Silicon anodes are promising for use in lithium-ion batteries.However,their practical application is severely limited by their large volume expansion leading to irreversible material fracture and electrical disconnect...Silicon anodes are promising for use in lithium-ion batteries.However,their practical application is severely limited by their large volume expansion leading to irreversible material fracture and electrical disconnects.This study proposes a new top-down strategy for preparing microsize porous silicon and introduces polyacrylonitrile(PAN)for a nitrogen-doped carbon coating,which is designed to maintain the internal pore volume and lower the expansion of the anode during lithiation and delithiation.We then explore the effect of temperature on the evolution of the structure of PAN and the electrochemical behavior of the composite electrode.After treatment at 400℃,the PAN coating retains a high nitrogen content of 11.35 at%,confirming the presence of C—N and C—O bonds that improve the ionic-electronic transport properties.This treatment not only results in a more intact carbon layer structure,but also introduces carbon defects,and produces a material that has remarkable stable cycling even at high rates.When cycled at 4 A g^(-1),the anode had a specific capacity of 857.6 mAh g^(-1) even after 200 cycles,demonstrating great potential for high-capacity energy storage applications.展开更多
Based on spin-unrestricted hartree fock theory, we present the spin unrestricted multi- configuration time dependent hartree lock theory (UMCTDHF) to describe the electron correlation dynamics of systems interacting...Based on spin-unrestricted hartree fock theory, we present the spin unrestricted multi- configuration time dependent hartree lock theory (UMCTDHF) to describe the electron correlation dynamics of systems interacting with laser field. The positive spin orbitals and the negative spin orbitals are propagated in their own subspace respectively. The spin orbital in the spin-down subspace acts with that in the spin-up subspace by the reduced density matrix and mean field operator. The ground energy is acquired by propagating the trial wave function in the imaginary time by using spin-restricted MCTDHF (RMCTDHF) and UMCTDHF respectively. Then the ionization probabilities and the electrons energies are calculated by using RMCTDHF and UMCTDHF when the laser field is present. The ionization probability calculated with UMCTDHF agrees with the previous theoretical reports very well. The UMCTDHF method is accurate and applicable for open shell system beyond the capability of the RMCTDHF method.展开更多
Polysilicon ohmic contacts to n-type 4H-SiC have been fabricated. TLM (transfer length method) test patterns with polysilicon structure are formed on n-wells created by phosphorus ion (P^+) implantation into a Si...Polysilicon ohmic contacts to n-type 4H-SiC have been fabricated. TLM (transfer length method) test patterns with polysilicon structure are formed on n-wells created by phosphorus ion (P^+) implantation into a Si-faced p-type 4H-SiC epilayer. The polysilicon is deposited using low-pressure chemical vapor deposition (LPCVD) and doped by phosphorous ions implantation followed by diffusion to obtain a sheet resistance of 22Ω/□. The specific contact resistance pc of n^+ polysilicon contact to n-type 4H-SiC as low as 3.82 × 10^-5Ω· cm^2 is achieved. The result for sheet resistance Rsh of the phosphorous ion implanted layers in SiC is about 4.9kΩ/□. The mechanisms for n^+ polysilicon ohmic contact to n-type SiC are discussed.展开更多
Aim To analyze the fragmentation patterns of diquaternary dipiperaziniumscontaining dithiocarboxyl groups. Methods Positive ion electrospray ionization mass spectrometry inconjunction with tandem mass spectrometry (ES...Aim To analyze the fragmentation patterns of diquaternary dipiperaziniumscontaining dithiocarboxyl groups. Methods Positive ion electrospray ionization mass spectrometry inconjunction with tandem mass spectrometry (ESI-MS^n) was used. Results The fragment ion [M^(2+) Cl^-]^+ showed characteristic double peaks with high intensity instead of the parent molecular ionbeing detected. And [M^(2+) - CH_3^+ ]^+ ion had relatively low intensity. Meanwhile, [M^(2+) Cl^- -Cl^- - PhCH_2^+ ]^+ species had the highest intensity as the base peak, which was originated from[M^(2+) Cl^- ]^+, The detailed fragmentation mechanisms are supported with the tandem massspectrometry.展开更多
