Color center production by femtosecond-pulse laser irradiation in fluoride crystals

Color centers are lattice vacancy defects trapping electrons or holes. They are easily created in single crystals by irradiation with ionizing radiation. We report the production of color centers in LiF and LiYF₄ single crystals by ultrashort high-intensity laser pulses (60 fs, 12.5 GW). An intensity threshold for color center creation of 1.9 and 2 TW/cm² was determined in YLF and LiF, respectively, which is slightly smaller than the continuum generation threshold. Due to the high energy density of the coherent radiation of the focused laser beam, we were able to identify a large amount of F centers, which gave rise to aggregates such as F₂, F ₂ ⁺ , and F ₃ ⁺ . The proposed mechanism of formation is based on multiphoton excitation, which also produces short-lived F ₂ ⁺ centers. It is also shown that it is possible to write tracks in the LiF crystals with dimensional control.     

A method for studying the multipolarity and orientation of elementary oscillators in cubic crystals on the basis of axially periodic dependence of the luminescence intensity

A new method for determining the multipolarity and orientation of elementary quantum oscillators in cubic crystals is proposed. This method is based on studying the spatially periodic dependences of the intensity of luminescence observed in crystals with an induced anisotropy. The method was experimentally verified on LiF crystals containing F ₂ and F ₃ ⁺ color centers. It is shown that the observed spatially periodic dependences are in good agreement with the calculated dependences. The proposed method supplements the known methods for studying polarized luminescence (the methods of azimuthal dependences and polarization ratios and their various modifications). However, the new method, in contrast to the known ones, does not require measurements of the polarization ratios (for example, the degree of luminescence polarization), which in some cases significantly simplifies the experiment. Another advantage of the proposed method is its universality; i.e., it can be applied with equal success to both anisotropic and cubic crystals.     

Radioluminescence of ionized electron color centers in LiF crystals

Photoluminescence (PL) and temporal variation of optical absorption and radioluminescence (RL) of LiF crystals after irradiation with an electron impulse are investigated by pulse spectrometry methods using different irradiation regimes and different degrees of initial radiation damage. The difference in the RL and PL characteristics of ionized F ₂ ⁺ and F ₃ ⁺ centers is revealed. Several mechanisms for inducing these centers by irradiation, which differ in energy and kinetic parameters and in temperature dependence, are proposed. It is established that the ionized centers in the radiation active state are created due to the interaction of the respective neutral centers with holes of different thermalization extent. A mechanism for the excitation of these radiation-active centers is proposed.     

Electronic color centers in SrF2-Na crystals

It was shown that optical bleaching of M _A ⁺ color centers at 80 K in SrF₂-Na crystals causes the core of an M _A ⁺ -center to transform into the V _a ⁺ Me ⁺ V _a ⁺ configuration, in which all three point defects are arranged diagnonally in the cube cell. Reirradiation of an optically bleached crystal by x-rays generates F _D centers in it: V _a ⁺ Me ⁺ V _a ⁺ + e ^? → V _a ⁰ Me ⁺ V _a ⁺ ≡ F _D. The F _D → M _A ⁺ transformation in SrF₂-Na crystals proceeds at T = 135 K, in contrast to the F _A → M _A ⁺ transformations, which take place at T > 200 K.     

Luminescence centers in silicate and germanate glasses activated by bismuth

Concentration series of silicate and germanate glasses activated by bismuth are studied. It is shown that luminescence in the IR region is controlled by several active centers related to bismuth. Based on a comparison of spectroscopic characteristics of the studied glasses with the data previously obtained for chloride glass, the observed centers were identified as Bi⁺, Bi ₂ ⁴⁺ , and Bi ₅ ³⁺ in germanate glass and Bi⁺, Bi ₂ ⁴⁺ in silicate glass.     

