Scalar and vectorial degenerate four-wave-mixing (DFWM) in azobenzene molecular K-RJ-4-3 [N,N-bis(5,5,5- tryphenylpentyl)-4-((4-tritylphenyl)diazenyl)aniline] and in chalcogenide a-As2S3 glassy films is experimentally investigated. A coherent self-enhancement (CSE) of holographic gratings (HG) in this geometry was experimentally confirmed, for the first time to our knowledge, thus establishing a new method of HG recording, the DFWM CSE recording. Scalar linear s-s, p-p and circular R-R(right) polarizations and orthogonal linear s-p and circular L(left)-R polarizations were used for HG recording with 2 μm period at 532 nm. In the case of K-RJ-4-3 film L-R polarizations were the most efficient enabling the maximum DFWM efficiency ρmax=14.5% whereas in the case of a-As2S3 film s-s polarizations were the best with ρmax=6.0%. DFWM CSE recording has exhibited a different polarization dependence compared to normal DWFM recording. CSE factor ρ/ρ0 (ρ0 being the initial ρ) was the highest for K-RJ-4-3 film (6.8) with s-s polarizations compared to 3 for a-As2S3 film with p-p polarizations. Two-wave HG recording was also studied for comparison.
Molecular organic compounds with electron donating fragment bounded through π-conjugated system with electron acceptor fragment, as well as with incorporated triphenyl groups in their molecules show potential for creating cheap and simple solution processable materials with nonlinear optical properties. Additional insertion of azobenzene fragment in their structures makes them also possible to form holographic volume and surface relief gratings (SRG) after exposure to laser radiation, which could be useful for holographic data storage. For these purposes polymers are generally used. However, their application is complicated and challenging task as in every attempt to obtain the same polymer it will have different physical properties. On the other hand, the synthetic procedure of molecular glasses is more simple as their structure and physical properties are strongly defined. Unfortunately, there is still no clear relation between compound organic structures and their thermal, glass-forming and optical properties.
In order to investigate the above mentioned regularities, we have synthesized and investigated ten molecular glassy organic compounds with three different fragments as main backbones of the molecules: indene-1,3-dione (WE-1, WE-2, WE-3), isophorene (IWK-1D, IWK-2M, IWK-2D) and pyranylidene (DWK-2TB, ZWK-2TB, JWK-2TB, ZWK-3AZO). Compounds containing isophorene fragment in their molecules had the highest NLO efficiencies (d33 up to 125.7 pm/V for IWK-2D) and also were the most effective holographic data storage compounds with holographic self diffraction efficiency 13% and holographic diffraction efficiency 20%, also for IWK-2D, but their thermal stability (Td from 288°C to 295°C) and glass transition (Tg from 90°C to 105°C) values were just average. Pyranylidene type compounds had the highest thermal stability and highest glass transition (Tg from 115°C to 180°C). But their ability to form and maintain amorphous structure were low and they had average NLO efficiencies (d33 up to 66.2 pm/V for ZWK-2TB) and average holographic self diffraction efficiency 2% and holographic diffraction efficiency 8% for ZWK-3AZO. The molecules with just azobenzene fragment and indene-1,3-dione as electron acceptor has the lowest thermal (Td from 250°C to 282°C, Tg from 70°C to 98°C) and also the lowest holographic properties with holographic diffraction and self diffraction efficiencies at 4% for WE-1 and lower for other compounds. Nevertheless, some of the investigated molecular glasses show potential as multifunctional optical materials.
New glassy 1,3-dioxo-1H-inden-2(3H)-ylidene fragment und (3-(dicyanomethylene)-5,5-dimethylcyclohex-1-enyl)vinyl
fragment containing push-pull type derivatives of azobenzene able to create thin layers have been synthesized. Thin
films of synthesized glasses for holographic recording were prepared using spin coating technique from saturated
chloroform solution. Holographic grating recording in films of 6a-b, 7 and 12 has been experimentally studied at 633
and 532 nm in both transmission and reflection modes with p-p recording beam polarizations. The film 12 was found to
be the most efficient at both wavelengths in transmission mode exhibiting the maximum self-diffraction efficiency of
9.9% at 633 nm, and 15.3% at 532 nm. The film of 6a was the most efficient in reflection mode with the maximum selfdiffraction
efficiency of about 3%.
