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# Spin-phonon interaction in doped high-TC superconductors from density functional calculations.

Effects of coupling between phonon distortions and stripe-like spin waves in the CuO plane of HgBa2CuO4 are studied by band calculations. Local exchange enhancements depend sensitively on the local structure around Cu sites. Interactions where spin waves have twice as long wave length as phonon waves can lead to a ’dip’ in the density of states (DOS) below the Fermi energy, $`E_F`$. This type of interaction is compatible with several seemingly contradictory observations among high-$`T_C`$ cuprates, like the isotope effect, anti-ferromagnetic fluctuations, stripes and pseudogaps. It can also account for a large $`T_C`$.

Numerous studies of high-TC superconductors have revealed unusual properties in the normal and superconducting states. A common feature of the different Hg-, Bi-, Y- or La-based high-TC copper oxides is the almost planar CuO sheets, which generates a cylindrical Fermi-surface (FS) in density functional (DF) band calculations. However, real undoped materials become anti-ferromagnetic (AF) insulators and it is only within a rather narrow range of (usually hole-) doping that high-TC superconductivity can be observed. This delicate balance of the normal state property from being metallic or AF insulating leads naturally to the AF pairing interactions  as an alternative to the conventional electron-phonon coupling as a possible mechanism for high-TC superconductivity. Complex isotope effects, d-wave gap symmetry, magnetic excitations, stripes and pseudo gaps all contribute to the ”unconventional” properties of these materials . The concept of stripes has been developed from models of strong correlation , where Hubbard model calculations produce gaps in the spectral functions . From DF calculations it has been shown that ”stripe-like” AF modulations (AFM) of spin-waves or phonons in the CuO-plane lead to gaps in the one-particle DOS . Such modulations decrease the total energy if the gap opens at $`E_F`$, which leads to a connection between wave length and doping. Taken separately, both waves (spin or phonon) give large coupling parameters (spin fluctuation or electron-phonon). This motivates a closer look at the possible interaction of such modes. We show that structural distortions modify local Stoner enhancement and hence the calculations confirm that spin-phonon coupling is large. Secondly, it is shown that a double gap structure in the DOS occurs when the wave lengths of the spin wave is twice that of the phonon mode.

Interactions between AFM fluctuations and phonon modes are modeled for one of the structurally simplest high-TC materials, HgBa2CuO4 (HBCO), where electronic structure calculations are done for ”frozen” phonon and spin waves. The DF-calculations use the LMTO method based on the local spin density approximation  (LDSA) for supercells of HBCO, including staggered magnetic fields to generate spin-waves (”stripes”) or atomic displacements to model phonons. The calculations for the two types of modes are similar, but atomic displacements generate multipolar changes of the potential and calculations of changes of total energies require full potential methods. Long wave length spin modulations are simpler since the change in potential is spherical within each atom. The calculations are still lengthy because of the very large supercells. Therefore, in this work we refrain from calculating total energies, but we focus on the exchange enhancements and double gap structures in the DOS. The details of the methods can be found in refs. .

A forced AF (on Cu) configuration in undoped HBCO, modeled by LSDA calculations, requires applied field amplitudes of about 23 mRy to open a gap, cf. Table 1. If the Ba atoms are moved 0.1 a.u. closer to the CuO plane, the critical field is reduced to about 16, while the opposite movement requires about 30 mRy. Other distortions have similar effects, the Ba mode is one example. When the atomic distortions are modulated along the cell (but with no modulation of the applied AF field) one can notice that the local AF Cu-moments are largest in a region where the Ba are closest to the CuO-planes. Another example is the ”half-breathing” mode , where two planar oxygens are moved closer or further away from the Cu, so that Cu-sites along  alternatively have two O-neighbours at +x and -x closer than normal (”compressed” Cu), or more distant than normal (”dilated ” Cu). The calculated exchange enhancement is roughly 50 % larger on the dilated than on the compressed Cu. The spin induced gap is situated at the stoichiometric band filling, 63 valence electrons per HBCO cell or at 1008 electrons for a 16 formula unit (f.u.) supercell, when the AF configuration has no modulation. But as was shown in ref. , if there is a modulation (AFM or phonon) then the gap is always found at a band filling corresponding to 2 electrons below the position of the gap in the unmodulated case. That is, at 1006 electrons for the 16 f.u. cell, at 502 instead of at 504 electrons for the half as long cell, etc.. The gain in kinetic energy is largest if the AFM wave has the largest moments coinciding with the optimal local distortions around Cu (Ba close to the CuO plane, dilated Cu, etc.). The nodes of the AFM wave, where the moments are zero, coincide with the parts of the phonon which are most unfavorable to magnetism. Furthermore, this implies that the AFM spin wave is twice as long as the wave of the phonon modulation.

As an example we consider a long supercell containing 16 f.u., oriented along , cf. fig 1. According to the rules for gap positions one expects a gap near 1006 electrons, caused by one complete spin modulation along this cell. We call this gap a ’spin gap’. Simultaneously, there are two wave lengths of a phonon modulation within the cell, which gives a gap (called ’phonon gap’) at a band filling of 1004 electrons. Such features are seen in the DOS from the band calculations. The gaps are complete with zero DOS in a narrow energy interval, if the amplitudes of the atomic distortions or the magnetic fields are large. If the amplitudes are moderate, the gaps are partial ’pseudo gaps’, where the DOS is reduced to make ’dips’ at the corresponding band fillings. Unpolarized band calculations for different phonon modulations (Ba, apical-O, ”breathing-O”) show the expected pseudo gaps. When the cell contains both the double phonon wave and the AFM wave, one should expect two gaps. The DOS shown in fig. 2, is calculated for a spin wave distribution along the cell which generates a charge modulation of two wave lengths along the cell. The strongest gap is at $`E_F`$ (1006 electrons) and it is caused by the spin wave. A second smaller ’dip’ approximately 2 electrons below $`E_F`$ is caused by a component $`V_q`$ from the charge distribution. Note that no phonon distortion is needed to see the charge gap in this case, but for a paramagnetic calculation with two wave lengths of a phonon, one can see a tendency for a gap near 1004 electrons, see fig. 2. A similar charge redistribution appears in this separate paramagnetic calculation as in the spin polarized case with only the AFM wave. There seems to be a mutual enforcement of spin and charge gap, as well as increased amplitude of the charge transfers in calculations containing both the phonon and the AFM wave.

Another example of this is the half-breathing modes within a 8 f.u. cell along . Two half-breathing modes, which are the shortest possible double phonon mode that can fit into this cell, induce similar charge transfers as the spin wave, as seen in Table 2. The combination of an unmodulated (AF) spin configuration and the phonon wave gives moments that are about 60 percent larger on the ”dilated” than on the ”compressed” Cu, for the same applied field amplitudes on both types. The ”compressed” Cu atoms gain charge in the paramagnetic calculations, just as the Cu at nonmagnetic node positions of a spin wave do. Both the phonon and the spin wave enforce the $`V_q`$ coefficient for a (charge) gap (at 500 electrons for the 8 f.u. cell). This can interpreted as a type of valence fluctuation. These have been suggested for a mechanism for exotic pairing and superconductivity . The results from the 8 f.u. cell show that they are coupled to the spin-phonon modes.

A few combinations of phonon and spin modulations along  show partly similar trends. There are 2 electrons per supercell separating the gaps induced by the spin- and phonon waves. For long wave lengths (long supercells), i.e. for underdoped cases, this means that the two gaps should appear relatively close to each other. The energy difference between gaps $`\mathrm{\Delta }En/N`$, where $`n`$ and $`N`$ are the number of states and the DOS per f.u., respectively. For instance, for the 16 f.u. cell here, where n is 2/16 per f.u. and N is about 11 states/Ry per f.u. , the energy difference would be about 140 meV. For overdoped cases, when the wave length is short, the two gaps should be more separated, although there is some compensation from the increased DOS as $`E_F`$ approaches a van-Hove singularity at increased doping.

Photoemission  and tunneling  measurements in the Bi-based material reveal a dip at about 80 meV below $`E_F`$ even above $`T_C`$. We suggest that this dip corresponds to the phonon gap of the DOS, as discussed above. The DOS at $`E_F`$ per CuO plane in the Bi-compound is larger than in HBCO, and increasing further with doping . The position of the dip is of the correct order to correspond to the phonon dip. The origin of this dip was much discussed a few years ago, because from tunneling it was shown to be pronounced only in the occupied part. This is in qualitative agreement with the spin-phonon model.

Not all phonon displacements produce double gaps. A mode with Cu displaced along $`z`$ makes a relatively small difference between the moments on displaced and undistorted atoms. This distortion is symmetric with respect to the CuO plane, and the wave length of an AFM modulation can be equal to the wave length of the phonon. Spin and phonon gaps are weak and appear at the same energy.

As was mentioned above, precise total energies are not calculated. However, we can make a number of qualitative observations of how a strong AF exchange enhancement and a pseudo gap will change the total energy. The spin gap is strongest if a system is close to an AFM transition when there is almost no limit for the exchange enhancement. Vibrational amplitudes are of the order 0.1 a.u. at low T . Normal harmonic vibrations follow a parabolic potential, where the potential energy $`U`$ is a quadratic function of the displacement $`x`$, $`U=\frac{1}{2}Kx^2`$. $`K`$ is a force constant $`d^2U/dx^2`$. If, at low T and large $`x`$, it is possible to gain energy because of a spin wave, it will also soften the phonon. The quadratic behavior of $`U`$ will be flattened out ($`K`$ diminishes with $`x`$) which allows a further increase of $`x`$. Mutual enhancements of distortion and moment will enforce both gap structures. Several coupled spin-phonon modes may compete at large T, when the free energy gain from a gap formation is less efficient because of the Fermi-Dirac smearing and thermal disorder. A selection at lower T may leave one mode with the largest gain in energy to be dominant with a more coherent effect on the DOS.

The Stoner enhancement $`S`$ is useful for a discussion of ferro magnetism. An extension for AF can be done via generalized spin susceptibility $`\chi _q`$. An approximate approach can be based on local $`S`$-factors (defined within each site) calculated for AFM waves. Here they are defined as the exchange splitting of the logarithmic derivative of the Cu-d band divided with the applied field ($`ϵ`$) at the same site. The local Stoner factor $`\overline{S}`$ defines the local exchange integral $`I`$, $`\overline{S}=NI=11/S`$. An important decrease of the total energy is coming from the opening of a gap via the potential component $`V_q`$, which in the idealized case is close to $`\frac{1}{2}N_qV_q^2`$, where $`V_q`$ is the band shift at $`q`$ and $`N_q`$ is a fraction of the total DOS that is affected by the splitting. The total energy has also kinetic and exchange contributions from each site, which can be summed up, if each site is independent of its neighbors.

$$E=(N_iϵ^2N_i^2I_iϵ^2)=1/NSm_i^2$$
(1)
where $`m=Nϵ`$ is the magnetic moment, and it is assumed that $`N`$ and $`S`$ are not much varying from site to site. The additional hybridization energy due to nonequivalent neighboring atoms in the AF case is accounted for in local $`S`$-values, defined from spin-polarized results for the real spin-wave configuration. All these contributions make $`S`$ to vary non-linearly with the field, as can be seen in Table 1 for the simple AF configuration of the undoped 2 f.u. cell. It is noted that the LSDA potential is too weak to explain a spontaneous AF order and a full gap. The local $`I`$ (or $`N`$) needs to be almost twice as large to get a gap. A similar reasoning can be made for the doped cases, with modulations of AFM waves.

