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# The pulling force of a single DNA molecule condensed by spermidine

## Abstract

In a recent experiment, a single DNA double helix is stretched and relaxed in the presence of spermidine, a short positive polyelectrolyte, and the pulling force is measured as a function of DNA extension. In a certain range of spermidine concentration, a force plateau appears whose value shows maximum as a function of spermidine concentration. We present a quantitative theory of this plateau force based on the theory of reentrant condensation and derive almost parabolic behavior of the plateau force as a function of the logarithm of the spermidine concentration in the range of condensation. Our result is in good agreement with experimental data.

DNA condensation by strongly positively charged proteins, histones, is used by nature for compaction of DNA in cell nucleus (DNA is strongly negatively charged). Positive proteins, protamines, are used for additional compaction of DNA in the sperm cell . Gene therapy uses complexes of DNA with long positive polyelectrolytes or other macrocations. The net charge of these complexes can be positive and therefore they are not repelled by negative cell membrane in the course of gene delivery. Thus, condensation of DNA by positive macrocations is an extremely important physical phenomenon. It is intensively studied in the model system of double helix DNA with spermidine, a flexible polymer with length $`15`$ $`\AA `$ and charge $`+3`$. It is known that in a dilute DNA solution at some concentration of spermidine, $`s=s_c`$, each long DNA molecule self-condenses into a toroid Bloomfield0 . When $`s`$ grows farther, at a much larger concentration, $`s=s_d`$, DNA dissolves back Experiments . This phenomenon is called reentrant condensation and has got theoretical explanations Olvera ; Rouzina .

Recently, a new single molecule technique has been used to measure the force necessary to pull a single DNA double helix from a toroidal condensate of DNA Murayama  (Fig. 1). In the experiment, extremely small concentration of DNA (2 nM of nucleotides) is dissolved in water with certain concentrations of spermidine (varying from 200 $`\mu `$M to 200 mM). Dual-trap tweezers are used to stretch a single DNA molecule tethered between two protein-coated polystyrene beads. DNA is first stretched and then relaxed. During these processes, the pulling force $`f`$ is measured. Experiments are repeated at various spermidine concentrations. It is observed that in the interval $`s_c<s<s_d`$, there is a fairly large range of DNA extension, $`x`$, where force $`f`$ is significantly larger than the force described in the wormlike chain model Marko . Moreover, in this range of $`x`$, $`f`$ is almost a constant (a force plateau, see Fig. 2). The plateau value of the force, $`f_p`$, is plotted as a function of $`s`$ in Fig. 3.

In this paper, we suggest a quantitative theory of the $`f_p(s)`$ curve based on the theory of reentrant condensation Rouzina . We assume that the whole process is slow enough so that the system is always in equilibrium. Then in zero order approximation, the force needed to detach DNA from the condensate is just the free energy difference per unit length between the free coil state and the condensed state of the DNA-spermidine complex. We call it $`f_0`$. The pulling force $`f_p`$ measured in the experiment is somewhat larger than $`f_0`$ since the detached part of the DNA molecule is stretched, and therefore loses entropy with respect of its free coil state. In the end of the paper, we show that this effect adds a small correction to the pulling force,

$$f_p=f_0\left(1+\sqrt{\frac{k_BT}{lf_0}}\right)$$
(1)
when $`k_BT/lf_01`$. Here $`l`$ is the persistence length of DNA. In this paper, we first calculate $`f_0`$ and then $`f_p`$ using Eq. (1). Our result is shown in Fig 3. It demonstrates reasonably good agreement with experimental data.

Let us start from the theory of reentrant condensation of DNA with spermidine without any external forces. In the solution, positively charged spermidine molecules are absorbed on the negatively charged surface of double helix DNA. Since spermidine molecules are strongly charged ($`+3`$), they form a two dimensional strongly correlated liquid on the surface of the DNA molecule. When a new spermidine molecule approaches the DNA helix, it repels already absorbed spermidine molecules and creates an electrostatic image of itself, similar to the image on a conventional metallic surface. Attraction to the image leads to an additional negative chemical potential $`\mu _c`$ for spermidine molecules on the surface of DNA. As a result, if $`s`$ exceeds some concentration, $`s_0`$, charge of the DNA-spermidine complex changes sign and becomes positive, i.e., spermidine molecules overcharge DNA (see review of the theory of charge inversion in Ref. Nguyen-review ).

Adsorbed layers of the correlated spermidine liquid also lead to self-attraction of DNA. In the spot where two turns of DNA touch each other, the surface density of the correlated liquid is doubled and the correlation energy per spermidine molecule is reduced Bloomfield . This short range force of self-attraction leads to condensation of DNA if the macroscopic Coulomb repulsion is not very strong. As a result, in the vicinity of the neutralizing concentration $`s_0`$ ($`s_c<s_0<s_d`$), DNA-spermidine complex is condensed into a toroid.

The condition of equilibrium between spermidine molecules in the bulk and on the surface of DNA has a form

$$\mu _c+Ze\varphi =k_BT\mathrm{ln}(sv_0),$$
(2)
where $`Z=+3`$ is the valence of spermidine, $`\varphi `$ is the electric potential on the surface of the DNA-spermidine complex, and $`v_0`$ is the normalizing volume of spermidine. The left hand side is the chemical potential of a spermidine molecule in the complex, the right hand side is its chemical potential in the bulk of the solution. Notice that the entropy of spermidine can be expressed through the total concentration $`s`$ because absorbtion of spermidine by DNA practically does not change $`s`$ (the concentration of DNA nucleotides is at least $`10^5`$ times smaller than $`s`$). In the vicinity of $`s_0`$ ($`s_c<s<s_d`$), the net charge of the complex is small and the spermidine concentration on the DNA surface does not change much. Since $`\mu _c`$ is determined by this concentration, it is approximately a constant. According to Eq. (2), when $`\varphi =0`$, i.e., the complex is neutral, there is a simple relation between $`\mu _c`$ and $`s_0`$,

$$s_0=\frac{1}{v_0}\mathrm{exp}\left(\frac{|\mu _c|}{k_BT}\right).$$
(3)
Now we calculate the free energy of the charged complex in its coil state. For this purpose, we treat the DNA-spermidine complex as a capacitor with the capacitance per unit length $`C`$. Suppose $`s`$ is such that the complex is overcharged ($`s_0<s<s_d`$). Overcharging enhances the Coulomb self-energy and reduces both the correlation energy and the entropy of spermidine molecules. Taking the free energy of a neutral coil as zero, and using Eq. (2), we get the free energy of the complex per unit length

$$f_1=\frac{1}{2}C\varphi ^2+\frac{C\varphi }{Ze}\mu _c\frac{C\varphi }{Ze}k_BT\mathrm{ln}(sv_0)=\frac{1}{2}C\varphi ^2,$$
(4)
where the three terms allow for the three parts of the free energy mentioned above, and $`C\varphi /Ze`$ is the number of spermidine molecules overcharging the complex. The final expression is the same as the free energy of a capacitor kept under a constant voltage $`\varphi `$. It is easy to see that this expression is also true for an undercharged complex. Since the DNA-spermidine complex can be considered as a long cylinder, $`C`$ is given by expression

$$C=\frac{D}{2\mathrm{ln}(1+r_s/R)},$$
(5)
where $`D=80`$ is the dielectric constant of water, $`r_s`$ is the Debye-Hückel screening radius, and $`R=10`$ $`\AA `$ is the radius of the double helix cross section.

We first assume that $`r_sR`$. In this case, the complex in the condensed state is practically neutral. Indeed, if the condensed complex were charged, the Coulomb-self energy of the macroscopic condensate would be too large to hold it. We define phenomenological parameter $`\epsilon <0`$ as the free energy per unit length of the condensed complex calculated from the free energy of a neutral coil. It includes the gain of correlation energy in the spots where two turns of DNA touch each other, and also the loss of certain entropic elasticity of the coil in the condensate.

When the complex goes from the neutral condensed state to the charged coil state, the free energy increment per unit length is

$$f_0=\frac{1}{2}C\varphi ^2\epsilon .$$
(6)
If $`r_s`$ is comparable with $`R`$ (as in experiment Murayama ), the approximation used above that the condensate is neutral has to be revised and the Coulomb energy of the condensate should be taken into account. If we introduce $`C^{}`$ as the effective capacitance per unit length of the complex in the condensate, similarly to Eq. (4), the free energy per unit length is just $`C^{}\varphi ^2/2`$. Accordingly, in Eq. (6), $`C`$ should be replaced by $`CC^{}`$. Using Eqs. (2) and (3), we rewrite Eq. (6) as

$$f_0=|\epsilon |\frac{(CC^{})k_B^2T^2}{2Z^2e^2}\mathrm{ln}^2\frac{s}{s_0}.$$
(7)
The function $`f_0(\mathrm{ln}s)`$ is shown in Fig. 4 by an inverted parabola. According to Eq. (7), the maximum value $`f_0=|\epsilon |`$ is achieved at $`s=s_0`$ where the free complex is neutral. Also, we get the two concentrations $`s_c`$ and $`s_d`$ at which $`f_0`$ goes to zero,

$`s_{c,d}=s_0\mathrm{exp}\left({\displaystyle \frac{1}{k_BT}}\sqrt{{\displaystyle \frac{2|\epsilon |Z^2e^2}{CC^{}}}}\right),`$ (8)
where the upper (lower) sign corresponds to the first (second) subscript of $`s_{c,d}`$. Exactly at these two concentrations, one can see transition from the coil state to the condensed state or vice versa in light scattering experiments with solutions of DNA and spermidine Rouzina .

In order to calculate $`C^{}`$, we assume that the condensate is macroscopic and densely packed. Then

$$\varphi =_0^{\mathrm{}}\frac{\rho e^{r/r_s}}{Dr}4\pi r^2𝑑r=\frac{4\pi r_s^2\rho }{D},$$
(9)
where $`\rho `$ is the charge density of the condensate. The charge of the complex per unit length is $`\pi R^2\rho /\alpha `$ where $`\alpha =0.91`$ is the filling factor for the hexagonal dense packing of cylinders. This gives

$$C^{}=\frac{\rho }{\varphi }\frac{\pi R^2}{\alpha }=\frac{DR^2}{4\alpha r_s^2}.$$
(10)
We see that when $`r_sR`$, we can drop $`C^{}`$ in $`CC^{}`$ because $`C^{}C`$, i.e., the condensate is almost neutral.

As we mentioned before, $`f_0`$ is only the zero order approximation to the pulling force. The pulling force $`f_p`$ is given by Eq. (1). We need four experimental parameters to calculate it. The spermidine concentrations $`s_{c,d}`$ at which the condensate dissolves, the average DNA persistence length $`l`$, and the average Debye-Hückel screening radius $`r_s`$. Following Ref. Murayama , we take $`s_c=0.35`$ mM, $`s_d=150`$ mM. Therefore $`s_0=7.2`$ mM (Using Eq. (8)). We use $`l=500`$ $`\AA `$ corresponding to the persistence length of a neutral DNA coil. At $`s_0=7.2`$ mM, spermidine and its counter ion contribute to $`r_s`$ even more than monovalent salt ($`10`$ mM). Treating every spermidine molecule as a point-like trivalent ion, we get $`r_s=13`$ $`\AA `$ from the standard Debye-Hückel expression rs . Calculating $`C`$ and $`C^{}`$ according to Eqs. (5) and (10), we finally get $`|\epsilon |=0.11`$ $`k_BT`$/bp (1bp $`=3.4`$ $`\AA `$) from Eq. (8).

For these parameters, $`f_0`$ and $`f_p`$ are shown together with the experimental data in Fig. 3. We see that our result for $`f_p`$ agrees pretty well with the experimental data. Notice that correction $`f_pf_0`$ is much smaller than $`f_0`$ in the range of experimental data. This justifies the use of the perturbative result Eq. (1).

