In the present work,we extend the Coulomb and Proximity Potential Model(CPPM)to study two-proton(2p)radioactivity from excited states while the proximity potential is chosen as AW95 proposed by Aage Withner in 1995.De...In the present work,we extend the Coulomb and Proximity Potential Model(CPPM)to study two-proton(2p)radioactivity from excited states while the proximity potential is chosen as AW95 proposed by Aage Withner in 1995.Demonstration reveals that the theoretical results acquired by CPPM exhibit a high level of consistency with prior theoretical models such as the unified fission model(UFM),generalized liquid-drop model(GLDM)and effective liquid-drop model(ELDM).Furthermore,within the CPPM,we predicted the half-lives of potential 2p radioactive nuclei for which experimental data are currently unavailable.The predicted results were then assessed,compared with UFM,ELDM and GLDM models,and examined in detail.展开更多
We theoretically investigate high-order harmonic generation(HHG) of helium(He), lithium cation(Li+), and beryllium dication(Be2+) using the time-dependent Hartree–Fock method to solve the three-dimensional time-depen...We theoretically investigate high-order harmonic generation(HHG) of helium(He), lithium cation(Li+), and beryllium dication(Be2+) using the time-dependent Hartree–Fock method to solve the three-dimensional time-dependent Schr ¨odinger equation. It is found that the intensity of the HHG increases significantly from a certain harmonic order below the ionization threshold, and the initial position of the enhancement does not depend on the intensity or the wavelength of the driving laser field. Further analysis shows that excited states play an important role on this enhancement,consistent with the excited-state tunneling mechanism [Phys. Rev. Lett. 116 123901(2016)]. Our results unambiguously show that excited-state tunneling is essential for understanding the enhancement of HHG. Accordingly, a four-step model is herein proposed to illustrate the multiphoton excitation effect in helium-like ions, which enriches the physics of HHG enhancement.展开更多
Investigating the impact of microhydration on the excited-states and electronic excitation properties of biomolecules has remained one of the important yet challenging aspects of science because of the complexity of d...Investigating the impact of microhydration on the excited-states and electronic excitation properties of biomolecules has remained one of the important yet challenging aspects of science because of the complexity of developing models. However, with the advent of computational chemistry methods such as TD-DFT, many useful insights about the electronic excitation energy and excited-state nature of biomolecules can be explored. Accordingly, in our study, we have incorporated the TD-DFT/wB97XD/cc-pVTZ method to study the excited state properties of N-acetyl phenylalanine amide (NAPA-A(H<sub>2</sub>O) <sub>n</sub>) (n = 1 to 4) clusters from ground to the tenth lowest gaseous singlet excited state. We found that the C=O bond length gradually increases both in N-terminal amide and C-terminal amide after the sequential addition of water molecules because of intermolecular H-bonding and this intermolecular H-bonding becomes weaker after the sequential addition of H<sub>2</sub>O molecules. The UV absorption maxima of NAPA-A (H<sub>2</sub>O)<sub>n</sub> (n = 1 - 4) clusters consisted of two peaks that are S<sub>5</sub>←S<sub>0</sub> (1<sup>st</sup> absorption) and S<sub>6</sub>←S<sub>0</sub> (2<sup>nd</sup> absorption) excitations. The first absorption maxima were blue-shifted with the increase in oscillator strength. This means that strong H-bonds reduce the charge transfer and make clusters more rigid. On the other hand, the second absorption maxima were red-shifted with the decrease in oscillator strength. In the ECD spectra, the negative bands indicate the presence of an amide bond and L-configuration of micro hydrated NAPA-A clusters. Finally, our calculated absorption and fluorescence energy confirm that all the NAPA-A (H<sub>2</sub>O) <sub>n</sub> (n = 0 - 4) clusters revert to the ground state from the fluorescent state by emitting around 5.490 eV of light.展开更多
In this study,we systematically investigated the two-proton(2p)radioactivity half-lives from the excited state of nuclei near the proton drip line within the Gamowlike model(GLM)and modified Gamow-like model(MGLM).The...In this study,we systematically investigated the two-proton(2p)radioactivity half-lives from the excited state of nuclei near the proton drip line within the Gamowlike model(GLM)and modified Gamow-like model(MGLM).The calculated results were highly consistent with the theoretical values obtained using the unified fission model[Chin.Phys.C 45,124105(2021)],effective liquid drop model,and generalized liquid drop model[Acta Phys.Sin 71,062301(2022)].Furthermore,utilizing the GLM and MGLM,we predicted the 2p radioactivity halflives from the excited state for some nuclei that are not yet available experimentally.Simultaneously,by analyzing the calculated results from these theoretical models,it was found that the half-lives are strongly dependent on Qand l.展开更多
