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The discovery of small organic compounds for inducing stem cell differentiation is a time- and resource-intensive process. While data science could, in principle, facilitate the discovery of these compounds, novel approaches are required due to the difficulty of acquiring training data from large numbers of example compounds. In this paper, we demonstrate the design of a new compound for inducing cardiomyocyte differentiation using simple regression models trained with a data set containing only 80 examples. We introduce decorated shape descriptors, an information-rich molecular feature representation that integrates both molecular shape and hydrophilicity information. These models demonstrate improved performance compared to ones using standard molecular descriptors based on shape alone. Model overtraining is diagnosed using a new type of sensitivity analysis. Our new compound is designed using a conservative molecular design strategy, and its effectiveness is confirmed through expression profiles of cardiomyocyte-related marker genes using real-time polymerase chain reaction experiments on human iPS cell lines. This work demonstrates a viable data-driven strategy for designing new compounds for stem cell differentiation protocols and will be useful in situations where training data is limited., Comment: 26 pages (main paper), including 7 figures and 3 tables. 23 pages of supporting information. To be submitted to a journal

Human breath contains over 3000 volatile organic compounds, abnormal concentrations of which can indicate the presence of certain diseases. Recently, metal-organic framework (MOF)-metal oxide composite materials have been explored for chemiresistive sensor applications, however their ability to detect breath compounds associated with specific diseases remains unknown. In this work, we present a new high-throughput computational protocol for evaluating the sensing ability of MOF-metal oxide towards small organic compounds. This protocol uses a cluster-based method for accelerated structure relaxation, and a combination of binding energies and density-of-states analysis to evaluate sensing ability, the latter measured using Wasserstein distances. We apply this protocol to the case of the MOF-metal oxide composite material NM125-TiO2 and show that it is consistent with previously reported experimental results for this system. We examine the sensing ability of NM125-TiO2 for over 100 human-breath compounds spanning 13 different diseases. Statistical inference then allows us to identifies ones which subsequent experimental efforts should focus on. Overall, this work provides new tools for computational sensor research, while also illustrating how computational materials science can be integrated into the field of preventative medicine., Comment: 20 pages with 22 pages of supporting information. 7 figures and 1 table. In preparation for submission to a journal

Simulations of exciton and charge hopping in amorphous organic materials involve numerous physical parameters. Each of these parameters must be computed from costly ab initio calculations before the simulation can commence, resulting in a significant computational overhead for studying exciton diffusion, especially in large and complex material datasets. While the idea of using machine learning to quickly predict these parameters has been explored previously, typical machine learning models require long training times which ultimately contribute to simulation overheads. In this paper, we present a new machine learning architecture for building predictive models for intermolecular exciton coupling parameters. Our architecture is designed in such a way that the total training time is reduced compared to ordinary Gaussian process regression or kernel ridge regression models. Based on this architecture, we build a predictive model and use it to estimate the coupling parameters which enter into an exciton hopping simulation in amorphous pentacene. We show that this hopping simulation is able to achieve excellent predictions for exciton diffusion tensor elements and other properties as compared to a simulation using coupling parameters computed entirely from density functional theory. This result, along with the short training times afforded by our architecture, therefore shows how machine learning can be used to reduce the high computational overheads associated with exciton and charge diffusion simulations in amorphous organic materials., Comment: 29 pages. Supporting information starts on page 26

Advances in algorithms and hardware have enabled computers to design new materials atom-by-atom. However, in order for these computer-generated materials to truly address problems of societal importance, such as clean energy generation, it is not enough for them to have superior physical properties. It is also important for them to be adopted by as many users as possible. In this paper, we present a simple binary choice model for comparing catalyst materials on the basis of consumer preferences. This model considers a population of utility maximisers who select one of two materials by comparing catalytic turnover rates with sales prices. Through a mixture of numerical simulation and analytic theorems, we characterise the predictions of the model in a variety of regimes of consumer behavior. We also show how the model can be used as a guide for crafting policies for lowering catalyst prices in order to improve their market shares. This work represents a first step towards understanding how material properties should be balanced against production costs and consumer demand when designing new materials, an intellectual advance which may facilitate the spread of green materials in society., Comment: 23 pages, 6 figures, 1 table. Re-write and expansion of a previous version

Data-driven methodologies for designing new materials are developing apace, yet advances for organic crystals have been infrequent. For organic crystals, the need to predict solid-state electronic properties from molecular structure alone is an exceedingly difficult task for typical, regression-based design strategies. In this paper, we present a new strategy for designing organic crystals which circumvents the need to regress solid-state physical properties directly. At the core of this strategy is an electronic structure chart, a two-dimensional projection of an organic crystal database in which each material is positioned according to its solid-state electronic properties. We illustrate this strategy by identifying a new molecule which is predicted to show a targeted band gap and better-than-average band curvatures in the crystalline state. This strategy is the first data-driven method which can design new molecules on the basis of genuine solid-state electronic properties, and has potential to accelerate breakthroughs in the field of organic electronics and beyond., Comment: 20 pages (main paper) + 6 pages (supporting information). 4 figures (main paper). Download links to the supporting files "data_cod.txt" and "SI3.xlsx" are provided in the supporting information. Manuscript in preparation for submission to a journal

