This paper studies the molecular rotational excitation and field-free spatial alignment in a nonresonant intense laser field numerically and analytically by using the time-dependent SchrSdinger equation. The broad rot...This paper studies the molecular rotational excitation and field-free spatial alignment in a nonresonant intense laser field numerically and analytically by using the time-dependent SchrSdinger equation. The broad rotational wave packets excited by the femtosecond pulse are defined in conjugate angle space, and their coefficients are obtained by solving a set of coupled linear equations. Both single molecule orientation angles and an ensemble of O2 and CO molecule angular distributions are calculated in detail. The numerical results show that, for single molecule highest occupied molecular orbital （HOMO） symmetry σ tends to have a molecular orientation along the laser polarization direction and the permanent dipole moment diminishes the mean of the orientation angles; for an ensemble of molecules, angular distributions provide more complex and additional information at times where there are no revivals in the single molecule plot. In particular, at the revival peak instant, with the increase of temperature of the molecular ensemble, the anisotropic angular distributions with respect to the laser polarization direction of the πg orbital gradually transform to the symmetrical distributions regarding the laser polarization vector and for two HOMO configurations angular distributions of all directions are confined within a smaller angle when the temperature of the molecular ensemble is higher.展开更多
The highest occupied molecular orbital（HOMO） energies of fullerenes are found by quantitative first-principles calculations to be raised by negative charging, and the rising rate rank of the fullerenes is C60 >C7...The highest occupied molecular orbital（HOMO） energies of fullerenes are found by quantitative first-principles calculations to be raised by negative charging, and the rising rate rank of the fullerenes is C60 >C70 >C80 >C90>C100 >C180. Then we compare fullerenes with carbon nanotubes（CNTs） and graphene sheets（GSs） and find that the increase of the HOMO energy of a fullerene is much faster than that of CNTs and graphene sheets with the same number of C atoms. The rising rate rank is fullerene>CNT>GS, which holds no matter what the number of C atoms is or which structure the fullerene isomer is. This work paves a new path for developing all-carbon devices with low-dimensional carbon nanomaterials as different functional elements.展开更多
Significant interest has been focused on graphene materials for their unique properties as Hydrogen storage materials. The development of their abilities by modifying their configuration with doped or decorated transi...Significant interest has been focused on graphene materials for their unique properties as Hydrogen storage materials. The development of their abilities by modifying their configuration with doped or decorated transition metals </span><span style="font-family:Verdana;">was also of great interest. In this work</span><span style="font-family:Verdana;">,</span><span style="font-family:Verdana;"> using the DFT/B3LYP/6-31G/LanL2DZ</span><span style="font-family:Verdana;"> level of theory, graphene sheet (GS) as one of the materials of interest was doped with two transition metals, Osmium (Os) and Tungsten (W). Two active sites on the GS were tested (C4 and C16) resulted into adsorbed systems, H2@C4-GS and H2@C16-GS. C16 position showed the largest adsorption energy compared to that at C4. Therefore, C4 was replaced by the two metals and two adsorbed systems were formed</span><span style="font-family:Verdana;">: </span><span style="font-family:Verdana;">H</span><sub><span style="font-family:Verdana;vertical-align:sub;">2</span></sub><span style="font-family:Verdana;">@Os-GS and H2@W-GS. The binding energy of H</span><sub><span style="font-family:Verdana;vertical-align:sub;">2</span></sub><span style="font-family:Verdana;">@Os-GS was found to be greater than that of H2@W-GS.展开更多
The use of quantitative structure-activity relationships (QSARs) started with the research into drugs and pesticides. It can be applied to predicting biological activity of new organic compounds from their molecular s...The use of quantitative structure-activity relationships (QSARs) started with the research into drugs and pesticides. It can be applied to predicting biological activity of new organic compounds from their molecular structure,or from their physicochemical parameters, andto direct synthesis of new drug and pesticide.展开更多
