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Identifying a gas source in turbulent environments presents a significant challenge for critical applications such as environmental monitoring and emergency response. This issue is addressed through an approach that combines distributed IoT smart sensors with an algorithm based on Bayesian inference and Monte Carlo sampling techniques. Employing a probabilistic model of the environment, such an algorithm interprets the gas readings obtained from an array of static sensors to estimate the location of the source. The performance of our methodology is evaluated by its ability to estimate the source's location within a given time frame. To test the robustness and practical applications of the methods under real-world conditions, we deployed an advanced distributed sensors network to gather water vapor data from a controlled source. The proposed methodology performs well when using both the synthetic data generated by the model of the environment and those measured in the real experiment, with the source localization error consistently lower than the distance between one sensor and the next in the array.

Despite decades of research, demonstration of all-optical detection and control of free electron spins in silicon remains elusive. Here, we directly probe the electron spin properties in bulk silicon by measuring the polarization of luminescence following circularly polarized light excitation. The experiments performed for both direct and indirect gap excitation allow not only an experimental determination of the optical selection rules in silicon for the different phononassisted transitions but they also lead to the measurement of the spin relaxation of electrons in conditions which are not accessible using transport techniques. We also measure the spin properties of free excitons in bulk silicon, a very little explored field.

In transition metal dichalcogenide semiconductor monolayers the spin dynamics of electrons is controlled by the original spin-valley locking effect resulting from the interplay between spin-orbit interaction and inversion asymmetry. As a consequence, for electrons occupying bottom conduction bands, a carrier spin flip occurs only if there is a simultaneous change of valley. However, very little is known about the intra-valley spin relaxation processes. In this work we have performed stationary and time-resolved photoluminescence measurements in high quality WSe$_2$ monolayers. Our experiments highlight an efficient relaxation from bright to dark excitons, due to a fast intra-valley electron transfer from the top to the bottom conduction band with opposite spins. A combination of experiments and theoretical analysis allows us to infer a spin relaxation time of about $\tau_s\sim10~$ps, driven by the interplay between $\Gamma$-valley chiral phonons and spin-orbit mixing., Comment: 10 pages, 4 figures

The optical emission spectra of semiconducting transition-metal dichalcogenide monolayers highlight fascinating recombination processes of charged excitons (trions). When charge tunable WSe$_2$ monolayers are moderately doped with electrons, a strong luminescence peak emerges just below the well-understood spectral lines associated with the recombination of negatively charged bright and dark trions. Despite previous investigations, its origin remains elusive. Here, we demonstrate that this luminescence peak is the result of electron-electron assisted recombination that brightens the dark trion emission. Supporting evidence for this second-order recombination process comes from identifying the brightened emission of positively charged dark trions when the monolayer is electrostatically doped with holes. Remarkably, the discovered hole-hole assisted luminescence peak emerges in the near infrared, about 500 meV below the well-studied spectral region of excitons and trions. In magneto-photoluminescence experiments we find that the $g$-factor of this new transition ($g$ = +4) has an opposite sign compared to the well-known $g$-factor of neutral or charged excitons. This allows us to propose a mechanism of brightening of the positively charged dark trion involving the $\Gamma$ valence band., Comment: 16 pages, 6 figures

We investigate the diffusion process of negatively charged excitons (trions) in WSe2 transition metal dichalcogenide monolayer. We measure time-resolved photoluminescence spatial profiles of these excitonic complexes which exhibit a non-linear diffusion process with an effective negative diffusion behavior. Specifically, we examine the dynamics of the two negatively charged bright excitons (intervalley and intravalley trion) as well as the dark trion. The time evolution allows us to identify the interplay of different excitonic species: the trionic species appear after the neutral excitonic ones, consistent with a bimolecular formation mechanism. Using the experimental observations, we propose a phenomenological model suggesting the coexistence of two populations: a first one exhibiting a fast and efficient diffusion mechanism and a second one with a slower dynamics and a less efficient diffusion process. These two contributions could be attributed to hot and cold trion populations.

