Ultrafast dynamics and temperature effects on the quantum efficiency of the ring-opening reaction of a photochromic indolylfulgide

The ultrafast ring-opening reaction of the molecular switch 1,2-Dimethyl-3-indolylfulgide dissolved in acetonitrile is investigated by temperature dependent quantum efficiency measurements and time-resolved transient absorption spectroscopy in the ultraviolet and visible spectral range. The photoreaction is found to be thermally activated with an activation energy of about 1640 cm^− 1. The transient absorption signal is bi-exponential with the time constants τ₁ = 0.7 ps and τ₂ = 12 ps. The fast time constant is due to solvation dynamics, while the main component τ₂ is attributed to the excited state lifetime and product formation. A long-lived intermediate state in the photoreaction can be excluded.     

Formation and solvation dynamics of electrons in polyols

Using pump-probe transient absorption spectroscopy we studied the solvation dynamics of the electron in liquid polyalcohols: ethane-1,2-diol, propane-1,2-diol, propane-1,3-diol and propane-1,2,3-triol. First, transmission measurements allowed us to assess that electrons were produced via two-photon ionization of the solvent with 263 nm femtosecond laser pulses, and to determine the two-photon absorption coefficient of the polyols. Second, time-resolved absorption spectra ranging from 440 to 710 nm were measured. Our study shows that the excess electron in the diols presents an intense and wide absorption band in the visible and near-IR spectral domain at early time after photoionization. Then, for the first tens of picoseconds the electron spectrum shifts toward the blue domain and its bandwidth decreases as the red part of the initial spectrum drops rapidly while the blue part hardly evolves. Using Bayesian data analysis method, the observed picosecond solvation dynamics were reconstructed with three models: a two-step mechanism and two continuous relaxation models. Comparison between the ability of models to reproduce the experimental kinetics is in favor of a heterogeneous continuous relaxation. Recent results obtained in propane-1,2,3-triol show that the electron solvation dynamics is very fast in this solvent despite its high viscosity and highlight the role of the OH group in that process.     

Ultrafast reaction dynamics of the complete photo cycle of an indolylfulgimide studied by absorption, fluorescence and vibrational spectroscopy

The reaction dynamics of the complete photo cycle, ring-opening (C → E) and ring-closure (E → C), of N-methyl-(6-bromo-1,2-dimethyl-3-indolyl)fulgimide dissolved in acetonitrile are analysed via steady-state and ultrafast spectroscopy using transient absorption in the UV/VIS and mid-IR complemented by ultrafast fluorescence broad-band spectroscopy with a Kerr-gate setup. For the C → E ring-opening reaction induced by light at ~ 550 nm, a time constant of ~ 3 ps was found for the S₁ decay and the S₀ repopulation. Non-exponential signatures, which occur in the 10 ps time domain, were observed and are assigned to the cooling of hot molecules in the electronic ground state. The E → C reaction dynamics induced by UV-light pulses at 360 nm and 387 nm occur within less than 1 ps and are followed by vibrational cooling on the 10 ps time domain. Thus, both ring-opening and ring-closure reactions are completed within a few picoseconds. From transient IR studies and fluorescence measurements it is concluded that these pericyclic reactions occur from different geometries on the excited state potential energy surface.     

Time- and frequency-domain measurements of carrier lifetimes in GaN epilayers

Results on time-resolved study of GaN photoluminescence (PL) in a power density range from 0.5 mW/cm² under CW excitation by ultraviolet light emitting diode (UV LED) to 1 GW/cm² under pulsed excitation by YAG:Nd laser in the temperature range from 8 to 300 K are presented. Measurements of PL response in the frequency domain by using amplitude-modulated emission of a UV LED as well as time-resolved PL measurements using a streak camera and light-induced transient grating technique have been used in the study. Yellow luminescence (YL) intensity increases with increasing temperature up to 120 K and faster components in YL decay switch to slower components with increasing temperature under UV LED excitation. At low carrier densities, the trapping decreases the carrier lifetime below 250 ps, while the carrier lifetime in the same GaN sample under excitation ensuring saturation of the traps equals 2 ns.     

