| 1. |
- Baljozovic, Milos, et al.
(författare)
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Self-Assembly and Magnetic Order of Bi-Molecular 2D Spin Lattices of M(II,III) Phthalocyanines on Au(111)
- 2021
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Ingår i: MAGNETOCHEMISTRY. - : MDPI. - 2312-7481. ; 7:8
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Tidskriftsartikel (refereegranskat)abstract
- Single layer low-dimensional materials are presently of emerging interest, including in the context of magnetism. In the present report, on-surface supramolecular architecturing was further developed and employed to create surface supported two-dimensional binary spin arrays on atomically clean non-magnetic Au(111). By chemical programming of the modules, different checkerboards were produced combining phthalocyanines containing metals of different oxidation and spin states, diamagnetic zinc, and a metal-free 'spacer'. In an in-depth, spectro-microscopy and theoretical account, we correlate the structure and the magnetic properties of these tunable systems and discuss the emergence of 2D Kondo magnetism from the spin-bearing components and via the physico-chemical bonding to the underlying substrate. The contributions of the individual elements, as well as the role of the electronic surface state in the bottom substrate, are discussed, also looking towards further in-depth investigations.
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| 2. |
- Girovsky, Jan, et al.
(författare)
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Long-range ferrimagnetic order in a two-dimensional supramolecular Kondo lattice
- 2017
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 8
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Tidskriftsartikel (refereegranskat)abstract
- Realization of long-range magnetic order in surface-supported two-dimensional systems has been challenging, mainly due to the competition between fundamental magnetic interactions as the short-range Kondo effect and spin-stabilizing magnetic exchange interactions. Spin-bearing molecules on conducting substrates represent a rich platform to investigate the interplay of these fundamental magnetic interactions. Here we demonstrate the direct observation of long-range ferrimagnetic order emerging in a two-dimensional supramolecular Kondo lattice. The lattice consists of paramagnetic hexadeca-fluorinated iron phthalocyanine (FeFPc) and manganese phthalocyanine (MnPc) molecules co-assembled into a checkerboard pattern on single-crystalline Au(111) substrates. Remarkably, the remanent magnetic moments are oriented in the out-of-plane direction with significant contribution from orbital moments. First-principles calculations reveal that the FeFPc-MnPc antiferromagnetic nearest-neighbour coupling is mediated by the Ruderman-Kittel-Kasuya-Yosida exchange interaction via the Au substrate electronic states. Our findings suggest the use of molecular frameworks to engineer novel low-dimensional magnetically ordered materials and their application in molecular quantum devices.
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| 3. |
- Avdoshenko, S. M., et al.
(författare)
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Partial magnetic ordering in one-dimensional arrays of endofullerene single-molecule magnet peapods
- 2018
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Ingår i: Nanoscale. - 2040-3372. ; , s. 18153-18160
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Tidskriftsartikel (refereegranskat)abstract
- The magnetic ordering and bistability of one-dimensional chains of endofullerene Dy2ScN@C80 single-molecule magnets (SMMs) packed inside single-walled carbon nanotubes (SWCNTs) have been studied using high-resolution transmission electron microscopy (HRTEM), X-ray magnetic circular dichroism (XMCD), and ab initio calculations. X-ray absorption measurements reveal that the orientation of the encapsulated endofullerenes differs from the isotropic distribution in the bulk sample, indicating a partial ordering of the endofullerenes inside the SWCNTs. The effect of the one-dimensional packing was further investigated by ab initio calculations, demonstrating that for specific tube diameters, the encapsulation is leading to energetically preferential orientations of the endohedral clusters. Additionally, element-specific magnetization curves reveal a decreased magnetic bistability of the encapsulated Dy2ScN@C80 SMMs compared to the bulk analog.
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| 4. |
- Caputo, Marco, et al.
