Experimental and numerical study of self-induced transparency in a neon absorber

Self-induced transparency on the neon transition 2s ₂(J=1)–2p ₄(J=2) is studied both experimentally by investigating the propagation of 3-nsec laser pulses at 1.15 µm in an absorber discharge and theoretically by a numerical integration of Bloch's equations and the wave equation.—The application of linearly and circularly polarized light corresponds to the interaction with a quasi-nondegenerate and degenerate transition, respectively. Pulse shapes, delays, and transmittancevs. input peak intensity are found in quantitative agreement with the calculated data. While with linear light polarization all SIT characteristics clearly appear, with circular polarization the pulse break-up and the oscillation of transmittance due to optical nutations are washed out.—The homogeneous linewidth derived from pulse delay data agrees with the value from conventional measurements. The results prove SIT useful as a quantitative spectroscopic method.Work supported by the Deutsche Forschungsgemeinschaft     

Effect of polarization on population transfer in H2 by stimulated Raman transition with partially overlapping laser pulses

Polarization effects on population transfer by stimulated Raman transition using overlapping time dependent pump and Stokes laser pulses from the ground X ¹Σ _g ^/+ (v _g=0, J _g=1) level of H₂ to the final X ¹Σ _g ^/+ (v _f=1, J _f=1) level via the intermediate B ¹Σ _u ^/+ (v _i=14, J _i=0,2), C ¹Π _u ^/+ (v _i=3, J _i=2) and C ¹Π _u ^/− (v _i=3, J _i=1) levels have been theoretically investigated by applying the density matrix formalism. We have studied in detail the dependence of the population transfer on time delay between two pulses for the cases of on-resonance excitations considering linear parallel and same-sense circular polarizations of the fields. The pump and Stokes fields are taken as having Gaussian pulse shapes with peak intensities I _P ^/0 (I _S ^/0 )=2 × 10⁶ and 1 × 10⁷ W/cm². Density matrix equations have been solved for each value of the magnetic quantum number M _g(0, ±1) of the initial ground level taking into account the M _g dependence of the Rabi frequencies. M _g — averaged population transfer to the final level has also been calculated. For resonance excitations to the B(14, 0) or C(3, 1) levels, appreciable population transfer is achieved for intuitive pulse order for some particular values of M _g and M _i (magnetic quantum number of the resonant intermediate level) depending on the nature of polarizations. The calculated values of M _g — averaged population transfer for the two cases of polarizations show that for on-resonance excitation to the B(14, 0) or the C(3, 1) level, linear parallel polarization of the laser fields yield more transfer efficiency whereas for resonance excitation to the B(14, 2) level, larger population transfer results from the same-sense circular polarizations. For resonance excitation to the C(3, 2) level, M _g — averaged population is found to be almost polarization independent. The calculations for the six-level H₂ system reveal some interesting features of polarization effects on the population transfer efficiency.     

Study of in flight

An analysis of data on is presented at beam momenta 600 to 1940 MeV/c. There is evidence for an I=1, J^PC=2⁻⁺ resonance in ηηπ⁰ with mass M=1880±20 MeV and width 255±45 MeV, decaying strongly to a₂(1320)η; it is too strong to be explained as the high mass tail of π₂(1670)→a₂(1320)η. There is tentative evidence also for weak decays to f₀(1500)π. It makes a natural partner to the η₂(1860).     

Contribution of hexadecapole alignment to the polarization of quadrupole emission under laser excitation conditions

The linear polarization of quadrupole emission by the J=2-J ₀=0 transition under conditions of laser excitation in a gas medium is studied. Cases of excitation through dipole and quadrupole absorption of monochromatic laser radiation are considered. Taking into account the anisotropy of collisional relaxation, the contributions of polarization moments of the second and fourth ranks, i.e., those with usual and hexadecapole alignments, to the signal of linear polarization of quadrupole emission are calculated. The dependence of this signal on the laser frequency, the density of the gas medium, and the angles determining the orientation of the system of axes of observation of light polarization relative to a laser ray is studied. The numerical calculations of contributions of usual and hexadecapole alignment to the signal of linear polarization are made for the magnetic quadrupole transition J=2-J ₀=0 between the states 2p ⁵(² P ₁ ^2/0 )3p′[3/2]₂ and 2p ⁵(² P ₁ ^2/0 )3s 3s′[1/2]⁰ of neon atoms in the xenon atmosphere.     

