Ultrafast Thermal Modification of Strong Coupling in an Organic Microcavity

There is growing interest in using strongly coupled organic microcavities to tune molecular dynamics, including the electronic and vibrational properties of molecules. However, very little attention has been paid to the utility of cavity polaritons as sensors for out-of-equilibrium phenomena, including thermal excitations. Here, we demonstrate that non-resonant infrared excitation of an organic microcavity system induces a transient response in the visible spectral range near the cavity polariton resonances. We show how these optical response can be understood in terms of ultrafast heating of electrons in the metal cavity mirror, which modifies the effective refractive index and subsequently the strong coupling conditions. The temporal dynamics of the microcavity are strictly determined by carriers in the metal, including the cooling of electrons via electron-phonon coupling and excitation of propagating coherent acoustic modes in the lattice. We rule out multiphoton excitation processes and verify that no real polariton population exists despite their strong transient features. These results suggest the promise of cavity polaritons as sensitive probes of non-equilibrium phenomena

An XMM-Newton Observation of the Local Bubble Using a Shadowing Filament in the Southern Galactic Hemisphere

We present an analysis of the X-ray spectrum of the Local Bubble, obtained by simultaneously analyzing spectra from two XMM-Newton pointings on and off an absorbing filament in the Southern galactic hemisphere (b ~ -45 deg). We use the difference in the Galactic column density in these two directions to deduce the contributions of the unabsorbed foreground emission due to the Local Bubble, and the absorbed emission from the Galactic halo and the extragalactic background. We find the Local Bubble emission is consistent with emission from a plasma in collisional ionization equilibrium with a temperature $\log T_{LB} = 6.06^{+0.02}_{-0.04}$ and an emission measure of 0.018 cm^{-6} pc. Our measured temperature is in good agreement with values obtained from ROSAT All-Sky Survey data, but is lower than that measured by other recent XMM-Newton observations of the Local Bubble, which find $\log T_{LB} \approx 6.2$ (although for some of these observations it is possible that the foreground emission is contaminated by non-Local Bubble emission from Loop I). The higher temperature observed towards other directions is inconsistent with our data, when combined with a FUSE measurement of the Galactic halo O VI intensity. This therefore suggests that the Local Bubble is thermally anisotropic. Our data are unable to rule out a non-equilibrium model in which the plasma is underionized. However, an overionized recombining plasma model, while observationally acceptable for certain densities and temperatures, generally gives an implausibly young age for the Local Bubble (\la 6 \times 10^5 yr).Comment: Accepted for publication in the Astrophysical Journal. 16 pages, 9 figure

Maximum Entropy Reconstruction of the Interstellar Medium: I. Theory

We have developed a technique to map the three-dimensional structure of the local interstellar medium using a maximum entropy reconstruction technique. A set of column densities N to stars of known distance can in principle be used to recover a three-dimensional density field n, since the two quantities are related by simple geometry through the equation N = C n, where C is a matrix characterizing the stellar spatial distribution. In practice, however, there is an infinte number of solutions to this equation. We use a maximum entropy reconstruction algorithm to find the density field containing the least information which is consistent with the observations. The solution obtained with this technique is, in some sense, the model containing the minimum structure. We apply the algorithm to several simulated data sets to demonstrate its feasibility and success at recovering ``real'' density contrasts. This technique can be applied to any set of column densities whose end points are specified. In a subsequent paper we shall describe the application of this method to a set of stellar color excesses to derive a map of the dust distribution, and to soft X-ray absorption columns to hot stars to derive a map of the total density of the interstellar medium.Comment: 23 pages, 7 fig.; accepted for publication in the Ap.

Discovery of Reflection Nebulosity Around Five Vega-like Stars

Coronagraphic optical observations of six Vega-like stars reveal reflection nebulosities, five of which were previously unknown. The nebulosities illuminated by HD 4881, HD 23362, HD 23680, HD 26676, and HD 49662 resemble that of the Pleiades, indicating an interstellar origin for dust grains. The reflection nebulosity around HD 123160 has a double-arm morphology, but no disk-like feature is seen as close as 2.5 arcsec from the star in K-band adaptive optics data. We demonstrate that uniform density dust clouds surrounding HD 23362, HD 23680 and HD 123160 can account for the observed 12-100 micron spectral energy distributions. For HD 4881, HD 26676, and HD 49662 an additional emission source, such as from a circumstellar disk or non-equilibrium grain heating, is required to fit the 12-25 micron data. These results indicate that in some cases, particularly for Vega-like stars located beyond the Local Bubble (>100 pc), the dust responsible for excess thermal emission may originate from the interstellar medium rather than from a planetary debris system.Comment: The Astrophysical Journal, in press for March, 2002 (32 pages, 13 figures

