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# np-nh bands in the N=28 isotones

## Abstract

The existence of n-particle n-hole deformed yrare bands in the N=28 isotones is explored using full $`pf`$-shell diagonalizations and the Lanczos Strength Function method. We find different 2p-2h and 4p-4h collective bands that, when allowed to mix, more often disappear. Only the 2p-2h yrare band in 52Cr and the 4p-4h yrare band in 56Ni survive, and only in this latter case, due to the reduced density of 2p-2h states, can the band be seen as a $`\gamma `$-cascade.

The occurrence of yrare bands of enhanced collectivity, with a well defined particle-hole structure on top of the ground state, has been recently documented by experiments in 56Ni , 36Ar  and 40Ca . In the Ni and Ar cases the bands are dominantly made of 4p-4h excitations while in the 40Ca the leading structure is 8p-8h . In 56Ni the band is clasified as highly deformed $`\beta `$= 0.3/0.4 , while in 36Ar and 40Ca they are characterised as superdeformed with $`\beta `$= 0.4/0.5 and $`\beta `$= 0.5/0.6 respectively. In a recent study , Mizusaki and co-workers have carried out a theoretical search for this kind of bands in the N=28 isotopes, using the Monte Carlo shell model approach. In this article we examine the same topic, in the framework of full $`pf`$-shell diagonalizations using the Lanczos method.

The $`pf`$-shell has been the locus of a lot of activity in nuclear structure since the advent of the exact 0$`\mathrm{}\omega `$ calculations in 48Cr . In a recent article  we have extend the full $`pf`$-shell calculations up to A=52 and we have introduced the interaction KB3G, the one used in this work. The diagonalizations are performed in the $`m`$-scheme using a fast implementation of the Lanczos algorithm through the code antoine  or in J-coupled scheme using the code nathan . Some details may be found in ref. . The Lanczos Strength Function (LSF) method, following Whitehead’s prescription , is explained and illustrated in refs. .

The calculation of yrare bands in nuclei with large shell model dimensionalities, poses serious computational problems. The reason is that, most often, the interesting states lie at excitation energies where the level density is high. This represents a real challenge for all the shell model approaches, because it requires the calculation of many states of the same spin and parity. While this can be easily done for m-scheme dimensions of a few millions, the task becomes formidable for dimensions of tens of millions. The method of ref  relies in the existence of local minima in the projected energy surface resulting of a constrained Hartree-Fock calculation. The Slater determinants corresponding to these minima are then fed into the quantum Monte Carlo diagonalization method ($`qmcd`$). While this method is reasonably under control for the yrast states and other states originating in well defined minima, it is not clear how would it work in less clear-cut situations. As an example, ref  claims that the $`qmcd`$ method is unpractical to describe a possible 4p-4h band in 54Fe, which is then studied at a lower level of approximation, doing variation after projection (VAP) on the cranked Hartree-Fock solution.

Our method proceeds by three steps:

I) The space of solutions is explored by means of diagonalizations restricted to configurations with a fixed number of particle-hole excitations on the top of the reference one (1f7/2)N, searching for collective bands.

II) If such bands are found, we proceed to immerse the bandhead state in the full space by means of the Lanczos Strength Function method, i.e. we take the np-nh ground state and use it as starting vector for the Lanczos iterations in the full space, in order to know whether it stands the mixing or not.

III) If it survives to the mixing, we try to build the physical band acting repeatedly upon it with the quadrupole operator and using again the LSF method as described below.

Let’s proceed with the first step in the four cases of interest, 50Ti, 52Cr, 54Fe and 56Ni. In tables 123 and 4 we list the excitation energies and the BE2’s corresponding to the fixed 2p-2h and 4p-4h bands. In 50Ti none of the bands appear to be really collective, even though there is a certain quadrupole linking among the states. In 52Cr both are quite regular, with large BE2’s in the 4p-4h case. For 54Fe the situation is more complex; the 2p-2h band is clearly less collective than the corresponding one in 52Cr, with a neat bifurcation at J=6, while the 4p-4h band mimics perfectly a well deformed rotor. The same is valid for the 4p-4h band of 56Ni; in this nucleus the 2p-2h band shows no collectivity at all.

In our second step, we take the 0+ band-head and allow it to mix with all the states. To optimize the calculation as well as to keep track of the initial state, we take it as starting vector (“pivot”) in the Lanczos construction in the full space (or in a large enough one). After N iterations, we compute its overlaps with the N quasi-physical states. For the fixed np-nh bandhead to be representative of a “physical” bandhead, there must be a single state that has a large overlap with it. As a bonus, this state is converged in very few iterations, what makes the method computationally efficient. In figure 1 we have plotted the overlaps for the 2p-2h (upper panel) and 4p-4h (lower panel) band-heads in 52Cr. The calculations are carried out in the full $`pf`$-shell (m-scheme dimension 45 millions) using the coupled code Nathan (0+ dimension, 8 $`\times `$ 105) and 150 iterations are made. Notice how the 2p-2h state is concentrated at 45% in one “physical” state with no other one taking any relevant share. The excitation energy of this state, 2.43 MeV, is in correspondence with the experimental 0$`{}_{2}{}^{}{}_{}{}^{+}`$ at 2.65 MeV. It has a 46% content of 2p-2h, 26% of 3p-3h, 18% of 4p-4h and minor percentages of the other components. The fact that the mixing takes place with components of higher p-h rank should result in an increase of collectivity with respect to the fixed 2p-2h band. Besides the “coherent” 2p-2h state, the next four 0+ states produced by the calculation are also in correspondence with the experimental 0+’s:

0$`{}_{3}{}^{}{}_{}{}^{+}`$; exp. 4.74 MeV; th. 5.15 MeV,

0$`{}_{4}{}^{}{}_{}{}^{+}`$; exp. 5.60 MeV; th. 5.47 MeV,

0$`{}_{5}{}^{}{}_{}{}^{+}`$; exp. 5.75 MeV; th. 6.04 MeV,

0$`{}_{6}{}^{}{}_{}{}^{+}`$; exp. 6.10 MeV; th. 6.30 MeV,

a rather spectacular achievement of the shell model spectroscopy!!

On the contrary, the much more collective 4p-4h band-head is completely dissolved in the full space; no physical state carries a dominant fraction of the overlap. According to that, no 4p-4h band exists in 52Cr. Whether the 2p-2h band has any experimental relevance or not, will be discussed below.

Very much the same occurs in 50Ti; the 2p-2h bandhead survives at 61% in the full space 0$`{}_{2}{}^{}{}_{}{}^{+}`$ at 4.08 MeV (exp. at 3.87 MeV); the 4p-4h bandhead is fully dispersed among many physical states.

For 54Fe the full space calculations of the overlap distribution become unaffordable. However, we think that it is sufficiently safe to compute the np-nh mixing at a level of truncation t=n+4. In figure 2 we present the results of these calculations (t=6 for the 2p-2h -upper panel- and t=8 for the 4p-4h -lower panel-). In this last case, the m-scheme dimension is 177 millions. Using the coupled code Nathan we deal with a 0+ dimension of 2.5 $`\times `$ 106 and make 150 iterations. The situation resembles that of 52Cr; the coherent 2p-2h state represents 43% of the 0$`{}_{2}{}^{}{}_{}{}^{+}`$ at 2.77 MeV (exp. at 2.56 MeV) and no other state carries a significant fraction of it. In the 4p-4h case the fragmentation is complete, no residue of a band is left. According to this result, the claim in ref.  of the existence of a 4p-4h band in this nucleus, based on a VAP-CHF calculation, has to be taken with some skepticism.

For 56Ni we refer to our calculations in  and to the experimental results to state the existence of a 4p-4h band. The reason why it survives in this nucleus and not in 54Fe, is clearly the very different level density in both nuclei. In 56Ni, because it is doubly magic, the number of 2p-2h states is nearly an order of magnitude smaller that in 54Fe, whose 4p-4h bands wrecks in a sea of 2p-2h states.

This brings us to step III. We have now several candidates to bandheads, but, do they develop a real band? The answer is “yes” in the well known case of the 4p-4h band in 56Ni. We shall now proceed to examine the situation in the other cases. It could be done “brute force” by computing many states of each spin and their E2 transition probabilities and looking for band-like patterns, but this approach is only realistic (from the computational point of view) in 50Ti, where we have actually used it to check our approximations. The method we use is, once again, an application of the Lanczos strength function technique. We start with the bandhead 0+ and apply the quadrupole operator on it: $`Q|0^+`$. This operation generates a threshold vector that we take as the “pivot” in the Lanczos procedure. We perform N$``$100 iterations to produce an approximate strength function. At this stage, either there is one state that carries most of the strength, signaling its pertenence to the band, or not, in which case there is no band. In the positive case the resulting $`|2^+`$ state is retained as a band member and we proceed to act with $`Q`$ on it. Now there are several possible angular momentum couplings, but we follow the $`\mathrm{\Delta }`$J=2 path in the even-even nuclei. The procedure is repeated until the strength bifurcates, dilutes or plainly disappears.

In 50Ti we obtain a sequence of states that fulfill the requirements discussed above. However, their energy spacings are not very much rotor-like and their B(E2)’s are only about 100 $`e^2fm^4`$. These values are comparable to those of the yrast band. Some of these states have been measured, but they do not appear to show any band signature.

