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# Creep rupture of viscoelastic fiber bundles

## Abstract

We study the creep rupture of bundles of viscoelastic fibers occurring under uniaxial constant tensile loading. A novel fiber bundle model is introduced which combines the viscoelastic constitutive behaviour and the strain controlled breaking of fibers. Analytical and numerical calculations showed that above a critical external load the deformation of the system monotonically increases in time resulting in global failure at a finite time $`t_f`$, while below the critical load the deformation tends to a constant value giving rise to an infinite lifetime. Our studies revealed that the nature of the transition between the two regimes, i.e the behaviour of $`t_f`$ at the critical load $`\sigma _c`$, strongly depends on the range of load sharing: for global load sharing $`t_f`$ has a power law divergence at $`\sigma _c`$ with a universal exponent of $`0.5`$, however, for local load sharing the transition becomes abrupt: at the critical load $`t_f`$ jumps to a finite value, analogous to second and first order phase transitions, respectively. The acoustic response of the bundle during creep is also studied.

PACS number(s): 46.50.+a, 62.20.Mk

Fiber reinforced composites are of great technological importance due to their very good performance under extreme circumstances. Under high steady stresses these fiber composites may exhibit time dependent failure called creep rupture, which limits their life time and consequently has a high impact on the applicability of these materials for construction elements. Both natural fiber composites like wood  and various types of fiber reinforced composites  show creep rupture phenomena, which have attracted continuous theoretical and experimental interest over the past years. The underlying microscopic failure mechanism of creep rupture is very complex depending on several characteristics of the specific types of materials, and is far from being well understood. From technological point of view, one of the most important aspects of creep rupture is the statistics of life time (or time to failure) as a function of the external steady load, however, only a limited number of systematic experimental works is available for fiber reinforced composites , more information has been accumulated about natural fiber composites . In Ref.  a theoretical model of creep rupture of brittle matrix composites reinforced with time dependent fibers was worked out, where the fibers are assumed to have a finite life time under a constant load in the spirit of the classical model of Coleman . For natural fiber composites a so-called damage accumulation model has been developed, which simply assumes that the time derivative of the accumulated damage depends exponentially on the external load history of the specimen .

In the present letter we study the creep rupture of fiber composites where the fibers have viscoelastic behaviour and the microscopic damage mechanism leading to creep rupture is the strain dependent breaking of fibers under the time evolution of the deformation of the system. Creep failure tests are usually performed under uniaxial tensile loading when the specimen is subjected either to a constant load $`\sigma _\mathrm{o}`$ or to an increasing load (ramp-loading) and the time evolution of the damage process is followed by recording the strain $`\epsilon `$ of the specimen and the acoustic signals emitted by microscopic failure events. In the present study we focus on the general aspects of creep rupture, i.e. the behaviour of the life time of the bundle as a function of the external load, its dependence on the range of load redistribution, furthermore, general aspects of the acoustic response of the bundle are considered without fitting the theoretical results to any specific materials.

In order to work out a theoretical description of creep failure of viscoelastic fiber composites we improve the classical fiber bundle model  which has proven very successful in the study of fracture of disordered materials . Our model consists of $`N`$ parallel fibers having viscoelastic constitutive behaviour. For simplicity, the pure viscoelastic behaviour of fibers is modeled by a Kelvin-Voigt element which consists of a spring and a dashpot in parallel and results in the constitutive equation

$`\sigma _\mathrm{o}=\beta \dot{\epsilon }+E\epsilon ,`$ (1)
where $`\beta `$ denotes the damping coefficient, and $`E`$ the Young modulus of fibers, respectively. Eq. (1) provides the time dependent deformation $`\epsilon (t)`$ of a fiber at a fixed external load $`\sigma _\mathrm{o}`$

$`\epsilon (t)={\displaystyle \frac{\sigma _o}{E}}\left[1e^{Et/\beta }\right]+\epsilon _\mathrm{o}e^{Et/\beta },`$ (2)
where $`\epsilon _o`$ denotes the initial strain at $`t=0`$. It can be seen that $`\epsilon (t)`$ converges to $`\sigma _\mathrm{o}/E`$ for $`t\mathrm{}`$, which implies that the asymptotic strain fulfills Hook’s law.

If no fiber failure occurs Eq. (2) would fully describe the time evolution of the system. Motivated by the experimental observations of the acoustic response  of fiber composites during creep, we introduce a strain controlled failure criterion to incorporate damage in the model: a fiber fails during the time evolution of the system if its strain exceeds a damage threshold $`\epsilon _d`$, which is an independent identically distributed random variable of fibers with probability density $`p(\epsilon _d)`$ and cumulative distribution $`P(\epsilon _d)={\displaystyle _0^{\epsilon _d}}p(x)𝑑x`$. Similar strain controlled breaking was recently used in Ref. . Due to the validity of Hook’s law for the asymptotic strain values, the formulation of the failure criterion in terms of strain instead of stress implies that under a certain steady load the same amount of damage occurs as in the case of stress controlled failure, however, the breaking of fibers is not instantaneous but distributed over time. When a fiber fails its load has to be redistributed to the intact fibers. As the simplest approach, we assume global load sharing , i.e. after a failure event the excess load is equally distributed among the intact fibers, and hence, at a certain strain $`\epsilon `$ the load on the surviving fibers of the number $`N_s(\epsilon )`$ can be cast into the form $`\sigma (\epsilon )=\sigma _\mathrm{o}N/N_s(\epsilon )=\sigma _\mathrm{o}/(1P(\epsilon ))`$. The time evolution of the system under a steady external load $`\sigma _o`$ is finally described by the equation

$`{\displaystyle \frac{\sigma _\mathrm{o}}{1P(\epsilon )}}=\beta \dot{\epsilon }+E\epsilon ,`$ (3)
where the viscoelastic behaviour of fibers is coupled with the failure of fibers in a global load sharing framework.

For the behaviour of the solutions of Eq. (3) two distinct regimes can be distinguished depending on the value of the external load $`\sigma _\mathrm{o}`$: When $`\sigma _\mathrm{o}`$ is below a critical value $`\sigma _\mathrm{c}`$ Eq. (3) has a stationary solution $`\epsilon _s`$, which can be obtained by setting $`\dot{\epsilon }=0`$

$`\sigma _\mathrm{o}=E\epsilon _s[1P(\epsilon _s)].`$ (4)
It means that until this equation can be solved for $`\epsilon _s`$ at a given external load $`\sigma _\mathrm{o}`$, the solution $`\epsilon (t)`$ of Eq. (3) converges to $`\epsilon _s`$ when $`t\mathrm{}`$, and no macroscopic failure occurs. However, when $`\sigma _\mathrm{o}`$ exceeds the critical value $`\sigma _c`$ no stationary solution exists, furthermore, $`\dot{\epsilon }`$ remains always positive, which implies that for $`\sigma >\sigma _c`$ the strain of the system $`\epsilon (t)`$ monotonically increases until the system fails globally at a time $`t_f`$.

In the regime $`\sigma _\mathrm{o}\sigma _\mathrm{c}`$ Eq. (4) also provides the asymptotic constitutive behaviour of the fiber bundle which can be measured by controlling the external load $`\sigma _\mathrm{o}`$ and letting the system relax to $`\epsilon _s`$. It follows from the above argument that the critical value of the load $`\sigma _c`$ is the static fracture strength of the bundle which can be determined from Eq. (4) as $`\sigma _c=E\epsilon _c[1P(\epsilon _c)]`$, where $`\epsilon _c`$ is the solution of the equation $`d\sigma _\mathrm{o}/d\epsilon _s|_{\epsilon _\mathrm{c}}=0`$, as shown by Sornette . Since $`\sigma _\mathrm{o}(\epsilon _\mathrm{s})`$ has a maximum of the value $`\sigma _\mathrm{c}`$ at $`\epsilon _\mathrm{c}`$, in the vicinity of $`\epsilon _\mathrm{c}`$ it can be approximated as

$`\sigma _\mathrm{o}\sigma _\mathrm{c}A(\epsilon _\mathrm{c}\epsilon _s)^2,`$ (5)
where the multiplication factor $`A`$ depends on the probability distribution $`P`$. A complete description of the system can be obtained by solving the differential equation Eq. (3). After separation of variables the integral arises

$`t=\beta {\displaystyle 𝑑\epsilon \frac{1P(\epsilon )}{\sigma _\mathrm{o}E\epsilon \left[1P(\epsilon )\right]}}+C,`$ (6)
where the integration constant $`C`$ is determined by the initial condition $`\epsilon (t=0)=0`$.

