Dynamics of light-induced diffraction gratings in silicon excited by picosecond pulses

On the basis of a numerical solution of the system of continuity equations we analyze the formation and decay of light-induced diffraction gratings in silicon under excitation by picosecond pulses. The concentration of nonequilibrium carriers generated at excitation-pulse intensities I₀ 10¹⁰ W/cm² reaches values of 10¹⁹–10²⁰ cm^–3. Estimates of the relaxation time of diffraction gratings from widely used formulas are shown to be too low because of the nonlinearity of the evolution of nonequilibrium carriers. The internal electric fields are calculated. The dynamics of diffraction gratings that are nonuniform over the depth of the sample have been studied experimentally as a function of the intensity of the excitation pulses. The experimental data accord with the results of numerical calculations.Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 3, pp. 53–58, March, 1990.     

Pulsed optoacoustic detection of multiple photon excitation in molecules

Multiple photon excitation, saturation, and linear absorption of SF₆-argon mixtures when irradiated by a high power CO₂ TEA laser is investigated using a pulsed optoacoustic technique. At low intensities the expected linear dependence of the absorption on laser intensity is observed. At intermediate intensities the absorption exhibits a square root dependence on the incident laser intensity, a dependence which is typical for saturation of an inhomogeneously broadened absorption. At even higher intensities, the absorption shows an intensity dependence typical of multiple photon excitation. The laser intensity was varied between 0.016 kW/cm² and 5 MW/cm², values lower than that needed to produce multiple photon dissociation of SF₆. Increasing the collision frequency of the absorbing molecules with an inert buffer gas is observed to quench the multiple photon excitation.     

Study of lattice vibrational modes in CuGaS2 by using fourier transform spectroscopy

The lattice dynamics of a single crystal of CuGaS₂, grown by iodine transport technique, have been studied by using far IR absorption spectroscopy. All the absorption maxima caused by the phonon excitation are compared with the lattice vibrational modes obtained by Raman spectroscopy and by IR reflection techniques. An absorption maximum located at 175 cm^?1 cannot be explained with the help of phonon excitation; however this peak can be attributed to the defect frequency originating from the replacement of gallium atom by sulphur in the v₁₇ mode of vibration. The frequency of this defect-induced vibrational mode is calculated by taking a modified molecular model approach, and is found to be 166.9 cm^?1, which is in reasonably good agreement with the experimentally observed value of 175 cm^?1.     

Photodiffraction in InGaAs/InGaAsP multiple quantum wells enclosed in a microcavity

We report new results on the diffraction properties of photoinduced gratings in InGaAs/InGaAsP MQW structures. The original feature of this device is that the QWs are enclosed in an asymmetric Fabry–Perot microcavity in order to increase the diffraction efficiency. We observe oscillations in the diffraction efficiency due to resonant effects in the microcavity. The experimental spectra are compared with theory. Diffraction efficiency at 1.55 μm attains a maximum value of 2.7% at a write beam fluence of 260 μ J cm⁻², and then decreases at higher fluences. We explain this phenomenon by an absorption saturation at high excitation.     

Femtosecond multicolor transient absorption spectroscopy of colloidal silver nanoparticles

Time-resolved femtosecond multicolor absorption spectroscopy of silver nanoparticle (NP) colloids with particle diameter in range of 10–30 nm is presented. The amplified femtosecond excitation of the surface plasmon resonance band resulted in transient absorption spectra reflecting the electron-phonon relaxation dynamics, which takes place on the early picosecond time scale. The monitored band with enhanced absorption in the 490–540 nm spectral range exhibited red-shift with increasing pump fluency from 0.4 mJ/cm² to the 1.5 mJ/cm² level. The growth of the relaxation time with increasing pump fluency reveals the temperature dependent relaxation dynamics caused by the nanometer sized electron confinement in the case of silver. This effect was confirmed also by identification of the relaxation time dependence on the particle diameter at constant pump fluency. The complex experimental results revealed nonlinearities both in the laser excitation and electron relaxation processes.     

