Absorption and Emission Properties of a New Two-photon Absorption Dye

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Absorption and Emission Properties of a New Two-photon Absorption Dye

The emission properties of a newly synthesized organic two-photon absorption dye, trans-4-[p-(N-ethyl-N-ethylamino)-styryl]-N-methyl-pyridinium tetraphenylborate, have been investigated. When pumped by infrared pulses from a picosecond Nd∶YAG laser, the dye exhibits intense upconverted fluorescence and strong superradiance properties. For comparison, the one-photon induced fluorescence and superradiance are also measured. The one- and two-photon excited fluorescent lifetimes are 86 and 64 ps, respectively. The maximum efficiency of the dye is measured to be 1.97% and the upconversion efficiencies at different pump wavelengths have also been investigated by the optical parametric amplifier.     

Simple cases of spontaneous emission from an atom-photon cluster localized in a microcavity

The spontaneous emission from an atomic ensemble localized in a microcavity with the participation of microcavity photons and an external broadband quantized electromagnetic field at the Raman resonance of photons with an optically forbidden (two-photon) atomic transition has been studied. The average spontaneous decay intensity has been calculated for simple cases. It is shown that the dynamics of spontaneous emission from this atomic ensemble differs generally from the conventional superradiance (spontaneous emission of an atomic ensemble at a one-photon optically allowed transition from excited to the ground state. When the atomic ensemble is strongly excited, the delay times and the emission pulse shape differ significantly. The parameter ranges where the spontaneous emission from the atomic ensemble under consideration at a two-photon Raman transition can be described as conventional superradiance with renormalized parameters are found. In the case of single excitation the photon emission probability depends on the number of photons and atoms in the microcavity.     

Two-photon induced optical-power limiting and upconverted superradiance properties of a new organic dye HEASPI

A new organic dye trans-4-[p-(N-ethyl-N-hydroxyethylamino)styryl]-N-methylpyridinium iodide (abbreviated as HEASPI hereafter) with large two-photon absorption (TPA) cross section and excellent upconverted superradiance properties was synthesized in our group recently. The TPA cross section was measured to be σ₂′=7.0×10⁻⁴⁸ cm⁴ s/photon by using an open aperture Z-scan system. Linear absorption, single-photon induced fluorescence, two-photon induced fluorescence and two-photon pumped (TPP) upconverted superradiance properties were systematically studied. The highest net upconversion efficiency from the absorbed pump energy to the output upconverted superradiance energy is as high as 19.6% at the pump energy of 2.07 mJ from a mode-locked Nd : YAG picosecond laser. The dye solution also shows a clear optical power limiting effect.     

Photon echo under superradiance

The dynamics of optical coherence and phase memory in three-level medium in conditions of superradiance pulse emission is considered. In the case of coherent excitation of the upper level in three-level system of lambda configuration it is shown that the superradiance eliminates optical coherence on the adjacent transitions of excitation and superradiance emission and induces optical coherence on the remain transition. This, in turn, makes it possible to observe new effects of photon-echo, simple example of which is described in the present Letter.     

Linear and nonlinear optical properties of two-photon absorption dye doped linear copolymer

2-hydroxyethyl methacrylate (abbreviated as HEMA) and acrylonitrile have been used as the monomers to form a trans-4-[p-(N-hydroxyethyl-N-methylamino)styryl]-N-methylpyridinium p-toluene sulfonate (abbreviated as HMASPS) doped linear copolymer. The spectra of one and two-photon excited fluorescence and two-photon pumped superradiance and two-photon pumped lasing of the polymer all shifted to short wavelengths compared with the solution sample of the dye. The copolymer shows much longer one- and two-photon excited fluorescence lifetimes of nanoseconds. When pumped by the picosecond Nd:YAG laser, the superradiance and lasing can be simultaneously obtained. The maximum two-photon pumped lasing conversion efficiency is 3.3%. The place of the maximum upconversion efficiency of the copolymer does not coincide with that of the maximum nonlinear absorption.     

Characterization of the two-photon absorption resonance that is due to the internal charge-transfer transition of a push pull molecule, 4-(diethylamino)-beta-nitrostyrene

The two-photon absorption resonance that is due to the internal charge-transfer transition of an organic push-pull molecule has been characterized. A nonlinear absorption spectrum of the 4-(diethylamino)- beta-nitrostyrene molecule was measured in a tetrahydrofuran solution by optical Kerr ellipsometry. The shape and the amplitude of the two-photon absorption spectrum are well described by a model that uses the relevant one-photon absorption spectrum related to the internal charge-transfer transition.     

