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# Order-Parameter Fluctuations in Ising Spin Glasses at Low Temperatures

## I Introduction

Understanding the low-temperature physics of short-range spin glasses books  remains a major unsolved problem. Much of the current debate concentrates on the equilibrium thermodynamics of the Edwards-Anderson model with Ising spins (EAI model), the canonical short-range spin glass. Since analytical approaches pose formidable difficulties, the problem is often studied numerically. However, the existence of large barriers between low-energy configurations has limited so far numerical calculations to small systems sizes, from which it is hard to draw definite conclusions on the large-volume limit.

Two main issues have been addressed in many numerical studies: the existence and character of the finite-temperature spin-glass transition, and the nature of the low-temperature spin-glass phase. A central quantity of interest in the description of the spin-glass phase is the scaling exponent $`\theta ^{}`$ governing the typical energy of the lowest-lying excitations with linear size of order $`l`$, which is assumed to scale as $`El^\theta ^{}`$. In general, $`\theta ^{}`$ may be distinct KM00 ; PY00  from the stiffness exponent $`\theta `$ measured in domain-wall computations DW ; HARTMANN ; HARTMANN4D ; PY99 , and the stability of the spin-glass phase requires to have $`\theta ^{}0`$. In a “many-state” picture foot\_states  such as the replica-symmetry-breaking picture inspired by mean-field theory parisi ; books ; MPRRZ , one has $`\theta ^{}=0`$, hence there are excitations whose energy remains finite (of the order of the coupling strength between two spins) even as their length scale diverges. In a “two-state” picture, such as the droplet model fh ; bm , one has $`\theta ^{}>0`$, hence the energy of large-scale excitations diverges with their size. In this case the identity $`\theta ^{}=\theta `$ is often assumed.

Both the spin-glass transition and the ordered phase have been usually investigated numerically by computing sample-averaged quantities such as the Binder cumulant binder  or the distribution of the order parameter (OP) and related observables. Recently MNPPRZ ; PPRi , it was observed that useful information on both issues can be drawn from the sample-to-sample fluctuations of the OP. In particular, two dimensionless measures of the OP fluctuations were considered MNPPRZ ; PPRi : $`A`$, the normalized fluctuation of the spin-glass susceptibility, and $`G`$, a ratio between two cumulants of the OP distribution. These two parameters are related to the Binder cumulant, $`B`$, via the relation $`B=1A/(2G)`$. For a model without time-reversal symmetry (TRS), $`A,G`$, and $`B`$ are given by Eqs. (2), (3), and (4) below. The parameter $`G`$ serves as a good indicator of the existence of phase transitions PPRi  in systems lacking TRS (for which $`B`$ is generally a bad indicator), as recently shown for several systems, including Migdal-Kadanoff spin glasses COMREP , RNA folding models PPRICCI , chiral spin systems HK , and mean-field models such as the SK model (with and without a magnetic field), the infinite-range $`p`$-spin model PRS , and the infinite-range Potts model POTTS . The parameter $`A`$ has also been studied before for random diluted models at criticality WD96 ; AH .

In this paper, we investigate the OP fluctuations in the EAI model with Gaussian couplings in three and four dimensions by low-temperature Monte Carlo simulations. We study the case with no external field, which satisfies TRS. In three dimensions (3D), numerical data are available in the literature for $`A`$ in the high-temperature phase MPR94  and for $`G`$ near the critical point BCF , for the “$`\pm J`$” coupling distribution. In four dimensions (4D), $`G`$ was measured at moderately low temperatures, also for the $`\pm J`$ distribution MNPPRZ . Here, we study much lower temperatures than in these studies, in order to reduce crossover effects associated to the critical point BDM ; KPY , which complicate the interpretation of the numerical data at higher temperatures.

A summary of our results is as follows. First, we estimate $`\theta ^{}`$ from the system-size dependence of $`A`$, finding, for the system sizes we could reach, a small value of $`\theta ^{}`$ incompatible with the accepted values of the domain-wall exponent ($`\theta 0.2`$ in 3D DW ; HARTMANN ; PY99  and $`\theta 0.7`$ in 4D HARTMANN4D ), and compatible with zero. This agrees with recent determinations of $`\theta ^{}`$ from ground-state perturbation methods KM00 ; PY00 ; MP01  and from low-temperature measurements of the OP distribution KPY ; RB90 ; MZ ; MPRRZ  (which all consider sample-averaged quantities), and supports a picture of the spin-glass phase characterized by two distinct exponents, $`\theta >0`$ and $`\theta ^{}=0`$. The result $`\theta ^{}=0`$ implies that the OP is not self-averaging in the thermodynamic limit.

Second, we find good evidence that the identity $`G=1/3`$ holds in the whole spin-glass phase in the thermodynamic limit, confirming the validity of sum rules proposed by Guerra GUERRA1  and first derived for the SK model, which follow from the property of “replica equivalence” BMY ; MPSV .

Third, we find that $`A`$ and $`G`$ allow to locate the spin-glass transition reasonably well although, as expected due to TRS and as previously numerically observed BCF , $`B`$ provides a better determination (a much more accurate determination is provided by the correlation length BCF , which we do not investigate here).

We do not study in this paper the surface fractal dimension $`d_s`$ of the excitations, which is the other exponent, besides $`\theta ^{}`$, characterizing the spin-glass phase (in particular, $`d_s=0`$ in the standard replica-symmetry-breaking picture MPRRZ , $`d_s>0`$ in the droplet model, while the “TNT” picture KM00 ; PY00  predicts the “mixed” behavior $`d_s>0`$, $`\theta ^{}=0`$).

The rest of the paper is organized as follows. In Sec. II we introduce the different models and observables studied, and discuss the theoretical predictions for these observables. In Sec. III we present and analyze our numerical results for the quantities $`A`$, $`G`$ and $`B`$. Finally, in Sec. IV we summarize our conclusions.

## II Models, observables, and theoretical predictions

We study the EAI model defined by the Hamiltonian

$$=\underset{i,j}{}J_{ij}S_iS_j,S_i=\pm 1,$$
(1)
where $`L^D`$ Ising spins $`S_i`$ sit on a (hyper-)cubic lattice in $`D`$ dimensions with linear size $`L`$ and periodic boundary conditions in all directions. The couplings $`J_{ij}`$ are drawn from a Gaussian distribution of zero mean and unit variance. We consider two different models: (i) the case with interactions $`i,j`$ restricted to nearest neighbors (referred to as NN model) in $`D=3`$ and $`4`$; (ii) the case with interactions restricted to nearest, next-nearest, and next-next-nearest neighbors (referred to as NNN model) in $`D=3`$, which has a coordination number $`z=26`$.

The NN model has been extensively studied and is known to display a finite-temperature continuous spin-glass transition for $`D3`$. Recent estimates of the critical temperature for Gaussian-distributed couplings are $`T_c=0.95\pm 0.04`$ in 3D MPR  and $`T_c=1.80\pm 0.03`$ in 4D PRR96 .

The NNN model has been much less studied. In Ref. MPR94, , the 3D case with $`\pm J`$ couplings was considered, but no conclusive evidence of a finite-temperature transition was obtained, the data being compatible with both $`T_c3.27`$ and a zero-temperature singularity. Incidentally, in the NNN case we do not expect a large difference in $`T_c`$ between binary and Gaussian distributions, due to the large coordination number. For the NNN model, we did not consider temperatures as low as for the NN model, but focused on the phase transition region. Another of the results of this paper is a convincing evidence that indeed a finite-temperature transition exists in this model in 3D.

We measure $`A`$, $`G`$, and $`B`$ as a function of temperature $`T`$ and size $`L`$ using the following definitions:

$`A(T,L)`$ $`=`$ $`{\displaystyle \frac{\overline{q^2^2}\overline{q^2}^2}{\overline{q^2}^2}}`$ (2)
$`G(T,L)`$ $`=`$ $`{\displaystyle \frac{\overline{q^2^2}\overline{q^2}^2}{\overline{q^4}\overline{q^2}^2}}`$ (3)
$`B(T,L)`$ $`=`$ $`{\displaystyle \frac{1}{2}}\left(3{\displaystyle \frac{\overline{q^4}}{\overline{q^2}^2}}\right)`$ (4)
where $`q=\frac{1}{L^D}_iS_i^aS_i^b`$ is the spin overlap of two independent systems $`S_i^a`$ and $`S_i^b`$ with the same random couplings, and $`\mathrm{}`$ and $`\overline{(\mathrm{})}`$ stand for thermal and disorder averages, respectively. The OP for a given realization of the disorder is $`q^2`$, therefore $`A`$ is nothing but the normalized sample-to-sample variance of the OP.

In the paramagnetic phase, $`T>T_c`$, and for sufficiently large $`L`$ so that $`L\xi `$ (where $`\xi `$ is the correlation length), the OP follows a Gaussian distribution and all three parameters vanish as $`1/L^D`$, as follows from the central limit theorem. Following the terminology of Wiseman and Domany WD96 , this means that the OP is strongly self-averaging.

