Coherent effects in the incoherent channel of resonant radiation scattering from excited atoms

Scattering of a resonance electromagnetic field from excited atoms cannot be described by the semiclassical theory of radiation operating with nonquantized electromagnetic fields. Field quantization effects are manifested in this case on the macroscopic level and lead to evolution of statistical properties of radiation in the course of scattering. It is found that a combined process coupling elastic scattering from an atom and induced emission from the same atom, which cannot be studied by the methods of the standard perturbation theory, plays a significant role in this effect. The process of combined scattering in extended media exhibits coherent properties that cannot be described by the standard refractive index.     

Transition radiation in the presence of excited media

The transition radiation in excited dispersing media is determined by the quantum index of refraction found in this paper. In the resonant-frequency region it is not related to the dielectric constant of the medium and cannot be calculated on the basis of the semiclassical radiation theory.Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 11, pp. 11–14, November, 1984.The author is grateful to the participants in the seminar conducted by V. L. Bonch-Bruevich for their attention to this paper.     

Investigation of the fluorescence emitted from polyallyl diglycol carbonate modified by gamma-ray radiation excited by UV radiation

The fluorescence emitted from the gamma-ray-irradiated polyallyl diglycol carbonate upon illumination by the 346 nm UV radiation is studied. The fluorescence spectra show two distinct phenomena, the variation of fluorescence wavelength and intensity with received irradiation dose. These variations are found to be correlated to the change in the dielectric constant and the change in absorption. The dielectric constant is measured at three guiding frequencies, while the absorption is predicted with the reflected first and second diffractions of the excitation monochromator. The results support the donor-bridge-acceptor molecular origin of the fluorescence.     

The b-type rotational transitions of HNCO in the lowest excited vibrational state

In the microwave and millimeter wave spectra of HNCO, the b-type transitions between the K_a = 0 and 1 levels in the lowest excited vibrational state have been observed. Because of strong a-type Coriolis resonances among the three bending excited states the energy difference between the levels for K_a = 0 and 1 is much smaller in the lowest excited state than in the ground state. The subband origin of these b-type transitions has been found in the millimeter wave region at 275 697.309 MHz (9.1963 cm^?1). The effect of the Coriolis resonances is discussed in relation to the molecular quasi-linearity and is compared with the case of HNCS.     

The structure of the triethylenediamine molecule in an excited electronic state

Ultraviolet absorption spectrum has been observed of triethylenediamine (1,4 diazabicyclo[2.2.2]octane) ($\text{D}{}_{\mathrm{<mtext>3</mtext><mtext>A</mtext><mtext>?</mtext>}}$) vapor in the 2200–2600 Å region, and an analysis has been made of its vibrational structure. The vibronic 0-0 transition was determined to be at 2513.65 Å (39782.8 cm^?1), and in the 2540–2590 Å region there were four hot bands found: two from the a₁′-type vibrational levels and two from the a₂″-type vibrational levels of the ground electronic state. The fine structures of these hot bands were examined with 0.49 Å/mm dispersion (slit width = 50 μm). For each of the two a₂″-type hot bands, a progression with 30 ～ 40 cm^?1 spacings was observed; whereas, no such progressions were found for the a₁′-type hot bands, in which absorption peaks are much more concentrated within narrow ranges. These progressions were attributed to a large-amplitude twisting motion of triethylene-diamine molecule. For explaining the whole energy-level structure, another large-amplitude motion, has been postulated. That is a double-minimum deformation motion along the molecular axis; in each minimum, one of the two NC₃ umbrellas is half-way open and the other NC₃ umbrella is half-way closed. The height of the potential barrier between these two minima has been estimated to be 1586 cm^?1.     

Nonradiative deactivation of the lowest excited triplet state of the dibenzo-<Emphasis Type="Italic">p</Emphasis>-dioxin molecule

In the nonadiabatic approximation, we study how intramolecular interactions affect the nonradiative energy degradation T ₁ ^s ↝ S ₀ of triplet sublevels s of the lowest triplet state of the dibenzo-p-dioxin molecule. We consider the role played in the degradation by the shape of promoting high- and low-frequency vibrational modes and by spin-orbit interactions separately in the carbon backbone of the molecule and in heteroatoms (oxygen). We find that σ-electrons of oxygen that correspond to the lone pair and to valence electrons play different roles in the nonadiabatic interaction.     