Time-Reverse ODESSA. A 1D Exchange Experiment for Rotating Solids with Several Groups of Equivalent Nuclei

A one-dimensional exchange experiment is proposed for magic-angle-spinning samples with several groups of equivalent nuclei undergoing internal exchange, such as pure reorientation, as opposed to mutual exchange. The method, which we term time-reverse ODESSA, is an extension of the recently proposed 1D ODESSA experiment for a single group of exchanging nuclei. When several different groups of spins are present, as is usually the case for carbon-13 in polymers and molecular crystals, the normal ODESSA spectrum yields phase-twisted spectra which are difficult to analyze quantitatively. This problem is solved in the time-reverse ODESSA experiment which yields pure absorption spectra for all families of side bands, as long as only internal exchange need be considered. The experiment consists of the usual three pulse sequence of 2D exchange,P1—t₁—P2—τ_m—P3—t₂(acquisition), except that the evolution time is fixed at half a rotation period,t₁= T_R/2, the mixing time is set to an odd number of half rotation periods, τ_m= (2G− 1)T_R/2, and the acquisition starts att₂= T_R/2 after the detection pulse,P3. The method is demonstrated using the carbon-13 spectra of dimethyl sulfone and an enriched sample of tropolone, and is applied to the study of the π flip of the inner benzene ring of 1,4-diphenoxybenzene. The scope and limitations of the method are discussed.     

Nonlinear forward scattering of resonant laser light from excited neon systems

We investigate forward scattering induced by a powerful single mode dye laser interacting with excited neon systems. We present experimental data obtained with the three transitions: 1s ₄(J=1)-2p ₃(J=0), 1s ₂(J=1)-2p ₁(J=0), and 1s ₅(J=2)-2p ₄(J=2). The lineshape dependences on the gas pressure, the laser power and the laser field fluctuations are discussed in the context of published theories. Our data resemble the calculated lineshapes in which fluctuations in the interaction processes between atoms and laser fields are taken into account. In atomic systems having more complex level degeneracies [1s ₅(J=2)-2p ₄(J=2)] signal structures expected from higher order nonlinear coherences can occur. To theoretically reproduce these lineshapes a simple J=1J=0 model is fully appropriate provided that the level with J=1 has a narrow width.     

Contribution to the Analysis of theA2←XA1“Wulf” Transition of Ozone by High-Resolution Fourier Transform Spectrometry

The analysis of the rotational structure of the high-resolution Fourier transform 0⁰₀absorption spectrum of the³A₂←X¹A₁band system of the “Wulf” transition of the isotopomer¹⁶O₃of ozone is reported for the first time. With a near pure case (b) coupling model for the upper triplet state, we have assigned a significant portion of the spectrum, mainly theF₁(J=N+ 1) andF₂(J=N) spin components, primarily in the lower frequency region of the band. The lines corresponding to theF₃(J=N− 1) component are weak at lower frequencies and heavily congested in the central and higher frequency regions of the spectrum. Perturbations and predissociation phenomena have reduced the effective lifetime of the metastable³A₂state and have also limited the number of transitions included in the least-squares fit of the band. Approximately 100 lines have been assigned in the range from 9100–9550 cm⁻¹. Three rotational, three centrifugal distortion, three spin–rotation, and one spin–spin constant were varied. The geometry of the molecule in the³A₂state, as determined from these constants, isr= 1.345 Å and θ = 98.9°, in good agreement withab initioresults.     

