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1.
Nano Lett ; 24(1): 180-186, 2024 Jan 10.
Article in English | MEDLINE | ID: mdl-38150551

ABSTRACT

We investigated the Kondo effect of cobalt(II)-5-15-bis(4'-bromophenyl)-10,20-bis(4'-iodophenyl)porphyrin (CoTPPBr2I2) molecules on Au(111) with low-temperature scanning tunneling microscopy under ultrahigh vacuum conditions. The molecules exhibit four adsorption configurations at the top and bridge sites of the surface with different molecular orientations. The Kondo resonance shows extraordinary sensitivity to the adsorption configuration. By switching the molecule between different configurations, the Kondo temperature is varied over a wide range from ≈8 up to ≈250 K. Density functional theory calculations reveal that changes of the adsorption configuration lead to distinct variations of the hybridization between the molecule and the surface. Furthermore, we show that surface reconstruction plays a significant role for the molecular Kondo effect.

2.
Nano Lett ; 23(19): 8988-8994, 2023 Oct 11.
Article in English | MEDLINE | ID: mdl-37782684

ABSTRACT

Harnessing the spin of single atoms is at the heart of quantum information nanotechnology based on magnetic concepts. By attaching single Co atoms to monatomic Cu chains, we demonstrate the ability to control the spin orientation by the atomic environment. Due to spin-orbit coupling (SOC), the spin is tilted by ≈58° from the surface normal toward the chain as evidenced by inelastic tunneling spectroscopy. These findings are reproduced by density functional theory calculations and have implications for Co atoms on pristine Cu(111), which are believed to be Kondo systems. Our quantum Monte Carlo calculations suggest that SOC suppresses the Kondo effect of Co atoms at chains and on the flat surface. Our work impacts the fundamental understanding of low-energy excitations in nanostructures on surfaces and demonstrates the ability to manipulate atomic-scale magnetic moments, which can have tremendous implications for quantum devices.

3.
Phys Rev Lett ; 129(11): 116801, 2022 Sep 09.
Article in English | MEDLINE | ID: mdl-36154405

ABSTRACT

Molecular vibrational spectroscopy with the scanning tunneling microscope is feasible but usually detects few vibrational modes. We harness sharp Yu-Shiba-Rusinov states observed from molecules on a superconductor to significantly enhance the vibrational signal. From a lead phthalocyanine molecule 46 vibrational peaks are resolved enabling a comparison with calculated modes. The energy resolution is improved beyond the thermal broadening limit and shifts induced by neighbor molecules or the position of the microscope tip are determined. Vice versa, spectra of vibrational modes are used to measure the effect of an electrical field on the energy of Yu-Shiba-Rusinov states. The method may help to further probe the interaction of molecules with their environment and to better understand selection rules for vibrational excitations.

4.
Phys Chem Chem Phys ; 24(47): 28864-28869, 2022 Dec 07.
Article in English | MEDLINE | ID: mdl-36437692

ABSTRACT

Sub-monolayer amounts of trioxatriangulenium (TOTA) molecules functionalized with biphenyl on Ag(111) were investigated with scanning tunnelling microscopy. The molecule is comprised of a rod-shaped axial ligand and a triangular platform that tends to form hydrogen bonds in arrays. Two superstructures are observed, a hexagonal tiling and a phase of molecular double rows. While the former structure matches previous observations from other functionalized TOTA molecules the latter one was unexpected. Aided by density functional theory results, we analyse the observed intramolecular contrast and present a model of the new phase. We discuss possible interaction mechanisms underlying the molecular pattern.

5.
Phys Rev Lett ; 116(2): 027201, 2016 Jan 15.
Article in English | MEDLINE | ID: mdl-26824562

ABSTRACT

All-trans-retinoic acid (ReA), a closed-shell organic molecule comprising only C, H, and O atoms, is investigated on a Au(111) substrate using scanning tunneling microscopy and spectroscopy. In dense arrays single ReA molecules are switched to a number of states, three of which carry a localized spin as evidenced by conductance spectroscopy in high magnetic fields. The spin of a single molecule may be reversibly switched on and off without affecting its neighbors. We suggest that ReA on Au is readily converted to a radical by the abstraction of an electron.

6.
Phys Rev Lett ; 114(1): 016602, 2015 Jan 09.
Article in English | MEDLINE | ID: mdl-25615489

ABSTRACT

Single atoms on Au(111) surfaces have been contacted with the Au tip of a low temperature scanning tunneling microscope. The shot noise of the current through these contacts has been measured up to frequencies of 120 kHz and Fano factors have been determined to characterize the transport channels. The noise at Fe and Co atoms, the latter displaying a Kondo effect, indicates spin-polarized transport through a single channel. Transport calculations reproduce this observation.

