde{A}-tilde{X} electronic spectrum of NO_3 has been observed using both room-temperature and jet-cooled samples. A recent analysis of this structure is consistent with the Jahn-Teller effect (JTE) in the e^' ν_3 vibrational mode (N-O stretch) being quite strong while the JTE in the e^' ν_4 mode (O-N-O) bend) is rather weak. Electronic structure calculations qualitatively predict these results but the calculated magnitude of the JTE is quantitatively inconsistent with the spectral analysis. Rotationally resolved spectra have been obtained for over a dozen vibronic bands of the tilde{A}-tilde{X} electronic transition in NO_3. An analysis of these spectra should provide considerably more experimental information about the JTE in the tilde{A} state of NO_3 as the rotational structure should be quite sensitive to the geometric distortion of the molecule due to the JTE. This talk will focus upon the parallel bands, which terminate on tilde{A} state levels of a''_1 vibronic symmetry, which were the subject of a preliminary analysis reported at this meeting in 2014. We have now recorded the rotational structure of over a half-dozen parallel bands and have completed analysis on the 3^1_0 and 3^1_0 4^1_0 transitions with several other bands being reasonably well understood. Two general conclusions emerge from this work. (i) All the spectral bands show evidence of perturbations which can reasonably be assumed to result from interactions of the observed tilde{A} state levels with high vibrational levels of the tilde{X} state. The perturbations range from severe in some bands to quite modest in others. (ii) Analyses of observed spectra, insofar as the perturbations permit, have all been performed with an oblate symmetric top model including only additional spin-rotation effects. This result is, of course, consistent with an effective, undistorted geometry for NO_3 of D3h symmetry on the rotational timescale.

Iridates and RuCl3 - from Heisenberg antiferromagnets to potential Kitaev spin-liquids

NASA Astrophysics Data System (ADS)

van den Brink, Jeroen

The observed richness of topological states on the single-electron level prompts the question what kind of topological phases can develop in more strongly correlated, many-body electron systems. Correlation effects, in particular intra- and inter-orbital electron-electron interactions, are very substantial in 3 d transition-metal compounds such as the copper oxides, but the spin-orbit coupling (SOC) is weak. In 5 d transition-metal compounds such as iridates, the interesting situation arises that the SOC and Coulomb interactions meet on the same energy scale. The electronic structure of iridates thus depends on a strong competition between the electronic hopping amplitudes, local energy-level splittings, electron-electron interaction strengths, and the SOC of the Ir 5d electrons. The interplay of these ingredients offers the potential to stabilise relatively well-understood states such as a 2D Heisenberg-like antiferromagnet in Sr2IrO4, but in principle also far more exotic ones, such a topological Kitaev quantum spin liquid, in (hyper)honeycomb iridates. I will discuss the microscopic electronic structures of these iridates, their proximity to idealized Heisenberg and Kitaev models and our contributions to establishing the physical factors that appear to have preempted the realization of quantum spin liquid phases so far and include a discussion on the 4d transition metal chloride RuCl3. Supported by SFB 1143 of the Deutsche Forschungsgemeinschaft.

Coherent manipulation of non-thermal spin order in optical nuclear polarization experiments

NASA Astrophysics Data System (ADS)

Buntkowsky, Gerd; Ivanov, Konstantin L.; Zimmermann, Herbert; Vieth, Hans-Martin

2017-03-01

Time resolved measurements of Optical Nuclear Polarization (ONP) have been performed on hyperpolarized triplet states in molecular crystals created by light excitation. Transfer of the initial electron polarization to nuclear spins has been studied in the presence of radiofrequency excitation; the experiments have been performed with different pulse sequences using different doped molecular systems. The experimental results clearly demonstrate the dominant role of coherent mechanisms of spin order transfer, which manifest themselves in well pronounced oscillations. These oscillations are of two types, precessions and nutations, having characteristic frequencies, which are the same for the different molecular systems and the pulse sequences applied. Hence, precessions and nutations constitute a general feature of polarization transfer in ONP experiments. In general, coherent manipulation of spin order transfer creates a powerful resource for improving the performance of the ONP method, which paves the way to strong signal enhancement in nuclear magnetic resonance.

Dirac electron in a chiral space-time crystal created by counterpropagating circularly polarized plane electromagnetic waves

NASA Astrophysics Data System (ADS)

Borzdov, G. N.

2017-10-01

The family of solutions to the Dirac equation for an electron moving in an electromagnetic lattice with the chiral structure created by counterpropagating circularly polarized plane electromagnetic waves is obtained. At any nonzero quasimomentum, the dispersion equation has two solutions which specify bispinor wave functions describing electron states with different energies and mean values of momentum and spin operators. The inversion of the quasimomentum results in two other linearly independent solutions. These four basic wave functions are uniquely defined by eight complex scalar functions (structural functions), which serve as convenient building blocks of the relations describing the electron properties. These properties are illustrated in graphical form over a wide range of quasimomenta. The superpositions of two basic wave functions describing different spin states and corresponding to (i) the same quasimomentum (unidirectional electron states with the spin precession) and (ii) the two equal-in-magnitude but oppositely directed quasimomenta (bidirectional electron states) are also treated.

Spatially-resolved studies on the role of defects and boundaries in electronic behavior of 2D materials

NASA Astrophysics Data System (ADS)

Hus, Saban M.; Li, An-Ping

2017-08-01

Two-dimensional (2D) materials are intrinsically heterogeneous. Both localized defects, such as vacancies and dopants, and mesoscopic boundaries, such as surfaces and interfaces, give rise to compositional or structural heterogeneities. The presence of defects and boundaries can break lattice symmetry, modify the energy landscape, and create quantum confinement, leading to fascinating electronic properties different from the ;ideal; 2D sheets. This review summarizes recent progress in understanding the roles of defects and boundaries in electronic, magnetic, thermoelectric, and transport properties of 2D layered materials. The focus is on the understanding of correlation of atomic-scale structural information with electronic functions by interrogating heterogeneities individually. The materials concerned are graphene, transition metal dichalcogenides (TMDs), hexagonal boron nitride (hBN), and topological insulators (TIs). The experimental investigations benefit from new methodologies and techniques in scanning tunneling microscopy (STM), including spin-polarized STM, scanning tunneling potentiometry (STP), scanning tunneling thermopower microscopy, and multi-probe STM. The experimental effort is complemented by the computational and theoretical approaches, capable of discriminating between closely competing states and achieving the length scales necessary to bridge across features such as local defects and complex heterostructures. The goal is to provide a general view of current understanding and challenges in studying the heterogeneities in 2D materials and to evaluate the potential of controlling and exploiting these heterogeneities for novel functionalities and electron devices.

An approach to spin-resolved molecular gas microscopy

NASA Astrophysics Data System (ADS)

Covey, Jacob P.; De Marco, Luigi; Acevedo, Óscar L.; Rey, Ana Maria; Ye, Jun

2018-04-01

Ultracold polar molecules are an ideal platform for studying many-body physics with long-range dipolar interactions. Experiments in this field have progressed enormously, and several groups are pursuing advanced apparatus for manipulation of molecules with electric fields as well as single-atom-resolved in situ detection. Such detection has become ubiquitous for atoms in optical lattices and tweezer arrays, but has yet to be demonstrated for ultracold polar molecules. Here we present a proposal for the implementation of site-resolved microscopy for polar molecules, and specifically discuss a technique for spin-resolved molecular detection. We use numerical simulation of spin dynamics of lattice-confined polar molecules to show how such a scheme would be of utility in a spin-diffusion experiment.

Electronic structure and magnetic properties of dilute U impurities in metals

NASA Astrophysics Data System (ADS)

Mohanta, S. K.; Cottenier, S.; Mishra, S. N.

2016-05-01

The electronic structure and magnetic moment of dilute U impurity in metallic hosts have been calculated from first principles. The calculations have been performed within local density approximation of the density functional theory using Augmented plane wave+local orbital (APW+lo) technique, taking account of spin-orbit coupling and Coulomb correlation through LDA+U approach. We present here our results for the local density of states, magnetic moment and hyperfine field calculated for an isolated U impurity embedded in hosts with sp-, d- and f-type conduction electrons. The results of our systematic study provide a comprehensive insight on the pressure dependence of 5f local magnetism in metallic systems. The unpolarized local density of states (LDOS), analyzed within the frame work of Stoner model suggest the occurrence of local moment for U in sp-elements, noble metals and f-block hosts like La, Ce, Lu and Th. In contrast, U is predicted to be nonmagnetic in most transition metal hosts except in Sc, Ti, Y, Zr, and Hf consistent with the results obtained from spin polarized calculation. The spin and orbital magnetic moments of U computed within the frame of LDA+U formalism show a scaling behavior with lattice compression. We have also computed the spin and orbital hyperfine fields and a detail analysis has been carried out. The host dependent trends for the magnetic moment, hyperfine field and 5f occupation reflect pressure induced change of electronic structure with U valency changing from 3+ to 4+ under lattice compression. In addition, we have made a detailed analysis of the impurity induced host spin polarization suggesting qualitatively different roles of f-band electrons on moment stability. The results presented in this work would be helpful towards understanding magnetism and spin fluctuation in U based alloys.

Online SAXS investigations of polymeric hollow fibre membranes.

PubMed

Pranzas, P Klaus; Knöchel, Arndt; Kneifel, Klemens; Kamusewitz, Helmut; Weigel, Thomas; Gehrke, Rainer; Funari, Sérgio S; Willumeit, Regine

2003-07-01

Polymeric membranes are used in industrial and analytical separation techniques. In this study small-angle X-ray scattering (SAXS) with synchrotron radiation has been applied for in-situ characterisation during formation of polymeric membranes. The spinning of a polyetherimide (PEI) hollow fibre membrane was chosen for investigation of dynamic aggregation processes during membrane formation, because it allows the measurement of the dynamic equilibrium at different distances from the spinning nozzle. With this system it is possible to resolve structural changes in the nm-size range which occur during membrane formation on the time-scale of milliseconds. Integral structural parameters, like radius of gyration and pair-distance distribution, were determined. Depending on the chosen spinning parameters, e.g. the flow ratio between polymer solution and coagulant water, significant changes in the scattering curves have been observed. The data are correlated with the distance from the spinning nozzle in order to get information about the kinetics of membrane formation which has fundamental influence on structure and properties of the membrane.

Picosecond Control of Photogenerated Radical Pair Lifetimes Using a Stable Third Radical.

