Search results for "transient absorption"
showing 10 items of 15 documents
Photodynamics of a Molecular Water-Soluble Nanocluster Identified as Au130(pMBA)50
2015
Photodynamics of a highly monodisperse sample of a water-soluble gold nanocluster tentatively identified as Au130(pMBA)50 (pMBA = p-mercaptobenzoic acid) was studied by mid-IR transient absorption spectroscopy with visible excitation. The observed long-lived excited states (>1 ns) indicate a molecular behavior of the cluster. By combining the transient absorption data with DFT calculation results the observed relaxation dynamics could be fully explained by identifying several relaxation processes involving singlet and triplet manifolds. The results indicate that the cluster may have interesting transient magnetic properties due to a long-lived triplet population.
Molecule-like photodynamics of Au102(pMBA)44 nanocluster.
2015
Photophysical properties of a water-soluble cluster Au102(pMBA)44 (pMBA = para-mercaptobenzoic acid) are studied by ultrafast time-resolved mid-IR spectroscopy and density functional theory calculations in order to distinguish between molecular and metallic behavior. In the mid-IR transient absorption studies, visible or near-infrared light is used to electronically excite the sample, and the subsequent relaxation is monitored by studying the transient absorption of a vibrational mode in the ligands. Based on these studies, a complete picture of energy relaxation dynamics is obtained: (1) 0.5-1.5 ps electronic relaxation, (2) 6.8 ps vibrational cooling, (3) intersystem crossing from the low…
Ab Initio Simulation of Attosecond Transient Absorption Spectroscopy in Two-Dimensional Materials
2018
We extend the first-principles analysis of attosecond transient absorption spectroscopy to two-dimensional materials. As an example of two-dimensional materials, we apply the analysis to monolayer hexagonal boron nitride (h-BN) and compute its transient optical properties under intense few-cycle infrared laser pulses. Nonadiabatic features are observed in the computed transient absorption spectra. To elucidate the microscopic origin of these features, we analyze the electronic structure of h-BN with density functional theory and investigate the dynamics of specific energy bands with a simple two-band model. Finally, we find that laser-induced intraband transitions play a significant role in…
Photodynamics studies of ligand-protected gold nanoclusters by using ultrafast transient infrared spectroscopy
2015
Highly monodisperse samples of three ligand-protected gold nanoclusters Au102(pMBA)44, Au144(SC2H4Ph)60, and a cluster tentatively identified as Au130(pMBA)50, were characterized by UV/vis and infrared spectroscopy, and their photodynamics was studied by transient absorption spectroscopy. The dynamics study for each cluster was performed by electronically exciting the cluster with a pump pulse in the visible or near infrared region and by monitoring the transient absorption of vibrational modes of the ligands with a mid-IR probe pulse. The photodynamics studies were used to determine the molecular or metallic behavior of the cluster, and also to gain important size dependent information abo…
Transient absorption with a femtosecond tunable excitation pump reveals the emission kinetics of color centers in amorphous silica.
2021
We report a set of femtosecond (fs) transient absorption (TA) measurements following the dynamics of the so-called nonbridging oxygen hole center in silica, a model color center in wide bandgap amorphous solids, characterized by a very large Stokes shift between the UV excitation and its associated red emission at 1.9 eV. The changes in the TA spectrum were probed in the UV-visible range at various delays after photoexcitation and analyzed as a function of the UV excitation energy, in single-photon absorption conditions. The combination of the experiments helps to clarify the defect photocycle, highlighting how TA measurements with tunable UV excitation could represent a powerful tool to in…
Photocycle of point defects in highly- and weakly-germanium doped silica revealed by transient absorption measurements with femtosecond tunable pump.
2022
AbstractWe report pump-probe transient absorption measurements addressing the photocycle of the Germanium lone pair center (GLPC) point defect with an unprecedented time resolution. The GLPC is a model point defect with a simple and well-understood electronic structure, highly relevant for several applications. Therefore, a full explanation of its photocycle is fundamental to understand the relaxation mechanisms of such molecular-like systems in solid state. The experiment, carried out exciting the sample resonantly with the ultraviolet (UV) GLPC absorption band peaked at 5.1 eV, gave us the possibility to follow the defect excitation-relaxation dynamics from the femto-picosecond to the nan…
Heptagon-Containing Nanographene Embedded into [10]Cycloparaphenylene
2023
We report the synthesis and characterization of a novel type of nanohoop, consisting of a cycloparaphenylene derivative incorporating a curved heptagon-containing π-extended polycyclic aromatic hydrocarbon (PAH) unit. We demonstrate that this new macrocycle behaves as a supramolecular receptor of curved π-systems such as fullerenes C60 and C70, with remarkably large binding constants (ca. 107 M−1), as estimated by fluorescence measurements. Nanosecond and femtosecond spectroscopic analysis show that these host-guest complexes are capable of quasi-instantaneous charge separation upon photoexcitation, due to the ultrafast charge transfer from the macrocycle to the complexed fullerene. These r…
Characterization of Locally Excited and Charge-Transfer States of the Anticancer Drug Lapatinib by Ultrafast Spectroscopy and Computational Studies
2020
[EN] Lapatinib (LAP) is an anticancer drug, which is metabolized to theN- and O-dealkylated products (N-LAP andO-LAP, respectively). In view of the photosensitizing potential of related drugs, a complete experimental and theoretical study has been performed on LAP,N-LAP andO-LAP, both in solution and upon complexation with human serum albumin (HSA). In organic solvents, coplanar locally excited (LE) emissive states are generated; they rapidly evolve towards twisted intramolecular charge-transfer (ICT) states. By contrast, within HSA only LE states are detected. Accordingly, femtosecond transient absorption reveals a very fast switching (ca. 2 ps) from LE (lambda(max)=550 nm) to ICT states (…
Effect of Halogen Ions on the Photocycle of Fluorescent Carbon Nanodots
2019
Carbon dots (C-dots) are well-known for their strong sensitivity to the environment, which reflects on intensity and shape changes of their fluorescence, induced by various interacting ions and molecules in solution. Although these interactions have been extensively studied in the last few years, especially in view of their possible sensing applications, the existing works have mostly focused on the quenching of C-dot fluorescence induced by metal cations. In fact, these latter easily bind to C-dots surfaces, which are negatively charged in most cases, promoting an electron transfer from the surface to them. Much less is known from the literature on the effect induced on C-dots by prototypi…
Strongly Coupled Coherent Phonons in Single-Layer MoS 2
2019
We present a transient absorption setup combining broadband detection over the visible-UV range with high temporal resolution ($\sim$20fs) which is ideally suited to trigger and detect vibrational coherences in different classes of materials. We generate and detect coherent phonons (CPs) in single layer (1L) MoS$_2$, as a representative semiconducting 1L-transition metal dichalcogenide (TMD), where the confined dynamical interaction between excitons and phonons is unexplored. The coherent oscillatory motion of the out-of-plane $A'_{1}$ phonons, triggered by the ultrashort laser pulses, dynamically modulates the excitonic resonances on a timescale of few tens fs. We observe an enhancement by…