The creep rupture of the viscoelastic bundle can be interpreted so that for $`\sigma _\mathrm{o}\sigma _\mathrm{c}`$ the life time (or the time to failure) of the bundle is infinite $`t_f=\mathrm{}`$, while above the critical load $`\sigma _\mathrm{o}>\sigma _\mathrm{c}`$ global failure occurs at a finite time $`t_f`$, which can be determined by evaluating the integral Eq. (6) over the whole domain of definition of $`P(\epsilon )`$. From the theoretical and experimental point of view it is very important how $`t_f`$ depends on the external load above $`\sigma _\mathrm{c}`$. When $`\sigma _\mathrm{o}`$ is in the vicinity of $`\sigma _\mathrm{c}`$, i.e. $`\sigma _\mathrm{o}=\sigma _\mathrm{c}+\mathrm{\Delta }\sigma _\mathrm{o}`$, where $`\mathrm{\Delta }\sigma _\mathrm{o}<<\sigma _\mathrm{c}`$, it can be expected that the curve of $`\epsilon (t)`$ falls very close to $`\epsilon _\mathrm{c}`$ for a very long time and the breaking of the system occurs suddenly. Hence, the total time to failure, i.e. the integral in Eq. (6), is dominated by the region close to $`\epsilon _\mathrm{c}`$ when $`\mathrm{\Delta }\sigma _\mathrm{o}`$ is small. Making use of the power series expansion Eq. (5) the integral in Eq. (6) can be rewritten as

$`t_f\beta {\displaystyle 𝑑\epsilon \frac{1P(\epsilon )}{\mathrm{\Delta }\sigma _\mathrm{o}A(\epsilon _\mathrm{c}\epsilon )^2}},`$ (7)
which has to be evaluated over a small $`\epsilon `$ interval in the vicinity of $`\epsilon _\mathrm{c}`$. After performing the integration it follows

$`t_f(\sigma _\mathrm{o}\sigma _\mathrm{c})^{1/2},\text{for}\sigma _\mathrm{o}>\sigma _\mathrm{c}.`$ (8)
Thus, $`t_f`$ has a power law divergence at $`\sigma _\mathrm{c}`$ with a universal exponent $`\frac{1}{2}`$ independent of the specific form of the disorder distribution $`p(\epsilon )`$.

For the purpose of explicit calculations we considered the case of a uniform distribution of the damage thresholds between $`0`$ and a maximum value $`\epsilon _m`$, thus, $`p(\epsilon _d)=1/\epsilon _m`$ and $`P(\epsilon _d)=\epsilon _d/\epsilon _m`$. The stationary solution, the critical load and the corresponding critical strain can be obtained as $`\sigma _\mathrm{o}=E\epsilon [1\epsilon /\epsilon _m]`$, $`\sigma _c=E\epsilon _m/4`$, $`\epsilon _c=\epsilon _m/2`$, respectively. Finally, the solution of the integral Eq. (6) taking the initial condition also into account can be cast into the implicit form

$`t={\displaystyle \frac{\beta }{2E}}`$ $`\{{\displaystyle \frac{1}{\sqrt{1\frac{4\sigma _\mathrm{o}}{E\epsilon _m}}}}\mathrm{ln}{\displaystyle \frac{\frac{\epsilon }{\epsilon _m}\left[1+\sqrt{1\frac{4\sigma _\mathrm{o}}{E\epsilon _m}}\right]+\frac{2\sigma _\mathrm{o}}{E\epsilon _m}}{\frac{\epsilon }{\epsilon _m}\left[1\sqrt{1\frac{4\sigma _\mathrm{o}}{E\epsilon _m}}\right]+\frac{2\sigma _\mathrm{o}}{E\epsilon _m}}}`$ (10)
$`\mathrm{ln}{\displaystyle \frac{E\epsilon ^2E\epsilon _m\epsilon +\sigma _\mathrm{o}\epsilon _m}{\sigma _\mathrm{o}\epsilon _m}}\}`$
for $`\sigma _\mathrm{o}<\sigma _c`$ (below the critical point), and

$`t={\displaystyle \frac{\beta }{E}}\{{\displaystyle \frac{1}{\sqrt{\frac{4\sigma _\mathrm{o}}{E\epsilon _m}1}}}[arctg{\displaystyle \frac{2\frac{\epsilon }{\epsilon _m}1}{\sqrt{\frac{4\sigma _\mathrm{o}}{E\epsilon _m}1}}}`$ (11)
$`arctg{\displaystyle \frac{1}{\sqrt{\frac{4\sigma _\mathrm{o}}{E\epsilon _m}1}}}]{\displaystyle \frac{1}{2}}\mathrm{ln}{\displaystyle \frac{E\epsilon ^2E\epsilon _m\epsilon +\sigma _\mathrm{o}\epsilon _m}{\sigma _\mathrm{o}\epsilon _m}}\}`$ (12)
for $`\sigma _\mathrm{o}>\sigma _c`$ (above the critical point). The behaviour of this analytic solution is illustrated in Fig. 1 for several different values of $`\sigma _\mathrm{o}`$.

The time to failure $`t_f`$ can be determined by setting $`\epsilon =\epsilon _m`$ in Eq. (11), which results in the form

$`t_f{\displaystyle \frac{\beta \pi }{2}}\sqrt{{\displaystyle \frac{\epsilon _m}{E}}}\left(\sigma _\mathrm{o}\sigma _c\right)^{1/2},`$ (13)
in accordance with the above general arguments.

A further important general property of $`\epsilon (t)`$ that can be deduced from Eqs. (3,6) is that at the time to failure $`t_f`$ the deformation rate $`d\epsilon /dt`$ diverges. For disorder distributions $`P(\epsilon )`$ defined in a finite interval the exponent is universal $`d\epsilon /dt(t_ft)^{1/2}`$.

In order to obtain information about the gradual breaking of fibers during the creep process, in the experiments the acoustic signal emitted by breaking events in a short time interval is investigated. In our fiber bundle model the number of fibers $`N_b(t)`$ which have been broken up to time $`t`$ can be determined as $`N_b(t)=NP(\epsilon (t))`$, and hence, its derivative provides the quantity

$`{\displaystyle \frac{1}{N}}{\displaystyle \frac{N_b}{t}}={\displaystyle \frac{dP}{d\epsilon }}{\displaystyle \frac{d\epsilon }{dt}}={\displaystyle \frac{p(\epsilon )E\epsilon }{\beta }}\left[{\displaystyle \frac{\sigma _\mathrm{o}}{E\epsilon \left[1P(\epsilon )\right]}}1\right],`$ (14)
which is a measure for the acoustic response. The behaviour of Eq. (14) for the uniform distribution is illustrated in Fig. 2, where it can be observed that the acoustic activity, i.e. fiber breaking, practically disappears in the plateau region of $`\epsilon (t)`$ (compare to Fig. 1), however, it diverges at $`t_f`$ due to the diverging deformation rate.

Since during a creep test $`\epsilon (t)`$ is monitored from which $`d\epsilon /dt`$ can be calculated, furthermore, $`N_b/t`$ is measured by means of acoustic emission techniques, Eq. (14) makes possible to determine experimentally the distribution of the failure thresholds $`p(\epsilon _d)`$.

To complement the predictions of the analytic approach Monte Carlo simulations of the failure process have been performed using global load sharing (GLS) and local load sharing (LLS) for the stress redistribution. The GLS simulation of the creep failure process of a bundle of $`N`$ fibers proceeds as follows: $`(i)`$ random breaking thresholds $`\epsilon _i,i=1,\mathrm{},N`$ were chosen according to a probability distribution $`p`$, then the thresholds were put into increasing order. $`(ii)`$ Since the fibers break one-by-one, the actual load on the fibers after the failure of $`i`$ fibers is $`\sigma _i=\sigma _oN/(Ni)`$ where $`i=0,\mathrm{},N1`$, and the time between the breaking of the $`i`$th and $`i+1`$th fibers reads as $`t_i={\displaystyle \frac{\beta }{E}}\mathrm{ln}\left[\left(\epsilon _{i+1}{\displaystyle \frac{\sigma _i}{E}}\right)/\left(\epsilon _i{\displaystyle \frac{\sigma _i}{E}}\right)\right].`$ $`(iii)`$ Finally, the time as a function of $`\epsilon `$ can be obtained as $`t(\epsilon _i)=_{j=0}^it_j(\epsilon _j)`$ from which $`\epsilon _i(t)`$ can be determined. The time to failure $`t_f`$ of a finite bundle is defined as the time of the failure of the last fiber. To test the validity of the power law behaviour of $`t_f`$ given by Eq. (8) simulations were performed with various distributions in the framework of GLS. The results are presented in Fig. 3 where an excellent agreement of the simulations and the analytic results can be observed. The macroscopic strain of the system $`\epsilon (t)`$ and the acoustic response obtained by simulations was also found to be in agreement with the analytic results.

To clarify how the damage process and the behaviour of $`t_f`$ is affected by the range of interaction among fibers, i.e. by the range of load sharing we performed simulations with LLS on a square lattice of $`200\times 200`$ sites, redistributing the load of the failed fiber on its nearest neighbors. The critical load $`\sigma _c`$ was first determined as the static fracture strength of a dry fiber bundle with LLS assuming perfectly elastic behaviour for the fibers. Comparing the results of the LLS simulations to the global load sharing results it was observed that above $`\sigma _c`$ the failure of the viscoelastic bundle occurs much more abruptly than in the case of GLS.

Varying $`\sigma `$ as a control parameter the two regimes of the creep rupture process are characterized by an infinite life time below $`\sigma _c`$ and by a finite one above the critical point. The nature of the transition between the regimes in the global and local load sharing models can be characterized by studying $`1/t_f`$ as a function of the control parameter $`\sigma `$. In Fig. 4 it can be observed that below the critical point, when no global failure occurs, $`1/t_f`$ is zero, while above $`\sigma _c`$ it takes a finite value for both LLS and GLS. However, the behaviour of $`1/t_f`$ in the vicinity of $`\sigma _c`$ is completely different in the two cases, for GLS the transition is continuous, while for LLS $`1/t_f`$ has a finite jump, analogously to a second and first order phase transition, respectively.

Summarizing, we studied the creep rupture of viscoelastic fiber composites by enhancing the classical fiber bundle model. Varying the external load, two regimes of the creep process were revealed characterized by an infinite life time below, and by a finite one above the critical load. The transition between the two regimes was found to be continuous for global load sharing, while it is abrupt for localized load redistribution, analogous to a second and first order phase transition, respectively.

