The controlled excitation of forbidden transitions in the two-photon spectrum of strontium by using collisions and electric fields

We present experimental results involving controlled configuration mixing in two-photon spectroscopy of highly-excited states by exploiting a weak external electric field and collisions. The method has allowed new extensions to high members of the two-photon forbidden J = 3 odd-parity 5snf ¹F₃ and the J = 0, even-parity 5sns ¹S₀ Rydberg series of neutral strontium to be observed. We achieve resonant two-photon transverse excitation of a high density atomic jet by using a narrow bandwidth tunable dye laser in a heat pipe setup with sensitive ionization detection. Experimental term values are extended for the 5sns ¹S₀ series up to n = 46. By suitable exploitation of the composition and pressure of the buffer gases in conjunction with the electric field strength in the excitation region and the exciting laser beam intensity we have also extended observations up to n = 44 for the 5snf ¹F₃ series and up to n = 46 for the 5snp ¹P₁ series. Our results demonstrate a novel and remarkably simple experimental method to access high Rydberg states to which transitions are forbidden from the ground state by parity and other selection rules.     

Chemical bond formation during laser bonding of Teflon FEP and titanium

Teflon^® FEP (fluorinated ethylene propylene) is resistant to most chemical solvents, is heat sealable and has low moisture uptake, which make this polymer attractive as a packaging materials for electronics and implantable devices. Teflon^® FEP/Ti microjoints were fabricated by using focused infrared laser irradiation. Teflon^® FEP/Ti interfaces were studied by using X-ray photoelectron spectroscopy (XPS), Auger electron spectroscopy (AES) and scanning electron microscopy coupled with energy dispersive spectroscopy (SEM-EDS). The XPS results give evidence for the formation of Ti-F bonds in the interfacial region. The AES and SEM-EDS results show that the chemical bond formation occurs only in the actual bond area. No evidence for chemical bond formation was found in the heat affected zone surrounding the laser bonds.     

Selective excitation through tapered silica fibers of fluorescent two-photon polymerized structures

Two-photon polymerization has emerged as a powerful tool to design complex three-dimensional microstructures for applications ranging from biology to nanophotonics. To broaden the application spectrum of such microstructures, different materials have been incorporated to the polymers, aiming at specific applications. In this paper we report the fabrication of microstructures containing rhodamine 610, which display strong fluorescence upon one- and two-photon excitation. The latter increases light-penetration depth and spatial selectivity of luminescence. We also demonstrate that by using silica submicrometric wires we were able to select individual microstructures to be excited, which could be explored for designing microstructure-based optical circuits.     

原子内壳层双光子衰变的相对论效应和屏蔽效应

本文系统地计算了H原子,类H-Xe离子及Xe原子内壳层的双光子衰变速率。阐明其相对论效应和电子屏蔽效应。并与最新的实验结果和他人的理论计算结果进行了比较和分析讨论。 关键词：     

Preparation and the optical nonlinearity of surface chemistry improved titania nanoparticles in poly(methyl methacrylate)-titania hybrid thin films

With 800-nm, 120-fs laser pulses, optical nonlinearity has been studied in a series of thin films containing poly(methyl methacrylate) (PMMA), filled with surfactant acetylacetone (Acac) capped TiO₂ nanoparticles, which were synthesized by a simple in situ sol-gel/polymerization process, assisted by spin coating and multi-step baking. The resulting nanohybrid thin films have highly optical transparency and demonstrate a unique nonlinear optical (NLO) response. The highest nonlinear refractive index (n₂) is observed up to 6.55 × 10⁻² cm² GW⁻¹ in the nanohybrid thin film of 60 wt% Ti(OBu)₄ in PMMA, with a negligible two-photon absorption (TPA), as confirmed by the Z-scan technique. The titanium precursor loading combined with the nature of the capping molecules are used to influence the ability of nanoparticles to nonlinear optical response. Indeed, the ligands at the nanoparticles’ surface can not only control the extent of the interaction between the organic molecules and the embedded nanoparticles but also influence the optical nonlinearities of nanoparticles.     

