arXiv subjects

Kristian S. Thygesen

Publications and source records attributed to Kristian S. Thygesen.

At least 55 records · Page 3Linked to original sources

arXiv2020

Conductance of quantum spin Hall edge states from first principles: the critical role of magnetic impurities and inter-edge scattering

The outstanding transport properties expected at the edge of two-dimensional time-reversal invariant topological insulators have proven to be challenging to realize experimentally, and have so far only been demonstrated in very short devices. In search for an explanation to this puzzling observation, we here report a full first-principles calculation of topologically protected transport at the edge of novel quantum spin Hall insulators - specifically, Bismuth and Antimony halides - based on the non-equilibrium Green's functions formalism. Our calculations unravel two different scattering mechanisms that may affect two-dimensional topological insulators, namely time-reversal symmetry breaking at vacancy defects and inter-edge scattering mediated by multiple co-operating impurities, possibly non-magnetic. We discuss their drastic consequences for typical non-local transport measurements as well as strategies to mitigate their negative impact. Finally, we provide an instructive comparison of the transport properties of topologically protected edge states to those of the trivial edge states in MoS$_2$ ribbons. Although we focus on a few specific cases (in terms of materials and defect types) our results should be representative for the general case and thus have significance beyond the systems studied here.

cond-mat.mes-hall↗

arXiv2020

High throughput computational screening for 2D ferromagnetic materials: the critical role of anisotropy and local correlations

The recent observation of ferromagnetic order in two-dimensional (2D) materials has initiated a booming interest in the subject of 2D magnetism. In contrast to bulk materials, 2D materials can only exhibit magnetic order in the presence of magnetic anisotropy. In the present work we have used the Computational 2D Materials Database (C2DB) to search for new ferromagnetic 2D materials using the spinwave gap as a simple descriptor that accounts for the role of magnetic anisotropy. In addition to known compounds we find 12 novel insulating materials that exhibit magnetic order at finite temperatures. For these we evaluate the critical temperatures from classical Monte Carlo simulations of a Heisenberg model with exchange and anisotropy parameters obtained from first principles. Starting from 150 stable ferromagnetic 2D materials we find five candidates that are predicted to have critical temperatures exceeding that of CrI3. We also study the effect of Hubbard corrections in the framework of DFT+U and find that the value of U can have a crucial influence on the prediction of magnetic properties. Our work provides new insight into 2D magnetism and identifies a new set of promising monolayers for experimental investigation.

cond-mat.mtrl-sci↗

arXiv2019

Accurate ground state- and quasiparticle energies: beyond the RPA and GW methods with adiabatic exchange-correlation kernels

We review the theory and application of adiabatic exchange-correlation (xc-) kernels for ab initio calculations of ground state energies and quasiparticle excitations within the frameworks of the adiabatic connection fluctuation dissipation theorem and Hedin's equations, respectively. Various different xc-kernels, which are all rooted in the homogeneous electron gas, are introduced but hereafter we focus on the specific class of renormalized adiabatic kernels, in particular the rALDA and rAPBE. The kernels drastically improve the description of short-range correlations as compared to the random phase approximation (RPA), resulting in significantly better correlation energies. This effect greatly reduces the reliance on error cancellations, which is essential in RPA, and systematically improves covalent bond energies while preserving the good performance of the RPA for dispersive interactions. For quasiparticle energies, the xc-kernels account for vertex corrections that are missing in the GW self-energy. In this context, we show that the short-range correlations mainly correct the absolute band positions while the band gap is less affected in agreement with the known good performance of GW for the latter. The renormalized xc-kernels offer a rigorous extension of the RPA and GW methods with clear improvements in terms of accuracy at little extra computational cost.

cond-mat.mtrl-sci↗

arXiv2019

Discovering new two-dimensional topological insulators from computational screening

