The proposal to use entropy as a metric for optimization of image processing has been subjected to further critical examination, on the basis of experiments with contrast adjustment, HDR imaging, bimodal brightness distributions, and unsharp masking. Consequently our original expectation that entropy may be a directly useful response metric for optimizing image processing now appears to us to be naïve and limited in its applicability. One purpose of the present investigation is to ascertain the nature of these limits. We also infer from the unsharp masking studies that the human visual system (HVS) has evolved not so much to maximize information captured from the visual field as to enhance compressibility and to effect image simplification.
The purpose of this work is to suggest a way to utilize image statistics to guide optimization of brightness distributions,
towards a goal of complete systematization of image processing to achieve a purely aesthetic objective, with entropy as a
response metric. We start with a survey of classic pictorial photographs, proceed to a heuristic theoretical treatment of
the brightness distribution function, and follow with several pictorial illustrations of the proposed concept.
We report preparation of silver nanoparticles in the 10 nm size range by exhastive reduction of a well-known and well-characterized AgBr nanosol. These silver nanoparticles exhibit a second order hyperpolarizability tensor, β=(100±10) x 10-30 esu per atom. The nanoparticles chmisorb a monolayer of iodide ions with concomitant bleaching of the surface plasmon absorption but no attenuation of Hyper-Rayleigh (second harmonic light) Scattering (HRS). Further addition of iodide leads to significant enhancement of HRS, which we attribute so surface-enhanced second harmonic scattering (SESHS) from iodide ion physisorbed on the AgI adlayer. A merocyanine dye, which does not exhibit HRS in solution, chemisorbs as a monolayer to the nanosilver, with formation of J-aggregates. These aggregates, like the free dye, are not active in second harmonic scattering. Further addition of dye leads to HRS enhancement, which we interpret as physisorption of dye onto the J-aggregate monolayer; the non-centrosymmetric surface environment allows observation of SESHS. A lower-limit estimate of the second order hyperpolarizability of the adsorbed dye is 200 X 10-30 esu per molecule.
We have observed fluorescence from Coumarin 334 in solution using light of twice an actinic wavelength for excitation. The effect is demonstrated to be biphotonic, but is observed at optical powers below those required for resonant biphotonic excitation, and with an incoherent source. We infer operation of HRS. By extrapolation we propose that this effect should contribute to fluorescence under usual conditions for multiphoton fluorescence microscopy, and that it might be exploited in fluorescence microscopy under conditions where usual mechanisms are inapplicable.
An unusual slow rise of fluorescence intensity from Coumarins 102, 314, and 334, observed under conditions of high intensity laser excitation prompted further investigation of their photophysics by photoquenching, time-resolved transient absorption spectroscopy and time- resolved amplified stimulated emission. The slow rise was found to be the consequence of multi-photon excitation. Principal fate of coumarin molecules so excited was shown to be intersystem crossing to the nonemissive triplet manifold. Rate of intersystem crossing was estimated as ca. 1010 s-1; energy matching between a higher excited singlet state, Sn, and a higher triplet, Tn, is implicated.
The photophysics of 1,3,5-triphenyl-2-pyrazoline (I) and 1,3-diphenyl-5-(p-nitrophenyl)-2- pyrazoline (II) have been probed using steady-state and time-resolved fluorescence spectroscopy, laser flash transient absorption spectroscopy, and photochemical observations. II (and to a lesser extent, I) undergoes efficient H-D exchange at the 5-position on the pyrazoline ring when irradiated at 365 nm in CD3OD. These observations are interpreted in terms of initial photoexcitation to S2, which partitions between S1 and a non-emissive intramolecular charge-transfer state. This viewpoint helps rationalise some of the differences between solution and solid state photophysics of the pyrazolines.
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