Highly efficient and photostable solid-state dye lasers based on modified copolymers doped with PM567

Solid-state dye samples based on modified copolymers of methyl methacrylate (MMA) and 2-hydroxyethyl methacrylate (HEMA) with methanol doped with PM567 were first prepared. The volume proportions of methanol have great effects on the laser's characteristics including spectra, lasing output and thermal properties. The highest slope efficiency of 64.25% was achieved in the sample MP (MMA:HEMA = 85:15 + 10% methanol). Pumping the samples at a repetition rate of 5 Hz with a pulse energy as high as 100 mJ (the fluence was 0.26 J/cm²), the maximum lifetime of 278,000 shots was obtained in the sample MP (MMA:HEMA = 85:15 + 15% methanol), and the corresponding normalized photostability reached 180.7 GJ/mol. The obtained ten-shots damage thresholds were as high as 6.7 J/cm². The results indicate that the laser properties of solid-state dyes can be greatly enhanced by using modified copolymers of MMA and HEMA with methanol as solid hosts.     

Photophysical parameters and fluorescence quenching of 7-diethylaminocoumarin (DEAC) laser dye

The optical properties including electronic absorption spectrum, emission spectrum, fluorescence quantum yield, and dipole moment of electronic transition of 7-diethylaminocoumarin (DEAC) laser dye have been measured in different solvents. Both electronic absorption and fluorescence spectra are red shifted as the polarity of the medium increases, indicating that the dipole moment of molecule increases on excitation. The fluorescence quantum yield of DEAC decreases as the polarity of solvent increases, a result of the role of solvent polarity in stabilization of the twisting of the intramolecular charge transfer (TICT) in excited state, which is a non-emissive state, as well as hydrogen bonding with the hetero-atom of dye. The emission spectrum of DEAC has also been measured in cationic (CTAC) and anionic (SDS) micelles, the intensity increases as the concentration of surfactant increases, and an abrupt change in emission intensity is observed at critical micelle concentration (CMC) of surfactant. 2×10⁻³ mol dm⁻³ of DEAC gives laser emission in the blue region on pumping with nitrogen laser (λ_ex=337.1 nm). The laser parameters such as tuning range, gain coefficient (α), emission cross section (σ_e), and half-life energy have been calculated in different solvents, namely acetone, dioxane , ethanol, and dimethyforamide (DMF). The photoreactivity of DEAC has been studied in CCl₄ at a wavelength of 366 nm. The values of photochemical yield (?_c) and rate constant (k) are determined. The interaction of organic acceptors such as picric acid (PA), tetracyanoethylene (TCNE), and 7,7,8,8-tetracynoquinonedimethane (TCNQ) with DEAC is also studied using fluorescence measurements in acetonitrile (CH₃CN); from fluorescence quenching study we assume the possible electron transfer from excited donor DEAC to organic acceptor forming non-emissive exciplex.     

Spectroscopic properties and amplified spontaneous emission of a new derivative of fluorescein

The new laser dye, 2-(6-acryloyloxy-3-oxo-3H-xanthen-9-yl)-benzoic acid ethyl ester [AOXBE] has been synthesized. Its chemical structure was confirmed by ¹HNMR, IR, MS and elemental analysis. This new dye was covalently bonded with methyl methacrylate (MMA) and 2-hydroxy ethyl-methacrylate (HEMA) copolymer backbone. Its optical properties were experimentally investigated. Amplified spontaneous emission (ASE) and photostability were studied by pumping the dye polymeric sample with a 355 nm (8 ns) pulsed Nd:YAG laser. PACS 42.55.Mv; 42.70.Hj; 42.70.Jk; 42.55.Px     

An efficient lasing action from pyrromethene 556 dye-doped organically modified silicates

Organically modified solid-state silicates (ORMOSILS) doped with a new laser dye 1,3,5,7,8-pentamethylpyrromethene-2,6-disulfonate-BF₂ complex (pyrromethene 556) have been synthesized by a sol-gel method and the compositional effects on pore characteristics, fluorescence and lasing properties have been investigated. It is found that the use of dimethylsulfoxide and γ-glycidoxypropyltrimethoxysilane could greatly change the structure properties of sol-gel derived ORMOSILS cage, and thus the fluorescence and lasing properties of the materials could improve significantly. A successful laser oscillation from this dye-doped ORMOSILS sample has been achieved upon pumping with a Q-switched frequency-doubled Nd:YAG laser at 532 nm. A slope efficiency of 54% with a useful lifetime greater than 10,000 shots has been demonstrated at a pump repetition rate of 1 Hz and a pump intensity of 1 J/cm² by using the new ORMOSILS cage on our newly designed laser system. Our results have shown that it is possible to obtain a high-efficiency with a long-lifetime for a compact new laser device by low cost dye-doped solid-state ORMOSILS.     

