arXiv subjects

Samuel Poncé

Publications and source records attributed to Samuel Poncé.

64 records · Page 4Linked to original sources

arXiv2017

First-principles study of Ce$^{3+}$ doped lanthanum silicate nitride phosphors: Neutral excitation, Stokes shift, and luminescent center identification

We study from first principles two lanthanum silicate nitride compounds, LaSi$_{3}$N$_{5}$ and La$_{3}$Si$_{6}$N$_{11}$, pristine as well as doped with Ce$^{3+}$ ion, in view of explaining their different emission color, and characterising the luminescent center. The electronic structures of the two undoped hosts are similar, and do not give a hint to quantitatively describe such difference. The $4f\rightarrow 5d$ neutral excitation of the Ce$^{3+}$ ions is simulated through a constrained density-functional theory method coupled with a $Δ$SCF analysis of total energies, yielding absorption energies. Afterwards, atomic positions in the excited state are relaxed, yielding the emission energies and Stokes shifts. Based on these results, the luminescent centers in LaSi$_{3}$N$_{5}$:Ce and La$_{3}$Si$_{6}$N$_{11}$:Ce are identified. The agreement with the experimental data for the computed quantities is quite reasonable and explains the different color of the emitted light. Also, the Stokes shifts are obtained within 20\% difference relative to experimental data.

cond-mat.mtrl-sci↗

arXiv2017

Precise effective masses from density functional perturbation theory

The knowledge of effective masses is a key ingredient to analyze numerous properties of semiconductors, like carrier mobilities, (magneto-)transport properties, or band extrema characteristics yielding carrier densities and density of states. Currently, these masses are usually calculated using finite-difference estimation of density functional theory (DFT) electronic band curvatures. However, finite differences require an additional convergence study and are prone to numerical noise. Moreover, the concept of effective mass breaks down at degenerate band extrema. We assess the former limitation by developing a method that allows to obtain the Hessian of DFT bands directly, using density functional perturbation theory (DFPT). Then, we solve the latter issue by adapting the concept of `transport equivalent effective mass' to the $\vec{k} \cdot \hat{\vec{p}}$ framework. The numerical noise inherent to finite-difference methods is thus eliminated, along with the associated convergence study. The resulting method is therefore more general, more robust and simpler to use, which makes it especially appropriate for high-throughput computing. After validating the developed techniques, we apply them to the study of silicon, graphane, and arsenic. The formalism is implemented into the ABINIT software and supports the norm-conserving pseudopotential approach, the projector augmented-wave method, and the inclusion of spin-orbit coupling. The derived expressions also apply to the ultrasoft pseudopotential method.

cond-mat.mtrl-sci↗

arXiv2017

Origin of superconductivity and latent charge density wave in NbS$_2$

We elucidate the origin of the phonon-mediated superconductivity in 2$H$-NbS$_2$ using the ab initio anisotropic Migdal-Eliashberg theory including Coulomb interactions. We demonstrate that superconductivity is associated with Fermi surface hot spots exhibiting an unusually strong electron-phonon interaction. The electron-lattice coupling is dominated by low-energy anharmonic phonons, which place the system on the verge of a charge density wave instability. We also provide definitive evidence for two-gap superconductivity in 2$H$-NbS$_2$, and show that the low- and high-energy peaks observed in tunneling spectra correspond to the $Γ$- and $K$-centered Fermi surface pockets, respectively. The present findings call for further efforts to determine whether our proposed mechanism underpins superconductivity in the whole family of metallic transition metal dichalcogenides.

cond-mat.supr-con↗

arXiv2016

Temperature Dependence of the Energy Levels of Methylammonium Lead Iodide Perovskite from First Principles

