Molecular multifunctionality preservation upon surface deposition for a chiral single-molecule magnet

Dmitri Mitcov; Anders H. Pedersen; Marcel Ceccato; Rikke M. Gelardi; Tue Hassenkam; Andreas Konstantatos; Anders Reinholdt; Mikkel A. Sørensen; Peter W. Thulstrup; Morten G. Vinum; Fabrice Wilhelm; Andrei Rogalev; Wolfgang Wernsdorfer; Euan K. Brechin; Stergios Piligkos

doi:10.1039/c8sc04917c

Molecular multifunctionality preservation upon surface deposition for a chiral single-molecule magnet

Dmitri Mitcov, Anders H. Pedersen, Marcel Ceccato, Rikke M. Gelardi, Tue Hassenkam, Andreas Konstantatos, Anders Reinholdt, Mikkel A. Sørensen, Peter W. Thulstrup, Morten G. Vinum, Fabrice Wilhelm, Andrei Rogalev, Wolfgang Wernsdorfer, Euan K. Brechin, Stergios Piligkos^*

^*Corresponding author for this work

7 Citations (Scopus)

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Abstract

The synthesis and characterization of a chiral, enneanuclear Mn(iii)-based, Single-Molecule Magnet, [Mn₉O₄(Me-sao)₆(L)₃(MeO)₃(MeOH)₃]Cl (1; Me-saoH₂ = methylsalicylaldoxime, HL = lipoic acid) is reported. Compound 1 crystallizes in the orthorhombic P2₁2₁2₁ space group and consists of a metallic skeleton describing a defect super-tetrahedron missing one vertex. The chirality of the [Mn^III₉] core originates from the directional bridging of the Me-sao^2- ligands via the -N-O- oximate moieties, which define a clockwise (1ΔΔ) or counter-clockwise (1ΛΛ) rotation in both the upper [Mn^III₃] and lower [Mn^III₆] subunits. Structural integrity and retention of chirality upon dissolution and upon deposition on (a) gold nanoparticles, 1@AuNPs, (b) transparent Au(111) surfaces, 1ΛΛ@t-Au(111); 1ΔΔ@t-Au(111), and (c) epitaxial Au(111) on mica surfaces, 1@e-Au(111), was confirmed by CD and IR spectroscopies, mass spectrometry, TEM, XPS, XAS, and AFM. Magnetic susceptibility and magnetization measurements demonstrate the simultaneous retention of SMM behaviour and optical activity, from the solid state, via dissolution, to the surface deposited species.

Original language	English
Journal	Chemical Science
Volume	10
Issue number	10
Pages (from-to)	3065-3073
Number of pages	9
ISSN	2041-6520
DOIs	https://doi.org/10.1039/c8sc04917c
Publication status	Published - 1 Jan 2019

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10.1039/c8sc04917cLicence: CC BY-NC

Molecular multifunctionality preservation upon surface deposition for a chiral single-molecule magnetFinal published version, 1.3 MBLicence: CC BY-NC

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Mitcov, D., Pedersen, A. H., Ceccato, M., Gelardi, R. M., Hassenkam, T., Konstantatos, A., Reinholdt, A., Sørensen, M. A., Thulstrup, P. W., Vinum, M. G., Wilhelm, F., Rogalev, A., Wernsdorfer, W., Brechin, E. K., & Piligkos, S. (2019). Molecular multifunctionality preservation upon surface deposition for a chiral single-molecule magnet. Chemical Science, 10(10), 3065-3073. https://doi.org/10.1039/c8sc04917c

Mitcov, D, Pedersen, AH, Ceccato, M, Gelardi, RM, Hassenkam, T, Konstantatos, A, Reinholdt, A, Sørensen, MA, Thulstrup, PW, Vinum, MG, Wilhelm, F, Rogalev, A, Wernsdorfer, W, Brechin, EK & Piligkos, S 2019, 'Molecular multifunctionality preservation upon surface deposition for a chiral single-molecule magnet', Chemical Science, vol. 10, no. 10, pp. 3065-3073. https://doi.org/10.1039/c8sc04917c

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title = "Molecular multifunctionality preservation upon surface deposition for a chiral single-molecule magnet",

abstract = "The synthesis and characterization of a chiral, enneanuclear Mn(iii)-based, Single-Molecule Magnet, [Mn9O4(Me-sao)6(L)3(MeO)3(MeOH)3]Cl (1; Me-saoH2 = methylsalicylaldoxime, HL = lipoic acid) is reported. Compound 1 crystallizes in the orthorhombic P212121 space group and consists of a metallic skeleton describing a defect super-tetrahedron missing one vertex. The chirality of the [MnIII9] core originates from the directional bridging of the Me-sao2- ligands via the -N-O- oximate moieties, which define a clockwise (1ΔΔ) or counter-clockwise (1ΛΛ) rotation in both the upper [MnIII3] and lower [MnIII6] subunits. Structural integrity and retention of chirality upon dissolution and upon deposition on (a) gold nanoparticles, 1@AuNPs, (b) transparent Au(111) surfaces, 1ΛΛ@t-Au(111); 1ΔΔ@t-Au(111), and (c) epitaxial Au(111) on mica surfaces, 1@e-Au(111), was confirmed by CD and IR spectroscopies, mass spectrometry, TEM, XPS, XAS, and AFM. Magnetic susceptibility and magnetization measurements demonstrate the simultaneous retention of SMM behaviour and optical activity, from the solid state, via dissolution, to the surface deposited species.",

