Efficient simulations with electronic open boundaries

We present a reformulation of the hairy-probe method for introducing electronic open boundaries that is appropriate for steady-state calculations involving nonorthogonal atomic basis sets. As a check on the correctness of the method we investigate a perfect atomic wire of Cu atoms and a perfect nonorthogonal chain of H atoms. For both atom chains we find that the conductance has a value of exactly one quantum unit and that this is rather insensitive to the strength of coupling of the probes to the system, provided values of the coupling are of the same order as the mean interlevel spacing of the system without probes. For the Cu atom chain we find in addition that away from the regions with probes attached, the potential in the wire is uniform, while within them it follows a predicted exponential variation with position. We then apply the method to an initial investigation of the suitability of graphene as a contact material for molecular electronics. We perform calculations on a carbon nanoribbon to determine the correct coupling strength of the probes to the graphene and obtain a conductance of about two quantum units corresponding to two bands crossing the Fermi surface. We then compute the current through a benzene molecule attached to two graphene contacts and find only a very weak current because of the disruption of the π conjugation by the covalent bond between the benzene and the graphene. In all cases we find that very strong or weak probe couplings suppress the current.

Multiscale Analysis for Field-Effect Penetration through Two-Dimensional Materials

Gate-tunable two-dimensional (2D) materials-based quantum capacitors (QCs) and van der Waals heterostructures involve tuning transport or optoelectronic characteristics by the field effect. Recent studies have attributed the observed gate-tunable characteristics to the change of the Fermi level in the first 2D layer adjacent to the dielectrics, whereas the penetration of the field effect through the one-molecule-thick material is often ignored or oversimplified. Here, we present a multiscale theoretical approach that combines first-principles electronic structure calculations and the Poisson–Boltzmann equation methods to model penetration of the field effect through graphene in a metal–oxide–graphene–semiconductor (MOGS) QC, including quantifying the degree of “transparency” for graphene two-dimensional electron gas (2DEG) to an electric displacement field. We find that the space charge density in the semiconductor layer can be modulated by gating in a nonlinear manner, forming an accumulation or inversion layer at the semiconductor/graphene interface. The degree of transparency is determined by the combined effect of graphene quantum capacitance and the semiconductor capacitance, which allows us to predict the ranking for a variety of monolayer 2D materials according to their transparency to an electric displacement field as follows: graphene > silicene > germanene > WS2 > WTe2 > WSe2 > MoS2 > phosphorene > MoSe2 > MoTe2, when the majority carrier is electron. Our findings reveal a general picture of operation modes and design rules for the 2D-materials-based QCs.

Dielectric screening in atomically thin boron nitride nanosheets

Two-dimensional (2D) hexagonal boron nitride (BN) nanosheets are excellent dielectric substrate for graphene, molybdenum disulfide, and many other 2D nanomaterial-based electronic and photonic devices. To optimize the performance of these 2D devices, it is essential to understand the dielectric screening properties of BN nanosheets as a function of the thickness. Here, electric force microscopy along with theoretical calculations based on both state-of-the-art first-principles calculations with van der Waals interactions under consideration, and nonlinear Thomas-Fermi theory models are used to investigate the dielectric screening in high-quality BN nanosheets of different thicknesses. It is found that atomically thin BN nanosheets are less effective in electric field screening, but the screening capability of BN shows a relatively weak dependence on the layer thickness.

Manifestation of Colossal Thermoelectric Power by Charge Ordered Small and Intermediate Bandwidth Manganites

