Broadband cavity-enhanced ultrafast spectroscopy

Broadband ultrafast optical spectroscopy methods, such as transient absorption spectroscopy and 2D spectroscopy, are widely used to study molecular dynamics. However, these techniques are typically restricted to optically thick samples,...

An organic quantum battery

Quantum batteries harness the unique properties of quantum mechanics to enhance energy storage compared to conventional batteries. In particular, they are predicted to undergo superextensive charging, where batteries with larger capacity actually take less time to charge. Up until now however, they have not been experimentally demonstrated, due to the challenges in quantum coherent control. Here we implement an array of two-level systems coupled to a photonic mode to realise a Dicke quantum battery. Our quantum battery is constructed with a microcavity formed by two dielectric mirrors enclosing a thin film of a fluorescent molecular dye in a polymer matrix. We use ultrafast optical spectroscopy to time resolve the charging dynamics of the quantum battery at femtosecond resolution. We experimentally demonstrate superextensive increases in both charging power and storage capacity, in agreement with our theoretical modelling. We find that decoherence plays an important role in stabilising energy storage, analogous to the role that dissipation plays in photosynthesis. This experimental proof-of-concept is a major milestone towards the practical application of quantum batteries in quantum and conventional devices. Our work opens new opportunities for harnessing collective effects in light-matter coupling for nanoscale energy capture, storage, and transport technologies, including the enhancement of solar cell efficiencies.

Photophysical implications of ring fusion, linker length, and twisting angle in a series of perylenediimide–thienoacene dimers

Ring fusion and conjugated bridge length dependent exciton dynamics and electronic coupling in a series of perylenediimide dimers with acceptor–donor–acceptor arrangement are investigated by ultrafast optical spectroscopy and TDDFT calculations.

Carrier multiplication in van der Waals layered transition metal dichalcogenides

Carrier multiplication (CM) is a process in which high-energy free carriers relax by generation of additional electron-hole pairs rather than by heat dissipation. CM is promising disruptive improvements in photovoltaic energy conversion and light detection technologies. Current state-of-the-art nanomaterials including quantum dots and carbon nanotubes have demonstrated CM, but are not satisfactory owing to high-energy-loss and inherent difficulties with carrier extraction. Here, we report CM in van der Waals (vdW) MoTe2 and WSe2 films, and find characteristics, commencing close to the energy conservation limit and reaching up to 99% CM conversion efficiency with the standard model. This is demonstrated by ultrafast optical spectroscopy with independent approaches, photo-induced absorption, photo-induced bleach, and carrier population dynamics. Combined with a high lateral conductivity and an optimal bandgap below 1 eV, these superior CM characteristics identify vdW materials as an attractive candidate material for highly efficient and mechanically flexible solar cells in the future.

Ultrafast Dynamic Microscopy of Carrier and Exciton Transport

We highlight the recent progress in ultrafast dynamic microscopy that combines ultrafast optical spectroscopy with microscopy approaches, focusing on the application transient absorption microscopy (TAM) to directly image energy and charge transport in solar energy harvesting and conversion systems. We discuss the principles, instrumentation, and resolutions of TAM. The simultaneous spatial, temporal, and excited-state-specific resolutions of TAM unraveled exciton and charge transport mechanisms that were previously obscured in conventional ultrafast spectroscopy measurements for systems such as organic solar cells, hybrid perovskite thin films, and molecular aggregates. We also discuss future directions to improve resolutions and to develop other ultrafast imaging contrasts beyond transient absorption.