arXiv subjects

Giovanni Marini

Publications and source records attributed to Giovanni Marini.

At least 19 recordsLinked to original sources

arXiv2026

Doping tunable charge density waves in misfit layer compounds

The ability to tune charge density waves (CDWs) through external control knobs, such as doping, pressure or strain is crucial for exploring the phase diagram of two dimensional (2D) or quasi-2D materials. Yet, controlling CDWs critical temperature and ordering vector remains a challenge for current experimental techniques. In this work, we establish misfit layer compound heterostructures as a reliable platform to manipulate CDWs in transition metal dichalcogenides. By combining ab initio calculations with low-temperature scanning tunneling microscopy, we show how to achieve doping tunable control over NbSe2 CDW by chemically alloying in the rocksalt subunit. Crucially, we prove that tuning the La Pb ratio in the misfit family (LaxPb1xSe)1.14(NbSe2)2 enables stabilization of different CDW orders, such as 2x2 or 3x3 patterns, and even coexisting phases. This work paves the way for engineering transition metal dichalcogenides with tailored charge density waves within misfit heterostructures.

cond-mat.mtrl-sci↗

arXiv2026

Ab Initio Spinor Kadanoff-Baym Approach to Nonequilibrium Electron, Phonon and Magnon Dynamics in Itinerant Ferromagnets

This work introduces a theoretical framework based on the Kadanoff-Baym equations in spinor space to study ultrafast magnetization dynamics in itinerant ferromagnetic systems from first principles. By incorporating spin-orbit coupling into the ab initio Hamiltonian and generalizing the self-energies to include terms beyond the charge sector, I derive scattering integrals within the Markov approximation and quasiparticle renormalizations for electrons and phonons in the presence of spin-dependent effective interactions within a many-body perturbation theory approach. I explicitly discuss how magnons emerge in this framework, and derive, through suitable approximations, a close and tractable set of equations for coupled electron,phonon and magnon dynamics that can be solved from first principles. I discuss the equations of motion within a minimal ferromagnetic model, where the coupled equations are solved numerically. This approach allows to treat coherent and incoherent magnetic dynamics on an equal footing, paving the way for a first principles understanding of ultrafast magnetic dynamics and demagnetization, and opening to a truly predictive theory of femtomagnetism in periodic systems.

cond-mat.mtrl-sci↗

arXiv2026

Tuning the Charge Transfer of Transition Metal Dichalcogenides via Misfit Layer Compounds

Misfit layer compounds (MLCs) are a versatile platform for exploring the electronic phase diagram of two dimensional (2D) materials beyond the limits of conventional gating techniques. This work demonstrates the precise tunability of electron doping in NbSe2 monolayers through chemical alloying within the rocksalt layer of (LaxPb1xSe)1.14(NbSe2)2 heterostructures. By combining first principles density functional theory (DFT) calculations with angle resolved photoemission spectroscopy (ARPES), we prove that the rocksalt unit acts as an universal electron donor. We show that varying the La Pb ratio results in a rigid Fermi level shift, still preserving the NbSe2 electronic structure. Crucially, photon energy dependent ARPES confirms that the NbSe2 layers nearly maintain their intrinsic 2D character and orbital identity within the three dimensional misfit. This study establishes MLCs as a reliable platform for engineering emergent states in 2D transition metal dichalcogenides through precise stoichiometric control.

cond-mat.mtrl-sci↗

arXiv2026

Disorder-Driven Enhancement of Coulomb Repulsion Governs The Superconducting Dome in Ionic-Liquid-Gated Quasi-2D Materials