Thermoelectric materials are revisited for various applications including power generation. The direct conversion of temperature differences into electric voltage and vice versa is known as thermoelectric effect. Possible applications of thermoelectric materials are in eco-friendly refrigeration, electric power generation from waste heat, infrared sensors, temperature controlled-seats and portable picnic coolers. Thermoelectric materials are also extensively researched upon as an alternative to compression based refrigeration. This utilizes the principle of Peltier cooling. The performance characteristic of a thermoelectric material, termed as figure of merit (ZT) is a function of several transport coefficients such as electrical conductivity (σ), thermal conductivity (κ) and Seebeck coefficient of the material (S). ZT is expressed asκσTZTS2=, where T is the temperature in degree absolute. A large value of Seebeck coefficient, high electrical conductivity and low thermal conductivity are necessary to realize a high performance thermoelectric material. The best known thermoelectric materials are phonon-glass electron – crystal (PGEC) system where the phonons are scattered within the unit cell by the rattling structure and electrons are scattered less as in crystals to obtain a high electrical conductivity. A survey of literature reveals that correlated semiconductors and Kondo insulators containing rare earth or transition metal ions are found to be potential thermoelectric materials. The structural magnetic and charge transport properties in manganese oxides having the general formula of RE1−xAExMnO3 (RE = rare earth, AE= Ca, Sr, Ba) are solely determined by the mixed valence (3+/4+) state of Mn ions. In strongly correlated electron systems, magnetism and charge transport properties are strongly correlated. Within the area of strongly correlated electron systems the study of manganese oxides, widely known as manganites exhibit unique magneto electric transport properties, is an active area of research.Strongly correlated systems like perovskite manganites, characterized by their narrow localized band and hoping conduction, were found to be good candidates for thermoelectric applications. Manganites represent a highly correlated electron system and exhibit a variety of phenomena such as charge, orbital and magnetic ordering, colossal magneto resistance and Jahn-Teller effect. The strong inter-dependence between the magnetic order parameters and the transport coefficients in manganites has generated much research interest in the thermoelectric properties of manganites. Here, large thermal motion or rattling of rare earth atoms with localized magnetic moments is believed to be responsible for low thermal conductivity of these compounds. The 4f levels in these compounds, lying near the Fermi energy, create large density of states at the Fermi level and hence they are likely to exhibit a fairly large value of Seebeck coefficient.

Studio multi-banda dal sub-parsec al kilo-parsec dell'emissione del getto nella radio galassia IC 1531

In questo lavoro di tesi si presenta il primo studio multi-scala e multi-frequenza focalizzato sul getto della radiogalassia IC1531 (z=0.026) con i satelliti Chandra, XMM-Newton e Fermi con l’obiettivo di tracciarne l’emissione alle alte energie; definire i processi radiativi responsabili dell’emissione osservata e stimare i principali parametri fisici del getto; stimare l’energetica del getto alle diverse scale. La sorgente è stata selezionata per la presenza di un getto esteso (≈5’’) osservato in radio e ai raggi X, inoltre, era riportata come possibile controparte della sorgente gamma 3FGLJ0009.6-3211 presente nel terzo catalogo Fermi (3FGL). La presenza di emissione ai raggi γ, confermata dal nostro studio, è importante per la modellizzazione della SED della regione nucleare. L’emissione X del nucleo è dominata da una componente ben riprodotta da una legge di potenza con indice spettrale Γ=2.2. L’analisi dell’emissione in banda gamma ha evidenziato una variabilità su scale di 5 giorni, dalla quale è stato possibile stimare le dimensioni delle regione emittente. Inoltre viene presentato lo studio della distribuzione spettrale dell’energia della regione nucleare di IC 1531 dalla banda radio ai raggi γ. I modelli ci permettono di determinare la natura dell’emissione gamma e stimare la potenza cinetica del getto a scale del su-pc. Gli osservabili sono stati utilizzati per ottenere le stime sui parametri del modello. La modellizzazione così ottenuta ha permesso di stimare i parametri fisici del getto e la potenza trasportata del getto a scale del sub-pc. Le stime a 151MHz suggerisco che il getto abbia basse velocita' (Γ≤7) e angolo di inclinazione rispetto alla linea di vista 10°<ϑ<20°; nel complesso, il trasporto di energia da parte del getto risulta efficiente. L’origine dell’emissione X del getto a grandi scale è consistente con un’emissione di sincrotrone, che conferma la classificazione di IC1531 come sorgente di bassa potenza MAGN.

