A vacuum ultraviolet(VUV)spectroscopy with a focal length of 1 m has been engineered specifically for observing edge impurity emissions in Experimental Advanced Superconducting Tokamak(EAST).In this study,wavelength c...A vacuum ultraviolet(VUV)spectroscopy with a focal length of 1 m has been engineered specifically for observing edge impurity emissions in Experimental Advanced Superconducting Tokamak(EAST).In this study,wavelength calibration for the VUV spectroscopy is achieved utilizing a zinc lamp.The grating angle and charge-coupled device(CCD)position are carefully calibrated for different wavelength positions.The wavelength calibration of the VUV spectroscopy is crucial for improving the accuracy of impurity spectral data,and is required to identify more impurity spectral lines for impurity transport research.Impurity spectra of EAST plasmas have also been obtained in the wavelength range of 50–300 nm with relatively high spectral resolution.It is found that the impurity emissions in the edge region are still dominated by low-Z impurities,such as carbon,oxygen,and nitrogen,albeit with the application of fulltungsten divertors on the EAST tokamak.展开更多
The photodegradation of persistent and bioaccumulative perftuorooctanoic acid (PFOA) in water by 185 nm vacuum ultraviolet (VUV) light was examined to develop an effective technology to deal with PFOA pollution. P...The photodegradation of persistent and bioaccumulative perftuorooctanoic acid (PFOA) in water by 185 nm vacuum ultraviolet (VUV) light was examined to develop an effective technology to deal with PFOA pollution. PFOA degraded very slowly under irradiation of 254 nm UV light. However, 61.7% of initial PFOA was degraded by 185 nm VUV light within 2 h, and defluorination ratio reached 17.1%. Pseudo first-order-kinetics well simulated its degradation and defluorination. Besides, fluoride ion formed in water, 4 shorter-chain perfluorinated carboxylic acids (PFCAs), that is, perfluoroheptanoic acid, perfluorohexanoic acid, perfluoropentanoic acid, and perfluorobutanoic acid. These were identified as intermediates by LC-MS measurement. These PFCAs consecutively formed and further degraded with irradiation time. According to the mass balance calculation, no other byproducts were formed. It was proposed that PFCAs initially are decarboxylated by 185 nm light, and the radical thus formed reacts with water to form shorter-chain PFCA with one less CF2 unit.展开更多
Vacuum ultraviolet photon-induced ionization and dissociation of isoleucine are investi- gated with synchrotron radiation photoionization mass spectroscopy and theoretical cal- culations. The main fragment ions at m/z...Vacuum ultraviolet photon-induced ionization and dissociation of isoleucine are investi- gated with synchrotron radiation photoionization mass spectroscopy and theoretical cal- culations. The main fragment ions at m/z=86, 75, 74, 69, 57, 46, 45, 44, 41, 30, 28, and 18 from isoleucine are observed in the mass spectrum at the photon energy of 13 eV. From the photoionization efficiency curves, appearance energies for the principal fragment ions CsH12N+ (rn/z=86), C2H5NO2+ (m/z=75), C5H9+ (rn/z=-69), C4H9+ (m/z=57), and CH4N+ (m/z=30) are determined to be 8.844-0.07, 9.254-0.06, 10.20-4-0.12, 9.254-0.10, and 11.05+0.07 eV, respectively, and possible formation pathways are established in detail by the calculations at the B3LYP/6-31++G(d, p) levels. These proposed channels include simple bond cleavage reactions as well as reactions involving intermediates and transition structures. The experimental and computational appearance energies or barriers are in good agreement.展开更多
Polytetrafluoroethylene (Teflon), a widely used spacecraft material, isstudied to investigate the vacuum ultraviolet (VUV) effects and its synergistic effects with atomicoxygen (AO) in a ground-based simulation facili...Polytetrafluoroethylene (Teflon), a widely used spacecraft material, isstudied to investigate the vacuum ultraviolet (VUV) effects and its synergistic effects with atomicoxygen (AO) in a ground-based simulation facility. The samples before and after the experiments arecompared in appearance, mass, optical properties and surface composition. The reactioncharacteristics of Teflon are summarized and the reaction mechanisms are analyzed. The followingconclusion can be drawn: at the action of VUV the Teflon sample surface is darkened for theaccumulation of carbon; and when the sample is exposed to AO, the carbon is oxidized and thedarkening surface is bleached; the synergistic effects of VUV and AO may cause the erosion of Teflonmore severe.展开更多
As an Hg-free lamp using phosphor, the Bi^3+ and EH^3+ co-doped Y2O2S phosphors were prepared and their luminescence properties under vacuum ultraviolet(VUV) excitation were investigated. The VUV photoluminescent ...As an Hg-free lamp using phosphor, the Bi^3+ and EH^3+ co-doped Y2O2S phosphors were prepared and their luminescence properties under vacuum ultraviolet(VUV) excitation were investigated. The VUV photoluminescent intensity of Y2O2S:Eu^3+ was weak, however, considerably stronger red emission at 626 nm with good color purity was observed in Y2O2S:Eu^3+,Bi^3+ systems. Investigation on the photoluminescence reveals that the strong VUV luminescence of Y2O2S:Eu^3+,Bi^3+ at 147 nm is mainly because the Bi^3+ acts as a medium and effectively performs the energy transfer process: Y^3+-O^2-→Bi^3+→Eu^3+, while the intense emission band at 172 nm is attributed to the absorption of the characteristic ^1So-^1P1 transition of Bi^3+ and the direct energy transfer from Bi^3+ to Eu^3+. The Y2O2S:Eu^3+,Bi^3+ shows excellent VUV optical properties compared with the commercial (Y,Gd)BO3:Eu^3+. Thus, the Y2O2S:Eu^3+,Bi^3+ can be a potential red VUV-excited candidate applied in Hg-free lamps for backlight of liquid crystal display.展开更多
Vacuum ultraviolet radiation of Upilex-S polyimide film 25 μm thick was performed using a gas jet type of vacuum ultraviolet simulator which gives unfixed wavelength from 5 nm to 200 nm.Nanoparticles redeposited on t...Vacuum ultraviolet radiation of Upilex-S polyimide film 25 μm thick was performed using a gas jet type of vacuum ultraviolet simulator which gives unfixed wavelength from 5 nm to 200 nm.Nanoparticles redeposited on the films were observed and the nanoparticles formed on the surface consist mainly of carbon clusters.Changes in the composition and the chemical characteristics of film surface after radiation were identified by X-ray photoelectron spectroscopy(XPS).Relative O content in the radiated area was found to be higher,while N content was lower than in the pristine area.This indicates that Upilex-S polyimide film releases N atoms as volatile species.And the C1s,O1s envelopes were fitted using Multipak Spectrum software.The surface morphologies on iradiated area were examined by Atomic Force Microscope(AFM).Pieces of radiant products protrude from the eradiated surface,leading to considerable roughness for the iradiated area.And the surface transmittance of Upilex-S film after radiation reduces.展开更多
