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1. Tailoring topological order and {\pi}-conjugation to engineer quasi-metallic polymers

Author

Cirera, B., Sánchez-Grande, A., de la Torre, B., Santos, J., Edalatmanesh, S., Rodríguez-Sánchez, E., Lauwaet, K., Mallada-Faes, B., Zbořil, R., Miranda, R., Gröning, O., Jelínek, P., Martín, N., and Écija, D.

Subjects
Condensed Matter - Mesoscale and Nanoscale Physics, Condensed Matter - Materials Science
Abstract

Topological band theory provides a conceptual framework to predict or even engineer robust metallic states at the boundaries of topologically distinct phases. The bulk-boundary correspondence requires that a topological electronic phase transition between two insulators must proceed via closing of the electronic gap. Therefore, it can provide a conceptual solution to the instability of metallic phases in {\pi}-conjugated 1D polymers. In this work we predict and demonstrate that a clever design and on-surface synthesis of polymers consisting of 1D linearly bridged polyacene moieties, can position the resulting polymer near the topological transition from a trivial to a non-trivial quantum phase featuring a very narrow bandgap with in-gap zero-energy edge-states at the topologically non-trivial phase. We also reveal the fundamental connection between topological classes and electronic transformation of 1D {\pi}-conjugated polymers.

Published
2019
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6. Dysprosium-directed metallosupramolecular network on graphene/Ir(111)

Author

Moreno D., Cirera B., Parreiras S.O., Urgel J.I., Giménez-Agulló N., Lauwaet K., Gallego J.M., Galán-Mascarós J.R., Martínez J.I., Ballester P., Miranda R., Écija D. and This project has received funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement no. 766555). This work has also been financed by the Spanish Ministerio de Ciencia, Innovación y Universidades (projects PGC 2018-098613-B-C21, SpOrQuMat, MAT2017-85089-C2-1-R) and the Comunidad de Madrid (projects S2018/NMT-4321, NanoMagCost). IMDEA Nanociencia thanks support from the ‘‘Severo Ochoa’’ Programme for Centers of Excellence in R&D (MINECO, Grant SEV-2016-0686).

Published
2021

7. Unravelling the Open-Shell Character of Peripentacene on Au(111)

Author

Sánchez-Grande A., Urgel J.I., Veis L., Edalatmanesh S., Santos J., Lauwaet K., Mutombo P., Gallego J.M., Brabec J., Beran P., Nachtigallová D., Miranda R., Martín N., Jelínek P., Écija D. and This project has received funding from Comunidad de Madrid [projects QUIMTRONIC-CM (Y2018/NMT-4783), MAD2D, and NanoMagCost], and Ministerio de Ciencia, Innovación y Universidades (projects SpOrQuMat, CTQ2017-83531-R, PID2019-108532GB-I00, and CTQ2016-81911-REDT). IMDEA Nanociencia is appreciative of support from the 'Severo Ochoa' Programme for Centers of Excellence in R&D (MINECO, grant SEV-2016-0686). We acknowledge support from the Praemium Academie of the Academy of Science of the Czech Republic, the GACR 18-09914S, and the CzechNanoLab Research Infrastructure supported by MEYS CR (LM2018110). This study has also been part of the research project RVO of the IOCB of the CAS (61388963). J.I.U. thanks the JCB Atracción de Talento program from the Comunidad de Madrid (contract no. IND-12535). L.V. acknowledges support from the Czech Science Foundation (18-18940Y) and the Center for Scalable and Predictive Methods for Excitation and Correlated Phenomena (SPEC), which was funded by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, the Division of Chemical Sciences, Geosciences, and Biosciences. This work was also supported by the Czech Ministry of Education, Youth, and Sports from the Large Infrastructures for Research, Experimental Development, and Innovations project, e-Infrastructure CZ-LM2018140.