We are grateful to S. Aicher, G. Dill-Langer, F. Wittel, F. Tzchichholz, and to J. Aström for valuable discussions. This work was supported by the project SFB381. F. Kun acknowledges financial support of the Alexander von Humboldt Foundation (Roman Herzog Fellowship) and of the Bólyai János Fellowship of the Hungarian Academy of Sciences.


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# First Investigation of the Clustering Environment of Damped Lyman 𝛼 Absorbers at 𝑧≃41

## 1 Introduction

Galaxy formation is one of the great unsolved problems in astrophysics. We have clear evidence that many galaxies were in place at redshifts of $`34`$ but little knowledge of how or when they formed. Using Lyman-break imaging techniques, Steidel et al. (1996) discovered a large sample of $`z`$ $``$ 3 galaxies with rest-frame ultraviolet luminosities $`L_{UV}`$ $`>`$ 10$`L_{}`$ and comoving number density comparable to that of $`L_{}`$ galaxies today. These Lyman-break galaxies (LBGs) exhibit surprisingly strong clustering for $`z3`$, with overdensities $`\delta \rho /\rho `$ $`>`$ 3 and comoving correlation length $`r_0`$ $``$ 5$`h^1`$ Mpc (Adelberger et al. 1998). In hierarchical models of structure formation such as $`\mathrm{\Lambda }`$CDM, the LBGs will undergo significant merging and should be even more clustered, rare massive galaxies today.

The damped Lyman $`\alpha `$ absorption systems (DLAs), on the other hand, are thought to be the progenitors of typical present-day galaxies (Wolfe et al. 1986; Kauffmann 1996). We therefore must learn about the mass and environment of high-redshift DLAs if we want to understand the formation of typical galaxies like the Milky Way. The damped Lyman $`\alpha `$ absorbers are dense clouds of neutral hydrogen seen in absorption along the line of sight to distant quasars. They appear to be drawn from the bulk of the protogalactic mass distribution; this conclusion is supported by the agreement between the comoving mass density of neutral gas at $`z>2`$ and the mass density of visible stars in current galaxy disks (Wolfe et al. 1995). However, the total gas content cannot distinguish CDM scenarios in which DLAs are numerous low-mass protogalaxies from passive evolution models in which the DLAs are more rarely occurring massive objects. Determining the mass of individual DLAs is also critical for testing models of galaxy formation within the CDM paradigm. This determination cannot be performed using the absorption characteristics of the DLAs, as the comoving density of DLAs cannot be determined without knowing their typical cross-sectional area. One way to distinguish among models for the DLAs is to measure the kinematics of the gas (Prochaska & Wolfe 1997, 1998; Wolfe & Prochaska 2000a, b). This paper describes an independent method which seeks to determine the mass of the DLAs by investigating the extent to which they cluster with LBGs. Since DLAs are predicted by hierarchical cosmologies to be rather weak in emission, and observation is consistent with this (Steidel et al. 1995), it may be easier to constrain their mass using large-scale structure techniques than by searching for their emission (see Wolfe 1993).

Section 2 describes the theoretical basis for our investigation of the cross-correlation of DLAs and LBGs. Imaging observations and photometric data reduction are described in §3, and our multislit spectroscopy is presented in §4. We discuss the search for emission from the DLAs themselves in §5, search for evidence of clustering with nearby LBGs in §6, and discuss our results in §7.

## 2 Large-Scale Structure at High Redshift

Hierarchical models of structure formation predict that the most massive galaxies tend to form in regions of unusually high density, whereas low-mass galaxies are more uniformly distributed in space. This leads to an enhancement in the clustering of high-mass galaxies, referred to as bias, since they typically form near each other in rare overdense regions. Clustering thus provides a way to probe the mass distribution of DLAs; if there is a significant overdensity of LBGs near damped Lyman $`\alpha `$ absorbers it indicates that the DLAs reside in massive dark halos. If, on the other hand, the DLAs are preferentially found in regions with an underdensity of LBGs, it would argue that some environmental effect, perhaps ionizing radiation from massive stars in the LBGs (see Steidel et al. 2000), prevents the occurrence of large column densities of neutral hydrogen in overdense regions. The expected result in hierarchical cosmologies is intermediate; DLAs are predicted to be low-mass objects and should be found in both the (proto)clusters and the field with typically only a small enhancement of LBGs nearby.

While the cross-correlation of galaxies and clusters has been studied at low redshift (e.g. Mo et al. 1993), these objects can also be studied through their autocorrelation. The inevitable sparse sampling of DLAs and other absorption systems caused by only being able to detect them on the line of sight towards quasars or bright galaxies makes it very difficult to measure their autocorrelation. Hence, the cross-correlation is the best, and perhaps only, way to study the bias of DLAs. Another advantage is that the cross-correlation of DLAs and LBGs can be established without detecting emission from the galaxy causing the damped Lyman $`\alpha `$ absorption.

The probability of finding an LBG in a small volume $`dV`$ a distance $`r`$ from a known DLA is enhanced versus the average density of LBGs,

$$dP_{LBG}=[1+\xi _{DL}(r)]\rho _{LBG}dV,$$
(1)
where $`\xi _{DL}`$ is the cross-correlation function of DLAs and LBGs. On scales where linear bias is a good model, the cross-correlation of any two classes of objects is determined by multiplying the dark matter correlation function $`\xi (r)`$ by the product of the bias factors of each class:

$$\xi _{12}(r)=b_1b_2\xi (r).$$
(2)
The bias of a set of collapsed objects of a given mass can be determined using the extended Press-Schechter method (see Mo et al. 1996 ). The autocorrelation of LBGs ($`\xi _{LL}`$) is known at $`z=3`$ (Adelberger et al. 1998) but has not yet been determined at $`z=4`$ (Steidel et al. 1999, hereafter S99), probably due to the increased difficulty of obtaining redshifts at $`z4`$. The bias of other high-redshift objects such as quasars, radio galaxies, or Lyman $`\alpha `$ emitters can also be determined using the cross-correlation function.

## 3 Imaging and Photometry

We took deep BRI images of the field around the $`z=4.37`$ quasar BR 0951$``$04 (Storrie-Lombardi et al. 1996) with the LRIS instrument (Oke et al. 1995) at the Keck Observatory. This field was chosen because there are two DLAs along the line of sight towards BR 0951$``$04, at $`z=3.86`$ and $`z=4.20`$ (Storrie-Lombardi & Wolfe 2000). Table 1 lists the exposure time and final depth in each filter. Images were reduced using a mix of standard IRAF routines and customized code. The final images cover a $`5^{}\times 7^{}`$ field. Photometry was performed on the R image using SExtractor (Bertin & Arnouts 1996) and then a custom code was used to extract photometry from the final B and I images using the exact apertures selected in R. Prochaska et al. (in preparation) describe our data reduction methods in greater detail and make our photometric catalog and images public.

We modified the $`G\mathrm{}i`$ color selection criteria of S99 for our Johnson-Cousins BRI filter set.111Our filter set corresponds closely to their custom set except for an overall 200Å ($`\mathrm{\Delta }z0.2`$) shift bluewards in B and R, allowing the approximation (B$``$R)$`{}_{AB}{}^{}=`$($`G\mathrm{}`$). Because our I filter is close to theirs in effective wavelength, our (R$``$I)AB colors should be roughly 1.6 times their ($`\mathrm{}i`$) colors. Objects located in the region of color-color space bounded by (B$``$R)$`{}_{AB}{}^{}2.0`$, (B$``$R)$`{}_{AB}{}^{}1.2`$(R$``$I)$`{}_{AB}{}^{}+1.6`$, and (R$``$I)$`{}_{AB}{}^{}1.0`$, have a high probability of being Lyman-break galaxies at $`z>3.5`$. We have also used photometric redshifts (see Yahata et al. 2000) and have found at least one LBG that would have been missed using only the two-color region of S99. Almost all of the color-selected candidates are identified by the photometric redshift technique as having a high probability of being at $`3.5<z<4.5`$. The photometric redshift method accounts for the individual photometric uncertainties in the B,R, and I fluxes of each object and compares the object fluxes with a set of template spectra rather than a single two-color region. Carefully designed seven-color photometric redshift schemes yield a scatter of $`\mathrm{\Delta }z=0.2`$ at these redshifts (Hogg et al. 1998). It should therefore be impossible for photometric redshift selection to create a redshift distribution as narrow as the $`\mathrm{\Delta }z0.04`$ ($``$2000 km/s) redshift spikes seen by Adelberger et al. (1998).

We visually inspected all candidate galaxies in our images and rejected roughly half of the initial candidates for having suspect photometry. Many of the rejected objects lied near the edge of our imaging field in regions of lower signal-to-noise. It is no surprise that such a high fraction of the initial candidates had suspect photometry, as the color selection region is sparsely populated and therefore the small fraction of low-redshift galaxies scattered into the color-selection region by photometric errors can easily comprise a large fraction of the candidates. Bright (I$`<23`$) objects with clearly non-stellar morphology were rejected as low-redshift interlopers, but bright stellar objects were retained in case they were new quasars or lensing-magnified LBGs; most LBGs will look similar to point sources at the resolution of our images.

