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# Kinetic pathways of multi-phase surfactant systems

## I Introduction

The study of nonequilibrium phase behaviour in complex fluid systems provides a new challenge. Specifically, in the case of surfactant systems, relaxation to equilibrium has recently attracted interest . For example, this has been studied in phase penetration scan experiments , and in directional growth studies . In these experiments the evolution of a mesophase is followed in the presence of a concentration or temperature gradient respectively. This may result in unstable interfaces which can lead to spectacular instabilities.

The kinetics of phase behaviour has been well studied in other areas of soft matter physics. For example the nucleation behaviour in colloid-polymer mixtures has been investigated experimentally and theoretically . In these systems, three-phase samples consisting of colloidal gas, liquid and crystal, can be prepared at different compositions. In , three-phase samples were homogenised and observed while equilibrating. By identifying the fast and slow composition variables in the system, and then considering the evolving free-energy landscape for the slow component, restrictions can be placed on the kinetic pathway the system will follow as it evolves towards equilibrium. This free-energy landscape theory  promises to be a powerful way to predict kinetic pathways, at least in systems where one combination of the composition variables evolves more slowly than the others, so that time scales can be separated. It is used below (Section IV) to give a possible explanation for the observations in surfactant systems that will be presented here (Section III).

In this paper we investigate the temporal evolution of a two-phase system, comprising sponge ($`L_3`$) and lamellar ($`L_\alpha `$) phase, and a three-phase system, comprising $`L_3`$, $`L_\alpha `$ and micellar ($`L_1`$) phase, in samples that have been subjected to a temperature quench. Using dark-field macroscopy (explained below) we have observed a number of interesting nonequilibrium features that occur as the sample progresses to its new equilibrium state. In the two-phase sample we have observed dense nucleation of lamellar phase droplets within $`L_3`$ which appear to form a ‘gel’ of droplets that compacts over time. In addition, we present microscopic images of the ‘gel’ formation. In three-phase samples we observed three regimes of behaviour. Initially the sponge phase forms an emulsion which proceeds to a homogeneous sponge phase. In the second regime nucleation of lamellar phase in the sponge phase occurs close to the $`L_3`$/$`L_1`$ interface. The growing droplets rise through the $`L_3`$ phase and arrive at the $`L_3`$/$`L_\alpha `$ interface, building up the $`L_\alpha `$ phase over time. Finally a plume pushes through the sponge phase connecting the $`L_1`$ and $`L_\alpha `$. These results are described in Section III and discussed in Section IV. Section V gives a brief conclusion.

## II Experimental Section

### A Materials

SDS and octanol (both $`99\%`$ purity) were supplied by Sigma-Aldrich and used without further purification. Samples were prepared by dissolving SDS and octanol in brine ($`20`$g/l of NaCl in distilled water) and then tumbled for 2 days and subsequently allowed to equilibrate at a higher temperature of $`40^{}\text{C}`$. Experiments were performed after approximately two weeks, when the samples had reached equilibrium.

### B Dark-field macroscopy

Compared to a direct observation, dark-field macroscopy allows us to obtain better contrast from regions in the sample that scatter light only weakly . The scattering of light is caused by refractive index inhomogeneities in the sample which, e.g., result from regions of different concentration. The term macroscopy is introduced since the sample is larger than its image, which matches the size of the CCD chip, and therefore the optical setup is designed to reduce the image size. We have used dark-field macroscopy to observe samples whose cell dimensions are $`4\text{cm}\times 1\text{cm}\times 1\text{cm}`$.

The general layout of the dark-field macroscope is similar to a dark-field microscope and shown in figure 1. A white light source and a collimator are used to produce parallel light to illuminate the sample which is placed in the object plane. The unscattered light is focused into the back focal plane of the objective. A beam stop is placed in this plane to black the unscattered light. In the case of no scattering the image is completely dark, hence the name dark-field. If there is scattered light, it is collimated by the objective and focused onto the CCD chip. Therefore, whenever there are refractive index differences in the sample these will appear as bright spots on a dark background. All samples observed are temperature controlled in a heat bath.

### C Microscopy

All microscopy observations were made using an Olympus BX50 microscope in bright-field mode between crossed polarisers with long working distance objectives. The evolution of the samples were recorded using a CCD camera and time lapse video recorder together with a framegrabber PC. The contrast of the presented images has been enhanced by thresholding. All microscopy experiments were done in a Linkam LTS hot-stage which ensured a controlled and stable temperature.

## III Results

We have studied two phase ($`L_\alpha `$,$`L_3`$) and three-phase ($`L_\alpha `$,$`L_3`$,$`L_1`$) samples upon a large temperature change. Initially the samples are in equilibrium at $`\text{T}=40^{}\text{C}`$ where they have been observed for one week and showed no further change. The sample is then placed in the dark-field macroscope which is kept at a temperature of $`20^{}\text{C}`$. Its behaviour upon this temperature quench is then followed. We have studied samples with different bilayer (SDS + octanol) concentrations and octanol/SDS ratios. We will first present the typical behaviour of two phase and three phase samples, before we describe the dependence on octanol/SDS ratio.

### A Two-phase samples

#### 1 Macroscopic observations

Temperature quench experiments on a two-phase sample ($`L_\alpha `$,$`L_3`$) were performed for an octanol/SDS ratio of 1.36 and a bilayer concentration of $`30\%`$. At this composition and at a temperature of $`40^{}\text{C}`$ the sample has two phases, $`L_\alpha `$ at the top and $`L_3`$ on the bottom, where the $`L_3`$ phase is in abundance ($`95\%`$). At lower temperature ($`\text{T}=20^{}\text{C}`$) most of the volume ($`70\%`$) of the sample is present as $`L_\alpha `$ phase which replaces $`L_3`$ phase.

When the sample is quenched from $`\text{T}=40^{}\text{C}`$ to $`20^{}\text{C}`$, we have observed two regimes of behaviour. Almost immediately, ($`L_3`$ \+ $`L_\alpha `$) nucleates in the $`L_3`$ phase and appears to completely fill the sample (figure 2A). Over time this mixed sponge/lamellar phase decreases in volume and the ’pure’ sponge phase now reforms at the bottom of the sample (figure 2B). As the volume of ($`L_3`$ \+ $`L_\alpha `$) decreases there is a noticeable change in its texture. The lower part is rough in texture and separated by an interface from the top part which has a smooth texture (figure 2C). The rough texture appears to be a gel of $`L_\alpha `$ droplets in $`L_3`$; this is confirmed by microscopy observations (see below). Over time the smooth part grows as the rough part shrinks (figure 2C-D). The final state of the sample (not shown) contains only a smooth lamellar phase in peaceful coexistence with the sponge phase where the two phases occupy comparable volumes of the sample.

The same generic behaviour is observed in samples with octanol/SDS ratios up to 1.44 at 30$`\%`$ bilayer concentration. In figure 3 the relaxation to equilibrium observed with these samples is schematically presented.

#### 2 Microscopic observations

To obtain more detailed information, part of the sponge phase was extracted from a two-phase sample. It was subsequently observed with a microscope during a temperature ramp from $`\text{T}=40^{}\text{C}`$ to $`20^{}\text{C}`$. Droplets of $`L_\alpha `$ phase, which have the birefringent ‘Maltese cross’ signature of multilamellar vesicles or onions, are observed to nucleate homogeneously in the $`L_3`$ phase. These droplets continue to grow to $`1050\mu \text{m}`$ over the next 60 minutes (figures 4A-C). However, after 30 minutes the onions start to move towards each other forming an onion ‘gel’ (figure 4D). This structure coarsens over time leaving voids of pure sponge phase (figure 4E-F). As more onions form in the $`L_3`$ phase they coalesce. The heterogeneity of the gel is presumably responsible for the rough texture reported above.

Figure 5 shows a close-up of two droplets, with Maltese crosses visible, when observed through partially crossed polars. In this case the two droplets have partially merged. On closer inspection these lamellar droplets have a distinctive pattern of focal conic defects that form within the onion (figure 6A). These defects in the onion are presumably due to an epitaxial tilt of the bilayers at the surface of the droplet, which is surrounded by sponge phase. This has also been observed at the interface between a homeotropic lamellar and sponge phase . The epitaxial tilt is required to match the repeat distance in the lamellar phase onto the characteristic bilayer spacing in the sponge (figure 6B). This observation suggest that, at the observed temperature and time scales, the internal structure of each onion is capable of reorganizing to minimize the interfacial energy of the onion.

### B Three-phase samples

Samples within the three-phase region have been observed with $`5\%`$ and $`10\%`$ bilayer concentration over a range of octanol/SDS ratio $`1.22`$ to $`1.32`$. At these compositions and at $`\text{T}=40^{}\text{C}`$, all samples consist of three phases: $`L_\alpha `$ at the top, $`L_3`$ in the middle and $`L_1`$ on the bottom, where the $`L_3`$ phase has the largest volume. At a lower temperature of $`20^{}\text{C}`$ most of the volume is occupied by $`L_\alpha `$ phase with only a small volume of $`L_3`$ phase remaining. The $`L_1`$ phase is observed to have a slightly larger volume at $`\text{T}=20^{}\text{C}`$ than at $`40^{}\text{C}`$. After a temperature quench from $`\text{T}=40^{}\text{C}`$ to $`20^{}\text{C}`$ the relaxation to equilibrium is found to proceed through three regimes. They are described below for a sample that has a bilayer concentration of $`5\%`$ and an octanol/SDS ratio of $`1.22`$. Other three-phase samples behave in a similar fashion, although the time constants were found to depend on the actual composition.

#### 1 Early stages

After the temperature quench, the $`L_3`$ phase becomes turbid as inhomogeneities form within it (figure 7A). This texture appears to be an emulsion of $`L_1`$ droplets separated by $`L_3`$ or vice versa. (see Section IV for a discussion). The texture is first seen close to the $`L_1`$/$`L_3`$ interface, and then spreads up to the $`L_3`$/$`L_\alpha `$ interface while large convection currents are also observed within the $`L_3`$ phase.

In addition some large droplets of $`L_1`$ fall rapidly from the $`L_\alpha `$ phase through the inhomogeneous $`L_3`$ phase into the $`L_1`$ phase (figure 8). These droplets are initially of a diameter of about $`90\mu \text{m}`$ and fall with speed $`1000\mu \text{m}\text{s}^1`$. Within 3 hours their size decreases to $`14\mu \text{m}`$ and their speed is reduced to $`15\mu \text{m}\text{s}^1`$. About one hour later the $`L_3`$ phase becomes homogeneous once again, by a clearing process which starts close to the $`L_3`$/$`L_\alpha `$ interface. A schematic summary of these features is given in figure 9. These features are typical of samples at $`510\%`$ bilayer composition with octanol/SDS ratios $`1.221.32`$.

#### 2 Lamellar nucleation and growth

After about one hour, droplets of $`L_\alpha `$ phase of approximately $`1020\mu \text{m}`$ in size begin to form in the $`L_3`$ phase. The number of $`L_\alpha `$ drops observed increases over the next 30 minutes. While droplets are observed to nucleate throughout the $`L_3`$ phase, this mainly happens near the $`L_1`$/$`L_3`$ interface (figure 10). The droplets move up towards the $`L_\alpha `$ phase with a speed of about 4$`\mu \text{m}\text{s}^1`$, gaining size as they do so. Over a period of $`12`$ days they build the $`L_\alpha `$ phase. The quantity of the $`L_\alpha `$ phase steadily increases, however after 12 hours the number of droplets within $`L_3`$ is observed to have decreased. Eventually after about 36 hours further droplets are not observed to form despite the continuing growth of the lamellar phase. These findings are summarized schematically in Fig. 11.

