First publ.

in: Phonons 89 : Proceedings of the Third International Conference on Phonon Physiscs and the Sixth International Conference on Phonon Scattering in Condensed Matter 1989, pp. 904-906

DIRECT OBSERVATION OF RrPPLONS IN 4 ~ FILMS BY NEUTRON e SCATTERING

H . G d r i n 1, ~ . ~ . ~ . ~ r a n ~ l ,~2. ,h u t and ~ . ~ c i d e r c r ~ k. al

I Imritut Low-Langevin. BP 156X, f -38042 Grenobb, France 2 University of Komtanz, D-7750 Konrranz, West G e m a n y

.surface. Their existence in bulk 4

~ and in films has been pdiot&dby theoe'hild c indirectly confirmed by txpenment[l,2]. At long wavttcngrhs the npplon dispersion relation i s easily evaluated using bydtdynamic relatibns for an incornprcssible fluid: K? = (ua/p~) k3 where ag is the zero temperature surface tension, po thc 4He density at zero pressure and k the wavevector. 'She temperatux dependence of the surface tension ( a ( T ) ) very low at temperatures can be deduced from the ripplon dispersion relation. Detailed mcasurcments[3] of u(T) revealed a much Iarger t e m p t r a m depende~cc than expected from formula { 1 1. Several modified dispersion curves have been proposed which differ rnarnIy for wavevectors a b v e 0.5A- The idea of a 'surface roton', with a minimum at 1. -2K. was introduced by Reut and Fisher[4] improving the agrtement with the available t h e d y n a m i c data. Edwards et a1.[1,3], taking into account the curvature dependence of a. were abIt to fit the experimental data on the excess surface entropy. Their model ~nvolvestwo parameters: a length M ( E n q)/dK where K=(rl-1 + r2-1) is the curvature of the surface, and an area a = dsJdK. Within rhe precision of the enuopy data, several sets of parameters hav'e been us$ (a=+1.5A2, ~3 [ 3 ] and a=+l.,0A2, +-0.336A [ I]), the latter pving a somewhat bettkt a b e r n t b f ; Spqh f gr;$~upvation in the parameters coresponds to very different ripplon dlsptrsimEurves a wavevectors -1A-1. Little direct expenmental evtdence ISavailable[S], however, on the ripplon dispersion c w e at these wavevectars. Such a study ~ q u t r t a rmcmscopic prok like: inelastic neu'tron scattcring s (INS), but due to he low neutron cross section of 4He the measurement has to be performed on samples with a large surface to vo~urnc ratio. We have measured the melas~c r m m factor of 4Ht adsorbed on the b a d plane of s graphite. The INS measurements were performed at the tm of fligth spbcmtneter N6 at i the Instirut Laue-Langevin's reactor unng a waveltngb of 5.12A. The elasnc energy resolution depends sligthly on the momentum transfer Q due to sampfe size effects, increasing f o 80 to 1 l Y wk scanenng mgle. rm m i The sample consisted of 3T.70g of Papyex[6] sheets oriented with their c-axis normal to the scattaing plane. The temperatun of the sample was kept at 0.65Kfm all the measurements. An adequate annealing of the adsorbad films was pcrformtd a f i a each change in coverage. The rota1 surface arca was determined by adsorption isotherms and neutron diffraction to be 7 3 h 2 r 2%. The 4Hc monolayer coverage ( . 12 atorndA2) 01 was 304cc STP. The data obtained before any 4 ~ was adsorbed were used as e background and substracted from subsequent measurements. The result of two measurements will be rcported here: a) at a total coverage of0.&8atosrl~A2, equivalent roughly to 5 atomic layen and b) a scan with the cell filled wt bulk superfluid 4 ~ e . ih The first and second layers are ~ Z l d these coverages and thtu density rs well at known[7,8) / I s t Eayer=O.11 ~ a t / A 2 , 2nd 1a~cr=0.094at/A2). Thus, 0 . 2 ~ a t l A 2 correspond to the solid and the remaining amount of 4Wt to the liquid layers. WCuse a mtan density of 0.018at./b2 fora liquid layer to evaluate the thickness of the film. This v d u e has to bt laken with cart, since microscopic calculations showed that tht density of the bulk liqmd-vacuum ~nterfact decrtasts slowly whin a distance of -5Ai91.

