Action spectroscopy for single-molecule reactions – Experiments and theory

Kim, Y.; Motobayashi, Kenta; Frederiksen, Thomas; Ueba, H.; Kawai, Maki

doi:10.1016/j.progsurf.2014.12.001

Cited by 98 publications

(96 citation statements)

References 142 publications

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“…Table 2.1 summarizes STM-induced molecular processes reported in the past. These experiments clearly show STM capability to investigate molecular dynamics on conductive surfaces at the single-molecule level (see also recent reviews [82][83][84][85]). We have employed low-temperature STM to directly image and control H-bond dynamics [86,87].…”

Section: Direct Observation and Control Of Molecular Processes Using mentioning

confidence: 68%

Direct observation and control of hydrogen-bond dynamics using low-temperature scanning tunneling microscopy

Kumagai

2015

Progress in Surface Science

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Section: Direct Observation and Control Of Molecular Processes Using mentioning

confidence: 68%

Direct observation and control of hydrogen-bond dynamics using low-temperature scanning tunneling microscopy

Kumagai

2015

Progress in Surface Science

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“…The vibrational excitation of adsorbate on metal surfaces is one of the fundamental processes in various surface dynamic phenomena [1][2][3]. Action spectroscopy with a scanning tunneling microscope (STM-AS) [4,5] has been widely used to investigate vibration-mediated molecular dynamic behavior on solid surfaces, such as hopping, rotation, desorption, and chemical reaction, at the singlemolecule level. In the STM-AS, the vibrational modes leading to molecular motions and reactions can be detected as the dynamic responses to the excitation energy of inelastically tunneled electrons from the STM tip.…”

mentioning

confidence: 99%

Lateral Hopping of CO on Ag(110) by Multiple Overtone Excitation

Lim

Arafune

et al. 2016

Phys. Rev. Lett.

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A novel type of action spectrum representing multiple overtone excitations of the vðM-CÞ mode was observed for lateral hopping of a CO molecule on Ag(110) induced by inelastically tunneled electrons from the tip of a scanning tunneling microscope. The yield of CO hopping shows sharp increases at 261 AE 4 mV, corresponding to the C-O internal stretching mode, and at 61 AE 2, 90 AE 2, and 148 AE 7 mV, even in the absence of corresponding fundamental vibrational modes. The mechanism of lateral CO hopping on Ag (110) was explained by the multistep excitation of overtone modes of vðM-CÞ based on the numerical fitting of the action spectra, the nonlinear dependence of the hopping rate on the tunneling current, and the hopping barrier obtained from thermal diffusion experiments.

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“…36 In order to further ascertain the suitability of the asymmetric Cu-H 2 -Cu junction model, we have studied its dynamical properties. At variance with the gas phase in which only a stretching mode exists, the H 2 molecule in the asymmetric Cu-H 2 -Cu junction has four types of vibration modes: the longitudinal stretching mode (ST), the longitudinal translation mode (TZ) with the center of mass of the H 2 molecule vibrating along the transport direction, the two transverse rotation modes (RX, RY) in which the angle between the H-H bond and the transport direction vibrates, and the two transverse translation modes (TX, TY) in which the center of mass of the H 2 molecule vibrates along the transverse directions.…”

Section: Resultsmentioning

confidence: 99%

Effects of the molecule-electrode interface on the low-bias conductance of Cu–H2–Cu single-molecule junctions

Jiang

Wang

Shen

et al. 2016

The Journal of Chemical Physics

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The atomic structure and electronic transport properties of a single hydrogen molecule connected to both symmetric and asymmetric Cu electrodes are investigated by using the non-equilibrium Green's function formalism combined with the density functional theory. Our calculations show that in symmetric Cu-H 2 -Cu junctions, the low-bias conductance drops rapidly upon stretching, while asymmetric ones present a low-bias conductance spanning the 0.2-0.3 G 0 interval for a wide range of electrode separations. This is in good agreement with experiments on Cu atomic contacts in a hydrogen environment. Furthermore, the distribution of the calculated vibrational energies of the two hydrogen atoms in the asymmetric Cu-H 2 -Cu junction is also consistent with experiments. These findings provide clear evidence for the formation of asymmetric Cu-H 2 -Cu molecular junctions in breaking Cu atomic contacts in the presence of hydrogen and are also helpful for the design of molecular devices with Cu electrodes. Published by AIP Publishing. [http://dx

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Action spectroscopy for single-molecule reactions – Experiments and theory

Cited by 98 publications

References 142 publications

Direct observation and control of hydrogen-bond dynamics using low-temperature scanning tunneling microscopy

Direct observation and control of hydrogen-bond dynamics using low-temperature scanning tunneling microscopy

Lateral Hopping of CO on Ag(110) by Multiple Overtone Excitation

Effects of the molecule-electrode interface on the low-bias conductance of Cu–H2–Cu single-molecule junctions

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