At larger bilayer concentrations ($`3040\%`$) we have observed a much larger density of lamellar droplets in the $`L_3`$ phase. At a much larger octanol/SDS ratio of 1.35 and 1.41 the droplets that form are very dense. Furthermore, by increasing the octanol/SDS ratio, we have observed a noticeable change in the dynamics. At higher octanol/SDS ratio we observe an increase in the rate of formation of the $`L_\alpha `$ droplets and the speed of the droplets as they move towards the $`L_\alpha `$ phase.

#### 3 The plume

After 36 hours the $`L_\alpha `$ droplets are no longer observed to nucleate in the $`L_3`$ phase. However, the $`L_\alpha `$ phase still continues to grow. Eventually at some later time a plume grows from the $`L_1`$ phase and extends up to the $`L_\alpha `$ phase (figure 12).

Prior to this, in the $`L_1`$ phase small droplets of $`L_\alpha `$ phase are observed to move up towards the $`L_3`$/$`L_1`$ interface and eventually push their way through the $`L_3`$ phase by forming the plume. The plume connects the $`L_1`$ phase to the $`L_\alpha `$ phase cutting straight through the $`L_3`$ phase. It is about $`50100\mu \text{m}`$ in diameter. On the plume near the $`L_1`$/$`L_3`$ interface a large bulbous piece with a diameter of about $`100\mu \text{m}`$ can be observed. We followed the movement of this over the next 12 hours. Initially the bulbous piece rises up toward the $`L_\alpha `$/$`L_3`$ interface (figure 12B-C). Then it begins to move back towards the other interface (figure 12C-E). Eventually the plume detaches from the $`L_3`$/$`L_1`$ interface and the whole plume is ‘pulled’ up into the $`L_\alpha `$ phase (figure 12E-G) while the bulbous bit remains at the loose end of the plume. The only way to describe the motion of the plume is that it behaves in a ‘lava-lamp’ like fashion.

The occurrence of the plume is a reproducible effect and has been seen in many separate experiments. However, in the range of samples we have observed we only find plumes when there is $`L_1`$ phase present. Depending on the composition we can even observe multiple plumes forming. The plumes are observed late in the lamellar nucleation regime. However, at larger octanol/SDS ratios plumes form earlier in the $`L_\alpha `$ nucleation regime. In addition, we have observed streaks in the $`L_3`$ phase at the $`L_\alpha `$ interface, which persist for the remaining duration of the growth of $`L_\alpha `$. They are found during and after the formation of the plume.

#### 4 Octanol/SDS dependence

As already mentioned in section III B 2, a higher octanol/SDS ratio also results in an increase in the rate of formation of the $`L_\alpha `$ droplets and the speed of the droplets as they move towards the $`L_\alpha `$ phase. In addition, the density of droplets is increased upon an increase in the octanol/SDS ratio. By varying the octanol content in the bilayer we influence the time scale of each regime that is observed. The initial regime, where we have observed the transient formation of a sponge emulsion, appears to persist for a shorter period of time as we increase the octanol/SDS ratio.

This is also the case for the second regime of lamellar nucleation and growth. Furthermore the nucleation regime starts earlier for samples with higher octanol content so that these regimes overlap. This is also the case for the observation of the plume which can be observed earlier at higher octanol/SDS ratio. Figure 13 gives a semi-quantitative diagram of these observations.

## IV Discussion

An initially equilibrated sample that is subjected to a sudden temperature change will relax to a new equilibrium state. In three- and two-phase surfactant samples we have observed interesting behaviour as the samples proceed to this final equilibrium state. Below we discuss these observations first for the three- and then for the two-phase samples. This will be followed by some possible explanations for the observed behaviour.

### A Early stages

When the three phase sample is quenched from $`\text{T}=40^{}\text{C}`$ to $`20^{}\text{C}`$ the $`L_1`$ phase volume is found to increase during the early stages. This indicates that during the quench the majority phase, $`L_3`$, increases its bilayer concentration with a concomitant reduction in its bilayer spacing, expelling $`L_1`$. This would explain the formation of a ‘sponge emulsion’, which appears as an inhomogeneous texture (figure 7). A minority of $`L_1`$ phase in sponge phase has previously been observed in other experiments . Furthermore, the subsequent separation of $`L_1`$ and $`L_3`$ phase may lead to the observed convection currents. The sample begins to homogenise again as the compositions reorganise into a more favourable state. The homogenisation of the $`L_3`$ phase is found to start at the $`L_\alpha `$ phase and moves towards the $`L_1`$ phase. This is not surprising, since the $`L_1`$ phase has to drain through the sponge emulsion during the homogenisation process (figure 7).

A similar decrease in bilayer spacing is also expected for the $`L_\alpha `$ phase. Consequently the bilayer concentration will increase and excess brine will be expelled, possibly together with a low concentration of surfactant and cosurfactant. It seems conceivable that this leads to the formation of droplets of $`L_1`$ within $`L_\alpha `$, which are then observed to fall through the $`L_3`$ phase (figure 8). As the equilibrium bilayer concentration is approached, the $`L_1`$ flux is reduced. This is reflected in the reduction of the $`L_1`$ droplet size and consequently leads to a reduction in the speed of the droplets.

By expelling excess brine, both the $`L_3`$ and $`L_\alpha `$ phase increase their bilayer concentration. The decrease in undulation repulsions between layers as a result of the lowered temperature seems likely to be responsible for this behaviour . This change in bilayer concentration occurs during the early stages and appears to be much faster than reorganisation within the bilayer. The slower intra-bilayer reorganisation is thus expected to influence the behaviour during the subsequent stages.

### B Lamellar nucleation and growth

After the early stage described above (and sometimes overlapping with it – see figure 13), lamellar phase is found to nucleate and grow within $`L_3`$ at the expense of sponge phase. One of the most striking features of this process is that the nucleation of the $`L_\alpha `$ phase in the $`L_3`$ phase is not homogeneous throughout the $`L_3`$ phase, but is most abundant close to the $`L_1`$/$`L_3`$ interface. It seems peculiar that such nucleation should occur in the part of the $`L_3`$ region furthest from the existing slab of $`L_\alpha `$ phase. A possible explanation for this can be found by analysing the way the free energy landscape changes after the temperature jump .

First let us consider a three phase sample ($`L_1`$,$`L_3`$,$`L_\alpha `$) at equilibrium. To our knowledge there is no published phase diagram for this system that would show the phase boundaries close to the three-phase region. However, from our experience with these samples we present a schematic phase diagram of this region as a function of the volume fraction of SDS $`\varphi _{\mathrm{SDS}}`$ and octanol $`\varphi _{\mathrm{oct}}`$ (figure 14).

Figure 15 gives a schematic free energy landscape that is consistent with the observed phase diagram of the system. The free energy of the sample in equilibrium is a function of the volume fractions of two independent components, SDS and octanol.

At equilibrium the chemical potentials ($`\mu _{\mathrm{SDS},\mathrm{oct}}=f/\varphi _{\mathrm{SDS},\mathrm{oct}}`$) of each component must be equal in all of the coexisting phases, $`\mu _{\mathrm{SDS},\mathrm{oct}}^{L_1}=\mu _{\mathrm{SDS},\mathrm{oct}}^{L_3}=\mu _{\mathrm{SDS},\mathrm{oct}}^{L_\alpha }`$. The same also applies to the osmotic pressure of each phase. This means that the tangents (shaded plane, Fig. 15) to the free energy ‘wells’ at the equilibrium compositions will all be the same. The points of tangency will correspond to the corners of the three-phase triangle on the phase diagram (figure 14).

Note that this analysis is invariant under arbitrary linear combination of the composition variables. Here we will choose linear combinations $`\varphi _\mathrm{f},\varphi _\mathrm{s}`$ as indicated in figure 14. (These are related to the volume fraction of bilayer and the composition of the bilayer, respectively, as we discuss below.) With these as the densities, the phase diagram looks like figure 16.

Now we ask: How does a three-phase sample (marked in figure 16 by ‘$``$’) change upon a temperature quench? Suppose at a given temperature its composition is close to the $`L_3`$ corner of the three-phase triangle (gray area in figure 16). It thus mainly consists of $`L_3`$, but also contains small amounts of $`L_\alpha `$ and $`L_1`$. Upon a change in temperature the free energy landscape rearranges such that the free energy minima move to new positions. This changes the position of the three phase triangle (dashed lines in figure 16). Although the chemical composition of the sample remains constant, its relative position in the three-phase region is changed. In the case shown, it is now located much closer to the $`L_\alpha `$ corner and also moved towards the $`L_1`$ corner. The sample is thus forced to change its compositions locally and nucleate $`L_\alpha `$ and $`L_1`$ at the expense of $`L_3`$. This is what happens in our three-phase samples when we quench from $`40^{}\text{C}`$ to $`20^{}\text{C}`$.

Following reference , a quasi-equilibrium free energy landscape can be constructed after the temperature quench if fast and slow composition variables can be identified. Application of this free energy landscape analysis to our system depends on the relation between the fast and slow components ($`\varphi _\mathrm{f},\varphi _\mathrm{s}`$) and the volume fractions of octanol ($`\varphi _{\mathrm{oct}}`$) and SDS ($`\varphi _{\mathrm{SDS}}`$). Our observations indicate that changes in bilayer concentration occur during the early stages and can thus be identified with the fast component. In contrast, changes in the organisation of the bilayer such as the transition from $`L_3`$ to $`L_\alpha `$ are found to happen later. From the phase diagram (figure 14) it is clear that this $`L_3`$-$`L_\alpha `$ transition must involve changes in the bilayer composition (at nearly constant bilayer fraction). This is also supported by our separate observations of contact experiments between lamellar phase and water, where myelin patterns form .

Immediately after contact the myelin formation is always observed before the formation of any other intermediate phase, such as $`L_3`$ phase. Thus the time for bilayers to swell to the miscibility gap is faster than the formation of sponge phase which requires local reorganisation in the bilayer structure, and also a change in its composition.

We therefore assume that, starting from a given initial state, changes in volume fraction of the fast component $`\varphi _\mathrm{f}`$ correspond to changes in total bilayer concentration at fixed SDS/octanol ratio. (This is expected to be a fast, ‘collective diffusion’ mode.) We also assume that the slow component corresponds to changes in SDS/octanol ratio at roughly fixed bilayer volume fraction. This second assumption is physically reasonable, but less obvious: formally, the fast and slow directions are eigenvectors of a diffusion matrix, which need not be symmetric, and they need not be at rightangles. However, if we make both assumptions, the fast and slow direction correspond to radial and tangential directions in figure 14, which is probably a good enough approximation for the present discussion. For a state near the $`L_3`$ corner initially, these are as indicated in the figure.

