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# References

BARYON NUMBER TRANSFER

IN HADRONIC INTERACTIONS

G. H. Arakelyan1, A. Capella, A. Kaidalov2 and Yu. M. Shabelski3
Laboratoire de Physique Théorique***Unité Mixte de Recherche - CNRS - UMR n 8627,

Université de Paris Sud, Bâtiment 210, 91405 Orsay Cedex, France

E-mail: Alphonse.Capella@th.u-psud.fr

ABSTRACT

The process of baryon number transfer due to string junction propagation in rapidity is considered. It has a significant effect in the net baryon production in $`pp`$ collisions at mid-rapidities and an even larger effect in the forward hemisphere in the cases of $`\pi p`$ and $`\gamma p`$ interactions. The results of numerical calculations in the framework of the Quark-Gluon String model are in reasonable agreement with the data.

1Permanent address: Yerewan Physics Institute, Armenia and JINR, Dubna, Russia E-mail: argev@jerewan1.yerphi.am 2Permanent address: Institute of Theoretical and Experimental Physics, Moscow, Russia
E-mail: kaidalov@vitep5.itep.ru 3Permanent address: Petersburg Nuclear Physics Institute, Gatchina, St.Petersburg, Russia E-mail: shabelsk@thd.pnpi.spb.ru

LPT-Orsay 01-24

March 2001

1. INTRODUCTION

The Quark–Gluon String Model (QGSM) and the Dual Parton Model (DPM) are based on the Dual Topological Unitarization (DTU) and describe quite reasonably many features of high energy production processes, including the inclusive spectra of different secondary hadrons, their multiplicities, KNO–distributions, etc., both in hadron–nucleon and hadron–nucleus collisions . High energy interactions are considered as proceeding via the exchange of one or several pomerons and all elastic and inelastic processes result from cutting through or between pomerons . The possibility of exchanging a different number of pomerons introduces absorptive corrections to the cross sections which are in agreement with the experimental data on production of hadrons consisting of light quarks. Inclusive spectra of hadrons are related to the corresponding fragmentation functions of quarks and diquarks, which are constructed using the reggeon counting rules .

In the present paper we discuss the processes connected with the transfer of baryon charge over long rapidity distances. In the string models baryons are considered as configurations consisting of three strings attached to three valence quarks and connected in a point called “string junction” . Such a configuration corresponds in QCD to the following gauge-invariant operator

$$\psi _i(x_1)\psi _j(x_2)\psi _k(x_3)G[P(x_1,x)]_i^{}^iG[P(x_2,x)]_j^{}^jG[P(x_3,x)]_k^{}^k\epsilon ^{i^{}j^{}k^{}},$$
(1)
where

$$G[P(x_1,x)]_j^i=\left[T\mathrm{exp}(g_{P(x_1,x)}A_\mu (x)𝑑x^\mu )\right]_j^i.$$
(2)
It is very important to understand the role of the string-junction in the dynamics of high-energy hadronic interactions. Now we have several different experimental results concerning such processes. First of all the data  clearly show that in the forward hemisphere the number of secondary protons produced in $`\pi ^+p`$ interactions is significantly larger than the number of $`\overline{p}`$ produced in $`\pi ^{}p`$ collisions. This difference can not be described  without the assumption that the baryon charge is transferred from the target proton to the pion hemisphere.

Similar data on the differences of $`p\overline{p}`$ yields in $`\frac{1}{2}(\pi ^+p+\pi ^{}p)`$ collisions at 158 GeV/c were presented by the NA49 Coll. .

A second group of data concerns the energy dependence of the differences in yields of the protons and antiprotons at 90o (i.e. at $`x_F`$ = 0) at ISR energies .

Another sample of data includes the measurements of hyperon production asymmetries in 500 GeV/c $`\pi ^{}`$-nucleus interactions .

Finally, the proton-antiproton asymmetry in photoproduction was recently measured at HERA .

In this paper we present a simultaneous description of all these data and extract information on the properties of the string junction dynamics.

2. INCLUSIVE SPECTRA OF SECONDARY HADRONS IN QGSM

As mentioned above high energy hadron–nucleon and hadron–nucleus interactions are considered in the QGSM and in DPM as proceeding via the exchange of one or several pomerons. Each pomeron corresponds to a cylindrical diagram (see Fig. 1a), and thus, when cutting a pomeron two showers of secondaries are produced (Fig. 1b). The inclusive spectrum of secondaries is determined by the convolution of diquark, valence and sea quark distributions $`u(x,n)`$ in the incident particles and the fragmentation functions $`G(z)`$ of quarks and diquarks into secondary hadrons. The diquark and quark distribution functions depend on the number $`n`$ of cut pomerons in the considered diagram. In the following we use the formalism of QGSM. In the case of a nucleon target the inclusive spectrum of a secondary hadron $`h`$ has the form :

$$\frac{x}{\sigma _{inel}}\frac{d\sigma }{dx}=\underset{n=1}{\overset{\mathrm{}}{}}w_n\varphi _n^h(x),$$
(3)
where the functions $`\varphi _n^h(x)`$ determine the contribution of diagrams with $`n`$ cut pomerons and $`w_n`$ is the probability of this process. Here we neglect the contributions of diffraction dissociation processes which are comparatively small in most of the processes considered below. It can be accounted for separately .

For $`pp`$ collisions

$$\varphi _{pp}^h(x)=f_{qq}^h(x_+,n)f_q^h(x_{},n)+f_q^h(x_+,n)f_{qq}^h(x_{},n)+2(n1)f_s^h(x_+,n)f_s^h(x_{},n),$$
(4)
$$x_\pm =\frac{1}{2}[\sqrt{4m_T^2/s+x^2}\pm x],$$
(5)
where $`f_{qq}`$, $`f_q`$ and $`f_s`$ correspond to the contributions of diquarks, valence and sea quarks respectively. They are determined by the convolution of the diquark and quark distributions with the fragmentation functions, e.g.,

$$f_q^h(x_+,n)=_{x_+}^1u_q(x_1,n)G_q^h(x_+/x_1)𝑑x_1.$$
(6)
In the case of a meson beam the diquark contributions in Eq. (4) should be changed by the contribution of valence antiquarks:

$$\varphi _{\pi p}^h(x)=f_{\overline{q}}^h(x_+,n)f_q^h(x_{},n)+f_q^h(x_+,n)f_{qq}^h(x_{},n)+2(n1)f_s^h(x_+,n)f_s^h(x_{},n).$$
(7)
The diquark and quark distributions as well as the fragmentation functions are determined from Regge intercepts. Their expressions are given in Appendix 1.

The net baryon charge can be obtained from the fragmentation of the diquark giving rise to a leading baryon (Fig. 2a). A second possibility is to produce a (leading) meson in the first break-up of the string and the baryon in a subsequent break-up (Fig. 2b).

As discussed above, in the approach  the baryon consists of three valence quarks together with string junction (SJ), which is conserved during the interactionAt very high energies one or even several SJ pairs can be produced..

This gives a third possibility for secondary net baryon production in non-diffractive hadron-nucleon interactions (Fig. 2c).

The secondary baryon consists of the SJ together with two valence and one sea quarks (Fig. 2a), one valence and two sea quarks (Fig. 2b) or three sea quarks (Fig. 2c). The fraction of the incident baryon energy carried by the secondary baryon decreases from a) to c), whereas the mean rapidity gap between the incident and secondary baryon increases.

The probability to find a comparatively slow SJ in the case of Fig. 2c can be estimated from the data on $`\overline{p}p`$ annihilation into mesons (see Figs. 1c, d). This probability is known experimentally only at comparatively small energies where it is proportional to $`s^{\alpha _{SJ}1}`$ with $`\alpha _{SJ}0.5`$.

However, it has been argued  that the annihilation cross section contains a small piece which is independent of $`s`$ and thus $`\alpha _{SJ}1`$. Irrespectively of the value of $`\alpha _{SJ}`$, the contribution of the graph in Fig. 2c corresponds to annihilation and, thus, has a small coefficient which will be denoted by $`\epsilon `$. In our calculation we shall use

$$\alpha _{SJ}=0.5$$
(8)
and will treat $`\epsilon `$ as a free parameter. A contribution with $`\alpha _{SJ}1`$, if present at all, is expected to be important only at very high energies (see a discussion of this point in section 5). The values of $`\alpha _{SJ}`$ and $`\epsilon `$ can only be determined with the help of accurate data.

3. COMPARISON WITH THE DATA

The mechanism of the baryon charge transfer via SJ without valence quarks (Fig. 2c) was not accounted for in previous papers .

The data at comparatively low energies ($`\sqrt{s}15÷40`$ GeV) can be described with $`\alpha _{SJ}=0.5`$. Unfortunately, the value of $`\epsilon `$ cannot be determined in a unique way. Many sets of data can be described with $`\epsilon =0.05`$. However, other data sets favor a value four times larger, $`\epsilon =0.2`$. Because of that, we will present our results for these two values of $`\epsilon `$, leaving all other parameters in the model unchanged. Thus, the results for meson and antibaryon production are the same in the two cases.

The inclusive spectra of secondary protons and antiprotons produced in $`pp`$ collisions at lab. energies 100 and 175 GeV  are shown in Figs. 3a and 3b together with the curves calculated in the QGSM. The agreement of our results with $`\epsilon =0.05`$ with the data is quite reasonable, on the same level (or even better) as in the previous papers which did not incorporate the SJ mechanism of Fig. 2c. The variant with $`\epsilon =0.2`$ gives too large multiplicity of secondary protons at small $`x_F`$. The description of the antiproton yields is reasonable.

The data of Ref.  are in some regions of $`x_F`$ in disagreement with the data of Ref.  as well as with our calculations. However, one can see from Figs. 3c and 3d that the experimental points can not be described by any smooth curve. Probably this is connected with the use of different detectors for different $`x_F`$ regions and to the influence of the trigger in . Again, the value $`\epsilon =0.05`$ is preferable.

The data on secondary proton and antiproton production in $`pp`$ collisions at ISR energies  at $`90^o`$ in c.m.s. are presented in Figs. 3e and 3f. Their differences, which are more sensitive to the baryon charge transfer, are presented in Fig. 3g. One can see that the last data, as well as the yields of protons and antiprotons separately, are described quite reasonably by QGSM with $`\epsilon =0.2`$. However, it is necessary to note, that the systematic errors in  are of the order of 30 %, so the value $`\epsilon =0.05`$ can not be excluded. Thus the disagreement between ISR data  and more recent data  on spectra of protons in $`pp`$-collisions does not allow to determine uniquely the value of $`\epsilon `$.

The data on baryon production in the pion fragmentation region  are presented in Fig. 4. The spectra of antiprotons produced in $`\pi ^{}p`$ collisions, shown in Fig. 4a, allows one to fix the fragmentation function of a quark into baryon/antibaryon. If the contribution of the baryon charge transfer were negligibly small, the inclusive spectra of reactions $`\pi ^{}p\overline{p}X`$ and $`\pi ^+ppX`$ in the pion fragmentation region would be practically the same . Actually, the data for the second reaction are significantly higher than for the first one providing evidence for the baryon charge transfer due to the SJ propagation. The difference of the inclusive spectra in the two considered processes allows one to estimate quantitatively the contribution of the baryon charge transfer, and the parametrization of these processes given in Appendix leads to a reasonable description of proton yields in $`\pi ^+p`$ collisions with $`\epsilon =0.2`$. The value $`\epsilon =0.05`$ seems to be too small here. Note, however, that our factorized formulae, Eqs. 4 and 7, imply that the slowed down proton is made out of SJ and three sea quarks (see Fig. 2c). Thus, they should be modified for the reaction $`\pi ^+ppX`$ in the pion fragmentation region due to the possibility of SJ recombination with a pion valence quark – which would change the ratio of protons and neutrons. A simple estimate based on the quark combinatorics given in Appendix 1 leads to an increase of the proton yield in the reaction $`\pi ^+ppX`$ by about 50 %. In this case the value of $`\epsilon =0.05`$ can be consistent with the data. This problem disappears if we consider the sum of $`\pi ^+p`$ and $`\pi ^{}p`$. Preliminary data on $`\frac{1}{2}(\pi ^+p+\pi ^{}p)(p\overline{p})X`$ were obtained by the NA49 Coll. . One can see from Fig.4c, that they are in good agreement with our calculations with $`\epsilon =0.05`$ and in total disagreement with $`\epsilon =0.2`$.

The data on $`\mathrm{\Lambda }`$ and $`\overline{\mathrm{\Lambda }}`$ production in $`pp`$ collisions , presented in Fig. 5, are also in agreement with QGSM and the value $`\epsilon =0.05`$ is again favored.

In Fig. 6 we show the data  on the asymmetry of strange baryons produced in $`\pi ^{}`$ interactionsThese data were obtained from pion interactions on a nuclear target where different materials were used in a very complicated geometry. We assume that the nuclear effects are small in the asymmetry ratio (9), and compare the pion-nucleus data with calculations for $`\pi ^{}p`$ collisions. at 500 GeV/c. The asymmetry is determined as

$$A(B/\overline{B})=\frac{N_BN_{\overline{B}}}{N_B+N_{\overline{B}}}$$
(9)
for each $`x_F`$ bin.

