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# Decoherence Rate of Semiconductor Charge Qubit Coupled to Acoustic Phonon Reservoir

## Abstract

We analyze decoherence of an electron in a double-dot due to the interaction with acoustic phonons. For large tunneling rates between the quantum dots, the main contribution to decoherence comes from the phonon emission relaxation processes, while for small tunneling rates, the virtual-phonon, dephasing processes dominate. Our results show that in common semiconductors, such as Si and GaAs, the latter mechanism determines the upper limit for the double-dot charge qubit performance measure.

Recently, there has been a lot of interest in implementation of quantum logic gates by manipulating two-level electron systems in semiconductor quantum dots (artificial atoms) Barenco . Several designs for solid state quantum information processing have been suggested solid ; Fedichkin ; Dzurak . Quantum-dot architecture of a quantum computer is very attractive because it is possibly scalable and the most compatible with the recent microelectronics technology. However, it is a great challenge to maintain a satisfactory level of coherence of an electron in semiconductor to perform even elementary quantum gates Ekert . Hopefully, coherence can be enhanced by encoding of the logical qubit states into a subspace of the electron states in a large quantum dot array (artificial crystal) Zanardi . It is also noted that in a gate-engineered structure of two coupled identical quantum dots one can control decoherence rates by several orders of magnitude Fedichkin . Recent advances in technology of fabrication of double-dot Fujisawa ; Cain  and double-donor Dzurak  qubits have been reported. Coherent oscillations in double-dot qubit are observed Hayashi . It have been demonstrated that scattering by phonons can significantly influence electron transport through double-dot system Brandes  and qubit dynamics during measurement Gurvitz . In this work, we analyze decoherence of an electron in a double-dot potential due to acoustic phonons during one qubit gate cycle.

We consider a single electron in the double well potential shown schematically in Fig. 1. Such a structure can be fabricated as two gate-engineered quantum dots Fujisawa ; Cain ; Hayashi , whose geometry is determined by the pattern of external metallic gates and electric potential at them, or by the coupling the two nearby phosphorus donors embedded in silicon Dzurak . The resulting qubit is supposed to evolve in the basis spanned by the states $`|0`$ and $`|1`$ which describe the electron localized around the left and right minima of the potential, respectively. We assume that the parameters of the double-dot qubit structure are selected appropriately and the temperature is low enough such that the effects of the electron transitions to the higher energy levels can be neglected. Investigation of decoherence due to acoustic phonons is the primary goal of our work. Below, we will present the model and describe the two main mechanisms of decoherence. We will introduce the appropriate approximations schemes, quantify the overall error rate and discuss the ways to minimize it.

The Hamiltonian of the electron and the phonon bath is

$$H=H_e+H_p+H_{ep}.$$
(1)
Here qubit term in Hamiltonian is

$$H_e=\frac{1}{2}\epsilon _A(t)\sigma _x\frac{1}{2}\epsilon _P(t)\sigma _z,$$
(2)
where $`\sigma _x,\sigma _z`$ are the Pauli matrices. The parameters $`\epsilon _A,\epsilon _P`$ are controlled by the external metallic gates and can be used to perform on demand single-qubit rotations. These parameters determine the splitting, $`\epsilon `$, between the ground state and the first excited state of the electron in the energy basis. This splitting is given by $`\epsilon =\sqrt{\epsilon _A^2+\epsilon _P^2}`$. The phonon term in the Hamiltonian is

$$H_p=\underset{𝐪,\lambda }{}\mathrm{}sqb_{𝐪,\lambda }^{}b_{𝐪,\lambda },$$
(3)
where $`b_{𝐪,\lambda }^{}`$ and $`b_{𝐪,\lambda }`$ are the creation and annihilation operators of the phonons with the wave vector $`𝐪`$ and polarization $`\lambda .`$ For simplicity we consider isotropic acoustic phonons with the linear dispersion law. The electron-phonon interaction term is Mahan

$$H_{ep}=\underset{𝐪,\lambda }{}\sigma _z\left(g_{𝐪,\lambda }b_{𝐪,\lambda }^{}+g_{𝐪,\lambda }^{}b_{𝐪,\lambda }\right),$$
(4)
where $`g_{𝐪,\lambda }`$ is the coupling constant, which depends on the specific configuration of the system and the type of the interaction. Both the distance $`L`$ between quantum dots centers and their finite size $`a`$ will cut off the effect of the electron-phonon interaction at the tails of the phonon spectrum.

One can show that for the interaction of an electron bound in a gate-engineered Gaussian-shaped double-dot with deformation phonons, the coupling constant is

$$g_𝐪=iq\mathrm{\Xi }\left(\frac{\mathrm{}}{2\rho qsV}\right)^{1/2}e^{i𝐪𝐑a^2q^2/4}\mathrm{sin}(𝐪𝐋/2),$$
(5)
where $`\mathrm{\Xi }`$ is the deformation potential, $`s`$ is the speed of sound, $`\rho `$ is the density of the crystal, $`V`$ is normalizing volume, and $`𝐑`$ is the coordinate of the middle point of the double-dot. For crystal structures with inversion symmetry, like Si, there is no additional interaction due to the piezopotential. For crystals of the symmetry class $`T_d`$, like GaAs, the piezoelectric phonon coupling is

$`g_{𝐪,\lambda }=`$ $`\left({\displaystyle \frac{\mathrm{}}{2\rho qsV}}\right)^{1/2}Me^{i𝐪𝐑a^2q^2/4}`$ (6)
$`\times (\xi _1e_2e_3+\xi _2e_1e_3+\xi _3e_1e_2)\mathrm{sin}(𝐪𝐋/2),`$
where $`e_i=q_i/q`$, $`\xi `$ is the polarization vector and $`M`$ is the piezoconstant of the substrate.

For a double-donor system composed of two coupled hydrogen-like dopant impurity states, e.g., for two phosphorus atoms embedded in silicon, the following expression for the coupling constant with the deformation phonons was obtained

$$g_𝐪=iq\mathrm{\Xi }\left(\frac{\mathrm{}}{2\rho qsV}\right)^{1/2}\frac{e^{i𝐪𝐑}}{\left(1+a^2q^2/4\right)^2}\mathrm{sin}(𝐪𝐋/2).$$
(7)
The interaction term (4) leads to decoherence of the qubit. The resulting loss of coherence is some functional of $`\epsilon _A(t)`$ and $`\epsilon _P(t)`$. Here we consider two representative cases of the single-qubit gate functions and derive estimates for the error rate due to phonons. First, we consider the relaxation of an electron during the NOT gate ($`\sigma _x`$), implemented by setting $`\epsilon _A(t)=\epsilon const`$ and $`\epsilon _P(t)=0`$ in the Hamiltonian (2), for the time interval (cycle time of the quantum computer) $`\mathrm{\Delta }t=\pi \mathrm{}/\epsilon `$. Second, we consider the decoherence of an electron during the $`\pi `$-phase-rotation gate ($`\sigma _z`$), implemented by setting $`\epsilon _A(t)=0`$ and $`\epsilon _P(t)=\epsilon const`$ for the same time interval $`\mathrm{\Delta }t=\pi \mathrm{}/\epsilon `$.

To evaluate the relaxation of a double-dot qubit due to acoustic phonons, we will follow Fedichkin ; Brandes ; Barrett . We assume that the temperature is low compared to energy gaps of the system. Therefore we consider the qubit at zero temperature. The major parameter of dots influencing the interaction with phonons is their size $`a`$. For gate-engineered quantum dots the actual shape of wave function of confined electron can vary. We consider Gaussian-shaped dots in which electron wave function is Gaussian $`\left(\mathrm{\Psi }(𝐫)\mathrm{exp}\left(r^2/\left(2a^2\right)\right)\right)`$. With these assumptions, the following result for the relaxation rate due to the interaction with deformation phonons can be obtained,

$$\mathrm{\Gamma }_{DA}=\frac{\mathrm{\Xi }^2k^3}{4\pi \rho s^2\mathrm{}}\mathrm{exp}\left(a^2k^2/2\right)\left(1\frac{\mathrm{sin}\left(kL\right)}{kL}\right),$$
(8)
where $`k=\epsilon /(s\mathrm{})`$ is the wave-vector of the emitted phonon. For the piezoelectric type of interaction, we get

$$\mathrm{\Gamma }_{PA}=\frac{M^2}{20\pi \rho s^2\mathrm{}L^5k^4}\mathrm{exp}\left(a^2k^2/2\right)\left(\left(kL\right)^5+5kL\left(2\left(kL\right)^221\right)\mathrm{cos}\left(kL\right)+15\left(73\left(kL\right)^2\right)\mathrm{sin}\left(kL\right)\right).$$
(9)
In double phosphorus dopant structures in silicon, the relaxation rate due to the deformation phonons for the hydrogen-like impurity states is

$$\mathrm{\Gamma }_{IDA}=\frac{\mathrm{\Xi }^2}{4\pi \rho s^2\mathrm{}}\frac{k^3}{\left(1+a^2k^2/4\right)^4}\left(1\frac{\mathrm{sin}(kL)}{kL}\right).$$
(10)
If the wavelength of the phonon to be emitted is high enough compared to the size of dots, $`a`$, and the distance between the dots, $`L`$, i.e.,

$$ak1;Lk1,$$
(11)
which is often the case in present-day heterostructures, then the following approximate expressions are valid

$$\mathrm{\Gamma }_{DA}=\mathrm{\Gamma }_{IDA}=\frac{\mathrm{\Xi }^2L^2\epsilon ^5}{24\pi \rho s^7\mathrm{}^6}$$
(12)
and

$$\mathrm{\Gamma }_{PA}=\frac{M^2L^2\epsilon ^3}{120\pi \rho s^5\mathrm{}^4}.$$
(13)
Right after the implementation of the NOT gate the density matrix in the energy basis $`\{|+,|\}`$, where $`|\pm =\left(|0\pm |1\right)/\sqrt{2}`$, will be Blum

$$\left(\begin{array}{cc}1\rho _{}(0)e^{\mathrm{\Gamma }\mathrm{\Delta }t}& \rho _+(0)e^{(\mathrm{\Gamma }/2i\epsilon /\mathrm{})\mathrm{\Delta }t}\\ \rho _+(0)e^{(\mathrm{\Gamma }/2+i\epsilon /\mathrm{})\mathrm{\Delta }t}& \rho _{}(0)e^{\mathrm{\Gamma }\mathrm{\Delta }t}\end{array}\right),$$
(14)
where $`\rho _{\pm \pm }(0)`$ are the elements of the electron density matrix before the implementation of the NOT gate and the parameter $`\mathrm{\Gamma }`$ should be taken from Eqs. (810), respectively.

