Propagation of a signal beam in an Al Ga As/Ga As waveguide multiple-prism light deflector is theoretically investigated by solving the scalar Helmholtz equation to obtain the dependences of the temporal and spatial r...Propagation of a signal beam in an Al Ga As/Ga As waveguide multiple-prism light deflector is theoretically investigated by solving the scalar Helmholtz equation to obtain the dependences of the temporal and spatial resolvable characteristics of the ultrafast deflector on the material dispersion of Ga As including group velocity dispersion and angular dispersion,interface reflection,and interface scattering of multiple-prism deflector.Furthermore,we experimentally confirm that,in this ultrafast beam deflection device,the deflecting angle of the signal light beam is linear with the pump fluence and the temporal resolution of the ultrafast deflection is 10 ps.Our results show that the improvement of the temporal and spatial resolvable performances is possible by properly choosing the structural parameters and enhancing the quality of the device.展开更多
Understanding the ultrafast carrier dynamics and the mechanism of two-dimensional(2D)transition metal dichalcogenides(TMDs)is key to their applications in the field of optoelectronic devices.In this work,a single puls...Understanding the ultrafast carrier dynamics and the mechanism of two-dimensional(2D)transition metal dichalcogenides(TMDs)is key to their applications in the field of optoelectronic devices.In this work,a single pulse pump probe method is introduced to detect the layer-dependent ultrafast carrier dynamics of monolayer and few-layer WS_(2) excited by a femtosecond pulse.Results show that the ultrafast carrier dynamics of the layered WS_(2) films can be divided into three stages:the fast photoexcitation phase with the characteristic time of 2–4 ps,the fast decay phase with the characteristic time of 4–20 ps,and the slow decay phase lasting several hundred picoseconds.Moreover,the layer dependency of the characteristic time of each stage has been observed,and the corresponding mechanism of free carrier dynamics has been discussed.It has been observed as well that the monolayer WS_(2) exhibits a unique rising time of carriers after photoexcitation.The proposed method can be expected to be an effective approach for studying the dynamics of the photoexcited carriers in 2D TMDs.Our results provide a comprehensive understanding of the photoexcited carrier dynamics of layered WS_(2),which is essential for its application in optoelectronics and photovoltaic devices.展开更多
This paper reports that a one-colour fs pump probe measurement has been carried out for studying photoionization/photodissociation of cyclohexanone （C6H10O） in intense laser field. Two of the fragments from eyclohex...This paper reports that a one-colour fs pump probe measurement has been carried out for studying photoionization/photodissociation of cyclohexanone （C6H10O） in intense laser field. Two of the fragments from eyclohexanone, C2H＋ and C3H3＋, are studied under 800 nm laser pump-probe and the results obtained show similar time evolutions. It proposes a feasible model for analysing the experimental observations of the one-colour fs pump-probe measurement. The results demonstrate that as an intermediate product, the excited molecular parent ions play a very important role in photionization/photodissociation processes in intense laser field.展开更多
Resonance enhancement has been increasingly employed in the emergent felntosecond stimu- lated Raman spectroscopy （FSRS） to selectively monitor molecular structure and dynamics with improved spectral and temporal re...Resonance enhancement has been increasingly employed in the emergent felntosecond stimu- lated Raman spectroscopy （FSRS） to selectively monitor molecular structure and dynamics with improved spectral and temporal resolutions and signal-to-noise ratios. Such joint eflforts by the technique- and application-oriented scientists and engineers have laid the foundation for exploiting the tunable FSRS methodology to investigate a great variety of photosensitive systems and elucidate the underlying functional mechanisms on molecular time scales. Dur- ing spectral analysis, peak line shapes remain a major concern with an intricate dependence on resonance conditions. Here, we present a comprehensive study of line shapes by tuning the Rarnan pump wavelength from red to blue side of the ground-state absorption band of the fluorescent dye rhodarnine 6G in solution. Distinct line shape patterns in Stokes and anti-Stokes FSRS as well as from the low to high-frequency modes highlight the competition between multiple third-order and higher-order nonlinear pathways, governed by difl^rent res- onance conditions