The two-photon absorption induced lasing spectrum shows that the synthesized ASPBPh4, trans-4- [p- (N-methyl-N- (hydroxyethyl)amino) styryl]-N-methylpyridinium, has a distinct ef- ficiency of laser frequency up-conver...The two-photon absorption induced lasing spectrum shows that the synthesized ASPBPh4, trans-4- [p- (N-methyl-N- (hydroxyethyl)amino) styryl]-N-methylpyridinium, has a distinct ef- ficiency of laser frequency up-conversion. This nonlinear optical property of such a kind of com- pounds is related to two-photon absorption (TPA). In our work, we used the intermediate ne- glect of differential overlap (INDO) plus single-excitation configuration interaction (SCI) method to get the basic properties of the molecule, and calculated the second hyperpolarizability and the cross section of two-photon absorption by means of sum-over-state (SOS) expression. The rela- tionship between the structure and the properties is discussed.展开更多
The study of the linear and nonlinear optical properties of Zn Ge P2 based on density functional theory has been carried out. In order to get a more physical picture in the infrared region, terms which are considered ...The study of the linear and nonlinear optical properties of Zn Ge P2 based on density functional theory has been carried out. In order to get a more physical picture in the infrared region, terms which are considered as the phonon effect were added to the calculated refractive dispersion curves. The phonon-corrected calculation curves show excellent agreement with experimental refractive indexes, which gives a better comprehension of the linear optical proprieties in the transparent region. The static nonlinear optical susceptibility was investigated using approaches based on the ＂sum over states＂ and the2 n ＋ 1 theorem methods. Both of the results of these two methods reasonably coincided with the experimental results.展开更多
Polymeric membranes with diverse structures have attracted much attention as new materials for nonlinear optical devices. In this report, a novel oligomer of poly(aromatic ether sulfone)(OAES) has been synthesized and...Polymeric membranes with diverse structures have attracted much attention as new materials for nonlinear optical devices. In this report, a novel oligomer of poly(aromatic ether sulfone)(OAES) has been synthesized and characterized. The electronic structure as well as linear and nonlinear optical properties has been studied by density function theory. The effect for general nonlinear optical polarizability of various condition has been further researched such as absence of side chains and introduction of phenyl substituent on side chains. The static and frequency-dependent hyperpolarizabilities of OAES and its derivatives have been calculated. This work interprets an efficient adjustment for the frequency response and the intensity of nonlinear optical polarizability can be achieved by regulating the structure of system, which provides a new potential for the application of oligomeric materials on nonlinear optical field.展开更多
Based on the equilibrium structures from quantum mechanics AM1 method, employing INDO/CI method and the sum-over-state （SOS） formula, the one-photon absorption （OPA） and two-photon absorption （TPA） properties as...Based on the equilibrium structures from quantum mechanics AM1 method, employing INDO/CI method and the sum-over-state （SOS） formula, the one-photon absorption （OPA） and two-photon absorption （TPA） properties as well as the second hyperpolarizabilities were discussed in detail for a kind of PPV derivative poly 2-（9-phenylanthracen-10-yl）-1,4-phenylenevinylene （P1）. The results indicate that the two-photon cross section （3） increases with the increasing of the number of repeating segment （n）, however only a slight increase corresponds to the increasing of molecular weight when the repeating unit number arrives at a certain number. From this point of view, the TPA cross section values of P1 were extrapolated through the linear fit of 3 value vs. 1/n. The δ value of P1 is as high as 181 GM （1 GM=10^-50 cm^4·s·photon^-1）. Concerning the influence of pendent group and extension of π-conjugation on 3 values, another four oligomers P2, PPV, P1-1, and P2-1 were investigated for comparison. The calculation results reveal that the position and property of pendent group have great influence on the OPA and TPA properties. A most crucial role for relatively larger 3 value was played by the extension of π-conjugation.展开更多
The current study has obtained excellent potential nonlinear optical(NLO)materials by combining density functional theory methods with sum-over-states model to predict the second order NLO properties of helical graphe...The current study has obtained excellent potential nonlinear optical(NLO)materials by combining density functional theory methods with sum-over-states model to predict the second order NLO properties of helical graphene nanoribbons(HGNs)through introducing azulene defects or/and BN units.The introduction of these functional groups deforms the pristine HGN(compression or tension)and enhances obviously the static first hyperpolarizability(〈β0〉)of system by up to two orders of magnitude.The tensor components along the helical axis of HGNs play a dominant role in the total〈β0〉.The azulene defects and the BN units polarize the pristine HGN to different degrees,and the azulenes and contiguous benzenes are involved in the major electron excitations with significant contributions to〈β0〉but the BN units are not.The BN-doped chiral HGNs have good kinetic stability and strong second order NLO properties(6.84×10^(5)×10^(−30) esu),and can be a potential candidate of high-performance second order NLO materials.The predicted two-dimensional second order NLO spectra provide useful information for further exploration of those helicenes for electro-optic applications.展开更多
文摘The two-photon absorption induced lasing spectrum shows that the synthesized ASPBPh4, trans-4- [p- (N-methyl-N- (hydroxyethyl)amino) styryl]-N-methylpyridinium, has a distinct ef- ficiency of laser frequency up-conversion. This nonlinear optical property of such a kind of com- pounds is related to two-photon absorption (TPA). In our work, we used the intermediate ne- glect of differential overlap (INDO) plus single-excitation configuration interaction (SCI) method to get the basic properties of the molecule, and calculated the second hyperpolarizability and the cross section of two-photon absorption by means of sum-over-state (SOS) expression. The rela- tionship between the structure and the properties is discussed.
