Broadband Absorption and Efficient Hot-Carrier Photovoltaic Conversion based on Sunlight-induced Non-radiative Decay of Propagating Surface Plasmon Polaritons

Localized surface plasmon polaritons (SPPs), which can decay non-radiatively into hot carriers, have been widely employed to extend the responses of traditional semiconductor-based photocatalytic and photovoltaic devices to sub-bandgap photons. However, radiative decay is unavoidable and adverse to device performances. Here, we propose to take advantage of propagating SPPs, another form of SPPs, which possess non-radiative decay only. A special gold-titanium dioxide nanowire array with each nanowire capped with a nanocone is proposed. The adjacent nanocones forming top gradual openings attribute to efficient sunlight harvesting, while the neighbouring nanowires forming bottom nanoslots allow sufficient absorption due to the propagating SPPs. With the combined advantages, almost 100% of light is absorbed by a very thin gold film in the visible range, and 73% in the whole considered range of 400–1170 nm, superior to the nanocone cell based on localized SPPs, let alone the nanowire-based and planar counterparts. Therefore, much better photovoltaic conversion performance is achieved with short-circuit current density of 0.74 mA/cm(2) and open-circuit voltage of 0.41 V. This work confirms the superiority of non-radiative decay of propagating SPPs to the localized SPPs in terms of generation of hot carriers, providing a promising way of extracting electrons in metal into photocurrent.