双光子吸收的Franz-Keldysh效应

从实验上证实Hg_0.695Cd_0.305Te 光电二极管空间电荷区中存在双光子吸收的Franz-Keldysh效应.利用一个皮秒Nd:YAG激光器抽运的光学参量产生器和差频产生器作为激发光源,测量了入射波长为λ₀=7.92μm的脉冲激光所激发的光响应随入射光强的变化关系.脉冲光响应峰值强度随入射光强的增大呈现二次幂函数增强趋势.采用等效RC电路模型将脉冲光伏信号峰值与入射光强相关联,得到空间电荷区中强电场下单光束 关键词： Franz-Keldysh效应 碲镉汞 双光子吸收 脉冲光伏信号     

Dipyrrylmetheneboron Difluorides as Labels in Two-Photon Excited Fluorometry. Part II–Nucleic Acid Hybridization Assays

Five two-photon excitable dipyrrylmetheneboron difluoride labels (dipyrrylmethene-BF₂ labels) with fluorescence emission maximum between 530 and 590 nm, and a frequently used rhodamine label, TAMRA, were conjugated to aminomodified oligonucleotides. The performance of the labeled oligonucleotides was studied in a separation-free nucleic acid hybridization assay using ArcDia^™ TPX bioaffinity assay technology. The results show that oligonucleotide conjugates of dipyrrylmethene-BF₂ labels provide higher two-photon excited fluorescence yield and better assay sensitivity than corresponding TAMRA conjugate. The effect of conjugation on photophysical properties of the labels and performance of the labeled oligonucleotides in separation-free hybridization assay is discussed.     

Optical properties of in situ doped and undoped titania nanocatalysts and doped titania sol-gel nanofilms

In this paper we present spectroscopic properties of doped and undoped titanium dioxide (TiO₂) as nanofilms prepared by the sol-gel process with rhodamine 6G doping and studied by photoacoustic absorption, excitation and emission spectroscopy. The absorption spectra of TiO₂ thin films doped with rhodamine 6G at very low concentration during their preparation show two absorption bands, one at 2.3 eV attributed to molecular dimmer formation, which is responsible for the fluorescence quenching of the sample and the other at 3.0 eV attributed to TiO₂ absorption, which subsequently yields a strong emission band at 600 nm. The electronic band structure and optical properties of the rutile phase of TiO₂ are calculated employing a fully relativistic, full-potential, linearized, augmented plane-wave (FPLAPW) method within the local density approximation (LDA). Comparison of this calculation with experimental data for TiO₂ films prepared for undoped sol-gels and by sputtering is performed.     

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.     

GaS0.4Se0.6: Relevant properties and potential for 1064 nm pumped mid-IR OPOs and OPGs operating above 5 μm

We present measurements of the transparency, refractive index dispersion, nonlinear coefficient, damage threshold, and two-photon absorption of mixed GaS _x Se_{1 − x} crystals and show that GaS_0.4Se_0.6 is a promising nonlinear material for down conversion of pulsed 1064 nm radiation to the mid-IR above 5 μm without significant two-photon absorption.     

硅的间接跃迁双光子吸收系数谱

利用皮秒Nd:YAG脉冲激光器作为激发光源,测量出光子能量介于1.36 μm (0.912 eV)—1.80 μm (0.689 eV)之间的硅间接跃迁双光子吸收系数谱.尽管此波段范围内的激光光子能量小于硅间接带隙,但当激光辐照在硅基光电二极管受光面时,在二极管两电极端仍然探测到了显著的脉冲光伏信号.光伏信号峰值强度与入射光强呈二次幂函数关系,表明其是双光子吸收过程.采用pn结等效结电容充放电模型,将光伏响应信号峰值与入射光强相关联,从中提取出硅的间接跃迁双光子吸收系数,改变入射波长得到系数谱.研究表明:     

Two-Photon Absorption in Nanoheterostructures with <Emphasis Type="Italic">D</Emphasis><Superscript>(−)</Superscript>-Centers

A two-photon impurity absorption coefficient of the “quantum dot — D⁽⁻⁾-center” complexes synthesized in a transparent dielectric matrix is calculated within the model of zero-radius potential. The evolution of spectral dependence of the absorption coefficient of the nanoheterostructure based on semiconductor CdS _x Se _1−x glasses is studied versus the average quantum-dot radius. It is shown that the contribution of the two-photon impurity absorption to the exited two-photon luminescence is fairly significant at a reasonable quantum-dot concentration. __________ Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 7, pp. 46–50, July, 2005.     

