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This PDF file contains the front matter associated with SPIE Proceedings Volume 7049, including the Title Page, Copyright information, Table of Contents, Introduction (if any), and the Conference Committee listing.
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We measure two-photon absorption (2PA) spectra and 2PA cross sections in an assortment of different molecules such
as substituted diphenylaminostilbenes and push-pull porphyrins using femtosecond fluorescence excitation method. The
peak 2PA cross section in the lowest dipole-allowed transition is well described by two level model and can be estimated
with better than 50% absolute accuracy from the value of transition dipole moment and permanent dipole moment
difference between ground and excited state that we obtain solely from linear spectroscopic measurements. 2PA peaks
corresponding to transition to higher energy states are quantitative described by three-level model. We find also that
larger value of the permanent dipole moment difference correlates with a smaller value of permanent dipole moment in
the electronic ground state.
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The developments in porphyrin chemistry over the last decades give great advantages for the practical use of
porphyrin-based compounds. The properties of these compounds can be systematically tuned by rational utilization of
substituents on meso- and/or β-positions as well as by using different metal atoms in the center of the tetrapyrrole
macrocycle.
Recently we prepared novel mono- and bis-functionalized cycloketo-porphyrins (CKPors). In this work the results
of detailed spectroscopic investigations of these compounds are presented. It was found that a seven-membered ketone
exocycle remarkably influences the photophysical properties of the CKPor systems. For mono-functionalized CKPors it
results in strongly enhanced probability of intersystem crossing S1 → T1 with an ISC quantum yield up to 90%.
Moreover, the absorption of all CKPors undergoes a bathochromic shift and the Q-bands extinction is above two times
higher compared to that of H2TPP, what makes these compounds promising candidates for use as photosensitizers in
photodynamic therapy of tumors.
For the first time two NH-tautomers of nonsymmetrical CKPors were experimentally resolved at room
temperature using optical spectroscopic methods. It was found that the concentration of tautomer A with a lower
frequency of the S0,0 → S1,0 transition is higher than that one of tautomer B at room temperature, and becomes dominant
with cooling down. In contrast - and as it is expected - only one optical active species was observed for non-symmetrical
CKPor with a central Zn(II) atom as well as for symmetrical bis-CKPor.
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There has been much interest in the development of two-photon absorbing materials and many efforts to understand the
nonlinear absorption properties of these dyes. We have recently explored a new type of two photon absorbing dye
containing a platinum center with ligands that vary in length that contain electron withdrawing benzothiazole. With
increased π-π* conjugation we expect to observe a red shift in the absorption properties of the material. We have
investigated the photophysical properties of the platinum chromophores using a variety of experimental techniques.
Previously we determined that the singlet and triplet excited states are responsible for nearly all of the nonlinearity in the
nanosecond regime accept the two photon mechanism that is primarily used for excitation. Therefore we would like to
tune the photophysical properties of both the singlet and triplet excited state in these materials. To our surprise we found
there is quite a bit of red shifting due to a metal-to-ligand charge transfer from the platinum to the ligand rather than the
expected shifting due to increased π-π* conjugation. However, with increased ligand length the chromophore does take
on more π-π* character.
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To learn about excited state geometry in biphenyl-containing platinum acetylides, we synthesized a series of
compounds that have biphenyl ligands. The ligands consisted of biphenyl(I), the hindered 2'-methyl biphenyl(III) and
planar fluorenyl(IV) groups. We also synthesized a "half" complex(II) consisting of one ligand attached to the platinum
atom. The optical properties of these compounds were measured by ground state absorption, phosphorescence, ultrafast
transient absorption and nanosecond transient absorption spectroscopy. DFT calculations were performed to determine
the ground state and triplet state geometries and the lowest triplet energy. TDDFT calculations were performed to
determine singlet excited state energies. Compared to the reference compound I, ground state spectra show a blue shift
in II and III and red shift in IV, showing the singlet energy is sensitive to conjugation and biphenyl twist angle.