In 52Cr we can definitely speak of a “theoretical” yrare band. Our results for the excitation energies are very close to those of ref. . In table 5 we list the excitation energies, the percentage of the B(E2)$``$ of the transition from J-2 to J carried by each state, the amount of 2p-2h components, the B(E2)$``$ and the spectroscopic quadrupole moments. All these numbers are consistent with a deformed band up to J=10, afterwards a bifurcation and reduction of the strength takes place. Notice the large B(E2) values, similar to those of the yrast band of 48Cr, corresponding to $`\beta `$ 0.3. Besides, the energy spacings are very close to those of a rigid rotor;

$`{\displaystyle \frac{\mathrm{\Delta }E(4^+)}{\mathrm{\Delta }E(2^+)}}`$=3(3.33);

$`{\displaystyle \frac{\mathrm{\Delta }E(6^+)}{\mathrm{\Delta }E(4^+)}}`$=1.9(2.1);

$`{\displaystyle \frac{\mathrm{\Delta }E(8^+)}{\mathrm{\Delta }E(6^+)}}`$=1.65(1.71);

$`{\displaystyle \frac{\mathrm{\Delta }E(10^+)}{\mathrm{\Delta }E(8^+)}}`$=1.46(1.53);

(the values in parenthesis are those of the rigid rotor limit). The percentage of the 2p-2h components as well as the occupation numbers of the individual orbits are nicely constant too. The spectroscopic quadrupole moments correspond to a prolate rotor and are fully consistent with the B(E2)’s. The sequence of calculated states, 0+ at 2.43 MeV, 2+ at 2.87 MeV, 4+ at 3.75 MeV and 6+ at 4.94 MeV can be put in correspondence with the experimental ones at 2.64 MeV (0+), 3.16 MeV (2+), 4.04 MeV (4+) and 5.14 MeV (6+). However, there are no transitions experimentally observed linking these states. This means that, due to the presence of many other 2p-2h states to which to decay by M1 transitions and to the phase space enhancement of the E2 transitions to the yrast band, the “theoretical” yrare band does not show up experimentally as a $`\gamma `$-cascade. In 54Fe the situation is even worse. The bifurcation, already present at the fixed 2p-2h level, appears also in the “physical” band. Only the sequence 0+, 2+, 4+ behaves like a band, but with B(E2)’s substantially smaller than in the 52Cr yrare band.

In summary, we have found that yrare bands of a definite np-nh character exist in the N=28 isotones. When full mixing is permitted, only the 2p-2h bands survive in 50Ti, 52Cr and 54Fe, with different degrees of collectivity. In 56Ni it is the 4p-4h band which is physical. This is due to the difference in the 2p-2h level density in the doubly magic case. In addition, we find that the 2p-2h bands preferentially decay out, making their experimental identification very difficult.

This work has been partly supported by MCyT (Spain), grant BFM2000-30 and by the IN2P3 (France)-CICyT (Spain) agreements. We also thank the CCC-UAM for a computational grant.


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# Theory of microphase separation of homopolymer–oligomer mixtures

## I Introduction

Various mesomorphic structures can be prepared using the strong (ionic) or weak (hydrogen) bonding, respectively, between homopolymers and head–functionalized oligomers or surfactants 1 . The interaction between the head group of the oligomeric molecule and suitable groups on the homopolymer chain, on the one hand, and unfavorable polar–nonpolar interactions between the non–polar tail of the oligomer and the rest of the system, on the other one, can cause the microphase separation. The latter effect results in a periodic alternation of the layers of stretched homopolymer chains surrounded by perpendicularly oriented oligomeric tails as it is shown in Figure 1.

An example of the ionically bonded system is represented by the homopolymer-oligomer mixture of atactic poly(4-vinyl pyridine) (P4VP) and dodecyl benzene sulfonic acid (DBSA) where due to a very strong interaction the microphase separation is realized over the whole temperature region 2 . The peculiarity of the systems of this kind is an increasing long space period $`L`$ as a function of the oligomeric fraction $`x`$ defined as the number of the oligomeric (DBSA) molecules per one pyridine ring (see Figure 2).

More complicated behavior is inherent in the hydrogen bonded systems where the weak interaction causes an order–disorder transition to homogeneous high–temperature state 1 ; 3 . An example of the system of this kind represents the mixture P4VP–(PDP)x of the same homopolymer P4VP with the surfactant 3-pentadecyl phenol (PDP). Here, contrary to the ionically bonded systems, the long space period decreases with increasing $`x`$ (see Figure 3).

As it is shown in Figure 2, an intermediate behavior (non–monotonous $`x`$–dependence of the long space period) was found in the system P4VP-(Zn(DBS)2)x where the ionic interaction between zinc dodecyl benzene sulfonate Zn(DBS)2 and P4VP is somewhat weaker than in the P4VP-(DBSA)x system4 .

Principally important for our considerations is the decreasing character of the temperature dependence of the long period found experimentally for all the systems mentioned above 1 4 . However, such a character of the dependence appears in the hydrogen bonded systems only within a finite temperature interval limited by the temperatures of crystallization (or glass transition $`T_g`$) from below and of the order–disorder transition $`T_c`$ from above (see Figure 4).

As it is shown in Figure 5, an increase of the oligomeric fraction leads to a non–monotonous dependence of the temperature $`T_c`$ with a maximum occuring near $`x=0.85`$.

The aim of this paper is to explain peculiarities of the microphased separated homopolymer–oligomer mixtures with both, strong and weak bonding, within a framework of the unified scheme of stochastic systems 5 .

Our consideration is based on the obvious equality for the long period $`L=2l+D`$ where $`l`$ is the oligomeric chain length and $`D`$ is the thickness of the homopolymer layer being fixed due to sharing of the surfactant molecules by homopolymer chains (see Figure 1). Physically, this share is reduced to the inverse magnitude $`2\pi /\omega `$ of the circular frequency of the alternation of the oligomer heads along the homopolymer chain. Then, the long period can be expressed by the following equation 1

$$L=2l+D_0\omega ^1,D_02\pi \left(\chi ^{1/6}n_0^{1/3}\right)bb$$
(1)
where $`\chi 10/N`$ is the Flory interaction parameter ($`N10^4`$ is the degree of polymerization of the homopolymer chains), $`n_010`$ is the number of segments in the oligomer chain, $`b`$ is the segment length. The frequency $`\omega `$ will be found from the effective equation of motion which is stochastic in nature and where the segment number $`n`$ ($`nN`$) plays the role of imagined time 6 .

## II Basic equations

The problem under consideration is addressed by the definition of effective law of motion $`c(n)`$ that determines the sequence of the alternation of oligomers along the homopolymer chain by means of the occupation number, $`c(n)`$, being $`c(n)=1`$ if the oligomer is attached to the segment $`n`$, and $`c(n)=0`$ otherwise. In the limit $`N\mathrm{}`$, the argument $`n`$ may be considered as a continuous one, and the behavior of the system is governed by the action and the dissipative functional

$$S=T\underset{0}{\overset{N}{}}L(c(n),\dot{c}(n))dn,R=\frac{\mathrm{\Theta }}{2}\underset{0}{\overset{N}{}}\left(\dot{c}(n)\right)^2dn$$
(2)
with dimensionless Lagrangian

$$L=K\mathrm{\Pi };K\frac{m}{2}\left(\dot{c}(n)\right)^2,\mathrm{\Pi }\frac{\tau }{2}\left(c(n)\right)^2.$$
(3)
Here dot denotes the derivative with respect to the segment number $`n`$, $`T`$ is temperature in energy units, $`\mathrm{\Theta }`$, $`m`$ and $`\tau `$ are inverse kinetic coefficient, inhomogeneity and interaction parameters, respectively. The key point in our consideration consists in that the effective mass $`m`$ in Eq.(3) is a fluctuating parameter with the mean value $`\overline{m}`$ and the variance $`\overline{(m\overline{m})^2}\sigma ^2`$ (bar denotes the average, as usually). Then, after the averaging of the exponent $`\mathrm{exp}(S/T)`$ over Gaussian distribution of the bare mass $`m`$, we obtain renormalized inhomogeneity energy

$$K=\frac{1}{2}\left(\overline{m}\stackrel{~}{\mathrm{\Delta }}\right)\left(\dot{c}(n)\right)^2,\stackrel{~}{\mathrm{\Delta }}\frac{\sigma ^2}{2}\underset{0}{\overset{N}{}}\left(\dot{c}(n^{})\right)^2dn^{}.$$
(4)
As a result, taking into account the stochastic source $`\zeta `$, relevant Euler equation arrives at non–linear Langevin equation

$$\stackrel{~}{m}\ddot{c}+n_c\dot{c}+\tau c=\zeta $$
(5)
where the effective mass $`\stackrel{~}{m}=\stackrel{~}{m}\{c(n)\}`$, characteristic number of correlating segments $`n_c`$ and $`\delta `$–correlated noise $`\zeta (n)`$, respectively, are introduced in accordance with definitions:

