arXiv subjects

Pedro Miguel M. C. de Melo

Publications and source records attributed to Pedro Miguel M. C. de Melo.

4 recordsLinked to original sources

arXiv2022

High-throughput analysis of Fröhlich-type polaron models

The electronic structure of condensed matter can be significantly affected by the electron-phonon interaction, leading to important phenomena such as electrical resistance, superconductivity or the formation of polarons. This interaction is often neglected in band structure calculations but can have a strong impact on band gaps or optical spectra. Commonly used frameworks for electron-phonon energy corrections are the Allen-Heine-Cardona theory and the Fröhlich model. While the latter shows qualitative agreement with experiment for many polar materials, its simplicity should bring hard limits to its applicability in real materials. Improvements can be made by introducing a generalized version of the model, which considers anisotropic and degenerate electronic bands, and multiple phonon branches. In this work, we search for trends and outliers on over a thousand materials in existing databases of phonon and electron band structures. We use our results to identify the limits of applicability of the standard Frölich model by comparing to the generalized version, and by testing its basic hypothesis of a large radius for the polaronic wavefunction and the corresponding atomic displacement cloud. Among our extended set of materials, most exhibit large polaron behavior as well as validity of the perturbative treatment. For the valence band, there is also a significant fraction of the materials for which the perturbative treatment cannot be applied and/or for which the size of the self-trapping region is close to the atomic repetition distance. We find a large variety of behaviors, and employ much more accurate, fully ab initio Allen-Heine-Cardona calculations to understand extreme cases, where the Fröhlich model should fail and unusually large zero-point renormalization energies occur.

cond-mat.mtrl-sci↗

arXiv2020

Optical Signatures of Defect Centres in Transition Metal Dichalcogenide Monolayers

Even the best quality 2D materials have non-negligible concentrations of vacancies and impurities. It is critical to understand and quantify how defects change intrinsic properties, and use this knowledge to generate functionality. This challenge can be addressed by employing many-body perturbation theory to obtain the optical absorption spectra of defected transition metal dichalcogenides. Herein metal vacancies, which are largely unreported, show a larger set of polarized exitons than chalcogenide vacancies, introducing localized excitons in the sub-optical-gap region, whose wave functions and spectra make them good candidates as quantum emitters. Despite the strong interaction with substitutional defects, the spin texture and pristine exciton energies are preserved, enabling grafting and patterning in optical detectors, as the full optical-gap region remains available. A redistribution of excitonic weight between the A and B excitons is visible in both cases and may allow the quantification of the defect concentration. This work establishes excitonic signatures to characterize defects in 2D materials and highlights vacancies as qubit candidates for quantum computing.

cond-mat.other↗

arXiv2019

Spin States Protected from Intrinsic Electron-Phonon-Coupling Reaching 100 ns Lifetime at Room Temperature in MoSe$_2$

We present time-resolved Kerr rotation measurements, showing spin lifetimes of over 100 ns at room temperature in monolayer MoSe$_2$. These long lifetimes are accompanied by an intriguing temperature dependence of the Kerr amplitude, which increases with temperature up to 50 K and then abruptly switches sign. Using ab initio simulations we explain the latter behavior in terms of the intrinsic electron-phonon coupling and the activation of transitions to secondary valleys. The phonon-assisted scattering of the photo-excited electron-hole pairs prepares a valley spin polarization within the first few ps after laser excitation. The sign of the total valley magnetization, and thus the Kerr amplitude, switches as a function of temperature, as conduction and valence band states exhibit different phonon-mediated inter-valley scattering rates. However, the electron-phonon scattering on the ps time scale does not provide an explanation for the long spin lifetimes. Hence, we deduce that the initial spin polarization must be transferred into spin states which are protected from the intrinsic electron-phonon coupling, and are most likely resident charge carriers which are not part of the itinerant valence or conduction band states.

cond-mat.mes-hall↗

arXiv2016

Lamb shift of the Dirac cone of graphene

The fluctuations of the electromagnetic vacuum are one of the most powerful manifestations of the quantum structure of nature. Their effect on the Dirac electrons of graphene is known to induce some spectacular and purely quantistic phenomena, like the Casimir and the Aharanov--Bohm effects. In this work we demonstrate, by using a first principles approach, that the Dirac cone of graphene is also affected by a sizable Lamb shift.We show that the microscopic electronic currents flowing on the graphene plane couple efficiently with the vacuum fluctuations causing a renormalization of the electronic levels (as large as 4 meV) and of the velocities. This Lamb shift is one order of magnitude larger than the value predicted for an isolated carbon atom.

cond-mat.mes-hall↗