PubMed

Horwitz, Noah E; Phelan, Brian T; Nelson, Jordan N; Krzyaniak, Matthew D; Wasielewski, Michael R

2016-05-12

Photoinduced electron transfer reactions in organic donor-acceptor systems leading to long-lived radical ion pairs (RPs) have attracted broad interest for their potential applications in fields as diverse as solar energy conversion and spintronics. We present the photophysics and spin dynamics of an electron donor - electron acceptor - stable radical system consisting of a meta-phenylenediamine (mPD) donor covalently linked to a 4-aminonaphthalene-1,8-dicarboximide (ANI) electron-accepting chromophore as well as an α,γ-bisdiphenylene-β-phenylallyl (BDPA) stable radical. Selective photoexcitation of ANI produces the BDPA-mPD(+•)-ANI(-•) triradical in which the mPD(+•)-ANI(-•) RP spins are strongly exchange coupled. The presence of BDPA is found to greatly increase the RP intersystem crossing rate from the initially photogenerated BDPA-(1)(mPD(+•)-ANI(-•)) to BDPA-(3)(mPD(+•)-ANI(-•)), resulting in accelerated RP recombination via the triplet channel to produce BDPA-mPD-(3*)ANI as compared to a reference molecule lacking the BDPA radical. The RP recombination rates observed are much faster than those previously reported for weakly coupled triradical systems. Time-resolved EPR spectroscopy shows that this process is also associated with strong spin polarization of the stable radical. Overall, these results show that RP intersystem crossing rates can be strongly influenced by stable radicals nearby strongly coupled RP systems, making it possible to use a third spin to control RP lifetimes down to a picosecond time scale.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yan, Qiang; Zhou, Liping, E-mail: zhoulp@suda.edu.cn; Cheng, Jue-Fei

Electronic structures and coherent quantum transport properties are explored for spin-crossover molecule iron-benzene Fe(Bz){sub 2} using density functional theory combined with non-equilibrium Green’s function. High- and low-spin states are investigated for two different lead-molecule junctions. It is found that the asymmetrical T-shaped contact junction in the high-spin state behaves as an efficient spin filter while it has a smaller conductivity than that in the low-spin state. Large spin Seebeck effect is also observed in asymmetrical T-shaped junction. Spin-polarized properties are absent in the symmetrical H-shaped junction. These findings strongly suggest that both the electronic and contact configurations play significant rolesmore » in molecular devices and metal-benzene complexes are promising materials for spintronics and thermo-spintronics.« less

Electrical detection of nuclear spins in organic light-emitting diodes

NASA Astrophysics Data System (ADS)

Malissa, H.; Kavand, M.; Waters, D. P.; Lupton, J. M.; Vardeny, Z. V.; Saam, B.; Boehme, C.

2014-03-01

We present pulsed combined electrically detected electron paramagnetic and nuclear magnetic resonance experiments on MEH-PPV OLEDs. Spin dynamics in these structures are governed by hyperfine interactions between charge carriers and the surrounding hydrogen nuclei, which are abundant in these materials. Hyperfine coupling has been observed by monitoring the device current during coherent spin excitation. Electron spin echoes (ESEs) are detected by applying one additional readout pulse at the time of echo formation. This allows for the application of high-resolution spectroscopy based on ESE detection, such as electron spin echo envelope modulation (ESEEM) and electron nuclear double resonance (ENDOR) available for electrical detection schemes. We conduct electrically detected ESEEM and ENDOR experiments and show how hyperfine interactions in MEH-PPV with and without deuterated polymer side groups can be observed by device current measurements. We acknowledge support by the Department of Energy, Office of Basic Energy Sciences under Award #DE-SC0000909.

Electronic structure of charge- and spin-controlled Sr(1-(x+y))La(x+y)Ti(1-x)Cr(x)O3.

PubMed

Iwasawa, H; Yamakawa, K; Saitoh, T; Inaba, J; Katsufuji, T; Higashiguchi, M; Shimada, K; Namatame, H; Taniguchi, M

2006-02-17

We present the electronic structure of Sr(1-(x+y))La(x+y)Ti(1-x)Cr(x)O3 investigated by high-resolution photoemission spectroscopy. In the vicinity of the Fermi level, it was found that the electronic structure was composed of a Cr 3d local state with the t(2g)3 configuration and a Ti 3d itinerant state. The energy levels of these Cr and Ti 3d states are well interpreted by the difference of the charge-transfer energy of both ions. The spectral weight of the Cr 3d state is completely proportional to the spin concentration x irrespective of the carrier concentration y, indicating that the spin density can be controlled by x as desired. In contrast, the spectral weight of the Ti 3d state is not proportional to y, depending on the amount of Cr doping.

Understanding Unimer Exchange Processes in Block Copolymer Micelles using NMR Diffusometry, Time-Resolved NMR, and SANS

NASA Astrophysics Data System (ADS)

Madsen, Louis; Kidd, Bryce; Li, Xiuli; Miller, Katherine; Cooksey, Tyler; Robertson, Megan

Our team seeks to understand dynamic behaviors of block copolymer micelles and their interplay with encapsulated cargo molecules. Quantifying unimer and cargo exchange rates micelles can provide critical information for determining mechanisms of unimer exchange as well as designing systems for specific cargo release dynamics. We are exploring the utility of NMR spectroscopy and diffusometry techniques as complements to existing SANS and fluorescence methods. One promising new method involves time-resolved NMR spin relaxation measurements, wherein mixing of fully protonated and 2H-labeled PEO-b-PCL micelles solutions shows an increase in spin-lattice relaxation time (T1) with time after mixing. This is due to a weakening in magnetic environment surrounding 1H spins as 2H-bearing unimers join fully protonated micelles. We are measuring time constants for unimer exchange of minutes to hours, and we expect to resolve times of <1 min. This method can work on any solution NMR spectrometer and with minimal perturbation to chemical structure (as in dye-labelled fluorescence methods). Multimodal NMR can complement existing characterization tools, expanding and accelerating dynamics measurements for polymer micelle, nanogel, and nanoparticle developers.

Quantized spin-momentum transfer in atom-sized magnetic systems

NASA Astrophysics Data System (ADS)

Loth, Sebastian

2010-03-01

Our ability to quickly access the vast amounts of information linked in the internet is owed to the miniaturization of magnetic data storage. In modern disk drives the tunnel magnetoresistance effect (TMR) serves as sensitive reading mechanism for the nanoscopic magnetic bits [1]. At its core lies the ability to control the flow of electrons with a material's magnetization. The inverse effect, spin transfer torque (STT), allows one to influence a magnetic layer by high current densities of spin-polarized electrons and carries high hopes for applications in non-volatile magnetic memory [2]. We show that equivalent processes are active in quantum spin systems. We use a scanning tunneling microscope (STM) operating at low temperature and high magnetic field to address individual magnetic structures and probe their spin excitations by inelastic electron tunneling [3]. As model system we investigate transition metal atoms adsorbed to a copper nitride layer grown on a Cu crystal. The magnetic atoms on the surface possess well-defined spin states [4]. Transfer of one magnetic atom to the STM tip's apex creates spin-polarization in the probe tip. The combination of functionalized tip and surface adsorbed atom resembles a TMR structure where the magnetic layers now consist of one magnetic atom each. Spin-polarized current emitted from the probe tip not only senses the magnetic orientation of the atomic spin system, it efficiently transfers spin angular momentum and pumps the quantum spin system between the different spin states. This enables further exploration of the microscopic mechanisms for spin-relaxation and stability of quantum spin systems. [4pt] [1] Zhu and Park, Mater. Today 9, 36 (2006).[0pt] [2] Huai, AAPPS Bulletin 18, 33 (2008).[0pt] [3] Heinrich et al., Science 306, 466 (2004).[0pt] [4] Hirjibehedin et al., Science 317, 1199 (2007).

Spin-orbit coupling and surface magnetism coexisting in spin-dependent low-energy He+-ion surface scattering

NASA Astrophysics Data System (ADS)

Suzuki, T. T.; Sakai, O.

2017-04-01

Surface magnetism is analyzed by spin-dependent He+-ion neutralization (the Auger neutralization) in the vicinity of a surface using an electron spin-polarized low-energy He+-ion beam [spin-polarized ion scattering spectroscopy (SP-ISS)]. Recently, spin-orbit coupling (SOC) has been found to act as another mechanism of spin-dependent low-energy He+-ion scattering. Thus, it is crucial for surface magnetism analyses by SP-ISS to separate those two mechanisms. In the present study, we investigated the spin-induced asymmetry in scattering of low-energy He+ ions on ultrathin Au and Sn films as well as the oxygen adsorbate on a magnetized-Fe(100) surface where these two mechanisms may coexist. We found that the Fe surface magnetism immediately disappeared with the growth of those overlayers. On the other hand, we observed no induced spin polarization in the Au and Sn thin films even in the very initial stage of the growth. We also observed that the spin asymmetry of the O adsorbate was induced by the magnetism of the underlying Fe substrate. The present study demonstrates that the two mechanisms of the spin-asymmetric He+-ion scattering (the ion neutralization and SOC) can be separated by an azimuthal-angle-resolved SP-ISS measurement.

Electronic Structures of Silicene Nanoribbons: Two-Edge-Chemistry Modification and First-Principles Study.

PubMed

Yao, Yin; Liu, Anping; Bai, Jianhui; Zhang, Xuanmei; Wang, Rui

2016-12-01

In this paper, we investigate the structural and electronic properties of zigzag silicene nanoribbons (ZSiNRs) with edge-chemistry modified by H, F, OH, and O, using the ab initio density functional theory method and local spin-density approximation. Three kinds of spin polarized configurations are considered: nonspin polarization (NM), ferromagnetic spin coupling for all electrons (FM), ferromagnetic ordering along each edge, and antiparallel spin orientation between the two edges (AFM). The H, F, and OH groups modified 8-ZSiNRs have the AFM ground state. The directly edge oxidized (O1) ZSiNRs yield the same energy and band structure for NM, FM, and AFM configurations, owning to the same s p (2) hybridization. And replacing the Si atoms on the two edges with O atoms (O2) yields FM ground state. The edge-chemistry-modified ZSiNRs all exhibit metallic band structures. And the modifications introduce special edge state strongly localized at the Si atoms in the edge, except for the O1 form. The modification of the zigzag edges of silicene nanoribbons is a key issue to apply the silicene into the field effect transistors (FETs) and gives more necessity to better understand the experimental findings.

Spin-valley locking in the normal state of a transition-metal dichalcogenide superconductor.

PubMed

Bawden, L; Cooil, S P; Mazzola, F; Riley, J M; Collins-McIntyre, L J; Sunko, V; Hunvik, K W B; Leandersson, M; Polley, C M; Balasubramanian, T; Kim, T K; Hoesch, M; Wells, J W; Balakrishnan, G; Bahramy, M S; King, P D C

2016-05-23

Metallic transition-metal dichalcogenides (TMDCs) are benchmark systems for studying and controlling intertwined electronic orders in solids, with superconductivity developing from a charge-density wave state. The interplay between such phases is thought to play a critical role in the unconventional superconductivity of cuprates, Fe-based and heavy-fermion systems, yet even for the more moderately-correlated TMDCs, their nature and origins have proved controversial. Here, we study a prototypical example, 2H-NbSe2, by spin- and angle-resolved photoemission and first-principles theory. We find that the normal state, from which its hallmark collective phases emerge, is characterized by quasiparticles whose spin is locked to their valley pseudospin. This results from a combination of strong spin-orbit interactions and local inversion symmetry breaking, while interlayer coupling further drives a rich three-dimensional momentum dependence of the underlying Fermi-surface spin texture. These findings necessitate a re-investigation of the nature of charge order and superconducting pairing in NbSe2 and related TMDCs.

Dependence of spin pumping and spin transfer torque upon Ni81Fe19 thickness in Ta/Ag /Ni 81Fe19/Ag/Co 2MnGe /Ag /Ta spin-valve structures

NASA Astrophysics Data System (ADS)

Durrant, C. J.; Shelford, L. R.; Valkass, R. A. J.; Hicken, R. J.; Figueroa, A. I.; Baker, A. A.; van der Laan, G.; Duffy, L. B.; Shafer, P.; Klewe, C.; Arenholz, E.; Cavill, S. A.; Childress, J. R.; Katine, J. A.