$`\stackrel{~}{m}\overline{m}\stackrel{~}{\mathrm{\Delta }},n_c{\displaystyle \frac{\mathrm{\Theta }}{T}},`$ (6)
$`\zeta (n)=0,\zeta (n)\zeta (n^{})=\delta (nn^{}).`$ (7)
To linearize the equation of motion (5) within the self–consistent approach, it is necessary to replace the fluctuational term $`\stackrel{~}{\mathrm{\Delta }}`$ of the renormalized mass in Eq. (4) by the averaged expression

$$\mathrm{\Delta }=\sigma ^2S(\nu )\nu ^2\frac{\mathrm{d}\nu }{2\pi }$$
(8)
where $`S(\nu )|c(\nu )|^2`$ is the structure factor in the frequency representation (angle brackets denote average over noise $`\zeta `$). Then, the Green function $`G\delta c/\delta \zeta `$ and the structure factor $`S=|G|^2`$ take the forms:

$$G=\left[\tau (\nu )\mathrm{i}n_c\nu \right]^1,S=\left[\tau ^2(\nu )+n_c^2\nu ^2\right]^1$$
(9)
where renormalized interaction parameter is introduced by equalities

$`\tau (\nu )\tau m_{ef}\nu ^2,m_{ef}\overline{m}\mathrm{\Delta }.`$ (10)
## III Determination of the period of microphase structure

To obtain physically observable values, at first one has to determine the effective mass $`m_{ef}`$ given by Eqs.(10), (8). On the basis of the theory of residues, using the structure factor, Eq.(9) arrives at the expression for renormalization mass parameter

$$\mathrm{\Delta }=\frac{\sigma ^2}{n_cm_{ef}}.$$
(11)
Inserting here Eqs.(6), (10), we obtain the effective inhomogeneity parameter

$$m_{ef}=\mu (T)\overline{m},\mu \frac{1}{2}\left(1+\sqrt{1\frac{T}{T_c}}\right)$$
(12)
where the temperature domain is bounded above by the characteristic temperature

$$T_c\left(\frac{\overline{m}}{2\sigma }\right)^2\mathrm{\Theta }.$$
(13)
According to Eq.(12) the effective mass decreases monotonously with increasing temperature from the bare magnitude $`\overline{m}`$ at $`T=0`$ to $`\overline{m}/2`$ at $`T=T_c`$.

The divergency condition of the Green function (9) arrives at the proper frequency of the oligomer alternation

$$\nu _0=\mathrm{i}\varpi \pm \omega $$
(14)
with imaginary and real parts

$$\omega ^2\omega _0^2\varpi ^2,\omega _0^2\frac{\tau }{m_{ef}},\varpi \frac{n_c}{2m_{ef}}.$$
(15)
Insertion of Eqs.(6), (12) gives the temperature dependence of the proper frequency

$$\omega ^2=\frac{\overline{\omega }_0^2}{\mu ^2}\left(\mu \frac{T_0^2}{T^2}\right)$$
(16)
where the bare frequency $`\overline{\omega }_0`$ and another characteristic temperature $`T_0`$ are introduced as follows:

$$\overline{\omega }_0^2\frac{\tau }{\overline{m}},T_0\frac{\mathrm{\Theta }}{2\sqrt{\overline{m}\tau }}.$$
(17)
As a result, combination of Eqs.(1), (16) leads to the final result

$$L=2l+\frac{\mu (T)}{\sqrt{\mu (T)T_0^2/T^2}}L_0$$
(18)
where the characteristic length, $`L_0`$, is defined as

$$L_0\frac{D_0}{\overline{\omega }_0}\sqrt{\frac{\overline{m}}{\tau }}b.$$
(19)
## IV Discussion

The behavior of the system is determined by the relation

$$\kappa =\frac{T_c}{T_0}\frac{\sqrt{\overline{m}\tau }}{2}\left(\frac{\overline{m}}{\sigma }\right)^21$$
(20)
where the minimal magnitude $`\kappa =1`$ fixes the choice of the theory parameters according to the condition: $`\sigma 2^{1/2}\overline{m}^{5/4}\tau ^{1/4}`$. It would seem from Eq.(20) that the decrease of the temperaure $`T_c`$ with weakening interaction when passing from the ionically bonded system (such as P4VP-(DBSA)x) to the hydrogen bonded one (e.g., P4VP–(PDP)x) is caused only by the growth of the fluctuation parameter $`\sigma `$ with respect to the mean magnitude of the inhomogeneity parameter $`\overline{m}`$. It appeares, however, that the main reason for such behavior is a decrease of the mean–geometrical magnitude $`\sqrt{\overline{m}\tau }`$ of the principle coefficients in the generic Lagrangian (3).

To clarify this problem, assume the three–parametric $`x`$–dependencies for the above parameters

$$\overline{m}=m_0+Ax(x_mx),\tau =\tau _0+Bx(x_\tau x)$$
(21)
with positive constants $`m_0`$, $`\tau _0`$, $`A`$, $`B`$, $`x_m`$, $`x_\tau `$. In limiting case, $`\kappa 1`$ relevant to the ionically bonded systems, when $`m_{ef}\overline{m}`$, $`\mu (T)1`$, the temperature $`T_c`$ is so large that the temperature dependence (18) takes the form

$$L=2l+\frac{L_0}{\sqrt{1T_0^2/T^2}},L_0\sqrt{\frac{\overline{m}}{\tau }}b.$$
(22)
Then, fitting of the experimental data shown in Figure 2 according to Eq.(22) arrives at the following results. The system P4VP-(DBSA)x: $`m_0=49`$, $`A=21`$, $`x_m=0.5`$; $`\tau _0=1`$, $`B=1.1`$, $`x_\tau =0.5`$; $`b=1`$ nm; $`l=10`$ nm. The system P4VP-(Zn(DBS)2)x: $`m_0=18`$, $`A=55`$, $`x_m=1.8`$; $`\tau _0=1`$, $`B=0.1`$, $`x_\tau =2`$; $`b=1`$ nm; $`l=10`$ nm. Respectively, for $`x=1`$ Eq.(20) gives values $`\kappa =10^3,10^2`$ at ratios $`\sigma /\overline{m}0.045,0.203`$.

A much more complicated situation occurs in hydrogen bonded system P4VP–(PDP)x, where the reduction of the parameter (20) leads to a more narrow temperature domain $`T_0÷T_c`$. As a result, the temperature dependence of the period $`L(T)`$ obtains a more complicated form (18) which keeps the decreasing character as shown in Figures 3 and 4. The dependence $`L(x)`$ at a fixed temperature may be described by the estimation

$$L2l+\sqrt{\overline{m}/\tau }b$$
(23)
following from Eq.(18) and conditions $`\mu 1`$, $`T_0T`$. Then, the experimental data shown in Figure 3 give the following constrains: $`\sqrt{m_0/\tau _0}=33.5`$, $`B/\tau _0=1.6`$, $`x_\tau =3.1`$. Respectively, the comparison of the experimental data shown in Figure 4 with the fitting results using Eqs.(12), (13), (17) and (18) yields $`\mathrm{\Theta }/\sqrt{m_0\tau _0}=1517`$, $`l=8.7`$ nm. Finally, Figure 5 and Eq.(13) give $`A/m_0=0.16`$, $`x_m=1.6`$, $`\mathrm{\Theta }m_0^2/4\sigma ^2=276`$.

As a result, taking $`m_0=1`$ at $`x=1`$ the magnitudes $`A=0.16`$, $`\mathrm{\Theta }=5.5`$, $`\sigma =0.07`$ are obtained and they provide the value of $`\tau _0`$ smaller than $`10^3`$ which arrive at the parameter $`\kappa 6.7`$ and ratio $`\sigma /\overline{m}=0.069`$. It is worth to mention that the value of the parameter $`\tau _0<10^3`$ is extremally small that guarantees the validity of the Flory–Huggins approach.

To conclude, the model desribed above can explain successfully all peculiarities obtained experimentally for various homopolymer–oligomer mixtures with interaction of different strength.

Acknowledgement In this work, financial support by the Grant Agency of the Czech Republic (grant GAČR 203/02/0653) is gratefully acknowledged.


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# References

The critical temperature of nuclear matter and fragment distributions in multifragmentation of finite nuclei.

R. Ogul1,2 and A.S. Botvina1,3

1Gesellschaft fur Schwerionenforschung, D–64291 Darmstadt, Germany.

2Department of Physics, University of Selcuk, 42079 Kampus, Konya, Turkey.

3Institute for Nuclear Research, Russian Academy of Science, 117312 Moscow, Russia.

## Abstract

The fragment production in multifragmentation of finite nuclei is affected by the critical temperature of nuclear matter. We show that this temperature can be determined on the basis of the statistical multifragmentation model (SMM) by analyzing the evolution of fragment distributions with the excitation energy. This method can reveal a decrease of the critical temperature that, e.g., is expected for neutron-rich matter. The influence of isospin on fragment distributions is also discussed.

PACS numbers: 25.70.Pq, 21.65.+f

Properties of nuclear matter have been under investigation for several decades (see e.g. ). Besides their general interest for nuclear physics, these studies are very important for our understanding astrophysical objects, such as neutron stars. The information about nuclear matter in its ground state and at low temperatures is usually obtained as a theoretical extrapolation, based on nuclear models designed to describe the structure of real nuclei.

