A review is presented of studies of polymeric membranes by applying positron annihilation lifetime spectroscopy (PALS). PALS has been used to study subnanometer-sized holes, to determine their size distribution and ...A review is presented of studies of polymeric membranes by applying positron annihilation lifetime spectroscopy (PALS). PALS has been used to study subnanometer-sized holes, to determine their size distribution and free-volume fractions, and to probe molecular-sized vacancies in glassy polymers. At present, PALS is believed to be a highly effective physical method for the examination of polymeric membranes.展开更多
Fluorescence correlation spectroscopy (FCS) is a widely used method for measuring molecular diffusion and chemical kinetics. However, when a mixture of fluorescent species is taken into account, the conven- tional F...Fluorescence correlation spectroscopy (FCS) is a widely used method for measuring molecular diffusion and chemical kinetics. However, when a mixture of fluorescent species is taken into account, the conven- tional FCS method has limitations in extracting autocorrelations for different species and cross correla- tions between different species. Recently developed fluorescence lifetime correlation spectroscopy (FLCS) based on time-tagged time-resolved (TITR) photon recording, which can record the global and micro arrival time for each individual photon, has been used to discriminate different species according to fluorescence lifetime. Here, based on two-dimensional lifetime decay maps constructed from TITR photon stream, we have developed a quantitative lifetime-deconvolution FCS model (LDFCS) to extract precise chemical rates for chemical conversions in multi-species systems. The key point of LDFCS model is separation of different species according to the global distribution of fluorescence lifetime and then deconvolution of autocorrelations and cross-correlations from the two-dimensional lifetime decay maps constructed bv the micro arrival times of photon pairs at each delay time.展开更多
This paper presents the application of lifetime spectroscopy to the study of carrier-induced degradation ascribed to the boron-oxygen (BO) defect. Specifically, a large data set of p-type silicon samples is used to ...This paper presents the application of lifetime spectroscopy to the study of carrier-induced degradation ascribed to the boron-oxygen (BO) defect. Specifically, a large data set of p-type silicon samples is used to investigate two important aspects of carrier lifetime analysis: ① the methods used to extract the recombination lifetime associated with the defect and ② the underlying assumption that cartier injection does not affect lifetime components unrelated to the defect. The results demonstrate that the capture cross section ratio associated with the donor level of the BO defect (kl) vary widely depending on the specific method used to extract the defect-specific recombination lifetime. For the data set studied here, it was also found that illumination used to form the defect caused minor, but statistically significant changes in the surface passivation used. This violation of the fundamental assumption could be accounted for by applying appropriate curve fitting methods, resulting in an improved estimate of k1 (11.90±0.45) for the fully formed BO defect when modeled using the donor level alone. Illumination also appeared to cause a minor, apparently injectionindependent change in lifetime that could not be attributed to the donor level of the BO defect alone and is likely related to the acceptor level of the BO defect. While specific to the BO defect, this study has implications for the use of lifetime spectroscopy to study other carrier induced defects. Finally, we demonstrate the use of a unit-less regression goodness-of-fit metric for lifetime data that is easy to interpret and accounts for repeatability error.展开更多
To realize efficient atmospheric CO_(2) chemisorption and activation,abundant Ti^(3+) sites and oxygen vacancies in TiO_(2) ultrathin layers were designed.Positron annihilation lifetime spectroscopy and theoretical ca...To realize efficient atmospheric CO_(2) chemisorption and activation,abundant Ti^(3+) sites and oxygen vacancies in TiO_(2) ultrathin layers were designed.Positron annihilation lifetime spectroscopy and theoretical calculations first unveil each oxygen vacancy is associated with the formation of two Ti^(3+)sites,giving a Ti^(3+)-V_(o)-Ti^(3+) configuration.The Ti^(3+)-V_(o)-Ti^(3+) sites could bond with CO_(2) molecules to form a stable configuration,which converted the endoergic chemisorption step to an exoergic process,verified by in-situ Fourier-transform infrared spectra and theoretical calculations.Also,the adjacent Ti^(3+)sites not only favor CO_(2) activation into COOH*via forming a stable Ti^(3+)–C–O–Ti^(3+) configuration,but also facilitate the rate-limiting COOH^(*)scission to CO^(*)by reducing the energy barrier from 0.75 to 0.45 e V.Thus,the Ti^(3+)-V_(o)-TiO_(2) ultrathinlayers could directly capture and photofix atmospheric CO_(2) into near-unity CO,with the corresponding CO_(2)-to-CO conversion ratio of ca.20.2%.展开更多
Void swelling,which induces the degradation of the original properties of nuclear materials under high-energy particleirradiation,is an important problem.The incubation period,a transient stage before the steady void ...Void swelling,which induces the degradation of the original properties of nuclear materials under high-energy particleirradiation,is an important problem.The incubation period,a transient stage before the steady void growth,determines the duration of service of nuclear materials.Several experimental studies have been performed on void observations by transmission electron microscopy(TEM),which,however,has a resolution limit for the size of defect clusters.Positron annihilation lifetime spectroscopy(PALS)enables the detection of small vacancy clusters,single vacancies,dislocations and precipitates.The use of these two methods provides complementary information toward detecting defect information in the incubation period.Here,defect structures during the incubation period in austenitic stainless steels,by means of PALS and TEM are reviewed.The role of alloying elements into determining the period is explained.Furthermore,the existing problems and research directions in this field are presented.展开更多
基金The project supported by the Hundred-Persons Plan Foundation of Chinese Academy of Sciences in 2003
文摘A review is presented of studies of polymeric membranes by applying positron annihilation lifetime spectroscopy (PALS). PALS has been used to study subnanometer-sized holes, to determine their size distribution and free-volume fractions, and to probe molecular-sized vacancies in glassy polymers. At present, PALS is believed to be a highly effective physical method for the examination of polymeric membranes.
