Here we report a quantitative study of the orientational structure and motion of water molecule at the air/water interface. Analysis of Sum Frequency Generation （SFG） vibrational peak of the free O-H stretching band...Here we report a quantitative study of the orientational structure and motion of water molecule at the air/water interface. Analysis of Sum Frequency Generation （SFG） vibrational peak of the free O-H stretching band at 3700 cm^-1 in four experimental configurations showed that orientational motion of water molecule at air/water interface is libratory within a limited angular range. The free OH bond of the interracial water molecule is tilted around 33°from the interface normal and the orientational distribution or motion width is less than 15°. This picture is significantly different from the previous conclusion that the interracial water molecule orientation varies over a broad range within the ultrafast vibrational relaxation time, the only direct experimental study concluded for ultrafast and broad orient, ational motion of a liquid interface by Wei et al. （Phys. Rev. Lett. 86, 4799, （2001）） using single SFG experimental configuration.展开更多
Single nanoparticle tracking(SPT)is a unique and powerful tool to investigate the interaction between nanoparticles and cells,which is of considerable importance for nanotechnology applications in biomedical fields an...Single nanoparticle tracking(SPT)is a unique and powerful tool to investigate the interaction between nanoparticles and cells,which is of considerable importance for nanotechnology applications in biomedical fields and in-depth understanding of biological activities.However,previous work typically focused on translations of single nanoparticles while they undergo both translational and rotational motions.In this study,we obtained both the translational and rotational dynamics of single gold nanorods during their cellular internalization process using dual-channel polarization microscopy.In particular,the azimuth and polar angles were integrated into a polar coordinate systemto obtain three general orientation distribution patterns,found to have a close relationship with the nanoparticle cellular internalization process and time-dependent alterations.Moreover,the patterns accompanied by trajectories,translational and rotational coefficients,the azimuth and polar angles,and other parameters provided a wealth of knowledge on the nanoparticle cellular internalization dynamics with unprecedented details.We observed that the gold nanorods could initially assume a tip-first quick rotation state with partially restricted orientations,then change to a strongly confined near-vertical insertion state with slight angular fluctuations,and eventually transform into a random and fast rotation state.Our methodology opens up a new avenue for a detailed understanding of biological processes.展开更多
基金This work was supported by Chines Academy of Scieuces（No.CMS-cx200305）,National Natural Science Foundation of China（NSFC No.20425309,No.20573117）and Chinese Ministry of Science and Technology （M0ST No.G1999075305）.
文摘Here we report a quantitative study of the orientational structure and motion of water molecule at the air/water interface. Analysis of Sum Frequency Generation （SFG） vibrational peak of the free O-H stretching band at 3700 cm^-1 in four experimental configurations showed that orientational motion of water molecule at air/water interface is libratory within a limited angular range. The free OH bond of the interracial water molecule is tilted around 33°from the interface normal and the orientational distribution or motion width is less than 15°. This picture is significantly different from the previous conclusion that the interracial water molecule orientation varies over a broad range within the ultrafast vibrational relaxation time, the only direct experimental study concluded for ultrafast and broad orient, ational motion of a liquid interface by Wei et al. （Phys. Rev. Lett. 86, 4799, （2001）） using single SFG experimental configuration.
基金supported by the National Natural Science Foundation of China(grant nos.21127009,21221003,and 21425519)the Training Program for Excellent Young Innovators of Changsha(grant no.kq1905061)the Natural Science Foundation of Hunan Province,China(grant no.020RC3042).
文摘Single nanoparticle tracking(SPT)is a unique and powerful tool to investigate the interaction between nanoparticles and cells,which is of considerable importance for nanotechnology applications in biomedical fields and in-depth understanding of biological activities.However,previous work typically focused on translations of single nanoparticles while they undergo both translational and rotational motions.In this study,we obtained both the translational and rotational dynamics of single gold nanorods during their cellular internalization process using dual-channel polarization microscopy.In particular,the azimuth and polar angles were integrated into a polar coordinate systemto obtain three general orientation distribution patterns,found to have a close relationship with the nanoparticle cellular internalization process and time-dependent alterations.Moreover,the patterns accompanied by trajectories,translational and rotational coefficients,the azimuth and polar angles,and other parameters provided a wealth of knowledge on the nanoparticle cellular internalization dynamics with unprecedented details.We observed that the gold nanorods could initially assume a tip-first quick rotation state with partially restricted orientations,then change to a strongly confined near-vertical insertion state with slight angular fluctuations,and eventually transform into a random and fast rotation state.Our methodology opens up a new avenue for a detailed understanding of biological processes.