## 4 Spectroscopy and Redshift Determination

We performed longslit spectroscopy of two objects near BR 0951$``$04 and multislit spectroscopy of this field with four different slitmasks, all with 1.5′′ width slitlets and the 150 line/mm grating (30 Å resolution) on Keck-LRIS. Table 1 lists details of our observations. Each slitmask targeted about 15 candidate objects. The entire LRIS imaging field was covered using 2 slitmasks (termed left and right) that overlap in the region near the quasar. These masks were redesigned for the March 2000 run to eliminate slits on objects whose redshifts were already determined and to add slits on additional candidate LBGs. We used a GG495 dichroic filter to block second order light in December 1999 but decided against this in the subsequent run because wavelengths below 4950 Å can be used to check for the presence of the Lyman limit. The spectroscopic data were reduced using standard IRAF techniques called by a customized version of the BOGUS code222Available at http://zwolfkinder.jpl.nasa.gov/$``$stern/homepage/bogus.html. The functions response (halogen lamp spectrum fitting), background (sky subtraction) and apall (spectrum extraction) were performed interactively following the multislit data reduction cookbook available at http://mamacass.ucsd.edu/people/gawiser/cookbooks.html . Redshifts were determined interactively using a customized PGPLOT routine which compared the measured spectra with templates of expected absorption (and emission) lines for LBGs (Steidel et al. 2000; Lowenthal et al. 1997) and E+A galaxies (Zabludoff et al. 1996). Gawiser et al. (in preparation) describe our spectroscopic data reduction in greater detail.

We obtained spectra of 35 candidate galaxies in the field of BR 0951$``$04 (see Table 2). Eight candidates turn out to be galaxies at $`z>3.5`$, thirteen appear to be low-redshift interlopers (typically ellipticals at $`z0.5`$) and fourteen have inconclusive spectra. Our color-selected sample with I$`{}_{AB}{}^{}25`$ is directly comparable to the objects observed by S99. We find 0.5 candidates per sq. arcmin, twice the candidate density of S99; the difference is unlikely to be caused solely by Poisson fluctuations given that there are 19 objects in this category in Table 2. Our rate of determining redshifts for objects observed spectroscopically is comparable to S99, and the fraction of candidates identified as interlopers, i.e. at $`z<3.5`$, is higher but very sensitive to small-number statistics at present. We will revisit this comparison once a larger sample of BRI-selected galaxies is available.

Figure 1 shows the two-color diagram of all 2254 objects with I$`{}_{AB}{}^{}<25.5`$ detected in the field with the status of LBG candidates shown. Table 3 lists photometry and photometric redshift information on each $`z>3.5`$ galaxy with its best-fit redshift and uncertainty. The photometric redshifts based on BRI alone are impressively accurate for the confirmed high-redshift galaxies, with a dispersion of $`\sigma =0.18`$, including three cases where $`z_{phot}`$ differs from the spectroscopic redshift by only 0.01. However, adding in the catastrophic failures where $`z0.5`$ galaxies were assigned photometric redshifts $`z_{phot}4`$ would drastically increase this dispersion. Adding near-infrared (JHK) or optical Z-band photometry would be quite helpful in discriminating against these intrinsically-red low-redshift interlopers.

The increased fraction of interlopers among candidates selected primarily by photometric redshift confirms that the S99 color selection region is the most efficient place to find LBGs. However, we differ from S99 in one major respect. We do not assume that the spectra with insufficient signal-to-noise for redshift determination are drawn from the same population of objects as those with identified redshifts. Thus there is a factor of two uncertainty in the number abundance of color-selected $`z>3.5`$ galaxies, both here and in S99, caused by almost half of the candidates lacking redshift identifications. Extrapolating from the observed color distribution of LBGs at $`z=3`$, S99 predict that roughly half of the $`z=4`$ LBGs will lie outside of the color selection region. The failure of photometric redshifts to find these LBGs implies either that this incompleteness has been overestimated or that the photometric redshift technique needs to be modified to better identify LBGs with unusual colors.

Figure 2 shows the rest-frame spectra of the confirmed $`z>3.5`$ galaxies. These spectra show the typical mix of Lyman $`\alpha `$ emission (G4,G6,G7) and Lyman $`\alpha `$ absorption (G1,G2,G8) as well as two vague suggestions of emission within a broad absorption trough (G3,G5). The signal-to-noise is generally quite poor, illustrating why I=25 is usually considered the limit for ground-based optical spectroscopy.

## 5 Search for Emission from Damped Lyman $`\alpha `$ Absorbers

At $`z4`$, Lyman-break galaxies found within a 10′′ radius of the quasar may be the source of damped Lyman $`\alpha `$ absorption. This radius corresponds to the maximum impact parameter ($`100`$ kpc) inferred from absorption line statistics in the passive evolution model (Storrie-Lombardi & Wolfe 2000; Bunker et al. 1999). If DLAs represent formed disk galaxies as postulated by Wolfe (1997), we should be able to detect emission from up to $`20\%`$ of them at R$`25`$ (Maller et al. 2000). However, in hierarchical models of structure formation, a much higher fraction of DLAs are expected to be too dim and/or too close to the quasar to yield detectable emission (Haehnelt et al. 1998, 2000). Our survey hopes to differentiate between these hypotheses; if emission from DLAs is found repeatedly at large impact parameters or high luminosity it will represent a serious conflict with the predictions of hierarchical cosmology.

We performed a complete survey for possible emission from DLAs on the line of sight toward the quasar down to I$`{}_{AB}{}^{}=26`$ at angular distances up to $`10^{\prime \prime }`$, although the PSF of the quasar hampers our survey at angles less than $`2^{\prime \prime }`$ where hierarchical cosmology predicts that the emission from most DLAs will be found. We identified three objects within $`10^{\prime \prime }`$ of the QSO line-of-sight that had a reasonable chance of being at high redshift (our selection criteria were less stringent in this region). One of these, G1, meets the color selection criteria but has I$`{}_{AB}{}^{}=25.7`$ and appears to have a redshift of $`3.69`$. Although G1 is $`10^{\prime \prime }`$ from the QSO, it may be responsible for the $`z=3.703`$ absorption system seen in SiIV and CIV (Storrie-Lombardi et al. 1996). The second nearby object appears to be a low-redshift interloper, and the third has inconclusive redshift. Another color-selected galaxy, G2 at $`z=3.81`$, lies $`15^{\prime \prime }`$ ($`200`$ kpc) from the QSO and may be responsible for the $`z=3.818`$ absorption system seen in Lyman $`\alpha `$ and CIV in our Keck-HIRES spectrum of BR 0951$``$04 (Prochaska & Wolfe 1999). It will be interesting to determine the fraction of galaxies detected in both emission and absorption as a function of distance from the quasar line-of-sight. We have not detected emission physically associated with either of the damped Lyman $`\alpha `$ absorbers towards BR 0951$``$04 spectroscopically, but all of the models predict that a larger sample is needed before we should expect to find an LBG physically associated with a DLA.

## 6 Clustering Analysis

Figure 3 shows the redshift histogram of objects in the field of BR 0951$``$04, with a binsize of $`\mathrm{\Delta }z=0.05`$ ($`10h^1`$ Mpc) chosen because most of our redshift uncertainties are smaller than this value. We chose to place the $`z=3.86`$ DLA in the center of a bin in order to maximize the chance of finding an overdensity (or underdensity) of LBGs near the DLA if one exists. However, the results described below are not altered by shifting the bin locations.

There are eight confirmed LBGs in the BR 0951$``$04 field, so the search for clustering is plagued by small number statistics. Before trying to determine the amplitude of a cross-correlation function, it makes sense to ask if any clustering has been observed that is inconsistent with poisson fluctuations about the expected redshift distribution of LBGs. The expected redshift distribution refers to the multiplication of the true redshift distribution of LBGs on an average line of sight times the observational selection function. While the observational selection function can be simulated (see S99), the true redshift distribution of LBGs is unknown, so it is necessary to determine the expected redshift distribution empirically. We have not yet observed a sufficient number of LBGs to determine how our expected redshift distribution differs from that of S99, who found $`<z>=4.13,\sigma =0.26`$. We do expect a shift of 0.2 in redshift, so we choose to bracket the possibilities by showing three possible expected redshift distributions in Figure 3. The mean of all three is $`z=3.9`$; the dashed one is a gaussian with $`\sigma =0.3`$ and is considered the most likely, the dot-dashed one is a gaussian with $`\sigma =0.2`$ and is considered the narrowest possible, and the flat dotted one is the broadest possible (a uniform distribution from $`z=3.3`$ to $`z=4.5`$). The presence of a bin in our redshift histogram that contains three LBGs is only a weak indication of autocorrelation of the LBGs, because Poisson fluctuations of any of the three expected redshift distributions generate an appearance of clustering at least this strong over 10% of the time in our Monte Carlo simulations.333Because this bin centered at $`z=3.71`$ is below the mean redshift, the result is more significant for the gaussian expected redshift distributions, but this could easily be weakened if the true mean of the expected redshift distribution is $`z=3.8`$. We will revisit this issue when the expected redshift distribution is better determined by observations in additional fields. A Kolmogorov-Smirnov test of the unbinned cumulative redshift distribution versus the three expected distributions fails to find any inconsistencies at the 95% confidence level. A similar analysis of the reported redshifts of S99 indicates that the redshift histograms of all 7 of their fields are consistent with Poisson fluctuations of their expected redshift distribution.

We are interested primarily in the clustering environment of the DLAs. This allows us to select the bins known a priori to contain a DLA and to ask if a statistically significant overdensity (or deficit) of LBGs has been found there. Finding zero LBGs in the bin containing the $`z=3.86`$ DLA should occur at least 40% of the time for any of the expected redshift distributions. Finding zero LBGs in the bins containing the $`z=4.20`$ DLA or $`z=4.37`$ quasar is at least as common. Even the apparent triple coincidence of finding no LBGs in any of those bins occurs in at least 30% of our Monte Carlo simulations, so we do not have good evidence for an anticorrelation of DLAs and LBGs. Our results provide an upper limit on the amplitude of the DLA-LBG cross-correlation function, but it is not a particularly interesting upper limit, as even the observed strong autocorrelation function of $`z=3`$ LBGs would be difficult to detect with so few objects. A vast improvement in statistics will be required to measure the cross-correlation of LBGs and DLAs.