Bardeen-Cooper-Schrieffer (BCS) theory without strong coupling effects is often sufficient to understand the mechanism for superconductivity based on electron-phonon or paramagnon coupling . A potential perturbation, as from a phonon, with Fourier component $`V_q`$ leads to a ”Cooper” pairing of electrons of opposite momentum $`\pm q`$. The BCS relation for $`T_C`$ contains the electron-phonon coupling $`\lambda _{\mathrm{ph}}`$;

$$k_BT_C=1.13\mathrm{}\mathrm{\Omega }_Dexp(1/\lambda _{\mathrm{ph}})$$
(2)
where $`\mathrm{\Omega }_D`$ is a characteristic phonon frequency. Here the coupling is for electronic states of opposite spin. Since $`\lambda _{ph}NV^2/K=NV^2/M\mathrm{\Omega }_D^2`$, where $`V`$ is matrix element of the perturbation potential due to a displacement, there is normally low coupling for stiff phonons. High phonon energies in combination with fairly large $`\lambda _{\mathrm{ph}}`$, estimated from band theory, can hardly explain the very large observed $`T_C`$’s in the copper oxides , although the role of phonons on superconductivity cannot be ignored . An analogous formulation for equal spin pairing  is;

$$k_BT_C=1.13\mathrm{}\omega _{sf}exp(1/\lambda _{\mathrm{sf}})$$
(3)
The prefactor $`\omega _{sf}`$ is the frequency of the spin fluctuation and $`\lambda _{\mathrm{sf}}`$ is the coupling strength. These properties are in the ferro magnetic case related as :

$$\mathrm{}\omega _{sf}=2/NS;\lambda _{\mathrm{sf}}=\frac{1}{2}S\overline{S}^2$$
(4)
As for phonons there is an antagonistic dependence of $`T_C`$ on frequency and coupling strength. For instance, if the spin coupling is large via a large $`S`$-factor there is a softening, so that $`\omega _{sf}`$ and $`T_c`$ goes down. The equal spin pairing has been suggested to give small $`T_C`$’s near the FM transition in C15 compounds . Extreme softening leads to static spin for magnetic coupling or to a structural transformation for phonon coupling. The major contribution to the matrix element $`V`$ for an AFM perturbation comes from the opening of a gap. An approximate value can be obtained from the gap model, where the gap is equal to the maximum value of the exchange enhanced field. The model permits for an evaluation of the matrix element $`V1`$, which with the denominator $`K=d^2E/dϵ^2=2N/S`$ makes $`\lambda _{\mathrm{sf}}\frac{1}{2}S`$. Eq. 1 is formally as for ferro magnetic cases, whereby one can use $`\mathrm{}\omega _{sf}2/NS`$. Near the region for AF fluctuations, one can expect very large $`\lambda _{\mathrm{sf}}`$, but unless a there is a mechanism for a large $`\omega _{sf}`$, it will not produce a large $`T_C`$.

As was discussed above, Cu-moments can vary 50 percent or more along a phonon with realistic distortions. This implies strong nonlinear variations as function of time and position, between low and high values of local Stoner enhancements and $`\omega _{sf}`$. If the development of a spin wave is strongly coupled to the atomic distortions, as is suggested from the calculations, it is unlikely that the excitation spectrum for the spins would be given by $`\omega _{sf}`$, since that quantity is independent of the phonons. It is more realistic if the spin excitation spectrum is connected to $`\mathrm{\Omega }_D`$. The nonlinear variations of $`S`$ permits a rapid development of a spin wave ($`\omega _{sf}\mathrm{\Omega }_D`$) when the local $`S`$ is small, alternated by strong coupling when $`S`$ is large. Simultaneous large of values of the prefactor and $`S`$ can explain a much larger $`T_C`$’s than if $`T_C`$ is evaluated from spin fluctuations alone. A major difficulty for quantitative results from LSDA calculations is that the tendency towards AFM is too weak. As indicated above, the exchange integral (or $`N`$) needs to be larger to explain a gap in the undoped system. If such an increase can be justified for the modulated cases, it will make the difference between high and low $`S`$ values along a phonon distortion even more spectacular. The average LSDA values for $`\overline{S}`$ are about 0.5 in the modulated cases, corresponding to a $`\lambda _{\mathrm{sf}}`$ of the order 1. Omission of effects from strong coupling and non-linearity in a BCS-like formula with a frequency prefactor of 50 meV as for oxygen phonon modes, leads to a large $`T_C`$ of the order 200 K. This is very approximate, but it shows qualitatively the possibilities of having a large $`T_C`$ from large AFM enhancements in combination with high excitation frequencies. Impurities and strong electron phonon coupling are destructive to superconductivity based on the paramagnon mechanism . However, with spin-phonon coupling there are mutual enforcements between phonons and spin waves which can make $`T_C`$ more insensitive to perturbations or disorder. Spin-phonon coupling would be consistent with a number of unusual observations among the high-$`T_C`$ materials such as an isotope effect on TC and pseudo gaps, even in the case of pairing mediated by spin fluctuations. A crucial test of spin-phonon coupling would be to measure the isotope effect on the spin excitation spectrum, since large isotope shifts are expected from the model.

The calculations show that the conditions for AF depend sensitively on the local structure around Cu. This effect is probably more important than in the present results, since LSDA calculations underestimate the tendency towards AF. Therefore, it can be concluded that spin-phonon coupling is important in these materials. Similar charge transfers caused by phonons and spin waves, or charge transfers induced by stripe-like spin waves alone, give a second gap in the DOS just below the main gap at $`E_F`$. The energy difference between the gaps depends on doping, and as was shown previously , the wave length of the stripes are predicted to vary with doping as well. Other effects from spin-phonon coupling are consistent with many observations in the high-$`T_C`$ oxides. In particular, this coupling might be important for the mechanism of high-$`T_C`$ superconductivity.


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

## I Introduction

The C15-Laves phase CeFe2 compound, which crystalizes in the form of cubic MgCu2-type structure, is an unstable ferromagnet with a Curie temperature, TC $``$235K. On doping with small concentrations of metals like Co, Ru, Ir, Al, Os, Re etc., at the Fe-site, the ferromagnetic (FM) behaviour disappears at low temperature, and the pseudobinary system Ce(Fe1-xRx)2 exhibits a stable antiferromagnetic (AFM) phase  below a certain temperature which we shall henceforth refer to as TN. There exists an extensive amount of research work on this interesting magnetic system. Various experimental tools have been employed to know the true magnetic state of Ce sublattice and the instablities related with the Fe-sublattice. Studies based on neutron scattering , magnetic circular X-ray dichroism , magneto-optic Kerr effect , high energy spectroscopy (including x-ray photoemission, absorption, ultraviolet) , magnetic Compton scattering , specific heat , magnetisation , magnetotransport  ac-susceptibility  etc. have been reported in pure and doped CeFe2 alloys. While these studies were mainly associated with the understanding of the magnetic instability in Ce(Fe1-xRx)2, we have recently started probing the exact nature of the magnetic phase transition (AFM to FM), whcih can be driven by high enough magnetic field (H) even at temperatures (T) much below TN $``$ 100K. Our preliminary attempt on this front started initially with the ac-susceptibility study  and investigation of the DC-magnetisation behaviour  in the Ru- and Ir-doped CeFe2 alloys, namely, the polycrystalline Ce(Fe0.95Ir0.05)2 and Ce(Fe0.93Ru0.07)2 samples. In these studies (based primarily on arguments of hysteresis and phase coexistence) the AFM to FM transition is found to be of first order in nature. Due to the very narrow hysteretic regime in these Ru and Ir doped CeFe2 alloys, we decided to investigate the Ce(Fe0.96Al0.04)2 alloy wherein the AFM to FM transition is relatively gradual ; this sample also provided us a distinctly wider H-T phase space (permitted by the maximum magnetic field (i.e., 5.5T) in our SQUID magnetometer) for a more comprehensive study of the nature of magnetic transition in this system. This revealed further interesting DC-magnetisation behaviour  which along with some of our preliminary results of magnetotransport measurements , have led us to clearly establish the first order nature of the AFM to FM transition in the Ce(Fe0.96Al0.04)2 alloy. The present paper deals with our detailed magnetotransport study on the same sample used in Refs. and . Although preliminary results of magnetotransport study on Ce(Fe0.96Al0.04)2 have been published in (Ref.), in this paper we (i) extend our investigation regime in the the resistivity $`\rho `$ vs. T hysteresis data to higher H; (ii) present $`\rho `$ vs. H hysteresis data to lower T; (iii) measure minor hysteresis loops in $`\rho `$ vs. T; (iv) compare $`\rho `$ vs. T data obtained in zero-field cooled and field cooled cooling histories with that recorded while field cooled warming of the sample; and (v) study $`\rho `$ by following a more contrived history dependence of the external magnetic field. The present work shows that the Ce(Fe0.96Al0.04)2 compound can be taken as a model system where one can observe most of the generic features related with a first order phase transition. We interpret all these results in the light of a first order transition and its associated behaviour (e.g., hysteresis, phase coexistance, supercooling and superheating, field dependent thermomagnetic history of magnetotransport behaviour). In addition, a comparison of the present work on Ce(Fe0.96Al0.04)2 alloy has been made with the existing work on perovskite type manganese oxide compounds  at appropriate places.

## II Experimental

The Ce(Fe0.96Al0.04)2 alloy sample employed in the present magnetotransport study belongs to the same batch of samples used earlier in the study of bulk magnetic and transport properties , and neutron measurements. Details of the sample preparation and characterization can be found in Ref.. A commercial cryostat (Oxford Instruments Inc., UK) with a maximum magnetic field of 16T is being used for carrying out the four probe resistivity measurement as a function of temperature and magnetic field H applied transverse to the measuring current. The isofield $`\rho `$ vs. T data was recorded with the following different protocols:
1. Zero Field Cooling (ZFC): The sample was first cooled from above TC down to lowest temperature of measurement in zero field, then subjected to the magnetic field, and $`\rho `$(T) data was recorded during warming of the sample.
2. Field Cooled Cooling (FCC): The sample was subjected to desired magnetic field strength above its TC, and the $`\rho `$(T) data was recorded while cooling the sample.
3. Field Cooled Warming (FCW): The resistivity of the sample was measured as a function of T during warming of the sample which had been earlier field cooled to the lowest investigated temperature.

## III Results

Figure 1 shows the T-dependence of resistivity for the Ce(Fe0.96Al0.04)2 sample in absence of magnetic field recorded during the initial cooling cycle starting from 290K, as well as during the subsequent warming cycle. During the initial decrease in temperature, while the paramagnetic (PM) to FM transition is reflected in the change of slope in $`\rho `$ vs. T plot at about 200K, the rise of $`\rho `$ is observed below about 84K due to a second magnetic phase transition from FM to AFM ordered state. This second transition gets completed at about 35K (while cooling), below which the resistivity once again decreases with decrease in temperature. For comparison, we present in the inset of Fig.1 a dc-magnetisation, M vs. T plot for the same sample in 2mT magnetic field. The three magnetic phases marked as PM, FM and AFM in different T-regimes complements our present results of the resistivity measurement. During the thermal cycling (i.e., warming and cooling), the resistivity behaviour exhibited distinct hysteresis across the FM to AFM transition (see main panel of Fig.1).

