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# 𝐵⁰_𝑠 Oscillation Results

## 1 INTRODUCTION

Studies of the time dependence of $`B_d^0\text{}\overline{B_d^0}`$ and $`B_s^0\text{}\overline{B_s^0}`$ mixing continue to play an important role in the exploration of both the Cabibbo-Kobayashi-Maskawa (CKM) quark mixing matrix and the phenomenon of CP violation. The $`B_d^0`$ oscillation frequency is related to the poorly known CKM element $`V_{td}`$ according to

$`\mathrm{\Delta }m_d`$ $`=`$ $`{\displaystyle \frac{G_F^2}{6\pi ^2}}m_{B_d}m_t^2F(m_t^2/m_W^2)f_{B_d}^2B_{B_d}`$ (1)
$`\times \eta _{QCD}\left|V_{tb}^{}V_{td}\right|^2`$
and has recently been precisely measured by the BaBar and Belle collaborations—the current world average is $`\mathrm{\Delta }m_d=0.503\pm 0.006`$ $`\text{ps}^1`$ . However, this measurement cannot be translated into a precise determination of $`|V_{td}|`$ due the 15-20% theoretical uncertainty in $`f_{B_d}\sqrt{B_{B_d}}`$ (see Ref.  for a review of Lattice QCD calculations). Uncertainties are reduced for the ratio

$$\frac{\mathrm{\Delta }m_s}{\mathrm{\Delta }m_d}=\frac{m_{B_s}}{m_{B_d}}\xi ^2\left|\frac{V_{ts}}{V_{td}}\right|^2,$$
(2)
where the quantity $`\xi (f_{B_s}\sqrt{B_{B_s}})/(f_{B_d}\sqrt{B_{B_d}})`$ is estimated to be $`1.18\pm 0.04_{0.00}^{+0.12}`$ from Lattice QCD . This implies that the ratio $`|V_{ts}/V_{td}|`$ can be determined with an uncertainty smaller than that for $`|V_{td}|`$ . In the Wolfenstein parameterization of the CKM matrix, we have $`\mathrm{\Delta }m_d|V_{td}|^2A^2\lambda ^6[(1\rho )^2+\eta ^2]`$ and $`\mathrm{\Delta }m_s|V_{ts}|^2A^2\lambda ^4`$, where $`\lambda =0.2237\pm 0.0033`$ and $`A=0.819\pm 0.040`$ , but $`\rho `$ and $`\eta `$ are not well known. Studies of $`B_d^0`$ and $`B_s^0`$ oscillations thus provide some of the strongest constraints on the CKM unitarity triangle parameters $`\rho `$ and $`\eta `$.

Experimental studies of $`B_s^0`$ oscillations require two main ingredients: (i) reconstruction of the $`B_s^0`$ decay and its proper time, (ii) determination of the $`B_s^0`$ or $`\overline{B_s^0}`$ flavor at both production and decay to classify the decay as either ‘mixed’ (if the tags disagree) or ‘unmixed’ (otherwise). The significance for a $`B_s^0`$ oscillation signal can be approximated by

$$S=\sqrt{\frac{N}{2}}f_s\left[12w\right]e^{\frac{1}{2}(\mathrm{\Delta }m_s\sigma _t)^2},$$
(3)
where $`N`$ is the total number of decays selected, $`f_s`$ is the fraction of $`B_s^0`$ mesons in the selected sample, $`w`$ is the probability to incorrectly tag a decay as mixed or unmixed (i.e. the mistag rate) and $`\sigma _t`$ is the proper time resolution. The proper time resolution depends on both the decay length resolution $`\sigma _L`$ and the momentum resolution $`\sigma _p`$ according to $`\sigma _t^2=(\sigma _Lm_B/p)^2+(t\sigma _p/p)^2`$. Based on the Wolfenstein parameterization, we see that $`\mathrm{\Delta }m_s/\mathrm{\Delta }m_d1/\lambda ^2`$, which is of order of 20 (the other Wolfenstein parameters are of order 1). Therefore, $`B_s^0`$ oscillations are expected to be much more rapid than $`B_d^0`$ oscillations. The ability to resolve such rapid oscillations thus requires excellent decay length and momentum resolution, and benefits from having a low mistag rate and a high $`B_s^0`$ purity.

## 2 RECONSTRUCTION METHODS

The study of the time dependence of $`B_s^0\text{}\overline{B_s^0}`$ mixing has been performed with different analysis techniques, ranging from fully inclusive to fully exclusive reconstruction of $`B_s^0`$ decay candidates. The study of $`B_s^0`$ oscillations is more chalenging than that of $`B_d^0`$ oscillations due to two main differences. First, only about 10% of $`b`$ quarks fragment into $`B_s^0`$ mesons, as compared to about 40% into $`B_d^0`$ mesons. Second, the $`B_s^0`$ oscillation frequency is expected to be at least a factor of 20 larger than that for $`B_d^0`$ oscillations. To address this, sophisticated analyses have been developed with an emphasis on lowering the mistag rate, increasing the $`B_s^0`$ purity and, especially, improving the proper time resolution, all of which affect the sensitivity to $`B_s^0`$ oscillations.

The production flavor tag combines a number of different individual tags. The single most powerful tag exploits the large polarized forward-backward asymmetry in $`Z^0b\overline{b}`$ decays. This tag is available at SLD thanks to the large electron beam polarization ($`P_e=73\%`$). A left- (right-) handed incident electron tags the quark produced in the forward hemisphere as a $`b`$ ($`\overline{b}`$) quark. This method yields a mistag rate of $`28\%`$ with nearly 100% efficiency. Tags used in all analyses rely on charge information from the event hemisphere opposite that of the $`B_s^0`$ candidate: (i) charge of lepton from the direct transition $`b\mathrm{}^{}`$, (ii) momentum-weighted jet charge, (iii) secondary vertex charge, (iv) charge of secondary vertex kaon from the dominant transition $`bcs`$, (v) charge dipole of secondary vertex (SLD only). Other tags from the same hemisphere as the $`B_s^0`$ candidate are also used: (i) unweighted (or weighted) jet charge, and (ii) charge of fragmentation kaon accompanying the $`B_s^0`$ meson. These various tags are combined on an event-by-event basis to yield an average mistag rate of approximately 22% at SLD and 27-29% at LEP.

The analyses differ in the way the $`B_s^0`$ decay is reconstructed and thus in the way the decay flavor is determined. Three general classes can be identified: inclusive, semi-exclusive and fully exclusive. Inclusive analyses benefit from the large available statistics but suffer from low $`B_s^0`$ purity, whereas more exclusive analyses benefit from higher purity and resolution but suffer from the lack of statistics (this is particularly true for the fully exclusive analyses). Several analyses are discussed below to highlight these differences.

Inclusive analyses have been performed by ALEPH, DELPHI, OPAL and SLD. The SLD charge dipole analysis is the most sensitive fully inclusive method . It aims to reconstruct the $`b`$-hadron decay chain topology. This method takes full advantage of the superb decay length resolution of the SLD CCD pixel vertex detector to separate secondary tracks (from the $`B`$ decay point) from tertiary tracks (from the $`D`$ decay point). The decay length resolution is parameterized by the sum of two Gaussians with $`\sigma _L=78\mu `$m (60% fraction) and $`304\mu `$m (40%), whereas the momentum resolution is parameterized with $`\sigma _p/p=0.07`$ (60%) and 0.21 (40%). A “charge dipole” $`\delta Q`$ is defined as the distance between secondary and tertiary vertices signed by the charge difference between them such that $`\delta Q>0`$ ($`\delta Q<0`$) tags $`\overline{B^0}`$ ($`B^0`$) decays. The average decay flavor mistag rate is estimated to be 22% and is mostly due to decays producing two charmed hadrons. A sample of 11,462 decays is selected with a $`B_s^0`$ purity estimated to be 16% (higher than the production rate of 10% due to the fact that only neutral decays are selected).

The most sensitive of all analyses is the ALEPH inclusive lepton analysis , which selects semileptonic $`B`$ decays. In this analysis, a $`D`$ meson is reconstructed inclusively based on topological and kinematical properties of the decay, and a resultant $`D`$ track is vertexed with the lepton and the $`b`$-hadron direction (from the jet direction) to form a $`B`$ decay vertex. The average decay length and momentum resolutions are $`\sigma _L=251\mu `$m (75% fraction) and $`718\mu `$m (25%), $`\sigma _p/p=0.064`$ (60%) and 0.20 (40%). Fairly loose selection criteria are used at the various stages of the analysis to obtain a high statistics sample of 74,026 events. The analysis relies on several neural network algorithms to perform the following tasks: production flavor tagging, $`b\overline{b}`$ event selection, direct $`(b\mathrm{})`$ lepton selection, and $`B_s^0`$ fraction enhancement. To maximize sensitivity to $`B_s^0`$ oscillations, the analysis incorporates all the information event by event, including estimates of the decay length and momentum resolution.

Semi-exclusive analyses have been performed by ALEPH, CDF, DELPHI, OPAL and SLD. $`B_s^0`$ decays are partially reconstructed in the modes $`B_s^0D_s^{}\mathrm{}^+\nu _{\mathrm{}}X`$ and $`B_s^0D_s^{}h^+X`$, where $`h`$ represents any charged hadron (or system of several hadrons) and the $`D_s^{}`$ meson decay is either fully or partially reconstructed in the modes $`D_s^{}\varphi \pi ^{}`$, $`K^0K^{}`$, $`K^0K^{}`$, $`\varphi \pi ^{}\pi ^+\pi ^{}`$, $`\varphi \mathrm{}^{}\overline{\nu _{\mathrm{}}}`$, etc.

The most sensitive semi-exclusive analysis performed by DELPHI selects 436 $`D_s^{}\mathrm{}^+`$ events . The small statistics is compensated by the high $`B_s^0D_s^{}\mathrm{}^+\nu _{\mathrm{}}`$ purity, estimated to be $`53\%`$, and the good decay length and momentum resolution, $`\sigma _L=200\mu `$m (82% fraction) and $`670\mu `$m (16%), $`\sigma _p/p=0.07`$ (82%) and 0.16 (16%). Analyses selecting $`D_s^{}h^+`$ final states benefit from higher statistics but are less sensitive than those selecting $`D_s^{}\mathrm{}^+`$ states because of lower $`B_s^0`$ purity and worse proper time resolution. The SLD $`D_s`$+Tracks analysis  combines fully reconstructed $`D_s`$ mesons with either a lepton or one (or more) charged hadron(s). It contributes especially at large values of $`\mathrm{\Delta }m_s`$ thanks to a $`B_s^0`$ purity of 40% and the best available decay length resolution: $`\sigma _L=50\mu `$m (60% fraction) and $`151\mu `$m (40%).

