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PubMed2002

Comparison of the molecular mass and optical properties of colored dissolved organic material in two rivers and coastal waters by flow field-flow fractionation.

Colored dissolved organic material (CDOM) is an important sunlight absorbing substance affecting the optical properties of natural waters. However, little is known about its structural and optical properties mainly due to its complex matrix and the limitation of the techniques available. A comparison of two southwestern Florida rivers [the Caloosahatchee River (CR) and the Shark River (SR)] was done in terms of molecular mass (MM) and diffusion coefficients (D). The novel technique Frit inlet/frit outlet-flow field-flow fractionation (FIFO-FIFFF) with absorbance and fluorescence detectors was used to determine these properties. The SR receives organic material from the Everglades. By contrast, the CR arises from Lake Okeechobee in central Florida, receiving anthropogenic inputs, farming runoff, and natural organics. Both rivers discharge to the Gulf of Mexico. Fluorescence identified, for both rivers, two different MM distributions in low salinity water samples: the first was centered at approximately 1.7 kDa (CR) and approximately 2 kDa (SR); the second centered at approximately 13 kDa for both rivers, which disappeared gradually in the river plumes to below detection limit in coastal waters. Absorbance detected only one MM distribution centered at approximately 2 kDa (CR) and 2.2-2.4 kDa (SR). Fluorescence in general peaked at a lower MM than absorbance, suggesting a different size distribution for fluorophores vs chromophores. A photochemical study showed that, after sunlight, irradiated freshwater samples have similar characteristics to more marine waters, including a shift in MM distribution of chromophores. The differences observed between the rivers in the optical characteristics, MM distributions, and D values suggest that the CDOM sources, physical, and photochemical degradation processes are different for these two rivers.

Adsorption↗
PubMed2003

Photochemical alkylation of inorganic selenium in the presence of low molecular weight organic acids.

Using a flow-through photochemical reactor and a low pressure mercury lamp as a UV source, alkyl selenium species are formed from inorganic selenium(IV) in the presence of low molecular weight organic acids (LMW acids). The volatile alkyl Se species were cryogenically trapped and identified by GC-MS and GC-ICP-MS. In the presence of formic, acetic, propionic and malonic acids, inorganic selenium(IV) is converted by UV irradiation to volatile selenium hydride and carbonyl, dimethylselenide and diethylselenide, respectively. Se(IV) was successfully removed from contaminated agricultural drainage waters (California, U.S.A.) using a batch photoreactor system Se. Photochemical alkylation may thus offer a promising means of converting toxic selenium salts, present in contaminated water, to less toxic dimethylselenide. The LMW acids and photochemical alkylation process may also be key to understanding the source of atmospheric selenium and are likely involved in its mobility in the natural anaerobic environment.

Acids↗
PubMed2002

Epitaxial growth and photochemical annealing of graded CdS/ZnS shells on colloidal CdSe nanorods.

We report the preparation and structural characterization of core/shell CdSe/CdS/ZnS nanorods. A graded shell of larger band gap is grown around CdSe rods using trioctylphosphine oxide as a surfactant. Interfacial segregation is used to preferentially deposit CdS near the core, providing relaxation of the strain at the core/shell interface. The reported synthesis allows for variation of the shell thickness between one and six monolayers, on core nanorods ranging from aspect ratios of 2:1 to 10:1. After an irreversible photochemical annealing process, the core/shell nanorods have increased quantum efficiencies and are stable in air under visible or UV excitation. In addition to their robust optical properties, these samples provide an opportunity for the study of the evolution of epitaxial strain as the shape of the core varies from nearly spherical to nearly cylindrical.

Journal Article↗
PubMed2026

Photocatalytic Golgi Proteomics Reveals Palmitoylation-Regulated Golgiphagy.

