Electrical pump & probe and injected carrier losses quantification in Er doped Si slot waveguides

Electrically driven Er3+ doped Si slot waveguides emitting at 1530 nm are demonstrated. Two different Er3+ doped active layers were fabricated in the slot region: a pure SiO2 and a Si-rich oxide. Pulsed polarization driving of the waveguides was used to characterize the time response of the electroluminescence (EL) and of the signal probe transmission in 1 mm long waveguides. Injected carrier absorption losses modulate the EL signal and, since the carrier lifetime is much smaller than that of Er3+ ions, a sharp EL peak was observed when the polarization was switched off. A time-resolved electrical pump & probe measurement in combination with lock-in amplifier techniques allowed to quantify the injected carrier absorption losses. We found an extinction ratio of 6 dB, passive propagation losses of about 4 dB/mm, and a spectral bandwidth > 25 nm at an effective d.c. power consumption of 120 μW. All these performances suggest the usage of these devices as electro-optical modulators.

Femtosecond pump-probe study of the spreading and recurrence of a vibrational wave packet in Na_2

The motion of a vibrational wave packet in the bound A(^1 \summe^+_u) electronic state of the sodium dimer is detected in a femtosecond pump/probe molecular beam experiment. For short times harmonic motion is seen in the total ion yield of Na^+_2 as a function of delay time between the two laser pulses. The spreading of the wave packet results in the loss of the periodic variation of the ion signal. For longer delay times (47 ps) the wave packet regains its initial form which is reflected in the revival structure of the Na^+_2 signal. Time-dependent quantum calculations reproduce the measured effects.

The relaxation dynamics of the excited electronic states of retinal in bacteriorhodopsin by two-pump-probe femtosecond studies

We present the results of two-pump and probe femtosecond experiments designed to follow the relaxation dynamics of the lowest excited state (S1) populated by different modes. In the first mode, a direct (S0 → S1) radiative excitation of the ground state is used. In the second mode, an indirect excitation is used where the S1 state is populated by the use of two femtosecond laser pulses with different colors and delay times between them. The first pulse excites the S0 → S1 transition whereas the second pulse excites the S1 → Sn transition. The nonradiative relaxation from the Sn state populates the lowest excited state. Our results suggest that the S1 state relaxes faster when populated nonradiatively from the Sn state than when pumped directly by the S0 → S1 excitation. Additionally, the Sn → S1 nonradiative relaxation time is found to change by varying the delay time between the two pump pulses. The observed dependence of the lowest excited state population as well as its dependence on the delay between the two pump pulses are found to fit a kinetic model in which the Sn state populates a different surface (called S′1) than the one being directly excited (S1). The possible involvement of the Ag type states, the J intermediate, and the conical intersection leading to the S0 or to the isomerization product (K intermediate) are discussed in the framework of the proposed model.

High-frequency conductivity of optically excited charge carriers in hydrogenated nanocrystalline silicon investigated by spectroscopic femtosecond pump-probe reflectivity measurements

We report an investigation into the high-frequency conductivity of optically excited charge carriers far from equilibrium with the lattice. The investigated samples consist of hydrogenated nanocrystalline silicon films grown on a thin film of silicon oxide on top of a silicon substrate. For the investigation, we used an optical femtosecond pump-probe setup to measure the reflectance change of a probe beam. The pump beam ranged between 580 and 820nm, whereas the probe wavelength spanned 770 to 810nm. The pump fluence was fixed at 0.6mJ/cm2. We show that at a fixed delay time of 300fs, the conductivity of the excited electron-hole plasma is described well by a classical conductivity model of a hot charge carrier gas found at Maxwell-Boltzmann distribution, while Fermi-Dirac statics is not suitable. This is corroborated by values retrieved from pump-probe reflectance measurements of the conductivity and its dependence on the excitation wavelength and carrier temperature. The conductivity decreases monotonically as a function of the excitation wavelength, as expected for a nondegenerate charge carrier gas.