The superconducting dome in the Tc versus doping phase diagram, found in cuprates, nickelates, twisted bilayer graphene, and transition metal dichalcogenides, is often considered a signature of unconventional pairing. Identifying the underlying mechanisms of any of these phase diagrams and developing a reliable theoretical understanding of it remains a critical challenge. Here we demonstrate that, in ionic-liquid-gated quasi-2D materials, the disordered ionic potential from the frozen ionic liquid drives the system close to Anderson transition. In this regime, quenched charge fluctuations and reduced screening markedly enhance repulsive Coulomb interactions, suppressing Tc and naturally leading to the formation of a superconducting dome. By integrating a many-body approach including disorder with first-principles calculations, we obtain the phase diagrams and tunneling spectra of gated few-layers transition metal dichalchogenides in robust quantitative agreement with experiments. Our findings establish that disorder-driven enhancement of Coulomb repulsion is a fundamental feature of ionic-liquid-gated quasi-2D materials at high bias.

cond-mat.supr-con↗

arXiv2025

Photoinduced phase heterogeneity and charge localization in SnSe

Time-resolved multi-terahertz (THz) spectroscopy is used to observe pump fluence-dependent dynamics in the optical conductivity of photoexcited tin selenide (SnSe) over an ultrabroadband spectral range of 0.5 - 11 THz at fluences from 0.1 - 7.5 mJ/cm$^2$. A free carrier Drude spectrum is observed at pump fluences below 3 mJ/cm$^2$, with optical phonons well described by the equilibrium Pnma structural phase. With increasing fluence, a suppression of the DC photoconductivity is observed, indicating an interruption of long range transport due to phase disorder. Concomitantly, the optical phonons exhibit features that can no longer be explained by a pure Pnma phase, with a frequency shift and narrowing of the $B^2_{1u}$ mode and a new mode appearing at $\sim$3.0 THz consistent with a transition to a higher-symmetry structure. At an intermediate fluence of 3.1 mJ/cm$^2$, a high frequency Lorentzian component consistent with phase heterogeneity appears that rapidly redshifts after 2 ps and whose amplitude exponentially decays on a 90 ps time scale. Our experimental measurements and theoretical calculations provide evidence for a non-thermal, photo-induced nucleation of higher symmetry, semi-metallic phase domains in SnSe appearing within 200 fs.

cond-mat.mtrl-sci↗

arXiv2025

Nonequilibrium Photocarrier and Phonon Dynamics from First Principles: a Unified Treatment of Carrier-Carrier, Carrier-Phonon, and Phonon-Phonon Scattering

We develop a first-principles many-body framework to describe the dynamics of photocarriers and phonons in semiconductors following ultrafast excitation. Our approach incorporates explicit ab initio light-matter coupling and first-principles collision integrals for carrier-carrier, carrier-phonon, and phonon-phonon scattering. It also yields time-dependent quasiparticle and phonon frequency renormalizations, along with light-induced coherent atomic motion. The equations of motion are solved in a maximally localized Wannier basis, ensuring gauge-consistent scattering integrals and ultradense momentum sampling, thereby enabling direct comparison with pump-probe experiments. The method can be coupled to constrained density-functional theory to access light-induced structural phase transitions at longer times after the light pulse. We showcase the capabilities and predictive power of this framework on MoS$_2$ and h-BN monolayers. For MoS$_2$, we resolve photoinduced renormalizations of electronic and lattice properties, ultrafast carrier relaxation, hot-phonon dynamics, and displacive coherent atomic motion. Including carrier-carrier scattering is crucial to obtain realistic photocarrier equilibration times, while omitting phonon-phonon scattering leads to incorrect long-time lattice thermalization and a factor of two larger A$_{1g}$ coherent phonon damping time. For h-BN, we quantify photoinduced changes in the electronic, optical, and lattice responses in quasi-equilibrium, demonstrating a fluence-dependent enhancement of screening and melting of excitonic features.

cond-mat.mtrl-sci↗

arXiv2025

Nonthermal magnetization pathways in photoexcited semiconductors

The stabilization of long-range magnetic order in nominally non-magnetic semi-conductors using femtosecond light pulses is an exciting yet experimentally challenging goal. Theoretical studies indicate that certain non-magnetic semi-conductors can exhibit transient magnetic instabilities following above-gap laser excitation, but the dynamical pathways leading to these states remain largely unexplored. In this work, I introduce a minimal real-time spin-orbital model and identify the fundamental microscopic mechanisms that enable the emergence of a transient magnetic order. I then discuss the relevance of these findings for real materials employing a phenomenological time-dependent Ginzburg-Landau model. Finally, I analyze the strengths and limitations of current first-principles methodologies for investigating dynamically induced broken-symmetry states in the light of the present results.

