arXiv subjects

Jan Wilhelm

Publications and source records attributed to Jan Wilhelm.

35 records · Page 2Linked to original sources

arXiv2024

Giant DC Residual Current Generated by Subcycle Laser Pulses

Experimental indications have been reported suggesting that laser pulses shining on materials with relativistic dispersion can produce currents that survive long after the illumination has died out. Such residual currents ('remnants') have applications in petahertz logical gates. The remnants' strength strongly depends on the pulse-shape. We develop an analytical formula that allows to optimize the pulse-shape for remnant production; we predict remnants exceeding the values observed so far by orders of magnitude. In fact, remnants can be almost as strong as the peak current under irradiation.

physics.optics↗

arXiv2023

Low-scaling GW algorithm applied to twisted transition-metal dichalcogenide heterobilayers

The $GW$ method is widely used for calculating the electronic band structure of materials. The high computational cost of $GW$ algorithms prohibits their application to many systems of interest. We present a periodic, low-scaling and highly efficient $GW$ algorithm that benefits from the locality of the Gaussian basis and the polarizability. The algorithm enables $G_0W_0$ calculations on a MoSe$_2$/WS$_2$ bilayer with 984 atoms per unit cell, in 42 hours using 1536 cores. This is four orders of magnitude faster than a plane-wave $G_0W_0$ algorithm, allowing for unprecedented computational studies of electronic excitations at the nanoscale.

physics.chem-ph↗

arXiv2023

Influence of chirp and carrier-envelope phase on non-integer high-harmonic generation

High harmonic generation (HHG) is a versatile technique for probing ultrafast electron dynamics. While HHG is sensitive to the electronic properties of the target, HHG also depends on the waveform of the laser pulse. As is well known, (peak) positions, $ω$, in the high-harmonic spectrum can shift when the carrier envelope phase (CEP), $φ$ is varied. We derive formulae describing the corresponding parametric dependencies of CEP shifts; in particular, we have a transparent result for the (peak) shift, $dω/dφ= {-} 2 \bar{\mathfrak f}' ω/ω_0$, where $ω_0$ describes the fundamental frequency and $\bar{\mathfrak f}'$ characterizes the chirp of the driving laser pulse. We compare the analytical formula to full-fledged numerical simulations finding only 17 % average relative absolute deviation in $dω/dφ$. Our analytical result is fully consistent with experimental observations.

physics.optics↗

arXiv2022

Growth optimization and device integration of narrow-bandgap graphene nanoribbons

The electronic, optical and magnetic properties of graphene nanoribbons (GNRs) can be engineered by controlling their edge structure and width with atomic precision through bottom-up fabrication based on molecular precursors. This approach offers a unique platform for all-carbon electronic devices but requires careful optimization of the growth conditions to match structural requirements for successful device integration, with GNR length being the most critical parameter. In this work, we study the growth, characterization, and device integration of 5-atom wide armchair GNRs (5-AGNRs), which are expected to have an optimal band gap as active material in switching devices. 5-AGNRs are obtained via on-surface synthesis under ultra-high vacuum conditions from Br- and I-substituted precursors. We show that the use of I-substituted precursors and the optimization of the initial precursor coverage quintupled the average 5-AGNR length. This significant length increase allowed us to integrate 5-AGNRs into devices and to realize the first field-effect transistor based on narrow bandgap AGNRs that shows switching behavior at room temperature. Our study highlights that optimized growth protocols can successfully bridge between the sub-nanometer scale, where atomic precision is needed to control the electronic properties, and the scale of tens of nanometers relevant for successful device integration of GNRs.

cond-mat.mtrl-sci↗

arXiv2021

Towards GW Calculations on Thousands of Atoms

The GW approximation of many-body perturbation theory is an accurate method for computing electron addition and removal energies of molecules and solids. In a canonical implementation, however, its computational cost is $O(N^4)$ in the system size N, which prohibits its application to many systems of interest. We present a full-frequency GW algorithm in a Gaussian type basis, whose computational cost scales with $N^2$ to $N^3$. The implementation is optimized for massively parallel execution on state-of-the-art supercomputers and is suitable for nanostructures and molecules in the gas, liquid or condensed phase, using either pseudopotentials or all electrons. We validate the accuracy of the algorithm on the GW100 molecular test set, finding mean absolute deviations of 35 meV for ionization potentials and 27 meV for electron affinities. Furthermore, we study the length-dependence of quasiparticle energies in armchair graphene nanoribbons of up to 1734 atoms in size, and compute the local density of states across a nanoscale heterojunction.

physics.chem-ph↗

arXiv2021

Semiconductor-Bloch Formalism: Derivation and Application to High-Harmonic Generation from Dirac Fermions

We rederive the semiconductor Bloch equations emphasizing the close link to the Berry connection. Our rigorous derivation reveals the existence of two further contributions to the current, in addition to the frequently considered intraband and polarization-related interband terms. The extra contributions become sizable in situations with strong dephasing or when the dipole-matrix elements are strongly wave-number dependent. We apply the formalism to high-harmonic generation for a Dirac metal. The extra terms add to the frequency-dependent emission intensity (high-harmonic spectrum) significantly at certain frequencies changing the total signal up to a factor of 10.