achieved by Raman pump and probe pulses. In particular, the resonance condition of probe wavelength is revealed to play an important role in generating circular line shape changes through oppositely phased dispersion via hot luminescence （HL） pathways. Meanwhile, on-resonance conditions of the Rarnan pump could promote excited-state vibrational modes which are broadened and red-shifted from the coincident ground-state vibrational modes, posing challenges for spectral analysis. Certain strategies in tuning the Raman pump and probe to characteristic regions across an electronic transition band are discussed to improve the FSRS usability and versatility as a powerful structural dynamics toolset to advance chemical, physical, materials, and biological sciences.展开更多
Surface states are expected to play a key role in broadband terahertz(THz) emitters, where photoexcited carrier distributions are confined within about 1 μm of the surface. Optical pump and THz probe spectroscopy was...Surface states are expected to play a key role in broadband terahertz(THz) emitters, where photoexcited carrier distributions are confined within about 1 μm of the surface. Optical pump and THz probe spectroscopy was used to study the dynamics of nonequilibrium charge carriers in both textured and non-textured GaAs substrates.Our findings show that the textured surface acts as an antireflective layer, greatly boosting the infrared pump laser's coupling efficiency into the semi-insulating GaAs substrate. Additionally, texturing introduces a trapassisted recombination pathway, speeding up carrier relaxation and thus reducing Joule heating. Under the same pumping and bias field conditions, the coarse-textured GaAs photoconductive antenna shows nearly 7.85 times stronger THz emission amplitude than the non-textured device, along with improvement in signal-to-noise ratio.At a fixed bias field, higher pump power increases photogenerated carrier density, causing bias field screening and subsequent saturation of THz emission. At fixed pump power, when the bias field reaches ~2.5 kV/cm, both THz emission and photocurrent spectra show a clear kink, signaling intervalley scattering from the Γ valley to the L(X) valleys under high electric fields.展开更多
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11274377 and 61176006)the State Major Research Equipment ProChina(Grant No.ZDY2011-2)
文摘Propagation of a signal beam in an Al Ga As/Ga As waveguide multiple-prism light deflector is theoretically investigated by solving the scalar Helmholtz equation to obtain the dependences of the temporal and spatial resolvable characteristics of the ultrafast deflector on the material dispersion of Ga As including group velocity dispersion and angular dispersion,interface reflection,and interface scattering of multiple-prism deflector.Furthermore,we experimentally confirm that,in this ultrafast beam deflection device,the deflecting angle of the signal light beam is linear with the pump fluence and the temporal resolution of the ultrafast deflection is 10 ps.Our results show that the improvement of the temporal and spatial resolvable performances is possible by properly choosing the structural parameters and enhancing the quality of the device.
基金supported by the National Natural Science Foundation of China (Nos. 51975232 and 51727809)the Experiment Center for Advanced Manufacturing and Technology in the School of Mechanical Science & Engineering of HUST for the technical support.
文摘Understanding the ultrafast carrier dynamics and the mechanism of two-dimensional(2D)transition metal dichalcogenides(TMDs)is key to their applications in the field of optoelectronic devices.In this work,a single pulse pump probe method is introduced to detect the layer-dependent ultrafast carrier dynamics of monolayer and few-layer WS_(2) excited by a femtosecond pulse.Results show that the ultrafast carrier dynamics of the layered WS_(2) films can be divided into three stages:the fast photoexcitation phase with the characteristic time of 2–4 ps,the fast decay phase with the characteristic time of 4–20 ps,and the slow decay phase lasting several hundred picoseconds.Moreover,the layer dependency of the characteristic time of each stage has been observed,and the corresponding mechanism of free carrier dynamics has been discussed.It has been observed as well that the monolayer WS_(2) exhibits a unique rising time of carriers after photoexcitation.The proposed method can be expected to be an effective approach for studying the dynamics of the photoexcited carriers in 2D TMDs.Our results provide a comprehensive understanding of the photoexcited carrier dynamics of layered WS_(2),which is essential for its application in optoelectronics and photovoltaic devices.
