Circularly polarized luminescence(CPL)and two-photon absorption(TPA)materials have garnered considerable attentions due to their minimal energy loss and superior optical penetration[1,2].However,the current challenge ...Circularly polarized luminescence(CPL)and two-photon absorption(TPA)materials have garnered considerable attentions due to their minimal energy loss and superior optical penetration[1,2].However,the current challenge lies in the absence of well-developed strategies for designing materials that combine these two exceptional optical properties.展开更多
In recent years,S-scheme heterojunctions have garnered significant attention,with their carrier trans-fer mechanism primarily understood as the recombination of less reactive photogenerated carriers while preserving t...In recent years,S-scheme heterojunctions have garnered significant attention,with their carrier trans-fer mechanism primarily understood as the recombination of less reactive photogenerated carriers while preserving the highly reactive ones.However,the detailed interfacial electron transfer process can vary slightly among different S-scheme heterojunctions.Here we design a well-structured S-scheme covalent organic framework(COF)/TiO_(2) heterojunction to explore its microscopic interfacial electron transfer pro-cesses.Notably,we identify a cross-interface secondary electron pumping phenomenon within the S-scheme heterojunction,leading to the formation of high-energy anti-Kasha excited states.This discovery deepens our understanding of the S-scheme charge transfer mechanism and suggests that the redox ca-pabilities of S-scheme heterojunctions exceed traditional expectations.Our findings provide new insights into the origins of the high activity observed in S-scheme heterojunctions and enhance our understanding of their electron transfer processes.展开更多
We present a minimal theoretical model for self-sustained oscillations of a thin elastic sheet on a hot plate,induced by thermomechanical coupling.As the plate temperature increases,the sheet’s static deflection beco...We present a minimal theoretical model for self-sustained oscillations of a thin elastic sheet on a hot plate,induced by thermomechanical coupling.As the plate temperature increases,the sheet’s static deflection becomes unstable via a Hopf bifurcation at a critical temperature TC,giving rise to spontaneous periodic motion.Linear stability analysis yields analytical expressions for the critical oscillation temperature TC and the oscillation period at onset.Numerical simulations of the nonlinear equations confirm the bifurcation and reveal how key parameters(stiffness,thermal softening,thermal coupling,etc.)govern the oscillation amplitude and waveform.Finally,we demonstrate that the self-oscillating sheet can perform mechanical work as a heat engine,and we compare its performance to the Carnot efficiency limit.This work provides design principles for thermally driven selfoscillators with potential applications in soft robotics,adaptive structures,and thermal energy harvesting.展开更多
Carbazole-core multi-branched chromophores 9-ethyl- 3, 6-bis （ 2- { 4- [ 5- （4-tert-butyl-phenyl） - [ 1, 3, 4 ] oxadiazol-2-yl ] - phenyl }-vinyl） -carbazole（3） and 9-ethyl-3-（ 2- {4-[ 5-（4-tert-butyl- phenyl...Carbazole-core multi-branched chromophores 9-ethyl- 3, 6-bis （ 2- { 4- [ 5- （4-tert-butyl-phenyl） - [ 1, 3, 4 ] oxadiazol-2-yl ] - phenyl }-vinyl） -carbazole（3） and 9-ethyl-3-（ 2- {4-[ 5-（4-tert-butyl- phenyl） -[ 1, 3, 4 ] oxadiazol-2-yl ] -phenyl }-vinyl ） -carbazole （ 2 ） are synthesized through Wittig reaction and characterized by nuclear magnetic resonance（NMR）and infrared（IR）. The two- photon absorption properties of chromophores are investigated. These chromophores exhibit large two-photon absorption crosssections and strong blue two-photon excited fluorescence. The cooperative enhancement of two-photon absorption（TPA） in the multi-branched structures is observed. This enhancement is partly attributed to the electronic coupling between the branches. The electronic push-pull structures in the arm and their cooperative effects help the extended charge transfer for TPA.展开更多
Vicinal diamines are key motifs widely-found in many pharmaceuticals and biologically active molecules.An appealing approach for synthesizing these molecules is the amination of enamines,but few examples have been exp...Vicinal diamines are key motifs widely-found in many pharmaceuticals and biologically active molecules.An appealing approach for synthesizing these molecules is the amination of enamines,but few examples have been explored.With the utilization of nitrogen-centered radicals(NCRs),here we present the development of a dual bio-/photo-catalytic system for achieving enantioselective hydroamination of enamides,which can give easy access to diverse enantioenriched vicinal diamines.These reactions progress efficiently under green light excitation and exhibit excellent enantioselectivities(up to>99%enantiomeric excess).Mechanistic studies uncovered the synergistic effect of the enzyme and the externally added organophotoredox catalyst Rhodamine B(RhB).This work demonstrates the effectiveness of photobiocatalysis to generate and control high-energy radical intermediates,addressing a long-standing challenge in chemical synthesis.展开更多
