Double-resonance Raman(DRR)scattering in two-di-mensional(2D)materials describes the intravalley or intervalley scattering of an electron or a hole excited by incident photons.Although the presence of defects can prov...Double-resonance Raman(DRR)scattering in two-di-mensional(2D)materials describes the intravalley or intervalley scattering of an electron or a hole excited by incident photons.Although the presence of defects can provide additional momentum and influence the scat-tering process involving one or two phonons,only the idealized defects without any structural details are considered in tra-ditional DRR theory.Here,the second-order DRR spectra of WSe_(2) monolayer with different types of defects are calculated involving the combinations of acoustic and optical phonons in the vicinity of K(K')and M points of the Brillouin zone.The electronic band structures are modified due to the presence of defects,and the band unfolding method is adopted to show the bending of valence and conduction bands for the defective WSe_(2) monolayers.The associ-ated phononic band structures also exhibit different changes in phonon dispersion curves,re-sulting in different DRR spectra corresponding to the different types of defects in the WSe_(2) monolayers.For example,the existence of W vacancy in the WSe_(2) monolayer would result in downshifts in vibrational frequencies and asymmetrical broadenings in linewidths for most combination modes due to the dramatic changes in contour shape of electronic valleys at K and K'.Moreover,the scattering from K to Q is found to be forbidden for the two Se vacan-cies because of the elevation of conduction band at the Q point.Our work highlights the role of defect structures in the intervalley scattering and may provide better understanding in the underlying physics of DRR process in 2D materials.展开更多
Investigation on vibrational excitation and relaxation process will provide important in- formation for a better understanding of ultrafast dynamic response of energetic materials. Using sub-ps time-resolved coherent ...Investigation on vibrational excitation and relaxation process will provide important in- formation for a better understanding of ultrafast dynamic response of energetic materials. Using sub-ps time-resolved coherent anti-Stokes Raman scattering (CARS) experiments, we directly observe excitation of vibrational mode vs(NO2) and its relaxation process of ground state HNS (2,2',4,4',6,6'-hexanitrostillbenein) in solution. The results show that vs(NO2) at 1385 cm-1 has been excited and relaxation time of 0.38 and 8.5 ps is obtained. The possible quantum beat frequencies are also discussed via fs-CARS experiments. The original results provide an insight into ultrafast process of energetic materials.展开更多
Raman scattering is a versatile and powerful technique and has been widely used in modern scientific research and vast industrial applications. It is one of the fundamental experimental techniques in condensed matter ...Raman scattering is a versatile and powerful technique and has been widely used in modern scientific research and vast industrial applications. It is one of the fundamental experimental techniques in condensed matter physics, since it can sensitively probe the basic elementary excitations in solids like electron, phonon, magnon, etc. The application of extreme conditions (low temperature, high magnetic field, high pressure, etc.) to Raman scattering, will push its capability up to an unprecedented level, because this enables us to look into new quantum phases driven by extreme conditions, trace the evolution of the excitations and their coupling, and hence uncover the underlying physics. This review contains two topics. In the first part, we will introduce the Raman facility under extreme conditions, belonging to the optical spectroscopy station of Synergetic Extreme Condition User Facilities (SECUF), with emphasis on the system design and the capability the facility can provide. Then in the second part we will focus on the applications of Raman scattering under extreme conditions to a variety of condensed matter systems such as superconductors, correlated electron systems, charge density waves (CDW) materials, etc. Finally, as a rapidly developing technique, time-resolved Raman scattering will be highlighted here.展开更多
C60·2CHBr3 polycrystalline powder was prepared by the solution method. The vibrational modes of the sample were studied by Raman scattering and infrared adsorption techniques. The Raman spectra showed that the Ag...C60·2CHBr3 polycrystalline powder was prepared by the solution method. The vibrational modes of the sample were studied by Raman scattering and infrared adsorption techniques. The Raman spectra showed that the Ag modes were downshifted by 4-5 cm1, while the Hg(1) mode was unshifted. The analyses of the downshifts of the Ag modes revealed that a small amount of electrons were transferred from the hydrogen atoms to the C60 molecules. In the infrared spectra, the F1u modes of the pristine C60 were unshifted after the intercalation with CHBr3. However, the vibrational modes of CHBr3 changed remarkably. The C-Br stretching mode was downshifted by ~4 cm1. The adsorption of the C-H twisting mode was weakened obviously, and the adsorption of the C-H stretching mode was not observed. These results exhibited that there were nonnegligible interactions between CHBr3 and C60 molecules, and that the strongest interaction took place between the hydrogen atoms and the C60 molecules. The interaction should induce not only the changes of the vibrational modes reported here, but also those of the electronic states. So this work should offer important glues to the mechanism of the superconductivity at 117 K of the field-doped C60·2CHBr3.展开更多
基金supported by the National Natural Sci-ence Foundation of China(No.22174135,No.21790352)the National Key R&D Program of China(No.2021YFA1500500,No.2016YFA0200600)+4 种基金the Strategic Priority Research Program of Chinese Academy of Sciences(No.XDB36000000)Anhui Initiative in Quantum Information Technologies(No.AHY090100)CAS Project for Young Scientists in Basic Research(No.YSBR-054)Innovation Program for Quantum Science and Technology(No.2021ZD0303301)the Fundamental Research Funds for the Central Universities.
