光化学与光电转化器件中的量子效应和热力学特性研究

Designing artificial photochemical and photoelectric converters based on the quantum mechanisms and fundamental principles of thermodynamics in photosynthesis will efficiently improve the development and utilization of solar energy. In this project, based on some novel physical phenomena such as the quantum coherence and nonlinear thermal rectifying behaviors generated by the non-equilibrium nanoelectronic systems, dipole-dipole interaction between organic molecules, spin-boson coupling between the three-level system and the phonon thermal bath, and collective excitation of light-harvesting antennas with cyclic structures, we will establish several new types of photochemical and photoelectric devices. These studies will combine with the theories of open quantum systems, quantum optics, and quantum thermodynamics, and consider the microscopic explanations of the irreversible processes. The power output will be accurately defined by relying on the energy transfer within the composite system and the thermodynamic entropy. The techniques for reducing the electron spontaneous emission and the irreversible entropy production arising from the electron transport will be searched. The influences of the system-environment coupling strength, multi-level structures, ambient temperatures, and chemical potentials on the thermodynamic performances of the system will be discussed. In addition, the intermediate band, upconversion, and downconversion materials will be proposed to achieve photochemical and photoelectric conversions by capturing solar energy with wider spectral range. The optimal parameter values will be obtained through the optimization of coherent control. The results will provide guidance for developing new micro energy harvesting devices.

基于光合作用中的量子机制和热力学基本规律，设计具有光化学和光电转换性能的器件，将促进太阳能的高效开发与利用。本项目基于纳米电子系统的非平衡特性、有机分子间的偶极-偶极相互作用、三能级与声子热库的自旋玻色耦合、环状人工光吸收作用体的集体激发等物理现象，建立具有量子相干效应和非线性热整流特性的光化学与光电转化器件。研究将结合开放量子系统、量子光学和量子热力学基本理论，探索不可逆过程的微观机理。根据复合系统内部的能量转移和热力学熵重新定义功率输出，探索如何有效抑制器件中电子自发辐射复合损失和电子转移过程中的不可逆熵增，获得系统-环境耦合强度、多能级结构、环境温度和化学势等因素对器件热力学性能的影响。此外，利用中间带、上转换和下转换材料的新构型，实现多光谱太阳能光化学与光电转换。进一步改进完善新模型，通过量子相干优化调控，确定各参数的最佳合理范围，为新型微纳能量转换器件的设计与开发提供有益指导。

基于光合作用中的量子机制和热力学基本规律，设计具有光化学和光电转换性能的器件，有望促进太阳能的高效开发与利用。本项目基于纳米电子系统的非平衡特性、有机分子间的偶极-偶极相互作用和三能级与声子热库的自旋玻色耦合等物理现象，建立了具有量子相干效应和非线性热整流特性的光化学与光电转化器件。结合开放量子系统、量子光学和量子热力学基本理论，探讨了器件中不可逆过程的微观机理。根据复合系统内部的能量转移和热力学熵准确定义了功率输出，从而揭示了量子效应如何有效抑制器件中电子自发辐射复合损失和电子转移过程中的不可逆熵增，获得了系统-环境耦合强度、多能级结构、环境温度和化学势等因素对器件热力学性能的影响。通过量子相干优化调控，确定了各参数的最佳合理范围。此外，研究还建立了一些有创新性的理论模型，例如近场热辐射光电系统，中间带热辐射电池，三能级热整流器，量子测量热机，量子点热电器件。这些研究促进了新型微纳能量转换器件的开发与应用。