As one of the major volatile components in extraterrestrial materials,nitrogen(N2)isotopes serve not only as tracers for the formation and evolution of the solar system,but also play a critical role in assessing pl...As one of the major volatile components in extraterrestrial materials,nitrogen(N2)isotopes serve not only as tracers for the formation and evolution of the solar system,but also play a critical role in assessing planetary habitability and the search for extraterrestrial life.The integrated measurement of N2and argon(Ar)isotopes by using noble gas mass spectrometry represents a state-of-the-art technique for such investigations.To support the growing demands of planetary science research in China,we have developed a high-efficiency,high-precision method for the integrated analysis of N2and Ar isotopes.This was achieved by enhancing gas extraction and purification systems and integrating them with a static noble gas mass spectrometer.This method enables integrated N2-Ar isotope measurements on submilligram samples,significantly improving sample utilization and reducing the impact of sample heterogeneity on volatile analysis.The system integrates CO2laser heating,a modular two-stage Zr-Al getter pump,and a CuO furnace-based purification process,effectively reducing background levels(N2blank as low as 0.35×10−6cubic centimeters at standard temperature and pressure[ccSTP]).Analytical precision is ensured through calibration with atmospheric air and CO corrections.To validate the reliability of the method,we performed N2-Ar isotope analyses on the Allende carbonaceous chondrite,one of the most extensively studied meteorites internationally.The measured N2concentrations range from 19.2 to 29.8 ppm,withδ15N values between−44.8‰and−33.0‰.Concentrations of 40Ar,36Ar,and 38Ar are(12.5-21.1)×10−6ccSTP/g,(90.9-150.3)×10−9ccSTP/g,and(19.2-30.7)×10−9ccSTP/g,respectively.These values correspond to cosmic-ray exposure ages of 4.5-5.7 Ma,consistent with previous reports.Step-heating experiments further reveal distinct release patterns of N and Ar isotopes,as well as their associations with specific mineral phases in the meteorite.In summary,the combined N2-Ar isotopic system offers significant advantages for tracing volatile sources in extraterrestrial materials and will provide essential analytical support for upcoming Chinese planetary missions,such as Tianwen-2.展开更多
The cross sections and rate constants for the formation of phosphorus monobromide(PBr)and phosphorus monoiodide(PI)radicals through radiative association have been theoretically estimated using fully quantum mechanica...The cross sections and rate constants for the formation of phosphorus monobromide(PBr)and phosphorus monoiodide(PI)radicals through radiative association have been theoretically estimated using fully quantum mechanical methods.For temperatures ranging from 10 K to 15000 K,the thermal rate coefficients are found to vary from 2.86×10-23cm3·s-1to 1.20×10-18cm3·s-1and from 7.73×10-24cm3·s-1cm3·s-1to 1.12×10-18cm3·s-1for PBr and PI,respectively.Implications of PBr and PI radiative association to various astrochemical environments are briefly discussed.展开更多
In the interstellar medium,formic acid(HCOOH)plays a significant role in the synthesis of the simplest amino acid,glycine(NH2CH2COOH).The presence of HCOOH suggests that oxygen-bearing molecules may be directly ...In the interstellar medium,formic acid(HCOOH)plays a significant role in the synthesis of the simplest amino acid,glycine(NH2CH2COOH).The presence of HCOOH suggests that oxygen-bearing molecules may be directly involved in the chemical and physical evolution of star formation regions,particularly in hot molecular cores.This paper presents the first detection of the rotational emission lines of the trans-conformer of HCOOH toward the hot molecular core G358.93-0.03 MM1,located in the massive star formation region G358.93-0.03.This study employed high-resolution observations from the Atacama Large Millimeter/submillimeter Array in Band 7.The column density and excitation temperature of t-HCOOH are determined as(8.13±0.72)×1015cm-2 and 120±15 K,respectively.The fractional abundance of t-HCOOH relative to H2 is(2.62±0.29)×10-9.The column density ratios of t-HCOOH/CH3OH and t-HCOOH/H2CO are(1.56±0.12)×10-2 and(1.16±0.12),respectively.We computed a three-phase warm-up chemical model of HCOOH using the gas-grain chemical code UCLCHEM.We found that the observed and modeled abundances of HCOOH are almost identical,within a factor of 0.89.Based on chemical modeling,we showed that HCOOH may be formed through the reaction between HCO and OH on the grain surface,which is further released in the gas-phase.展开更多
