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
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.
