The octupole deformation and collectivity in octupole double-magic nucleus 144Ba are investigated using the Cranking covariant density functional theory in a three-dimensional lattice space.The reduced B(E3)transition...The octupole deformation and collectivity in octupole double-magic nucleus 144Ba are investigated using the Cranking covariant density functional theory in a three-dimensional lattice space.The reduced B(E3)transition probability is implemented for the first time in semiclassical approximation based on the microscopically calculated electric octupole moments.The available data,including the I-ωrelation and electric transitional probabilities B(E2)and B(E3)are well reproduced.Furthermore,it is shown that the ground state of 144Ba exhibits axial octupole and quadrupole deformations that persist up to high spins(I≈24h).展开更多
The phase transition of gallium phosphide （GAP） from zinc-blende （ZB） to a rocksalt （RS） structure is investigated by the plane-wave pseudopotential density functional theory （DFT）. Lattice constant a0, elasti...The phase transition of gallium phosphide （GAP） from zinc-blende （ZB） to a rocksalt （RS） structure is investigated by the plane-wave pseudopotential density functional theory （DFT）. Lattice constant a0, elastic constants cij, bulk modulus B0 and the pressure derivative of bulk modulus B0 are calculated. The results are in good agreement with numerous experimental and theoretical data. From the usual condition of equal enthalpies, the phase transition from the ZB to the RS structure occurs at 21.9 GPa, which is close to the experimental value of 22.0 GPa. The elastic properties of GaP with the ZB structure in a pressure range from 0 GPa to 21.9 GPa and those of the RS structure in a pressure range of pressures from 21.9 GPa to 40 GPa are obtained. According to the quasi-harmonic Debye model, in which the phononic effects are considered, the normalized volume V/Vo, the Debye temperature 8, the heat capacity Cv and the thermal expansion coefficient a are also discussed in a pressure range from 0 CPa to 40 GPa and a temperature range from 0 K to 1500 K.展开更多
The concepts of Markov process in random environment and homogeneous random transition functions are introduced. The necessary and sufficient conditions for homogeneous random transition function are given. The main r...The concepts of Markov process in random environment and homogeneous random transition functions are introduced. The necessary and sufficient conditions for homogeneous random transition function are given. The main results in this article are the analytical properties, such as continuity, differentiability, random Kolmogorov backward equation and random Kolmogorov forward equation of homogeneous random transition functions.展开更多
Time-dependent density functional theory(TDDFT)method is used to investigate the details of the excited state intramolecular proton transfer(ESIPT)process and the mechanism for temperature effect on the Enol^(*)/Keto^...Time-dependent density functional theory(TDDFT)method is used to investigate the details of the excited state intramolecular proton transfer(ESIPT)process and the mechanism for temperature effect on the Enol^(*)/Keto^(*)emission ratio for the Me_(2)N-substited flavonoid(MNF)compound.The geometric structures of the S_(0) and S_(1) states are denoted as the Enol,Enol^(*),and Keto*.In addition,the absorption and fluorescence peaks are also calculated.It is noted that the calculated large Stokes shift is in good agreement with the experimental result.Furthermore,our results confirm that the ESIPT process happens upon photoexcitation,which is distinctly monitored by the formation and disappearance of the characteristic peaks of infrared(IR)spectra involved in the proton transfer and in the potential energy curves.Besides,the calculations of highest occupied molecular orbital(HOMO)and lowest unoccupied molecular orbital(LUMO)reveal that the electronegativity change of proton acceptor due to the intramolecular charge redistribution in the S_(1) state induces the ESIPT.Moreover,the thermodynamic calculation for the MNF shows that the Enol^(*)/Keto^(*)emission ratio decreasing with temperature increasing arises from the barrier lowering of ESIPT.展开更多
We report on a temperature-dependent resonance Raman spectral characterization of the polyene chain of canthax- anthin. It is observed that all vibrational intensities of the polyene chain are inversely proportional t...We report on a temperature-dependent resonance Raman spectral characterization of the polyene chain of canthax- anthin. It is observed that all vibrational intensities of the polyene chain are inversely proportional to temperature, which is analyzed by the resonance Raman effect and the coherent weakly damped electron/lattice vibrations. The increase in intensity of the CC overtone/combination relative to the fundamental with temperature decreasing is detected and discussed in terms of electron/phonon coupling and the activation energy Uop. Moreover, the polyene chain studies using the density functional theory B3LYP/6-31 G＊ level reveal a prominent peak at 1525 cm-1 consisting of two closely spaced modes that are both dominated by C=C stretching coordinates of the polyene chain.展开更多
