Superfluidity in solid helium and solid hydrogen E. Kim*, A. Clark, X. Lin, J. West, M. H. W. Chan Penn State University * KAIST, Korea Outline Introduction Theoretical background for supersolid Experimental setup - Torsional oscillator technique Supersolid in porous media Supersolid in bulk 4He Heat Capacity of solid helium. Results in para-hydrogen Summary Phase diagram of 4He Solid Normal Liquid, (He I) Superfluid (He II) Fritz London is the first person to recognize that superfluidity in liquid 4He is a BEC phenomenon. Condensation fraction was predicted and measured to be 10% near T=0. Superfluid fraction at T=0, however is 100%. Can a solid be ‘superfluid’?* - In a perfect solid when each atom is localized at a specific lattice site and symmetry is ignored, then there is no BEC at T=0. Penrose and Onsager, Phys. Rev. 104, 576 (1956) - Off Diagonal Long Range Order, or superfluidity, which is directly related to Bose-Einstein Condensation, may occur in a solid phase if particles are not localized. C. N. Yang, Rev. Mod. Phys. 34, 694 (1962) *A.J.Leggett ,PRL 25, 1543 (1970) Lindemann Parameter the ratio of the root mean square of the displacement of atoms to the interatomic distance (da) total energy zero-point energy u2 L 0.26 da Zero-point Energy Inter-atomic potential A classical solid will melt if the Lindemann’s parameter exceeds the critical value of ~0.1 . X-ray measurement of the Debye-Waller factor of solid helium at ~0.7K and near melting curve shows this ratio to be 0.262. (Burns and Issacs, Phys. Rev. B 55, 5767(1997)) Superfluidity in solid: not impossible! - If solid 4He can be described by a Jastraw-type wavefunction that is commonly used to describe liquid helium then crystalline order (with finite fraction of vacancies) and BEC can coexist. G.V. Chester, Lectures in Theoretical Physics Vol XI-B(1969); Phys. Rev. A 2, 256 (1970) J. Sarfatt, Phys. Lett. 30A, 300 (1969) L. Reatto, Phys. Rev. 183, 334 (1969) - Andreev and Liftshitz assume the specific scenario of zero-point vacancies and other defects ( e.g. interstitial atoms) undergoing BEC and exhibit superfluidity. Andreev & Liftshitz, Zh.Eksp.Teor.Fiz. 56, 205 (1969). The ideal method to detect superflow would be to subject solid helium to undergo dc or ac rotation to look for evidence of ‘Non-Classical Rotational Inertia’. Leggett, Phys. Rev. Lett. 25, 1543 (1970) Quantum exchange of particles arranged in an annulus under rotation leads to a measured moment of inertia that is smaller than the classical value R I(T)=Iclassical[1-fs(T)] fs(T) is the supersolid fraction Its upper limit is estimated by different theorists to range from 10-6 to 0.4; Leggett: 10-4 Solid Helium No experimental evidence of superfluidity in solid helium prior to 2004 • Plastic flow measurement Andreev et al. Sov. Phys. JETP Lett 9,306(1969) Suzuki J. Phys. Soc. Jpn. 35, 1472(1973) Tsymbalenko Sov. Phys. JETP Lett. 23, 653(1976) Dyumin et al.Sov. J. Low Temp. Phys. 15,295(1989); • Torsional oscillator Bishop et al. Phys. Rev. B 24, 2844(1981) • Mass flow Greywall Phys. Rev. B 16, 1291(1977) Bonfait, Godfrin and Castaing, J. de Physique 50, 1997(1989) Day, Herman and Beamish, Phys. Rev. Lett. 95, 035301 (2005) • PV(T) measurement Adams et al. Bull. Am. Phys. Soc. 35,1080(1990) Haar et al. J. low Temp. Phys. 86,349(1992) •However, interesting results are found in Ultrasound Measurements at UCSD. Goodkind Phys. Rev. Lett. 89,095301(2002) and references therein Ultrasound velocity and dissipation measurements in solid 4He with 27.5ppm of 3He The results are interpreted by the authors as showing BEC of thermally activated vacancies above 200mK. 9.3 MHz x 28MHz 46MHz P.C. Ho, I.P. Bindloss and J. M. Goodkind, J. Low Temp. Phys. 109, 409 (1997) TEM of Vycor glass Solid helium in a porous medium should have more disorder and defects, which may facilitate the appearance of superflow in solid? Amorphous boundary layer Solidification