Aggregation-induced thermally activated delayed fluorescence(TADF)phenomena have attracted extensive attention recently.In this paper,several theoretical models including monomer,dimer,and complex are used for the exp...Aggregation-induced thermally activated delayed fluorescence(TADF)phenomena have attracted extensive attention recently.In this paper,several theoretical models including monomer,dimer,and complex are used for the explanation of the luminescent properties of(R)-5-(9H-carbazol-9-yl)-2-(1,2,3,4-tetrahydronaphthalen-1-yl)isoindoline-1,3-dione((R)-ImNCz),which was recently reported[Chemical Engineering Journal 418129167(2021)].The polarizable continuum model(PCM)and the combined quantum mechanics and molecular mechanics(QM/MM)method are adopted in simulation of the property of the molecule in the gas phase,solvated in acetonitrile and in aggregation states.It is found that large spin–orbit coupling(SOC)constants and a smaller energy gap between the first singlet excited state and the first triplet excited state(△E_(st))in prism-like single crystals(SC_(p)-form)are responsible for the TADF of(R)-lmNCz,while no TADF is found in block-like single crystals(SC_(b)-form)with a larger △E_(st).The multiple ultralong phosphorescence(UOP)peaks in the spectrum are of complex origins,and they are related not only to ImNCz but also to a minor amount of impurities(ImNBd)in the crystal prepared in the laboratory.The dimer has similar phosphorescence emission wavelengths to the(R)-lmNCz-SC_(p) monomers.The complex composed of(R)-lmNCz and(R)-lmNBd contributes to the phosphorescent emission peak at about 600 nm,and the phosphorescent emission peak at about 650 nm is generated by(R)-lmNBd.This indicates that the impurity could also contribute to emission in molecular crystals.The present calculations clarify the relationship between the molecular aggregation and the light-emitting properties of the TADF emitters and will therefore be helpful for the design of potentially more useful TADF emitters.展开更多
报道了激射波长为2.1μm的Ga In Sb/Al Ga As Sb双量子阱激光器。通过优化外延结构设计和欧姆接触,无镀膜的宽条激光器达到了9.8%的峰值功率转换效率,这比原来的值提高了1.5倍,室温下得到了615 m W的连续激射功率输出和1.5 W的脉冲激射...报道了激射波长为2.1μm的Ga In Sb/Al Ga As Sb双量子阱激光器。通过优化外延结构设计和欧姆接触,无镀膜的宽条激光器达到了9.8%的峰值功率转换效率,这比原来的值提高了1.5倍,室温下得到了615 m W的连续激射功率输出和1.5 W的脉冲激射功率输出。这些激光器的阈值电流密度低至126 A/cm2,斜率效率高达0.3 W/A。通过测试不同腔长的激光器,测得内损耗和内量子效率分别为6 cm-1和75.5%,均比原有器件有很大提升。激光器在连续工作3 000 h后,功率没有明显下降。展开更多
Potential energies of LiS（^2∏）, LiS-（^1E＋） and LiS＋ （^3E-） are calculated by using the multi- reference configuration interaction method including Davidson correction and the augmented correlation-consistent ...Potential energies of LiS（^2∏）, LiS-（^1E＋） and LiS＋ （^3E-） are calculated by using the multi- reference configuration interaction method including Davidson correction and the augmented correlation-consistent basis sets aug-cc-PV（X＋d）Z （X=T, Q）. Such obtained potential energies are subsequently extrapolated to the complete basis set limit. Both the core-valence correction and the relativistic effect are also considered. The analytical potential energy functions are then obtained by fitting such accurate energies utilizing a least-squares fitting procedure. By using such analytical potential energy functions, we obtain the accurate spectroscopic parameters, complete set of vibrational levels and classical turning points. The present results are compared well with the experimental and other theoretical work.展开更多
The dynamics of C+H_(2)→H+CH reaction is theoretically studied using the quasiclassical trajectory and quantum mechanical wave packet methods.The analysis of reaction probabilities,integral cross sections,and rate co...The dynamics of C+H_(2)→H+CH reaction is theoretically studied using the quasiclassical trajectory and quantum mechanical wave packet methods.The analysis of reaction probabilities,integral cross sections,and rate coefficients reveal the essential Coriolis coupling effects in the quantum mechanical wave packet calculations.The calculated polarizationdependent differential cross section,P(θ_(r))and P(Φ_(r))show that the j'of product rotational angular momentum is not only aligned along the y axis and the direction of the vector x+z,but also strongly oriented along the positive y axis.展开更多
