Florian Libisch

• Professor
• Professor (Associate) at TU Wien

We report on the investigation of periodic superstructures in twisted bilayer graphene (tBLG) van der Waals heterostructures, where one of the graphene layers is aligned to hexagonal boron nitride (hBN). Our theoretical simulations reveal that if the ratio of the resulting two moiré unit-cell areas is a simple fraction, the graphene/hBN moiré latti...

Stacking two layers of two-dimensional materials slightly twisted relative to each other causes significant alternations of the physical properties of the resulting bilayer. For graphene, at the right twist angle, the electronic band structure features a flat band at the Fermi level that gives rise to interesting many-body physics such as correlate...

Quantum Hall edge states are the paradigmatic example of bulk-boundary correspondence. They are prone to intricate reconstructions calling for their detailed investigation at high spatial resolution. Here, we map quantum Hall edge states of monolayer graphene at a magnetic field of 7 T with scanning tunneling microscopy. Our graphene sample feature...

We investigate the stability of destructive quantum interference (DQI) in electron transport through graphene nanostructures connected to source and drain electrodes. The fingerprint of DQI is the presence of an antiresonance in the transmission function, and its origin is deeply connected to the topology of the atomic structure, which we discuss i...

Transient absorption spectroscopy is a powerful tool to monitor the out-of-equilibrium optical response of photoexcited semiconductors. When this method is applied to two-dimensional semiconductors deposited on different substrates, the excited state optical properties are inferred from the pump-induced changes in the transmission/reflection of the...

Mechanical strain is a powerful tuning knob for excitons, Coulomb-bound electron–hole complexes dominating optical properties of two-dimensional semiconductors. While the strain response of bright free excitons is broadly understood, the behaviour of dark free excitons (long-lived excitations that generally do not couple to light due to spin and mo...

Quantum Hall edge states are the paradigmatic example of the bulk-boundary correspondence. They are prone to intricate reconstructions calling for their detailed investigation at high spatial resolution. Here, we map quantum Hall edge states of monolayer graphene at a magnetic field of 7 T with scanning tunneling microscopy. The graphene sample fea...

Particlelike scattering states allow for noiseless transport through quantum dots by closely retracing bundles of classical trajectories. We identify such raylike states for electron transport through graphene ribbons. Remarkably, we find that these quasiclassical scattering states can be unambiguously associated with well-defined quantum numbers o...

Mechanical strain is a powerful tuning knob for excitons, Coulomb-bound electron-hole complexes dominating optical properties of two-dimensional semiconductors. While the strain response of bright free excitons is broadly understood, the behavior of dark free excitons (long-lived excitations that generally do not couple to light due to spin and mom...

We employ machine learning to derive tight-binding parametrizations for the electronic structure of defects. We test several machine learning methods that map the atomic and electronic structure of a defect onto a sparse tight-binding parameterization. Since Multi-layer perceptrons (i.e., feed-forward neural networks) perform best we adopt them for...

Understanding the water splitting mechanism in photocatalysis is a rewarding goal as it will allow producing clean fuel for a sustainable life in the future. However, identifying the photocatalytic mechanisms by modeling photoactive nanoparticles requires sophisticated computational techniques based on multiscale modeling. In this review, we will s...

Light-field driven charge motion links semiconductor technology to electric fields with attosecond temporal control. Motivated by ultimate-speed electron-based signal processing, strong-field excitation has been identified viable for the ultrafast manipulation of a solid’s electronic properties but found to evoke perplexing post-excitation dynamics...

Transient field-resolved spectroscopy enables studies of ultrafast dynamics in molecules, nanostructures, or solids with sub-cycle resolution, but previous work has so far concentrated on extracting the dielectric response at frequencies below 50 THz. Here, we implemented transient field-resolved reflectometry at 50–100 THz (3–6 µm) with MHz repeti...

The moir\'e potential of graphene on hexagonal boron nitride (hBN) generates a supercell sufficiently large as to thread a full magnetic flux quantum $\Phi_0$ for experimentally accessible magnetic field strengths. Close to rational fractions of $\Phi_0$, $p/q \cdot\Phi_0$, magnetotranslation invariance is restored giving rise to Brown-Zak fermions...

