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Title: Controlled Heterometallic Composition in Linear Trinuclear [LnCeLn] Lanthanide Molecular Assemblies

Abstract

Here, the combination of two different β-diketone ligands facilitates the size-controlled assembly of pure heterometallic [LnLn'Ln] linear compounds thanks to two different coordination sites present in the molecular scaffold. [HoCeHo], [ErCeEr], and [YbCeYb] analogues are presented here and are characterized both in the solid state and in solution, demonstrating the selectivity of this unique method to produce heterometallic 4f molecular entities.

Authors:
 [1];  [1];  [1]; ORCiD logo [2];  [2];  [3]; ORCiD logo [1]; ORCiD logo [1]
  1. University of Barcelona (Spain)
  2. Univ. de Zaragoza (Spain)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
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:
1581608
Alternate Identifier(s):
OSTI ID: 1571306
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry - A European Journal
Additional Journal Information:
Journal Volume: 25; Journal Issue: 67; Journal ID: ISSN 0947-6539
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; coordination chemistry; heterometallic complexes; lanthanides; ligand design; quantum computing

Citation Formats

Velasco, Verónica, Barrios, Leoní A., Schütze, Mike, Roubeau, Olivier, Luis, Fernando, Teat, Simon J., Aguilà, David, and Aromí, Guillem. Controlled Heterometallic Composition in Linear Trinuclear [LnCeLn] Lanthanide Molecular Assemblies. United States: N. p., 2019. Web. https://doi.org/10.1002/chem.201903829.
Velasco, Verónica, Barrios, Leoní A., Schütze, Mike, Roubeau, Olivier, Luis, Fernando, Teat, Simon J., Aguilà, David, & Aromí, Guillem. Controlled Heterometallic Composition in Linear Trinuclear [LnCeLn] Lanthanide Molecular Assemblies. United States. https://doi.org/10.1002/chem.201903829
Velasco, Verónica, Barrios, Leoní A., Schütze, Mike, Roubeau, Olivier, Luis, Fernando, Teat, Simon J., Aguilà, David, and Aromí, Guillem. Tue . "Controlled Heterometallic Composition in Linear Trinuclear [LnCeLn] Lanthanide Molecular Assemblies". United States. https://doi.org/10.1002/chem.201903829. https://www.osti.gov/servlets/purl/1581608.
@article{osti_1581608,
title = {Controlled Heterometallic Composition in Linear Trinuclear [LnCeLn] Lanthanide Molecular Assemblies},
author = {Velasco, Verónica and Barrios, Leoní A. and Schütze, Mike and Roubeau, Olivier and Luis, Fernando and Teat, Simon J. and Aguilà, David and Aromí, Guillem},
abstractNote = {Here, the combination of two different β-diketone ligands facilitates the size-controlled assembly of pure heterometallic [LnLn'Ln] linear compounds thanks to two different coordination sites present in the molecular scaffold. [HoCeHo], [ErCeEr], and [YbCeYb] analogues are presented here and are characterized both in the solid state and in solution, demonstrating the selectivity of this unique method to produce heterometallic 4f molecular entities.},
doi = {10.1002/chem.201903829},
journal = {Chemistry - A European Journal},
number = 67,
volume = 25,
place = {United States},
year = {2019},
month = {9}
}

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Works referenced in this record:

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Discriminating between lanthanide ions: self-assembly of heterodimetallic triple-stranded helicates
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    Works referencing / citing this record:

    Indium-Catalyzed Retro-Claisen Condensation
    journal, October 2007

    • Kawata, Atsushi; Takata, Kazumi; Kuninobu, Yoichiro
    • Angewandte Chemie, Vol. 119, Issue 41
    • DOI: 10.1002/ange.200702798

    Cryogenic Magnetocaloric Effect in a Ferromagnetic Molecular Dimer
    journal, June 2011

    • Evangelisti, Marco; Roubeau, Olivier; Palacios, Elias
    • Angewandte Chemie, Vol. 123, Issue 29
    • DOI: 10.1002/ange.201102640

    A Dysprosium Metallocene Single-Molecule Magnet Functioning at the Axial Limit
    journal, July 2017

    • Guo, Fu-Sheng; Day, Benjamin M.; Chen, Yan-Cong
    • Angewandte Chemie, Vol. 129, Issue 38
    • DOI: 10.1002/ange.201705426

    Indium-Catalyzed Retro-Claisen Condensation
    journal, October 2007

    • Kawata, Atsushi; Takata, Kazumi; Kuninobu, Yoichiro
    • Angewandte Chemie International Edition, Vol. 46, Issue 41
    • DOI: 10.1002/anie.200702798

    Cryogenic Magnetocaloric Effect in a Ferromagnetic Molecular Dimer
    journal, June 2011

    • Evangelisti, Marco; Roubeau, Olivier; Palacios, Elias
    • Angewandte Chemie International Edition, Vol. 50, Issue 29
    • DOI: 10.1002/anie.201102640

