*J Chem Phys ; 154(16): 164116, 2021 Apr 28.*

##### RESUMO

In this paper, we present a novel efficient and parallel implementation, RelaxSE, for the calculation of the low-lying excited states and energies of strongly correlated systems. RelaxSE is based on the fully uncontracted multi-reference method of Selected Active Space + Single excitations. This method has been specifically designed to be able to tackle systems with numerous open shells per atoms. It is, however, computationally challenging due to the rapid scaling of the number of determinants and their non-trivial ordering induced by the selection process. We propose a combined determinant-driven and integral-driven approach designed for hybrid OpenMP/MPI parallelization. The performances of RelaxSE are evaluated on a controlled test set and show linear scaling with respect to the number of determinants and a small overhead due to the parallelization. Systems with up to 1 × 109 determinants are successfully computed.

*Acta Crystallogr B Struct Sci Cryst Eng Mater ; 75(Pt 4): 687-696, 2019 Aug 01.*

##### RESUMO

The room-temperature structural properties of the RMn2O5 multiferroics have been investigated under pressure, using powder X-ray scattering and density functional theory (DFT) calculations. It was possible to determine the lattice parameters and the main atomic positions as a function of pressure. Good agreement was observed between the X-ray and DFT results for most of the determined crystallographic data. From the DFT calculations, it was possible to infer the pressure evolution of the exchange interactions, and this analysis led to the conclusion that the onset of the q = (½, 0, ½) magnetic structure under pressure is related to the increase in the J1 super-exchange terms (due to the reduction in the Mn-O distances) compared with the Mn-R exchange interactions. In addition, the 1D antiferromagnetic character of the compounds should be reinforced under pressure.

*Phys Rev Lett ; 113(13): 137602, 2014 Sep 26.*

##### RESUMO

We report here the discovery of multiferroicity and large magnetoelectric coupling in the type I orbital order system GeV4S8. Our study demonstrates that this clustered compound displays a para-ferroelectric transition at 32 K. This transition originates from an orbital ordering which reorganizes the charge within the transition metal clusters. Below the antiferromagnetic transition at 17 K, the application of a magnetic field significantly affects the ferroelectric polarization, revealing thus a large magnetoelectric coupling. Our study suggests that the application of a magnetic field induces a metamagnetic transition which significantly affects the ferroelectric polarization thanks to an exchange striction phenomenon.

*J Phys Condens Matter ; 25(41): 416002, 2013 Oct 16.*

##### RESUMO

We performed magnetic and ferroelectric measurements, associated with Landau theory and symmetry analysis, in order to clarify the situation of the YMnO3 system, a classical example of type I multiferroics. We found that the only magnetic group compatible with all experimental data (neutron scattering, magnetization, polarization, dielectric constant, second harmonic generation) is the P6'(3) group. In this group a small ferromagnetic component along c is induced by the Dzyaloshinskii-Moriya interaction, and observed here in magnetization measurements. We found that the ferromagnetic and antiferromagnetic components can only be switched simultaneously, while the magnetic orders are functions of the polarization square and therefore insensitive to its sign.

##### Assuntos

Campos Magnéticos , Compostos de Manganês/química , Modelos Químicos , Modelos Moleculares , Simulação por Computador , Teste de Materiais*Phys Rev Lett ; 108(8): 087202, 2012 Feb 24.*

##### RESUMO

The control of matter properties (transport, magnetic, dielectric, ) using synthesis as thin films is strongly hindered by the lack of reliable theories, able to guide the design of new systems, through the understanding of the interface effects and of the way the substrate constraints are imposed on the material. The present Letter analyzes the energetic contributions at the interfaces, and proposes a model describing the microscopic mechanisms governing the interactions at an epitaxial interface between a manganite and another transition metal oxide in perovskite structure (as for instance SrTiO3). The model is checked against experimental results and literature analysis.