The holographic recording efficiency in doped LiNbO3 crystals has been studied both experimentally and theoretically depending on the type of dope, on the recording geometry and on the polarizations of the recording and readout light.. The studied crystals can be arranged in the following order by their efficiency: LiNbO3:Cu, LiNbO3:Fe (yet having a smaller thickness and donor concentration than LiNbO3:Cu), LiNbO3:Fe+Cu, LiNbO3:Fe+Ti, LiNbO3:Ti. It was found that the recording geometry with the holographic grating vector along the optical axis is much more efficient than in the perpendicular configuration.This fact is in accordance with the photorefraction theory based on photogalvanic and linear electro-optic effects (PGE-LEO theory). Other recording mechanisms are active, too, but much less eficient. The recording efficiency polarization dependence is mainly determined by dopes.It is different in the cases of Fe and Cu impurities. It also follows from our studies that photoconductivity along the optical axis is much larger than in the perpendicular direction.
The minimum average optical signal power, Pmin., in optical communications is limited by the photodetector quantum efficiency and by noise. In this paper, the effect of thermal photons irradiated by all materials at absolute temperatures T>0 on optical information detection in communication lines is quantitatively considered. Usually, only the thermal current fluctuations in the photodetector are taken into account. Basing on the negentropy principle of information, assuming the Planck's blackbody radiation spectral distribution of photons, and describing the optical communication channel as non-symmetric noisy binary channel we have calculated the minimum energy required for the detection of one bit of information, ε= 6.5kT/bit, k =1.38×10-23 J/K being the Boltzmann constant. This ε value corresponds to the large error probability q = 0.20. At T = 20°C ε=4.05×10-21 J/bit and for the bit rate of R = 1010 bits/s one finds Pmin = Rε2.63×10-7 mW. In the case of more realistic value of q=10-9 ε=26kT/bit=1.05×10-19 J/bit, Pmin = 1.05×10-6 mW. This is only about 10 times lower than the quantum photodetection limit of conventional photodetectors. For more sensitive photodetectors the thermal photon noise can become important. It is shown that the minimum signal energy estimate ε≈10-19 J/bit is applicable also in a wider error probability range of q=10-3-10-15.
The transmission light intensity dependences of different silica glass fibres have been experimentally studied when
nanosecond pulse trains were incident. A pronounced 13-42% transmission increase was found in contrast to the
picosecond pulse irradiation when a monotonic transmission decrease took place. The photoinduced transmission
increase is explained in terms of photothermally increased numerical aperture, the photothermal lens effect, and the
photoinduced saturation of a weak impurity absorption. The obtained results can be applied in high power applications
of fibres such as WDM fibre communication systems.
Sub-bandgap light recording (SBLR) of holograms is studied basing on the experiments in a-As2S3 films and literature
data. Holographic grating recording with focused (light intensity I = 14 - 124 W/cm2 ) and unfocused (I = 0.50 - 0.78 W/cm2) 632.8 nm He-Ne laser sub-bandgap light in non-annealed and annealed a-As2S3 films has been experimentally studied. The focused light recording is found to be much more efficient (diffraction efficiency up to 14.9%, specific
recording energy down to 216 J/(cm2%)) than the unfocused light recording (0.11%, 72400 J/(cm2%)). Some other
properties are also different. The focused light recording is explained by the photothermally stimulated relaxational
structural changes (RSC) accompanied by the photoinduced generation and recharging of D-centers. The unfocused
light recording is explained by the photorientation of D-centers with some contribution of RSC . SBLR in materials other
than a-As2S3 films was considered and the conclusion was made that amorphous sulfides and selenides are expected to be the best SBLR recording materials. SBLR is advantageous because of its bulk nature enabling the production of
homogeneous holographic optical volume elements and devices.
