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# Measurement of the (𝛾,n) reaction rates of the nuclides 190Pt, 192Pt, and 198Pt in the astrophysical 𝛾 process

## I Introduction

The bulk of the nuclei heavier than iron have been synthesized by neutron capture in the astrophysical $`r`$ and $`s`$ processes. Those neutron-capture processes cannot account for the synthesis of some of the heavy (A $``$ 100) neutron-deficient nuclei. These nuclei are shielded from the chain of $`\beta ^{}`$ decays by other stable isobars. The production mechanism for these so-called p-nuclei is photodisintegration in the astrophysical $`\gamma `$ process by successive ($`\gamma `$,n), ($`\gamma `$,p), and ($`\gamma `$,$`\alpha `$) reactions. The natural abundances for the p-nuclei are very low in the order of 0.01 % to 1 %. A complete list of the p-nuclei can be found in Table 1 of Ref. . The starting point for the photon-induced reactions are heavy seed nuclei which have been synthesized in the $`r`$ and $`s`$ processes.

In order to reproduce the abundances of p-nuclei measured in the solar system, temperatures in the $`\gamma `$ process must be in the range of $`T_9=23`$ ($`T_9`$ is the temperature in 109 K), densities about $`\rho 10^6`$ g/cm3, and time scales $`\tau `$ of the order of seconds. A possible astrophysical site which fulfills these requirements could be the oxygen- and neon-rich layers of type II supernovae. However, there has been no definite conclusion to this question yet. Details about the $`\gamma `$ process and its astrophysical scenarios can be found in the reviews by Lambert , Arnould and Takahashi , Langanke , Wallerstein et al.  and in Refs. .

For the calculation of the p-nuclei abundances resulting from the $`\gamma `$ process, large reaction networks containing all relevant nuclei and reaction rates are needed . Until now, there have been almost no experimental data available for these reaction rates in the relevant energy region. Although in the last decades a large number of ($`\gamma `$,n) cross sections have been measured around the giant dipole resonance (GDR), the energies of astrophysical interest are much lower, and practically no data exist for the p-nuclei because of their low abundance. All reaction rates have been derived theoretically, using statistical model calculations. Reliable experimental data would be a great improvement to reduce the nuclear physics uncertainties of astrophysical model calculations, especially because of the typical uncertainties of such statistical model calculations which are at least of the order of a factor of 2.

As a starting point for the measurement of the needed reaction rates, we have measured the ($`\gamma `$,n) reaction rates of the platinum isotopes 190Pt(natural abundance: 0.014%), 192Pt(0.782%), and 198Pt(7.163%). The natural abundances have been taken from .
The ($`\gamma `$,n) reaction rate for a nucleus in a thermal photon bath is given by

$$\lambda (T)=_0^{\mathrm{}}cn_\gamma (E,T)\sigma _{(\gamma ,\mathrm{n})}(E)𝑑E$$
(1)
with the speed of light $`c`$ and the cross section of the ($`\gamma `$,n) reaction $`\sigma _{(\gamma ,n)}`$. The number of photons $`n_\gamma (E,T)`$ at energy $`E`$ per unit of volume and per energy interval is given by the well-known Planck distribution

$$n_\gamma (E,T)=\left(\frac{1}{\pi }\right)^2\left(\frac{1}{\mathrm{}c}\right)^3\frac{E^2}{\mathrm{exp}(E/kT)1}$$
(2)
For the measurement of the ($`\gamma `$,n) reaction rates we used the method of photoactivation. We irradiated platinum samples with bremsstrahlung. Then we measured the number of decays of generated unstable platinum nuclei 189,191,197Pt.

The biggest difficulty in the determination of the ($`\gamma `$,n) reaction rates is the reproduction of the thermal photon bath. In our experiment, the platinum samples were irradiated with bremsstrahlung. We are able to generate a quasi-thermal photon spectrum in the relevant energy region by the superposition of several bremsstrahlung spectra with different endpoint energies. This idea has been presented in our previous paper .

## II Experimental setup

The irradiation of the platinum samples was performed at the real photon facility of the superconducting Darmstadt linear electron accelerator S–DALINAC . This setup is mainly used for Nuclear Resonance Fluorescence experiments which can be performed up to endpoint energies of 10 MeV without disturbing neutron-induced background .

As targets we used metallic platinum disks of natural isotopic composition with a diameter of 2r = 20 mm and a thickness of d = 0.125 mm with masses of around 800 mg. The platinum disks were sandwiched between two thin boron layers with masses of about 650 mg each. In order to normalize the photon flux we measured spectra of resonantly scattered photons from nuclear levels of 11B during the activation. For this measurement, we used two high purity germanium (HPGe) detectors with 100 % efficiency (relative to a 3” $`\times `$ 3” NaI detector) which were mounted at $`90^{}`$ and $`127^{}`$ relative to the beam axis of the incoming photons. Further information on the ($`\gamma `$,$`\gamma ^{}`$) experiments can be found in .

The platinum samples were irradiated for about 24 h, then their activity was measured for another 24 h. For the measurement of the activity the samples were mounted directly in front of a third HPGe detector with 30 % relative efficiency. Some typical activation spectra are shown in Fig. 1. Altogether, six measurements with endpoint energies of the bremsstrahlung spectra between $`76509900`$ keV in steps of 450 keV were performed.

## III Analysis of the experimental data

The aim of this experiment was the determination of the ($`\gamma `$,n) reaction rates of several platinum isotopes. These reaction rates are given by Eq. (1).

The result of the analysis of the platinum activation spectra is an integral over the ($`\gamma `$,n) cross section:

$$I_\sigma =_0^{\mathrm{}}N_\gamma ^{\mathrm{brems}}(E_0,E)\sigma _{(\gamma ,\mathrm{n})}(E)𝑑E$$
(3)
where $`N_\gamma ^{\mathrm{brems}}(E_0,E)`$ is the total number of bremsstrahlung photons at energy E per area and per energy interval during the irradiation. $`E_0`$ is the endpoint energy of the respective bremsstrahlung spectrum. In order to determine the ($`\gamma `$,n) reaction rates from these results we used two different methods (see Sect. III B, III C).

### A The Gamow-like window for ($`\gamma `$,n) reactions

The integrand of Eq. (1) is given by the product of the photon flux $`cn_\gamma `$, which decreases exponentially with increasing energy, and the ($`\gamma `$,n) cross section $`\sigma _{(\gamma ,n)}`$, which increases with E to the Giant Dipole Resonance (GDR). Additionally, the threshold behavior has to be parametrized because the Lorentzian parametrization of the GDR is not valid close to the ($`\gamma `$,n) threshold (see Sect. III B). The Planck distribution, a typical ($`\gamma `$,n) cross section, and the resulting integrand of Eq. (1) are shown in Fig. 2 for 198Pt at $`T_9=3.0`$. The maximum of the integrand is located at about kT/2 above the ($`\gamma `$,n) threshold. The behavior of the integrand is similar to the well-known Gamow window (see e.g. Ref. ) for charged particle reactions at thermonuclear energies. The properties of the window for ($`\gamma `$,n) reactions have been discussed in detail in .

### B The conventional analysis

One can assume the shape of the ($`\gamma `$,n) cross section to show a typical threshold behavior:

$$\sigma (E)=\sigma _0\sqrt{(EE_{\mathrm{thr}})/E_{\mathrm{thr}}}.$$
(4)
This equation holds only in the vicinity of the reaction threshold. Nevertheless, it should be sufficiently accurate since only a small energy region above the threshold energy is relevant for the analysis. By combining Eqs. (3) and (4) it is possible to derive the parameter $`\sigma _0`$ from our experimental data. From the parameter $`\sigma _0`$ we calculated the ($`\gamma `$,n) reaction rate using Eq. (1). The serious drawback of this method is that it is not possible to estimate how much the real shape of $`\sigma `$(E) deviates from the approximation by Eq. (4).

### C The superposition of bremsstrahlung spectra

In order to derive the ($`\gamma `$,n) reaction rates directly from our experimental data, that is to say without any assumptions on the shape of the $`\sigma (E)`$ curve, we approximated the thermal Planck spectrum $`n_\gamma (E,T)`$ in Eq. (2) by the superposition of several bremstrahlung spectra with different endpoint energies:

$$cn_\gamma (E,T)\underset{i}{}a_i(T)N_\gamma ^{\mathrm{brems}}(E_{0,\mathrm{i}},E)$$
(5)
where the $`a_i(T)`$ are strength coefficients which have to be adjusted for each temperature T. With these strength coefficients, the ($`\gamma `$,n) reaction rates can be obtained by combining Eq. (5) with Eq. (1):

$$\lambda (T)=\underset{i=1}{\overset{N}{}}a_i(T)N_\gamma ^{\mathrm{brems}}(E_{0,\mathrm{i}},E)\sigma (E)𝑑E$$
(6)
An example for this superposition is shown in Fig. 3. In the energy range from 7.5 to 10 MeV the agreement between the thermal Planck spectrum at $`T_9=2.0`$ and the weighted sum of the different bremsstrahlung spectra is reasonably good. Typical deviations are of the order of 10%. Obviously, the huge deviations at energies below the ($`\gamma `$,n) reaction threshold are not relevant for our analysis.