We report a donor-acceptor(D-A)type non-luminescent neutral radical,tris-2,4,6-trichlorophenylmethyl-N,N-dimethyl-9H-carbazol-3-amine(TTM-Cz-DMA).The results of cyclic voltammetry and quantum chemistry calculation con...We report a donor-acceptor(D-A)type non-luminescent neutral radical,tris-2,4,6-trichlorophenylmethyl-N,N-dimethyl-9H-carbazol-3-amine(TTM-Cz-DMA).The results of cyclic voltammetry and quantum chemistry calculation confirm TTM-Cz-DMA has the non-Aufbau electronic structure,which means the singly occupied molecular orbital(SOMO)lies below the highest doubly occupied molecular orbital(HOMO).The non-Aufbau electronic structure changes to the Aufbau electronic structure after protonation and exhibits proton-responsive turn-on fluorescence,which is totally reversible by deprotonation.The dihedral angle between donor and acceptor moieties of TTM-Cz-DMA in excited state reduces from 88°to 62°after protonation,causing the turn-on fluorescence.Our results offer a viewing angle to understand the luminescence of radicals and provide a possible application of proton detection.展开更多
To increase the current density of the hole only device, 1, 4, 5, 8, 9, 11-hexaazatriphenylene-hexacarbonitrile (HAT-CN) material has been inserted in the device at the indium tin oxide (ITO)/organic interface. Since ...To increase the current density of the hole only device, 1, 4, 5, 8, 9, 11-hexaazatriphenylene-hexacarbonitrile (HAT-CN) material has been inserted in the device at the indium tin oxide (ITO)/organic interface. Since HATCN molecule can withdraw electrons, it can alter electronic properties of the electrodes and hence inserted between the organic/metal interfaces. This paper deals with the optimization of the thickness of organic-metal layers to enhance the efficiency. Also, efforts have been made to increase the current density and reduce the operating voltage of the device. The material 2, 7-bis [N, N-bis (4- methoxy-phenyl) amino]-9, 9-spirobifluorene (Meo-Spiro-TPD) is used to simulate the hole only device because it is a thermally stable hole transport material. Simulated results shows that better current density values can be achieved compared to fabricated one by optimizing the organic metal layer thickness. The best optimized layer thickness of 22 nm for Alq3, 25 nm for *CBP doped with Ir(ppy)3, 9 nm for Meo-Spiro TPD and 4 nm for HAT-CN which results in current density of 0.12 A/cm2 with a reduction in operating voltage by approximately 2 V.展开更多
基金supported by the Program of Excellent Team in Harbin Institute of Technologythe Program for New Century Excellent Talents in University (NCET)National Natural Science Foundation of China (Grant Nos 10774033,60878018 and 10674036)
文摘This paper studies the molecular rotational excitation and field-free spatial alignment in a nonresonant intense laser field numerically and analytically by using the time-dependent SchrSdinger equation. The broad rotational wave packets excited by the femtosecond pulse are defined in conjugate angle space, and their coefficients are obtained by solving a set of coupled linear equations. Both single molecule orientation angles and an ensemble of O2 and CO molecule angular distributions are calculated in detail. The numerical results show that, for single molecule highest occupied molecular orbital （HOMO） symmetry σ tends to have a molecular orientation along the laser polarization direction and the permanent dipole moment diminishes the mean of the orientation angles; for an ensemble of molecules, angular distributions provide more complex and additional information at times where there are no revivals in the single molecule plot. In particular, at the revival peak instant, with the increase of temperature of the molecular ensemble, the anisotropic angular distributions with respect to the laser polarization direction of the πg orbital gradually transform to the symmetrical distributions regarding the laser polarization vector and for two HOMO configurations angular distributions of all directions are confined within a smaller angle when the temperature of the molecular ensemble is higher.
基金Supported by the National Natural Science Foundation of China under Grant Nos 11374174,51390471,51527803,and 51701143the National Basic Research Program of China under Grant No 2015CB654902+4 种基金the National Key Research and Development Program under Grant No 2016YFB0700402the Foundation for the Author of National Excellent Doctoral Dissertation under Grant No 201141the National Program for Thousand Young Talents of China,the Tianjin Municipal Education Commissionthe Tianjin Municipal Science and Technology Commissionthe Fundamental Research Fund of Tianjin University of Technology
文摘The highest occupied molecular orbital（HOMO） energies of fullerenes are found by quantitative first-principles calculations to be raised by negative charging, and the rising rate rank of the fullerenes is C60 >C70 >C80 >C90>C100 >C180. Then we compare fullerenes with carbon nanotubes（CNTs） and graphene sheets（GSs） and find that the increase of the HOMO energy of a fullerene is much faster than that of CNTs and graphene sheets with the same number of C atoms. The rising rate rank is fullerene>CNT>GS, which holds no matter what the number of C atoms is or which structure the fullerene isomer is. This work paves a new path for developing all-carbon devices with low-dimensional carbon nanomaterials as different functional elements.
