We theoretically investigate the Autler-Townes （AT） splitting in the photoelectron spectra of three-level ladder K2 molecule driven by a pump-probe pulse via employing the time- dependent wave packet approach. The d...We theoretically investigate the Autler-Townes （AT） splitting in the photoelectron spectra of three-level ladder K2 molecule driven by a pump-probe pulse via employing the time- dependent wave packet approach. The dependence of AT splitting on two laser intensities and wavelengths are studied in detail. We firstly quantify these effects on peak shift and AT separation. The photoelectron spectra show double splitting with symmetric profiles, but with asymmetric profiles when the wavelength is changed. The magnitude of AT splitting increases with the pump laser intensity, but does not vary with probe intensity. The shifts of the absorption peaks and the splitting between AT doublet are predicted by using an analyt- ical fitting function when the intensity/wavelength of one of the two fields is changed. These novel results are of importance for the molecular spectroscopy and may further stimulate the first principles theoretical studies analytically.展开更多
A perturbation theory model that describes splitting of the spectra in highly symmetrical molecular species in electrostatic field is proposed. An anahrmonie model of a two-dimensional oscillator having Kratzer potent...A perturbation theory model that describes splitting of the spectra in highly symmetrical molecular species in electrostatic field is proposed. An anahrmonie model of a two-dimensional oscillator having Kratzer potential energy function is used to model the molecular species and to represent the unperturbed system. A selection rule for the radial quantum number of the oscillator is derived. The eigenfunctions of a two-dimensional anharmonic oscillator in cylindrical coordinates are used for the matrix elements representing the probability for energy transitions in dipole approximation to be calculated. Several forms of perturbation operators are proposed to model the interaction between the polyatomic molecular species and an electrostatic field. It is found that the degeneracy is removed in the presence of the electric field and spectral splitting occurs. Anharmonic approximation for the unperturbed system is more accurate and reliable representation of a reaJ polyatomic molecular species.展开更多
Optical absorption bands at -18772 and -18807 cm-1, previously assigned to A2A-X2H electronic origin band transitions of the linear carbon-chain radicals CsH and CsD, respectively, have been reinvestigated. The spectr...Optical absorption bands at -18772 and -18807 cm-1, previously assigned to A2A-X2H electronic origin band transitions of the linear carbon-chain radicals CsH and CsD, respectively, have been reinvestigated. The spectra have been recorded in direct absorption applying cavity ring-down spectroscopy to a supersonically expanding acetylene/helium plasma. The improved spectra allow deducing a l-CsH upper state spin-orbit coupling constant X=-0.7（3） cm-1 and a A2A lifetime of 1.65=0.3 ps.展开更多
Spontaneously bundled nanotubes assembled from chiral perylene diimide molecules exhibit greatly enhanced emission via inter-nanotube excitation energy transfer. The formation of densely packed superstructures is an e...Spontaneously bundled nanotubes assembled from chiral perylene diimide molecules exhibit greatly enhanced emission via inter-nanotube excitation energy transfer. The formation of densely packed superstructures is an effective approach for high fluorescence quantum yield in assembled nanomaterials without compromising optoelectronic properties.展开更多
基金The code used in our calculation is provided by Pro- fessor Ke-li Han from Dalian Institute of Chemical Physics, Chinese Academy of Science, and we appreci- ate his help and kind advice. This work was supported by the National Natural Science Foundation of China （No.11447020）, the Natural Science Foundation of Hu- nan province （No.2015JJ3104）, and the Scientific Re- search Foundation for the Returned Overseas Chinese Scholars, State Education Ministry.
文摘We theoretically investigate the Autler-Townes （AT） splitting in the photoelectron spectra of three-level ladder K2 molecule driven by a pump-probe pulse via employing the time- dependent wave packet approach. The dependence of AT splitting on two laser intensities and wavelengths are studied in detail. We firstly quantify these effects on peak shift and AT separation. The photoelectron spectra show double splitting with symmetric profiles, but with asymmetric profiles when the wavelength is changed. The magnitude of AT splitting increases with the pump laser intensity, but does not vary with probe intensity. The shifts of the absorption peaks and the splitting between AT doublet are predicted by using an analyt- ical fitting function when the intensity/wavelength of one of the two fields is changed. These novel results are of importance for the molecular spectroscopy and may further stimulate the first principles theoretical studies analytically.
文摘A perturbation theory model that describes splitting of the spectra in highly symmetrical molecular species in electrostatic field is proposed. An anahrmonie model of a two-dimensional oscillator having Kratzer potential energy function is used to model the molecular species and to represent the unperturbed system. A selection rule for the radial quantum number of the oscillator is derived. The eigenfunctions of a two-dimensional anharmonic oscillator in cylindrical coordinates are used for the matrix elements representing the probability for energy transitions in dipole approximation to be calculated. Several forms of perturbation operators are proposed to model the interaction between the polyatomic molecular species and an electrostatic field. It is found that the degeneracy is removed in the presence of the electric field and spectral splitting occurs. Anharmonic approximation for the unperturbed system is more accurate and reliable representation of a reaJ polyatomic molecular species.
文摘Optical absorption bands at -18772 and -18807 cm-1, previously assigned to A2A-X2H electronic origin band transitions of the linear carbon-chain radicals CsH and CsD, respectively, have been reinvestigated. The spectra have been recorded in direct absorption applying cavity ring-down spectroscopy to a supersonically expanding acetylene/helium plasma. The improved spectra allow deducing a l-CsH upper state spin-orbit coupling constant X=-0.7（3） cm-1 and a A2A lifetime of 1.65=0.3 ps.
基金supported by the National Natural Science Foundation of China(21577147,21221002,21590811,21322701)the“Youth 1000 Talent Plan”Fund,the National Basic Research Program of China(2013CB632405)the“Strategic Priority Research Program”of the Chinese Academy of Sciences(XDA09030200)
文摘Spontaneously bundled nanotubes assembled from chiral perylene diimide molecules exhibit greatly enhanced emission via inter-nanotube excitation energy transfer. The formation of densely packed superstructures is an effective approach for high fluorescence quantum yield in assembled nanomaterials without compromising optoelectronic properties.
