Spatial-mode demultiplexing for enhanced intensity and distance measurement.

Spatial-mode demultiplexing (SPADE) has recently been adopted to measure the separation in the transverse plane between two incoherent point-like sources with sub-wavelength separation. It has been argued that this approach may yield extraordinary performances in the photon-counting regime. Here, we explore SPADE as a tool for precision measurements in the regime of bright, incoherent sources. First we analyze the general problem of estimating the second moments of the source's intensity distribution, for an extended incoherent source of any shape. Our theory predicts a substantial improvement in signal-to-noise ratio (SNR) of SPADE over direct imaging in the sub-wavelength regime. Second, we present an experimental application of SPADE to the case of two point-like, bright sources. We demonstrate the use of this setup for the estimation of the transverse separation and for the estimation of the relative intensity, confirming the expected improvement in SNR.

Attosecond-Level Delay Sensing via Temporal Quantum Erasing.

Traditional Hong-Ou-Mandel (HOM) interferometry, insensitive to photons phase mismatch, proved to be a rugged single-photon interferometric technique. By introducing a post-beam splitter polarization-dependent delay, it is possible to recover phase-sensitive fringes, obtaining a temporal quantum eraser that maintains the ruggedness of the original HOM with enhanced sensitivity. This setup shows promising applications in biological sensing and optical metrology, where high sensitivity requirements are coupled with the necessity to keep light intensity as low as possible to avoid power-induced degradation. In this paper, we developed a highly sensitive single photon birefringence-induced delay sensor operating in the telecom range (1550 nm). By using a temporal quantum eraser based on common path Hongr-Ou-Mandel Interferometry, we were able to achieve a sensitivity of 4 as for an integration time of 2·104 s.

Testing the speed of "spooky action at a distance" in a tabletop experiment.

Nonlocality, probably the principal friction between Quantum Physics and Relativity, disturbed the physicists even more than realism since it looks to originate superluminal signalling, the Einsteinian "Spooky action at a distance". From 2000 on, several tests to set lower bounds of the Spooky action at a distance velocity ([Formula: see text]) have been performed. They are usually based on a Bell Test performed in km long and carefully balanced experimental setups to fix a more and more improved bound making some assumptions dictated by the experimental conditions. By exploiting advances in quantum technologies, we performed a Bell's test with an improved bound in a tabletop experiment of the order of few minutes, thus being able to control parameters otherwise uncontrollable in an extended setup or in long lasting experiments.

Exploiting Sentinel-5P TROPOMI and Ground Sensor Data for the Detection of Volcanic SO2 Plumes and Activity in 2018-2021 at Stromboli, Italy.

Sulfur dioxide (SO2) degassing at Strombolian volcanoes is directly associated with magmatic activity, thus its monitoring can inform about the style and intensity of eruptions. The Stromboli volcano in southern Italy is used as a test case to demonstrate that the TROPOspheric Monitoring Instrument (TROPOMI) onboard the Copernicus Sentinel-5 Precursor (Sentinel-5P) satellite has the suitable spatial resolution and sensitivity to carry out local-scale SO2 monitoring of relatively small-size, nearly point-wise volcanic sources, and distinguish periods of different activity intensity. The entire dataset consisting of TROPOMI Level 2 SO2 geophysical products from UV sensor data collected over Stromboli from 6 May 2018 to 31 May 2021 is processed with purposely adapted Python scripts. A methodological workflow is developed to encompass the extraction of total SO2 Vertical Column Density (VCD) at given coordinates (including conditional VCD for three different hypothetical peaks at 0-1, 7 and 15 km), as well as filtering by quality in compliance with the Sentinel-5P Validation Team's recommendations. The comparison of total SO2 VCD time series for the main crater and across different averaging windows (3 × 3, 5 × 5 and 4 × 2) proves the correctness of the adopted spatial sampling criterion, and practical recommendations are proposed for further implementation in similar volcanic environments. An approach for detecting SO2 VCD peaks at the volcano is trialed, and the detections are compared with the level of SO2 flux measured at ground-based instrumentation. SO2 time series analysis is complemented with information provided by contextual Sentinel-2 multispectral (in the visible, near and short-wave infrared) and Suomi NPP VIIRS observations. The aim is to correctly interpret SO2 total VCD peaks when they either (i) coincide with medium to very high SO2 emissions as measured in situ and known from volcanological observatory bulletins, or (ii) occur outside periods of significant emissions despite signs of activity visible in Sentinel-2 data. Finally, SO2 VCD peaks in the time series are further investigated through daily time lapses during the paroxysms in July-August 2019, major explosions in August 2020 and a more recent period of activity in May 2021. Hourly wind records from ECMWF Reanalysis v5 (ERA5) data are used to identify local wind direction and SO2 plume drift during the time lapses. The proposed analysis approach is successful in showing the SO2 degassing associated with these events, and warning whenever the SO2 VCD at Stromboli may be overestimated due to clustering with the plume of the Mount Etna volcano.

