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# Clouds and Clearings in the Atmospheres of the L and T Dwarfs

## 1. Introduction

Long before the first discoveries of brown dwarfs, it was recognized that condensates would play a critical role in controlling their atmospheric opacity, at least in certain effective temperature ranges (Stevenson 1986; Lunine et al. 1989). It was also evident that the correct choice for the vertical distribution of the condensates was not obvious (Lunine et al. 1989). Condensates might be well mixed in the atmosphere above their condensation level, or might coalesce into large particles, fall below their condensation level and be removed from the atmosphere. Of course many intermediate cases are possible as well.

After the discovery of what came to be known as the L and T dwarfs, modelers initially focused on simple end cases. Condensates were either assumed to have either completely settled from the atmosphere or else were mixed uniformly throughout the observable atmosphere. The prior approach works reasonably well for objects like Gl 229 B (Allard et al. 1996; Marley et al. 1996; Saumon et al. 2000; Tsuji et al. 1996), while the latter works for very late M and early L dwarfs like Kelu 1 (Ruiz, Leggett & Allard 1997). Neither approach, however, could adequately reproduce the colors, let alone the spectra of the latest Ls or the ‘transition’ late L/early T objects, like SDSS 1254 (Fig. 1).

Models (Fig. 1) in which the condensates are absent from the atmosphere produce $`JK`$ colors that are much bluer than the observed L dwarfs. The blue color arises from water, pressure-induced $`\mathrm{H}_2`$, and for lower effective temperatures ($`T_{\mathrm{eff}}<1400\mathrm{K}`$) $`\mathrm{CH}_4`$ absorption in $`K`$ band. Models with condensates distributed uniformly through the atmosphere match the early Ls in which the condensate column optical depth is small, but are much redder than the colors of the later L dwarfs. The reason is that as the cloud deck falls progressively deeper in the atmosphere the column abundance of dust gets progressively larger. Since the cloud is forming at higher air densities the abundance of condensates to be mixed upwards from cloud base is larger with falling effective temperature. Thus an outside observer sees an ever increasing dust optical depth until the observer is effectively looking at a dirt-filled atmosphere. Like blackbodies, such objects becomes progressively redder in $`JK`$ as they cool. These models cannot reproduce the observed transition from red to blue in $`JK`$ between the L and T dwarfs.

An obvious shortcoming of the first generation models is that none of them employed cloud decks like those seen throughout the solar system. Condensates in planetary atmospheres are generally neither completely settled out of the atmosphere nor distributed uniformly to the top of the atmosphere. Rather they tend to exist in horizontally-extended cloud decks. The $`\mathrm{H}_2\mathrm{SO}_4`$ clouds of Venus, stratiform water clouds on Earth, the ammonia cloud decks on Jupiter, and the methane clouds in Uranus and Neptune are all examples of this.

To demonstrate that a vertically constrained cloud deck would qualitatively be more in line with the available data, Marley (2000) constructed a simple model in which all clouds were 1 scale height thick. He showed that such a model produced less red $`JK`$ colors than well mixed models and also naturally explained the turnover in $`JK`$ color from the red L dwarfs to the blue T dwarfs. As the cloud forms progressively lower in the atmosphere as the object cools, the cloud disappears while the clear atmosphere above takes on the appearance of the cloud-free models. Tsuji (2001) also used a simple model with a finite-thickness cloud to make the same point.

Given the apparent importance of correctly modeling cloud behavior, Ackerman & Marley (2001) developed a more rigorous cloud model for use in substellar atmosphere models. The model attempts to capture the key ‘zeroth order’ physics which influence the vertical condensate abundance and size profiles in a realistic (but 1-D) atmosphere. This model was used by Marley et al. (2002) and Burgasser et al. (2002) to model the atmospheres of L and T dwarfs. Other workers have recently turned to the work of Rossow (1978), originally developed to study the microphysics of clouds in planetary atmospheres, to model cloud behavior in substellar atmospheres. Finally Tsuji (2002) has further developed his model in which the cloud top temperature is an adjustable parameter. In Section 2 we review and compare these cloud models. In Section 3 we summarize the results of Burgasser et al. in applying the Ackerman & Marley cloud model to L and T dwarfs and consider the role of dynamically-induced holes in the global cloud coverage.

## 2. A Comparison of Cloud Models

Calculating the opacity of condensates in an atmosphere requires estimating the distribution of particles over space and particle size. Estimates of condensate opacities in brown dwarf atmospheres have all assumed a steady state, horizontally homogeneous distribution. Beyond those common assumptions, a number of distinct approaches have appeared in the literature in recent years, ranging in complexity from (a) the simple approach of Tsuji (2002), in which the size of cloud particles is fixed, as are the temperatures at the bottom and top of the cloudy layer; (b) the more physically motivated method of Ackerman & Marley (2001), in which the size of cloud particles and the profile of condensate mass are coupled through an eddy mixing assumption and a parameter describing the sedimentation efficiency; and (c) the more detailed approach of Cooper et al. (2002), in which a number of time microphysical and transport time constants are evaluated in the spirit of Rossow (1978). We briefly describe and compare these three approaches below.

### 2.1. Tsuji (2002)

Tsuji (2002) simply assumes that all condensate particles are 10 nanometers in radius, and are vertically located between their condensation temperature (establishing cloud base for each condensate, assuming solar abundances) and a prescribed temperature corresponding to cloud top for all species. No mention is made of the assumed vertical distribution of condensate mass. Likely possibilities include the assumption of a uniform mixing ratio or concentration.

All particles are prescribed to have a single fixed radius, which is described as the critical radius corresponding to the Gibbs free energy of formation of a molecular cluster, in which the surface tension is just offset by the supersaturation of a condensing gas. Assumed values of critical supersaturations and surface tensions are not given, so the validity of a uniform critical radius for all species is not easily evaluated. Tsuji argues that particles larger than this critical radius will grow and sediment out, and therefore only particles at this critical radius can remain within the cloud layer. These arguments assume that there are no vertical motions within the cloudy air to offset sedimentation, and that the formation of the particle clusters does not deplete the supersaturation that gave rise to them. It is not clear how this first argument is to be considered consistent with other elements of the atmospheric model, in which convective velocities are shown to vary between 10 and 80 m/s, which are strong enough to offset the sedimentation of particles hundreds of microns in radius. Furthermore, the notion that particles in long-lived clouds are limited to their critical radius is clearly invalid in the only atmosphere in which we have direct cloud microphysical measurements. Water cloud particles in the terrestrial troposphere typically range in modal size from 10 to 100 microns. In the terrestrial stratosphere sulfuric acid cloud particle sizes are of order microns, still over one hundred times that assumed by Tsuji.

Condensates (such as enstatite) that form at levels cooler than the prescribed cloud top temperature are assumed to not exist in the model atmospheres. Tsuji suggests that such condensates nucleate on other condensed species, and therefore rapidly sediment out, a process akin to seeding terrestrial cumulus clouds with large condensation nuclei to enhance precipitation. However, depending upon the meteorological and background aerosol conditions, increasing the concentration of condensation nuclei can instead suppress precipitation in terrestrial clouds (e.g., Ackerman et al. 1993). This second possibility is ruled out by Tsuji’s model.

For the same cloud top temperatures, Tsuji finds that cloud opacities in the atmospheres of T dwarfs are greatly reduced from that in L dwarfs because the clouds that form in the former (colder) atmospheres are limited (by virtue of his cloud-top temperature cutoff) to levels below the photosphere. This result effectively reproduces the result of earlier models that assume cloud layers are limited to one scale height in depth (e.g., Marley et al., 2000).

Tsuji’s choice of cloud top temperature does reproduce the limiting value of $`JK2`$ seen in the latest L dwarfs as well as several other observed trends in the available data (Tsuji 2002). However since his model photometry is not combined with an evolution model to provide radii, hence absolute magnitudes, it is not clear if these ‘Unified’ models are able to reproduce the observed rapid transition in $`JK`$ from the Ls to the Ts discussed in Section 3.

### 2.2. Ackerman & Marley (2001)

The treatment of Ackerman & Marley has been inaccurately described (by Cooper et al., 2002) as being based on microphysical time scales. Instead the microphysical time scale approach pioneered by Rossow (1978), in which highly uncertain estimates are made for a number of microphysical processes, was bypassed by Ackerman & Marley in favor of a much simpler approach, in which a steady-state balance between sedimentation (of condensate) and mixing (of condensate and vapor) is solved at each model level. This advective-diffusive balance provides the profile of condensed mass in their model atmospheres. Condensate size distributions at each model level are represented as a log-normal distribution that is coupled to the advective-diffusive steady-state profile. The width of the distribution is a free parameter (a fixed geometric standard deviation of 2 is assumed), while the other two unknowns in the size distribution (total number concentration and modal radius) are calculated from, respectively, the steady-state condensate concentration and the sedimentation flux. The sedimentation flux is calculated by integrating particle sedimentation velocity over the log-normal particle size distribution.

