arXiv subjects

Alessandro De Vita

Publications and source records attributed to Alessandro De Vita.

17 recordsLinked to original sources

arXiv2026

Ultrafast Formation and Annihilation of Strongly Bound, Anisotropic Excitons

Van der Waals (vdW) layered materials with long-range magnetic order have the potential to enable novel optoelectronic and spintronic applications. Among these, CrSBr is an air-stable, direct band gap semiconductor that hosts interlayer antiferromagnetic order, a highly anisotropic electronic structure, and strongly bound excitons. In particular, excitons in CrSBr have been shown to inherit the quasi-one-dimensional nature of the material and also couple to the underlying spinorder. However, mechanisms of exciton formation, dissociation, and interaction with free carriers remain largely unexplored, despite being crucial for spintronic and optoelectronic applications. Here, we employ time- and angle-resolved photoemission spectroscopy to map the electronic structure and excited state dynamics in CrSBr. We directly resolve an exceptionally large exciton binding energy (~800 meV) and a highly anisotropic momentum space distribution of the exciton, revealing its quasi-1D real-space character. We observe an excitation-density-dependent interconversion between bound excitons and quasi-free carriers on sub- to few-picosecond timescales, indicating that many-body effects govern the excited-state dynamics and optical properties during the initial stages of relaxation. Our work highlights the strongly bound, anisotropic character of excitons in CrSBr, as well as the microscopic interactions steering relaxation pathways after photoexcitation in elevated density regimes relevant for future device applications.

cond-mat.mtrl-sci↗

arXiv2026

Orbital mixing and strong Hund's coupling stabilize spin order in van der Waals ferromagnet CrI3

Recent years have seen a vast increase in research into van der Waals magnetic materials. In many of these systems, magnetism is introduced via light 3d-transition metal elements, combined with chalcogenides or halogens. Despite the high technological promise in the field of spintronics, the connection between the d-orbital configuration and the occurrence of low-dimensional magnetic order is currently unclear. Here we address the prototypical two-dimensional ferromagnet CrI3, via complementary spectroscopies and density functional theory calculations. We reveal the electronic structure and orbital character of bulk CrI3 in the paramagnetic and ferromagnetic phases, describing the couplings underpinning its energy diagram, and providing a robust experimental demonstration that the stabilization of ferromagnetism is attributable to orbital mixing between I p and Cr eg states, and to the presence of strong Hund's coupling. These findings reveal the microscopic connection between orbital and spin degrees of freedom, providing fundamental insights into the behavior of low-dimensional magnetic materials.

cond-mat.mtrl-sci↗

arXiv2026

Robust spin splitting and fermiology in a layered altermagnet

Altermagnetism defies conventional classifications of collinear magnetic phases, standing apart from ferromagnetism and antiferromagnetism with its unique combination of spin-dependent symmetries, net-zero magnetization, and anomalous Hall transport. Although altermagnetic states have been realized experimentally, their integration into functional devices has been hindered by the structural rigidity and poor tunability of existing materials. First, through cobalt intercalation of the superconducting 2H-NbSe$_2$ polymorph, we induce and stabilize a robust altermagnetic phase and using both theory and experiment, we directly observe the lifting of Kramers degeneracy. Additionally, we present spectroscopic insight into a previously hinted low-temperature phase, and provide evidence of its electronic origin. While shedding light on overlooked aspects of altermagnetism, these findings open pathways to spin-based technologies and lay a foundation for advancing the emerging field of altertronics.

cond-mat.str-el↗

arXiv2025

Discovery of magnetic-field-tunable density waves in a layered altermagnet

Altermagnets recently came into the spotlight as a new class of magnetic materials, arising as a consequence of specific crystal symmetries. They are characterized by a spin-polarized electronic band structure similar to ferromagnets, but with net zero magnetization, and touted as a promising platform to host a slew of exotic properties, many of which are yet to be explored. Here we study a new layered triangular lattice altermagnet, Co-intercalated NbSe$_2$ using scanning tunneling microscopy and spectroscopy (STM/S). Differential conductance dI/dV spectra at low temperature reveal a surprising partial gap opening centered at the Fermi level, which is not captured by density functional theory calculations of the system in the pure altermagnetic state. Spatial mapping using spectroscopic-imaging STM and spin-polarized STM further reveals emergent tri-directional charge and spin density modulations with a 2a$_0$ wave length. Interestingly, we discover that out-of-plane magnetic field can serve as a knob to tune the amplitudes of the modulations as well as alter the overall electronic density-of-states in a manner that is strongly dependent on the field direction and strength. This can be attributed to the tilting of spins by the external magnetic field, which can have profound implications on the electronic properties of the altermagnet. By providing elusive atomic-scale insights, our work uncovers a tunable density wave accompanied by concomitant changes in the electronic band structure, and sets the foundation for studies of correlated electronic phenomena in altermagnets.

