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Volume

17, number

OPTICS COMMUNICATIONS

June 1976

HIGH-RESOLUTION S.L. KAUFMAN

LASER SPECTROSCOPY

IN FAST BEAMS

Institut ftir Physik, Johannes Gutenberg-Universitiit, D-6500 Maim, Fed. Rep. of Germany Received 3 March 1976

A method of obtaining narrow absorption lines is proposed, based on a simple property of accelerated beams, which would yield a resolution of a few megahertz at optical frequencies. Important linewidth contributions and systematic shifts are estimated. Applications to optical and mass spectroscopy are discussed, with emphasis on investigations of short-lived isotopes.

The purpose of this paper is to point out that a velocity-bunching phenomenon occurring in fast beams of ions and atoms can be exploited to produce extremely narrow optical absorption lines. The proposed method promises a resolution of a few megahertz at optical frequencies and a sensitivity sufficient for experiments on short-lived isotopes [ I] . The large Doppler shifts [2] involved make it possible in all cases to resolve signals from different isotopes and should permit mass determinations useful in the region of nuclides far from stability. We consider first the velocity bunching and the linewidth obtainable in fast beams, including an estimate of the effects of charge-transfer collisions used to obtain fast neutral atoms. After a discussion of the unique features of the method, we describe briefly a proposed experiment to obtain isotope shifts and spectroscopic quadrupole moments of short-lived cesium isotopes. For convenience, we use as an example throughout the paper the 62S1,2-72P3,2 transition of neutral cesium (Cs 45.55). The extension to other cases will be obvious. The velocity-bunching phenomenon is a simple one occurring in most ion beams. Consider two identical ions of mass m, having velocity components in the z-direction of 0 and u0 N (2kT/m)l12. If both ions are now accelerated in the z-direction through a potential difference U, the final velocities will be, respectively, u, = (2eU/m)1/2 and

The difference in velocities is reduced, due to the acceleration, by a factor R = a(kT/eU)l12. For T = 2000 K and U = 10 kV, R = 2.1 X 10e3. The velocity distribution in the direction perpendicular to z is, of course, unchanged. The simple explanation of the bunching effect is that ions having a large initial velocity spend less time in the accelerating field and thus gain less velocity than the initially slower ions. If the fast beam is now probed along the z-direction by a parallel monochromatic beam of laser light, the width of an absorption line, neglecting all other sources of broadening, is Aoz N w,,(u,/c)R where o. is the unshifted frequency. For Cs 4555 at the above source temperature and beam energy, Ao, = 2.3 MHz. The linewidth obtainable in practice will depend upon the angular divergence A0 representing the spread of effective acceleration directions about the beam axis z. (The angular divergence of a suitably expanded, diffraction-limited laser beam is much smaller than typical ion beam divergence, and may be neglected.) The distribution of z-components of u, leads to a width Aw, = oo(uo/c) (A0)2/4R,

and the components of the thermal velocity perpendicular to the acceleration directions contribute Ao, N w,(u,/c)Af?. For an angular divergence of 309

Volume

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OPTICS COMMUNICATIONS

June 1976

5 milliradians, readily achieved in ion beams, and for Cs 4555 under the above conditions, Ao, = 3.3 MHz and Aw2 N 5.5 MHz. Since tunable lasers having suitably narrow linewidths are mainly restricted to the visible, whereas ion lines lie mostly in the ultraviolet [2] , it is important to know whether charge-transfer collisions may be used to obtain a fast beam of neutral atoms without broadening the line profile significantly. If oK is the total elastic cross section and oT the cross section for charge transfer, then OK/oT of the neutralized beam, or about 1% in the above example, will be lost due to large-angle scattering. The rest will be scattered at small angles due to the collision interaction, and will simultaneously lose energy to the collision partner. Using the potential e2 a/2r4 (charge-induceddipole interaction, atomic polarizability a) and averaging over classical impact parameters from (cK/n)122 to (oT/?r)2, one obtains the expression w (u /c> (ea/2V12 Aw c --552L-a . u;(& 112