The Golgi apparatus (GA) orchestrates protein modification, trafficking, and secretion through highly dynamic remodeling, yet its proteomic complexity remains difficult to resolve in living systems. Here, we report CAT-Golgi, a genetically independent and light-controlled photocatalytic proximity labeling strategy for in situ spatiotemporal mapping of the Golgi-associated proteome. Combining a cysteine-conjugated eosin photocatalyst (GolgiCat) with an aniline probe, CAT-Golgi enables rapid and precise protein labeling within minutes under mild green light, requiring no genetic manipulation and operating efficiently in hard-to-transfect and primary cells. Leveraging our extensive efforts in organelle-targeted photocatalytic systems, we extended this chemistry to the highly dynamic and reversible Golgi apparatus. CAT-Golgi achieved quantitative and comparative proteomics in HeLa, K562, Jurkat and primary HEKa cells, revealing both conserved and cell-type-specific profiles. Under Brefeldin A-induced Golgiphagy, CAT-Golgi captured large-scale proteome remodeling and identified palmitoyl-protein thioesterase 1 (PPT1) as a potential regulatory component. PPT1 downregulation enhanced ULK1 and TRPML1 palmitoylation, disrupted redox balance, and activated Golgiphagy. CAT-Golgi provides a broadly applicable chemical platform for decoding organelle dynamics, offering both conceptual and technical foundations for extending photocatalytic proteomics to other transient organelles and illuminating molecular mechanisms of organelle plasticity and disease progression.

Golgi Apparatus↗
PubMed2006

Hybrid junctions of zinc(II) and magnesium(II) phthalocyanine with wide-band-gap semiconductor nano-oxides: spectroscopic and photoelectrochemical characterization.

The optical properties of zinc phthalocyanine (ZnIIPc) and magnesium phthalocyanine (MgIIPc) in DMSO and DMF solutions have been extensively investigated, and the photoelectrochemical behaviors of layer-by-layer hybrid junctions formed of the two metallo(II) phthalocyanines (MIIPcs) and wide-band-gap colloidal semiconductors, namely, ZnO and TiO2 nanocrystals (NCs), have been probed. Different experimental conditions, such as the Pc center metal ion, dye concentration, and solvent identity, were investigated in order to elucidate their effects on the photoelectrochemical performances of the prepared heterojunctions. Finally, thermal treatment of either dye and NC films and control of the NC shape and surface chemistry were also studied and, interestingly, were found to be critical in affecting the performance of photochemical sensitization processes, occurring at the dye/oxide and oxide/solution interfaces.

Journal Article↗
PubMed2006

Control of nanopore wetting by a photochromic spiropyran: a light-controlled valve and electrical switch.

By modifying the surface of nanoporous alumina membranes using mixtures of a photochromic spiropyran and hydrophobic molecules, it is possible to control the admission of water into the membrane using light. When the spiropyran is in the thermally stable, relatively hydrophobic closed form, the membrane is not wet by an aqueous solution. Upon exposure to UV light, the spiropyran photoisomerizes to the more polar merocyanine form, allowing water to enter the pores and cross the membrane. Thus, the photosensitive membrane acts as a burst valve, allowing the transport of water and ions across the membrane. If the aqueous solution contains ions, then the membrane acts as an electrical switch; photoisomerization leads to a two-order-of-magnitude increase in ionic conductance, allowing a current to flow across the membrane. Exposure to visible light causes photoisomerization of the merocyanine back to the closed, spiro form, but dewetting of the membrane does not occur spontaneously, due to a high activation barrier.

Benzopyrans↗
PubMed2001

Background light adaptation of the retinal neuronal adaptive system. I. Effect of background light intensity.

The behaviour of the neuronal adaptive retinal mechanisms to environmental light exposures was studied by measuring the oscillatory potentials (OPs) of the electroretinogram. Dark adapted rats were exposed to four levels of background light (BG), starting at a 'low scotopic' level of 1.43x 10(6) cd/m2, increased by steps of two log units, through 'high scotopic' -, 'low mesopic' - and finally the 'high mesopic' BG of 1.43x 10(0) cd/m2. The summed oscillatory response significantly increased as the BG intensity was raised, except at the 'high mesopic' level. The amplitudes of the a- and b-waves reduced as the BG light increased above the 'high scotopic' level. Each OP responded individually to the different BGs. O1 and O2, significantly enhanced at the 'low scotopic' BG. The amplitudes of the three later OPs increased significantly at the 'low mesopic' BG. The adaptational behaviour of the retinal oscillatory response to BG illumination was different to that of the a- and b- waves. The results indicate that the adaptational neuronal system, as reflected by the OPs, seems to be relatively robust and is separate from the slower photochemical adaptive process in the distal retina. The tentative corollary suggests the oscillatory system to play a vision-preserving role, possibly as an alert against undue depletion of the slowly regenerating visual pigment. The enhancement of the oscillatory response at the 'mesopic' illumination levels indicate both scotopic and photopic processes to contribute to neuronal adaptive activity of the retina.

Adaptation, Ocular↗
PubMed2006

Electronic structures of intermolecular charge-transfer states in fast electron transfers with tetrathiafulvalene donor. Thermal and photoactivation of [2 + 4] cycloaddition to o-chloranil acceptor.

