Nonlinear optical properties of GaAs/(AlGa)XOY heterostructures using interband excitation by 150 fs laser pulses is
reported. A considerable wideband nonlinear response is observed. Mean decay time for nonlinear reflection in
heterostructures ranges from 1.5 to 3.5 ps. The shift of the GaAs energy-band structure caused by the high tensions in
GaAs/(AlGa)XOY structure is observed.
Reflectivity kinetics of semiconductor samples with GaAs/AlGaAs multiple quantum wells is investigated by the
pump-probe technique with temporal resolution of about 150 fs. Excitons of type E1HH1 and E1LH1 appear in
the kinetics of non-stationary spectra of reflectivity in spite of high density of photo-generated two-dimensional
electron gas. The difference in the shape and kinetics of nonstationary reflectivity spectra is found for the samples
with different detuning of exciton transition relative the pump radiation frequency.
The paper presents recent experimental results on the peculiarities of fluorescence and transient absorption exhibited by indotricarbocyanine dyes in solutions of different nature. The dynamics of transient absorption spectra of the molecules under study is analyzed within the framework of the concept of intra- and intermolecular vibrational relaxation and ultrafast charge transfer in contact ion pairs.
The dynamics and pathways of relaxation processes in meso-ortho-nitrophenyl substituted octaethylporphyrins OEP-OEPPh(o-NO2) and PdOEP-Ph(o-NO2) occurring with the participation of the S1 and T1 states was studied in polar
Ph((dimethylformamide) and nonpolar (toluene) solvents at 295 and 77 K using pico- and nanosecond laser kinetic
spectroscopy. At 295 K, steric interactions between bulky β-alkyl substituents and ortho-nitro groups of meso-phenyl in
these compounds create optimal conditions for overlapping of molecular orbitals of the porphyrin macrocycle (donor) and
NO2-group (acceptor), thus leading to an efficient photoinduced electron transfer (PET). For free-base OEP-Ph(o-NO2),
PET occurs only via the porphyrin S1 state within 40 ps (dimethylformamide) and 125 ps (toluene), whereas the competing
intersystem crossing S1 ~~>T1 is low probable. For metallocomplex PdOEP-Ph(o-NO2), PET involves both S1 and T1 states. In
the last case, the direct PET from the T1 state to CT state also occurs within picosecond range (20 and 46 ps for
dimethylformamide and toluene, respectively, at 295 K). Rate constants for PET with participation of T1 states are by 3-5
times smaller with respect to those found for PET occurring via the S1 state. For both compounds, the observed long-lived
component (250-700 ns) in decays of the transient T1-Tn absorption is due to the recombination processes of radical-ion
pairs whose lifetime decreases with an increase of the surrounding polarity and is hardly dependent on the presence of
molecular oxygen in the solution. For both compounds, PET is completely absent in rigid solutions at 77 K.
ZnS/ZnSe heterostructures under condition of ZnSe interband excitation by a 150 fs laser pulse exhibit strong narrow-band
modification of absorption and wide-band modification of reflection. Mean decay time for nonlinear reflection in
heterostructures ranges from 2 to 3 ps whereas in bare ZnSe monolayer it exceeds 5 ps. Possible physical processes
responsible for nonlinear refraction in the transparency region include interplay of absorption driven nonlinear refraction
via Kramers-Kronig relations and intrinsic dielectric properties of dense electron-hole plasma. For nonlinear absorption
at ZnSe band edge, interplay of plasma screening effects and states filling effects are relevant.
ZnS/ZnSe Bragg reflectors under condition of ZnSe interband excitation by a femtosecond laser pulse exhibit strong
narrow-band modification of absorption and wide-band modification of reflection. Mean decay time for nonlinear
reflection in heterostructures ranges from 2 to 3 ps whereas in bare ZnSe monolayer it exceeds 5 ps. Possible underlying
physical processes responsible for nonlinear refraction in the transparency region include interplay of absorption driven
nonlinear refraction via Kramers-Kronig relations and intrinsic dielectric properties of dense electron-hole plasma. For
nonlinear absorption at ZnSe band edge, interplay of plasma screening effects and states filling effects are relevant.
Nonlinear optical response of periodic structures based on ZnSe/ZnS heterostructures using interband excitation of a ZnSe sublattice by 1 50 fs laser pulses is reported. A considerable shift of reflection spectrum and large relative reflection changes were observed in a wide spectral range corresponding to the transparency region of ZnSe far from the intrinsic absorption onset. Evaluated refraction index change is about -0.02 with the relaxation time being about 3 picoseconds. The nonlinear refraction is supposed to be controlled by population induced absorption changes in ZnSe single crystals and relevant refraction index modification via Kramers-Kronig relations. The nonlinearity relaxation time is supposed to trace a transition from non-equilibrium to quasi-equilibrium distribution of electrons and holes within ZnSe conduction and valence bands, respectively, rather than electron-hole recombination time. The nonlinearity
mechanism does not reduce to just population dependent absorption saturation but essentially results from the specific distribution function in the first instance after excitation.