Measurement of Magnitude and Sign of Heteronuclear Coupling Constants in Transition Metal Complexes

Sets of specifically tailored E.COSY-type correlation experiments and double-quantum/zero-quantum (DQ/ZQ) experiments are presented which enable the determination of sign and size of small heteronuclear coupling constants across the metal center of transition metal complexes. For the octahedrally coordinated complexes, [Ru(TPM)(H)(CO)(PPh₃)]⁺[BF₄]⁻(1) and [Ir(TPM)(H)(CO)(CO₂CH₃)]⁺[BF₄]⁻(2), 14 of 15 and 15 of 15 possible two-bond scalar coupling constants across the metal center were measured, respectively, using¹⁵N and¹⁵N/¹³C enriched samples (TPM = tris(1-pyrazolyl)methane)). The reduced coupling constants²K_X-M-Y= 4π²²J/(hγ_Xγ_Y) were found to be positive when the coupled nuclei X and Y weretranswith respect to the metal center, and negative when the coupled nuclei were incisposition. The validity of this sign rule was verified forJ_CC,J_NN,J_PN,J_PC,J_CN,J_HP,J_HC, andJ_HNcouplings. Idiosyncracies associated with 2D NMR spectra for the sign determination of coupling constants with¹⁵N which lead to corrections for the signs ofJ_HN,J_PN, andJ_CNcouplings reported previously are discussed.     

Manifestation of higher polarization moments in the dipole emission under conditions of stepwise excitation and anisotropic collisions

The induction of higher polarization moments-the octupole orientation and the hexadecapole alignment—in the case of two-step excitation of atoms through dipole transitions and their manifestation in the polarization of dipole emission under conditions of anisotropic collisions are studied. For all channels of the two-step excitation process J ₀→J ₁ J, the efficiencies of production of higher polarization moments with integer and half-integer angular momenta from J=2 to J=7 through the absorption of linearly or circularly polarized light are calculated. The rates of collisional relaxation and interconversion of higher polarization moments, for both orientation and alignment, as functions of frequency detuning of the laser line from the center of the Doppler profile are calculated. The theory is illustrated by an example of two channels of excitation of the atomic state J=2 by circularly polarized light: J ₀=0→J ₁=1J=2 and J ₀=3→J 1=2 (or 3)→J=2. In the first case, the octupole orientation enhances or attenuates the signal of circular polarization depending on the laser frequency detuning. In the second case, it represents the only source producing orientation and circular polarization of the emitted light.     

Quantitative Evaluation of the Lactate Signal Loss and Its Spatial Dependence in PRESS Localized H NMR Spectroscopy

Localized ¹H NMR spectroscopy using the 90°−t₁−180°−t₁+t₂−180°−t₂−Acq. PRESS sequence can lead to a signal loss for the lactate doublet compared with signals from uncoupled nuclei which is dependent on the choice of t₁ and t₂. The most striking signal loss of up to 78% of the total signal occurs with the symmetrical PRESS sequence (t₁=t₂) at an echo time of 2/J (290 ms). Calculations have shown that this signal loss is related to the pulse angle distributions produced by the two refocusing pulses which leads to the creation of single quantum polarization transfer (PT) as well as to not directly observable states (NDOS) of the lactate AX₃ spin system: zero- and multiple-quantum coherences, and longitudinal spin orders. In addition, the chemical shift dependent voxel displacement (VOD) leads to further signal loss. By calculating the density operator for various of the echo times TE=n/J, n=1, 2, 3, …, we calculated quantitatively the contributions of these effects to the signal loss as well as their spatial distribution. A maximum signal loss of 75% can be expected from theory for the symmetrical PRESS sequence and TE=2/J for Hamming filtered sinc pulses, whereby 47% are due to the creation of NDOS and up to 28% arise from PT. Taking also the VOD effect into account (2 mT/m slice selection gradients, 20-mm slices) leads to 54% signal loss from NDOS and up to 24% from PT, leading to a maximum signal loss of 78%. Using RE-BURP pulses with their more rectangular pulse angle distributions reduces the maximum signal loss to 44%. Experiments at 1.5 T using a lactate solution demonstrated a maximum lactate signal loss for sinc pulses of 82% (52% NDOS, 30% PT) at TE=290 ms using the symmetrical PRESS sequence. The great signal loss and its spatial distribution is of importance for investigations using a symmetrical PRESS sequence at TE=2/J.     

