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# Collective ferromagnetism in two-component Fermi-degenerate gas trapped in finite potential

## I Introduction

Recent developments of laser trapping and cooling of atomic gases, which realized the Bose-Einstein condensates (BEC) for Alkali atoms , have opened up new interests for condensed atomic gases with multi-components: multi-component BEC  and fermi degenerate (FD) gas , and also bose-fermi mixed gas in trapped potentials .

One of interesting physics in such systems is the phase structures in the ground states. In general, multi-component systems show a variety of phase structures and phase transitions between them. A typical example is seen in the superfluid 3He (a system with $`2\times 2`$ components of orbital and spin angular momenta), where there exist more than two condensed phases resulted from different combinations of condensed components .

In the condensed system of trapped atomic gases with multi-components, several studies have been done about new phases and phase transitions: the BCS states in attractive two-component fermi gas , a transition to the superfluid states in the crossover region between BCS and BEC theories , phase separations of different components in the BEC , fermi gas  and bose-fermi mixed system .

In this paper, we discuss the trapped fermi-degenerate atomic gas with two-components: $`m=\pm 1/2`$ (magnetic quantum number) states of spin-$`1/2`$ atoms, or two of the hyperfine states of fermionic atoms with larger total spin ($`F>1/2`$). Thus, we denote these components as spin degrees of freedom (up and down components, or up and down atoms) in this paper.

When the interaction between different spin components is weak, the stable ground state of the system has a symmetric state in spin-component distributions at $`T=0`$ where equal number of up and down atoms make similar fermi-degenerate distributions so that the total spin of the whole system vanishes (paramagnetic state). However, for sufficiently strong interactions between components, an asymmetric state with unequal numbers of up/down atoms can be stable because it can be energetically favorable to increase the fermi energy of one component rather than the increase of the interaction energy between up-down components. (The interaction energy between up-up/down-down components can be neglected due to the Pauli blocking effects.) We call it “collective ferromagnetic state” of two-component fermi gas.

As the terms “paramagnetic” and “ferromagnetic” suggest, this theory is related with a mechanism of the metallic magnetism, originally proposed by Bloch and developed by Stoner et.al. , where fermi particles are the electrons in conductive bands. It should be noted that, in the theory of metallic magnetism, a role of $`E_{\mathrm{int}}`$ is done by the Hartree-Fock exchange energy. Studies of “collective ferromagnetic states” of atom gas are also interesting as experimental testing grounds of theoretical ideas in magnetism. Recently, such ferromagnetism aroused new interests in neutron-star physics as a mechanism of the magnetar (neutron stars with strong magnetic fields) .

In the uniform system, such ferromagnetic states have been discussed for the atom gas of 6Li in relation with the stability of the BCS states . The ferromagnetic states have also been discussed on the trapped BEC where the interactions between different spin components are the origin of the asymmetry . In this paper, we treat the ferromagnetic states in the trapped and finite fermion system.

In the next section of this paper, we formulate a set of equations for the two-component fermi gas at $`T=0`$ and the stability condition of its solutions in the Thomas-Fermi (TF) approximations. In Section III, solutions of the TF-equations are analyzed algebraically, and a critical condition for the collective ferromagnetic states is obtained. In Section IV, we show the density distributions of the two-component fermi gas and discuss paramagnetic-ferromagnetic transitions in it. In Section V, we summarize the results and discuss the experimental conditions to obtain the ferromagnetic states.

## II Thomas-Fermi equations for Two-component Fermi gas

We consider a $`T=0`$ system of two-component Fermi gas trapped in an isotropic harmonic oscillator potential; densities of spin up/down components are denoted by $`\rho _1(r)`$ and $`\rho _2(r)`$. To describe the ground-state behaviors of the system, we use the Thomas-Fermi approximation , where the total energy of the system is a functional of the densities:

$$E=d^3r\left[\underset{\sigma =1,2}{}\left\{\frac{\mathrm{}^2}{2m}\frac{3}{5}(6\pi ^2)^{\frac{2}{3}}\rho _\sigma ^{\frac{5}{3}}+\frac{1}{2}m\omega ^2r^2\rho _\sigma \right\}+g\rho _1\rho _2\right].$$
(1)
The $`m`$ and $`\omega `$ in (1) are the fermion mass and the oscillator frequency of the trapping potential. The last term in Eq. (1) corresponds to the interaction energy between different components of fermion, and the strength of the coupling constant $`g`$ is given by $`g=4\pi \mathrm{}^2a/m`$ where $`a`$ is the $`s`$-wave scattering length. The interactions between the same components are neglected; the elastic $`s`$-wave scattering is absent because of the Pauli blocking effects and the $`p`$-wave scattering is suppressed below $`100`$$`\mu `$K. In the present paper, we discuss a system of repulsive interaction, so that the parameter $`g`$ should be positive ($`g>0`$).

As we show later, the collective ferromagnetic states of two-component fermi gas show up in the case of large particle number ($`10^610^{13}`$), which validates the use of the Thomas-Fermi approximation. Also the validity of the approximation can be estimated from the smoothness of the mean-field potential: $`V_{\mathrm{eff}}=\frac{1}{2}m\omega ^2r^2+g\rho _{1,2}`$. As a parameter that represent its smoothness, we can take a local de Broglie wave length $`\lambda (r)=\mathrm{}/p(r)`$, where $`p(r)`$ is a TF local momentum defined by $`p(r)=\sqrt{2m(ϵ_FV_{\mathrm{eff}})}`$ ($`ϵ_F`$ : Fermi energy). As presented in , a validity condition with $`\lambda (r)`$ is given by $`f(r)|\frac{d\lambda }{dr}|1`$. Evaluating $`f(r)`$ with the parameters given in the last section (for 40K), we obtain $`f(r)10^3`$ except the classical turning points. It also supports the validity of the TF approximations in the present case.

To simplify Eq. (1), we introduce the scaled dimensionless variables:

$$n_\sigma =\frac{128}{9\pi }\rho _\sigma a^3,x=\frac{4}{3\pi }\frac{ar}{\xi ^2},\stackrel{~}{E}=\frac{2^{18}}{3^7\pi ^6}\left(\frac{a}{\xi }\right)^8\frac{E}{\mathrm{}\omega },$$
(2)
where $`\xi =\sqrt{\mathrm{}/m\omega }`$ is the oscillator length. Using these variables, Eq. (1) becomes

$$\stackrel{~}{E}=d^3x\left[\underset{\sigma =1,2}{}\left(\frac{3}{5}n_\sigma ^{\frac{5}{3}}+x^2n_\sigma \right)+n_1n_2\right].$$
(3)
The Thomas-Fermi equations for the densities $`n_{1,2}`$ are derived from the variations of the total Energy $`\stackrel{~}{E}`$ on $`n_{1,2}`$ with a constraint on the total particle number $`\stackrel{~}{N}`$: $`\frac{\delta }{\delta n_\sigma }(\stackrel{~}{E}\lambda \stackrel{~}{N})=0`$, where $`\stackrel{~}{N}`$ is the scaled total particle number defined by

$$\stackrel{~}{N}=\stackrel{~}{N}_1+\stackrel{~}{N}_2=\underset{\sigma }{}d^3xn_\sigma =\frac{2^{13}}{3^5\pi ^4}\left(\frac{a}{\xi }\right)^6N0.346\left(\frac{a}{\xi }\right)^6N.$$
(4)
The Lagrange multiplier $`\lambda `$ in the variational equation is for the fermion-number constraint, and related with the scaled chemical potential $`\stackrel{~}{\mu }`$ through the relation $`\stackrel{~}{\mu }N=\lambda \stackrel{~}{N}`$; using Eq. (4), we obtain

$$\stackrel{~}{\mu }0.346\left(\frac{a}{\xi }\right)^6\lambda .$$
(5)
It should be noted that, in Eq. (3), parameters $`(m,\omega ,g)`$ has been scaled out and no parameters are included except $`\lambda `$. The Lagrange multiplier $`\lambda `$ is determined by the total fermion number $`\stackrel{~}{N}`$, so that $`\stackrel{~}{N}`$ is the only parameter that determine the ground-state properties of the system.

Using Eqs. (3) and (4) for the variational equation, we obtain the TF equations:

$$n_1^{\frac{2}{3}}+n_2=\lambda x^2M(x),n_2^{\frac{2}{3}}+n_1=M(x).$$
(6)
The stability condition for solutions of Eq. (6) can be derived from the second-order variations of the energy functional:

$$\left|\begin{array}{cc}\frac{\delta ^2\stackrel{~}{E}}{\delta n_1^2}& \frac{\delta ^2\stackrel{~}{E}}{\delta n_1\delta n_2}\\ \frac{\delta ^2\stackrel{~}{E}}{\delta n_2\delta n_1}& \frac{\delta ^2\stackrel{~}{E}}{\delta n_2^2}\end{array}\right|0.$$
(7)
Using Eq. (3), we obtain the stability condition for the present case:

$$n_1n_2\left(\frac{2}{3}\right)^6.$$
(8)
## III Solutions of Thomas-Fermi Equations

In this section, we show solutions of coupled TF equations (6) in algebraic form and discuss their stability based on the stability condition (8).

Let’s introduce variables $`s`$ and $`t`$ as $`n_1=s^3`$ and $`n_2=t^3`$, then Eq. (6) becomes

$$s^3+t^2=M,t^3+s^2=M.$$
(9)
Making sum and difference of them, we obtain two equations equivalent with Eq. (9):

$$s^3+t^3+s^2+t^2=2M,s^3t^3(s^2t^2)=(st)(s^2+st+t^2st)=0.$$
(10)
The factorized form of the second equation gives two alternatives: 1) $`s=t`$ or 2) $`s^2+st+t^2st=0`$.

In the case 1), $`s=t`$, the first equation in (10) becomes $`s^3+s^2=M`$, which can be solved algebraically with the Caldano’s formula. It includes only one positive root when $`M0`$:

$$s=\frac{f(M)}{6}+\frac{2}{3f(M)}\frac{1}{3},f(M)=\left[8+108M+12\sqrt{81M^212M}\right]^{1/3}.$$
(11)
For this solution, the stability condition (8) gives $`s2/3`$, which leads to the constraint for $`M`$:

$$M=s^3+s^2\left(\frac{2}{3}\right)^2+\left(\frac{2}{3}\right)^3=\frac{20}{27}.$$
(12)
Thus, the stable symmetric solutions exist when $`0M20/27`$.

