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Chemical Engineering of Quasicrystal Approximants in Lanthanide-Based Coordination Solids

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Chemical Engineering of Quasicrystal Approximants in Lanthanide-Based Coordination Solids Downloaded from orbit.dtu.dk on: Sep 26, 2021 Chemical engineering of quasicrystal approximants in lanthanide-based coordination solids Voigt, Laura; Kubus, Mariusz; Pedersen, Kasper Steen Published in: Nature Communications Link to article, DOI: 10.1038/s41467-020-18328-5 Publication date: 2020 Document Version Publisher's PDF, also known as Version of record Link back to DTU Orbit Citation (APA): Voigt, L., Kubus, M., & Pedersen, K. S. (2020). Chemical engineering of quasicrystal approximants in lanthanide-based coordination solids. Nature Communications, 11(1), [4705]. https://doi.org/10.1038/s41467- 020-18328-5 General rights Copyright and moral rights for the publications made accessible in the public portal are retained by the authors and/or other copyright owners and it is a condition of accessing publications that users recognise and abide by the legal requirements associated with these rights. Users may download and print one copy of any publication from the public portal for the purpose of private study or research. You may not further distribute the material or use it for any profit-making activity or commercial gain You may freely distribute the URL identifying the publication in the public portal If you believe that this document breaches copyright please contact us providing details, and we will remove access to the work immediately and investigate your claim. ARTICLE https://doi.org/10.1038/s41467-020-18328-5 OPEN Chemical engineering of quasicrystal approximants in lanthanide-based coordination solids ✉ Laura Voigt 1, Mariusz Kubus1 & Kasper S. Pedersen 1 Tessellation of self-assembling molecular building blocks is a promising strategy to design metal-organic materials exhibiting geometrical frustration and ensuing frustrated physical properties. Appearing in two-dimensional quasiperiodic phases, tilings consisting of five- 1234567890():,; vertex nodes are regarded as approximants for quasicrystals. Unfortunately, these structural motifs are exceedingly rare due to the complications of acquiring five-fold coordination confined to the plane. Lanthanide ions display the sufficient coordinative plasticity, and large ionic radii, to allow their incorporation into irregular molecule-based arrays. We herein present the use of ytterbium(II) as a five-vertex node in a two-dimensional coordination solid, YbI2(4,4′-bipyridine)2.5. The semi-regular Archimedean tessellation structure verges on quasicrystallinity and paves the way for lanthanide-based metal-organic materials with interesting photonic and magnetic properties. ✉ 1 Department of Chemistry, Technical University of Denmark, Kemitorvet, Building 207, DK-2800 Kgs Lyngby, Denmark. email: [email protected] NATURE COMMUNICATIONS | (2020) 11:4705 | https://doi.org/10.1038/s41467-020-18328-5 | www.nature.com/naturecommunications 1 ARTICLE NATURE COMMUNICATIONS | https://doi.org/10.1038/s41467-020-18328-5 uasicrystals are ordered materials lacking translational handles on controlling dimensionality and topology of metal- symmetry1, which leads to unique physical properties2, organic coordination solids, suitable for targeting complex tes- Q 3–5 including novel magnetic and photonic phenomena . sellations. Indeed, applying this strategy resulted in a singular They exhibit symmetries that are forbidden for any periodic example of a metal-organic quasicrystal consisting of a surface structure, such as the 5-fold rotational symmetry first discovered self-assembled array of Eu atom nodes linked by ditopic carbo- in an Al–Mn alloy by Shechtman et al.6 or the 12-fold symmetry nitrile bridging ligands7. This network is reminiscent of a random in dodecagonal quasicrystals7. Dodecagonal symmetry is achieved tiling containing nanoscale motifs of the semi-regular ATs. The in a maximally random assembly of squares and triangles linked flexibility and the large atomic radii of Eu allowed for coordi- through four-, five-, and six-vertex nodes8,9. Dodecagonal qua- nating up to six ligands in the equatorial plane allowing the sicrystallinity has been observed in a plethora of materials formation of local dodecagonal symmetry7. Notably, small dif- including alloys10,11, mesoporous silica12, nanoparticle super- ferences in the preparation conditions led to the formation of lattices13, and copolymers14. Notably, all of these quasicrystalline prevailing 33.42 or 32.4.3.4 tilings, which underlines the close phases have motifs of, or coexist with, domains of periodic tilings relationship of the periodic approximants with the dodecagonal of squares and triangles, whose existence was hypothesized by phase. Accordingly, the assembly of atomic Ce and the same Frank and Kasper15, and whose topologies were first introduced ditopic ligand on a Ag(111) surface lead to the formation of a by Kepler in Harmonices Mundi in 161916. The tilings of squares 32.4.3.4 tiling30. Only recently, an ionic liquid-based approach led and triangles belong to the uniform tessellations of the two- to the