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Jerzy Leszczynski

Publications and source records attributed to Jerzy Leszczynski.

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Investigating charge transfer dynamics at the nanoscale

Acquiring quantitative information on charge transfer (CT) dynamics at the nanoscale remains an important scientific challenge. In particular, CT processes in single molecules at surfaces needs to be investigated to be properly controlled in various devices. To address this issue, the dynamics of switching molecules can be exploited. Here, a Nickel-tetraphenylporphyrin adsorbed on the Si(100) surface is used to study the CT process ruling the reversible activation of two chiral molecular conformations. Via the electrons of a scanning tunneling microscope (STM), a statistical study of the molecular switching reveals two specific locations of the molecule for which their efficiency is optimized. The CT mechanism is shown to propagate from two lateral aryls groups towards the porphyrin macrocycle inducing an intramolecular movement of two symmetric pyrroles. The measured switching efficiencies can thus be related with a Markus-Jordner model to estimate relevant parameters that describe the dynamics of the CT process. Numerical simulations provide a precise description of the molecular conformations and unveil the molecular energy levels that are involved in the CT process. This quantitative method opens a completely original approach to study CT at the nanoscale.

cond-mat.mes-hall

Non-adiabatic molecular Hamiltonian: Canonical transformation coupling electronic and vibrational motions

The coupling of electronic and vibrational motion is studied by two canonical transformations namely normal coordinate transformation and momentum transformation on molecular Hamiltonian. It is shown that by these transformations we can pass from crude approximation to adiabatic approximation and then to non-adiabatic (diabatic) Hamiltonian. This leads to renormalized fermions and renormalized diabatic phonons. Simple calculations on $H_{2}$, $HD$, and $D_{2}$ systems are performed and compared with previous approaches. Problem of electronic quasi-degeneracy is discussed.

physics.chem-ph