In this paper, we have declined the formalism of the method of the Modified Atomic Orbital Theory (MAOT) applied to the calculations of energies of doubly excited states 2<em>snp</em>, 3<em>snp</e...In this paper, we have declined the formalism of the method of the Modified Atomic Orbital Theory (MAOT) applied to the calculations of energies of doubly excited states 2<em>snp</em>, 3<em>snp</em>, and 4<em>snp</em> Helium-like systems. Then we also applied the variational procedure of the Modified Atomic Orbital Theory to the computations of total energies, excitation energies of doubly-excited states 2<em>snp</em>, 3<em>snp</em>, 4<em>snp</em> types of Helium-like systems. The results obtained in this work are in good agreement with the experimental and theoretical values available.展开更多
As one of the biological endogenous pigments,biliverdin(BV)and its dimethyl ester(BVE)have extremely weak uorescence in solution with quantum yield less than 0.01%.However,the situation reverses with the addition of z...As one of the biological endogenous pigments,biliverdin(BV)and its dimethyl ester(BVE)have extremely weak uorescence in solution with quantum yield less than 0.01%.However,the situation reverses with the addition of zinc ions.The strength for uorescence of BVE-Zn^2+ complex is greatly enhanced and uorescence quantum yield can increase to5%.Herein,we studied ultrafast excited state dynamics of BVE-Zn^2+ complex in ethanol,npropanol,and DMSO solutions in order to reveal the mechanism of uorescence quantum yield enhancement.The results show that BVE can form a stable coordination complex with zinc with 1:1 stoichiometry in solution.BVE is structurally and energetically more stable in the complex.Using picosecond time-resolve uorescence and femtosecond transient absorption spectroscopy,we show that smaller non-radiative rate constant of BVE-Zn^2+ complex in DMSO is the key to increasing its uorescence quantum yield and the excited state decay mechanism is also revealed.These results provide valuable information about the uorescence property change after BVE binding to metal ions and may provide a guidance for the study of phytochromes or other uorescence proteins in which BV/BVE acts as chromophores.展开更多
A four-level decay model of 6P7/2 excited state of Eu(2+ ion in KMgF3: Eu2+ has been proposed. The decay profiles of the 6P7/2 excited state of Eu2+ are two exponential and the physical implication of each term in the...A four-level decay model of 6P7/2 excited state of Eu(2+ ion in KMgF3: Eu2+ has been proposed. The decay profiles of the 6P7/2 excited state of Eu2+ are two exponential and the physical implication of each term in the fit equation responsible for the model is interpreted. The data obtained spectroscopically are in good agreement with the fit results.展开更多
Two-photon absorption in systems with parity permits access to states that cannot be directly prepared by onephoton absorption. Here we investigate ultrafast internal conversion(IC) dynamics of furan by using this str...Two-photon absorption in systems with parity permits access to states that cannot be directly prepared by onephoton absorption. Here we investigate ultrafast internal conversion(IC) dynamics of furan by using this strategy in combination with femtosecond time-resolved photoelectron imaging. The dark Rydberg S_1 and bright valence S_2 states are simultaneously excited by two photons of 405 nm, and then ionized by two photons of 800 nm. The IC from S_2 to S_1 is clearly observed and extracted from the time dependence of the higher photoelectron kinetic energy(PKE) component. More importantly, the internal conversions to hot S_0 from directly-prepared S_1 and secondarily-populated S_1 are unambiguously identified by the time-dependence of the lower PKE component.The average lifetime of the S_2 and S_1 states is measured to be 29 fs. The internal conversions of S_2 to S_1, S_1 to hot S_0 occur on estimated timescales of 15.4 fs and 38 fs, respectively.展开更多
In this work, the total energies of doubly excited states (<em>ns</em><sup>2</sup>) <sup>1</sup>S<sup>e</sup>, (<em>np</em><sup>2</sup>) <sup&...In this work, the total energies of doubly excited states (<em>ns</em><sup>2</sup>) <sup>1</sup>S<sup>e</sup>, (<em>np</em><sup>2</sup>) <sup>1</sup>D<sup>e</sup>, (<em>nd</em><sup>2</sup>) <sup>1</sup>G<sup>e</sup>, (<em>nf</em><sup>2</sup>) <sup>1</sup>I<sup>e</sup>, (<em>ng</em><sup>2</sup>) <sup>1</sup>K<sup>e</sup>, and (<em>nh</em><sup>2</sup>) <sup>1</sup>M<sup>e</sup> of the helium isoelectronic sequence with Z ≤ 10 are calculated in the framework of the variational method of the Screening Constant by Unit Nuclear Charge (SCUNC). These calculations are performed using a new wavefunction correlated to Hylleraas-type. The possibility of using the SCUNC method in the investigation of high-lying Doubly Excited States(DES) in two-electron systems is demonstrated in the present work in the case of the (<em>nl</em><sup>2</sup>) <sup>1</sup><em>L</em><sup><span style="white-space:nowrap;"><span style="white-space:nowrap;"><span style="white-space:nowrap;"><em>π</em></span></span></span></sup> doubly excited states, where accurate total energies are tabulated up to <em>n</em> = 20. All the results obtained in this paper are in agreement with the values of the available literature and may be useful for future experimental and theoretical studies on the doubly excited (<em>nl</em><sup>2</sup>) <sup>1</sup><em>L</em><sup><span style="white-space:nowrap;"><span style="white-space:nowrap;"><em>π</em></span></span></sup> states of two-electron systems.展开更多
