JOURNAL D PHYSIQUE E C o l l o q u e C1, Suppl6ment a u n'3,

Tome 49, Mars 1 9 8 8

GENERATION OF X W SPECTRA BY POWERFUL PICOSECOND LASER C.H. NAM, W. TIGHE, S. SUCKEWER, U. FELDMAN* a n d J. SEELY'
P r i n c e t o n U n i v e r s i t y , Plasma P h y s i c s L a b o r a t o r y , P r i n c e t o n . NJ 08544, U . S . A . ' ~ a v a lR e s e a r c h L a b o r a t o r y , Washington, DC 20375, U.S.A.

ABSTRACT
The development of laser action a t wavelengths shorter than those of current X-ray lasers is being investigated along two fronts. In the first case, w e are exploring the possibilities for laser action a t 15.4 nm In Li-like AlXI and 12.9 nm in Li-like SiXIl in a magnetically confined recombining plasma. Previous work on hydrogen-like carbon, CVI, led to lasing action a t 18.2 nm. Recently, this has been applied to microscopy and first results from a soft X-ray laser microscope a r e presented. A new technique to generate shorter wavelength X-ray lasing involves the interaction of a high power laser with a preformed plasma.. The Powerful Picosecond Laser (PP-~aser)System with a n output power level o 20-30 GW and focussed power density of loi6 - 1017 f w/cm2 has recently become operational The spectra o highly ionized atoms in f the X V region were recorded on a high resolution erazing incidence U spectrometer for the PP-Laser beam interacting with different solid targets.

Extension of the operating range of soft X-ray lasers1i2 to shorter wavelengths is important for applications such a s microscopy o live biological f specimens. Earlier work a t ~ r i n c e t o n ~ - ~ resulted in a soft X-ray laser has with the following characteristics. 18.2 nm, wavelength amplification 500; 1-3 m J pulse energy; 10-30 nsec pulse duration and 5 mrad beam divergence. This work has been extended to shorter wavelengths by obtaining a population inversion and gain on the 4f-3d transition for lithium-like ions, AlXI and SiXII.

A s part o the program in which multiphoton excitation is being considered f a s a means to provide short wavelength X-ray lasing, w e present the first high-resolution X V spectra obtained by the interaction of powerful picosecond U laser pulses with solid targets. The targets were composed o elements with f atomic numbers in the range 2=3 to 2=26 and were irradiated using a KrF* laser with a pulse duration of 1.2 picosecond and focussed to an intensity o f loi6 w/cm2. The spectra in the range o 6 A to 370 A were recorded by a 3 f meter grazing incidence spectrograph with a resolving power sufficient to observe the line profiles o transitions in highly-charged ions. f
EXPERIMENTAL: SETUP AND RESULTS

In the recombination scheme, the C02 laser is focussed onto an aluminum or silicon disc and creates a plasma column which is confined by a strong (- 50 kG) magnetic field. The maximum laser power density on target is 2 x loi3 w/cm2. The plasma cools rapidly after the laser pulse and fast three-body recombination, followed by cascading processes, provides a high 4f population while the 3d level decays rapidly by the 3d+2p radirtive transitions and in this w a y a 4f-3d population inversion and gain is built up. Maximum gain occurs in the high density, low temperature off-axis regions and a slot in the target disc transmits the axial stimulated emission.

Article published online by EDP Sciences and available at http://dx.doi.org/10.1051/jphyscol:1988139