The Ackerman & Marley treatment of mean particle size can be viewed as resembling an extremely simplified variant of the Rossow time scale approach in that the mean particle size calculation does use particle sedimentation speeds, and Rossow’s sedimentation time scale calculation also uses particle sedimentation speeds. Rossow divides the atmospheric scale height by the sedimentation speed to calculate a time scale, but ignores eddy mixing time scales in his analysis, and instead compares the sedimentation time scale to time scale estimates for particle condensation, coagulation, or gravitational coalescence. In contrast, Ackerman & Marley effectively compare particle sedimentation speed to the convective velocity scale to calculate mean particle size.

A notable extension of the Ackerman & Marley approach beyond preceding efforts along the same lines (e.g., Lunine et al., 1989) is to incorporate a sedimentation scaling factor in their computations of advective-diffusive balance and the mean particle size. This factor was originally called $`f_{\mathrm{rain}}`$ (for “rain factor”), but rain is associated by some researchers in the astrophysics field with the process that has been termed “rain-out”, in which all condensate is removed from a saturated layer, and furthermore rain is a term specific to condensed water. Hence, a more appropriate description of the scaling factor would be “sedimentation factor” or $`f_{\mathrm{sed}}`$. Ackerman & Marley found that $`f_{\mathrm{sed}}=3`$ reasonably reproduces the observations of Jupiter’s ammonia ice cloud, and results in a condensate opacity scale height of approximately 1/4 of a pressure scale height.

The Ackerman & Marley model has a small number of free parameters, but only $`f_{\mathrm{sed}}`$ has been adjusted to fit observations in practice. The other free microphysical parameters, the geometric standard deviation of the particle size distributions and the supersaturation that persists after condensation, are fixed at 2 and 0, respectively. The remaining free parameters relate to the difficulty of calculating eddy diffusion coefficients from mixing length theory in stable regions of the atmosphere. In such regions they calculate the mixing length by scaling the atmospheric scale height by the ratio of the local to the adiabatic temperature lapse rate, with a minimum scaling fixed at 0.1. They also specify that the minimum eddy diffusion coefficient is fixed (currently at $`10^5\mathrm{cm}^2/\mathrm{s}`$) to represent residual sources of turbulence such as breaking buoyancy waves.

### 2.3. Cooper et al. (2002)

Cooper et al. (2002) and Allard et al. (this volume) draw on the approach of Rossow (1978) to compute cloud models. While Rossow’s microphysical and transport time constant approach is appealing, it is not without its own set of stumbling blocks. To highlight some of the assumptions inherent in this approach we scrutinize in this section the cloud model111Comments here refer to the pre-publication version of Cooper et al. that appeared on astro-ph on May 15, 2002. of Cooper et al. (2002).

For their profiles of condensate mass, Cooper et al. evidently assume that all the condensate resides within one pressure scale height above the base of each condensate cloud. It is not immediately obvious from their description how the condensate mass is distributed vertically within that scale height. They state that all the supersaturated vapor above cloud base condenses, as assumed by Ackerman & Marley (2001). Recall that Ackerman & Marley calculate vertical profiles through the assumption of advective-diffusive steady-state. Cooper et al. calculate profiles of convective velocity scale (though unlike Ackerman & Marley, they do not give their formulation), which they use to calculate convective time scales to estimate particle sizes (described below). However, Cooper et al. do not state whether or not (or how) they might use the convective velocity scale to calculate their vertical distribution of condensate mass. It may be the case that they are calculating an advective-diffusive steady-state profile, as done by Ackerman & Marley, except that Cooper would presumably assume all the vapor to be condensed and that $`f_{\mathrm{sed}}=1`$, which would be somewhat consistent with a condensate scale height matching the pressure scale height. However, such a profile would not be entirely consistent with their description, which states that 100% of the available vapor condenses within one scale height of cloud base. Perhaps the condensate profile within that scale height assumes that the vapor plus condensate is well mixed (uniform mixing ratio). Or perhaps they use the method of Lewis (1969) without stating so directly. As described further in the review of other models by Ackerman & Marley, the approach of Lewis is easiest to understand in terms of a parcel in an updraft, in which all the condensate sediments at exactly the updraft speed. Ackerman & Marley show that the Lewis model of Jupiter’s ammonia cloud gives the equivalent condensate profile for the Ackerman & Marley model with $`f_{\mathrm{sed}}5`$. Hence if Cooper et al. are using the method of Lewis (1969) to calculate their condensate profile, their clouds are more physically compact than those of the baseline Ackerman and Marley model (with $`f_{\mathrm{sed}}=3`$), in contrast to the opposite conclusion stated by Cooper et al.

To calculate the size of condensate particles, Cooper et al. evidently assume a monodisperse distribution as done by Tsuji, rather than distributing the condensate over a range of sizes as done by Ackerman & Marley. Our only evidence of this assumption is their omission of any mention of droplet size distributions. Further unlike Ackerman & Marley but like Tsuji, Cooper et al. also assume that the particle size is fixed with altitude, as stated in their Section 6.3, although they show a profile of particle sizes in their Figure 5, which is somewhat puzzling.

Cooper et al. (2002) essentially apply a hybrid approach toward calculating the size of condensate particles. In convective regions they effectively calculate their particle size through a simplified form (by virtue of their monodisperse size distribution) of the treatment by Ackerman & Marley (2001), in which Cooper et al. assume $`f_{\mathrm{sed}}=1`$. In radiative regimes Cooper et al. use a modification of the Rossow (1978) treatment to calculate particle size. For this detailed treatment, Cooper et al. estimate time scales for sedimentation, heterogeneous nucleation, homogeneous nucleation, coagulation (collision from thermal motions), and coalescence (collisions from differential sedimentation speeds). Rossow argues that the condensational time scale for cloud particles is much longer than the nucleation time scale in planetary atmospheres because cloud particles heterogeneously nucleate on condensation nuclei at a rapid rate compared to the cooling rate of the cloudy atmosphere. Hence, Rossow ignores the nucleation time scales in calculating characteristic particle sizes. In contrast, Cooper et al. consider the process of homogeneous nucleation to be important in the water and iron clouds of brown dwarf atmospheres, and therefore estimate nucleation time scales. These detailed calculations require estimating a number of additional parameters, such as surface tension, which requires estimating whether the cloud particles are crystalline, glassy, or liquid. Cooper et al. do not state their assumptions regarding this difficult issue. Furthermore, in his treatment of nucleation and condensation time scales, Rossow shows that they must be considered in tandem to calculate a growth rate. That is, the overall condensational time scale is equal to inverse of the sum of the growth rate of the particle masses plus the growth rate of the total number of particles. However, Cooper et al. treat the nucleation rate as a growth process on its own, a divergence from the method of Rossow that is not obviously justifiable, nor is the departure explained.

Other important parameters that must be estimated in their approach include the maximum supersaturation, and the coagulation and coalescence efficiencies. Additionally, the shape and breadth of the size distributions must be estimated to calculate coagulation and coalescence time scales. Cooper et al. provide no information regarding their assumed size distributions for these purposes, but presumably for their estimates of coagulation and particularly coalescence time scales they assume that their size distributions have some breadth, since a monodisperse size distribution would lack dispersion of terminal sedimentation speeds, and hence coalescence will be inoperative.

## 3. The L to T Transition

Marley et al. (2002) employed the Ackerman & Marley (2001) cloud model to compute atmosphere models for L and T dwarfs. Burgasser et al. (2002) combined these models with the evolution calculation of Burrows et al. (1997) to prepare a $`M_J`$ vs $`M_JM_K`$ color magnitude diagram (Fig. 1). Since Burrows et al. used an earlier set of atmosphere models (that utilized the Lunine et al. (1986) dust model) as atmospheric boundary conditions, Figure 1 is not entirely self-consistent. However since model radii vary relatively little over the magnitude range plotted, this is not an important source of error. In the future we will present an entirely self-consistent evolutionary calculation.

