鉴于国内核物理实验对高性能硅探测器有大量需求,而国外对中国进行技术封锁,满足实验需求的高性能探测器不易获得.中国科学院近代物理研究所在原有制备工艺基础上首次采用套刻技术,有效减少了光刻及腐蚀过程造成的Si O2沾污,大幅提高了...鉴于国内核物理实验对高性能硅探测器有大量需求,而国外对中国进行技术封锁,满足实验需求的高性能探测器不易获得.中国科学院近代物理研究所在原有制备工艺基础上首次采用套刻技术,有效减少了光刻及腐蚀过程造成的Si O2沾污,大幅提高了探测器性能和成品率.本文对采用该工艺研制的300μm厚,有效面积50 mm×50 mm硅探测器进行电学性能测试和在束探测性能测试.探测器在-45 V耗尽电压下,其漏电流小于40 n A,对5 Me V左右的a粒子的能量分辨(σ)约为45 ke V.将该探测器作为能量沉积(ΔE)探测器,利用250 Me V/u的11C放射性束流及其在次级碳靶上的反应产物对探测器进行了探测性能测试.测试结果显示,该探测器对于C元素的电荷数Z的分辨为0.17,与文献中记录的国外生产的同类型探测器的实验数据(Z分辨0.19)相当,可以满足中高能放射性束实验对轻质量区粒子鉴别的要求.展开更多
Junctions are an important structure that allows charge separation in solar cells and photocatalysts. Here, we studied the charge transfer at an anatase/rutile TiO2 phase junction using time-resolved photoluminescence...Junctions are an important structure that allows charge separation in solar cells and photocatalysts. Here, we studied the charge transfer at an anatase/rutile TiO2 phase junction using time-resolved photoluminescence spectroscopy. Visible （-S00 nm） and near-infrared （NIR, -830 nm） emissions were monitored to give insight into the photoinduced charges of anatase and rutile in the junction, respectively, New fast photoluminescence decay components appeared in the visible emission of futile-phase dominated TiO2 and in the NIR emission of many mixed phase TiO2samples. The fast decays confirmed that the charge separation occurred at the phase junction. The visible emission intensity from the mixed phase TiO2 increased, revealing that charge transfer from rutile to anatase was the main pathway. The charge separation slowed the microsecond time scale photolumines- cence decay rate for charge carriers in both anatase and rutile. However, the millisecond decay of the charge carriers in anatase TiO2 was accelerated, while there was almost no change in the charge carrier dynamics of rutile TiO2. Thus, charge separation at the anatase/rutile phase junction caused an increase in the charge carrier concentration on a microsecond time scale, because of slower electron-hole recombination. The enhanced photocatalytic activity previously observed at ana- tase/rutile phase junctions is likely caused by the improved charge carrier dynamics we report here. These findings may contribute to the development of improved photocatalytic materials.展开更多
The function of protein in long-range biological electron transfer is a question of debate. We report some preliminary results in femtosecond spectroscopic study of photosynthetic bacterial light-harvesting antenna co...The function of protein in long-range biological electron transfer is a question of debate. We report some preliminary results in femtosecond spectroscopic study of photosynthetic bacterial light-harvesting antenna complex assembled onto TiO2 nanoparticle with an average size of 8 nm in diameter. Crystal structure shows that photosynthetic bacterial antenna complex LH2 has a ring-like structure composed by alpha- and beta-apoprotein helices. The alpha- and beta-transmembrance helices construct two concentric cylinders with pigments bacteriochlorophyll a (Bchl a) and carotenoid (Car) buried inside the protein. We attempt to insert TiO2 nanoparticle into the cavity of the inner cylindrical hollow of LH2 to investigate the nature of the electron transfer between the excited-state Bchl a and the TiO2 nanoparticle. A significant decrease in the ground state bleaching recovery time constant for Bchl a at 850 run (B850) in respect to that of the Bchl a in free LH2 has been observed. By using the relation of distance-dependent long-range electron transfer rate in protein, the distance between the donor B850 and the acceptor TiO2 nanoparticle has been estimated, which is about 0.6 nm. The proposed method of assembling proteins onto wide-gap semiconductor nanoparticle can be a promising way to determine the role of the protein playing in biological electron transfer processes.展开更多