Next, we take the case 2) : $`s^2+st+t^2st=0`$. Now, this and the another equation in (10) are symmetric under the exchange between $`s`$ and $`t`$, so that they can be represented by elementary symmetric polynomials, $`As+t`$ and $`Bst`$:

$$A^3A^2A+M=0,A^2AB=0.$$
(13)
The first equation has a real positive solution:

$$A=\frac{g(M)}{6}+\frac{8}{3g(M)}+\frac{1}{3},g(M)=\left[108M+44+12\sqrt{81M^266M15}\right]^{1/3}.$$
(14)
Substituting it in (13), we obtain the solution for $`B`$:

$$B=\frac{[g(M)]^2}{36}\frac{g(M)}{18}+\frac{4}{9}\frac{8}{9g(M)}+\frac{64}{9[g(M)]^2}.$$
(15)
The $`s`$ and $`t`$ can be recovered as two solutions of the equation: $`x^2Ax+B=0`$. These solutions are generally asymmetric ($`st`$).

We can check the stability of the asymmetric solutions with Eq. (8), which gives a constraint for $`B`$: $`B=st=(n_1n_1)^{1/3}4/9`$. Then, from the second equation in (13), we obtain that for $`A`$: $`1A4/3`$. Differentiating the first equation in (13) by $`A`$, we find that $`M`$ is a monotonically decreasing function of $`A`$ within the interval $`1A4/3`$. Combining these results, we obtain the stability range of $`M`$ for the asymmetric solutions: $`20/27<M1`$.

In summary, the stable solutions of Eq. (10) are

$$\begin{array}{ccc}\hfill 1.& 0M\frac{20}{27}\hfill & \text{symmetric},\hfill \\ \hfill 2.& \frac{20}{27}<M1\hfill & \text{asymmetric},\hfill \\ \hfill 3.& 1<M\hfill & \text{(no stable solutions)}.\hfill \end{array}$$
(16)
In case that $`1<M`$, Eq. (10) have no stable solutions. In the TF variational equation $`\frac{\delta }{\delta n_\sigma }(\stackrel{~}{E}\lambda \stackrel{~}{N})=0`$, we assumed the chemical equilibrium between fermion 1 and 2, and put their chemical potentials (Lagrange multipliers) equal: $`\lambda =\lambda _1=\lambda _2`$. Accordingly, in $`1<M`$, we should say that the system has no stable solutions in “equilibrium”. Thus, for $`1<M`$, we should take the nonequilibrium states where all fermions occupy one component (complete asymmetry). If we assume $`s=0`$, $`t`$ is obtained by solving the equation:

$$t^2=M,s=0.$$
(17)
## IV Density Profiles of Two-component Fermi Gas

Using the results in the previous section, we can calculate the density profiles of the two-component fermi gas for any values of $`\lambda `$. Corresponding to the classification by $`M=\lambda x^2`$ in (16), we should divide $`\lambda `$ into three regions:

$$\text{(i) }\mathrm{\hspace{0.17em}0}\lambda \frac{20}{27},\text{(ii) }\frac{20}{27}<\lambda 1,\text{(iii) }\mathrm{\hspace{0.17em}1}<\lambda ,$$
(18)
and discuss qualitative profiles of the density distributions $`n_{1,2}`$.

1. Paramagnetic ground states. In these cases, $`M(x)`$ satisfies $`M(x)=\lambda x^220/27`$ for any value of $`x`$. Thus, from (16), the density distributions are composed of the symmetric solution (11) in all spatial region. Consequently, the ground states are paramagnetic in the region (i): $`n_1(x)=n_2(x)`$. In Fig. 1(a), the density profiles are shown when $`\lambda =1/2`$. They monotonically decreases with the scaled radial distance $`x`$, and vanishes at the TF cut-off: $`x_{\mathrm{TF}}\sqrt{\lambda }=1/\sqrt{2}`$ in this case. These states occurs in the case of small fermion number.
2. Ferromagnetic ground states in equilibrium. In these cases, we obtain $`M(x)20/27`$ in the outside region ($`x\sqrt{\lambda 20/27}`$), but $`20/27<M(x)1`$ in the inside region ($`x<\sqrt{\lambda 20/27}`$). Correspondingly, the density distributions become symmetric in the outside region and asymmetric in the inside region, so that the ground states become ferromagnetic in the region (ii). Because the condition $`M(x)1`$ is satisfied, solutions are in equilibrium in all spatial regions, and densities are partially asymmetric in the inside region. In Fig. 1(b), the density profiles are shown when $`\lambda =4/5`$ for $`n_1`$ (solid line) and $`n_2`$ (dotted line). The border between symmetric and asymmetric regions is given by $`x_{\mathrm{AS}}\sqrt{\lambda 20/27}=\sqrt{8/135}`$ in this case. In the outside (symmetric) region, the both lines overlap and vanishes at $`x_{\mathrm{TF}}=2/\sqrt{5}`$.
3. Ferromagnetic ground states in nonequilibrium. In these cases, density profiles are also asymmetric in the inside region ($`x<x_{\mathrm{AS}}`$) as in the above region. However, in the most inside region ($`x<\sqrt{\lambda 1}`$), $`M(x)>1`$ is satisfied and, according to the condition 3 in (16), the density profiles become nonequilibrium and are given by complete asymmetric solutions in (17). In Fig. 1(c), we show the density profiles when $`\lambda =3/2`$ for $`n_1`$ (solid line) and $`n_2`$ (dotted line). In the most inside region ($`x<x_{\mathrm{EQ}}=\sqrt{\lambda 1}=1/\sqrt{2}`$), the density profiles are completely asymmetric ($`n_2=0`$), and, in $`x_{\mathrm{EQ}}x<x_{\mathrm{AS}}=\sqrt{41/54}`$, they are partially asymmetric. In the outside (symmetric) region ($`x>x_{\mathrm{AS}}`$), two lines overlap and vanishes at $`x=x_{\mathrm{TF}}=\sqrt{3/2}`$. Thus, the ground states are ferromagnetic and in nonequilibrium in the region (iii) which corresponds to the cases of large fermion number.

In Fig. 2, we show the dependence of $`\lambda `$ on the fermion number $`\stackrel{~}{N}`$, which is calculated by Eq. (4) using the fermion densities $`n_{1,2}(x)`$ obtained above; for the ground states (solid line) and the paramagnetic states (dotted line). From the above discussions, for $`\lambda 20/27`$, the ground states are paramagnetic, so that the both lines overlap. As can be read off in this figure, the critical value $`\lambda =20/27`$ corresponds to $`\stackrel{~}{N}_C=0.53`$, which is the critical fermion number for the transition between paramagnetic and ferromagnetic states.

In Fig. 3(a), the variations of the scaled total energies $`\stackrel{~}{E}`$ are shown against $`\stackrel{~}{N}`$, for the ground (solid line) and paramagnetic (dotted) states. The $`\stackrel{~}{E}`$ can be obtained by Eq. (3) as a function of $`\lambda `$ using the fermion densities $`n_{1,2}(x)`$; combined with the $`\stackrel{~}{N}`$-dependence of $`\lambda `$ (shown in Fig. 2), we can obtain its $`\stackrel{~}{N}`$-dependence. In $`\stackrel{~}{N}\stackrel{~}{N}_C=0.53`$, both lines overlap completely because the ground states become paramagnetic. In Fig. 3(b), we plot the energy difference between the ground and paramagnetic states. In this figure, we can find that, in $`\stackrel{~}{N}>\stackrel{~}{N}_C`$, the ground-state energy (solid line) shifts lower than that of the paramagnetic states (dotted line); it shows that the ferromagnetic ground states become more stable in this region.

As can be seen in Fig. 3(a) when $`\stackrel{~}{N}>0.53`$, the energy difference between ferromagnetic and paramagnetic states $`|\stackrel{~}{E}\stackrel{~}{E}_{\mathrm{para}}|`$ is very small in comparison with the total energy $`\stackrel{~}{E}`$: e.g. $`|\stackrel{~}{E}\stackrel{~}{E}_{\mathrm{para}}|/\stackrel{~}{E}0.01`$ at $`\stackrel{~}{N}=2.0`$. A large part of $`\stackrel{~}{E}`$ consist of the stacked kinetic energy due to the fermi degeneracy of fermions. Roughly speaking, its size can be estimated from the total energy of the noninteracting fermi gas ($`g=0`$) trapped in the same harmonic oscillator potential; $`\stackrel{~}{E}_{\text{non}}=\frac{3}{16}\pi ^2(\frac{4}{\pi ^2}\stackrel{~}{N})^{4/3}`$, which increases rapidly with increasing $`\stackrel{~}{N}`$. The $`\stackrel{~}{E}_{\text{non}}`$ is plotted also in Fig. 3(a) (dot-dashed line), the amounts of which are almost $`75\%`$ of $`\stackrel{~}{E}`$.

However, to evaluate the scale of the energy difference, we should compare it with an one-particle excitation energy at the Fermi surface, which can be estimated from the scaled chemical potential $`\stackrel{~}{\mu }`$ defined in (5). In case of 40K with the harmonic oscillator frequency $`\omega =1000\mathrm{Hz}`$ (for other parameters, see the next section), Eq. (5) becomes $`\stackrel{~}{\mu }10^{13}\lambda `$. When $`\stackrel{~}{N}2`$ ($`\lambda 1`$ from Fig. 2), the ratio $`\mathrm{\Delta }\stackrel{~}{E}/\stackrel{~}{\mu }`$ becomes $`10^{13}`$. Thus, we should say that the energy difference between ferromagnetic and paramagnetic states are fairly large.

In Fig. 4, we show the fermion number asymmetry $`(\stackrel{~}{N}_1\stackrel{~}{N}_2)/\stackrel{~}{N}=(N_1N_2)/(N_1+N_2)`$ against the total fermion number $`\stackrel{~}{N}`$.

## V Summary and Discussions

We discussed the possibility of transition to ferromagnetic states in the two-component fermi gas using the Thomas-Fermi approximation from theoretical points of view. Based on the results that we obtained, let’s discuss experimental conditions and also difficulties to observe ferromagnetic ground states in the trapped atomic gas. We hope that these difficulties are overcome in future developments in experimental technics.

