Search results for "EXCITATION"
showing 10 items of 1290 documents
Light-induced nonthermal population of optical phonons in nanocrystals
2017
Raman spectroscopy is widely used to study bulk and nanomaterials, where information is frequently obtained from spectral line positions and intensities. In this study, we monitored the Raman spectrum of ensembles of semiconductor nanocrystals (NCs) as a function of optical excitation intensity (optical excitation experiments). We observe that in NCs the red-shift of the Raman peak position with increasing light power density is much steeper than that recorded for the corresponding bulk material. The increase in optical excitation intensity results also in an increasingly higher temperature of the NCs as obtained with Raman thermometry through the commonly used Stokes/anti-Stokes intensity …
A QM/MM Approach Using the AMOEBA Polarizable Embedding: From Ground State Energies to Electronic Excitations
2016
International audience; A fully polarizable implementation of the hybrid Quantum Mechanics/Molecular Mechanics approach is presented, where the classical environment is described through the AMOEBA polarizable force field. A variational formalism, offering a self-consistent 1 relaxation of both the MM induced dipoles and the QM electronic density is used for ground state energies and extended to electronic excitations in the framework of Time-Dependent Density Functional Theory combined with a state specific response of the classical part. An application to the calculation of the solvatochromism of the pyridinium N-phenolate betaine dye used to define the solvent ET30 scale is presented. Th…
Dynamic Polarizability and Higher-Order Electric Properties of Fluorene, Carbazole, and Dibenzofuran
2019
Static electric properties, from the dipole moment to the second-hyperpolarizability tensor γ, of the 3-membered, isoelectronic ring molecules, fluorene (FL), carbazole (CR), and dibenzofuran (DBF), have been calculated at various levels of approximation. The electron correlation effects have been included at the coupled-cluster (CC) level, using CCSD and CC2 versions of the method. DFT calculations with the CAM-B3LYP functional have also been performed, and the results are compared to the CC values. The electric property-tailored Pol basis set and its more compact Z3Pol version have been employed in all static calculations. Differences between dipole polarizability values computed at the P…
Effect of molecular Stokes shift on polariton dynamics
2021
When the enhanced electromagnetic field of a confined light mode interacts with photoactive molecules, the system can be driven into the regime of strong coupling, where new hybrid light-matter states, polaritons, are formed. Polaritons, manifested by the Rabi split in the dispersion, have shown potential for controlling the chemistry of the coupled molecules. Here, we show by angle-resolved steady-state experiments accompanied by multi-scale molecular dynamics simulations that the molecular Stokes shift plays a significant role in the relaxation of polaritons formed by organic molecules embedded in a polymer matrix within metallic Fabry-Pérot cavities. Our results suggest that in the case …
The first example of cofacial bis(dipyrrins)
2016
International audience; Two series of cofacial bis(dipyrrins) were prepared and their photophysical properties as well as their bimolecular fluorescence quenching with C-60 were investigated. DFT and TDDFT computations were also performed as a modeling tool to address the nature of the fluorescence state and the possible inter-chromophore interactions. Clearly, there is no evidence for such interactions and the bimolecular quenching of fluorescence, in comparison with mono-dipyrrins, indicates that C-60-bis(dipyrrin) contacts occur from the outside of the "mouth" of the cofacial structure.
High-resolution rovibrational spectroscopy of c-C3H2+: The ν7 C–H antisymmetric stretching band
2020
Abstract The ν 7 antisymmetric C–H stretching fundamental of c- C 3 H 2 + has been characterized in a cryogenic 22-pole ion trap by a novel type of action spectroscopy, in which the rovibrational excitation of c- C 3 H 2 + is detected as a slowing down of the low-temperature reaction c- C 3 H 2 + + H2 → C 3 H 3 + + H. Ninety-one rovibrational transitions with partly resolved fine structure doublets were measured in high resolution. Supported by high-level quantum chemical calculations, spectroscopic parameters were determined by fitting the observed lines with an effective Hamiltonian for an asymmetric rotor in a doublet electronic ground state, X ˜ A 1 2 , yielding a band origin at 3113.6…
Bowl-shape electron donors with absorptions in the visible range of the solar spectrum and their supramolecular assemblies with C 60
2012
We describe the synthesis, electronic, optical and photophysical properties of a family of three electron-donor bowl-shaped organic molecules that absorb light in the whole range of the visible spectrum (up to 800 nm in one case), and associate C60 in solution with binding constants in the range of 104–102 M−1 as measured from both UV-vis and fluorescence titrations in several solvents. These molecules are π-extended derivatives of tetrathiafulvalene, based on a truxene core to which two or three units of dithiole are covalently attached. The inclusion of the bulky dithiole groups is responsible for their bowl-shape geometry, which allows them to associate with C60, and their electron-donor…
Functional rearrangement of the light-harvesting antenna upon state transitions in a green alga
2014
AbstractState transitions in the green alga Chlamydomonas reinhardtii serve to balance excitation energy transfer to photosystem I (PSI) and to photosystem II (PSII) and possibly play a role as a photoprotective mechanism. Thus, light-harvesting complex II (LHCII) can switch between the photosystems consequently transferring more excitation energy to PSII (state 1) or to PSI (state 2) or can end up in LHCII-only domains. In this study, low-temperature (77 K) steady-state and time-resolved fluorescence measured on intact cells of Chlamydomonas reinhardtii shows that independently of the state excitation energy transfer from LHCII to PSI or to PSII occurs on two main timescales of <15 ps and …
Modeling of an active torsion bar automotive suspension for ride comfort and energy analysis in standard road profiles
2019
Abstract Chassis technology is evolving towards active suspension, in which actuators can provide forces to each wheel individually. This overcomes the traditional trade-off between comfort and handling, at the expense of increased complexity and electric consumption. To reduce power demand, regenerative solutions capable of harvesting a certain amount of energy otherwise dissipated in vehicle suspensions and to enhance vehicle dynamics for improving ride comfort and road safety at the same time have been researched. In this paper, an active suspension based on a torsion bar is modeled and analyzed under the excitation from standardized road profiles according to the ISO 8608 norm. A skyhoo…
Use of second-order sliding mode observer for low-accuracy sensing in hydraulic machines
2018
Low-accuracy sensing is very common for the large hydraulic machines and does not allow for directly measuring the relative velocity which can be, otherwise, required for the control and monitoring purposes. This paper provides a case study of designing the second-order sliding mode observer based on the super-twisting robust exact differentiator. The nominal part of the system dynamics is derived from the simple available system measurements and incorporated into the observer structure. Parasitic by-effects, arising from the sensor sampling, quantization, and non-modeled distortions due to mechanical sensor interface, are shown as the main causes of hampering the final (steady-state) conve…