All-optical 2R regeneration with a vertical microcavity based saturable absorber

International audienceThis paper gives an overview of recent demonstrations of optical 2R regeneration achieved by vertical microcavity mirror based multiple-quantum-well Saturable Absorber (SA). The potential of the device to perform WDM regeneration is firstly demonstrated through the first pigtailed saturable absorber chip implemented with 8 independent fibres using a cost effective coupling technique. The cascadability and wavelength tunability assessment of this module associated to a power limiter fibre-based function has been experimentally demonstrated at 42.6 Gbit/s. Because this method of power limiting is not a suitable solution for all-optical multichannel 2R regeneration, a new SA structure allowing a power limiting function was proposed. We describe and characterize such a structure in this paper. This new SA opens the door to a complete passive all-optical 2R regeneration relying upon a single technology, as shown in this paper through the use of two SA: SA.0 for extinction ratio enhancement and SA.1 for power level equalization allowing receiver sensitivity (up to 3.5 dB) and Q factor (up to 1.4 dB) improvement for a RZ signal at 42.6 Gbit/s. The limitation of SA.1 when the regenerator must be cascaded a large number of times is also described, leading to the observation that SA.1 should be more suitable for phase encoded formats which are more spectrally efficient than OOK formats. A SA.1 used as a phase-preserving amplitude regenerator in a 42.6 Gbit/s RZ-DPSK transmission system is therefore assessed. A fibre launched power margin of 2 dB and a receiver sensitivity improvement of 5.5 dB are obtained. Finally, we use, for the first time an SA.1 as a phase-preserving amplitude regenerator of RZ DQPSK signals. The regenerator is assessed in a recirculating loop at 28 Gbaud. The system tolerance to nonlinear phase noise is enhanced by 3 dB and the distance improvement factor was 1.3 for a BER=10-4

The Role of Nonequilibrium Dynamical Screening in Carrier Thermalization

We investigate the role played by nonequilibrium dynamical screening in the thermalization of carriers in a simplified two-component two-band model of a semiconductor. The main feature of our approach is the theoretically sound treatment of collisions. We abandon Fermi's Golden rule in favor of a nonequilibrium field theoretic formalism as the former is applicable only in the long-time regime. We also introduce the concept of nonequilibrium dynamical screening. The dephasing of excitonic quantum beats as a result of carrier-carrier scattering is brought out. At low densities it is found that the dephasing times due to carrier-carrier scattering is in picoseconds and not femtoseconds, in agreement with experiments. The polarization dephasing rates are computed as a function of the excited carrier density and it is found that the dephasing rate for carrier-carrier scattering is proportional to the carrier density at ultralow densities. The scaling relation is sublinear at higher densities, which enables a comparison with experiment.Comment: Revised version with additional refs. 12 pages, figs. available upon request; Submitted to Phys. Rev.

Coherent Optical polarization of Bulk GaAs Studied by Femtosecond Photon-Echo Spectroscopy

The nonlinear polarization close to the band gap of GaAs is studied by spectrally and temporally resolved four-wave mixing. Excitonic and free carrier contributions both excited within the bandwidth of the 100 fs pulses are distinguished for the first time. The excitonic part dominates at carrier densities below 1016 cm-3. At higher density, nonthermalized free carriers give rise to an additional component resonant to the pulse that shows a photon-echo-like time behavior. Monte Carlo simulations including the coherent polarization and the scattering dynamics of the carriers account for the data

Diquat Derivatives: Highly Active, Two-Dimensional Nonlinear Optical Chromophores with Potential Redox Switchability

