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# Universal Similarity Factorization Equalities over Complex Clifford Algebras

## 1 Introduction

Let $`𝒞_n`$ be the complex Clifford algebra, with the identity 1, defined on $`n`$ generators $`e_1,e_2,\mathrm{},e_n`$ subject to the multiplication laws:

$`e_i^2`$ $`=1,i=1,2,\mathrm{},n,`$ (1)
$`e_ie_j+e_je_i`$ $`=0,ij,i,j=1,2,\mathrm{},n,`$ (2)
and $`e_1e_2\mathrm{}e_n\pm 1.`$ In that case $`𝒞_n`$ is spanned as a $`2^n`$-dimensional vector space with $`2^n`$ basis $`\{e_A\},`$ where the multi index $`A`$ ranges all naturally ordered subsets of the first positive integer set $`\{1,2,\mathrm{},n\};`$ the basis element $`e_A,`$ where $`A=(i_1,i_2,\mathrm{},i_k)`$ with $`1i_1<i_2<\mathrm{}<i_kn,`$ is defined as the product

$$e_Ae_{(i_1,i_2,\mathrm{},i_k)}=e_{i_1}e_{i_2}\mathrm{}e_{i_k},e_{A=\mathrm{}}=1.$$

For simplicity, the volume element $`e_{12\mathrm{}n}=e_1e_2\mathrm{}e_n`$ of $`𝒞_n`$ will be denoted by $`e_{[n]}`$ in the sequel. The square of the volume element is

$$e_{[n]}^2=(1)^{\frac{1}{2}n(n1)}e_1^2e_2^2\mathrm{}e_n^2.$$

In that case, all $`a𝒞_n`$ can be expressed as

$$a=\underset{A}{}a_Ae_A,a_A𝒞,$$

where $`A`$ ranges all naturally ordered subsets of $`\{1,2,\mathrm{},n\}.`$ We shall adopt the following notation from now on: $`𝒞_n:=𝒞\{e_1,\mathrm{},e_n\}.`$

Clifford algebras (real or complex) have been studied for many years and their algebraic properties are well known. In particular, all Clifford algebras are classified as matrix algebras, or as direct sums of matrix algebras over the fields of real or complex numbers, or the quaternion ring (see, e.g., ). For complex Clifford algebras $`𝒞_n,`$ it is well known that they can faithfully be realized as certain matrix algebras over $`𝒞,`$ and the general algebraic isomorphism is

$$𝒞_n\{\begin{array}{cc}𝒞(2^{\frac{n}{2}})\hfill & \text{if }n\text{ is even,}\hfill \\ {}_{}{}^{2}𝒞(2^{\frac{n1}{2}})\hfill & \text{if }n\text{ is odd,}\hfill \end{array}$$
(3)
where $`𝒞(s)`$ stands for the $`s\times s`$ total complex matrix algebra, and $`{}_{}{}^{2}𝒞(s)`$ stands for the complex matrix algebra

$${}_{}{}^{2}𝒞(s)=\left\{\left[\begin{array}{cc}A& 0\\ 0& B\end{array}\right]\right|A,B𝒞(s)\}.$$

In this article we improve this relationship to a new level by establishing a set of valuable universal similarity factorization equalities between elements of $`𝒞_n`$ and complex matrices over $`𝒞(2^{\frac{n}{2}})`$ or $`𝒞(2^{\frac{n1}{2}})`$ for all $`n.`$ Through these universal factorization equalities the complex matrix representations of elements in $`𝒞_n`$ can explicitly be established. Based on them various results in the complex matrix theory can directly be extended to complex Clifford numbers. Moreover, one can also easily develop matrix analysis over complex Clifford algebras.

