A Universal Approach for Solving Real-World Problems Using Quantum Dynamics: Coherent States for Molecular Simulations (COSMOS)

使用现代激光技术和新光源的实验着眼于经历动态变化的量子系统，以了解分子功能并回答与化学、材料和量子技术相关的基本问题。典型的问题是：在能量收集、紫外线防护或光催化过程中，如何设计分子以实现最大效率？当强而快速变化的激光场作用于原子和分子中的电子时，会发生什么？由于与环境的相互作用，量子比特丢失信息的速度有多快？未来量子计算机中的一组相互作用的量子比特是否会在长时间尺度上保持稳定？为了解释旨在回答这些问题的时间分辨实验，需要量子动力学(QD)模拟，即量子运动理论。QD即将能够对大分子系统做出定量预测，通过求解依赖于时间的薛定谔方程，将有助于解开来自最先进实验的复杂信号，并提供量子过程的机械细节。然而，重要的方法挑战仍然存在，例如计算费用和实验观测的准确预测，需要团队协调一致的努力。解决这些问题将极大地惠及更广泛的实验和计算QD社区。在这项计划拨款中，我们将开发变革性的新QD模拟策略，这些策略将独特地为一系列技术和生物领域的现实世界应用提供影响和洞察力。我们愿景的关键是开发、传播和广泛适应用于量子点模拟的强大的新的通用软件，建立在我们利用轨迹制导的基函数的量子点方法的集体工作的基础上。然而，目前的能力受到学术软件开发通常分散的方法的阻碍。这种缺乏统一性使得很难使用一个小组的想法来改进另一个小组的方法，即使是简单的QD模拟方法的比较也不是微不足道的。在这里，我们将把广泛的现有方法组合成一个统一的代码，适合于计算和实验研究人员使用，以模拟基本的光激发分子行为并解释最先进的实验。重要的是，我们将在这套软件中开发和实施新的数学和数值思想，明确的目标是推动系统大小和时间尺度的限制，使之超出目前“标准”量子点模拟所能达到的范围。我们的统一代码将带来强大而可靠的QD方法，同时使非专业人员能够轻松采用；第一次，开发和使用QD模拟的科学家将能够访问、开发和部署通用软件框架，消除了当前QD领域利基软件设置中存在的许多社区间和社区内的障碍。电子结构和经典分子动力学软件包有力地说明了方法开发和代码集成的变革性影响，这些软件包经常被世界各地的数千名研究人员使用，并在过去几十年里获得了几个诺贝尔奖的认可。我们的计划拨款旨在通过改善QD模拟的可及性来实现类似的步骤变化。我们计划赠款的成功将是在广泛的最终用户群体(例如光谱学、材料科学家、分子设计师)中采用先进的量子点模拟的明显增加。此外，通过支持大量但集成的早期职业研究人员，这项计划拨款将极大地加速QD的发展，在我们从经典计算和模拟时代进入未来几十年的量子时代之际，将英国定位为该领域的全球领先者。

Experiments using modern laser technologies and new light sources look at quantum systems undergoing dynamic change to understand molecular function and answer fundamental questions relevant to chemistry, materials and quantum technologies. Typical questions are: How can molecules be engineered for maximum efficiency during energy harvesting, UV protection or photocatalysis? What happens when strong and rapidly changing laser fields act on electrons in atoms and molecules? How fast do qubits lose information due to interactions with the environment? Will an array of interacting qubits in future quantum computers remain stable over long time-scales? Interpreting time-resolved experiments that aim to answer these questions requires Quantum Dynamics (QD) simulations, the theory of quantum motion. QD is on the cusp of being able to make quantitative predictions about large molecular systems, solving the time-dependent Schrödinger equation in a way that will help unravel the complicated signals from state-of-the-art experiments and provide mechanistic details of quantum processes. However, important methodological challenges remain, such as computational expense and accurate prediction of experimental observables, requiring a concerted team-effort. Addressing these will greatly benefit the wider experimental and computational QD communities.In this programme grant we will develop transformative new QD simulation strategies that will uniquely deliver impact and insight for real-world applications across a range of technological and biological domains. The key to our vision is the development, dissemination, and wide adaptation of powerful new universal software for QD simulations, building on our collective work on QD methods exploiting trajectory-guided basis functions. Present capability is, however, held back by the typically fragmented approach to academic software development. This lack of unification makes it difficult to use ideas from one group to improve the methods of another group, and even the simple comparison of QD simulation methods is non-trivial. Here, we will combine a wide range of existing methods into a unified code suitable for use by both computational and experimental researchers to model fundamental photo-excited molecular behaviour and interpret state-of-the-art experiments. Importantly we will develop and implement new mathematical and numerical ideas within this software suite, with the explicit objective of pushing the system-size and time-scale limits beyond what is currently accessible within "standard" QD simulations. Our unified code will lead to powerful and reliable QD methods, simultaneously enabling easy adoption by non-specialists; for the first time, scientists developing and using QD simulations will be able to access, develop and deploy a common software framework, removing many of the inter- and intra-community barriers that exist within the current niche software set-ups across the QD domain. The transformative impact of method development and code integration is powerfully illustrated by electronic structure and classical molecular dynamics packages, used routinely by thousands of researchers around the world and recognised by several Nobel Prizes in the last few decades. Our programme grant aims to deliver a similar step-change by improving accessibility for QD simulations. Success in our programme grant would be the demonstrated increase in adoption of advanced QD simulations across a broad range of end-user communities (e.g. spectroscopy, materials scientists, molecular designers). Furthermore, by supporting a large yet integrated cohort of early-career researchers, this programme grant will provide an enormous acceleration to developments in QD, positioning the UK as a global leader in this domain as we move from the era of classical computation and simulation into the quantum era of the coming decades.