Adiabatic and vertical ionization potentials （IPs） mad valence electron affmities （EAs） of alaninamide in gas phase have been detennined using density functional theory （BLYP, B3LYP, B3P86） methods with 6-311＋...Adiabatic and vertical ionization potentials （IPs） mad valence electron affmities （EAs） of alaninamide in gas phase have been detennined using density functional theory （BLYP, B3LYP, B3P86） methods with 6-311＋＋G（d, p） basis set, respectively. IPs and EAs of alaninamide in solutions have been calculated at the B3LYP/6-311＋＋G（d, p） level. Five possible conformers of alaninamide and their charged states have been optimized employing density functional theory B3LYP method with 6-311＋＋（d, p） basis set, respectively.展开更多
Abstract In this work, ionization potentials and quantum effects of ls^2 np^2 P Rydberg states of lithium are calculated based on the calibrated quantum defect function. Energy levels and quantum defects for ls^2np^2P...Abstract In this work, ionization potentials and quantum effects of ls^2 np^2 P Rydberg states of lithium are calculated based on the calibrated quantum defect function. Energy levels and quantum defects for ls^2np^2P bound states and their adjacent continuum states are calculated with the R-matrix theory, and then the quantum defect function of the ls^2np （n ≥ 7） channel is obtained, which varies smoothly with the energy based on the quantum defect theory. The accurate quantum defect of the ls^2 7p^2P state derived from the experimental data is used to calibrate the original quantum defect function. The new function is used to calculate ionization potentials and quantum effects of ls^2np ^2P （n ≥ 7） Rydberg states. Present calculations are in agreement with recent experimental data in whole.展开更多
The properties of Pbn（n=2―30） clusters including binding energies,second differences in energy,and HOMO-LUMO gaps,especially fragmentation energies and ionization potentials,have been studied by ab initio calculati...The properties of Pbn（n=2―30） clusters including binding energies,second differences in energy,and HOMO-LUMO gaps,especially fragmentation energies and ionization potentials,have been studied by ab initio calculation.The main fragmentation products of Pbn＋ are shown to be Pb＋Pbn-1＋ for n≤14 and two small cluster fragments for larger ones with n14.The Pb13＋ appears frequently as the products in the fragmentations of large clusters.Also,the calculated ionization potentials of the clusters are consistent with the experiment data.展开更多
The multi-configuration Dirac-Fock method is used in this work to calculate ground-state ionization potentials of Boron and Carbon isoelectronic sequences from Z = 6 to Z=42. And the contribution of relativistic corre...The multi-configuration Dirac-Fock method is used in this work to calculate ground-state ionization potentials of Boron and Carbon isoelectronic sequences from Z = 6 to Z=42. And the contribution of relativistic corrections, nuclear volume effect, Breit and QED effects to tile results is discussed in the calculation. The results are compared with the scanty existing theoretical and experimental data in the literature and good agreements are achieved. Then analytical expressions of lonization potential along Boron and Carbon isoelectronic sequences are obtained.展开更多
Ionization potentials and electron affinities of Cux (n = 2-7) atomic clusters with the optimal geom etries have been calculated by use of SC F-Xa-SW method and Slater's transition state theory. Theo retical calc...Ionization potentials and electron affinities of Cux (n = 2-7) atomic clusters with the optimal geom etries have been calculated by use of SC F-Xa-SW method and Slater's transition state theory. Theo retical calcuIations show that the ionization potentiaIs and electron affinities of Cu. (n = 2-7) atom ic clusters have a sharp even / odd alternation with increasing their sizes, which are related to the electronic structure of Cun atomic clusters. The theoretical results are consistent with the related ex perimental ones.展开更多
By means of the energy level formula E(p)=α+2βcos(pπ/(n+t+1)). the pseudo π ionization potentials of H-(CH_2)_n-X (X=H, F, Cl, Br, I, OH, and SH) are identified by optimizing linear regression analysis, from which...By means of the energy level formula E(p)=α+2βcos(pπ/(n+t+1)). the pseudo π ionization potentials of H-(CH_2)_n-X (X=H, F, Cl, Br, I, OH, and SH) are identified by optimizing linear regression analysis, from which α=13.54±0.50eV and β=1.75±0.13eV are obtained.展开更多