In moiré crystals formed by stacking van der Waals materials, surprisingly diverse correlated electronic phases and optical properties can be realized by a subtle change in the twist angle. Here, we discover that phonon spectra are also renormalized in MoS2 twisted bilayers, adding an insight to moiré physics. Over a range of small twist angles, th...

A Correction to this paper has been published: https://doi.org/10.1038/s41563-021-00998-1.

We construct a continuum model of twisted trilayer graphene using ab initio density-functional-theory calculations, and we apply it to address twisted trilayer electronic structure. Our model accounts for moiré variation in site energies, hopping between outside layers, and hopping within layers. We focus on the role of a mirror symmetry present in...

Transient field-resolved spectroscopy enables studies of excited charge carrier dynamics in solids with sub-cycle resolution. Field-resolved spectroscopy of solids has been limited to frequencies below 50 THz. Here, we demonstrate transient field-resolved reflectometry at 50-150 THz (2-6 $\mu$m) with MHz repetition rate employing 800 nm 8 fs excita...

We present an embedding approach to treat local electron correlation effects in periodic environments. In a single consistent framework, our plane wave based scheme embeds a local high-level correlation calculation [here, Coupled Cluster (CC) theory], employing localized orbitals, into a low-level correlation calculation [here, the direct Random Ph...

We present an embedding approach to treat local electron correlation effects in periodic environments. In a single, consistent framework, our plane-wave based scheme embeds a local high-level correlation calculation (here Coupled Cluster Theory, CC), employing localized orbitals, into a low-level correlation calculation (here the direct Random Phas...

A finite-size normal conductor, proximity-coupled to a superconductor has been predicted to exhibit a so-called minigap, in which quasiparticle excitations are prohibited. Here, we report on the direct observation of such a minigap in ballistic graphene, coupled to superconducting MoRe leads. The minigap is probed by finite bias spectroscopy throug...

Two-particle spectroscopy with correlated electron pairs is used to establish the causal link between the secondary electron spectrum, the (π+σ) plasmon peak, and the unoccupied band structure of highly oriented pyrolytic graphite. The plasmon spectrum is resolved with respect to the involved interband transitions and clearly exhibits final state e...

Smoothly confined graphene quantum dots (GQDs) localize Dirac electrons with conserved spin and valley degrees of freedom. Recent experimental realization of such structures using a combination of magnetic fields and a scanning tunneling microscope tip showcased their potential in locally probing and adjusting the valley degree of freedom. The pres...

Electron and hole Bloch states in bilayer graphene exhibit topological orbital magnetic moments with opposite signs, which allows for tunable valley-polarization in an out-of-plane magnetic field. This property makes electron and hole quantum dots (QDs) in bilayer graphene interesting for valley and spin-valley qubits. Here, we show measurements of...

We construct a continuum model of twisted trilayer graphene devices using information from {\it ab-initio} density-functional theory calculations and apply it to address electronic structure and transport properties. When the middle layer of an ABA Bernal stacked graphene trilayer is twisted, its important mirror symmetry is retained. The mirror sy...

A gate‐defined quantum dot in bilayer graphene is utilized as a sensitive probe for the charge density of its environment. Under the influence of a perpendicular magnetic field, the charge carrier density of the channel region next to the quantum dot oscillates due to the formation of Landau levels. This is experimentally observed as oscillations i...

In moir\'e crystals formed by stacking van der Waals (vdW) materials, surprisingly diverse correlated electronic phases and optical properties can be realized by a subtle change in the twist angle. Here, we discover that phonon spectra are also renormalized in MoS$_2$ twisted bilayers, adding a new perspective to moir\'e physics. Over a range of sm...

Tailoring of heterostructure properties post-growth would greatly benefit from a modification technique with a monolayer precision. However, appropriate techniques for material modification with this precision are still missing. To achieve such control, slow highly charged ions appear ideal as they carry high amounts of potential energy, which is r...

We report on measurements of quantized conductance in gate-defined quantum point contacts in bilayer graphene that allow the observation of subband splittings due to spin-orbit coupling. The size of this splitting can be tuned from 40 to 80 μeV by the displacement field. We assign this gate-tunable subband splitting to a gap induced by spin-orbit c...