At $`T=T_c`$, the correlation length diverges and the central limit theorem cannot be applied. For strongly disordered systems such as spin glasses it is known that the OP is not self-averaging at criticality WD96 ; AH , namely $`A`$ tends to a finite value in the thermodynamic limit. If $`A`$ is finite then clearly $`G`$ must be finite, and standard renormalization-group arguments show that $`B`$ is also finite at $`T_c`$. Since $`B`$ and $`G`$ are dimensionless and monotonic in $`T`$, in plots of these quantities as a function of $`T`$, the curves for different values of $`L`$ must all cross at $`T=T_c`$, and one can use this to determine $`T_c`$. From standard finite-size scaling, one can then determine the critical exponent $`\nu `$. Since much work has been devoted to measuring $`\nu `$ from the standard observables (see for instance Refs. YOUNG, ; BCF, ; PC, ; ky, ; MPR, ), and we are primarily interested in the low-temperature phase here, we will not attempt a precise determination.

In the spin-glass phase, $`T<T_c`$, $`A`$ is expected RSb ; DBM  to vanish linearly with $`T`$ according to the scaling law

$$A(T,L)TL^\theta ^{},$$
(5)
where $`\theta ^{}`$ is the exponent discussed in the Introduction. This law holds under two hypothesis (both satisfied in the case of continuous couplings studied here): (i) the ground state is unique; (ii) the probability distribution of the energy of the lowest-lying excitations has finite weight at zero energy RSb ; DBM .

From the above scaling law we see that if $`\theta ^{}>0`$, then $`A`$ vanishes for $`L\mathrm{}`$, namely the OP is weakly self-averaging (where “weakly” indicates WD96  that the OP fluctuations vanish more slowly than $`1/L^d`$, a consequence of the inequality $`\theta ^{}<d`$). This situation is encountered in the droplet model fh ; bm , as discussed in the Introduction, and also in mean-field models with a marginally stable replica-symmetric solution at low temperatures (such as the spherical SK model RS ). If $`\theta ^{}=0`$, as in a “many-state” picture, $`A`$ remains finite in the thermodynamic limit, namely the OP is not self-averaging.

Turning now to $`G`$, it is known BMY ; MPSV  that in the SK model the following relation holds for $`T<T_c`$:

$$\underset{L\mathrm{}}{lim}G(T,L)=1/3.$$
(6)
According to Guerra GUERRA1 , this relation should hold (for $`T<T_c`$) in any model which is “stochastically stable” with respect to a mean-field perturbation and which has a non-self-averaging OP. Under the hypothesis (i) and (ii) above, the more general conjecture has also been made RS  that the above relation holds for $`T<T_c`$ even if the OP is self-averaging. In this case, $`G`$ would be finite but both the numerator and the denominator in Eq.(3) would vanish, as for example in the Migdal-Kadanoff spin glass (see Bokil et al. in Ref. COMREP, ) and the SK spherical model RS . It has also been explicitly proven RSb , under the hypothesis (i) and (ii), that one has $`G(T=0,L)=1/3`$ for any $`L`$. Note that models in which $`G(T=0,L)1/3`$ in general will not satisfy the conjecture of Ref. RS, .

## III Numerical results

We simulated the various models with the parallel tempering technique HN , which allows to reach significantly lower temperatures than conventional Monte Carlo methods. The parameters of the simulation are given in Table 1. Equilibration of the Monte Carlo runs was tested by monitoring all the measured observables on a logarithmic time scale, checking that they had all converged within their statistical errors, and by applying the equilibration test discussed in Ref. KPY, .

### III.1 Parameter $`A`$

In Figures 1, 2, and 3 we show our numerical results for $`A`$ in the 3D NN, 4D NN, and 3D NNN models, respectively. The vertical lines in Figures 1 and 2 indicate the estimated value of $`T_c`$. In all cases, the behavior of $`A`$ resembles that observed in the SK model (see Refs. MNPPRZ, ; HK, ; PRS, ). At high temperatures, $`A`$ decreases with $`L`$, approximately as $`1/L^D`$, showing that the OP is strongly self-averaging in this regime, as expected. Near $`T=T_c`$, there is a maximum whose position shifts towards $`T_c`$ as $`L`$ increases, an effect of finite-size corrections. The shift is modest in the 4D NN model but quite noticeable in the 3D NN model, where even for the largest $`L`$ the position of the maximum is still significantly larger than $`T_c`$. In the 3D NNN model, the position of the maximum is also larger than $`T_c`$ (see discussion in Sec. III.3 on the value of $`T_c`$ in this model), but the shift is less pronounced. The height of the maximum increases with $`L`$ in all models, indicating that $`A`$ attains a finite value in the thermodynamic limit (since it is bounded from above), namely that the OP is not self-averaging at $`T_c`$, as expected.

At low temperatures ($`T<T_c`$), Figures 1, 2, and 3 show that $`A`$ is approximately linear in $`T`$, in agreement with Eq. (5). Most interestingly, the data for different values of $`L`$ tend to superimpose to each other. In a scenario with $`\theta ^{}>0`$, the data should tend to zero for large $`L`$ in the whole region below $`T_c`$. In 3D, we see no decrease at all in the data with increasing $`L`$, while a modest decrease is observed in 4D.

To analyze in more detail the size dependence of $`A`$ at low temperatures, in Figure 4 we plot the ratio $`A/T`$ as function of $`L`$ at different temperatures for the three models. The straight lines represent the scaling law Eq.(5) assuming $`\theta ^{}=\theta `$, and using the estimates of $`\theta `$ from domain-wall calculations, $`\theta =0.2`$ in 3D DW ; HARTMANN ; PY99  and $`\theta =0.7`$ in 4D HARTMANN4D . No estimates of $`\theta `$ are available for the 3D NNN model, so we use that for the NN model (we expect that $`\theta `$ is a universal exponent equal for both models). Clearly, the data in Figure 4 do not agree with the hypothesis $`\theta ^{}=\theta `$ for the range of sizes considered, and seem to saturate to a constant value instead. We fitted the data with the form $`A(T,L)/T=aL^{\widehat{\theta }^{}}`$, where $`\widehat{\theta }^{}`$ should be seen as an “effective” exponent which depends on the temperature and which effectively takes into account corrections to the leading scaling behavior, with $`\widehat{\theta ^{}}\theta ^{}`$ in the limit $`TL^\theta ^{}0`$. The fits give $`\widehat{\theta ^{}}`$ varying from $`0.03\pm 0.02`$ ($`T=0.7`$) to $`0.00\pm 0.06`$ ($`T=0.2`$) in the 3D NN model, from $`0.30\pm 0.05`$ ($`T=1.0`$) to $`0.003\pm 0.006`$ ($`T=0.32`$) in the 4D NN model, and from $`0.03\pm 0.04`$ ($`T=2.8`$) to $`0.08\pm 0.04`$ ($`T=2.0`$) in the 3D NNN model.

Therefore, in all cases the data is compatible with $`\theta ^{}=0`$, in agreement with the “many-state” picture, and is statistically incompatible with with $`\theta ^{}=\theta `$, in disagreement with the “two-state” picture. As usual, we cannot exclude a crossover BDM  to a larger value of $`\theta ^{}`$ for larger $`L`$. In this case, in the large-volume limit $`A`$ would be zero at all temperatures, except at $`T=T_c`$.

A value of $`\theta ^{}`$ compatible with zero was also obtained from the OP distribution KPY ; RB90 ; MZ ; YOUNG ; MPRRZ  and from direct measurements of the energy of low-lying excitations created by perturbing the ground state KM00 ; PY00 ; MP01 .

### III.2 Parameters $`G`$ and $`B`$

Figures 5, 6 and 7 show our numerical results for $`G`$ and $`B`$ for the three models. At high temperatures, $`G`$ and $`B`$ vanish approximately as $`1/L^D`$ in all three models, again indicating strong self-averaging. Near $`T=0`$, the data for the NN model in both 3D and 4D are compatible with $`G(T=0,L)=1/3`$ and $`B(T=0,L)=1`$, as expected RS ; RSb  for a continuous coupling distribution. More importantly, $`G(T,L)`$ seems to converge to the value 1/3 for large $`L`$ in the whole low-temperature region, in agreement with Eq.(6). This is particularly evident in the 4D NN model (Figure 6), where $`G(T,L)`$ has already converged to 1/3 for $`L=5`$ at temperatures below $`TT_c/20.9`$ (the data points above $`1/3`$ are due to incomplete equilibration PRS ). It is quite unlikely that the saturation is a finite-size effect, therefore our results strongly suggest that indeed $`G=1/3`$ in the whole spin-glass phase. As discussed above, if $`A`$ remains finite as $`L\mathrm{}`$ (as indicated by our data), this is an expected consequence of stochastic stability GUERRA1 . If $`A`$ vanishes, instead, our results would support the more general conjecture of Ref. RS, .

### III.3 Critical region

In this subsection we comment on the behavior of $`G`$ and $`B`$ near the critical temperature, starting from the NN model.

In 3D, the vertical lines in Figure 5 indicates the position of the critical temperature, using the value $`T_c=0.95\pm 0.04`$ quoted in Ref. MPR, , which was obtained from the parameter $`B`$ measured in a large-scale simulation. One sees that the data for both $`B`$ and $`G`$ for different values of $`L`$ come together as $`T`$ approaches $`T_c`$ from above, as indicative of a phase transition. Below $`T_c`$, the data for $`G`$ separate again in a statistically significant way, while for $`B`$ one would need a substantially larger statistics (or larger sizes) to see a clear separation, as observed in previous studies MPR ; ky . For example, at $`T=0.82`$ the separation between the $`L=12`$ and the $`L=4`$ data is 1.4 standard deviations for $`B`$ and 2.5 standard deviations for $`G`$. The small separation below $`T_c`$ is probably due to the vicinity of $`D=3`$ to the lower critical dimension MPR ; ky ; PC . We also note that the crossing point of $`G`$ is at temperatures larger than $`T_c`$, and close inspection shows that it shifts towards $`T_c`$ from above as $`L`$ increases. A similar shift was observed for the position of the maximum of $`A`$ in Figure 1.

