Gelbwaser-Klimovsky David, Aspuru-Guzik Alán
Department of Chemistry and Chemical Biology , Cambridge , MA 02138 , USA . Email:
Chem Sci. 2017 Feb 1;8(2):1008-1014. doi: 10.1039/c6sc04350j. Epub 2016 Oct 26.
We analyze standard theoretical models of solar energy conversion developed to study solar cells and photosynthetic systems. We show that assuming the energy transfer to the reaction center/electric circuit is through a decay rate or "sink", contradicts the second law of thermodynamics. We put forward a thermodynamically consistent alternative by explicitly considering parts of the reaction center/electric circuit and by employing a Hamiltonian transfer. The predicted energy transfer by the new scheme differs from the one found using a decay rate, casting doubts on the validity of the conclusions obtained by models which include the latter.
我们分析了为研究太阳能电池和光合系统而开发的太阳能转换标准理论模型。我们表明，假设能量通过衰减率或“汇”转移到反应中心/电路，这与热力学第二定律相矛盾。我们通过明确考虑反应中心/电路的各个部分并采用哈密顿转移，提出了一种热力学上一致的替代方案。新方案预测的能量转移与使用衰减率得出的结果不同，这使人对包含后者的模型所得出结论的有效性产生怀疑。
