Controllable broadening of zero-phonon lines by means of the Doppler effect and prospects of using spectral hole burning in optical informatics

An attempt is made to extend the spectacular variant of optical informatics efficient at liquid helium temperature—holography based on zero-phonon lines (ZPLs) and spectral hole burning, including time-and-space-domain holography—to higher temperatures, up to room temperature. At room temperature, both optical and Mössbauer narrow ZPLs exist; however, they do not have the inhomogeneous broadening that transforms a ZPL into a broad band, which is necessary for informatics based on light pulses. The idea of producing a band with an appropriate width from narrow ZPLs by using the Doppler effect is advanced. A variant of experimental realization of this idea by means of a scheme with a rotating disk covered by a layer of a material sensitive to spectral hole burning is considered. Numerical estimates were performed for narrow optical ZPLs and for the yet experimentally unconfirmed Mössbauer ZPL in the visible spectral range (dark blue nuclear light) that corresponds to a transition between the two low-lying levels of the ²²⁹Th isomer. For the narrowest optical ZPLs known at present, with a width of about 100 Hz, the estimates give favorable results, in particular, for prospects of realizing a photoelectrically accumulated stimulated photon echo.     

The EPR dipolar broadening of irradiated solids as detected using FID and ESE following selective hole burning

A novel electron spin echo method employing detection of FID and transient echo shape following selective hole burning in the EPR spectrum has been applied to study γ-irradiated malonic acid. The dipolar lineshapes of stabilized free radicals are separated into bulk and pairwise contributions; both of them have proved to be Lorentzian.     

光谱烧孔技术

论述了光谱烧孔技术的动力学理论模型 ;介绍了单光子烧孔和多光子烧孔所取得的实验结果 ;讨论了光谱烧孔的发展趋势 :提高烧孔度 ,实现室温烧孔和提高探测及读出时的信噪比。问题的关键在于光致填孔机制的研究。同时提出将它投入实际应用亟待解决的问题 ,即作为一种可能的高密度频域光信息存储手段所亟待解决的问题是开发适应于此技术的新材料 ,深入研究材料体系的烧扎特性     

Application of the broad hole burning technique for studying low-temperature photoreactions in impurity amorphous bodies

A new experimental method is developed for measuring kinetics of low-temperature photoreactions—the broad hole burning technique, which eliminates the nonexponentiality of the hole burning kinetics caused by the inhomogeneous broadening. The method is successfully used to study the low-temperature photoreactions in various impurity amorphous systems. Examples of single-and two-exponential kinetics have been found, as well as kinetics with a moderate or large dispersion of the hole burning quantum efficiency. The results obtained show a good outlook for the broad hole burning technique for studying low-temperature photoreactions and illustrate the diversity of photoreactions occurring in specific chromophore-matrix pairs.     

Stark broadening of isolated lines emitted by singly-ionized tin

Calculations have been performed on the electron impact broadening of isolated lines from singly-ionized tin from a cool plasma. These have been compared with results of measurements recently performed by Miller, Roig, and Bengtson on a plasma produced by a conventional shock tube, and satisfactory overall agreement has been obtained. Our method is similar in procedure to that of the semi-empirical approximation of Griem, but we take into account the details of the radiator structure, including configuration interaction for two of the terms. We propose a new expression from which the relevant effective Gaunt factors for singly-charged ions can be calculated for incident energies above threshold. In some cases, a significant variation of line width within multiplets is noted. Some difficulties have been experienced with transitions to states involving equivalent electrons.     

Stark broadening of the Al resonance lines

Absolute Stark-broadened profiles of the Al resonance lines (3p-4s, γ = 3961.5 and 3944.0 Å) have been measured under conditions of complete LTE in a conventional shock-tube. Plasma electron densities were determined by using a laser-interferometer. Uncertainties in the measurements (15% for the widths and 13% for the shifts) are discussed. The results are compared with impact-broadening calculations.     