cond-mat.str-el↗

arXiv2025

Anomalous spin-optical helical effect in Ti-based kagome metal

The kagome lattice stands as a rich platform for hosting a wide array of correlated quantum phenomena, ranging from charge density waves and superconductivity to electron nematicity and loop current states. Direct detection of loop currents in kagome systems has remained a formidable challenge due to their intricate spatial arrangements and the weak magnetic field signatures they produce. This has left their existence and underlying mechanisms a topic of intense debate. In this work, we uncover a hallmark reconcilable with loop currents: spin handedness-selective signals that surpass conventional dichroic, spin, and spin-dichroic responses. We observe this phenomenon in the kagome metal CsTi$_3$Bi$_5$ and we call it the anomalous spin-optical helical effect. This effect arises from the coupling of light' s helicity with spin-orbital electron correlations, providing a groundbreaking method to visualize loop currents in quantum materials. Our discovery not only enriches the debate surrounding loop currents but also paves the way for new strategies to exploit the electronic phases of quantum materials via light-matter interaction.

cond-mat.str-el↗

arXiv2024

Bilayer orthogonal ferromagnetism in CrTe$_2$-based van der Waals system

Systems with pronounced spin anisotropy play a pivotal role in advancing magnetization switching and spin-wave generation mechanisms, which are fundamental for spintronic technologies. Quasi-van der Waals ferromagnets, particularly Cr$_{1+δ}$Te$_2$ compounds, represent seminal materials in this field, renowned for their delicate balance between frustrated layered geometries and magnetism. Despite extensive investigation, the precise nature of their magnetic ground state, typically described as a canted ferromagnet, remains contested, as does the mechanism governing spin reorientation under external magnetic fields and varying temperatures. In this work, we leverage a multimodal approach, integrating complementary techniques, to reveal that Cr$_{1+δ}$Te$_2$ ($δ= 0.25 - 0.50$) hosts a previously overlooked magnetic phase, which we term orthogonal-ferromagnetism. This single phase consists of alternating atomically sharp single layers of in-plane and out-of-plane ferromagnetic blocks, coupled via exchange interactions and as such, it differs significantly from crossed magnetism, which can be achieved exclusively by stacking multiple heterostructural elements together. Contrary to earlier reports suggesting a gradual spin reorientation in CrTe$_2$-based systems, we present definitive evidence of abrupt spin-flop-like transitions. This discovery, likely due to the improved crystallinity and lower defect density in our samples, repositions Cr$_{1+δ}$Te$_2$ compounds as promising candidates for spintronic and orbitronic applications, opening new pathways for device engineering.

cond-mat.str-el↗

arXiv2024

Pomeranchuk instability from electronic correlations in CsTi$_3$Bi$_5$ kagome metal

Among many-body instabilities in correlated quantum systems, electronic nematicity, defined by the spontaneous breaking of rotational symmetry, has emerged as a critical phenomenon, particularly within high-temperature superconductors. Recently, this behavior has been identified in CsTi$_3$Bi$_5$, a member of the AV$_3$Sb$_5$ (A = K, Rb, Cs) kagome family, recognized for its intricate and unconventional quantum phases. Despite accumulating indirect evidence, the fundamental mechanisms driving nematicity in CsTi$_3$Bi$_5$ remain inadequately understood, sparking ongoing debates. In this study, we employ polarization-dependent angle-resolved photoemission spectroscopy to reveal definitive signatures of an orbital-selective nematic deformation in the electronic structure of CsTi$_3$Bi$_5$. This direct experimental evidence underscores the pivotal role of orbital degrees of freedom in symmetry breaking, providing new insights into the complex electronic environment. By applying the functional renormalization group technique to a fully interacting ab initio model, we demonstrate the emergence of a finite angular momentum ($d$-wave) Pomeranchuk instability in CsTi$_3$Bi$_5$, driven by the concomitant action of electronic correlations within specific orbital channels and chemical potential detuning away from Van Hove singularities. By elucidating the connection between orbital correlations and symmetry-breaking instabilities, this work lays a crucial foundation for future investigations into the broader role of orbital selectivity in quantum materials, with far-reaching implications for the design and manipulation of novel electronic phases.

cond-mat.str-el↗

arXiv2023

Observation of termination-dependent topological connectivity in a magnetic Weyl kagome-lattice

