Research Groups

RESEARCH UNIT: Theory and Simulation

Laboratory of Electronic Structure of Materials (LEEM)

We advance the state of the art in materials design by performing simulations for systems of technological relevance, and in turn by developing and implementing efficient computational methods.

Our group is at the forefront of the development of methods for materials simulation, and also holds a very strong position in their application to a wide range of problems, with a solid network of collaborations. The simulation expertise of the group extends from semi-empirical methods to first-principles approaches. In particular, we are one of the nodes developing the SIESTA program, and contribute to major international initiatives in scientific software.

We have world-class expertise in low-dimensional conductors, in which the particular topologies of the Fermi surface and its nesting properties are responsible for electronic instabilities. In oxide-based systems, we study novel functionalities while at the same time developing accurate modeling strategies to relate the microscopic and macroscopic views of response. Thermal transport at the nanoscale, including its control through external fields, is another relevant area of research.

Members

Prof. Enric Canadell - Research Professor
Dr. Alberto García - Research Scientist
Dr. Riccardo Rurali - Tenured Scientist
Dr. Massimiliano Stengel - ICREA Research Professor
Dr. Miquel Royo - Postdoctoral Researcher
Dr. Madhura Marathe - Postdoctoral Researcher
Dr. Konstantin Shapovalov - Postdoctoral Researcher
Dr. Alexander Edström - Postdoctoral Researcher
Dr. Emanuele Bosoni - Postdoctoral Researcher
Matteo Springolo - PhD Researcher
Asier Zabalo - PhD Researcher
Vladimir Dikan - PhD Researcher

Calculated Fermi surface (bottom left) and Lindhard response function (bottom right) for the (TMTSF)₂PF₆ molecular superconductor.

Achievements

For the first time we have calculated and analyzed the Lindhard response for a molecular metal based on the real crystal structure using a first-principles DFT approach. The evolution of the dimensionality and the nature of the 2kF spin density wave could be explained.

We generalized the treatment of long-range interatomic forces in insulators by incorporating the effect of dipole-quadrupole interactions. We demonstrated the importance of the latter in the interpolation of the phonon dispersion curves and electron-phonon matrix elements.

We have shown how strain can be used to control the competition between different metallic and semiconducting states of TaSe3 single layers on the basis of DFT calculations. The nanoscale rotational dynamics of a crystalline solid containing crowded layers with four independent rotors were studied using for the first time first-principles Car-Parrinello molecular dynamics simulations. The almost perfect agreement between the simulation results and variable-temperature 1H spin-lattice relaxation experiments allowed a full characterization of the rotational dynamics.

We rationalized the behavior of common dopant impurities in different crystal phases of III-V semiconductors, a relevant piece of information for the emerging field of crystal phase engineering.

A fully ab initio scheme to study phonon transport in the quasi-ballistic regime was developed, and we provided new insights into the lattice dynamics of WSe2 in a fruitful theory-experiment collaboration.

We have continued the development of the Siesta program and related utilities, and our contributions to scientific software initiatives, notably the Electronic Structure Library.

Publications

Using High Multipolar Orders to Reconstruct the Sound Velocity in Piezoelectrics from Lattice Dynamics
Miquel Royo, Konstanze R. Hahn, Massimiliano Stengel
Physical Review Letters 2020, 125, 217602, 10.1103/PhysRevLett.125.217602

Mechanical Softness of Ferroelectric 180 degrees Domain Walls
Christina Stefani; Louis Ponet; Konstantin Shapovalov; Peng Chen; Eric Langenberg; Darrell G.Schlom; Sergey Artyukhin; Massimiliano Stengel; Neus Domingo; Gustau Catalan
Physical Review X 2020, 10, 4, 41001, 10.1103/PhysRevX.10.041001

Phonon-limited electron mobility in Si, GaAs, and GaP with exact treatment of dynamical quadrupoles
Brunin, Guillaume; Coutada Miranda, Henrique Pereira; Giantomassi, Matteo; Royo, Miquel; Stengel, Massimiliano; Verstraete, Matthieu J.; Gonze, Xavier; Rignanese, Gian-Marco; Hautier, Geoffroy
Physical Review B 2020, 102, 9, 94308, 10.1103/PhysRevB.102.094308