Environmental effects and intrinsic energy-loss processes lead to fluctuations in the operational temperature of solar cells, which can profoundly influence their power conversion efficiency. Here we determine from first principles the effects of temperature on the band gap and band edges of the hybrid pervoskite CH$_3$NH$_3$PbI$_3$ by accounting for electron-phonon coupling and thermal expansion. From $290$ to $380$ K, the computed band gap change of $40$ meV coincides with the experimental change of $30$-$40$ meV. The calculation of electron-phonon coupling in CH$_3$NH$_3$PbI$_3$ is particularly intricate, as the commonly used Allen-Heine-Cardona theory overestimates the band gap change with temperature, and excellent agreement with experiment is only obtained when including high-order terms in the electron-phonon interaction. We also find that spin-orbit coupling enhances the electron-phonon coupling strength, but that the inclusion of nonlocal correlations using hybrid functionals has little effect. We reach similar conclusions in the metal-halide perovskite CsPbI$_3$. Our results unambiguously confirm for the first time the importance of high-order terms in the electron-phonon coupling by direct comparison with experiment.

cond-mat.mtrl-sci↗

arXiv2016

EPW: Electron-phonon coupling, transport and superconducting properties using maximally localized Wannier functions

The EPW (Electron-Phonon coupling using Wannier functions) software is a Fortran90 code that uses density-functional perturbation theory and maximally localized Wannier functions for computing electron-phonon couplings and related properties in solids accurately and efficiently. The EPW v4 program can be used to compute electron and phonon self-energies, linewidths, electron-phonon scattering rates, electron-phonon coupling strengths, transport spectral functions, electronic velocities, resistivity, anisotropic superconducting gaps and spectral functions within the Migdal-Eliashberg theory. The code now supports spin-orbit coupling, time-reversal symmetry in non-centrosymmetric crystals, polar materials, and $\mathbf{k}$ and $\mathbf{q}$-point parallelization. Considerable effort was dedicated to optimization and parallelization, achieving almost a ten times speedup with respect to previous releases. A computer test farm was implemented to ensure stability and portability of the code on the most popular compilers and architectures. Since April 2016, version 4 of the EPW code is fully integrated in and distributed with the Quantum ESPRESSO package, and can be downloaded through QE-forge at http://qe-forge.org/gf/project/q-e.

cond-mat.mtrl-sci↗

arXiv2015

Dynamical and anharmonic effects on the electron-phonon coupling and the zero-point renormalization of the electronic structure

The renormalization of the band structure at zero temperature due to electron-phonon coupling is investigated in diamond, BN, LiF and MgO crystals. We implement a dynamical scheme to compute the frequency-dependent self-energy and the resulting quasiparticle electronic structure. Our calculations reveal the presence of a satellite band below the Fermi level of LiF and MgO. We show that the renormalization factor (Z), which is neglected in the adiabatic approximation, can reduce the zero-point renormalization (ZPR) by as much as 40%. Anharmonic effects in the renormalized eigenvalues at finite atomic displacements are explored with the frozen-phonon method. We use a non-perturbative expression for the ZPR, going beyond the Allen-Heine-Cardona theory. Our results indicate that high-order electron-phonon coupling terms contribute significantly to the zero-point renormalization for certain materials.

cond-mat.mtrl-sci↗

arXiv2015

A many-body perturbation theory approach to the electron-phonon interaction with density-functional theory as a starting point

The electron-phonon interaction plays a crucial role in many fields of physics and chemistry. Nevertheless, its actual calculation by means of modern many-body perturbation theory is weakened by the use of model Hamiltonians that are based on parameters difficult to extract from the experiments. Such shortcoming can be bypassed by using density-functional theory to evaluate the electron-phonon scattering amplitudes, phonon frequencies and electronic bare energies. In this work, we discuss how a consistent many-body diagrammatic expansion can be constructed on top of density-functional theory. In that context, the role played by screening and self-consistency when all the components of the electron-nucleus and nucleus-nucleus interactions are taken into account is paramount. A way to avoid over-screening is notably presented. Finally, we derive cancellations rules as well as internal consistency constraints in order to draw a clear, sound and practical scheme to merge many-body perturbation and density-functional theory.

cond-mat.mtrl-sci↗

arXiv2015

Temperature dependence of the electronic structure of semiconductors and insulators