Excitonic light-absorption and amplification bands in the presence of laser radiation

We examine the absorption and amplification bands of a weak probe signal in the presence of Bose-Einstein condensation of excitons that emerges in nonequilibrium conditions in the field of coherent laser radiation with a wave vector k ₀. We assume that the detuning from resonance between the energy ħω _ex (k ₀)+L ₀ of the exciton level, which is shifted because of exciton-exciton interaction, and the laser photon energy ħω _L , is generally nonzero. The elementary excitation spectrum consisting of the quasiexcitonic and quasienergy branches determines the optical properties of the system. When there is real induced Bose-Einstein condensation, at the two branches touch, as they do in spontaneous Bose-Einstein condensation. In virtual induced Bose-Einstein condensation, when , instabilities emerge in the spectrum in certain regions of the k-space. These instabilities are caused by a real transformation of two laser photons into two extracondensate particles. Nonequilibrium extracondensate excitons strongly affect the absorption and amplification of the probe light signal. We show that light absorption is due to the quantum transition from the ground state of the crystal to the quasiexcitonic branch of the spectrum. On the other hand, amplification of the signal is caused by the transition from the quasienergy branch to the ground state of the crystal. The same transition can be explained by a real transformation of two laser photons into a vacuum photon of frequency ħcq and a crystal exciton with a wave vector 2k ₀−q. Finally, we show that the excitonic absorption and light-amplification bands are essentially anisotropic at and depend on the orientation of the vectors q and k ₀. Zh. éksp. Teor. Fiz. 112, 167–179 (July 1997)     

Excitation transfer between excited electronic states of the H2 molecule due to interaction with a CO2 Laser beam

A spectroscopic study of the band systemsG ¹ Σ _g →B ¹ Σ _u andI ¹ Π _g →B ¹ Σ _u of H₂ emitted by a glow discharge in H₂ gas showed that the populations of theG ¹ Σ _g (v, J) states decrease for the benefit of theI ¹ Π _u (v′, J′) states when the discharge is irradiated by a powerful CO₂ Laser beam (power density 70 kW/cm²). The effect is interpreted as an absorption process in which two Laser photons intervene according to the transition scheme:G ¹ Σ _g →B″¹ Σ _u →I ¹ Π _g. A change of the populations of excited electronic states should lead to a change of the populations of excited atomic states as well.     

Collision-induced amplification of short-wave radiation on transitions to the ground state of atoms

A new version of obtaining short-wave lasing on transition between highly excited states and the ground state of active atoms in the buffer gas atmosphere is studied theoretically. The mechanism of obtaining population inversion on such a transition is associated with the establishment of the local Boltzmann distribution of populations in a group of highly excited levels due to frequent collisions. If the excitation of the upper-lying level is performed by two laser radiation sources with frequencies ω₁ and ω₂, short-wave lasing can be obtained at a frequency close to the total frequency ω₁ + ω₂. The conditions for the emergence of population inversion are analyzed and simple analytic formulas are derived. It is shown that collision-induced enhancement of short-wave radiation can occur for pumping intensities on the order of 100 W/cm². For pumping intensities on the order of 1000 W/cm², the amplification factor for short-wave radiation may attain values of 3 cm^?1 (for an active atom concentration of N ～ 10¹⁵ cm^?3), which is sufficient for the development of lasing per path through an active medium (superradiance condition) for a length of the active medium on the order of 10 cm.     

激发态下甘氨酸与水分子间氢键性质研究

在生物体中氨基酸通常以水作为溶剂,是形成细胞的重要成分.在该环境下,分子间氢键的产生会对氨基酸分子与水分子的结构和性质产生影响.为了研究其在基态和激发态下的性质,本文利用密度泛函理论(DFT)和含时密度泛函理论(TD-DFT)对甘氨酸分子和H₂O分子在基态和激发态下的分子间氢键的静电势、键长、自然键轨道(NBO)电荷、分子中的原子理论(AIM)分析、Wiberg键级b、红外(IR)光谱、空穴-电子轨道和基态与激发态之间的电子转移进行了理论研究.结果表明：分子间氢键的形成会导致分子结构的改变和红外光谱振动频率的移动.在激发态下,分子间氢键有不同程度的增强或减弱.该计算结果为氢键的形成和激发态下分子间氢键的研究提供理论依据.     

Inversion of the Ka = 0 and 1 rotational levels in the lowest excited vibrational state of HNCS

Fairly strong, regularly spaced absorption lines have been observed in the microwave spectrum of HNCS and assigned to b-type, K_a = 0 ← 1, Q-branch transitions arising from molecules in the lowest excited vibrational state. The Fortrat diagram of these lines has the appearance of a c-type Q branch, which is impossible in HNCS because of its symmetry. This anomalous b-type Q-branch spectrum is caused by strong a-type Coriolis interactions among the three low-lying bending modes; the K_a = 1 levels of the lowest excited vibrational state are perturbed and shifted lower in energy than the K_a = 0 levels for each J. This interpretation has been confirmed by the observation of P- and R-branch transitions associated with this Q branch. The band origin has been determined to be ?40 104.287 MHz (?1.3377 cm^?1). The inversion of the K_a = 0 and 1 energy levels is consistent with the interpretation of HNCS as a quasi-linear molecule.     

The potential energy surface for the lowest quartet state of H3

SCF MO calculations with CI are carried out on the quartet state of H₃ using an extended (4s, 2p STO) basis and all single and double excitations. The ratio of 3-body to 2-body contributions to the potential at short distance is similar in the two calculations, and at 10 a ₀ the ratio is adequately described by Axilrod-Teller theory.