PROPERTIES OF METALLIC FILMS IN PRECISE CALCULATION OF THE CASIMIR FORCE 4 0 0 VITALYB. SVETOVOY 2 Transducers Science and Technology Group, EWI, University of Twente, n P.O. 217, 7500 AE Enschede, The Netherlands a J E-mail: [email protected] 7 2 Opticalpropertiesofthedepositedgoldfilmsarediscussedinconnectionwiththe Casimir force prediction. Voids in the films and electron scattering on the grain boundaries reduce the force at small separations on the 2 % level in comparison ] i withthebulkmaterialprediction. Thecontributionofthepatchpotential dueto c polycrystallinestructureofthefilmsisshowntobesmallfortheexistingCasimir s forceexperiments. - l r t m 1 Introduction . t a m Detailed investigation of the Casimir force1 between two uncharged metallic - plates, predicted in 1948, became possible only recently with the progress in d microtechnologiesallowingto controlseparationbetweenbodies smallerthan n 1 µm. The development of the experiment2,3,4,5 is characterized by steady o 2 5 c improvementintheprecisionoftheforcemeasurementfrom5% to0.25% . [ The progressintheoreticalpredictionof the forceis notso impressive. Start- 1 ing from the first precise calculations6,7,8,9 and up to now5 the force is cal- v culated using the optical properties of bulk metals taken in the handbooks. 2 However, in all the experiments the force was measured between deposited 6 metallic films. Typically it was gold with the thickness 100−200 nm. It is 5 clearthatthedepositedmaterialandbulkmaterialaredifferentifwepretend 1 0 onhigh precisioncalculations. Inthis paper the questionis analyzedto what 4 extend the properties of real deposited metallic films can change the force in 0 comparisonwiththatpredictedforthebulkmaterial. Toanswerthisquestion / t weinevitably haveto turntothe materialscience. The stepsinthis direction a never been done before but without understanding ofthe used materialthere m will be no further progress in the prediction of the Casimir force. - 1 d Originally the Casimir force was calculated between ideal metallic n plates. In this case it does not include any material parameters: F = c o π2/240 ¯hc/a4 , where a is the separationbetween plates. At small separa- c : (cid:0)tions the(cid:1)(cid:0)deviati(cid:1)on of the used metal from the ideal one becomes significant v 10 and one has to calculate the force using a more general Lifshitz formula . i X This formula takes into account real optical properties of the plate material 11 r via the dielectric function ε(ω), which is taken in the handbooks . Gold a is the best material for the force measurement since it is chemically inactive and its low frequency behavior, where the handbook data unaccessible, can 1 be reliably predicted with the Drude model. 2 Voids in the films Optical properties of Au films were investigated widely in 60th-70th. The re- 11 sults are collected in the handbooks . Significant deviation in the optical data was attributed to genuine sample differences caused by different sam- 11 11 ple preparation methods . The handbook data were carefully chosen to represent the bulk material as close as possible. A special investigation of 12 the sample preparationeffect was undertaken with the conclusion that the mostsignificantroleplayedvoidsinthesamples. Annealedfilmsdemonstrated larger density due to larger grain size. A single parameter model represent- ing voids in an otherwise homogeneous medium was shown to account for the major discrepancies in the above-band-gap (E = 2.5 eV) spectra for Au samples prepared in different ways. It allowed to get information about the volume fraction of voids f in different samples. For f ≪ 1 and |ε| ≫ 1 V V the model gave the effective dielectric function hεi defined by the relation 3 hεi = ε 1− f . For the film (150 nm) evaporated with e-beam on NaCl 2 V substrat(cid:0)e at room(cid:1) temperature with a deposition rate of 23 ˚A/s the volume of voids was found to be larger on 4% than in the annealed samples used for 11 the handbook data . For the 50 nm thick sputtered films deposited at the rate smaller than 13 ˚A/s the volume of voids was found to be 4 % at room ◦ temperature deposition and 1% at 250 C. The cleaved NaCl substrate was chosenbecause the films start to growepitaxially on it. The same conclusion 13 was made in a more recent investigation . 