In 4D, both $`B`$ and $`G`$ display a very clear crossing (see Figure 6), as also observed in previous studies PRR96 ; MZ . From $`B`$ we estimate $`T_c=1.80\pm 0.03`$ in agreement with the results of Refs. BY, ; PRR96, . This value is indicated by the vertical lines in Figure 6. As in 3D, the crossing point of $`G`$ is at temperatures larger than $`T_c`$ and shifts towards $`T_c`$ as $`L`$ increases.

Overall, this confirms that both in 3D and 4D the corrections to scaling are significantly larger for $`G`$ and $`A`$ than for $`B`$. Since $`G`$ and $`A`$ have also much larger statistical errors than $`B`$, the latter quantity is to be preferred to $`G`$ and $`A`$ for locating $`T_c`$ in models with TRS. As already mentioned, a much more accurate quantity for this purpose is the correlation length, which shows a very clear crossing in 3DBCF , unlike $`B`$ and $`G`$.

Finally, in the 3D NNN model both $`G`$ and $`B`$ show a rather clear crossing (see Figure 7). This provides a clear evidence for the existence of a phase transition in 3D Ising spin glasses, confirming recent results for the NN model ky ; PC ; BCF  that obtained a convincing evidence (especially Ref.BCF, ) after the issue had remained unsolved for a long time. The crossing point is at $`T3.3`$ for $`B`$ and at somewhat higher temperatures for $`G`$, although also here the crossing for $`G`$ shifts to the left as $`L`$ increases. From the data for $`B`$ one might be tempted to conclude that the critical temperature is $`T_c3.3`$. However, if this was the case, the value of $`B`$ at $`T_c`$ (which is a universal quantity) would be lower in the 3D NNN model than in the 3D NN model, violating universality. This suggests that the actual value of $`T_c`$ is significantly lower than 3.3, despite the clear crossing of $`B`$ (which would then be strongly affected by scaling corrections), and for this reason we have not indicated the position of $`T_c`$ in Figures 3 and 7. A more detailed analysis matteo\_preparation  clearly shows that indeed $`T_c`$ is significantly lower than 3.3 in this model.

## IV Conclusions

To conclude, we have provided evidence that the order parameter is not self-averaging in the low-temperature phase of the Edwards-Anderson Ising spin glass in 3D and 4D, which implies an exponent $`\theta ^{}0`$, in agreement with a “many-state” picture of the spin-glass phase, such as the replica-symmetry-breaking picture or the “TNT” picture. As usual, due to the limited system sizes that are currently reachable in numerical simulations, we cannot exclude that for larger sizes one recovers self-averaging, nevertheless our result is consistent with other studies which used sample-averaged quantities KPY ; KM00 ; PY00 ; MP01  and also found $`\theta ^{}0`$. Independently of whether there is self-averaging or not, we have provided evidence that the identity $`G=1/3`$ holds in the thermodynamic limit in the whole spin-glass phase, a fact that calls for a theoretical explanation in terms of the geometry and energetics of the low-lying excitations. We have confirmed that $`G`$ and $`A`$ can be used to locate the spin-glass transition, although in models with time-reversal symmetry the usual sample-averaged parameters provide a better determination. Finally,we have confirmed the existence of a spin-glass phase transition at finite temperature in three dimensions.

###### Acknowledgements.

We acknowledge support from Spanish Ministerio de Ciencia y Tecnología, Grants BFM2001-3525 (F.R.), AP98-36523875 (M.S.), Generalitat de Catalunya (F.R.). M.P. acknowledges support from the European Commission, contract HPRN-CT-2002-00319 (STIPCO).


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# Components of Antineutrino Emission in Nuclear Reactor

## Introduction

It has many times been underlined (see e.g. recent reviews ) that it is important to have an exact knowledge of the reactor antineutrino ($`\overline{\nu }_e`$) energy spectrum for planning and for analyzing the experiments on neutrino intrinsic properties and on searches for New Physics at reactors.

In widely used Pressurized Water Reactors (PWR, VVER in Russian abbreviation) summed U and Pu isotope fission rate is $`3.1\times 10^{19}`$/s per 1 GW thermal power. About $`N_\nu 6.7`$ $`\overline{\nu }_e`$ are emitted per one fission event. 75% of them belong to the energy range E $`<`$ 1.80 MeV, below the threshold of the inverse beta decay reaction on proton. Quantity $`N_\nu `$ receives contribution from six sources:

$$N_\nu =^FN+^UN+\delta ^FN$$
(1)
Here $`{}_{}{}^{F}N5.5\overline{\nu }_e`$/fission represents summed contribution from beta decays of fission fragments of four fissile isotopes 235U, 239Pu, 238U and 241Pu, undistorted by their interaction with reactor neutrons, $`{}_{}{}^{U}N1.2\overline{\nu }_e`$/fission comes from beta decay of 239U $`^{239}`$Np $`^{239}`$Pu chain produced via neutron radiative capture in 238U and $`\delta ^FN<0.03\overline{\nu }_e`$/fission originate from neutron capture in accumulated fission fragments and give small but not negligible local distortions of the total energy spectrum of the reactor $`\overline{\nu }_e`$.

Plan of this report is as follows:

First, we present a short (and incomplete) overview of a half a century long history, which has led to the present understanding of the reactor antineutrinos.

Second, we give new results on the computed evolution of $`\overline{\nu }_e`$ energy spectra corresponding to four fissile isotopes vs fuel irradiation time and their decay after the end of the irradiation; we compare all available data and estimate relevant uncertainties.

After these data are presented on antineutrinos due to neutron radiative capture in 238U and in accumulated fission fragments.

Finally we consider small corrections to the ILL spectra.

## 1 Short history

Alvarez (unpublished report, 1949 y) did historically the first estimation of the reactor $`\overline{\nu }_e`$ spectrum using conception of fission radiation developed by K. Way and E. Wigner . The next were Perkins and King in 1958 y . These studies were stimulated by B. Pontecorvo’s proposal to look for Cl $``$ Ar transitions near atomic reactor (1946 y) and by famous F. Reines $``$ C. Cowan experiments. At that time and many years after it was assumed that the only source of reactor antineutrinos is the decay of 235U fission fragments.

Kurchatov Institute’s Rovno group in 1974-77 yy noticed that in nuclear reactors fission of other heavy isotopes produces flux of comparable to that of 235U and their energy spectra can be quite different from that of 235U, which, among other effects, would cause time variation of the neutrino induced reaction cross sections (burn up effect) . Calculated energy spectrum for $`\overline{\nu }_e`$ emitted by 239Pu fission fragments was first published in  and for each of four fissile isotopes was given in . F. Avignone III et al. in 1980 y were the first to publish results on 238U . B. Davis, P. Vogel et al. in 1979 y  also calculated spectrum for 239Pu and P. Vogel, G. Schenter et al. published results for four fissile isotopes in 1981 y . In these publications mainly ”high” energy parts ($`E>11.5`$ MeV) of the antineutrino spectra were presented.

Quoted calculations done in 1976-1981 years \[6-10\] have confirmed the idea that $`\overline{\nu }_e`$ spectra associated with fission of different isotopes considerably differ one from another. Thus, relative to $`\overline{\nu }_e`$ spectrum generated in the decay of 235U fission fragments, fission of 238U gives much harder spectrum while 239Pu fission produces $`\overline{\nu }_e`$ of lower energies. The absolute values of each of the four spectra was established, however, with large uncertainties associated with poor knowledge of the decay schemes of short lived fission fragments, which significantly contribute to the hard part of the $`\overline{\nu }_e`$ spectra.

Accurate knowledge of the $`\overline{\nu }_e`$ spectra came from experiments in which relevant beta-electron spectra were measured. Electrons and $`\overline{\nu }_e`$ come from the same beta decay process and are closely related. This simple idea is used in the conversion method in which $`\overline{\nu }_e`$ spectrum can be reconstructed (at least for not too low energies) if the spectrum of fission electrons is known. This idea was first proposed and used for 235U by C. Muehlhause and S. Oleksa in 1957  and by F. Reines group in 1959 y . Later the correlation between calculated electron and $`\overline{\nu }_e`$ fission spectra was analyzed in 1979-1981 yy in already quoted papers , by K. Schreckenbach et al.  in 1981 y and by the Rovno group in 1982 y . First experiment in which 235U and 239Pu fission electron spectra have been measured and their considerable difference observed was performed by Rovno group in 1980-1981 yy . The best $`\overline{\nu }_e`$ spectra for 235U, 239Pu and 241Pu thermal fission at the neutrino energies $`E2.0`$ MeV have been found by the ILL group in a number of experiments carried out in 1981-1989 yy ; they accurately measured relevant electron spectra and effectively modified the conversion procedure. These ILL spectra above 2 MeV are commonly used now. For 238U is used spectrum calculated in .

Voloshin, Vysotskii and L. Okun’ , Akhmedov , Vogel and Engel  in 1986-1989 yy stimulated new efforts to search for anomalous magnetic moment of the neutrino in $`\overline{\nu }_e,e`$ scattering experiments at reactors and further studies of the components of reactor $`\overline{\nu }_e`$ spectrum. The Moscow MEPhI group in 1989 y calculated time-evolution of $`\overline{\nu }_e`$ spectra emitted by U and Pu fission fragments .