In this article, we present a detailed study of structure−activity relationships in diquaternized 2,2′-bipyridyl (diquat) derivatives. Sixteen new chromophores have been synthesized, with variations in the amino electron donor substituents, π-conjugated bridge, and alkyl diquaternizing unit. Our aim is to combine very large, two-dimensional (2D) quadratic nonlinear optical (NLO) responses with reversible redox chemistry. The chromophores have been characterized as their PF_6^− salts by using various techniques including electronic absorption spectroscopy and cyclic voltammetry. Their visible absorption spectra are dominated by intense π → π^* intramolecular charge-transfer (ICT) bands, and all show two reversible diquat-based reductions. First hyperpolarizabilities β have been measured by using hyper-Rayleigh scattering with an 800 nm laser, and Stark spectroscopy of the ICT bands affords estimated static first hyperpolarizabilities β_0. The directly and indirectly derived β values are large and increase with the extent of π-conjugation and electron donor strength. Extending the quaternizing alkyl linkage always increases the ICT energy and decreases the E_(1/2) values for diquat reduction, but a compensating increase in the ICT intensity prevents significant decreases in Stark-based β_0 responses. Nine single-crystal X-ray structures have also been obtained. Time-dependent density functional theory clarifies the molecular electronic/optical properties, and finite field calculations agree with polarized HRS data in that the NLO responses of the disubstituted species are dominated by ‘off-diagonal’ β_(zyy) components. The most significant findings of these studies are: (i) β_0 values as much as 6 times that of the chromophore in the technologically important material (E)-4′-(dimethylamino)-N-methyl-4-stilbazolium tosylate; (ii) reversible electrochemistry that offers potential for redox-switching of optical properties over multiple states; (iii) strongly 2D NLO responses that may be exploited for novel practical applications; (iv) a new polar material, suitable for bulk NLO behavior

Evolution of Linear Absorption and Nonlinear Optical Properties in V-Shaped Ruthenium(II)-Based Chromophores

In this article, we describe a series of complexes with electron-rich cis-{Ru^(II)(NH_3)_4}^(2+) centers coordinated to two pyridyl ligands bearing N-methyl/arylpyridinium electron-acceptor groups. These V-shaped dipolar species are new, extended members of a class of chromophores first reported by us (Coe, B. J. et al. J. Am. Chem. Soc. 2005, 127, 4845−4859). They have been isolated as their PF_6− salts and characterized by using various techniques including ^1H NMR and electronic absorption spectroscopies and cyclic voltammetry. Reversible Ru^(III/II) waves show that the new complexes are potentially redox-switchable chromophores. Single crystal X-ray structures have been obtained for four complex salts; three of these crystallize noncentrosymmetrically, but with the individual molecular dipoles aligned largely antiparallel. Very large molecular first hyperpolarizabilities β have been determined by using hyper-Rayleigh scattering (HRS) with an 800 nm laser and also via Stark (electroabsorption) spectroscopic studies on the intense, visible d → π^* metal-to-ligand charge-transfer (MLCT) and π → π^* intraligand charge-transfer (ILCT) bands. The latter measurements afford total nonresonant β_0 responses as high as ca. 600 × 10^(−30) esu. These pseudo-C_(2v) chromophores show two substantial components of the β tensor, β_(zzz) and β_(zyy), although the relative significance of these varies with the physical method applied. According to HRS, β_(zzz) dominates in all cases, whereas the Stark analyses indicate that β_(zyy) is dominant in the shorter chromophores, but β_(zzz) and β_(zyy) are similar for the extended species. In contrast, finite field calculations predict that β_(zyy) is always the major component. Time-dependent density functional theory calculations predict increasing ILCT character for the nominally MLCT transitions and accompanying blue-shifts of the visible absorptions, as the ligand π-systems are extended. Such unusual behavior has also been observed with related 1D complexes (Coe, B. J. et al. J. Am. Chem. Soc. 2004, 126, 3880−3891)

Excitonic and free-carrier polarizations of bulk GaAs studied by femtosecond coherent spectroscopy

The transient third-order polarization at the band gap of undoped and p-doped GaAs is investigated by spectrally and temporally resolved four-wave mixing. Excitonic and free-carrier contributions simultaneously excited within the bandwidth of the 100-fs pulses are clearly distinguished by their different spectral envelopes. The excitonic part dominates at carrier densities below 1016 cm-3 and shows a time evolution governed by exciton-free-carrier scattering and by many-body effects. At higher density, the free-carrier polarization has a strength similar to the exciton contribution and exhibits a spectrum resonant to the femtosecond pulses with a photon-echo-like temporal behavior. The data are analyzed by a numerical solution of the semiconductor Bloch equations including an ensemble Monte Carlo simulation of the scattering dynamics of the carriers. The theoretical model is in good agreement with the experimental results

Ultrafast Coherent Generation of Hot Electrons Studied via Band-to-Acceptor Luminescence in GaAs

The distribution of hot electrons excited with femtosecond laser pulses is studied via spectrally resolved band-to-acceptor luminescence. Our data demonstrate for the first time that the coherent coupling between the laser pulse and the interband polarization strongly influences the initial carrier distribution. The energetic width of carrier generation is broadened due to rapid phase-breaking scattering events. Theoretical results from a Monte Carlo solution of the semiconductor Bloch equations including on the same kinetic level coherent and incoherent phenomena, are in excellent agreement with the experimental data

