Optical bistability in fluorescein dyes

Optical bistability has been observed in highly concentrated fluorescein dye solutions and in thin (1 m) doped polymeric films. At concentrations larger than 10^–5 mole/l dye dimers are formed. For fluorescein dye, the dimer-monomer equilibrium constant is 10⁵ l/mole so that most of the dye species are in the dimer form. At 480 nm the dimer absorption cross section is 10^–18 cm²/molecule, while that for the dye monomer molecule is 7.6×10^–17 cm²/molecule. Upon laser excitation dimers dissociate to form monomers thus providing a highly nonlinear laser induced absorption. This high nonlinear absorption coefficient can be utilized for optically bistable response of the dye system.Optical bistability was observed by placing dye solutions or dye thin films inside a Fabry-Perot resonator and exciting it with 480 nm dye laser pulses of 10 ns duration. The effect is more pronounced in 10^–4 mole/l fluorescein than in 10^–6 mole/l fluorescein in which dimer formation is not that efficient.In disodium fluorescein no significant dimer formation is observed even at 10^–3 mole/l dye concentration. The observed bistability both in solution and in thin films can be explained in terms of recent models for optical bistability in nonlinearly absorbing molecular systems.     

High power DFB laser tunable in the 7420 Å-10500 Å range

The dye DDI (1,1'-diethyl 2,2'-dicarbocyanin iodid) dissolved in DMSO (dimethyl sulphoxid) was used in giant pulse ruby laser pumped DFB laser configuration. Wide generation band, narrow (0.1 cm^-1) bandwidth, high power as 1.33 MW at the peak of the tuning curve and power conversion factor as high as 30% was found.     

A microchip-laser-pumped DFB-polymer-dye laser

A miniaturized, high repetition rate, picosecond all solid state photo-induced distributed feedback (DFB) polymer-dye laser is described by applying a passively Q-switched and frequency-doubled Cr⁴⁺:Nd³⁺:YAG-microchip laser (pulse width Δτ=540 ps, repetition rate ν=3 kHz, pump energy E_pump=0.15 μJ) as a pump source. A poly-methylmethacrylate film doped with rhodamine B dye serves as active medium. The DFB-laser pulses are temporally and spectrally characterized, and the stability of the thin polymer/dye film at high repetition rates is analyzed. The shortest DFB-laser pulses obtained have a duration of 11 ps. After the emission of 350000 pulses the intensity of the DFB-laser output has decreased by a factor of two and the pulse duration has increased by a factor of 1.2. For single DFB-laser pulses of 20-ps duration the spectral bandwidth is measured to be Δλ=0.03 nm, which is only 0.005 nm above the calculated Fourier limit assuming a Gaussian profile for the temporal shape of the pulses. Coarse wavelength tuning of the DFB laser between 590 and 619 nm is done by turning the prism. Additionally, a fine tuning of the DFB-polymer-laser wavelength is achieved by changing the temperature of the polymer/dye layer (=-0.05 nm/°C) in the range from 20 to 40 °C. Received: 1 March 2001 / Revised version: 23 May 2001 / Published online: 18 July 2001     

Stimulated emission at the second order stop-zone edge of the two-dimensional opal–zinc oxide photonic crystal

The fabrication of the 2D periodic structures in ZnO thin films by magnetron sputtering on the opal matrices was developed. The microstructures were characterized by AFM and SEM. The spontaneous and stimulated emissions of the ZnO layers on opal were studied at N₂ laser excitation (λ = 337 nm). The stimulated emission near 397 nm was observed at room temperature from ZnO–opal structure. The threshold of the electron–hole plasma recombination laser process was 300 kW/cm² for this structure. This threshold is two orders of magnitude smaller of that one for the flat ZnO–SiO₂ films owing to DFB resonator effect in 2D structure.     

Solid-state dye laser with moiré gratings

We fabricated distributed-feedback (DFB) solid-state dye lasers with moiré gratings. We formed a moiré grating pattern by superimposing two grating patterns with a rotation angle. The moiré gratings were fabricated by an “etchless” process utilizing a two-beam interference method. The gratings were coated with solidified rhodamine-B. The five laser devices were pumped with the second harmonic generation of a Nd:YAG laser and we obtained narrow-banded laser oscillations at 590, 600, 610, 620, and 630 nm wavelength. Full widths at half maximum of laser spectra were less than 0.5 nm. The results indicated that a moiré fringe can function as a resonator of DFB solid-state dye lasers.     

