arXiv subjects

A. Molina-Sánchez

Publications and source records attributed to A. Molina-Sánchez.

15 recordsLinked to original sources

arXiv2023

Beyond spin models in orbitally-degenerate open-shell nanographenes

The study of open-shell nanographenes has relied on a paradigm where spins are the only low-energy degrees of freedom. Here we show that some nanographenes can host low-energy excitations that include strongly coupled spin and orbital degrees of freedom. The key ingredient is the existence of orbital degeneracy, as a consequence of leaving the benzenoid/half-filling scenario. We analyze the case of nitrogen-doped triangulenes, using both density-functional theory and Hubbard model multiconfigurational and random-phase approximation calculations. We find a rich interplay between orbital and spin degrees of freedom that confirms the need to go beyond the spin-only paradigm, opening a new venue in this field of research.

cond-mat.mes-hall↗

arXiv2023

Broken-symmetry magnetic phases in two-dimensional triangulene crystals

We provide a comprehensive theory of magnetic phases in two-dimensional triangulene crystals, using both Hubbard model and density functional theory (DFT) calculations. We consider centrosymmetric and non-centrosymmetric triangulene crystals. In all cases, DFT and mean-field Hubbard model predict the emergence of broken-symmetry antiferromagnetic (ferrimagnetic) phases for the centrosymmetric (non-centrosymmetric) crystals. This includes the special case of the [4,4]triangulene crystal, whose non-interacting energy bands feature a gap with flat valence and conduction bands. We show how the lack of contrast between the local density of states of these bands, recently measured via scanning tunneling spectroscopy, is a natural consequence of a broken-symmetry Néel state that blocks intermolecular hybridization. Using random phase approximation, we also compute the spin wave spectrum of these crystals, including the recently synthesized [4,4]triangulene crystal. The results are in excellent agreement with the predictions of a Heisenberg spin model derived from multi-configuration calculations for the unit cell. We conclude that experimental results are compatible with an antiferromagnetically ordered phase where each triangulene retains the spin predicted for the isolated species.

cond-mat.mes-hall↗

arXiv2021

Decoding the DC and optical conductivities of disordered MoS$_{2}$ films: an inverse problem

To calculate the conductivity of a material having full knowledge of its composition is a reasonably simple task. To do the same in reverse, i.e., to find information about the composition of a device from its conductivity response alone, is very challenging and even more so in the presence of disorder. An inversion methodology capable of decoding the information contained in the conductivity response of disordered structures has been recently proposed but despite claims of generality and robustness, the method has only been used with 2D systems possessing relatively simple electronic structures. Here we put these claims to the test and generalise the inversion method to the case of monolayer MoS$_2$, a material whose electronic structure is far more complex and elaborate. Starting from the spectral function that describes the DC conductivity of a disordered sample of a single layered MoS$_2$ containing a small concentration of randomly dispersed vacancies, we are able to invert the signal and find the exact composition of defects with an impressive degree of accuracy. Remarkably, equally accurate results are obtained with the optical conductivity. This is indicative of a methodology that is indeed suitable to extract composition information from different 2D materials, regardless of their electronic structure complexity. Calculated conductivity results were used as a proxy for their experimental counterpart and were obtained with an efficient quantum transport code (KITE) based on a real-space multi-orbital tight-binding model with parameters generated by density functional theory.

cond-mat.dis-nn↗

arXiv2021

Phonons in MoSe2/WSe2 van der Waals heterobilayer

We report first-principles calculations of the structural and vibrational properties of the synthesized two-dimensional van der Waals heterostructures formed by single-layers dichalcogenides MoSe2 and WSe2. We show that, when combining these systems in a periodic two-dimensional heterostructures, the intrinsic phonon characteristics of the free-standing constituents are to a large extent preserved but, furthermore, exhibit shear and breathing phonon modes that are not present in the individual building blocks. These peculiar modes depend strongly on the weak vdW forces and has a great contibution to the thermal properties of the layered materials. Besides these features, the departure of flexural modes of heterobilayer from the ones of its monolayer parents are also found.

cond-mat.mtrl-sci↗

arXiv2021

Electronic and magnetic properties of VOCl/FeOCl antiferromagnetic heterobilayers

We study the electronic properties of the heterobilayer of vanadium and iron oxychlorides, VOCl and FeOCl, two layered air stable van der Waals insulating oxides with different types of antiferromagnetic order in bulk: VOCl monolayers are ferromagnetic (FM) whereas the FeOCl monolayers are antiferromagnetic (AF). We use density functional theory (DFT) calculations, with Hubbard correction that is found to be needed to describe correctly the insulating nature of these compounds. We compute the magnetic anisotropy and propose a spin model Hamiltonian. Our calculations show that interlayer coupling in weak and ferromagnetic so that magnetic order of the monolayers is preserved in the heterobilayers providing thereby a van der Waals heterostructure that combines two monolayers with different magnetic order. Interlayer exchange should lead both to exchange bias and to the emergence of hybrid collective modes that that combine FM and AF magnons. The energy band of the heterobilayer show a type II band alignment, and feature spin-splitting of the states of the AF layer due to the breaking of the inversion symmetry.

