We review the technique and research of the ultrahigh spatiotemporal resolved spectroscopy and its applications in the field of the ultrafast dynamics of mesoscopic systems and nanomaterials. Combining femtosecond tim...We review the technique and research of the ultrahigh spatiotemporal resolved spectroscopy and its applications in the field of the ultrafast dynamics of mesoscopic systems and nanomaterials. Combining femtosecond time-resolved spectroscopy and scanning near-field optical microscopy (SNOM),we can obtain the spectra with ultrahigh temporal and spatial resolutions simultaneously. Some problems in doing so are discussed. Then we show the important applications of the ultrahigh spatiotemporal resolved spectroscopy with a few typical examples.展开更多
In this article, we primarily review the time-resolved imaging of THz phonon polariton, which is generated by femtosecond laser in ferroelectric crystal. We pay more attention to the imaging in thin crystal, which can...In this article, we primarily review the time-resolved imaging of THz phonon polariton, which is generated by femtosecond laser in ferroelectric crystal. We pay more attention to the imaging in thin crystal, which can be used as an integration platform for terahertz-optics or terahertz-electrics. The imaging techniques, which can get quantitatively in-focus time-resolved images, are introduced in more detail. They have made enormous progress in recent years, and are powerful tools for the research of phonon polariton, optics, and THz wave. We also briefly introduce the generation principle and general propagation properties of THz phonon polariton.展开更多
Aluminum ablation by multiple femtosecond laser pulses is investigated via time-resolved shadowgraphs and scanning electron microscope （SEM） images of the ablation spot. The spatial distribution of the ejected mater...Aluminum ablation by multiple femtosecond laser pulses is investigated via time-resolved shadowgraphs and scanning electron microscope （SEM） images of the ablation spot. The spatial distribution of the ejected material and the radius of the shock wave generated during the ablation are found to vary with the increase in the number of pulses. In the initial two pulses, nearly concentric and semicircular stripes within the shock wave front are observed, unlike in subsequent pulses. Ablation by multiple femtosecond pulses exhibits different characteristics compared with the case induced by single femtosecond pulse because of the changes to the aluminum target surface induced by the preceding pulses.展开更多
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
We experimentally investigated the forward 353.8 nm radiation from plasma filaments in pure nitrogen gas pumped by intense circularly polarized 800 nm femtosecond laser pulses.This emission line corresponds to the B^2...We experimentally investigated the forward 353.8 nm radiation from plasma filaments in pure nitrogen gas pumped by intense circularly polarized 800 nm femtosecond laser pulses.This emission line corresponds to the B^2Σu^+(u'=4)-X^2Σg^+(u=3)transition of nitrogen ions.In the presence of an external seeding pulse,the 353.8 nm signal was amplified by 3 orders of magnitude.Thanks to the much enhanced intensity,we performed time-resolved measurement of the amplified 353.8 nm emission based on the sum-frequency generation technique.It was revealed that the built-up time and duration of these emissions are both inversely proportional to the gas pressure,while the radiation peak power grows up nearly quadratically with pressure,indicating that the 353.8 nm radiation is of the nature of superradiance.展开更多
The femtosecond time-resolved difference absorption spectra of all-trans-β-Apo-8′-carotenal have been recorded and analyzed by the singular-value decomposition (SVD) method followed by global fitting using a sequent...The femtosecond time-resolved difference absorption spectra of all-trans-β-Apo-8′-carotenal have been recorded and analyzed by the singular-value decomposition (SVD) method followed by global fitting using a sequential model for the excited-state energy relaxation. With this model, we have obtained the excited-state absorption spectra and the lifetimes of the corresponding excited states both in nonpolar solvent n-hexane and polar solvent methanol. Three excited states, namely S3(170fs), S2(2.32ps) and S1(26ps) in n-hexane, and two excited states S2(190fs) and S1(9.4ps) in methanol have been observed. The excited-state absorption spectra of all-trans-β-Apo-8′-carotenal in methanol display a red shift and broadeness, while the lifetime of S1 state becomes shorter. It is proposed that these effects are related to the presence of a carbonyl functional group that leads to the solvent effect on the excited-state energy level. At the same time, it is shown that the SVD method is a useful tool in resolving the time-resolved absorption spectra.展开更多
The S_(1) state decay dynamics of 2-hydroxypyridine following UV excitation at a wavelength range of 276.9-250.0 nm is investigated using femtosecond time-resolved photoelectron imaging technique.Based on pump wavelen...The S_(1) state decay dynamics of 2-hydroxypyridine following UV excitation at a wavelength range of 276.9-250.0 nm is investigated using femtosecond time-resolved photoelectron imaging technique.Based on pump wavelength dependence of the decay dynamics,a refined decay picture is proposed.At pump wavelength of 276.9 nm,the S_(1) state is depopulated through intersystem crossing to lower triplet state(s).At 264.0 nm,both intersystem crossing to lower triplet state(s)and internal conversion to the ground state are in operation.At 250.0 nm,internal conversion to the ground state becomes dominated.展开更多
基金Supported by the National Natural Science Foundation of China (Grant Nos. 10434020, 90501007 and 10521002)the National Basic Research Program of China (Grant No. 2007CB307001)
文摘We review the technique and research of the ultrahigh spatiotemporal resolved spectroscopy and its applications in the field of the ultrafast dynamics of mesoscopic systems and nanomaterials. Combining femtosecond time-resolved spectroscopy and scanning near-field optical microscopy (SNOM),we can obtain the spectra with ultrahigh temporal and spatial resolutions simultaneously. Some problems in doing so are discussed. Then we show the important applications of the ultrahigh spatiotemporal resolved spectroscopy with a few typical examples.