As shown in the previous section, the ferromagnetic ground states become stable when $`\stackrel{~}{N}0.53`$; using Eq. (4), the unscaled critical number $`N_C`$ becomes

$$N_C\frac{0.53}{0.346}\left(\frac{\xi }{a}\right)^6=1.5\left(\frac{\xi }{a}\right)^6.$$
(19)
As an example, we take the 40K atoms (mass $`m=0.649\times 10^{25}\mathrm{kg}`$) trapped in the harmonic oscillator potential with $`\omega =1000\mathrm{Hz}`$. For the scattering length, we take the value $`a=169a_B`$ ($`a_B`$: Bohr radius) given in . Using these parameters, we obtain $`N_C10^{13}`$. In recent experiments, the trapped Fermi-degenerate gas has been performed up to $`10^6`$ atoms, so that the larger trapping potential are necessary for realization of the ferromagnetic ground state than currently used one. In addition, because of the high central density ($`10^{17}\mathrm{cm}^3`$) for $`10^{13}`$ atoms, the inelastic/multi-body scattering processes in them becomes important, which might destroy the trapped atoms before they reach the required density.

There can be several possibilities for the reduction of $`N_C`$. For example, if the scattering length can be increased by the Feshbach resonance for 40K, which has been observed experimentally , the value of $`N_C`$ decreases and the ferromagnetic ground states can be obtained in small fermion number: simple estimation gives, $`a=820a_B`$ for $`N_C10^9`$ and $`a=2600a_B`$ for $`N_C10^6`$. However, in current experiments, the tuning into Feshbach resonances is done by applying the magnetic field, which should make the energy difference between the up and down states and makes the ferromagnetic transition into a crossover in the spin asymmetry. The ways to tune Feshbach resonances by non-magnetic external forces (e.g. electric fields) are preferred for the present purpose.

The use of heavier elements, e.g. Sr or Yb, is also effective for the ferromagnetic states. We hope that the combination of these methods may lead to the experimental achievements.

We also comment on the process to perform the ferromagnetic states. There exist two possibilities:

1. The experiment starts with the magnetic field in some direction which makes the spin asymmetry (e.g. $`N_1>N_2`$). Then, the magnetic field is switched off adiabatically in the cooling process. When the number of the remaining atoms is enough large, it shows the ferromagnetic states.
2. The experiment starts with the symmetric trap ($`N_1=N_2`$), and, after some relaxation time elapses, the atoms release their spin angular momenta and become the ferromagnetic state.

The case a) is similar with a standard processe for observing the phase transition in the ferromagnetic materials. In case b), the spin relaxation time is considered to be the same order with that of clusterization, so that it might be difficult to observe the ferromagnetic transition within the lifetime of the atomic gas.

Finally, we comment on the spacially phase-separated states in the trapped fermionic gas in the case of the large particle number and interaction strength . They correspond to the phase separation in the uniform system (two-phase coexistent region), discussed in . The naive TF calculations give smaller energy for the ferromagnetic states, but the energy difference is very small. The competition/coexistence of these states should be an interesting problem in future.

We are very grateful to T. Maruyama, T. Suzuki and T. Miyakwa for fruitful discussions. Special thanks are also for T. Tatsumi for introducing us the physics of collective ferromagnetism.


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# Appendix : computations for 𝔰𝔩(3)

## 1. Notations

We keep the notations of the article, with $`G=\mathrm{SL}(3,\mathrm{𝕜})`$, and denote $`\alpha _1,\alpha _2`$ the simple roots of $`G`$ and $`\omega _1,\omega _2`$ the fundamental weights. Let $`s_j`$ be the reflection $`s_{\alpha _j}W`$. We denote by $`\stackrel{𝑖}{}\stackrel{~}{𝒩}\stackrel{𝑝}{}`$ the inclusion of the zero section and the natural projection. There are two natural maps $`\pi _j:^2`$ mapping a flag $`0V_1V_2\mathrm{𝕜}^3`$ to $`V_j,j=1,2`$. For $`n`$ we have isomorphisms: $`\pi _i^{}𝒪_^2(n)𝒪_{}(n\omega _i),i=1,2`$, and $`\mathrm{Fr}_{}^{}𝒪_{^{(1)}}(\lambda )𝒪_{}(p\lambda )`$ for $`\lambda \mathrm{\Lambda }`$. We will study irreducible $`G`$-modules $`L(\lambda )`$ of highest weight $`\lambda `$ for reduced dominant weights $`\lambda `$ in $`W_{\mathrm{aff}}^{}0`$. Recall the exact sequence

$`()0\mathrm{\Omega }_^2^1𝒪_^2(1)^3𝒪_^20.`$

For simplicity, in what follows we will omit the Frobenius twist <sup>(1)</sup> (except in the proof of theorem 2.1, where we have to be more careful); it should appear on (almost) every variety we consider.

## 2. Irreducible modules

###### Theorem 2.1.

The irreducible $`U_{\widehat{0}}^0`$-modules and the corresponding coherent sheaves are :

| $`L(0)=\mathrm{𝕜}`$ | $`i_{}𝒪_{}`$ | $`L((p2)\omega _1+\omega _2)`$ | $`i_{}\pi _1^{}(\mathrm{\Omega }_^2^1(1))[1]`$ |
| --- | --- | --- | --- |
| $`L((p3)\omega _2)`$ | $`i_{}𝒪_{}(\omega _1)[2]`$ | $`L(\omega _1+(p2)\omega _2)`$ | $`i_{}\pi _2^{}(\mathrm{\Omega }_^2^1(1))[1]`$ |
| $`L((p3)\omega _1)`$ | $`i_{}𝒪_{}(\omega _2)[2]`$ | $`L((p2)\rho )`$ | $``$ |

where $``$ is the cone of the only (up to a constant) nonzero morphism $`i_{}𝒪_{}i_{}𝒪_{}(\rho )[3]`$.

*Proof.* We have $`\mathrm{{\rm Y}}(i_{}𝒪_{})=R\mathrm{\Gamma }(,𝒪_{})=\mathrm{𝕜}`$. Also, $`\mathrm{{\rm Y}}(i_{}𝒪_{}(\omega _j))=R\mathrm{\Gamma }(𝒪_^2(p))`$, which gives the claim for $`L((p3)\omega _j)`$, $`j=1,2`$.

Similarly $`\mathrm{{\rm Y}}(i_{}\pi _1^{}(\mathrm{\Omega }_{(^2)^{(1)}}^1(1))[1])=R\mathrm{\Gamma }(,\mathrm{Fr}_{}^{}\pi _1^{}(\mathrm{\Omega }_{(^2)^{(1)}}^1(1)))[1]`$. Using the exact sequence $`()`$ we obtain a distinguished triangle $`R\mathrm{\Gamma }(,𝒪_{})^3R\mathrm{\Gamma }(,𝒪_{}(p\omega _1))\mathrm{{\rm Y}}(i_{}\pi _1^{}(\mathrm{\Omega }_{(^2)^{(1)}}^1(1))[1]).`$ Here the second arrow is the inclusion of $`G`$-modules $`L(\omega _1)^{(1)}H^0(p\omega _1)`$. Hence $`\mathrm{{\rm Y}}(i_{}\pi _1^{}(\mathrm{\Omega }_{(^2)^{(1)}}^1(1))[1])L((p2)\omega _1+\omega _2).`$ The claim for $`L(\omega _1+(p2)\omega _2)`$ follows by applying the outer automorphism of $`𝔰𝔩(3)`$.

Finally, the last irreducible module $`L((p2)\rho )`$ is a quotient of the Weyl module $`[H^0((p2)\rho )]^{}`$, moreover, we have a short exact sequence $`0\mathrm{𝕜}[H^0((p2)\rho )]^{}L((p2)\rho )0.`$ Applying $`\mathrm{{\rm Y}}^1`$, we get distinguished triangle $`i_{}𝒪_{}i_{}𝒪_{}(\rho )[3]`$, where we used that $`\mathrm{{\rm Y}}(i_{}𝒪_{^{(1)}}(\rho ))=R\mathrm{\Gamma }(,𝒪_{}(p\rho ))=[H^0((p2)\rho )]^{}[3]`$ by Serre duality. Since $`\mathrm{Hom}(\mathrm{𝕜},[H^0((p2)\rho )]^{})`$ is one dimensional, we see that the first arrow in this triangle is the unique (up to a constant) map between the two objects. ∎

*Remark.* We have just shown, using equivalence $`\mathrm{{\rm Y}}`$, that $`\mathrm{Ext}_{\stackrel{~}{𝒩}}^3(i_{}𝒪_{},i_{}𝒪_{}(\rho ))`$ is one dimensional. One can compute this Ext group more directly: using the Koszul resolution of $`𝒪_{}`$ over $`\mathrm{S}(𝒯_{})`$ one can identify it with $`H^3(\rho )H^2(\mathrm{\Omega }_{}^1(\rho ))H^1(\mathrm{\Omega }_{}^2(\rho ))H^0(\mathrm{\Omega }_{}^3(\rho ))`$. One can show that $`H^3(\rho )`$, $`H^0(\mathrm{\Omega }_{}^3(\rho ))`$ and $`H^1(\mathrm{\Omega }_{}^2(\rho ))`$ are $`0`$, while $`H^2(\mathrm{\Omega }_{}^1(\rho ))\mathrm{𝕜}`$ (by Serre duality the last claim is equivalent to $`H^1(𝒯_{}(\rho ))\mathrm{𝕜}`$, which is checked below).

## 3. Projective covers

###### Theorem 3.1.

The coherent sheaves corresponding to the projective covers of the irreducible modules are :

| $`i_{}𝒪_{}`$ | $`𝒫`$ | $`i_{}\pi _1^{}(\mathrm{\Omega }_^2^1(1))[1]`$ | $`𝒪_{\stackrel{~}{𝒩}}(\omega _1)`$ |
| --- | --- | --- | --- |
| $`i_{}𝒪_{}(\omega _1)[2]`$ | $`p^{}((\pi _2^{}\mathrm{\Omega }_^2^1)(\omega _1+2\omega _2))`$ | $`i_{}\pi _2^{}(\mathrm{\Omega }_^2^1(1))[1]`$ | $`𝒪_{\stackrel{~}{𝒩}}(\omega _2)`$ |
| $`i_{}𝒪_{}(\omega _2)[2]`$ | $`p^{}((\pi _1^{}\mathrm{\Omega }_^2^1)(2\omega _1+\omega _2))`$ | $``$ | $`𝒪_{\stackrel{~}{𝒩}}(\rho )`$ |

where $`𝒫`$ is the nontrivial extension of $`𝒪_{\stackrel{~}{𝒩}}(\rho )`$ by $`𝒪_{\stackrel{~}{𝒩}}`$ given by a non-zero element in the one dimensional space $`H^1(𝒯_{}(\rho ))H^1(𝒪_{\stackrel{~}{𝒩}}(\rho ))`$.

*Remark.* In fact, the sheaves corresponding to the projective covers are vector bundles on the formal completion of $`\stackrel{~}{𝒩}`$ at $``$. The objects displayed in the above table are vector bundles on $`\stackrel{~}{𝒩}`$. The former are obtained from the latter by pull-back to the formal completion.

