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 switches.However,the intr...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 switches.However,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 state.Thus,the room-temperature operation of single-molecule devices has not yet been achieved.Herein,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)technique.The 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)porphyrin.The bias-dependent conductance evolution proves that the strong electric field between the nanoelectrodes plays a crucial role in the coordination reaction.The 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)ion.Our work provides a new avenue to investigate room-temperature spin-related sensors and molecular spintronics.展开更多
基金supported by the National Natural Science Foundation of China(nos.21673195,21722305,21703188,21973079,and 21933012)the National Key R&D Program of China(no.2017YFA0204902)+2 种基金supported by the FET Open project 767187-QuIETthe EU project BAC-TO-FUELthe UK EPSRC grants EP/N017188/1 and EP/M014452/1 in Lancaster.
文摘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 switches.However,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 state.Thus,the room-temperature operation of single-molecule devices has not yet been achieved.Herein,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)technique.The 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)porphyrin.The bias-dependent conductance evolution proves that the strong electric field between the nanoelectrodes plays a crucial role in the coordination reaction.The 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)ion.Our work provides a new avenue to investigate room-temperature spin-related sensors and molecular spintronics.