Electron-Phonon beyond Frohlich: Dynamical Quadrupoles in Polar and Covalent Solids
Brunin, Guillaume; Coutada Miranda, Henrique Pereira; Giantomassi, Matteo; Royo, Miquel; Stengel, Massimiliano; Verstraete, Matthieu J.; Gonze, Xavier; Rignanese, Gian-Marco; Hautier, Geoffroy
Physical Review Letters 2020, 125, 13, 136601, 10.1103/PhysRevLett.125.136601

Visualization of moire superlattices
McGilly, Leo J.; Kerelsky, Alexander; Finney, Nathan R.; Shapovalov, Konstantin; Shih, En-Min; Ghiotto, Augusto; Zeng, Yihang; Moore, Samuel L.; Wu, Wenjing; Bai, Yusong; Watanabe, Kenji; Taniguchi, Takashi; Stengel, Massimiliano; Zhou, Lin; Hone, James; Zhu, Xiaoyang; Basov, Dmitri N.; Dean, Cory; Dreyer, Cyrus E.; Pasupathy, Abhay N.
Nature Nanotechnology 2020, 15, 7, 580, 10.1038/s41565-020-0708-3

Photoflexoelectric effect in halide perovskites
Shu, Longlong; Ke, Shanming; Fei, Linfeng; Huang, Wenbin; Wang, Zhiguo; Gong, Jinhui; Jiang, Xiaoning; Wang, Li; Li, Fei; Lei, Shuijin; Rao, Zhenggang; Zhou, Yangbo; Zheng, Ren-Kui; Yao, Xi; Wang, Yu; Stengel, Massimiliano; Catalan, Gustau
Nature Materials 2020 19 6 605 10.1038/s41563-020-0659-y

ABINIT: Overview and focus on selected capabilities
Romero, Aldo H.; Allan, Douglas C.; Amadon, Bernard; Antonius, Gabriel; Applencourt, Thomas; Baguet, Lucas; Bieder, Jordan; Bottin, Francois; Bouchet, Johann; Bousquet, Eric; Bruneval, Fabien; Brunin, Guillaume; Caliste, Damien; Cote, Michel; Denier, Jules; Dreyer, Cyrus; Ghosez, Philippe; Giantomassi, Matteo; Gillet, Yannick; Gingras, Olivier; Hamann, Donald R.; Hautier, Geoffroy; Jollet, Francois; Jomard, Gerald; Martin, Alexandre; Miranda, Henrique P. C.; Naccarato, Francesco; Petretto, Guido; Pike, Nicholas A.; Planes, Valentin; Prokhorenko, Sergei; Rangel, Tonatiuh; Ricci, Fabio; Rignanese, Gian-Marco; Royo, Miquel; Stengel, Massimiliano; Torrent, Marc; van Setten, Michiel J.; Van Troeye, Benoit; Verstraete, Matthieu J.; Wiktor, Julia; Zwanziger, Josef W.; Gonze, Xavier
Journal of Chemical Physics 2020, 152, 12, 124102, 10.1063/1.5144261

In Search of Chiral Molecular Superconductors: kappa-[(S,S)-DM-BEDT-TTF](2)ClO(4)Revisited
Mroweh, Nabil; Meziere, Cecile; Pop, Flavia; Auban-Senzier, Pascale; Alemany, Pere; Canadell, Enric; Avarvari, Narcis
Advanced Materials 2020, 32, 36, 2002811 10.1002/adma.202002811

Intermolecular Resonance Correlates Electron Pairs Down a Supermolecular Chain: Antiferromagnetism in K-Doped p-Terphenyl
Natalia A. Gadjieva, Péter Szirmai, Olivér Sági, Pere Alemany, Amymarie K. Bartholomew, Ilana Stone, Sergio Conejeros, Daniel W. Paley, Raúl Hernández Sánchez, Brandon Fowler, Samuel R. Peurifoy, Bálint Náfrádi, László Forró, Xavier Roy, Patrick Batail, Enric Canadell, Michael L. Steigerwald, and Colin Nuckolls
Journal of the American Chemical Society 2020, 142, 49, 20624-20630, 10.1021/jacs.0c05606

