Search results for " resolve"

Vibrational properties of the surface-nonbridging oxygen in silica nanoparticles

2008

By studying the site-selective luminescence spectra of oxidized silica nanoparticles we identify the electronic and the vibrational lines associated with the surface nonbridging oxygen, $\ensuremath{\equiv}{\text{Si-O}}^{\ifmmode\bullet\else\textbullet\fi{}}$. This defect emits a zero-phonon line inhomogeneously distributed around 2.0 eV with full width at half maximum of 0.04 eV, weakly coupled with the local ${\text{Si-O}}^{\ifmmode\bullet\else\textbullet\fi{}}$ stretching mode whose frequency is measured to be $920\text{ }{\text{cm}}^{\ensuremath{-}1}$. These findings are different from those of the well-characterized defect in the bulk silica thus evidencing structural peculiarities of …

Time Resolved Photoluminescence Associated with Non Bridging Oxygen Hole Centers in Irradiated Silica

2007

Self-limiting and complete oxidation of silicon nanostructures produced by laser ablation in water

2016

Oxidized Silicon nanomaterials produced by 1064 nm pulsed laser ablation in deionized water are investigated. High-resolution transmission electron microscopy coupled with energy dispersive X-ray spectroscopy allows to characterize the structural and chemical properties at a sub-nanometric scale. This analysis clarifies that laser ablation induces both self-limiting and complete oxidation processes which produce polycrystalline Si surrounded by a layer of SiO2 and amorphous fully oxidized SiO2, respectively. These nanostructures exhibit a composite luminescence spectrum which is investigated by time-resolved spectroscopy with a tunable laser excitation. The origin of the observed luminescen…

The origin of slow electron recombination processes in dye-sensitized solar cells with alumina barrier coatings

2004

We investigate the effect of a thin alumina coating of nanocrystalline TiO2 films on recombination dynamics of dye-sensitized solar cells. Both coated and uncoated cells were measured by a combination of techniques: transient absorption spectroscopy, electrochemical impedance spectroscopy, and open-circuit voltage decay. It is found that the alumina barrier reduces the recombination of photoinjected electrons to both dye cations and the oxidized redox couple. It is proposed that this observed retardation can be attributed primarily to two effects: almost complete passivation of surface trap states in TiO2 that are able to inject electrons to acceptor species, and slowing down by a factor of…

Commutators, C0-semigroups and resolvent estimates

2004

Abstract We study the existence and the continuity properties of the boundary values on the real axis of the resolvent of a self-adjoint operator H in the framework of the conjugate operator method initiated by Mourre. We allow the conjugate operator A to be the generator of a C 0 -semigroup (finer estimates require A to be maximal symmetric) and we consider situations where the first commutator [ H ,i A ] is not comparable to H . The applications include the spectral theory of zero mass quantum field models.

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…