Nonlinear fluorescence through intermolecular energy transfer and resolution increase in fluorescence microscopy

We investigate a novel concept to efficiently generate multiphoton induced fluorescence from organic molecules. The concept is based on frustrating the energy transfer between a fluorescent donor and one or more acceptors in conjugated molecules. The nonlinearity is not based on higher order molecular susceptibilities but entirely on their linear properties. Therefore, in contrast to nonresonant multiphoton absorption, this method does not require high local intensities. Likewise, the production of visible fluorescence does not require an infrared excitation wavelength. Hence, when applied to scanning microscopy this property is predicted to increase spatial resolution. Instead of the ∼10 GW/cm² required in non-resonant multiphoton excitation, focal intensities ∼10 MW/cm² are expected to produce an equally strong nonlinear signal. The predicted resolution is up to 30% greater than that of an ideal confocal microscope operating at the same fluorescence wavelength. The resolution improvement over non-resonant two-photon absorption microscopes is about two-fold in all directions.     

Electronic spectroscopy of Se2- in KBr

Rapid quenching of KBr crystals doped with Se^2- gives isolated Se^2- ions which are strongly luminescent. Two emission spectra were observed, one with a maximum intensity at about 14100 cm^-1 and the other with a maximum intensity at about 17200 cm^-1. Only the red emission is observed by excitation into the lowest energy absorption band at 24600 cm^-1, while between 10 K and about 150 K both red and yellow emissions are observed by excitation into the second absorption band at 26770 cm^-1. Both are assigned to the isolated Se^2- center in different distorted charge transfer states. The yellow emission is observed below about 100 K, reaches maximum intensity at about 35 K and is absent below 10 K. There are complementary changes in the intensity of the red emission so that the sum of the two emission intensities is constant. The absorption spectra of the isolated Se^2- and the (Se^2--vacancy) pair have been identified as well as the spectrum of a cluster of two or more (Se^2--vacancy) pairs.     

Er3+离子掺杂钡镓锗玻璃上转换发光机理研究

研究了Er³⁺离子掺杂钡镓锗玻璃的吸收光谱、拉曼光谱和上转换光谱.分析了Er³⁺离子在钡镓锗玻璃中的上转换发光机理.结果表明：玻璃的最大声子能量为828cm^-1，紫外截止波长为275nm.采用800nm和980nmLD激发玻璃样品，在室温下观察到强烈的上转换绿光和红光发射.随着Er³⁺离子浓度的增加，绿光发光强度先增加后减小，而红光发光强度呈单调递增趋势.能量分析表明：800nmLD激发产生的绿光主要源于Er³⁺离子4I_13/2能级的激发态吸收过程；红光发射主要源于Er³⁺离子4I_13/2能级与4I_11/2能级之间的能量转移过程.980nmLD激发产生的绿光主要源于Er³⁺离子4I_11/2能级之间的能量转移过程；而红光发射主要源于Er³⁺离子4I_13/2能级与4I_11/2能级之间的能量转移过程和4I_13/2能级的激发态吸收过程.通过量子效率分析，发现采用800nmLD激发Er³⁺离子掺杂浓度为1mol% 的样品时，上转换绿光发光效率最高. 关键词： 上转换发光机理 3+离子掺杂')" href="#">Er³⁺离子掺杂 钡镓锗玻璃     

Evidences for charge‐transfer complex formation in the benzene adsorption on sulfated TiO2–a resonance Raman spectroscopy investigation

Benzene adsorbed on highly acidic sulfated TiO₂ (S‐TiO₂) shows an intriguing resonance Raman (RR) effect, with excitation in the blue‐violet region. There are very interesting spectral features: the preferential enhancement of the e_2g mode (1595 cm⁻¹) in relation to the a_1g mode (ring‐breathing mode at 995 cm⁻¹) and the appearance of bands at 1565 and 1514 cm⁻¹. The band at 1565 cm⁻¹ is probably one of the components of the e_2g split band, originally a doubly degenerate mode (8a, 8b) in neat benzene, and the band at 1514 cm⁻¹ is assigned to the 19a mode, an inactive mode in neat benzene. These facts indicate a lowering of symmetry in adsorbed benzene, which may be caused by a strong interaction between S‐TiO₂ and the benzene molecule with formation of a benzene to Ti (IV) charge transfer (CT) complex or by the formation of a benzene radical cation species. However, the RR spectra of the adsorbed benzene cannot be assigned to the benzene radical cation because the observed wavenumber of the ring‐breathing mode does not have the value expected for this species. Moreover, it was found by ESR measurements that the amount of radicals was very low, and so it was concluded that a CT complex is the species that originates the RR spectra. The most favorable intensification of the band at 1595 cm⁻¹ in the RR spectra of benzene/S‐TiO₂ at higher excitation energy corroborates this hypothesis, as an absorption band in this energy range, assigned to a CT transition, is observed. Copyright © 2008 John Wiley & Sons, Ltd.     