Conservation of structural arrangements and 3: 1 stoichiometry in a series of crystalline conductors of TMTTF, TMTSF, BEDT-TTF, and chiral DM-EDT-TTF with the oxo-bis[pentafluorotantalate(V)] dianion
Mroweh, Nabil; Meziere, Cecile; Allain, Magali; Auban-Senzier, Pascale; Canadell, Enric; Avarvari, Narcis
Chemical Science 2020, 11, 37, 10078-10091, 10.1039/d0sc03665j

Engineering Polar Oxynitrides: Hexagonal Perovskite BaWON2
Oro-Sole, Judith; Fina, Ignasi; Frontera, Carlos; Gazquez, Jaume; Ritter, Clemens; Cunquero, Marina; Loza-Alvarez, Pablo; Conejeros, Sergio; Alemany, Pere; Canadell, Enric; Fontcuberta, Josep; Fuertes, Amparo
Angewandte Chemie - International Edition 2020, 59, 42, 18395-18399, 10.1002/anie.202006519

Doping of III-V arsenide and phosphide wurtzite semiconductors
G. Giorgi, M. Amato, S. Ossicini, X. Cartoixà, E. Canadell, and R. Rurali
J. Phys. Chem. C 2020, 124, 49, 27203–27212, 10.1021/acs.jpcc.0c09391

Nanoscale rotational dynamics of four independent rotators confined in crowded crystalline layers
Rodriguez-Fortea, Antonio; Canadell, Enric; Wzietek, Pawel; Lemouchi, Cyprien; Allain, Magali; Zorina, Leokadiya; Batail, Patrick
Nanoscale 2020, 12, 15, 8294-8302, 10.1039/d0nr00858c

Bilayer Molecular Metal with a Polymeric Anion, beta-(CNB-EDT-TTF)(6) Ag similar to 7.95I similar to 9.19
Brotas, Graca; da Gama, Vasco; Santos, Isabel C.; Lopes, Elsa B.; Rabaca, Sandra; Paixao, Joseprime A.; Canadell, Enric; Almeida, Manuel
Crystal Growth & Design 2020, 20, 7, 4224-4227, 10.1021/acs.cgd.0c00524

Glycine Residue Twists HOMO center dot center dot center dot HOMO Interactions in a Molecular Conductor
El-Ghayoury, Abdelkrim; Meziere, Cecile; Simonov, Sergey; Zorina, Leokadiya; Auban-Senzier, Pascale; Alemany, Pere; Canadell, Enric; Batail, Patrick
Crystal Growth & Design 2020, 20, 5, 3546-3554, 10.1021/acs.cgd.0c00394

Weak localization competes with the quantum oscillations in a natural electronic superlattice: The case of Na-1.(5)(PO2)(4)(WO3)(20)
Kolincio, Kamil K.; Perez, Olivier; Canadell, Enric; Alemany, Pere; Duverger-Nedellec, Elen; Minelli, Arianna; Bosak, Alexei; Pautrat, Alain
Physical Review B 2020, 101, 16, 161117, 10.1103/PhysRevB.101.161117

Fermi surface electron-hole instability of the (TMTSF)(2)PF6 Bechgaard salt revealed by the first-principles Lindhard response function
Guster, Bogdan; Pruneda, Miguel; Ordejon, Pablo; Canadell, Enric; Pouget, Jean-Paul
Journal of Physics - Condensed Matter 2020, 32, 34, 345701, 10.1088/1361-648X/ab8522

Ab-initio studies of the optoelectronic structure of undoped and doped silicon nanocrystals and nanowires: the role of size, passivation, symmetry and phase
Ossicini, Stefano; Marri, Ivan; Amato, Michele; Palummo, Maurizia; Canadell, Enric; Rurali, Riccardo
Faraday Discussions 2020, 222, 0, 217-239, 10.1039/c9fd00085b

Combining chirality and hydrogen bonding in methylated ethylenedithiotetrathiafulvalene primary diamine precursors and radical cation salts
N. Mroweh. F. Pop, C. Mezière, M. Allain, P. AubanSenzier, N. Vanthuyne, P. Alemany, E. Canadell, N. Avarvari
Cryst. Growth & Design 2020, 20, 2516-2526 10.1021/acs.cgd.9b01665

Strain control of the competition between metallic and semiconducting states in single-layers of TaSe3
Silva-Guillen, Jose angel; Canadell, Enric
2D Materials 2020, 7, 2, 25038, 10.1088/2053-1583/ab72d9