Finally, let us derive Eq. (1). For this purpose, we consider the detached part of DNA as a wormlike chain with the contour length $`L`$ and end-to-end distance $`x`$ (see Fig. 1), while the contour length of the whole DNA molecule is $`L_0`$. We also assume that the system is always in equilibrium during the whole process. The free energy of the system is

$`F(x,L)=(L_0L)f_0+F_e`$
$`=(L_0L)f_0+{\displaystyle \frac{k_BT}{l}}\left[{\displaystyle \frac{x^2}{2L}}+{\displaystyle \frac{L}{4(1x/L)}}{\displaystyle \frac{x+L}{4}}\right],`$
(11)
where $`(L_0L)f_0`$ is the free energy of the condensed part of DNA, and $`F_e`$ is related to the entropic elasticity of the detached part of DNA. The expression for $`F_e`$ is obtained for a *free* wormlike chain with fixed contour length $`L`$ and end-to-end distance $`x`$: $`F_e(x)=_0^xf_e(x^{})𝑑x^{}+const.`$. Here $`f_e`$ is the force needed to keep the end-to-end distance $`x`$ for a *free* wormlike chain with length $`L`$ and is given by an interpolation formula Marko

$$f_e=\frac{k_BT}{l}\left[\frac{x}{L}\frac{1}{4}+\frac{1}{4(1x/L)^2}\right].$$
(12)
The energy zero point has been chosen at $`x=0,L=L_0`$, i.e., at the free energy of a DNA-spermidine complex in its coil state.

For a given $`x`$, the contour length $`L`$ of detached DNA can be found from the condition of minimal free energy, namely, $`F/L|_x=0`$. If we define $`ax/L<1`$, this minimum condition can be written as

$$2a^2(1a)^2+a^2\frac{4lf_0}{k_BT}(1a)^2=0.$$
(13)
Finding $`a`$ from this equation and putting $`L=x/a`$ back to Eq. (11), we calculate the magnitude of the pulling force

$$f_p\left|\frac{F}{x}\right|=\frac{f_0}{a}+\frac{k_BT}{l}\left[\frac{a}{2}\frac{1}{4}+\frac{1}{4(1a)}\right].$$
(14)
Notice that $`a`$ does not depend on $`x`$ and $`L`$ (see Eq. (13)). Therefore, according to the definition $`x=aL`$, the two lengths $`x`$ and $`L`$ are always proportional to each other. This result was also obtained in Ref. Wada  using a different approach. From Eq. (14) it is easy to see that $`f_p>f_0`$ since $`a<1`$. There are two contributions to $`f_pf_0`$. The first is a geometrical effect (the term $`f_0/a`$ in Eq. (14)). Namely, to change the end-to-end distance by $`\mathrm{\Delta }x`$, a larger length $`\mathrm{\Delta }L=\mathrm{\Delta }x/a`$ must be pulled out of the condensate. The second contribution is the free energy increment of the detached part of DNA, $`F_e`$. These two contributions are equal in the limiting case of $`k_BTlf_0`$ (see Eqs. (15), (16) and (1)). Since $`f_p`$ does not depend on $`x`$, we get a force plateau with increasing $`x`$, as observed in the experiment (see Fig. 2). This plateau ends when $`x`$ reaches $`x_0=aL_0`$ and all DNA is pulled out of the condensate. At $`x>x_0`$, the pulling force starts to increase with $`x`$ according to Eq. (12ForcePlateau .

When $`k_BT/lf_01`$, we have $`1a1`$, and Eq. (14) becomes

$$f_p=\frac{f_0}{a}+\frac{k_BT}{4l(1a)}.$$
(15)
Solving Eq. (13) in the same limit, we get

$$a=1\frac{1}{2}\sqrt{\frac{k_BT}{lf_0}}.$$
(16)
Substituting Eq. (16) in Eq. (15), we arrive at our final result Eq. (1). It gives the pulling force $`f_p`$ in the first order perturbation theory in the small parameter $`\sqrt{k_BT/lf_0}`$. In experiment Murayama , we have $`k_BT/lf_0=0.06`$ at $`s=s_0`$. Therefore, Eq. (1) can be used in almost all the range $`s_c<s<s_d`$. At $`s`$ close to $`s_{c,d}`$, where $`f_00`$, the perturbation theory fails. In principle, we can calculate $`f_p`$ numerically using Eqs. (13) and (14) in the whole interval $`s_c<s<s_d`$.

###### Acknowledgements.

The authors are grateful to A. Yu. Grosberg, Y. Murayama, Y. Rabin, I. Rouzina, and J. Zhang for useful discussions. This work is supported by NSF No. DMR-9985785 and DMI-0210844.


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# Orbital and spin moment in CoO∗

## I Introduction

A consistent description of properties of CoO, in general of 3d-atom oxides, including monooxides, reconciling its insulating state with the unfilled 3$`d`$ shell is still not reached as one can learnt from recent papers 1 ; 2 ; 3 ; 4 ; 5 ; 6 ; 7 ; 8 .

The aim of this short paper, 9 , is to report the calculations of the magnetic moment of CoO, its spin and orbital contribution. The direct motivation was a recent paper of Ref. 8 , published in Phys. Rev. B 65 (2002) 125111, in which a presented theoretical approach was unable to calculate the orbital moment. In our approach we attribute the moment of CoO to the Co2+ ions. We have calculated the moment of the Co2+ ion in the CoO6 octahedral complex, its spin and orbital parts. The orbital moment at 0 K as large as 1.38 $`\mu _B`$ has been found. The approach used can be called the quasi-atomic approach 10 ; 11  as the starting point for the description of a solid, containing open-shell atoms, is the consideration of the atomic-like low-energy electronic structure of the constituting atoms/ions, in the present case of the Co2+ ions.

## II Theoretical outline

The used Hamiltonian is the same as we have used earlier for FeBr2 and NiO 10 ; 11 ; 12 . Our Hamiltonian for CoO consists of two terms: the single-ion-like term $`H_d`$ for the outer seven $`d`$ electrons and the $`d`$-$`d`$ intersite spin-dependent term, important for the formation of the magnetic state. We treat the 7 outer electrons of the Co2+ ion as forming the highly-correlated electron system 3$`d^7`$. The correlations among electrons in the unfilled 3$`d`$ shell are approximated by two Hund’s rules, that yield the ground-term quantum numbers $`S`$=3/2 and $`L`$=3, i.e. the ground term $`{}_{}{}^{4}F`$ 13 ; 14 . Such the localized highly-correlated electron system interacts in a solid with the charge (it is known as crystal-field interactions) and spin surroundings. The charge surrounding has the octahedral symmetry owing to the $`NaCl`$-type of structure of CoO. We take into account the small tetragonal distortion as is experimentally observed 7 . For the quasi-atomic single-ion-like Hamiltonian of the 3$`d^7`$ system we take into account the crystal-field interactions of the octahedral symmetry, with the octahedral CEF parameter $`B_4`$=-40 K like we have assumed in our earliest paper 15  (on basis of our recent studies 16  a value of -30 K seems to be more appropriate, but it affects only very slightly the presented results as $`B_4`$ determines excitations in the optical region; the most important is the negative sign that is determined by negative charges of the oxygen octahedron), the spin-orbit interactions with the spin-orbit coupling $`\lambda _{so}`$=-260 K like in the free ion 13 , p. 399, and a small tetragonal distortion approximated by the term $`B_2^0`$=-10 K. The calculated single-ion states under the octahedral crystal field and the spin-orbit coupling (the CoO6 complex) are presented in Fig. 1 of Ref. 9 . All states have at least double Kramers degeneracy in agreement with the Kramers theorem. Magnetic interactions are considered within the mean-field approximation with the molecular-field coefficient $`n`$ = -40 T/ $`\mu _B`$, that yields the experimental value TN of 290 K.

## III Results and discussion

For the purely octahedral symmetry the ground-state doublet is characterized by the total moment of $`\pm `$2.21 $`\mu _B`$ ($`\pm `$ corresponds to the Kramers states). This moment is built up from the orbital and spin moments of $`\pm `$0.55 and $`\pm `$1.66 $`\mu _B`$, respectively. The presence of the tetragonal distortion B$`{}_{}{}^{0}{}_{2}{}^{}`$=-10 K causes a slight increase of these moments, to $`\pm `$2.54 $`\mu _B`$, $`\pm `$0.70 and $`\pm `$1.84 $`\mu _B`$, respectively. The presence of the magnetic field, external or internal in case of the magnetically-ordered state polarizes two doublet states. We have calculated that the Co moment in the magnetic state at 0 K experiences the molecular field of 161 T. This field gradually diminishes to TN of 290 K. In the magnetic state there appears a spin-like gap of 40 meV (see Fig. 2 of Ref. 9 ).

At 0 K in the magnetically-ordered state the magnetic moment was calculated to be 4.02 $`\mu _B`$. It is built up from the spin moment of 2.64 $`\mu _B`$ ($`S_z`$=1.32) and the orbital moment of 1.38 $`\mu _B`$. The calculated total moment is in good agrement with the very recent experimental datum of 3.98$`\pm `$0.06 $`\mu _B`$ for the Co moment 8 . The calculated orbital moment is quite substantial being more than 34% of the total moment. Our theoretical outcome, revealing the substantial orbital moment is in nice agreement with the recent magnetic x-ray experimental result that has revealed the $`L`$/$`S`$ ratio of 0.95 17 \- the calculated by us values lead to $`L`$/$`S`$ ratio, in fact their $`z`$ components, of 1.04.

It is trivial to remind that the evaluation of the orbital moment is possible provided the spin-orbit coupling is taken into account. Our calculations of the orbital moment of the 3$`d`$ atom and mostly the growing experimental evidence 17  for the existence of the significant orbital moment in the 3$`d`$-atom compounds confirm the importance of the spin-orbit coupling for the description of the 3$`d`$ magnetism. The present model allows, apart of the ordered moment and its spin and orbital components to calculate many physically important properties like temperature dependence of the magnetic susceptibility, temperature dependence of the heat capacity, the spectroscopic $`g`$ factor, the fine electronic structure in the energy window below 4 eV with at least 28 localized states. Although we consider here the Co2+ ion in the oxygen octahedron, the physical relevance of the obtained results to bulk CoO is obvious - the $`NaCl`$ structure is built up by the edge sharing Co2+ octahedra and the similar electronic structure occurs at each Co site.

## IV Conclusions

The orbital and spin moment of the Co2+ ion in CoO has been calculated within the quasi-atomic approach taking into account the intra-atomic spin-orbit interactions by the same approach as we have earlier used for NiO 12 , for FeBr2 11  and for LaCoO3 16 . The orbital moment of 1.38 $`\mu _B`$ amounts at 0 K, in the magnetically-ordered state, to more than 34% of the total moment of 4.02 $`\mu _B`$. In our description we largely employ the atomic physics. We use only four parameters, B4, $`\lambda _{so}`$, B$`{}_{}{}^{0}{}_{2}{}^{}`$ and $`n`$ \- all of them have the clear physical meaning. Our atomic-like approach can be extended to take into account other physical phenomena. Our approach takes into account very strong correlations among $`d`$ electrons in agreement with the general conviction about their fundamental importance in 3$`d`$ oxides. We take these correlations to be stronger than crystal-field interactions. In contrary to Ref. 8 , where an effective charge of +1.66 only has been found at the Co site we work with the +2.0 charge. According to our calculation the +2.0 state lowers the cohession energy by 45 % - so our solution is energetically favoured. Our theoretical model can be regarded as a model with $`U`$ = $`\mathrm{}`$ and the Hund coupling constant $`J_H`$ = $`\mathrm{}`$. Our model, presenting here in the purely ionic form, explains the insulating ground state despite the open 3$`d`$ shell. Our studies indicate that it is the highest time in solid-state physics to ”unquench” the orbital moment in the description of 3$`d`$-atom containing compounds.

This version has been resubmitted 8 October 2003 to Phys. Rev. B as LS8314. It is the revised version of the original submission 14-05-2002 to Phys.Rev.Lett. as Orbital moment in CoO. Later, 27-03-2003, it was transferred to Phys.Rev.B that is available at cond-mat/0211705.