Figure 1 compares cloudy ($`f_{\mathrm{sed}}=3`$) and cloud-free models of L and T dwarfs with parallaxes measured by the Flagstaff USNO group (Dahn et al. 2002; Harris, this volume). Also shown is the track predicted by the well-mixed DUSTY models of Chabrier et al. (2000). The main conclusion to be drawn is that neither the cloud-free nor the DUSTY models fit the colors of the L-dwarfs. The cloudy models better fit the data, including the saturation in $`JK`$ at around 2 seen in the latest L dwarfs. Models that do not include particle sedimentation produce redder colors because more condensate mass remains in the atmosphere. Models with more efficient sedimentation, in contrast, produce colors intermediate between the clear and the $`f_{\mathrm{sed}}=3`$ case.

Interestingly Ackerman & Marley find that the value of $`f_{\mathrm{sed}}`$ which best fits the (poorly constrained) particle size and vertical profile of Jupiter’s ammonia cloud deck is also 3. More sophisticated dynamical studies of giant planet and brown dwarf atmospheric convection may ultimately shed light on the mechanisms underlying this result.

The challenge facing any model with a global, 1-D, cloud is that the $`JK`$ colors of brown dwarfs swing from the red to the blue over a very small interval in effective temperature and $`M_J`$. This is shown by the data in Figure 1 as well as other parallax data presented at the workshop by Tinney and collaborators (this volume). Maria Zapeterio-Osario presented colors and J magnitudes of objects in the $`\sigma `$ Orionis cluster (this volume) that are also consistent with the rapid change in color. It is very difficult for a globally uniform cloud to make such a sudden transition since the cloud base and, more importantly, the optical depth of the overlying gas change slowly with effective temperature. The $`f_{\mathrm{sed}}=3`$ model in Fig. 1 typifies this relatively slow transition.

The rapid transition suggests that something special may be happening at the L to T transition. One possibility might be that the global atmospheric dynamics change in such a way to rapidly favor more efficient particle sedimentation (larger $`f_{\mathrm{sed}}`$) at the transition. A second possibility, originally suggested by Ackerman & Marley (2001), is that horizontal patchiness, or holes, develop in the cloud layer at the L to T transition. Holes, or optically thin regions in the global cloud deck, cover less than 10% of Jupiter’s disk. At most thermal wavelengths optical depth unity is reached near or above these cloud tops, so the reduced cloud opacity in the holes is of little consequence. Near $`5\mu \mathrm{m}`$, however, there is a minimum in the combined $`\mathrm{H}_2\mathrm{O}`$, $`\mathrm{CH}_4`$, and $`\mathrm{H}_2`$ gas opacity. Over most of the planet the cloud deck provides an opacity ‘floor’ at this wavelength, but in the cloud holes flux from deeper, warmer, and thus brighter regions can emerge. Essentially all of Jupiter’s $`5\mu \mathrm{m}`$ radiation emerges through these ‘hot spots’, which were first recognized in the 1960’s (Gillett, Low & Stein 1969). A $`5\mu \mathrm{m}`$ image of Jupiter is shown in Figure 2. The long path lengths through the atmosphere into the hole regions allow relatively rare species, such as $`\mathrm{PH}_3`$ and $`\mathrm{GeH}_4`$, to be detected in Jupiter’s atmosphere (Kunde et al. 1982).

Burgasser et al. (2002) argue that a similar gas opacity window exists at 1 $`\mu `$m in late-L/early-T dwarfs, and deeper, hotter layers can be probed at this wavelength in breaks in the upper condensate cloud decks. They point to the rapid change in $`JK`$ color at the L to T transition as well as the observed resurgence in FeH absorption in the earliest T dwarfs (after monotonically declining through the L dwarfs) as supporting that clouds are patchy on brown dwarfs as well. In the L dwarfs gaseous FeH abundance presumably declines as iron and silicates condense into clouds, leading to a simultaneous increase in the $`JK`$ color as the atmosphere becomes cloudier. Near the bottom of the L dwarf sequence holes begin to appear in the clouds, allowing bright, blue (in $`JK`$) flux to emerge. This flux pulls the integrated color over the disk blueward and can even lead to a brightening at J band (Fig. 1). Simultaneously FeH gas, lying below the cloud base, again becomes detectable through the holes.

The patchy cloud model predicts that the effective temperature range of the earliest (T0 to T5) dwarfs is very small, the variations in spectral properties depending more on the fractional cloud cover than a varying effective temperature. There are some indications that this is true (Leggett et al., this volume), although more work is needed. Furthermore the patchy model suggests that the early T dwarfs will exhibit substantial variability in the infrared. At this conference evidence was presented that the T2 dwarf SDSS 1254 is indeed apparently variable in $`J`$ and $`H`$ bands (Artigau et al., this volume).

The mechanism responsible for clearings in Jupiter’s cloud deck is still not perfectly understood, although downdrafts of warm, dry air are likely involved (Showman & Dowling 2000). The principle brown dwarf cloud decks (iron and silicate) will become subject to such vertical flows when cloud base and the cloud tops become well seated in the atmospheric convection zone. In earlier type dwarfs much of the cloud opacity lies within the statically stable radiative zone where vertical motions are substantially smaller. Clouds in these regions may be similar to the stratospheric photochemical hazes of Jupiter and Titan, which are globally fairly uniform.

## 4. Summary

It appears that a complete description of the behavior of L and T dwarfs will require a thorough understanding of the behavior of condensates in their atmospheres. In doing so models must simultaneously and self-consistently account for a number of influences including particle nucleation, sedimentation, and vertical transport. Other influences, including large scale atmospheric dynamics which may be responsible for cloud patchiness, may also be important. Given this daunting task, it is worth remembering that even after half a century of dedicated effort, such key properties as the particle sizes and vertical structure of most of the cloud decks in the solar system are still poorly known. The mechanisms responsible for those characteristics which are constrained are themselves only partly understood. Despite these challenges a coherent story for the behavior of L and T dwarf condensates is emerging, although our understanding is certainly still not complete. Clouds vary in time and in space and we should perhaps not be suprised that weather prediction is a challenging business.

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# The Ultrasensitivity of Living Polymers

## Abstract

Synthetic and biological living polymers are self-assembling chains whose chain length distributions (CLDs) are dynamic. We show these dynamics are ultrasensitive: even a small perturbation (e.g. temperature jump) non-linearly distorts the CLD, eliminating or massively augmenting short chains. The origin is fast relaxation of mass variables (mean chain length, monomer concentration) which perturbs CLD shape variables before these can relax via slow chain growth rate fluctuations. Viscosity relaxation predictions agree with experiments on the best-studied synthetic system, $`\alpha `$-methylstyrene.

preprint: submitted to Phys. Rev. Lett.

The term “Living Polymers” labels a remarkable and diverse family of self-assembling systems in which molecules or other microscopic units spontaneously aggregate into long chains by continuously adding to chain ends. Their technological and biological importance and their unusual properties as examples of soft condensed matter have driven a large body of experimental and theoretical researchgreer:review ; webster:szwarc:prl\_combo ; schafer:living\_theory\_prl\_combo ; miyakestockmayer:living ; das:greer:living\_7\_mwd\_etal ; zhuang:greer\_kinetics\_etal ; garcia:greer:living\_nonumber ; patten:livingfrp\_prl\_short ; pollard:living\_biorefs\_prl\_combo ; frischknechtmilner:living\_aggregation ; aniansson:micelle\_kinetics\_theory\_expt\_etal ; livingpol\_wlike\_dynamics . The classic synthetic example is ionic living polymerizationgreer:review ; webster:szwarc:prl\_combo ; schafer:living\_theory\_prl\_combo ; miyakestockmayer:living ; das:greer:living\_7\_mwd\_etal ; zhuang:greer\_kinetics\_etal ; garcia:greer:living\_nonumber  where monomers assemble into flexible polymer chains by adding to charged chain ends which remain “alive” even after monomer is consumed, a property widely exploited commercially to synthesize high performance block copolymers and other novel materialswebster:szwarc:prl\_combo . A recent variant on this theme with immense technological potential is living free radical polymerizationpatten:livingfrp\_prl\_short  where ingenious capping-decapping schemes prevent termination and yet permit chain propagation. In the biological world, actin and microtubule filaments, rapidly assembled from the proteins actin and tubulin, are essential to the motility and structural integrity of living cells pollard:living\_biorefs\_prl\_combo .

As polymeric or filamentous materials, the novel and distinguishing feature of these systems is that unlike inert polymers the chains are dynamic or “living” objects whose lengths constantly fluctuate. The polymerization processes are alive: when external conditions change, chain length distributions can respond dynamically and relax to a new equilibrium. This adaptability is the crucial property exploited in both synthetic and natural applications. For example, it enables living cells to rapidly initiate motion or shape changes by altering cellular conditions in response to extracellular signals.