Luminescence of Sc3+ and La3+ isoelectronic impurities in Lu3Al5O12 single-crystal films

The time-resolved luminescence and luminescence excitation spectra, and luminescence decay kinetics at 8 and 300 K of Lu₃A₁₅O₁₂ (LuAG) single-crystal films doped with Sc³⁺ and La³⁺ isoelectronic impurities and excited by synchrotron radiation are investigated. It is established that the La³⁺ isoelectronic impurity in the ?ub;c?ub; positions of the garnet lattice forms La _Lu ³⁺ luminescence centers emitting in the band with λ_max = 280 nm and the decay time of the main component τ = 300 ns at 300 K. The Sc³⁺ isoelectronic impurity located in the ?ub;c?ub; and (a) positions of the LuAG lattice forms two luminescence centers, Sc _Lu ³⁺ and Sc _Al ³⁺ , emitting in the bands with λ_max = 290 nm and τ = 240 ns and λ_max = 335 nm and τ = 375 ns, respectively, at 300 K. It is shown that the luminescence excitation of the La³⁺ and Sc³⁺ isoelectronic impurities in LuAG single-crystal films occurs through radiative decay of excitons localized near La _Lu ³⁺ , Sc _Lu ³⁺ , and Sc _Al ³⁺ centers. The energies of formation of these excitons are determined to be 6.8, 6.88, and 7.3 eV, respectively. It was found that the excited state of the excitons genetically related to the La _Lu ³⁺ , Sc _Lu ³⁺ , and Sc _Al ³⁺ enters has two radiative levels with different transition probabilities. This configuration leads to the presence of fast (2.3–8.4 ns) and slow (150–375 ns) main components in the luminescence of the centers formed by isoelectronic impurities in garnets.     

Control of radiation spatial coherence under synchronous amplification in crystalline LiF:F 2 − amplifier

A technique of spatial coherence control, based on the synchronous amplification of a radiation in LiF crystals with F ₂ ^? color centers, is demonstrated. Spatial radiation distributions of stimulated Raman scattering (SRS) in oxide crystals were investigated under picosecond laser excitation. Low spatial radiation coherence was revealed for both the transient and quasi-stationary SRS. Spatially incoherent SRS was transformed to spatially coherent radiation as a result of phase—locked picosecond synchronous laser pumping of nonlinear Raman and LiF: F ₂ ^? crystals and the Stokes radiation amplification in the color center crystal.     

Relaxation processes in colored crystals of LiF after the coaction of UV radiation and a shock wave

The relaxation of F ₂ ⁺ centers in radiation-colored crystals of lithium fluoride starting from the moment of the coaction of pulsed UV irradiation and a shock wave is investigated. It is shown that the annealing curve of these centers displays a nonmonotonic character at room temperature and is a consequence of three + processes. The first two are the processes of disintegration of unstable (short-lived) and stable F ₂ ⁺ centers, and the third process involves the formation of stable centers upon a random encounter of appropriate constituents in the course of their diffusive wandering over the lattice.     

g-factor of the second 4+ state in24Mg

The transient field technique has been used to determine theg-factor of the 4 ₂ ⁺ state at 6.010MeV excitation in²⁴Mg. The deduced value ofg=+0.5(4) is consistent with collective model expectations. Further, the equality within experimental accuracies, of the g-factors of the 2 ₁ ⁺ , 2 ₂ ⁺ , 4 ₁ ⁺ and 4 ₂ ⁺ states agrees with theoretical predictions for thisT=0 self-conjugate nucleus, in contrast to the results for²⁰Ne.     

Dual nature of RN-centers in LiF crystals

An alternative model of the N_c-center as a complex defect consisting of the F ₂ ⁺ -center perturbed by the F_L defect (where F_L is Li⁰ in the F-center) is confirmed by the methods of optical spectroscopy and X-ray diffraction analysis of LiF crystals. Upon selective optical excitation, these centers are decomposed into F₂ and F_L defects.     

Collision-induced dissociation of H 3 + ions

For collision energies between 100 and 500 eV the collision induced dissociation of H ₃ ⁺ colliding with H₂, He and Kr gas targets was measured. We obtained total cross sections and angular distributions of the charged collision fragments for the main reaction channels. H ₃ ⁺ +H₂→H⁺+2H² and H ₃ ⁺ +H₂→H ₂ ⁺ +H₂+H. An analysis of the kinetics yields that the dissociation proceeds via vibrational-rotational excitation of H ₃ ⁺ by mutually induced dipolmoments.     

E2 andE3 transition strengths in some rare-earth nuclei

Coulomb excitation byα-particles of vibrational-like states in even-mass rare-earth nuclei is used to determine the reduced transition probabilitiesB(E2; 0 _gs ⁺ →2 _γ ⁺ ),B(E2; 0 _gs ⁺ →2 _β ⁺ ),B(E2; 2 _gs ⁺ →0 _β ⁺ ) andB(E2; 0 _gs ⁺ →3 _oct ^? ) in¹⁵⁰Nd,^{152, 154}Sm,^{154, 158}Gd,¹⁶⁴Dy and¹⁶⁶Er. TheB(Eλ; 0 _gs ⁺ →I=λ)-values range from 2.4 to 6.5 single-particle units for transitions to the 2 _γ ⁺ -states, 0.8 single-particle units for the 2 _β ⁺ -states and from 14.1 to 21.7 single-particle units for the 3^?-states.     

