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Florian Libisch

Publications and source records attributed to Florian Libisch.

At least 19 recordsLinked to original sources

Feasibility study of continuous electronic Pomeranchuk cooling with a flavor-degenerate Wigner crystal

Achieving sub-millikelvin electron temperatures in nanoelectronic devices could unveil new transport phenomena, extend quantum coherence times, and enhance the precision of quantum metrology. However, maintaining such low temperatures continuously remains a long-standing challenge. Here, we propose and simulate an on-chip cooling cycle that harnesses the entropy difference between an electron liquid (EL) and a Wigner crystal (WC) in flavor-degenerate flat-band materials. Cooling is driven by a current through a device with a locally gated region. Within this region, the charge carrier density is tuned such that a WC forms beneath the gate. As carriers transition from an EL to WC phase, their entropy increases, extracting heat and the sliding WC advects this heat along the device. The heat is then released when carriers transition back to the EL phase, which establishes distinct hot and cold regions and a steady temperature gradient over the device. Simulations show net cooling for sufficiently low current densities, typically below $1~\mathrm{nA}/\mu\mathrm{m}$, whereas Joule heating dominates at higher currents. Within the gated region, we estimate cooling powers of up to $8.4~\mathrm{aW}/\mu\mathrm{m}$ at a bath temperature of $4~\mathrm{mK}$. Our approach can achieve electron temperatures well below $1~\mathrm{mK}$ under suitable conditions, promising a route towards continuous on-chip cooling in this temperature regime. Our approach applies to any flat-band material with low-energy flavor degeneracy (valley and/or orbital) and low disorder, including gapped Bernal-stacked bilayer graphene, rhombohedral-stacked multilayer graphene, and magic-angle twisted bilayer graphene.

cond-mat.mes-hall

Hydrogen Activation via Dihydride Formation on a Rh1/Fe3O4(001) Single-Atom Catalyst

Hydrogen activation is a key elementary step in catalytic hydrogenation. In heterogeneous catalysis, it usually proceeds through dissociative adsorption on metal nanoparticles followed by surface diffusion or spillover, whereas homogeneous catalysts activate H2 through dihydride or dihydrogen intermediates at a single metal center. Here, we show that isolated Rh adatoms supported on Fe3O4(001) activate hydrogen through formation of a stable dihydride species without atomic H spillover. Temperature-programmed desorption, X-ray photoelectron spectroscopy, and scanning tunneling microscopy collectively reveal strong (approximately 1 eV) hydrogen adsorption exclusively at isolated Rh1 sites, while isotope-exchange experiments further demonstrate that hydrogen remains localized. Density-functional theory based calculations indicate a barrierless conversion from molecular H2 to the dihydride, and random-phase approximation calculations further confirm the relative stability of the dihydride. Together, these results show that single-atom Rh sites cleave and bind H2 through a dihydride pathway analogous to homogeneous complexes, establishing a mechanistic bridge between homogeneous and heterogeneous catalysis.

cond-mat.mtrl-sci

Radio-frequency charge detection on graphene electron-hole double quantum dots

High-fidelity detection of charge transitions in quantum dots (QDs) is a key ingredient in solid state quantum computation. We demonstrate high-bandwidth radio-frequency charge detection in bilayer graphene quantum dots (QDs) using a capacitively coupled quantum point contact (QPC). The device design suppresses screening effects and enables sensitive QPC-based charge readout. The QPC is arranged to maximize the readout contrast between two neighboring, coupled electron and hole QDs. We apply the readout scheme to a single-particle electron-hole double QD and demonstrate time-resolved detection of charge states as well as magnetic field dependent tunneling rates. This promises a high-fidelity readout scheme for individual spin and valley states, which is important for the operation of spin, valley or spin-valley qubits in bilayer graphene.

cond-mat.mes-hall

Machine-Learned Force Fields for Lattice Dynamics at Coupled-Cluster Level Accuracy

We investigate Machine-Learned Force Fields (MLFFs) trained on approximate Density Functional Theory (DFT) and Coupled Cluster (CC) level potential energy surfaces for the carbon diamond and lithium hydride solids. We assess the accuracy and precision of the MLFFs by calculating phonon dispersions and vibrational densities of states (VDOS) that are compared to experiment and reference ab initio results. To overcome limitations from long-range effects and the lack of atomic forces in the CC training data, a delta-learning approach based on the difference between CC and DFT results, as well as a charge aware MLFF approach is explored. Compared to DFT, MLFFs trained on CC theory yield higher vibrational frequencies for optical modes, agreeing better with experiment. Furthermore, the MLFFs are used to estimate anharmonic effects on the VDOS of lithium hydride at the level of CC theory.