Investigation of the optical absorption and emission spectra of CdCl2: Ni2+ single crystals

The optical absorption, emission, and excitation spectra of CdCl₂: Ni²⁺ single crystals are investigated. The absorption bands around 19,200 cm^-1 are reassigned and a few new bands above 22,000 cm^-1 are observed and assigned to singlet states. The emission bands at 77 K are examined in more detail and the previous assignments seem to be not correct.     

Optical bistability in fluorescein dyes

Optical bistability has been observed in highly concentrated fluorescein dye solutions and in thin (1 m) doped polymeric films. At concentrations larger than 10^–5 mole/l dye dimers are formed. For fluorescein dye, the dimer-monomer equilibrium constant is 10⁵ l/mole so that most of the dye species are in the dimer form. At 480 nm the dimer absorption cross section is 10^–18 cm²/molecule, while that for the dye monomer molecule is 7.6×10^–17 cm²/molecule. Upon laser excitation dimers dissociate to form monomers thus providing a highly nonlinear laser induced absorption. This high nonlinear absorption coefficient can be utilized for optically bistable response of the dye system.Optical bistability was observed by placing dye solutions or dye thin films inside a Fabry-Perot resonator and exciting it with 480 nm dye laser pulses of 10 ns duration. The effect is more pronounced in 10^–4 mole/l fluorescein than in 10^–6 mole/l fluorescein in which dimer formation is not that efficient.In disodium fluorescein no significant dimer formation is observed even at 10^–3 mole/l dye concentration. The observed bistability both in solution and in thin films can be explained in terms of recent models for optical bistability in nonlinearly absorbing molecular systems.     

Growth and spectral properties of Nd:GdVO4 laser crystal

In this paper, the Czochralski growth, absorption spectra, and photoluminescence spectra of Nd:GdVO₄ crystals are studied. From its absorption spectra, Nd:GdVO₄ is found to exhibit an anisotropic optical absorption effect, and its effective Judd-Ofelt parameters are calculated: Ω₂=10.281×10⁻²⁰ cm², Ω₄=5.426×10⁻²⁰ cm² and Ω₆=9.943×10⁻²⁰ cm². By these parameters, the absorption oscillator strengths, emission oscillator strengths, transition probabilities, fluorescence branch ratios, energy lifetimes, and integrated emission cross-sections are also derived. The photoluminescence spectra of Nd:GdVO₄ crystal consist of a wide emission band of host and the characteristic emission bands of Nd³⁺. Based on the excitation spectrum, both the two evident peaks locating at 345 and 371 nm are ascribed to the characteristic excitation of Nd³⁺, and an energy transfer from the host to its doping Nd³⁺ ions is indicated.     

Absorption of Dy3+ and Nd3+ ions in BaR 2F8 single crystals

The Dy³⁺ absorption and excitation spectra of BaY₂F₈ and BaYb₂F₈ single crystals are investigated in the ultraviolet, vacuum ultraviolet, and visible ranges at a temperature of 300 K. These crystals exhibit intense broad absorption bands due to the spin-allowed 4f-5d transitions in the range (56–78) × 10^?3 cm^?1 and less intense absorption bands that correspond to the spin-forbidden transitions in the range (50–56) × 10^?3 cm^?1. The Nd³⁺ absorption spectra of BaY₂F₈ single crystals are studied in the range (34–82) × 10^?3 cm^?1 at 300 K for different crystal orientations.     

The low-lying level structure of atomic lawrencium (Z = 103): energies and absorption rates

The low-lying level structure of atomic lawrencium has been calculated by using medium- to large-scale multiconfiguration Dirac-Fock wave functions. From these computations, an overview on the excitation energies and absorption rates is compiled for the 30 lowest levels of the neutral atom with regard to its 7s² 7p ²P_1/2 ^○ ground state. For many of these levels, an accuracy of ∼1200 cm^-1 is estimated by performing analogue computations for the homologous element lutetium. From the predicted level scheme, the excitation energies of about 15 levels fall into the spectroscopically relevant region between 20 000 and 30 000 cm^-1 and, hence, might help in the set-up and interpretation of forthcoming experiments on the resonant excitation of atomic Lr.     