The encounter desorption(ED)approach significantly deviates from the more rigorous microscopic Monte Carlo method when the surface H2coverage is high.We propose an improved method that removes this limitation under...The encounter desorption(ED)approach significantly deviates from the more rigorous microscopic Monte Carlo method when the surface H2coverage is high.We propose an improved method that removes this limitation under high H2coverage.This method is applied to explain the coverage-dependent H2desorption energy observed in experiments,EexptD2(θ).Hydrogen molecules adsorbed on bare surfaces and those adsorbed on H2substrates are distinguished and treated as different species,each characterized by distinct diffusion barriers and desorption energies.We find that the effective desorption energy calculated using the improved method shows much better agreement with EexptD2(θ)than that obtained with the conventional ED approach.Moreover,the improved method clearly outperforms the original approach under conditions of high surface H2coverage.展开更多
Ammonia hydrates are important components in planetary interiors,among which ammonia hemihydrate(AHH)exhibits remarkable stability under high pressure.In this study,we report for the first time the elastic properties ...Ammonia hydrates are important components in planetary interiors,among which ammonia hemihydrate(AHH)exhibits remarkable stability under high pressure.In this study,we report for the first time the elastic properties of the recently discovered quasibcc ammonia hemihydrate(AHH-qbcc)at high pressures,using externally heated diamond anvil cells combined with Raman spectroscopy and Brillouin scattering.We synthesized single crystals of AHH-qbcc in the diamond anvil cell(DAC).Subsequently,we measured its full elastic tensor up to 17.6 GPa at room temperature via Brillouin scattering.The results show that the elastic constants increase linearly with increasing pressure.Based on the obtained elastic constants,we calculated the bulk modulus,shear modulus,Poisson's ratio,and velocity anisotropy.The results reveal significant anisotropy in wave velocities and Poisson's ratio on the(110)crystallographic plane of AHHqbcc.Compared to iceⅦ,AHH-qbcc has a lower bulk modulus and shear modulus,yet exhibits a higher compressional wave velocity and a similar shear wave velocity.Our findings provide important constraints for understanding the internal structure and seismic velocity profiles of icy planets.展开更多
The 2024 MRE HP Special Volume selects papers on new theoretical and experimental developments in the use of static largevolume presses(LVPs)1–3 and dynamic compression4,5 for studies under extreme high-pressure and ...The 2024 MRE HP Special Volume selects papers on new theoretical and experimental developments in the use of static largevolume presses(LVPs)1–3 and dynamic compression4,5 for studies under extreme high-pressure and high-temperature(HPHT)conditions.It also continues the previous year’s6 contemporary focus on superhydrides7–11 with extremely high superconducting temperatures Tc and addresses some controversial issues.12–14 In addition,it explores unconventional pressure-induced chemistry,particularly novel chemical stoichiometry and its impact on geochemistry and cosmochemistry in the deep interiors of Earth and other planets.18–21.展开更多
Sulfur-bearing species are widely utilized to investigate the physical structure of star-forming regions in interstellar media;however,the underlying sulfur chemistry in these environments remains poorly understood.Th...Sulfur-bearing species are widely utilized to investigate the physical structure of star-forming regions in interstellar media;however,the underlying sulfur chemistry in these environments remains poorly understood.Therefore,further studies of S-bearing species are fundamentally important,as they can enhance our understanding of the physical evolution of star-forming regions.This study presents observations of C2S and C3S in L1544,acquired using the Nanshan 26-m radio telescope,along with simulations of their chemical behavior using a one-dimensional physical model.The simulation results reveal significant radial variations in the column densities of C2S and C3S.Additionally,the column densities of both molecules are found to be sensitive to the cosmic ray ionization rate at several radial positions,while variations in the C/O ratio have comparatively minimal impact on L1544.展开更多