Engineering surfaces and interfaces of materials promises great potential in the field of heterostructures and quantum matter designer, with the opportunity of driving new many-body phases that are absent in the bulk compounds. Here, we focus on the magnetic Weyl kagome system Co$_3$Sn$_2$S$_2$ and show how for different sample's terminations the Weyl-points connect also differently, still preserving the bulk-boundary correspondence. Scanning-tunnelling microscopy has suggested such a scenario indirectly. Here, we demonstrate this directly for the fermiology of Co$_3$Sn$_2$S$_2$, by linking it to the system real space surfaces distribution. By a combination of micro-ARPES and first-principles calculations, we measure the energy-momentum spectra and the Fermi surfaces of Co$_3$Sn$_2$S$_2$ for different surface terminations and show the existence of topological features directly depending on the top-layer electronic environment. Our work helps to define a route to control bulk-derived topological properties by means of surface electrostatic potentials, creating a realistic and reliable methodology to use Weyl kagome metals in responsive magnetic spintronics.

cond-mat.str-el↗

arXiv2021

Quantitative Ultrafast Electron-Temperature Dynamics in Photo-Excited Au Nanoparticles

The femtosecond evolution of the electronic temperature of laser-excited gold nanoparticles is measured, by means of ultrafast time-resolved photoemission spectroscopy induced by extreme-ultraviolet radiation pulses. The temperature of the electron gas is deduced by recording and fitting high-resolution photo emission spectra around the Fermi edge of gold nanoparticles providing a direct, unambiguous picture of the ultrafast electron-gas dynamics. These results will be instrumental to the refinement of existing models of femtosecond processes in laterally-confined and bulk condensed-matter systems, and for understanding more deeply the role of hot electrons in technological applications.

cond-mat.mtrl-sci↗

arXiv2020

Gaussian Process States: A data-driven representation of quantum many-body physics

We present a novel, non-parametric form for compactly representing entangled many-body quantum states, which we call a `Gaussian Process State'. In contrast to other approaches, we define this state explicitly in terms of a configurational data set, with the probability amplitudes statistically inferred from this data according to Bayesian statistics. In this way the non-local physical correlated features of the state can be analytically resummed, allowing for exponential complexity to underpin the ansatz, but efficiently represented in a small data set. The state is found to be highly compact, systematically improvable and efficient to sample, representing a large number of known variational states within its span. It is also proven to be a `universal approximator' for quantum states, able to capture any entangled many-body state with increasing data set size. We develop two numerical approaches which can learn this form directly: a fragmentation approach, and direct variational optimization, and apply these schemes to the Fermionic Hubbard model. We find competitive or superior descriptions of correlated quantum problems compared to existing state-of-the-art variational ansatzes, as well as other numerical methods.

cond-mat.str-el↗

arXiv2019

Space Charge Free Ultrafast Photoelectron Spectroscopy on Solids by a Narrowband Tunable Extreme Ultraviolet Light Source

Here we report on a novel High Harmonic Generation (HHG) light source designed for space charge free ultrafast photoelectron spectroscopy (PES) on solids. The ultimate overall energy resolution achieved on a polycrystalline Au sample is ~22 meV at 40 K. These results have been obtained at a photon energy of 16.9 eV with a pulse bandwidth of ~19 meV, by varying, up to 200 kHz, the photon pulses repetition rate and the photon fluence on the sample. These features set a new benchmark for tunable narrowband HHG sources. By comparing the PES energy resolution and the photon pulse bandwidth with a pulse duration of ~105 fs, as retrieved from time-resolved (TR) angle resolved (AR) PES experiments on Bi$_2$Se$_3$, we validate a way for a space charge free photoelectric process close to Fourier transform limit conditions for ultrafast TR-PES experiments on solids.

physics.optics↗

arXiv2019

Building nonparametric $n$-body force fields using Gaussian process regression

Constructing a classical potential suited to simulate a given atomic system is a remarkably difficult task. This chapter presents a framework under which this problem can be tackled, based on the Bayesian construction of nonparametric force fields of a given order using Gaussian process (GP) priors. The formalism of GP regression is first reviewed, particularly in relation to its application in learning local atomic energies and forces. For accurate regression it is fundamental to incorporate prior knowledge into the GP kernel function. To this end, this chapter details how properties of smoothness, invariance and interaction order of a force field can be encoded into corresponding kernel properties. A range of kernels is then proposed, possessing all the required properties and an adjustable parameter $n$ governing the interaction order modelled. The order $n$ best suited to describe a given system can be found automatically within the Bayesian framework by maximisation of the marginal likelihood. The procedure is first tested on a toy model of known interaction and later applied to two real materials described at the DFT level of accuracy. The models automatically selected for the two materials were found to be in agreement with physical intuition. More in general, it was found that lower order (simpler) models should be chosen when the data are not sufficient to resolve more complex interactions. Low $n$ GPs can be further sped up by orders of magnitude by constructing the corresponding tabulated force field, here named "MFF".