cond-mat.mtrl-sci↗

arXiv2024

Wannier interpolation of reciprocal-space periodic and non-periodic matrix elements in the optimally smooth subspace

Maximally localized Wannier functions use the gauge freedom of Bloch wavefunctions to define the optimally smooth subspace with matrix elements that depend smoothly on crystal momentum. The associated Wannier functions are real-space localized, a feature often used to Fourier interpolate periodic observables in reciprocal space on ultradense momentum grids. However, Fourier interpolation cannot handle non-periodic quantities in reciprocal space, such as the oscillator strength matrix elements, which are crucial for the evaluation of optical properties. We show that a direct multidimensional interpolation in the optimally smooth subspace yields comparable accuracy with respect to Fourier interpolation at a similar or lower computational cost. This approach can also interpolate and extrapolate non-periodic observables, enabling the calculation of optical properties on ultradense momentum grids. Finally, we underline that direct interpolation in the optimally smooth subspace can be employed for periodic and non-periodic tensors of any order without any information on the position of the Wannier centers in real space.

cond-mat.mtrl-sci↗

arXiv2024

Anomalous amplitude mode dynamics below the expected charge-density-wave transition in 1$T$-VSe$_2$

A charge-density-wave (CDW) is characterized by a dynamical order parameter consisting of a time-dependent amplitude and phase, which manifest as optically-active collective modes of the CDW phase. Studying the behaviour of such collective modes in the time-domain, and their coupling with electronic and lattice order, provides important insight into the underlying mechanisms behind CDW formation. In this work, we report on femtosecond broadband transient reflectivity experiments on bulk 1$T$-VSe$_2$ using near-infrared excitation. At low temperature, we observe coherent oscillations associated with the CDW amplitude mode and phonons of the distorted lattice. Across the expected transition temperature at 110 K, we confirm signatures of a rearrangement of the electronic structure evident in the quasiparticle dynamics. However, we find that the amplitude mode instead softens to zero frequency at 80 K, possibly indicating an additional phase transition at this temperature. In addition, we demonstrate photoinduced CDW melting, associated with a collapse of the electronic and lattice order, which occurs at moderate excitation densities, consistent with a dominant electron-phonon CDW mechanism.

cond-mat.str-el↗

arXiv2024

Anisotropic sub-band splitting mechanisms in strained HgTe: a first principles study

Mercury telluride is a canonical material for realizing topological phases, yet a full understanding of its electronic structure remains challenging due to subtle competing effects. Using first-principles calculations and $\mathbf{k}\cdot\mathbf{p}$ modelling, we study its topological phase diagram under strain. We show that linearly $k$-dependent higher-order $C_4$ strain terms are important for capturing the correct low-energy behaviour. These terms lead to a nontrivial $k$-dependence of the sub-band splitting arising from the interplay of strain and bulk inversion asymmetry. This explains the camel-back feature in the tensile regime and supports the emergence of a Weyl semimetal phase under compressive strain.

cond-mat.mtrl-sci↗

arXiv2024

Ultrafast creation of a light induced semimetallic state in strongly excited 1T-TiSe$_2$

Screening, a ubiquitous phenomenon associated with the shielding of electric fields by surrounding charges, has been widely adopted as a means to modify a material's properties. While so far most studies have relied on static changes of screening through doping or gating, here we demonstrate that screening can also drive the onset of distinct quantum states on the ultrafast timescale. By using time and angle-resolved photoemission spectroscopy we show that intense optical excitation can drive 1T-TiSe$_2$, a prototypical charge density wave material, almost instantly from a gapped into a semimetallic state. By systematically comparing changes in bandstructure over time and excitation strength with theoretical calculations we find that the appearance of this state is likely caused by a dramatic reduction of the screening length. In summary, this work showcases how optical excitation enables the screening driven design of a non-equilibrium semimetallic phase in TiSe$_2$, possibly providing a general pathway into highly screened phases in other strongly correlated materials.