APPENDIX A
Submission letter to Physical Review Letters of 14-05-2002

From: sfradwan@cyf-kr.edu.pl To: prltex@aps.org
Subject: submit PRL Radwanski Date sent: Tue, 14 May 2002 21:03:12 +0200
From R.J. Radwanski and Z. Ropka 14.05.2002 To: Editor of Phys.Rev.Lett.

Dear Sir,

Please find attached my paper: The orbital moment in CoO by R.J. Radwanski, Z.Ropka, that I submit for publication in Phys.Rev. Lett..

Paper is prepared in the tex.file. Paper contains three Figures that are attached in EPS.file.The paper offers novel theoretical result for the orbital and spin moment in CoO. Such calculations have not been published up to now. It is the first consistent calculations for the orbital moment. Our calculations are taking into account the spin-orbit coupling. Practically all calculations presented up to now in literature were not able to calculate orbital moment. The orbital magnetism is a hot topic in the nowadays magnetism.

The paper accounts 4 pages, Plus figure caption (page 5) and 3 figures in eps.

We would appreciate publication of our paper.

Sincerely Yours, R.J.Radwanski
Attachments: C:$`\backslash `$3d-02$`\backslash `$CoO-prl$`\backslash `$Radwanski-CoO.tex,

Fig1-Radw.eps, Fig2-Radw.eps, Fig3-Radw.eps

APPENDIX B
Rejection by the Editor of Physical Review Letters of 24-05-2002

Due to reasons independent on authors it is only available on www.css-physics.edu.pl

APPENDIX C
Resubmission letter to Physical Review Letters of 27-05-2002

From: sfradwan@cyf-kr.edu.pl R.J. Radwanski and Z. Ropka
To: Physical Review Letters $`<`$prl@ridge.aps.org$`>`$
Subject: resub LS8314, 3 fig. like before Date sent: Mon, 27 May 2002 22:19:21 +0200

To Editor of Phys.Rev.Lett. Reinhardt B. Schuhmann

concerns: LS8314 -The orbital moment in CoO

Dear Editor,

In the answer to your fast rejection of our a/m Letter, please take at first the sincere congratulations for becoming the Editor of Phys.Rev.Lett.. It is, however, very responsible job. Secondly, great thanks for fast answer. However, please be so kind to say a word why our Letter is not suitable for the publication in Phys.Rev.Lett. Our Letter presents, for the first time according to our knowledge, the calculations of the orbital moment in CoO (if not, please write where it was published). The topic of the orbital moment is very important in 3d magnetism, see just published papers in Phys.Rev. B and J.Phys.Chem. Solids mentioned in our reference list.

We resubmit our Letter - 3 figures are as previously. Hoping to hear from you good news

Sincerely Yours, R.J. Radwanski and Z. Ropka
Attachments: C:$`\backslash `$3d-02$`\backslash `$CoO-prl$`\backslash `$Radwanski-CoO.tex

APPENDIX D
Secend rejection by the Editor of Physical Review Letters of 05-June-2002

Due to reasons independent on authors it is only available on www.css-physics.edu.pl

APPENDIX E
Submission to Phys. Rev. B 27.03.2003 - transfer from Phys. Rev. Lett.

From: sfradwan@cyf-kr.edu.pl
To: prbtex@aps.org
Subject: submit PRB Radwanski
Date sent: Thu, 27 Mar 2003 20:50:09 +0100
From: R.J. Radwanski and Z. Ropka 27.03.2003
To: Editor of Phys.Rev. B

Dear Editor,

Dear Dr P.D. Adams

Please find attached our paper: The orbital moment in CoO by R.J. Radwanski, Z.Ropka, that I submit for publication in Phys.Rev. B.

Paper is prepared in the tex.file. Paper accounts 4 pages, 16 Refs, three Figures that are attached in EPS.file.

The paper offers novel theoretical result for the orbital and spin moment in CoO. Such calculations have not been published up to now. It is the first consistent calculations for the orbital moment. Our calculations are taking into account the intra-atomic spin-orbit coupling. Practically all calculations presented up to now in literature were not able to calculate orbital moment.

The orbital magnetism is a hot topic in the nowadays magnetism. The direct motivation for this paper was a publication by Jauch and Reehuis in Phys.Rev. B 65 (2002) 125111 as well as earlier PRB 64 (01) 052102, PRB 44 (91) 943 and 1364, PRB 49 (94) 10864 and 10170; Phys.Rev.Lett. 80 (98) 5758.

We would appreciate the publication of our paper and the scientific referee process.

Sincerely Yours,

R.J.Radwanski
Attachments: C:$`\backslash `$3d-02$`\backslash `$CoO-prl$`\backslash `$Radwanski-CoOb.tex,
Fig1-Radw.eps, Fig2-Radw.eps, Fig3-Radw.eps

APPENDIX F
Rejection by the Editor of Physical Review B of 15-09-2003

Due to reasons independent on authors it is only available on www.css-physics.edu.pl

APPENDIX G
RESUBMISSION TO Phys. Rev. B 8 October 2003

From: sfradwan@cyf-kr.edu.pl
To: Physical Review B $`<`$prbtex@ridge.aps.org$`>`$
Subject: resub PRB LS8314B Radwanski
Date sent: Wed, 8 Oct 2003 18:04:26 +0200
From: R.J. Radwanski Krakow, 08-10-2003
Re: LS8314B: $`>`$ Orbital moment in CoO, By: R.J. Radwanski and Z. Ropka

submitted 14-05-02 to PRL, transferred to PRB 28-03-03.

Dear Editor of Phys. Rev. B,

In the answer to your last e-mail of 15-09-03 of Julie Kim-Zajonz, about our apper LS8314B: Orbital moment in CoO, we say that we highly appreciate great physical knowledge of the Editor of PRB, however, than the Editor should openly publish his scientific view, as extremaly scientifically important as conventional paper. Otherwise, a nonsense situation is created that very important scientific problems are discussed in private letters whereas in Phys. Rev. are published papers on much lower importance.

I hope that we agree that this situation is highly improper. Please understand that in this way the Editor of Phys.Rev. B, being aware of this fact or not, manipulates Physics.Thus we propose to forget about it and we ask the Editor of PRB to follow the scientific procedure - we remind we chose PRB due to just published theoretical paper about CoO (PRB 65 (02) 125111).

Two statements, given as example in your last e-mail and added to a standard rejection letter of Editor of Phys. Rev. B are wrong:

1. ”the manuscript does not appear to contain enough information for a reader to reproduce the results” - we stress that in our paper there are all (exactly all) information that a physicist who knows the standard book of Van Vleck from 1932 can reproduce our results (but please do not use an argument that our approach is too old),

2. ”the manuscript … also lacks concrete scientific arguments as to why your approach is superior.” - At first, we calculate the orbital moment, 1.38 miu-bi, whereas the paper PRB 65, 125111 does not calculate this physical value. In the last paper the orbital moment is inferred as 1.6 miu-bi (p. 7, left column, line 3 bottom) obtained by the simple substraction of the calculated spin-moment, of 2.40 miu-bi, p. 7, left, 23top) from the know-from-literature total moment of 3.98 (p. 7, left, line 4 b). Is it enough for your demand for a proof of the superiority? Please remember, that up to now the orbital moment was not calculated -according to the paper PRB 65, 125111 there were only rough prediction for the orbital moment in size of 1 miu-bi as is mentioned on p. 7 right column, l 2 t after two Refs 23,26. Ref. 23 it is PRL paper from 1998.

For us our approach is very natural. It is in agreement with all modern solid-state physics understanding like atomistic building of matter, atomic physics, strong correlations, local symmetry, spin-orbit coupling, … Your objection that our paper ”lacks concrete scientific arguments for the superiority of our approach” would indicate that Editor of Phys.Rev. B does not accept this understandings and prefers not well defined poetrical concepts. We take, however, these two sentences as a confirmation by the Editor PRB of the originality and the novelty of our approach. In such the situation, being fully convinced about importance of our paper and knowing that the paper on this problem just appears in Phys. Rev. B, 65 (2002) 125111, we resubmit our paper in a shorter form (in order to save the space in the journal) without figures. In order to satisfied the remarks of the Editor of PRB i) we stressed that all four parameters needed for the reproduction of our results are in our paper and ii) we added some scientific comments and arguments for the superiority of our approach.

Paper contains 4 pages + 17 references, mainly from Phys.Rev.. All 3 figures are skipped.

Owing to the publication of the paper 65 (2002) 125111 in Phys. Rev. B, the submision of our paper about CoO to Phys. Rev. B is fully justified. We would appreciate the scientific procedure of our paper and its fast publication in Phys.Rev. B. It enables the open scientific discussion.

Sincerely Yours,

R.J. Radwanski and Z. Ropka
Attachments: C:$`\backslash `$3d-02$`\backslash `$CoO-prl$`\backslash `$Radwanski-CoO-X-03.tex


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# Untitled Document

Baltic Astronomy, vol.12, XXX--XXX, 2003.

HOMOGENEITY OF BRIGHT RADIO SOURCES AT 15 GHz ON THE SKY AND IN THE SPACE

T. G. Arshakian1,333On leave from Byurakan Astrophysical Observatory, Byurakan 378433, Armenia, E. Ros1, J. A. Zensus1, M. L. Lister2

1   Max-Planck-Institut für Radioastronomie, Auf dem Hügel 69, 53121 Bonn, Germany
2   Department of Physics, Purdue University, 525 Northwestern Ave., W. Lafayette, IN 47907-2036, U.S.A.

Received: 12 October 2003

## Abstract

A revised sample of the 2 cm Very Long Baseline Array (VLBA) survey is studied to test the isotropic distribution of radio sources on the sky and their uniform distribution in space. The revised sample is complete to flux-density limits of 1.5 Jy for positive declinations and 2 Jy for $`0^\mathrm{o}>\delta >20^\mathrm{o}`$. At present the active galactic nuclei sample comprises 122 members. Application of the two-dimensional Kolmogorov-Smirnov (K-S) test shows that there is no significant deviation from the homogenous distribution in the sky, while the $`V/V_{\mathrm{max}}`$ test shows that the space distribution of active nuclei is not uniform at high confidence level (99.9 %). This is indicative of a strong luminosity and/or density evolution implying that active nuclei (or jet activity phenomena) were more populous at high redshifts, $`z2`$.

Key words:  surveys – quasars: general – galaxies: active – galaxies: nuclei – galaxies: jets – BL Lacertae objects: general

1.   INTRODUCTION AND THE SAMPLE

The original 2 cm sample (Kellermann et al. 1998 and Zensus et al. 2002) was selected from the Stickel catalog (Stickel et al. 1994) with the aim of including flat-spectrum, core-dominated active galactic nuclei with spectral indices $`>0.5`$. This sample was enlarged by adding some sources of special interest, such as steep spectrum sources, a few lobe-dominated sources and gigahertz-peaked spectrum sources. The 2 cm sample is being used to study the morphology of compact radio sources, their variability and jet kinematics. To investigate statistically significant correlations between the jet parameters, to compare theoretical predictions of relativistic beaming model, it has been necessary to define a complete flux-density limited sample. The revised sample consists of 122 AGN (see e.g., Zensus et al. 2003). The main selection criterion is the flux-density limit at 15 GHz; all variable sources with galactic latitude $`\left|b\right|>2.5^{}`$ and with measured VLBA flux densities exceeding 1.5 Jy (2 Jy for southern sources) at any epoch since 1994 are included in the sample. All 122 AGN are radio-loud and core-dominated. Most of them have superluminal radio jets on parsec-scales. At present there are 99 members and 23 candidates. Among members there are 73 quasars, 14 BL Lacs, 7 radio galaxies and 5 sources with no optical counterparts. All AGN except 0642+449 ($`z=3.41`$) have redshifts less than 2.43.

Since this sample is a subsample selected from the Stickel catalog it is important to understand what selection effects it might contain. Here, we investigate the homogeneity of the 2 cm flux-density limited sample on the sky and in the space.

3.   SKY DISTRIBUTION

If the sample of radio sources is free from selection effects, then we should expect that radio sources are distributed uniformly in the sky. The distribution of the 99 member AGN on the celestial sphere is shown in Figure 1.