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The axial emission is imaged by a grazing-incidence mirror onto the entrance slit of a multichannel soft X-ray spectrometer. A second spectrometer views the plasma transversely. A transverse scan of the axial spectrometer gives information on the relative divergence of the st~mulated emission compared to spontaneous emission lines. In lithium-like ions the 4d-3p and A 4p-3s transitions have g values significantly less than the 4f-3d transition. (g is the statistical weight o the upper level and A is the transition probability). f In the prescence of a n = 4 to m = 3 population inversion, gain is expected to be A first apparent in the transition with the highest g value. A convenient measure of this increase is the 4f-3d intensity relative to the 4d-3p and 4p-3s transitions. The measurements indicate a maximum gain length ( g ~ )o gL = f 3-4 a t 15.4 nm and gl, = 1-2 at 12.9 nm (~i-likeS ~ X I I ) . ~ A important new avenue o research at Princeton is the application o n f f the 18.2 nm soft X-ray laser to high resolution contact microscopy. The soft X-ray laser beam is collimated by a rudimentary toroidal mirror onto a biological specimen chamber in a contact microscope. The specimen is isolated from the laser vacuum system by a silicon nitride window, 1000 thick and, during the exposure, the shadow of the specimen is recorded in PMMA-MAA copolymer photoresist. The experiment is in an early stage but experiments are planned for the near future using live cells in which the resist will be viewed at high resolution using an electron microscope. Higher quality optics and more advanced microscopes are being designed and constructed
A s part o a larger system which is being constructed for the development f of short wavelength X-ray lasers and which includes a C02 laser (1 kJ energy, 10-50 nsec pulse duration), a powerful picosecond KrF* laser has been developed and used in initial target interaction e ~ ~ e r i m e n t s . ~ > master oscillator o The ~ f the PP-laser system was a cavity-dumped dye laser tuned to a wavelength of ,648 nm. The dye laser used a hybrid mode-locking scheme and produced 1 psec pulses. The dye laser w a s pumped by the frequency-doubled output of a mode-locked Y G laser. A The output of the dye laser w a s injected into a three-stage dye amplifier that w a s pumped by amplified, frequency-doubled pulses from the Y G laser. A The amplified 648 nm pulses were frequency-doubled and, then, mixed with 1064 nm Y G pulses. The resulting A 248 nm pulses were injected into two KrF* amplifiers. The amplified pulses f typically had a n energy o 20 to 25 mJ and a duration o 1 to 1.2 psec. The f f pulses were focused by an f/5 spherical lens to a n intensity o approximately 1016 ~ / c m 2 ,

The laser pulses were incident on a rotating cylindrical target either composed or else coated with the material under study. The spectra were recorded on Kodak 101 photographic plates, and the spectra produced by up to 7000 laser shots, were integrated onto each exposure. The spectrum from a solid aluminum target is shown in Fig. la. Transitions (not shown) occurring in the low-density expansion plasma, have line widths consistent with the 30 mA instrumental broadening (resulting from the 10 pm entrance slit) and Doppler source broadening. The much larger widths of the Li-like n = 2 - 4 and n = 2 - 5 transitions shown in Fig. 1 are consistent with quasi-static ion Stark broadening at an electron density In the ~ m - . ~The same transitions in Li-like fluorine from a teflon . range 1021 target are shown in Fig. lb. These line profiles a r e asymmetric and are up to 2 A in width. It is well known that the microfield due to the plasma can cause shifts of the energy levels of emitting ions.9 In dense plasmas, when the shifts become comparable to the energy level splittings, the wave functions of neighboring states become mixed, and this permits transitions that a r e not allowed in the absence of the microfield. The ratio of the intensities of the forbidden and allowed transitions increases with plasma density.

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Figure I : High resolution XUV spectra. Figure Ial i s a r e s u l t from an a2uminz.m t a r g e t showing Li-like AIXI and Be-like AIX. Figure Ibl i s a r e s u l t from a t e f l o n target showing Li--like FVII and Be-ZikeFVI.