Shift photocurrent induced by two-quantum transitions

A theory of the shift current induced by direct two-photon and indirect one-photon absorption is developed for noncentrosymmetric crystals. A formula is derived for the microscopic shifts of Bloch electrons induced by two-quantum processes. It is shown that the ratio of the two-photon photocurrent at the photon frequency ω to the photocurrent induced by direct one-photon transitions at the photon frequency 2ω, as compared to the corresponding absorption-rate ratio, contains a large factor {ie152-1}ω/(2{ie152-2}ω − E _g), where E _g is the bandgap; i.e., these photocurrent can be comparable in order of magnitude. For crystals of T _d symmetry, the photocurrents induced by one- and two-photon absorption are compared in terms of polarization dependence.     

Rapid internal conversion in a symmetric molecule LD 700 studied by means of femtosecond fluorescence depletion

The rapid internal conversion dynamics at room temperature is determined by using the femtosecond time-resolved fluorescence depletion measurements of a complex solvated molecule of LD 700 (rhodamine 700) combined with steady-state absorption and fluorescence spectroscopy, as well as quantum chemical calculation. The molecule is excited by a 50fs laser pulse at 400nm which directly populated the highly excited singlet state, the rapid internal conversions (ICs) are observed, which leads to the directional changes of the emission transition moment following photoexcitation to the highly excited singlet state S₅ of LD 700.     

Saturable absorbers with concentration-dependent absorption recovery time

The ground-state bleaching of highly concentrated rhodamine 6G solutions in methanol is studied with intense picosecond light pulses. The ground-state recovery time changes with concentration from about 3.9 ns at low concentration (10^–5 mol/dm³) to about 1 ps at high concentration (0.6 mol/dm³). The shortening of the absorption recovery time is determined by the concentration dependent quenching of theS ₁-state population due to unbound dimers and by the intensity dependent longitudinal and transverse amplified spontaneous emission.     

Dependence of nonlinear refractive index of ZnSe on Be and Mg content

The values of the nonlinear refractive index n₂ and the two-photon absorption coefficient β of ternary and quaternary ZnSe-based mixed crystals were extracted from the standard backward degenerate four wave mixing (DFWM) and nonlinear transmission measurements at 532 nm, respectively. Studied crystals were grown by the modified high-pressure Bridgman method. We found that the value of the nonlinear refractive index n₂ for Zn_0.79Be_0.21Se is higher than that for Zn_0.80Mg_0.20Se. However, the opposite behaviour was found in the case of two-photon absorption coefficient β for these compounds. We also found that the values of the nonlinear refractive index n₂ and the two-photon absorption coefficient β for Zn_0.83Be_0.04Mg_0.13Se are about five times lower and three times higher than that for Zn_0.80Mg_0.13Se, respectively. In the case of ternary ZnSe-based crystals we noticed that the value of the nonlinear refractive index n2 decreases with increasing Mg or Be content. However, the value of the two-photon absorption coefficient β increases with increasing Mg or Be content.     

Effect of excited state absorption on the transmissivity of organic-dye-based media under two-photon excitation

duration ranging from femtoseconds to nanoseconds has been simulated. The effect of the absorption from excited singlet and triplet states on the transmissivity of the medium under two-photon excitation has been investigated. It has been shown that in a medium excited by monopulses, the S ₁→ S _n and T ₁→ T _m absorption makes a considerable contribution to the total nonlinear absorption of the medium only for nanosecond pulse durations. When a medium is excited by a sequence of femtosecond pulses with a repetition frequency of some tens of megahertz, significant additional nonlinear absorption can arise only due to T ₁→T _m transitions that occur due to accumulation of molecules in triplet states. This effect should be taken into account in determining the cross-section for two-photon absorption in dyes and also in developing radiation intensity limiters for femtosecond lasers.     

Fluorescence of horse liver alcohol dehydrogenase using one- and two-photon excitation

We examined the steady-state and time-resolved emission of liver alcohol dehydrogenase resulting from one-photon and two-photon excitation. Previous studies with one-photon excitation revealed that the two nonidentical tryptophan residues display different emission spectra and decay times. The use of two-photon excitation resulted in similar emission spectra, multiexponential intensity decays, time-resolved emission spectra, and anisotropy decays as was observed for one-photon excitation. These results suggest that both nonidentical tryptophan residues are excited to a similar extent for one- and two-photon excitation. However, the limiting anisotropy (r ₀) with two-photon excitation from 585 to 610 nm is below 0.1 and appears distinct from that observed previously forN-acetyl-l-tryptophanamide.Abbreviations LADH liver alcohol dehydrogenase - -NAD⁺ -nicotinamide adenine dinucleotide - OPE one-photon excitation - OPIF one-photon induced fluorescence - TPE two-photon excitation - TCSPC time-correlated single photon counting - TPIF two-photon induced fluorescence     

