arXiv subjects

Thomas G. Pedersen

Publications and source records attributed to Thomas G. Pedersen.

At least 19 recordsLinked to original sources

arXiv2022

Nanoscale view of engineered massive Dirac quasiparticles in lithographic superstructures

Massive Dirac fermions are low-energy electronic excitations characterized by a hyperbolic band dispersion. They play a central role in several emerging physical phenomena such as topological phase transitions, anomalous Hall effects and superconductivity. This work demonstrates that massive Dirac fermions can be controllably induced by lithographically patterning superstructures of nanoscale holes in a graphene device. Their band dispersion is systematically visualized using angle-resolved photoemission spectroscopy with nanoscale spatial resolution. A linear scaling of effective mass with feature sizes is discovered, underlining the Dirac nature of the superstructures. In situ electrostatic doping dramatically enhances the effective hole mass and leads to the direct observation of an electronic band gap that results in a peak-to-peak band separation of (0.64 $\pm$ 0.03) eV, which is shown via first-principles calculations to be strongly renormalized by carrier-induced screening. The presented methodology outlines a new approach for band structure engineering guided by directly viewing structurally- and electrically-tunable massive Dirac quasiparticles in lithographic superstructures at the nanoscale.

cond-mat.mes-hall↗

arXiv2021

Efficient ionization of two dimensional excitons by intense single cycle terahertz pulses

External electric fields are highly attractive for dynamical manipulation of excitons in two-dimensional materials. Here, we theoretically study the ionization of excitons in monolayer transition metal dichalcogenides (TMDs) by intense pulsed electric fields in the terahertz (THz) regime. We find that THz pulses with realistic field strengths are capable of ionizing a significant fraction of photogenerated excitons in TMDs into free charge carriers. Short THz pulses are therefore an efficient, non-invasive method of dynamically controlling the free carrier concentration in monolayer TMDs, which is useful for applications such as THz modulators. We further demonstrate that exciton ionization probabilities should be experimentally measurable by comparing free carrier absorption before and after the THz pulse. Detailed results are provided for different TMDs in various dielectric environments.

cond-mat.mtrl-sci↗

arXiv2021

Calculation of the nonlinear response functions of intra-exciton transitions in two-dimensional transition metal dichalcogenides

In this paper, we study the third-order nonlinear optical response due to transitions between excitonic levels in two-dimensional transition metal dichalcogeniedes. To accomplish this, we use methods not applied to the description of excitons in two-dimensional materials so far and combined with a variational approach to describe the $1s$ excitonic state. The aforementioned transitions allow to probe dark states which are not revealed in absorption experiments. We present general formulas capable of describing any third-order process. The specific case of two-photon absorption in WSe2 is studied. The case of the circular well is also studied as a benchmark of the theory.

cond-mat.mes-hall↗

arXiv2020

Two-dimensional Materials with Giant Optical Nonlinearities Near the Theoretical Upper Limit

Nonlinear optical (NLO) phenomena such as harmonic generation, Kerr, and Pockels effects are of great technological importance for lasers, frequency converters, modulators, switches, etc. Recently, two-dimensional (2D) materials have drawn significant attention due to their strong and unique NLO properties. Here, we describe an efficient first-principles workflow for calculating the quadratic optical response and apply it to 375 non-centrosymmetric semiconductor monolayers from the Computational 2D Materials Database (C2DB). Sorting the non-resonant nonlinearities with respect to bandgap $E_g$ reveals an upper limit proportional to $E_g^{-4}$, which is neatly explained by two distinct generic models. We identify multiple promising candidates with giant nonlinearities and bandgaps ranging from 0.4 to 5 eV, some of which approach the theoretical upper limit and greatly outperform known materials. Our comprehensive library of ab initio NLO spectra for all 375 monolayers is freely available via the C2DB website. We expect this work to pave the way for highly efficient and compact opto-electronic devices based on 2D materials.

physics.optics↗

arXiv2020

Ionisation rate and Stark shift of a one-dimensional model of the Hydrogen molecular ion