Published
2021

10. Tracking the Light-Induced Excited-State Dynamics and Structural Configurations of an Extraordinarily Long-Lived Metastable State at Room Temperature

Author

Iglesias S., Gamonal A., Abudulimu A., Picón A., Carrasco E., Écija D., Liu C., Luer L., Zhang X., Costa J.S., Moonshiram D. and 'This work was supported by the Severo Ochoa Excellence program (SEV?2016?0686) from the Instituto IMDEA Nanociencia, the Acciones de Dinamización 'Europa Investigacion' grant (EIN2019?103399), and the Spanish Ministerio de Ciencia, Innovación y Universidades grant (PID2019?111086RA?I00). The research leading to part of the results has further been supported by the project CALIPSOplus under the Grant Agreement 730872 from the EU Framework Programme for Research and Innovation HORIZON 2020. A.P. and S.I. acknowledge funding from Comunidad de Madrid through TALENTO grant ref. 2017?T1/IND?5432 and Ayudante de Investigación grant ref. PEJ?2019?AI/AMB?13038. The DFT calculations and XANES simulations have been performed in the Scientific Computing Center?Autonomous University of Madrid (CatDesignProject, PI: D. Moonshiram)',' thanks to CPU time and other resources granted by the institution.. J.S.C. is grateful to the Spanish MINECO for financial support through National Research Project (CTQ2016?80635?P), the Ramón y Cajal Research program (RYC?2014?16866), and the Comunidad Autónoma de Madrid (PEJD?2017?PRE/IND?4037) for funding support. We would like to thank the XALOC?ALBA synchrotron source under the project no. 2018012561, for help with single?crystal diffraction measurements. In addition, this research used resources of the XAFS beamline at the Elettra light source (Italy), Petra P64 beamline at DESY, a member of the Helmholtz Association (HGF) (Germany), and the Advanced Photon Source (APS, Beamline 11 ID?D) at Argonne National Laboratory (USA). The APS is a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE?AC02?06CH11357. The laser system at 11 ID?D at APS was funded through New Facility and Midscale Instrumentation grants to Chemical Sciences and Engineering Division, Argonne National Laboratory (PI: Prof. Dr. Lin X Chen). We also thank Dr. Wolfgang Caliebe and Dr. Luca Olivi for help with experiments at Petra P64 (Germany) and the XAFS beamline at ELETTRA (Italy) respectively.'

Published
2020

11. Metal-Coordination Network vs Charge Transfer Complex: The Importance of the Surface

Author

Rodr?guez-Fernández J., Lauwaet K., Écija D., Otero R., Miranda R., Gallego J.M. and This work has been financed by the Spanish Ministerio de Economa, Industria y Competitividad (Projects FIS2016-78591-C3-1-R and PGC2018-098613-B-C21) and the Comunidad de Madrid (Projects S2013/MT-2850 and P2018/NMT-4321).

Published
2020

12. Diradical Organic One-Dimensional Polymers Synthesized on a Metallic Surface

Author

Sánchez-Grande A., Urgel J.I., Cahlík A., Santos J., Edalatmanesh S., Rodríguez-Sánchez E., Lauwaet K., Mutombo P., Nachtigallová D., Nieman R., Lischka H., de la Torre B., Miranda R., Gröning O., Martín N., Jelínek P., Écija D. and This work has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programme (grant agreement No 766555), the Comunidad de Madrid [project QUIMTRONIC-CM (Y2018/NMT-4783), MAD2D and NanoMagCost] and the Spanish MINECO (projects FIS 2013-40667-P, FIS 2015-67287-P, SpOrQuMat, CTQ2018-102815-REDT, CTQ2017-83531-R and CTQ2016-81911-REDT). IMDEA Nanociencia thanks for support from the ?Severo Ochoa? Programme for Centers of Excellence in R&D (MINECO, Grant SEV-2016-0686). This work was also a part of the research project RVO (61388963) of the IOCB of the CAS (D.N.). We are grateful for support from the School of Pharmaceutical Science and Technology (SPST), Tianjin University, Tianjin, China, for computer time on the SPST computer cluster Arran. J.I.U thanks the JCB Atracci?n de Talento program from Comunidad de Madrid (contract no. IND-12535).