Finally, fully exclusive analyses have been performed by ALEPH  and DELPHI  via the (all charged particles) modes $`B_s^0D_s^{}\pi ^+`$, $`D_s^{}a_1^+`$, $`\overline{D^0}K^{}\pi ^+`$, and $`\overline{D^0}K^{}a_1^+`$ (last two for DELPHI only), where the $`D_s^{}`$ and $`\overline{D^0}`$ are fully reconstructed. The decays $`B_s^0D_s^{}\pi ^+`$, $`D_s^{}a_1^+`$ and $`D_s^{()}\rho ^+`$ are also reconstructed by adding one or more photons to the above final states (ALEPH only) or by including the “satellite” mass region below the $`B_s^0`$ mass peak. The number of decay candidates is 80 for ALEPH and 44 for DELPHI with signal purities of approximately 36% and 50%, respectively. The main advantage of the exclusive method is its excellent proper time resolution with a negligible contribution from momentum resolution ($`0.5\%`$). As a result, unlike all other methods, $`\sigma _t`$ does not grow significantly with increasing proper time $`t`$ and thus the oscillation amplitude is not damped as $`t`$ increases. Due to limited statistics, this method is not competitive with respect to the inclusive and semi-exclusive methods. However, this is the method of choice for future studies of $`B_s^0`$ oscillations at hadron colliders.

## 3 RESULTS

Studies of the time dependence of $`B_s^0\text{}\overline{B_s^0}`$ mixing are carried out with the amplitude method, which is equivalent to a normalized Fourier transform . The oscillation amplitude $`A`$ is expected to be $`A=0`$ ($`A=1`$) for frequencies sufficiently far from (close to) the true oscillation frequency. All available measurements of the oscillation amplitude at $`\mathrm{\Delta }m_s=15\text{ps}^1`$ are summarized in Figure 1. Also shown are the sensitivities for each analysis to set a 95% C.L. lower limit on $`\mathrm{\Delta }m_s`$ ($`\mathrm{\Delta }m_s`$ value at which $`1.645\sigma _A=1`$).

The measured oscillation amplitudes are combined , taking statistical and systematic correlations into account, to obtain the world average amplitude spectrum shown in Figure 2. The combination also corrects for the different input parameters used ($`\mathrm{\Delta }m_d`$, $`b`$-hadron lifetimes and production rates). Furthermore, the amplitude statistical uncertainties measured by the inclusive analyses are adjusted to take into account the $`B_s^0`$ production rate of $`(9.3\pm 1.1)\%`$. The rise in statistical error as $`\mathrm{\Delta }m_s`$ increases comes from the fact that an increasingly smaller fraction of the data sample has sufficient proper time resolution to resolve more rapid oscillations; the better the resolution, the smaller the rise. The preliminary combined amplitude spectrum excludes mixing $`(A=1)`$ for $`\mathrm{\Delta }m_s<14.4`$ $`\text{ps}^1`$ at the 95% C.L., whereas the sensitivity is 19.2 $`\text{ps}^1`$. The significance of the deviation from $`A=0`$ near $`\mathrm{\Delta }m_s=17.5\text{ps}^1`$ is $`2.3\sigma `$.

It is interesting to note that, while the sensitivity has been increasing steadily over the past 8 years, the limit has remained near 15 $`\text{ps}^1`$ for the past 3 years. In August 1999, the limit was $`\mathrm{\Delta }m_s>14.3`$ $`\text{ps}^1`$ but the sensitivity was only 14.7 $`\text{ps}^1`$.

Many of the LEP and SLD analyses have been or are being finalized. One will thus have to wait for the next generation of experiments to measure the $`B_s^0`$ oscillation frequency. Prospects for such a measurement during Run 2 of the Fermilab Tevatron are excellent.

I wish to thank D.Abbaneo, P.Kluit, F.Parodi, O.Schneider, and A.Stocchi for their help with the preparation of the talk.


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# Untitled Document

Local-Ether Wave Equation of Electric Field

and Interferometry Experiments with Moving Medium and Path

Ching-Chuan Su

Department of Electrical Engineering

National Tsinghua University

Hsinchu, Taiwan

Abstract – Recently, we have presented the local-ether model, whereby the propagation of earthbound waves is supposed to be referred uniquely to a geostationary inertial frame. Further, in order to comply with this propagation model, the modified Lorentz force law is developed. Thereby, the corresponding wave equations of potentials and fields are derived in this investigation. It is shown that the local-ether wave equation of electric field can account for various precision interferometry experiments in a consistent way, including the one-way-link experiment with a geostationary fiber, the Sagnac rotating-loop experiment with a comoving or a geostationary dielectric medium, and Fizeau’s experiment with a moving dielectric medium in a geostationary interferometer. These experiments together then provide a support for the local-ether wave equation. Meanwhile, some other phenomena are predicted, which provide a means to test its validity.

1. Introduction

Recently, we have presented the local-ether model of wave propagation whereby electromagnetic wave is supposed to propagate via a medium like the ether . However, the ether is not universal. Specifically, it is proposed that in the region under sufficient influence of the gravity due to the Earth, the Sun, or another celestial body, there forms a local ether which in turn moves with the gravitational potential of the respective body. Thereby, each local ether together with the gravitational potential moves with the associated celestial body. Thus, as well as earth’s gravitational potential, the earth local ether for earthbound propagation is stationary in an ECI (earth-centered inertial) frame. Consequently, earthbound wave phenomena can depend on earth’s rotation but are entirely independent of earth’s orbital motion around the Sun or whatever. Meanwhile, the sun local ether for interplanetary propagation is stationary in a heliocentric inertial frame. This local-ether model has been adopted to account for the effects of earth’s motions in a wide variety of propagation phenomena, particularly the Sagnac correction in GPS (global positioning system), the Sagnac effect in rotating-loop interferometers, the time comparison via intercontinental microwave link, and the echo time in interplanetary radar. As examined within the present accuracy, the local-ether model is still in accord with the Michelson-Morley experiment which is known to make the classical ether notion obsolete. Moreover, by modifying the speed of light in a gravitational potential, this simple propagation model leads to the deflection of light by the Sun and the increment of echo time in the interplanetary radar which are important phenomena supporting the general theory of relativity .

Further, it is noticed that the electric current generating the magnetic field is commonly electrically neutralized. That is, the mobile charged particles which form the current are actually drifting in a matrix and the ions which constitute the matrix tend to electrically neutralize the mobile particles, such as electrons in a metal wire. Thus the velocity which determines the current density is the drift velocity of the mobile particles with respect to the neutralizing matrix. Consequently, the neutralized current density remains unchanged when observed in different reference frames. In order to comply with the local-ether propagation model and the frame-independence of the current density, we have developed an electromagnetic force law which complies with Galilean transformations while it can reduce to a familiar form under some common condition . In this new classical theory all of the involved position vectors, time derivatives, and velocities are referred specifically to their respective reference frames. Owing to this simple feature, the associated potentials and electromagnetic force remain unchanged when observed in different frames. Under the common low-speed condition where the source particles forming the current drift very slowly with respect to the neutralizing matrix, this force law reduces to a form similar to the Lorentz force law. However, the fundamental modification is that the current density generating the magnetic field, the time derivative applied to the magnetic vector potential in the electric induction force, and the particle velocity connecting to the magnetic field in the magnetic force are all referred specifically to the matrix frame in which the matrix is stationary. The modified equation is identical to the Lorentz force law, if the latter is observed in the matrix frame as done tacitly in common practice.

The propagation of the electromagnetic potentials is supposed to follow the local-ether model. Accordingly, the wave equations of potentials are derived in this investigation. Further, based on the modified Lorentz force law and the associated definitions of electric and magnetic fields in terms of the potentials, the local-ether wave equations of fields are derived. Thereby, the phase speed and propagation constant of the electromagnetic wave propagating in a moving medium are explored. Then, after the Sagnac effect due to the movement of the propagation path is taken into consideration, we present consistent reinterpretations for some precision interferometry experiments, including the fiber-link experiment with a geostationary setup and a geostationary optical fiber, the Sagnac rotating-loop experiments with a comoving or a geostationary dielectric medium, and Fizeau’s experiment with a geostationary interferometer and a moving dielectric medium.

2. Modified Lorentz Force Law

Based on Galilean transformations, we have presented an electromagnetic force law expressed in terms of the augmented scalar potential, which is the electric scalar potential enhanced slightly with a term associated with the difference between the velocities of the effector and the source particles . Consider the electromagnetic force exerted on an effector particle of charge $`q`$ due to an ensemble of source particles of charge density $`\rho _v`$ drifting in a matrix of charge density $`\rho _m`$. The drift velocity of the mobile source particles with respect to the matrix is given by the difference $`𝐯_{sm}=𝐯_s𝐯_m`$, where $`𝐯_s`$ and $`𝐯_m`$ are the velocities of the source particles and the matrix, respectively, both with respect to a particular frame. The matrix can be a metal wire, a dielectric medium, or a magnet and tends to electrically neutralize the mobile source particles to some extent.

Under the common low-speed condition where the speeds of the involved particles are low and the source particles drift very slowly with respect to the matrix, the electromagnetic force law proposed in terms of the augmented potentials has been shown to reduce to the modified Lorentz force law

$$𝐅(𝐫,t)=q\left\{𝐄(𝐫,t)+𝐯_{em}\times 𝐁(𝐫,t)\right\},$$
$`(1)`$
where the velocity difference $`𝐯_{em}`$ ($`=𝐯_e𝐯_m`$) is the velocity of the effector particle with respect to the matrix and $`𝐯_e`$ is the effector velocity with respect to the aforementioned particular frame. The electric and magnetic fields in turn are defined explicitly in terms of the potentials $`\mathrm{\Phi }`$ and $`𝐀`$ as

$$𝐄(𝐫,t)=\mathrm{\Phi }(𝐫,t)\left(\frac{}{t}𝐀(𝐫,t)\right)_m$$
$`(2)`$
and

$$𝐁(𝐫,t)=\times 𝐀(𝐫,t),$$
$`(3)`$
where the time derivative $`(/t)_m`$ is referred specifically to the matrix frame. Quantitatively, the electric scalar potential $`\mathrm{\Phi }`$ and the magnetic vector potential $`𝐀`$ are defined explicitly as

$$\mathrm{\Phi }(𝐫,t)=\frac{1}{ϵ_0}\frac{\rho _n(𝐫^{},tR/c)}{4\pi R}𝑑v^{}$$
$`(4)`$
and

$$𝐀(𝐫,t)=\frac{1}{ϵ_0c^2}\frac{𝐉_n(𝐫^{},tR/c)}{4\pi R}𝑑v^{},$$
$`(5)`$
where the net charge density $`\rho _n=\rho _v+\rho _m`$, the neutralized current density $`𝐉_n=𝐯_{sm}\rho _v`$, the propagation range $`R=|𝐫𝐫^{}|`$, and the position vectors $`𝐫`$ and $`𝐫^{}`$ are referred to a particular frame.