Polysiloxane/SiO2 hybrid coatings have been prepared on Kapton films by a sol-gel process. The erosion resistance of polysiloxane/Si02 (20 wt pct) coating was evaluated by exposure tests of vacuum ultraviolet radiat...Polysiloxane/SiO2 hybrid coatings have been prepared on Kapton films by a sol-gel process. The erosion resistance of polysiloxane/Si02 (20 wt pct) coating was evaluated by exposure tests of vacuum ultraviolet radiation (VUV) and atomic oxygen beam (AO) in a ground-based simulation facility. The experimental results indicate that this coating exhibits better AO resistance than pure polysiloxane coating. The erosion yield (Ey) of the polysiloxane/Si02 (20 wt pct) hybrid coating is about 10-27 cm3/atom, being one or two orders of magnitude lower than that of polysiloxane. VUV radiation can affect the erosion process greatly. Under simultaneous AO and VUV exposure, the value of Ey of the polysiloxane/5iO2 (20 wt pct) hybrid coating increases by 3g% compared with that under single AO exposure.展开更多
Novel Dy3+-doped GdPO4 white light phosphors with monoclinic system were successfully synthesised by hydrothermal method at 240℃. This paper investigates the luminescence properties of white-light Gd1-xPO4 : xDy3+...Novel Dy3+-doped GdPO4 white light phosphors with monoclinic system were successfully synthesised by hydrothermal method at 240℃. This paper investigates the luminescence properties of white-light Gd1-xPO4 : xDy3+ under vacuum ultraviolet (VUV) excitation. The strong absorption at around 147 nm in excitation spectrum energy can be transferred to the energy levels of Dy3+ ion from the host absorption. Additionally, this white light phosphors are activated by a single Dy3+ ion and with a lower preparation temperature, which tend to decrease the consumption of rare earth resource and energy. Therefore, the luminescence of Gd1-xPO4 : xDy3+ under VUV excitation is effective, and proves to be promising in application to mercury-flee lamp.展开更多
α-pinene is the most abundant monoterpene that represents an important family of volatile organic compounds.Molecular identification of key transient compounds during theα-pinene ozonolysis has been proven to be a c...α-pinene is the most abundant monoterpene that represents an important family of volatile organic compounds.Molecular identification of key transient compounds during theα-pinene ozonolysis has been proven to be a challenging experimental target because of a large number of intermediates and products involved.Here we exploit the recently developed hybrid instruments that integrate aerosol mass spectrometry with a vacuum ultraviolet free-electron laser to study theα-pinene ozonolysis.The experiments ofα-pinene ozonolysis are performed in an indoor smog chamber,with reactor having a volume of 2 m^(3) which is made of fluorinated ethylene propylene film.Distinct mass spectral peaks provide direct experimental signatures of previously unseen compounds produced from the reaction ofα-pinene with O_(3).With the aid of quantum chemical calculations,plausible mechanisms for the formation of these new compounds are proposed.These findings provide crucial information on fundamental understanding of the initial steps ofα-pinene oxidation and the subsequent processes of new particle formation.展开更多
Spectroscopic characterization of clusters is crucial to understanding the structures and reaction mechanisms at the microscopic level,but it has been proven to be a grand challenge for neutral clusters because the ab...Spectroscopic characterization of clusters is crucial to understanding the structures and reaction mechanisms at the microscopic level,but it has been proven to be a grand challenge for neutral clusters because the absence of a charge makes it di伍cult for the size selection and detection.Infrared(IR)spectroscopy based on threshold photoionization using a tunable vacuum ultraviolet free electron laser(VUV-FEL)has recently been developed in the lab.The IR-VUV depletion and IR+VUV enhancement spectroscopic techniques open new avenues for size-selected IR spectroscopies of a large variety of neutral clusters without confinement(i.e.,an ultraviolet chromophore,a messenger tag,or a host matrix).The spectroscopic principles have been demonstrated by investigations of some neutral water clusters and some metal carbonyls.Here,the spectroscopic principles and their applications for neutral clusters are reviewed.展开更多
Photodissociation of H2S in the VUV region plays an important role in the atmospheric chemistry and interstellar chemistry.To date,however,few studies have been focused on this topic.In this article,we have described ...Photodissociation of H2S in the VUV region plays an important role in the atmospheric chemistry and interstellar chemistry.To date,however,few studies have been focused on this topic.In this article,we have described a laser dispersion method applied in the apparatus combining the high-n H atom Rydberg tagging time-of-flight technique with the vacuum ultraviolet free electron laser(VUV FEL).The Lyman-αlaser beam(121.6 nm)used in the H-atom detection was generated by the difference frequency four-wave mixing schemes in a Kr/Ar gas cell.After passing through an off-axis biconvex LiF lens,the 121.6 nm beam was dispersed from the 212.6 nm and 845 nm beams due to the different deflection angles experienced by these laser beams at the surfaces of the biconvex lens.This method can eliminate the background signal from the 212.6 nm photolysis.Combined with the VUV FEL,photodissociation of H2S at 122.95 nm was studied successfully.The TOF spectrum was measured and the derived total kinetic energy release spectrum was displayed.The results suggest that the experimental setup is a powerful tool for investigating photodissociation dynamics of molecules in the VUV region which involves the H-atom elimination processes.展开更多
