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Critical Role of the Exchange Interaction for the Electronic Structure and Charge-Density-Wave Formation in TiSe2 ; ; et al in Physical Review Letters (2017), 119 We show that the inclusion of screened exchange via hybrid functionals provides a unified description of the electronic and vibrational properties of TiSe2. In contrast to local approximations in density ... [more ▼] We show that the inclusion of screened exchange via hybrid functionals provides a unified description of the electronic and vibrational properties of TiSe2. In contrast to local approximations in density functional theory, the explicit inclusion of exact, nonlocal exchange captures the effects of the electron-electron interaction needed to both separate the Ti-d states from the Se-p states and stabilize the charge-density- wave (CDW) (or low-T) phase through the formation of a p-d hybridized state. We further show that this leads to an enhanced electron-phonon coupling that can drive the transition even if a small gap opens in the high-T phase. Finally, we demonstrate that the hybrid functionals can generate a CDW phase where the electronic bands, the geometry, and the phonon frequencies are in agreement with experiments. [less ▲] Detailed reference viewed: 18 (2 UL)Ab Initio Calculations of Ultrashort Carrier Dynamics in Two-Dimensional Materials: Valley Depolarization in Single-Layer WSe2 Molina-Sanchez, Alejandro ; ; Wirtz, Ludger et al in Nano Letters (2017), 17 Detailed reference viewed: 53 (2 UL)Ab initio calculation of the G peak intensity of graphene: Laser-energy and Fermi-energy dependence and importance of quantum interference effects Reichardt, Sven ; Wirtz, Ludger in Physical Review B (2017), 95(19), 195422 We present the results of a diagrammatic, fully ab initio calculation of the G peak intensity of graphene. The flexibility and generality of our approach enables us to go beyond the previous analytical ... [more ▼] We present the results of a diagrammatic, fully ab initio calculation of the G peak intensity of graphene. The flexibility and generality of our approach enables us to go beyond the previous analytical calculations in the low-energy regime. We study the laser and Fermi energy dependence of the G peak intensity and analyze the contributions from resonant and nonresonant electronic transitions. In particular, we explicitly demonstrate the importance of quantum interference and nonresonant states for the G peak process. Our method of analysis and computational concept is completely general and can easily be applied to study other materials as well. [less ▲] Detailed reference viewed: 50 (7 UL)Tuning the Pseudospin Polarization of Graphene by a Pseudomagnetic Field ; ; et al in Nano Letters (2017), 17 One of the intriguing characteristics of honeycomb lattices is the appearance of a pseudomagnetic field as a result of mechanical deformation. In the case of graphene, the Landau quantization resulting ... [more ▼] One of the intriguing characteristics of honeycomb lattices is the appearance of a pseudomagnetic field as a result of mechanical deformation. In the case of graphene, the Landau quantization resulting from this pseudomagnetic field has been measured using scanning tunneling microscopy. Here we show that a signature of the pseudomagnetic field is a local sublattice symmetry breaking observable as a redistribution of the local density of states. This can be interpreted as a polarization of graphene’s pseudospin due to a strain induced pseudomagnetic field, in analogy to the alignment of a real spin in a magnetic field. We reveal this sublattice symmetry breaking by tunably straining graphene using the tip of a scanning tunneling microscope. The tip locally lifts the graphene membrane from a SiO2 support, as visible by an increased slope of the I(z) curves. The amount of lifting is consistent with molecular dynamics calculations, which reveal a deformed graphene area under the tip in the shape of a Gaussian. The pseudomagnetic field induced by the deformation becomes visible as a sublattice symmetry breaking which scales with the lifting height of the strained deformation and therefore with the pseudomagnetic field strength. Its magnitude is quantitatively reproduced by analytic and tight-binding models, revealing fields of 1000 T. These results might be the starting point for an effective THz valley filter, as a basic element of valleytronics. [less ▲] Detailed reference viewed: 16 (0 UL)Quantum Interference Effects in Resonant Raman Spectroscopy of Single- and Triple-Layer MoTe2 from First-Principles Pereira Coutada Miranda, Henrique ; Reichardt, Sven ; et al in Nano Letters (2017), 17(4), 2381--2388 We present a combined experimental and theoretical study of resonant Raman spectroscopy in single- and triple-layer MoTe2. Raman intensities are computed