The investigation of electronic excited states in single-molecule junctions not only provides platforms to reveal the photophysical and photochemical processes at the molecular level,but also brings opportunities for ...The investigation of electronic excited states in single-molecule junctions not only provides platforms to reveal the photophysical and photochemical processes at the molecular level,but also brings opportunities for the development of single-molecule optoelectronic devices.Understanding the interaction mechanisms between molecules and nanocavities is essential to obtain ondemand properties in devices by artificial design,since molecules in junctions exhibit unique behaviors of excited states benefited from the structures of metallic nanocavities.Here,we review the excitation mechanisms involved in the interplay between molecules and plasmonic nanocavities,and reveal the influence of nanostructures on excited-state properties by demonstrating the differences in excited state decay processes.Furthermore,vibronic transitions of molecules between nanoelectrodes are also discussed,offering a new single-molecule characterization method.Finally,we provide the potential applications and challenges in single-molecule optoelectronic devices and the possible directions in exploring the underlying mechanisms of photophysical and photochemical processes.展开更多
Acryloyl fluoride is an ideal molecule for investigating the phenomenon of hindered internal rotation.In concert with recently acquired high-resolution UV absorption spectrum of acryloyl fluoride,in this study,the abs...Acryloyl fluoride is an ideal molecule for investigating the phenomenon of hindered internal rotation.In concert with recently acquired high-resolution UV absorption spectrum of acryloyl fluoride,in this study,the absorption spectra of the s-trans and s-cis isomers of acryloyl fluoride were theoretically simulated.The simulated spectra were convoluted by a Gaussian function with displacement,distortion,Franck-Condon,Herzberg-Teller,and Duschinsky effects in the framework of the time-independent model.The statistical vibronic transition analysis reveals the unity of the spectrum transition property,the relevant normal modes,and the primary geometrical variations,enriching the understanding of the experimental observation.The discrepancy between the theoretical and experimental spectra was interpreted clearly.展开更多
基金supported by the National Natural ScienceFoundation of China (Nos. 22173075, 21933012 and 31871877)the National Key R&D Program of China (No. 2017YFA0204902)+1 种基金the Fundamental Research Funds for the Central Universities(Nos. 20720200068 and 20720190002)the Beijing NationalLaboratory for Molecular Sciences (No. BNLMS202005).
文摘The investigation of electronic excited states in single-molecule junctions not only provides platforms to reveal the photophysical and photochemical processes at the molecular level,but also brings opportunities for the development of single-molecule optoelectronic devices.Understanding the interaction mechanisms between molecules and nanocavities is essential to obtain ondemand properties in devices by artificial design,since molecules in junctions exhibit unique behaviors of excited states benefited from the structures of metallic nanocavities.Here,we review the excitation mechanisms involved in the interplay between molecules and plasmonic nanocavities,and reveal the influence of nanostructures on excited-state properties by demonstrating the differences in excited state decay processes.Furthermore,vibronic transitions of molecules between nanoelectrodes are also discussed,offering a new single-molecule characterization method.Finally,we provide the potential applications and challenges in single-molecule optoelectronic devices and the possible directions in exploring the underlying mechanisms of photophysical and photochemical processes.
文摘Acryloyl fluoride is an ideal molecule for investigating the phenomenon of hindered internal rotation.In concert with recently acquired high-resolution UV absorption spectrum of acryloyl fluoride,in this study,the absorption spectra of the s-trans and s-cis isomers of acryloyl fluoride were theoretically simulated.The simulated spectra were convoluted by a Gaussian function with displacement,distortion,Franck-Condon,Herzberg-Teller,and Duschinsky effects in the framework of the time-independent model.The statistical vibronic transition analysis reveals the unity of the spectrum transition property,the relevant normal modes,and the primary geometrical variations,enriching the understanding of the experimental observation.The discrepancy between the theoretical and experimental spectra was interpreted clearly.