The vacuum ultraviolet (VUV) luminescent properties of Pr^3+ -activated LaB3O6 were investigated with highenergetic synchrotron radiation from 20 to 300 K. In the emission spectra, the parity-forbidden 4f^2→4f^2 a...The vacuum ultraviolet (VUV) luminescent properties of Pr^3+ -activated LaB3O6 were investigated with highenergetic synchrotron radiation from 20 to 300 K. In the emission spectra, the parity-forbidden 4f^2→4f^2 and parity-allowed 4f5d→4f^2 transitions were observed simultaneously. In addition, it was also observed that the intensity of 4f5d→4f^2 emission bands increased relative to the intensity of 4f^2→4f^2 emissions with increasing temperature. The thermal equilibrium model of energy levels was employed with respect to the lowest 4f5d state and ^1S0 state of LaB3O6:Pr^3+ , as a result of which the fitted curve had a good agreement with the experiment values, which clarified the physical nature of temperature-dependent emission characteristics of Pr^3+ in LaB3O6.展开更多
The Gd2O2CO3:Eu^3+ with type-Ⅱ structure phosphor was successfully synthesized via flux method at 400 ℃ and their photoluminescence properties in vacuum ultraviolet (VUV) region were examined. The broad and stro...The Gd2O2CO3:Eu^3+ with type-Ⅱ structure phosphor was successfully synthesized via flux method at 400 ℃ and their photoluminescence properties in vacuum ultraviolet (VUV) region were examined. The broad and strong excitation bands in the range of 153-205 nm owing to the CO3^2- host absorption and charge transfer (CT) of Gd^3+-O2^- were observed for Gd2O2CO3:Eu^3+. Under 172 nm excitation, Gd2O2CO3:Eu^3+ exhibited strong red emission with good color purity, indicating Eu^3+ ions located at low symmetry sites and the chromaticity coordination of luminescence for Gd2O2CO3:Eu^3+ was (x=0.652, y=0.345). The photoluminescence quenching concentration of Eu^3+ excited by 172 nm for Gd2O2CO3:Eu^3+ was about 5%. Gd2O2CO3:Eu^3+ would be a potential VUV-excited red phosphor applied in mercury-free fluorescent lamps.展开更多
A negative unipolar pulsed voltage is applied to study internal electrical parameters of the xenon filled dielectric barrier discharge (DBD) sources. The VUV radiation emitted from these sources is characterized by ...A negative unipolar pulsed voltage is applied to study internal electrical parameters of the xenon filled dielectric barrier discharge (DBD) sources. The VUV radiation emitted from these sources is characterized by means of the photoluminescence intensity of the red phosphor pellet. The red phosphor converts the VUV radiation into visible radiation and the emission spectra include a peak at 619.56 nm. The emission characteristics of the red phosphor are analyzed in terms of the pressure-distance (pd), rise time and frequency of the pulsed voltage waveform. The emission intensity measured at different operational conditions confirms that the formation and decay of the xenon excimer, Xe2^*, increase with the increase in reduced electric field, E/N. After exceeding certain limits of E/N, the intensity of Xe2^* decreases rapidly.展开更多
Vacuum ultraviolet photodissociation dynamics of N2O+hν→N2(X^(1)Σg+)+O(^(1)S0)in the short wavelength tail of D^(1)Σ+band has been investigated using the time-sliced velocity-mapped ion imaging technique by probin...Vacuum ultraviolet photodissociation dynamics of N2O+hν→N2(X^(1)Σg+)+O(^(1)S0)in the short wavelength tail of D^(1)Σ+band has been investigated using the time-sliced velocity-mapped ion imaging technique by probing the images of the O(^(1)S0)photoproducts at a set of photolysis wavelengths including 121.47 nm,122.17 nm,123.25 nm and 123.95 nm.The product total kinetic energy release distributions,vibrational state distributions of the N2(X^(1)Σg+)photofragments and angular anisotropy parameters have been obtained by analyzing the raw O(^(1)S0)images.It is noted that additional vibrationally excited photoproducts(3≤v≤8)with a Boltzmann-like feature start to appear except the non-statistical component as the photolysis wavelength decreases to 123.25 nm,and the corresponding populations become more pronounced with decreasing of the photolysis wavelength.Furthermore,the vibrational state specific anisotropy parameterβat each photolysis wavelength exhibits a drastic fluctuation nearβ=1.75 at v<8,and decreases to a minimum as the vibrational quantum number further increases.While the overall anisotropy parameterβfor the N2(X^(1)Σg+)+O(^(1)S0)channel presents a roughly monotonical increase from 1.63 at 121.47 nm to 1.95 at 123.95 nm.The experimental observations suggest that there is at least one fast nonadiabatic pathway from initially prepared D^(1)Σ+state to the dissociative state with bent geometry dominating to generate the additional vibrational structures at high photoexcitation energies.展开更多
We show that by scanning the frequency of a single mode infrared (IR) optical parametric oscillator (IR- OPO) laser to excite the molecular species of interest and fixing the frequency of a vacuum ultraviolet (VU...We show that by scanning the frequency of a single mode infrared (IR) optical parametric oscillator (IR- OPO) laser to excite the molecular species of interest and fixing the frequency of a vacuum ultraviolet (VUV) laser to photoionize the IR excited species, high-resolution IR spectra of polyatomic neutrals can be obtained with high sensitivity. The fact that this IR-VUV-photoion (IR-VUV-PI) method is based on VUV photoionization probe, and thus, allows the identification of the neutral IR absorber, makes it applicable for IR spectroscopy measurements of isotopemers, radicals, and clusters, which usually exist as impure samples. The highly resolved IR-VUV-PI measurements achieved using the single mode IR-OPO laser have made possible the selection of single rovibrational states of CH3X (X=Br and I), C2H4, and C3H4 for VUV-pulsed field ionization-photoelectron (VUV-PFI-PE) measurements, resulting in rovibrationally resolved photoelectron spectra for these polyatomic molecules. These experiments show that the signal- to-noise ratios of the IR-VUV-PI and IR-VUV-PFI-PE spectra obtained by employing the high-resolution IR-OPO laser are significantly higher than those observed in previous IR-VUV-PI and IR-VUV-PFI-PE studies using a low-resolution IR-OPO laser. Further improvement in sensitivity of IR-VUV-PI and IR- VUV-PFI-PE measurements by using the collinear arrangement of IR-VUV lasers and molecular beam is discussed.展开更多