In this letter we study this dynamical responsiveness theoretically. Whilst a rather clear picture of equilibrium properties greer:review ; schafer:living\_theory\_prl\_combo  has been established, living polymer dynamics are far less well understood miyakestockmayer:living ; das:greer:living\_7\_mwd\_etal ; zhuang:greer\_kinetics\_etal ; garcia:greer:living\_nonumber . We focus on the synthetic system which has received most experimental attentiongreer:review ; das:greer:living\_7\_mwd\_etal ; zhuang:greer\_kinetics\_etal ; garcia:greer:living\_nonumber , the anionic living polymer poly $`\alpha `$-methylstyrene (PAMS) and we compare our predictions to PAMS viscosity relaxation measurements at the end of this letter. Aside from its intrinsic importance, PAMS is a model system for more complex cases such as biological living polymers and most of our results are completely general. We use the term “Living Polymers” in the traditional sense greer:review ; webster:szwarc:prl\_combo  to denote systems where (i) the concentration of living chains, $`\rho _{\mathrm{chains}}`$, is fixed for all time by the number of initiators, and (ii) chains grow at their ends only. Related classes include systems where surfactants aggregate into spherical aniansson:micelle\_kinetics\_theory\_expt\_etal  or elongated (“wormlike”) micelles livingpol\_wlike\_dynamics  whose number is not fixed, and whose dynamicsaniansson:micelle\_kinetics\_theory\_expt\_etal ; livingpol\_wlike\_dynamics  are very different.

The principal conclusion of this work is that living polymers are ultrasensitive, i. e. highly dynamically susceptible to small perturbations. Thus a small change in external conditions, inducing a small change in the equilibrium state well-described by a linear susceptibility, has nonetheless a large dynamical effect: intermediate states deviate strongly from equilibrium in that some observables are perturbed in a highly non-linear manner. To quantify this, consider PAMS whose equilibrium chain length distribution (CLD) is close to the broad exponential greer:review ; das:greer:living\_7\_mwd\_etal  predicted by theory, $`\varphi _{eq}(N)e^{N/\overline{N}_{eq}}`$ (see fig. 1), with typical mean number of monomer units per chain $`\overline{N}_{eq}`$ in the range garcia:greer:living\_nonumber  of a few 100 to several 1000. A standard experimental procedure is the “T-jump” where temperature is suddenly changed by an amount $`\mathrm{\Delta }T`$. Consider a PAMS system with $`\overline{N}_{eq}=1000`$ subjected to a small decrease $`\mathrm{\Delta }T=5`$0C as measured by the small parameter $`ϵ\mathrm{\Delta }T/T_00.1`$, where $`T_0T/\mathrm{ln}m_{eq}50`$0C for typical PAMS studies and $`m_{eq}`$ is the equilibrium monomer concentration. The theory presented here predicts the onset after $`3`$ hours of a drastic depletion of short chains. By 10 hours a hole has appeared in the CLD in the region $`0<N\stackrel{<}{}\mathrm{\hspace{0.17em}400}`$ (see fig. 1) and lengths $`N\stackrel{<}{}\mathrm{\hspace{0.17em}100}`$ have virtually disappeared. This is despite the fact that the change in the equilibrium CLD $`\varphi _{eq}(N)`$, which is recovered after $`10^3`$ hours, is destined to be small, $`\delta \varphi _{eq}(N)/\varphi _{eq}(N)=𝒪(ϵ)`$ for all $`N`$. This hole completely invalidates perturbation theory: there are no small perturbations (other than those so tiny as to be beyond typical experimental resolution). This is the essence of ultrasensitivity.

We consider living polymers, such as the PAMS systems studied by Greer and coworkers greer:review ; das:greer:living\_7\_mwd\_etal ; zhuang:greer\_kinetics\_etal ; garcia:greer:living\_nonumber , where monomers spontaneously polymerize below a ceiling temperature $`T_p`$, see fig. 2. The dynamics of $`\varphi _{t,N}`$, the number of chains of length $`N`$, are $`\dot{\varphi }_{t,N}=v^+\varphi _{t,N1}(v^++v^{})\varphi _{t,N}+v^{}\varphi _{t,N+1}`$ where $`v^+=k^+m`$ and $`v^{}`$ are monomer addition and dissociation rates from chain endsliving:kplusvminus\_independentofN\_note  ($`k^+`$ is the addition rate constant). Rearranging terms and taking the continuous limit immediately gives

$`\varphi _t/t=v_t\varphi _t/N+D_t^2\varphi _t/N^2,`$
$`v_t\varphi _t(0)D_t[\varphi _t/N]_{N=0}=0,`$ (1)
where a zero current boundary condition applies at $`N=0`$. Note a second derivative term naturally emerges, with a “diffusivity” coefficient $`D_t(v^++v^{})/2`$, representing fluctuations about the average growth rate or “velocity” $`v_tv^+v^{}`$. Both $`v_t`$ and $`D_t`$ depend on $`\varphi _t`$ (see eq. (7) and following remarks). Setting $`\varphi _t/t=0`$ gives the equilibrium exponential CLD with $`\overline{N}_{eq}=D_{\mathrm{eq}}/v_{\mathrm{eq}}`$. Since $`\overline{N}_{eq}1`$, it follows that in equilibrium $`v^+v^{}`$, the diffusivity is $`D_{\mathrm{eq}}v^{}`$ and the velocity has a small negative value relative to the characteristic scale $`v^{}`$

$$v_{\mathrm{eq}}=v^{}/\overline{N}_{eq}.$$
(2)
This is just sufficient to negate diffusive broadening which would otherwise smear out the equilibrium MWD of width $`\overline{N}_{eq}`$ after time $`\tau _{\mathrm{slow}}=\overline{N}_{eq}^2/D_{\mathrm{eq}}`$; i. e. , $`v_{\mathrm{eq}}\tau _{\mathrm{slow}}=\overline{N}_{eq}`$. Note that since the average velocity over all chains must vanish in equilibrium (there can be no net dissociation to the monomer pool) the $`N>0`$ chains must have a small negative velocity to balance the unique $`N=0`$ chains (consisting of an initiator only, fig. 2) which cannot depolymerize and so have a positive velocity.

A clue as to the origin of ultrasensitivity is already apparent in this equilibrium situation. The significance of eq. (2) is that equilibrium is an extremely delicate balance sustained by a tiny negative velocity easily overwhelmed by even a very small perturbation. Consider an equilibrium system suddenly subjected to a small negative T-jump $`\mathrm{\Delta }T`$, after which the current monomer concentration $`m`$ exceeds its equilibrium value for the new temperature by $`\delta m(\mathrm{\Delta }T/T_0)m_{eq}ϵm_{eq}`$ ($`\delta X`$ denotes the deviation of any property $`X`$ from its equilibrium value, $`X_{\mathrm{eq}}`$, which will eventually be attained after relaxation). This generates a velocity boost $`\delta v=k^+\delta m`$. Since $`k^+m_{eq}v^{}`$ to order $`1/\overline{N}_{eq}`$, we have

$$\delta vϵv^{}.$$
(3)
Comparing eqs. (2) and (3) one sees that despite the smallness of the perturbation, $`ϵ1`$, the delicate balance of velocity and diffusion which characterizes equilibrium is destroyed since the boost $`\delta v`$ greatly exceeds the equilibrium velocity $`v_{\mathrm{eq}}`$. This holds for any $`ϵ`$ above a tiny threshold $`1/\overline{N}_{eq}`$. Immediately after the perturbation, diffusive broadening $`(D_{\mathrm{eq}}t)^{1/2}`$ is still stronger than coherent chain growth $`ϵv^{}t`$. But for times larger than $`t^{}D_{\mathrm{eq}}/ϵ^2v^{}`$ chains grow coherently, i. e. $`\overline{N}`$ will increase until the excess mass $`\delta m`$ held by the monomer reservoir has been transferred to the polymer system and the velocity boost has decayed. In the process the mean chain length increases by an amount $`\delta \overline{N}`$ determined by conservation of total concentration of monomers $`m_{\mathrm{total}}`$:

$`m`$ $`+\rho _{\mathrm{chains}}\overline{N}=m_{\mathrm{total}},\delta \overline{N}/\overline{N}_{eq}=ϵ\theta ^1.`$ (4)
The parameter $`\theta (m_{\mathrm{total}}m_{eq})/m_{eq}(T_pT)/T_0`$ measures distance into the polymerization regime, and will be taken as order unity here. Thus, the entire CLD translates uniformly by $`ϵ\overline{N}_{eq}`$ (fig. 1) in time

$$\tau _{\mathrm{fast}}=\delta \overline{N}/(ϵv^{})=\overline{N}_{eq}/(\theta v^{}).$$
(5)
This leaves behind a hole in the CLD: chains with lengths less than $`ϵ\overline{N}_{eq}`$ have disappeared.