proceeds in two different directions: 1) In the center of the pore a solid cluster has crystalline order identical to bulk 4He 2) On the wall of a pore amorphous solid layers are found due to the van der Waals force of the substrate Crystalline solid Elbaum et al. Adams et al. Brewer et al. Torsional oscillator is ideal for the detection of superfluidity Be-Cu Torsion Rod Resolution Torsion Bob containing helium Resonant period (o) ~ 1 ms Drive Detection I o 2 K /o = 5×10-7 Amp stability in is 0.1ns f Mass sensitivity ~10-7g Q=f0/f ~ 2×106 f0 Torsional oscillator studies of superfluid films Vycor Δ Above Tc the adsorbed normal liquid film behaves as solid and oscillates with the cell, since the viscous penetration depth at 1kHz is about 3 m. Berthold,Bishop, Reppy, PRL 39,348(1977) Solid helium in Vycor glass f0 = 1024Hz Q ~ 1*106 0.38mm Torsion Rod 2.2mm Torsion Bob (vycor glass) 5cm Drive Detect A=A0sinωt v=|v|maxcosωt |v|max=rA0ω Solid 4He at 62 bars in Vycor glass Period shifted by 4260ns due to mass loading of solid helium *=966,000ns Supersolid response of helium in Vycor glass • Period drops at 175mK appearance of NCRI • size of period drop - ~17ns *=971,000ns Superfluid response Total mass loading =4260ns Measured decoupling -o=17ns -*[ns] “ Apparent supersolid fraction”= 0.4% (with tortuosity correction s/ =2% Weak pressure dependence *=971,000ns Δ0[ns] Strong velocity dependence • For liquid film adsorbed on Vycor glass vc > 20cm/s Chan et. al. Phys. Rev. Lett. 32, 1347(1974). • For superflow in solid 4He vc < 30 µm/s Control experiment I : Solid 3He? Nature 427,225(2004) 4He solid diluted with low concentration of 3He Effect of the addition of 3He impurities At 0.3ppm, the separation of the 3He atoms is about 450Å Search for the supersolid phase in the bulk solid 4He. Be-Cu Torsion Rod Torsion cell with helium in annulus I D=0.4mm Filling line OD=2.2mm Mg disk Filling line Channel OD=10mm Width=0.63mm Al shell Solid helium in annulus channel Detection Drive Torsional Oscillator (bulk solid helium-4) Torsion rod Torsion cell 3.5 cm Detection Drive Porous media are not essential ! Solid 4He at 51 bars 4µm/s corresponds to amplitude of oscillation of 7Å NCRI appears below 0.25K Strong |v|max dependence (above 14µm/s) Amplitude minimum, Tp 0= 1,096,465ns at 0 bar 1,099,477ns at 51 bars (total mass loading=3012ns due to filling with helium) Science 305, 1941(2004) Non-Classical Rotational Inertia Fraction NCRIF ρS/ρ |v|max NCRIF total mass loading Total mass loading =3012ns at 51 bars Non-Classical Rotational Inertia Fraction ρS/ρ |v|max NCRIF total mass loading Total mass loading =3012ns at 51 bars Control experiment II With a barrier in the annulus, there should be NO simple superflow and the measured superfluid decoupling should be vastly reduced Torsion cell with blocked annulus Mg barrier Filling line Mg barrier Mg disk Mg Disk Al shell Al shell Solid helium Channel OD=15mm Width=1.5mm Solid helium in annulus channel -*[ns] If there is no barrier, then the supersolid fraction appears to be stationary in the laboratory frame; with respect to the torsional oscillator it is executing oscillatory superflow. Superflow viewed in the rotating frame -*[ns] * If no block, the expected Δ=90ns With a block in the annulus, irrotational flow of the supersolid fraction contributes about 1% (Erich Mueller) of the barrier-free decoupling. Δ~1.5ns Irrotational flow pattern in a blocked annular channel (viewed in the rotating frame) A. L. Fetter, JLTP(1974) [ns] Similar reduction in superfluid response is seen in liquid helium at 19 bars in the same blocked cell measured superfluid decoupling in the blocked cell Δ(T=0)≈ 93ns. While the expected decoupling in unblocked cell is 5270ns. Hence the ratio is 1.7% similar to that for solid. Conclusion : superflow in solid as in superfluid is irrotational. Superflow persists up to at least 136 bars ! 