This study investigates two secondary electron emission(SEE)models for photoelectric energy distribution curves f(E_(ph),hγ),B,E_(mean),absolute quantum efficiency(AQE),and the mean escape depth of photo-emitted elec...This study investigates two secondary electron emission(SEE)models for photoelectric energy distribution curves f(E_(ph),hγ),B,E_(mean),absolute quantum efficiency(AQE),and the mean escape depth of photo-emitted electronsλof metals.The proposed models are developed from the density of states and the theories of photo-emission in the vacuum ultraviolet and SEE,where B is the mean probability that an internal photo-emitted electron escapes into vacuum upon reaching the emission surface of the metal,and E_(mean)is the mean energy of photo-emitted electrons measured from vacuum.The formulas for f(E_(ph),hγ),B,λ,E_(mean),and AQE that were obtained were shown to be correct for the cases of Au at hγ=8.1–11.6 eV,Ni at hγ=9.2–11.6 eV,and Cu at hγ=7.7–11.6 eV.The photoelectric cross sections(PCS)calculated here are analyzed,and it was confirmed that the calculated PCS of the electrons in the conduction band of Au at hγ=8.1–11.6eV,Ni at hγ=9.2–11.6 eV,and Cu at hγ=7.7–11.6 eV are correct.展开更多
Photoreflectance(PR)spectroscopy is a powerful and non-destructive experimental technique to explore interband transitions of semiconductors.In most PR systems,the photon energy of the pumping beam is usually chosen t...Photoreflectance(PR)spectroscopy is a powerful and non-destructive experimental technique to explore interband transitions of semiconductors.In most PR systems,the photon energy of the pumping beam is usually chosen to be higher than the bandgap energy of the sample.To the best of our knowledge,the highest energy of pumping laser in reported PR systems is 5.08 eV(244 nm),not yet in the vacuum ultraviolet(VUV)region.In this work,we report the design and construction of a PR system pumped by VUV laser of 7.0 eV(177.3 nm).At the same time,dual-modulated technique is applied and a dual channel lock-in-amplifier is integrated into the system for efficient PR measurement.The system’s performance is verified by the PR spectroscopy measurement of well-studied semiconductors,which testifies its ability to probe critical-point energies of the electronic band in semiconductors from ultraviolet to near-infrared spectral region.展开更多
Vacuum ultraviolet(VUV)photodissociation dynamics of carbonyl sulfide was investigated experimentally by using a tunable photolysis light source and the timesliced velocity map ion imaging technique.Ion images of S(^(...Vacuum ultraviolet(VUV)photodissociation dynamics of carbonyl sulfide was investigated experimentally by using a tunable photolysis light source and the timesliced velocity map ion imaging technique.Ion images of S(^(3)P_(J=2,1,0))dissociation products were measured at five photolysis wavelengths from 133.26 nm to 139.96 nm,corresponding to the F Rydberg state of OCS.Two dissociation channels:S(^(3)P_(J))+CO(X^(1)Σ+)and S(^(3)P_(J))+CO(A^(3)Π)were observed with the former being dominant.The vibrational states of CO co-products were partially resolved in the ion images.The product total kinetic energy releases,anisotropy parameters(β),and the branching ratios of high-lying CO vibrational states were determined for the S(^(3)P_(J))+CO(X^(1)Σ^(+))channel.We found that the anisotropy parameters suddenly changed from negative to positive when OCS was excited to the higher vibrational levels of the F state.Furthermore,the anisotropy parameters for S(^(3)P_(J))products of J=2,1,0 were even different.These anomalous phenomena may result from the simultaneous existence of both parallel and perpendicular dissociation mechanisms,suggesting the involvement of other electronic states with different symmetry in the initially-excited energy region.This work provides a further understanding of the nonadiabatic couplings in the VUV photodissociation process of OCS.展开更多
Microscopes in vacuum ultraviolet and soft X-ray regions using a normal incidence type of Schwarzschild objective are reviewed. The objective consists of a concave mirror and a convex mirror coated with a high reflect...Microscopes in vacuum ultraviolet and soft X-ray regions using a normal incidence type of Schwarzschild objective are reviewed. The objective consists of a concave mirror and a convex mirror coated with a high reflectance multilayer,having a large numerical aperture comparing with other objectives. The microscopes have been used to diagnose inertia-confinement-fusion plasmas,and to investigate small samples or microstructures of in- organic and organic materials by imaging them using laboratory light sources. Synchrotron radiation has been also used to obtain a microbeam for a photoelectron scanning microscope with a spatial resolution of 0.1 μm. The struc- ture and performance of two laboratory microscopes developed at Tohoku University are demonstrated. One of them is a soft X-ray emission imaging microscope. An image of an artificial pattern made of W and SiO2 on Si wafer by focusing Si L emission was presented. The other is an ultraviolet photoelectron scanning microscope using a He (he- lium) gas discharge lamp. The valence band spectra of a microcrystal of FeWO4 were presented. Furthermore other applications such as demagnifying optics for lithography and optics to gather fluorescence for emission spectroscopy are introduced.展开更多
基金partially supported by National Natural Science Foundation of China(Nos.U23A2077,12175278,12205072)the National Magnetic Confinement Fusion Science Program of China(Nos.2019YFE0304002,2018YFE0303103)+2 种基金the Comprehensive Research Facility for Fusion Technology Program of China(No.2018-000052-73-01-001228)Major Science and Technology Infrastructure Maintenance and Reconstruction Projects of the Chinese Academy of Sciences(2021)the University Synergy Innovation Program of Anhui Province(No.GXXT2021-029)。
文摘A vacuum ultraviolet(VUV)spectroscopy with a focal length of 1 m has been engineered specifically for observing edge impurity emissions in Experimental Advanced Superconducting Tokamak(EAST).In this study,wavelength calibration for the VUV spectroscopy is achieved utilizing a zinc lamp.The grating angle and charge-coupled device(CCD)position are carefully calibrated for different wavelength positions.The wavelength calibration of the VUV spectroscopy is crucial for improving the accuracy of impurity spectral data,and is required to identify more impurity spectral lines for impurity transport research.Impurity spectra of EAST plasmas have also been obtained in the wavelength range of 50–300 nm with relatively high spectral resolution.It is found that the impurity emissions in the edge region are still dominated by low-Z impurities,such as carbon,oxygen,and nitrogen,albeit with the application of fulltungsten divertors on the EAST tokamak.