The distribution of radio sources looks patchy with a few clusters and voids in the sky. We also generated 99 points randomly distributed in the same region of the sky and saw that for small number of random points there are modest clusterings and voids as seen in the real data. To confirm this result we performed two dimensional K-S test to test the consistency of the coordinates of sources with the coordinates of uniformly distributed points on the sphere. No significant deviation between data and model is found for any redshift bin.

If sources are randomly distributed in the sky, then the right ascensions will be uniformly distributed and declinations will be $`\mathrm{sin}\left(\pi /2\delta \right)`$ distributed. The one-dimensional K-S test does not show significant deviation of the declinations from the expected distribution. One interesting result comes for the right ascensions of 15 sources between $`1.3<z<2`$: there is a clustering of 14 sources between $`03^\mathrm{h}<\alpha <15^\mathrm{h}`$, so, the uniform distribution can be rejected at high, 99.92 %, confidence level. The non-uniform distribution is still significant for 24 sources with $`z>1.3`$, but since this result is based on small number statistics, it can only be taken as a provisional conclusion.

4.   SPACE DISTRIBUTION

We use the distribution of $`V/V_{\mathrm{max}}`$ (Schmidt 1969) to test the null hypothesis of a uniform distribution of AGN in the space. Here $`V`$ is the volume of space enclosed by the distance of the AGN having certain flux density, and $`V_{\mathrm{max}}`$ is the maximum volume of space within which this source could be observed and still be included in the complete sample. If sources have a uniform distribution in space, then $`V/V_{\mathrm{max}}=0.5`$. The difference between the expected and observed values of $`V/V_{\mathrm{max}}`$ allows the significance of a deviation of real distribution from the uniform to be estimated.

The distribution of $`V/V_{\mathrm{max}}`$ for 88 AGN with redshifts is presented in Figure 2. For quasars, the distribution is not uniform at high confidence levels (see Table 1), and it is biased towards large $`V/V_{\mathrm{max}}`$ which indicates that quasars, and hence the jet activity phenomena, were more populous at high redshifts, $`z2`$. The BL Lacs show a similar trend but this is not statistically significant because of the small number of sources. The distribution seems to be uniform for radio galaxies, i.e. with no luminosity/density evolution. This can be understand since all seven radio galaxies occupy the low redshift region where the density/luminosity evolution is negligible, but a larger sample would be needed to confirm this result.

The results are in agreement with the value of $`V/V_{\mathrm{max}}=0.68\pm 0.04`$ for steep-spectrum quasars and radio galaxies (Longair & Scheuer 1970) having extended double structure from the complete 3CRR sample. Dunlop & Peacock (1990) studied the evolution of the radio luminosity function for extragalactic radio sources combining different flux-density limited, complete samples at 2.7 GHz from the literature. They conclude that both the steep- and flat-spectrum radio sources show the same form of evolutionary behavior: radio luminosity function of quasars and radio galaxies displays positive luminosity evolution out to $`z2`$, and it declines at high redshifts. A similar evolutionary behavior up to $`z2`$ is shown by the bright flat-spectrum radio quasars and BL Lacs from the 2 cm sample.

The main conclusions are: (i) the distribution of bright AGN at 15 GHz is uniform on the sky, and (ii) the distribution of quasars and BL Lacs is biased towards large redshifts which is indicative of a strong luminosity and/or density evolution.

ACKNOWLEDGMENTS. We thank Marshall Cohen for valuable comments, Alan Roy and the members of 2 cm survey team for discussions. TGA is grateful to the AvHF for the award of a Humboldt Post-Doctoral Fellowship.

REFERENCES Dunlop J. S., Peacock, J. A. 1990, MNRAS, 247, 19 Kellermann K. I., Vermuelen R. C., Zensus J. A., Cohen M. H. 1998, AJ, 115, 1295 Longair M. S., Scheuer P. A. G. 1970, MNRAS, 151, 45 Schmidt M. 1969, ApJ, 151, 393 Stickel M., Meisenheimer K., Kuehr H. 1994, A&AS, 105, 211 Zensus J. A., Ros E., Kadler M., et al. 2003, in Radio Astronomy at the Fringe, ASP Conf. Ser. 300, eds. J.A. Zensus, M.H. Cohen, E. Ros, p. 27 Zensus J. A., Ros E., Kellermann K. I., et al. 2002, AJ, 124, 662


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# Cornering Solar Radiative-Zone Fluctuations with KamLAND and SNO Salt

## I Introduction

Neutrino-oscillation measurements are entering an era of unprecedented precision, with the solar neutrino data sol02 ; Ahmad:2002jz ; Fukuda:2002pe  and atmospheric neutrino data atm02 ; Fukuda:1998mi  combining to give a concordant picture of conversions amongst three species of active neutrinos Maltoni:2003da ; pakvasa:2003zv . The oscillation parameters which describe these conversions are the two mass-squared differences, $`\mathrm{\Delta }m_{\mathrm{sol}}^2`$ and $`\mathrm{\Delta }m_{\mathrm{atm}}^2`$, the three mixing angles, $`\theta _{12}`$, $`\theta _{23}`$ and $`\theta _{13}`$, plus phases which violate CP Schechter:1980gr  and are still to be probed. The best fits to these parameters are consistent with a maximal atmospheric mixing angle, $`\theta _{23}`$, and give a preferred solar mixing angle in the so-called large mixing angle (LMA-MSW) regime Gonzalez-Garcia:2000aj . The third angle, $`\theta _{13}`$, is strongly constrained mainly by reactor experiments Apollonio:1999ae .

A crucial recent development has been the verification of these oscillation parameters in purely terrestrial measurements, with the KamLAND experiment kamland  reporting measurements which are consistent with the oscillation parameters indicated by the solar neutrino analysis. Such an independent measurement of oscillation properties is invaluable since it allows a cleaner separation to be made between neutrino properties and solar physics, thereby opening a new observational window deep into the solar interior Bahcall .

In particular, the precise terrestrial observation of oscillations relevant to solar neutrinos allows the removal of a theoretical uncertainty in the inference of neutrino properties. This uncertainty arises because specific types of fluctuations of the solar medium deep within the solar radiative zone are known to affect neutrino oscillations Balantekin:1996pp ; Nunokawa:1996qu ; Burgess:1996 ; Bamert:1997jj , if they have sufficient size. Consequently the inference of neutrino properties from solar data require the use of prior assumptions concerning these such fluctuations.

Traditionally, the necessity for making these prior assumptions concerning solar fluctuations has not been regarded as being worrisome for several reasons. First, helioseismic measurements can constrain deviations of solar properties from Standard Solar Model predictions at better than the percent level. Second, preliminary studies of the implications for neutrino oscillations of radiative-zone helioseismic waves Bamert:1997jj  showed that they were very unlikely to have observable effects. Third, no other known sources of fluctuations seemed to have the properties required to influence neutrino oscillations.

All three of these points have been re-examined in recent years, with the result that the presence of solar fluctuations seems more likely than previously thought. First, direct helioseismic bounds turn out to be insensitive to fluctuations whose size is as small as those to which neutrinos are sensitive Castellani:1997pk ; Christensen-Dalsgaard:2002ur  (which, as we argue below, turn out to be those whose size is only several hundreds of km). Second, recent studies of magnetic fields deep inside the solar radiative zone heliomag  have identified potential fluctuations to which neutrinos might be sensitive after all (due to a resonance between Alfvén waves and helioseismic $`g`$-modes).

These studies motivate us to investigate again the extent to which neutrino-oscillation parameters can be extracted independent of prior assumptions concerning the solar fluctuations. In principle, sufficiently precise separate measurement of oscillation parameters by KamLAND and by solar neutrino detectors may allow this type of prior assumption to be relaxed. Unfortunately, global fits to the post-KamLAND data in the presence of fluctuations us ; them  have indicated that the data were not yet sufficiently precise to allow the neutrino-oscillation parameters and the solar fluctuations to be disentangled with good accuracy.

The recent release of the SNO salt results SNOsalt  call for a re-evaluation of this conclusion, since these considerably improve the precision with which solar neutrino properties are determined. It is the purpose of the letter to show that with these new data solar neutrino measurements have now changed the picture, inasmuch as global fits to neutrino properties no longer need to make prior assumptions about solar medium fluctuations in order to infer neutrino oscillation parameters. We also summarize the direct constraints on these fluctuations which may now be convincingly inferred for the first time, without making prior assumptions concerning the details of neutrino oscillations. Finally we forecast the precision which will be possible to achieve with subsequent terrestrial neutrino measurements.

## II Sensitivity to Fluctuations

The standard description of MSW oscillations Wolfenstein:1977ue  amount to the use of a mean-field approximation for the solar medium. The corrections to this mean-field approximation are due to the fluctuations in the solar medium about this mean, and the leading interaction of neutrinos with these fluctuations are parameterized by the electron-density autocorrelation, $`\delta n_e(t)\delta n_e(t^{})`$, measured along the neutrino trajectory Balantekin:1996pp ; Nunokawa:1996qu ; Burgess:1996 ; Bamert:1997jj .

As fig. (1) shows, such fluctuations act to degrade the efficiency of neutrino conversions. They can do so because successive neutrinos ‘see’ slightly different solar properties, and so in particular do not experience an equally adiabatic transition as they pass through the neutrino resonance region. The net effect is to degrade the effectiveness of the neutrino conversion because those neutrinos for which the transition is less adiabatic are more likely to survive as electron-type neutrinos. Since criterion for the transition to be adiabatic depends on how quickly the electron distribution varies near resonance, fluctuations give observable effects for neutrinos if they occur at resonance with sufficient amplitude, and if their correlation length, $`L_0`$, is comparable to the local neutrino oscillation length, $`L_{\mathrm{osc}}100`$ km.

## III The Implications of the SNO Salt Result

We now report on the result of fits which are obtained using a global analysis of the solar data, including radiochemical experiments (Chlorine, Gallex-GNO and SAGE) sol02  as well as the latest SNO data in the form of 17 (day) + 17 (night) recoil energy bins (which include CC, ES and NC contributions, see Maltoni:2002ni Ahmad:2002jz  and the Super-Kamiokande spectra in the form of 44 bins Fukuda:2002pe  (8 energy bins, 6 of which are further divided into 7 zenith angle bins). We have also used the improved measurement with enhanced neutral current sensitivity due to neutron capture on salt, which has been added to the heavy water in the SNO detector. The data are presented in the form of the neutral current (NC), charged current (CC) and elastic scattering (ES) fluxes SNOsalt . Following Ref. Maltoni:2002aw  we used data from the KamLAND collaboration given in 13 bins of prompt energy above 2.6 MeV kamland .

The sensitivity of the solar neutrino data to fluctuations in the solar medium is summarized by figures (2) and (3). Fig. (2) is taken from ref. us , and summarizes the sensitivity before the SNO salt measurements. Fig. (3) gives the same results after SNO salt. Comparing these figures shows the improvement in constraints due to the SNO salt data, and comparing the panels in each figure shows the importance of a precise determination of the neutrino oscillation parameters for obtaining a constraint on the magnitude of fluctuations.

The importance of the KamLAND and the SNO-salt measurements in these results is most easily seen from fig. (4), which compares the dependence of the fit’s $`\chi ^2`$ on the amplitude of the fluctuations for various individual data sets. This figure makes clear how the KamLAND results are largely responsible for localizing the best fit near zero fluctuation amplitude. This is as should be expected, since the evidence for the absence of fluctuations follows from the comparison of solar neutrino observations with terrestrial measurements of neutrino oscillation properties.

Note, however, that further precise determination of neutrino parameters at KamLAND due to higher statistics will have a very modest impact on the limit on the amplitude of density fluctuations within the 99% C.L. region, as can be seen from the dot–dashed line in Fig. 4.

