Stretching vibrational band intensities of XH3 （X=N, Sb） molecules are investigated employing three-dimensional dipole moment surfaces combined with the local mode Hamiltonian model. The dipole moment surfaces of NH...Stretching vibrational band intensities of XH3 （X=N, Sb） molecules are investigated employing three-dimensional dipole moment surfaces combined with the local mode Hamiltonian model. The dipole moment surfaces of NH3 and SbH3 are calculated with the density functional theory and at the correlated MP2 level, respectively. The calculated band intensities are in good agreement with the available experimental data. The contribution to the band intensities from the different terms in the polynomial expansion of the dipole moments of four group V hydrides （NH3, PH3, AsH3 and SbH3） are discussed. It is concluded that the breakdown of the bond dipole approximation must be considered. The intensity “borrowing” effect due to the wave function mixing among the stretching vibrational states is found to be less significant for the molecules that reach the local mode limit.展开更多
The reasonable dissociation limit of the A^1∑＋ state ^7LiH molecule is obtained. The accurate dissociation energy and the equilibrium geometry of this state are calculated using a symmetry-adapted-cluster configurat...The reasonable dissociation limit of the A^1∑＋ state ^7LiH molecule is obtained. The accurate dissociation energy and the equilibrium geometry of this state are calculated using a symmetry-adapted-cluster configuration-interaction method in complete active space for the first time, The whole potential energy curve and the dipole moment function for the A^1∑＋ state are calculated over a wide internuclear separation range from about 0.1 to 1.4 nm. The calculated equilibrium geometry and dissociation energy of this potential energy curve are of Re=0.2487 nm and De=1.064eV, respectively. The unusual negative values of the anharmonicity constant and the vibration-rotational coupling constant are of ωeXe=-4.7158cm^-1 and αe=0.08649cm^-1, respectively. The vertical excitation energy from the ground to the A^1∑＋ state is calculated and the value is of 3.613eV at 0.15875nm （the equilibrium position of the ground state）. The highly anomalous shape of this potential energy curve, which is exceptionally flat over a wide radial range around the equilibrium position, is discussed in detail. The harmonic frequency value of 502.47cm^-1 about this state is approximately estimated. Careful comparison of the theoretical determinations with those obtained by previous theories about the A^1∑＋ state dissociation energy clearly shows that the present calculations are much closer to the experiments than previous theories, thus represents an improvement.展开更多
We report a sensitive detection of high Rydberg atom with large dipole moment utilizing its deflection near a pair of parallel cylindrical copper rods which are oppositely charged. When the low-field seeking state Ryd...We report a sensitive detection of high Rydberg atom with large dipole moment utilizing its deflection near a pair of parallel cylindrical copper rods which are oppositely charged. When the low-field seeking state Rydberg atoms fly across the gradient electric field formed by the pair of rods, they will be pushed away from the rods while the high-field seeking state ones will be attracted towards the rods. These atoms will form different patterns on an ion imaging system placed downwards at the end of the rods. The spatial distribution of the deflected atoms on the imaging system is also simulated, in good agreement with the experimental results, from which we can deduce the quantum state information of the excited atoms. This state resolvable Rydberg atom detection can be used for the dynamics research of the dipole-dipole interaction between atoms with large dipole moments.展开更多
The quantum phase effects for induced electric and magnetic dipole moments are investigated. It is shown that the phase shift received by the induced electric dipole has the same form as the one induced by magnetic di...The quantum phase effects for induced electric and magnetic dipole moments are investigated. It is shown that the phase shift received by the induced electric dipole has the same form as the one induced by magnetic dipole moment, therefore the total phase is a hybrid of these two types of phase. This feature indicates that to have a decisive measurement on either one of these two phases, it is necessary to measure the velocity dependence of the observed phase.展开更多
Recently, the diverse properties of Rydberg atoms, which probably arise from its large electric dipole moment （EDM）, have been explored. In this paper, we report electric dipole moments along with Stark energies and...Recently, the diverse properties of Rydberg atoms, which probably arise from its large electric dipole moment （EDM）, have been explored. In this paper, we report electric dipole moments along with Stark energies and charge densities of lithium Rydberg states in the presence of electric fields, calculated by matrix diagonalization. Huge electric dipole moments are discovered. In order to check the validity of the EDMs, we also use these electric dipole moments to calculate the Stark energies by numerical integration. The results agree with those calculated by matrix diagonalization.展开更多