基金Project supported by the National Natural Science Foundation of China (No. 20577026) the New Century Excellent Talents in University (No. NCET-04-0090).
文摘The photodegradation of persistent and bioaccumulative perftuorooctanoic acid (PFOA) in water by 185 nm vacuum ultraviolet (VUV) light was examined to develop an effective technology to deal with PFOA pollution. PFOA degraded very slowly under irradiation of 254 nm UV light. However, 61.7% of initial PFOA was degraded by 185 nm VUV light within 2 h, and defluorination ratio reached 17.1%. Pseudo first-order-kinetics well simulated its degradation and defluorination. Besides, fluoride ion formed in water, 4 shorter-chain perfluorinated carboxylic acids (PFCAs), that is, perfluoroheptanoic acid, perfluorohexanoic acid, perfluoropentanoic acid, and perfluorobutanoic acid. These were identified as intermediates by LC-MS measurement. These PFCAs consecutively formed and further degraded with irradiation time. According to the mass balance calculation, no other byproducts were formed. It was proposed that PFCAs initially are decarboxylated by 185 nm light, and the radical thus formed reacts with water to form shorter-chain PFCA with one less CF2 unit.
基金V. ACKNOWLEDGMENTS This work is supported by the National Natural Science Foundation of China (No.10875126 and No.10979048) and the Specialized Research Fund for the Doctoral Program of Higher Education, SRF for ROCS, SEM.
文摘Vacuum ultraviolet photon-induced ionization and dissociation of isoleucine are investi- gated with synchrotron radiation photoionization mass spectroscopy and theoretical cal- culations. The main fragment ions at m/z=86, 75, 74, 69, 57, 46, 45, 44, 41, 30, 28, and 18 from isoleucine are observed in the mass spectrum at the photon energy of 13 eV. From the photoionization efficiency curves, appearance energies for the principal fragment ions CsH12N+ (rn/z=86), C2H5NO2+ (m/z=75), C5H9+ (rn/z=-69), C4H9+ (m/z=57), and CH4N+ (m/z=30) are determined to be 8.844-0.07, 9.254-0.06, 10.20-4-0.12, 9.254-0.10, and 11.05+0.07 eV, respectively, and possible formation pathways are established in detail by the calculations at the B3LYP/6-31++G(d, p) levels. These proposed channels include simple bond cleavage reactions as well as reactions involving intermediates and transition structures. The experimental and computational appearance energies or barriers are in good agreement.
文摘Polytetrafluoroethylene (Teflon), a widely used spacecraft material, isstudied to investigate the vacuum ultraviolet (VUV) effects and its synergistic effects with atomicoxygen (AO) in a ground-based simulation facility. The samples before and after the experiments arecompared in appearance, mass, optical properties and surface composition. The reactioncharacteristics of Teflon are summarized and the reaction mechanisms are analyzed. The followingconclusion can be drawn: at the action of VUV the Teflon sample surface is darkened for theaccumulation of carbon; and when the sample is exposed to AO, the carbon is oxidized and thedarkening surface is bleached; the synergistic effects of VUV and AO may cause the erosion of Teflonmore severe.
基金Supported by the Project of the Combination of Industry and Research by the Ministry of Education of China and Guang-dong Province, China(No.0712226100023)
文摘As an Hg-free lamp using phosphor, the Bi^3+ and EH^3+ co-doped Y2O2S phosphors were prepared and their luminescence properties under vacuum ultraviolet(VUV) excitation were investigated. The VUV photoluminescent intensity of Y2O2S:Eu^3+ was weak, however, considerably stronger red emission at 626 nm with good color purity was observed in Y2O2S:Eu^3+,Bi^3+ systems. Investigation on the photoluminescence reveals that the strong VUV luminescence of Y2O2S:Eu^3+,Bi^3+ at 147 nm is mainly because the Bi^3+ acts as a medium and effectively performs the energy transfer process: Y^3+-O^2-→Bi^3+→Eu^3+, while the intense emission band at 172 nm is attributed to the absorption of the characteristic ^1So-^1P1 transition of Bi^3+ and the direct energy transfer from Bi^3+ to Eu^3+. The Y2O2S:Eu^3+,Bi^3+ shows excellent VUV optical properties compared with the commercial (Y,Gd)BO3:Eu^3+. Thus, the Y2O2S:Eu^3+,Bi^3+ can be a potential red VUV-excited candidate applied in Hg-free lamps for backlight of liquid crystal display.