We first establish some basic universal similarity factorization equalities for elements in Clifford algebras with dimensions $`2`$ and $`4,`$ which will be directly applied to establish some more general results for $`𝒞_n.`$

Lemma 1. Let $``$ be an algebraically closed field and $`_1=\{e|e^2=u\}`$ be a Clifford algebra defined on a generator $`e`$ with $`e^2=u`$ and $`u0.`$ Then all $`a_1`$ can be written as $`a=a_0+a_1e,`$ where $`a_0,a_1.`$ Moreover, define $`\overline{a}=a_0a_1e.`$ In that case, $`a`$ and $`\overline{a}`$ satisfy the following universal similarity factorization equality

$$P\left[\begin{array}{cc}\hfill a& \hfill 0\\ \hfill 0& \hfill \overline{a}\end{array}\right]P^1=\left[\begin{array}{cc}a_0+\sqrt{u}a_1& 0\\ 0& a_0\sqrt{u}a_1\end{array}\right],$$
(4)
where $`P`$ and $`P^1`$ have the following universal forms (no relation with $`a):`$

$`P`$ $`={\displaystyle \frac{1}{2}}\left[\begin{array}{cc}1+\frac{1}{\sqrt{u}}e& (\sqrt{u}e)\\ \frac{1}{u}(\sqrt{u}e)& 1+\frac{1}{\sqrt{u}}e\end{array}\right],`$ (7)
$`P^1`$ $`={\displaystyle \frac{1}{2}}\left[\begin{array}{cc}1+\frac{1}{\sqrt{u}}e& \sqrt{u}e\\ \frac{1}{u}(\sqrt{u}e)& 1+\frac{1}{\sqrt{u}}e\end{array}\right].`$ (10)
Proof. Note that $`e^2=u.`$ It is easy to verify that

$$\left[\begin{array}{cc}1& e\\ e^1& 1\end{array}\right]\left[\begin{array}{cc}a& \hfill 0\\ 0& \hfill \overline{a}\end{array}\right]\left[\begin{array}{cc}1& e\\ e^1& 1\end{array}\right]=\left[\begin{array}{cc}a_0& ua_1\\ a_1& a_0\overline{a}\end{array}\right].$$

On the other hand, it is also easy to verify that

$$\left[\begin{array}{cc}1& \sqrt{u}\\ \frac{1}{\sqrt{u}}& 1\end{array}\right]\left[\begin{array}{cc}a_0+ua_1& 0\\ 0& a_0ua_1\end{array}\right]\left[\begin{array}{cc}1& \sqrt{u}\\ \frac{1}{\sqrt{u}}& 1\end{array}\right]=\left[\begin{array}{cc}a_0& ua_1\\ a_1& a_0\overline{a}\end{array}\right].$$

Combining the above two equalities yields (4) and (10). $`\mathrm{}`$

Lemma 2. Let $`M_2()`$ be the $`2\times 2`$ total matrix algebra over an arbitrary field $``$ with its basis satisfying the multiplication rules

$$\tau _{pq}\tau _{st}=\{\begin{array}{cc}\tau _{pt},\hfill & q=s,\hfill \\ 0,\hfill & qs,\hfill \end{array}$$
(11)
for $`p,q,s,t=1,2.`$ Then all $`a=a_{11}\tau _{11}+a_{12}\tau _{12}+a_{21}\tau _{21}+a_{22}\tau _{22}M_2(),`$ where $`a_{pq},`$ satisfy the following universal similarity factorization equality

$$Q\left[\begin{array}{cc}a& 0\\ 0& a\end{array}\right]Q^1=\left[\begin{array}{cc}a_{11}& a_{12}\\ a_{21}& a_{22}\end{array}\right],$$
(12)
where $`Q`$ has the following universal form

$$Q=Q^1=\left[\begin{array}{cccc}\tau _{11}& \tau _{21}& & \\ \tau _{12}& \tau _{22}& & \end{array}\right].$$
(13)
Proof. Follows directly from a verification. $`\mathrm{}`$