In this paper we study the ionization rate and the Stark shift of a one-dimensional model of the H$_{2}^{+}$ ion. The finding of these two quantities is reduced to the solutions of a complex eigenvalue problem. We solve this problem both numerically and analytically. In the latter case we consider the regime of small external electrostatic fields and small internuclear distances. We find an excellent agreement between the ionization rate computed with the two approaches, even when the approximate result is pushed beyond its expected validity. The ionization rate is very sensitive to small changes of the external electrostatic field, spanning many orders of magnitude for small changes of the intensity of the external field. The dependence of the ionization on the internuclear distance is also studied, as this has a direct connection with experimental methods in molecular physics. It is shown that for large distances the ionization rate saturates, which is a direct consequence of the behavior of the energy eigenvalue with the internuclear distance. The Stark shift is computed and from it we extract the static polarizability of H$_{2}^{+}$ and compare our results with those found by other authors using more sophisticated methods.

physics.atom-ph↗

arXiv2020

Anisotropic Stark shift, field-induced dissociation, and electroabsorption of excitons in phosphorene

We compute binding energies, Stark shifts, electric-field-induced dissociation rates, and the Franz-Keldysh effect for excitons in phosphorene in various dielectric surroundings. All three effects show a pronounced dependence on the direction of the in-plane electric field, with the dissociation rates in particular decreasing by several orders of magnitude upon rotating the electric field from the armchair to the zigzag axis. To better understand the numerical dissociation rates, we derive an analytical approximation to the anisotropic rates induced by weak electric fields, thereby generalizing the previously obtained result for isotropic two-dimensional semiconductors. This approximation is shown to be valid in the weak-field limit by comparing it to the exact rates. The anisotropy is also apparent in the large difference between armchair and zigzag components of the exciton polarizability tensor, which we compute for the five lowest lying states. As expected, we also find much more pronounced Stark shifts in either the armchair or zigzag direction, depending on the symmetry of the state in question. Finally, an isotropic interaction potential is shown to be an excellent approximation to a more accurate anisotropic interaction derived from the Poisson equation, confirming that the anisotropy of phosphorene is largely due to the direction dependence of the effective masses.

cond-mat.mes-hall↗

arXiv2020

Analytical Quantitative Semi-Classical Approach to the LoSurdo-Stark Effect and Ionization in 2D excitons

Using a semi-classical approach, we derive a fully analytical expression for the ionization rate of excitons in two-dimensional materials due to an external static electric field, which eliminates the need for complicated numerical calculations. Our formula shows quantitative agreement with more sophisticated numerical methods based on the exterior complex scaling approach, which solves a non-hermitian eigenvalue problem yielding complex energy eigenvalues, where the imaginary part describes the ionization rate. Results for excitons in hexagonal boron nitride and the $A-$exciton in transition metal dichalcogenides are given as a simple examples. The extension of the theory to include spin-orbit-split excitons in transition metal dichalcogenides is trivial.

cond-mat.mes-hall↗

arXiv2020

Interlayer excitons in van der Waals heterostructures: Binding energy, Stark shift, and field-induced dissociation

Photoexcited intralayer excitons in van der Waals heterostructures (vdWHs) with type-II band alignment have been observed to tunnel into interlayer excitons on ultrafast timescales. Such interlayer excitons have sufficiently long lifetimes that inducing dissociation with external in-plane electric fields becomes an attractive option of improving efficiency of photocurrent devices. In the present paper, we calculate interlayer exciton binding energies, Stark shifts, and dissociation rates for six different transition metal dichalcogenide (TMD) vdWHs using a numerical procedure based on exterior complex scaling (ECS). We utilize an analytical bilayer Keldysh potential describing the interaction between the electron-hole pair, and validate its accuracy by comparing to the full multilayer Poisson equation. Based on this model, we obtain an analytical weak-field expression for the exciton dissociation rate. The heterostructures analysed are MoS$_2$/MoSe$_2$, MoS$_2$/WS$_2$, MoS$_2$/WSe$_2$, MoSe$_2$/WSe$_2$, WS$_2$/MoSe$_2$, and WS$_2$/WSe$_2$ in various dielectric environments. For weak electric fields, we find that WS$_2$/WSe$_2$ supports the fastest dissociation rates among the six structures. We, furthermore, observe that exciton dissociation rates in vdWHs are significantly larger than in their monolayer counterparts.

