Polaritonic Chemistry Enabled by Non-Local Metasurfaces.

Vibrational strong coupling can modify chemical reaction pathways in unconventional ways. Thus far, Fabry-Perot cavities formed by pairs of facing mirrors have been mostly utilized to achieve vibrational strong coupling. In this study, we demonstrate the application of non-local metasurfaces that can sustain surface lattice resonances, enabling chemical reactions under vibrational strong coupling.

Disentangling Hot Carrier Decay and the Nature of Low- to High- Transfer Processes in Quasi-Two-Dimensional Layered Perovskites.

Quasi-two-dimensional (2D) metal halide perovskites (MHPs) are promising photovoltaic (PV) materials because of their impressive optical and optoelectronic properties and improved stability compared to their 3D counterparts. The presence of domains with varying numbers of inorganic layers between the organic spacers (-phases), each with different bandgaps, makes the photoinduced carrier dynamics in films of these materials complex and intriguing. Existing interpretations of the ultrafast femto- or picosecond spectroscopy data have been inconsistent, most of them focusing either on exciton/charge transfer from low- to high- phases or on hot carrier cooling, but not combined.

Nanoscale Thermometry of Plasmonic Structures via Raman Shifts in Copper Phthalocyanine.

Temperature measurements at the nanoscale are vital for the application of plasmonic structures in medical photothermal therapy and materials science but very challenging to realize in practice. In this work, we exploit a combination of surface-enhanced Raman spectroscopy together with the characteristic temperature dependence of the Raman peak maxima observed in β-phase copper phthalocyanine (β-CuPc) to measure the surface temperature of plasmonic gold nanoparticles under laser irradiation. We begin by measuring the temperature-dependent Raman shifts of the three most prominent modes of β-CuPc films coated on an array of Au nanodisks over a temperature range of 100-500 K.

Pulsed Photothermal Heterogeneous Catalysis.

Anthropogenic climate change urgently calls for the greening and intensification of the chemical industry. Most chemical reactors make use of catalysts to increase their conversion yields, but their operation at steady-state temperatures limits their rate, selectivity, and energy efficiency. Here, we show how to break such a steady-state paradigm using ultrashort light pulses and photothermal nanoparticle arrays to modulate the temperature of catalytic sites at timescales typical of chemical processes.

Ultrafast Thermal Imprinting of Plasmonic Hotspots.

Plasmonic photochemistry is driven by a rich collection of near-field, hot charge carrier, energy transfer, and thermal effects, most often accomplished by continuous wave illumination. Heat generation is usually considered undesirable, because noble metal nanoparticles heat up isotropically, losing the extreme energy confinement of the optical resonance. Here it is demonstrated through optical and heat-transfer modelling that the judicious choice of nanoreactor geometry and material enables the direct thermal imprint of plasmonic optical absorption hotspots onto the lattice with high fidelity.