For the fast component, the chemical potential $`\mu _\mathrm{f}=\frac{f}{\varphi _\mathrm{f}}`$ will become uniform rapidly. Essentially, we move to an equilibrium state through a sequence of metastable states, for which the chemical potential of the fast component $`\mu _\mathrm{f}`$ is uniform. However, the value of $`\mu _\mathrm{f}`$ is evolving in time and depends on the (nonuniform) evolution of the slow variable $`\varphi _\mathrm{s}`$. Instead of drawing the free energy landscape as a function of two components (figure 15) we now concentrate on the slow variable $`\varphi _\mathrm{s}`$ only. (This defines a free energy $`f(\varphi _\mathrm{s},\mu _\mathrm{f})`$, as a function of $`\varphi _\mathrm{s}`$ in a semi-grand ensemble, under conditions of uniform, but time dependent, $`\mu _\mathrm{f}`$.) Figure 17A shows the initial (equilibrium) free energy landscape at high temperature as a function of the slow composition variable. After a temperature quench the three minima do not have a common tangent (figure 17B) since $`\mu _\mathrm{f}`$ has not yet relaxed to its equilibrium value and the initial condition now represents a metastable state. In this diagram we may assume that the free energy curve of $`L_3`$ phase lies higher than the common tangent of the other two so as to favour producing more $`L_1`$ and $`L_\alpha `$ phase. (If the free energy minimum of $`L_3`$ phase is below the tangent of the other two then no nucleation will occur. In fact, this would be the case where the change in phase diagram is in the opposite direction to the one shown in figure 16.) Once the sample reaches equilibrium at the lower temperature, the three minima again have a common tangent (a situation similar to figure 17A is recovered).

The local composition of the phases near their interfaces with one another can be determined from the metastable common tangents to the free energy landscape (figure 17B); the compositions at each end of a tangent have the same chemical potential $`\mu _\mathrm{s}`$ of the slow component which is the condition for local equilibrium of the interface. From these tangents, the local composition of the $`L_3`$ phase near to its interfaces can be determined. The $`L_3`$ phase will reorganise to have two different compositions, $`\varphi _\mathrm{s}=\varphi _1`$ near the $`L_\alpha `$/$`L_3`$ (upper) interface and $`\varphi _\mathrm{s}=\varphi _2`$ near the $`L_3`$/$`L_1`$ (lower) interface. The $`L_3`$ phase thus has a higher bilayer volume fraction nearer the $`L_3`$/$`L_1`$ interface. The resulting composition profile as a function of sample height $`z`$ is shown in figure 18. Since the nucleation of the phases $`L_\alpha `$ and $`L_1`$ will be induced by composition fluctuations in $`L_3`$ phase, $`L_\alpha `$ is more likely to nucleate close to the $`L_3`$/$`L_1`$ interface with its higher volume fraction. The difference in concentrations at the two interfaces requires a concentration gradient across the $`L_3`$ phase. Since $`\varphi _1<\varphi _2`$ then the upper part of the phase has higher mass density than the lower part. (This could cause the system to become unstable under gravity.) The concentration gradient as well as gravity favours driving the $`L_\alpha `$ droplets up towards the $`L_\alpha `$ phase.

Note that these features directly depend on the presence of the $`L_1`$ phase which fixes $`\varphi _\mathrm{s}=\varphi _2`$ at the bottom of the sponge phase. Also, the inversion of the concentration profile predicted by this model follows directly from the fact that the homogeneous $`L_3`$ region in the initial state is metastable: its common tangents to $`L_1`$ and $`L_\alpha `$ cross each other (figure 17B).

### C The plume

The formation of a plume which extends from the $`L_1`$/$`L_3`$ interface into the $`L_\alpha `$ phase appears to result from the nucleation of lamellar phase in the $`L_1`$ phase. The formed lamellar phase might build up at the $`L_1`$/$`L_3`$ interface, because the density difference between $`L_\alpha `$ and $`L_3`$ is very small and the surface tension between $`L_\alpha `$ and $`L_3`$ is large. Eventually the $`L_\alpha `$ phase formed in the $`L_1`$ phase pushes through the sponge phase in a ‘lava-lamp’ like fashion.

### D Comparison of two- and three-phase samples

The absence of the $`L_1`$ phase leads to a clearly different relaxation behaviour of the two-phase samples, although for both kinds of samples the main change upon a temperature quench from $`\text{T}=40^{}\text{C}`$ to $`20^{}\text{C}`$ is the formation of $`L_\alpha `$ at the expense of $`L_3`$ phase. There is no indication for the formation of a (metastable) $`L_1`$ phase within the $`L_\alpha `$ or $`L_3`$ phase during the early stages as observed for the three-phase samples. This could, however, be due to the large octanol/SDS ratio of the two-phase samples, which leads to an overlap of the early stages and the lamellar nucleation in the case of the three phase sample (figure 13) and could mask the (intermediate) formation of $`L_1`$.

In the case of the two-phase samples, the nucleation of $`L_\alpha `$ occurs homogeneously throughout all of the $`L_3`$ phase. Since only one interface ($`L_\alpha `$/$`L_3`$) is present, the $`L_3`$ phase cannot develop a density inversion which could influence the local nucleation rate. The quantity of nucleating $`L_\alpha `$ is large due to the relatively high bilayer concentration ($`30\%`$). The nucleated $`L_\alpha `$ droplets (onions) appear to form a dense network in the $`L_3`$ phase (figure 4), similar to a colloidal gel structure. This is followed by a compaction process, which could be viewed as the drainage and collapse of a ‘gel’ of $`L_\alpha `$ droplets in the $`L_3`$ phase. (For analogous phenomena in colloids see .) Due to the lower mass density of the $`L_\alpha `$ phase, the onion ‘gel’ collapses towards the upper phase boundary of the $`L_3`$ phase. This results in the observed smooth texture above the still uncompacted onion gel in the $`L_3`$ phase with its rough texture (figures 2 and 3). This is reminiscent of the creaming of emulsions. The final equilibrium state of the two-phase samples consists of a completely compacted lamellar phase and ‘pure’ $`L_3`$ phase. Since there is no $`L_1`$ phase present, it is no surprise that the plume has not been observed in two-phase samples.

### E Other features

We have performed a small number of experiments in which the temperature quench was reversed before the reorganization of the phases was complete. During an increase in temperature, we have observed smectic bubbles in the $`L_3`$ phase. These are $`L_\alpha `$ films which contain focal conic defects (figure 19). Each bubble once contained a lamellar onion droplet suspended in the $`L_3`$ phase. On raising the temperature, the central region melts and we observe changes in the birefringence of the bubble.

Eventually the bubble rapidly shrinks down into a small lamellar droplet (figure 20). In some cases we observe the bubble to rapidly collapse and then completely vanish after it bursts. The kinetic behaviour of such processes remains to be fully investigated.

## V Conclusion

Temperature quench experiments in surfactant systems have led to a variety of interesting observations. In the initial stages after the temperature quench, disruption of the $`L_3`$ phase occurs and $`L_1`$ droplets are found to move from the $`L_\alpha `$ through the $`L_3`$ to the $`L_1`$ phase. This is attributed to a sudden reduction in the bilayer concentration which causes the $`L_3`$ and $`L_\alpha `$ phase to expel solvent forming a ‘sponge emulsion’, and a suspension of $`L_1`$ droplets, respectively. This is only observed in the first few hours after the quench. After this rapid equilibration of the bilayer concentration, we observe the formation of lamellar droplets in the sponge phase close to the $`L_1`$/$`L_3`$ interface. This observation can be explained in terms of the evolution through a free energy landscape. As the system proceeds to equilibrium it goes through a series of metastable states. Under such conditions the bilayer concentration at the $`L_1`$/$`L_3`$ interface can be larger than at the $`L_\alpha `$/$`L_3`$ interface. In this case the sponge phase is more likely to nucleate lamellar phase droplets close to the micellar/sponge interface. However until we can directly probe the density of the sponge phase as a function of sample height during this process this explanation remains speculative, and the inverted density profile of figure 18 remains a conjecture.

At a later stage we observe a plume to form at the $`L_1`$/$`L_3`$ interface which connects up to the $`L_\alpha `$ phase. This may be due to the nucleation of lamellar phase droplets in the micellar phase, $`L_1`$ which get ‘stuck’ when they reach the sponge phase interface. If the surface tension of the $`L_\alpha `$/$`L_3`$ interface is large then the lamellar phase will build up until there is enough to break through. The break through is driven by gravity as in a lava-lamp.

In two-phase samples which were prepared at a larger bilayer concentration we have observed different features. The absence of the third phase ($`L_1`$) means we do not observe the nucleation at the bottom of the cell or the formation of the plume. This gives weight to the free-energy landscape explanation of the nucleation kinetics.

## Acknowledgements

We are grateful to P. Garrett, D. Roux, J. Leng, G. Tiddy, J. Walsh and P. Warren for useful discussions. LS thanks the Institute of Food Research for a CASE award. MB thanks Unilever PLC and EPSRC (UK) for a CASE award. Work funded in part under EPSRC Grant GR/K59606.


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# Electric field induced strong localization of electrons on solid hydrogen surface: possible applications to quantum computing

\[

## Abstract

Two-dimensional electron system on the liquid helium surface is one of the leading candidates for constructing large analog quantum computers (P.M. Platzman and M.I. Dykman, Science 284, 1967 (1999)). Similar electron systems on the surfaces of solid hydrogen or solid neon may have some important advantages with respect to electrons on liquid helium in quantum computing applications, such as larger state separation $`\mathrm{\Delta }E`$, absence of propagating capillary waves (or ripplons), smaller vapor pressure, etc. As a result, it may operate at higher temperatures. Surface roughness is the main hurdle to overcome in building a realistic quantum computer using these states. Electric field induced strong localization of surface electrons is shown to be a convenient tool to characterize surface roughness.

PACS no.: 73.20.Fz; 73.20.Dx; 03.67.Lx

\]

Quantum computers may provide an enormous gain in the computation rate due to high parallelism of multi-qubit quantum evolution . They are viewed as a system of N two-level interacting quantum systems (qubits) that evolve in time under the action of some time-dependent Hamiltonian (computer program). The computer operation is based on a controlled series of qubit couplings together with one-qubit rotations.

Two-dimensional electron system on the liquid helium surface is one of the leading candidates for constructing large analog quantum computers . It consists of a set of electrons $`N10^9`$ trapped in vacuum in the image states on the surface of a liquid helium film. The ground and the first excited state of an electron in the image potential may represent 0 and 1 state of a qubit. The electron states (qubits) and electron-electron interactions can be easily manipulated by external electric fields and resonant microwave radiation. On the other hand, these electrons are sufficiently isolated from the outside world: they are coupled to it only through the irregularities of the helium film, such as capillary waves and the substrate defects, and through the collisions with vapor molecules. Thus, these two-dimensional electron systems can behave as quantum computers with many qubits. Unfortunately, the operation temperature of such a computer must be below $`10^2K`$  which is caused by small quantum state separation $`\mathrm{\Delta }E8K`$, thermal excitation of propagating capillary waves (or ripplons) on the liquid He surface, large He vapor pressure at higher temperatures, etc.

In this Letter we are going to show that similar two-dimensional electron systems on the surfaces of solid hydrogen or neon may have some important advantages with respect to electrons on liquid helium in quantum computing applications. Since surface roughness is the main hurdle to overcome in building a realistic quantum computer using these states, it is very important to develop reliable tools for its characterization. Electric field induced strong localization of electrons on solid hydrogen surface observed in the experiment is suggested as such a reliable tool to characterize roughness of solid hydrogen or solid neon surface.