The theoretical curves for the data on all asymmetries calculated with $`\epsilon =0.05`$ are in reasonable agreement with the data with the exception of $`\mathrm{\Xi }^{}/\mathrm{\Xi }^+`$ at positive $`x_F`$. However in this region the effect of recombination of SJ with valence (d) quark of $`\pi ^{}`$ can be important and can lead to an increase of cross section analogous to the one in $`\pi ^+ppX`$ discussed above. In the case of $`\mathrm{\Omega }/\overline{\mathrm{\Omega }}`$ production we predict a non-zero asymmetry in agreement with experimental data. Let us note that the last asymmetry is absent, say, in the naive quark model because $`\mathrm{\Omega }`$ and $`\overline{\mathrm{\Omega }}`$ have no common valence quarks with the incident particles. The value $`\epsilon =0.2`$ seems to be excluded.

Preliminary data on $`p/\overline{p}`$ asymmetry in $`ep`$ collisions at HERA were presented by the H1 Collaboration . Here the asymmetry is defined as

$$A_B=2\frac{N_pN_{\overline{p}}}{N_p+N_{\overline{p}}},$$
(10)
i.e. with an additional factor 2 in comparison with Eq. (9). The experimental value of $`A_B`$ is equal to $`8.0\pm 1.0\pm 2.5`$ %  for secondary baryons produced at $`x_F0.04`$ in the $`\gamma p`$ c.m. frame. QGSM with $`\epsilon =0.05`$ predicts here 2.9 %, i.e. a smaller value, whereas the calculation with $`\epsilon =0.2`$ gives the value 7.7 %, in agreement with the data.

5. CONCLUSIONS

We have demonstrated that experimental data on high-energy hadronic interactions support the possibility of baryon charge transfer over large rapidity distances. Probably, the most important are the baryon-antibaryon asymmetry in $`\mathrm{\Omega }`$ and $`\overline{\mathrm{\Omega }}`$  in $`\pi ^{}p`$ collisions, where both secondary particles have no common valence quarks with the incident particles. This asymmetry is provided by baryon charge transfer due to string junction diffusion.

Also the production of net baryons in $`\pi p`$ and $`\gamma p`$ interactions in the projectile hemisphere provides good evidence for such a mechanism.

As for the values of the parameters $`\alpha _{SJ}`$ and $`\epsilon `$ which govern the baryon charge transfer we have seen that the data, at comparative low energies ($`\sqrt{s}15÷40`$ GeV), without providing a clear cut answer, strongly favor the values $`\alpha _{SJ}=0.5`$ and $`\epsilon =0.05`$. Indeed, as discussed above, the data which favor $`\epsilon =0.2`$ have either a large systematic error  or correspond to situations where effects, not incorporated in the present version of the model, are expected to be important (as in $`\pi ^+ppX`$ ; see the discussion in Section 3).

At HERA energies the situation is different. Here the observed asymmetry is better described with $`\epsilon =0.2`$. Note, however, that HERA data are preliminary and have rather large errors (the prediction for asymmetry with $`\epsilon =0.05`$ deviates from the data by about two standard deviations). If this discrepancy is real can it be solved ? The data at $`\sqrt{s}<`$ 40 GeV that we have examined provide information for the transfer of baryon charge over about five rapidity units. In contrast, the HERA data provide information for the corresponding transfer over more than seven units. In ref.  HERA data were described under the assumption that there is a component with $`\alpha _{SJ}1`$ and a very small strength. Another possibility would be to use $`\alpha _{SJ}0.5`$ and to assume, following Ref. - that the strength of the $`SJ`$ transfer contribution increases with the number of inelastic collisions. In this way the asymmetry would increase with energy since the average number of inelastic collisions, determined from Eqs. (42) and (43), increases with $`s`$. (This mechanism also allows to explain the increase of stopping in heavy ion collisions with increasing centrality) -.

In conclusion, the study of the transfer of baryon charge over large rapidity distances is very important. Good experimental data in $`pp`$, $`pA`$ and $`AB`$ collisions for different centralities are needed in order to understand the dynamics of this mechanism.

Acknowledgments: We thank H.G.Fisher from NA49 Collaboratiomn for providing the preliminary data in Fig. 4c prior to publication.

This paper was supported by grant NATO OUTR. LG 971390 and NATO PSTCLG 977275.

APPENDIX. QUARK AND DIQUARK DISTRIBUTIONS AND THEIR FRAGMENTATION FUNCTIONS

In the present calculations we use quark and diquark distributions in the proton for one-pomeron exchange given by the correspondent Regge behaviour

$`u_{uu}(x,n)`$ $`=`$ $`C_{uu}x^{\alpha _R2\alpha _B+1}(1x)^{\alpha _R},`$ (11)
$`u_{ud}(x,n)`$ $`=`$ $`C_{ud}x^{\alpha _R2\alpha _B}(1x)^{\alpha _R},`$ (12)
$`u_u(x,n)`$ $`=`$ $`C_ux^{\alpha _R}(1x)^{\alpha _R2\alpha _B+1},`$ (13)
$`u_d(x,n)`$ $`=`$ $`C_dx^{\alpha _R}(1x)^{n+\alpha _R2\alpha _B},`$ (14)
In the case of multipomeron exchange the distributions of valence quarks and diquarks are softened due to the appearance of sea quark contribution. Aslo it is necessary to account that $`d`$-quark distribution is more soft in comparison with $`u`$-quark one. There is some freedom  how to account for these effects. We use the simplest way and write diquark and quark distributions (for $`\alpha _R=0.5`$ and $`\alpha _B=0.5`$) as

$`u_{uu}(x,n)`$ $`=`$ $`C_{uu}x^{\alpha _R2\alpha _B+1}(1x)^{frac43(n1)\alpha _R},`$ (16)
$`u_{ud}(x,n)`$ $`=`$ $`C_{ud}x^{\alpha _R2\alpha _B}(1x)^{n1\alpha _R},`$ (17)
$`u_u(x,n)`$ $`=`$ $`C_ux^{\alpha _R}(1x)^{n+\alpha _R2\alpha _B+1},`$ (19)
$`u_d(x,n)`$ $`=`$ $`C_dx^{\alpha _R}(1x)^{\frac{4}{3}(n1)+\alpha _R2\alpha _B+1},`$ (21)
$`u_{\overline{u}}(x,n)`$ $`=`$ $`u_{\overline{d}}(x,n)=C_{\overline{u}}x^{\alpha _R}`$ (23)
$`\times `$ $`[(1x)^{n+\alpha _R2\alpha _B1}\delta /2(1x)^{n+2\alpha _R2\alpha _B1}],n>1,`$
$`u_s(x,n)`$ $`=`$ $`C_sx^{\alpha _R}(1x)^{n+2\alpha _R2\alpha _B1},n>1.`$ (24)
In the case of a pion beam we use

$$u_q(x,n)=C_qx^{\alpha _R}(1x)^{n\alpha _R1},u_{\overline{q}}(x,n)=C_{\overline{q}}x^{\alpha _R}(1x)^{n\alpha _R1},$$
(25)
for valence quarks, and

$$u(x,n)=Cx^{\alpha _R}(1x)^{n\alpha _R1}[1\delta \sqrt{1x}],n>1,$$

$$u_s(x,n)=C_sx^{\alpha _R}(1x)^{n1},n>1,$$
(26)
for sea quarks, where $`\delta =0.2`$ is the relative probability to find a strange quark in the sea. The values of $`\alpha _R`$ and $`\alpha _B`$ are given in Table 1. The factors $`C_i`$ are determined from the normalization condition

$$_0^1u_i(x,n)𝑑x=1.$$
(27)
and sum rule

$$_0^1\underset{i}{}u_i(x,n)xdx=1.$$
(28)
is fulfilled.

The fragmentation functions of quarks and diquarks were changed a little in comparison with Refs.  to obtain a better agreement with the existing experimental data, because the old functions  correspond to $`\epsilon `$ = 0. We use the quark fragmentation functions in the form

$$G_u^p=G_d^p=a_{\overline{N}}(1z)^{\lambda +\alpha _R2\alpha _B}(1+a_1z^2),G_u^{\overline{p}}=G_d^{\overline{p}}=(1z)G_u^p$$
(29)
$$G_u^\mathrm{\Lambda }=G_d^\mathrm{\Lambda }=\frac{a_{\overline{\mathrm{\Lambda }}}}{a_{\overline{N}}}(1z)^{\mathrm{\Delta }\alpha }G_u^p,G_u^{\overline{\mathrm{\Lambda }}}=(1z)G_d^\mathrm{\Lambda }$$
(30)
$$G_d^\mathrm{\Xi }^{}=\frac{a_{\overline{\mathrm{\Xi }}}}{a_{\overline{\mathrm{\Lambda }}}}(1z)^{\mathrm{\Delta }\alpha }G_u^p,G_u^\mathrm{\Xi }^{}=G_u^{\overline{\mathrm{\Xi }}}=(1z)G_d^\mathrm{\Xi }^{}$$
(31)
$$G_u^\mathrm{\Omega }=G_d^\mathrm{\Omega }=G_u^{\overline{\mathrm{\Omega }}}=G_d^{\overline{\mathrm{\Omega }}}=\frac{a_{\overline{\mathrm{\Omega }}}}{a_{\overline{\mathrm{\Xi }}}}(1z)^{\mathrm{\Delta }\alpha }G_u^\mathrm{\Xi },$$
(32)
with

$$\mathrm{\Delta }\alpha =\alpha _\rho \alpha _\varphi =1/2,\lambda =2\alpha ^{}<p_t^2>=0.5.$$
(33)
Diquark fragmentation functions have more complicate forms. They contain two contributions. The first one corresponds to the central production of a $`B\overline{B}`$ pair and can be described by the previous formulas. They have the form:

$$G_{uu}^p=G_{ud}^p=G_{uu}^{\overline{p}}=G_{ud}^{\overline{p}}=a_{\overline{N}}(1z)^{\lambda \alpha _R+4(1\alpha _B)},$$
(34)
$$G_{uu}^\mathrm{\Lambda }=G_{ud}^\mathrm{\Lambda }=G_{uu}^{\overline{\mathrm{\Lambda }}}=G_{ud}^{\overline{\mathrm{\Lambda }}}=\frac{a_{\overline{\mathrm{\Lambda }}}}{a_{\overline{N}}}(1z)^{\mathrm{\Delta }\alpha }G_{uu}^p,$$
(35)
$$G_{uu}^\mathrm{\Xi }^{}=G_{ud}^\mathrm{\Xi }^{}=G_{uu}^{\overline{\mathrm{\Xi }}}=G_{ud}^{\overline{\mathrm{\Xi }}}=\frac{a_{\overline{\mathrm{\Xi }}}}{a_{\overline{\mathrm{\Lambda }}}}(1z)^{\mathrm{\Delta }\alpha }G_{uu}^\mathrm{\Lambda },$$
(36)
$$G_{uu}^\mathrm{\Omega }=G_{ud}^\mathrm{\Omega }=G_{uu}^{\overline{\mathrm{\Omega }}}=G_{ud}^{\overline{\mathrm{\Omega }}}=\frac{a_{\overline{\mathrm{\Omega }}}}{a_{\overline{\mathrm{\Xi }}}}(1z)^{\mathrm{\Delta }\alpha }G_{uu}^\mathrm{\Xi }$$
(37)
with the same $`\mathrm{\Delta }\alpha `$ Eq. (29).

The second contribution is connected with the direct fragmentation of the initial baryon into the secondary one with conservation of the string junction. As discussed above, there exists three different types of such contributions (Figs. 2a-2c). Obviously, in the case of $`\mathrm{\Xi }`$ production only two possibilities exist with string junction plus either one valence quark and two sea quarks or three sea quarks. In the case of production of a secondary baryon having no common quarks with the incident nucleons only the bare string junction without valence quarks can contribute (Fig. 2c).

All these contributions are determined by Eqs. similar to Eq. (6) with the corresponding fragmentation functions given by

$$G_{uu}^p=G_{ud}^p=a_N\sqrt{z}[v_0\epsilon (1z)^2+v_qz^{3/2}(1z)+v_{qq}z^2],$$
(38)
$$G_{ud}^\mathrm{\Lambda }=a_N\sqrt{z}[v_0\epsilon (1z)^2+v_qz^{3/2}(1z)+v_{qq}z^2](1z)^{\mathrm{\Delta }\alpha },G_{uu}^\mathrm{\Lambda }=(1z)G_{ud}^\mathrm{\Lambda }$$
(39)
$$G_{d,SJ}^\mathrm{\Xi }^{}=a_N\sqrt{z}[v_0\epsilon (1z)^2+v_qz^{3/2}(1z)](1z)^{2\mathrm{\Delta }\alpha },G_{u,SJ}^\mathrm{\Xi }^{}=(1z)G_{d,SJ}^\mathrm{\Xi }^{},$$
(40)
$$G_{SJ}^\mathrm{\Omega }=a_Nv_0\epsilon \sqrt{z}(1z)^{2+3\mathrm{\Delta }\alpha }.$$
(41)
The factor $`\sqrt{z}`$ is really $`z^{1\alpha _{SJ}}`$ with $`\alpha _{SJ}=1/2`$ (8). As for the factor $`\sqrt{z}z^{3/2}`$ of the second term it is just $`2(\alpha _R\alpha _B)`$ . For the third term we have just added an extra factor $`z^{1/2}`$.