cond-mat.mes-hall↗

arXiv2024

NbSe$_{2}$'s charge density wave collapse in the (LaSe)$_{1.14}$(NbSe$_{2}$)$_{2}$ misfit layer compound

Misfit layer compounds, heterostructures composed by a regular alternating stacking of rocksalt monochalcogenides bilayers and few-layer transition metal dichalchogenides, are an emergent platform to investigate highly doped transition metal dichalcogenides. Among them, (LaSe)$_{1.14}$(NbSe$_2$)$_2$ displays Ising superconductivity, while the presence of a charge density wave (CDW) in the material is still under debate. Here, by using polarized Raman spectroscopy and first-principles calculations, we show that NbSe$_2$ undergoes a doping-driven collapse of the CDW ordering within the misfit, and no signature of the CDW is detected down to 8~K. We provide a complete experimental and theoretical description of the lattice dynamics of this misfit compound. We show that the vibrational properties are obtained from those of the two subunits, namely the LaSe unit and the NbSe$_2$ bilayer, in the presence of a suitable field-effect doping, and then highlight the 2D nature of the lattice dynamics of NbSe$_2$ within the (LaSe)$_{1.14}$(NbSe$_2$)$_2$ 3D structure.

cond-mat.mtrl-sci↗

arXiv2024

First-order rhombohedral to cubic phase transition in photoexcited GeTe

Photoexcited GeTe undergoes a non-thermal phase transition from a rhombohedral to a rocksalt crystalline phase. The microscopic mechanism and the nature of the transition are unclear. By using constrained density functional perturbation theory and by accounting for quantum anharmonicity within the stochastic self-consistent harmonic approximation, we show that the non-thermal phase transition is strongly first order and does not involve phonon softening, at odd with the thermal one. The transition is driven by the closure of the single particle gap in the photoexcited rhombohedral phase. Finally, we show that ultrafast X-ray diffraction data are consistent with a coexistence of the two phases, as expected in a first order transition. Our results are relevant for the understanding of phase transitions and bonding in phase change materials.

cond-mat.mtrl-sci↗

arXiv2024

Optical absorption and photoluminescence of single layer boron nitride from a first principles cumulant approach

The photoluminescence spectrum of a single-layer boron nitride remains elusive, marked by enigmatic satellites that hint at a significant but unidentified exciton-phonon coupling.Here, by employing a first principles approach based on the many-body cumulant expansion of the charge response, we calculate the optical absorption and photoluminescence of a single layer boron nitride. We identify the specific exciton-phonon scattering channels and unravel their impact on the optical absorption and photoluminescence spectra thereby providing an interpretation of the experimental features. Finally, we show that, even in a strongly polar material such as h-BN monolayer, the electron-hole interaction responsible for the excitonic effect results in the cancellation of the Frölich interaction at small phonon momenta. This effect is captured only if the invariance of the exciton-phonon matrix elements under unitary transformations in the Bloch functions manifold is preserved in the calculation.

cond-mat.mtrl-sci↗

arXiv2023

Light-Induced Nonthermal Phase Transition to the Topological Crystalline Insulator State in SnSe

Femtosecond pulses have been used to reveal hidden broken symmetry states and induce transitions to metastable states. However, these states are mostly transient and disappear after laser removal. Photoinduced phase transitions towards crystalline metastable states with a change of topological order are rare and difficult to predict and realize experimentally. Here, by using constrained density functional perturbation theory and accounting for light-induced quantum anharmonicity, we show that ultra-fast lasers can permanently transform the topologically-trivial orthorhombic structure of SnSe into the topological crystalline insulating rocksalt phase via a first-order non-thermal phase transition. We describe the reaction path and evaluate the critical fluence and the possible decay channels after photoexcitation. Our simulations of the photoexcited structural and vibrational properties are in excellent agreement with recent pump-probe data in the intermediate fluence regime below the transition with an error on the curvature of the quantum free energy of the photoexcited state that is smaller than 2%.

