Theory of optical spectra of polar quantum wells: Temperature effects

Theoretical and numerical calculations of the optical absorption spectra of excitons interacting with longitudinal-optical phonons in quasi-2D polar semiconductors are presented. In II-VI semiconductor quantum wells, exciton binding energy can be tuned on- and off-resonance with the longitudinal-optical phonon energy by varying the quantum well width. A comprehensive picture of this tunning effect on the temperature-dependent exciton absorption spectrum is derived, using the exciton Green's function formalism at finite temperature. The effective exciton-phonon interaction is included in the Bethe-Salpeter equation. Numerical results are illustrated for ZnSe-based quantum wells. At low temperatures, both a single exciton peak as well as a continuum resonance state are found in the optical absorption spectra. By contrast, at high enough temperatures, a splitting of the exciton line due to the real phonon absorption processes is predicted. Possible previous experimental observations of this splitting are discussed.Comment: 10 pages, 9 figures, to appear in Phys. Rev. B. Permanent address: [email protected]

Fine structure of excitons in Cu2_2O

Three experimental observations on 1s-excitons in Cu$_2$O are not consistent with the picture of the exciton as a simple hydrogenic bound state: the energies of the 1s-excitons deviate from the Rydberg formula, the total exciton mass exceeds the sum of the electron and hole effective masses, and the triplet-state excitons lie above the singlet. Incorporating the band structure of the material, we calculate the corrections to this simple picture arising from the fact that the exciton Bohr radius is comparable to the lattice constant. By means of a self-consistent variational calculation of the total exciton mass as well as the ground-state energy of the singlet and the triplet-state excitons, we find excellent agreement with experiment.Comment: Revised abstract; 10 pages, revtex, 3 figures available from G. Kavoulakis, Physics Department, University of Illinois, Urban

On the determination of the Fermi surface in high-Tc superconductors by angle-resolved photoemission spectroscopy

We study the normal state electronic excitations probed by angle resolved photoemission spectroscopy (ARPES) in Bi2201 and Bi2212. Our main goal is to establish explicit criteria for determining the Fermi surface from ARPES data on strongly interacting systems where sharply defined quasiparticles do not exist and the dispersion is very weak in parts of the Brillouin zone. Additional complications arise from strong matrix element variations within the zone. We present detailed results as a function of incident photon energy, and show simple experimental tests to distinguish between an intensity drop due to matrix element effects and spectral weight loss due to a Fermi crossing. We reiterate the use of polarization selection rules in disentangling the effect of umklapps due to the BiO superlattice in Bi2212. We conclude that, despite all the complications, the Fermi surface can be determined unambiguously: it is a single large hole barrel centered about (pi,pi) in both materials.Comment: Expanded discussion of symmetrization method in Section 5, figures remain the sam

Ab initio simulation of photoemission spectroscopy in solids: Plane-wave pseudopotential approach, with applications to normal-emission spectra of Cu(001) and Cu(111)

We introduce a new method for simulating photoemission spectra from bulk crystals in the ultra-violet energy range, within a three-step model. Our method explicitly accounts for transmission and matrix-element effects, as calculated from state-of-the-art plane-wave pseudopotential techniques within density-functional theory. Transmission effects, in particular, are included by extending to the present problem a technique previously employed with success to deal with ballistic conductance in metal nanowires. The spectra calculated for normal emission in Cu(001) and Cu(111) are in fair agreement with previous theoretical results and with experiments, including a newly determined spectrum. The residual discrepancies between our results and the latter are mainly due to the well-known deficiencies of density-functional theory in accounting for correlation effects in quasi-particle spectra. A significant improvement is obtained by the LDA+U method. Further improvements are obtained by including surface-optics corrections, as described by Snell's law and Fresnel's equations.Comment: 25 pages, 7 figures, accepted in PR

Pb0.4Bi1.6Sr2Ca1Cu2O8+xPb_{0.4}Bi_{1.6}Sr_{2}Ca_{1}Cu_{2}O_{8+x} and Oxygen Stoichiometry: Structure, Resistivity, Fermi Surface Topology and Normal State Properties

