Kipras Redeckas

Unveiling the excited state energy transfer pathways in peridinin-chlorophyll a-protein by ultrafast multi-pulse transient absorption spectroscopy

Time-resolved multi-pulse methods were applied to investigate the excited state dynamics, the interstate couplings, and the excited state energy transfer pathways between the light-harvesting pigments in peridinin-chlorophyll a-protein (PCP). The utilized pump-dump-probe techniques are based on perturbation of the regular PCP energy transfer pathway. The PCP complexes were initially excited with an ultrashort pulse, resonant to the S0→S2 transition of the carotenoid peridinin. A portion of the peridinin-based emissive intramolecular charge transfer (ICT) state was then depopulated by applying an ultrashort NIR pulse that perturbed the interaction between S1 and ICT states and the energy flow from the carotenoids to the chlorophylls. The presented data indicate that the peridinin S1 and ICT states are spectrally distinct and coexist in an excited state equilibrium in the PCP complex. Moreover, numeric analysis of the experimental data asserts ICT→Chl-a as the main energy transfer pathway in the photoexcited PCP systems.

Enhanced Nonlinear Optical Response of Resonantly Coupled Silver Nanoparticle–Organic Dye Complexes

The influence of metal nanoparticles on linear and nonlinear optical properties of surrounding organic molecules has been widely investigated, whereas much less attention has been paid to the influence of molecules on properties of nanoparticles. Here, we employ transient absorption spectroscopy to address the nonlinear optical responses of the resonantly coupled silver nanoparticle–organic dye systems and demonstrate that silver nanoparticles covered with dye molecules show enhanced and spectrally different nonlinear extinction changes from pristine nanoparticles. We identify changes of the plasmon resonance band of nanoparticles induced by excitation of surrounding dye. We attribute these exciton–plasmon coupling effects to the excitation-induced refractive index modifications of the dye layer surrounding a nanoparticle and to the back-transfer of the oscillator strength borrowed by the dye from the nanoparticle.

Probing of Carrier Recombination in n- and p-Type 6H-SiC Using Ultrafast Supercontinuum Pulses

Excess carrier dynamics in 6H-SiC substrates with n- and p-type moderate doping were detected using femtosecond pump-probe measurements with supercontinuum probing. Band-to-band recombination and carrier trapping were determined as the main recombination processes in both materials. Spectral fingerprints corresponding to each of these recombination components were obtained using the global and target analysis. It was shown that, in spite of background doping, the band-to-band recombination in 6H-SiC is dominated by the excess electron absorption component and the carrier trapping is dominated by the excess hole absorption.