Kinetics of the Excited States of Helium in an Atmospheric-Pressure Glow Discharge in a Helium-Nitrogen Mixture

Using an atomic-absorption spectral analysis technique, we determined the concentrations of helium atoms in states 2¹S, 2¹P, 2³S, and 2³P in an atmospheric-pressure glow discharge in helium (99.98%) and in a mixture of helium with nitrogen (99.5%He+0.5%N₂). It is shown that the population of the lower excited levels of helium atoms (n = 2) in its mixture with nitrogen is almost an order of magnitude smaller than in the case of a discharge in helium. The maximum of the concentration of excited atoms in a discharge both in helium and in its mixture with nitrogen is in the cathode region at a distance of about 0.1 mm from the cathode. The reaction of quenching of excited helium atoms by nitrogen molecules is responsible for the sharp decrease in the concentration of He(n = 2) on addition of nitrogen into helium. Presented at the 5th Symposium on Physics and Diagnostics of Laboratory and Astrophysical Plasmas, Belarus, Serbia and Montenegro, Minsk, Belarus, September 20–23, 2004; 12th International Congress on Plasma Physics, October 25–29, 2004, Nice, France. __________ Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 72, No. 4, pp. 530–537, July–August, 2005.     

The quenching of Pb(6p 2 1 D 2) atoms in collisions with molecules

The collisions of metastable Pb(6p ^{2 1} D ₂) atoms with various molecules were studied by the diagnostics of radiation from a hollow cathode lamp and a laser on lead vapor. Experiments were performed for a gas flow of lead atoms with argon. The Pb(6p ^{2 1} D ₂) states were excited in a gas discharge in the presence of reagent gas molecules. The absolute rate constants for the quenching and chemical reactions of lead atoms in the ground and excited states were determined. The quantum efficiency of chemical reactions was close to one for the N₂O, CH₂Cl₂, SF₆, and CuBr molecules. Long-lived chemical compounds were formed in these reactions.     

Multiphoton ionization of iodine atoms and CF<Subscript> 3</Subscript>I molecules by XeCl laser radiation

We report about effective ionization of iodine atoms and CF₃I molecules under the action of intense XeCl laser radiation (308 nm). The only ion fragment resulting from the irradiation of the CF₃I molecules is the I⁺ ion. We have studied the influence of the intensity, spectral composition, and polarization of the laser radiation used on the intensity of the ion signal and the shape of its time-of-flight peak. Based on the analysis of the results obtained, we have suggested the mechanism of this effect. The conclusion drawn is that the ionization of the iodine atoms by the ordinary XeCl laser with a nonselective cavity results from a three- (2 + 1)-photon REMPI process. This process is in turn due to the presence of accidental two-photon resonances between various spectral components of the laser radiation and the corresponding intermediate excited states of the iodine atom. The probability of ionization of the atoms from their ground state I(²P_3/2) by the radiation of the ordinary XeCl laser is more than two orders of magnitude higher than the probability of their ionization from the metastable state I^*(²P_1/2). The ionization of the CF₃I molecules by the XeCl laser radiation occurs as a result of a four-photon process involving the preliminary one-photon dissociation of these molecules and the subsequent (2 + 1)-photon REMPI of the resultant neutral iodine atoms.     

Photophysics ofβ-carotene and related compounds (review)

A review of data on the photophysics of carotenoids is presented. Results of investigations of spectroscopic, temporal, and energy parameters of excited S₁ and S₂ singlet states of β-carotene and related compounds are critically examined. These states give rise to extremely high probabilities (10¹¹–10¹³ sec⁻¹) of radiationless deactivation of the electronic excitation energy in carotenoids. Results of investigations of photophysical properties of triplet states of carotenoids are considered mainly from the standpoint of quenching of singlet oxygen and triplet states of organic molecules by carotenoids. Institute of Molecular and Atomic Physics, Academy of Sciences of Belarus, 70, F. Skorina Ave., Minsk, 220072, Belarus. Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 64, No. 1, pp. 5–19, January–February, 1997.     