The newly discovered neutron halos in the excited states of nuclei 12B, 13C, and 209pb are studied by therelativistic mean-field theory. The calculated binding energies are very close to the experimental ones. The exp...The newly discovered neutron halos in the excited states of nuclei 12B, 13C, and 209pb are studied by therelativistic mean-field theory. The calculated binding energies are very close to the experimental ones. The experimentally extracted root-mean-square radii of the last neutron with different occupations in nuclei are well reproduced bycalculations. New candidates for the neutron halos in excited states are predicted and are useful for further search ofneutron halos in the excited states of stable nuclei.展开更多
Based on the obtained energy values of 1s 2 n p (n ≤ 9) states for lithium-like systems from Z =11 to 20 (by the authors of this paper:Hu M H and Wang Z W 2004 Chin.Phys.13 662),this paper determines the quantum defe...Based on the obtained energy values of 1s 2 n p (n ≤ 9) states for lithium-like systems from Z =11 to 20 (by the authors of this paper:Hu M H and Wang Z W 2004 Chin.Phys.13 662),this paper determines the quantum defects,as slowly varying function of energy,of this Rydberg series.Using them as input,it can predict the energies of any highly excited states below the ionization threshold for this series according to the quantum defect theory.The regularities of variation for quantum defects of the series along this isoelectronic sequence are physically analysed and discussed.The screening parameters,which are equal to the effective screening charge of the core-electrons,are also obtained.展开更多
Excited-state hydrogen-bonding dynamics of N-methylformamide (NMF) in water has been investigated by time-dependent density functional theory (TDDFT) method. The ground-state geometry optimizations were calculated by ...Excited-state hydrogen-bonding dynamics of N-methylformamide (NMF) in water has been investigated by time-dependent density functional theory (TDDFT) method. The ground-state geometry optimizations were calculated by density functional theory (DFT) method, while the electronic transition energies and corresponding oscillation strengths of the low-lying electronically excited states of isolated NMF, water monomers and the hydrogen-bonded NMF-H 2 O were calculated by TDDFT method. According to Zhao's rule on the excited-state hydrogen bonding dynamics, our results demonstrate that the intermolecular hydrogen bond C=O···O-H is strengthened and weakened in different electronically excited states. The hydrogen bond strengthening and weakening in the electronically excited state plays an important role in the photophysics of NMF in solutions.展开更多
With hydrogen-like impurity(HLI) located in the center of Cs I quantum pseudodot(QPD) and by using the variational method of Pekar type(VMPT), we investigate the first-excited state energy(FESE), excitation energy and...With hydrogen-like impurity(HLI) located in the center of Cs I quantum pseudodot(QPD) and by using the variational method of Pekar type(VMPT), we investigate the first-excited state energy(FESE), excitation energy and transition frequency of the strongly-coupled bound polaron in the present paper. Temperature effects on bound polaron properties are calculated by employing the quantum statistical theory(QST). According to the present work's numerical results, the FESE, excitation energy and transition frequency decay(amplify) with raising temperature in the regime of lower(higher)temperature. They are decreasing functions of Coulomb impurity potential strength.展开更多
We theoretically investigate the contribution of the excited state to the ellipticity of the harmonics from H+2 at different orientation angles irradiated by a linearly polarized laser pulse. It is found that the firs...We theoretically investigate the contribution of the excited state to the ellipticity of the harmonics from H+2 at different orientation angles irradiated by a linearly polarized laser pulse. It is found that the first excited state has a significant influence to the ellipticity of the harmonics, and the contribution of higher excited states to the ellipticity can be neglected.Moreover, the conclusion is not dependent on the laser intensity.展开更多
Owing to the importance of excited state dynamical relaxation, the excited state intramolecular proton transfer(ESIPT) mechanism for a novel compound containing dual hydrogen bond(abbreviated as "1-enol") is...Owing to the importance of excited state dynamical relaxation, the excited state intramolecular proton transfer(ESIPT) mechanism for a novel compound containing dual hydrogen bond(abbreviated as "1-enol") is studied in this work.Using density functional theory(DFT) and time-dependent density functional theory(TDDFT) method, the experimental electronic spectra can be reproduced for 1-enol compound. We first verify the formation of dual intramolecular hydrogen bonds, and then confirm that the dual hydrogen bond should be strengthened in the first excited state. The photo-excitation process is analyzed by using frontier molecular orbital(HOMO and LUMO) for 1-enol compound. The obvious intramolecular charge transfer(ICT) provides the driving force to effectively facilitate the ESIPT process in the S1 state. Exploration of the constructed S0-state and S1-state potential energy surface(PES) reveals that only the excited state intramolecular single proton transfer occurs for 1-enol system, which makes up for the deficiencies in previous experiment.展开更多