For times beyond $`\tau _{\mathrm{fast}}`$, mass transfer is essentially complete and $`m,v`$ and $`\overline{N}`$ are very nearly relaxed. These are the fast variables. The process of CLD shape relaxation needs much more time. It relies on the far slower diffusive process of incoherent reshuffling of monomers between chains. The time $`\tau _{\mathrm{fill}}`$ needed to fill the hole is simply the diffusion time corresponding to the hole width,

$$\tau _{\mathrm{fill}}=ϵ^2\tau _{\mathrm{slow}}/\theta ^2.$$
(6)
The last process is global CLD shape relaxation on the scale $`\overline{N}_{eq}`$, requiring a diffusion time $`\tau _{\mathrm{slow}}=\overline{N}_{eq}^2/D_{\mathrm{eq}}`$. These events are depicted in fig. 1.

In summary, relaxation to the new equilibrium state involves 3 distinct episodes: (i) coherent chain growth for $`0<t<\tau _{\mathrm{fast}}`$ during which fast mass variables relax, (ii) hole-filling, i. e. recovery of short chains, during $`\tau _{\mathrm{fast}}<t<\tau _{\mathrm{fill}}`$ and (iii) global diffusive relaxation for $`t>\tau _{\mathrm{fill}}`$ during which slow shape variables relax on a timescale $`\tau _{\mathrm{slow}}`$. It is this conflict of timescales which is the origin of the non-linear hole produced by (i): slow diffusive shape equilibration simply cannot keep pace with the rapid deformation produced by mass transfer.

It is interesting to compare this with spherical micelle aggregation which involves two distinct relaxation processes aniansson:micelle\_kinetics\_theory\_expt\_etal . The first entails fast mass exchange between monomers and nearly monodisperse micelles whose number remains essentially fixed due to large aggregate nucleation/dissociation barriers. This is similar to process (i) above. However, a crucial difference is that the number of aggregates can ultimately change and the timescale for this process in consequence depends inversely on total monomer concentration (whereas $`\tau _{\mathrm{fast}}`$ is independent of $`m_{\mathrm{total}}`$). During a second, much slower process, the number of micelles re-equilibrates. This process has no analogue for the living polymers we study.

Let us now briefly outline formal calculations justifying these arguments, starting from eq. (The Ultrasensitivity of Living Polymers). Its steady state solution is the equilibrium Flory-Schultz greer:review  CLD, $`\varphi _{eq}(N)=e^{N/\overline{N}_{eq}}/\overline{N}_{eq}`$ with $`\overline{N}_{eq}m_{\mathrm{total}}\theta /[\rho _{\mathrm{chains}}(1+\theta )]`$. Multiplying eq. (The Ultrasensitivity of Living Polymers) by $`N`$ and integrating one has

$$\dot{v}_t=v_t/\tau _{\mathrm{fast}}D_t\varphi _t(0)/\tau _{\mathrm{fast}},$$
(7)
after using eqs. (4) and (5). Given the CLD $`\varphi _t`$, this relationship determines the time-dependent velocity $`v_t`$ and thence diffusivity $`D_t=v_t/2+v^{}`$. The technical difficulty is that both $`v_t`$ and $`D_t`$ depend non-locally on $`\varphi _t`$, i. e. eq. (The Ultrasensitivity of Living Polymers) is a non-linear and non-local system.

Consider a negative T-jump perturbation inducing, as discussed, a velocity $`v_0ϵv^{}`$ at $`t=0`$. Now, to order $`ϵ`$, $`D_tv^{}D_{\mathrm{eq}}`$. Thus in the velocity kinetics, eq. (7), the $`v_t`$ term is initially much greater than the $`D_t`$ term (provided $`ϵ>1/\overline{N}_{eq}`$). Hence $`v_tϵv^{}e^{t/\tau _{\mathrm{fast}}}`$ in the CLD evolution kinetics eq. (The Ultrasensitivity of Living Polymers) in which, for $`t>t^{}`$, the coherent term wins and the CLD translates along the N axis, $`\varphi _t(N)\varphi _0(N_0^tv_t)`$. Its displacement converges for $`t\tau _{\mathrm{fast}}`$ to $`ϵ\overline{N}_{eq}/\theta `$. In other words the CLD translates and then halts on a timescale $`\tau _{\mathrm{fast}}`$, leaving a hole of size $`ϵ\overline{N}`$ in its wake (see fig. 1). More precisely, the trailing edge broadens by $`(D_{\mathrm{eq}}t)^{1/2}`$ and produces an exponentially small amplitude at the origin, $`\varphi _t(0)e^{t/t^{}}`$.

This concludes episode (i). The linearly related fast variables $`v,m`$ and $`\overline{N}`$ have the same decay kinetics and for $`t\tau _{\mathrm{fast}}`$ have all relaxed. Since the velocity is exponentially small, the CLD kinetics eq. (The Ultrasensitivity of Living Polymers) now describe essentially pure diffusion with reflecting boundary conditions. This is episode (ii): on the timescale $`\tau _{\mathrm{fill}}`$, diffusion fills the hole (see fig. 1) and replenishes the amplitude at the origin, $`\varphi _t(0)(t/\tau _{\mathrm{fill}})^{1/2}e^{4\tau _{\mathrm{fill}}/t}/\overline{N}_{eq}`$. This recovery of $`\varphi _t(0)`$ and the decay of $`v_t`$ imply that at time $`\tau _{\mathrm{qs}}(\tau _{\mathrm{fast}}\tau _{\mathrm{fill}})^{1/2}`$ the two RHS terms in the velocity dynamics eq. (7) become equal. Self-consistently, one finds that thereafter they remain matched, i. e. $`\dot{v}_t`$ is much smaller than either of these terms. Thus from this time onwards, the fast velocity variable (intrinsic timescale $`\tau _{\mathrm{fast}}`$) evolves quasi-statically, enslaved to the slow variable $`\varphi _t(0)`$ (intrinsic timescale $`\tau _{\mathrm{slow}}`$) according to

$$v_tv^{}\varphi _t(0)(t>\tau _{\mathrm{qs}}).$$
(8)
It follows that the velocity now undergoes a recovery as the hole fills up. By $`\tau _{\mathrm{fill}}`$ its magnitude is of order the equilibrium value and can thus compete with diffusion. This heralds the onset of episode (iii): we return to the basic dynamics, eq. (The Ultrasensitivity of Living Polymers), with velocity and diffusion terms now of equal importance. For the first time, relative perturbations of all quantities are now small, and we can apply standard perturbation theory. We find the $`N=0`$ chains recover as $`\delta \varphi _t(0)t^{1/2}`$ up to $`\tau _{\mathrm{slow}}`$ and $`e^{t/\tau _{\mathrm{slow}}}`$ for $`t>\tau _{\mathrm{slow}}`$. During these very late stages the fast variables, which long ago decayed close to equilibrium, are fine-tuned to their true equilibrium values, following $`\varphi _t(0)`$ quasi-statically according to eq. (8).

Note we implicitly assumed sufficient time for the hole to develop before mass transfer is complete, i. e. $`\tau _{\mathrm{fast}}>t^{}`$. This is true provided $`ϵ>ϵ_c=1/\overline{N}_{eq}^{1/2}`$. For very small perturbations $`ϵ<ϵ_c`$ the relative depth of the hole though much greater than $`ϵ`$ is less than unity. Finally, we have studied $`\mathrm{\Delta }T<0`$. The response to a positive $`T`$-jump is similar, but instead of a hole a large peak $`\overline{N}_{eq}ϵ^2`$ develops for small $`N`$, decaying after $`\tau _{\mathrm{fill}}`$.

We tested our theory by numerical integration of coupled ODEs describing the monomer-polymer dynamics. Fig. 1 shows the predicted deep hole developing after a small negative $`T`$-jump. Long time enslavement of fast variables to slow ones is clearly demonstrated (inset).