The structure-property characteristics of a series of newly synthesized intramolecular charge- transfer （ICT） compounds, single-branch monomer with triphenylmethane as electron donor and 2,1,3-benzothiadiazole as ac...The structure-property characteristics of a series of newly synthesized intramolecular charge- transfer （ICT） compounds, single-branch monomer with triphenylmethane as electron donor and 2,1,3-benzothiadiazole as acceptor, the corresponding two-branch dimer and three- branch trimer, have been investigated by means of steady-state and femtosecond time- resolved stimulated emission fluorescence depletion （FS TR-SEP FD） techniques in different polar solvents. The TD-DFT calculations are further performed to explain the observed ICT properties. The interpretation of the experimental results is based on the comparative studies of the series of compounds which have increased amount of identical branch moiety. The similarity of the absorption and fluorescence spectra as well as strong solvent-dependence of the spectral properties for the three compounds reveal that the excited state of the dimer and trimer are nearly the same with that of the monomer, which may localize on one branch. It is found that polar excited state emerged through multidimensional intramolecular charge transfer from the donating moiety to the acceptor upon excitation, and quickly relaxed to one branch before emission. Even so, the red-shift in the absorption and emission spectra and decreased fluorescence radiative lifetime with respect to their monomer counterpart still suggest some extent delocalization of excited state in the dimer and trimer upon excitation. The similar behavior of their excited ICT state is demonstrated by FS TR-SEP FD measurements, and shows that the trimer has the largest charge-separate extent in all studied three samples. Finally, steady-state excitation anisotropy measurements has further been carried out to estimate the nature of the optical excitation and the mechanism of energy redistribution among the branches, where no plateau through the ICT band suggests the intramolecular excitation transfer process between the branches in dimer and trimer.展开更多
Investigation of the charge dynamics and roles of cocatalysts is crucial for understanding the reaction of photocatalytic water splitting on semiconductor photocatalysts.In this work,the dynamics of photogenerated ele...Investigation of the charge dynamics and roles of cocatalysts is crucial for understanding the reaction of photocatalytic water splitting on semiconductor photocatalysts.In this work,the dynamics of photogenerated electrons in Ga_(2)O_(3) loaded with Cr_(2)O_(3)-Rh cocatalysts was studied using time-resolved mid-infrared spectroscopy.The structure of these Cr_(2)O_(3)-Rh cocatalysts was identified with high-resolution transmission electron microscopy and CO adsorption Fourier-transform infrared spectroscopy,as Rh particles partly covered with Cr_(2)O_(3).The decay dynamics of photogenerated electrons reveals that only the electrons trapped by the Rh particles efficiently participate in the H2 evolution reaction.The loaded Cr_(2)O_(3) promotes electron transfer from Ga_(2)O_(3) to Rh,which accelerates the electron-consuming reaction for H2 evolution.Based on these observations,a photocatalytic water-splitting mechanism for Cr_(2)O_(3)-Rh/Ga_(2)O_(3) photocatalysts has been proposed.The elucidation of the roles of the Cr_(2)O_(3)-Rh cocatalysts aids in further understanding the reaction mechanisms of photocatalytic water splitting and guiding the development of improved photocatalysts.展开更多
CdZnTe is an excellent material candidate for high efficiency,high-resolution room-temperature nuclear radiation detectors,and the CdZnTe detectors are being widely used in medicine,industry,safeguard and scientific X...CdZnTe is an excellent material candidate for high efficiency,high-resolution room-temperature nuclear radiation detectors,and the CdZnTe detectors are being widely used in medicine,industry,safeguard and scientific X-ray and γ-ray imaging and spectroscopic applications.In this work,three CdZnTe planar detectors with different grades,named CZT-1,CZT-2 and CZT-3,respectively,were fabricated.And the effects of mobility,lifetime and de-trapping time on the performance of CdZnTe planar detector,such as the energy resolution,charge collection efficiency and peak to valley ratio,were analyzed.The charge collection efficiency depends on the product of carrier mobility and lifetime,which has a great effect on the energy resolution of detector when the efficiency is less than 90%.The de-trapping time of carriers in deep levels should be responsible for the peak to valley ratio and "polarization".展开更多
