Spin resonant optical mixing in InSb — CW-measurements and transient effects

Optical four-wave mixing due to the resonant spin nonlinearity in n-InSb was observed in magnetic fields up to 1.4 T. The mixing of two CO-laser frequencies ω₁ and ω₂ = ω₁ - Δω yields radiation with frequencies ω₁ + 2Δω, ω₁ + Δω, ω₁ - 2Δω, and ω₁ - 3Δω. We found the resonant contribution to the third order nonlinear susceptibility arising from the spin-flip interaction to increase by more than two orders of magnitude when ω₁ is varied from 1760 cm^-1 to 1896 cm^-1. With the lasers working simultaneously Q-switched we observed radiation at ω₁ + Δω and ω₁ - 2Δω due to the mixing caused by the nonparabolicity of the conduction electrons even without an external magnetic field. At the resonant magnetic field the intensity of the mixed radiation is increased by more than one order of magnitude and is also observed when the laser pulses do not hit the sample simultaneously as long as the time difference between the two pulses does not exceed 450 ns. This points to a spin dephasing time T₂ of about 100 ns.     

Cooperative and interference effects in the resonance fluorescence of two identical three-level atoms at high photon densities

The excitation spectrum of two identical three-level atoms is considered when a strong electromagnetic field operates resonantly between two levels of the atoms. While undergoing the transition into the excited state, the atoms interact through their dipole-dipole interaction and radiate to each other as well, and subsequently, they decay radiatively into another excited state. For such a system, the spectral functions are calculated describing the cooperative and interference spectra for the symmetric and antisymmetric modes arising from the decay of the atoms from one excited state into another. In the absence of the pump field, the spectral function for the symmetric modes consists of two peaks, which are described by Lorentzian lines peaked at the frequencies ω = ω₂₃ + V_AB and ω = ω₂₃ ? V_AB and having spectral widths of the order of γ⁰₂₁ + γ⁰₂₃ and γ⁰₂₃, respectively, where ω₂₃ is the transition frequency between the two excited states, V_AB is the dipole-dipole interaction and $\text{1}\text{2}\text{γ}{}^0{}_{21}$ is the natural width for a photon spontaneously emitted from the 2 → 1 transition of an isolated atom. The splitting of the central peak for the transition in question and the broadening of the spectral widths are due entirely to the dipole-dipole and radiative interactions between the atoms. The spectral function for the antisymmetric modes describes a stable mode at the frequency ω = ω₂₃ ? V_AB, which has a delta-function distribution, and a Lorentzian line peaked at the frequency ω = ω₂₃ + V_AB and has a spectral width of the order of γ⁰₂₁. In the presence of the pump field, the spectral function for the symmetric modes contains, in addition to the central peaks, two pairs of sidebands, one pair of which is induced by the pump field with an energy shift equal to $\text{Ω}{}_{\mathrm{<mtext>a</mtext>}}\text{/√2}$, while the other pair of sidebands is due to the dipole-dipole interaction between the atoms; the probability of occurrence of the latter pair of sidebands is proportional to $\text{V}{}_{\mathrm{AB}}\text{/Ω}{}_{\mathrm{<mtext>a</mtext>}}$, while the induced energy shift is equal to $\text{3Ω}{}_{\mathrm{<mtext>a</mtext>}}\text{/√2}$, where $\text{√2Ω}{}_{\mathrm{<mtext>a</mtext>}}$ is the induced by the laser field energy shift (Rabi frequency) for a single two-level atom. The spectral widths for both pairs of sidebands are of the order of γ⁰₂₁ + γ⁰₂₃. The excitation spectrum of the antisymmetric modes consists of, in addition to the central peaks, a pair of stable sidebands, which have delta-function distributions, and two pairs of sidebands, which are similar but sharper than those for the symmetric modes. Detail comparisons are given between the one- and two-atom excitation spectra for the systems under investigation.     

