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Ultrafast spectroscopy paved the way for probing transient states of matter produced through photoexcitation. Despite significant advances, the microscopic processes governing the formation of these states remain largely unknown. This study discloses the nuclear quantum dynamics of $\mathrm{SrTiO_3}$ when excited by THz laser pumping. We use a first-principles machine-learning approach accounting for all atomistic degrees of freedom to examine the time-resolved energy flow across phonon modes following the photoexcitation, revealing the mechanism underpinning the observed phonon upconversion and quantifying the lifetime of the out-of-equilibrium motion. Crucially, our simulations predict that THz pump pulses can generate persistent out-of-equilibrium stress capable of inducing polar order. We observe a correlation between the experimentally measured lifetime of the transient inversion-symmetry-broken state and the duration of the out-of-equilibrium nuclear state. This work not only explains the experimental results on $\mathrm{SrTiO_3}$ but also establishes a framework for simulating the photoexcited quantum dynamics of nuclei from first principles without any empirical input. It lays the groundwork for systematic explorations of complex materials sensitive to photoexcitation.

The rapid advancements in ultrafast laser technology have paved the way for pumping and probing the out-of-equilibrium dynamics of nuclei in crystals. However, interpreting these experiments is extremely challenging due to the complex nonlinear responses in systems where lattice excitations interact, particularly in crystals composed of light atoms or at low temperatures where the quantum nature of ions becomes significant. In this work, we address the nonequilibrium quantum ionic dynamics from first principles. Our approach is general and can be applied to simulate any crystal, in combination with a first-principles treatment of electrons or external machine-learning potentials. It is implemented by leveraging the nonequilibrium time-dependent self-consistent harmonic approximation (TD-SCHA), with a stable, energy-conserving, correlated stochastic integration scheme that achieves an accuracy of $\mathcal{O}(dt^3)$. We benchmark the method with both a simple one-dimensional model to test its accuracy and a realistic 40-atom cell of SrTiO3 under THz laser pump, paving the way for simulations of ultrafast THz-Xray pump-probe spectroscopy like those performed in synchrotron facilities.

Multi-component metal nanoparticles (NPs) are of paramount importance in the chemical industry, as most processes therein employ heterogeneous catalysts. While these multi-component systems have been shown to result in higher product yields, improved selectivities, and greater stability through catalytic cycling, the structural dynamics of these materials in response to various stimuli (e.g. temperature, adsorbates, etc.) are not understood with atomistic resolution. Here, we present a highly accurate equivariant machine-learned force field (MLFF), constructed from ab initio training data collected using Bayesian active learning, that is able to reliably simulate PdAu surfaces and NPs in response to thermal treatment as well as exposure to reactive H$_2$ atmospheres. We thus provide a single model that is able to reliably describe the full space of geometric and chemical complexity for such a heterogeneous catalytic system across single crystals, gas-phase interactions, and NPs reacting with H$_2$, including catalyst degradation and explicit reactivity. Ultimately, we provide direct atomistic evidence that verifies existing experimental hypotheses for bimetallic catalyst deactivation under reaction conditions, namely that Pd preferentially segregates into the Au bulk through aggressive catalytic cycling and that this degradation is site-selective, as well as the reactivity for hydrogen exchange as a function of Pd ensemble size. We demonstrate that understanding of the atomistic evolution of these active sites is of the utmost importance, as it allows for design and control of material structure and corresponding performance, which can be vetted in silico., Comment: 19 pages, 8 figures (main + SI)

Predicting response of materials to external stimuli is a primary objective of computational materials science. However, current methods are limited to small-scale simulations due to the unfavorable scaling of computational costs. Here, we implement an equivariant machine-learning framework where response properties stem from exact differential relationships between a generalized potential function and applied external fields. Focusing on responses to electric fields, the method predicts electric enthalpy, forces, polarization, Born charges, and polarizability within a unified model enforcing the full set of exact physical constraints, symmetries and conservation laws. Through application to $\alpha$-SiO$_2$, we demonstrate that our approach can be used for predicting vibrational and dielectric properties of materials, and for conducting large-scale dynamics under arbitrary electric fields at unprecedented accuracy and scale. We apply our method to ferroelectric BaTiO$_3$ and capture the temperature-dependence and time evolution of hysteresis, revealing the underlying microscopic mechanisms of nucleation and growth that govern ferroelectric domain switching., Comment: 15 pages, 6 figures