Frequency stabilization of a frequency-doubled 197.2 THz distributed feedback diode laser on rubidium 5S1/2→7S1/2 two-photon transitions

A 197.2 THz (1520.2 nm) ITU-T grid distributed feedback (DFB) diode laser is frequency stabilized at 197.198 THz by 1ocking its second harmonic (SH) signal on the rubidium 5S_1/2→7S_1/2 two-photon transition at 394.396 THz (760.1 nm). With 100 mW from the DFB diode laser and amplifying by an erbium-doped fiber amplifier, we obtain an SH power of 15 mW using a periodically poled lithium niobate (PPLN) waveguide frequency doubler. The stability was 2×10⁻¹¹ (10 s), corresponding to a frequency variation of 4 kHz at 1520.2 nm. Our scheme provides a compact and high performance frequency reference in the communication band.     

Lasing characteristics of Rhodamine B and Rhodamine 6G as a sensitizer in sol–gel silica

We report lasing characteristics of Rhodamine B (Rh. B) in sol–gel silica under excitation with frequency-doubled Nd:YAG laser and sensitization with Rhodamine 6G (Rh. 6G). The principle of radiative energy transfer (from Rh. 6G to Rh. B) has been utilized as a longitudinally Rh. 6G laser (at 585 nm)-pumped Rh. B laser process in the same sample. Rh. B offers a high photostable and efficient laser dye in sol–gel silica sensitized with Rh. 6G; 75,000 shots as a laser half-lifetime of the sample and 24% efficiency at pumping intensity 0.1 J/cm² of 532 nm. Wavelength shift occurs from 606 to 630 nm in the Rh. B laser with increasing its concentration from 1×10⁻⁴ to 8×10⁻⁴ M. The measured optical gain for Rh. B sensitized with Rh. 6G in sol–gel silica is higher than that in ethanol. A new effect has been observed; at 1×10⁻⁴ M of Rh. B and 0.5×10⁻⁴ M of Rh. 6G mixture, the emitted color of laser is changed by changing the pump intensity of frequency-doubled Nd:YAG laser.     

Energy transfer in slab dye lasers

A simple model of the energy transfer between a booster dye and the active dye in a flashlamp pumped planar waveguide dye laser is described.Analytical results are compared with experiments for several dyes in the 600–650 nm region.A twofold increase of laser output was found at a wavelength (630 nm) which is of particular interest for several applications.     

Vertically emitting, dye-doped polymer laser in the green (λ ∼ 536 nm) with a second order distributed feedback grating fabricated by replica molding

Lasing in the green from a distributed feedback (DFB) structure, based upon a second order grating fabricated by replica molding in a dye-doped UV curable polymer, has been demonstrated. For a Bragg grating having a periodicity and depth of 360 ± 2 nm and 78 ± 5 nm, respectively, a coumarin 540-polymer laser operates at 535.6 nm, which is in agreement with calculations of the photonic band diagram for the structure. The fabricated laser exhibits a linewidth of 0.15 nm, a threshold pump fluence of ∼0.7 mJ cm⁻² at 355 nm, and a slope efficiency of ∼14%. Incorporation of the dye gain medium into a one- (or two-) dimensional photonic crystal and fabrication of the grating by replica molding at room temperature provides an inexpensive approach to fabricating polymer-based DFB lasers on flexible substrates of large area.     

Picosecond fluorescence studies by intracavity gain spectroscopy in a modelocked dye laser

This article presents measurements which combine modelocking technique with intracavity spectroscopy. To test this approach, a sample (10^–5 m ethanolic solution of 1,4-dihydroxyanthranquinone) was inserted in a modelocked Ar⁺ ion laser and probed by intracavity pulses of a synchronously pumped dye laser. The probing of the sample results in an amplification of the dye laser output. Maximum output was measured if the pulses of the dye laser temporally overlapped with those of the Ar⁺ ion laser inside the sample. Under this condition, the spectral laser intensity was shaped by the spectrum of stimulated fluorescence which originated from a molecular vibronic state populated by pump laser excitation.Presented at LASERION '91, June 12–14, 1991, München (Germany)     