Lemma 3. Let $``$ be an algebraically closed field of characteristic not two, and $`_2=\{e_1,e_2\}`$ be a Clifford algebra defined on two generators $`e_1,e_2`$ with $`e_1^2=u,e_2^2=v`$ and $`u0,v0.`$ Then all $`a_2`$ can be written as

$$a=a_0+a_1e_1+a_2e_2+a_3e_{12},$$
(14)
where $`a_0,\mathrm{},a_3.`$ In that case, $`aI_2`$ satisfies the following universal similarity factorization equalities

$$R\left[\begin{array}{cc}\hfill a& \hfill 0\\ \hfill 0& \hfill a\end{array}\right]R^1=\left[\begin{array}{cc}a_0+\sqrt{u}a_1& v(a_2+\sqrt{u}a_3)\\ a_2\sqrt{u}a_3& a_0\sqrt{u}a_1\end{array}\right],$$
(15)
and

$$T\left[\begin{array}{cc}\hfill a& \hfill 0\\ \hfill 0& \hfill a\end{array}\right]T^1=\left[\begin{array}{cc}a_0+\sqrt{v}a_1& u(a_1\sqrt{v}a_3)\\ a_1+\sqrt{v}a_3& a_0\sqrt{v}a_1\end{array}\right],$$
(16)
where

$$R=R^1=\frac{1}{2}\left[\begin{array}{cc}1+\frac{1}{\sqrt{u}}e_1& e_2\frac{1}{\sqrt{u}}e_{12}\\ \frac{1}{v}(e_2+\frac{1}{\sqrt{u}}e_{12})& 1\frac{1}{\sqrt{u}}e_1\end{array}\right],$$
(17)
and

$$T=T^1=\frac{1}{2}\left[\begin{array}{cc}1+\frac{1}{\sqrt{v}}e_2& e_1+\frac{1}{\sqrt{v}}e_{12}\\ \frac{1}{u}(e_1\frac{1}{\sqrt{v}}e_{12})& 1\frac{1}{\sqrt{v}}e_2\end{array}\right].$$
(18)
Proof. By Lemma 2, we take the change of basis of $`_2`$ as follows

$`\tau _{11}`$ $`={\displaystyle \frac{1}{2}}\left(1+{\displaystyle \frac{1}{\sqrt{u}}}e_1\right),`$ $`\tau _{12}`$ $`={\displaystyle \frac{1}{2v}}\left(e_2+{\displaystyle \frac{1}{\sqrt{u}}}e_{12}\right),`$ (19a)
$`\tau _{21}`$ $`={\displaystyle \frac{1}{2}}\left(e_2{\displaystyle \frac{1}{\sqrt{u}}}e_{12}\right),`$ $`\tau _{22}`$ $`={\displaystyle \frac{1}{2}}\left(1{\displaystyle \frac{1}{\sqrt{u}}}e_1\right).`$ (19b)
Then it is not hard to verify that this new basis satisfies the multiplication rules in (11). In this new basis, any $`a=a_0+a_1e_1+a_2e_2+a_3e_{12}_2`$ can be rewritten as

$$a=(a_0+\sqrt{u}a_1)\tau _{11}+(va_2+\sqrt{u}a_3)\tau _{12}+(a_2\sqrt{u}a_3)\tau _{21}+(a_0\sqrt{u}a_1)\tau _{22}.$$

Substituting this and (19) into (12) and (13), we can obtain (15) and (17). By the similar approach, we can get (16) and (18). $`\mathrm{}`$

## 2 Main results

Notice that $`𝒞`$ is an algebraically closed field. We then can establish a set of universal similarity factorization equalities for elements in $`𝒞_n`$ on the basis of Lemmas 1 and 3.