Comparison of the phosphorescence spectra of I and II shows the triplet exciton is confined to one ligand. The time
behavior of the ultrafast excited state absorption spectrum of I shows a red shift within 1 ps from the initial spectrum.
This behavior is not seen in IV. The different behavior suggests formation of the triplet state of I is accompanied by
conversion from a non-planar to a planar conformation while IV retains a planar conformation.
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Hyper-Rayleigh scattering (HRS) is the only second-order nonlinear optical (NLO) technique allowed in an isotropic solution. Being an even-order technique, it is sensitive to (non-centro)symmetry. Therefore, HRS is a unique tool to determine solution-phase structure, both in a qualitative and a quantitative way. Examples are presented of the elucidation of the actual D2d octopolar structure of highly symmetric, yet non-centrosymmetric chromophores and of the
determination of the value for the opening angle of a chromophore-functionalized alkynyl-calix[4]arene cavity.
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We report on a pump-probe photothermal lens experiment aimed for the measurement of thermal diffusivity
coefficient of organic samples in the CW regime. We show that when the probe beam is collimated and the pump
beam is focused the time dependence of the signal does not depend on the sample position. This effect allows simple
determination of the thermal diffusivity coefficient and its effective calibration using reference samples. We use this
method to determine the thermal diffusivity of distilled water, methanol, chloroform, nitrobenzene and other organic
solvents.
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Optical properties such as index of refraction and optical absorption of many chromophore-doped polymers are sensitive to the physical and chemical environment to which the polymers are exposed. Detection sensitivity is further enhanced by optical micro-resonator structures such as waveguide micro-ring resonator and fiber Bragg gratings.
Chromophore-doped polymers also offer some desirable flexibility in device fabrication. Ultraviolet light and electron beam can reduce the index of refraction of the polymer. The photobleaching and electron beam bleaching methods form optical waveguides in a single fabrication step and do not involve solvents or wet chemicals, and can be applied to polymers that are not compatible with other waveguide fabrication techniques. This Paper provides an overview of the basic principles and designs of such sensors. A chemical sensor to detect trace explosives and a broadband fiber optic
electric-field sensor are presented as practical examples.
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In the optical materials, the remarkable change of refractive index due to optical intensity is important for making
photo-devices such as optical switching, memory and logic circuits. The optical waveguide consisted of poly
(3-hexylthiophene)/polymethylmethacrylate (P3HT/PMMA) composite film and a prism was fabricated to find out its
optical bistable characteristics. The refractive index of P3HT/PMMA composite film measured by ellipsometry was 1.48.
Moreover, the refractive indexes of the atmosphere and the prism were 1.00 and 1.52 respectively. Therefore, the
fabricated waveguide satisfied the condition of the quasi-waveguide. For improving the nonlinear optical characteristic
of the composite film, P3HT/PMMA composite film was exposed to organic gas for 25 hrs. As the laser light source,
Nd:YAG laser (wavelength: 1064 nm, pulse width: 5 ns, repetition frequency: 10 Hz) was adopted for optical bistability
and third-harmonic intensity measurement. The input light intensity dependences of the optical bistable characteristics of
the quasi-waveguide consisting of the P3HT/PMMA composite thin film, which was exposed to organic gas for 25 hrs
were investigated. The measured optical bistability displaced excellent stability and hysteresis characteristics. It suggests
that the composite film exposed to organic gas has larger grain size, better molecular orientation, homogeneous bulk and
smooth surface than that of before organic gas treatment.
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Surface relief structures are optically inscribed onto azobenzene containing thin films. We present a brief review of the
technique and results. The films act either as optical waveguides of as substrates upon which thin gold films are
deposited to support surface plasmon waves. Multiple gratings are inscribed to act as optical couplers and Bragg
gratings. Here, we report on the amplitude and phase changes that occur when the incident light is resonantly coupled
into waveguide or surface plasmon modes. We illustrate the method of obtaining the dispersion curve of the device. The
effects on amplitude are readily observed in the transmission or reflection spectra. In addition, since the structures can be
made such that the resonant TE and TM modes to be well separated, we can measure the phase changes of the
transmitted or reflected beams near resonance. A simple device showing polarization to wavelength modulation
encoding is presented.