2017-10-01

Spin pumping has been studied within Ta / Ag / Ni81Fe19 (0-5 nm) / Ag (6 nm) / Co2MnGe (5 nm) / Ag / Ta large-area spin-valve structures, and the transverse spin current absorption of Ni81Fe19 sink layers of different thicknesses has been explored. In some circumstances, the spin current absorption can be inferred from the modification of the Co2MnGe source layer damping in vector network analyzer ferromagnetic resonance (VNA-FMR) experiments. However, the spin current absorption is more accurately determined from element-specific phase-resolved x-ray ferromagnetic resonance (XFMR) measurements that directly probe the spin transfer torque (STT) acting on the sink layer at the source layer resonance. Comparison with a macrospin model allows the real part of the effective spin mixing conductance to be extracted. We find that spin current absorption in the outer Ta layers has a significant impact, while sink layers with thicknesses of less than 0.6 nm are found to be discontinuous and superparamagnetic at room temperature, and lead to a noticeable increase of the source layer damping. For the thickest 5-nm sink layer, increased spin current absorption is found to coincide with a reduction of the zero frequency FMR linewidth that we attribute to improved interface quality. This study shows that the transverse spin current absorption does not follow a universal dependence upon sink layer thickness but instead the structural quality of the sink layer plays a crucial role.

Electronic-structure calculations of praseodymium metal by means of modified density-functional theory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Svane, A.; Trygg, J.; Johansson, B.

1997-09-01

Electronic-structure calculations of elemental praseodymium are presented. Several approximations are used to describe the Pr f electrons. It is found that the low-pressure, trivalent phase is well described using either the self-interaction corrected (SIC) local-spin-density (LSD) approximation or the generalized-gradient approximation (GGA) with spin and orbital polarization (OP). In the SIC-LSD approach the Pr f electrons are treated explicitly as localized with a localization energy given by the self-interaction of the f orbital. In the GGA+OP scheme the f-electron localization is described by the onset of spin and orbital polarization, the energetics of which is described by spin-moment formation energymore » and a term proportional to the total orbital moment, L{sub z}{sup 2}. The high-pressure phase is well described with the f electrons treated as band electrons, in either the LSD or the GGA approximations, of which the latter describes more accurately the experimental equation of state. The calculated pressure of the transition from localized to delocalized behavior is 280 kbar in the SIC-LSD approximation and 156 kbar in the GGA+OP approach, both comparing favorably with the experimentally observed transition pressure of 210 kbar. {copyright} {ital 1997} {ital The American Physical Society}« less

Structure of siderite FeCO[subscript 3] to 56 GPa and hysteresis of its spin-pairing transition

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lavina, Barbara; Dera, Przemyslaw; Downs, Robert T.

2010-09-17

The structure of siderite, FeCO{sub 3}, was determined to 56 GPa, beyond the spin-pairing transition of its iron d electrons. Fe{sup 2+} in the siderite structure is in the high-spin state at low pressures and transforms to the low-spin (LS) state over a narrow pressure range, 44 to 45 GPa, that is concomitant with a shrinkage of the octahedral bond distance by 4%, and a volume collapse of 10%. The structural rearrangements associated with the electronic transition are nearly isotropic in contrast with other properties of siderite, which mostly are highly anisotropic. Robust refinements of the crystal structure from single-crystalmore » x-ray diffraction data were performed at small pressure intervals in order to accurately evaluate the variation in the interatomic distances and to define the geometry of the carbonate hosting LS-Fe{sup 2+}. Thermal vibrations are remarkably lowered in the LS-Sd as shown by atomic displacement parameters. The formation of like-spin domains at the transition shows a hysteresis of more than 3 GPa, compatible with a strong cooperative contribution of neighboring clusters to the transition.« less

Lesion-induced DNA weak structural changes detected by pulsed EPR spectroscopy combined with site-directed spin labelling.

PubMed

Sicoli, Giuseppe; Mathis, Gérald; Aci-Sèche, Samia; Saint-Pierre, Christine; Boulard, Yves; Gasparutto, Didier; Gambarelli, Serge

2009-06-01

Double electron-electron resonance (DEER) was applied to determine nanometre spin-spin distances on DNA duplexes that contain selected structural alterations. The present approach to evaluate the structural features of DNA damages is thus related to the interspin distance changes, as well as to the flexibility of the overall structure deduced from the distance distribution. A set of site-directed nitroxide-labelled double-stranded DNA fragments containing defined lesions, namely an 8-oxoguanine, an abasic site or abasic site analogues, a nick, a gap and a bulge structure were prepared and then analysed by the DEER spectroscopic technique. New insights into the application of 4-pulse DEER sequence are also provided, in particular with respect to the spin probes' positions and the rigidity of selected systems. The lesion-induced conformational changes observed, which were supported by molecular dynamics studies, confirm the results obtained by other, more conventional, spectroscopic techniques. Thus, the experimental approaches described herein provide an efficient method for probing lesion-induced structural changes of nucleic acids.

LSMS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Eisenbach, Markus; Li, Ying Wai; Liu, Xianglin

2017-12-01

LSMS is a first principles, Density Functional theory based, electronic structure code targeted mainly at materials applications. LSMS calculates the local spin density approximation to the diagonal part of the electron Green's function. The electron/spin density and energy are easily determined once the Green's function is known. Linear scaling with system size is achieved in the LSMS by using several unique properties of the real space multiple scattering approach to the Green's function.

Suppression of spin and optical gaps in phosphorene quantum dots

NASA Astrophysics Data System (ADS)

Zhang, Yingjie; Sheng, Weidong

2018-05-01

Electronic structure and optical properties of triangular phosphorene quantum dots have been investigated theoretically. Based on systematic configuration interaction calculations, the ground and excited states of the interacting many-electron system together with its optical absorption spectrum are obtained. For the nanodot with 60 phosphorus atoms in various dielectric environments, it is found that the spin gap of the correlated system surprisingly overlaps its optical gap over a large range of the effective dielectric constant. The overlapping of the spin and optical gaps can be attributed to the fact that the extra correlation energy in the spin singlet almost compensates the exchange energy in the spin triplet in the presence of strong long-range electron-electron interactions. Moreover, both the spin and optical gaps are shown to be greatly suppressed as the screening effect becomes strong. When the dielectric constant decreases below 2.65, it is seen that the spin gap becomes negative and the quantum dot undergoes a phase transition from nonmagnetic to ferromagnetic. Our results are compared with the previous experimental and theoretical works.

From single magnetic adatoms on superconductors to coupled spin chains

NASA Astrophysics Data System (ADS)

Franke, Katharina J.

Magnetic adsorbates on conventional s-wave superconductors lead to exchange interactions that induce Yu-Shiba-Rusinov (YSR) states inside the superconducting energy gap. Here, we employ tunneling spectroscopy at 1.1 K to investigate magnetic atoms and chains on superconducting Pb surfaces. We show that individual Manganese (Mn) atoms give rise to a distinct number of YSR-states. The single-atom junctions are stable over several orders of magnitude in conductance. We identify single-electron tunneling as well as Andreev processes. When the atoms are brought into sufficiently close distance, the Shiba states hybridize, thus giving rise to states with bonding and anti-bonding character. It has been shown that the Pb(110) surface supports the self-assembly of Fe chains, which exhibit fingerprints of Majorana bound states. Using superconducting tips, we resolve a rich subgap structure including peaks at zero energy and low-energy resonances, which overlap with the putative Majorana states. We gratefully acknowledge funding by the Deutsche Forschungsgemeinschaft through collaborative research Grant Sfb 658, and through Grant FR2726/4, as well by the European Research Council through Consolidator Grant NanoSpin.

Unified one-band Hubbard model for magnetic and electronic spectra of the parent compounds of cuprate superconductors

NASA Astrophysics Data System (ADS)

Dalla Piazza, B.; Mourigal, M.; Guarise, M.; Berger, H.; Schmitt, T.; Zhou, K. J.; Grioni, M.; Rønnow, H. M.

2012-03-01

Using low-energy projection of the one-band t-t'-t'' Hubbard model we derive an effective spin Hamiltonian and its spin-wave expansion to order 1/S. We fit the spin-wave dispersion of several parent compounds to the high-temperature superconducting cuprates La2CuO4, Sr2CuO2Cl2, and Bi2Sr2YCu2O8. Our accurate quantitative determination of the one-band Hubbard model parameters allows prediction and comparison to experimental results. Among those we discuss the two-magnon Raman peak line shape, the K-edge resonant inelastic x-ray scattering 500-meV peak, and the high-energy kink in the angle-resolved photoemission spectroscopy quasiparticle dispersion, also known as the waterfall feature.

Magnetic field effect on the optoelectronic response of amorphous hydrogenated silicon

NASA Astrophysics Data System (ADS)

McLaughlin, Ryan; Sun, Dali; Zhang, Chuang; Ehrenfreund, Eitan; Vardeny, Zeev Valy

We have studied the magneto-photoluminescence and magneto photoconductivity in amorphous hydrogenated silicon (a-Si:H) thin films and devices as a function of temperature up to field of 5 Tesla. The magnetic field effects (MFE) are interpreted as spin mixing between spin-singlet and spin-triplet charge pairs due to the ''delta- g'' mechanism that is based on the g-value difference between the paired electron and hole, which directly affects the rate of radiative recombination and charge carrier separation, respectively. We found that the MFE(B) response does not form a Lorentzian (that is expected from the ''delta- g'' mechanism) due to disorder in the film that results in a broad distribution of e-h recombination rates, which could be extracted directly by time-resolved photoluminescence.

Efficient spin filter and spin valve in a single-molecule magnet Fe{sub 4} between two graphene electrodes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zu, Feng-Xia; School of Physics and Wuhan National High Magnetic Field Center, Huazhong University of Science and Technology, Wuhan 430074; Gao, Guo-Ying

2015-12-21

We propose a magnetic molecular junction consisting of a single-molecule magnet Fe{sub 4} connected two graphene electrodes and investigate transport properties, using the nonequilibrium Green's function method in combination with spin-polarized density-functional theory. The results show that the device can be used as a nearly perfect spin filter with efficiency approaching 100%. Our calculations provide crucial microscopic information how the four iron cores of the chemical structure are responsible for the spin-resolved transmissions. Moreover, it is also found that the device behaves as a highly efficient spin valve, which is an excellent candidate for spintronics of molecular devices. The ideamore » of combining single-molecule magnets with graphene provides a direction in designing a new class of molecular spintronic devices.« less

First-principles investigation of the interlayer coupling in chromium-trichloride-a layered magnetic insulator

NASA Astrophysics Data System (ADS)

Kc, Santosh; McGuire, Michael A.; Cooper, Valentino R.

The crystallographic, electronic and magnetic properties of layered CrCl3were investigated using density functional theory. We use the newly developed spin van der Waals density functional (svdW-DF) in order to explore the atomic, electronic and magnetic structure. Our results indicate that treatment of the long-range interlayer forces with the svdW-DF improves the accuracy of crystal structure predictions. The cleavage energy was estimated to be 0.29 J/m2 suggesting that CrCl3 should be cleavable using standard mechanical exfoliation techniques. The inclusion of spin in the non-local vdW-DF allows us to directly probe the coupling between the magnetic structure and lattice degrees of freedom. An understanding of the link between electronic, magnetic and structural properties can be useful for novel device applications such as magnetoelectric devices, spin transistors, and 2D magnet. Research was sponsored by the US DOE, Office of Science, BES, MSED and Early Career Research Programs and used resources at NERSC.