isolation of a bulk coordination solid containing layers of 17 (1/2)− fi dimensional (2D) (Euclidian) plane , where all vertices are [(UO2)(1,2,4-triazolate)2.5] , constituting the rst example of identical and the tilings are labeled by the sequence of their an 32.4.3.4 tiling realized through fivefold coordinated trans- 2+ 20 surrounding polygons. For instance, six-vertex nodes are found {UO2} nodes . Herein, however, the presence of a net charge only in the regular triangular tiling (36; Fig. 1a) containing a of the 2D layer could impede the possibilities for further pro- single equilateral polygon, whereas five-vertex nodes are part of cessing of this material for nanostructuring and the nonmagnetic the snub hexagonal (34.6), elongated triangular (33.42), and snub uranyl nodes hinder the exploration of magnetic properties. square tilings (32.4.3.4; cf. Fig. 1b, e, f). Due to their similarities Similar to uranium, the lanthanide ion series distinguishes itself with the local structure of dodecagonal quasicrystals, crystalline by a strong propensity to high coordination numbers. In addition, phases with structure motifs of five-vertex semi-regular Archi- the lanthanide ions exhibit paramount plasticity in their chemical medean tessellations (ATs) are referred to as quasicrystal bonding and unique optical and magnetic properties, of immense approximants9,12,18–20. The appearance of approximants suggests technological importance, which are not paralleled by any other the possibility of designing quasicrystallinity by chemical means. elements31. Motivated by the possibilities to extend these prop- The realization of regular tilings in chemistry and nature is ubi- erties to ATs and quasiperiodic materials, we, herein, report a quitous. However, of the ATs only the trihexagonal tiling ((3.6)2; coordination-assembly strategy and the crystallographic char- cf. Fig. 1c), the kagomé lattice, appears frequently21. Notably, ATs acterization of the first example of a lanthanide-based AT in a in materials have been hailed as a key component for exploring bulk, molecule-based material. novel photonics applications22–24 and to host peculiar magnetic phenomena, such as frustration25–28, which call for novel syn- thetic strategies to their authentication. Whereas for inter- Results metallics29 numerous quasicrystalline approximants have been Structural characterization and description. Numerous exam- isolated, ATs have remained almost elusive in metal-organic ples of first-row transition element-based 2D coordination solids materials. Reticular coordination chemistry harbors the synthetic pillared on 4,4′-bipyridine (bipy) and related ditopic, organic ligands are known32. Therein, the limiting, prevailing coordina- 4 abc tion number of six imposes a square (4 ; cf. Fig. 1d) tessellation of the 2D plane calling for employment of significantly larger metal ions for the generation of ATs. The tendency to high coordina- 6 3 3 tion numbers in di- and trivalent lanthanide (Ln(II/III)) com- 3 3 3 3 pounds offers the possibility of generating, for instance, 3 3 +/0 33 34 [LnI2(pyridine)5] (Ln = Lu ,Sm ). Notably, these systems 3 3 6 6 33 closely resemble a local D5h coordination geometry of the Ln(II/ III) with the organic ligands placed in the equatorial plane, pre- sumably directed by the space-filling, axial iodide ligands. 36 34.6 (3.6)2 Translating this structure-directing motif to 2D coordination solids seems key for tailoring metal-organic ATs and quasicrys- tals. Indeed, the self-assembly reaction of ytterbium(II) iodide d e f with bipy in acetonitrile at room temperature under strictly anaerobic conditions yielded dark blue, block-shaped crystals of 1 YbI2(bipy)2.5·1.5 CH3CN ( ) suitable for single-crystal X-ray 3 4 diffraction analysis. Compound 1 crystallizes in the triclinic space 44 3 3 4 3 4 group P1 hosting a single Yb in the asymmetric unit (Fig. 2 and 4 3 Supplementary Fig. 1). The {YbN } moiety deviates marginally 44 3 5 from planarity with a maximal distortion from ideality of ∼5% for – – I2 Yb N3 and approximates closely a D5h coordination envir- onment with N–Yb–N angles in the range from 69° to 77°, close 44 33.42 32.4.3.4 to the ideal angle of 72° (Fig. 2b). Within the 2D plane, the Fig. 1 Archimedean tessellations. Six of the 11 regular (a, d) and semi- linking of bipy and Yb(II) forms both square and triangular regular (b, c, e, f) Archimedean tessellations of the Euclidean plane: a tiles with the bipy linkers spanning the edges. The squares triangular, b snub hexagonal, c trihexagonal (kagomé), d square, e and triangles closely approximate equilateral geometries with elongated triangular, and f snub square tiling. edge lengths of 12.14 Å and 12.25 Å for the squares and 12.32 Å, 2 NATURE COMMUNICATIONS | (2020) 11:4705 | https://doi.org/10.1038/s41467-020-18328-5 | www.nature.com/naturecommunications NATURE COMMUNICATIONS | https://doi.org/10.1038/s41467-020-18328-5 ARTICLE ab 90° 90° 77° 75° 71° 70° 69° 61° 60° 59° Fig. 2 Structure of 1. Representations of the crystal structure of 1 as determined by single-crystal X-ray diffraction at T = 120(1) K. a Fragment of the 3 2 constituent coordination layers with an overlay of the ideal 3 .4 tessellation.
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