Chiral Conducting MeEDTTTF and EtEDTTTF based Radical Cation Salts with the Perchlorate Anion
N. Mroweh, P. AubanSenzier, N. Vanthuyne, E. B. Lopes, M. Almeida, E. Canadell, N. Avarvari,
Crystals 2020, 10.3390/cryst10111069

New insights into the structural properties of kappa-(BEDT-TTF)(2)Ag-2 (CN)(3) spin liquid
Foury-Leylekian, Pascale; Ilakovac, Vita; Fertey, Pierre; Baledent, Victor; Milat, Ognjen; Miyagawa, Kazuya; Kanoda, Kazushi; Hiramatsu, Takaaki; Yoshida, Yukihiro; Saito, Gunzi; Alemany, Pere; Canadell, Enric; Tomic, Silvia; Pouget, Jean-Paul
Acta Crystallographica Section B - Structural Science Crystal Engineering and Materials 2020, 76, 581-590, 10.1107/S2052520620005545

Doping of III-V arsenide and phosphide wurtzite semiconductors
G. Giorgi, M. Amato, S. Ossicini, X. Cartoixà, E. Canadell, and R. Rurali
J. Phys. Chem. C 2020, 124, 49, 27203–27212, 10.1021/acs.jpcc.0c09391

Optimisation of the thermoelectric efficiency of zirconium trisulphide monolayers through unixial and biaxial strain
Saiz, Fernan; Carrete, Jesus; Rurali, Riccardo
Nanoscale Advances 2020, 2, 11, 5352-5361, 10.1039/d0na00518e

Quasiballistic phonon transport from first principles
Torres, Pol; Royo, Miquel; Lopez-Suarez, Miquel; Shiomi, Junichiro; Rurali, Riccardo
Physical Review B 2020, 102, 14, 144305, 10.1103/PhysRevB.102.144305

Probing Lattice Dynamics and Electronic Resonances in Hexagonal Ge and SixGe1-x Alloys in Nanowires by Raman Spectroscopy
de Matteis, Diego; De Luca, Marta; Fadaly, Elham M. T.; Verheijen, Marcel A.; Lopez-Suarez, Miquel; Rurali, Riccardo; Bakkers, Erik P. A. M.; Zardo, Ilaria
ACS Nano 2020, 14, 6, 6845-6856, 10.1021/acsnano.0c00762

Strain Engineering of the Electronic and Thermoelectric Properties of Titanium Trisulphide Monolayers
F. Saiz and R. Rurali
Nano Express 2020, 1, 010026, 10.1088/2632-959X/ab89ea

Anisotropic Thermal Conductivity in Few-Layer and Bulk Titanium Trisulphide from First Principles
Saiz, Fernan; Carrete, Jesus; Rurali, Riccardo
Nanomaterials 2020, 10, 4, 704, 10.3390/nano10040704

Experimental demonstration of the suppression of optical phonon splitting in 2D materials by Raman spectroscopy
Marta De Luca, Xavier Cartoixà, David I Indolese, Javier Martín-Sánchez, Kenji Watanabe, Takashi Taniguchi, Christian Schönenberger, Rinaldo Trotta, Riccardo Rurali and Ilaria Zardo
2D Materials 2020, 7, 3, 10.1088/2053-1583/ab81b1

New insights in the lattice dynamics of monolayers, bilayers, and trilayers of WSe2 and unambiguous determination of few-layer-flakes' thickness
De Luca, Marta; Cartoixa, Xavier; Martin-Sanchez, Javier; Lopez-Suarez, Miquel; Trotta, Rinaldo; Rurali, Riccardo; Zardo, Ilaria
2D Materials 2020, 7, 2, 025004, 10.1088/2053-1583/ab5dec

Siesta: Recent developments and applications
Garcia, Alberto; Papior, Nick; Akhtar, Arsalan; Artacho, Emilio; Blum, Volker; Bosoni, Emanuele; Brandimarte, Pedro; Brandbyge, Mads; Cerda, J., I; Corsetti, Fabiano; Cuadrado, Ramon; Dikan, Vladimir; Ferrer, Jaime; Gale, Julian; Garcia-Fernandez, Pablo; Garcia-Suarez, V. M.; Garcia, Sandra; Huhs, Georg; Illera, Sergio; Korytar, Richard; Koval, Peter; Lebedeva, Irina; Lin, Lin; Lopez-Tarifa, Pablo; Mayo, Sara G.; Mohr, Stephan; Ordejon, Pablo; Postnikov, Andrei; Pouillon, Yann; Pruneda, Miguel; Robles, Roberto; Sanchez-Portal, Daniel; Soler, Jose M.; Ullah, Rafi; Yu, Victor Wen-zhe; Junquera, Javier
Journal of Chemical Physics 2020, 152, 20, 10.1063/5.0005077

