Important Insight into Electron Transfer in Single-Molecule Junctions Based on Redox Metalloproteins from Transition Voltage Spectroscopy
Important Insight into Electron Transfer in Single-Molecule Junctions Based on Redox Metalloproteins from Transition Voltage Spectroscopy
复制标题
DOI：
10.1021/jp408873c
复制
发表时间：
2013-12-05
影响因子：
3.7
通讯作者：
Baldea, Joan
中科院分区：
文献类型：
--
作者：
Baldea, Joan
在最近的实验工作中，第一跃迁电压谱（TVS）的研究结果天青已报告。这形成了一个很好的案例，以更好地理解通过细菌氧化还原金属蛋白的电子转移，从化学，物理和生物学的角度来看，这是一个非常重要的过程，对纳米（生物）电子学具有实际意义。在本文中，我们挑战的尝试性的解释提出了上述实验研究，并提出了不同的理论解释。为了解释实验TVS数据，我们采用了一个扩展的Newns安德森框架，其准确性和鲁棒性的证明。我们表明，这个框架显然满足需要获得一致的描述跨实验。最重要的是，目前提出的理论方法允许解开的电化学扫描显微镜环境上的电荷传输通过单（生物）分子结的氧化还原单元的基础上的影响的新方面。TVS作为一种通用的调查方法，也能够提供重要的洞察力通过金属蛋白的电荷传输的有用性，强调。
In a recent experimental work, results of the first transition voltage spectroscopy (TVS) investigation on azurin have been reported. This forms a great case to better understand the electron transfer through bacterial redox metalloproteins, a process of fundamental importance from chemical, physical, and biological perspectives, and of practical importance for nano(bio)electronics. In the present paper we challenge the tentative interpretation put forward in the aforementioned experimental study and propose a different theoretical interpretation. To explain the experimental TVS data, we adopt an extended Newns Anderson framework, whose accuracy and robustness is demonstrated. We show that that this framework clearly meets the need to obtain a consistent description across experiments. Most importantly, the presently proposed theoretical approach permits unraveling novel aspects on the impact of the electrochemical scanning microscope environment on the charge transport through single(bio)molecule junctions based on redox units. The usefulness of TVS as a versatile method of investigation, also able to provide important insight into the charge transport through metalloproteins, is emphasized.