We obtain the rotational spectra for cyanopolyynes HC2n+1N(n=0-8)and their cations through quantum chemical calculations.Rotational constants,quartic centrifugal distortion constants,and hyperfine constants are cal...We obtain the rotational spectra for cyanopolyynes HC2n+1N(n=0-8)and their cations through quantum chemical calculations.Rotational constants,quartic centrifugal distortion constants,and hyperfine constants are calculated.The rotational constants are determined at the theoretical level of B3PW91/cc-pVTZ,incorporating with the calibration for the moment of inertia.This significantly improves the accuracy with respect to the uncalibrated ones.Quartic centrifugal distortion constants are estimated using the empirical relation,achieving an accuracy of∼0.02%with respect to the experiment.Hyperfine constants are computed at the B3PW91/6-311+G(df,pd)and B3PW91/aug-cc-pVTZ levels.The overall frequency characteristics of all the target molecules are discussed and their detectability in the interstellar medium is also quantitatively evaluated.The rotational spectra of selected species(HC13N,HC15N,HC17N,and HC5N+)are reproduced,showing satisfied consistency with experiments or observations.Our results provide useful reference for observations and experiments,even that more advanced calculation levels and basis sets are required to achieve better accuracy.展开更多
基金supported by the Bureau of Frontier Sciences and Basic Research,Chinese Academy of Sciences(Grant No.QYJ-2025-0103)the National Natural Science Foundation of China(Grant Nos.42441834,42241105,42441825,and 42203048)the Key Research Program of the Institute of Geology and Geophysics,Chinese Academy of Sciences(Grant No.IGGCAS-202401).
摘要As one of the major volatile components in extraterrestrial materials,nitrogen(N2)isotopes serve not only as tracers for the formation and evolution of the solar system,but also play a critical role in assessing planetary habitability and the search for extraterrestrial life.The integrated measurement of N2and argon(Ar)isotopes by using noble gas mass spectrometry represents a state-of-the-art technique for such investigations.To support the growing demands of planetary science research in China,we have developed a high-efficiency,high-precision method for the integrated analysis of N2and Ar isotopes.This was achieved by enhancing gas extraction and purification systems and integrating them with a static noble gas mass spectrometer.This method enables integrated N2-Ar isotope measurements on submilligram samples,significantly improving sample utilization and reducing the impact of sample heterogeneity on volatile analysis.The system integrates CO2laser heating,a modular two-stage Zr-Al getter pump,and a CuO furnace-based purification process,effectively reducing background levels(N2blank as low as 0.35×10−6cubic centimeters at standard temperature and pressure[ccSTP]).Analytical precision is ensured through calibration with atmospheric air and CO corrections.To validate the reliability of the method,we performed N2-Ar isotope analyses on the Allende carbonaceous chondrite,one of the most extensively studied meteorites internationally.The measured N2concentrations range from 19.2 to 29.8 ppm,withδ15N values between−44.8‰and−33.0‰.Concentrations of 40Ar,36Ar,and 38Ar are(12.5-21.1)×10−6ccSTP/g,(90.9-150.3)×10−9ccSTP/g,and(19.2-30.7)×10−9ccSTP/g,respectively.These values correspond to cosmic-ray exposure ages of 4.5-5.7 Ma,consistent with previous reports.Step-heating experiments further reveal distinct release patterns of N and Ar isotopes,as well as their associations with specific mineral phases in the meteorite.In summary,the combined N2-Ar isotopic system offers significant advantages for tracing volatile sources in extraterrestrial materials and will provide essential analytical support for upcoming Chinese planetary missions,such as Tianwen-2.