Obviously, the values of the neutralized current density and the potentials remain unchanged when observed in different frames. Moreover, since the time derivative in the definition of field $`𝐄`$ and the effector velocity in the force law are referred uniquely to the matrix frame, the values of fields $`𝐄`$ and $`𝐁`$ and hence the electromagnetic force exerted on a charged particle given in the preceding formulas also remain unchanged in different frames. That is, based on Galilean transformations, the values of potentials, fields, and electromagnetic force are independent of reference frame. Further, it is noted that the drift velocity $`𝐯_{sm}`$ involved in the neutralized current density is a Newtonian relative velocity and hence this current density complies with Galilean relativity. For quasi-static case where the propagation time $`R/c`$ in the potentials can be neglected, the potentials $`\mathrm{\Phi }`$ and $`𝐀`$ then comply also with Galilean relativity and comove with the matrix.

It is seen that the force law (1) looks like the Lorentz force law. However, the fundamental modification is that the current density generating the magnetic vector potential, the time derivative applied to this potential in the electric induction force, and the particle velocity connecting to the curl of this potential in the magnetic force are all referred specifically to the matrix frame. Meanwhile, in applying the Lorentz force law to the analysis of, say, a motor or the magnetic deflection, the adopted reference frame is usually the one with respect to which the magnetic field and the magnet are stationary. Thus the matrix frame has been adopted tacitly as the reference frame. Therefore, the modified equation is identical to the Lorentz force law, if the latter is observed in the matrix frame as done tacitly in common practice.

3. Local-Ether Wave Equations of Potentials and Fields

Based on the local-ether model of wave propagation and the electromagnetic force in terms of the potentials, it is supposed here that each individual source particle continuously excites the electric scalar potential and hence other local-ether potentials. These potentials in turn propagate radially outward from the source position at an isotropic speed $`c`$ with respect to the associated local-ether frame, independent of the motions of source and effector. That is, the position vectors $`𝐫`$ and $`𝐫^{}`$ and hence the propagation range $`R`$ in the potentials $`\mathrm{\Phi }`$ and $`𝐀`$ defined in (4) and (5) are referred specifically to the local-ether frame and the ratio $`R/c`$ represents the propagation time from the source point $`𝐫^{}`$ at the instant $`t^{}`$ ($`=tR/c`$) of wave emission to the field point $`𝐫`$ at the instant $`t`$. To comply with the frame of the position vectors, the velocities $`𝐯_e`$, $`𝐯_s`$, and $`𝐯_m`$ are also referred to the local-ether frame.

By applying the Laplacian operator to both sides of the integral formulas for potentials (4) and (5) and then expanding the Laplacians of the time-dependent charge and current densities divided by $`R`$ , it can be shown that the wave equations of these local-ether potentials are given by

$$^2\mathrm{\Phi }(𝐫,t)\frac{1}{c^2}\frac{^2}{t^2}\mathrm{\Phi }(𝐫,t)=\frac{1}{ϵ_0}\rho _n(𝐫,t)$$
$`(6)`$
and

$$^2𝐀(𝐫,t)\frac{1}{c^2}\frac{^2}{t^2}𝐀(𝐫,t)=\mu _0𝐉_n(𝐫,t),$$
$`(7)`$
where $`\mu _0=1/ϵ_0c^2`$ and the position vector $`𝐫`$ together with the time derivative $`/t`$ is referred to the local-ether frame, the reference frame of the wave propagation.

Then, by manipulating the wave equations of potentials according to the definitions of fields, the wave equations of fields can be derived. By so doing, we have the local-ether wave equation of magnetic field

$$^2𝐁(𝐫,t)\frac{1}{c^2}\frac{^2}{t^2}𝐁(𝐫,t)=\mu _0\times 𝐉_n(𝐫,t)$$
$`(8)`$
and the local-ether wave equation of electric field

$$^2𝐄(𝐫,t)\frac{1}{c^2}\frac{^2}{t^2}𝐄(𝐫,t)=\frac{1}{ϵ_0}\rho _n(𝐫,t)+\mu _0\left(\frac{}{t}𝐉_n(𝐫,t)\right)_m,$$
$`(9)`$
where, again, the position vector $`𝐫`$ together with the time derivative $`/t`$ is referred to the local-ether frame. It is noted that in the preceding equation the time derivative applied to the current density is referred to the matrix frame and the velocity of the mobile source particles forming this current density is also referred to this frame. In free space having no sources, the local-ether wave equations take a simpler form of

$$^2\mathrm{\Psi }(𝐫,t)\frac{1}{c^2}\frac{^2}{t^2}\mathrm{\Psi }(𝐫,t)=0,$$
$`(10)`$
where $`\mathrm{\Psi }`$ denotes the scalar potential $`\mathrm{\Phi }`$ or any Cartesian component of the vector potential $`𝐀`$, electric field $`𝐄`$, or magnetic field $`𝐁`$. It is seen that both electric and magnetic fields as well as the potentials propagate at the speed $`c`$ with respect to the local-ether frame. These local-ether wave equations made their debut in .

Consider the case of wave propagation in a uniform magnetic medium of permeability $`\mu `$, where $`𝐉_n=\times 𝐌`$ for the magnetization current and the magnetization vector $`𝐌=(1/\mu _01/\mu )𝐁`$. Thereby, the wave equation of magnetic field becomes

$$\frac{\mu _0}{\mu }^2𝐁(𝐫,t)\frac{1}{c^2}\frac{^2}{t^2}𝐁(𝐫,t)=0,$$
$`(11)`$
where we have made use of the relation $`𝐁=0`$, which in turn is a consequence of (3). It is seen that in a uniform magnetic medium of $`\mu `$, electromagnetic wave propagates at the speed $`c\sqrt{\mu _0/\mu }`$ with respect to the local-ether frame. In the preceding derivation, no information about the motion of the magnetic medium is involved. Thus the derived propagation speed is independent of the motion of a uniform magnetic medium.

Consider the analogous case of wave propagation in a dielectric medium of permittivity $`ϵ`$, where

$$𝐉_n(𝐫,t)=\left(\frac{}{t}𝐏(𝐫,t)\right)_m$$
$`(12)`$
for the polarization current and the polarization vector $`𝐏=(ϵϵ_0)𝐄`$. Note that the polarization current density is associated with the time derivative of the polarization vector with respect to the matrix frame, since the displacement of the polarization charge under the influence of electric field is relative to the ions forming the matrix and the drift velocity $`𝐯_{sm}`$ of the source particles forming a neutralized current is also referred to the matrix frame. Another consequence pertinent to this drift velocity is that the conservation of charge leads to another relation between $`𝐉_n`$ and $`\rho _v`$ of

$$𝐉_n(𝐫,t)=\left(\frac{}{t}\rho _v(𝐫,t)\right)_m.$$
$`(13)`$
This relation is just the continuity equation, except that the time derivative applied to the charge density is referred specifically to the matrix frame. Further, this matrix-frame continuity equation can be given in terms of the net charge density as

$$𝐉_n(𝐫,t)=\left(\frac{}{t}\rho _n(𝐫,t)\right)_m.$$
$`(14)`$
This is owing to the fact that the matrix charge density $`\rho _m`$ is time-independent in the matrix frame. The preceding continuity equation leads to a relation between the polarization charge density and the polarization vector as $`\rho _n=𝐏`$, where we have made use of the initial condition that a uniform polarization ($`𝐏=0`$) corresponds to the complete neutralization ($`\rho _n=0`$). Thereby, by using electric field to express the net charge density and the neutralized current density induced in a dielectric medium, the wave equation of electric field becomes

$$^2𝐄(𝐫,t)\frac{1}{c^2}\frac{^2𝐄(𝐫,t)}{t^2}=\frac{1}{ϵ_0}[(ϵϵ_0)𝐄(𝐫,t)]+\frac{ϵϵ_0}{ϵ_0}\frac{1}{c^2}\left(\frac{^2𝐄(𝐫,t)}{t^2}\right)_m.$$
$`(15)`$
It is noted that this wave equation involves two time derivatives of electric field referred to different frames.

Remark that based on Galilean transformations, the time derivatives of an arbitrary function $`f`$ of space and time with respect to the matrix and the local-ether frames are related by

$$\left(\frac{f}{t}\right)_m=\frac{f}{t}+𝐯_mf,$$
$`(16)`$
where the time derivatives $`/t`$ and $`(/t)_m`$ are understood to be taken under constant $`𝐫`$ and ($`𝐫𝐯_mt`$), respectively, as the position vector $`𝐫`$ is referred to the local-ether frame. Further, from the preceding relation, the second-order time derivative in the matrix frame can be given in terms of the derivatives in the local-ether frame as

$$\left(\frac{^2f}{t^2}\right)_m=\frac{^2f}{t^2}+2\left(𝐯_m\right)\frac{f}{t}+\left(𝐯_m\right)\left(𝐯_m\right)f.$$
$`(17)`$
The Galilean formulas (16) and (17) have been given in  and , respectively.

Then, by using the Galilean formula (17), the wave equation of electric field can be rewritten as

$$^2𝐄(𝐫,t)\frac{ϵ}{ϵ_0}\frac{1}{c^2}\frac{^2𝐄(𝐫,t)}{t^2}=\frac{1}{ϵ_0}[(ϵϵ_0)𝐄(𝐫,t)]$$

$$+\frac{ϵϵ_0}{ϵ_0}\frac{1}{c^2}\left[2\left(𝐯_m\right)\frac{𝐄(𝐫,t)}{t}+\left(𝐯_m\right)\left(𝐯_m\right)𝐄(𝐫,t)\right].$$
$`(18)`$
It is noted that this wave equation of electric field involves the matrix velocity with respect to the local-ether frame. This feature is quite different from that in the wave equation of magnetic field (11). Physically, this difference is due to the situation that polarization current is associated with the matrix-frame time derivative of field, while magnetization current is with a space derivative. In terms of the matrix-frame time derivatives, the local-ether wave equation of electric field can be rewritten as

$$^2𝐄\frac{ϵ}{ϵ_0}\frac{1}{c^2}\left(\frac{^2𝐄}{t^2}\right)_m=\frac{1}{ϵ_0}[(ϵϵ_0)𝐄]\frac{2}{c^2}\left(𝐯_m\right)\left(\frac{𝐄}{t}\right)_m,$$
$`(19)`$
where the second-order term of the normalized speed $`v_m/c`$ is ignored. It is seen that the last term in the preceding matrix-frame wave equation is smaller in magnitude than the other terms by a factor of the order of the normalized speed $`v_m/c`$.