    A Dysprosium Metallocene Single-Molecule Magnet Functioning at the Axial Limit
    journal, July 2017

    • Guo, Fu-Sheng; Day, Benjamin M.; Chen, Yan-Cong
    • Angewandte Chemie International Edition, Vol. 56, Issue 38
    • DOI: 10.1002/anie.201705426

    Programming Heteropolymetallic Lanthanide Helicates: Thermodynamic Recognition of Different Metal Ions Along the Strands
    journal, March 2004

    • Floquet, Sébastien; Borkovec, Michal; Bernardinelli, Gérald
    • Chemistry - A European Journal, Vol. 10, Issue 5
    • DOI: 10.1002/chem.200305498

    A Metal-Organic Framework as Attractive Cryogenic Magnetorefrigerant
    journal, August 2012

    • Sibille, Romain; Mazet, Thomas; Malaman, Bernard
    • Chemistry - A European Journal, Vol. 18, Issue 41
    • DOI: 10.1002/chem.201200861

    Lanthanide Contraction within a Series of Asymmetric Dinuclear [Ln 2 ] Complexes
    journal, March 2013

    • Aguilà, David; Barrios, Leoní A.; Velasco, Verónica
    • Chemistry - A European Journal, Vol. 19, Issue 19
    • DOI: 10.1002/chem.201204451

    Heterodinuclear Lanthanoid-Containing Polyoxometalates: Stepwise Synthesis and Single-Molecule Magnet Behavior
    journal, September 2013

    • Sato, Rinta; Suzuki, Kosuke; Sugawa, Midori
    • Chemistry - A European Journal, Vol. 19, Issue 39
    • DOI: 10.1002/chem.201302596

    Thermodynamic Stability of Heterodimetallic [LnLn′] Complexes: Synthesis and DFT Studies
    journal, March 2017

    • Gónzalez-Fabra, Joan; Bandeira, Nuno A. G.; Velasco, Verónica
    • Chemistry - A European Journal, Vol. 23, Issue 21
    • DOI: 10.1002/chem.201700095

    An Efficient Iron-Catalyzed Carbon-Carbon Single-Bond Cleavage via Retro-Claisen Condensation: A Mild and Convenient Approach to Synthesize a Variety of Esters or Ketones
    journal, April 2010

    • Biswas, Srijit; Maiti, Sukhendu; Jana, Umasish
    • European Journal of Organic Chemistry, Vol. 2010, Issue 15
    • DOI: 10.1002/ejoc.201000128

    Shape maps and polyhedral interconversion paths in transition metal chemistry
    journal, September 2005

    • Alvarez, S.; Alemany, P.; Casanova, D.
    • Coordination Chemistry Reviews, Vol. 249, Issue 17-18
    • DOI: 10.1016/j.ccr.2005.03.031

    A Long Journey in Lanthanide Chemistry: From Fundamental Crystallogenesis Studies to Commercial Anticounterfeiting Taggants
    journal, April 2016

    • Guillou, Olivier; Daiguebonne, Carole; Calvez, Guillaume
    • Accounts of Chemical Research, Vol. 49, Issue 5
    • DOI: 10.1021/acs.accounts.6b00058

    Selective Lanthanide Distribution within a Comprehensive Series of Heterometallic [LnPr] Complexes
    journal, June 2018


    Lanthanide Single-Molecule Magnets
    journal, March 2013

    • Woodruff, Daniel N.; Winpenny, Richard E. P.; Layfield, Richard A.
    • Chemical Reviews, Vol. 113, Issue 7
    • DOI: 10.1021/cr400018q

    Upconversion Luminescent Materials: Advances and Applications
    journal, November 2014

    • Zhou, Jing; Liu, Qian; Feng, Wei
    • Chemical Reviews, Vol. 115, Issue 1
    • DOI: 10.1021/cr400478f

    Structure-Based Description of a Step-by-Step Synthesis of Homo- and Heterodinuclear (4f, 4f ‘) Lanthanide Complexes
    journal, October 2003

    • Costes, Jean-Pierre; Dahan, Françoise; Nicodème, Franck
    • Inorganic Chemistry, Vol. 42, Issue 20
    • DOI: 10.1021/ic034564q

    Supramolecular Recognition of Heteropairs of Lanthanide Ions:  A Step toward Self-Assembled Bifunctional Probes
    journal, January 2004

    • André, Nicolas; Jensen, Thomas B.; Scopelliti, Rosario
    • Inorganic Chemistry, Vol. 43, Issue 2
    • DOI: 10.1021/ic0351996

    Synthesis and Properties of a Family of Unsymmetric Dinuclear Complexes of Ln III (Ln = Eu, Gd, Tb)
    journal, August 2010