The probabilities of transition into the secondary baryon of SJ without valence quarks, $`I_3`$, SJ plus one valence quark, $`I_2`$, and SJ plus a valence diquark, $`I_1`$, were taken from the simplest quark combinatorics . Assuming that the strange quark suppression is the same in all these cases, we obtain for the relative yields of different baryons from SJ fragmentation without valence quarks :

$$I_3=4L^3:4L^3:12L^2S:3LS^2:3LS^2:S^3$$
(42)
for secondary $`p`$, $`n`$, $`\mathrm{\Lambda }+\mathrm{\Sigma }`$, $`\mathrm{\Xi }^0`$, $`\mathrm{\Xi }^{}`$ and $`\mathrm{\Omega }`$, respectively.

For $`I_2`$ we obtain

$$I_{2u}=3L^2:L^2:4LS:S^2:0$$
(43)
and

$$I_{2d}=L^2:3L^2:4LS:0:S^2$$
(44)
for secondary $`p`$, $`n`$, $`\mathrm{\Lambda }+\mathrm{\Sigma }`$, $`\mathrm{\Xi }^0`$ and $`\mathrm{\Xi }^{}`$.

For $`I_1`$ we have

$$I_{1uu}=2L:0:S$$
(45)
and

$$I_{1ud}=L:L:S$$
(46)
for secondary $`p`$, $`n`$ and $`\mathrm{\Lambda }+\mathrm{\Sigma }`$. The ratio $`S/L`$ determines the strange suppression factor and $`2L+S`$ = 1. In the numerical calculations we used $`S/L=0.2`$.

In agreement with experimental data we assume that $`\mathrm{\Sigma }^++\mathrm{\Sigma }^{}=0.6\mathrm{\Lambda }`$  in Eqs. (38)-(40). This is obtained when, say, an $`uus`$ state can turn into $`\mathrm{\Sigma }^+`$ with probability 3/4 and into $`\mathrm{\Lambda }`$ (via $`\mathrm{\Sigma }^+(1385)\mathrm{\Lambda }\pi ^+`$ decay) with probability 1/4 §§§These probabilities are in disagreement with simplest quark statistic rules .. In the case of Eqs. (41) and (42) $`\mathrm{\Sigma }^{}`$ can not be produced and we assume that $`\mathrm{\Sigma }^+=0.3\mathrm{\Lambda }`$.

The values of $`v_0`$, $`v_q`$ and $`v_{qq}`$ are determined directly by the corresponding coefficients of Eqs. (38)-(42), together with the probabilities to fragment a $`qqs`$ system into $`\mathrm{\Sigma }^++\mathrm{\Sigma }^{}`$ and into $`\mathrm{\Lambda }`$, given above. For example, we have for incident $`uu`$ diquark and secondary proton :

$$v_0=4L^3,v_q=3L^2,v_{qq}=2L;$$
(47)
for incident $`ud`$ diquark and secondary proton :

$$v_0=4L^3,v_q=2L^2,v_{qq}=L;$$
(48)
for incident $`uu`$ diquark and secondary $`\mathrm{\Lambda }`$ :

$$v_0=\frac{12}{1.6}SL^2,v_q=\frac{4}{1.6}SL,v_{qq}=\frac{1}{4}S;$$
(49)
for incident $`ud`$ diquark and secondary $`\mathrm{\Lambda }`$ :

$$v_0=\frac{12}{1.6}SL^2,v_q=\frac{4}{1.6}SL,v_{qq}=S;$$
(50)
for incident $`u`$ quark and secondary $`\mathrm{\Xi }^{}`$ :

$$v_0=3S^2L,v_q=0;$$
(51)
for incident $`d`$ quark and secondary $`\mathrm{\Xi }^{}`$ :

$$v_0=3S^2L,v_q=S^2;$$
(52)
and incident SJ and secondary $`\mathrm{\Omega }^{}`$ :

$$v_0=S^3.$$
(53)
The probability for a process to have $`n`$ cutted pomerons was calculated using the quasi-eikonal approximation :

$$w_n=\sigma _n/\underset{n=1}{\overset{\mathrm{}}{}}\sigma _n,\sigma _n=\frac{\sigma _P}{nz}(1e^z\underset{k=0}{\overset{n1}{}}\frac{z^k}{k!}),$$
(54)
$$z=\frac{2C\gamma }{R^2+\alpha ^{}\xi }e^{\mathrm{\Delta }\xi },\sigma _P=8\pi \gamma e^{\mathrm{\Delta }\xi },\xi =\mathrm{ln}(s/1\mathrm{GeV}^2),$$
(55)
with parameters

$`\mathrm{\Delta }=0.139,\alpha ^{}=0.21\mathrm{GeV}^2,\gamma _{pp}=1.77\mathrm{GeV}^2,\gamma _{\pi p}=1.07\mathrm{GeV}^2,`$
$`R_{pp}^2=3.18\mathrm{GeV}^2,R_{\pi p}^2=2.48\mathrm{GeV}^2,C_{pp}=1.5,C_{\pi p}=1.65.`$

The model parameters for quark and diquark distributions and their fragmentation are presented in Table 1. They were mainly taken from the description of the data in Refs. .

Table 1

The values of the parameters used for the calculations in QGSM.

| Parameter | value |
| --- | --- |
| $`a_N`$ | 1.8 |
| $`a_{\overline{N}}`$ | 0.18 |
| $`a_1`$ | 12 |
| $`\alpha _R`$ | 0.5 |
| $`\alpha _B`$ | -0.5 |

Figure captions

Fig. 1. Cylindrical diagram corresponding to the one–pomeron exchange contribution to elastic $`\overline{p}p`$ scattering (a) and its cut which determines the contribution to inelastic $`\overline{p}p`$ annihilation cross section (b) (string-junction is indicated by a dashed line). c) the diagram for elastic $`\overline{p}p`$-scattering with an exchange by SJ in the $`t`$-channel and its $`s`$-channel discontinuity d).

Fig. 2. Three different possibilities of secondary baryon production in $`pp`$ interactions: string junction together with two valence and one sea quark (a), together with one valence and two sea quarks (b), together with three sea quarks (c).

Fig. 3. The spectra of secondary protons (a), and antiprotons (b) in $`pp`$ collisions at 100 and 175 GeV/c  and at 400 GeV/c  (c) and (d) and their description by QGSM. Secondary proton (e) and antiproton (f) yields at ISR energies  at $`90^o`$ in c.m.s. and their difference (g) together with QGSM model predictions. In all cases the calculations with $`ϵ`$ = 0.05 are shown by solid curves and the variants with $`ϵ`$ = 0.2 are shown by dashed curves.

Fig. 4. The spectra of secondary antiprotons in $`\pi ^{}p`$ collisions (a) and of protons in $`\pi ^+p`$ collisions (b) at lab. energies 100 and 175 GeV  and its description by QGSM. The differences $`dN/dx`$ of $`p\overline{p}`$ yields in $`\frac{1}{2}(\pi ^+p+\pi ^{}p)`$ collisions at 158 GeV/c compared to preliminary data from NA49  (c). In all cases the calculations with $`ϵ`$ = 0.05 are shown by solid curves and the variants with $`ϵ`$ = 0.2 are shown by dashed curves.

Fig. 5. The spectra of secondary $`\mathrm{\Lambda }`$ (a) and $`\overline{\mathrm{\Lambda }}`$ (b) in $`pp`$ collisions (data are taken from ) and its description by QGSM model. The calculations with $`ϵ`$ = 0.05 are shown by solid curves and a variant with $`ϵ`$ = 0.2 are shown by dashed curves.

Fig. 6. The asymmetries of secondary $`\mathrm{\Lambda }/\overline{\mathrm{\Lambda }}`$ (a), $`\mathrm{\Xi }^{}/\mathrm{\Xi }^+`$ (b), and $`\mathrm{\Omega }/\overline{\mathrm{\Omega }}`$ (c), in $`\pi ^{}p`$ collisions at 500 GeV/c  and its description by QGSM model. In all cases the calculations with $`ϵ`$ = 0.05 are shown by solid curves and the variants with $`ϵ`$ = 0.2 are shown by dashed curves.


format: text

text:
# Experimental evidence for Fröhlich superconductivity in high magnetic fields

## Abstract

Resistivity and irreversible magnetisation data taken within the high magnetic field CDWx phase of the quasi-two-dimensional organic metal $`\alpha `$-(BEDT-TTF)2KHg(SCN)4 are shown to be consistent with a field-induced inhomogeneous superconducting phase. In-plane skin depth measurements show that the resistive transition on entering the CDWx phase is both isotropic and representative of the bulk.

: J. Phys. C: Solid State Phys.

Prior to the development of the BCS theory of superconductivity , Fröhlich proposed a novel form of superconductivity in one-dimensional (1D) metals due to spontaneously sliding charge-density waves (CDWs) . CDWs were subsequently discovered in many materials containing quasi-one-dimensional (Q1D) Fermi-surface sections ; in such systems, a gap opens up over part or all of the Q1D Fermi-surface section(s) due to a nesting instability . However, this gap, and the pinning of the CDW to impurities, generally prevent a CDW from contributing to the electrical conductivity, so that the electrical transport properties are dominated by any remaining normal carriers . Conduction by sliding CDWs due to their depinning may occur under large electric fields, but is accompanied by considerable dissipation . In this respect, the organic conductor $`\alpha `$-(BEDT-TTF)2KHg(SCN)4 (together with the analogue compounds in which K has been substituted by Tl or Rb) may be an exception . This highly anisotropic layered metal exhibits what is thought to be a CDW with an exceptionally low transition temperature $`T_\mathrm{p}`$ 8 K . At applied magnetic fields ($`\mu _0H`$) greater than 23 T and temperatures ($`T`$) less than 2 K, $`\alpha `$-(BEDT-TTF)2KHg(SCN)4 possesses a phase which carries dissipationless currents .

In this Letter, we present compelling evidence that these currents are conveyed by the CDW itself. Measurements of the skin depth reveal that the currents propogate deep into the bulk of the material. Furthermore, the drop in resistivity with decreasing temperature is shown to be isotropic, possessing a form characteristic of a transition into an inhomogeneous superconducting phase.

Fröhlich’s original model neglects interactions with impurities ; these spatially pin the CDW, preventing the spontaneous sliding motion required for superconductivity . This pinning is often conveniently represented by a “particle” in a sinusoidally-varying ‘washboard’ potential . There are, however, limits in which this model should fail. For example, if the “particles’s” zero point energy $`\epsilon _0=\mathrm{}^2Q^2/4m^{}`$ exceeds the potential depth $`V`$, the washboard potential can no longer confine the CDW. Here, $`Q`$ is the wavevector (or nesting vector) representing the spatial periodicity of the potential and $`2m^{}`$ is the paired electron-hole mass, enhanced due to interactions between the CDW and the crystal lattice . The degree to which $`m^{}`$ is renormalised with respect to the effective mass characteristic of the unperturbed band ($`m_\mathrm{b}`$) is proportional to the square of the gap that opens at the Fermi energy on formation of the CDW .

The energy gap in $`\alpha `$-(BEDT-TTF)2KHg(SCN)4 at $`T=\mu _0H=`$ 0 can be estimated using the BCS relation $`2\mathrm{\Delta }_0=3.52k_\mathrm{B}T_\mathrm{p}`$ 3 meV . It has been suggested that this gap is closed by the Zeeman energy when $`\mu _0\mu _\mathrm{B}H/\sqrt{2}2\mathrm{\Delta }_0`$, corresponding to $`\mu _0H`$ 23 T ; this causes a first-order phase transition (the “kink” transition) into a proposed spatially modulated CDWx phase , (see notional phase diagram in Fig. 1). $`\alpha `$-(BEDT-TTF)2KHg(SCN)4 is therefore unusual in two respects: (1) it exhibits the only known CDW state in which $`\mathrm{\Delta }_0`$ is sufficiently small for such a transition to have been shown to occur in experimentally-accessible magnetic fields ; and (2) the reduced gap $`2\mathrm{\Delta }_x`$ 1 meV that characterizes the CDWx phase  is two orders of magnitude smaller than those in typical CDW materials . The smallness of the gap leads to a negligibly small enhancement of $`m^{}`$ with respect to $`m_\mathrm{b}`$ (in contrast to that in more typical CDWs), leading to estimates of $`\epsilon _0`$ in the range $`10^2`$ \- $`10^3`$ meV (using $`Q`$ 7 $`\times `$ 109 m-1 from Reference ). Hence $`\epsilon _0`$ greatly exceeds both $`2\mathrm{\Delta }_x`$ and $`V`$, given that $`V`$ must be less than $`\mathrm{\Delta }_x`$ for the CDW to be stable . These arguments lead one to expect that the CDWx phase may undergo the spontaneous sliding necessary for Fröhlich superconductivity . In the following, we will show that the resistivity and the magnetisation of $`\alpha `$-(BEDT-TTF)2KHg(SCN)4 within the CDWx phase do indeed exhibit behaviour characteristic of an inhomogeneous superconductor.