Functional polymers by two-photon 3D lithography

In the presented work, two-photon 3D lithography and selective single-photon photopolymerization in a prefabricated polydimethylsiloxane matrix is presented as an approach with potential applicability of waveguide writing in 3D by two-photon polymerization.Photopolymers based on acrylate chemistry were used in order to evaluate the optical capabilities of the available two-photon system. Several photoinitiators, tailored for two-photon absorption, were tested in a mixture of trimethylolpropane triacrylate and ethoxylated trimethylolpropane triacrylate. Best results were obtained with a recently synthesized diynone-based photoinitiator. Feature resolutions in the range of 300 nm were achieved. Due to the cross-conjugated nature of that donor-π-acceptor-π-donor system a high two-photon absorption activity was achieved. Therefore, a resin mixture containing only 0.025 wt% of photoinitiator was practical for structuring by two-photon polymerization. The required initiator content was therefore a factor of 100 lower than in traditional one-photon lithography.The aim of the second part of this work was to fabricate optical waveguides by selectively irradiating a polymer network, which was swollen by a monomer. The monomer was polymerized by conventional single-photon polymerization and the uncured monomer was removed by evaporation at elevated temperatures. This treatment leads to a local change in refractive index. Refractive index changes in the range of Δn = 0.01 (Δn/n = 0.7%) were achieved, which is sufficient for structuring waveguides for optoelectronic applications.     

Synthesis and Characterization of New Fluorene-Based Singlet Oxygen Sensitizers

The synthesis, photophysical characterization, and determination of singlet oxygen quantum yields (Φ_Δ) for a class of fluorene derivatives with potential application in two-photon photodynamic therapy (PDT) is reported. It has been demonstrated that these compounds possess the ability to generate singlet oxygen (¹O₂) upon excitation. A photochemical method, using 1,3-diphenylisobenzofuran (DPBF) as ¹O₂ chemical quencher, was employed to determine the singlet oxygen quantum yields (Φ_Δ) of the fluorene-based photosensitizers in ethanol. Φ_Δ values ranged from 0.35 to 0.75. These derivatives may have potential application as two-photon photosensitizers when pumped via two-photon excitation in the near-IR spectral region.     

Synthesis and optical properties of silver nanoparticles in ORMOCER

Experimental results on synthesis of metal nanoparticles in ORMOCER by ion implantation are presented. Silver ions were implanted into organic/inorganic matrix at an accelerating energy of 30?keV and doses in the range of 0.25?10¹⁷ to 0.75?10¹⁷?ion/cm². The silver ions form metal nanoparticles, which demonstrate surface plasmon absorption at the wavelength of 425?C580?nm. The nonlinear absorption of new composite materials is measured by Z-scan technique using 150?fs laser pulses at 780?nm wavelength. ORMOCER matrix shows two-photon nonlinear absorption, whereas ORMOCER with silver nanoparticles demonstrates saturated absorption. Some optical applications of these composite materials are discussed.     

Singlet Oxygen Quantum Yield Determination for a Fluorene-Based Two-Photon Photosensitizer

The quantum yield, Φ_Δ, of singlet oxygen generation under two-photon excitation has been determined for a fluorene derivative. A photochemical method was developed using 1,3-diphenylisobenzofuran (DPBF), a chemical quencher of ¹O₂, and 2-(9,9-didecyl-7-nitrofluoren-2-yl)benzothiazole (1) as a two-photon photosensitizer (PS). The photochemical kinetics of the quencher was measured by two different fluorescence methods. Fluorene 1 exhibited relatively high singlet oxygen quantum yield, Φ_Δ ≈ 0.4 ± 0.1, and had a two-photon absorption cross-section of 28 ± 5 GM. Thus, 1 may have potential for use as a two-photon PS in the near-IR spectral region for biomedical applications.     

