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Title: Multiscale study of mononuclear CoII SMMs based on curcuminoid ligands

Abstract

This work introduces a novel family of CoII species having a curcuminoid (CCMoid) ligand, 9Accm, attached, namely [Co(9Accm) 2 (py) 2 ] (1) and [Co(9Accm)2(2,2'-bpy)] (2), achieved in high yields by the use of a microwave reactor, and exhibiting two different arrangements for the 9Accm ligands, described as "cis"(2) and "trans"(1). The study of the similarities/differences of the magnetic, luminescent and surface behaviors of the two new species, 1 and 2, is the main objective of the present work. The determined single-crystal structures of both compounds are the only CoII -CCMoid structures described in the literature so far. Both compounds exhibit large positive D values, that of 1 (D = +74 cm-1 ) being three times larger than that of 2 (D = +24 cm-1 ), and behave as mononuclear Single-Molecule Magnets (SMMs) in the presence of an external magnetic field. Their similar structures but different anisotropy and SMM characteristics provide, for the first time, deep insight on the spin-orbital effects thanks to the use of CASSCF/NEVPT2 calculations implementing such contributions. Further magnetic studies were performed in solution by means of paramagnetic 1H NMR, where both compounds (1 and 2) are stable in CDCl3 and display high symmetry. Paramagnetic NMRmore » appears to be a useful diagnostic tool for the identification of such molecules in solution, where the resonance values found for the methine group (-CH-) of 9Accm vary significantly depending on the cis or trans disposition of the ligands. Fluorescence studies show that both systems display chelation enhancement of quenching (CHEQ) with regard to the free ligand, while 1 and 2 display similar quantum yields. Deposition of 1-2 on HOPG and Si(100) surfaces using spin-coating was studied using AFM; UV photoemission experiments under the same conditions display 2 as the most robust system. The measured occupied density of states of 2 with UV photoemission is in excellent agreement with theoretical DFT calculations.« less