Stimulated Raman spectra of a strong bichromatic field interacting with a three-level atom

We have studied the stimulated Raman spectra arising from the interaction of a three-level atom with two strong electromagnetic fields whose initially populated modes ω _a and ω _b are in resonance with the two atomic transition frequencies. The Green's function formalism has been used in the limit of high photon densities to calculate the excitation spectra near the frequencies ω = ± ω _ab = ± (ω _a - ω _b ). Expressions are derived for the relative intensities, which describe, apart from the usual Raman peak at the frequency ω = ω _ab , four pairs of lorentzian lines peaked at the frequencies ω - ω _ab = ± Ω _a /√2, ± Ω _b /√2, ± Ω and ± 2Ω, respectively, and having spectra widths of the order of 3γ₀/4. The parameter Ω is defined as Ω² = (Ω _a ² + Ω _b ²)/2, where Ω _a and Ω _b are the Rabi frequencies of the two laser fields and γ₀ is the spontaneous emission probability. Numerical calculations for selected values of the Rabi frequencies are graphically presented and discussed. Conditions have been established for which Raman gain processes are anticipated to take place.     

Coagulation equations with gelation

Smoluchowski's equation for rapid coagulation is used to describe the kinetics of gelation, in which the coagulation kernelK _ij models the bonding mechanism. For different classes of kernels we derive criteria for the occurrence of gelation, and obtain critical exponents in the pre- and postgelation stage in terms of the model parameters; we calculate bounds on the time of gelationt _c , and give an exact postgelation solution for the modelK _ij =(ij ^ω ) (ω>1/2) andK _ij =a ^i+j (a>1). For the modelK _ij =i ^ω +j ^ω (ω<1, without gelation) initial solutions are given. It is argued that the kernelK _ij ～ij ^ω with ω?1?1/d (d is dimensionality) effectively models the sol-gel transformation in polymerizing systems and approximately accounts for the effects of cross-linking and steric hindrance neglected in the classical theory of Flory and Stockmayer (Ω=1). For allΩ the exponents,t=Ω+3/2 andσ=Ω?1/2,γ=(3/2?Ω)/(Ω ? 1/2) andΒ=1, characterize the size distribution, at and slightly below the gel point, under the assumption that scaling is valid.     

Magnetopolaron states involving confined phonons in a semiconductor quantum well

Energy splitting ΔE _res in double magnetopolaron energy spectrum in rectangular quantum wells as functions of the well width d have been calculated. We have considered in the capacity of interaction leading to resonant coupling between electrons and phonons the interaction with confined phonons and (for comparison) with bulk LO phonons. We have obtained the conditions when the interaction with bulk phonons yields correct results. Calculations for AlAs/GaAs/AlAs and AlSb/InSb/AlSb structures have been performed. Alongside the parameter ΔE _res for a polaron, whose resonant magnetic field is determined by the condition Ω=ω _L1, where Ω is the cyclotron frequency and ω _L1 is the LO phonon frequency in the quantum well (A-polaron), we have calculated ΔE _res for D-(Ω=2ω _L1) and F-polarons (Ω=3ω _L1), which is a factor of $\sqrt 2 $ and $\sqrt 3 $ , respectively, smaller than ΔE _res for the A-polaron. Since the splitting ΔE _res for the A-polaron is very large (up to 0.2?ω _L1), it is more convenient to study in experiments D-and F-polarons since their resonant magnetic fields are lower. We have predicted existence of “weak” magnetopolarons, in which the splitting is proportional to a higher power of Frölich’s coupling constant α than α ^1/2.     

Relative partial photoionization cross-sections and photoelectron branching ratios of ethylene

Relative partial photoionization cross-sections and photoelectron branching ratios of the valence bands (~10–25 eV binding energy) of ethylene are reported over the photon energy ranges 18–100 eV and 21–100 eV, respectively. The four lowest ionization energy bands (1b⁻¹_1u, 1b⁻¹_1g, 3a⁻¹_g, and 1b⁻¹_2u) show monotonic cross-section decreases with photon energy from 33 eV, the 1b⁻¹_1u CC π band showing the least rapid decline. In contrast, the 2b⁻¹_3u and 2a⁻¹_g bands show almost constant cross-sections up to ~50 eV photon energy, followed by similar, although slower, monotonic decreases. This is attributed to the substantial carbon 2s character of the 2b_3u and 2a_g orbitais. The cross-section behaviour of all bands is interpreted with the aid of SCF-LCAO-MO calculations on the neutral molecule using the Gaussian-80 series of programs.     