Single-frequency ytterbium-doped fiber laser stabilized by spatial hole burning

We have exploited spatial hole burning to achieve remarkably stable single-frequency operation and mode-hop-free tuning over 300 free spectral ranges in an ytterbium-doped fiber laser with a sample standing-wave geometry. This approach makes possible stable and narrow-linewidth single-frequency fiber lasers that do not require components such as Faraday isolators, fiber couplers, and Fabry-Perot filters.     

Study on Ion-dynamics in solids by hole burning spectroscopy

The importance of hole burning spectroscopy for studying elementary migration processes of ions in superionic conductors is being discussed using two examples. In β″-alumina, the potential energy for the conduction of ions along the conduction path, as obtained from the analysis of the results of hole burning spectroscopy, showed that there are two different bare-potentials along the ionic conduction path. One of them is higher than the activation energy for ionic conductivity. This result gives direct evidence that an ionic interaction among the conducting ions plays an important role for ion migration in β″-alumina. In YSZ with various concentration of Y₂O₃, we have observed persistent holes in Pr³⁺ ions doped samples. Their disordered nature will be discussed using the bandwidth considerations. Paper presented at the 9th EuroConference on Ionics, Ixia, Rhodes, Greece, Sept. 15–21, 2002.     

Stark broadening of neutral helium lines

Using a semiclassical approach for the Stark broadening of atomic lines, we have calculated electron and proton impact line widths and shifts of 56 neutral He lines in the ultraviolet, visible and i.r. region of the spectrum. The comprehensive set of results obtained is used for investigation of Stark-broadening parameter regularities within the spectral series.     

Collisional broadening of infra-red absorption lines

The Lorentz half-widths of collision-broadened lines in the rotation-vibration bands of diatomic molecules vary with line number |m| in the P and R branches. The observed variation of half-width for lines in the 0 → 1 and 0 → 2 bands of CO and HCl are interpreted in terms of a simple fitting procedure. One dominant source of line broadening is assumed to consist of diabatic hard collisions involving transitions from each rotational level to all higher rotational levels; the effectiveness of this process, which varies from line to line, is described in terms of an empirically adjusted collision cross section, a maximum collision parameter related to independently measured molecular properties, and upon the availability of the required energy and angular momentum in molecular collisions. The second source of line broadening, assumed to be the same for all lines, includes all other types of collisions and is represented by a single empirically adjusted cross section. The simple fitting procedure is applied successfully to self-broadening of CO lines and to foreign-gas broadening of CO and HCl; for HCl self-broadening an additional cross section for resonant-dipole processes must be included. Possible applications of the fitting procedure to HBr, HF, and CO₂ are discussed. The simple procedure presented represents an approximation that may prove useful pending the development of readily applicable complete theories based on first principles.     

Stark broadening of neutral sodium lines

A semiclassical approach has been used to evaluate Stark broadening of atomic lines and also electron-and proton-impact line widths and shifts of 30 neutral sodium lines. The results are used to investigate Stark broadening-parameter regularities within the spectral series.     

Stark broadening of neutral potassium lines

Using a semiclassical approach, we have calculated electron-proton and Ar II impact line widths and shifts of 50 neutral potassium lines. The comprehensive set of results obtained is used for investigation of Stark-broadening-parameter regularities within the spectral series.     

On the stark broadening of ionized nitrogen lines

In this paper, we report an analysis of the experimental procedure and results obtained in a recently published paper on the Stark broadening of singly-, doubly-, and triply-ionized nitrogen lines. The results of this analysis indicate that the influence of self-absorption on the line profiles is not taken into account properly and that therefore the results of Ref. 6 cannot be applied with confidence. Comparisons of experimental results with numerous theoretical calculations have also been performed.     

Effect of low-frequency modes on temperature broadening of optical lines of impurity centres in glasses

Anomalous temperature dependences of impurity homogenous linewidth in glasses are explained quantitatively on the basis of the ordinary two-phonon Raman-like broadening mechanism without using “two-level” system.     