Efficient lasing action from Rhodamine-110 (Rh-110) impregnated sol-gel silica samples prepared by dip method

Rhodamine-110/sol-gel samples are prepared by sol-gel technique using dip method. Concentration dependent photophysical studies of these samples have indicated about the least possibility of aggregate formation. The lasing action of Rh-110 in silica samples is studied as a function of dye concentration. An efficient laser emission is observed when the samples are transversely pumped at 337.1 nm and 1.5 Hz repetition rate using a nitrogen laser (400 μJ energy/pulse and 4 ns pulse duration). The maximum of 166% laser efficiency of dye doped sol-gel samples compared to Rhodamine-6G (Rh-6G) in methanol is achieved. The photostability is also measured by using N₂ laser at 1 Hz and it is found nearly 165 pulses. The possible reasons for the photodegradation of the dye molecules are discussed in detail.     

Femtosecond pulsed laser deposition of diamond-like carbon films: The effect of double laser pulses

The bonding structure of carbon films prepared by pulsed laser deposition is determined by the plasma properties especially the change of the kinetic energy. Using double laser pulses the ablation process and the characteristics of the generated plasma can be controlled by the setting of the delay between the pulses. In our experiments, amorphous carbon films have been deposited in vacuum onto Si substrates by double pulses from a Ti:sapphire laser (180 fs, λ = 800 nm, at 1 kHz) and a KrF laser system (500 fs, λ = 248 nm, at 5 Hz). The intensities have been varied in the range of 3.4 × 10¹² to 2 × 10¹³ W/cm². The morphology and the main properties of the thin layers were investigated as a function of the time delay between the two ablating pulses (0-116.8 ps) and as a function of the irradiated area on the target surface. Atomic force microscopy, spectroscopic ellipsometry and Raman-spectroscopy were used to characterize the films. It was demonstrated that the change of the delay and the spot size results in the modification of the thickness distribution of the layers, and the carbon sp²/sp³ bonding ratio.     

Enhanced laser characteristics of pyrromethene 650 using modified PMMA as solid hosts

Solid-state samples based on modified polymethyl methacrylate (MPMMA) with methanol doped with the dye pyrromethene 650 (PM650) are prepared.The effects of a volume percentage of methanol on the laser characteristics of the sample,including spectra properties,slope efficiency,photostability and tunable properties,are investigated.The broadband dye laser output wavelength is around 655 nm and a highest slope efficiency of 32.23% is achieved.Pumping the samples at a repetition rate of 5 Hz with a pulse energy of as high as 100 mJ (the fluence is 0.26 J/cm 2),the longest lifetime (168000 shots) is obtained in the sample (MMA:methanol=18:2),and the corresponding normalized photostability reaches 109.19 GJ/mol.When the sample (MMA:methanol=18:2) is placed in a Shoshan-type oscilla-tor,the narrow-linewidth operation is a continuous tuning range (up to 64 nm).The results indicate that the laser characteristics of solid-state dyes can be greatly enhanced by using modified PMMA with methanol serving as the solid host.     

Measurements of the linewidth of a continuous-wave distributed feedback quantum cascade laser

Two-sample (Allan) variance with a modified algorithm was applied to the determination of the experimental linewidth of a thermoelectrically-cooled continuous-wave distributed feedback quantum cascade laser at a wavelength of 4.333 μm. From successive laser transmittance scans over the CO₂ ν₃, (01¹1 − 01¹0) P(33) absorption line at 2307.653 cm^− 1, two-sample variances were calculated for the laser frequency difference between different points on the sides of the absorption peak. From the minimum two-sample variance of the laser frequency difference between two adjacent points (5 μs between the points) on the same side of the absorption line the experimental laser linewidth was estimated to be less than 36(7) kHz at a laser power of ~ 25 mW, a laser current of 976 mA and a laser temperature of + 19.5 °C.     

Competition between green and infrared emission in Er:YLiF4 upconversion lasers

The competition between two laser transitions in Er:YLiF₄ (⁴S_3/2 → ⁴I_15/2 at 551 nm and ⁴S_3/2 → ⁴I_13/2 at 850 nm) is studied using a model based on rate equations. The laser emission is pumped by upconversion at 795 nm; for comparison, we also discuss upconversion pumping by another mechanism, at 970 nm. The conditions that favor laser emission in various regimes on these two transitions are found.     