文摘Significant interest has been focused on graphene materials for their unique properties as Hydrogen storage materials. The development of their abilities by modifying their configuration with doped or decorated transition metals </span><span style="font-family:Verdana;">was also of great interest. In this work</span><span style="font-family:Verdana;">,</span><span style="font-family:Verdana;"> using the DFT/B3LYP/6-31G/LanL2DZ</span><span style="font-family:Verdana;"> level of theory, graphene sheet (GS) as one of the materials of interest was doped with two transition metals, Osmium (Os) and Tungsten (W). Two active sites on the GS were tested (C4 and C16) resulted into adsorbed systems, H2@C4-GS and H2@C16-GS. C16 position showed the largest adsorption energy compared to that at C4. Therefore, C4 was replaced by the two metals and two adsorbed systems were formed</span><span style="font-family:Verdana;">: </span><span style="font-family:Verdana;">H</span><sub><span style="font-family:Verdana;vertical-align:sub;">2</span></sub><span style="font-family:Verdana;">@Os-GS and H2@W-GS. The binding energy of H</span><sub><span style="font-family:Verdana;vertical-align:sub;">2</span></sub><span style="font-family:Verdana;">@Os-GS was found to be greater than that of H2@W-GS.
基金Project supported by the National Natural Science Foundation of China.
文摘The use of quantitative structure-activity relationships (QSARs) started with the research into drugs and pesticides. It can be applied to predicting biological activity of new organic compounds from their molecular structure,or from their physicochemical parameters, andto direct synthesis of new drug and pesticide.
基金This work was supported by the National Natural Science Foundation of China(Nos.51925303 and 91833304)the Programme for Jilin University Science and Technology Innovative Research Team(JLUSTIRT),China(No.2019TD-33).
文摘We report a donor-acceptor(D-A)type non-luminescent neutral radical,tris-2,4,6-trichlorophenylmethyl-N,N-dimethyl-9H-carbazol-3-amine(TTM-Cz-DMA).The results of cyclic voltammetry and quantum chemistry calculation confirm TTM-Cz-DMA has the non-Aufbau electronic structure,which means the singly occupied molecular orbital(SOMO)lies below the highest doubly occupied molecular orbital(HOMO).The non-Aufbau electronic structure changes to the Aufbau electronic structure after protonation and exhibits proton-responsive turn-on fluorescence,which is totally reversible by deprotonation.The dihedral angle between donor and acceptor moieties of TTM-Cz-DMA in excited state reduces from 88°to 62°after protonation,causing the turn-on fluorescence.Our results offer a viewing angle to understand the luminescence of radicals and provide a possible application of proton detection.
文摘To increase the current density of the hole only device, 1, 4, 5, 8, 9, 11-hexaazatriphenylene-hexacarbonitrile (HAT-CN) material has been inserted in the device at the indium tin oxide (ITO)/organic interface. Since HATCN molecule can withdraw electrons, it can alter electronic properties of the electrodes and hence inserted between the organic/metal interfaces. This paper deals with the optimization of the thickness of organic-metal layers to enhance the efficiency. Also, efforts have been made to increase the current density and reduce the operating voltage of the device. The material 2, 7-bis [N, N-bis (4- methoxy-phenyl) amino]-9, 9-spirobifluorene (Meo-Spiro-TPD) is used to simulate the hole only device because it is a thermally stable hole transport material. Simulated results shows that better current density values can be achieved compared to fabricated one by optimizing the organic metal layer thickness. The best optimized layer thickness of 22 nm for Alq3, 25 nm for *CBP doped with Ir(ppy)3, 9 nm for Meo-Spiro TPD and 4 nm for HAT-CN which results in current density of 0.12 A/cm2 with a reduction in operating voltage by approximately 2 V.