Most of the experimental and theoretical work on two-dimensional electron states above the dielectric surfaces with $`(ϵ1)<<1`$ has been done for the case of liquid helium . In the simplest model, the interaction potential $`\varphi `$ for an electron near the surface of such a dielectric depends only on the electrostatic image force, and on the external electric field $`E`$, which is normal to the surface and is necessary for the electron confinement near the surface:

$$\varphi (z)=e^2(ϵ1)/(4z(ϵ+1))+eEz=Qe^2/z+eEz$$
(1)
for $`z>0`$, and $`\varphi (z)=V_0`$ for $`z<0`$, where the z axis is normal to the surface, and $`V_0`$ is the surface potential barrier. If $`V_0\mathrm{}`$ one obtains the electron energy spectrum:

$$E_n=Q^2me^4/(2\mathrm{}^2n^2)+eE<z_n>+p^2/(2m)$$
(2)
The first term in this expression gives the exact solution for $`E=0`$. The second term is the first-order correction for a non-zero confining field, where the average distance of electrons from the surface in the $`n`$th energy level is $`<z_n>=3n^2\mathrm{}^2/(2me^2Q)`$. This correction provides an extremely convenient way of fine-tuning the energy spectrum with electric signals. In  it was proposed to use patterned electrodes to adjust separately the field $`E`$ acting on each electron (qubit), so that one can address each qubit with a correctly chosen frequency of a microwave driving field. The maximum density of electrons on the dielectric surface is determined by the average external confining field: $`nE/(4\pi e)`$ . Density values of the order of $`10^9`$ cm<sup>-2</sup> are routinely observed which correspond to a reasonable (from the point of view of current state of lithographical techniques) $`300`$ nm spacing between individual electrons (and, hence, individual electrodes necessary to address each of the electrons separately). The last term in (2) corresponds to free electron’s motion parallel to the surface.

Similar two-dimensional electron layers have been observed on the surface of liquid and solid hydrogen and neon . Resonant absorption of light for $`12`$ and $`13`$ transitions in the spectrum of electrons levitating above the surfaces of solid hydrogen and neon has been reported and the frequencies of these transitions have been measured as a function of the confining electric field . Because of approximately three times larger values of $`Q`$ for solid hydrogen and neon, the electrons levitate closer (at a distance of $`25\AA `$) to the surface and have an order of magnitude larger separation $`\mathrm{\Delta }E`$ between quantum energy states. Nevertheless, like electrons on liquid helium surface, they have pretty high mobility $`\mu 10^4cm^2/Vs`$  limited by surface roughness. Coupling to surface roughness ($`H_{sr}=eE\delta `$, where $`\delta `$ represents the surface height variations) is supposed to determine the relaxation time $`T`$ from the n=2 to n=1 state for a moving electron. It is essential to keep $`T`$ as large as possible for a successful operation of a quantum computer. Although the photoresonance linewidth ($`\mathrm{\Delta }\nu 3\times 10^{10}`$ Hz) measured in  is not sufficiently narrow for quantum computer operation, it was most probably caused by inhomogeneous broadening due to variations in height of the samples and crystal orientation. Simple estimate of a homogeneous line width for electrons on atomically flat crystal surface gives six orders of magnitude smaller linewidth of $`\mathrm{\Delta }\nu \omega _{12}^3d_{12}^2/(3\mathrm{}c^3)10^4`$ Hz, where $`\omega _{12}`$ and $`d_{12}`$ are the frequency and the average dipole moment of the $`12`$ transition. This value is just slightly larger than the value expected for electrons on liquid helium surface. Thus, ability to grow high quality atomically flat surfaces of solid hydrogen or solid neon would be of critical importance for building a quantum computer using surface electron states. Most of the other properties of electron systems on solid hydrogen and neon give them substantial advantages with respect to electrons on liquid helium in quantum computing applications. Larger separation $`\mathrm{\Delta }E`$ between the energy states, much smaller vapor pressure at low temperatures, and the absence of propagating capillary waves (or ripplons) may allow a quantum computer operation at sufficiently higher temperatures around 4K. This would make a quantum computer based on surface electron states much more feasible from the technological point of view.

Surface electrons have been previously suggested as a tool to characterize surface roughness of solid hydrogen films prepared by quench condensation on a glass substrate at 1.5K . Surface electron conductivity has been studied as a function of temperature, and thermal-activation-type dependencies have been observed for the ”very rough” samples obtained. The measured activation energy of the order of 10K or more has been suggested as an indicator of surface quality of the hydrogen samples used. This method may not be appropriate for higher quality samples since surface roughness may itself be a function of temperature in the state of thermal equilibrium. The idea of alternative isothermic surface roughness measurements based on Anderson localization is illustrated in Fig.1. Variation of external confining field $`E`$ applied to an electron localized in the ground state over a rough hydrogen surface leads to linear variations in the random potential relief ($`H_{sr}=eE\delta (x,y)`$) seeing by the electron in its lateral motion. For a lateral roughness scale smaller than the electron wavelength ($`\lambda =2\pi \mathrm{}/(2mkT)^{1/2}40`$ nm at T=10K) we may expect a classic case of Anderson localization  at a sufficiently high confining field strength.

According to the measurements of electron mobility on high quality crystals of solid hydrogen , at 13.4K the main contributions to surface electron scattering come from the collisions with hydrogen molecules in the vapor phase, and from the collisions with surface defects. The value of the electron mobility $`\mu =7500cm^2/Vs`$ measured at 13.4K is above the ”minimal metallic mobility” value $`\mu _{min}`$ that corresponds to the electron free propagation length $`l`$ of the order of the electron wavelength $`\lambda `$: the electron mobility may be written as

$$\mu =e\tau /m=\frac{\pi e\mathrm{}}{mkT}\frac{l}{\lambda }$$
(3)
where $`\tau `$ is the free propagation time. At $`l/\lambda 1`$ and T=13.4K the minimal metallic mobility value is equal to $`\mu _{min}3100cm^2/Vs`$. These numbers show that although the surface electrons are supposed to have the diffusive type of conductivity, they are not far from strong localization. Increase in scattering by the surface defects due to application of higher confining electric field should cause such a localization.

An exponential drop in surface electron conductivity under the applied confining electric field has been indeed observed in the experiment. The method of conductivity measurements has been discussed in detail in . A 1.0 mm thick solid hydrogen crystal was grown on the polished sapphire substrate from the liquid hydrogen phase at the triple point. A two-dimensional electron layer levitating above the hydrogen crystal surface was created at a temperature of 13.4K by a pulse of electric current through a tungsten filament located above the crystal. Two electrodes separated by 2.3 mm produced a uniform confining electric field perpendicular to the crystal surface. The upper electrode was grounded. The lower (aluminum) electrode was deposited on the sapphire by vacuum sputtering. The electrodes were 30 mm in diameter and were large enough so that the fringe fields could be neglected near the center of the hydrogen surface. The lower electrode was separated by a narrow gap into two parts that were connected in parallel to a superconducting LC circuit with a resonant frequency of 94 kHz. Appearance of an electron layer on the hydrogen surface led to a decrease of the LC circuit’s Q-factor (initially equaled to $`Q1000`$), and to the decrease of the output signal proportional to the non-resonant radio-frequency absorption of the electron layer. The absorption of the electron layer (proportional to its conductivity which is determined by the electrons density and the mobility of individual electrons in the layer) was recorded while scanning the potential of the lower electrode (see Fig.2). Electrons completely charged the hydrogen surface at point (1) when the pulse of current through the filament occurred. The data obtained on the way from the point (1) to points (2), (4), and (6) correspond to irreversible escape of the electrons from the surface with the electron density determined by $`n=E/(4\pi e)`$. The drop in absorption upon the confining field increase on the way from (2) to (3), or from (4) to (5) was reversible with the average surface electron density unchanged over the duration of the measurements. This drop in absorption is mainly caused by the increase in the electron scattering by surface defects due to larger scattering cross-sections of the topographical defects at larger confining electric fields. In principle, some electron redistribution over the crystal surface may also happen, although this effect is supposed to be small in the geometry of the experiment. The surface area covered by electrons may only change by a few percents due to the fact that the horizontal component of the confining field exists only near the edges of the closely spaced top and bottom electrodes (and in the narrow gap between the electrodes and the walls of the experimental chamber). Moreover, such a redistribution of electrons would cause an opposite effect on the absorption signal due to an increase in the electron density.

Thus, a signal proportional to the electron mobility was measured as a function of the confining electric field. While the behavior of electron absorption on the way (4-5) clearly exhibits evidences of strong localization, the measurements (2-3) performed at higher electron density do not show any sign of localization within the measurements range. This behavior may be attributed to the two-dimensional screening of the lateral potential relief by the conductive electron layer. According to , the screening parameter of a non-degenerate 2D electron gas equals to $`S=2\pi e^2n/(kT)`$, which gives the values of $`S_{45}^1=36`$ nm and $`S_{23}^1=8`$ nm for the electron densities of $`n_{45}=3.6\times 10^8cm^2`$ and $`n_{23}=1.6\times 10^9cm^2`$ in the measurements (4-5) and (2-3) respectively. It seems reasonable to assume that the screening would strongly affect the character of electron’s conductivity when the screening length becomes comparable to the characteristic size of surface defects. Thus, the numbers obtained for the screening length indicate the characteristic lateral size (in the 8 - 36 nm range) of the surface roughness seen by the electrons. The fact that this lateral size is smaller than the electron’s wavelength justifies the applicability of the Anderson localization model to our experimental situation.

The data of the transport measurements were also supported by the simultaneous measurements of photoresonance $`12`$ transition in the electron spectrum (2). These data are presented in Fig.2(b,c). The optical signal proportional to the derivative of the optical absorption at $`\lambda =84.3\mu m`$ was measured using 50V modulation of the bottom electrode potential. A substantial asymmetric photoresonance line broadening can be seen as a direct result of Anderson localization. This is a natural result since each localized electron is supposed to see different local topographical environment.

Fig.3 represents the data obtained in the measurements (4-5) plotted as a logarithm of electrons mobility versus confining electric field $`E`$. These data clearly show the transition from the diffusive to the activation-type of conductivity of the surface electron layer ($`\sigma exp(E_c/kT)`$), with the conductivity threshold $`E_c`$ that depends linearly on the confining field. This linear dependence is exactly the behavior one would expect from the model shown in Fig.1. Thus, the average height variation of the hydrogen surface may be recovered as $`\delta =\frac{kT}{e}\frac{d(ln\mu )}{dE}16`$ nm. The developed technique may be used in the growth and characterization of higher quality crystals of hydrogen and neon that is necessary in quantum computing applications. The confining field strength necessary to induce strong localization may serve as a convenient indicator of surface quality.

The observed electric field induced Anderson localization may also be treated as a simple example of qubit coupling and de- coupling using external electric signals, which is also very important from the point of view of building a large quantum computer. The degree of overlap of the electrons wave functions may be conveniently adjusted by modifying the confining electric field.

In conclusion, it was pointed out that two-dimensional electron systems on the surfaces of solid hydrogen or solid neon may have some important advantages with respect to electrons on liquid helium in quantum computing applications. Such quantum computers may be operational at higher temperatures around 4K if a sufficient smoothness of solid hydrogen or solid neon surfaces may be achieved. Electric field induced strong localization of surface electrons is shown to be a reliable tool to characterize surface roughness.


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# FERMION DAMPING RATE EFFECTS IN COLD DENSE MATTER 11footnote 1Talk given at “Strong and Electroweak Matter 2000”, Marseille, June 2000. 22footnote 2CERN-TH/2000-277

## 1 Introduction

There is an increasing interest in studying how matter behaves at very high density. While high density effects in non-relativistic systems have been studied thoroughly in the past, the same does not hold true for relativistic ultradegenerate plasmas. Relativistic effects cannot be avoided if the chemical potential $`\mu `$ of the system is much larger than the mass of the particles that form the medium. This situation certainly occurs in the interior of neutron stars. The astrophysical scenario is the natural domain of application of the physics of ultradegenerate relativistic plasmas.