Published
2020

13. On-surface synthesis of doubly-linked one-dimensional pentacene ladder polymers

Author

Biswas K., Urgel J.I., Sánchez-Grande A., Edalatmanesh S., Santos J., Cirera B., Mutombo P., Lauwaet K., Miranda R., Jelínek P., Martín N., Écija D. and We acknowledge the Comunidad de Madrid [project QUIMTRONIC-CM (Y2018/NMT-4783)], the EC FP7-PEOPLE-2011-COFUND AMAROUT II, the Spanish Ramón y Cajal programme (no. RYC-2012-11133), the Spanish MINECO (projects FIS 2013-40667-P, FIS 2015-67287-P) and Ministerio de Ciencia, Innovación y Universidades (project SpOrQuMat) and the Comunidad de Madrid (projects MAD2D, NanoMagCost). The MINECO of Spain (projects CTQ2017-83531-R and CTQ2016-81911-REDT) is also acknowledged. IMDEA Nanociencia thanks support from the ‘‘Severo Ochoa’’ Programme for Centers of Excellence in R&D (MINECO, Grant SEV-2016-0686). P. J. acknowledges support from Praemium Academie of the Academy of Science of the Czech Republic, GACR 18-09914S.

Published
2020

14. Tailoring π-conjugation and vibrational modes to steer on-surface synthesis of pentalene-bridged ladder polymers

Author

de la Torre B., Mat?j A., Sánchez-Grande A., Cirera B., Mallada B., Rodríguez-Sánchez E., Santos J., Mendieta-Moreno J.I., Edalatmanesh S., Lauwaet K., Otyepka M., Medve? M., Buendía Á., Miranda R., Martín N., Jelínek P., Écija D. and We acknowledge financial support from the Comunidad de Madrid [project QUIMTRONIC-CM (Y2018/NMT-4783)]. This project has received funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (grant agreement No 766555). MINECO of Spain (projects CTQ2017-83531-R and RED2018-102815-T) is also acknowledged. IMDEA Nanociencia thanks support from the 'Severo Ochoa' Program for Centers of Excellence in R&D (MINECO, Grant SEV-2016-0686). We also acknowledge support from Praemium Academie of the Academy of Science of the Czech Republic, GACR 18-09914S and Operational Program Research, Development and Education financed by European Structural and Investment Funds and the Czech Ministry of Education, Youth and Sports (Project No. CZ.02.1.01/0.0/0.0/16_019/0000754). A.M. and B.M. acknowledge the support from the Internal Student Grant Agency of the Palacký University in Olomouc, Czech Republic IGA_PrF_2020_022 and IGA PrF 2020_034.

Published
2020

16. On-Surface Synthesis of Gold Porphyrin Derivatives via a Cascade of Chemical Interactions: Planarization, Self-Metalation, and Intermolecular Coupling

Author

Cirera B., De La Torre B., Moreno D., Ondrá?ek M., Zbo?il R., Miranda R., Jelínek P., Écija D. and Work supported by the ERC Consolidator Grant ELECNANO (n° 766555), the EC FP7-PEOPLE-2011-COFUND AMAR-OUT II program, the Spanish Ramo? and Cajal Program (n° RYC-2012-11133), the Spanish Ministerio de Economiá y Competitividad (Projects FIS 2013-40667-P and FIS 2015- 67287-P), the Comunidad de Madrid [Projects Y2018/NMT-4783 (QUIMTRONIC-CM), S2013/MIT-3007 (MAD2D), and CMS2018/NMT-4321 (NANOMAGCOST)], and the IMDEA Foundation. P.J. and M.O. acknowledge support from Praemium Academie of the Academy of Sciences of the Czech Republic, MEYS LM2015087 and GACR 18-09914S, and Operational Programme Research, Development and Education financed by European Structural and Investment Funds and the Czech Ministry of Education, Youth and Sports (Projects SOLID21 - CZ.02.1.01/0.0/0.0/16_019/0000760 and CZ.02.1.01/0.0/0.0/16_019/0000754). IMDEA Nano-ciencia is grateful for support from the 'Severo Ochoa' Programme for Centers of Excellence in R&D (MINECO, Grant SEV-2016-0686). The authors acknowledge Willi Auwarter,? Francesco Allegretti, and Anthoula C. Papageorgiou for fruitful discussions.

