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Physical Review Letters

Electronic Raman Processes in Rydberg Matter of Cs: Circular Rydberg States in Cs and Cs+

Robert Svensson, Leif Holmlid

Published Aug 30, 1999• 41 citations
Publisher

Abstract

We report the first Raman study of the Rydberg matter form of Cs, using a ns pulsed dye laser. Electronic Raman anti-Stokes and mixed Stokes processes are detected in the range 290--920 nm after nonresonant excitation at 564 nm. No fluorescence is observed. The anti-Stokes transitions are from a high circular Rydberg state to a low circular state $8J$ in ${\mathrm{Cs}}^{+}$, close to $4F$ in Cs. The Stokes transitions are mixed in one more step with the laser radiation, and go from low circular states to Rydberg matter states. The transitions observed agree well with transitions in ${\mathrm{Cs}}^{+}$.

DOI
10.1103/physrevlett.83.1739

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Cambridge University Press eBooks•Sep 29, 2011•0 citations
We report the first Raman study of the Rydberg matter form of Cs, using a ns pulsed dye laser. Electronic Raman anti-Stokes and mixed Stokes processes are detected in the range 290--920 nm after nonresonant excitation at 564 nm. No fluorescence is observed. The anti-Stokes transitions are from a high circular Rydberg state to a low circular state 8J8J8J in Cs+{\mathrm{Cs}}^{+}Cs+, close to 4F4F4F in Cs. The Stokes transitions are mixed in one more step with the laser radiation, and go from low circular states to Rydberg matter states. The transitions observed agree well with transitions in Cs+{\mathrm{Cs}}^{+}Cs+.
Wave-number blueshifts of single-mode laser light in low-density Rydberg matter are found to be due to stimulated Raman processes. The Rydberg matter is mainly formed from Rydberg states of K atoms. The lasers used are mW continuous-wave lasers in the ir, lead-salt tunable diode lasers. Of special significance is the blueshifting observed as shifts of Fabry-Perot etalon fringes of the order of 0.05 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$. This blueshifting is explained as due to complete conversion to anti-Stokes radiation through higher-order stimulated Raman shifting by extremely small quanta from the near continuum of energy levels in the metallic Rydberg matter phase. Complicated strong shifts of intensity to larger wave numbers in the laser modes are also observed, due to coupling of laser side modes to the anti-Stokes waves. The high efficiency of the stimulated Raman process is partly due to the weak coupling to other degrees of freedom.
The coherent anti-Stokes Raman spectroscopy (CARS) of electronic states of the Ce3+ ion in a CeF3 crystal at 3.8 K is reported. CARS resonances involving the ground state of the 2F5/2 manifold and the Stark components of the 2F7/2 manifold at 2161 and 2239 cm−1 have been detected. Measurements were made with both visible (λ1 ≈ 476 nm, λ2 = 532 nm) and near-ultraviolet (λ1 = 355 nm, λ2 ≈ 385 nm) lasers. The enhancement of the third-order susceptibility owing to the electronic transitions, |χ(3)R/χ(3)NR|max, is as great as 4.8. This represents an order-of-magnitude increase over that in singly resonant electronic CARS experiments in other rare-earth crystals. The CARS data also yielded accurate measurements of the Ce3+ electronic Raman cross sections. In the visible region, σzz(2161 cm−1) = (5.0 ± 1.1) × 10−30 cm2 and σzz(2239 cm−1) = (1.9 ± 0.7) × 10−30 cm2. One could calculate both the absolute magnitude and the dispersion of |χ(3)R|max by modeling the virtual intermediate states as a single degenerate 5d state at 45 000 cm−1.
The first observation of nonresonant, stimulated anti-Stokes Raman emission is reported. A metastable Tl(6p2P32o)\mathrm{Tl}(6p^{2}P_{\frac{3}{2}}^{o})Tl(6p2P23​o​) inversion is created by selective photodissociation of TlCl. Raman scattering from the Tl metastable state to ground using 532- and 355-nm pump lasers resulted in stimulated emission at 376 and 278 nm, respectively. Conversion efficiencies up to 10% are reported.
The traditional Raman process alluded to in Chap. 13 is a three-state sequence of transitions in which radiative excitation (induced by a pump field) is followed by spontaneous emission that produces a final state differing from the initial state [Her50b] [Sho90, § 17.5]. When the final state of the sequence is more energetic than the initial state the resulting emission line (to the red of the pump wavelength) is known as a Stokes spectral line. The difference between the pump frequency and the Stokes frequency, the Raman frequency , defines the excitation energy of the final state relative to the initial state. When, instead, the final state has lower energy than the initial state, as can occur when the initial quantum state is already excited, then the emission is an anti-Stokes line, at a bluer wavelength than the pump field. The overall Raman scattering is a two-photon process. Typically Raman spectroscopy deals with molecules; the two-photon transitions are then between vibrational-rotational states, through electronically excited intermediate states, that are characterized in part by vibrational quantum number v and rotational angular momentum quantum numbers J, M . From any given excited electronic state there are many fluorescing transitions, corresponding to various vibrational and rotational quantum numbers of the final state. The wavelengths of the various Stokes and anti-Stokes lines (i.e. the Raman frequencies) characterize the particular molecular species, and so they have provided a valuable diagnostic tool for spectroscopists.