A simplified ab initio treatment of diradicaloid structures produced from stretching and breaking chemical bonds

2017 ◽  
Vol 19 (33) ◽  
pp. 22282-22301 ◽  
Author(s):  
Suvonil Sinha Ray ◽  
Anirban Ghosh ◽  
Anindita Shit ◽  
Rajat K. Chaudhuri ◽  
Sudip Chattopadhyay
Keyword(s):  
Perturbation Theory ◽  
Ab Initio ◽  
Computational Cost ◽  
Proper Choice ◽  
Chemical Bonds ◽  
Single Root ◽  
Low Computational Cost ◽  
Virtual Orbitals

With a proper choice of active spaces, the single root perturbation theory employing improved virtual orbitals can flawlessly describe the ground, excited, ionized, and dissociated states having varying degrees of degeneracy at the expense of low computational cost.

Active Learning Accelerates Ab Initio Molecular Dynamics on Pericyclic Reactive Energy Surfaces

2020 ◽  
Author(s):  
Shi Jun Ang ◽  
Wujie Wang ◽  
Daniel Schwalbe-Koda ◽  
Simon Axelrod ◽  
Rafael Gomez-Bombarelli
Keyword(s):  
Molecular Dynamics ◽  
Potential Energy ◽  
Transition State ◽  
Potential Energy Surface ◽  
Ab Initio ◽  
Energy Surface ◽  
Computational Cost ◽  
Reactive Trajectories ◽  
Dynamics Simulations ◽  
Energy Surfaces

<div>Modeling dynamical effects in chemical reactions, such as post-transition state bifurcation, requires <i>ab initio</i> molecular dynamics simulations due to the breakdown of simpler static models like transition state theory. However, these simulations tend to be restricted to lower-accuracy electronic structure methods and scarce sampling because of their high computational cost. Here, we report the use of statistical learning to accelerate reactive molecular dynamics simulations by combining high-throughput ab initio calculations, graph-convolution interatomic potentials and active learning. This pipeline was demonstrated on an ambimodal trispericyclic reaction involving 8,8-dicyanoheptafulvene and 6,6-dimethylfulvene. With a dataset size of approximately</div><div>31,000 M062X/def2-SVP quantum mechanical calculations, the computational cost of exploring the reactive potential energy surface was reduced by an order of magnitude. Thousands of virtually costless picosecond-long reactive trajectories suggest that post-transition state bifurcation plays a minor role for the reaction in vacuum. Furthermore, a transfer-learning strategy effectively upgraded the potential energy surface to higher</div><div>levels of theory ((SMD-)M06-2X/def2-TZVPD in vacuum and three other solvents, as well as the more accurate DLPNO-DSD-PBEP86 D3BJ/def2-TZVPD) using about 10% additional calculations for each surface. Since the larger basis set and the dynamic correlation capture intramolecular non-covalent interactions more accurately, they uncover longer lifetimes for the charge-separated intermediate on the more accurate potential energy surfaces. The character of the intermediate switches from entropic to thermodynamic upon including implicit solvation effects, with lifetimes increasing with solvent polarity. Analysis of 2,000 reactive trajectories on the chloroform PES shows a qualitative agreement with the experimentally-reported periselectivity for this reaction. This overall approach is broadly applicable and opens a door to the study of dynamical effects in larger, previously-intractable reactive systems.</div>

scholarly journals Computing Expectiles Using k-Nearest Neighbours Approach

Symmetry ◽  
2021 ◽  
Vol 13 (4) ◽  
pp. 645
Author(s):  
Muhammad Farooq ◽  
Sehrish Sarfraz ◽  
Christophe Chesneau ◽  
Mahmood Ul Hassan ◽  
Muhammad Ali Raza ◽  
...  
Keyword(s):  
Computational Cost ◽  
Real Life ◽  
Distance Measures ◽  
Computational Time ◽  
High Dimensional ◽  
Test Error ◽  
Nearest Neighbours ◽  
Comparable Performance ◽  
Asymmetric Least Squares ◽  
Low Computational Cost