Figure 2 compares different measurements of the resistivity of $`\alpha `$-(BEDT-TTF)2KHg(SCN)4; the interplane resistivity component $`\rho _{zz}`$ is measured using conventional four-terminal transport . However, the highly anisotropic conductivity of $`\alpha `$-(BEDT-TTF)2KHg(SCN)4 makes it very difficult to measure the average in-plane resistivity $`\rho _{}`$ using such techniques . By contrast, the radio-frequency skin depth $`\delta _{}=\sqrt{2\rho _{}/\mu _0\omega }`$ enables both $`\rho _{}`$ and the extent to which the currents penetrate the sample to be determined simultaneously . The single-crystal sample is placed inside the inductor of a tunnel diode oscillator (TDO) tank circuit , with the oscillating magnetic field $`\stackrel{~}{𝐡}`$ perpendicular to the conducting layers. Screening within the sample results in a reduction in inductance, and consequently to an increase in the resonant frequency $`\omega /2\pi `$. Changes in frequency can be measured to high precision, with $`\delta _{}`$ being approximately related to $`\omega `$ by $`\delta _{}[\frac{1}{2}+(\omega \omega _0)/\eta \omega _0]r`$. Here, $`\omega _0/2\pi =`$ 38.975 $`\pm `$ 0.005 MHz is the resonant frequency without the sample, $`\eta =`$ 0.053 $`\pm `$ 0.002 is the effective filling factor of the sample with respect to the total inductance of the circuit and $`r=`$ 250 $`\pm `$ 50 $`\mu `$m is the effective sample radius .

Figure 2b shows $`\rho _{}`$ extracted from $`\delta _{}`$ at several different temperatures. At temperatures $`T>`$ 8 K, $`\alpha `$-(BEDT-TTF)2KHg(SCN)4 displays the positive magnetoresistance exhibited by most organic metals . At temperatures below 8 K, the magnetoresistance develops a semiconducting-type behaviour for 3 $`<\mu _0H<`$ 23 T (i.e. $`\rho _{}`$ increases with decreasing $`T`$), enabling $`\stackrel{~}{𝐡}`$ to fully penetrate; however, above 23 T, the resistivity is lower, the change becoming more distinct as the temperature decreases. The Shubnikov-de Haas (SdH) oscillations in Fig. 2 are due to an additional two-dimensional (2D) band  that, while remaining largely unaffected by the CDW order, becomes quantized in a series of sharply-defined Landau levels at high magnetic fields . Since the number of filled levels $`\nu `$ is proportional to $`1/B`$ (owing to an increase in the degeneracy of each level with magnetic induction $`B\mu _0H`$) , the field can be used to tune the position of the chemical potential relative to the Landau levels; at integer filling factors $`\nu =F/B`$, where $`F`$ is the frequency of the SdH oscillations, the chemical potential resides in a Landau gap between the highest filled and lowest empty Landau level.

The data in Fig. 2 are very important, because they show that in almost all respects, including the detailed phase behaviour of the SdH oscillations, the variation of $`\rho _{}`$ (estimated from $`\delta _{}`$) with $`\mu _0H`$ and $`T`$ at high fields is identical to that of $`\rho _{zz}`$. (Of course $`\rho _{zz}`$ is several orders of magnitude greater than $`\rho _{}`$ owing to the anisotropy of the band structure ). We can therefore assert that the changes taking place in the resistivity as a function of $`\mu _0H`$ and $`T`$ are intrinsic, bulk properties of $`\alpha `$-(BEDT-TTF)2KHg(SCN)4.

The temperature dependences of $`\rho _{zz}`$ and $`\rho _{}`$ are shown in Fig. 3 for both integer and half-integer $`\nu `$. Remarkably, the temperature dependence of $`\rho _{zz}`$ and $`\rho _{}`$ at integer $`\nu `$ is exactly the same as a transition into an inhomogeneous superconducting phase . In such systems, the (normally sharp) transition into the zero resistivity ground state becomes statistically broadened by a gaussian distribution with standard deviation $`\mathrm{\Delta }T_\mathrm{c}`$ about a mean critical temperature $`\overline{T}_\mathrm{c}`$ . As can be seen in Fig. 3, the convolution of a sharp transition into a zero resistivity state with gaussian broadening (i.e. the error function) provides an excellent fit to both the $`\rho _{zz}`$ and $`\rho _{}`$ data at integer filling factors. This implies that an increasing fraction of the sample no longer contributes to the resistivity as $`T`$ is lowered, in a manner consistent with the carriers (within this fraction) having condensed into a superconducting phase. As $`\mathrm{\Delta }T_\mathrm{c}`$ 1 K is a significant fraction of $`\overline{T}_\mathrm{c}`$ 2 K, the transition is never entirely complete, so that the total resistivity of the inhomogeneous phase does not actually fall to zero at $`T=`$ 0. Instead, the resistivity drops off exponentially in the limit $`T`$ 0 (i.e. $`\rho \mathrm{e}^{T/T_0}`$) in a manner similar to that observed in several well-known examples of inhomogeneous superconductors . This resistivity model can also be fitted to the data at half-integer filling factors with a very similar $`\overline{T}_\mathrm{c}`$, but with the transition width $`\mathrm{\Delta }T_\mathrm{c}`$ being considerably broadened. The fact that the midpoint of the transition $`\overline{T}_\mathrm{c}`$ is virtually unaffected by the Landau-level filling factor of the 2D quasiparticles (see Figure 1 inset) is consistent with the gap formation being solely determined by the Q1D sheets. The Q2D Landau density of states appears only to modulate the width of the transition, possibly as a result of its influence on the scattering rate; there is an increased density of available states at the chemical potential at half-integer filling factors(see Fig. 1 inset) .

Finally, we turn to the magnetisation, which exhibits a behaviour entirely consistent with that of an inhomogeneous superconductor in the CDWx phase. Figure 4a shows an example of a hysteresis loop in the irreversible magnetisation $`M`$ obtained using a torque magnetometer (see Reference  for a detailed description of this technique); two important features of this loop are consistent with Bean’s critical state model for vortex pinning in type II superconductors . Firstly, the irreversible magnetic susceptibility $`M/H`$ is diamagnetic (i.e. negative) or reversing the direction of sweep of $`H`$ ; this effect can only be ascribed to circulating currents  (while circulating currents are not expected in a purely 1D CDW system, they can occur in 2D CDW systems such as $`\alpha `$-(BEDT-TTF)2KHg(SCN)4 ). Secondly, the magnitude of the hysteresis saturates at a critical value $`M_{\mathrm{sat}}`$ enabling us to identify a critical current density $`j_\mathrm{c}`$ . Because the hysteresis occurs at all filling factors $`\nu `$, the currents cannot originate from the quantum Hall effect (QHE), as earlier experiments had appeared to suggest . In the limit $`\nu `$ 1 that applies here, the QHE is expected to operate only at integer filling factors .

Thus, our reasons for attributing these effects within the high magnetic field phase of $`\alpha `$-(BEDT-TTF)2KHg(SCN)4 to Fröhlich superconductivity  can be summarized as follows: (1) the semiclassical model for CDW pinning is expected to fail ; (2) both the magnetisation and the resistivity display effects found only in superconductors; the induced currents are consistent with Bean’s critical state model , while the resistivity has exactly the form of a transition into an inhomogeneous superconducting phase ; (3) these effects are observed at all filling factors for $`\mu _0H>`$ 23 T; and (4) only a single resistive transition is observed as a function of $`T`$ on entering the region in $`H`$ and $`T`$ over which the currents are observed, with the midpoint $`\overline{T}_\mathrm{c}`$ of this transition (being virtually independent of the 2D density of states) coinciding with the transition into the CDWx phase predicted by theory .

The small diamagnetic fraction ($`M/H`$ 1 %) , large skin depth ($`\delta _{}>`$ 30 $`\mu `$m, being an appreciable fraction of $`r`$) and broadness of the resistive transition ($`\mathrm{\Delta }T_\mathrm{c}13`$ K) all suggest that the persistent currents are confined to many small islands or filaments throughout the sample surrounded by regions that are normal. Fig. 4b provides further support for this picture, where it is apparent that both the size of the irreversible magnetisation $`M`$ and the conductivity $`1/\rho `$ obey an approximate $`\mathrm{e}^{T/T_0}`$ law in the limit $`T`$ 0 (see Fig. 4b). It is interesting that the transition width $`\mathrm{\Delta }T_\mathrm{c}`$ is so broad for a material that should most definitely be in the clean limit. We can infer this from the fact that the mean free path $`l=v_\mathrm{F}\tau `$ 4000 Å (estimated from the results of de Haas-van Alphen measurements , where $`v_\mathrm{F}`$ 80,000 ms-1 is the Fermi velocity) greatly exceeds the coherence length $`\zeta _0=\mathrm{}v_\mathrm{F}/\pi \mathrm{\Delta }`$ 200 Å(conservatively estimated using the BCS formula ). Should $`\alpha `$-(BEDT-TTF)2KHg(SCN)4 possess a vortex state, inhomogeneity could be a consequence of the transition being broadened by a magnetic field in a similar manner to that observed in other highly anisotropic superconductors . Another possibility to consider is that, unlike Cooper pairs in conventional superconductors , a CDW charge modulation experiences additional Coulomb interactions with impurities . While the Coulomb force may not necessarily be able to pin the CDW condensate if $`\mathrm{\Delta }`$ is too small, it may still affect the stability of the CDW order should $`V`$ become comparable to $`\mathrm{\Delta }`$ (see Reference ).

In conclusion, both transport and magnetisation measurements within the low temperature, high magnetic field CDWx phase of $`\alpha `$-(BEDT-TTF)2KHg(SCN)4 are shown to be consistent with inhomogeneous superconductivity, realised in small filaments or islands throughout the bulk of the sample. The locality of this effect with respect to the CDW phase diagram in $`H`$ and $`T`$ leads us to propose that Fröhlich superconductivity (or perhaps a 2D variant thereof ) is realised in this material at high magnetic fields.

This work is supported by the Department of Energy, the National Science Foundation (NSF) and the State of Florida. JS acknowledges EPSRC (UK) for support. We should like to thank Albert Migliori and Steve Blundell for useful discussions.


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# Active Membrane Fluctuations Studied by Micropipet Aspiration

## I Introduction

Biological membranes are made up of a complex mixture of lipids and proteins. The lipid molecules form a bilayer structure which separates the cytoplasm of the cell from the outside. In addition to this structural role, the membrane also participates in a number of the living cell functions , mostly performed by proteins embedded inside the lipid bilayer, such as solute transport via ion channels or pumps, cell locomotion and adhesion, membrane transport through exocytic and endocytic pathways, signal transduction… Consequently, from the statistical physics point of view, biological membranes are strongly out of thermodynamic equilibrium, whereas most studies on membranes reported in the physics literature have been done at thermodynamic equilibrium . In order to achieve a more complete physical description of biological membranes, this nonequilibrium aspect clearly has to be included. The field of membrane shape fluctuations is a good test case in which to examine the relevance of nonequilibrium effects. At thermodynamic equilibrium, the membrane shape fluctuates because of thermal noise, i.e., the Brownian motion of the bilayer. Such membrane will be called a ‘passive’ membrane in this paper. If a nonequilibrium noise source is superimposed to thermal noise, due for instance to the activity of membrane proteins, then the membrane is no longer at thermodynamic equilibrium. In that case, the membrane will be called ‘active’.

Recently, micropipet experiments on fluctuating giant vesicles containing bacteriorhodopsin (BR) reconstituted in the lipid bilayer have shown that the light-driven proton pumping activity of BR induces an amplification of the membrane shape fluctuations . In these experiments, a larger excess area could be pulled out by micropipet aspiration when the proteins were activated. The results were qualitatively interpreted in terms of an increase of the effective membrane temperature and were not directly compared to theoretical predictions. In the present article, we give details about the experimental procedure (section II) and develop a theoretical framework to analyze quantitatively the micropipet experiments (sections III and IV). According to theory, a qualitatively new fluctuation spectrum is expected in the presence of a nonequilibrium noise source . These earlier theories introduced the nonequilibrium activity in the membrane conformation equation only. This restrictive choice was made because the nonequilibrium force-density arising from the active proteins, when included in the Stokes equation for the solvent velocity field, altered the membrane fluctuation spectrum through terms which were subdominant at small wavenumber.

We show here that those nominally subdominant terms provide the most important contribution in the experimentally relevant range. This unexpected behavior is due to the very small value of the permeation coefficient. With this implementation, theory and experiment are brought in agreement (section IV). Even the absence of sensivity of the experimental data on the active center density appears as a natural consequence of the developed theory.

## II Experimental procedure and results

### A Bacteriorhodopsin

The bacteriorhodopsin (BR) is a $`27`$ kDa protein  purified from the so-called purple membrane of the halophilic bacteria Halobacterium salinarum . Its structure is known at the atomic level with high resolution . The BR absorption spectrum shows a maximum in the green-yellow wavelength around $`566`$ nm (Fig. 1).