Combined Monte Carlo and quantum mechanics study of the solvatochromism of phenol in water. The origin of the blue shift of the lowest pi-pi* transition

A combined and sequential use of Monte Carlo simulations and quantum mechanical calculations is made to analyze the spectral shift of the lowest pi-pi* transition of phenol in water. The solute polarization is included using electrostatic embedded calculations at the MP2/aug-cc-pVDZ level giving a dipole moment of 2.25 D, corresponding to an increase of 76% compared to the calculated gas-phase value. Using statistically uncorrelated configurations sampled from the MC simulation,first-principle size-extensive calculations are performed to obtain the solvatochromic shift. Analysis is then made of the origin of the blue shift. Results both at the optimized geometry and in room-temperature liquid water show that hydrogen bonds of water with phenol promote a red shift when phenol is the proton-donor and a blue shift when phenol is the proton-acceptor. In the case of the optimized clusters the calculated shifts are in very good agreement with results obtained from mass-selected free jet expansion experiments. In the liquid case the contribution of the solute-solvent hydrogen bonds partially cancels and the total shift obtained is dominated by the contribution of the outer solvent water molecules. Our best result, including both inner and outer water molecules, is 570 +/- 35 cm(-1), in very good agreement with the small experimental shift of 460 cm(-1) for the absorption maximum.

Femtosecond time-resolved wave packet motion in molecular multiphoton ionization and fragmentation

The dynamics of molecular multiphoton ionization and fragmentation of a diatomic molecule (Na_2) have been studied in molecular beam experiments. Femtosecond laser pulses from an amplified colliding-pulse mode-locked (CPM) ring dye laser are employed to induce and probe the molecular transitions. The final continuum states are analyzed by photoelectron spectroscopy, by ion mass spectrometry and by measuring the kinetic energy of the formed ionic fragments. Pump-probe spectra employing 70-fs laser pulses have been measured to study the time dependence of molecular multiphoton ionization and fragmentation. The oscillatory structure of the transient spectra showing the dynamics on the femtosecond time scale can best be understood in terms of the motion of wave packets in bound molecular potentials. The transient Na_2^+ ionization and the transient Na^+ fragmentation spectra show that contributions from direct photoionization of a singly excited electronic state and from excitation and autoionization of a bound doubly excited molecular state determine the time evolution of molecular multiphoton ionization.

Femtosecond time-resolved molecular multiphoton ionization: the Na_2 system

We report here the first experimental study of femtosecond time-resolved molecular multiphoton ionization. Femtosecond pump-probe techniques are combined with time-of-flight spectroscopy to measure transient ionization spectra of Na_2 in a molecular-beam experiment. The wave-packet motions in different molecular potentials show that incoherent contributions from direct photoionization of a singly excited state and from excitation and autoionization of a bound doubly excited molecular state determine the observed transient ionization signal.

Fundamental interactions of molecules (Na_2, Na_3) with intense femtosecond laser pulses

The real-time dynamics of multiphoton ionization and fragmentation of molecules Na_2 and Na_3 has been studied in molecular beam experiments employing ion and electron spectroscopy together with femtosecond pump-probe techniques. Experiments with Na_2 and Na_3 reveal unexpected features of the dynamics of the absorption of several photons as seen in the one- and three-dimensional vibrational wave packet motion in different potential surfaces and in high laser fields: In Na_2 a second major resonance-enhanced multiphoton ionization (REMPI) process is observed, involving the excitation of two electrons and subsequent electronic autoionization. The possibility of controlling a reaction by controlling the duration of propagation of a wave packet on an electronically-excited surface is demonstrated. In high laser fields, the contributions from direct photoionization and from the second REMPI process to the total ion yield change, due to different populations in the electronic states participating in the multiphoton ionization (MPI) processes. In addition, a vibrational wave packet motion in the electronic ground state is induced through stimulated emission pumping by the pump laser. The 4^1 \summe^+_g shelf state of Na_2 is given as an example for performing frequency spectroscopy of highlying electronic states in the time domain. Pure wave packet effects, such as the spreading and the revival of a vibrational wave packet, are investigated. The three-dimensional wave packet motion in the Na_3 reflects the normal modes in the X and B states, and shows in addition the pseudorotational motion in the B state in real time.

Técnica de bombeio e prova para medidas de absorção de estado excitado e de emissão estimulada, em materiais sólidos dopados com íons terras raras

Rare earth ion doped solid state materials are the most important active media of near-infrared and visible lasers and other photonic devices. In these ions, the occurrence of Excited State Absorptions (ESA), from long lived electronic levels, is commonplace. Since ESA can deeply affect the efficiencies of the rare earth emissions, evaluation of these transitions cross sections is of greatest importance in predicting the potential applications of a given material. In this paper a detailed description of the pump-probe technique for ESA measurements is presented, with a review of several examples of applications in Nd3+, Tm3+ and Er3+ doped materials.

