arXiv subjects

Enric Canadell

Publications and source records attributed to Enric Canadell.

At least 19 recordsLinked to original sources

arXiv2024

The rich structural, electronic and bonding landscape of 1$T$-type TaTe$_2$ single-layers

Charge density waves (CDW) in single-layer 1$T$-MTe$_2$ (M= Nb, Ta) recently raised large attention because of the contrasting structural and physical behavior with the sulfide and selenide analogues. A first-principles study of fourteen different 1$T$-type TaTe$_2$ single-layers is reported. The importance of Te to Ta electron transfer and multicenter metal-metal bonding in stabilizing different structural modulations is highlighted. Analysis of the electronic structure of the optimized structures provides a rationale for what distinguishes 1$T$-TaTe$_2$ from the related disulfide and diselenide, what are the more stable structural modulations for 1$T$-type TaTe$_2$ single-layers, the possible role of Fermi surface nesting on some of these CDW instabilities, how the CDW affects the metallic properties of the non-distorted lattice and the possibility that some of these CDW phases exhibit exotic properties. All CDW phases studied exhibit band structures typical of metallic systems although some exhibit both very flat and dispersive bands at the Fermi level so that Mott effects could develop; one of the (4$\times$4) phases studied exhibits a Dirac cone at the Fermi level.

cond-mat.mtrl-sci↗

arXiv2023

Metastable polymorphic phases in monolayer TaTe2

Polymorphic phases and collective phenomena - such as charge density waves (CDWs) - in transition metal dichalcogenides (TMDs) dictate the physical and electronic properties of the material. Most TMDs naturally occur in a single given phase, but the fine-tuning of growth conditions via methods like molecular beam epitaxy (MBE) allows to unlock otherwise inaccessible polymorphic structures. Exploring and understanding the morphological and electronic properties of new phases of TMDs is an essential step to enable their exploitation in technological applications. Here, we use scanning tunneling microscopy to map MBE-grown monolayer TaTe2. We report the first observation of the 1H polymorphic phase, coexisting with the 1T, and demonstrate that their relative coverage can be controlled by adjusting synthesis parameters. Several super-periodic structures, compatible with CDWs, are observed to coexist on the 1T phase. Finally, we provide theoretical insight on the delicate balance between Te...Te and Ta-Ta interactions that dictates the stability of the different phases. Our findings demonstrate that TaTe2 is an ideal platform to investigate competing interactions, and indicate that accurate tuning of growth conditions is key to accessing metastable states in TMDs.

cond-mat.mtrl-sci↗

arXiv2021

Competition between Ta-Ta and Te-Te bonding leading to the commensurate charge density wave in TaTe4

The origin of the charge density wave in TaTe$_4$ is discussed on the basis of a first-principles DFT analysis of the Fermi surface, electron-hole response function, phonon band structure of the average structure and structural optimization of the modulated phase. Analysis of the band structure and Fermi surface of the average structure clearly proves that despite the presence of TaTe$_4$ chains in the crystal structure, TaTe$_4$ is in fact a 3D material as far as the electronic structure near the Fermi level is concerned. A Fermi surface nesting mechanism is dismissed as the origin of the 2$a\times2a\times3c$ structural modulation. The optimized 2$a$\xone2$a$\xone3$c$ structure, which is found to be the more stable modulation in agreement with the experimental observations, can be obtained directly from a soft-phonon mode computed for the undistorted structure. Our results suggest that the driving force for the distortion is the maximization of Ta-Ta metal-metal bonding subject to inducing the minimum bonding decrease in the Te sublattice.

cond-mat.mtrl-sci↗

arXiv2020

Electron-hole response function of transition metal trichalcogenides NbSe$_3$ and monoclinic-TaS$_3$

NbSe$_3$ and monoclinic-TaS$_3$ ($m$-TaS$_3$) are quasi-1D metals containing three different types of chains and undergoing two different charge density wave (CDW) Peierls transitions at T$_{P_1}$ and T$_{P_2}$. The nature of these transitions is discussed on the basis of first-principles DFT calculation of their electron-hole Lindhard response function. As a result of stronger inter-chain interactions the Fermi surface (FS) and Lindhard function of NbSe$_3$ are considerably more complex than those for $m$-TaS$_3$; however a common scenario can be put forward to rationalize the results. The intra-chain inter-band nesting processes dominate the strongest response for both type I and type III chains of the two compounds. Two well-defined maxima of the Lindhard response for NbSe$_3$ are found with the (0$a$*, 0$c$*) and (1/2$a$*, 1/2$c$*) transverse components at T$_{P_1}$ and T$_{P_2}$, respectively, whereas the second maximum is not observed for $m$-TaS$_3$ at T$_{P2}$. Analysis of the different inter-chain coupling mechanisms leads to the conclusion that FS nesting effects are only relevant to set the transverse $a$* components in NbSe$_3$. For the transverse coupling along $c$* in NbSe$_3$ and along both $a$* and $c$* for $m$-TaS$_3$, one must take into account the strongest inter-chain Coulomb coupling mechanism. Phonon spectrum calculations show the formation of a giant 2$k_F$ Kohn anomaly in $m$-TaS$_3$. All these results support the weak coupling scenario for the Peierls transition of transition metal trichalcogenides.