We now consider the implementation of the phase gate. In this case, decoherence emerges as pure dephasing. There is no relaxation because the interaction term (4) commutes with the electron term in the Hamiltonian (2). The basis $`\{|0,|1\}`$ coincides with the energy basis of the electron. For evaluation of the dephasing rate we used the general analytical expression for the density operator of the electron in the boson bath given in vanKampen ; Privman1 ,

$$\rho =\left(\begin{array}{cc}\rho _{00}(0)& \rho _{01}(0)e^{B^2(\mathrm{\Delta }t)+i\epsilon \mathrm{\Delta }t/\mathrm{}}\\ \rho _{10}(0)e^{B^2(\mathrm{\Delta }t)i\epsilon \mathrm{\Delta }t/\mathrm{}}& \rho _{11}(0)\end{array}\right).$$
(15)
Thus, the evolution of the system is determined by the spectral function $`B(t)`$ Palma ; vanKampen , which in our case is expressed as

$$B^2(t)=\frac{8}{\mathrm{}^2}\underset{𝐪,\lambda }{}\frac{\left|g_{𝐪,\lambda }\right|^2}{s^2q^2}\mathrm{sin}^2\frac{sqt}{2}.$$
(16)
By performing the summation in Eq. (16), we get the spectral functions determining the density matrices after the $`\pi `$-phase rotation of both the qubits made of double-dots with deformation and piezoelectric electron-phonon interaction, and of double-impurity qubit states, respectively,

$$B_{DA}^2=\frac{\mathrm{\Xi }^2}{2\pi ^2\rho s^3a^2\mathrm{}},$$
(17)
$$B_{PA}^2=\frac{M^2L^2\left(1\mathrm{exp}\left({\displaystyle \frac{a^2\pi ^2}{2L^2}}\right)+{\displaystyle \frac{3a^2}{L^2}}E_1\left({\displaystyle \frac{a^2\pi ^2}{2L^2}}\right)\right)}{60\pi ^2\rho s^3a^2\mathrm{}},$$
(18)
$$B_{IDA}^2=\frac{\mathrm{\Xi }^2}{3\pi ^2\rho s^3a^2\mathrm{}}.$$
(19)
Here $`E_1(z)=\underset{z}{\overset{\mathrm{}}{}}t^1e^t𝑑t`$. Expressions (1719) were obtained by using an additional observation that the duration of the qubit phase rotation is large compared to the phonon transit time $`\mathrm{\Delta }ta/s`$. This condition holds for the GaAs and Si structures considered.

To analyze the double-dot qubit architecture with respect to the fault-tolerant quantum computing criteria DiVincenzo , one should be able to estimate the error generated during the ”clock” time of the quantum computer $`\mathrm{\Delta }t`$. To quantify the error due to decoherence, we use the approach of Ref. norm . We consider the norm of the deviation operator, $`\sigma `$

$$\sigma (t)=\rho (t)\rho _{\mathrm{ideal}}(t),$$
(20)
where the ”ideal” evolution is defined as that at zero interaction with the environment,

$$\rho _{\mathrm{ideal}}(t)=e^{iH_et/\mathrm{}}\rho (0)e^{iH_et/\mathrm{}}.$$
(21)
The error is characterized norm  by the value

$$D(t)=\underset{\rho (0)}{sup}\left(\sigma (t,\rho (0))_\lambda \right),$$
(22)
which is the maximal norm of the deviation operator over all the possible initial density operators of the electron $`\rho (0)`$. For fault-tolerant computation we need to satisfy the condition $`D(\mathrm{\Delta }t)O\left(10^4\right)`$ DiVincenzo . For the density operators after the NOT and phase gates given by Eqs. (14, 15), the corresponding errors $`D_A,D_P`$ can be expressed in a compact and elegant form as

$$D_A(\mathrm{\Delta }t)=1e^{\mathrm{\Gamma }\mathrm{\Delta }t},$$
(23)
$$D_P(\mathrm{\Delta }t)=\frac{1}{2}\left(1e^{B^2(\mathrm{\Delta }t)}\right).$$
(24)
To evaluate the single-gate error rate we take the maximum of the two gate errors considered which are typical single-qubit gates in quantum algorithms. The error rate per each step can be estimated as the larger of the above errors

$$D(\mathrm{\Delta }t)=\mathrm{max}(D_A(\mathrm{\Delta }t),D_P(\mathrm{\Delta }t)).$$
(25)
The obtained error rates for GaAs and Si quantum dots are shown in Fig. 2. It should be noted that dephasing appears to be the limiting factor of qubit fault tolerance. For a qubit made of impurity states, the corresponding spectral function (19) determining its dephasing rate is, in fact, material constant and cannot be changed significantly. Since the estimated minimal error rate for the Si double-impurity qubit is more than 1/400, the construction of a practically useful fault-tolerant quantum computer by using this design is questionable. Still, phonon decoherence can be reduced by the change of phonon spectrum with the help of phonon cavities Fujisawa ; Debald . Gate-engineered quantum dots show better coherence. Moreover, their performance can be improved because their geometric parameters are flexible.

In conclusion, we evaluated error rate in semiconductor charge qubits due to interaction with acoustic phonons. Our results shows that the expected error rate for double-phosphorus impurity states in silicon is above the fault-tolerance threshold for quantum computation. On the other hand, larger gate-engineered double quantum dots both in Si and GaAs, with parameters close to those in modern experiments Hayashi ; Cain ; Dzurak , can be controlled more coherently. Realization of those qubits would be a significant step toward the implementation of a full-scale solid state quantum computer.

###### Acknowledgements.

We gratefully acknowledge helpful discussions with Prof. V. Privman, D. Mozyrsky and L.C.L. Hollenberg. This research was supported by the National Science Foundation, Grants DMR-0121146 and ECS-0102500, and by the National Security Agency and Advanced Research and Development Activity under Army Research Office Contract DAAD 19-02-1-0035.


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# Point-Contact Spectroscopy in MgB2: from Fundamental Physics to Thin-Film Characterization

## 1 Introduction

From the point of view of fundamental physics, magnesium diboride (MgB2, discovered to be superconducting below 39 K in 2001 ) is particularly interesting because it is the clearest example of two-band superconductor ever studied . However, this simple compound is also interesting because of its possible applications, that could take advantage of its rather low production cost and of its rather high $`T_\mathrm{c}`$. At present, one of the most promising fields of application is superconducting electronics, with the perspective of MgB2-based devices with good performances operating at a temperature ($``$ 10-15 K) accessible to one-stage cryocoolers. After the early observation of the Josephson effect in MgB2 break junctions , the efforts in this directions have led to the fabrication of various kinds of Josephson and tunnel junctions  as well as prototypal SQUIDs .

Point-contact spectroscopy (PCS) has proved particularly useful in the fundamental research on MgB2, since it allows measuring in a direct way both the gaps of this compound  with great accuracy . Actually, being a surface-sensitive probe, PCS is also a unique experimental technique to study the surface superconducting properties of the material. Thus, we also used it as a diagnostic tool within a process of optimization of MgB2 thin films, in view of the fabrication of Josephson junctions of different kinds and, finally, of simple superconducting electronic devices (e.g. SQUIDs).

In this paper we will first present some results of relevant fundamental interest we obtained by directional PCS in MgB2 single crystals in the presence of magnetic fields up to 9 T, among which the temperature dependence of the critical field for $`𝐁c`$ and $`𝐁ab`$, and the temperature and magnetic-field dependence of the gap amplitudes. We will show how these results address some important subjects of present debate in the fundamental physics of MgB2. Then, we will report the results of PCS measurements in MgB2 thin films grown by different techniques on various substrates. These measurements provide information (e.g. about film orientation) that can be compared to structural and morphological results, such as XRD and AFM/STM. We will also show that PCS can give very useful indications about the conditions of the very surface (e.g., presence and effectiveness of impurities, oxidation, degradation) that are of crucial importance for the fabrication of tunnel and Josephson junctions for electronic applications, but *cannot* be provided by bulk-sensitive techniques.

## 2 Experimental details

### 2.1 The samples

The state-of-the-art MgB2 single crystals used in our experiments were produced by J. Karpinski’s group at the Solid State Physics Laboratory of ETH, Zurich (Switzerland). The crystal growth procedure occurs under a pressure of 30-35 kbar and is described in detail elsewhere (see for example Ref. ). For our purposes, we had to use crystals with regular shape (i.e. flat upper surface and sharp edges) even if they were rather small ($`0.6\times 0.6\times 0.06`$ mm3 at most).

The thin films were produced either at the National Electrotechnical Institute (IEN) “Galileo Ferraris” in Turin (Italy) or at the LAMIA Laboratory of the National Institute for the Physics of Matter (INFM), in Genoa (Italy). Films on $`c`$-cut sapphire and MgO (111) (both with hexagonal surface symmetry, similar to that of MgB2) were produced by using a two-step procedure by the Genoa group . The first step consists in the PLD deposition of an amorphous, non-superconducting precursor layer in UHV ($`10^9`$ mbar) at room temperature, starting from a stoichiometric MgB2 sintered target. The second step is an ex-situ annealing process in magnesium atmosphere, necessary to crystallize the superconducting phase. The samples are sealed in tantalum crucibles under Ar pressure with Mg lumps, closed in an evacuated quartz tube and kept at 850C for half an hour with a following rapid quenching to room temperature. In addition to sapphire, the group from Turin also used amorphous silicon nitride (SiN) as substrate, which is particularly advantageous in view of the fabrication of bolometers . The 500 nm-thick, amorphous SiN layer is grown on silicon wafer by LPCVD. The MgB2 films are then deposited by simultaneous evaporation of Mg and B at constant temperature in a pressure of 5$`10^7`$ mbar from a Mo resistive heater and from a Mo crucible by e-beam heating, respectively. The resulting precursor is annealed *in situ* (i.e. in the deposition chamber) in Ar atmosphere, at 500C. The resulting films look golden-brownish and mirror-like, are always very homogeneous and cover the whole surface of the substrates (about 5 cm2).

### 2.2 Directional PCS in single crystals

As described elsewhere , the point contacts (of about $`50\times 50\mu \mathrm{m}^2`$) were made by using a small piece of indium or a drop of Ag conductive paint. This ensured better mechanical stability on thermal cycling and reproducibility of the conductance curves with respect to the standard technique that employs a metallic tip pressed against the sample. The contacts were placed either on the top surface or on the side of the crystals, so as to inject the current mainly along the $`c`$ axis or along the $`ab`$ planes, respectively 777Actually, the current is injected within a cone whose angle $`\varphi `$ depends on the potential barrier at the interface: $`\varphi 0`$ for tunneling ($`Z\mathrm{}`$) and $`\varphi =\pi /2`$ for metallic contact with no barrier ($`Z=0`$). Our contacts are always in an intermediate case, but the probability for electrons to be injected along an angle $`\phi `$ in the cone is proportional to $`\mathrm{cos}\phi `$  so that it is maximum along the normal direction anyway..

Knowing the direction of current injection is important because of the anisotropy of MgB2. In fact, PCS gives the $`IV`$ characteristics and the conductance curves (d$`I`$/d$`V`$ vs. $`V`$) of a normal metal/superconductor junction. In the case of MgB2, the conductance across such a junction contains (separate) contributions of the $`\sigma `$ and $`\pi `$ bands . Since the $`\sigma `$ bands are almost 2D (and originate from the overlapping of in-plane $`sp^2`$ boron orbitals), their contribution to the conductance is maximum for current flowing along the $`ab`$ planes. This is thus the most favorable configuration to observe clearly the $`\sigma `$-band gap together with the $`\pi `$-band one. The use of MgB2 single crystals allowed us to perform these measurements and to test the predictions of the two-band model concerning the amplitudes of the gaps, their temperature- and magnetic field-dependency, and the relative weight of the two bands for $`ab`$-plane and $`c`$-axis current injection.