The Rashba effect in Ge/Si$_{0.15}$Ge$_{0.85}$ multiple quantum wells embedded in a p-i-n diode is studied through polarization and time-resolved photoluminescence. In addition to a sizeable redshift arising from the quantum-confined Stark effect, a threefold enhancement of the circular polarization degree of the direct transition is obtained by increasing the pump power over a 2kW/cm$^2$ range. This marked variation reflects an efficient modulation of the spin population and is further supported by dedicated investigations of the indirect gap transition. This study demonstrates a viable strategy to engineer the spin-orbit Hamiltonian through contactless optical excitation and opens the way towards the electro-optical manipulation of spins in quantum devices based on group-IV heterostructures.

Species-sampling problems (SSPs) refer to a vast class of statistical problems calling for the estimation of (discrete) functionals of the unknown species composition of an unobservable population. A common feature of SSPs is their invariance with respect to species labeling, which is at the core of the Bayesian nonparametric (BNP) approach to SSPs under the popular Pitman-Yor process (PYP) prior. In this paper, we develop a BNP approach to SSPs that are not "invariant" to species labeling, in the sense that an ordering or ranking is assigned to species' labels. Inspired by the population genetics literature on age-ordered alleles' compositions, we study the following SSP with ordering: given an observable sample from an unknown population of individuals belonging to species (alleles), with species' labels being ordered according to weights (ages), estimate the frequencies of the first $r$ order species' labels in an enlarged sample obtained by including additional unobservable samples. By relying on an ordered PYP prior, we obtain an explicit posterior distribution of the first $r$ order frequencies, with estimates being of easy implementation and computationally efficient. We apply our approach to the analysis of genetic variation, showing its effectiveness in estimating the frequency of the oldest allele, and then we discuss other potential applications.

Given an observed sample from a population of individuals belonging to species, "species-sampling" problems (SSPs) call for estimating some features of the unknown species composition of additional unobservable samples from the same population. Within SSPs, the problems of estimating coverage probabilities, the number of unseen species and coverages of prevalences have emerged in the past three decades for being the subject of numerous methodological and applied works, mostly in biological sciences but also in statistical machine learning, electrical engineering, theoretical computer science, information theory and forensic statistics. In this paper, we focus on these popular SSPs, and present an overview of their Bayesian nonparametric (BNP) analysis under the Pitman--Yor process (PYP) prior. While reviewing the literature, we improve on computation and interpretability of existing posterior inferences, typically expressed through complicated combinatorial numbers, by establishing novel posterior representations in terms of simple compound Binomial and Hypergeometric distributions. We also consider the problem of estimating the discount and scale parameters of the PYP prior, showing a property of Bayesian consistency with respect to estimation through the hierarchical Bayes and empirical Bayes approaches, that is: the discount parameter can be estimated consistently, whereas the scale parameter cannot be estimated consistently, thus advising caution in posterior inference. We conclude our work by discussing some generalizations of SSPs, mostly in the field of biological sciences, which deal with "feature-sampling", multiple populations of individuals sharing species and classes of Markov chains.

Estimation of the spatial heterogeneity in crime incidence across an entire city is an important step towards reducing crime and increasing our understanding of the physical and social functioning of urban environments. This is a difficult modeling endeavor since crime incidence can vary smoothly across space and time but there also exist physical and social barriers that result in discontinuities in crime rates between different regions within a city. A further difficulty is that there are different levels of resolution that can be used for defining regions of a city in order to analyze crime. To address these challenges, we develop a Bayesian non-parametric approach for the clustering of urban areal units at different levels of resolution simultaneously. Our approach is evaluated with an extensive synthetic data study and then applied to the estimation of crime incidence at various levels of resolution in the city of Philadelphia.

We demonstrate the application of a two stage machine learning algorithm that enables to correlate the electrical signals from a GaAs$_x$N$_{1-x}$ circular polarimeter with the intensity, degree of circular polarization and handedness of an incident light beam. Specifically, we employ a multimodal logistic regression to discriminate the handedness of light and a 6-layer neural network to establish the relationship between the input voltages, the intensity and degree of circular polarization. We have developed a particular neural network training strategy that substantially improves the accuracy of the device. The algorithm was trained and tested on theoretically generated photoconductivity and on photoluminescence experimental results. Even for a small training experimental dataset (70 instances), it is shown that the proposed algorithm correctly predicts linear, right and left circularly polarized light misclassifying less than $1.5\%$ of the cases and attains an accuracy larger than $97\%$ in the vast majority of the predictions ($92\%$) for intensity and degree of circular polarization. These numbers are significantly improved for the larger theoretically generated datasets (4851 instances). The algorithm is versatile enough that it can be easily adjusted to other device configurations where a map needs to be established between the input parameters and the device response. Training and testing data files as well as the algorithm are provided as supplementary material., Comment: 20 pages, 13 figures

