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. Transition metal nitrides (TMNs, e.g., TiN/HfN) embody the ideal material requirements, where ultrafast electron–phonon coupling prevents fast electronic heat dissipation and low thermal conductivity prolongs the heat confinement. The extreme energy confinement leads to unprecedented peak temperatures and internal heat gradients (>10 K nm−1) that cannot be achieved using noble metals or any current heating method. TMN nanoreactors consequently yield up to ten thousand times more product in pulsed photothermal chemical conversion compared with noble metals (Ag, Au, Cu). These findings open up a completely unexplored realm of nano-photochemistry, where adjacent reaction centers experience substantially different temperatures for hundreds of picoseconds, long enough for bond breaking to occur

A techno-economic perspective on rigid and flexible perovskite solar modules

Perovskite solar cells have shown considerable developments in the last decade, and commercial applications are drawing closer. In this article, we present a techno-economic study of perovskite PV technologies. We compare published data on manufacturing costs of single-junction perovskite modules and find that they are dependent on the module design (rigid or flexible) and vary from 10 to almost 100 € per m2. We calculate the LCOE as a function of module efficiency and stability for a set of four module cost scenarios at 12.5, 25, 50, and 100 € per m2. The resulting LCOE varies from 4.3 to 25.5 ct kW−1 h−1 and shows low potential for immediate competition with crystalline silicon PV in the utility sector. Perovskite PV's competitive advantage lies in both lighter and less rigid modules, and in the development of tandem modules together with silicon. We hence extend the LCOE equation to highlight the benefit of producing flexible low-weight modules by roll-to-roll manufacturing, and modify the LCOE maps to showcase the benefits of tandem modules. Based on learning curve analyses applied to the CAPEX of single-junction and tandem modules, we develop three scenarios for the evolution of the LCOE of perovskite modules from 2025 to 2050. Under the optimistic scenarios, we find that the LCOE could reduce to 2.8 ct kW−1 h−1 by 2050.</p

Ultrafast Photoinduced Heat Generation by Plasmonic HfN Nanoparticles

There is great interest in the development of alternatives to noble metals for plasmonic nanostructures. Transition metal nitrides are promising due to their robust refractory properties. However, the photophysics of these nanostructures, particularly the hot carrier dynamics and photothermal response on ultrafast timescales, are not well understood. This limits their implementation in applications such as photothermal catalysis or solar thermophotovoltaics. In this study, the light-induced relaxation processes in water-dispersed HfN nanoparticles are, for the first time, elucidated by fs transient absorption, Lumerical FDTD and COMSOL Multiphysics simulations, and temperature-dependent ellipsometry. It is unequivocally demonstrated that HfN nanoparticles convert absorbed photons into heat within <100 fs; no signature of hot charge carriers is observed. Interestingly, under high photon energy or intense irradiation stimulated Raman scattering characteristic of oxynitride surface termination is observed. These findings suggest that transition metal nitrides could offer benefits over noble metals in the field of plasmonic photothermal catalysis

Directional quantum dot emission by soft-stamping on silicon Mie resonators

We present a soft-stamping method to selectively print a homogenous layer of CdSeTe/ZnS core–shell quantum dots (QDs) on top of an array of Si nanocylinders with Mie-type resonant modes. Using this new method, we gain accurate control of the quantum dot's angular emission through engineered coupling of the QDs to these resonant modes. Using numerical simulations we show that the emission into or away from the Si substrate can be precisely controlled by the QD position on the nanocylinder. QDs centered on a 400 nm diameter nanocylinder surface show 98% emission directionality into the Si substrate. Alternatively, for homogenous ensembles placed over the nanocylinder top-surface, the upward emission is enhanced 10-fold for 150 nm diameter cylinders. Experimental PL intensity measurements corroborate the simulated trends with cylinder diameter. PL lifetime measurements reflect well the variations of the local density of states at the QD position due to coupling to the resonant cylinders. These results demonstrate that the soft imprint technique provides a unique manner to directly integrate optical emitters with a wide range of nanophotonic geometries, with potential applications in LEDs, luminescent solar concentrators, and up- and down-conversion schemes for improved photovoltaics

BMO spaces associated with semigroups of operators

We study BMO spaces associated with semigroup of operators and apply the results to boundedness of Fourier multipliers. We prove a universal interpolation theorem for BMO spaces and prove the boundedness of a class of Fourier multipliers on noncommutative Lp spaces for all 1 < p < \infty, with optimal constants in p.Comment: Math An

Silicon and Germanium Nanostructures for Photovoltaic Applications: Ab-Initio Results

Actually, most of the electric energy is being produced by fossil fuels and great is the search for viable alternatives. The most appealing and promising technology is photovoltaics. It will become truly mainstream when its cost will be comparable to other energy sources. One way is to significantly enhance device efficiencies, for example by increasing the number of band gaps in multijunction solar cells or by favoring charge separation in the devices. This can be done by using cells based on nanostructured semiconductors. In this paper, we will present ab-initio results of the structural, electronic and optical properties of (1) silicon and germanium nanoparticles embedded in wide band gap materials and (2) mixed silicon-germanium nanowires. We show that theory can help in understanding the microscopic processes important for devices performances. In particular, we calculated for embedded Si and Ge nanoparticles the dependence of the absorption threshold on size and oxidation, the role of crystallinity and, in some cases, the recombination rates, and we demonstrated that in the case of mixed nanowires, those with a clear interface between Si and Ge show not only a reduced quantum confinement effect but display also a natural geometrical separation between electron and hole