Rayleigh Imaging of Graphene and Graphene Layers

We investigate graphene and graphene layers on different substrates by monochromatic and white-light confocal Rayleigh scattering microscopy. The image contrast depends sensitively on the dielectric properties of the sample as well as the substrate geometry and can be described quantitatively using the complex refractive index of bulk graphite. For few layers (<6) the monochromatic contrast increases linearly with thickness: the samples behave as a superposition of single sheets which act as independent two dimensional electron gases. Thus, Rayleigh imaging is a general, simple and quick tool to identify graphene layers, that is readily combined with Raman scattering, which provides structural identification.Comment: 8 pages, 9 figure

Ultrafast supercontinuum spectroscopy of carrier multiplication and biexcitonic effects in excited states of PbS quantum dots

We examine the multiple exciton population dynamics in PbS quantum dots by ultrafast spectrally-resolved supercontinuum transient absorption (SC-TA). We simultaneously probe the first three excitonic transitions over a broad spectral range. Transient spectra show the presence of first order bleach of absorption for the 1S_h-1S_e transition and second order bleach along with photoinduced absorption band for 1P_h-1P_e transition. We also report evidence of the one-photon forbidden 1S_{h,e}-1P_{h,e} transition. We examine signatures of carrier multiplication (multiexcitons for the single absorbed photon) from analysis of the first and second order bleaches, in the limit of low absorbed photon numbers (~ 10^-2), at pump energies from two to four times the semiconductor band gap. The multiexciton generation efficiency is discussed both in terms of a broadband global fit and the ratio between early- to long-time transient absorption signals.. Analysis of population dynamics shows that the bleach peak due to the biexciton population is red-shifted respect the single exciton one, indicating a positive binding energy.Comment: 16 pages, 5 figure

Singlet fission in a hexacene dimer: energetics dictate dynamics

Singlet fission (SF) is an exciton multiplication process with the potential to raise the efficiency limit of single junction solar cells from 33% to up to 45%. Most chromophores generally undergo SF as solid-state crystals. However, when such molecules are covalently coupled, the dimers can be used as model systems to study fundamental photophysical dynamics where a singlet exciton splits into two triplet excitons within individual molecules. Here we report the synthesis and photophysical characterization of singlet fission of a hexacene dimer. Comparing the hexacene dimer to analogous tetracene and pentacene dimers reveals that excess exoergicity slows down singlet fission, similar to what is observed in molecular crystals. Conversely, the lower triplet energy of hexacene results in an increase in the rate of triplet pair recombination, following the energy gap law for radiationless transitions. These results point to design rules for singlet fission chromophores: the energy gap between singlet and triplet pair should be minimal, and the gap between triplet pair and ground state should be large

Distribution and Kinematics of O VI in the Galactic Halo

FUSE spectra of 100 extragalactic objects are analyzed to obtain measures of O VI absorption along paths through the Milky Way thick disk/halo. Strong O VI absorption over the approximate velocity range from -100 to 100 km/s reveals a widespread but highly irregular distribution of thick disk O VI, implying the existence of substantial amounts of hot gas with T ~ 3x10^5 K in the Milky Way halo. Large irregularities in the distribution of the absorbing gas are found to be similar over angular scales extending from less than one to 180 degrees, indicating a considerable amount of small and large scale structure in the gas. The overall distribution of Galactic O VI is not well described by a symmetrical plane-parallel layer of patchy O VI absorption. The simplest departure from such a model that provides a reasonable fit to the observations is a plane-parallel patchy absorbing layer with a scale height of 2.3 kpc, and a 0.25 dex excess of O VI in the northern Galactic polar region. The O VI absorption has a Doppler parameter b = 30 to 99 km/s, with an average value of 60 km/s . Thermal broadening alone cannot explain the large observed profile widths. The average O VI absorption velocities toward high latitude objects range from -46 to 82 km/s, with a sample average of 0 km/s and a standard deviation of 21 km/s. O VI associated with the thick disk moves both toward and away from the plane with roughly equal frequency. A combination of models involving the radiative cooling of hot fountain gas, the cooling of supernova bubbles in the halo, and the turbulent mixing of warm and hot halo gases is required to explain the presence of O VI and other highly ionized atoms found in the halo. (abbreviated)Comment: 70 pages, single-spaced, PDF format. Bound copies of this manuscript and two accompanying articles are available upon request. Submitted to ApJ