### D Analysis of the platinum activation spectra

Fig. 1 shows three partial platinum activation spectra. Lines from the decay of the platinum isotopes 189Pt, 191Pt, and 197Pt can clearly be identified in the upper spectrum which shows the decay of a platinum sample which has been irradiated with a bremsstrahlung spectrum with an endpoint energy of 9900 keV. In the two lower spectra, which correspond to endpoint energies of 9450 keV and 9000 keV, respectively, the lines from the decay of 189Pt and 191Pt vanish because the endpoint energies of the bremsstrahlung get close to the neutron separation energies of these isotopes (see Table I). In the complete activation spectrum (see ) several additional lines, including two lines from the decay of 195mPt can be identified; this isomer is mainly populated by the ($`\gamma `$,$`\gamma ^{}`$) reaction. The spectra were analyzed using the computer code tv .
For the derivation of the ($`\gamma `$,n) reaction rates of the platinum isotopes 190Pt, 192Pt and 198Pt, the integral (3) must be calculated from the number of counts A in the decay lines of the platinum isotopes 189Pt, 191Pt and 197Pt, respectively. The dependence of these quantities is given by

$$A=ϵI_\gamma \frac{T_{\mathrm{life}}}{T_{\mathrm{real}}}\frac{N_{\mathrm{decay}}}{N_{\mathrm{total}}}N_{\mathrm{Pt}}\sigma (E)N_\gamma ^{\mathrm{brems}}𝑑E$$
(7)
where $`ϵ`$ is the absolute detector efficiency, $`I_\gamma `$ the absolute intensity of the platinum decay lines per decay, $`T_{\mathrm{life}}`$/$`T_{\mathrm{real}}`$ the ratio from lifetime to realtime, and $`N_{\mathrm{Pt}}`$ the total number of platinum nuclei of the respective isotope in the target. $`N_{\mathrm{decay}}`$/$`N_{\mathrm{total}}`$ is the ratio between the number of nuclei which decay during the measurement and the total number of produced unstable nuclei. This ratio is given by:

$$N_{\mathrm{decay}}/N_{\mathrm{total}}=e^{\lambda T_{\mathrm{loss}}}\frac{(1e^{\lambda T_{\mathrm{irr}}})}{\lambda T_{\mathrm{irr}}}(1e^{\lambda T_{\mathrm{measure}}})$$
(8)
where $`T_{\mathrm{measure}}`$ is the duration of the measurement, $`T_{\mathrm{irr}}`$ the duration of the irradiation, and $`T_{\mathrm{loss}}`$ the time between the end of the irradiation and the beginning of the measurement. These equations only hold for a constant production rate during the irradiation, which is approximately given for our experiment since the electron beam current was approximately constant.

The energies and relative intensities of the examined lines of the platinum isotopes are shown in Table I. Note that the relatively big uncertainties in the absolute intensities are responsible for the major part of the errors in our results as seen in Table II.

For the calculation of the factor $`N_{\mathrm{decay}}/N_{\mathrm{total}}`$, precise knowledge of the half-lives of the produced unstable platinum isotopes is necessary. Because of that, those half-lives have been determined in an additional measurement .

### E Determination of the photon flux

For the approximation of the thermal Planck spectrum the precise shape of the different bremsstrahlung spectra especially in the high energy region had to be determined. Therefore Monte Carlo simulations using the computer code GEANT  were performed. To check the uncertainties of the GEANT calculations ($`\gamma `$,$`\gamma ^{}`$) measurements of well known 11B lines have been performed during the irradiation of the platinum samples in order to normalize the GEANT generated photon spectra. At the energies of these 11B lines, the absolute photon flux could be calculated. For these calculations, the efficiencies of the two detectors used for the measurement during the irradiation of the platinum samples had to be calibrated up to the energy of 10 MeV (see Sect. III F).

However, the shape of the bremsstrahlung spectra derived from the results of the ($`\gamma `$,$`\gamma ^{}`$) measurements and the spectra from the GEANT calculations show deviations near the endpoint energy. Unfortunately, the shape of the bremsstrahlung spectra could not be determined by the 11B lines alone, because there are only two lines (see Tab. III) in the high energy region.

Therefore, we tried to reproduce the measured 11B lines by using theoretical formulas. The energy distribution of bremsstrahlung is approximately given by the Schiff formula . However, this formula is only valid for bremsstrahlung from thin radiator targets, which means that each electron participates only in one scattering process and therefore emits only one photon. In our experiment, the electron beam was completely stopped within the radiator target. Thus, neither the Schiff formula nor newer approximation formulas given by Seltzer and Berger  reproduce the shape of our bremsstrahlung spectra with sufficient accuracy. Especially in the high energy region, the deviations are still considerable.

Therefore, the shape of the bremsstrahlung spectra was interpolated in the high energy region between 80 % and 100 % of the endpoint energy using cubic splines with the 11B lines as points of support. Unfortunately, in the spectrum with the lowest endpoint energy of 7650 keV, no 11B line can be seen in the relevant energy region. Therefore, no points of support are available for the spline interpolation of this spectrum. So we adjusted the GEANT calculated spectra in the high energy region by multiplying an energy-dependent correction factor F:

$$F=\{\begin{array}{cc}\hfill 1510^4\left(\frac{E0.8E_0}{\mathrm{keV}}\right)^{3/4};& E>0.8E_0\hfill \\ \hfill 1;& E0.8E_0\hfill \end{array}$$
(9)
where $`E_0`$ is the endpoint energy of the respective bremsstrahlung spectra. The shapes of the bremsstrahlung spectra resulting from both methods are shown in Fig. 4 for all measured endpoint energies. The results of the spline interpolation are represented by the dashed lines, the results of the GEANT simulations multiplied by the correction factor $`F`$ are represented by the straight lines. The good overall agreement between these curves and the data points of the 11B measurements is quite satisfactory. Since the spline interpolation is not reliable for the spectrum with 7650 keV endpoint energy, we used the bremsstrahlung spectra adjusted by the correction factor $`F`$ for the calculations of the reaction rates. The correction factor $`F`$ leads to a significant reduction of the photon flux close to the endpoint energy $`E_0`$. A precise knowledge of this energy region is essential for the superposition of the quasi-thermal spectrum. If one neglects this correction in the bremsstrahlung spectra, the reaction rates are underestimated by up to a factor of 2.

### F Determination of detector efficiencies

#### 1 Detectors for photon flux normalization

The calibration measurement was performed in two steps. First, a measurement of the absolute efficiency using 60Co, 137Cs, and 22Na calibration sources was performed. This was followed by a second measurement using a 56Co source. Since the intensity of this source was not calibrated, only a relative efficiency could be determined, but these data points were adjusted to fit those of the absolute efficiency measurement. Since there were no decay lines of these sources at energies above 3548.3 keV, an additional GEANT calculation was performed to determine the efficiency in the high energy region.

As can be seen in Fig. 5, the results of the measurement and the calculation correspond well with each other, and it has been shown that the detection efficiencies of large volume HPGe detectors can be calculated with good accuracy . The decrease in the efficiency at low energies results from lead and copper filters which were mounted in front of the detectors in order to reduce low energy background.

#### 2 Detector for activation measurements

Because the activity of the platinum samples was relatively low, they have been mounted directly in front of the 30 % HPGe detector used for the activation measurement. Since the activity of the available calibration sources was much higher, only a small number of lines could be used for the calibration measurements of the HPGe detector. However, some of the calculated data points for the efficiency still have relatively big errors, as is shown in Fig. 6. These errors are mainly due to summing effects resulting from the high count rate of the detector. For the calculations we used a doubly logarithmic interpolation of the data points in the relevant energy interval.

It had to be considered that due to the thickness of the platinum disks of 0.125 mm a portion of the emitted $`\gamma `$ rays was absorbed within the disks. This portion has been estimated using the computer code GEANT. The necessary corrections were of the order of a few percent, except for the 77.4 keV line of the 197Pt, where approximately two thirds of the $`\gamma `$ rays were absorbed within the platinum sample.

## IV Experimental results

### A Results for the cross section $`\sigma _{(\gamma ,n)}`$

The cross section parameters $`\sigma _0`$ from Eq. (4) have been calculated twice for every isotope, using both the spline interpolated and the by the factor $`F`$ corrected photon spectra. The two results are given in Tab. II, averaged over all measurements with different endpoint energies.

For 190Pt an additional measurement has been performed. This was necessary because the evaluation of the 190Pt lines was close to the statistical limit. For this measurement the platinum target was placed directly behind the radiator target because of the much higher photon flux. In this target position the ($`\gamma `$,$`\gamma ^{}`$) lines of the 11B samples could not be measured. Therefore, the shape of the photon spectrum could not be determined. However, since the neutron separation energies of 190Pt and of 192Pt are close to each other (Tab. II), we were able to calculate the ratio of the cross sections of these isotopes by determining the ratio of the number of counts in their respective lines. Then we calculated the cross section of 190Pt by multiplying this ratio with the known value for the cross section of 192Pt from the previous measurement. This value is considered in the average in Tab. II.

