Thermopower in Two-Dimensional Electron Systems

The subject of this thesis is the measurement and interpretation of thermopower in high-mobility two-dimensional electron systems (2DESs). These 2DESs are realized within state-of-the-art GaAs/AlGaAs heterostructures that are cooled to temperatures as low as T = 20 mK. Much of this work takes place within strong magnetic fields where the single-particle density of states quantizes into discrete Landau levels (LLs), a regime best known for the quantum Hall effect (QHE). In addition, we review a novel hot-electron technique for measuring thermopower of 2DESs that dramatically reduces the influence of phonon drag.

Early chapters concentrate on experimental materials and methods. A brief overview of GaAs/AlGaAs heterostructures and device fabrication is followed by details of our cryogenic setup. Next, we provide a primer on thermopower that focuses on 2DESs at low temperatures. We then review our experimental devices, temperature calibration methods, as well as measurement circuits and protocols.

Latter chapters focus on the physics and thermopower results in the QHE regime. After reviewing the basic phenomena associated with the QHE, we discuss thermopower in this regime. Emphasis is given to the relationship between diffusion thermopower and entropy. Experimental results demonstrate this relationship persists well into the fractional quantum Hall (FQH) regime.

Several experimental results are reviewed. Unprecedented observations of the diffusion thermopower of a high-mobility 2DES at temperatures as high as T = 2 K are achieved using our hot-electron technique. The composite fermion (CF) effective mass is extracted from measurements of thermopower at LL filling factor ν = 3/2. The thermopower versus magnetic field in the FQH regime is shown to be qualitatively consistent with a simple entropic model of CFs. The thermopower at ν = 5/2 is shown to be quantitatively consistent with the presence of non-Abelian anyons. An abrupt collapse of thermopower is observed at the onset of the reentrant integer quantum Hall effect (RIQHE). And the thermopower at temperatures just above the RIQHE transition suggests the existence of an unconventional conducting phase.

Part I. Approximate Hartree-Fock wavefunctions one-electron properties and electronic structure of the water molecule. Part II. Perturbation-variational calculation of the nuclear spin-spin isotope coupling constant in HD

Part I

Several approximate Hartree-Fock SCF wavefunctions for the ground electronic state of the water molecule have been obtained using an increasing number of multicenter s, p, and d Slater-type atomic orbitals as basis sets. The predicted charge distribution has been extensively tested at each stage by calculating the electric dipole moment, molecular quadrupole moment, diamagnetic shielding, Hellmann-Feynman forces, and electric field gradients at both the hydrogen and the oxygen nuclei. It was found that a carefully optimized minimal basis set suffices to describe the electronic charge distribution adequately except in the vicinity of the oxygen nucleus. Our calculations indicate, for example, that the correct prediction of the field gradient at this nucleus requires a more flexible linear combination of p-orbitals centered on this nucleus than that in the minimal basis set. Theoretical values for the molecular octopole moment components are also reported.

Part II

The perturbation-variational theory of R. M. Pitzer for nuclear spin-spin coupling constants is applied to the HD molecule. The zero-order molecular orbital is described in terms of a single 1s Slater-type basis function centered on each nucleus. The first-order molecular orbital is expressed in terms of these two functions plus one singular basis function each of the types e^-r/r and e^-r ln r centered on one of the nuclei. The new kinds of molecular integrals were evaluated to high accuracy using numerical and analytical means. The value of the HD spin-spin coupling constant calculated with this near-minimal set of basis functions is J_HD = +96.6 cps. This represents an improvement over the previous calculated value of +120 cps obtained without using the logarithmic basis function but is still considerably off in magnitude compared with the experimental measurement of J_HD = +43 0 ± 0.5 cps.

Determination of electronic energy levels of molecules by 90° low energy electron scattering

A review of the theory of electron scattering indicates that low incident beam energies and large scattering angles are the favorable conditions for the observation of optically forbidden transitions in atoms and molecules.

An apparatus capable of yielding electron impact spectra at 90° with incident electron beam energies between 30 and 50 electron volts is described. The resolution of the instrument is about 1 electron volt.

Impact spectra of thirteen molecules have been obtained. Known forbidden transitions to the helium 2³S, the hydrogen b³Ʃ⁺_u, the nitrogen A³Ʃ⁺_u, B³π_g, a’π_g, and C³π_u, the carbon monoxide a³π, the ethylene ᾶ³B_1u, and the benzene ᾶ³B_1u states from the corresponding ground states have been observed.

In addition, singlet-triplet vertical transitions in acetylene, propyne, propadiene, norbornadiene and quadricyclene, peaking at 5.9, 5.9, 4.5, 3.8, and 4.0 ev (±0.2 ev), respectively, have been observed and assigned for the first time.

I. Proton magnetic resonance of polynucleotides and transfer RNA. II. Electron spin relaxation studies of manganese (II) complexes in acetonitrile

Part I. Proton Magnetic Resonance of Polynucleotides and Transfer RNA.