Investigation into the power-law dependence of fibre Bragg grating growth

We have undertaken a detailed experimental and numerical investigation of fibre Bragg grating growth rates over relatively long timescales, in which we consider the influence of zero-order UV irradiation, jitter and drift. In contrast to other studies, our results show that measurements of grating growth dynamics are in good agreement with numerical expressions describing exponential decay of a population of defect sites if the influence of small lateral displacements between the optical fibre and the modulated UV beam (jitter) are accounted for.     

Analysis of nonlinearity in a high-resolution grating interferometer

Metrological feasibilities of a high-resolution grating interferometer (GI) based on a transverse Zeeman laser are investigated. When the grating pitch equals 20 μm, a resolution of 0.7 nm is obtained by means of a heterodyne signal processing method. The comparison of two approaches for determining the residual nonlinearity is presented. One is to evaluate the maximum residual error by determining the amplitude modulation degree of the measurement signal. The other is to do a high precision calibration with a differential dual-frequency interferometer that has a higher precision. The experimental results show that the nonlinearity is no more than 25 nm which fits well with the estimating result. Analysis of the depolarization effect of the grating indicates that it has little influence on the measurement accuracy.     

Coherent transients in gases

A great variety of coherent transient processes in atomic and molecular gases is investigated. The degeneracy with respect to magnetic sublevels, which is typical of working levels of atomic and molecular transitions in gases, leads to new phenomena. In particular, the non-Faraday rotation of the coherent-response polarization vector at the 0 ↔ 1 transition is investigated in the presence of the longitudinal magnetic field in the ¹⁷⁴Yb vapor for both photon echo and stimulated photon echo. A specific relaxation channel that involves the depolarizing collisions emerges in a gas due to the degeneracy of working levels. Such collisions are especially important for atoms and are also observed in molecules. The anisotropy of the depolarizing collisions leads to a new phenomenon of the collision photon echo, which is experimentally demonstrated for the 0 ↔ 1 transition in the ¹⁷⁴Yb mixtures with atomic buffers. The velocity-dependent relaxation rates are observed for various coherent phenomena in molecular gases. The coherent control of a few coherent transient processes is implemented.     

Ultrafast X-ray experiments on structural changes in single crystals of polar molecules

Intramolecular charge transfer in aminobenzonitrile (DIABN) single crystals is studied by a combination of ultrafast techniques. The intramolecular dynamics is probed by time-resolved spectroscopy in the UV/Vis and mid-IR. The intermolecular structural response is investigated by transient X-ray scattering and transmission experiments. A theoretical analysis shows that diffuse scattering and dipole solvation determine the X-ray data. The observed dynamics results from charge transfer reaction leading to strong local changes of molecular dipole moments and related structural rearrangements in the crystal.     

Novel B/Ge codoped photosensitive fiber and dispersion compensation in an 8×10 Gbit/s DWDM system

We used the Modified Chemical Vapor Deposition (MCVD) method to fabricate a B/Ge codoped fiber with a depressed cladding in which boron and germanium were also doped, the depressed cladding was photosensitive, which can greatly suppress the cladding mode coupling. The transmission spectrum of written grating in this fiber made by the phase mask method verified its larger photosensitivity and great suppression of the cladding mode coupling. We then analyzed the Bragg wavelength tuning theory in the phase mask method in detail which gave us a more exact equation. The ultra-violet (UV) exposure system was modified, and eight cascaded Fiber Bragg Gratings (FBG) centered at different wavelengths were written in this photosensitive fiber successfully using a 248 nm KrF excimer laser and one piece of 1067 nm phase mask. Each channel spacing was 100 GH according to the Densed Wavelength Division Multiplexing (DWDM) standards of the International Telecommunication Union (ITU-T). At the same time, we also wrote in chirp in each grating by tilting the phase mask to realize dispersion compensation. The dispersion in 44 km SMF was successfully compensated by the cascaded chirped gratings in the eight channel WDM system with each channel being 10 Gbit/s.     