3 In the most sensitive experiments the Au films were evaporated or 5 sputtered at room temperature, no annealing was reported. One can 12 expect that in both cases the volume of voids was of about of 4%. The correction to the Casimir force due presence of voids was calculated 11 usingthedata forε. Thesedatawerescaledinaccordancewiththeeffective 3 dielectricfunctionhεi=ε 1− f . Calculationswereperformedintheway 2 V similar to 7 for plate-plat(cid:0)e and sph(cid:1)ere-plate geometries. The results for the relativecorrectiontotheforceareshowninFig. 1(a)forminimalseparations 3 in the experiments: a = 63 nm for sphere-plate and a = 260 nm for the 5 effective plate-plate geometries . Let us stress that this correction always make the force for films smaller than that for the bulk material. 3 Scattering on the grain boundaries It is well known that the resistivity of deposited films deviates significantly fromthebulkresistivity. Ifthefilmisnotverythin,saythickerthan10nm,it haspolycrystallinestructure. Thegrainboundariescontributetotheelectron 2 14 14 transport (for the references see ). In a recent paper the optical charac- teristics of the films were treated as the grains with bulk material properties plus electron scattering on the grain boundaries. Thegoldfilmswiththegrainsizefrom15to45nmweredepositedonglass 14 withtwodifferentmethods . Reflectanceofthefilmswasinvestigatedinthe wavelength range 0.3-50 µm. The grain boundaries were modelled with the deltapotentials,scatteringfromphononsandpointdefectswereaccountedby the relaxation time. The grain size distribution had no significant influence, so the films were characterized only by the mean grain size D. The material is described by the two dielectric functions longitudinal ε and transverse ε . l t Only ε changes because the grain boundaries are perpendicular to the film t surface. In the local limit for ε the following expression was found t 3ω2 1 p 2 3 −1 ε (ω)=ε(ω)+ α−α +α ln 1+α , (1) t ω(ω+iω )(cid:20)2 (cid:21) τ (cid:0) (cid:1) −1 v R ω F α ≡ 1−i , (2) Dω 1−R(cid:18) ω (cid:19) τ τ where ε(ω) = ε (ω) is the dielectric function of the crystalline gold, ω is l τ the Drude relaxation frequency, v is the Fermi velocity, R is the reflection F coefficientofelectronsonthegrainboundary. Thelatteristheonlyempirical parameter, which was found in the same experiment to be R ≈ 0.65. The reflectance of the film was expressed via the surface impedance. Comparison with the experimental reflectance showed that the model describes well the effect of the grain size except for the very small grains D ≈15nm when the electron mean free path becomes comparable with D. Weusedtheexpression(1)atimaginaryfrequenciesω =iζ andcalculated the impedances for s and p polarizations following the Kliewer and Fuchs 15 procedure . The impedances are different due to the nonzero wave vector q along the plates in the Lifshitz formula. The details will be reported later. The relative correction to the Casimir force as a function of the grain size is presented in Fig. 1(b). The typical grain size for the films 100−200 nm 16 thick deposited on the substrate at room temperature is less than 50 nm but it can depend on the deposition details and we take as the upper limit D <100nm. 4 Patch potential The importance of the patch potential for the Casimir force measurement 17 was stressed in a recent paper . For a crystal the work function has dif- ferent values for different crystallographic planes. This difference should be compensated by the potential distribution aroundthe crystal. The deposited filmsarepolycrystallineandforthisreasontherewillbelocalvariationofthe 3 5 2 (a) (b) 1 a=63 nm 4 % 2 2 a=260 nm a), 1.5 3 ∆on ( 1 a=63 nm 2 1 correcti 1 2 a=260 nm e v 1 2 Relati0.5 1 0 0 2 4 6 8 10 20 40 60 80 100 120 140 Voids fraction f, % Grain size D, nm V Figure 1. The relative corrections to the Casimir force ∆(a) in percents for the minimal separationsexploredintheexperimentsa=63nm3anda=260nm5: (a)correctiondue tovoidsinthefilm;(b)correctionduetoscatteringonthegrainboundariesasafunction ofthemeangrainsizeD potentialnearbythe surface. Itwillresultinanadditionalforce,electrostatic in nature, which will be measured together with the Casimir force. A simple 17 model was proposed to estimate the effect. In this model the dipoles were distributed on the planes. Their interaction gives the force which is defined bythespectraldensityofthesurfacepotentialcorrelationfunctionC(k). The