Search results for "ultrafast"
showing 10 items of 170 documents
Ligand-Centred Fluorescence and Electronic Relaxation Cascade at Vibrational Time Scales in Transition-Metal Complexes
2015
Using femtosecond-resolved photoluminescence up-conversion, we report the observation of the fluorescence of the high-lying ligand-centered (LC) electronic state upon 266 nm excitation of an iridium complex, Ir(ppy)(3), with a lifetime of 70 +/- 10 fs. It is accompanied by a simultaneous emission of all lower-lying electronic states, except the lowest triplet metal-to-ligand charge-transfer ((MLCT)-M-3) state that shows a rise on the same time scale. Thus, we observe the departure, the intermediate steps, and the arrival of the relaxation cascade spanning similar to 1.6 eV from the (LC)-L-1 state to the lowest 3MLCT state, which then yields the long-lived luminescence of the molecule. This …
Negative and positive Kerr nonlinearity of air calibrated with transient molecular alignment
2009
Talk given by O. Faucher; International audience; Nonlinear electronic Kerr index of the major air constituents has been measured up to high order terms using transient molecular alignment as a reference. Sign reversal associated to negative nonlinearity is observed above a pulse intensity of 26 TW/cm^.2
Unravelling the Intertwined Atomic and Bulk Nature of Localised Excitons by Attosecond Spectroscopy
2021
The electro-optical properties of most semiconductors and insulators of technological interest are dominated by the presence of electron-hole quasi-particles, called excitons. The manipulation of excitons in dielectrics has recently received great attention, with possible applications in different fields including optoelectronics and photonics. Here, we apply attosecond transient reflection spectroscopy in a sequential two-foci geometry and observe sub-femtosecond dynamics of a core-level exciton in bulk MgF2 single crystals. Furthermore, we access absolute phase delays, which allow for an unambiguous comparison with theoretical calculations. Our results show that excitons surprisingly exhi…
Ultrafast Interface Charge Separation in Carbon Nanodot-Nanotube Hybrids
2021
Carbon dots are an emerging family of zero-dimensional nanocarbons behaving as tunable light harvesters and photoactivated charge donors. Coupling them to carbon nanotubes, which are well-known electron acceptors with excellent charge transport capabilities, is very promising for several applications. Here, we first devised a route to achieve the stable electrostatic binding of carbon dots to multi- or single-walled carbon nanotubes, as confirmed by several experimental observations. The photoluminescence of carbon dots is strongly quenched when they contact either semiconductive or conductive nanotubes, indicating a strong electronic coupling to both. Theoretical simulations predict a favo…
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…
Realization of time-resolved two-vacuum-ultraviolet-photon ionization
2009
International audience; Ultrafast dynamics of excited molecules is studied through time-resolved two-vacuum-ultraviolet (vuv)- photon ionization using a nonlinear volume autocorrelator unit. The two-vuv-photon process is induced by the intense fifth harmonic radiation of a femtosecond Ti:sapphire laser. In a proof-of-principle experiment, ultrafast dynamics of excited ethylene and oxygen molecules are investigated. Molecular decay times are deduced by comparing the experimental data with the results of a numerical model that accounts for the spatial and temporal characteristics of the harmonic field. The present experiments pave a convenient way for time domain investigations in the vuv-xuv s…
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…
Ultrafast Coherent THz Lattice Dynamics Coupled to Spins in the van der Waals Antiferromagnet FePS3
2022
Coherent THz optical lattice and hybridized phonon–magnon modes are triggered by femtosecond laser pulses in the antiferromagnetic van der Waals semiconductor FePS3. The laser-driven lattice and spin dynamics are investigated in a bulk crystal as well as in a 380 nm-thick exfoliated flake as a function of the excitation photon energy, sample temperature and applied magnetic field. The pump-probe magneto-optical measurements reveal that the amplitude of a coherent phonon mode oscillating at 3.2 THz decreases as the sample is heated up to the Néel temperature. This signal eventually vanishes as the phase transition to the paramagnetic phase occurs, thus revealing its connection to the long-ra…
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…
Ultrafast solvent-assisted level crossing in 1-Naphthol
2013
The nonadiabatic inversion dynamics of the energetic order of the electronic excited states of the photoacid 1-naphthol have been revealed by ultrafast spectroscopy on a femtosecond timescale (see picture; IC=internal conversion). The energetic order of the excited states La and Lb of 1-naphthol is reversed in 60 fs in polar dimethyl sulfoxide solvent.