We have performed a computational screening of topological two-dimensional (2D) materials from the Computational 2D Materials Database (C2DB) employing density functional theory. A full \textit{ab initio} scheme for calculating hybrid Wannier functions directly from the Kohn-Sham orbitals has been implemented and the method was used to extract $\mathbb{Z}_2$ indices, Chern numbers and Mirror Chern numbers of 3331 2D systems including both experimentally known and hypothetical 2D materials. We have found a total of 46 quantum spin Hall insulators, 7 quantum anomalous Hall insulators and 9 crystalline topological insulators that are all predicted to be dynamically stable. Roughly one third of these were known prior to the screening. The most interesting of the novel topological insulators are investigated in more detail. We show that the calculated topological indices of the quantum anomalous Hall insulators are highly sensitive to the approximation used for the exchange-correlation functional and reliable predictions of the topological properties of these materials thus require methods beyond density functional theory. We also performed $GW$ calculations, which yield a gap of 0.65 eV for the quantum spin Hall insulator PdSe$_2$ in the MoS$_2$ crystal structure. This is significantly higher than any known 2D topological insulator and three times larger than the Kohn-Sham gap.

cond-mat.mtrl-sci↗

arXiv2018

The Computational 2D Materials Database: High-Throughput Modeling and Discovery of Atomically Thin Crystals

We introduce the Computational 2D Materials Database (C2DB), which organises a variety of structural, thermodynamic, elastic, electronic, magnetic, and optical properties of around 1500 two-dimensional materials distributed over more than 30 different crystal structures. Material properties are systematically calculated by state-of-the art density functional theory and many-body perturbation theory (G$_0\!$W$\!_0$ and the Bethe-Salpeter Equation for $\sim$200 materials) following a semi-automated workflow for maximal consistency and transparency. The C2DB is fully open and can be browsed online or downloaded in its entirety. In this paper, we describe the workflow behind the database, present an overview of the properties and materials currently available, and explore trends and correlations in the data. Moreover, we identify a large number of new potentially synthesisable 2D materials with interesting properties targeting applications within spintronics, (opto-)electronics, and plasmonics. The C2DB offers a comprehensive and easily accessible overview of the rapidly expanding family of 2D materials and forms an ideal platform for computational modeling and design of new 2D materials and van der Waals heterostructures.

cond-mat.mes-hall↗

arXiv2018

Efficient Charge Separation in 2D Janus van der Waals Structures with Build-in Electric Fields and Intrinsic p-n Doping

Janus MoSSe monolayers were recently synthesised by replacing S by Se on one side of MoS$_2$ (or vice versa for MoSe$_2$). Due to the different electronegativity of S and Se these structures carry a finite out-of-plane dipole moment. As we show here by means of density functional theory (DFT) calculations, this intrinsic dipole leads to the formation of built-in electric fields when the monolayers are stacked to form $N$-layer structures. For sufficiently thin structures ($N<4$) the dipoles add up and shift the vacuum level on the two sides of the film by $\sim N \cdot 0.7$ eV. However, for thicker films charge transfer occurs between the outermost layers forming atomically thin n- and p-doped electron gasses at the two surfaces. The doping concentration can be tuned between about $5\cdot 10^{12}$ e/cm$^{2}$ and $2\cdot 10^{13}$ e/cm$^{2}$ by varying the film thickness. The surface charges counteract the static dipoles leading to saturation of the vacuum level shift at around 2.2 eV for $N>4$. Based on band structure calculations and the Mott-Wannier exciton model, we compute the energies of intra- and interlayer excitons as a function of film thickness suggesting that the Janus multilayer films are ideally suited for achieving ultrafast charge separation over atomic length scales without chemical doping or applied electric fields. Finally, we explore a number of other potentially synthesisable 2D Janus structures with different band gaps and internal dipole moments. Our results open new opportunities for ultrathin opto-electronic components such as tunnel diodes, photo-detectors, or solar cells.

cond-mat.mtrl-sci↗

arXiv2018

Edge-dependent reflection and inherited fine structure of higher-order plasmons in graphene nanoribbons