Exploring advanced techniques capable of probing nanometric acoustic waves in nanostructures is critically important for the development of miniaturized acoustic devices.In this study,we probe the optically-excited ac...Exploring advanced techniques capable of probing nanometric acoustic waves in nanostructures is critically important for the development of miniaturized acoustic devices.In this study,we probe the optically-excited acoustic waves in a single silicon nanowire(NW)using the time-resolved(tr-)high-order Laue-zone(HOLZ)lines under convergent-beam electron diffraction(CBED)conditions in an ultrafast transmission electron microscope(UTEM).We devise an experimental scheme to obtain tr-HOLZ lines under off-zone-axis CBED conditions.We also propose a geometric description of HOLZ line formation and use this alternative description to quantitatively evaluate the dynamics of optically-excited silicon NW.Using part of the deformation gradient tensor,our simulations of the dynamics of Si NW reproduce the experimental results.We further discuss the feasibility of a full retrieval of the deformation gradient tensor by using a set of HOLZ lines from three zone axes.Our findings illustrate a strategy for the quantitative access to dynamical acoustic waves optically excited in micro-and nano-structures using UTEM.展开更多
Recently, the quantum description of electromagnetic waves in conducting media has been performed. It has been demonstrated that in particular case, the Hamiltonian of the corresponding field can be expressed by Caldi...Recently, the quantum description of electromagnetic waves in conducting media has been performed. It has been demonstrated that in particular case, the Hamiltonian of the corresponding field can be expressed by Caldirola–Kanai Hamiltonian. In this paper, using the associated annihilation and creation operators of the above-mentioned quantized field, the time-and conductivity-dependent squeezed vacuum and one-photon squeezed states as well as their superpositions, and also the time-and conductivity-dependent excited even and odd coherent states are produced. Also,using a few well-known nonclassicality criteria, the time evolution of nonclassicality features of the above classes of obtained states, in addition to the influence of medium conductivity on them are demonstrated, numerically. It has been shown that the nonclassicality indicators may be adjusted by tuning the conductivity of media.展开更多
The electronic structure of methanol/TiO2（ll0） interface has been studied by photoemis- sion spectroscopy. The pronounced resonance which appears at 5.5 eV above the Fermi level in two-photon photoemission spectrosc...The electronic structure of methanol/TiO2（ll0） interface has been studied by photoemis- sion spectroscopy. The pronounced resonance which appears at 5.5 eV above the Fermi level in two-photon photoemission spectroscopy （2PPE） is associated with the photocatalyzed dissociation of methanol at fivefold coordinated Ti sites （Ti5c） on TiO2 （110） surface [Chem- ical Science 1, 575 （2010）]. To check whether this resonance signal arises from initial or intermediate states, photon energy dependent 2PPE and comparison between one-photon photoemission spectroscopy and 2PPE have been performed. Both results consistently sug- gest the resonance signal originates from the initially unoccupied intermediate states, i.e., excited states. Dispersion measurements suggest the excited state is localized. Time-resolved studies show the lifetime of the excited state is 24 fs. This work presents comprehensive char- acterization of the excited states on methanol/TiO2（110） interface, and provides elaborate experimental data for the development of theoretical methods in reproducing the excited states on TiO2 surfaces and interfaces.展开更多
A surface femtosecond two-photon photoemission （2PPE） spectrometer devoted to the study of ultrafast excited electron dynamics and photochemical kinetics on metal and metal oxide surfaces has been constructed. Low e...A surface femtosecond two-photon photoemission （2PPE） spectrometer devoted to the study of ultrafast excited electron dynamics and photochemical kinetics on metal and metal oxide surfaces has been constructed. Low energy photoelectrons are measured using a hemispherical electron energy analyzer with an imaging detector that allows us to detect the energy and the angular distributions of the photoelectrons simultaneously. A Mach-Zehnder interferom- eter was built for the time-resolved 2PPE （TR-2PPE） measurement to study ultrafast surface excited electron dynamics, which was demonstrated on the Cu（111） surface. A scheme for measuring time-dependent 2PPE （TD-2PPE） spectra has also been developed for studies of surface photochemistry. This technique has been applied to a preliminary study on the photochemical kinetics on ethanol/TiO2（110）. We have also shown that the ultrafast dynamics of photoinduced surface excited resonances can be investigated in a reliable way by combining the TR-2PPE and TD-2PPE techniques.展开更多