The excited state intramolecular proton transfer of four derivatives(FM, BFM, BFBC, CCM) of 3-hydroxychromone is investigated.The geometries of different substituents are optimized to study the substituent effects on ...The excited state intramolecular proton transfer of four derivatives(FM, BFM, BFBC, CCM) of 3-hydroxychromone is investigated.The geometries of different substituents are optimized to study the substituent effects on proton transfer.The mechanism of hydrogen bond enhancement is qualitatively elucidated by comparing the infrared spectra, the reduced density gradient, and the frontier molecular orbitals.The calculated electronic spectra are consistent with the experimental results.To quantify the proton transfer, the potential energy curves(PECs) of the four derivatives in S0 and S1 states are scanned.It is concluded that the ability of proton transfer follows the order: FM > BFM > BFBC > CCM.展开更多
Undoped and Eu3+-doped Sr2CeO4 luminescent materials were prepared by sol-gel method. The structure and uncommon photoluminescence of Sr2CeO4∶Eu3+ phosphors were investigated in detail by powder X-ray diffraction (XR...Undoped and Eu3+-doped Sr2CeO4 luminescent materials were prepared by sol-gel method. The structure and uncommon photoluminescence of Sr2CeO4∶Eu3+ phosphors were investigated in detail by powder X-ray diffraction (XRD), Raman spectrum, and photoluminescence spectrum, respectively. The XRD results demonstrate that the as-prepared Sr2CeO4 phosphor is single phase and well crystallized. For Sr2CeO4∶Eu3+ phosphor, its excitation spectrum consists of a broad intense band from host and Eu3+-O2-charge transfer and a number of small peaks from Eu3+ ion. The broad emission band originated from Sr2CeO4 host and Eu3+ emission lines in the blue, green, and red regions coexist. Not only the characteristic transition lines from the lowest excited 5D0 level of Eu3+ but also those from higher energy levels 5DJ (J=1, 2) of Eu3+ ions are observed. These unusual luminescence properties result from the low vibration energy of Sr2CeO4 host-lattice and different energy transfer process from host to activator.展开更多
Dynamic nonlinearities of C 70 /toluene solution are measured and analysed by an improved picosecond time-resolved pump-probe system based on a nonlinear imaging technique with phase object.The photophysical parameter...Dynamic nonlinearities of C 70 /toluene solution are measured and analysed by an improved picosecond time-resolved pump-probe system based on a nonlinear imaging technique with phase object.The photophysical parameters are determined by the five-level model,which is adopted to interpret the experimental data.The change of refraction index per unit density of the excited state obtained by a numerically simulation is a critical factor to determine the nonlinear behaviour of C 70 in picosecond time regime.展开更多
Organic optoelectronics is an emerging research field, which has attracted extensive interests in the last few decades owing to its practical applications, like organic light-emitting diodes (OLEDs), organic memory de...Organic optoelectronics is an emerging research field, which has attracted extensive interests in the last few decades owing to its practical applications, like organic light-emitting diodes (OLEDs), organic memory devices, organic photovoltaic (OPV), sensors, and organic field-effect transistors[1, 2]. Organic semiconductors play a crucial role in this field. Compared to the traditional inorganic semiconductors, organic semiconductors open a fascinating research direction because of some unique advantages, such as flexible design, low cost, and rich optical and electronic properties. In organic optoelectronics, the excited states greatly determine the photoelectronic properties and application areas as shown in Fig. 1. Based on the electron spin in the molecule, the excited states of organic semiconductors include singlet and triplet states. As we know, the radiative transitions of singlet and triplet excited states are always accompanied by fluorescence and phosphorescence emission, respectively.展开更多
基金supported by the National Natural Science Foundation of China(Nos.12175100 and 11975132)the Construct Program of the Key Discipline in Hunan Province,the Research Foundation of Education Bureau of Hunan Province,China(No.18A237)+1 种基金the Natural Science Foundation of Hunan Province,China(No.2018JJ2321)the Innovation Group of Nuclear and Particle Physics in USC,the Opening Project of Cooperative Innovation Center for Nuclear Fuel Cycle Technology and Equipment,University of South China(No.2019KFZ10).