$Pb_{0.4}Bi_{1.6}Sr_2CaCu_2O_{8+x}$ ($Bi(Pb)-$2212) single crystal samples were studied using transmission electron microscopy (TEM), $ab-$plane ($\rho_{ab}$) and $c-$axis ($\rho_c$) resistivity, and high resolution angle-resolved ultraviolet photoemission spectroscopy (ARUPS). TEM reveals that the modulation in the $b-$axis for $Pb(0.4)-$doped $Bi(Pb)-$2212 is dominantly of $Pb-$type that is not sensitive to the oxygen content of the system, and the system clearly shows a structure of orthorhombic symmetry. Oxygen annealed samples exhibit a much lower $c-$axis resistivity and a resistivity minimum at $80-130$K. He-annealed samples exhibit a much higher $c-$axis resistivity and $d\rho_c/dT<0$ behavior below 300K. The Fermi surface (FS) of oxygen annealed $Bi(Pb)-$2212 mapped out by ARUPS has a pocket in the FS around the $\bar{M}$ point and exhibits orthorhombic symmetry. There are flat, parallel sections of the FS, about 60\% of the maximum possible along $k_x = k_y$, and about 30\% along $k_x = - k_y$. The wavevectors connecting the flat sections are about $0.72(\pi, \pi)$ along $k_x = k_y$, and about $0.80(\pi, \pi)$ along $k_x = - k_y$, rather than $(\pi,\pi)$. The symmetry of the near-Fermi-energy dispersing states in the normal state changes between oxygen-annealed and He-annealed samples.Comment: APS_REVTEX 3.0, 49 pages, including 11 figures, available upon request. Submitted to Phys. Rev. B

Controlled assembly of SNAP-PNA-fluorophore systems on DNA templates to produce fluorescence resonance energy transfer

The SNAP protein is a widely used self-labeling tag that can be used for tracking protein localization and trafficking in living systems. A model system providing controlled alignment of SNAP-tag units can provide a new way to study clustering of fusion proteins. In this work, fluorescent SNAP-PNA conjugates were controllably assembled on DNA frameworks forming dimers, trimers, and tetramers. Modification of peptide nucleic acid (PNA) with the O6-benzyl guanine (BG) group allowed the generation of site-selective covalent links between PNA and the SNAP protein. The modified BG-PNAs were labeled with fluorescent Atto dyes and subsequently chemo-selectively conjugated to SNAP protein. Efficient assembly into dimer and oligomer forms was verified via size exclusion chromatography (SEC), electrophoresis (SDS-PAGE), and fluorescence spectroscopy. DNA directed assembly of homo- and hetero-dimers of SNAP-PNA constructs induced homo- and hetero-FRET, respectively. Longer DNA scaffolds controllably aligned similar fluorescent SNAP-PNA constructs into higher oligomers exhibiting homo-FRET. The combined SEC and homo-FRET studies indicated the 1:1 and saturated assemblies of SNAP-PNA-fluorophore:DNA formed preferentially in this system. This suggested a kinetic/stoichiometric model of assembly rather than binomially distributed products. These BG-PNA-fluorophore building blocks allow facile introduction of fluorophores and/or assembly directing moieties onto any protein containing SNAP. Template directed assembly of PNA modified SNAP proteins may be used to investigate clustering behavior both with and without fluorescent labels which may find use in the study of assembly processes in cells

Skillful long-range prediction of European and North American winters

This is the final version. Available from AGU via the DOI in this recordUntil recently, long-range forecast systems showed only modest levels of skill in predicting surface winter climate around the Atlantic Basin and associated fluctuations in the North Atlantic Oscillation at seasonal lead times. Here we use a new forecast system to assess seasonal predictability of winter North Atlantic climate. We demonstrate that key aspects of European and North American winter climate and the surface North Atlantic Oscillation are highly predictable months ahead. We demonstrate high levels of prediction skill in retrospective forecasts of the surface North Atlantic Oscillation, winter storminess, near-surface temperature, and wind speed, all of which have high value for planning and adaptation to extreme winter conditions. Analysis of forecast ensembles suggests that while useful levels of seasonal forecast skill have now been achieved, key sources of predictability are still only partially represented and there is further untapped predictability. Key Points The winter NAO can be skilfully predicted months ahead The signal-to-noise ratio of the predictable signal is anomalously low Predictions of the risk of regional winter extremes are possibleThis work was supported by the Joint DECC/Defra Met Office Hadley Centre Climate Programme (GA01101), the UK Public Weather Service research program, and the European Union Framework 7 SPECS project. Leon Hermanson was funded as part of his Research Fellowship by Willis as part of Willis Research Network (WRN)