Theorem 4. Let $`a𝒞_1=𝒞\{e\}`$ be given. Then $`a`$ can be written as $`a=a_0+a_1e,`$ where $`a_0,a_1𝒞=\{x+iy|x,y\}.`$ Moreover denote by $`\overline{a}=a_0a_1e,`$ called the conjugate of $`a.`$ Then $`a`$ and $`\overline{a}`$ satisfy the following universal similarity factorization equality

$$P_1\left[\begin{array}{cc}\hfill a& \hfill 0\\ \hfill 0& \hfill \overline{a}\end{array}\right]P_1^1=\left[\begin{array}{cc}a_0+a_1i& 0\\ 0& a_0a_1i\end{array}\right],$$
(20)
where $`P_1`$ and $`P_1^1`$ have the following universal forms (no relation with $`a):`$

$$P_1=\frac{1}{2}\left[\begin{array}{cc}1ie& (ie)\\ (ie)& 1ie\end{array}\right],P_1^1=\frac{1}{2}\left[\begin{array}{cc}1ie& ie\\ ie& 1ie\end{array}\right].$$
(21)
Proof. Let $`=𝒞`$ and $`u=1`$ as in Lemma 1. Then (20) and (21) follow directly from (4) and (10). $`\mathrm{}`$

It is easy to verify that

$$\overline{\overline{a}}=a,\overline{a+b}=\overline{a}+\overline{b},\overline{ab}=\overline{a}\overline{b},\overline{\lambda a}=\overline{a\lambda }=\lambda \overline{a}.$$
(22)
hold for all $`a,b𝒞_1`$ and $`\lambda 𝒞.`$ According to (20), we define a map from $`𝒞_1`$ to the double field $`𝒞𝒞`$ by

$$\varphi _1:a=a_0+a_1e𝒞_1\left[\begin{array}{cc}a_0+a_1i& 0\\ 0& a_0a_1i\end{array}\right]𝒞𝒞.$$
(23)
Then it is easy to derive from (20) and (22) the following properties.

Corollary 5. Let $`a=a_0+a_1e,b=b_0+b_1e𝒞_1,\lambda 𝒞`$ be given, and $`\varphi _1`$ be defined by (23). Then

* $`a=b\varphi _1(a)=\varphi _1(b).`$
* $`\varphi _1(a+b)=\varphi _1(a)+\varphi _1(b),\varphi _1(ab)=\varphi _1(a)\varphi _1(b),\varphi _1(\lambda a)=\lambda \varphi _1(a),`$ $`\varphi _1(1)=I_2.`$
* $`\varphi _1(\overline{a})=\left[\begin{array}{cc}0& 1\\ 1& 0\end{array}\right]\varphi _1(a)\left[\begin{array}{cc}0& 1\\ 1& 0\end{array}\right].`$
* Denote $`a^\mathrm{\#}=\overline{a_0}\overline{a_1}e,`$ then $`\varphi _1(a^\mathrm{\#})=\varphi _1^{}(a),`$ the conjugate transpose of the complex matrix $`\varphi _1(a).`$
* $`a=\frac{1}{4}[1ie,ie]\varphi _1(a)[1ie,ei]^T.`$
* $`det[\varphi _1(a)]=a_0^2+a_1^2.`$
* $`a`$ is invertible $``$ $`\varphi _1(a)`$ is invertible, in which case $`\varphi _1(a^1)=\varphi _1^1(a).`$

The properties in Corollary 5(a) and (b) show that through the bijective map (23), the Clifford algebra $`𝒞_1`$ is algebraically isomorphic to the double field $`𝒞𝒞`$, and $`\varphi _1(a)`$ is a faithful matrix representation of $`a`$ in $`𝒞𝒞.`$

Notice that $`P_1`$ and $`P_1^1`$ in (20) have no relation with $`a.`$ Thus the equality in Theorem 4 can also be extended to all matrices over the complex Clifford algebra $`𝒞_1.`$

Theorem 6. Let $`A=A_0+A_1e𝒞_1^{m\times n}`$ be given, where $`A_0,A_1𝒞^{m\times n}.`$ Then $`A`$ and its conjugate $`\overline{A}=A_0A_1e`$ satisfy the following universal factorization equality

$`J_{2m}\left[\begin{array}{cc}A& 0\\ 0& \overline{A}\end{array}\right]J_{2n}^1`$ $`=\left[\begin{array}{cc}A_0+A_1i& 0\\ 0& A_0A_1i\end{array}\right],`$ (28)
where

$`J_{2m}`$ $`={\displaystyle \frac{1}{2}}\left[\begin{array}{cc}(1ie)I_m& (ie)I_m\\ (ie)I_m& (1ie_1)I_m\end{array}\right],`$ (31)
$`J_{2n}^1`$ $`={\displaystyle \frac{1}{2}}\left[\begin{array}{cc}(1ie_1)I_n& (ie)I_n\\ (ie)I_n& (1ie)I_n\end{array}\right].`$ (34)
In particular, if $`m=n,`$ then (28) becomes a universal similarity factorization equality over $`𝒞_1`$.