The electronic structure of Ag_n and Au_n(n=2,3,4) calculated by DV—X_α method, are different each other, and the ionization potentials of Ag_n and Au_n as a function of cluster size n exhibit an interesting 'sa...The electronic structure of Ag_n and Au_n(n=2,3,4) calculated by DV—X_α method, are different each other, and the ionization potentials of Ag_n and Au_n as a function of cluster size n exhibit an interesting 'saw—tooth' behavior. The interactions between atom Ag—Ag and Au —Au in Ag_2, Au_2 for different bond length are analyzed. The DOS of the orbitals shows those interactions directly.展开更多
Al2-Al40 clusters were studied by means of the all-electron DFT method. The properties of the aluminum clusters including binding energy, the second difference in energy, HOMO-LUMO gap, especially fragmentation energi...Al2-Al40 clusters were studied by means of the all-electron DFT method. The properties of the aluminum clusters including binding energy, the second difference in energy, HOMO-LUMO gap, especially fragmentation energies and ionization potentials, were analyzed. The main products from the dissociations of aluminum cluster ions are shown to be Al ＋ Al^＋n-1 for the larger clusters, and Al^＋ ＋Aln-1 for the smaller ones. And, the calculated ionization potentials are consistent with the experiment data.展开更多
The relations of oxygen content, critical temperature TC and mean ionization potential < U0> of superconducting oxides are reported. We found that in oxides oxygen is the major element which governs their < U...The relations of oxygen content, critical temperature TC and mean ionization potential < U0> of superconducting oxides are reported. We found that in oxides oxygen is the major element which governs their < U0> te values and thus oxygen content plays an jmportant role in their superconducting properties. As for Y(123)- and T1-systems oxygenation may improve their TC values, but for Biand Hg-systems oxygenation process is not so important. In Y(123), as the oxygen content increase results in the increase of TC upon < U0>to, while the substitution of Ba2+ by Sr2+ causes the decrease of TC upon < U0 >. These results may provide some clues about the superconductivity of oxides and support further that < Uo > is really a good criterion for oxide superconductivity. Two kinds of possible superconducting oxides are predicted in this paper according to the mean ionization potential criterion.展开更多
The authors found the effect of magnetic field on the ionization of atoms and ions and shown that the magnetic field affected the rate of ionization and electron emission at angle of 60°, 120°, 240° and...The authors found the effect of magnetic field on the ionization of atoms and ions and shown that the magnetic field affected the rate of ionization and electron emission at angle of 60°, 120°, 240° and 300°. It is shown that the calculation must take into account the ionization potential of the magnetic field.展开更多
Extreme ultraviolet(EUV)lithography systems operate under limited light intensity.To address this issue and improve lithographic sensitivity,considerable attention has been paid to the addition of atoms(such as F,I,an...Extreme ultraviolet(EUV)lithography systems operate under limited light intensity.To address this issue and improve lithographic sensitivity,considerable attention has been paid to the addition of atoms(such as F,I,and metal atoms)with high EUV absorption to photoresists.However,the subsequent reaction intensification involved in lithography is always ignored.Herein,the considerable influence of different ligands in photoresists on lithographic sensitivity is reported.The regulated molecular orbitals of metal-oxo clusters can increase lithographic sensitivity besides introducing high EUV-absorbing elements.It is illustrated firstly that aromatic groups with electron-donating groups as ligands provide low vertical ionization potential(VIP)and high occupied molecular orbital to metal-oxo(Zn_(2)Ti_(4)O_(4))cluster photoresists,drastically increasing photoelectron yields during exposure and ultimately enhancing lithographic sensitivity.The synergistic effect of reduced VIP and double bond crosslinking can considerably reduce the EUV dose required for lithography.Leveraging this synergistic effect,35 nm(L/S)half-pitch patterns are achieved with only 25 mJ/cm^(2)EUVexposure dose.Thus,the proposed mechanism might prove important for ligand screening for metal-oxo cluster photoresists for advanced lithography.展开更多