The minimum redshift uncertainty of our LBGs is $`\mathrm{\Delta }z=0.01`$, so correlations on comoving scales of a few Mpc and smaller can only be probed via angular clustering. While 8 LBGs and 2 DLAs are insufficient to measure the angular cross-correlation precisely, we can again test whether the observed distribution is consistent with being random. The presence of 1 out of 7 LBGs from our I$`{}_{AB}{}^{}25.5`$ sample within 15′′ of the QSO line-of-sight is inconsistent with a random distribution at the 95% confidence level.444G1 was selected only because it lies within 10′′ of the quasar and was therefore excluded from this analysis. Since G2 is not particularly close to the QSO or DLAs in redshift this angular overdensity appears to be a coincidence rather than the projection of a three-dimensional structure.

## 7 Discussion

We have not found significant evidence for autocorrelation amongst the 8 LBGs at $`z>3.5`$ in our current sample. It is therefore not surprising that we find no evidence for a cross-correlation between LBGs and damped Lyman $`\alpha `$ absorbers, as the latter should be more difficult to detect if the DLAs are indeed less massive than the LBGs. Our results at $`z4`$ are comparable to the limited studies of the clustering environment of damped Lyman $`\alpha `$ systems that have been performed at $`z3`$. Steidel et al. (1996) found only one out of eleven Lyman-break galaxies in the field of Q0000-263 to be within $`\mathrm{\Delta }z=0.04`$ of the $`z=3.39`$ DLA. Ellison et al. (2000) found two out of 27 LBGS in the field containing Q0201+1120 to be within $`\mathrm{\Delta }z=0.02`$ of the $`z=3.39`$ DLA. This failure to detect clustering of LBGs with DLAs at $`z3`$ stands in contrast to the detection of strong autocorrelation of LBGs at $`z3`$ (Adelberger et al. 1998), although the latter was determined from a much larger sample of galaxies.

In order to obtain better statistics in the future, we have begun a systematic survey for Lyman-break galaxies associated with damped Lyman $`\alpha `$ absorbers at $`z3`$. The increased sky density of LBGs bright enough for spectroscopic identification at $`z3`$ and reduced sky noise near 5000 Å should allow us to obtain significantly improved statistics. The coincidence of LBG overdensity and damped Lyman $`\alpha `$ redshifts in a number of fields would argue in favor of strong biasing and hence large mass of the damped Lyman $`\alpha `$ absorbers, which is counter to the predictions of the $`\mathrm{\Lambda }`$CDM model.

We see no positive indication of clustering of LBGs with the quasar BR 0951$``$04, but this quasar is at too high a redshift for us to be sensitive to an LBG-quasar cross-correlation except in the unlikely case that our expected redshift distribution is uniform. Observing fields with a quasar at lower redshift will allow us to measure the cross-correlation of quasars and LBGs, which will test the belief that quasars are highly biased markers of protoclusters (Djorgovski 1997). With better statistics, this observational program will measure the bias of DLAs, quasars, and Lyman-break galaxies, revealing much about the typical mass and environment of these high-redshift objects.

We wish to thank Kurt Adelberger, Chuck Steidel, and Dan Stern for invaluable conversations and Jeff Newman, Andy Bunker, Max Pettini, and the referee for their comments which improved this paper. We thank the Keck Observatory staff for their patient and skillful assistance with the observations. We used the BOGUS package written by Dan Stern, Andy Bunker, and Adam Stanford and cosmic ray removal routines written by Mark Dickinson to reduce our multislit data. AMW was partially supported by NSF grant AST 0071257, and JXP acknowledges support from a Carnegie postdoctoral fellowship.

a An AB magnitude of zero corresponds to $`3.64\times 10^{23}`$ W m-2 Hz-1. AB95 magnitudes (Fukugita et al. 1996) can be converted to the Johnson-Cousins system using $`B_{JC}=B_{AB}+0.15`$, $`R_{JC}=R_{AB}0.18`$, and $`I_{JC}=I_{AB}0.43`$.

I: meets two-color criteria, I$`{}_{AB}{}^{}`$25
II: selected based on photometric redshift, I$`{}_{AB}{}^{}`$25
III: meets two-color criteria, $`25<`$I$`{}_{AB}{}^{}25.5`$
IV: selected based on photometric redshift, $`25<`$I$`{}_{AB}{}^{}25.5`$
V: within 10′′ of quasar, 25.5$`<`$I$`{}_{AB}{}^{}`$26.0

a A plus or minus sign indicates that a specific other redshift, z $`+\sigma _z`$ is also a good fit. Otherwise, the errors are approximately symmetrical and roughly correspond to 95% confidence.
b Defined as the integrated probability that the redshift is in the range $`3.5<z<4.5`$. The method corresponds to assuming a uniform prior as a function of redshift but then optimizing the likelihood at each redshift over a set of possible template spectra.
c The redshift which maximizes the photometric redshift likelihood function.
d G4 falls outside of the color selection region and was included on the basis of its photometric redshift. The very blue $`RI`$ color makes it fall directly on the evolutionary track of starburst galaxies at $`z3.6`$ which are at too low redshift to drop out of the $`B`$ filter as fully as the color criteria require.


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# Quantum enhanced positioning and clock synchronization

A wide variety of positioning and ranging procedures are based on repeatedly sending electromagnetic pulses through space and measuring their time of arrival. This paper shows that quantum entanglement and squeezing can be employed to overcome the classical power/bandwidth limits on these procedures, enhancing their accuracy. Frequency entangled pulses could be used to construct quantum positioning systems (QPS), to perform clock synchronization, or to do ranging (quantum radar): all of these techniques exhibit a similar enhancement compared with analogous protocols that use classical light. Quantum entanglement and squeezing have been exploited in the context of interferometry , frequency measurements , lithography , and algorithms . Here, the problem of positioning a party (say Alice) with respect to a fixed array of reference points will be analyzed.

Alice’s position may be obtained simply by sending pulses that originate from her position and measuring the time it takes for each pulse to reach the reference points. The time of flight, the speed of the pulses and the arrangement of the reference points determine her position. The accuracy of such a procedure depends on the number of pulses, their bandwidth and the number of photons per pulse. This paper shows that by measuring the correlations between the times of arrival of $`M`$ pulses which are frequency-entangled, one can in principle increase the accuracy of such a positioning procedure by a factor $`\sqrt{M}`$ as compared to positioning using unentangled pulses with the same bandwidth. Moreover, if number-squeezed pulses can be produced , it is possible to obtain a further increase in accuracy of $`\sqrt{N}`$ by employing squeezed pulses of $`N`$ quanta, vs. employing “classical” coherent states with $`N`$ mean number of quanta. Combining entanglement with squeezing gives an overall enhancement of $`\sqrt{MN}`$. In addition, the procedure exhibits improved security: because the timing information resides in the entanglement between pulses, it is possible to implement  quantum cryptographic schemes that do not allow an eavesdropper to obtain information on the position of Alice. The primary drawbacks of this scheme are the difficulty of creating the requisite entanglement and the sensitivity to loss. On the other hand, the frequency entanglement allows similar schemes to be highly robust against pulse broadening due to transit through dispersive media .

The clock synchronization problem can be treated using the same method. In Refs.  and  two novel techniques for clock synchronization using entangled states are presented. However, the authors of Ref.  themselves point out that the resources needed by their scheme could be used to perform conventional clock synchronization without entanglement. Similarly, all the enhancement of  arises from employing high-frequency atoms which themselves could be used for clock synchronization to the same degree of accuracy without any entanglement. In neither case do these proposals give an obvious enhancement over classical procedures that use the same resources. Here, by contrast, it is shown that quantum features such as entanglement and squeezing can in principle be used to supply a significant enhancement of the accuracy of clock synchronization as compared to classical protocols using light of the same frequency and power. In fact, the clock synchronization can be accomplished by sending pulses back and forth between the parties whose clocks are to be synchronized and measuring the times of arrival of the pulses (Einstein’s protocol). In this way synchronization may be treated on the same basis as positioning and the same accuracy enhancements may be achieved through entanglement and squeezing. In this paper only the positioning accuracy enhancement will be addressed in detail.

