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The prominent role of electron-electron interactions in two-dimensional (2D) materials versus three-dimensional (3D) ones is at the origin of the great variety of fermionic correlated states reported in the literature. In this respect, artificial van der Waals heterostructures comprising single layers of highly correlated insulators allow one to explore the effect of the subtle interlayer interaction in the way electrons correlate. In this work, we study the temperature dependence of the electronic properties of a van der Waals heterostructure composed of a single-layer Mott insulator lying on a metallic substrate by performing quasi-particle interference (QPI) maps. We show the emergence of a Fermi contour in the 2D Mott insulator at temperatures below 11K, which we attribute to the delocalization of the Mott electrons associated with the formation of a quantum coherent Kondo lattice. This Kondo lattice introduces a new periodicity in the system, so that the resulting Fermi surface encompasses both the substrate conduction electrons and the now delocalized correlated electrons from the 2D Mott insulator. Density Functional Theory calculations allow us to pinpoint the scattering vectors responsible for the experimentally observed quasi-particle interference maps, thus providing a complete picture of the delocalization of highly correlated electrons in a 2D Mott insulator., Comment: 15 pages, 4 figures

The capability to excite, probe, and manipulate vibrational modes is essential for understanding and controlling chemical reactions at the molecular level. Recent advancements in tip-enhanced Raman spectroscopies have enabled the probing of vibrational fingerprints in a single molecule with Angstrom-scale spatial resolution. However, achieving controllable excitation of specific vibrational modes in individual molecules remains challenging. Here, we demonstrate the selective excitation and probing of vibrational modes in single deprotonated phthalocyanine molecules utilizing resonance Raman spectroscopy in a scanning tunneling microscope. Selective excitation is achieved by finely tuning the excitation wavelength of the laser to be resonant with the vibronic transitions between the molecular ground electronic state and the vibrational levels in the excited electronic state, resulting in the state-selective enhancement of the resonance Raman signal. Our approach sets the stage for steering chemical transformations in molecules on surfaces by selective excitation of molecular vibrations.

The motion of atoms is at the heart of any chemical or structural transformation in molecules and materials. Upon activation of this motion by an external source, several (usually many) vibrational modes can be coherently coupled, thus facilitating the chemical or structural phase transformation. These coherent dynamics occur on the ultrafast time scale, as revealed, e.g., by nonlocal ultrafast vibrational spectroscopic measurements in bulk molecular ensembles and solids. Tracking and controlling vibrational coherences locally at the atomic and molecular scales is, however, much more challenging and in fact has remained elusive so far. Here, we demonstrate that the vibrational coherences induced by broadband laser pulses on a single graphene nanoribbon (GNR) can be probed by femtosecond coherent anti-Stokes Raman spectroscopy (CARS) when performed in a scanning tunnelling microscope (STM). In addition to determining dephasing (~ 440 fs) and population decay times (~1.8 ps) of the generated phonon wave packets, we are able to track and control the corresponding quantum coherences, which we show to evolve on time scales as short as ~ 70 fs. We demonstrate that a two-dimensional frequency correlation spectrum unequivocally reveals the quantum couplings between different phonon modes in the GNR., Comment: 18 pages

Strongly correlated materials exhibit exotic electronic states arising from the strong correlation between electrons. Dimensionality provides a tuning knob because thinning down to atomic thickness reduces screening effects and enhances electron correlations. In this work, a 2D Kondo lattice has been created by stacking a layer of 1T-TaS2 on a 2H-TaS2 crystal, which are bound by weak van der Waals interactions. By using high-resolution scanning tunnelling spectroscopy and density functional theory, we unambiguously demonstrate the formation of a 2D Kondo lattice from an ensemble of independent Kondo impurities present at higher temperatures. The possibility to create 2D Kondo lattices in van der Waals heterostructures paves the way for the exploration of unconventional metallic, magnetic and superconducting states not present in more standard correlated materials.

We achieve fine tuning of graphene effective doping by applying ultrahigh pressures (> 10 GPa) using Atomic Force Microscopy (AFM) diamond tips. Specific areas in graphene flakes are irreversibly flattened against a SiO2 substrate. Our work represents the first demonstration of local creation of very stable effective p-doped graphene regions with nanometer precision, as unambiguously verified by a battery of techniques. Importantly, the doping strength depends monotonically on the applied pressure, allowing a controlled tuning of graphene electronics. Through this doping effect, ultrahigh pressure modifications include the possibility of selectively modifying graphene areas to improve their electrical contact with metal electrodes, as shown by Conductive AFM. Density Functional Theory calculations and experimental data suggest that this pressure level induces the onset of covalent bonding between graphene and the underlying SiO2 substrate. Our work opens a convenient avenue to tuning the electronics of 2D materials and van der Waals heterostructures through pressure with nanometer resolution.

Among their amazing properties, graphene and related low-dimensional materials show quantized charge-density fluctuations--known as plasmons--when exposed to photons or electrons of suitable energies. Graphene nanoribbons offer an enhanced tunability of these resonant modes, due to their geometrically controllable band gaps. The formidable effort made over recent years in developing graphene-based technologies is however weakened by a lack of predictive modeling approaches that draw upon available {\it ab initio} methods. An example of such a framework is presented here, focusing on narrow-width graphene nanoribbons organized in periodic planar arrays. Time-dependent density-functional calculations reveal unprecedented plasmon modes of different nature at visible to infrared energies. Specifically, semimetallic~(zigzag) nanoribbons display an intraband plasmon following the energy-momentum dispersion of a two-dimensional electron gas. Semiconducting~(armchair) nanoribbons are instead characterized by two distinct intraband and interband plasmons, whose fascinating interplay is extremely responsive to either injection of charge carriers or increase in electronic temperature. These oscillations share some common trends with recent nanoinfrared imaging of confined edge and surface plasmon modes detected in graphene nanoribbons of $100$-$500$~nm width., Comment: 6 Pages, Plus Supplemental Material