Molecular self-assembly will not become a routine method for building nanomaterials unless our ability to predict the outcome of this process is dramatically improved. Even then, reliable strategies for realizing molecular assemblies with novel properties are required for building nanomaterials for specific device applications. In this paper, I simulate the self-assembly of metal phthalocyanine derivatives adsorbed to gold(111) surfaces using a detailed statistical mechanical model and a new computational method based upon genetic algorithms and Markov chain Monte Carlo (MCMC). This method yields predictions that are not only are superior to those of ordinary MCMC but also show good agreement with experimental results. Crucially, it is predicted that molecular assemblies displaying locally disordered magnetic moments - and having potential applications as non-Gaussian noise sources for device applications - can be realized by the simple strategy of introducing asymmetry into the phthalocyanine ligands., Comment: 25 pages (main paper) + 10 pages (supporting information). 5 figures (main paper). Manuscript in preparation for submission to a journal

We introduce the stochastic Boltzmann equation (SBE) as an approach for exploring the spin dynamics of magnetic molecules coupled to a stochastic environment. The SBE is a time-evolution equation for the probability density of the spin density matrix of the system. This probability density is relevant to experiments which take measurements on single molecules, in which probabilities of observing particular spin states (rather than ensemble averages) are of interest. By analogy with standard treatments of the regular Boltzmann equation, we propose a relaxation-time approximation for the SBE, and show that solutions to the SBE under the relaxation-time approximation can be obtained by performing simple trajectory simulations for the case of a boson gas environment. Cases where the relaxation-time approximation are satisfied can therefore be investigated by careful choice of the parameters for the boson gas environment, even if the actual environment is quite different from a boson gas. The application of the SBE approach is demonstrated through an illustrative example., Comment: 46 pages, only PDF available

An open problem in applied mathematics is to predict interesting molecules which are realistic targets for chemical synthesis. In this paper, we use a spin Hamiltonian-type model to predict molecular magnets (MMs) with magnetic moments that are intrinsically robust under random shape deformations to the molecule. Using the concept of convergence in probability, we show that for MMs in which all spin centers lie in-plane and all spin center interactions are ferromagnetic, the total spin of the molecule is a `weak topological invariant' when the number of spin centers is sufficiently large. By weak topological invariant, we mean that the total spin of the molecule only depends upon the arrangement of spin centers in the molecule, and is unlikely to change under shape deformations to the molecule. Our calculations show that only between 20 and 50 spin centers are necessary for the total spin of these MMs to be a weak topological invariant. The robustness effect is particularly enhanced for 2D ferromagnetic MMs that possess a small number of spin rings in the structure., Comment: 21 pages, 5 figures

We study a gas containing two components, a small component P and a large component Q. P is selectively heated to a high temperature and then returns to equilibrium via collisions with Q. This thermal equilibration process is analysed in a new way. We divide the kinetic energy space of the molecules of P into two regions F and D, and show that the molecules of P randomly switch (`oscillate') between the two states as time proceeds due to collisions with the molecules of Q. Initially, the molecules of P are all in the state D, however because each molecule in P collides with the molecules of Q at different times, the oscillations occur out of step with each other. There is a net destructive interference between the oscillations, and so they are not observed when monitoring the average kinetic energy of the molecules of P as a function of time. We will explain the similarities and differences between this observation and transverse relaxation processes that occur in magnetic resonance spectroscopy. This study employs a stochastic model of elastic collisions between the molecules of P and Q, and for completeness we examine its relationship with the two major models of thermal equilibration in statistical physics, namely the Boltzmann equation and the Ornstein-Uhlenbeck process., Comment: 33 pages, 4 figures

Stochastic treatments of magnetic resonance spectroscopy and optical spectroscopy require evaluations of functions like , where t is time, Q(s) is the value of a stochastic process at time s, and the angular brackets denote ensemble averaging. This paper gives an exact evaluation of these functions for the case where Q is a continuous-time random walk process. The continuous time random walk describes an environment that undergoes slow, step-like changes in time. It also has a well-defined Gaussian limit, and so allows for non-Gaussian and Gaussian stochastic dynamics to be studied within a single framework. We apply the results to extract qubit-lattice interaction parameters from dephasing data of P-doped Si semiconductors (data collected elsewhere), and to calculate the two-dimensional spectrum of a three level harmonic oscillator undergoing random frequency modulations., Comment: 25 pages, 4 figures

We present an analytic method for computing the moments of a sum of independent and identically distributed random variables. The limiting behavior of these sums is very important to statistical theory, and the moment expressions that we derive allow for it to be studied relatively easily. We show this by presenting a new proof of the central limit theorem and several other convergence results., Comment: 13 pages