cond-mat.mes-hall↗

arXiv2021

Low-scaling $GW$ with benchmark accuracy and application to phosphorene nanosheets

$GW$ is an accurate method for computing electron addition and removal energies of molecules and solids. In a conventional $GW$ implementation, however, its computational cost is $O(N^4)$ in the system size $N$, which prohibits its application to many systems of interest. We present a low-scaling $GW$ algorithm with notably improved accuracy compared to our previous algorithm [J. Phys. Chem. Lett. 2018, 9, 306-312]. This is demonstrated for frontier orbitals using the $GW100$ benchmark set, for which our algorithm yields a mean absolute deviation of only 6 meV with respect to canonical implementations. We show that also excitations of deep valence, semi-core and unbound states match conventional schemes within 0.1 eV. The high accuracy is achieved by using minimax grids with 30 grid points and the resolution of the identity with the truncated Coulomb metric. We apply the low-scaling $GW$ algorithm with improved accuracy to phosphorene nanosheets of increasing size. We find that their fundamental gap is strongly size-dependent varying from 4.0 eV (1.8 nm $\times$ 1.3 nm, 88 atoms) to 2.4 eV (6.9 nm $\times$ 4.8 nm, 990 atoms) at the $\text{ev}GW_0$@PBE level.

physics.chem-ph↗

arXiv2020

CP2K: An Electronic Structure and Molecular Dynamics Software Package -- Quickstep: Efficient and Accurate Electronic Structure Calculations

CP2K is an open source electronic structure and molecular dynamics software package to perform atomistic simulations of solid-state, liquid, molecular and biological systems. It is especially aimed at massively-parallel and linear-scaling electronic structure methods and state-of-the-art ab-initio molecular dynamics simulations. Excellent performance for electronic structure calculations is achieved using novel algorithms implemented for modern high-performance computing systems. This review revisits the main capabilities of CP2k to perform efficient and accurate electronic structure simulations. The emphasis is put on density functional theory and multiple post-Hartree-Fock methods using the Gaussian and plane wave approach and its augmented all-electron extension.

physics.chem-ph↗

arXiv2017

Fast evaluation of solid harmonic Gaussian integrals for local resolution-of-the-identity methods and range-separated hybrid functionals

An integral scheme for the efficient evaluation of two-center integrals over contracted solid harmonic Gaussian functions is presented. Integral expressions are derived for local operators that depend on the position vector of one of the two Gaussian centers. These expressions are then used to derive the formula for three-index overlap integrals where two of the three Gaussians are located at the same center. The efficient evaluation of the latter is essential for local resolution-of-the-identity techniques that employ an overlap metric. We compare the performance of our integral scheme to the widely used Cartesian Gaussian-based method of Obara and Saika (OS). Non-local interaction potentials such as standard Coulomb, modified Coulomb and Gaussian-type operators, that occur in range-separated hybrid functionals, are also included in the performance tests. The speed-up with respect to the OS scheme is up to three orders of magnitude for both, integrals and their derivatives. In particular, our method is increasingly efficient for large angular momenta and highly contracted basis sets.

physics.chem-ph↗

arXiv2015

Ab initio spin-flip conductance of hydrogenated graphene nanoribbons: Spin-orbit interaction and scattering with local impurity spins

We calculate the spin-dependent zero-bias conductance $G_{σσ'}$ in armchair graphene nanoribbons with hydrogen adsorbates employing a DFT-based ab initio transport formalism including spin-orbit interaction. We find that the spin-flip conductance $G_{σ\barσ}$ can reach the same order of magnitude as the spin-conserving one, $G_{σσ}$, due to exchange-mediated spin scattering. In contrast, the genuine spin-orbit interaction appears to play a secondary role, only.

cond-mat.mes-hall↗

arXiv2014

Ab initio quantum transport through armchair graphene nanoribbons: Streamlines in the current density

We calculate the local current density in pristine armchair graphene nanoribbons (AGNRs) with varying width, $N_\mathrm{C}$, employing a density-functional-theory-based ab initio transport formalism. We observe very pronounced current patterns (streamlines) with threefold periodicity in $N_\mathrm{C}$. They arise as a consequence of quantum confinement in the transverse flow direction. Neighboring streamlines are separated by stripes of almost vanishing flow. As a consequence, the response of the current to functionalizing adsorbates is very sensitive to their placement: adsorbates located within the current filaments lead to strong backscattering, while adsorbates placed in other regions have almost no impact at all.