### 2.3 PCS in thin films

As in single crystals, point contacts on films were made either by using a spot of Ag paint or a piece of indium placed on the top surface 666Note that the conventional PCS technique using a metallic tip could be unadvisable in this case, due to the risk of cracks in the film itself.. In this case, the weight of the $`\sigma `$-band contribution to the total normalized conductance is an indicator of the film orientation. For perfectly $`c`$-axis oriented films an almost pure $`c`$-axis conductance is expected, with little or no traces of the $`\sigma `$-band gap (as an example, see the lower curve in Figure1a). However, even in highly oriented films the $`\sigma `$-band contribution could be greater than expected if the surface roughness is not small enough, since microcontacts could be established also on the edge of grains or mesas. Similarly, even in films with very flat surface (such as those grown by hybrid physical-chemical vapour deposition (HPCVD) ) conventional PCS can give an excess $`\sigma `$-band contribution due to the partial penetration of the tip in the films. Probably, this explains the recent results by Bugoslavskij and coworkers .

In addition to the information about film orientation, PCS also provides information about possible enhancements or reductions of the superconducting properties at the surface the clean- or dirty-limit conditions at the surface (i.e., roughly speaking, the effectiveness of interband scattering due to impurities) and the existence of a degraded insulating layer, for example of MgO (which can arise from the reaction with atmosphere).

## 3 Results and discussion

### 3.1 Directional PCS in single crystals

Figure 1 reports some results of PCS in single crystals. In panel (a) symbols represent typical conductance curves of $`ab`$-plane and $`c`$-axis contacts. In the first case (upper curve) four conductance peaks are present, at $`V\pm 2.8`$ mV and $`V\pm 7.6`$ mV. These features are connected to the two gaps, $`\mathrm{\Delta }_\pi `$ and $`\mathrm{\Delta }_\sigma `$. In $`c`$-axis contacts (lower curve) at the same voltages we observe clearly defined maxima and smooth shoulders, respectively. Such a difference is due to the aforementioned anisotropy of the $`\sigma `$ bands, whose contribution to the conductance is minimum for $`c`$-axis current. That this contribution is not zero is clearly shown by the fact that the standard $`s`$-wave, single-band Blonder-Tinkham-Klapwijk (BTK) model  is not able to fit the conductance curves. On the contrary, the same model generalised to the two-band case, where the total *normalized* conductance is $`\sigma =w_\pi \sigma _\pi +(1w_\pi )\sigma _\sigma `$, gives rather good results (solid lines). The best fit is obtained with values of the gaps and of the weight $`w_\pi `$  that agree very well with the predictions of the two-band model in the Eliashberg formulation . However, the accuracy of these values is rather poor since the fitting function contains 7 adjustable parameters: $`\mathrm{\Delta }_\sigma `$ and $`\mathrm{\Delta }_\pi `$, the broadening parameters $`\mathrm{\Gamma }_\sigma `$ and $`\mathrm{\Gamma }_\pi `$ (that account for pair-breaking effects), the barrier transparency coefficients $`Z_\sigma `$ and $`Z_\pi `$ (proportional to the potential barrier height), and $`w_\pi `$.

Figure 1b illustrates the procedure we used to improve this accuracy . Symbols represent the experimental normalized conductance curves of a $`c`$-axis In contact, measured in zero field (“B=0”) and in the presence of a field of 1 Tesla (“B=1T”), together with the difference between these two, vertically shifted by 1 for best comparison (“diff.+1”). As discussed elsewhere , the $`\pi `$-band contribution to the experimental conductance is strongly suppressed by the field and, at $`B1`$ T, it is no longer detectable by our fitting procedure, while the $`\sigma `$-band gap remains practically unchanged. Thus, the conductance curve measured in a field of 1 T practically contains the $`\sigma `$-band conductance alone. If the conductance in zero field is given by $`\sigma _{\mathrm{B}=0}=w_\pi \sigma _\pi +(1w_\pi )\sigma _\sigma `$, the curve measured in $`B=1`$ T is obtained by putting $`\sigma _\pi =1`$ and thus has the functional form $`\sigma _{\mathrm{B}=1\mathrm{T}}=w_\pi +(1w_\pi )\sigma _\sigma `$. Consequently, the difference between the two curves is expressed by $`\sigma _{\mathrm{diff}}=\sigma _{\mathrm{B}=0}\sigma _{\mathrm{B}=1\mathrm{T}}=w_\pi (\sigma _\pi 1)`$ and only contains the $`\pi `$-band contribution.

Fitting the experimental curves reported in the figure (symbols) with the corresponding functions $`\sigma _{\mathrm{B}=0}`$, $`\sigma _{\mathrm{B}=1\mathrm{T}}`$ and $`\sigma _{\mathrm{diff}}`$ gives indeed very good results. The fitting curves are reported in Figure1b as solid lines. The best-fitting parameters are: $`\mathrm{\Delta }_\sigma =7.1\pm 0.1`$ meV, $`\mathrm{\Gamma }_\sigma =1.7`$ meV, $`Z_\sigma =0.6`$ from the fit of the curve in magnetic field; $`\mathrm{\Delta }_\pi =2.80\pm 0.05`$ meV, $`\mathrm{\Gamma }_\pi =2.0`$ meV, $`Z_\pi =0.6`$ from the fit of the difference. The clear advantage of this procedure, that allows separating the partial $`\sigma `$\- and $`\pi `$-band conductances, is that the number of free parameters in each fitting function is reduced to three ($`w_\pi `$ is fixed to the value one gets from the fit of $`\sigma _{\mathrm{B}=0}`$, i.e., in the case of Figure 1b, $`w_\pi =0.98`$) with a consequent reduction of the uncertainty on the gap amplitudes.

If this procedure is repeated at any temperature, one obtains the complete temperature dependence of the gaps reported in Figure 1c (symbols). Two BCS-like curves (dots) and the $`\mathrm{\Delta }_{\sigma ,\pi }(T)`$ curves predicted by the two-band model  (solid lines) are reported for comparison. It is clear that our data are so precise that they reproduce the theoretically-predicted downward deviation of $`\mathrm{\Delta }_\pi `$ from the BCS-like behaviour. However, the actual shape of the curve does not correspond to the theoretical one, maybe indicating that, in our samples, the values of some parameters are slightly different from those used in the model.

It is clear that the whole procedure described so far (that gave one of the clearest direct evidences of the existence of two distinct gaps in MgB2 up to $`T_\mathrm{c}`$ ) is based on the disappearance of the $`\pi `$-band contribution to the conductance in a field of about 1 Tesla. To obtain the whole magnetic-field dependence of the gaps, we measured the conductance curves of Ag-paint, $`ab`$-plane contacts at $`T=4.2`$ K, in the presence of a magnetic field of increasing intensity applied parallel to the $`c`$ axis. An example of the results is shown in Figure 2a (symbols). The solid lines in the same graph are the best-fitting curves of the form $`\sigma (B)=w_\pi \sigma _\pi (B)+(1w_\pi )\sigma _\sigma (B)`$, where $`w_\pi `$ is assumed to be field-independent. Above 1 Tesla the best fit is obtained by keeping $`\sigma _\pi (B)=1`$ (for details on the fitting procedure see Ref. ). The values of the gaps are shown in Figure 2b as solid symbols. For comparison, superimposed to the experimental $`\mathrm{\Delta }_{\sigma ,\pi }(B)`$ curves we report also the theoretically-predicted values of the maximum order parameter (calculated at the boundary of the vortex-lattice unit cell ) in the case where the $`\pi `$-band diffusivity $`D_\pi `$ is 5 times greater than $`D_\sigma `$. The comparison is only qualitative, since PCS rather measures an average of the pair potential in different regions of the vortex lattice, but the agreement is surprising. This indicates that, even in best-quality single crystals, the $`\pi `$ band is in the moderate dirty limit 777In this context, the expression “clean” and “dirty” refer to *intraband* scattering. According to Anderson’s theorem, this scattering cannot reduce the critical temperature of the compound nor the amplitude of the gaps., in agreement with the results of STM  and de Haas-van Alphen measurements .

In the case of Figure 2 the junction featured very good curves, but broke down before the normal state was reached. In many other cases we were able to follow the evolution of the conductance curves up to the critical field , here defined as the field that marks the return to the normal-state conductance. Because of the anisotropy of MgB2, the values of the critical field depends very much on whether $`𝐁ab`$ or $`𝐁c`$. The resulting values of the critical field $`B_{\mathrm{c2}}`$ are reported in Figure 3a as a function of the reduced temperature $`T/T_\mathrm{c}`$.

In the same figure, the shaded regions are lower-bounded by the values of the critical field given by bulk measurements (i.e. thermal conductivity , specific heat  and torque magnetometry ) and upper-bounded by the field that, at any temperature, marks the onset of the superconducting transition in the $`\rho (B)`$ curve . This field has been recently identified  with the surface critical field $`B_{\mathrm{c3}}`$ . It is clearly seen that, in both the $`𝐁c`$ and $`𝐁ab`$ configurations, our values practically coincide with the bulk critical field at high temperatures, then approach the surface critical field at lower temperature and finally turn again toward the bulk values. The “crossover” from $`B_{\mathrm{c2}}`$ to nearly $`B_{\mathrm{c3}}`$ always occurs at $`T/T_\mathrm{c}0.7`$ and thus seems to be temperature-induced rather than field-induced. The more pronounced curvature of our data with respect to other results gives rise to a temperature dependence of the anisotropy ratio $`\gamma =B_{\mathrm{c2}}^{ab}/B_{\mathrm{c2}}^c`$ (solid circles in Figure 3b) which, at $`T<0.7T_\mathrm{c}`$, differs very much from that given by bulk techniques (open symbols). However, it is interesting to note that a similar $`\gamma (T)`$ behaviour was theoretically predicted and reported in Ref.  in the case where $`D_\pi =10D_\sigma `$. Again, this indicates that – at least at the surface – our MgB2 single crystals present a $`\pi `$ band in the moderate dirty limit, in complete agreement with the results of Figure 2. Notice that this conclusion has a great fundamental importance since the role and the amount of intraband scattering in MgB2 is still a matter of debate, and alternative models (for negligible  and non-negligible  intraband scattering) have been proposed to explain experimental findings in this compound.

### 3.2 PCS in thin films

Figure 4 reports the conductance curves of two In/MgB2 point contacts made on the surface of a thin film (“FILM 0”) grown on silicon nitride by co-deposition of Mg and B and subsequent *in situ* annealing. The resistive critical temperature of the film is $`T_\mathrm{c}=36`$ K , and the transition is very sharp ($`\mathrm{\Delta }T_\mathrm{c}1`$ K). The normal-state resistance of the contacts is also indicated. The conductance curves feature clear maxima, related to the small gap, at $`\pm 2.6`$ mV (upper curve) and $`\pm 3.4`$ mV (lower curve). A shoulder at about $`\pm 7.2`$ mV is clearly seen in the upper curve, but is also present (even if smoother) in the lower one. Comparing the curves to those obtained in single crystals (see Figure 1) it is clear that their shape is compatible with a *preferential* $`c`$-axis orientation of the films. However, the rather evident contribution of the $`\sigma `$ band (especially in the upper curve) indicates that this orientation is not complete.