The fifth component of the spectrum $`{}_{}{}^{U}N`$, which originates from 238U(n,$`\gamma `$) reaction, was ”discovered” only in 1996 y . The last component $`\delta ^FN`$, which comes from reactor neutron capture in fission fragments was estimated in  and considered in .

## 2 Main results

### 2.1 Fission antineutrinos from four fissile isotopes

For each of four fissile isotope we calculate the time evolution of the $`\overline{\nu }_e`$ spectrum during fuel irradiation time $`t_{on}`$ and its decay as a function of time $`t_{off}`$ after the end of irradiation. Calculations involve summation of all beta branches of 571 fission fragments. For fragments yields we use data compiled in . For the decay schemes is used information accumulated in our laboratory during past 25 years. Our code evaluates the spectra in the energy range 0-10 MeV (200 points per 1 MeV) for $`t_{on}`$ and $`t_{off}`$ intervals from 0.2 hour to infinity.

Time evolution of the four spectra for $`\overline{\nu }_e`$ energy below 3.5 MeV is presented in Tables 1 and 2. One can see that at 3.5 MeV full saturation is achieved already in $``$1 day time after the beginning of fission process, in 2-3 MeV energy range $``$ 3% increase takes place at long irradiation times while low energies do not reach equilibrium even in 2 years. (In typical PWR reactors 2 year is the average fuel irradiation time at the end of the operational run). In Table 3 one can see that at $`t_{on}`$ = 2 y 50% of fission $`\overline{\nu }_e`$’s are emitted below (1.2-1.3) MeV and $``$ 30% of them have energy higher than 2.0 MeV.

Fuel continues to emit $`\overline{\nu }_e`$ after the irradiation is stopped (Table 4). In the softest part of the spectrum (50-500 keV) the residual $`\overline{\nu }_e`$ emission rate is at a level of $``$50-5% during the first month and does not completely vanish at $`t_{off}`$ = 1 year.

To what extend are reliable calculated $`\overline{\nu }_e`$ spectra in the energy range E $`<`$ 3 MeV? Here, in contrast with the E $`>`$ 3 MeV region, contribution of well-established beta emitters amounts to 85-90%. We estimate that relative uncertainties here do not exceed 5-6% (68% C.L.). This estimate is confirmed by comparison of present results with spectra calculated earlier by Vogel and Engel , by MEPhI group  and with the ILL conversion spectra  (Fig.1).

### 2.2 Antineutrinos from neutron capture in 238U and in fission fragments

Nuclear fuel in PWR reactors contains 95-97% of 238U. 238U absorbs $``$0.6 neutron per fission via (n,$`\gamma `$) reaction: 238U + $`n`$ 239U($`E_{max}`$ = 1.26 MeV) $``$ 239Np($`E_{max}`$ = 0.71 MeV) $``$ 239Pu. This process contributes $`{}_{}{}^{U}N`$ 20% to the total flux. The quantity $`{}_{}{}^{U}N`$ is practically constant over reactor run and is known with an uncertainty of 5%. Note, that in reactors with fuel elements of natural uranium $`\overline{\nu }_e`$ production rate in the channel considered is $``$1.5 times higher.

Neutron capture in fission fragments can either increase or decrease intensity depending on energy of $`\overline{\nu }_e`$ (Fig. 2). The term $`\delta ^FN`$ (Eq.1) is negative for energies below 0.9 MeV and positive for higher energies; it slowly changes along the reactor run and its contribution to the total flux of $`\overline{\nu }_e`$ does not exceed 0.3%. The negative part of $`\delta ^FN`$ originates mainly from intensive absorption of neutrons in the fragment 135Xe ($`T_{1/2}`$ = 9.1 h, $`E_{max}`$ = 0.91 MeV), which is produced in reactor at a rate of $``$0.07/fission. Due to very high cross section of (n,$`\gamma `$) reaction (a few million barn) the majority of 135Xe nuclei absorb neutrons before they decay.

Neutron interactions with reactor construction materials have been found to contribute less than 0.3% to the total flux and have been neglected at this stage of study.

### 2.3 Small corrections to the ILL spectra

The ILL spectra have been obtained after 1-1.5 day exposure time. Their uncertainties are estimated as 2.5%. These spectra do not contain time dependent contributions due to decay of long-lived fission fragments (see Tables 1, 2) and due to additional radiation associated with neutron capture (Fig. 2), which affect part of the $`\overline{\nu }_e`$ spectra above 1.80 MeV, the threshold of the inverse beta decay reaction on proton. We mention here this point because it may appear to be of some importance in searches of very small mixing angle oscillations at reactors, which have been discussed at this Conference.

## Conclusions

In this report we have tried to give a short story of the long process of developments in understanding reactor antineutrino source and to outline present status of the problem. New efforts to improve the accuracy may be needed in the future. So far, however, we do not feel challenges coming from current or planned experiment, which could stimulate such efforts.

## Aknowledgements

This work is partially funded by grants 1246.2003.2 (Support of leading scientific schools) and 03-02-16055 (RFBR).

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text:
# Infrared optical properties of the spin-1/2 quantum magnet 𝑇𝑖𝑂𝐶𝑙

## I Introduction

Low-dimensional quantum spin systems, based on complex transition metal oxides, recently attracted a lot of attention, particularly as a fascinating playground to study spin-charge separation, spin-gap states and quantum disorder. Proposals, that the exotic properties of low-dimensional spin-1/2 quantum magnets might also play a major role in shaping the mechanism for high temperature superconductivity, led to a vigorous experimental activity on materials involving $`Cu^{2+}`$ ions with a 3d9 configuration (S=1/2). Other examples of S=1/2 are notably $`Ti^{3+}`$ and $`V^{4+}`$ systems in d1 configuration (i.e., one single d-electron occupies one of the t2g orbitals). In this respect, the layered $`TiOX`$ ($`X=Cl`$ and $`Br`$) compounds are most promising and are candidates for exotic electronic configurations as in the resonating-valence-bond (RVB) model beynon  and for superconductivity based on dimer fluctuations seidel2 ; seidel .

$`TiOCl`$ has been first considered as a two-dimensional antiferromagnet, an electron analog to the high-temperature cuprates. This was based on considerations about the electronic properties and on the bi-layer structure of the compound formed by edge-sharing, distorted $`TiO_4Cl_2`$ octahedra seidel . High quality single crystals of $`TiOCl`$ display a kink in the spin susceptibility $`\chi (T)`$ below about $`T_{c2}`$=94 $`K`$, followed by a pronounced drop at $`T_{c1}`$=67 $`K`$. This leads to a non-magnetic ground state at $`T_{c1}`$, therefore signaling the opening of a singlet-triplet spin-gap seidel ; imai . It has been proposed that the effective dimensionality of the $`TiO`$ layers is reduced from two to one by an orbital ordering at $`Ti^{3+}`$ sites and that the singlet ground state is reached by a phase transition also involving lattice degrees of freedom. Consequently, the spin gap formation and the associated fluctuations in $`TiOCl`$ emerge in an entirely new perspective from a quantum antiferromagnet and a scenario based on a spin-Peierls (SP) transition occurring below $`T_{c1}`$ has been accredited as the most plausible interpretation of the experimental findings seidel .

The title compound seems to be also an ideal material to investigate a broken symmetry ground state with orbital degrees of freedom but without charge ordering. The relevant role played by large electronic energy scales, associated to the orbital degrees of freedom, differentiates $`TiOCl`$ from $`CuGeO_3`$ and $`NaV_2O_5`$, two other intensively studied spin-Peierls systems: $`CuGeO_3`$ being characterized by a state without orbital and charge degrees of freedom, $`NaV_2O_5`$ with orbital and charge degrees of freedom imai ; smolinski ; mostovoy ; lemmensrev . In this context, it is worth mentioning that the coupling of orbital to spin degrees of freedom in a chain system may establish a novel route to the formation of spin gap states and spin-orbital excitations pati ; yamashita ; koleshuk .

Optical methods, like infrared or Raman spectroscopy, are powerful experimental tools in revealing the characteristic energy scales associated to the development of broken symmetry ground states, driven by magnetic and/or structural phase transitions. Indeed, information on the nature of the electronic (magnetic) ground state, lattice distortion and interplay of electronic (magnetic) and lattice degrees of freedom can be obtained studying in detail the electronic (magnetic) excitations and the phonon spectrum, as a function of temperature. Furthermore, the role played by strong quantum fluctuations in S=1/2 systems, an issue of key importance, can be addressed as well. We provide here a complete set of infrared optical data on $`TiOCl`$ and a thorough analysis of its electrodynamic response. The paper is organized as follows: we first briefly describe the experiment and present the data; the discussion will then emphasize the temperature dependence of the phonon spectrum from where we extract relevant information about the spin-gap ground state below $`T_{c1}`$.

## II Experiment and Results

Our $`TiOCl`$ single crystals were synthesized by standard vapor-transport techniques from $`TiO_2`$ and $`TiCl_3`$, according to the procedure described in Ref. schaefer, . The crystals were checked by X-ray diffraction experiments and static magnetic susceptibility seidel ; imai . $`TiOCl`$ is an oxyhalogenide with layered structure formed of $`Ti^{3+}O^2`$ bi-layers, separated by $`Cl^{}`$ bi-layers. The basic $`TiO_4Cl_2`$ octahedra build an edge-shared network in the ab-plane of the orthorhombic unit cell. $`\chi (T)`$, besides the already mentioned kink and sharp drop at $`T_{c2}`$ and $`T_{c1}`$ respectively, is also characterized by a broad maximum around 400 $`K`$. Above 100 $`K`$ $`\chi (T)`$ can be fitted by a S=1/2 Heisenberg spin chain model with an antiferromagnetic (AF) exchange coupling constant $`J=660`$ $`K`$ (Ref. seidel, ). Furthermore, the specific heat $`C_p(T)`$ displays an anomaly only at $`T_{c2}`$ (Ref. lee, ).