基金Project supported by the National Natural Science Foundation of China (Grant No 10534010)
文摘This paper reports that a one-colour fs pump probe measurement has been carried out for studying photoionization/photodissociation of cyclohexanone （C6H10O） in intense laser field. Two of the fragments from eyclohexanone, C2H＋ and C3H3＋, are studied under 800 nm laser pump-probe and the results obtained show similar time evolutions. It proposes a feasible model for analysing the experimental observations of the one-colour fs pump-probe measurement. The results demonstrate that as an intermediate product, the excited molecular parent ions play a very important role in photionization/photodissociation processes in intense laser field.
基金supported by the U.S.National Science Foundation CAREER grant(CHE-1455353)the Oregon State University(OSU) Research Equipment Reserve Fund(Spring 2014)to C.Fang(USTC9603)the Wei Family Private Foundation in supporting C.Chen(USTC 0903) during his graduate studies at OSU Chemistry
文摘Resonance enhancement has been increasingly employed in the emergent felntosecond stimu- lated Raman spectroscopy （FSRS） to selectively monitor molecular structure and dynamics with improved spectral and temporal resolutions and signal-to-noise ratios. Such joint eflforts by the technique- and application-oriented scientists and engineers have laid the foundation for exploiting the tunable FSRS methodology to investigate a great variety of photosensitive systems and elucidate the underlying functional mechanisms on molecular time scales. Dur- ing spectral analysis, peak line shapes remain a major concern with an intricate dependence on resonance conditions. Here, we present a comprehensive study of line shapes by tuning the Rarnan pump wavelength from red to blue side of the ground-state absorption band of the fluorescent dye rhodarnine 6G in solution. Distinct line shape patterns in Stokes and anti-Stokes FSRS as well as from the low to high-frequency modes highlight the competition between multiple third-order and higher-order nonlinear pathways, governed by difl^rent res- onance conditions achieved by Raman pump and probe pulses. In particular, the resonance condition of probe wavelength is revealed to play an important role in generating circular line shape changes through oppositely phased dispersion via hot luminescence （HL） pathways. Meanwhile, on-resonance conditions of the Rarnan pump could promote excited-state vibrational modes which are broadened and red-shifted from the coincident ground-state vibrational modes, posing challenges for spectral analysis. Certain strategies in tuning the Raman pump and probe to characteristic regions across an electronic transition band are discussed to improve the FSRS usability and versatility as a powerful structural dynamics toolset to advance chemical, physical, materials, and biological sciences.
基金supported by the National Key Research and Development Program of China (Grant No.2023YFF0719200)the National Natural Science Foundation of China (Grant Nos.62322115,U24A20226,62588201,62435010,and 62335012)+2 种基金the 111 Project (Grant No.D18014)the Key project supported by Science and Technology Commission Shanghai Municipality (Grant No.YDZX20193100004960)Science and Technology Commission of Shanghai Municipality (Grant Nos.22JC1400200 and 21S31907400)。
文摘Surface states are expected to play a key role in broadband terahertz(THz) emitters, where photoexcited carrier distributions are confined within about 1 μm of the surface. Optical pump and THz probe spectroscopy was used to study the dynamics of nonequilibrium charge carriers in both textured and non-textured GaAs substrates.Our findings show that the textured surface acts as an antireflective layer, greatly boosting the infrared pump laser's coupling efficiency into the semi-insulating GaAs substrate. Additionally, texturing introduces a trapassisted recombination pathway, speeding up carrier relaxation and thus reducing Joule heating. Under the same pumping and bias field conditions, the coarse-textured GaAs photoconductive antenna shows nearly 7.85 times stronger THz emission amplitude than the non-textured device, along with improvement in signal-to-noise ratio.At a fixed bias field, higher pump power increases photogenerated carrier density, causing bias field screening and subsequent saturation of THz emission. At fixed pump power, when the bias field reaches ~2.5 kV/cm, both THz emission and photocurrent spectra show a clear kink, signaling intervalley scattering from the Γ valley to the L(X) valleys under high electric fields.
