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Thomas G. Pedersen

Publications and source records attributed to Thomas G. Pedersen.

31 records · Page 2Linked to original sources
arXiv2016

Boron and nitrogen doping in graphene antidot lattices

Bottom-up fabrication of graphene antidot lattices (GALs) has previously yielded atomically precise structures with sub-nanometer periodicity. Focusing on this type of experimentally realized GAL, we perform density functional theory calculations on the pristine structure as well as GALs with edge carbon atoms substituted with boron or nitrogen. We show that p- and n-type doping levels emerge with activation energies that depend on the level of hydrogenation at the impurity. Furthermore, a tight-binding parameterization together with a Green's function method are used to describe more dilute doping.

cond-mat.mes-hall↗
arXiv2016

Nonlinear photocurrents in two-dimensional systems based on graphene and boron nitride

DC photoelectrical currents can be generated purely as a non-linear effect in uniform media lacking inversion symmetry without the need for a material junction or bias voltages to drive it, in what is termed photogalvanic effect. These currents are strongly dependent on the polarization state of the radiation, as well as on topological properties of the underlying Fermi surface such as its Berry curvature. In order to study the intrinsic photogalvanic response of gapped graphene (GG), biased bilayer graphene (BBG), and hexagonal boron nitride (hBN), we compute the non-linear current using a perturbative expansion of the density matrix. This allows a microscopic description of the quadratic response to an electromagnetic field in these materials, which we analyze as a function of temperature and electron density. We find that the intrinsic response is robust across these systems and allows for currents in the range of pA cm/W to nA cm/W. At the independent-particle level, the response of hBN-based structures is significant only in the ultra-violet due to their sizeable band-gap. However, when Coulomb interactions are accounted for by explicit solution of the Bethe-Salpeter equation, we find that the photoconductivity is strongly modified by transitions involving exciton levels in the gap region, whose spectral weight dominates in the overall frequency range. Biased bilayers and gapped monolayers of graphene have a strong photoconductivity in the visible and infrared window, allowing for photocurrent densities of several nA cm/W. We further show that the richer electronic dispersion of BBG at low energies and the ability to change its band-gap on demand allows a higher tunability of the photocurrent, including not only its magnitude but also, and significantly, its polarity.

cond-mat.mes-hall↗
arXiv2015

Observation of excitonic resonances in the second harmonic spectrum of MoS$_2$

We measure the second-harmonic (SH) response of MoS$_2$ in a broad fundamental photon energy range between 0.85 and 1.7 eV, and present a continuous SH spectrum capturing signatures of both the fundamental A and B excitons in addition to the intense C resonance. Moreover, we interpret our results in terms of the first exciton simulation of the SH properties of multi-layered MoS$_2$ samples, represented by a study of trilayer MoS$_2$. The good agreement between theory and experiments allows us to establish a connection between the measured spectrum and the underlying electronic structure, in the process elucidating the non-linear excitation of electron-hole pairs.

cond-mat.mes-hall↗
arXiv2012

Exact polarizability and plasmon resonances of partly buried nanowires

The electrostatic polarizability for both vertical and horizontal polarization of two conjoined half-cylinders partly buried in a substrate is derived in an analytical closed-form expression. Using the derived analytical polarizabilities we analyze the localized surface plasmon resonances of three important metal nanowire configurations: (1) a half-cylinder, (2) a half-cylinder on a substrate, and (3) a cylinder partly buried in a substrate. Among other results we show that the substrate plays an important role for spectral location of the plasmon resonances. Our analytical results enable an easy, fast, and exact analysis of many complicated plasmonic nanowire configurations including nanowires on substrates. This is important both for comparison with experimental data, for applications, and as benchmarks for numerical methods.

physics.optics↗
arXiv2012

Polarizability of nanowires at surfaces: Exact solution for general geometry

The polarizability of a nanostructure is an important parameter that determines the optical properties. An exact semi-analytical solution of the electrostatic polarizability of a general geometry consisting of two segments forming a cylinder that can be arbitrarily buried in a substrate is derived using bipolar coordinates, cosine-, and sine-transformations. Based on the presented expressions, we analyze the polarizability of several metal nanowire geometries that are important within plasmonics. Our results provide physical insight into the interplay between the multiple resonances found in the polarizability of metal nanowires at surfaces.

physics.optics↗
arXiv2010

Correlation and dimensional effects of trions in carbon nanotubes

We study the binding energies of singlet trions, i.e. charged excitons, in carbon nanotubes. The problem is modeled, through the effective-mass model, as a three-particle complex on the surface of a cylinder, which we investigate using both one- and two-dimensional expansions of the wave function. The effects of dimensionality and correlation are studied in detail. We find that the Hartree-Fock approximation significantly underestimates the trion binding energy. Combined with band structures calculated using a non-orthogonal nearest neighbour tight binding model, the results from the cylinder model are used to compute physical binding energies for a wide selection of carbon nanotubes. In addition, the dependence on dielectric screening is examined. Our findings indicate that trions are detectable at room temperature in carbon nanotubes with radius below 8Å.