For the calculation of errors, the uncertainties in the detector efficiencies, the statistical errors from the number of counts in the respective peaks and the errors in the relative and absolute intensities of the decay lines have been considered. In order to estimate the error resulting from the uncertainty in the shape of the photon spectra, we calculated the mean difference of the interpolated spectra and the spectra which were adjusted by the correction factor $`F`$. For 190Pt an additional error of 7% has been considered, resulting from an uncertainty in the natural abundance of this isotope.

### B Results for the $`(\gamma ,n)`$ reaction rates

The ($`\gamma `$,n) reaction rates $`\lambda `$ have been determined from $`\sigma _0`$ and with the superposition method (see Sect. III). With both methods, the reaction rates in the complete relevant temperature region ($`T_9=23`$) have been calculated. The results are given in Tables IV, V, and VI. These results are averaged over all evaluated lines of the respective isotopes. For the superposition of the bremsstrahlung spectra, the bremsstrahlung spectra adjusted by the correction factor $`F`$ of Eq. (9) have been used. For the conventional method, only the values of $`\sigma _0`$ calculated with the corrected photon spectra have been used in order to be able to compare the results of both methods. For the isotope 190Pt the superposition method could not be used because the decay lines of 189Pt could not be evaluated in all measurements. For this isotope the average value of $`\sigma _0`$ which is given in Tab. II has been used for the calculation in the conventional method. The relative errors for the reaction rates calculated by the conventional method are the same as the error for the parameter $`\sigma _0`$.

The temperature dependence of the reaction rates is shown in Fig. 7 for the isotopes 190Pt, 192Pt, and 198Pt. The given values are calculated using the superposition method. The comparison of the results of both methods shows good overall agreement. The error of the conventional method seems to be smaller than the error of the superposition method because of the additional error resulting from the difference between thermal and superposed photon spectra. It has to be pointed out that the most important systematic uncertainty in the conventional method cannot be estimated, i.e. the uncertainty how good Eq. (4) approximates the shape of the cross section energy dependence. Therefore, the superposition method should prove much more reliable.

### C Comparison with other results

In Fig. 8 our result for the ($`\gamma `$,n) cross section of the isotope 198Pt is compared with a previous experiment by Goryachev et al. . They measured the ($`\gamma `$,n) cross section at various energies in and below the GDR region whereas we determined the cross section parameter $`\sigma _0`$. Therefore a comparison of both results is only possible if one assumes the behavior of the cross section to follow Eq. (4). Since this parametrization only holds in the vicinity of the threshold energy, the deviations at higher energies are not surprising.

Previous direct experiments had to be performed with huge amounts of highly enriched target material of the order of several grams. Such an amount of highly enriched material is not available for the low abundant platinum isotopes 190Pt and 192Pt, and hence no data exist in literature for these isotopes and for the p isotopes of other elements . To our knowledge our data are the first experimental ($`\gamma `$,n) cross sections and astrophysical reaction rates measured for the p-nuclei.

## V Theoretical consideratons

### A Calculation of laboratory and stellar rates

Experimental data can only provide photodisintegration rates of targets in their ground state. In a stellar plasma of the required temperature and density, nuclei are thermally equilibrated with their environment and therefore also excited states will be populated. The laboratory cross section $`\sigma _{(\gamma ,\mathrm{n})}^{\mathrm{lab}}=_\nu \sigma ^{0\nu }`$ has to be replaced by the stellar cross section

$$\sigma ^{}(E,T)=\frac{\underset{\mu }{}(2J^\mu +1)\mathrm{exp}(E^\mu /kT)\underset{\nu }{}\sigma ^{\mu \nu }(E)}{_\mu (2J^\mu +1)\mathrm{exp}(E^\mu /kT)},$$
(10)
where $`\mu `$ and $`\nu `$ denote the target states and the states in the final nucleus, respectively. Depending on plasma temperature $`T`$, spins $`J^\mu `$ and location $`E^\mu `$ of the target states, the stellar cross section can become considerably different from the one measured in the laboratory.

Up to now, astrophysical photodisintegration rates were calculated in a purely theoretical way by deriving them from capture rates via detailed balance (e.g. ). It should be noted that only stellar capture rates can be used to correctly apply detailed balance and, vice versa, only stellar photodisintegration rates can be used for the derivation of the respective stellar capture rates. Those stellar capture rates are usually also calculated theoretically. Detailed balance is valid for exoergic reactions ($`Q>0`$) and it has recently been shown that it is still quite accurate for charged particle capture with $`Q<0`$ .

Nevertheless, laboratory measurements are an important way to check the validity of the involved assumptions and the nuclear properties needed for the prediction of cross sections and rates. A direct measurement of the ($`\gamma `$,n) cross section can not only test detailed balance but also the description used for the low-energy tail of the GDR and the neutron optical potential for nuclei in excited states. Measurements using neutron capture are more limited in this respect.

Here, we compare the experimental results to calculations with the statistical model code NON-SMOKER . For the calculations presented here, the code NON-SMOKER was modified in such a way to be able to calculate photodisintegration reactions directly instead of deriving them via detailed balance (like e.g. in Ref. ). This modification also allows to compute rates for targets in the ground state which can easily be compared to our experimental results. The theoretical results are collected in Tab. VII and a comparison to the data is shown in Tab. VIII.

### B Discussion

In general, the theoretical rates are in good agreement with the present data, as can be seen from Tab. VIII. For the global statistical model calculations compared here, a typical average deviation of the order of 30 % should be expected but locally larger deviations up to a factor of two are possible. In this sense, the agreement is excellent for 198Pt and acceptable for the other isotopes, depending on which error is used. A visible trend of the accuracy with mass cannot be established.

The temperature dependence of the ratios from Tab. VIII can, in principle, be used to study how well the energy dependence of the cross section is reproduced. The latter, in turn, is mainly determined by the low-energy tail of the GDR. In addition, there is a weaker dependence on the neutron potential in the exit channel. The effect of possible inaccuracies in the theoretical description of those properties are weakened, however, by the smoothing due to the integration over the effective Gamow-like energy window in the derivation of the rate. A direct comparison of cross sections may be more sensitive but the relevant quantity for astrophysics is the reaction rate.

As discussed before (Sec. IV B), the values derived by the use of the conventional method agree well with those of the superposition method, indicating that the threshold behavior of the ($`\gamma `$,n) cross section is roughly reproduced by Eq. (4). This is supported by the comparison to the ($`\gamma `$,n) cross sections of Ref. . However, it cannot be expected in general that the cross section exhibits a structureless behavior proportional to $`\sqrt{EE_{\mathrm{thr}}}`$. The astrophysically relevant cross section depends on the dipole strength distribution in a narrow region above the threshold. Therefore, it is of importance to study this strength distribution experimentally. It is well known that the E1 strength exhibits significant fine structure like the so-called ‘pygmy resonance’ close to the particle threshold . The presence or absence of such a strength accumulation can change the astrophysical reaction rates significantly, while it will affect the position and width of the Gamow-like window on a small scale only.

There seem to be minor deviations between the two methods at $`T_9=2.0`$ for 198Pt and at $`T_9=3.0`$ for 192Pt. These minor discrepancies can be explained by the fact that the assumed threshold behavior of the cross section underestimates the cross section at higher energies (see also Fig. 8) which leads to a somewhat smaller slope of the reaction rate in the conventional analysis.

Within the errors the temperature dependence of the theoretical rates agrees with the data. Oddly enough, there seems to be a slight difference for 198Pt which is otherwise reproduced best. However, further conclusions can only be drawn pending a reduction of the experimental error bars.

Since the theoretical ($`\gamma `$,n) values have been confirmed for laboratory rates, detailed balance can be tested by comparing our stellar rates to the stellar photodisintegration rates derived from stellar neutron capture rates, as provided in Refs. . We find perfect agreement in all cases, confirming the validity of detailed balance.

As can be seen from Tab. VII, the stellar rates are larger by several orders of magnitude than the laboratory rates due to the facilitation of photodisintegration for thermally excited targets. This effect is sensitive to the used level density and structure but cannot be directly tested in the laboratory.

## VI Summary and conclusions

It has been shown that a thermal distribution of photons at astrophysically relevant temperatures can be simulated by the appropriate superposition of several bremsstrahlung spectra with different endpoint energies. Several platinum samples were irradiated with this quasi-thermal photon spectrum, and the ($`\gamma `$,n) reaction of 190Pt, 192Pt, and 198Pt was analyzed using the photoactivation technique. The high sensitivity of this method allows the measurement of the ($`\gamma `$,n) reaction even for isotopes with very low natural abundances.

The measured reaction rates in the laboratory have been compared to a statistical model calculation, and good agreement was found for all analyzed isotopes. Furthermore, stellar reaction rates have been calculated which are enhanced by the thermal population of excited states in the target nucleus.