Proton magnetic resonance was used to follow the temperature dependent intramolecular stacking of the bases in the polynucleotides of adenine and cytosine. Analysis of the results on the basis of a two state stacked-unstacked model yielded values of -4.5 kcal/mole and -9.5 kcal/mole for the enthalpies of stacking in polyadenylic and polycytidylic acid, respectively.

The interaction of purine with these molecules was also studied by pmr. Analysis of these results and the comparison of the thermal unstacking of polynucleotides and short chain nucleotides indicates that the bases contained in stacks within the long chain poly nucleotides are, on the average, closer together than the bases contained in stacks in the short chain nucleotides.

Temperature and purine studies were also carried out with an aqueous solution of formylmethionine transfer ribonucleic acid. Comparison of these results with the results of similar experiments with the homopolynucleotides of adenine, cytosine and uracil indicate that the purine is probably intercalating into loop regions of the molecule.

The solvent denaturation of phenylalanine transfer ribonucleic acid was followed by pmr. In a solvent mixture containing 83 volume per cent dimethylsulf oxide and 17 per cent deuterium oxide, the tRNA molecule is rendered quite flexible. It is possible to resolve resonances of protons on the common bases and on certain modified bases.

Part II. Electron Spin Relaxation Studies of Manganese (II) Complexes in Acetonitrile.

The electron paramagnetic resonance spectra of three Mn⁺² complexes, [Mn(CH₃CN)₆]⁺², [MnCl₄]^-2, and [MnBr₄]^-2, in acetonitrile were studied in detail. The objective of this study was to relate changes in the effective spin Hamiltonian parameters and the resonance line widths to the structure of these molecular complexes as well as to dynamical processes in solution.

Of the three systems studied, the results obtained from the [Mn(CH₃CN)₆]⁺² system were the most straight-forward to interpret. Resonance broadening attributable to manganese spin-spin dipolar interactions was observed as the manganese concentration was increased.

In the [MnCl₄]^-2 system, solvent fluctuations and dynamical ion-pairing appear to be significant in determining electron spin relaxation.

In the [MnBr₄]^-2 system, solvent fluctuations, ion-pairing, and Br- ligand exchange provide the principal means of electron spin relaxation. It was also found that the spin relaxation in this system is dependent upon the field strength and is directly related to the manganese concentration. A relaxation theory based on a two state collisional model was developed to account for the observed behavior.

Digital holographic aberration compensation in electron holography

This paper proposes a new digital method to compensate for the aberration of an electron objective lens in electron holography. In this method, the object wavefront in the exit pupil plane is numerically reconstructed from a digitized electron hologram, and is corrected by multiplying it with the conjugated phase-error function. Then, an aberration-free image can be obtained by calculating the Fresnel integral of this corrected wavefront. In comparison with traditional methods, this method is much more convenient and accurate. Some verifying experiments are also presented in this paper. (C) 2003 Society of Photo-optical Instrumentation Engineers.

Second-harmonic generation in Ge20As25S55 glass irradiated by an electron beam

Second-harmonic generation was observed in Ge(20)AS(25)S(55) chalcogenide glass irradiated by an electron beam. The second-harmonic intensity increased with increasing electron-beam current and accelerating voltage. The second-harmonic generation in Ge20As25S55 glass was caused by the space-charge electrostatic field that was generated by irradiation of an electron beam. Second-order nonlinearity chi ((2)) as great as 0.8 pm/V was obtained. The results of measurements of thermally stimulated depolarization current indicated that the glass was poled in the thin layers of its surface (several micrometers) and that the nonlinearity was stable. (C) 2001 Optical Society of America.

Femtosecond laser pulse irradiation of Sb-rich AgInSbTe films: Scanning electron microscopy and atomic force microscopy investigations

The single-layer and multilayer Sb-rich AgInSbTe films were irradiated by a single femtosecond laser pulse with the duration of 120 fs. The morphological feature resulting from the laser irradiation have been investigated by scanning electron microscopy and atom force microscopy. For the single-layer film, the center of the irradiated spot is a dark depression and the border is a bright protrusion; however, for the multilayer film, the center morphology changes from a depression to a protrusion as the energy increases. The crystallization threshold fluence of the single-layer and the multilayer films is 46.36 mJ/cm(2), 63.74 mJ/cm(2), respectively.

Precipitation of Ge nanoparticles from GeO2 glasses in transmission electron microscope

We show, using spatially resolved energy loss spectroscopy in a transmission electron microscopy (TEM), that GeO2 and GeO2-SiO2 glasses are extremely sensitive to high energy electrons. Ge nanoparticles can be precipitated in GeO2 glasses efficiently by the high-energy electron beam of a TEM. This is relevant to TEM characterization of luminescent Ge nanoparticles in silicate glasses, which may produce artificial results. (C) 2005 American Institute of Physics.