Molecular hot spots in surface-enhanced Raman scattering

The chemical and electromagnetic (EM) enhancements both contribute to surface-enhanced Raman scattering (SERS). It is well-known that the EM enhancement is induced by the intense local field of surface plasmon resonance (SPR). This report shows that the polarizability of the molecules adsorbed on the metal surface can lead to another channel for the EM field enhancement. When aromatic molecules are covalently bonded to the Au surface, they strongly interact with the plasmon, leading to a modification of the absorption spectrum and a strong SERS signal. The effect is seen in both 3 nm-Au nanoparticles with a weak SPR and 15 nm-Au nanoparticles with a strong SPR, suggesting that the coupling is through both EM field and chemical means. Linear-chain molecules on the 3 nm-Au nanoparticles do not have a SERS signal. However, when the aromatic and linear molecules are co-adsorbed, the strong SPR/molecular polarizability interaction spatially extends the local EM field, leading to a strong SERS signal from the linear-chain molecules. The results show that aromatic molecules immobilized on Au can create “hot spots” just like plasmonic nanostructures

Algebraic expressions for the polarisation response of spin-VCSELs

Closed-form expressions are derived for the relationship between the polarisation of the output and that of the pump for spin-polarised vertical-cavity surface-emitting lasers. These expressions are based on the spin-flip model (SFM) combined with the condition that the carrier recombination time is much greater than both the spin relaxation time and the photon lifetime. Allowance is also included for misalignment between the principal axes of birefringence and dichroism. These expressions yield results that are in excellent agreement both with previously published numerical calculations and with further tests for a wide range of parameters. Trends with key parameters of the SFM are easily deduced from these expression

Stability Boundaries in Laterally-Coupled Pairs of Semiconductor Lasers

The dynamic behaviour of coupled pairs of semiconductor lasers is studied using normal-mode theory, applied to one-dimensional (slab) and two-dimensional (circular cylindrical) real index confined structures. It is shown that regions of stable behaviour depend not only on pumping rate and laser separation, but also on the degree of guidance in the structures. Comparison of results between normal-mode and coupled-mode theories for these structures leads to the tentative conclusion that the accuracy of the latter is determined by the strength of self-overlap and cross-overlap of the symmetric and antisymmetric normal modes in the two lasers

Stability Analysis of Quantum-Dot Spin-VCSELs

Spin-polarized vertical-cavity surface-emitting lasers (spin-VCSELs) and vertical external-cavity surface-emitting lasers (spin-VECSELs) are of interest since their output polarization can be manipulated by spin-selective pumping, either optical or electrical. These devices, using quantum dot (QD) material for the active region, have shown instability (periodic oscillations) and polarization switching in previous theoretical simulations based on a rate equation model. It has been recognized that the polarization switching occurs between two possible sets of solutions, termed here in-phase and out-of-phase. The present contribution seeks to give enhanced understanding of these behaviors by applying a stability analysis to the system of equations used for such simulations. The results indicate that the choice of in-phase and out-of-phase solutions that appear in a time-dependent simulation is determined by the condition that the corresponding steady-state solutions are stable against small perturbations. The stability analysis is shown to be a valuable theoretical tool for future study of spin-V(E)SELs in the context of understanding and guiding future experimental research

Mapping bifurcation structure and parameter dependence in quantum dot spin-VCSELs

We consider a modified version of the spin-flip model (SFM) that describes optically pumped quantum dot (QD) spin-polarized vertical-cavity surface-emitting lasers (VCSELs). Maps showing different dynamical regions and those consisting of various key bifurcations are constructed by direct numerical simulations and a numerical path continuation technique, respectively. A comparison between them clarifies the physical mechanism that governs the underlying dynamics as well as routes to chaos in QD spin-VCSELs. Detailed numerical simulations illustrate the role played by the capture rate from wetting layer (WL) to QD ground state, the gain parameter, and the amplitude-phase coupling. By tuning the aforementioned key parameters in turn we show how the dynamical regions evolve as a function of the intensity and polarization of the optical pump, as well as in the plane of the spin relaxation rate and linear birefringence rate, which is of importance in the design of spin lasers promising potential applications. By increasing the capture rate from WL to QD our simulation accurately describes the transition from the QD spin-VCSEL to the quantum well case, in agreement with a previous mathematical derivation, and thus validates the modified SFM equations

Plasmon-induced photonic and energy-transfer enhancement of solar water splitting by a hematite nanorod arra

Plasmonic metal nanostructures offer a promising route to improve the solar energy conversion efficiency of semiconductors. Here we show that incorporation of a hematite nanorod array into a plasmonic gold nanohole array pattern significantly improves the photoelectrochemical water splitting performance, leading to an approximately tenfold increase in the photocurrent at a bias of 0.23 V versus Ag|AgCl under simulated solar radiation. Plasmon-induced resonant energy transfer is responsible for enhancement at the energies below the band edge, whereas above the absorption band edge of hematite, the surface plasmon polariton launches a guided wave mode inside the nanorods, with the nanorods acting as miniature optic fibres, enhancing the light absorption. In addition, the intense local plasmonic field can suppress the charge recombination in the hematite nanorod photoanode in a photoelectrochemical cell. Our results may provide a general approach to overcome the low optical absorption and spectral utilization of thin semiconductor nanostructures, while further reducing charge recombination losses

Plasmon-Induced Photonic And Energy-Transfer Enhancement Of Solar Water Splitting By A Hematite Nanorod Array

Plasmonic metal nanostructures offer a promising route to improve the solar energy conversion efficiency of semiconductors. Here we show that incorporation of a hematite nanorod array into a plasmonic gold nanohole array pattern significantly improves the photoelectrochemical water splitting performance, leading to an approximately tenfold increase in the photocurrent at a bias of 0.23 V versus Ag|AgCl under simulated solar radiation. Plasmon-induced resonant energy transfer is responsible for enhancement at the energies below the band edge, whereas above the absorption band edge of hematite, the surface plasmon polariton launches a guided wave mode inside the nanorods, with the nanorods acting as miniature optic fibres, enhancing the light absorption. In addition, the intense local plasmonic field can suppress the charge recombination in the hematite nanorod photoanode in a photoelectrochemical cell. Our results may provide a general approach to overcome the low optical absorption and spectral utilization of thin semiconductor nanostructures, while further reducing charge recombination losses