    • Aguilà, David; Barrios, Leoní A.; Luis, Fernando
    • Inorganic Chemistry, Vol. 49, Issue 15
    • DOI: 10.1021/ic1008285

    Revised Ionic Radii of Lanthanoid(III) Ions in Aqueous Solution
    journal, May 2011

    • D’Angelo, Paola; Zitolo, Andrea; Migliorati, Valentina
    • Inorganic Chemistry, Vol. 50, Issue 10
    • DOI: 10.1021/ic200260r

    Lanthanide Double-Decker Complexes Functioning as Magnets at the Single-Molecular Level
    journal, July 2003

    • Ishikawa, Naoto; Sugita, Miki; Ishikawa, Tadahiko
    • Journal of the American Chemical Society, Vol. 125, Issue 29
    • DOI: 10.1021/ja029629n

    Lanthanide-Sensitized Lanthanide Luminescence:  Terbium-Sensitized Ytterbium Luminescence in a Trinuclear Complex
    journal, September 2003

    • Faulkner, Stephen; Pope, Simon J. A.
    • Journal of the American Chemical Society, Vol. 125, Issue 35
    • DOI: 10.1021/ja035634v

    Purely Heterometallic Lanthanide(III) Macrocycles through Controlled Assembly of Disulfide Bonds for Dual Color Emission
    journal, February 2011

    • Lewis, David J.; Glover, Peter B.; Solomons, Melissa C.
    • Journal of the American Chemical Society, Vol. 133, Issue 4
    • DOI: 10.1021/ja109157g

    Heterodimetallic [LnLn′] Lanthanide Complexes: Toward a Chemical Design of Two-Qubit Molecular Spin Quantum Gates
    journal, August 2014

    • Aguilà, David; Barrios, Leoní A.; Velasco, Verónica
    • Journal of the American Chemical Society, Vol. 136, Issue 40
    • DOI: 10.1021/ja507809w

    Synthesis and Spectroscopic Studies on Azo-Dye Derivatives of Polymetallic Lanthanide Complexes: Using Diazotization to Link Metal Complexes Together
    journal, July 2009

    • Placidi, Matteo P.; Villaraza, Aaron Joseph L.; Natrajan, Louise S.
    • Journal of the American Chemical Society, Vol. 131, Issue 29
    • DOI: 10.1021/ja904362f

    Toward Molecular 4f Single-Ion Magnet Qubits
    journal, April 2016

    • Pedersen, Kasper S.; Ariciu, Ana-Maria; McAdams, Simon
    • Journal of the American Chemical Society, Vol. 138, Issue 18
    • DOI: 10.1021/jacs.6b02702

    Coherent Manipulation of a Molecular Ln-Based Nuclear Qudit Coupled to an Electron Qubit
    journal, July 2018

    • Hussain, Riaz; Allodi, Giuseppe; Chiesa, Alessandro
    • Journal of the American Chemical Society, Vol. 140, Issue 31
    • DOI: 10.1021/jacs.8b05934

    Molecular magnetic hysteresis at 60 kelvin in dysprosocenium
    journal, August 2017

    • Goodwin, Conrad A. P.; Ortu, Fabrizio; Reta, Daniel
    • Nature, Vol. 548, Issue 7668
    • DOI: 10.1038/nature23447

    Discriminating between lanthanide ions: self-assembly of heterodimetallic triple-stranded helicates
    journal, January 2002

    • André, Nicolas; Scopelliti, Rosario; Hopfgartner, Gérard
    • Chemical Communications, Issue 3
    • DOI: 10.1039/b109065h

    Controlled preparation of a heterometallic lanthanide complex containing different lanthanides in symmetrical binding pockets
    journal, January 2009

    • Natrajan, Louise S.; Villaraza, Aaron Joseph L.; Kenwright, Alan M.
    • Chemical Communications, Issue 40
    • DOI: 10.1039/b913702e

    Synthesis and characterization of dinuclear heterometallic lanthanide complexes exhibiting MRI and luminescence response
    journal, January 2010

    • Mamedov, Ilgar; Parac-Vogt, Tatjana N.; Logothetis, Nikos K.
    • Dalton Transactions, Vol. 39, Issue 24
    • DOI: 10.1039/b925556g

    Self-assembly between dicarboxylate ions and a binuclear europium complex: formation of stable adducts and heterometallic lanthanide complexes
    journal, January 2011

    • Tilney, James A.; Sørensen, Thomas Just; Burton-Pye, Benjamin P.
    • Dalton Transactions, Vol. 40, Issue 45
    • DOI: 10.1039/c1dt11103e

    Increasing the dimensionality of cryogenic molecular coolers: Gd-based polymers and metal–organic frameworks
    journal, January 2012

    • Lorusso, Giulia; Palacios, Maria A.; Nichol, Gary S.
    • Chemical Communications, Vol. 48, Issue 61
    • DOI: 10.1039/c2cc33485b