The fabrication of multifunctional electronic devices based on the intriguing natures of organic semiconductors is crucial for organic electronics.Ultranarrow-bandgap materials are in urgent demand for fabricating hig...The fabrication of multifunctional electronic devices based on the intriguing natures of organic semiconductors is crucial for organic electronics.Ultranarrow-bandgap materials are in urgent demand for fabricating high-performance organic photovoltaic(OPV)cells and highly sensitive near-infrared organic photodetectors(OPDs).By combining alkoxy modification and an asymmetric strategy,three narrowbandgap electronic acceptors(BTP-4F,DO-4F,and QO-4F)were synthesized with finely tuned molecular electrostatic potential(ESP)distributions.Through the careful modulation of electronic configurations,the optical absorption onsets of DO-4F and QO-4F exceeded 1μm.The experimental and theoretical results suggest that the small ESP of QO-4F is beneficial for achieving a low nonradiative voltage loss,while the large ESP of BTP-4F can help obtain high exciton dissociation efficiency.By contrast,the asymmetric acceptor DO-4F with a moderate ESP possesses balanced voltage loss and exciton dissociation,yielding the best power conversion efficiency of 13.6%in the OPV cells.OPDs were also fabricated based on the combination of PBDB-T:DO-4F,and the as-fabricated device outputs a high shot-noise-limited specific detectivity of 3.05×10^(13) Jones at 850 nm,which is a very good result for near-infrared OPDs.This work is anticipated to provide a rational way of designing high-performance ultranarrow-bandgap organic semiconductors by modulating the molecular ESP.展开更多
The methylamine and 2,4-dichoro-5-intropyreddine have been optbozed byab initio method at DZ basis function level. In the equilibrium geometry of reactant(Ⅰ),there are 28.6 ° degrees of dihedral angles between t...The methylamine and 2,4-dichoro-5-intropyreddine have been optbozed byab initio method at DZ basis function level. In the equilibrium geometry of reactant(Ⅰ),there are 28.6 ° degrees of dihedral angles between the pyrimidine plane and nitro groupplane. The electrostatic potentials and molecular orbital properties for the reactant(Ⅰ)and methylalnine are discussed too. It can be concluded that the 4 site of reactant(Ⅰ) iseasier than the 2 site to proceed talnation reaction. This conclusion is in good agreementwith expered results.展开更多
We present a parallel and linear scaling implementation of the calculation of the electrostatic potential arising from an arbitrary charge distribution.Our approach is making use of the multi-resolution basis of multi...We present a parallel and linear scaling implementation of the calculation of the electrostatic potential arising from an arbitrary charge distribution.Our approach is making use of the multi-resolution basis of multiwavelets.The potential is obtained as the direct solution of the Poisson equation in its Green’s function integral form.In the multiwavelet basis,the formally non local integral operator decays rapidly to negligible values away from the main diagonal,yielding an effectively banded structure where the bandwidth is only dictated by the requested accuracy.This sparse operator structure has been exploited to achieve linear scaling and parallel algorithms.Parallelization has been achieved both through the shared memory(OpenMP)and the message passing interface(MPI)paradigm.Our implementation has been tested by computing the electrostatic potential of the electronic density of long-chain alkanes and diamond fragments showing(sub)linear scaling with the system size and efficent parallelization.展开更多
Halogenated methyl-phenyl ethers （anisoles） are ubiquitous organic compounds in the environment. In the present study, geometrical optimization and electrostatic potential calculations have been performed for 42 hal...Halogenated methyl-phenyl ethers （anisoles） are ubiquitous organic compounds in the environment. In the present study, geometrical optimization and electrostatic potential calculations have been performed for 42 halogenated anisoles at the HF/6-31 G^＊ level. A number of statistically based parameters have been obtained. By multiple regression method, linear relationships between the gas-chromatographic relative retention time （RRT） and structural descriptors have been established for the training set of 32 halogenated anisoles. The result showed that the parameters derived from electrostatic potentials （ESPs） together with the molecular volume （Vmc） could be well used to express the quantitative structure-RRT relationships of halogenated anisoles. The best two-variable regression model gives a correlation coefficient of 0.980 and a standard deviation of 0.07, and the leave-one-out cross-validated correlation coefficient is 0.975. The goodness of the model has been further validated through exploring the predictive power for the testing set of 10 halogenated anisoles.展开更多
