Search results for "resolve"
showing 10 items of 258 documents
Ultrafast excitation dynamics of low energy pigments in reconstituted peripheral light-harvesting complexes of photosystem I
2000
AbstractUltrafast dynamics of a reconstituted Lhca4 subunit from the peripheral LHCI-730 antenna of photosystem I of higher plants were probed by femtosecond absorption spectroscopy at 77 K. Intramonomeric energy transfer from chlorophyll (Chl) b to Chl a and energy equilibration between Chl a molecules observed on the subpicosecond time scale are largely similar to subpicosecond energy equilibration processes within LHCII monomers. However, a 5 ps equilibration process in Lhca4 involves unique low energy Chls in LHCI absorbing at 705 nm. These pigments localize the excitation both in the Lhca4 subunit and in LHCI-730 heterodimers. An additional 30–50 ps equilibration process involving red …
Defects in quantum ring to control high-harmonic spectrum
2017
AbstractThe high-harmonic generation from a structured quantum ring (SQR) driven by an intense laser field is presented within the single active electron approximation. The spectrum is studied by varying the symmetry of the physical system. The standard SQR (six identical and equidistant dots in a ring) presents a 60° rotational symmetry, that in this work is broken, moving or changing only one potential hole. We find that careful designed breaking of the geometrical symmetry of the SQR opens the possibility of controlling the characteristics of the harmonic lines such as intensity and polarization. HHG analysis of the emission spectrum performed through a Morlet wavelet, shows that the hig…
CHAPTER 12: Real-time and Real-space Time-dependent Density-functional Theory Approach to Attosecond Dynamics
2018
After the advances in strong infrared laser sources and high harmonic generation techniques, the measurement of attosecond dynamics of excited states in molecules has become a reality in many laboratories around the world. The interpretation of these novel ultrafast experiments, aiming at increasingly large molecules, poses considerable theoretical and computational challenges that can be tackled in the framework of time-dependent density functional theory (TDDFT). In this chapter we survey the basics of TDDFT in its real-time and real-space implementation, with particular emphasis on its advantages and limitations in the description of attosecond dynamics. The applicability of this approac…
Simulating pump-probe photo-electron and absorption spectroscopy on the attosecond time-scale with time-dependent density-functional theory
2013
Molecular absorption and photoelectron spectra can be efficiently predicted with real-time time-dependent density functional theory. We show herein how these techniques can be easily extended to study time-resolved pump-probe experiments, in which a system response (absorption or electron emission) to a probe pulse is measured in an excited state. This simulation tool helps with the interpretation of fast-evolving attosecond time-resolved spectroscopic experiments, in which electronic motion must be followed at its natural timescale. We show how the extra degrees of freedom (pump-pulse duration, intensity, frequency, and time delay), which are absent in a conventional steady-state experimen…
Frequency-modulation spectroscopy with blue diode lasers
2000
Frequency-modulation spectroscopy provides ultrasensitive absorption measurements. The technique is especially adaptable to diode lasers, which can be modulated easily, and has been used extensively in the near-infrared and infrared spectral regions. The availability of blue diode lasers now means that the accessible wavelength region can be increased. We successfully demonstrate wavelength-modulation spectroscopy and two-tone frequency-modulation spectroscopy for the weak second resonance line of potassium at 404.8 nm and for the transition at 405.8 nm in lead, starting from the thermally populated 6p(2) P-3(2) metastable level, information on the modulation parameters is obtained with a f…
Generalized Browder’s Theorem and SVEP
2007
A bounded operator \(T \in L(X), X\) a Banach space, is said to verify generalized Browder’s theorem if the set of all spectral points that do not belong to the B-Weyl’s spectrum coincides with the set of all poles of the resolvent of T, while T is said to verify generalized Weyl’s theorem if the set of all spectral points that do not belong to the B-Weyl spectrum coincides with the set of all isolated points of the spectrum which are eigenvalues. In this article we characterize the bounded linear operators T satisfying generalized Browder’s theorem, or generalized Weyl’s theorem, by means of localized SVEP, as well as by means of the quasi-nilpotent part H0(λI − T) as λ belongs to certain …
Valence electronic structure of C60: Theoretical analysis of photoemission data
1993
Abstract We present a theoretical investigation of the valence band photoemission spectra of C 60 using the nonempirical valence effective Hamiltonian (VEH) method. The VEH-DOVS curves calculated for the C 60 molecule are found to be in excellent agreement with synchrotron-radiation photoemission spectra reported for C 60 films. A detailed interpretation of all the photoemission bands is performed in the light of the VEH results.
Valence-band electronic structure of CdO, ZnO, and MgO from x-ray photoemission spectroscopy and quasi-particle-corrected density-functional theory c…
2009
The valence-band density of states of single-crystalline rock-salt CdO(001), wurtzite $c$-plane ZnO, and rock- salt MgO(001) are investigated by high-resolution x-ray photoemission spectroscopy. A classic two-peak structure is observed in the VB-DOS due to the anion $2p$-dominated valence bands. Good agreement is found between the experimental results and quasi-particle-corrected density-functional theory calculations. Occupied shallow semicore $d$ levels are observed in CdO and ZnO. While these exhibit similar spectral features to the calculations, they occur at slightly higher binding energies, determined as 8.8 eV and 7.3 eV below the valence band maximum in CdO and ZnO, respectively. Th…
Collinear laser spectroscopy of ZrII
2003
A new technique involving collinear laser spectroscopy of ion bunches has been used to study the radio-isotopes 87,87m,88,89,89m Zr.
Towards Iron(II) Complexes with Octahedral Geometry: Synthesis, Structure and Photophysical Properties
2020
The control of ligand-field splitting in iron (II) complexes is critical to slow down the metal-to-ligand charge transfer (MLCT)-excited states deactivation pathways. The gap between the metal-centered states is maximal when the coordination sphere of the complex approaches an ideal octahedral geometry. Two new iron(II) complexes (C1 and C2), prepared from pyridylNHC and pyridylquinoline type ligands, respectively, have a near-perfect octahedral coordination of the metal. The photophysics of the complexes have been further investigated by means of ultrafast spectroscopy and TD-DFT modeling. For C1, it is shown that&mdash