Consider the simpler case where a $`z`$-polarized uniform plane wave propagates along the $`x`$ direction in a uniform dielectric medium. The medium is moving at a velocity $`𝐯_f`$ with respect to a laboratory frame which in turn is moving at a velocity $`𝐯_0`$ with respect to the local-ether frame. Based on Galilean transformations, the matrix velocity with respect to the local-ether frame is simply $`𝐯_m=𝐯_f+𝐯_0`$. Then, to the first order of normalized speed, the wave equation (18) can be simplified to a form of

$$\frac{^2}{x^2}E_z(x,t)\frac{ϵ}{ϵ_0}\frac{1}{c^2}\frac{^2}{t^2}E_z(x,t)=2v_{mx}\frac{ϵϵ_0}{ϵ_0}\frac{1}{c^2}\frac{^2}{xt}E_z(x,t),$$
$`(20)`$
where $`v_{mx}=𝐯_m\widehat{x}`$. It is noted that the term $`(ϵϵ_0)𝐄`$ associated with the polarization charge vanishes, since both permittivity $`ϵ`$ and field $`𝐄`$ are supposed to have no variations along the $`z`$ direction of the field.

Suppose that the solution of this wave equation is of a harmonic form as $`E_z=E_0e^{ikx}e^{i\omega t}`$, where $`x`$ is referred to the local-ether frame and $`E_0`$ is an arbitrary constant. Then the preceding wave equation immediately leads to an algebraic equation

$$k^2\frac{ϵ}{ϵ_0}\frac{\omega ^2}{c^2}=2v_{mx}\frac{ϵϵ_0}{ϵ_0}\frac{1}{c^2}k\omega .$$
$`(21)`$
It is easy to show that to the first order of normalized speed, the propagation constant $`k`$ can be given in terms of the angular frequency $`\omega `$ as

$$k=\frac{\omega }{c}\left\{\sqrt{\frac{ϵ}{ϵ_0}}\frac{v_{mx}}{c}\frac{ϵϵ_0}{ϵ_0}\right\}.$$
$`(22)`$
It is noted that this propagation constant depends on the speed $`v_{mx}`$, in addition to the familiar dependence on permittivity $`ϵ`$. Consequently, this relation presents a modification of the propagation constant due to the motion of the dielectric medium with respect to the local ether. Physically, the dependence on the matrix speed originates from the situation that the polarization current and its time derivative in the wave equation are referred to the matrix frame rather than to the local-ether one.

The phase speed $`c^{}`$ ($`=\omega /k`$) of the electromagnetic wave propagating in the moving dielectric medium is then given by

$$c^{}=\frac{c}{n}+v_{mx}\left(1\frac{1}{n^2}\right),$$
$`(23)`$
where the phase speed is referred to the local-ether frame and the refractive index $`n=\sqrt{ϵ/ϵ_0}`$. It is seen that the component of the matrix velocity parallel to the propagation direction affects the phase speed, while the transverse components do not.

The wave equation (20) can also be written in the matrix frame. To the first order of normalized speed, this wave equation reads

$$\frac{^2}{x^2}E_z(x,t)\frac{ϵ}{ϵ_0}\frac{1}{c^2}\left(\frac{^2}{t^2}E_z(x,t)\right)_m=2v_{mx}\frac{1}{c^2}\left(\frac{^2}{xt}E_z(x,t)\right)_m.$$
$`(24)`$
It can be shown that $`k=(\omega _m/c)(n+v_{mx}/c)`$ and $`c_m^{}=\omega _m/k=c/nv_{mx}/n^2`$, where $`\omega _m`$ and $`c_m^{}`$ are the angular frequency and the phase speed of the wave when observed in the matrix frame, respectively. It is seen that

$$c_m^{}=c^{}v_{mx},$$
$`(25)`$
which states that the difference in the observed phase speed between the two reference frames is just the relative speed between the frames along the propagation direction. In other words, the derived phase speeds in the two frames comply with Galilean transformations.

The phase speed given in (23) is similar to the speed obtained from the velocity transformation in the special relativity, which in turn is known to have been demonstrated in the famous Fizeau’s interferometry experiment with flowing water. However, the fundamental difference is that the phase speed $`c^{}`$ and the matrix velocity $`𝐯_m`$ are referred specifically to the local-ether frame. Thus the matrix velocity $`𝐯_m`$ incorporates the laboratory velocity $`𝐯_0`$ with respect to the local-ether frame. An old interpretation of the dependence of the phase speed on the medium velocity given in (23) is known as the Fresnel drag effect , whereby the ether is dragged partially by the moving medium to an extent depending on the index $`n`$. If $`n`$ is large enough, $`c^{}c/n+v_{mx}`$ and $`c_m^{}c/n`$. It is seen that the phase speed with respect to the moving medium is independent of the velocity of the medium. Thus it seems that the ether is completely dragged by the medium. However, according to the wave equation of electric field (15), the earth local ether is still stationary in an ECI frame, regardless of the permittivity and the velocity of a terrestrial medium. The change in the phase speed of a wave propagating in a dielectric medium, stationary or moving, is due to the effect of the polarization which in turn is induced by and related to electric field. Further, it is noted that the interpretation similar to the ether dragging is applicable only for a uniform plane wave propagating in a uniform dielectric medium and is correct only to the first order. In other words, according to the local-ether wave equation, the phase-speed formula (23) does not hold in a magnetic medium and can be no longer valid in a nonuniform dielectric medium where polarization charge emerges. Thus the applicability of the phase-speed formula has some hidden restrictions. This presents a viewpoint different from the ether-dragging notion and another discrepancy from the special relativity.

4. Reexamination of Various Interferometry Experiments

In this section we reexamine some precision interferometry experiments reported in the literature to test the local-ether wave equation of electric field. They include the fiber-link experiment with a geostationary setup and a geostationary optical fiber, the Sagnac loop interferometry with a rotating path and a comoving or geostationary dielectric medium, and Fizeau’s experiment with a geostationary interferometer and a moving dielectric medium. For these earthbound experiments, the local ether is stationary in an ECI frame and hence earth’s rotation should be taken into consideration, even for a geostationary medium or path. On the other hand, these experiments are entirely independent of earth’s orbital motion around the Sun or others.

4.1. Phase variation with moving medium and path

First of all, consider an interferometer of which each segment of propagation path has a fixed shape and is implemented with a pair of mirrors in air, with a pipe filled with flowing dielectric liquid, or with a solid dielectric fiber. Remark that for an electromagnetic wave propagating in an arbitrary direction $`\widehat{l}`$ along a path filled with a dielectric medium moving at a velocity $`𝐯_m`$ with respect to the local-ether frame, the propagation constant can be written as

$$k=k_0\left\{n+\left(1n^2\right)\widehat{l}𝐯_m/c\right\},$$
$`(26)`$
where $`k_0=\omega /c`$ and $`n`$ is the refractive index of the uniform moving medium.

Further, consider a propagation path segment of length $`l`$, such as a linear section of the pipe or fiber. Owing to the movement of the segment during the wave propagation through it, the propagation range which represents the actual propagation length is not actually $`l`$. As in the classical propagation model, the propagation range $`l^{}`$ depends on the velocity of the path segment with respect to the local ether. The influence on propagation due to the difference between the propagation range $`l^{}`$ and the path length $`l`$ is known as the Sagnac effect. By following the derivation of the Sagnac effect for electromagnetic wave propagating in free space discussed elaborately in , the propagation range $`l^{}`$ for a wave propagating in the direction $`\widehat{l}`$ along a moving segment, when given to the first order of normalized speed, is

$$l^{}=l\left\{1+n\widehat{l}𝐯_l/c\right\},$$
$`(27)`$
where $`𝐯_l`$ is the velocity of the path segment with respect to the local-ether frame.

It is supposed that the phase variation over the propagation path is given by $`\varphi =kl^{}`$. To the first order of normalized speed, the phase variation associated with the moving medium and path is then given from the two preceding formulas by

$$\varphi =k_0l\left\{n+(1n^2)\widehat{l}𝐯_m/c+n^2\widehat{l}𝐯_l/c\right\}.$$
$`(28)`$
It is seen that the phase variation depends on the longitudinal (to the propagation path) $`\widehat{l}`$ components of the medium velocity and the path velocity both with respect to the local-ether frame. Furthermore, these longitudinal-speed terms connect with the refractive index. Thereby, in addition to the familiar effect on the propagation constant, the refractive index also has effects on the matrix-velocity modification of the propagation constant and the path-velocity modification of the propagation length. The preceding phase-variation formula can be rewritten as

$$\varphi =k_0l\left\{n+n^2\widehat{l}𝐯_{lm}/c+\widehat{l}𝐯_m/c\right\},$$
$`(29)`$
where $`𝐯_{lm}=𝐯_l𝐯_m`$ denotes the Newtonian relative velocity of the moving path with respect to the moving dielectric medium. It is seen that one of the velocity-dependent terms depends on the refractive index and is associated with a Newtonian relative velocity, while the other velocity-dependent term is independent of the index and is associated with the individual velocity of the dielectric medium. For the case where the medium comoves with the propagation path ($`𝐯_{lm}=0`$), the velocity-dependent phase variation is no longer dependent on the index.