7.
Phys Rev Lett ; 115(1): 016802, 2015 Jul 03.
Article in English | MEDLINE | ID: mdl-26182113

ABSTRACT

A Mn-porphyrin was contacted on Au(111) in a low-temperature scanning tunneling microscope (STM). Differential conductance spectra show a zero-bias resonance that is due to an underscreened Kondo effect according to many-body calculations. When the Mn center is contacted by the STM tip, the spectrum appears to invert along the voltage axis. A drastic change in the electrostatic potential of the molecule involving a small geometric relaxation is found to cause this observation.

8.
Phys Rev Lett ; 110(22): 226101, 2013 May 31.
Article in English | MEDLINE | ID: mdl-23767734

ABSTRACT

Single donors close to the ZnO(0001) surface are investigated with scanning tunneling microscopy. Their binding energies and depths are determined from spatially resolved spectra of the differential conductance. At elevated bias of the STM tip, vertical motion of the donors can be induced. The direction of the motion can be controlled by the bias polarity.

9.
ACS Nano ; 17(2): 1268-1274, 2023 Jan 24.
Article in English | MEDLINE | ID: mdl-36440841

ABSTRACT

Spin-flip excitations of iron porphyrin molecules on Au(111) are investigated with a low-temperature scanning tunneling microscope. The molecules adopt two distinct adsorption configurations on the surface that exhibit different magnetic anisotropy energies. Density functional theory calculations show that the different structures and excitation energies reflect unlike occupations of the Fe 3d levels. We demonstrate that the magnetic anisotropy energy can be controlled by changing the adsorption site, the orientation, or the tip-molecule distance.

10.
ACS Nano ; 17(11): 10608-10616, 2023 Jun 13.
Article in English | MEDLINE | ID: mdl-37224165

ABSTRACT

The magnetic properties of transition-metal ions are generally described by the atomic spins of the ions and their exchange coupling. The orbital moment, usually largely quenched due the ligand field, is then seen as a perturbation. In such a scheme, S = 1/2 ions are predicted to be isotropic. We investigate a Co(II) complex with two antiferromagnetically coupled 1/2 spins on Au(111) using low-temperature scanning tunneling microscopy, X-ray magnetic circular dichroism, and density functional theory. We find that each of the Co ions has an orbital moment comparable to that of the spin, leading to magnetic anisotropy, with the spins preferentially oriented along the Co-Co axis. The orbital moment and the associated magnetic anisotropy is tuned by varying the electronic coupling of the molecule to the substrate and the microscope tip. These findings show the need to consider the orbital moment even in systems with strong ligand fields. As a consequence, the description of S = 1/2 ions becomes strongly modified, which have important consequences for these prototypical systems for quantum operations.

11.
ACS Nano ; 16(10): 16987-16995, 2022 Oct 25.
Article in English | MEDLINE | ID: mdl-36153959

ABSTRACT

Large ordered islands of aluminum phthalocyanine (AlPc) molecules, which are unstable in air, are synthesized from ClAlPc on Pb(100) via dechlorination. Low-temperature scanning tunneling microscopy reveals that isolated AlPc molecules lose their spin moment on superconducting Pb(100). Molecular magnetism, which is detected via Yu-Shiba-Rusinov (YSR) resonances, may be restored by surrounding a molecule with an array of neighbor molecules in artificial arrays or in a self-assembled monolayer. Unlike phthalocyanine (H2Pc) or lead phthalocyanine (PbPc) monolayers, where the YSR energy was found to depend strongly on the detailed configuration of the neighboring molecules, we find a similar magnetic moment on every second molecule for AlPc. In addition, YSR resonances lead to unusually high conductance peaks that are due to vibrational excitations. Twelve vibrational modes are resolved and discussed with respect to similar results from PbPc. The enhancement of the inelastic transitions is tentatively attributed to the large amplitude of the YSR resonances and the long lifetime of electrons in the molecular bound state. By assembling neighboring molecules into configurations that differ from those of the monolayer, the YSR energy may be fine-tuned, and a simple spin-state switching device is constructed.

12.
ACS Nano ; 14(12): 17387-17395, 2020 Dec 22.
Article in English | MEDLINE | ID: mdl-33225694

ABSTRACT

Diamagnetic H2 phthalocyanine molecules are probed on superconducting Pb(100) using a low-temperature scanning tunneling micoscope (STM). In supramolecular arrays made with the STM, the molecules acquire a spin as detected via the emergence of Yu-Shiba-Rusinov resonances. The spin moments vary among the molecules and are determined by the electrostatic field that results from polar bonds in the surrounding Pc molecules. The moments are further finely tuned by repositioning the hydrogen atoms of the inner macrocycle of the surrounding molecules.