The (γ,p) reaction in Au

Proton energy spectra of the ¹⁹⁷Au(e,p) reaction were measured in the region between 17 and 30 MeV at three angles: 40°, 90° and 140°. Two prominent bumps were observed in the (γ,p) spectra converted using virtual photon theory. The higher-energy bump shifts with photon energies and the lower-energy one stays at 10.5 MeV. The higher-energy bump is much larger at 40° than at 140°; on the contrary the angular dependence of the lower-energy bump is small. Neither bump can be described by a statistical calculation. A calculation of a microscopic shell model shows that the lower-energy bump is attributed to the decay of proton-particle–neutron-hole pairs in the T_> states, leaving a neutron hole around the Fermi surface. The higher-energy bump can be ascribed to the direct–semidirect mechanism. This paper gives the solution to a part of the long-standing question about the origin of photo-proton emission in heavy nuclei.     

Non-Markovian dynamics in a dense atomic vapor

Two- and three-pulse photon echo spectroscopy in a dense potassium vapor reveals a non-Markovian correlation function of frequency fluctuations. Through comparison with calculations using an exciton picture a slowly-decaying component of the correlation function is attributed to long-range resonant interactions. A time-resolved photon echo experiment shows the photon-echo-like behavior at short timescales.     

Coherent phonon and electron spectroscopy on surfaces using time-resolved second-harmonic generation

pump (ω)E_probe ^*(ω)|E_probe(ω)|². This is much easier to detect than transient grating, photon echo, or four-wave mixing schemes that use higher-order nonlinearities. We have applied this technique to measure the energy gap and dephasing time of the dangling bond interband transition on the GaAs(110)-relaxed (1×1) surface. Surface-carrier/surface-phonon interaction plays an important and perhaps dominant role in surface carrier dephasing consistent with the larger electron-phonon coupling on the surface compared to the bulk. Received: 13 October 1998     

Coherent control of optical transient processes in a gas

The possibility of controlling the processes of the free-polarization decay and photon echo in a gas by means of resonant CW radiation has been shown. The photon echo and free-polarization decay are formed using the method of the Stark switching of levels in a low-intensity radiation field in the presence of an orthogonally polarized strong field. The experiments in the gas at the R(4, 3) transition in the vibrational band 0 ? 1 v₃ ¹³CH₃F in the presence of radiation from a CW CO₂ laser and the calculations by the evolution operator method show a strong effect of the high-intensity radiation field on the photon echo and free-polarization decay to its complete suppression.     

Upgrade of beamline BL08B at Taiwan Light Source from a photon‐BPM to a double‐grating SGM beamline

During the last 20 years, beamline BL08B has been upgraded step by step from a photon beam‐position monitor (BPM) to a testing beamline and a single‐grating beamline that enables experiments to record X‐ray photo‐emission spectra (XPS) and X‐ray absorption spectra (XAS) for research in solar physics, organic semiconductor materials and spinel oxides, with soft X‐ray photon energies in the range 300–1000 eV. Demands for photon energy to extend to the extreme ultraviolet region for applications in nano‐fabrication and topological thin films are increasing. The basic spherical‐grating monochromator beamline was again upgraded by adding a second grating that delivers photons of energy from 80 to 420 eV. Four end‐stations were designed for experiments with XPS, XAS, interstellar photoprocess systems (IPS) and extreme‐ultraviolet lithography (EUVL) in the scheduled beam time. The data from these experiments show a large count rate in core levels probed and excellent statistics on background normalization in the L‐edge adsorption spectrum.     