We investigate higher-order plasmons in graphene nanoribbons, and present how electronic edge states and wavefunction fine structure influence the graphene plasmons. Based on nearest-neighbor tight-binding calculations, we find that a standing-wave model based on nonlocal bulk plasmon dispersion is surprisingly accurate for armchair ribbons of widths even down to a few nanometers, and we determine the corresponding phase shift upon edge reflection and an effective ribbon width. Wider zigzag ribbons exhibit a similar phase shift, whereas the standing-wave model describes few-nanometer zigzag ribbons less satisfactorily, to a large extent because of their edge states. We directly confirm that also the larger broadening of plasmons for zigzag ribbons is due to their edge states. Furthermore, we report a prominent fine structure in the induced charges of the ribbon plasmons, which for armchair ribbons follows the electronic wavefunction oscillations induced by inter-valley coupling. Interestingly, the wavefunction fine structure is also found in our analogous density-functional theory calculations, and both these and tight-binding numerical calculations are explained quite well with analytical Dirac theory for graphene ribbons.

cond-mat.mes-hall↗

arXiv2018

Emergent scale invariance of non-classical plasmons in graphene nanoribbons

Using a nearest-neighbor tight-binding model we investigate quantum effects of plasmons on few-nanometer wide graphene nanoribbons, both for zigzag and armchair edge terminations. With insight from the Dirac description we find an emerging scale-invariant behavior that deviates from the classical model both for zigzag and armchair structures. The onset of the deviation can be related to the position of the lowest parabolic band in the band structure. Dirac theory is only valid in the parameter subspace where the scale invariance holds that relates narrow ribbons with high doping to wide ribbons with low doping. We also find that the edge states present in zigzag ribbons give rise to a blueshift of the plasmon, in contrast to earlier findings for graphene nanodisks and nanotriangles.

cond-mat.mes-hall↗

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↗

arXiv2017

Simple vertex correction improves GW band energies of bulk and two-dimensional crystals

The GW self-energy method has long been recognized as the gold standard for quasiparticle (QP) calculations of solids in spite of the fact that the neglect of vertex corrections and the use of a DFT starting point lacks rigorous justification. In this work we remedy this situation by including a simple vertex correction that is consistent with an LDA starting point. We analyse the effect of the self-energy by splitting it into a short-range and long-range term which are shown to govern respectively the center and size of the band gap. The vertex mainly improves the short-range correlations and therefore has a small effect on the band gap, while it shifts the band gap center up in energy by around 0.5 eV in good agreement with experiments. Our analysis also explains how the relative importance of short- and long-range interactions in structures of different dimensionality is reflected in their QP energies. Inclusion of the vertex comes at practically no extra computational cost and even improves the basis set convergence compared to GW. The method thus provides an efficient and rigorous improvement over the GW approximation and sets a new standard for quasiparticle calculations of solids.

cond-mat.mtrl-sci↗

arXiv2017

Strong plasmon-phonon splitting and hybridization in 2D materials revealed through a self-energy approach

We reveal new aspects of the interaction between plasmons and phonons in 2D materials that go beyond a mere shift and increase in plasmon width due to coupling to either intrinsic vibrational modes of the material or phonons in a supporting substrate. More precisely, we predict strong plasmon splitting due to this coupling, resulting in a characteristic avoided crossing scheme. We base our results on a computationally efficient approach consisting in including many-body interactions through the electron self-energy. We specify this formalism for a description of plasmons based upon a tight-binding electron Hamiltonian combined with the random-phase approximation. This approach is accurate provided vertex corrections can be neglected, as is is the case in conventional plasmon-supporting metals and Dirac-fermion systems. We illustrate our method by evaluating plasmonic spectra of doped graphene nanotriangles with varied size, where we predict remarkable peak splittings and other radical modifications in the spectra due to plasmons interactions with intrinsic optical phonons. Our method is equally applicable to other 2D materials and provides a simple approach for investigating coupling of plasmons to phonons, excitons, and other excitations in hybrid thin nanostructures.

cond-mat.mes-hall↗

arXiv2017

Quasiparticle band structure engineering in van der Waals heterostructures via dielectric screening