An ab initio calculations on the ground and low-lying excited statesX2∑＋,2^2∑＋,3^2∑＋,1^4∏,2^4∏,1^4∑＋,2^4∑＋,and 3^4∑＋of KBe molecule have been performed using multireference configuration interaction （M...An ab initio calculations on the ground and low-lying excited statesX2∑＋,2^2∑＋,3^2∑＋,1^4∏,2^4∏,1^4∑＋,2^4∑＋,and 3^4∑＋of KBe molecule have been performed using multireference configuration interaction （MRCI） plus Davidsoncorrections （MRCI＋Q） approach with all electron basis set aug-cc-pCV5Z-DK for Be and def2-AQZVPP-JKFI for K.3^2∑＋,1^4∏,2^4∏,1^4∑＋,2^4∑＋and3^4∑＋states are investigated for the first time. Inner shell electron correlations are computed on the potential energy curves （PECs） calculations. The spectroscopic and molecular parameters are also predicted. In addition, The transition properties including transition dipole moment, Franck-Condon factors qv′v″, Einstein coefficients Av′v″, and the radiative lifetimesτ′for the2^2∑＋-X2∑＋,3^2∑＋-X2∑＋,and 2^4∏-1^4∏ transitions are predictedat the same time.展开更多
An accurate electric dipole moment function(EDMF) is obtained for the carbon monoxide(CO) molecule(X1+Σ)by fitting the experimental rovibrational transitional moments. Additionally, an accurate ab initio EDMF is foun...An accurate electric dipole moment function(EDMF) is obtained for the carbon monoxide(CO) molecule(X1+Σ)by fitting the experimental rovibrational transitional moments. Additionally, an accurate ab initio EDMF is found using the highly accurate, multi-reference averaged coupled-pair functional(ACPF) approach with the basis set, aug-cc-p V6 Z, and a finite-field with ±0.005 a.u.(The unit a.u. is the abbreviation of atomic unit). This ab initio EDMF is very consistent with the fitted ones. The vibrational transition matrix moments and the Herman–Wallis factors, calculated with the Rydberg–Klein–Rees(RKR) potential and the fitted and ab initio EDMFs, are compared with experimental measurements. The consistency of these line intensities with the high-resolution transmission(HITRAN) molecular database demonstrates the improved accuracy of the fitted and ab initio EDMFs derived in this work.展开更多
A dressed-state perturbation theory beyond the rotating wave approximation （RWA） is presented to investigate the interaction between a two-level electronic transition of polar molecules and a quantized cavity field....A dressed-state perturbation theory beyond the rotating wave approximation （RWA） is presented to investigate the interaction between a two-level electronic transition of polar molecules and a quantized cavity field. Analytical expressions can be explicitly derived for both the ground- and excited-state-energy spectrums and wave functions of the system, where the contribution of permanent dipole moments （PDM） and the counter-rotating wave term （CRT） can be shown separately. The validity of these explicit results is discussed by comparison with the direct numerical simulation. Compared to the CRT coupling, PDM results in the coupling of more dressed states and the energy shift is proportional to the square of the normalized permanent dipole difference, and a greater Bloch-Siegert shift can be produced in the giant dipole molecule cavity QED. In addition, our method can also be extended to the solution of the two-level atom Rabi model Hamiltonian beyond the RWA.展开更多
The transition dipole moments（TDMs） of ultracold85 Rb133 Cs molecules between the lowest vibrational ground level, （X^1Σ~＋（ v= 0, J= 1）, and the two excited rovibrational levels, 2~3Π0＋（v′= 10, J′= 2） and...The transition dipole moments（TDMs） of ultracold85 Rb133 Cs molecules between the lowest vibrational ground level, （X^1Σ~＋（ v= 0, J= 1）, and the two excited rovibrational levels, 2~3Π0＋（v′= 10, J′= 2） and 2~1Π1（v′= 22,J′= 2）, are measured using depletion spectroscopy. The ground-state85 Rb133 Cs molecules are formed from cold mixed component atoms via the 2~3Π0-（ v= 11, J= 0） short-range level, then detected by time-of-flight mass spectrum. A home-made external-cavity diode laser is used as the depletion laser to couple the ground level and the two excited levels. Based on the depletion spectroscopy, the corresponding TDMs are then derived to be 3.5（2）×10^（-3）eαα and 1.6（1）×10^（-2）eαα, respectively, where 0）（60 represents the atomic unit of electric dipole moment. The enhance of TDM with nearly a factor of 5 for the 21Π1（v′= 22, J′= 2） excited level means that it has stronger coupling with the ground level. It is meaningful to find more levels with much more strong coupling strength by the represented depletion spectroscopy to realize direct stimulated Raman adiabatic passage transfer from scattering atomic states to deeply molecular states.展开更多
The coherent exciton plays an important role in the photosynthetic primary process, and its functions are deeply dependent on the orientation arrangements of local transition dipole moments （TDMs）. We theoretically ...The coherent exciton plays an important role in the photosynthetic primary process, and its functions are deeply dependent on the orientation arrangements of local transition dipole moments （TDMs）. We theoretically and systematically study the physical property of the coherent exciton at different orientation arrangements of the local TDMs in circular light-harvesting （LH） complexes. Especially, if the orientation arrangements are different, the delocalized TDMs of the coherent excitons and the energy locations of the optically active coherent excitons （OACEs） can be obviously different, and then there are more manners to capture, store and transfer light energy in and between LH complexes. Similarly, if the orientation arrangements are altered, light absorption and radiative intensities can be converted fully between the OACEs in the upper and lower coherent exciton bands, and then the blue and red shifts of the absorption and radiative bands of the pigment molecules can occur simultaneously at some orientation arrangements. If the systems are in the vicinities of the critical orientation arrangements, the weak static disorder or small thermal excitation can destroy the coherent electronic excitations, and then the coherent exciton cannot exist any more.展开更多