In Figs.2a-d, $`\rho `$ vs. T plots for magnetic field strengths of 0.7T, 1.5T, 2.5T and 4.0T, are respectively shown for the three different histories of application of magnetic field, e.g., ZFC, FCC and FCW ($`\rho `$ vs. T plots in ZFC and FCC protocols for other fields; 0.5T, 2.0T and 3.0T can be found in Fig.4 of Ref..). As is evident from Figs.2a-d, the resistivity plots for all the three protocols - ZFC, FCC and FCW are strongly affected by the strength of the applied magnetic field across the FM-AFM transition. Note that both the onset and completion of AFM-FM transitions are shifted to lower temperatures in the presence of magnetic field. This shift is again found to be strongly field dependent. Compared to a value of $``$93K for completion of AFM-FM transition while warming the sample in the absence of field (see Fig.1), the same transition gets completed only by $``$46K when a magnetic field of 4T is applied (see Fig.2d). The magnetic field has another interesting effect in the low temperature AFM-state. Above a certain value of H (i.e., 0.5T), the FCC resistivity stays below the ZFC resistivity at low temperatures (see also Fig.4 of Ref.). At any temperature, this difference of resistivity is field-dependent, increasing with the applied magnetic field. Furthermore starting at 4.5K, the FCW-data overlapped with the FCC-data upto some field-dependent temperature. Above this temperature, the FCW-curve continues to rise (in contrast to the falling FCC-curve) until it merges with the ZFC-curve at some slightly higher T. Thus the $`\rho `$ vs. T curves under the FCC and FCW protocols show the downturn at different temperatures. It is to be noted here that above the merger point of FCW- and ZFC-$`\rho `$(T) curves, the $`\rho `$(T) curve of the FCC-protocol lies distinctly below that recorded in the FCW-protocol. We stress here that FCW-protocol is basically a minor hysteresis loop of second kind (as would be described in next para) initiated from the lowest investigated temperature.

Figure 3 shows the results obtained across what are called the ”minor hysteresis loops” (MHL’s) in absence of external magnetic field. Two kinds of MHL’s are recorded. In the first kind, the sample is initially warmed from sufficiently low temperature, and then from a predetermined temperature the sample is cooled back. The MHL initiated at 44.5K from the warming cycle (Fig.3) is an example of this kind. In the second kind, the sample is initially cooled (from well above TC) upto a predetermined temperature, and then it is warmed. The MHL’s inititated on the cooling curve at 60K, 75K and 84K in the Fig.3 are examples of this kind. It can be clearly seen that the two MHLs initiated near the onset and completion of AFM-FM transition, respectively at 44.5K and 84K are reversible. However, the MHL’s initiated from cooling curve at 60K and 75K followed an altogether different path. They finally merged with the warming curve (initiated from 4.5K, and would be henceforth referred to as envelope warming curve).

The isothermal $`\rho `$ vs. H data was also recorded at various temperatures ranging from 2K to 120K. We show in Figs.4a and 4b, the $`\rho `$ vs. H data for the lowest temperature (i.e., 2K) and at 100K, respectively. Within our accuracy of measurements, the $`\rho `$ vs. H plots for T $``$ 100K were found to be linear right from 0T. As pointed out previously , the $`\rho `$(H) behaviour at lower temperatures is quite interesting. A small rise in $`\rho `$ with initial increase of H (within the AFM regime) along the virgin-curve is observed only at 2K (see Fig.4a).

Finally, we present in Fig.5, the results of resistivity measurements in 0.7T magnetic field during a warming cycle starting from 4.5K temperature point which has been approached using an altogether different protocol. In this protocol, the final state (i.e., 4.5K,0.7T) is being prepared following two steps. The first step involved the FCC protocol in 2.5T from above TC to 4.5K. Subsequent to this, in a second step, the field was reduced isothermally from 2.5T to 0.7T (these two steps are indicated as path-I in the inset of Fig.5). For the purpose of comparison, the $`\rho `$(T) plots for FCC and FCW protocols at 0.7T (corressponding to cooling and warming along the path-II as indicated in the inset of Fig.5) are also shown in Fig.5. With the initial reduction of field from 2.5T to 0.7T field at 4.5K, the resistivity value showed a jump (as indicated by a vertical arrow from point marked ”A” at 4.5K in Fig.5) to a value (marked as point ”B”, Fig.5) which was smaller than the $`\rho `$(4.5K,0.7T) value recorded in any of the conventional ZFC, FCC or FCW measurement protocols for H=0.7T. However, on subsequent warming of the sample, the resistivity was found to increase as shown in Fig.5 until it finally merged with the $`\rho `$ vs. T curve in 0.7T corressponding to the FCW protocol.

## IV Discussion

### A First order AFM to FM transition and the associated hysteresis

Based on the $`\rho `$ vs. T data, we first argue that with increase in temperature and/or field, the low temperature low field AFM phase transforms to FM phase through a FOT. The first indication of a FOT comes in the form of hysteresis in resistivity which is observed in both the temperature (Figs.1 and 2) and field cyclings (Fig.4). During the cooling of the sample, the onset of the rise of resistivity starts with the nucleation of AFM phase at $``$84K (Fig.1). This upturn in resistivity basically occurs due to the appearence of magnetic superzones at the onset of FM-AFM transition  (i.e., at TN). Further cooling converts more and more fraction of the sample from FM state to AFM state, with the result that the entire sample transforms into AFM state below about 35K. During the warming cycle, the decrease in resistivity at the transition is slightly delayed compared to the cooling cycle, and starts at around 48K. This decreasing $`\rho `$(T) across the transition is again associated with the more and more fraction of sample getting converted into FM-state. Within the hysteretic resistivity regime, the difference in resistivity values at any temperature is associated with the relative fraction of coexisting phases. (i.e., at any temperature within the hysteretic $`\rho `$(T) regime, this fraction has a different value for the cooling and warming cycles.)

It is to be emphasized here that the transition from AFM to FM state during the warming cycle completes at distinctly higher temperature ($``$ 93K) than the onset of FM to AFM transition ($``$ 84K) during a cooling cycle. Similar to this, the onset of AFM to FM transition during warming cycle takes place at a relatively higher temperature (i.e., $``$ 48K) compared to completion of FM to AFM transition at $``$ 35K during the cooling cycle. The difference in the two temperatures at both the ends of the hysteretic regime is an indication that the FM to AFM transition in the present investigations of Ce(Fe0.96Al0.04)2 is first order in nature. As we shall see later, the effect of the applied field is to affect these various transition temperatures and the magnitude of thermal hysteresis in the resistivity (Fig.2).

We wish to state here that the FM to AFM transition in the present case of Ce(Fe0.96Al0.04)2 sample is quite broad on temperature axis in comparison to relatively sharp FM to AFM transition observed in single crystal manganese oxide perovskite samples . The broadening of a first order transition with the disorder in the sample is predicted theoretically  way back in 1979, and very recently the magneto-optic imaging study on the vortex matter of single crystal Bi-2212 sample has shown how the disorder leads to a distribution of transition temperatures and/or fields across the solid to liquid melting transition, which leads to heterogeneous nucleation across the transition . We believe that a similar distribution of transition temperatures and/or fields exists in the present case of polycrystalline sample of Ce(Fe0.96Al0.04)2. Accordingly, the transition from one magnetic phase to another magnetic phase in the present work on Ce(Fe0.96Al0.04)2 should be designated here by a band, instead of a transition line on H-T phase space.

### B Minor Hysteresis Loops and Phase-coexistence

The study of minor hysteresis loops  (MHL’s) has been recently recognised as an important experimental technique to study the phenomenon of phase coexistence across the FOT in more detail . Our magnetotransport results (Fig.3) provide support in favor of phase coexistence across the foregoing AFM to FM transition. Consider the MHL’s that were initiated well inside the hysteretic regime. They showed a strong irreversible behaviour. For example, the MHL initiated on cooling cycle at 60K, during its course (i.e., while warming) did not come reversibly along the $`\rho `$(T) of cooling curve due to the already transformed AFM phase at 60K. Instead, a slight increase in resistivity with T is observed along this initial course of MHL due to the temperature dependence of transformed AFM phase akin to $`\rho `$(T) behaviour in the low temperature AFM regime below 35K. On further warming along the MHL, this increasing resistivity behaviour changes back to decreasing resistivity behaviour due to more and more AFM to FM conversion with the result that the MHL finally merges with the envelope warming cycle at about 70K. The evidence of (a) phase coexistence and (b) the hysteresis due to the different fractions of FM and AFM phases is clearly obvious from the fact that the resistivity of the sample measured at any temperature within the irreversible portion of MHL, is drastically different than that recorded along either the envelope cooling or warming cycle at the same temperature.

On the other hand, the reversible behaviour of MHL initiated from the warming-cycle at 44.5K (a temperature at which a distinct thermal hysteresis in resistivity exists between the envelope cooling and warming cycles) comes due to the fact that the onset of nucleation of FM has not taken place until 44.5K during the warming cycle. Thus while the sample is purely in the AFM state until 44.5K during warming cycle, a finite fraction of the sample continued to remain ferromagnetic upto 35K while cooling. With the same argument, the MHL initiated from the cooling cycle at 84K which took a overlapping course along the envelope cooling cycle indicated the absence of any AFM phase at or above 84K during the initial cooling cycle. This state of the sample (i.e. fully FM) at 84K during the cooling cycle (as well as along the MHL under consideration) is in sharp contrast to that along the envelope warming cycle where the sample contains a finite fraction of AFM phase (which is yet to transform into FM state) for even for T$`>`$84K as indicated by $`\rho `$ vs. T plot for 84K$`<`$T$`<`$93K (Fig.3). We note here that a clear co-existence of FM and AFM phases was also observed in zero field neutron measurement  in a substantial T-regime below the onset of the phase transition in Ce(Fe1-xAlx)2 samples with 0.2$``$x$``$0.08.

### C Metamagnetic transition and associated metastabilities

The $`\rho `$ vs. H plots for T $``$ 100K exhibited typical ferromagnetic response i.e., negative magnetoresistance which increases in magnitude with field right from H = 0. However, at lower temperatures, the $`\rho `$ vs. H plots in the virgin as well as field increasing envelope cycle showed field induced AFM to FM transition, commonly referred to as ”metamagnetic transition”, resulting from spin-flipping in the AFM phase at high enough fields . The decrease of resistivity due to onset of ferromagnetism at Hm(T) continues (due to conversion of more and more antiferro-phase into ferro-phase) until some higher field after which the resistivity decreases linearly with the field indicating the usual negative magnetoresistance ($``$ H) behaviour of the fully transformed high field FM state of the entire sample. We note here that the positive magnetoresistance behaviour (i.e., $`\rho `$ increasing with increase in H) of the AFM state is distinctly observed only in the low temperature $`\rho `$ vs. H plot recorded at 2K (Fig.4a). This positive sign of magnetoresistance in a AFM state is consistent with the previous reports  on Fe-Mn-Cr ternary alloys.

