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Register a new userUltrafast long-range energy transport via light-matter coupling in organic semiconductor films
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The formation of exciton-polaritons allows the transport of energy over hundreds of nanometres at velocities up to 10^6 m s^-1 in organic semiconductors films in the absence of external cavity structures.
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We investigate the effect of hypersonic (> 1 GHz) acoustic phonon wavepackets on electron transport in a semiconductor superlattice. Our quantum mechanical simulations demonstrate that a GHz train of picosecond deformation strain pulses propagating through a superlattice can generate current oscillations whose frequency is several times higher than that of the strain pulse train. The shape and polarity of the calculated current pulses agree well with experimentally measured electric signals. The calculations also explain and accurately reproduce the measured variation of the induced current pulse magnitude with the strain pulse amplitude and applied bias voltage. Our results open a route to developing acoustically-driven semiconductor superlattices as sources of millimetre and sub-millimetre electromagnetic waves.
Ultracold atom magnetic field microscopy enables the probing of current flow patterns in planar structures with unprecedented sensitivity. In polycrystalline metal (gold) films we observe long-range correlations forming organized patterns oriented at +/- 45 deg relative to the mean current flow, even at room temperature and at length scales orders of magnitude larger than the diffusion length or the grain size. The preference to form patterns at these angles is a direct consequence of universal scattering properties at defects. The observed amplitude of the current direction fluctuations scales inversely to that expected from the relative thickness variations, the grain size and the defect concentration, all determined independently by standard methods. This indicates that ultracold atom magnetometry enables new insight into the interplay between disorder and transport.
Energy relaxation in light-harvesting complexes has been extensively studied by various ultrafast spectroscopic techniques, the fastest processes being in the sub-100 fs range. At the same time much slower dynamics have been observed in individual complexes by single-molecule fluorescence spectroscopy (SMS). In this work we employ a pump-probe type SMS technique to observe the ultrafast energy relaxation in single light-harvesting complexes LH2 of purple bacteria. After excitation at 800 nm, the measured relaxation time distribution of multiple complexes has a peak at 95 fs and is asymmetric, with a tail at slower relaxation times. When tuning the excitation wavelength, the distribution changes in both its shape and position. The observed behaviour agrees with what is to be expected from the LH2 excited states structure. As we show by a Redfield theory calculation of the relaxation times, the distribution shape corresponds to the expected effect of Gaussian disorder of the pigment transition energies. By repeatedly measuring few individual complexes for minutes, we find that complexes sample the relaxation time distribution on a timescale of seconds. Furthermore, by comparing the distribution from three long-lived complexes with the whole ensemble, we demonstrate that the ensemble can be considered ergodic. Our findings thus agree with the commonly used notion of an ensemble of identical LH2 complexes experiencing slow random fluctuations.
Near-field radiative heat transfer (RHT) between two bodies can significantly exceed the far-field limit set by Plancks law due to the evanescent wave tunneling, which typically can only occur when the two bodies are separated at subwavelength distances. We show that the RHT between two SiC nanoparticles with separation distances much larger than the thermal wavelength can still exceed the far-field limit when the particles are located within a subwavelength distance away from a SiC substrate. In this configuration, the localized surface phonon polariton (SPhP) of the particles couples to the propagating SPhP of the substrate which then provides a new channel for the near-field energy transport and enhances the RHT by orders of magnitude at large distances. The enhancement is also demonstrated to appear in a chain of closely spaced SiC nanoparticles located in the near field of a SiC substrate. The findings provide a new way for the long-distance transport of near-field energy.
In polymeric semiconductors, charge carriers are polarons, which means that the excess charge deforms the molecular structure of the polymer chain that hosts it. This effect results in distinctive signatures in the vibrational modes of the polymer. We probe polaron photo- generation dynamics at polymer:fullerene heterojunctions by monitoring its time-resolved resonance-Raman spectrum following ultrafast photoexcitation. We conclude that polarons emerge within 200 fs, which is nearly two orders of magnitude faster than exciton localisation in the neat polymer film. Surprisingly, further vibrational evolution on <50-ps timescales is modest, indicating that the polymer conformation hosting nascent polarons is not signif- icantly different from that in equilibrium. This suggests that charges are free from their mutual Coulomb potential, under which vibrational dynamics would report charge-pair relaxation. Our work addresses current debates on the photocarrier generation mechanism at organic semiconductor heterojunctions, and is, to our knowledge, the first direct probe of molecular conformation dynamics during this fundamentally important process in these materials.
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