- Quarttized capillary waves~(tipp1ons).am lf~t demcmary excitations of a frce lfquld

Konstanzer Online-Publikations-System (KOPS) - URL: http://www.ub.uni-konstanz.de/kops/volltexte/2007/2974/ URN: http://nbn-resolving.de/urn:nbn:de:bsz:352-opus-29742

The result of the mcasurtmcnt for 5 layers is depicted in figure 1 as a contour plot of n l S(Q, o)i order m give a g c n d ovuview of d channels and detectors. One can easily recognitc two excitation branches. The higher energy one agrees well with the bulk phor on-roton dispersion relation (solid linc in fig.1). The lower branch, located at about , nwr rht energy of the previous one, is the main object of this paper. Evidence of the existence o f this branch has k e n found previously on measurcments[5] done on a different substrate (Vulcan Ill graphite powder), together with the observation of dispersionless m+s. In the present experiment no dspersionlcss d e r were observed fnr Q a 1.5A-1; this may be dm to the larger coherence length o to the preferential r . sample. The absence of these flat modes enables us to oriel~tatia;t>f.our,Pyycx demmine she Iower branch dispwsion relation unambiguously up to Q 1.5A-1.
3 -

.".

Contour plat of S(Q,m) (arbitrary units) f a covetagc o 0.448atlAZ. The conuxu lines 1 t w f o 10 t 15 by 30 u .'She hick d i d linc vi thc bulk 4He p h m - r o t o n o b 9 art stparattd by 1 units. 0 dispasion relation. Thc elastic Q values arc: given in h i s & cwtgant Q lim are indicated by Lhin golid lines i the graph. The da&d Iinz uxrwporuk to Lht ripplon dispersm curve detmrned by Edwards and n Saam[l]. using a = + 1.0AZ. 6 = - 0.336A.

To determine the origin of the lower excitation branch we ptrformtd a measurement with the cell filled with bulk liquid. This procedure suppresses the Iiquid-vapour interface, but dms not affect the adsorkd solid-liquid interface. As seen in figure 2. the phonon-mton part is smngly enhanced while the peak at 0.47meV is suppessed. This is observed for all the measured spccm. Therefore, we conclude that the low energy excitation branch &longs to the liquid h e surface and is identifitd a a rippion.

The expcrimenral ripplan dispersion c m e displap a strong downward curvature and seems to m r g t with h e bulk roton minimum for 0-2k-1. Due to the high intensity of the roton signal it is difficult to follow the ripplon pcak ar rhcsc wavevcctm. Below ~=1.5A-lour result agrees well wt the calculation of Edwards and Saam[l] ih for a=+~.oAz. &=-0.336A and dms not agree with the disptrsion curves given in references 3 and 9.

Energy [meV]

FiellrL.2r I e a t c specuum (arbitrq units) nlsi

lor QrO.8A-I as a funclim of energy. Thc solid 11nt corresponds to thc measurement with coverage 0.448atlAZ (5 a m l c laycn). Thc peak at -0.47meV corresponds to h e ripplon and tht o at -1.05mV to tht bulk phomxl. Barhtd lint:samt spactrum with w the XI! lined w ~ t h bulk liqu~d; hta thc ripplon p k has now & r.* at h . Dotted lint: buJk -bum d~wded la): the pcalr at 0.75meV ts duc ro multiple a m g . by

En conclusion. we have directly determined the ripplon s p a w m at large wavevectors for rhc first hmt. With the cell filled with 4Hc, the surfact mode is suppressed, showng clearly that this excitation comesponds to the liquid-gas interface. Measurements of the temperam and coverage dcptndenct and a higher Q att in progress. t This work has been partially suppond by the West Germany Federal Minisay of R e m h and Technique (BMFT).
Edwarh D.O. and S a m W.F., Pmg. in Low Tmp.Phys.. Ed. D.F.Bmwer, 283 ( 1978), Nonh Holland Vinen W.F., Spnngcr Seriw in Sol.StSci.. Ed, K.Ohbayashi & M.Wa&, 189 (19R9). Spnngu Yerlag, Fdwards D.O.. EEkardt JR. and Gaspariru F.M.. Phys.Rcv. A 9,2070 (1974) Reut S and Fisha I .%v.Phys. IETP Z. 981 (1971) Lauter HJ.. Frank Y L P . . Gadfrin H, and Lcidertr P , Springer Series in Sol.St.Sci., Ed. . K.Ohhayashi & M.watak. m, (1989), S w g c r Vtrlag. W Papye* s podwed by C a h n c m m ,45 Rlrt dcs A d , F-75821FarisCcdcx 17 h u t e r HJ.. Schildkrg H.P.. C d r i n H.. Wltchen H. and Haenscl R , CsnJ.Phys. 61, 1435 .

w,

u,

(1987) and refmaces thatul Sch~ldbergH.P., PhD Thes~s, Kicl University. Wtst G-my, 1988 4754 (1987) K r o l s c k k E., Seingan S. and T t n r I Phys.Rev. B rte .