Theπ-πstacking is a well-recognized intermolecular interaction that is responsible for the construction of electron hopping channels in numerous conducting frameworks/aggregates.However,the exact role ofπ-to-πchan...Theπ-πstacking is a well-recognized intermolecular interaction that is responsible for the construction of electron hopping channels in numerous conducting frameworks/aggregates.However,the exact role ofπ-to-πchannels within typical single crystalline organic semiconductors remains unclear as the orientations of these molecules are diverse,and their control usually requires additional side chain groups that misrepresent the intrinsic properties of the original semiconducting molecules.Therefore,the construction of conduction channels with intrinsicπ-πstacking in the molecule-based device is crucial for the utilization of their unique transport characteristics and understanding of the transport mechanism.To this end,we present a molecular intercalation strategy that integrates two-dimensional layered materials with functional organic semiconductor molecules for functional molecule-based electronics.Various organic semiconductor molecules can be effectively intercalated into the van der Waals gaps of semi-metallic TaS_(2) withπ-πstacking configuration and controlled intercalant content.Our results show that the vertical charge transport in the stacking direction shows a tunneling-dominated mechanism that strongly depends on the molecular structures.Furthermore,we demonstrated a new type of molecule-based vertical transistor in which TaS_(2) andπ-πstacked organic molecules function as the electrical contact and the active channel,respectively.On/off ratios as high as 447 are achieved under electrostatic modulation in ionic liquid,comparable to the current state-of-the-art molecular transistors.Our study provides an ideal platform for probing intrinsic charge transport acrossπ-πstacked conjugated molecules and also a feasible approach for the construction of high-performance molecule-based electronic devices.展开更多
基金support by the National Natural Science Foundation of China(Nos.22172075,92156024)the Fundamental Research Funds for the Central Universities in China(Nos.0210/14380174,14380273)+4 种基金Beijing National Laboratory for Molecular Sciences(No.BNLMS202107)Thousand Talents Plan of Jiangxi Province(No.jxsq2019102002)support by the National Natural Science Foundation of China(No.22033004)support from Early Career Scheme Project(No.21302821)General Research Fund Project(No.11314322)from the University Grants Committee of Hong Kong.
文摘Theπ-πstacking is a well-recognized intermolecular interaction that is responsible for the construction of electron hopping channels in numerous conducting frameworks/aggregates.However,the exact role ofπ-to-πchannels within typical single crystalline organic semiconductors remains unclear as the orientations of these molecules are diverse,and their control usually requires additional side chain groups that misrepresent the intrinsic properties of the original semiconducting molecules.Therefore,the construction of conduction channels with intrinsicπ-πstacking in the molecule-based device is crucial for the utilization of their unique transport characteristics and understanding of the transport mechanism.To this end,we present a molecular intercalation strategy that integrates two-dimensional layered materials with functional organic semiconductor molecules for functional molecule-based electronics.Various organic semiconductor molecules can be effectively intercalated into the van der Waals gaps of semi-metallic TaS_(2) withπ-πstacking configuration and controlled intercalant content.Our results show that the vertical charge transport in the stacking direction shows a tunneling-dominated mechanism that strongly depends on the molecular structures.Furthermore,we demonstrated a new type of molecule-based vertical transistor in which TaS_(2) andπ-πstacked organic molecules function as the electrical contact and the active channel,respectively.On/off ratios as high as 447 are achieved under electrostatic modulation in ionic liquid,comparable to the current state-of-the-art molecular transistors.Our study provides an ideal platform for probing intrinsic charge transport acrossπ-πstacked conjugated molecules and also a feasible approach for the construction of high-performance molecule-based electronic devices.