cond-mat.mes-hall↗

arXiv2021

Out-of-plane emission of trions in monolayer WSe2 revealed by whispering gallery modes of dielectric microresonators

The manipulation of light emitted by two-dimensional semiconductors grounds forthcoming technologies in the field of on-chip communications. However, these technologies require from the so elusive out-of-plane photon sources to achieve an efficient coupling of radiated light into planar devices. Here we propose a versatile spectroscopic method that enables the identification of the out-of-plane component of dipoles. The method is based on the selective coupling of light emitted by in-plane and out-of-plane dipoles to the whispering gallery modes of spherical dielectric microresonators, in close contact to them. We have applied this method to demonstrate the existence of dipoles with an out-of-plane orientation in monolayer WSe2 at room temperature. Micro-photoluminescent measurements, numerical simulations based on finite element methods, and ab-initio calculations have identified trions as the source responsible for this out-of-plane emission, opening new routes for realizing on-chip integrated systems with applications in information processing and quantum communications.

physics.optics↗

arXiv2020

Interplay between spin proximity effect and charge-dependent exciton dynamics in MoSe$_2$ / CrBr$_3$ van der Waals heterostructures

Semiconducting ferromagnet-nonmagnet interfaces in van der Waals heterostructures present a unique opportunity to investigate magnetic proximity interactions dependent upon a multitude of phenomena including valley and layer pseudospins, moiré periodicity, or exceptionally strong Coulomb binding. Here, we report a charge-state dependency of the magnetic proximity effects between MoSe$_2$ and CrBr$_3$ in photoluminescence, whereby the valley polarization of the MoSe$_2$ trion state conforms closely to the local CrBr$_3$ magnetization, while the neutral exciton state remains insensitive to the ferromagnet. We attribute this to spin-dependent interlayer charge transfer occurring on timescales between the exciton and trion radiative lifetimes. Going further, we uncover by both the magneto-optical Kerr effect and photoluminescence a domain-like spatial topography of contrasting valley polarization, which we infer to be labyrinthine or otherwise highly intricate, with features smaller than 400 nm corresponding to our optical resolution. Our findings offer a unique insight into the interplay between short-lived valley excitons and spin-dependent interlayer tunnelling, while also highlighting MoSe$_2$ as a promising candidate to optically interface with exotic spin textures in van der Waals structures.

cond-mat.mes-hall↗

arXiv2019

Strongly coupled coherent phonons in single-layer MoS$_2$

We present a transient absorption setup combining broadband detection over the visible-UV range with high temporal resolution ($\sim$20fs) which is ideally suited to trigger and detect vibrational coherences in different classes of materials. We generate and detect coherent phonons (CPs) in single layer (1L) MoS$_2$, as a representative semiconducting 1L-transition metal dichalcogenide (TMD), where the confined dynamical interaction between excitons and phonons is unexplored. The coherent oscillatory motion of the out-of-plane $A'_{1}$ phonons, triggered by the ultrashort laser pulses, dynamically modulates the excitonic resonances on a timescale of few tens fs. We observe an enhancement by almost two orders of magnitude of the CP amplitude when detected in resonance with the C exciton peak, combined with a resonant enhancement of CP generation efficiency. Ab initio calculations of the change in 1L-MoS$_2$ band structure induced by the $A'_{1}$ phonon displacement confirm a strong coupling with the C exciton. The resonant behavior of the CP amplitude follows the same spectral profile of the calculated Raman susceptibility tensor. This demonstrates that CP excitation in 1L-MoS$_2$ can be described as a Raman-like scattering process. These results explain the CP generation process in 1L-TMDs, paving the way for coherent all-optical control of excitons in layered materials in the THz frequency range.

cond-mat.mtrl-sci↗

arXiv2019

Magneto-optical response of chromium trihalide monolayers: chemical trends

Chromium trihalides (CrI$_3$, CrBr$_3$ and CrCl$_3$) form a prominent family of isostructural insulating layered materials in which ferromagnetic order has been observed down to the monolayer. Here we provide a comprehensive computational study of magneto-optical properties that are used as probes for the monolayer ferromagnetic order: magnetic circular dichroism and magneto-optic Kerr effect. Using a combination of density functional and Bethe-Salpeter theories, we calculate both the optical absorption and the magneto-optical Kerr angle spectra, including both excitonic effects and spinorial wave functions. We compare the magneto-optical response of the chromium trihalides series and we find that its strength is governed by the spin-orbit coupling of the ligand atoms (I, Br, Cl).

