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 »
- Authors:
-
[1];
[2];
[4];
[6];
[7];
[8]
- Univ. de Barcelona (Spain). Dept. de Quimica Inorganica
- Inst. de Ciencia de Materials de Aragon (ICMAP-CSIC), Zaragoza (Spain); Univ. de Zaragoza (Spain)
- CSIC-ICMAB (Institut de Ciència dels Materials de Barcelona) Campus de la Universitat Autònoma de Barcelona; 08193 Bellaterra, Spain
- Univ. de Barcelona (Spain). Dept. de Quimica Inorganica and Inst. de Nanociencia i Nanotecnologia-UB
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
- Catalan Inst. of Nanoscience and Nanotechnology (ICN2), Consejo Superior de Investigaciones Cientificas (CSIC) and The Barcelona Inst. of Science and Technology, Barcelona (Spain)
- Univ. de Barcelona (Spain). Dept. de Quimica Inorganica; Univ. de Barcelona (Spain). Inst. de QuiÂmica Teorica i Computacional
- 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. 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, and Aliaga-Alcalde, Núria. Thu .
"Multiscale study of mononuclear CoII SMMs based on curcuminoid ligands". United States. doi: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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Works referencing / citing this record:
A Click-Functionalized Single-Molecule Magnet Based on Cobalt(II) and Its Analogous Manganese(II) and Zinc(II) Compounds: A Click-Functionalized Single-Molecule Magnet
journal, December 2014
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