Influence of the Stark effect on multiphoton ionization of atoms when the dynamic polarizability depends strongly on the laser frequency

The influence of the Stark effect on multiphoton ionization of Ba atoms under conditions when the dynamic polarizability depends strongly on the frequency of the laser radiation is investigated. It is found that for some electric field strengths ε of the laser radiation this effect gives rise to resonance peaks in the Ba⁺ ion yield as a function of the laser radiation frequency at frequencies corresponding to single-photon transitions between the excited states. These frequencies can differ substantially from the frequencies corresponding to the conventional multiphoton excitation of these states from the ground states of the atoms. Peaks in the ion yield as a function of ε behave differently from the conventional Stark effect—their position on the frequency scale does not depend strongly on ε. The conditions under which such an induced resonance structure appears are determined. Zh. éksp. Teor. Fiz. 113, 499–512 (February 1998)     

Spectral-time characteristics of combined-target laser plasma

From the analysis of the contours of the spectral lines of target-material atoms, the electron and atomic concentrations and their variation with time are determined in the laser plasma of a combined Cu–Al–Cu target. The time dependences for the concentrations of electrons and atoms in the ground and excited states are explained within the framework of a model that allows for plasma decay being determined by processes of three-particle recombination and ionization as well as by the variation in the particle concentration in plasma expansion. Institute of Molecular and Atomic Physics, National Academy of Sciences of Belarus, 70, F. Skorina Ave., Minsk, 220072, Belarus. Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 65, No. 3, pp. 426–432, May–June, 1998.     

Dynamics of erosion plasma formation and formation of a plasma flame with a condensed disperse phase when quasi-continuous laser radiation acts on bismuth

The dynamics of near-surface plasma formation and the formation of an erosion plasma flame was investigated for quasi-continuous laser radiation (λ=1.06 μm, q=0.1–10 MW/cm², τ∼1.5 msec) acting on bismuth targets in air. The absence of low-threshold plasma formation at q<2 MW/cm² was established and explained. Instabilities in the plasma formation were revealed and the range of laser radiation power densities (2≤q≤4 MW/cm²) at which these instabilities take place was determined. At q≥5.4 MW/cm², brightening of the flame was noted. The dependence of the luminescence temperature of the flame on the laser radiation power density q was determined. Institute of Molecular and Atomic Physics, National Academy of Sciences of Belarus, 70, F. Skorina Ave., Minsk, 220072, Belarus. Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 65, No. 1, pp. 126–133, January–February, 1998.     

Intramolecular photoinduced electron transfer in Pd-porphyrin-quinone in the picosecond time range

Photoinduced electron transfer (PET) was studied in toluene solutions of the Pd-porphyrin-quinone (Pd-PQ) dyad by flash photolysis in the picosecond time range and by a luminescence method. It is found that Pd-PQ has a high rate of intercombination conversion K_isc=(7.7±0.2)·10¹⁰ sec⁻¹. Competing intramolecular PET occurs from the lower excited singlet state of the dyad with the rate constant K _et ^s =(2.7 ±0.3)·10¹⁰ sec⁻¹. Therefore, ∼74% of excited molecules from the dyad make a transition to the triplet T₁ state and 26% take part in intramolecular PET resulting in formation of radical products. The radical products relax to the ground state with the rate constant K=(7.4±0.2)·10⁹ sec⁻¹. Institute of Molecular and Atomic Physics of the National Academy of Sciences of Belarus, 70, F. Skorina St., Minsk, 220072, Belarus. Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 66, No. 1, pp. 11–18, January–February, 1999.     

Kinetics of triplet-triplet absorption of anionic water-soluble porphyrins

It was established that in aqueous solutions of anionic porphyrins the processes of triplet-triplet (T-T) annihilation are absent (K₂<2.5·10⁵ M⁻¹ sec⁻¹), while a delayed annihilation fluorescence can be detected for these porphyrins in methanol (K₂≊3.5·10⁷ M⁻¹ sec⁻¹) and for their lipophilic analogs in organic solutions (K ₂≊2.5·10⁹ M⁻¹ sec⁻¹), and the kinetics of absorption of the latter porphyrins in triplet states is dependent on the intensity of the exciting radiation. The extremely small constant of T-T annihilation of anionic porphyrins can be due to the formation of a relatively dense solvate shell consisting of water molecules around the charged groups of the porphyrin molecules, which increases steric barriers and thus prevents an exchange-resonance transfer of energy between triplet excited molecules in aqueous solutions. It is also shown that porphyrin molecules can electrostatically repel one another when in their structure there are charged groups. To whom correspondence should be addressed. Deceased. Institute of Molecular and Atomic Physics, National Academy of Sciences of Belarus, 70 F. Skorina Ave., Minsk, 220072, Belarus; e-mail: llum@imaph.bas-net.by. Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 66, No. 6, pp. 791–795, November–December, 1999.     

Adaptive Correction of a High-Power Titanium-Sapphire Laser Radiation

An adaptive optical closed-loop feedback system based on a phase-conjugation algorithm has been developed and investigated. It includes a deformable bimorph mirror and a Shack-Hartmann wavefront sensor. This system was used to improve the radiation focusing in an ultrashort-pulse laser designed for basic research in the field of high-energy physics. With the indicated system, the power density of 10-TW radiation pulses in the focal plane of a Ti:Al₂O₃ laser reached 4 ⋅ 10¹⁹ W/cm². Report at the Fifth International Scientific and Technical Conference “Quantum Electronics,” November 22–25, 2004, Minsk, Belarus. __________ Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 72, No. 5, pp. 678–683, September–October, 2005.     

