Photo-induced intramolecular electron transfer （PIET） and intramolecular vibrational relaxation （IVR） dynamics of the excited state of rhodamine 6G （Rh6G＋） in DMSO are investigated by multiplex transient gratin...Photo-induced intramolecular electron transfer （PIET） and intramolecular vibrational relaxation （IVR） dynamics of the excited state of rhodamine 6G （Rh6G＋） in DMSO are investigated by multiplex transient grating. Two major compo- nents are resolved in the dynamics of Rh6G＋. The first component, with a lifetime τTPIET = 140 fs-260 fs, is attributed to PIET from the phenyl ring to the xanthene plane. The IVR process occurring in the range ZIVR = 3.3 ps-5.2 ps is much slower than the first component. The PIET and IVR processes occurring in the excited state of Rh6G＋ are quantitatively determined, and a better understanding of the relationship between these processes is obtained.展开更多
Femtosecond time-resolved transient grating(TG) technique is used to study the intermolecular dynamics in liquid phase. Non-resonant excitation of the sample by two crossing laser pulses results in a transient Kerr gr...Femtosecond time-resolved transient grating(TG) technique is used to study the intermolecular dynamics in liquid phase. Non-resonant excitation of the sample by two crossing laser pulses results in a transient Kerr grating, and the molecular motion of liquid can be detected by monitoring the diffraction of a third time-delayed probe pulse. In liquid nitrobenzene(NB), three intermolecular processes are observed with lifetimes of 37.9±1.4 ps, 3.28±0.11 ps, and 0.44±0.03 ps, respectively. These relaxations are assigned to molecular orientational diffusion, dipole/induced dipole interaction, and libration in liquid cage, respectively. Such a result is slightly different from that obtained from OKE experiment in which the lifetime of the intermediate process is measured to be 1.9 ps. The effects of electric field on matter are different in TG and optical Kerr effect(OKE) experiments, which should be responsible for the difference between the results of these two types of experiments. The present work demonstrates that TG technique is a useful alternative in the study of intermolecular dynamics.展开更多
Experiments on fs laser-induced transient grating （LITG） in carbon bisulfide （CS2） are carried out to explore the chirp characteristics of a white-light supercontinuum （SC） generated by a 800-nm, 160-fs laser pu...Experiments on fs laser-induced transient grating （LITG） in carbon bisulfide （CS2） are carried out to explore the chirp characteristics of a white-light supercontinuum （SC） generated by a 800-nm, 160-fs laser pulse in a 4-mm thick Al2O3 crystal. Two orders of diffraction signals of SC by fs LITG in CS2 are observed, demonstrating that both the third-order process and the fifth-order process are present simultaneously. The experimental results also imply that the formation of an fs transient refractive-index grating in CS2 is mainly due to the electronic polarization process.展开更多
Time-and frequency-resolved broadband transient grating(BB-TG) spectroscopy is used to distinguish between ground-and excite-electronic state vibrational coherence at different wavelengths. Qualitative theoretical ana...Time-and frequency-resolved broadband transient grating(BB-TG) spectroscopy is used to distinguish between ground-and excite-electronic state vibrational coherence at different wavelengths. Qualitative theoretical analysis using double-sided Feynman diagrams indicates that a superposition of ground and excited state vibrational coherence are contained in the ground state absorption(GSA) and stimulated emission(SE) overlap band, while only the excited state is contained in the excited state absorption(ESA) band. The TG experiment, in which a white light continuum(WLC) is adopted as a probe, is conducted with rhodamine101(Rh101~+) as the target molecule. Fourier analysis of TG dynamics in a positive delay time range at specific wavelengths enables us to distinguish the low-frequency vibrational modes of Rh101 in ground-and excite-electronic states.展开更多
Multiple exciton generation （MEG） dynamics in colloidal PbS quantum dots （QDs） characterized with an im- proved transient grating （TG） technique will be reported. Only one peak soon after optical absorption and ...Multiple exciton generation （MEG） dynamics in colloidal PbS quantum dots （QDs） characterized with an im- proved transient grating （TG） technique will be reported. Only one peak soon after optical absorption and a fast decay within 1 ps can be observed in the TG kinetics when the photon energy of the pump light hv is smaller than 2.7Eg （Eg： band gap between LUMO and HOMO in the QDs）, which corresponds to hot carrier cooling. When hv is greater than 2.7Eg, however, after the initial peak, the TG signal decreases first and soon increases, and then a new peak appears at about 2 to 3 ps. The initial peak and the new peak correspond to hot carriers at the higher excited state and MEG at the lowest excited state, respectively. By proposing a theoretical model, we can calculate the hot carrier cooling time constant and MEG occurrence time constant quantitatively. When MEG does not happen for hv smaller than 2.7Eg, hot carrier cools with a time con- stant of 400 fs. When MEG occurs for hv larger than 2.7Eg, hot carrier cools with a time constant as small as 200 fs, while MEG occurs with a time constant of 600 fs. The detailed hot carrier cooling and MEG occurrence dynamics characterized in this work would shed light on the further understanding of MEG mechanism of various type of semiconductor QDs.展开更多