136bar 108bar ρs/ρ ρs/ρ Strong and ‘universal’ velocity dependence in all samples ω R vC~ 10µm/s h vs dl m n h vs n 2Rm =3.16µm/s for n=1 Pressure dependence As a function of pressure the supersolid fraction shows a maximum near 55bars. The supersolid fraction extrapolates to zero near 170 bars. Superfluidity in ultra-pure Solid Helium: 1ppb 3He 0 ~ 0.77ms [1300Hz] 4He - 0 = 3920ns NCRIF ~ 1.25/3920 = 0.03% 4724.0 -* [ns] 4723.5 4723.0 Exp. done at at U. of Florida 4722.5 4722.0 0 * = 770,000ns 50 100 150 Temperature [mK] 200 250 Phase Diagram of 4He Heat Capacity signature? No reliable heat capacity measurement of solid 4He below 200mK because of large background contribution due to the sample cell. Experimental cell of Xi Lin and Tony Clark Silicon!! Results: pure 4He (0.3ppm 3He) Results: pure 4He (0.3ppm 3He) Results: pure 4He (0.3ppm 3He) Results: pure 4He (0.3ppm 3He) Results: pure 4He (0.3ppm 3He) Heat capacity peak near the supersolid transition Is the supersolid phase unique with 4He? Apparently not! Preliminary torsional oscillator data of Tony Clark and Xi Lin indicate similar supersolidlike decoupling in solid H2. de Boer parameter 3He 3.09 4He 2.68 H2 1.73 HD 1.41 D2 1.22 More quantum mechanical Hydrogen in a cylindrical cell Inside Mg bob: Oscillation Period vs. Temperature Period Change [ns] 2.0 1.5 Hydrogen space BeCu wall 1.0 0.5 0.0 Empty Cell -0.5 0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 Temperature [K] (PO = 560,400ns) Q = 1.6million P0 = 560,400ns P ~0.05ns Hydrogen in a cylindrical cell Inside Mg bob: Oscillation Period vs. Temperature Period Change [ns] 2.0 1.5 Hydrogen space BeCu wall 1.0 0.5 PHD = 4014ns (93% filling) 0.0 Empty Cell Cell Full of HD HD -0.5 0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 Temperature [K] (PO = 560,400ns) Hydrogen in a cylindrical cell Inside Mg bob: Oscillation Period vs. Temperature Period Change [ns] 2.0 1.5 Hydrogen space BeCu wall 1.0 0.5 0.0 -0.5 0.0 PH2 = 1638ns (64% filling) Empty Cell HDFull of HD Cell Cell H2 Full of H2 0.1 0.2 0.3 0.4 0.5 0.6 0.7 Temperature [K] (PO = 560,400ns) Hydrogen in a cylindrical cell Temperature below 50mK uncertain, thermometer not on the torsional cell Oscillation Period vs. Temperature 0.5 0.4 Period Change [ns] 0.3 0.2 0.1 Ortho concentration is most likely less than 0.5% 0.0 -0.1 -0.2 Empty Cell Cell Full of HD HD Cell Full of H2 H2 -0.3 -0.4 -0.5 0.00 0.05 0.10 0.15 0.20 0.25 0.30 Temperature [K] (PO = 560,400ns) HD concentration uncertain NCRIF ~ 0.015% Hydrogen in an annular cell Samples contain < 50ppm HD 83% filling, x1~2.0% 0.05 68% filling, x1<0.5% NCRIF [%] 0.04 Mg 88% filling, x1<0.5% Hydrogen space BeCu (h=3.5mm wall w=2.3mm) 0.03 X is the ortho conc, 0.02 0.01 0.00 0.0 Inside Mg bob: 0.1 0.2 0.3 Temperature [K] 0.4 0.5 Q = 350,000 P0 = 709,700ns P <0.1ns Hydrogen in an annular cell Comparison of 50 and 200ppm HD 0.05 88% filling, x1<0.5% 68% filling, x1<0.5% NCRIF [%] 0.04 Mg 94% filling, x1<1.0%** 83% filling, x1~2.0% 0.03 0.02 0.01 0.00 0.0 Inside Mg bob: 0.1 0.2 0.3 Temperature [K] 0.4 0.5 **200ppm HD Hydrogen space BeCu wall Summary Superflow is seen in solid helium confined in Vycor glass with pores diameter of 7nm and also in bulk. Results in bulk have been replicated in three other labs. Supersolid fraction is on the order of 1% for He-4 sample with 0.3ppm of He-3 impurities. For ultra-high purity sample (1ppb He-3) the supersolid fraction is on the order of 0.03% and the transition temp. is depressed. There is preliminary evidence of a heat capacity peak at the transition. Superflow is also seen in para-hydrogen. The supersolid fraction is on the order of 0.05% We are grateful for many informative discussions with many colleagues, too numerous to acknowledge all of them. P.W. Anderson J. R. Beamish, D. J. Bishop, D. M. Ceperley, J. M. Goodkind, T. L. Ho, J. K. Jain, A. J. Leggett, E. Mueller, M. A. Paalanen, J. D. Reppy, W. M. Saslow, D.S. Weiss Xi, Tony, Eunseong, Josh