When illuminated with green-yellow light, proton pumping is activated through a photocycle involving several distinct photointermediates . The total duration of the photocycle is $`\tau 5`$ ms. Structural changes of the BR during the photocycle have been investigated to elucidate the translocation pathway of the proton across the protein. The pumping mechanism has been recently completely elucidated, so that BR is to date the best understood ion pump . The proton pumping activity has been extensively studied in reconstituted systems, mostly in large unilamellar vesicles ($`0.11\mu \mathrm{m}`$ in diameter) .

### B Giant vesicle formation

In reference , the electroformation technique of giant unilamellar vesicles ($`10100\mu \mathrm{m}`$ in diameter) , modified according to  for BR incorporation in the lipid bilayer, was used to grow giant vesicles from a mixed lipid/protein dried film. The phospholipid EPC (Egg Phosphatidylcholine; Avanti Polar Lipids, Alabaster, Alabama, USA) is a mixture of lipids with different chain lengths and degrees of saturation and is known to be adequate for BR incorporation . EPC ($`0.5`$ mg/ml) was first resuspended in diethyl ether. Concentrated BR ($`18`$ mg/ml) was then added at a molar ratio of $`80`$ lipid molecules per BR molecule. The mixture was sonicated at $`0{}_{}{}^{\mathrm{o}}\mathrm{C}`$ for $`30`$ seconds and a few microliters were deposited on ITO (Indium Tin Oxide) treated glass slides at $`4{}_{}{}^{\mathrm{o}}\mathrm{C}`$. The protein/lipid film was dried under vacuum overnight. A vesicle electroformation chamber was formed by assembling and sealing with wax (Sigillum wax; Vitrex, Copenhagen, Denmark) two ITO slides separated by $`1`$ mm Teflon spacers. The film was hydrated by injecting a $`50`$ mM sucrose solution in the chamber. An electric field ($`1.5`$ V AC) was applied across the chamber by connecting the ITO slides to copper electrodes. Giant vesicles were obtained in about two hours and transferred in a micromanipulation chamber filled with $`50`$ mM glucose to enhance the optical contrast between the inside and the outside of the vesicles. Sodium azide ($`1`$ mM) was first added to the sucrose and glucose solutions to avoid bacteria proliferation. In some experiments, respectively $`16`$ and $`25\%`$ (w/w) glycerol was added to both the internal and external solutions in order to increase the viscosity to respectively $`1.5\eta _w`$ and $`2\eta _w`$, where $`\eta _w`$ is the viscosity of water.

BR incorporation was checked by fluorescent labelling of BR with FITC (Fluorescein Isothiocyanate, F-143; Molecular Probes, Eugene, Oregon, USA) following a published protocol . Excitation of the FITC was performed at $`488`$ nm with an argon laser (Spectra Physics, Les Ulis, France) through the epi-illumination pathway of an inverted microscope (Axiovert $`135`$; Zeiss, Oberkochen, Germany). The fluorescence images of the vesicles were acquired by a low light level SIT (Silicon Intensified Target) camera (LH4036; Lhesa, France) (see Fig. 2). The fluorescence intensity $`I_F=(I_{ves}I_{bgd})/I_{bgd}`$, where $`I_{ves}`$ is the fluorescence intensity of the vesicle contour and $`I_{bgd}`$ is the background intensity, was measured by computer image analysis using a C++ custom software running on a Pentium 200-based computer with a Meteor frame grabber (Matrox, Rungis, France).

The BR was activated by illumination through a high-pass ($`500`$ nm) green-yellow filter located in the trans-illumination pathway (see Figs. 1 and 2), to avoid the non-pumping branched photocycle initiated if the M intermediate absorbs at $`440`$ nm . To image the vesicles without activating the BR, a high-pass ($`650`$ nm) red filter was substituted for the green-yellow filter (see Figs. 1 and 2). The illumination power was in the same range as that known to fully activate BR reconstituted in large unilamellar vesicles ($`10^3\mathrm{W}/\mathrm{m}^2`$) . To correct for the different bandwidths of the green-yellow and red filters, the trans-illumination light focused on the specimen plane was adjusted to about $`100\mathrm{mW}/\mathrm{cm}^2`$ in all the experiments. The sample was illuminated for at least $`15`$ minutes before starting an experiment, so that the BR was always in its light-adapted form .

It has been shown that the reverse phase evaporation technique used to incorporate BR in large unilamellar vesicles (typically $`200`$ nm in diameter) results in an asymmetrical orientation of the BR molecules across the lipid bilayer . Consequently, for these vesicles, a proton gradient builds up across the lipid membrane upon activation, which inhibits BR pumping activity. However, since the electroformation technique is symmetrical, we do not expect any asymmetry in the BR orientation, and thus we do not expect inhibition of the pumping activity. To be on the safe side, we have performed additional experiments which were designed to cancel any proton gradient according to the following procedure. A classical way of suppressing the inhibitory proton gradient, without incorporating any additional active molecule in the membrane, is to add KCl (potassium chloride) to the solution, since protons can then codiffuse passively through the bilayer in the form of HCl, and since chloride ions can diffuse inside the vesicle to ensure electroneutrality. In reference , KCl was added to both the internal and external solutions up to $`2`$ mM, a concentration above which electroformation of giant vesicles fails, in order to get rid of a possible proton gradient. Our results proved to be insensitive to the addition of KCl .

### C Micropipet experiments

The micropipet technique developed by Evans and coworkers  allows a quantification of the excess surface area stored in the membrane fluctuations by pulling it out with a micropipet aspiration: when a pressure difference is applied, the membrane is put under tension and sucked inside the pipet. The experimental set-up was built on an inverted microscope equipped with a $`40`$x objective (N.A. 0.75 air Ph2 Plan Neofluoar, Zeiss) for epi-fluorescence, phase contrast and differential interference contrast (DIC) microscopy. The transmission phase contrast or DIC images were recorded by a CCD (Charge Coupled Device) camera (Sony, Paris, France). The sample cell was temperature controlled at $`15{}_{}{}^{\mathrm{o}}\mathrm{C}`$ by a water flow to limit evaporation of the solution (see Fig. 2, bottom).

Glass micropipets were pulled from $`1`$ mm outer diameter borosilicate capillaries (GC 100T-10; Phymep, Paris, France) with a micropipet-puller (P-97; Sutter Instruments Co., Novato, California, USA). The micropipet tip was cut on a microforge to obtain diameters up to $`510\mu \mathrm{m}`$. The pipets were treated with BSA (bovine serum albumin, $`1\%`$) for $`30`$ minutes to prevent adhesion of the lipid membrane to the glass pipet walls. A pipet holder was mounted on a three-dimensional piezo micromanipulator stage (Physik Instrumente, Waldbron, Germany) in order to control the position of the pipet tip within $`0.1\mu \mathrm{m}`$ accuracy. The pressure difference $`\mathrm{\Delta }P`$ between the outside and the inside of the pipet was measured by a liquid-liquid pressure transducer (DP103-20; Validyne, SEI3D, France) with $`0.01`$ Pa accuracy. The pressure is imposed by a water height difference between two water filled tanks equipped with micrometric displacements (see Fig. 2, bottom). The absence of any air bubble in the water circuit running from the tanks to the micropipet is crucial and was checked before each experiment. The relationship between the pressure difference $`\mathrm{\Delta }P`$ and the imposed membrane tension $`\sigma `$ directly derives from Laplace’s law :

$$\sigma =\frac{R_{pip}}{2(1R_{pip}/R_{ves})}\mathrm{\Delta }P$$

where $`R_{pip}`$ is the pipet radius and $`R_{ves}`$ is the vesicle radius, both measured directly from the DIC image (see Fig. 3).

The excess area stored in the membrane shape fluctuations $`\alpha `$ is defined as $`\alpha =(AA_p)/A`$, where $`A`$ is the actual area of the fluctuating membrane and $`A_p`$ is the area projected on the mean plane of the membrane. During a micropipet experiment, the excess area decreases as the membrane undulations are pulled out by the increasing pressure difference. For a given $`\mathrm{\Delta }P`$, an intrusion length $`L`$ is aspirated inside the pipet (see Fig. 3). A reference state $`(\mathrm{\Delta }P_0,L_0)`$ is defined as the lowest suction pressure that can be applied in the experiment to aspirate the fluctuating vesicle inside the micropipet . The variation of the excess area as compared to this reference state, the so-called areal strain $`\mathrm{\Delta }\alpha =\alpha _0\alpha `$, follows from geometrical considerations. To first order in $`\mathrm{\Delta }L=LL_0`$, we have :

$$\mathrm{\Delta }\alpha =\alpha _0\alpha =\frac{(R_{pip}/R_{ves})^2(R_{pip}/R_{ves})^3}{2R_{pip}}\mathrm{\Delta }L$$

The increase of the intrusion length $`\mathrm{\Delta }L`$ was measured by image analysis with pixel accuracy, i.e. $`0.2\mu \mathrm{m}`$ with the $`40`$x objective.

The excess area can be expressed using the local displacement $`u`$ of the membrane around its mean plane :

$$\alpha =(_{}u)^2/2=\frac{1}{(2\pi )^2}_0^{q_{max}}\frac{1}{2}q_{}^2u(𝐪_{})^22\pi q_{}𝑑q_{}$$
(1)
In the low q regime the convergence of the integral is guaranteed by a crossover from a curvature dominated regime $`u(𝐪_{})^2=kT/\kappa q_{}^4`$ to a tension dominated regime $`u(𝐪_{})^2=kT/\sigma q_{}^2`$ for a passive membrane, where $`k`$ is the Boltzmann constant, $`T`$ is the absolute temperature and $`\kappa `$ is the bending modulus of the membrane. The upper limit is $`q_{max}=2\pi /a`$, where $`a`$ is a microscopic length. In the entropic regime, i.e. at low tension, inserting the fluctuation spectrum of an equilibrium membrane gives the dependence of the excess area $`\alpha `$ as a function of the membrane tension $`\sigma `$ : $`\alpha =(kT/8\pi \kappa )\mathrm{ln}(cst/\sigma )`$, where $`cst`$ is an integration constant. The areal strain $`\mathrm{\Delta }\alpha =\alpha _0\alpha `$ is thus:

$$\mathrm{\Delta }\alpha =\alpha _0\alpha =\frac{kT}{8\pi \kappa }\mathrm{ln}\frac{\sigma }{\sigma _0}.$$
(2)
For a passive membrane, the linear relationship between the logarithm of the tension $`\mathrm{ln}\sigma `$ and the areal strain $`\mathrm{\Delta }\alpha `$ allows the determination of the bending modulus $`\kappa `$. We will give in section IV a similar relation relevant to the active case.

### D Essential results

The results reported in  and duplicated in Figure 4 show that when the vesicles are illuminated with green-yellow light, the slope of the logarithm of tension versus the areal strain is smaller than in the case where the vesicles are illuminated with red light. This indicates that the excess area is larger when the BR is illuminated with green-yellow light, and consequently that BR activity induces an amplification of the membrane shape fluctuations. The quality of the fit suggests that one can describe the effect of the BR activity in terms of an effective temperature $`T^{eff}2T`$.

An other important feature of the experiment concerns the dependence of $`T^{eff}`$ on BR concentration. Fig. 5 shows that in a concentration range that we estimate between approximatively $`10^{15}`$ and $`10^{16}\mathrm{BR}/\mathrm{m}^2`$ the effective temperature is essentially independent on BR concentration. This may look surprising since the BR activity is the driving force.

Before developing the interpretation of these results, we must first guarantee their reliability, i.e. that it is an effect related to the out-of-equilibrium pumping activity of BR and nothing else. The control experiments with pure lipid vesicles obviously exclude a role of the lipids themselves. For these, we find for both green-yellow and red illumination the expected $`kT/\kappa 0.1`$ value . Using simple estimates, we can also rule out the possibility of any thermally induced artefact due to the larger absorption of light by BR in the green-yellow wavelength. Assuming that one BR molecule absorbs one photon each $`\tau 5`$ ms, the total stationary flux (total energy received per unit area of membrane and per unit of time) is:

$$W=\frac{h\nu }{\tau }\times \overline{\rho }$$

where $`h`$ is the Planck constant, $`\nu `$ is the photon frequency and $`\overline{\rho }`$ is the mean BR density. In a pessimistic estimate, we assume that this total flux $`W`$ is dissipated via conduction in the surrounding water. The sample cell is temperature controlled by a cold water circulation and we assume that a temperature gradient arises from the BR heating between the membrane and the sample cell wall. This gradient extends over a typical length $`L=1`$ mm which is the size of the sample cell. With $`C=4.18\times 10^6\mathrm{J}.\mathrm{m}^3.{}_{}{}^{\mathrm{o}}\mathrm{K}_{}^{1}`$ the heat capacity of water and $`K_T=1.5\times 10^7\mathrm{m}^2/\mathrm{s}`$ the heat diffusion coefficient, we have:

$$CK_T\frac{\mathrm{\Delta }T}{L}=W=\frac{h\nu }{\tau }\times \overline{\rho }$$

and

$$\mathrm{\Delta }T=\frac{h\nu }{\tau }\times \overline{\rho }\times \frac{L}{CK_T}$$

This yields a temperature increase of $`\mathrm{\Delta }T=2\times 10^3{}_{}{}^{\mathrm{o}}\mathrm{K}`$, five orders of magnitude smaller than the reported increase in effective temperature, which can not account for the observed effect . Direct heating is just totally inefficient (note also that direct heating of water is clearly ruled out by the experiments on pure phospholipidic vesicles).