Structure and dynamics of spin-labeled insulin entrapped in a silica matrix by the sol-gel method.

PubMed

Vanea, E; Gruian, C; Rickert, C; Steinhoff, H-J; Simon, V

2013-08-12

The structure and conformational dynamics of insulin entrapped into a silica matrix was monitored during the sol to maturated-gel transition by electron paramagnetic resonance (EPR) spectroscopy. Insulin was successfully spin-labeled with iodoacetamide and the bifunctional nitroxide reagent HO-1944. Room temperature continuous wave (cw) EPR spectra of insulin were recorded to assess the mobility of the attached spin labels. Insulin conformation and its distribution within the silica matrix were studied using double electron-electron resonance (DEER) and low-temperature cw-EPR. A porous oxide matrix seems to form around insulin molecules with pore diameters in the order of a few nanometers. Secondary structure of the encapsulated insulin investigated by Fourier transform infrared spectroscopy proved a high structural integrity of insulin even in the dried silica matrix. The results show that silica encapsulation can be used as a powerful tool to effectively isolate and functionally preserve biomolecules during preparation, storage, and release.

Room-temperature electron spin relaxation of nitroxides immobilized in trehalose: Effect of substituents adjacent to NO-group

NASA Astrophysics Data System (ADS)

Kuzhelev, Andrey A.; Strizhakov, Rodion K.; Krumkacheva, Olesya A.; Polienko, Yuliya F.; Morozov, Denis A.; Shevelev, Georgiy Yu.; Pyshnyi, Dmitrii V.; Kirilyuk, Igor A.; Fedin, Matvey V.; Bagryanskaya, Elena G.

2016-05-01

Trehalose has been recently promoted as efficient immobilizer of biomolecules for room-temperature EPR studies, including distance measurements between attached nitroxide spin labels. Generally, the structure of nitroxide influences the electron spin relaxation times, being crucial parameters for room-temperature pulse EPR measurements. Therefore, in this work we investigated a series of nitroxides with different substituents adjacent to NO-moiety including spirocyclohexane, spirocyclopentane, tetraethyl and tetramethyl groups. Electron spin relaxation times (T1, Tm) of these radicals immobilized in trehalose were measured at room temperature at X- and Q-bands (9/34 GHz). In addition, a comparison was made with the corresponding relaxation times in nitroxide-labeled DNA immobilized in trehalose. In all cases phase memory times Tm were close to 700 ns and did not essentially depend on structure of substituents. Comparison of temperature dependences of Tm at T = 80-300 K shows that the benefit of spirocyclohexane substituents well-known at medium temperatures (∼100-180 K) becomes negligible at 300 K. Therefore, unless there are specific interactions between spin labels and biomolecules, the room-temperature value of Tm in trehalose is weakly dependent on the structure of substituents adjacent to NO-moiety of nitroxide. The issues of specific interactions and stability of nitroxide labels in biological media might be more important for room temperature pulsed dipolar EPR than differences in intrinsic spin relaxation of radicals.

Atomic Scale Control of Competing Electronic Phases in Ultrathin Correlated Oxides

NASA Astrophysics Data System (ADS)

Shen, Kyle

2015-03-01

Ultrathin epitaxial thin films offer a number of unique advantages for engineering the electronic properties of correlated transition metal oxides. For example, atomically thin films can be synthesized to artificially confine electrons in two dimensions. Furthermore, using a substrate with a mismatched lattice constant can impose large biaxial strains of larger than 3% (Δa / a), much larger than can achieved in bulk single crystals. Since these dimensionally confined or strained systems may necessarily be less than a few unit cells thick, investigating their properties and electronic structure can be particularly challenging. We employ a combination of reactive oxide molecular beam epitaxy (MBE) and angle-resolved photoemission spectroscopy (ARPES) to investigate how dimensional confinement and epitaxial strain can be used to manipulate electronic properties and structure in correlated transition metal oxide thin films. We describe some of our recent work manipulating and studying the electronic structure of ultrathin LaNiO3 through a thickness-driven metal-insulator transition between three and two unit cells (Nature Nanotechnology 9, 443, 2014), where coherent Fermi liquid-like quasiparticles are suppressed at the metal-insulator transition observed in transport. We also will describe some recent unpublished work using epitaxial strain to drive a Lifshitz transition in atomically thin films of the spin-triplet ruthenate superconductor Sr2RuO4, where we also can dramatically alter the quasiparticle scattering rates and drive the system towards non-Fermi liquid behavior near the critical point (B. Burganov, C. Adamo, in preparation). Funding provided by the Office of Naval Research and Air Force Office of Scientific Research.

Electronic structure and optical properties of GdNi2Mnx compounds

NASA Astrophysics Data System (ADS)

Knyazev, Yu. V.; Lukoyanov, A. V.; Kuz'min, Yu. I.; Gaviko, V. S.

2018-02-01

The electronic structure and optical properties of GdNi2Mnx compounds (x = 0, 0.4, 0.6) were investigated. Spin-polarized electronic structure calculations were performed in the approximation of local electron spin density corrected for strong electron correlations using the LSDA+U method. The changes in the magnetic moments and exchange interactions in GdNi2Mnx (x = 0, 0.4, 0.6) governing the increase in the Curie temperature with manganese concentration were determined. The optical constants of the compounds were measured by the ellipsometric method in the wide spectral range of 0.22-15 μm. The peculiarities of the evolution of the frequency dependences of optical conductivity with a change in the manganese content were revealed. Based on the calculated densities of electron states, the behavior of these dispersion curves in the region of interband absorption of light was discussed. The concentration dependences of several electronic characteristics were determined.

Strong lattice correlation of non-equilibrium quasiparticles in a pseudospin-1/2 Mott insulator Sr 2IrO 4

DOE PAGES

Li, Yuelin; Schaller, Richard D.; Zhu, Mengze; ...

2016-01-20

In correlated oxides the coupling of quasiparticles to other degrees of freedom such as spin and lattice plays critical roles in the emergence of symmetry-breaking quantum ordered states such as high temperature superconductivity. We report a strong lattice coupling of photon-induced quasiparticles in spin-orbital coupling Mott insulator Sr 2IrO 4 probed via optical excitation. Combining time-resolved x-ray diffraction and optical spectroscopy techniques, we reconstruct a spatiotemporal map of the diffusion of these quasiparticles. Lastly, due to the unique electronic configuration of the quasiparticles, the strong lattice correlation is unexpected but extends the similarity between Sr 2IrO 4 and cuprates tomore » a new dimension of electron-phonon coupling which persists under highly non-equilibrium conditions.« less

Spin-polarized structural, elastic, electronic and magnetic properties of half-metallic ferromagnetism in V-doped ZnSe

NASA Astrophysics Data System (ADS)

Monir, M. El Amine.; Baltache, H.; Murtaza, G.; Khenata, R.; Ahmed, Waleed K.; Bouhemadou, A.; Omran, S. Bin; Seddik, T.

2015-01-01

Based on first principles spin-polarized density functional theory, the structural, elastic electronic and magnetic properties of Zn1-xVxSe (for x=0.25, 0.50, 0.75) in zinc blende structure have been studied. The investigation was done using the full-potential augmented plane wave method as implemented in WIEN2k code. The exchange-correlation potential was treated with the generalized gradient approximation PBE-GGA for the structural and elastic properties. Moreover, the PBE-GGA+U approximation (where U is the Hubbard correlation terms) is employed to treat the "d" electrons properly. A comparative study between the band structures, electronic structures, total and partial densities of states and local moments calculated within both GGA and GGA+U schemes is presented. The analysis of spin-polarized band structure and density of states shows the half-metallic ferromagnetic character and are also used to determine s(p)-d exchange constants N0α (conduction band) and N0β (valence band) due to Se(4p)-V(3d) hybridization. It has been clearly evidence that the magnetic moment of V is reduced from its free space change value of 3 μB and the minor atomic magnetic moment on Zn and Se are generated.

Effect of on-site Coulomb interaction on electronic and transport properties of 100% spin polarized CoMnVAs

NASA Astrophysics Data System (ADS)

Bhat, Tahir Mohiuddin; Gupta, Dinesh C.

2017-08-01

The structural, electronic, magnetic and transport properties of a new quaternary Heusler alloy CoMnVAs have been investigated by employing generalized gradient approximation (GGA), modified Becke-Johnson (mBJ) and GGA with Hubbard U correction (GGA + U). The alloy is energetically more stable in ferromagnetic Y1 type structure. Elastic parameters reveal high anisotropy and ductile nature of the material. CoMnVAs shows half-metallic ferromagnet character with 100% spin polarization at Fermi level with band gap of 0.55 eV in the minority spin state. The alloy also possesses high electrical conductivity and Seebeck coefficients with 15 μVK-1 at room temperature, achieving a figure of merit of 0.65 at high temperatures. The high degree of ductility, 100% spin polarization and large Seebeck coefficient, makes it an attractive candidate to be used in spin voltage generators and thermoelectric materials.

Photoinduced reactions of dibenzoyl peroxide as studied by EPR and spin-trapping

NASA Astrophysics Data System (ADS)

Rosenthal, Ionel; Mossoba, Magdi M.; Riesz, Peter

The photochemical reactions of dibenzoyl peroxide with some organic compounds were found by EPR and spin-trapping to generate free radicals in dimethyl sulfoxide solutions at room temperature. Two reaction mechanisms occur which determine the structures of the radicals generated. The first involves a one-electron oxidation and the second a hydrogen atom transfer. The prevailing mechanism is primarily dependent on the structure of the substrate. With carboxylic acids the one-electron oxidation occurs exclusively, leading to the loss of the carboxyl group and to formation of the alkyl radical. For alcohols both alkoxy radicals and hydrogen-abstraction α-carbon radicals were spin trapped. The alkoxy radicals were generated by the electron transfer mechanism. Finally pyrimidine bases such as thymine and cytosine yielded C(5)-centered radicals which could also be explained by an electron transfer mechanism. These observations are of interest because of the recently observed skin tumor-promoting activity of dibenzoyl peroxide.

Electronic Structure of Fullerene Acceptors in Organic Bulk-Heterojunctions. A Combined EPR and DFT Study

DOE PAGES

Mardis, Kristy L.; Webb, J.; Holloway, Tarita; ...