Nitride-based photodetectors: from visible to X-ray monitoring

The performance of nitride-based photodetectors is investigated beyond the usual near-UV (400–300 nm) and mid-UV (300–200 nm) operation ranges. The responses of metal–semiconductor–metal (MSM) photodiodes were analyzed in the vacuum–UV and soft X-ray regions. To interpret the results, the absorption properties and the attributes of each of the photons with energies for producing multiple electron–hole pairs were considered. The soft X-ray characterization showed that in-plane MSMs worked efficiently up to photon energies of 600 eV. Above this value, the absorption decrease makes the diffusion length and layer thickness become critical parameters for the detector behavior. To perform detection in the violet and near-UV, InGaN-based photoconductors were fabricated and spectrally characterized. The devices presented abrupt wavelength cut-offs, demonstrating that the InGaN compositional fluctuations were tolerable up to In contents of 10% for fabricating selective photodetectors. Back-face illumination allowed us to obtain bandpass detectors for these spectral ranges.     

Finite Range of Large Perturbations in Hamiltonian Dynamics

The dynamics defined by the Hamiltonian , where the _m are fixed random phases, is investigated for large values of A, and for . For a given P ^* and for , this Hamiltonian is transformed through a rigorous perturbative treatment into a Hamiltonian where the sum of all the nonresonant terms, having a Q dependence of the kind cos(kQ – nt + _m) with \Delta \upsilon$$ " align="middle" border="0"> , is a random variable whose r.m.s. with respect to the _m is exponentially small in the parameter . Using this result, a rationale is provided showing that the statistical properties of the dynamics defined by H, and of the reduced dynamics including at each time t only the terms in H such that , can be made arbitrarily close by increasing . For practical purposes close to 5 is enough, as confirmed numerically. The reduced dynamics being nondeterministic, it is thus analytically shown, without using the random-phase approximation, that the statistical properties of a chaotic Hamiltonian dynamics can be made arbitrarily close to that of a stochastic dynamics. An appropriate rescaling of momentum and time shows that the statistical properties of the dynamics defined by H can be considered as independent of A, on a finite time interval, for A large. The way these results could generalize to a wider class of Hamiltonians is indicated.     

Characterisation of defects in rare earth implanted GaN by deep level transient spectroscopy

Deep level transient spectroscopy (DLTS) was used to investigate the electrical properties of GaN implanted with the rare earth (RE) ions erbium and thulium. The GaN layers have been grown by metal-organic chemical vapor deposition (MOCVD) onto (0001) sapphire substrates. We used the channeled implantation geometry to implant a dose of 5×10¹⁴ RE cm⁻² with an energy of 150 keV. For each species, two different annealing procedures were used in a nitrogen atmosphere for 120 s. Indeed, the annealing temperature plays an important role in the lattice recovery, even if RE-related defects remain present. After annealing at 1000 C, the appearance of two new peaks, for both studied RE ions, is associated with the lattice damage induced by the implantation, such as the presence of nitrogen vacancies. After annealing at 1100 C, the recovery of the lattice is observed while a hole trap appears for both implanted RE ions with corresponding energy values E_v+0.61 eV and E_v+1.59 eV, in the case of Er and Tm, respectively.     

Phase contribution to dynamic gratings recorded in Er-doped fiber with saturable absorption

Experimental observation of phase (i.e. refractive index) component in the dynamic gratings recorded in erbium-doped optical fiber with saturation of optical absorption is reported. We utilized configuration of transient two-wave mixing with rectangular phase modulation of one of counterpropagating recording waves, where unshifted phase grating resulted in a transient energy exchange. The reported experiments were performed with heavily doped (≈5400 ppm erbium) fibers in a wide spectral range of Er³⁺ fundamental absorption at selected laser wavelengths 1492, 1526, 1549, and 1568 nm. Relative contribution of phase grating was especially large (up to ≈100% of the maximal amplitude component) at the opposite sides of the investigated spectral range and was significantly lower in its central part. The amplitude grating was found especially strong at short wavelength side of the spectrum (i.e. at 1492 nm), where the grating amplitude proved to be only two times lower than the theoretically predicted from consideration of two-level model.