Electromagnetic transition probability from the ground to the first excited 2+ state in138ce

The ratio of the B(E2) values for the 0 ₁ ⁺ → 2 ₁ ⁺ transitions in¹³⁸Ce and¹⁴²Ce was measured by Coulomb excitation with α-particles. From the known value of the transition probability in¹⁴²Ce it results: B(E2,¹³⁸Ce, 0 ₁ ⁺ → 2 ₁ ⁺ =0.45 +/?0.03 e² b ²     

Comparison of electron spin polarization of P 870 + Qa a − observed in Zn2+-containing and Fe2+-depleted bacterial reaction centers

Recently, a general model has been developed to explain electron spin polarized (ESP) electron paramagnetic resonance (EPR) signals found in systems where radical pairs are formed sequentially. The photosynthetic bacterial reaction center (RC) is such a system in which we can experimentally vary parameters (lifetime, structure, and magnetic interactions in the sequentially formed radical pairs) that affect ESP development in order to test this model. In Fe²⁺-depleted transfer step from intermediate radical pair, P ₈₇₀ ⁺ Q _a ^? which is produced in an electron transfer step from intermediate radical pair, P ₈₇₀ ⁺ I^?. (P ₈₇₀ ⁺ is the oxidized primary donor, a special pair of bacteriochlorophyll molecules, I^? is the reduced bacteriopheophytin acceptor, and Q _a ^? is the reduced primary quinone acceptor.) The lifetime of P ₈₇₀ ⁺ I^? can be shortened relative to the lifetime of P ₈₇₀ ⁺ I^? in Fe²⁺-depleted RCs by substitution of Zn²⁺. We report the first observation of X-band and Q-band ESP EPR signals due to P ₈₇₀ ⁺ Q^? from bacterial reaction centers that contain Zn²⁺. Comparison of these signals to those observed from Fe²⁺-depleted bacterial reaction centers shows intensity differences and g-factor shifts. The results are discussed in terms of the general sequential radical pair model.     

Study of collisional deactivation of O2(b 1Σ g + ) molecules in a hydrogen-oxygen mixture at high temperatures using laser-induced gratings

Collisional deactivation of O₂(b ¹Σ _g ⁺ ) molecules resonantly excited by a 10 ns pulse of laser radiation with a wavelength of 762 nm in H₂/O₂ mixtures is experimentally studied. The radiation intensity and hence the molecule excitation efficiency have a spatially periodic modulation that leads to the formation of laser-induced gratings (LIGs) of the refractive index. The study of LIG temporal evolution allows collisional relaxation rates of molecular excited states and gas temperature to be determined. In this work, the b ¹Σ _g ⁺ state of O₂ molecules deactivation rates are measured in a 4.3 vol % H₂ mixture at the number density of 2 amg in the temperature range 291–850 K. The physical deactivation is shown to dominate in the collisions of H₂ with O₂(b ¹Σ _g ⁺ ) and O₂(a ¹Δ _g ) up to temperatures of 780–790 K at time delays up to 10 μs after the excitation pulse. The parameters of the obtained temperature dependence of the (b ¹Σ _g ⁺ state deactivation rate agree well with the data of independent measurements performed earlier at lower temperatures (200–400 K). Tunable diode laser absorption spectroscopy is used to measure the temperature dependence of the number density of the H₂O molecules which appear as the mixture, as the result of the dark gross reaction with O₂ molecules in the ground state, O₂ + 2H₂ → 2H₂O. The measurements show that this reaction results in complete transformation of H₂ into H₂O at temperatures of 790–810 K.     

Paramagnetic relaxation kinetics of the cation radical C 60 + in C60 powder

The kinetics of spin-lattice and phase relaxation of C ₆₀ ⁺ radicals in C₆₀ powder has been studied at room temperature by pulsed EPR. It is found that the kinetics can be described by the relation exp $( - a\sqrt t )$ characteristic of the case in which the paramagnetic centers are distributed over relaxation times. It is concluded that the observed kinetics are due to the presence of oxygen molecules, which act as a fast-relaxing impurity and accelerate the relaxation of the C ₆₀ ⁺ radicals. The results obtained offer an explanation for a number of features of C ₆₀ ⁺ relaxation in fullerites discovered earlier.     