Fig. (5) shows how the existence of solar fluctuations influences the determination of the neutrino oscillation parameters, and contains our main result. The two panels of the figure contrast the precision of the fit with and without solar fluctuations. The left panel gives results subject to the usual prior assumption of no solar fluctuations, while the right panel leaves the amplitude of such fluctuations to be obtained from the fit. (When fluctuations are included, they are assumed to have the optimal correlation length $`L_0=100`$ km.) The lines indicate contours of fixed confidence level when the KamLAND data are not included, while the coloured regions give the same information when KamLAND is included.

The main conclusion which follows from this figure is that the precision with which the neutrino oscillations are known is now largely independent of whether a prior assumption is made about the existence of solar fluctuations. With the release of the SNO salt results the comparison of solar neutrino with KamLAND data suffices to robustly determine the oscillation parameters independent of the assumed amplitude of solar fluctuations. The SNO salt data are crucial for reaching this conclusion, as is clear from fig. (6), which compares the right panel of fig. (5) with the same fit performed without using the SNO salt results.

## IV Outlook

We see that the SNO salt data, when combined with KamLAND results, for the first time places the determination of neutrino-oscillation parameters beyond the reach of sensitivity to prior assumptions concerning the existence of fluctuations in the solar radiative zone. Besides making more robust the determination of neutrino-oscillation parameters, this allows a much sharper determination of the kinds of solar fluctuations that may still be allowed deep within the solar radiative zone. As we have seen, the resulting constraints apply to fluctuations whose spatial scales are of order 100 km, and so are complementary to those obtained from helioseismology, which are insensitive to fluctuations on such short scales.

Ref. heliomag  has suggested one possible mechanism for obtaining observable fluctuations in the relevant part of the sun. In that picture fluctuations having the appropriate distance scale may arise if magnetic fields of order 10 kG should exist deep in the solar core. Magnetic fields of this size would be consistent with current observational bounds Couvidat:2002bs ; Friedland .

It is instructive to ask how the precision of these results is likely to improve given the new neutrino experiments which are currently being planned. In addition to further statistics from the KamLAND reactor experiment, we expect a high statistics of solar neutrinos above 5 MeV at the UNO experiment, which would make solar precision measurements possible Yanagisawa . Quantifying the sensitivity of upcoming detectors as probes of the Sun deep within the radiative zone lies outside the scope of this note.

Work supported by Spanish grants BFM2002-00345, by the European Commission RTN network HPRN-CT-2000-00148, by the European Science Foundation network grant N. 86, by CSIC-RAS agreement (VBS) and by MECD grants SB-2000-0464 (TIR) and AP2000-1953 (MAT). C.B.’s research is supported by grants from NSERC (Canada), FCAR (Quebec) and McGill University. VBS, NSD and TIR were partially supported by the program of Presidium RAS “Non-stationary phenomena in astronomy”.


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# Reply to Comment on “Fluctuation-dissipation relations in the non-equilibrium critical dynamics of Ising models”

## Abstract

We have recently shown that in non-equilibrium spin systems at criticality the limit $`X^{\mathrm{}}`$ of the fluctuation-dissipation ratio $`X(t,t_\mathrm{w})`$ for $`tt_\mathrm{w}1`$ can be measured using observables such as magnetization or energy \[Phys. Rev. E 68, 016116 (2003)\]. Pleimling argues in a Comment \[cond-mat/0309652\] on our paper that for such observables correlation and response functions are dominated by one-time quantities dependent only on $`t`$, and are therefore not suitable for a determination of $`X^{\mathrm{}}`$. Using standard scaling forms of correlation and response functions, as used by Pleimling, we show that our data do have a genuine two-time dependence and allow $`X(t,t_\mathrm{w})`$ and $`X^{\mathrm{}}`$ to be measured, so that Pleimling’s criticisms are easily refuted. We also compare with predictions from renormalization-group calculations, which are consistent with our numerical observation of a fluctuation-dissipation plot for the magnetization that is very close to a straight line. A key point remains that coherent observables make measurements of $`X^{\mathrm{}}`$ easier than the traditionally used incoherent ones, producing fluctuation-dissipation plots whose slope is close to $`X^{\mathrm{}}`$ over a much larger range.

In our recent paper Mayer et al. (2003) we analysed out-of-equilibrium fluctuation-dissipation (FD) relations in ferromagnetic spin systems quenched to criticality. One measures a response at time $`t`$ to a perturbation at an earlier time $`t_\mathrm{w}`$, the waiting time, and compares with the corresponding two-time correlation. The FD ratio (FDR), $`X(t,t_\mathrm{w})`$, then captures how much the response deviates from what would be expected in equilibrium. In many situations, $`T/X`$ can be thought of as an effective temperature $`T_{\mathrm{eff}}`$ governing the out-of-equilibrium dynamics Cugliandolo et al. (1997). In the context of critical dynamics the role of the long-time limit value $`X^{\mathrm{}}`$ of $`X(t,t_\mathrm{w})`$ for $`tt_\mathrm{w}1`$ as a universal amplitude ratio has been emphasized, see e.g. Godrèche and Luck (2000).

Exact results in Mayer et al. (2003) for the $`d=1`$ case with $`T_c=0`$, showed that $`X^{\mathrm{}}`$ is identical for all spin observables, whether one considers incoherent (short-range) observables or coherent (long-range) ones such as the total magnetization. For the coherent case, the limiting FD plot at long times is in fact a straight line, from which $`X^{\mathrm{}}`$ can be determined trivially. Similar results were found for the case of bond observables, where the incoherent observable corresponds to an indicator for a local domain wall while the coherent observable is the total energy. $`X^{\mathrm{}}`$ was again found to be identical for these observables. The advantage of using coherent observables is much more dramatic here: for the incoherent case the window in the FD plot where the slope is close to $`X^{\mathrm{}}`$ shrinks to zero with increasing times, while for the coherent observable one finds again a straight line FD plot of slope $`X^{\mathrm{}}`$. Numerical simulations in $`d=2`$ strongly suggested that these results carry over to higher dimensions. In particular, FD plots for both the magnetization and the energy were numerically indistinguishable from straight lines. We also found the resulting values for $`X^{\mathrm{}}`$ to be equal within numerical error, suggesting that there may be a well-defined effective temperature $`T_{\mathrm{eff}}`$ for a broad range of observables.

In a Comment Pleimling (2003), Pleimling argues that magnetization and energy are unsuitable for measuring $`X^{\mathrm{}}`$ because their correlation and response functions are dominated by one-time contributions depending only on the measurement time $`t`$. We show in this reply that Pleimling’s remarks trivially apply in the regime $`tt_\mathrm{w}`$, but say nothing about the regime where $`t`$ and $`t_\mathrm{w}`$ are of the same order. It is in this regime that our numerical data were taken, and so they do carry non-trivial two-time information. Pleimling also argues that our results are in “marked contrast” with the results of renormalization group (RG) calculations Calabrese and Gambassi (2002). We show explicitly that the RG results are in excellent agreement, predicting a limiting FD plot for the magnetization which is very close to a straight line. We also answer an “interesting question” raised, but left unanswered, by Pleimling.

We begin by reviewing the construction of the FD plots from which we determine $`X(t,t_\mathrm{w})`$, since Pleimling argues that the introduction of some one-time quantities render our plots “unsuitable”. Consider a connected two-time correlation function $`C(t,t_\mathrm{w})=A(t)B(t_\mathrm{w})A(t)B(t_\mathrm{w})`$, with $`A,B`$ two observables, and the conjugate response $`R(t,t_\mathrm{w})=T\delta A(t)/\delta h_B(t_\mathrm{w})|_{h_B=0}`$. Here $`h_B`$ is the field thermodynamically conjugated to $`B`$ and a factor of $`T`$ has been included in the response. The non-equilibrium FDR $`X(t,t_\mathrm{w})`$ is defined via

$$R(t,t_\mathrm{w})=X(t,t_\mathrm{w})\frac{}{t_\mathrm{w}}C(t,t_\mathrm{w}).$$
(1)
This relation can be cast in terms of the step response $`\chi (t,t_\mathrm{w})=_{t_\mathrm{w}}^tdt^{}R(t,t^{})`$, i.e. the response to a field $`h_B`$ switched on at $`t_\mathrm{w}`$ and kept constant since:

$`{\displaystyle \frac{}{t_\mathrm{w}}}\chi (t,t_\mathrm{w})`$ $`=`$ $`R(t,t_\mathrm{w})=X(t,t_\mathrm{w}){\displaystyle \frac{}{t_\mathrm{w}}}C(t,t_\mathrm{w})`$ (2)
$`=`$ $`X(t,t_\mathrm{w}){\displaystyle \frac{}{t_\mathrm{w}}}[C(t,t)C(t,t_\mathrm{w})].`$
Two things are important to note. First, the correlation $`C(t,t_\mathrm{w})`$ is a connected one, see the definition above. Second, it is physically sensible to compare the integrated response $`\chi (t,t_\mathrm{w})=_{t_\mathrm{w}}^tdt^{}R(t,t^{})`$ to the integral $`_{t_\mathrm{w}}^tdt^{}\frac{}{t^{}}C(t,t^{})=C(t,t)C(t,t_\mathrm{w})\mathrm{\Delta }C(t,t_\mathrm{w})`$, rather than just to $`C(t,t_\mathrm{w})`$. These observations are irrelevant in the usual situation of incoherent spin observables, for which one-time correlations are constant, but are important in our case where they do change in time (a situation sometimes referred to as physical aging). This point is discussed in detail in Refs. Mayer et al. (2003); Fielding and Sollich (2002); Buhot and Garrahan (2002); Sollich et al. (2002).

From (2) it follows that a parametric plot of $`\chi (t,t_\mathrm{w})`$ versus $`\mathrm{\Delta }C(t,t_\mathrm{w})`$ has slope $`X(t,t_\mathrm{w})`$. This is obvious if $`t_\mathrm{w}`$ is varied along the curve while $`t`$ is held fixed. However, if a series of such plots converges to a limit plot for $`t\mathrm{}`$, then this limit plot and its slope $`X`$ can clearly be obtained by varying either $`t_\mathrm{w}`$ or $`t`$, as long as both times are large. For shorter times or if no limit plot exists, plots where $`t`$ is varied and $`t_\mathrm{w}`$ is fixed will not in general have a slope related to $`X`$, whether one plots $`\chi (t,t_\mathrm{w})`$ versus $`C(t,t_\mathrm{w})`$ or versus $`\mathrm{\Delta }C(t,t_\mathrm{w})`$. However, in the simple case where $`X(t,t_\mathrm{w})`$ is constant, one has from (2) that $`\chi (t,t_\mathrm{w})=X\mathrm{\Delta }C(t,t_\mathrm{w})`$, so that a $`(\mathrm{\Delta }C,\chi )`$-plot does have the correct slope. A $`(C,\chi )`$-plot does not, on the other hand, since $`(\chi /t)(t,t_\mathrm{w})=X(d/dt)C(t,t)X(C/t)(t,t_\mathrm{w})X(C/t)(t,t_\mathrm{w})`$. This lends further support to our choice of plotting $`\chi `$ versus $`\mathrm{\Delta }C`$ rather than $`C`$ 111When using normalized FD plots, the choice of $`\mathrm{\Delta }C`$ vs $`C`$ is immaterial, since $`\mathrm{\Delta }C(t,t_\mathrm{w})/C(t,t)=1\stackrel{~}{C}(t,t_\mathrm{w})`$ differs from $`C(t,t_\mathrm{w})/C(t,t)=\stackrel{~}{C}(t,t_\mathrm{w})`$ only by a constant..