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Passive sol-gel materials play an important role in the development of electro-optic(EO) polymer-based modulators,
because of their variety of available refractive indices. They can be used to form passive waveguide transitions to
minimize coupling loss or as cladding layers for the EO polymer. The demands for these two applications are different.
For waveguide transitions the most important factor is the optical loss. Cladding layers should have a relatively high
conductivity at elevated temperatures to improve poling efficiency. Both demands are addressed in this study. The
synthesis of low loss (down to 0.45 dB/cm) sol-gel materials is shown. Slab waveguides as well as ridge waveguides
were fabricated and characterized by liquid prism measurements and cut-back loss measurements, respectively. For use
in cladding layers surrounding the EO polymer, materials with higher conductivity were developed. The conductivity of
the materials was increased, (3•10-9 S/m) through the use of a silane, which allows in situ formation of proton donating
functionalities. All developed materials can be used as solvent free resins, which enables classic photolithography as
well as patterning by UV-imprinting. The available refractive index range (at 1.55 μm) is from 1.495 to 1.562.
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Poly(methyl methacrylate-co-9-anthrylmethyl methacrylate) (PMMA-AMA) LP-136 with various AMA contents was
prepared. The polymer was modified via Diels-Alder (D-A) type "click chemistry". In one approach, the side-chain was
grafted stepwise with maleimide-containing chromophore AJL-04 followed with N-phenylmaleimide (PI) to form LP-160. LP-160 was doped with 30 wt % of chromophore AJLS-102 to give electro-optic (EO) core polymer AJ-415. In the
other approach, all the pending AMA groups were modified with PI in one step to yield LP-165. Doping 33.7 wt %
AJLS-102 in LP-165 gives another core polymer AJ-416. The EO and material properties of both polymers were
systematically studied. Via careful selection of bottom and top cladding materials with proper optical and electrical
properties, Mach-Zehnder type modulators were fabricated based on both core materials. At the operational wavelength
of 1550 nm, modulator with AJ-415 core has half-wave driving voltage (Vπ) of 0.95 V and insertion loss of 19.1 dB,
while the best results from modulators with AJ-416 core are 0.75 V of Vπ and 17.1 dB of insertion loss. AJ-416 also has
the advantage over AJ-415 for building EO modulator with better processibility and long-term stability.
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The fluorescence of chromophores embedded in a photonic crystal is inhibited by the presence of a photonic pseudo-gap. We present the influence of such an incomplete bandgap on the emission and energy transfer by studying the steady-state and time-resolved emission properties of both a donor and an acceptor fluorophore in a self-assembled photonic crystal. Our results clearly show an inhibition of the donor emission and a concomitant enhancement of the acceptor emission, indicating improved energy transfer from donor to acceptor. This is explained by the decreased number of available
photonic modes for radiative decay for the donor in a suitable engineered photonic crystal with respect to in the effective
homogeneous medium.
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We report a technique for embedding submicrometer-scale polymer defects in the interior of self-organized
two-dimensional photonic crystals by controlled two-photon induced polymerization. They demonstrate a rapid and
flexible technique for optical fabrication by creating polymer features in registration with a photonic crystal. Polymer
features were embedded in individual pores with a diameter of 100 nm by controlled photopolymerization under
confocal optical microscopy. Spectrum measurements confirm that the photonic stop band limits the light propagation
of the emission from the embedded polymer structures.
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Gold clusters with the sizes close to the Fermi wavelength of electron shows interesting quantum size effects. Linear and
nonlinear optical properties show dramatic trends when the sizes of clusters are in the range of quantum confinement.