In chemical science,the vertical ionization potential(VIP)is a crucial metric for understanding the electronegativity,hardness and softness of chemical material systems as well as the electronic structure and stabilit...In chemical science,the vertical ionization potential(VIP)is a crucial metric for understanding the electronegativity,hardness and softness of chemical material systems as well as the electronic structure and stability of molecules.Ever since the last century,the model chemistry composite methods have witnessed tremendous developments in computing the thermodynamic properties as well as the barrier heights.However,their performance in realm of the vertical electron processes of molecular systems has been rarely explored.In this study,we for the first time benchmarked the model chemistry composite methods(e.g.,CBS-QB3,G4 and W1BD)in comparison with the commonly used Koopmans's theorem(KT),electron propagator theory(e.g.,OVGF,D2,P3 and P3+)and CCSD(T)methods in calculating the VIP for up to 613 molecular systems with available experimental measurements.The large-scale test calculations strongly showed that the CBS-QB3 model chemistry composite technique can be well recommended to calculate VIP from the perspectives of accuracy,economy and applicability.Notably,the VIP values of up to 7 molecules were identified to have the absolute errors of larger than 0.3 e V at all calculation levels,which have strong hints that their VIP experimental values should be re-investigated.展开更多
Extreme ultraviolet(EUV)photoresists have become the core materials in lithography with nanometer-sized patterns and are actively explored on the path to realizing smaller critical dimensions.These photoresists can be...Extreme ultraviolet(EUV)photoresists have become the core materials in lithography with nanometer-sized patterns and are actively explored on the path to realizing smaller critical dimensions.These photoresists can be small molecule-,polymer-,or organic–inorganic hybrid-based,with the full molecular working mechanism under investigation.For the rational design of EUV photoresists,theoretical guidance using tools like first-principle calculations and multi-scale simulations can be of great help.Considering the extremely high standard of accuracy in EUV lithography,it is critical to ensure the adoption of the appropriate methodologies in the theoretical evaluation of EUV photoresists.However,it is known that density func-tionals and semi-empirical methods differ in accuracy and efficiency,without a universal rule across materials.This poses a challenge in developing a reliable theoretical framework for calculating EUV photoresists.Here,we present a benchmark investigation of density functionals and semi-empirical methods on the three main types of EUV photoresists,focusing on the ionization potential,a key parameter in their microscopic molecular reactions.The vertical detachment energies(VDE)and adiabatic detachment energies(ADE)were calculated using 12 functionals,including pure functionals,hybrid functionals,Minnesota functionals,and the recently developed optimally tuned range-separated(OTRS)functionals.Several efficient semi-empirical methods were also chosen,including AM1,PM6,PM7,and GFN1-xTB in the extended tight-binding theo-retical framework.These results guide the accurate and efficient calculation of EUV photoresists and are valuable for the development of multi-scale lithography protocols.展开更多
We theoretically investigate the low energy part of the photoelectron spectra in the tunneling ionization regime by numerically solving the time-dependent Schrdinger equation for different atomic potentials at various...We theoretically investigate the low energy part of the photoelectron spectra in the tunneling ionization regime by numerically solving the time-dependent Schrdinger equation for different atomic potentials at various wavelengths.We find that the shift of the first above-threshold ionization（ATI） peak is closely related to the interferences between electron wave packets,which are controlled by the laser field and largely independent of the potential.By gradually changing the short-range potential to the long-range Coulomb potential,we show that the long-range potential＇s effect is mainly to focus the electrons along the laser＇s polarization and to generate the spider structure by enhancing the rescattering process with the parent ion.In addition,we find that the intermediate transitions and the Rydberg states have important influences on the number and the shape of the lobes near the threshold.展开更多