Along the H-decreasing envelope branch of a $`\rho `$ vs. H curve (for T $``$ 80K), the entire sample remains in the form of high field FM phase down to relatively lower field values compared to those along either the virgin curve or the H-increasing envelope curve. This is expected across a first order transition  as a sign of metastable behaviour due to (a) the supercooling of the high field FM phase below the transition field, and (b) superheating of low field AFM phase above the transition field, when field is cycled across the transition field (i.e., Hm line or more prescise Hm-band). Further, one expects that for some value of H below Hm(T) the resistivity behaviour of the sample should once again become AFM like. However, the results of Fig.4a (this work) and Fig.2 of Ref.) clearly show that this is not the case with Ce(Fe0.96Al0.04)2. This is so because resistivity along the H-decreasing envelope curve is anomalous since on cycling the field back to H=0, the resistivity value corresponding to the low field stable AFM phase \[i.e., that of H-increasing envelope curve (in case of T$`>`$10K) and/or virgin curve (in case of T$``$10K)\] is not completely restored back, with the result that a ”open hysteresis loop” is being obtained. Similar behaviour was found in virgin curve initiated in negative H direction for T$``$10K (Ref.). This indicates that FM phase persists in some finite quantity even at zero field after being cycled from +Hmax or -Hmax. It is to be recalled here that although similar open hysteresis loops were also reported for Nd0.5Sr0.5MnO3 (Ref.), the hysteresis loops in case of Pr0.5Sr0.5MnO3 did not display any such open hysteresis loop (Ref.).

At lower temperatures, the anomalous open hysteresis loop in the $`\rho `$(H) behaviour is manifested in the form of another anomaly below 10K, in that the virgin resistivity curve lie outside the butterfly shaped (envelope) hysteresis loop (e.g., Fig.4a, the resistivity along the virgin $`\rho `$(H) curve remains (upto Hm or so) distinctly above both the envelope H-increasing as well as H-decreasing $`\rho `$ vs. H curves.). In case of magnetisation measurement, this anomaly is observed in the form of virgin M(H) curve lying outside the butterfly (envelope) hysteresis loop . We would come back to this anomalous result below Hm a little later. We are unaware of any such comparison based on the resistivity measurements in all the three protocols (i.e., along the virgin, field-increasing envelope, and field-decreasing envelope curve) exists for either Nd0.5Sr0.5MnO3, Nd0.25Sm0.25Sr0.5MnO3 and/or Pr0.5Sr0.5MnO3 (Refs.\[37-39\]).

### D Limits of metastability: effect of magnetic field on the temperature dependence of resistivity

It is important here to recall that there exists a limit of metastability , below (above) the first order transition line (in our case, the Hm(T) or TN(H)) upto which one can supercool (superheat) the high (low) field phase. Outside these two bounds (designated as T(H) for supercooling, and T∗∗(H) for superheating) on either side of the transition line, no metastable behaviour, and hence no superheating and/or supercooling can be observed. (Recall that like TN(H), as stated earlier these two bounds T(H) and T∗∗(H) should be represented by the bands in the present case of polycrytalline Ce(Fe0.96Al0.04)2 sample.). It is also known that the metastable region widens with increase (decrease) of field (temperature). Natural question at this moment is - do we see such features of FOT in the present $`\rho `$(H,T) data of Ce(Fe0.96Al0.04)2 sample?

The comparison of the resistivity behaviour recorded on the Ce(Fe0.96Al0.04)2 sample under different protocols (ZFC, FCC, and FCW) has turned out to be very interesting, and displays almost all the above mentioned generic features of a first order phase transition. We find that the magnetic field has a very drastic effect on the $`\rho `$(T) behaviour, e.g., with increasing magnetic field,
(a) the completion of FM to AFM transition while cooling the sample (which marks the lower limiting value of T(H)-band, and is inferred by the temperature below which the FCC and FCW-resistivities merge) is suppressed much faster than the decrease in the onset of AFM to FM transition temperature while warming the sample (i.e., the upper limiting value of T∗∗(H)).
(b) the hysteretic regime is substantially enhanced in temperature across the transition, and
(c) most importantly, the low temperature reversible $`\rho `$(T) regime (with respect to the overlapping ZFC and FCC) disappears by H$``$0.7T.

These results ((a) and (b) above) clearly imply that with the increase in H, the lower limit of metastability, T(H) band (below which one should see the reversible response of the stable AFM phase) gets suppressed (towards lower temperature) even faster in comparison to T∗∗(H) band, and the metastable regime (existing between lower limiting value of T(H) band and the upper limiting value of T∗∗(H) bands) thus widens with the decrease in T or with increase in H. This is further supported from the isothermal $`\rho `$ vs. H data, where the hysteretic field regime drastically increased at low temperatures (Fig.4a). Based on these T dependence of resistivity in differents fields, a phase diagram using the mid point of T(H)- and T∗∗(H)-band has been shown in our preliminary work .

Along the FCW curve, the resistivity rising past this merger point of FCW and FCC exhibits the superheating of low temperature AFM phase. The FCW curve finally merges with the ZFC curve at a temperature where the supercooled (metastable) FM-phase formed during the FCC-protocol vanishes. Above this field dependent merger temperature of FCW and ZFC resistivities, the sample comprises of three fractions;
1. stable transformed/nucleated FM phase,
2. superheated metastable AFM phase, and
3. stable AFM phase which has not yet transformed in FM-phase becuase of the distributuion in the TN’s in the sample.

It is now quite evident that the present study of $`\rho `$(T) under different histories of applied magnetic field (i.e., ZFC, FCC, and FCW) in Ce(Fe0.96Al0.04)2 has an edge over the previous work on Nd0.5Sr0.5MnO3, Nd0.25Sm0.25Sr0.5MnO3 and/or Pr0.5Sr0.5MnO3, where resistivity data is compared only during FCC with FCW .

From the thermomagnetic irreversibility increasing with the field as observed in the DC-magnetisation data of the same Ce(Fe0.96Al0.04)2 sample , it was argued that the hysteresis in the magnetisation vs. field was entirely due to the first order nature of the magnetic transition rather than arising due to pinning of the domians formed in the FM state. All the results of present magnetotransport study are in excellent agreement with those observed in the DC-magnetisation studies . This is so because, the hysteresis observed in the present bulk magnetotransport behaviour can not be again related with the domain formation, since the domain size is normally much greater than the mean free path of the carriers .

### E Anomalous aspects of thermomagnetic history effects across the AFM to FM transition

We once again recall here that in case of first order transition, the free energy barrier between the stable AFM phase and the metastable FM phase ceases to exists just below the T(H), and any infinitesimal fluctuations can drive the entire sample to stable AFM below the T(H) line/band . But, a few questions still remain unanswered in this picture:
1. Why does not the resistivity of the sample recorded in FCC and FCW protocol restore back to that recorded in ZFC protocol at lower temperatures (e.g., at 5K) for H $``$ 0.7T? (We tend to believe that similar feature would appear in case of resistivity behaviour in Nd0.5Sr0.5MnO3 and Pr0.5Sr0.5MnO3.) In our magnetisation studies on same Ce(Fe0.96Al0.04)2 sample , this anomaly is reflected in the observation that the FC magnetisation curve MFC(T) lie above the MZFC(T).
2. Why does the virgin $`\rho `$ vs. H curve lie outside the envelope butterfly $`\rho `$(H) loop at lower temperatures, T$``$10K?
3. Why is the full AFM resistivity not distinctly restored at H=0 on the envelope H-decreasing $`\rho `$ vs. H curve?

It is once again to be remembered that structural transition in Ce(Fe1-xAlx)2 system for 0.2$``$x$``$0.08 from cubic to rhombohedral accompanies the AFM/FM transition . We now argue here that every structural transition is characterized by a characteristic relaxation time, which increases with decreasing temperature due to reduction in the displacive motion of the atoms . A typical example is the supercooled liquid-to-glass transition. It is our conjecture that in the present case of Ce(Fe0.96Al0.04)2 sample, this characteristic relaxation time at low temperature may become much larger than the actual experimental time scale with the result that kinetics of transition gets hindered. Within this picture, the anomalies enumerated above can be explained as follows. When the temperature is lowered, some high temperature high field metastable FM phase remains frozen-in resulting in the arrest of FM to AFM transition at low temperature. In the $`\rho `$ vs. H cycling, due to the low temperature, a finite amount of supercooled FM phase continues to exist even when the applied field is reduced to zero. (Note that the magnetic field also induces the structural transition in Ce(Fe0.96Al0.04)2 (Ref.).) This metastable FM phase is then carried over when the direction of field is changed, and results in an H-decreasing (increasing) envelope curve that lie below the virgin curve recorded in the negative (positive) H direction. As expected, such hysteresis loops are not seen at higher temperatures ($`>`$10K).

Another evidence supporting the presence of hindered kinetics which, if not considered properly, might tempt one to draw false conclusion about the lower limit of metastable behaviour, comes from the results of Fig.5. As discussed above, the initial field cooling of the sample in a magnetic field of 2.5T results into a finite fraction of high temperature FM phase existing at 4.5K due to the hindered kinetics as mentioned in the preceeding para. Subsequent to this FC protocol, the isothermal (i.e., at 4.5K) field reduction from 2.5T to 0.7T yielded a resistivity value which is significantly smaller than either of $`\rho `$(4.5K,0.7T,ZFC) and/or $`\rho `$(4.5K,0.7,FCC/FCW), indicating as if the metastable behaviour in the sample existed at or below 4.5K in 0.7T field. This we believe is due to the hindered kinetics because while cooling the sample in 2.5T a large fraction (compared to 0.7T, FCC state at 4.5K) of supercooled high temperature FM phase is frozen, i.e., its transformation to stable AFM phase at T(H) gets arrested. As a result, the resistivity of the sample at 4.5K after the field is reduced to 0.7T is significantly smaller than the FCC/FCW resistivity in 0.7T at 4.5K. On warming the sample, this anomalously low resistivity of the sample at 4.5K increases fast (as the sample gains energy in the warming process), and the resistivity merges at about 20K with that of kinetically hindered resistivity curve of 0.7T. We thus say that compared to field cooling in 0.7T to 4.5K (i.e., path II in inset of Fig.5), the kinetics of the FM to AFM transition experienced relatively more hindrance when the sample was field cooled to the same 4.5K, 0.7T point but following path ’I’.

It is to be noted here that results obtained follwoing path-I experimental protocol (Fig.5) are similar to the results of magnetic annealing effect reported in the Cr-doped manganite crystals of Nd0.5Ca0.5Mn1-yCryO3 (See Fig.2b of ref.). \[We believe that the value of magnetisation at 5K in their sample at the annealing field of 7T (which is not shown in Ref.) would be much larger than the value obtained after field was reduced to 0.5T at 5K (See Fig.2b of Ref.).\] The authors of ref. explained their data on the basis of random field quenching due to Cr-substitution which produced the FM-microembryos. Our experimental results of magnetotransport studies (Fig.5) are ascribed with arresting of the first order transition process at low temperature and high magnetic field. We further wish to point here that we have confirmed the magnetotransport results of Fig.5 by DC-magnetisation measurement (which are not shown here for the sake of concizeness) following similar path-I as indicated in the inset of Fig.5.

In the Ref., the hindrance to the kinetics of the transition has been indicated on the H-T phase diagram through a (Hk,Tk) band (see Fig.3b of Ref.). The reader is referred to Fig.3c of Ref. and the related text for a more illustrative understanding of hindered kinetics in the present case of Ce(Fe0.96Al0.04)2.