The excited state intramolecular proton transfer （ESIPT） coupled charge transfer of baicalein has been investigated using steady-state spectroscopic experiment and quantum chemistry calculations. The absence of the ...The excited state intramolecular proton transfer （ESIPT） coupled charge transfer of baicalein has been investigated using steady-state spectroscopic experiment and quantum chemistry calculations. The absence of the absorption peak from S1 excited state both in the experi-mental and calculated absorption spectra indicates that S1 is a dark state. The dark excited state S1 results in the very weak fluorescence of solid baicalein in the experiment. The fron- tier molecular orbital and the charge difference densities of baicalein show clearly that the S1 state is a charge-transfer state whereas the S2 state is a locally excited state. The only one stationary point on the potential energy profile of excited state suggests that the ESIPT reaction of baicalein is a barrierless process.展开更多
Herein we have employed high-level multi-reference CASSCF and MS-CASPT2 electronic structure methods to systematically study the photochemical mechanism of intramolecularly hydrogen-bonded 2-（2＇-hydroxyphenyl）-4-me...Herein we have employed high-level multi-reference CASSCF and MS-CASPT2 electronic structure methods to systematically study the photochemical mechanism of intramolecularly hydrogen-bonded 2-（2＇-hydroxyphenyl）-4-methyloxazole. At the CASSCF level, we have optimized minima, conical intersections, minimum-energy reaction paths relevant to the excited-state intramolecular proton transfer （ESIPT）, rotation, photoisomerization, and the excited-state deactivation pathways. The energies of all structures and paths are refined by the MS-CASPT2 method. On the basis of the present results, we found that the ESIPT process in a conformer with the OH... N hydrogen bond is essentially barrierless process; whereas, the ESIPT process is inhibited in the other conformer with the OH... O hydrogen bond. The central single-bond rotation of the S1 enol species is energetically unfavorable due to a large barrier. In addition, the excited-state deactivation of the S1 keto species, as a result of the ultrafast ESIPT, is very efficient because of the existence of two easily-approached keto S1/S0 conical intersections. In stark contrast to the S1 keto species, the decay of the S1 enol species is almostly blocked. The present theoretical study contributes valuable knowledge to the understanding of photochemistry of similar intramolecularly hydrogen-bonded molecular and biological systems.展开更多
This paper considers the dynamical behavior of a Duffing-Mathieu type system with a cubic single-well potential during the principal parametric resonance. Both the cases of constant and time-dependent excitation ampli...This paper considers the dynamical behavior of a Duffing-Mathieu type system with a cubic single-well potential during the principal parametric resonance. Both the cases of constant and time-dependent excitation amplitude are used to observe the variation of the extent and the rate of the erosion in safe basins. It is evident that the appearance of fractal basin boundaries heralds the onset of the losing of structural integrity. The minimum value of control parameter to prevent the basin from erosion is given along with the excitation amplitude varying. The results show the time-dependence of excitation amplitude can be used to control the extent and the rate of the erosion and delay the first occurrence of heteroclinic tangency.展开更多
We study the H＋CH4/CD4-＋H2/HD＋CH3/CD3 reactions using the time sliced velocity map ion imaging technique. Ion images of the CH3/CD3 products were measured by the （2＋1） resonance enhanced multi-photon ionization ...We study the H＋CH4/CD4-＋H2/HD＋CH3/CD3 reactions using the time sliced velocity map ion imaging technique. Ion images of the CH3/CD3 products were measured by the （2＋1） resonance enhanced multi-photon ionization （REMPI） detection method. Besides the CH3/CD3 products in the ground state, ion images of the vibrationally excited CH3/CD3 products were also observed at two collision energies of 0.72 and 1.06 eV. It is shown that the angular distribution of the products CH3/CD3 in vibrationally excited states gradually vary from backward scattering to sideways scattering as the collision energy increases. Compared to the CH3/CD3 products in the ground state, the CH3/CD3 products in vibrationally excited states tend to be more sideways scattered, indicating that larger impact parameters play a more important role in the vibrationally excited product channels.展开更多