physics.comp-ph↗

arXiv2018

Building machine learning force fields for nanoclusters

We assess Gaussian process (GP) regression as a technique to model interatomic forces in metal nanoclusters by analysing the performance of 2-body, 3-body and many-body kernel functions on a set of 19-atom Ni cluster structures. We find that 2-body GP kernels fail to provide faithful force estimates, despite succeeding in bulk Ni systems. However, both 3- and many-body kernels predict forces within a $\sim$0.1 eV/$\textÅ$ average error even for small training datasets, and achieve high accuracy even on out-of-sample, high temperature, structures. While training and testing on the same structure always provides satisfactory accuracy, cross-testing on dissimilar structures leads to higher prediction errors, posing an extrapolation problem. This can be cured using heterogeneous training on databases that contain more than one structure, which results in a good trade-off between versatility and overall accuracy. Starting from a 3-body kernel trained this way, we build an efficient non-parametric 3-body force field that allows accurate prediction of structural properties at finite temperatures, following a newly developed scheme [Glielmo et al. PRB 97, 184307 (2018)]. We use this to assess the thermal stability of Ni$_{19}$ nanoclusters at a fractional cost of full ab initio calculations.

physics.comp-ph↗

arXiv2018

Efficient nonparametric $n$-body force fields from machine learning

We provide a definition and explicit expressions for $n$-body Gaussian Process (GP) kernels which can learn any interatomic interaction occurring in a physical system, up to $n$-body contributions, for any value of $n$. The series is complete, as it can be shown that the "universal approximator" squared exponential kernel can be written as a sum of $n$-body kernels. These recipes enable the choice of optimally efficient force models for each target system, as confirmed by extensive testing on various materials. We furthermore describe how the $n$-body kernels can be "mapped" on equivalent representations that provide database-size-independent predictions and are thus crucially more efficient. We explicitly carry out this mapping procedure for the first non-trivial (3-body) kernel of the series, and show that this reproduces the GP-predicted forces with $\text{meV/} Å$ accuracy while being orders of magnitude faster. These results open the way to using novel force models (here named "M-FFs") that are computationally as fast as their corresponding standard parametrised $n$-body force fields, while retaining the nonparametric character, the ease of training and validation, and the accuracy of the best recently proposed machine learning potentials.

physics.comp-ph↗

arXiv2017

Accurate Interatomic Force Fields via Machine Learning with Covariant Kernels

We present a novel scheme to accurately predict atomic forces as vector quantities, rather than sets of scalar components, by Gaussian Process (GP) Regression. This is based on matrix-valued kernel functions, on which we impose the requirements that the predicted force rotates with the target configuration and is independent of any rotations applied to the configuration database entries. We show that such covariant GP kernels can be obtained by integration over the elements of the rotation group SO(d) for the relevant dimensionality d. Remarkably, in specific cases the integration can be carried out analytically and yields a conservative force field that can be recast into a pair interaction form. Finally, we show that restricting the integration to a summation over the elements of a finite point group relevant to the target system is sufficient to recover an accurate GP. The accuracy of our kernels in predicting quantum-mechanical forces in real materials is investigated by tests on pure and defective Ni, Fe and Si crystalline systems.

physics.chem-ph↗

arXiv1999

Thermal Contraction and Disordering of the Al(110) Surface

Al(110) has been studied for temperatures up to 900 K via ensemble density-functional molecular dynamics. The strong anharmonicity displayed by this surface results in a negative coefficient of thermal expansion, where the first interlayer distance decreases with increasing temperature. Very shallow channels of oscillation for the second-layer atoms in the direction perpendicular to the surface support this anomalous contraction, and provide a novel mechanism for the formation of adatom-vacancy pairs, preliminary to the disordering and premelting transition. Such characteristic behavior originates in the free-electron-gas bonding at a loosely packed surface.

cond-mat.mtrl-sci↗

arXiv1997

Amorphous indium phosphide from first principles

We report detailed and extensive first-principles molecular-dynamics (MD) simulations of the structure and electronic properties of amorphous InP produced by rapid quenching from the liquid. The structure of the material is found to be strongly ordered chemically, even though there is a significant number of coordination defects and despite the presence of odd-membered rings. We find, as a consequence, that there exists ``wrong bonds'' in the system, in an amount of about 8%; these result from the presence of coordination defects, not of local composition fluctuations, as has been conjectured. The system, in fact, is found to be over-coordinated, which might be the reason for the observed higher density of a-InP compared to c-InP. We have also investigated the possibility of pressure-amorphizing InP. Our calculations indicate that the cost of a transformation of the compressed zinc-blende crystal into an amorphous phase is so large that it is very unlikely that it would take place.

cond-mat.mtrl-sci↗