Consistency and discrepancy in the atmospheric response to Arctic sea-ice loss across climate models

This is the author accepted manuscript. The final version is available from Springer Nature via the DOI in this recordThe decline of Arctic sea ice is an integral part of anthropogenic climate change. Sea-ice loss is already having a significant impact on Arctic communities and ecosystems. Its role as a cause of climate changes outside of the Arctic has also attracted much scientific interest. Evidence is mounting that Arctic sea-ice loss can affect weather and climate throughout the Northern Hemisphere. The remote impacts of Arctic sea-ice loss can only be properly represented using models that simulate interactions among the ocean, sea ice, land and atmosphere. A synthesis of six such experiments with different models shows consistent hemispheric-wide atmospheric warming, strongest in the mid-to-high-latitude lower troposphere; an intensification of the wintertime Aleutian Low and, in most cases, the Siberian High; a weakening of the Icelandic Low; and a reduction in strength and southward shift of the mid-latitude westerly winds in winter. The atmospheric circulation response seems to be sensitive to the magnitude and geographic pattern of sea-ice loss and, in some cases, to the background climate state. However, it is unclear whether current-generation climate models respond too weakly to sea-ice change. We advocate for coordinated experiments that use different models and observational constraints to quantify the climate response to Arctic sea-ice loss.J.A.S. and R.B. were funded by the Natural Environment Research Council (NE/P006760/1). C.D. acknowledges the National Science Foundation (NSF), which sponsors the National Center for Atmospheric Research. D.M.S. was supported by the Met Office Hadley Centre Climate Programme (GA01101) and the APPLICATE project, which is funded by the European Union’s Horizon 2020 programme. X.Z. was supported by the NSF (ARC#1023592). P.J.K. and K.E.M. were supported by the Canadian Sea Ice and Snow Evolution Network, which is funded by the Natural Science and Engineering Research Council of Canada. T.O. was funded by Environment and Climate Change Canada (GCXE17S038). L.S. was supported by the National Oceanic and Atmospheric Administration’s Climate Program Office

Intramolecular Cooperative Effects in Multichromophoric Cavitands Exhibiting Nonlinear Optical Properties

We report on the design, synthesis, and characterization of a new class of multichromophoric cavitands based on resorcin[4]arenes. The novel compounds have exhibited high values of second-order nonlinear optical (NLO) properties, as evidenced by electric-field-induced second harmonic generation (EFISHG) measurements. Theoretical calculations indicate the presence of edge-to-face T-shaped interactions between the aromatic building blocks within these multichromophoric systems, which is further supported by the detection of hypsochromic shifts in UV-vis and upfield aromatic chemical shifts in 1H NMR. We proved for the first time that the gain in the quadratic hyperpolarizabilities of multichromophoric NLO macrocycles, originating from the near parallel orientations of the subchromophores, can be partially suppressed if the distance between the dipolar subunits falls into a specific range, where intramolecular cooperative and/or collective effects are operative. Our finding will contribute to the better understanding of the phenomenon of cooperativity in new molecular materials with promising NLO properties. (Figure Presented). © 2015 American Chemical Society

Knot-isomers of Moebius Cyclacene: How Does the Number of Knots Influence the Structure and First Hyperpolarizability?

Four large ring molecules composed by 15 nitrogen-substituted benzene rings, named as "knot-isomers of Moebius cyclacene", i.e. non-Moebius cyclacenes without a knot (0), Moebius cyclacenes with a knot (1), non-Moebius cyclacenes with two knots (2), and Moebius cyclacenes with three knots (3), are systematically studied for their structures and nonlinear optical properties. The first hyperpolarizability (beta_0) values of these four knot-isomers structures are 4693 (0) < 10484 (2) < 25419 (3) < 60846 au (1). The beta_0 values (60846 for 1, 10484 for 2 and 25419 au for 3) of the knot-isomers with knot(s) are larger than that (4693 au for 0) of the knot-isomer without a knot. It shows that the beta_0 value can be dramatically increases (13 times) by introducing the knot(s) to the cyclacenes structures. It is found that introducing knots to cyclacenes is a new means to enhance the first hyperpolarizability.Comment: 12 pages, 4 figure