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Future generations of photoelectrodes for solar fuel generation must employ inexpensive, earth-abundant absorber materials in order to provide a large-scale source of clean energy. These materials tend to have poor electrical transport properties and exhibit carrier diffusion lengths which are significantly shorter than the absorption depth of light. As a result, many photo-excited carriers are generated too far from a reactive surface, and recombine instead of participating in solar-to-fuel-conversion. We demonstrate that plasmonic resonances in metallic nanostructures and multi-layer interference effects can be engineered to strongly concentrate sunlight close to the electrode/liquid interface, precisely where the relevant reactions take place. By comparing spectral features in the enhanced photocurrent spectra to full-field electromagnetic simulations, the contribution of surface plasmon excitations is verified. These results open the door to the optimization of a wide variety of photochemical processes by leveraging the rapid advances in the field of plasmonics.
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Optical control of electronic spins is the basis for ultrafast spintronics: circularly polarized light in combination with spin-orbit coupling of the electronic states allows for spin manipulation in condensed matter. However, the conventional approach is limited to spin orientation along one particular orientation that is dictated by the direction of photon propagation. Plasmonics opens new capabilities, allowing one to tailor the light polarization at the nanoscale. Here, we demonstrate ultrafast optical excitation of electron spin on femtosecond time scales via plasmon to exciton spin conversion. By time-resolving the THz spin dynamics in a hybrid (Cd,Mn)Te quantum well structure covered with a metallic grating, we unambiguously determine the orientation of the photoexcited electron spins which is locked to the propagation direction of surface plasmon-polaritons. Using the spin of the incident photons as additional degree of freedom, one can orient the photoexcited electron spin at will in a two-dimensional plane.
Implementation of an optically active material on silicon has been a persistent technological challenge. For tandem photovoltaics using a Si bottom cell, as well as for other optoelectronic applications, there has been a longstanding need for optically active, wide band gap materials that can be integrated with Si. ZnSiP$_2$ is a stable, wide band gap (2.1 eV) material that is lattice matched with silicon and comprised of inexpensive elements. As we show in this paper, it is also a defect-tolerant material. Here, we report the first ZnSiP$_2$ photovoltaic device. We show that ZnSiP$_2$ has excellent photoresponse and high open circuit voltage of 1.3 V, as measured in a photoelectrochemical configuration. The high voltage and low band gap-voltage offset are on par with much more mature wide band gap III-V materials. Photoluminescence data combined with theoretical defect calculations illuminate the defect physics underlying this high voltage, showing that the intrinsic defects in ZnSiP$_2$ are shallow and the minority carrier lifetime is 7 ns. These favorable results encourage the development of ZnSiP$_2$ and related materials as photovoltaic absorber materials.
We present a model for exciton-plasmon coupling based on an energy exchange mechanism between quantum emitters (QE) and localized surface plasmons in metal-dielectric structures. Plasmonic correlations between QEs give rise to a collective state exchanging its energy cooperatively with a resonant plasmon mode. By defining carefully the plasmon mode volume for a QE ensemble, we obtain a relation between QE-plasmon coupling and a cooperative energy transfer rate that is expressed in terms of local fields. For a single QE near a sharp metal tip, we find analytically the enhancement factor for QE-plasmon coupling relative to QE coupling to a cavity mode. For QEs distributed in an extended region enclosing a plasmonic structure, we find that the ensemble QE-plasmon coupling saturates to a universal value independent of system size and shape, consistent with the experiment.
The great potential of Dirac electrons for plasmonics and photonics has been readily recognized after their discovery in graphene, followed by applications to smart optical devices. Dirac carriers are also found in topological insulators (TI) --quantum systems having an insulating gap in the bulk and intrinsic Dirac metallic states at the surface--. Here, we investigate the plasmonic response of ring structures patterned in Bi$_2$Se$_3$ TI films, which we investigate through terahertz (THz) spectroscopy. The rings are observed to exhibit a bonding and an antibonding plasmon modes, which we tune in frequency by varying their diameter. We develop an analytical theory based on the THz conductivity of unpatterned films, which accurately describes the strong plasmon-phonon hybridization and Fano interference experimentally observed as the bonding plasmon is swiped across the promineng 2,THz phonon exhibited by this material. This work opens the road for the investigation of plasmons in topological insulators and for their application in tunable THz devices.
We investigate exemplary the longitudinal optical (LO) mode order in compounds with a plasmon or plasmon-like phonon mode and additional phonon modes. When the oscillator strength of the plasmon or plasmon-like mode is gradually increased, a reordering of the modes takes place. Since it is not possible in crystals with orthorhombic or higher symmetry that a LO mode crosses a transverse optical (TO) modes position, this reordering takes place via mode hybridization. During this mode hybridization, the plasmon or plasmon-like LO mode gradually becomes the originally higher situated LO mode while the latter morphs into the former. As a consequence, an inner (LO-TO) and an outer (TO-LO) mode pair is formed. This process continues until the LO oscillator strength is so high that all other phonons are inverted and form LO-TO pairs within the outer TO-LO mode pair of the plasmon or plasmon-like mode. These insights can be readily transferred to other semiconductors or many mode materials with reststrahlen bands and allow simple mode assignments. These mode assignments will help to understand the nature of surface modes of structured layers of these materials for application of surface plasmon polariton and surface phonon polaritons based metamaterials.
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