Photon induced dissociation investigations of neutral tyramine and dopamine are carried out with synchrotron vacuum uRraviolet photoionization mass spectrometry and theoretical calculations. At low photon energy, only...Photon induced dissociation investigations of neutral tyramine and dopamine are carried out with synchrotron vacuum uRraviolet photoionization mass spectrometry and theoretical calculations. At low photon energy, only molecular ions are measured by virtue of nearthreshold photoionization. While increasing photon energy to 11.7 eV or more, four distinct fragment ions are obtained for tyramine and dopamine, respectively. Besides, the ionization energies of tyramine and dopamine are determined to be 7.984-0.05 and 7.674-0.05 eV by measuring the photoionization efficiency curves of corresponding molecular ions. With help of density function theory calculations, the detailed fragmentation pathways are established as well. These two molecular cations have similar aminoethyl group elimination pathways, CTHsO2+ (m/z=124) and C7H8O+ (m/z=108) are supposed to be generated by the McLafferty rearrangement via γ-hydrogen (7-H) shift inducing β-fission. And CH2NH2+ is proposed to derive from the direct fission of C7-C8 bond. Besides, the McLafferty rearrangement and the C7-C8 bond fission are validated to be dominant dissociation pathways for tyramine and dopamine cations.展开更多
This work focused on the influence of TiC reinforcing particles on the tribological properties of titanium matrix composites(TMCs)with open porosity,processed by spark plasma sintering(SPS).Materials composed of an eq...This work focused on the influence of TiC reinforcing particles on the tribological properties of titanium matrix composites(TMCs)with open porosity,processed by spark plasma sintering(SPS).Materials composed of an equimolar mixture of Ti and TiH2 with 0,3,10 and 30 vol.% of TiC were sintered at 850 ℃.Nanoindentation and wear tests were carried out to assess the nanohardness and the wear resistance in a tribometer with a reciprocating sliding ball-on-flat configuration.Results showed a nanohardness increment from 5 to 14 GPa with increasing TiC content.The coefficient of friction(CoF)showed a minimum of 0.2 for 10% TiC grade,which also showed the lowest wear rate.For the low TiC content sample,adhesive wear with severe plastic deformation was identified.Meanwhile,medium content TiC sample showed a mechanical mixed layer(MML),whereas high TiC content composite showed abrasive as the main wear mechanism.In conclusion,the wear mechanisms,CoFs and wear volume changed with TiC content.展开更多
Resonance-enhanced multiphoton ionization of the titanium atoms has been investigated in the 293 321 nm wavelength. We couple a laser-ablated metal target into a molecular beam to produce free atoms. Ions produced fro...Resonance-enhanced multiphoton ionization of the titanium atoms has been investigated in the 293 321 nm wavelength. We couple a laser-ablated metal target into a molecular beam to produce free atoms. Ions produced from photoionization of the neutral atoms are monitored by a home-built time-of-flight mass spectrometer. Photoionization cross sections of the excited states of Ti I were deduced from the dependence of the ion signal intensity on the laser intensity for photon energies close to the ionization threshold. The values obtained range from 0.2 Mb to 6.0 Mb. No significant isotope-dependence was found from measurements of the photoionization cross sections of ^46Ti, ^47Ti, and ^48Ti.展开更多
Hierarchical porous Co_(3)O_(4)spheres were synthesized by a solvothermal method followed by high-temperature calcination.XRD,SEM,TEM and electrochemical tests were used to study the structure and performance of the h...Hierarchical porous Co_(3)O_(4)spheres were synthesized by a solvothermal method followed by high-temperature calcination.XRD,SEM,TEM and electrochemical tests were used to study the structure and performance of the hierarchical porous Co_(3)O_(4)spheres.The results show that the Co_(3)O_(4)synthesized at a calcination temperature of 700°C(Co_(3)O_(4)-700)is micro-sized spheres(1-2μm)consisting of plentiful nanoparticles(50-200 nm)and numerous pores(~100 nm).Due to its numerous porous morphology,the Co_(3)O_(4)-700 anode exhibits the highest cycling performance with excellent reversible discharge and charge specific capacities of 745 and 755 m A·h/g at the current density of 100 m A/g after 100 charge-discharge cycles,respectively.展开更多
The multiphoton ionization of acetone-water clusters were detected at 355 nm laser wavelength by using the time of flight mass spectrometer(TOF-MS). The experiments show that all products are proto- nated. Three mai...The multiphoton ionization of acetone-water clusters were detected at 355 nm laser wavelength by using the time of flight mass spectrometer(TOF-MS). The experiments show that all products are proto- nated. Three main products such as (CH3COCH3),-(H2O)n_2 H^+ , (CH3COCH3),-(H2O)n-1 H^+ and (CH3COCH3),-(H2O),H^+ are concluded from the results. In order to study the equilibrium structures of the (CH3 COCH3 ),-(H2O)n-2 H^+ , the ab-initio calculation is used on them. The experiment is even done when the volume rate of acetone to water is 1:2.展开更多
