Identifying Charge States of Molecules with Spin-Flip Spectroscopy

Fu, Ying-Shuang; Zhang, Tong; Ji, Shuai‐Hua; Chen, Xi; Ma, Xu-Cun; Jia, Jin‐Feng; Xue, Qi‐Kun

doi:10.1103/physrevlett.103.257202

Cited by 127 publications

(238 citation statements)

References 27 publications

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“…[1][2][3][4][5][6][7][8] It was shown that single adsorbates on metal surfaces with an ultrathin insulator coating can carry a local spin which interacts with the adsorbate surroundings. This interaction leads to a magnetic anisotropy of the local spin, i.e., to the existence of several magnetic energy levels of the adsorbate corresponding to the relative orientation of the local spin with respect to the substrate.…”

Section: Introductionmentioning

confidence: 99%

Excitation of spin waves by tunneling electrons in ferromagnetic and antiferromagnetic spin-12Heisenberg chains

Gauyacq

Lorente

2011

Phys. Rev. B

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Excitation of finite chains of magnetic atoms adsorbed on a surface by tunneling electrons from a scanning tunneling microscope tip is studied using a Heisenberg Hamiltonian description of the magnetic couplings along the chain and a strong coupling approach to inelastic tunneling. The excitation probability of the magnetic levels is very high and the excitation spectra in chains of different lengths are very similar. The excitations in finite chains can be considered as spin waves quantized in the finite object. The energy and momentum spectra of the spin waves excited in the idealized infinite chain by tunneling electrons are determined from the results on the finite chains. Both ferromagnetic and antiferromagnetic couplings are considered, leading to very different results. In particular, in the antiferromagnetic case, excitations linked to the entanglement of the chain ground state are evidenced.

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Section: Introductionmentioning

confidence: 99%

Excitation of spin waves by tunneling electrons in ferromagnetic and antiferromagnetic spin-12Heisenberg chains

Gauyacq

Lorente

2011

Phys. Rev. B

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“…The STM-IETS technique was first applied to the study of vibrational excitations of single molecules on surfaces 1 and has more recently been used to study spin excitations of a single and a few magnetic atoms and molecules deposited on surfaces. [2][3][4][5][6][7][8][9][10][11][12][13] In STM-IETS, electrons tunnel between the tip and the conducting substrate going through the magnetic system. As the bias voltage V is increased, a new conduction channel opens whenever |eV | is larger than the energy of some internal excitation of the atom, which results in a stepwise increase of the differential conductance dI/dV and a peak or dip in the d 2 I/dV 2 .…”

Section: Introductionmentioning

confidence: 99%

Cotunneling theory of atomic spin inelastic electron tunneling spectroscopy

Delgado

Fernández-Rossier

2011

Phys. Rev. B

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We propose cotunneling as the microscopic mechanism that makes possible inelastic electron tunneling spectroscopy of magnetic atoms in surfaces for a wide range of systems, including single magnetic adatoms, molecules, and molecular stacks. We describe electronic transport between the scanning tip and the conducting surface through the magnetic system (MS) with a generalized Anderson model, without making use of effective spin models. Transport and spin dynamics are described with an effective cotunneling Hamiltonian in which the correlations in the magnetic system are calculated exactly and the coupling to the electrodes is included up to second order in the tip MS and MS substrate. In the adequate limit our approach is equivalent to the phenomenological Kondo exchange model that successfully describes the experiments. We apply our method to study in detail inelastic transport in two systems, stacks of cobalt phthalocyanines and a single Mn atom on Cu 2 N. Our method accounts for both the large contribution of the inelastic spin exchange events to the conductance and the observed conductance asymmetry.

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“…[1][2][3][4][5][6][7] Low-temperature STM experimental studies revealed that, in certain cases, a local spin could be associated with individual adsorbates at surfaces. Under the variation in the STM bias, the tip-adsorbate junction exhibits conductance steps at well-defined energies in the few meV energy range.…”

Section: Introductionmentioning

confidence: 99%

“…In this respect, one can mention several spectacular results obtained in this way: evidence of spin coupling between neighboring atomic adsorbates ͑antiferromagnetic coupling along adsorbed Mn chains͒, 2 large magnetic anisotropy of atomic adsorbates ͑Mn and Fe adsorbates on CuN͒, 3 change in magnetic structure of a molecular adsorbate on various substrates ͑Fe-Phthalocyanine on Cu and CuO͒, 4 evidence of superexchange interactions, 5 interaction of molecular adsorbates with magnetic substrates, 6 and charging of adsorbed magnetic nano-objects. 7 Magnetic transitions could be easily evidenced in these systems due to the presence of a coating on the metal substrate that efficiently decouples the adsorbate from the continua of metallic states. When magnetic atoms are directly adsorbed on a metal, magnetic transitions could be observed but much broadened by the interaction with the substrate.…”

Section: Introductionmentioning

confidence: 99%

Magnetic transitions induced by tunneling electrons in individual adsorbedM-phthalocyanine molecules (M=Feand Co)

2010

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We report on a theoretical study of magnetic transitions induced by tunneling electrons in individual adsorbed M-Phthalocyanine ͑M-Pc͒ molecules where M is a metal atom: Fe-Pc on a Cu͑110͒͑2 ϫ 1͒-O surface and Co-Pc layers on Pb͑111͒ islands. The magnetic transitions correspond to the change in orientation of the spin angular momentum of the metal ion with respect to the surroundings and possibly an applied magnetic field. The adsorbed Fe-Pc system is studied with a density-functional-theory-transport approach showing that ͑i͒ the magnetic structure of the Fe atom in the adsorbed Fe-Pc is quite different from that of the free Fe atom or of other adsorbed Fe systems and ͑ii͒ that injection of electrons ͑holes͒ into the Fe atom in the adsorbed Fe-Pc molecule dominantly involves the Fe 3d z 2 orbital. These results fully specify the magnetic structure of the system and the process responsible for magnetic transitions. The dynamics of the magnetic transitions induced by tunneling electrons is treated in a strong-coupling approach. The Fe-Pc treatment is extended to the Co-Pc case. The present calculations accurately reproduce the strength of the magnetic transitions as observed by magnetic inelastic electron tunneling spectroscopy experiments; in particular, the dominance of the inelastic current in the conduction of the adsorbed M-Pc molecule is accounted for.

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Identifying Charge States of Molecules with Spin-Flip Spectroscopy

Cited by 127 publications

References 27 publications

Excitation of spin waves by tunneling electrons in ferromagnetic and antiferromagnetic spin-12Heisenberg chains

Excitation of spin waves by tunneling electrons in ferromagnetic and antiferromagnetic spin-12Heisenberg chains

Cotunneling theory of atomic spin inelastic electron tunneling spectroscopy

Magnetic transitions induced by tunneling electrons in individual adsorbedM-phthalocyanine molecules (M=Feand Co)

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