The Electric Dipole Moment of the CO2–CO van der Waals Complex

Radiofrequency transitions withinK= 2 asymmetry doublets have been observed for the CO₂–CO van der Waals complex. A Stark effect measurement on theJ= 2,K= 2 transition provides an electric dipole moment of μ = 0.2493(1) D. Combining this result with the permanent moment of CO, μ_CO= 0.1098 D, gives a change of moment on complex formation of Δμ = 0.140 D. The sign of Δμ is such that the CO end of the complex is more positive than CO₂. The origin of Δμ should not be attributed to any single mechanism, and several different contributions to Δμ are discussed.     

High-resolution infrared spectra of HCF3 in the ν6 (500 cm) and 2ν6 (1000 cm) regions: rovibrational analysis and accurate determination of the ground state constants C0 and DK

The high-resolution infrared spectrum of HCF₃ was studied in the ν₆ fundamental (near 500 cm⁻¹) and in the 2ν₆ overtones (near 1000 cm⁻¹) regions. The present study reports on the analysis of the hot bands in the ν₆ region, as well as the first observation and assignment of the 2ν₆² perpendicular band. Using ν₆, 2ν₆^±2–ν₆^±1 and 2ν₆² experimental wavenumbers, accurate coefficients C₀ and D_K⁰ of the K-dependent ground-state energy terms were obtained, using the so-called “loop method.” Ground-state energy differences Δ(K,J)=E₀(K,J)−E₀(K−3,J) were obtained for K=3–30. A least-squares fit of 81 such differences gave the following results (in cm⁻¹): C₀=0.1892550(15); D_K⁰=2.779(26) × 10⁻⁷.     

High-resolution infrared and millimeterwave spectra of the v3=1 vibrational state of NF3 at 907 cm

The ν₃^±1 perpendicular band of ¹⁴NF₃ ( cm⁻¹) has been studied with a resolution of 2.5 × 10⁻³ cm⁻¹, and 3682 infrared (IR) transitions (J_max=55, K_max=45) have been assigned. These transitions were complemented by 183 millimeterwave (MMW) rotational lines (J_max=25, K_max=19) in the 150–550 GHz region (precision 50–100 kHz). The kl=+1 level reveals a strong A₁/A₂ splitting due to the l(2,2) rotational interaction (q=−4.05 × 10⁻³ cm⁻¹) while the kl=−2 and +4 levels exhibit small A₁/A₂ splittings due to l(2,−4) and l(0,6) rotational interactions. All these splittings were observed by both experimental methods. Assuming the v₃=1 vibrational state as isolated, a Hamiltonian model of interactions in the D reduction, with l(2,−1) rotational interaction (r=−1.96 × 10⁻⁴ cm⁻¹) added, accounted for the observations. A set of 26 molecular constants reproduced the IR observations with σ_IR=0.175 × 10⁻³ cm⁻¹ and the MMW data with σ_MMW=134 kHz. The Q reduction was also performed and found of comparable quality while the QD reduction behaved poorly. This may be explained by a predicted Coriolis interaction between v₃=1 and v₁=1 (A₁, 1032.001 cm⁻¹) which induces a slow convergence of the Hamiltonian in the QD reduction but has no major influence on the other reductions. The experimental equilibrium structure could be calculated as: r_e(N–F)=1.3676 Å and (FNF)=101.84°.     