cond-mat.mes-hall↗

arXiv2019

Theory of EELS in atomically thin metallic films

We study strongly confined plasmons in ultrathin gold and silver films by simulating electron energy-loss spectroscopy (EELS). Plasmon dispersion relations are directly retrieved from the energy- and momentum-resolved loss probability under normal incidence conditions, whereas they can also be inferred for aloof parallel beam trajectories from the evolution of the plasmon features in the resulting loss spectra as we vary the impinging electron energy. We find good agreement between nonlocal quantum-mechanical simulations based on the random-phase approximation and a local classical dielectric description for silver films of different thicknesses down to a few atomic layers. We further observe only a minor dependence of quantum simulations for these films on the confining out-of-plane electron potential when comparing density-functional theory within the jellium model with a phenomenological experimentally-fitted potential incorporating atomic layer periodicity and in-plane parabolic bands of energy-dependent effective mass. The latter shows also a small dependence on the crystallographic orientation of silver films, while the unphysical assumption of energy-independent electron mass leads to spurious features in the predicted spectra. Interestingly, we find electron band effects to be more relevant in gold films, giving rise to blue shifts when compared to classical or jellium model simulations. In contrast to the strong nonlocal effects found in few-nanometer metal nanoparticles, our study reveals that a local classical description provides excellent quantitative results in both plasmon strength and dispersion when compared to quantum-mechanical simulations down to silver films consisting of only a few atomic layers, thus emphasizing the in-plane nearly-free conduction-electron motion associated with plasmons in these structures.

cond-mat.mes-hall↗

arXiv2019

Plasmons in ultra-thin gold slabs with quantum spill-out: Fourier modal method, perturbative approach, and analytical model

We numerically study the effect of the quantum spill-out (QSO) on the plasmon mode indices of an ultra-thin metallic slab, using the Fourier modal method (FMM). To improve the convergence of the FMM results, a novel nonlinear coordinate transformation is suggested and employed. Furthermore, we present a perturbative approach for incorporating the effects of QSO on the plasmon mode indices, which agrees very well with the full numerical results. The perturbative approach also provides additional physical insight, and is used to derive analytical expressions for the mode indices using a simple model for the dielectric function. The analytical expressions reproduce the results obtained from the numerically-challenging spill-out problem with much less effort and may be used for understanding the effects of QSO on other plasmonic structures.

physics.optics↗

arXiv2019

Finite-difference time-domain simulation of strong-field ionization: Perfectly matched layer approach

A Finite-Difference Time-Domain (FDTD) scheme with Perfectly Matched Layers (PMLs) is considered for solving the time-dependent Schrödinger equation, and simulate the ionization of an electron initially bound to a one-dimensional $δ$-potential, when applying a strong time-oscillating electric field. The performance of PMLs based on different absorption functions are compared, where we find slowly growing functions to be preferable. PMLs are shown to be able to reduce the computational domain, and thus the required numerical resources, by several orders of magnitude. This is demonstrated by testing the proposed method against an FDTD approach without PMLs and a very large computational domain. We further show that PMLs outperform the well known Exterior Complex Scaling (ECS) technique for short-range potentials when implemented in FDTD, though ECS remains superior for long-range potentials. The accuracy of the method is furthermore demonstrated by comparing with known numerical and analytical results for the $δ$-potential.

cond-mat.mes-hall↗

arXiv2019

Field-induced dissociation of two-dimensional excitons in transition-metal dichalcogenides

Generation of photocurrents in semiconducting materials requires dissociation of excitons into free charge carriers. While thermal agitation is sufficient to induce dissociation in most bulk materials, an additional push is required to induce efficient dissociation of the strongly bound excitons in monolayer transition-metal dichalcogenides (TMDs). Recently, static in-plane electric fields have proven to be a promising candidate. In the present paper, we introduce a numerical procedure, based on exterior complex scaling, capable of computing field-induced exciton dissociation rates for a wider range of field strengths than previously reported in literature. We present both Stark shifts and dissociation rates for excitons in various TMDs calculated within the Mott-Wannier model. Here, we find that the field induced dissociation rate is strongly dependent on the dielectric screening environment. Furthermore, applying weak-field asymptotic theory (WFAT) to the Keldysh potential, we are able to derive an analytical expression for exciton dissociation rates in the weak-field region.

cond-mat.mes-hall↗

arXiv2019

Tuning of impurity-bound interlayer complexes in a van der Waals heterobilayer

Due to their unique two-dimensional nature, charge carriers in semiconducting transition metal dichalcogenides (TMDs) exhibit strong unscreened Coulomb interactions and sensitivity to defects and impurities. The versatility of van der Waals layer stacking allows spatially separating electrons and holes between different TMD layers with staggered band structure, yielding interlayer few-body excitonic complexes whose nature is still debated. Here we combine quantum Monte Carlo calculations with spectrally and temporally resolved photoluminescence measurements on a top- and bottom-gated MoSe2/WSe2 heterostructure, and identify the emitters as impurity-bound interlayer excitonic complexes. Using independent electrostatic control of doping and out-of-plane electric field, we demonstrate control of the relative populations of neutral and charged complexes, their emission energies on a scale larger than their linewidth, and an increase of their lifetime into the microsecond regime. This work unveils new physics of confined carriers and is key to the development of novel optoelectronics applications.