S0-S1 two photon absorption dynamics of organic dye solutions

The two-photon absorption cross-sections and excited-state absorption cross-sections of the dyes rhodamine 6G, methylene blue and fuchsin dissolved in methanol, and of the dyes safranine T, 1,3,3,1,3,3-hexamethylindocarbocyanine iodide (HMICI) and 1,3,1,3-tetramethyl-2,2-dioxopyrimidi-6,6-carbocyanine hydrogen sulphate (PYC) dissolved in hexafluoroisopropanol (HFIP) are determined. The excitation is achieved with picosecond light pulses of a passively mode-locked Nd-glass laser (_L = 1.054m). The influence of amplified spontaneous emission on the two-photon absorption dynamics is analysed.     

Multi-quantum photoconductivity in Cdln2S4

A study has been made of photoconductivity in Cdln₂S₄ induced by 1.17 eV photons from a Q-switched neodymium laser. Both three-photon absorption, and two-photon absorption involving the emission of a phonon, have been investigated. The experimental data are in satisfactory agreement with the theory of multi-quantum transitions which takes into account the peculiarities of crystal zone structure.The investigation of competing multi-quantum transitions is a new method which permits one to obtain information on the fundamental optical constants of solids.     

Observation of superfluorescence and stimulated emission in Bi I after nonresonant two-photon pumping

We report the observation of superfluorescence and of stimulated emission in the near-infrared at 965.69 nm in atomic Bi. The atoms are prepared in the 6p ²(³ P ₀)7p _3/2 upper state by nonresonant two-photon excitation. The cooperative character of the emission is demonstrated by the delay of the light pulses and their N² dependence upon the atomic density.     

Ultrafast nonlinear optical properties of dye-doped PMMA discs irradiated by 40 fs laser pulses

The two-photon absorption (TPA) characteristics of PMMA discs doped with three different dyes were studied using an fs-pulsed Ti-Sapphire laser as the pump source, and employing the open-aperture Z-scan technique. TPA cross-sections obtained for PMMA doped with the dyes PM597, DCM and rhodamine 6G–rhodamine B (co-doped) were found to be equal to 24.7, 33.3 and 32.3 GM, respectively (1 GM=10^?50 cm⁴ s phot^?1 mol^?1). Furthermore, two-photon fluorescence was measured for the samples containing DCM and rhodamine 6G–rhodamine B (co-doped). Compared to the one-photon fluorescence spectrum, the peaks in the two-photon fluorescence spectrum were red shifted and the extent of red shift increased with increasing doping concentration. We have also observed that the red shift in the two-photon fluorescence peak of the samples in the solid form is much larger than that in the solution state. This phenomenon could be explained by a twisted intra-molecular charge transfer model.     

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.     

Infrared free-electron laser measurement of power limiting by two-photon absorption in InSb

We have performed the first experiment on the free-electron laser (CLIO) at the Laboratoire pour l'Utilisation du Rayonnement Électromagnétique (LURE). In a transmission experiment we observed strong power limiting at wavelengths longer than the absorption edge associated with induced free carrier absorption produced by direct interband two-photon transitions in InSb. We have estimated the two-photon absorption (TPA) coefficient () of InSb at 8.9 m to be 2 cm MW^-1, by fitting the power-limiting effect with a simple theoretical model. An important feature of this result is that we are utilizing the broad tunability of the FEL to explore the TPA theory to shorter wavelengths than hitherto available with CO₂ lasers. The result is in broad agreement with the longer-wavelength measurements of Sheik-Bahae et al.     

Large near resonance third order nonlinearity in GaN

We have studied third order nonlinearities, including two-photon absorption coefficient and nonlinear refractive index n ₂, of GaN in below bandgap ultraviolet (UV) wavelength regime by using UV femtosecond pulses. Two-photon absorption was investigated by demonstrating femtosecond UV pulsewidth autocorrelation in a GaN thin film while femtosecond Z-scan measurements revealed information for both n ₂ and . The distribution of n ₂ versus wavelength was found to be consistent with a model described by the quadratic Stark effect, which is the dominant factor contributed to the nonlinear refractive index near the bandgap. Large on the order of 10 cm/GW and large negative n ₂ with a magnitude on the order of several 10^–12 cm²/W were obtained. The at near mid-gap infrared (IR) wavelength was also found to be on the order of several cm/GW by using two-photon-type autocorrelations in a GaN thin film. Taking advantage of the large two-photon absorption at mid-gap wavelengths, we have demonstrated excellent image quality on two-photon confocal microscopy, including two-photon-scanning-photoluminescence imaging and two-photon optical-beam-induced current microscopy, on a GaN Hall measurement sample and an InGaN green light emitting diode.