Channel sounding is a vital step in understanding wireless channels for the design and deployment of wireless communication systems. In this paper, we present the design and implementation of a coherent distributed massive MIMO channel sounder operating at 5-6 GHz with a bandwidth of 400 MHz based on the NI USRP X410. Through the integration of transceiver chains and RF switches, the design facilitates the use of a larger number of antennas without significant compromise in dynamic capability. Our current implementation is capable of measuring thousands of antenna combinations within tens of milliseconds. Every radio frequency switch is seamlessly integrated with a 16-element antenna array, making the antennas more practical to be transported and flexibly distributed. In addition, the channel sounder features real-time processing to reduce the data stream to the host computer and increase the signal-to-noise ratio. The design and implementation are verified through two measurements in an indoor laboratory environment. The first measurement entails a single-antenna robot as transmitter and 128 distributed receiving antennas. The second measurement demonstrates a passive sensing scenario with a walking person. We evaluate the results of both measurements using the super-resolution algorithm SAGE. The results demonstrate the great potential of the presented sounding system for providing high-quality radio channel measurements, contributing to high-resolution channel estimation, characterization, and active and passive sensing in realistic and dynamic scenarios.

Ionic liquids (ILs) are an exciting class of electrolytes finding applications in many areas from energy storage to solvents, where they have been touted as ``designer solvents'' as they can be mixed to precisely tailor the physiochemical properties. As using machine learning interatomic potentials (MLIPs) to simulate ILs is still relatively unexplored, several questions need to be answered to see if MLIPs can be transformative for ILs. Since ILs are often not pure, but are either mixed together or contain additives, we first demonstrate that a MLIP can be trained to be compositionally transferable, i.e., the MLIP can be applied to mixtures of ions not directly trained on, whilst only being trained on a few mixtures of the same ions. We also investigate the accuracy of MLIPs for a novel IL, which we experimentally synthesize and characterize. Our MLIP trained on $\sim$200 DFT frames is in reasonable agreement with our experiments and DFT.

Nickel titanium (NiTi) is a protypical shape-memory alloy used in a range of biomedical and engineering devices, but direct molecular dynamics simulations of the martensitic B19' -> B2 phase transition driving its shape-memory behavior are rare and have relied on classical force fields with limited accuracy. Here, we train four machine-learned force fields for equiatomic NiTi based on the LDA, PBE, PBEsol, and SCAN DFT functionals. The models are trained on the fly during NPT molecular dynamics, with DFT calculations and model updates performed automatically whenever the uncertainty of a local energy prediction exceeds a chosen threshold. The models achieve accuracies of 1-2 meV/atom during training and are shown to closely track DFT predictions of B2 and B19' elastic constants and phonon frequencies. Surprisingly, in large-scale molecular dynamics simulations, only the SCAN model predicts a reversible B19' -> B2 phase transition, with the LDA, PBE, and PBEsol models predicting a reversible transition to a previously uncharacterized low-volume phase, which we hypothesize to be a new stable high-pressure phase. We examine the structure of the new phase and estimate its stability on the temperature-pressure phase diagram. This work establishes an automated active learning protocol for studying displacive transformations, reveals important differences between DFT functionals that can only be detected in large-scale simulations, provides an accurate force field for NiTi, and identifies a new phase.

Crystal dislocation dynamics, especially at high temperatures, represents a subject where experimental phenomenological input is commonly required, and parameter-free predictions, starting from quantum methods, have been beyond reach. This is especially true for phenomena like stacking faults and dislocation cross-slip, which are computationally intractable with methods like density functional theory, as $\sim 10^5-10^6$ atoms are required to reliably simulate such systems. Hence, this work extends quantum-mechanical accuracy to mesoscopic molecular dynamics simulations and opens unprecedented possibilities in material design for extreme mechanical conditions with direct atomistic insight at the deformation mesoscale. To accomplish this, we construct a Bayesian machine-learned force field (MLFF) from ab initio quantum training data, enabling direct observations of high-temperature and high-stress dislocation dynamics in single-crystalline Cu with atomistic resolution. In doing so, a generalizable training protocol is developed for construction of MLFFs for dislocation kinetics, with wide-ranging applicability to other single element systems and alloys. The resulting FLARE MLFF provides excellent predictions of static bulk elastic properties, stacking fault widths and energies, dynamic evolutions and mobilities of edge and screw dislocations, as well as cross-slip energy barriers for screw dislocations, all of which are compared to available experimental measurements. This work marks the first reliable quantitative determination of dislocation mobilities and cross-slip barriers, demonstrating a substantial advancement over previous empirical and machine learned force field models., Comment: 15 pages, 7 figures, 3 tables