Published
2019

17. On-Surface Synthesis of Ethynylene-Bridged Anthracene Polymers

Author

Sánchez-Grande A., de la Torre B., Santos J., Cirera B., Lauwaet K., Chutora T., Edalatmanesh S., Mutombo P., Rosen J., Zbo?il R., Miranda R., Björk J., Jelínek P., Martín N., Écija D. and This work was supported by the Comunidad de Madrid (Projects Y2018/NMT-4783 (QUIMTRONIC-CM), S2013/ MIT-3007 (MAD2D), and S2018/NMT (NANOMAGCOST-CM)), the European Research Council (ERC-320441-Chir-allcarbon and ERC-766555-ELECNANO), the Spanish Ramón y Cajal programme (No. RYC-2012-11133), and the MINECO of Spain (Projects FIS 2015-67287-P, CTQ2017-83531-R, and CTQ2016-81911-REDT). The IMDEA Nano-ciencia acknowledges support from the Severo Ochoa Programme for Centers of Excellence in R&D (MINECO, Grant SEV-2016-0686). P.J. acknowledges support from the Prae-mium Academie of the Academy of Science of the Czech Republic, MEYS LM2015087 and GACR 18–09914S, and the Operational Programme Research, Development, and Education financed by the European Structural and Investment Funds and the Czech Ministry of Education, Youth, and Sports (Project No. CZ.02.1.01/0.0/0.0/16 019/0000754). The authors acknowledge the support from the Czech Science Foundation under Project No. 19-27454X. J.B. and J.R. acknowledge financial support from the Swedish Research Council (642-2013-2080), the Swedish Strategic Research Area in Materials Science on Functional Materials at Link-çping University (Faculty Grant SFO-Mat-LiU No 2009 00971), and computational resources at the National Supercomputer Centre, Sweden, allocated by SNIC. The authors thank Dr. Oliver Grçning for fruitful discussions.

Published
2019

18. In-Situ Growth of Gadolinium Phthalocyaninato Sandwich Complexes on the Ag(111) Surface

Author

Urgel J.I., Écija D., Vijayaraghavan S., Pörtner M., Bocquet M.-L., Auwärter W., Barth J.V. and This work was supported by the European Research Council Advanced Grant MolArt (Grant No. 247299), the Munich Center for Advanced Photonics (MAP), the Technische Universitat M?nchen-Institute for Advanced Study, funded by the German Research Foundation (DFG) via the German Excellence Initiative, and the ANR-DFG project RidePorph. W.A. acknowledges funding by the DFG via a Heisenberg professorship. M.P. and M.-L.B. thank the HPC resources from GENCI-[TGCC/CINES/IDRIS] (Grant 2018-[A0050807364]).

Published
2019

20. Lanthanide-Directed Assembly of Interfacial Coordination Architectures-From Complex Networks to Functional Nanosystems

Author

Écija D., Urgel J.I., Seitsonen A.P., Auwärter W., Barth J.V. and We appreciate financial support by the EU (Projects ERC Advanced Grant MolArt (247299), EC FP7-PEOPLE-2011-COFUND AMAROUT II Program), the TUM?HKUST Sponsorship Scheme for Targeted Strategic Partnerships, the Spanish Ministerio de Economiá y Competitividad (MINECO) (RYC-2012-11133, FIS 2013-40667-P, FIS 2015-67287-P), the Comunidad de Madrid (Project MAD2D), the IMDEA Foundation, and the Munich-Center for Advanced Photonics (MAP). W.A. acknowledges a Heisenberg Professorship funded by the German Research Foundation. We warmly thank all (former) team members and project partners coauthoring the cited joint publications, in particular our esteemed colleagues D. Bonifazi, S. Klyatskaya, N. Lin, M. Ruben, and K. Tashiro.

Published
2018

21. Investigating the molecule-substrate interaction of prototypic tetrapyrrole compounds: Adsorption and self-metalation of porphine on Cu(111).

Author

Diller, K., Klappenberger, F., Allegretti, F., Papageorgiou, A. C., Fischer, S., Wiengarten, A., Joshi, S., Seufert, K., Écija, D., Auwärter, W., and Barth, J. V.

