Characterization of real-time and ultrafast motions of the complex molecules at surface and interface is critical to understand how interracial molecules function. It requires to develop surface-sensitive, fast-identi...Characterization of real-time and ultrafast motions of the complex molecules at surface and interface is critical to understand how interracial molecules function. It requires to develop surface-sensitive, fast-identification, and time-resolved techniques. In this study, we employ several key technical procedures and successfully develop a highly sensitive femtosecond time-resolved sum frequency generation vibrational spectroscopy （SFG-VS） system. This system is able to measure the spectra with two polarization combinations （ssp and ppp, or psp and ssp） simultaneously. It takes less than several seconds to collect one spectrum. To the best of our knowledge, it is the fastest speed of collecting SFG spectra reported by now. Using the time-resolved measurement, ultrafast vibrational dynamics of the N-H mode of α-helical peptide at water interface is determined. It is found that the membrane environment does not affect the N-H vibrational relaxation dynamics. It is expected that the time-resolved SFG system will play a vital role in the deep understanding of the dynamics and interaction of the complex molecules at surface and interface. Our method may also provide an important technical proposal for the people who plan to develop time-resolved SFG systems with simultaneous measurement of multiple polarization combinations.展开更多
This paper demonstrates an approach that negative uniaxial crystal has a relative anomalous dispersion effect which can compensate group velocity delay, and applies this approach to nonlinear frequency conversion of a...This paper demonstrates an approach that negative uniaxial crystal has a relative anomalous dispersion effect which can compensate group velocity delay, and applies this approach to nonlinear frequency conversion of an ultrafast laser field. High efficiency of the third harmonic generation is experimentally fulfilled by adopting a collinear configuration of doubing-compensation-tripling system. Through finely adjusting the incident angle and optical axis direction of the compensation plate, it obtains ultraviolet （UV） output energy of 0.32 mJ centered at 270 nm with spectral bandwidth of 2 nm when input beam at 800 nm was 70 fs pulse duration and 6 mJ pulse energy which was extracted from Ti：sapphire laser system by a diaphragm, corresponding to an 800-to-270 nm conversion efficiency of 5.3% and a factor-of-l.6 improvement in the third harmonic generation of UV band in comparison with a general conventional configuration. Furthermore, when the full energy of 18 mJ from a Ti：sapphire laser system was used and optimized, the UV emission could reach 0.83 mJ.展开更多
文摘Characterization of real-time and ultrafast motions of the complex molecules at surface and interface is critical to understand how interracial molecules function. It requires to develop surface-sensitive, fast-identification, and time-resolved techniques. In this study, we employ several key technical procedures and successfully develop a highly sensitive femtosecond time-resolved sum frequency generation vibrational spectroscopy （SFG-VS） system. This system is able to measure the spectra with two polarization combinations （ssp and ppp, or psp and ssp） simultaneously. It takes less than several seconds to collect one spectrum. To the best of our knowledge, it is the fastest speed of collecting SFG spectra reported by now. Using the time-resolved measurement, ultrafast vibrational dynamics of the N-H mode of α-helical peptide at water interface is determined. It is found that the membrane environment does not affect the N-H vibrational relaxation dynamics. It is expected that the time-resolved SFG system will play a vital role in the deep understanding of the dynamics and interaction of the complex molecules at surface and interface. Our method may also provide an important technical proposal for the people who plan to develop time-resolved SFG systems with simultaneous measurement of multiple polarization combinations.
基金Project supported by the National Basic Research Program of China (Grant No 2006CB0806001)the Program for Changjiang and Innovative Research Team in UniversityShanghai Leading Academic Discipline Project (Grant No B408)
文摘This paper demonstrates an approach that negative uniaxial crystal has a relative anomalous dispersion effect which can compensate group velocity delay, and applies this approach to nonlinear frequency conversion of an ultrafast laser field. High efficiency of the third harmonic generation is experimentally fulfilled by adopting a collinear configuration of doubing-compensation-tripling system. Through finely adjusting the incident angle and optical axis direction of the compensation plate, it obtains ultraviolet （UV） output energy of 0.32 mJ centered at 270 nm with spectral bandwidth of 2 nm when input beam at 800 nm was 70 fs pulse duration and 6 mJ pulse energy which was extracted from Ti：sapphire laser system by a diaphragm, corresponding to an 800-to-270 nm conversion efficiency of 5.3% and a factor-of-l.6 improvement in the third harmonic generation of UV band in comparison with a general conventional configuration. Furthermore, when the full energy of 18 mJ from a Ti：sapphire laser system was used and optimized, the UV emission could reach 0.83 mJ.
