Energy harvesting at the nanoscale: From principles to functions

我们计划的目标是建立模型，开发理论方法和计算实现，建议新的功能，并优化在纳米级运行的能量转换系统的性能。令人感兴趣的换能器是光伏电池、热电结和热机，如热泵和冰箱，由单分子、量子点、薄膜、有机异质结等物理化学成分制成。我们的计划是使用简单的模型，重点研究这些系统中电荷和能量载流子的动力学，并询问量子效应对传输率、损耗过程、涨落、电流以及功率输出和效率的作用。感兴趣的系统的一个中心方面是，参与粒子的动力学，从而产生的操作，强烈地受到电子和非电子自由度之间的相互作用的影响，后者包括分子的核运动、辐射场和其他集体激发。我们工作的另一个重要方面是，它本质上与传统热力学的设置不同，因为量子效应和操作系统与其热环境之间的强烈相互作用可能控制着动力学。 我们的计划将由三个相互关联的部分组成： (I)方法发展：我们将提出各种原创的理论和计算方法、数值精确路径积分方法、近似方法和唯象处理方法，来描述复杂环境中相互作用系统的量子动力学。我们将专门采用这些技术来研究分子机器典型模型中的电荷、能量和自旋转移过程。 (Ii)量子热力学：我们将通过研究量子热机的最小设计，从量子原理出发探索宏观热力学的出现。 (3)能量收集系统：利用开发的模型、定义以及理论和计算工具，我们将模拟能量转换过程，特别是实际的纳米系统。具体地说，我们将研究热电和光伏系统，并探索有望改善运营的概念。 我们的工作将对分子系统、电子和热设备的组件中的电荷和能量转移过程提供基本和实用的见解。此外，所开发的方法也可以用于描述量子信息技术中溶液中化学反应和退相干效应的核心过程。拟议的研究计划将通过开发处理复杂系统中的量子多体效应的第一原理方法来促进知识的进步，并通过为纳米级能量转换系统提出新的设计来促进新兴技术。

The objectives of our program is to build models, develop theoretical methodologies and computational implementations, suggest new functions, and optimize performance of energy conversion systems operating at the nanoscale. Transducers of interest are photovoltaic cells, thermoelectric junctions, and heat engines such as heat pumps and refrigerators, made from physical-chemical components such as single molecules, quantum dots, thin films, organic hetero-junctions. Using simple models, our plan is to focus on the dynamics of charge and energy carriers in these systems, and interrogate the role of quantum effects on transfer rates, loss processes, fluctuations, currents, and power output and efficiency. A central aspect of systems of interest is that the dynamics of participating particles, thus the resulting operation, is strongly affected by the interaction between electronic and nonelectronic degrees of freedom, the latter comprising nuclear motion of molecules, radiation fields, and other collective excitations. Another nontrivial aspect of our work is that it inherently departs from the setting of traditional thermodynamics since quantum effects and strong interactions between the operating system and its thermal environment may govern the dynamics. Our program will constitute three interrelated parts: (i) Method development: We will advance various original theoretical and computational methodologies, numerically exact path integral methods, approximate approaches, and phenomenological treatments, to describe quantum dynamics of interacting systems in complex environments. We will specifically adapt these techniques to study charge, energy and spin transfer processes in representative models for molecular-based machines. (ii) Quantum thermodynamics: We will probe the emergence of macroscopic thermodynamics from quantum principles by studying minimal designs of quantum heat engines. (iii) Energy harvesting systems: Using the developed models, definitions, and theoretical and computational tools, we will simulate energy conversion processes in particular-factual nano-systems. Specifically, we will study thermoelectric and photovoltaic systems, and probe concepts of promise for an improved operation. Our work will contribute fundamental and practical insights over charge and energy transfer processes in molecular systems, components of electronic and thermal devices. As well, developed methods could be applied to describe processes at the core of chemical reactivity in solution and decoherence effects in quantum information technologies. The proposed research program will contribute to the advancement of knowledge, with the development of first-principle approaches for treating quantum many-body effects in complex systems, and to emerging technologies, by suggesting novel designs for nanoscale energy conversion systems.