*Proof.* We only have to check that for each $`𝒫_i`$ in the list and each irreducible $`_j`$, we have $`\mathrm{Ext}_{\stackrel{~}{𝒩}}^{}(𝒫_i,_j)=\mathrm{𝕜}^{\delta _{ij}}`$. Let us begin with $`𝒪_{\stackrel{~}{𝒩}}(\rho )`$. We have $`\mathrm{Ext}_{\stackrel{~}{𝒩}}^{}(𝒪_{\stackrel{~}{𝒩}}(\rho ),i_{}𝒪_{})\mathrm{Ext}_{}^{}(𝒪_{}(\rho ),𝒪_{})H^{}(,𝒪_{}(\rho ))=0`$ by adjunction. Similarly for $`i_{}𝒪_{}(\omega _j)[2]`$ ($`j=1,2`$). The sequence $`()`$ gives $`\mathrm{Ext}_{\stackrel{~}{𝒩}}^{}(𝒪_{\stackrel{~}{𝒩}}(\rho ),i_{}\pi _j^{}(\mathrm{\Omega }_^2^1(1))[1])=\mathrm{Ext}_{}^{}(𝒪_{}(\rho ),\pi _j^{}(\mathrm{\Omega }_^2^1(1))[1])=0`$ ($`j=1,2`$). Using the distinguished triangle from the definition of $``$ we get $`\mathrm{Ext}_{\stackrel{~}{𝒩}}^{}(𝒪_{\stackrel{~}{𝒩}}(\rho ),)=\mathrm{𝕜}`$. The cases of $`𝒪_{\stackrel{~}{𝒩}}(\omega _j)`$ ($`j=1,2`$) are similar.

Now let us consider $`p^{}((\pi _1^{}\mathrm{\Omega }_^2^1)(2\omega _1+\omega _2))`$. The exact sequence $`()`$ and Borel-Weil-Bott Theorem \[Ja\] give the result for the first 5 irreducible modules. For $``$, we have $`\mathrm{Ext}_{}^{}((\pi _1^{}\mathrm{\Omega }_^2^1)(2\omega _1+\omega _2),𝒪_{})=0`$, and in computing $`\mathrm{Ext}_{}^{}((\pi _1^{}\mathrm{\Omega }_^2^1)(2\omega _1+\omega _2),𝒪_{}(\rho )[3])`$, two non-zero modules appear in degree $`0`$ : $`[H^3(2\rho )]^3`$ and $`H^0(\omega _1)`$. The map between these two modules is an isomorphism as in the proof of Theorem 2.1, hence $`\mathrm{Ext}_{\stackrel{~}{𝒩}}^{}(p^{}((\pi _1^{}\mathrm{\Omega }_^2^1)(2\omega _1+\omega _2)),)=0`$.

We claim that $`H^1(𝒯_{}(\rho ))\mathrm{𝕜}`$, this follows by the Borel-Weil-Bott Theorem from the exact sequence $`0𝒪_{}(\alpha _1)𝒯_{}\pi _2^{}(𝒯_^2)0`$, and vanishing of $`R\mathrm{\Gamma }(\pi _2^{}(𝒯_^2)(\rho ))`$ (see, e.g., \[D\]). Thus we have the line $`H^1(𝒯_{}(\rho ))H^1(\mathrm{S}(𝒯_{})(\rho ))=\mathrm{Ext}_{\stackrel{~}{𝒩}}^1(𝒪_{\stackrel{~}{𝒩}}(\rho ),𝒪_{\stackrel{~}{𝒩}})`$, which defines a triangle $`𝒪_{\stackrel{~}{𝒩}}𝒫𝒪_{\stackrel{~}{𝒩}}(\rho )`$. Standard calculations give the result for $`𝒫`$ and the first three irreducible modules. The triangle defining $`𝒫`$ gives $`\mathrm{Ext}_{\stackrel{~}{𝒩}}^{}(𝒫,i_{}\pi _1^{}(\mathrm{\Omega }_^2^1(1))[1])=H^{}(\pi _1^{}(\mathrm{\Omega }_^2^1(1)))[1].`$ Using $`()`$, we have an exact sequence $`0H^0(\pi _1^{}(\mathrm{\Omega }_^2^1(1)))\mathrm{𝕜}^3H^0(\omega _1)H^1(\pi _1^{}(\mathrm{\Omega }_^2^1(1)))0`$ with invertible middle arrow (the other cohomology modules vanish).

Finally, let us show that $`\mathrm{Ext}_{\stackrel{~}{𝒩}}^{}(𝒫,)=0`$. We have $`R\mathrm{Hom}_{\stackrel{~}{𝒩}}(𝒫,i_{}𝒪_{})R\mathrm{\Gamma }(𝒪_{})\mathrm{𝕜},R\mathrm{Hom}_{\stackrel{~}{𝒩}}(𝒫,i_{}𝒪_{}(\rho )[3])R\mathrm{\Gamma }(𝒪_{}(2\rho )[3])\mathrm{𝕜}`$, thus we only need to check that for nonzero morphisms $`b:i_{}𝒪_{}i_{}𝒪_{}(\rho )[3]`$, $`\varphi :𝒫i_{}𝒪_{}`$ we have $`b\varphi 0`$. It is clear from Remark after Theorem 2.1 that $`b=i_{}(\beta )\delta `$, where $`\delta :i_{}𝒪_{}i_{}𝒯_{}[1]`$ is the class of the extension $`0i_{}𝒯_{}𝒪_{\stackrel{~}{𝒩}}/𝒥_{}^2i_{}𝒪_{}0`$, and $`\beta :𝒯_{}[1]𝒪_{}(\rho )[3]`$ is a non-zero morphism; here $`𝒥_{}`$ is the ideal sheaf on the zero section in $`\stackrel{~}{𝒩}`$.

We claim that $`\delta \varphi =i_{}(\gamma )\psi `$, where $`\psi :𝒫i_{}𝒪_{}(\rho )`$ and $`\gamma :𝒪_{}(\rho )𝒯_{}[1]`$ are nonzero morphisms. This follows from the definition of $`𝒫`$, which implies that $`𝒫`$ has a quotient, which is an extension of $`i_{}𝒪_{}i_{}𝒪_{}(\rho )`$ by $`i_{}𝒯_{}`$, such that the corresponding class in $`\mathrm{Ext}^1(i_{}𝒪_{},i_{}(𝒯_{}))`$ equals $`\delta `$, while the corresponding class in $`\mathrm{Ext}^1(i_{}𝒪_{}(\rho ),i_{}(𝒯_{}))`$ is non-trivial and is an image under $`i_{}`$ of an extension of coherent sheaves on $``$.

It remains to show that the composition $`i_{}\beta i_{}\gamma \psi `$ is nonzero. The composition $`\beta \gamma \mathrm{Ext}^3(𝒪_{}(\rho ),𝒪_{}(\rho ))=H^3(,𝒪(2\rho ))=\mathrm{𝕜}`$ is nonzero, because it coincides with the Serre duality pairing of nonzero elements $`\beta `$, $`\gamma `$ in the two dual one-dimensional spaces $`H^1(𝒯_{}(\rho ))`$, $`H^2(𝒯_{}^{}(\rho ))`$. Consequently, the composition $`i_{}(\beta \gamma )\psi `$ is also nonzero, since under the isomorphism $`\mathrm{Hom}(𝒫,i_{}𝒪_{}(\rho )[3])\mathrm{Hom}(i^{}𝒫,𝒪_{}(\rho )[3])\mathrm{Hom}(𝒪_{}𝒪_{}(\rho ),𝒪_{}(\rho )[3])`$ it corresponds to the composition of $`\beta \gamma `$ and projection to the second summand. ∎


text:
# First results from the Very Small Array – I. Observational methods

## 1 INTRODUCTION

Sensitive measurements of the cosmic microwave background (CMB) radiation are increasingly important in cosmology and astrophysics. Observations of both the primary imprints on the CMB originating at the surface of last scattering and secondary imprints such as the Sunyaev-Zel’dovich effect contain a wealth of information, if they can be made with sufficient sensitivity and freedom from systematic errors. We have constructed a telescope, the Very Small Array (VSA), for measuring intensity structures in the CMB on degree and sub-degree angular scales. The telescope itself is described in detail in Rusholme et al. (in prep.). The present paper discusses the observational methods underlying VSA observations, and the procedures used to eliminate systematic errors from the data (such as contaminating emission from the Sun). In three accompanying papers we then present results from the first year’s observations with the VSA. Paper II (Taylor et al., 2002) describes the first season’s observations and issues of foreground removal; Paper III (Scott et al., 2002) presents the power spectrum results and analysis, while Paper IV (Rubiño-Martin et al., 2002) derives cosmological parameters from the VSA results and other data.

Many different experimental approaches have been used to measure features in the CMB, mostly using switched- or swept-beam systems with total power detectors. Such systems can be made with very high sensitivity, particularly when using broad-band bolometric detectors, and progress in the field has mostly been due to improved techniques for suppressing unwanted signals such as atmospheric emission and differential emission from the telescope optics. An alternative approach, which we have adopted, is to use interferometers. These provide excellent rejection of systematics, since only signals entering both antennas with the correct path and phase modulation are detected while signals such as ground radiation and atmospheric emission are strongly suppressed (eg Church (1995)). For similar reasons they are relatively insensitive to receiver gain fluctuations. Interferometric systems also offer the opportunity to target a specific range of angular scales on the sky, determined by the spacing and the size of the elements of the array, and are well-suited to measuring the power spectrum of the CMB since they directly sample the Fourier modes on the sky which can then be converted to a power spectrum. Their main disadvantages are the restricted bandwidth compared to bolometers, due to the need for coherent receivers, and the relative complexity and expense of the correlator. We have previously demonstrated the success of the interferometric approach with the detection of CMB fluctuations with the Cosmic Anisotropy Telescope (CAT) from a sea-level site (Scott et al. (1996), Baker et al. (1999)); the VSA is a direct descendant of CAT.

## 2 THE INSTRUMENT

In this section we briefly describe the VSA and its capabilities, and compare it with other current CMB telescopes.