2015-12-03

Organic photovoltaic (OPV) devices are a promising alternative energy source. Attempts to improve their performance have focused on the optimization of electron-donating polymers, while electron-accepting fullerenes have received less attention. Here, we report an electronic structure study of the widely used soluble fullerene derivatives PC61BM and PC71BM in their singly reduced state, that are generated in the polymer:fullerene blends upon light-induced charge separation. Density functional theory (DFT) calculations characterize the electronic structures of the fullerene radical anions through spin density distributions and magnetic resonance parameters. The good agreement of the calculated magnetic resonance parameters with those determined experimentally by advancedmore » electron paramagnetic resonance (EPR) allows the validation of the DFT calculations. Thus, for the first time, the complete set of magnetic resonance parameters including directions of the principal g-tensor axes were determined. For both molecules, no spin density is present on the PCBM side chain, and the axis of the largest g-value lies along the PCBM molecular axis. While the spin density distribution is largely uniform for PC61BM, it is not evenly distributed for PC71BM.« less

Tuning the Magnetic and Electronic Properties of Iron(x )Silicon(1-x) Thin Films for Spintronics

NASA Astrophysics Data System (ADS)

Karel, Julie Elizabeth

This dissertation investigated the magnetic and electronic properties of a potentially better alternative: off-stoichimetry, bcc-like FexSi 1-x thin films (0.43800 K) and theoretically predicted high spin polarization (100%). However, little work has been done on off-stoichiometry FexSi1-x thin films (0.43

Characterization of the Solution Structure of Human Serum Albumin Loaded with a Metal Porphyrin and Fatty Acids

PubMed Central

Junk, Matthias J.N.; Spiess, Hans W.; Hinderberger, Dariush

2011-01-01

The structure of human serum albumin loaded with a metal porphyrin and fatty acids in solution is characterized by orientation-selective double electron-electron resonance (DEER) spectroscopy. Human serum albumin, spin-labeled fatty acids, and Cu(II) protoporphyrin IX—a hemin analog—form a fully self-assembled system that allows obtaining distances and mutual orientations between the paramagnetic guest molecules. We report a simplified analysis for the orientation-selective DEER data which can be applied when the orientation selection of one spin in the spin pair dominates the orientation selection of the other spin. The dipolar spectra reveal a dominant distance of 3.85 nm and a dominant orientation of the spin-spin vectors between Cu(II) protoporphyrin IX and 16-doxyl stearic acid, the electron paramagnetic resonance reporter group of the latter being located near the entry points to the fatty acid binding sites. This observation is in contrast to crystallographic data that suggest an asymmetric distribution of the entry points in the protein and hence the occurrence of various distances. In conjunction with the findings of a recent DEER study, the obtained data are indicative of a symmetric distribution of the binding site entries on the protein's surface. The overall anisotropic shape of the protein is reflected by one spin-spin vector orientation dominating the DEER data. PMID:21539799

Angle-resolved molecular beam scattering of NO at the gas-liquid interface.

PubMed

Zutz, Amelia; Nesbitt, David J

2017-08-07

This study presents first results on angle-resolved, inelastic collision dynamics of thermal and hyperthermal molecular beams of NO at gas-liquid interfaces. Specifically, a collimated incident beam of supersonically cooled NO ( 2 Π 1/2 , J = 0.5) is directed toward a series of low vapor pressure liquid surfaces ([bmim][Tf 2 N], squalane, and PFPE) at θ inc = 45(1)°, with the scattered molecules detected with quantum state resolution over a series of final angles (θ s = -60°, -30°, 0°, 30°, 45°, and 60°) via spatially filtered laser induced fluorescence. At low collision energies [E inc = 2.7(9) kcal/mol], the angle-resolved quantum state distributions reveal (i) cos(θ s ) probabilities for the scattered NO and (ii) electronic/rotational temperatures independent of final angle (θ s ), in support of a simple physical picture of angle independent sticking coefficients and all incident NO thermally accommodating on the surface. However, the observed electronic/rotational temperatures for NO scattering reveal cooling below the surface temperature (T elec < T rot < T S ) for all three liquids, indicating a significant dependence of the sticking coefficient on NO internal quantum state. Angle-resolved scattering at high collision energies [E inc = 20(2) kcal/mol] has also been explored, for which the NO scattering populations reveal angle-dependent dynamical branching between thermal desorption and impulsive scattering (IS) pathways that depend strongly on θ s . Characterization of the data in terms of the final angle, rotational state, spin-orbit electronic state, collision energy, and liquid permit new correlations to be revealed and investigated in detail. For example, the IS rotational distributions reveal an enhanced propensity for higher J/spin-orbit excited states scattered into near specular angles and thus hotter rotational/electronic distributions measured in the forward scattering direction. Even more surprisingly, the average NO scattering angle (⟨θ s ⟩) exhibits a remarkably strong correlation with final angular momentum, N, which implies a linear scaling between net forward scattering propensity and torque delivered to the NO projectile by the gas-liquid interface.

Angle-resolved molecular beam scattering of NO at the gas-liquid interface

NASA Astrophysics Data System (ADS)

Zutz, Amelia; Nesbitt, David J.

2017-08-01

This study presents first results on angle-resolved, inelastic collision dynamics of thermal and hyperthermal molecular beams of NO at gas-liquid interfaces. Specifically, a collimated incident beam of supersonically cooled NO (2 Π 1/2, J = 0.5) is directed toward a series of low vapor pressure liquid surfaces ([bmim][Tf2N], squalane, and PFPE) at θinc = 45(1)°, with the scattered molecules detected with quantum state resolution over a series of final angles (θs = -60°, -30°, 0°, 30°, 45°, and 60°) via spatially filtered laser induced fluorescence. At low collision energies [Einc = 2.7(9) kcal/mol], the angle-resolved quantum state distributions reveal (i) cos(θs) probabilities for the scattered NO and (ii) electronic/rotational temperatures independent of final angle (θs), in support of a simple physical picture of angle independent sticking coefficients and all incident NO thermally accommodating on the surface. However, the observed electronic/rotational temperatures for NO scattering reveal cooling below the surface temperature (Telec < Trot < TS) for all three liquids, indicating a significant dependence of the sticking coefficient on NO internal quantum state. Angle-resolved scattering at high collision energies [Einc = 20(2) kcal/mol] has also been explored, for which the NO scattering populations reveal angle-dependent dynamical branching between thermal desorption and impulsive scattering (IS) pathways that depend strongly on θs. Characterization of the data in terms of the final angle, rotational state, spin-orbit electronic state, collision energy, and liquid permit new correlations to be revealed and investigated in detail. For example, the IS rotational distributions reveal an enhanced propensity for higher J/spin-orbit excited states scattered into near specular angles and thus hotter rotational/electronic distributions measured in the forward scattering direction. Even more surprisingly, the average NO scattering angle (⟨θs⟩) exhibits a remarkably strong correlation with final angular momentum, N, which implies a linear scaling between net forward scattering propensity and torque delivered to the NO projectile by the gas-liquid interface.

Electrical spin injection from an n-type ferromagnetic semiconductor into a III-V device heterostructure

NASA Astrophysics Data System (ADS)

Kioseoglou, George; Hanbicki, Aubrey T.; Sullivan, James M.; van't Erve, Olaf M. J.; Li, Connie H.; Erwin, Steven C.; Mallory, Robert; Yasar, Mesut; Petrou, Athos; Jonker, Berend T.

2004-11-01

The use of carrier spin in semiconductors is a promising route towards new device functionality and performance. Ferromagnetic semiconductors (FMSs) are promising materials in this effort. An n-type FMS that can be epitaxially grown on a common device substrate is especially attractive. Here, we report electrical injection of spin-polarized electrons from an n-type FMS, CdCr2Se4, into an AlGaAs/GaAs-based light-emitting diode structure. An analysis of the electroluminescence polarization based on quantum selection rules provides a direct measure of the sign and magnitude of the injected electron spin polarization. The sign reflects minority rather than majority spin injection, consistent with our density-functional-theory calculations of the CdCr2Se4 conduction-band edge. This approach confirms the exchange-split band structure and spin-polarized carrier population of an FMS, and demonstrates a litmus test for these FMS hallmarks that discriminates against spurious contributions from magnetic precipitates.

Electronic Transitions of Tungsten Monosulfide

NASA Astrophysics Data System (ADS)

Tsang, L. F.; Chan, Man-Chor; Zou, Wenli; Cheung, Allan S. C.

2017-06-01

Electronic transition spectrum of the tungsten monosulfide (WS) molecule in the near infrared region between 725 nm and 885 nm has been recorded using laser ablation/reaction free-jet expansion and laser induced fluorescence spectroscopy. The WS molecule was produced by reacting laser - ablated tungsten atoms with 1% CS_{2} seeded in argon. Fifteen vibrational bands with resolved rotational structure have been recorded and analyzed, which were organized into seven electronic transition systems. The ground state has been identified to be the X^{3}Σ^{-}(0^{+}) state, and the determined vibrational frequency, ΔG_{1/2} and bond length, r_{0}, are respectively 556.7 cm^{-1} and 2.0676 Å. In addition, vibrational bands belong to another transition system involving lower state with Ω = 1 component have also been analyzed. Least-squares fit of the measured line positions yielded molecular constants for the electronic states involved. The low-lying Λ-S states and Ω sub-states of WS have been calculated using state-averaged complete active space self-consistent field (SA-CASSCF) and followed by MRCISD+Q (internally contracted multi-reference configuration interaction with singles and doubles plus Davidson's cluster correction). The active space consists of 10 electrons in 9 orbitals corresponding to the W 5d6s and S 3p shells. The lower molecular orbitals from W 5s5p and S 3s are inactive but are also correlated, and relativistic effective core potential (RECPs) are adopted to replace the core orbitals with 60 (W) and 10 (S) core electrons, respectively. Spin-orbit coupling (SOC) is calculated via the state-interaction (SI) approach with RECP spin-orbit operators using SA-CASSCF wavefunctions, where the diagonal elements in the SOC matrix are replaced by the corresponding MRCISD+Q energies calculated above. Spectroscopic constants and potential energy curves of the ground and many low-lying Λ-S states and Ω sub-states of the WS molecule are obtained. The calculated spectroscopic constants of the ground and low-lying states are generally in good agreement with our experimental determination. This work represents the first experimental investigation of the electronic and molecular structure of the WS molecule.

Electronic structure and O vacancy formation/migration in La0.825(Mg/Ca/Ba)0.125CoO3

NASA Astrophysics Data System (ADS)

Omotayo Akande, Salawu; Gan, Li-Yong; Schwingenschlögl, Udo

2016-04-01

The effect of A-site hole doping (Mg2+, Ca2+ or Ba2+) on the electronic and magnetic properties as well as the O vacancy formation and migration in perovskite LaCoO3 is studied using first-principles calculations. All three dopants are found to facilitate O vacancy formation. Substitution of La3+ with Ba2+/Mg2+ yields the lowest O vacancy formation energy for low/intermediate spin Co, implying that not only the structure but also the spin state of Co is a key parameter. Only for low spin Co the ionic radius is correlated with the O migration barrier. Enhanced migration for intermediate spin Co is ascribed to the availability of additional space at the transition state.

Correlation, temperature and disorder: Recent developments in the one-step description of angle-resolved photoemission

NASA Astrophysics Data System (ADS)

Braun, Jürgen; Minár, Ján; Ebert, Hubert

2018-04-01

Various apparative developments extended the potential of angle-resolved photoemission spectroscopy tremendously during the last two decades. Modern experimental arrangements consisting of new photon sources, analyzers and detectors supply not only extremely high angle and energy resolution but also spin resolution. This provides an adequate platform to study in detail new materials like low-dimensional magnetic structures, Rashba systems, topological insulator materials or high TC superconductors. The interest in such systems has grown enormously not only because of their technological relevance but even more because of exciting new physics. Furthermore, the use of photon energies from few eV up to several keV makes this experimental technique a rather unique tool to investigate the electronic properties of solids and surfaces. The following article reviews the corresponding recent theoretical developments in the field of angle-resolved photoemission with a special emphasis on correlation effects, temperature and relativistic aspects. The most successful theoretical approach to deal with angle-resolved photoemission is the so-called spectral function or one-step formulation of the photoemission process. Nowadays, the one-step model allows for photocurrent calculations for photon energies ranging from a few eV to more than 10 keV, to deal with arbitrarily ordered and disordered systems, to account for finite temperatures, and considering in addition strong correlation effects within the dynamical mean-field theory or similar advanced approaches.