Angle resolved photoemission spectroscopy of Sr_2CuO_2Cl_2 - a revisit

We have investigated the lowest binding-energy electronic structure of the model cuprate Sr_2CuO_2Cl_2 using angle resolved photoemission spectroscopy (ARPES). Our data from about 80 cleavages of Sr_2CuO_2Cl_2 single crystals give a comprehensive, self-consistent picture of the nature of the first electron-removal state in this model undoped CuO_2-plane cuprate. Firstly, we show a strong dependence on the polarization of the excitation light which is understandable in the context of the matrix element governing the photoemission process, which gives a state with the symmetry of a Zhang-Rice singlet. Secondly, the strong, oscillatory dependence of the intensity of the Zhang-Rice singlet on the exciting photon-energy is shown to be consistent with interference effects connected with the periodicity of the crystal structure in the crystallographic c-direction. Thirdly, we measured the dispersion of the first electron-removal states along G->(pi,pi) and G->(pi,0), the latter being controversial in the literature, and have shown that the data are best fitted using an extended t-J-model, and extract the relevant model parameters. An analysis of the spectral weight of the first ionization states for different excitation energies within the approach used by Leung et al. (Phys. Rev. B56, 6320 (1997)) results in a strongly photon-energy dependent ratio between the coherent and incoherent spectral weight. The possible reasons for this observation and its physical implications are discussed.Comment: 10 pages, 8 figure

Control of Length and Spatial Functionality of Single-Wall Carbon Nanotube AFM Nanoprobes

Single-wall carbon nanotube (SWNT) nanofibrils were assembled onto conductive atomic force microscopy (AFM) probes with the help of dielectrophoresis (DEP). This process involved the application of a 10 V, 2 MHz, AC bias between a metal-coated AFM probe and a dilute suspension of SWNTs. This exerted a positive dielectrophoretic force onto the nanotubes that caused them to align while precipitating out onto the probe. The gradual removal of the AFM probe away from the SWNT suspension consolidated these nanotubes into nanofibrils with a high degree of alignment as demonstrated with polarization Raman experiments. By varying the pulling speed, immersion time, and concentration of the SWNT suspension, one can tailor the diameter and thus the stiffness of these probes. Precise length trimming of these nanofibrils was also performed by their gradual immersion and dissolution into a liquid that strongly interacted with nanotubes, (i.e., sodium dodecyl sulfate (SDS) solution). Vacuum annealing these nanoprobes at temperature up to 450 degree C further increased their stiffness and rendered them insoluble to SDS and all other aqueous media. Regrowth of a new SWNT nanofibril from the side or at the end of a previously grown SWNT nanofibril was also demonstrated by a repeated dielectrophoretic assembly at the desired immersion depth. These SWNT nanofibril-equipped AFM probes are electrically conductive and mechanically robust for use as high-aspect-ratio electrochemical nanoprobes

ARPES: A probe of electronic correlations

Angle-resolved photoemission spectroscopy (ARPES) is one of the most direct methods of studying the electronic structure of solids. By measuring the kinetic energy and angular distribution of the electrons photoemitted from a sample illuminated with sufficiently high-energy radiation, one can gain information on both the energy and momentum of the electrons propagating inside a material. This is of vital importance in elucidating the connection between electronic, magnetic, and chemical structure of solids, in particular for those complex systems which cannot be appropriately described within the independent-particle picture. Among the various classes of complex systems, of great interest are the transition metal oxides, which have been at the center stage in condensed matter physics for the last four decades. Following a general introduction to the topic, we will lay the theoretical basis needed to understand the pivotal role of ARPES in the study of such systems. After a brief overview on the state-of-the-art capabilities of the technique, we will review some of the most interesting and relevant case studies of the novel physics revealed by ARPES in 3d-, 4d- and 5d-based oxides.Comment: Chapter to appear in "Strongly Correlated Systems: Experimental Techniques", edited by A. Avella and F. Mancini, Springer Series in Solid-State Sciences (2013). A high-resolution version can be found at: http://www.phas.ubc.ca/~quantmat/ARPES/PUBLICATIONS/Reviews/ARPES_Springer.pdf. arXiv admin note: text overlap with arXiv:cond-mat/0307085, arXiv:cond-mat/020850