Phenolic compounds are a class of hazardous substances for human.To study the antiradical potential of a series of phenolic compounds from the aspect of position and substituent type,phenol,o⁃dihydroxybenzene(ODB),m⁃d...Phenolic compounds are a class of hazardous substances for human.To study the antiradical potential of a series of phenolic compounds from the aspect of position and substituent type,phenol,o⁃dihydroxybenzene(ODB),m⁃dihydroxybenzene(MDB),p⁃dihydroxybenzene(PDB),paranitrophenol(PNP),and o⁃chlorophenol(OCP)were selected as typical targets.In addition,to elucidate the degradation discrepancy of phenolic compounds,quantum chemical calculations(QCCs)were obtained using the B3LYP method along with a 6-311G(d,p)basis set.Calculations indicate that phenol,ODB,MDB,and PDB,with electron⁃donating groups,exhibited high antiradical potential,while PNP and OCP,with electron⁃withdrawing groups,exhibited low antiradical potential.The chemical indices calculations show that para⁃compounds and ortho⁃compounds had high antiradical ability.Moreover,phenol,ODB,MDB,and PDB possessed higher bond dissociation enthalpy(BDE)and lower adiabatic ionization potential(AIP)values compared with those of OCP and PNP.Medium effects,even in vacuo,were also taken into account to reveal the antiradical ability of phenolic compounds.展开更多
The ionization spectrum of sulfur dioxide has been successfully studied by using the symmetry-adapted-cluster configuration-interaction （SAC-CI） general-R and SD-R methods and the basis set correlation-consistent po...The ionization spectrum of sulfur dioxide has been successfully studied by using the symmetry-adapted-cluster configuration-interaction （SAC-CI） general-R and SD-R methods and the basis set correlation-consistent polarized valence triple-zeta （cc-pVTZ）. The SAC-CI general-R method reproduces the experimental spectrum well for both the main peaks and the satellite peaks of ionization spectrum of SO2. The sequence of ionic states corresponding to main peaks of SO2 has been re-determined according to the SAC-CI conclusions and it is reordered as X^2A1, A^2B2, B2A2, C^2B1,D^2A1, E^2B2 and F^2A1. Besides, the equilibrium structures and adiabatic ionization potentials （AIPs） of ionic states of main peaks of SO2 are calculated by using the SAC-CI SD-R method.展开更多
The potential energy surfaces for butanone isomerization have been investigated by density function theory calculation. Six main reaction pathways are confirmed using the intrinsic reaction coordinate method, and the ...The potential energy surfaces for butanone isomerization have been investigated by density function theory calculation. Six main reaction pathways are confirmed using the intrinsic reaction coordinate method, and the corresponding isomerization products are 1-buten-2-ol, 2-buten-2-ol, butanal or 1-buten-l-ol, methyl 1-propenyl ether, methyl allyl ether, and ethyl vinyl ether, respectively. Among them, there are three pathways through butylene oxide, indicating butylene oxide is an important intermediate product during butanone isomer ization. The calculated vertical ionization energies of the reactant and its products are in a good agreement with the experimental values available. From the consideration for the relative energies Of transition states and the number of high-energy barriers we infer that the reaction pathway butanone-＊l-buten-2-ol---2-buten-2-oi is the most competitive. The obtained results are informative for future studies on isomerization of ketone molecules.展开更多
We derive a simple ionization rate formula for the ground state of a hydrogen atom in the velocity gauge under the conditions：ω〈〈1 a.u.（a.u.is short for atomic unit） and γ〈〈1（ω is the laser frequency and y ...We derive a simple ionization rate formula for the ground state of a hydrogen atom in the velocity gauge under the conditions：ω〈〈1 a.u.（a.u.is short for atomic unit） and γ〈〈1（ω is the laser frequency and y is the Keldysh parameter）.Comparisons are made among the different versions of the Keldysh-Faisal-Reiss（KFR） theory.The numerical study shows that with considering the quasi-classical（WKB） Coulomb correction in the final state of the ionized electron,the photoionization rate is enhanced compared with without considering the Coulomb correction,and the Reiss theory with the WKB Coulomb correction gives the correct result in the tunneling regime.Our concise formula of the ionization rate may provide an insight into the ionization mechanism for the ground state of a hydrogen atom.展开更多
Influences of lanthanum stearate （LaSt3） and calcium stearate/zinc stearate （Ca/Zn） stabilizers on stabilization efficiency of dibutyltin dilaurate （DBTDL） to polyvinyl chloride （PVC） in air were investigated....Influences of lanthanum stearate （LaSt3） and calcium stearate/zinc stearate （Ca/Zn） stabilizers on stabilization efficiency of dibutyltin dilaurate （DBTDL） to polyvinyl chloride （PVC） in air were investigated. The results revealed that the stabilization effect of DBTDL could be achieved by the La/Sn stabilizers with a ratio of 8/2. Addition of DBTDL could enhance thermal property and reduce dynamic storage modulus （G＇） at 180℃ for PVC containing LaSt3 or Ca/Zn stabilizers. On the other hand, incorporation of LaSh did not influence the stabilization efficiency of DBTDL markedly; while addition of Ca/Zn stabilizers could significantly decrease thermal property for the DBTDL stabilized PVC. Furthermore, the effects of LaSt3 and Ca/Zn stabilizers on the stabilization efficiency of DBTDL were explained in the framework of ionization potential.展开更多
