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Nanoparticle surface structural dynamics is believed to play a significant role in regulating functionalities such as diffusion, reactivity, and catalysis but the atomic-level processes are not well understood. Atomic resolution characterization of nanoparticle surface dynamics is challenging since it requires both high spatial and temporal resolution. Though ultrafast transmission electron microscopy (TEM) can achieve picosecond temporal resolution, it is limited to nanometer spatial resolution. On the other hand, with the high readout rate of new electron detectors, conventional TEM has the potential to visualize atomic structure with millisecond time resolutions. However, the need to limit electron dose rates to reduce beam damage yields millisecond images that are dominated by noise, obscuring structural details. Here we show that a newly developed unsupervised denoising framework based on artificial intelligence enables observations of metal nanoparticle surfaces with time resolutions down to 10 ms at moderate electron dose. On this timescale, we find that many nanoparticle surfaces continuously transition between ordered and disordered configurations. The associated stress fields can penetrate below the surface leading to defect formation and destabilization making the entire nanoparticle fluxional. Combining this unsupervised denoiser with electron microscopy greatly improves spatio-temporal characterization capabilities, opening a new window for future exploration of atomic-level structural dynamics in materials.

In this article we establish two fundamental results for the sublevel set persistent homology for stationary processes indexed by the positive integers. The first is a strong law of large numbers for the persistence diagram (treated as a measure "above the diagonal" in the extended plane) evaluated on a large class of sets and functions$\unicode{x2014}$more than just continuous functions with compact support. We prove this result subject to only minor conditions that the sequence is ergodic and the tails of the marginals are not too heavy. The second result is a central limit theorem for the persistence diagram evaluated on the class of all step functions; this result holds as long as a $\rho$-mixing criterion is satisfied and the distributions of the partial maxima do not decay too slowly. Our results greatly expand those extant in the literature to allow for more fruitful use in statistical applications, beyond idealized settings. Examples of distributions and functions for which the limit theory holds are provided throughout., Comment: 30 pages, 1 figure. Versions 1 and 2 uploaded to arXiv should be disregarded as they contained an erroneous proof of the CLT, which has been corrected in Version 3

We present a Bayesian method for multivariate changepoint detection that allows for simultaneous inference on the location of a changepoint and the coefficients of a logistic regression model for distinguishing pre-changepoint data from post-changepoint data. In contrast to many methods for multivariate changepoint detection, the proposed method is applicable to data of mixed type and avoids strict assumptions regarding the distribution of the data and the nature of the change. The regression coefficients provide an interpretable description of a potentially complex change. For posterior inference, the model admits a simple Gibbs sampling algorithm based on P\'olya-gamma data augmentation. We establish conditions under which the proposed method is guaranteed to recover the true underlying changepoint. As a testing ground for our method, we consider the problem of detecting topological changes in time series of images. We demonstrate that our proposed method $\mathtt{bclr}$, combined with a topological feature embedding, performs well on both simulated and real image data. The method also successfully recovers the location and nature of changes in more traditional changepoint tasks., Comment: 34 pages (main), 18 pages (supplementary), 12 figures, and 10 tables

We present new spatially resolved astrometry and photometry of the CD-27 11535 system, a member of the $\beta$ Pictoris moving group consisting of two resolved K-type stars on a $\sim$20-year orbit. We fit an orbit to relative astrometry measured from NIRC2, GPI, and archival NaCo images, in addition to literature measurements. However, the total mass inferred from this orbit is significantly discrepant from that inferred from stellar evolutionary models using the luminosity of the two stars. We explore two hypotheses that could explain this discrepant mass sum; a discrepant parallax measurement from Gaia due to variability, and the presence of an additional unresolved companion to one of the two components. We find that the $\sim$20-year orbit could not bias the parallax measurement, but that variability of the components could produce a large amplitude astrometric motion, an effect which cannot be quantified exactly without the individual Gaia measurements. The discrepancy could also be explained by an additional star in the system. We jointly fit the astrometric and photometric measurements of the system to test different binary and triple architectures for the system. Depending on the set of evolutionary models used, we find an improved goodness of fit for a triple system architecture that includes a low-mass ($M=0.177\pm0.055$\,$M_{\odot}$) companion to the primary star. Further studies of this system will be required in order to resolve this discrepancy, either by refining the parallax measurement with a more complex treatment of variability-induced astrometric motion, or by detecting a third companion., Comment: 12 pages + references and appendix, 12 figures, 5 tables