On the theory of vibronic superradiance

The Dicke superradiance on vibronic transitions of impurity crystals is considered. It is shown that parameters of the superradiance (duration and intensity of the superradiance pulse and delay times) on each vibronic transition depend on the strength of coupling of electronic states with the intramolecular impurity vibration (responsible for the vibronic structure of the optical spectrum in the form of vibrational replicas of the pure electronic line) and on the crystal temperature through the Debye-Waller factor of the lattice vibrations. Theoretical estimates of the ratios of the time delays, as well as of the superradiance pulse intensities for different vibronic transitions well agree with the results of experimental observations of two-color superradiance in the polar dielectric KCl:O ₂ ^? . In addition, the theory describes qualitatively correctly the critical temperature dependence of the superradiance effect.     

Phase-transition radiation and the growth of a new phase

It was shown that, under certain conditions, the growth of a new phase becomes much like a cooperative optical phenomenon during which the heat of phase transition evolves as a sequence of superradiance pulses (phase-transition radiation). The optical control of new-phase growth and the effect of optical properties of substances on the kinetics of phase transitions are considered.     

Properties of two-photon fluorescence and superradiance of a new organic dye C46H51N2B

Linear and nonlinear optical properties of a new organic dye, trans-4-[p-(N-n-butyl-N-n-butylamino)-styryl]-N-methyl-pyridinium tetraphenylborate solution in dimethyl formamide (DMF) have been studied systematically. When excited with mode-locked picosecond 1 064 nm laser beam, intense upconversion fluorescence and superradiance can be obtained. The temporal behaviors of one-photon absorption and two-photon absorption (TPA) fluorescence and superradiance have been studied. The highest upconversion efficiency was found to be 4.1% at a pump energy of 4 mJ. By using an optical parameter amplifier (OPA) as the pump laser, the nonlinear transmittance and upconversion efficiencies of the dye solution at different wavelengths were measured. The strongest linear absorption was found at a wavelength of 930 nm whereas the highest upconversion efficiency was at 1 030 nm. The 100 nm red-shift for the highest upconversion efficiency wavelength compared with the strongest nonlinear absorption are caused by excited state absorption. Received 17 October 2001 and Received in final form 21 December 2001     

Superradiant emission of LaF<Subscript>3</Subscript>:Pr<Superscript>3+</Superscript> in resonator

Experimental data concerning superradiant emission from the LaF₃ medium doped with impurity praseodymium ions are presented in the cases of a free medium and when the medium is placed into an optical resonator. The spike structure of superradiance is registered and studied. When the medium is placed inside a cavity, a new channel of energy removal by superradiance related to the cavity mode appears; the old noncavity channels are preserved. The duration of superradiance in the cavity channel is decreased, and regular modulation arises. These peculiarities of superradiance induced by the presence of an optical resonator are explained.     

Ultrafast carrier dynamics of Cu2O thin film induced by two-photon excitation

Cuprous oxide (Cu₂O) has attracted plenty of attention for potential nonlinear photonic applications due to its superior third-order nonlinear optical property such as two-photon absorption. In this paper, we investigated the two-photon excitation induced carrier dynamics of a Cu₂O thin film prepared by radio-frequency magnetron sputtering, using the femtosecond transient absorption experiments. Biexponential dynamics including an ultrafast carrier scattering (< 1 ps) followed by a carrier recombination (> 50 ps) were observed. The time constant of carrier scattering under two-photon excitation is larger than that under one-photon excitation, due to the different transition selection rules and smaller absorption coefficient of the two-photon excitation.     

Two-photon absorption-induced optical properties of a new lasing dye in two solvents

Pumped by an infrared lasing and its frequency-doubling source, the fluorescence and superradiance emission properties of a new lasing dye trans-4-[4^′-(N,N-diethylamino)styryl]-N-methyl pyridinium methyl sulfate (abbreviated DEASPS), have been studied in benzyl alcohol and chloroform. The two-photon absorption (TPA) and emission properties of DEASPSare influenced by the solvents used. The emission wavelength of the dye in benzyl alcohol is redshifted relative to that in chloroform. The lifetime of two-photon absorption-induced fluorescence is about 529 ps in benzyl alcohol, whereas it is 340 ps in chloroform. Correspondingly, the one-photon-excited fluorescence lifetimes in the two solvents are also given. The upconversion efficiency of DEASPS in chloroform is higher than in benzyl alcohol. Finally, the effective molecular two-photon absorption cross-sections were measured by the nonlinear transmittance method. It is found that the optical limiting effect of the dye in benzyl alcohol is stronger than that in chloroform. Received: 3 May 2001 / Revised version: 6 July 2001 / Published online: 19 September 2001     

Two-color two-photon Rabi oscillation of biexciton in single InAs/GaAs quantum dot

A two-photon absorption resonance is observed when the sum-frequency of two laser pulses equals the creation energy of a biexciton in a single InAs/GaAs semiconductor quantum dot. Resonant excitation of the two-color two-photon transition results in a coherent oscillation that is remarkably similar to a single-color two-photon Rabi oscillation of the crystal-ground to biexciton optical transition. A model explaining the coherent two-photon absorption is presented.     

