A general theoretical description is derived for the resonance fluorescence of dilute gases and molecular single crystals with special emphasis on optical rotation spectra. The validity of previous theoretical work on dilute gases is confirmed by proving that the damping constants connecting excited states on different molecules are zero. It is shown that the intensities of optical rotation spectra of molecular crystals are much larger than the corresponding quantities for gases. An important theoretical prediction is that the natural line breadth of a resonance fluorescence emission band belonging to an exciton state in a molecular crystal should be larger than the width of the corresponding optical absorption line. The dependence of the intensity of the optical rotation spectrum on the relative orientation of the crystal with respect to the incident beam of light is discussed.A general theoretical description is derived for the resonance fluorescence of dilute gases and molecular single crystals with special emphasis on optical rotation spectra. The validity of previous theoretical work on dilute gases is confirmed by proving that the damping constants connecting excited states on different molecules are zero. It is shown that the intensities of optical rotation spectra of molecular crystals are much larger than the corresponding quantities for gases. An important theoretical prediction is that the natural line breadth of a resonance fluorescence emission band belonging to an exciton state in a molecular crystal should be larger than the width of the corresponding optical absorption line. The dependence of the intensity of the optical rotation spectrum on the relative orientation of the crystal with respect to the incident beam of light is discussed.

The Journal of Chemical PhysicsMay 1, 196314 citations

Reply to ‘Comment on “Discrepancies in the resonance-fluorescence spectrum calculated with two methods” ’

Qing Yang Xu, Xiangming Hu, Jian-wu Yin

Physical Review AMay 11, 20090 citations

Resonance fluorescence revisited

Haakil Lee, Tin-Lun Ho, Marlan O. Scully

Brazilian Journal of PhysicsJan 1, 19951 citation

Investigations of Resonance Fluorescence.

Harry J. Kimble

May 1, 19780 citations

Comment on “Resonance-fluorescence and absorption spectra of a two-level atom driven by a strong bichromatic field”

David L. Aronstein, Ryan S. Bennink, Robert W. Boyd +1 more

We identify discrepancies between two published predictions of the resonance fluorescence from a two-level atom driven by a strong bichromatic field [J. Opt. Soc. Am. B $8,$ 1163 (1991) and Phys. Rev. A $48,$ 3092 (1993)]. These discrepancies are shown to arise from subtleties in extracting the time-averaged resonance fluorescence from the expansions used to solve the optical Bloch equations. We construct a solution to these equations that corrects the results of the latter reference and reconciles the two predictions.We identify discrepancies between two published predictions of the resonance fluorescence from a two-level atom driven by a strong bichromatic field [J. Opt. Soc. Am. B $8,$ 1163 (1991) and Phys. Rev. A $48,$ 3092 (1993)]. These discrepancies are shown to arise from subtleties in extracting the time-averaged resonance fluorescence from the expansions used to solve the optical Bloch equations. We construct a solution to these equations that corrects the results of the latter reference and reconciles the two predictions.

Physical Review AJun 17, 200222 citations

We identify discrepancies between two published predictions of the resonance fluorescence from a two-level atom driven by a strong bichromatic field [J. Opt. Soc. Am. B

8,

1163 (1991) and Phys. Rev. A

48,

3092 (1993)]. These discrepancies are shown to arise from subtleties in extracting the time-averaged resonance fluorescence from the expansions used to solve the optical Bloch equations. We construct a solution to these equations that corrects the results of the latter reference and reconciles the two predictions.