We conclude by discussing our results and comparing to experiment. We found that, following a perturbation, living polymers relax by adjusting (a) their total mass, proportional to first moment $`\overline{N}`$ and (b) the shape of their CLD. Mass variables are fast (relaxation time $`\tau _{\mathrm{fast}}\overline{N}`$) because monomer-polymer mass transfer is a coherent process. Coherent chain growth, however, cannot affect CLD shape whose relaxation therefore relies on slow diffusion-like fluctuations in chain growth rates (relaxation time $`\tau _{\mathrm{slow}}\overline{N}^2`$.) These timescales are typically separated by 2 or 3 orders of magnitude. In fig. 3 we reproduce viscosity relaxation measurements by Ruiz-Garcia and Greer garcia:greer:living\_nonumber  after small positive and negative temperature jump perturbations of the living polymer PAMS at 6 different temperatures. Now generally we expect viscosity $`\eta c_\varphi \overline{N}^\gamma `$ where $`\gamma `$ is a characteristic exponent garcia:greer:living\_nonumber  and $`c_\varphi `$ depends on the entire CLD, $`\varphi (N)`$, including shape properties. Our theory thus predicts a fast initial relaxation of $`\eta `$ in a time $`\tau _{\mathrm{fast}}`$ followed by a very slow relaxation in $`\tau _{\mathrm{slow}}`$. Now garcia:greer:living\_nonumber  $`\rho _{\mathrm{chains}}2.7\times 10^4`$ gm/cm3 while zhuang:greer\_kinetics\_etal  $`k^+0.2M^1`$ sec-1 was measured to vary by $`10\%`$ over this temperature range. Thus, rewriting $`\tau _{\mathrm{fast}}=1/\rho _{\mathrm{chains}}k^+`$, we predict a constant relaxation time ($`\pm 10\%`$) for all 12 measurements, $`\tau _{\mathrm{fast}}2000`$ seconds. This agrees very closely with experiment (see fig. 3) despite the fact that the observed viscosities varied by an order of magnitude and the mean chain lengths are estimated to vary from almost zero up to several thousand units at the lowest temperature. Note $`\tau _{\mathrm{slow}}=\tau _{\mathrm{fast}}^2v^{}\theta `$ 1 week-1 month, after estimating greer:review  $`\theta 0.5`$ and using $`v^{}=0.1`$ sec-1. The second shape-derived relaxation of $`\eta `$ is therefore unobservably long for this experiment.

Very large temperature quenches were studied in ref. das:greer:living\_7\_mwd\_etal, . $`\overline{N}`$ relaxed faster than the second moment, though it was unclear if $`m`$ and $`\overline{N}`$ were coupled as required by mass conservation, possibly due to ionic aggregationfrischknechtmilner:living\_aggregation . The authors of ref. miyakestockmayer:living,  studied large perturbations theoretically, identifying the timescales $`\tau _{\mathrm{fast}}`$ and $`\tau _{\mathrm{slow}}`$. Their analytical results were valid for short times and very small $`\theta `$.

In this letter we showed that even a small perturbation leads to a non-linear dynamical response. This ultrasensitivity is due to the inability of slow CLD shape variables to keep pace with the fast relaxation of $`\overline{N}`$ which entails simple translation of the CLD leaving a hole or peak at small N. Of all slow variables, the most sensitive is $`\varphi _t(0)`$, the number of $`N=0`$ chains, which becomes exponentially small or massively enhanced. These free initiators also govern the very late fine-tuning of the fast variables $`\overline{N}`$ and $`m`$, the free monomer concentration. Physically, this is because monomers add to chain ends only. But all ends are identical except for the $`N=0`$ chains which cannot shed monomers. Thus $`\varphi _t(0)`$ is the only dynamic polymer property featuring in the kinetics of $`m`$. Given its central role, we propose measurement of the number of free initiators by spectroscopic or other methods as a revealing probe of ultrasensitivity.

This work was supported by the Petroleum Research Fund under grant no. 33944-AC7.


text:
# Scheme for preparation of nonmaximal entanglement between two atomic ensembles

## Abstract

We propose an experimentally feasible scheme to generate nonmaximal entanglement between two atomic ensembles. The degree of entanglement is readily tunable. The scheme involves laser manipulation of atomic ensembles, adjustable quarter- and half-wave plates, beam splitter, polarizing beam splitters, and single-photon detectors, and well fits the status of the current experimental technology. Finally we use the nonmaximally entangled state of ensembles to demonstrate quantum nonlocality by detecting the Clauser-Horne-Shimony-Holt inequality.

PACS number(s): 03.65.Ud, 03.67.-a, 42.50.Gy, 42.50.-p

Quantum entanglement is one of the most striking features of quantum mechanics. The recent surge of interest and progress in quantum information theory allows one to take a more positive view of entanglement and regard it as an essential resource for many ingenious applications such as quantum computation , quantum teleportation , superdense coding , and quantum cryptography . The technology of generation and manipulation of bipartite or multipartite entangled states has been realized in some systems . In most of the above schemes, the subsystems are taken as single-particle. Remarkably, Lukin and Duan et al. have proposed some schemes  for preparation of entanglement, in which atomic ensembles with a large number of identical atoms are used as the basic system. For example, one can use atomic ensembles for generation of substantial spin squeezing  and continuous variable entanglement , and for efficient preparation of Einstein-Podolsky-Rosen (EPR) , Greenberger-Horne-Zeilinger (GHZ) type of maximally entangled states  and W class of maximally entangled states . The schemes have some special advantages compared with other quantum information schemes based on the control of single particles .

In all experimental efforts, it is hard to vary the degree of entanglement, and to produce nonmaximally entangled states without compromising the purity of the state. Nonmaximally entangled states have been shown to reduce the required detector efficiencies for loophole-free tests of Bell inequalities , as well as allowing logical arguments that demonstrate the nonlocality of quantum mechanics without inequalities . Recently, we have proposed some schemes for applications of nonmaximal entanglement . Up to now, nonmaximally entangled states have been deterministically generated with an ion-trap , and with a spontaneous down converter (SPDC) .

Here, we describe an experimental scheme of preparing nonmaximally entangled states based on Raman type laser manipulation of the atomic ensembles and single photon detection which postselects the desired state in a probabilistic fashion.

The basic element of this scheme is an ensemble of many identical alkali atoms with a Raman type $`\mathrm{\Lambda }`$-level configuration shown as Fig. 1, the experimental realization of which can be either a room-temperature dilute atomic gas  or a sample of cold trapped atoms . We continue to use the symbols and corresponding definitions in Refs. . The collective atomic operator is defined as

$$s=\left(1/\sqrt{N_a}\right)\underset{i=1}{\overset{N_a}{}}|g_is|,$$
(1)
where $`N_a1`$ is the total atom number. The Raman transition $`|g|e`$ is coupled by the classical laser and the forward scattered Stokes light comes from the transition $`|e|s`$ . The scheme for preparation nonmaximally entangled states works in the following way (seeing Fig. 2). Here we choose a $`\mathrm{\Lambda }`$ configuration of atomic states of 87Rb by way of example, which is coupled by a pair of optical fields.

There are two light fields with the Rabi frequencies $`\mathrm{\Omega }`$ and $`\omega `$, respectively, which couple pairs of Zeeman sublevels of electronic ground state $`5S_{1/2}`$ 87Rb atoms $`(|g,|s)`$, with magnetic quantum numbers differing by two, via the excited $`5P_{1/2}`$ state . In this case $`|g`$ and $`|s`$ of the simplified three-level model correspond, respectively, to $`|F=2,M_F=2`$ and $`|F=2,M_F=0`$. The atoms in the ensembles are initially prepared to the ground state $`|g`$ through optical pumping. The two ensembles 1 and 2 are illuminated by the synchronized classical laser pulses of right circularly polarized ($`\sigma _{}`$) light. The excitations $`5S_{1/2}`$ $`F=2`$, $`M_F=25P_{1/2}`$ $`F=1`$, $`M_F=1`$ can be transferred to optical excitations. Assume that the light-atom interaction time $`t_0`$ is short so that the mean photon number in the forward scattered Stokes light is much smaller than 1. It is defined in Ref.  an effective single-mode bosonic operator $`a`$ for this Stokes pulse. The whole state of the atomic collective mode and the forward scattering Stokes mode can be written as

$$|\phi =|vac_a|vac_p+\sqrt{p_c}s^+a^+|vac_a|vac_p+o\left(p_c\right),$$
(2)
where $`|vac_a`$ and $`|vac_p`$ denote the vacuum states of atomic ensembles and Stokes light respectively, and $`p_c`$ is the small excitation probability . The forward scattered Stokes pulses of left circularly polarized ($`\sigma _+`$) light from both ensembles are combined at a $`50\%50\%`$ beam splitter (BS) and a single-photon detector click in one of the four detectors, after the quarter-and half-wave plates (QWP and HWP), and polarizing beam splitter (PBS). Adjustable QWP, HWP and PBS allow polarization analysis in any basis, i.e., at any position on the Poincare sphere .