Fabry-Perot Interferometer(FPI) has been used widely for wind measurements of the middle and upper atmosphere.To date, most of FPIs have been based on full-closed circular fringe, which needs 15–25 min to obtain a gr...Fabry-Perot Interferometer(FPI) has been used widely for wind measurements of the middle and upper atmosphere.To date, most of FPIs have been based on full-closed circular fringe, which needs 15–25 min to obtain a group of wind velocity(zonal and meridional). However, it is hard to improve the temporal resolution because full-closed circular fringe in several directions cannot be easily imaged onto the same Charge-Coupled Device(CCD) with enough airglow intensity. In this paper, a data processing method is proposed for non-full circular fringe of FPI, which can support CCD with enough area of observations in several directions simultaneously. The method is focused on the center determination of non-full fringe. It includes radial cross-section, peak coordinate determination, and center calculation. Based on the calculated center, the fringe is annular summed. Then its radius is determined subsequently using Gaussian fitting. Finally, the wind is retrieved from the fringe radius. For validation, fringes from two ground-based FPIs were used, which are deployed in Kelan(38.71°N, 111.58°E) and Xinglong(40.40°N, 117.59°E) in China. The results retrieved from non-full fringes of FPIs were compared with that from full-closed circular fringe. The averaged wind deviation between them demonstrates reasonable difference with 5.38 ms^-(1) for 892.0 nm airglow emission, 5.81 ms^-(1) for 630.0 nm emission, and 3.03 ms^-(1) for 557.7 nm emission. Besides, wind results of Xinglong FPI are compared roughly with measurements of meteor radar which is deployed in Ming Tombs of Beijing(40.3°N,116.2°E). Good agreement demonstrates that this method is robust enough for FPI wind retrieval of mesosphere and thermosphere.展开更多
文摘鉴于国内核物理实验对高性能硅探测器有大量需求,而国外对中国进行技术封锁,满足实验需求的高性能探测器不易获得.中国科学院近代物理研究所在原有制备工艺基础上首次采用套刻技术,有效减少了光刻及腐蚀过程造成的Si O2沾污,大幅提高了探测器性能和成品率.本文对采用该工艺研制的300μm厚,有效面积50 mm×50 mm硅探测器进行电学性能测试和在束探测性能测试.探测器在-45 V耗尽电压下,其漏电流小于40 n A,对5 Me V左右的a粒子的能量分辨(σ)约为45 ke V.将该探测器作为能量沉积(ΔE)探测器,利用250 Me V/u的11C放射性束流及其在次级碳靶上的反应产物对探测器进行了探测性能测试.测试结果显示,该探测器对于C元素的电荷数Z的分辨为0.17,与文献中记录的国外生产的同类型探测器的实验数据(Z分辨0.19)相当,可以满足中高能放射性束实验对轻质量区粒子鉴别的要求.
基金supported by the National Natural Science Foundation of China (21203185, 21373209)the National Basic Research Program of China (2014CB239400)
文摘Junctions are an important structure that allows charge separation in solar cells and photocatalysts. Here, we studied the charge transfer at an anatase/rutile TiO2 phase junction using time-resolved photoluminescence spectroscopy. Visible （-S00 nm） and near-infrared （NIR, -830 nm） emissions were monitored to give insight into the photoinduced charges of anatase and rutile in the junction, respectively, New fast photoluminescence decay components appeared in the visible emission of futile-phase dominated TiO2 and in the NIR emission of many mixed phase TiO2samples. The fast decays confirmed that the charge separation occurred at the phase junction. The visible emission intensity from the mixed phase TiO2 increased, revealing that charge transfer from rutile to anatase was the main pathway. The charge separation slowed the microsecond time scale photolumines- cence decay rate for charge carriers in both anatase and rutile. However, the millisecond decay of the charge carriers in anatase TiO2 was accelerated, while there was almost no change in the charge carrier dynamics of rutile TiO2. Thus, charge separation at the anatase/rutile phase junction caused an increase in the charge carrier concentration on a microsecond time scale, because of slower electron-hole recombination. The enhanced photocatalytic activity previously observed at ana- tase/rutile phase junctions is likely caused by the improved charge carrier dynamics we report here. These findings may contribute to the development of improved photocatalytic materials.
