Luminescence detection of multiphoton ionization-fragmentation of the molecular CrO 4 2− anions adsorbed on the surface of dispersed SiO2

It is shown that luminescence detection of multiphoton ionization-fragmentation of the molecular CrO ₄ ²⁻ anions adsorbed on the surface of dispersed SiO₂ is possible under excitation with the fundamental frequency of a Nd:YAG pulsed laser (λ=1.064 μm). The structure and the process of formation of the adsorbed complexes under thermal activation of the surface and the nature of luminescence transitions in CrO ₄ ²⁻ anions are studied in detail. It is shown that luminescence is excited as a result of the recombination of photoelectrons and ionized chromate ions. Multiphoton ionization of the ions occurs under three-photon resonance conditions. The resonance level is an antibonding state of the adsorption complex formed with the participation of an oxygen vacancy on the SiO₂ surface. The dynamics of the multiphoton luminescence excitation process includes autoionization (stimulated by intercomplex electronic excitation) in superexcited states, fragmentation of chromate anions, and annealing of surface oxygen vacancies. The rate equations for three-photon-resonance multiphoton ionization are studied. The cross sections for two-and one-photon transitions on the nonresonance steps of multiphoton absorption are obtained. It is concluded that the nonlinear polarizability of the donor-acceptor adsorption bond in “chromate anion-oxygen vacancy” complexes is very important. Zh. éksp. Teor. Fiz. 111, 1748–1774 (May 1997)     

Isotopic selectivity of IR laser photodissociation of CF3I molecules

The selectivity dependence of multiphoton dissociation of CF₃I on the conditions of excitation (pulse duration, concentration of the isotope under excitation and gas pressure) has been studied. It has been shown that the main mechanism of selectivity loss isV-V exchange during a laser pulse. The elaborated model is in good agreement with the experiment.     

用受激拉曼泵浦方法高效制备v=2振动激发态氘分子

We report the preparation of D₂ molecules in v=2 level in molecular beam condition. A single longitudinal mode laser system was used for excitation of D₂ from (v=0, j=0) to (v=2, j=0) with the scheme of stimulated Raman pumping. An excitation efficiency of 25.2% has been achieved, which was determined by the scheme of resonance-enhanced multiphoton ionization. Dependence of relative excitation efficiency on laser energy has been measured. We found that the increasing rate of excitation efficiency became slower as pulse energy of Stokes laser increase, while the excitation efficiency still increases approximately linearly with pump pulse energies up to 60 mJ. The spectral line shapes of Raman transition was also measured at different laser energies and considerable dynamical Stark effect was observed. A single peak was found on the three dimension surface of relative excitation efficiency, indicating the process occurred in the present study is a process of stimulated Raman pumping instead of stimulated adiabatic Raman passage.     

PbWO<Subscript>4</Subscript> crystal for laser energy accumulation and transformation

The picosecond interband two-photon laser excitation of PbWO₄ crystals at a temperature of 10 K leads to electronic excitation energy accumulation, which results in almost 100% induced absorption in the 450–750 nm spectral range. The relaxation time of this induced absorption exceeds 100 min. The electronic excitation energy accumulated in the PbWO₄ crystal at T = 10 K excites the intrinsic luminescence with a decay time longer than 45 min. The decay kinetics and the spectra of the intrinsic luminescence of the PbWO₄ crystal at a temperature of 10 K were measured under two-photon and single-photon excitation. The luminescence under two-photon and single-photon excitation revealed a difference in the structure of the spectra.     

Analysis of Gain Volume in Random Laser in a Spherical Multiple Scattering Medium

We performed numerical simulation of a random laser in a spherical multiple scattering medium in order to examine the saturation absorption in the excitation process and the resultant increasing process of the gain volume under the random laser action. The size of the gain volume increases with 1/3 power of the excitation pulse energy in the weak excitation region, and then approaches a critical value L_th when the excitation pulse energy is increased above the threshold. The dependence of L_th, as well as the dependence of the threshold excitation pulse energy on the dye concentration, transport mean free path, stimulated emission cross section and excited state lifetime were also examined. These results of the simulation well correspond to the experimental results by a two-beam spatial-correlation method.     

Relaxation Processes at High Levels of Vibrational Excitation of Polyatomic Molecules in the Ground Electronic State

By the spectral and kinetic characteristics of the luminescence of vapors of polyatomic molecules (anthracene, anthraquinone, fluorenone) initiated by selective IR multiphoton excitation (IR MPE) of molecules in the ground electronic state S ₀ the relaxation processes proceeding under vibrational excitation of molecules to energies exceeding the energies of the lower excited electronic states have been investigated. The changes in the spectral and kinetic characteristics with increasing CO₂ laser energy density and vapor P _v and foreign gas pressure P _FG are analyzed. They are similar to the characteristics obtained for normal fluorescence of these molecules with changing vibrational energy E _vib content. On the basis of experimental data and model calculations it has been concluded that at the laser radiation densities used in the case of IR MPE the molecules reach energies considerably exceeding the energies of the electronic levels. It is shown that a nonadiabatic connection between the electronic states leads to the population of mixed electronic states isoenergetic to the vibrational levels of the ground electronic state and to emission of delayed luminescence spectrally identical to the normal luminescence of these molecules. It has been found that when high vibrational levels are populated, new relaxation channels, such as reverse electron relaxation, emission from high vibrational levels of the ground electronic state, and multiquantum vibrational energy transfer at collisions leading to a rapid establishment of vibrational equilibrium become important.     