In this paper various structural possibilities for AlnO neutral and cationic isomers were investigated by using the B3LYP/6-311G（3df） method. Calculations of this paper predicted the existence of a number of previou...In this paper various structural possibilities for AlnO neutral and cationic isomers were investigated by using the B3LYP/6-311G（3df） method. Calculations of this paper predicted the existence of a number of previously unknown isomers. The stabilities of the AlnO （n = 2 - 7） clusters with even n are greater than those with odd n, however the stabilities Of cationic ions have the opposite odd-even alternation. The mass spectra observations of Al17O^＋ and Al19O^＋ ions support our theoretical predictions on their stabilities.展开更多
基金the Natural Science Foundation of Shandong Province (Z2004F01)the State Key Laboratory Foundation of Crystal Materialthe National Natural Science Foundation of China (29673025)
文摘Adiabatic and vertical ionization potentials （IPs） mad valence electron affmities （EAs） of alaninamide in gas phase have been detennined using density functional theory （BLYP, B3LYP, B3P86） methods with 6-311＋＋G（d, p） basis set, respectively. IPs and EAs of alaninamide in solutions have been calculated at the B3LYP/6-311＋＋G（d, p） level. Five possible conformers of alaninamide and their charged states have been optimized employing density functional theory B3LYP method with 6-311＋＋（d, p） basis set, respectively.
基金National Natural Science Foundation of China under Grant No.10404017the Basic Research Foundation of Beijing Institute of Technology
文摘Abstract In this work, ionization potentials and quantum effects of ls^2 np^2 P Rydberg states of lithium are calculated based on the calibrated quantum defect function. Energy levels and quantum defects for ls^2np^2P bound states and their adjacent continuum states are calculated with the R-matrix theory, and then the quantum defect function of the ls^2np （n ≥ 7） channel is obtained, which varies smoothly with the energy based on the quantum defect theory. The accurate quantum defect of the ls^2 7p^2P state derived from the experimental data is used to calibrate the original quantum defect function. The new function is used to calculate ionization potentials and quantum effects of ls^2np ^2P （n ≥ 7） Rydberg states. Present calculations are in agreement with recent experimental data in whole.
基金Supported by the National Natural Science Foundation of China(Nos.20773047 and 21043001)
文摘The properties of Pbn（n=2―30） clusters including binding energies,second differences in energy,and HOMO-LUMO gaps,especially fragmentation energies and ionization potentials,have been studied by ab initio calculation.The main fragmentation products of Pbn＋ are shown to be Pb＋Pbn-1＋ for n≤14 and two small cluster fragments for larger ones with n14.The Pb13＋ appears frequently as the products in the fragmentations of large clusters.Also,the calculated ionization potentials of the clusters are consistent with the experiment data.
基金Supported by the Science Fund for Young Scholars of Southwest University under Grant No.SWU208035 Fundamental Research Funds of Central University under Grant No.XDJK2009C020
文摘The multi-configuration Dirac-Fock method is used in this work to calculate ground-state ionization potentials of Boron and Carbon isoelectronic sequences from Z = 6 to Z=42. And the contribution of relativistic corrections, nuclear volume effect, Breit and QED effects to tile results is discussed in the calculation. The results are compared with the scanty existing theoretical and experimental data in the literature and good agreements are achieved. Then analytical expressions of lonization potential along Boron and Carbon isoelectronic sequences are obtained.
文摘Ionization potentials and electron affinities of Cux (n = 2-7) atomic clusters with the optimal geom etries have been calculated by use of SC F-Xa-SW method and Slater's transition state theory. Theo retical calcuIations show that the ionization potentiaIs and electron affinities of Cu. (n = 2-7) atom ic clusters have a sharp even / odd alternation with increasing their sizes, which are related to the electronic structure of Cun atomic clusters. The theoretical results are consistent with the related ex perimental ones.