In order to introduce the formalism, the simple case of position measurement with classical coherent pulses is now presented. Since each dimension can be treated independently, the analysis will be limited to the one-dimensional case. For the sake of simplicity, consider the situation in which Alice wants to measure her position $`x`$ by sending a pulse to each of $`M`$ detectors placed in a known position (refer to Fig. 1). This can be easily generalized to different setups, such as the case in which the detectors are not all in the same location, the case in which only one detector is employed with $`M`$ time-separated pulses, the case in which the pulses originate from the reference points and are measured by Alice (as in GPS), etc. Alice’s estimate of her position is given by $`x=c\frac{1}{M}_{i=1}^Mt_i`$, where $`t_i`$ is the travel time of the $`i`$th pulse and $`c`$ is the light speed. The variable $`t_i`$ has an intrinsic indeterminacy dependent on the spectral characteristics and mean number of photons $`N`$ of the $`i`$-th pulse. For example, given a Gaussian pulse of frequency spread $`\mathrm{\Delta }\omega `$, according to the central limit theorem, $`t_i`$ cannot be measured with an accuracy better than $`1/(\mathrm{\Delta }\omega \sqrt{N})`$ since it is estimated at most from $`N`$ data points (i.e. the times of arrival of the single photons, each having an indeterminacy $`1/\mathrm{\Delta }\omega `$). Thus, if Alice uses $`M`$ Gaussian pulses of equal frequency spread, the accuracy in the measurement of the average time of arrival is

$$\mathrm{\Delta }t=\frac{1}{\mathrm{\Delta }\omega \sqrt{MN}}.$$
(1)
Quantum Mechanics allows us to do much better. In order to demonstrate the gain in accuracy afforded by Quantum Mechanics, it is convenient to provide first a fully quantum analysis of the problem of determining the average time of arrival of a set of $`M`$ classical pulses, each having mean number of photons $`N`$. Such a quantum treatment for a classical problem may seem like overkill, but once the quantum formalism is presented, the speed-up attainable in the fully quantum case can be derived directly. In addition, it is important to verify that no improvement over Eq. (1) is obtainable using classical pulses. The $`M`$ coherent pulses are described by a state of the radiation field of the form

$`|\mathrm{\Psi }_{cl}{\displaystyle \underset{i=1}{\overset{M}{}}}{\displaystyle \underset{\omega }{}}|\alpha (\varphi _\omega \sqrt{N})_i,`$ (2)
where $`\varphi _\omega `$ is the pulses’ spectral function, $`|\alpha (\lambda _\omega )_i`$ is a coherent state of amplitude $`\lambda _\omega `$ in the mode at frequency $`\omega `$ directed towards the $`i`$-th detector, and $`N`$ is the mean number of photons in each pulse. The pulse spectrum $`|\varphi _\omega |^2`$ has been normalized so that $`𝑑\omega |\varphi _\omega |^2=1`$. For detectors with perfect time resolution, the joint probability for the $`i`$-th detector to detect $`N_i`$ photons in the $`i`$-th pulse at times $`t_{i,k}`$ is given by

$$p(\{t_{i,k}\}):\underset{i=1}{\overset{M}{}}\underset{k=1}{\overset{N_i}{}}E_i^{()}(t_{i,k})E_i^{(+)}(t_{i,k}):,$$
(3)
where $`t_{i,k}`$ is the time of arrival of the $`k`$-th photon in the $`i`$-th pulse, shifted by the position of the detectors $`t_{i,k}t_{i,k}+x/c`$. The signal field at the position of the $`i`$-th detector at time $`t`$ is given by $`E_i^{()}(t)𝑑\omega a_i^{}(\omega )e^{i\omega t}`$ and $`E_i^{(+)}\left(E_i^{()}\right)^{}`$, where $`a_i(\omega )`$ is the field annihilator of a quantum of frequency $`\omega `$ at the $`i`$-th detector, which satisfies $`[a_i(\omega ),a_j^{}(\omega ^{})]=\delta _{ij}\delta (\omega \omega ^{})`$. The estimation of the ensemble average in Eq. (3) on the state $`|\mathrm{\Psi }_{cl}`$, using the property $`a(\omega ^{})_\omega |\alpha (\lambda _\omega )=\lambda _\omega ^{}_\omega |\alpha (\lambda _\omega )`$, gives

$`p(\{t_{i,k}\}){\displaystyle \underset{i=1}{\overset{M}{}}}{\displaystyle \underset{k=1}{\overset{N_i}{}}}|g(t_{i,k})|^2,`$ (4)
where $`g(t)`$ is the Fourier transform of the spectral function $`\varphi _\omega `$. Averaging over the times of arrival $`t_{i,k}`$ and over the number of photons $`N_i`$ detected in each pulse, one has

$`t={\displaystyle \frac{1}{M}}{\displaystyle \underset{i=1}{\overset{M}{}}}{\displaystyle \frac{1}{N_i}}{\displaystyle \underset{k=1}{\overset{N_i}{}}}t_{i,k}=\overline{\tau };\mathrm{\Delta }t{\displaystyle \frac{\mathrm{\Delta }\tau }{\sqrt{MN}}},`$ (5)
with approximate equality for $`N1`$. Here $`\overline{\tau }𝑑tt|g(t)|^2`$ and $`\mathrm{\Delta }\tau ^2𝑑tt^2|g(t)|^2\overline{\tau }^2`$ are independent of $`i`$ and $`k`$ since all the photons have the same spectrum. Eq. (5) is the generalization of (1) for non-Gaussian pulses.

Quantum light can exhibit phenomena that are not possible classically such as entanglement and squeezing, which, as will now be seen, can give significant enhancement for determining the average time of arrival. First consider entanglement. The framework just established allows the direct comparison between frequency entangled pulses and unentangled ones. For the sake of clarity, consider initially single photon entangled pulses.

Define the “frequency state” $`|\omega `$ for the electromagnetic field the state in which all modes are in the vacuum state, except for the mode at frequency $`\omega `$ which is populated by one photon. Thus the state $`𝑑\omega \varphi _\omega |\omega `$ represents a single photon wave packet with spectrum $`|\varphi _\omega |^2`$. Consider the $`M`$-photon frequency entangled state given by

$`|\mathrm{\Psi }_{en}{\displaystyle 𝑑\omega \varphi _\omega |\omega _1|\omega _2\mathrm{}|\omega _M},`$ (6)
where the ket subscripts indicate the detector each photon is traveling to. Inserting $`|\mathrm{\Psi }_{en}`$ in Eq. (3), and specializing to the case $`N_i=1`$, it follows that

$`p(t_1,\mathrm{},t_M)|g({\displaystyle \underset{i=1}{\overset{M}{}}}t_i)|^2.`$ (7)
That is, the entanglement in frequency translates into the bunching of the times of arrival of the photons of different pulses: although their individual times of arrival are random, the average $`t\frac{1}{M}_{i=1}^Mt_i`$ of these times is highly peaked. (The measurement of $`t`$ follows from the correlations in the times of arrival at the different detectors). Indeed, from Eq. (7) it results that the probability distribution of $`t`$ is $`|g\left(Mt\right)|^2`$. This immediately implies that the average time of arrival is determined to an accuracy

$`\mathrm{\Delta }t={\displaystyle \frac{\mathrm{\Delta }\tau }{M}},`$ (8)
where $`\mathrm{\Delta }\tau `$ is the same of Eq. (5). This result shows a $`\sqrt{M}`$ improvement over the classical case (5).

To emphasize the importance of entanglement, Eq. (8) should be compared to the result one would obtain from an unentangled state analogous to $`|\mathrm{\Psi }_{en}`$. To this end, consider the state defined as

$`|\mathrm{\Psi }_{un}{\displaystyle \underset{i=1}{\overset{M}{}}}{\displaystyle 𝑑\omega _i\varphi _{\omega _i}|\omega _i_i},`$ (9)
which describes $`M`$ uncorrelated single photon pulses each with spectral function $`\varphi _\omega `$. By looking at the spectrum of the state obtained by tracing away all but one of the modes in (6), each of the photons in (9) can be shown to have the same spectral characteristics as the photons in the entangled state $`|\mathrm{\Psi }_{en}`$. Now, using Eq. (3) for the uncorrelated $`M`$ photon pulses $`|\mathrm{\Psi }_{un}`$, it follows that

$`p(t_1,\mathrm{},t_M){\displaystyle \underset{i=1}{\overset{M}{}}}|g(t_i)|^2,`$ (10)
which is the same result that was obtained for the classical state (2). Thus Eq. (5) holds, with $`N=1`$, also for $`|\mathrm{\Psi }_{un}`$. From the comparison of Eqs. (5) and (8), one sees that, employing frequency-entangled pulses, an accuracy increase by a factor $`\sqrt{M}`$ is obtained in the measurement of $`t`$ with respect to the case of unentangled photons.

Since $`|\mathrm{\Psi }_{en}`$ is tailored as to give the least indetermination in the quantity $`t`$, it is appropriate for the geometry of the case given in Fig. 1, where the sum of the time of arrival is needed. Other entangled states can be tailored for different geometric dispositions of the detectors, as will be shown through some examples.

How is it possible to create the needed entangled states? In the case $`M=2`$, the twin beam state at the output of a cw pumped parametric downconverter will be shown to be fit. It is a 2 photon frequency entangled state of the form $`𝑑\omega \varphi _\omega |\omega _s|\omega _0\omega _i`$, where $`\omega _0`$ is the pump frequency and $`s`$ and $`i`$ refer to the signal and idler modes respectively. This state is similar to (6) and it can be employed for position measurements when the two reference points are in opposite directions, e.g. one to the left and one to the right of Alice. In fact, it can be seen that $`p(t_1,t_2)|g(t_1t_2)|^2`$ and hence such a state is optimized for time of arrival difference measurements, as experimentally reported in . In the case of $`M=3`$, a suitable state can be obtained starting from a $`3`$-photon generation process that creates a state of the form $`𝑑\omega 𝑑\omega ^{}f(\omega ,\omega ^{})|\omega |\omega ^{}|\omega _0\omega \omega ^{}`$, and then performing a non-demolition (or a post-selection) measurement of the frequency difference of two of the photons. This would create a maximally entangled $`3`$-photon state, tailored for the case in which Alice has one detector on one side and two detectors on the other side. However, for $`M>2`$, the creation of such frequency-entangled states represents a continuous variable generalization of the GHZ state, and, as such, is quite an experimental challenge.

