Fluorescence intensity and anisotropy decay of the 4′,6-diamidino-2-phenylindole-DNA complex resulting from one-photon and two-photon excitation

We examined the emission spectra, intensity decays, and anisotropy decays of the DNA-4,6-diamidino-2-phenylindole (DAPI) complex resulting from one- and two-photon excitation of fluorescence. Similar lifetimes and correlation times were recovered from the frequency-domain data. However, the initial anisotropies of DAPI for one- and two-photon excitation revealed different angles between the absorption and the emission oscillators, 17.8 and 23.8°, respectively. This suggests the presence of two overlapping transitions in DAPI with different one- and two-photon cross sections for absorption.     

3,3′-Benzene-1,4-diylbis[1-(substituted)phenylprop-2-en-1-one] derivatives: A new class of materials for third-order nonlinear optical applications

We have investigated the third-order nonlinear optical parameters of Bischalcones embedded in DMF solution and in solid PMMA matrix, by Z-scan technique using nanosecond laser pulse trains at 532 nm. Z-scan results reveal that the Bischalcones exhibits negative nonlinear refractive index as high as 10⁻¹¹ esu. The molecular two-photon absorption cross-section of Bischalcones were of the order 10⁻⁴⁶ cm⁴ s/photon, which is nearly two orders of magnitude larger than that of Rhodamine 6G which is 10⁻⁴⁸ - 10⁻⁵⁰ cm⁴ s/photon. We found that, the two-photon absorption (TPA) is the dominating nonlinear process leading to nonlinear absorption in both the cases in solution and as well as in solid medium. Based on TPA process, the Bischalcones exhibit good optical power limiting of nanosecond laser pulses at the input wavelength. The nonlinear optical parameters found to increase on enhancing the strength of the electron donor groups indicating the dependence and importance of electron donor/acceptor units on third-order nonlinear optical susceptibility χ⁽³⁾.     

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     

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.     

Cavity operation of a pulsed C13H3F laser

Cavity operation of an optically pumped, pulsed, C¹³H₃F far-infrared laser is described. The use of a Fabry-Perot output coupler has resulted in selectable line emission at 1222, 1207, 1006, 388 and 412 m with power levels in the 1–20 kW range. In addition, single mode operation on the longer wavelength lines has been achieved. Experimental evidence is also presented for a collisionally coupled two-photon absorption process which is responsible for the observed short wavelength emission.     

Theoretical study on the photoelectric emission spectra of a field-assisted Au-BaO thin film

The dependence of the spectral distribution of photoelectron emission from gold nano-particles embedded in BaO semiconductor thin film on applied voltage and surface plasmon resonance of gold nano-particles is predicted and investigated theoretically. The photoelectron emission response curves to light wavelength between 0.2 and are given. The dependence of the wavelength threshold on the size of gold nano-particles and external field strength is also shown. The reason that the theoretical photoelectron emission spectra is in the visible region is explained. The probabilities increased for photoexcited electrons to overcome the barrier and escape from the surface are discussed. This could be of importance in designing field-assisted thin film and finding their optimum operation conditions.     

Vacuum ultraviolet 178.7 nm emission in sodium vapour under two-photon resonance excitation

We have observed a fixed wavelength emission at 178.7 nm in sodium vapour under 578.7 nm two-photon resonance excitation. The proposed non-linear wave mixing scheme is described by _{178.7 nm} = 2_L + _{465.7 nm}; where _178.7 is the 178.7 nm photon frequency, _L is the laser-photon frequency, and _465.7 is the 465.7 nm photon frequency. This 465.7 nm emission comes from another six-wave mixing process involving two hyper-electronic Raman scattering photons. The excitation spectrum of the 178.7 nm emission has a typical multiwave mixing pattern with a competing effect appearing at higher temperatures under two-photon resonance excitation. Numerical analysis indicates that this vacuum ultraviolet emission has a poor phase-match condition that will depress the emission intensity to a certain extent. This makes the observation more difficult compared with other reported four-wave mixing generated emissions. Fortunately, on the one hand, it is enhanced by quasi-auto-ionization resonance when the 3s–5s transition is coupled to the sodium continuum by a 330.2 nm photon. On the other hand, its wavelength sits so close to the sodium Cooper minimum that weak absorption will not suppress this vacuum ultraviolet emission further.     