Low-temperature spectroscopy of organic molecules in solids by photochemical hole burning

Characteristic features of photochemical hole-burning (PHB) in the impurity spectra of low-temperature solids and PHB applications in molecular spectroscopy are considered. The evolution of a no-phonon hole and a phonon sidehole in excitation and fluorescence spectra is analysed on the basis of model calculations. Some more complex models for PHB are considered, which take into account reverse reactions, the optical thickness of the sample, the inhomogeneous dispersion of both homogeneous linewidths and transition energies of the photoproduct and quasi-static impurity-impurity interactions. The effects of PHB on fluorescence line narrowing are discussed. By PHB homogeneous linewidths of purely electronic and vibronic no-phonon lines in the spectra of some porphine and phthalocyanine derivatives in various matrices are measured and their temperature dependence is studied. The latter is found to be essentially different in polycrystalline and glassy matrices. Line-broadening mechanisms are discussed. By PHB the existence of an inhomogeneous distribution of vibrational frequencies in molecular impurities is established. The applications of PHB in the studies of photochemical reactions in solid solutions of phthalocyanine derivatives and tetracene are regarded and the mechanisms of these reactions are discussed. The results obtained by PHB for chlorophyll and its derivatives are presented.     

Nonresonant hole burning spectroscopy of the relaxor ferroelectric PLZT

The polydispersive dielectric response of a lanthanum-modified lead zirconate titanate relaxor ferroelectric was studied using nonresonant hole burning (NHB) spectroscopy. The dynamic heterogeneity of this material was evidenced by the fact that it was possible to burn frequency-dependent spectral holes. The maximum position of the spectral holes depended on the square root of the pump frequency Ω. The refilling of the spectral holes was monitored subsequent to excitation using various pump frequencies. The refilling data could be collapsed onto a master curve by re-scaling them, again, using Ω^−0.5 as scaling factor. The refilling time was found to be much longer than the time scale addressed most by the pump process. This behavior underscores the importance of domain wall motions for the dielectric relaxation process.     

On the drastic temperature broadening of hard mode Raman lines of ferroelectric KDP type crystals near Tc

The drastic broadening of a few A₁ Raman lines of ferroelectric KH₂PO₄(KDP) and KH₂AsO₄(KDA) crystals have been measured at various temperatures near T_c. The results in KDP are in fair agreement with two different simplified expressions of linewidths, which are based on pseudospin-phonon interaction arguments. No such agreement is found between the results and a simplified linewidth expression derived from a theory based on soft mode-hard mode interaction arguments. The linewidths and the reciprocal of the proton spin-lattice relaxation time in KDP exhibit a very similar temperature dependence below T_c but behave differently above T_c. This phenomena is presented in detail, and discussed.     

The phase shifts leading to the broadening and shift of spectral lines

The classical theory of collisional broadening and shift parameters (β, δ) of an isolated spectral line was used to obtain simple analytical formulas for calculating both β and δ. These formulas were obtained on the assumption that the short range interaction is effective only in the broadening while the long range is effective in the shift of the spectral line. These parameters β and δ depend on the limiting phase shifts responsible for broadening η_b and shift ηδ. It was found that the values of η_b and η_δ are not equal to each other as was proposed by Weisskopf η_b=η_δ=1. The maximum and average values of η_b (η_b max, η_b av) and η_δ (η_δ max, η_δ av) were obtained by numerical evaluation, using different inverse power potentials. By introducing these parameters into the approximated formulas for β and δ using Van der Waals and Lennard-Jones potential, it was found that the results of calculations for (β and δ) with different atomic transitions perturbed by different inert gases are in close agreement with earlier results. Those results, obtained earlier, were based on the Lindholm-Foley theory especially with the average values of η_b [η_b av=0.6057] and the maximum values of η_δ [η_δ max=1.57625]. The impact parameters ρ_b and ρ_δ leading to the broadening and shift of the spectral line were also obtained for different interactions. It was found that the end parameter for the broadening ρ_b is not equal to the starting parameter for the shift ρ_δ.