arXiv subjects

Michele Pisarra

Publications and source records attributed to Michele Pisarra.

11 recordsLinked to original sources

arXiv2026

The Hidden Cost of Alloying: Disorder-Driven Transport Collapse in TMDs

Alloying in two dimensional semiconductors is widely used to tune bandgaps, yet its implications for charge and energy transport remain poorly understood. Here, we investigate MoS2xSe2(1-x) alloys as a model system to study the interplay between composition, thickness, and disorder. Optical transitions and valence band dispersions evolve continuously with both stoichiometry and number of layers, with negligible bandgap bowing and a composition dependent attenuation of thickness driven renormalization. In contrast, time resolved spatial mapping of photoexcited carriers reveals a pronounced and asymmetric collapse of carrier diffusivity at intermediate compositions, which cannot be accounted for by changes in effective mass or band alignment, and instead emerges from strong real space fluctuations in the local energetic landscape generated by random chalcogen substitution. Microscopic simulations reproduce the experimental trends and show that the character of disorder depends critically on the direction of alloying, producing either scattering barriers or deep trapping sites. Together, these results demonstrate that transport in TMD alloys is governed by disorder physics, overlooked by conventional optical and photoemission probes at equilibrium. Our findings establish transport as a stringent metric of electronic quality and high-light intrinsic limitations in the usage of TMD alloys for layered semiconductor devices.

cond-mat.mtrl-sci↗

arXiv2026

Magic distances in twisted bilayer graphene

Twisted bilayer graphene exhibits isolated, relatively flat electronic bands near charge neutrality when the interlayer rotation is tuned to specific magic angles. These small misalignments, typically below 1.1°, result in long-period moiré patterns with anomalous electronic properties, posing severe challenges for accurate atomistic simulations due to the large supercell sizes required. Here, we introduce a framework to map arbitrarily stacked graphene bilayers, characterized by specific rotation angles corresponding to precise interplanar distances, onto an equivalence class represented by magic-angle twisted bilayer graphene. Using a continuum model, we derive the equivalence relation defining this class and extend its implementation to tight-binding approaches. We further explore the applicability of this mapping within density functional theory, demonstrating that the magic-angle physics can be efficiently studied using twisted bilayer graphene configurations with larger stacking angles and computationally manageable supercell sizes. This approach offers a pathway for ab initio investigations into unconventional topological phases and emergent excitations in the low-energy quasi-flat bands of twisted bilayer materials.

cond-mat.mes-hall↗

arXiv2026

Electronic structure of Graphene/Co interfaces

Photoemission, from core levels and valence band, and low-energy electron diffraction (LEED) have been employed to investigate the electronic and structural properties of novel graphene-ferromagnetic (G-FM) systems,obtained by intercalation of one mono-layer (1ML) and several layers (4ML) of Co on G grown on Ir(111). Upon intercalation of 1ML of Co, the Co lattice is resized to match the Ir-Ir lattice parameter, resulting in a mismatched G/Co/Ir(111) system. The intercalation of further Co layers leads to a relaxation of the Co lattice and a progressive formation of a commensurate G layer lying on top. We show the C 1s line shape and the band structure of G in the two artificial phases, mismatched and commensurate G/Co, through a comparison with the electronic structure of G grown directly on a Co thick film. Our results show that while the G valence band mainly reflects the hybridization with the d states of Co, regardless of the structural phase, the C 1s line shape is very sensitive to the rumpling of the G layer and the coordination of carbon atoms with the underlying Co. Even in the commensurate (1x1) G/Co phase, where graphene is in register with the Co film, from the angular dependence of the C 1s core level we infer the presence of a double component, due to in-equivalent adsorption sites of carbon sub-lattices.

cond-mat.mtrl-sci↗

arXiv2025

Orbital-resolved imaging of coherent femtosecond exciton dynamics in coupled molecules

Optical excitation and control of excitonic wavepackets in organic molecules is the basis to energy conversion processes. To gain insights into such processes, it is essential to establish the relationship between the coherence timescales of excitons with the electronic inhomogeneity in the molecules, as well as the influence of intermolecular interactions on exciton dynamics. Here, we demonstrate orbital-resolved imaging of optically induced coherent exciton dynamics in single copper napthalocyanine (CuNc) molecules, and selective coherent excitation of dark and bright triplet excitons in coupled molecular dimers. Ultrafast photon-induced tunneling current enabled atomic-scale imaging and control of the excitons in resonantly excited molecules by employing excitonic wavepacket interferometry. Our results reveal an ultrafast exciton coherence time of ~ 70 fs in a single molecule, which decreases for the triplet excitons in interacting molecules.

physics.optics↗

arXiv2025

Predicting fermionic densities using a Projected Quantum Kernel method

We use a support vector regressor based on a projected quantum kernel method to predict the density structure of 1D fermionic systems of interest in quantum chemistry and quantum matter. The kernel is built on with the observables of a quantum reservoir implementable with interacting Rydberg atoms. Training and test data of the fermionic system are generated using a Density Functional Theory approach. We test the performance of the method for several Hamiltonian parameters, finding a general common behavior of the error as a function of measurement time. At sufficiently large measurement times, we find that the method outperforms the classical linear kernel method and can be competitive with the radial basis function method.

quant-ph↗

arXiv2024

Electron delocalization in a 2D Mott insulator

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.

cond-mat.str-el↗

arXiv2024

Selective Excitation of Vibrations in a Single Molecule

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.

physics.optics↗

arXiv2023

Probing the phase transition to a coherent 2D Kondo lattice

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.

cond-mat.str-el↗

arXiv2022

Imaging and Controlling Coherent Phonon Wave Packets in Single Graphene Nanoribbons

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.

physics.optics↗

arXiv2019

Tunable Graphene Electronics with Local Ultrahigh Pressure

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.

cond-mat.mes-hall↗

arXiv2016

Plasmon modes of graphene nanoribbons with periodic planar arrangements

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.

cond-mat.str-el↗