Electrical properties of doped 3-tetradecylpolypyrrole/metal devices

The electrical properties of devices made of doped 3-tetradecylpolypyrrole (PPy-C₁₄) thin films sandwiched between indium-tin-oxyde (ITO) and gold metal electrodes are reported. The current density–voltage (J–V) curves are asymmetric and nonlinear implying a non Ohmic rectifying contact. Using standard thermionic emission theory (Schottky) J–V characteristics were satisfactorily fitted with a saturation current of J₀=1.5×10^-5 A cm^-2, a barrier height of ϕ_b=0.7 eV, and an ideality factor of n=5.3. Characteristics from the plot of J–V versus 1/T show that the activation energy of the thermionic emission process is higher below the glass transition temperature of PPy-C₁₄ (T_g=45 °C) than above, which seems to indicate that the hopping conduction process is enhanced at T>T_g. The carrier concentration has been calculated from capacitance–voltage (C-V) measurements (N=1.9×10¹⁷ cm^-3) allowing estimation of the carrier mobility μ=2.6×10^-2 cm² V^-1 s^-1. PACS 73.61.Ph; 73.40.Sx; 73.30.+y     

Correlation inequalities and the Kosterlitz-Thouless transition for anisotropic rotators

I give a proof of the Kosterlitz-Thouless transition for sufficiently anisotropic (J _zJ _x ^–1 =J _zJ _y ^–1 <2q ^–(JKT)^–J) two-dimensionalN-component rotators (N 3). The method is based on Wells' inequality and is related to mean field Gaussian inequalities.     

Observation of the π(1800) and (1880) mesons in decay

A partial-wave analysis of the reaction π⁻p→ηηπ⁻p at 18 GeV/c has been performed on a data sample of approximately 4000 events obtained by Brookhaven experiment E852. The J^PC=0⁻⁺π(1800) state is observed in the a₀(980)η and f₀(1500)π decay modes. It has a mass of 1876±18±16 MeV/c² and a width of 221±26±38 MeV/c². The J^PC=2⁻⁺π₂(1880) meson is observed decaying through a₂(1320)η. It has a mass of 1929±24±18 MeV/c² and a width of 323±87±43 MeV/c². Both states are potential candidates for non-exotic hybrid mesons.     

High-resolution infrared spectrum and analysis of the ν2 band of CF3Cl

The rotational structure of the ν₂ band of CF₃Cl, with natural isotopic abundance, has been investigated using a tunable diode laser spectrometer. The spectra have been obtained for a low-temperature (200 K) sample, to reduce the interfering contributions of hot-band transitions. Due to the very small value of the (ΔA − ΔB) constant for both isotopic species, the K structure of most P(J) and R(J) multiplets is generally not resolvable. Only for CF₃³⁵Cl, the K structure could be resolved for P(J) multiplets with J≥55. Molecular constants for the ν₂ fundamental of both isotopic species have been obtained using least-squares fitting routines in combination with band contour simulations for unresolved K structure.     

