A polarized laser beam can bleach narrow, long-lived, anisotropic holes in the 607-nm zero-phonon line of the NaF ${N}_{1}$ center. The width of these holes is twice the homogeneous linewidth, and three orders of magnitude less than the inhomogeneous width of the line. We report a polarization-spectroscopy technique which detects the dichroism and birefringence of the hole with better sensitivity than absorption spectroscopy. A simple rateequation model is developed to account for hole burning, but the recovery of the initial isotropic absorption profile appears to be a complex, slow, and intractable process.A polarized laser beam can bleach narrow, long-lived, anisotropic holes in the 607-nm zero-phonon line of the NaF ${N}_{1}$ center. The width of these holes is twice the homogeneous linewidth, and three orders of magnitude less than the inhomogeneous width of the line. We report a polarization-spectroscopy technique which detects the dichroism and birefringence of the hole with better sensitivity than absorption spectroscopy. A simple rateequation model is developed to account for hole burning, but the recovery of the initial isotropic absorption profile appears to be a complex, slow, and intractable process.

Physical review. B, Condensed matterNov 15, 198036 citations

Zero-phonon selective spectroscopy: where do we stand now?

Karl K. Rebane

Journal of LuminescenceApr 1, 20006 citations

High-resolution spectroscopy of the zero-phonon line of the deep donor EL2 in GaAs

Christoph Hecht, R. Kummer, M. Thoms +1 more

We investigated the zero-phonon line (ZPL) of the deep donor EL2 in GaAs by means of high-resolution absorption spectroscopy with a narrow-band laser. Frequency-selective bleaching (``spectral-hole burning'') experiments and the measurement of the temperature broadening of the ZPL prove an essentially homogeneous broadening of the transition. The observed asymmetry of the line shape is interpreted to be caused by a Fano resonance of the $^{1}\mathrm{T}_{2}$ excited state with the conduction band. A splitting of the $^{1}\mathrm{T}_{2}$ state as the reason for the asymmetry seems unrealistic. The homogeneous broadening of the ZPL prevents the use of spectral-hole burning spectroscopy to study the effect of external perturbations on the ZPL of the EL2.We investigated the zero-phonon line (ZPL) of the deep donor EL2 in GaAs by means of high-resolution absorption spectroscopy with a narrow-band laser. Frequency-selective bleaching (``spectral-hole burning'') experiments and the measurement of the temperature broadening of the ZPL prove an essentially homogeneous broadening of the transition. The observed asymmetry of the line shape is interpreted to be caused by a Fano resonance of the $^{1}\mathrm{T}_{2}$ excited state with the conduction band. A splitting of the $^{1}\mathrm{T}_{2}$ state as the reason for the asymmetry seems unrealistic. The homogeneous broadening of the ZPL prevents the use of spectral-hole burning spectroscopy to study the effect of external perturbations on the ZPL of the EL2.

Physical review. B, Condensed matterMay 15, 19974 citations

Long-Lived Electronic Coherence of Iodine in the Condensed Phase: Sharp Zero-Phonon Lines in the B↔X Absorption and Emission of I2 in Solid Xe

Eero Hulkko, Johan Lindgren, Toni Kiljunen +1 more

Our study of B←X absorption of molecular iodine (I2) isolated in a low-temperature crystalline xenon has revealed an exceptionally long-lived electronic coherence in condensed phase conditions. The visible absorption spectrum shows prominent vibronic structure in the form of zero-phonon lines (ZPLs) and phonon side bands (PSBs). The resolved spectrum implies weak interaction of the chromophore to the lattice degrees of freedom. The coherence extends past the vibrational period of the excited state molecule, unlike that observed in any condensed phase environment for I2 so far. The ZP transitions from the relaxing B-state populations were resolved in the hot luminescence when the 532 nm laser was used for excitation.Our study of B←X absorption of molecular iodine (I2) isolated in a low-temperature crystalline xenon has revealed an exceptionally long-lived electronic coherence in condensed phase conditions. The visible absorption spectrum shows prominent vibronic structure in the form of zero-phonon lines (ZPLs) and phonon side bands (PSBs). The resolved spectrum implies weak interaction of the chromophore to the lattice degrees of freedom. The coherence extends past the vibrational period of the excited state molecule, unlike that observed in any condensed phase environment for I2 so far. The ZP transitions from the relaxing B-state populations were resolved in the hot luminescence when the 532 nm laser was used for excitation.

The Journal of Physical Chemistry LettersJun 20, 20121 citation

A polarized laser beam can bleach narrow, long-lived, anisotropic holes in the 607-nm zero-phonon line of the NaF

{N}_{1}

center. The width of these holes is twice the homogeneous linewidth, and three orders of magnitude less than the inhomogeneous width of the line. We report a polarization-spectroscopy technique which detects the dichroism and birefringence of the hole with better sensitivity than absorption spectroscopy. A simple rateequation model is developed to account for hole burning, but the recovery of the initial isotropic absorption profile appears to be a complex, slow, and intractable process.

^{1}\mathrm{T}_{2}

excited state with the conduction band. A splitting of the

^{1}\mathrm{T}_{2}

state as the reason for the asymmetry seems unrealistic. The homogeneous broadening of the ZPL prevents the use of spectral-hole burning spectroscopy to study the effect of external perturbations on the ZPL of the EL2.