Most importantly, the experiments with glycerol prove that the observed effect is of nonequilibrium origin. The addition of glycerol modifies dynamic parameters such as the solvent viscosity $`\eta `$, the permeation coefficient $`\lambda _p`$ and the active force $`F_a`$. At thermodynamic equilibrium, such parameters cannot play a role in the fluctuation spectrum as imposed by the fluctuation-dissipation theorem. For an active membrane however, these parameters play a role as can be seen from references  or . The addition of glycerol increases the solvent viscosity while it decreases its permeation coefficient. The results given in reference  report a lower increase in the effective temperature when $`16\%`$ and $`25\%`$ (w/w) glycerol is added, clearly revealing the out of equilibrium nature of the effect. This result is qualitatively consistent with the observation that the BR pumping activity is diminished upon addition of glycerol due to an increase in the lifetime of the M intermediate . Finally, the fact that the observed effect does not depend on the measuring sequence (red light experiment or green light experiment first) rules out a potential role of the conformational change between the light-adapted and the dark-adapted states . This is also consistent with the result that the ratio $`kT/\kappa `$ in the passive case is the same as that of the pure phospholipidic vesicles. The renormalisation of the bending rigidity by the BR is not measurable. All these observations give strong support to the assertion that the effect is indeed due to the proton pumping activity.

The use of an effective temperature to qualitatively interpret the results according to equation (2) is justified by the good quality of the linear fits of the micropipet experiments performed in . However, we need to develop a complete theoretical analysis to understand all these experimental features quantitatively.

## III Theory

As in references , we consider situations in which a membrane under tension is subjected to random forces of two different origins. These arise (i) from thermal agitation, i.e., the Brownian motion of the membrane, simply because membrane and solvent have a thermodynamic temperature, and (ii) from ‘biological’ activity such as proton pumping of the BR. The membrane equation of motion can be written to lowest order:

$$\lambda _P^1(\frac{u}{t}(𝐫_{},t)V_z(𝐫_{},t))=\delta P(𝐫_{},t)\delta \mathrm{\Pi }(𝐫_{},t)+F_a\psi (𝐫_{},t)+F_a^{}\rho \mathrm{\Delta }_{}u(𝐫_{},t)+f_p(𝐫_{},t)$$
(3)
In this expression, $`u(𝐫_{},t)`$ is the membrane displacement at point $`𝐫_{}=(x,y)`$ with respect to a $`(x,y)`$ reference plane orthogonal to $`\widehat{𝐳}`$, the average membrane normal and $`\mathrm{\Delta }_{}`$ is the Laplacian in the $`xy`$ plane. $`V_z(𝐫_{},t)`$ is the fluid velocity, in the normal direction at the membrane surface; $`\lambda _P`$ is the membrane permeation coefficient. $`\delta P(𝐫_{},t)=P(𝐫_{},z=0^+,t)P(𝐫_{},z=0^{},t)`$ is the pressure difference across the membrane and $`\delta \mathrm{\Pi }(𝐫_{},t)=\mathrm{\Pi }(𝐫_{},z=0^+,t)\mathrm{\Pi }(𝐫_{},z=0^{},t)`$ the osmotic pressure difference. This osmotic pressure difference results from the proton pumping activity: for each BR cycle one proton is transferred across the membrane. In principle the calculation of $`\delta \mathrm{\Pi }`$ cannot be achieved without solving all dynamical equations of the problem. However, considering the convective term of the proton flux as a second order correction allows to evaluate $`\delta \mathrm{\Pi }`$ separately. We postpone this derivation to appendix A. $`f_p`$ is the brownian noise acting on the membrane corresponding to the dissipation of energy in the permeation process and satisfies:

$$f_p(𝐫_{},t)=0$$

$$f_p(𝐫_{},t)f_p(𝐫_{}^{},t^{})=2kT\lambda _P^1\delta (𝐫_{}𝐫_{}^{})\delta (tt^{})$$

The term $`F_a\psi (𝐫_{},t)`$ results from the BR activity. More precisely $`\psi (𝐫_{},t)=\rho ^{}(𝐫_{},t)\rho ^{}(𝐫_{},t)`$ is the local difference between the density $`\rho ^{}(𝐫_{},t)`$ of BR molecules transferring protons in the direction $`\widehat{𝐳}`$ (up) and the density $`\rho ^{}(𝐫_{},t)`$ of BR molecules transfering protons in the -$`\widehat{𝐳}`$ direction (down). $`F_a`$ is the average elementary force transmitted to the membrane by a steady proton transfer. The flip-flop of BR is expected to be much slower than that of phospholipids and thus $`\rho ^{}(𝐫_{},t)`$ and $`\rho ^{}(𝐫_{},t)`$ can be considered as separately conserved quantities. As explained in section II, with our experimental conditions, the probability of inserting a BR molecule into the phospholipid membrane does not depend on the pumping direction, thus $`\rho ^{}=\rho ^{}`$ and $`\psi =0`$. $`\lambda _PF_a`$ can be understood as measuring the average volume transferred through the membrane per BR and per unit time. Thus, $`\lambda _PF_a\psi (𝐫_{},t)`$, which we will refer to as the ‘active-permeative’ term, can also be understood as the local volume transferred through the membrane per unit area and per unit time due to the pumping imbalance between up and down BR molecules. Terms corresponding to the stochastic nature of the pumping activity have been omitted since they have been shown to lead to smaller effects than those due to the collective $`\psi `$ fluctuations . As discussed in , the fourth term describes the fact that pumping may work better when the membrane is curved with a given sign: $`F_a^{}`$ measures this sensitivity per pump and $`\rho =\rho ^{}(𝐫_{},t)+\rho ^{}(𝐫_{},t)`$. There is experimental evidence for such a coupling in the functioning of certain ion-channels called TRAAK and TREK .

We further need equations for the fluid and for the BR density dynamics. Navier-Stokes equations have to be implemented in two ways: one first has to keep track of the Laplace force exerted by the membrane on the fluid, and this can be done in the usual way .

Secondly, each BR has a small but finite spatial extent. Its activity will disturb the ambient solvent in the form of a distribution of force densities in its vicinity. Since no external force source is present, the total force must vanish, but its first moment will in general be present. For convenience, we adopt the simplest set of force-densities consistent with this requirement: a pair of oppositely directed point forces, separated by a distance of order the size of a BR molecule. This implies a dipolar force density $`F_a\left[\delta (zw^{})\delta (z+w^{})\right]\psi (𝐫_{},t)`$ in the Stokes equations (this term will be called the ‘active-hydrodynamic’ term). $`w^{}`$ and $`w^{}`$ are lengths of the order of the BR size; their values are a priori unequal since the BR, or any molecule with unidirectional activity, is not up-down symmetric. Similarly, the term $`F_a^{}[\delta (zw^{})\delta (z+w^{}]\rho \mathrm{\Delta }_{}u(𝐫_{},t)`$ describing the sensitivity of the force dipole to curvature should be kept. Thus, in the low Reynolds number regime appropriate to these experiments, we can write:

$$\begin{array}{ccc}\hfill 0& =& P(𝐫,t)\frac{\delta F}{\delta u}(𝐫_{},t)\delta (z)\widehat{𝐳}\hfill \\ & & +F_a\left[\delta (zw^{})\delta (z+w^{})\right]\psi (𝐫,t)\widehat{𝐳}\hfill \\ & & +F_a^{}\mathrm{\Delta }_{}u\left[\delta (zw^{})\delta (z+w^{})\right]\rho (𝐫_{},t)\widehat{𝐳}\hfill \\ & & +\eta \mathrm{\Delta }𝐕(𝐫,t)+𝐟_h(𝐫,t),\hfill \end{array}$$
(4)
where $`𝐫`$ refers to the three-dimensional position vector, and $`𝐫_{}`$ has the same meaning as in (3). $`P(𝐫,t)`$ is the three-dimensional pressure field, $`𝐕(𝐫,t)`$ the three-dimensional fluid velocity field, $`F`$ is the membrane free energy:

$$F=\frac{1}{2}d^2𝐫_{}\left[\kappa (\mathrm{\Delta }_{}u(𝐫_{}))^2+\sigma (u(𝐫_{}))^22\mathrm{\Xi }\psi (𝐫_{})\mathrm{\Delta }_{}u+\chi \psi ^2(𝐫_{})\right]$$

$`\kappa `$ is the membrane ‘bare’ bending modulus, $`\sigma `$ the membrane tension, $`\mathrm{\Xi }`$ a coefficient linking membrane curvature and BR imbalance, $`\chi `$ the ‘bare’ susceptibility corresponding to that imbalance (for small enough densities $`\chi kT/\rho `$). Orders of magnitude will be given in the next section. The third term of equation (4), is the ‘force dipole’ density already described, the fifth and sixth are the usual viscous terms and associated forces:

$`\begin{array}{c}𝐟_h(𝐫,t)=0\\ f_{hi}(𝐫,t)f_{hj}(𝐫^{},t^{})=2kT\eta \{\delta _{ij}^2+_i_j\}\delta (𝐫𝐫^{})\delta (tt^{})\end{array}`$

Last, we need a dynamical equation for the BR imbalance density $`\psi `$. Following , we can write in the linear regime:

$$\frac{\psi }{t}=\mathrm{\Lambda }\mathrm{\Delta }_{}\frac{\delta F}{\delta \psi }+_{}𝐟_\psi $$
(5)
with $`\mathrm{\Lambda }=D/\chi `$, where $`D`$ is the diffusion coefficient of the BR molecules in the membrane. This expression is valid for $`\psi =0`$, in the absence of fluctuation corrections, and the last term of (5) is a conserving noise, i.e., the divergence of a random current with

$`\begin{array}{c}𝐟_\psi (𝐫_{},t)=0\\ f_{\psi i}(𝐫_{},t)f_{\psi j}(𝐫_{}^{}{}_{}{}^{},t^{})=2\mathrm{\Lambda }kT\delta _{ij}\delta (𝐫_{}𝐫_{}^{})\delta (tt^{})\end{array}`$

In order to compare experiment and theory, we need to calculate the equal time correlation function $`u(𝐪_{},t)u(𝐪_{}^{},t)`$. We first eliminate $`V_z`$ in (3) by solving for it from the Stokes equation (4) in Fourier space to get:

$$\frac{u}{t}(𝐪_{},t)+\tau _u^1u(𝐪_{},t)=\beta \psi (𝐪_{},t)+\mu $$
(6)
$$\frac{\psi }{t}(𝐪_{},t)+\tau _\psi ^1\psi (𝐪_{},t)=\gamma u(𝐪_{},t)+\nu $$
(7)
in which we have chosen the convention

$`f(𝐪_{},t)={\displaystyle f(𝐫_{},t)\mathrm{exp}(i𝐪_{}𝐫_{})d^2𝐫_{}}`$

for Fourier transforms, and used $`\delta \mathrm{\Pi }2kT\dot{a}\psi (𝐪_{},t)/D_Pq_{}`$ where $`\dot{a}`$ is the proton pumping rate and $`D_P`$ an effective proton diffusion coefficient (see appendix A). The parameters entering equations (6) and (7) are listed below:

$`\begin{array}{cc}\tau _u^1=(\lambda _P+\frac{1}{4\eta q_{}})(\sigma q_{}^2+\kappa q_{}^4)+\rho \lambda _PF_a^{}q_{}^2\frac{\rho 𝒫_a^{}w}{4\eta }q_{}^3\hfill & \\ \tau _\psi ^1=\mathrm{\Lambda }\chi q_{}^2=Dq_{}^2\hfill & \hfill \overline{F_a}=F_a2kT\dot{a}/D_Pq_{}\\ \beta =\lambda _P\overline{F_a}𝒫_a\frac{q_{}w}{4\eta }\mathrm{\Xi }q_{}^2(\lambda _P+\frac{1}{4\eta q_{}})\hfill & \hfill 𝒫_a=F_a\frac{w_{}^2w_{}^2}{2w}\\ \mu =\lambda _Pf_p(𝐪_{},t)+\frac{1}{2\pi \eta }\frac{𝐟_h(𝐪,t)\widehat{𝐳}}{q^2}𝑑q_z\hfill & \hfill 𝒫_a^{}=F_a^{}\frac{w_{}^2w_{}^2}{2w}\\ \gamma =\mathrm{\Lambda }\mathrm{\Xi }q_{}^4\hfill & \\ \nu =i𝐪_{}𝐟_\psi (𝐪_{},t)\hfill & \end{array}`$

Calculating the equal time $`u(𝐪_{},t)u(𝐪_{}^{},t)`$ correlation function is straightforward although somewhat tedious; we find

$$u(𝐪_{},t)u(𝐪_{},t)=\frac{kT}{(\tau _u^1+\tau _\psi ^1)(\tau _{u}^{e}{}_{}{}^{1}+\tau _a^1)}\left[\frac{(\lambda _PF_a𝒫_a\frac{q_{}w}{4\eta })^2}{\chi }+(\tau _u^1+\tau _\psi ^1+\tau _a^1)(\lambda _P+\frac{1}{4\eta q_{}})\right]$$
(8)
with

$$\tau _a^1=\frac{\mathrm{\Xi }}{\chi }q_{}^2\left(\lambda _PF_a𝒫_a\frac{q_{}w}{4\eta }\right)$$

$`\tau _{u}^{e}{}_{}{}^{1}`$ has exactly the same structure than $`\tau _u^1`$, but $`\kappa `$ is replaced by $`\kappa ^e=\kappa \mathrm{\Xi }^2/\chi `$. Note that in the absence of active noise, (8) reduces to its thermal equilibrium expression, as it should.