The AFM images of the film surface reported in Figure 5a clarify this point. The main image and its enlargement (inset) clearly show vertically- and horizontally-packed plate-like grains, that in PCS measurements behave as a set of crystals in which the current is injected along to the $`c`$ axis or along the $`ab`$ planes. This explains not only the shape of the curves, with the excess of $`ab`$-plane contribution, but also its variability from point to point. An analysis of the images reported in Figure 5a gives the average grain size ($`200÷250`$ nm) and the RMS roughness, that in this case is about 30 nm (even if values down to 10 nm were obtained). The small roughness is particularly important in view of the fabrication of planar Josephson junctions, where the control of the interface smoothness is crucial. The XRD spectrum reported in Figure 5b shows clear (001) and (002) diffraction maxima, coming from the $`c`$-axis oriented main phase, whose intensity is however smaller than in single crystals. The absence of a clear (101) reflection, that is the most intense in powders, indicates that most of the film is oriented, in spite of the amorphous SiN substrate. A very intense spurious peak due to the crystalline Si substrate (on which SiN is deposited) is also shown.

In addition to the information on the orientation, two other important indications can be extracted from the Andreev-reflection spectra reported in Figure 4. First, the possibility to observe Andreev reflection by PCS means that the contact is S-N, i.e. the potential barrier $`Z`$ at the interface is very small . In other words, there cannot be any insulating layer (for example, of MgO due to the reaction with air) covering the surface 111Notice that this conclusion can be drawn here because the contact is “soft”. On the contrary, in the conventional technique the tip can damage and even perforate the surface layer and this information is lost.. This finding is consistent with the remarkable durability of these films that, if kept in suitably dry atmosphere, retain their properties for several months. The second important indication concerns the “clean” or ‘dirty” limit conditions at the surface of the film. In this context, the expressions “clean” and “dirty” are referred to the *interband* scattering. According to the two-band model appeared in literature , if the interband scattering is sufficiently strong, the critical temperature falls drastically and the two gaps merge in one single isotropic gap $`\mathrm{\Delta }_{\mathrm{dirty}}`$, with BCS-like temperature dependence and zero-temperature value $`\mathrm{\Delta }_{\mathrm{dirty}}4.2`$ meV. It is clear that the evidence of two distinct gaps in the curves of Figure 4 indicates that the surface of the films is in clean limit, even if this kind of measurements cannot provide a measure of the scattering rate.

Figure 6a reports the conductance curves of a Ag-paint spot contact on a 100 nm-thick MgB2 film grown on $`c`$-cut sapphire by PLD and then annealed *ex situ* in Mg vapour (“FILM 1” in Refs.). The critical temperature of the film, measured by transport, is $`T_\mathrm{c}=29.5`$ K, with $`\mathrm{\Delta }T_\mathrm{c}=2`$ K. The strong $`c`$-axis orientation of the film is witnessed both by the XRD spectrum reported in Figure 6b (note that the (101) peak, that is the most intense in powders, is absent) and by the large values of the low-temperature anisotropy ($`\gamma =3.0`$), one of the highest reported in literature for films. The film also features in-plane orientation, with a 30-tilt with respect to the substrate, as shown by $`\mathrm{\Phi }`$-scan measurements ; other characteristics are reported in Ref.. The conductance curve of Figure 6a shows maxima at $`\pm 4.5`$ mV and no clear shoulders. The absence of multigap features and the position of the maxima suggests that the measured gap is very likely to be $`\mathrm{\Delta }_{\mathrm{dirty}}`$. Since in the dirty limit the material becomes isotropic, it is clear that, in this case, PCS is unable to give any information about the orientation of the film. However, it provides a direct evidence of the degradation of the material, e.g. due to the exposition to air and moisture. This degradation is definitely restricted to the very top layer of the film (in fact, transport measurements gave reproducible values of the critical field  even if repeated after several months) and is thus difficult or even impossible to detect with bulk-sensitive techniques. In this sense, PCS has the unique capability to probe the conditions of the surface, that is particularly useful in view of the fabrication of planar Josephson junctions, where the control of the interface is crucial.

Figure 7a reports the conductance curve of a Ag-paint contact on a MgB2 film grown on MgO (111) substrate (“FILM 2” in Ref.). The critical temperature of the film is a little higher than that of FILM 1, i.e. $`T_\mathrm{c}=32`$ K with $`\mathrm{\Delta }T_\mathrm{c}=1.5`$ K. As shown by the XRD spectrum reported in Figure 7b, the film is strongly $`c`$-oriented, even if it does not feature in-plane orientation. The shape of the conductance curve clearly denotes that the contact is in the “tunnelling” regime (large $`Z`$) rather than in the Andreev-reflection regime (small $`Z`$). As in the case of Figure 6a, the curve in Fig. 7a presents conductance maxima at energies ($`\pm 4.2`$ meV) that correspond to the gap in dirty limit, $`\mathrm{\Delta }_{\mathrm{dirty}}`$. In this case, however, additional features are present in the form of shoulders at $`\pm 2.7`$ meV, that should correspond to the small gap $`\mathrm{\Delta }_\pi `$. This result can be explained by admitting that parallel microcontacts are established between the Ag glue and the film, in regions of the film where the surface is clean (and thus $`\mathrm{\Delta }_\pi `$ is observed) and dirty (where $`\mathrm{\Delta }_{\mathrm{dirty}}`$ is measured). In principle, the absence of any clear evidence of $`\mathrm{\Delta }_\sigma `$ in the conductance curves could be interpreted as a further indication of good $`c`$-axis orientation of the clean material; however, in the present case the measure is probably too noisy and broadened for this conclusion to be definitely drawn.

As in the previous case, the observation of $`\mathrm{\Delta }_{\mathrm{dirty}}`$ in some regions of the contact speaks in favour of aging effects, that cannot be excluded due to the rather long time elapsed between the film deposition and the PCS measurements (several months). Further support to this hypothesis comes from the fact that we could never observe Andreev reflection in contacts made on this films. In other words, we always obtained S-I-N contacts, with a non-negligible potential barrier at the interface, and with tunnelling-like characteristics. This is probably due to the presence of an oxide layer on the top of the film – i.e. MgO due to the exposition to air and moisture – acting as an insulating barrier and preventing the direct contact between the superconductor and the normal metal. As a matter of fact, some peaks due to MgO are often found in the XRD spectra, as in Figure 6 (in the case of FILM 2, however, they are not conclusive since the substrate is made of MgO too). It is worth noting that, again, no evidence of this surface degradation was found in critical field measurements, that always gave a very high value of the anisotropy ($`\gamma =3.5`$) supporting the spectroscopic evidence of $`c`$-axis orientation.

## 4 Conclusions

In conclusion, we have shown that “soft” PCS, that employs small In spots or Ag-paste drops to make the “point” contacts, presents unique advantages for the investigation of the fundamental superconducting properties of MgB2 as well as for the characterization of the morphological and electronic properties of crystal and film surfaces. It is clear that these advantages hold for any superconductor, provided that its surface is sufficiently clean, stable in air, metallic and homogeneous to obtain clear Andreev-reflection curves. Morever, some of these requirements are not really strict. For example, even in the presence of an insulating surface layer (either intentionally grown or consequent to degradation) this technique permits the creation of useful weak-link SIN junctions (as shown in Figure 7).

In particular, with respect to standard PCS – where a metallic tip is pressed against the sample surface – our “soft” PCS technique ensures: i) greater stability and reproducibility of the junctions at the change of temperature and magnetic field; ii) absence of damage or perforation of the surface, that prevents unwanted contributions from the underlying bulk material; iii) greater control of the directionality of the contact, that can be essential in the study of anisotropic superconductors like MgB2. On the other hand, the smaller area of the contact usually obtained by metallic tips can be useful in the study of superconductors with non-homogeneous or granular surfaces. In this respect, a further improvement of the technique with a reduction of the minimum apparent contact area is under study.

This work was done within the project PRA ”UMBRA” of INFM, the ASI contract N. I/R/109/02 and the INTAS project N. 01-0617. V.A.S. acknowledges the support from RFBR (project N. 02-02-17133) and the Ministry of Science and Technologies of the Russian Federation (contract N. 40.012.1.1.1357).

## References


text:
# Neutron Moderation in the Oklo Natural Reactor and the Time Variation of 𝛼 LA-UR 03-6686

## I Introduction

It was recognized by Shlyakhter 1  that isotopic ratios of fission products and secondary neutron absorption reactions that occurred with the Oklo natural reactor phenomenon some 2 billion years ago could be used to test whether the fine-structure constant $`\alpha `$ varies with time. Specifically, if a neutron absorber (e.g., 149Sm) has a low-energy neutron absorption resonance, and the excited compound state can decay by gamma emission, the resonance energy will change in a predictable way if $`\alpha `$ varies. The overlap of the resonance with the reactor neutron spectrum will subsequently change thereby altering the ratios of nearby isotopes.

In addition to 1 , two other detailed analyses of the Oklo phenomenon have been completed 2 ; 3 . The purpose of this note is to assess the validity of the assumption in these analyses that the neutron spectrum can be described by a Maxwell-Boltzmann (MB) distribution, and to determine the effects on the limit of the time variation of $`\alpha `$ for different neutron spectra. The possibility of a non-MB spectrum was discussed in 2  (footnote 3), but was not considered to be important. However, for the high-accuracy results presented in 3 , the effects due to deviations from a MB spectrum become very important.

## II The Oklo Phenomenon as a Homogeneous Reactor

The fact that the Oklo phenomenon occurred was indicated when uranium taken from this mine was found to be deficient in 235U; subsequent tests confirmed this discovery. From core samples and knowledge of reactor dynamics, the age of the Oklo phenomenon was determined to be about 2 billion years. The conditions necessary for the multiple reactor zones to exist can be used to place constraints upon many parameters such as concentrations of various elements, temperature, moderator type and concentration, etc. while the reactor was operating. For example, it can be shown that only hydrogen or deuterium could have served as moderators at Oklo and hydrogen present in water or as hydration of the uranium oxide appears to be the only plausible choice. As a first approximation to the reactor geometry, it seems reasonable to assume that the Oklo phenomenon was a homogeneous reactor of infinite extent. This simplifies the estimation of the multiplication factor $`k`$ and the neutron flux $`\mathrm{\Phi }(E,T)`$ which we will see depends on the amount of hydrogen and neutron absorbing impurities in the ore.

With the present isotopic ratio of 235U/238U, the maximum $`k`$ that can be obtained in a homogeneous mixture of water and natural uranium is $`k=.838`$, which occurs where there are 2.43 molecules of water per atom of uranium 4  (see table 18.1, p. 612). The fractional isotopic abundance of 235U in natural U at present is 0.711%. Extrapolating this result implies a 235U relative isotopic concentration of about 1.2% to achieve $`k=1`$. Two billion years ago, the relative concentration of 235U was about 3.7% (due to the different lifetimes of 235U and 238U). This implies that two billion years ago, $`k1.3`$ for a system with 2.4 H2O molecules/U atom. If such a large fractional concentration of water was present, the Oklo reactor would have been highly divergent. Of the possible effects that can reduce $`k`$, the two most likely are a low water (or hydrogen) concentration in the U deposit, and the presence of impurities. It is interesting to note that the reactor would have been somewhat self-stabilizing as a runaway to high temperatures would drive water out of the ore deposit.