Electromagnetic plasmas behave in a drastically different way in their non-relativistic and ultrarelativistic limits. This is so because the magnetic interactions are suppressed in the non-relativistic limit by powers of $`v^2/c^2`$, where $`v`$ is the typical velocity of the particles in the plasma, and $`c`$ is the velocity of light. Electric and magnetic interactions behave in a very different way in a plasma. In the medium, static electric fields are completely screened. This is the well-known Debye screening phenomenon, also known as Thomas-Fermi screening for ultradegenerate plasmas. But magnetic interactions are only weakly dynamically screened, through Landau damping. Thus, while electric interactions are short-ranged, magnetic interactions are long-ranged. This fact has several relevant consequences for ultradegenerate plasmas and makes the relativistic and non-relativistic phases of the plasma to look completely different.

In this talk we will discuss how the long-range character of magnetic interactions affects the lifetime of a quasiparticle in the medium. This is based on work done in collaboration with Michel Le Bellac . We will then see how the fermion lifetime effects also correct the value of the gap of color superconductivity .

## 2 Lifetime of a quasiparticle and non-Fermi liquid behavior of the relativistic plasmas

One of the central concepts in a plasma is that of a quasiparticle. A particle immersed in a medium modifies its propagation properties by interacting with the surrounding medium. In field theoretical language, we would say that the particle is “dressed” by a self-energy cloud. In the ultradegenerate plasma, the relevant degrees of freedom are those of quasiparticles or quasiholes (absences of particles in the Fermi sea) living close to the Fermi surface. Because of the exclusion principle, quasiparticles/quasiholes can only live if they are outside/inside the Fermi sea. These excitations tend to lower their energy by undergoing collisions with the particles in the Fermi sea. They decay, and thus have a finite lifetime. The concept of quasiparticle, however, only makes sense if its lifetime is long enough, or in other words, if its damping rate is much smaller than its energy.

If the interactions in the system are repulsive and short-ranged, some of the propagation properties of the quasiparticles can be deduced on general grounds. In that case, Luttinger’s theorem  states the energy dependence of the damping rate of a quasiparticle that lives close to the Fermi surface. The damping rate can be obtained either by computing the imaginary part of the fermion self-energy or, alternatively, by computing the decay rate

$`\mathrm{\Gamma }(E)`$ $`=`$ $`{\displaystyle \frac{1}{E}}{\displaystyle \frac{\mathrm{d}^3p^{}}{(2\pi )^3}\frac{\left(1\mathrm{\Theta }(\mu E_p^{})\right)}{2E_p^{}}\frac{\mathrm{d}^3k}{(2\pi )^3}\frac{\mathrm{\Theta }(\mu E_k)}{2E_k}}`$
$`\times `$ $`{\displaystyle \frac{\mathrm{d}^3k^{}}{(2\pi )^3}\frac{\left(1\mathrm{\Theta }(\mu E_k^{})\right)}{2E_k^{}}(2\pi )^4\delta ^{(4)}(P+KP^{}K^{})||^2},`$
where $`||^2`$ is the scattering matrix element squared, and $`\mathrm{\Theta }`$ is the step function. The above decay rate represents the interaction of the quasiparticle with one fermion inside the Fermi sea with energy $`E_k`$. As a result, two new particles appear, with energies $`E_k^{}`$ and $`E_p^{}`$, which are outside the Fermi sea. If the interaction is repulsive and short-ranged, and for $`E\mu \mu `$, one can take $`||^2`$ with the value of the fermion energies at $`\mu `$. Then, one can deduce that $`\mathrm{\Gamma }(E)(E\mu )^2`$, only using the phase-space restrictions of fermion-fermion scattering.

The damping rate can also be obtained from the imaginary part of the fermion self-energy, and the computation agrees with that obtained from Eq. (2). Since the real and imaginary parts of the self-energy corrections are related by dispersion relations, Luttinger’s theorem implies that the leading order behavior of the real part of the self-energy is $`|E\mu |`$. For weakly coupled systems, the dispersion relations of the quasiparticles (or quasiholes) are not drastically affected by medium effects.

For systems with long-range interactions, it is not possible to make the previous general statements, as in general the integral in Eq. (2) will depend on the form of the interaction, and in general, Luttinger’s theorem will be violated. This is actually what happens in relativistic QED plasmas, due to the long-range character of the magnetic interactions. A closer look into the decay rate Eq. (2) in a relativistic plasma shows that it is dominated by scattering in the forward or collinear direction, mediated by a soft Landau damped magnetic photon. The momentum of the photon in the process is space-like, so the fermion damping rate would vanish in the absence of Landau damping. In particular, one finds

$$\mathrm{Im}\mathrm{\Sigma }_+(E,p)\frac{e^2}{24\pi }|E\mu |,$$
(2)
where $`e`$ is the electromagnetic coupling constant. The real part of the self-energy can be computed from the imaginary part, using a dispersion relation. One then finds

$$\mathrm{Re}\mathrm{\Sigma }_+(E,p)\frac{e^2}{12\pi ^2}(E\mu )\mathrm{ln}\frac{M}{|E\mu |}+𝒪((E\mu )).$$
(3)
The wavefunction renormalization factor $`Z`$ can then be equally computed from the above values. One finds

$$Z^11\frac{e^2}{12\pi ^2}\mathrm{ln}\frac{M}{|E\mu |}.$$
(4)
Thus, in the limit $`E\mu `$, the fermion propagator vanishes, instead of showing the typical step discontinuity associated to the existence of a Fermi surface . This is an anomalous behavior for a typical Fermi liquid. Its origin is the long-range character of the magnetic interactions in the relativistic system.

## 3 Color superconductivity at weak coupling

QCD at very high baryonic density behaves as a color superconductor . This is a consequence of Cooper’s theorem, as any attractive interaction occurring close to the Fermi surface makes the system unstable to the formation of particle pairing. In QCD the attractive interaction is provided by one-gluon exchange in a color antisymmetric $`\overline{3}`$ channel.

In the weak coupling limit the value of the gap can be computed in perturbation theory. The condensation process is dominated by the exchange of very soft magnetic gluons, which are dynamically screened by Landau damping. The Meissner effect is a subleading effect in the gap equation. At leading order, one finds

$$\varphi _02\frac{b_0}{g^5}\mu \mathrm{exp}\left(\frac{3\pi ^2}{\sqrt{2}g}\right)\left[1+𝒪(g)\right],b_0=256\pi ^4(\frac{2}{N_f})^{5/2}b_0^{},$$
(5)
where $`g`$ is the gauge coupling constant, $`N_f`$ is the number of quark flavors, and $`b_0^{}`$ is a constant of order one. The dependence on the coupling constant of the gap is quite different from the one that arises in a system with short-range interactions.

It is possible to compute next to leading order corrections to Eq. (5) by introducing one-loop corrections in the quark propagators of the gap equation. Here, we will mainly concentrate on studying how the quark damping rate affects the value of the gap close to the Fermi surface. At leading order one finds a modified gap equation

$$\varphi _k=\frac{g^2}{36\pi ^2}_0^{\mathrm{}}d(q\mu )\left[\mathrm{ln}\left(\frac{\mu ^2b^2}{|ϵ_q^2ϵ_k^2|}\right)\right]\frac{\varphi _q}{ϵ_q}\frac{2}{\pi }\mathrm{arctan}\left(\frac{ϵ_q}{\mathrm{\Gamma }_q}\right),$$
(6)
where $`b=b_0/g^5`$, $`ϵ_q=\sqrt{(q\mu )^2+\varphi _q^2}`$, and $`\mathrm{\Gamma }_q`$ is the quark damping rate. The most relevant effect of the damping rate is introducing a physical ultraviolet cutoff in the gap equation: when the ratio $`ϵ_q/\mathrm{\Gamma }_q`$ starts to be small, the integrand in Eq. (6) tends to zero. This situation actually occurs for quarks that are far away from the Fermi surface. As expected, the condensation process only occurs close to the Fermi surface.

For a leading order computation of the gap at the Fermi surface one can take the value of $`\mathrm{\Gamma }_q`$ in the normal phase of the system (that is, using Eq. (2), replacing $`e^2`$ by $`\frac{4}{3}g^2`$). This is so because the one-loop fermion self-energy in the normal phase differs from that in the superconducting phase by, at most, values of the order of the squared of the condensate. Also, the Meissner effect in the gluon propagator to arrive at the value of $`\mathrm{\Gamma }_q`$ is a subleading effect. The dominant scattering processes are those occurring in the forward direction, and these processes are dominated by soft Landau-damped color magnetic interactions, exactly as it happens in the gap equation. To leading order one finds

$$\varphi _0^{damp}2\frac{b_0}{g^5}\mu \mathrm{exp}\left(\frac{\pi }{2\overline{g}_{eff}}\right),$$
(7)
where $`\overline{g}_{eff}^2=\overline{g}^2\left(12\overline{g}^2\right)`$, and $`\overline{g}=g/3\sqrt{2}\pi `$. The value of the gap at the Fermi surface is then reduced. This can be understood in very intuitive terms. The fact that the quarks decay limits their efficiency to condense. The decay of the quasiparticles should also affect the critical temperature of transition to the normal phase of the system computed in Refs. .

The fermion damping rate effects represent a correction of order $`g^2`$ to the leading order value Eq. (5). It is worth emphasizing that this is not the complete next-to-leading order correction, which it should be possible to compute using the Schwinger-Dyson equations.

Acknowledgements

I would like to thank H. Ren for very useful discussions on the non-Fermi liquid behavior of the QED plasmas. My gratitude also goes to the organizers of this nice meeting. Financial support from a Marie Curie EC Grant (HPMF-CT-1999-00391) is acknowledged.

## References


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# NUC-MINN-00/19-T Will Strangeness Win the Prize?

## 1 Introduction

In the spring of 1998 Barbara Jacak, Xin-Nian Wang and I organized a workshop named Probes of Dense Matter in Ultrarelativistic Heavy Ion Collisions at the Institute for Nuclear Theory (INT), University of Washington, Seattle. During this workshop we discussed the desirability of making predictions for the first data to come from RHIC rather than fitting model parameters after the data was taken. To encourage these predictions we set up a competition. The winner would be the one that made the best prediction for any data taken during the first year of running. We three would be the judges. The winner would be awarded a case of wine that now resides in a cellar in Washington. This competition was widely advertised by the organizers, including announcements made at the last Quark Matter meeting and in a Division of Nuclear Physics, American Physical Society newsletter. The deadline for submissions is now past since the first data at RHIC has been taken.

Eleven submissions were made to the competition. These may be viewed at the web site ftp://www-hpc.lbl.gov/ by clicking on int-prediction. Of the eleven, five involve predictions for strangeness production of one sort or another. These may be categorized as phase space models, hydrodynamic models, and cascade or transport models. I will briefly review the predictions here. For more details the interested reader is directed to the aforementioned web site. All predictions are for Au+Au collisions at the full RHIC beam energy of 100 GeV. Unless otherwise stated the predictions are for central collisions.