基金This work is financially supported by Development Program for Outstanding Young Teachers in Harbin Institute of Technology(No HIT2006 32)
文摘Vacuum ultraviolet radiation of Upilex-S polyimide film 25 μm thick was performed using a gas jet type of vacuum ultraviolet simulator which gives unfixed wavelength from 5 nm to 200 nm.Nanoparticles redeposited on the films were observed and the nanoparticles formed on the surface consist mainly of carbon clusters.Changes in the composition and the chemical characteristics of film surface after radiation were identified by X-ray photoelectron spectroscopy(XPS).Relative O content in the radiated area was found to be higher,while N content was lower than in the pristine area.This indicates that Upilex-S polyimide film releases N atoms as volatile species.And the C1s,O1s envelopes were fitted using Multipak Spectrum software.The surface morphologies on iradiated area were examined by Atomic Force Microscope(AFM).Pieces of radiant products protrude from the eradiated surface,leading to considerable roughness for the iradiated area.And the surface transmittance of Upilex-S film after radiation reduces.
文摘Polysiloxane/SiO2 hybrid coatings have been prepared on Kapton films by a sol-gel process. The erosion resistance of polysiloxane/Si02 (20 wt pct) coating was evaluated by exposure tests of vacuum ultraviolet radiation (VUV) and atomic oxygen beam (AO) in a ground-based simulation facility. The experimental results indicate that this coating exhibits better AO resistance than pure polysiloxane coating. The erosion yield (Ey) of the polysiloxane/Si02 (20 wt pct) hybrid coating is about 10-27 cm3/atom, being one or two orders of magnitude lower than that of polysiloxane. VUV radiation can affect the erosion process greatly. Under simultaneous AO and VUV exposure, the value of Ey of the polysiloxane/5iO2 (20 wt pct) hybrid coating increases by 3g% compared with that under single AO exposure.
基金Project supported by the Combination of Industry and Research by the Ministry of Education and Guangdong Province (Grant No 0712226100023)
文摘Novel Dy3+-doped GdPO4 white light phosphors with monoclinic system were successfully synthesised by hydrothermal method at 240℃. This paper investigates the luminescence properties of white-light Gd1-xPO4 : xDy3+ under vacuum ultraviolet (VUV) excitation. The strong absorption at around 147 nm in excitation spectrum energy can be transferred to the energy levels of Dy3+ ion from the host absorption. Additionally, this white light phosphors are activated by a single Dy3+ ion and with a lower preparation temperature, which tend to decrease the consumption of rare earth resource and energy. Therefore, the luminescence of Gd1-xPO4 : xDy3+ under VUV excitation is effective, and proves to be promising in application to mercury-flee lamp.
基金financially supported by the National Natural Science Foundation of China(No.22125303,No.92061203,and No.21688102)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB17000000)+2 种基金Dalian Institute of Chemical Physics(DICP DCLS201701)Chinese Academy of Sciences(No.GJJSTD20190002)K.C.Wong Education Foundation(No.GJTD-2018-06)。
文摘α-pinene is the most abundant monoterpene that represents an important family of volatile organic compounds.Molecular identification of key transient compounds during theα-pinene ozonolysis has been proven to be a challenging experimental target because of a large number of intermediates and products involved.Here we exploit the recently developed hybrid instruments that integrate aerosol mass spectrometry with a vacuum ultraviolet free-electron laser to study theα-pinene ozonolysis.The experiments ofα-pinene ozonolysis are performed in an indoor smog chamber,with reactor having a volume of 2 m^(3) which is made of fluorinated ethylene propylene film.Distinct mass spectral peaks provide direct experimental signatures of previously unseen compounds produced from the reaction ofα-pinene with O_(3).With the aid of quantum chemical calculations,plausible mechanisms for the formation of these new compounds are proposed.These findings provide crucial information on fundamental understanding of the initial steps ofα-pinene oxidation and the subsequent processes of new particle formation.
基金This work was supported by the National Natural Science Foundation of China(No.92061203 and No.21688102)the Strategic Priority Research Program of Chinese Academy of Sciences(XDB17000000)+3 种基金International Partnership Program of Chinese Academy of Sciences(121421KYSB20170012)Chinese Academy of Sciences(GJJSTD20190002)K.C.Wong Education Foundation(GJTD-2018-06)Dalian Institute of Chemical Physics(DICP DCLS201702).
文摘Spectroscopic characterization of clusters is crucial to understanding the structures and reaction mechanisms at the microscopic level,but it has been proven to be a grand challenge for neutral clusters because the absence of a charge makes it di伍cult for the size selection and detection.Infrared(IR)spectroscopy based on threshold photoionization using a tunable vacuum ultraviolet free electron laser(VUV-FEL)has recently been developed in the lab.The IR-VUV depletion and IR+VUV enhancement spectroscopic techniques open new avenues for size-selected IR spectroscopies of a large variety of neutral clusters without confinement(i.e.,an ultraviolet chromophore,a messenger tag,or a host matrix).The spectroscopic principles have been demonstrated by investigations of some neutral water clusters and some metal carbonyls.Here,the spectroscopic principles and their applications for neutral clusters are reviewed.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences (No.XDB17000000)the National Natural Science Foundation of China (NSFC Center for Chemical Dynamics (No.21688102)+4 种基金the National Natural Science Foundation of China (No.21673232, No.21873099, No.21922306)the International Partnership Program of Chinese Academy of Sci-ences (No.121421KYSB20170012)supported by the National Natural Science Foundation of China (No.21973010)supported by the National Natural Science Foundation of China (No.21773236)supported by the Natural Science Research Project of Education Department of Anhui Province (No.KJ2019A0521).