Precise knowledge of the nature and concentration of neutron-absorbing impurities at the time the Oklo reactor was running is lacking. However, we can make a reasonable estimate of the possible maximum absorption by impurities. The forgoing arguments can made rigorous by estimating $`k`$ as a function of the hydrogen atomic number density fraction, $`f_H=\rho _H/\rho _U`$ and the atomic fraction of absorbing impurities $`f_i=\rho _i/\rho _U`$, relative to the number density of U atoms. With 235U isotopic fraction $`x`$, for thermal neutrons:

$`k`$ $``$ $`\nu p{\displaystyle \frac{\rho _Ux\sigma _f^{235}}{\rho _U\left[x\sigma _a^{235}+(1x)\sigma _a^{238}\right]+\rho _H\sigma _a^H+_i\rho _i\sigma _a^i}}`$ (1)
$``$ $`2.47e^{.7031(1/f_H)^{.58}}`$
$`\times `$ $`{\displaystyle \frac{580x}{690x+2.7(1x)+0.33f_H+_if_i\sigma _a^i}}`$
where $`\nu =2.47`$ is the number of neutrons released per 235U fission, $`p`$ is the resonance escape probability obtained from Eqs. (10.29) and (13.3) of 4 , $`\sigma _f^{235}=580`$ b is the 235U fission cross section, $`\sigma _a^{235}=690`$ b is the total 235U total neutron absorption cross section, $`\sigma _a^{238}=2.7`$ b is the 238U total neutron absorption cross section, $`\sigma _a^H=0.33`$ b is the hydrogen absorption cross section. The total impurity absorption can be parameterized by

$$\beta =\underset{i}{}f_i\sigma _a^i$$
(2)
Furthermore, the effects of oxygen have been neglected. For $`x=.037`$, $`k`$ as a function of $`f_H`$, and as a function of impurity concentration parameterized by $`\beta `$, is shown in Fig. 1. With no impurities, $`k=1`$ is achieved when $`f_H=1.5`$. For a higher hydrogen concentration, the reactor would have run away and the resulting high temperatures would have driven water out of the ore; the system was likely self-stabilizing to $`k=1`$. As the impurity concentration, parameterized by $`\beta `$ in Fig. 1, increases, $`f_H`$ required for $`k=1`$ increases also; at $`\beta =5`$, $`f_H=2.6`$ to achieve $`k=1`$. For $`\beta >11`$ b, it is not possible to achieve $`k1`$. It is also known that the reactor operated until $`x0.02`$ which implies a more restrictive limit of $`\beta 3`$ b, for which $`f_H=5.8`$. We note that criticality calculations at these high 235,238U concentrations are subject to a number of corrections (see 4 , pp. 463-468) so the figures derived here are to be considered as providing guidelines for the operation of the natural reactor which indicates that $`f_H`$ is about 3, with $`\beta =2`$.

A ubiquitous substance that offers a significant thermal neutron absorption cross section is sodium chloride. The thermal absorption cross section for sodium is $`\sigma _a=0.5`$ b, but for chlorine $`\sigma _a=33`$ b which limits $`f_{Cl}<.1`$. The relative atomic concentrations of other impurities can be similarly estimated.

## III Calculation of $`\widehat{\sigma }`$ for a non-MB Neutron Spectrum

It is well-known that when neutrons are moderated in the presence of a $`1/v`$ absorber (such as U), the low-energy part of the spectrum becomes suppressed relative to a high-energy $`1/E`$ component of the flux. The relevant parameter that describes this suppression is (4 , pp. 335- 340)

$$\mathrm{\Delta }=\frac{2A\mathrm{\Sigma }_a(v_T)}{\mathrm{\Sigma }_s}$$
(3)
where $`\mathrm{\Sigma }_a(v_T)=\rho _a\sigma _a(v_T)`$ is net absorption cross section of the homogeneous mixture for a neutron rms velocity corresponding to the moderator temperature, $`\mathrm{\Sigma }_s=\rho _s\sigma _s`$ is the net scattering cross section of the moderating atoms, and $`A`$ is the atomic mass of the moderating atoms. In the present case, for neutron energies about 1 eV, the atomic mass $`A=1`$ for H which is responsible for most of the neutron moderation. When $`\mathrm{\Delta }2`$, the $`1/E`$ tail contains the bulk of the neutrons. This is illustrated in Fig. 2 where the flux as a function of $`\mathrm{\Delta }/2`$ as obtained from a Monte Carlo calculation following the procedure in 6 .

For the parameters derived in the last Section, that is $`f_H=3`$, $`x=0.037`$, and $`\beta =2`$, $`\mathrm{\Delta }1`$. However, for neutron energies less than 1 eV, molecular effects become important; it is no longer a good approximation to assume that the neutron moderation occurs by scattering from free atoms. The chemical bonding effect can be estimated by setting $`A=2`$, so in the low neutron energy region ($`.001<E<0.1`$ eV), $`\mathrm{\Delta }2`$ at 300 K, and scales with temperature as

$$\mathrm{\Delta }=2\sqrt{\frac{300}{T}}.$$
(4)
The elements 149Sm and 155Gd have low energy neutron resonances and are particularly interesting to test for possible time variation of $`\alpha `$. The formalism developed in 1 ; 2 ; 3  for the effective cross section of a substance with a low-energy neutron resonance can be understood as follows. The interaction of a neutron with a nucleus can be parameterized through the optical model, where the Hamiltonian is

$$H=U(E)+iW(E)$$
(5)
where the absorption rate for neutrons with energy $`E`$ is $`\mathrm{\Gamma }(E)=2W(E)/\mathrm{}`$. The absorption cross section can be expressed as

$$\sigma (E)=\frac{g\pi }{k^2}\frac{\mathrm{\Gamma }_n\mathrm{\Gamma }_\gamma }{(EE_r)^2/\mathrm{}^2+\mathrm{\Gamma }_{tot}^{}{}_{}{}^{2}/4}.$$
(6)
where $`\mathrm{}k`$ is the neutron momentum, $`g`$ is a parameter that depends upon the spins of the neutron and interacting nuclei, $`E_r`$ is the resonance energy and $`\mathrm{\Gamma }_{n,\gamma }`$ are the rates for neutron and gamma ray absorption respectively. The parameters $`g`$, $`E_r`$, and $`\mathrm{\Gamma }_{n,\gamma }`$ for elements of interest here can be found in 2 ; 3 .

The absorption cross section at a particular energy can also be described as the product of the rate of absorption and the times $`\tau =L/v(E)`$ spent in the material, normalized to the propagation length $`L`$,

$$\sigma (E)=\mathrm{\Gamma }(E)/v(E).$$
(7)
Far away from $`E_r`$, $`\mathrm{\Gamma }(E)`$ is nearly constant and $`\sigma (E)=\sigma _0v_0/v(E)`$, where $`v_0`$ is the velocity at which the cross section was measured. Nuclei whose cross sections can be described this way are know as “$`1/v`$” absorbers. This is a more efficient representation for thermal neutron absorption of many nuclei such as U.

The net absorption cross section is given by the integral of the cross section time the neutron flux $`\mathrm{\Phi }(E)`$,

$$\sigma =\sigma (E)\mathrm{\Phi }(E)𝑑E.$$
(8)
In assessing the effects of a varying low-energy resonance, because all $`1/v`$ cross sections follow the same universal function which have exactly the same form up to a constant, it is useful to define an effective relative cross section for the nuclei with a varying $`\mathrm{\Gamma }(E)`$ as

$$\widehat{\sigma }=\frac{\sigma (E)\mathrm{\Phi }(E,T)𝑑E}{v_0\rho (E,T)𝑑E}$$
(9)
where $`\sigma (E)`$ is the energy-dependent cross section, $`T`$ is the moderator temperature, $`\mathrm{\Phi }(E,T)`$ and $`\rho (E,T)`$ are the neutron flux and energy distributions, respectively, and $`v_0`$ is the velocity at which $`1/v`$ absorption cross sections are measured.

In this analysis and the others that have been performed so far, the finite temperature and motion of the absorbing nuclei is ignored. This is a small correction to the resonance width because $`A>100`$ for the nuclei being considered, so the absorber velocity is much lower than the neutron velocity. Assuming $`\mathrm{\Delta }=2`$ at 300 K, as a function of $`T`$, $`\mathrm{\Delta }=2\sqrt{300/T}`$. A procedure similar to that described in 3  (numerical integration) was used to calculate the change in $`\widehat{\sigma }`$ as a function of change in resonance energy, but replacing the MB spectrum with spectra derived from Fig. 2. The same resonance parameters as employed in 3  were used, and the numerical integration was tested with a MB spectrum for which the same results as Fig. 1 of 3  were obtained.

It is possible to determine the value of the cross section for 149Sm, $`\widehat{\sigma }_{149}`$, from detailed isotopic analyses of core samples from Oklo and similarly for 155Gd to determine $`\widehat{\sigma }_{155}`$. Such an analysis was performed in 3  and indicates that

$$\widehat{\sigma }_{149}=91\pm 6\mathrm{kb}.$$
(10)
This result can be used subsequently to determine the ancient value of $`E_r`$ which can be compared to the present-day measured value.

Results of the numerical integration for 149Sm are shown in Fig. 2 as a function of moderator temperature with $`\mathrm{\Delta }=2`$ at 300 K. In 3 , the mean temperature of the Oklo reactor was estimated to be about 600 K. From the curve for 600 K in Fig. 3 (expanded around the $`91\pm 6`$ kb in the lower plot), we find that the change in resonance energy is

$$\mathrm{\Delta }E_r=\left[45\begin{array}{cc}+7& \\ 15& \end{array}\right]\times 10^3\mathrm{eV}$$
(11)
which indicates more than a $`6\sigma `$ deviation from zero. Note that the“two solution” problem does not really exist in this case, but the upper magnitude range is expanded.

In the calculation of the moderated neutron spectrum, effects of chemical bonds (which suppress the low energy spectrum) have been approximately included. As the atoms become more tightly bound, $`A\mathrm{}`$ so ($`\mathrm{\Delta }\mathrm{}`$), and in this limit the neutron flux spectrum becomes pure $`1/E`$; the result of a calculation for this case is shown in Fig. 4. In this case, for which two solutions exist,

$$\mathrm{\Delta }E_r=(135\pm 5)\times 10^3\mathrm{eV}\mathrm{or}(58\pm 5)\times 10^3\mathrm{eV}.$$
(12)
This result is roughly consistent with the $`\mathrm{\Delta }=2`$ result; reality likely is somewhere between the $`\mathrm{\Delta }=`$2 and $`\mathrm{}`$ results. However, the result for $`\mathrm{\Delta }=2`$ clearly indicates a non-zero change in $`E_r`$ at a level of more than $`6\sigma `$.

Results for a calculation of 155Gd are shown in Fig. 5. The interpretation of the 155Gd data is complicated by the presence of impurities, and an extensive analysis is given in 3 . The Oklo data imply $`\widehat{\sigma }_{155}28\pm 10`$ kb, which, from Fig. 5, indicates, for the left-hand solution,

$$\mathrm{\Delta }E_r=(90\pm 20)\times 10^3\mathrm{eV}$$
(13)
This is consistent with the 149Sm result because impurities shift $`E_r`$ slightly, and the simple $`1/E`$ spectrum overestimates $`E_r`$.