We have measured the optical reflectivity $`R(\omega )`$ from the far infrared (FIR) up to the ultra-violet (UV) spectral range at temperatures between 10 and 300 $`K`$ and also as a function of magnetic field. Since we did not find any magnetic field dependence, we will focus on the temperature dependence only. The Kramers-Kronig (KK) transformation of $`R(\omega )`$ allows us to evaluate the optical functions, like the real part $`\sigma _1(\omega )`$ of the optical conductivity. Further details pertaining to the experimental method can be found elsewhere wooten . Light was linearly polarized along the chain b-axis and the transverse a-axis seidel ; beynon . In order to avoid leakage effects of the polarizer, the polarization of light in our experiment always coincides with the vertical axis of the sample mounting so that the investigated crystallographic direction was perfectly parallel to the polarization of the light beam. Therefore, the polarization dependence was obtained by rotating the sample (instead of the polarizer) by 900 degrees inside the cryostat. This assures that no undesired projections of the light polarization along any transverse crystallographic direction occurs in our experiment.

Figure 1 summarizes our results, by focusing the attention on the temperature dependence of $`R(\omega )`$ in the infrared spectral range and for both polarization directions. The insets display the whole $`R(\omega )`$ spectra at 300 $`K`$ with a logarithmic energy scale. The first obvious observation is the strong anisotropy of the optical response within the ab-plane and for photon energies below $`10^4cm^1`$. Despite the two dimensional layered-like structure, the anisotropy in the lattice dynamics may be considered as a signature for the low dimensionality of $`TiOCl`$. Figure 2 reproduces the real part $`\sigma _1(\omega )`$ of the optical conductivity at 300 $`K`$ in the far infrared spectral range, as obtained from the KK transformation of $`R(\omega )`$. The inset in panel (b) enhances the visible spectral range, stressing the feature around 8x103 $`cm^1`$ ($``$ 1 $`eV`$) for both polarization directions. Above 4x104 $`cm^1`$ the $`\sigma _1(\omega )`$ spectra (not shown here, see Ref. lemmens,  for more details) were found to be polarization independent.

## III Discussion

The high frequency part of the excitation spectrum lemmens  is dominated by electronic interband transitions (Fig. 1 and inset Fig. 2b). Recent LDA+U calculations seidel , using the full-potential LMTO method, predict a split-off of the (one-dimensional) t2g bands creating an insulating state with a (charge) gap of about $`8100cm^1`$ (1 $`eV`$). The t2g band is derived from the dxy orbitals corresponding to the linear $`Ti`$-chains along the crystallographic b-axis seidel . This agrees with our data displaying a peak at $`8`$x10$`{}_{}{}^{3}cm^1`$ along the chain b-axis and a pronounced shoulder at the same energy along the transverse a-axis (see arrow in inset of Fig. 2b). The same band structure calculations seidel  suggest furthermore interband transitions between the $`O`$ and $`Cl`$ p-levels and the $`Ti`$ d-levels at energies between 3.2x104 and 5.6x10$`{}_{}{}^{4}cm^1`$ (4 and 7 $`eV`$). This is again very much in agreement with the absorption features seen in our $`\sigma _1(\omega )`$ spectra (see insets of Fig. 1 in Ref. lemmens, ) along both polarization directions.

In the far infrared spectral range (main panels of Fig. 1), several absorptions dominate the $`R(\omega )`$ spectra. The absorption features are better seen in the real part $`\sigma _1(\omega )`$ of the optical conductivity (Fig. 2). On the one hand, along the chain b-axis (Fig. 2b) there is a strong peak at 294 $`cm^1`$ with additional absorptions, overlapped to its low frequency tail, at 251 and 231 $`cm^1`$. Moreover, we recognize broad absorptions at 177 $`cm^1`$ and around 90 $`cm^1`$. Along the transverse a-axis (Fig. 2a) on the other hand, there is a strong peak at 438 $`cm^1`$ and less intensive absorptions at 68, 104, 294, 347 and 387 $`cm^1`$, as well as a very broad feature around 200 $`cm^1`$. A few absorptions are furthermore characterized by an asymmetric shape (see below). The strongest modes at 294 and 438 $`cm^1`$ along the b- and a-axis, respectively, display rather broad high frequency tails, which might be indicative of some anharmonicity.

For $`TiOCl`$ with the bisandwich layer structure of $`FeOCl`$-type beynon , the space group $`Pmmn(59,D_{2h})`$ can be considered at room temperature, for which two $`B_{3u}`$ modes polarized along the a-axis, two $`B_{2u}`$ along the b-axis and two $`B_{1u}`$ along the c-axis can be predicted as infrared (IR) active phonons. Because our samples are rather thin, we only have access to the $`B_{2u}`$ and $`B_{3u}`$ modes of the ab-plane. We note that 3$`A_g`$, 3$`B_{2g}`$ and 3$`B_{3g}`$ Raman active phonons are expected, as well. For light polarized within the ab-plane only the 3$`A_g`$ modes, inducing displacements along the c-axis, can be detected lemmens . Classical shell model calculations allow to extract eigenfrequencies and eigenvectors for both Raman and IR-active phonons of $`TiOCl`$ (Ref. kovaleva, ). As far as the IR phonons are concerned, the calculations predict the $`B_{3u}`$ (a-axis) phonons at 91 and 431 $`cm^1`$ and the $`B_{2u}`$ (b-axis) at 198 and 333 $`cm^1`$. The agreement between the calculated phonon frequencies and the experimental observation is pretty good. Particularly, the two high frequency ones can be identified with the most pronounced features in the experimental a- and b-axis spectra, respectively. Figure 3 shows the normal mode eigenvector patters for the IR active phonons, resulting from our shell model calculations. Table I summarizes the predicted and the so far experimentally determined phonon frequencies for the IR-active modes and, as complement, for the Raman-active modes lemmens , as well.

Even though the calculated frequencies of the IR phonon modes agree well with some features in our spectra, a larger number of phonon-like absorptions than theoretically predicted is found for both polarizations. The sample mounting chosen in our experiment (see above) allows us to exclude leakage effects due to the polarizer. However, one might invoke some twinning of the specimens. This could lead to additional phonon modes, due to the mixing of different polarization directions. This possibility is, nevertheless, rather unlikely because of the strong anisotropy of the optical spectra. If domains would be present because of twinning, phonons for both crystallographic axes would be detected for both polarizations of light and no anisotropy would be found. For instance the peaks at 387 and 438 $`cm^1`$ along the a-axis (Fig. 2a) are totally absent in the spectra along the b-axis (Fig. 2b). The same applies for the sharp feature at about 104 $`cm^1`$ for the a-axis. Moreover as it will be discussed in details below, the temperature dependence in $`\sigma _1(\omega )`$ can differ substantially even for absorptions coinciding at the same frequency in both polarizations. Therefore, we are confident that no common features are shared in FIR among the two polarizations. We propose that the effective space group corresponds to a lower symmetry than assumed so far, or that additional surface modes may become IR-active.

In order to shed light on the temperature dependence of the phonon spectrum we have fitted the optical conductivity with the so-called Fano expression cardona ; fano :

$$\stackrel{~}{\sigma }(\omega )=\underset{j}{}i\sigma _{0j}\frac{(q_j+i)^2}{i+x(\omega )},$$
(1)
with $`x(\omega )=\frac{\omega _{0j}^2\omega ^2}{\gamma _j\omega }`$, where $`\omega _{0j}`$ is the resonance frequency, $`\gamma _j`$ is the width (i.e., damping) and $`\sigma _{0j}=\omega _{pj}^2/\gamma _jq_j^2`$ with $`\omega _{pj}`$ as the oscillator strength and $`q_j`$ as the so-called asymmetry factor of the $`j`$-absorption. The asymmetric line shape for the (sharp) phonon modes derives from an interaction between lattice vibrations and a continuum, usually given by an electronic background. The interaction with a magnetic continuum may also lead to a Fano lineshape, as shown in the Raman scattering spectra of low dimensional spin systems lemmensrev ; choi . It is verified easily that for the dimension-less Fano parameter $`q_j\mathrm{}`$ one can recover the lineshape of the harmonic Lorentzian oscillator wooten ; cardona . The approach of eq. (1) was successfully applied by Damascelli et al. damascelli2 ; damascelli3  to the spin-Peierls system $`\alpha ^{^{}}NaV_2O_5`$.

Alternative approaches, based on the Fano theory fano , are available in the literatures. Here, we quote first of all the work by Lupi et al. lupi  on the phonon interaction with a polaronic background in $`Nd_{1.96}Ce_{0.04}CuO_{4+y}`$. This approach is based on the extension of Fano’s formalism by Davis and Feldkamp (DF) davis , who considered the case of an interaction between an arbitrary number of discrete states and continua. In this work, we will primarily focus our attention on the fits of $`\sigma _1(\omega )`$ after eq. (1). Nevertheless, in order to stress the equivalence among different approaches, we will discuss and compare the relevant asymmetry $`q_j`$-factors obtained with eq. (1) and by the DF formalism. Secondly, we also mention the discussion of the c-axis phonon modes in $`YBa_2Cu_3O_y`$ by Schützmann et al. schuetzmann . In this phenomenological approach, the conventional Lorentz shape was modified by a factor $`e^{i\theta }`$, where $`\theta `$ accounts for the asymmetry. This model, however, does not add relevant physical insight to the discussion with respect to the more simple Lorentz model wooten . Therefore, it will not be considered further.