We show that it is possible to simulate an anyon by a trapped atom which possesses an induced electric dipole moment in the background of electric and magnetic fields in a specific configuration.The electric and magne...We show that it is possible to simulate an anyon by a trapped atom which possesses an induced electric dipole moment in the background of electric and magnetic fields in a specific configuration.The electric and magnetic fields we applied contain a magnetic and two electric fields.We find that when the atom is cooled down to the limit of the negligibly small kinetic energy,the atom behaves like an anyon because its angular momentum takes fractional values.The fractional part of the angular momentum is determined by both the magnetic and one of the electric fields.Roles electric and magnetic fields played are analyzed.展开更多
The 18 A-S states correlated to the lowest dissociation limit of SiTe were calculated by using a high-level multirefer-ence configuration interaction （MRCI） method, including scalar relativistic and spin-orbit coupl...The 18 A-S states correlated to the lowest dissociation limit of SiTe were calculated by using a high-level multirefer-ence configuration interaction （MRCI） method, including scalar relativistic and spin-orbit coupling effects. Based on the calculated potential energy curves, the spectroscopic constants of bound states were determined, which are well consistent with previous experimental results. The spin-orbit matrix elements between the A-S states were computed, which lead to an in-deoth understanding, of oerturbations on the electronic state a^3∏. Finally. the transition dioole moments of allowed transitionsA^1∏-X^1∑^＋,E^1∑^＋-X^1∑^＋,a^3∏-d^3△,a^3∏-d^3△,a^∏-a′^3∑^＋,a^3∏-e^3∑^-,and the radiative lifetimes of A^1∏,E^1∑^＋,and a^3∏ were evaluated.展开更多
This work is devoted to the experimental determination of the electrostatic properties of the molecular 4-methyl-7-（salicylidene amino） coumarin（C17H13NC3） using high resolution x-ray diffraction data. The experim...This work is devoted to the experimental determination of the electrostatic properties of the molecular 4-methyl-7-（salicylidene amino） coumarin（C17H13NC3） using high resolution x-ray diffraction data. The experimental results are compared with those obtained theoretically from calculation type ab initio. The experimental investigation is carried out using the molecular electron charge density distribution based on the multipolar model of Hansen and Coppens. However the theoretical calculations are conducted by using the molecular orbital B3 LYP method and the Hartree-Fock（HF） approximation with the basis set 6-31G（d,p） implemented in the Gaussian program. In addition to the structural analysis,the thermal agitation is also analyzed in terms of rigid blocks to ensure a better precision of the results. Subsequently, the electrostatic atomic and molecular properties such as the net charges, the molecular dipolar moment to highlight the nature of charge transfer existing within the molecule studied are derived. Moreover, the obtained electrostatic potential enables the localization of the electropositive and the electronegative parts of the investigated molecule. The present work reports in detail the obtained electrostatic properties of this biologically important molecule.展开更多
The high accuracy ab initio calculation method of multi-reference configuration interaction（MRCI） is used to compute the low-lying eight electronic states of CuN.The potential energy curves（PECs） of the X;∑;,1;Π...The high accuracy ab initio calculation method of multi-reference configuration interaction（MRCI） is used to compute the low-lying eight electronic states of CuN.The potential energy curves（PECs） of the X;∑;,1;Π,2;∑;,1;△,1;△,1;∑;,1;Π,and;∑;in a range of R=0.1 nm-0.5 nm are obtained and they are goodly asymptotes to the Cu（;S;） + N（;S;） and Cu（;S;）+N（;D;） dissociation limits.All the possible vibrational levels,rotational constants,and spectral constants for the six bound states of X;∑;,1;Π,2;∑;,1;△,1;∑;,and 1;Π are obtained by solving the radial Schrdinger equation of nuclear motion with the Le Roy provided Level 8.0 program.Also the transition dipole moments from the ground state X;∑;to the excited states 1;Π and 2;∑;are calculated and the result indicates that the 2;∑-X;∑ transition has a much higher transition dipole moment than the 1;Π-X;∑;transition even though the l;Π state is much lower in energy than the 2;∑;state.展开更多
We investigate the effect of Zn doping on the dielectricity and ferroelectricity of a series of polycrystalline Sr0.9-xZnxBa0.1TiO3（0.0% ≤ x ≤ 5.0%） ceramics. It is surprisingly observed that the Zn doping will pr...We investigate the effect of Zn doping on the dielectricity and ferroelectricity of a series of polycrystalline Sr0.9-xZnxBa0.1TiO3（0.0% ≤ x ≤ 5.0%） ceramics. It is surprisingly observed that the Zn doping will produce the multifold polar states, i.e., the Zn-doped ceramic will convert a reduced polar state into an enhanced polar state, and eventually into a stabilized polar state with increasing the doping level x. It is revealed that in the background of quantum fluctuations, the competition between the Zn-doping-induced lattice contraction and the Ba-doping-induced lattice expansion is responsible for both the reduced polar state and the enhanced polar state coming into being. Also, the addition of the antiferrodistortive effect, which is the antipolar interaction originating from the opposite tilted-Ti O6 octahedra rotation, represents the core physics behind the stabilized polar state.展开更多
