Effects of light quenching on the emission spectra and intensity decays of fluorophore mixtures

We examined a series of fluorophore mixtures to determine the wavelength selectivity of light quenching and the effects of light quenching on the emission spectra and intensity decays. Light quenching can be accomplished using a single excitation pulse train and quenching wavelength (one-beam) or with longer-wavelength quenching pulses time-delayed relative to the excitation pulses (two-beam). Both one-beam and two-beam light quenching were found to alter the intensity decays of the mixtures. The frequency-domain intensity decay data were analyzed to reveal the fractional intensity of each fluorophore in the mixture and the effects of light quenching on the fractional contribution of each fluorophore to the total intensity. Fluorophores were selected to provide a range of decay times and emission wavelengths. The extent of quenching in the mixtures was dependent on which fluorophore had the higher radiative decay rate and emission intensity at the quenching wavelength. A general theory is presented which describes the intensity decays in terms of the extent of quenching of each fluorophore and the time delay between excitation and quenching pulses. The effects of light quenching on the fractional intensities of each fluorophore in the mixture, recovered from the intensity decay analysis, were found to be in quantitative agreement with that predicted from steady-state measurements of light quenching and from the spectral properties of the fluorophores. The data on light quenching of mixtures demonstrate that light quenching may be used for selective quenching of fluorophores and thus of potential value for studies of multichromophoric systems.     

Polarization Kinetics of the Fluorescence of Solutions of Complex Molecules Undergoing Impulse Optical Quenching

The influence of optical quenching on the polarization of the integral (in time) fluorescence of solutions of complex molecules using picosecond pulses has been investigated theoretically. The resulting dependences of the degree of polarization on the time shift of pulses for the case of a thin layer of a medium (with no regard for the change in the intensity of the pulses) are in qualitative agreement with the results obtained for quasistationary excitation. A calculation has been made for the case of an extended medium with regard for the amplification of the quenching pulse. It is shown that scanning of the degree of polarization along the length of the cuvette makes it possible to obtain additional information on the mechanism of optical quenching in solutions and on the routes of deactivation of the energy of the molecule's excited state.     

The optical limitation effect and features of luminescence kinetics in hybrid nanosystems with CdSe/ZnS quantum dots and organic agents

The optical limitation effect in three-component systems formed in colloidal solutions of semiconductor CdSe/ZnS quantum dots with participation of fullerene C₆₀ and perylene, has been experimentally investigated. The first and second harmonics of a YAG:Nd³⁺ laser operating in the single-shot mode with a pulse duration of 7 ns and laser pulses subjected to stimulated Brillouin scattering (SBS)-stimulated Raman scattering (SRS) compression with a duration of about 20 ps near 560 nm have been used as radiation sources. It is shown that the optical limitation efficiency in the systems studied is determined by electron transfer. This is confirmed by the analysis of luminescence quenching.     

Anisotropy Spectra of the Solvent-Sensitive Fluorophore 4-Dimethylamino-4′-Cyanostilbene in the Presence of Light Quenching

We examined the emission wavelength-dependent anisotropies of the solvent-sensitive fluorophore 4-dimethylamino-4-cyanostilbene (DCS) under conditions of light quenching by polarized time-delayed quenching pulses. Illumination on the long-wavelength side of the emission spectrum with time-delayed light pulses resulted in a progressive decrease in the emission anisotropy as the observation wavelength increased toward the stimulating wavelength. The anisotropy changes of DCS were most wavelength dependent when spectral relaxation occurred during the excited-state lifetime. Light quenching of DCS in a low-viscosity solvent revealed no wavelength-dependent anisotropies. Control measurements using a solvent-insensitive fluorophore did not show any wavelength-dependent anisotropy with light quenching. The data for DCS can be explained by a model which allows wavelength-selective quenching of the long-wavelength emission formed by time-dependent spectral relaxation. These results indicate that polarized light quenching can be used to study systems which display multiple emissions and/or time-dependent spectral shifts.     

Generation of ultrashort electromagnetic radiation pulses with a repetition rate of ∼100 MHz by a vacuum photoemission element with an antimony cesium photocathode

We studied the generation of ultrashort electromagnetic radiation pulses with the maximal repetition rate by a vacuum photoemission element with an antimony cesium photocathode. Photoelectrons are emitted as a result of supplying four nanosecond initiating laser radiation pulses with a wavelength of 527 nm and an interval from 3.65 to 6.7 ns between the pulses. The voltage between the anode and the photocathode (from 5 to 60 kV) is measured in experiments.     

The Spectral Intensity of the Plasma of Single and Double Laser Pulses

We compare radiation of plasma flares produced on exposure of metals to laser radiation in a monopulse generation mode in the case of single and double pulses with change in air pressure. For double pulses, we established an increase in the duration and intensity of the radiation of spectral lines and also an analogy between the change in their intensities and those of single pulses obtained at a reduced air pressure.     

