scholarly journals Charge Transfer Landscape Manifesting Structure-Rate Relationship in the Condensed Phase via Machine Learning

2021 ◽  
Author(s):  
Dominikus Brian ◽  
Xiang Sun
Keyword(s):  
Molecular Structure ◽  
Machine Learning ◽  
Charge Transfer ◽  
Condensed Phase ◽  
Energy Levels ◽  
Absolute Error ◽  
Free Energies ◽  
Explicit Solvent ◽  
Reorganization Energies ◽  
Shed Light

In this work, we develop a machine learning (ML) strategy to map molecular structure to condensed-phase charge transfer (CT) properties including CT rate constants, energy levels, electronic couplings, energy gaps, reorganization energies, and reaction free energies, which are called CT fingerprints. The CT fingerprints of selected landmark structures covering the conformation space of an organic photovoltaic molecule dissolved in explicit solvent are computed and used to train ML models using kernel ridge regression. The ML models show high predictive power with R2>0.97, and both mean absolute error and root mean square error within chemical accuracy. The CT landscape for millions of molecular dynamics sampled structures is thus constructed, which allows for instant prediction of CT rate properties given any molecular structure. The unprecedented CT landscape will shed light on real-time CT dynamics in nanoscale and mesoscale condensed-phase systems, and the optimal fabrication design for homogeneous and heterogeneous optoelectronic devices.

Scalable Approach to High Coverages on Oxides via Iterative Training of a Machine-Learning Algorithm

2019 ◽  
Author(s):  
Andrew Medford ◽  
Shengchun Yang ◽  
Fuzhu Liu
Keyword(s):  
Machine Learning ◽  
Chemical Potential ◽  
Learning Algorithm ◽  
Absolute Error ◽  
Low Energy ◽  
Training Data ◽  
High Coverage ◽  
Metal Compounds ◽  
Adsorption Energies ◽  
The Stability

Understanding the interaction of multiple types of adsorbate molecules on solid surfaces is crucial to establishing the stability of catalysts under various chemical environments. Computational studies on the high coverage and mixed coverages of reaction intermediates are still challenging, especially for transition-metal compounds. In this work, we present a framework to predict differential adsorption energies and identify low-energy structures under high- and mixed-adsorbate coverages on oxide materials. The approach uses Gaussian process machine-learning models with quantified uncertainty in conjunction with an iterative training algorithm to actively identify the training set. The framework is demonstrated for the mixed adsorption of CH<sub>x</sub>, NH<sub>x</sub> and OH<sub>x</sub> species on the oxygen vacancy and pristine rutile TiO<sub>2</sub>(110) surface sites. The results indicate that the proposed algorithm is highly efficient at identifying the most valuable training data, and is able to predict differential adsorption energies with a mean absolute error of ~0.3 eV based on <25% of the total DFT data. The algorithm is also used to identify 76% of the low-energy structures based on <30% of the total DFT data, enabling construction of surface phase diagrams that account for high and mixed coverage as a function of the chemical potential of C, H, O, and N. Furthermore, the computational scaling indicates the algorithm scales nearly linearly (N<sup>1.12</sup>) as the number of adsorbates increases. This framework can be directly extended to metals, metal oxides, and other materials, providing a practical route toward the investigation of the behavior of catalysts under high-coverage conditions.

Understanding Conformational Entropy in Small Molecules

2020 ◽  
Author(s):  
Lucian Chan ◽  
Garrett Morris ◽  
Geoffrey Hutchison
Keyword(s):  
Small Molecules ◽  
Degrees Of Freedom ◽  
Absolute Error ◽  
Low Energy ◽  
Standard Entropy ◽  
Free Energies ◽  
Conformational Entropy ◽  
Wide Range ◽  
High Degree ◽  
Empirical Corrections

The calculation of the entropy of flexible molecules can be challenging, since the number of possible conformers grows exponentially with molecule size and many low-energy conformers may be thermally accessible. Different methods have been proposed to approximate the contribution of conformational entropy to the molecular standard entropy, including performing thermochemistry calculations with all possible stable conformations, and developing empirical corrections from experimental data. We have performed conformer sampling on over 120,000 small molecules generating some 12 million conformers, to develop models to predict conformational entropy across a wide range of molecules. Using insight into the nature of conformational disorder, our cross-validated physically-motivated statistical model can outperform common machine learning and deep learning methods, with a mean absolute error ≈4.8 J/mol•K, or under 0.4 kcal/mol at 300 K. Beyond predicting molecular entropies and free energies, the model implies a high degree of correlation between torsions in most molecules, often as- sumed to be independent. While individual dihedral rotations may have low energetic barriers, the shape and chemical functionality of most molecules necessarily correlate their torsional degrees of freedom, and hence restrict the number of low-energy conformations immensely. Our simple models capture these correlations, and advance our understanding of small molecule conformational entropy.