文摘In the present work,we extend the Coulomb and Proximity Potential Model(CPPM)to study two-proton(2p)radioactivity from excited states while the proximity potential is chosen as AW95 proposed by Aage Withner in 1995.Demonstration reveals that the theoretical results acquired by CPPM exhibit a high level of consistency with prior theoretical models such as the unified fission model(UFM),generalized liquid-drop model(GLDM)and effective liquid-drop model(ELDM).Furthermore,within the CPPM,we predicted the half-lives of potential 2p radioactive nuclei for which experimental data are currently unavailable.The predicted results were then assessed,compared with UFM,ELDM and GLDM models,and examined in detail.
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 12274294 and 12075036)。
文摘We theoretically investigate high-order harmonic generation(HHG) of helium(He), lithium cation(Li+), and beryllium dication(Be2+) using the time-dependent Hartree–Fock method to solve the three-dimensional time-dependent Schr ¨odinger equation. It is found that the intensity of the HHG increases significantly from a certain harmonic order below the ionization threshold, and the initial position of the enhancement does not depend on the intensity or the wavelength of the driving laser field. Further analysis shows that excited states play an important role on this enhancement,consistent with the excited-state tunneling mechanism [Phys. Rev. Lett. 116 123901(2016)]. Our results unambiguously show that excited-state tunneling is essential for understanding the enhancement of HHG. Accordingly, a four-step model is herein proposed to illustrate the multiphoton excitation effect in helium-like ions, which enriches the physics of HHG enhancement.
文摘Investigating the impact of microhydration on the excited-states and electronic excitation properties of biomolecules has remained one of the important yet challenging aspects of science because of the complexity of developing models. However, with the advent of computational chemistry methods such as TD-DFT, many useful insights about the electronic excitation energy and excited-state nature of biomolecules can be explored. Accordingly, in our study, we have incorporated the TD-DFT/wB97XD/cc-pVTZ method to study the excited state properties of N-acetyl phenylalanine amide (NAPA-A(H<sub>2</sub>O) <sub>n</sub>) (n = 1 to 4) clusters from ground to the tenth lowest gaseous singlet excited state. We found that the C=O bond length gradually increases both in N-terminal amide and C-terminal amide after the sequential addition of water molecules because of intermolecular H-bonding and this intermolecular H-bonding becomes weaker after the sequential addition of H<sub>2</sub>O molecules. The UV absorption maxima of NAPA-A (H<sub>2</sub>O)<sub>n</sub> (n = 1 - 4) clusters consisted of two peaks that are S<sub>5</sub>←S<sub>0</sub> (1<sup>st</sup> absorption) and S<sub>6</sub>←S<sub>0</sub> (2<sup>nd</sup> absorption) excitations. The first absorption maxima were blue-shifted with the increase in oscillator strength. This means that strong H-bonds reduce the charge transfer and make clusters more rigid. On the other hand, the second absorption maxima were red-shifted with the decrease in oscillator strength. In the ECD spectra, the negative bands indicate the presence of an amide bond and L-configuration of micro hydrated NAPA-A clusters. Finally, our calculated absorption and fluorescence energy confirm that all the NAPA-A (H<sub>2</sub>O) <sub>n</sub> (n = 0 - 4) clusters revert to the ground state from the fluorescent state by emitting around 5.490 eV of light.