cond-mat.mtrl-sci

Multi-Technique Characterization of Rhodium Gem-Dicarbonyls on TiO$_2$(110)

Gem-dicarbonyls of transition metals supported on metal (oxide) surfaces are common intermediates in heterogeneous catalysis. While infrared (IR) spectroscopy is a standard tool for detecting these species on applied catalysts, the ill-defined crystallographic environment of species observed on powder catalysts renders data interpretation challenging. In this work, we apply a multi-technique surface science approach to investigate rhodium gem-dicarbonyls on a single-crystalline rutile TiO$_2$(110) surface. We combine spectroscopy, scanning probe microscopy, and Density Functional Theory (DFT) to determine their location and coordination on the surface. IR spectroscopy shows the successful creation of gem-dicarbonyls on a titania single crystal by exposing deposited Rh atoms to CO gas, followed by annealing to 200-250 K. Low-temperature scanning tunneling microscopy (STM) and non-contact atomic force microscopy (nc-AFM) data reveal that these complexes are mostly aligned along the [001] crystallographic direction, corroborating theoretical predictions. Notably, x-ray photoelectron spectroscopy (XPS) data reveal multiple rhodium species on the surface, even when the IR spectra show only the signature of rhodium gem-dicarbonyls. As such, our results highlight the complex behavior of carbonyls on metal oxide surfaces, and demonstrate the necessity of multi-technique approaches for the adequate characterization of single-atom catalysts.

physics.chem-ph

Strain engineering of valley-polarized hybrid excitons in a 2D semiconductor

Encoding and manipulating digital information in quantum degrees of freedom is one of the major challenges of today's science and technology. The valley indices of excitons in transition metal dichalcogenides (TMDs) are well-suited to address this challenge. Here, we demonstrate a new class of strain-tunable, valley-polarized hybrid excitons in monolayer TMDs, comprising a pair of energy-resonant intra- and intervalley excitons. These states combine the advantages of bright intravalley excitons, where the valley index directly couples to light polarization, and dark intervalley excitons, characterized by low depolarization rates. We demonstrate that the hybridized state of dark KK' intervalley and defect-localized excitons exhibits a degree of circular polarization of emitted photons that is three times higher than that of the constituent species. Moreover, a bright KK intravalley and a dark KQ exciton form a coherently coupled hybrid state under energetic resonance, with their valley depolarization dynamics slowed down a hundredfold. Overall, these valley-polarized hybrid excitons with strain-tunable valley character emerge as prime candidates for valleytronic applications in future quantum and information technology.

cond-mat.mes-hall

Identifying Electronic Doorway States in the Secondary Electron Emission from Layered Materials

We investigate the secondary low-energy electron emission induced by inelastic electron scattering from graphene and layered materials thereof. By applying a coincidence detection of the primary scattered and the emitted secondary electron we unravel pronounced resonance features otherwise overshadowed by the largely structureless secondary electron energy distribution. Supported by density functional theory calculations we show that these structures are the signature of prominent Feshbach resonances above the vacuum threshold which originate from interlayer states acting as a doorway state for electron emission. Remarkably, some of these doorway states open up only for samples with more than five layers.

cond-mat.mes-hall

Corrugation-dominated mechanical softening of defect-engineered graphene

We measure the two-dimensional elastic modulus $E^\text{2D}$ of atomically clean defect-engineered graphene with a known defect distribution and density in correlated ultra-high vacuum experiments. The vacancies are introduced via low-energy (< 200 eV) Ar ion irradiation and the atomic structure is obtained via semi-autonomous scanning transmission electron microscopy and image analysis. Based on atomic force microscopy nanoindentation measurements, a decrease of $E^\text{2D}$ from 286 to 158 N/m is observed when measuring the same graphene membrane before and after an ion irradiation-induced vacancy density of $1.0\times 10^{13}$ cm$^{-2}$. This decrease is significantly greater than what is predicted by most theoretical studies and in stark contrast to some measurements presented in the literature. With the assistance of atomistic simulations, we show that this softening is mostly due to corrugations caused by local strain at vacancies with two or more missing atoms, while the influence of single vacancies is negligible. We further demonstrate that the opposite effect can be measured when surface contamination is not removed before defect engineering

cond-mat.mtrl-sci

Current-induced brightening of vacancy-related emitters in hexagonal boron nitride