We report on measurements of quantized conductance in gate-defined quantum point contacts in bilayer graphene, which show ballistic transport with spin polarized conductance of 6 $e^2/h$ at high in-plane magnetic fields. At the crossings of the Zeeman spin-split subbands of opposite spins, we observe signatures of interaction effects comparable to...

High carrier mobilities play a fundamental role for high-frequency electronics, integrated optoelectronics as well as for sensor and spintronic applications, where device performance is directly linked to the magnitude of the carrier mobility. Van der Waals heterostructures formed by graphene and hexagonal boron nitride (hBN) already outperform all...

Single-photon emitters play a key role in present and emerging quantum technologies. Several recent measurements have established monolayer WSe$_2$ as a promising candidate for a reliable single photon source. The origin and underlying microscopic processes have remained, however, largely elusive. We present a multi-scale tight-binding simulation f...

Photoemission spectroscopy is central to understanding the inner workings of condensed matter, from simple metals and semiconductors to complex materials such as Mott insulators and superconductors¹. Most state-of-the-art knowledge about such solids stems from spectroscopic investigations, and use of subfemtosecond light pulses can provide a time-d...

We present measurements of quantized conductance in electrostatically induced quantum point contacts in bilayer graphene. The application of a perpendicular magnetic field leads to an intricate pattern of lifted and restored degeneracies with increasing field: at zero magnetic field the degeneracy of quantized one-dimensional subbands is four, beca...

Coherent manipulation of binary degrees of freedom is at the heart of modern quantum technologies. Graphene, the first atomically thin 2D material, offers two binary degrees: the electron spin and the valley degree of freedom. Efficient spin control has been demonstrated in many solid state systems, while exploitation of the valley has only recentl...

We present an approach for embedding defect structures modeled by density functional theory into large-scale tight-binding simulations. We extract local tight-binding parameters for the vicinity of the defect site using Wannier functions. In the transition region between the bulk lattice and the defect the tight-binding parameters are continuously...

We present magneto-Raman spectroscopy measurements on suspended graphene to investigate the charge carrier density-dependent electron-electron interaction in the presence of Landau levels. Utilizing gate-tunable magneto-phonon resonances, we extract the charge carrier density dependence of the Landau level transition energies and the associated eff...

We present magneto-Raman spectroscopy measurements on suspended graphene to investigate the charge carrier density-dependent electron-electron interaction in the presence of Landau levels. Utilizing gate-tunable magneto-phonon resonances, we extract the charge carrier density dependence of the Landau level transition energies and the associated eff...

We demonstrate coherently controlled two-color above-threshold photoemission from a single crystal tungsten nanotip. With optimized fundamental and second harmonic intensities near perfect phase contrast can be obtained.

We extend projection-based embedding techniques to bulk systems to treat point defects in semiconductors and insulators. To avoid non-additive kinetic energy contributions, we construct the density partition using orthogonal subsets of orbitals. We have implemented our approach in the popular Vienna ab initio simulation package software package. We...

We present an embedding approach for semiconductors and insulators based on or- bital rotations in the space of occupied Kohn-Sham orbitals. We have implemented our approach in the popular VASP software package. We demonstrate its power for defect structures in silicon and polaron formation in titania, two challenging cases for conventional Kohn-Sh...

We numerically examine the high-harmonic generation in graphene caused by an intense few-cycle terahertz laser field by solving the time-dependent Dirac equation. The observed spectra feature a complex interplay of interband and intraband electron dynamics. At high harmonic frequencies, we observe a plateau region with a cut-off frequency linearly...

We simulate electron transport through graphene nanoribbons of realistic size containing a p-n junction patterned by electrostatic gates. For a sharp p-n interface, Klein tunneling leads to refocusing of a divergent beam forming a Veselago lens. Wider transition regions allow only electrons with near-perpendicular incidence to pass the junction, fo...

In this article, we present coherent control of above-threshold photoemission from a tungsten nanotip achieving nearly perfect modulation. Depending on the pulse delay between fundamental ( 1560nm ) and second harmonic ( 780nm ) pulses of a femtosecond fiber laser at the nanotip, electron emission is significantly enhanced or depressed during temp...