entirely from first-principles by calculating ... [more ▼] We present a combined experimental and theoretical study of resonant Raman spectroscopy in single- and triple-layer MoTe2. Raman intensities are computed entirely from first-principles by calculating finite differences of the dielectric susceptibility. In our analysis, we investigate the role of quantum interference effects and the electron−phonon coupling. With this method, we explain the experimentally observed intensity inversion of the A′1 vibrational modes in triple-layer MoTe2 with increasing laser photon energy. Finally, we show that a quantitative comparison with experimental data requires the proper inclusion of excitonic effects. [less ▲] Detailed reference viewed: 37 (5 UL)Raman Spectroscopy of Graphene Reichardt, Sven ; Wirtz, Ludger in Binder, Rolf (Ed.) Optical Properties of Graphene (2017) Raman spectroscopy of graphene is reviewed from a theoretical perspective. After an introduction of the building blocks (electronic band structure, phonon dispersion, electron-phonon interaction, electron ... [more ▼] Raman spectroscopy of graphene is reviewed from a theoretical perspective. After an introduction of the building blocks (electronic band structure, phonon dispersion, electron-phonon interaction, electron-light coupling), Raman intensities are calculated using time-dependent perturbation theory. The analysis of the contributing terms allows for an intuitive understanding of the Raman peak positions and intensities. The Raman spectrum of pure graphene only displays two principle peaks. Yet, their variation as a function of internal and external parameters and the occur- rence of secondary, defect-related peaks, conveys a lot of information about the system. Thus, Raman spectroscopy is used routinely to analyze layer number, defects, doping and strain of graphene samples. At the same time, it is an intriguing playground to study the optical properties of graphene. [less ▲] Detailed reference viewed: 76 (3 UL)Valence band splitting in Cu2(Sn,Ge, Si)S3: effect on optical absorption spectra De Wild, Jessica ; Kalesaki, Efterpi ; Wirtz, Ludger et al in Physica Status Solidi. Rapid Research Letters (2017) We perform a detailed analysis of the valence band splitting (VBS) effect on the absorption spectra of monoclinic Cu2(Sn,Ge,Si)S3 combining theory and experiment. We cal- culate the imaginary part of the ... [more ▼] We perform a detailed analysis of the valence band splitting (VBS) effect on the absorption spectra of monoclinic Cu2(Sn,Ge,Si)S3 combining theory and experiment. We cal- culate the imaginary part of the dielectric function for all three compounds using hybrid functionals and maximally lo- calized Wannier functions in remarkably dense k-meshes to ensure an accurate description of the low energy spectral regime. We find that the VBS will affect the absorption spectra of these materials leading to multiple absorption onsets. Our experimental spectra on Cu2(Sn,Ge)S3, analysed using both Tauc plots and inflection points, verify this prediction. A good agreement between theory and experiment in terms of VBS values is recorded. [less ▲] Detailed reference viewed: 115 (8 UL)Excitons in boron nitride single layer ; Paleari, Fulvio ; Pereira Coutada Miranda, Henrique et al in Physical Review. B : Condensed Matter (2016), 94(125303), Boron nitride single layer belongs to the family of two-dimensional materials whose optical properties are currently receiving considerable attention. Strong excitonic effects have already been observed ... [more ▼] Boron nitride single layer belongs to the family of two-dimensional materials whose optical properties are currently receiving considerable attention. Strong excitonic effects have already been observed in the bulk and still stronger effects are predicted for single layers. We present here a detailed study of these properties by combining ab initio calculations and a tight-binding Wannier analysis in both real and reciprocal space. Due to the simplicity of the band structure with single valence (π) and conduction (π∗) bands the tight-binding analysis becomes quasiquantitative with only two adjustable parameters and provides tools for a detailed analysis of the exciton properties. Strong deviations from the usual hydrogenic model are evidenced. The ground-state exciton is not a genuine Frenkel exciton, but a very localized tightly bound one. The other ones are similar to those found in transition-metal dichalcogenides and, although more localized, can be described within a Wannier-Mott scheme. [less ▲] Detailed reference viewed: 142 (16 UL)Theoretical Study of the Raman G Peak Intensity of Graphene Reichardt, Sven ; Wirtz, Ludger Poster (2016, February 18) Detailed reference viewed: 79 (11 UL)Temperature-dependent excitonic effects in the optical properties of single-layer MoS2 Molina-Sanchez, Alejandro ; ; et al in Physical Review. B : Condensed Matter (2016), 93 The electron-phonon interaction alters substantially the conventional picture of the band structure. It also changes the properties of excitonic states, which are very pronounced in many 2D materials ... [more ▼] The electron-phonon interaction alters substantially the conventional picture of the band structure. It also changes the properties of excitonic states, which are very pronounced in many 2D materials. Using many-body perturbation theory, the authors describe how the inclusion of temperature modifies the electronic bands of single-layer MoS2. Different bands and different regions in the Brillouin zone are affected in different ways by electron-phonon coupling. Using the temperature-broadened bands as input for the Bethe-Salpeter equation, the authors explain why, for the bound A and B excitons, the electron-phonon coupling changes mainly the position, and for the C exciton, only the width is affected by temperature, while the energy is rather constant. [less ▲] Detailed reference viewed: 178 (11 UL)Vibrational and optical properties of MoS2: From monolayer to bulk Molina-Sanchez, Alejandro ; ; Wirtz, Ludger in Surface Science Reports (2015), 70(4), 554-586 Molybdenum disulfide, MoS2, has recently gained considerable attention as a layered material where neighboring layers are only weakly interacting and can easily slide against each other. Therefore ... [more ▼] Molybdenum disulfide, MoS2, has recently gained considerable attention as a layered material where neighboring layers are only weakly interacting and can easily slide against each other. Therefore, mechanical exfoliation allows the fabrication of single and multi-layers and opens the possibility to generate atomically thin crystals with outstanding properties. In contrast to graphene, it has an optical gap of ~1.9 eV. This makes it a prominent candidate for transistor and opto-electronic applications. Single-layer MoS2 exhibits remarkably different physical properties compared to bulk MoS2 due to the absence of interlayer hybridization. For instance, while the band gap of bulk and multi-layer MoS2 is indirect, it becomes direct with decreasing number of layers. In this review, we analyze from a theoretical point of view the electronic, optical, and vibrational properties of single-layer, few-layer and bulk MoS2. In particular, we focus on the effects of spin–orbit interaction, number of layers, and applied tensile strain on the vibrational and optical properties. We examine the results obtained by different methodologies, mainly ab initio approaches. We also discuss which approximations are suitable for MoS2 and layered materials. The effect of external strain on the band gap of single-layer MoS2 and the crossover from indirect to direct band gap is investigated. We analyze the excitonic effects on the absorption spectra. The main features, such as the double peak at the absorption threshold and the high-energy exciton are presented. Furthermore, we report on the the phonon dispersion relations of single-layer, few-layer and bulk MoS2. Based on the latter, we explain the behavior of the Raman-active A1gA1g and View the MathML sourceE2g1 modes as a function of the number of layers. Finally, we compare theoretical and experimental results of Raman, photoluminescence, and optical-absorption spectroscopy. [less ▲] Detailed reference viewed: 141 (12 UL)Semi-empirical discription of Kohn anomalies in the phonon dispersion of graphene Reichardt, Sven ; Wirtz, Ludger Poster (2015, September 08) Detailed reference viewed: 68 (5 UL)Unified Description of the Optical Phonon Modes in N-Layer MoTe2 ; ; et al in Nano Letters (2015), 15 N-layer transition metal dichalcogenides provide a unique platform to investigate the evolution of the physical properties between the bulk (three-dimensional) and monolayer (quasi-two-dimensional) limits ... [more ▼] N-layer transition metal dichalcogenides provide a unique platform to investigate the evolution of the physical properties between the bulk (three-dimensional) and monolayer (quasi-two-dimensional) limits. Here, using high-resolution micro-Raman spectroscopy, we report a unified experimental description of the Γ-point optical phonons in N-layer 2H-molybdenum ditelluride (MoTe2). We observe series of N-dependent low-frequency interlayer shear and breathing modes (below 40 cm–1, denoted LSM and LBM) and well-defined Davydov splittings of the mid-frequency modes (in the range 100–200 cm–1, denoted iX and oX), which solely involve displacements of the chalcogen atoms. In contrast, the high-frequency modes (in the range 200–300 cm–1, denoted iMX and oMX), arising from displacements of both the metal and chalcogen atoms, exhibit considerably reduced splittings. The manifold of phonon modes associated with the in-plane and out-of-plane displacements are quantitatively