The line profiles were modeled using a formalism developed for the calculation of spectral line profiles of multielectron ions in dense plasmas using the quasi-static ion approximation.1 A quantum mechanical relaxation theory w a s used to calculate the piasma electron broadening of the spectral lines. The calculated profile of the F6+ 2p-3d spectral feature showed that a t electron ~ m - the, 2p-3p forbidden component contributes ~ densities greater than 5 x significantly to the red wing of the spectral feature. This is consistent with the enhanced red wing of the observed 2p-3d spectral feature shown in Fig. 2b. Similarly, the red wing of the observed 2p-4d feature is enhanced by the 2p-4p forbidden component. From numerical computations the line width and asymmetry of the observed F6+ 2p-3d spectral feature are consistent with an electron density o f ~ m - ~ . However, not all features show such agreement and approximately cannot be explained in terms of density alone. It is possible that the electric field associated with the intense laser pulse m a y also be influencing the character of the spectral emission Nevertheless, it is of interest to note that the density implied from calculations is more comparable to the critical electron density (2 x ~ m - ~ ) 248 nm laser radiation than the target for density (4 x ~ m - ~ ) Since the plasma expansion during the picosecond . laser pulse is negligible, it seems likely that the observed emission occurs in the expanding plasma immediately after the laser pulse. Furthermore, the time for collisional ionization to F6' is approximately 1 psec, and the time for n = 2-3 collisional excitation is less than a picosecond. The times for the radiative transitions 3p-2s and 3d-2p a r e 20 psec and 6 psec, respectively, and a r e much larger than the laser pulse duration. Thus it seems reasonable that the excited F6+ ions a r e formed during the picosecond laser pulse, and the bulk of the emission occurs after the laser pulse. The F5+ ionization energy is 160 eV and the F ~ + = 2-3 excitation energy is 100 eV, and it is possible that n multiphoton (nonresonance) processes, requiring a large number of 248 n m (5 eV) photons, contribute to the formation of excited F6+ during the laser pulse. Finally w e note that w i t h the iron target the presence of Na-like el" lines, representing the most highly charged ion roduced in plasmas created by a picosecond laser. The He-like ls2 - ls2p Pi resonance line of aluminum a t 7.757 A (1.6 keV excitation energy) w a s identified in the spectra from the aluminum targets (more details in Ref. 8).

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CONCLUSIONS AND FUTURE PLANS

We have demonstrated gain at 15.4 nm and 12.9 nm in a recombining X-ray laser scheme. We hope to achieve still shorter wavelength output by using higher Z elements (e.g. sulphur). Another area in which an intensive effort is being directed is the development o an X-ray laser cavity using soft f X-ray mirrors with -,40% reflectivity. We have also obtained high resolution X V spectra from the interaction o U f the powerful picosecond KrF laser system with several solid targets. Extremely broad and asymmetric line profiles were observed along with high levels o ionization. Experiments to study the effect o a prepulse on the f f interaction and with new layered targets a r e beginning. The development of a final stage amplifier For the PP-laser, which will provide much higher power levels, is proceeding.

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1. S. Suckewer, C.A. Skinner, D. Kim, D. Voorhees, and A. Wouters, Phys. Rev. Lett. 3, 1004 (1986).

D. Matthews, M. Rosen, S. Brown, N. Ceglio, D. Eder, A. Hawryluk, C. Keane, R. London, B. MacGowan, S. Maxon, D. Wilson, J. Scofield, and J . Trebes, J. Opt. Soc. Am. B & 575-587 (1987).
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S. Suckewer, C.H. Skinner, H. Milchberg. C. Keane, and D. Voorhees, 3. Phys. Rev. Lett. 1753-1756 (1985).

C.H. Nam, E. Valeo, S. Suckewer, and U. Feldman, J. Opt. Soc. Am. B 3, 4. 1199 (1986).
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, C.H. Skinner and C. Keane, Appl. Phys. Lett. & 1334 (1986).

6. C.H. Skinner, D. Kim, A Wouters, D. Voorhees, and S. Suckewer, Proc. . of SPIE 31st Int. Tech, Sym., 831 3 (1987). 6

7.

W.G. Tighe, C.H. Nam, S. Suckewer, and J . Robinson, to be published.

C.H. Nam, W.G. Tighe, S. Suckewer, J.F. Seely, U. Feldman, and L.A. 8. Woltz, Phys. Rev. Lett. 2427 (1987).
9. 10. H.R. Griem, Academic Press, New York, (1974).

L.A. Woltz and C.P. Hooper, to be published in Phys. Rev. A. (1987).