Efficient Spin-Flip Excitation of a Nickelocene Molecule

Ormaza, Maider; Bachellier, Nicolas; Faraggi, Marisa N.; Verlhac, Benjamin; Abufager, Paula; Ohresser, P.; Joly, L.; Roméo, M.; Scheurer, F.; Bocquet, Marie‐Laure; Lorente, Nicolás; Limot, L.

doi:10.1021/acs.nanolett.6b05204

Cited by 65 publications

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“…Given the similarity to the spin excitation spectrum measured above nickelocene [dashed line in Fig. 2(a)], which is known from previous studies [19,27], we assign 1 to a spin excitation. To confirm this assignment, we carried out spin-polarized DFT calculations (Supplemental Sec.…”

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confidence: 74%

“…1(d); noted Nc hereafter] coupled to a Ni atom. Nickelocene is a spin S = 1 molecule of the metallocene family with magnetic anisotropy, where spin excitations produce a sizable increase of the electronic transport [19]. We show that the on-surface assembly of a nickel-nickelocene complex (NiNc, hereafter) on Cu(100) can promote a sizable vibrational mode.…”

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confidence: 92%

“…For this purpose, we engineered the NiNc complex outside the network via a tip-assisted manipulation [35]. To do so, we first transferred an isolated Nc to the tip [19,27] and then transferred it back atop an isolated Ni adatom on the surface [Figs. 4(a) and 4(b)].…”

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confidence: 99%

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Vibron-assisted spin excitation in a magnetically anisotropic molecule

et al. 2020

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The ability to electrically-drive spin excitations in molecules with magnetic anisotropy is key for high-density storage and quantum-information technology. Electrons, however, also tunnel via the vibrational excitations unique to a molecule. The interplay of spin and vibrational excitations offers novel routes to study and, ultimately, electrically manipulate molecular magnetism. Here we use a scanning tunneling microscope to electrically induce spin and vibrational excitations in a single molecule consisting of a nickelocene magnetically coupled to a Ni atom. We evidence a vibron-assisted spin excitation at an energy one order of magnitude higher compared to the usual spin excitations of nickelocene and explain it using first-principles calculations that include electron correlations. Furthermore, we observe that spin excitations can be quenched by modifying the Ni-nickelocene coupling. Our study suggests that nickelocene-based complexes constitute a model playground for exploring the interaction of spin and vibrations in the electron transport through single magnetic molecules.Magnetic molecules are potential candidates for information-storing technology [1], molecular spintronics [2] and quantum computing [3], provided that their axial magnetic anisotropy DS 2 z ensures a magnetic bistability among longlived magnetic states. But molecules also vibrate. In particular, in magnetic molecules the interplay of vibrational modes, or vibrons, with the spin degrees of freedom is known to impact the spin lifetime [4][5][6]. Since vibrational modes can couple to the electric charge, producing vibron-assisted electron excitations in transport [7][8][9], expectations are that similar effects should be also observed with the electronic spin [10,11].Concerning this last point, experimental work has predominantly focused on a well-known spin-related manybody effect, the Kondo effect. The electron-vibron interaction in Kondo molecules was shown to produce satellite Kondo resonances in the differential conductance spectra at the bias of the vibron's excitation energy [12][13][14]. These resonances were ascribed to tunneling electrons that have their spin flipped when elastically scattering off the molecular spin, but with sufficient energy to activate a vibrational mode in the molecule [15]. The question arises whether a similar mechanism is also possible with other spin scattering mechanisms that magnetically excite a molecule such as inelastic scattering involving magnetic anisotropy [16]. These so-called spin excitations show great potential in view of an all-electrical manipulation of the molecular spin [17,18].Here, we use scanning tunneling microscopy (STM) to demonstrate the presence of a combined vibrational-spin excitation in a single nickelocene molecule [Ni(C 5 H 5 ) 2 , see Fig. 1(d); noted Nc hereafter] coupled to a Ni atom. Nickelocene is a spin S = 1 molecule of the metallocene family with magnetic anisotropy, where spin excitations produce a sizable increase of the electronic transport [19]. We show that the o...

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Vibron-assisted spin excitation in a magnetically anisotropic molecule

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“…In general, compared to low-temperature transport across wellcharacterized quantum objects (e.g. from single atoms and dimers to molecules and atomic clusters [43][44][45][46][47][48][49] ) thanks to a scanning tunneling microscope (STM), it is thus far difficult to assemble and ascertain the effective nanotransport path 50 in a solid state device, especially for the oxides used as MTJ barriers. Here, uncontrolled imperfections such as oxygen vacancies in the MgO tunnel barrier can concentrate electronic tunneling transport across a macrojunction onto a nanotransport path 50,51 , such that the device operates due to a rare tunneling event 52 .…”

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Spin-driven electrical power generation at room temperature

et al. 2019

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Ongoing research is exploring novel energy concepts ranging from classical to quantum thermodynamics. Ferromagnets carry substantial built-in energy due to ordered electron spins. Here, we propose to generate electrical power at room temperature by utilizing this magnetic energy to harvest thermal fluctuations on paramagnetic centers using spintronics. Our spin engine rectifies current fluctuations across the paramagnetic centers' spin states by utilizing so-called 'spinterfaces' with high spin polarization. Analytical and ab-initio theories suggest that experimental data at room temperature from a single MgO magnetic tunnel junction (MTJ) be linked to this spin engine. Device downscaling, other spintronic solutions to select a transport spin channel, and dual oxide/organic materials tracks to introduce paramagnetic centers into the tunnel barrier, widen opportunities for routine device reproduction. At present MgO MTJ densities in next-generation memories, this spin engine could lead to 'always-on' areal power densities that are highly competitive relative to other energy harvesting strategies.

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“…We use here a tip decorated by a spin S = 1 nickelocene molecule ( Fig. 1a) [26,27], which comprises a Ni atom sandwiched between two C 5 H 5 cyclopentadienyl rings, and accurately capture the junction geometry through the comparison to first-principles calculations.…”

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Atomic-scale spin sensing with a single molecule at the apex of a scanning tunneling microscope

Verlhac

Bachellier

Garnier

et al. 2019

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Recent advances in scanning probe techniques rely on the chemical functionalization of the probe-tip termination by a single molecule. The success of this approach opens the tantalizing prospect of introducing spin sensitivity through the functionalization by a magnetic molecule. Here, we use a nickelocene-terminated tip (Nc-tip), which offers the possibility of producing spin excitations on the tip apex of a scanning tunneling microscope (STM). We show that when the Nc-tip is a hundred pm away from point contact with a surface-supported object, magnetic effects may be probed through changes in the spin excitation spectrum of nickelocene. We use this detection scheme to simultaneously determine the exchange field and the spin polarization of the sample with atomic-scale resolution. Our findings demonstrate that the Nc-tip is a powerful probe for investigating surface magnetism with STM, from single magnetic atoms to surfaces.

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Efficient Spin-Flip Excitation of a Nickelocene Molecule

Cited by 65 publications

References 47 publications

Vibron-assisted spin excitation in a magnetically anisotropic molecule

Vibron-assisted spin excitation in a magnetically anisotropic molecule

Spin-driven electrical power generation at room temperature

Atomic-scale spin sensing with a single molecule at the apex of a scanning tunneling microscope

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