The emergence of sixth-generation (6G) networks has spurred the development of novel testbeds, including sub-THz networks, cell-free systems, and 6G simulators. To maximize the benefits of these systems, it is crucial to make the generated data publicly available and easily reusable by others. Although data sharing has become a common practice, a lack of standardization hinders data accessibility and interoperability. In this study, we propose the Dataset Storage Standard (DSS) to address these challenges by facilitating data exchange and enabling convenient processing script creation in a testbed-agnostic manner. DSS supports both experimental and simulated data, allowing researchers to employ the same processing scripts and tools across different datasets. Unlike existing standardization efforts such as SigMF and NI RF Data Recording API, DSS provides a broader scope by accommodating a common definition file for testbeds and is not limited to RF data storage. The dataset format utilizes a hierarchical structure, with a tensor representation for specific experiment scenarios. In summary, DSS offers a comprehensive and flexible framework for enhancing the FAIR principles (Findability, Accessibility, Interoperability, and Reusability) in 6G testbeds, promoting open and efficient data sharing in the research community.

The need to use a short time step is a key limit on the speed of molecular dynamics (MD) simulations. Simulations governed by classical potentials are often accelerated by using a multiple-time-step (MTS) integrator that evaluates certain potential energy terms that vary more slowly than others less frequently. This approach is enabled by the simple but limiting analytic forms of classical potentials. Machine learning interatomic potentials (MLIPs), in particular recent equivariant neural networks, are much more broadly applicable than classical potentials and can faithfully reproduce the expensive but accurate reference electronic structure calculations used to train them. They still, however, require the use of a single short time step, as they lack the inherent term-by-term scale separation of classical potentials. This work introduces a method to learn a scale separation in complex interatomic interactions by co-training two MLIPs. Initially, a small and efficient model is trained to reproduce short-time-scale interactions. Subsequently, a large and expressive model is trained jointly to capture the remaining interactions not captured by the small model. When running MD, the MTS integrator then evaluates the smaller model for every time step and the larger model less frequently, accelerating simulation. Compared to a conventionally trained MLIP, our approach can achieve a significant speedup (~3x in our experiments) without a loss of accuracy on the potential energy or simulation-derived quantities., Comment: Working paper. 11 pages, 2 figures

Metal surfaces have long been known to reconstruct, significantly influencing their structural and catalytic properties. Many key mechanistic aspects of these subtle transformations remain poorly understood due to limitations of previous simulation approaches. Using active learning of Bayesian machine-learned force fields trained from ab initio calculations, we enable large-scale molecular dynamics simulations to describe the thermodynamics and time evolution of the low-index mesoscopic surface reconstructions of Au (e.g., the Au(111)-`Herringbone,' Au(110)-(1$\times$2)-`Missing-Row,' and Au(100)-`Quasi-Hexagonal' reconstructions). This capability yields direct atomistic understanding of the dynamic emergence of these surface states from their initial facets, providing previously inaccessible information such as nucleation kinetics and a complete mechanistic interpretation of reconstruction under the effects of strain and local deviations from the original stoichiometry. We successfully reproduce previous experimental observations of reconstructions on pristine surfaces and provide quantitative predictions of the emergence of spinodal decomposition and localized reconstruction in response to strain at non-ideal stoichiometries. A unified mechanistic explanation is presented of the kinetic and thermodynamic factors driving surface reconstruction. Furthermore, we study surface reconstructions on Au nanoparticles, where characteristic (111) and (100) reconstructions spontaneously appear on a variety of high-symmetry particle morphologies., Comment: Main: 17 pages, 7 figures, 1 table. SI: 9 pages, 15 figures, 1 table

This work brings the leading accuracy, sample efficiency, and robustness of deep equivariant neural networks to the extreme computational scale. This is achieved through a combination of innovative model architecture, massive parallelization, and models and implementations optimized for efficient GPU utilization. The resulting Allegro architecture bridges the accuracy-speed tradeoff of atomistic simulations and enables description of dynamics in structures of unprecedented complexity at quantum fidelity. To illustrate the scalability of Allegro, we perform nanoseconds-long stable simulations of protein dynamics and scale up to a 44-million atom structure of a complete, all-atom, explicitly solvated HIV capsid on the Perlmutter supercomputer. We demonstrate excellent strong scaling up to 100 million atoms and 70% weak scaling to 5120 A100 GPUs.