文摘In this article, we primarily review the time-resolved imaging of THz phonon polariton, which is generated by femtosecond laser in ferroelectric crystal. We pay more attention to the imaging in thin crystal, which can be used as an integration platform for terahertz-optics or terahertz-electrics. The imaging techniques, which can get quantitatively in-focus time-resolved images, are introduced in more detail. They have made enormous progress in recent years, and are powerful tools for the research of phonon polariton, optics, and THz wave. We also briefly introduce the generation principle and general propagation properties of THz phonon polariton.
基金Project supported by the Science and Technology Development Fund Planning Project for the Universities of Tianjin,China(Grant No.20140902)the Natural Science Foundation of Tianjin City,China(Grant No.16JCQNJC01900)+1 种基金the National Natural Science Foundation of China(Grant Nos.51376136and 61474082)the Science and Technology Achievement Award Project for the Universities of Tianjin,China
文摘Aluminum ablation by multiple femtosecond laser pulses is investigated via time-resolved shadowgraphs and scanning electron microscope （SEM） images of the ablation spot. The spatial distribution of the ejected material and the radius of the shock wave generated during the ablation are found to vary with the increase in the number of pulses. In the initial two pulses, nearly concentric and semicircular stripes within the shock wave front are observed, unlike in subsequent pulses. Ablation by multiple femtosecond pulses exhibits different characteristics compared with the case induced by single femtosecond pulse because of the changes to the aluminum target surface induced by the preceding pulses.
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supported in part by the National Natural Science Foundation of China(Nos.11574213 and 11904232)Innovation Program of Shanghai Municipal Education Commission(No.2017-01-07-00-07-E00007)+1 种基金the Shanghai Municipal Science and Technology Commission(No.17060502500)the support of the Program for Professor of Special Appointment(Eastern Scholar)at the Shanghai Institutions of Higher Learning(No.TP2014046).
文摘We experimentally investigated the forward 353.8 nm radiation from plasma filaments in pure nitrogen gas pumped by intense circularly polarized 800 nm femtosecond laser pulses.This emission line corresponds to the B^2Σu^+(u'=4)-X^2Σg^+(u=3)transition of nitrogen ions.In the presence of an external seeding pulse,the 353.8 nm signal was amplified by 3 orders of magnitude.Thanks to the much enhanced intensity,we performed time-resolved measurement of the amplified 353.8 nm emission based on the sum-frequency generation technique.It was revealed that the built-up time and duration of these emissions are both inversely proportional to the gas pressure,while the radiation peak power grows up nearly quadratically with pressure,indicating that the 353.8 nm radiation is of the nature of superradiance.
文摘The femtosecond time-resolved difference absorption spectra of all-trans-β-Apo-8′-carotenal have been recorded and analyzed by the singular-value decomposition (SVD) method followed by global fitting using a sequential model for the excited-state energy relaxation. With this model, we have obtained the excited-state absorption spectra and the lifetimes of the corresponding excited states both in nonpolar solvent n-hexane and polar solvent methanol. Three excited states, namely S3(170fs), S2(2.32ps) and S1(26ps) in n-hexane, and two excited states S2(190fs) and S1(9.4ps) in methanol have been observed. The excited-state absorption spectra of all-trans-β-Apo-8′-carotenal in methanol display a red shift and broadeness, while the lifetime of S1 state becomes shorter. It is proposed that these effects are related to the presence of a carbonyl functional group that leads to the solvent effect on the excited-state energy level. At the same time, it is shown that the SVD method is a useful tool in resolving the time-resolved absorption spectra.
基金supported by the National Natural Science Foundation of China(No.21833003)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB17000000)the Key Technology Team of the Chinese Academy of Sciences(GJJSTD20190002)。
文摘The S_(1) state decay dynamics of 2-hydroxypyridine following UV excitation at a wavelength range of 276.9-250.0 nm is investigated using femtosecond time-resolved photoelectron imaging technique.Based on pump wavelength dependence of the decay dynamics,a refined decay picture is proposed.At pump wavelength of 276.9 nm,the S_(1) state is depopulated through intersystem crossing to lower triplet state(s).At 264.0 nm,both intersystem crossing to lower triplet state(s)and internal conversion to the ground state are in operation.At 250.0 nm,internal conversion to the ground state becomes dominated.