We perform photoluminescence measurements on vacancy-related emitters in hexagonal boron nitride (hBN) that are notorious for their low quantum yields. The gating of these emitters via few-layer graphene electrodes reveals a reproducible, gate-dependent brightening of the emitter, which coincides with a change in the direction of the simultaneously measured leakage current across the hBN layers. At the same time, we observe that the relative increase of the brightening effect scales linearly with the intensity of the excitation laser. Both observations can be explained in terms of a photo-assisted electroluminescence effect. Interestingly, emitters can also show the opposite behavior, i.e. a decrease in emitter intensity that depends on the gate leakage current. We explain these two opposing behaviors with different concentrations of donor and acceptor states in the hBN and show that precise control of the doping of hBN is necessary to gain control over the brightness of vacancy-related emitters by electrical means. Our findings contribute to a deeper understanding of vacancy-related defects in hBN that is necessary to make use of their potential for quantum information processing.

cond-mat.mes-hall

Negative electronic compressibility in charge islands in twisted bilayer graphene

We report on the observation of negative electronic compressibility in twisted bilayer graphene for Fermi energies close to insulating states. To observe this negative compressibility, we take advantage of naturally occurring twist angle domains that emerge during the fabrication of the samples, leading to the formation of charge islands. We accurately measure their capacitance using Coulomb oscillations, from which we infer the compressibility of the electron gas. Notably, we not only observe the negative electronic compressibility near correlated insulating states at integer filling, but also prominently near the band insulating state at full filling, located at the edges of both the flat- and remote bands. Furthermore, the individual twist angle domains yield a well-defined carrier density, enabling us to quantify the strength of electronic interactions and verify the theoretical prediction that the inverse negative capacitance contribution is proportional to the average distance between the charge carriers. A detailed analysis of our findings suggests that Wigner crystallization is the most likely explanation for the observed negative electronic compressibility.

cond-mat.mes-hall

Band gap formation in commensurate twisted bilayer graphene/hBN moir\'e lattices

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 moir\'e unit cell areas is a simple fraction, the graphene/hBN moir\'e lattice acts as a staggered potential, breaking the degeneracy between tBLG AA sites. This leads to additional band gaps at energies where a subset of tBLG AA sites is fully occupied. These gaps manifest as Landau fans in magnetotransport, which we experimentally observe in an aligned tBLG/hBN heterostructure. Our study demonstrates the identification of commensurate tBLG/hBN van-der-Waals heterostructures by magnetotransport, highlights the persistence of moir\'e effects on length scales of tens of nanometers, and represents an interesting step forward in the ongoing effort to realise designed quantum materials with tailored properties.

cond-mat.mes-hall

Strain fingerprinting of exciton valley character

Momentum-indirect excitons composed of electrons and holes in different valleys define optoelectronic properties of many semiconductors, but are challenging to detect due to their weak coupling to light. The identification of an excitons' valley character is further limited by complexities associated with momentum-selective probes. Here, we study the photoluminescence of indirect excitons in controllably strained prototypical 2D semiconductors (WSe$_2$, WS$_2$) at cryogenic temperatures. We find that these excitons i) exhibit valley-specific energy shifts, enabling their valley fingerprinting, and ii) hybridize with bright excitons, becoming directly accessible to optical spectroscopy methods. This approach allows us to identify multiple previously inaccessible excitons with wavefunctions residing in K, $Γ$, or Q valleys in the momentum space as well as various types of defect-related excitons. Overall, our approach is well-suited to unravel and tune intervalley excitons in various semiconductors.

cond-mat.mes-hall

Strain control of hybridization between dark and localized excitons in a 2D semiconductor

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 momentum conservation) or localized excitons related to defects remains mostly unexplored. Here, we develop a technique capable of straining pristine suspended WSe2 kept at cryogenic temperatures up to 3\% to study the strain behavior of these fragile many-body states. We find that under the application of strain, dark and localized excitons in monolayer WSe2 - a prototypical 2D semiconductor - are brought into energetic resonance, forming a new hybrid state that inherits the properties of the constituent species. The characteristics of the hybridized state, including an order-of-magnitude enhanced light/matter coupling, avoided-crossing energy shifts, and strain tunability of many-body interactions, are all supported by first-principles calculations. The hybridized exciton reported here may play a critical role in the operation of single quantum emitters based on WSe2. Furthermore, the techniques we developed may be used to fingerprint unidentified excitonic states

