Anti-stokes fluorescence of polymethine dyes excited by a titanium-sapphire laser

Fluorescence of symmetric polymethine dye solutions (λ _abs ^max ≈ 700 nm) upon anti-Stokes excitation by cw radiation of a titanium-sapphire laser (781 nm) is first investigated. A series of six compounds with analogous composition and spectral and luminescent properties is investigated. It is demonstrated that in addition to the anti-Stokes component, the Stokes component with a maximum at 820 nm (referred to the H-aggregates of initial dyes) is observed in the fluorescence spectra of solutions of the examined molecules when dye concentration increases to 10⁻³ M. Dependences of the anti-Stokes and Stokes component intensities on the exciting radiation power are obtained that confirm a linear excitation character. On examples of xanthene and polymethine dyes, the use of organic fluorophors for anti-Stokes laser cooling and some other possible applications of the anti-Stokes fluorescence are discussed. __________ Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 3, pp. 63–70, March, 2007.     

Phototransformations of substituted <Emphasis Type="Italic">p</Emphasis>-terphenyl upon excitation by a XeCl laser

Phototransformations of 1,8-dicarboxyisobutyl-substituted p-terphenyl in ethanol are studied upon excitation by a XeCl laser at a power density of up to 180 MW/cm² for different types of radiation and different excitation geometries. The absorption and emission spectra are studied before and after irradiation. The resources of the lasing medium, quantum yields of phototransformations, and relative quantum yields of photoproducts are determined. The transmission of the solutions at the excitation wavelength and the shape of radiation pulses are measured as functions of the pump power density.     

Specific Features of XeCl*-Laser Radiation Absorption by Concentrated Solutions of Organic Dyes

The transmission of focused laser radiation with power densities in the range (1–250) MW/cm² through solutions of laser dyes (substituted paraterphenyls and rhodamine 6G) is investigated. The dependence of the transmission on the exciting radiation power density is measured, and numerical modeling is used to estimate the lifetime of the fluorescent state of molecules and the influence of stimulated emission on the lifetime of the S ₁ state. The effect of scattering on the transmission of highly absorbing media is demonstrated under nanosecond excitation.     

Specific features of the two-photon absorption of cationic symmetric polymethine dyes

The two-photon absorption of a number of cationic symmetric polymethine dyes based on 3H-indolium and benzothiazolium is experimentally studied upon excitation by nanosecond radiation from a Nd:YAG laser (1064 nm, 12 ns). The two-photon absorption cross section of dye molecules is determined by the two-quantum standard method. The influence of the spectral-luminescent properties and structure of the polymethine dyes on the two-photon absorption cross section is discussed. It is shown that, upon excitation in the range of the long-wavelength band of the dyes studied (the S ₀ → S ₁ transition), the maximum of their two-photon absorption is blue shifted. The reasons for a considerable increase in the two-photon absorption of symmetric polymethine dyes upon their excitation in the range of the S ₂ state are discussed. Using the data of quantum-chemical calculations, it is shown that, along with changes in the selection rules for two-photon transitions, this increase is connected with an increase in the size of the delocalized π electron cloud of HOMOs involved in the S ₀ → S ₂ transition.     

The effect of two-photon absorption and optical excitation area on the generation of THz radiation

It was found experimentally that the THz radiation throughput based on optical rectification is strongly related to the optical excitation size in a ZeTe emitter. The factors affecting the THz radiation throughput are investigated in detail both experimentally and theoretically. By taking into account optical rectification, diffraction and two-photon absorption effects, a theoretical model is established to describe the emitting field intensity of THz radiation. There is excellent agreement between the theoretical results and the experimental data under high excitation power. Both theoretical and experimental results demonstrate that there is a trade-off between these three effects for THz radiation, and that in order to increase the THz radiation throughput based on optical rectification, one should choose suitable excitation size under a given pump power.     

Upconversion CW laser at 284 nm in a Nd:YAG-pumped double-cladding thulium-doped ZBLAN fiber laser

A successful continuous-wave (CW) ultraviolet (UV) laser in a Tm⁺³-doped ZBLAN fiber, operated at 284 nm (¹ I ₆ → ³ H ₆ transition of Tm⁺³) is demonstrated. The excitation uses a four-step upconversion scheme. The pump source is a Nd:YAG laser operated at 1.064 μm. A laser output power of 42 μW continuous wave was obtained for 590 mW of the launched pump power. The slope efficiency with respect to the launched pump power was measured to be 9%. Ultraviolet (at 365 nm) and visible (at 453 and 480 nm) radiation was also observed.     