The total fit of $`\sigma _1(\omega )=Re(\stackrel{~}{\sigma }(\omega ))`$, covering the whole spectral range from FIR up to UV, is obtained by summing over eleven and ten contributions in eq. (1) for the a- and b-axis (Ref. param, ), respectively. The fit of $`\sigma _1(\omega )`$ at 300 $`K`$ and the single components in FIR for both polarization directions are shown in Fig. 2. The reproduction of the experimental $`\sigma _1(\omega )`$ curve is astonishingly good and the same fit quality is obtained at all temperatures. In passing, we also note that the same set of fit parameters param  allows us to reproduce the measured $`R(\omega )`$ spectra (see, e.g., the fit of $`R(\omega )`$ at 300 $`K`$ in the insets of Fig. 1).

The temperature dependence of the fit parameters ($`\omega _{0j},\gamma _j,\omega _{pj}`$ and $`q_j`$) param  is shown, as percentage change with respect to the 300 $`K`$ data (e.g., $`\mathrm{\Delta }\omega _{0j}(T)/\omega _{0j}(300K)`$, with $`\mathrm{\Delta }\omega _{0j}(T)=\omega _{0j}(T)\omega _{0j}(300K)`$), in Figs. 4, 5 and 6 for both polarizations. Along the a-axis the lower seven while along the b-axis the lower six oscillators are temperature dependent and will be here discussed further. The overall temperature dependence mainly develops below 200 $`K`$ and tends to saturate below 100 $`K`$ (particularly for the chain b-axis). The temperature dependence, occurring in a broad temperature interval and extending well above $`T_{c1}`$, is indicative of an extended fluctuation regime, which has been recognized in NMR data imai , as well. The relaxation rates of $`{}_{}{}^{35}Cl`$ sites show dynamic lattice distortion with onset at 200 $`K`$ while for the $`{}_{}{}^{46,49}Ti`$ sites, $`1/TT_1`$, which probes the spin degrees of freedom, forms a maximum at about 135 $`K`$ (Ref. imai, ). Therefore, the interplay between the lattice and spin degrees of freedom must be already taking place at high temperatures. The temperature dependence of $`1/TT_1`$ implies a pseudo-gap phase in the homogeneous state of the spin system with an estimated pseudo-gap $`\mathrm{\Delta }_{fluct}430K`$ (Ref. imai, ). The temperature dependence of the ESR parameters (i.e., the ESR line width $`\mathrm{\Delta }H`$ and the so-called ESR $`g`$-tensor) also displays a progressive evolution over a broad temperature range between 200 $`K`$ and $`T_{c1}`$ (Ref. kataev, ). From the analysis of the ESR signal it is claimed that a strong coupling between spin and lattice degrees of freedom exists and that spin as well as orbital fluctuation effects above $`T_{c1}`$ may be responsible for the peculiar temperature dependence of various quantities (e.g., $`\chi (T)`$).

The resonance frequencies ($`\omega _{0j}`$) of almost all phonons tend to increase (Fig. 4a and 5a), though moderately (i.e., the change does not exceed 4 $`\%`$), with decreasing temperature, indicating a progressive hardening of the modes. The resonance at 320 $`cm^1`$ along the b-axis, accounting for the broad high frequency tail of the mode at 294 $`cm^1`$, displays on the contrary a weak softening. A well-defined soft mode is in principal expected in models for the conventional SP transition where the structural deformation is driven by a linear coupling between the lattice and the magnetic degrees of freedom. As far as the dynamical interplay between spins and phonons in $`TiOCl`$ is concerned, it is clear from the temperature dependence of our optical spectra that neither a soft mode nor a generalized red-shift in the resonance frequency of the phonons have been detected. At this point, apart from the 320 $`cm^1`$ mode along the b-axis, we speculate that the transition at $`T_{c1}`$ is not driven by a softening of the IR phonon spectrum. A final word on the soft mode issue will only be possible with neutron scattering experiments, since the lattice dimerization involved in the Peierls transition is related to normal modes away from the Brillouin zone center. From the perspective of the IR spectrum, one could have hoped that the presence of a soft mode would have resulted in an overall softening of the phonon-branch it belongs to. The absence of a clear signature for IR phonons softening is common to other spin-Peierls systems, like $`CuGeO_3`$ (Ref. damascelli, ). Nevertheless, evidence for phonon softening has been found in the Raman scattering experiments lemmens . A broad feature was identified at about 160 $`cm^1`$ for the chain b-axis polarization. The weight of this signal gets confined and softens down to 130 $`cm^1`$, i.e, by $`20\%`$, with decreasing temperature. This mode is ascribed to a Brillouin zone boundary phonon. The experimentally observed $`A_g`$ mode at 203 $`cm^1`$ (Table I) with light polarization along the b-axis is its related $`\mathrm{\Gamma }`$-point Raman-allowed phonon lemmens .

Most of the phonon modes get narrow with decreasing temperature (Fig. 4c and 5c). Only the mode at 294 $`cm^1`$ along the a-axis displays a broadening with decreasing temperature. Particularly the width $`\gamma _j`$ of quite all phonons along the chain b-axis follows very closely the temperature dependence of the magnetic susceptibility $`\chi (T)`$. The temperature dependence of $`\gamma _j`$ in $`TiOCl`$ is very similar to the findings in $`\alpha ^{^{}}NaV_2O_5`$ (Refs. damascelli2, ). The pronounced narrowing of the modes occur in the temperature interval of the so-called pseudo spin-gap phase identified in the NMR spectra imai . It seems therefore natural to relate this phonon narrowing with the suppression of low frequency spin fluctuations and to consider it as another fingerprint for the coupled spin-lattice fluctuations.

It turns out that most of the absorptions, seen in our spectra (Fig. 1 and 2) and described by the $`j`$-components in eq. (1), reduce to the Lorentzian-like (i.e., $`q_j\mathrm{}`$) shape. Only the peak at 104 $`cm^1`$ along the a-axis and at 294 $`cm^1`$ along the b-axis display a Fano-like asymmetry. The asymmetry (Fig. 6) of the mode at 104 $`cm^1`$ along the a-axis gradually decreases (i.e., $`q_j`$ gets larger) with decreasing temperature, although the mode remains considerably asymmetric at all temperatures. This indicates that there is a predominant interaction with the continuum both above and below $`T_{c1}`$. On the other hand, the temperature dependence of the asymmetry for the 294 $`cm^1`$ mode along the b-axis displays a clear crossover between 200 $`K`$ and $`T_{c2}`$ from an asymmetric Fano-like shape (i.e., $`q_j`$ small) to a Lorentzian oscillator (i.e., $`q_j`$ very large). The distinct behaviour in the temperature dependence of the $`q_j`$-factors within the ab-plane is a further fingerprint for the anisotropy of the lattice dynamics as well as of the coupling between phonon and continuum. The clear Fano-Lorentz cross-over along the chain b-axis suggests moreover the suppression of the interaction with the continuum with decreasing temperature damascelli2 . This, combined with the anisotropic temperature dependence of the $`q_j`$-factors themselves, hints once more to a progressive dimensionality cross-over (two-to-one) within the ab-plane with decreasing temperature. Since $`q_j<0`$ for both asymmetric modes, the relevant continuum of excitations, that is renormalized with temperature, covers an energy interval below the phonon resonance frequencies. For the chain b-axis, this identifies a characteristic energy scale of the order of 400 $`K`$. In Fig. 6, we also report, for comparison, the $`q_j`$-factor for both modes as calculated from the Fano model based on the approach of Davis and Feldkamp davis . Even though the two Fano approaches cardona ; davis  (eq. (1) and DF) are formally different (i.e., they are characterized by different energy powerlaw decays of the absorption coefficient), the corresponding $`q_j`$-factors are identical both in absolute value param  and in the relative percentage change (Fig. 6). This stresses the equivalence of the Fano asymmetry concept (parameterized by the $`q_j`$-factors) for both calculations.

The temperature dependence of the spectral weight encountered in the phonon spectrum is also of interest. We have observed lemmens  that the spectral weight encountered in $`\sigma _1(\omega )`$ at low frequencies tends to decrease below 200 $`K`$. The total spectral weight, obtained by integrating $`\sigma _1(\omega )`$ up to the UV spectral range, however, is conserved and it is fully recovered already by $`10^4cm^1`$ ($``$ 1 $`eV`$) lemmens . This is confirmed by the behaviour of the squared ($`\omega _{pj}^2`$) oscillator strengths (Fig. 4b and 5b). Particularly for the b-axis, the spectral weight is progressively removed with decreasing temperature over a spectral range of roughly 400 $`K`$. This is in agreement with the energy scale identified above in the analysis of the phonon asymmetry within the Fano approach. Most of the suppressed weight at low frequencies moves into the modes at 294 or 438 $`cm^1`$ or into their high frequency tails along the b- and a-axis, respectively. The remaining part of the suppressed weight shifts from the elastic degrees of freedom towards zone boundary (folded) modes or, as we favor for $`TiOCl`$, to the electronic degrees of freedom at high energies. Again this overall shift mainly occurs between $`T_{c2}`$ and 200 $`K`$.