The Redox Potentials of n-type Colloidal Semiconductor Nanocrystals

Thesis (Ph.D.)--University of Washington, 2016-08

Degenerate mixtures of rubidium and ytterbium for engineering open quantum systems

In the last two decades, experimental progress in controlling cold atoms and ions now allows us to manipulate fragile quantum systems with an unprecedented degree of precision. This has been made possible by the ability to isolate small ensembles of atoms and ions from noisy environments, creating truly closed quantum systems which decouple from dissipative channels. However in recent years, several proposals have considered the possibility of harnessing dissipation in open systems, not only to cool degenerate gases to currently unattainable temperatures, but also to engineer a variety of interesting many-body states. This thesis will describe progress made towards building a degenerate gas apparatus that will soon be capable of realizing these proposals. An ultracold gas of ytterbium atoms, trapped by a species-selective lattice will be immersed into a Bose-Einstein condensate (BEC) of rubidium atoms which will act as a bath. Here we describe the challenges encountered in making a degenerate mixture of rubidium and ytterbium atoms and present two experiments performed on the path to creating a controllable open quantum system. The first experiment will describe the measurement of a tune-out wavelength where the light shift of $\Rb{87}$ vanishes. This wavelength was used to create a species-selective trap for ytterbium atoms. Furthermore, the measurement of this wavelength allowed us to extract the dipole matrix element of the $5s \rightarrow 6p$ transition in $\Rb{87}$ with an extraordinary degree of precision. Our method to extract matrix elements has found use in atomic clocks where precise knowledge of transition strengths is necessary to account for minute blackbody radiation shifts. The second experiment will present the first realization of a degenerate Bose-Fermi mixture of rubidium and ytterbium atoms. Using a three-color optical dipole trap (ODT), we were able to create a highly-tunable, species-selective potential for rubidium and ytterbium atoms which allowed us to use $\Rb{87}$ to sympathetically cool $\Yb{171}$ to degeneracy with minimal loss. This mixture is the first milestone creating the lattice-bath system and will soon be used to implement novel cooling schemes and explore the rich physics of dissipation.

Universality of weakly bound dimers and Efimov trimers close to Li-Cs Feshbach resonances

We study the interspecies scattering properties of ultracold Li-Cs mixtures in their two energetically lowest spin channels in the magnetic field range between 800 and 1000 G. Close to two broad Feshbach resonances (FR) we create weakly bound LiCs dimers by radio-frequency association and measure the dependence of their binding energy on the external magnetic field strength. Based on the binding energies and complementary atom loss spectroscopy of three other Li-Cs s-wave FRs we construct precise molecular singlet and triplet electronic ground state potentials using a coupled-channels calculation. We extract the Li-Cs interspecies scattering length as a function of the external field and obtain almost a ten-fold improvement in the precision of the values for the pole positions and widths of the s-wave FRs as compared to our previous work (Pires et al 2014 Phys. Rev. Lett. 112 250404). We discuss implications on the Efimov scenario and the universal geometric scaling for LiCsCs trimers.

High-temperature superconductivity in the two-dimensional t-J model: Gutzwiller wavefunction solution

A systematic diagrammatic expansion for Gutzwiller wavefunctions (DE-GWFs) proposed very recently is used for the description of the superconducting (SC) ground state in the two-dimensional square-lattice t-J model with the hopping electron amplitudes t (and t') between nearest (and next-nearest) neighbors. For the example of the SC state analysis we provide a detailed comparison of the method's results with those of other approaches. Namely, (i) the truncated DE-GWF method reproduces the variational Monte Carlo (VMC) results and (ii) in the lowest (zeroth) order of the expansion the method can reproduce the analytical results of the standard Gutzwiller approximation (GA), as well as of the recently proposed 'grand-canonical Gutzwiller approximation' (called either GCGA or SGA). We obtain important features of the SC state. First, the SC gap at the Fermi surface resembles a d(x2-y2) wave only for optimally and overdoped systems, being diminished in the antinodal regions for the underdoped case in a qualitative agreement with experiment. Corrections to the gap structure are shown to arise from the longer range of the real-space pairing. Second, the nodal Fermi velocity is almost constant as a function of doping and agrees semi-quantitatively with experimental results. Third, we compare the

