<i>Ab initio</i>study of a mechanically gated molecule: From weak to strong correlation

Greuling, Andreas; Rohlfing, Michael; Temirov, Ruslan; Tautz, F. Stefan; Anders, Frithjof B.

doi:10.1103/physrevb.84.125413

Cited by 29 publications

(70 citation statements)

References 35 publications

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“…In this direction a number of different ab initio based approaches were suggested. [36][37][38][39][40][41][42][43][44][45][46][47][48][49][50] It should be noted that many-body calculations usually require sophisticated analytical and numerical methods and can be very time consuming. Hence, the methods of transport theory cannot usually be applied directly to large realistic systems; instead a combined approach is preferable where an effective model takes only the states predominantly participating in transport into account.…”

Section: Introductionmentioning

confidence: 99%

“…Progress in this direction recently was achieved in applications to Coulomb blockade phenomena, 37 correlated transport through atomic wires, 38,39 many-body interference, 40 and the Kondo effect. [44][45][46][47][48] Besides, Coulomb blockade phenomena in benzene and benzenedithiol junctions were also considered on the basis of semiempirical atomistic models. [51][52][53] However, a systematic ab initio based many-body theory of molecular transport is still lacking.…”

Section: Introductionmentioning

confidence: 99%

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Many-body localized molecular orbital approach to molecular transport

et al. 2013

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An ab initio based theoretical approach to describe nonequilibrium many-body effects in molecular transport is developed. We introduce a basis of localized molecular orbitals and formulate the many-body model in this basis. In particular, the Hubbard-Anderson Hamiltonian is derived for single-molecule junctions with intermediate coupling to the leads. As an example we consider a benzenedithiol junction with gold electrodes. An effective few-level model is obtained from which spectral and transport properties are computed and are analyzed. Electron-electron interaction crucially affects transport and induces multiscale Coulomb blockade at low biases. At large bias, transport through asymmetrically coupled molecular edge states results in the occurrence of "anomalous" conductance features, i.e., of peaks with unexpectedly large/small height or even not located at the expected resonance energies.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Many-body localized molecular orbital approach to molecular transport

et al. 2013

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“…An upper limit of 2 eV for U can be derived from the change in HOMO-LUMO separation from non-interacting molecules in multilayers to NTCDA at the interface. In addition, for the similar, yet larger, molecule PTCDA U is estimated to about 400 meV if adsorbed on Ag(111) [56]. Following simple size arguments this value can be regarded as a lower limit for U of the smaller NTCDA.…”

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confidence: 98%

Low-energy scale excitations in the spectral function of organic monolayer systems

et al. 2012

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Using high-resolution photoemission spectroscopy we demonstrate that the electronic structure of several organic monolayer systems, in particular 1,4,5,8-naphthalene tetracarboxylic dianhydride and Copper-phtalocyanine on Ag(111), is characterized by a peculiar excitation feature right at the Fermi level. This feature displays a strong temperature dependence and is immediatly connected to the binding energy of the molecular states, determined by the coupling between the molecule and the substrate. At low temperatures, the line-width of this feature, appearing on top of the partly occupied lowest unoccupied molecular orbital of the free molecule, amounts to only ≈ 25 meV, representing an unusually small energy scale for electronic excitations in these systems. We discuss possible origins, related e.g. to many-body excitations in the organic-metal adsorbate system, in particular a generalized Kondo scenario based on the single impurity Anderson model. For more than twenty years there has been a thorough investigation on π-conjugated organic molecules, which have shown to be suitable for the application in organic electronic devices [1][2][3]. These molecules often form long-range ordered films on single-crystalline metal substrates, allowing a systematic and fundamental study by various surface sensitive techniques. In particular from electron spectroscopy methods, as photoemission spectroscopy (PES), inverse photoemission (IPES), and x-ray absorption (XAS), deep insight into many important features of the electronic properties of condensed films and their interfaces has been achieved [4][5][6][7][8]. The latter are of particular importance since they crucially determine the properties of possible devices. Additional microscopic and spectroscopic information has been obtained by use of scanning tunneling microscopy (STM), leading to complementary information about the relation between geometrical and electronic structure [9][10][11][12].Usually, even the spectra of highly ordered films show features with a line-width of several hundreds of meV, mostly determined by vibronic excitations within the adsorbed molecule [7,13,14]. Therefore, even experiments with modern high-resolution photoemission spectrometers for VUV photoemission (UPS) display only features which are about two orders of magnitude larger than the most narrow peaks in other solid state or surface systems [15]. Local spectroscopic measurements by STM, on the other hand, show narrow features in the tunneling conductivity measurements through a single molecule [10,[16][17][18][19], which have been attributed to a possible Kondo like process within the charge transport through * present address: SOLEIL L'Orme des Merisiers, Saint-Aubin -BP 48, 91192 GIF-sur-YVETTE CEDEX FRANCE SOLEIL, Paris, France the adsorbed molecule. However, neither a direct evidence of a local magnetic moment, necessary for the Kondo effect, nor an immediate experimental observation of the spectral function does exist yet.Here we report about a high-resolution photoemission study o...

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“…1) [19]. STM is used for high resolution imaging and location of the functional group at which to dock the tip to the molecule, and FM-AFM is used to measure the junction stiffness dF z =dz [20] while manipulating the molecule off the surface by tip retraction (z ¼ vertical tip coordinate) [21][22][23]. Because the stiffness of the surface-molecule-tip junction is measured throughout the complete removal process, the strength of all interaction potentials constituting the PTCDA-Au(111) bond is probed, albeit in a tangled manner.…”

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Measurement of the Binding Energies of the Organic-Metal Perylene-Teracarboxylic-Dianhydride/Au(111) Bonds by Molecular Manipulation Using an Atomic Force Microscope

et al. 2012

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Based on single molecule manipulation experiments in a combined scanning tunneling microscope/frequency modulated atomic force microscope, we quantify the individual binding energy contributions to an organic-metal bond experimentally. The method allows the determination of contributions from, e.g., local chemical bonds, metal-molecule hybridization, and van der Waals interactions, as well as the total adsorption energy.

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Ab initiostudy of a mechanically gated molecule: From weak to strong correlation

Cited by 29 publications

References 35 publications

Many-body localized molecular orbital approach to molecular transport

Many-body localized molecular orbital approach to molecular transport

Low-energy scale excitations in the spectral function of organic monolayer systems

Measurement of the Binding Energies of the Organic-Metal Perylene-Teracarboxylic-Dianhydride/Au(111) Bonds by Molecular Manipulation Using an Atomic Force Microscope

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