Optical measurement of <Superscript>3</Superscript>He nuclear polarization for metastable exchange optical pumping studies at high magnetic field

An accurate optical method to measure the nuclear polarization of ³He atoms in the 1¹S ground state is described. The absorption of a weak, probe laser beam is used to measure the relative populations of two hyperfine sublevels of the 2³S metastable state that are not addressed by the pumping laser beam. Since a common spin temperature between the ground and metastable states is established by metastable exchange collisions, the nuclear polarization can be derived from these absorption measurements. The method is highly sensitive, robust, and can be used to monitor the dynamics of optical pumping and relaxation processes without interfering with them. It was successfully implemented and tested in the 0.45–2.0 T magnetic field range at the ³He gas pressure up to 67 mbar.     

Spectral Analysis for Systems of Atoms and Molecules Coupled to the Quantized Radiation Field

We consider systems of static nuclei and electrons – atoms and molecules – coupled to the quantized radiation field. The interactions between electrons and the soft modes of the quantized electromagnetic field are described by minimal coupling, p→p−e A (x), where A(x) is the electromagnetic vector potential with an ultraviolet cutoff. If the interactions between the electrons and the quantized radiation field are turned off, the atom or molecule is assumed to have at least one bound state. We prove that, for sufficiently small values of the fine structure constant α, the interacting system has a ground state corresponding to the bottom of its energy spectrum. For an atom, we prove that its excited states above the ground state turn into metastable states whose life-times we estimate. Furthermore the energy spectrum is absolutely continuous, except, perhaps, in a small interval above the ground state energy and around the threshold energies of the atom or molecule. Received: 3 September 1998 / Accepted: 17 March 1999     

Infrared multiphoton excitation of polyatomic molecules

Results of investigations of the process of multiphoton excitation of polyatomic molecules by CO₂-laser radiation are presented. The mechanism of formation of the profiles of IR absorption bands of polyatomic molecules is discussed. New experimental methods of investigation of relaxation processes at high levels of vibrational excitation of molecules in the ground and triplet states are considered. For vapors of polyatomic molecules and their mixtures with foreign gases, the quantitative characteristics of the collisional exchange and the vibrational-energy transfer as well as the rates of intercombinational conversion ⇛ and triplet-triplet transfer are presented and their dependences on the vibrational-excitation level are discussed. Institute of Molecular and Atomic Physics of the National Academy of Sciences of Belarus, 70, F. Skorina Ave., Minsk, 220072, Belarus. Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 65, No. 5, pp. 675–693, September–October, 1998.     

Spectroscopic diagnostics of the laser erosion plasma of an AgGaS<Subscript>2</Subscript> polycrystalline target

Results are presented from experimental studies of the radiation emitted from a plasma produced in vacuum after irradiating a polycrystalline target by 1.06-μm laser radiation with an intensity of (3–5)×10⁸ W/cm². Plasma radiation from regions located at distances of 1 and 7 mm from the target is analyzed. It is shown that the main contribution to the plasma radiation in the 220–600 nm spectral range is made by transitions from the excited states of single-charged Ag⁺ and S⁺ ions. The atomic component of plasma radiation is represented by intense spectral lines corresponding to transitions from the Rydberg states of Ag and Ga atoms, whereas no resonance lines of these atoms are observed.     

Anti-stokes luminescence of Zn<Subscript>0.6</Subscript>Cd<Subscript>0.4</Subscript>S solid solutions with adsorbed organic dye molecules and few-atom silver clusters

For microcrystals of Zn_0.6Cd_0.4S with adsorbed molecules of a number of organic dyes, we have observed sensitized anti-Stokes luminescence excited by radiation with wavelengths in the range 610–750 nm and flux density 10¹⁴–10¹⁵ photons/cm²·sec. The positions of the bands in the excitation spectra for such luminescence match those of the absorption spectra for the adsorbed dye molecules, which is evidence in favor of a cooperative mechanism for its appearance. We have shown that enhancement of the anti-Stokes luminescence is possible when silver atoms and few-atom clusters appear on the Zn_0.6Cd_0.4S surface in addition to the dye molecules. We hypothesize that its excitation in the latter case occurs as a result of two-photon optical transitions. These transitions occur sequentially, with transfer of an electron or the electronic excitation energy from the dye molecules to silver atoms and few-atom clusters adsorbed on the surface of Zn_0.6Cd_0.4S, creating deep localized states in the bandgap with photoionization energies 1.80–2.00 eV. __________ Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 74, No. 5, pp. 617–621, September–October, 2007.     