The excess Helmholtz free energy functional for nonpolar chain-like molecules is formulated in terms of a weighted density approximation （WDA） for short-range interactions and a Weaks Chandler Andersen （WCA） appro...The excess Helmholtz free energy functional for nonpolar chain-like molecules is formulated in terms of a weighted density approximation （WDA） for short-range interactions and a Weaks Chandler Andersen （WCA） approximation and a Barker Henderson （BH） theory for long-range attraction. Within the framework of density functional theory （DFT）, vapour liquid interracial properties including density profile and surface tension, and vapour-liquid nucleation properties including density profile, work of formation and number of particles are investigated for spherical and chain- like molecules. The obtained vapour liquid surface tension and the number of particles in critical nucleus for Lennard- Jones （L J） fluids are consistent with the simulation results. The influences of supersaturation, temperature and chain length on vapour liquid nucleation properties are discussed.展开更多
This paper uses the generalised gradient approximation based on density functional theory to analyse the geometric structure and properties of the 3d transition metal atom doped endohedral fullerene M@C20F20 （M = Sc...This paper uses the generalised gradient approximation based on density functional theory to analyse the geometric structure and properties of the 3d transition metal atom doped endohedral fullerene M@C20F20 （M = Sc-Ni）. The geometric optimization shows that the cage centre is the most stable position for M, forming the structure named as M@C20F20-4. The inclusion energy, zero-point energy, and energy gap calculations tell us that Ni@C20F20-4 should be thermodynamically and kinetically stablest. M@C20F20-4 （M = Sc-Co） possesses high magnetic moments varied from 1 to 6 μB, while Ni@C20F20-4 is nonmagnetic. The Ni-C bond in Ni@C20F20-4 contains both the covalent and ionic characters.展开更多
A density functional theory （DFT） is used to investigate molecular orientation of hard rod fluids in a hard slit. The DFT approach combines a modified fundamental measure theory （MFMT） for excluded-volume effect w...A density functional theory （DFT） is used to investigate molecular orientation of hard rod fluids in a hard slit. The DFT approach combines a modified fundamental measure theory （MFMT） for excluded-volume effect with the first order thermodynamics perturbation theory for chain connectivity. In the DFT approach, the intra-molecular bonding orientation function is introduced. We consider the effects of molecular length （i.e. aspect ratio of rod） and packing fraction on the orientations of hard rod fluids and flexible chains. For the flexible chains, the chain length has no significant effect while the packing fraction shows slight effect on the molecular orientation distribution. In contrast, for the hard rod fluids, the chain length determines the molecular orientation distribution, while the packing fraction has no significant effect on the molecular orientation distribution. By making a comparison between molecular orientations of the flexible chain and the hard rod fluid, we find that the molecular stiffness distinctly affects the molecular orientation. In addition, partitioning coefficient indicates that the longer rodlike molecule is more difficult to enter the confined phase, especially at low bulk packing fractions.展开更多
The geometric structures, electronic and magnetic properties of the 3d transition metal doped clusters Pd12M （M = Sc-Ni） are studied using the semi^core pseudopots density functional theory. The groundstate geometri...The geometric structures, electronic and magnetic properties of the 3d transition metal doped clusters Pd12M （M = Sc-Ni） are studied using the semi^core pseudopots density functional theory. The groundstate geometric structure of the Pd12M cluster is probably of pseudoicosahedron. The Ih-Pd12M cluster has the most thermodynamic stability in five different symmetric isomers. The energy gap shows that Pd12M cluster is partly metallic. Both the absolutely predominant metal bond and very weak covalent bond might exist in the Pdl2M cluster. The magnetic mo- ment of Pd12M varies from 0 to 5 μB, implying that it has a potential application in new nanomaterials with tunable magnetic properties.展开更多