These photon induced reactions are important for the nucleosynthesis of the neutron-deficient p-nuclei which are synthesized in the astrophysical $`\gamma `$ process in supernova explosions at temperatures of $`T_9=23`$. Almost no experimental data exist for the reactions relevant for the $`\gamma `$ process. For a better understanding of the $`\gamma `$ process more experimental data for ($`\gamma `$,n) and ($`\gamma `$,$`\alpha `$) reactions in the astrophysically relevant energy region are required. A systematic study is necessary to verify the predictions of statistical model calculations.

###### Acknowledgements.

We thank the S–DALINAC group around H.-D. Gräf for the reliable beam during the photoactivation and U. Kneissl and A. Richter for valuable discussions. This work was supported by the Deutsche Forschungsgemeinschaft (contracts Zi 510/2-1 and FOR 272/2-1). T. R. is supported by a PROFIL professorship from the Swiss National Science Foundation (grants 2124-055832.98, 2000-061822.00) and by the NSF (grant NSF-AST-97-31569).


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# Mixed State Entanglement: Manipulating Polarisation-Entangled Photons

## I Introduction

Since the foundations of quantum mechanics were laid, one of its most curious, and perhaps defining, features has been entanglement. Historically this has been discussed with regard to questions of nonlocal behaviour of quantum systems, a consequence of the famous EPR paper  and subsequent work by Bell . In the past decade the focus has shifted to a more information-theoretic interpretation of entanglement in line with the global effort to understand and eventually build a quantum computer. Quantum computing is not the only avenue that has motivated interest. In more immediate terms, realistic endeavours involve quantum cryptographic schemes, dense coding and teleportation as well as general questions regarding quantum information . While the realisation of a quantum computer is a long term goal, these pursuits are motivating an enormous amount of cross-disciplinary collaboration in questioning some of the fundamentals of quantum mechanics, information theory, and how the two are related.

The centerpiece of much of this work is entanglement. Quantifying, generating, distributing and maintaining entanglement make up the cornerstones of an enormous amount of research in quantum information science. A means of manipulating entanglement will be vital in distributing and maintaining entanglement, and photons provide the most realistic and accessible means of achieving this. In this paper we refine an experimentally realisable  protocol for manipulating arbitrary states of polarisation entangled photons which we have previously introduced. This scheme has been significantly improved and we provide here extensive analysis of the protocol in the context of entanglement transformations. This scheme specifically targeted mixed states, as experimentally it is unrealistic to consider the system isolated from interactions with the environment. We would also like to connect some of the mathematical concepts regarding entangled mixed states with a more intuitive and realistic experimental proposal. In terms of manipulating a state’s entanglement and purity there was a proposal of Kent et al.  pertaining to the requirements for an optimal entanglement transformation. This is all performed in the context of local filtering operations and in this paper we will show how and why this works in a system using polarisation entangled photons and allowing for imperfect photo-detection.

As only two qubit states are considered, an exact expression for the Entanglement of Formation ($`EOF`$), introduced by Wooters , will be used.

The $`EOF`$ is

$`E(C(\rho ))`$ $`=`$ $`h\left(\left[1+\sqrt{1C(\rho )^2}\right]/2\right)`$ (1)
where $`h`$ is the binary entropy function,

$$h(x)=x\mathrm{log}(x)(1x)\mathrm{log}(1x)$$
(2)
This is derived in terms of the spin flip operation

$$\stackrel{~}{\rho }=(\sigma _y^A\sigma _y^B)\rho ^{}(\sigma _y^A\sigma _y^B)$$
(3)
where $`\sigma _y`$ are Pauli operators and the complex conjugation is taken in the computational basis. From this the Concurrence can be found

$`C(\rho )=\mathrm{max}\{\stackrel{~}{\lambda }_1\stackrel{~}{\lambda }_2\stackrel{~}{\lambda }_3\stackrel{~}{\lambda }_4,0\}`$ (4)
where the square root of the eigenvalues for $`\rho \stackrel{~}{\rho }`$, $`\stackrel{~}{\lambda _i}`$, are sorted into descending order.

The other characteristic that is considered here is the purity of the state and the von Neumann Entropy provides a convenient and useful measure. The entropy of the bipartite density matrix, $`\rho _{AB}`$, is

$`S(\rho _{AB})=\mathrm{Tr}\left[\rho _{AB}\mathrm{log}_4\rho _{AB}\right]`$ $`=`$ $`{\displaystyle \underset{i=1}{\overset{4}{}}}\lambda _i\mathrm{log}_4\lambda _i`$ (5)
where $`\lambda _i`$ are the eigenvalues of $`\rho _{AB}`$. In the latter form this is analogous to the classical Shannon entropy. The $`\mathrm{log}`$ to base 4 is used as this is the joint state, and hence in this form returns a normalised entropy ranging from zero, for a pure state, to one for the Identity or totally mixed state.

For a correlated system the entropy of the whole system is less than the entropy of its parts due to the information that is present in the correlations between the two systems. For a maximally entangled pure state $`S(\rho _A)=S(\rho _B)=\mathrm{log}(2)`$ and $`S(\rho _{AB})=0`$. How the state was prepared cannot be determined by considering measurements on the two subsystems. The correlation in the joint state measurements must be considered.

The characteristics of the entropy for a mixed state, regarding both the joint state and local subsystem, will be useful when discussing state transformations. The entropy provides a key element in discussing bounds on the Hilbert space associated with mixed states in the context of state manipulation in general and the scheme introduced here. These concepts will be discussed primarily in terms of a proposed bound on mixed state entanglement enhancement  that requires the subsystem entropies to be maximised.

## II Entanglement Manipulation using Beam Splitters

The entanglement manipulation protocol that is to be introduced here relies on the very simple process of filtering, a method proposed by several people  as a means of manipulating entangled states. This protocol is conceptually similar to the Procrustean Method introduced by Bennett et al.  which dealt with pure states of entangled spin-half particles, in a very generic way.

Our aim is for two parties, $`A`$ and $`B`$, who are spatially separated, to share the optimal entanglement available. The qubits we consider here are polarisation states, where $`|V,|H`$ correspond to the $`|0,|1`$ states within the standard computational basis.

The schematic in Figure (1) represents the proposed manipulation protocol which will be referred to from here on as the Beam Splitter Protocol. Everything to the left of, and including, the BBO (Beta-Barium-Borate) crystal and decohering elements (DEs) are representative of the source that can supply the initial entangled states that we propose to manipulate. The first Polarising Beam Splitter (PBS) at the input, before the crystal, varies the weighting of a superposition state which is then Down-converted at the Parametric crystal generating pure entangled pairs. The decohering elements, after the crystal, vary the mixedness of the state. The recent advances in the preparation of non-maximally entangled pure  and mixed  polarisation-entangled states allows for the consideration of a wide variety of initial states, with high production rates for the entangled photons.

The scheme operates in the following manner. The output from the crystal, the two arms labelled signal and idler, are incident on PBSs, spatially separating the vertical and horizontal polarisation modes of the two separate beams. These modes will be labelled, $`|V_A,|H_A,|V_B,|H_B`$. Both the polarisation modes, $`V`$ and $`H`$, in both the arms, $`A`$ and $`B`$, will then be incident on Variable Beam Splitters (VBSs). These variable beam splitters can then be adjusted to obtain the desired output state dependent on the transmission coefficient, $`\eta `$, for each mode. This transmission is polarisation dependent. Due to low detector efficiencies, in this protocol the reflected modes are ignored and the final state that is considered is the state that has coincidence detections at both $`A`$ and $`B`$. This will be justified shortly.

All four Bell-type states will be considered here. A mixture of two of these non-maximally entangled Bell-type states,

$`|\varphi ^\pm _{AB}=\mathrm{cos}\theta _1|VV_{AB}\pm \mathrm{sin}\theta _1|HH_{AB}`$ (6)
$`|\psi ^\pm _{AB}=\mathrm{cos}\theta _2|VH_{AB}\pm \mathrm{sin}\theta _2|HV_{AB}`$ (7)
will be used to illustrate the extension from pure to mixed state manipulation. The degree of entanglement in each of these states is determined by the value of $`\theta `$, i.e. a maximally entangled state will have equal weighting of the coefficients, $`\theta _{1,2}=\pi /4`$.

When we consider a beam splitter interaction we must also consider that as well as the incident mode, the other port of the beam splitter is subject to the vacuum and similarly the output will also have two modes. The effect that the beam splitters have on a polarisation-entangled state is to transform the modes in the following way

$`|V,H_{AB}|0\eta _{V,H}|V,H_{AB}|0+\sqrt{(1\eta _{V,H}^2)}|0_{AB}|1`$ (8)
This can be interpreted as the vertical or horizontal modes being passed by the beam splitter with a probability $`\eta _{V,H}^2`$, with a component at the reflected port that now has a photon in an ancilla mode with a probability $`(1\eta _{V,H}^2)`$. This approach has a similar interpretation to those found by modelling imperfect detectors as a perfect detector plus a beam splitter attenuating the input field .