High-resolution infrared study of the 2ν3 (A1, E) and ν1 + ν3 (E) bands of NF3

The 2ν₃ overtone (A₁, E) and the ν₁ + ν₃ (E) combination bands of the oblate symmetric top ¹⁴NF₃ were studied by FTIR spectroscopy with a resolution of 2.5 × 10⁻³ cm⁻¹. Nearly 500 lines up to K_max/J_max = 30/43 were observed for the weak A₁ component reaching the v₃ = 2⁰ substate (1803.1302 cm⁻¹), the majority of which corresponded to reinforced K = 3p-type transitions. For the strong E component reaching the v₃ = 2^±2 substate (1810.4239 cm⁻¹), about 3550 transitions were assigned up to K_max/J_max = 65/69, favoring a clear observation of the ℓ(4, −2) and ℓ(4, 4) splittings within the kℓ = −2 and +4 sublevels, respectively. The two v₃ = 2 substates are linked by the ℓ(2, 2)- and ℓ(2, −1)-type interactions, providing severe crossings, respectively, at K′ = 6 and near K′ = 24 on the v₃ = 2⁺² side. A model working in the D-reduction and including all these ℓ-type interactions could reproduce together 3695 nonzero weighted experimental data (NZW) through 33 free parameters with a standard deviation of σ = 0.357 × 10⁻³  cm⁻¹. As for the ν₁ + ν₃ (E) combination band, about 3690 lines were assigned up to K_max/J_max = 45/55. Its v₁ = v₃ = 1 upper state (1931.577 5 cm⁻¹) was treated using the same model recently applied to the v₃ = 1 (E, 907.5413 cm⁻¹) state. It yielded 21 free parameters through 3282 NZW experimental data, adjusted with σ = 0.344 × 10⁻³  cm⁻¹ in the D-reduction. For the two excited states, the small and unobserved ℓ(0, 6) interaction was tested as useless. To confirm the adequacy of the vibrationally isolated models used, some other reductions of the Hamiltonian were tried. For the v₃ = 2 state, the D-, L-, and LD-reductions led to similar σ’s, while the Q one was not successful. For the v₁ = v₃ = 1 state, the D- and Q-reductions gave comparable σ’s, while the QD-reduction was not as good. The corresponding unitary equivalence relations are generally more nicely fulfilled for the v₃ = 2 state than for the v₁ = v₃ = 1 state. The three derivable anharmonicity constants in cm⁻¹ are x₃₃ = −4.1528, g₃₃ = +1.8235 and x₁₃ = −7.9652.     

Analysis of the 2ν3 band of CD3F at 5.06 μm recorded under high resolution

The 2ν₃(A₁) band of ¹²CD₃F near 5.06 μm has been recorded with a resolution of 20–24 × 10⁻³ cm⁻¹. The value of the parameter (α^B − α^A) for this band was found to be very small and, therefore, the K structure of the R(J) and P(J) manifolds was unresolved for J < 15 and only partially resolved for larger J values. The band was analyzed using standard techniques and values for the following constants determined: ν₀ = 1977.178(3) cm⁻¹, B″ = 0.68216(9) cm⁻¹, D″_J = 1.10(30) × 10⁻⁶ cm⁻¹, α^B = (B″ − B′) = 3.086(7) × 10⁻³ cm⁻¹, and β^J = (D″_J − D′_J) = −3.24(11) × 10⁻⁷ cm⁻¹. A value of α^A = (A″ − A′) = 2.90(5) × 10⁻³ cm⁻¹ has been obtained through band contour simulations of the R(J) and P(J) multiplets.     

Evaluation method for Raman depolarization measurements including geometrical effects and polarization aberrations

In this article, we address the notoriously difficult problem to quantitatively link measured Raman depolarization values to theoretical polarizability tensor quantities, since quantum calculations do not incorporate experimental parameters. For this, we introduce a numerical model to calculate, for realistic experimental configurations, effective Raman line strength functions, Φ, which find their way into depolarization ratios, ρ. The model is based on interlinked integrations over the angles in the light collection path and a finite Raman source volume along the excitation laser beam. The model deals also with the conditional aperture parameters, associated with more than one optical component in the light collection path. Finally, we also can take into account polarization aberrations introduced by the sample cell windows. The procedure was fully tested for Raman depolarization spectra of selected hydrogen isotopologues. Distinct aspects affecting Raman depolarization data were validated, namely: (1) excitation polarization impurities; (2) extended Raman excitation volumes; (3) Raman light collection over finite solid angles; and (4) polarization aberrations introduced by optics in the light collection path. The correction of the experimental measurement data for the aforementioned effects resulted in depolarization ratios for the Q₁(J " ) Raman lines of H₂ and T₂, which mostly differed by less than 5% from those obtained by quantum‐calculations. Copyright © 2013 John Wiley & Sons, Ltd.