Applying time-independent non-perturbative formalism to the photo-ionization of hydrogen atom immersed in a strong circularly polarized standing electromagnetic wave, we calculate the shift of energy levels and the di...Applying time-independent non-perturbative formalism to the photo-ionization of hydrogen atom immersed in a strong circularly polarized standing electromagnetic wave, we calculate the shift of energy levels and the distortion of wave functions for the hydrogen atom, the ionization cross section induced by the standing wave, and the angular distribution of photoelectrons and obtain some interesting results.展开更多
Sliced velocity mapping ion imaging technique was employed to investigate the dynamics of the hydroxyl elimination channel in the photodissociaiton of nitric acid in the ultraviolet region. The OH product was detected...Sliced velocity mapping ion imaging technique was employed to investigate the dynamics of the hydroxyl elimination channel in the photodissociaiton of nitric acid in the ultraviolet region. The OH product was detected by (2+1) resonance enhanced multiphoton ionization via the D^2∑^- electronic state. The total kinetic energy spectra of the OH+NO2 channel from the photolysis of HONO2 show that both :NO2(X2A1) and NO2(A2B2) channels are present, suggesting that both 1^1A″ and 2^1A″ excited electronic states of HONO2 are involved in the excitation. The parallel angular distributions suggest that the dissociation of the nitric acid is a fast process in comparison with the rotational period of the HNO3 molecule. The anisotropy parameter β for the hydroxyl elimination channel is found to be dependent on the OH product rotational state as well as the photolysis energy.展开更多
The geometric structures and vibration frequencies of para-chlorofluorobenzene(p-Cl FPh)in the first excited state of neutral and ground state of cation were investigated by resonanceenhanced multiphoton ionization an...The geometric structures and vibration frequencies of para-chlorofluorobenzene(p-Cl FPh)in the first excited state of neutral and ground state of cation were investigated by resonanceenhanced multiphoton ionization and slow electron velocity-map imaging.The infrared spectrum of S0 state and absorption spectrum for S1←S0 transition in p-Cl FPh were also recorded.Based on the one-color resonant two-photon ionization spectrum and two-color resonant two-photon ionization spectrum,we obtained the adiabatic excited-state energy of p-Cl FPh as 36302±4 cm^-1.In the two-color resonant two-photon ionization slow electron velocity-map imagin spectra,the accurate adiabatic ionization potential of p-Cl FPh was extrapolated as 72937±8 cm^-1 via threshold ionization measurement.In addition,FranckCondon simulation was performed to help us confidently ascertain the main vibrational modes in the S1 and D0 states.Furthermore,the mixing of vibrational modes between S0→S1 and S1→D0 has been analyzed.展开更多
Langevin dynamics simulations were conducted to study the collapse of grafted partially charged 4-arm star chains onto the oppositely charged grafting electrode in the presence of trivalent salt coions.Simulation resu...Langevin dynamics simulations were conducted to study the collapse of grafted partially charged 4-arm star chains onto the oppositely charged grafting electrode in the presence of trivalent salt coions.Simulation results reveal that the average charge fraction of the grafted star chains and the salt concentration play critical roles in the competitive adsorption of charged monomers and trivalent salt coions onto the oppositely charged electrode.For grafted star chains with relatively high charge fraction,charged monomers are the dominant species collapsing on the oppositely charged electrode with the emergence of charge reversal on the grafting electrode.At a low charge fraction such that the total amount of charges on a grafted star molecule is comparable to that of a trivalent salt coion,trivalent salt coions absorb more strongly onto the electrode than grafted stars even at very low salt concentration.It is found that at relatively low charge fraction of star chains,the addition of trivalent salt coions does not lead to charge overcompensation of the surface charges on the grafting electrode.The stretching of star brushes under an electric field in the presence of trivalent salt coions was also briefly investigated.展开更多