Nanosecond Photodynamics Simulations of a Cis-Trans Isomerization Are Enabled by Machine Learning

2020 ◽  
Author(s):  
Jingbai Li ◽  
Patrick Reiser ◽  
André Eberhard ◽  
Pascal Friederich ◽  
Steven Lopez
Keyword(s):  
Machine Learning ◽  
Neural Networks ◽  
Excited State ◽  
Adaptive Sampling ◽  
Computational Cost ◽  
Ground Truth ◽  
Absolute Error ◽  
Photochemical Reactions ◽  
Computational Techniques ◽  
Full Potential

<p>Photochemical reactions are being increasingly used to construct complex molecular architectures with mild and straightforward reaction conditions. Computational techniques are increasingly important to understand the reactivities and chemoselectivities of photochemical isomerization reactions because they offer molecular bonding information along the excited-state(s) of photodynamics. These photodynamics simulations are resource-intensive and are typically limited to 1–10 picoseconds and 1,000 trajectories due to high computational cost. Most organic photochemical reactions have excited-state lifetimes exceeding 1 picosecond, which places them outside possible computational studies. Westermeyr <i>et al.</i> demonstrated that a machine learning approach could significantly lengthen photodynamics simulation times for a model system, methylenimmonium cation (CH<sub>2</sub>NH<sub>2</sub><sup>+</sup>).</p><p>We have developed a Python-based code, Python Rapid Artificial Intelligence <i>Ab Initio</i> Molecular Dynamics (PyRAI<sup>2</sup>MD), to accomplish the unprecedented 10 ns <i>cis-trans</i> photodynamics of <i>trans</i>-hexafluoro-2-butene (CF<sub>3</sub>–CH=CH–CF<sub>3</sub>) in 3.5 days. The same simulation would take approximately 58 years with ground-truth multiconfigurational dynamics. We proposed an innovative scheme combining Wigner sampling, geometrical interpolations, and short-time quantum chemical trajectories to effectively sample the initial data, facilitating the adaptive sampling to generate an informative and data-efficient training set with 6,232 data points. Our neural networks achieved chemical accuracy (mean absolute error of 0.032 eV). Our 4,814 trajectories reproduced the S<sub>1</sub> half-life (60.5 fs), the photochemical product ratio (<i>trans</i>: <i>cis</i> = 2.3: 1), and autonomously discovered a pathway towards a carbene. The neural networks have also shown the capability of generalizing the full potential energy surface with chemically incomplete data (<i>trans</i> → <i>cis</i> but not <i>cis</i> → <i>trans</i> pathways) that may offer future automated photochemical reaction discoveries.</p>

Prediction of aircraft estimated time of arrival using machine learning methods

2021 ◽  
pp. 1-15
Author(s):  
O. Basturk ◽  
C. Cetek
Keyword(s):  
Machine Learning ◽  
Web Application ◽  
Absolute Error ◽  
Machine Learning Algorithms ◽  
Weather Data ◽  
Time Of Arrival ◽  
Learning Models ◽  
Trajectory Data ◽  
Different Sources ◽  
Machine Learning Models

ABSTRACT In this study, prediction of aircraft Estimated Time of Arrival (ETA) is proposed using machine learning algorithms. Accurate prediction of ETA is important for management of delay and air traffic flow, runway assignment, gate assignment, collaborative decision making (CDM), coordination of ground personnel and equipment, and optimisation of arrival sequence etc. Machine learning is able to learn from experience and make predictions with weak assumptions or no assumptions at all. In the proposed approach, general flight information, trajectory data and weather data were obtained from different sources in various formats. Raw data were converted to tidy data and inserted into a relational database. To obtain the features for training the machine learning models, the data were explored, cleaned and transformed into convenient features. New features were also derived from the available data. Random forests and deep neural networks were used to train the machine learning models. Both models can predict the ETA with a mean absolute error (MAE) less than 6min after departure, and less than 3min after terminal manoeuvring area (TMA) entrance. Additionally, a web application was developed to dynamically predict the ETA using proposed models.