cond-mat.mtrl-sci↗

arXiv2020

Strain control of the competition between metallic and semiconducting states in single-layers of TaSe$_3$

TaSe$_3$ is a metallic layered material whose structure is built from TaSe$_3$ trigonal prismatic chains. In this work we report a first-principles density functional theory study of TaSe$_3$ single-layers and we find that, despite the existence of non negligible Se...Se interlayer interactions, TaSe$_3$ single layers are found to be metallic. However, an interesting competition between metallic and semiconducting states is found under the effect of strain. The single-layers keep the metallic behaviour under biaxial strain although the nature of the hole carriers changes. In contrast, uniaxial strain along the chains direction induces the stabilization of a semiconducting state. Potential electronic instabilities due to Fermi surface nesting are found for single-layers under either biaxial strain or uniaxial strain along the long (inter-chain) axis of the layers. Bilayers and trilayers have also been considered. The structural and electronic features behind these unexpected observations are analyzed.

cond-mat.mtrl-sci↗

arXiv2020

Weak localization competes with the quantum oscillations in a natural electronic superlattice: the case of Na$_{1.5}$(PO$_2$)$_4$(WO$_3$)$_{20}$

We report an investigation of the combined structural and electronic properties of the bronze Na$_{1.5}$(PO$_{2}$)$_{4}$(WO$_{3}$)$_{20}$. Its low dimensional structure and possible large reconstruction of the Fermi surface due to charge density wave instability makes this bulk material a natural superlattice with a reduced number of carriers and Fermi energy. Signatures of multilayered 2D electron weak localization are consequently reported, with an enhanced influence of quantum oscillations. A crossover between these two antagonistic entities previously observed only in genuine low dimensional materials and devices, is shown to occur in a bulk crystal due to its hidden 2D nature.

cond-mat.str-el↗

arXiv2018

Polymorphism in Bi-based perovskite oxides: a first-principles study

Under normal conditions, bulk crystals of BiScO$_3$ , BiCrO$_3$, BiMnO$_3$, BiFeO$_3$, and BiCoO$_3$ present three very different variations of the perovskite structure: an antipolar phase, a rhombohedral phase with a large polarization along the space diagonal of the pseudocubic unit cell, and a supertetragonal phase with even larger polarization. With the aim of understanding the causes for this variety, we have used a genetic algorithm to search for minima in the surface energy of these materials. Our results show that the number of these minima is very large when compared to that of typical ferroelectric perovskites like BaTiO$_3$ and PbTiO$_3$ , and that a fine energy balance between them results in the large structural differences seen. As byproducts of our search we have identified charge-ordering structures with low energy in BiMnO$_3$ , and several phases with energies that are similar to that of the ground state of BiCrO$_3$. We have also found that a inverse supertetragonal phase exists in bulk, likely to be favored in films epitaxially grown at large values of tensile misfit strain.

cond-mat.mtrl-sci↗

arXiv2018

Meta-screening and permanence of polar distortion in metallized ferroelectrics

Ferroelectric materials are characterized by a spontaneous polar distortion. The behavior of such distortions in the presence of free charge is the key to the physics of metallized ferroelectrics in particular, and of structurally-polar metals more generally. Using first-principles simulations, here we show that a polar distortion resists metallization and the attendant suppression of long-range dipolar interactions in the vast majority of a sample of 11 representative ferroelectrics. We identify a meta-screening effect, occurring in the doped compounds as a consequence of the charge rearrangements associated to electrostatic screening, as the main factor determining the survival of a non-centrosymmetric phase. Our findings advance greatly our understanding of the essentials of structurally-polar metals, and offer guidelines on the behavior of ferroelectrics upon field-effect charge injection or proximity to conductive device elements.

cond-mat.mtrl-sci↗

arXiv2015

Non-Lifshitz-Kosevich field-and temperature-dependent amplitude of quantum oscillations in the quasi-two dimensional metal $θ$-(ET) 4 ZnBr 4 (C 6 H 4 Cl 2 )