cond-mat.mtrl-sci

Wannier Diagram and Brown-Zak Fermions of Graphene on Hexagonal Boron-Nitride

The moiré potential of graphene on hexagonal boron nitride (hBN) generates a supercell sufficiently large as to thread a full magnetic flux quantum $Φ_0$ for experimentally accessible magnetic field strengths. Close to rational fractions of $Φ_0$, $p/q \cdotΦ_0$, magnetotranslation invariance is restored giving rise to Brown-Zak fermions featuring the same dispersion relation as in the absence of the field. Employing a highly efficient numerical approach we have performed the first realistic simulation of the magnetoconductance for a 250 nm wide graphene ribbon on hexagonal boron nitride using a full ab-initio derived parametrization including strain. The resulting Hofstadter butterfly is analyzed in terms of a novel Wannier diagram for Landau spectra of Dirac particles that includes the lifting of the spin and valley degeneracy by the magnetic field and the moiré potential. This complex diagram can account for many experimentally observed features on a single-particle level, such as spin and valley degeneracy lifting and a non-periodicidy in $Φ_0$.

cond-mat.mes-hall

Minigap and Andreev bound states in ballistic graphene

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 through a weakly coupled junction in the graphene region and its value is given by the dimensions of the device. Besides the minigap, we observe a distinct peak in the differential resistance, which we attribute to weakly coupled Andreev bound states (ABS) located near the superconductor-graphene interface. For weak magnetic fields, the phase accumulated in the normal-conducting region shifts the ABS in quantitative agreement with predictions from tight-binding calculations based on the Bogolioubov-de Gennes equation as well as with an analytical semiclassical model.

cond-mat.mes-hall

Mirror Symmetry Breaking and Lateral Stacking Shifts in Twisted Trilayer Graphene

We construct a continuum model of twisted trilayer graphene using {\it ab initio} density-functional-theory calculations, and apply it to address twisted trilayer electronic structure. Our model accounts for moiré variation in site energies, hopping between outside layers and within layers. We focus on the role of a mirror symmetry present in ABA graphene trilayers with a middle layer twist. The mirror symmetry is lost intentionally when a displacement field is applied between layers, and unintentionally when the top layer is shifted laterally relative to the bottom layer. We use two band structure characteristics that are directly relevant to transport measurements, the Drude weight and the weak-field Hall conductivity, and relate them via the Hall density to assess the influence of the accidental lateral stacking shifts currently present in all experimental devices on electronic properties, and comment on the role of the possible importance of accidental lateral stacking shifts for superconductivity in twisted trilayers.

cond-mat.mes-hall

Local embedding of Coupled Cluster theory into the Random Phase Approximation using plane-waves

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 Phase Approximation, RPA). This choice allows for an accurate and effcient treatment of long-range dispersion effects. Accelerated convergence with respect to the local fragment size can be observed if the low-level and high-level long-range dispersion are quantitatively similar, as is the case for CC in RPA. To demonstrate the capabilities of the introduced embedding approach, we calculate adsorption energies of molecules on a surface and in a chabazite crystal cage, as well as the formation energy of a lattice impurity in a solid at the level of highly accurate many-electron perturbation theories. The absorption energy of a methane molecule in a zeolite chabazite, for instance, is converged with an error well below 20 meV at the CC level. As our largest periodic benchmark system, we apply our scheme to the adsorption of a water molecule on titania in a supercell containing more than 1000 electrons.

physics.chem-ph

Time-dependent screening explains the ultrafast excitonic signal rise in 2D semiconductors

We calculate the time evolution of the transient reflection signal in an MoS$_2$ monolayer on a SiO$_2$/Si substrate using first-principles out-of-equilibrium real-time methods. Our simulations provide a simple and intuitive physical picture for the delayed, yet ultrafast, evolution of the signal whose rise time depends on the excess energy of the pump laser: at laser energies above the A- and B-exciton, the pump pulse excites electrons and holes far away from the K valleys in the first Brillouin zone. Electron-phonon and hole-phonon scattering lead to a gradual relaxation of the carriers towards small $\textit{Active Excitonic Regions}$ around K, enhancing the dielectric screening. The accompanying time-dependent band gap renormalization dominates over Pauli blocking and the excitonic binding energy renormalization. This explains the delayed buildup of the transient reflection signal of the probe pulse, in excellent agreement with recent experimental data. Our results show that the observed delay is not a unique signature of an exciton formation process but rather caused by coordinated carrier dynamics and its influence on the screening.

cond-mat.mtrl-sci