## V Conclusion

The magnetotransport behaviour across the first order phase transition from low field and low temperature antiferromagnetic state to high field and high temperature ferromagnetic state has been studied in Ce(Fe0.96Al0.04)2 polycrystalline sample. This study on Ce(Fe0.96Al0.04)2 has clearly demonstrated the various generic features of a first order phase transitions, viz., hysteresis, phase coexistence, field dependent limits and existence of the metastable supercooled and superheated phases across the transition boundary in a magnetic system. These results of magnetotransport study not only supported our previous work of dc-magnetisation study on the same sample, but also provided new results extending to relatively higher magnetic field and low temperature regime on the H-T phase space. We found some unusal magnetoresistance behaviour (most interesting one is the virgin resistivity curve lying outside the envelope resistivity loop) at lower temperatures. Based on the observed magnetotransport behaviour using an unconventional history of application of magnetic field, we have ascribed the origin of these unusal features with the arresting of the transition at lower temperature.
Acknowledgements
We thank R.K. Meena and Anil Chouhan for the assistance provided in the magnetotransport measurements.
Corresponding author, E-mail : sujeetc@cat.ernet.in


text:
# Production of neutrons, neutrinos and gamma-rays by a very fast pulsar in the Galactic Center region

## 1 Introduction

Recently the AGASA collaboration has reported the existence of an extended excess of cosmic rays (CRs) over a narrow energy range $`10^{17.9}10^{18.3}`$ eV from directions close to the Galactic Center (GC) and the Cygnus region with the significance of 4.5$`\sigma `$ and $`3.9\sigma `$, respectively (Hayashida et al. 1999). The GC excess was confirmed in the analysis of the SUGAR data (Bellido et al. 2001), in which case the observed signal in the energy range $`10^{17.9}10^{18.5}`$ eV is consistent with that from a point-like source of neutral particles, with an estimated flux of $`(9\pm 3)\times 10^{14}`$ m-2 s-1, offset from the true location of the GC by about $`7.5^\mathrm{o}`$. Hayashida et al. (1999) suggested that such an anisotropy of CRs in a narrow energy range can be explained naturally by neutrons due to the fact that particles with such energies are able to reach the Earth before decaying from distance of the GC. Numerical simulations of charged particles (protons) propagation in reasonable models of the Galactic magnetic field give rise to the more extended source which may even be significantly shifted in the sky from the original direction towards the source (e.g. Clay 2000, Bednarek, Giller & Zielińska 2001). However, the results of charged hadrons propagation strongly depend on the details of the magnetic field model which is not well known at present.

The production of neutrons in discrete galactic sources was already discussed some time ago by Jones (1990), Sommers & Elbert (1990) and Bednarek (1992) in relation to reports of the excess of EeV particles from the direction of Cygnus X-3 (Cassiday et al. 1989, Teshima et al. 1990). It has recently been suggested that in the GC region neutrons might be produced in collisions of hadrons with matter (Takahashi & Nagataki 2001). Hadrons can be accelerated by a massive black hole associated with the Sgr A (Levinson & Boldt 2000), or by the shock waves of supernovae which explode into their own stellar winds (Rhode, Enslin & Biermann 1998).

The Galactic Center region (inner $`50`$ pc) is rich in many massive stellar clusters with a few to more than 100 OB stars (Morris & Serabyn 1996, Blum et al. 2001). These stars should soon explode as supernovae. In fact recent multiple supernova explosions in the GC region ($`10^3`$ supernovae in the past $`10^5`$ years) are suggested by the observations of the diffuse hot plasma emitting X-rays (Yamauchi et al. 1990). For example one remnant of such a young supernova with the age of $`80`$ years (G0.570-0.018) has recently been reported by Senda et al. (2001). Since it is expected that pulsars are formed in explosions of such massive stars, we can expect that the GC region should contain some young pulsars, a number of them being $`10^210^3`$ yrs old. Motivated by these observational results we may assume that at least one of these young pulsars, formed in a supernova explosion of the type Ib/c, has parameters which allow the acceleration of iron nuclei to energies $`10^{20}`$ eV, as postulated by some models for the Galactic origin of the highest energy cosmic rays (Blasi, Epstein & Olinto 2000; De Goubeia Dal Pino & Lazarian 2000). We suggest that neutrons from desintegration of iron nuclei, which are accelerated by such energetic pulsar in the GC region, can be responsible for the observed excess of the cosmic rays with energies $`10^{18}`$ eV. Note that the iron nuclei with energies $`10^{20}`$ eV and neutrons with energies $`2\times 10^{18}`$ eV have the same Lorentz factors. In order to test this hypothesis we predict the neutrino and $`\gamma `$-ray fluxes accompaning the process of neutron injection by iron nuclei.

## 2 A pulsar inside a molecular cloud

We investigate the scenario in which a very young pulsar is formed in a core collapse of the type Ib/c supernova immersed within a huge molecular cloud (or high density medium), characteristic of the GC region. Such supernovae are probably projenitors of neutron stars with extreme parameters (period, magnetic field surface), which allow them to accelerate iron nuclei to the highest energies observed in the CRs. In about a year after supernova explosion, the pulsar is surrounded by such a dense expanding envelope that hadrons, accelerated in the pulsar magnetosphere or the pulsar wind zone, are not injected into the surrounding. These hadrons lose energy on multiple inelastic collisions producing high energy neutrinos (Protheroe, Bednarek & Luo 1998, Bednarek 2001, Beall & Bednarek 2001). In later stages the particles can escape into the surrounding and diffuse in the magnetic field of the cloud, suffering collisions with the matter from time to time. In our further considerations we discuss, as an example, two media typical of the GC region in which the pulsar may be immersed. The first one is a huge molecular cloud with the radius $`R_\mathrm{c}=10`$ pc, the density $`n_\mathrm{c}=10^3`$ cm-3, and the magnetic field $`B_\mathrm{c}=10^4`$ G ( the total mass $`10^5M_{}`$), and the second one is an extended high density region inside the GC with $`R_\mathrm{c}=50`$ pc, $`n_\mathrm{c}=10^2`$ cm-3, and $`B_\mathrm{c}=3\times 10^5`$ G (the total mass $`10^6M_{}`$). The clouds with such parameters are typical of the GC region and of the Nuclear Bulge, which is a narrow layer of the interstellar matter in the central $`600`$ pc of the Galaxy with the height of $`50`$ pc.

### 2.1 Acceleration of nuclei by a pulsar

Following the recent works of Blasi, Epstein & Olinto (2000), Beall & Bednarek (2001), and Bednarek (2001) we assume that pulsars can accelerate iron nuclei in its wind zone (the mechanism called magnetic slingshot, Gunn & Ostriker 1969). The maximum energies which the nuclei can reach in this model, are determined by the magnetic field energy per particle in the pulsar wind zone and depend on the pulsar parameters as,

$`E_{\mathrm{Fe}}={\displaystyle \frac{B^2(r_{\mathrm{LC}})}{8\pi n_{\mathrm{GJ}}(r_{\mathrm{LC}})}}1.8\times 10^{11}B_{12}P_{\mathrm{ms}}^2\mathrm{GeV},`$ (1)
where $`P=10^3P_{\mathrm{ms}}`$ s is the pulsar period, $`B=10^{12}B_{12}`$ G is the pulsar’s surface magnetic field, $`n_{\mathrm{GJ}}=B(r_{\mathrm{LC}})/(2ecP)3.3\times 10^{11}B_{12}P_{\mathrm{ms}}^4`$ cm$`^_3`$ is Goldreich & Julian (1969) density, $`r_{\mathrm{LC}}=cP/2\pi 4.77\times 10^6P_{\mathrm{ms}}`$ cm, and $`c`$ is the velocity of light. According to the slingshot mechanism, the acceleration of nuclei occurs very fast so that they do not lose energy during this stage. During the first $`1`$ yr after explosion these nuclei interact with the radiation field and matter of the supernova envelope (Beall & Bednarek 2001). Only when the envelope becomes transparent, can the iron nuclei be injected into the surrounding of the parent pulsar’s supernova. We obtain the spectrum of iron nuclei injected by the pulsar following the derivation by Beall & Bednarek (2001). Their calculation is based on the general prescription given by Blasi, Epstein & Olinto (2000) in which the number of nuclei accelerated to energies $`E`$ scales as a part $`\xi `$ of the Goldreich & Julian (1969) density at the light cylinder radius. Beall & Bednarek (2001) modify this approach by noting that the spectrum injected by the pulsar at a fixed time ’t’ should be non-monoenergetic due to the fact that the magnetic energy density, responsible for the acceleration of particles, changes along the pulsar’s light cylinder height. As a result, a pulsar with specific parameters injects nuclei with the spectrum which can be below $`E_{\mathrm{Fe}}`$ described by (see details in Beall & Bednarek 2001),

$$\begin{array}{c}\frac{dN}{dEdt}=\frac{2\pi c\xi r_{\mathrm{LC}}^2n_{\mathrm{GJ}}(E_{\mathrm{Fe}}E^2)^{1/3}}{3\left[(E_{\mathrm{Fe}}/E)^{2/3}1\right]^{1/2}}\hfill \\ \frac{3\times 10^{30}\xi (B_{12}P_{\mathrm{ms}}^2E^1)^{2/3}}{\left[(E_{\mathrm{Fe}}/E)^{2/3}1\right]^{1/2}}\frac{\mathrm{Fe}}{\mathrm{s}\mathrm{GeV}}.\hfill \end{array}$$
(2)
We estimated that these nuclei can escape through the supernova envelope after $`1`$ yr after the supernova explosion for typical parameters of the supernova, i.e the mass of the envelope in the case of type Ib/c supernovae $`M_{\mathrm{env}}=3M_{}`$, and the expansion velocity of the envelope at the inner radius is $`v_{\mathrm{env}}=3\times 10^8`$ cm s-1 (Beall & Bednarek 2001). The iron nuclei diffuse in the magnetic field of the high density medium in the GC region, i.e. huge molecular clouds. Some of them interact producing neutrons, neutrinos, and $`\gamma `$-rays.

In order to obtain the equilibrium spectrum of iron nuclei inside the cloud, we have to integrate over the activity time of the pulsar since its parameters evolve in time due to the pulsar’s energy losses. If we assume that the pulsar loses energy only on electromagnetic waves, then its period changes according to the formula $`P_{\mathrm{ms}}^2(t_{\mathrm{obs}})=1.04\times 10^9t_{\mathrm{obs}}B_{12}^2+P_{0,\mathrm{ms}}^2`$, where $`P_{0,\mathrm{ms}}`$ $`P_{\mathrm{ms}}(t_{\mathrm{obs}})`$ are the initial and present periods of the pulsar. The equilibrium spectrum of iron nuclei at a specific observation time, $`t_{\mathrm{obs}}`$, is calculated from

$`{\displaystyle \frac{dN}{dE}}={\displaystyle _{t_0}^{t_{\mathrm{obs}}}}{\displaystyle \frac{dN}{dEdt}}Ke^{c(t_{\mathrm{obs}}t)/\lambda }𝑑t,`$ (3)
where $`t_0=1`$ yr, $`K`$ gives the part of nuclei produced at the time ’t’ which do not escape from the cloud due to the diffusion and are still present inside the cloud at the time $`t_{\mathrm{obs}}`$. $`\lambda `$ is the mean free path for collision of the iron nuclei with the matter of the cloud. Note that for the parameters considered in this paper the value $`c(t_{\mathrm{obs}}t)/\lambda `$, in Eq. 3, is always less than one. Therefore, a significant part of iron nuclei with energies $`10^{20}`$ eV can escape without interaction as postulated by the model of Blasi, Epstein & Olinto (2000). The value of $`K`$ is estimated from $`K=(R_\mathrm{c}/D_{\mathrm{dif}})^3`$, where $`D_{\mathrm{dif}}=(r_\mathrm{L}ct/3)^{1/2}`$ is the diffusion distance of iron nuclei in the magnetic field of the cloud, and $`r_\mathrm{L}`$ is the Larmor radius of the iron nuclei with energy $`E`$. For the case, $`D_{\mathrm{dif}}R_\mathrm{c}`$, we take $`K=1`$. We assume that the giant molecular cloud does not expand. So then the nuclei do not suffer adiabatic energy losses.