4.2. Geostationary fiber-link experiment

Then we consider the experiment of one-way fiber link by Krisher et al., where the phase difference between two waves generated from two identical stable hydrogen masers at 100 MHz was measured by using a network analyzer . The two masers are separated by a long distance of 21 km and linked by a stable optical fiber. One signal was fed directly into the analyzer, while the other was used to modulate a laser carrier to propagate over the fiber. For a geostationary fiber, $`𝐯_m=𝐯_l=𝐯_E`$, where $`𝐯_E`$ is the linear velocity due to earth’s rotation. Then formula (29) immediately leads to that the phase variation $`d\varphi `$ over a geostationary fiber segment of differential length $`dl`$ is given by

$$d\varphi =k_0\left(n+\widehat{l}𝐯_E/c\right)dl.$$
$`(30)`$
Thus the phase variation over a propagation path $`L`$ of length $`l`$ is given by the path integral

$$\varphi =k_0\left(nl+\frac{1}{c}_L𝐯_E𝑑𝐥\right),$$
$`(31)`$
where the directed differential length $`d𝐥=\widehat{l}dl`$. It is noted that the velocity-dependent part is independent of the refractive index, since the velocity difference $`𝐯_{lm}=0`$. Furthermore, it is noted that although the velocity-dependent phase variation is due to earth’s rotation, its value is invariant under this rotation. This is because that both $`𝐯_E`$ and $`d𝐥`$ change in a coordinated way such that their dot product remains unchanged during earth’s rotation. This invariance is in accord with the spatial isotropy demonstrated in the one-way fiber-link experiment, where it is observed that the phase variation is highly stable (as determined from the phase difference between the two waves measured every a few seconds during a couple of days), regardless of earth’s rotational and orbital motions .

When the fiber link is placed in a geographically small region such that the velocity $`𝐯_E`$ due to earth’s rotation is substantially constant, the phase variation over the link becomes

$$\varphi =k_0\left(nl+\frac{1}{c}𝐯_E𝐝\right),$$
$`(32)`$
where $`𝐝`$ is the directed separation distance from the end through which the light enters the fiber to the other end. It is noted that the phase variation is independent of the actual wiring, but depends on the orientation of the distance $`𝐝`$ with respect to the ground. If the fiber-link experimental setup is put on a turntable or a rotor, it is expected that the phase variation will change as the turntable is rotating even slowly. From the minor term in the preceding formula, the dependence of the phase variation on the orientation of the rotor is given by

$$\delta \varphi =\frac{\omega }{c^2}\omega _ER_E|𝐝|\mathrm{cos}\theta _l\mathrm{cos}\theta _T,$$
$`(33)`$
where $`R_E`$ is earth’s radius, $`\theta _l`$ is the latitude, $`\theta _T`$ is the angle of the distance $`𝐝`$ from the east, and the turntable is suitably positioned on a horizontal plane so that the gravitational effect on $`\omega `$ is avoided. The phase variation associated with earth’s rotation is independent of the refractive index of the fiber and hence is identical to the one in the case with a free-space link discussed in . It is noted that the phase variation becomes maximum and minimum, as the distance $`𝐝`$ points to the east and the west, respectively. Furthermore, the phase variation changes sinusoidally with the angle $`\theta _T`$. This dipole anisotropy in phase variation predicted in the proposed one-way-link rotor experiment then provides a means to test the local-ether wave equation.

4.3. Sagnac rotating-loop experiments

Consider the Sagnac effect in a rotating-loop interferometer associated with the interference between two coherent waves corotating and counterrotating with respect to the propagation loop, respectively. Commonly, the propagation path is composed of beam splitter and mirrors in air. Then the phase difference between the two waves results from the situation that the modification of propagation length due to the rotation of the loop is different between these waves propagating in opposite directions. Here, we deal with a propagation path filled with a general dielectric medium rather than a free space.

Suppose that the loop is rotating about an axis as observed from a laboratory, which in turn is rotating with the Earth. The velocity of the path segment with respect to the an ECI frame is given by $`𝐯_l=𝐯_I+𝐯_{E0}+𝐯_0`$, where $`𝐯_0`$ is the laboratory velocity with respect to an ECI frame referred to a suitable point $`𝐫_0`$ on the interferometer rotation axis, $`𝐯_I=\overline{\omega }_I\times (𝐫𝐫_0)`$ and $`𝐯_{E0}=\overline{\omega }_E\times (𝐫𝐫_0)`$ denote the other contributions to the path velocity due to the rotations of the loop and the Earth at the directed rotation rates $`\overline{\omega }_I`$ and $`\overline{\omega }_E`$, respectively, and $`𝐫`$ is the position vector of the path segment in the frame of the reference point $`𝐫_0`$.

Consider the case where the medium is comoving with the rotating loop. Thus the velocity difference $`𝐯_{lm}=0`$ and hence formula (29) leads to that the phase variation $`d\varphi `$ over a propagation path of differential length $`dl`$ is given by

$$d\varphi =k_0\left(n+\widehat{l}𝐯_l/c\right)dl.$$
$`(34)`$
The unit vectors $`\widehat{l}`$ denoting the propagation directions of the two counterpropagating waves are antiparallel to each other in each path segment. Thus the difference in the phase variation over the loop $`L`$ between the two waves is then given by the path integral

$$\mathrm{}\varphi =\frac{2k_0}{c}_L(𝐯_I+𝐯_{E0})𝑑𝐥,$$
$`(35)`$
where we have made use of the facts that the major term $`k_0ndl`$ in (34) is identical for the two waves and hence its contributions to the phase difference cancel out and that the contributions of a constant vector $`𝐯_0`$ to the phase variation over a closed path cancel out collectively, regardless of the actual structure of the loop.

Suppose the loop is coplanar. Then, by using a vector identity, the phase difference can be given by

$$\mathrm{}\varphi =\frac{4k_0}{c}(\overline{\omega }_I+\overline{\omega }_E)𝐒,$$
$`(36)`$
where $`𝐒`$ ($`=\frac{1}{2}_L(𝐫𝐫_0)\times 𝑑𝐥`$) denotes the directed area enclosed by loop $`L`$. It is noted that the phase difference is independent of the index $`n`$ and hence is identical to the one in the case with a free-space path discussed in . Again, this independence is owing to the coincidence that the index-dependent modification of the propagation constant happens to cancel the one of the propagation length. This null effect of the refractive index on the phase difference in the Sagnac loop interferometry has been demonstrated experimentally by Harzer in as early as 1914 . Further, the preceding phase-difference formula has been put in practical use in fiber gyroscopes \[10-12\]. Alternative derivations of this formula by taking the Sagnac effect and the modifications of phase speed into account can be found in \[9-11\]. Anyway, in spite of the restriction on reference frame, the local-ether wave equation of electric field is in accord with the Sagnac interferometry experiment with a rotating loop and a comoving dielectric medium. On the other hand, the local-ether wave equation precludes the possibility of detecting earth’s orbital motion by using earthbound fiber gyroscopes.

Next, consider the case where the medium is geostationary while the propagation loop is still rotating with respect to the laboratory. Thus $`𝐯_{lm}=𝐯_I`$, $`𝐯_m=𝐯_{E0}+𝐯_0`$, and hence formula (29) leads to that the phase variation $`d\varphi `$ over a path of differential length $`dl`$ is given by

$$d\varphi =k_0dl\left(n+n^2\widehat{l}𝐯_I/c+\widehat{l}𝐯_{E0}/c+\widehat{l}𝐯_0/c\right).$$
$`(37)`$
The corresponding phase difference between the waves becomes

$$\mathrm{}\varphi =\frac{4k_0}{c}(n^2\overline{\omega }_I+\overline{\omega }_E)𝐒.$$
$`(38)`$
It is seen that the phase difference then depends on the index $`n`$ which in turn connects to the loop rotation rate $`\overline{\omega }_I`$. Again, the phase variation associated with earth’s rotation is independent of the index and the phase difference is independent of the laboratory velocity $`𝐯_0`$. Ordinarily, $`\omega _E\omega _I`$ and hence the phase difference is substantially proportional to $`n^2`$. This index-dependence of the phase difference is identical to that given in , although the approach is quite different. The increase of phase difference in the presence of a stationary dielectric medium has been demonstrated experimentally by Dufour and Prunier in 1942 . The various index-dependences among the terms connected to the rate $`\overline{\omega }_I`$ or $`\overline{\omega }_E`$ in (36) and (38) then provide another means to test the local-ether wave equation.

4.4. Fizeau’s experiment with moving medium

The last case is then the one where the interferometer is stationary while the medium is moving. Consider Fizeau’s experiment dealing with the interference between two optical waves propagating in opposite directions along a stationary pipe filled with flowing water. For generality, suppose that the pipe together with beam splitters, mirrors, and other components of the interferometer is stationary in a laboratory frame which in turn moves at a velocity $`𝐯_0`$ with respect to an ECI frame. As the interferometer is geographically small, the path velocity is substantially constant over the setup. Thus the path velocity $`𝐯_l=𝐯_0`$. Further, suppose that the water is flowing at a velocity $`𝐯_f`$ with respect to the pipe. Then the velocity difference $`𝐯_{lm}=𝐯_f`$, the matrix velocity $`𝐯_m=𝐯_f+𝐯_0`$, and hence formula (29) leads to that the phase variation $`d\varphi `$ over a pipe of differential length $`dl`$ is given by

$$d\varphi =k_0dl\left\{n+(1n^2)\widehat{l}𝐯_f/c+\widehat{l}𝐯_0/c\right\},$$
$`(39)`$
where $`n`$ is the index of the flowing water and $`\widehat{l}𝐯_f=\pm v_f`$ for the two beams.

It is seen that the phase variation depends on the laboratory velocity. However, the effect of this velocity on phase variation can not be detected in Fizeau’s experiment. This is because that the optical path actually adopted in the experiment is closed, part of the path is filled with flowing water and part is merely with air (see the figure in  or ). It is noted that in the preceding formula the velocity $`𝐯_0`$ does not connect to the index $`n`$. Again, the phase variation over a closed path given by the circulation of a constant vector $`𝐯_0`$ is zero.

As in the Sagnac loop interferometry, the two waves to be interfered propagate in opposite directions in each individual segment of the path. From the preceding formula it is seen that those parts of the path filled with air or with a dielectric at rest with the pipe do not contribute to the phase difference between the waves. The contribution comes only from the water-flowing pipe. Suppose that the water speed $`v_f`$ is uniform and the total length of the water-flowing pipe is $`l`$. Then the difference in phase variation between the two counterpropagating waves is given by

$$\mathrm{}\varphi =2k_0l(n^21)v_f/c.$$
$`(40)`$
It is noted that the phase difference is linearly proportional to ($`n^21`$) and to the water speed $`v_f`$ with respect to the pipe. The preceding phase-difference formula agrees with the interference fringe observed in Fizeau’s experiment with various speeds $`v_f`$ and indices $`n`$.