We demonstrate an all-optical technique for in situ monitoring of strong-field ionization(SFI)dynamics.The method relies on coherent scattering of a probe pulse from a transient plasma grating(TPG)formed by two interf...We demonstrate an all-optical technique for in situ monitoring of strong-field ionization(SFI)dynamics.The method relies on coherent scattering of a probe pulse from a transient plasma grating(TPG)formed by two interfering femtosecond pulses in a gas target.The diffracted signal provides a real-time,relative measure of the ionization yield.We demonstrate the method’s sensitivity by resolving the attosecond-scale coherent control of the ionization rate.Unlike conventional diagnostics that directly measure charged particles,our ensemble-based optical method is non-invasive and particularly suited for non-vacuum environments.To demonstrate its utility,we apply the technique to investigate the relationship between ionization and terahertz(THz)generation in a two-color(ω+2ω)field.We measure a phase offset of(0.18±0.05)π between the maxima of the ionization yield and the THz emission.This result provides a quantitative benchmark for theoretical models and establishes the TPG technique as a practical tool for probing SFI dynamics in ensemble systems.展开更多
This paper uses finite element method to obtain the three-dimensional temperature field of laser-induced transient thermal grating （TTG） for two-layered structure of diamond film on ZnSe substrate. The numerical res...This paper uses finite element method to obtain the three-dimensional temperature field of laser-induced transient thermal grating （TTG） for two-layered structure of diamond film on ZnSe substrate. The numerical results indicate that unique two-times heating process is gradually experienced in the area between two adjacent grating stripes. However, there is a little change for the temperature field along the depth direction for the diamond film due to its great thermal conductivity. It further finds that the thickness of the diamond film has a significant influence on the temperature field in diamond/ZnSe system. The results are useful for the application of laser-induced TTG technique in film/substrate system.展开更多
Femtosecond time-resolved transient grating technique was adopted to insight into the intra-chain exciton diffusion of MEH-PPV in solution with different polarity. Broadband white-light continuum was introduced as the...Femtosecond time-resolved transient grating technique was adopted to insight into the intra-chain exciton diffusion of MEH-PPV in solution with different polarity. Broadband white-light continuum was introduced as the probe to observe the transient absorption and the femtosecond time-resolved transient grating information simultaneously. The vibrational dephasing behaviors, single exciton relaxation, and population relaxation dynamics of MEH-PPV were systematically investigated. The result shows that the relaxation processes of the sample solution will be accelerated in the solvent with larger polarity.展开更多
基金Project supported by the National Natural Science Foundation of China(Grant Nos.21003033 and 21203047)the Guangxi Provincial Natural Science Foundation,China(Grant Nos.2012GXNSFBA053012 and 2014GXNSFAA118019)the Research Foundation of Education Bureau of Guangxi Zhuang Autonomous Region,China(Grant No.ZD2014127)
文摘Photo-induced intramolecular electron transfer （PIET） and intramolecular vibrational relaxation （IVR） dynamics of the excited state of rhodamine 6G （Rh6G＋） in DMSO are investigated by multiplex transient grating. Two major compo- nents are resolved in the dynamics of Rh6G＋. The first component, with a lifetime τTPIET = 140 fs-260 fs, is attributed to PIET from the phenyl ring to the xanthene plane. The IVR process occurring in the range ZIVR = 3.3 ps-5.2 ps is much slower than the first component. The PIET and IVR processes occurring in the excited state of Rh6G＋ are quantitatively determined, and a better understanding of the relationship between these processes is obtained.
基金supported by the National Natural Science Foundation of China(Grant Nos.11304058 and 11404307)NSAF(Grant No.U1330106)
文摘Femtosecond time-resolved transient grating(TG) technique is used to study the intermolecular dynamics in liquid phase. Non-resonant excitation of the sample by two crossing laser pulses results in a transient Kerr grating, and the molecular motion of liquid can be detected by monitoring the diffraction of a third time-delayed probe pulse. In liquid nitrobenzene(NB), three intermolecular processes are observed with lifetimes of 37.9±1.4 ps, 3.28±0.11 ps, and 0.44±0.03 ps, respectively. These relaxations are assigned to molecular orientational diffusion, dipole/induced dipole interaction, and libration in liquid cage, respectively. Such a result is slightly different from that obtained from OKE experiment in which the lifetime of the intermediate process is measured to be 1.9 ps. The effects of electric field on matter are different in TG and optical Kerr effect(OKE) experiments, which should be responsible for the difference between the results of these two types of experiments. The present work demonstrates that TG technique is a useful alternative in the study of intermolecular dynamics.