The interaction of intralayer and interlayer excitons is studied in a two-dimensional semiconductor, homobilayer MoS$_2$. It is shown that the measured optical susceptibility reveals both the magnitude and the sign of the coupling constants. The interlayer exciton interacts capacitively with the intralayer B-exciton (positive coupling constant) consistent with hole tunnelling from one monolayer to the other. Conversely, the interlayer exciton interacts inductively with the intralayer A-exciton (negative coupling constant). First-principles many-body calculations show that this coupling arises via an intravalley exchange-interaction of A- and B-excitons., Comment: Main text: 6 pages, 4 figures; Supplementary Information: 17 pages, 15 figures

Stillbirth and preterm birth are major public health challenges. Using a Bayesian spatial model, we quantified patient-specific and neighborhood risks of stillbirth and preterm birth in the city of Philadelphia. We linked birth data from electronic health records at Penn Medicine hospitals from 2010 to 2017 with census-tract-level data from the United States Census Bureau. We found that both patient-level characteristics (e.g. self-identified race/ethnicity) and neighborhood-level characteristics (e.g. violent crime) were significantly associated with patients' risk of stillbirth or preterm birth. Our neighborhood analysis found that higher-risk census tracts had 2.68 times the average risk of stillbirth and 2.01 times the average risk of preterm birth compared to lower-risk census tracts. Higher neighborhood rates of women in poverty or on public assistance were significantly associated with greater neighborhood risk for these outcomes, whereas higher neighborhood rates of college-educated women or women in the labor force were significantly associated with lower risk. Several of these neighborhood associations were missed by the patient-level analysis. These results suggest that neighborhood-level analyses of adverse pregnancy outcomes can reveal nuanced relationships and, thus, should be considered by epidemiologists. Our findings can potentially guide place-based public health interventions to reduce stillbirth and preterm birth rates., Comment: 32 pages, 5 figures, 8 tables

Second harmonic generation (SHG) is a non-linear optical process, where two photons coherently combine into one photon of twice their energy. Efficient SHG occurs for crystals with broken inversion symmetry, such as transition metal dichalcogenide monolayers. Here we show tuning of non-linear optical processes in an inversion symmetric crystal. This tunability is based on the unique properties of bilayer MoS2, that shows strong optical oscillator strength for the intra- but also inter-layer exciton resonances. As we tune the SHG signal onto these resonances by varying the laser energy, the SHG amplitude is enhanced by several orders of magnitude. In the resonant case the bilayer SHG signal reaches amplitudes comparable to the off-resonant signal from a monolayer. In applied electric fields the interlayer exciton energies can be tuned due to their in-built electric dipole via the Stark effect. As a result the interlayer exciton degeneracy is lifted and the bilayer SHG response is further enhanced by an additional two orders of magnitude, well reproduced by our model calculations., Comment: main paper and supplement

The detection of light helicity is key to several research and industrial applications from drugs production to optical communications. However, the direct measurement of the light helicity is inherently impossible with conventional photodetectors based on III-V or IV-VI semiconductors, being naturally non-chiral. The prior polarization analysis of the light by a series of often moving optical elements is necessary before light is sent to the detector. A method is here presented to effectively give to the conventional dilute nitride GaAs-based semiconductor epilayer a chiral photoconductivity in paramagnetic-defect-engineered samples. The detection scheme relies on the giant spin-dependent recombination of conduction electrons and the accompanying spin polarization of the engineered defects to control the conduction band population via the electrons' spin polarization. As the conduction electron spin polarization is, in turn, intimately linked to the excitation light polarization, the light polarization state can be determined by a simple conductivity measurement. This effectively gives the GaAsN epilayer a chiral photoconductivity capable of discriminating the handedness of an incident excitation light in addition to its intensity. This approach, removing the need of any optical elements in front of a non-chiral detector, could offer easier integration and miniaturisation. This new chiral photodetector could potentially operate in a spectral range from the visible to the infra-red using (In)(Al)GaAsN alloys or ion-implanted nitrogen-free III-V compounds., Comment: 7 pages, 7 figures

