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On-surface synthesis and collective spin excitations of a triangulene-based nanostar

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 Added by Nacho Pascual
 Publication date 2021
  fields Physics
and research's language is English




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Triangulene nanographenes are open-shell molecules with predicted high spin state due to the frustration of their conjugated network. Their long-sought synthesis became recently possible over a metal surface. Here, we present a macrocycle formed by six [3]triangulenes, which was obtained by combining the solution synthesis of a dimethylphenyl-anthracene cyclic hexamer and the on-surface cyclodehydrogenation of this precursor over a gold substrate. The resulting triangulene nanostar exhibits a collective spin state generated by the interaction of its 12 unpaired {pi}-electrons along the conjugated lattice, corresponding to the antiferromagnetic ordering of six S = 1 sites (one per triangulene unit). Inelastic electron tunneling spectroscopy resolved three spin excitations connecting the singlet ground state with triplet states. The nanostar behaves close to predictions from the Heisenberg model of a S = 1 spin ring, representing a unique system to test collective spin modes in cyclic systems.



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Triangular zigzag nanographenes, such as triangulene and its pi-extended homologues, have received widespread attention as organic nanomagnets for molecular spintronics, and may serve as building blocks for high-spin networks with long-range magnetic order - of immense fundamental and technological relevance. As a first step toward these lines, we present the on-surface synthesis and a proof-of-principle experimental study of magnetism in covalently bonded triangulene dimers. On-surface reactions of rationally-designed precursor molecules on Au(111) lead to the selective formation of triangulene dimers in which the triangulene units are either directly connected through their minority sublattice atoms, or are separated via a 1,4-phenylene spacer. The chemical structures of the dimers have been characterized by bond-resolved scanning tunneling microscopy. Scanning tunneling spectroscopy and inelastic electron tunneling spectroscopy measurements reveal collective singlet-triplet spin excitations in the dimers, demonstrating efficient inter-triangulene magnetic coupling.
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We propose a pump-probe set-up to analyse the properties of the collective excitation spectrum of a spinor polariton fluid. By using a linear response approximation scheme, we carry on a complete classification of all excitation spectra, as well as their intrinsic degree of polarisation, in terms of two experimentally tunable parameters only, the mean-field polarisation angle and a rescaled pump detuning. We evaluate the system response to the external probe, and show that the transmitted light can undergo a spin rotation along the dispersion for spectra that we classify as diffusive-like. We show that in this case, the spin flip predicted along the dispersion is enhanced when the system is close to a parametrically amplified instability.
A theory of collective states in a magnetically quantized two-dimensional electron gas (2DEG) with half-filled Landau level (quantized Hall ferromagnet) in the presence of magnetic 3d impurities is developed. The spectrum of bound and delocalized spin-excitons as well as the renormalization of Zeeman splitting of the impurity 3d levels due to the indirect exchange interaction with the 2DEG are studied for the specific case of n-type GaAs doped with Mn where the Lande` g-factors of impurity and 2DEG have opposite signs. If the sign of the 2DEG g-factor is changed due to external influences, then impurity related transitions to new ground state phases, presenting various spin-flip and skyrmion-like textures, are possible. Conditions for existence of these phases are discussed. PACS: 73.43.Lp, 73.21.Fg, 72.15.Rn
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