S. Arnold et al., FLUORESCENCE MICROSCOPY AND SPECTROSCOPY OF AN ISOLATED MICRO-DROPLET, Materials science & engineering. B, Solid-state materials for advanced technology, 48(1-2), 1997, pp. 139-146
Fluorescence microscopy and spectroscopy experiments are carried out o
n individual microdroplets (mu-drops) isolated within an electrodynami
c levitator-trap (Paul type) at atmospheric pressure. Imaging experime
nts on spatially homogeneous donor and acceptor dyes within particles
of radius a similar to 10 mu m reveal a 'global' transfer mechanism wi
th a yield exceeding conventional dipole-dipole transfer (Forster tran
sfer) by similar to 1000 x between molecules at a particular radial di
stance r > 0.93 (S. Arnold, S. Holler, S.D. Druger, J. Chem. Phys. 104
(1996) 7741), but is consistent with the quantum theory of enhanced e
nergy transfer through morphology dependent resonances (MDRs) of the s
phere (P.T. Leung, K. Young, J. Chem. Phys. 89 (1988) 2894). To gain a
better understanding for the primary step in this process, we investi
gate fluorescence from a particle with a dilute layer of surface activ
e molecules. These surfactant molecules have a fixed orientation relat
ive to the surface as revealed both qualitatively from a heuristic int
erpretation of polarization analyzed images (S. Arnold, L.M. Folan, Pr
oc. SPIE 1862 (1993) 218), and quantitatively through the preferential
cavity enhanced selection of various polarized modes in emission spec
troscopy. The spectra are adequately described through semi-classical
theory (S.D. Druger, S. Arnold, L.M. Folan, J. Chem. Phys. 87 (1987) 2
649). This theory has also been applied to the description of reported
'anomalous' fluorescence lifetime measurements (M.D. Barnes, C.-Y. Ku
ng, W.B. Whitten, J.M. Ramsey, S. Arnold, S. Holler, Phys. Rev. Lett.
76 (1996) 3931) from a dilute surface layer. Although sum rules based
on density of states of high Q whispering gallery modes fail to descri
be the data at particle sizes for which the homogeneous linewidth is l
arger than the free spectral range (M.D. Barnes, C.-Y. Kung, W.B. Whit
ten, J.M. Ramsey, S. Arnold, S. Holler, Phys. Rev. Lett. 76 (1996) 393
1), semi-classical theory, including all modes, is in considerably bet
ter agreement with the data. (C) 1997 Elsevier Science S.A.