In this article we address a well-known problem at the intersection of ergodic theory and statistical mechanics. We prove that there exists a continuous eigenfunction for the transfer operator corresponding to pair potentials that satisfy a square summability condition, when the inverse temperature is subcritical. As a corollary we obtain a continuous eigenfunction for the classical Dyson model, with interactions $\J(k)=\beta \, k^{-\alpha}$, $k\ge1$, in the whole subcritical regime $\beta<\beta_c$ for which the parameter $\alpha$ is greater than $3/2$.

This paper shows how an ultrawideband channel sounder can be built with the latest National Instruments (NI) Universal Software Radio Peripheral (USRP) equipment, featuring onboard FPGA processing and utilizing open-source tools. Compared to other USRP-based channel sounders, our design is versatile, eases the requirements on the data link between the USRPs and the host, limits the measurement data size, and increases the signal-to-interference-plus-noise ratio due to averaging. Furthermore, this paper serves as a proof-of-concept for other researchers seeking to build a channel sounder based on the USRP equipment., Comment: Accepted to IEEE CAMA 2022

Quantum-mechanically accurate reactive molecular dynamics (MD) at the scale of billions of atoms has been achieved for the heterogeneous catalytic system of H$_2$/Pt(111) using the FLARE Bayesian force field. This achievement provides accelerated time-to-solution from first principles, with Bayesian active learning enabling efficient and autonomous training of the machine learning model. The resulting model is then deployed in LAMMPS on GPUs using the Kokkos performance portability library. The Bayesian force field provides quantitative uncertainty of predictions on every atomic environment, critical for detecting configurations in large reactive simulations that are outside of the training set. Scaling benchmarks were performed using real-application MD of the H$_2$/Pt(111) heterogeneous catalysis on the Summit supercomputer, with simulations reaching 0.5 trillion atoms on 4556 GPU nodes., Comment: 10 pages, 9 figures

A simultaneously accurate and computationally efficient parametrization of the energy and atomic forces of molecules and materials is a long-standing goal in the natural sciences. In pursuit of this goal, neural message passing has lead to a paradigm shift by describing many-body correlations of atoms through iteratively passing messages along an atomistic graph. This propagation of information, however, makes parallel computation difficult and limits the length scales that can be studied. Strictly local descriptor-based methods, on the other hand, can scale to large systems but do not currently match the high accuracy observed with message passing approaches. This work introduces Allegro, a strictly local equivariant deep learning interatomic potential that simultaneously exhibits excellent accuracy and scalability of parallel computation. Allegro learns many-body functions of atomic coordinates using a series of tensor products of learned equivariant representations, but without relying on message passing. Allegro obtains improvements over state-of-the-art methods on the QM9 and revised MD-17 data sets. A single tensor product layer is shown to outperform existing deep message passing neural networks and transformers on the QM9 benchmark. Furthermore, Allegro displays remarkable generalization to out-of-distribution data. Molecular dynamics simulations based on Allegro recover structural and kinetic properties of an amorphous phosphate electrolyte in excellent agreement with first principles calculations. Finally, we demonstrate the parallel scaling of Allegro with a dynamics simulation of 100 million atoms.

Machine learning interatomic force fields are promising for combining high computational efficiency and accuracy in modeling quantum interactions and simulating atomistic dynamics. Active learning methods have been recently developed to train force fields efficiently and automatically. Among them, Bayesian active learning utilizes principled uncertainty quantification to make data acquisition decisions. In this work, we present a general Bayesian active learning workflow, where the force field is constructed from a sparse Gaussian process regression model based on atomic cluster expansion descriptors. To circumvent the high computational cost of the sparse Gaussian process uncertainty calculation, we formulate a high-performance approximate mapping of the uncertainty and demonstrate a speedup of several orders of magnitude. We demonstrate the autonomous active learning workflow by training a Bayesian force field model for silicon carbide (SiC) polymorphs in only a few days of computer time and show that pressure-induced phase transformations are accurately captured. The resulting model exhibits close agreement with both \textit{ab initio} calculations and experimental measurements, and outperforms existing empirical models on vibrational and thermal properties. The active learning workflow readily generalizes to a wide range of material systems and accelerates their computational understanding.

