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We propose a statistical approach for estimating the mean line width in spectra comprising Lorentzian, Gaussian, or Voigt line shapes. Our approach uses Gaussian processes in two stages to jointly model a spectrum and its Fourier transform. We generate statistical samples for the mean line width by drawing realizations for the Fourier transform and its derivative using Markov chain Monte Carlo methods. In addition to being fully automated, our method enables well-calibrated uncertainty quantification of the mean line width estimate through Bayesian inference. We validate our method using a simulation study and apply it to an experimental Raman spectrum of $\beta$-carotene.

We propose an approach utilizing gamma-distributed random variables, coupled with log-Gaussian modeling, to generate synthetic datasets suitable for training neural networks. This addresses the challenge of limited real observations in various applications. We apply this methodology to both Raman and coherent anti-Stokes Raman scattering (CARS) spectra, using experimental spectra to estimate gamma process parameters. Parameter estimation is performed using Markov chain Monte Carlo methods, yielding a full Bayesian posterior distribution for the model which can be sampled for synthetic data generation. Additionally, we model the additive and multiplicative background functions for Raman and CARS with Gaussian processes. We train two Bayesian neural networks to estimate parameters of the gamma process which can then be used to estimate the underlying Raman spectrum and simultaneously provide uncertainty through the estimation of parameters of a probability distribution. We apply the trained Bayesian neural networks to experimental Raman spectra of phthalocyanine blue, aniline black, naphthol red, and red 264 pigments and also to experimental CARS spectra of adenosine phosphate, fructose, glucose, and sucrose. The results agree with deterministic point estimates for the underlying Raman and CARS spectral signatures.

We propose a statistical model for narrowing line shapes in spectroscopy that are well approximated as linear combinations of Lorentzian or Voigt functions. We introduce a log-Gaussian Cox process to represent the peak locations thereby providing uncertainty quantification for the line narrowing. Bayesian formulation of the method allows for robust and explicit inclusion of prior information as probability distributions for parameters of the model. Estimation of the signal and its parameters is performed using a sequential Monte Carlo algorithm followed by an optimization step to determine the peak locations. Our method is validated using a simulation study and applied to a mineralogical Raman spectrum.

In Bayesian statistics, exploring multimodal posterior distribution poses major challenges for existing techniques such as Markov Chain Monte Carlo (MCMC). These problems are exacerbated in high-dimensional settings where MCMC methods typically rely upon localised proposal mechanisms. This paper introduces the Annealed Leap-Point Sampler (ALPS), which augments the target distribution state space with modified annealed (cooled) target distributions, in contrast to traditional approaches which have employed tempering. The temperature of the coldest state is chosen such that its corresponding annealed target density can be sufficiently well-approximated by a Laplace approximation. As a result, a Gaussian mixture independence Metropolis-Hastings sampler can perform mode-jumping proposals even in high-dimensional problems. The ability of this procedure to "mode hop" at this super-cold state is then filtered through to the target state using a sequence of tempered targets in a similar way to that in parallel tempering methods. ALPS also incorporates the best aspects of current gold-standard approaches to multimodal sampling in high-dimensional contexts. A theoretical analysis of the ALPS approach in high dimensions is given, providing practitioners with a gauge on the optimal setup as well as the scalability of the algorithm. For a $d$-dimensional problem the it is shown that the coldest inverse temperature level required for the ALPS only needs to be linear in the dimension, $\mathcal{O}(d)$, and this means that for a collection of multimodal problems the algorithmic cost is polynomial, $\mathcal{O}\left(d^{3}\right)$. ALPS is illustrated on a complex multimodal posterior distribution that arises from a seemingly-unrelated regression (SUR) model of longitudinal data from U.S. manufacturing firms.

Spatial statistics is an area of study devoted to the statistical analysis of data that have a spatial label associated with them. Geographers often refer to the "location information" associated with the "attribute information," whose study defines a research area called "spatial analysis." Many of the ways to manipulate spatial data are driven by algorithms with no uncertainty quantification associated with them. When a spatial analysis is statistical, that is, it incorporates uncertainty quantification, it falls in the research area called spatial statistics. The primary feature of spatial statistical models is that nearby attribute values are more statistically dependent than distant attribute values; this is a paraphrasing of what is sometimes called the First Law of Geography (Tobler, 1970).

Markov chain Monte Carlo methods for exponential family models with intractable normalizing constant, such as the exchange algorithm, require simulations of the sufficient statistics at every iteration of the Markov chain, which often result in expensive computations. Surrogate models for the likelihood function have been developed to accelerate inference algorithms in this context. However, these surrogate models tend to be relatively inflexible, and often provide a poor approximation to the true likelihood function. In this article, we propose the use of a warped, gradient-enhanced, Gaussian process surrogate model for the likelihood function, which jointly models the sample means and variances of the sufficient statistics, and uses warping functions to capture covariance nonstationarity in the input parameter space. We show that both the consideration of nonstationarity and the inclusion of gradient information can be leveraged to obtain a surrogate model that outperforms the conventional stationary Gaussian process surrogate model when making inference, particularly in regions where the likelihood function exhibits a phase transition. We also show that the proposed surrogate model can be used to improve the effective sample size per unit time when embedded in exact inferential algorithms. The utility of our approach in speeding up inferential algorithms is demonstrated on simulated and real-world data.