Synthesis and electronic structure determination of N-alkyl-substituted bis(imino)pyridine iron imides exhibiting spin crossover behavior.

PubMed

Bowman, Amanda C; Milsmann, Carsten; Bill, Eckhard; Turner, Zoë R; Lobkovsky, Emil; DeBeer, Serena; Wieghardt, Karl; Chirik, Paul J

2011-11-02

Three new N-alkyl substituted bis(imino)pyridine iron imide complexes, ((iPr)PDI)FeNR ((iPr)PDI = 2,6-(2,6-(i)Pr(2)-C(6)H(3)-N═CMe)(2)C(5)H(3)N; R = 1-adamantyl ((1)Ad), cyclooctyl ((Cy)Oct), and 2-adamantyl ((2)Ad)) were synthesized by addition of the appropriate alkyl azide to the iron bis(dinitrogen) complex, ((iPr)PDI)Fe(N(2))(2). SQUID magnetic measurements on the isomeric iron imides, ((iPr)PDI)FeN(1)Ad and ((iPr)PDI)FeN(2)Ad, established spin crossover behavior with the latter example having a more complete spin transition in the experimentally accessible temperature range. X-ray diffraction on all three alkyl-substituted bis(imino)pyridine iron imides established essentially planar compounds with relatively short Fe-N(imide) bond lengths and two-electron reduction of the redox-active bis(imino)pyridine chelate. Zero- and applied-field Mössbauer spectroscopic measurements indicate diamagnetic ground states at cryogenic temperatures and established low isomer shifts consistent with highly covalent molecules. For ((iPr)PDI)FeN(2)Ad, Mössbauer spectroscopy also supports spin crossover behavior and allowed extraction of thermodynamic parameters for the S = 0 to S = 1 transition. X-ray absorption spectroscopy and computational studies were also performed to explore the electronic structure of the bis(imino)pyridine alkyl-substituted imides. An electronic structure description with a low spin ferric center (S = 1/2) antiferromagnetically coupled to an imidyl radical (S(imide) = 1/2) and a closed-shell, dianionic bis(imino)pyridine chelate (S(PDI) = 0) is favored for the S = 0 state. An iron-centered spin transition to an intermediate spin ferric ion (S(Fe) = 3/2) accounts for the S = 1 state observed at higher temperatures. Other possibilities based on the computational and experimental data are also evaluated and compared to the electronic structure of the bis(imino)pyridine iron N-aryl imide counterparts.

Excitations in a spin-polarized two-dimensional electron gas

NASA Astrophysics Data System (ADS)

Kreil, Dominik; Hobbiger, Raphael; Drachta, Jürgen T.; Böhm, Helga M.

2015-11-01

A remarkably long-lived spin plasmon may exist in two-dimensional electron liquids with imbalanced spin-up and spin-down population. The predictions for this interesting mode by Agarwal et al. [Phys. Rev. B 90, 155409 (2014), 10.1103/PhysRevB.90.155409] are based on the random phase approximation. Here, we show how to account for spin-dependent correlations from known ground-state pair correlation functions and study the consequences on the various spin-dependent longitudinal response functions. The spin-plasmon dispersion relation and its critical wave vector for Landau damping by minority spins turn out to be significantly lower. We further demonstrate that spin-dependent effective interactions imply a rich structure in the excitation spectrum of the partially spin-polarized system. Most notably, we find a "magnetic antiresonance," where the imaginary part of both, the spin-spin as well as the density-spin response function vanish. The resulting minimum in the double-differential cross section is awaiting experimental confirmation.

ESR Experiments on a Single Donor Electron in Isotopically Enriched Silicon

NASA Astrophysics Data System (ADS)

Tracy, Lisa; Luhman, Dwight; Carr, Stephen; Borchardt, John; Bishop, Nathaniel; Ten Eyck, Gregory; Pluym, Tammy; Wendt, Joel; Witzel, Wayne; Blume-Kohout, Robin; Nielsen, Erik; Lilly, Michael; Carroll, Malcolm

In this talk we will discuss electron spin resonance experiments in single donor silicon qubit devices fabricated at Sandia National Labs. A self-aligned device structure consisting of a polysilicon gate SET located adjacent to the donor is used for donor electron spin readout. Using a cryogenic HEMT amplifier next to the silicon device, we demonstrate spin readout at 100 kHz bandwidth and Rabi oscillations with 0.96 visibility. Electron spin resonance measurements on these devices show a linewidth of 30 kHz and coherence times T2* = 10 us and T2 = 0.3 ms. We also discuss estimates of the fidelity of our donor electron spin qubit measurements using gate set tomography. This work was performed, in part, at the Center for Integrated Nanotechnologies, a U.S. DOE Office of Basic Energy Sciences user facility. Sandia National Laboratories is a multi-program laboratory operated by Sandia Corporation, a Lockheed-Martin Company, for the U. S. Department of Energy under Contract No. DE-AC04-94AL85000. ESR Experiments on a Single Donor Electron in Isotopically Enriched Silicon.

Mechanism of the high transition temperature for the 1111-type iron-based superconductors R FeAsO (R =rare earth ): Synergistic effects of local structures and 4 f electrons

NASA Astrophysics Data System (ADS)

Zhang, Lifang; Meng, Junling; Liu, Xiaojuan; Yao, Fen; Meng, Jian; Zhang, Hongjie

2017-07-01

Among the iron-based superconductors, the 1111-type Fe-As-based superconductors REFeAs O1 -xFx (RE = rare earth) exhibit high transition temperatures (Tc) above 40 K. We perform first-principles calculations based on density functional theory with the consideration of both electronic correlations and spin-orbit couplings on rare earths and Fe ions to study the underlying mechanism as the microscopic structural distortions in REFeAsO tuned by both lanthanide contraction and external strain. The electronic structures evolve similarly in both cases. It is found that there exist an optimal structural regime that will not only initialize but also optimize the orbital fluctuations due to the competing Fe-As and Fe-Fe crystal fields. We also find that the key structural features in REFeAsO, such as As-Fe-As bond angle, intrinsically induce the modification of the Fermi surface and dynamic spin fluctuation. These results suggest that the superconductivity is mediated by antiferromagnetic spin fluctuations. Simultaneously, we show that the rare-earth 4 f electrons play important roles on the high transition temperature whose behavior might be analogous to that of the heavy-fermion superconductors. The superconductivity of these 1111-type iron-based superconductors with high-Tc is considered to originate from the synergistic effects of local structures and 4 f electrons.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Li, Lu

The objective of this research is to investigate the high-field magnetic properties of high temperature superconductors, materials that conduct electricity without loss. A technique known as high-resolution torque magnetometry that was developed to directly measure the magnetization of high temperature superconductors. This technique was implemented using the 65 Tesla pulsed magnetic field facility that is part of the National High Magnetic Field Laboratory at Los Alamos National Laboratory. This research addressed unanswered questions about the interplay between magnetism and superconductivity, determine the electronic structure of high temperature superconductors, and shed light on the mechanism of high temperature superconductivity and onmore » potential applications of these materials in areas such as energy generation and power transmission. Further applications of the technology resolve the novel physical phenomena such as correlated topological insulators, and spin liquid state in quantum magnets.« less

Spin-orbit coupling effects in indium antimonide quantum well structures

NASA Astrophysics Data System (ADS)

Dedigama, Aruna Ruwan

Indium antimonide (InSb) is a narrow band gap material which has the smallest electron effective mass (0.014m0) and the largest electron Lande g-facture (-51) of all the III-V semiconductors. Spin-orbit effects of III-V semiconductor heterostructures arise from two different inversion asymmetries namely bulk inversion asymmetry (BIA) and structural inversion asymmetry (SIA). BIA is due to the zinc-blende nature of this material which leads to the Dresselhaus spin splitting consisting of both linear and cubic in-plane wave vector terms. As its name implies SIA arises due to the asymmetry of the quantum well structure, this leads to the Rashba spin splitting term which is linear in wave vector. Although InSb has theoretically predicted large Dresselhaus (760 eVA3) and Rashba (523 eA 2) coefficients there has been relatively little experimental investigation of spin-orbit coefficients. Spin-orbit coefficients can be extracted from the beating patterns of Shubnikov--de Haas oscillations (SdH), for material like InSb it is hard to use this method due to the existence of large electron Lande g-facture. Therefore it is essential to use a low field magnetotransport technique such as weak antilocalization to extract spin-orbit parameters for InSb. The main focus of this thesis is to experimentally determine the spin-orbit parameters for both symmetrically and asymmetrically doped InSb/InxAl 1-xSb heterostructures. During this study attempts have been made to tune the Rashba spin-orbit coupling coefficient by using a back gate to change the carrier density of the samples. Dominant phase breaking mechanisms for InSb/InxAl1-xSb heterostructures have been identified by analyzing the temperature dependence of the phase breaking field from weak antilocalization measurements. Finally the strong spin-orbit effects on InSb/InxAl1-xSb heterostructures have been demonstrated with ballistic spin focusing devices.

Can Positron 2D-ACAR Resolve the Electronic Structure of HIGH-Tc Superconductors?

NASA Astrophysics Data System (ADS)

Chan, L. P.; Lynn, K. G.; Harshman, D. R.

We examine the ability of the positron Two-Dimensional Angular Correlation Annihilation Radiation (2D-ACAR) technique to resolve the electronic structures of high-Tc cuprate superconductors. Following a short description of the technique, discussions of the theoretical assumptions, data analysis and experimental considerations, in relation to the high-Tc superconductors, are given. We briefly review recent 2D-ACAR experiments on YBa2Cu3O7-x, Bi2Sr2CaCuO8+δ and La2-xSrxCuO4. The 2D-ACAR technique is useful in resolving the band crossings associated with the layers of the superconductors that are preferentially sampled by the positrons. Together with other Fermi surface measurements (namely angle-resolved photoemission), 2D-ACAR can resolve some of the electronic structures of high-Tc cuprate superconductors. In addition, 2D-ACAR measurements of YBa2Cu3O7-x and Bi2Sr2CaCuO8+δ also reveal an interesting temperature dependence in the fine structures, and a change in the positron lifetime in the former.

Alternative difference analysis scheme combining R -space EXAFS fit with global optimization XANES fit for X-ray transient absorption spectroscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhan, Fei; Tao, Ye; Zhao, Haifeng

Time-resolved X-ray absorption spectroscopy (TR-XAS), based on the laser-pump/X-ray-probe method, is powerful in capturing the change of the geometrical and electronic structure of the absorbing atom upon excitation. TR-XAS data analysis is generally performed on the laser-on minus laser-off difference spectrum. Here, a new analysis scheme is presented for the TR-XAS difference fitting in both the extended X-ray absorption fine-structure (EXAFS) and the X-ray absorption near-edge structure (XANES) regions.R-space EXAFS difference fitting could quickly provide the main quantitative structure change of the first shell. The XANES fitting part introduces a global non-derivative optimization algorithm and optimizes the local structure changemore » in a flexible way where both the core XAS calculation package and the search method in the fitting shell are changeable. The scheme was applied to the TR-XAS difference analysis of Fe(phen) 3spin crossover complex and yielded reliable distance change and excitation population.« less

Alternative difference analysis scheme combining R-space EXAFS fit with global optimization XANES fit for X-ray transient absorption spectroscopy.