(författare)
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Charge Transfer and Orbital Reconstruction at an Organic-Oxide Interface
- 2023
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Ingår i: Nano Letters. - 1530-6984. ; 23:23, s. 11211-11218
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Tidskriftsartikel (refereegranskat)abstract
- The two-dimensional electron system (2DES) located at the surface of strontium titanate (STO) and at several other STO-based interfaces has been an established platform for the study of novel physical phenomena since its discovery. Here we report how the interfacing of STO and tetracyanoquinodimethane (TCNQ) results in a charge transfer that depletes the number of free carriers at the STO surface, with a strong impact on its electronic structure. Our study paves the way for efficient tuning of the electronic properties, which promises novel applications in the framework of oxide/organic-based electronics.
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| 5. |
- Dreiser, Jan, et al.
(författare)
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Direct observation of a ferri-to-ferromagnetic transition in a fluoride-bridged 3d-4f molecular cluster
- 2012
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Ingår i: Chemical Science. - : Royal Society of Chemistry (RSC). - 2041-6520. ; 3:4, s. 1024-1032
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Tidskriftsartikel (refereegranskat)abstract
- We report on the synthesis, crystal structure and magnetic characterisation of the trinuclear, fluoride-bridged, molecular nanomagnet [Dy(hfac)(3)(H2O)-CrF2(py)(4)-Dy(hfac)(3)(NO3)] (1) (hfacH = 1,1,1,5,5,5-hexafluoroacetylacetone, py = pyridine) and a closely related dinuclear species [Dy(hfac)(4)-CrF2( py)(4)]center dot 1/2 CHCl3 (2). Element-specific magnetisation curves obtained on 1 by X-ray magnetic circular dichroism (XMCD) allow us to directly observe the field-induced transition from a ferrimagnetic to a ferromagnetic arrangement of the Dy and Cr magnetic moments. By fitting a spin-Hamiltonian model to the XMCD data we extract a weak antiferromagnetic exchange coupling of j -0.18 cm(-1) between the Dy-III and Cr-III ions. The value found from XMCD is consistent with SQUID magnetometry and inelastic neutron scattering measurements. Furthermore, alternating current susceptibility and muon-spin relaxation measurements reveal that 1 shows thermally activated relaxation of magnetisation with a small effective barrier for magnetisation reversal of Delta(eff) 3 cm(-1). Density-functional theory calculations show that the Dy-Cr couplings originate from superexchange via the fluoride bridges.
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| 6. |
- Dreiser, Jan, et al.
(författare)
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Exchange Interaction of Strongly Anisotropic Tripodal Erbium Single-Ion Magnets with Metallic Surfaces
- 2014
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Ingår i: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 8:5, s. 4662-4671
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Tidskriftsartikel (refereegranskat)abstract
- We present a comprehensive study of Er(trensal) single-ion magnets deposited in ultrahigh vacuum onto metallic surfaces. X-ray photoelectron spectroscopy reveals that the molecular structure is preserved after sublimation, and that the molecules are physisorbed on Au(111) while they are chemisorbed on a Ni thin film on 0(100) single-crystalline surfaces. X-ray magnetic circular dichroism (XMCD) measurements performed on Au(111) samples covered with molecular monolayers held at temperatures down to 4 K suggest that the easy axes of the strongly anisotropic molecules are randomly oriented. Furthermore XMCD indicates a weak antiferromagnetic exchange coupling between the single-ion magnets and the ferromagnetic Ni/Cu(100) substrate. For the latter case, spin-Hamiltonian fits to the XMCD M(H) suggest a significant structural distortion of the molecules. Scanning tunneling microscopy reveals that the molecules are mobile on Au(111) at room temperature, whereas they are more strongly attached on Ni/Cu(100). X-ray photoelectron spectroscopy results provide evidence for the chemical bonding between Er(trensal) molecules and the Ni substrate. Density functional theory calculations support these findings and, in addition, reveal the most stable adsorption configuration on Ni/Cu(100) as well as the Ni-Er exchange path. Our study suggests that the magnetic moment of Er(trensal) can be stabilized via suppression of quantum tunneling of magnetization by exchange coupling to the Ni surface atoms. Moreover, it opens up pathways toward optical addressing of surface-deposited single-ion magnets.
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| 7. |
- Dreiser, Jan, et al.