Tetrathiafulvalene (TTF) spontaneously forms a series of unusual charge-transfer complexes with various quinonoid acceptors such as o-chloranil (CA) that show pronounced near-IR absorption (lambda(CT) = 1100 nm). The successful isolation of the corresponding [1 : 1] donor-acceptor complex from solution and X-ray crystallographic analysis at low temperatures reveal the polarized charge-transfer state: [TTF(q+),CA(q-)] with high degree of charge-transfer (q = 0.6), which is spectrally and crystallographically distinguished from the separate redox (ion-pair) state: [TTF(+*) + CA(-*) ]. The unique interconversion of charge-transfer and electron-transfer states is theoretically well-accommodated by Mulliken theory using semi-empirical valence-bond and molecular-orbital methodologies. Mechanistic implications are discussed of both the thermally activated and the photochemically promoted processes via fast (intracomplex) electron transfer followed by collapse of the adiabatic and the non-adiabatic (vibrationally-excited) ion-pairs, respectively, to the [2 + 4] cycloadduct of tetrathiafulvalene and o-chloranil.

Journal Article↗
PubMed2006

The nonadiabatic deactivation paths of pyrrole.

Multireference configuration interaction (MRCI) calculations have been performed for pyrrole with the aim of providing an explanation for the experimentally observed photochemical deactivation processes. Potential energy curves and minima on the crossing seam were determined using the analytic MRCI gradient and nonadiabatic coupling features of the COLUMBUS program system. A new deactivation mechanism based on an out-of-plane ring deformation is presented. This mechanism directly couples the charge transfer 1pipi* and ground states. It may be responsible for more than 50% of the observed photofragments of pipi*-excited pyrrole. The ring deformation mechanism should act complementary to the previously proposed NH-stretching mechanism, thus offering a more complete interpretation of the pyrrole photodynamics.

Journal Article↗
PubMed2003

Photoexcited breathers in conjugated polyenes: an excited-state molecular dynamics study.

pi-conjugated polymers have become an important class of materials for electronic devices. Design of these devices requires understanding such processes as photochemical reactions, spatial dynamics of photoexcitations, and energy and charge transport, which in turn involve complex coupled electron-vibrational dynamics. Here we study nonlinear photoexcitation dynamics in the polyene oligomers by using a quantum-chemical method suitable for the simulation of excited-state molecular dynamics in extended molecular systems with sizes up to hundreds of atoms. The method is based on the adiabatic propagation of the ground-state and transition single-electron density matrices along the trajectory. The simulations reveal formation of a self-localized vibronic excitation ("breather" or multiquanta bound state) with a typical period of 34 fs and allows us to identify specific slow and fast nuclear motions strongly coupled to the electronic degrees of freedom. The effect of chain imperfections and chemical defects on the dynamics is also investigated. A complementary two-dimensional analysis of corresponding transition density matrices provides an efficient way to monitor time-dependent real-space localization of the photoexcitation by identifying the underlying changes in charge densities and bond orders. Possible correlated electronic and vibrational spectroscopic signatures of photoexcited breathers are predicted, and generalizations to energy localization in complex macromolecules are discussed.

Algorithms↗
PubMed1978

Visual pigment and photoreceptor sensitivity in the isolated skate retina.

Photoreceptor potentials were recorded extracellularly from the aspartate-treated, isolated retina of the skate (Raja oscellata and R. erinacea), and the effects of externally applied retinal were studied both electrophysiologically and spectrophotometrically. In the absence of applied retinal, strong light adaptation leads to an irreversible depletion of rhodopsin and a sustained elevation of receptor threshold. For example, after the bleaching of 60% of the rhodopsin initially present in dark-adapted receptors, the threshold of the receptor response stabilizes at a level about 3 log units above the dark-adapted value. The application of 11-cis retinal to strongly light-adapted photoreceptors induces both a rapid, substantial lowering of receptor threshold and a shift of the entire intensity-response curve toward greater sensitivity. Exogenous 11-cis retinal also promotes the formation of rhodopsin in bleached photoreceptors with a time-course similar to that of the sensitization measured electrophysiologically. All-trans and 13-cis retinal, when applied to strongly light-adapted receptors, fail to promote either an increase in receptor sensitivity or the formation of significant amounts of light-sensitive pigment within the receptors. However, 9-cis retinal isin. These findings provide strong evidence that the regeneration of visual pigment in the photoreceptors directly regulates the process of photochemical dark adaptation.