## 2 Phase Space Model

Given the number of people who have used the thermal/statistical/phase space model over the years it is somewhat surprising that there is only one entry in this category. This entry is from J. Rafelski and J. Letessier. In its pure form, with kinetic and chemical equilibrium, one calculates the abundances of hadrons of any type using a Fermi-Dirac or Bose-Einstein phase space distribution. One may allow for a system in kinetic, but not chemical, equilibrium by introducing a factor $`\gamma `$ which multiplies the phase space density. Then the parameters consist of temperature $`T`$; baryon, electric charge, and strangeness chemical potentials $`\mu _i`$ (or fugacity $`\lambda _i=\mathrm{exp}(\mu _i/T)`$); and a factor of $`\gamma _q`$ for $`u`$ and $`d`$ and $`\gamma _s`$ for $`s`$ quark content, respectively. Since this approach has no nucleus-nucleus dynamics, one must estimate these parameters at the moment the matter ceases interaction, or freezes out. Of course, they can be fit to the data once it becomes available. Based on existing data from the SPS and elsewhere, and making reasonable and judicious assumptions about what happens at higher energies, the predictions are shown in Tables I and II. Various possibilities for fugacities and enhancement factors are given, but in all cases the temperature is taken to be 150 MeV. It is the numerical value of $`T`$ and the fact that the $`\gamma `$ are not equal to 1 that primarily differentiate this approach from other thermal model approaches. Actually there is not much room to maneuver if one takes the fitted values at the SPS ($`T=160\pm 10`$ and $`\mu _B=200\pm 70`$ MeV) and extrapolates to RHIC. (See the presentation by J. Cleymans in this proceedings.) If the RHIC data show anything close to the predictions of the phase space model as they do at the SPS, particularly for strange hadrons, one is still confronted by the details of the hadronization dynamics that somehow populate phase space.

## 3 Hydrodynamic Models

Hydrodynamic models of high energy collisions go back to Landau in the 1950’s. The advantage of this approach is that it readily incorporates the equation of state and a possible phase transition which is, after all, what we are primarily interested in. The main issues: What are the initial conditions? How accurate is the assumption of local thermal and chemical equilibrium? How is the final stage from hydrodynamic flow to free streaming particles handled? Two groups have entered the competition based on the hydrodynamic approach.

A. Dumitru and D. Rischke solved the relativistic perfect fluid equations assuming longitudinal scaling flow. They used various microscopic models, namely PCM, RQMD, FRITIOF, and HIJING, to assist in estimating the initial conditions. The baryon rapidity density $`dN_B/dy`$ was taken to be 25 and the entropy per baryon was taken to be 200. The formation time of the system was taken as 0.6 fm/c, which is about 1/10 of the radius of a gold nucleus. This resulted in an initial energy density of 17 GeV/fm3 and baryon density of 2.3 times normal nuclear matter density. For a near ideal quark-gluon plasma this yields an initial temperature of 300 MeV and a light quark chemical potential of 47 MeV. The phase transition to hadrons is first order with a critical temperature of 160 MeV (when the baryon chemical potential is zero). The sensitivity of the observed spectra to several different initial density profiles was investigated. They found that the average transverse flow velocity is rather similar to that in central Pb+Pb collisions at the SPS due to the stall of the flow within the mixed phase. Figure 1 shows the calculated transverse momentum spectra for 11 different species of hadrons. The left panel is the distribution immediately after the phase transition is completed, the right panel shows the distribution calculated along the isotherm of $`T=130`$ MeV. One sees clearly that the flow continues to evolve after the phase transition. It is especially apparent for heavier hadrons. Figure 2 shows average transverse velocity (left panel) and transverse momentum (right panel) as a function of the mass of the hadron. Hydrodynamics predicts a linear increase of the average transverse momentum with mass, whereas FRITIOF alone shows a more complicated dependence on the flavor composition of the hadrons. As can be seen, the results do depend on the hypersurface on which the hadron spectra are computed.

S. Bass and A. Dumitru also solved boost invariant hydrodynamic equations. The initial conditions were essentially identical to those of Dumitru and Rischke. The initial transverse energy and baryon density profile was taken to be proportional to $`\sqrt{1(r_T/R_T)^2}`$ with the transverse radius $`R_T=6`$ fm and the formation time 1/10 of that. After the phase transition is complete and the matter has been evolved to a temperature of 130 MeV the hadron spectra are computed using the Cooper-Frye formula, as in Dumitru and Rischke, but the resulting spectra is then used as an initial condition for the hadronic cascade UrQMD. In this way the transition from perfect local thermal equilibrium to free streaming hadrons is done in a more sophisticated manner than making a sudden, abrupt transition from one to the other. The resulting transverse mass distributions for baryons with different strangeness content and for pions and kaons are shown in Figure 3 for SPS, RHIC, and LHC energies. At least for the SPS and RHIC there is not much effect of using UrQMD as the intermediary between hydrodynamic flow and free streaming. Figure 4 shows the average transverse momentum for hadrons as a function of their mass for the three energies. Once again the effect of UrQMD is small but measurable.

These entries nicely illustrate the beautiful evolution of a quark-gluon plasma, through a phase transition, into a hadronic gas and the final nonequilibrium freezeout into free streaming particles. They could be elaborated even more with the use of imperfect fluid dynamics (viscosity and heat conduction) and finite nucleation rates for the phase transition. The main uncertainty is still the choice of initial conditions. The most reasonable choices are to take them from a microscopic model of the early stages of a heavy ion collision, such as these two entries do, or to adjust them so that the computed final state spectra agree with data. Although the second choice is certainly valid and worthwhile it is difficult to refer to it as a prediction.

## 4 Microscopic Transport Models

The most ambitious entries compute the whole nucleus-nucleus collision from beginning to end on the basis of microscopic dynamics with no assumptions about local equilibrium. By necessity this is done with Monte Carlo techniques. There are two entries in this category which are relevant for strange particle production.

B. Zhang, C.M. Ko, B.-A. Li and Z. Lin take the initial parton distributions from HIJING and evolve them according to their parton cascade model ZPC. They allow the partons to hadronize, after which hadrons interact according to the cascade model ART until all particles free stream to infinity. As with any parton cascade there are uncertainties arising from the nature of infrared singularities in QCD. The predictions for $`K^+`$ and for all mesons are shown in Figure 5. The main point is that multiple collisions in the partonic and hadronic phases produce more particles than that input from HIJING. The extra particle production occurs in the central rapidity range where the initial particle density is the highest, of course. The kaon abundance is especially enhanced, by about 50%.

The UrQMD collaboration entry was submitted by M. Bleicher. The UrQMD creates particles at high energies from strings, and at low energies exclusive reactions are parametrized, usually in terms of resonances. It is a very ambitious model which can predict almost anything desired in a heavy ion collision. This also means that it is easier to find fault with it, either in terms of the details of its dynamics, or in terms of predictions not consistent with experimental data. I have selected a subset of all the submitted predictions involving strange hadrons. In Figure 6 are shown the predictions for the rapidity distributions of protons, antiprotons, negative pions, and kaons. In each panel there are two sets of numbers: the open symbols have meson-meson and meson-baryon and certain quark interactions turned off, the full symbols have them all turned on. Just like the previous cascade approach, multiple scattering among the produced particles creates more particles. It also shows that baryons are moved in toward central rapidity from the fragmentation regions. Figure 7 shows the average transverse momentum for pions, kaons, and protons as functions of rapidity. Multiple scatterings increase the mean transverse momentum for protons and kaons, but slightly reduce it for pions. This may be a consequence of the ability of higher energy pions to produce kaons whereas the lower energy pions remain. UrQMD is even so bold as to predict the directed and elliptic flow parameters, $`v_1`$ and $`v_2`$, for every species of hadron. These are shown for pions and kaons in Figures 8 and 9. Pions and kaons flow in about the same way, but the magnitude of the flow coefficients is greater for pions. Similar figures comparing protons, antiprotons, and lambdas may be found at the web site. These observables give information on the degree of equilibration and on the amount of energy loss of the hadrons as they traverse hadronic matter.

Any cascade-like dynamical model requires detailed assumptions about production cross sections, off-shell behavior of propagating particles, formation times, etc. It is very good to see these firm predictions for they can be tested in the very near future!

## 5 Summary

There is a proverb which says “May you live in interesting times.” The three of us eagerly look forward to comparing all the predictions with RHIC data as they emerge. We should be ready to announce the winner in the summer of 2001. The most exciting outcome would be something that was not predicted!

## Acknowledgements

This work was supported by the US Department of Energy under grant DE-FG02-87ER40328.


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# Direct Photon Production in 158 A GeV 208Pb+208Pb Collisions

## 1 Introduction

The observation of a new phase of strongly interacting matter, the quark gluon plasma (QGP), is one of the most important goals of current nuclear physics research. To study QGP formation photons (both real and virtual) were one of the earliest proposed signatures . They are likely to escape from the system directly after production without further interaction, unlike hadrons. Thus, photons carry information on their emitting sources from throughout the entire collision history, including the initial hot and dense phase. Recently, it was shown by Aurenche et al.  that photon production rates in the QGP when calculated up to two loop diagrams, are considerably greater than the earlier lowest order estimates. Following this result, Srivastava  has shown that at sufficiently high initial temperatures the photon yield from quark matter may significantly exceed the contribution from the hadronic matter to provide a direct probe of the quark matter phase.

A large number of measurements of prompt photon production at high transverse momentum ($`p_T>3\mathrm{GeV}/c`$) exist for proton-proton, proton-antiproton, and proton-nucleus collisions (see e.g. ). First attempts to observe direct photon production in ultrarelativistic heavy-ion collisions with oxygen and sulphur beams found no significant excess . The WA80 collaboration  provided the most interesting result with a $`p_T`$ dependent upper limit on the direct photon production in S+Au collisions at 200$`A`$GeV. In this paper we report on the first observation of direct photon production in ultrarelativistic heavy-ion collisions.

## 2 Data Analysis

The results are from the CERN experiment WA98  which consists of large acceptance photon and hadron spectrometers. Photons are measured with the WA98 lead-glass photon detector, LEDA, which consisted of 10,080 individual modules with photomultiplier readout. The detector was located at a distance of 21.5 m from the target and covered the pseudorapidity interval $`2.35<\eta <2.95`$ $`(y_{cm}=2.9)`$. The particle identification was supplemented by a charged particle veto detector in front of LEDA.

The results presented here were obtained from an analysis of the data taken with Pb beams in 1995 and 1996. The 20% most peripheral and the 10% most central reactions have been selected from the minimum bias cross section ($`\sigma _{min.bias}6300\mathrm{mb}`$) using the measured transverse energy $`E_T`$. In total, $`6.710^6`$ central and $`4.310^6`$ peripheral reactions have been analyzed.

The extraction of direct photons in the high multiplicity environment of heavy-ion collisions must be performed on a statistical basis by comparison of the measured inclusive photon spectra to the background expected from hadronic decays. Neutral pions and $`\eta `$ mesons are reconstructed via their $`\gamma \gamma `$ decay branch. For a detailed description of the detectors and the analysis procedure see .

The final measured inclusive photon spectra are then compared to the calculated background photon spectra to check for a possible photon excess beyond that from long-lived radiative decays. The background calculation is based on the measured $`\pi ^0`$ spectra and the measured $`\eta /\pi ^0`$-ratio. The spectral shapes of other hadrons having radiative decays are calculated assuming $`m_T`$-scaling  with yields relative to $`\pi ^0`$’s taken from the literature. It should be noted that the measured contribution (from $`\pi ^0`$ and $`\eta `$) amounts to $`97\%`$ of the total photon background.