Spectroscopic and laser properties of photoexcited organic fluorescers embedded in composite gel systems

The spectral luminescence and lasing characteristics of rhodamine 101T and phenalemine 512 embedded in simple and composite gel matrices of different compositions based on tetraethoxysilane were excited by XeCl laser radiation and the second harmonic of a Nd:YAG laser. It is established that a dye interacts with a solid matrix through formation of donor-acceptor and hydrogen-bonded solvates. The dependence of the lasing efficiency on the excitation intensity was determined, as well as the laser photostability of gel systems with dyes. It is shown that the pump conversion efficiency and the laser photostability of dyes in composite gel systems are higher than in simple gel matrices.     

Limiting the intensity of femtosecond pulses with anti-stokes excitation of organic dye solutions

Results of experimental investigations into the nonlinear absorption of the symmetric polymethine 1-butyl -3,3-dimethyl-2-[5-(1-butyl-3,3-dimethyl-3H-benz[e]indoline-2-uledene)-1,3-pentadienyl]-3H-benz[e]indolium perchlorate dye solution excited by radiation of a femtosecond titanium-sapphire laser (20 fs, 800 nm, 75 MHz, and 300 mW) by the open aperture z-scan method are presented. Record limitation of the femtosecond laser radiation intensity (by 300 times at a 93% linear transmission of the medium) was achieved. The nonlinear absorption mechanisms in organic dyes with anti-Stokes excitation by wideband high-power pulsed radiation to the absorption band edge and the prospects for organic dye application for limitation of the femtosecond laser radiation intensity are discussed.     

Electronic excitation dynamics and energy transfer in lithium-gadolinium borates doped by rare earths

This paper reports on luminescence studies of lithium borate Li₆Gd(BO₃)₃ doped with Eu³⁺ and Ce³⁺ and Li₆Eu(BO₃)₃ crystals upon selective excitation by synchronous radiation in the pump energy region 3.7–27 eV at temperatures of 10 and 290 K. The effective energy transfer between the rare-earth ions Gd³⁺ → Ce³⁺ and Gd³⁺ → Eu³⁺ is found to operate by the resonant mechanism, as well as through electron-hole recombination. A study is made of the fast decay kinetics of the Ce³⁺-center activator luminescence under intracenter photoexcitation and excitation in the interband transition region. The mechanisms underlying luminescence excitation and radiative relaxation of electron states of rare-earth ions are analyzed and energy transfer processes active in these crystals are discussed.     

Generation of nanosecond terahertz pulses by the optical rectification method

The possibility of the generation of quasi-cw terahertz radiation by the optical rectification method for broad-band Fourier unlimited nanosecond laser pulses has been experimentally demonstrated. The broadband radiation of a LiF dye-center laser is used as a pump source of a nonlinear optical oscillator. The energy efficiency of terahertz optical frequency conversion in a periodically polarized lithium niobate crystal is 4 × 10⁻⁹ at a pump power density of 7 MW/cm².     

On the excitation mechanisms of the infrared-excited visible luminescence in Yb,Er-doped fluorides

Lattices doped with Yb³⁺ and Er³⁺ can be excited by infrared radiation (970 nm) to give green and red emission. Information upon the excitation mechanisms of the infrared-excited visible luminescence is obtained from the emission spectra under 365 nm and under 970 nm excitation and from the excitation spectra of the green and red emission in the excitation region between 350 nm and 500 nm. This is demonstrated for a number of Yb³⁺, Er³⁺-doped fluorides showing a high infrared-to-visible conversion efficiency.     

香豆素440/荧光素钠/藏红混合染料体系的光谱研究

通过对C440/Fl.Na/Saf.-T三元混合染料体系的荧光光谱研究,了解到这三种染料之间有较充分的能量转移。又通过对C440/Fl.Na和Fl.Na/Saf.-T两个混合染料体系的荧光寿命测量,讨论了分子间能量转移过程和机理,并做了一些定量的分析。     

One- and two-barrier excilamps on xenon dimers operating in the VUV range

Spontaneous emission sources in the VUV range based on one- and two-barrier pulsed-periodic gas (Xe) discharges are experimentally investigated. Volt-coulomb figures, as well as typical waveforms of current pulses and discharge voltage are presented. The time dependences of the voltage drop across the gas-discharge plasma, excitation power, and excitation energy are calculated. The radiation power versus xenon pressure, exciting pulse repetition rate, and average excitation power is determined. The radiation power average densities for one- and two-barrier excilamps are found to be 20–30 and ～40 mW/cm², respectively.     