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 20973050 and 10904023)
文摘Experiments on fs laser-induced transient grating （LITG） in carbon bisulfide （CS2） are carried out to explore the chirp characteristics of a white-light supercontinuum （SC） generated by a 800-nm, 160-fs laser pulse in a 4-mm thick Al2O3 crystal. Two orders of diffraction signals of SC by fs LITG in CS2 are observed, demonstrating that both the third-order process and the fifth-order process are present simultaneously. The experimental results also imply that the formation of an fs transient refractive-index grating in CS2 is mainly due to the electronic polarization process.
基金Project supported by the Science Challenge Project,China(Grant No.TZ2016001)the National Natural Science Foundation of China(Grant No.21673211)
文摘Time-and frequency-resolved broadband transient grating(BB-TG) spectroscopy is used to distinguish between ground-and excite-electronic state vibrational coherence at different wavelengths. Qualitative theoretical analysis using double-sided Feynman diagrams indicates that a superposition of ground and excited state vibrational coherence are contained in the ground state absorption(GSA) and stimulated emission(SE) overlap band, while only the excited state is contained in the excited state absorption(ESA) band. The TG experiment, in which a white light continuum(WLC) is adopted as a probe, is conducted with rhodamine101(Rh101~+) as the target molecule. Fourier analysis of TG dynamics in a positive delay time range at specific wavelengths enables us to distinguish the low-frequency vibrational modes of Rh101 in ground-and excite-electronic states.
基金supported by MEXT KAKENHI Grant no. 26286013the PRESTO program Photoenergy conversion systems and materials for the next generation solar cells,Japan Science and Technology Agency (JST)
文摘Multiple exciton generation （MEG） dynamics in colloidal PbS quantum dots （QDs） characterized with an im- proved transient grating （TG） technique will be reported. Only one peak soon after optical absorption and a fast decay within 1 ps can be observed in the TG kinetics when the photon energy of the pump light hv is smaller than 2.7Eg （Eg： band gap between LUMO and HOMO in the QDs）, which corresponds to hot carrier cooling. When hv is greater than 2.7Eg, however, after the initial peak, the TG signal decreases first and soon increases, and then a new peak appears at about 2 to 3 ps. The initial peak and the new peak correspond to hot carriers at the higher excited state and MEG at the lowest excited state, respectively. By proposing a theoretical model, we can calculate the hot carrier cooling time constant and MEG occurrence time constant quantitatively. When MEG does not happen for hv smaller than 2.7Eg, hot carrier cools with a time con- stant of 400 fs. When MEG occurs for hv larger than 2.7Eg, hot carrier cools with a time constant as small as 200 fs, while MEG occurs with a time constant of 600 fs. The detailed hot carrier cooling and MEG occurrence dynamics characterized in this work would shed light on the further understanding of MEG mechanism of various type of semiconductor QDs.
基金supported by the NUDT Science Foundation for Indigenous Innovation(Grant No.24-ZZCX-ZXGC-15)the National Natural Science Foundation of China(Grant Nos.12234020,12450403,and 12374263)。
文摘We demonstrate an all-optical technique for in situ monitoring of strong-field ionization(SFI)dynamics.The method relies on coherent scattering of a probe pulse from a transient plasma grating(TPG)formed by two interfering femtosecond pulses in a gas target.The diffracted signal provides a real-time,relative measure of the ionization yield.We demonstrate the method’s sensitivity by resolving the attosecond-scale coherent control of the ionization rate.Unlike conventional diagnostics that directly measure charged particles,our ensemble-based optical method is non-invasive and particularly suited for non-vacuum environments.To demonstrate its utility,we apply the technique to investigate the relationship between ionization and terahertz(THz)generation in a two-color(ω+2ω)field.We measure a phase offset of(0.18±0.05)π between the maxima of the ionization yield and the THz emission.This result provides a quantitative benchmark for theoretical models and establishes the TPG technique as a practical tool for probing SFI dynamics in ensemble systems.
基金Project supported by the National Natural Science Foundation of China (Grant Nos 10374041 and 10574071)
文摘This paper uses finite element method to obtain the three-dimensional temperature field of laser-induced transient thermal grating （TTG） for two-layered structure of diamond film on ZnSe substrate. The numerical results indicate that unique two-times heating process is gradually experienced in the area between two adjacent grating stripes. However, there is a little change for the temperature field along the depth direction for the diamond film due to its great thermal conductivity. It further finds that the thickness of the diamond film has a significant influence on the temperature field in diamond/ZnSe system. The results are useful for the application of laser-induced TTG technique in film/substrate system.
基金supported by the National Natural Science Foundation of China(No.61704120)Science & Technology Development Foundation of Tianjin Higher Education Institutions(No.20140904)
文摘Femtosecond time-resolved transient grating technique was adopted to insight into the intra-chain exciton diffusion of MEH-PPV in solution with different polarity. Broadband white-light continuum was introduced as the probe to observe the transient absorption and the femtosecond time-resolved transient grating information simultaneously. The vibrational dephasing behaviors, single exciton relaxation, and population relaxation dynamics of MEH-PPV were systematically investigated. The result shows that the relaxation processes of the sample solution will be accelerated in the solvent with larger polarity.