In the long wavelength limit, one finds for a membrane under tension (neglecting the osmotic contribution):

$$u(𝐪_{},t)u(𝐪_{},t)=\frac{kT^e}{\sigma q_{}^2}$$
(9)
with $`T^e=T(1+16\lambda _P^2F_a^2\eta ^2/\chi \sigma )`$ which means that a tense membrane is flat at longwavelength, even in the presence of non-thermal noise, and that one can define an effective temperature higher than the actual one.

For a tensionless membrane, we now find for $`q_{}0`$:

$$u(𝐪_{},t)u(𝐪_{},t)=\frac{kT_{}^{}{}_{}{}^{e}}{\kappa q_{}^4}$$
(10)
with $`T_{}^{}{}_{}{}^{e}=T(\lambda _PF_a)^2\kappa /[\chi (D+\rho \lambda _PF_a^{})(\rho \lambda _PF_a^{}+\frac{\mathrm{\Xi }}{\chi }\lambda _PF_a)]`$. This expression is equivalent to the one given in , and in particular the effective temperature does not depend on the pumping density for small enough densities. At long enough wavelength, the osmotic term should always dominate, but we show in the next section that the experimentally relevant regimes in fact imply the contribution of the force dipoles.

## IV Experimentally relevant regime and discussion

Let us first point out that in all equations the active-permeative and the active-hydrodynamic terms come in the combination:

$`\lambda _PF_a{\displaystyle \frac{𝒫_a}{4\eta }}q_{}w`$

This tells us that in the long wavelength limit, the active-permeative term always dominates over the active-hydrodynamic term. However, the crossover wavevector, below which the active-permeative term wins reads:

$`q_c={\displaystyle \frac{4(\eta \lambda _P)F_a}{w𝒫_a}}`$

or for the corresponding length:

$`l_c=2\pi {\displaystyle \frac{w}{4\eta \lambda _P}}({\displaystyle \frac{𝒫_a}{F_a}})`$

That is with $`\eta \lambda _P=l_P`$ the permeation length, and $`𝒫_a/F_aw`$:

$$l_c2\pi \frac{w^2}{4l_P}$$

At first sight, one might be tempted to state that this crossover length is microscopic, but it turns out that $`l_P`$ is of the order of, or smaller than, a Fermi. Indeed, with $`\eta =10^3`$ kg/m.s and $`\lambda _P10^{12}\mathrm{m}^3/\mathrm{N}.\mathrm{s}`$  , we find $`l_P10^{15}`$ m. Then, with $`w510^9`$ m, we find:

$$l_c310^2\mathrm{m}$$

As a result, all active-permeation terms may be omitted in the micron and submicron length scales we are dealing with ($`2\pi /R_{ves}310^5\mathrm{m}^{}1q2\pi /a610^{10}\mathrm{m}^{}1`$, with $`R_{ves}20\mu \mathrm{m}`$ and $`a0.1`$ nm).

The osmotic contribution is negligible as well. To see this, compare $`2\lambda _PkT\dot{a}/D_Pq_{}`$ and $`𝒫_aq_{}w/4\eta `$: this yields the cross over wavevector

$$q_c^{}=\left(\frac{8\lambda _P\eta kT\dot{a}}{𝒫_awD_P}\right)^{1/2}$$

or the cross over length

$$l_c^{}=2\pi \left(\frac{𝒫_awD_P}{8\lambda _P\eta kT\dot{a}}\right)^{1/2}$$

With an effective proton diffusivity $`D_P10^9\mathrm{m}^2/\mathrm{s}`$, a pumping rate $`\dot{a}=10^3\mathrm{s}^1`$, $`𝒫_a\kappa 10kT`$ (see appendix B), and other material parameters as above, one finds $`l_c^{}10^2`$ m: the osmotic contribution is totally negligible as well. In the case of ion channels for which $`\dot{a}=10^7\mathrm{s}^1`$, the cross over length is reduced by a factor hundred, that is to a few tens of microns; this may be accessible to experiment. Similarly, since $`ł_Pq^1`$, terms arising from permeative friction may entirely be omitted in the equations. We have now:

$`\begin{array}{cc}\tau _u^1=\frac{1}{4\eta }(\sigma q_{}+\stackrel{~}{\kappa }q_{}^3)\hfill & \hfill \text{with}\stackrel{~}{\kappa }=\kappa \rho 𝒫_a^{}w\\ \tau _{u}^{e}{}_{}{}^{1}=\frac{1}{4\eta }(\sigma q_{}+\stackrel{~}{\kappa ^e}q_{}^3)\hfill & \hfill \stackrel{~}{\kappa ^e}=\kappa ^e\rho 𝒫_a^{}w\\ \tau _\psi ^1=Dq_{}^2\hfill & \\ \tau _a^1=\frac{\mathrm{\Xi }}{4\chi \eta }𝒫_awq_{}^3\hfill & \end{array}`$

A further simplification can be obtained with the remark that in our experimental conditions $`D(\sigma \kappa )^{1/2}\eta ^1`$ (i.e., more precisely, $`D10^2(\sigma \kappa )^{1/2}\eta ^1`$ with $`D10^{12}\mathrm{m}^2/\mathrm{s}`$ ). This means that one can further ignore the diffusion term in the $`u(𝐪_{},t)u(𝐪_{},t)`$ correlation function. Under such conditions, equation (8) reduces to the expression:

$$u(𝐪_{},t)u(𝐪_{},t)\frac{kT}{\sigma q_{}^2+\stackrel{~}{\stackrel{~}{\kappa ^e}}q_{}^4}+\frac{kT\left[𝒫_a^2w^2\mathrm{\Xi }𝒫_aw\right]}{\chi (\sigma +\stackrel{~}{\kappa }q_{}^2)(\sigma +\stackrel{~}{\stackrel{~}{\kappa ^e}}q_{}^2)}$$
(11)
where $`\stackrel{~}{\stackrel{~}{\kappa ^e}}=\stackrel{~}{\kappa ^e}𝒫_aw\mathrm{\Xi }/\chi `$
From this correlation function, we can calculate the relationship between the areal strain and the membrane tension:

$$\mathrm{\Delta }\alpha =\alpha _0\alpha =\frac{kT}{8\pi }\left(\frac{𝒫_a^2w^2\mathrm{\Xi }𝒫_aw}{\stackrel{~}{\stackrel{~}{\kappa ^e}}\stackrel{~}{\kappa }\chi }+\frac{1}{\stackrel{~}{\stackrel{~}{\kappa ^e}}}\right)\mathrm{ln}\left(\frac{\sigma }{\sigma _0}\right)$$
(12)
or

$$\mathrm{\Delta }\alpha =\alpha _0\alpha =\frac{kT^{eff}}{8\pi \kappa }\mathrm{ln}(\frac{\sigma }{\sigma _0})$$
(13)
with

$$\frac{T^{eff}}{T}=\frac{\kappa }{\stackrel{~}{\stackrel{~}{\kappa ^e}}}\left(1+\frac{𝒫_a^2w^2\mathrm{\Xi }𝒫_aw}{\stackrel{~}{\kappa }\chi }\right)$$
(14)
The functional relation (13) is identical to the one holding in the equilibrium case (except that the ‘temperature’ is an effective nonequilibrium noise level) and is clearly compatible with the experimental results. The whole theory accounts well for the experimental observations if we note in addition the following four results:

* the value of the bending modulus, measured in the passive case, is insensitive to the BR concentration and equal to that of pure phospholipidic membrane,
* the effective temperature is about twice as large as the actual temperature,
* the effective temperature is essentially independent of the BR surface concentration in the investigated domain,
* the reduced effective temperature difference $`(T^{eff}T)/T`$ decreases by a factor 3 when 25 $`\%`$ glycerol is added.

The first observation is easily explained, as detailed in appendix B. In order to discuss the second and third observations one must estimate the different terms entering equation (14). We provide details on these estimates in appendix B. We expect:

$`\begin{array}{c}|𝒫_a|\kappa \\ |\mathrm{\Xi }|wkT\\ |𝒫_a^{}|\kappa w\\ \chi kT/\rho kTl^2\end{array}`$

where $`l`$ is the average distance between BR molecules. We have been able to vary the concentration $`\rho `$ over approximately one order of magnitude, that is roughly $`l`$ from $`w`$ to $`3w`$. With such estimates, and chosing the signs in such a way that the system is stable, we expect:

$$\frac{T^{eff}}{T}\frac{1+\left(\frac{\kappa }{kT}+2\right)\frac{w^2}{l^2}}{\left(1+\frac{w^2}{l^2}\right)\left(1+\left(2\frac{kT}{\kappa }\right)\frac{w^2}{l^2}\right)}$$

with $`0.3w/l1`$ and knowing that $`\kappa 10kT`$, we find:

$$1.7\frac{T^{eff}}{T}2.3$$

which is in very reasonable agreement with experiment. Of course, the numbers chosen above have some degree of arbitrariness, but one can change them appreciably while retaining a ratio $`T^{eff}/T`$ of order 2. For instance, $`\mathrm{\Xi }`$ may be set to zero, keeping other values unchanged, and one finds $`2<T^{eff}/T<2.7`$, which is less satisfactory but not off scale.

Let us now turn to the glycerol dependence. It has been measured that a 25 $`\%`$ glycerol addition to water reduces the pumping activity of the bacteriorhodopsin by a factor $`2.5`$ . It is thus clear that both $`𝒫_a`$ and $`𝒫_a^{}`$ (and perhaps $`\mathrm{\Xi }`$) have to be reduced by a factor $`2.5`$; all other parameters are essentially unchanged, as shown by the experiments performed with red light. The same type of estimate as before give the expected reduction of $`(T^{eff}T)/T`$ by a factor three.

The net conclusion is thus that our analysis provides a satisfactory account of the experiment, although it is not able to pinpoint accurately values for $`\mathrm{\Xi }`$, $`𝒫_a^{}`$ and $`𝒫_a`$. A more accurate experiment should reveal that the effective temperature should depend on BR density in a non trivial way. At low density, the effective temperature should be essentially equal to the actual temperature; it should increase proportionally to the density at moderate densities; eventually, at larger densities, it could even decrease after going through a maximum. Together with an independent measurement of $`\chi `$, it should allow us to measure at least $`𝒫_a`$ and $`𝒫_a^{}`$. Our current accuracy does not allow for such a detailed analysis.

Thus, the proposed analysis gives a natural interpretation of the experimental data. It is one of those intriguing cases in which terms nominally subdominant in wavenumber provide by far the leading contribution. This pecularity is due to the very small value of the permeation coefficient: in the experimentally accessible domain, the membrane is practically impermeable and the effects due directly to the force exerted by the active centers on the membrane are negligible.