文摘By means of the energy level formula E(p)=α+2βcos(pπ/(n+t+1)). the pseudo π ionization potentials of H-(CH_2)_n-X (X=H, F, Cl, Br, I, OH, and SH) are identified by optimizing linear regression analysis, from which α=13.54±0.50eV and β=1.75±0.13eV are obtained.
基金The project supported by National Nature Science Foundation of China and National Advanced Materials Commlttee of China
文摘The electronic structure of Ag_n and Au_n(n=2,3,4) calculated by DV—X_α method, are different each other, and the ionization potentials of Ag_n and Au_n as a function of cluster size n exhibit an interesting 'saw—tooth' behavior. The interactions between atom Ag—Ag and Au —Au in Ag_2, Au_2 for different bond length are analyzed. The DOS of the orbitals shows those interactions directly.
基金Supported by the National Natural Science Foundation of China(Nos.20773047 and 20473030)
文摘Al2-Al40 clusters were studied by means of the all-electron DFT method. The properties of the aluminum clusters including binding energy, the second difference in energy, HOMO-LUMO gap, especially fragmentation energies and ionization potentials, were analyzed. The main products from the dissociations of aluminum cluster ions are shown to be Al ＋ Al^＋n-1 for the larger clusters, and Al^＋ ＋Aln-1 for the smaller ones. And, the calculated ionization potentials are consistent with the experiment data.
文摘The relations of oxygen content, critical temperature TC and mean ionization potential < U0> of superconducting oxides are reported. We found that in oxides oxygen is the major element which governs their < U0> te values and thus oxygen content plays an jmportant role in their superconducting properties. As for Y(123)- and T1-systems oxygenation may improve their TC values, but for Biand Hg-systems oxygenation process is not so important. In Y(123), as the oxygen content increase results in the increase of TC upon < U0>to, while the substitution of Ba2+ by Sr2+ causes the decrease of TC upon < U0 >. These results may provide some clues about the superconductivity of oxides and support further that < Uo > is really a good criterion for oxide superconductivity. Two kinds of possible superconducting oxides are predicted in this paper according to the mean ionization potential criterion.
文摘The authors found the effect of magnetic field on the ionization of atoms and ions and shown that the magnetic field affected the rate of ionization and electron emission at angle of 60°, 120°, 240° and 300°. It is shown that the calculation must take into account the ionization potential of the magnetic field.
基金supported by the National Natural Science Foundation of China(22090011,22378052)the Fundamental Research Funds for the Central Universities(DUT22LAB608)。
文摘Extreme ultraviolet(EUV)lithography systems operate under limited light intensity.To address this issue and improve lithographic sensitivity,considerable attention has been paid to the addition of atoms(such as F,I,and metal atoms)with high EUV absorption to photoresists.However,the subsequent reaction intensification involved in lithography is always ignored.Herein,the considerable influence of different ligands in photoresists on lithographic sensitivity is reported.The regulated molecular orbitals of metal-oxo clusters can increase lithographic sensitivity besides introducing high EUV-absorbing elements.It is illustrated firstly that aromatic groups with electron-donating groups as ligands provide low vertical ionization potential(VIP)and high occupied molecular orbital to metal-oxo(Zn_(2)Ti_(4)O_(4))cluster photoresists,drastically increasing photoelectron yields during exposure and ultimately enhancing lithographic sensitivity.The synergistic effect of reduced VIP and double bond crosslinking can considerably reduce the EUV dose required for lithography.Leveraging this synergistic effect,35 nm(L/S)half-pitch patterns are achieved with only 25 mJ/cm^(2)EUVexposure dose.Thus,the proposed mechanism might prove important for ligand screening for metal-oxo cluster photoresists for advanced lithography.
