A quantum Monte Carlo study of the one-dimensional ionic Hubbard model

Quantum Monte Carlo methods are used to study a quantum phase transition in a 1D Hubbard model with a staggered ionic potential (D). Using recently formulated methods, the electronic polarization and localization are determined directly from the correlated ground state wavefunction and compared to results of previous work using exact diagonalization and Hartree-Fock. We find that the model undergoes a thermodynamic transition from a band insulator (BI) to a broken-symmetry bond ordered (BO) phase as the ratio of U/D is increased. Since it is known that at D = 0 the usual Hubbard model is a Mott insulator (MI) with no long-range order, we have searched for a second transition to this state by (i) increasing U at fixed ionic potential (D) and (ii) decreasing D at fixed U. We find no transition from the BO to MI state, and we propose that the MI state in 1D is unstable to bond ordering under the addition of any finite ionic potential. In real 1D systems the symmetric MI phase is never stable and the transition is from a symmetric BI phase to a dimerized BO phase, with a metallic point at the transition

Born Effective Charges of Barium Titanate: band by band decomposition and sensitivity to structural features

The Born effective charge tensors of Barium Titanate have been calculated for each of its 4 phases. Large effective charges of Ti and O, also predicted by shell model calculations and made plausible by a simplified model, reflect the partial covalent character of the chemical bond. A band by band decomposition confirms that orbital hybridization is not restricted to Ti and O atoms but also involves Ba which appears more covalent than generally assumed. Our calculations reveal a strong dependence of the effective charges on the atomic positions contrasting with a relative insensitivity on isotropic volume changes.Comment: 13 page

Bloch bundles, Marzari-Vanderbilt functional and maximally localized Wannier functions

We consider a periodic Schroedinger operator and the composite Wannier functions corresponding to a relevant family of its Bloch bands, separated by a gap from the rest of the spectrum. We study the associated localization functional introduced by Marzari and Vanderbilt, and we prove some results about the existence and exponential localization of its minimizers, in dimension d < 4. The proof exploits ideas and methods from the theory of harmonic maps between Riemannian manifolds.Comment: 37 pages, no figures. V2: the appendix has been completely rewritten. V3: final version, to appear in Commun. Math. Physic

Sigma-2 Receptor Ligand Binding Modulates Association between TSPO and TMEM97

Sigma-2 receptor (S2R) is a S2R ligand-binding site historically associated with reportedly 21.5 kDa proteins that have been linked to several diseases, such as cancer, Alzheimer's disease, and schizophrenia. The S2R is highly expressed in various tumors, where it correlates with the proliferative status of the malignant cells. Recently, S2R was reported to be the transmembrane protein TMEM97. Prior to that, we had been investigating the translocator protein (TSPO) as a potential 21.5 kDa S2R candidate protein with reported heme and sterol associations. Here, we investigate the contributions of TMEM97 and TSPO to S2R activity in MCF7 breast adenocarcinoma and MIA PaCa-2 (MP) pancreatic carcinoma cells. Additionally, the role of the reported S2R-interacting partner PGRMC1 was also elucidated. Proximity ligation assays and co-immunoprecipitation show a functional association between S2R and TSPO. Moreover, a close physical colocalization of TMEM97 and TSPO was found in MP cells. In MCF7 cells, co-immunoprecipitation only occurred with TMEM97 but not with PGRMC1, which was further confirmed by confocal microscopy experiments. Treatment with the TMEM97 ligand 20-(S)-hydroxycholesterol reduced co-immunoprecipitation of both TMEM97 and PGRMC1 in immune pellets of immunoprecipitated TSPO in MP cells. To the best of our knowledge, this is the first suggestion of a (functional) interaction between TSPO and TMEM97 that can be affected by S2R ligands

Phonons and related properties of extended systems from density-functional perturbation theory

This article reviews the current status of lattice-dynamical calculations in crystals, using density-functional perturbation theory, with emphasis on the plane-wave pseudo-potential method. Several specialized topics are treated, including the implementation for metals, the calculation of the response to macroscopic electric fields and their relevance to long wave-length vibrations in polar materials, the response to strain deformations, and higher-order responses. The success of this methodology is demonstrated with a number of applications existing in the literature.Comment: 52 pages, 14 figures, submitted to Review of Modern Physic