Geometrical optimization and electrostatic potential calculations have been performed for a series of halogenated hydrocarbons at the HF/Gen-6d level. A number of electrostatic potentials and the statistically based s...Geometrical optimization and electrostatic potential calculations have been performed for a series of halogenated hydrocarbons at the HF/Gen-6d level. A number of electrostatic potentials and the statistically based structural descriptors derived from these electrostatic potentials have been obtained. Multiple linear regression analysis and artificial neural network are employed simultaneously in this paper. The result shows that the parameters derived from electrostatic 2 potentials σtot^2, V s and ∑ Vs^＋, together with the molecular volume （Vine） can be used to express the quantitative structure-infinite dilution activity coefficients （γ^∞） relationship of halogenated hydrocarbons in water. The result also demonstrates that the model obtained by using BFGS quasiNewton neural network method has much better predictive capability than that from multiple linear regression. The goodness of the model has been validated through exploring the predictive power for the external test set. The model obtained via neural network may be applied to predict γ^∞ of other halogenated hydrocarbons not present in the data set.展开更多
The nature of halogen bonding in five complexes formed between the thiocyanate （NCS） radical and a BrC1 molecule was analyzed by quantum theory of atoms in molecules （QTAIM） and electron-localization function （EL...The nature of halogen bonding in five complexes formed between the thiocyanate （NCS） radical and a BrC1 molecule was analyzed by quantum theory of atoms in molecules （QTAIM） and electron-localization function （ELF） in this paper. The calculated results show that the geometry of the halogen atom bonded at the N-atom is stable than those bonded at S- or C-atom. The molecular electrostatic potentials determine the geometries and stabilities of the complexes. The valence basin of the S- or N-atom in the electron-donating NCS radical is compressed and its population decreases during the process of formation of the halogen-bonded complexes.展开更多
基金the support from the National Natural Science Foundation of China(NSFC,21835006)the financial support from the NSFC(22075301 and 22122905)+2 种基金the Youth Innovation Promotion Association CAS(2018043)the Key Research Program of the Chinese Academy of Sciences,Grant NO.XDPB13-3supported by the Beijing National Laboratory for Molecular Sciences(BNLMS-CXXM-201903)。
文摘The fabrication of multifunctional electronic devices based on the intriguing natures of organic semiconductors is crucial for organic electronics.Ultranarrow-bandgap materials are in urgent demand for fabricating high-performance organic photovoltaic(OPV)cells and highly sensitive near-infrared organic photodetectors(OPDs).By combining alkoxy modification and an asymmetric strategy,three narrowbandgap electronic acceptors(BTP-4F,DO-4F,and QO-4F)were synthesized with finely tuned molecular electrostatic potential(ESP)distributions.Through the careful modulation of electronic configurations,the optical absorption onsets of DO-4F and QO-4F exceeded 1μm.The experimental and theoretical results suggest that the small ESP of QO-4F is beneficial for achieving a low nonradiative voltage loss,while the large ESP of BTP-4F can help obtain high exciton dissociation efficiency.By contrast,the asymmetric acceptor DO-4F with a moderate ESP possesses balanced voltage loss and exciton dissociation,yielding the best power conversion efficiency of 13.6%in the OPV cells.OPDs were also fabricated based on the combination of PBDB-T:DO-4F,and the as-fabricated device outputs a high shot-noise-limited specific detectivity of 3.05×10^(13) Jones at 850 nm,which is a very good result for near-infrared OPDs.This work is anticipated to provide a rational way of designing high-performance ultranarrow-bandgap organic semiconductors by modulating the molecular ESP.