quant-ph↗
arXiv2009

Electronic properties of graphene antidot lattices

Graphene antidot lattices constitute a novel class of nano-engineered graphene devices with controllable electronic and optical properties. An antidot lattice consists of a periodic array of holes which causes a band gap to open up around the Fermi level, turning graphene from a semimetal into a semiconductor. We calculate the electronic band structure of graphene antidot lattices using three numerical approaches with different levels of computational complexity, efficiency, and accuracy. Fast finite-element solutions of the Dirac equation capture qualitative features of the band structure, while full tight-binding calculations and density functional theory are necessary for more reliable predictions of the band structure. We compare the three computational approaches and investigate the role of hydrogen passivation within our density functional theory scheme.

cond-mat.mes-hall↗
arXiv2009

DFT study of graphene antidot lattices: The roles of geometry relaxation and spin

Graphene sheets with regular perforations, dubbed as antidot lattices, have theoretically been predicted to have a number of interesting properties. Their recent experimental realization with lattice constants below 100 nanometers stresses the urgency of a thorough understanding of their electronic properties. In this work we perform calculations of the band structure for various hydrogen-passivated hole geometries using both spin-polarized density functional theory (DFT) and DFT based tight-binding (DFTB) and address the importance of relaxation of the structures using either method or a combination thereof. We find from DFT that all structures investigated have band gaps ranging from 0.2 eV to 1.5 eV. Band gap sizes and general trends are well captured by DFTB with band gaps agreeing within about 0.2 eV even for very small structures. A combination of the two methods is found to offer a good trade-off between computational cost and accuracy. Both methods predict non-degenerate midgap states for certain antidot hole symmetries. The inclusion of spin results in a spin-splitting of these states as well as magnetic moments obeying the Lieb theorem. The local spin texture of both magnetic and non-magnetic symmetries is addressed.

cond-mat.mes-hall↗
arXiv2008

Optical properties of graphene antidot lattices

Undoped graphene is semi-metallic and thus not suitable for many electronic and optoelectronic applications requiring gapped semiconductor materials. However, a periodic array of holes (antidot lattice) renders graphene semiconducting with a controllable band gap. Using atomistic modelling, we demonstrate that this artificial nanomaterial is a dipole-allowed direct gap semiconductor with a very pronounced optical absorption edge. Hence, optical infrared spectroscopy should be an ideal probe of the electronic structure. To address realistic experimental situations, we include effects due to disorder and the presence of a substrate in the analysis.

cond-mat.mes-hall↗
arXiv2008

Graphene Antidot Lattices - Designed Defects and Spin Qubits

Antidot lattices, defined on a two-dimensional electron gas at a semiconductor heterostructure, are a well-studied class of man-made structures with intriguing physical properties. We point out that a closely related system, graphene sheets with regularly spaced holes ("antidots"), should display similar phenomenology, but within a much more favorable energy scale, a consequence of the Dirac fermion nature of the states around the Fermi level. Further, by leaving out some of the holes one can create defect states, or pairs of coupled defect states, which can function as hosts for electron spin qubits. We present a detailed study of the energetics of periodic graphene antidot lattices, analyze the level structure of a single defect, calculate the exchange coupling between a pair of spin qubits, and identify possible avenues for further developments.

cond-mat.mes-hall↗
arXiv2007

Optical second harmonic generation from Wannier excitons

Excitonic effects in the linear optical response of semiconductors are well-known and the subject of countless experimental and theoretical studies. For the technologically important second order nonlinear response, however, description of excitonic effects has proved to be difficult. In this work, a simplified three-band Wannier exciton model of cubic semiconductors is applied and a closed form expression for the complex second harmonic response function including broadening is derived. Our calculated spectra are found to be in excellent agreement with the measured response near the band edge. In addition, a very substantial enhancement of the nonlinear response is predicted for the transparency region.

cond-mat.str-el↗
arXiv2006

The Faraday effect revisited: General theory

This paper is the first in a series revisiting the Faraday effect, or more generally, the theory of electronic quantum transport/optical response in bulk media in the presence of a constant magnetic field. The independent electron approximation is assumed. At zero temperature and zero frequency, if the Fermi energy lies in a spectral gap, we rigorously prove the Widom-Streda formula. For free electrons, the transverse conductivity can be explicitly computed and coincides with the classical result. In the general case, using magnetic perturbation theory, the conductivity tensor is expanded in powers of the strength of the magnetic field $B$. Then the linear term in $B$ of this expansion is written down in terms of the zero magnetic field Green function and the zero field current operator. In the periodic case, the linear term in $B$ of the conductivity tensor is expressed in terms of zero magnetic field Bloch functions and energies. No derivatives with respect to the quasi-momentum appear and thereby all ambiguities are removed, in contrast to earlier work.

cond-mat.mes-hall↗