Direct Comb Vernier Spectroscopy for Fractional Isotopic Ratio Determinations.

Accurate isotopic composition analysis of the greenhouse-gasses emitted in the atmosphere is an important step to mitigate global climate warnings. Optical frequency comb-based spectroscopic techniques have shown ideal performance to accomplish the simultaneous monitoring of the different isotope substituted species of such gases. The capabilities of one such technique, namely, direct comb Vernier spectroscopy, to determine the fractional isotopic ratio composition are discussed. This technique combines interferometric filtering of the comb source in a Fabry-Perot that contains the sample gas, with a high resolution dispersion spectrometer to resolve the spectral content of each interacting frequency inside of the Fabry-Perot. Following this methodology, simultaneous spectra of ro-vibrational transitions of 12C16O2 and 13C16O2 molecules are recorded and analyzed with an accurate fitting procedure. Fractional isotopic ratio 13C/12C at 3% of precision is measured for a sample of CO2 gas, showing the potentialities of the technique for all isotopic-related applications of this important pollutant.

Synergistic Approach of Ultrafast Spectroscopy and Molecular Simulations in the Characterization of Intramolecular Charge Transfer in Push-Pull Molecules.

The comprehensive characterization of Intramolecular Charge Transfer (ICT) stemming in push-pull molecules with a delocalized π-system of electrons is noteworthy for a bespoke design of organic materials, spanning widespread applications from photovoltaics to nanomedicine imaging devices. Photo-induced ICT is characterized by structural reorganizations, which allows the molecule to adapt to the new electronic density distribution. Herein, we discuss recent photophysical advances combined with recent progresses in the computational chemistry of photoactive molecular ensembles. We focus the discussion on femtosecond Transient Absorption Spectroscopy (TAS) enabling us to follow the transition from a Locally Excited (LE) state to the ICT and to understand how the environment polarity influences radiative and non-radiative decay mechanisms. In many cases, the charge transfer transition is accompanied by structural rearrangements, such as the twisting or molecule planarization. The possibility of an accurate prediction of the charge-transfer occurring in complex molecules and molecular materials represents an enormous advantage in guiding new molecular and materials design. We briefly report on recent advances in ultrafast multidimensional spectroscopy, in particular, Two-Dimensional Electronic Spectroscopy (2DES), in unraveling the ICT nature of push-pull molecular systems. A theoretical description at the atomistic level of photo-induced molecular transitions can predict with reasonable accuracy the properties of photoactive molecules. In this framework, the review includes a discussion on the advances from simulation and modeling, which have provided, over the years, significant information on photoexcitation, emission, charge-transport, and decay pathways. Density Functional Theory (DFT) coupled with the Time-Dependent (TD) framework can describe electronic properties and dynamics for a limited system size. More recently, Machine Learning (ML) or deep learning approaches, as well as free-energy simulations containing excited state potentials, can speed up the calculations with transferable accuracy to more complex molecules with extended system size. A perspective on combining ultrafast spectroscopy with molecular simulations is foreseen for optimizing the design of photoactive compounds with tunable properties.