### 2.2 Interaction of nuclei inside the cloud

The part of iron nuclei confined within the molecular cloud, interact with a relatively dense medium suffering desintegrations and pion energy losses. The pions decay into neutrinos and $`\gamma `$-rays. Applying the equilibrium spectrum of iron nuclei (see Eq. 3), we calculate the differential spectra of neutrons (from desintegrations of the iron nuclei), muon neutrinos, and $`\gamma `$-rays (from inelastic collisions of iron). In these calculations we assume that: (1) in a single interaction, the iron nuclei desintegrate into two nuclei and the rest of neutrons is released with the Lorentz factors comparable to the Lorentz factor of the primary nuclei; (2) pions, produced in interactions of iron nuclei with the matter of the cloud, have Lorentz factors comparable to their parent nuclei. They are produced with multiplicities given in Orth & Buffington (1976).

The computations of differential neutron, neutrino, and $`\gamma `$-ray spectra have been done for the pulsar with the surface magnetic field $`B_{12}=6`$ (typical of the observed radio pulsars) and the initial period $`P_{\mathrm{ms}}=2`$. Such a pulsar is able to accelerate nuclei to such high energies (see Eq. 1) that neutrons from their desintegration fulfil the observational constraint put by the excess of cosmic ray particles at $`10^{7.9}10^{8.5}`$ GeV (Hayashida et al. 1999, Bellido et al. 2001). The pulsar born with such parameters slows down due to the dipole energy losses to 11 ms after $`10^2`$ yr, 34 ms ($`10^3`$ yr), 60 ms ($`3\times 10^3`$ yr), and to 106 ms ($`10^4`$ yr). So then it is still fast enough to produce pulsaed $`\gamma `$-rays (Crab and Vela type pulsars).

As an example in Fig. 1 we show the spectra of neutrons (dashed curves) and $`\gamma `$-rays (full curves) produced by the iron nuclei inside a cloud with the radius $`R_\mathrm{c}=10`$ pc, the density $`n_\mathrm{c}=10^3`$ cm-3 (the cloud mass $`10^5M_{}`$), and the magnetic field $`B_\mathrm{c}=10^4`$ G at different times after the pulsar formation $`t_{\mathrm{obs}}=10,10^2,10^3,3\times 10^3`$, and $`10^4`$ yrs. As expected, the spectra of neutrons extend up to a few $`10^{18}`$ eV. However, their intensities at these highest energies significantly drop with time after the pulsar formation due to the escape of iron nuclei from the cloud for the time $`t_{\mathrm{obs}}>10`$ yr, which is caused by their diffusion in the magnetic field. Due to the large multiplicities of pion production at these high energies, the maximum energies of neutrinos and $`\gamma `$-rays are about 2 orders of magnitude lower than for neutrons. Their spectra at the higiest energies also drop with time due to the escape of nuclei from the cloud.

## 3 Neutrons, neutrinos, and gamma-rays on Earth

The large distance to the GC, $`D_{\mathrm{GC}}8.5`$ kpc, has influence on the expected fluxes of neutrons and $`\gamma `$-rays measured on Earth, due to the decay of unstable neutrons and the absorption of $`\gamma `$-rays in the microwave background radiation (MBR). The mean free path for neutrons depends only on their energy, $`\lambda _\mathrm{N}=c\tau _\mathrm{N}\gamma _\mathrm{N}9.8E_{\mathrm{N},\mathrm{EeV}}`$ kpc, where a neutron’s lifetime is $`\tau _\mathrm{N}=918`$ s, its energy $`E_\mathrm{N}=9.38\times 10^{10}\gamma _\mathrm{N}`$ in EeV, and $`\gamma _\mathrm{N}`$ is the Lorentz factor. The mean free path for the absorption of photons in MBR, $`\lambda _{\gamma \gamma }`$, was computed in several papers just after the discovery of MBR (e.g. Gould & Schreder 1966). $`\lambda _{\gamma \gamma }`$ becomes comparable to the distance of the GC at energies of $`1`$ PeV. Therefore the fluxes of neutrons and $`\gamma `$-rays observed on Earth are reduced by the factor $`\mathrm{exp}(D_{\mathrm{GC}}/\lambda _{\gamma \gamma ;\mathrm{N}})`$, where $`\lambda _{\gamma \gamma ;\mathrm{N}}=\lambda _{\gamma \gamma }`$ or $`\lambda _\mathrm{N}`$ respectively. In Fig. 2, we show the fluxes of neutrons and $`\gamma `$-rays observed on Earth at different times after the pulsar formation for the case of the pulsar with the previously mentioned initial parameters and two different sets of parameters describing the medium in the GC region mentioned in section 2: the case of the molecular cloud (the upper figure), and the case of a more extended and lower density region around the GC (the lower figure). The comparison of Figs. 1, and 2 allows us to conclude that the absorption effects of $`\gamma `$-rays become important in the PeV energy range, and that neutrons with energies below $`10^8`$ GeV are not able to reach the Earth. Since the propagation of neutrinos is not influenced by any process, their fluxes can be simply obtained for the known distance to the GC. In Fig. 2 we mark also the observed spectrum of cosmic rays (CR) below $`3\times 10^{18}`$ eV within the $`20^\mathrm{o}`$ circle (the analysis box of the AGASA data). We find that only the pulsars born within the last $`3\times 10^3`$ yrs are able to provide fluxes of neutrons which exceed the CR limit, provided that they accelerate nuclei with the efficiency $`\xi =1`$ (see Eq. 2).

## 4 Discussion and Conclusion

The SUGAR group estimates the flux of particles which causes reported excess of the cosmic ray particles in the energy range $`10^{17.9}10^{18.5}`$ eV on $`(9\pm 3)\times 10^{14}`$ m-3 s-1 (Bellido et al. 2001). If this excess is caused by neutrons produced in the pulsar model discussed here, then the expected flux of neutrons can be compared with the observed one. Basing on this normalization we predict the fluxes of neutrinos and gamma-rays on Earth. This procedure allows us to derive the free parameter of our model (i.e. the efficiency $`\xi `$ of iron acceleration by the pulsar) and limit the age of the pulsar for other fixed parameters, $`P,B,R_\mathrm{c},n_\mathrm{c},B_\mathrm{c}`$, which are in fact constrained by the observations. We consider five different sets of parameters describing our scenario: model (I) R = 10 pc, $`n=10^3`$ cm-3, $`B_\mathrm{c}=10^4`$ G, $`t_{\mathrm{obs}}=10^4`$ yr; (II) $`t_{\mathrm{obs}}=3\times 10^3`$ yr and other parameters as above; (III) $`t_{\mathrm{obs}}=10^3`$ yr and other parameters as above; (IV) R = 50 pc, $`n=10^2`$ cm-3, $`B_\mathrm{c}=3\times 10^5`$ G, $`t_{\mathrm{obs}}=10^4`$ yr; and (V) $`t_{\mathrm{obs}}=3\times 10^3`$ yr and other parameters as in (IV). They all concern two sets of parameters for the medium in which the pulsar is formed, and differ in the pulsar’s age which is not constrained by any observations. In all these models we assume that the pulsar is born with $`B=6\times 10^{12}`$ G and $`P_\mathrm{o}=2`$ ms. Normalizing the predicted neutron flux to the observed excess of CR particles we derive the value of the parameter $`\xi `$ which has to be $`\xi 1`$ (model I), $`0.18`$ (II), $`0.03`$ (III), $`0.3`$ (IV), and $`0.09`$ (V).

Using the above estimates for $`\xi `$ we can now predict the expected fluxes of $`\gamma `$-rays and muon neutrinos and antineutrinos in the case of every model. The integral spectra of $`\gamma `$-rays from the GC region are presented in Fig. 3, together with the sensitivities of the present HEGRA telescope system and the planned next generation of telescopes, i.e. CANGAROO III, HESS, VERITAS. We also report in Table 1 the $`\gamma `$-ray fluxes above 1 TeV and 10 TeV in units cm-2 s-1. Although the $`\gamma `$-ray spectra have a maximum above 10 TeV for all models, the $`\gamma `$-ray fluxes in the energy range 1-10 TeV produced in models, (I) $`2.1\times 10^{12}`$ cm-2 s-1, and (II) $`2.1\times 10^{13}`$ cm-2 s-1, and probably also in (IV) $`8\times 10^{14}`$ cm-2 s-1, should be observed by the future systems of Cherenkov telescopes of the CANGAROO III, HESS, and VERITAS type. Models (III) and (V) predict fluxes below the sensitivity limit of these Observatories. Only the HEGRA Collaboration observed the Galactic disk including the GC region (Pöhlhofer et al. 1999). The upper limit on the possible sources, equals 1/4 Crab in the Galactic plane which is above the $`\gamma `$-ray flux predicted even by the model (I). However, since the GC region can be observed by this experiment only at zenith angles larger than $`60^\mathrm{o}`$, this limit does not refer to the GC region.

In Fig. 4 we show the muon neutrino and anti-neutrino spectra expected in the discussed model. At energies $`>10`$ TeV, these spectra are above the expected flux of atmospheric neutrino background (ANB) and also above the 3 yr sensitivity limit of the planned large size neutrino detector IceCube (Hill 2001). We estimate the number of muon neutrino events during one year in the IceCube detector basing on the calculations of the likelihood of detecting such neutrinos by a detector with a surface area of 1 km2 obtained by Gaisser & Grillo (1987). The results of these calculations are shown in Table 1. We distinguish the case of neutrinos coming to the neutrino detector from directions close to the horizon, i.e. not absorbed by the Earth ($`N_\nu ^{\mathrm{na}}`$), and neutrinos which arrive moving upward from the nadir direction, i.e. partially absorbed by the Earth ($`N_\nu ^\mathrm{a}`$) (for absorption coefficients see Gandhi 2000). From Table 1 it is clear that the IceCube detector should detect a few up to several neutrinos per year from the Galactic Center region provided that the excess of cosmic rays at $`10^{18}`$ eV from the GC region is caused by neutrons from desintegrations of iron nuclei, accelerated by a very fast pulsar. The detection of the predicted fluxes of neutrinos from the Galactic Center (or lack) will also place constraints on the recent model of extremely high energy cosmic ray production in the pulsar scenario (Blasi, Epstein & Olinto 2000), since the parent iron nuclei which inject neutrons with energies $`10^{18}`$ eV, have to be accelerated to energies $`10^{20}`$ eV.