Pulse train fluorescence technique for measuring triplet state dynamics

We report on a method to study the dynamics of triplet formation based on the fluorescence signal produced by a pulse train. Basically, the pulse train acts as sequential pump-probe pulses that precisely map the excited-state dynamics in the long time scale. This allows characterizing those processes that affect the population evolution of the first excited singlet state, whose decay gives rise to the fluorescence. The technique was proven to be valuable to measure parameters of triplet formation in organic molecules. Additionally, this single beam technique has the advantages of simplicity, low noise and background-free signal detection. (C) 2011 Optical Society of America

Er-Coupled Si Nanocluster Waveguide

Rib-loaded waveguides containing Er3+-coupled Si nanoclusters (Si-nc) have been produced to observe optical gain at 1535 nm. The presence ofSi-nc strongly improves the efficiency ofEr 3+ excitation but may introduce optical loss mechanisms, such as Mie scattering and confined carrier absorption. Losses strongly affect the possibility of obtaining positive optical gain. Si-nc-related losses have been minimized to 1 dB/cm by lowering the annealing time ofthe Er3+-doped silicon-rich oxide deposited by reactive magnetron cosputtering. Photoluminescence (PL) and lifetime measurements show that all Er3+ ions are optically active while those that can be excited at high pump rates via Si-nc are only a small percentage. Er3+ absorption cross section is found comparable to that ofEr 3+ in SiO 2.However, dependence on the effective refractive index has been found. In pump-probe measurements, it is shown how the detrimental role ofconfined carrier absorption can be attenuated by reducing the annealing time. A maximum signal enhancement ofabout 1.34 at 1535 nm was measured.

Técnica de bombeio e prova para medidas de absorção de estado excitado e de emissão estimulada, em materiais sólidos dopados com íons terras raras

Rare earth ion doped solid state materials are the most important active media of near-infrared and visible lasers and other photonic devices. In these ions, the occurrence of Excited State Absorptions (ESA), from long lived electronic levels, is commonplace. Since ESA can deeply affect the efficiencies of the rare earth emissions, evaluation of these transitions cross sections is of greatest importance in predicting the potential applications of a given material. In this paper a detailed description of the pump-probe technique for ESA measurements is presented, with a review of several examples of applications in Nd3+, Tm3+ and Er3+ doped materials.

Localization of the mechanism of pH-dependent non- photochemical fluorescence quenching in thylakoid membranes

Higher plants have evolved a well-conserved set of photoprotective mechanisms, collectively designated Non-Photochemical Quenching of chlorophyll fluorescence (qN), to deal with the inhibitory absorption of excess light energy by the photosystems. Their main contribution originates from safe thermal deactivation of excited states promoted by a highly-energized thylakoid membrane, detected via lumen acidification. The precise origins of this energy- or LlpH-dependent quenching (qE), arising from either decreased energy transfer efficiency in PSII antennae (~ Young & Frank, 1996; Gilmore & Yamamoto, 1992; Ruban et aI., 1992), from alternative electron transfer pathways in PSII reaction centres (~ Schreiber & Neubauer, 1990; Thompson &Brudvig, 1988; Klimov et aI., 1977), or from both (Wagner et aI., 1996; Walters & Horton, 1993), are a source of considerable controversy. In this study, the origins of qE were investigated in spinach thylakoids using a combination of fluorescence spectroscopic techniques: Pulse Amplitude Modulated (PAM) fluorimetry, pump-probe fluorimetry for the measurement of PSII absorption crosssections, and picosecond fluorescence decay curves fit to a kinetic model for PSII. Quenching by qE (,..,600/0 of maximal fluorescence, Fm) was light-induced in circulating samples and the resulting pH gradient maintained during a dark delay by the lumenacidifying capabilities of thylakoid membrane H+ ATPases. Results for qE were compared to those for the addition of a known antenna quencher, 5-hydroxy-1,4naphthoquinone (5-0H-NQ), titrated to achieve the same degree of Fm quenching as for qE. Quenching of the minimal fluorescence yield, F0' was clear (8 to 130/0) during formation of qE, indicative of classical antenna quenching (Butler, 1984), although the degree was significantly less than that achieved by addition of 5-0H-NQ. Although qE induction resulted in an overall increase in absorption cross-section, unlike the decrease expected for antenna quenchers like the quinone, a larger increase in crosssection was observed when qE induction was attempted in thylakoids with collapsed pH gradients (uncoupled by nigericin), in the absence of xanthophyll cycle operation (inhibited by DTT), or in the absence of quenching (LlpH not maintained in the dark due to omission of ATP). Fluorescence decay curves exhibited a similar disparity between qE-quenched and 5-0H-NQ-quenched thylakoids, although both sets showed accelerated kinetics in the fastest decay components at both F0 and Fm. In addition, the kinetics of dark-adapted thylakoids were nearly identical to those in qEquenched samples at F0' both accelerated in comparison with thylakoids in which the redox poise of the Oxygen-Evolving Complex was randomized by exposure to low levels of background light (which allowed appropriate comparison with F0 yields from quenched samples). When modelled with the Reversible Radical Pair model for PSII (Schatz et aI., 1988), quinone quenching could be sufficiently described by increasing only the rate constant for decay in the antenna (as in Vasil'ev et aI., 1998), whereas modelling of data from qE-quenched thylakoids required changes in both the antenna rate constant and in rate constants for the reaction centre. The clear differences between qE and 5-0H-NQ quenching demonstrated that qE could not have its origins in the antenna alone, but is rather accompanied by reaction centre quenching. Defined mechanisms of reaction centre quenching are discussed, also in relation to the observed post-quenching depression in Fm associated with photoinhibition.