## 3 Results

Fig. 1 shows the fully corrected inclusive photon spectra for peripheral and central collisions. The spectra cover the $`p_T`$ range of $`0.34.0\mathrm{GeV}/c`$ (slightly less for peripheral collisions) and extend over six orders of magnitude. Fig. 1 also shows the distributions of neutral pions which extend over a similar momentum range with slightly larger statistical errors.

The ratio of measured photons to calculated background photons is displayed in Fig. 2 as a function of transverse momentum. The upper plot shows the ratio for peripheral collisions which is seen to be compatible with one, i.e. no indication of a direct photon excess is observed. The lower plot shows the same ratio for central collisions. It rises from a value of $`1`$ at low $`p_T`$ to exhibit an excess of about 20% at high $`p_T`$.

A careful study of possible systematical errors is crucial for the direct photon analysis. The largest contributions are from the $`\gamma `$ and $`\pi ^0`$ identification efficiencies and the uncertainties related to the $`\eta `$ measurement. It should be emphasized that the inclusive photon and neutral meson (the basis for the background calculation) yields have been extracted from the same detector for exactly the same data sample. This decreases the sensitivity to many detector related errors and eliminates all errors associated with trigger bias or absolute yield normalization. Full details on the systematical error estimates are given in . The total $`p_T`$-dependent systematical errors are shown by the shaded regions in Fig. 2. A significant photon excess is clearly observed in central collisions for $`p_T>1.5\mathrm{GeV}/c`$.

The final invariant direct photon yield per central collision is presented in Fig. 3. The statistical and asymmetric systematical errors of Fig. 2 are added in quadrature to obtain the total upper and lower errors shown in Fig. 3. An additional $`p_T`$-dependent error is included to account for that portion of the uncertainty in the energy scale which cancels in the ratios. In the case that the lower error is less than zero a downward arrow is shown with the tail of the arrow indicating the 90% confidence level upper limit ($`\gamma _{Excess}+1.28\sigma _{Upper}`$).

No published prompt photon results exist for proton-induced reactions at the $`\sqrt{s}`$ of the present measurement. Instead, prompt photon yields for proton-induced reactions on fixed targets at 200 GeV are shown in Fig. 3 for comparison . These results have been scaled for comparison with the present measurements according to the calculated average number of nucleon-nucleon collisions (660) for the central Pb+Pb event selection and according to the beam energy under the assumption that $`Ed^3\sigma _\gamma /dp^3=f(x_T)/s^2`$, where $`x_T=2p_T/\sqrt{s}`$ . This comparison indicates that the observed direct photon production in central 208Pb+208Pb collisions has a shape similar to that expected for proton-induced reactions at the same $`\sqrt{s}`$ but a yield which is enhanced.

## 4 Summary

The first observation of direct photons in ultrarelativistic heavy-ion collisions has been presented. While peripheral Pb+Pb collisions exhibit no significant photon excess, the 10% most central reactions show a clear excess of direct photons in the range of $`p_T`$ greater than about $`1.5\mathrm{GeV}/c`$. The invariant direct photon multiplicity as a function of transverse momentum was presented for central 208Pb+208Pb collisions and compared to proton-induced results at similar incident energy. The comparison indicates excess direct photon production in central 208Pb+208Pb collisions beyond that expected from proton-induced reactions. The result suggests modification of the prompt photon production in nucleus-nucleus collisions, or additional contributions from pre-equilibrium or thermal photon emission. The result should provide a stringent test for different reaction scenarios, including those with quark gluon plasma formation, and may provide information on the initial temperature attained in these collisions.


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# Wavepacket-current ⟷ supercurrent conversion in closed N/S/N circuits

## Abstract

The rise and decay in space and time of a supercurrent in a superconductor between two normal current leads connected to a reservoir is computed with the help of quasiparticle wavepackets which suffer Andreev scattering in the interfaces between the normal current leads and the superconductor. Stills from a computer movie visualize electron $``$ hole scattering and the creation and destruction of the supercurrent.

preprint: preprint number

Andreev scattering (AS) of electrons into holes and vice versa by spatial variations of the superconducting pair potential , in competition and cooperation with conventional scattering, determines the electronic structure and transport properties of inhomogeneous superconductors. The Tomasch effect in tunnel junctions , Josephson currents , excess currents, and subharmonic gap structures  in superconducting ($`S`$)-normal conducting ($`N`$)-superconducting junctions, as well as the transfer of half of the Magnus force to the core electrons of a moving vortex line  are due to AS. There is AS in He3, too . A wealth of AS phenomena has been discussed recently in  and .

While the conversion of a normal current into a supercurrent by electron $``$ hole scattering in the interface between an $`N`$ and an $`S`$ region of semi-infinite lengths has been described before , it is the purpose of this paper to analyze the normal-current $``$ supercurrent conversion processes in a superconducting layer of finite length $`L_z`$ between two normal current leads. These normal leads are connected to a reservoir (“battery”) which acts as the current source in the closed circuit. The extensions of the $`N`$ and $`S`$ regions in $`x`$\- and $`y`$-directions are $`L_x`$ and $`L_y`$. The metal-vacuum boundaries are treated as rigid walls. By varying $`L_x`$ and $`L_y`$ one can vary the dimensionality of the system. The much investigated quasi-two-dimensional (Q2D) superconducting/semiconducting heterojunctions  and superconducting quantum dots in Q2D channels are systems for which our analysis may prove useful.

AS and the associated formation and destruction of Cooper pairs and supercurrents can be calculated from the Time-dependent Bogoliubov-de Gennes Equations (TdBdGE) . They describe the evolution of the spinor quasiparticle (q.p.) wavefunction with the electron component $`u_n(𝐫,t)`$ and the hole component $`v_n(𝐫,t)`$ under the influence of scalar and vector potentials $`V(𝐫,t)`$ and $`𝐀(𝐫,t)`$ in the single-electron Hamiltonian

$$H_0(𝐫,t)=\frac{1}{2m}\left[\frac{\mathrm{}}{i}e𝐀(𝐫,t)\right]^2+V(𝐫,t)\mu $$

via the matrix equation

$$i\mathrm{}\frac{}{t}\left(\genfrac{}{}{0pt}{}{u_n(𝐫,t)}{v_n(𝐫,t)}\right)=\stackrel{ˇ}{}(𝐫,t)\left(\genfrac{}{}{0pt}{}{u_n(𝐫,t)}{v_n(𝐫,t)}\right).$$
(1)
Here, the matrix Hamiltonian $`\stackrel{ˇ}{}(𝐫,t)`$ has $`H_0(𝐫,t)`$ and $`H_0^{}(𝐫,t)`$ in the diagonal, and the pair potential $`\mathrm{\Delta }(𝐫,t)`$ and its complex-conjugate in the off-diagonal. The chemical potential $`\mu `$ in $`H_0`$ is that of the reservoir. We neglect all influences of entropy production associated with current flow on the chemical potential, because the number of degrees of freedom of the reservoir is assumed to be much larger than that of the normal leads and the superconductor. Thus, $`\mu `$ is constant in space and time .

AS is a many-body process. For its analysis it is convenient to consider a non-equilibrium configuration $`|T_{l\sigma }`$ of the many-body system where one quasiparticle state $`(l\sigma )`$, characterized by a tripel $`l`$ of quantum numbers and spin $`\sigma `$, is definitely occupied and all other q.p. states $`(n\sigma )`$ are occupied according to the equilibrium Fermi distribution function $`f_n`$. All interactions that might affect the spin are neglected. Then, it has been shown  with the help of the TdBdGE (1) that the expectation values $`T_{l\sigma }|\rho (𝐫,t)|T_{l\sigma }`$ and $`T_{l\sigma }|𝐣(𝐫,t)|T_{l\sigma }`$ of the many-body charge- and current-density operators satisfy the relation

$$\frac{}{t}T_{l\sigma }|\rho (𝐫,t)|T_{l\sigma }+\mathrm{div}T_{l\sigma }|𝐣(𝐫,t)|T_{l\sigma }$$

$$=4\frac{e}{\mathrm{}}\mathrm{Im}\left[\mathrm{\Delta }^{}(𝐫,t)u_l(𝐫,t)v_l^{}(𝐫,t)\right](1f_l)+\mathrm{div}𝐣_{sl}.$$

The electron and hole wavefunctions $`u_l`$ and $`v_l`$ satisfy eq. (1), and $`𝐣_{sl}`$ is the supercurrent density induced by the momentum transfer from the q.p. in $`(l\sigma )`$ to the superconducting condensate by AS. The requirement that charge is conserved in the many-body system results in the source equation for the supercurrent density

$$\mathrm{div}𝐣_{sl}=4\frac{e}{\mathrm{}}\mathrm{Im}[\mathrm{\Delta }^{}(𝐫,t)u_l(𝐫,t)v_l^{}(𝐫,t)](1f_l).$$
(2)
A shifted Fermi sphere (or its equivalent in Q2D and Q1D conductors) represents the current-carrying many-body configurations in the two parts of the normal current leads that are parallel to the $`z`$-axis and connected to the superconductor. (We do not consider the parts of the normal current leads bent towards the reservoir.) In this non-equilibrium distribution of electrons above the Fermi surface in states with positive momentum in $`z`$-direction and unoccupied states with negative $`z`$-momentum below the Fermi surface the force of the electric field from the battery is balanced by the frictional forces from electron-phonon interaction. In the following we try to obtain the details of normal current $``$ supercurrent conversion by studying the motion of electron and hole wavepackets that are part of the shifted Fermi sphere. The quasiparticles in this normal-state configuration are uncorrelated. Thus, the total current in the closed circuit is the sum of the currents from the individual wavepackets.

The $`z`$-momenta of the electrons (+) and holes ($``$) in the shifted Fermi sphere are $`\mathrm{}k^\pm `$, with $`k^\pm (E)=[k_{zF}^2\pm E2m/\mathrm{}^2]^{1/2}`$. Here, $`k_{zF}=[k_F^2(n_x\pi /L_x)^2(n_y\pi /L_y)^2]^{1/2}`$ is the $`z`$-component of the Fermi wavenumber $`k_F[2m\mu /\mathrm{}^2]^{1/2}`$, and $`(n_x\pi /L_x)`$ and $`(n_y\pi /L_y)`$, $`n_{x,y}`$ integers, are the wavenumbers of the standing waves between the rigid walls that limit the metals in $`x`$\- and $`y`$-directions. The energy $`E`$ of both electrons and holes is positive and measured relative to the surface of the unshifted Fermi sphere at the chemical potential $`\mu `$. For normal current densities below the critical current densities of conventional superconductors all $`E`$ are less than the modulus $`\mathrm{\Delta }`$ of the pair potential $`\mathrm{\Delta }(z)\mathrm{\Delta }\mathrm{\Theta }(z)\mathrm{\Theta }(L_zz)`$, where $`\mathrm{\Theta }(z)`$ is the Heavyside function.