文摘The function of protein in long-range biological electron transfer is a question of debate. We report some preliminary results in femtosecond spectroscopic study of photosynthetic bacterial light-harvesting antenna complex assembled onto TiO2 nanoparticle with an average size of 8 nm in diameter. Crystal structure shows that photosynthetic bacterial antenna complex LH2 has a ring-like structure composed by alpha- and beta-apoprotein helices. The alpha- and beta-transmembrance helices construct two concentric cylinders with pigments bacteriochlorophyll a (Bchl a) and carotenoid (Car) buried inside the protein. We attempt to insert TiO2 nanoparticle into the cavity of the inner cylindrical hollow of LH2 to investigate the nature of the electron transfer between the excited-state Bchl a and the TiO2 nanoparticle. A significant decrease in the ground state bleaching recovery time constant for Bchl a at 850 run (B850) in respect to that of the Bchl a in free LH2 has been observed. By using the relation of distance-dependent long-range electron transfer rate in protein, the distance between the donor B850 and the acceptor TiO2 nanoparticle has been estimated, which is about 0.6 nm. The proposed method of assembling proteins onto wide-gap semiconductor nanoparticle can be a promising way to determine the role of the protein playing in biological electron transfer processes.
基金We sincerely thank Prof. Yong-fang Li for providing the samples. S. Vdovi5 thanks CAS for support through a CAS Research Fellowship for International Young Researchers. This work was supported by National Natural Science Foundation of China, the Chinese Academy of Sciences, and the State Key Project for Fundamental Research.
文摘The structure-property characteristics of a series of newly synthesized intramolecular charge- transfer （ICT） compounds, single-branch monomer with triphenylmethane as electron donor and 2,1,3-benzothiadiazole as acceptor, the corresponding two-branch dimer and three- branch trimer, have been investigated by means of steady-state and femtosecond time- resolved stimulated emission fluorescence depletion （FS TR-SEP FD） techniques in different polar solvents. The TD-DFT calculations are further performed to explain the observed ICT properties. The interpretation of the experimental results is based on the comparative studies of the series of compounds which have increased amount of identical branch moiety. The similarity of the absorption and fluorescence spectra as well as strong solvent-dependence of the spectral properties for the three compounds reveal that the excited state of the dimer and trimer are nearly the same with that of the monomer, which may localize on one branch. It is found that polar excited state emerged through multidimensional intramolecular charge transfer from the donating moiety to the acceptor upon excitation, and quickly relaxed to one branch before emission. Even so, the red-shift in the absorption and emission spectra and decreased fluorescence radiative lifetime with respect to their monomer counterpart still suggest some extent delocalization of excited state in the dimer and trimer upon excitation. The similar behavior of their excited ICT state is demonstrated by FS TR-SEP FD measurements, and shows that the trimer has the largest charge-separate extent in all studied three samples. Finally, steady-state excitation anisotropy measurements has further been carried out to estimate the nature of the optical excitation and the mechanism of energy redistribution among the branches, where no plateau through the ICT band suggests the intramolecular excitation transfer process between the branches in dimer and trimer.