*Dalton Trans ; 40(20): 5538-48, 2011 May 28.*

##### RESUMO

Microcrystalline single-phase strontium oxotellurate(IV) monohydrate, SrTeO(3)(H(2)O), was obtained by microwave-assisted hydrothermal synthesis under alkaline conditions at 180 °C for 30 min. A temperature of 220 °C and longer reaction times led to single crystal growth of this material. The crystal structure of SrTeO(3)(H(2)O) was determined from single crystal X-ray diffraction data: P2(1)/c, Z = 4, a = 7.7669(5), b = 7.1739(4), c = 8.3311(5) Å, ß = 107.210(1)°, V = 443.42(5) Å(3), 1403 structure factors, 63 parameters, R[F(2)>2σ(F(2))] = 0.0208, wR(F(2) all) = 0.0516, S = 1.031. SrTeO(3)(H(2)O) is isotypic with the homologous BaTeO(3)(H(2)O) and is characterised by a layered assembly parallel to (100) of edge-sharing [SrO(6)(H(2)O)] polyhedra capped on each side of the layer by trigonal-prismatic [TeO(3)] units. The cohesion of the structure is accomplished by moderate O-H···O hydrogen bonding interactions between donor water molecules and acceptor O atoms of adjacent layers. In a topochemical reaction, SrTeO(3)(H(2)O) condensates above 150 °C to the metastable phase Îµ-SrTeO(3) and transforms upon further heating to Î´-SrTeO(3). The crystal structure of Îµ-SrTeO(3), the fifth known polymorph of this composition, was determined from combined electron microscopy and laboratory X-ray powder diffraction studies: P2(1)/c, Z = 4, a = 6.7759(1), b = 7.2188(1), c = 8.6773(2) Å, ß = 126.4980(7)°, V = 341.20(18) Å(3), R(Fobs) = 0.0166, R(Bobs) = 0.0318, Rwp = 0.0733, Goof = 1.38. The structure of Îµ-SrTeO(3) shows the same basic set-up as SrTeO(3)(H(2)O), but the layered arrangement of the hydrous phase transforms into a framework structure after elimination of water. The structural studies of SrTeO(3)(H(2)O) and Îµ-SrTeO(3) are complemented by thermal analysis and vibrational spectroscopic measurements.

*Phys Rev Lett ; 104(4): 046804, 2010 Jan 29.*

##### RESUMO

Using first principle calculations we showed that the Curie temperature of manganites thin films can be increased by far more than an order of magnitude by applying appropriate strains. Our main breakthrough is that the control of the orbital ordering responsible for the spectacular T{C} increase cannot be imposed by the substrate only. Indeed, the strains, first applied by the substrate, need to be maintained over the growth direction by the alternation of the manganite layers with another appropriate material. Following these theoretical findings, we synthesized such superlattices and verified our theoretical predictions.

*J Phys Condens Matter ; 22(34): 345603, 2010 Sep 01.*

##### RESUMO

We used quantum chemical ab initio methods to determine the effective parameters of Hubbard and t-J models for the Na(x)CoO(2) compounds (x = 0 and 0.5). As for the superconducting compound we found the a(1g) cobalt orbitals above the e'(g) ones by a few hundreds of meV due to the e'(g)-e(g) hybridization of the cobalt 3d orbitals. The correlation strength was found to increase with the sodium content x, whereas the in-plane AFM coupling decreases. The less correlated system was found to be the pure CoO(2), however it is still strongly correlated and very close to the Mott transition. Indeed we found U/t â¼ 15, which is the critical value for the Mott transition in a triangular lattice. Finally, we found the magnetic exchanges in the CoO(2) layers to be strongly dependent on the weak local structural distortions.

*J Chem Phys ; 128(24): 244716, 2008 Jun 28.*

##### RESUMO

An efficient real space method is derived for the evaluation of the Madelung's potential of ionic crystals. The proposed method is an extension of Evjen's method. It takes advantage of a general analysis of the potential convergence in real space. Indeed, we show that the series convergence is exponential as a function of the number of canceled multipolar moments in the unit cell. The method proposed in this work reaches such an exponential convergence rate. Its efficiency is comparable to Ewald's method. However, unlike the latter, it uses only simple algebraic functions.

*Phys Rev Lett ; 92(23): 236402, 2004 Jun 11.*

##### RESUMO

We study the influence of the structural modulation on the low energy physics of the Sr14-xCaxCu24O41 oxides, using ab initio determination of the on-site and nearest-neighbor effective parameters. The structural modulations appear to be the key degree of freedom responsible for the low energy properties, such as the electron localization, the formation of dimers in the x=0 compound, or the antiferromagnetic order in the x=13.6 compound.

*Phys Rev Lett ; 88(5): 056405, 2002 Feb 04.*

##### RESUMO

We report ab initio calculations of the charge ordering in alpha'NaV2O5 using large configurations interaction methods on embedded fragments. Our major result is that the 2p(y) electrons of the bridging oxygen of the rungs present a very strong magnetic character and should thus be explicitly considered in any relevant effective model. The most striking consequence of this result is that the spin and charge ordering differ substantially, as differ the experimental results depending on whether they are sensitive to the spin or charge density.