Nonmaximally entangled states are produced simply by adjusting the relative inclination between the optic axes of QWP and HWP. After some filters which filter out the pumping laser pulses, by rotating the optic axis of QWP, the Stokes light is turned to linearly polarized photon and the orientation of the linear polarizer lies in the vertical plane. For an inclination $`\theta _i`$ between the optic axis of HWP and the orientation of the linear polarizer of the Stokes light in arm $`i`$ ($`i=1,2`$), the Stokes photon is $`\mathrm{sin}2\theta _i|H+e^{i\varphi }\mathrm{cos}2\theta _i|V`$, where $`H`$ and $`V`$, respectively, represent the horizontal and vertical polarizations of the photon, and $`\theta _1=\frac{\pi }{4}\theta _2`$. Then the Stokes pulses in both arms are combined at the BS and the output light goes through a PBS, respectively, and a single-photon detector click in one of the four detectors D1, D2, D3 and D4 measures the combination radiation from the samples $`A^+A`$ or $`A^+A^{}`$. Here,

$$A=\alpha a_1+e^{i\varphi _{12}}\beta a_2,$$
(3)
or

$$A^{}=\beta a_1+e^{i\varphi _{12}}\alpha a_2,$$
(4)
where $`\varphi _{12}=\varphi _2\varphi _1`$ is a difference of the phase shift which is fixed by the optical channel connecting the two atomic ensembles, and $`\alpha =\mathrm{sin}2\theta _1`$, $`\beta =\mathrm{cos}2\theta _1`$. That is, if D1 or D3 clicks, the two ensembles are entangled in the form

$$|\psi _{12}=\left(\alpha s_1^++e^{i\varphi _{12}}\beta s_2^+\right)|vac_{12};$$
(5)
if D2 or D4 clicks, the state of the ensembles is

$$|\psi ^{}_{12}=\left(\beta s_1^++e^{i\varphi _{12}}\alpha s_2^+\right)|vac_{12}\text{.}$$
(6)
The subscripts $`1`$ and $`2`$ are used to distinguish the atomic ensemble $`E1`$ and $`E2`$ (seeing Fig. 2). If one excitation is registered, we succeed to entangle the two ensembles in a nonmaximally entangled state. Otherwise, we need to repeat the above steps until we get a click in one of the four detectors.

Now, we consider the efficiency of this scheme, which is usually described by the total generation time. The preparation based on the Raman driving $`|g|e|s`$, succeeds with a controllable probability $`p_c`$ for each Raman driving pulse, and needs to be repeated in average $`1/p_c`$ times for the final successful state generation. In the generation process, the dominant noise is the photon loss, which includes the contributions from the channel attenuation, the spontaneous emissions in the atomic ensembles, the coupling inefficiency of Stokes light into and out of the channel, and the inefficiency of the single-photon detectors which can no perfectly distinguish between one and two photons. All the above noise is described by an overall loss probability $`\eta `$. Due to the noise, the total generation time is represented by $`Tt_0/\left[\left(1\eta \right)p_c\right]`$, where $`t_0`$ is the light-atom interaction time.

Also with the noise, the state of the ensembles is actually described by

$$\rho _{12}=\frac{1}{c+1}\left(c|vac_{12}vac|+|\psi _{12}\psi |\right),$$
(7)
and

$$\rho _{12}^{}=\frac{1}{c+1}\left(c|vac_{12}vac|+|\psi ^{}_{12}\psi ^{}|\right),$$
(8)
where the vacuum coefficient $`c`$ is basically given by the conditional probability for the inherent mode-mismatching noise contribution .

Since the nonmaximally entangled states shown in Eqs. (5) and (6) are entangled in the Fock basis, it is experimentally hard to do certain single-bit rotation. In the following we will show how the nonmaximally entangled states can be used to realize the communication protocols, such as the CHSH detection, with simple experimental configurations.

The first step is to share an EPR type of entangled state

$$|\mathrm{\Psi }_\varphi _{L_1R_1}=\left(s_{L_1}^++e^{i\varphi }s_{R_1}^+\right)/\sqrt{2}|vac_{L_1R_1}$$
(9)
between two distant ensembles $`L_1`$ and $`R_1`$, and the presence of the noise modifies the projected state of the ensembles to

$$\rho _{L_1R_1}=\frac{1}{c+1}\left(c|vac_{L_1R_1}vac|+|\mathrm{\Psi }_\varphi _{L_1R_1}\mathrm{\Psi }_\varphi |\right).$$
(10)
The ensembles $`L_2`$ and $`R_2`$ are prepared in a nonmaximally entangled state $`\rho _{L_2R_2}`$ shown in Eq. (7). The $`\varphi `$-parameters in $`\rho _{L_1R_1}`$ and $`\rho _{L_2R_2}`$ are the same provided that the two states are established over the same stationary channels.

A basis of the “polarization” qubit (in analogy to the language for photons) can be defined from the states $`|H_i=s_{i_1}^+|vac_{i_1i_2}`$, $`|V_i=s_{i_2}^+|vac_{i_1i_2}`$ ($`i=L,R`$). Single-bit rotations in this basis can be done using the phase shift $`\varphi _i`$ together with the corresponding beam splitter operation with the rotation angle $`\theta _i=\varphi _i/2`$ similarly to the manipulations shown in Ref. .

The four ensembles are illuminated by the synchronized classical laser pulses with the frequency $`\omega `$. If the ensemble is in the metastable state after the repumping pulse, the transition $`|e|s`$ will occur determinately. We register only the coincidences of the two-side detectors, so the protocol is successful only if there is a click on each side. Under this condition, the vacuum components in the entangled states and the state $`s_{L_1}^+s_{L_2}^+|vac_{L_1L_2R_1R_2}`$ and $`s_{R_1}^+s_{R_2}^+|vac_{L_1L_2R_1R_2}`$ have no contributions to the experimental results. Then, for the measurement scheme shown by Fig. 3, the state $`\rho _{L_1R_1}\rho _{L_2R_2}`$ is effectively equivalent to the following “polarization” nonmaximally entangled (PNE) state

$$|\psi _{PNE}=\left(\alpha s_{L_2}^+s_{R_1}^++\beta s_{L_1}^+s_{R_2}^+\right)|vac_{L_1L_2R_1R_2}\text{.}$$
(11)
The success probability for the projection is given by $`p=1/\left[4\left(c+1\right)^2\right]`$.

Now, it is clear how to do the Clauser-Horne-Shimony-Holt (CHSH) inequality detection . We define the measurement results to be $`1`$ if D1 or D3 clicks, and $`1`$ if D2 or D4 clicks. Then the quantity

$$E(\varphi _L,\varphi _R)=P_{D_1D_3}+P_{D_2D_4}P_{D_1D_4}P_{D_2D_3}$$
(12)
is the corresponding coefficient of the measurements performed by Side L in the basis rotated by $`\varphi _L/2`$ and by Side R in the basis rotated by $`\varphi _R/2`$. According to the quantum rules

$$E(\varphi _L,\varphi _R)=4\alpha ^2\beta ^2\mathrm{cos}\left(\varphi _L\varphi _R\right),$$
(13)
one can define the quantity $`S`$ composed of the correlation coefficients for which both sides used analysis (phase shift $`\varphi _i`$) of different orientation

$`S`$ $`=`$ $`E(\varphi _L^1,\varphi _R^3)+E(\varphi _L^1,\varphi _R^2)+E(\varphi _L^2,\varphi _R^3)E(\varphi _L^2,\varphi _R^2)`$ (14)
$`=`$ $`8\sqrt{2}\alpha ^2\beta ^2,`$ ()
where $`\varphi _L^1=0`$, $`\varphi _L^2=\frac{\pi }{2}`$, $`\varphi _L^3=\frac{\pi }{4}`$, and $`\varphi _R^1=0`$, $`\varphi _R^2=\frac{\pi }{4}`$, $`\varphi _R^3=\frac{\pi }{4}`$. Any local realistic theory requires $`S<2`$. As Eq. (14) shows, $`S`$ varies with degree of entanglement, for maximally entangled states, the quantity is $`2\sqrt{2}`$. For $`0.479\alpha 0.878`$ or $`0.878\alpha 0.479`$, the inequality is violated.