Energy transfer and thermalization in LiYF4:Tm, Ho

Energy transfer processes are very important in solid-state laser systems because they can cause an enhancement of the luminescence emission resulting in a reduction of the laser threshold. In this work, a detailed investigation to understand the basic processes of energy transfer between Tm and Ho ions in LiYF₄, a solid-state laser crystal, was made. Data includes absorption, luminescence excitation and response to pulsed excitation. Dynamics of the energy transfer was analyzed by considering the kinetic evolution of the emissions of both ions. It was found that the energy transfer process between the ³ F ₄ spectral manifold of Tm and the ⁵ I ₇ spectral manifold of Ho results in thermal equilibration of these two manifolds. Received: 20 May 1999 / Revised version: 20 August 1999 / Published online: 27 January 2000     

Efficient multiphoton-absorption-induced luminescence in single-crystalline ZnO at room temperature

At room temperature, multiphoton absorption- (MPA-) induced photoluminescence in ZnO strongly driven by a femtosecond (fs) near-infrared laser is studied. Two-photon absorption and three-photon absorption are proved to be responsible for the intense luminescence, when the wavelength of the fs excitation laser is above and below the half-bandgap of ZnO, respectively. Strong MPA absorption in ZnO is unambiguously evidenced by the interferometric autocorrelation measurements of the luminescence signal.     

Multiphoton Excitation and Ionisation in the 9–12 eV Region of O2 by a 1.06 μm Glass Laser

In this letter we report results of a selective multiphoton excitation of O₂ in the 9–12 eV region by a neodymium glass laser. The main feature of this experiment is the major presence of the ion specie O₂+ in the interaction volume with the values 10 ± 1 for the nonlinear interaction order. This result can be interpreted as a double mechanisms namely: a one step process, the direct absorption from the ground state or a two step process via an intermediate resonant state which has been attributed as the second (B′³Σ_u^?, v′=2) state of O₂ located at 10.56 ± 0.03 eV. The probability of multiphoton formation of O₂⁺ for a flux value of 1,5 × 10¹² W/cm² is equal to 2 × 10^7±1 sec^?1.     

Atomic and molecular ions in intense ultra-fast laser fields

The interaction of a 60 fs 790 nm laser pulse with beams of Ar⁺, C⁺, H₂ ⁺, HD⁺ and D₂ ⁺ are discussed. Intensities up to 10¹⁶ Wcm^-2 are employed. An experimental z-scanning technique is used to resolve the intensity dependent processes in the confocal volume.Received: 6 January 2003, Published online: 15 July 2003PACS: 32.80.Fb Photoionization of atoms and ions - 33.80.Rv Multiphoton ionization and excitation to highly excited states (e.g., Rydberg states) - 42.50.Hz Strong-field excitation of optical transitions in quantum systems; multiphoton processes; dynamic Stark shift     

Nonlinear light absorption and luminescence in silicate glasses

The study of luminescence of high-purity multicomponent silicate glasses excited by radiation of a N₂ laser (λ=337 nm, P≈12kW) showed darkening of a sample and a monotone decrease in luminescence intensity and the transmitted radiation intensity from pulse to pulse. Additional illumination with radiation of an Ar⁺ laser (λ=514.5 nm) caused an increase in luminescence intensity. An increase in absorption and a decrease in luminescence intensity were found to be caused by two-photon absorption and electron-hole pair production.     

Enhanced luminescence of silver nanoclusters in mesoporous film

Luminescence of silver nanoparticles photodeposited on titan dioxide nanoparticles of mesoporous film is studied. Luminescence was registered under the two-photon excitation by femtosecond laser pulses of Ti:sapphire laser. It occurs that Ag/TiO₂ mesoporous films have high concentration of bright luminescence spots which reveal stability to degradation under long illumination. Various configurations of silver nanoparticles are analyzed to explain the physics of bright luminescence spots (“hot spots”). Luminescence intensity reveals “hot spots” dependence on excitation laser pulse polarization. Properties of Ag/TiO₂ system show its promising usage for single molecule spectroscopy and biological objects visualization.     