The CECAM electronic structure library and the modular software development paradigm
Oliveira, Micael J. T.; Papior, Nick; Pouillon, Yann; Blum, Volker; Artacho, Emilio; Caliste, Damien; Corsetti, Fabiano; de Gironcoli, Stefano; Elena, Alin M.; Garcia, Alberto; Garcia-Suarez, Victor M.; Genovese, Luigi; Huhn, William P.; Huhs, Georg; Kokott, Sebastian; Kucukbenli, Emine; Larsen, Ask H.; Lazzaro, Alfio; Lebedeva, Irina, V; Li, Yingzhou; Lopez-Duran, David; Lopez-Tarifa, Pablo; Lueders, Martin; Marques, Miguel A. L.; Minar, Jan; Mohr, Stephan; Mostofi, Arash A.; O'Cais, Alan; Payne, Mike C.; Ruh, Thomas; Smith, Daniel G. A.; Soler, Jose M.; Strubbe, David A.; Tancogne-Dejean, Nicolas; Tildesley, Dominic; Torrent, Marc; Yu, Victor Wen-zhe
Journal of Chemical Physics 2020, 153, 2, 24117, 10.1063/5.0012901

ELSI — An Open Infrastructure for Electronic Structure Solvers
Yu, Victor Wenzhe; Carmen Campos; William Dawson; Alberto García; Ville Havu; Ben Hourahine; William P. Huhn; et al
Computer Physics Communications 2020, 256, 107459 10.1016/j.cpc.2020.107459

Main projects

Hierarchical multiscale modeling of flexoelectricity and related materials properties from first principles (MULTIFLEXO)
ERC Consolidator Grant
M. Stengel
2017-2022 // 1.470.000 €

Phase and Antiphase Boundaries and Domains in Antiferroelectrics (PHABADA)
MINECO (proyectos I+D+i excelencia)
M. Stengel and G. Catalan (coordinated project between ICMAB and ICN2, MS is PI of the ICMAB node)
2016-2020 // 50.000 € + 1 FPI Ph.D. fellowship for the ICMAB node

MaX Materials design at the eXascale ‐
EU H2020 EINFRA 2018-1 (ref. 824143)
E. Molinari (Coordinator); A. García (PI at CSIC)
12/2018-11/2021 // 250.000 €

Siesta and its interoperability for the new challenges in atomistic simulations (SIESTA-CSIC)
Spanish MICINN (PGC2018-096955-B-C44)
Alberto García and Eduardo Hernández
2019-2022 // 119.790 €

Interoperable Material-to-Device simulation box for disruptive electronics (INTERSECT)
EU H2020-NMBP-TO-IND-2018 (ref. 814487)
A. Calzolari (Coordinator); A. García (PI at CSIC)
1/2019-1/2022 // 25.000 €

Battery Interface Genome -- Materials Acceleration Platform (BIGMAP)
EU H2020 - GA 957189
Tejs Vegge (coordinator); R. Palacín (PI at CSIC)
9/2020-8/2023

Strain-driven phononic and bandgap engineering of Si and Ge nanowires
i-LINK, Consejo Superior de Investigaciones Científicas (LINKA20047)
R. Rurali
05/2019-12/2021 // 10.000 €

Thermal and electronic transport in inorganic-organic thermoelectric superlattices (TELIOTES)
Marie Sklodowska-Curie individual fellowships (H2020-MSCA-IF-2017), European Union
(793726). Principal Investigator: R. Rurali (158 k€).; fellow Fernán Saiz Poyatos.
10/2018-09/2020.

Towards Next Generation Nanoscale Thermal Sensing
Proyectos de I+D “Excelencia”, Ministerio de Economía, Industria y Competitividad (MAT2017-90024-P). PI: J. S. Reparaz
01/2018-12/2020 // 130.000 €