Two-photon-pumped amplified spontaneous emission and cavity lasing of an organic dye HEASPS in PHEMA polymer

Two-photon-absorption (TPA)-induced upconverted amplified spontaneous emission (ASE) and cavity lasing of a styrylpyridinium dye: trans-4-[p-(N-hydroxyethyl-N-ethylamino)styryl]-N-methylpyridinium p-toluene sulfonate (abbreviated as HEASPS) in poly(2-hydroxyethyl methacrylate) (abbreviated as PHEMA) polymer were observed under a picosecond pump condition. The spectral and temporal behaviors of TPA-induced fluorescence, ASE and cavity lasing were studied. The cavity lasing with a total oscillation time of more than 200 ps was achieved when pumped with 1064-nm, 50-ps laser irradiation. The population inversion could persist for three times longer than the duration of the pump pulse. The gain coefficients of the dye-doped polymer at various wavelengths were calculated based on cavity lasing spectra and one-photon fluorescence spectra. PACS 78.20.Ek; 42.65.Ky; 42.65.Re; 78.47.+p     

Investigation of the spontaneous emission rate of perylene dye molecules encapsulated into three-dimensional nanofibers via FLIM method

The decay dynamics of perylene dye molecules encapsulated in polymer nanofibers produced by electrospinning of polymethyl methacrylate are investigated using a confocal fluorescence lifetime imaging microscopy technique. Time-resolved experiments show that the fluorescence lifetime of perylene dye molecules is enhanced when the dye molecules are encapsulated in a three-dimensional photonic environment. It is hard to produce a sustainable host with exactly the same dimensions all the time during fabrication to accommodate dye molecules for enhancement of spontaneous emission rate. The electrospinning method allows us to have a control over fiber diameter. It is observed that the wavelength of monomer excitation of perylene dye molecules is too short to cause enhancement within nanofiber photonic environment of 330 nm diameters. However, when these nanofibers are doped with more concentrated perylene, in addition to monomer excitation, an excimer excitation is generated. This causes observation of the Purcell effect in the three-dimensional nanocylindrical photonic fiber geometry.     

Strong amplified spontaneous emission and lasing from a narrow-gap RF-excited Ar-He-Xe gas mixture

The performance of a RF excited cw atomic xenon laser at wavelengths of 2.03 μm and 2.65 μm was studied theoretically and experimentally as a function of electrode distance. Results for inter-electrode distances from 2 to 0.25 mm are presented. A high pumping rate resulted in strong 40 mW cw amplified spontaneous emission at 2.65 μm wavelength from the configuration with the smallest distance of 0.25 mm between the electrodes. The maximum laser output of 2.7 W (0.24 W/cm³) was obtained with an active medium volume of 2×15×370 mm³ whereas the maximum specific output of 1.9 W/cm³ was received for an active medium volume of 0.25×2.25×370 mm³. A fluid model of the RF discharge was developed to analyze the laser behavior for different distances between the electrodes. Received: 30 November 1999 / Revised version: 21 April 2000 / Published online: 6 September 2000     

Cooperative emission of dye molecules at high dephasing rates

The dependence of the emission of a concentrated (～10¹⁹ cm^?3 solution of Rhodamine C on the power density Φ of exciting laser radiation was studied. The emission intensity for the power density of exciting radiation above ～10²⁵ cm^?2 s^?1 was found to have a nearly quadratic dependence on the power density Φ, and this emission was interpreted as the cooperative spontaneous emission of a Dicke type. For Φ?10²⁵ cm^?2 s^?1, the emission intensity increased with increasing Φ according to the exponential law. This emission was interpreted as the amplified spontaneous emission. The spectra of cooperative emission depended on the pump radiation power only weakly. The absence of lasing in dye solutions at high concentrations, which is a well-known phenomenon, was shown to be caused by the development of the cooperative spontaneous emission and not by the concentration quenching, and the former process is more rapid than the latter.     

Laser cooling of molecules via single spontaneous emission

A general scheme for reducing the center-of-mass entropy is proposed. It is based on the repetition of a cycle, composed of three concepts: velocity selection, deceleration and irreversible accumulation. Well-known laser techniques are used to represent these concepts: Raman π-pulse for velocity selection, STIRAP for deceleration, and a single spontaneous emission for irreversible accumulation. No closed pumping cycle nor repeated spontaneous emissions are required, so the scheme is applicable to cool a molecular gas. The quantum dynamics are analytically modelled using the density matrix. It is shown that during the coherent processes the gas is translationally cooled. The internal states serve as an entropy sink, in addition to spontaneous emission. This scheme provides new possibilities to translationally laser-cool molecules for high precision molecular spectroscopy and interferometry. Received 25 June 2002 / Received in final form 28 September 2002 Published online 12 November 2002 RID="a" ID="a"e-mail: ooi@spock.physik.uni-konstanz.de RID="b" ID="b"e-mail: Peter.Marzlin@uni-konstanz.de RID="c" ID="c"e-mail: Juergen.Audretsch@uni-konstanz.de     

