Slow light in molecular aggregates nanofilms

We study slow light performance of molecular aggregates arranged in nanofilms by means of coherent population oscillations (CPO). The molecular cooperative behavior inside the aggregate enhances the delay of input signals in the GHz range in comparison with other CPO-based devices. Moreover, the problem of residual absorption present in CPO processes, is removed. We also propose an optical switch between different delays by exploiting the optical bistability of these aggregates.Comment: 4 pages, 4 figure

A comprehensive analysis of the contributions to the nonlinear optical properties of thin Ag films

© 2010 American Institute of Physics. The electronic version of this article is the complete one and can be found at: http://dx.doi.org/10.1063/1.3429118DOI: 10.1063/1.3429118The nonlinear optical properties of 20 nm thick Ag films are investigated by time-resolved white- light continuum pump-probe experiments in both transmission and reflection mode. The dynamics of changes in permittivity Δε are measured at wavelengths between 500 to 700 nm. The data is fitted to a modified Drude model in the frequency domain and to a two-temperature model in the time domain. Changes in the individual Drude parameters are calculated as a function of time. A single, coherent model is proposed based on these fittings that describes the dynamics of the nonlinear optical properties of Ag, which could be used to model the nonlinear responses of multilayer structures containing thin films of Ag. The physical origins of the observed responses are discussed

Rapid, broadband two-photon-excited fluorescence spectroscopy and its application to red-emitting secondary reference compounds

© 2011 Optical Society of AmericaThe definitive version of this paper is available at: http://dx.doi.org/10.1364/OME.1.000551DOI: 10.1364/OME.1.000551We present a methodology for rapidly acquiring broadband two-photon absorption (2PA) spectra by means of a compact two-channel femtosecond fluorescence excitation apparatus. This technique is insensitive to differences in excitation and collection geometries as well as detection efficiencies between the sample and reference, in addition to variations in average power, pulse duration and spatial beam profile, as it utilizes sequential measurement of the sample and reference in each of the two cell positions. Our approach eliminates the need to determine the fluorescence quantum yields of the sample and reference, as it allows measurement of emission from samples at a common specified wavelength. These attributes allow for acquisition of 2PA spectra with an estimated accuracy of ± 15% (limited almost exclusively by the uncertainty in the 2PA cross section for the reference standards) over an excitation range of 550-1600 nanometers with a typical time per spectrum of ~30-60 minutes. We have applied this technique to determine the 2PA spectra of six commercially available organic dyes over a wide range of excitation wavelengths (670-1600 nm), which can be used as secondary reference standards emitting in the red and near-infrared spectral region (600-1000 nm). We have also characterized some of these compounds using the femtosecond-pulsed Z-scan method and found very good agreement with the fluorescence-based measurements

Diagnosing 0.1–10 au Scale Morphology of the FU Ori Disk Using ALMA and VLTI/GRAVITY

We report new Atacama Large Millimeter/submillimeter Array Band 3 (86–100 GHz; ~80 mas angular resolution) and Band 4 (146–160 GHz; ~50 mas angular resolution) observations of the dust continuum emission toward the archetypal and ongoing accretion burst young stellar object FU Ori, which simultaneously covered its companion, FU Ori S. In addition, we present near-infrared (2–2.45 μm) observations of FU Ori taken with the General Relativity Analysis via VLT InTerferometrY (GRAVITY; ~1 mas angular resolution) instrument on the Very Large Telescope Interferometer (VLTI). We find that the emission in both FU Ori and FU Ori S at (sub)millimeter and near-infrared bands is dominated by structures inward of ~10 au radii. We detected closure phases close to zero from FU Ori with VLTI/GRAVITY, which indicate the source is approximately centrally symmetric and therefore is likely viewed nearly face-on. Our simple model to fit the GRAVITY data shows that the inner 0.4 au radii of the FU Ori disk has a triangular spectral shape at 2–2.45 μm, which is consistent with the H2O and CO absorption features in a 10−4 M ⊙ yr−1, viscously heated accretion disk. At larger (~0.4–10 au) radii, our analysis shows that viscous heating may also explain the observed (sub)millimeter and centimeter spectral energy distribution when we assume a constant, ~10−4 M ⊙ yr−1 mass inflow rate in this region. This explains how the inner 0.4 au disk is replenished with mass at a modest rate, such that it neither depletes nor accumulates significant masses over its short dynamic timescale. Finally, we tentatively detect evidence of vertical dust settling in the inner 10 au of the FU Ori disk, but confirmation requires more complete spectral sampling in the centimeter bands

Fluorene-based fluorescent probes with high two-photon action cross-sections for biological multiphoton imaging applications

Two-photon fluorescence microscopy is a powerful tool for the study of dynamic cellular processes and live-cell imaging. Many commercially available fluorescent probes have been used in multiphoton-based imaging studies despite exhibiting relatively low two-photon absorption cross-section values in the tunability range of ultrafast Ti:sapphire lasers commonly used in multiphoton microscopy imaging. Furthermore, available fluorophores may be plagued with low fluorescence quantum yield and/or photoinstability (i.e., photobleaching) on exposure to the high peak power and photon density provided by the ultrafast laser source. To address the demand for better performing dyes, we prepare fluorophores tailored for multiphoton imaging. These fluorophores are based on the fluorene ring system, known to exhibit high fluorescence quantum yield ( \u3e 0.7) and high photostability. Furthermore, an amine-reactive fluorescent probe for the covalent attachment onto amine-containing biomolecules is also prepared. Epi-fluorescence and two-photon fluorescence microscopy images of H9c2 rat cardiomyoblasts stained with an efficient two-photon absorbing fluorene fluorophore is demonstrated. Additionally, single-photon spectral characteristics of the amine-reactive fluorophore, as well as the two-photon absorption cross sections of its model adduct in solution, and spectral characterization of a bovine serum albumin (BSA) as a model bioconjugate are presented