for the rms contribution to the linewidth. The shift is of order (uK/uT)~/~ times smaller. (In the case of non-resonant charge transfer with energy defect A,, there is an additional shift 6w, = aO(ua/c) (A/2ew, which must in some cases be taken into consideration.) For Cs, using UT = 1.6 X lo-l4 cm2 and oK = 2 X lo-l6 cm2, one obtains Awe = 1.2 MHz. Since the rm4 potential certainly overestimates the deflection in the neighborhood of the lower cutoff, it may be concluded that in this and most other cases neutralization by charge transfer collisions will not significantly affect the beam quality*. A further source of line broadening and shift is the recoil momentum imparted to the atoms by the light beam. If N photons per atom on the average are absorbed from the beam and reemitted spontaneously, the resulting shift is 60, = h%/mh2 and the average rms linewidth contribution is Aw, = SwR/fi. For lines in the visible, 60~ r 1 MHz for N = M, where M is the atomic mass number. In many cases, including that of Cs 4555, optical pumping will restrict N to small values for most transitions, as dis* This conclusion and Hall [ 31. has been confirmed for one case by Snyder

cussed below. We have thus shown that the width of absorption lines for light parallel to a fast atomic beam is extremely narrow, even when angular divergence, charge transfer neutralization, and photon recoil are taken into consideration. For our example Cs 4555, the expected composite linewidth, estimated by adding all contributions including the natural linewidth in quadrature, is 7.5 MHz under the conditions specified. Except for the shift due to the energy defect in nonresonant charge transfer, all systematic shifts of the line center are of th?same order of magnitude as, or smaller than, the associated linewidth contributions. It should be pointed out that the phenomenon under discussion is similar to the energy narrowing observed in merging beam atomic collision experiments (for a review, see ref. [4]). However, the low relative velocities in such experiments increase greatly the effects of small angular divergences. Since our proposed method involves only the relative velocity c, angular divergence effects remain small as shown above. Note that the linewidth obtainable in parallel excitation is much smaller than that which would be obtained in perpendicular incidence under the same conditions. In that case, the largest term in the linewidth would be oo(ua/c) Ae, which is in our example 1.3 GHz. We now discuss some of the unique features of laser-spectroscopic experiments using this line-narrowing method. The hyperfine structure (hfs) of a spectral line may be scanned by varying the laser frequency, or alternatively, the accelerating potential. Isotopeshift determinations, of interest because of their relationship with the nuclear rms radius [5] * require a measurement of the rest frequency w. (or the center of gravity in the case of hfs) of the spectral line relative to that of some stable reference isotope. The rest frequency may be obtained by plotting the Dopplershifted frequency w against (2eu1i2 as abscissa. The intercept of the resulting straight line is wo. It should be pointed out that the second-order Doppler shift [7] is in many cases larger than the linewidth and must be taken into account. The slope of the above plot is (wo/c)m-2, which together with w. yields the mass of the atoms in the * For a recent compilation
see ref. [6].

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June 1976

beam. Viewed as a mass spectrometer, would have a resolution M/m = &+,/Aw) (u,/c),

the experiment

which is under the conditions of our example about 3 X 104. It should thus be possible using this method to make mass determinations with sufficient accuracy to be useful in the region of nuclides far from stability [8]. The mass dependence of the Doppler shift will also be useful in separating fluorescence signals in mixtures of isotopes whose lines would otherwise coincide. Since the linewidths of the proposed experiment are well matched to the widths of available singlemode dye lasers (for a review, see ref. [9]), a significant fraction of the atoms in the beam may be excited, an important feature for any experiment on short-lived isotopes. The laser power required may be estimated to be a few mW/cm2, and is in most cases limited by optical pumping, which removes the atoms from the absorbing ground state levels within a few pumping cycles. This will limit the fluorescence yield of the experiment to about one photon per atom, but insures that the effects of photon recoil discussed above remain small. For Cs 4555, the transitions (F=I+4,1mFl=F)~(F=zt~,lmFl=F) are not subject to pumping, and will be useful in searching for the fluorescence lines. For experiments on short-lived isotopes, the proposed method has the further advantage of permitting continuous and direct use of the output ion beam of an on-line mass separator, thus avoiding the losses of collection and reevaporation schemes presently in use [lo] . This feature is especially important for chemically active elements such as the alkalies [ 1 l] . Experiments are planned, using the proposed method, in which the hfs and isotope shift of the Cs 4555 line will be studied in order to obtain information on nuclear moments of short-lived cesium isotopes. We estimate the overall sensitivity of a fluorescence experiment, for transitions limited by optical pumping, as follows. it should be possible to neutralize 40% of the ion beam. If 5% of the resulting atoms are excited and emit a 4555 8, photon within the observation region, and 10% of the light is collected onto a photo-cathode having 25% quantum efficiency,