described by a force constant model, including interactions up to the second nearest neighbor and surface effects as fitting parameters. The splittings for the iX and oX modes observed in N-layer crystals are directly correlated to the corresponding bulk Davydov splittings between the E2u/E1g and B1u/A1g modes, respectively, and provide a measurement of the frequencies of the bulk silent E2u and B1u optical phonon modes. Our analysis could readily be generalized to other layered crystals [less ▲] Detailed reference viewed: 109 (8 UL)Electronic and Vibrational proprieties of graphene on Ir(111) and SiC(100) Pereira Coutada Miranda, Henrique ; Molina-Sanchez, Alejandro ; Wirtz, Ludger Poster (2015, September) In the last years, graphene has become one of the most studied materials due to its peculiar electronic, optical, thermal, and mechanical properties. It is thus of major importance, for practical ... [more ▼] In the last years, graphene has become one of the most studied materials due to its peculiar electronic, optical, thermal, and mechanical properties. It is thus of major importance, for practical applications, to study how the electronic and vibrational proprieties of graphene change when deposited on a substrate. The non-commensurability of the unit cell of graphene with the substrate leads to the formation of Moiré patterns with accordingly large supercell sizes. Ab-initio calculations using standard plane-wave based codes on these large systems are of high computational cost even for the ground-state calculations. We show the effect that such Moiré patterns have on the band structure by projecting the resulting electronic structure and phonon dispersion onto the unit cell of free-standing graphene with an unfolding scheme. We compare our results with HREELS measurements of the phonon dispersion of graphene on Ir(111). The accurate knowledge of the interaction graphene-substrate will provide important information for future applications of graphene on electronic devices. Work performed in collaboration with the experimental groups of J. Kroeger (TU Ilmenau, Germany) and T. Seyller (TU Chemnitz, Germany). [less ▲] Detailed reference viewed: 161 (3 UL)Phonon-limited carrier mobility and resistivity from carbon nanotubes to graphene ; Pereira Coutada Miranda, Henrique ; et al in Physical Review. B: Condensed Matter and Materials Physics (2015) Under which conditions do the electrical transport properties of one-dimensional (1D) carbon nanotubes (CNTs) and 2D graphene become equivalent? We have performed atomistic calculations of the phonon ... [more ▼] Under which conditions do the electrical transport properties of one-dimensional (1D) carbon nanotubes (CNTs) and 2D graphene become equivalent? We have performed atomistic calculations of the phonon-limited electrical mobility in graphene and in a wide range of CNTs of different types to address this issue. The theoretical study is based on a tight-binding method and a force-constant model from which all possible electron-phonon couplings are computed. The electrical resistivity of graphene is found in very good agreement with experiments performed at high carrier density. A common methodology is applied to study the transition from one to two dimensions by considering CNTs with diameter up to 16 nm. It is found that the mobility in CNTs of increasing diameter converges to the same value, i.e., the mobility in graphene. This convergence is much faster at high temperature and high carrier density. For small-diameter CNTs, the mobility depends strongly on chirality, diameter, and the existence of a band gap. [less ▲] Detailed reference viewed: 141 (8 UL)Ab-initio study of the temperature effects on the optical properties of transition metal dichalcogenides Molina-Sanchez, Alejandro ; ; et al Scientific Conference (2015, March 05) Detailed reference viewed: 44 (0 UL)A force-constant model of graphene for conductivity calculations Pereira Coutada Miranda, Henrique ; Wirtz, Ludger Poster (2015, January) Transport in graphene is strongly limited by the electron-phonon interaction. Accurate description of the phonon dispersion relations is essential for the study of this interaction. Using current state-of ... [more ▼] Transport in graphene is strongly limited by the electron-phonon interaction. Accurate description of the phonon dispersion relations is essential for the study of this interaction. Using current state-of-the-art ab initio density-functional theory plane-wave codes, we are limited to systems with few atoms. For larger systems (e.g., nanotubes, nanoribbons), accurate semi-empircal models are needed. We have developed a force constant model for the phonon dispersion of graphene. Our implementation can include a large number of neighbours, which allows us to simulate accurately long-range interaction effects. As shown in previous publications