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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 small twist angles, the phonon spectra evolve rapidly due to ultra-strong coupling between different phonon modes and atomic reconstructions of the moir\'e pattern. We develop a new low-energy continuum model for phonons that overcomes the outstanding challenge of calculating properties of large moir\'e supercells and successfully captures essential experimental observations. Remarkably, simple optical spectroscopy experiments can provide information on strain and lattice distortions in moir\'e crystals with nanometer-size supercells. The newly developed theory promotes a comprehensive and unified understanding of structural, optical, and electronic properties of moir\'e superlattices., Comment: 21 pages, 4 figures

The growing family of 2D materials led not long ago to combining different 2D layers and building artificial systems in the form of van der Waals heterostructures. Tailoring of heterostructure properties postgrowth 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 released rapidly upon ion neutralization at the position of the ion. The resulting potential energy deposition is thus limited to just a few atomic layers (in contrast to the kinetic energy deposition). Here, we irradiated a freestanding van der Waals MoS2/graphene heterostructure with 1.3 keV/amu xenon ions in high charge states of 38, which led to nanometer-sized pores that appear only in the MoS2 facing the ion beam, but not in graphene beneath the hole. Reversing the stacking order leaves both layers undamaged, which we attribute to the high conductivity and carrier mobility in graphene acting as a shield for the MoS2 underneath. Our main focus is here on monolayer MoS2, but we also analyzed areas with few-layer structures and observed that the perforation is limited to the two topmost MoS2 layers, whereas deeper layers remain intact. Our results demonstrate that in addition to already being a valuable tool for materials processing, the usability of ion irradiation can be extended to mono- (or bi)layer manipulation of van der Waals heterostructures when the localized potential energy deposition of highly charged ions is also added to the toolbox.

A gate-defined quantum dot in bilayer graphene is utilized as a sensitive electrometer for probing 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 in the gate-voltage positions of the Coulomb resonances of the nearby quantum dot. From the frequency of the oscillations, we extract the charge carrier density in the channel and from the amplitude the shift of the quantum dot potential. We compare these experimental results with an electrostatic simulation of the device and find good agreement., Comment: 5 Pages, 4 Figures

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 to obtain size quantization signatures in very recent experiments. Employing a quasi-classical Monte-Carlo simulation, we are able to reproduce and explain key qualitative features of the full quantum-mechanical calculations.

Since the first experimental realizations of graphene nanoribbons,1 graphene nanodevices2 have attracted enormous attention in the quest for future nanoscale technologies. Because of their small band gaps and high charge-carrier mobilities, n-acenes (Figure ​(Figure1)1) and functionalized acenes are being considered as highly interesting building units for organic electronic materials.3 Zigzag nanoribbons feature remarkable spin-polarization and half-metallic properties4 and chemically fascinating challenges have to be solved in the synthesis of such extended polyaromatic hydrocarbons (PAHs).5 Moreover, the chemical properties of graphene nanoribbons may be linked to the reactivity of black carbon surfaces and PAHs in soils, affecting the accumulation of persistent organic pollutants with environmental implications.6

We study wave functions and their nodal patterns in Andreev billiards consisting of a normal-conducting (N) ballistic quantum dot in contact with a superconductor (S). The bound states in such systems feature an electron and a hole component which are coherently coupled by the scattering of electrons into holes at the S-N interface. The wave function “lives” therefore on two sheets of configuration space, each of which features, in general, distinct nodal patterns. By comparing the wave functions and their nodal patterns for holes and electrons detailed tests of semiclassical predictions become possible. One semiclassical theory based on ideal Andreev retroreflection predicts the electron- and hole eigenstates to perfectly mirror each other. We probe the limitations of validity of this model both in terms of the spectral density of the eigenstates and the shape of the wavefunctions in the electron and hole sheet. We identify cases where the Chladni figures for the electrons and holes drastically differ from each other and explain these discrepancies by limitations of the retroreflection picture.

A tunable microwave scattering device is presented which allows the controlled variation of Fano line shape parameters in transmission through quantum billiards. We observe a non-monotonic evolution of resonance parameters that is explained in terms of interacting resonances. The dissipation of radiation in the cavity walls leads to decoherence and thus to a modification of the Fano profile. We show that the imaginary part of the complex Fano q-parameter allows to determine the absorption constant of the cavity. Our theoretical results demonstrate further that the two decohering mechanisms, dephasing and dissipation, are equivalent in terms of their effect on the evolution of Fano resonance lineshapes., 9 pages, 7 figures, submitted to Physica E (conference proceedings)

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 interestingly, we find a complex interplay between quantum capacitance effects in the graphene nanoribbon and the lateral graphene side gates, giving rise to an unconventional negative quantum capacitance. The emerging non-linear capacitive couplings are investigated in detail. The experimentally relevant relative lever arm, the ratio between the coupling of the different gate structures, is discussed., Comment: 8 pages, 6 figures

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 potential energy surfaces (PESs) requires multireference correlated wavefunction theories. Here we use bond dissociation energies (BDEs) as a foundational metric to benchmark methods based on multireference configuration interaction (MRCI) for several classes of oxygenated compounds (alcohols, aldehydes, carboxylic acids, and methyl esters). We compare results from multireference singles and doubles configuration interaction to those utilizing a posteriori and a priori size-extensivity corrections, benchmarked against experiment and coupled cluster theory. We demonstrate that size-extensivity corrections are necessary for chemically accurate BDE predictions even in relatively small molecules and furnish examples of unphysical BDE predictions resulting from using too-small orbital active spaces. We also outline the specific challenges in using MRCI methods for carbonyl-containing compounds. The resulting complete basis set extrapolated, size-extensivity-corrected MRCI scheme produces BDEs generally accurate to within 1 kcal/mol, laying the foundation for this scheme's use on larger molecules and for more complex regions of combustion PESs.

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-domain perspective. For example, attosecond (10-18 seconds) metrology allows electron wave packet creation, transport and scattering to be followed on atomic length scales and on attosecond timescales2-7. However, previous studies could not disclose the duration of these processes, because the arrival time of the photons was not known with attosecond precision. Here we show that this main source of ambiguity can be overcome by introducing the atomic chronoscope method, which references all measured timings to the moment of light-pulse arrival and therefore provides absolute timing of the processes under scrutiny. Our proof-of-principle experiment reveals that photoemission from the tungsten conduction band can proceed faster than previously anticipated. By contrast, the duration of electron emanation from core states is correctly described by semiclassical modelling. These findings highlight the necessity of treating the origin, initial excitation and transport of electrons in advanced modelling of the attosecond response of solids, and our absolute data provide a benchmark. Starting from a robustly characterized surface, we then extend attosecond spectroscopy towards isolating the emission properties of atomic adsorbates on surfaces and demonstrate that these act as photoemitters with instantaneous response. We also find that the tungsten core-electron timing remains unchanged by the adsorption of less than one monolayer of dielectric atoms, providing a starting point for the exploration of excitation and charge migration in technologically and biologically relevant adsorbate systems.