It is easy to determine how a single beam splitter in one arm of the system could be coupled to a specific vertical or horizontal mode. It is not much harder to do this for a beam splitter at $`A`$ and $`B`$, however, we wish to introduce two beam splitters, both vertical and horizontal, to each polarisation arm of the system. This couples a controllable variable, the transmission coefficient, to each mode, where the four variable beam splitters act independently on the four polarisation modes of the bipartite system.

Consider a non-maximally entangled pure state of the form of eq.(7). After interactions with all four of the variable beam splitters, the final state, before anything is discarded, is

$`|\psi _{tot}`$ $`=`$ $`\stackrel{~}{𝒩}\{[\mathrm{cos}\theta \eta _{VA}\eta _{HB}|VH_{AB}\pm \mathrm{sin}\theta \eta _{HA}\eta _{VB}|HV_{AB}]|00`$ (9)
$`+\mathrm{cos}\theta \eta _{VA}\sqrt{(1\eta _{HB}^2)}\left(|V0_{AB}|01+|0H_{AB}|10\right)`$ (10)
$`\pm \mathrm{sin}\theta \eta _{HA}\sqrt{(1\eta _{VB}^2)}\left(|V0_{AB}|01+|0H_{AB}|10\right)`$ (11)
$`+\mathrm{cos}\theta \sqrt{(1\eta _{VA}^2)}\sqrt{(1\eta _{HB}^2)}|00_{AB}|11`$ (12)
$`\pm \mathrm{sin}\theta \sqrt{(1\eta _{HA}^2)}\sqrt{(1\eta _{VB}^2)}|00_{AB}|11\}`$ (13)
The modes can be interpreted as those labeled $`AB`$ being the transmitted modes and the others being the ancilla. Also, for convenience, information regarding the polarisation of the photons in the ancilla modes has been discarded and a simple record of whether there is, or isn’t, a photon in a reflected port at $`A`$ or $`B`$, which is all that is required, has been kept.

It has been remarked previously that due to low detector efficiencies the reflected component is ignored and the state with coincidence detection at $`A`$ and $`B`$ is considered. In eq.(9) it can be seen that the only components of the state having coincidence detections at $`A`$ and $`B`$ are the two components on the first line. This can be considered to be a coincidence basis state. The coincidence basis state is the state that would have coincidence detections at both $`A`$ and $`B`$, i.e. detections for any of $`\{|VV_{AB},|VH_{AB},|HV_{AB},|HH_{AB}\}`$. Alternatively, if it was at all possible to efficiently detect single photons, then perfect single-photon detectors could replace each of the beam blocks in the signal and idler arms in Figure (1b). This would allow the system to operate a gate-like device at the output that, with the aid of classical communication between $`A`$ and $`B`$, was open and letting maximally entangled pairs through as long as a detection is made at one of the previously discarded ports. Again with reference to eq.(9), if this condition was satisfied then the output state to which $`A`$ and $`B`$ would have access corresponds to what has been referred to as the coincidence basis state. As perfect photodetection is not a realisable process with current technologies, the beam blocks remain and the state having joint coincidences for $`A`$ and $`B`$ is considered. This leaves a reduced output state

$`|\psi _f=𝒩\left[\eta _{VA}\eta _{HB}\mathrm{cos}\theta |VH_{AB}+\eta _{HA}\eta _{VB}\mathrm{sin}\theta |HV_{AB}\right]`$ (14)
with the normalisation

$$𝒩=\left[\eta _{VA}^2\eta _{HB}^2\mathrm{cos}^2\theta +\eta _{HA}^2\eta _{VB}^2\mathrm{sin}^2\theta \right]^{1/2}$$
(15)
This is a post-selective operation, selecting a subensemble with improved entanglement characteristics and discarding the rest of the ensemble. If no detection is made then the state can be jointly discarded by both $`A`$ and $`B`$. This post-selective process has the advantage that poor detector efficiencies only decrease the coincidence count rate. The requirement for a maximally entangled state is therefore given by

$$\mathrm{cos}^2\theta \eta _{VA}^2\eta _{HB}^2=\mathrm{sin}^2\theta \eta _{HA}^2\eta _{VB}^2$$
(16)
If $`\mathrm{cos}\theta >\mathrm{sin}\theta `$ then either $`\eta _{VA}`$ or $`\eta _{HB}`$, or both, can be varied such that $`\eta _{VA}^2\eta _{HB}^2=\mathrm{tan}^2\theta `$, thus obtaining a maximally entangled state with probability

$$P=2\mathrm{sin}^2\theta $$
(17)
which constitutes an optimal transformation for single-copy pure states . The probability of producing the maximally entangled pure state for this protocol is dependent on the beam splitter transmission coefficients and is determined from the trace of the reduced output state density matrix. This is the probability of obtaining the desired state after the beam splitter settings are determined.

This provides an intuitively simple explanation of this process, for pure states at least, but if mixed states are to be considered then a more convenient representation can be obtained by using the generalised measurement formalism. This procedure constitutes a generalised measurement in that an ancilla is attached to the system, unitary transformations are performed in the extended Hilbert space where measurements are made and then part of the system is traced out and discarded .

As we are only interested in the coincidence basis output state, an equivalent local filtering operation can be derived that retains the polarisation coupling characteristics derived for the pure state case. Therefore an effective transmission matrix for the joint system can be written

$`(AB)`$ $`=`$ $`\left[\begin{array}{cccc}\eta _{VA}\eta _{VB}& 0& 0& 0\\ 0& \eta _{VA}\eta _{HB}& 0& 0\\ 0& 0& \eta _{HA}\eta _{VB}& 0\\ 0& 0& 0& \eta _{HA}\eta _{HB}\end{array}\right]`$ (22)
It can easily be seen that this effective transmission matrix allows for the completely positive mapping of the input state to the coincidence basis output state. The total state transformation matrix is operating in an Hilbert space considerably larger than the original state space, and in this expanded Hilbert space there is now a greater degree of freedom in which to manipulate the state. This is, in part, where the original Procrustean Method obtained its name in that it takes an initial state, places it in an extended Hilbert space, and then manipulates and discards anything not needed.

Thus with all the transmission coefficients acting independently on the $`\{|V_A,|H_A,|V_B,|H_B\}`$ modes, the transmission matrix of eq.(22) represents the Beam Splitter manipulation process. This process is analogous to many of the filtering operations that have been proposed . Any of the beam splitter transmission coefficients $`\eta _{VA},\eta _{HA},\eta _{VB},\eta _{HB}`$, can be manipulated individually or in unison. The key feature of this proposal is that each polarisation mode in $`A`$ and B can be manipulated independently. The degree of freedom that this protocol provides means that a wide variety of operations for transforming a bipartite system can be satisfied.

The output state, or more specifically, the reduced coincidence basis output state, can now be written in the form

$`\widehat{\rho }_{out}={\displaystyle \frac{AB\widehat{\rho }_{in}A^{}B^{}}{\mathrm{Tr}[AB\widehat{\rho }_{in}A^{}B^{}]}}`$ (23)
This state describes the subensemble that passes the filtering process and would have coincidence detections at $`A`$ and $`B`$. The probability of this state being realised is given by

$`P=\mathrm{Tr}[AB\widehat{\rho }_{in}A^{}B^{}]`$ (24)
The only restriction on these operations is that they must satisfy $`A^{}AI`$ and $`B^{}BI`$, being completely positive maps .

The case of pure states provided a straightforward example of how this protocol works. So far though, only two of the Bell-type states have been considered. To illustrate the transmission matrix method and cover the other Bell state variants, consider the pure state

$$|\varphi ^\pm _{in}=\mathrm{cos}\theta |VV\pm \mathrm{sin}\theta |HH$$
(25)
This state has the explicit density matrix representation

$`\widehat{\rho }_{in}`$ $`=`$ $`\left[\begin{array}{cccc}\mathrm{cos}^2\theta & 0& 0& \pm \mathrm{cos}\theta \mathrm{sin}\theta \\ 0& 0& 0& 0\\ 0& 0& 0& 0\\ \pm \mathrm{cos}\theta \mathrm{sin}\theta & 0& 0& \mathrm{sin}^2\theta \end{array}\right]`$ (30)
If we apply the Transmission matrix to this state then the output state, given the matrix notation, is

$`\widehat{\rho }_{out}`$ $`=`$ $`{\displaystyle \frac{1}{P}}\left[\begin{array}{cccc}\eta _{VA}^2\eta _{VB}^2\mathrm{cos}^2\theta & 0& 0& \pm \overline{\eta }\mathrm{cos}\theta \mathrm{sin}\theta \\ 0& 0& 0& 0\\ 0& 0& 0& 0\\ \pm \overline{\eta }\mathrm{cos}\theta \mathrm{sin}\theta & 0& 0& \eta _{HA}^2\eta _{HB}^2\mathrm{sin}^2\theta \end{array}\right]`$ (35)
with $`\overline{\eta }=\eta _{VA}\eta _{HA}\eta _{VB}\eta _{HB}`$, and the probability is given by the trace of the unnormalised, beam-splitter-transformed, density matrix