Signature optique d’effet Stark dans une bicouche de CuPc:C60

Les hétérojonctions formées de deux matériaux, un donneur et un accepteur (D/A), sont la base de la majorité des mélanges photovoltaïques organiques. Les mécanismes de séparation des charges dans ces systèmes représentent aujourd'hui l'un des sujets les plus chauds et les plus débattus dans ce domaine. Nous entrons au coeur de ce débat en choisissant un système D/A à base de phtalocyanine de cuivre (CuPc) et de fullerène (C60). Pour sonder les états excités de nos molécules et obtenir de l'information sur les phénomènes à l'interface D/A, nous réalisons une expérience pompe-sonde, appelée absorption photoinduite (PIA). Nous y mesurons le changement fractionnaire de transmission au travers de l'échantillon. Les mesures de PIA sont réalisées à l'état de quasi équilibre, à T=10K. Nous observons une modulation prononcée dans la région du photoblanchiment de l'état fondamental qui nous indique que la pompe induit un décalage du spectre d'absorption de l'état fondamental. Ce décalage peut être expliqué par deux processus : soit l'échantillon est chauffé par la pompe (effet thermique) ou bien des charges sont créées à l'interface entre les deux matériaux (effet Stark). La dépendance en température du spectre d'absorption entre 10K et 290K montre une signature thermique pour un changement de température de 80K. Grâce au ratio des raies Raman anti-Stokes et Stokes, nous démontrons que la pompe chauffe l'échantillon de 34 K, température insuffisante pour attribuer notre signal à un effet thermique. Nous évaporons ensuite la bicouche CuPc/C60 sur de l'ITO et du saphir, substrats qui possèdent des conductivités thermiques différentes et nous observons le même signal de PIA, excluant par le fait même l'hypothèse de l'effet thermique. Puisque notre étude est comparable à la spectroscopie à effet Stark, nous procédons à une analyse similaire en comparant notre signal de PIA au spectre de la transmittance et à ses dérivés première et seconde. Nous observons alors que notre signal reproduit presque parfaitement la dérivée seconde de la transmittance. Ces résultats sont conformes à une signature optique d'effet Stark due à la création de charges à l'interface D/A.

Photothermal deflection measurement on heat transport in GaAs epitaxial layers

In this paper, we report the in-plane and cross-plane measurements of the thermal diffusivity of double epitaxial layers of n-type GaAs doped with various concentrations of Si and a p-type Be-doped GaAs layer grown on a GaAs substrate by the molecular beam epitaxial method, using the laser-induced nondestructive photothermal deflection technique. The thermal diffusivity value is evaluated from the slope of the graph of the phase of the photothermal deflection signal as a function of pump-probe offset. Analysis of the data shows that the cross-plane thermal diffusivity is less than that of the in-plane thermal diffusivity. It is also seen that the doping concentration has a great influence on the thermal diffusivity value. Measurement of p-type Be-doped samples shows that the nature of the dopant also influences the effective thermal diffusivity value. The results are interpreted in terms of a phonon-assisted heat transfer mechanism and the various scattering process involved in the propagation of phonons.