For systems where $`C(t,t)`$ does not converge for $`t\mathrm{}`$ it is convenient to consider normalized functions $`\stackrel{~}{\chi }(t,t_\mathrm{w})=\chi (t,t_\mathrm{w})/C(t,t)`$ and $`\stackrel{~}{C}(t,t_\mathrm{w})=C(t,t_\mathrm{w})/C(t,t)`$ Mayer et al. (2003); Fielding and Sollich (2002); Sollich et al. (2002). According to (2) these are also linked by

$$\frac{}{t_\mathrm{w}}\stackrel{~}{\chi }(t,t_\mathrm{w})=X(t,t_\mathrm{w})\frac{}{t_\mathrm{w}}[1\stackrel{~}{C}(t,t_\mathrm{w})].$$
(3)
Again, $`X`$ is the slope of a plot of $`\stackrel{~}{\chi }`$ vs $`1\stackrel{~}{C}`$. If a limit plot is approached for large times, either $`t`$ or $`t_\mathrm{w}`$ can be varied to obtain this plot. Explicitly, if for large times $`X`$ depends on $`t`$ and $`t_\mathrm{w}`$ only through $`\stackrel{~}{C}(t,t_\mathrm{w})`$, the shape of the limit plot follows by integration of (3) as

$$\stackrel{~}{\chi }(t,t_\mathrm{w})=_{\stackrel{~}{C}(t,t_\mathrm{w})}^1d\stackrel{~}{C}X(\stackrel{~}{C}).$$
(4)
In equilibrium $`X(t,t_\mathrm{w})1`$ and one recovers the standard FDT relation $`\stackrel{~}{\chi }(t,t_\mathrm{w})=1\stackrel{~}{C}(t,t_\mathrm{w})`$.

In Mayer et al. (2003), we showed FD plots for the total magnetization $`M=_is_i`$ (i.e. $`A=B=M`$ above) and energy $`E=_{(ij)}s_is_j`$ for a $`d=2`$ system of Ising spins $`s_i`$ quenched to its critical temperature. These were produced by varying $`t`$ at several fixed $`t_\mathrm{w}`$, and without normalization. While a priori the slope of the plot does then not necessarily correspond to $`X`$, the numerical data for $`\chi (t,t_\mathrm{w})`$ vs $`C(t,t)C(t,t_\mathrm{w})`$ fall on a straight line. Normalization only shrinks both axes of the plot in a $`t`$-dependent manner. The normalized plots will thus have the same slope, as shown explicitly in Fig. 1. The data clearly point towards the existence of a limit plot for large times which must be very close to a straight line. The asymptotic FDR $`X^{\mathrm{}}`$, which is obtained for $`tt_\mathrm{w}1`$, i.e. $`\stackrel{~}{C}0`$, is the slope at the end point of the limit plot (see the sketch in Fig. 2). Our data do not reach this end point, but RG calculations (see below) show that the slope should remain constant on approaching it. $`X^{\mathrm{}}`$ can therefore be determined from the slope in the central part of the plot (i.e., the regime $`tt_\mathrm{w}1`$).

We now summarize the scaling relations used by Pleimling, taking as he did the case of the total magnetization as an example. For large times, one expects the two-time autocorrelation of $`M`$ to scale as

$$C(t,t_\mathrm{w})=t_\mathrm{w}^{a+1}f_C(t/t_\mathrm{w}),$$
(5)
with $`a`$ expressed in terms of standard critical exponents as $`a+1=(2\eta )/z=(d2\beta /\nu )/z`$. The scaling function $`f_C`$ decays as $`f_C(r)r^\theta ^{}`$ for large $`r=t/t_\mathrm{w}`$ with $`\theta ^{}0.19`$ for the $`d=2`$ Ising model; in the limit $`r1`$, $`f_C(r)`$ has to tend to a constant to have consistency with the scaling of the equal-time correlation $`C(t,t)t^{(d2\beta /\nu )/z}=t^{a+1}`$. A similar scaling relation holds for the response, $`R(t,t_\mathrm{w})=t_\mathrm{w}^af_R(t/t_\mathrm{w})`$. As a result, $`X(t,t_\mathrm{w})`$ becomes for large times a function of $`r`$ only Godrèche and Luck (2000); this is confirmed by explicit RG calculations Calabrese and Gambassi (2002). The normalized two-time correlation

$$\stackrel{~}{C}(t,t_\mathrm{w})=\frac{C(t,t_\mathrm{w})}{C(t,t)}=(t_\mathrm{w}/t)^{a+1}\frac{f_C(t/t_\mathrm{w})}{f_C(1)},$$
(6)
likewise only depends on $`r=t/t_\mathrm{w}`$ only. Eliminating $`r`$, $`X`$ can be expressed for large times as a function of $`\stackrel{~}{C}`$. As discussed above, it follows that a plot of $`\stackrel{~}{\chi }`$ versus $`1\stackrel{~}{C}`$ must approach a limiting shape for large times; this is consistent with our numerical data in Fig. 1. Explicitly, if $`\stackrel{~}{C}(r)`$ and $`X(r)`$ are known then the limit plot is from (4)

$$\stackrel{~}{\chi }(\stackrel{~}{C})=_1^{r(\stackrel{~}{C})}dr\left(\frac{\mathrm{d}\stackrel{~}{C}}{\mathrm{d}r}\right)X(r)$$
(7)
where $`r(\stackrel{~}{C})`$ is the inverse function of $`\stackrel{~}{C}(r)`$ and the minus arises because $`\stackrel{~}{C}(r)`$ is a decreasing function.

Pleimling deduces from (5) that, in the limit $`t\mathrm{}`$ at fixed $`t_\mathrm{w}`$, $`C(t,t)C(t,t_\mathrm{w})C(t,t)`$ because $`C(t,t_\mathrm{w})C(t,t)`$. This is correct, but not surprising. As stated above, one generically expects that $`\stackrel{~}{C}(t,t_\mathrm{w})=C(t,t_\mathrm{w})/C(t,t)0`$ for $`tt_\mathrm{w}`$. For the step response $`\chi (t,t_\mathrm{w})`$ he shows similarly that this becomes independent of $`t_\mathrm{w}`$ for $`t\mathrm{}`$ and grows with the same power law as $`C(t,t)`$, so that the ratio $`\stackrel{~}{\chi }(t,t_\mathrm{w})=\chi (t,t_\mathrm{w})/C(t,t)`$ approaches a constant which we shall call $`Y`$ 222The limit $`t\mathrm{}`$ here has to be understood as taken after the zero-field limit $`h0`$. As Pleimling discusses, if one considers instead a fixed nonzero field then the response eventually becomes nonlinear, on a timescale for $`t`$ which diverges for $`h0`$. While correct, this observation is irrelevant for the present discussion: we have checked carefully that all our data are taken in the time window where the response is linear, as Pleimling’s Fig. 2 also confirms.. Summarizing, for $`t\mathrm{}`$ at fixed $`t_\mathrm{w}`$, one has $`\stackrel{~}{C}0`$ and $`\stackrel{~}{\chi }Y`$. Referring to Fig. 2, Pleimling’s statements thus fix a single point on the limiting normalized FD plot, namely its “end point” on the right. Geometrically, $`Y`$ is the axis ratio of the FD plot. It is important to stress that Pleimling’s reasoning says nothing about the rest of the limiting FD plot, which corresponds to the time regime where $`t`$ and $`t_\mathrm{w}`$ are of the same order: his limit $`t\mathrm{}`$ at fixed $`t_\mathrm{w}`$ always implies the assumption $`tt_\mathrm{w}`$. It is also clear from Fig. 2 that the axis ratio $`Y`$ and the asymptotic slope $`X^{\mathrm{}}`$ of the FD plot are not in general related. This answers the “interesting question” which Pleimling poses at the end of his Comment: $`Y`$ and $`X^{\mathrm{}}`$ are identical exactly if the limiting FD plot is a straight line. They have otherwise no reason to be related and there is no need to invoke RG calculations to “clarify” this issue.

Pleimling’s criticism would apply if, somewhat bizarrely, we had contrived only to collect data in the regime $`tt_\mathrm{w}`$. Such data would, in a normalized FD plot, fall very close to the plot’s end point at $`(1\stackrel{~}{C},\stackrel{~}{\chi })=(1,Y)`$. In an unnormalized plot, the $`t`$-dependent stretching of the plot by $`C(t,t)`$ would then indeed mean that the data trivially fall on a straight line. This line would be $`t_\mathrm{w}`$-independent and have slope $`Y`$ rather than $`X^{\mathrm{}}`$. To check for such trivial behaviour, it is sufficient to normalize the data as explained above. We re-emphasize that, as Fig. 1 shows, our data are not in the regime where such trivial behaviour is expected, covering a wide range of values of $`1\stackrel{~}{C}`$ and remaining well away from the end point of the plot. Our observation of a close-to-straight line FD plot is therefore not explained by scaling arguments, and remains highly nontrivial. This is transparent from Pleimling’s own data Pleimling (2003): one sees that his FD plots in Fig. 3 actually show data for which the $`t_\mathrm{w}`$-dependence of $`C(t,t)C(t,t_\mathrm{w})`$ (his Fig. 1) and $`\chi (t,t_\mathrm{w})`$ (his Fig. 2) is still significant.

We now comment on Pleimling’s statement that our numerical results are in “marked contrast” to the RG calculations of Calabrese and Gambassi (2002). These calculations give $`X(t,t_\mathrm{w})`$ as a function of the time ratio $`r=t/t_\mathrm{w}`$ in the form

$$X(r)=X^{\mathrm{}}\frac{F_R(r)}{F_C(r)}$$
(8)
where $`F_R`$ and $`F_C`$ are appropriate scaling functions for $`R(t,t_\mathrm{w})`$ and $`(C/t_\mathrm{w})(t,t_\mathrm{w})`$, consistent with the definition (1). Both scaling functions are of the form $`F(r)=1+ϵ^2\mathrm{\Delta }F(r)`$, within a second-order expansion in $`ϵ=4d`$. The extrapolation to $`d=2`$, $`ϵ=2`$ therefore has a certain arbitrariness. To $`𝒪(ϵ^2)`$ in the RG calculation one could replace $`F(r)`$ by e.g. $`\mathrm{exp}(ϵ^2\mathrm{\Delta }F(r))`$. We show both versions of the resulting RG predictions for $`X(r)`$ in Fig. 3. It is clear that $`X(r)`$ is close to $`X^{\mathrm{}}`$ except for $`r1`$; where it does deviate, the RG predictions also become less reliable. The near-constancy of $`X(r)`$ already suggests that the FD plot will be almost straight.

To find the limiting normalized FD plot predicted by RG explicitly, we combined the RG result for the scaling function $`F_C(r)`$ with the scaling exponents as quoted by Pleimling to obtain $`\mathrm{d}\stackrel{~}{C}/\mathrm{d}r`$ and then used (7). The result is shown in Fig. 4 and demonstrates that the RG calculations predict a limiting FD plot which is extremely close to a straight line. Quantitatively, the plot is shifted upwards from a straight line of slope $`X^{\mathrm{}}`$ by no more than $`0.01X^{\mathrm{}}`$; its axis ratio $`Y`$ therefore also lies no more than $`1\%`$ above $`X^{\mathrm{}}`$. Contrary to Pleimling’s remark, our numerical data are therefore entirely consistent with RG calculations.

As a final point, we comment on our observation in Mayer et al. (2003) that the values of $`X^{\mathrm{}}`$ are, to within numerical accuracy, identical for the magnetization (a spin observable) and the energy (a bond observable). While this may be surprising from the point of view of non-equilibrium critical dynamics 333RG calculations of $`X^{\mathrm{}}`$ for the energy are in progress for the $`O(n)`$ model in order to clarify this point (P. Calabrese, personal communication)., it is natural if one thinks of $`T_{\mathrm{eff}}=T_c/X^{\mathrm{}}`$ as an effective temperature which should govern the long-time non-equilibrium critical dynamics of all (or at least a broad range of) observables. This is supported by an analysis of the spherical model, where the values of $`X^{\mathrm{}}`$ for spin and bond observables do indeed coincide. We will report on a more detailed investigation of this point in a future publication.

In summary, Pleimling’s criticisms of our method of measuring $`X^{\mathrm{}}`$ using coherent observables do not apply. His reasoning only addresses the limit $`tt_\mathrm{w}`$, where the normalized correlation function $`\stackrel{~}{C}(t,t_\mathrm{w})=C(t,t_\mathrm{w})/C(t,t)`$ is negligibly small, while our data are taken in a regime where $`\stackrel{~}{C}(t,t_\mathrm{w})`$ is of order unity. This is most easily demonstrated using a normalized FD plot of $`\chi (t,t_\mathrm{w})/C(t,t)`$ versus $`1\stackrel{~}{C}(t,t_\mathrm{w})`$. Our observation that, for the magnetization in the $`d=2`$ Ising model quenched to criticality, the normalized FD plot is close to a straight line therefore remains nontrivial, and is consistent with RG predictions.