Subjects
TETRAPYRROLES, METALATION, COPPER surfaces, X-ray photoelectron spectroscopy, X-ray absorption near edge structure, SUBSTRATES (Materials science), CHARGE exchange, SCANNING tunneling microscopy
Abstract

We report on the adsorption and self-metalation of a prototypic tetrapyrrole compound, the free-base porphine (2H-P), on the Cu(111) surface. Our multitechnique study combines scanning tunneling microscopy (STM) results with near-edge X-ray absorption fine-structure (NEXAFS) and X-ray photoelectron spectroscopy (XPS) data whose interpretation is supported by density functional theory calculations. In the first layer in contact with the copper substrate the molecules adsorb coplanar with the surface as shown by angle-resolved NEXAFS measurements. The quenching of the first resonance in the magic angle spectra of both carbon and nitrogen regions indicates a substantial electron transfer from the substrate to the LUMO of the molecule. The stepwise annealing of a bilayer of 2H-P molecules sequentially transforms the XP and NEXAFS signatures of the nitrogen regions into those indicative of the coordinated nitrogen species of the metalated copper porphine (Cu-P), i.e., we observe a temperature-induced self-metalation of the system. Pre- and post-metalation species are clearly discriminable by STM, corroborating the spectroscopic results. Similar to the free-base porphine, the Cu-P adsorbs flat in the first layer without distortion of the macrocycle. Additionally, the electron transfer from the copper surface to the molecule is preserved upon metalation. This behavior contrasts the self-metalation of tetraphenylporphyrin (2H-TPP) on Cu(111), where both the molecular conformation and the interaction with the substrate are strongly affected by the metalation process. [ABSTRACT FROM AUTHOR]

Published
2013
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22. Tuning Intermolecular Charge Transfer in Donor-Acceptor Two-Dimensional Crystals on Metal Surfaces

Author

Rodríguez-Fernández J., Robledo M., Lauwaet K., Martín-Jiménez A., Cirera B., Calleja F., Díaz-Tendero S., Alcamí M., Floreano L., Domínguez-Rivera M., Vázquez De Parga A.L., Écija D., Gallego J.M., Miranda R., Martín F., Otero R. and The authors acknowledge financial support from the Spanish Ministry for Economy and Competitiveness (Grants FIS2012-33011, FIS2015-67367-C2-1-P, FIS2013-42002-R, FIS2016-77889-R, CTQ2013-43698-P, CTQ2016-76061-P), the regional government of Comunidad de Madrid (Grants S2009/ MAT1726 and S2013/MIT-3007), Universidad Autonomá de Madrid (UAM/48) and IMDEA Nanoscience. L.F. acknowledges financial support from MIUR (PRIN-2010BNZ3F2, Project DESCARTES), S.D.-T. acknowledges the ‘'Ramo? y Cajal'’ program of the MINECO (RYC-2010-07019), and the Mariá de Maeztu Programme for Units of Excellence in R&D of the MINECO (MDM-2014-0377). We thank the Center for Scientific Computing of the Autonomous University (CCC-UAM) and the Spanish Supercomputing Network (RES) for the allocation of computer time. Technical support for the realization of the experiments by Dr. M. Á. Matarrubia is gratefully acknowledged.

Published
2017

23. Quasicrystallinity expressed in two-dimensional coordination networks

Author

Urgel J.I., Écija D., Lyu G., Zhang R., Palma C.-A., Auwärter W., Lin N., Barth J.V. and This work was supported by a European Research Council Advanced Grant MolArt (No. 247299), the European Commission FP7-PEOPLE-2011-COFUND AMAROUT II program, the Spanish Ram?n and Cajal Program (No. RYC-2012-11133), the Comunidad de Madrid (project MAD2D), the Hong Kong Research Grants Council (No. 603213) and the TUMHKUST Sponsorship Scheme for Targeted Strategic Partnerships. W.A. acknowledges funding by the German Research Foundation (DFG) via a Heisenberg professorship.

Published
2016

26. Flexible Coordination Polymers on Metallic Surfaces

Author

Heim, D. Écija D., Seufert, K., Auwärter, W., Aurisicchio, C., Fabbro, C., Bonifazi, Davide, Barth, J. V., Heim, D. Écija D., Seufert, K., Auwärter, W., Aurisicchio, C., Fabbro, C., Bonifazi, Davide, and Barth, J. V.

