This work presents a theoretical insight into the variation of the site-specific intermolecular hydrogen-bonding （HB）, formed between C=O group of fluorenone （FN） and O-H groups of methanol （MeOL） molecules, ind...This work presents a theoretical insight into the variation of the site-specific intermolecular hydrogen-bonding （HB）, formed between C=O group of fluorenone （FN） and O-H groups of methanol （MeOL） molecules, induced by both the electronic excitation and the bulk solvent effect. Through the calculation of molecular ground- and excited-state properties, we not only demonstrate the characters of HB strengthening induced by electronic excitation and the bulk solvent effect but also reveal the underlying physical mechanism which leads to the HB variation. The strengthening of the intermolecular HB in electronically excited states and in liquid solution is characterized by the reduced HB bond-lengths and the red-shift IR spectra accompanied by the increasing intensities of IR absorption corresponding to the characteristic vibrational modes of the O-H and C--O stretching. The HB strengthening in the excited electronic states and in solution mainly arises from the charge redistribution of the FN molecule induced by the electronic excitation and bulk solvent instead of the intermolecular charge transfer. The charge redistribution of the solute molecule increases the partial dipole moment of FN molecule and the FN-MeOL intermolecular interaction, which subsequently leads to the HB strengthening. With the bulk solvent effect getting involved, the theoretical IR spectra of HBed FN-MeOL complexes agree much better with the experiments than those of gas-phase FN-MeOL dimer. All the calculations are carried out based on our developed analytical approaches for the first and second energy derivatives of excited electronic state within the time-dependent density functional theory.展开更多
Deposition of clean and defect-free atomically thin two-dimensional crystalline flakes on surfaces by mechanical exfoliation of layered bulk materials has proven to be a powerful technique, but it requires a fast, rel...Deposition of clean and defect-free atomically thin two-dimensional crystalline flakes on surfaces by mechanical exfoliation of layered bulk materials has proven to be a powerful technique, but it requires a fast, reliable and non-destructive way to identify the atomically thin flakes among a crowd of thick flakes. In this work, we provide general guidelines to identify ultrathin flakes of TaSe2 by means of optical microscopy and Raman spectroscopy. Additionally, we determine the optimal substrates to facilitate the optical identification of atomically thin TaSe2 crystals. Experimental realization and isolation of ultrathin layers of TaSe2 enables future studies on the role of the dimensionality in interesting phenomena such as superconductivity and charge density waves.展开更多
We report the plasmon-enhanced polymer bulk-heterojunction solar cells with Ag nanoparticles (AgNPs) obtained via chemical method. Here, the AgNPs films with different particle densities are introduced between the pol...We report the plasmon-enhanced polymer bulk-heterojunction solar cells with Ag nanoparticles (AgNPs) obtained via chemical method. Here, the AgNPs films with different particle densities are introduced between the poly (3,4-ethylene dioxythiophene) poly (styrenesulfonate) (PEDOT: PSS) buffer layer and the poly (3-hexythiophene):[6,6]-phenyl-c61 butyric acid methyl ester (P3HT: PCBM) layer. By improving the optical absorption of the active layer owing to the localized surface plasmons, the power conversion efficiency of the solar cells is increased compared with the control device. It is shown that the efficiency of the device increases with the density of AgNPs. For the device employing higher density, the resulted power conversion efficiency is found to increase from 2.89% to 3.38%, enhanced by 16.96%.展开更多
文摘This work presents a theoretical insight into the variation of the site-specific intermolecular hydrogen-bonding （HB）, formed between C=O group of fluorenone （FN） and O-H groups of methanol （MeOL） molecules, induced by both the electronic excitation and the bulk solvent effect. Through the calculation of molecular ground- and excited-state properties, we not only demonstrate the characters of HB strengthening induced by electronic excitation and the bulk solvent effect but also reveal the underlying physical mechanism which leads to the HB variation. The strengthening of the intermolecular HB in electronically excited states and in liquid solution is characterized by the reduced HB bond-lengths and the red-shift IR spectra accompanied by the increasing intensities of IR absorption corresponding to the characteristic vibrational modes of the O-H and C--O stretching. The HB strengthening in the excited electronic states and in solution mainly arises from the charge redistribution of the FN molecule induced by the electronic excitation and bulk solvent instead of the intermolecular charge transfer. The charge redistribution of the solute molecule increases the partial dipole moment of FN molecule and the FN-MeOL intermolecular interaction, which subsequently leads to the HB strengthening. With the bulk solvent effect getting involved, the theoretical IR spectra of HBed FN-MeOL complexes agree much better with the experiments than those of gas-phase FN-MeOL dimer. All the calculations are carried out based on our developed analytical approaches for the first and second energy derivatives of excited electronic state within the time-dependent density functional theory.
文摘Deposition of clean and defect-free atomically thin two-dimensional crystalline flakes on surfaces by mechanical exfoliation of layered bulk materials has proven to be a powerful technique, but it requires a fast, reliable and non-destructive way to identify the atomically thin flakes among a crowd of thick flakes. In this work, we provide general guidelines to identify ultrathin flakes of TaSe2 by means of optical microscopy and Raman spectroscopy. Additionally, we determine the optimal substrates to facilitate the optical identification of atomically thin TaSe2 crystals. Experimental realization and isolation of ultrathin layers of TaSe2 enables future studies on the role of the dimensionality in interesting phenomena such as superconductivity and charge density waves.
基金supported by the Project of Tianjin Ministry of Education (No. 20100723)the National Natural Science Foundation of China (No. 60876046)
文摘We report the plasmon-enhanced polymer bulk-heterojunction solar cells with Ag nanoparticles (AgNPs) obtained via chemical method. Here, the AgNPs films with different particle densities are introduced between the poly (3,4-ethylene dioxythiophene) poly (styrenesulfonate) (PEDOT: PSS) buffer layer and the poly (3-hexythiophene):[6,6]-phenyl-c61 butyric acid methyl ester (P3HT: PCBM) layer. By improving the optical absorption of the active layer owing to the localized surface plasmons, the power conversion efficiency of the solar cells is increased compared with the control device. It is shown that the efficiency of the device increases with the density of AgNPs. For the device employing higher density, the resulted power conversion efficiency is found to increase from 2.89% to 3.38%, enhanced by 16.96%.