Selective excitation of the luminescence of a polymer film at room temperature

Selective laser excitation of the luminescence of a thin film of the π-conjugated polymer poly(p-phenylene) at room temperature is achieved. Monochromatic excitation is selective only for excitation in the long-wavelength wing of the absorption spectrum. This is manifested as a shift of the luminescence spectrum with excitation frequency. The experimental results are interpreted on the basis of model calculations. Pis’ma Zh. éksp. Teor. Fiz. 63, No. 3, 171–175 (10 February 1996)     

The absorption of pulsed CO2-laser radiation by tetrafluorosilane at various wavenumbers,fluences, pulse durations,temperatures, optical path lengths and pressures of absorbing and non-absorbing gases

The absorption of three linesP(30) (1037.4 cm^–1),P(36) (1031.5 cm^–1) andP(40) (1027.4cm^–1) of the pulsed CO₂ laser (00⁰1–02⁰0 transition) by SiF₄ was examined at various pulse energies, pulse durations, temperatures, optical path lengths and pressures of this compound and several non-absorbing gases. In addition, the low-intensity infrared absorption spectrum of tetrafluorosilane was compared with high-intensity absorption data for all lines of the laser. The experimental dependences demonstrate nonlinear features of the absorption phenomena originating from the high power of the incident radiation and collisions of absorbing molecules with surroundings. These effects are included in the analytical formula, being an extended form of the Lambert-Beer law. which reasonably approximates all experimental data. The importance of the results obtained for understanding general features of multiphoton absorption and for revealing potential applications of SiF₄ as a sensitizer for the infrared region is presented in brief.     

Spectral dependent kinetics of the EHD luminescence in As-doped Ge

Following pulsed laser excitation of As-doped Ge with impurity concentrations between 10¹⁵-10¹⁷cm^-3, we observe the electron-hole drop (EHD) and excitonic luminescence decay. The spectrum resolved no-phonon (NP) EHD luminescence kinetics are found to depend on its spectral position. “Plateaus” on the kinetic curves for the high energy side of NP-spectrum are observed at high excitation. The data suggest this luminescence is due to the states which are in dynamical equilibrium during some time after excitation pulse.     

Luminescence decay of rare earth ions in an orthophosphate matrix

Abstract

Investigations of the luminescence decay of Ce³⁺- and Tb³⁺-ions in solid solutions of the system K₃La_1?x?yCe_xTb_y(P0₄)₂ were carried out at 298 K and 10 K using a laser pulse spectrometer or synchrotron radiation as excitation sources. A comparison of the decay times determined in the host absorption range (160 nm) and in the Ce³⁺- and Tb³⁺- ion levels shows a delayed decay of the host excitation. The results are discussed in regard to energy transfer.     

Dynamics of optical response of solutions of pseudoisocyanine <Emphasis Type="Italic">J</Emphasis> aggregates upon pico- and subnanosecond excitation

The luminescence kinetics of solutions of pseudoisocyanine iodide (PIC) J aggregates is studied upon excitation by pico- and subnanosecond laser pulses into the main superintense long-wavelength absorption band. The dependences of the transmission and luminescence energy on the pump energy are measured. It is found that the shape of the luminescence kinetics depends on the recording and excitation spectral regions, which is obviously related to the energy transfer between coherently coupled fragments of J aggregates.     

Direct measurement of multiphoton molecular absorption of IR laser radiation by pyroelectric detector

The applicability of a pyroelectric detector (PED) to multiphoton absorption measurements (MPA) under ir laser excitation of molecules was examined. The possibility of MPA measurement of SF₆ molecules in the pressure range of 10⁻³÷10⁻¹ Torr with a time resolution of ∼ 7 μs has been shown. It has been demonstrated that the degree of vibrational relaxation of highly vibrationally excited molecules at PED surface does not depend on excitation level under the studied conditions.     

TiO2∶Mo体系的光子雪崩上转换

在978nm激光二极管的激发下，Mo掺杂的TiO₂材料表现出很强的宽带上转换发光 ，该发光来源于［MoO₄］^2-基团的激发态³T₁, ³T₂能级到基态¹A₁能级的电子跃迁.通过研究发光强度与抽运功率的关系及上转换发光的上升时间曲线，发现TiO₂∶Mo体系的上转换发光中存在着雪崩机制，应用转 关键词： 上转换 光子雪崩 转移函数理论     

Polarization dependence of luminescence induced by two-photon excitation in LiF crystals with F 3 + laser color centers and the symmetry of the excited state

The energy level structure of F ₃ ⁺ laser color centers in crystals of LiF is discussed. A high-power laser (λ _ex=920 nm) is used to excite luminescence from LiF crystals with F ₃ ⁺ centers via two-photon absorption, and the dependence of the polarization and intensity of this luminescence on the polarization of the laser light is measured and calculated. It is shown that the two-photon transition involves the excitation of a previously unknown state of the F ₃ ⁺ center—a spin singlet whose wave function has ¹ A ₁ symmetry. Fiz. Tverd. Tela (St. Petersburg) 39, 1373–1379 (August 1996)