Laser-controlled switching of molecular arrays in an dissipative environment
Abstract
The optical switching of molecular ensembles in a dissipative environment is a subject of various fields of chemical physics and physical chemistry. Here we try to switch arrays of molecules from a stable collective ground state to a state in which all molecules have been transferred to another stable higher-energy configuration. In our model switching proceeds through electronically excited intermediates which are coherently coupled to each other through dipolar interactions, and which decay incoherently within a finite lifetime by coupling to a dissipative environment. The model is quite general, but parameters are chosen to roughly resemble the all-trans → all-cis isomerization of an array of azobenzene molecules on a surface. Using analytical and optimal control pulses and the concept of “laser distillation,” we demonstrate that for various aggregates (dimers up to hexamers), controlled and complete switching should be possible.
- Publication:
-
Physical Review B
- Pub Date:
- March 2011
- DOI:
- 10.1103/PhysRevB.83.104301
- Bibcode:
- 2011PhRvB..83j4301F
- Keywords:
-
- 82.20.Rp;
- 31.70.Hq;
- 33.80.-b;
- State to state energy transfer;
- Time-dependent phenomena: excitation and relaxation processes and reaction rates;
- Photon interactions with molecules