We investigated ultrafast nonlinear optical properties of periodic structures based on ZnSe/ZnS using interband and two-photon excitation of ZnSe sublatice by nano-, pico-, and femtosecond laser pulses. A considerable shift of reflection spectrum and large relative reflection changes were observed in a wide spectral range corresponding to the transparency region of ZnSe far from the intrinsic absorption onset. The nonlinear refraction is supposed to be controlled by population induced absorption changes in ZnSe and the relaxation time is controlled by a transition from non-equilibrium to quasi-equilibrium distribution of electrons and holes.
The photophysical and nonlinear properties of some push-pull fluorinated 4-(dicyanomethylene)- pyranes using the steady- sate and time-resolved picosecond spectroscopies with an electric-field-induced second-harmonic-generation technique have been investigated. Strong fluorescence quenching and large shifts of time-resolved transient picosecond spectra on going form nonpolar to polar solvents are connected with effective charge transfer interactions of polar singlet excited molecules with a polar environment. The high second- order polarizabilty (beta) equals 260 X 10-30 esu for one of the investigated push-pull pyranes allows to propose using such kind of molecules in the development of second- harmonic-generation elements.
We report on experimental and theoretical studies of a pulsed synchronously pumped Kerr Lens Mode-locking Ti:sapphire laser singularities as well as femtosecond pulses formation dynamics in a such system. The optimum resonator parameters were derived with the help of theoretical analysis based on nonlinear ABCD matrix formalism, conditions of pulsed synchronous pumping being taken into account. On this basis the practical recommendations for a resonator design necessary under such circumstances are offered.
Bleaching and darkening occurring in thin-film matrices with high concentrations of doped microcrystallites were explained in terms of the filling of quantum-well and surface energy levels with carriers excited by the picosecond laser pulses. The possibility of creating of the picosecond optically controlled interference and cavityless switches is discussed.
The process of the oxygen photodissociation and rebinding with human hemoglobin have been studied by the time-resolved absorption spectroscopy. The primary quantum yield (gamma) o does not depend on the pH and its estimated value is 0.3 +/- 0.1. The apparent quantum yield (gamma) corresponding to the portion of O2 molecules which escape from the protein to the solvent depends on the pH. It has been shown that the entrance and exit of the oxygen molecules into/from the globin matrix is controlled by the same Bohr residues. The pK values were calculated and the attribution was made. The unusual behavior of the oxygenation parameters at pH > 8.5 was observed and explained by the action of the (alpha) 140-Tyr and (beta) 145-Tyr. The picosecond ligand rebinding dynamics were measured and the phenomenon of the pK value change was studied. It was explained by the subunit tertiary structure relaxation in terms of the transition between deoxy-R- and oxy-R- structures of the tetramer protein.
To our knowledge we report the first fabrication of vacuum deposited thin film interferometers with an intermediate layer doped by quantum-confined semiconductor microcrystallites. These filters demonstrate new spectral and optical properties in addition to those typical for samples deposited by conventional thermal evaporation, and, in particular, high-speed optical switching with picosecond on/off time.
The experimental studies on ultrafast relaxation processes in organic radicals are presented. Three mechanisms of ketyl radical formation are established and separated: direct transfer of a hydrogen atom as a whole; two-stage transfer of an electron and of a proton in an excited complex; and proton transfer at diffusion encounters of anion and cation radicals. The thiyl radicals formation at homolytical photodissociation of organic sulfides by picosecond laser pulses occurs at a rate constant k
KEYWORDS: Picosecond phenomena, Absorption, Luminescence, Information operations, Temperature metrology, Bioalcohols, Silicon, Photosynthesis, Systems modeling, Polymers
Light energy absorption, as well as the subsequent photochemical and photophysical processes of cis -+trans
isomerisation (vision and bacteriorhodopsin photosynthesis) and energy transfer (photosynthesis in green plants and
micro organisms) take place in a pigment-protein complex including polyene chromophors, retinoids and carotenoids.
Picosecond and subpicosecond studies of the spectral and kinetic characteristics of these processes are carried out in
both complex photoreceptor and photosynthetic ms'2 and model systems with the use of solutions of retinoids
and carotenoids.36
The lifetimes of the lower singlet-exited states S (21A; ) ofsome carotenoids in toluene at room temperature have
been measured by the method of picosecond photolysis and amount to 8.6± 0.5 for all-trans-fl -carotene1 and 5.2 0.6
PS for canthaxanthin.5 /3 -carotene fluorescence at room temperature is practically absent, its yield being less than
iO (Ref. 7). /1 -carotene fluorescence at 77 and 4.2 K in isopentane discovered by us8 is characterized by yields of
(4±2) .iO and (8±3) . i0- and lifetimes of(4±2) .iO' and (8±3) .iO' and is due to the transitions from the
higher S(1' B) state. The picosecond transient S -S absorption of/I - carotene in different solvents at 293 K is
characterized by spectra in the 550-600 nm range.8 For retinoids, there is one work (Ref. 4) which gives the S, +-Si
absorption spectrum of the Schiff base (aldimine) of retinal with amaz 465 mn in n-hexane at 290 K. The duration
of transient absorption was 21 5 ps, although the fluorescence kinetics measured in this work (Ref. 4) at 298 K
were characterized by two-component decay with r1 = 22 and r2 = 265 ps. The transient picosecond absorption
spectra for retinal are absent in the literature and the lifetimes of its singlet-excited state at room temperature,
measured by absorption and fluorescence, amount to 20±10 Ps in n-hexane3 and 17 Ps in ethanol,'9 respectively.
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