The angular selectivity of thin gratings is studied both experimentally and theoretically. The concepts of thick and thin
gratings are analyzed. Thin holographic gratings recorded in a-As-S-Se films have exhibited pronounced and oscillatory
diffraction efficiency angular dependences. These results are explained by the obliquity factor in Fresnel-Kirchhof
diffraction integral and by finite beam and grating sizes. It is also shown that oscillatory diffraction efficiency angular
dependences, most probably, arise due to the interference of diffracted waves of different orders because dephasing can
be significant for small grating strengths and large enough readout angles. Fabry-Perot resonator effect can contribute as
well. Thick gratings in a-As2S3 and a-As-S-Se films are also studied for comparison. The conclusion is made that
normally all gratings possess angular selectivity and existing criterions underestimate the angular selectivity of thin
gratings because they neglect factors other than dephasing.
Light wavefront inversion (phase conjugation) in a-As-S-Se films has been studied experimentally. Phase conjugation (PC) of plane and spherical waves is carried out in a-As40S15Se45 films using degenerate four-wave-mixing (DFWM) geometry at 633 nm. In the plane wave case simultaneous PC efficiency and DE measurements have been made versus
exposure time, light intensity and holographic grating period. The maximal PC efficiency was 2.3% and the minimal PC specific recording energy was 2 J/(cm2%) whereas the maximal DE was 0.9% and the minimal specific hologram recording energy was 10 J/(cm2%). The optimal grating period was 2 μm. When compared to a-Se films a-As-S-Se films exhibit lower PC efficiency but higher photosensitivity. The advantages of a PC setup for the investigation of photoinduced processes in comparison with a usual holographic setup are observed.
Diffraction anisotropy (DA) defined as the polarization dependence of the amplitudes (amplitude DA) and phases (phase DA) of the diffracted light waves is studied in the case of a sinusoidal transmission amplitude-phase grating both theoretically and experimentally. Theoretical analysis was mainly based on the Kogelnik's coupled wave theory (KCWT) and also on the conclusions of rigorous coupled wave theory (RCWT) and effective medium theory (EMT). Experimentally gratings with 0.42 μm period in a-As-S-Se films at 632.8 nm were studied. KCWT predictions were compared with those of RCWT and EMT as well as with the experimental DA results. It is found that KCWT properly describes the first order amplitude DA, and more roughly also the zeroth order amplitude DA. The zeroth order phase DA is wrongly described by KCWT. It is also found that polarization dependent Fresnel reflection effect is much stronger than DA therefore p-polarized hologram recording is preferable.
Elementary hologram (holographic grating) recording and their coherent optical erasure have been experimentally studied in azobenzene oligomer (ABO) layers differing by their chemical composition, matrices and by the connection type of azobenzene chromophores to the matrix (dispersed or covalently bound). The best holographic parameters (7.9% diffraction efficiency and 86 J/cm2 specific recording energy) were achieved in the samples with covalent bonding to the matrix. Vector recording is also possible. Recording is unstable and reversible. The coherent optical erasure studies have shown its efficiency dependencies on the initial diffraction efficiency, erasing beam intensity and grating period which are different for three groups of ABO samples. The conclusion is made that recording is due to the photoinduced alignment of the azobenzene chromophores followed by refractive index changes. These are the first results and further studies are in progress.