Finally, the giant reduction of the phonon width, the behaviour of the Fano $`q_j`$-factors (particularly along the b-axis) as well as the suppression of spectral weight in FIR (Figs. 4, 5 and 6) suggest the presence and development of a characteristic energy scale. Above all the depletion of spectral weight over an energy range of the order of 400 $`K`$ is very much reminiscent of a similar behaviour in the Raman spectra, occurring over the same energy interval with decreasing temperature and associated to the spin-gap opening lemmens . Setting $`2\mathrm{\Delta }_{opt}`$ 300 $`cm^1`$ ($`430`$ K) as lower bound for the spin-gap energy, we obtain a reduced gap ratio $`2\mathrm{\Delta }_{opt}/k_BT_{c1}4.6`$ and 6.7 for $`T_{c2}`$ and $`T_{c1}`$, respectively. With respect to the mean-field results (i.e., $`2\mathrm{\Delta }/k_BT_c`$ 3.52) our larger gap ratios might reveal competing exchange paths or electronic degrees of freedom lemmens , but are more reasonable than those obtained from recent NMR study imai . Indeed, the extraordinary larger spin-gap $`\mathrm{\Delta }_{fluct}`$ would correspond to a reduced gap ratio ranging between 9 and 13 for $`T_{c1}`$ and $`T_{c2}`$, respectively. One can reconcile the outcome of a typical local probe like NMR with the optical results, which notably give an average perspective of the excitation spectrum, by following the development of both the magnetic and structural correlations. With decreasing temperature down to $`T_{c2}`$ the coherence length of the structural distortion increases and the magnetic correlations cross-over from 2D to 1D (Ref. lemmens, ). The energy gain at $`T<T_{c2}`$ is mainly related to the spin system. Therefore, the related anomaly in the specific heat lee  is small and in conventional X-ray scattering no sign of a coherent structural distortion can be found kataev . With further decreasing $`T`$ the structural distortion becomes long range. Below $`T_{c1}`$, $`TiOCl`$ has a conventional behaviour closely related to a spin-Peierls system. Therefore, the spin-gap $`2\mathrm{\Delta }_{fluct}`$ (from NMR imai ) is the lowest energy for the local double spin-flip in the short range order distorted phase, while $`2\mathrm{\Delta }_{opt}`$ (from IR and Raman lemmens ) is the energy for the global spin-gap of the fully dimerized chain.

## IV Conclusion

The phase transition of $`TiOCl`$ at $`T_{c1}`$ is not of simple character and several features point towards an unconventional spin-gap formation. Particularly intriguing is the temperature dependence of the phonon spectrum which, alike the NMR and ESR spectra, and the magnetic susceptibility, hints towards the key role of both orbital and magnetic degrees of freedom in shaping the magnetic properties of $`TiOCl`$. Fluctuation effects, extending over a broad temperature range from $`T_{c1}`$ up to 200 $`K`$, seem to be the most peculiar property of this low-dimensional spin-1/2 quantum system and may be indicative of a novel coupling between low and high energy scales.

###### Acknowledgements.

The authors wish to thank J. Müller for technical help, and A. Damascelli, B. Schlein, P. Calvani and A. Perucchi for fruitful discussions. This work has been supported by the Swiss National Foundation for the Scientific Research, INTAS 01-278, DFG SPP1073 and by the MRSEC Program of the National Science Foundation under award number DMR 02-13282.


text:
# Classical capacity of the lossy bosonic channel: the exact solution

## Classical capacity.–

The classical capacity of a channel can be expressed in terms of the Holevo information

$`\chi (p_j,\sigma _j)S({\displaystyle \underset{j}{}}p_j\sigma _j){\displaystyle \underset{j}{}}p_jS(\sigma _j),`$ (1)
where $`p_j`$ are probabilities, $`\sigma _j`$ are density operators and $`S(\varrho )`$Tr$`[\varrho \mathrm{log}_2\varrho ]`$ is the von Neumann entropy. Since it is not known if $`\chi `$ is additive, $`C`$ must be calculated by maximizing the Holevo information over successive uses of the channel, so that $`C=sup_n(C_n/n)`$ with

$`C_n=\underset{p_j,\sigma _j}{\mathrm{max}}\chi (p_j,𝒩^n[\sigma _j]),`$ (2)
where the states $`\sigma _j`$ live in the Hilbert space $`^n`$ of $`n`$ successive uses of the channel and $`𝒩`$ is the completely positive map that describes the channel hsw . In our case, $``$ is the Hilbert space associated with the bosonic modes used in the communication and $`𝒩`$ is the loss map. Because $``$ is infinite dimensional, $`C_n`$ diverges unless the maximization in Eq. (2) is constrained: here we assume that the mean energy of the input state in each of the $`n`$ realizations of the channel is a fixed quantity $``$. For multimode bosonic channels, $`𝒩`$ is given by $`_k𝒩_k`$, where $`𝒩_k`$ is the loss map for the $`k`$th mode, which can be obtained, tracing away the vacuum noise mode $`b_k`$, from the Heisenberg evolution

$`a_k^{}=\sqrt{\eta _k}a_k+\sqrt{1\eta _k}b_k,`$ (3)
with $`a_k`$ and $`a_k^{}`$ being the annihilation operators of the input and output modes and $`0\eta _k1`$ is the mode transmissivity (quantum efficiency).

The main result of this paper is that the capacity of the lossy bosonic channel, in bits per channel use, is

$`C=\underset{N_k}{\mathrm{max}}{\displaystyle \underset{k}{}}g(\eta _kN_k),`$ (4)
where $`g(x)(x+1)\mathrm{log}_2(x+1)x\mathrm{log}_2x`$ and where the maximization is performed on the modal average photon-number sets $`\{N_k\}`$ that satisfy the energy constraint

$`{\displaystyle \underset{k}{}}\mathrm{}\omega _kN_k=,`$ (5)
($`\omega _k`$ is the frequency of the $`k`$th mode).

We derive Eq. (4) by giving coincident lower and upper bounds for $`C`$. The right-hand side of Eq. (4) was shown, in nostro , to be a lower bound for $`C`$ by generalizing the narrowband analysis of holevo . This expression was obtained from Eq. (2) by calculating $`\chi `$ for $`n=1`$ under the following encoding: in every mode $`k`$ we use a mixture of coherent states $`|\mu _k`$ weighted with the Gaussian probability distribution

$`p_k(\mu )=\mathrm{exp}[|\mu |^2/N_k]/(\pi N_k).`$ (6)
This corresponds to feeding the channel the input state

$`\varrho ={\displaystyle \underset{k}{}}{\displaystyle 𝑑\mu p_k(\mu )|\mu _k\mu |},`$ (7)
which is a thermal state that contains no entanglement or squeezing. The right-hand side of Eq. (4) is also an upper bound for $`C`$. To see that this is so, let $`\overline{p}_j`$, $`\overline{\sigma }_j`$ be the optimal encoding on $`n`$ uses of the channel, which gives the capacity $`C_n`$ of Eq. (2). The definition of $`\chi `$ and the subadditivity of the von Neumann entropy allow us to write

$`C_nS(𝒩^n[\overline{\sigma }]){\displaystyle \underset{l=1}{\overset{n}{}}}{\displaystyle \underset{k}{}}S(𝒩_k[\varrho _k^{(l)}]),`$ (8)
where $`\overline{\sigma }_j\overline{p}_j\overline{\sigma }_j`$ and $`𝒩_k[\varrho _k^{(l)}]`$ is the reduced density operator of the $`k`$th mode in the $`l`$th realization of the channel, which is obtained from $`𝒩^n[\overline{\sigma }]`$ by tracing over all the other modes and over the other $`n1`$ channel realizations. The first inequality in Eq. (8) comes from bounding $`C_n`$ by the amount of information that can be transmitted through a lossless channel with input state $`𝒩^n[\overline{\sigma }]`$, viz., the output of the lossy channel with optimal input state $`\overline{\sigma }`$ yuenmax . Now let $`N_k^{(l)}`$ be the average photon number for the state $`\varrho _k^{(l)}`$; $`\{N_k^{(l)}\}`$ must satisfy the energy constraint (5) for all $`l`$ nota3 . Moreover, the loss will leave only $`\eta _kN_k^{(l)}`$ photons, on average, in the corresponding output state $`𝒩_k[\varrho _k^{(l)}]`$. This implies that

$`S(𝒩_k[\varrho _k^{(l)}])g(\eta _kN_k^{(l)}),`$ (9)
where the inequality follows from the fact that the term on the right is the maximum entropy associated with states that have $`\eta _kN_k^{(l)}`$ photons on average bekenstein ; caves . Introducing Eq. (9) into (8), we obtain the desired result

$`C_n{\displaystyle \underset{l=1}{\overset{n}{}}}{\displaystyle \underset{k}{}}g(\eta _kN_k^{(l)})n\underset{N_k}{\mathrm{max}}{\displaystyle \underset{k}{}}g(\eta _kN_k),`$ (10)
where the maximization is performed over the sets $`\{N_k\}`$ that satisfy Eq. (5). Because Eq. (10) holds for any $`n`$, we conclude that the right-hand side of (4) is indeed also an upper bound for $`C`$.