In this paper the first-principles calculations within local spin density approximation （LSDA）＋U show that BiFeO3 experiences a mixed phase state with P4mm structure being the intermediate phase before the pressure...In this paper the first-principles calculations within local spin density approximation （LSDA）＋U show that BiFeO3 experiences a mixed phase state with P4mm structure being the intermediate phase before the pressure of phase transition is reached. The critical pressure for the insulator-metal transition （IMT） is found to be about 50 GPa. A pressure induced crossover of high-spin states and low-spin states is observed close to the IMT pressure in R3c structure. The LSDA＋U calculations account well for the mechanism of the IMT and crossover of spin states predicted in recent experiment （Ref.[1]）.展开更多
There are three parts in this article. In Section 1, we establish the model of branching chain with drift in space-time random environment （BCDSTRE）, i.e., the coupling of branching chain and random walk. In Section...There are three parts in this article. In Section 1, we establish the model of branching chain with drift in space-time random environment （BCDSTRE）, i.e., the coupling of branching chain and random walk. In Section 2, we prove that any BCDSTRE must be a Markov chain in time random environment when we consider the distribution of the particles in space as a random element. In Section 3, we calculate the first-order moments and the second-order moments of BCDSTRE.展开更多
With first-principles virtual-crystal approximation calculations, we systematically investigate the geometric and elec- tronic structures as well as the phase transition of lead zirconate titanate （PbZr 1-xTixO3 or ...With first-principles virtual-crystal approximation calculations, we systematically investigate the geometric and elec- tronic structures as well as the phase transition of lead zirconate titanate （PbZr 1-xTixO3 or PZT） as a function of Ti content for the whole range of 0 〈 XTi 〈 1. It can be found that, with the increase of the Ti content, the PbZr1-xTixO3 solid solutions undergo a rhombohedral-to-tetragonal phase transition, which is consistent with the experimental results. In addition, we also show the evolution in geometric and electronic structures of rhombohedral and tetragonal PbZr1-xTixO3 with the increasing content of Ti.展开更多
基金supported by the National Natural Science Foundation of China(NSFC)(No.12205097)the Fundamental Research Funds for the Central Universities(No.2024MS071)。
文摘The octupole deformation and collectivity in octupole double-magic nucleus 144Ba are investigated using the Cranking covariant density functional theory in a three-dimensional lattice space.The reduced B(E3)transition probability is implemented for the first time in semiclassical approximation based on the microscopically calculated electric octupole moments.The available data,including the I-ωrelation and electric transitional probabilities B(E2)and B(E3)are well reproduced.Furthermore,it is shown that the ground state of 144Ba exhibits axial octupole and quadrupole deformations that persist up to high spins(I≈24h).
文摘The phase transition of gallium phosphide （GAP） from zinc-blende （ZB） to a rocksalt （RS） structure is investigated by the plane-wave pseudopotential density functional theory （DFT）. Lattice constant a0, elastic constants cij, bulk modulus B0 and the pressure derivative of bulk modulus B0 are calculated. The results are in good agreement with numerous experimental and theoretical data. From the usual condition of equal enthalpies, the phase transition from the ZB to the RS structure occurs at 21.9 GPa, which is close to the experimental value of 22.0 GPa. The elastic properties of GaP with the ZB structure in a pressure range from 0 GPa to 21.9 GPa and those of the RS structure in a pressure range of pressures from 21.9 GPa to 40 GPa are obtained. According to the quasi-harmonic Debye model, in which the phononic effects are considered, the normalized volume V/Vo, the Debye temperature 8, the heat capacity Cv and the thermal expansion coefficient a are also discussed in a pressure range from 0 CPa to 40 GPa and a temperature range from 0 K to 1500 K.
基金Supported by the NNSF of China (10371092)the Foundation of Wuhan University.
文摘The concepts of Markov process in random environment and homogeneous random transition functions are introduced. The necessary and sufficient conditions for homogeneous random transition function are given. The main results in this article are the analytical properties, such as continuity, differentiability, random Kolmogorov backward equation and random Kolmogorov forward equation of homogeneous random transition functions.
