EAGER: CDS&E: An Open-Source Software Package for Assessing and Controlling Photocatalytic Reactions

光催化是捕捉太阳光并利用其为催化材料加速的化学反应提供能量的过程。一个好的光催化体系不仅能有效地吸收光，还能有效地利用光生电子来促进催化反应。光和化学/材料系统之间的相互作用使许多光催化应用成为可能，所有这些都有助于可再生能源，可用于太阳能发电、环境修复和化学制造等各种应用。随着我们对发生在这些系统中的光引发过程的进一步了解，充分利用这些光催化系统的能力具有巨大的潜力。光催化过程背后的物理和化学基础极其复杂。近年来，利用预测量子力学技术计算和理解光催化过程的效率的计算技术的发展，为识别新的捕光和光催化材料提供了反复尝试的方法。该项目将进一步推动这些技术的发展，并为普通催化界评估光催化过程的效率提供一个新的、开放源代码的软件包。完全开放源代码和计算能力的可获得性鼓励世界各地的学生和研究人员更深入地了解如何使用这些方法和工具来评估光催化效率，并加速发现新的光催化材料和操作条件。本项目将利用激发态量子计算方法来探索光催化体系中的电子动力学。本项目中使用的激发态计算方法将与量子控制算法相结合，最终操纵光诱导反应动力学。通过提供一种明确的方法来控制反应动力学，量子控制方法在光催化系统中的使用将在多个化学工程领域产生开创性的影响。具体地说，这些计算技术将给出导致所需反应产物的光的波长/频率的严格界限。因此，在这个热切项目中开发的软件工具既可以用作(1)诊断工具，以验证光催化实验中确实使用了正确的光频率，也可以用作(2)计算控制光催化系统所需的允许光频率的预测工具(可以通过计算或实验获得数据集)。因此，这些计算方法为交叉研究开辟了新的途径，为操纵电子动力学和理解光催化系统中可能的最佳效率建立了严格的形式主义。最后，该项目的更广泛影响将导致一套开放源码的工具，CBET和催化社区的计算和实验研究人员都可以很容易地将其用于未来的开发。在该项目中开发的完全开放源代码的可用性鼓励世界各地的研究人员获得详细的“幕后调查”，以更深入地了解这些算法是如何在实践中以数字方式并入的。这一奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

Photocatalysis is the process by which sunlight is captured and used to provide energy for chemical reactions accelerated by catalytic materials. A good photocatalytic system is one which absorbs light efficiently, and also efficiently uses the photo-generated electrons to promote catalytic reactions. The interaction between light and chemical/material systems enables numerous photocatalytic applications, all of which contribute to renewable energy that can be used for applications as diverse as solar fuel generation, environmental remediation, and chemical manufacturing. The capability to fully harness these photocatalytic systems has tremendous potential to grow as we further our understanding of the light-initiated processes that occur in these systems. The physics and chemistry underlying photocatalytic processes are extremely complicated. Trial-and-error approaches to identifying new light-harvesting and photocatalytic materials have been aided in recent years by the development of computational techniques to calculate and understand the efficiency of photocatalytic processes using predictive quantum mechanical techniques. This project will further advance those techniques and provide a new, open-source software package for the general catalysis community to assess the efficiency of photocatalytic processes. The availability of fully open-source codes and computational capability encourages both students and researchers worldwide to obtain a deeper understanding of how these approaches and tools can be used to assess photocatalytic efficiencies and hasten the discovery of new photocatalytic materials and operating conditions.This project will utilize excited-state quantum computational methods to probe the electron dynamics in photocatalytic systems. The excited-state computational approaches used in this project will be coupled with quantum control algorithms to ultimately manipulate photo-induced reaction dynamics. The use of quantum control approaches in photocatalytic systems will have ground-breaking implications across multiple chemical engineering domains by providing a defined way to control reaction dynamics. Specifically, these computational techniques will give rigorous bounds on the wavelengths/frequencies of light that will lead to the desired reaction products. As such, the software tool developed in this EAGER project can serve as both (1) a diagnostic tool to verify that the correct frequency of light is indeed being used as intended in a photocatalysis experiment, as well as (2) a predictive tool for calculating the allowed frequencies of light required to control photocatalytic systems (which may be obtained as data sets obtained from calculation or experiment). Consequently, these computational methods open new avenues of cross-cutting research by establishing a rigorous formalism for manipulating the electron dynamics and understanding the optimal efficiencies that are possible in photocatalytic systems. Finally, the broader impacts of this project will result in an open-source suite of tools that both computational and experimental researchers in the CBET and catalysis communities can easily use for future development. The availability of the fully open-source codes developed in this project encourages researchers worldwide to get a detailed "look under the hood" to obtain a deeper understanding of how these algorithms are numerically incorporated in practice.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.