基金supported by the National Natural Science Foundation of China(Nos.12175100 and 11975132)the Construct Program of the Key Discipline in Hunan Province+3 种基金the Research Foundation of the Education Bureau of Hunan Province,China(No.18A237)the Natural Science Foundation of Hunan Province,China(No.2018JJ2321)the Innovation Group of Nuclear and Particle Physics in USCthe Opening Project of the Cooperative Innovation Center for Nuclear Fuel Cycle Technology and Equipment,University of South China(No.2019KFZ10)。
文摘In this study,we systematically investigated the two-proton(2p)radioactivity half-lives from the excited state of nuclei near the proton drip line within the Gamowlike model(GLM)and modified Gamow-like model(MGLM).The calculated results were highly consistent with the theoretical values obtained using the unified fission model[Chin.Phys.C 45,124105(2021)],effective liquid drop model,and generalized liquid drop model[Acta Phys.Sin 71,062301(2022)].Furthermore,utilizing the GLM and MGLM,we predicted the 2p radioactivity halflives from the excited state for some nuclei that are not yet available experimentally.Simultaneously,by analyzing the calculated results from these theoretical models,it was found that the half-lives are strongly dependent on Qand l.
文摘In this paper, we have declined the formalism of the method of the Modified Atomic Orbital Theory (MAOT) applied to the calculations of energies of doubly excited states 2<em>snp</em>, 3<em>snp</em>, and 4<em>snp</em> Helium-like systems. Then we also applied the variational procedure of the Modified Atomic Orbital Theory to the computations of total energies, excitation energies of doubly-excited states 2<em>snp</em>, 3<em>snp</em>, 4<em>snp</em> types of Helium-like systems. The results obtained in this work are in good agreement with the experimental and theoretical values available.
基金the National Nature Science Foundation of China(No.11674101,No.21873030 and No.91850202)。
文摘As one of the biological endogenous pigments,biliverdin(BV)and its dimethyl ester(BVE)have extremely weak uorescence in solution with quantum yield less than 0.01%.However,the situation reverses with the addition of zinc ions.The strength for uorescence of BVE-Zn^2+ complex is greatly enhanced and uorescence quantum yield can increase to5%.Herein,we studied ultrafast excited state dynamics of BVE-Zn^2+ complex in ethanol,npropanol,and DMSO solutions in order to reveal the mechanism of uorescence quantum yield enhancement.The results show that BVE can form a stable coordination complex with zinc with 1:1 stoichiometry in solution.BVE is structurally and energetically more stable in the complex.Using picosecond time-resolve uorescence and femtosecond transient absorption spectroscopy,we show that smaller non-radiative rate constant of BVE-Zn^2+ complex in DMSO is the key to increasing its uorescence quantum yield and the excited state decay mechanism is also revealed.These results provide valuable information about the uorescence property change after BVE binding to metal ions and may provide a guidance for the study of phytochromes or other uorescence proteins in which BV/BVE acts as chromophores.
基金the national key project for fundamental research.
文摘A four-level decay model of 6P7/2 excited state of Eu(2+ ion in KMgF3: Eu2+ has been proposed. The decay profiles of the 6P7/2 excited state of Eu2+ are two exponential and the physical implication of each term in the fit equation responsible for the model is interpreted. The data obtained spectroscopically are in good agreement with the fit results.
基金Supported by the National Natural Science Foundation of China under Grant Nos 21303255,21273274 and 91121006
文摘Two-photon absorption in systems with parity permits access to states that cannot be directly prepared by onephoton absorption. Here we investigate ultrafast internal conversion(IC) dynamics of furan by using this strategy in combination with femtosecond time-resolved photoelectron imaging. The dark Rydberg S_1 and bright valence S_2 states are simultaneously excited by two photons of 405 nm, and then ionized by two photons of 800 nm. The IC from S_2 to S_1 is clearly observed and extracted from the time dependence of the higher photoelectron kinetic energy(PKE) component. More importantly, the internal conversions to hot S_0 from directly-prepared S_1 and secondarily-populated S_1 are unambiguously identified by the time-dependence of the lower PKE component.The average lifetime of the S_2 and S_1 states is measured to be 29 fs. The internal conversions of S_2 to S_1, S_1 to hot S_0 occur on estimated timescales of 15.4 fs and 38 fs, respectively.
