In a previous paper, we have already considered the system composed by a two level atom interacting with a coherent external electromagnetic field. No application whatsoever has been made of the rotating wave approximation. Being specially interested in the problem of higher harmonic generations for the case of very intense laser fields, we have developed in this letter a much more efficient way to obtain these solutions as well as to carry out some calculations in a range in which the parameters take extreme values. Also the formalism allows us now to provide analytic expressions in the WKB regime for the electric dipole moment and the population inversion. The spectrum can be decomposed in periodic and non-periodic contributions. Only the latter depends upon the Floquet exponent and can be responsible of the main complexities of the observed Rabi revivals and the hyper-Raman shift.
In a previous paper, we have already considered the system composed by a two level atom interacting with a coherent external electromagnetic field. No application whatsoever has been made of the rotating wave approximation. Being specially interested in the problem of higher harmonic generations for the case of very intense laser fields, we have developed in this letter a much more efficient way to obtain these solutions as well as to carry out some calculations in a range in which the parameters take extreme values. Also the formalism allows us now to provide analytic expressions in the WKB regime for the electric dipole moment and the population inversion. The spectrum can be decomposed in periodic and non-periodic contributions. Only the latter depends upon the Floquet exponent and can be responsible of the main complexities of the observed Rabi revivals and the hyper-Raman shift.
The spectral and dynamic effects associated with a non-zero difference, d, between the permanent dipole moments of two molecular states involved in a transition, are investigated for a variety of electromagnetic field-molecule interactions. Both analytical and exact numerical techniques are used to solve the time-dependent Schrodinger equation and to obtain the temporal populations of the molecular states and the associated absorption spectra, for molecular interactions with a Gaussian pulsed, or one or two continuous wave (CW), laser(s).;Analytical rotating wave approximation results are derived for a single CW laser interacting with a two-level d {dollar}\\ne{dollar} 0 molecule with an excited state lifetime, and for a two-level d {dollar}\\ne{dollar} 0 molecule interacting with two CW lasers. A symmetry-adapted Riemann product integral method for exact calculations of pulsed laser-molecule interactions is developed and applied to specific problems. The Floquet technique for the treatment of periodic Hamiltonians is extended to accommodate the interaction of a molecule with two CW lasers.;The one-field RWA results are used to predict and interpret the effects of permanent dipoles on the temporal behaviour of the molecular states for a decaying two-level system interacting with a CW laser, and for a non-decaying two-level system interacting with a pulsed laser. It is shown that the excited state lifetime and the pulse duration can act as internal and external probes, respectively, of the temporal effects of permanent dipoles, relative to the often-studied d = 0 problem. The two-field analytical RWA solutions are used to help discuss and predict the effects of permanent dipole moments in two-laser multi-photon transitions. Several examples of multi-photon, two-colour, two-level resonance profiles, calculated in the RWA and by using exact Floquet techniques, are used to demonstrate how particular multi-photon transitions can be optimized, and to help quantify the conditions for the validity of the two-colour RWA. The effects of neighbouring energy levels on the transition of interest, for both probe and pump-probe laser-molecule interactions, are investigated using a series of three- to seven-level model molecular systems.
The problem of a two-level atom interacting with a non-monochromatic radiation pulse is studied in the resonant approximation for arbitrary detunings, and without the resonant approximation. By using the time-dependent theory of perturbation the analytical expressions for the transition probability and induced dipole moment of the atom are obtained. It is shown that the upper level population of the atom exhibits oscillations that are absent in the resonant approximation. The temporal shape of the pulse is shown to affect significantly the atomic transition probability. The behaviour of the transition probability and dipole moment spectrum for arbitrary pulse shapes, phases and detunings is investigated. The interference between the spectral components arising in nonlinear processes is shown to play a considerable role in the formation of a dipole moment spectrum.
We consider here the exact solution of a nonrelativistic quantum system composed of a two-level atom interacting with a laser with arbitrary large frequency and intensity. We use the analogy of this system and a ℏ/2-spin particle interacting with a time-dependent magnetic field. A systematic use of the dynamical symmetry underlying the physical system is made. Actually the Hamiltonian is a Hermitian element of the SU(2) Lie Algebra. The exact Temporal Evolution Operator in terms of a Generalized Displacement Operator of the group is constructed. It is possible to develop a nonperturbative method that allows us to solve exactly the model for any value of the relevant frequencies (Rabi, Laser, and Atom Frequencies) and in so doing the usual Rotating Wave and Small Interaction approximations are unnecessary. The properties of periodicity of this model and the phenomenon of harmonic generation are considered by using Floquet Analysis. We find that in addition to the so far well-known spectrum composed by odd harmonics, this model generates another type of noninteger harmonics whose frequencies and amplitudes are determined for any value of the relevant parameters of the system.
The interaction is studied of a Gaussian pulsed or a continuous wave (CW) electric field with a molecule that has a nonzero difference d between the permanent dipoles of the ground and excited states involved in a transition. The unusual spectral effects associated with the transition with d ≠ 0, relative to the often studied case with d = 0, have been investigated previously in the two-level approximation and for continuous wave lasers. The observation of these effects, including markedly increased periods of excited state populations and negative Bloch-Siegart shifts, will often require the intense fields associated with pulsed rather than purely continuous wave electric fields. Transitions induced by continuous wave and pulsed laser-‘permanent dipole molecule’ interactions, for high field intensities and varying pulse durations, are investigated with model calculations carried out using exact Floquet and symmetry-adapted Riemann product integral methods. These calculations illustrate how the increased period of the excited state populations for dipolar molecules, and the associated molecule-field couplings, can be probed by sampling the time-dependent populations of the excited states using ultrashort to short pulses. The discussion illustrates the predictive and interpretive importance of the analytical expression for the molecule-EMF coupling provided by the rotating wave approximation (RWA) with d ≠ 0. The examples considered show, for example, temporal beating effects between the field and the RWA or Rabi frequencies and their dependence on d.
The wave function of a two-level atom driven by a low-frequency laser pulse is obtained in analytical form and is used to determine the power spectrum of the dipole moment of the atom for different initial atomic states. The solution goes over some known approximate solutions and gives the energy of the two dressed states, the position of the hyper-Raman lines, the amplitudes both of the hyper-Raman lines and of the odd harmonics, and the position of the cutoff. The form of the hyper-Raman spectrum results independently of the initial atomic state and shows an onset and a cutoff of the emission.
The interaction of two continuous wave electric fields (lasers) with a two-level molecule, that has a nonzero difference d, between the permanent dipoles of the two states involved in a multiphoton two-color transition, is studied in the rotating wave approximation and by using exact methods. Analytical rotating wave approximation results for the time-dependent populations of the molecular states and for the resonance profiles are derived and used to help discuss the effects of permanent dipole moments in the two-color absorption problem. Several examples of multiphoton, two-color, two-level resonance profiles calculated in the rotating wave approximation and by using exact techniques, are employed for illustrative purposes. They are used to help quantify the conditions for the validity of the two-color rotating wave approximation, which are considerably more restrictive than the analogous conditions for the one-color rotating wave approximation with d≠0, and to illustrate the interpretive and predictive nature of the rotating wave approximation results. For example, there are many multiphoton, two-color transitions that are available if a molecule possesses permanent dipoles (d≠0). The analytic rotating wave approximation expression for the molecule-two laser coupling can often be used to reliably estimate the field parameters of the two lasers that are required to optimize a given transition relative to others.