CS molecule, which plays a key role in atmospheric and astrophysical circumstances, has drawn great attention for long time. Owing to its large state density, the detailed information of the electronic structure of CS...CS molecule, which plays a key role in atmospheric and astrophysical circumstances, has drawn great attention for long time. Owing to its large state density, the detailed information of the electronic structure of CS is still lacking. In this work, the high-level MRCI+Q method is used to compute the potential energy curves, dipole moments and transition dipole moments of singlet and triplet states correlated with the lowest dissociation limit of CS, based on which high accurate vibration-rotation levels and spectroscopic constants of bound states are evaluated. The opacity of CS relevant to atmospheric circumstance is computed at a pressure of 100 atms for different temperatures. With the increase of temperature,band systems from different transitions mingle with each other, and band boundaries become blurred, which are originated from the increased population on vibrational excited states and electronic excited states at high temperature.展开更多
Multireference configuration interaction calculations are carried out on 11 Λ–S low-lying electronic states of indium dimers. The states are investigated with spin–orbit pseudopotentials via the state-interacting m...Multireference configuration interaction calculations are carried out on 11 Λ–S low-lying electronic states of indium dimers. The states are investigated with spin–orbit pseudopotentials via the state-interacting method, and characterized by fitted spectroscopic constants based on computed potential energy curves. The vibrational structures of the double-potential well 0^＋g （I） （ ^3 Σ g^- ） state are also analyzed. The experimentally observed absorption spectrum centred at ～ 13000cm-1 is simulated and assigned to X 3 Πu （v＇=0）–3Πg transition according to the present ab initio calculations on transition energies and dipole moment functions.展开更多
The ground state of osmium monoxide(OsO) has long been controversial. In this paper, the low-lying Λ–S and ? electronic states of OsO have been comprehensively studied by the high-precision multi-reference calculati...The ground state of osmium monoxide(OsO) has long been controversial. In this paper, the low-lying Λ–S and ? electronic states of OsO have been comprehensively studied by the high-precision multi-reference calculations. The ground state of OsO is unexpectedly the closed-shell1Σ+state with a double bond instead of the previously reported3Φ or5Σ+state;after including the spin–orbit coupling effects, the ground state becomes3Π2. With the help of the theoretical spectroscopic constants and transition dipole moments, the emission spectra in the region of 405 nm–875 nm are assigned.Our results will facilitate the future studies of absorption and emission spectra of OsO.展开更多
Potential energy curves for the lowest electronic states of LaB and LaB- have been calculated by ab initio calculations.The diffusion Monte Carlo method has been employed in combination with three different trial func...Potential energy curves for the lowest electronic states of LaB and LaB- have been calculated by ab initio calculations.The diffusion Monte Carlo method has been employed in combination with three different trial functions. Spectroscopic constants have also been numerically derived for the neutral molecule and compared with the only available theoretical work;^（[19]） however, predictions are provided for the corresponding constants for the anionic species which have not been reported yet. Our calculations suggest the high spin quintet state of LaB as the ground state with the triplet state higher in energy irrespective of the type of the functional used. This suggestion is in good accordance with the previous theoretical results calculated at B3LYP/LANL2DZ level of theory, whereas it contradicts with the prediction based upon B3LYP/SDD calculations in the same study. Moreover, variations of the permanent dipole moments as a function of the internuclear separations for the two electronic states of the neutral molecule have been studied and analyzed.展开更多
One of the great difficulties in understanding nitrogen plasma elementary processes is the lack of an available database of the cross-sections of electron-impact excitations and radiations. Ab initio calculations of v...One of the great difficulties in understanding nitrogen plasma elementary processes is the lack of an available database of the cross-sections of electron-impact excitations and radiations. Ab initio calculations of vibrational excitation cross sections for electron collisions with nitrogen molecules in low-lying states using similarity function approach, such as a-a＇, a-w, B-B＇ and B-W transition systems, are reported here for the first time. In the meantime, the average excitation energies of neighboring levels of these systems have been calculated. In order to obtain the cross sections, accurate spectroscopic constants and transition dipole moments have been investigated. Potential energy curves and other electronic transition dipole moments for the low-lying states of N2 have been re-evaluated using complete active space self-consistent field （CASSCF） approach with aug-cc-pVqZ basis set. The calculated cross-sections could provide a database for studying the elementary processes and the properties in N2 plasma.展开更多
基金Project supported by the National Natural Science Foundation of China （Grant Nos 20103007 and 20473079）.
