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Charge Transfer States (charge + transfer_states)
Selected AbstractsObservation of a Charge Transfer State in Low-Bandgap Polymer/Fullerene Blend Systems by Photoluminescence and Electroluminescence StudiesADVANCED FUNCTIONAL MATERIALS, Issue 20 2009Yi Zhou Abstract The presence of charge transfer states generated by the interaction between the fullerene acceptor PCBM and two alternating copolymers of fluorene with donor,acceptor,donor comonomers are reported; the generation leads to modifications in the polymer bandgap and electronic structure. In one of polymer/fullerene blends, the driving force for photocurrent generation, i.e., the gap between the lowest unoccupied molecular orbitals of the donor and acceptor, is only 0.1,eV, but photocurrent is generated. It is shown that the presence of a charge transfer state is more important than the driving force. The charge transfer states are visible through new emission peaks in the photoluminescence spectra and through electroluminescence at a forward bias. The photoluminescence can be quenched under reverse bias, and can be directly correlated to the mechanism of photocurrent generation. The excited charge transfer state is easily dissociated into free charge carriers, and is an important intermediate state through which free charge carriers are generated. [source] Exploiting a Dual-Fluorescence Process in Fluorene,Dibenzothiophene- S,S -dioxideCo-Polymers to Give Efficient Single Polymer LEDs with Broadened EmissionADVANCED FUNCTIONAL MATERIALS, Issue 4 2009Simon M. King Abstract A description of the synthesis of random (9,9-dioctylfluorene-2,7-diyl),(dibenzothiophene- S,S -dioxide-3,7-diyl) co-polymers (p(F-S)x) by palladium-catalyzed Suzuki cross-coupling polymerization where the feed ratio of the latter is varied from 2 to 30,mol % (i.e., x,=,2,30) is given. Polymer light emitting devices are fabricated with the configuration indium tin oxide/poly(3,4-ethylenedioxythiophene):poly(styrenesulfonic acid)/p(F,S)x/Ba/Al. The device external quantum efficiency increased as the ratio of the S co-monomer was increased, up to a maximum of 1.3% at 100,mA cm,2 for p(F-S)30 and a brightness of 3 770,cd m,2 (at 10,V). The S units impart improved electron injection, more balanced mobilities, and markedly improved device performance compared to poly(9,9-dioctylfluorene) under similar conditions. These co-polymers display broad emission, observed as greenish-white light, which arises from dual fluorescence, viz. both local excited states and charge transfer states. Utilizing dual emission can reduce problems associated with Förster energy transfer from high-energy to-low energy excited states. [source] The electronically excited states of RDX (hexahydro-1,3,5-trinitro-1,3,5-triazine): Vertical excitationsINTERNATIONAL JOURNAL OF QUANTUM CHEMISTRY, Issue 11 2009Itamar Borges Jr Abstract The RDX molecule, hexahydro-1,3,5-trinitro-1,3,5-triazine, is a key component for several energetic materials, which have important practical applications as explosives. A systematic study of the electronic excited states of RDX in gas phase using time-dependent density functional theory (TDDFT), algebraic diagrammatic construction through second order method [ADC (2)], and resolution of the identity coupled-cluster singles and doubles method (RI-CC2) was carried out. Transition energies and optical oscillator strengths were computed for a maximum of 40 transitions. RI-CC2 and ADC (2) predict a spectrum shaped by three intense ,-,* transitions, two with charge transfer and one with localized character. TDDFT fails in the description of the charge transfer states. The low-energy band of the experimental UV spectrum of RDX is assigned to the first charge transfer state. Two alternative assignments of the high-energy band are proposed. © 2009 Wiley Periodicals, Inc. Int J Quantum Chem, 2009 [source] Theoretical investigation of charge transfer excitation and charge recombination in acenaphthylene,tetracyanoethylene complexINTERNATIONAL JOURNAL OF QUANTUM CHEMISTRY, Issue 1 2003Hai-Bo Yi Abstract Ab initio calculations were performed to investigate the charge separation and charge recombination processes in the photoinduced electron transfer reaction between tetracyanoethylene and acenaphthylene. The excited states of the charge-balanced electron donor,acceptor complex and the singlet state of ion pair complex were studied by employing configuration interaction singles method. The equilibrium geometry of electron donor,acceptor complex was obtained by the second-order Mřller,Plesset method, with the interaction energy corrected by the counterpoise method. The theoretical study of ground state and excited states of electron donor,acceptor complex in this work reveals that the S1 and S2 states of the electron donor,acceptor complexes are excited charge transfer states, and charge transfer absorptions that corresponds to the S0 , S1 and S0 , S2 transitions arise from ,,,* excitations. The charge recombination in the ion pair complex will produce the charge-balanced ground state or excited triplet state. According to the generalized Mulliken,Hush model, the electron coupling matrix elements of the charge separation process and the charge recombination process were obtained. Based on the continuum model, charge transfer absorption and charge transfer emission in the polar solvent of 1,2-dichloroethane were investigated. © 2003 Wiley Periodicals, Inc. Int J Quantum Chem 94: 23,35, 2003 [source] Excited-state molecular structures captured by X-ray transient absorption spectroscopy: a decade and beyondACTA CRYSTALLOGRAPHICA SECTION A, Issue 2 2010Lin X. Chen Transient molecular structures along chemical reaction pathways are important for predicting molecular reactivity, understanding reaction mechanisms, as well as controlling reaction pathways. During the past decade, X-ray transient absorption spectroscopy (XTA, or LITR-XAS, laser-initiated X-ray absorption spectroscopy), analogous to the commonly used optical transient absorption spectroscopy, has been developed. XTA uses a laser pulse to trigger a fundamental chemical process, and an X-ray pulse(s) to probe transient structures as a function of the time delay between the pump and probe pulses. Using X-ray pulses with high photon flux from synchrotron sources, transient electronic and molecular structures of metal complexes have been studied in disordered media from homogeneous solutions to heterogeneous solution,solid interfaces. Several examples from the studies at the Advanced Photon Source in Argonne National Laboratory are summarized, including excited-state metalloporphyrins, metal-to-ligand charge transfer (MLCT) states of transition metal complexes, and charge transfer states of metal complexes at the interface with semiconductor nanoparticles. Recent developments of the method are briefly described followed by a future prospective of XTA. It is envisioned that concurrent developments in X-ray free-electron lasers and synchrotron X-ray facilities as well as other table-top laser-driven femtosecond X-ray sources will make many breakthroughs and realise dreams of visualizing molecular movies and snapshots, which ultimately enable chemical reaction pathways to be controlled. [source] | ||||||||||