Bosonization and entanglement spectrum for one-dimensional polar bosons on disordered lattices

Ultra cold polar bosons in a disordered lattice potential, described by the extended Bose-Hubbard model, display a rich phase diagram. In the case of uniform random disorder one finds two insulating quantum phases-the Mott-insulator and the Haldane insulator-in addition to a superfluid and a Bose glass phase. In the case of a quasiperiodic potential, further phases are found, e.g. the incommensurate density wave, adiabatically connected to the Haldane insulator. For the case of weak random disorder we determine the phase boundaries using a perturbative bosonization approach. We then calculate the entanglement spectrum for both types of disorder, showing that it provides a good indication of the various phases.

Functional surface chemistry of carbon-based nanostructures

The recently discovered abilities to synthesize single-walled carbon nanotubes and prepare single layer graphene have spurred interest in these sp2-bonded carbon nanostructures. In particular, studies of their potential use in electronic devices are many as silicon integrated circuits are encountering processing limitations, quantum effects, and thermal management issues due to rapid device scaling. Nanotube and graphene implementation in devices does come with significant hurdles itself. Among these issues are the ability to dope these materials and understanding what influences defects have on expected properties. Because these nanostructures are entirely all-surface, with every atom exposed to ambient, introduction of defects and doping by chemical means is expected to be an effective route for addressing these issues. Raman spectroscopy has been a proven characterization method for understanding vibrational and even electronic structure of graphene, nanotubes, and graphite, especially when combined with electrical measurements, due to a wealth of information contained in each spectrum. In Chapter 1, a discussion of the electronic structure of graphene is presented. This outlines the foundation for all sp2-bonded carbon electronic properties and is easily extended to carbon nanotubes. Motivation for why these materials are of interest is readily gained. Chapter 2 presents various synthesis/preparation methods for both nanotubes and graphene, discusses fabrication techniques for making devices, and describes characterization methods such as electrical measurements as well as static and time-resolved Raman spectroscopy. Chapter 3 outlines changes in the Raman spectra of individual metallic single-walled carbon nantoubes (SWNTs) upon sidewall covalent bond formation. It is observed that the initial degree of disorder has a strong influence on covalent sidewall functionalization which has implications on developing electronically selective covalent chemistries and assessing their selectivity in separating metallic and semiconducting SWNTs. Chapter 4 describes how optical phonon population extinction lifetime is affected by covalent functionalization and doping and includes discussions on static Raman linewidths. Increasing defect concentration is shown to decrease G-band phonon population lifetime and increase G-band linewidth. Doping only increases G-band linewidth, leaving non-equilibrium population decay rate unaffected. Phonon mediated electron scattering is especially strong in nanotubes making optical phonon decay of interest for device applications. Optical phonon decay also has implications on device thermal management. Chapter 5 treats doping of graphene showing ambient air can lead to inadvertent Fermi level shifts which exemplifies the sensitivity that sp2-bonded carbon nanostructures have to chemical doping through sidewall adsorption. Removal of this doping allows for an investigation of electron-phonon coupling dependence on temperature, also of interest for devices operating above room temperature. Finally, in Chapter 6, utilizing the information obtained in previous chapters, single carbon nanotube diodes are fabricated and characterized. Electrical performance shows these diodes are nearly ideal and photovoltaic response yields 1.4 nA and 205 mV of short circuit current and open circuit voltage from a single nanotube device. A summary and discussion of future directions in Chapter 7 concludes my work.

