Search results for "Time Resolved"
showing 10 items of 41 documents
Luminescence of the surface nonbridging oxygen hole center in silica: Spectral and decay properties
2008
We investigated the red luminescence in a porous film of silica nanoparticles, originating from surface nonbridging oxygen hole centers. The excitation spectrum was measured from 1.8 to 8.0 eV by a tunable laser system and a synchrotron radiation source; this spectrum evidences a peak at 2.0 eV, nearly overlapping with the emission, and an ultraviolet broadband with peaks at 4.8 and 6.0 eV. The emission is characterized by a spectrum with two subbands split by 0.07 eV, its decay occurs with lifetime longer than 30 microsec and undergoes a thermal quenching by a factor aboout 2 with increasing temperature from 10 to 290 K. The optical characteristics of surface and bulk centers are discussed…
Do fluorescence and transient absorption probe the same intramolecular charge transfer state of 4-(dimethylamino)benzonitrile?
2009
International audience; We present here the results of time-resolved absorption and emission experiments for 4-(dimethylamino)benzonitrile in solution, which suggest that the fluorescent intramolecular charge transfer (ICT) state may differ from the twisted ICT (TICT) state observed in transient absorption.
Observation of an excitonic Mott transition through ultrafast core-cum-conduction photoemission spectroscopy
2020
Time-resolved soft-X-ray photoemission spectroscopy is used to simultaneously measure the ultrafast dynamics of core-level spectral functions and excited states upon excitation of excitons in WSe$_2$. We present a many-body approximation for the Green's function, which excellently describes the transient core-hole spectral function. The relative dynamics of excited-state signal and core levels reveals a delayed core-hole renormalization due to screening by excited quasi-free carriers, revealing an excitonic Mott transition. These findings establish time-resolved core-level photoelectron spectroscopy as a sensitive probe of subtle electronic many-body interactions and an ultrafast electronic…
Heterogeneity of aggregates in the fibrillation mechanisms of proteins probed by time resolved fluorescence
2010
Under appropriate conditions almost all proteins are able to aggregate to form long, well-ordered and beta-sheet rich arrays known as amyloid fibrils. The formation of such structures involves complex intra and intermolecular interactions modulated by the structure and dynamics of the native protein, and by the physico-chemical properties of the solvent. Multiple interactions and cross-feedback during the aggregation pathway cause different ultimate aggregates’ morphologies and the possible simultaneous occurrence of multiple species. The structural definition of such assemblies is complicated by the polymorphism of the amyloid fibrils. Aim of this study is to inquire on the different natur…
Real-time observation of a correlation-driven sub 3 fs charge migration in ionised adenine
2021
Sudden ionisation of a relatively large molecule can initiate a correlation-driven process dubbed charge migration, where the electron density distribution is expected to rapidly move along the molecular backbone. Capturing this few-femtosecond or attosecond charge redistribution would represent the real-time observation of electron correlation in a molecule with the enticing prospect of following the energy flow from a single excited electron to the other coupled electrons in the system. Here, we report a time-resolved study of the correlation-driven charge migration process occurring in the nucleic-acid base adenine after ionisation with a 15–35 eV attosecond pulse. We find that the produ…
Quantum correlation of electron and ion energy in the dissociative strong-field ionization of H2
2023
We report on the strong field ionization of H2 by a corotating two-color laser field. We measure the electron momentum distribution in coincidence with the kinetic energy release (KER) of dissociating hydrogen molecules. In addition to a characteristic half-moon structure, we observe a low-energy structure in the electron momentum distribution at a KER of about 3.5 eV. We speculate that the outgoing electron interacts with the molecular ion, despite the absence of classical recollisions under these conditions. Time-dependent density functional theory simulations support our conclusions.
Femtosecond Raman time-resolved molecular spectroscopy
2004
International audience; The applicability of several femtosecond time resolved non-linear coherent techniques such as Raman induced polarization spectroscopy (RIPS), degenerate four-wave mixing (DFWM) and coherent anti-Stokes Raman spectroscopy (CARS) for molecular spectroscopy is presented. All methods rely on the initial coherent excitation of molecular states producing wavepackets, whose time evolution is then measured. In the case of RIPS and DFWM only pure rotational transitions are involved, whereas in CARS vibrational states can be excited. First the methodology of concentration and temperature measurements using RIPS in gas mixtures involving N2, CO2, O2, and N2O is shown. In additi…
Bright Visible Luminescence in Silica Nanoparticles
2011
International audience; We demonstrate that a porous film of silica nanoparticles emits a bright visible luminescence associated with defects stabilized by oxygen chemisorption at oxygen deficient center sites. Time-resolved spectra excited by a tunable laser allow us to distinguish the luminescence at 1.99 eV, characteristic of the nonbridging oxygen hole center (NBOHC) (Si-O)3 Si-O*, and a fast and a slow emission: the first (lifetime τ ≈ 25 ns) is peaked at 2.27 eV with an excitation spectrum centered at 5.5 eV; the second (τ ≈ 7.5 μs) is peaked at 2.41 eV and is excited around 3.2 and 5.2 eV. Reaction in an air atmosphere leads to the disappearance of the NBOHC luminescence and of the …
Alignment of linear molecules by short duration laser pulses
2005
Alignment of linear molecules is efficiently induced by strong linearly polarized laser pulses. In the case of short pulses with respect to molecular rotation, periodic alignment appears in field-free conditions after the extinction of the field. This manuscript presents three techniques where the value of allows to quantify alignment without molecular dissociation nor additional alignment. They use a weak time-delayed probe pulse which experiences the optical properties of an aligned sample and shows modification of its characteristics. The first of them measures a depolarization due to the birefringence of the sample. The second one is based on the defocusing produced by the spatial distr…