Amplified spontaneous emission from nitrogen laser pumped dye lasers

The nitrogen laser pumped dye laser output has been studied with emphasis on the behaviour of amplified spontaneous emission (ASE) with respect to the tuning wavelength, pump energy, dyes and their concentration and solvents. Spectral spread of ASE is narrower than fluorescence and its maximum is shifted towards the red side. However, lasing occurs beyond the ASE region. ASE is small at high gain wavelength and increases at the edges of the gain curve. Laser energy is highest at the ASE peak with minimum ASE present in the output. ASE is reduced with increased laser energy in the energy transfer dye lasers.     

Amplified spontaneous emission and spatial dependence of gain in dye amplifiers

Dye amplifiers are studied theoretically in the presence of amplified spontaneous emission (A.S.E.). The set of coupled rate equations is solved analytically in the steady state regime. Analytical relations are derived which express the spectral and spatial dependence of A.S.E. From the spatial dependence of A.S.E., the spatial dependence of the excited state population is obtained. A case of practical interest is treated: that of a rhodamine 6G amplifier transversely excited by a neo-dymium laser.     

带有多孔二氧化硅间隔层的导模共振光栅实现染料激光器发射增强

导模共振光栅是一种典型的平面波导共振结构,可在光栅表面或波导层内形成较强的局域电场,能增强光与物质的相互作用.本文在导模共振结构的光栅层和基底层之间,引入低折射率的多孔二氧化硅间隔层,显著增强了局域电场与增益介质的接触度.结果表明,引入多孔二氧化硅后,共振产生的电场增强区域上移至激光染料层,增加了激光染料与电场的相互作用,实现了激光出射增强.本文基于时域有限差分法,对结构参数进行分析优化,研究了820 nm共振波长激发下的出射激光特性,得到了连续的激光出射,其能量阈值约为2.5 mJ/cm^2,线宽约为0.3 nm.本文提出的结构实现了对表面局域电场的有效调控,增强了激发光与增益介质的相互作用,不但可应用于激光器,还为其它发光器件的设计提供了参考.     

Theory of spontaneous emission reduction at lasing with long delays in GaAs junction lasers

In this work it is shown that the large abrupt reduction of the spontaneous emission of a single heterostructure laser that lases with a long delay, can be explained with the dynamic behavior of the diffraction losses during the current pulse.In our calculations the diffraction losses are governed by the perturbation of refractive index of the laser active region caused by the injected carriers, Joule heating and gain guiding.     

Spectroscopic and lasing characterisation of a dicarbazovinylene-MEH-benzene dye

The dye 1,4-bis(9-ethyl-3-carbazovinylene)-2-methoxy-5-(2′-ethyl-hexyloxy)-benzene (abbreviated 2CzV-MEH-B) dissolved in tetrahydrofuran (THF) and as neat film is characterised by optical absorption and emission spectroscopy. The absorption and stimulated emission cross-section spectra, the fluorescence quantum distributions, fluorescence quantum yields, degrees of fluorescence polarisation, and fluorescence lifetimes are determined. A lasing characterisation is carried out by pumping with single second harmonic pulses of a mode-locked ruby laser (wavelength 347.15 nm, pulse duration 35 ps). The excited-state absorption at the pump laser wavelength is determined by saturable absorption measurements. Laser oscillation of the dye in THF in a rectangular cell is achieved by transverse pumping using the uncoated cell windows for light feedback. From the emission behaviour around threshold the excited-state absorption cross-section spectrum in the laser active spectral region is extracted. The wave-guided travelling-wave lasing behaviour of the dye as neat film is studied by analysis of the amplification of the transverse pumped spontaneous emission. Surface emitting distributed-feedback lasing was achieved with a neat film on corrugated second-order periodic gratings.     

Collective spontaneous emission in a waveguide with a near-zero refractive index

The optimum conditions for observing superradiance and subradiance effects in an ensemble of two-level atoms, placed in a waveguide cladding with a metamaterial with near-zero refractive index, are discussed.     

Wide-range amplified spontaneous emission wavelength tuning in a solid-state dye waveguide

Amplified spontaneous emission (ASE) in an organic-dye- (DCM-) doped poly(methyl methacrylate)/silica-gel hybrid material planar waveguide was investigated. ASE wavelength control and tuning in a wedge waveguide were realized. The tuning range of the waveguide can reach as much as 30 nm. This method can be applied to wide-range wavelength tuning in solid-state tunable lasers.     