## IV Interpretation of the Results

A shift in resonance energy can be related to a shift in $`\alpha `$ by

$$\frac{\mathrm{\Delta }\alpha }{\alpha }=\frac{\mathrm{\Delta }E_r}{E_0}.$$
(14)
A reasonable estimate of $`E_0=1`$ MeV was presented in 2 , and is roughly the same for 149Sm and 155Gd. Taking the result Eq. (11) determines

$$\frac{\alpha _{now}\alpha _{past}}{\alpha }=\left[45\begin{array}{cc}+15& \\ 7& \end{array}\right]\times 10^9$$
(15)
which is non-zero by more than $`6\sigma `$. The central value plus twice the upper uncertainty can be used to set a 95% confidence limit on the magnitude of the integrated rate of change over the last two billion years

$$|\frac{\dot{\alpha }}{\alpha }|<3.8\times 10^{17}/\mathrm{yr}(95\%\mathrm{conf})$$
(16)
By assuming higher temperatures, this limit decreases slightly. However, a significant modification of this result requires temperatures beyond physically reasonable values as assumed in 3 .

It is expected that the neutron absorption resonance parameters (e.g., the neutron and gamma widths), other than $`E_r`$, do not change significantly with $`\alpha `$. In estimating $`E_0`$ it was assumed that $`E_r`$ represents a fixed energy above the ground states of nuclei with $`A`$ and $`A+1`$, and $`E_0`$ is approximately the difference in the Coulomb energies of the ground states. This result is in agreement with a more sophisticated analysis 7 .

## V Conclusion

If a $`1/v`$ absorber is present in the moderator of a neutron chain reactor, the neutron energy spectrum can deviate significantly from the a Maxwell-Boltzmann distribution. The Oklo phenomenon was rich in uranium which is a strong $`1/v`$ absorber. By considering realistic deviations from a Maxwell-Boltzmann low-energy neutron spectrum, we have shown that a recent analysis of the Oklo natural reactor phenomenon implies an non-zero ($`>6\sigma `$) variation of $`\alpha `$ over the last 2 billion years. The result is of opposite sign and an order of magnitude smaller than a recent astrophysical determination of the change in $`\alpha `$ 8 , which is non-zero, but over a different time scale. It has been suggested that the time variation of $`\alpha `$ is not monotonic 8a . Our results are probably accurate to within 20%; a full MCNP model of the reactor, assuming reasonable estimates of the temperature and impurities are possible, would be useful in light of the importance and interest in the possibility of a varying $`\alpha `$. Finally, these results might be interpreted more efficiently in terms of $`m_q/\mathrm{\Lambda }_{QCD}`$ for which the sensitivity is about two orders of magnitude higher than the sensitivity to $`\alpha `$ variation 9 .

We thank Tuan Nguyen for critical comments and in particular for clarifying the issues with the sign of the effect.


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# The Diffusion Equation on a Hypersphere

## Abstract

We study the diffusion equation on the surface of a $`4D`$ sphere and obtain a Kubo formula for the diffusion coefficient.

Since numerical simulations of fluids or plasmas within hyperspherical boundary conditions are appealing, it is not without interest to dispose of an explicit expression for the diffusion coefficient $`D`$ in terms of time averages of microscopic quantities.Hansen  Our starting point will be the diffusion equation

$$𝒟\rho (M,t)\left(\frac{}{t}D\mathrm{\Delta }^{𝒮_3}\right)\rho (M,t)=0,$$
(1)
where the point $`M`$ lives on the surface of the four dimensional ($`4D`$) sphere $`𝒮_3`$ of center $`O`$ and radius $`R`$ (a hypersphere for short). $`D(>0)`$ is the diffusion coefficient and $`\mathrm{\Delta }^{𝒮_3}`$ is the Laplacian appropriate to the geometry.Nissfolk ; Caillol1  Eq. (1) was solved recently by Nissfolk et al.; their expression for $`\rho (M,t)`$ is however akward and does not allow to obtain an explicit expression for $`D`$. A more convenient expression for $`\rho (M,t)`$ is obtained in this paper which yields an explicit expression for $`D`$.

We first note that the Brownian motion of a particle in $`𝒮_3`$ may also be viewed as the Brownian rotation of a linear $`4D`$ molecule. As the expression of the rotational diffusion coefficient of a $`3D`$ rotator is known since the work of Debye Debye ; Berne ; Caillol2  it should be easy to extend this old result to the $`4D`$ case. Following Berne and Pecora Berne  we first expand $`\rho (M,t)`$ on the complete basis set of hyperspherical harmonics Caillol1 ; Bander

$$\rho (M,t)=\underset{L=0}{\overset{\mathrm{}}{}}\underset{𝜶}{}\rho _{L,𝜶}(t)Y_{L,𝜶}(𝝃),$$
(2)
where the unit vector $`𝝃=𝑶𝑴/R`$ denotes the orientation of vector $`𝑶𝑴`$ in $`\mathrm{}^4`$ and $`Y_{L,𝜶}(𝝃)`$ is a $`4D`$ hyperspherical harmonics. We recall that the quantum number $`L`$ is a positive integer and that $`𝜶=(m_1,m_2)`$ where $`m_i(i=1,2)`$ takes the $`L+1`$ values $`m_i=L/2,L/2+1,\mathrm{},L/2`$. The $`4D`$ harmonics $`Y_{L,𝜶}(𝝃)`$ satisfy the following properties:Caillol1 ; Bander

* (i) orthogonality

$$𝑑\mathrm{\Omega }(𝝃)Y_{L,𝜶}^{}(𝝃)Y_{L^{},𝜶^{}}(𝝃)=\delta _{L,L^{}}\delta _{𝜶,𝜶^{}},$$
(3)
where $`d\mathrm{\Omega }(𝝃)`$ denotes the infinitesimal volume element (or $`4D`$ infinitesimal solid angle) on the hypersphere of unit radius.
* (ii) completeness

$$\underset{L,𝜶}{}Y_{L,𝜶}^{}(𝝃)Y_{L,𝜶}(𝝃^{})=\delta ^{𝒮_3}(𝝃,𝝃^{}),$$
(4)
where $`\delta ^{𝒮_3}`$ is the Dirac distribution for the unit hypersphere defined as

$$𝑑\mathrm{\Omega }(𝝃)f(𝝃)\delta ^{𝒮_3}(𝝃,𝝃^{})=f(𝝃^{}).$$
(5)
* (iii) addition theorem

$$\underset{𝜶}{}Y_{L,𝜶}^{}(𝝃)Y_{L,𝜶}(𝝃^{})=P_L(𝝃𝝃^{}),$$
(6)
where the dot denotes the usual $`4D`$ scalar product, i.e $`𝝃𝝃^{}=\mathrm{cos}(\psi )`$ where $`\psi `$ is the angle between the two unit vectors $`𝝃`$ and $`𝝃^{}`$ and

$$P_L\left(\mathrm{cos}\left(\psi \right)\right)=\frac{L+1}{2\pi ^2}\frac{\mathrm{sin}(L+1)\psi }{\mathrm{sin}(\psi )}.$$
(7)
Note that $`R\psi `$ is the geodesic length between the points $`M`$ and $`M^{}`$ of $`𝒮_3`$.

Moreover the $`Y_{L,𝜶}(𝝃)`$ are the eigenvectors of the Laplace-Beltrami operator $`\mathrm{\Delta }^{𝒮_3}`$ with eigenvalues $`L(L+2)/R^2`$. Caillol1 ; Bander It follows from this important property that eq. (1) is equivalent to the set of equations

$$\left(\frac{}{t}+D\frac{L(L+2)}{R^2}\right)\rho _{L,𝜶}(t)=0,$$
(8)
the solution of which reads obviously as

$$\rho _{L,𝜶}(t)=\rho _{L,𝜶}(0)\mathrm{exp}\left(DL\left(L+2\right)t/R^2\right).$$
(9)
We shall denote by $`\rho (M,t|M_0,0)`$ the solution of (1) corresponding to the initial condition $`\rho (M,0)=\delta ^{𝒮_3}(M,M_0)R^3\delta ^{𝒮_3}(𝝃,𝝃_0)`$, i.e. the solution of

$$𝒟\rho (M,t|M_0,0)=\delta (t)R^3\delta ^{𝒮_3}(𝝃,𝝃_0).$$
(10)
It follows readily from eqs. (9) and (4) that the Green function $`\rho (M,t|M_0,0)`$ can be expressed as

$`\rho (M,t|M_0,0)`$ $`=`$ $`0(t<0)`$
$`\rho (M,t|M_0,0)`$ $`=`$ $`{\displaystyle \frac{1}{R^3}}{\displaystyle \underset{L,𝜶}{}}Y_{L,𝜶}^{}(𝝃_0)Y_{L,𝜶}(𝝃)\mathrm{exp}\left(DL\left(L+2\right)t/R^2\right)(t>0).`$ (11)
Eq. (The Diffusion Equation on a Hypersphere) can be further simplified with the help of the addition theorem (6) which yields our final result

$$\rho (M,t|M_0,0)=\frac{1}{R^3}\underset{L}{}P_L(𝝃_0𝝃)\mathrm{exp}\left(DL\left(L+2\right)t/R^2\right)(t>0).$$
(12)
Some comments are in order.

(i) The solution (12) is invariant upon rotations about the axis $`𝝃_0`$ as expected. Eq. (12) is a trivial generalization of Debye’s resultDebye ; Berne ; Caillol2  (for the $`3D`$ rotor the Tchebychev polynomial $`P_L`$ in eq. (12) has to be replaced by a Legendre polynomial, up to a multiplicative constant)

(ii) Note that

$$R^3𝑑\mathrm{\Omega }(𝝃)\rho (M,t|M_0,0)=1(t>0),$$
(13)
i.e. the probability is conserved, the particle does not evaporate.

(iii) We have also

$$\underset{t+\mathrm{}}{lim}\rho (M,t|M_0,0)=\frac{1}{2\pi ^2R^3},$$
(14)
i.e. the solution of the diffusive process is uniform after infinite time (the volume of $`𝒮_3`$ is equal precisely to $`2\pi ^2R^3`$)

(iv) Let us define, following Berne and PecoraBerne , the time correlation function

$`C_L(t)`$ $``$ $`P_L\left(𝝃\left(0\right)𝝃\left(t\right)\right)`$ (15)
$`=`$ $`{\displaystyle \frac{d\mathrm{\Omega }(𝝃_0)}{2\pi ^2}R^3𝑑\mathrm{\Omega }(𝝃)P_L(𝝃_0𝝃)\rho (M,t|M_0,0)},`$
where we have averaged the initial position uniformly on $`𝒮_3`$. As a consequence of the orthogonality properties of the $`P_L`$ we find that

$$C_L(t)=\frac{(L+1)^2}{2\pi ^2}\mathrm{exp}\left(DL\left(L+2\right)t/R^2\right).$$
(16)
Defining now the reorientational time $`\tau _L`$ of our $`4D`$ rotor as

$`\tau _L`$ $`=`$ $`{\displaystyle _0^{\mathrm{}}}𝑑t{\displaystyle \frac{C_L(t)}{C_L(0)}}`$ (17)
$`=`$ $`{\displaystyle \frac{R^2}{DL(L+2)}},`$
we have now at our disposal an explicit expression of the diffusion coefficient $`D`$. Note the aesthetic relation $`\tau _L/\tau _L^{}=L^{}(L^{}+2)/L(L+2)`$ which generalizes Debye’s relation to the $`4D`$ rotor.