More precisely, the path velocity $`𝐯_l`$ is not actually a constant value $`𝐯_0`$ over the closed path. That is, $`𝐯_l=𝐯_{E0}+𝐯_0`$ and $`𝐯_m=𝐯_f+𝐯_{E0}+𝐯_0`$, where $`𝐯_0`$ is referred to a suitable point in the setup. Hence the Sagnac effect in a loop interferometer due to earth’s rotation should also appear in Fizeau’s experiment. However, as earth’s rotation rate is relatively slow, its effect in Fizeau’s experiment is ordinarily much smaller than that due to the motion of the medium, just as its effect in the rotating-loop experiment is ordinarily much smaller than that due to the rotation of the loop. Thereby, the phase difference is substantially independent of earth’s rotation. Furthermore, at least to the first order of normalized speed, Fizeau’s experiment together with the Sagnac rotating-loop experiments is independent of the laboratory velocity $`𝐯_0`$ and hence complies with Galilean relativity, in spite of the restriction on reference frame of the medium and the path velocities.

5. Conclusion

Based on the local-ether model of wave propagation, the propagation of the potentials is referred specifically to an ECI frame in earthbound experiments. Further, under the ordinary condition of low drift speed, the electromagnetic force can be given in terms of electric and magnetic fields which in turn are given explicitly in terms of the local-ether potentials. The position vectors, time derivatives, particle velocities, propagation velocity, and current density involved are all referred specifically to their respective reference frames. Consequently, the values of potentials, fields, and force remain unchanged in different frames.

Further, based on the definitions of fields in terms of potentials, the local-ether wave equations of fields are derived. From the wave equation of magnetic field, the phase speed of electromagnetic wave in a uniform magnetic medium is found to depend on the permeability, but not on the motion of the medium. However, from the wave equation of electric field, the phase speed of a uniform plane wave propagating in a moving uniform dielectric medium is found to depend on the longitudinal component of the medium velocity and hence to incorporate the familiar Fresnel drag coefficient. This phase speed looks like the speed obtained from the velocity transformation in the special relativity. However, the fundamental difference is that the phase and the matrix speeds are referred specifically to the local-ether frame. Moreover, this phase-speed formula is not expected to hold in a magnetic or a nonuniform dielectric medium.

By taking the matrix-velocity modification of the propagation constant and the Sagnac path-velocity modification of the propagation length into account, the phase variation over a moving path filled with a moving dielectric medium is presented. Thereby, this phase-variation formula is applied to analyze various precision interferometry experiments in a consistent way. It is found that this formula is actually in accord with the spatial isotropy in the one-way fiber-link experiment, with the null effect of permittivity in the Sagnac interferometer with a dielectric medium comoving with the rotating loop, with the increase of phase difference in the Sagnac interferometer with a geostationary dielectric medium, and with the dependence of phase difference on the speed and index of the flowing water in Fizeau’s experiment. These together provide a support for the local-ether wave equation of electric field. Moreover, it is predicted that as the fiber-link experimental setup is put on a turntable, the phase variation over the link will change sinusoidally as the orientation of turntable is changing. This proposed one-way-link rotor experiment, the predicted null effect of earth’s orbital motion in earthbound interferometers, the predicted various index-dependences among the phase-shift terms connected to the rotation rate of the loop or of the Earth in the Sagnac interferometer, and the aforementioned discrepancies in the phase-speed formula for a moving medium and the restrictions on this formula then provide different approaches to test the local-ether wave equation.

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# 1

Osmotic properties of polyethyleneglycols:
quantitative features of brush and bulk scaling laws
Per Lyngs Hansen,†⋆ Joel A. Cohen,†‡ Rudi Podgornik,†§
and V. Adrian Parsegian
Laboratory of Physical and Structural Biology
National Institute of Child Health and Human Development
National Institutes of Health, Bethesda, MD 20892-5626
MEMPHYS - Center for Biomembrane Physics
University of Southern Denmark
Campusvej 55, DK-5230 Odense M
Denmark
Department of Physiology, University of the Pacific
San Francisco, CA 94115
§Department of Physics
Faculty of Mathematics and Physics
University of Ljubljana, SI-1000 Ljubljana, Slovenia
Keywords: PEG-grafted liposomes, bulk polymer solutions, osmotic pressure, osmotic stress, polymer brush, scaling laws

Running title: PEG brush and bulk scaling laws

Abstract

From glycosylated cell surfaces to sterically stabilized liposomes, polymers attached to membranes attract biological and therapeutic interest. Can the scaling laws of polymer ”brushes” describe the physical properties of these coats? We delineate conditions where the Alexander - de Gennes theory of polymer brushes successfully describes the intermembrane distance vs. applied osmotic stress data of Kenworthy et al. for PEG-grafted multilamellar liposomes \[Biophys. J. (1995) 68:1921\]. We establish that the polymer density and size in the brush must be high enough that, in a bulk solution of equivalent density, the polymer osmotic pressure is independent of polymer molecular weight (the des Cloizeaux semi-dilute regime of bulk polymer solutions). The condition that attached polymers behave as semi-dilute bulk solutions offers a rigorous criterion for brush scaling-law behavior. There is a deep connection between the behaviors of polymer solutions in bulk and polymers grafted to a surface at a density such that neighbors pack to form a uniform brush. In this regime, two-parameter unconstrained fits of the Alexander - de Gennes brush scaling laws yield effective monomer lengths of 3.3 to 3.5 Å, which agree with structural predictions. The fitted distances between grafting sites are larger than expected from the nominal content of PEG-lipids; the chains apparently saturate the surface. Osmotic stress measurements can be used to estimate the actual densities of membrane-grafted polymers.

INTRODUCTION

Membrane surfaces decorated with end-grafted polymers are ubiquitous in biology (for example, glycosylated cell surfaces such as the red blood cell glycocalyx). Organelles (e.g., microtubules) also posses polymeric ”hairs” that are integral to their function (Sackett, 1995). A relatively well-defined example of a surface-attached polymeric coat is that of poly(ethylene glycol) (PEG), also known as poly(ethylene oxide) (PEO). These polymer coatings attract strong interest because of their ability to shield surfaces from close interactions with other surfaces including macromolecules. They thus provide steric stabilization to colloidal suspensions (Lasic and Martin, 1995), biocompatibility to medically-implanted materials (Dumitriu, 2002), and ”stealth” properties to intravenously-injected liposomes. Such liposomes are in current therapeutic use as vehicles for in-vivo drug delivery (Lasic and Martin, 1995).

It is commonly believed that in order to provide effective shielding of a surface from interactions with aqueous substances, the attached polymers must provide a surface layer of adequate coverage and thickness, i.e., they must approximate a surface ”brush” (Szleifer, 1997). Polymers dilutely grafted to a surface are said to form ”mushrooms” when the mean distance between grafting sites $`D`$ is larger than the polymer size $`R_F`$ (Flory radius), so that individual polymer chains remain widely separated and do not interact with each other. If $`D`$ is decreased (higher grafting density) and/or $`R_F`$ is increased (longer polymers) such that $`DR_F`$, then individual chains start to overlap and the polymers begin to interact. This ”overlap criterion” defines the so called ”mushroom-to-brush transition”, and is commonly used to signify the beginning of brush-like behavior of the grafted polymer layer. A major point of this paper is that brush scaling laws are not applicable in this so-called ”weak overlap regime”. Validity of brush scaling laws can be expected only for strong overlap, which is defined by a criterion different than the above.

The physicochemical characterization of a system of PEG chains end-grafted to the surface of a supporting lipid bilayer has biological and practical significance, but is also relevant to polymer physics (de Gennes, 1987). A well-tested scaling theory of the polymer brush, due to Alexander and de Gennes (AdG) exists and is currently well accepted (Alexander, 1977; de Gennes, 1987). It is thus important to ascertain whether, or under what conditions, the grafted PEG system adheres to established brush scaling laws.

To date, several investigators have addressed this issue by performing compression experiments in which two or more PEG-grafted bilayers are forced together, and force vs. intermembrane distance is measured. The geometry of such an arrangement is illustrated in Fig. 1, where parameters relevant to the theoretical analysis (see below) are also shown. For such data to be relevant to brush scaling laws, two criteria must be met: (1) The intermembrane forces must be dominated by interactions between the polymer chains, as opposed to electrostatic, van der Waals, hydration, or undulation forces. (2) The grafted polymer chains must exist in a strong brush conformation, as opposed to mushrooms or a weak brush-like state not far from the mushroom-to-brush transition.

Kuhl et al. (1994), using a surface force apparatus (SFA), measured force vs. intermembrane distance for mica-supported bilayers whose apposed surfaces were composed of mixtures of distearoylphosphatidylethanolamine (DSPE) and PEG-grafted DSPE. Long-range repulsive forces were observed, and subtraction of the electrostatic component yielded repulsions attributable to interactions between the PEG surface layers. The densest conditions studied were PEG-2000 (45 monomers) at a grafting density corresponding to 9 mol % PEG-PE.

Kenworthy et al. (1995a), using osmotic stress (OS), measured osmotic pressure vs. intermembrane distance for multilamellar liposomes composed of mixtures of distearoylphosphatidylcholine (DSPC) and PEG-grafted DSPE. Clear evidence was given for interactions mediated by the PEG chains. Nominal densities of the grafted PEGs (for Avanti lipids) ranged up to 30 mol % PEG-2000 and 20 mol % PEG-5000 (113 monomers).

Another technique for measuring intermembrane force vs. distance with PEG-grafted liposomes is that of micropipet manipulations (Needham et al., 1992; Evans et al., 1996). However, the conditions for these experiments have thus far not been amenable to brush scaling analysis.

In cases where results were analyzed in terms of the AdG brush scaling theory (Kuhl et al., 1994; Kenworthy et al., 1995a; Lasic, 1997), agreement between theory and experiment was not satisfactory. However, it has been noted (Szleifer, 1996) that most of the above data lies in a broad mushroom-to-brush transition region, and since scaling laws do not apply to this intermediate regime, quantitative fits are not to be expected. Szleifer (1996) has discussed the successful application of computer simulations and molecular theories to experimental data in the mushroom-to-brush transition regime. While such approaches apply also in the strong-brush limit, they do not yield scaling laws and lack the robust predictions of scaling theory for semidilute solutions. Our interest here is to ascertain whether bulk and surface-grafted PEG systems can fulfill the criteria for analytical scaling theories, and if so, whether the scaling laws can be successfully applied.

The unanswered questions remain: can the grafted PEG layers on lipid membrane surfaces exist in a brush regime, and if so, do they obey brush scaling laws?

In this paper we first examine the relation between brush scaling laws and the behavior of polymer chains in bulk solution. Bulk PEG solutions are shown to exhibit scaling behavior under experimentally-realizable conditions. We then examine the validity of AdG scaling laws as applied to PEG-grafted lipid bilayers. An operational criterion is presented for determining the PEG brush scaling regime, and the range of validity of the scaling laws is shown to be more restrictive than often supposed. When applied to those data of Kenworthy et al. that satisfy the brush criterion, brush scaling laws are found to be valid. Further, fits to the data yield hitherto difficult-to-obtain information on the density of PEG grafts present on the bilayer surface. As a function of mol fraction of added PEG-lipid, these densities plateau at values smaller than the nominal densities, indicative of surface saturation effects. The saturation mol fractions of PEG lipids in the bilayer are consistent with earlier estimates of this phenomenon.

