A Method of Developing Analytical Multipartite Delocalization Measures for Mixed W-like States

We present a method of developing analytical measures of $k$-partite delocalization in arbitrary $n$-body W-like states, otherwise known as mixed states in the single excitation subspace. These measures calculate the distance of a state to its closest reference state with $k-1$ entanglement. We find that the reference state is determined by the purity of the state undergoing measurement. Measures with up to 6-body delocalization for a 6-body system are derived in full, while an algorithm for general $k$-partite measures is given.Comment: 8 pages, 3 figure

Resonance Energy Transfer

Resonance energy transfer, also known as Förster- or fluorescence- resonance energy transfer, or electronic energy transfer, is a photonic process whose relevance in many major areas of science is reflected both by a wide prevalence of the effect and through numerous technical applications. The process, operating through an optical near-field mechanism, effects a transport of electronic excitation between physically distinct atomic or molecular components, based on transition dipole-dipole coupling. In this chapter a comprehensive survey of the process is presented, beginning with an outline of the history and highlighting the early contributions of Perrin and Förster. A review of the photophysics behind resonance energy transfer follows, and then a discussion of some prominent applications of resonance energy transfer. Particular emphasis is given to analysis and sensing techniques used in molecular biology, ranging from the ‘spectroscopic ruler’ measurements of functional group separation, to fluorescence lifetime microscopy. The chapter ends with a description of the role of energy transfer in photosynthetic light harvesting

Quantum-coherence and correlations in π-conjugated molecules and multichromophoric systems

AbstractChemistry is intrinsically founded on quantum mechanical principles and examples of quantum-mechanical phenomena abound on a range of energy and length scales. In this article some examples of quantum-mechanical phenomena that can be probed by optical spectroscopy are discussed. Recent experimental studies of quantumcoherence in electronic energy transfer in π-conjugated polymers are reported as examples of weak correlations. The nature of the electron-hole binding energy for excitons in organic systems is investigated as a case of intermediate correlations. Possible experimental probes of strong correlations involved in chemical reactions are critically examined in the final section of the paper

Thermal light cannot be represented as a statistical mixture of single pulses

We ask whether or not thermal light can be represented as a mixture of single broadband coherent pulses. We find that it cannot. Such a mixture is simply not rich enough to mimic thermal light; indeed, it cannot even reproduce the first-order correlation function. We show that it is possible to construct a modified mixture of single coherent pulses that does yield the correct first-order correlation function at equal space points. However, as we then demonstrate, such a mixture cannot reproduce the second-order correlation function.Comment: 5 pages, 2 figures. Published versio

Anisotropic conjugated polymer chain conformation tailors the energy migration in nanofibers

Conjugated polymers are complex multi-chromophore systems, with emission properties strongly dependent on the electronic energy transfer through active sub-units. Although the packing of the conjugated chains in the solid state is known to be a key factor to tailor the electronic energy transfer and the resulting optical properties, most of the current solution-based processing methods do not allow for effectively controlling the molecular order, thus making the full unveiling of energy transfer mechanisms very complex. Here we report on conjugated polymer fibers with tailored internal molecular order, leading to a significant enhancement of the emission quantum yield. Steady state and femtosecond time-resolved polarized spectroscopies evidence that excitation is directed toward those chromophores oriented along the fiber axis, on a typical timescale of picoseconds. These aligned and more extended chromophores, resulting from the high stretching rate and electric field applied during the fiber spinning process, lead to improved emission properties. Conjugated polymer fibers are relevant to develop optoelectronic plastic devices with enhanced and anisotropic properties.Comment: 43 pages, 15 figures, 1 table in Journal of the American Chemical Society, (2016