Acoustic NMR in spin-1 systems

Acoustic magnetic resonance, both pulsed and continuous has been discussed in terms of the Bloch-Wangsness-Redfield formulation of the magnetic resonance phenomenon. The quadrupolar mechanism has been taken for the spin-phonon coupling and the mutual interaction has been treated in the ‘effective field approximation’. The expressions for the power absorbed both for Δm=±1 and Δm=±2 have been obtained. It is found that from the measurements of the relaxation parameters for Δm=±1 and Δm=±2 it is possible to estimate the non-secular contributions to the line-width. The power absorbed in pulse excitation comes out to be small for short pulse (short compared to the relaxation parameter) and it reduces to the value obtained in continuous excitation for a long pulse. It is seen that for a given pulse-width the signal decreases with the increase of the relaxation parameter and this happens as temperature is lowered. The saturation of electromagnetic signal in presence of the acoustic excitation has also been studied. The analysis indicates that the relaxation parameter obtained from the plot of the relative signal (〈〉_ω/〈〉₀) vs the acoustic frequency ω, is always less than its true value which can be determined by observing the frequency dependence of the relative fractional signal defined as [(〈〉₀?〈〉_ω)/〈〉_ω]/[(〈〉₀?〈〉_2ω0)/〈〉_2ω0].     

NO2分子的光学-光学双色双共振多光子离化谱

以Nd:YAG激光器的二倍频输出光为抽运光,其三倍频输出抽运的光学参量发生/放大器输出光为探测光,利用光学-光学双色双共振多光子离化光谱技术(OODR-MPI),获得了NO₂分子在605—675nm探测光波长范围内的多光子离化激发谱. 通过对NO₂分子离化机理的分析,确定了在此波长区间,NO₂分子经1+3+1双共振多光子过程离化,离化通道为NO₂(X²A₁)hν 关键词： 2')" href="#">NO₂ 光学-光学双共振多光子离化谱 里德伯态 分子常数     

Comparative study of the semiempirical three-parameter potential energy functions for diatomic molecules

A comparative study is made of four three-parameter semiempirical potential energy functions for 32 electronic states of diatomic molecules and their ions:n ₂:X¹gS _g ⁺ ,B ³π_g,A ³ gS_u,C ³ _u,B′ ³ gS_u.a ¹ π_g, a′gS _u ^? ,Ω ¹δ_u N ₂ ⁺ :X ² gS _g ^gS +A ² π,C ² gS _u ⁺ ,B ² gS _u ⁺ CO:X¹gS⁺,a ³ π, a′³ gS_u,e ³ gS^?,d ³gD₁,A ¹π CO⁺:X²gS⁺,A ² π,B ²gS⁺ O₂:X³gS _g ^? ,B ³ gS_u,c ¹ gS _u ^? ,b ¹gS _g ^s ,a ¹ δ_g,c ³ δ_u O ₂ ⁺ :X ²π_g,A ² π_g, a¹ π_g,b ⁴ gS _g ^? A program for numerically integrating the radial Schrödinger equation by the Cooley method is worked out. Certain additional units are introduced to conserve computer time. The resulting vibrational levels are compared with the experimental levels for all the electronic states studied. It is concluded on the basis of this analysis that it is not possible to describe equally well all the electronic states of various molecules on the basis of any single three-parameter potential function. A method for choosing a potential function for describing some particular electronic state of a diatomic molecule is proposed.     

Resonance fluorescence spectrum of two atoms,coherently driven by a strong resonant laser field

In Lehmberg's approach, we consider the resonance fluorescence spectrum of two radiatively interacting atoms. In the strong field limit we have obtained analytical solutions for the spectrum of the symmetric and antisymmetric modes without decoupling approximation. Our solutions are valid for all values of the distance r₁₂ separating the atoms. The spectrum of the symmetric modes contains additional sidebands in 2Ω (Ω is the Rabi frequency) with amplitude dependent on (a/Ω)², where a is a parameter dependent on r₁₂. The antisymmetric part of the spectrum has no additional sidebands in 2Ω. For small distances r₁₂ (a=1) our results for the symmetric modes are identical with those of Agarwal et al. apart from the so-called scaling factor. For large distances r₁₂ (a=0) the spectra of the symmetric and antisymmetric modes are identical with the well-known one-atom spectrum.     