Investigation of N 2 + (C 2Σ u + → X 2Σ g + fluorescence excited through auger decay of the 1s −1π* resonance

A theoretical investigation of N ₂ ⁺ (C ²Σ _u ⁺ → X ²Σ _g ⁺ molecular fluorescence excited through the Auger decay of the 1s ^?1π* resonance is carried out. The fluorescence cross sections are calculated with due regard for the dependence of the matrix element of the C → X dipole transition on the internuclear distance, the interference between channels of excitation via different vibrational levels v _r of the 1s ^?1π* resonance, the rotational structure of the fluorescence band, and the predissociation of the N ₂ ⁺ C ²Σ _u ⁺ v′ ≥3) states. The calculated cross sections are in good agreement with the experimental results of recent measurements. The results of the calculations have demonstrated that the observed dependence of the cross section of the (C ²Σ _u ⁺ (v′) → X ²Σ _g ⁺ (v″) fluorescence on the excitation energy and the fluorescence wavelength for a group of bands with equal values of the difference Δv = v′ ? v″ is associated with transitions between the vibrational levels of the electronic states involved in the excitation and subsequent cascade decay of the 1s ^?1π* resonance: N₂ (v ₀ = 0) → N*₂(1s ^?1π*(v _r)) ? N ₂ ⁺ : (C ²Σ _u ⁺ (v′) → X ²Σ _g ⁺ (v″).     

Stoßdissoziation von H 2 + - und D 2 + -Ionen

The angular and energy distribution of protons produced by collision-induced dissociations of H ₂ ⁺ ions with energies of 10 and 20 keV were measured in a parabola spectrograph. From these measurements the velocity distribution of the protons in the center of mass system of the H ₂ ⁺ ion can be calculated. This gives information about the type, the abundance, and the anisotropy of the processes involved. The most frequent transitions leading to dissociations are the excitation of the 2pσ_u state, the ionisation of the H ₂ ⁺ ion, the transition into the vibrational continuum, and the electron capture into the 1³ σ _u ⁺ state of the hydrogen. It is shown that the cross section for an electronic transition depends on the velocity of the ion, the distance of the nuclei in the ion, the angle between the internuclear axis and the direction of the primary ion beam, and the excitation energy of the target. The fraction of protons produced by vibrational excitation increases with increasing atomic number of the target. Concerning electronic transitions D ₂ ⁺ ions equal H ₂ ⁺ ions of the same velocity.     

Mass spectrometer studies of the ion composition in the pink afterglow

The time dependences of the ion number densities in the pink afterglow of nitrogen, as represented by the ion wall currents, have been measured. The ions were extracted through an orifice from a flow system and analysed by a quadrupol mass spectrometer. It has been found thatN ₂ ⁺ ions are dominating in the early afterglow. With the beginning of the ionization processN ₃ ⁺ and at pressure >6 TorrN ₄ ⁺ become the majority ions. The ratio of the number densities(N ₃ ⁺ )/(N ₂ ⁺ ) reaches a maximum during the increase of the ionization processes before the maximum is reached. This behaviour suggestsN ₃ ⁺ ions to be the primary ions created by the ionization processes. The time dependences of the ion number densities (N ₂ ⁺ ), (N ₃ ⁺ ) and(N ₄ ⁺ ) are found to vary similar, showing that the ions are strongly coupled by conversion processes. The conversion processes are discussed. In the maximum of ionization at a total pressure of 4.4 Torr the ratios of the number densities of the afterglow ions (N ₂ ⁺ )∶(N ₃ ⁺ )∶(N ₄ ⁺) are 1∶1.9∶0.64.     

g-factors of the lowest 2+ and 4+ states in198, 200, 202Hg

Theg-factors of the 2 ₁ ⁺ and 4 ₁ ⁺ states in^198,200,202Hg were simultaneously measured by means of the transient-field perturbed angular correlation method in Coulomb excitation using multi-isotopic targets and thin polarized Gd foils as ferromagnetic host. Theg(2 ₁ ⁺ ) andg(4 ₁ ⁺ ) were found identical within errors in^{198, 200}Hg, while in²⁰⁰Hg lowerg-factor values have been determined. The experimentalg-factors were compared with the predictions of the pairing-plus-quadrupole, dynamical deformation and interacting boson models.