According to band structure calculations, the Fermi surface of the quasi-two dimensional metal $θ$-(ET) 4 ZnBr 4 (C 6 H 4 Cl 2) illustrates the linear chain of coupled orbits model. Accordingly, de Haas-van Alphen oscillations spectra recorded in pulsed magnetic field of up to 55 T evidence many Fourier components, the frequency of which are linear combinations of the frequencies relevant to the closed $α$ and the magnetic breakdown $β$ orbits. The field and temperature dependence of these component's amplitude are quantitatively accounted for by analytic calculations including, beyond the Lifshitz-Kosevich formula, second order terms in damping factors due to the oscillation of the chemical potential as the magnetic field varies. Whereas these second order terms are negligible for the orbits $α$, $β$ and 2$β$ -- $α$, they are solely responsible for the 'forbidden orbit' $β$ -- $α$ and its harmonic and have a significant influence on Fourier components such as 2$α$ and $β$ + $α$, yielding strongly non-Lifshitz-Kosevich behaviour in the latter case.

cond-mat.str-el↗

arXiv2014

De Haas-van Alphen oscillations in the compensated organic metal alpha-'pseudo-kappa'-(ET)4H3O[Fe(C2O4)3].(C6H4Br2)

Field-, temperature- and angle-dependent Fourier amplitude of de Haas-van Alphen (dHvA) oscillations are calculated for compensated two-dimensional (2D) metals with textbook Fermi surface (FS) composed of one hole and two electron orbits connected by magnetic breakdown. It is demonstrated that, taking into account the opposite sign of electron and hole orbits, a given Fourier component involves combination of several orbits, the contribution of which must be included in the calculations. Such FS is observed in the strongly 2D organic metal alpha-'pseudo-kappa'-(ET)4H3O[Fe(C2O4)3].(C6H4Br2), dHvA oscillations of which have been studied up to 55 T for various directions of the magnetic field with respect to the conducting plane. Calculations are in good quantitative agreement with the data.

cond-mat.str-el↗

arXiv2013

Onsager phase factor of quantum oscillations in the organic metal theta-(BEDT-TTF)4CoBr4(C6H4Cl2)

De Haas-van Alphen oscillations are studied for Fermi surfaces illustrating the Pippard's model, commonly observed in multiband organic metals. Field- and temperature-dependent amplitude of the various Fourier components, linked to frequency combinations arising from magnetic breakdown between different bands, are considered. Emphasis is put on the Onsager phase factor of these components. It is demonstrated that, in addition to the usual Maslov index, field-dependent phase factors must be considered to precisely account for the data at high magnetic field. We present compelling evidence of the existence of such contributions for the organic metal theta-(BEDT-TTF)4CoBr4(C6H4Cl2).

cond-mat.str-el↗

arXiv2012

Quantum oscillations in the linear chain of coupled orbits: the organic metal with two cation layers theta-(ET)(4)CoBr(4)(C(6)H(4)Cl(2))

Analytical formulae for de Haas-van Alphen (dHvA) oscillations in linear chain of coupled two-dimensional (2D) orbits (Pippard's model) are derived systematically taking into account the chemical potential oscillations in magnetic field. Although corrective terms are observed, basic (alpha) and magnetic breakdown-induced (beta and 2beta - alpha) orbits can be accounted for by the Lifshits-Kosevich (LK) and Falicov-Stachowiak semiclassical models in the explored field and temperature ranges. In contrast, the 'forbidden orbit' beta - alpha amplitude is described by a non-LK equation involving a product of two classical orbit amplitudes. Furthermore, strongly non-monotonic field and temperature dependence may be observed for the second harmonics of basic frequencies such as 2alpha and the magnetic breakdown orbit beta + alpha, depending on the value of the spin damping factors. These features are in agreement with the dHvA oscillation spectra of the strongly 2D organic metal theta- theta-(ET)(4)CoBr(4)(C(6)H(4)Cl(2)).

cond-mat.str-el↗

arXiv2011

The metallic transport of (TMTSF)_2X organic conductors close to the superconducting phase

Comparing resistivity data of quasi-one dimensional superconductors (TMTSF)_2PF_6 and (TMTSF)_2ClO_4 along the least conducting c*-axis and along the high conductivity a -axis as a function of temperature and pressure, a low temperature regime is observed in which a unique scattering time governs transport along both directions of these anisotropic conductors. However, the pressure dependence of the anisotropy implies a large pressure dependence of the interlayer coupling. This is in agreement with the results of first-principles DFT calculations implying methyl group hyperconjugation in the TMTSF molecule. In this low temperature regime, both materials exhibit for rc a temperature dependence aT + bT^2. Taking into account the strong pressure dependence of the anisotropy, the T-linear rc is found to correlate with the suppression of the superconducting Tc, in close analogy with ra data. This work is revealing the domain of existence of the 3D coherent regime in the generic (TMTSF)_2X phase diagram and provides further support for the correlation between T-linear resistivity and superconductivity in non-conventional superconductors.