We propose a Bayesian statistical model for analyzing coherent anti-Stokes Raman scattering (CARS) spectra. Our quantitative analysis includes statistical estimation of constituent line-shape parameters, underlying Raman signal, error-corrected CARS spectrum, and the measured CARS spectrum. As such, this work enables extensive uncertainty quantification in the context of CARS spectroscopy. Furthermore, we present an unsupervised method for improving spectral resolution of Raman-like spectra requiring little to no \textit{a priori} information. Finally, the recently-proposed wavelet prism method for correcting the experimental artefacts in CARS is enhanced by using interpolation techniques for wavelets. The method is validated using CARS spectra of adenosine mono-, di-, and triphosphate in water, as well as, equimolar aqueous solutions of D-fructose, D-glucose, and their disaccharide combination sucrose.

This article surveys computational methods for posterior inference with intractable likelihoods, that is where the likelihood function is unavailable in closed form, or where evaluation of the likelihood is infeasible. We review recent developments in pseudo-marginal methods, approximate Bayesian computation (ABC), the exchange algorithm, thermodynamic integration, and composite likelihood, paying particular attention to advancements in scalability for large datasets. We also mention R and MATLAB source code for implementations of these algorithms, where they are available., Comment: arXiv admin note: text overlap with arXiv:1503.08066

Raman spectroscopy can be used to identify molecules such as DNA by the characteristic scattering of light from a laser. It is sensitive at very low concentrations and can accurately quantify the amount of a given molecule in a sample. The presence of a large, nonuniform background presents a major challenge to analysis of these spectra. To overcome this challenge, we introduce a sequential Monte Carlo (SMC) algorithm to separate each observed spectrum into a series of peaks plus a smoothly-varying baseline, corrupted by additive white noise. The peaks are modelled as Lorentzian, Gaussian, or pseudo-Voigt functions, while the baseline is estimated using a penalised cubic spline. This latent continuous representation accounts for differences in resolution between measurements. The posterior distribution can be incrementally updated as more data becomes available, resulting in a scalable algorithm that is robust to local maxima. By incorporating this representation in a Bayesian hierarchical regression model, we can quantify the relationship between molecular concentration and peak intensity, thereby providing an improved estimate of the limit of detection, which is of major importance to analytical chemistry.

The inverse temperature parameter of the Potts model governs the strength of spatial cohesion and therefore has a major influence over the resulting model fit. A difficulty arises from the dependence of an intractable normalising constant on the value of this parameter and thus there is no closed-form solution for sampling from the posterior distribution directly. There are a variety of computational approaches for sampling from the posterior without evaluating the normalising constant, including the exchange algorithm and approximate Bayesian computation (ABC). A serious drawback of these algorithms is that they do not scale well for models with a large state space, such as images with a million or more pixels. We introduce a parametric surrogate model, which approximates the score function using an integral curve. Our surrogate model incorporates known properties of the likelihood, such as heteroskedasticity and critical temperature. We demonstrate this method using synthetic data as well as remotely-sensed imagery from the Landsat-8 satellite. We achieve up to a hundredfold improvement in the elapsed runtime, compared to the exchange algorithm or ABC. An open source implementation of our algorithm is available in the R package "bayesImageS."

In images with low contrast-to-noise ratio (CNR), the information gain from the observed pixel values can be insufficient to distinguish foreground objects. A Bayesian approach to this problem is to incorporate prior information about the objects into a statistical model. This paper introduces a method for representing spatial prior information as an external field in a hidden Potts model of the image lattice. The prior distribution of the latent pixel labels is a mixture of Gaussian fields, centred on the positions of the objects at a previous point in time. This model is particularly applicable in longitudinal imaging studies, where the manual segmentation of one image can be used as a prior for automatic segmentation of subsequent images. The model is demonstrated by application to cone-beam computed tomography (CT), an imaging modality that exhibits distortions in pixel values due to X-ray scatter. The external field prior results in a substantial improvement in segmentation accuracy, reducing the mean pixel misclassification rate on our test images from 87% to 6%.

Most of the existing algorithms for approximate Bayesian computation (ABC) assume that it is feasible to simulate pseudo-data from the model at each iteration. However, the computational cost of these simulations can be prohibitive for high dimensional data. An important example is the Potts model, which is commonly used in image analysis. Images encountered in real world applications can have millions of pixels, therefore scalability is a major concern. We apply ABC with a synthetic likelihood to the hidden Potts model with additive Gaussian noise. Using a pre-processing step, we fit a binding function to model the relationship between the model parameters and the synthetic likelihood parameters. Our numerical experiments demonstrate that the precomputed binding function dramatically improves the scalability of ABC, reducing the average runtime required for model fitting from 71 hours to only 7 minutes. We also illustrate the method by estimating the smoothing parameter for remotely sensed satellite imagery. Without precomputation, Bayesian inference is impractical for datasets of that scale., Comment: 5th IMS-ISBA joint meeting (MCMSki IV)