## A Osmotic pressure difference

Since BR selectively pumps protons, we just have to consider the osmotic pressure resulting from the three dimensional proton density $`n(𝐫,t)`$:

$$\mathrm{\Pi }=kTn(𝐫,t)$$
(A1)
The protons dynamics is described as usual by conservation equations in each half space, above and below the membrane:

$$\frac{n}{t}(𝐫,t)+𝐉_n=0$$
(A2)
$$𝐉_n=n𝐕D_Pn$$

At the membrane, the coarsegrained proton flux $`𝐉_n\widehat{𝐳}`$ in the membrane normal direction $`\widehat{𝐳}`$, is given by the BR active transport:

$$𝐉_n\widehat{𝐳}=\psi (𝐫,t)\dot{a}$$

where $`\dot{a}`$ is the pumping rate, and $`\psi (𝐫,t)`$ is defined in the main text. For a macroscopically symmetric membrane, $`\psi `$, $`n`$ and $`𝐕`$ are ‘small’ fluctuating quantities. So the convective term can be omitted, as a second order correction. Now to the linear order, equation (A2) becomes in ‘hybrid’ Fourier space (with obvious notations):

$$\begin{array}{c}i\omega n(z,𝐪_{},\omega )+D_Pq_{}^2n(z,𝐪_{},\omega )D_P\frac{^2}{z^2}n(z,𝐪_{},\omega )=0\\ D_P\frac{n}{z}(z=0^+,𝐪_{},\omega )=D_P\frac{n}{z}(z=0^{},𝐪_{},\omega )=\psi (𝐪_{},\omega )\dot{a}\end{array}$$
(A3)
The solution to this problem is straightforward. One finds:

$$n(z=0^+,𝐪_{},\omega )n(z=0^{},𝐪_{},\omega )=\frac{2\psi (𝐪_{},\omega )\dot{a}}{D_P(i\frac{\omega }{D_P}+q_{}^2)^{1/2}}$$

so that

$$\delta \mathrm{\Pi }(𝐪_{},\omega )=\frac{2kT\psi (𝐪_{},\omega )\dot{a}}{D_P(\frac{i\omega }{D_P}+q_{}^2)^{1/2}}$$
(A4)
The typical frequency over which $`\psi (𝐪_{},\omega )`$ varies is $`Dq_{}^2`$. Eventhough $`D_P`$ is an effective diffusion coefficient renormalized by the time the proton spends attached to the hydrazoic acid resulting from the conversion of sodium azide in solution , one always has $`D_PD`$, and thus the term $`\omega /D_P`$ may be safely omitted in equation (A4). Then, one can equivalently write:

$$\delta \mathrm{\Pi }(𝐪_{},\omega )\frac{2kT\psi (𝐪_{},\omega )\dot{a}}{D_Pq_{}}$$
(A5)
## B Orders of magnitude of the theoretical parameters

The long wavelength effective membrane curvature modulus $`\kappa ^e`$, is as shown in section III:

$$\kappa ^e=\kappa \frac{\mathrm{\Xi }^2}{\chi }$$
(B1)
It is easy to convince oneself that the coupling term $`\mathrm{\Xi }`$ in fact depends on the pumping activity. Let us first consider the passive case, and call the corresponding coeffiecient $`\mathrm{\Xi }_p`$. A BR molecule with a given orientation may ’prefer’ a given curvature sign for several different reasons. The first and most obvious one is linked to a putative wedge shape. In such a case, one expects:

$$\mathrm{\Xi }_p\kappa R\theta $$

in which $`R`$ is the ’radius’ of the BR molecule and $`\theta `$ the wedge angle. The experiments performed with red light tell us:

$$\frac{\mathrm{\Xi }_p^2}{\chi }\kappa $$

That is:

$$\theta ^2\frac{kT}{\kappa }\left(\frac{l}{R}\right)^2$$

At the highest densities $`lwR`$, so with $`\kappa =10kT`$ the experiment requires $`\theta 1/3`$, which is obviously a ‘weak’ requirement: the absence of up-down symmetry in BR requires the existence of a wedge, but inspection of the molecular structure suggests that it is very small (for instance, it is very hard to coin a sign to it). So, the ‘steric’ contribution to $`\mathrm{\Xi }_p`$ can be safely neglected.

There can however, be other contributions and the next most obvious one results from flexoelectricity: a curved membrane generates an electric polarisation, hence a transmembrane electric field. Again, the absence of up-down symmetry in BR tells us that it must have a non zero electric dipole. The energy of the dipole in this transmembrane field, provides the coupling between curvature and $`\psi `$. With the usual definitions, the transmembrane electric field can be written:

$$E=\frac{e}{ϵw}\mathrm{\Delta }_{}u$$
(B2)
in which $`ϵ`$ is the dielectric permittivity of the hydrophobic layer and $`e`$ is the flexoelectric coefficient discussed by Petrov for instance . If we call $`p`$ the BR average longitudinal dipole, one has:

$$\mathrm{\Xi }_p^f=\frac{ep}{ϵw}$$

The flexoelectric coefficient $`e`$ is a measured quantity :

$$|e|1.310^{20}\mathrm{C}$$

Estimating $`p\text{a few}q\delta `$, in which $`q`$ is a unit charge and $`\delta `$ a distance of the order of a fraction of the membrane thickness, e.g. the hydrophilic part (note that it cannot be much larger otherwise the BR would not be membrane soluble), and taking the dielectric permittivity of the hydrophobic layer of the order of $`ϵ3ϵ_0`$, with the dielectric permittivity of vacuum $`ϵ_08.810^{12}\mathrm{F}.\mathrm{m}^1`$, we find:

$$\frac{\mathrm{\Xi }_p^{f\mathrm{\hspace{0.17em}2}}}{\kappa \chi }<10^2$$

So in this case as well, one does find $`\kappa ^{eff}\kappa `$.

When the BR undergoes its pumping activity, the flexoelectric energy is dominated by the time average energy of the proton in the flexoelectric potential $`e\mathrm{\Delta }_{}u/ϵ`$; assuming a duty ratio of one tenth, we expect then:

$$\mathrm{\Xi }_a^f\frac{qe}{10ϵ}\frac{1}{100ϵ}q^2wkT$$

The force dipole $`𝒫_a`$ has the dimensions of an energy, and hence must be a fraction of the green-yellow photon energy. As a rough rule of thumb, we take again a duty ratio of a tenth:

$$𝒫_a\frac{h\nu }{10}\kappa $$

The curvature dependence of the force dipole can be estimated in a way similar to that used for $`\mathrm{\Xi }`$. During its pumping cycle, the BR/proton system has probably to overcome a potential barrier $`W_b`$. The pumping rate is then controled by a Boltzmann factor $`\mathrm{exp}(W_b/kT)`$. In the presence of curvature, the barrier is modified by the energy of the proton in the flexoelectric potential at the barrier location. We call $`xW_b`$ this location. Thus, the activity is multiplied by a factor $`\mathrm{exp}\left[x(eq\mathrm{\Delta }_{}u)/(ϵkT)\right]`$ which can be linearized for small curvatures. Hence, we expect (with $`x`$ of the order of a few tenths):

$$𝒫_a^{}𝒫_ax\frac{eq}{ϵkT}\text{a few}w\kappa $$

Note that one could in principle estimate this coefficient by measuring the pumping activity in liposomes, as a function of liposome radius: the net result would strongly depend on the value of $`x`$. For $`x`$ a few tenths, one would need % accuracy to measure the curvature dependence. For $`x1`$, the effects would be much larger and the exponential nature of the relation should start to show up. However, even if the direct effect is not easily measurable, the incidence on formula (14) can be important.


text:
# References

Non-resonant microwave absorption studies of superconducting MgB2

Janhavi P. Joshi, Subhasis Sarangi, A. K. Sood and S. V. Bhat
Department of Physics, Indian Institute of Science, Bangalore-560012, India
and
Dilip Pal
Tata Institute of Fundamental Research, Mumbai, 400005, India

Non-resonant microwave absorption(NRMA) studies of superconducting MgB2 at a frequency of 9.43 GHz in the field range -50 Gauss to 5000 Gauss are reported. The NRMA results indicate near absence of intergranular weak links. A linear temperature dependence of the lower critical field H$`{}_{c}{}^{}1`$ is observed indicating a non s-wave superconductivity. However, the phase reversal of the NRMA signal which could suggest d-wave symmetry is also not observed.

The newly discovered  intermetallic compound superconductor MgB2 has given rise to a flurry of scientific activity as well as its own share of controversies. While the observation of boron isotope effect in MgB2 indicated it to be a phonon mediated BCS superconductor, the temperature dependence of the lower critical field Hc1 was found to be linear expected for a d-wave symmetry of the order parameter. Another pleasant surprise has been the reported absence of weaklink structure between intergranular contacts in the polycrystalline samples, leading to high critical current density (Jc) even in the presence of a magnetic field. This result, which is in quite a contrast to the high Tc superconductors(HTSC), that abound in intergranular weak links, makes MgB2 a very good potential candidate for practical applications.

The technique of non-resonant microwave absorption (NRMA) has proven to be a valuable tool in detecting and characterising superconductivity in the case of HTSC. In this technique, the sample is studied using a continuous wave Electron Paramagneic Resonance (EPR) spectrometer, by recording the magnetic field dependence of the power absorption. In standard EPR spectrometers, the magnetic field is usually modulated at 100 kHz and phase sensitive detection is used to record the field derivative dP/dH of the power absorbed. In the case of HTSC two processes mainly contribute to this field dependent dissipation. One, the decoupling of the Josephson junctions (JJs) due to the magnetic field and the other the Lorentz force driven motion of the quantised flux lines, the so called fluxons. In all but the extremely well prepared thin film and single crystalline HTSC samples the former contribution dominates, especially at low fields making dP/dH vs H look like a regular EPR signal except for the reversal of the phase. The latter is a consequence of the loss in the mixed state of the superconductors being an increasing function of the field with a minimum at zero field. It turns out that the two contributions can be easily distinguished from each other from the characteristic field dependences, reflected in the line shapes. Thus, the decoupling of the JJs leads to a narrow derivative looking signal centred around zero field while the fluxon motion results in a quasi-linear dependence on field and therefore the dP/dH appears to have near field independence. In this report, we examine superconducting MgB2 samples with a view to charactarise them using the technique of NRMA.

The sample of MgB2 used was obtained from M/s Alpha Aesar of John Matthey GmBH, Germany and was used without further processing except for pelletising under a pressure of 2 tons. AC susceptibility measurements indicated a Tc of 39K. The NRMA signals were recorded using a Bruker 200D X band (microwave frequency: 9.43 GHz) EPR spectrometer equipped with an Oxford Instruments ESR 900 continuous flow cryostat, in the temperature range 4 K to room temperature. A typical modulation amplitude of 4 Gauss peak to peak and a microwave power of 20 mW were used. The sample was zero field cooled to 4 K and the signals were recorded between -50 and 5000 Gauss for both forward and reverse scans of the field during both cooling and warming of the sample.

Fig. 1 shows typical NRMA signals recorded at a few representative temperatures recorded in the warming run. The signals recorded while cooling (not shown)are essentially similar. In the normal state only a very weak EPR signal due to some impurity in the cavity is observed. Below Tc ($``$ 39 K) the NRMA signal appears centred at zero field which on cooling increases both in intensity and extent in the field. By 34 K it is seen to have extended beyond the limits of our magnetic field (0.5 Tesla). At zero field, a sudden rise in the signal (note its opposite phase to that of the EPR signal as expected for a normal NRMA signal) is observed and at a temperature dependent higher field there is a change in the slope of the signal. The point at which the slope change is observed (as marked by the arrows on a few signals) can be associated with the lower critical field. We denote this field by H$`{}_{c1}{}^{}{}_{}{}^{}`$ to indicate that it is uncorrected for demagnetisation factor and geometric and/or surface barriers. Figure 2 shows the temperature dependence of H$`{}_{c1}{}^{}{}_{}{}^{}`$. It is seen that the temperature dependence is approximately linear, attributed to a non s-wave superconductor. Such linear dependences have also been observed by other workers. The opposite scans of the magnetic field bring out the rectangular nature of the hysteresis loops similar to the ones observed in single crystal HTSC at low temperatures indicative of the large critical current densities.

The crucial difference between these NRMA signals and those observed in polycrystalline samples of HTSC is the near absence of narrow derivative looking signal observed in the latter at low fields commonly attributed to JJs. This might indicate the absence of intergranular weak links. However, the presence of a significant field dependent dissipation below Hc1 (indicated by ellipses in fig. 1) obtained in MgB2 needs to be explained. While quasi-particle excitation is a possible candidate, we believe the temperature and field dependences of the observed signals, do not favor this mechanism. NRMA technique being very sensitive to the JJs, can pick up even minute contributions from them. Therefore, we attribute the signal which is observed below Hc1 to the presence of a few weak JJs in the sample. The temperature dependence of the signal below Hc1 also supports this possibility.

Another interesting feature of the NRMA signals is the absence of phase reversal of the signal as a function of temperature. Such a phase reversal has been observed in almost all HTSC materials  especially in their granular form; one of the causes is understood to be the paramagnetic Meissner effect(PME) arising due to d-wave symmetry of the order parameter and/or the presence of $`\pi `$ junctions . However, inspite of varying microwave power and modulation amplitude, we were unable to observe any such phase reversal in the NRMA signals from MgB2. It appears therefore, that the linear temperature dependence of H$`{}_{c}{}^{}1`$ and the absencce of the phase reversal in NRMA signals need to be examined and understood further with regard to their implications for the symmetry of the order parameter.

In conclusion, we have studied the novel superconductor MgB2 using the technique of NRMA. The NRMA signals from MgB2 are very different from that of HTSC. Low field derivative like narrow signals characteristic of the Josephson junctions is absent while the rectangular hysteresis loops indicative of large critical current densities are observed. The lower critical field is observed to decrease linearly with temperature. The absence of phase reversal of the NRMA signal is noted as another unique feature of this superconductor, especially because such a phase reversal can point towards the d-wave symmetry of the order parameter through PME.

Acknowledgments
The authors acknowledge Professors Arun Grover and S. Ramakrishnan of TIFR, Bombay for providing the samples. JJ would like to thank CSIR, India, AKS and SVB acknowledge DST and UGC, India for financial support.

Figure Captions

Figure 1
The typical NRMA signals recorded during the warming of the sample at a few representative temperatures for both forward and reverse scans of the magnetic field. The dotted ellipse indicates the part of the signal tentatively attributed to a very small number of weak links forming JJs in the sample. The vertical arrows mark the field at which the slope changes indicating the onset of the entry of the magnetic field in the form of vortices in the sample.

Figure 2
The H$`{}_{c1}{}^{}{}_{}{}^{}`$ obtained from the slope change in the NRMA signals and uncorrected for demagnetisation factors geometrical and/or surface barrier effects, plotted as a function of reduced temperature (T/Tc), showing quasi-linear behaviour.