The heterogeneity of the viscoelasticity of a lamellar gel network based on cetyl-trimethylammonium chloride (CTAC) and ceto-stearyl alcohol was studied using particle tracking microrheology. A recurrent neural network (RNN) architecture was used for estimating the Hurst exponent, $H$, on small sections of tracks of probe spheres moving with fractional Brownian motion. Thus dynamic segmentation of tracks via neural networks was used in microrheology for the first time and it is significantly more accurate than using mean square displacements. An ensemble of 414 particles produces a mean squared displacement (MSD) that is subdiffusive in time, $t$, with a power law of the form $t^{0.74\pm0.02}$, indicating power law viscoelasticity. RNN analysis of the probability distributions of $H$, combined with detailed analysis of the time-averaged MSDs of individual tracks, revealed diverse diffusion processes belied by the simple scaling of the ensemble MSD, such as caging phenomena, which give rise to the complex viscoelasticity of lamellar gels., Comment: 15 pages without references (17 with references), 13 figures

Ridge detection is a classical tool to extract curvilinear features in image processing. As such, it has great promise in applications to material science problems; specifically, for trend filtering relatively stable atom-shaped objects in image sequences, such as Transmission Electron Microscopy (TEM) videos. Standard analysis of TEM videos is limited to frame-by-frame object recognition. We instead harness temporal correlation across frames through simultaneous analysis of long image sequences, specified as a spatio-temporal image tensor. We define new ridge detection algorithms to non-parametrically estimate explicit trajectories of atomic-level object locations as a continuous function of time. Our approach is specially tailored to handle temporal analysis of objects that seemingly stochastically disappear and subsequently reappear throughout a sequence. We demonstrate that the proposed method is highly effective and efficient in simulation scenarios, and delivers notable performance improvements in TEM experiments compared to other material science benchmarks., Comment: 27 pages, 11 figures

We propose a flexible algorithm for feature detection and hypothesis testing in images with ultra low signal-to-noise ratio using cubical persistent homology. Our main application is in the identification of atomic columns and other features in transmission electron microscopy (TEM). Cubical persistent homology is used to identify local minima and their size in subregions in the frames of nanoparticle videos, which are hypothesized to correspond to relevant atomic features. We compare the performance of our algorithm to other employed methods for the detection of columns and their intensity. Additionally, Monte Carlo goodness-of-fit testing using real valued summaries of persistence diagrams derived from smoothed images (generated from pixels residing in the vacuum region of an image) is developed and employed to identify whether or not the proposed atomic features generated by our algorithm are due to noise. Using these summaries derived from the generated persistence diagrams, one can produce univariate time series for the nanoparticle videos, thus providing a means for assessing fluxional behavior. A guarantee on the false discovery rate for multiple Monte Carlo testing of identical hypotheses is also established., Comment: 42 pages, 21 figures, 9 tables

We discuss the VC-dimension of a class of multiples of integers and primes (equivalently indicator functions) and demonstrate connections to prime counting functions. Additionally, we prove limit theorems for the behavior of an empirical risk minimization rule as well as the weights assigned to the output hypothesis in AdaBoost for these "prime-identifying" indicator functions, when we sample $m_n$ i.i.d. points uniformly from the integers $\{2, \dots, n\}$., Comment: 9 pages, 0 figures

We consider the stochastic behavior of a class of local $U$-statistics of Poisson processes$-$which include subgraph and simplex counts as special cases, and amounts to quantifying clustering behavior$-$for point clouds lying in diverging halfspaces. We provide limit theorems for distributions with light and heavy tails. In particular, we prove finite-dimensional central limit theorems. In the light tail case we investigate tails that decay at least as slow as exponential and at least as fast as Gaussian. These results also furnish as a corollary that $U$-statistics for halfspaces diverging at different angles are asymptotically independent, and that there is no asymptotic independence for heavy-tailed densities. Using state-of-the-art bounds derived from recent breakthroughs combining Stein's method and Malliavin calculus, we quantify the rate of this convergence in terms of Kolmogorov distance. We also investigate the behavior of local $U$-statistics of a Poisson Process conditioned to lie in diverging halfspace and show how the rate of convergence in the Kolmogorov distance is faster the lighter the tail of the density is., Comment: 25 pages, 3 figures