It is instructive to investigate the thermodynamical properties of neutron–rich matter under extreme conditions of low densities and high temperatures. This situation is expected, for example, at supernova II explosions and during the formation of neutron stars. We believe that the liquid-gas type phase transition is manifested, in this case, in the forms of instabilities leading to fragment production. The models used for extracting nuclear matter properties in the phase transition region should be capable of describing the disintegration of homogeneous matter into fragments. It is also important that they should allow to be tested in nuclear reactions leading to the total disintegration of real nuclei at high excitation energy. The multifragmentation reactions, which started to be investigated experimentally nearly 20 years ago (see reviews ), suit perfectly for this purpose.

Naturally, a thermodynamical model involved in this kind of analysis has to include the ingredients necessary for the description of nuclear matter and to provide a good reproduction of experimental data. So far, the statistical multifragmentation model (SMM)  satisfies these requirements. The SMM has been designed to describe fragmentation and multifragmentation of excited finite nuclei . It includes a liquid-drop approximation for individual fragments which corresponds to the liquid-drop description of nuclear matter . This is an essential difference of the SMM from other multifragmentation models, e.g. , which do not take the nuclear matter properties explicitly into account. Examples of very successful applications of the SMM for the description of different experimental data can be found in \[3,9–17\]. Furthermore, the descriptions of data with statistical models confirm that multifragmentation of nuclei, despite of being a very fast process, proceeds under a high degree of thermalization.

Details of the SMM can be found in , here we concentrate on parts of the model which are important for the following discussion. The model describes the fragment formation at a low-density freeze-out ($`\rho \stackrel{<}{}\mathrm{\hspace{0.17em}1}/3\rho _0`$, $`\rho _00.15`$fm-3 is the normal nuclear density), where the nuclear liquid and gas phases coexist. The SMM phase diagram has already been under intensive investigations (see e.g. Ref. ). The liquid-drop approximation suggests that the fragmentation process is accompanied by an increase of the surface of nuclear drops. The surface entropy contributes essentially to the statistical partition sum. We should point out that the surface free energy depends on the ratio of the temperature $`T`$ to the critical temperature of nuclear matter $`T_c`$. In the SMM the surface tension $`\sigma (T)`$ is given by

$$\sigma (T)=\sigma (0)\left(\frac{T_c^2T^2}{T_c^2+T^2}\right)^{5/4}.$$
(1)
This formula is obtained as a parameterization of the calculations of thermodynamical properties of the interface between two phases (liquid and gas) of nearly symmetric nuclear matter, which were performed with the Thomas–Fermi and Hartree–Fock methods by using the Skyrme forces . In addition the scaling properties in the vicinity of the critical point (see ) were taken into account. At the critical temperature $`T_c`$ for the liquid-gas phase transition, the isotherm in the phase diagram has an inflection point. The surface tension vanishes at $`T_c`$ and only the gas phase is possible above this temperature. We emphasize that our analysis is based on this general effect and that our conclusions will remain qualitatively true in the case of other parametrizations satisfying this condition. This surface effect provides an effective way to study the influence of $`T_c`$ on fragment production in the multi-fragment decay of hot finite nuclei.

As was established by numerous studies (see e.g. \[3–5,9,15,16\]) the mass (charge) distribution of fragments produced in the disintegration of nuclei evolves with the excitation energy. At low temperatures ($`T\stackrel{<}{}\mathrm{\hspace{0.17em}5}`$ MeV), there is a so-called $`U`$-shape distribution corresponding to partitions with few small fragments and one big residual fragment. This distribution looks like a result of an evaporative emission. At high temperatures ($`T\stackrel{>}{}\mathrm{\hspace{0.17em}6}`$ MeV) the big fragments disappear, and there is an exponential-like fall of the mass distribution with mass number $`A`$. In the transition region $`T56`$ MeV, however, there is a smooth transformation of the first distribution into the second one. The mass distribution of intermediate mass fragments (IMFs, fragments with $`A=540`$) can be approximated by a power law $`A^\tau `$ . The $`\tau `$ parameter decreases with the temperature, goes through the minimum at $`T56`$ MeV, and then increases again. The small values of $`\tau `$ indicate that the probability for survival of the biggest fragment decreases drastically with the temperature. This behavior may be associated with a phase transition in finite systems. It has been shown in many studies (see e.g.  and references therein), that there are numerous peculiarities in this region, such as a plateau-like behavior of the caloric curve, large fluctuations of the temperature and of the number of the produced fragments, scaling laws for fragment yields, and other phenomena expected for critical behavior. Therefore, the temperature characterizing these phenomena is sometimes called the critical temperature for finite systems, and $`\tau `$ is considered as one of the critical exponents. The SMM can describe the critical behavior observed in the experiments \[15–17\]. However, in the present work we use the $`\tau `$ parametrization only for the characterization of shapes of the fragment mass distributions. In order to avoid any confusion with the standard definition of the critical temperature for nuclear matter, we note, in the following, the temperature corresponding to the critical phenomena as a break-up temperature for the disintegration of finite nuclei .

The decrease of the surface energy with increasing $`T/T_c`$ (see formula (1)) influences the fragment production and, therefore, can be observed in the fragment distributions. In this paper we show that this effect can be used for the evaluation of $`T_c`$ by finding the minimum $`\tau `$ parameter $`\tau _{min}`$ and the corresponding temperature $`T_{min}`$. The physics behind the phenomenon is quite transparent: If the contribution of the surface energy is rapidly decreasing, a nucleus prefers to disintegrate into small fragments already at low temperatures. Simultaneously, fluctuations of size of the fragments increase considerably. As a result the mass distribution becomes flatter in the transition region, and this leads to a decrease of $`\tau `$.

The SMM calculations were carried out for the $`Au`$ nucleus ($`A_0`$=197, $`Z_0`$=79) at different excitation energies and at a freeze-out density of one-third of the normal nuclear density. This choice is justified by the previous descriptions of the experimental data obtained for peripheral collisions \[9,12–16\]. Below we present results as a function of both the temperature and the excitation energy, since they are related quantities .

We have started by using the standard value of the critical temperature implemented in the SMM, $`T_c`$=18 MeV. This value is consistent with many theoretical studies . In Fig. 1 we show typical mass and IMF charge distributions, $`N_AA^\tau `$ and $`N_ZZ^{\tau _z}`$, at an excitation energy $`E_x`$=7 MeV/nucleon. One can see from this figure that the extracted $`\tau `$ and $`\tau _z`$ values are very close to each other, since the neutron-to-proton ratio of produced IMFs changes very little within their narrow charge range . As seen from Fig. 2, the dependences of these parameters versus excitation energy are nearly the same. The parameters obtained for primary hot fragments (excited nuclear matter drops) and after their secondary de-excitation (measured cold fragments) are also shown in this figure. One can see that the difference between the two cases is smallest around the minimum $`\tau `$ parameter. Therefore, the $`\tau _{min}`$ point is weakly affected by secondary processes.

The critical temperature reflects the properties of nuclear matter, however, these properties depend on the composition of this matter. For example, $`T_c`$ tends to decrease for neutron rich matter . As it was discussed by many authors, see e.g. , the critical temperature can be traced back towards neutron rich matter by studies of the disassembly of nuclei far from stability. We consider $`T_c`$ as a free parameter in the SMM and analyze how $`\tau `$ and the break-up temperature can change. In Fig. 3 we show the results for $`T_c=`$10 and 30 MeV. In these cases the evolution of $`\tau `$ with the excitation energy is similar to the one shown in Fig. 2. However, the values of $`T_{min}`$ and $`\tau _{min}`$ are essentially different. This reflects a considerable change of masses for the dominating fragments. These values are plotted in Fig. 4 versus the critical temperature. It is seen that both parameters increase with $`T_c`$ and that they tend to saturate at $`T_c\mathrm{}`$ corresponding to the case of the temperature-independent surface. This behavior is expected, since in this case only the translational and bulk entropies of fragments, but not the surface entropy, influence the probability for the fragment formation.