Conjugated polymer-fullerene blend with strong optical limiting in the near-infrared

© 2009 Optical Society of AmericaThe definitive version of this paper is available at: http://dx.doi.org/10.1364/OE.17.022062DOI: 10.1364/OE.17.022062Optical-quality, melt processable thick films of a conjugated polymer blend containing poly(2-methoxy-5-(2-ethyl-hexyloxy)-(phenylene vinylene)) (MEH-PPV), a ₆₀ derivative (PCBM) and a plasticizer (1,2-di-iso-octylphthalate) have been developed and their nonlinear absorption and optical limiting properties have been investigated. These blend materials exhibited strong optical limiting characteristics in the near infrared region (750-900 nm), with broad temporal dynamic range spanning femtosecond to nanosecond pulse widths. The dispersion of the optical limiting figure-of-merit of the MEH-PPV:PCBM:DOP blend shows a peak near the wavelength of the MEH-PPV cation, indicating an important role of one-photon and two-photon induced charge transfer in the nonlinear absorption response

Quasi-three-level Model Applied to Measured Spectra of Nonlinear Absorption and Refraction in Organic Molecules

Materials with a large nonlinear refractive index (2) and relatively small linear and nonlinear absorption losses, namely, two-photon absorption (2PA, of coefficient 2), have long been sought after for applications such as all-optical switching (AOS). Here we experimentally determine the linear and 2PA properties of several organic molecules, which we approximate as centrosymmetric, and use a simplified essential-state model (quasi-three-level model) to predict the dispersion of 2. We then compare these predictions with experimental measurements of 2 and find good agreement. Here “quasi”-three-level means using a single one-photon allowed intermediate state and multiple (here two) two-photon allowed states. This also allows predictions of the figure-of-merit (FOM), defined as the ratio of nonlinear refractive phase shift to the 2PA fractional loss, that determines the viability for such molecules to be used in device applications. The model predicts that the optimized wavelength range for a large FOM lies near the short wavelength linear absorption edge for cyanine-like dyes where the magnitude of 2 is quite large. However, 2PA bands lying close to the linear absorption edge in certain classes of molecules can greatly reduce this FOM. We identify two molecules having a large FOM for AOS. We note that the FOM is often defined as the ratio of real to imaginary parts of the third-order susceptibility ((3)) with multiple processes leading to both components. As explained later in this paper, such definitions require care to only include the 2PA contribution to the imaginary part of (3) in regions of transparency.Abstract © 2016 Optical Society of Americ

Nature of the electronic transitions in thiacarbocyanines with a long polymethine chain

Abstract A detailed experimental investigation and quantum-chemical analysis of symmetric cyanines of different conjugation lengths have been performed with the goal of understanding the nature of the electronic transitions in molecules that possess a long chromophore. The nature of electronic transitions in cyanines with a relatively short chromophore (inside the cyanine limit) has already been investigated and many properties of these molecules are well understood. However, little is known about the nature of the transitions beyond the cyanine limit. Their unusual properties, which were proposed by Tolbert and Zhao to be connected with symmetry breaking, still remain unexplored. The analysis of the spectral data in various solvents and results of femtosecond pumpprobe saturable absorption measurements enable us to conclude that an increase in the length of the chain leads to a symmetry breaking and the appearance of two forms with symmetrical and asymmetrical distributions of the charge density in the ground state. For thiacarbocyanines, symmetry breaking is predicted and observed for a pentacarbocyanine dye. Quantum-chemical calculations provide additional proof of this hypothesis. The excited-state absorption properties of a pentacarbocyanine in the visible region are also reported. For the first time we have observed an excited-state cross-section that is larger (%3·) than the ground state cross-section at the peak spectral position

Characterisation of a dipolar chromophore with third-harmonic generation applications in the near-IR

E-2-Tricyanovinyl-3-n-hexyl-5-[4-{bis(4-n-butylphenyl)amino}-2-methoxystyryl]-thiophene, 1, has previously been used to demonstrate applications relying on frequency tripling of 1.55 μm light. Here we report the synthesis and chemical characterisation of 1, along with quantum-chemical calculations and additional experimental investigations of its third-order nonlinear properties that give more insight into its frequency tripling properties. Although 1 can be processed into amorphous films, crystals can also be grown by slow evaporation of solutions; the crystal structure determined by X-ray diffraction shows evidence of significant contributions from zwitterionic resonance forms to the ground-state structure, and reveals centrosymmetric packing exhibiting π–π and C–H···N≡C interactions. Both solutions and films of 1 exhibit near-infrared two-photon absorption into the low-lying one-photon-allowed state with a peak two-photon cross-section of cɑ. 290 GM (measured using the white-light continuum method with a pump wavelength of 1800 nm) at a transition energy equivalent to degenerate two-photon absorption at cɑ. 1360 nm; two related chromophores are also found to show comparable near-IR two-photon cross-sections. Closed-aperture Z-scan measurements and quantum-chemical calculations indicate that the nonlinear refractive index and third-harmonic generation properties of 1 are strongly dependent on frequency in the telecommunications range, due the aforementioned two-photon resonance