We have investigated the size dependence of the non-linear optical property of two-photon absorption (TPA) cross-sections
of the gold clusters. Absolute TPA cross-sections are measured by a combination of one and two-photon excited
fluorescence upconversion measurements. Large cross-sections and abrupt changes in the trend of cross-sections are
observed in the size-dependence when size is reduced from nanoparticles to cluster. The results can be attributed to the
appearance of quantum confinement in these monolayer protected gold clusters.
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Holographic polymerization (H-P) has been used to fabricate polymer-dispersed liquid crystals, block copolymers and
pattern inert nanoparticles. In this article, one-dimensional grating structures of Norland resin and a polymer blend were
achieved using the H-P technique. A reflection grating structure known as a Bragg reflector (BR) was fabricated. The
hierarchical structure and morphology of the BR were studied using synchrotron X-ray, polarized light microscopy and
transmission electron microscopy. The structure of the BR containing a polymer blend displayed lamellae structures
formed with periodicity of 200 nm. Polycaprolactone and Poly(L-lactide) crystals were found to be confined in ~
60 nm thick layers in the BR. The polymer chains tended to orient themselves parallel to the grating when the two polymers
where blended together. The phase separation and structure of the polymer blend inside the H-P grating could be of great
interest for multifunctional optical sensors or devices.
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We present the design, fabrication and characterization of the optical properties of one-dimensional metal-organic
photonic bandgaps (MO-PBGs) composed of a tetraphenyldiaminobiphenyl-based polymer and ultrathin electrically
continuous Cu layers. The fabricated MO-PBGs achieve a peak transmission of around 44% at 620 nm combined with
very large spectral, around 120 nm FWHM, and angular, more than 120° field-of-view, bandwidths. Using 140 fs pulses
at various wavelengths we have found up to 10 × enhancements in the nonlinear optical (NLO) properties of the MO-PBGs
when compared with the NLO response of ultrathin electrically continuous Cu layers.
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Polymeric Integrated Optics for Communication Applications
Multiple users could be multiplexed into a single Coarse Wavelength Division Multiplexing (CWDM) channel of
metropolitan area networks using an Optical Code Division Multiple Access (OCDMA) scheme increasing the total
number of users of the system. Thermally tunable holographic filters operated using an edge illuminated transmission
hologram configuration, can provide a compact and tunable solution for this application. The filters are realized by a
thick unslanted grating. The gratings are recorded in PQ (phenanthrenequinone)-doped PMMA (poly
methylmethacrylate) photopolymer substrate in a holographic setup. The gratings are designed to filter light from the
propagation direction for specific segments of a CWDM channel. The filters can be thermally tuned using thermo-electric
cooler plates to change the period of the grating. In this paper we present the construction and performance
characteristics of these filters.
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The third-order nonlinear optical properties of regioregular poly(3-hexylthiophene) (RR-P3HT) thin films
prepared on fused glass substrate were evaluated. The surface modification by hexamethyldisilazane (HMDS) and
octadecyltrichlorosilane (ODTS) was performed on the glass substrate to form self-assembled monolayer (SAM) layers.
The formation of SAM layers on the glass substrate increase the contact angle of the solution and the optical property of
the RR-P3HT thin films is enhanced due to the excellent orientation and alignment of the thin film. The π-conjugated
macromolecule thin films can be prepared by spin-coating and drop-casting methods and the structure and orientation
alignment of thin films can be controlled by the solution processing and deposition techniques. The nonlinear optical
property, third-harmonic generation of RR-P3HT thin films has been evaluated by Maker-fringe method. The third-order
nonlinear optical susceptibilities χ(3) (-3ω; ω, ω, ω) of drop-cast RR-P3HT thin films on quartz glass substrate were
estimated from optical third-harmonics (TH) intensity measurement. An Nd:YAG laser with a wavelength of 1064 nm,
pulse width of 5 ns and a repetition frequency of 10 Hz was used to evaluate the TH intensity. The effect of surface
modification of quartz glass substrate by HMDS and ODTS on the RR-P3HT film structure was also investigated. The
orientation alignment and crystallinity of the RR-P3HT thin films were evaluated using X-ray diffraction (XRD) and
UV-vis absorption spectra. The UV-vis and XRD profile reveals the better orientation and crystallinity of the RR-P3HT
thin film after surface modification by HMDS and ODTS. Moreover the incident angle dependences of third harmonic
(TH) intensity was measured and the TH intensity of RR-P3HT thin film prepared on glass substrate with SAM layer
was found to higher than that of non-treated substrate. The SAM layers significantly enhances the optical property of the
material and the third-order nonlinear optical susceptibility (χ(3)) of RR-P3HT thin films on quartz glass surface modified
by ODTS is 1.90 × 10-8 esu. The third-order nonlinear optical susceptibility (χ(3)) of RR-P3HT thin film was found to
higher than poly(p-phenylenevinylene) (PPV).
