Chirality hold broad applications in life sciences,quantum devices,and various other areas.Traditionally,molecular chirality can be characterized by using steady-state circular dichroism spectroscopy.However,the techn...Chirality hold broad applications in life sciences,quantum devices,and various other areas.Traditionally,molecular chirality can be characterized by using steady-state circular dichroism spectroscopy.However,the techniques that can characterize excited state chirality are progressively capturing the public interest as it can provide the dynamic information for chirality generation and transfer.In this review,we focus on the theoretical background and the developmental history of femtosecond time-resolved circular dichroism spectroscopy(TRCD)techniques around the world.Additionally,we provide examples to showcase the utility of these techniques in the analysis of the dynamical molecular chemical structures,the investigation of molecular chirality generation,and the detection of electron spin dynamics in semiconductor quantum dots.展开更多
The intra- and inter-band relaxation dynamics of CdSe/CdS/ZnS core/shell/shell quantum dots are investigated with the aid of time-resolved nonlinear transmission spectra which are obtained using femtosecond pump-probe...The intra- and inter-band relaxation dynamics of CdSe/CdS/ZnS core/shell/shell quantum dots are investigated with the aid of time-resolved nonlinear transmission spectra which are obtained using femtosecond pump-probe technique. By selectively exciting the core and shell carrier, the dynamics are studied in detail. Carrier relaxation is found faster in the conduction band of the CdS shell （about 130 fs） than that in the conduction band of the CdSe core （about 400 fs）. From the experiments it is distinctly demonstrated the existence of the defect states in the interface between the CdSe core and the CdS shell, indicating that ultrafast spectroscopy might be a suitable tool in studying interface and surface morphology properties in nanosystems.展开更多
To overcome the shortcomings of the single-shot autocorrelation SSA where only one pulse width is obtained when the SSA is applied to measure the pulse width of ultrashort laser pulses a modified SSA for measuring the...To overcome the shortcomings of the single-shot autocorrelation SSA where only one pulse width is obtained when the SSA is applied to measure the pulse width of ultrashort laser pulses a modified SSA for measuring the spatiotemporal characteristics of ultrashort laser pulses at different spatial positions is proposed. The spatiotemporal characteristics of femtosecond laser pulses output from the Ti sapphire regenerative amplifier system are experimentally measured by the proposed method. It was found that the complex spatial characteristics are measured accurately.The pulse widths at different spatial positions are various which obey the Gaussian distribution.The pulse width at the same spatial position becomes narrow with the increase in input average power when femtosecond laser pulses pass through a carbon disulfide CS2 nonlinear medium.The experimental results verify that the proposed method is valid for measuring the spatiotemporal characteristics of ultrashort laser pulses at different spatial positions.展开更多
The measurement techniques of femtosecond spectroscopy are effective method to investigate ultrafast dynamics, they are widely used in the fields of physics, chemistry and biology. In this paper, the principle, exper...The measurement techniques of femtosecond spectroscopy are effective method to investigate ultrafast dynamics, they are widely used in the fields of physics, chemistry and biology. In this paper, the principle, experiment setup and the approaches to deal with the experiment data were presented. Then different measurement techniques such as transient absorption spectroscopy, photon echoes, optical Kerr effect and degenerate four-wave mixing were explained with special examples. At last, the application prospect of measurement techniques of femtosecond spectroscopy was forecasted.展开更多
Femtosecond pulsed lasers have been widely used over the past decades due to their capability to fabricate precise patterns at the micro-and nano-lengths scales. A key issue for efficient material processing is the de...Femtosecond pulsed lasers have been widely used over the past decades due to their capability to fabricate precise patterns at the micro-and nano-lengths scales. A key issue for efficient material processing is the determination of the laser parameters used in the experimental set ups. Despite a systematic investigation that has been performed to highlight the impact of every parameter independently, little attention has been drawn on the role of the substrate material on which the irradiated solid is placed. In this work, the influence of the substrate is emphasised for films of various thicknesses, which demonstrates that both the optical and thermophysical properties of the substrate affect the thermal fingerprint on the irradiated film while the impact is manifested to be higher at smaller film sizes. Two representative materials, silicon and fused silica, have been selected as typical substrates for thin films(gold and nickel) of different optical and thermophysical behaviour and the thermal response and damage thresholds are evaluated for the irradiated solids. The pronounced influence of the substrate is aimed to pave the way for new and more optimised designs of laserbased fabrication set ups and processing schemes.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
When femtosecond （fs） timeresolved experiments are used to study ultrafast processes, quantum beat phenomena are often observed. In this paper, to analyze the fs timeresolved spectra, we will present the density mat...When femtosecond （fs） timeresolved experiments are used to study ultrafast processes, quantum beat phenomena are often observed. In this paper, to analyze the fs timeresolved spectra, we will present the density matrix method, a powerful theoretical technique, which describes the dynamics of population and coherence of the system. How to employ it to study the pumpprobe experiments and fs ultrafast processes is described. The transition of pyrazine is used as an example to demonstrate the application of the density matrix method. Recently, Suzuki＇s group have employed the 22 fs time resolution laser to study the dynamics of the state of pyrazine. In this case, conical intersection is commonly believed to play an important role in this nonadiabatic process. How to treat the effect of conical intersection on nonadiabatic processes and fs timeresolved spectra is presented. Another important ultrafast process, vibrational relaxation, which takes place in subps and ps range and has never been carefully studied, is treated in this paper. The vibrational relaxation in water dimer is chosen to demonstrate the calculation. It should be noted that the vibrational relaxation of （H20）2 has not been experimentally studied but it can be accomplished by the pump-probe experiments.展开更多
基金funded by the National Natural Science FoundationofChina(No.92156024and No.92356307 to Jinquan Chen)Menghui Jia thanks the Materials Characterization Center and the Office of Laboratory and Equipment of East China Normal University for funding support(ECNUETR2023-13).
