Contributions of the substrate electric field to the molecular adsorbate optical nonlinearities
- Groupe Polymeres, Photonique et Optoelectronique, Faculte des Sciences de Bizerte, 7021 Zarzouna (Tunisia)
The nonlinear optical response of an adsorbate, whose structure is altered by the inhomogeneous electrostatic field of the substrate, has been evaluated with a particular emphasis on the sum-frequency generation process. In the limiting case of an homogeneous electrostatic field, besides the contributions associated with the induced dipole moments, we have additional contributions which only exist if the adsorbed molecule has permanent dipole moments. Also, the Franck-Condon factors of the unperturbed molecule weight the internal couplings induced by the electrostatic field. For the more general inhomogeneous electrostatic field case, while the main observations remain valid, the Franck-Condon factors are modified by the molecular structure changes induced by the electrostatic field. In addition, we have a strong redistribution of the vibronic couplings resulting from the analytical Q dependence of the partial charge distribution which is a signature of the field inhomogeneities.
- OSTI ID:
- 20718802
- Journal Information:
- Physical Review. A, Vol. 72, Issue 4; Other Information: DOI: 10.1103/PhysRevA.72.043810; (c) 2005 The American Physical Society; Country of input: International Atomic Energy Agency (IAEA); ISSN 1050-2947
- Country of Publication:
- United States
- Language:
- English
Similar Records
High-resolution photoelectron imaging and resonant photoelectron spectroscopy via noncovalently bound excited states of cryogenically cooled anions
Vibronic coupling in energy transfer dynamics and two-dimensional electronic–vibrational spectra