RESULTS

When flexible polymers such as PEG are end-grafted to a surface, brush formation begins when $`DR_F`$, i.e., when the average distance between grafting sites $`D`$ is comparable to the Flory radius $`R_F=aN^{3/5}`$, where $`a`$ is the effective monomer length, and $`N`$ is the number of monomers per polymer chain. However, it is important to realize that a brush is not fully developed unless the monomer density $`\overline{\varphi }`$ is large enough (and chain overlap is strong enough) that a semi-dilute solution is formed. For a description of semi-diluteness in a brush, see the Appendix and de Gennes (1979). It is important to emphasize that in a non-compressed brush, the celebrated linear relation between the brush thickness and number of monomers $`L_0aN(a/D)^{2/3}`$, as well as the molecular-weight-independent relation $`\overline{\varphi _0}(a/D)^{4/3}`$ between the spatially-constant volume fraction of monomers111The Alexander - de Gennes model may be improved in several respects. For instance, one may self consistently calculate an improved monomer density profile, as in Milner-Witten-Cates theory (Milner et al., 1988). Such improvements affect our force and osmotic pressure predictions to a very limited extent (Kenworthy et al., 1995a) and we shall ignore them here. and $`D`$, are both consequences of semi-dilute solution behavior in brushes (Alexander, 1977; de Gennes, 1987).

The natural way to test for possible semi-dilute solution behavior in PEG-lipid structures is to consider PEG under bulk conditions. We argue that flexible end-grafted PEG chains will form semi-dilute solutions only if PEGs of comparable density form semi-dilute bulk solutions. In bulk solutions one may check for the desired property by determining whether the osmotic pressure $`\mathrm{\Pi }`$ is related to the bulk monomer volume fraction $`\varphi `$ in the manner predicted by des Cloizeaux (de Gennes, 1979):

$$\mathrm{\Pi }=\alpha (k_BT/a^3)\varphi ^{9/4},$$
(1)
where $`\alpha `$ is a constant $`𝒪(1)`$. In Fig. 2 we have plotted the room-temperature bulk osmotic pressure as a function of bulk monomer volume fraction for PEG polymers of various molecular weights between 1000 and 20000. The data were obtained from Rand (2002). Additional data consistent with those shown here are also available (Reid and Rand, 1997).

Fig. 2 illustrates three points not previously addressed in studies of bulk PEG osmotic properties, including virial-expansion (Cohen and Highsmith, 1997) and excluded-volume (Reid and Rand, 1997) analyses of PEG osmotic pressures: (i) At high densities, the osmotic pressures of PEGs with molecular weight exceeding $``$1500 Da indeed approach the des Cloizeaux result Eq. 1, if we take $`a=3.5`$ Å (Kenworthy et al., 1995a) and fit $`\alpha =0.8`$. Thus, sufficiently long PEG chains under bulk conditions indeed form semi-dilute solutions. (ii) A crossover from ideal-gas behavior $`\mathrm{\Pi }=(k_BT/a^3)\varphi /N`$ at low volume fractions to des Cloizeaux behavior at high volume fractions takes place at higher concentrations the lower the molecular weight. Moreover, the chain overlap condition $`\varphi \varphi ^{}=N^{4/5}`$ (de Gennes, 1979) does not provide a sufficient criterion for the attainment of des Cloizeaux behavior. (iii) PEG-2000 solutions are in the scaling regime when the volume fraction is larger than $`\varphi _{2000}^\mathrm{\#}0.15`$, rather than the overlap concentration $`\varphi _{2000}^{}=0.05`$. Similarly, in view of the experimental uncertainty, PEG-5000 solutions are not in the scaling regime until the volume fraction is larger than $`\varphi _{5000}^\mathrm{\#}0.070.09`$, rather than $`\varphi _{5000}^{}=0.02`$.

Bulk-solution analysis of PEG data helps us establish whether AdG theory applies to stressed PEG-liposomes (Kuhl et al., 1994; Kenworthy et al., 1995a). Specifically, just before two brush-covered surfaces are brought into first contact, $`\mathrm{\Pi }0`$ and the thickness of the layers is $`LL_0`$. The volume fraction of monomers is therefore $`\overline{\varphi }_0(a/D)^{4/3}`$. If we assume $`a=3.5`$ Å and use the relation $`D(A/f)^{1/2}`$, where $`f`$ is the mol fraction of PEG-lipids and $`A`$ is the area per DSPC lipid $`=48`$ Å2 (Kenworthy et al., 1995a), we find that solutions of DSPC:PEG-2000 reach the critical value $`\varphi _{2000}^\mathrm{\#}=0.15`$ at mol fraction $`f_{2000}^\mathrm{\#}=0.23`$. Similarly, solutions of DSPC:PEG-5000 reach the critical value $`\varphi _{5000}^\mathrm{\#}=0.070.09`$ mol fraction at $`f_{5000}^\mathrm{\#}=0.070.10`$.

In Fig. 3 we display the Avanti DSPC:PEG-5000 OS data reported by Kenworthy et al. (1995a). We focus on the behavior at the highest coverages corresponding nominally to $`f=0.1`$ and $`0.2`$, where bulk analysis leads us to believe that AdG theory may well apply.

According to AdG theory (Alexander, 1977; de Gennes, 1987) (see Appendix) the formation of a brush is a compromise between excluded-volume repulsions, which lead to an osmotic contribution similar to the des Cloizeaux result, and grafting constraints that are responsible for entropic elastic tensions. The expression for the osmotic pressure reflects the difference between these effects:

$$\mathrm{\Pi }(L)=\alpha \frac{k_BT}{D^3}\left[\left(\frac{L_0}{L}\right)^{9/4}\left(\frac{L}{L_0}\right)^{3/4}\right]$$
(2)
where

$$L_0=aN\left(\frac{a}{D}\right)^{2/3}.$$
(3)
We conjecture that $`\alpha =0.8`$ as for bulk PEG solutions (see Eq. 1).

One may test AdG theory by substituting $`D(L_0,a)`$ from Eq. 3 into the expression $`\mathrm{\Pi }(L)`$ in Eq. 2, and performing unconstrained fits with the two free parameters $`a`$ and $`L_0`$. The solid lines in Fig. 3 are the results of such fits. The quality of the procedure is gauged by the degree to which roughly constant and ”reasonable” values of $`a`$ are obtained. We indeed get nearly constant $`a`$’s close to the values cited in the literature (Kenworthy et al., 1995a): $`a_{0.1}=3.56`$ Å and $`a_{0.2}=3.30`$ Å. Taking $`a=3.5`$ Å, the fitted values for the brush thicknesses are $`L_0=105`$ Å for $`f=0.1`$, and $`L_0=109`$ Å for $`f=0.2`$, respectively. The uncompressed brush thickness $`L_0`$ varies as expected: the higher the coverage, the thicker the brush. However, the grafting densities implied by these fits are systematically lower than the nominal values. Assuming, as before, $`fA/D^2`$ with $`A=48`$ Å2, we find $`f_{0.1}=0.07`$ and $`f_{0.2}=0.08`$.

In summary, good fits producing nearly constant (unconstrained) values of $`a`$, with fitted $`f`$’s lower than nominal values but still within the semi-dilute regime ($`f`$’s $`>f_{5000}^\mathrm{\#}`$), indicate that scaling analysis of the PEG-5000 data of Kenworthy et al. is valid and self-consistent. Saturation effects in these dense brushes are indicated by lower than nominal values of $`f`$.

For DSPC:PEG-2000, AdG analysis shows similar saturation effects. In the case of 30 mol % PEG-lipid, fits yield $`f_{0.3}<f_{2000}^\mathrm{\#}`$, thus the monomer density is below the onset of semi-dilute behavior. Therefore in this case the fitting procedure is not self-consistent. AdG theory is even less applicable for smaller mol fractions of PEG-2000 lipids.

DISCUSSION

This paper emphasizes that brush and bulk scaling laws are related and illustrates how this relation yields information about brush formation in PEG-grafted liposomes. On one hand, a scaling analysis of bulk osmotic pressure data for PEGs of various molecular weights establishes criteria stronger than the popular overlap criterion $`D=R_F`$ (Kuhl et al., 1994; Kenworthy et al., 1995a; Belsito et al., 2000) for invoking AdG theory of brush behavior: In order to invoke Eq. 2, it must be established that the polymer size and density in the compressed brush are in a regime where bulk des Cloizeaux scaling applies. Consequently, we are forced to forego AdG analysis for PEG-grafted liposomes containing PEGs of molecular weight 2000 or less. On the other hand, having established that semi-dilute scaling regimes are within reach for long bulk PEG polymers, we are increasingly confident that AdG theory (or improvements thereof - see Footnote 1) is the correct framework for analyzing densely-grafted liposomes containing PEGs of molecular weight greater than $``$2000.

Other experimental studies lend support to the view that long polymers end-grafted to non-adsorbing substrates under good solvent conditions have bulk scaling behavior as predicted by des Cloizeaux, and brush scaling behavior as described by Alexander and de Gennes (Auroy et al., 1991; Taunton et al., 1990). Our analysis illustrates that brush formation with long water-soluble polymers is fundamentally no different than brush formation with synthetic polymers in organic solvent.

The fact that our two-parameter fits to the AdG expression (Eqs. 2 and 3) are of such quality that they lead to unbiased prediction of fairly constant effective monomer lengths $`a3.5`$ Å, in good agreement with structural predictions (Kenworthy et al., 1995a), leads us to conjecture that osmotic-stress (OS) measurements constitute a method for non-trivial, semi-quantitative structure determination of PEG-grafted liposomes. Hitherto few physicochemical methods (Belsito et al., 2000; Montesano et al., 2001) have been invoked to refine estimates of grafting densities beyond nominal values. Additional methods are desireable, not the least because of the technological importance of PEG-grafted liposomes. With OS analysis, seemingly reliable determination of the brush monomer density $`\overline{\varphi }_0`$ is possible, assuming of course that reliable OS data can be obtained in the semi-dilute regime.