We propose and numerically simulate an optoelectronic compact circular polarimeter. It allows to electrically measure the degree of circular polarization and light intensity at room temperature for a wide range of incidence angles in a single shot. The device, being based on GaAsN, is easy to integrate into standard electronics and does not require bulky movable parts nor extra detectors. Its operation hinges mainly on two phenomena: the spin dependent capture of electrons and the hyperfine interaction between bound electrons and nuclei on Ga$^{2+}$ paramagnetic centers in GaAsN. The first phenomenon confers the device with sensitivity to the degree of circular polarization and the latter allows to discriminate the handedness of the incident light., Comment: 12 pages, 7 figures

We present a magneto-optical study of the carrier dynamics in compressively strained Ge(1-x)Sn(x) films having Sn compositions up to 10% epitaxially grown on blanket Ge on Si (001) virtual substrates. We leverage the Hanle effect under steady-state excitation to study the spin-dependent optical transitions in presence of an external magnetic field. This allowed us to obtain direct access to the dynamics of the optically-induced carrier population. Our approach singled out that at cryogenic temperatures the effective lifetime of the photogenerated carriers in coherent Ge(1-x)Sn(x) occurs in the sub-ns time scale. Supported by a model estimate of the radiative lifetime, our measurements indicate that carrier recombination is dominated by non-radiative processes. Our results thus provide central information to advance the fundamental understanding of carrier kinetics in this novel direct-gap group-IV material system. Such knowledge can be a stepping stone in the quest for the implementation of Ge(1-x)Sn(x)-based functional devices.

Photon helicity-dependent photocurrent is measured at zero magnetic field on a device based on an ensemble of InGaAs/GaAs quantum dots that are embedded into a GaAs-based p-i-n diode. Our main goal is to take advantage of the long electron spin relaxation time expected in these nano-objects. In these experiments, no external magnetic field is required thanks to the use of an ultrathin magnetic CoFeB/MgO electrode, presenting perpendicular magnetic anisotropy (PMA). We observe a clear asymmetry of the photocurrent measured under respective right and left polarized light that follows the hysteresis of the magnetic layer. The amplitude of this asymmetry at zero magnetic field decreases with increasing temperatures and can be controlled with the bias. Polarization-resolved photoluminescence is detected in parallel while the device is operated as a photodetector. This demonstrates the multifunctional capabilities of the device and gives valuable insights into the spin relaxation of the electrons in the quantum dots.

The linear varying coefficient models posits a linear relationship between an outcome and covariates in which the covariate effects are modeled as functions of additional effect modifiers. Despite a long history of study and use in statistics and econometrics, state-of-the-art varying coefficient modeling methods cannot accommodate multivariate effect modifiers without imposing restrictive functional form assumptions or involving computationally intensive hyperparameter tuning. In response, we introduce VCBART, which flexibly estimates the covariate effect in a varying coefficient model using Bayesian Additive Regression Trees. With simple default settings, VCBART outperforms existing varying coefficient methods in terms of covariate effect estimation, uncertainty quantification, and outcome prediction. We illustrate the utility of VCBART with two case studies: one examining how the association between later-life cognition and measures of socioeconomic position vary with respect to age and socio-demographics and another estimating how temporal trends in urban crime vary at the neighborhood level. An R package implementing VCBART is available at https://github.com/skdeshpande91/VCBART

2D semiconducting nanosheets of Transition Metal Dichalcogenides are attractive materials for solar energy conversion because of their unique absorption properties. Here, we propose Mo thio- and oxo-thio-complexes anchored on 2D p-WSe2 nanosheets for efficient water splitting under visible light irradiation with photocurrent density up to 2.0 mA cm-2 at -0.2 V/NHE. Besides developing high electro-catalytic activity, the Mo complexe films were shown to display ability to heal surface defects. We propose that the observed healing of surface defects arises from the strong adsorption on point defects of the 2D WSe2 substrate of Mo complexes such as (MoS4)2-, (MoOS3)2-, (Mo2S6O2)2- as shown from DFT calculations. In addition to display catalytic and healing effects, the thio-, oxo-thio Mo complexes films were shown to enhance charge carrier separation and migration for the hydrogen evolution reaction, thus representing an example of multicomponent passivation layer exhibiting multiple properties.