Adaptation, Physiological↗
PubMedDate not supplied

A new microporous polyurethane vascular graft prepared by an excimer laser ablation technique.

Three types of polyurethane (PU) based tubes (internal diameter, 2 mm; wall thickness, 100 microns) with micropores of well controlled size and arrangement were fabricated using an excimer laser (KrF) ablation technique. The pore size (100 microns) and the longitudinal pore-to-pore distance (200 microns) were constant, and the circumferential pore-to-pore intervals were 60 degrees (type 1), 30 degrees (type 2), and 15 degrees (type 3). The surface of the fabricated tube was photochemically modified with photoreactive gelatin. Scanning electron microscopy showed that pore size and arrangement were precisely controlled as designed, and that a gelatinous layer thoroughly covered the luminal surface. The stiffness parameter (beta), inversely related to compliance, was determined from the change in external diameter against intraluminal pressure. An increase in the number of pores around the circumference decreased the beta value. The type 1 tubes implanted preliminarily in rats for 4 weeks showed good patency (80%). The combination of excimer laser-directed microporing and photochemical surface processing techniques enabled the development of a novel compliant small caliber vascular graft, which is expected to show enhanced transmural tissue ingrowth in vivo.

Animals↗
PubMed1992

Quenching of singlet molecular oxygen by phthalocyanines and naphthalocyanines.

Using the direct measurement of the photosensitized luminescence of singlet molecular oxygen (1O2) the rate constants (kq) have been determined for 1O2 quenching by the monomeric molecules of the following phthalocyanines and naphthalocyanines in chloroform: tetra-(4-tert-butyl) phthalocyanine (I); octa-(3,6-butoxy) phthalocyanine (II), tetra-(6-tert-butyl)-2,3 naphthalocyanine (III), aluminium tetra-(1-tert-phenyl)-2,3 naphthalocyanine (IV), tri-(n-hexyl-siloxy) derivatives of silicon- (V), tin- (VI), aluminium- (VII) and gallium- (VIII) 2,3 naphthalocyanine. The following kq values were obtained (kq x 10(-8) M-1 s-1): 2.9 (I), 59 (II), 100 (III), 20 (IV), 3.9 (V), 53 (VI), 33 (VII), 110 (VIII). As most of the quenchers have the low-lying triplet levels, a contribution of the quenching mechanism based on the energy transfer from 1O2 to these levels has been analysed. A formula is proposed describing the relation between kq values caused by this mechanism, and photophysical constants of the quencher triplet state. This formula was applied to phthalocyanines, naphthalocyanines, beta-carotene and bacterochlorophyll a. The data suggest that the energy transfer can fully explain the activity of V and strongly contributes into the activities of II, III and VI-VIII. A charge transfer interaction might be an additional mechanism involved in 1O2 quenching by compounds studied. As some phthalocyanines and naphthalocyanines are strong physical quenchers of singlet oxygen they can be used as efficient inhibitors for photodestructive processes in photochemical systems.

Indoles↗
PubMed2001

Photochemical effects and hypericin photosensitized processes in collagen.

Emission and excitation spectra of collagen were recorded in the ultraviolet and visible regions. The existence of several types of chromophores absorbing and emitting throughout these spectral regions was observed. It was shown that laser irradiation at 355 and 532 nm caused collagen fluorescence photobleaching by 30%, when the delivered light doses were 9 and 18 J/cm2, respectively. This process of collagen fluorophores photodestruction was found to be a one-photon effect. The effect of hypericin (HYP), a polycyclic quinone, photosensitization on collagen was also studied. Addition of HYP aqueous solution to collagen produced quenching, redshift of the maximum, and broadening of the spectral form of its fluorescence. These effects became more prominent with increasing HYP concentration. The fluorescence of HYP sensitized collagen decreased in a spectrally nonproportional manner during laser irradiation at both 355 and 532 nm.

Animals↗
PubMed2002

A new method of marking dentures using microchips.

Over the years various methods of denture marking have been reported in the literature. They include surface marking and inclusion techniques using metallic or non-metallic materials, microchips and microlabels. The microchips are preferred because of their small size and aesthetic acceptability. They are not however widely used due to the high cost of manufacture and data incorporation. This article details the procedures involved in inscribing a microchip using the photochemical etching process used in the electronics industry. The resulting microchip was cosmetically appealing, cost effective and was able to satisfy all the forensic requirements for a suitable denture marker.

Acids↗