On the validity of the quasiresonant approximation for molecular infrared-multiphoton excitation

Abstract

Articles you may be interested inTimeresolved infraredspectroscopic observation of relaxation and reaction processes during and after infraredmultiphoton excitation of 12CF3I and 13CF3I with shaped nanosecond pulsesThe rotating wave approximation, including the incorporation and importance of diagonal dipole moment matrix elements, for infrared multiphoton excitations Infraredmultiphoton excitation and wave packet motion of the harmonic and anharmonic oscillators: Exact solutions and quasiresonant approximation

Theoretical study of the IR excitation of the ClNO molecule in a multimode laser field

“…This approximation is particularly well adapted when the molecular hamiltonian Hmo I is diagonal in the molecular basis set {IM(i))} or with very small coupling terms. It has been shown [16,17] to be a quasi-exact formulation for laser intensities up to 100 GW/cm 2. The extension of QRA to a multi-mode formulation has been given by Whaley and Light [18]: for a field with p modes, the approximation will consists in keeping In the above criterion A~o R is a parameter which must be varied until convergence, typical values of which are given in the next section.…”

Electron-flux infrared response to varying π-bond topology in charged aromatic monomers

“…Although the multiple-photon excitation relies on the anharmonic character of IVR coupled modes, which could induce noticeable nonlinear effects37, there are examples such as the naphthyl + action spectrum3839 confirming the quasi-resonant harmonic description of adiabatic molecular potentials probed by multiple-photon action spectroscopy3740. Here, the bands observed in the action spectra are summarized in Table 1 with their spectral deconvolutions and harmonic mode assignments (from Supplementary Tables 7–16) based on the B3LYP vibrational analysis of Fig.…”

Theoretical Methods for Ultrafast Spectroscopy

“…The QRA has been implemented and used in many different applications, ranging from the far-infrared to the UV spectral range within the URIMIR program package (for unimolecular reactions induced by multi-photon infrared radiation). [56] Its validity and accuracy has been verified several times, in particular for the simulation of multi-photon excitation processes [48,57,58] .…”