Optical properties of new indotricarbocyanine dye as a limiter of laser radiation power

We present results of experimental and theoretical studies of the optical characteristics of a new indotricarbocyanine dye that is capable of effectively limiting the power of laser radiation in the visible spectral range. The spectral-luminescent and energy characteristics of the dye molecules and their absorption spectra from the excited state with nanosecond resolution are investigated experimentally. Quantum-chemical methods are used to calculate electronic absorption spectra from the ground (S₀ → S_n) and excited (S₁ → S_n) states and to determine the nature of electronic states of the molecule and the rate constants of intramolecular photophysical processes. The results of the theoretical research agree with experimental data. It is shown that the investigated dye has singlet-singlet absorption at 400–600 nm. Nonlinear absorption of the dye upon excitation by radiation of the second harmonic of a Nd:YAG laser is studied by z-scanning with an open diaphragm. The ratio of dye absorption cross sections from the excited and ground states at 532 nm is determined in the framework of a three-level model. The results are compared with those for previously studied compounds. __________ Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 74, No. 4, pp. 473–480, July–August, 2007.     

Analysis of the production and clusterization of iron atoms under pulsed laser photolysis of Fe(CO)5

Atomic-resonance absorption spectroscopy is used to study the production and loss of iron atoms under dissociation of the Fe(CO)₅ vapor in a quartz reactor that is induced by the pulses of the KrF excimer laser. Iron atoms populate the ground state owing to the quenching of the excited states generated in the course of the laser photolysis and are detected using the resonance absorption at a wavelength of 385.99 nm. The effective quenching rates are in good agreement with the known rates of the quenching of metastable iron atoms by the Fe(CO)₅ molecules. It is demonstrated that a loss of iron atoms is related to the recombination with dimer and trimer formation and the secondary atomic reactions with the Fe(CO)₅, CO, and FeCO molecules. The rates of the main elementary reactions responsible for the loss of iron atoms are determined using the comparison of the experimental results and kinetic simulation data.     

Multilevel rotational transitions in the intermediate stage of three-photon ionization of molecules

Ionization and dissociation of diatomic molecules induced by a weak field (after preliminarily populating an intermediate level) and by intense, linearly polarized monochromatic radiation have been studied. Field-induced mixing of rotational components of various electronic-vibrational states of molecules (such as CO, NO, etc.) at field strength f∼10⁻⁴–10⁻⁵ atomic units can lead to migration among states with different angular momenta J. Therefore, ions with rotational momenta J ⁺ much higher than those prescribed by selection rules for three-photon absorption can be formed from molecules in the ground state. The possibility of selective formation of ions with J ⁺≫1 and zero projection of the angular momentum on the polarization vector of the external electromagnetic radiation has been investigated. Zh. éksp. Teor. Fiz. 111, 1624–1632 (May 1997)     

Shaping dynamics and structure of large-scale surface plasma formations under single-pulse laser action on various materials

It is established that, in the case of laser action on materials in large illuminated spots in atmospheric-pressure air for a laser radiation power density q≤2 MW/cm² (λ=1.315 μm), an evaporative regime with plane scattering of the laser-produced erosion plasma is realized while, for q≈5–17 MW/cm², the plasma front is transferred to the air, leading to plasma screening of the target and shaping of a subsonic radiation wave in the air. As the duration of the laser pulses increases (τ∼160 μsec), in spite of the large illuminated spots (S∼150 cm²) the evaporative regime of the laser action with plane plasma scattering goes over into a regime with jet outlow and formation of a quasistationary shock wave. Deceased. Institute of Molecular and Atomic Physics, National Academy of Sciences of Belarus, 70, F. Skorina Ave., Minsk, 220072, Belarus. Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 65, No. 2, pp. 261–268, March–April, 1998.     

The excitation cross section of cadmium atoms from metastable 5<Emphasis Type="Italic">s</Emphasis>5<Emphasis Type="Italic">p</Emphasis><Superscript>3</Superscript><Emphasis Type="Italic">P</Emphasis><Subscript>0, 2</Subscript> states by electron impact

By means of the optical method using the technique of crossed electron and atomic beams, we obtained the absolute values of the excitation cross sections of metastable cadmium atoms and their energy dependences. The absolute cross section values reach ∼10⁻¹⁶ cm² (at 30 eV). Sharp resonance-like maxima are observed in the energy dependences of the excitation cross section near the excitation thresholds, which are supposedly related to the formation and decay of negative-ion excited states of.