Fluorescence spectra of matrix-isolated Se2

Laser induced fluorescence spectra are reported for samples of natural selenium and of the separated ⁷⁸Se and ⁸⁰Se isotopes in Ar and Kr matrices. The B(0_u⁺) → X(0_g⁺) and B(1_u) → X(1_g) systems of Se₂, already known in the gas, are observed by both single photon and biphotonic excitation considerably red-shifted in the matrices. The A(0_u⁺) → X(0_g⁺) emission of Se₂, not observed in the vapor, appears in the matrices with its origin near 15 100 cm^?1. Another system with ν₀₀ = 24 429 cm^?1 and ω″_e = 538 cm^?1 is thought to belong most probably to some polyatomic Se_n molecule.     

Determination of fine structure intervals in a series of excited sodium D states using doppler free two-photon spectroscopy

Using Doppler free two-photon spectroscopy technique, we have measured the absolute values of fine-structure (fs) intervals in a series of excited sodium n²D states (n = 3,6,7, and 8). We have shown the structures are inverted and our measured values for these states are: Δ_fs(3²D) = -1523 ± 8 MHz, Δ_fs(6²D) = -385 ± 5 MHz, Δ_fs(7²D) = -253 ± MHz, and Δ_fs(8²D) = -173 ± 10 MHz.     

Meson-photon transition form factors and resonance cross-sections in e+e− collisions

Meson-photon-photon transition form factors for S-, P-, and D-wave states are calculated, the meson being treated as a non-relativistic heavy-quark-antiquark pair. The full dependence on both photon virtualities is included. Cross-section formulas for charge-conjugation even mesons with J^p = 0⁻, 0⁺, 1⁺, 2⁺, and 2⁻ in electron-positron collisions are presented and numerical results for LEP energies are given. In particular, we find two-photon event rates for χ_c1, η_c(2S), and η_b(1S) within reach of LEP.With minor modifications to incorporate SU(3)-flavour breaking we estimate rates for 18 light mesons as well, based on the observation that their two-photon decay widths agree remarkably well with measured data. Finally we point out that e⁺e⁻ cross sections for 1⁺ states do not vanish at low Q², the Landau-Yang suppression factors of the two-photon cross sections being compensated by the photon propagators.     

Vibrational analysis of the a3Σ+-X1Σ+ and b3Π-X1Σ+ band systems of GeS

Spectra of GeS have been obtained in a chemiluminescent flame produced by the reaction Ge + OCS → GeS + CO. Neither of the known band systems, D¹Π-X¹Σ⁺ and E¹Σ⁺-X¹Σ⁺, was observed, but two new band systems in the regions 350–400 and 420–650 nm were obtained. By comparison with similar systems in isovalent molecules, these were assigned as b³Π₁-X¹Σ⁺ and a³Σ⁺-X¹Σ⁺, respectively. Vibrational assignments were made with the help of the germanium isotope effect and vibrational constants were obtained for the states involved. Approximate Morse potential Franck-Condon factors were computed and were shown to fit the general trend of the intensity distribution for both systems. Addition of active nitrogen to the flame was shown to increase the intensity of the b-X system by an order of magnitude while hardly affecting the a-X system. Constants (in cm^?1) obtained for the two new states are: a³Σ⁺: T_e = 21986.3 ± 2.3, ω_e = 388.9 ± 1.0, ω_ex_e = 1.35 ± 0.11; b³Π₁: T_e = 27192.0 ± 1.8, ω_e = 435.4 ± 1.1, ω_ex_e = 1.68 ± 0.20.     

Direct observation of the torsional fundamental of gaseous C2F6 in the far infrared

The forbidden a_1u torsional vibration of C₂F₆ has been observed in far-infrared absorption at 67.5 cm^?1 with an integrated intensity of 0.20 ± 0.08 × 10^?2 cm^?2. The observed intensity is compared with that expected theoretically from Coriolis coupling of the torsion to the infarred-active a_2u and e_u vibrations. For certain force fields and choices of sign for the dipole moment derivatives the agreement is satisfactory. The potential barrier to internal rotation has been recomputed from the observed torsional frequency to be 1367 cm^?1. (3.91 kcal mole^?1). This value is compared with those of ethane and partially fluorinated ethanes.     