There are two key conclusions of our original study Mayer et al. (2003) which we have emphasized throughout this reply. First, FD plots for coherent observables are able to reveal nontrivial two-time dependences in non-equilibrium dynamics, and do so unambiguously when normalized. Second, FD plots for coherent observables typically have a wide range where their slope is close to the asymptotic value $`X^{\mathrm{}}`$. For measurements of $`X^{\mathrm{}}`$ this makes them preferable to the traditionally used incoherent observables, where this range shrinks to zero for long times.

We are grateful to P. Calabrese for discussions. We acknowledge financial support from CNRS France, EPSRC Grants No. 00800822, GR/R83712/01 and GR/S54074/01, E.U. Marie Curie Grant No. HPMF-CT-2002-01927, the Glasstone Fund, Nuffield Grant No. NAL/00361/G, Österreichische Akademie der Wissenschaften, and Worcester College Oxford. Some of the numerical results were obtained on Oswell at the Oxford Supercomputing Center, Oxford University.


text:
# Teleportation scheme implementing contextually the Universal Optimal Quantum Cloning Machine and the Universal Not Gate. Complete experimental realization

## Abstract

By a significant modification of the standard protocol of quantum state Teleportation two processes ”forbidden” by quantum mechanics in their exact form, the Universal NOT gate and the Universal Optimal Quantum Cloning Machine, have been implemented contextually and optimally by a fully linear method. In particular, the first experimental demonstration of the Tele-UNOT Gate, a novel quantum information protocol has been reported (cfr. quant-ph/0304070). A complete experimental realization of the protocol is presented here.

Classical information is encoded in bits, viz. dichotomic variables that can assume the values $`0`$ or $`1.`$ For such variables there are no theoretical limitations as far as the ”cloning” and/or ”spin-flipping” processes are concerned. However manipulations on the quantum analogue of a bit, a qubit, have strong limitations due to fundamental requirements by quantum mechanics. For instance, it has been shown that an arbitrary unknown qubit cannot be perfectly cloned: $`|\mathrm{\Psi }|\mathrm{\Psi }|\mathrm{\Psi }`$, a consequence of the so-called “no cloning theorem” . Another ”impossible” device is the quantum NOT gate, the transformation that maps any qubit into the orthogonal one $`|\mathrm{\Psi }|\mathrm{\Psi }^{}`$ . In the last years a great deal of theoretical investigation has been devoted to finding the best approximation allowed by quantum mechanics to these processes and to establish the corresponding ”optimal” values of the ”fidelity” $`F<1`$. This problem has been solved in the general case . In particular, it was found that a one-to-two universal optimal quantum cloning machine (UOQCM), i.e. able to clone one qubit into two qubits ($`12`$), can be realized with a fidelity $`F_{CLON}=\frac{5}{6}`$. The UOQCM has been experimentally realized by a quantum optical ”amplification” method, i.e. by associating the cloning effect with a QED ”stimulated emission” process . Very recently it has been argued by  that when the cloning process is realized in a subspace $`H`$ of a larger nonseparable Hilbert space $`HK`$ which is acted upon by a physical apparatus, the same apparatus performs contextually in the space $`K`$ the ”flipping” of the input injected qubit, then realizing a $`(11)`$ Universal-NOT gate (U-NOT) with a fidelity $`F_{NOT}=\frac{2}{3}`$ . As an example, a UOQCM can be realized on one output mode of a non-degenerate ”quantum-injected” optical parametric amplifier (QI-OPA), while the U-NOT transformation is realized on the other mode .

In the present work this relevant, somewhat intriguing result is investigated under a new perspective implying a modified Quantum State Teleportation (QST) protocol, according to the following scheme. The QST protocol implies that an unknown input qubit $`|\varphi _S=\alpha |0_S+\beta |1_S`$is destroyed at a sending place (Alice: $`𝒜`$) while its perfect replica appears at a remote place (Bob: $``$) via dual quantum and classical channels . Let us assume that Alice and Bob share the entangled ”singlet” state $`|\mathrm{\Psi }^{}_{AB}=2^{\frac{1}{2}}\left(|0_A|1_B|1_A|0_B\right)`$, and that we want to teleport the generic qubit $`|\varphi _S|\varphi `$. The singlet state is adopted hereafter because its well known invariance under SU(2) transformations will ensure the ”universality” of the cloning and U-NOT processes, as we shall see . The overall state of the system is then $`|\mathrm{\Omega }_{SAB}`$= $`|\varphi _S|\mathrm{\Psi }^{}_{AB}`$. Alice performs a Bell measurement by projecting the joint state of the qubits $`S`$ and $`A`$ into the four Bell states $`\{|\mathrm{\Psi }^{}_{SA},|\mathrm{\Psi }^+_{SA},|\mathrm{\Phi }^{}_{SA},|\mathrm{\Phi }^+_{SA}\}`$ spanning the 4-dimensional Hilbert space $`H`$ $`H_AH_S`$ and then sends the result to Bob by means of 2 bits of classical information. In order to obtain $`|\varphi _B`$, Bob applies to the received state the appropriate unitary transformation $`U_B`$ according to the following protocol: $`|\mathrm{\Psi }^{}_{SA}U_B=𝕀`$, $`|\mathrm{\Psi }^+_{SA}U_B=\sigma _Z`$, $`|\mathrm{\Phi }^{}_{SA}U_B=\sigma _X`$, $`|\mathrm{\Phi }^+_{SA}U_B=\sigma _Y`$ where the kets express the received corresponding information,$`I,\sigma _Z,\sigma _X`$ are respectively the identity, phase flip, spin flip operators and $`\sigma _Y=i\sigma _Z\sigma _X`$. At last, the QST channel acts on the input state $`\rho _S|\varphi \varphi |`$ as the identity operator: $`E_{QST}(\rho _S)=\rho _B`$. In absence of the classical channel, i.e. of the appropriate $`U_B`$ transformation, the apparatus realizes the map $`E_B(\rho _S)=\frac{1}{2}𝕀_B`$, corresponding to the depolarization channel $`E_{DEP}`$. This is the worst possible case because any information about the initial state $`\rho _S`$ is lost.

In order to implement the UOQCM and U-NOT at Alice’s and Bob’s sites, in the present work we modify the QST protocol by performing a different measurement on the system $`S`$ $`+`$ $`A`$. This leads to a different content of information to be transferred by the classical channel from $`𝒜`$ to $``$. Precisely, the ”Bell measurement”, able to discriminate between the 4 Bell states, is replaced here by a dichotomic ”projective measurement” able to identify $`|\mathrm{\Psi }^{}_{SA}`$ , i.e. the anti-symmetric subspace of $`H`$ $`H_AH_S`$, and its complementary symmetric subspace. Let us analyze the outcomes of such strategy, schematically represented by Figure 1. With a probability $`p=\frac{1}{4}`$ the $`|\mathrm{\Psi }^{}_{SA}`$ is detected by $`𝒜`$. In this case the correct QST channel $`E_{QST}`$ is realized. However, if this is not the case, with probability $`p=\frac{3}{4}`$, Bob cannot apply any unitary transformation to the set of the non identified Bell states $`\{|\mathrm{\Psi }^+_{SA},|\mathrm{\Phi }^{}_{SA},|\mathrm{\Phi }^+_{SA}\}`$, and then the QST channel implements the statistical map $`E\left(\rho \right)`$ = $`\frac{1}{3}\left[\sigma _Z\rho \sigma _Z+\sigma _X\rho \sigma _X+\sigma _Y\rho \sigma _Y\right]`$. As we shall see, this map coincides with the map $`E_{UNOT}\left(\rho _S\right)`$ which realizes the Universal Optimal-NOT gate, i.e. the one that approximates optimally the flipping of one qubit $`|\varphi `$ into the orthogonal qubit $`|\varphi ^{}`$, i.e. $`\rho _S`$ into $`\rho _S^{}|\varphi ^{}\varphi ^{}|`$. Bob identifies the two different maps realized at his site by reading the information (1 bit) received by Alice on the classical channel. For example, such bit can assume the value $`0`$ if Alice identifies the Bell state $`|\mathrm{\Psi }^{}_{SA}`$ and $`1`$ if she does not. We name this process $`TeleUNOT`$ since it consists in the Teleportation of an optimal antiunitary map acting on any input qubit, the U-NOT Gate .

As already stated, it has been shown that in a bipartite entangled system the optimal U-NOT Gate is generally realized contextually together with an optimal quantum cloning process . Therefore it is worth analyzing what happens when the overall state $`|\mathrm{\Omega }_{SAB}`$ is projected onto the subspace orthogonal to $`|\mathrm{\Psi }^{}_{SA}\mathrm{\Psi }^{}|_{SA}H_B`$ by the projector:

$$P_{SAB}=(𝕀_{SA}|\mathrm{\Psi }^{}_{SA}\mathrm{\Psi }^{}|_{SA})𝕀_B.$$
(1)
This procedure generates the normalized state $`|\stackrel{~}{\mathrm{\Omega }}P_{SAB}|\mathrm{\Omega }_{SAB}=\sqrt{\frac{2}{3}}[|\xi _1_{SA}|1_B|\xi _0_{SA}|0_B]`$ where: $`|\xi _1_{SA}`$= $`\alpha |0_S|0_A`$ \+ $`\frac{1}{2}\beta (|1_S|0_A+|0_S|1_A)`$ and $`|\xi _0_{SA}`$= $`\beta |1_S|1_A`$\+ $`\frac{1}{2}\alpha (|1_S|0_A+|0_S|1_A)`$. By tracing this state over the $`SA`$ and $`B`$ manifolds we get: $`\rho _{SA}Tr_B|\stackrel{~}{\mathrm{\Omega }}\stackrel{~}{\mathrm{\Omega }}|`$ = $`\frac{2}{3}|\varphi |\varphi _{SA}\varphi \left|\varphi |_{SA}+\frac{1}{3}\right|\{\varphi ,\varphi ^{}\}_{SA}\{\varphi ,\varphi ^{}\}|_{SA}`$ and $`\rho _B^{out}Tr_{SA}|\stackrel{~}{\mathrm{\Omega }}\stackrel{~}{\mathrm{\Omega }}|=\frac{1}{3}(2\rho _S^{}+\rho _S)`$ , where: $`|\{\varphi ,\varphi ^{}\}_{SA}`$= $`2^{\frac{1}{2}}\left(|\varphi ^{}_S|\varphi _A+|\varphi _S|\varphi ^{}_A\right)`$. We further project on the spaces $`A`$ and $`B`$ and obtain the output states, which are found mutually equal: $`\rho _S^{out}Tr_A\rho _{SA}`$ = $`\frac{1}{6}(5\rho _S+\rho _S^{})`$ = $`\rho _A^{out}Tr_S\rho _{SA}`$. At last, by these results the expected optimal values for the fidelities of the two ”forbidden” processes are obtained: $`F_{CLON}=Tr[\rho _S^{out}\rho _S]=Tr[\rho _A^{out}\rho _S]=\frac{5}{6}`$ and $`F_{UNOT}=Tr[\rho _B^{out}\rho _S^{}]=\frac{2}{3}`$.