cond-mat.str-el↗

arXiv2011

Temperature- and pressure-dependent metallic states in (BEDT-TTF)8[Hg4Br12(C6H5Br)2]

Temperature-driven metal-insulator and pressure-driven insulator-metal transitions observed in(BEDT-TTF)8[Hg4X12(C6H5Y)2]] with X = Y = Br are studied through band structure calculations based on X-ray crystal structure determination and Shubnikov-de Haas (SdH) oscillations spectra, respectively. In connection with chemical pressure effect, the transition, which is not observed for X = Cl, is due to gap opening linked to structural changes as the temperature decreases. Even though many body interactions can be inferred from the pressure dependence of the SdH oscillations spectra, all the data can be described within a Fermi liquid picture.

cond-mat.str-el↗

arXiv2009

Indication for the coexistence of closed orbit and quantum interferometer with the same cross section in the organic metal (ET)4(H3O)[Fe(C2O4)3].C6H4Cl2: Persistence of SdH oscillations above 30 K

Shubnikov-de Haas (SdH) and de Haas-van Alphen (dHvA) oscillations spectra of the quasi-two dimensional charge transfer salt $β$"-(ET)$_4$(H$_3$O)[Fe(C$_2$O$_4$)$_3$]$\cdot$C$_6$H$_4$Cl$_2$ have been investigated in pulsed magnetic fields up to 54 T. The data reveal three basic frequencies F$_a$, F$_b$ and F$_{b - a}$, which can be interpreted on the basis of three compensated closed orbits at low temperature. However a very weak thermal damping of the Fourier component F$_b$, with the highest amplitude, is evidenced for SdH spectra above about 6 K. As a result, magnetoresistance oscillations are observed at temperatures higher than 30 K. This feature, which is not observed for dHvA oscillations, is in line with quantum interference, pointing to a Fermi surface reconstruction in this compound.

cond-mat.str-el↗

arXiv2009

Comment on "Direct evidence for hidden one-dimensional Fermi surface of hexagonal K0.25WO3"

We comment a recent work titled "Direct evidence for hidden one-dimensional Fermi surface of hexagonal K0.25WO3". In this paper the authors report photoemission and theoretical results on the K0.25WO3 system which led them to propose that a Charge Density Wave (CDW), associated with hidden one-dimensional bands, was responsible for the well known resistivity anomaly in such system. In the present comment we report the results of a first principles density functional theory (DFT) study showing that there are no one-dimensional bands as suggested by these authors.

physics.chem-ph↗

arXiv2008

Shubnikov-de Haas oscillations spectrum of the strongly correlated quasi-2D organic metal (ET)8[Hg4Cl12(C6H5Br)]2 under pressure

Pressure dependence of the Shubnikov-de Haas (SdH) oscillations spectra of the quasi-two di- mensional organic metal (ET)8[Hg4Cl12(C6H5Br)]2 have been studied up to 1.1 GPa in pulsed magnetic fields of up to 54 T. According to band structure calculations, its Fermi surface can be regarded as a network of compensated orbits. The SdH spectra exhibit many Fourier components typical of such a network, most of them being forbidden in the framework of the semiclassical model. Their amplitude remains large in all the pressure range studied which likely rules out chemical potential oscillation as a dominant contribution to their origin, in agreement with recent calculations relevant to compensated Fermi liquids. In addition to a strong decrease of the magnetic breakdown field and effective masses, the latter being likely due to a reduction of the strength of electron correlations, a sizeable increase of the scattering rate is observed as the applied pressure increases. This latter point, which is at variance with data of most charge transfer salts is discussed in connection with pressure-induced features of the temperature dependence of the zero-field interlayer resistance

cond-mat.str-el↗

arXiv2008

Understanding the Unique Structural and Electronic Properties of SrFeO2

We report a first-principles study of SrFeO$_2$, an infinite-layer oxide with Fe atoms in a perfect square-planar coordination down to essentially 0 K. Our results reveal this striking behavior relies on the double occupation of the 3$d_{z^2}$ orbitals of high-spin Fe$^{2+}$. Such an electronic state results from the hybridization of iron's 3$d_{z^2}$ and 4$s$ orbitals, which enables a large reduction of the intra-atomic exchange splitting of the $z^2$ electrons. The generality of the phenomenon is discussed.

cond-mat.mtrl-sci↗