Spectro-temporal behavior of dye-based solid-state random lasers under a picosecond pumping regime: Part III.

In two recent works, the authors have investigated the spectro-temporal properties of the random laser emission from solid state dye-doped powders in picosecond pumping regime. Each emission pulse consists, both above and below threshold, in a collection of narrow peaks of a spectro-temporal width at the theoretical limit (ΔωΔt≅1). The distribution of path lengths traveled inside the diffusive active medium by photons that can be amplified by stimulated emission explains this behavior, as demonstrated by a simple theoretical model developed by the authors. The aim of the present work is, first, to develop an implemented model that does not depend on fitting parameters, and which is compatible with the energetic and spectro-temporal properties of the material; and second, to get knowledge about the spatial properties of the emission. The transverse coherence size of each emitted photon packet has been measured; and in addition, we have shown the existence of spatial fluctuations of the emission of these materials, as our model predicts.

Spectro-temporal behavior of dye-based solid-state random lasers under picosecond pumping regime: part II.

In a very recent work the spectral and temporal properties of the random laser emission from solid state dye-doped powders have been investigated by the authors in picosecond pumping regime. The emission shows within each pulse, peaks of more intensity than background, and of a spectro-temporal width at the theoretical limit (ΔωΔt≅1), even in conditions well below the threshold. The relationship between the distribution of paths lengths traveled by photons inside the active medium, and the amplification by stimulated emission explains this behavior. The aim of the present work is to propose a simple model that, in addition to explaining these characteristics of the emission, is compatible with the energetic properties of the material. Particularly interesting is the behavior predicted by the model for the emission decay in sub-threshold conditions, as well as its very good fit with the experimental measurements and its comparison with the one found in low dispersive media, that shows the decisive effect of scattering. The set of results is hardly compatible with a mode structure.

Spectro-temporal behavior of dye-based solid-state random lasers under picosecond pumping regime.

In this work, the spectral and temporal properties of the random laser emission from dye-doped solid state powders are investigated in picosecond pumping regime. Ultrafast time-resolved spectroscopy achieved with a streak-camera has been used to perform a detailed study of the temporal evolution of the spectrum of their single pulses. Under conditions of low population inversion density, it is observed that the detected radiation occurs as isolated peaks with a very narrow spectro-temporally spread (ΔωΔt≅1). This behavior remains under conditions of high population inversion density, suggesting that the underlying physical mechanism that produces the emission is the same whatever the pumping conditions. Measurements carried out by varying the numerical aperture of the detection system show that each detected peak within a single pulse is associated with a photon pack emitted in a random direction and wavelength. The relationship between the distribution of paths lengths done by photons inside the active medium, and the gain explains the observed behavior.

Input/output energy in solid state dye random lasers.

A new approach to the problem of energy in solid state dye random lasers is presented. The measurements performed in terms of absolute energy show that the slope efficiency depends on the measurement conditions. In particular, in lasers with pumping in the picoseconds range, the result is really different if measured by recording the emission in the same time range or in a longer one (nanoseconds range). In the last case, no energy threshold is observed. A previously developed model has been applied to the solid state dye random laser. It is a rate-equations model, based on a distribution of paths with different lengths, which partially share population inversion. The results of the model are satisfactory and show that the dynamic behavior is pretty similar in solid state dye random lasers and in inorganic powders.

Tunable upconversion emission in NaLuF4-glass-ceramic fibers doped with Er3+ and Yb3.

Novel glass-ceramic optical fibers containing NaLuF4 nanocrystals doped with 0.5ErF3 and 2YbF3 (mol%) have been prepared by the rod-in-tube method and controlled crystallization. NaLuF4 nanocrystals with a size around 20 nm are obtained after heat treatment at 600 °C. Intense upconverted green and red emissions due to (2H11/2, 4S3/2) → 4I15/2 and 4F9/2 → 4I15/2 transitions, respectively, together with a blue emission due to 2H9/2 → 4I15/2 transition have been observed under excitation at 980 nm. The intensity of the green and red upconversion bands shows a nearly linear dependence on the excitation power which can be explained by saturation effects in the intermediate energy states and proves that a sensitized energy transfer upconversion process is responsible for the population of the emitting levels of Er3+ ions. The upconversion emission color changes from yellow to green by increasing the excitation power density which allows to manipulate the color output of the Er3+ emission in the glass-ceramic fibers. The tunable emission color is easily detected with the naked eye. This interesting characteristic makes these glass-ceramic fibers promising materials for photonic applications.