猝灭式染料激光器理论研究

理论上研究了由准分子激光泵浦的猝灭式染料激光器的猝灭机理，对于一些具体的泵浦情况，通过激光速率方程理论上探讨了激光器的猝灭效果，并且对激光器的一些重要参数进行了一些研究。     

用ICCD作光开关测量储存环中光学速调管谐波超辐射

 用高通断比ICCD作为快速光开关,在中国科学技术大学的800MeV电子储存环上建造了一套光学速调管谐波超辐射测量系统,从每隔106个自发辐射脉冲1个谐波超辐射脉冲所形成的脉冲链里选出超辐射脉冲,测量谐波辐射的相干增强因子和谱宽。     

Characteristic features of generation of few-cycle pulses in infrared and terahertz spectral ranges upon interaction of two femtosecond pulses of different frequencies in air

The results of a theoretical analysis of the generation of broadband radiation in the infrared and terahertz spectral ranges upon the excitation of plasma in air by two femtosecond pulses at the fundamental and second-harmonic frequencies of a Ti-sapphire laser are presented. It is found that the appearance of long-wavelength radiation in a strong field of pulses of different frequencies can be described in terms of strongly anharmonic oscillations of optical electrons, whereby electrons are pulled far away from their atoms; these oscillations are accompanied by cascade transitions of electrons from their ground state to a bound excited state, followed by a transition to the continuum. It is shown that the generated infrared and terahertz radiation appears in the form of pulses containing a few oscillations of the light field. The efficiency of terahertz generation varies periodically with an increase in the interaction length of the femtosecond pulses of different frequencies.     

The influence of phase fluctuations and phase modulation on two-photon fluorescence

In the present paper the two-photon fluorescence (TPF) quenching produced by ruby lasers in dye is calculated on the basis of an electronic energy level system adapted for the special conditions of Rhodamine 6G. The model used here takes into consideration the action of competing one-photon processes. It will be shown that the reversed profile of TPF quenching in the overlap region is produced by the superposition of pulses with a time-dependent fluctuating phase as well as with a determinate quadratically time-dependent phase.     

Undulators and generation of X-ray pulses in free-electron lasers with self-amplified spontaneous emission

The results of theoretical examination and comparative analysis of synchrotron radiation sources (specifically, undulators and X-ray free-electron lasers (FELs)) are presented. The problem of generation of shorter radiation pulses is prioritized; undulator systems and their corresponding FELs, which are considered to be the most promising in terms of generation of high-frequency ultrashort pulses of such radiation (in particular, in the X-ray range) are studied. The possibility of generation of higher harmonics is explored. The advantages and disadvantages of single-pass (with no reflecting elements) and multi-pass (with mirrors) FEL lasing schemes are revealed. The potential to reduce the duration of laser pulses produced by undulators and FELs and use them as sources of femtosecond pulses is investigated. The prospects for further development of X-ray free-electron lasers and the ways to improve the quality of their radiation with the given parameters are discussed.     

多脉冲激光增强太赫兹辐射的PIC模拟

 模拟了强激光和稀薄非均匀等离子体相互作用在界面辐射超强太赫兹波的物理过程,提出了利用多脉冲激光增强太赫兹辐射的方案,详细研究了多脉冲激光的脉冲个数（取１～４个）、脉冲间距等因素对太赫兹辐射功率和频率的影响。当入射激光包含4个脉冲时,辐射最强,此时的辐射功率是相同条件下单脉冲的6倍,可达到7.16 MW,辐射的太赫兹波的脉宽约为330 fs,总能量约为1 μJ。研究结果表明:多脉冲激光可以显著增强太赫兹辐射,且随着脉冲个数的增加,激起的电子静电波振幅变大,辐射功率也随之变大,直到尾流场饱和;当脉冲间距等于入射激光脉宽时辐射最强。     

Generation of ultrabroadband terahertz radiation under optical breakdown of air by two femtosecond pulses of different frequencies

Experimental results on the generation of terahertz (THz) electromagnetic radiation under ionization of air by femtosecond pulses at fundamental and second-harmonic frequencies of a Ti-sapphire laser are presented. The mean power of the generated THz radiation as a function of the time delay between two pulses of different frequencies is found to be quasi-periodical. Theoretically, we show that efficient generation of THz radiation is governed by the inertial part of the nonlinear response of the medium, which is determined by the dynamics of population of highly excited states with subsequent emission of electrons.     