In the case of neutron-rich matter, the contribution of the symmetry energy increases considerably. It is necessary to take into account the standard dependence of the $`\tau `$ parameter on the isospin of the source, while searching for $`T_c`$. We performed SMM calculations of multifragmentation of $`{}_{}{}^{124}Sn`$ and $`{}_{}{}^{124}La`$ nuclei, which can be used in experiments , and compare them with the results obtained for $`Au`$ nuclei. This $`Sn`$ nucleus is nearly as neutron-rich as the gold nucleus, while the $`La`$ nucleus is neutron-poor. We have used the same model parameters as for the $`Au`$ case, with the standard $`T_c=`$18 MeV. It is seen from Fig. 5 that the neutron-poor source results in slightly lower microcanonical temperatures in the transition region ($`E_x35`$ MeV/nucleon). In Fig. 5 we show also the evolution of the $`\tau `$ parameter with the excitation energy. The results for $`Au`$ and $`Sn`$ are very similar and different from those obtained for the $`La`$. One can conclude, that IMF distributions approximately scale with the size of the sources, and that they depend on the neutron-to-proton (N/Z) ratios of the sources. This is because the symmetry energy still dominates over the Coulomb interaction energy for these intermediate-size sources. One can see from Fig. 5 that the source with the lower N/Z ratio leads to smaller $`\tau `$ parameters, i.e. to the flatter fragment distribution. We can explain this as an effect of the isospin (i.e. the symmetry energy) on fragment formation: A high N/Z ratio of the source favors the production of big clusters, since they have a large isospin. Therefore, in the transition region, partitions consisting of small IMFs and a big cluster dominate. This leads to a very prominent U-shape distribution with large $`\tau `$. When the N/Z ratio is low, the probability for a big cluster to survive is small and the system can disintegrate into IMFs, which have a favorable isospin in this case. The dominant fragment partitions tend to include IMFs of different sizes, and the fragment distribution is characterized by small $`\tau `$. Since the difference in the $`\tau `$ parameters between the neutron-rich and neutron-poor sources is quite large, it can be easily identified. The evolutions of fragment mass distributions caused by decreasing $`T_c`$ and changing N/Z ratio can interfere and, therefore, the influence of the critical temperature can be separated only after the comparison of experimental data with calculations.

In view of these theoretical findings it is instructive to demonstrate the possibility of the application of such an approach for the analysis of experimental data. Presently, there are several experimental analyses aimed at the extraction of the critical exponent $`\tau `$ in reactions with $`Au`$ nuclei . Those methods are not equivalent to the one suggested above, however, they are related to the fragment distributions, and the critical exponents can be used for an estimation of $`\tau _{min}`$ and $`T_c`$. The extracted break-up excitation energies $`E_x`$ vary within 3.8 to 4.5 MeV/nucleon, while $`\tau `$ is in the range from 2.12 to 2.18. As seen from Figs. 2 and 3, for $`T_c`$ 18, at these excitation energies $`\tau `$ is larger than $`\tau _{min}`$. We have performed an interpolation of the SMM calculations for the Au sources and found that they fit the experimental values of $`E_x`$ and $`\tau `$ if $`T_c`$ is in the range between 18 and 22 MeV. We have also seen from our analysis that $`\tau _{min}`$ is lower than the extracted $`\tau `$ by around 15%. The $`T_c`$ estimated in this way is very close to the standard SMM parametrization. This conclusion is supported by the analyses of Refs. \[15–17\] showing that the standard SMM reproduces both the experimental critical exponents and other characteristics of produced fragments. It is interesting that in Ref.  a small critical exponent $`\tau `$ 1.88 is reported for multifragmentation of $`Kr`$ nuclei, which have N/Z ratios lower than $`Au`$ nuclei. This is an indication of the importance of the isospin effects, as discussed above. It is worth noting that recently a very close critical temperature ($`T_c16.6`$ MeV) was extracted from analysis of the break-up (”limiting”) temperatures in Ref. . It is also in agreement with the temperature $`T_c20`$ MeV obtained in the experiment of Ref. . However, it would be important to identify regular changes of $`T_c`$, which needs involving new sources with different isospins.

In summary, we have pointed out that within the SMM the critical temperature of nuclear matter can influence the fragment production in multifragmentation of nuclei through the surface energy. We have suggested that this influence can be observed in the $`A^\tau `$ parameterization of the fragment yields by finding the minimum $`\tau `$ parameter. In the experiments the measured values of the parameters are consistent with the standard SMM assumption and slightly higher values of the critical temperature, $`T_c1822`$ MeV. The SMM predicts that variations of $`\tau _{min}`$ are especially large in the region of low $`T_c`$. Therefore, there is a possibility to investigate the decrease of $`T_c`$ for nuclear matter under extreme conditions, by studying the evolution of $`\tau _{min}`$ and $`T_{min}`$ in the multifragmentation of finite nuclei. This could be realized in the case of the neutron-rich nuclei delivered by current accelerators with radioactive heavy-ion beams . The isospin of the source influences also the fragment production through the symmetry energy. We have demonstrated how the isospin affects the fragment distributions, that should be taken into account in these studies.

The authors thank GSI for hospitality and support. We appreciate stimulating discussions with V.A.Karnaukhov and I.N.Mishustin. We are very indebted to W. Trautmann and J. Lukasik for discussions and help in preparation of the manuscript. R. Ogul acknowledges financial support of TUBITAK-DFG cooperation.

Figure captions

Fig.1: Average fragment mass and charge yields $`N_A`$ and $`N_Z`$, after multifragmentation of $`Au`$ nuclei at an excitation energy of 7 MeV/nucleon. Solids lines are $`A^\tau `$ and $`Z^{\tau _z}`$ fits of the IMF yields.

Fig.2: Evolution of $`\tau _z`$ (top panel) and $`\tau `$ (bottom panel) parameters with the excitation energy $`E_x`$ of $`Au`$ sources calculated with the standard SMM parameterization. The open circles are for hot primary fragments and the full squares are for observed cold fragments.

Fig.3: Evolution of $`\tau `$ parameters in the SMM for cold fragments with the excitation energy $`E_x`$. The top panel is for the critical temperature $`T_c`$=10 MeV, the bottom panel for $`T_c`$=30 MeV.

Fig.4: The minimum $`\tau _{min}`$ parameter for cold fragments (top panel) and the corresponding temperature $`T_{min}`$ (bottom panel) as function of the critical temperature $`T_c`$ of nuclear matter.

Fig.5: The temperature (top panel) and $`\tau `$ parameters for cold fragments (bottom panel) versus excitation energy in multifragmentation. The solid, dashed and dotted lines are SMM calculations performed for sources with different sizes or isospin (see the figure) with the standard $`T_c`$=18 MeV.


text:
# Upper Bounds for the Number of Quantum Clones under Decoherence

## 1 Introduction

Although the “no-cloning theorem” by Wootters and Zurek  states that it is impossible to copy arbitrary quantum information perfectly, quantum mechanics does allow us to make approximate copies. Since Bužek and Hillery first presented a unitary transformation, known as a universal quantum cloning machine (UQCM), to make two identical approximate copies of an input qubit , the subject of quantum cloning has been investigated intensely (for example, see ) and experiments have recently been carried out .

One application of quantum cloning is in quantum computation, as copying is a fundamental process in information processing. It has been shown that there are some quantum-computational tasks whose performance can be enhanced by making use of quantum cloning . However, physical realizations of quantum circuits are always fraught with difficulties due to decoherence, as it is virtually impossible to isolate a quantum system from its environment perfectly.

Here, we investigate the circuit complexity of universal quantum cloning and estimate the time $`T`$ a quantum cloning machine requires to make $`M`$ copies of $`N`$ identical pure state inputs. By comparing $`T`$ with the decoherence time $`\tau _{\mathrm{dec}}`$ of the qubits in a physical system, we can estimate how $`M`$ or $`N`$ will be restricted and how much quantum information can be copied practically. In order to estimate the decoherence time, one needs to model a specific realization, and several are possible: cavity QED, parametric down-conversion, and ion traps. To provide a concrete example, we examine an ion-trap realization of the UQCM network, and assume all instrumental sources of decoherence  have been eliminated, leaving us with spontaneous emission as a well-characterizable source of decoherence.

The analysis of the times $`T`$ and $`\tau _{\mathrm{dec}}`$ is analogous to that reported in , in which upper bounds are determined for the bit size $`L`$ of the number to be factorized by using Shor’s algorithm.

In the next section, we briefly review the ideas of quantum cloning, and then, in Section 3, count the number of elementary logical operations needed to build a quantum circuit for $`NM`$ cloning. In Section 4, we compare the cloning time $`T`$ with the decoherence time $`\tau _{\mathrm{dec}}`$ of the quantum circuit when it is implemented with trapped ions, as in . Other sources of decoherence (vibrational quanta damping, heating, inhomogeneous trap fields, and laser fluctuations) will also lead to limitations in the number of good quality copies such a UQCM can generate.

## 2 Quantum Cloning Transformation

The task of a general universal quantum cloning machine is to copy $`N`$ identical pure states, described as $`\rho ^{\mathrm{in}}=(|\psi \psi |)^N`$, into $`M`$-particle output states ($`M>N`$), $`\rho ^{\mathrm{out}}`$, with the following conditions:

1. The reduced density operators for any one of the $`M`$ outputs are identical to each other, i.e.,

$$\rho _i^{\mathrm{out}}=\rho _j^{\mathrm{out}},$$
(1)
where $`\rho _i^{\mathrm{out}}`$ is a reduced density operator with respect to the $`i`$-th particle.
2. The quality of the copies does not depend on the input states, i.e. the fidelity between the input and the output states is independent of the input state. The fidelity $`F`$ is defined by $`F=\psi |\rho _i^{\mathrm{out}}|\psi `$. The word “universal” refers to this condition.
3. The copies are as close as possible to the input state as a natural requirement for a cloning machine. Thus, the fidelity $`F`$ should be as close as possible to 1.

Here, we consider only a two-dimensional system (qubit) as a physical system, as systems of higher dimension are beyond the scope of current candidates for the realizations of quantum circuits.