Atomistic origins of high-performance in hybrid halide perovskite solar cells

The performance of organometallic perovskite solar cells has rapidly surpassed that of both conventional dye-sensitised and organic photovoltaics. High power conversion efficiency can be realised in both mesoporous and thin-film device architectures. We address the origin of this success in the context of the materials chemistry and physics of the bulk perovskite as described by electronic structure calculations. In addition to the basic optoelectronic properties essential for an efficient photovoltaic device (spectrally suitable band gap, high optical absorption, low carrier effective masses), the materials are structurally and compositionally flexible. As we show, hybrid perovskites exhibit spontaneous electric polarisation; we also suggest ways in which this can be tuned through judicious choice of the organic cation. The presence of ferroelectric domains will result in internal junctions that may aid separation of photoexcited electron and hole pairs, and reduction of recombination through segregation of charge carriers. The combination of high dielectric constant and low effective mass promotes both Wannier-Mott exciton separation and effective ionisation of donor and acceptor defects. The photoferroic effect could be exploited in nanostructured films to generate a higher open circuit voltage and may contribute to the current-voltage hysteresis observed in perovskite solar cells.Comment: 6 pages, 5 figure

Nature of the insulating phases in the half-filled ionic Hubbard model

We investigate the ground-state phase diagram of the one-dimensional "ionic" Hubbard model with an alternating periodic potential at half-filling by numerical diagonalization of finite systems with the Lanczos and density matrix renormalization group (DMRG) methods. We identify an insulator-insulator phase transition from a band to a correlated insulator with simultaneous charge and bond-charge order. The transition point is characterized by the vanishing of the optical excitation gap while simultaneously the charge and spin gaps remain finite and equal. Indications for a possible second transition into a Mott-insulator phase are discussed.Comment: final for

Multiband tight-binding theory of disordered ABC semiconductor quantum dots: Application to the optical properties of alloyed CdZnSe nanocrystals

Zero-dimensional nanocrystals, as obtained by chemical synthesis, offer a broad range of applications, as their spectrum and thus their excitation gap can be tailored by variation of their size. Additionally, nanocrystals of the type ABC can be realized by alloying of two pure compound semiconductor materials AC and BC, which allows for a continuous tuning of their absorption and emission spectrum with the concentration x. We use the single-particle energies and wave functions calculated from a multiband sp^3 empirical tight-binding model in combination with the configuration interaction scheme to calculate the optical properties of CdZnSe nanocrystals with a spherical shape. In contrast to common mean-field approaches like the virtual crystal approximation (VCA), we treat the disorder on a microscopic level by taking into account a finite number of realizations for each size and concentration. We then compare the results for the optical properties with recent experimental data and calculate the optical bowing coefficient for further sizes

The physics of dynamical atomic charges: the case of ABO3 compounds

Based on recent first-principles computations in perovskite compounds, especially BaTiO3, we examine the significance of the Born effective charge concept and contrast it with other atomic charge definitions, either static (Mulliken, Bader...) or dynamical (Callen, Szigeti...). It is shown that static and dynamical charges are not driven by the same underlying parameters. A unified treatment of dynamical charges in periodic solids and large clusters is proposed. The origin of the difference between static and dynamical charges is discussed in terms of local polarizability and delocalized transfers of charge: local models succeed in reproducing anomalous effective charges thanks to large atomic polarizabilities but, in ABO3 compounds, ab initio calculations favor the physical picture based upon transfer of charges. Various results concerning barium and strontium titanates are presented. The origin of anomalous Born effective charges is discussed thanks to a band-by-band decomposition which allows to identify the displacement of the Wannier center of separated bands induced by an atomic displacement. The sensitivity of the Born effective charges to microscopic and macroscopic strains is examined. Finally, we estimate the spontaneous polarization in the four phases of barium titanate.Comment: 25 pages, 6 Figures, 10 Tables, LaTe