Massive Parallelization of Exact Quantum Dynamics Calculations: Computing (ro)vibrational states for real molecular applications

德克萨斯理工大学的Lionel(Bill)Poirier获得了化学系理论、模型和计算方法计划颁发的奖项的支持，以开发和测试大规模并行的高性能计算代码，使精确的量子动力学(QD)振动光谱计算能够用于比目前可能的更大和更具挑战性的分子应用。该奖项是由保监处的一个试点计划共同资助的，该计划促进了数字基础设施(CI)元素的再利用。这种能力对于各种动力学、动力学和统计建模工作是有价值的，对这些工作来说，对所涉及的分子物种的振动状态和配分函数的准确知识通常是至关重要的。与以前的量子动力学研究相比，这项研究的一个新特点是使用了大规模并行化。许多必要的网络基础设施，即以前由国际和平协会开发的并行线性代数代码，已经到位。为了评估并行代码的性能、可扩展性和广泛的适用性，正在考虑两种极具挑战性但非常不同的基准分子应用，这两种应用都远远超出了当前技术水平的精确QD方法的能力。第一个是霓虹团簇中的异构化。第二种是丙二醛中的分子内氢原子转移，作为中间屏障酶催化质子转移的原型，以及更复杂的生物体系。建议的计算规模是可调整的，并将变化到PI可用的1000多个核心的化学计算集群(CCC)的最大容量。PI和他的研究小组正在投入大量精力，通过开发一个用户友好的“前端”，使他们的计算机代码和一般精确的量子动力学更容易被“非专家”使用。他们还在德克萨斯理工大学(TTU)化学和生物化学部为TTU、地区和其他用户举办培训研讨会。并行二维码正在通过协调中心进行更新和分发。这些软件工具极大地扩展了可以动态研究量子的系统的复杂性，同时使更广泛的化学动力学社区能够自己执行此类计算。

Lionel (Bill) Poirier of Texas Tech University is supported by an award from the Theory, Models and Computational Methods program in the Chemistry division to develop and test massively parallel high performance computing codes that enable exact quantum dynamics (QD) rovibrational spectroscopy calculations for larger and more challenging molecular applications than are currently possible. The award is co-funded by a pilot program in OCI promoting the reuse of Cyberinfrastructure (CI) elements. This capability is valuable for various dynamical, kinetic, and statistical modeling endeavors, for which accurate knowledge of rovibrational states and partition function of the molecular species involved is often vitally important. A novel feature of this research over previous quantum dynamics efforts is use of massive parallelization. Much of the requisite cyberinfrastructure, i.e., parallel linear algebra codes, developed by the PI previously, is already in place. To assess the performance, scalability, and broad applicability of the parallel codes, two extremely challenging, but very different, benchmark molecular applications are being considered, both well beyond the capabilities of the current state of the art in exact QD methods. The first is isomerization in neon clusters. The second is intramolecular hydrogen atom transfer in malonaldehyde, as a prototype for proton transfer in intermediate-barrier enzyme catalysis, and more complex biological systems. The scale of the proposed calculations is designed to be adjustable, and will be varied up to the maximum capacity of the 1000-plus-core Chemistry Computation Cluster (CCC) available to the PI. The PI and his research group are devoting much effort to make their computer codes, and exact quantum dynamics in general, easier for "non experts" to use, by developing a user-friendly "front end". They are also hosting training workshop at the Texas Tech (TTU) Department of Chemistry and Biochemistry, for TTU, regional and other users. The parallelQD codes are being updated and disseminated through the CCC. These software tools greatly extend the complexity of systems that can be studied quantum dynamically, while simultaneously cyber-enabling a broader cross section of the chemical dynamics community to perform such calculations on their own.