Subjects
Porphyrin, scanning tunneling microscopy, metal-organic coordination, supramolecules, Porphyrin, supramolecules, scanning tunneling microscopy, metal-organic coordination, copper surface, copper surface
Abstract

We employed de novo synthesized porphyrin modules to construct discrete cyclic supramolecular architectures supported on a copper surface. The programmed geometry and functionality of the molecular modules together with their conformational flexibility and substrate interaction yields symmetric discrete assemblies, including dimers and chains as well as three- to six-membered cyclic structures. The area of the molecular cavities is extended by creating bicomponent structures combining building blocks with different symmetry.

Published
2010

29. Porphyrins at interfaces

Author

Auwärter W., Écija D., Klappenberger F., Barth J.V. and We are grateful for support from the European Research Council Advanced Grant MolArt (no. 247299), the Munich Centre for Advanced Photonics (MAP) and TUM Institute for Advanced Study funded by the German Research Foundation (DFG) via the German Excellence Initiative, Canadian NSERC and CFI, the Spanish RyC Programme and other funding schemes. We thank all team members and project partners co-authoring cited joint publications.

Published
2015

32. Subphthalocyanine-based nanocrystals

Author

Trelka M., Medina A., Écija D., Urban C., Gröning O., Fasel R., Gallego J.M., Claessens C.G., Otero R., Torres T., Miranda R.

Published
2011

36. Charge-transfer-induced structural rearrangements at both sides of organic/metal interfaces

Author

Tseng T.-C., Urban C., Wang Y., Otero R., Tait S.L., Alcamí M., Écija D., Trelka M., Gallego J.M., Lin N., Konuma M., Starke U., Nefedov A., Langner A., Wöll C., Herranz M.Á., Martín F., Martín N., Kern K., Miranda R. and Studies at MPI Stuttgart were supported by the European Science Foundation (ESF) EUROCORES-SONS2 programme FunSMARTs II. Work in Madrid was financed by the Spanish MICINN (projects FIS2007-61114, FIS2007-60064, NAN2004-08881-C02-01, CTQ2006-08558 and Consolider CSD2007-00010), the Comunidad de Madrid (projects S-0505-MAT-0194 and S2009/MAT-1726) and the European Union (‘MONET’ project, MEST-CT-2005-020908). R.O. thanks the MEC for salary support through the Ramón & Cajal programme. All the computations were performed at Mare Nostrum Barcelona Supercomputer Center and Centro de Computación Científica de la UAM.

Published
2010

37. The adsorption of atomic N and the growth of copper nitrides on Cu(1 0 0)

Author

Écija D., Gallego J.M., Miranda R. and This work has been financed by the Spanish MEC (Project NAN2004-08881-C02-01, Project FIS2007-61114 and Project CONSOLIDER-INGENIO EN NANOCIENCIA MOLECULAR ref. CSD2007-00010), and the Comunidad de Madrid (Project GR/MAT/0435/2004 and Project NANOMAGNET S-0505/MAT/0194).

Published
2009

39. Templated growth of an ordered array of organic bidimensional mesopores

Author

Écija D., Trelka M., Urban C., De Mendoza P., Echavarren A., Otero R., Gallego J.M., Miranda R. and This work has been financially supported by the MEC of Spain (MSR-FIS2007-61114, MAT2006-13470, NAN-2004-08881-002-01, NAN-2004-08881-C02-02, and CONSOLIDER CSD2007-00010), Comunidad de Madrid (NANOMAGNET S-0505/MAT/0194), and EU ('MONET' project, MEST-CT-2005-020908).

Published
2008

45. A Kagome Lattice of Lanthanide Atoms in a 2D Er‐Directed Metal‐Organic Coordination Network.

Author

Moreno, Daniel, Parreiras, Sofía O., Mathialagan, Shanmugasibi K., Tenorio, María, Lauwaet, Koen, Urgel, José I., Gallego, José M., and Écija, D.