The idea of combining different two-dimensional (2D) crystals in van der Waals heterostructures (vdWHs) has led to a new paradigm for band structure engineering with atomic precision. Due to the weak interlayer couplings, the band structures of the individual 2D crystals are largely preserved upon formation of the heterostructure. However, regardless of the details of the interlayer hybridisation, the size of the 2D crystal band gaps are always reduced due to the enhanced dielectric screening provided by the surrounding layers. The effect can be on the order of electron volts, but its precise magnitude is non-trivial to predict because of the non-local nature of the screening in quasi-2D materials, and it is not captured by effective single-particle methods such as density functional theory. Here we present an efficient and general method for calculating the band gap renormalization of a 2D material embedded in an arbitrary vdWH. The method evaluates the change in the GW self-energy of the 2D material from the change in the screened Coulomb interaction. The latter is obtained using the quantum-electrostatic heterostructure (QEH) model. We benchmark the G$Δ$W method against full first-principles GW calculations and use it to unravel the importance of screening-induced band structure renormalisation in various vdWHs. A main result is the observation that the size of the band gap reduction of a given 2D material when inserted into a heterostructure scales inversely with the polarisability of the 2D material. Our work demonstrates that dielectric engineering \emph{via} van der Waals heterostructuring represents a promising strategy for tailoring the band structure of 2D materials.

cond-mat.mes-hall↗

arXiv2016

Interlayer excitons and Band Alignment in MoS$_2$/hBN/WSe$_2$ van der Waals Heterostructures

Van der Waals heterostructures (vdWH) provide an ideal playground for exploring light-matter interactions at the atomic scale. In particular, structures with a type-II band alignment can yield detailed insight into free carrier-to-photon conversion processes, which are central to e.g. solar cells and light emitting diodes. An important first step in describing such processes is to obtain the energies of the interlayer exciton states existing at the interface. Here we present a general first-principles method to compute the electronic quasi-particle (QP) band structure and excitonic binding energies of incommensurate vdWHs. The method combines our quantum electrostatic heterostructure (QEH) model for obtaining the dielectric function with the many-body GW approximation and a generalized 2D Mott-Wannier exciton model. We calculate the level alignment together with intra and interlayer exciton binding energies of bilayer MoS$_2$/WSe$_2$ with and without intercalated hBN layers, finding excellent agreement with experimental photoluminescence spectra. Comparison to density functional theory calculations demonstrate the crucial role of self-energy and electron-hole interaction effects.

cond-mat.mtrl-sci↗

arXiv2016

Efficient many-body calculations of 2D materials using exact limits for the screened potential: Band gaps of MoS$_2$, hBN, and phosphorene

Calculating the quasiparticle (QP) band structure of two-dimensional (2D) materials within the GW self-energy approximation has proven to be a rather demanding computational task. The main reason is the strong $\mathbf{q}$-dependence of the 2D dielectric function around $\mathbf{q} = \mathbf{0}$ that calls for a much denser sampling of the Brillouin zone than is necessary for similar 3D solids. Here we use an analytical expression for the small $\mathbf{q}$-limit of the 2D response function to perform the BZ integral over the critical region around $\mathbf{q} = \mathbf{0}$. This drastically reduces the requirements on the $\mathbf{q}$-point mesh and implies a significant computational speed-up. For example, in the case of monolayer MoS$_2$, convergence of the $G_0W_0$ band gap to within $\sim 0.1\,\mathrm{eV}$ is achieved with $12\times 12$ $\mathbf{q}$-points rather than the $36\times 36$ mesh required with discrete BZ sampling techniques. We perform a critical assessment of the band gap of the three prototypical 2D semiconductors MoS$_2$, hBN, and phosphorene including the effect of self-consistency at the GW$_0$ and GW level. The method is implemented in the open source GPAW code.