### 2.1 VSA main array

The VSA is a 14-element heterodyne interferometer array, tuneable between 26 and 36 GHz with a 1.5 GHz bandwidth and a system temperature of approximately $`30\mathrm{K}`$, sited at 2400 m altitude at the Teide Observatory in Tenerife. Each receiving element consists of a corrugated horn-reflector antenna (CHRA) feeding a cooled HEMT amplifier, measuring one linear polarisation. The CHRA (Yassin et al., 1993) consists of a conical corrugated horn feeding a section of a paraboloidal mirror at $`90^{}`$ to the horn axis. This arrangement gives a compact antenna with an unblocked aperture, and hence low sidelobes. The mirror can be rotated about the axis of the feedhorn, allowing tracking in one dimension. The receivers are mounted on a tilting table hinged along its northern edge, providing tracking in a second dimension (see Figure 1). In order to achieve close packing of the antenna apertures, the receivers are mounted at an angle of $`35^{}`$ to the table; the elevation range of the table is $`0^{}`$$`70^{}`$ and thus gives a range of zenith angle of $`\pm 35^{}`$ in the north-south direction, with the rotating mirrors providing approximately $`\pm 45^{}`$ in the other diection. The array is surrounded by an aluminium ground screen to limit interference and groundspill; the internal sides are sloped to direct rays from the table into the sky.

The antennas used for the observations reported here and in papers II–IV have illuminated apertures of 143 mm diameter, giving a primary (envelope) beam of $`4.6^{}`$ FWHM at 34 GHz and are designed for use in a “compact array”, for observations up to a maximum spherical harmonic multipole of about $`\mathrm{}=900`$. For subsequent observations at higher $`\mathrm{}`$ the antennas have been modified by increasing the length of the horn and fitting a larger mirror, giving an aperture of 322 mm and a beam of $`2.0^{}`$ FWHM; observations are currently underway with this “extended array”.

The signals are downconverted at the antennas to a first IF frequency centred at 9 GHz, and again at a point just outside the enclosure to a centre frequency of 1 GHz. This double downconversion allows the RF band to be tuned by changing the first local oscillator frequency without the need for high-Q tunable image filters. The first LO is also phase-switched with orthogonal switching functions at each antenna to allow subsequent phase-sensitive detection in the correlator. The second downconversion uses LOs in quadrature to produce real and imaginary channels for each antenna.

The second IF signals are carried on cables inside a screened enclosure within the control building. To compensate for the changing path to the source as the antennas track, lengths of delay line are switched into each IF channel, eight units providing up to 1.8 m delay in steps of 7 mm. After further gain, equalisation, and automatic gain control, the signals are split with a cascade of power splitters and fed into the corrrelators. Each real or imaginary correlation is done on a separate board, where the product of the inputs is formed and detected synchronously with the first LO switching functions. The data are integrated in an analogue integrator for 1 s before being sampled and read out into the control computer. The synchronous detection circuit also includes a switch which reduces the correlator gain by a factor of about 20, increasing the dynamic range of the correlator for observation of very bright calibrators such as the Moon.

### 2.2 Source subtraction baseline

The most important foreground contaminant for CMB observations at these angular scales and frequency is radio sources. The effect of sources on the power spectrum increases as $`\mathrm{}^2`$, but even at the lower $`\mathrm{}`$’s sampled by the compact array sources are significant (Taylor et al., 2001). Ideally one would survey the CMB fields at the same frequency as the CMB observations with sufficiently high sensitivity and resolution to detect all the sources that would contaminate the power spectrum. This would require a telescope rather more expensive than the VSA itself. Instead, we adopt a two-part strategy based on existing facilities; VSA fields are surveyed at 15 GHz with the Ryle Telescope (RT) (Waldram et al., 2002), and then each of the sources found is monitored at 34 GHz by a source subtractor interferometer located next to the VSA. More details of the source subtraction procedure are given in Paper II.

The source subtraction interferometer consists of two 3.7-m diameter dishes fitted with the same receivers as the main array, and equipped with identical IF and correlator. The dishes are mounted such that they track with the same rotation of parallactic angle as the main array, so that polarized sources will be observed in the same orientation with respect to the polarization of the feeds. The antennas are housed in separate ground screens identical to the main array ground screen, to limit ground pickup and to provide shielding from the wind. The baseline is 9 m, giving a resolution of 4 arcmin in a 9 arcmin field, which will not resolve any of the sources we observe, while completely resolving out the CMB.

### 2.3 The site

The VSA is located at the Teide Observatory, Tenerife at an altitude of 2400 m. The observatory is well established and, although on-site support is always available, we are able to control both the telescope and observations remotely. The site provides excellent observing conditions and has been well-tested for atmospheric seeing over a 15-year period. The inversion layer lies below the observatory for 75 per cent of the year; the twice-daily meteorological balloon flights show that the precipitable water vapour is as low as 2 mm for 30 per cent of the launches. For observations in the region $`2636`$ GHz, the typical transparency is 95 per cent. Correlated signals due to atmospheric emission decrease with higher angular resolution. For example, at 33 GHz, the $`8^{}`$ Tenerife beam-switch experiment (for example, Davies et al. (1996)) was affected by water vapour fluctuations for 80 per cent of the time while the Jodrell Bank-IAC 33 GHz interferometer (Melhuish et al., 1999) was affected for 20 per cent of the time at $`2^{}`$ resolution ($`\mathrm{}110`$) and $`10`$ percent at $`1^{}`$ resolution ($`\mathrm{}210`$). On the VSA baselines ($`\mathrm{}150900`$) we expect even less loss of data due to atmospheric effects. In fact, during our first season of observations (September 2000 – September 2001), the site proved to have exceptional conditions; only 5 percent of the data were rejected due to weather.

### 2.4 Comparison with other CMB instruments

An important factor in assessing the confidence we can place in measurements as difficult, yet as important, as the CMB power spectrum, is the agreement between experiments with different methods that are susceptible to different systematic effects. The VSA is similar in its sensitivity and angular coverage to several other CMB experiments that have reported results recently; BOOMERanG (Netterfield et al., 2002), MAXIMA (Hanany et al., 2000), DASI (Halverson et al., 2002) and CBI (Padin et al., 2001). Here we consider briefly the important systematic effects in the VSA in comparison to these experiments.

BOOMERanG and MAXIMA are focal-plane arrays of bolometers on small, off-axis telescopes suspended from stratospheric balloons. They have very high instantaneous sensitivity at frequencies where the total galactic and extragalactic foregrounds are at their minima, and they operate above most of the atmosphere, eliminating that as a source of contaminating emission. Their main problems are concerned with calibration; the uncertainties in the shapes and areas of the beams from each detector, and their pointing on the sky, limit the ability to recover the power spectrum at resolutions close to the beam size. Recovery of the power spectrum at very low $`\mathrm{}`$ is limited by receiver stability during each scan of the telescope. There is also an overall uncertainty in the temperature scale due to the lack of knowledge of the beam areas and, particularly for BOOMERanG, the lack of good flux calibration sources observed during the flight. The quoted uncertainty for the BOOMERanG power spectrum due to the temperature calibration is 20 percent, in addition to the beam uncertainty (Netterfield et al., 2002). Foreground contamination at 150 GHz is small, and dominated by galactic dust emission, the effect of which declines at higher $`\mathrm{}`$.

Calibration of instruments such as the VSA is much less problematic. Flux calibrators with well-studied properties are available (such as Cas A or Jupiter) and these can be observed repeatedly, and cross-checked with other secondary calibrators. Overall calibration error is dominated by the uncertainty in the absolute temperature of Jupiter, which is about 3.5 percent (Mason et al., 1999), leading to a 7 percent error in the power spectrum. The VSA is much less sensitive than the balloon experiments, however, with slightly worse random errors from 500 hours observation than MAXIMA’s from 3 hours. The main foreground contaminant is extragalactic point sources, whose effect increases as $`\mathrm{}^2`$. The dominant errors and contaminants are thus quite different from the balloon experiments, so agreement between VSA, BOOMERanG and MAXIMA would be a very good sign of the believability of the current power spectrum measurements.

Much the same arguments apply to the results from the other interferometers, DASI and CBI, which are very similar to the VSA in many respects, having similar numbers of antennas and the same observing frequency. However, there are significant differences between the three interferometer experiments which also allow for independent cross-checks of calibration and systematics. The VSA and CBI use the same primary flux calibrators; DASI, located at the south pole, is unable to see these and instead uses an absolute measurement of system temperature based on hot and cold loads. CBI, and DASI in its first season, had no ground screen, and hence suffered from significant pick-up of correlated emission from the ground, which had to be removed by differencing fields observed at the same ground angles. The VSA avoided this problem but suffered from a spurious correlated signal related to cross-coupling between the closest-spaced antennas, which is removed by Fourier filtering of the time-ordered data (see section 4.2).

The biggest design difference between the CBI and DASI on one hand and the VSA on the other is that the VSA has semi-independent tracking rather than fully co-mounted antennas. The resulting variation of path length to a source as the earth rotates imposes a modulation on the signal which can be used to very effectively reject signals from elsewhere in the sky, for example from the Sun or the Moon. This allows the VSA to observe during daylight, improving the observing efficiency. (Note that on a typical baseline there are 50 fringes during an observation of a primordial field.)

All of the current CMB experiments thus have different calibration and systematic problems, markedly so in the case of the interferometers versus the balloons, and therefore agreement between them is essential to establish the reliability of the power spectrum measurements.

## 3 CALIBRATION AND DATA REDUCTION

### 3.1 Amplitude and phase calibration

Absolute flux calibration of VSA observations is based on the flux scale of Mason et al. (1999). Our primary flux calibrator is Jupiter, for which the brightness temperature is taken to be 154.5 K at our observing frequency of 34 GHz. The solid angle of the planet is calculated at the epoch of each calibration observation and the flux determined. Jupiter is unresolved on all VSA baselines (including the source subtractor baseline) so no further correction is made for the angular size. We also observe Tau A and Cas A, whose fluxes are determined via our primary calibration of Jupiter. Transferring our calibration scale to both Cas A and Tau A ensures that an alternative bright calibrator source is always available should a Jupiter observation be lost due to, for example, bad weather, or obscured by the Sun or Moon. Care has to be taken, however, when transferring our flux calibration to Tau A, since it is known to be polarized (approximately 8 percent at 34 GHz, (Johnston & Hobbs, 1969)), and hence the flux as observed by the VSA changes with the hour angle of observation. To ensure that this does not introduce any systematic error, our calibration observations of Tau A are short and are made at the same hour angle each day.

We also make daily observations of two fainter sources, 3C48 and NGC7027, allowing us to check the quality of observations throughout the observing day. The measured flux ratios of these sources to our primary calibrators agree well with those reported by Mason et al., suggesting that the accuracy of our flux calibration is dominated by the error estimate of the absolute temperature of Jupiter, which is approximately 3.5 percent. Further to this, we have cross-checked our calibration with that used by the CBI instrument (Padin et al., 2001). CBI also uses Jupiter as one of its primary calibrators and, since they have a bandwidth of 10 GHz centred on 31 GHz, this has enabled them to estimate the spectral index of Jupiter and Saturn over the frequency range 26-36 GHz and hence cross-check our calibration at 34 GHz. We have cross-calibrations based on Jupiter and Saturn which agree to 1 percent.

