Laser intensity induced nonradiative processes in molecules

Journal Article · Thu Aug 20 04:00:00 EDT 1981 · J. Phys. Chem.; (United States)

DOI:https://doi.org/10.1021/j150617a025· OSTI ID:6040961

Needham, C; Rhodes, W

The effects of the coupling strength (i.e., the Rabi frequency) of a coherent radiation mode interacting with a multilevel molecule are considered. A doorway-state basis is used in which the radiative doorway state, carrying all of the radiative interaction strength from the ground (initial) state, is coupled by intramolecular (nonradiative) interaction to other excited states. The resulting coupling scheme involves an effective Hamiltonian formulation in an extended rotating basis. Quantitative results from the theory are obtained by computer simulation. It is shown how variation of the laser coupling strength can modify the dynamics of nonradiative transitions, thereby producing: (1) decoupling of radiationless decay; (2) enhancement of radiationless decay; (3) selectivity of photophysical and photochemical processes; or (4) laser-induced isolation of states, depending on the conditions of the system. The case of two states coupled through a common manifold of states and the conditions for biexponential decay are also considered.

• Research Organization: Florida State Univ., Tallahassee
• DOE Contract Number: AS05-78EV05784
• OSTI ID: 6040961
• Journal Information: J. Phys. Chem.; (United States), Journal Name: J. Phys. Chem.; (United States) Vol. 85:17; ISSN JPCHA
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
400201* -- Chemical & Physicochemical Properties
COUPLING
DE-EXCITATION
ELECTROMAGNETIC RADIATION
ENERGY LEVELS
ENERGY TRANSFER
ENERGY-LEVEL TRANSITIONS
EXCITED STATES
FUNCTIONS
HAMILTONIAN FUNCTION
LASER RADIATION
MOLECULES
RADIATIONLESS DECAY
RADIATIONS