文摘In this work, the total energies of doubly excited states (<em>ns</em><sup>2</sup>) <sup>1</sup>S<sup>e</sup>, (<em>np</em><sup>2</sup>) <sup>1</sup>D<sup>e</sup>, (<em>nd</em><sup>2</sup>) <sup>1</sup>G<sup>e</sup>, (<em>nf</em><sup>2</sup>) <sup>1</sup>I<sup>e</sup>, (<em>ng</em><sup>2</sup>) <sup>1</sup>K<sup>e</sup>, and (<em>nh</em><sup>2</sup>) <sup>1</sup>M<sup>e</sup> of the helium isoelectronic sequence with Z ≤ 10 are calculated in the framework of the variational method of the Screening Constant by Unit Nuclear Charge (SCUNC). These calculations are performed using a new wavefunction correlated to Hylleraas-type. The possibility of using the SCUNC method in the investigation of high-lying Doubly Excited States(DES) in two-electron systems is demonstrated in the present work in the case of the (<em>nl</em><sup>2</sup>) <sup>1</sup><em>L</em><sup><span style="white-space:nowrap;"><span style="white-space:nowrap;"><span style="white-space:nowrap;"><em>π</em></span></span></span></sup> doubly excited states, where accurate total energies are tabulated up to <em>n</em> = 20. All the results obtained in this paper are in agreement with the values of the available literature and may be useful for future experimental and theoretical studies on the doubly excited (<em>nl</em><sup>2</sup>) <sup>1</sup><em>L</em><sup><span style="white-space:nowrap;"><span style="white-space:nowrap;"><em>π</em></span></span></sup> states of two-electron systems.
文摘The newly discovered neutron halos in the excited states of nuclei 12B, 13C, and 209pb are studied by therelativistic mean-field theory. The calculated binding energies are very close to the experimental ones. The experimentally extracted root-mean-square radii of the last neutron with different occupations in nuclei are well reproduced bycalculations. New candidates for the neutron halos in excited states are predicted and are useful for further search ofneutron halos in the excited states of stable nuclei.
基金V. ACKNOWLEDGMENTS This work is supported by the National Natural Science Foundation of China （No.10674002 and No.20973001） and the Science Foundation of Anhui Education Committee （No.ZD2007001-1）.
基金Project supported by the National Natural Science Foundation of China(Grant Nos 10474029 and 10774063)
文摘Based on the obtained energy values of 1s 2 n p (n ≤ 9) states for lithium-like systems from Z =11 to 20 (by the authors of this paper:Hu M H and Wang Z W 2004 Chin.Phys.13 662),this paper determines the quantum defects,as slowly varying function of energy,of this Rydberg series.Using them as input,it can predict the energies of any highly excited states below the ionization threshold for this series according to the quantum defect theory.The regularities of variation for quantum defects of the series along this isoelectronic sequence are physically analysed and discussed.The screening parameters,which are equal to the effective screening charge of the core-electrons,are also obtained.
基金Supported by the Fundamental Research Funds for the Central Universities (No.2012QN066,2011QN142)
文摘Excited-state hydrogen-bonding dynamics of N-methylformamide (NMF) in water has been investigated by time-dependent density functional theory (TDDFT) method. The ground-state geometry optimizations were calculated by density functional theory (DFT) method, while the electronic transition energies and corresponding oscillation strengths of the low-lying electronically excited states of isolated NMF, water monomers and the hydrogen-bonded NMF-H 2 O were calculated by TDDFT method. According to Zhao's rule on the excited-state hydrogen bonding dynamics, our results demonstrate that the intermolecular hydrogen bond C=O···O-H is strengthened and weakened in different electronically excited states. The hydrogen bond strengthening and weakening in the electronically excited state plays an important role in the photophysics of NMF in solutions.
基金Project supported by the National Natural Science Foundation of China(Grant No.11464033)
文摘With hydrogen-like impurity(HLI) located in the center of Cs I quantum pseudodot(QPD) and by using the variational method of Pekar type(VMPT), we investigate the first-excited state energy(FESE), excitation energy and transition frequency of the strongly-coupled bound polaron in the present paper. Temperature effects on bound polaron properties are calculated by employing the quantum statistical theory(QST). According to the present work's numerical results, the FESE, excitation energy and transition frequency decay(amplify) with raising temperature in the regime of lower(higher)temperature. They are decreasing functions of Coulomb impurity potential strength.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.91026021,11075068,10875054,11175076,and 10975065)the Fundamental Research Funds of the Central Universities of China(Grant No.lzujbky-2010-k08)
文摘We theoretically investigate the contribution of the excited state to the ellipticity of the harmonics from H+2 at different orientation angles irradiated by a linearly polarized laser pulse. It is found that the first excited state has a significant influence to the ellipticity of the harmonics, and the contribution of higher excited states to the ellipticity can be neglected.Moreover, the conclusion is not dependent on the laser intensity.