The way conduction electrons respond to ultrafast external perturbations in low dimensional materials is at the core of the design of future devices for (opto)electronics, photodetection and spintronics. Highly charged ions provide a tool for probing the electronic response of solids to extremely strong electric fields localized down to nanometre-s...

Supplementary Figures, Supplementary Notes and Supplementary References.

The video illustrates the induced charge density for an incoming ion with qin=20 at v=0.87 nm fs-1. The polarization of the surface of graphene due to the approaching HCI, the charge transfer from graphene to the projectile and the excitation of the graphene layer while and after the crossing of the ion are clearly visible.

The nonlinear response of graphene to a THz laser pulse is studied by solving the time-dependent Dirac equation and the time-dependent Schrödinger equation within a tight-binding approximation applied to finite-sized structures. We compare predictions of these two approximations for the harmonic spectrum with the recent experiment by P. Bowlan et a...

The electrostatic confinement of massless charge carriers is hampered by Klein tunneling. Circumventing this problem in graphene mainly relies on carving out nanostructures or applying electric displacement fields to open a band gap in bilayer graphene. So far, these approaches suffer from edge disorder or insufficiently controlled localization of...

Physical systems with loss or gain have resonant modes that decay or grow exponentially with time. Whenever two such modes coalesce both in their resonant frequency and their rate of decay or growth, an 'exceptional point' occurs, giving rise to fascinating phenomena that defy our physical intuition. Particularly intriguing behaviour is predicted t...

Quantum point contacts (QPCs) are cornerstones of mesoscopic physics and central building blocks for quantum electronics. Although the Fermi wave-length in high-quality bulk graphene can be tuned up to hundreds of nanometers, the observation of quantum confinement of Dirac electrons in nanostructured graphene systems has proven surprisingly challen...

Supplementary Figures 1-15, Supplementary Table 1, Supplementary Notes 1-9 and Supplementary References

We demonstrate coherent control of multiphoton and above-threshold photoemission from a single solid-state nanoemitter driven by a fundamental and a weak second harmonic laser pulse. Depending on the relative phase of the two pulses, electron emission is modulated with a visibility of up to 94%. Electron spectra reveal that all observed photon orde...

Quantum point contacts (QPCs) are cornerstones of mesoscopic physics and central building blocks for quantum electronics. Although the Fermi wave-length in high-quality bulk graphene can be tuned up to hundreds of nanometers, the observation of quantum confinement of Dirac electrons in nanostructured graphene systems has proven surprisingly challen...

Physical systems with loss or gain feature resonant modes that are decaying or growing exponentially with time. Whenever two such modes coalesce both in their resonant frequency and their rate of decay or growth, a so-called "exceptional point" occurs, around which many fascinating phenomena have recently been reported to arise. Particularly intrig...

We report a new implementation of the density functional embedding theory (DFET) in the VASP code, using the projector-augmented-wave (PAW) formalism. Newly developed algorithms allow us to efficiently perform optimized effective potential optimizations within PAW. The new algorithm generates robust and physically correct embedding potentials, as w...

Magneto-optical transitions between Landau levels can provide precise spectroscopic information on the electronic structure and excitation spectra of graphene, enabling probes of substrate and many-body effects. We calculate the magneto-optical conductivity of large-size graphene flakes using a tight-binding approach. Our method allows us to direct...

We have investigated electronic transport in graphene nanoribbon devices with additional bar-shaped extensions ("wings") at each side of the device. We find that the Coulomb-blockade dominated transport found in conventional ribbons is strongly modified by the presence of the extensions. States localized far away from the central ribbon contribute...

We investigate the presence of percolating states in disordered two-dimensional topological insulators. In particular, we uncover a close connection between these states and the so-called topological Anderson insulator (TAI), which is a topologically non-trivial phase induced by the presence of disorder. The decay of this phase could previously be...

The interaction between O2 molecules and Al surfaces has long been poorly understood despite its importance in diverse chemical phenomena. Early experimental investigations of adsorption dynamics indicated that abstraction of a single O atom by the surface, instead of dissociative chemisorption, dominates at low O2 incident kinetic energies. Abstra...

We present a shared-memory parallelization of our open-source, local correlation multi-reference framework, TigerCI. Benchmarks of the total parallel speedup show a reasonable scaling for typical modern computing system setups. The efficient use of available computing resources will extend simulations on this high level of theory into a new size re...