Time-resolved UV absorption of polyimide

The 355-nm transient absorption of polyimide thin films has been measured following excitation withsubablative, 24-ps long, 355-nm laser pulses. The 355-nm absorption increases by 25% following 355-nm, 20 mJ/cm² excitation and recovers with a fast time constant 34 ps, and a slow time constant which is much longer than 6 ns. The data are fitted by a three-level rate equation model incorporating the temperature dependence of the ground state absorption coefficient. The fast component is attributed to the decay ofS ₁ and the slow component results from increased ground state absorption caused by a laser-induced temperature rise. The nonlinear intensity dependence is attributed to excited state (S ₁) absorption. These results indicate the importance of considering the dynamic absorption in modelling ablation.     

Dynamics and spectra of excited states of water-micellar suspensions of single-walled carbon nanotubes

The dynamics of the photoinduced differential absorption and excited-state bleaching spectra of single-walled carbon nanotubes suspended in a micellar solution were studied in the spectral range from 40 to 1000 nm within a time interval from 70 fs to 150 ps under excitation by 50-fs pulses with photon energies 2 and 4 eV. The bleaching and absorption bands were observed in the spectra; the positions of the bleaching peaks were independent of the photon energy of the exciting femtosecond pulse in the range 2–4 eV. It was established that, for delay times shorter than 1 ps, the shape of the differential spectrum of excited nanotubes coincided with the shape of the second derivative of the absorption spectrum of unexcited nanotubes in the frequency range of exciting pulse above 18000 cm^?1 (the range of absorption bands of metallic nanotubes). In the frequency range below 16000 cm^?1 (the range of absorption peaks of semiconducting nanotubes), the bleaching peaks in the differential spectrum of excited nanotubes undergo a high-frequency shift of 200–300 cm^?1 with respect to the second-derivative spectrum of unexcited nanotubes. The excited-state relaxation rate constants were measured. They are well approximated by the exponential dependences and depend on the probe-pulse wavelength. An assumption was made about the nature of the observed spectra of excited nanotubes and about the excitation relaxation.     

Pulsed photoconductivity in diamond upon quasi-continuous laser excitation at 222 nm at the formation of an electron–hole liquid

An order-of-magnitude enhancement of the pulsed photocurrent in a polycrystalline diamond sample synthesized by chemical vapor deposition is observed under the conditions of formation of an electron–hole liquid. Nonequilibrium charge carriers are excited by laser pulses at a wavelength of 222 nm with FWHM pulse duration of 18 ns and peak intensity above 2.5 MW/cm² upon cooling the sample to 90 K. For peak intensities of laser excitation lower than 1 MW/cm², sample cooling from 300 to 90 K leads to a decrease in pulsed photocurrent by about a factor of 5. The observed increase in pulsed photocurrent is attributed to the formation of the electron–hole liquid.     

Narrow resonances (Δv=2·10−2 cm−1) of multiple-photon IR absorption in ethylene

Narrow peaks of multiple-photon absorption in thev ₇ band of ethylene with the spectral width 0.02 cm⁻¹ and the contrast factor of up to 10² have been observed at the intensity of laser radiation 0.04 and 0.6 MW/cm². The multiple-photon spectra of ethylene in intense IR field have been studied with the use of a quasi-single-mode continuously tunable CO₂ laser. The results of the experiments are interpreted within the model of spepwise molecular excitation due to weak transitions.     

Far-infrared optical absorption due to surface phonon excitations in small metal particles

In this paper, the role played by the excitation of surface phonons in the far infrared optical absorption of small metallic spheres is explored. We find that for frequencies ranging between 100 cm^-3 and 200 cm^-1 this absorption mechanism is dominating over the ones coming from considering electronic excitations or the Joule heating.     

Changes in Structural and Optical Properties of Polycarbonate Induced by Ag+ Ion Implantation

Transparent polycarbonate samples were implanted with 1 MeV Ag⁺ ions to various doses ranging from 5 × 10¹⁴ to 3 × 10¹⁶ ions cm^?2 with a beam current density of 900 nA cm^?2. Modification in the structure of polycarbonate as a function of the implantation fluence was investigated using micro-Raman spectroscopy, glancing angle X-ray diffraction, and UV-Vis spectroscopy. Raman spectroscopy pointed toward the formation of graphite structures/clusters due to the ion implantation. UV-Vis absorption analysis suggests the formation of a carbonaceous layer and a drastic decrease in optical band gap from 4.12 eV to 0.50 eV at an implanted dose of 3 × 10¹⁶ ions cm^?2. The correlation between the decrease in band gap and the structural changes is discussed.