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.     

Three-photon excitation ofp-quaterphenyl with a mode-locked femtosecond Ti:sapphire laser

We observed emission fromp-quaterphenyl (p-QT) at 360 nm when exposed to the focused light from a femtosecond (fs) Ti:sapphire laser at 850 nm. This wavelength is too long to allow two-photon excitation of p-QT. The emission intensity of p-QT was found to depend on the cube of the laser power at 850 nm, suggesting that excitation occurs due to a three-photon process. The same emission spectrum and single exponential decay times were observed for three-photon excitation at 850 nm as for two-photon excitation at 586 nm and for one-photon excitation at 283 nm. The same rotational correlation times were observed for one-, two-, and three-photon excitation, but higher time-zero anisotropies were observed for two- and three-photon excitation. The steady-state anisotropies for one-, two-, and three-photon excitation are precisely consistent with cos², cos⁴, and cos⁶ excitation photoselection, where is the angle between the electric field of the incident light and the absorption dipole. These experiments were performed with 3×10^–5 M solutions of p-QT. Use of such low concentrations was possible because p-QT displays one of the highest apparent cross sections we have observed to date for three-photon excitation. The spatial distribution of the excited fluorescence was less for three-photon excitation than for two-photon excitation of Coumarin 102 at the same 850-nm excitation wavelength. The high cross section, photostability, and clear cos⁶ photoselection of p-QT make it an ideal three-photon standard for spectroscopy and microscopy.     

Three-photon absorption and its limitation of third-order nonlinear optical effects in rutile

Three-photon absorption and three-photon-induced excited-state absorption of rutile are studied by transmission measurements using picosecond pulses of a mode-locked Nd: glass laser. The nonlinear absorption limits efficient stimulated Raman scattering. It reduces the efficiency of two-photon absorption of a picosecond probe continuum. Three-photon absorption coefficients, excited-state absorption cross sections, a Raman gain factor, and two-photon absorption cross-section spectra are determined. The arrangementsEc andE c are considered.     

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.     

Suppression of stimulated hyer-Raman scattering in lithium vapor

The stimulated hyper-Raman scattering (SHRS) in lithium vapor has been observed in both the forward and the backward directions as the laser was tuned near the 2S–3S and 2S–4S two-photon resonances. It is found that in the forward direction the SHRS associated with the 2P excitation near the 2S–3S or the 2S–4S two-photon resonance is completely suppressed, but the SHRS associated with the 3P excitation near the 2S–4S two-photon resonance can be observed. A condition under which the forward SHRS takes place, given by Malakyan [3], has been examined. A reasonable agreement between the theory and the experiment is obtained. Near the 2S–3S two-photon resonance, instead of the expected emission _2P–2S corresponding to the 2P–2S transition, an emission at the 2_P–_3S–2P frequency, which is close to the _2P–2S, has been observed in the backward direction. The process generating this emission could be considered as an inverse SHRS process induced by the 3S–2P spontaneous emission. For the SHRS emission a shift of the observed frequency from the calculated frequency has been found. In order to explain the shift, the Stark effect has been calculated. The results show that the shift can not be attributed to the Stark effect.     

One- and Two-Photon Fluorescence Anisotropy of Selected Fluorene Derivatives

The steady-state excitation anisotropy spectra of fluorene derivatives were measured in viscous solvents, under the one- and two-photon excitation, over a broad spectral range (UV–Visible). The orientation of their absorption transition moments for the first, S₀S₁, and second, S₀S₂, excited states were determined. It was shown experimentally that a decrease in the angle between S₀S₁and S₀S₂ transitions corresponded to an increased value of two-photon absorption (2PA) cross section for these molecules. Two-photon excitation anisotropy was nearly constant over the spectral region investigated (in contrast to one-photon excitation anisotropy spectra) and can be roughly explained by a simple model of 2PA based on the single intermediate state approximation. For comparison, the same trend in two-photon excitation anisotropy was observed for Rhodamine B inglycerol.     