Equilibration of quantum gases

Finding equilibration times is a major unsolved problem in physics with few analytical results. Here we look at equilibration times for quantum gases of bosons and fermions in the regime of negligibly weak interactions, a setting which not only includes paradigmatic systems such as gases confined to boxes, but also Luttinger liquids and the free superfluid Hubbard model. To do this, we focus on two classes of measurements: (i) coarse-grained observables, such as the number of particles in a region of space, and (ii) few-mode measurements, such as phase correlators.Weshow that, in this setting, equilibration occurs quite generally despite the fact that the particles are not interacting. Furthermore, for coarse-grained measurements the timescale is generally at most polynomial in the number of particles N, which is much faster than previous general upper bounds, which were exponential in N. For local measurements on lattice systems, the timescale is typically linear in the number of lattice sites. In fact, for one-dimensional lattices, the scaling is generally linear in the length of the lattice, which is optimal. Additionally, we look at a few specific examples, one of which consists ofNfermions initially confined on one side of a partition in a box. The partition is removed and the fermions equilibrate extremely quickly in time O(1 N).

Insights into the emission of the blazar 1ES 1011+496 through unprecedented broadband observations during 2011 and 2012

Context. 1ES 1011+496 (z = 0.212) was discovered in very high-energy (VHE, E >100 GeV) γ rays with MAGIC in 2007. The absence of simultaneous data at lower energies led to an incomplete characterization of the broadband spectral energy distribution (SED). Aims. We study the source properties and the emission mechanisms, probing whether a simple one-zone synchrotron self-Compton (SSC) scenario is able to explain the observed broadband spectrum. Methods. We analyzed data in the range from VHE to radio data from 2011 and 2012 collected by MAGIC, Fermi-LAT, Swift, KVA, OVRO, and Metsähovi in addition to optical polarimetry data and radio maps from the Liverpool Telescope and MOJAVE. Results. The VHE spectrum was fit with a simple power law with a photon index of 3.69 ± 0.22 and a flux above 150 GeV of (1.46±0.16)×10^(−11) ph cm^(−2) s^(−1) . The source 1ES 1011+496 was found to be in a generally quiescent state at all observed wavelengths, showing only moderate variability from radio to X-rays. A low degree of polarization of less than 10% was measured in optical, while some bright features polarized up to 60% were observed in the radio jet. A similar trend in the rotation of the electric vector position angle was found in optical and radio. The radio maps indicated a superluminal motion of 1.8 ± 0.4 c, which is the highest speed statistically significant measured so far in a high-frequency-peaked BL Lac. Conclusions. For the first time, the high-energy bump in the broadband SED of 1ES 1011+496 could be fully characterized from 0.1 GeV to 1 TeV, which permitted a more reliable interpretation within the one-zone SSC scenario. The polarimetry data suggest that at least part of the optical emission has its origin in some of the bright radio features, while the low polarization in optical might be due to the contribution of parts of the radio jet with different orientations of the magnetic field with respect to the optical emission.

Investigating the peculiar emission from the new VHE gamma-ray source H1722+119

The MAGIC (Major Atmospheric Gamma-ray Imaging Cherenkov) telescopes observed the BL Lac object H1722+119 (redshift unknown) for six consecutive nights between 2013 May 17 and 22, for a total of 12.5 h. The observations were triggered by high activity in the optical band measured by the KVA (Kungliga Vetenskapsakademien) telescope. The source was for the first time detected in the very high energy (VHE, E > 100 GeV) γ-ray band with a statistical significance of 5.9 σ. The integral flux above 150 GeV is estimated to be (2.0 ± 0.5) per cent of the Crab Nebula flux. We used contemporaneous high energy (HE, 100MeV < E < 100 GeV) γ-ray observations from Fermi-LAT (Large Area Telescope) to estimate the redshift of the source. Within the framework of the current extragalactic background light models, we estimate the redshift to be z = 0.34±0.15. Additionally, we used contemporaneous X-ray to radio data collected by the instruments on board the Swift satellite, the KVA, and the OVRO (Owens Valley Radio Observatory) telescope to study multifrequency characteristics of the source. We found no significant temporal variability of the flux in the HE and VHE bands. The flux in the optical and radio wavebands, on the other hand, did vary with different patterns. The spectral energy distribution (SED) of H1722+119 shows surprising behaviour in the ∼ 3×1014 −1018 Hz frequency range. It can be modelled using an inhomogeneous helical jet synchrotron self-Compton model.