Random laser model for Nd3+-doped powders and its application to stimulated emission cross-section calculations.

A new theoretical approach for random lasing of Nd3+doped powders is presented. The model's singularity lies in the fact that it proposes a probability distribution of the stimulated photon paths lengths in the sample, as well as a population inversion shared by different photon paths. The model's predictions satisfactorily compare with the results of laser threshold and absolute input/output energy slope of a real Random Laser. The main novel issue is that the best fit to the experimental results requires considering a high level of shared population inversion among different paths. The model simulation of local and spatially integrated Random Laser emissions, as well as their time evolution, is in accordance with the experimental behavior. These results also provide a new method of measuring the stimulated emission cross-section in this kind of random laser materials.

Random laser properties of Nd3+ crystal powders.

This work presents an overview of near infrared random lasing emitters based on a variety of neodymium (Nd3+)-doped crystal powders with different Nd3+ concentrations and different grain sizes. The pump-configuration used allows for an absolute measurement of both pumping and emitted energies. The results provide an absolute measure of the random laser efficiency and prove a relation of direct proportionality between the absorbance of the material and the laser slope efficiency. Likewise, they suggest a relationship close to an inverse proportionality between the absorbance and the threshold energy per unit area. The temporal behavior of the random laser emission shows noteworthy differences between local and spatially integrated registers.

Effects of pumping wavelength and pump density on the random laser performance of stoichiometric Nd crystal powders.

Laser slope and threshold properties have been investigated in Nd stoichiometric crystal powders as a function of pump wavelength and pump beam size. Above a given pumped area, the laser slope and the threshold pump energy per unit area are invariant and the known theoretical expressions are well fulfilled. Likewise, the size of the stimulated emission zone as a function of the pump beam area has been measured, also showing a different behavior above or below a given pumped area value which coincides with the one mentioned above. In conclusion, two different operating regimes with different performances are clearly observed as a function of the pump beam area.

On the temporal behavior of Nd3+ random lasers.

The temporal dynamics of random laser emission from Nd-doped crystal powders has been investigated by using an improved detection device. The precise conditions to detect high contrast, fast oscillations are described. The measured period is about one order of magnitude shorter than the one given in the literature for relaxation oscillations in these materials. The origin of these differences is discussed.

Spectral study of the stimulated emission of Nd3+ in fluorotellurite bulk glass.

In this work we present, for the first time to our knowledge, laser emission under wavelength selective laser-pulsed pumping in Nd(3+)-doped TeO(2)-ZnO-ZnF(2) bulk glass for two different Nd(3+) concentrations. The fluorescence properties of Nd(3+) ions in this matrix which include, Judd-Ofelt calculation, stimulated emission cross-section of the laser transition and lifetimes are also presented. The site-selective emission and excitation spectra along the (4)I(9/2)→(4)F(3/2) absorption band show the inhomogeneous behaviour of the crystal field felt by Nd(3+) ions in this fluorotellurite glass which allows for spectral tuning of the laser output pulse as a function of the pumping wavelength. The emission cross-section obtained from the Judd-Ofelt analysis and spectral data (4.9x10(-20) cm(2)) is in fairly good agreement with the value obtained from the analysis of the laser threshold data (4x10(-20) cm(2)).

Time-resolved fluorescence line-narrowing of Eu3+ in biocompatible eutectic glass-ceramics.