The cloning transformation of Bužek and Hillery  makes two copies from one original qubit. It is written as

$`|0_a|0_b|0_x`$ $``$ $`\sqrt{{\displaystyle \frac{2}{3}}}|0_a|0_b|0_x+\sqrt{{\displaystyle \frac{1}{6}}}(|0_a|1_b+|1_a|0_b)|1_x`$
$`|1_a|0_b|0_x`$ $``$ $`\sqrt{{\displaystyle \frac{2}{3}}}|1_a|1_b|1_x+\sqrt{{\displaystyle \frac{1}{6}}}(|0_a|1_b+|1_a|0_b)|0_x.`$ (2)
In Eq. (2), the first qubit with subscript $`a`$ is the state to be copied, the second one labelled $`b`$ is the blank paper that becomes one of the copies after the process, and the qubit with $`x`$ is an ancilla bit which can be regarded as the state of the machine. The fidelity of this process is found to be $`\frac{5}{6}`$, which is independent of the input state, as desired.

Bužek et al. also presented a way to construct a quantum network for this UQCM  (Figure 1(a)). In Figure 1(a), R is a single qubit gate which rotates the basis vectors by an angle $`\theta `$ as

$`R(\theta )|0`$ $`=`$ $`\mathrm{cos}\theta |0+\mathrm{sin}\theta |1,`$
$`R(\theta )|1`$ $`=`$ $`\mathrm{sin}\theta |0+\mathrm{cos}\theta |1,`$ (3)
and $``$ and $``$ symbols connected with a line denote a controlled NOT gate (CNOT) with $``$ and $``$ as a control bit and a target bit, respectively. By adjusting the rotation angles of three single qubit gates, any two of the three states at the output represent copies of the qubit $`a`$.

Eq. (2) was generalized by Gisin and Massar  to produce $`M`$ copies out of $`N`$ inputs. This transformation is described by

$`U_{N,M}|N\psi |0^{2(MN)}`$ $`=`$ $`{\displaystyle \underset{j=0}{\overset{MN}{}}}\alpha _j|(Mj)\psi ,j\psi ^{}R_j(\psi ),`$ (4)
$`\alpha _j`$ $`=`$ $`\sqrt{{\displaystyle \frac{N+1}{M+1}}}\sqrt{{\displaystyle \frac{(MN)!(Mj)!}{(MNj)!M!}}},`$
$`R_j(\psi )`$ $`=`$ $`|(MNj)\psi ^{},j(\psi ^{})^{},`$
where $`|N\psi `$ is the input state consisting of $`N`$ qubits, all in the state $`|\psi `$. $`|(Mj)\psi ,j\psi ^{}`$ is the symmetric and normalized state with $`Mj`$ qubits in the state $`|\psi `$ and $`j`$ qubits in the orthogonal state $`|\psi ^{}`$. $`R_j(\psi )`$ represent the internal state of the machine and $`R_j(\psi )R_k(\psi )`$ holds for all $`jk`$.

## 3 Generic Quantum Cloning Circuit

Bužek et al. constructed a quantum circuit for $`1M`$ UQCM which explicitly realizes Eq. (4) by generalizing the corresponding circuit for the $`12`$ case . Figure 1(b) shows their circuit for $`1M`$ cloning machine. It is basically a natural extension of the $`12`$ circuit, consisting a preparation stage and a cloning (permutation) stage. Let us consider if it is possible to extend this $`1M`$ cloning circuit further to an $`NM`$ cloning circuit, by making up a circuit in Figure 2 in which the preparation stage is built up with both single and two qubit operations and the cloning stage is a sequence of CNOT or similar multi-qubit operation gates.

Eq. (4) gives us a few hints on the possible construction of the quantum circuit for an $`NM`$ UQCM. First, $`M1`$ qubits are necessary to represent the internal states of the machine. The total number of qubits needed to implement this transformation is $`2MN`$.

Second, every basis of the form of $`|(Mj)\psi ,j\psi ^{}`$ or $`R_j(\psi )`$ in Eq. (4) is a basis in the symmetrical subspace of the Hilbert space $`^M`$ or $`^{(MN)}`$, where $``$ is the space spanned by $`|0`$ and $`|1`$. Although the symmetrical subspace is a rather small subspace in the whole Hilbert space, almost all computational bases are involved in Eq. (4), especially when $`N`$ is small.

Therefore, almost $`2^{2MN}`$ amplitudes need to be distributed to appropriate computational bases to perform the transformation (4), although the number of distinct amplitudes, $`\alpha _j`$, is only $`MN+1`$. The fact that such a great number of amplitudes are necessary imposes a certain condition upon the values of $`N`$ and $`M`$ in order for an $`NM`$ cloning machine in Figure 2 to work properly.

Because the task of the cloning stage which consists of a sequence of CNOTs is to permute the amplitudes of all basis vectors which span the whole Hilbert space, all the amplitudes in Eq. (4), $`\alpha _j`$, must be provided by the preparation stage. Therefore, the preparation stage should be able to generate an entangled $`2(MN)`$-qubit state with a set of any real amplitudes that may appear in Eq. (4) by adjusting the rotation angles of each single qubit gate.

For example, in the $`12`$ UQCM (Eq. (2) and Figure 1(a)), the amplitudes appearing in the output states are $`\sqrt{\frac{2}{3}}`$, $`\sqrt{\frac{1}{6}}`$, and $`\sqrt{\frac{1}{6}}`$. Thus, the preparation stage needs to provide these three coefficients and it turns out that, with the configuration of the cloning stage of Figure 1(a), the two-qubit state emerging from the preparation stage should be

$$|\psi ^{\mathrm{prep}}=\sqrt{\frac{2}{3}}|00+\sqrt{\frac{1}{6}}|01+\sqrt{\frac{1}{6}}|11,$$
(5)
when the third qubit is used as the internal state of the machine. The rotation angles of the single qubit gates in this stage are determined accordingly.

However, this scheme only works when the number of distinct computational bases in Eq. (4) is smaller than the dimension of the Hilbert space that the preparation stage deals with. Otherwise, the preparation stage cannot generate enough amplitudes required by Eq. (4). This condition is written as

$$\underset{k=0}{\overset{MN}{}}\left(\genfrac{}{}{0pt}{}{M}{k}\right)\left(\genfrac{}{}{0pt}{}{MN}{k}\right)2^{2(MN)},$$
(6)
where the LHS represents the number of bases that appear in Eq. (4) and the RHS is the dimension of the Hilbert space where qubits in the preparation stage lie.

Eq. (6) is fulfilled for any $`M`$ when $`N=1`$, which is the case of Figure 1(b), and when $`N=2`$. Still, it becomes rather complicated when it comes to other combinations of $`N`$ and $`M`$. An example in which we can see the violation of Eq. (6) clearly is the case of $`2N=M`$, where the LHS of Eq. (6) for $`N1`$ can be estimated as

$$\underset{k=0}{\overset{N}{}}\left(\genfrac{}{}{0pt}{}{2N}{k}\right)\left(\genfrac{}{}{0pt}{}{N}{k}\right)=\left(\genfrac{}{}{0pt}{}{3N}{N}\right)\sqrt{\frac{3}{4\pi }}\left(\frac{27}{4}\right)^N\frac{1}{\sqrt{N}}.$$
(7)
This always exceeds the corresponding RHS of Eq. (6), $`2^{2N}`$. Nevertheless, Eq. (6) is satisfied for $`M`$ which are sufficiently large compared with $`N`$, since its LHS is approximately $`2^{2M1}/\sqrt{\pi M}`$, which is smaller than the RHS when $`M>\pi ^12^{4N2}`$.

Note that the condition (6) is not necessary if we are allowed to make use of more auxiliary qubits inside a cloning machine. Providing $`2MN`$ qubits at most, instead of $`2(MN)`$, enables the preparation stage to generate enough number of amplitudes for the cloning transformation. Then the cloning stage can complete the whole process by allocating those amplitudes to appropriate bases, leaving the auxiliary qubits disentangled, in state $`|0`$, from the legitimate $`2MN`$ output qubits. Introducing these auxiliary qubits does not affect the estimation of the number of gates, which is discussed in the following.

Let us now count the number of elementary gates in the quantum cloning circuit, especially CNOT gates, as a CNOT gate takes a longer time to be performed than a single qubit gate .

The preparation stage should be designed so that it generates an arbitrary set of real amplitudes whose number is written by the LHS of Eq. (6). As far as the quantum cloning transformation Eq. (4) is concerned, the amplitudes should not necessarily be arbitrary as they are specifically described as in Eq. (4). However, in order to keep the full “controllability” on the output states, as in the case of $`12`$ UQCM, we assume that the preparation stage can generate arbitrary superpositions of $`2^{d_{\mathrm{prep}}}`$ bases with real amplitudes, where $`d_{\mathrm{prep}}=2^{2(MN)}`$ is the dimension of the $`2(MN)`$-qubit Hilbert space.

The transformation that the preparation stage performs can be written as $`|00\mathrm{}0_{k=0}^{d_{\mathrm{prep}}1}c_k|k`$, where $`c_k`$ are real numbers complying with the normalization condition $`_kc_k^2=1`$. This is a unitary transformation which can be described by a $`d_{\mathrm{prep}}\times d_{\mathrm{prep}}`$ matrix, on the $`d_{\mathrm{prep}}`$-dimensional initial state vector $`(1,0,\mathrm{},0)^T`$, and its components are given by $`u_{m1}=c_m`$ and the rest of them are arbitrary for our purpose.