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The refractive index is a key characteristic of polymer materials in optical applications. For organic
polymers, typical refractive indices are in the range of 1.35 to 1.65. Extending the refractive index beyond
the limits is of fundamental scientific interest and would enhance the utility of polymers in many
applications. Polymeric thin films fabricated by plasma enhanced chemical vapor deposition (PECVD)
have been investigated in the fields of electronics and optics and their utility is becoming more widespread
in a variety of applications. Outstanding attributes of the PECVD photonic films include a smooth surface,
dense crosslinking structure, robustness, environmental resistance, optical transparency in either visible or
IR regions, and good adhesion to many optical window and substrate materials. In recent years, our
laboratory has fabricated novel polymer optical coatings and films by PECVD. One focus of this research
has been to expand the achievable maximum refractive index. This goal has been sought using two
approaches including increasing the conjugation and crosslinking of chemical moieties of the bulk film and
incorporation of metal ions into the structure. The techniques of XPS, FTIR, HRSEM, and ellipsometry
were used to characterize both the optical properties and the chemical structure of plasma polymerized
benzene, ferrocene, and metal-phthalocyanine thin films. The structure-property relationship and the effect
of PECVD processing conditions are also discussed in this presentation.
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It was studied the influence of F, Sbt, Sil, Sbo monomer and homodimer Dst-5, Dst-10, Dbt-5, Dbt-10, Dil-10, Dbo-10 styryl dyes on blood erythrocytes of white rats. It was shown that the homodimer styryl
dyes Dst-5, Dbt-5 and Dbo-10 decrease the erythrocytes quantity by 1.5-2 times more as compared with
monomer dyes Sbt and Sbo. The main cause of dyes different action is the different oxidation degree of
intracellular hemoglobin evoked by these dyes. It was established that the observed effects was connected
with different penetration of these dyes through membrane of erythrocytes and with interaction of these dyes
with albumin localized in membranes of cells.
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We present a detailed study of the local environmental sensitivity of the commercially available laser dye, Styryl-9M.
Positions of the one-photon and two-photon absorption maxima and
two-photon absorption minimum of the dye are
sensitive to the solvent polarity. In aqueous solution its absorption and fluorescence spectra consist of two peaks whose
relative strength depend on the surrounding pH-s. The dye shows one of the highest two-photon absorption cross
sections, 700-1300 GM at the peak, among widely available compounds. Comparison of the linear and nonlinear
properties shows that its maximum cross section can be described by an effective two-level model. Based on the
properties of Styryl-9M we propose a new method of sensing local environment polarity in solutions and biological phantoms. We show that the dye is a promising candidate for two-photon biological imaging and microscopy.
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We report on Fourier transform spectra of deuterated proteins: Bovine Serum Albumin, Leptin, Insulin-like Growth
Factor II, monoclonal antibody to ovarian cancer antigen CA125 and Osteopontin. The spectra exhibit changes in
the relative amplitude and spectral width of certain peaks. New peaks not present in the non-deuterated sample are
also observed. Ways for improving the deuteration of proteins by varying the temperature and dilution time are
discussed. We propose the use of deuterated proteins to increase the sensitivity of immunoassays aimed for early
diagnostic of diseases most notably cancer.
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