Nonlinear optical properties of an azo-based dye irradiated by picosecond and nanosecond laser pulses

The nonlinear optical properties of an azo-based dye were investigated using Z-scan technique employing 38 ps pulses at 532 and 1064 nm, and 6 ns laser pulses at 532 nm. Large nonlinear absorption and nonlinear refraction were observed at both ps and ns 532 nm in the azoic dye. When excited at ps 1064 nm, this dye displayed a large two-photon absorption cross-section (σ₂=1810 GM). Meanwhile, the optical nonlinearity mechanism was discussed in terms of molecular structure, excitation wavelength, and pulse width.     

Mid-infrared polarization spectroscopy of C2H2: Non-intrusive spatial-resolved measurements of polyatomic hydrocarbon molecules for combustion diagnostics

Polarization spectroscopy in the mid-infrared (IRPS) has been applied to the detection of acetylene molecules making use of the asymmetric C-H stretching vibration at around 3 μm. The infrared laser pulses were produced through difference frequency generation in a LiNbO₃ crystal pumped by a Nd:YAG and dye laser system. By directly probing the ro-vibrational transitions with IRPS, sensitive detection of molecules with otherwise inaccessible electronic states was realized with high temporal and spatial resolution by using a pulsed laser and a cross-beam geometry. Detection sensitivities of 2 × 10¹³ molecules/cm³ (10 ppm in 70 mbar gas mixture) of C₂H₂ were achieved using the P(1 1) line of the (0 1 0(1 1)⁰)-(0 0 0 0⁰ 0⁰) band. The dependence of the IRPS signal on the pump laser fluence, acetylene mole fraction, and buffer gas pressure of Ar, N₂, H₂, and CO₂ has been studied experimentally. The investigation demonstrates the quantitative nature of IRPS for sensitive detection of polyatomic IR active molecules. In order to fully demonstrate the technique for combustion applications, nascent acetylene molecules were measured in a low pressure methane/oxygen flame.     

Photoluminescence of PMMA doped with fluorescein and carbosilane dendrimer and lasing in PBG resonance cavity

Carbosilane dendrimers with terminal allyl groups were synthesized and used to encapsulate the allyl derivative of fluorescein (allyl-FL) doped in PMMA. The optical property of this system was investigated and the results showed that the concentration of allyl-FL in PMMA could be increased to 4.5 wt% without decrease of the luminescence efficiency by adding the dendrimer into the system. The allyl-FL/dendrimer/PMMA film was embedded into a resonance cavity composed of two pieces of photonic band gap (PBG) materials to form a new-type solid-state laser. A laser emission at 589 nm was obtained when excited with a third harmonic generation (THG) of a pulsed Nd:YAG laser (355 nm) and its full-width at half-maximum of the spectrum was 1.7 nm.     

Fabrication of p-type Li-doped ZnO films by pulsed laser deposition

p-Type ZnO thin films have been realized via doping Li as acceptor by using pulsed laser deposition. In our experiment, Li₂CO₃ was used as Li precursor, and the growth temperature was varied from 400 to 600 °C in pure O₂ ambient. The Li-doped ZnO film prepared at 450 °C possessed the lowest resistivity of 34 Ω cm with a Hall mobility of 0.134 cm² V⁻¹ s⁻¹ and hole concentration of 1.37 × 10¹⁸ cm⁻³. X-ray diffraction (XRD) measurements showed that the Li-doped ZnO films grown at different substrate temperatures were of completely (0 0 2)-preferred orientation.     

Surface texturing of the carbon steel AISI 1045 using femtosecond laser in single pulse and scanning regime

Surface texturing of the metals, including steels, gained a new dimension with the appearance of femtosecond lasers. These laser systems enable highly precise modifications, which are very important for numerous applications of metals. The effects of a Ti:sapphire femtosecond laser with the pulse duration of 160 fs, operating at 775 nm wavelength and in two operational regimes - single pulse (SP) and scanning regime, on a high quality AISI 1045 carbon steel were studied. The estimated surface damage threshold was 0.22 J/cm² (SP). Surface modification was studied for the laser fluences of 0.66, 1.48 and 2.37 J/cm². The fluence of 0.66 J/cm², in both working regimes, induced texturing of the material, i.e. formation of periodic surface structures (PSS). Their periodicity was in accordance with the used laser wavelength. Finally, changes in the surface oxygen content caused by ultrashort laser pulses were recorded.     