The field-free alignment of molecule Cl CN is investigated by using a terahertz few-cycle pulse(THz FCP)based on the time-dependent density matrix theory.It is shown that a high degree of molecular alignment can be ob...The field-free alignment of molecule Cl CN is investigated by using a terahertz few-cycle pulse(THz FCP)based on the time-dependent density matrix theory.It is shown that a high degree of molecular alignment can be obtained by changing the matching number of the THz FCPs in the adiabatic regime and the non-adiabatic regime.The matching number can affect both the maximum value of the alignment and the time at which it is achieved.It is also found that a higher degree of alignment can be achieved by using the THz FCP at lower intensity and there exists an optimal threshold of molecular alignment with the increase of the field amplitude.Also found is the frequency sensitive region in which the degree of maximum alignment can be enhanced greatly by modulating the center frequencies of different THz FCPs.The investigation demonstrates that comparing with a THz single-cycle pulse,a better result of the field-free alignment can be created by a THz FCP at a constant rotational temperature of molecule.展开更多
The potential energy curves（PECs） of the first electronic excited state of S2（a^1△g） are calculated employing a multi-reference configuration interaction method with the Davidson correction in combination with a ...The potential energy curves（PECs） of the first electronic excited state of S2（a^1△g） are calculated employing a multi-reference configuration interaction method with the Davidson correction in combination with a series of correlationconsistent basis sets from Dunning： aug-cc-p VX Z（X = T, Q, 5, 6）. In order to obtain PECs with high accuracy, PECs calculated with aug-cc-p V（Q, 5）Z basis sets are extrapolated to the complete basis set limit. The resulting PECs are then fitted to the analytical potential energy function（APEF） using the extended Hartree–Fock approximate correlation energy method. By utilizing the fitted APEF, accurate and reliable spectroscopic parameters are obtained, which are consistent with both experimental and theoretical results. By solving the Schr o¨dinger equation numerically with the APEFs obtained at the AV6 Z and the extrapolated AV（Q, 5）Z level of theory, we calculate the complete set of vibrational levels, classical turning points, inertial rotation and centrifugal distortion constants.展开更多
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11974216,11874242,21933002 and 11904210)Shandong Provincial Natural Science Foundation,China(Grant No.ZR2019MA056)+1 种基金the support of the Taishan Scholar Project of Shandong Provincethe project funded by China Postdoctoral Science Foundation(Grant No.2018M642689)。
文摘Aggregation-induced thermally activated delayed fluorescence(TADF)phenomena have attracted extensive attention recently.In this paper,several theoretical models including monomer,dimer,and complex are used for the explanation of the luminescent properties of(R)-5-(9H-carbazol-9-yl)-2-(1,2,3,4-tetrahydronaphthalen-1-yl)isoindoline-1,3-dione((R)-ImNCz),which was recently reported[Chemical Engineering Journal 418129167(2021)].The polarizable continuum model(PCM)and the combined quantum mechanics and molecular mechanics(QM/MM)method are adopted in simulation of the property of the molecule in the gas phase,solvated in acetonitrile and in aggregation states.It is found that large spin–orbit coupling(SOC)constants and a smaller energy gap between the first singlet excited state and the first triplet excited state(△E_(st))in prism-like single crystals(SC_(p)-form)are responsible for the TADF of(R)-lmNCz,while no TADF is found in block-like single crystals(SC_(b)-form)with a larger △E_(st).The multiple ultralong phosphorescence(UOP)peaks in the spectrum are of complex origins,and they are related not only to ImNCz but also to a minor amount of impurities(ImNBd)in the crystal prepared in the laboratory.The dimer has similar phosphorescence emission wavelengths to the(R)-lmNCz-SC_(p) monomers.The complex composed of(R)-lmNCz and(R)-lmNBd contributes to the phosphorescent emission peak at about 600 nm,and the phosphorescent emission peak at about 650 nm is generated by(R)-lmNBd.This indicates that the impurity could also contribute to emission in molecular crystals.The present calculations clarify the relationship between the molecular aggregation and the light-emitting properties of the TADF emitters and will therefore be helpful for the design of potentially more useful TADF emitters.