author = "Dmitri Mitcov and Pedersen, {Anders H.} and Marcel Ceccato and Gelardi, {Rikke M.} and Tue Hassenkam and Andreas Konstantatos and Anders Reinholdt and S{\o}rensen, {Mikkel A.} and Thulstrup, {Peter W.} and Vinum, {Morten G.} and Fabrice Wilhelm and Andrei Rogalev and Wolfgang Wernsdorfer and Brechin, {Euan K.} and Stergios Piligkos",

year = "2019",

month = jan,

day = "1",

doi = "10.1039/c8sc04917c",

language = "English",

volume = "10",

pages = "3065--3073",

journal = "Chemical Science",

issn = "2041-6520",

publisher = "Royal Society of Chemistry",

number = "10",

}

TY - JOUR

T1 - Molecular multifunctionality preservation upon surface deposition for a chiral single-molecule magnet

AU - Mitcov, Dmitri

AU - Pedersen, Anders H.

AU - Ceccato, Marcel

AU - Gelardi, Rikke M.

AU - Hassenkam, Tue

AU - Konstantatos, Andreas

AU - Reinholdt, Anders

AU - Sørensen, Mikkel A.

AU - Thulstrup, Peter W.

AU - Vinum, Morten G.

AU - Wilhelm, Fabrice

AU - Rogalev, Andrei

AU - Wernsdorfer, Wolfgang

AU - Brechin, Euan K.

AU - Piligkos, Stergios

PY - 2019/1/1

Y1 - 2019/1/1

N2 - The synthesis and characterization of a chiral, enneanuclear Mn(iii)-based, Single-Molecule Magnet, [Mn9O4(Me-sao)6(L)3(MeO)3(MeOH)3]Cl (1; Me-saoH2 = methylsalicylaldoxime, HL = lipoic acid) is reported. Compound 1 crystallizes in the orthorhombic P212121 space group and consists of a metallic skeleton describing a defect super-tetrahedron missing one vertex. The chirality of the [MnIII9] core originates from the directional bridging of the Me-sao2- ligands via the -N-O- oximate moieties, which define a clockwise (1ΔΔ) or counter-clockwise (1ΛΛ) rotation in both the upper [MnIII3] and lower [MnIII6] subunits. Structural integrity and retention of chirality upon dissolution and upon deposition on (a) gold nanoparticles, 1@AuNPs, (b) transparent Au(111) surfaces, 1ΛΛ@t-Au(111); 1ΔΔ@t-Au(111), and (c) epitaxial Au(111) on mica surfaces, 1@e-Au(111), was confirmed by CD and IR spectroscopies, mass spectrometry, TEM, XPS, XAS, and AFM. Magnetic susceptibility and magnetization measurements demonstrate the simultaneous retention of SMM behaviour and optical activity, from the solid state, via dissolution, to the surface deposited species.

AB - The synthesis and characterization of a chiral, enneanuclear Mn(iii)-based, Single-Molecule Magnet, [Mn9O4(Me-sao)6(L)3(MeO)3(MeOH)3]Cl (1; Me-saoH2 = methylsalicylaldoxime, HL = lipoic acid) is reported. Compound 1 crystallizes in the orthorhombic P212121 space group and consists of a metallic skeleton describing a defect super-tetrahedron missing one vertex. The chirality of the [MnIII9] core originates from the directional bridging of the Me-sao2- ligands via the -N-O- oximate moieties, which define a clockwise (1ΔΔ) or counter-clockwise (1ΛΛ) rotation in both the upper [MnIII3] and lower [MnIII6] subunits. Structural integrity and retention of chirality upon dissolution and upon deposition on (a) gold nanoparticles, 1@AuNPs, (b) transparent Au(111) surfaces, 1ΛΛ@t-Au(111); 1ΔΔ@t-Au(111), and (c) epitaxial Au(111) on mica surfaces, 1@e-Au(111), was confirmed by CD and IR spectroscopies, mass spectrometry, TEM, XPS, XAS, and AFM. Magnetic susceptibility and magnetization measurements demonstrate the simultaneous retention of SMM behaviour and optical activity, from the solid state, via dissolution, to the surface deposited species.

U2 - 10.1039/c8sc04917c

DO - 10.1039/c8sc04917c

M3 - Journal article

C2 - 30996888

AN - SCOPUS:85062631871

SN - 2041-6520

VL - 10

SP - 3065

EP - 3073

JO - Chemical Science

JF - Chemical Science

IS - 10

ER -

Molecular multifunctionality preservation upon surface deposition for a chiral single-molecule magnet

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