Coherent Electron Transport across a 3 nm Bioelectronic Junction Made of Multi-Heme Proteins.
Coherent Electron Transport across a 3 nm Bioelectronic Junction Made of Multi-Heme Proteins.
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DOI：
10.1021/acs.jpclett.0c02686
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发表时间：
2020-11-19
期刊：
影响因子：
--
通讯作者：
Blumberger J
中科院分区：
文献类型：
--
作者：
Futera Z;Ide I;Kayser B;Garg K;Jiang X;van Wonderen JH;Butt JN;Ishii H;Pecht I;Sheves M;Cahen D;Blumberger J
多血红素细胞色素（MHC）是细菌生物体用来在细胞内、细胞间和细胞外穿梭电子的迷人蛋白质。当置于固态电子结中时，MHC支持超过几纳米的温度无关电流，与其他类似大小的氧化还原蛋白质相比高出3个数量级。为了从分子水平上深入了解它们的超高电导率，我们将联合收割机实验光电子能谱与DFT+ DFT电流-电压计算结合起来，对一个代表性的金-MHC-金结进行了计算。我们发现，通过非共振相干隧穿，介导的大量的蛋白质的价带轨道，强烈离域血红素和蛋白质残基的干，3 nm长的蛋白质的传导发生。这一现象与水溶液中电化学或光化学诱导的电子跳跃机制截然不同。我们的研究结果意味着，在固态结的电流输出可以进一步增加谐振，例如，通过施加栅极电压，从而允许下一代生物纳米电子器件的量子跳跃。
Multi-heme cytochromes (MHCs) are fascinating proteins used by bacterial organisms to shuttle electrons within, between, and out of their cells. When placed in solid-state electronic junctions, MHCs support temperature-independent currents over several nanometers that are 3 orders of magnitude higher compared to other redox proteins of similar size. To gain molecular-level insight into their astonishingly high conductivities, we combine experimental photoemission spectroscopy with DFT+Σ current–voltage calculations on a representative Gold-MHC-Gold junction. We find that conduction across the dry, 3 nm long protein occurs via off-resonant coherent tunneling, mediated by a large number of protein valence-band orbitals that are strongly delocalized over heme and protein residues. This picture is profoundly different from the electron hopping mechanism induced electrochemically or photochemically under aqueous conditions. Our results imply that the current output in solid-state junctions can be even further increased in resonance, for example, by applying a gate voltage, thus allowing a quantum jump for next-generation bionanoelectronic devices.
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影响因子：
16.6
作者：
Fereiro, Jerry A.;Kayser, Ben;Cahen, David
通讯作者：
Cahen, David
影响因子：
3.3
作者：
Amdursky, Nadav;Ferber, Doron;Cahen, David
通讯作者：
Cahen, David
影响因子：
3.9
作者：
Breuer, Marian;Zarzycki, Piotr;Rosso, Kevin M.
通讯作者：
Rosso, Kevin M.
DOI：
10.1073/pnas.1316156111
发表时间：
2014-01-14
影响因子：
11.1
作者：
Breuer, Marian;Rosso, Kevin M.;Blumberger, Jochen
通讯作者：
Blumberger, Jochen
影响因子：
4.6
作者：
Edwards MJ;White GF;Norman M;Tome-Fernandez A;Ainsworth E;Shi L;Fredrickson JK;Zachara JM;Butt JN;Richardson DJ;Clarke TA
通讯作者：
Clarke TA