Expectiles have gained considerable attention in recent years due to wide applications in many areas. In this study, the k-nearest neighbours approach, together with the asymmetric least squares loss function, called ex-kNN, is proposed for computing expectiles. Firstly, the effect of various distance measures on ex-kNN in terms of test error and computational time is evaluated. It is found that Canberra, Lorentzian, and Soergel distance measures lead to minimum test error, whereas Euclidean, Canberra, and Average of (L1,L∞) lead to a low computational cost. Secondly, the performance of ex-kNN is compared with existing packages er-boost and ex-svm for computing expectiles that are based on nine real life examples. Depending on the nature of data, the ex-kNN showed two to 10 times better performance than er-boost and comparable performance with ex-svm regarding test error. Computationally, the ex-kNN is found two to five times faster than ex-svm and much faster than er-boost, particularly, in the case of high dimensional data.

scholarly journals Directional TGV-Based Image Restoration under Poisson Noise

2021 ◽  
Vol 7 (6) ◽  
pp. 99
Author(s):  
Daniela di Serafino ◽  
Germana Landi ◽  
Marco Viola
Keyword(s):  
Computed Tomography ◽  
Image Restoration ◽  
Gaussian Noise ◽  
Computational Cost ◽  
Data Fitting ◽  
Poisson Noise ◽  
Glass Fibres ◽  
Leibler Divergence ◽  
Generalized Variation ◽  
Low Computational Cost

We are interested in the restoration of noisy and blurry images where the texture mainly follows a single direction (i.e., directional images). Problems of this type arise, for example, in microscopy or computed tomography for carbon or glass fibres. In order to deal with these problems, the Directional Total Generalized Variation (DTGV) was developed by Kongskov et al. in 2017 and 2019, in the case of impulse and Gaussian noise. In this article we focus on images corrupted by Poisson noise, extending the DTGV regularization to image restoration models where the data fitting term is the generalized Kullback–Leibler divergence. We also propose a technique for the identification of the main texture direction, which improves upon the techniques used in the aforementioned work about DTGV. We solve the problem by an ADMM algorithm with proven convergence and subproblems that can be solved exactly at a low computational cost. Numerical results on both phantom and real images demonstrate the effectiveness of our approach.

scholarly journals An optimal and low computational cost fractional Newton-type method for solving nonlinear equations

2021 ◽  
pp. 107650
Author(s):  
Giro Candelario ◽  
Alicia Cordero ◽  
Juan R. Torregrosa ◽  
María P. Vassileva
Keyword(s):  
Nonlinear Equations ◽  
Computational Cost ◽  
Type Method ◽  
Low Computational Cost

Low-Computational Cost Estimation Algorithm for Adaptive Optics Systems*

2011 ◽  
Vol 44 (1) ◽  
pp. 5573-5578
Author(s):  
M. Abbas Turki ◽  
D. Esqueda Merino ◽  
K. Kasper ◽  
C. Durieu
Keyword(s):  
Adaptive Optics ◽  
Cost Estimation ◽  
Computational Cost ◽  
Estimation Algorithm ◽  
Low Computational Cost

scholarly journals Status Estimation and In-Process Connection of Kanbans Using BLE Beacons and LPWA Network to Implement Intra-Traceability for the Kanban System

Sensors ◽  
2021 ◽  
Vol 21 (15) ◽  
pp. 5038
Author(s):  
Kosuke Shima ◽  
Masahiro Yamaguchi ◽  
Takumi Yoshida ◽  
Takanobu Otsuka
Keyword(s):  
Inventory Management ◽  
Low Cost ◽  
Computational Cost ◽  
Low Energy ◽  
Manufacturing Strategy ◽  
Implementation Cost ◽  
Measurement Systems ◽  
Process Route ◽  
Kanban System ◽  
Low Computational Cost

IoT-based measurement systems for manufacturing have been widely implemented. As components that can be implemented at low cost, BLE beacons have been used in several systems developed in previous research. In this work, we focus on the Kanban system, which is a measure used in manufacturing strategy. The Kanban system emphasizes inventory management and is used to produce only required amounts. In the Kanban system, the Kanban cards are rotated through the factory along with the products, and when the products change to a different process route, the Kanban card is removed from the products and the products are assigned to another Kanban. For this reason, a single Kanban cannot trace products from plan to completion. In this work, we propose a system that uses a Bluetooth low energy (BLE) beacon to connect Kanbans in different routes but assigned to the same products. The proposed method estimates the beacon status of whether the Kanban is inside or outside a postbox, which can then be computed by a micro controller at low computational cost. In addition, the system connects the Kanbans using the beacons as paired connection targets. In an experiment, we confirmed that the system connected 70% of the beacons accurately. We also confirmed that the system could connect the Kanbans at a small implementation cost.

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