文摘Stretching vibrational band intensities of XH3 （X=N, Sb） molecules are investigated employing three-dimensional dipole moment surfaces combined with the local mode Hamiltonian model. The dipole moment surfaces of NH3 and SbH3 are calculated with the density functional theory and at the correlated MP2 level, respectively. The calculated band intensities are in good agreement with the available experimental data. The contribution to the band intensities from the different terms in the polynomial expansion of the dipole moments of four group V hydrides （NH3, PH3, AsH3 and SbH3） are discussed. It is concluded that the breakdown of the bond dipole approximation must be considered. The intensity “borrowing” effect due to the wave function mixing among the stretching vibrational states is found to be less significant for the molecules that reach the local mode limit.
基金Project supported by the National Natural Science Foundation of China （Grant No 10174019）, the Natural Science Foundation of Henan Province, China （Grant No 2006,140008） and Henan Innovation for University Prominent Research Talents （Grant No 2006KYCX002）.Acknowledgement We heartily thank Professor Zhu Zheng-He at Sichuan University for his helpful discussion about the reasonable dissociation limits during the planning stage of these calculations.
文摘The reasonable dissociation limit of the A^1∑＋ state ^7LiH molecule is obtained. The accurate dissociation energy and the equilibrium geometry of this state are calculated using a symmetry-adapted-cluster configuration-interaction method in complete active space for the first time, The whole potential energy curve and the dipole moment function for the A^1∑＋ state are calculated over a wide internuclear separation range from about 0.1 to 1.4 nm. The calculated equilibrium geometry and dissociation energy of this potential energy curve are of Re=0.2487 nm and De=1.064eV, respectively. The unusual negative values of the anharmonicity constant and the vibration-rotational coupling constant are of ωeXe=-4.7158cm^-1 and αe=0.08649cm^-1, respectively. The vertical excitation energy from the ground to the A^1∑＋ state is calculated and the value is of 3.613eV at 0.15875nm （the equilibrium position of the ground state）. The highly anomalous shape of this potential energy curve, which is exceptionally flat over a wide radial range around the equilibrium position, is discussed in detail. The harmonic frequency value of 502.47cm^-1 about this state is approximately estimated. Careful comparison of the theoretical determinations with those obtained by previous theories about the A^1∑＋ state dissociation energy clearly shows that the present calculations are much closer to the experiments than previous theories, thus represents an improvement.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.91421305,91121005,and 11674359)the National Key Basic Research Program of China(Grant No.2013CB922003)
文摘We report a sensitive detection of high Rydberg atom with large dipole moment utilizing its deflection near a pair of parallel cylindrical copper rods which are oppositely charged. When the low-field seeking state Rydberg atoms fly across the gradient electric field formed by the pair of rods, they will be pushed away from the rods while the high-field seeking state ones will be attracted towards the rods. These atoms will form different patterns on an ion imaging system placed downwards at the end of the rods. The spatial distribution of the deflected atoms on the imaging system is also simulated, in good agreement with the experimental results, from which we can deduce the quantum state information of the excited atoms. This state resolvable Rydberg atom detection can be used for the dynamics research of the dipole-dipole interaction between atoms with large dipole moments.
基金Supported by the China Scholarship Councilthe Hanjiang Scholar Project of Shaanxi University of Technology
文摘The quantum phase effects for induced electric and magnetic dipole moments are investigated. It is shown that the phase shift received by the induced electric dipole has the same form as the one induced by magnetic dipole moment, therefore the total phase is a hybrid of these two types of phase. This feature indicates that to have a decisive measurement on either one of these two phases, it is necessary to measure the velocity dependence of the observed phase.
基金supported by the National Basic Research Program of China(Grant No.2012CB921603)the National Natural Science Foundation of China(GrantNos.61378039,61078013,61178009,and 11274209)+3 种基金the Program for Changjiang Scholars and Innovative Research Team in University,China(Grant No.IRT13076)the Fund for Fostering Talents in Basic Science of the National Natural Science Foundation of China(Grant No.J1210036)the Natural Science Foundation of Shanxi Province,China(Grant No.2012011003-2)the Shanxi International Collaboration Program,China(Grant No.2010081046)
文摘Recently, the diverse properties of Rydberg atoms, which probably arise from its large electric dipole moment （EDM）, have been explored. In this paper, we report electric dipole moments along with Stark energies and charge densities of lithium Rydberg states in the presence of electric fields, calculated by matrix diagonalization. Huge electric dipole moments are discovered. In order to check the validity of the EDMs, we also use these electric dipole moments to calculate the Stark energies by numerical integration. The results agree with those calculated by matrix diagonalization.