基金Project supported by the Science and Technology Development Plan Project of Jilin Province,China(Grant No.YDZJ202201ZYTS314)the National Natural Science Foundation of China(Grant Nos.12274178 and 11874177)the support from the High Performance Computing Center(HPCC)of Jilin University and the High-Performance Computing Cluster Tiger@IAMP。
摘要The cross sections and rate constants for the formation of phosphorus monobromide(PBr)and phosphorus monoiodide(PI)radicals through radiative association have been theoretically estimated using fully quantum mechanical methods.For temperatures ranging from 10 K to 15000 K,the thermal rate coefficients are found to vary from 2.86×10-23cm3·s-1to 1.20×10-18cm3·s-1and from 7.73×10-24cm3·s-1cm3·s-1to 1.12×10-18cm3·s-1for PBr and PI,respectively.Implications of PBr and PI radiative association to various astrochemical environments are briefly discussed.
基金the Swami Vivekananda Merit-cum-Means Scholarship(SVMCM)for providing financial support for this research。
摘要In the interstellar medium,formic acid(HCOOH)plays a significant role in the synthesis of the simplest amino acid,glycine(NH2CH2COOH).The presence of HCOOH suggests that oxygen-bearing molecules may be directly involved in the chemical and physical evolution of star formation regions,particularly in hot molecular cores.This paper presents the first detection of the rotational emission lines of the trans-conformer of HCOOH toward the hot molecular core G358.93-0.03 MM1,located in the massive star formation region G358.93-0.03.This study employed high-resolution observations from the Atacama Large Millimeter/submillimeter Array in Band 7.The column density and excitation temperature of t-HCOOH are determined as(8.13±0.72)×1015cm-2 and 120±15 K,respectively.The fractional abundance of t-HCOOH relative to H2 is(2.62±0.29)×10-9.The column density ratios of t-HCOOH/CH3OH and t-HCOOH/H2CO are(1.56±0.12)×10-2 and(1.16±0.12),respectively.We computed a three-phase warm-up chemical model of HCOOH using the gas-grain chemical code UCLCHEM.We found that the observed and modeled abundances of HCOOH are almost identical,within a factor of 0.89.Based on chemical modeling,we showed that HCOOH may be formed through the reaction between HCO and OH on the grain surface,which is further released in the gas-phase.
基金supported by the National Natural Science Foundation of China(No.12173023)。
摘要The encounter desorption(ED)approach significantly deviates from the more rigorous microscopic Monte Carlo method when the surface H2coverage is high.We propose an improved method that removes this limitation under high H2coverage.This method is applied to explain the coverage-dependent H2desorption energy observed in experiments,EexptD2(θ).Hydrogen molecules adsorbed on bare surfaces and those adsorbed on H2substrates are distinguished and treated as different species,each characterized by distinct diffusion barriers and desorption energies.We find that the effective desorption energy calculated using the improved method shows much better agreement with EexptD2(θ)than that obtained with the conventional ED approach.Moreover,the improved method clearly outperforms the original approach under conditions of high surface H2coverage.
基金supported by the Synergetic Extreme Condition User Facility(SECUF)the National Natural Science Foundation of China(Grants Nos.42472065,12274168,and 42102030)+2 种基金the Jilin Provincial Science and Technology Development Project(Grant No.SKL202502017JC)the Technology Development Plan Project of Changchun,China(Grant No.2024GZZ06)the Project of"Medical+X"Interdisciplinary Innovation Team of Norman Bethune Health Science Center of Jilin University(Grant No.2025JBGS03)。
摘要Ammonia hydrates are important components in planetary interiors,among which ammonia hemihydrate(AHH)exhibits remarkable stability under high pressure.In this study,we report for the first time the elastic properties of the recently discovered quasibcc ammonia hemihydrate(AHH-qbcc)at high pressures,using externally heated diamond anvil cells combined with Raman spectroscopy and Brillouin scattering.We synthesized single crystals of AHH-qbcc in the diamond anvil cell(DAC).Subsequently,we measured its full elastic tensor up to 17.6 GPa at room temperature via Brillouin scattering.The results show that the elastic constants increase linearly with increasing pressure.Based on the obtained elastic constants,we calculated the bulk modulus,shear modulus,Poisson's ratio,and velocity anisotropy.The results reveal significant anisotropy in wave velocities and Poisson's ratio on the(110)crystallographic plane of AHHqbcc.Compared to iceⅦ,AHH-qbcc has a lower bulk modulus and shear modulus,yet exhibits a higher compressional wave velocity and a similar shear wave velocity.Our findings provide important constraints for understanding the internal structure and seismic velocity profiles of icy planets.
