In this paper, TitaiJum dioxide （TiO2） rutile single crystal was irradiated by infrared femtosecond laser pulses with repetition rate of 250 kHz. For a P-polarized femtosecond laser, the periodic nanograting structu...In this paper, TitaiJum dioxide （TiO2） rutile single crystal was irradiated by infrared femtosecond laser pulses with repetition rate of 250 kHz. For a P-polarized femtosecond laser, the periodic nanograting structure on the ablation crater surface was formed . The periodicity is much less than the laser wavelength. The direction of nanograting alignment depends on the polarization laser beam. Micro-Raman spectra show that the intensity of Eg Raman vibrating mode of rutile phase increases and that of Alg Raman vibrating mode decreases apparently within the ablation crater. With the increase of irradiation time and laser average power, the Raman vibrating modes of anatase phase emerged. Rutile phase of TiO2 single crystal is partly transformed into anatase phase.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
Over the past decade the integration of ultrafast spectroscopy with nanoscience has greatly propelled the development of nanoscience, as the key information gleaned from the mechanistic studies with the assistance of ...Over the past decade the integration of ultrafast spectroscopy with nanoscience has greatly propelled the development of nanoscience, as the key information gleaned from the mechanistic studies with the assistance of ultrafast spectroscopy enables a deeper understanding of the structure–function interplay and various interactions involved in the nanosystems.This mini-review presents an overview of the recent advances achieved in our ultrafast spectroscopy laboratory that address the ultrafast dynamics and related mechanisms in several representative nanomaterial complex systems by means of femtosecond time-resolved transient absorption spectroscopy. We attempt to convey instructive, consistent information regarding the important processes, pathways, dynamics, and interactions involved in the nanomaterial complex systems,most of which exhibit excellent performance in photocatalysis.展开更多
Optical properties and ultrafast exciton relaxation dynamics in PbS and core/shell PbS/CdS quantum dots(QDs) have been studied using UV-vis absorption and fluorescence spectroscopy as well as femtosecond(fs) transient...Optical properties and ultrafast exciton relaxation dynamics in PbS and core/shell PbS/CdS quantum dots(QDs) have been studied using UV-vis absorption and fluorescence spectroscopy as well as femtosecond(fs) transient absorption spectroscopy.The electronic absorption spectrum of the PbS QDs features broad absorption in the entire near IR-vis-UV region with a monotonic increase in intensity towards shorter wavelength.Relative to PbS,the absorption of the core/shell PbS/CdS QDs shows a slight blue shift in the 600?800 nm region,due to the decrease of the PbS crystal size caused by the synthetic process of the core/shell structure,and increased absorption near 400 nm due to the CdS shell.The PL of the PbS/CdS QDs was ~2.6 times more intense than that of the PbS QDs,due to surface passivation of PbS by CdS,and blue-shifted,attributable to smaller PbS size and thereby stronger quantum confinement in the core/shell QDs.Fs transient absorption measurements of both systems showed a strong transient absorption feature from 600 to 750 nm following excitation at 750 nm.The transient absorption decays can be fit to a biexponential with time constants of 8 and 100 ps for PbS and 6 and 80 ps for PbS/CdS.The amplitude and lifetime of the fast component were excitation intensity dependent,with the amplitude increasing more than linearly with increasing excitation intensity and the lifetime decreasing with increasing intensity.The fast decay is attributed to exciton-exciton annihilation and it occurs more readily for the PbS/CdS than the PbS QDs,which is attributed to a lower density of trap states in the core/shell QDs,as supported by their stronger PL.展开更多
基金Project supported by Shanghai Leading Academic Discipline Project, China （Grant No T0104）, the Shanghai Nano-technology Promotion Center and Science ＆ Technology of Shanghai Municipality, China （Grant No 0652nm005）, Science Foundation of Shanghai Municipal Commission Education and Science and Technology Commission of Shanghai Municipal, China （Grant No 06PJ14042）.
文摘In this paper, TitaiJum dioxide （TiO2） rutile single crystal was irradiated by infrared femtosecond laser pulses with repetition rate of 250 kHz. For a P-polarized femtosecond laser, the periodic nanograting structure on the ablation crater surface was formed . The periodicity is much less than the laser wavelength. The direction of nanograting alignment depends on the polarization laser beam. Micro-Raman spectra show that the intensity of Eg Raman vibrating mode of rutile phase increases and that of Alg Raman vibrating mode decreases apparently within the ablation crater. With the increase of irradiation time and laser average power, the Raman vibrating modes of anatase phase emerged. Rutile phase of TiO2 single crystal is partly transformed into anatase phase.
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support from the National Natural Science Foundation of China (21573211 and 21421063)the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB01020200)the Fundamental Research Funds for the Central Universities of China (WK2340000063)
文摘Over the past decade the integration of ultrafast spectroscopy with nanoscience has greatly propelled the development of nanoscience, as the key information gleaned from the mechanistic studies with the assistance of ultrafast spectroscopy enables a deeper understanding of the structure–function interplay and various interactions involved in the nanosystems.This mini-review presents an overview of the recent advances achieved in our ultrafast spectroscopy laboratory that address the ultrafast dynamics and related mechanisms in several representative nanomaterial complex systems by means of femtosecond time-resolved transient absorption spectroscopy. We attempt to convey instructive, consistent information regarding the important processes, pathways, dynamics, and interactions involved in the nanomaterial complex systems,most of which exhibit excellent performance in photocatalysis.
基金supported by the Basic Energy Sciences Division of the US DOE (DE-FG02-ER46232)
文摘Optical properties and ultrafast exciton relaxation dynamics in PbS and core/shell PbS/CdS quantum dots(QDs) have been studied using UV-vis absorption and fluorescence spectroscopy as well as femtosecond(fs) transient absorption spectroscopy.The electronic absorption spectrum of the PbS QDs features broad absorption in the entire near IR-vis-UV region with a monotonic increase in intensity towards shorter wavelength.Relative to PbS,the absorption of the core/shell PbS/CdS QDs shows a slight blue shift in the 600?800 nm region,due to the decrease of the PbS crystal size caused by the synthetic process of the core/shell structure,and increased absorption near 400 nm due to the CdS shell.The PL of the PbS/CdS QDs was ~2.6 times more intense than that of the PbS QDs,due to surface passivation of PbS by CdS,and blue-shifted,attributable to smaller PbS size and thereby stronger quantum confinement in the core/shell QDs.Fs transient absorption measurements of both systems showed a strong transient absorption feature from 600 to 750 nm following excitation at 750 nm.The transient absorption decays can be fit to a biexponential with time constants of 8 and 100 ps for PbS and 6 and 80 ps for PbS/CdS.The amplitude and lifetime of the fast component were excitation intensity dependent,with the amplitude increasing more than linearly with increasing excitation intensity and the lifetime decreasing with increasing intensity.The fast decay is attributed to exciton-exciton annihilation and it occurs more readily for the PbS/CdS than the PbS QDs,which is attributed to a lower density of trap states in the core/shell QDs,as supported by their stronger PL.