Time-resolved laser-induced fluorescence of atomic nitrogen in afree-burning arc discharge

An experiment to detect ground-state atomic nitrogen in an atmospheric-pressure argon-nitrogen free-burning 200 A arc by time-resolved two-photon laser-induced fluorescence is described. The time decay of the fluorescence pulses showed that quenching of the laser-excited state is rapid. Upper bound estimates of the pulse-decay time were determined as a function of radius, and were found to be on the order of 1 ns, and to decrease with increasing radii. The implications of rapid quenching of the laser-excited state to the application of laser-induced fluorescence as a plasma diagnostic tool are discussed     

Selection of single,mode-locked CO2 laser pulses by semiconductor reflection switching

Reflection switching of high power, 10 μm radiation by optically induced carriers in a semiconductor has been achieved by irradiating germanium with 3 ns pulses of 1.06 μm radiation. This has permitted the selection of single mode-locked pulses of 10 μm radiation with energies in the 1–2 joule range.     

Few-cycle attosecond pulses via periodic resonance interaction with hydrogenlike atoms

We show that it is possible to produce nearly bandwidth-limited few-cycle attosecond pulses based on periodic resonance interaction of a quasi-monochromatic radiation with the bound states of hydrogenlike atoms. A periodic resonance is provided by a far-off-resonant laser field with intensity much below the atomic ionization threshold via periodic tunnel ionization from the excited states and adiabatic Stark splitting of the excited energy levels. Without external synchronization of the spectral components, it is possible to produce 135 as pulses at 13.5 nm in Li2?-plasma controlled by radiation of a mode-locked Nd:YAG laser, as well as 1.25 fs pulses at 122 nm in atomic hydrogen controlled by radiation of a CO? laser.     

Femtosecond terahertz radiation from femtoslicing at BESSY

Femtosecond far-infrared radiation pulses in the THz spectral range were observed as a consequence of the energy modulation of 1.7 GeV electrons by femtosecond laser pulses in the BESSY storage ring in order to generate femtosecond x-ray pulses ("femtoslicing"). In addition to being crucial for diagnostics of the laser-electron interaction, the THz radiation itself is useful for experiments where intense ultrashort THz pulses of well-defined temporal and spectral characteristics are required.     

Simultaneous one-dimensional fluorescence lifetime measurements of OH and CO in premixed flames

A method for simultaneous measurements of fluorescence lifetimes of two species along a line is described. The experimental setup is based on picosecond laser pulses from two tunable optical parametric generator/optical parametric amplifier systems together with a streak camera. With an appropriate optical time delay between the two laser pulses, whose wavelengths are tuned to excite two different species, laser-induced fluorescence can be both detected temporally and spatially resolved by the streak camera. Hence, our method enables one-dimensional imaging of fluorescence lifetimes of two species in the same streak camera recording. The concept is demonstrated for fluorescence lifetime measurements of CO and OH in a laminar methane/air flame on a Bunsen-type burner. Measurements were taken in flames with four different equivalence ratios, namely ? = 0.9, 1.0, 1.15, and 1.25. The measured one-dimensional lifetime profiles generally agree well with lifetimes calculated from quenching cross sections found in the literature and quencher concentrations predicted by the GRI 3.0 mechanism. For OH, there is a systematic deviation of approximately 30 % between calculated and measured lifetimes. It is found that this is mainly due to the adiabatic assumption regarding the flame and uncertainty in H₂O quenching cross section. This emphasizes the strength of measuring the quenching rates rather than relying on models. The measurement concept might be useful for single-shot measurements of fluorescence lifetimes of several species pairs of vital importance in combustion processes, hence allowing fluorescence signals to be corrected for quenching and ultimately yield quantitative concentration profiles.     

Complex resonance in Fresnel reflection of radiation pulses

The Fresnel reflection of radiation pulses with an exponential temporal amplitude profile is analyzed. The conditions for the relevance of the concept of reflectance at a complex frequency, the imaginary part of which determined the rate of time variation of the amplitude, are specified. For the radiation pulses under study, we demonstrate a complex resonance, i.e., an increase in the magnitude of reflectance for the complex frequency of incident radiation (trailing edge of a pulse) that approaches the complex frequency of natural oscillations of oscillators in the medium.     

Coherent transmittance quenching effect in thin films of polymer-dispersed ferroelectric liquid crystals

The conditions for vanishing of the coherent component of radiation transmitted through a monolayer of polymer-dispersed ferroelectric liquid-crystal droplets are found. The influence of polydispersity and disorientation of axes of semispherical droplets on the conditions of interference quenching is studied. It is shown that these factors cause a change in the average size and concentration of droplets for which the quenching effect is realized. Data on the contrast ratio and the modulation depth of a monolayer, determined from the coherent component of transmitted radiation, are presented. It is shown that these characteristics can be considerably improved under quenching conditions for a film of polymer-dispersed ferroelectric liquid-crystal droplets.