文摘报道了激射波长为2.1μm的Ga In Sb/Al Ga As Sb双量子阱激光器。通过优化外延结构设计和欧姆接触,无镀膜的宽条激光器达到了9.8%的峰值功率转换效率,这比原来的值提高了1.5倍,室温下得到了615 m W的连续激射功率输出和1.5 W的脉冲激射功率输出。这些激光器的阈值电流密度低至126 A/cm2,斜率效率高达0.3 W/A。通过测试不同腔长的激光器,测得内损耗和内量子效率分别为6 cm-1和75.5%,均比原有器件有很大提升。激光器在连续工作3 000 h后,功率没有明显下降。
基金This work was supported by the National Natural Science Foundation of China （No.11304185）, Taishan scholar project of Shandong Province, China Postdoctoral Science Foundation （No.2014M561957）, and Post-doctoral Innovation Project of Shandong Province （No.201402013）, Shandong Provincial Natural Science Foundation （No.ZR2014AM022）. The authors gratefully acknowledge Dr. S. Li for useful discussion in this work.
文摘Potential energies of LiS（^2∏）, LiS-（^1E＋） and LiS＋ （^3E-） are calculated by using the multi- reference configuration interaction method including Davidson correction and the augmented correlation-consistent basis sets aug-cc-PV（X＋d）Z （X=T, Q）. Such obtained potential energies are subsequently extrapolated to the complete basis set limit. Both the core-valence correction and the relativistic effect are also considered. The analytical potential energy functions are then obtained by fitting such accurate energies utilizing a least-squares fitting procedure. By using such analytical potential energy functions, we obtain the accurate spectroscopic parameters, complete set of vibrational levels and classical turning points. The present results are compared well with the experimental and other theoretical work.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11904394 and 12004216)the Natural Science Foundation of Shandong Province,China(Grant No.ZR2020QA064)。
文摘The dynamics of C+H_(2)→H+CH reaction is theoretically studied using the quasiclassical trajectory and quantum mechanical wave packet methods.The analysis of reaction probabilities,integral cross sections,and rate coefficients reveal the essential Coriolis coupling effects in the quantum mechanical wave packet calculations.The calculated polarizationdependent differential cross section,P(θ_(r))and P(Φ_(r))show that the j'of product rotational angular momentum is not only aligned along the y axis and the direction of the vector x+z,but also strongly oriented along the positive y axis.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.12274265 and 11874241)the Taishan Scholar Project of Shandong Province,China。
文摘The field-free alignment of molecule Cl CN is investigated by using a terahertz few-cycle pulse(THz FCP)based on the time-dependent density matrix theory.It is shown that a high degree of molecular alignment can be obtained by changing the matching number of the THz FCPs in the adiabatic regime and the non-adiabatic regime.The matching number can affect both the maximum value of the alignment and the time at which it is achieved.It is also found that a higher degree of alignment can be achieved by using the THz FCP at lower intensity and there exists an optimal threshold of molecular alignment with the increase of the field amplitude.Also found is the frequency sensitive region in which the degree of maximum alignment can be enhanced greatly by modulating the center frequencies of different THz FCPs.The investigation demonstrates that comparing with a THz single-cycle pulse,a better result of the field-free alignment can be created by a THz FCP at a constant rotational temperature of molecule.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11304185 and 11074151)
文摘The potential energy curves（PECs） of the first electronic excited state of S2（a^1△g） are calculated employing a multi-reference configuration interaction method with the Davidson correction in combination with a series of correlationconsistent basis sets from Dunning： aug-cc-p VX Z（X = T, Q, 5, 6）. In order to obtain PECs with high accuracy, PECs calculated with aug-cc-p V（Q, 5）Z basis sets are extrapolated to the complete basis set limit. The resulting PECs are then fitted to the analytical potential energy function（APEF） using the extended Hartree–Fock approximate correlation energy method. By utilizing the fitted APEF, accurate and reliable spectroscopic parameters are obtained, which are consistent with both experimental and theoretical results. By solving the Schr o¨dinger equation numerically with the APEFs obtained at the AV6 Z and the extrapolated AV（Q, 5）Z level of theory, we calculate the complete set of vibrational levels, classical turning points, inertial rotation and centrifugal distortion constants.