Dioxin and Related Compound Detection: Perspectives for Optical Monitoring.

Dioxins and related compounds are environmental xenobiotics that are dangerous to human life, due to the accumulation and persistence in the environment and in the food chain. Cancer, reproductive and developmental issues, and damage to the immune system and endocrine system are only a few examples of the impact of such substances in everyday life. For these reasons, it is fundamental to detect and monitor these molecules in biological samples. The consolidated technique for analytical evaluation is gas chromatography combined with high-resolution mass spectrometry. Nowadays, the development of mid-infrared optical components like broadband laser sources, optical frequency combs, high performance Fourier-transform infrared spectroscopy, and plasmonic sensors open the way to new techniques for detection and real time monitoring of these organic pollutants in gaseous or liquid phase, with sufficient sensitivity and selectivity, and in short time periods. In this review, we report the latest techniques for the detection of dioxins, furans and related compounds based on optical and spectroscopic methods, looking at future perspectives.

TCDD Toxicity Mediated by Epigenetic Mechanisms.

Dioxins are highly toxic and persistent halogenated organic pollutants belonging to two families i.e., Polychlorinated Dibenzo-p-Dioxins (PCDDs) and Polychlorinated Dibenzo Furans (PCDFs). They can cause cancer, reproductive and developmental issues, damage to the immune system, and can deeply interfere with the endocrine system. Dioxins toxicity is mediated by the Aryl-hydrocarbon Receptor (AhR) which mediates the cellular metabolic adaptation to these planar aromatic xenobiotics through the classical transcriptional regulation pathway, including AhR binding of ligand in the cytosol, translocation of the receptor to the nucleus, dimerization with the AhR nuclear translocator, and the binding of this heterodimeric transcription factor to dioxin-responsive elements which regulate the expression of genes involved in xenobiotic metabolism. 2,3,7,8-TCDD is the most toxic among dioxins showing the highest affinity toward the AhR receptor. Beside this classical and well-studied pathway, a number of papers are dealing with the role of epigenetic mechanisms in the response to environmental xenobiotics. In this review, we report on the potential role of epigenetic mechanisms in dioxins-induced cellular response by inspecting recent literature and focusing our attention on epigenetic mechanisms induced by the most toxic 2,3,7,8-TCDD.

A New Precision Spectroscopy Based Method for Boltzmann Constant Determination and Primary Thermometry.

We propose a new independent thermometry method, line strength ratio thermometry (LRT), based on optical spectroscopy measurement of the line strength intensity ratio R between pairs of molecular transitions. Due to strong dependence of R on kT, a given measurement uncertainty δR for R reflects in a small uncertainty of kT determination. By assuming experimental uncertainties of R and T to be those reported in literature, we foresee a k determination at the 5 ppm level, which is better than the most precise k determination by using Doppler broadening thermometry (DBT). In the frame of a new definition of the SI Kelvin unit, based on k as fixed constant, once the k constant is exactly established, LRT is proposed as a high resolution noncontact thermometry technique for absolute temperature measurements of gas samples at the ppm level.

Tunable Microcavity-Stabilized Quantum Cascade Laser for Mid-IR High-Resolution Spectroscopy and Sensing.

The need for highly performing and stable methods for mid-IR molecular sensing and metrology pushes towards the development of more and more compact and robust systems. Among the innovative solutions aimed at answering the need for stable mid-IR references are crystalline microresonators, which have recently shown excellent capabilities for frequency stabilization and linewidth narrowing of quantum cascade lasers with compact setups. In this work, we report on the first system for mid-IR high-resolution spectroscopy based on a quantum cascade laser locked to a CaF2 microresonator. Electronic locking narrows the laser linewidth by one order of magnitude and guarantees good stability over long timescales, allowing, at the same time, an easy way for finely tuning the laser frequency over the molecular absorption line. Improvements in terms of resolution and frequency stability of the source are demonstrated by direct sub-Doppler recording of a molecular line.