Modeling Optical Spectra of Large Organic Systems Using Real-Time Propagation of Semiempirical Effective Hamiltonians
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Abstract not provided.
The primary photoexcited species in excitonic semiconductors is a bound electron–hole pair, or exciton. An important strategy for producing separated electrons and holes in photoexcited excitonic semiconductors is the use of donor/acceptor heterojunctions, but the degree to which the carriers can escape their mutual Coulomb attraction is still debated for many systems. Here, we employ a combined pump–probe ultrafast transient absorption (TA) spectroscopy and time-resolved microwave conductivity (TRMC) study on a suite of model excitonic heterojunctions consisting of mono-chiral semiconducting single-walled carbon nanotube (s-SWCNT) electron donors and small-molecule electron acceptors. Comparison of the charge-separated state dynamics between TA and TRMC photoconductance reveals a quantitative match over the 0.5 microsecond time scale. Charge separation yields derived from TA allow extraction of s-SWCNT hole mobilities of ca. 1.5 cm 2 V -1 s -1 (at 9 GHz) by TRMC. We find that the correlation between the techniques conclusively demonstrates that photoinduced charge carriers separated across these heterojunctions do not form bound charge transfer states, but instead form free/mobile charge carriers.
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The ternary silver halides CH 3 NH 3 AgBr 2 and CH 3 NH 3 Ag 2 I 3 are low-dimensional, wide band gap semiconductors made up of edge-sharing silver halide tetrahedra.
(Ba 1− x Sr x ) 0.98 Eu 0.02 ScO 2 F produces a tunable emission from cyan to green upon Sr 2+ substitution. Ab initio molecular dynamics simulations revealed that Sr 2+ weakens the local rigidity lowering the efficiency and thermal stability of the phosphors.
Pure and Sn doped ZnO nanostructures have been grown on SiO{sub 2}/Si substrates by vapor-solid technique without using any catalysts. It has been found that the morphology of the nanostructures depend strongly on the growth temperature and doping concentration. By proper tuning of the growth temperature, morphology of pure ZnO can be changed from tetrapods to multipods. On the other hand, by varying the doping concentration of Sn in ZnO, the morphology can be tuned from tetrapods to flower-like multipods to nanowires. X-ray diffraction pattern reveals that the nanostructures have a preferred (0002) growth orientation, and they are tensile strained with the increase of Sn doping in ZnO. Temperature-dependent photoluminescence characteristics of these nanostructures have been investigated in the range from 10 to 300 K. Pure ZnO tetrapods exhibited less defect state emissions than that of pure ZnO multipods. The defect emission is reduced with low concentration of Sn doping, but again increases at higher concentration of doping because of increased defects. Transport properties of pure and Sn doped ZnO tetrapods have been studied using complex-plane impedance spectroscopy. The contribution from the arms and junctions of a tetrapod could be distinguished. Sn doped ZnO samples showed lower conductivity but higher relaxation time than that of pure ZnO tetrapods.
A tight binding model is used to investigate photoinduced tunneling current through a molecular bridge coupled to two semiconductor electrodes. A quantum master equation is developed within a non-Markovian theory based on second-order perturbation theory with respect to the molecule-semiconductor electrode coupling. The spectral functions are generated using a one dimensional alternating bond model, and the coupling between the molecule and the electrodes is expressed through a corresponding correlation function. Since the molecular bridge orbitals are inside the bandgap between the conduction and valence bands, charge carrier tunneling is inhibited in the dark. Subject to the dipole interaction with the laser field, virtual molecular states are generated via the absorption and emission of photons, and new tunneling channels open. Interesting phenomena arising from memory are noted. Such a phenomenon could serve as a switch.
High-speed beam choppers are a crucial part of time-resolved x-ray studies as well as a necessary component to enable elemental contrast in synchrotron x-ray scanning tunneling microscopy (SX-STM). However, many chopper systems are not capable of operation in vacuum, which restricts their application to x-ray studies with high photon energies, where air absorption does not present a significant problem. To overcome this limitation, we present a fully ultra-high vacuum (UHV) compatible chopper system capable of operating at variable chopping frequencies up to 4 kHz. The lightweight aluminum chopper disk is coated with Ti and Au films to provide the required beam attenuation for soft and hard x-rays with photon energies up to about 12 keV. The chopper is used for lock-in detection of x-ray enhanced signals in SX-STM.