It is known that an outright circuit implementation of a $`d\times d`$ unitary matrix requires, in general, $`O(d^2(\mathrm{log}d)^2)`$ elementary operations . However, a more efficient circuit to create an arbitrary quantum superposition starting from $`|00\mathrm{}0`$ has been proposed in  and its complexity is given by $`O(d(\mathrm{log}d)^2)`$. Thus we simply take $`O(d_{\mathrm{prep}}(\mathrm{log}d_{\mathrm{prep}})^2)`$ as the number of CNOTs in the preparation stage of a UQCM in the following calculations.

The cloning stage is also generically hard to construct. The only exception we know of is the case of $`1M`$ UQCM, which can be realized by the circuit in Figure 1(b). In a more generic $`NM`$ case, we can build up a circuit as follows. As mentioned above, the cloning stage only permutes all bases with non-zero amplitudes among all computational bases of $`^{(2MN)}`$. Thus, we can estimate the number of gates with only the knowledge of number of bases involved, even if we have no information on the actual permutation, i.e. which basis goes to which.

Let us take the $`12`$ quantum cloning circuit as an example to simplify our description of its construction, although its efficient circuit is already given in Figure 1. Table 1 shows all the necessary permutations of bases to complete the transformation from Eq. (5) to Eq. (2). This permutation can be implemented as a circuit by carrying out each transformation one by one. Since $`|010`$ is not used in the preparation state, $`|101|010`$ should be performed first, otherwise any other destination state may be used as a preparation state later and thus the preceding transformation comes to naught. A basis which is exempted from being used in the preparation, such as $`|010`$ in this case, always exists in a more general $`NM`$ case as the equality in condition (6) never holds for $`N,M\mathrm{I}\mathrm{N}`$. Hence, the appropriate order of transformation is $`|101|010,|001|101,|111|001,|100|111,|001|100`$, where $`|001`$ is used as a buffer in the last three operations, as it is not used in the final state, to swap $`|100`$ and $`|111`$.

Figure 3 shows a general way to permute bases. In this figure, an unfilled circle, $``$, denotes a control bit in-between two NOT gates. Unlike a filled circle $``$, $``$ activates connected operations when the bit value at $``$ is $`0`$.

Here, an ancilla qubit is introduced in order to flip the incoming binary numbers according to the permutation required for a UQCM, as shown in Table 1. Finding a circuit for the basis permutation without ancillas is generally very hard, hence we make use of it here for convenience. The ancilla is prepared by the UQCM in a state $`|0`$ and it ends up in the same state $`|0`$ after the whole process. As the ancilla qubit is necessarily disentangled by the end of the process, we do not have to take it as a part of the output state.

In the earlier paragraph of this section, we have identified the generic features required of a copying circuit. For concreteness, it is important to show a specific example and in the following we do this for a $`24`$ cloner. Our circuit is not unique and other examples of course can be found.

The transformation of the state $`|00`$ by the $`24`$ quantum cloning can be written from Eq. (4) as

$`|00|0000`$ $``$ $`\sqrt{{\displaystyle \frac{3}{5}}}|0000|11`$ (8)
$`+\sqrt{{\displaystyle \frac{3}{80}}}(|0001+|0010+|0100+|1000)(|01+|10),`$
$`+\sqrt{{\displaystyle \frac{1}{60}}}(\stackrel{6\mathrm{bases}}{\stackrel{}{|0011+\mathrm{}+|1100}})|00,`$
and the transformation for $`|11|0000`$ can be obtained by flipping every bit in Eq. (8).

As mentioned earlier in this section, we need four qubits for the preparation stage in addition to two input qubits, thus, six qubits in total. The preparation stage generates all amplitudes for the 15 bases appearing in Eq. (8). The output from the preparation stage is, for example,

$`|0000|\psi ^{\mathrm{prep}}`$ $`=`$ $`\sqrt{{\displaystyle \frac{3}{5}}}|0000+\sqrt{{\displaystyle \frac{3}{80}}}(\stackrel{8\mathrm{bases}}{\stackrel{}{|0001+\mathrm{}+|1000}})`$ (9)
$`+\sqrt{{\displaystyle \frac{1}{60}}}(\stackrel{6\mathrm{bases}}{\stackrel{}{|1001+\mathrm{}+|1110}}).`$
The quantum circuit to carry out this transformation is given in  and is also depicted in Figure 4. The boxes represent a single qubit operation $`U_\theta `$ of the form

$$U_\theta =\left(\begin{array}{cc}\mathrm{cos}\theta & \mathrm{sin}\theta \\ \mathrm{sin}\theta & \mathrm{cos}\theta \end{array}\right),$$
(10)
and all $`\theta `$ in Figure 4 are given by

$$\theta _1=\mathrm{tan}^1\sqrt{\frac{11}{69}},\theta _{20}=\mathrm{tan}^1\sqrt{\frac{4}{19}},\theta _{21}=\mathrm{tan}^1\sqrt{\frac{4}{7}},$$

$$\theta _{30}=\mathrm{tan}^1\sqrt{\frac{2}{17}},\theta _{31}=\frac{\pi }{4},\theta _{32}=\mathrm{tan}^1\sqrt{\frac{8}{13}},\theta _{33}=\mathrm{tan}^1\frac{1}{\sqrt{2}},$$

$$\theta _{40}=\mathrm{tan}^1\frac{1}{4},\theta _{41}=\theta _{42}=\theta _{43}=\theta _{45}=\theta _{46}=\frac{\pi }{4},\theta _{44}=\mathrm{tan}^1\frac{2}{3},\theta _{47}=0,$$
(11)
One possible permutation of bases that achieves the transformation (8) from $`|\psi ^{\mathrm{prep}}`$ in Eq. (9) is shown in Table 2. This can be implemented by the quantum circuit in Figure 5. With the quantum circuits of Figures 4 and 5, the quantum cloning transformation (8) is carried out faithfully and the upper three qubits in Figure 5 will be the clones, while the next two qubits are the state of the cloner and the lowest disentangled qubit is an ancilla which can be discarded.

We can now estimate the number of CNOTs in the whole cloning circuit. In , the number of basic operations, i.e. single qubit operations and CNOTs, to simulate a multi-qubit controlled operation has been given as $`O(n^2)`$ for a controlled-$`U`$ gate with $`n1`$ control qubits and one auxiliary qubit. Therefore, the upper bound for the number of CNOTs in the cloning stage is the order of the number of bases involved, which is approximately twice of the number of amplitudes produced in the preparation stage, multiplied by the square of the number of qubits. As the number of the bases is given by the RHS of Eq. (6), $`O(2^{2M}M^{\frac{1}{2}})`$, and there are $`O(2^{2(MN)}(MN)^2)`$ CNOTs in the preparation stage, a quantum cloning circuit of the type of Figure 2 contains $`O(2^{2M}(MN)^2(2^{2N}+M^{\frac{1}{2}}))`$ CNOTs at most in total.

This circuit looks rather inefficient especially because of the preparation stage. The inefficiency comes partly from our requirement that the preparation stage should be able to generate arbitrary superpositions. If both $`N`$ and $`M`$ can be fixed and we do not have to control the parameters of each single qubit gate, the task of the preparation stage is much easier and the configuration of its circuit may well be much simpler and more efficient.

The cloning stage is also inefficient due to the complexity of the network for a general permutation. Despite the linear dependence on $`M`$ in the case of $`1M`$ UQCM, the number of CNOTs grows exponentially as $`M`$ increases when there are $`N`$ inputs, since each permutation is done one by one in our circuit. It might be possible to find a more efficient circuit, however, we have not succeeded.

## 4 Decoherence Time and Cloning Time

With the number of CNOT gates estimated in the previous section, we can now compare the cloning time $`T`$ with the decoherence time $`\tau _{\mathrm{dec}}`$. We focus on a quantum computing realization which makes use of cooled trapped ions . In the following, we assume that spontaneous emissions are the only source of decoherence, and we only discuss the process without error correction codes. Going beyond these constraints will be discussed elsewhere.

The Hamiltonian operator for a two-level ion of mass $`m`$, interacting with a phonon as a result of the centre-of-mass (c.m.) motion with frequency $`\nu `$, is then given by ,

$$H=\frac{\eta }{\sqrt{2MN}}\frac{\mathrm{\Omega }_1}{2}[|10|a+|01|a^{}],$$
(12)
where $`\eta =(2\pi /\lambda )\sqrt{\mathrm{}/2m\nu }`$ is the Lamb-Dicke parameter, $`\mathrm{\Omega }_1`$ is the Rabi frequency of the $`01`$ transition with 0 and 1 denoting the ground and the excited states of the ion. The $`a`$ and $`a^{}`$ are the annihilation and creation operators of the phonon. As in the original proposal , we assume that qubits are encoded in the internal state of ions and the phonons are used as the information bus. The denominator $`\sqrt{2MN}`$ is a consequence of the fact that an $`NM`$ UQCM network needs $`2MN`$ qubits (ions).