Transition metal dichalcogenides (TMDs) constitute a versatile platform for atomically thin optoelectronics devices and spin-valley memory applications. In monolayers optical absorption is strong, but the transition energy is not tunable as the neutral exciton has essentially no out-of-plane electric dipole. In contrast, interlayer exciton transitions in heterobilayers are widely tunable in applied electric fields, but their coupling to light is considerably reduced. Here, we show tuning over 120 meV of interlayer excitons with high oscillator strength in bilayer MoS2. These shifts are due to the quantum confined Stark effect, here the electron is localised to one of the layers yet the hole is delocalised across the bilayer. We optically probe the interaction between intra- and interlayer excitons as they are energetically tuned into resonance. This allows studying their mixing supported by beyond standard density functional theory calculations including excitonic effects. In MoS2 trilayers our experiments uncover two types of interlayer excitons with and without in-built electric dipoles, respectively. Highly tunable excitonic transitions with large oscillator strength and in-built dipoles, that lead to considerable exciton-exciton interactions, hold great promise for non-linear optics with polaritons., Comment: final author version

Accurate estimation of the change in crime over time is a critical first step towards better understanding of public safety in large urban environments. Bayesian hierarchical modeling is a natural way to study spatial variation in urban crime dynamics at the neighborhood level, since it facilitates principled ``sharing of information'' between spatially adjacent neighborhoods. Typically, however, cities contain many physical and social boundaries that may manifest as spatial discontinuities in crime patterns. In this situation, standard prior choices often yield overly-smooth parameter estimates, which can ultimately produce mis-calibrated forecasts. To prevent potential over-smoothing, we introduce a prior that partitions the set of neighborhoods into several clusters and encourages spatial smoothness within each cluster. In terms of model implementation, conventional stochastic search techniques are computationally prohibitive, as they must traverse a combinatorially vast space of partitions. We introduce an ensemble optimization procedure that simultaneously identifies several high probability partitions by solving one optimization problem using a new local search strategy. We then use the identified partitions to estimate crime trends in Philadelphia between 2006 and 2017. On simulated and real data, our proposed method demonstrates good estimation and partition selection performance.

Spin dependent recombination in GaAsN offers many interesting possibilities in the design of spintronic devices mostly due to its astounding capability to reach conduction band electron spin polarizations close to 100% at room temperature. The mechanism behind the spin selective capture of electrons in Ga$^{2+}$ paramagnetic centers is revisited in this paper to address inconsistencies common to most previously presented models. Primarily, these errors manifest themselves as major disagreements with the experimental observations of two key characteristics of this phenomenon: the effective Overhauser-like magnetic field and the width of the photoluminescence Lorentzian-like curves as a function of the illumination power. These features are not only essential to understand the spin dependent recombination in GaAsN, but are also key to the design of novel spintronic devices. Here we demonstrate that the particular structure of the electron capture expressions introduces spurious electron-nucleus correlations that artificially alter the balance between the hyperfine and the Zeeman contributions. This imbalance strongly distorts the effective magnetic field and width characteristics. In this work we propose an alternative recombination mechanism that preserves the electron-nucleus correlations and, at the same time, keeps the essential properties of the spin selective capture of electrons. This mechanism yields a significant improvement to the agreement between experimental and theoretical results. In particular, our model gives results in very good accord with the experimental effective Overhauser-like magnetic field and width data, and with the degree of circular polarization under oblique magnetic fields., Comment: 13 pages, 6 figures

Understanding the relationship between change in crime over time and the geography of urban areas is an important problem for urban planning. Accurate estimation of changing crime rates throughout a city would aid law enforcement as well as enable studies of the association between crime and the built environment. Bayesian modeling is a promising direction since areal data require principled sharing of information to address spatial autocorrelation between proximal neighborhoods. We develop several Bayesian approaches to spatial sharing of information between neighborhoods while modeling trends in crime counts over time. We apply our methodology to estimate changes in crime throughout Philadelphia over the 2006-15 period, while also incorporating spatially-varying economic and demographic predictors. We find that the local shrinkage imposed by a conditional autoregressive model has substantial benefits in terms of out-of-sample predictive accuracy of crime. We also explore the possibility of spatial discontinuities between neighborhoods that could represent natural barriers or aspects of the built environment.