Geometry and vibrational frequencies of the ground state of Si2O2 molecule are studied using density function theory （DFT） at the level of cc-pvtz and 6-311-k＋G^＊＊. It is found that the optimizing value by B31yp/...Geometry and vibrational frequencies of the ground state of Si2O2 molecule are studied using density function theory （DFT） at the level of cc-pvtz and 6-311-k＋G^＊＊. It is found that the optimizing value by B31yp/cc-pvtz is closer to the experimental data. The excited properties under different external electric fields are also investigated by the time-dependent-DFT method. Transitions from the ground state of Si2O2 molecule to the first singlet state under different external electric fields can take place more easily. The corresponding absorption spectral line is about 360 nm in wavelength and the excitation energy is about 3.4 eV.展开更多
This paper investigates the excited states of Si3O molecule by using the single-excitation configuration interaction and density functional theory. It finds that the visible light absorption spectrum of Si3O molecule ...This paper investigates the excited states of Si3O molecule by using the single-excitation configuration interaction and density functional theory. It finds that the visible light absorption spectrum of Si3O molecule comprises the yellow and the purple light without external electric field, however all the visible light is included except the green light under the action of external electric field. Oxygen-deficient defects, which also can be found in Si3O molecule, have been used to explain the 1 from silicon-based materials but the microstructures of the materials are still uncertain Our results accord with the experimental values perfectly, this fact suggests that the structure of Si3O molecule is expected to be one of the main basic structures of the materials, so the oxygen-deficient defect structural model for Si3O molecule also has been provided to research the structures of materials.展开更多
Based on the obtained energy values of 1s^2np （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...Based on the obtained energy values of 1s^2np （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 a^cording 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
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
Nonlinear behaviors are investigated for a structure coupled with a nonlinear energy sink. The structure is linear and subject to a harmonic excitation, modeled as a forced single-degree-of-freedom oscillator. The non...Nonlinear behaviors are investigated for a structure coupled with a nonlinear energy sink. The structure is linear and subject to a harmonic excitation, modeled as a forced single-degree-of-freedom oscillator. The nonlinear energy sink is modeled as an oscillator consisting of a mass,a nonlinear spring, and a linear damper. Based on the numerical solutions, global bifurcation diagrams are presented to reveal the coexistence of periodic and chaotic motions for varying nonlinear energy sink mass and stiffness. Chaos is numerically identified via phase trajectories, power spectra,and Poincaré maps. Amplitude-frequency response curves are predicted by the method of harmonic balance for periodic steady-state responses. Their stabilities are analyzed.The Hopf bifurcation and the saddle-node bifurcation are determined. The investigation demonstrates that a nonlinear energy sink may create dynamic complexity.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
The parametric excited vibration of a pipe under thermal loading may occur because the fluid is often transported heatedly. The effects of thermal loading on the pipe stability and local bifurcations have rarely been ...The parametric excited vibration of a pipe under thermal loading may occur because the fluid is often transported heatedly. The effects of thermal loading on the pipe stability and local bifurcations have rarely been studied. The stability and the local bifurcations of the lateral parametric resonance of the pipe induced by the pulsating fluid velocity and the thermal loading are studied. A mathematical model for a simply supported pipe is developed according to the Hamilton principle. Two partial differential equations describing the lateral and longitudinal vibration are obtained. The singularity theory is utilized to anMyze the stability and the bifurcation of the system solutions. The transition sets and the bifurcation diagrams are obtained both in the unfolding parameter space and the physical parameter space, which can reveal the relationship between the thermal field parameter and the dynamic behaviors of the pipe. The frequency response and the relationship between the critical thermal rate and the pulsating fluid velocity are obtained. The numerical results demonstrate the accuracy of the single-mode expansion of the solution and the stability and local bifurcation analyses. It also confirms the existence of the chaos. The presented work can provide valuable information for the design of the pipeline and the controllers to prevent the structural instability.展开更多
基金supported by NSFC(22271282)the Self-deployment Project Research Program of Haixi Institutes,Chinese Academy of Sciences with the grant number of CXZX-2022-JQ04.