The photodissociation dynamics of acetaldehyde in the radical channel CH3+HCO has been reinvestigated using time-sliced velocity map imaging technique in the photolysis wavelength range of 275-321 nm. The CH3 fragmen...The photodissociation dynamics of acetaldehyde in the radical channel CH3+HCO has been reinvestigated using time-sliced velocity map imaging technique in the photolysis wavelength range of 275-321 nm. The CH3 fragments have been probed via (2+1) resonance-enhanced multiphoton ionization. Images are measured for CH3 formed in the ground and excited states (v2=0 and 1) of the umbrella vibrational mode. For acetaldehyde dissociation on T1 state after intersystem crossing from S1 state, the products are formed with high translational energy release and low internal excitation. The rotational and vibrational energy of both fragments increases with increasing photodissociation energy. The triplet barrier height is estimated at 3.8814-0.006 eV above the ground state of acetaldehyde.展开更多
文摘Silicon anodes are promising for use in lithium-ion batteries.However,their practical application is severely limited by their large volume expansion leading to irreversible material fracture and electrical disconnects.This study proposes a new top-down strategy for preparing microsize porous silicon and introduces polyacrylonitrile(PAN)for a nitrogen-doped carbon coating,which is designed to maintain the internal pore volume and lower the expansion of the anode during lithiation and delithiation.We then explore the effect of temperature on the evolution of the structure of PAN and the electrochemical behavior of the composite electrode.After treatment at 400℃,the PAN coating retains a high nitrogen content of 11.35 at%,confirming the presence of C—N and C—O bonds that improve the ionic-electronic transport properties.This treatment not only results in a more intact carbon layer structure,but also introduces carbon defects,and produces a material that has remarkable stable cycling even at high rates.When cycled at 4 A g^(-1),the anode had a specific capacity of 857.6 mAh g^(-1) even after 200 cycles,demonstrating great potential for high-capacity energy storage applications.
文摘Based on spin-unrestricted hartree fock theory, we present the spin unrestricted multi- configuration time dependent hartree lock theory (UMCTDHF) to describe the electron correlation dynamics of systems interacting with laser field. The positive spin orbitals and the negative spin orbitals are propagated in their own subspace respectively. The spin orbital in the spin-down subspace acts with that in the spin-up subspace by the reduced density matrix and mean field operator. The ground energy is acquired by propagating the trial wave function in the imaginary time by using spin-restricted MCTDHF (RMCTDHF) and UMCTDHF respectively. Then the ionization probabilities and the electrons energies are calculated by using RMCTDHF and UMCTDHF when the laser field is present. The ionization probability calculated with UMCTDHF agrees with the previous theoretical reports very well. The UMCTDHF method is accurate and applicable for open shell system beyond the capability of the RMCTDHF method.
文摘Polysilicon ohmic contacts to n-type 4H-SiC have been fabricated. TLM (transfer length method) test patterns with polysilicon structure are formed on n-wells created by phosphorus ion (P^+) implantation into a Si-faced p-type 4H-SiC epilayer. The polysilicon is deposited using low-pressure chemical vapor deposition (LPCVD) and doped by phosphorous ions implantation followed by diffusion to obtain a sheet resistance of 22Ω/□. The specific contact resistance pc of n^+ polysilicon contact to n-type 4H-SiC as low as 3.82 × 10^-5Ω· cm^2 is achieved. The result for sheet resistance Rsh of the phosphorous ion implanted layers in SiC is about 4.9kΩ/□. The mechanisms for n^+ polysilicon ohmic contact to n-type SiC are discussed.
文摘Aim To analyze the fragmentation patterns of diquaternary dipiperaziniumscontaining dithiocarboxyl groups. Methods Positive ion electrospray ionization mass spectrometry inconjunction with tandem mass spectrometry (ESI-MS^n) was used. Results The fragment ion [M^(2+) Cl^-]^+ showed characteristic double peaks with high intensity instead of the parent molecular ionbeing detected. And [M^(2+) - CH_3^+ ]^+ ion had relatively low intensity. Meanwhile, [M^(2+) Cl^- -Cl^- - PhCH_2^+ ]^+ species had the highest intensity as the base peak, which was originated from[M^(2+) Cl^- ]^+, The detailed fragmentation mechanisms are supported with the tandem massspectrometry.
基金Authors thank Dr. Yang Pan for useful discussions This work was supported by the National Natural Science Foundation of China (No.10805047).