Subjects
*MAGNETIC properties, *MONOMOLECULAR films, *ATOMS, *NANOSTRUCTURED materials, *METALS
Abstract

Kagome lattices have attracted much attention due the very interesting properties they can exhibit, both from the electronic and the magnetic points of view, although much of the experimental studies have been reported on 3D metals or 2D nanosheets. In the past few years, on‐surface synthesis has allowed the fabrication of strictly monolayer 2D metal‐organic networks, many of them containing transition metals. In this paper we report the fabrication and the study of the electronic and magnetic properties of a monolayer 2D metal‐organic network where the nodes are lanthanide atoms forming a kagome lattice. [ABSTRACT FROM AUTHOR]

Published
2024
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46. Hierarchic self-assembly of nanoporous chiral networks with conformationally flexible porphyrins

Author

Johannes V. Barth, Claudia Aurisicchio, Daniel Heim, Willi Auwärter, Davide Bonifazi, David Écija, Chiara Fabbro, Knud Seufert, Écija, D., Seufert, K., Heim, D., Auwärter, W., Aurisicchio, C., Fabbro, C., Bonifazi, Davide, and Barth, J. V.

Subjects
Materials science, Nanoporous, General Engineering, Supramolecular chemistry, General Physics and Astronomy, Nanotechnology, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Porphyrin, Combinatorial chemistry, Supramolecular Chemistry, 0104 chemical sciences, chemistry.chemical_compound, Enantiopure drug, chemistry, Molecule, General Materials Science, Self-assembly, Enantiomer, 0210 nano-technology, Chirality (chemistry)
Abstract

We report the hierarchic design of homochiral 2D nanoporous networks under ultrahigh vacuum conditions on the Ag(111) surface by using a flexible porphyrin derivative as a primary unit. The conformational adaptation of the molecular module gives rise to two enantiomers upon 2D confinement, which self-assemble in enantiopure clusters made of three molecules reflecting chiral recognition, which constitute the secondary supramolecular building block mediating the formation of the tertiary complex open networks. Our results show that the creation of homochiral superstructures based on the hierarchical assembly of conformationally flexible molecular components constitutes a unique pathway toward the design of novel and functional chiral structures. © 2010 American Chemical Society.

Published
2010

47. Coronene-Based 2D Networks by On-Surface Skeletal Rearrangement of Sumanene Precursors.

Author

Pérez-Elvira E, Barragán A, Gallardo A, Santos J, Martín-Fuentes C, Lauwaet K, Gallego JM, Miranda R, Sakurai H, Urgel JI, Björk J, Martín N, and Écija D

Abstract

The design of novel low-dimensional carbon materials is at the forefront of modern chemistry. Recently, on-surface covalent synthesis has emerged as a powerful strategy to synthesize previously precluded compounds and polymers. Here, we report a scanning probe microscopy study, complemented by theoretical calculations, on the sequential skeletal rearrangement of sumanene-based precursors into a coronene-based organometallic network by stepwise intra- and inter-molecular reactions on Au(111). Interestingly, upon higher annealing, the formed organometallic networks evolve into two-dimensional coronene-based covalently linked patches through intermolecular homocoupling reactions. A new reaction mechanism is proposed based on the role of C-Au-C motifs to promote two stepwise carbon-carbon couplings to form cyclobutadiene bridges. Our results pave avenues for the conversion of molecular precursors on surfaces, affording the design of unexplored two-dimensional organometallic and covalent materials., (© 2024 The Author(s). Angewandte Chemie International Edition published by Wiley-VCH GmbH.)

Published
2025
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48. Coordinative Self-assembly of π-Electron Magnetic Porphyrins.