文摘Circularly polarized luminescence(CPL)and two-photon absorption(TPA)materials have garnered considerable attentions due to their minimal energy loss and superior optical penetration[1,2].However,the current challenge lies in the absence of well-developed strategies for designing materials that combine these two exceptional optical properties.
基金financially supported by the National Key Re-search and Development Program of China(No.2022YFB3803600)the National Natural Science Foundation of China(Nos.22202187,22361142704,22238009,U24A2071,and 22411540244)+3 种基金the National Postdoctoral Program for Innovative Talents(No.BX2021275)the Natural Science Foundation of Hubei Province of China(No.2022CFA001)the Project funded by China Postdoctoral Science Foundation(No.2022M712957)the Postdoctoral Funding Program of Hubei Province.
文摘In recent years,S-scheme heterojunctions have garnered significant attention,with their carrier trans-fer mechanism primarily understood as the recombination of less reactive photogenerated carriers while preserving the highly reactive ones.However,the detailed interfacial electron transfer process can vary slightly among different S-scheme heterojunctions.Here we design a well-structured S-scheme covalent organic framework(COF)/TiO_(2) heterojunction to explore its microscopic interfacial electron transfer pro-cesses.Notably,we identify a cross-interface secondary electron pumping phenomenon within the S-scheme heterojunction,leading to the formation of high-energy anti-Kasha excited states.This discovery deepens our understanding of the S-scheme charge transfer mechanism and suggests that the redox ca-pabilities of S-scheme heterojunctions exceed traditional expectations.Our findings provide new insights into the origins of the high activity observed in S-scheme heterojunctions and enhance our understanding of their electron transfer processes.
基金supported by the Guangdong Basic and Applied Basic Research Foundation(Grant Nos.2025B1515020077 and 2024A15150301-39)the National Natural Science Foundation of China(Grant No.12205138)the Shenzhen Science and Technology Innovation Committee(Grant No.JCYJ2022-0530113206015).
文摘We present a minimal theoretical model for self-sustained oscillations of a thin elastic sheet on a hot plate,induced by thermomechanical coupling.As the plate temperature increases,the sheet’s static deflection becomes unstable via a Hopf bifurcation at a critical temperature TC,giving rise to spontaneous periodic motion.Linear stability analysis yields analytical expressions for the critical oscillation temperature TC and the oscillation period at onset.Numerical simulations of the nonlinear equations confirm the bifurcation and reveal how key parameters(stiffness,thermal softening,thermal coupling,etc.)govern the oscillation amplitude and waveform.Finally,we demonstrate that the self-oscillating sheet can perform mechanical work as a heat engine,and we compare its performance to the Carnot efficiency limit.This work provides design principles for thermally driven selfoscillators with potential applications in soft robotics,adaptive structures,and thermal energy harvesting.
基金The National Natural Science Foundation of China(No.60678042)the Natural Science Foundation of Jiangsu Province(No.BK2006553)the Pre-Research Project of the National Natural Science Foundation supported by Southeast University(No.9207041399)
文摘Carbazole-core multi-branched chromophores 9-ethyl- 3, 6-bis （ 2- { 4- [ 5- （4-tert-butyl-phenyl） - [ 1, 3, 4 ] oxadiazol-2-yl ] - phenyl }-vinyl） -carbazole（3） and 9-ethyl-3-（ 2- {4-[ 5-（4-tert-butyl- phenyl） -[ 1, 3, 4 ] oxadiazol-2-yl ] -phenyl }-vinyl ） -carbazole （ 2 ） are synthesized through Wittig reaction and characterized by nuclear magnetic resonance（NMR）and infrared（IR）. The two- photon absorption properties of chromophores are investigated. These chromophores exhibit large two-photon absorption crosssections and strong blue two-photon excited fluorescence. The cooperative enhancement of two-photon absorption（TPA） in the multi-branched structures is observed. This enhancement is partly attributed to the electronic coupling between the branches. The electronic push-pull structures in the arm and their cooperative effects help the extended charge transfer for TPA.