The EGRET detector on board the Compton GRO has detected a strong $`\gamma `$-ray source with luminosity of $`2\times 10^{37}`$ erg s-1 (Mayer-Hasselwander et al. 1998). This emission seems to come from the extended region with the radius of $`80`$ pc around the GC. In another paper (in preparation) we suggest that this emission can be explained in terms of the general scenario discussed here if a part of energy of the accelerated iron nuclei is transferred to the relativistic positrons due to the resonant scattering in the pulsar shock region (see Gallant & Arons 1994). These positrons, accumulated in the cloud, produce high energy radiation in synchrotron and inverse Compton processes.

## Acknowledgements

This work is supported by the Polish KBN grant No. 5P03D02521.


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# A Thermodynamical Approach to Quantifying Quantum Correlations

## Abstract

We consider the amount of work which can be extracted from a heat bath using a bipartite state $`\rho `$ shared by two parties. In general it is less then the amount of work extractable when one party is in possession of the entire state. We derive bounds for this ”work deficit” and calculate it explicitly for a number of different cases. For pure states the work deficit is exactly equal to the distillable entanglement of the state, and this is also achievable for maximally correlated states. In these cases a form of complementarity exists between physical work which can be extracted and distillable entanglement. The work deficit is a good measure of the quantum correlations in a state and provides a new paradigm for understanding quantum non-locality.

Strong connections exist between information, and thermodynamics. Work is required to erase a magnetic tape in an unknown state Landauer  and bits of information can be used to draw work from single heat bath szilard Bennett-inf . The second law of thermodynamics forbids the drawing of work from a single heat bath, however, if one has an engine which contains ”negentropy” (bits of information) then one can draw work from it. The process does not violate the second law because the information is depleted as entropy from the heat bath accumulates in the engine. Typically, the source of information is particles in a known states, and these states can be thought of as a type of fuel or resource. In particular, quantum states can be used as fuelPeres , and recently, physically realizable micro-engines have been proposed Scully .

The field of quantum information theory has also yielded tantalizing connections between entanglement and thermodynamics forgetting . Bipartite states (jointly held by two parties) such as the maximally entangled state

$$\mathrm{\Psi }_{AB}=\frac{1}{\sqrt{2}}\left(|00+|11\right),$$
(1)
exhibit mysterious non-localities which can be exploited to perform quantum useful logical work balance  such as teleporting qubits teleportation . For many states, one can distill singlets in order to perform logical work, but there is also bound entanglement bound  which cannot be distilled from the state and it has been proposed that this is analogous to heat therm . Pure bipartite states can be reversible transformed into each other in a manner which is reminiscent of a Carnot cycle RP ; VP . Furthermore, the preparation of certain jointly held states appears to result in a greater loss of information when the state is prepared by two separated observers than when the entire state is prepared by a single party nlwe . Connections between Landauer erasure, measurement, error correction, and distillation have also been explored Vedral-eras .

In this paper we ask how much work can be drawn from a single heat bath if the information is distributed between two separated parties Alice and Bob. It turns out that in general their engines will be more efficient when information is localised, and that the degree to which this is the case provides a powerful new paradigm to understand and quantify non-locality in quantum mechanics.

As with the distant labs scenario for entanglement analysis, we allow Alice and Bob to perform local operations on their states, and communicate classically with each other (LOCC). We will quantify the amount of potential work that cannot be extracted by two separated parties by introducing the concept of a work deficit $`\mathrm{\Delta }`$, defined to be the difference in the amount of work that can be extracted from a state under LOCC versus the amount that can be extracted by a party who holds the entire state. For pure states we find that the work deficit is exactly equal to the amount of distillable entanglement $`E_D`$ of the state (i.e. the number of singlets that can be extracted from the state under LOCC). This also seems to be the case for so called maximally correlated states. We also prove bounds for $`\mathrm{\Delta }`$ and show that it is a good measure for the amount of quantum correlations present in a state jointly held by two parties. A more detailed analysis of the concepts introduced here will be presented elsewhere inprep .

Before proceeding with the quantum case it may be worthwhile to review the connections between information and thermodynamical work for classical states. Consider a number of classical bits $`n`$ which are all initially in the standard state 0. These bits can be used to draw work from a heat reservoir of temperature $`T`$. To visualize this, one might imagine that a bit is represented by a box divided by a wall in the center. A particle placed in the left hand side represents the $`0`$ state, while if the particle is in the right hand side, the bit is in the $`1`$ state.

Now imagine that we know that the bit is in the $`0`$ state. We can draw work from the heat reservoir by replacing the central wall with a piston and then allowing the particle to reversible push it out, drawing $`kT\mathrm{ln}2`$ of work from the reservoir kT . We now no longer know where the particle is, so the entropy of the bit has been increased by the same amount. No more work can be drawn from the bit, since we don’t know on which side to place the piston.

Although we cannot extract work from an unknown state, we can extract work if we know that classical correlations exist. Imagine for example that we have two classical bits in unknown states, but we know that they are in the same unknown state. We can then perform a control not (cnot) gate on the bits which flips the second bit if the first bit is a $`1`$. After the cnot gate has been performed the control bit is still in an unknown state, but the target bit is now in the $`0`$ state and one bit of work can be extracted from it. In general, for a n-bit random variable $`X`$ with Shannon entropy $`H(X)`$ one can use the first law of thermodynamics to see that the amount of work $`W_C`$ that can be extracted is just the change in entropy of the state

$$W_C=nH(X).$$
(2)
The same methods can be used to extract work from quantum bits (qubits)Peres . If we have n qubits in a state $`\rho `$ and entropy $`S(\rho )`$, then one can extract

$$W_t=nS(\rho ).$$
(3)
This is the amount of work that can be extracted in total by someone who has access to the entire system $`\rho `$. As with the classical case, all correlations can be exploited to extract work from the state.

We now ask how much work two individuals can extract under LOCC using a shared state $`\rho _{AB}`$. We imagine that Alice and Bob each have an engine which can be used to locally extract work from a common heat bath. Then, under LOCC they try to extract the largest amount of local work $`W_l`$ possible. We then define the work deficit to be the amount of potential work which cannot be extracted under LOCC

$$\mathrm{\Delta }W_tW_l.$$
(4)
Before proving some general results, it may be useful to give a few simple examples. Consider the classically correlated state

$$\rho _{AB}=\frac{1}{2}\left(|0000|+|1111|\right)$$
(5)
where the first bit is held by Alice, and the second by Bob. We can see that $`\mathrm{\Delta }`$ is zero for this case, since Alice can measure her bit, send the result to Bob who can then extract one bit of work by performing a cnot. Alice can then reset the memory of her measuring apparatus by using the work extracted from the bit that she held. The total amount of work extracted under LOCC is therefore $`1`$ bit, which from Eq. (3) is the same as the amount of work that can be extracted under all operations. In more detail, the steps involved in the process are: (a) Alice uses a measuring device represented by a qubit prepared in the standard state $`|0`$. She performs a cnot using her original state as the control qubit, and the measuring qubit as the target. (b) The measurement qubit is now in the same state as her original bit and can be dephased (i.e. decohered) in the $`|0,|1`$ basis so that the information is purely ”classical” (dephasing simply brings the off-diagonal elements of the density matrix to zero, destroying all quantum coherence). For this state, dephasing doesn’t change the state since the state is already classical. (c) The measuring qubit can now be sent to Bob who (d) performs a cnot using the measuring qubit as the control. His original qubit is now in the standard state $`|0`$. (e) Bob sends the measuring qubit back to Alice who (f) resets the measuring device by performing a cnot using her original bit as the control. Alice’s state is now in the same state as it was originally, while Bob’s state is known and can be used to extract $`1`$ bit of work.

We now consider how much work can be extracted from the maximally entangled qubits of Eq. (1). The same protocol as above can be used to find $`\mathrm{\Delta }=1`$ (later we will show that this is optimal). Alice and Bob can extract one bit of work by following steps (a)-(f). However, unlike the previous case, the measurement in step (b) is an irreversible process and the original state and the entanglement is destroyed by the dephasing that must occur for a measurement to be made. On the other hand, someone with access to the entire state can extract two bits of work since the state is pure and has zero entropy.

Basic questions now arise: How much work can be drawn from a given state $`\rho `$? For which states is $`\mathrm{\Delta }=0`$? How is $`\mathrm{\Delta }`$ related to entanglement?

To deal with these questions we have to state the paradigm for drawing work from bipartite states more precisely. First we will clarify the class of operations Alice and Bob are allowed to perform. The crucial point is that here, unlike in usual LOCC schemes, one must explicitely account for all entropy transferred to measuring devices or ancillas. So in defining the class of allowable operations one must ensure that no information loss is being hidden when operations are being carried out. One way to do this is to define elementary allowable operations as follows: (a) adding separable pure state ancillas to the system (b) local unitary operations (i.e. $`U_AI_B`$ or $`I_AU_B`$ ) (c) sending qubits through a dephasing channel.

The dephasing operation can be written as $`_iP_i\rho _{AB}P_i`$ where the $`P_i`$ are orthogonal local projection operators. The class of operations (c) are equivalent to local measurements and classical communication but has the advantage that we don’t need to worry about erasing the memory of measuring devices. Alice or Bob could also make measurements without sending the information, but in this scheme it is wasteful. Furthermore, it is equivalent to Alice sending qubits down the dephasing channel and having Bob send the qubits back. We therefore do not need to consider measurement and sending qubits as separate operations.

We imagine that Alice and Bob share an $`n`$ qubit state $`\rho _{AB}`$ composed of $`n_A`$ qubits held by Alice and $`n_B`$ by Bob. The part of the state which Alice holds is given by tracing out the degrees of freedom associated with Bob’s state i.e. $`\rho _A=Tr_B(\rho _{AB})`$ and visa-versa. Alice and Bob then perform combinations of operations (a)-(c) to arrive at a final state $`\rho _{AB}^{}`$ composed of $`n^{}=n_A^{}+n_B^{}`$ qubits. The difference $`k=n^{}n`$ is the number of pure state ancillas which they have added to the state, and therefore we must subtract $`k`$ bits of work from the amount of work they can draw using the $`n^{}`$ bits. Since they must extract the work from $`\rho _{AB}`$ locally, we find that the total amount of local work that can be extracted is

$`W_l`$ $`=`$ $`n_A^{}S(\rho _A^{})+n_B^{}S(\rho _B^{})k`$ (6)
$`=`$ $`nS(\rho _A^{})S(\rho _B^{}).`$
The goal is now clear. Alice and Bob perform their operations to arrive at a state which has $`S(\rho _A^{})+S(\rho _B^{})`$ as low as possible. They then draw work locally using this new state $`\rho _{AB}^{}`$.

Consider now the state of the form

$$\rho _{AB}=\underset{ij}{}p_{ij}|i_A|j_Bj_B|i_A|$$
(7)
where $`|i_A`$ and $`|j_B`$ are a local orthonormal basis. Such states can be called classically correlated odroz . The natural protocol is that Alice sends her part to Bob down the dephasing channel. This will not change the entropy of the state. The final state $`\rho ^{}`$ will have $`S(\rho _A^{})=0`$ (strictly speaking Alice will now have no system) while $`S(\rho _B^{})=S(\rho )`$. Thus according to Eq. (6) $`W_l=nS(\rho )=W_t`$, so that $`\mathrm{\Delta }=0`$ for the above states. Note that local dephasing in the eigenbases of $`\rho _A^{}`$, $`\rho _B^{}`$ does not change the optimal $`W_l`$ (6) but brings the state $`\rho _{AB}^{}`$ to the form (7). This gives another method to evaluate work: instead of minimizing $`S(\rho _A^{})+S(\rho _B^{})`$ we can minimize $`S(\rho ^{})`$ over classically correlated states $`\rho ^{}`$ that can be achieved from $`\rho `$ by the allowed class of operations. Now we are in position to prove a general upper bound on the amount of work that can be drawn using distributed information.