文摘The methylamine and 2,4-dichoro-5-intropyreddine have been optbozed byab initio method at DZ basis function level. In the equilibrium geometry of reactant(Ⅰ),there are 28.6 ° degrees of dihedral angles between the pyrimidine plane and nitro groupplane. The electrostatic potentials and molecular orbital properties for the reactant(Ⅰ)and methylalnine are discussed too. It can be concluded that the 4 site of reactant(Ⅰ) iseasier than the 2 site to proceed talnation reaction. This conclusion is in good agreementwith expered results.
基金supported by the Research Council of Norway through a Cen-tre of Excellence Grant(Grant No.179568/V30)from the Norwegian Super-computing Program(NOTUR)through a grant of computer time(Grant No.NN4654K).
文摘We present a parallel and linear scaling implementation of the calculation of the electrostatic potential arising from an arbitrary charge distribution.Our approach is making use of the multi-resolution basis of multiwavelets.The potential is obtained as the direct solution of the Poisson equation in its Green’s function integral form.In the multiwavelet basis,the formally non local integral operator decays rapidly to negligible values away from the main diagonal,yielding an effectively banded structure where the bandwidth is only dictated by the requested accuracy.This sparse operator structure has been exploited to achieve linear scaling and parallel algorithms.Parallelization has been achieved both through the shared memory(OpenMP)and the message passing interface(MPI)paradigm.Our implementation has been tested by computing the electrostatic potential of the electronic density of long-chain alkanes and diamond fragments showing(sub)linear scaling with the system size and efficent parallelization.
基金This work was supported by the National Natural Science Foundation of China (No. 20502022) and the Ph.D. Fund of Ningbo ( No. 2004A610010)
文摘Halogenated methyl-phenyl ethers （anisoles） are ubiquitous organic compounds in the environment. In the present study, geometrical optimization and electrostatic potential calculations have been performed for 42 halogenated anisoles at the HF/6-31 G^＊ level. A number of statistically based parameters have been obtained. By multiple regression method, linear relationships between the gas-chromatographic relative retention time （RRT） and structural descriptors have been established for the training set of 32 halogenated anisoles. The result showed that the parameters derived from electrostatic potentials （ESPs） together with the molecular volume （Vmc） could be well used to express the quantitative structure-RRT relationships of halogenated anisoles. The best two-variable regression model gives a correlation coefficient of 0.980 and a standard deviation of 0.07, and the leave-one-out cross-validated correlation coefficient is 0.975. The goodness of the model has been further validated through exploring the predictive power for the testing set of 10 halogenated anisoles.
文摘Geometrical optimization and electrostatic potential calculations have been performed for a series of halogenated hydrocarbons at the HF/Gen-6d level. A number of electrostatic potentials and the statistically based structural descriptors derived from these electrostatic potentials have been obtained. Multiple linear regression analysis and artificial neural network are employed simultaneously in this paper. The result shows that the parameters derived from electrostatic 2 potentials σtot^2, V s and ∑ Vs^＋, together with the molecular volume （Vine） can be used to express the quantitative structure-infinite dilution activity coefficients （γ^∞） relationship of halogenated hydrocarbons in water. The result also demonstrates that the model obtained by using BFGS quasiNewton neural network method has much better predictive capability than that from multiple linear regression. The goodness of the model has been validated through exploring the predictive power for the external test set. The model obtained via neural network may be applied to predict γ^∞ of other halogenated hydrocarbons not present in the data set.
基金Project supported by the National Natural Science Foundation of China （Nos. 20973053, 20801017）, the Natural Science Foundation of Hebei Province （Nos. B 2011205058, B2010000371）, the Education Department Foundation of Hebei Province （Nos. 2009137, ZD2010126 ）.
文摘The nature of halogen bonding in five complexes formed between the thiocyanate （NCS） radical and a BrC1 molecule was analyzed by quantum theory of atoms in molecules （QTAIM） and electron-localization function （ELF） in this paper. The calculated results show that the geometry of the halogen atom bonded at the N-atom is stable than those bonded at S- or C-atom. The molecular electrostatic potentials determine the geometries and stabilities of the complexes. The valence basin of the S- or N-atom in the electron-donating NCS radical is compressed and its population decreases during the process of formation of the halogen-bonded complexes.