Assuming the area per lipid, $`A`$, to be well-determined, the mol fraction of PEG-lipids $`f=f(\overline{\varphi }_0)`$ can be determined too. Several values have been reported for the area per lipid of DSPC (Kenworthy et al., 1995a; Rand and Parsegian, 1989; Lis et al., 1982). Irrespective of which value is used in the calculations, we predict that densely-grafted DPSC:PEG-lipid liposomes are subject to surface saturation effects. For example, for DSPC:PEG-5000 with nominal mol fractions $`0.1`$ and $`0.2`$, the difference between the fitted grafting densities is small. Assuming $`A=48`$ Å2 (Kenworthy et al., 1995a), $`f_{0.1}=0.07`$ and $`f_{0.2}=0.08`$. The origin of such saturation effects is not yet well understood. On theoretical grounds (Hristova and Needham, 1995), one expects that addition of extra PEG-lipids will cause an increase in lateral pressure and a decrease in lipid packing area until formation of non-bilayer structures such as micelles is favored. In PEG-grafted liposomes with dipalmitoylphosphatidylcholine (DPPC) as the host lipid, this mechanism seems to be active (Belsito et al., 2000; Montesano et al., 2001). In DSPC:PEG liposomes below the chain-melting temperature the situation is more complicated. For DSPC:PEG-5000, Kenworthy et al. (1995b) suggest that before micelle formation sets in, a moderate increase in PEG-lipid content is accompanied by a transformation from an $`L_\beta ^{}`$-like phase to an $`L_\beta `$-like phase. Interestingly, the transformation between these phases is argued to set in at mol fractions of PEG-lipid corresponding approximately to the saturation limit calculated here, i.e., $`f_{5000}0.1`$.

CONCLUSIONS

Sufficiently long PEG polymers in bulk solution may form semi-dilute solutions with osmotic properties as foreseen by des Cloizeaux (de Gennes, 1979). Sufficiently dense and thick ”brushes” of PEG-lipids end-grafted to lipid bilayers are therefore expected to behave as confined semi-dilute solutions with a scaling structure as predicted by Alexander and de Gennes (Alexander, 1977; de Gennes, 1987). The approach to bulk semi-dilute behavior is slow for PEGs of molecular weight less than several $`1000`$s. When attached to lipids, those PEGs will form brushes satisfying AdG theory only if they are rather dense with grafting densities exceeding $`f^\mathrm{\#}0.2`$. In practice this condition may be difficult to realize. Of all the data reported in the literature (Kuhl et al., 1994; Kenworthy et al., 1995a) only the osmotic stress data for DSPC:PEG-5000 with nominal grafting densities in excess of $`f^\mathrm{\#}0.10`$ approximately satisfy the AdG theory. Two-parameter unconstrained fits using the AdG prediction for osmotic pressure vs. bilayer separation yield good fits with an effective monomer length $`a3.5`$ Å in agreement with structural predictions. The coverages inferred from the fits are lower than the nominal coverages, an indication of surface saturation effects in PEG-liposomes which are now beginning to be understood. We conjecture that osmotic-stress measurements form the basis for semi-quantitative structure determinations of PEG-grafted-liposome surfaces.

A quantitative characterization of brush scaling behavior and structure relies on a precise identification of semi-diluteness that is more rigorous than the simple, and often-used, chain-overlap criterion, $`DR_F`$.

Acknowledgments

We thank Dr. A. Kenworthy for valuable discussions. One of us (PLH) would like to thank Prof. F. Pincus for valuable comments.

APPENDIX

Isolated, non-compressed brush: (de Gennes, 1987; de Gennes, 1979) In a fully-developed non-compressed brush, chain overlap is so strong that a semi-dilute solution of spatially-constant monomer volume fraction $`\overline{\varphi }_0`$ is formed (however, see Footnote 1). We recall that under semi-dilute solution conditions (i) the relevant degree of freedom is a ”blob” characterized by its size $`\xi (\overline{\varphi }_0)`$ and its free energy $`k_BT`$; (ii) the gas of blobs is non-interacting, but the chains inside a blob interact solely via excluded-volume repulsions so the number of monomers $`g_\xi `$ inside a blob is related to blob size by the Flory relation $`\xi (\overline{\varphi }_0)=ag_\xi ^{3/5}`$, where $`a`$ is the effective monomer length; and (iii) most physical properties become molecular-weight independent.

In non-compressed brushes the blob size is determined by the distance between grafting sites, $`\xi (\overline{\varphi }_0)D`$. At the same time, molecular-weight independence of physical properties in semi-dilute solutions implies that $`g_\xi =g_D\overline{\varphi }_0^{5/4}`$, and $`\xi (\overline{\varphi }_0)a\overline{\varphi }_0^{3/4}`$. It follows that $`\overline{\varphi }_0(a/D)^{4/3}`$. Polymer chains in the brush form strings of blobs. The length of a non-compressed string is the blob size times the number of blobs, i.e., $`L_0D\times (N/g_D)aN(a/D)^{2/3}`$. This well-known linear relation between $`L_0`$ and $`N`$ reflects the strong stretching of chains in a brush and is largely a consequence of semi-dilute solution behavior in the brush.

Compressed brush: It is instructive to view the formation of a brush as a compromise between excluded-volume monomer repulsions, which lead to an osmotic contribution, and confinement effects (due to the grafts) that are responsible for entropic elastic tensions. In the absence of osmotic stress these effects balance each other. When subjected to compression, apposing brushes begin to overlap, the brush thickness $`L`$ decreases, and the monomer density in the brush increases: $`\overline{\varphi }_L=\overline{\varphi }_0\times (L_0/L)`$. The osmotic stress generates an imbalance between osmotic and elastic terms which may be described as compression of a string of blobs. In fact, the resulting osmotic pressure can be derived from the free energy per chain $`F_c=F_{os}+F_e`$, where the osmotic term is $`F_{os}k_BTN\overline{\varphi }_{L}^{}{}_{}{}^{5/4}`$, namely $`k_BT`$ per blob times the number of blobs, as in bulk semi-dilute solutions. The elastic term is a Flory-type entropic elastic free energy for an ideal random walk of blobs, $`F_ek_BTL^2/R^2(\overline{\varphi }_L)`$, with ideal radius squared given by the blob size squared times the number of blobs, $`R^2(\overline{\varphi }_L)=\xi ^2(\overline{\varphi }_L)\times (N/g_L)`$. If we invoke the Alexander conditions $`g_L\overline{\varphi }_L^{5/4}`$ and $`\xi (\overline{\varphi }_L)a\overline{\varphi }_L^{3/4}`$ (the relation $`\xi (\overline{\varphi }_L)D`$ is not valid), the osmotic pressure $`\mathrm{\Pi }=\overline{\varphi }_L^2_{\overline{\varphi }_L}F_c/(Na^3)`$ (de Gennes, 1979) can be derived in the form Eq. 2.

Relation to bulk solution behavior: For free polymer in solution, $`\overline{\varphi }_L\varphi `$, and the free energy contains no elastic restoring term. From the blob expresion $`F_{os}k_BTN\varphi ^{5/4}`$ we readily infer the des Cloizeaux expression Eq. 1 for bulk polymers in the semi-dilute regime. It is important to note that the validity of Eq. 1 for bulk polymers is a necessary condition for the validity of Eq. 2 for the compressed brush. In order to invoke Eq. 2, it must be established that the polymer size and density in the compressed brush are in a regime where bulk des Cloizeaux scaling applies.

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Figure 1: Schematic drawing of two apposed brush layers of surface-grafted PEG polymers in a multilamellar liposome. $`L_0`$ is the unperturbed thickness of the polymer brush, $`d_f`$ is the surface-to-surface distance, $`Ld_f/2`$, and $`D`$ is the distance between grafting sites. Osmotic stress forces the surfaces together, leading to interaction and interpenetration of the brushes such that $`L<L_0`$. $`\xi `$ is the blob size of the polymer. The yellow regions denote the lipid bilayers, and the blue region denotes the aqueous solution in between lamellae of the liposome.

Figure 2: Room-temperature bulk osmotic pressure $`\mathrm{\Pi }`$ of various PEG polymers vs. monomer volume fraction $`\varphi `$. The symbols are data obtained from Rand (2002) for PEGs of molecular weights $`1000,1500,2000,4000,8000,10000`$ and $`20000`$ Da. The monomer volume fraction is $`\varphi 0.59\times w`$, where $`0<w<0.5`$ is the weight fraction of polymer (Rand, 2002). (In obtaining the relation between $`\varphi `$ and $`w`$ we have assumed the specific density of PEG solutions to be $`1`$ g/cm3 (Hasse et al., 1995).) The solid line is the des Cloizeaux equation $`\mathrm{\Pi }=\alpha (k_BT/a^3)\varphi ^{9/4}`$, with $`a=3.5`$ Å (Kenworthy et al., 1995a) and $`\alpha =0.8`$. Note that at high $`\varphi `$ the data converge to a universal straight line independent of molecular weight, in agreement with the des Cloizeaux prediction. For reference, the vertical dashed lines are the molecular-weight-independent monomer volume fractions in an uncompressed brush $`\overline{\varphi }_0=(a/D)^{4/3}`$ for PEG-lipid mol fractions $`f=0.05,0.1,`$ and $`0.2`$ if $`a=3.5`$ Å and $`D=(A/f)^{1/2}`$, where $`A=48`$ Å2 (Kenworthy et al., 1995a). A surface-grafted PEG layer is in the brush scaling regime if its free-polymer bulk $`\mathrm{\Pi }`$ lies on the des Cloizeaux line at the monomer volume-fraction $`\varphi `$ present in the surface layer (vertical dashed lines). Thus, at a 10% grafting density, a PEG-6000 layer is in the brush regime, but a PEG-1500 layer is not. (See text and Appendix for details.)

Figure 3: Osmotic pressure $`\mathrm{\Pi }`$ vs. fluid spacing $`d_f=2L`$ between apposing PEG-grafted bilayers. The symbols are data from Kenworthy et al. (1995a) for Avanti DSPC:PEG-5000 complexes with nominal grafting mol fractions $`f=0,0.015,0.03,0.05,0.1,`$ and $`0.2`$. The solid curves are fits to the $`f=0.1`$ and $`0.2`$ data using Eqs. 2 and 3. Two-parameter unconstrained fits of the AdG prediction for osmotic pressure vs. fluid spacing yield nearly constant effective monomer lengths $`a_{0.1}=3.56\pm 0.07`$ Å and $`a_{0.2}=3.30\pm 0.15`$ Å. These values agree well with structural predictions reported in the literature (Kenworthy et al., 1995a), lending veracity to the applicability of AdG theory to these data. The $`f=0.015,0.03,0.05`$ data do not meet the brush criterion (see Fig. 2) and thus AdG theory is not applicable. (See text for details.)