The renormalization of electronic eigenenergies due to electron-phonon coupling is sizable in many materials with light atoms. This effect, often neglected in ab-initio calculations, can be computed using the perturbation-based Allen-Heine-Cardona theory in the adiabatic or non-adiabatic harmonic approximation. After a short description of the numerous recent progresses in this field, and a brief overview of the theory, we focus on the issue of phonon wavevector sampling convergence, until now poorly understood. Indeed, the renormalization is obtained numerically through a q-point sampling inside the BZ. For q-points close to G, we show that a divergence due to non-zero Born effective charge appears in the electron-phonon matrix elements, leading to a divergence of the integral over the BZ for band extrema. Although it should vanish for non-polar materials, unphysical residual Born effective charges are usually present in ab-initio calculations. Here, we propose a solution that improves the coupled q-point convergence dramatically. For polar materials, the problem is more severe: the divergence of the integral does not disappear in the adiabatic harmonic approximation, but only in the non-adiabatic harmonic approximation. In all cases, we study in detail the convergence behavior of the renormalization as the q-point sampling goes to infinity and the imaginary broadening parameter goes to zero. This allows extrapolation, thus enabling a systematic way to converge the renormalization for both polar and non-polar materials. Finally, the adiabatic and non-adiabatic theory, with corrections for the divergence problem, are applied to the study of five semiconductors and insulators: a-AlN, b-AlN, BN, diamond and silicon. For these five materials, we present the zero-point renormalization, temperature dependence, phonon-induced lifetime broadening and the renormalized electronic bandstructure.

cond-mat.mtrl-sci↗

arXiv2014

The temperature dependence of electronic eigenenergies in the adiabatic harmonic approximation

The renormalization of electronic eigenenergies due to electron-phonon interactions (temperature dependence and zero-point motion effect) is important in many materials. We address it in the adiabatic harmonic approximation, based on first principles (e.g. Density-Functional Theory), from different points of view: directly from atomic position fluctuations or, alternatively, from Janak's theorem generalized to the case where the Helmholtz free energy, including the vibrational entropy, is used. We prove their equivalence, based on the usual form of Janak's theorem and on the dynamical equation. We then also place the Allen-Heine-Cardona (AHC) theory of the renormalization in a first-principle context. The AHC theory relies on the rigid-ion approximation, and naturally leads to a self-energy (Fan) contribution and a Debye-Waller contribution. Such a splitting can also be done for the complete harmonic adiabatic expression, in which the rigid-ion approximation is not required. A numerical study within the Density-Functional Perturbation theory framework allows us to compare the AHC theory with frozen-phonon calculations, with or without the rigid-ion terms. For the two different numerical approaches without rigid-ion terms, the agreement is better than 7 $μ$eV in the case of diamond, which represent an agreement to 5 significant digits. The magnitude of the non rigid-ion terms in this case is also presented, distinguishing specific phonon modes contributions to different electronic eigenenergies.

cond-mat.mtrl-sci↗

arXiv2013

Band widths and gaps from the Tran-Blaha functional : Comparison with many-body perturbation theory

For a set of ten crystalline materials (oxides and semiconductors), we compute the electronic band structures using the Tran-Blaha [Phys. Rev. Lett. 102, 226401 (2009)] (TB09) functional. The band widths and gaps are compared with those from the local-density approximation (LDA) functional, many-body perturbation theory (MBPT), and experiments. At the density-functional theory (DFT) level, TB09 leads to band gaps in much better agreement with experiments than LDA. However, we observe that it globally underestimates, often strongly, the valence (and conduction) band widths (more than LDA). MBPT corrections are calculated starting from both LDA and TB09 eigenenergies and wavefunctions. They lead to a much better agreement with experimental data for band widths. The band gaps obtained starting from TB09 are close to those from quasi-particle self-consistent GW calculations, at a much reduced cost. Finally, we explore the possibility to tune one of the semi-empirical parameters of the TB09 functional in order to obtain simultaneously better band gaps and widths. We find that these requirements are conflicting.

cond-mat.mtrl-sci↗