## Discussion.–

Some important consequences derive from our analysis. First, capacity is achieved by a single use of the channel ($`n=1`$) employing random coding—factorized over the channel modes—on coherent states as shown in Eq. (7). This means that, at least for this channel, entangled codewords are not necessary and that the Holevo information is not superadditive. Notice that the lossy bosonic channel can accommodate entanglement among successive uses of the channel, as well as entanglement among different modes in each channel use. Surprisingly, neither of these two strategies is necessary to achieve capacity. Nor is it necessary to use any non-classical state, such as a photon number state or a squeezed state, to achieve capacity; classical (coherent state) light is all that is needed. Classical light suffices because the loss map $`𝒩`$ simply contracts coherent-state codewords in phase space toward the vacuum state. Coherent states retain their purity in this process, and hence the non-positive part of the Holevo information—the second term of the right-hand side of Eq. (1)—retains its maximum value of zero. Despite the preceding properties, quantum effects are relevant to communication over the lossy bosonic channel. For example, our proof does not exclude the possibility of achieving capacity using quantum encodings, and such encodings may have lower error probabilities, for finite-length block codes, than those of the capacity-achieving coherent state encoding. This is certainly true for the lossless case. In particular, it was already known that $`C`$ can be achieved with a number-state alphabet yuen ; caves ; our work shows that there is also a coherent-state encoding that achieves capacity for this case. \[The two procedures employ the same average input state, Eq. (7)\]. However, the probability of the receiver confusing any two distinct finite-length number state codewords is zero in the lossless case, whereas it is positive for all pairs of finite-length coherent-state codewords. The lossless case also provides an example of the possible role of quantum effects at the receiver: the optimal coherent-state system uses a classical transmitter, but its detection strategy, can be highly non-classical hsw . In contrast, the optimal number-state system for the lossless channel requires a non-classical light source, but its receiver uses simple modal photon counting.

How well can we approach this capacity using conventional decoding procedures? Using the coherent-state encoding of Eq. (7) with either heterodyne or homodyne detection, the amount of information that can be reliably transmitted is

$`I=\underset{N_k}{\mathrm{max}}{\displaystyle \underset{k}{}}\xi \mathrm{log}_2(1+\eta _kN_k/\xi ^2),`$ (11)
where $`\xi =1/2`$ for homodyne and $`\xi =1`$ for heterodyne, and where, as usual, the maximization must be performed under the energy constraint (5). Equation (11) has been obtained by summing over $`k`$ the Shannon capacities for the appropriate detection procedure caves . In general $`I<C`$: heterodyne or homodyne detection cannot be used to achieve the capacity. However, heterodyne is asymptotically optimal in the limit of large numbers of photons in all modes, $`N_k\mathrm{}`$ for all $`k`$, because $`g(x)/\mathrm{log}_2(x)1`$ as $`x\mathrm{}`$.

The capacity expression $`C`$ can be simplified by using standard variational techniques to perform the constrained maximization in Eq. (4), yielding nostro

$`C={\displaystyle \underset{k}{}}g\left(\eta _kN_k(\beta )\right),`$ (12)
where $`N_k(\beta )`$ is the optimal photon number distribution

$`N_k(\beta )={\displaystyle \frac{1/\eta _k}{e^{\beta \mathrm{}\omega _k/\eta _k}1}},`$ (13)
with $`\beta `$ being a Lagrange multiplier that is determined through the constraint on average transmitted energy.

In the following sections we calculate the capacities of some bosonic channels. The first two examples help clarify the derivation of Eq. (4); the last is a realistic model of frequency-dependent lossy communication, on which we also evaluate the performance of homodyne and heterodyne detection.

## Narrowband channel.–

Consider the narrowband channel in which a single mode of frequency $`\omega `$ is employed. In this case, Eq. (12) becomes

$`C=g\left({\displaystyle \frac{\eta }{\mathrm{}\omega }}\right),`$ (14)
where $`N=/(\mathrm{}\omega )`$ is the average photon number at the input. Equation (14) was conjectured in holevo , where it was given as a lower bound on $`C`$. The following simple argument shows that $`g(\eta N)`$ is also an upper bound for $`C`$. Consider the lossless channel that employs $`\eta N`$ photons on average per channel use. Its capacity is given by $`\mathrm{max}_\varrho S(\varrho )`$, where the maximization is performed over input states $`\varrho `$ with mean energy $`^{}=\eta \mathrm{}\omega N`$ nota . The maximum, computed through variational techniques, is $`g(\eta N)`$ caves ; bekenstein . The lossless channel cannot have a lower capacity than the lossy channel, because both have the same average received energy, and the set of receiver density operators achievable over the lossy channel is a proper subset of those achievable in the lossless system yuenmax . This implies that $`g(\eta N)`$ is an also upper bound on $`C`$ and hence equal to $`C`$.

## Frequency-independent loss.–

Now consider a broadband channel with uniform transmissivity, $`\eta _k=\eta `$, that employs a set of frequencies $`\omega _k=k\delta \omega `$ for $`k`$. In this case, Eq. (12) gives nota2

$`C={\displaystyle \frac{\sqrt{\eta }}{\mathrm{ln}2}}\sqrt{{\displaystyle \frac{\pi 𝒫}{3\mathrm{}}}}𝒯,`$ (15)
where $`𝒯=2\pi /\delta \omega `$ is the transmission time, and $`𝒫=/𝒯`$ is the average transmitted power. Equation (15) was derived for the lossless case ($`\eta =1`$) in yuen  and was shown to provide a lower bound on $`C`$ in nostro . In order to show that the right-hand side of Eq. (15) is also an upper bound, consider the lossless broadband channel in which the average input power is equal to $`\eta 𝒫`$, viz., the average output power of the lossy channel. According to yuen , the capacity of this channel is $`(\sqrt{\pi \eta 𝒫/3})𝒯/\mathrm{ln}2`$, which coincides with the right-hand side of Eq. (15). The reasoning given above for the single-mode case now implies that the broadband lossless channel’s capacity cannot be less than that of the broadband lossy channel, thus completing the proof.

## Far-field, free-space optical communication.–

Consider the free-space optical communication channel in which the transmitter and the receiver communicate through circular apertures of areas $`A_t`$ and $`A_r`$ that are separated by an $`L`$-m-long propagation path. At frequency $`\omega `$ there will only be a single spatial mode in the transmitter aperture that couples appreciable power to the receiver aperture when the Fresnel number $`D(\omega )A_tA_r(\omega /2\pi cL)^2`$ satisfies $`D(\omega )1`$, ff . This is the far-field power transfer regime at frequency $`\omega `$, and $`D(\omega )`$ is the transmissivity achieved by the optimal spatial mode. A broadband far-field channel results when the transmitter and receiver use the optimal spatial modes at frequencies up to a critical frequency $`\omega _c`$, with $`D(\omega _c)1`$. In this case we use $`\eta _k=D(\omega _k)`$ in Eq. (12), and the capacity $`C`$ becomes nota2

$`C={\displaystyle \frac{\omega _c𝒯}{2\pi y_0}}{\displaystyle _0^{y_0}}𝑑xg\left({\displaystyle \frac{1}{e^{1/x}1}}\right),`$ (16)
where $`y_0`$ is a dimensionless parameter inversely proportional to the Lagrange multiplier $`\beta `$, which is determined from the power constraint

$`𝒫={\displaystyle \frac{2\pi \mathrm{}c^2L^2}{A_tA_r}}{\displaystyle _0^{y_0}}{\displaystyle \frac{dx}{x}}{\displaystyle \frac{1}{e^{1/x}1}}.`$ (17)
Although $`C`$ is proportional to the maximum frequency $`\omega _c`$, this factor cannot be increased without bound, for fixed transmitter and receiver apertures, because of the far-field assumption. Figure 1 plots $`C`$ versus $`𝒫`$ obtained from numerical evaluation of Eqs. (16) and (17).

To compare the capacity of Eq. (16) with the information transmitted using heterodyne or homodyne detection, we perform the Eq. (11) maximization. The Lagrange multiplier technique gives the optimal value $`N_k(\beta )=\mathrm{max}\{1/(\beta \mathrm{}\omega _k)\xi ^2/\eta _k,\mathrm{\hspace{0.33em}0}\}`$, plotted in Fig. 2. \[Notice that the non-negativity of this solution forbids the use of frequencies lower than $`\omega _0\xi ^2\beta \mathrm{}\omega _c^2/D(\omega _c)`$.\] With this photon number distribution, Eq. (11) becomes

$`I=\xi \omega _c𝒯\left(1/y_01+\mathrm{ln}y_0\right)/(2\pi \mathrm{ln}2),`$ (18)
where $`y_0`$ is now determined from the condition $`𝒫=\xi ^22\pi \mathrm{}c^2L^2(y_01\mathrm{ln}y_0)/(A_rA_s)`$. We have plotted $`I`$ versus $`P`$ in Fig. 1 for heterodyne and homodyne detection. At low power, the noise advantage of homodyne makes its capacity higher than that of heterodyne. At high power levels heterodyne prevails thanks to its bandwidth advantage, and its capacity approaches $`C`$ asymptotically.

## Conclusions.–

We have derived the classical capacity of the lossy multimode bosonic channel when the average energy devoted to the transmission is bounded. Interestingly, quantum features of the signals (such as entanglement or squeezing) are not required to achieve capacity, because an optimal coherent-state encoding exists. At the decoding stage, however, quantum effects might still be necessary (e.g., in the form of joint measurements on the output) as standard homodyne and heterodyne measurements are not optimal, except for the high power regime where heterodyne detection is asymptotically optimal. The focus of this paper has been the lossy channel with minimal (vacuum-state) noise. A more general treatment would include non-vacuum noise, and would allow for amplification.

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