A novel scheme is proposed for sequential cooling of rotation, translation, and vibration of molecules. More generally, this scheme manipulates and controls the states and energies of molecules. The scheme, while somewhat complex, is simpler and more feasible than simply providing a large number of synchronously but independently tunable lasers. The key component is a multiple single frequency laser (MSFL) in which a single narrow band pump laser generates an ensemble of resonant ‘‘stimulated Raman’’ (RSR) sidebands (subsequently amplified and selected) in a sample of the molecules to be cooled. Starting with a relatively cold molecular sample (e.g., a supersonic beam of Cs2), the rotation of molecules is cooled by sequential application of P branch electronic transition frequencies transverse to the molecular beam beginning at higher rotational angular momentum J. Then translation of molecules is cooled by application of multiple low J, P, and R branch transition frequencies which counterpropagate with the molecular beam and are synchronously chirped over their Doppler profiles. Finally, vibration of molecules is cooled by blocking the R(0) line of the 0–0 band. Only this specific order of rotation–translation–vibration appears feasible (using molecules produced by photoassociation of ultracold atoms avoids the requirement for translational cooling). Each step employs true dissipative cooling (i.e., reduction of system entropy in three degrees of freedom) by spontaneous emission and should yield a large translationally cold sample of molecules in the lowest (v=0, J=0) level of the ground electronic state, suitable for studies such as molecule trapping, ‘‘molecule optics,’’ or long range intermolecular states.

Pulsed laser oscillation in the B1Πu→X1Σ+ g transition of Na2 pumped by a dye laser AIP Conf. Proc. 191, 91 (1989); 10.1063/1.38587Laser induced bound-bound and bound-continuum emission of the Sr2 A 1Σ+ u -X 1Σ+ g systemWe report an interesting spectrum ofN~ excited by a Kr+ 15682 A) laser which shows a long series of R-P doublets in the region 5600-8000 A and a continuum with three very broad maxima beyond 8000 A. Our spectral analysis reveals that the laser populates the v' = 34, J' = 50 level in theA II: state from where Na, molecules fluoresce not only to the bound vibrational levels of the entire ground state potential well 13 ~ v' ~ 56) but also to the continuum levels above the well. We have made an independent theoretical quantitative prediction of the continuous emission and the agreement between experiment and theory is found to be excellent. Almost the entire (99.6%) ground state RKR potential is constructed using the bound state experimental data which leads to a more accurate value of the dissociation energy (D;' = 6024±6 em-I). The feasibility of a continuously tunable near infrared N~ laser based upon this radiative dissociation process is discussed. Finally, we present a comprehensive bibliography for the N~ molecule similar to that given by Hessel and Vidal for Li, [J. Chem. Phys. 70, 4439 (1979)].

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A scheme is proposed for making highly rotationally excited diatomic molecules (“super rotors”) in their ground vibrational and electronic state, e.g., 6Li2X 1Σg+ (v=0,J⩾115) where the rotational energy exceeds the bond strength (E(0,J)−E(0,0)⩾D00). Such levels, while strictly speaking quasibound, have very long tunneling lifetimes (>1011 s for J⩽130), and should have very interesting and unique collisional properties, especially at low temperature. The rotation of the molecules is “spun up” by sequential irradiation by R branch photons in the A 1Σu+–X 1Σg+ bands starting with cold molecules at low J. Spontaneous emission to other vibrational levels is overcome by using a pump laser and its multiple Raman sidebands as in previous work on “spinning down” diatomics.

This paper reports the experimental observation of the 2 3Σ+g, 3 3Σ+g, and 4 3Σ+g states of 7Li2 by cw perturbation facilitated optical–optical double resonance spectroscopy. Molecular constants and RKR potential curves have been obtained. Our experimental Te and Re for the 2 3Σ+g state are 27 297.45(16) cm−1 and 3.0797(18) Å, respectively, and for the 3 3Σ+g state are 31 043.93(53) cm−1 and 3.0378(19) Å, respectively. The above values are in very good agreement with theoretical calculations. Hyperfine splitting for both states has been resolved. Both states follow Hund’s case (bβS) hyperfine coupling scheme. The experimental Fermi contact parameter, bF, is approximately 96±2 MHz for the 2 3Σ+g state and 95.6±3 MHz for the 3 3Σ+g state. These values are in good agreement with the previously obtained value 98.6±4 MHz [Li et al., J. Chem. Phys. 96, 3342 (1992)]. One level of the 4 3Σ+g state has been observed and its hyperfine structure has been resolved and characterized with Hund’s coupling case (bβS).

Surface plasmon polaritons launched at concentric arcs can be focused into a subwavelength wide focal spot of high near-field light intensity. The focused plasmons give rise to enhanced Raman scattering from R6G molecules placed in the focal area. By exploiting the polarization dependence of the focusing the authors establish an enhancement of the Raman signal by a factor of ∼6. The results show that focusing of propagating surface plasmons on flat metal surfaces may be an alternative to localized plasmons on metal nanostructures for achieving enhanced Raman scattering. In particular, a flat metal substrate enables better control over the local electric fields and the placement of analyte molecules, and, therefore, ultimately better fidelity of Raman spectra.

Resolved fluorescence from the K2 43 Σ+g state to the a3 Σ+u state has been measured by the perturbation-facilitated optical–optical double resonance (PFOODR) technique. Data have been fit to an improved set of molecular constants for the a3 Σ+u state. In particular, the new Te value for this state has been determined as 4197.935±0.047 cm−1, nearly 1.8 cm−1 higher than previously reported. By combining the new results for the a3 Σ+u state and the recent results for the ground X1 Σ+g state [J. Chem. Phys. 103, 3350 (1995)], we report in this paper an improved analysis of long-range dispersion and exchange interactions between two K atoms and of the X1 Σ+g and a3 Σ+u state dissociation energies De of 4450.674±0.072 cm−1 and 252.74±0.12 cm−1, respectively.