PubMed

Zhan, Fei; Tao, Ye; Zhao, Haifeng

2017-07-01

Time-resolved X-ray absorption spectroscopy (TR-XAS), based on the laser-pump/X-ray-probe method, is powerful in capturing the change of the geometrical and electronic structure of the absorbing atom upon excitation. TR-XAS data analysis is generally performed on the laser-on minus laser-off difference spectrum. Here, a new analysis scheme is presented for the TR-XAS difference fitting in both the extended X-ray absorption fine-structure (EXAFS) and the X-ray absorption near-edge structure (XANES) regions. R-space EXAFS difference fitting could quickly provide the main quantitative structure change of the first shell. The XANES fitting part introduces a global non-derivative optimization algorithm and optimizes the local structure change in a flexible way where both the core XAS calculation package and the search method in the fitting shell are changeable. The scheme was applied to the TR-XAS difference analysis of Fe(phen) 3 spin crossover complex and yielded reliable distance change and excitation population.

Spin polarized electronic states and spin textures at the surface of oxygen-deficient SrTiO3

NASA Astrophysics Data System (ADS)

Jeschke, Harald O.; Altmeyer, Michaela; Rozenberg, Marcelo; Gabay, Marc; Valenti, Roser

We investigate the electronic structure and spin texture at the (001) surface of SrTiO3 in the presence of oxygen vacancies by means of ab initio density functional theory (DFT) calculations of slabs. Relativistic non-magnetic DFT calculations exhibit Rashba-like spin winding with a characteristic energy scale ~ 10 meV. However, when surface magnetism on the Ti ions is included, bands become spin-split with an energy difference ~ 100 meV at the Γ point. This energy scale is comparable to the observations in SARPES experiments performed on the two-dimensional electronic states confined near the (001) surface of SrTiO3. We find the spin polarized state to be the ground state of the system, and while magnetism tends to suppress the effects of the relativistic Rashba interaction, signatures of it are still clearly visible in terms of complex spin textures. We gratefully acknowledge financial support from the Deutsche Forschungsgemeinschaft through grants SFB/TR 49 and FOR 1346.

Teleportation between distant qudits via scattering of mobile qubits

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ciccarello, Francesco; Zarcone, Michelangelo; Bose, Sougato

2010-04-15

We consider a one-dimensional structure where noninteracting spin-s scattering centers, such as quantum impurities or multilevel atoms, are embedded at given positions. We show that the injection into the structure of unpolarized flying qubits, such as electrons or photons, along with path detection suffice to accomplish spin-state teleportation between two centers via a third ancillary one. No action over the internal quantum state of both the spin-s particles and the flying qubits is required. The protocol enables the transfer of quantum information between well-separated static entities in nanostructures by exploiting a very low control mechanism, namely scattering.

Electron spin resonance modes in a strong-leg ladder in the Tomonaga-Luttinger liquid phase

NASA Astrophysics Data System (ADS)

Ozerov, M.; Maksymenko, M.; Wosnitza, J.; Honecker, A.; Landee, C. P.; Turnbull, M. M.; Furuya, S. C.; Giamarchi, T.; Zvyagin, S. A.

2015-12-01

Magnetic excitations in the strong-leg quantum spin ladder compound (C7H10N) 2CuBr4 (known as DIMPY) in the field-induced Tomonaga-Luttinger spin-liquid phase are studied by means of high-field electron spin resonance (ESR) spectroscopy. The presence of a gapped ESR mode with unusual nonlinear frequency-field dependence is revealed experimentally. Using a combination of analytic and exact-diagonalization methods, we compute the dynamical structure factor and identify this mode with longitudinal excitations in the antisymmetric channel. We argue that these excitations constitute a fingerprint of the spin dynamics in a strong-leg spin-1/2 Heisenberg antiferromagnetic ladder and owe their ESR observability to the uniform Dzyaloshinskii-Moriya interaction.

Electrical control of spin dynamics in finite one-dimensional systems

NASA Astrophysics Data System (ADS)

Pertsova, A.; Stamenova, M.; Sanvito, S.

2011-10-01

We investigate the possibility of the electrical control of spin transfer in monoatomic chains incorporating spin impurities. Our theoretical framework is the mixed quantum-classical (Ehrenfest) description of the spin dynamics, in the spirit of the s-d model, where the itinerant electrons are described by a tight-binding model while localized spins are treated classically. Our main focus is on the dynamical exchange interaction between two well-separated spins. This can be quantified by the transfer of excitations in the form of transverse spin oscillations. We systematically study the effect of an electrostatic gate bias Vg on the interconnecting channel and we map out the long-range dynamical spin transfer as a function of Vg. We identify regions of Vg giving rise to significant amplification of the spin transmission at low frequencies and relate this to the electronic structure of the channel.

Spin-dependent electron scattering at graphene edges on Ni(111).

PubMed

Garcia-Lekue, A; Balashov, T; Olle, M; Ceballos, G; Arnau, A; Gambardella, P; Sanchez-Portal, D; Mugarza, A

2014-02-14

We investigate the scattering of surface electrons by the edges of graphene islands grown on Ni(111). By combining local tunneling spectroscopy and ab initio electronic structure calculations we find that the hybridization between graphene and Ni states results in strongly reflecting graphene edges. Quantum interference patterns formed around the islands reveal a spin-dependent scattering of the Shockley bands of Ni, which we attribute to their distinct coupling to bulk states. Moreover, we find a strong dependence of the scattering amplitude on the atomic structure of the edges, depending on the orbital character and energy of the surface states.

Crystal structures of (Mg1-x,Fe(x))SiO3 postperovskite at high pressures.

PubMed

Yamanaka, Takamitsu; Hirose, Kei; Mao, Wendy L; Meng, Yue; Ganesh, P; Shulenburger, Luke; Shen, Guoyin; Hemley, Russell J

2012-01-24

X-ray diffraction experiments on postperovskite (ppv) with compositions (Mg(0.9)Fe(0.1))SiO(3) and (Mg(0.6)Fe(0.4))SiO(3) at Earth core-mantle boundary pressures reveal different crystal structures. The former adopts the CaIrO(3)-type structure with space group Cmcm, whereas the latter crystallizes in a structure with the Pmcm (Pmma) space group. The latter has a significantly higher density (ρ = 6.119(1) g/cm(3)) than the former (ρ = 5.694(8) g/cm(3)) due to both the larger amount of iron and the smaller ionic radius of Fe(2+) as a result of an electronic spin transition observed by X-ray emission spectroscopy (XES). The smaller ionic radius for low-spin compared to high-spin Fe(2+) also leads to an ordered cation distribution in the M1 and M2 crystallographic sites of the higher density ppv structure. Rietveld structure refinement indicates that approximately 70% of the total Fe(2+) in that phase occupies the M2 site. XES results indicate a loss of 70% of the unpaired electronic spins consistent with a low spin M2 site and high spin M1 site. First-principles calculations of the magnetic ordering confirm that Pmcm with a two-site model is energetically more favorable at high pressure, and predict that the ordered structure is anisotropic in its electrical and elastic properties. These results suggest that interpretations of seismic structure in the deep mantle need to treat a broader range of mineral structures than previously considered.

Hybrid spin and valley quantum computing with singlet-triplet qubits.

PubMed

Rohling, Niklas; Russ, Maximilian; Burkard, Guido

2014-10-24

The valley degree of freedom in the electronic band structure of silicon, graphene, and other materials is often considered to be an obstacle for quantum computing (QC) based on electron spins in quantum dots. Here we show that control over the valley state opens new possibilities for quantum information processing. Combining qubits encoded in the singlet-triplet subspace of spin and valley states allows for universal QC using a universal two-qubit gate directly provided by the exchange interaction. We show how spin and valley qubits can be separated in order to allow for single-qubit rotations.

Electronic properties of one-dimensional nanostructures of the Bi2Se3 topological insulator

NASA Astrophysics Data System (ADS)

Virk, Naunidh; Autès, Gabriel; Yazyev, Oleg V.

2018-04-01

We theoretically study the electronic structure and spin properties of one-dimensional nanostructures of the prototypical bulk topological insulator Bi2Se3 . Realistic models of experimentally observed Bi2Se3 nanowires and nanoribbons are considered using the tight-binding method. At low energies, the band structures are composed of a series of evenly spaced degenerate subbands resulting from circumferential confinement of the topological surface states. The direct band gaps due to the nontrivial π Berry phase show a clear dependence on the circumference. The spin-momentum locking of the topological surface states results in a pronounced 2 π spin rotation around the circumference with the degree of spin polarization dependent on the momentum along the nanostructure. Overall, the band structures and spin textures are more complicated for nanoribbons, which expose two distinct facets. The effects of reduced dimensionality are rationalized with the help of a simple model that considers circumferential quantization of the topological surface states. Furthermore, the surface spin density induced by an electric current along the nanostructure shows a pronounced oscillatory dependence on the charge-carrier energy, which can be exploited in spintronics applications.

Spin structure in high energy processes: Proceedings

DOE Office of Scientific and Technical Information (OSTI.GOV)

DePorcel, L.; Dunwoodie, C.

1994-12-01

This report contains papers as the following topics: Spin, Mass, and Symmetry; physics with polarized Z{sup 0}s; spin and precision electroweak physics; polarized electron sources; polarization phenomena in quantum chromodynamics; polarized lepton-nucleon scattering; polarized targets in high energy physics; spin dynamics in storage rings and linear accelerators; spin formalism and applications to new physics searches; precision electroweak physics at LEP; recent results on heavy flavor physics from LEP experiments using 1990--1992 data; precise measurement of the left-right cross section asymmetry in Z boson production by electron-positron collisions; preliminary results on heavy flavor physics at SLD; QCD tests with SLD andmore » polarized beams; recent results from TRISTAN at KEK; recent B physics results from CLEO; searching for the H dibaryon at Brookhaven; recent results from the compton observatory; the spin structure of the deuteron; spin structure of the neutron ({sup 3}HE) and the Bjoerken sum rule; a consumer`s guide to lattice QCD results; top ten models constrained by b {yields} sy; a review of the Fermilab fixed target program; results from the D0 experiment; results from CDF at FNAL; quantum-mechanical suppression of bremsstrahlung; report from the ZEUS collaboration at HERA; physics from the first year of H1 at HERA, and hard diffraction. These papers have been cataloged separately elsewhere.« less

Structure and dynamics in B12 enzyme catalysis revealed by electron paramagnetic resonance spectroscopy

NASA Astrophysics Data System (ADS)

Warncke, Kurt

2009-03-01

Challenges to the understanding of how protein structure and dynamics contribute to catalysis in enzymes, and the use of time-resolved electron paramagnetic resonance (EPR) spectroscopic techniques to address the challenges, are examined in the context of the coenzyme B12-dependent enzyme, ethanolamine ammonia-lyase (EAL), from Salmonella typhimurium. EAL conducts the homolytic cleavage of the coenzyme cobalt-carbon bond, intraprotein radical migration (5-6 å), and hydrogen atom transfers, which enable the core radical-mediated rearrangement reaction. Thermodynamic and activation parameters are measured in two experimental systems, which were developed to isolate sub-sequences from the multi-step catalytic cycle, as follows: (1) A dimethylsulfoxide (DMSO)/water cryosolvent system is used to prepare the kinetically-arrested enzyme/coenzyme/substrate ternary complex in fluid solution at 230 K.[1] Temperature-step initiated cobalt-carbon bond cleavage and radical pair separation to form the Co(II)-substrate radical pair are monitored by using time-resolved, full-spectrum EPR spectroscopy (234<=T<=250 K).[1] (2) The Co(II)-substrate radical pair is cryotrapped in frozen aqueous solution at T<150 K, and then promoted to react by a temperature step. The reaction of the substrate radical along the native pathway to form the diamagnetic bound products is monitored by using time-resolved, full-spectrum EPR spectroscopy (187<=T<=217 K).[2] High temporal resolution is achieved, because the reactions are dramatically slowed at the low temperatures, relative to the initiation and spectrum acquistion times. The results are combined with high resolution structures of the reactant centers, obtained by pulsed-EPR spectroscopies,[3] and the protein, obtained by structural proteomics[4] and EPR and electron spin echo envelope modulation (ESEEM) in combination with site directed mutagenesis,[5] to approach a molecular level description of protein contributions to catalysis in EAL. [4pt] [1] Wang, M. & Warncke, K. J. Am. Chem. Soc. 2008, 130, 4846. [0pt] [2] Chen, Z. and Warncke, K. Biophys. J. 2008, 95 (December) [0pt] [3] Canfield, J. M. and Warncke, K. J. Phys. Chem. B 2002, 106, 8831. [0pt] [4] Sun, L. and Warncke, K. Proteins 2006, 64, 308. [0pt] [5] Sun, L., Groover, O., Canfield, J. M., and Warncke, K. Biochemistry 2008, 47, 5523.

