Oriented thin films of a benzodithiophene covalent organic framework.

A mesoporous electron-donor covalent organic framework based on a benzodithiophene core, BDT-COF, was obtained through condensation of a benzodithiophene-containing diboronic acid and hexahydroxytriphenylene (HHTP). BDT-COF is a highly porous, crystalline, and thermally stable material, which can be handled in air. Highly porous, crystalline oriented thin BDT-COF films were synthesized from solution on different polycrystalline surfaces, indicating the generality of the synthetic strategy.

Charge photogeneration in donor-acceptor conjugated materials: influence of excess excitation energy and chain length.

We investigate the role of excess excitation energy on the nature of photoexcitations in donor-acceptor π-conjugated materials. We compare the polymer poly(2,6-(4,4-bis(2-ethylhexyl)-4H-cyclopenta[1,2-b;3,4-b']dithiophene)-4,7-benzo[2,1,3]thiadiazole) (PCPDTBT) and a short oligomer with identical constituents at different excitation wavelengths, from the near-infrared up to the ultraviolet spectral region. Ultrafast spectroscopic measurements clearly show an increased polaron pair yield for higher excess energies directly after photoexcitation when compared to the exciton population.

Spectral signatures of polarons in conjugated co-polymers.

We study electronic and optical properties of the low-bandgap co-polymer PCPDT-BT (poly-cyclopentadithiophene-co-benzothiadiazole) and compare it with the corresponding homo-polymer PCPDT (poly-cyclopentadithiophene). We investigate the linear absorptivity in these systems for neutral molecules and for their singly charged ions based on quantum-chemical calculations and experiments. One of our main findings is that the ions of the homo-polymer show a polaron absorption that is symmetric between anion and cation, whereas for polaron excitations in the co-polymer this symmetry is strongly lifted.

Structural correlations in the generation of polaron pairs in low-bandgap polymers for photovoltaics.

Polymeric semiconductors are materials where unique optical and electronic properties often originate from a tailored chemical structure. This allows for synthesizing conjugated macromolecules with ad hoc functionalities for organic electronics. In photovoltaics, donor-acceptor co-polymers, with moieties of different electron affinity alternating on the chain, have attracted considerable interest.

Reduced charge transfer exciton recombination in organic semiconductor heterojunctions by molecular doping.

We investigate the effect of molecular doping on the recombination of electrons and holes localized at conjugated-polymer-fullerene interfaces. We demonstrate that a low concentration of p-type dopant molecules (<4% weight) reduces the interfacial recombination via charge transfer excitons and results in a favored formation of separated carriers. This is observed by the ultrafast quenching of photoluminescence from charge transfer excitons and the increase in photoinduced polaron density by ~70%.

Dispersion control with reflection grisms of an ultra-broadband spectrum approaching a full octave.

We report the design, implementation, and characterization of a grism-pair stretcher in a near-infrared noncollinear optical parametric chirped-pulse amplifier (OPCPA) that is capable of controlling a bandwidth of 440 nm. Our dynamic dispersion control scheme relies on the grism stretcher working in conjunction with an acousto-optic programmable dispersive filter (Dazzler) to jointly compensate large amount of material dispersion. A spectral interference technique is used to characterize the spectral phase of the grism stretcher.

Investigation of two-beam-pumped noncollinear optical parametric chirped-pulse amplification for the generation of few-cycle light pulses.

We demonstrate a new and compact Phi-plane-pumped noncollinear optical parametric chirped-pulse amplification (NOPCPA) scheme for broadband pulse amplification, which is based on two-beam-pumping (TBP) at 532 nm. We employ type-I phase-matching in a 5 mm long BBO crystal with moderate pump intensities to preserve the temporal pulse contrast. Amplification and compression of the signal pulse from 675 nm - 970 nm is demonstrated, which results in the generation of 7.

Generation of sub-three-cycle, 16 TW light pulses by using noncollinear optical parametric chirped-pulse amplification.

We present a two-stage noncollinear optical parametric chirped-pulse amplification system that generates 7.9 fs pulses containing 130 mJ of energy at an 805 nm central wavelength and 10 Hz repetition rate. These 16 TW light pulses are compressed to within 5% of their Fourier limit and are carefully characterized by the use of home-built pulse diagnostics.