Luminescent sensitization and blue shift emission of Ir(ppy)2(VPHD) by copolymerization with MMA

Ir(ppy)₂(VPHD) (ppy=2-phenyl pyridine, VPHD=6-(4-vinylphenyl)-2,4-hexanedione) was copolymerized with methyl methacrylate (MMA). The copolymer had high quantum yield of 52.3±0.5% in dilute ethyl acetate solution, and the yield increased around 45% than that of the iridium monomer. The maximum emission peaks for the copolymers shifted from 515 to 489 nm while the iridium complex content was less than 0.005 mol% in the feed. The blue emission at 489 nm and the green emission at 520 nm were analyzed by Lorenz function. They are attributed to ¹MLCT and ³MLCT emissions, respectively.     

Highly efficient Nd:GdVO4/BiBO laser at 456 nm under direct 880 nm diode laser pumping

The continuous-wave high-efficiency laser emission of Nd:GdVO₄ at the second-harmonic of 456 nm obtained by intracavity frequency doubling with an BiB₃O₆(BiBO) nonlinear crystal is investigated under pumping by diode laser at 880 nm into emitting level ⁴F_3/2. About 3.8 W at 456 nm with M² = 1.4 was obtained from a 5 mm-thick 0.4 at.% Nd:GdVO₄ laser medium and a 12 mm-long BiBO nonlinear crystal in a Z-type cavity for 13.9 W absorbed pump power. An optical-to-optical efficiency with respect to the absorbed pump power was 0.274. Comparative results obtained for the pump with diode laser at 808 nm, into the highly-absorbing ⁴F_5/2 level, are given in order to prove the advantages of the 880 nm wavelength pumping.     

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.     

Radio-frequency assisted pulsed laser deposition of nanostructured WOx films

The synthesis of tungsten oxide films with large surface area is promising for gas sensing applications. Thin WO_x films were obtained by radio-frequency assisted pulsed laser deposition (RF-PLD). A tungsten target was ablated at 700 and 900 Pa in reactive oxygen, or in a 50% mixed oxygen-helium atmosphere at the same total pressure values. Corning glass was used as substrate, at temperatures including 673, 773 and 873 K. Other deposition parameters such as laser fluence (4.5 J cm⁻²), laser wavelength (355 nm), radiofrequency power (150 W), target to substrate distance (4 cm), laser spot area (0.7 mm²), and number of laser shots (12,000) were kept fixed. The sensitivity on the deposition conditions of morphology, nanostructure, bond coordination, and roughness of the obtained films were analyzed by scanning and transmission electron microscopy, micro-Raman spectroscopy, and atomic force microscopy.     

Single beam Z-scan measurement of the third order optical nonlinearities of styryl7 dye

The optical nonlinearity of styryl7 dye in ethanol solution at different concentrations has been studied using pulsed Nd:YAG laser at 532 nm as the source of excitation. The optical responses were characterized by measuring the intensity dependent refractive index (n₂) of the medium using the Z-scan technique. The open aperture Z-scan trace of the dye in solution displayed saturable absorption. The closed aperture Z-scan trace of the dye exhibited a negative nonlinearity. The styryl7 dye at 1 mM concentration exhibited nonlinear refractive co-efficient n₂ = −1.24 × 10⁻⁸ cm²/W, nonlinear absorption coefficient β = − 3.9 × 10⁻⁴ cm/W and real and imaginary parts of third-order nonlinear optical susceptibility χ³ = 3.26 × 10⁻⁶ esu in ethanol. These results showed that the dye has potential application in nonlinear optics.     

Electric field induced hyperfine level-crossings in (nD)Cs at two-step laser excitation: Experiment and theory

The pure electric field level-crossing of m_F Zeeman sublevels of hyperfine F levels at two-step laser excitation is described theoretically and studied experimentally for the nD_3/2 states in Cs with n = 7, 9 and 10, by applying a diode laser in the first 6S_1/2 → 6P_3/2 step and a diode or dye laser for the second 6P_3/2 → nD_3/2 step. Level-crossing resonance signals are observed in the nD_3/2 → 6P_1/2 fluorescence. A theoretical model is presented to describe quantitatively the resonance signals by correlation analysis of the optical Bloch equations in the case when an atom simultaneously interacts with two laser fields in the presence of an external dc electric field. The simulations describe well the experimental signals. The tensor polarizabilities α₂ (in ) are determined to be 7.45(20) × 10⁴ for the 7D_3/2 state and 1.183(35) × 10⁶ for the 9D_3/2 state; the electric field calibration is based on measurements of the 10D_3/2 state, for which α₂ is well established. The α₂ value for the 7D_3/2 state differs by ca. 15% from the existing experimentally measured value.