文摘Vicinal diamines are key motifs widely-found in many pharmaceuticals and biologically active molecules.An appealing approach for synthesizing these molecules is the amination of enamines,but few examples have been explored.With the utilization of nitrogen-centered radicals(NCRs),here we present the development of a dual bio-/photo-catalytic system for achieving enantioselective hydroamination of enamides,which can give easy access to diverse enantioenriched vicinal diamines.These reactions progress efficiently under green light excitation and exhibit excellent enantioselectivities(up to>99%enantiomeric excess).Mechanistic studies uncovered the synergistic effect of the enzyme and the externally added organophotoredox catalyst Rhodamine B(RhB).This work demonstrates the effectiveness of photobiocatalysis to generate and control high-energy radical intermediates,addressing a long-standing challenge in chemical synthesis.
基金supported by the Guangxi Natural Science Foundation(Grant No.2024GXNSFDA010014)the National Natural Science Foundation of China(Grant Nos.12364018 and U22A6005)+1 种基金the Guangxi Science and Technology Major Program(Grant No.AA23073019)the Innovation Project of Guangxi Graduate Education(Grant Nos.YCBZ2022049 and YCBZ2023015)。
文摘Exploring advanced techniques capable of probing nanometric acoustic waves in nanostructures is critically important for the development of miniaturized acoustic devices.In this study,we probe the optically-excited acoustic waves in a single silicon nanowire(NW)using the time-resolved(tr-)high-order Laue-zone(HOLZ)lines under convergent-beam electron diffraction(CBED)conditions in an ultrafast transmission electron microscope(UTEM).We devise an experimental scheme to obtain tr-HOLZ lines under off-zone-axis CBED conditions.We also propose a geometric description of HOLZ line formation and use this alternative description to quantitatively evaluate the dynamics of optically-excited silicon NW.Using part of the deformation gradient tensor,our simulations of the dynamics of Si NW reproduce the experimental results.We further discuss the feasibility of a full retrieval of the deformation gradient tensor by using a set of HOLZ lines from three zone axes.Our findings illustrate a strategy for the quantitative access to dynamical acoustic waves optically excited in micro-and nano-structures using UTEM.
文摘Recently, the quantum description of electromagnetic waves in conducting media has been performed. It has been demonstrated that in particular case, the Hamiltonian of the corresponding field can be expressed by Caldirola–Kanai Hamiltonian. In this paper, using the associated annihilation and creation operators of the above-mentioned quantized field, the time-and conductivity-dependent squeezed vacuum and one-photon squeezed states as well as their superpositions, and also the time-and conductivity-dependent excited even and odd coherent states are produced. Also,using a few well-known nonclassicality criteria, the time evolution of nonclassicality features of the above classes of obtained states, in addition to the influence of medium conductivity on them are demonstrated, numerically. It has been shown that the nonclassicality indicators may be adjusted by tuning the conductivity of media.
文摘The electronic structure of methanol/TiO2（ll0） interface has been studied by photoemis- sion spectroscopy. The pronounced resonance which appears at 5.5 eV above the Fermi level in two-photon photoemission spectroscopy （2PPE） is associated with the photocatalyzed dissociation of methanol at fivefold coordinated Ti sites （Ti5c） on TiO2 （110） surface [Chem- ical Science 1, 575 （2010）]. To check whether this resonance signal arises from initial or intermediate states, photon energy dependent 2PPE and comparison between one-photon photoemission spectroscopy and 2PPE have been performed. Both results consistently sug- gest the resonance signal originates from the initially unoccupied intermediate states, i.e., excited states. Dispersion measurements suggest the excited state is localized. Time-resolved studies show the lifetime of the excited state is 24 fs. This work presents comprehensive char- acterization of the excited states on methanol/TiO2（110） interface, and provides elaborate experimental data for the development of theoretical methods in reproducing the excited states on TiO2 surfaces and interfaces.
