Conformational Control of Exciton-Polariton Physics in Metal - Poly(9,9-dioctylfluorene) - Metal Cavities

Control is exerted over the exciton-polariton physics in metal - Poly(9,9-dioctyl fluorene) - metal microcavities via conformational changes to the polymer backbone. Using thin-film samples containing increasing fractions of $\beta$-phase chain segments, a systematic study is reported for the mode characteristics and resulting light emission properties of cavities containing two distinct exciton sub-populations within the same semiconductor. Ultrastrong coupling for disordered glassy-phase excitons is observed from angle-resolved reflectivity measurements, with Rabi splitting energies in excess of 1.05 eV (more than 30% of the exciton transition energy) for both TE- and TM-polarized light. A splitting of the lower polariton branch is then induced via introduction of $\beta$-phase excitons and increases with their growing fraction. In all cases, the photoluminescence emanates from the lowermost polariton branch, allowing conformational control to be exerted over the emission energy and its angular variation. Dispersion-free cavities with highly saturated blue-violet emission are thus enabled. Experimental results are discussed in terms of the full Hopfield Hamiltonian generalized to the case of two exciton oscillators. The importance of taking account of the molecular characteristics of the semiconductor for an accurate description of its strong coupling behaviour is directly considered, in specific relation to the role of the vibronic structure

Retrieval of interatomic separations of molecules from laser-induced high-order harmonic spectra

We illustrate an iterative method for retrieving the internuclear separations of N$_2$, O$_2$ and CO$_2$ molecules using the high-order harmonics generated from these molecules by intense infrared laser pulses. We show that accurate results can be retrieved with a small set of harmonics and with one or few alignment angles of the molecules. For linear molecules the internuclear separations can also be retrieved from harmonics generated using isotropically distributed molecules. By extracting the transition dipole moment from the high-order harmonic spectra, we further demonstrated that it is preferable to retrieve the interatomic separation iteratively by fitting the extracted dipole moment. Our results show that time-resolved chemical imaging of molecules using infrared laser pulses with femtosecond temporal resolutions is possible.Comment: 14 pages, 9 figure

Theoretical analysis of dynamic chemical imaging with lasers using high-order harmonic generation

We report theoretical investigations of the tomographic procedure suggested by Itatani {\it et al.} [Nature, {\bf 432} 867 (2004)] for reconstructing highest occupied molecular orbitals (HOMO) using high-order harmonic generation (HHG). Using the limited range of harmonics from the plateau region, we found that under the most favorable assumptions, it is still very difficult to obtain accurate HOMO wavefunction, but the symmetry of the HOMO and the internuclear separation between the atoms can be accurately extracted, especially when lasers of longer wavelengths are used to generate the HHG. We also considered the possible removal or relaxation of the approximations used in the tomographic method in actual applications. We suggest that for chemical imaging, in the future it is better to use an iterative method to locate the positions of atoms in the molecule such that the resulting HHG best fits the macroscopic HHG data, rather than by the tomographic method.Comment: 13 pages, 14 figure

A mathematical formalization of the parallel replica dynamics

The purpose of this article is to lay the mathematical foundations of a well known numerical approach in computational statistical physics and molecular dynamics, namely the parallel replica dynamics introduced by A.F. Voter. The aim of the approach is to efficiently generate a coarse-grained evolution (in terms of state-to-state dynamics) of a given stochastic process. The approach formally consists in concurrently considering several realizations of the stochastic process, and tracking among the realizations that which, the soonest, undergoes an important transition. Using specific properties of the dynamics generated, a computational speed-up is obtained. In the best cases, this speed-up approaches the number of realizations considered. By drawing connections with the theory of Markov processes and, in particular, exploiting the notion of quasi-stationary distribution, we provide a mathematical setting appropriate for assessing theoretically the performance of the approach, and possibly improving it

Effects of burying and removing dead leaves from the ground on the development of scab epidemics in an apple organic orchard.

Ascospores produced on scabbed leaves in the leaf litter constitute the primary inoculum causing scab infections in apple orchards during the year. The trial, carried out in a commercial organic orchard, permitted to evaluate the effects of the removal of dead leaves located on the inter-row supplemented by the ploughing in of the leaves left on the row, on the development of scab epidemics. From the first recorded contamination to harvest time, lesions on leaves and fruits were counted to determine reduction in disease incidence and severity, compared with the untreated plots. Disease severity as a function of the distance from the untreated plot was also observed, to evaluate the spore dispersal gradient within the orchard. The results show that the ploughing in and the removal of the litter reduced disease incidence by 62% on leaves, and by almost 82% on fruits to harvest. Moreover, measurements of the dispersal gradient show that the spores do not disperse, or little, beyond 20m of the untreated zone