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Coupling between dynamical heterogeneity of ionic liquids and their structural periodicity on different length-scales can be directly probed by quasielastic neutron scattering with polarization analysis. The technique provides the tools to investigate single-particle and cooperative ion motions separately and, thus, dynamics of ion associations affecting the net charge transport can be experimentally explored. The focus of this study is the structure-dynamic relationship in the protic ionic liquid, triethylammonium triflate, characterized by strong hydrogen bonds between cations and anions. The site-selective deuterium/hydrogen-isotope substitution was applied to modulate the relative contributions of different atom groups to the total coherent and incoherent scattering signal. This approach in combination with molecular dynamics simulations allowed us to obtain a sophisticated description of cation self-diffusion and confined ion pair dynamics from the incoherent spectral component by using the acidic proton as a tagged particle. The coherent contribution of the neutron spectra demonstrated substantial ion association leading to collective ion migration that preserves charge alteration on picosecond time scale, as well as correlation of the localized dynamics occurring between adjacent ions.

The optomechanical character of molecules was discovered by Raman about one century ago. Today, molecules are promising contenders for high-performance quantum optomechanical platforms because their small size and large energy-level separations make them intrinsically robust against thermal agitations. Moreover, the precision and throughput of chemical synthesis can ensure a viable route to quantum technological applications. The challenge, however, is that the coupling of molecular vibrations to environmental phonons limits their coherence to picosecond time scales. Here, we improve the optomechanical quality of a molecule by several orders of magnitude through phononic engineering of its surrounding. By dressing a molecule with long-lived high-frequency phonon modes of its nanoscopic environment, we achieve storage and retrieval of photons at millisecond time scales and allow for the emergence of single-photon strong coupling in optomechanics. Our strategy can be extended to the realization of molecular optomechanical networks.

Absorption spectroscopy is known to be a powerful tool to gain spatially and temporally resolved information on excited and reactive species in a plasma discharge. Furthermore, the interaction of the discharge with short intense laser pulses can trigger the ignition and the transition into other transient states of the plasma. In this context laser-assisted ‘pump-probe’ experiments involving simultaneously generated supercontinuum radiation yield highly temporally resolved and spatially well-defined information on the transient phenomena. In this paper we demonstrate the possibility for ‘pump–probe’ experiments by initiating breakdown on a picosecond time scale (‘pump’) with a high-power beam and measuring the broadband absorption with the simultaneously provided supercontinuum (‘probe’). Since both pulses are generated from the same mode-locked master oscillator, they have a strong level of synchronization.

The nonlinear optical properties of silver-nanoparticle-decorated functionalized (hydrogen-induced reduction, exfoliated) multilayered graphene (AgNP/fG) composite have been investigated in the picosecond time scale by using the Z-scan technique. Drastic changes in the Z-scan profiles are obtained in AgNP/fG at 1064 nm as the profile flips from the behavior of strong saturable absorption (SA) to reverse saturable absorption (RSA) on increasing the incident intensity. On the other hand, in graphene, the effect of weaker SA is observed at low intensities, but it flips to RSA at higher incident intensities. The strong SA in the case of the composite has been attributed to the electronic interaction between graphene and silver nanoparticles. The metallic plasmonic transition has a contribution to the optical nonlinearity in AgNP/fG at 532 nm. � 2012 Optical Society of America.

We have applied time-resolved THz spectroscopy to probe the transient photoexcited carrier dynamics and THz conductivity in Si nanocrystal films with varying silicon volume filling fractions and nanocrystal sizes on picosecond time scales. The THz conductivity reveals microscopic carrier motion with significant interface scattering within nanocrystals as well as percolative transport between nanocrystals. The time variation of the THz conductivity is analyzed within the framework of the Drude-Smith model, an extension of the Drude model that characterizes carrier localization in nanostructured materials. Below the percolation threshold, transport between nanocrystals is inhibited and photoexcited carriers are localized within individual nanocrystals. These films also exhibit efficient optical emission. In films with Si filling fractions above the percolation threshold, photoluminescence is suppressed and a transition from long-range inter-nanocrystal transport immediately after photoexcitation to increased carrier localization over a 50 ps time scale due to accumulation of charges at interface defect sites is observed., 2nd International Symposium on Nanoscale Luminescent Materials - 221st ECS Meeting, May 6-10, 2012, Seattle, WA, USA, Series: ECS Transactions

Nonlinear optical properties of a standard dye IR26 have been studied by using the Z-scan technique to decipher the difference in the mechanism of nonlinear absorption on picosecond time scale at two wavelengths i.e. at 1064 nm and 532 nm. A prominent contribution of nonlinear absorption is observed in the Z-scan profiles at 1064 nm. The dye exhibits the mechanism of self-defocusing at 1064 nm in contrast to that of self-focusing at 532 nm. While the two photon absorption has been found to be the dominant mechanism of reverse saturable absorption at 1064 nm, the mechanism of excited state absorption is operating at 532 nm. Additionally, the optical phase conjugate geometry of degenerate four wave mixing (DFWM) technique has been used to measure the third order nonlinear susceptibility values at 532 nm to compare with those obtained from the Z-scan profiles. � 2010 Elsevier B.V.