J. Koltai

Raman spectra of titanium dioxide (anatase, rutile) with identified oxygen isotopes (16, 17, 18)

Six representative isotope-labeled samples of titanium dioxide were synthesized: Ti(16)O(2), Ti(17)O(2) and Ti(18)O(2), each in anatase and rutile forms. Their Raman scattering was analyzed at temperatures down to 5 K. Spectral assignment was supported by numerical simulation using DFT calculations. The combination of experimental and theoretical Raman frequencies with the corresponding isotopic shifts allowed us to address various still-open questions about the second-order Raman scattering in rutile, and the analysis of overlapping features in the anatase spectrum.

Fine tuning the charge transfer in carbon nanotubes via the interconversion of encapsulated molecules

Tweaking the properties of carbon nanotubes is a prerequisite for their practical applications. Here we demonstrate fine-tuning the electronic properties of single-wall carbon nanotubes via filling with ferrocene molecules. The evolution of the bonding and charge transfer within the tube is demonstrated via chemical reaction of the ferrocene filler ending up as secondary inner tube. The charge transfer nature is interpreted well within density functional theory. This work gives the first direct observation of a fine-tuned continuous amphoteric doping of single-wall carbon nanotubes.

Oxygen-isotope labeled titania: Ti18O2

(18)O-isotope labelled titania (anatase, rutile) was synthesized. The products were characterized by Raman spectra together with their quantum chemical modelling. The interaction with carbon dioxide was investigated using high-resolution FTIR spectroscopy, and the oxygen isotope exchange at the Ti(18)O(2)/C(16)O(2) interface was elucidated.

Electron spin resonance signal of Luttinger liquids and single-wall carbon nanotubes

A comprehensive theory of electron spin resonance (ESR) for a Luttinger liquid state of correlated metals is presented. The ESR measurables such as the signal intensity and the linewidth are calculated in the framework of Luttinger liquid theory with broken spin rotational symmetry as a function of magnetic field and temperature. We obtain a significant temperature dependent homogeneous line broadening which is related to the spin-symmetry breaking and the electron-electron interaction. The result crosses over smoothly to the ESR of itinerant electrons in the noninteracting limit. These findings explain the absence of the long-sought ESR signal of itinerant electrons in single-wall carbon nanotubes when considering realistic experimental conditions.

Density of states deduced from ESR measurements on low‐dimensional nanostructures; benchmarks to identify the ESR signals of graphene and SWCNTs

Electron spin resonance (ESR) spectroscopy is an important tool to characterize the ground state of conduction electrons and to measure their spin-relaxation times. Observing ESR of the itinerant electrons is thus of great importance in graphene and in single-wall carbon nanotubes. Often, the identification of CESR signal is based on two facts: the apparent asymmetry of the ESR signal (known as a Dysonian lineshape) and on the temperature independence of the ESR signal intensity. We argue that these are insufficient as benchmarks and instead the ESR signal intensity (when calibrated against an intensity reference) yields an accurate characterization. We detail the method to obtain the density of states from an ESR signal, which can be compared with theoretical estimates. We demonstrate the success of the method for K doped graphite powder. We give a benchmark for the observation of ESR in graphene.

Nonthermal broadening in the conductance of double quantum dot structures

We study the transport properties of a double quantum dot (DQD) molecule at zero and at finite temperature. The properties of the zero-temperature conductance depend on whether the level attraction between the symmetric and antisymmetric states of the DQD, produced by the coupling to the leads, exceeds or not the interdot tunneling. For finite temperature, we find a remarkable nonthermal broadening effect of the conductance resonance when the energy levels of the individual dots are detuned.

Observation of conduction electron spin resonance in boron-doped diamond

We observe the electron spin resonance of conduction electrons in boron-doped (6400 ppm) superconducting diamond (Tc=3.8 K). We clearly identify the benchmarks of conduction electron spin resonance (CESR): the nearly temperature independent electron spin resonance signal intensity and its magnitude, which is in good agreement with that expected from the density of states through the Pauli spin susceptibility. The temperature dependent CESR linewidth weakly increases with increasing temperature, which can be understood in the framework of the Elliott-Yafet theory of spin relaxation. An anomalous and yet unexplained relation is observed between the g-factor, CESR linewidth, and the resistivity using the empirical Elliott-Yafet relation.

Proximity-induced subgaps in Andreev billiards

We examine the density of states of an Andreev billiard and show that any billiard with a finite upper cutoff in the path length distribution P(s) will possess an energy gap on the scale of the Thouless energy. An exact quantum mechanical calculation for different Andreev billiards gives good agreement with the semiclassical predictions when the energy dependent phase shift for Andreev reflections is properly taken into account. Based on this new semiclassical Bohr-Sommerfeld approximation of the density of states, we derive a simple formula for the energy gap. We show that the energy gap, in units of Thouless energy, may exceed the value predicted earlier from random matrix theory for chaotic billiards.

Preparing local strain patterns in graphene by atomic force microscope based indentation

Patterning graphene into various mesoscopic devices such as nanoribbons, quantum dots, etc. by lithographic techniques has enabled the guiding and manipulation of graphene’s Dirac-type charge carriers. Graphene, with well-defined strain patterns, holds promise of similarly rich physics while avoiding the problems created by the hard to control edge configuration of lithographically prepared devices. To engineer the properties of graphene via mechanical deformation, versatile new techniques are needed to pattern strain profiles in a controlled manner. Here we present a process by which strain can be created in substrate supported graphene layers. Our atomic force microscope-based technique opens up new possibilities in tailoring the properties of graphene using mechanical strain.

Resonance Raman Optical Activity of Single Walled Chiral Carbon Nanotubes

Resonance (vibrational) Raman Optical Activity (ROA) spectra of six chiral single-walled carbon nanotubes (SWCNTs) are studied by theoretical means. Calculations are performed imposing line group symmetry. Polarizability tensors, computed at the π-electron level, are differentiated with respect to DFT normal modes to generate spectral intensities. This computational protocol yields a ROA spectrum in good agreement with the only experiment on SWCNT, available at present. In addition to the conventional periodic electric dipole operator we introduce magnetic dipole and electric quadrupole operators, suitable for conventional k-space calculations. Consequences of the complex nature of the wave function on the scattering cross section are discussed in detail. The resonance phenomenon is accounted for by the short time approximation. Involvement of fundamental vibrations in the region of the intermediate frequency modes is found to be more notable in ROA than in Raman spectra. Calculations indicate exceptionally strong resonance enhancement of SWCNT ROA signals. Resonance ROA profile of the (6,5) tube shows an interesting sign change that may be exploited experimentally for SWCNT identification.