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.     

A single-crystal source of path/polarization entanglement at non-degenerate wavelengths

We demonstrate a bright, narrowband, compact, quasi-phase-matched single-crystal source generating path-polarization-entangled photon pairs at 810 nm and 1550 nm at a maximum rate of 3 × 10⁶ s⁻¹ THz⁻¹ mW⁻¹ after coupling to single-mode fiber, and with two-photon interference visibility above 90%. While the source can already be used to implement quantum communication protocols such as quantum key distribution, this work is also instrumental for narrowband applications such as entanglement transfer from photonic to atomic qubits, or entanglement of photons from independent sources.     

Dipyrrylmetheneboron Difluorides as Labels in Two-Photon Excited Fluorometry. Part I-Immunometric Assays

Seven different two-photon excitable dipyrrylmetheneboron difluoride labels (dipyrrylmethene-BF₂ labels) and a frequently used TAMRA label were conjugated to mouse IgG against α-fetoprotein in variable substitution degrees. Altogether 40 IgG conjugates were prepared, and studied with respect to one-photon absorption and emission properties, and two-photon fluorescence efficiency using 1064 nm laser as illumination source. Performance of the IgG conjugates as tracers in a separation-free immunometric assay of α-fetoprotein was evaluated using two-photon excitation assay technology, ArcDia^TM TPX. The results show that the dipyrrylmethene-BF₂ labels provide subpicomolar sensitivity, which is an order of magnitude better than that of TAMRA label. The effect of chromophore structure and substitution degree of IgG-label conjugates on the assay performance is discussed.     

Optical nonlinearities in hyperbranched polyyne studied by?two-photon excited fluorescence and third-harmonic generation spectroscopy

The nonlinear optical properties of a hyperbranched polyyne (hb-Polyyne) have been measured at infrared wavelengths by using femtosecond and nanosecond pulsed excitation. This hyperbranched polyyne exhibited strong and intrinsic (simultaneous) two-photon absorption and upconverted blue fluorescent emission under femtosecond excitation around 800 nm. The hb-Polyyne in chloroform solution is characterized by a large two-photon absorption cross section of 9068 GM (1GM=10⁻⁵⁰ cm⁴ s) and a fluorescence quantum yield of 0.57. On the other hand, by third-harmonic generation (THG) spectroscopy with nanosecond excitation, the measured third-order nonlinear susceptibility χ ⁽³⁾ for solid films of hb-Polyyne ranged from 2.4×10⁻¹¹ to 6.1×10⁻¹¹ esu in the spectral range of 1100–1600 nm, with results comparable to the values exhibited by the well-known conjugated polymer MEH:PPV, but with a much better transparency for visible wavelengths.     

Effect of externally injected radiation on amplified spontaneous emission in CO

The effect of externally injected radiation on the two-photon laser-induced amplified spontaneous emission (TP-LIASE) is reported. The wave generated via the same LIASE process in a seeder cell acts as a seeder field for the inverted medium created in a main cell. A nearly tenfold gain is achieved in the B¹ Σ ⁺ ?A¹ Π (0, 3) transition of the CO molecule. We demonstrate that the single rotational transition in the B¹ Σ ⁺ ?A¹ Π (0, 4) band is selectively amplified by injection of laser radiation. This pump and seed arrangement facilitates detection of molecular spectra by simply tuning the seed-laser frequency. The polarization effect of the input laser radiation is briefly discussed. Received: 9 June 2000 / Revised version: 2 October 2000 / Published online: 21 February 2001     

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.     

Calculation of the 1s–2s two-photon excitation cross-section in atomic hydrogen

The two-photon excitation cross-section of atomic hydrogen is calculated using explicit summation over intermediate states within the framework of dipole approximation. The matrix element for two-photon excitation is transformed into finite sums, consisting of the product of a radial and angular part. Nine intermediate states are employed in the calculation of the transition matrix element. The two-photon excitation cross-section obtained for the transition 1s ²S_1/2–2s ²S_1/2in atomic hydrogen is a good agreement with the literature.     

