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- Alonso, Benjamin, et al.
(författare)
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Characterization of sub-two-cycle pulses from a hollow-core fiber compressor in the spatiotemporal and spatiospectral domains
- 2013
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Ingår i: Applied Physics B. - : Springer Science and Business Media LLC. - 0946-2171 .- 1432-0649. ; 112:1, s. 105-114
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Tidskriftsartikel (refereegranskat)abstract
- We have post-compressed 25 fs (Fourier limit) amplified pulses in an argon-filled hollow-core fiber. The output pulses were compressed using a pair of wedges and chirped mirrors down to 4.5 fs (Fourier limit of 4.1 fs), which corresponds to less than two optical cycles. We then performed the characterization of the pulses by combining the d-scan and the STARFISH techniques. The temporal (and spectral) measurement of the pulses is done with d-scan, which is used as the reference to extend the characterization to the spatiotemporal (and spatiospectral) amplitude and phase of the pulses by means of STARFISH. The post-compressed pulses at the output of the hollow-fiber had an energy of 150 mu J. The analysis of the pulses revealed larger spectral broadening and blue-shift, and shorter duration at the center of the beam. For the first time, we demonstrate the complete characterization of intense ultra-broadband pulses in the sub-two-cycle regime, which provides an improved insight into the properties (space-time and space-frequency) of the pulses and is highly relevant for their applications.
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| 2. |
- Dahlstrand, Christian
(författare)
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Ground and Excited State Aromaticity : Design Tools for π-Conjugated Functional Molecules and Materials
- 2012
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- The main focus of this thesis is on the aromaticity of the ground state and electronically excited states of π-conjugated molecules and polymers, as well as how aromaticity is connected to their properties.The electronic structures of polybenzenoid hydrocarbons (PBHs) were explored through density functional theory (DFT) calculations and the π-component of the electron localization function (ELFπ). The study revealed how the π-electronic structure is influenced by the fusion of double bonds or benzene rings to the PBHs. We also demonstrated that the π-electrons of benzene extend to accommodate as much aromaticity as possible when bond length distorted. The aromatic chameleon property displayed by fulvenes, isobenzofulvenes, fulvalenes, bis(fulvene)s, and polyfulvenes were investigated using DFT calculations. The tria-, penta-, and heptafulvenes were shown to possess ionization energies and electron affinities which can be tuned extensively by substitution, some of which even outperform TTF and TCNQ, the prototypical electron donor and acceptor, respectively. The singlet-triplet energy gap of pentafulvenes can be tuned extensively by substitution to the point that the triplet state is lower than the singlet state and thus becomes the ground state. The ELFπ of isobenzofulvene shows that the benzene ring in an electronically excited state can be more aromatic than the corresponding ring in the ground state. We have shown that the 6-ring of [5.6.7]quinarene is influenced by a Hückel aromatic resonance structure with 4n+2 π-electrons in the excited quintet state. The bis(fulvene)s which are composed of a donor type heptafulvene and an acceptor type pentafulvene, retain the basic donor-acceptor properties of the two fragments and could function as compact donor-acceptor dyads. A few of the designed polyfulvenes were found to have band gaps below 1 eV at the PBC-B3LYP/6-31G(d) level.Various 2,7-disubstituted fluorenones and dibenzofulvenes were synthesized and their excited state properties were investigated by absorption spectroscopy and time-dependent DFT calculations. It was found that the 1A → 1B transition of ππ* character can be tuned by substitution in the 2,7-positions. The 2,7-bis(N,N-dimethyl) derivatives of fluorenone and dibenzofulvene displayed low energy transitions at 2.18 and 1.61 eV, respectively, in toluene.
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