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 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.

Jan 1, 19910 citations

Multiphoton Spectroscopy

P. Bräunlich

Springer eBooksJan 1, 19790 citations

Electromagnetic radiation emanating from the molecular nanomagnet Fe 8

Oren Shafir, Amit Keren

Photons emitted by transition between the discrete levels of single molecular magnets might obey the elementary condition for Dicke's super-radiance. We investigate this possibility in the ${\text{Fe}}_{8}$ molecule where magnetization jumps are known to occur at discrete magnetic-field values. We found energy bursts each time the molecule undergoes a magnetization jump, confirming their quantum nature. A series of tests indicated that photons carry out the energy and that indeed these photons obey the elementary conditions for super-radiance.Photons emitted by transition between the discrete levels of single molecular magnets might obey the elementary condition for Dicke's super-radiance. We investigate this possibility in the ${\text{Fe}}_{8}$ molecule where magnetization jumps are known to occur at discrete magnetic-field values. We found energy bursts each time the molecule undergoes a magnetization jump, confirming their quantum nature. A series of tests indicated that photons carry out the energy and that indeed these photons obey the elementary conditions for super-radiance.

arXiv:0902.2540Physical Review BMay 11, 20098 citations

Photons emitted by transition between the discrete levels of single molecular magnets might obey the elementary condition for Dicke's super-radiance. We investigate this possibility in the

{\text{Fe}}_{8}

molecule where magnetization jumps are known to occur at discrete magnetic-field values. We found energy bursts each time the molecule undergoes a magnetization jump, confirming their quantum nature. A series of tests indicated that photons carry out the energy and that indeed these photons obey the elementary conditions for super-radiance.