cond-mat.mtrl-sci↗

arXiv2019

Many-body perturbation theory calculations using the yambo code

yambo is an open source project aimed at studying excited state properties of condensed matter systems from first principles using many-body methods. As input, yambo requires ground state electronic structure data as computed by density functional theory codes such as quantum-espresso and abinit. yambo's capabilities include the calculation of linear response quantities (both independent-particle and including electron-hole interactions), quasi-particle corrections based on the GW formalism, optical absorption, and other spectroscopic quantities. Here we describe recent developments ranging from the inclusion of important but oft-neglected physical effects such as electron-phonon interactions to the implementation of a real-time propagation scheme for simulating linear and non-linear optical properties. Improvements to numerical algorithms and the user interface are outlined. Particular emphasis is given to the new and efficient parallel structure that makes it possible to exploit modern high performance computing architectures. Finally, we demonstrate the possibility to automate workflows by interfacing with the yambopy and AiiDA software tools.

cond-mat.mtrl-sci↗

arXiv2018

Inter- and intra-layer excitons in MoS$_2$/WS$_2$ and MoSe$_2$/WSe$_2$ heterobilayers

Accurately described excitonic properties of transition metal dichalcogenide heterobilayers (HBLs) are crucial to comprehend the optical response and the charge carrier dynamics of them. Excitons in multilayer systems posses inter or intralayer character whose spectral positions depend on their binding energy and the band alignment of the constituent single-layers. In this study, we report the electronic structure and the absorption spectra of MoS$_2$/WS$_2$ and MoSe$_2$/WSe$_2$ HBLs from first-principles calculations. We explore the spectral positions, binding energies and the origins of inter and intralayer excitons and compare our results with experimental observations. The absorption spectra of the systems are obtained by solving the Bethe-Salpeter equation on top of a G$_0$W$_0$ calculation which corrects the independent particle eigenvalues obtained from density functional theory calculations. Our calculations reveal that the lowest energy exciton in both HBLs possesses interlayer character which is decisive regarding their possible device applications. Due to the spatially separated nature of the charge carriers, the binding energy of inter-layer excitons might be expected to be considerably smaller than that of intra-layer ones. However, according to our calculations the binding energy of lowest energy interlayer excitons is only $\sim$ 20\% lower due to the weaker screening of the Coulomb interaction between layers of the HBLs. Therefore, it can be deduced that the spectral positions of the interlayer excitons with respect to intralayer ones are mostly determined by the band offset of the constituent single-layers. By comparing oscillator strengths and thermal occupation factors, we show that in luminescence at low temperature, the interlayer exciton peak becomes dominant, while in absorption it is almost invisible.

cond-mat.mtrl-sci↗

arXiv2013

Screening of electron-phonon coupling in graphene on Ir(111)

The phonon dispersion of graphene on Ir(111) has been determined by means of angle-resolved inelastic electron scattering and density functional calculations. Kohn anomalies of the highest optical-phonon branches are observed at the $Γ$ and K point of the surface Brillouin zone. At K the Kohn anomaly is weaker than observed from pristine graphene and graphite. This observation is rationalized in terms of a decrease of the electron-phonon coupling due to screening of graphene electron correlations by the metal substrate.

cond-mat.mtrl-sci↗

arXiv2013

LDA+U and tight-binding electronic structure of InN nanowires

In this paper we employ a combined {\it ab initio} and tight-binding approach to obtain the electronic and optical properties of hydrogenated InN nanowires. We first discuss InN band structure for the wurtzite structure calculated at the LDA+U level and use this information to extract the parameters needed for an empirical tight-binging implementation. These parameters are then employed to calculate the electronic and optical properties of InN nanowires in a diameter range that would not be affordable by {\it ab initio} techniques. The reliability of the large nanowires results is assessed by explicitly comparing the electronic structure of a small diameter wire studied both at LDA+U and tight-binding level.

cond-mat.mes-hall↗

arXiv2012

Contribution of the buffer layer to the Raman spectrum of epitaxial graphene on SiC(0001)

We report a Raman study of the so-called buffer layer with $(6\sqrt3\times6\sqrt3)R30^{\circ}$ periodicity which forms the intrinsic interface structure between epitaxial graphene and SiC(0001). We show that this interface structure leads to a nonvanishing signal in the Raman spectrum at frequencies in the range of the D- and G-band of graphene and discuss its shape and intensity. Ab-initio phonon calculations reveal that these features can be attributed to the vibrational density of states of the buffer-layer.

cond-mat.mtrl-sci↗

arXiv2011

Phonons in single and few-layer MoS2 and WS2

We report ab-initio calculations of the phonon dispersion relations of the single-layer and bulk dichalcogenides MoS2 and WS2. We explore in detail the behavior of the Raman active modes, A1g and E2g as a function of the number of layers. In agreement with recent Raman spectroscopy measurements [C. Lee et. al., ACS Nano Vol. 4, 2695 (2010)] we find that the A1g mode increases in frequency with increasing layer number while the E2g mode decreases. We explain this decrease by an enhancement of the dielectric screening of the long-range Coulomb interaction between the effective charges with growing number of layers. This decrease in the long-range part over-compensates the increase of the short-range interaction due to the weak inter-layer interaction.

cond-mat.mtrl-sci↗