基金Project supported by the National Natural Science Foundation of China(Grant No.11647075)the Scientific Research Fund of Sichuan Provincial Education Department,China(Grant No.14ZB0284)the Scientific Research Key Project of Yibin University,China(Grant No.2013QD09)
文摘An ab initio calculations on the ground and low-lying excited statesX2∑＋,2^2∑＋,3^2∑＋,1^4∏,2^4∏,1^4∑＋,2^4∑＋,and 3^4∑＋of KBe molecule have been performed using multireference configuration interaction （MRCI） plus Davidsoncorrections （MRCI＋Q） approach with all electron basis set aug-cc-pCV5Z-DK for Be and def2-AQZVPP-JKFI for K.3^2∑＋,1^4∏,2^4∏,1^4∑＋,2^4∑＋and3^4∑＋states are investigated for the first time. Inner shell electron correlations are computed on the potential energy curves （PECs） calculations. The spectroscopic and molecular parameters are also predicted. In addition, The transition properties including transition dipole moment, Franck-Condon factors qv′v″, Einstein coefficients Av′v″, and the radiative lifetimesτ′for the2^2∑＋-X2∑＋,3^2∑＋-X2∑＋,and 2^4∏-1^4∏ transitions are predictedat the same time.
基金supported by the National Natural Science Foundation of China(Grant Nos.11374217 and 11474207)
文摘An accurate electric dipole moment function(EDMF) is obtained for the carbon monoxide(CO) molecule(X1+Σ)by fitting the experimental rovibrational transitional moments. Additionally, an accurate ab initio EDMF is found using the highly accurate, multi-reference averaged coupled-pair functional(ACPF) approach with the basis set, aug-cc-p V6 Z, and a finite-field with ±0.005 a.u.(The unit a.u. is the abbreviation of atomic unit). This ab initio EDMF is very consistent with the fitted ones. The vibrational transition matrix moments and the Herman–Wallis factors, calculated with the Rydberg–Klein–Rees(RKR) potential and the fitted and ab initio EDMFs, are compared with experimental measurements. The consistency of these line intensities with the high-resolution transmission(HITRAN) molecular database demonstrates the improved accuracy of the fitted and ab initio EDMFs derived in this work.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB01010200)the Hundred Talents Program of the Chinese Academy of Sciences(Grant No.Y321311401)+2 种基金the National Natural Science Foundation of China(Grant Nos.61475139,11347147,and11247014)the National Basics Research Program of China(Grant No.2013CB329501)the Zhejiang Provincial Natural Science Foundation(Grant No.LQ13A040006)
文摘A dressed-state perturbation theory beyond the rotating wave approximation （RWA） is presented to investigate the interaction between a two-level electronic transition of polar molecules and a quantized cavity field. Analytical expressions can be explicitly derived for both the ground- and excited-state-energy spectrums and wave functions of the system, where the contribution of permanent dipole moments （PDM） and the counter-rotating wave term （CRT） can be shown separately. The validity of these explicit results is discussed by comparison with the direct numerical simulation. Compared to the CRT coupling, PDM results in the coupling of more dressed states and the energy shift is proportional to the square of the normalized permanent dipole difference, and a greater Bloch-Siegert shift can be produced in the giant dipole molecule cavity QED. In addition, our method can also be extended to the solution of the two-level atom Rabi model Hamiltonian beyond the RWA.
基金Supported by the National Key Research and Development Program of China under Grant No 2017YFA0304203the National Natural Science Foundation of China under Grant Nos 61675120 and 11434007+3 种基金the National Natural Science Foundation of China for Excellent Research Team under Grant No 61121064the Shanxi Scholarship Council of China,the 1331KSCthe PCSIRT under Grant No IRT13076the Applied Basic Research Project of Shanxi Province under Grant No 201601D202008
文摘The transition dipole moments（TDMs） of ultracold85 Rb133 Cs molecules between the lowest vibrational ground level, （X^1Σ~＋（ v= 0, J= 1）, and the two excited rovibrational levels, 2~3Π0＋（v′= 10, J′= 2） and 2~1Π1（v′= 22,J′= 2）, are measured using depletion spectroscopy. The ground-state85 Rb133 Cs molecules are formed from cold mixed component atoms via the 2~3Π0-（ v= 11, J= 0） short-range level, then detected by time-of-flight mass spectrum. A home-made external-cavity diode laser is used as the depletion laser to couple the ground level and the two excited levels. Based on the depletion spectroscopy, the corresponding TDMs are then derived to be 3.5（2）×10^（-3）eαα and 1.6（1）×10^（-2）eαα, respectively, where 0）（60 represents the atomic unit of electric dipole moment. The enhance of TDM with nearly a factor of 5 for the 21Π1（v′= 22, J′= 2） excited level means that it has stronger coupling with the ground level. It is meaningful to find more levels with much more strong coupling strength by the represented depletion spectroscopy to realize direct stimulated Raman adiabatic passage transfer from scattering atomic states to deeply molecular states.
基金project supported by the National Natural Science Foundation of China （Grant Nos 60438020 and 60321003）, and the Knowledge innovation program of the Chinese Academy of Sciences （Grant No KJCX2-SW-W14）.
