Ae. Obukhov, The influence of electronically excited triplet states on the photophysical properties of polyatomic heterocyclic azoles as laser active elements, LASER PHYS, 10(5), 2000, pp. 1101-1135
This paper considers series of azoles (organic compounds whose structure in
cludes benzene, furan, thiophene, oxazole, and oxadiazole cycles chemically
coupled with each other) to investigate the dependence of the main lasing
characteristics of these compounds (the wavelength and the threshold pump d
ensity) on the magnitude of pump-induced triplet losses within the fluoresc
ence band. It is shown that only organic compounds with a definite type of
spatial structure satisfy the condition of maximum separation of the band o
f limiting gain (which coincides with the maximum of the fluorescence band)
and the spectra of pump-induced triplet-triplet reabsorption in excited st
ates. The latter condition simultaneously ensures (a) the minimum threshold
pump densities required for lasing, (b) hypsochromic shift of the fluoresc
ence band, (c) the maximum fluorescence quantum yield, and (d) the invarian
ce of the ratio gamma (fl)/tau (fl) const in different solvents. In LCAO MO
CSF CI quantum-chemical models, this phenomenon is attributed to the fact
that only certain compounds of bisoxazoles, oxadizoles, oxazolyls, and oxad
iazolyls in excited fluorescent (and phosphorescent) states allow the exces
sive electron-vibrational excitation to be delocalized exclusively on atoms
and bonds with similar positions and nature. We will consider practical ex
amples showing that, when excitation corresponding to S-1* --> S-0 and T-1
--> S-0 optical transitions and the spectra of pump-induced losses through
S-1* --> S-n* and T-1 --> T-n transitions is localized within the bonds of
the same type, emission spectra overlap with the spectra of induced losses.
This effect gives rise to a strong increase in the threshold pump density.
Optical radiation in the ultraviolet range of wavelengths shorter than lam
bda (max)(GEN) approximate to = 330-320 nm cannot be generated under these
conditions directly (without nonlinear frequency conversion). We will perfo
rm a comparative analysis of the methods for the investigation of lasing bu
ild-up with the use of two-, three-, and five-level models of heteroaromati
c azoles as laser active elements.