cond-mat.mes-hall↗

arXiv2013

C58 on Au(111): a scanning tunneling microscopy study

C58 fullerenes were adsorbed onto room temperature Au(111) surface by low-energy (~6 eV) cluster ion beam deposition under ultrahigh vacuum conditions. The topographic and electronic properties of the deposits were monitored by means of scanning tunnelling microscopy (STM at 4.2 K). Topographic images reveal that at low coverages fullerene cages are pinned by point dislocation defects on the herringbone reconstructed gold terraces (as well as by step edges). At intermediate coverages, pinned monomers, act as nucleation centres for the formation of oligomeric C58 chains and 2D islands. At the largest coverages studied, the surface becomes covered by 3D interlinked C58 cages. STM topographic images of pinned single adsorbates are essentially featureless. The corresponding local densities of states are consistent with strong cage-substrate interactions. Topographic images of [C58]n oligomers show a stripe-like intensity pattern oriented perpendicular to the axis connecting the cage centers. This striped pattern becomes even more pronounced in maps of the local density of states. As supported by density functional theory, DFT calculations, and also by analogous STM images previously obtained for C60 polymers (M. Nakaya et al., J. Nanosci. Nanotechnol. 11, 2829 (2011)), we conclude that these striped orbital patterns are a fingerprint of covalent intercage bonds. For thick C58 films we have derived a band gap of 1.2 eV from scanning tunnelling spectroscopy data, STS, confirming that the outermost C58 layer behaves as a wide band semiconductor.

cond-mat.mes-hall↗

arXiv2006

Entropic forces generated by grafted semiflexible polymers

The entropic force exerted by the Brownian fluctuations of a grafted semiflexible polymer upon a rigid smooth wall are calculated both analytically and by Monte Carlo simulations. Such forces are thought to play an important role for several cellular phenomena, in particular, the physics of actin-polymerization-driven cell motility and movement of bacteria like Listeria. In the stiff limit, where the persistence length of the polymer is larger than its contour length, we find that the entropic force shows scaling behavior. We identify the characteristic length scales and the explicit form of the scaling functions. In certain asymptotic regimes we give simple analytical expressions which describe the full results to a very high numerical accuracy. Depending on the constraints imposed on the transverse fluctuations of the filament there are characteristic differences in the functional form of the entropic forces; in a two-dimensional geometry the entropic force exhibits a marked peak.

cond-mat.soft↗

arXiv2003

Elasticity of Stiff Polymer Networks

We study the elasticity of a two-dimensional random network of rigid rods (``Mikado model''). The essential features incorporated into the model are the anisotropic elasticity of the rods and the random geometry of the network. We show that there are three distinct scaling regimes, characterized by two distinct length scales on the elastic backbone. In addition to a critical rigidiy percolation region and a homogeneously elastic regime we find a novel intermediate scaling regime, where elasticity is dominated by bending deformations.

cond-mat.soft↗

arXiv1998

Statistical Mechanics of Semiflexible Polymers: Theory and Experiment

We review the physical properties of macromolecular networks, consisting of semiflexible polymers such as actin. We start by giving a theoretical analysis of the conformational statistics and mechanical response of single filaments. Experimentally relevant quantities such as the end-to-end distribution function and the force-extension relation are discussed. The results are used to analyze the elastic modulus of an entangled solution of such objects. We also discuss the short time and long time (terminal regime) dynamics and compare our results with recent dynamic light scattering and viscoelastic measurements. Furthermore, we analyze the elasticity transition in stochastic models of crosslinked networks.

cond-mat.soft↗

arXiv1998

Physics of Solutions and Networks of Semiflexible Macromolecules and the Control of Cell Function

Living cells are soft bodies of a characteristic form, but endowed with a capacity for a steady turnover of their structures. Both of these material properties, i.e. recovery of the shape after an external stress has been imposed and dynamic structural reorganization, are essential for many cellular phenomena. Examples are mechanical properties of tissue, cell motility, cell growth and division, and active intracellular transport. Numerous experiments in vivo and in vitro have shown that the structural element responsible for the extraordinary mechanical and dynamical properties of eukaryotic cells is the cytoskeleton, a three-dimensional assembly of protein fibers such as actin filaments and microtubules. In addition to those biopolymers various proteins with structural and regulatory functions have a major influence on the mechanical properties. At the relevant length-scales (a few microns at most) the building blocks of these biomaterials are very different from conventional polymeric material. In contrast to flexible polymers the persistence length is of the same order of magnitude as their total contour length or even larger. This implies that the physics of such a system is determined by a subtle interplay between energetic and entropic contributions. We review our present understanding of the physics of biopolymers using concepts from macromolecular and statistical physics complemented by computer simulation. These systems open up a new field of soft condensed matter research, which to date is only poorly understood but has a great potential for interesting new physical phenomena.

cond-mat.soft↗

arXiv1996

Radial distribution function of semiflexible polymers

We calculate the distribution function of the end--to--end distance of a semiflexible polymer with large bending rigidity. This quantity is directly observable in experiments on single semiflexible polymers (e.g., DNA, actin) and relevant to their interpretation. It is also an important starting point for analyzing the behavior of more complex systems such as networks and solutions of semiflexible polymers. To estimate the validity of the obtained analytical expressions, we also determine the distribution function numerically using Monte Carlo simulation and find good quantitative agreement.

cond-mat↗