文摘The coherent exciton plays an important role in the photosynthetic primary process, and its functions are deeply dependent on the orientation arrangements of local transition dipole moments （TDMs）. We theoretically and systematically study the physical property of the coherent exciton at different orientation arrangements of the local TDMs in circular light-harvesting （LH） complexes. Especially, if the orientation arrangements are different, the delocalized TDMs of the coherent excitons and the energy locations of the optically active coherent excitons （OACEs） can be obviously different, and then there are more manners to capture, store and transfer light energy in and between LH complexes. Similarly, if the orientation arrangements are altered, light absorption and radiative intensities can be converted fully between the OACEs in the upper and lower coherent exciton bands, and then the blue and red shifts of the absorption and radiative bands of the pigment molecules can occur simultaneously at some orientation arrangements. If the systems are in the vicinities of the critical orientation arrangements, the weak static disorder or small thermal excitation can destroy the coherent electronic excitations, and then the coherent exciton cannot exist any more.
基金the National Natural Science Foundation of China(Grant No.11465006),20200981-SIP-IPN,and the CONACyT(Grant No.288856-CB-2016).
文摘We show that it is possible to simulate an anyon by a trapped atom which possesses an induced electric dipole moment in the background of electric and magnetic fields in a specific configuration.The electric and magnetic fields we applied contain a magnetic and two electric fields.We find that when the atom is cooled down to the limit of the negligibly small kinetic energy,the atom behaves like an anyon because its angular momentum takes fractional values.The fractional part of the angular momentum is determined by both the magnetic and one of the electric fields.Roles electric and magnetic fields played are analyzed.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11034003,11074095,and 11274140)the Natural Science Foundation of Heilongjiang Province,China(Grant No.F201335)the Scientific and Technological Research Foundation of Qiqihar,China(Grant No.GYGG-201209-1)
文摘The 18 A-S states correlated to the lowest dissociation limit of SiTe were calculated by using a high-level multirefer-ence configuration interaction （MRCI） method, including scalar relativistic and spin-orbit coupling effects. Based on the calculated potential energy curves, the spectroscopic constants of bound states were determined, which are well consistent with previous experimental results. The spin-orbit matrix elements between the A-S states were computed, which lead to an in-deoth understanding, of oerturbations on the electronic state a^3∏. Finally. the transition dioole moments of allowed transitionsA^1∏-X^1∑^＋,E^1∑^＋-X^1∑^＋,a^3∏-d^3△,a^3∏-d^3△,a^∏-a′^3∑^＋,a^3∏-e^3∑^-,and the radiative lifetimes of A^1∏,E^1∑^＋,and a^3∏ were evaluated.
文摘This work is devoted to the experimental determination of the electrostatic properties of the molecular 4-methyl-7-（salicylidene amino） coumarin（C17H13NC3） using high resolution x-ray diffraction data. The experimental results are compared with those obtained theoretically from calculation type ab initio. The experimental investigation is carried out using the molecular electron charge density distribution based on the multipolar model of Hansen and Coppens. However the theoretical calculations are conducted by using the molecular orbital B3 LYP method and the Hartree-Fock（HF） approximation with the basis set 6-31G（d,p） implemented in the Gaussian program. In addition to the structural analysis,the thermal agitation is also analyzed in terms of rigid blocks to ensure a better precision of the results. Subsequently, the electrostatic atomic and molecular properties such as the net charges, the molecular dipolar moment to highlight the nature of charge transfer existing within the molecule studied are derived. Moreover, the obtained electrostatic potential enables the localization of the electropositive and the electronegative parts of the investigated molecule. The present work reports in detail the obtained electrostatic properties of this biologically important molecule.
文摘The high accuracy ab initio calculation method of multi-reference configuration interaction（MRCI） is used to compute the low-lying eight electronic states of CuN.The potential energy curves（PECs） of the X;∑;,1;Π,2;∑;,1;△,1;△,1;∑;,1;Π,and;∑;in a range of R=0.1 nm-0.5 nm are obtained and they are goodly asymptotes to the Cu（;S;） + N（;S;） and Cu（;S;）+N（;D;） dissociation limits.All the possible vibrational levels,rotational constants,and spectral constants for the six bound states of X;∑;,1;Π,2;∑;,1;△,1;∑;,and 1;Π are obtained by solving the radial Schrdinger equation of nuclear motion with the Le Roy provided Level 8.0 program.Also the transition dipole moments from the ground state X;∑;to the excited states 1;Π and 2;∑;are calculated and the result indicates that the 2;∑-X;∑ transition has a much higher transition dipole moment than the 1;Π-X;∑;transition even though the l;Π state is much lower in energy than the 2;∑;state.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.1130415851431006+5 种基金51102277and 11104118)the Scientific Research Foundation of Nanjing University of Posts and TelecommunicationsChina(Grant No.NY213020)the Qing Lan Project of Jiangsu ProvinceChina
文摘We investigate the effect of Zn doping on the dielectricity and ferroelectricity of a series of polycrystalline Sr0.9-xZnxBa0.1TiO3（0.0% ≤ x ≤ 5.0%） ceramics. It is surprisingly observed that the Zn doping will produce the multifold polar states, i.e., the Zn-doped ceramic will convert a reduced polar state into an enhanced polar state, and eventually into a stabilized polar state with increasing the doping level x. It is revealed that in the background of quantum fluctuations, the competition between the Zn-doping-induced lattice contraction and the Ba-doping-induced lattice expansion is responsible for both the reduced polar state and the enhanced polar state coming into being. Also, the addition of the antiferrodistortive effect, which is the antipolar interaction originating from the opposite tilted-Ti O6 octahedra rotation, represents the core physics behind the stabilized polar state.