13.
Nat Nanotechnol ; 15(1): 18-21, 2020 Jan.
Article in English | MEDLINE | ID: mdl-31873288

ABSTRACT

Molecular spin switches are attractive candidates for controlling the spin polarization developing at the interface between molecules and magnetic metal surfaces1,2, which is relevant for molecular spintronics devices3-5. However, so far, intrinsic spin switches such as spin-crossover complexes have suffered from fragmentation or loss of functionality following adsorption on metal surfaces, with rare exceptions6-9. Robust metal-organic platforms, on the other hand, rely on external axial ligands to induce spin switching10-14. Here we integrate a spin switching functionality into robust complexes, relying on the mechanical movement of an axial ligand strapped to the porphyrin ring. Reversible interlocked switching of spin and coordination, induced by electron injection, is demonstrated on Ag(111) for this class of compounds. The stability of the two spin and coordination states of the molecules exceeds days at 4 K. The potential applications of this switching concept go beyond the spin functionality, and may turn out to be useful for controlling the catalytic activity of surfaces15.

14.
J Phys Condens Matter ; 30(42): 424001, 2018 Oct 24.
Article in English | MEDLINE | ID: mdl-30191885

ABSTRACT

In the scanning tunnelling microscope, the many-body Kondo effect leads to a zero-bias feature of the differential conductance spectra of magnetic adsorbates on surfaces. The intrinsic line shape of this Kondo resonance and its temperature dependence in principle contain valuable information. We use measurements on a molecular Kondo system, all- trans retinoic acid on Au(1 1 1), and model calculations to discuss the role of instrumental broadening. The modulation voltage used for the lock-in detection, noise on the sample voltage, and the temperature of the microscope tip are considered. These sources of broadening affect the apparent line shapes and render difficult a determination of the intrinsic line width, in particular when variable temperatures are involved.

15.
Beilstein J Nanotechnol ; 9: 3048-3052, 2018.
Article in English | MEDLINE | ID: mdl-30643703

ABSTRACT

Spatially resolved measurements of the apparent tunneling barrier height Φapp in scanning tunneling microscopy have been used to estimate variations of the local work function Φ of surface structures. We experimentally show that Φapp can fail as a measure of Φ. The discrepancies are attributed to a kinetic-energy contribution to Φapp. This contribution depends on the lateral extent of the tunneling current filament and, consequently, on the local surface structure.

16.
Chem Commun (Camb) ; 54(66): 9135-9138, 2018 Aug 14.
Article in English | MEDLINE | ID: mdl-30059079

ABSTRACT

Tuning the spin-dependent electron transport through molecules is of fundamental importance in single-molecule spintronics. Here, the transport properties of iron phthalocyanine on Au(111) was investigated by a combination of scanning tunneling microscopy and density functional theory calculations. Using high-resolution scanning tunneling spectroscopy performed at 0.5 K, a Kondo resonance was observed on FePc. After removing its eight outermost hydrogen atoms, the spectroscopic feature changed into a double-step structure, which reflected inelastic transitions of molecular spin states. The density functional theory calculations revealed that the coupling between Fe and Au(111) became much weaker after cutting the hydrogen atoms. This explained the change of the spin-related fingerprints in the differential spectra.

17.
Nat Commun ; 5: 2992, 2014.
Article in English | MEDLINE | ID: mdl-24390611

ABSTRACT

In devices like the single-electron transistor the detailed transport properties of a nanostructure can be measured by tuning its energy levels with a gate voltage. The scanning tunnelling microscope in contrast usually lacks such a gate electrode. Here we demonstrate tuning of the levels of a donor in a scanning tunnelling microscope without a third electrode. The potential and the position of the tip are used to locally control band bending. Conductance maps in this parameter space reveal Coulomb diamonds known from three-terminal data from single-electron transistors and provide information on charging transitions, binding energies and vibrational excitations. The analogy to single-electron transistor data suggests a new way of extracting these key quantities without making any assumptions about the unknown shape of the scanning tunnelling microscope tip.

18.
Science ; 323(5918): 1190-3, 2009 Feb 27.
Article in English | MEDLINE | ID: mdl-19251623

ABSTRACT

The Fermi surface that characterizes the electronic band structure of crystalline solids can be difficult to image experimentally in a way that reveals local variations. We show that Fermi surfaces can be imaged in real space with a low-temperature scanning tunneling microscope when subsurface point scatterers are present: in this case, cobalt impurities under a copper surface. Even the very simple Fermi surface of copper causes strongly anisotropic propagation characteristics of bulk electrons that are confined in beamlike paths on the nanoscale. The induced charge density oscillations on the nearby surface can be used for mapping buried defects and interfaces and some of their properties.

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