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Register a new userEvidence for Excimer Photoexcitations in an Ordered {pi}-Conjugated Polymer Film
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We report pressure-dependent transient picosecond and continuous-wave photomodulation studies of disordered and ordered films of 2-methoxy-5-(2-ethylhexyloxy) poly(para-phenylenevinylene). Photoinduced absorption (PA) bands in the disordered film exhibit very weak pressure dependence and are assigned to intrachain excitons and polarons. In contrast, the ordered film exhibits two additional transient PA bands in the midinfrared that blueshift dramatically with pressure. Based on high-order configuration interaction calculations we ascribe the PA bands in the ordered film to excimers. Our work brings insight to the exciton binding energy in ordered films versus disordered films and solutions. The reduced exciton binding energy in ordered films is due to new energy states appearing below the continuum band threshold of the single strand.
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Inter- or intramolecular coupling processes between chromophores such as excimer formation or H- and J-aggregation are crucial to describing the photophysics of closely packed films of conjugated polymers. Such coupling is highly distance dependent, and should be sensitive to both fluctuations in the spacing between chromophores as well as the actual position on the chromophore where the exciton localizes. Single-molecule spectroscopy reveals these intrinsic fluctuations in well-defined bi-chromophoric model systems of cofacial oligomers. Signatures of interchromophoric interactions in the excited state - spectral red-shifting and broadening, and a slowing of photoluminescence decay - correlate with each other but scatter strongly between single molecules, implying an extraordinary distribution in coupling strengths. Furthermore, these excimer-like spectral fingerprints vary with time, revealing intrinsic dynamics in the coupling strength within one single dimer molecule, which constitutes the starting point for describing a molecular solid. Such spectral sensitivity to sub-Angstrom molecular dynamics could prove complementary to conventional FRET-based molecular rulers.
Following the recent discovery of large magnetoresistance at room temperature in polyfluorence sandwich devices, we have performed a comprehensive magnetoresistance study on a set of organic semiconductor sandwich devices made from different pi-conjugated polymers and small molecules. The measurements were performed at different temperatures, ranging from 10K to 300K, and at magnetic fields, $B < 100mT$. We observed large negative or positive magnetoresistance (up to 10% at 300K and 10mT) depending on material and device operating conditions. We compare the results obtained in devices made from different materials with the goal of providing a comprehensive picture of the experimental data. We discuss our results in the framework of known magnetoresistance mechanisms and find that none of the existing models can explain our results.
Electric fields are central to the operation of optoelectronic devices based on conjugated polymers since they drive the recombination of electrons and holes to excitons in organic light-emitting diodes but are also responsible for the dissociation of excitons in solar cells. One way to track the microscopic effect of electric fields on charge carriers formed under illumination of a polymer film is to exploit the fluorescence arising from delayed recombination of carrier pairs, a process which is fundamentally spin dependent. Such spin-dependent recombination can be probed directly in fluorescence, by optically detected magnetic resonance (ODMR). Depending on the relative orientation, an electric field may either dissociate or stabilize an electron-hole carrier pair. We find that the ODMR signal in a polymer film is quenched in an electric field, but that, at fields exceeding 1 MV/cm, this quenching saturates. This finding contrasts the complete ODMR suppression that was previously observed in polymeric photodiodes, indicating that exciton-charge interactions---analogous to Auger recombination in crystalline semiconductors---may constitute the dominant carrier-pair dissociation process in organic electronics.
We present results of x-ray study of spatial properties of $pi-pi$ conjugated networks in polymer thin films. We applied the x-ray cross-correlation analysis to x-ray scattering data from blends of poly(3-hexylthiophene) (P3HT) and gold nanoparticles. The Fourier spectra of the intensity cross-correlation functions for different films contain non-zero components of orders $n=2,4$ and $6$ measuring the degree of structural order in the system.
We utilize terahertz time domain spectroscopy to investigate thin films of the heavy fermion compound SmB6, a prototype Kondo insulator. Temperature dependent terahertz (THz) conductivity measurements reveal a rapid decrease in the Drude weight and carrier scattering rate at ~T*=20 K, well below the hybridization gap onset temperature (100 K). Moreover, a low-temperature conductivity plateau (below 20K) indicates the emergence of a surface state with an effective electron mass of 0.1me. Conductivity dynamics following optical excitation are also measured and interpreted using Rothwarf-Taylor (R-T) phenomenology, yielding a hybridization gap energy of 17 meV. However, R-T modeling of the conductivity dynamics reveals a deviation from the expected thermally excited quasiparticle density at temperatures below 20K, indicative of another channel opening up in the low energy electrodynamics. Taken together, these results suggest the onset of a surface state well below the crossover temperature (100K) after long-range coherence of the f-electron Kondo lattice is established.
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