The luminescence of unactivated alkali iodides

Two shorter wave-length emission bands have been observed in activated alkali iodides at — and light excitation apart from activator emission. The shortest wave-length band, observed only at low temperatures, is excited in exciton absorption bands and it may be due to exciton emission.This emission has greater intensity in unactivated crystals grown from the solution. We have observed this emission on CsI, KI and RbI crystals.The intermediate emission band is excited in a narrow excitation band, situated on the sharp slope of the fundamental absorption in crystals and it can apparently be ascribed to structural defects.We wish to thank M. D. Galanin for interest in this work and L. M. amovski for providing us with crystals.     

反-4,4''-双(N,N-二丁胺基)二苯乙烯分子双光子吸收性质研究

对于实验室合成的反-4,4'-双(N,N-二丁胺基)二苯乙烯分子,实验测量了该分子的单光子和双光子荧光谱,然后从理论上研究了其单光子和双光子吸收特性.研究结果表明,在低能量范围内,分子的单光子吸收主要发生在分子的第一激发态,而分子的双光子吸收主要发生在分子的第二和第四激发态上.该分子在相应系列衍生物中具有最大的双光子吸收截面.分子的相关能对分子的激发态能量影响较大.我们给出了分子基态与电荷转移态的电荷转移过程,并从理论上定性解释了双光子聚合反应的聚合机理.     

Two color oscillations of TE-CO2 laser and applications to two photon process of optically pumped FIR laser

We have developed the resonance system which is able to operate a TE-CO₂ discharge tube in two color emission source. The two color source is excellent in pumping efficiency, spacial overlap and time synchronization of the two emission CO₂ lines.We indicate that the competitive operation of the two emissions is well explained by a simple model.When a TE-CO₂ laser operates at the total pressure of below half atmospheric pressure, we make clear in this work that the operation of a TE-CO₂ laser forms depression like hole burning, with regards to the J of the upper laser level by J-J collisional relaxation during the laser emission.As an example of the two-photon source, two-photon pumping of NH₃ and FIR emissions are given in this paper.     

Two-photon four-level hologram recording in poly-(alkyl-α-cyanoacrylates)

We have investigated the suitability of poly-(alkyl--cyanoacrylates) (p-(alkyl-CAc)) for two-photon four-level holographic recording. It is shown that these materials follow indeed a two-photon four-level mechanism with the second absorption step in the near infrared. Light induces the polymerization of residual monomer in the matrix. The reaction is associated with positive density changes. The sensitivity ofp-(alkyl-CAc) depends strongly on composition and age of the sample. Maximum sensitivities achieved are comparable to the so far best-known two-photon four-level ir-sensitive systems.     

Experimental and theoretical investigation of third-harmonic generation in phase-matched dye solutions

The phase-matched third-harmonic light generation in dye solutions is studied experimentally and theoretically. In the experiments picosecond light pulses of a passive mode-locked Nd-glass laser are converted to the third-harmonic frequency. A third-harmonic conversion efficiency of up to 4×10^–4 was achieved for one of the dyes investigated (1,3,3,1,3,3-hexamethylindocarbocyanine iodide in hexafluoroisopropanol). The theoretical calculations determine the influence of various dye and solvent parameters on the conversion efficiency. The conversion efficiency is found to be limited by excited-state absorption of pump laser light and third-harmonic light from the S₁-state to higher singlet states. The S₁-state is mainly populated by two-photon absorption. Amplified spontaneous emission may reduce the limiting effects of excited-state absorption. Phase changes caused by the non-linear refractive index and the refractive index dispersion within the spectral bandwidth of the laser pulses reduce the conversion efficiency. Under ideal conditions conversion efficiencies up to 10% may be achieved.     

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.     

Resonance-enhanced multiphoton ionization spectroscopy of CH3 and CD3. Two-photon absorption selection rules and rotational line strengths of the ν3- and ν4-active vibronic transitions

To explore the possibility of K-level resolved, 2+1 resonance-enhanced multiphoton ionization (REMPI) processes of the methyl radical, the two-photon absorption selection rules and rotational line strengths of the 3₀¹ and 4₀¹ vibronic bands of the transition (n=3 or 4) were reported. Stringent selection rules, which were imposed upon these two-photon transitions, are the initial K″=3p (p=0,1,2,…), ΔK=±2, ΔU=±3, and ΔN=0,±1,±2 (O, P, Q, R, and S branches). The previously assigned 2₂² vibronic band of the methyl radical should be studied by the REMPI with a better spectral resolution and analyzed by the newly derived two-photon absorption selection rules and rotational line strength formulas.