ABSTRACT
Magnetic clusters on an insulating substrate are potential candidates for spin-based quantum devices. Here we investigate the geometric, electronic, and magnetic structures of small Ti and Cr clusters, from dimers to pentamers, adsorbed on a single-layer hexagonal boron nitride (h-BN) sheet within the framework of density functional theory. The stable adsorption configurations of the Ti clusters and Cr clusters composed of the same number of atoms are found to be totally different from each other. The difference in their bonding mechanisms has been revealed by the density of states and the charge density difference of the corresponding adsorption systems. While chemical bonds are formed between the Ti atoms and the supporting sheet, the Cr clusters are found in the physisorption state on the substrate. In addition, it is shown that the h-BN sheet is energetically favorable for building three-dimensional Ti clusters. These findings support the use of h-BN as a suitable decoupling substrate for manipulation of quantum spin states in small transition metal (TM) clusters and fabrication of devices based on them.
ABSTRACT
A controlled chemical reaction on a specific bond in a single molecule is an inevitable step toward atomic engineering and fabrication. Here, we explored the debromination of a single 9,10-dibromoanthracene (DBA) molecule on a surface as stimulated by the voltage pulse through the tip of a scanning tunneling microscope (STM). A voltage threshold of about 2.2 V is obtained, and the nature of single-electron process is revealed. The spatially resolved debromination yield is obtained as a function of the pulse magnitude, which presents strong asymmetry for the two C-Br bonds. The optimal stimulation parameters including the pulse magnitude and the tip locations are suggested. The distinct dynamics in dissociation of the two bonds are illustrated by their energy diagrams and recoil paths, as derived by the first-principles density functional theory (DFT) calculation. The influence of the local electric field due to the STM tip on the dissociation of the C-Br bond has also been discussed. The study presents detailed practice for the controlled debromination in a single DBA molecule, which may lead to automated atomic engineering and fabrication of artificial nanostructures in the future.
ABSTRACT
We investigate the orientation switching of individual azobenzene molecules adsorbed on a Au(111) surface using a laser-assisted scanning tunneling microscope (STM). It is found that the rotational motion of the molecule can be regulated by both sample bias and laser wavelength. By measuring the switching rate and state occupation as a function of both bias voltage and photon energy, the threshold in sample bias and the minimal photon energy are derived. It has been revealed that the tip-induced local electrostatic potential remarkably contributes to the reduction in hopping barrier. We also find that the tunneling electrons and photons play distinct roles in controlling rotational dynamics of single azobenzene molecules on the surface, which are useful for understanding dynamic behaviors in similar molecular systems.
ABSTRACT
Two low-energy excitations of a single water molecule are observed via inelastic electron tunneling spectroscopy, where a significant enhancement is achieved by attaching the molecule to the tip apex in a scanning tunneling microscope. Density functional theory simulations and quantum mechanical calculations of an asymmetric top are carried out to reveal the origin of both excitations. Variations in tunneling junction separation give rise to the quantum confinement effect on the quantum state of a water molecule in the tunneling junction. Our results demonstrate a potential method for measuring the dynamic behavior of a single molecule confined in a tunneling junction, where the molecule-substrate interaction can be purposely tuned.