Stationary generation of diode-pumped self-Raman Nd:YVO<Subscript>4</Subscript>/YVO<Subscript>4</Subscript> composite crystal laser

Output power dependences of composite Nd³⁺:YVO₄ Raman laser stationary generation on the longitudinal diode pump power are measured at different transmissions of the output mirror at the Stokes radiation frequency. The deviation of the measured dependences from linear is explained by the influence of thermal effects on both the overlap of the beams and diffraction losses. A method to estimate the laser and Stokes losses in the cavity and the parameters characterizing the overlap of the laser radiation with the pump and Stokes beams is proposed. A Stokes-component of power 2.1 W is obtained and corresponds to 12% diode-to-Stokes efficiency.     

Effect of the pump absorption on generation of infrared stimulated electronic Raman scattering in alkali-metal vapors

The main properties of infrared stimulated electronic Raman scattering (SERS) at the 6² S _1/2-7² S _{1/2, 3/2} transitions in cesium atoms are studied theoretically and experimentally as functions of the atomic concentration, which was varied from 10¹¹ to 10¹⁶ cm^?3. It is found that the efficiency of generation of Stokes radiation strongly depends on one-photon absorption of the pump radiation tuned near frequencies of the 6² S _1/2-7² P _{1/2, 3/2} transitions. By using the equation for the density matrix, which describes the evolution of a three-level system, the theory of resonance excitation of IR radiation upon one-photon absorption at an adjacent transition is developed. The theory describes well the main features of IR SERS in alkali-metal vapors.     

三芳胺和二氢吲哚作为给体的染料对钴电解质的染料敏化太阳能电池性能的影响

合成了两种有机染料,三芳胺染料XS51和二氢吲哚染料XS52,并分别用于钴基电解质和碘基电解质的染料敏化太阳能电池中. 考察了染料结构对光物理性能、电化学性能和电池性能的影响. XS51为含有四个己氧基的三芳胺结构,表现出较好的空间位阻,从而提高了光电压. XS52中二氢吲哚的给电子能力强,从而短路电流较大. 同碘电解质相比,所合成的染料更适合用于钴电解质的染料敏化电池中. 在100 mW/cm²的光强下,基于染料XS52的钴电解质太阳能电池总的光电转换效率达到6.58%.     

Kinetics of photoluminescence decay of KCl-Yb

We have investigated the kinetics of the luminescence decay of a KCl-Yb crystal excited in one of the long-wavelength absorption bands of the Yb²⁺ ion by nitrogen laser radiation with a power density less than 10³ W/cm². We found that, in both luminescence bands, both the one associated with the allowed transition (399 nm) and the one associated with the forbidden transition (430 nm), there are two stages of decay—an initial exponential stage that gives way to a hyperbolic stage. Non-exponential decay due to the optical electron tunneling back to the luminescence center is treated as evidence of delocalization of the electron upon intracenter excitation and is explained by the formation of an excimer-like molecular bond upon photoexcitation of the crystal. Fiz. Tverd. Tela (St. Petersburg) 41, 1763–1765 (October 1999)     

Blue up-conversion with excitation into Tm ions at 808 nm in YVO4 crystals co-doped with thulium and ytterbium

The up-conversion of infrared radiation at 808 nm, emitted by a diode laser, into blue emission centered at 480 nm in 1 at.% Tm, 5 at.% Yb: YVO₄; 1 at.% Tm, 8 at.% Yb: YVO₄ and 2 at.% Tm, 5 at.% Yb: YVO₄ has been studied. The highest intensity of blue emission is found for the 1 at.% Tm, 8 at.%Yb: YVO₄ system. The power dependence of up-converted emission upon continuous-wave excitation as well as the time evolution of its intensity upon short-pulse excitation were found to be consistent with a two-step excitation mechanism in which the forward Tm³⁺–Yb³⁺ energy transfer is followed by the back Yb³⁺–Tm³⁺ energy transfer. The effect of dopant concentrations on the up-conversion process is interpreted taking into account dynamics of the excited states involved.     

Non-collinear nanosecond optical parametric oscillator based on periodically poled LN with tilted domain walls

We report on a non-collinear, 1064 nm pumped, 10 kHz repetition rate ns-OPO which consists of a 13 mm long periodically poled lithium niobate (PPLN) crystal in a hemispherical optical cavity. The non-collinear phase-matching is achieved by tilting the domains by 60° with respect to the pump beam. This phase-matching avoids back conversion of signal and idler radiation into pump radiation and thus improves the spatial quality of the generated OPO radiation considerably. At a pump power of 5.5 W the OPO provided a conversion efficiency of up to 34%. The generated OPO pulses with a total power of up to 1.85 W were emitted in an almost diffraction limited beam with a M²-value of 1.1. The beam quality did not change when the pump power was varied in the range of 2–5 W. PACS 42.65.-k; 42.65.Yj