it is possible to reproduce the phonon dispersion frequencies of graphene with a 4th nearest neighbours force constant model. However, some features can only be captured using long-range interactions (Kohn-anomalies, certain phonon eigenvectors). Using an ab initio phonon dispersion calculated with DFPT as reference, we show the nature of the long-range interactions and explore different ways to include them in our semi-empirical model. We also study the dependence of the force constants on charge and strain. Work in collaboration with Jing Li, Yann-Michel Niquet, Luigi Genovese, and Ivan Duchemin from L_Sim, SP2M, UMR-E CEA/UJF-Grenoble 1, INAC, Grenoble, France and Christophe Delerue from IEMN - Dept. ISEN, UMR CNRS 8520, Lille, France [less ▲] Detailed reference viewed: 112 (7 UL)Ab initio perspective on the Mollwo-Ivey relation for F centers in alkali halides ; ; et al in Physical Review. B: Condensed Matter and Materials Physics (2015), 92 We revisit the well-known Mollwo-Ivey relation that describes the ``universal'' dependence of the absorption energies of F-type color centers on the lattice constant a of alkali-halide crystals, E-abs ... [more ▼] We revisit the well-known Mollwo-Ivey relation that describes the ``universal'' dependence of the absorption energies of F-type color centers on the lattice constant a of alkali-halide crystals, E-abs proportional to a(-n). We perform both state-of-the-art ab initio quantum chemistry and post-DFT calculations of F-center absorption spectra. By ``tuning'' independently the lattice constant and the atomic species we show that the scaling with the lattice constant alone 2 in agreement with the ``particle-in-the-box'' model. Keeping the lattice constant fixed and changing the atomic species enables us to quantify the ion-size effects which are shown to be responsible for the exponent n approximate to 1.8. [less ▲] Detailed reference viewed: 43 (1 UL)Raman spectroscopy of graphite intercalation compounds: Charge transfer, strain, and electron–phonon coupling in graphene layers ; Wirtz, Ludger ; in Physica Status Solidi B. Basic Research (2014), 251(12), 23372355 Graphite intercalation compounds (GICs) are an interesting and highly studied field since 1970’s. It has gained renewed interest since the discovery of superconductivity at high temperature for CaC6 and ... [more ▼] Graphite intercalation compounds (GICs) are an interesting and highly studied field since 1970’s. It has gained renewed interest since the discovery of superconductivity at high temperature for CaC6 and the rise of graphene. Intercalation is a technique used to introduce atoms or molecules into the structure of a host material. Intercalation of alkali metals in graphite has shown to be a controllable procedure recently used as a scalable technique for bulk production of graphene, and nano-ribbons by induced exfoliation of graphite. It also creates supra-molecular interactions between the host and the intercalant, inducing changes in the electronic, mechanical, and physical properties of the host. GICs are the mother system of intercalation also employed in fullerenes, carbon nanotubes, graphene, and carbon-composites. We will show how a combination of Raman and ab-initio calculations of the density and the electronic band structure in GICs can serve as a tool to elucidate the electronic structure, electron–phonon coupling, charge transfer, and lattice parameters of GICs and the graphene layers within. This knowledge of GICs is of high importance to understand superconductivity and to set the basis for applications with GICs, graphene and other nano-carbon based materials like nanocomposites in batteries and nanoelectronic devices. [less ▲] Detailed reference viewed: 123 (11 UL)Moiré-induced replica of graphene phonons on Ir(111) ; Pereira Coutada Miranda, Henrique ; Molina-Sanchez, Alejandro et al in Annalen der Physik (2014), 526(9-10), 372-380 The phonon dispersion of singly oriented graphene on Ir(111) has been determined by angle-resolved inelastic electron scattering. Replica of graphene phonon bands are induced by the moire superstructure ... [more ▼] The phonon dispersion of singly oriented graphene on Ir(111) has been determined by angle-resolved inelastic electron scattering. Replica of graphene phonon bands are induced by the moire superstructure. Calculations for a linear chain of C atoms attached to an infinitely heavy substrate reveal that imposing a superstructure by periodically varying the C-C interaction and the C-substrate coupling induces replicated phonons at wave vectors reflecting the supercell periodicity. Deviations between the phonon dispersion of graphene on Ir(111) and of pristine graphene are analyzed and rationalized in terms of the weak graphene-Ir(111) interaction. [less ▲] Detailed reference viewed: 116 (13 UL) |
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