cond-mat.mtrl-sci↗

arXiv2023

Electron-phonon driven charge density wave in CuTe

The compound CuTe (vulcanite) undergoes a quasi one dimensional charge density wave (CDW) at $T< T_{\mathrm{CDW}}=335$ K with a $5\times1\times2$ periodicity. The mechanism at its origin is debated. Several theoretical works claimed that semilocal functionals are unable to describe its occurrence and ascribed its formation only to strong electron-electron interaction. Moreover, the possible role of quantum anharmonicity has not been addressed. Here, by performing quantum anharmonic calculations, we show that semilocal functionals correctly describe the occurrence of a CDW in CuTe if ultradense electron momentum grids allowing for small electronic temperatures are used. The distortion is driven by the perfect nesting among 1D Fermi surface sheets extending in the $k_y$ direction. Quantum anharmonic effects are important and tend to suppress both the distortion and $T_{\mathrm{CDW}}$. The quantum anharmonic structural minimization of the CDW phase in the generalized gradient approximation leads, however, to distorted Te-Te bond lengths in the low temperature phase that are $21\%$ of the experimental ones at $T=20$ K. This suggests that, even if the electron-electron interaction is not crucial for the mechanism of CDW formation, it is relevant to accurately describe the structural data for the low-T phase. We assess the effect of correlation on the CDW by using the DFT+U+V approximation with parameters calculated from first principles. We find that correlation enhances the Te-Te distortion, T$_{CDW}$ and the total energy gain by the distortion.

cond-mat.mtrl-sci↗

arXiv2023

Misfit layer compounds as ultra-tunable field effect transistors: from charge transfer control to emergent superconductivity

Misfit layer compounds are heterostructures composed of rocksalt units stacked with few layers transition metal dichalcogenides. They host Ising superconductivity, charge density waves and good thermoelectricity. The design of misfits emergent properties is, however, hindered by the lack of a global understanding of the electronic transfer among the constituents. Here, by performing first principles calculations, we unveil the mechanism controlling the charge transfer and demonstrate that rocksalt units are always donor and dichalcogenides acceptors. We show that misfits behave as a periodic arrangement of ultra-tunable field effect transistors where a charging as large as 6\times10^{14} e^-cm^{-2} can be reached and controlled efficiently by the La-Pb alloying in the rocksalt. Finally, we identify a strategy to design emergent superconductivity and demonstrate its applicability in (LaSe)_{1.27}(SnSe_2)_2. Our work paves the way to the design synthesis of misfit compounds with tailored physical properties.

cond-mat.mtrl-sci↗

arXiv2023

EPIq : an open-source software for the calculation of electron-phonon interaction related properties

EPIq (Electron-Phonon wannier Interpolation over k and q-points) is an open-source software for the calculation of electron-phonon interaction related properties from first principles.Acting as a post-processing tool for a density-functional perturbation theory code ( Quantum ESPRESSO ) and wannier90, EPIq exploits the localization of the deformation potential in the Wannier function basis and the stationary properties of a force-constant functional with respect to the first-order perturbation of the electronic charge density to calculate many electron-phonon related properties with high accuracy and free from convergence issues related to Brillouin zone sampling. EPIq features includes: the adiabatic and non-adiabatic phonon dispersion, superconducting properties (including the superconducting band gap in the Migdal-Eliashberg formulation), double-resonant Raman spectra and lifetime of excited carriers. The possibility to customize most of its input makes EPIq a versatile and interoperable tool. Particularly relevant is the interaction with the Stochastic Self-Consistent Harmonic Approximation (SSCHA) allowing anharmonic effects to be included in the calculation of electron-properties. The scalability offered by the Wannier representation combined with a straightforward workflow and easy-to-read input and output files make EPIq accessible to the wide condensed matter and material science communities.

cond-mat.mtrl-sci↗