基金Project supported by the National Natural Science Foundation of China(Grant No.11404112)the Funding Scheme for Young Teachers in Colleges and Universities in Henan Province,China(Grant No.2017GGJS077)the Key Scientific Research Project of Colleges and Universities of Henan Province,China(Grant No.18A140023)
文摘Owing to the importance of excited state dynamical relaxation, the excited state intramolecular proton transfer(ESIPT) mechanism for a novel compound containing dual hydrogen bond(abbreviated as "1-enol") is studied in this work.Using density functional theory(DFT) and time-dependent density functional theory(TDDFT) method, the experimental electronic spectra can be reproduced for 1-enol compound. We first verify the formation of dual intramolecular hydrogen bonds, and then confirm that the dual hydrogen bond should be strengthened in the first excited state. The photo-excitation process is analyzed by using frontier molecular orbital(HOMO and LUMO) for 1-enol compound. The obvious intramolecular charge transfer(ICT) provides the driving force to effectively facilitate the ESIPT process in the S1 state. Exploration of the constructed S0-state and S1-state potential energy surface(PES) reveals that only the excited state intramolecular single proton transfer occurs for 1-enol system, which makes up for the deficiencies in previous experiment.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11874241,11847224,and 11804195)the Shandong Province Higher Educational Science and Technology Program,China(Grant No.J15LJ03)+1 种基金the Taishan Scholar Project of Shandong Province,China,China Post-Doctoral Foundation(Grant No.2018M630796)the Natural Science Foundation of Shandong Province,China(Grant No.ZR2018BA034)
文摘The excited state intramolecular proton transfer of four derivatives(FM, BFM, BFBC, CCM) of 3-hydroxychromone is investigated.The geometries of different substituents are optimized to study the substituent effects on proton transfer.The mechanism of hydrogen bond enhancement is qualitatively elucidated by comparing the infrared spectra, the reduced density gradient, and the frontier molecular orbitals.The calculated electronic spectra are consistent with the experimental results.To quantify the proton transfer, the potential energy curves(PECs) of the four derivatives in S0 and S1 states are scanned.It is concluded that the ability of proton transfer follows the order: FM > BFM > BFBC > CCM.
基金Project supported bythe JSTUFoundation of Science Research (KYY05039)
文摘Undoped and Eu3+-doped Sr2CeO4 luminescent materials were prepared by sol-gel method. The structure and uncommon photoluminescence of Sr2CeO4∶Eu3+ phosphors were investigated in detail by powder X-ray diffraction (XRD), Raman spectrum, and photoluminescence spectrum, respectively. The XRD results demonstrate that the as-prepared Sr2CeO4 phosphor is single phase and well crystallized. For Sr2CeO4∶Eu3+ phosphor, its excitation spectrum consists of a broad intense band from host and Eu3+-O2-charge transfer and a number of small peaks from Eu3+ ion. The broad emission band originated from Sr2CeO4 host and Eu3+ emission lines in the blue, green, and red regions coexist. Not only the characteristic transition lines from the lowest excited 5D0 level of Eu3+ but also those from higher energy levels 5DJ (J=1, 2) of Eu3+ ions are observed. These unusual luminescence properties result from the low vibration energy of Sr2CeO4 host-lattice and different energy transfer process from host to activator.
基金Project supported by the National Natural Science Fundation of China(Grant No.90922007)
文摘Dynamic nonlinearities of C 70 /toluene solution are measured and analysed by an improved picosecond time-resolved pump-probe system based on a nonlinear imaging technique with phase object.The photophysical parameters are determined by the five-level model,which is adopted to interpret the experimental data.The change of refraction index per unit density of the excited state obtained by a numerically simulation is a critical factor to determine the nonlinear behaviour of C 70 in picosecond time regime.
基金supported by the National Funds for Distinguished Young Scientists(No.61825503)China Postdoctoral Science Foundation Funded Project(No.2018M642282)+1 种基金Natural Science Foundation of Jiangsu Province of China(No.BK20180760)Jiangsu Planned Projects for Postdoctoral Research Funds(No.2018K155C)
文摘Organic optoelectronics is an emerging research field, which has attracted extensive interests in the last few decades owing to its practical applications, like organic light-emitting diodes (OLEDs), organic memory devices, organic photovoltaic (OPV), sensors, and organic field-effect transistors[1, 2]. Organic semiconductors play a crucial role in this field. Compared to the traditional inorganic semiconductors, organic semiconductors open a fascinating research direction because of some unique advantages, such as flexible design, low cost, and rich optical and electronic properties. In organic optoelectronics, the excited states greatly determine the photoelectronic properties and application areas as shown in Fig. 1. Based on the electron spin in the molecule, the excited states of organic semiconductors include singlet and triplet states. As we know, the radiative transitions of singlet and triplet excited states are always accompanied by fluorescence and phosphorescence emission, respectively.
