Publications by authors named "Philippe Klemm"

At low temperatures and high magnetic fields, electron and hole spins in an organic light-emitting diode become polarized so that recombination preferentially forms molecular triplet excited-state species. For low device currents, magnetoelectroluminescence perfectly follows Boltzmann activation, implying a virtually complete polarization outcome. As the current increases, the magnetoelectroluminescence effect is reduced because spin polarization is suppressed by the reduction in carrier residence time within the device.

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Gold nanoparticles emit broad-band upconverted luminescence upon irradiation with pulsed infrared laser radiation. Although the phenomenon is widely observed, considerable disagreement still exists concerning the underlying physics, most notably over the applicability of concepts such as multiphoton absorption, inelastic scattering, and interband vs intraband electronic transitions. Here, we study single particles and small clusters of particles by employing a spectrally resolved power-law analysis of the irradiation-dependent emission as a sensitive probe of these physical models.

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Metal-free dual singlet-triplet organic light-emitting diode (OLED) emitters can provide direct insight into spin statistics, spin correlations and spin relaxation phenomena, through a comparison of fluorescence to phosphorescence intensity. Remarkably, such materials can also function at room temperature, exhibiting phosphorescence lifetimes of several milliseconds. Using electroluminescence, quantum chemistry, and electron paramagnetic resonance spectroscopy, we investigate the effect of the conjugation pathway on radiative and nonradiative relaxation of the triplet state in phenazine-based compounds and demonstrate that the contribution of the phenazine nπ* excited state is crucial to enabling phosphorescence.

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Disordered noble-metal nanoparticle films exhibit highly localized and stable nonlinear light emission from subdiffraction regions upon illumination by near-infrared femtosecond pulses. Such hot spot emission spans a continuum in the visible and near-infrared spectral range. Strong plasmonic enhancement of light-matter interaction and the resulting complexity of experimental observations have prevented the development of a universal understanding of the origin of light emission.

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Nonlinear continuum generation from diffraction-limited hot spots in rough silver films exhibits striking narrow-band intensity resonances in excitation wavelength. Time-domain Fourier spectroscopy uncovers how these resonances arise due to the formation of a "plasmon staircase", a discreteness in the fundamental oscillation of the plasmon excitations responsible for generating the white-light continuum. Whereas multiple scattering from discrete antennas can be invoked to explain hot spot formation in random assemblies of isolated particles, hot spots in films of fused nanoparticles are excited by interfering propagating surface plasmons, launched by scattering from individual nanoparticle antennas.

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