J. Catalan et al., INTERRING TORSIONAL MODULATION IN MOLECULAR LASERS - ULTRAVIOLET LASING VIA AMPLIFIED SPONTANEOUS EMISSION-SPECTROSCOPY OF PHENYLIMIDAZOLES, The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory, 101(29), 1997, pp. 5284-5291
The intramolecularly torsion-capable molecules 2-phenylimidazole (I),
2-phenylbenzimidazole (II), 1-methyl-2-phenylimidazole (III), and 1-me
thyl-2-phenylbenzimidazole (IV) are shown to yield efficient UV lasing
action. The amplified spontaneous emission (ASE) laser spikes wavelen
gths (and gain coefficients) are for I, 321 nm (alpha = 7 cm(-1)); for
II, 341 Mn (alpha = 10.5 cm(-1)); for III, 324 nm (alpha = 8 cm(-1));
and for IV, 345.5 nm (alpha = 9 cm(-1)) (ASE cell optical length of 0
.8 cm). The laser spikes represent for each molecule the normal simple
case of wavelength coincidence with the fluorescence maximum. Theoret
ical calculations are presented to correlate electronic structural cha
nges with observed spectra and for theoretical torsional potential fun
ctions. In cases I and II, the torsional mode is active only in the ex
cited-state S-1, and serves merely to modulate by a large shift (simil
ar to 3000 cm(-1)) the ASE laser spike position, driven by stretching
mode vibronic excitation. In the cases of III and IV, the torsional mo
de is interpreted to be the driving mode, with an ASE laser spike Delt
a nu of 5000 cm(-1) or more (measured as the Franck-Condon shift of la
mbda(max) from absorption to fluorescence, and the ASE laser spike pos
ition), deduced from the theoretically calculated torsional potentials
offering a four-level population inversion system.