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Room-Temperature Single-Molecule Conductance Switch via Confined Coordination-Induced Spin-State Manipulation

CCS Chemistry 2022年第4期4卷 1357-1365页

作者： Jing Li Qingqing Wu Wei Xu Hai-Chuan Wang Hewei Zhang Yaorong Chen Yongxiang Tang Songjun Hou colin jlambert Wenjing Hong State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005 Department of Physics Lancaster UniversityLancaster LA14YB

The emergence of molecular spintronics offers a unique chance for the design of molecular devices with different spin-states,and the control of spin-state becomes essential for molecular spin ***,the intrinsic spin switching from low-to high-spin state is a temperature-dependent process with a small energy barrier where low temperature is required to maintain the low-spin ***,the room-temperature operation of single-molecule devices has not yet been ***,we present a reversible single-molecule conductance switch by manipulating the spin states of the molecule at room temperature using the scanning tunneling microscope break-junction(STM-BJ)*** manipulation of the spin states between S=0 and S=1 is achieved by complexing or decomplexing the pyridine derivative molecule with a square planar nickel(Ⅱ)*** bias-dependent conductance evolution proves that the strong electric field between the nanoelectrodes plays a crucial role in the coordination *** density functional theory(DFT)calculations further reveal that the conductance changes come from the geometric changes of the porphyrin ring and spin-state switching of the Ni(Ⅱ)*** work provides a new avenue to investigate room-temperature spin-related sensors and molecular spintronics.

关键词： confined coordination-induced spinstate manipulation molecular spintronics nickel(Ⅱ)porphyrin break junctions

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Solvent-molecule interaction induced gating of charge transport through single-molecule junctions

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Science Bulletin 2020年第11期65卷 944-950,M0004页

作者： Zheng Tang Songjun Hou Qingqing Wu Zhibing Tan Jueting Zheng Ruihao Li Junyang Liu Yang Yang Hatef Sadeghi Jia Shi Iain Grace colin jlambert Wenjing Hong State Key Laboratory of Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materials(iChEM)College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Department of Physics Lancaster UniversityLancaster LA14YBUK

To explore solvent gating of single-molecule electrical conductance due to solvent-molecule interactions, charge transport through single-molecule junctions with different anchoring groups in various solvent environments was measured by using the mechanically controllable break junction technique. We found that the conductance of single-molecule junctions can be tuned by nearly an order of magnitude by varying the polarity of solvent. Furthermore, gating efficiency due to solvent–molecule interactions was found to be dependent on the choice of the anchor group. Theoretical calculations revealed that the polar solvent shifted the molecular-orbital energies, based on the coupling strength of the anchor groups. For weakly coupled molecular junctions, the polar solvent–molecule interaction was observed to reduce the energy gap between the molecular orbital and the Fermi level of the electrode and shifted the molecular orbitals. This resulted in a more significant gating effect than that of the strongly coupled molecules. This study suggested that solvent–molecule interaction can significantly affect the charge transport through single-molecule junctions.

关键词： Solvent-induced gating Molecular electronics Single-molecule conductance Break junctions

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