基金funded by the National Natural Science Foundation of China(Nos.22073069,21773082)Science Research Project of Hebei Education Department(No.QN2024255)。
文摘In chemical science,the vertical ionization potential(VIP)is a crucial metric for understanding the electronegativity,hardness and softness of chemical material systems as well as the electronic structure and stability of molecules.Ever since the last century,the model chemistry composite methods have witnessed tremendous developments in computing the thermodynamic properties as well as the barrier heights.However,their performance in realm of the vertical electron processes of molecular systems has been rarely explored.In this study,we for the first time benchmarked the model chemistry composite methods(e.g.,CBS-QB3,G4 and W1BD)in comparison with the commonly used Koopmans's theorem(KT),electron propagator theory(e.g.,OVGF,D2,P3 and P3+)and CCSD(T)methods in calculating the VIP for up to 613 molecular systems with available experimental measurements.The large-scale test calculations strongly showed that the CBS-QB3 model chemistry composite technique can be well recommended to calculate VIP from the perspectives of accuracy,economy and applicability.Notably,the VIP values of up to 7 molecules were identified to have the absolute errors of larger than 0.3 e V at all calculation levels,which have strong hints that their VIP experimental values should be re-investigated.
基金supported by the National Natural Science Foundation of China(grant number 22090013)the Shanghai Committee of Science and Technology(grant numbers:21QA1402900 and YDZX20213100002672).
文摘Extreme ultraviolet(EUV)photoresists have become the core materials in lithography with nanometer-sized patterns and are actively explored on the path to realizing smaller critical dimensions.These photoresists can be small molecule-,polymer-,or organic–inorganic hybrid-based,with the full molecular working mechanism under investigation.For the rational design of EUV photoresists,theoretical guidance using tools like first-principle calculations and multi-scale simulations can be of great help.Considering the extremely high standard of accuracy in EUV lithography,it is critical to ensure the adoption of the appropriate methodologies in the theoretical evaluation of EUV photoresists.However,it is known that density func-tionals and semi-empirical methods differ in accuracy and efficiency,without a universal rule across materials.This poses a challenge in developing a reliable theoretical framework for calculating EUV photoresists.Here,we present a benchmark investigation of density functionals and semi-empirical methods on the three main types of EUV photoresists,focusing on the ionization potential,a key parameter in their microscopic molecular reactions.The vertical detachment energies(VDE)and adiabatic detachment energies(ADE)were calculated using 12 functionals,including pure functionals,hybrid functionals,Minnesota functionals,and the recently developed optimally tuned range-separated(OTRS)functionals.Several efficient semi-empirical methods were also chosen,including AM1,PM6,PM7,and GFN1-xTB in the extended tight-binding theo-retical framework.These results guide the accurate and efficient calculation of EUV photoresists and are valuable for the development of multi-scale lithography protocols.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11322437 and 11574010)the National Basic Research ProgramChina(Grant No.2013CB922402)
文摘We theoretically investigate the low energy part of the photoelectron spectra in the tunneling ionization regime by numerically solving the time-dependent Schrdinger equation for different atomic potentials at various wavelengths.We find that the shift of the first above-threshold ionization（ATI） peak is closely related to the interferences between electron wave packets,which are controlled by the laser field and largely independent of the potential.By gradually changing the short-range potential to the long-range Coulomb potential,we show that the long-range potential＇s effect is mainly to focus the electrons along the laser＇s polarization and to generate the spider structure by enhancing the rescattering process with the parent ion.In addition,we find that the intermediate transitions and the Rydberg states have important influences on the number and the shape of the lobes near the threshold.
基金Sponsored by the Open Project of State Key Laboratory of Urban Water Resource and Environment,Harbin Institute of Technology(Grant No.HCK201804).
文摘Phenolic compounds are a class of hazardous substances for human.To study the antiradical potential of a series of phenolic compounds from the aspect of position and substituent type,phenol,o⁃dihydroxybenzene(ODB),m⁃dihydroxybenzene(MDB),p⁃dihydroxybenzene(PDB),paranitrophenol(PNP),and o⁃chlorophenol(OCP)were selected as typical targets.In addition,to elucidate the degradation discrepancy of phenolic compounds,quantum chemical calculations(QCCs)were obtained using the B3LYP method along with a 6-311G(d,p)basis set.Calculations indicate that phenol,ODB,MDB,and PDB,with electron⁃donating groups,exhibited high antiradical potential,while PNP and OCP,with electron⁃withdrawing groups,exhibited low antiradical potential.The chemical indices calculations show that para⁃compounds and ortho⁃compounds had high antiradical ability.Moreover,phenol,ODB,MDB,and PDB possessed higher bond dissociation enthalpy(BDE)and lower adiabatic ionization potential(AIP)values compared with those of OCP and PNP.Medium effects,even in vacuo,were also taken into account to reveal the antiradical ability of phenolic compounds.