scholarly journals Non-invasive cuff-less blood pressure estimation using a hybrid deep learning model

2021 ◽  
Vol 53 (2) ◽  
Author(s):  
Sen Yang ◽  
Yaping Zhang ◽  
Siu-Yeung Cho ◽  
Ricardo Correia ◽  
Stephen P. Morgan
Keyword(s):  
Machine Learning ◽  
Blood Pressure ◽  
Deep Learning ◽  
Absolute Error ◽  
Learning Model ◽  
Physiological Measurement ◽  
British Hypertension Society ◽  
Non Invasive ◽  
Blood Pressure Estimation ◽  
Deep Learning Model

AbstractConventional blood pressure (BP) measurement methods have different drawbacks such as being invasive, cuff-based or requiring manual operations. There is significant interest in the development of non-invasive, cuff-less and continual BP measurement based on physiological measurement. However, in these methods, extracting features from signals is challenging in the presence of noise or signal distortion. When using machine learning, errors in feature extraction result in errors in BP estimation, therefore, this study explores the use of raw signals as a direct input to a deep learning model. To enable comparison with the traditional machine learning models which use features from the photoplethysmogram and electrocardiogram, a hybrid deep learning model that utilises both raw signals and physical characteristics (age, height, weight and gender) is developed. This hybrid model performs best in terms of both diastolic BP (DBP) and systolic BP (SBP) with the mean absolute error being 3.23 ± 4.75 mmHg and 4.43 ± 6.09 mmHg respectively. DBP and SBP meet the Grade A and Grade B performance requirements of the British Hypertension Society respectively.

scholarly journals Detection and Severity Evaluation of Combined Rail Defects Using Deep Learning

Vibration ◽  
2021 ◽  
Vol 4 (2) ◽  
pp. 341-356
Author(s):  
Jessada Sresakoolchai ◽  
Sakdirat Kaewunruen
Keyword(s):  
Neural Network ◽  
Machine Learning ◽  
Deep Learning ◽  
Mean Absolute Error ◽  
Absolute Error ◽  
Machine Learning Techniques ◽  
Rolling Stock ◽  
Raw Data ◽  
Learning Techniques ◽  
Combined Defects

Various techniques have been developed to detect railway defects. One of the popular techniques is machine learning. This unprecedented study applies deep learning, which is a branch of machine learning techniques, to detect and evaluate the severity of rail combined defects. The combined defects in the study are settlement and dipped joint. Features used to detect and evaluate the severity of combined defects are axle box accelerations simulated using a verified rolling stock dynamic behavior simulation called D-Track. A total of 1650 simulations are run to generate numerical data. Deep learning techniques used in the study are deep neural network (DNN), convolutional neural network (CNN), and recurrent neural network (RNN). Simulated data are used in two ways: simplified data and raw data. Simplified data are used to develop the DNN model, while raw data are used to develop the CNN and RNN model. For simplified data, features are extracted from raw data, which are the weight of rolling stock, the speed of rolling stock, and three peak and bottom accelerations from two wheels of rolling stock. In total, there are 14 features used as simplified data for developing the DNN model. For raw data, time-domain accelerations are used directly to develop the CNN and RNN models without processing and data extraction. Hyperparameter tuning is performed to ensure that the performance of each model is optimized. Grid search is used for performing hyperparameter tuning. To detect the combined defects, the study proposes two approaches. The first approach uses one model to detect settlement and dipped joint, and the second approach uses two models to detect settlement and dipped joint separately. The results show that the CNN models of both approaches provide the same accuracy of 99%, so one model is good enough to detect settlement and dipped joint. To evaluate the severity of the combined defects, the study applies classification and regression concepts. Classification is used to evaluate the severity by categorizing defects into light, medium, and severe classes, and regression is used to estimate the size of defects. From the study, the CNN model is suitable for evaluating dipped joint severity with an accuracy of 84% and mean absolute error (MAE) of 1.25 mm, and the RNN model is suitable for evaluating settlement severity with an accuracy of 99% and mean absolute error (MAE) of 1.58 mm.

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