Detail publikačního výsledku

Tetracoordinate Co(ii) complexes with semi-coordination as stable single-ion magnets for deposition on graphene

NAVARRO GIRALDO, J.; HRUBÝ, J.; VAVREČKOVÁ, Š.; FELLNER, O.F.; HAVLÍČEK, L.; HENRY, D.; DE SILVA, S.; HERCHEL, R.; BARTOŠ, M.; ŠALITROŠ, I.; SANTANA, V.; BARBARA, P.; NEMEC, I.; NEUGEBAUER, P.

Originální název

Tetracoordinate Co(ii) complexes with semi-coordination as stable single-ion magnets for deposition on graphene

Anglický název

Tetracoordinate Co(ii) complexes with semi-coordination as stable single-ion magnets for deposition on graphene

Druh

Článek WoS

Originální abstrakt

We present a theoretical and experimental study of two tetracoordinate Co(ii)-based complexes with semi-coordination interactions, i.e., non-covalent interactions involving the central atom. We argue that such interactions enhance the thermal and structural stability of the compounds, making them appropriate for deposition on substrates, as demonstrated by their successful deposition on graphene. DC magnetometry and high-frequency electron spin resonance (HF-ESR) experiments revealed an axial magnetic anisotropy and weak intermolecular antiferromagnetic coupling in both compounds, supported by theoretical predictions from complete active space self-consistent field calculations complemented by N-electron valence state second-order perturbation theory (CASSCF-NEVPT2), and broken-symmetry density functional theory (BS-DFT). AC magnetometry demonstrated that the compounds are field-induced single-ion magnets (SIMs) at applied static magnetic fields, with slow relaxation of magnetization governed by a combination of quantum tunneling, Orbach, and direct relaxation mechanisms. The structural stability under ambient conditions and after deposition was confirmed by X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy. Theoretical modeling by DFT of different configurations of these systems on graphene revealed n-type doping of graphene originating from electron transfer from the deposited molecules, confirmed by electrical transport measurements and Raman spectroscopy.

Anglický abstrakt

We present a theoretical and experimental study of two tetracoordinate Co(ii)-based complexes with semi-coordination interactions, i.e., non-covalent interactions involving the central atom. We argue that such interactions enhance the thermal and structural stability of the compounds, making them appropriate for deposition on substrates, as demonstrated by their successful deposition on graphene. DC magnetometry and high-frequency electron spin resonance (HF-ESR) experiments revealed an axial magnetic anisotropy and weak intermolecular antiferromagnetic coupling in both compounds, supported by theoretical predictions from complete active space self-consistent field calculations complemented by N-electron valence state second-order perturbation theory (CASSCF-NEVPT2), and broken-symmetry density functional theory (BS-DFT). AC magnetometry demonstrated that the compounds are field-induced single-ion magnets (SIMs) at applied static magnetic fields, with slow relaxation of magnetization governed by a combination of quantum tunneling, Orbach, and direct relaxation mechanisms. The structural stability under ambient conditions and after deposition was confirmed by X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy. Theoretical modeling by DFT of different configurations of these systems on graphene revealed n-type doping of graphene originating from electron transfer from the deposited molecules, confirmed by electrical transport measurements and Raman spectroscopy.

Klíčová slova

TOTAL-ENERGY CALCULATIONS; MOLECULE MAGNET; ZERO-FIELD; BASIS-SETS; ELECTRON LOCALIZATION; COBALT(II) COMPLEXES; ANISOTROPY; DENSITY; RELAXATION; LIGAND

Klíčová slova v angličtině

TOTAL-ENERGY CALCULATIONS; MOLECULE MAGNET; ZERO-FIELD; BASIS-SETS; ELECTRON LOCALIZATION; COBALT(II) COMPLEXES; ANISOTROPY; DENSITY; RELAXATION; LIGAND

Autoři

NAVARRO GIRALDO, J.; HRUBÝ, J.; VAVREČKOVÁ, Š.; FELLNER, O.F.; HAVLÍČEK, L.; HENRY, D.; DE SILVA, S.; HERCHEL, R.; BARTOŠ, M.; ŠALITROŠ, I.; SANTANA, V.; BARBARA, P.; NEMEC, I.; NEUGEBAUER, P.

Rok RIV

2024

Vydáno

08.11.2023

Nakladatel

ROYAL SOC CHEMISTRY

Místo

CAMBRIDGE

ISSN

1463-9084

Periodikum

PHYSICAL CHEMISTRY CHEMICAL PHYSICS

Svazek

25

Číslo

43

Stát

Spojené království Velké Británie a Severního Irska

Strany od

29516

Strany do

29530

Strany počet

15

URL

https://pubs.rsc.org/en/content/articlelanding/2023/cp/d3cp01426f

BibTex

@article{BUT187563,
  author="NAVARRO GIRALDO, J. and HRUBÝ, J. and VAVREČKOVÁ, Š. and FELLNER, O.F. and HAVLÍČEK, L. and HENRY, D. and DE SILVA, S. and HERCHEL, R. and BARTOŠ, M. and ŠALITROŠ, I. and SANTANA, V. and BARBARA, P. and NEMEC, I. and NEUGEBAUER, P.",
  title="Tetracoordinate Co(ii) complexes with semi-coordination as stable single-ion magnets for deposition on graphene",
  journal="PHYSICAL CHEMISTRY CHEMICAL PHYSICS",
  year="2023",
  volume="25",
  number="43",
  pages="29516--29530",
  doi="10.1039/d3cp01426f",
  issn="1463-9076",
  url="https://pubs.rsc.org/en/content/articlelanding/2023/cp/d3cp01426f"
}