Phase calibration of the VSA is also applied on a daily basis using the same three calibrators, Cas A, Tau A and Jupiter. The telescope is sufficiently phase stable that a single phase calibration made within $`\pm 12`$ hours of a CMB observation is adequate to calibrate the phases to $`<10^{}`$. In the same process, errors in the quadrature of up to $`15^{}`$ between the real and imaginary parts of each visibility are corrected for. These quadrature errors arise due to path differences in the cables going to the correlator boards. Consider two measured components of a visibility $``$ and $``$ at angles $`\varphi `$ and $`\psi `$ respectively from the theoretical fringe-rotated components $`^{\prime \prime }`$ and $`^{\prime \prime }`$. The quadrature error is $`\chi =\psi \varphi `$. Components $`^{}`$ and $`^{}`$ which are orthogonal to each other can be synthesised by rotating by $`\beta =\chi /2`$ in opposite directions. These can then be rotated by $`\alpha =\varphi +\beta `$ to give visibilities corresponding to the appropriate phase centre. Thus:

$$^{}=\frac{\mathrm{cos}\beta }{\mathrm{cos}\chi }+\frac{\mathrm{sin}\beta }{\mathrm{cos}\chi }$$

$$^{}=\frac{\mathrm{cos}\beta }{\mathrm{cos}\chi }+\frac{\mathrm{sin}\beta }{\mathrm{cos}\chi }$$

$$^{\prime \prime }=^{}\mathrm{cos}\alpha ^{}\mathrm{sin}\alpha $$

$$^{\prime \prime }=^{}\mathrm{cos}\alpha +^{}\mathrm{sin}\alpha $$

Figure 2 shows this scheme. Correcting for quadrature errors necessarily results in a loss of signal to noise by a factor $`\mathrm{cos}\chi `$ and the data must be down-weighted appropriately.

Figure 3 shows a typical CLEANed map of a calibrator, in this case Jupiter. Such maps are made daily to check the performance and stability of the telescope; the amplitude and phase stability are such that any un-CLEANed artefacts are below the thermal noise level. Since this observation has a higher signal-to-noise ratio than any CMB measurement, we can be confident that our CMB measurements are unaffected by dynamic range limitations.

### 3.2 Pointing and geometry accuracy

The pointing accuracy of the VSA is primarily determined by mechanical alignment tolerances, but we frequently make long observations of unresolved calibrators in order to check both the pointing and geometry of the array. Pointing is checked with two sets of observations. Firstly, the antennas in turn are offset in the antenna tracking co-ordinate on either side of the calibration source; secondly, the whole table is offset in the table tracking co-ordinate. These allow us to fit for offsets in the table and antenna encoders, and to check the co-alignment of the antennas. Alignment is better than 5 arcmin, about 1.5 percent of the beamwidth.

Geometry is checked using long observations of two or more calibrators at different declinations. In conjunction with a model of the telescope, we employ a maximum-likelihood technique to fit simultaneously for $``$400 parameters. These include the $`x`$, $`y`$ and $`z`$ co-ordinate of each antenna, complex gains for each of the 182 correlator channels and the effective observing bandwidth and frequency of each baseline. These parameters can be determined accurately enough to ensure that in subsequent CMB observations, phase and amplitude errors due to geometry errors are always less than the thermal noise.

### 3.3 System temperature calibration

The overall gain of each antenna is monitored via a noise injection system. A modulated noise signal is injected into each antenna via a probe in the horn, and is later measured using phase-sensitive detection after the automatic gain control stage in the IF system. The relative contribution of the constant noise source to the total output power from each antenna varies inversely with system temperature, and thus a correction can be made to the overall flux calibration. Assuming that the receiver temperature is constant, this system allows us to account for variations in atmospheric attenuation of the astronomical signal. It provides an excellent indication of the weather conditions and is used as a primary indicator for flagging data. For good observing conditions, the gain corrections applied using this system are typically less than a few percent.

### 3.4 Calibration of the source subtractor

Calibration of the source subtraction baseline is similar to that of the VSA main array. The primary flux calibrator for the source subtractor is NGC7027, whose flux is taken to be 5.45 Jy at 34 GHz. Observations of NGC7027 are made each day, in addition to observations of 3C48, 3C273 and Jupiter. The much higher flux sensitivity of the source subtractor makes it difficult to observe the same bright calibrators as the main array without using the low-gain setting of the correlator. Cross-calibration of the VSA and source subtractor is therefore achieved by low-gain observations of Jupiter; the gain switch is calibrated by observations of 3C273 in both gain states. Agreement between the VSA and source suntractor is found to be better than 3 percent.

Phase calibration of the source subtractor differs slightly from that for the main array. Since the source subtractor continually slews between pointed observations of point sources in the VSA fields, it is important to check the phase and pointing stability of source observation throughout an observing run. For this reason, between each set of 10 pointed source observations, we observe a phase calibrator source. The sources chosen to be phase calibrators need only be bright enough to get good signal-to-noise ratios in a 400 second integration, and are typically chosen to be the brightest sources already identified within a VSA field.

As with the main array, the long-term pointing accuracy and stability of the source subtractor baseline is monitored via long calibrator runs utilising the full range of hour angles.

### 3.5 Data reduction

The correlated signal from each of the 91 VSA baselines is sampled each second and, before the raw data are calibrated and smoothed, a series of preliminary flagging operations are performed. These are based on the status of the telescope each day, for which our main diagnostic tools are the system temperature monitor and automatic gain control levels, both of which monitor the power level from each antenna during an observation. This information can be used to flag for bad weather or warm cryostats. We also independently monitor the temperature of each cryostat, but the system temperature can be more sensitive and is useful as an early warning of problems with the cryogenics. Pointing errors are recorded throughout each observation, and the data are automatically flagged if the pointing error is greater than 0.5. Missing or repeated data samples, due to communication glitches between the correlator readout micro and the data recording computer, are also corrected. Finally, times at which the field centre is within 40 of the Sun or within 30 of the Moon are flagged, and a pre-analysis cut on the data at a 10-$`\sigma `$ level is applied. Typically, up to 3 percent of the data on each field is flagged in this manner.

As well as the fast ($`1`$ kHz) phase switching that is demodulated in hardware in the correlator, we also employ a slow phase switching sequence with a cycle time of 16s that is demodulated in software and removes any offsets in the hardware integration and sampling. After the initial flagging, the data are demodulated and smoothed over 16 seconds. Since this smoothing occurs before the data have been fringe rotated, a small amplitude correction must be applied to compensate for the reduction in amplitude of the raw fringes. The data can then be filtered for contaminating signals. As described in Section 4.2, the effects of contaminating signals, weather and bright sources outside the beam, can be effectively removed via the application of a high pass Fourier filter. For a typical VSA field observation, up to 20 percent of the data can be lost due to filtering, the majority of which is on baselines shorter than 30 $`\lambda `$. After filtering, the data are fringe-rotated to the centre of the field and calibrated. Phase calibration and quadrature correction are also implemented at this point. The system temperature correction is applied after the primary calibration, correcting for variations in the gain of each antenna and for changes in the atmospheric attenuation. Finally, the data are averaged to 64-second samples and a post-analysis chop at the 5-$`\sigma `$ level ($`150`$ Jy) is applied.

Although each day’s data must be examined and flagged individually, the basic data-reduction process outlined above can be applied automatically to the data for each field. As a further check on the data analysis, maps are made of both the calibrator and field observations for each day. The noise level on each map is checked to be consistent with that expected, and errors in the data analysis are easily detected.

## 4 CONTAMINANTS

As well as the CMB signal and thermal noise, the VSA data also include several types of contaminating signals, including bright sources such as the Sun and Moon, as well as instrumental artefacts. Here we describe the techniques for eliminating these from the data and checking the data for residual contaminants.

### 4.1 Spurious signal

Commissioning observations of blank fields showed that the VSA was detecting a correlated signal which did not originate from the sky (see Figure 4 for an example of this signal and its power spectrum).

Further investigation determined the following characteristics for the signal:

1. It is reasonably constant if the telescope is held stationary.
2. It is broad-band.
3. Its strength varies dramatically with baseline, peaking at approximately 1 mK on the shortest baselines but being undetectable on most longer baselines.
4. The signal vanishes if a large aluminium sheet is inserted between the antennas, indicating that the signal enters through the antennas and is related to coupling between them.
5. The signal does not vary when the tilt-table is driven in elevation, showing that the signal source is on the table rather than, for example, being radiation diffracting over the ground screen.
6. If the antennas are driven, the signal is modulated at a rate consistent with the rate of change of path between adjacent edges of the antennas. This means that during an observation of an astronomical source the maximum possible rate of change for the spurious signal is about 2 cycles per hour.

This spurious signal is not consistent with radiation from the receivers being coupled between the antennas, as the measured coupling even at the shortest spacings is less than $`100`$ dB, which would imply a correlated noise temperature of several hundred Kelvin being emitted by the receivers. Comparable levels of coupling have been measured by Padin et al. (2000) for the CBI telescope. Possible explanations for the source include thermal radiation from the antenna surface, or scattering of ambient radiation off one antenna that couples to another, an effect seen in the Australia Telescope Compact Array (R. Subrahmanyan, priv comm). However, the signal can be effectively removed from the data by suitable Fourier filtering of the time-ordered data.

### 4.2 Filtering according to astronomical fringe rate

Because of the semi-independent tracking of the VSA antennas, the correlated astronomical signal is modulated as the relative path length to the antennas changes. This modulation is typically much faster than the observed rate of change of the spurious signal. We can therefore filter out the spurious signal using a high-pass Fourier filter on the time-ordered data. We use a Hanning (cosine-edged) filter in order to minimise ringing, ie long-period correlations, in the time domain (Fig. 5).

Although most of the time the astronomical signals are modulated faster than the filter frequency and are thus not affected by it, at some times the fringe rate drops into the filter stop band; this depends on the baseline orientation, source position and hour angle. We flag out any data taken when the astronomical fringe rate lies within the cutoff range of the filter; in general this leads to approximately 20 percent of the visibilities for an observation being discarded. Figure 6 shows a single observation of a blank field with and without filtering; the filtered map is consistent with the thermal noise level.