Graphene flakes placed on hexagonal boron nitride feature in the presence of a magnetic field a complex electronic structure due to a hexagonal moir\'e potential resulting from the van der Waals interaction with the substrate. The slight lattice mismatch gives rise to a periodic supercell potential. Zone folding is expected to create replica of the...

Semiconductor heterostructures form the cornerstone of many electronic and optoelectronic devices, such as the double-heterostructure laser. Traditionally, they are fabricated using epitaxial growth techniques. Recently, heterostructures have also been obtained by vertical stacking of two-dimensional crystals, such as graphene and related materials...

This study examines the radical nature and spin symmetry of the ground state of the quasi-linear acene and two-dimensional periacene series. For this purpose, high-level ab initio calculations have been performed using the multireference averaged quadratic coupled cluster theory and the COLUMBUS program package. A reference space consisting of rest...

The surface potential of the herringbone reconstruction on Au(111) is known to guide surface-state electrons along the potential channels. Surprisingly, we find by scanning tunneling spectroscopy that hot electrons with kinetic energies twenty times larger than the potential amplitude (38 meV) are still guided. The efficiency even increases with ki...

We present electronic transport measurements through short and narrow (30x30 nm) single layer graphene constrictions on a hexagonal boron nitride substrate. While the general observation of Coulomb-blockade is compatible with earlier work, the details are not: we show that the area on which charge is localized can be significantly larger than the a...

Ab initio modeling of matter has become a pillar of chemical research: with ever-increasing computational power, simulations can be used to accurately predict, for example, chemical reaction rates, electronic and mechanical properties of materials, and dynamical properties of liquids. Many competing quantum mechanical methods have been developed ov...

Orbital-free density functional theory (OFDFT) directly solves for the ground-state electron density. It scales linearly with respect to system size, providing a promising tool for large-scale material simulations. Removal of the orbitals requires use of approximate noninteracting kinetic energy density functionals. If replacing ionic cores with ps...

We introduce a time-dependent potential-functional embedding theory (TD-PFET), in which atoms are grouped into subsystems. In TD-PFET, subsystems can be propagated by different suitable time-dependent quantum mechanical methods and their interactions can be treated in a seamless, first-principles manner. TD-PFET is formulated based on the time-depe...

The propagation of light through samples with random inhomogeneities can be described by way of transmission eigenchannels, which connect incoming and outgoing external propagating modes. Although the detailed structure of a disordered sample can generally not be fully specified, these transmission eigenchannels can nonetheless be successfully cont...

A Multireference Configuration Interaction (MRCI) wavefunction includes both static and dynamic electron correlation. MRCI's well-known flaw, a lack of size extensivity, can be ameliorated with the Multireference Averaged Coupled-Pair Functional (MRACPF). However, the original MRACPF is frequently unstable, sometimes producing unphysical results. T...

Oxygenated hydrocarbons play important roles in combustion science as renewable fuels and additives, but many details about their combustion chemistry remain poorly understood. Although many methods exist for computing accurate electronic energies of molecules at equilibrium geometries, a consistent description of entire combustion reaction potenti...

We present numerical simulations of the capacitive coupling between graphene nanoribbons of various widths and gate electrodes in different configurations. We compare the influence of lateral metallic or graphene side gate structures on the overall back gate capacitive coupling. Most interest- ingly, we find a complex interplay between quantum capa...

We report a novel and general formalism for linear scaling, angular momentum dependent (AMD) orbital free (OF) density functional theory (DFT) to advance the accuracy and applicability of OFDFT. To introduce angular momentum dependence in OFDFT, we devise a hybrid scheme by partitioning the system into muffin-tin spheres and an interstitial region:...

We present a semiclassical approximation to the scattering wavefunction $\Psi(\mathbf{r},k)$ for an open quantum billiard which is based on the reconstruction of the Feynman path integral. We demonstrate its remarkable numerical accuracy for the open rectangular billiard and show that the convergence of the semiclassical wavefunction to the full qu...