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 11934004 and 12203106)Fundamental Research Funds in Heilongjiang Province Universities, China (Grant No. 145109127)the Scientific Research Plan Projects of Heilongjiang Education Department, China (Grant Nos. WNCGQJKF202103 and DWCGQKF202104)。
文摘CS molecule, which plays a key role in atmospheric and astrophysical circumstances, has drawn great attention for long time. Owing to its large state density, the detailed information of the electronic structure of CS is still lacking. In this work, the high-level MRCI+Q method is used to compute the potential energy curves, dipole moments and transition dipole moments of singlet and triplet states correlated with the lowest dissociation limit of CS, based on which high accurate vibration-rotation levels and spectroscopic constants of bound states are evaluated. The opacity of CS relevant to atmospheric circumstance is computed at a pressure of 100 atms for different temperatures. With the increase of temperature,band systems from different transitions mingle with each other, and band boundaries become blurred, which are originated from the increased population on vibrational excited states and electronic excited states at high temperature.
基金Project supported by the National Magnetic Confinement Fusion Science Program of China (Grant No. 2010GB104003)the Fundamental Research Funds for the Central Universities (Grant No. 450060481375)
文摘Multireference configuration interaction calculations are carried out on 11 Λ–S low-lying electronic states of indium dimers. The states are investigated with spin–orbit pseudopotentials via the state-interacting method, and characterized by fitted spectroscopic constants based on computed potential energy curves. The vibrational structures of the double-potential well 0^＋g （I） （ ^3 Σ g^- ） state are also analyzed. The experimentally observed absorption spectrum centred at ～ 13000cm-1 is simulated and assigned to X 3 Πu （v＇=0）–3Πg transition according to the present ab initio calculations on transition energies and dipole moment functions.
基金Project supported by the National Natural Science Foundation of China (Grant No. 22073072)the Double First-Class University Construction Project of Northwest University。
文摘The ground state of osmium monoxide(OsO) has long been controversial. In this paper, the low-lying Λ–S and ? electronic states of OsO have been comprehensively studied by the high-precision multi-reference calculations. The ground state of OsO is unexpectedly the closed-shell1Σ+state with a double bond instead of the previously reported3Φ or5Σ+state;after including the spin–orbit coupling effects, the ground state becomes3Π2. With the help of the theoretical spectroscopic constants and transition dipole moments, the emission spectra in the region of 405 nm–875 nm are assigned.Our results will facilitate the future studies of absorption and emission spectra of OsO.
文摘Potential energy curves for the lowest electronic states of LaB and LaB- have been calculated by ab initio calculations.The diffusion Monte Carlo method has been employed in combination with three different trial functions. Spectroscopic constants have also been numerically derived for the neutral molecule and compared with the only available theoretical work;^（[19]） however, predictions are provided for the corresponding constants for the anionic species which have not been reported yet. Our calculations suggest the high spin quintet state of LaB as the ground state with the triplet state higher in energy irrespective of the type of the functional used. This suggestion is in good accordance with the previous theoretical results calculated at B3LYP/LANL2DZ level of theory, whereas it contradicts with the prediction based upon B3LYP/SDD calculations in the same study. Moreover, variations of the permanent dipole moments as a function of the internuclear separations for the two electronic states of the neutral molecule have been studied and analyzed.
基金supported by National Natural Science Foundation of China(Nos.11175035,10875023)the National Magnetic Confinement Fusion Science Program of China(No.2013GB109005)+1 种基金Chinesisch-Deutsches Forschungsprojekt(GZ768)the Fundamental Research Fundsfor the Central Universities of China(No.DUT12ZD(G)01)
文摘One of the great difficulties in understanding nitrogen plasma elementary processes is the lack of an available database of the cross-sections of electron-impact excitations and radiations. Ab initio calculations of vibrational excitation cross sections for electron collisions with nitrogen molecules in low-lying states using similarity function approach, such as a-a＇, a-w, B-B＇ and B-W transition systems, are reported here for the first time. In the meantime, the average excitation energies of neighboring levels of these systems have been calculated. In order to obtain the cross sections, accurate spectroscopic constants and transition dipole moments have been investigated. Potential energy curves and other electronic transition dipole moments for the low-lying states of N2 have been re-evaluated using complete active space self-consistent field （CASSCF） approach with aug-cc-pVqZ basis set. The calculated cross-sections could provide a database for studying the elementary processes and the properties in N2 plasma.