Now turn to the use of number-squeezed states to enhance positioning. The $`N`$-th excitation of a quantum system (i.e. the state $`|N`$ of exactly $`N`$ quanta) has a de Broglie frequency $`N`$ times the fundamental frequency of the state. Its shorter wavelength makes such a state appealing for positioning protocols. In this case, the needed “frequency state” is given by $`|N_\omega `$, defined as the state where all modes are in the vacuum except for the mode at frequency $`\omega `$, which is in the Fock state $`|N`$. The probability of measurement of $`N`$ quanta in a single pulse at times $`t_1,\mathrm{},t_N`$ is given by Eq. (3) with $`M=1`$ detectors. It is straightforward to see that, for a state of the form $`𝑑\omega \varphi _\omega |N_\omega `$, the time of arrival probability is given by

$`p(t_1,\mathrm{},t_N)|g({\displaystyle \underset{k=1}{\overset{N}{}}}t_k)|^2.`$ (11)
Such a result must be compared to what one would obtain employing a classical pulse $`|\mathrm{\Psi }_{cl}`$ of $`N`$ mean number of photons, i.e. the state (2) with $`M=1`$. Its probability (4) shows that employing the $`N`$-photon Fock state gives an accuracy increase of $`\sqrt{N}`$ vs. the coherent state with $`N`$ mean number of photons. The similarity of this result (11) with the one obtained in Eq. (7) stems from the fact that the Fock state $`|N_\omega `$ can be interpreted as composed by $`N`$ one-photon pulses of identical frequency. Hence, all the results and considerations obtained previously apply here. An experiment which involves such a state for $`N=2`$ is reported in .

Entangled pulses of number-squeezed states combine both these enhancements. By replacing $`|\omega `$ with the number-squeezed states $`|N_\omega `$ in the $`M`$-fold entangled state (6), one immediately obtains an improvement of $`\sqrt{MN}`$ over the accuracy obtainable by using $`M`$ classical pulses of $`N`$ photons each.

The enhanced accuracy achieved comes at the cost of an enhanced sensitivity to loss. If one or more of the photons fails to arrive, the time of arrival of the remaining photons do not convey any timing information. The simplest way to solve this problem is to ignore all trials where one or more photons is lost. A more sophisticated method is to use partially entangled states: these states provide a lower level of accuracy than fully entangled states, but are more tolerant to loss. As shown in figure 2, even the simple protocol of ignoring trials with loss still surpasses the unentangled state accuracy limit even for significant loss levels. The use of intrinsically loss-tolerant, partially entangled states does even better .

Before closing, it is useful to consider the following intuitive picture of quantum measurements of timing. A quantum system such as a pulse of photons or a measuring apparatus with spread in energy $`\mathrm{\Delta }E`$ can evolve from one state to an orthogonal state in time $`\mathrm{\Delta }t`$ no less than $`\pi \mathrm{}/(2\mathrm{\Delta }E)`$ . Accordingly, to make more accurate timing measurements, one requires states with sharp time dependence, and hence high spreads in energy. Classically, combining $`M`$ systems each with spread in energy $`\mathrm{\Delta }E`$ results in a joint system with spread in energy $`\sqrt{M}\mathrm{\Delta }E`$. Quantum-mechanically, however, $`M`$ systems can be put in entangled states in which the spread in energy is proportional to $`M\mathrm{\Delta }E`$. Similarly, $`N`$ photons can be joined in a squeezed state with spread in energy $`N\mathrm{\Delta }E`$. The Margolus-Levitin theorem  limits the time $`\mathrm{\Delta }t`$ it takes for a quantum system to evolve from one state to an orthogonal one by $`\mathrm{\Delta }t2\mathrm{}/\pi E`$, where $`E`$ is the average energy of a system (taking the ground state energy to be 0). This result implies that the $`\sqrt{MN}`$ enhancement presented here is the best one can do.

In conclusion, quantum entanglement and squeezing have been shown to increase the accuracy of position measurements, and, as a consequence, they can also be employed to improve the accuracy in distant clock synchronization. For maximally entangled $`M`$-particle states we have shown an accuracy increase $`\sqrt{M}`$ vs. unentangled states with identical spectral characteristics. A further increase $`\sqrt{N}`$ in accuracy in comparison with classical pulses was also shown for the measurement of $`N`$ quanta states. At least for the simple cases of $`M=2`$ or $`N=2`$, the described protocols are realizable in practice.

This work was funded by the ARDA, NRO, and by ARO under a MURI program.


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# First order transition from antiferromagnetism to ferromagnetism in Ce(Fe0.96Al0.04)2

## Abstract

Taking the pseudobinary C15 Laves phase compound Ce(Fe0.96Al0.04)2 as a paradigm for studying a ferromagnetic to antiferromagnetic phase transition, we present interesting thermomagnetic history effects in magnetotransport as well as magnetisation measurements across this phase transition. A comparison is made with history effects observed across the ferromagnetic to antiferromagnetic transition in R0.5Sr0.5MnO3 crystals.

The C15 Laves phase compound CeFe2, with its relatively low Curie temperature (TC $``$ 230K) and reduced magnetic moment ($`2.3\mu _B/`$f.u.)  is on the verge of a magnetic instability . Neutron measurements have shown the presence of antiferromagnetic (AFM) fluctuations in the ferromagnetic (FM) state of CeFe2 below 100K . With small but suitable change in electronic structure caused by doping with certain elements like Co, Al, Ru, Ir, Os, and Re at the Fe site , these AFM fluctuations get stabilized into a low temperature AFM state .

While most recent experimental efforts are focussed on understanding the cause of this magnetic instability in CeFe2 , we have recently addressed the question of the exact nature of this FM-AFM transition in Ru and Ir-doped CeFe2 alloys . Our results show that this is a first order transition. The nature of the FM to AFM transition in the perovskite-type manganese oxide compounds R0.5Sr0.5MnO3 (R=Nd, Pr, Nd0.25Sm0.75) has also been the subject of close scrutiny in recent years , and has also been shown to be a first order transition. The existence of metastable states, which are thought to be generic to a first order phase transition, has been highlighted.

In this paper we report interesting thermomagnetic history dependence in the magnetisation and magnetoresistance in a Ce(Fe0.96Al0.04)2 alloy, and argue that these are broader manifestations of the behaviour reported earlier in the perovskite-type manganese compounds . While the metastabilities can be partly explained by the phenomena of supercooling and superheating, we present clear signatures that the kinetics of this magnetic phase transition is hindered at low temperatures.

The details of the preparation and characterization of the sample can be found in Ref.6. The samples from the same batch have been used earlier in bulk magnetic, transport (Ref.6), and neutron (Ref.8) measurements. We have used a SQUID-magnetometer (Quantum Design MPMS5) for measuring magnetisation (M) as a function of temperature (T) and magnetic field (H).We have checked our results using scan length varying from 2 to 4 cm and no qualitative difference was found. We have used a commercial superconducting magnet and cryostat system (Oxford Instruments, UK) for magnetotransport measurements as a function of T and H. The resistivity was measured using standard dc four-probe technique.

The present Ce(Fe0.96Al0.04)2 sample undergoes a paramagnetic (PM) to FM transition at around 200K, followed by a FM to AFM transition at around 95K (Ref.6). We first plot in fig. 1 M-H data at some representative T. The behaviour of M at T=100K is consistent with that of a soft (coercive field $``$100 Oe) FM, reaching technical saturation by H$``$3kOe. With lowering of T the nature of the M-H curve changes drastically with the appearance of a hysteresis bubble. Such hysteresis, along with the observed cubic to rhombohedral transition (Ref.8), have been considered earlier as possible signatures of a field-induced first-order metamagnetic transition from AFM to FM in Co-doped CeFe2 (Ref.15). At T=5K, we find that if the maximum field excursion is less than $`|30|`$ kOe, the M-H curve remains reversible in the high field regime. In this field regime the sample remains in the AFM state.(The observed nonlinearity in $`\pm `$5 kOe regime is due to parasitic weak ferromagnetism  leading to a canted spin state ) When the applied H is increased beyond H$`{}_{M}{}^{}`$30 kOe, M rises rapidly and upon lowering H a hysteresis is observed. The hysteresis loop, however, collapses before H is reduced to zero (coercive field $``$ 300 Oe), and reappears again in the third quadrant, giving rise to a butterfly-like hysteresis loop. In fig. 2 we present resistivity ($`\rho `$) as a function of H, at the representative temperatures T= 3K, 5K, and 20K. The sample is initially cooled to each temperature in zero field. We see the clear signature of a field induced AFM-FM transition at a field HM(T), where the resistivity decreases sharply with increasing H. It is to be noted that in the present case of Ce(Fe0.96Al0.04)2 both FM and AFM phases are metallic, and the change in resistivity observed is not as drastic as in R0.5Sr0.5MnO3 with R=Nd . On reducing the field from well above HM, a clear hysteresis is seen in the $`\rho `$ vs H plot (see figures 2a to 2c). This hysteresis is due to metastable states expected across a first order transition where the inequality between the free energies of the two phases changes sign on a (H$`{}_{M}{}^{},T_N`$) line, but the transition to the higher entropy phase actually occurs on a (H$`{}_{}{}^{},T^{}`$) line because of superheating, and the transition to the lower entropy phase actually occurs on a (H$`{}_{}{}^{},T^{}`$) line because of supercooling. We accordingly attribute this hysteresis in M vs H and in $`\rho `$ vs H to the first order nature of the field induced FM-AFM transition. Similar hysteresis observed in the $`\rho `$-H plots of R0.5Sr0.5MnO3 has also been attributed to the first order nature of the phase transition .