基金the National Natural Science Foundation of China，the Doctoral Scientific Research Staring Foundation of Zhijiang College of Zhejiang University of Technology
基金supported by the National Natural Science Foundation of China(Grant No.51202250)the Knowledge Innovation Program of the Chinese Academy of Sciences(Grant No.13J131211)
文摘The study of the linear and nonlinear optical properties of Zn Ge P2 based on density functional theory has been carried out. In order to get a more physical picture in the infrared region, terms which are considered as the phonon effect were added to the calculated refractive dispersion curves. The phonon-corrected calculation curves show excellent agreement with experimental refractive indexes, which gives a better comprehension of the linear optical proprieties in the transparent region. The static nonlinear optical susceptibility was investigated using approaches based on the ＂sum over states＂ and the2 n ＋ 1 theorem methods. Both of the results of these two methods reasonably coincided with the experimental results.
基金financial support of the 100-Talent Program of Chinese Academy of Sciences。
文摘Polymeric membranes with diverse structures have attracted much attention as new materials for nonlinear optical devices. In this report, a novel oligomer of poly(aromatic ether sulfone)(OAES) has been synthesized and characterized. The electronic structure as well as linear and nonlinear optical properties has been studied by density function theory. The effect for general nonlinear optical polarizability of various condition has been further researched such as absence of side chains and introduction of phenyl substituent on side chains. The static and frequency-dependent hyperpolarizabilities of OAES and its derivatives have been calculated. This work interprets an efficient adjustment for the frequency response and the intensity of nonlinear optical polarizability can be achieved by regulating the structure of system, which provides a new potential for the application of oligomeric materials on nonlinear optical field.
基金Project supported by the National Natural Science Foundation of China （No. 20373009）, the Specialized Research Fund for the Doctoral Program in Higher Education Institutions of the Ministry of Education of China （No. 20030183063） and Science Foundation for Young Teachers of Northeast Normal University （No. 20060311）.
文摘Based on the equilibrium structures from quantum mechanics AM1 method, employing INDO/CI method and the sum-over-state （SOS） formula, the one-photon absorption （OPA） and two-photon absorption （TPA） properties as well as the second hyperpolarizabilities were discussed in detail for a kind of PPV derivative poly 2-（9-phenylanthracen-10-yl）-1,4-phenylenevinylene （P1）. The results indicate that the two-photon cross section （3） increases with the increasing of the number of repeating segment （n）, however only a slight increase corresponds to the increasing of molecular weight when the repeating unit number arrives at a certain number. From this point of view, the TPA cross section values of P1 were extrapolated through the linear fit of 3 value vs. 1/n. The δ value of P1 is as high as 181 GM （1 GM=10^-50 cm^4·s·photon^-1）. Concerning the influence of pendent group and extension of π-conjugation on 3 values, another four oligomers P2, PPV, P1-1, and P2-1 were investigated for comparison. The calculation results reveal that the position and property of pendent group have great influence on the OPA and TPA properties. A most crucial role for relatively larger 3 value was played by the extension of π-conjugation.
基金supported by the National Natural Science Foundation of China(No.21673025)the Open Projects of the Key Laboratory of Polyoxometalate Science of Ministry of Education(NENU),China and the Project of the State Key Laboratory of Supramolecular Structure and Materials(JLU),China(No.SKLSSM2021020).
文摘The current study has obtained excellent potential nonlinear optical(NLO)materials by combining density functional theory methods with sum-over-states model to predict the second order NLO properties of helical graphene nanoribbons(HGNs)through introducing azulene defects or/and BN units.The introduction of these functional groups deforms the pristine HGN(compression or tension)and enhances obviously the static first hyperpolarizability(〈β0〉)of system by up to two orders of magnitude.The tensor components along the helical axis of HGNs play a dominant role in the total〈β0〉.The azulene defects and the BN units polarize the pristine HGN to different degrees,and the azulenes and contiguous benzenes are involved in the major electron excitations with significant contributions to〈β0〉but the BN units are not.The BN-doped chiral HGNs have good kinetic stability and strong second order NLO properties(6.84×10^(5)×10^(−30) esu),and can be a potential candidate of high-performance second order NLO materials.The predicted two-dimensional second order NLO spectra provide useful information for further exploration of those helicenes for electro-optic applications.