Subnanosecond amplified spontaneous emission pulses by a nitrogen pumped dye laser

Pulses of 100 ps duration and peak power up to 100 kW are obtained with a dye laser pumped by an atmospheric pressure nitrogen laser of 0.5 ns duration. The shortening of the dye laser pulses is attributed to amplified spontaneous emission.     

Amplified spontaneous emission enhanced forward stimulated Raman scattering in dye solutions

We study forward stimulated Raman emission from the weakly fluorescent dye 4^′-diethylamino-N-methyl-4-stilbazolium tosylate (DEST) in 1,2 dichloroethane solution excited by a 28-ps, 532-nm Nd:YAG laser. Neat 1,2 dichloroethane emits the first Stokes line at 631 nm with a spectral width of 1.6 nm, corresponding to a Raman shift of 2956 cm^-1. We observe a reduction of spectral width with the addition of DEST in 1,2 dichloroethane solution. The single-pass conversion efficiency for forward Raman emission is as high as 10% in a 1-cm-path-length sample. The pulse duration of forward stimulated Raman emission, measured by a third-order autocorrelation technique, is 10 ps in neat 1,2 dichloroethane, whereas it is ～3 ps for 4×10^-5 mol/l of DEST solution.     

Numerical calculations of emission probabilities of primarily excited molecules in dye solutions

The “active sphere” concentration depolarization theory of Jabloński involves the probability, W_Dk, that a photon is emitted by the donor. Up till now, the mean value of W_Dk, has been exactly calculated only for k = 2 (1 donor and 1 acceptor in the active sphere). For k > 2 the approximate method of Knox was employed. In this paper the use of the Monte Carlo integration method to find <W_Dk > for k up to ten is described. The more accurate values thus obtained coincide closely with the ones found using the simplified method. This finding validates the use of the latter method without reservation up to high dye concentration.     

Wavelength and coherence effects on the growth mechanism of silicon nanopillars and their use in the modification of spontaneous lifetime emission of BODIPY dye molecules

Silicon nanopillars are grown by an electrochemical anodization of p-type silicon wafers at low current densities in a hydrofluoric acid solution. CW, white light, and various UV pulsed lasers are employed as illumination sources in sample preparation to study wavelength and coherence effects on the growth mechanism of the nanopillars. Coherence is observed to be the foundation of regularity in obtaining conical shapes. The pillar size is found to be almost linearly proportional to the employed illumination wavelength during their growth. BODIPY dye molecules are chemically attached to these silicon nanopillars and the radiative decay rates are investigated by means of a time-resolved fluorescence experiment. The decay rate of the dye molecules embedded in the vicinity of various size pillar tips is significantly affected due to different apex angles of the conical nature. It is demonstrated that the pillar size and the separation between pillars can be adjusted if one uses a coherent light source with an appropriate wavelength during the course of fabrication process. Since change in the decay rate is due to tips of the pillars only, separation of a few micrometers between pillar tips allows one to directly monitor a dye, which is embedded to the tip of a single nanopillar, via a confocal microscopic method for the spontaneous lifetime measurements, without having needed to any extra efforts for an in situ imaging process. It is observed that as the pillar size gets smaller, the inhibition in the spontaneous lifetime of BODIPY is more pronounced. In addition, a more regular pillar structure yields nonvarying decay rates of the dye molecules throughout the silicon sample.     

Cavity-mode selection in spontaneous emission from oriented molecules in a microparticle

We observe preferential cavity-mode selection in spontaneous emission by oriented molecules at the surface of a microparticle. Polarization-analyzed images of a levitated microdroplet containing surface active molecules reveal a well-defined system in terms of molecular position and orientation. The measured fluorescence spectrum is compared with that of a semiclassical emission-rate-enhancement model that treats the coupling between an excited state and Mie resonances as an oscillating dipole interacting with its self-scattered field. By comparing results obtained with this theory with the relative strengths of TE to TM modes measured in the emission spectrum, we show that one can elucidate the heterogeneity of a particle from this resonant structure and determine the orientation of the emission moments relative to the phase boundary.     

Theoretical investigation of amplified spontaneous emission with picosecond light pulses in dye solutions

The amplified spontaneous emission in dye solutions excited with intense picosecond light pulses is studied theoretically. A multi-level model is applied to take into account the effects of the various dye parameters such as ground-state absorption, stimulated emission, excited-state absorption, reabsorption and relaxations from populated excited levels. The influence of the pump laser duration and intensity and of the dye concentration and sample length is investigated. Optimum situations are derived for the generation of intense picosecond light pulses at new frequencies by amplified spontaneous emission. On the other hand, conditions are found where amplification of spontaneous emission may be neglected. The analysis allows the determination of unknown dye parameters by comparing the calculations with the experiment.