In this picture, the FM state continues to exist as a supercooled metastable state when H is lowered isothermally below HM, upto the limit H. Between HM and H fluctuations can help in nucleating droplets of the AFM state, and at H an infinitesimal fluctuation will drive the whole system to the stable AFM phase. Heterogeneous nucleation can thus cause a spatial distribution of the field till which supercooling is actually observed at T, resulting in the (H$`{}_{}{}^{},T^{}`$) line getting broadened into a band. Early theoretical arguments and recent measurements also showed that a sample with disorder can have a spatial distribution of the phase transition field HM in a general first order transition, hence broadening the (HM,TN) line into a band. This disorder would also cause the (H$`{}_{}{}^{},T^{}`$) and (H$`{}_{}{}^{},T^{}`$) lines to be broadened into bands. This is depicted schematically in fig. 3a, and is consistent with earlier neutron scattering observation in Al-doped CeFe2 of coexisting FM and AFM phases over a finite temperature regime  .

We now come to some interesting features seen at very low temperatures, where the effect of thermal fluctuations is reduced. As seen in figs. 2b and 2c, when the applied field is reduced to zero from Hmax well above HM at T=3 and 5K, the $`\rho `$(H=0) lies distinctly below the initial ZFC $`\rho `$(H=0), thus giving rise to an open hysteresis loop. This kind of open hysteresis loop has been reported earlier for single crystal Nd0.5Sr0.5MnO3 samples at low temperature . We attribute this lower resistance to the existence of a residual metastable FM phase even at H=0. Is (H=0,T=3K) within the (H,T) band, or can such a residual FM phase persist below the (H,T) band? We shall return to this question.

The envelope $`\rho `$-H hysteresis curves shown in fig. 2 are obtained by reducing the field from Hmax to zero to -Hmax, and raising it back to Hmax. We see in fig 2 that the virgin $`\rho `$-H curve lies outside the envelope hysteresis curve. As seen in fig 1, the virgin M-H curve at 5K also lies clearly outside the envelope hysteresis curve. We argue from existing data that this anomalous feature would also be seen in Nd0.5Sr0.5MnO3 at T$`<`$20K. The reported $`\rho `$-H curve (see fig.2B to 2D of Ref. 12) exhibits an open hysteresis loop. It appears obvious that if H were again increased fron zero to 120 kOe, the forward leg of this envelope curve would merge with the virgin $`\rho `$-H curve only at some finite (and large) field. We consider this anomalous relation between virgin and envelope hysteresis curves at low temperatures, seen in both magnetotransport and magnetisation measurements, as significant.

We now present in fig.4, $`\rho `$ vs T plots in fields of H=0, 5, 20, and 30 kOe. In each case we have cooled the sample to 5K in zero field and then applied H at this temperature. Resistivity is then measured as the sample is warmed well into the FM state. The sample is then cooled back to 5K in the field H, allowing a measurement of thermal hysteresis. The appearance of magnetic superzones at the AFM-FM transition gives rise to the distinct structure observed in $`\rho `$-T. There is a marked hysteresis between the warming and cooling cycles, because the FM (or AFM) phase can be supercooled (or superheated) and exists as a metastable phase between the (HM,TN) line and the (H$`{}_{}{}^{},T^{}`$) line (or the (H$`{}_{}{}^{},T^{}`$) line). For H=0 and 5 kOe, the FM to AFM transition is completed during cooldown at T$``$20K; this indicates that (H=0,T=5K) and (H=5kOe, T=5K) points lie below the (H,T) band and no supercooled FM phase is expected to be metastable at H=0 at T=3K or 5K. This is in striking contrast with the data in fig 2 which shows that the resistance of the AFM state is not restored when H is reduced to zero isothermally.(The $`\rho `$ vs T data in R0.5Sr0.5MnO3 shows the same contrast with the $`\rho `$-H data ) The data in fig. 4 also shows that for H=20 kOe and H=30 kOe the resistivity does not rise to its full AF state value on the cooling curve down to 5K, even though the FM to AFM transformation appears to have been arrested at around 15K. (This is again similar to the observations in Ref. 14 on the single crystal manganite samples.)

We now summarize the unusual findings of the present study.

1. The envelope $`\rho `$-H curve at 5K and 3K (fig.2) does not return at H=0 to the virgin curve value of $`\rho `$(H=0), while the FM to AFM transition is complete when the sample is cooled to these temperatures in low field. A similar behaviour is seen from the single crystal studies on R0.5Sr0.5MnO3 in another first order FM to AFM transition.
2. The butterfly $`\rho `$-H and M-H hysteresis loops have an anomalous virgin curve at low temperatures, in that the virgin curve lies outside the envelope hysteresis curve in both measurements.
3. In the field-cooled measurement of $`\rho `$ vs T at H=20 kOe, and 30 kOe, the FM to AFM transition appears to be arrested at about 15K even while the transformation is incomplete, and remains incomplete down to 5K. These results are supported by the study of T dependence of M in both the zero-field-cooled and field-cooled mode . Similar behaviour in the the resistivity studies are seen in the single crystal studies of R0.5Sr0.5MnO3 .

As a possible explanation we introduce the idea that the kinetics of the FM to AFM transition gets hindered at low T and in high H. We concentrate on the (H,T) band in fig. 3b, and recognize that for (H,T) values below this band the free energy barrier separating the FM from the AFM phase has dropped to zero throughout the sample . An infinitesimal fluctuation should drive any FM region to the AFM phase. But all our observations indicate that at very low T the unstable FM regions remain in the AFM phase. It is well known that at sufficiently low T the characteristic time for structural relaxation becomes larger than experimental time-scales . We postulate that at sufficiently low T the displacive motion of atoms involved in the structural distortion that is associated with the FM-AFM transition in Ce(Fe0.96Al0.04)2 (Ref. 8), becomes negligible on experimental time scales. The high temperature-high field FM phase is then frozen-in. We accordingly postulate that below a certain temperature TK(H) the kinetics of the FM-AFM transformation is hindered and arrested just like in a quenched metglass. (This is similar to observations at high pressures where the high density phase cannot transform to the low density phase below a certain TK, with TK rising as the pressure rises.) We would depict this as a (HK,TK) line in the two-control-variable (H,T) space, which we broaden into a band with the same argument used to replace the other thermodynamic transition lines by a band. At temperatures below the band the freezing-in occurs throughout the sample; within the band it occurs in some regions of the sample. With this conjecture we now explain the three unusual findings enumerated above. We use the schematic in fig 3b, where paths labeled by 1 and 2 indicate cooling in constant field and lowering H at constant T, respectively. We assume that we start always with a sample that is prepared to be completely in the FM phase by warming (or increasing field) to a point well above the (H$`{}_{}{}^{},T^{}`$) band.

Let us cool sequentially to points A, B, F, and G along path 1. At point A we observe FM and AFM coexistence (with FM being metastable) while at point B the entire sample is in the AFM phase. The (HK,TK) band has no observable effect as we cool to points F or G. This corresponds to our $`\rho `$-T data at H=0 or 5 kOe. Following path 1 again, we cool in higher fields to reach, sequentially, points C, D, E, and L. At C we have two phase coexistence with FM transforming to AFM as temperature is lowered. This transformation is arrested at D, and the FM fraction is frozen-in at E and L, even though it would have kept reducing in an ergodic system. Thus we have a frozen-in FM phase at L even though it is unstable. This explains the field-cooled $`\rho `$ vs T and M vs T (Ref.22) data at fields of 20 and 30 kOe. We now follow path 2 and lower the field sequentially to points C and B. At point C we see two-phase coexistence and at point B the sample is fully AFM. This explains our M-H data and our $`\rho `$-H data at higher T. We now follow path 2 and lower the field to points E and F. At point E the FM phase is frozen-in throughout, while at F some regions of the sample are no longer kinetically arrested and transform to the AFM phase. This corresponds to our $`\rho `$-H data at 3K and 5K, with only part recovery of the AFM phase even though path 1 gives a full recovery of the AFM phase. And in the ZFC state at H=0 we reached point F by path 1. This also explains the anomalous virgin curves because the virgin curve starts at F after path 1, then goes above the (H∗∗,T∗∗) band and returns to point F by path 2 thereby retaining a fraction of FM phase. The forward hysteresis curve now starts with coexisting FM-AFM phases unlike the virgin curve which had only AFM phase. Because of the larger M and lower $`\rho `$ of the FM phase, the forward hysteresis envelope thus lies above (or below) the virgin curve in isothermal M-H (or $`\rho `$-H) measurements. Finally, if we follow path 2 and reduce the field isothermally to reach point G, then the FM phase is frozen-in completely, and no AFM phase is recovered. This explains the $`\rho `$-H data at 10K reported (Ref.14) in the R0.5Sr0.5MnO3 single crystal with R=Nd0.25Sm0.75.

To conclude, we have observed unusual history effects in magnetization and magnetotransport measurements across the FM-AFM transition in Ce(Fe0.96Al0.04)2, and have discussed similarities with earlier single crystal data on R0.5Sr0.5MnO3 across another first order FM-AFM transition. We have argued that the kinetics of this FM-AFM transition is hindered at low T. This observation may be of relevance to other first order transitions where it is more difficult to vary two control variables; one example is the high density amorphous water (HDAW) to low density amorphous water (LDAW) transition which is observed with reducing pressure at 130K, but whose kinetics appears to be arrested at 77K . These FM-AFM transitions can be used as paradigms to study various interesting aspects of a first order transition like nucleation and growth, supercooling and superheating, hindered kinetics, etc in a relatively easy and reproducible manner.

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