cond-mat.mes-hall↗

arXiv2018

Quantum spill-out in nanometer-thin gold slabs: Effect on plasmon mode index and plasmonic absorption

A quantum mechanical approach and local response theory are applied to study plasmons propagating in nanometer-thin gold slabs sandwiched between different dielectrics. The metal slab supports two different kinds of modes, classified as long-range and short-range plasmons. Quantum spill-out is found to significantly increase the imaginary part of their mode indices, and, surprisingly, even for slabs wide enough to approach bulk the increase is 20%. This is explained in terms of enhanced plasmonic absorption, which mainly takes place at narrow peaks located near the slab surface.

physics.optics↗

arXiv2018

Dissociation of two-dimensional excitons in monolayer WSe2

Two-dimensional (2D) semiconducting materials are promising building blocks for optoelectronic applications, many of which require efficient dissociation of excitons into free electrons and holes. However, the strongly bound excitons arising from the enhanced Coulomb interaction in these monolayers suppresses the creation of free carriers. Here, we probe and identify the main exciton dissociation mechanism through time- and spectrally-resolved photocurrent measurements in a monolayer WSe2 p-n junction. We find that under static in-plane electric field, excitons dissociate at a rate corresponding to the one predicted for the tunnel ionization of 2D Wannier-Mott excitons. This study is essential for the understanding of the optoelectronic photoresponse in of 2D semiconductors, and offers design rules for the realization of efficient photodetectors, valley-dependent optoelectronics and novel quantum coherent phases.

cond-mat.mes-hall↗

arXiv2018

Fast Summation of Divergent Series and Resurgent Transseries in Quantum Field Theories from Meijer-G Approximants

We demonstrate that a Meijer-G-function-based resummation approach can be successfully applied to approximate the Borel sum of divergent series, and thus to approximate the Borel-Écalle summation of resurgent transseries in quantum field theory (QFT). The proposed method is shown to vastly outperform the conventional Borel-Padé and Borel-Padé-Écalle summation methods. The resulting Meijer-G approximants are easily parameterized by means of a hypergeometric ansatz and can be thought of as a generalization to arbitrary order of the Borel-Hypergeometric method [Mera {\it et al.} Phys. Rev. Lett. {\bf 115}, 143001 (2015)]. Here we illustrate the ability of this technique in various examples from QFT, traditionally employed as benchmark models for resummation, such as: 0-dimensional $ϕ^4$ theory, $ϕ^4$ with degenerate minima, self-interacting QFT in 0-dimensions, and the computation of one- and two-instanton contributions in the quantum-mechanical double-well problem.

hep-th↗

arXiv2017

Quantum spill out in few-nanometer metal gaps: Effect on gap plasmons and reflectance from ultrasharp groove arrays

Plasmons in ultranarrow metal gaps are highly sensitive to the electron density profile at the metal surfaces. Using a fully quantum mechanical approach, we study the effects of electron spill-out on gap plasmons and reflectance from ultrasharp metal grooves. We demonstrate that the mode index of ultranarrow gap plasmons converges to the bulk refractive index in the limit of vanishing gap and, thereby, rectify the unphysical divergence found in classical models. Surprisingly, spill-out also significantly increases the plasmonic absorption for few-nanometer gaps and lowers the reflectance from arrays of ultrasharp metal grooves. These findings are explained in terms of enhanced gap plasmon absorption taking place inside the gap 1-2 Å from the walls and delocalization near the groove bottom. Reflectance calculations taking spill-out into account are shown to be in much better agreement with measurements compared with classical models.

cond-mat.mes-hall↗

arXiv2017

On the existence of impurity bound excitons in one-dimensional systems with zero range interactions

We consider a three-body one-dimensional Schrödinger operator with zero range potentials, which models a positive impurity with charge $κ> 0$ interacting with an exciton. We study the existence of discrete eigenvalues as $κ$ is varied. On one hand, we show that for sufficiently small $κ$ there exists a unique bound state whose binding energy behaves like $κ^4$, and we explicitly compute its leading coefficient. On the other hand, if $κ$ is larger than some critical value then the system has no bound states.

math-ph↗