基金Project supported by the National Basic Research Program of China(Grant No.2013CB922204)the National Natural Science Foundation of China(Grant Nos.11574115 and 11704146)the Natural Science Foundation of Jilin Province,China(Grant No.20150101063JC)
文摘Time-dependent density functional theory(TDDFT)method is used to investigate the details of the excited state intramolecular proton transfer(ESIPT)process and the mechanism for temperature effect on the Enol^(*)/Keto^(*)emission ratio for the Me_(2)N-substited flavonoid(MNF)compound.The geometric structures of the S_(0) and S_(1) states are denoted as the Enol,Enol^(*),and Keto*.In addition,the absorption and fluorescence peaks are also calculated.It is noted that the calculated large Stokes shift is in good agreement with the experimental result.Furthermore,our results confirm that the ESIPT process happens upon photoexcitation,which is distinctly monitored by the formation and disappearance of the characteristic peaks of infrared(IR)spectra involved in the proton transfer and in the potential energy curves.Besides,the calculations of highest occupied molecular orbital(HOMO)and lowest unoccupied molecular orbital(LUMO)reveal that the electronegativity change of proton acceptor due to the intramolecular charge redistribution in the S_(1) state induces the ESIPT.Moreover,the thermodynamic calculation for the MNF shows that the Enol^(*)/Keto^(*)emission ratio decreasing with temperature increasing arises from the barrier lowering of ESIPT.
基金supported by the National Natural Science Foundation of China(Grant Nos.10974067 and 11104107)the Program of Jilin Province Science and Technology Department,China(Grant Nos.20090534 and 20101508)the China Postdoctoral Science Foundation,China(Grant No.20110491320)
文摘We report on a temperature-dependent resonance Raman spectral characterization of the polyene chain of canthax- anthin. It is observed that all vibrational intensities of the polyene chain are inversely proportional to temperature, which is analyzed by the resonance Raman effect and the coherent weakly damped electron/lattice vibrations. The increase in intensity of the CC overtone/combination relative to the fundamental with temperature decreasing is detected and discussed in terms of electron/phonon coupling and the activation energy Uop. Moreover, the polyene chain studies using the density functional theory B3LYP/6-31 G＊ level reveal a prominent peak at 1525 cm-1 consisting of two closely spaced modes that are both dominated by C=C stretching coordinates of the polyene chain.
基金Project supported by the National Natural Science Foundation of China （Grant Nos 20576030 and 20606009）, the Program for New Century Excellent Talents of China （Grant No 06-0206）, and the Research Fund of Key Laboratory for Nanomaterials, Ministry of Education of China （Grant No 2006-2）.
文摘The excess Helmholtz free energy functional for nonpolar chain-like molecules is formulated in terms of a weighted density approximation （WDA） for short-range interactions and a Weaks Chandler Andersen （WCA） approximation and a Barker Henderson （BH） theory for long-range attraction. Within the framework of density functional theory （DFT）, vapour liquid interracial properties including density profile and surface tension, and vapour-liquid nucleation properties including density profile, work of formation and number of particles are investigated for spherical and chain- like molecules. The obtained vapour liquid surface tension and the number of particles in critical nucleus for Lennard- Jones （L J） fluids are consistent with the simulation results. The influences of supersaturation, temperature and chain length on vapour liquid nucleation properties are discussed.
基金Project supported by the Research Starting Foundation of Hohai University (Grant No. 2084/40801130)the Natural Science Foundation of Hohai University (Grant Nos. 2008431211 and 2008430311)+2 种基金the Excellent Innovation Personal Support Plan of Hohai Universitythe Basic Scientific Research Foundation of National Centralthe Special Foundation of the Natural Natural Science (Grant No. 10947132)
文摘This paper uses the generalised gradient approximation based on density functional theory to analyse the geometric structure and properties of the 3d transition metal atom doped endohedral fullerene M@C20F20 （M = Sc-Ni）. The geometric optimization shows that the cage centre is the most stable position for M, forming the structure named as M@C20F20-4. The inclusion energy, zero-point energy, and energy gap calculations tell us that Ni@C20F20-4 should be thermodynamically and kinetically stablest. M@C20F20-4 （M = Sc-Co） possesses high magnetic moments varied from 1 to 6 μB, while Ni@C20F20-4 is nonmagnetic. The Ni-C bond in Ni@C20F20-4 contains both the covalent and ionic characters.