Optical Two-Photon Surface Nonlinear Waves

A theory of the optical surface two-photon small-amplitude breather in a multilayer system of the isotropic and anisotropic left-hand metamaterials, when there are a graphene monolayer (graphene-like twodimensional material) and a transition layer with impurity optical atoms (semiconductor quantum dots), is constructed. It is shown that the system of constitutive equations for two-photon transitions and wave equation for a surface plasmon–polariton TM mode are reduced to the nonlinear Schrödinger equation with damping. Explicit analytical expressions for a surface two-photon small-amplitude self-induced transparency breather (0π-pulse) are obtained. It is shown that the optical conductivity of graphene leads to the exponential damping of intensity of a surface two-photon nonlinear wave during the propagation. One- and two-photon small-amplitude breathers in graphene are compared, and it is shown that differences between their parameters are substantial.     

Nonlinear absorption and refraction of light in a colloidal solution of CdSe/ZnS quantum dots upon two-photon resonant excitation

This paper reports on the results of an investigation into the nonlinear transmission of individual ultrashort pulses of a train generated by a mode-locked laser through a colloidal solution of CdSe/ZnS quantum dots in toluene upon two-photon resonant excitation of the fundamental optical transition. The specific features of the nonlinear transmission are explained in terms of the two-photon absorption and self-defocusing processes. Analysis of the experimental results makes it possible to separate the self-defocusing processes that are governed by the inertialess change in the refractive index due to the interaction of high-power optical pulses with bound electrons and those determined by the nonlinear change in the refractive index under the action of two-photon-excited carriers in a quantum dot.     

Investigation of optical nonlinearities in Pd(po)2 by Z-scan technique

With nanosecond scale at a 532 nm wavelength, we firstly measured the nonlinear optical absorption and refraction coefficients of Pd(po)₂ complex by using Z-scan technique, here Hpo=1-hydioxy-2-pyridone. We describe an empirical expression for the case when nonlinear refraction is accompanied by nonlinear absorption to separately evaluate the nonlinear refraction and the nonlinear absorption by performing straightforward measurements with the aperture removed. The nonlinear optical response of Pd(po)₂ was determined by the linear decreasing irradiance-dependence. The nonlinear absorption originates from the near resonant two-photon absorption while the mechanism of the nonlinear refraction is the near resonant two-photon absorption transition enhancement. The linear increasing dependences of the optical nonlinearities on the incident irradiance arise from the population redistribution due to the near resonant two-photon absorption.     

Optical frequency standard for optical fiber communication based on the Rb 5s --> 5d two-photon transition

We report an optical frequency standard based on the 5s --> 5d two-photon transition in Rb atoms. The frequency of a lambda = 778 nm diode laser was locked to the two-photon transition. Second-harmonic generation and an optical phase-locked loop were used to transfer the frequency stability to lambda = 1.556 mum for use in optical fiber communication applications.     

Cooperative emission from an ensemble of three-level Λ radiators in a cavity: An insight from the viewpoint of dynamics of nonlinear systems

Cooperative radiation emitted by an ensemble of three-level optical systems with a doublet in the ground state (Λ scheme), which is placed into a cyclic cavity, is studied theoretically. In contrast to the two-level model of emitters, this process with such a configuration of operating transitions may occur without population inversion in the whole, if the doublet is prepared at the initial instant in a superposition (coherent) state. In the ideal case of a Hamilton system, in which the cavity losses and relaxation in the radiator ensemble are disregarded, the conservation laws are derived, which allow a substantial reduction of the dimension of the phase space of the model (?¹¹ → ?⁵) and the application of methods of dynamics of nonlinear systems for analyzing the three-level superradiance under these conditions. The possibility of different (both quasiperiodic and chaotic) scenarios of the three-level superradiance is demonstrated on the basis of Poincaré’s mappings. Global bifurcation of the system upon a transition from the conventional superradiance regime to inversionless one is revealed. The effects of cavity losses, as well as homogeneous and inhomogeneous broadening in the system of radiators on the regularities found are also discussed.