Coherence in Multiple Optical Spectroscopy

In this paper we describe a new technique for the generation of multiple pulse phase coherent sequences in optical spectroscopy. The technique is an extension of the acousto‐optic modulation and fluorescence detection methods developed for optical transitions by Zewail and Orlowski (Zewail et al., Chem. Phys. Lett.48, 256 (1977); Orlowski et al., Chem. Phys. Lett.54, 197 (1978)). Application of these multiple pulse trains (of different phases) to optical transitions of two‐level and multilevel systems is demonstrated experimentally. It is shown that they can be used to (i) suppress spontaneous emission background, (ii) enhance coherent transients such as photon echoes, (iii) measure additional relaxation parameters in systems with complex rotational‐vibrational levels, and (iv) enhance the effective laser bandwidths through composite pulse trains, as demonstrated on I2 gas. Finally, the potential of this development is extended to the possibility of observing selective multiquantum excitation in molecules.In this paper we describe a new technique for the generation of multiple pulse phase coherent sequences in optical spectroscopy. The technique is an extension of the acousto‐optic modulation and fluorescence detection methods developed for optical transitions by Zewail and Orlowski (Zewail et al., Chem. Phys. Lett.48, 256 (1977); Orlowski et al., Chem. Phys. Lett.54, 197 (1978)). Application of these multiple pulse trains (of different phases) to optical transitions of two‐level and multilevel systems is demonstrated experimentally. It is shown that they can be used to (i) suppress spontaneous emission background, (ii) enhance coherent transients such as photon echoes, (iii) measure additional relaxation parameters in systems with complex rotational‐vibrational levels, and (iv) enhance the effective laser bandwidths through composite pulse trains, as demonstrated on I2 gas. Finally, the potential of this development is extended to the possibility of observing selective multiquantum excitation in molecules.

Laser ChemistryJan 1, 19837 citations

Coherent nonlinear optical spectroscopy using photon-number squeezed light

Daniel C. Kilper, A. C. Schaefer, John Erland +1 more

Using coherent nonlinear optical spectroscopy below the band edge of a GaAs/ ${\mathrm{Al}}_{0.3}$ ${\mathrm{Ga}}_{1\ensuremath{-}0.3}$As multiple quantum well, photon-number squeezed light generated by a quantum-well laser is used to resolve the exciton resonances and the Urbach tail with detection sensitivity below the semiclassical shot-noise limit. The effect of polarization-dependent noise in the nonclassical probe field is also investigated.Using coherent nonlinear optical spectroscopy below the band edge of a GaAs/${\mathrm{Al}}_{0.3}$${\mathrm{Ga}}_{1\ensuremath{-}0.3}$As multiple quantum well, photon-number squeezed light generated by a quantum-well laser is used to resolve the exciton resonances and the Urbach tail with detection sensitivity below the semiclassical shot-noise limit. The effect of polarization-dependent noise in the nonclassical probe field is also investigated.

Physical Review ASep 1, 199619 citations

Using coherent nonlinear optical spectroscopy below the band edge of a GaAs/

{\mathrm{Al}}_{0.3}

${\mathrm{Ga}}_{1\ensuremath{-}0.3}$As multiple quantum well, photon-number squeezed light generated by a quantum-well laser is used to resolve the exciton resonances and the Urbach tail with detection sensitivity below the semiclassical shot-noise limit. The effect of polarization-dependent noise in the nonclassical probe field is also investigated.