基金financial support from the Shanghai Key Laboratory of MFree,China(Grant No.22dz2260800)the Shanghai Science and Technology Committee,China(Grant No.22JC1410300).
摘要The 2024 MRE HP Special Volume selects papers on new theoretical and experimental developments in the use of static largevolume presses(LVPs)1–3 and dynamic compression4,5 for studies under extreme high-pressure and high-temperature(HPHT)conditions.It also continues the previous year’s6 contemporary focus on superhydrides7–11 with extremely high superconducting temperatures Tc and addresses some controversial issues.12–14 In addition,it explores unconventional pressure-induced chemistry,particularly novel chemical stoichiometry and its impact on geochemistry and cosmochemistry in the deep interiors of Earth and other planets.18–21.
基金the support from the Natural Science Foundation of Xinjiang Uygur Autonomous Region(Grant No.2024D01E37)the National Science Foundation of China(Grant No.12473025)+5 种基金funded by the National Natural Science Foundation of China(Grant Nos.12373026,12203091,12173075,and 11973076)the Xinjiang Tianchi Talent Program(2024)the support from the Xinjiang Tianchi Talent Program(2023)the Shanghai Natural Science Foundation(Grant No.22ZR1421400)the Natural Science Foundation of Xinjiang Uygur Autonomous Region(Grant No.2022D01A156)partially funded by the Regional Collaborative Innovation Project of Xin jiang Uyghur Autonomous Region(Grant No.2022E01050)。
摘要Sulfur-bearing species are widely utilized to investigate the physical structure of star-forming regions in interstellar media;however,the underlying sulfur chemistry in these environments remains poorly understood.Therefore,further studies of S-bearing species are fundamentally important,as they can enhance our understanding of the physical evolution of star-forming regions.This study presents observations of C2S and C3S in L1544,acquired using the Nanshan 26-m radio telescope,along with simulations of their chemical behavior using a one-dimensional physical model.The simulation results reveal significant radial variations in the column densities of C2S and C3S.Additionally,the column densities of both molecules are found to be sensitive to the cosmic ray ionization rate at several radial positions,while variations in the C/O ratio have comparatively minimal impact on L1544.
基金funded by the Scientific Research Foundation of Education Bureau of Hunan Province(No.23A0132)the National Natural Science Foundation of China(NSFC)under Nos.12333005,12122302 and 62205278the Innovative Research Group Project of Natural Science Foundation of Hunan Province of China No.2024JJ1008.
摘要We obtain the rotational spectra for cyanopolyynes HC2n+1N(n=0-8)and their cations through quantum chemical calculations.Rotational constants,quartic centrifugal distortion constants,and hyperfine constants are calculated.The rotational constants are determined at the theoretical level of B3PW91/cc-pVTZ,incorporating with the calibration for the moment of inertia.This significantly improves the accuracy with respect to the uncalibrated ones.Quartic centrifugal distortion constants are estimated using the empirical relation,achieving an accuracy of∼0.02%with respect to the experiment.Hyperfine constants are computed at the B3PW91/6-311+G(df,pd)and B3PW91/aug-cc-pVTZ levels.The overall frequency characteristics of all the target molecules are discussed and their detectability in the interstellar medium is also quantitatively evaluated.The rotational spectra of selected species(HC13N,HC15N,HC17N,and HC5N+)are reproduced,showing satisfied consistency with experiments or observations.Our results provide useful reference for observations and experiments,even that more advanced calculation levels and basis sets are required to achieve better accuracy.