Note: Comparison between a prism-based and an acousto-optic tunable filter-based spectrometer for diffusive media

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Time-resolved laser spectroscopy for the in situ characterization of methacrylate monomer flow within spruce

Time-resolved diffuse optical spectroscopy (TRS) was investigated as a nondestructive method to characterize the post-impregnation distribution of methacrylate monomers within spruce ($\textit{Picea abies}$). TRS was also used to monitor the flow of methacrylate monomers in situ, within spruce, during impregnation with both spatial and temporal resolution. The data were compared to fluid flow models developed by Darcy and Bramhall demonstrating that neither of these models were able to accurately describe the experimental results, highlighting the need for development of new models. Nondestructive characterization by TRS did not require staining of the monomer treatment solution, multivariate analysis or complex sample pre-treatment, thus highlighting the facile applicability of this technique.The authors would like to thank Prof. Paul Linden and Dr. Henry Burridge for useful discussion during the preparation of this manuscript and the EPSRC, ERC Starting investigators Grant (ASPiRe, 240629), CUSBO, FP7 Laserlab-Europe (No. 284464) and the Walters Kundert Trust for financial support

Ultrafast valley relaxation dynamics in monolayer MoS2 probed by nonequilibrium optical techniques

We study the exciton valley relaxation dynamics in single-layer MoS2 by a combination of two nonequilibrium optical techniques: time-resolved Faraday rotation and time-resolved circular dichroism. The depolarization dynamics, measured at 77 K, exhibits a peculiar biexponential decay, characterized by two distinct time scales of 200 fs and 5 ps. The fast relaxation of the valley polarization is in good agreement with a model including the intervalley electron-hole Coulomb exchange as the dominating mechanism. The valley relaxation dynamics is further investigated as a function of temperature and photoinduced exciton density. We measure a strong exciton density dependence of the transient Faraday rotation signal. This indicates the key role of exciton-exciton interactions in MoS2 valley relaxation dynamics

Light dependent redox catalysis by Photosystem I complexes encapsulated in organic nanoparticles

Photosystem I (PSI) is a pigment binding multi-subunit protein complexes involved in photosynthesis. PSI is localized in the thylakoid membranes and catalyze the electron transfer reaction from plastocyanin to ferredoxin, as one of the main steps involved in conversion of light energy into chemical energy. PSI is highly efficiency with a photochemical efficiency close to one. Several attempts have doing in the past in order to exploit the high efficiency and high stability of PSI in an extra-cellular context in order to catalyze electron transfer reactions: in this work we present an innovative solution for exploiting the photochemical properties of PSI, by encapsulation of PSI complexes in organic nanoparticles. Nanoparticles offer a protected environment to the encapsulated molecule, giving it the possibility of preserving its functional properties and studying how they change over time. In this work the complete characterization, both morphological and functional, of nanostructures obtained by encapsulation of PSI complexes purified from higher plants with PLGA (poly lactic-co-glycolic acid) polymer is presented. The results obtained by transient absorption and time-resolved fluorescence demonstrate that encapsulated PSI were characterized by an higher photochemcial activity compared to PSI complexes in detergent solution. Moreover, encapsulated PSI maintained the high efficiency observed for several weeks even if exposed to very strong light, being more stable compared to PSI in detergent solution. Finally, the nanostructures obtained by encapsulated PSI were able to catalyze light dependent redox reactions with electron acceptors and donors outside the nanostructures Potential application of these PLGA encapsulated PSI in different fields are thus presented and discussed

Phonon coherences reveal the polaronic character of excitons in two-dimensional lead halide perovskites

Hybrid organic–inorganic semiconductors feature complex lattice dynamics due to the ionic character of the crystal and the softness arising from non-covalent bonds between molecular moieties and the inorganic network. Here we establish that such dynamic structural complexity in a prototypical two-dimensional lead iodide perovskite gives rise to the coexistence of diverse excitonic resonances, each with a distinct degree of polaronic character. By means of high-resolution resonant impulsive stimulated Raman spectroscopy, we identify vibrational wavepacket dynamics that evolve along different configurational coordinates for distinct excitons and photocarriers. Employing density functional theory calculations, we assign the observed coherent vibrational modes to various low-frequency (≲50 cm−1) optical phonons involving motion in the lead iodide layers. We thus conclude that different excitons induce specific lattice reorganizations, which are signatures of polaronic binding. This insight into the energetic/configurational landscape involving globally neutral primary photoexcitations may be relevant to a broader class of emerging hybrid semiconductor materials

Encapsulation of Photosystem i in Organic Microparticles Increases Its Photochemical Activity and Stability for Ex Vivo Photocatalysis

Photosystem I (PSI) is a pigment binding multisubunit protein complex involved in the light phase of photosynthesis, catalyzing a light-dependent electron transfer reaction from plastocyanin to ferredoxin. PSI is characterized by a photochemical efficiency close to one, suggesting its possible application in light-dependent redox reaction in an extracellular context. The stability of PSI complexes isolated from plant cells is however limited if not embedded in a protective environment. Here we show an innovative solution for exploiting the photochemical properties of PSI, by encapsulation of isolated PSI complexes in PLGA (poly lactic-co-glycolic acid) organic microparticles. These encapsulated PSI complexes were able to catalyze light-dependent redox reactions with electron acceptors and donors outside the PLGA microparticles. Moreover, PSI complexes encapsulated in PLGA microparticles were characterized by a higher photochemical activity and stability compared with PSI complexes in detergent solution, suggesting their possible application for ex vivo photocatalysis

InGaAs/InP Single Photon Avalanche Diode operated in gated mode for time-resolved diffuse optical spectroscopy up to 1700 nm

Time-domain diffuse optical spectroscopy is being applied with increasing success to study highly scattering media, mainly in the fields of non-invasive medical diagnostics and quality assessment of food and pharmaceutical products. The region beyond 1100 nm is still largely unexplored by time-domain techniques, probably due to the difficult combination of tunable pulsed sources and suitable single-photon detectors. We extend the spectral range up to 1700 nm thanks to a pulsed supercontinuum laser and a time-gated InGaAs/InP single-photon avalanche diode, with potential applications in medical diagnostics and in the study of scattering materials. A first application on collagen powder is shown