$`P`$ $`=`$ $`\eta _{VA}^2\eta _{VB}^2\mathrm{cos}^2\theta +\eta _{HA}^2\eta _{HB}^2\mathrm{sin}^2\theta `$ (36)
A maximally entangled state is recovered from the coincidence basis output state

$$|\varphi ^\pm _{out}=\frac{1}{\sqrt{P}}\left[\eta _{VA}\eta _{VB}\mathrm{cos}\theta |VV\pm \eta _{HA}\eta _{HB}\mathrm{sin}\theta |HH\right]$$
(37)
providing the requirement for a maximally entangled state

$`\mathrm{cos}\theta \eta _{VA}\eta _{VB}`$ $`=`$ $`\mathrm{sin}\theta \eta _{HA}\eta _{HB}`$ (38)
$`{\displaystyle \frac{\eta _{VA}\eta _{VB}}{\eta _{HA}\eta _{HB}}}`$ $`=`$ $`\mathrm{tan}\theta `$ (40)
are met. If $`\mathrm{cos}\theta >\mathrm{sin}\theta `$ then either $`\eta _{VA}`$ or $`\eta _{VB}`$, or both, can be varied producing a maximally entangled state with probability $`P=2\mathrm{sin}^2\theta `$. Conversely, if $`\mathrm{cos}\theta <\mathrm{sin}\theta `$ then varying $`\eta _{HA}`$ or $`\eta _{HB}`$, would yield a maximally entangled state with probability $`P=2\mathrm{cos}^2\theta `$. It could be argued that this constitutes nothing more than a simple variation on the Procrustean Method  and requires only filtering at either $`A`$ or $`B`$ to distill maximally entangled pure states. The reason for having four individually tunable filters is perhaps not clear yet, and though there is obviously a large degree of freedom in controlling the system, the necessity will become more apparent as the mixed state case is investigated.

## III Mixed States Manipulation

It is the aim of this section to show how the Beam Splitter Protocol can be extended from pure state manipulation to deal with the more complicated mixed state manipulation. To aid in the understanding of how the protocol can realise this, a state which involves a mixture of two of the non-maximally entangled pure states already discussed will be be introduced. The degree of entanglement of each of the states can be varied as a function of $`\theta _{1,2}`$ and the mixing of the two will be determined by another parameter $`\gamma `$, such that the state has the density matrix representation

$`\widehat{\rho }(\gamma )`$ $`=`$ $`\gamma |\varphi ^+\varphi ^+|+(1\gamma )|\psi ^+\psi ^+|`$ (41)
where $`|\varphi ^+`$ and $`|\psi ^+`$ correspond to positive variants of eq.(6) and eq.(7) respectively. This state will be discussed in terms of the effect that varying the entanglement and mixing of the components has on the entropy and entanglement of the system. In Figure (2) the variation in the entanglement of the system and the entropy of the joint and subsystems is compared as the degree of mixing is varied. This illustrates the result where the entanglement of one of the pure states is not at a maximum and we see that the entanglement of the joint state decreases as the mixing is increased, with $`\gamma =0`$ corresponding to the maximally entangled pure state and $`\gamma =1`$ the non-maximally entangled pure state. When the state is not maximally entangled the subsystems are not totally mixed and hence the system tends towards the maximally entangled pure state characteristics as the subsystem entropies tend towards $`\mathrm{log}(2)`$, as $`\gamma `$ goes to zero.

Figure (3) illustrates where the entropy of the subsystems are not always equal and how the entanglement peaks when the two subsystem entropies are both equal. The two turning points where the entanglement goes to zero correspond to separable points, analogous to the case of equal mixtures of maximally entangled components, where the entanglement switches from a reliance on one entangled component to the other.

Already a great deal of complexity can be seen to be emerging from a consideration of the entanglement and entropy characteristics of a relatively simple system involving two polarisation-entangled qubits. This is before the extended Hilbert space is introduced via the Beam Splitter Protocol which itself introduces four new variables and hence a higher degree of complexity again.

For pure states the question of optimality of an entanglement transformation for single-copy bipartite states is known. If optimality of mixed states is taken as the most entanglement that can be realised from a state regardless of the joint state entropy, then the conditions to obtain this can be found by looking at the local density matrices of $`A`$ and $`B`$. The local density matrices are found by tracing over the degrees of freedom for the other subsystem, $`\rho _A=\mathrm{Tr}_B\left[\rho _{AB}\right]`$ and $`\rho _B=\mathrm{Tr}_A\left[\rho _{AB}\right]`$. In terms of this, the condition for a Bell diagonal, optimally entangled, state is that $`\rho _A=\rho _B=I_2`$, corresponding to totally mixed, or random, local density matrices with a maximum amount of entropy, a condition proposed by Kent et al. .

How do the entanglement-entropy characteristics for the state vary under the influence of the Beam Splitter Protocol? In Figure (4) the characteristics of a range of states that are obtainable, using the Beam Splitter Protocol, for a given initial state are plotted. A state of the form of eq.(41) is employed as this can be varied with respect to the mixture and the degree of entanglement of the two pure-state components, which have already been considered. The data points marked with a circle indicate the entanglement-entropy characteristics of the initial state and the solid lines represent a range of states that can be accessed by varying the beam splitters. The two figures are for a range of initial states determined by the mixing parameter, $`\gamma `$, which is labeled on each curve. The degree of entanglement of one component is reduced below that of a maximally entangled pure state.

Consider the case of $`\gamma =0.7`$ in Figure (4). This state has a mixing which is weighted slightly towards the maximally entangled component, and the other component has only a small degree of entanglement. It is the modes with higher probability of being realised in the less entangled component that are targeted by the Beam Splitter Protocol, $`\eta _{VA}`$ and $`\eta _{HB}`$, and hence the mixed state tends towards the maximally entangled pure state component. The maximally entangled component is never fully extracted in this instance as a result of the problem inherent in most mixed state manipulation protocols in that the transformations affect all components of the mixture, not just the component that needs to be removed.

This protocol relies on a certain amount of prior knowledge of the state. This knowledge helps determine the required parameters to concentrate the state characteristics. We consider concentration as increasing both the entanglement and purity of a state. Recent advances in quantum state Tomography  allow for the measurement and reconstruction of the complete density matrix for a bipartite state, allowing before and after comparisons.

So far the manipulation protocol has been introduced and shown to work for pure states, and it has also been shown to increase both the entanglement and purity of a state consisting of a mixture of pure states, one non-maximally entangled and another maximally entangled. The pure state transformations have been shown to be optimal, both in the sense that the most amount of entanglement is obtained by the transformation and the transformation is carried out with an optimal efficiency. Can this be extended to arbitrary mixed states? How this protocol works will constitute the majority of the next section, where this state, as well as a range of other states, will be considered and an attempt made to extrapolate some of the results to general systems. Chiefly, the beam splitter dependence on the joint state and the subsystems will be examined in greater detail to determine whether a state can be transformed, and if it can, what beam splitters need to be varied, and by how much, to obtain the most amount of entanglement for the state.

## IV Analysing Mixed States

The main focus of this paper is the Polarising Beam Splitter Protocol and mixed state entanglement, however, one of the reasons for actually wanting such a device lies in its ability to explore mixed-state Hilbert space. To further illustrate the capabilities of the protocol and at the same time investigate some recent proposals concerning entanglement and various concepts and bounds, a few states will be discussed in detail. To describe the manipulations of a state and look at questions regarding optimality and how these manipulations can be realised, it will be necessary to look at the eigenvalues for the joint system and local subsystems. In this section a more detailed investigation into the mixed state already introduced will firstly take place. The second state that will be looked at will be the Werner state and then finally a state that is a mixture of a pure entangled state and a separable component will be introduced and discussed with a view to determining a bound on the entanglement-entropy plane. A parameterised density matrix will finally evolve from this, and then the Beam Splitter Protocol and the state manipulations will be discussed again in the context of this bound.