model is in agreement with the independent ab initio calculation of the po- 18 tential distribution near Al crystallite . For the sphere and plate the force was written in the form ∞ C(k)e−ka 2 Fpatch(a)=−ε0R dkk , (3) Z sinhka 0 C(k)= d2re−ikrc(r), c(r)=hv(r)v(0)i, (4) Z where ε0 is the permittivity of vacuum, R is the sphere radius, v(r) is the local potential on one of the surfaces and the potential distribution on differ- ent surfaces was assumed to be uncorrelated. The spectral density C(k) is 17 crucial for the force estimate. To our opinion, in the original paper it was overestimated. There was no clear idea around which value of k the spectral density should be centered and what is the width of this function, so these values were chosen quite arbitrary. Looking at the films surface images one can easy guess that the spectrum should be centered around the mean grain sizeDwiththewavelengthspresentedroughlyfromD/2to2D. Ifweconsider the spectrum in this range as flat, the force will be the following 4 F (a)≈−4πε0σv2Rexp −2πa . (5) patch 15a (cid:18) D (cid:19) Here σ2 is the variance of the potential distribution that was estimated17 as v 2 (90mV) . The relative contribution of the patch potential to the measured Casimirforceisestimatedtobesmallerthan0.4%fortheminimalseparation 3 a = 63nm in the AFM experiment and the largest grain size D =100nm. It decreases fast for smaller grain size or for larger separations. However, it should be stressed that the patch force mimics the Yukawa interaction and can be easily confused with a new force. 5 Discussion Aboveitwasdemonstratedthatthe opticalpropertiesofdepositedgoldfilms differfromthoseofthebulkmaterial. Themainreasonsforthedeviationsare the voids in the films and electron scattering on the grain boundaries. Both effects diminish the absolute value of the predicted Casimir force on the one percent level. We define the relative correction as F (a)−F (a) f b ∆(a)≡ , (6) (cid:12) F (a) (cid:12) (cid:12) b (cid:12) (cid:12) (cid:12) where the indexes b and f refer(cid:12) to the bulk a(cid:12)nd film materials, respec- 3 tively. For the AFM experiment in the sphere-plate geometry the ex- pected correction was found for the most probable values f = 4% and V D = 50 nm: ∆(63nm) = (1.9+0.5) % = 2.4%. The same correc- 5 tion for the MEMS experiment with the effective plate-plate geometry is ∆(260nm) = (1.0+0.9) % = 1.9%. One can see that these corrections cannot be ignored since in both experiments the precision was better than 1%. There is an additional effect which also reduces the absolute value of the predicted force. At frequencies larger than ω the charge density fluctuation p (plasmons) can propagate in the materialdecreasing the reflection coefficient for p-polarization. Importance of this nonlocal effect for the Casimir force at separationsoftheorderorsmallerthanplasmawavelengthλ wasstressedfor p 19 the first time in the paper where the correction due to plasmon excitation 3 was found. For the AFM experiment it is estimated as 3 % at a = 63 nm. 5 DuetolargerseparationthiscorrectionissmallerfortheMEMSexperiment , where it is 1%at a=260nm. The plasmoncorrectionwasdismissedin Ref. 5 onthebasisthattheseparationwasmuchlargerthanthepenetrationdepth δ =λ /2π. In this connectionwe shouldnote that the separationa has to be p comparedwithλ butnotδ. Otherwiseonthesamebasisonecouldconclude p 5 that the finite conductivity correction is negligible at a ∼ λ while in reality p 7 it is of about of 50% (see Fig. 1 in the paper where the transition point at a∼λ not at λ /2π is clearly seen). p p In conclusion,wedemonstratedthatitisimportanttotakeintoconsider- ation the optical characteristics of the metallic films used in the experiments andshowedthe wayhow the deviationfromthe bulk metalproperties canbe estimated. Voids in the films, scattering on the grain boundaries so as non- local effects all of them tend to reduce the force in comparison with the bulk metal prediction. Even without nonlocal effects the reduction is expected on the level of 2%. Acknowledgments This work was supported by the Dutch Technology Foundation References 1. H. B. G. Casimir, Proc. K. Ned. Akad. Wet. 51, 793 (1948). 2. S. K. Lamoreaux, Phys. Rev. Lett. 78, 5 (1997); 81, 5475 (1998). 3. B. W. Harris, F. Chen, and U. Mohideen, Phys. Rev. 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