The spectroscopic properties of Eu(3+) in biocompatible glass and glass-ceramic eutectic rods of composition 0.8CaSiO(3)-0.2Ca(3)(PO(4))(2) doped with 0.5 wt% of Eu(2)O(3) are investigated to explore their potential applications as optical probes. The samples were obtained by the laser floating zone technique. Depending on the growth rate, they exhibit three (two crystalline and one amorphous) or two (one crystalline and one amorphous) phases. The crystalline phases correspond to Ca(2)SiO(4) and apatite-like structures. At high growth rates the system presents an amorphous arrangement which gives a glass phase. The results of time-resolved fluorescence line narrowing spectroscopy obtained under excitation within the inhomogeneous broadened (7)F(0)→(5)D(0) absorption band allow to isolate the emission from Eu(3+) ions in the crystalline and amorphous environments and to accurately correlate the spectroscopic properties with the microstructure of these eutectics.

Site-selective laser spectroscopy of Nd3+ ions in 0.8CaSiO3-0.2Ca3(PO4)2 biocompatible eutectic glass-ceramics.

In this work we report the influence of the crystallization stage of the host matrix on the spectroscopic properties of Nd3+ ions in biocompatible glass-ceramic eutectic rods of composition 0.8CaSiO3-0.2Ca3(PO4)2 doped with 1 and 2 wt% of Nd2O3. The samples were obtained by the laser floating zone technique at different growth rates between 50 and 500 mm/h. The microstructural analysis shows that a growth rate increase or a rod diameter decrease leads the system to a structural arrangement from three (two crystalline and one amorphous) to two phases (one crystalline and one amorphous). Electron backscattering diffraction analysis shows the presence of Ca2SiO4 and apatite-like crystalline phases. Site-selective laser spectroscopy in the (4)I(9/2)→(4)F(3/2)/(4)F(5/2) transitions confirms that Nd(3+) ions are incorporated in crystalline and amorphous phases in these glass-ceramic samples. In particular, the presence of Ca(2)SiO(4) crystalline phase in the samples grown at low rates, which has an excellent in vitro bioactivity, can be unambiguously identified from the excitation spectra and lifetime measurements of the (4)F(3/2) state of Nd(3+) ions.

Spontaneous and stimulated emission spectroscopy of a Nd(3+)-doped phosphate glass under wavelength selective pumping.

The influence of the host matrix on the spectroscopic and laser properties of Nd(3+) in a K-Ba-Al phosphate glass has been investigated as a function of rare-earth concentration. Site-selective time resolved laser spectroscopy and stimulated emission experiments under selective wavelength laser pumping show the existence of a very complex crystal field site distribution of Nd(3+) ions in this glass. The peak of the broad stimulated (4)F(3/2)→(4)I(11/2) emission shifts in a non monotonous way up to 3 nm as a function of the excitation wavelength. This behavior can be explained by the relatively moderate inter-site energy transfer among Nd(3+) ions found in this system and measured by using fluorescence line narrowing spectroscopy. The best slope efficiency obtained for the laser emission was 40%.

Random lasing in Nd:LuVO4 crystal powder.

Room temperature random lasing action is demonstrated for the first time in a low concentrated neodymium doped vanadate crystal powder. Laser threshold and emission efficiency are comparable to the ones obtained in stoichiometric borate crystal powders. The present investigation provides a complete picture of the random lasing characteristics of Nd-doped vanadate powder both in the spectral and temporal domain, together with a simplified model which accounts for the most relevant features of the random laser.

Study of broadband near-infrared emission in Tm3+-Er3+ codoped TeO2-WO3-PbO glasses.

In this work, we report the near-infrared emission properties of Tm(3+)-Er(3+) codoped tellurite TeO(2)-WO(3)-PbO glasses under 794 nm excitation. A broad emission from 1350 to 1750 nm corresponding to the Tm(3+) and Er(3+) emissions is observed. The full width at half-maximum of this broadband increases with increasing [Tm]/[Er] concentration ratio up to a value of ~ 160 nm. The energy transfer between Tm(3+) and Er(3+) ions is evidenced by both the temporal behavior of the near-infrared luminescence and the effect of Tm3+ codoping on the visible upconversion of Er(3+) ions.