(v) It does not seem possible to obtain from eqs. (16) an expression for $`D`$ in term of the time autocorelation function of the velocity of the particle. Moreover one can deduce from eq. (12) that the mean square displacement of the stereographic projection of point $`M`$ vanishes for $`t\mathrm{}`$.

It remains now to show that the expression (12) of $`\rho (M,t|M_0,0)`$ is equivalent to that of ref.Nissfolk, . This can be done as follows. Let us rewrite the reduced $`\widehat{\rho }=2\pi ^2R^3\rho (M,t|M_0,0)`$ as

$$\widehat{\rho }=\underset{L=0}{\overset{\mathrm{}}{}}(L+1)\frac{\mathrm{sin}(L+1)\psi }{\mathrm{sin}\psi }\mathrm{exp}(KL(L+2)),$$
(18)
where $`K=Dt/R^2`$. A priori the angle $`\psi `$ is in the range $`(0,\pi )`$, however since the function is formally even in $`\psi `$ we define $`\widehat{\rho }(\psi )=\widehat{\rho }(\psi )`$ for negative angles. This gives us a periodic function of period $`2\pi `$ defined for all $`\psi \mathrm{}`$. We introduce now the periodic function

$$F(\psi )=_0^\psi 𝑑\psi ^{}\widehat{\rho }(\psi ^{})\mathrm{sin}(\psi ^{})$$
(19)
which can be rewritten after some algebra as

$$F(\psi )=F_0\frac{\mathrm{exp}K}{2}\underset{p=\mathrm{}}{\overset{+\mathrm{}}{}}\mathrm{exp}\left(Kp^2\right)\mathrm{exp}(ip\psi )$$
(20)
where $`F_0`$ is some unessential constant independent of angle $`\psi `$. At this point we recall Poisson summation theorem which states that for any function $`\phi (x)`$ holomorphic in the strip $`a<\mathrm{}z<a`$ one has

$$\underset{n=\mathrm{}}{\overset{+\mathrm{}}{}}\phi (x+2n\pi )=\frac{1}{2\pi }\underset{p=\mathrm{}}{\overset{+\mathrm{}}{}}\mathrm{exp}(ipx)\stackrel{~}{\phi }(p),$$
(21)
where

$$\stackrel{~}{\phi }(p)=_{\mathrm{}}^+\mathrm{}𝑑x\phi (x)\mathrm{exp}(ipx).$$
(22)
Applying Poisson theorem for the Gaussian we get

$$F(\psi )=F_0\frac{\sqrt{\pi }\mathrm{exp}K}{2\sqrt{K}}\underset{n=\mathrm{}}{\overset{+\mathrm{}}{}}\mathrm{exp}\left(\frac{(\psi +2n\pi )^2}{4K}\right),$$
(23)
which, after differentiation yields for $`\widehat{\rho }`$

$$\widehat{\rho }(\psi ,t)=\frac{\sqrt{\pi }\mathrm{exp}K}{4K^{3/2}\mathrm{sin}\psi }\underset{n=\mathrm{}}{\overset{+\mathrm{}}{}}(\psi +2n\pi )\mathrm{exp}\left(\frac{(\psi +2n\pi )^2}{4K}\right),$$
(24)
which coincides with the result of ref.Nissfolk,  apart the prefactor which is not specified.

###### Acknowledgements.

The author likes to thank J.-J. Weis for drawing his attention to ref. Nissfolk, .


text:
# Studies of Proximity Focusing RICH with an aerogel radiator using Flat-panel multi-anode PMTs (Hamamatsu H8500)

## 1 Introduction

Silica aerogel is a unique material with a refractive index ($`n`$) in the range between gases and liquids or solids. Its refractive index can be easily controlled from $`n=1.01`$ to $`1.06`$. As a result, the refractive index of the aerogel can be chosen such that for a given momentum interval in the few GeV/$`c`$ region charged pions radiate Cherenkov photons, while kaons stay below the Cherenkov radiation threshold . In the Belle experiment at KEK , a threshold type Cherenkov detector (Belle-ACC)  which uses aerogel as a radiator, is operated, providing at $`3.5\mathrm{GeV}/c`$ a kaon identification efficiency of $`88`$% with a pion missidentification probability of $`8`$% .

A new production method of hydrophobic aerogel with a high transmission length and $`n`$ in the interval between $`1.01`$ and $`1.03`$ was developed during the construction period of Belle-ACC . The improvement in quality allows the use of an aerogel radiator in a ring imaging Cherenkov counter (RICH) . In the HERMES experiment at DESY, a RICH counter is used with a dual-radiator (aerogel and gas), and mirrors to focus the Cherenkov photons . A similar detector is also designed for the LHCb experiment at CERN .

We are studying the feasibility of a RICH counter with an aerogel radiator for the Belle-ACC in the forward end-cap region . Since this part is now optimized for the pion/kaon separation needed for tagging of the $`B`$ flavor, and covering the momentum range below $`2\mathrm{GeV}/c`$, separation at high-momentum region of around $`4\mathrm{GeV}/c`$ is not adequate. This kinematic region is, however, very important for the studies of two-body decays such as $`B\pi \pi `$, $`K\pi `$. In order to achieve a $`\pi `$/$`K`$ separation for a wider momentum range, a ring imaging-type of detector is needed. Due to spatial restrictions, such a counter has to be of the proximity focusing type. To cover the identification in the lower momentum region (around $`0.7\mathrm{GeV}/c`$) as well as in the region up to $`4\mathrm{GeV}/c`$, the aerogel has to have a refractive index around $`n=1.05`$. The first beam test of such a detector was carried out in 2001 at the KEK-PS $`\pi 2`$ beam line . These tests used an array of multi-anode PMTs (Hamamatsu R5900-M16) for photo-detection. The detected number of photoelectrons was $`2.7`$ per ring for a $`2\mathrm{cm}`$ thick aerogel tile with $`n=1.05`$, and the Cherenkov angle resolution per photon was $`10\mathrm{mrad}`$. These results were consistent with expectations. The number of detected photons was, however, rather low, partly because only $`36`$% of the detector surface was covered by the photo-cathodes, and partly because the transmission length of the aerogel with $`n=1.05`$ could not be made large enough. For the second beam test, we improved the aerogel transmission by optimizing the materials used in the production process. The active area fraction of the photon detector was increased by employing recently developed flat-panel PMTs, Hamamatsu H8500. Although this type of PMT is not immune to magnetic field, and therefore cannot be applied in the Belle spectrometer, we consider this device as an intermediate step in our development. The paper is organized as follows. We first present the experimental set-up with flat-panel PMTs, briefly review the improvement in aerogel production, describe the measurements, and finally discuss the results.

## 2 The experiment set-up

### 2.1 Flat-panel PMT

The photon detector for the tested prototype RICH counter employed $`64`$ channel multi-anode PMTs (Hamamatsu H8500, so called flat-panel PMT) because of their large effective area. 16 PMTs were used in a $`4\times 4`$ array and aligned with a $`52.5\mathrm{mm}`$ pitch, as shown in Figure 1. The surface of each PMT is divided into $`64`$ ($`8\times 8`$) channels with a $`6.0\times 6.0\mathrm{mm}^2`$ pixel size. Therefore, the effective area of photon detection is increased to $`84\%`$. At the back of each PMT, an analog memory board is attached to read out multi-channel PMT signals, as described below. Among $`16`$ PMTs, $`8`$ PMTs were delivered in January, 2002, and the remaining PMTs were delivered in October, 2002. Since the manufacture method of the PMT was still under development, they exhibit a large variation in quantum efficiency and gain. The quantum efficiency at 400 nm varies between $`16`$% and $`25`$%; the gain varies from $`110^6`$ to $`610^6`$ when the maximal allowed high voltage of $`1100`$ V is applied to the photo-cathode . The PMTs from the later batch show a slightly better performance.

### 2.2 Aerogel radiator

The hydrophobic form of the aerogel radiator from Novosibirsk  is known to have a long transmission length. However we prefer hydrophobic aerogel than hydrophilic one for the application to a collider experiment. With a low refractive index ($`n=1.011.03`$), such an aerogel was developed for the Belle-ACC, and is characterized by a high transmission length ($`40`$ mm at a wave length of 400 nm) which was not achieved before. However, the transmission length of aerogel with a higher refractive index of $`n=1.05`$ fell below one half the value compared to the aerogel with $`n=1.03`$. Therefore, we reexamined the aerogel production technique in a joint development with Matsushita Electric Works Ltd. As a result, we found that the important factors determining the transmission length are the solvent and selection of the precursor to be used for its production. Originally, we used methyl-alcohol for the solvent, and methyl-silicate as a precursor . When we applied di-methyl-formamide (DMF) , and changed the supplier of the precursor, we could improve the transmission length of the aerogel.

Figure 2 shows the refractive indices of aerogel and the relation to transmission length for samples which were used in this beam test. The refractive index was determined by measuring the deflection angle of laser light (laser diode: $`405\mathrm{nm}`$) at a corner of each aerogel tile; the transmission length was measured with a photo-spectrometer (Hitachi U-3210). In addition to the samples produced with the new technique at Matsushita Electric Works Ltd. and Chiba university, samples from BINP (Novosibirsk) were tested ; for comparison, we also tested the samples used in the previous beam test. The thicknesses of the prepared aerogel samples ranged from $`10\mathrm{mm}`$ to $`25\mathrm{mm}`$. Various thickness of up to about $`50\mathrm{mm}`$ were tested by stacking these samples. Note that in the production of the aerogel samples at BINP propenol was used as the solvent, and the resulting aerogel was hydrophilic. Also note that the Matsushita aerogel samples produced with the new technique have a very similar transmission length as the BINP samples. The transmission length for $`n1.05`$ samples used in the first beam test was around $`15`$ mm, but was increased to $`45`$ mm for Matsushita’s sample with the new production method.

### 2.3 Beam set-up

For the beam test, pions with momenta between $`0.5\mathrm{GeV}/c`$ and $`4\mathrm{GeV}/c`$ were used. Beside the RICH detector under study, counters for triggering, tracking and particle identification were employed.

The set up of the aerogel RICH is shown in Figure 3. Two RICH counters were placed in a light-shield box and tested simultaneously. Each RICH was composed of a layer of aerogel radiator and a photo-detection plane, parallel to the radiator face at a distance of $`20\mathrm{cm}`$. The upstream Cherenkov counter was the detector under study; the downstream counter was the one employed in the previous beam test. Since the latter uses a well-known photo-detector, multi-anode PMTs Hamamatsu R5900, we regarded it as a reference.

Particle identification was done to remove particles other than pions. Two CO2 gas Cherenkov counters in the beam line were used to exclude electrons. Also, an aerogel counter was equipped and used to exclude protons for the high-momentum region. This detector was also used to exclude muons for the low-momentum region around $`0.5\mathrm{GeV}/c`$.