文摘A surface femtosecond two-photon photoemission （2PPE） spectrometer devoted to the study of ultrafast excited electron dynamics and photochemical kinetics on metal and metal oxide surfaces has been constructed. Low energy photoelectrons are measured using a hemispherical electron energy analyzer with an imaging detector that allows us to detect the energy and the angular distributions of the photoelectrons simultaneously. A Mach-Zehnder interferom- eter was built for the time-resolved 2PPE （TR-2PPE） measurement to study ultrafast surface excited electron dynamics, which was demonstrated on the Cu（111） surface. A scheme for measuring time-dependent 2PPE （TD-2PPE） spectra has also been developed for studies of surface photochemistry. This technique has been applied to a preliminary study on the photochemical kinetics on ethanol/TiO2（110）. We have also shown that the ultrafast dynamics of photoinduced surface excited resonances can be investigated in a reliable way by combining the TR-2PPE and TD-2PPE techniques.
基金ACKNOWLEDGMENTS This work was supported by the National Natural Science Foundation of China （No.61137005 and No.10974023）, the Program for Liaoning Excellent Talents in University （No.LJQ2012002）, and the Program for New Century Excellent Talents in University （No.NCET-12-0077）.
文摘The excited state intramolecular proton transfer （ESIPT） coupled charge transfer of baicalein has been investigated using steady-state spectroscopic experiment and quantum chemistry calculations. The absence of the absorption peak from S1 excited state both in the experi-mental and calculated absorption spectra indicates that S1 is a dark state. The dark excited state S1 results in the very weak fluorescence of solid baicalein in the experiment. The fron- tier molecular orbital and the charge difference densities of baicalein show clearly that the S1 state is a charge-transfer state whereas the S2 state is a locally excited state. The only one stationary point on the potential energy profile of excited state suggests that the ESIPT reaction of baicalein is a barrierless process.
文摘Herein we have employed high-level multi-reference CASSCF and MS-CASPT2 electronic structure methods to systematically study the photochemical mechanism of intramolecularly hydrogen-bonded 2-（2＇-hydroxyphenyl）-4-methyloxazole. At the CASSCF level, we have optimized minima, conical intersections, minimum-energy reaction paths relevant to the excited-state intramolecular proton transfer （ESIPT）, rotation, photoisomerization, and the excited-state deactivation pathways. The energies of all structures and paths are refined by the MS-CASPT2 method. On the basis of the present results, we found that the ESIPT process in a conformer with the OH... N hydrogen bond is essentially barrierless process; whereas, the ESIPT process is inhibited in the other conformer with the OH... O hydrogen bond. The central single-bond rotation of the S1 enol species is energetically unfavorable due to a large barrier. In addition, the excited-state deactivation of the S1 keto species, as a result of the ultrafast ESIPT, is very efficient because of the existence of two easily-approached keto S1/S0 conical intersections. In stark contrast to the S1 keto species, the decay of the S1 enol species is almostly blocked. The present theoretical study contributes valuable knowledge to the understanding of photochemistry of similar intramolecularly hydrogen-bonded molecular and biological systems.
基金the National Science Foundation of ChinaPSF of China
文摘This paper considers the dynamical behavior of a Duffing-Mathieu type system with a cubic single-well potential during the principal parametric resonance. Both the cases of constant and time-dependent excitation amplitude are used to observe the variation of the extent and the rate of the erosion in safe basins. It is evident that the appearance of fractal basin boundaries heralds the onset of the losing of structural integrity. The minimum value of control parameter to prevent the basin from erosion is given along with the excitation amplitude varying. The results show the time-dependence of excitation amplitude can be used to control the extent and the rate of the erosion and delay the first occurrence of heteroclinic tangency.
文摘We study the H＋CH4/CD4-＋H2/HD＋CH3/CD3 reactions using the time sliced velocity map ion imaging technique. Ion images of the CH3/CD3 products were measured by the （2＋1） resonance enhanced multi-photon ionization （REMPI） detection method. Besides the CH3/CD3 products in the ground state, ion images of the vibrationally excited CH3/CD3 products were also observed at two collision energies of 0.72 and 1.06 eV. It is shown that the angular distribution of the products CH3/CD3 in vibrationally excited states gradually vary from backward scattering to sideways scattering as the collision energy increases. Compared to the CH3/CD3 products in the ground state, the CH3/CD3 products in vibrationally excited states tend to be more sideways scattered, indicating that larger impact parameters play a more important role in the vibrationally excited product channels.