High-order stimulated electronic Raman scattering from lithium vapor

An intense radiation at 395.0 nm has been observed when lithium vapor is optically pumped in a heat pipe with a pulsed dye laser whose output wavelength is tuned near the Li 2s–4s two-photon resonance transition. The radiation is emitted in the direction along the pump laser beam. It is proposed that the 395.0 nm radiation is mainly generated through three-photon excitation and one-Raman-photon scattering followed by two-cascade (spontaneous) emission. The overall reaction mechanism can be described by a parametric six-wave mixing process. The quantum efficiency of the observed process is estimated to be of the order of 2 × 10^–6.This work was partially supported by the USC Faculty Research and Innovation Fund     

Laser performance of perylenebis (dicarboximide) dyes with long secondary alkyl chains

The laser performance and related photophysical properties of two very soluble perylene dyes with long chain secondary alkyl groups were investigated in cyclohexane solution. With a dye laser as pump source a tuning range of 555–580 nm was obtained at an optimum concentration of 3×10^–4 M. The quantum efficiencies (=0.29 and 0.21) were better than 1/2 that of rhodamine 6G. No photodegradation was observed over an excitation period of several hours.     

Polymeric distributed-feedback resonator with sub-micrometer fibers fabricated by two-photon induced photopolymerization

The authors observed amplified spontaneous emission (ASE) action with an ultra-low threshold under optical excitation from an active polymeric distributed-feedback (DFB) resonator which consists of sub-micrometer fiber grating. A dendrimer was used to modify the laser dye and increased its concentration up to 4.95 wt. % in the photocured resin. The DFB resonator was fabricated by using two-photon induced polymerization (TPIP) technique. The ASE at 556 nm was observed with a threshold of 0.30 μJ/pulse due to fourth-order diffraction feedback of the optical gain. This DFB could be expected to open a way for the fabrication and application of microscale polymeric mirrorless laser. PACS 42.70.-a; 81.40.Tv; 82.35.Ej; 82.50.Pt; 42.60.Da     

Diode-pumped distributed-feedback dye laser with an organic–inorganic microcavity

We present a diode-pumped microcavity dye laser composed of a top organic reflector and a bottom inorganic reflector. The top organic reflector consists of alternate thin films of cellulose acetate and poly(N-vinylcarbazole) doped with coumarin 540A to construct a distributed-feedback (DFB) resonator. Pumped directly by an InGaN-based blue laser diode (LD) with a pulse duration of 4 ns, the microcavity dye laser exhibited a single-mode oscillation at 563 nm with a threshold pump LD power of 290 mW/pulse. The emission of the microcavity dye laser was measured through an optical fiber, resulting in a peak power of 2.5 mW for a pump LD power of 320 mW. PACS  42.55.Mv; 42.55.Sa; 42.55.Xi     

Development of a tunable IR lidar system

A differential absorption lidar system (DIAL) based on a continuously tunable optical parametric amplifier (OPA) pumped by a Nd : YAG laser (200 mJ at λ=355 nm) operating at a maximum pulse repetition rate of 100 Hz has been developed. The system provides continuously tunable coherent radiation in the Visible–near IR range (0.4–2.5 μm), allowing to perform DIAL measurements in a spectral region where most of atmospheric constituents and pollutants display absorption lines. The spectral width of the OPA system is line-narrowed by using a master oscillator dye laser as seeder, achieving a linewidth of 0.04 cm⁻¹ (FWHM), a spectral purity larger than 99% and a frequency stability better than 1 pm h⁻¹, with an output energy in the IR of 1–10 mJ. The OPA system was used to perform DIAL measurements in the lower troposphere. Preliminary results in terms of water vapor content and aerosol backscattering profiles are presented and discussed.     

All organic DFB laser enhanced by intermediate high refractive index polymer layer

Performances of a distributed feedback (DFB) organic dye laser were enhanced by introducing an intermediate high refractive index layer of poly(N-vinylcarbazole) (PVCz) laminated between a glass substrate and a laser dye doped active polymer layer. The active layer is consisted of rhodamine 6G and cellulose acetate (CA). Introduction of an intermediate layer allows a single mode lasing. Slope efficiencies of 2.2 and 4.7% and thresholds of 0.3 and 0.14 mJ/cm²/pulse were measured for the waveguides with 1.7 and 3.4 μm active layers, respectively. Furthermore, permanent relief grating on an intermediate layer gave rise to the reduction of the threshold. With increasing in amplitude of the relief grating from 20 to 45 nm, lasing threshold was reduced from 0.18 to 0.04 mJ/cm²/pulse for the waveguide with 1.7 μm active layer. The slope efficiency increased from 3.5 to 4.2%.     

