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

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

Symmetric Rotating Wave Approximation for the Generalized Single-Mode Spin-Boson System

The single-mode spin-boson model exhibits behavior not included in the rotating wave approximation (RWA) in the ultra and deep-strong coupling regimes, where counter-rotating contributions become important. We introduce a symmetric rotating wave approximation that treats rotating and counter-rotating terms equally, preserves the invariances of the Hamiltonian with respect to its parameters, and reproduces several qualitative features of the spin-boson spectrum not present in the original rotating wave approximation both off-resonance and at deep strong coupling. The symmetric rotating wave approximation allows for the treatment of certain ultra and deep-strong coupling regimes with similar accuracy and mathematical simplicity as does the RWA in the weak coupling regime. Additionally, we symmetrize the generalized form of the rotating wave approximation to obtain the same qualitative correspondence with the addition of improved quantitative agreement with the exact numerical results. The method is readily extended to higher accuracy if needed. Finally, we introduce the two-photon parity operator for the two-photon Rabi Hamiltonian and obtain its generalized symmetric rotating wave approximation. The existence of this operator reveals a parity symmetry similar to that in the Rabi Hamiltonian as well as another symmetry that is unique to the two-photon case, providing insight into the mathematical structure of the two-photon spectrum, significantly simplifying the numerics, and revealing some interesting dynamical properties.Comment: 11 pages, 5 figure