(författare)
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The Metallofullerene Field-Induced Single-Ion Magnet HoSc2N@C-80
- 2014
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Ingår i: Chemistry - A European Journal. - : Wiley. - 0947-6539 .- 1521-3765. ; 20:42, s. 13536-13540
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Tidskriftsartikel (refereegranskat)abstract
- The low-temperature magnetic properties of the endohedral metallofullerene HoSc2N@C-80 have been studied by superconducting quantum interference device (SQUID) magnetometry. Alternating current (ac) susceptibility measurements reveal that this molecule exhibits slow relaxation of magnetization in a small applied field with timescales in the order of milliseconds. The equilibrium magnetic properties of HoSc2N@C-80 indicate strong magnetic anisotropy. The large differences in magnetization relaxation times between the present compound and the previously investigated DySc2N@C-80 are discussed.
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| 8. |
- Dreiser, Jan, et al.
(författare)
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X-ray induced demagnetization of single-molecule magnets
- 2014
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Ingår i: Applied Physics Letters. - : AIP Publishing. - 0003-6951 .- 1077-3118. ; 105:3, s. 032411-
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Tidskriftsartikel (refereegranskat)abstract
- Low-temperature x-ray magnetic circular dichroism measurements on the endohedral single-molecule magnet DySc2N@C-80 at the Dy M-4,M-5 edges reveal a shrinking of the opening of the observed hysteresis with increasing x-ray flux. Time-dependent measurements show that the exposure of the molecules to x-rays resonant with the Dy M-5 edge accelerates the relaxation of magnetization more than off-resonant x-rays. The results cannot be explained by a homogeneous temperature rise due to x-ray absorption. Moreover, the observed large demagnetization cross sections indicate that the resonant absorption of one x-ray photon induces the demagnetization of many molecules.
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| 9. |
- Fritz, Fabian, et al.
(författare)
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Nanoscale X-ray investigation of magnetic metallofullerene peapods
- 2017
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Ingår i: Nanotechnology. - : IOP Publishing. - 0957-4484 .- 1361-6528. ; 28:43
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Tidskriftsartikel (refereegranskat)abstract
- Endohedral lanthanide ions packed inside carbon nanotubes (CNTs) in a one-dimensional assembly have been studied with a combination of high resolution transmission electron microscopy (HRTEM), scanning transmission X-ray microscopy (STXM), and X-ray magnetic circular dichroism (XMCD). By correlating HRTEM and STXM images we show that structures down to 30 nm are resolved with chemical contrast and record X-ray absorption spectra from endohedral lanthanide ions embedded in individual nanoscale CNT bundles. XMCD measurements of an Er3N@C80 bulk sample and a macroscopic assembly of filled CNTs indicates that the magnetic properties of the endohedral Er3+ ions are unchanged when encapsulated in CNTs. This study demonstrates the feasibility of local magnetic X-ray characterization of low concentrations of lanthanide ions embedded in molecular nanostructures.
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| 10. |
- Kostanyan, Aram, et al.
(författare)
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Gadolinium as an accelerator for reaching thermal equilibrium and its influence on the ground state of Dy2GdN@ C80 single-molecule magnets
- 2021
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Ingår i: Physical Review B. - 2469-9950. ; 103:1
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Tidskriftsartikel (refereegranskat)abstract
- Endohedral fullerenes are perfect nanolaboratories for the study of magnetism. The substitution of a diamagnetic scandium atom in Dy2ScN@C80 with gadolinium decreases the stability of a given magnetization and demonstrates Gd to act as a single atom catalyst that accelerates the reaching of thermal equilibrium. X-ray magnetic circular dichroism at the M4,5 edges of Gd and Dy shows that Gd affects the ground state. The Gd magnetic moment follows the sum of the external and the dipolar magnetic field of the two Dy ions and compared to Dy2ScN@C80 a lower exchange barrier is found between the ferromagnetic and the antiferromagnetic Dy configuration. The Arrhenius equilibration barrier as obtained from superconducting quantum interference device magnetometry is more than one order of magnitude larger, though a much smaller prefactor imposes the faster equilibration in Dy2GdN@C80. This sheds light on the importance of angular momentum balance and symmetry in magnetic relaxation.
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