Non-covalent control of spin-state in metal-organic complex by positioning on N-doped graphene

Torre, Bruno de la; Švec, Martin; Hapala, Prokop; Redondo, Jesús; Krejčí, Ondřej; Lo, Rabindranath; Manna, Debashree; Sarmah, Amrit; Nachtigallová, Dana; Tuček, Jiří; Błoński, Piotr; Otyepka, Michal; Zbořil, Radek; Hobza, Pavel; Jelı́nek, Pavel

doi:10.1038/s41467-018-05163-y

Cited by 81 publications

(82 citation statements)

References 56 publications

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“…3 and 4), the AFM image demonstrates the dopant is in the graphitic configuration. STM imaging of graphitic nitrogen in graphene and electron doping were subsequently reported by other groups [53][54][55][56][57][58][59][60][61][62].…”

Section: Stm Imaging and Electronic Doping From Sts Spectramentioning

confidence: 79%

“…This effect has been exploited to perform catalysis, or electrochemical sensing with nitrogen-doped graphene [2,71]. The electronic properties of molecules interacting with nitrogen sites has been investigated with scanning probe microscopy [61,[72][73][74]. STM experiments on free base tetraphenylporphyrin molecules (H 2 TPP) have shown that at nitrogen sites, the molecules undergo a downshift of their highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) states, evidencing a local charge transfer at these sites ( Fig.…”

Section: Molecular Interactionmentioning

confidence: 99%

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Electronic properties of chemically doped graphene

Joucken

Henrard

Lagoute

2019

Phys. Rev. Materials

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Chemical doping of graphene is the most robust way of modifying graphene's electronic properties. We review here the results obtained so far on the electronic structure and transport properties of chemically-doped graphene, focusing on the results obtained with scanning tunneling micropscopy/spectroscopy (STM/S), angle-resolved photoemission spectroscopy (ARPES), and magnetoresistance (MR) measurements. The majority of the results reported have been obtained on nitrogendoped samples, but boron-doped graphene has also been well documented. Besides the appearance of the dopant on STM topographic images, the main questions that have been addressed are the atomic configurations of the doping and their doping efficiency (number of electron/hole brought to the graphene lattice). Both can be addressed by a local probe such as STM/S. The doping efficiency has also been complementary studied via direct visualization of the band structure with ARPES. The effect of the dopants on the electronic transport properties and in particular their influence on the scattering mechanisms is also presented. Finally, avenues for future research efforts are suggested.

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Section: Stm Imaging and Electronic Doping From Sts Spectramentioning

confidence: 79%

Section: Molecular Interactionmentioning

confidence: 99%

Electronic properties of chemically doped graphene

Joucken

Henrard

Lagoute

2019

Phys. Rev. Materials

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“…Recently, STM experiments have shown that molecules adsorbed at nitrogen sites exhibit a different electronic spectrum from those adsorbed on pristine areas, with a shifted or reduced electronic gap. [16][17][18] The effect of an applied electric field on these hybrid systems has however not yet been studied.…”

Section: Introductionmentioning

confidence: 99%

Selective control of molecule charge state on graphene using tip-induced electric field and nitrogen doping

et al. 2019

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The combination of graphene with molecules offers promising opportunities to achieve new functionalities. In these hybrid structures, interfacial charge transfer plays a key role in the electronic properties and thus has to be understood and mastered. Using scanning tunneling microscopy and ab initio density functional theory calculations, we show that combining nitrogen doping of graphene with an electric field allows for a selective control of the charge state in a molecular layer on graphene. On pristine graphene, the local gating applied by the tip induces a shift of the molecular levels of adsorbed molecules and can be used to control their charge state. Ab initio calculations show that under the application of an electric field, the hybrid molecule/graphene system behaves like an electrostatic dipole with opposite charges in the molecule and graphene sub-units that are found to be proportional to the electric field amplitude, which thereby controls the charge transfer. When local gating is combined with nitrogen doping of graphene, the charging voltage of molecules on nitrogen is greatly lowered. Consequently, applying the proper electric field allows one to obtain a molecular layer with a mixed charge state, where a selective reduction is performed on single molecules at nitrogen sites.

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“…This milestone initiated a vigorous development of the technique that now serves a variety of purposes. For example, it can identify molecular structures of natural and pure compounds [2–5], determine the bond order in conjugated systems [6], visualize intramolecular charge distributions [7–9], image three-dimensional molecular structures [10–12], discern complex molecular mixtures [13–14], resolve the intermediate states of chemical reactions [15–19] or discriminate the spin state of single molecules [20].…”

Section: Introductionmentioning

confidence: 99%

Nitrous oxide as an effective AFM tip functionalization: a comparative study

Chutora¹,

Mutombo²,

Hellerstedt³

et al. 2019

Beilstein J. Nanotechnol.

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We investigate the possibility of functionalizing Au tips by N2O molecules deposited on a Au(111) surface and their further use for imaging with submolecular resolution. First, we characterize the adsorption of the N2O species on Au(111) by means of atomic force microscopy with CO-functionalized tips and density functional theory (DFT) simulations. Subsequently we devise a method of attaching a single N2O to a metal tip apex and benchmark its high-resolution imaging and spectroscopic capabilities using FePc molecules. Our results demonstrate the feasibility of high-resolution imaging. However, we find an inherent asymmetry of the N2O probe-particle adsorption on the tip apex, in contrast to a CO tip reference. These findings are consistent with DFT calculations of the N2O- and CO tip apexes.

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Non-covalent control of spin-state in metal-organic complex by positioning on N-doped graphene

Cited by 81 publications

References 56 publications

Electronic properties of chemically doped graphene

Electronic properties of chemically doped graphene

Selective control of molecule charge state on graphene using tip-induced electric field and nitrogen doping

Nitrous oxide as an effective AFM tip functionalization: a comparative study

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