The construction of the representative wavepacket ensemble, whose motion and conversion into a supercurrent models the elementary process of current flow in the N/S/N circuit, starts with a normalized electron wavepacket, localized around $`z_0<0`$ in the normal current lead to the left of the superconductor at time $`t=0`$. In the center of the wavepacket the energy is $`E_l`$. We choose a Gaussian spectral function

$$D(E)=\frac{a_z}{\sqrt{2\pi }}e^{[k^+(E)k^+(E_l)]^2a_z^2/2}e^{i[k^+(E)k^+(E_l)]z_0};$$

the position-uncertainty parameter $`a_z|z_0|`$ is chosen so large that the related energy spread of the wavepacket, $`\delta E=\mathrm{}^2k_{zF}/ma_z`$, is less than $`\mathrm{\Delta }E_l`$. Solutions of eq. (1), where $`V`$ and $`𝐀`$ are neglected and $`\mathrm{\Delta }(𝐫,t)`$ is approximated by the real $`\mathrm{\Delta }(z)`$ (thereby neglecting repercussions of the q.p.-induced supercurrent on the q.p. and on itself, assuming sufficiently small $`L_x`$ and $`L_y`$) are multiplied by the spectral function $`D(E)`$, integrated over all energies, and matched at the left $`N/S`$ interface, i.e. $`z=0`$, in the usual Andreev approximation, neglecting terms of the order of $`\mathrm{\Delta }/\mu `$ outside the exponentials. In so doing, energy-dependent functions are Taylor expanded around $`E_l`$ up to first order in $`(EE_l)`$. This affects especially $`k^\pm (E)`$ and the amplitude of the Andreev-reflection probability

$$\gamma (E)e^{i\mathrm{arccos}E/\mathrm{\Delta }}\gamma (E_l)e^{(i/\mathrm{})(EE_l)\tau _l},$$

where $`\tau _l=\mathrm{}[\mathrm{\Delta }^2E_l^2]^{1/2}`$ is the time for one electron $``$ hole-scattering event and the associated formation of a Cooper pair, see eqs. (3,4). The resulting electron and hole wavepackets $`u_{NL}(𝐫,t)`$ and $`v_{NL}(𝐫,t)`$ in the left normal current lead, $`z<0`$, and the exponentially decaying solutions $`u_{SL}(𝐫,t)`$ and $`v_{SL}(𝐫,t)`$ in $`z>0`$, that contribute to the source equation (2) essentially in the left half of the superconductor, turn out to be

$`u_{NL}`$ $`=`$ $`w_le^{ik_l^+z}e^{[z_0z+v_l^+t]^2/2a_z^2},`$ (3)
$`v_{NL}`$ $`=`$ $`w_l\gamma (E_l)e^{ik_l^{}z}e^{[z_0+(v_l^+/v_l^{})z+v_l^+(t\tau _l)]^2/2a_z^2},`$ (4)
$`u_{SL}`$ $`=`$ $`w_le^{ik_{zF}z}e^{\kappa _lz}e^{[z_0+v_l^+t]^2/2a_z^2},`$ (5)
$`v_{SL}`$ $`=`$ $`w_l\gamma (E_l)e^{ik_{zF}z}e^{\kappa _lz}e^{[z_0+v_l^+(t\tau _l)]^2/2a_z^2},`$ (6)
where

$`w_l{\displaystyle \frac{2}{(L_xL_ya_z\sqrt{\pi })^{1/2}}}\mathrm{sin}\left({\displaystyle \frac{n_x\pi }{L_x}}x\right)\mathrm{sin}\left({\displaystyle \frac{n_y\pi }{L_y}}y\right)e^{iE_lt/\mathrm{}},`$

$`k_l^\pm k^\pm (E_l),`$ $`v_l^\pm \mathrm{}k_l^\pm /m`$, and $`\kappa _l(\mathrm{\Delta }^2E_l^2)^{1/2}/\mathrm{}v_{zF}=1/\tau _lv_{zF}`$, with $`v_{zF}\mathrm{}k_{zF}/m`$. \[For the sake of simplicity the complex wavenumbers in $`u_{SL}`$ and $`v_{SL}`$ have not been Taylor expanded in $`(EE_l)`$ but rather taken at $`E_l`$ right away.\]

Identifying the wavefunctions $`u_{SL}`$ and $`v_{SL}`$ from eqs. (5) and (6) with the $`u_l`$ and $`v_l`$ of the source equation (2) and integrating that equation from $`z=0`$ to $`z`$ yields the density of the supercurrent in $`z`$-direction induced in the left half of the superconductor by AS of the electron wavepacket $`u_{NL}`$ into the hole wavepacket $`v_{NL}`$ as

$`𝐣_{sl,L}`$ $`=`$ $`𝐞_z(2ev_{zF})|w_l|^2[1e^{2\kappa _lz}]`$ (8)
$`\times e^{\{[z_0+v_l^+(t\tau _l/2)]^2+(\tau _lv_l^+/2)^2\}/a_z^2}(1f_l).`$
Here we have assumed that $`L_z1/\kappa _l`$. In the opposite case one would have to add a second source term on the r.h.s. of eq. (2) which would contain the contribution from the solution $`u_{SR}(𝐫,t),v_{SR}(𝐫,t)`$ of eq. (1) for $`0<z<L_z`$ that matches to the current-carrying q.p. wavepackets in the right normal current lead at $`z=L_z`$ and decays exponentially with increasing distance from $`L_z`$. This solution determines the supercurrent in the right half of the superconductor essentially, and its energy and amplitude are obtained as $`E_l`$ and $`w_l`$ from the requirement that the two supercurrent densities, computed from $`u_{SL}v_{SL}^{}`$ and $`u_{SR}v_{SR}^{}`$, join smoothly at all times somewhere within the superconductor. (Since the many-body configurations in the left and right normal current leads are uncorrelated, only the current densities, not the wavefunctions, must join smoothly.) Because of the symmetry of the problem the matching point turns out to be $`L_z/2`$, and we obtain

$`u_{SR}`$ $`=`$ $`w_le^{ik_{zF}z}e^{\kappa _l(L_zz)}e^{[z_0+v_l^+(t\tau _l)]^2/2a_z^2},`$ (9)
$`v_{SR}`$ $`=`$ $`w_l\gamma (E_l)^1e^{ik_{zF}z}e^{\kappa _l(L_zz)}e^{[z_0+v_l^+t]^2/2a_z^2}.`$ (10)
The supercurrent density $`𝐣_{sl,R}`$ that results from integrating eq. (2) from $`L_z`$ to $`z`$, with $`u_{SR}v_{SR}^{}`$ in the place of $`u_lv_l^{}`$, has the same form as $`𝐣_{sl,L}`$ of eq. (8) except that $`\mathrm{exp}[2\kappa _lz]`$ is being replaced by $`\mathrm{exp}[2\kappa _l(L_zz)]`$. Finally, the wavepacket solutions $`u_{NR}(𝐫,t),v_{NR}(𝐫,t)`$ of eq. (1) in the right normal current lead, $`z>L_z`$, that match to the $`u_{SR}(𝐫,t),v_{SR}(𝐫,t)`$ at the right interface in $`z=L_z`$, become

$`u_{NR}`$ $`=`$ $`w_le^{ik_{zF}L_z}e^{ik_l^+(zL_z)}`$ (12)
$`\times e^{[z_0+L_zz+v_l^+(t\tau _l)]^2/2a_z^2},`$
$`v_{NR}`$ $`=`$ $`w_l\gamma (E_l)^1e^{ik_{zF}L_z}e^{ik_l^{}(zL_z)}`$ (14)
$`\times e^{[z_0+(v_l^+/v_l^{})(zL_z)+v_l^+t]^2/2a_z^2}.`$
Comparison of the $`u_{NL},v_{NL}`$ with the $`u_{NR},v_{NR}`$ shows that the center of the electron wavepacket $`u_{NL}`$, propagating to the right with velocity $`v_l^+`$ in the left normal current lead, and the center of the hole wavepacket $`v_{NR}`$, propagating to the left with velocity $`v_l^{}`$ in the right normal current lead, hit the left and right interfaces at $`z=0`$ and $`z=L_z`$ at the same time $`t_0=z_0/v_l^+`$, while the hole wavepacket $`v_{NL}`$, propagating to the left in $`z<0`$ with $`v_l^{}`$, and the electron wavepacket $`u_{NR}`$, propagating to the right in $`z>L_z`$, are retarded by the time $`\tau _l`$ with respect to the incident wavepackets. This means: electron $``$ hole scattering in the left interface combines the electron with spin up above the Fermi surface with another spin-down electron below the Fermi surface to form a Cooper pair at the chemical potential, leaving the hole with spin up in the left normal region, transferring the momentum $`2\mathrm{}k_{zF}`$ to the condensate, and simultaneously in the right interface a Cooper pair decays by hole $``$ electron scattering into the incident hole and the reflected electron of total momentum $`2\mathrm{}k_{zF}`$. The supercurrent density $`𝐣_{sl}`$ spreads instantaneously in the superconductor. Its spatial maximum is at $`z=L_z/2`$, and its maximum in time occurs at $`t=t_0+\tau _l/2`$. From the equations for $`𝐣_{sl}`$, $`u_{SL,R}`$ and $`v_{SL,R}`$ one sees that the quasiparticle current density

$$𝐣_{QPl}\frac{e}{m}\mathrm{Re}\left[u_l^{}\frac{\mathrm{}}{i}u_lv_l\frac{\mathrm{}}{i}v_l^{}\right](1f_l)$$

changes into the supercurrent density $`𝐣_{sl}`$ and vice versa within a distance $`1/\kappa _l=v_{zF}\tau _l`$ from the interfaces. Figure 1 shows stills from a computer movie of the described Andreev-scattering and wavepacket-current $``$ supercurrent–conversion processes.

By summing the current contributions from the steady flow of all quasiparticle wavepackets $`(l\sigma )`$, $`l(E_l,n_x,n_y)`$, that corresponds to the shifted Fermi sphere in the normal current leads, one obtains the total normal current and the total supercurrent within the closed $`N/S/N`$ circuit.

The supercurrent, carried by the condensate in the $`S`$ layer, involves only states with $`|E_n|\mathrm{\Delta }`$. It continues the current from the electrons and holes with energies $`E_l<\mathrm{\Delta }`$ in the normal current leads. If the total current density exceeds its critical value, i.e. if the center of the Fermi sphere in the normal current leads is shifted by more than $`\mathrm{}q_{cS}=\mathrm{\Delta }m/\mathrm{}k_F`$, depairing sets in, and when superconductivity has broken down the uncorrelated normal-state configuration reigns everywhere in the circuit. If the single $`S`$ layer is replaced by a mesoscopic $`SNS`$ junction, the many-body configuration in the central $`N`$ layer is a phase-coherent one and thus different from the uncorrelated configurations in the normal current leads. In an $`N/SNS/N`$ circuit the $`SNS`$ junction acts as a gapless superconductor . It can carry a dissipation-free Josephson current through the central $`N`$ layer via phasecoherent q.p. states with $`|E|<\mathrm{\Delta }`$ and $`|E|\mathrm{\Delta }`$ . This current converts as a whole into the total supercurrent of the $`S`$ layers, and vice versa, whereas, according to eq. (2), each uncorrelated q.p. from the normal current leads individually induces its proper fraction of the total supercurrent. If the total current density exceeds the critical Josephson-current density at a Fermi-sphere shift of $`\mathrm{}q_{cSNS}\mathrm{}/d`$, where $`d`$ is the length of the central $`N`$ layer , a voltage drop appears across the $`SNS`$ junction. There are different models  for $`SNS`$ junctions with voltage drops. They differ with respect to the implicit assumptions about the rate and energy range of q.p. creation in the central $`N`$ layer by supercurrent $``$ quasiparticle-current conversion. The question of how this rate and range depend upon the weakening of phase coherence in the $`SNS`$ junction by energy exchange between quasiparticles and electric fields, phonons, and thermal fluctuations like Nyquist-Johnson noise is presently investigated.