In the last years many experimental realizations of quantum state Teleportation have been achieved . Recently the first ”active”, i.e. complete version of the QST protocol was realized by our Laboratory by physically implementing the Bob’s unitary operation . In the present experiment the input qubit was codified as the polarization state of a single photon belonging to the input mode $`k_S`$: $`|\varphi _S=\alpha |H_S+\beta |V_S`$, $`\left|\alpha \right|^2+\left|\beta \right|^2=1`$: Figure 2. Here $`|H`$ and $`|V`$ correspond to the horizontal and vertical polarizations, respectively. In addition, an entangled pair of photons, $`A`$ and $`B`$ were generated on the modes $`k_A`$ and $`k_B`$ by Spontaneous Parametric Down Conversion (SPDC) in the singlet state: $`|\mathrm{\Psi }^{}_{AB}`$= $`2^{1/2}\left(|H_A|V_B|V_A|H_B\right)`$. The projective measurement in the space $`H=`$ $`H_AH_S`$ was realized by linear superposition of the modes $`k_S`$ and $`k_A`$ on a $`50:50`$ beam-splitter, $`BS_A.`$ Consider the overall output state realized on the two output modes $`k_1`$and $`k_2`$ of $`BS_A`$ and expressed by a linear superposition of the states: $`\{|\mathrm{\Psi }^{}_{SA},|\mathrm{\Psi }^+_{SA},|\mathrm{\Phi }^{}_{SA},|\mathrm{\Phi }^+_{SA}\}`$. As it is well known, the realization of the singlet $`|\mathrm{\Psi }_{SA}^{}`$ is identified by the emission of one photon on each output mode of $`BS_A`$ while the realization of the set of the other three Bell states implies the emission of 2 photons either on mode $`k_1`$or on mode $`k_2`$. The realization of the last process, sometimes dubbed as ”Bose Mode Coalescence” (BMC) or ”Mode-occupation enhancement”  was experimentally identified by the simultaneous clicking of the detectors $`D_2`$ and $`D_2^{}`$ coupled to the output mode $`k_2`$ by the $`50:50`$ beam-splitter $`BS_2`$. The identical effect expected on mode $`k_1`$ was not exploited, for simplicity. As shown by the theoretical analysis above, the last condition implied the simultaneous realization in our experiment of the U-NOT and UOQCM processes, here detected by a post-selection technique. Interestingly enough, the symmetry of the projected subspace of $`H`$ identified by BMC is implied by the intrinsic Bose symmetry of the 2 photon Fock state realized at the output of $`BS_A`$.

The source of the SPDC process was a Ti:Sa mode-locked pulsed laser with wavelength (wl) $`\lambda =795nm`$ and repetition rate $`76MHz`$. A weak beam, deflected from the laser beam by mirror $`M`$, strongly attenuated by grey filters $`(At)`$, delayed by $`Z`$ $`=2c\mathrm{\Delta }t`$ via a micrometrically adjustable optical ”trombone” was the source of the quasi single-photon state injected into $`BS_A`$ over the mode $`k_s`$. The average number of injected photons was $`\overline{n}`$ $``$ $`0.1`$ and the probability of a spurious 2 photon injection was evaluated to be a factor $`0.05`$ lower than for single photon injection. Different qubit states $`|\varphi _S`$ were prepared via the optical Wave-Plate (wp) $`WP_S`$, either a $`\lambda /2`$ or $`\lambda /4`$ wp. The main UV laser beam with wl $`\lambda _p=397.5nm`$. generated by Second Harmonic Generation, focused into a $`1.5mm`$ thick nonlinear (NL) crystal of $`\beta `$-barium borate (BBO) cut for Type II phase-matching, excited the SPDC source of the singlet $`|\mathrm{\Psi }^{}_{AB}`$. The photons $`A`$ and $`B`$ of each entangled pair were emitted over the modes $`k_A`$ and $`k_B`$ with equal wls $`\lambda =795nm`$. All adopted photodetectors $`(D)`$ were equal SPCM-AQR14 single photon counters. One interference filter with bandwidth $`\mathrm{\Delta }\lambda =3nm`$ was placed in front of each $`D`$ and determined the coherence time of the optical pulses: $`\tau _{coh}350f\mathrm{sec}`$.

In order to realize the $`TeleUNOT`$ protocol, the BMC process on the output mode $`k_2`$ of $`BS_A`$ was detected by a coincidence technique involving $`D_2`$ and $`D_2^{}`$ \[Fig.2, inset: (a)\]. In order to enhance the ”visibility” of the Ou-Mandel interference at the output of $`BS_A`$, a $`\pi `$preserving mode-selector $`(MS)`$ was inserted on mode $`k_2`$. On the Bob’s site, the polarization $`\pi state`$ on the mode $`k_B`$ was analyzed by the combination of the wp $`WP_B`$ and of the polarization beam splitter $`PBS_B`$. For each input $`\pi state`$ $`|\varphi _B`$, $`WP_B`$ was set in order to make the $`PBS_B`$ to transmit $`|\varphi _B`$ and to reflect $`|\varphi ^{}_B`$, by then exciting $`D_B`$ and $`D_B^{}`$ correspondingly. First consider the Teleportation (QST) turned off, by setting the optical delay $`\left|Z\right|c\tau _{coh\text{ }}`$i.e. by spoiling the interference of photons $`S`$ and $`A`$ in $`BS_A`$. In this case, since the states $`|\varphi _B`$ and $`|\varphi ^{}_B`$ were realized with the same probability on mode $`k_B`$, the rate of coincidences detected by the $`D`$-sets $`[D_B,D_2,D_2^{}]`$ and $`[D_B^{},D_2,D_2^{}]`$were expected to be equal. By turning on the QST, i.e. by setting $`\left|Z\right|<<c\tau _{coh}`$, the output state $`\rho _B^{out}=(2\rho _S^{}+\rho _S)/3`$ was realized implying a factor $`R=2`$ enhancement of the counting rate $`[D_B^{},D_2,D_2^{}]`$ and no enhancement of $`[D_B,D_2,D_2^{}]`$. The actual measurement of $`R`$ was carried out, and the universality of the $`TeleUNOT`$ process demonstrated, by the experimental results shown in Figure 3. These 3-coincidence results, involving the sets $`[D_B,D_2,D_2^{}]`$ and $`[D_B^{},D_2,D_2^{}]`$ correspond to the injection of three different input states: $`|\varphi _S=|H`$, $`|\varphi _S=2^{1/2}(|H+|V)`$, $`|\varphi _S=2^{1/2}(|H+i|V)`$. In Figure 3 the square and triangular markers refer respectively to the $`[D_B^{},D_2,D_2^{}]`$ and $`[D_B,D_2,D_2^{}]`$ coincidences versus the delay $`Z=2c\mathrm{\Delta }t.`$ We may check that the $`TeleUNOT`$ process only affects the $`|\varphi ^{}_B`$ component, as expected. The signal-to-noise $`(S/N)`$ ratio $`R`$was determined as the ratio between the peak values, i.e. for $`Z0`$, and the no BMC enhancement values, i.e. for $`\left|Z\right|c\tau _{coh\text{ }}`$. The experimental values of the $`UNOT`$ fidelity $`F=R(R+1)^1`$ are: $`F_H=0.641\pm 0.005`$;$`F_{H+V}=0.632\pm 0.006`$; $`F_{H+iV}=0.619\pm 0.006`$, for the three injection states $`|\varphi _S`$. These results, to be compared with the optimal value $`F_{th}=2/30.666`$ corresponding to the optimal$`R=2`$, have been evaluated by taking into account the reduction, by a factor $`\xi =0.7`$, of the coincidence rate due to the spurious simultaneous injection of two photons on the mode $`k_S`$ and to the simultaneous emission of two SPDC pairs. The factor $`\xi `$ was carefully evaluated by a side experiment involving the detectors $`D_2`$and $`D_2^{}`$. Note that the experimental Tele-UNot peaks shown in Figure 3 indeed demonstrate the simultaneous, contextual realization of the Quantum Cloning and UNot Processes on Alice’ s and Bob’s sites, respectively.

For the sake of completeness, we wanted to gain insight in the linear probabilistic UOQCM process by investigating whether at the output of $`BS_A`$ the photons $`S`$ and $`A`$ were indeed left in the state $`\rho _S^{out}=(5\rho _S+\rho _S^{})/6`$ = $`\rho _A^{out}`$ after the state projection. The cloning analysis was realized on the $`BS_A`$ output mode $`k_2`$ by replacing the measurement set (a) with the (b) one, shown in the inset of Figure 2. The polarization state on mode $`k_2`$ was analyzed by the combination of the wp $`WP_C`$ and of the polarizer beam splitters $`PBS`$. For each input $`\pi `$-state $`|\varphi _S`$, $`WP_C`$ was set in order to make $`PBS^{}`$s to transmit $`|\varphi _S`$ and to reflect $`|\varphi ^{}_S`$. The ”cloned” state $`|\varphi \varphi _S`$ was detected on mode $`k_2`$ by a coincidence between the detectors $`D_C`$, $`D_C^{}`$. The generation of an entangled pair was assured by detecting one photon on the mode $`k_B`$; in this case $`PBS_B`$ was removed and the field of mode $`k_B`$ was coupled directly to $`D_B`$. Any coincidence detected by the sets $`[D_C,D_C^{},D_B]`$ and $`[D_C,D_C^{},D_B]`$ implied the realization of the states $`|\varphi \varphi _S`$ and $`|\varphi \varphi ^{}_S`$, respectively. In analogy with the previous experiment, when $`\left|Z\right|>>c\tau _{coh\text{ }}`$ the rate of coincidences detected by $`[D_C,D_C^{},D_B]`$ and $`2\times [D_C^{},D_C^{},D_B]`$ were expected to be equal. By turning on the cloning machine, $`\left|Z\right|<<c\tau _{coh}`$, an enhancement by a factor $`R=2`$ of the counting rate by $`[D_C,D_C^{},D_B]`$ and no enhancement by $`[D_C,D_C^{},D_B]`$ were expected. The experimental results of the $`S/N`$ ratio $`R`$, carried out by coincidence measurements involving $`[D_C,D_C^{},D_B]`$ and $`[D_C,D_C^{},D_B]`$ are reported in the lower plots of Figure 3, again for the three different input states: $`|\varphi _S=|H`$, $`|\varphi _S=2^{1/2}(|H+|V)`$, $`|\varphi _S=2^{1/2}(|H+i|V)`$. The square and triangular markers there refer respectively to the $`[D_C,D_C^{},D_B]`$ and $`[D_C,D_C^{},D_B]`$ coincidence plots Vs the delay $`Z`$. The following values of the cloning fidelity $`F=(2R+1)(2R+2)^1`$ were found: $`F_H=0.821\pm 0.003`$;$`F_{H+V}=0.813\pm 0.003`$; $`F_{H+iV}=0.812\pm 0.003`$, to be compared with the optimal $`F_{th}=5/60.833`$ corresponding to the limit $`S/N`$ value: $`R=2`$. As for the $`TeleUNOT`$ gate experiment, the factor $`\xi =0.7`$ has been corrected during the evaluation of the fidelities. Finally note that, in the present context the entangled singlet state $`|\mathrm{\Psi }^{}_{AB}`$was not strictly necessary for the solely implementation of quantum cloning as we could model the local effect of the singlet on the input mode $`k_A`$ by a fully mixed state $`\rho _A=\frac{1}{2}𝕀_A`$ spanning a $`2`$ dimensional space. This has been realized successfully in another experiment .

In summary, two relevant quantum information processes, forbidden by quantum mechanics in their exact form are found to be connected contextually by a modified quantum state teleportation scheme and can be ”optimally” realized. At variance with previous experiments, the complete implementation of the new protocol has been successfully performed by a fully $`linear`$ optical setup. The results are found in full agreement with theory.

This work has been supported by the FET European Network on Quantum Information and Communication (Contract IST-2000-29681: ATESIT), by I.N.F.M. (PRA ”CLON”) and by M.I.U.R.(COFIN 2002).

Figure.1. (COLOR ONLINE) General scheme for the simultaneous realization of the Tele-UNOT Gate and of the probabilistic Universal Quantum Cloning Machine (UOQCM).

Figure.2. (COLOR ONLINE) Setup for the optical implementation of the Tele-UNOT Gate and the probabilistic UOQCM. The measurement setup used for the verification of the cloning experiment is reported in the INSET (b).

Figure.3. (COLOR ONLINE) Experimental results of the Tele-UNOT Gate and the UOQCM for three input qubits. Filled squares: plots corresponding to the ”correct” polarization; Open triangles: plots corresponding to the ”wrong” polarization. The solid line represents the best gaussian fit expressing the correct polarization.