Understanding the electrical and thermal transport properties of materials is critical to the design of electronics, sensors and energy conversion devices. Computational modeling can accurately predict materials properties but, in order to be reliable, require accurate descriptions of electron and phonon states and their interactions. While first-principles methods are capable of describing the energy spectrum of each carrier, using them to compute transport properties is still a formidable task, both computationally demanding and memory intensive, requiring integration of fine microscopic scattering details for estimation of macroscopic transport properties. To address this challenge, we present Phoebe - a newly developed software package that includes the effects of electron-phonon, phonon-phonon, boundary, and isotope scattering in computations of electrical and thermal transport properties of materials with a variety of available methods and approximations. This open source C++ code combines MPI-OpenMP hybrid parallelization with GPU acceleration and distributed memory structures to manage computational cost, allowing Phoebe to effectively take advantage of contemporary computing infrastructures. We demonstrate that Phoebe accurately and efficiently predicts a wide range of transport properties, opening avenues for accelerated computational analysis of complex crystals.

Due to the increase of Internet-of-Things (IoT) devices, IoT networks are getting overcrowded. Networks can be extended with more gateways, increasing the number of supported devices. However, as investigated in this work, massive MIMO has the potential to increase the number of simultaneous connections, while also lowering the energy expenditure of these devices. We present a study of the channel characteristics of massive MIMO in the unlicensed sub-GHz band. The goal is to support IoT applications with strict requirements in terms of number of devices, power consumption, and reliability. The assessment is based on experimental measurements using both a uniform linear and a rectangular array. Our study demonstrates and validates the advantages of deploying massive MIMO gateways to serve IoT nodes. While the results are general, here we specifically focus on static nodes. The array gain and channel hardening effect yield opportunities to lower the transmit-power of IoT nodes while also increasing reliability. The exploration confirms that exploiting large arrays brings great opportunities to connect a massive number of IoT devices by separating the nodes in the spatial domain. In addition, we give an outlook on how static IoT nodes could be scheduled based on partial channel state information.

Internet of Things (IoT) applications are emerging in many different areas, including maritime environments. One of the applications in this area is the monitoring of buoys at sea. To realize wireless tracking of buoys, an accurate prediction of the path loss in an open-sea environment is essential. So far, channel measurements at sea have mainly been conducted with antennas placed a couple of meters above the sea surface, which is higher than the buoys themselves. Therefore, we investigated the validity of the published channel models at sea by means of path loss measurements using a LoRa link with a transmitter antenna height of 0.35 m and a base station antenna height of 2.65 m and 5.2 m. Our results show that the round earth loss model is not accurate at these antenna heights. The ITU-R P.2001-3 model and a model by Bullington show a better agreement with our measurements. However, the difference between our two measurement campaigns shows that more investigation is needed on the dependence of the path loss on the sea state. Additionally, the availability of Sigfox, Narrowband Internet of Things (NB-IoT), and The Things Network at sea has been explored. We found that NB-IoT and Sigfox can be used for IoT applications in the tested area at low antenna heights.

Low-Power Wide-Area Networks operating in the unlicensed bands are being deployed to connect a rapidly growing number of Internet-of-Things devices. While the unlicensed sub-GHz band offers favorable propagation for long-range connections, measurements show that the energy consumption of the nodes is still mostly dominated by the wireless transmission affecting their autonomy. We investigate the potential benefits of deploying massive MIMO technology to increase system reliability and at the same time support low-energy devices with good coverage at sub-GHz frequencies. The impact of different antenna configurations and propagation conditions is analyzed. Both actual average experienced array gain and channel hardening are examined. The assessment demonstrates the effect of channel hardening as well as the potential benefits of the experienced array gain. These measurements serve as a first assessment of the channel conditions of massive MIMO at sub-GHz frequencies and are, to the best of our knowledge, the first of its kind.