### A Two Bell State Mixture

Consider again the state consisting of a mixture of two Bell-like states

$`\widehat{\rho }(\gamma )`$ $`=`$ $`\gamma |\varphi ^+\varphi ^+|+(1\gamma )|\psi ^+\psi ^+|`$ (42)
which has the explicit density matrix after the beam splitter interaction of

$`\stackrel{~}{\rho }=`$ $`{\displaystyle \frac{1}{P_B}}`$ $`[\gamma \left(\begin{array}{cccc}\eta _{VA}^2\eta _{VB}^2\mathrm{cos}^2\theta _1& 0& 0& \overline{\eta }\mathrm{cos}\theta _1\mathrm{sin}\theta _1\\ 0& 0& 0& 0\\ 0& 0& 0& 0\\ \overline{\eta }\mathrm{cos}\theta _1\mathrm{sin}\theta _1& 0& 0& \eta _{HA}^2\eta _{HB}^2\mathrm{sin}^2\theta _1\end{array}\right)`$ (47)
$`+`$ $`(1\gamma )\left(\begin{array}{cccc}0& 0& 0& 0\\ 0& \eta _{VA}^2\eta _{HB}^2\mathrm{cos}^2\theta _2& \overline{\eta }\mathrm{cos}\theta _2\mathrm{sin}\theta _2& 0\\ 0& \overline{\eta }\mathrm{cos}\theta _2\mathrm{sin}\theta _2& \eta _{HA}^2\eta _{VB}^2\mathrm{sin}^2\theta _2& 0\\ 0& 0& 0& 0\end{array}\right)]`$ (52)
with $`\overline{\eta }=\eta _{VA}\eta _{HA}\eta _{VB}\eta _{HB}`$ as previously, and where

$`P_B`$ $`=`$ $`\gamma \left[\eta _{VA}^2\eta _{VB}^2\mathrm{cos}^2\theta _1+\eta _{HA}^2\eta _{HB}^2\mathrm{sin}^2\theta _1\right]`$ (54)
$`+(1\gamma )\left[\eta _{VA}^2\eta _{HB}^2\mathrm{cos}^2\theta _2+\eta _{HA}^2\eta _{VB}^2\mathrm{sin}^2\theta _2\right]`$
To determine the conditions to optimise the entanglement, the reduced density operators for each of the subsystems need to be found. If the subsystem entropies are to be maximised, $`S_A=S_B=\mathrm{log}(2)`$, then the following constraints must be satisfied

$`\mathrm{tan}\theta _1={\displaystyle \frac{\eta _{VA}\eta _{VB}}{\eta _{HA}\eta _{HB}}}`$ (55)
$`\mathrm{tan}\theta _2={\displaystyle \frac{\eta _{VA}\eta _{HB}}{\eta _{HA}\eta _{VB}}}`$ (56)
As both the Entanglement of Formation and the Entropy are dependent on the eigenvalues of the system, it is beneficial to determine how these behave with regard to the subsystem constraints.

In satisfying the constraints on the local systems, the eigenvalues for the joint system simplify to

$`\lambda _1`$ $`=`$ $`2\gamma \eta _{VA}^2\eta _{VB}^2\mathrm{cos}^2\theta _1{\displaystyle \frac{1}{P_B}}`$ (57)
$`\lambda _2`$ $`=`$ $`2(1\gamma )\eta _{VA}^2\eta _{HB}^2\mathrm{cos}^2\theta _2{\displaystyle \frac{1}{P_B}}`$ (58)
Given this, consider the ratio of these eigenvalues:

$`{\displaystyle \frac{\lambda _1}{\lambda _2}}=\left({\displaystyle \frac{\gamma }{1\gamma }}\right){\displaystyle \frac{\mathrm{sin}2\theta _1}{\mathrm{sin}2\theta _2}}`$ (59)
Note that this ratio is independent of any transmission coefficients only when the subsystem constraints are satisfied. Thus by satisfying the subsystem constraints, the joint system requirements are also being realised in that the degree of mixing of the state is reduced as much as possible, given the parameters governing the initial state. When this ratio equals one, the joint system is maximally mixed and there is no entanglement present. Recall Figure (2), the entanglement minima corresponds to the point where $`\lambda _1/\lambda _2=1`$. For a maximally entangled state this is at $`\gamma =1/2`$ but if $`\theta \pi /4`$, then the minima will be appropriately shifted. Which one of the joint state eigenvalues will dominate is determined by both the mixing and the entanglement of the pure state components in the original mixture.

These constraints govern how much the state can be improved by the beam splitters. In general, the entanglement of a state is reduced as the degree of mixing is increased, and this provides a bound on the possible transformations for the state. By satisfying the local system constraints proposed by Kent et al., regarding optimal entanglement enhancement, the joint state eigenvalues obtain their optimal value.

### B Werner State

The Werner state can be considered as a weighted mixture of all four of the Bell states , a straightforward extension of the mixture of two Bell states just discussed. However, we consider the Werner state, in the form

$`\widehat{\rho }_w(\gamma )`$ $`=`$ $`(1\gamma ){\displaystyle \frac{I_4}{4}}+\gamma |\varphi ^+\varphi ^+|`$ (60)
where the initial state, $`|\varphi ^+`$, has a probability $`\gamma `$ of being transmitted without errors and there is a component $`(1\gamma )`$ of a totally mixed state. In the case where $`\gamma 1/3`$ the state is separable and as such has no entanglement to recover or maintain. If the pure state component of this mixture is maximally entangled then $`S_A=S_B=\mathrm{log}(2)`$ regardless of the degree of mixing and the state is as entangled as it can be. It is, perhaps, this characteristic that suggested it might provide a bound on how entangled a mixed state could be. If, however, the pure state component is not maximally entangled, this constraint does not hold.

If the Beam Splitter Protocol is now implemented on a Werner state, with a non-maximally entangled pure state component, then the constraints on the subsystem and joint state eigenvalues are determined, as in the case of the mixture of two Bell states previously. Firstly the subsystems are considered and the constraints that maximise the subsystem entropies are determined. The requirement for the local density matrices of the Werner state, post-beam splitters, to satisfy $`S_A=S_B=\mathrm{log}(2)`$ are

$`\eta _{VA}=\eta _{VB},`$ $`\eta _{HA}=\eta _{HB}`$ (61)
$`\mathrm{and}`$ $`\mathrm{tan}\theta ={\displaystyle \frac{\eta _{VA}^2}{\eta _{HA}^2}}`$ (62)
The joint system for the Werner state has four eigenvalues, which can be simplified using the previous constraints, and the ratios of the eigenvalues are again independent of the beam splitter coefficients, when the subsystem constraints are satisfied.

So, if the subsystem entropies can be made to equal $`\mathrm{log}(2)`$, the degree of mixing in the joint state is minimised with respect to the maximum amount of entanglement. Also, as there is no means of removing any of the eigenvalues, a relatively high degree of mixing will be inherent in the system even after the Beam Splitter Protocol. This mixing will however be the minimum obtainable while maintaining $`S_A=S_B=\mathrm{log}(2)`$. Immediately it can be seen, given the constraints of eq.(61) and eq.(62), that if $`\mathrm{tan}\theta 1`$, then by setting $`\eta _{HA}^2=\eta _{HB}^2=1`$ and $`\eta _{VA}^2=\eta _{VB}^2=\mathrm{tan}\theta `$, the mixing and entanglement are optimised.

In Figure (5) the entropies and the entanglement of the state are plotted as a function of the two transmission coefficients, $`\eta _{VA}`$ and $`\eta _{VB}`$. These two beam splitters are varied in unison, $`\eta ^2\eta _{VA}\eta _{VB}=\eta _{VA}^2`$, to satisfy the constraints on the subsystems. Given this, the entanglement of the state is maximised at the point where the entropy of the local subsystems reaches a maximum, $`\mathrm{log}(2)`$. The probability of the state with these characteristics being realised is also shown. When the state is as entangled as it can be (here an increase of around 20% is shown) it can be seen that the probability of obtaining this state is around 55%.

The variation in the entanglement-entropy characteristics, Figure (6), shows the results of individually varying the beam splitters, and the improvement that is achieved when they are varied in tandem. $`\eta _{VA}`$ and $`\eta _{VB}`$, when varied individually, increase the entropy at the cost of entanglement, but when varied in unison the increase in the entanglement is greater. The maximum entanglement in Figure (6) again corresponds to the point where $`\eta _{VA}^2=\eta _{VB}^2=\mathrm{tan}\theta 0.6`$.

A boundary curve has been introduced in Figure (6) (dotted line) onto the characteristic plane denoting the bound alluded to earlier for the Werner state, where the pure state component is maximally entangled. The curve denotes the characteristics as the $`\gamma `$ is varied. Regardless of whether the manipulations are made, individually or in unison, and how many beam splitters are utilised, the entanglement does not exceed this bound.

### C Entangled + Separable

In the preceding sections, discussion has revolved around mixtures of pure non-maximally entangled Bell states. The first, a mixture of two, and the second, a mixture of all four, and the behaviour of the characteristics of the state under the Beam Splitter Protocol have been observed. To observe the behaviour of a different class of state, a mixture of an entangled pure state and a separable state will now be considered, with the mixture having the form

$`\widehat{\rho }_{es}(\gamma )`$ $`=`$ $`\gamma |\psi ^+\psi ^+|+(1\gamma )|VVVV|`$ (63)
There are only two eigenvalues for the joint system, $`\lambda _1=\gamma ,\lambda _2=(1\gamma )`$, independent of $`\theta `$, however, the eigenvalues for the subsystems are dependent on both the mixing and the entanglement of the entangled component.