文摘Photon induced dissociation investigations of neutral tyramine and dopamine are carried out with synchrotron vacuum uRraviolet photoionization mass spectrometry and theoretical calculations. At low photon energy, only molecular ions are measured by virtue of nearthreshold photoionization. While increasing photon energy to 11.7 eV or more, four distinct fragment ions are obtained for tyramine and dopamine, respectively. Besides, the ionization energies of tyramine and dopamine are determined to be 7.984-0.05 and 7.674-0.05 eV by measuring the photoionization efficiency curves of corresponding molecular ions. With help of density function theory calculations, the detailed fragmentation pathways are established as well. These two molecular cations have similar aminoethyl group elimination pathways, CTHsO2+ (m/z=124) and C7H8O+ (m/z=108) are supposed to be generated by the McLafferty rearrangement via γ-hydrogen (7-H) shift inducing β-fission. And CH2NH2+ is proposed to derive from the direct fission of C7-C8 bond. Besides, the McLafferty rearrangement and the C7-C8 bond fission are validated to be dominant dissociation pathways for tyramine and dopamine cations.
基金The Mexican Council of Science and Technology (CONACYT) for the support received under the scholarship (449474)
文摘This work focused on the influence of TiC reinforcing particles on the tribological properties of titanium matrix composites(TMCs)with open porosity,processed by spark plasma sintering(SPS).Materials composed of an equimolar mixture of Ti and TiH2 with 0,3,10 and 30 vol.% of TiC were sintered at 850 ℃.Nanoindentation and wear tests were carried out to assess the nanohardness and the wear resistance in a tribometer with a reciprocating sliding ball-on-flat configuration.Results showed a nanohardness increment from 5 to 14 GPa with increasing TiC content.The coefficient of friction(CoF)showed a minimum of 0.2 for 10% TiC grade,which also showed the lowest wear rate.For the low TiC content sample,adhesive wear with severe plastic deformation was identified.Meanwhile,medium content TiC sample showed a mechanical mixed layer(MML),whereas high TiC content composite showed abrasive as the main wear mechanism.In conclusion,the wear mechanisms,CoFs and wear volume changed with TiC content.
基金V. ACKNOWLEDGMENTS This work is supported by the National Natural Science Foundation of China (No.10674002 and No.20973001) and the Science Foundation of Anhui Education Committee (No.ZD2007001-1).
文摘Resonance-enhanced multiphoton ionization of the titanium atoms has been investigated in the 293 321 nm wavelength. We couple a laser-ablated metal target into a molecular beam to produce free atoms. Ions produced from photoionization of the neutral atoms are monitored by a home-built time-of-flight mass spectrometer. Photoionization cross sections of the excited states of Ti I were deduced from the dependence of the ion signal intensity on the laser intensity for photon energies close to the ionization threshold. The values obtained range from 0.2 Mb to 6.0 Mb. No significant isotope-dependence was found from measurements of the photoionization cross sections of ^46Ti, ^47Ti, and ^48Ti.
基金funded by the Natural Science Foundation of Hunan Province,China(No.2020JJ4729)。
文摘Hierarchical porous Co_(3)O_(4)spheres were synthesized by a solvothermal method followed by high-temperature calcination.XRD,SEM,TEM and electrochemical tests were used to study the structure and performance of the hierarchical porous Co_(3)O_(4)spheres.The results show that the Co_(3)O_(4)synthesized at a calcination temperature of 700°C(Co_(3)O_(4)-700)is micro-sized spheres(1-2μm)consisting of plentiful nanoparticles(50-200 nm)and numerous pores(~100 nm).Due to its numerous porous morphology,the Co_(3)O_(4)-700 anode exhibits the highest cycling performance with excellent reversible discharge and charge specific capacities of 745 and 755 m A·h/g at the current density of 100 m A/g after 100 charge-discharge cycles,respectively.
文摘The multiphoton ionization of acetone-water clusters were detected at 355 nm laser wavelength by using the time of flight mass spectrometer(TOF-MS). The experiments show that all products are proto- nated. Three main products such as (CH3COCH3),-(H2O)n_2 H^+ , (CH3COCH3),-(H2O)n-1 H^+ and (CH3COCH3),-(H2O),H^+ are concluded from the results. In order to study the equilibrium structures of the (CH3 COCH3 ),-(H2O)n-2 H^+ , the ab-initio calculation is used on them. The experiment is even done when the volume rate of acetone to water is 1:2.
基金The project supported by National Natural Science Foundation of China under Grant No.10075004 with the calculations supported by the High Performance Computing Center of China (Beijing)
文摘Applying time-independent non-perturbative formalism to the photo-ionization of hydrogen atom immersed in a strong circularly polarized standing electromagnetic wave, we calculate the shift of energy levels and the distortion of wave functions for the hydrogen atom, the ionization cross section induced by the standing wave, and the angular distribution of photoelectrons and obtain some interesting results.