基金Project supported by the National Natural Science Foundation of China （Grant No 20646001）, the Beijing Novel Program （Grant No 2006B17）, the Program for New Century Excellent Talents in University （NCET）, the ＂Chemical Grid Program＂ and the Excellent Talent Fund of Beijing University of Chemical Technology.
文摘A density functional theory （DFT） is used to investigate molecular orientation of hard rod fluids in a hard slit. The DFT approach combines a modified fundamental measure theory （MFMT） for excluded-volume effect with the first order thermodynamics perturbation theory for chain connectivity. In the DFT approach, the intra-molecular bonding orientation function is introduced. We consider the effects of molecular length （i.e. aspect ratio of rod） and packing fraction on the orientations of hard rod fluids and flexible chains. For the flexible chains, the chain length has no significant effect while the packing fraction shows slight effect on the molecular orientation distribution. In contrast, for the hard rod fluids, the chain length determines the molecular orientation distribution, while the packing fraction has no significant effect on the molecular orientation distribution. By making a comparison between molecular orientations of the flexible chain and the hard rod fluid, we find that the molecular stiffness distinctly affects the molecular orientation. In addition, partitioning coefficient indicates that the longer rodlike molecule is more difficult to enter the confined phase, especially at low bulk packing fractions.
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 11104062,10947132,and 11004047)the Excellent Innovation Personal Support Plan of Hohai University,Chinathe Fundamental Research Funds for the Central Universities of China (Grant No. 2012B12914)
文摘The geometric structures, electronic and magnetic properties of the 3d transition metal doped clusters Pd12M （M = Sc-Ni） are studied using the semi^core pseudopots density functional theory. The groundstate geometric structure of the Pd12M cluster is probably of pseudoicosahedron. The Ih-Pd12M cluster has the most thermodynamic stability in five different symmetric isomers. The energy gap shows that Pd12M cluster is partly metallic. Both the absolutely predominant metal bond and very weak covalent bond might exist in the Pdl2M cluster. The magnetic mo- ment of Pd12M varies from 0 to 5 μB, implying that it has a potential application in new nanomaterials with tunable magnetic properties.
文摘In this paper the first-principles calculations within local spin density approximation （LSDA）＋U show that BiFeO3 experiences a mixed phase state with P4mm structure being the intermediate phase before the pressure of phase transition is reached. The critical pressure for the insulator-metal transition （IMT） is found to be about 50 GPa. A pressure induced crossover of high-spin states and low-spin states is observed close to the IMT pressure in R3c structure. The LSDA＋U calculations account well for the mechanism of the IMT and crossover of spin states predicted in recent experiment （Ref.[1]）.
基金Supported by the NSFC(10371092,11771185,10871200)
文摘There are three parts in this article. In Section 1, we establish the model of branching chain with drift in space-time random environment （BCDSTRE）, i.e., the coupling of branching chain and random walk. In Section 2, we prove that any BCDSTRE must be a Markov chain in time random environment when we consider the distribution of the particles in space as a random element. In Section 3, we calculate the first-order moments and the second-order moments of BCDSTRE.
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 11104203, 11075116, 50972014, 51072024, and 51132002)the Foundation of Introduction of Talent of Tianjin Normal University, China (Grant No. 5RL100)
文摘With first-principles virtual-crystal approximation calculations, we systematically investigate the geometric and elec- tronic structures as well as the phase transition of lead zirconate titanate （PbZr 1-xTixO3 or PZT） as a function of Ti content for the whole range of 0 〈 XTi 〈 1. It can be found that, with the increase of the Ti content, the PbZr1-xTixO3 solid solutions undergo a rhombohedral-to-tetragonal phase transition, which is consistent with the experimental results. In addition, we also show the evolution in geometric and electronic structures of rhombohedral and tetragonal PbZr1-xTixO3 with the increasing content of Ti.