基金Project supported by the National Natural Science Foundation of China (Grant No 10404030)
文摘The ionization spectrum of sulfur dioxide has been successfully studied by using the symmetry-adapted-cluster configuration-interaction （SAC-CI） general-R and SD-R methods and the basis set correlation-consistent polarized valence triple-zeta （cc-pVTZ）. The SAC-CI general-R method reproduces the experimental spectrum well for both the main peaks and the satellite peaks of ionization spectrum of SO2. The sequence of ionic states corresponding to main peaks of SO2 has been re-determined according to the SAC-CI conclusions and it is reordered as X^2A1, A^2B2, B2A2, C^2B1,D^2A1, E^2B2 and F^2A1. Besides, the equilibrium structures and adiabatic ionization potentials （AIPs） of ionic states of main peaks of SO2 are calculated by using the SAC-CI SD-R method.
文摘The potential energy surfaces for butanone isomerization have been investigated by density function theory calculation. Six main reaction pathways are confirmed using the intrinsic reaction coordinate method, and the corresponding isomerization products are 1-buten-2-ol, 2-buten-2-ol, butanal or 1-buten-l-ol, methyl 1-propenyl ether, methyl allyl ether, and ethyl vinyl ether, respectively. Among them, there are three pathways through butylene oxide, indicating butylene oxide is an important intermediate product during butanone isomer ization. The calculated vertical ionization energies of the reactant and its products are in a good agreement with the experimental values available. From the consideration for the relative energies Of transition states and the number of high-energy barriers we infer that the reaction pathway butanone-＊l-buten-2-ol---2-buten-2-oi is the most competitive. The obtained results are informative for future studies on isomerization of ketone molecules.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11274149 and 11304185)the Program of Shenyang Key Laboratory of Optoelectronic Materials and Technology,China(Grant No.F12-254-1-00)
文摘We derive a simple ionization rate formula for the ground state of a hydrogen atom in the velocity gauge under the conditions：ω〈〈1 a.u.（a.u.is short for atomic unit） and γ〈〈1（ω is the laser frequency and y is the Keldysh parameter）.Comparisons are made among the different versions of the Keldysh-Faisal-Reiss（KFR） theory.The numerical study shows that with considering the quasi-classical（WKB） Coulomb correction in the final state of the ionized electron,the photoionization rate is enhanced compared with without considering the Coulomb correction,and the Reiss theory with the WKB Coulomb correction gives the correct result in the tunneling regime.Our concise formula of the ionization rate may provide an insight into the ionization mechanism for the ground state of a hydrogen atom.
基金supported by Key Projects in the National Science & Technology Pillar Program(No. 2007BAE10B04)
文摘Influences of lanthanum stearate （LaSt3） and calcium stearate/zinc stearate （Ca/Zn） stabilizers on stabilization efficiency of dibutyltin dilaurate （DBTDL） to polyvinyl chloride （PVC） in air were investigated. The results revealed that the stabilization effect of DBTDL could be achieved by the La/Sn stabilizers with a ratio of 8/2. Addition of DBTDL could enhance thermal property and reduce dynamic storage modulus （G＇） at 180℃ for PVC containing LaSt3 or Ca/Zn stabilizers. On the other hand, incorporation of LaSh did not influence the stabilization efficiency of DBTDL markedly; while addition of Ca/Zn stabilizers could significantly decrease thermal property for the DBTDL stabilized PVC. Furthermore, the effects of LaSt3 and Ca/Zn stabilizers on the stabilization efficiency of DBTDL were explained in the framework of ionization potential.
基金Project supported by the Postdoctoral Science Foundation of China （Grant No 2004036454）.
文摘In this paper various structural possibilities for AlnO neutral and cationic isomers were investigated by using the B3LYP/6-311G（3df） method. Calculations of this paper predicted the existence of a number of previously unknown isomers. The stabilities of the AlnO （n = 2 - 7） clusters with even n are greater than those with odd n, however the stabilities Of cationic ions have the opposite odd-even alternation. The mass spectra observations of Al17O^＋ and Al19O^＋ ions support our theoretical predictions on their stabilities.