Expansion velocities of 0.5 ps KrF excimer laser induced plasma by Doppler-shift analysis of pump and probe measurements

High gradient laser plasma is formed by focused KrF laser pulses (248.3 nm, 450 fs, 10¹³ W/cm²) on liquids (water, styrene) and solids (silicon, aluminum, and polyimide). The hydrodynamic expansion of the plasma was studied by measuring the blue Doppler-shift of reflected probe pulses which was produced by a delayed dye laser (496.6 nm, 450 fs). The Doppler-shift corresponds to the velocity of the reflecting surface of the plasma which is defined by the critical electron density. Expansion is investigated as a function of delay time and laser intensity. The reflecting surface of the plasma accelerates over 1–2 ps after the onset of the ablating laser pulse. With increasing intensity up to 2×10¹³ W/cm² the maximum average velocities are monotonously increasing up to 1–2×10⁵ m/s. PACS 52.38.Kd; 52.50.Jm, 52.70.Kz     

Photophysical properties, laser activity and photoreactivity of a heteroaryl chalcone: A model of solvatochromic fluorophore

The absorption and fluorescence characteristics of 3-(4′-dimethylaminophenyl)-1-(2-thienyl)prop-2-en-1-one (DMATP) have been investigated in different solvents. DMATP dye exhibits a large red shift in both absorption and emission spectra as solvent polarity increases, indicating a large change in the dipole moment of molecules upon excitation due to an intramolecular charge transfer interaction. The fluorescence quantum yield depends strongly on the properties of the solvents, which was attributed to positive and negative solvatokinetic effects. A crystalline solid of DMATP gave an excimer like emission at 570 nm due to the excitation of molecular aggregates. This is expected from the idealized crystal structure of the dye that belongs to the B-type class of Steven's classification. A dye solution ca. 10⁻³ mol dm⁻³ in CHCl₃ gave a good laser emission in the range 480–560 nm with emission maximum at 530 nm upon pumping by nitrogen laser (λ_ex=337.1 nm). The excitation energy transfer from 7-dimethylamino-4-methyl coumarine (DMC) to DMATP has been also studied in CHCl₃ and the values of energy transfer rate constant and critical transfer distance indicate a Főrster-type mechanism. The photoreactivity and net photochemical quantum yield of DMATP in chloromethane solvents are also determined. We applied semiempirical MO calculation using AMI and ZINO/S calculation to understand the geometric and electronic structure of DMATP molecule in both ground and excited states.     

Orange,red and deep-red flashlamp-pumped Pr3+:LiYF4 laser with improved output energy and efficiency

Three laser transitions (607.2 nm, 639.5 nm, 720.9 nm) in a flashlamp-pumped Pr³⁺:LiYF₄ laser at room temperature are investigated. Cerium ions (Ce³⁺) doped into the fused-quartz envelope of the flashlamp efficiently transfer strong UV radiation from pumping light into the absorption region of Pr³⁺ ions ( = 420–480 nm), so that the slope efficiency of all three laser emissions could be increased by almost 100% compared to excitation with a pure quartz flashlamp. At a pump energy of 30 J the output energy of these three laser emissions reached 4.7 mJ, 87 mJ and 30 mJ.     

Visible-to-near infrared standard source generation using acetylene (C2H2)-stabilized comb-injection-locked technique

An ultra-stable visible laser source (VLS) was generated by the second harmonic of a selectively injection-locked distributed feedback (DFB) laser from an optical frequency comb with acetylene-stabilized laser seeding. For the second-harmonic generation (SHG) of the injection-locked DFB laser, we used periodically poled lithium niobate (PPLN) crystal and generated the VLS at a region of 771 nm, which was discretely locked to a spacing of 25 GHz within the PPLN bandwidth (180 GHz). The frequency stability of this source was estimated to be 1.1 × 10^− 12 with an average time of 1 s.