Coulomb bound electron-hole pairs, excitons, govern the optical properties of semi-conducting transition metal dichalcogenides like MoS$_2$ and WSe$_2$. We study optical transitions at the K-point for 2H homobilayer MoS$_2$ in Density Functional Theory (DFT) including excitonic effects and compare with reflectivity measurements in high quality samples encapsulated in hexagonal BN. In both calculated and measured spectra we find a strong interlayer exciton transition in energy between A and B intralayer excitons, observable for T$=4 -300$ K, whereas no such transition is observed for the monolayer in the same structure in this energy range. The interlayer excitons consist of an electron localized in one layer and a hole state delocalized over the bilayer, which results in the unusual combination of high oscillator strength and a static dipole moment. We also find signatures of interlayer excitons involving the second highest valence band (B) and compare absorption calculations for different bilayer stackings. For homotrilayer MoS$_2$ we also observe interlayer excitons and an energy splitting between different intralayer A-excitons originating from the middle and outer layers, respectively., Comment: 9 pages, 6 figures

We study experimentally and theoretically the exciton-phonon interaction in MoSe2 monolayers encapsulated in hexagonal BN, which has an important impact on both optical absorption and emission processes. The exciton transition linewidth down to 1 meV at low temperatures makes it possible to observe high energy tails in absorption and emission extending over several meV, not masked by inhomogeneous broadening. We develop an analytical theory of the exciton-phonon interaction accounting for the deformation potential induced by the longitudinal acoustic phonons, which plays an important role in exciton formation. The theory allows fitting absorption and emission spectra and permits estimating the deformation potential in MoSe2 monolayers. We underline the reasons why exciton-phonon coupling is much stronger in two-dimensional transition metal dichalcodenides as compared to conventional quantum well structures. The importance of exciton-phonon interactions is further highlighted by the observation of a multitude of Raman features in the photoluminescence excitation experiments., Comment: 12 pages, 5 figures

The emission of circularly polarized light from a single quantum dot relies on the injection of carriers with well-defined spin polarization. Here we demonstrate single dot electroluminescence (EL) with a circular polarization degree up to 35% at zero applied magnetic field. The injection of spin polarized electrons is achieved by combining ultrathin CoFeB electrodes on top of a spin-LED device with p-type InGaAs quantum dots in the active region. We measure an Overhauser shift of several $\mu$eV at zero magnetic field for the positively charged exciton (trion X$^+$) EL emission, which changes sign as we reverse the injected electron spin orientation. This is a signature of dynamic polarization of the nuclear spins in the quantum dot induced by the hyperfine interaction with the electrically injected electron spin. This study paves the way for electrical control of nuclear spin polarization in a single quantum dot without any external magnetic field., Comment: initial version, final version to appear in ACS Nano Letters

In III-V semiconductor nano-structures the electron and nuclear spin dynamics are strongly coupled. Both spin systems can be controlled optically. The nuclear spin dynamics is widely studied, but little is known about the initialization mechanisms. Here we investigate optical pumping of carrier and nuclear spins in charge tunable GaAs dots grown on 111A substrates. We demonstrate dynamic nuclear polarization (DNP) at zero magnetic field in a single quantum dot for the positively charged exciton X$^+$ state transition. We tune the DNP in both amplitude and sign by variation of an applied bias voltage V$_g$. Variation of $\Delta$V$_g$ of the order of 100 mV changes the Overhauser splitting (nuclear spin polarization) from -30 $\mu$eV (-22 %) to +10 $\mu$eV (+7 %), although the X$^+$ photoluminescence polarization does not change sign over this voltage range. This indicates that absorption in the structure and energy relaxation towards the X$^+$ ground state might provide favourable scenarios for efficient electron-nuclear spin flip-flops, generating DNP during the first tens of ps of the X$^+$ lifetime which is of the order of hundreds of ps. Voltage control of DNP is further confirmed in Hanle experiments., Comment: 5 pages, 2 figures