基金Project supported by the National Natural Science Foundation of China (Grant No. 10774039)the Natural Science Foundation of Henan Province,China (Grant No. 092300410249)+1 种基金the Natural Science Foundation of the Education Bureau of Henan Province,China (Grant No. 2010A140008)the Foundation for University Young Core Instructors of Henan Province,China (Grant No. 2009GGJS-044)
文摘Geometry and vibrational frequencies of the ground state of Si2O2 molecule are studied using density function theory （DFT） at the level of cc-pvtz and 6-311-k＋G^＊＊. It is found that the optimizing value by B31yp/cc-pvtz is closer to the experimental data. The excited properties under different external electric fields are also investigated by the time-dependent-DFT method. Transitions from the ground state of Si2O2 molecule to the first singlet state under different external electric fields can take place more easily. The corresponding absorption spectral line is about 360 nm in wavelength and the excitation energy is about 3.4 eV.
基金Project supported by the Foundation for University Young Core Instructors of Henan Province,China(Grant No.2009GGJS-044)the Natural Science Foundation of the Education Bureau of Henan Province,China(Grant No.2010A140008)+1 种基金the Natural Science Foundation of Henan Province,China(Grant No.092300410249)the Natural Science Foundation of the Education Bureau of Henan Province,China(Grant No.2010A140008)
文摘This paper investigates the excited states of Si3O molecule by using the single-excitation configuration interaction and density functional theory. It finds that the visible light absorption spectrum of Si3O molecule comprises the yellow and the purple light without external electric field, however all the visible light is included except the green light under the action of external electric field. Oxygen-deficient defects, which also can be found in Si3O molecule, have been used to explain the 1 from silicon-based materials but the microstructures of the materials are still uncertain Our results accord with the experimental values perfectly, this fact suggests that the structure of Si3O molecule is expected to be one of the main basic structures of the materials, so the oxygen-deficient defect structural model for Si3O molecule also has been provided to research the structures of materials.
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^2np （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 a^cording 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 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.
基金supported by the National Natural Science Foundation of China (Grants 11402151 and 11572182)
文摘Nonlinear behaviors are investigated for a structure coupled with a nonlinear energy sink. The structure is linear and subject to a harmonic excitation, modeled as a forced single-degree-of-freedom oscillator. The nonlinear energy sink is modeled as an oscillator consisting of a mass,a nonlinear spring, and a linear damper. Based on the numerical solutions, global bifurcation diagrams are presented to reveal the coexistence of periodic and chaotic motions for varying nonlinear energy sink mass and stiffness. Chaos is numerically identified via phase trajectories, power spectra,and Poincaré maps. Amplitude-frequency response curves are predicted by the method of harmonic balance for periodic steady-state responses. Their stabilities are analyzed.The Hopf bifurcation and the saddle-node bifurcation are determined. The investigation demonstrates that a nonlinear energy sink may create dynamic complexity.
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Project supported by the National Natural Science Foundation of Shandong Province(No.ZR2013AL017)the National Natural Science Foundation of China(No.11272357)the Fundamental Research Funds for the Central Universities of China(No.11CX04049A)
文摘The parametric excited vibration of a pipe under thermal loading may occur because the fluid is often transported heatedly. The effects of thermal loading on the pipe stability and local bifurcations have rarely been studied. The stability and the local bifurcations of the lateral parametric resonance of the pipe induced by the pulsating fluid velocity and the thermal loading are studied. A mathematical model for a simply supported pipe is developed according to the Hamilton principle. Two partial differential equations describing the lateral and longitudinal vibration are obtained. The singularity theory is utilized to anMyze the stability and the bifurcation of the system solutions. The transition sets and the bifurcation diagrams are obtained both in the unfolding parameter space and the physical parameter space, which can reveal the relationship between the thermal field parameter and the dynamic behaviors of the pipe. The frequency response and the relationship between the critical thermal rate and the pulsating fluid velocity are obtained. The numerical results demonstrate the accuracy of the single-mode expansion of the solution and the stability and local bifurcation analyses. It also confirms the existence of the chaos. The presented work can provide valuable information for the design of the pipeline and the controllers to prevent the structural instability.