文摘Photodissociation of H2S in the VUV region plays an important role in the atmospheric chemistry and interstellar chemistry.To date,however,few studies have been focused on this topic.In this article,we have described a laser dispersion method applied in the apparatus combining the high-n H atom Rydberg tagging time-of-flight technique with the vacuum ultraviolet free electron laser(VUV FEL).The Lyman-αlaser beam(121.6 nm)used in the H-atom detection was generated by the difference frequency four-wave mixing schemes in a Kr/Ar gas cell.After passing through an off-axis biconvex LiF lens,the 121.6 nm beam was dispersed from the 212.6 nm and 845 nm beams due to the different deflection angles experienced by these laser beams at the surfaces of the biconvex lens.This method can eliminate the background signal from the 212.6 nm photolysis.Combined with the VUV FEL,photodissociation of H2S at 122.95 nm was studied successfully.The TOF spectrum was measured and the derived total kinetic energy release spectrum was displayed.The results suggest that the experimental setup is a powerful tool for investigating photodissociation dynamics of molecules in the VUV region which involves the H-atom elimination processes.
基金Project supported by the National Natural Science Foundation of China (10204001 ,10374002 and 10434030) the"973"Program(2003CB314707)Beijing Jiaotong University Program(2006XM038)
文摘The vacuum ultraviolet (VUV) luminescent properties of Pr^3+ -activated LaB3O6 were investigated with highenergetic synchrotron radiation from 20 to 300 K. In the emission spectra, the parity-forbidden 4f^2→4f^2 and parity-allowed 4f5d→4f^2 transitions were observed simultaneously. In addition, it was also observed that the intensity of 4f5d→4f^2 emission bands increased relative to the intensity of 4f^2→4f^2 emissions with increasing temperature. The thermal equilibrium model of energy levels was employed with respect to the lowest 4f5d state and ^1S0 state of LaB3O6:Pr^3+ , as a result of which the fitted curve had a good agreement with the experiment values, which clarified the physical nature of temperature-dependent emission characteristics of Pr^3+ in LaB3O6.
基金the Program for New Century Talents in the University of China (NCET, 04-0978)the Chinese Specialized Research Fund for the Doctoral Program of Higher Education (SRFDP 20040730019)
文摘The Gd2O2CO3:Eu^3+ with type-Ⅱ structure phosphor was successfully synthesized via flux method at 400 ℃ and their photoluminescence properties in vacuum ultraviolet (VUV) region were examined. The broad and strong excitation bands in the range of 153-205 nm owing to the CO3^2- host absorption and charge transfer (CT) of Gd^3+-O2^- were observed for Gd2O2CO3:Eu^3+. Under 172 nm excitation, Gd2O2CO3:Eu^3+ exhibited strong red emission with good color purity, indicating Eu^3+ ions located at low symmetry sites and the chromaticity coordination of luminescence for Gd2O2CO3:Eu^3+ was (x=0.652, y=0.345). The photoluminescence quenching concentration of Eu^3+ excited by 172 nm for Gd2O2CO3:Eu^3+ was about 5%. Gd2O2CO3:Eu^3+ would be a potential VUV-excited red phosphor applied in mercury-free fluorescent lamps.
文摘A negative unipolar pulsed voltage is applied to study internal electrical parameters of the xenon filled dielectric barrier discharge (DBD) sources. The VUV radiation emitted from these sources is characterized by means of the photoluminescence intensity of the red phosphor pellet. The red phosphor converts the VUV radiation into visible radiation and the emission spectra include a peak at 619.56 nm. The emission characteristics of the red phosphor are analyzed in terms of the pressure-distance (pd), rise time and frequency of the pulsed voltage waveform. The emission intensity measured at different operational conditions confirms that the formation and decay of the xenon excimer, Xe2^*, increase with the increase in reduced electric field, E/N. After exceeding certain limits of E/N, the intensity of Xe2^* decreases rapidly.
基金supported by the National Natural Science Foundation of China(No.21773213)。
文摘Vacuum ultraviolet photodissociation dynamics of N2O+hν→N2(X^(1)Σg+)+O(^(1)S0)in the short wavelength tail of D^(1)Σ+band has been investigated using the time-sliced velocity-mapped ion imaging technique by probing the images of the O(^(1)S0)photoproducts at a set of photolysis wavelengths including 121.47 nm,122.17 nm,123.25 nm and 123.95 nm.The product total kinetic energy release distributions,vibrational state distributions of the N2(X^(1)Σg+)photofragments and angular anisotropy parameters have been obtained by analyzing the raw O(^(1)S0)images.It is noted that additional vibrationally excited photoproducts(3≤v≤8)with a Boltzmann-like feature start to appear except the non-statistical component as the photolysis wavelength decreases to 123.25 nm,and the corresponding populations become more pronounced with decreasing of the photolysis wavelength.Furthermore,the vibrational state specific anisotropy parameterβat each photolysis wavelength exhibits a drastic fluctuation nearβ=1.75 at v<8,and decreases to a minimum as the vibrational quantum number further increases.While the overall anisotropy parameterβfor the N2(X^(1)Σg+)+O(^(1)S0)channel presents a roughly monotonical increase from 1.63 at 121.47 nm to 1.95 at 123.95 nm.The experimental observations suggest that there is at least one fast nonadiabatic pathway from initially prepared D^(1)Σ+state to the dissociative state with bent geometry dominating to generate the additional vibrational structures at high photoexcitation energies.