the resulting detection efficiency is 5 X 10e4 photoelectrons/incident ion. The noise level is estimated at lo3 photoelectrons/s due to scattering from a I-mW laser beam [ 121, with dark current well below this level. There results a detection threshold for a onesecond integration of 2 X lo6 Cs+/s in the incident beam. Since the quadrupole interaction will just barely be resolved by the estimated 7.5 MHz linewidth in direct fluorescence spectroscopy, it is planned to use the proposed method to excite level crossings [ 131 in the 72P3/2 state. The linewidth of the crossing signal corresponds to the natural linewidth of 1.3 MHz and will suffice for an accurate measurement [ 141, and the narrow optical profile allows excitation of isolated crossings, thus increasing the contrast of the signal from the usual l-3% to 50% or more of the fluorescent light. The author would like to acknowledge helpful discussions with R. Neugart and with E.-W. Otten, who suggested investigating the possibility of exciting level crossings with laser light parallel to a fast beam and in that way initiated this work.

References
G. 111 Huber, C. Thibault, R. Klapisch, H.T. Duong, J.L. Vialle, J. Pinard, P. Juncar and P. Jacquinot, Phys. Rev. Lett. 34 (1975) 1209. 121 H.J. Andrg, A. Gaupp and W. Wittemann, Phys. Rev. Lett. 31 (1973) 501. 131 J.J. Snyder and J.L. Hall, Proc. Second Intern. Conf. Laser Spectroscopy, Meg&e, 1975 (Springer Verlag, Heidelberg, 1975). 141 G. Dunn, in: Proc. First Intern. Conf. Atomic Physics, New York City, 1968 (Plenum, New York. 1969). [51 H. Kopfermann, Nuclear Moments; Academic Press, 1958, ch. IV. [61 K. Heilig and A. Steudel, Atomic Data and Nuclear Data Tables 14 (1974) 613. [71 H.E. Ives and C.R. Stilwell, J. Opt. Sot. Am. 28 (1938) 215; H.I. Mandelberg and L. Witten, J. Opt. Sot. Am. 52 (1962) 529. PI R. Klapisch, A. Prieels, C. Thibault, A.M. Poskanzer, C. Rigaud and E. Roeckl, Phys. Rev. Lett. 31 (1973) 118. PI M.J. Colles and C.R. Pidgeon, Rep. Prog. Phys. 38 (1975) 329. 1101 J. Bonn, G. Huber, H.-J. Kluge, U. Kiipf, L. Kugler and E.-W. Otten, Phys. Lett. 36B (1971) 41.

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[ 111 P. Freilinger, Diplomarbeit, lnstitut fiir Physik, University of Mainz, 1975, unpublished. [12] cf. W.M. Fairbank Jr., T.W. H%rsch and A.L. Schawlow, J. Opt. Sot. Am. 65 (1975) 199.

[13]

F.D. Colegrove, P.A. Franken, R.R. Lewis and R.H. Sands, Phys. Rev. Lett. 3 (1959) 420. [ 141 F. Ackermann, E.-W. Otten, G. zu Putlitz, A. Schenck and S. Ulrich, Nucl. Phys. A 248 (1975) 157.

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