Francisco M. Fernández
In this letter we analyse an amazing variational approach to chemical reactions. Our results clearly show that the variational expressions are unsuitable for the analysis of empirical data obtained from chemical reactions.
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We extend the energetic variational approach so it can be applied to a chemical reaction system with general mass action kinetics. Our approach starts with an energy-dissipation law. We show that the chemical equilibrium is determined by the choice of the free energy and the dynamics of the chemical reaction is determined by the choice of the dissipation. This approach enables us to couple chemical reactions with other effects, such as diffusion and drift in an electric field. As an illustration, we apply our approach to a non-equilibrium reaction-diffusion system in a specific but canonical s…
On the time scales accessible to atomistic numerical modelling, chemical reactions are considered rare events. Atomistic simulations are typically biased along a low-dimensional representation of a chemical reaction in an atomic structure space, i.e., along the collective variable, to accelerate sampling of these improbable events. However, suitable collective variables are often complicated to guess due to the complexity of the transitions. Therefore, we present an automatic method of generating robust collective variables from atomic representation vectors, using either fixed Behler-Parrinel…
A Primary Unified Geometric Framework of Molecular Reaction Dynamics Based on the Variational Principle
本文提出基于变分原理的分子反应动力学几何框架，通过几何相位自然引入，结合人工智能技术构建势能面，并统一电子结构与量子动力学的变分方法。
Theoretical analysis of chemical reactions using a variational quantum eigensolver method without specifying molecular charge
本文提出一种不预先指定分子电荷的变分量子本征求解器方法，以电子化学势为输入，通过巨势形式成本函数分析化学反应，并验证了其在给吸电子分子及铜基催化剂吸附氧化反应中的可行性。
Molecule- and particle-based simulations provide the tools to test, in microscopic detail, the validity of classical nucleation theory. In this endeavour, determining nucleation mechanisms and rates for phase separation requires an appropriately defined reaction coordinate to describe the transformation of an out-of-equilibrium parent phase, for which myriad options are available to the simulator. In this article, we describe the application of the variational approach to Markov processes (VAMP) to quantify the suitability of reaction coordinates to study crystallisation from supersaturated co…
Reaction-Level Consistency within the Variational Quantum Eigensolver: Homodesmotic Ring Strain Energies of Cyclic Hydrocarbons
本文通过同构反应方案计算环状烃类的环张力能，利用对称性指导的活性空间选择协议，确保反应层面的电子关联处理一致，结果与DFT和CCSD基准一致。
Approximate solutions of the chemical master equation and the chemical Fokker-Planck equation are an important tool in the analysis of biomolecular reaction networks. Previous studies have highlighted a number of problems with the moment-closure approach used to obtain such approximations, calling it an ad-hoc method. In this article, we give a new variational derivation of moment-closure equations which provides us with an intuitive understanding of their properties and failure modes and allows us to correct some of these problems. We use mixtures of product-Poisson distributions to obtain a …
Elucidating photochemical reactions is vital to understand various biochemical phenomena and develop functional materials such as artificial photosynthesis and organic solar cells, albeit its notorious difficulty by both experiments and theories. The best theoretical way so far to analyze photochemical reactions at the level of ab initio electronic structure is the state-averaged multi-configurational self-consistent field (SA-MCSCF) method. However, the exponential computational cost of classical computers with the increasing number of molecular orbitals hinders applications of SA-MCSCF for l…
The analysis of a chemical reaction along the ground state potential energy surface in conjunction with an unknown spin state is challenging because electronic states must be separately computed several times using different spin multiplicities to find the lowest energy state. However, in principle, the ground state could be obtained with just a single calculation using a quantum computer without specifying the spin multiplicity in advance. In the present work, ground state potential energy curves for PtCO were calculated as a proof-of-concept using a variational quantum eigensolver (VQE) algo…
Quantum Simulations of Chemical Reactions: Achieving Accuracy with NISQ Devices
本文提出利用不同活性空间研究化学反应，结合基态和激发态的不可约表示，通过VQE算法实现反应能量的高精度预测，误差小于1 kcal/mol。
Coupled Chemical Reactions: Effects of Electric Field, Diffusion and Boundary Control
本文基于能量变分方法建立电解质中耦合化学反应的数学模型，并扩展至开放系统，通过双域模型仿真揭示电势抑制氧化反应、加速还原反应，为理解线粒体ATP生成中的自调节与切换机制提供理论依据。
The variational quantum eigensolver self-consistent field method within a polarizable embedded framework
本文将可极化嵌入（PE）与变分量子本征求解器自洽场（VQE-SCF）结合，提出PE-VQE-SCF算法，在量子模拟器上验证其门数开销仅略有增加且散粒噪声不增加，并展示了其在真实化学反应建模中的应用潜力。
A mathematical model for chemical reactions in electrolytes is developed using an Energy variational method consistent with classical thermodynamics. Electrostatics and chemical reactions are included in properly defined energetic and dissipative functionals. The energy variation method is generalized to deal with open systems with inputs of charge, mass, and energy. The open systems can transform input energy of one type into output energy of another type. The generalized method is used to analyze the conversion of electrical current into proton flow by cytochrome c oxidase, an important enzy…
We study an approximation scheme based on a second quantization method for a chemical master equation. Small systems, such as cells, could not be studied by the traditional rate equation approach because fluctuation effects are very large in such small systems. Although a Fokker-Planck equation obtained by the system size expansion includes the fluctuation effects, it needs large computational costs for complicated chemical reaction systems. In addition, discrete characteristics of the original master equation are neglected in the system size expansion scheme. It has been shown that the usage …
Quantum chemistry calculations such as the prediction of molecular properties and modeling of chemical reactions are a few of the critical areas where near-term quantum computers can showcase quantum advantage. We present a method to calculate energy derivatives for both ground state and excited state energies with respect to the parameters of a chemical system based on the framework of the variational quantum eigensolver (VQE). A low-depth implementation of quantum circuits within the hybrid variational paradigm is designed, and their computational costs are analyzed. We showcase the effectiv…
A family of Variational Quantum Eigensolver (VQE) methods is designed to maximize the resource of existing noisy intermediate-scale quantum (NISQ) devices. However, VQE approaches encounter various difficulties in simulating molecules of industrially relevant sizes, among which the choice of the ansatz for the molecular wavefunction plays a crucial role. In this work, we push forward the capabilities of adaptive variational algorithms (ADAPT-VQE) by demonstrating that the measurement overhead can be significantly reduced via adding multiple operators at each step while keeping the ansatz compa…
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