文摘We show that by scanning the frequency of a single mode infrared (IR) optical parametric oscillator (IR- OPO) laser to excite the molecular species of interest and fixing the frequency of a vacuum ultraviolet (VUV) laser to photoionize the IR excited species, high-resolution IR spectra of polyatomic neutrals can be obtained with high sensitivity. The fact that this IR-VUV-photoion (IR-VUV-PI) method is based on VUV photoionization probe, and thus, allows the identification of the neutral IR absorber, makes it applicable for IR spectroscopy measurements of isotopemers, radicals, and clusters, which usually exist as impure samples. The highly resolved IR-VUV-PI measurements achieved using the single mode IR-OPO laser have made possible the selection of single rovibrational states of CH3X (X=Br and I), C2H4, and C3H4 for VUV-pulsed field ionization-photoelectron (VUV-PFI-PE) measurements, resulting in rovibrationally resolved photoelectron spectra for these polyatomic molecules. These experiments show that the signal- to-noise ratios of the IR-VUV-PI and IR-VUV-PFI-PE spectra obtained by employing the high-resolution IR-OPO laser are significantly higher than those observed in previous IR-VUV-PI and IR-VUV-PFI-PE studies using a low-resolution IR-OPO laser. Further improvement in sensitivity of IR-VUV-PI and IR- VUV-PFI-PE measurements by using the collinear arrangement of IR-VUV lasers and molecular beam is discussed.
基金supported by the National Natural Science Foundation of China (No.11873013)
文摘This study investigates two secondary electron emission(SEE)models for photoelectric energy distribution curves f(E_(ph),hγ),B,E_(mean),absolute quantum efficiency(AQE),and the mean escape depth of photo-emitted electronsλof metals.The proposed models are developed from the density of states and the theories of photo-emission in the vacuum ultraviolet and SEE,where B is the mean probability that an internal photo-emitted electron escapes into vacuum upon reaching the emission surface of the metal,and E_(mean)is the mean energy of photo-emitted electrons measured from vacuum.The formulas for f(E_(ph),hγ),B,λ,E_(mean),and AQE that were obtained were shown to be correct for the cases of Au at hγ=8.1–11.6 eV,Ni at hγ=9.2–11.6 eV,and Cu at hγ=7.7–11.6 eV.The photoelectric cross sections(PCS)calculated here are analyzed,and it was confirmed that the calculated PCS of the electrons in the conduction band of Au at hγ=8.1–11.6eV,Ni at hγ=9.2–11.6 eV,and Cu at hγ=7.7–11.6 eV are correct.
基金Project supported by the National Development Project for Major Scientific Research Facility of China(Grant No.ZDYZ2012-2)the National Natural Science Foundation of China(Grant No.11874350)CAS Key Research Program of Frontier Sciences(Grant Nos.ZDBS-LY-SLH004 and XDPB22)。
文摘Photoreflectance(PR)spectroscopy is a powerful and non-destructive experimental technique to explore interband transitions of semiconductors.In most PR systems,the photon energy of the pumping beam is usually chosen to be higher than the bandgap energy of the sample.To the best of our knowledge,the highest energy of pumping laser in reported PR systems is 5.08 eV(244 nm),not yet in the vacuum ultraviolet(VUV)region.In this work,we report the design and construction of a PR system pumped by VUV laser of 7.0 eV(177.3 nm).At the same time,dual-modulated technique is applied and a dual channel lock-in-amplifier is integrated into the system for efficient PR measurement.The system’s performance is verified by the PR spectroscopy measurement of well-studied semiconductors,which testifies its ability to probe critical-point energies of the electronic band in semiconductors from ultraviolet to near-infrared spectral region.
基金supported by the National Key R&D Program of China(No.2016YFF0200500)the National Natural Science Foundation of China(No.22125302)。
文摘Vacuum ultraviolet(VUV)photodissociation dynamics of carbonyl sulfide was investigated experimentally by using a tunable photolysis light source and the timesliced velocity map ion imaging technique.Ion images of S(^(3)P_(J=2,1,0))dissociation products were measured at five photolysis wavelengths from 133.26 nm to 139.96 nm,corresponding to the F Rydberg state of OCS.Two dissociation channels:S(^(3)P_(J))+CO(X^(1)Σ+)and S(^(3)P_(J))+CO(A^(3)Π)were observed with the former being dominant.The vibrational states of CO co-products were partially resolved in the ion images.The product total kinetic energy releases,anisotropy parameters(β),and the branching ratios of high-lying CO vibrational states were determined for the S(^(3)P_(J))+CO(X^(1)Σ^(+))channel.We found that the anisotropy parameters suddenly changed from negative to positive when OCS was excited to the higher vibrational levels of the F state.Furthermore,the anisotropy parameters for S(^(3)P_(J))products of J=2,1,0 were even different.These anomalous phenomena may result from the simultaneous existence of both parallel and perpendicular dissociation mechanisms,suggesting the involvement of other electronic states with different symmetry in the initially-excited energy region.This work provides a further understanding of the nonadiabatic couplings in the VUV photodissociation process of OCS.
文摘Microscopes in vacuum ultraviolet and soft X-ray regions using a normal incidence type of Schwarzschild objective are reviewed. The objective consists of a concave mirror and a convex mirror coated with a high reflectance multilayer,having a large numerical aperture comparing with other objectives. The microscopes have been used to diagnose inertia-confinement-fusion plasmas,and to investigate small samples or microstructures of in- organic and organic materials by imaging them using laboratory light sources. Synchrotron radiation has been also used to obtain a microbeam for a photoelectron scanning microscope with a spatial resolution of 0.1 μm. The struc- ture and performance of two laboratory microscopes developed at Tohoku University are demonstrated. One of them is a soft X-ray emission imaging microscope. An image of an artificial pattern made of W and SiO2 on Si wafer by focusing Si L emission was presented. The other is an ultraviolet photoelectron scanning microscope using a He (he- lium) gas discharge lamp. The valence band spectra of a microcrystal of FeWO4 were presented. Furthermore other applications such as demagnifying optics for lithography and optics to gather fluorescence for emission spectroscopy are introduced.