Authors:
 [1]; ORCiD logo [1]; ORCiD logo [2];  [3];  [1]; ORCiD logo [4];  [5]; ORCiD logo [6]; ORCiD logo [7]; ORCiD logo [8]
  1. Univ. de Barcelona (Spain). Dept. de Quimica Inorganica
  2. Inst. de Ciencia de Materials de Aragon (ICMAP-CSIC), Zaragoza (Spain); Univ. de Zaragoza (Spain)
  3. CSIC-ICMAB (Institut de Ciència dels Materials de Barcelona) Campus de la Universitat Autònoma de Barcelona; 08193 Bellaterra, Spain
  4. Univ. de Barcelona (Spain). Dept. de Quimica Inorganica and Inst. de Nanociencia i Nanotecnologia-UB
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  6. Catalan Inst. of Nanoscience and Nanotechnology (ICN2), Consejo Superior de Investigaciones Cientificas (CSIC) and The Barcelona Inst. of Science and Technology, Barcelona (Spain)
  7. Univ. de Barcelona (Spain). Dept. de Quimica Inorganica; Univ. de Barcelona (Spain). Inst. de Qui­mica Teorica i Computacional
  8. Univ. Autonoma de Barcelona (Spain). Inst. Catalana de Recerca i Estudis Avancats (ICREA) and Inst. de Fisica d'Altes Energies (IFAE)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1377417
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Chemical Science
Additional Journal Information:
Journal Volume: 7; Journal Issue: 4; Journal ID: ISSN 2041-6520
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Díaz-Torres, Raúl, Menelaou, Melita, Roubeau, Olivier, Sorrenti, Alessandro, Brandariz-de-Pedro, Guillem, Sañudo, E. Carolina, Teat, Simon J., Fraxedas, Jordi, Ruiz, Eliseo, and Aliaga-Alcalde, Núria. Multiscale study of mononuclear CoII SMMs based on curcuminoid ligands. United States: N. p., 2016. Web. doi:10.1039/c5sc03298a.
Díaz-Torres, Raúl, Menelaou, Melita, Roubeau, Olivier, Sorrenti, Alessandro, Brandariz-de-Pedro, Guillem, Sañudo, E. Carolina, Teat, Simon J., Fraxedas, Jordi, Ruiz, Eliseo, & Aliaga-Alcalde, Núria. Multiscale study of mononuclear CoII SMMs based on curcuminoid ligands. United States. https://doi.org/10.1039/c5sc03298a
Díaz-Torres, Raúl, Menelaou, Melita, Roubeau, Olivier, Sorrenti, Alessandro, Brandariz-de-Pedro, Guillem, Sañudo, E. Carolina, Teat, Simon J., Fraxedas, Jordi, Ruiz, Eliseo, and Aliaga-Alcalde, Núria. Thu . "Multiscale study of mononuclear CoII SMMs based on curcuminoid ligands". United States. https://doi.org/10.1039/c5sc03298a. https://www.osti.gov/servlets/purl/1377417.
@article{osti_1377417,
title = {Multiscale study of mononuclear CoII SMMs based on curcuminoid ligands},
author = {Díaz-Torres, Raúl and Menelaou, Melita and Roubeau, Olivier and Sorrenti, Alessandro and Brandariz-de-Pedro, Guillem and Sañudo, E. Carolina and Teat, Simon J. and Fraxedas, Jordi and Ruiz, Eliseo and Aliaga-Alcalde, Núria},
abstractNote = {This work introduces a novel family of CoII species having a curcuminoid (CCMoid) ligand, 9Accm, attached, namely [Co(9Accm) 2 (py) 2 ] (1) and [Co(9Accm)2(2,2'-bpy)] (2), achieved in high yields by the use of a microwave reactor, and exhibiting two different arrangements for the 9Accm ligands, described as "cis"(2) and "trans"(1). The study of the similarities/differences of the magnetic, luminescent and surface behaviors of the two new species, 1 and 2, is the main objective of the present work. The determined single-crystal structures of both compounds are the only CoII -CCMoid structures described in the literature so far. Both compounds exhibit large positive D values, that of 1 (D = +74 cm-1 ) being three times larger than that of 2 (D = +24 cm-1 ), and behave as mononuclear Single-Molecule Magnets (SMMs) in the presence of an external magnetic field. Their similar structures but different anisotropy and SMM characteristics provide, for the first time, deep insight on the spin-orbital effects thanks to the use of CASSCF/NEVPT2 calculations implementing such contributions. Further magnetic studies were performed in solution by means of paramagnetic 1H NMR, where both compounds (1 and 2) are stable in CDCl3 and display high symmetry. Paramagnetic NMR appears to be a useful diagnostic tool for the identification of such molecules in solution, where the resonance values found for the methine group (-CH-) of 9Accm vary significantly depending on the cis or trans disposition of the ligands. Fluorescence studies show that both systems display chelation enhancement of quenching (CHEQ) with regard to the free ligand, while 1 and 2 display similar quantum yields. Deposition of 1-2 on HOPG and Si(100) surfaces using spin-coating was studied using AFM; UV photoemission experiments under the same conditions display 2 as the most robust system. The measured occupied density of states of 2 with UV photoemission is in excellent agreement with theoretical DFT calculations.},
doi = {10.1039/c5sc03298a},
journal = {Chemical Science},
number = 4,
volume = 7,
place = {United States},
year = {2016},
month = {1}
}

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Structural characterization and magnetic property studies of a mixed-valence {Co III CoII4} complex with a μ 4 -oxo tetrahedral {CoII4} motif
journal, January 2020

  • Fiorini, Guillermo; Carrella, Luca; Rentschler, Eva
  • Dalton Transactions, Vol. 49, Issue 3
  • DOI: 10.1039/c9dt03561c

Influence of ligand field on magnetic anisotropy in a family of pentacoordinate Co II complexes
journal, January 2020

  • Acharya, Joydev; Sarkar, Arup; Kumar, Pawan
  • Dalton Transactions, Vol. 49, Issue 15
  • DOI: 10.1039/d0dt00315h

Structure, magnetic anisotropy and relaxation behavior of seven-coordinate Co( ii ) single-ion magnets perturbed by counter-anions
journal, January 2020

  • Yi, Gangji; Zhang, Chunyang; Zhao, Wen
  • Dalton Transactions, Vol. 49, Issue 22
  • DOI: 10.1039/d0dt01232g

A Co(II)-Hydrazone Schiff Base Single Ion Magnet Exhibiting Field Induced Slow Relaxation Dynamics
journal, December 2018