The effect of photoinduced anisotropy and its application to vector hologram recording is reviewed focusing on amorphous chalcogenides. Vector holographic grating recording in amorphous As-S-Se(a-As-S-Se) films is experimentally studied and analyzed in comparison with scalar recording. It is holographically established that a linearly polarized 632.8 nm light produces photoinduced anisotropy and the chalcogen related D+, D- center reorientation and generation mechanism is proposed. It is used to explain the observed peculiarities of vector recording in comparison with scalar recording based on photoinduced structural changes: much lower diffraction efficiency (4 X 10-3% versus 4%), much larger specific recording energy [6.4 kJ/(cm2%) versus 20 J/(cm2%)], difference in spatial frequency response, instability (vector hologram lifetime of about two days versus practically permanent scalar holograms), the absence of hologram self-enhancement (present in scalar recording), near perfect reversibility. It is also experimentally found that vector holograms in a-As-S-Se films indeed reconstruct the signal wave polarization but only in the minus first diffraction order. It is also shown that photoinduced anisotropy also contributes to the scalar hologram recording in amorphous chalcogenides stimulating it by means of subbandgap readout light and enabling a subbandgap recording.
Holographic recording properties and mechanisms are analyzed and compared in dielectric electrooptic crystals (EOC), dielectric colored alkali halide crystals (AHC) and amorphous semiconductor films (ASF) basing on author's investigations as well as on the literature data. Holographic photosensitivity parameters are introduced enabling the characterization of the recording mechanism efficiency independently of the particular optical and geometrical sample parameters, and allowing also for recording optimization. Ultimate specific recording energies for EOC, AHC and ASF are theoretically estimated. It is concluded that the ultimate recording energy for both crystalline and amorphous materials is of order of about 10-6(cm2%). Now the best holographic parameters for the scalar hologram recording are achieved in EOC. Then come ASF and AHC. Yet AHC so far are superior at vector hologram recording. Finally, the conclusion is made that ASF can become serious rivals of EOC in holography and optical information processing if other material properties are taken into account such as hologram lifetime, sample size and cost, hologram self-enhancement possibilities.
The mechanisms of holographic recording in (mainly chalcogenide) amorphous semiconductor films are reviewed including photoinduced structural changes, relaxational structural changes, recharging of localized states in the band gap, and photoinduced anisotropy. The holographic properties in these cases are compared. Different effects of hologram self-enhancement are also considered.
The results of the experimental study of holographic recording in a-As2S3 films are reported such as exposure and intensity dependencies, spatial frequency dependence. Several peculiarities are found including recording intensity threshold, nonmonotonical intensity dependencies, nonlinear exposure curves, the change of the spatial frequency response due to films aging. These peculiarities are explained in terms of phenomenological model which is based on the simultaneous action of the photostructural changes and the relaxational structural changes.
The effect of holographic grating (HG) size on their diffraction efficiency (DE) at different spatial frequencies is experimentally studied in amorphous AS-S-Se films. The HG size was changed by focusing the recording beams. It is found that reduction of the size from 1100 micrometer to 150 micrometer increases the maximal DE from 0.9% to 1.8%. Further reduction down to 20 micrometer decreases the maximal DE down to 0.08%. DE at lower spatial frequencies is attenuated more than at higher ones. The observed effects are explained by the nonuniformity of thin HG recorded by Gaussian beams as well as by the curvature of the focused wavefronts and peculiarities of the recording mechanism in As-S-Se films. It is concluded that minimization of hologram size in AS-S-Se films is feasible only down to 150 micrometers.
The present state of the real time holographic recording in amorphous semiconductor films is reviewed including mechanisms, parameters, properties and applications. Effects of the coherent, incoherent and relaxational self- enhancement as well as the influence of the film structure relaxation are considered. Quasi-permanent sub-band-gap light holographic recording is reported for the first time. 157
Attenuation intensity dependences of 1064 nm and 532 nm picosecond pulses in multimode optical fibers produced for medical purposes by 'Anda' factory in Livani, Latvia are experimentally studied. A strong linear growth of inverse transmittance with intensity is found. The possible mechanism of nonlinear losses are analyzed and the conclusion is made that the observed effect is mainly due to the two-photon absorption involving defects levels. Strong attenuation intensity dependence can be used to make such fiber optical devices as light power limiters, optically driven light modulators and dynamic holographic frequency filters.
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