基金supported by ‘‘Strategic Priority Research Program” of Chinese Academy of Sciences (XDA09040300)Beijing Science and Technology Project (Z151100003915077)+1 种基金Beijing Nova Programme (Z151100000315081)Beijing Talents Fund (2015000021223ZK17)
文摘Fluorescence correlation spectroscopy (FCS) is a widely used method for measuring molecular diffusion and chemical kinetics. However, when a mixture of fluorescent species is taken into account, the conven- tional FCS method has limitations in extracting autocorrelations for different species and cross correla- tions between different species. Recently developed fluorescence lifetime correlation spectroscopy (FLCS) based on time-tagged time-resolved (TITR) photon recording, which can record the global and micro arrival time for each individual photon, has been used to discriminate different species according to fluorescence lifetime. Here, based on two-dimensional lifetime decay maps constructed from TITR photon stream, we have developed a quantitative lifetime-deconvolution FCS model (LDFCS) to extract precise chemical rates for chemical conversions in multi-species systems. The key point of LDFCS model is separation of different species according to the global distribution of fluorescence lifetime and then deconvolution of autocorrelations and cross-correlations from the two-dimensional lifetime decay maps constructed bv the micro arrival times of photon pairs at each delay time.
文摘This paper presents the application of lifetime spectroscopy to the study of carrier-induced degradation ascribed to the boron-oxygen (BO) defect. Specifically, a large data set of p-type silicon samples is used to investigate two important aspects of carrier lifetime analysis: ① the methods used to extract the recombination lifetime associated with the defect and ② the underlying assumption that cartier injection does not affect lifetime components unrelated to the defect. The results demonstrate that the capture cross section ratio associated with the donor level of the BO defect (kl) vary widely depending on the specific method used to extract the defect-specific recombination lifetime. For the data set studied here, it was also found that illumination used to form the defect caused minor, but statistically significant changes in the surface passivation used. This violation of the fundamental assumption could be accounted for by applying appropriate curve fitting methods, resulting in an improved estimate of k1 (11.90±0.45) for the fully formed BO defect when modeled using the donor level alone. Illumination also appeared to cause a minor, apparently injectionindependent change in lifetime that could not be attributed to the donor level of the BO defect alone and is likely related to the acceptor level of the BO defect. While specific to the BO defect, this study has implications for the use of lifetime spectroscopy to study other carrier induced defects. Finally, we demonstrate the use of a unit-less regression goodness-of-fit metric for lifetime data that is easy to interpret and accounts for repeatability error.
基金This work was supported by the National Key R&D Program of China(2019YFA0210004,2017YFA0207301,2017YFA0303500)the National Natural Science Foundation of China(21975242,U2032212,21890754,21805267,21703222,11975225)+7 种基金the Strategic Priority Research Program of Chinese Academy of Sciences(XDB36000000)Youth Innovation Promotion Association of CAS(CX2340007003)Key Research Program of Frontier Sciences of CAS(QYZDY-SSW-SLH011)Major Program of Development Foundation of Hefei Center for Physical Science and Technology(2020HSC-CIP003)Users with Excellence Program of Hefei Science Center CAS(2020HSCUE001)The University Synergy Innovation Program of Anhui Province(GXXT-2020-001)the Fok Ying-Tong Education Foundation(161012)Supercomputing USTC and National Supercomputing Center in Shenzhen are acknowledged for computational support.
文摘To realize efficient atmospheric CO_(2) chemisorption and activation,abundant Ti^(3+) sites and oxygen vacancies in TiO_(2) ultrathin layers were designed.Positron annihilation lifetime spectroscopy and theoretical calculations first unveil each oxygen vacancy is associated with the formation of two Ti^(3+)sites,giving a Ti^(3+)-V_(o)-Ti^(3+) configuration.The Ti^(3+)-V_(o)-Ti^(3+) sites could bond with CO_(2) molecules to form a stable configuration,which converted the endoergic chemisorption step to an exoergic process,verified by in-situ Fourier-transform infrared spectra and theoretical calculations.Also,the adjacent Ti^(3+)sites not only favor CO_(2) activation into COOH*via forming a stable Ti^(3+)–C–O–Ti^(3+) configuration,but also facilitate the rate-limiting COOH^(*)scission to CO^(*)by reducing the energy barrier from 0.75 to 0.45 e V.Thus,the Ti^(3+)-V_(o)-TiO_(2) ultrathinlayers could directly capture and photofix atmospheric CO_(2) into near-unity CO,with the corresponding CO_(2)-to-CO conversion ratio of ca.20.2%.
文摘Void swelling,which induces the degradation of the original properties of nuclear materials under high-energy particleirradiation,is an important problem.The incubation period,a transient stage before the steady void growth,determines the duration of service of nuclear materials.Several experimental studies have been performed on void observations by transmission electron microscopy(TEM),which,however,has a resolution limit for the size of defect clusters.Positron annihilation lifetime spectroscopy(PALS)enables the detection of small vacancy clusters,single vacancies,dislocations and precipitates.The use of these two methods provides complementary information toward detecting defect information in the incubation period.Here,defect structures during the incubation period in austenitic stainless steels,by means of PALS and TEM are reviewed.The role of alloying elements into determining the period is explained.Furthermore,the existing problems and research directions in this field are presented.