文摘Investigation of the charge dynamics and roles of cocatalysts is crucial for understanding the reaction of photocatalytic water splitting on semiconductor photocatalysts.In this work,the dynamics of photogenerated electrons in Ga_(2)O_(3) loaded with Cr_(2)O_(3)-Rh cocatalysts was studied using time-resolved mid-infrared spectroscopy.The structure of these Cr_(2)O_(3)-Rh cocatalysts was identified with high-resolution transmission electron microscopy and CO adsorption Fourier-transform infrared spectroscopy,as Rh particles partly covered with Cr_(2)O_(3).The decay dynamics of photogenerated electrons reveals that only the electrons trapped by the Rh particles efficiently participate in the H2 evolution reaction.The loaded Cr_(2)O_(3) promotes electron transfer from Ga_(2)O_(3) to Rh,which accelerates the electron-consuming reaction for H2 evolution.Based on these observations,a photocatalytic water-splitting mechanism for Cr_(2)O_(3)-Rh/Ga_(2)O_(3) photocatalysts has been proposed.The elucidation of the roles of the Cr_(2)O_(3)-Rh cocatalysts aids in further understanding the reaction mechanisms of photocatalytic water splitting and guiding the development of improved photocatalysts.
基金supported by the National Instrumentation Program (GrantNo. 2011YQ040082)the National Natural Science Foundation of China(Grant Nos. 50902113,50902114)+3 种基金Program for New Century Excellent Talents in University (Grant No. NCET-10-0076)the National Basic Research Program of China ("973" Project) (Grant No. 2011CB610406)the"111" Project of China (Grant No. B08040)NPU Foundation for Fundamental Research (Grant No. JC20100228)
文摘CdZnTe is an excellent material candidate for high efficiency,high-resolution room-temperature nuclear radiation detectors,and the CdZnTe detectors are being widely used in medicine,industry,safeguard and scientific X-ray and γ-ray imaging and spectroscopic applications.In this work,three CdZnTe planar detectors with different grades,named CZT-1,CZT-2 and CZT-3,respectively,were fabricated.And the effects of mobility,lifetime and de-trapping time on the performance of CdZnTe planar detector,such as the energy resolution,charge collection efficiency and peak to valley ratio,were analyzed.The charge collection efficiency depends on the product of carrier mobility and lifetime,which has a great effect on the energy resolution of detector when the efficiency is less than 90%.The de-trapping time of carriers in deep levels should be responsible for the peak to valley ratio and "polarization".
基金supported by National Space Science Center (Xinglong FPI data)Institute of Geology and Geophysics (meteor radar data)Beijing Municipal Science and Technology Commission (Grant No. Z151100003615001)
文摘Fabry-Perot Interferometer(FPI) has been used widely for wind measurements of the middle and upper atmosphere.To date, most of FPIs have been based on full-closed circular fringe, which needs 15–25 min to obtain a group of wind velocity(zonal and meridional). However, it is hard to improve the temporal resolution because full-closed circular fringe in several directions cannot be easily imaged onto the same Charge-Coupled Device(CCD) with enough airglow intensity. In this paper, a data processing method is proposed for non-full circular fringe of FPI, which can support CCD with enough area of observations in several directions simultaneously. The method is focused on the center determination of non-full fringe. It includes radial cross-section, peak coordinate determination, and center calculation. Based on the calculated center, the fringe is annular summed. Then its radius is determined subsequently using Gaussian fitting. Finally, the wind is retrieved from the fringe radius. For validation, fringes from two ground-based FPIs were used, which are deployed in Kelan(38.71°N, 111.58°E) and Xinglong(40.40°N, 117.59°E) in China. The results retrieved from non-full fringes of FPIs were compared with that from full-closed circular fringe. The averaged wind deviation between them demonstrates reasonable difference with 5.38 ms^-(1) for 892.0 nm airglow emission, 5.81 ms^-(1) for 630.0 nm emission, and 3.03 ms^-(1) for 557.7 nm emission. Besides, wind results of Xinglong FPI are compared roughly with measurements of meteor radar which is deployed in Ming Tombs of Beijing(40.3°N,116.2°E). Good agreement demonstrates that this method is robust enough for FPI wind retrieval of mesosphere and thermosphere.
