Folescu Dan E, Onufriev Alexey V
Department of Computer Science, Virginia Tech, Blacksburg, Virginia 24061, United States.
Department of Physics, Virginia Tech, Blacksburg, Virginia 24061, United States.
ACS Omega. 2022 Jul 19;7(30):26123-26136. doi: 10.1021/acsomega.2c01484. eCollection 2022 Aug 2.
Closed-form, analytical approximations for electrostatic properties of molecules are of unique value as these can provide computational speed, versatility, and physical insight. Here, we have derived a simple, closed-form formula for the apparent surface charge (ASC) as well as for the electric field generated by a molecular charge distribution in aqueous solution. The approximation, with no fitted parameters, was tested against numerical solutions of the Poisson equation, where it has produced a significant speed-up. For neutral small molecules, the hydration free energies estimated from the closed-form ASC formula are within 0.8 kcal/mol RMSD from the numerical Poisson reference; the electric field at the surface is in quantitative agreement with the reference. Performance of the approximation was also tested on larger structures, including a protein, a DNA fragment, and a viral receptor-target complex. For all structures tested, a near-quantitative agreement with the numerical Poisson reference was achieved, except in regions of high negative curvature, where the new approximation is still qualitatively correct. A unique efficiency feature of the proposed "source-based″ closed-form approximation is that the ASC and electric field can be estimated individually at any point or surface patch, without the need to obtain the full global solution. An open-source software implementation of the method is available: https://people.cs.vt.edu/~onufriev/CODES/aasc.zip.
分子静电性质的闭式解析近似具有独特价值,因为它们能提供计算速度、通用性和物理洞察力。在此,我们推导了一个简单的闭式公式,用于计算水溶液中分子电荷分布产生的表观表面电荷(ASC)以及电场。该近似公式无拟合参数,已针对泊松方程的数值解进行了测试,结果显示其显著加快了计算速度。对于中性小分子,根据闭式ASC公式估算的水合自由能与数值泊松参考值的均方根偏差在0.8千卡/摩尔以内;表面电场与参考值在定量上一致。该近似公式在更大的结构上也进行了测试,包括蛋白质、DNA片段和病毒受体 - 靶标复合物。对于所有测试结构,除了在高负曲率区域新近似仍定性正确外,均与数值泊松参考值实现了近乎定量的一致。所提出的“基于源”的闭式近似的一个独特效率特性是,可以在任何点或表面补丁单独估计ASC和电场,而无需获得完整的全局解。该方法的开源软件实现可在以下网址获取:https://people.cs.vt.edu/~onufriev/CODES/aasc.zip。