The elementary time step for a CNOT gate with this system can be written as

$$\tau _{\mathrm{el}}\frac{4\pi \sqrt{2MN}}{\eta \mathrm{\Omega }_1}.$$
(13)
The total processing time for cloning is

$$T\frac{4\pi \sqrt{2MN}}{\eta \mathrm{\Omega }_1}ϵ2^{2M+2}(MN)^2\left(\frac{1}{2^{2N}}+\frac{1}{\sqrt{\pi M}}\right),$$
(14)
where $`ϵ`$ is a some proportion factor. Here, we use the number of CNOTs in the preparation stage, because it is usually dominant over that of CNOTs in the cloning stage, as mentioned above. Also, we assume that all the CNOTs are performed sequentially one by one, despite the possibility of building up a circuit which performs several operations in parallel. Thus, the discussion below gives only a naive upper bound for the number of cloneable qubits. To minimize $`T`$, we wish to increase the value for $`\mathrm{\Omega }_1`$, which is related to the decay rate of the excited state by

$$\frac{\mathrm{\Omega }_1^2}{\mathrm{\Gamma }_1}=\frac{6\pi c^3ϵ_0}{\mathrm{}\omega _1^3}E^2,$$
(15)
where $`E,c,ϵ_0`$, and $`\omega _1`$ are the electric field strength of the laser, the speed of light, the permittivity of vacuum, and the transition frequency between the states 0 and 1, respectively. Clearly, we would like to minimize the decoherence effects of $`\mathrm{\Gamma }_1`$ by going to a metastable level, but then $`\mathrm{\Omega }_1`$ is also small. We can increase the Rabi frequency $`\mathrm{\Omega }_1`$ by increasing the electric field strength of the laser $`E`$, but it would then cause transitions to other higher levels which may be more rapidly decaying than state 1, and eventually spontaneous emissions which destroy the coherence of the system. Let $`|2`$ represent all other auxiliary levels which are coupled to the ground state $`|0`$.

As a stronger laser increases the population in the auxiliary level, it increases the rate of spontaneous emissions from level 2. Thus, we compute the probability of an emission from either level 1 and 2, and then minimize this probability to have an intensity-independent limit to the number of output qubits under the effect of spontaneous emission .

The probability of a spontaneous emission from the upper level of the qubit during the cloning process is

$$p_{10}=\frac{1}{2}2\mathrm{\Gamma }_1(2MN)T.$$
(16)
The factor $`\frac{1}{2}`$ is present because we can assume that on average half of the qubits are in the upper level during the whole cloning period $`T`$. Because the auxiliary level is populated only when interacting with the laser, the probability of a spontaneous emission from level 2 is written as

$$p_{20}=\frac{\mathrm{\Omega }_2^2}{8\mathrm{\Delta }_2^2}2\mathrm{\Gamma }_2T,$$
(17)
where $`\mathrm{\Delta }_2`$ is the detuning between the frequency of the laser and that of the transition $`01`$. We now obtain the total probability of spontaneous emission

$`p_{\mathrm{total}}`$ $`=`$ $`p_{10}+p_{20}`$ (18)
$`=`$ $`{\displaystyle \frac{4\pi ϵ\sqrt{(2MN)^3\mathrm{\Gamma }_1}}{\eta }}2^{2M+2}(MN)^2\left({\displaystyle \frac{1}{2^{2N}}}+{\displaystyle \frac{1}{\sqrt{\pi M}}}\right)`$
$`\times \left[{\displaystyle \frac{1}{x}}+{\displaystyle \frac{1}{2MN}}\left({\displaystyle \frac{\omega _1}{\omega _2}}\right)^3{\displaystyle \frac{\mathrm{\Gamma }_2^2}{4\mathrm{\Delta }_2^2\mathrm{\Gamma }_1}}x\right],`$
where $`x=\mathrm{\Omega }_1/\sqrt{\mathrm{\Gamma }_1}`$ and we used

$$\frac{\mathrm{\Omega }_1^2}{\mathrm{\Gamma }_1}=\left(\frac{\omega _2}{\omega _1}\right)^3\frac{\mathrm{\Omega }_2^2}{\mathrm{\Gamma }_2},$$

which is derived from Eq. (15). The minimum value of $`p_{\mathrm{total}}`$ with respect to $`x`$ is

$$p_{\mathrm{min}}=\frac{\pi ϵ}{\eta }\left(\frac{\omega _1}{\omega _2}\right)^{\frac{3}{2}}\frac{\mathrm{\Gamma }_2}{\mathrm{\Delta }_2}2^{2M+4}(2MN)(MN)^2\left(\frac{1}{2^{2N}}+\frac{1}{\sqrt{\pi M}}\right).$$
(19)
In order for the cloning process to be successful, $`p_{\mathrm{min}}`$ should be very small compared with unity. This requirement gives the upper bound on $`M`$ for a given $`N`$ in the expression of

$`2^{2M_{\mathrm{max}}}(2M_{\mathrm{max}}N)(M_{\mathrm{max}}N)^2\left({\displaystyle \frac{1}{2^{2N}}}+{\displaystyle \frac{1}{\sqrt{\pi M_{\mathrm{max}}}}}\right)`$
$`{\displaystyle \frac{\eta }{2^4\pi ϵ}}\left({\displaystyle \frac{\omega _2}{\omega _1}}\right)^{\frac{3}{2}}{\displaystyle \frac{\mathrm{\Delta }_2}{\mathrm{\Gamma }_2}}.`$ (20)
Table 3 shows the results of the actual calculations of the RHS of Eq. (4) for those ions often utilized in trap experiments along with their numerical data. Assuming $`ϵ=100`$ , $`\eta =0.01`$ and $`\mathrm{\Delta }_2=10^{13}[s^1]`$, we find that Eq. (4) has no solutions for $`M2`$ as the LHS of Eq. (4) is equal to 31.2 when $`N=1`$ and $`M=2`$. However, if we consider only the $`12`$ cloning network, where the number of CNOTs is six according to Figure 1(a), the probability of spontaneous emission during the whole process becomes rather small. For example, $`p_{\mathrm{min}}=0.062`$ for $`\mathrm{Ca}^+`$ and $`p_{\mathrm{min}}=0.017`$ for $`\mathrm{Ba}^+`$, therefore the cloning may be successful.

Overall, we see that even for a small number of outputs copied from one input the decoherence due to spontaneous emissions plays a critical role. If we make an optimistic assumption for $`\eta `$, as $`\eta =1.0`$, $`12`$ cloning with $`\mathrm{Ca}^+`$, $`12`$ and $`23`$ with $`\mathrm{Ba}^+`$ would become possible.

If we are allowed to have one more auxiliary qubit, the number of basic operations to simulate a $`(n2)`$-controlled operation can be reduced from $`O(n^2)`$ to $`O(n)`$ . Replacing the corresponding factors in the above calculations shows that, with $`\eta =1.0`$, $`12`$, $`13`$, and $`23`$ cloning may be possible with $`\mathrm{Ba}^+`$ as well as $`12`$ and $`13`$ cloning with $`\mathrm{Ca}^+`$.

## 5 Summary

We have first investigated a possible method to construct an $`NM`$ quantum cloning circuit in order to estimate the number of CNOT gates in it. We have estimated the number of CNOTs as $`O(2^{2M}(MN)^2(2^{2N}+M^{\frac{1}{2}}))`$, with $`N`$ and $`M`$ the numbers of input and output qubits, respectively. Therefore, the number of gates in the quantum cloning circuit of the type of Figure 1(b) or Figure 2 is always exponential with respect to the number of output qubits.

With the circuit complexity we obtained, it has been shown that the quantum cloning may be implemented by using the system of trapped ions for only a few combinations of small $`N`$ and $`M`$, when the system is not immune to decoherence due to spontaneous emissions, provided sophisticated quantum error correction codes are not used. As spontaneous emissions are the only source of decoherence we have considered here, the number of possible combinations of $`N`$ and $`M`$ might be lowered further by taking into account of other effects, such as phonon decoherence , the random phase fluctuations of the lasers, the heating of the ions’ vibrational motion .

Nevertheless, unlike the case of factorization by Shor’s algorithm , producing many clones is not necessarily what we expect from the quantum cloning. Since even a few copied qubits may be useful in quantum information processing , our results should not be interpreted too pessimistically. Furthermore, the use of quantum error correction codes will surely ease the condition for upper bounds.

In , it was shown that a quantum information distributor, which is a modification of the quantum cloning circuit, can be used as a universal programmable quantum processor in a probabilistic regime. From this point of view, our estimation on the upper bound for the clones implies physical bounds on the realization of such a processor with trapped ions.

One interesting subject we have not considered here is the effect of decoherence on the quality of the clones. If we allow a processing time which is longer than the decoherence time, the fidelity between the input and output states will surely be lower than what we expect from Eq. (4). We might be able to find a tradeoff between the fidelity and the number of cloneable qubits to have “useful” clones in terms of practical quantum information processing.

## Acknowledgement

We are very grateful to V. Bužek for a careful reading of the manuscript and helpful suggestions. This work was supported in part by the European Union IST Network QUBITS. K.M. acknowledges financial support by Fuji Xerox Co., Ltd. in Japan.