After the beam splitters, the eigenvalues for the subsystem and the constraints on the joint system are determined, resulting in two requirements, the first being that

$`\mathrm{tan}^2\theta ={\displaystyle \frac{\eta _{VA}^2\eta _{HB}^2}{\eta _{HA}^2\eta _{VB}^2}}`$ (64)
which is very similar to those constraints found for previous states. The second constraint poses an interesting problem, or perhaps it should be considered a feature. The second constraint requires that

$`\eta _{VA}^2\eta _{VB}^20`$ (65)
This implies that the subsystems are totally mixed only in the limit of no transmission. Previously, when the subsystem constraints were enforced on the joint system eigenvalues, the degree of mixing for the joint state had been minimised. In this instance the ratio of the eigenvalues is still dependent on the beam splitter transmission coefficients. As such, there is considerable control over the mixing of the state. This state falls in to the class of state that was recently shown by Verstraete et al.  that could be brought arbitrarily close to a Bell state by reducing the rank of the density operator.

The behaviour and the entanglement-entropy characteristics of this state, as the beam splitters are varied, is illustrated in Figure (7). The figure highlights the effects that both of these constraints have on the state characteristics.

The mixture consists of $`\gamma =0.3`$ of the entangled component and shows the results in the case where the two beam splitters are varied together, $`\eta _{VA}=\eta _{VB}`$. With these parameter settings the entropies of the subsystems are not equal, $`S_AS_B`$, and only in the limit as the transmission coefficients both go to zero do they converge, satisfying eq.(65), and when they do, they are not a maximum and hence the state is not maximally entangled.

If the first constraint, eq.(64), is satisfied and the transmission coefficients of the beam splitters are varied as $`\eta _{VA}=\eta _{VB}\mathrm{tan}\theta ,(\mathrm{tan}\theta 1)`$ then the behaviour is not that different from this case, except that the subsystem entropies are equal throughout the variation of the beam splitters and in the limit as the transmission tends to zero, the maximally entangled pure state characteristics are approached as $`S_A=S_B`$ approaches $`\mathrm{log}(2)`$. As this is achieved, the probability of obtaining these state characteristics tends to zero.

In Figure (8) the state is again considered and the behaviour of the characteristics on the entanglement-entropy plane examined. The dashed curve denotes the behaviour as the beam splitters are varied in tandem as in Figure (7), showing the pure but non-maximally entangled state characteristics being approached. The solid line shows the transformed states obtained by varying the beam splitters while satisfying both the subsystem constraints. This curve shown doesn’t pass through the circle marking the initial state characteristics, due to the fact that the initial state, numerically considered, has some $`\eta `$ dependence such that initial $`\eta 1`$, again due to the first constraint.

This state has already presented some quite unusual characteristics, however it can also be noted that for variations in the mixture and entanglement of this state, the same concentration characteristics as in Figure (8) are produced. In fact, this solid curve can be further extrapolated down the plane, for as long as there is some component of the entangled pure state present in the mixture, a state arbitrarily close to a maximally entangled state can be recovered. The probability of such a situation is proportionally unlikely. In the case of a third of the mixture having entanglement corresponding to a 1/3:2/3, weighting of the entangled pure state components, the probability of a maximally entangled pure state being recovered is of the order of $`10^6`$. Regardless of this, this state would provide an incredibly useful state to construct with a view to experimentally considering questions regarding mixed state quantum information, in that it covers so much of the entanglement-entropy plane.

The characteristics of the Werner state suggested that it might provide a bound on mixed state entanglement. In this figure, in the case where the first subsystem constraint is satisfied, there exist states with characteristics above the Werner bound. Clearly the Werner state does not provide an absolute bound for mixed state entanglement and a higher bound needs to be found.

## V Bounds on Entanglement

More recently, an attempt to put a bound on mixed state entanglement has resulted in a proposal by Munro et al. . The proposed bound involves a density matrix, not entirely dissimilar to the previous mixture of an entangled and a separable state. By considering a slight variation on this state, which involves placing some restrictions on the density matrix elements, a state of the form

$`\widehat{\rho }(\gamma )`$ $`=`$ $`\left(\begin{array}{cccc}12g(\gamma )& 0& 0& 0\\ 0& g(\gamma )& \gamma /2& 0\\ 0& \gamma /2& g(\gamma )& 0\\ 0& 0& 0& 0\end{array}\right)`$ (70)
is obtained, where $`g(\gamma )=\gamma /2`$ for $`\gamma 2/3`$ and $`g(\gamma )=1/3`$ for $`\gamma <2/3`$.

This state has a maximum amount of entanglement for the degree of purity, in terms of the Linear Entropy where the Linear Entropy , $`S_L=1P`$, is related to the purity of the state, $`P=\mathrm{Tr}[\rho ^2]`$. This is then normalised so that

$`S_L`$ $`=`$ $`{\displaystyle \frac{4}{3}}\left(1\mathrm{Tr}[\rho ^2]\right)`$ (71)
returns a value ranging from 0 for pure states, to 1 for a totally mixed state. This state has very similar behaviour to the previous state for $`\gamma 2/3`$ but significantly different below this point. For this state there are two non-zero eigenvalues for $`\gamma >2/3`$ and three below this point. Note here that $`\gamma `$ is not the mixture coefficient as previously defined.

If the subsystem constraints are again considered, the following restriction apply

$`\eta _{VA}^2\eta _{HB}^2`$ $`=`$ $`\eta _{HA}^2\eta _{VB}^2`$ (72)
and as before

$`\eta _{VA}^2\eta _{VB}^20`$ (73)
It is the case where $`\gamma <2/3`$ that the state has the most significant change in its entanglement-entropy characteristics. Below $`\gamma =2/3`$ the behaviour of this bounding state differs markedly from that of the previous state. The emergence of the extra eigenvalue increases the entropy and hence extends the coverage of the bound on the entanglement-entropy plane. As such this would suggest that there is some higher bound with respect to the Entanglement of Formation and entropy above what this state proposes. This might also suggest that if the bound is going to be complete, then at some point the emergence of a bounding state with four eigenvalues may be necessary as the entanglement tends to zero. At this point the Werner state may indeed provide the small entanglement - large mixing bound.

In Figure (9) the Werner state bound and the Linear Entropy bound are shown, and as just suggested, as the entanglement approaches zero, the Werner state bound is greater, going to zero at $`\gamma =1/3`$, $`S0.9`$, as the state becomes separable. The previous state is shown again here, where a mixture containing a maximally entangled pure state is used. This state and the Werner State both coincide with the Linear Entropy bound at $`\gamma =2/3`$. The previous state covers quite a large region of this space with the characteristics first increasing in entanglement at the cost of entropy before both the entanglement and the entropy improve, and concentration is realised.

The other curve on this figure to notice is the solid line starting at $`\gamma =1/2`$. This curve denotes the characteristics of the Linear Entropy bounding state when the Beam Splitter Protocol is applied to it. Notice that the boundary curve is exceeded, both above and below the bifurcation point for the state at $`\gamma =2/3`$. This should not be unexpected, as the subsystem entropies are not maximised for this state. The state was optimised in terms of the Linear Entropy of the joint state. Optimisation in terms of the von Neumann entropy is currently underway.

## VI Discussion

There have been several key points looked at in this paper and all of these have revolved around the Beam Splitter Protocol for manipulating mixed states. In doing this the equivalence between the coincidence detection state and that obtained by a “detect and discard” protocol, with perfect detectors at the reflected ports of the beam splitters, has also been justified. The process was then re-introduced, equivalently, in the context of local filtering operations. Although only a limited range of states were considered, the way the Beam Splitter Protocol transforms a state has shown that, due to the large number of degrees of freedom of the protocol, the scheme is highly adaptable. The transformations have been shown to extract the most amount of entanglement from a state that is possible for a given degree of mixing and in this sense could be considered optimal. The question of a bound on the amount of entanglement that a mixed state can have has been explored, firstly the Werner state and then the Linear Entropy bound.

For mixed states, questions of efficiency and optimality are not clear and as such discussion regarding these have been limited. The distinction is made regarding these concepts - it is one thing for the transformation to obtain the final state with the most amount of entanglement that is possible, and it is another to show the optimal probability or efficiency of carrying out a particular state transformation. The proposed bound on entanglement enhancement of Kent et al.  applies to the first interpretation and the protocol is shown to satisfy these requirements. In the case of the second interpretation, there has recently been a proposal by Vidal  which is an extension of his ideas on single-copy pure states and requires a minimisation over a set of entanglement monotones which has been left for future work.

The primary piece of information to note here is that: IF there is some initial amount of entanglement, AND the subsystems are not BOTH totally mixed, THEN more entanglement can be obtained by transforming the mixed state. The Beam Splitter Protocol introduced here can achieve this, it can do it in a very simple way, and one that is experimentally realisable.

The recovery and maintenance of an entanglement resource is a process that will be of paramount importance for any form of reliable quantum communication. Just as important is the investigation of mixed state entanglement in its own right. An understanding of the relationship between the classical and quantum probability distributions specifying an entangled mixed state is still not complete and any opportunity to investigate this in an experimental regime should be promoted.

The authors would like to thank A.G. White, P.G. Kwiat, K. Nemoto, M. Nielsen and G.J. Milburn for helpful discussions and support. We also thank S. Massar for bringing to our attention ref.