cond-mat.mtrl-sci↗

arXiv2016

Defect Tolerant Monolayer Transition Metal Dichalcogenides

Localized electronic states formed inside the band gap of a semiconductor due to crystal defects can be detrimental to the material's optoelectronic properties. Semiconductors with lower tendency to form defect induced deep gap states are termed defect tolerant. Here we provide a systematic first principles investigation of defect tolerance in 29 monolayer transition metal dichalcogenides (TMDs) of interest for nanoscale optoelectronics. We find that the TMDs based on group VI and X metals form deep gap states upon creation of a chalcogen (S, Se, Te) vacancy while the TMDs based on group IV metals form only shallow defect levels and are thus predicted to be defect tolerant. Interestingly, all the defect sensitive TMDs have valence and conduction bands with very similar orbital composition. This indicates a bonding/anti-bonding nature of the gap which in turn suggests that dangling bonds will fall inside the gap. These ideas are made quantitative by introducing a descriptor that measures the degree of similarity of the conduction and valence band manifolds. Finally, the study is generalized to non-polar nanoribbons of the TMDs where we find that only the defect sensitive materials form edge states within the band gap.

cond-mat.mtrl-sci↗

arXiv2016

Hubbard-$U$ corrected Hamiltonians for non-self-consistent random-phase approximation total-energy calculations: A study of ZnS, TiO$_2$, and NiO

In non-self-consistent calculations of the total energy within the random-phase approximation (RPA) for electronic correlation, it is necessary to choose a single-particle Hamiltonian whose solutions are used to construct the electronic density and non-interacting response function. Here we investigate the effect of including a Hubbard-$U$ term in this single-particle Hamiltonian, to better describe the on-site correlation of 3$d$ electrons in the transition metal compounds ZnS, TiO$_2$ and NiO. We find that the RPA lattice constants are essentially independent of $U$, despite large changes in the underlying electronic structure. We further demonstrate that the non-self-consistent RPA total energies of these materials have minima at nonzero $U$. Our RPA calculations find the rutile phase of TiO$_2$ to be more stable than anatase independent of $U$, a result which is consistent with experiments and qualitatively different to that found from calculations employing $U$-corrected (semi)local functionals. However we also find that the +$U$ term cannot be used to correct the RPA's poor description of the heat of formation of NiO.

cond-mat.mtrl-sci↗

arXiv2015

Simple Screened Hydrogen Model of Excitons in Two-Dimensional Materials

We present a generalized hydrogen model for the binding energies ($E_B$) of excitons in two-dimensional (2D) materials that sheds light on the fundamental differences between excitons in two and three dimensions. In contrast to the well-known hydrogen model of three-dimensional (3D) excitons, the description of 2D excitons is complicated by the fact that the screening cannot be assumed to be local. We show that one can consistently define an effective 2D dielectric constant by averaging the screening over the extend of the exciton. For an ideal 2D semiconductor this leads to a simple expression for $E_B$ that only depends on the excitonic mass and the 2D polarizability $α$. The model is shown to produce accurate results for 51 transition metal dichalcogenides. Remarkably, over a wide range of polarizabilities the expression becomes independent of the mass and we obtain $E_B^{2D}\approx3/(4πα)$, which explains the recently observed linear scaling of exciton binding energies with band gap. It is also shown that the model accurately reproduces the non-hydrogenic Rydberg series in WS$_2$ and can account for screening from the environment.

cond-mat.mes-hall↗

arXiv2015

Anharmonic stabilization and band gap renormalization in the perovskite CsSnI$_3$

Amongst the X(Sn,Pb)Y$_3$ perovskites currently under scrutiny for their photovoltaic applications, the cubic B-$α$ phase of CsSnI$_3$ is arguably the best characterized experimentally. Yet, according to the standard harmonic theory of phonons, this deceptively simple phase should not exist at all due to rotational instabilities of the SnI$_6$ octahedra. Here, employing self-consistent phonon theory we show that these soft modes are stabilized at experimental conditions through anharmonic phonon-phonon interactions between the Cs ions and their iodine cages. We further calculate the renormalization of the electronic energies due to vibrations and find an unusual opening of the band gap, estimated as 0.24 and 0.11 eV at 500 and 300 K, which we attribute to the stretching of Sn-I bonds. Our work demonstrates the important role of temperature in accurately describing these materials.

cond-mat.mtrl-sci↗