The particle trajectories were measured with multi-wire proportional chambers (MWPC) at the upstream and downstream ends of the light-shield box. These $`5\times 5\mathrm{cm}^2`$ MWPCs, with $`20\mu `$m diameter, gold-plated tungsten anode wires at $`2\mathrm{mm}`$ pitch and with $`90\%`$ Ar + $`10\%`$ $`\mathrm{CH}_4`$ gas flow, were read out by delay lines on the x and y cathode strips.

The trigger signal was generated as a coincidence of signals from several $`5\times 5\mathrm{cm}^2`$ plastic scintillation counters and anode signals from the MWPCs to ensure valid tracking information.

### 2.4 Readout electronics

For the beam test, a new read-out system was designed by using analog memory chips. The analog memory chip is based on a chip developed by H. Ikeda  for a cosmic-ray experiment. We borrowed the chips from NASDA (National Space Development Agency of Japan), and developed the chip control system. In the analog memory chip, the signals of 32 channels are preamplified, sampled in $`1\mu `$s intervals, and stored in an 8 steps deep analog pipeline. Figure 4 shows a schematic view of the readout system with these analog memories. Two 32 channel analog memories are attached to each 64 channel PMT. The memories corresponding to four PMTs are controlled by a 256 channel memory controller. When the gate pulse is formed from the trigger signal, a control signal is sent from the controller to the analog memories. The difference in the value of the analog memory between the latest and the first memory content is fed to the output. The obtained output values of 256 channels are clocked into one signal train with a period of 10 $`\mu `$s per channel. Each analog memory controller outputs the serial signal together with synchronized control signals. These signals are then read by a 12-bit VME ADC (DSP8112, MTT Co.) with a conversion time of 5 $`\mu `$s.

### 2.5 Reference RICH

A reference RICH was instrumented with multi-anode PMTs, Hamamatsu R5900-M16, the same photon detector as used in the previous test . The quantum efficiency of the PMTs is around 26% (at 400 nm), and the gain was around $`610^6`$ with $`900`$ V applied to the photo-cathode. The PMTs were grouped in a $`2\times 6`$ array at a $`30`$ mm pitch. Due to a limited number of available PMTs and read-out channels, only a part of the Cherenkov ring was covered with photon detectors.

## 3 Measurement and results

Most of the test measurements were performed with a $`\pi ^{}`$ beam at $`3\mathrm{GeV}/c`$. To systematically evaluate the detector performance, data were taken with different aerogel samples with various transmission lengths and thicknesses. Data were also taken by varying the $`\pi ^{}`$ momentum in the range from $`0.5\mathrm{GeV}/c`$ to $`4.0\mathrm{GeV}/c`$.

A few typical events are displayed in Figure 5. The hits on PMTs can be associated with the expected position of the Cherenkov ring. The hit near the center of the ring is due to Cherenkov radiation generated by the beam particle in the PMT window. The distribution of accumulated hits is shown in Figure 6. Cherenkov photons from the aerogel radiator are clearly seen with a low background level. The background hit distribution on the photon detector is consistent with the assumption that it originates from Cherenkov photons which were Rayleigh scattered in the radiator.

The pulse-height distribution of the Cherenkov photons detected in one of the flat-panel PMT is shown in Figure 7. The raw data were corrected as follows. A common-mode fluctuation of the base line was subtracted and signals due to cross-talk in the read-out electronics were removed. The signal mainly containing one photoelectron is clearly separated from the pedestal peak. Note, however, that this distribution differs considerably from tube to tube because of the large variation in performance, as described before. For further analysis we also applied a threshold cut to suppress the pedestal noise contribution.

### 3.1 Cherenkov-angle resolution for single photons

Figure 8(a) shows a typical distribution of the Cherenkov-angle for single photons. The angular resolution was obtained from a fit of this distribution with a Gaussian signal and a linear function for the background. Figure 9 shows the resolution in the Cherenkov angle for the $`\pi ^{}`$ beam at $`3\mathrm{GeV}/c`$ and $`20`$ mm thick aerogel samples. The resolution was around $`14`$ mrad, independent of the refractive index. The main contributions to the resolution of the Cherenkov angle come from the uncertainty in the emission point and from the pixel size of the PMT. The first contribution is estimated to be $`\sigma _{emp}=d\mathrm{sin}\theta _c\mathrm{cos}\theta _c/L\sqrt{12}`$, where $`d`$ is the aerogel thickness, $`\theta _c`$ is the Cherenkov angle and $`L`$ is the distance from an average emission point in the aerogel to the surface of the PMT. The second contribution is $`\sigma _{pix}=a\mathrm{cos}^2\theta _c/L\sqrt{12}`$, where $`a`$ is the pixel size. The measured variation of the resolution with the thickness of aerogel is shown in Figure 10. By comparing the measured resolution and the expected values, we observed a rather good agreement. There was, however, a discrepancy between the two, which can be accounted for by a contribution of about $`6`$ mrad. The discrepancy could arise from the effect of aerogel (non-flat aerogel surface and possible non-uniformities in the refractive index due to position variation and chromatic dispersion), which are subject to further investigation. The uncertainty in the track direction is expected to be negligible at $`3\mathrm{GeV}/c`$, but increases considerably at low momenta ($`0.5\mathrm{GeV}/c`$) due to the effect of multiple-scattering, as can be seen in Figure 11.

### 3.2 Photoelectron yield

Figure 8(b) shows a typical distribution of the number of hits within $`\pm 3\sigma `$ from the average Cherenkov angle. The number of hits for the signal region was estimated by subtracting the background from the fits to the Cherenkov-angle distribution. The number of detected photons ($`N_{pe}`$) depends on the aerogel thickness and the effect of scattering. It is expressed as
$`N_{pe}=C_0^dϵ(\lambda )\lambda ^2\mathrm{sin}^2\theta _c\mathrm{exp}(\frac{x}{\mathrm{\Lambda }(\lambda )\mathrm{cos}\theta _c})d\lambda dxC^{}\mathrm{sin}^2\theta _c\mathrm{\Lambda }\mathrm{cos}\theta _c(1\mathrm{exp}(\frac{d}{\mathrm{\Lambda }\mathrm{cos}\theta _c}))`$, where $`\mathrm{\Lambda }`$ is the transmission length of the aerogel at an average wave length of $`400`$ nm and $`ϵ(\lambda )`$ is quantum efficiency of the PMT. Figure 12 shows the dependence of the number of detected photons on the aerogel thickness. As expected from the above expression, the number of photons does not linearly increase with the aerogel thickness, but saturates due to the scattering effect in aerogel. Figure 13 shows the dependence of the number of photons with transmission length. From the figure the benefit of the improvement in the transmission length of the $`n=1.05`$ aerogel from around $`15`$ mm, as used in the previous beam test, to $`45`$ mm using the new production technique becomes evident. The dependence on the pion momentum, displayed in Figure 14, is fitted with the form expected from the Cherenkov relations, and shows a good agreement. For pions with momenta above $`1\mathrm{GeV}/c`$, the number of detected Cherenkov photons was typically around 6 for aerogel samples with $`n=1.05`$.

The performance of the RICH counter under study was compared in the same set-up with the performance of the reference counter with a well-known photon detector, Hamamatsu R5900-M16 multi-anode PMTs. Since the two counters have a different active area fraction ($`84`$% for the flat-panel PMTs, and $`36`$% for the R5900-M16 PMTs) and a different acceptance, the comparison of the photon yields was made by normalizing to the full active surface. While the flat-panel yield for a particular case was $`6.2`$, which resulted in $`7.8`$ if extrapolated to the full active area, the corresponding number for the R5900-M16 was $`12`$. It appears that this difference is mainly due to the rather low quantum efficiency and amplification of some of the flat-panel tubes employed. This, in turn, causes inefficiencies in single photon detection with a given threshold. If the best tube in the set is normalized to the full acceptance, the corresponding number increases to $`10`$, and we would expect about 8 photons per ring.

### 3.3 Particle Identification

Finally, we estimate the performance of pion/kaon separation in the momentum range of around $`4\mathrm{GeV}/c`$, which is of considerable importance for the Belle experiment. If we take into account a typical measured value for the single-photon angular resolution, $`\sigma _c14`$ mrad, and the number of detected photons $`N_{pe}6`$, typical for 20 mm thick aerogel samples with $`n=1.05`$, we can estimate the Cherenkov angle resolution per track to be $`\sigma _c/\sqrt{N_{pe}}=5.7`$ mrad. This naive estimate is also confirmed by the direct measurement shown in Figure 15. Here, the track-by-track Cherenkov angle is calculated by taking the average of the angles measured for hits around the predicted position of the Cherenkov ring. From this we can deduce that at $`4\mathrm{GeV}/c`$, where the difference of Cherenkov angles for pions and kaons is $`23`$ mrad, a $`4\sigma `$ separation between the two is possible. As an additional cross check, we have also collected data with the pion beam of $`1.1\mathrm{GeV}/c`$, which can be used to represent a kaon beam of $`4\mathrm{GeV}/c`$ (apart from a slightly larger sigma due to multiple scattering). As can be seen from Figure 15, the two peaks are well separated. Thus, the proximity focusing aerogel RICH seems to be promising for the upgrade of the Belle PID system at the forward region.

## 4 Conclusions

We report on the test beam results of a proximity focusing RICH using aerogel as the radiator. To obtain larger photoelectron yields, we used flat-panel multi-anode PMT with a large effective area, and aerogel samples produced with a recently developed method which have a higher transmission length than before. We also developed a multi-channel PMT read-out system using analog memory chips. A clear Cherenkov ring from the aerogel radiator could be observed, and the number of photons was enhanced compared to that in previous tests. We performed a systematic study of the detector using various samples of the aerogel. The typical angular resolution was around $`14`$ mrad and the number of detected photoelectrons was around $`6`$. The pion/kaon separation at $`4\mathrm{GeV}/c`$ is expected to be around $`4\sigma `$.

However, we still have some issues which have to be solved for implementation in the Belle spectrometer. The most important item is the development of a PMT which can be operated under a strong magnetic field (1.5T). An example of a candidate for such a device is a multi-anode hybrid photodiode (HPD) or hybrid avalanche photodiode (HAPD). Of course, for a good candidate, its ability to efficiently detect single photons on a large active area has to be demonstrated. The other item is mass production of the aerogel tiles. While we have demonstrated that the new production method significantly increases the transmission length of the $`n=1.05`$ aerogel, the production method has to be adapted to stable good-quality manufacturing. We will study these items at the next stage towards construction of a real detector.

## 5 Acknowledgment

We would like to thank the KEK-PS members for operation of accelerator and for providing the beam to the $`\pi 2`$ beam line. We also thank H. Ikeda (KEK) and the Meisei Co. for their help in preparing the read-out electronics, the Matsushita Electric Works Ltd. for the good collaboration in developing the new aerogel type, and Hamamatsu Photonics K.K. for their support in equipping the photon detector. We also thank A.Bondar (BINP, Novosibirsk) for providing us excellent aerogel samples, and Dr. T.Goka of NASDA for providing us their read-out chips. One of the authors (T.M.) is grateful to Fellowships of the Japan Society for the Promotion of Science (JSPS) for Young Scientists. This work was supported in part by a Grand-in-Aid for Scientific Research from JSPS and the Ministry of Education, Culture, Sports, Science and Technology under Grant No. 13640306, 14046223, 14046224, and in part by the Ministry of Education, Science and Sports of the Republic of Slovenia.