文摘Chirality hold broad applications in life sciences,quantum devices,and various other areas.Traditionally,molecular chirality can be characterized by using steady-state circular dichroism spectroscopy.However,the techniques that can characterize excited state chirality are progressively capturing the public interest as it can provide the dynamic information for chirality generation and transfer.In this review,we focus on the theoretical background and the developmental history of femtosecond time-resolved circular dichroism spectroscopy(TRCD)techniques around the world.Additionally,we provide examples to showcase the utility of these techniques in the analysis of the dynamical molecular chemical structures,the investigation of molecular chirality generation,and the detection of electron spin dynamics in semiconductor quantum dots.
基金This work was supported by the National Natural Science Foundation of China （No.11074003） and the Key Program of Educational Commission of Anhui Province of China （No.KJ2010AI32）. For the help of Prof. J. L. Zhao at Changchun Institute of Optics, Fine Mechanics and Physics, Chinese Academy of Sciences in sample preparation is greatly appreciated.
文摘The intra- and inter-band relaxation dynamics of CdSe/CdS/ZnS core/shell/shell quantum dots are investigated with the aid of time-resolved nonlinear transmission spectra which are obtained using femtosecond pump-probe technique. By selectively exciting the core and shell carrier, the dynamics are studied in detail. Carrier relaxation is found faster in the conduction band of the CdS shell （about 130 fs） than that in the conduction band of the CdSe core （about 400 fs）. From the experiments it is distinctly demonstrated the existence of the defect states in the interface between the CdSe core and the CdS shell, indicating that ultrafast spectroscopy might be a suitable tool in studying interface and surface morphology properties in nanosystems.
基金The National Natural Science Foundation of China(No.61171081,No.61471164)the Natural Science Foundation of Hunan Province(No.14JJ6043)
文摘To overcome the shortcomings of the single-shot autocorrelation SSA where only one pulse width is obtained when the SSA is applied to measure the pulse width of ultrashort laser pulses a modified SSA for measuring the spatiotemporal characteristics of ultrashort laser pulses at different spatial positions is proposed. The spatiotemporal characteristics of femtosecond laser pulses output from the Ti sapphire regenerative amplifier system are experimentally measured by the proposed method. It was found that the complex spatial characteristics are measured accurately.The pulse widths at different spatial positions are various which obey the Gaussian distribution.The pulse width at the same spatial position becomes narrow with the increase in input average power when femtosecond laser pulses pass through a carbon disulfide CS2 nonlinear medium.The experimental results verify that the proposed method is valid for measuring the spatiotemporal characteristics of ultrashort laser pulses at different spatial positions.
文摘The measurement techniques of femtosecond spectroscopy are effective method to investigate ultrafast dynamics, they are widely used in the fields of physics, chemistry and biology. In this paper, the principle, experiment setup and the approaches to deal with the experiment data were presented. Then different measurement techniques such as transient absorption spectroscopy, photon echoes, optical Kerr effect and degenerate four-wave mixing were explained with special examples. At last, the application prospect of measurement techniques of femtosecond spectroscopy was forecasted.
基金Projects(862016(Bio Combs4Nanofibres)HELLAS-CH+1 种基金MIS 5002735) funded by the Operational Programme “Competitiveness, Entrepreneurship and Innovation” and co-financed by Greece and the EU (European Regional Development Fund)Project (COST Action TUMIEE) supported by COST-European Cooperation in Science and Technology。
文摘Femtosecond pulsed lasers have been widely used over the past decades due to their capability to fabricate precise patterns at the micro-and nano-lengths scales. A key issue for efficient material processing is the determination of the laser parameters used in the experimental set ups. Despite a systematic investigation that has been performed to highlight the impact of every parameter independently, little attention has been drawn on the role of the substrate material on which the irradiated solid is placed. In this work, the influence of the substrate is emphasised for films of various thicknesses, which demonstrates that both the optical and thermophysical properties of the substrate affect the thermal fingerprint on the irradiated film while the impact is manifested to be higher at smaller film sizes. Two representative materials, silicon and fused silica, have been selected as typical substrates for thin films(gold and nickel) of different optical and thermophysical behaviour and the thermal response and damage thresholds are evaluated for the irradiated solids. The pronounced influence of the substrate is aimed to pave the way for new and more optimised designs of laserbased fabrication set ups and processing schemes.
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.
文摘When femtosecond （fs） timeresolved experiments are used to study ultrafast processes, quantum beat phenomena are often observed. In this paper, to analyze the fs timeresolved spectra, we will present the density matrix method, a powerful theoretical technique, which describes the dynamics of population and coherence of the system. How to employ it to study the pumpprobe experiments and fs ultrafast processes is described. The transition of pyrazine is used as an example to demonstrate the application of the density matrix method. Recently, Suzuki＇s group have employed the 22 fs time resolution laser to study the dynamics of the state of pyrazine. In this case, conical intersection is commonly believed to play an important role in this nonadiabatic process. How to treat the effect of conical intersection on nonadiabatic processes and fs timeresolved spectra is presented. Another important ultrafast process, vibrational relaxation, which takes place in subps and ps range and has never been carefully studied, is treated in this paper. The vibrational relaxation in water dimer is chosen to demonstrate the calculation. It should be noted that the vibrational relaxation of （H20）2 has not been experimentally studied but it can be accomplished by the pump-probe experiments.