Spectroscopic properties of the 1.4 microm emission of Tm3+ ions in TeO2-WO3-PbO glasses.

In this work, we report the spectroscopic properties of the infrared 3H4-->3F4 emission of Tm3+ ions in two different compositions of glasses based on TeO2, WO3, and PbO for three Tm2O3 concentrations (0.1,0.5, and 1 wt%). Judd-Ofelt intensity parameters have been determined and used to calculate the radiative transition probabilities and radiative lifetimes. The infrared emission at around 1490 nm corresponding to the 3H4-->F4 transition has two noticeable features if compared to fluoride glasses used for S-band amplifiers. On one hand, it is broader by nearly 30 nm, and on the other, the stimulated emission cross section is twice the value for fluoride glasses. Both the relative intensity ratio of the 1490 nm emission to 1820 nm and the measured lifetime of the 3H4 level decrease as concentration increases, due to the existence of energy transfer via cross-relaxation among Tm3+ ions. The analysis of the decays from the 3H4 level with increasing concentration indicates the presence of a dipole-dipole quenching process assisted by energy migration.

On the origin of bichromatic laser emission in Nd3+-doped fluoride glasses.

In this work we present a detailed study about the influence of the host matrix in the spectroscopic and laser properties of Nd3+ in three different fluoride glasses. Site-selective time-resolved techniques have been used to investigate the crystal field changes felt by the Nd3+ ion as a consequence of glass inhomogeneity. Stimulated emission experiments performed under selective wavelength laser pumping show the existence of bichromatic emission from two distinguishable site distributions for Nd3+ in fluoride glasses. This result can be explained by the moderate inter-site energy transfer among Nd3+ ions found in these systems.

Optical spectroscopic study of Eu3+ crystal field sites in Na3La9O3(BO3)8 crystal.

Time-resolved line-narrowed fluorescence spectroscopy of Eu(3+) ions in a new oxyborate Na(3)La(9)O(3)(BO(3))(8) crystal shows the existence of four independent symmetry crystal field sites for the rare-earth ion. A crystal field analysis and simulation of the experimental results have been performed in order to parametrize the crystal field at the Eu(3+) sites. A plausible argument about the crystallographic nature of these sites is given.

Food, audience and sex effects on pinyon jay (Gymnorhinus cyanocephalus) communication.

Pinyon jays (Gymnorhinus cyanocephalus) have a complex social system that may require a complex communication system. They need to interact with multiple flock members, and they form life-long pair-bonds. We researched whether pinyon jays would selectively vocalize depending on the presence or absence of food and certain flock members. We recorded the vocalizations of nine pinyon jays (four pair-bonds and one single male) in response to different audience types. The calls of the test bird were recorded after it was given either an empty food cup or one containing 50 pinyon pine (Pinus edulis) seeds, and the bird was in the presence of one of the following audience types: (1) two males and two females including subject's mate; (2) two males and two females excluding subject's mate; (3) four males excluding mate; (4) three females excluding mate; and (5) no audience. Birds gave fewer calls when there was food. When alone, birds called in a manner that may maximize long-distance transmission. Trends indicate that birds call differently to their mate. A sex effect was also found in that males and females called in a distinct manner, possibly reflecting differences in dominance status. Overall, birds responded to the presence or absence of an audience.

Anti-Stokes laser cooling in Yb(3+)-doped KPb(2) Cl(5) crystal.

We report internal laser cooling in Yb(3+) -doped KPb(2)Cl(5) . From the quantum efficiency values measured in the heating and cooling regions by use of the photothermal deflection technique, we have obtained a room-temperature cooling efficiency of 0.2% in a sample doped with ~5x10(19)ions/cm(3) . Excitation spectra obtained under high irradiation fluences show an excess of fluorescence with regard to those obtained at low fluences, which agrees with the prediction of a model based on photon-ion-phonon interaction.