Noble metal surfaces play a central role in heterogeneous catalysis. Lasers of the appropriate resonance frequency efficiently generate surface plasmons. These, in turn, may generate hot electrons, which can drive catalytic reactions at low temperatures. In this work, we demonstrate how embedding methods allow for the use of accurate ab-initio corr...

Kohn-Sham (KS) density functional theory (DFT) formulates equations for non-interacting electrons subject to a mean-field KS potential. The exchange and correlation (XC) between electrons are accounted for by density-based XC-functionals. The introduction of orbital-dependent functionals allows for a more accurate treatment of exchange and correlat...

Correlated-wavefunction/density functional theory (CW/DFT) embedding methods aim to combine the formally exact correlation treatment in CW methods with the high efficiency of DFT. By partitioning a system into a cluster and its environment, each part can be treated independently. Different embedding schemes have been proposed. The density-based sch...

When is an acene stable? The pronounced multiradical character of graphene nanoribbons of different size and shape was investigated with high-level multireference methods. Quantitative information based on the number of effectively unpaired electrons leads to specific estimates of the chemical stability of graphene nanostructures.

Wann ist ein Acen stabil? Der multiradikalische Charakter von Graphen‐Nanobändern unterschiedlicher Größe und Form wurde mit Multireferenzmethoden untersucht. Aus den erhaltenen quantitativen Informationen über die Zahl an effektiv ungepaarten Elektronen können spezifische Abschätzungen der chemischen Stabilität von Graphen‐Nanostrukturen getroffen...

We investigate the effect of spatially correlated disorder on two-dimensional topological insulators and on the quantum spin Hall effect which the helical edge states in these systems give rise to. Our work expands the scope of previous investigations which found that uncorrelated disorder can induce a nontrivial phase called the topological Anders...

We simulate electron transport through graphene nanoribbons of experimentally realizable size (length L up to 2 micrometer, width W approximately 40 nm) in the presence of scattering at rough edges. Our numerical approach is based on a modular recursive Green's function technique that features sub-linear scaling with L of the computational effort....

Heterogeneous catalysis is of paramount importance in chemistry and energy applications. Catalysts that couple light energy into chemical reactions in a directed, orbital-specific manner would greatly reduce the energy input requirements of chemical transformations, revolutionizing catalysis-driven chemistry. Here we report the room temperature dis...

Dissociative adsorption of molecular oxygen on the Al(111) surface exhibits mechanistic complexity that remains surprisingly poorly understood in terms of the underlying physics. Experiments clearly indicate substantial energy barriers and a mysteriously large number of adsorbed single oxygen atoms instead of pairs. Conventional first principles qu...

The boundaries of waveguides and nanowires have drastic influence on their coherent scattering properties. Designing the boundary profile is thus a promising approach for transmission and band-gap engineering with many applications. By performing an experimental study of microwave transmission through rough waveguides we demonstrate that a recently...

We investigate the interaction of dioxygen with a clean aluminum (111) surface. The theoretical description of this fundamental process is challenging due to the discrete, abrupt charge transfer (CT) from the metal surface to the molecule. Indeed, experimental investigations suggest a sizeable activation barrier not accounted for by a conventional...

We investigate transport through bulk-disordered graphene nanoribbons and nanoconstrictions. Employing a modular recursive Green's function algorithm, we study devices of realistic size (up to 100.000 nm2). By Fourier transforming the scattered wave we disentangle inter-valley scattering between the two Dirac cones of graphene and intra-valley scat...

Using low-temperature scanning tunneling spectroscopy, we map the local density of states (LDOS) of graphene quantum dots supported on Ir(111). Due to a band gap in the projected Ir band structure around the graphene K point, the electronic properties of the QDs are dominantly graphene-like. Indeed, we compare the results favorably with tight bindi...

We introduce a procedure to generate scattering states which display trajectorylike wave function patterns in wave transport through complex scatterers. These deterministic scattering states feature the dual property of being eigenstates to the Wigner-Smith time-delay matrix Q and to the transmission matrix t(†)t with classical (noiseless) transmis...

We investigate transport through nanoribbons in the presence of disorder scattering. We show that size quantization patterns are only present when SU(2) pseudospin symmetry is preserved. Symmetry breaking disorder renders transverse quantization invisible, which may provide an explanation for the necessity of suspending graphene nanoconstrictions t...