The molecular properties of the positronium negative ion

The dynamics of the positronium negative ion is described in a molecular adiabatic approximation. It is shown, how the classification of the spectrum, propensity rules for radiative and non-radiative transitions and conditions for the occurrence of shape resonances can easily be derived within this approach. Propensity rules for two-photon processes are also derived and used to demonstrate the possibility of an absorption experiment from the ground state to excite a¹S^e shape resonance, which is unique to Ps^–.     

Measurements of photoionization cross sections from the 4p, 5d and 7s excited states of potassium

New measurements of the photoionization cross sections from the 4p ²P_1/2,3/2, 5d ²D_5/2,3/2 and 7s ²S_1/2 excited states of potassium are presented. The cross sections have been measured by two-step excitation and ionization using a Nd:YAG laser in conjunction with a thermionic diode ion detector. By applying the saturation technique, the absolute values of the cross sections from the 4p ²P_3/2 and 4p ²P_1/2 states at 355 nm are determined as 7.2±1.1 and 5.6±0.8 Mb, respectively. The photoionization cross section from the 5d ²D_5/2,3/2 excited state has been measured using two excitation paths, two-step excitation and two-photon excitation from the ground state. The measured values of the cross sections from the 5d ²D_5/2 state by two-photon excitation from the ground state is 28.9±4.3 Mb, whereas in the two-step excitation, the cross section from the 5d ²D_3/2 state via the 4p ²P_1/2 state and from the 5d ²D_5/2,3/2 states via the 4p ²P_3/2 state are determined as 25.1±3.8 and 30.2±4.5 Mb, respectively. Besides, we have measured the photoionization cross sections from the 7s ²S_1/2 excited state using the two-photon excitation from the ground state as 0.61±0.09 Mb.     

Pressure- and temperature-induced transformations in crystalline polymers of C60

The great advantage of the C₆₀ molecule is its potential for polymerization, due to which the molecule can be the building block of new all carbon materials. In addition, it contains, both sp ² and sp ³ hybridized carbon atoms, which allows synthesizing new carbon materials with desired physicochemical properties using both types of carbon bonding. The one- and two-dimensional polymeric phases of C₆₀ are prototype materials of this sort. Their properties, especially polymerization under pressure and room temperature via covalent bonding between molecules belonging to adjacent polymeric chains or polymeric layers, can be used for further development of new materials. The present review focuses on the study of the pressure-induced polymerization and thermodynamic stability of these materials and their recovered new phases by in-situ high-pressure Raman and X-ray diffraction studies. The phonon spectra show that the fullerene molecular cage in the high-pressure phases is preserved, while these polymers decompose under heat treatment into the initial fullerene C₆₀ monomer.     

Enhanced generation of vacuum-ultraviolet radiation by four-wave mixing in mercury using pulsed laser vaporization

The efficiency of a coherent vacuum ultraviolet (VUV) source at 125 nm, based on two-photon resonant four-wave mixing in mercury vapor, has been enhanced by up to two orders of magnitude. This enhancement was obtained by locally heating a liquid mercury surface with a pulsed excimer laser, resulting in a high-density vapor plume in which the nonlinear interaction occurred. Energies up to 5 μJ (1 kW peak power) have been achieved while keeping the overall mercury cell at room temperature, avoiding the use of a complex heat pipe. We have observed a strong saturation of the VUV yield when peak power densities of the fundamental beams exceeded the GW/cm² range, as well as a large intensity-dependent broadening (up to ∼ 30 cm^-1) of the two-photon resonance. The source has potential applications for high-resolution interference lithography and photochemistry. PACS 42.65.Ky; 52.38.Mf