Photonic Excitation of a Micromechanical Cantilever in Electrostatic Fields.

We present a specific near-field configuration where an electrostatic force gradient is found to strongly enhance the optomechanical driving of an atomic force microscope cantilever sensor. It is shown that incident photons generate a photothermal effect that couples with electrostatic fields even at tip-surface separations as large as several wavelengths, dominating the cantilever dynamics. The effect is the result of resonant phenomena where the photothermal-induced parametric driving acts conjointly (or against, depending on electric field direction) with a photovoltage generation in the cantilever. The results are achieved experimentally in an atomic force microscope operating in vacuum and explained theoretically through numerical simulations of the equation of motion of the cantilever. Intrinsic electrostatic effects arising from the electronic work-function difference of tip and surface are also highlighted. The findings are readily relevant for other optomicromechanical systems where electrostatic force gradients can be implemented.

Electronic energy and electron transfer processes in photoexcited donor-acceptor dyad and triad molecular systems based on triphenylene and perylene diimide units.

We investigate the photophysical properties of organic donor-acceptor dyad and triad molecular systems based on triphenylene and perylene diimide units linked by a non-conjugated flexible bridge in solution using complementary optical spectroscopy techniques. When these molecules are diluted in dichloromethane solution, energy transfer from the triphenylene to the perylene diimide excited moieties is evidenced by time-resolved fluorescence measurements resulting in a quenching of the emission from the triphenylene moieties. Simultaneously, another quenching process that affects the emission from both donor and acceptor units is observed. Solution ultrafast transient absorption measurements provide evidence of photo-induced charge transfer from either the donor or the acceptor depending upon the excitation. Overall, the analysis of the detailed time-resolved spectroscopic measurements carried out in the dyad and triad systems as well as in the triphenylene and perylene diimide units alone provides useful information both to better understand the relations between energy and charge transfer processes with molecular structures, and for the design of future functional dyad and triad architectures based on donor and acceptor moieties for organic optoelectronic applications.

Photophysical, amplified spontaneous emission and charge transport properties of oligofluorene derivatives in thin films.

We investigate the photophysical and amplified spontaneous emission properties of a series of monodisperse solution-processable oligofluorenes functionalized with hexyl chains at the C9 position of each fluorene unit. Thin films of these oligofluorenes are then used in organic field-effect transistors and their charge transport properties are examined. We have particularly focused our attention on the influence of oligofluorene length on the absorption and steady-state fluorescence spectra, on the HOMO/LUMO energy levels, on the photoluminescence lifetime and quantum yield as well as on the amplified spontaneous emission properties and the charge carrier mobilities. Differential scanning calorimetry and X-ray diffraction measurements demonstrate that, among all oligofluorene derivatives used in this study, only the structure and morphology of the pentafluorene film is significantly modified by a thermal treatment above the glass transition temperature, resulting in a 9 nm blue-shift of the fluorescence spectrum without significant changes in the photoluminescence quantum yield and in the amplified spontaneous emission threshold. In parallel, hole field-effect mobility is significantly increased from 8.6 × 10(-7) to 3.8 × 10(-5) cm(2) V(-1) s(-1) upon thermal treatment, due to an increase of crystallinity. This study provides useful insights into the morphological control of oligofluorene thin films and how it affects their photophysical and charge transport properties. Moreover, we provide evidence that, because of the low threshold, the tunability of the amplified spontaneous emission and the photostability of the films, these oligofluorenes are promising candidates for organic solid-state laser applications.

Photovoltaic and photothermal effects induced by visible laser radiation in atomic force microscopy probes.

Excitation of electrons into higher energy states in solid state materials can be induced by absorption of visible light, a physical process generally studied by optical absorption spectroscopy. A promising approach for improving the spatial resolution of optical absorption spectroscopy beyond the diffraction limit is the detection of photoinduced forces by an atomic force microscope operating under wavelength-dependent light irradiation. Here, we report on a combined photovoltaic/photothermal effect induced by the absorption of visible light by the microscope probes. By monitoring the photoinduced modifications of the oscillation of the probes, it is found that the oscillation phase-voltage parabolic signals display specific fingerprints which depend on light intensity and the nature of the materials composing the probes. In particular, a localized surface photovoltage (SPV) is evidenced at the tip apex of uncoated Si probes, while none is observed on Au-coated Si probes. The photothermal effects are distinguished from photovoltaic effects by specific shifts of the phase-voltage parabolas. The findings are relevant for the whole range of atomic force microscopy techniques making use of visible light as an additional means of local optical characterization.