Julius Edgar Lilienfeld Prize Talk: Measuring the Electron Magnetic Moment and the Fine Structure Constant

NASA Astrophysics Data System (ADS)

Gabrielse, Gerald

2011-05-01

The electron magnetic moment in Bohr magnetons has been measured to a precision of 3 parts in 1013. This measurement, with quantum electrodynamics (AED) theory, provides the most precise value of the fine structure constant. This measurement, with a value of the fine structure from other measurements, also tests QED and sets a limit on the internal structure of the electron. A one-electron quantum cyclotron is at the heart of the measurement -- an electron suspended in a magnetic field and cooled enough that its lowest cyclotron and spin quantum states can be deduced with quantum nondemolition (QND) measurements. A cylindrical Penning trap cavity inhibits spontaneous emission and feedback methods make the electron excite and sustain its own motion for detection. A new apparatus is being commissioned in pursuit of more precise measurements. Adapted methods are promising for observing a proton spin flip, which should make it possible to compare the antiproton and proton magnetic moments a million times more accurately than is currently possible.

Angle-resolved photoemission spectroscopy with quantum gas microscopes

NASA Astrophysics Data System (ADS)

Bohrdt, A.; Greif, D.; Demler, E.; Knap, M.; Grusdt, F.

2018-03-01

Quantum gas microscopes are a promising tool to study interacting quantum many-body systems and bridge the gap between theoretical models and real materials. So far, they were limited to measurements of instantaneous correlation functions of the form 〈O ̂(t ) 〉 , even though extensions to frequency-resolved response functions 〈O ̂(t ) O ̂(0 ) 〉 would provide important information about the elementary excitations in a many-body system. For example, single-particle spectral functions, which are usually measured using photoemission experiments in electron systems, contain direct information about fractionalization and the quasiparticle excitation spectrum. Here, we propose a measurement scheme to experimentally access the momentum and energy-resolved spectral function in a quantum gas microscope with currently available techniques. As an example for possible applications, we numerically calculate the spectrum of a single hole excitation in one-dimensional t -J models with isotropic and anisotropic antiferromagnetic couplings. A sharp asymmetry in the distribution of spectral weight appears when a hole is created in an isotropic Heisenberg spin chain. This effect slowly vanishes for anisotropic spin interactions and disappears completely in the case of pure Ising interactions. The asymmetry strongly depends on the total magnetization of the spin chain, which can be tuned in experiments with quantum gas microscopes. An intuitive picture for the observed behavior is provided by a slave-fermion mean-field theory. The key properties of the spectra are visible at currently accessible temperatures.

Magnetic dimers and trimers in the disordered S =3/2 spin system BaTi1/2Mn1/2O3

NASA Astrophysics Data System (ADS)

Garcia, F. A.; Kaneko, U. F.; Granado, E.; Sichelschmidt, J.; Hölzel, M.; Duque, J. G. S.; Nunes, C. A. J.; Amaral, R. P.; Marques-Ferreira, P.; Lora-Serrano, R.

2015-06-01

We report a structural-magnetic investigation by x-ray absorption spectroscopy (XAS), neutron diffraction, dc susceptibility (χdc), and electron spin resonance (ESR) of the 12R-type perovskite BaTi1/2Mn1/2O3 . Our structural analysis by neutron diffraction supports the existence of structural trimers with chemically disordered occupancy of Mn4+ and Ti4+ ions, with the valence of the Mn ions confirmed by the XAS measurements. The magnetic properties are explored by combining dc-susceptibility and X -band (9.4 GHz) electron spin resonance, both in the temperature interval of 2 ≤T ≤1000 K. A scenario is presented under which the magnetism is explained by considering magnetic dimers and trimers, with exchange constants Ja/kB=200 (2 ) K and Jb/kB=130 (10 ) K, and orphan spins. Thus, BaTi1/2Mn1/2O3 is proposed as a rare case of an intrinsically disordered S =3/2 spin gap system with a frustrated ground state.

Tunability of the topological nodal-line semimetal phase in ZrSi X -type materials ( X = S ,   Se ,   Te )

DOE PAGES

Hosen, M. Mofazzel; Dimitri, Klauss; Belopolski, Ilya; ...

2017-04-03

The discovery of a topological nodal-line (TNL) semimetal phase in ZrSiS has invigorated the study of other members of this family. In this paper, we present a comparative electronic structure study ofmore » $$\\mathrm{ZrSi}X$$ (where $$X=\\text{S}$$, Se, Te) using angle-resolved photoemission spectroscopy (ARPES) and first-principles calculations. Our ARPES studies show that the overall electronic structure of $$\\mathrm{ZrSi}X$$ materials comprises the diamond-shaped Fermi pocket, the nearly elliptical-shaped Fermi pocket, and a small electron pocket encircling the zone center ($$\\mathrm{{\\Gamma}}$$) point, the $M$ point, and the $X$ point of the Brillouin zone, respectively. We also observe a small Fermi surface pocket along the $$M{-}\\mathrm{{\\Gamma}}{-}M$$ direction in ZrSiTe, which is absent in both ZrSiS and ZrSiSe. Furthermore, our theoretical studies show a transition from nodal-line to nodeless gapped phase by tuning the chalcogenide from S to Te in these material systems. Finally, our findings provide direct evidence for the tunability of the TNL phase in $$\\mathrm{ZrSi}X$$ material systems by adjusting the spin-orbit coupling strength via the $X$ anion.« less

Electronic and structural aspects of spin transitions observed by optical microscopy. The case of [Fe(ptz)6](BF4)2.

PubMed

Chong, Christian; Mishra, Haritosh; Boukheddaden, Kamel; Denise, Stéphane; Bouchez, Guillaume; Collet, Eric; Ameline, Jean-Claude; Naik, Anil D; Garcia, Yann; Varret, François

2010-02-11

The colorimetric analysis of images recorded with an optical microscope during the onset of the spin crossover transformation allows monitoring separately the involved electronic and structural aspects, through the separation of resonant absorption and scattering effects. Complementary information can also be obtained by using the polarized modes of the microscope. These potentialities are illustrated by the observation of [Fe(ptz)(6)](BF(4))(2) single crystals during the onset of the thermal transitions in the 110-140 K range. We characterized the interplay between the electronic (HS <--> LS) and structural (order <--> disorder) transformations. Elastic stresses and mechanical effects (hopping, self-cleavage) generated by the volume change upon electronic transition are also illustrated, with their impact on the photoswitching properties of the crystals.

Dependence of spin pumping and spin transfer torque upon Ni 81 Fe 19 thickness in Ta / Ag / Ni 81 Fe 19 / Ag / Co 2 MnGe / Ag / Ta spin-valve structures

DOE PAGES

Durrant, C. J.; Shelford, L. R.; Valkass, R. A. J.; ...

2017-10-18

Spin pumping has been studied within Ta / Ag / Ni 81Fe 19 (0–5 nm) / Ag (6 nm) / Co 2MnGe (5 nm) / Ag / Ta large-area spin-valve structures, and the transverse spin current absorption of Ni 81Fe 19 sink layers of different thicknesses has been explored. In some circumstances, the spin current absorption can be inferred from the modification of the Co 2MnGe source layer damping in vector network analyzer ferromagnetic resonance (VNA-FMR) experiments. However, the spin current absorption is more accurately determined from element-specific phase-resolved x-ray ferromagnetic resonance (XFMR) measurements that directly probe the spin transfermore » torque (STT) acting on the sink layer at the source layer resonance. Comparison with a macrospin model allows the real part of the effective spin mixing conductance to be extracted. We find that spin current absorption in the outer Ta layers has a significant impact, while sink layers with thicknesses of less than 0.6 nm are found to be discontinuous and superparamagnetic at room temperature, and lead to a noticeable increase of the source layer damping. For the thickest 5-nm sink layer, increased spin current absorption is found to coincide with a reduction of the zero frequency FMR linewidth that we attribute to improved interface quality. Furthermore, this study shows that the transverse spin current absorption does not follow a universal dependence upon sink layer thickness but instead the structural quality of the sink layer plays a crucial role.« less

Dependence of spin pumping and spin transfer torque upon Ni 81 Fe 19 thickness in Ta / Ag / Ni 81 Fe 19 / Ag / Co 2 MnGe / Ag / Ta spin-valve structures

DOE Office of Scientific and Technical Information (OSTI.GOV)

Durrant, C. J.; Shelford, L. R.; Valkass, R. A. J.

Spin pumping has been studied within Ta / Ag / Ni 81Fe 19 (0–5 nm) / Ag (6 nm) / Co 2MnGe (5 nm) / Ag / Ta large-area spin-valve structures, and the transverse spin current absorption of Ni 81Fe 19 sink layers of different thicknesses has been explored. In some circumstances, the spin current absorption can be inferred from the modification of the Co 2MnGe source layer damping in vector network analyzer ferromagnetic resonance (VNA-FMR) experiments. However, the spin current absorption is more accurately determined from element-specific phase-resolved x-ray ferromagnetic resonance (XFMR) measurements that directly probe the spin transfermore » torque (STT) acting on the sink layer at the source layer resonance. Comparison with a macrospin model allows the real part of the effective spin mixing conductance to be extracted. We find that spin current absorption in the outer Ta layers has a significant impact, while sink layers with thicknesses of less than 0.6 nm are found to be discontinuous and superparamagnetic at room temperature, and lead to a noticeable increase of the source layer damping. For the thickest 5-nm sink layer, increased spin current absorption is found to coincide with a reduction of the zero frequency FMR linewidth that we attribute to improved interface quality. Furthermore, this study shows that the transverse spin current absorption does not follow a universal dependence upon sink layer thickness but instead the structural quality of the sink layer plays a crucial role.« less