Our bound holds for pure statesinprep , but for more general states our proof relies on the following assumption, (although we conjecture that the bound holds in general).

Assumption: Bits which are sent down the communication channel are treated as classical in the sense that they are only dephased once, and not again in a second basis (which would destroy the encoded information).

Theorem: Under this assumption the maximum amount of work that can be extracted using LOCC operations on an $`n`$ qubit state $`\rho _{AB}`$ is bounded by $`W_lnmax\{S(\rho _A),S(\rho _B)\}`$.

The proof follows after noting that Alice (or Bob), rather than directly sending the results of measurements, can reversibly copy the measurement results by performing the cnot operation with the measurement bit as the control bit and an ancilla as the target. Alice can then send the copy to Bob who can use the information stored in the copy. At the end of the whole protocol all the copies can be sent back (this follows from our assumtion) and erased by performing a second reversible cnot. Alice and Bob’s protocol will therefore not be more inefficient if they keep their original measurement bits and only send copies to each other. Consider now any optimal protocol transforming $`\rho _{AB}`$ into the final state $`\rho _{AB}^{}`$ of the form (7) with minimal entropy $`S(\rho _{AB}^{})`$. As we already know the protocol can be followed by dephasing in the local eigenbases. Hence before sending copies back and erasing them, the entire system can be considered to be in another state $`\sigma _{AB}`$, still in the form (7), so Wehrl  $`S(\sigma _{AB})max\{S(\sigma _A),S(\sigma _B)\}`$. Now, as only copies of bit measurements were sent, and the bits themselves were kept, production of $`\sigma _{AB}`$ from $`\rho _{AB}`$ could only have increased local entropies because neither unitary operation nor dephasing decreases entropy. So one has

$$S(\sigma _{AB})max\{S(\rho _A),S(\rho _B)\}$$
(8)
where $`S(\rho _A)`$, $`S(\rho _B)`$ are local entropies of the initial state $`\rho _{AB}`$. Finally, because resending and erasing copies preserves the spectrum of the whole state, one has $`S(\sigma _{AB})=S(\rho _{AB}^{})`$ which gives

$$S(\rho _{AB}^{})max\{S(\rho _A),S(\rho _B)\}.$$
(9)
The theorem then follows directly from the fact that $`nS(\rho _{AB}^{})`$ is an upper bound on the amount of work that can be drawn from the state $`\rho _{AB}^{}`$. The corresponding work deficit obtained under our assumption will be denoted by $`\mathrm{\Delta }_r`$. For mixed states it is possible that $`\mathrm{\Delta }<\mathrm{\Delta }_r`$, but we conjecture equality. Also for one way LOCC schemes (classical communication from Alice to Bob only) $`\mathrm{\Delta }_r`$ coincides with the one way deficit $`\mathrm{\Delta }_{}`$. From the theorem we have lowerbound

$$\mathrm{\Delta }_r\mathrm{max}\{S(\rho _A),S(\rho _B)\}S(\rho )$$
(10)
This allows one to calculate the extractable work for pure states by exhibiting protocols that achieves this bound. To this end write a given pure state in the Schmidt decomposition $`\psi =_ia_i|e_i|f_i`$ where $`e_i,f_i`$ are local bases. Alice then performs dephasing in her basis. The resulting state is classically correlated and has entropy equal to $`S(\rho _A)`$ where $`\rho _A`$ is the reduction of $`|\psi \psi |`$. Note that the latter is the entanglement measure for pure states which is unique in the asymptotic regime and is equal to the distillable entanglement $`E_D`$ and the entanglement cost (i.e. the number of singlets which are required to create the state under LOCC) RP . Thus for pure states the work deficit is exactly equal to entanglement

$$\mathrm{\Delta }(\psi )=E(\psi ).$$
(11)
We are able to calculate $`\mathrm{\Delta }_r`$ for a broader class of states, the so called maximally correlated states of the form

$$\rho _{AB}=\underset{ij}{}\sigma _{ij}|iijj|.$$
(12)
To achieve bound (10) Alice dephases her part in the basis $`\{|i\}`$. The resulting state is $`\rho ^{}=_i\sigma _{ii}|iiii|`$, and has entropy equal to $`S(\rho _A)`$. Thus $`\mathrm{\Delta }_r(\rho )=S(\rho _A)S(\rho )`$. One can check that for states (12) local entropies are equal and no smaller than the total entropy so that $`\mathrm{\Delta }_r0`$ as it should be. Now it turns out that for the above states, we know $`E_D`$ Rains , and it is again equal to $`\mathrm{\Delta }_r`$. An example is the mixture of state (1) with $`1/\sqrt{2}(|00|11)`$: $`E_D=E_D^{}`$ (the latter being one way distillable entanglement) is equal to $`1S(\rho )`$. The explicit distillation protocol attaining this value was shown in huge . That one can not do better follows from the relative entropy bound VP ; Rains  which is equal to $`1S(\rho )`$ for those states.

The above result is rather surprising because the state (12) contains bound entanglement i.e. the entanglement cost of the state is greater than the entanglement of distillation Vidal-recent . This result shows that work can be drawn from the bound entanglement.

Although distillable entanglement cannot be used to perform physical work, it allows us to perform logical work (see balance ): each bit of distillable entanglement enables Alice to teleport one qubit to Bob. For these states, the total amount of extractable work $`W_t`$ gets divided between physical work $`W_l`$ and logical work $`E_D`$. Entanglement can therefore be thought of as a source of non-local negentropy which can be used to perform logical work. Just as with physical negentropy, logical negentropy can only decrease under LOCC ($`\delta E_D0`$). However, if one uses the state to extract physical work the ability to perform logical work is lost. Likewise, after performing logical work, the singlets are left in a maximally entropic state and the ability to perform physical work is lost. There is thus a new form of complementarity between the logical and physical work.

It is also worth investigating the connection between our approach and the measures of classical and quantum corelations introduced in VedralH  and Zurek-AnnPhys . It would also be desirable to consider collective actions on many copies of the given state. In the examples we considered, collective actions can’t help since the parameter $`\mathrm{\Delta }`$ turns out to be additive.

In conclusion, we have proposed a paradigm for quantifying quantum correlations motivated by thermodynamical and operational considerations. This approach is also fruitful in multipartite settings. The emerging function $`\mathrm{\Delta }`$ is nonzero for all entangled states, but need not vanish for separable states. It quantifies the part of correlations that must be destroyed during transmission via a classical channel (this is compatible with the observation that decoherence causes a Maxwell demon to be less efficient qdemon ). If a quantum channel was available, all information could be localized, and the full work $`nS(\rho )`$ could be drawn from local heat baths. Thus the work deficit $`\mathrm{\Delta }`$ quantifies truly quantum correlations. Finally, we hope that the present approach will prove fruitful in further investigations of quantum properties of compound systems, in particular that it may help discover a “new face” of the so called thermodynamics of entanglement.

This work is supported by EU grant EQUIP, Contract No. IST-1999-11053. J. O. thanks R. Laflamme and R. Cleve for interesting discussions, and NSERC and DITP for support.


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# Comments on ‘Stable Quantum Computation of Unstable Classical Chaos,’ ‘Efficient Quantum Computing Insensitive to Phase Errors,’ and ‘Quantum Computer Inverting Time Arrow for Macroscopic Systems’

Recently, a Letter GS1  published by Georgeot and Shepelyansky has been criticized zalka ; diosi . The Letter claims an exponential speedup and reduction in error sensitivity, when phase-space density evolution under the Arnold cat map is performed on a quantum computer (QC). On the one hand, some points have not yet been made in zalka ; diosi . On the other, the authors’ reaction GS3  raises new issues. The present note addresses both.

The first point concerns stability of the classical and quantum algorithms under their respective “natural errors.” By now, a consensus seems established that such comparison is fair only if both contestants operate on a discretized $`N\times N`$ map, say $`N=2^n`$. Then, the quantum errors considered are unitary gate noise (amplitude errors), plus phase errors either in those gates or during storage. Classical errors are taken to be one-cell shifts. The problem here is not a fine point of QC theory, but a misconstruction of *classical* binary numbers. In fact, errors in all bits of a register are equally likely, and digital technology is based on getting all of them right most of the time, so that integers are processed error-free. This is what enabled the simulations in GS1 . Thus, the classical algorithm has been deliberately handicapped.

Further, consider the evaluation of high harmonics of the evolved density, Fig. 1 in GS3 . Like Fig. 1 in GS1 , obtained on a *simulated* QC, it offers a glimpse of a real one’s wave function which nature does not allow one to see. Physically obtainable is a quantum measurement of the Fourier vector $`\stackrel{}{k}`$, yielding nontrivial information if the $`\stackrel{}{k}`$-density has strong peaks at high $`k`$. This is indeed the case for the cat map (GS3 , Fig. 1, bottom left and top right). Unfortunately, the latter’s evolution closes in $`\stackrel{}{k}`$-space GS3 , and can be handled classically without effort. In contrast, the data shown (middle/bottom right) for a nontrivial “perturbed cat map” only have a slanted band of density—in all likelihood a mere transient due to the low number of iterations $`t=5`$. The quantum approach now yields the gross features of this band. Fine structure, e.g. the small-amplitude low-$`k`$ peaks for the original map, is much easier obtained classically. Thus, the implicit claim (GS3 , bottom of col. 1) of being in the same situation as Shor’s algorithm (searching *one* period, verifiable a posteriori, of a spiked 1D $`k`$-space distribution) is valid only for a narrow set of questions, not substantiating the authors’ original scope.

Given the chronology, it is remarkable that Refs. zalka, ; diosi,  do not consider the follow-up GS2 . The latter, cited in the authors’ defence GS3 , boldly concludes that “the massive parallelism of QC is not necessarily related to quantum interference.” Again, one is shown figures of inaccessible wave functions, involving a phase-space coarse-graining of which no benefit or application is given except that it can apparently be performed quickly on a QC. It is worthwhile to read the “more detailed discussion of measurements” in version 2 of GS2 . The added penultimate paragraph, especially a casual remark in its last sentence, in fact refutes the whole paper and indeed its very title. An *in*coherent QC turns out to be an—expensive—classical one with random initial conditions, a basic point much in line with the remarks in diosi .

The discussion of GS4 , also cited in GS3 , can be brief: the only research added is an extension of the map’s $`y`$-axis, i.e., all the critiques zalka ; diosi  apply. Note that the QC derives its memory capacity from superposition. Thus, the evolution of an ensemble of orbits is necessarily *linear*, corresponding to chaotic one-particle dynamics rather than to a classical gas with collisions. Hence, calling the problem “macroscopic” is an exaggeration, and Boltzmann is better left out of it.

In conclusion, the authors continue an unreasonably positive appraisal of their QC algorithm vis-a-vis the classical one. In particular, Ref. GS2, , instead of supporting the authors’ case, is at fault in its basic premise and should be withdrawn.

I thank C.W.J. Beenakker, Yu.V. Gusev, P. Silvestrov, and A.M. Zagoskin for discussions.