We have a brief conclusion. In this report, we describe an experimental scheme of generating nonmaximal entanglement between two atomic ensembles. The degree of entanglement is readily tunable. This protocol fits well the status of the current experimental technology. Finally we use the nonmaximally entangled states to measure the CHSH inequality.

We thank L.-M. Duan for helpful discussion, and Y.-S. Zhang and Z.-W. Zhou for stimulating comments. This work was funded by National Fundamental Research Program (2001CB309300), National Natural Science Foundation of China, the Innovation funds from Chinese Academy of Sciences, and also by the outstanding Ph. D thesis award and the CAS’s talented scientist award entitled to Luming Duan.


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# Directional scintillation detector for the detection of the wind of WIMPs

## 1 Introduction

There is substantial evidence that most of the matter in our Galaxy must be dark matter and exist in the form of Weakly Interacting Massive Particles (WIMPs) . WIMPs can be directly detected through elastic scattering with nuclei in a detector. The typical recoil energy is of order of 10 keV. The detector is required to measure about 10 keV nuclear recoil energies and discriminate between nuclear recoils and $`\gamma `$-rays to reject background events.

For reliable detection of WIMPs, conventional searches depend mainly on observing the annual modulation of the counting rate arising from the orbital motion of the earth around the sun and the rotation of the solar system itself around the galactic center. However, this approach is subject to a small modulation amplitude and a large systematic error induced by long-term changes of the condition of the detector and seasonal variations of environmental radiations. For an alternative method, it might be useful to observe the wind of the WIMPs caused by the motion of the earth around the galactic center  (Fig. 1). The effect of the wind is large ($``$ 244 km/s) and a small systematic error can be achieved by means of periodically rotating the detector. To detect the wind of the WIMPs, a directional detector is required.

It is known that organic crystal scintillators such as anthracene and stilbene have directional anisotropies in their scintillation responses to heavy charged particles . Protons and carbon ions are produced internally by WIMPs scattering and the scintillation responses depend on the direction of their motion. These anisotropies can be used to obtain directional information of the WIMPs .

In using scintillation detectors to observe WIMPs, one needs to measure the scintillation efficiency or the quenching factor of the nuclear recoil. For organic crystal scintillators, the anisotropies of the scintillation responses are expressed in the directional variations of the quenching factor.

Measurements of the quenching factor for nuclear recoils have usually been performed with several MeV mono-energetic neutrons produced by nuclear reactions using accelerators . The nuclear recoil was caused by elastic scattering with neutrons instead of WIMPs. We performed the measurement employing a 252Cf neutron source which is easier to handle.

In this paper, we report on the measurement of the quenching factor of a stilbene scintillator as a function of the recoil energy and its dependence on the direction of the proton recoil.

## 2 Experiments

The size of the stilbene crystal was 2 cm $`\times `$ 2 cm $`\times `$ 2 cm. It was purchased from Amcrys-H111URL: http://www.amcrys-h.com. Stilbene is an aromatic hydrocarbon including two benzene nuclei and forms a molecular crystal at room temperature which has an anisotropic structure.

The crystal was covered with GORE-TEX R  to reflect the scintillation light and its cleavage plane was glued to a PMT (H1161-50, Hamamatsu Photonics) with optical grease.

The experimental setup is shown in Fig. 2. We employed a 3.56 MBq 252Cf as a neutron source located 60 cm away from the stilbene scintillator.

The recoil energy $`E_\mathrm{R}`$ is calculated by the kinematics as

$$E_\mathrm{R}=\frac{2\left(1+A\mathrm{cos}^2\theta \mathrm{cos}\theta \sqrt{A^21+\mathrm{cos}^2\theta }\right)}{(1+A)^2}E_\mathrm{n},$$
(1)
where $`\theta `$ is the scattering angle, $`E_\mathrm{n}`$ is the incident energy of the neutron and $`A`$ = (mass of nucleus)/(mass of neutron).

The scattering angle was determined by coincidence measurements between the stilbene scintillator and a liquid scintillator located 65 cm away from the stilbene scintillator at 60 degrees. Since the neutrons from 252Cf source are not monochromatic but have a continuous Maxwellian energy distribution, the incident energy of the neutron needs to be measured by the TOF method between the source and the stilbene scintillator. To determine the timing of the nuclear fission of 252Cf, a prompt $`\gamma `$-ray produced by the fission was detected with the plastic scintillator located by the neutron source. The energy of the scattered neutron was measured by the TOF between the stilbene scintillator and the liquid scintillator.

The quenching factor $`Q`$ is calculated by

$$Q=E_{\mathrm{visible}}/E_\mathrm{R},$$
(2)
where $`E_{\mathrm{visible}}`$ is the measured electron-equivalent energy of the stilbene scintillator as calibrated by $`\gamma `$-rays.

The recoil angle $`\varphi `$ is calculated by

$$\mathrm{cos}^2\varphi =\frac{1+A\mathrm{cos}^2\theta \mathrm{cos}\theta \sqrt{A^21+\mathrm{cos}^2\theta }}{2A}.$$
(3)
For proton recoil, $`\mathrm{cos}\varphi =\mathrm{sin}\theta `$. We measured the quenching factor for two directions of the proton recoil, perpendicular and parallel to the cleavage plane.

A schematic block-diagram of electronics for this experiment is shown in Fig. 3. The pulse height signal of the stilbene scintillator was taken from the dynode output of the PMT, while the timing signal was taken from the anode output. The timing signals of the three scintillators were used for start- and stop-signals for two TACs. The pulses of the amplifier and the TACs were simultaneously recorded with a 4ch digital oscilloscope Tektronix TDS3034B. The peak pulse heights of the signals were sensed and digitized by the oscilloscope and were sent to the PC using an RS232C serial line.

## 3 Analysis

Fig. 4 shows a scatter plot of the observed $`E_{\mathrm{visible}}`$ signal versus TOF between the neutron source and the stilbene scintillator. The events around 0 ns are due to the $`\gamma `$-rays from the neutron source. The proton recoil events were distributed between 20 and 100 ns. Carbon recoil events have lower $`E_{\mathrm{visible}}`$, so that they are not distinguished from background events.

The recoil energy $`E_\mathrm{R}`$ can be calculated from eq. (1) or by subtracting the energy of the scattered neutron from the incident energy calculated from the corresponding TOF. We used the latter method to obtain the recoil energy. The energy of the scattered neutron should be proportional to the incident energy as seen in eq. (1). We rejected background events which did not satisfy this relation within appropriate errors.

Fig. 5 shows a scatter plot of the observed $`E_{\mathrm{visible}}`$ versus energy of the scattered neutrons. In case of the proton recoil, neutrons deposit 75% of their energy in the stilbene, so that we disregarded the events below the dashed line shown in Fig. 5 which have large residual kinetic energies and small $`E_{\mathrm{visible}}`$ for the proton recoil. These events were most probably induced by carbon recoils and accidental coincidence background.

Fig. 6 shows a scatter plot of observed $`E_{\mathrm{visible}}`$ versus expected recoil energy $`E_\mathrm{R}`$. Taking the average of $`E_{\mathrm{visible}}/E_\mathrm{R}`$ of the events in each bin of $`E_\mathrm{R}`$, the measured quenching factor is shown in Fig. 7 as a function of the recoil energy. We measured the quenching factor for two recoil directions, parallel and perpendicular to the cleavage plane. The former is shown by filled squares and the latter by open circles in Fig. 7.

## 4 Results and Discussions

The quenching factor for proton recoils in a stilbene scintillator was measured with a 252Cf neutron source and was found to range from 0.10 to 0.17 with recoil energy from 300 keV to 3 MeV. The measurement was performed for two recoil directions and we confirmed that the quenching factor depends on the recoil direction. It was smaller for the recoils perpendicular to the cleavage plane than for the recoils parallel to it. A measurement of the scintillation responses for $`\alpha `$-particles was reported in Ref. , where the responses for the two directions are qualitatively consistent with our result.

For the carbon recoil, definite data were not obtained because of the low $`E_{\mathrm{visible}}`$ and the large background at low energies which were induced by accidental coincidences from $`\gamma `$-rays. To measure the quenching factor in the low $`E_{\mathrm{visible}}`$ region, we would need to improve the signal-to-background ratio.

For the dark matter search, one can obtain directional information through comparing the data collected with different orientations of the detector. We are planning to measure two energy spectra directing the crystal axes of maximum and minimum scintillation responses toward the direction of the motion of the earth around the galactic center.