Author

Tenorio M, Lozano M, Cerna L, Martínez García M, Urbani M, Lauwaet K, Biswas K, Soler-Polo D, Mathialagan SK, Parreiras SO, Gallego JM, Miranda R, Urgel JI, Torres T, Jelínek P, Bottari G, and Écija D

Abstract

π-Electron magnetic compounds on surfaces have emerged as a powerful platform to interrogate spin interactions at the atomic scale, with great potential in spintronics and quantum technologies. A key challenge is organizing these compounds over large length scales, while elucidating their resulting magnetic properties. Herein, we offer a relevant contribution toward this objective, which consists of using on-surface synthesis coupled with coordination chemistry to promote the self-assembly of π-electron magnetic porphyrin species. A porphyrin precursor equipped with carbonitrile moieties in a trans arrangement was prepared by solution synthesis and deposited on Au(111)/mica. Depending on the specific growth protocol, surface-promoted reactions led to the transformation of the precursor into non-magnetic Au-CN coordinated porphyrin monomers, covalent porphyrin dimers, and one-dimensional porphyrin polymers (based on porphyrin monomers or covalent porphyrin dimers), as revealed by scanning probe microscopy studies combined with theoretical calculations. Interestingly, the scanning tunneling microscopy tip could convert such closed-shell porphyrin units into open-shell species by the removal of some peripheral hydrogen atoms. The magnetic features (i.e., singlet or triplet ground state) of the porphyrin units comprising the polymers were investigated for polymers of different lengths. No magnetic exchange coupling between adjacent units was observed, suggesting protection of the magnetic entities., (© 2024 The Author(s). Angewandte Chemie International Edition published by Wiley-VCH GmbH.)

Published
2024
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49. On-Surface Synthesis of Covalently-Linked Carbaporphyrinoid-Based Low-Dimensional Polymers.

Author

Barragán A, Urbani M, Gallardo A, Pérez-Elvira E, Jover Ó, Lauwaet K, Gallego JM, Miranda R, Giovannantonio MD, Écija D, Torres T, and Urgel JI

Abstract

The synthesis of porphyrinoid-based low-dimensional polymers has recently attracted considerable interest in view of their intriguing electronic, optical, and catalytic properties. Here, this is introduced by the surface-assisted synthesis of two carbaporphyrinoid-based polymers of increasing dimensionality under ultrahigh-vacuum conditions. The structural and electronic characterization of the resulting polymers has been performed by scanning tunneling and non-contact atomic force microscopies, complemented by theoretical modeling. First, a carbon-carbon coupling between dicarbahemiporphyrazine precursors is achieved by thermal activation of their isopropyl substituents via a [3+3] cycloaromatization, giving rise to one-dimensional (1D) polymers. Second, the same precursor is functionalized with chlorine atoms to complement the [3+3] cycloaromatization with orthogonal dehalogenation and homocoupling, affording two-dimensional (2D) molecular nanostructures. In addition, both low-dimensional free-base porphyrinoid-based polymers are exposed to an atomic flux of cobalt atoms, giving rise to cobalt-metalated macrocycles, with the metal atoms coordinated only to the two pyrrolic nitrogens, in contrast to the typical four-fold coordination that occurs inside tetrapyrroles. This on-surface protocol renders atomically precise covalently-linked porphyrinoid polymers and provides promising model systems toward the exploration of low-coordinated metals with utility in diverse technological areas., (© 2024 Wiley‐VCH GmbH.)

Published
2024
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50. Atomically Precise Control of Topological State Hybridization in Conjugated Polymers.

Author

Jiménez-Martín A, Sosnová Z, Soler D, Mallada B, González-Herrero H, Edalatmanesh S, Martín N, Écija D, Jelínek P, and de la Torre B

Abstract

Realization of topological quantum states in carbon nanostructures has recently emerged as a promising platform for hosting highly coherent and controllable quantum dot spin qubits. However, their adjustable manipulation remains elusive. Here, we report the atomically accurate control of the hybridization level of topologically protected quantum edge states emerging from topological interfaces in bottom-up-fabricated π-conjugated polymers. Our investigation employed a combination of low-temperature scanning tunneling microscopy and spectroscopy, along with high-resolution atomic force microscopy, to effectively modify the hybridization level of neighboring edge states by the selective dehydrogenation reaction of molecular units in a pentacene-based polymer and demonstrate their reversible character. Density functional theory, tight binding, and complete active space calculations for the Hubbard model were employed to support our findings, revealing that the extent of orbital overlap between the topological edge states can be finely tuned based on the geometry and electronic bandgap of the interconnecting region. These results demonstrate the utility of topological edge states as components for designing complex quantum arrangements for advanced electronic devices.

Published
2024
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