We have studied the effect of this filtering on the data analysis by simulating CMB observations from sky realisations with $`\mathrm{\Lambda }`$CDM power spectra, following exactly the procedure used for real observations all the way through to maps and recovered power spectra, and have shown that any correlations introduced in the data by the filtering have negligible effect on the results.

### 4.3 Filtering of the Sun and Moon

It is possible to use the technique described above to remove the effects of very bright sources which lie well away from the field of view but are still detected in the sidelobes of the telescope beam. The source will in general have a different astronomical fringe rate to the field being observed. We therefore fringe rotate the data to the bright source, apply a high pass Fourier filter, fringe rotate back to the field centre, and flag any data where the fringe rate of the field lies within the range of the filter.

For the VSA the only sources that are bright enough to affect observations when they fall in distant sidelobes are the Sun and the Moon, which have approximate flux densities of 10 MJy and 0.3 MJy respectively at 34 GHz. For our observations of the CMB we do not observe any fields within $`40^{}`$ of the Sun or $`30^{}`$ of the Moon, and apply the above filtering technique whenever these sources are above the VSA ground screen.

The power of the technique is demonstrated in Figure 7 where Jupiter, with flux density of approximately 90 Jy, is observed within $`11^{}`$ of the Sun.

The filtered map shows that the contaminating effect of the Sun has been successfully removed and that the only significant feature in the map is a point source corresponding to Jupiter. Its flux density is as expected and the rms on the map is consistent with the thermal noise. We have examined the rms noise level on maps as a function of distance from the Sun with and without filtering. Figure 8 shows the rms noise levels per unit observation time on a sequence of 6-hour blank field observations at various distances from the Sun, both with and without filtering. Excess noise due to the Sun can be seen at angles less than $`40^{}`$ in the unfiltered case, but no excess noise is seen in the filtered data (although of course more and more data has to be flagged the closer the observation is to the Sun). For CMB observations, we do not use data taken less then $`40^{}`$ from the Sun, and we employ filtering.

## 5 Final commissioning observations

As a final checks of the telescope function we observed two regions in the Galactic plane. We observed the source NGC7027 with the telescope pointing and phase centres offset from the source position. This tests all the fringe rotation, calibration and mapping algorithms, as well as confirming the expected attenuation due to the primary beam. Also visible in the image (Figure 9) is some diffuse galactic emission (part of a larger structure that is cut off by the primary beam attenuation). This emission lies well outside of the primary beam of the source subtraction telescopes, which use NGC7027 as their primary calibrator.

We also observed the Cygnus-X region, an area of bright free-free extended emission, for which an independent observation with similar resolution at a close frequency was available. Fig 10 shows our observed 34 GHz contours are overlaid on 14.35 GHz Green Bank data (Langston et al., 2000). There is very good agreement between the structure observed at the two frequencies.

## 6 CONCLUSIONS

We have tested the operation of the VSA by observations of calibrators, blank sky, and extended galactic structure. The telescope has been demonstrated to work according to specification. In particular, we have shown that systematic effects such as the effects of the Sun and Moon, and coupling between the antennas, can be removed from the data to a very low level, allowing reliable long integrations on CMB fields. We have also shown that the data can be calibrated to an accuracy limited only by the absolute flux measurement of our primary calibrator, and that our separate telescope for observing point radio sources can be accurately cross-calibrated with the main array.

## ACKNOWLEDGEMENTS

We thank the staff of the Mullard Radio Astronomy Observatory, Jodrell Bank Observatory and the Teide Observatory for invaluable assistance in the commissioning and operation of the VSA. The VSA is supported by PPARC and the IAC. Partial financial support was provided by Spanish Ministry of Science and Technology project AYA2001-1657. A. Taylor, R. Savage, B. Rusholme, C. Dickinson acknowledge support by PPARC studentships. K. Cleary and J. A. Rubiño-Martin acknowledge Marie Curie Fellowships of the European Community programme EARASTARGAL, “The Evolution of Stars and Galaxies”, under contract HPMT-CT-2000-00132. K. Maisinger acknowledges support from an EU Marie Curie Fellowship. A. Slosar acknowledges the support of St. Johns College, Cambridge. We thank Professor Jasper Wall for assistance and advice throughout the project.


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# Optical band edge shift of anatase Ti1-xCoxO2-δ

(August 27, 2003)

## Abstract

We report on the optical properties of magnetic cobalt-doped anatase phase titanium dioxide Ti1-xCoxO2-δ films for low doping concentrations, $`0x0.02`$, in the spectral range $`0.2\mathrm{}\omega <5`$ eV. For well oxygenated films ($`\delta 1`$) the optical conductivity is characterized by an absence of optical absorption below an onset of interband transitions at 3.6 eV and a blue shift of the optical band edge with increasing Co concentration. The absence of below band gap absorption is inconsistent with theoretical models which contain midgap magnetic impurity bands and suggests that strong on-site Coulomb interactions shift the O-band to Co-level optical transitions to energies above the gap.

Dilute magnetic semiconductors (DMS) offer a possible system to realize control of the charge transport by using the spin degrees of freedom or ”spintronics”.Ohno (1998) DMS consist of magnetic impurities doped in a semiconducting host (e.g., Mn-doped GaAs). Such materials undergo a ferromagnetic phase transition below the Curie temperature, $`T_c`$ which is typically $`T_c100`$ K.

Therefore the recent discovery of ferromagnetism with $`T_c>300`$ K in cobalt-doped TiO2 has generated considerable interest in this system and similar dilute magnetic oxides.Matsumoto et al. (2001) High-temperature magnetization measurements using vibrating sample magnetometryShinde et al. (2003) find a $`T_c1180`$ K for $`x=0.07`$ Ti1-xCoxO2-δ, nearly that of bulk Co ($`T_c=1404`$ K). Such a large $`T_c`$, suggests that cobalt appears in clusters rather than substitutionally and that the resulting magnetism is due to clustered Co rather than a new dilute magnetic oxide. Indeed several groups report direct observation of cobalt clusters from transmission electron microscopy.Chambers et al. (2001); Shinde et al. (2003); Park et al.  In a careful study of doping dependence, Shinde et al.Shinde et al. (2003) find a limited solubility of cobalt in Ti1-xCoxO2-δ above a concentration of $`x0.02`$ with Co clustering beginning thereafter. Low-doped systems, $`x0.02`$, exhibit a $`T_c700`$ K and show no evidence of Co clusters. The existence of such a high $`T_c`$ for a dilute magnetic system showing no Co clustering remains puzzling. Thus, further measurements to elucidate the electronic structure and resolve the nature of the magnetism are warranted.

In this paper, we present measurements of the optical absorption of well-characterized thin films of anatase Ti1-xCoxO2-δ for low Co concentrations. Interband absorption above the band gap at 3.6 eV dominates the optical spectra. We discuss the implications of these results related to band structure calculations and compare our measured band edge shift to other optical studies.

Thin film samples of Ti1-xCoxO2-δ with $`x=0,0.01`$, and $`0.02`$ were grown on SrLaGaO4 (SLGO) substrates using pulsed laser deposition. Additionally, a pure TiO2 film was grown on LaAlO3 (LAO) for comparison. Films were deposited to $`1500`$ Å thickness with an oxygen partial pressure of 10-5 Torr corresponding to ($`\delta 1`$). 4-probe dc resistance measurements exhibit insulating behavior with room temperature resistivity $`\rho _{295\text{K}}10\mathrm{\Omega }`$cm. X-ray diffraction (XRD) measurementsShinde et al. (2003) of both pure and doped TiO2 films show peaks corresponding to those observed in bulk anatase TiO2. Values of the in-plane and out-of-plane ($`d_{004}`$) lattice constants obtained from XRD are discussed later in the paper.

Room temperature transmission $`𝒯(\omega )`$ and reflection $`(\omega )`$ measurements of near-normal incidence light at frequencies from 0.25 to 5 eV are performed using a Fourier-transform spectrometer.Quijada et al. (1998); Simpson et al. (1999) By numerically inverting the Fresnel formulasHeavens (1991) for $`𝒯`$ and $``$, we obtain the complex index of refraction $`\stackrel{~}{n}=n+ik`$ without the need for Kramers-Kronig analysis.Quijada et al. (1998); Simpson et al. (1999) From $`\stackrel{~}{n}(\omega )`$, we may derive other optical constants, e.g. the optical absorption $`\alpha (\omega )`$ or the complex optical conductivity $`\stackrel{~}{\sigma }(\omega )`$.

Historically, the spectral dependence of the band edge is characterized using the absorption coefficient, $`\alpha =4\pi \omega k`$, where $`\omega `$ is the frequency in cm-1 and $`k`$ is the extinction coefficient ($`k=`$ Im{$`\stackrel{~}{n}`$}). At photon energies above the band gap $`E_g`$, $`\alpha (\mathrm{}\omega E_g)^{1/2}`$ for a direct gap while $`\alpha (\mathrm{}\omega E_g)^2`$ for an indirect gap.Yu and Cardona (1996) Band structure calculationsAsahi et al. (2000) predict a direct gap at energies just lower than the onset of indirect transitions. In a detailed study of the absorption edge of single crystal anatase TiO2, Tang et al.Tang et al. (1995) report a band edge with $`E_g=3.420`$ eV and tentatively assigns the transition to a direct gap. Consistent with the behavior of a direct gap, we plot $`\alpha ^2`$ versus frequency in Fig. 1.

Linear fits to the high-frequency part above the band edge onset are extrapolated to zero absorption, giving the direct band gap energy $`E_g`$. Pure TiO2 exhibits $`E_g=3.6`$ eV, slightly larger than the value obtained by Tang et al.Tang et al. (1995) With increased Co concentration $`x`$, the band edge shifts to higher frequencies, showing a maximum shift of 100 meV for $`x=0.02`$. Apart from a band edge tail, there appears no evidence for strong absorption at frequencies below the gap. Additionally, we compared our results to linear fits of $`\sqrt{\alpha }`$ consistent with an indirect gap and found that while the indirect band edge is approximately 0.4 eV lower in energy, the shift of $`E_g`$ with doping remains unaffected. The exact nature of the gap (direct or indirect) remains uncertain.