Spectroscopy of the a3Σu + state and the coupling to the X1Σg + state of K2

We report on high resolution Fourier-transform spectroscopy of fluorescence to the a³Σ_u ⁺ state induced by two-photon or two-step excitation from the X¹Σ_g ⁺ state to the 2³Π_g state in the molecule K₂. These spectroscopic data are combined with recent results of Feshbach resonances and two-color photoassociation spectra for deriving the potential curves of X¹Σ_g ⁺ and a³Σ_u ⁺ up to the asymptote. The precise relative position of the triplet levels with respect to the singlet levels was achieved by including the excitation energies from the X¹Σ_g ⁺ state to the 2³Π_g state and the frequencies of the fluorescence down to the a³Σ_u ⁺ state in the simultaneous fit of both potentials. The derived precise potential curves allow for reliable modeling of cold collisions of pairs of potassium atoms in their ²S ground state. Electronic supplementary material Supplementary Online Material     

Time spectroscopy in theA 1 ∑ u + state of Li2. Perturbations by thea 3Π u state

We have employed time-resolved LIF spectroscopy in order to investigate perturbations in theA ¹ ∑ _u ⁺ state of the three isotopic Li₂ molecules. After a systematic check of more than 2000 individual rotation-vibration levels, 46 levels were found whose anomalous lifetimes can be interpreted by perturbations with thea ³ Π _u state. As almost all perturbed levels possess shortened lifetimes the predissociating nature of thea ³ Π _u state, caused by interaction with thex ³ ∑ _u ⁺ continuum, is revealed. On the basis of the Kovács-Budo theory of accidental predissociation we have fitted the molecular constants of thea ³ Π _u state, thex ³ ∑ _u ⁺ potential curve and the electronic parts of the perturbation matrix elements do that the observed lifetimes of all levels in the 78 investigatedA ¹ ∑ _u ⁺ ?a³ Π _u term-crossing regions can be understood.     

A photoelectron spectroscopic study of the second ionisation of the CF(X2Π) radical

The CF(X²Π) radical has been re-investigated with vacuum ultraviolet photoelectron spectroscopy. Two bands were observed and assigned to the ionisations CF⁺(X¹Σ⁺)←CF(X²Π) and CF⁺(a³Π)← CF(X²Π). The first band, which has been observed previously, has an adiabatic ionisation energy of (9.11±0.02) eV and a vertical ionisation energy of (9.55±0.02) eV. For the second band, three vibrational components were observed with the first, the most intense, at an ionisation energy of (13.94±0.02) eV. Analysis of the vibrational structure in the two observed bands allowed ω_e and r_e to be determined as 1810±30 cm⁻¹ and 1.154±0.005 Å, respectively for the first ionic state, CF⁺(X¹Σ⁺), and 1614±30 cm⁻¹ and 1.213±0.005 Å, respectively for the second ionic state, CF⁺(a³Π). Comparison of the ionisation energies and spectroscopic constants obtained has been made with values obtained from recent multi-reference configuration interaction calculations.     

On the theory of Boson peak in glasses

A universal mechanism of the Boson peak formation in glasses is proposed. The mechanism is based on the concept of interacting quasilocal oscillators. Even in the case of weak interaction, the low-frequency spectrum becomes unstable. Due to anharmonicity, the system undergoes a transition into a new stable configuration. As a result, below some characteristic frequency ω_c, proportional to the typical strength of interaction, the renormalized density of states becomes a universal function of ω with a Boson peak feature; i.e., the reduced density of states g(ω)/ω² has a maximum at a frequency ω_b?ω_c. We derive an analytic form of this function.     

Theory of transient two-photon resonant up-conversion with non-synchronized excitation

The theory of the two-photon resonant up-conversion process (ω_a + ω_a) + ω_c ? ω_d is developed for short pulse excitation. Prominence is given to the case where the pulse at frequency ω_c is not time-synchronized with the pulse ω_a but travels immediately behind it. Not only is the conversion efficiency thereby maximized, but the associated theoretical simplification enables several analytical formulae to be derived which provide new insight into the mechanism of resonant non- linear interactions. In particular, an expression is derived for the maximum useful energy per unit area of the pulse at ω_c. Exceeding this value is of little or no advantage in the non-synchronized case and is positively detrimental when the a- and c-pulses are coincident. The results are supported by computer solutions.