文摘Double-resonance Raman(DRR)scattering in two-di-mensional(2D)materials describes the intravalley or intervalley scattering of an electron or a hole excited by incident photons.Although the presence of defects can provide additional momentum and influence the scat-tering process involving one or two phonons,only the idealized defects without any structural details are considered in tra-ditional DRR theory.Here,the second-order DRR spectra of WSe_(2) monolayer with different types of defects are calculated involving the combinations of acoustic and optical phonons in the vicinity of K(K')and M points of the Brillouin zone.The electronic band structures are modified due to the presence of defects,and the band unfolding method is adopted to show the bending of valence and conduction bands for the defective WSe_(2) monolayers.The associ-ated phononic band structures also exhibit different changes in phonon dispersion curves,re-sulting in different DRR spectra corresponding to the different types of defects in the WSe_(2) monolayers.For example,the existence of W vacancy in the WSe_(2) monolayer would result in downshifts in vibrational frequencies and asymmetrical broadenings in linewidths for most combination modes due to the dramatic changes in contour shape of electronic valleys at K and K'.Moreover,the scattering from K to Q is found to be forbidden for the two Se vacan-cies because of the elevation of conduction band at the Q point.Our work highlights the role of defect structures in the intervalley scattering and may provide better understanding in the underlying physics of DRR process in 2D materials.
文摘Investigation on vibrational excitation and relaxation process will provide important in- formation for a better understanding of ultrafast dynamic response of energetic materials. Using sub-ps time-resolved coherent anti-Stokes Raman scattering (CARS) experiments, we directly observe excitation of vibrational mode vs(NO2) and its relaxation process of ground state HNS (2,2',4,4',6,6'-hexanitrostillbenein) in solution. The results show that vs(NO2) at 1385 cm-1 has been excited and relaxation time of 0.38 and 8.5 ps is obtained. The possible quantum beat frequencies are also discussed via fs-CARS experiments. The original results provide an insight into ultrafast process of energetic materials.
基金Project supported by the Ministry of Science and Technology of China(Grant Nos.2016YFA0300504 and 2017YFA0302904)the National Natural Science Foundation of China(Grant Nos.11474357,11774419,11604383,and 11704401)supported by the Scientific Equipment Development Project of Chinese Academy of Sciences(Grant No.YJKYYQ20170027)
文摘Raman scattering is a versatile and powerful technique and has been widely used in modern scientific research and vast industrial applications. It is one of the fundamental experimental techniques in condensed matter physics, since it can sensitively probe the basic elementary excitations in solids like electron, phonon, magnon, etc. The application of extreme conditions (low temperature, high magnetic field, high pressure, etc.) to Raman scattering, will push its capability up to an unprecedented level, because this enables us to look into new quantum phases driven by extreme conditions, trace the evolution of the excitations and their coupling, and hence uncover the underlying physics. This review contains two topics. In the first part, we will introduce the Raman facility under extreme conditions, belonging to the optical spectroscopy station of Synergetic Extreme Condition User Facilities (SECUF), with emphasis on the system design and the capability the facility can provide. Then in the second part we will focus on the applications of Raman scattering under extreme conditions to a variety of condensed matter systems such as superconductors, correlated electron systems, charge density waves (CDW) materials, etc. Finally, as a rapidly developing technique, time-resolved Raman scattering will be highlighted here.
基金supported by the National Natural Science Foundation of China(Grant No.10074053)the Natural Science Foundation of Zhejiang Province(Grant No.100019).
文摘C60·2CHBr3 polycrystalline powder was prepared by the solution method. The vibrational modes of the sample were studied by Raman scattering and infrared adsorption techniques. The Raman spectra showed that the Ag modes were downshifted by 4-5 cm1, while the Hg(1) mode was unshifted. The analyses of the downshifts of the Ag modes revealed that a small amount of electrons were transferred from the hydrogen atoms to the C60 molecules. In the infrared spectra, the F1u modes of the pristine C60 were unshifted after the intercalation with CHBr3. However, the vibrational modes of CHBr3 changed remarkably. The C-Br stretching mode was downshifted by ~4 cm1. The adsorption of the C-H twisting mode was weakened obviously, and the adsorption of the C-H stretching mode was not observed. These results exhibited that there were nonnegligible interactions between CHBr3 and C60 molecules, and that the strongest interaction took place between the hydrogen atoms and the C60 molecules. The interaction should induce not only the changes of the vibrational modes reported here, but also those of the electronic states. So this work should offer important glues to the mechanism of the superconductivity at 117 K of the field-doped C60·2CHBr3.