While $`\alpha `$ well characterizes the band edge onset, the optical conductivity better suites to compare experimental results to predictions of band theory. In particular, the real part of the optical conductivity is given by $`\sigma _1(\omega )2nk\omega `$, where $`n`$ and $`k`$ are the real and imaginary part of the complex index of refraction respectively and $`\omega `$ is the frequency. Figure 2 shows the frequency dependence of $`\sigma _1`$ at room temperature for several Co concentrations. Throughout the mid-infrared (mid-IR) to visible frequency range (0.25 to 3 eV), $`\sigma _1`$ remains essentially zero, consistent with the negligible dc conductivity ($`\sigma _{dc}0.1\mathrm{\Omega }^1`$cm-1). At frequencies larger than 3 eV, $`\sigma _1`$ increases rapidly corresponding to the increase in absorption as seen in Fig. 1. To further elucidate the minimal midgap conductivity, we expand the scale in the inset of Fig 2. Although no strong conductivity in the spectral range $`1\mathrm{}\omega 3`$ is observed, $`\sigma _1`$ increases slightly near the edge, although non-monotonically, with the addition of Co. Such an increase may result from the Co levels in the gap or disorder effects on the Urbach tailTang et al. (1995) of the fundamental absorption edge.

It is interesting to compare the optical conductivity and band edge shifts with photoluminescence (PL) spectra. PL studiesGuha et al. ; Tang et al. (1993, 1994) find a broad peak centered around 2.3 eV for anatase TiO2. The peak in the PL spectrum is Stokes shifted 1.3 eV lower than the onset of interband transitions in the optical conductivity and the peak in the photoluminescence excitation spectrum.Tang et al. (1994) Such a Stokes shift is consistent with that of a self-trapped exciton where the exciton loses energy nonradiatively to the lattice. With the addition of Co, the peak of the PL spectrum blue shifts,Guha et al.  similar to the shift observed in the band edge. Doping dependent shifts in the band edge and the PL peak are plotted together in Fig. 3 for comparison. The direct band gap energy increases monotonically with $`x`$, while the PL peak increases rather abruptly upon the addition of Co and saturates above $`x=0.02`$. The saturation of the shift at higher doping concentrations is consistent with the limited solubility of Co in TiO2 as reported earlier.Shinde et al. (2003)

Similar shifts of the band edge as observed here with Co doping are reported in a pressure-dependent optical study of single x-tal anatase TiO2. Sekiya et al.Sekiya et al. (2001) observe a blue shift of the band edge upon the application of hydrostatic pressure. For an applied pressure of 3.9 GPa, the edge shifts to higher energy by $`50`$ meV. We estimate the change in the TiO2 lattice resulting from the hydrostatic pressure by introducing the bulk modulus, $`B=V\mathrm{\Delta }P/\mathrm{\Delta }V`$, where $`V`$ is the volume, $`\mathrm{\Delta }V`$ is the change in volume, and $`P`$ is the applied pressure. Taking the bulk modulus for anatase TiO2, $`B=180`$ GPa,Arlt et al. (2000) the applied hydrostatic pressure of 3.9 GPa introduces a volume decrease of $`2`$%.

Given the blue shift of the band edge with increasing pressure or equivalently decreasing lattice size, we consider how substrate strain or the addition of cobalt may affect the lattice. Firstly the issue of substrate strain, the thin films studied suffer strain due to lattice mismatch with the substrates. For epitaxial films the initial layers grow coherently with the substrate but defects gradually relax the induced strain allowing the films to grow more like bulk. Values of the in-plane lattice constant, $`a`$, for bulk TiO2, LAO, and SLGO are listed in Table 1.

Both LAO and SLGO substrates have a larger in-plane lattice parameter than bulk TiO2, introducing a tensile strain in the films of approximately 0.12% and 1.5%, respectively. The tensile stress tends to expand the TiO2 lattice in the plane. For materials with a typical Poisson ratio, an expansion in the plane results in a reduction of the out-of-plane lattice constant, $`d_{004}`$. Indeed XRD measurements of the TiO2 films reveal such a decrease of $`d_{004}`$, as shown in Table 1. The film on SLGO, with the larger in-plane tensile strain, exhibits a larger reduction in $`d_{004}`$ relative to bulk TiO2 ($`0.45\%`$) compared with the film on LAO ($`0.08\%`$). To explore the effects of lattice strain on the band edge, the absorption of a TiO2 film grown on LAO is shown in Fig. 1. The band edge of the film on LAO with the smaller in-plane lattice is blue shifted ($`100`$ meV) relative to the TiO2 film grown on SLGO, consistent with the blue shift resulting from the application of hydrostatic pressure discussed above.

To address the effect of cobalt substitution on the shift of the band edge, we examine the change in size of the lattice with doping. Cobalt appears in the doped TiO2 system in the +2 formal oxidation state as determined from x-ray absorption spectroscopy.Chambers et al. (2001) The atomic radii of Co2+ and Ti4+ are 0.82 Å and 0.69 Å, respectively.Emsley (1998) Substitution of the larger Co2+ for Ti4+ should expand the lattice. XRD measurementsShinde et al. (2003) of films grown on LAO (plotted in Fig. 3) show $`d_{004}`$ increases with $`x`$, saturating at about $`x=0.02`$. The increase of $`d_{004}`$ supports the prediction of an increase in the size of the lattice with Co doping. For the films grown on SLGO, $`d_{004}`$ remains relatively constant with Co, $`d_{004}=2.3674\pm 0.0002`$ Å. An increasing (films on LAO) or relatively constant (films on SLGO) lattice size with $`x`$ should result in either a red shift or no shift of the band edge. Therefore, the observed blue shift with Co doping cannot be ascribed simply to a change of the lattice size.

In order to understand the observed blue shift of the band edge, we compare our conductivity to theoretical predictions of the electronic structure of both pure and Co-doped TiO2. Band structure calculationsMo and Chin (1995); Park et al.  indicate the valence band derives primarily from oxygen p-levels, the conduction band derives from the Ti d-levels, and that the crystal-field split Co d-levels fall within the energy gap.Park et al.  These midgap states would lead to below band gap optical absorption in a non-interacting electron picture of optical transitions. Using a first-principles density-functional approach, Yang et al.Yan et al. (2003) calculates the dielectric function for Co-doped TiO2. The resulting $`\sigma _1`$ for $`x=0.125`$ and pure TiO2 are shown in the inset of Fig. 2 for comparison.

The predicted increase in conductivity below the band gap results from transitions to cobalt levels. We may estimate the effective Co number density using optical sum rules.

$$S(\omega )=\frac{2}{\pi }_0^\omega \sigma _1(\omega ^{})𝑑\omega ^{}=\frac{N_{eff}e^2}{m},$$
(1)
where $`N_{eff}`$ is the effective carrier density, which in general will be somewhat less than the cobalt number density $`N`$, $`e`$ is the electron charge, and $`m`$ is the electron mass. The cobalt number density $`N`$ as a function of $`x`$ is given by $`N=\frac{fx}{V}`$, where $`f=4`$ is the number of Ti per unit cell and $`V=136.85`$ Å3 is the unit cell volume. Estimating $`N_{eff}`$ from the predicted conductivity using Eq. 1 and comparing to $`N`$, we find that approximately 0.75 of the total Co spectral weight appears in the predicted midgap absorption feature. In estimating the Co spectral weight from the experimental data we take the difference in $`\sigma _1`$ due to doping to be a constant $`10\mathrm{\Omega }^1`$cm-1 (corresponding to the error in our measurement) over the frequency range from 1 to 3 eV. Substituting into Eq. 1, we find the experimental upper bound for $`N_{eff}10^{20}`$ cm-3. Comparing this to the number density $`N`$ we find the upper bound on the observed density of Co is roughly 0.15 times the expected total.

The absence of below gap optical excitations in the measured conductance may be understood either as evidence that the band calculations are not capturing the electronic structure of this material under the assumed charge state of the cobalt or that the on-site Coulomb energy, $`U`$, for adding another electron to the Co ion is large. In the second scenario the experiment implies $`U3`$ eV.

Noting the absence of spectral weight associated with cobalt levels in the gap combined with the blue shift of the band edge, we examine the possible strong interaction effects on the optical transitions involving the Co ion. First we reject interpretations that consider the alloy within a rigid band picture. In this case a shift in the band edge results from uniform shifts of the conduction band due to the average Ti/Co potentials. Since the atomic potentials for Co are larger that those of Ti, the Ti/Co band would be lower than the pure Ti bands in TiO2 resulting in a red shift of the band edge, contrary to observation. Indeed the rigid band approach is more appropriate for delocalized states. For the transition metal ions in Ti1-xCoxO2-δ a localized picture is more appropriate. Therefore, we discuss the processes operating on the optical transitions involving the Co levels within a localized picture. A schematic view of the band structure is shown in Fig. 4.

In pure TiO2, the band edge $`E_g`$ consists of the energy difference between the filled O p-levels and the empty Ti d-levels with $`E_g3.6`$ eV (as discussed above). With the addition of cobalt, charge transfer transitions from the O p-levels to the empty localized Co2+ d-levels become possible. Allowed transitions from occupied Co levels to the Ti levels should be weaker since they involve a virtual transition through the O p-levels. The energy $`E_1`$ of the oxygen to cobalt transition is the sum of the charge transfer energy $`\mathrm{\Delta }_{\text{Co}}`$ plus the on-site Coulomb energy $`U`$; $`E_1=\mathrm{\Delta }_{\text{Co}}+U`$. The observed absence of below band gap absorption indicates that $`E_1`$ is greater than the band gap in the alloy $`E_g^{}`$. This is reasonable since the $`U`$ is estimated to be $`3`$ eV and the empty Co levels are $`2`$ eV above the oxygen band.Park et al.

We now turn our attention to the observed band edge shift, $`\mathrm{\Delta }E_g=\xi x`$, where $`\xi =5`$ eV. If the O and Ti band edges are not affected by the substitution of Co, this shift would be understood in terms of the reduction of the interband oscillator strength upon Ti dilution by Co and the extra absorption at $`E_1`$. However, this scenario leads not to a shift in the band edge but essentially to a change in the slope of $`\alpha ^2`$, contrary to observation. Therefore we conclude that O and Ti bands separate upon Co substitution. The large rate of separation ($`\xi =5`$ eV) implies strong level repulsion that might occur for interstitial incorporation of the Co. This large band edge shift is especially interesting because it implies strong interactions which are also required to provide the large exchange interaction and associated high ferromagnetic $`T_c`$ observed in this material.

In conclusion, optical measurements have revealed a shift of the band edge with Co doping and an absence of midgap absorption in anatase Ti1-xCoxO2-δ. The gap in the optical conductivity also implies strong Coulomb interaction effects on the optical processes involving the Co ions.

###### Acknowledgements.

We wish to thank A. J. Millis, S. Das Sarma, and G. A. Sawatzky for valuable discussions and Y. Zhao for help with experimentation. This work supported in part by NSF-MRSEC Grant No. DMR-00-80008 and DARPA (S.D.S.).