基金Ⅴ. ACKNOWLEDGMENTS This work was supported by the National Natural Science Foundation of China, the Ministry of Sciences and Technology, and the Chinese Academy of Sciences.
文摘Sliced velocity mapping ion imaging technique was employed to investigate the dynamics of the hydroxyl elimination channel in the photodissociaiton of nitric acid in the ultraviolet region. The OH product was detected by (2+1) resonance enhanced multiphoton ionization via the D^2∑^- electronic state. The total kinetic energy spectra of the OH+NO2 channel from the photolysis of HONO2 show that both :NO2(X2A1) and NO2(A2B2) channels are present, suggesting that both 1^1A″ and 2^1A″ excited electronic states of HONO2 are involved in the excitation. The parallel angular distributions suggest that the dissociation of the nitric acid is a fast process in comparison with the rotational period of the HNO3 molecule. The anisotropy parameter β for the hydroxyl elimination channel is found to be dependent on the OH product rotational state as well as the photolysis energy.
基金the National Natural Science Foundation of China(No.11674003,No.21873003,No.21503003,No.11704004,and No.61475001)Anhui Natural Science Foundation(No.1908085QA17)+1 种基金support from Special Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund(the second phase)(No.U1501501)Super Computation Center of Shenzhen。
文摘The geometric structures and vibration frequencies of para-chlorofluorobenzene(p-Cl FPh)in the first excited state of neutral and ground state of cation were investigated by resonanceenhanced multiphoton ionization and slow electron velocity-map imaging.The infrared spectrum of S0 state and absorption spectrum for S1←S0 transition in p-Cl FPh were also recorded.Based on the one-color resonant two-photon ionization spectrum and two-color resonant two-photon ionization spectrum,we obtained the adiabatic excited-state energy of p-Cl FPh as 36302±4 cm^-1.In the two-color resonant two-photon ionization slow electron velocity-map imagin spectra,the accurate adiabatic ionization potential of p-Cl FPh was extrapolated as 72937±8 cm^-1 via threshold ionization measurement.In addition,FranckCondon simulation was performed to help us confidently ascertain the main vibrational modes in the S1 and D0 states.Furthermore,the mixing of vibrational modes between S0→S1 and S1→D0 has been analyzed.
基金supported by the National Natural Science Foundation of China (No.21774067)the support from K. C. Wong Magna Fund in Ningbo University。
文摘Langevin dynamics simulations were conducted to study the collapse of grafted partially charged 4-arm star chains onto the oppositely charged grafting electrode in the presence of trivalent salt coions.Simulation results reveal that the average charge fraction of the grafted star chains and the salt concentration play critical roles in the competitive adsorption of charged monomers and trivalent salt coions onto the oppositely charged electrode.For grafted star chains with relatively high charge fraction,charged monomers are the dominant species collapsing on the oppositely charged electrode with the emergence of charge reversal on the grafting electrode.At a low charge fraction such that the total amount of charges on a grafted star molecule is comparable to that of a trivalent salt coion,trivalent salt coions absorb more strongly onto the electrode than grafted stars even at very low salt concentration.It is found that at relatively low charge fraction of star chains,the addition of trivalent salt coions does not lead to charge overcompensation of the surface charges on the grafting electrode.The stretching of star brushes under an electric field in the presence of trivalent salt coions was also briefly investigated.
基金ACKNOWLEDGMENTS This work was supported by the National Natural Science Foundation of China (No.21203186 and No.21073187), the National Key Basic Research Program of China (No.2010CB923302), 100 Talents Program of Chinese Academy of Sciences, and Knowledge Innovation Program of Chinese Academy of Sciences.
文摘The photodissociation dynamics of acetaldehyde in the radical channel CH3+HCO has been reinvestigated using time-sliced velocity map imaging technique in the photolysis wavelength range of 275-321 nm. The CH3 fragments have been probed via (2+1) resonance-enhanced multiphoton ionization. Images are measured for CH3 formed in the ground and excited states (v2=0 and 1) of the umbrella vibrational mode. For acetaldehyde dissociation on T1 state after intersystem crossing from S1 state, the products are formed with high translational energy release and low internal excitation. The rotational and vibrational energy of both fragments increases with increasing photodissociation energy. The triplet barrier height is estimated at 3.8814-0.006 eV above the ground state of acetaldehyde.