It is easy to verify that for any matrices $`A,B𝒞_1^{m\times n},C𝒞_1^{n\times p},`$ and $`\lambda 𝒞`$

$$\overline{\overline{A}}=A,\overline{A+B}=\overline{A}+\overline{B},\overline{AC}=\overline{A}\overline{C},\overline{\lambda A}=\overline{A\lambda }=\lambda \overline{A}.$$
(35)
Now according to (28), we define the complex matrix representation of a matrix $`A=A_0+A_1e𝒞_1^{m\times n}`$ by $`\mathrm{\Phi }_1(A)=\left[\begin{array}{cc}A_0+A_1i& 0\\ 0& A_0A_1i\end{array}\right].`$ Then the following properties can be easily derived from (28) and (35).

Corollary 7. Let $`A,B𝒞_1^{m\times n},C𝒞_1^{n\times p}`$ and $`\lambda 𝒞`$ be given. Then

* $`A=B\mathrm{\Phi }_1(A)=\mathrm{\Phi }_1(B).`$
* $`\mathrm{\Phi }_1(A+B)=\mathrm{\Phi }_1(A)+\mathrm{\Phi }_1(B).`$
* $`\mathrm{\Phi }_1(AC)=\mathrm{\Phi }_1(A)\mathrm{\Phi }_1(C),\mathrm{\Phi }_1(\lambda A)=\lambda \mathrm{\Phi }_1(A),\mathrm{\Phi }_1(I_m)=I_{2m}.`$
* $`\mathrm{\Phi }_1(\overline{A})=\left[\begin{array}{cc}0& I_m\\ I_m& 0\end{array}\right]\mathrm{\Phi }_1(A)\left[\begin{array}{cc}0& I_n\\ I_n& 0\end{array}\right].`$
* Let $`A=A_0+A_1e`$ and denote $`A^\mathrm{\#}=A_0^{}A_1^{}e,`$ where $`A_0^{}`$ and $`A_1^{}`$ are the conjugate transposes of the complex matrices $`A_0`$ and $`A_1.`$ Then $`\mathrm{\Phi }_1(A^\mathrm{\#})=\mathrm{\Phi }_1^{}(A),`$ the conjugate transpose of the complex matrix $`\mathrm{\Phi }_1(A).`$
* $`A=\frac{1}{4}[(1ie)I_m,(ie)I_m]\mathrm{\Phi }_1(A)[(1ie)I_n,(ei)I_n]^T.`$
* $`A`$ is invertible $``$ $`\mathrm{\Phi }_1(A)`$ is invertible, in which case $`\mathrm{\Phi }_1(A^1)=\mathrm{\Phi }_1^1(A).`$
* $`p_A(A)=0,`$ where $`p_A(x)=det[xI_{2m}\mathrm{\Phi }_1(A)].`$

Theorem 8. Let $`a𝒞_2=𝒞\{e_1,e_2\},`$ the complex quaternion algebra. Then $`a`$ can be written as

$$a=a_0+a_1e_1+a_2e_2+a_3e_{12},$$

where $`a_0,\mathrm{},a_3𝒞.`$ In that case, $`aI_2`$ satisfies the following universal similarity factorization equality

$$P_2\left[\begin{array}{cc}a& 0\\ 0& a\end{array}\right]P_2^1=\left[\begin{array}{cc}a_0+a_1i& (a_2+a_3i)\\ a_2a_3i& a_0a_1i\end{array}\right],$$
(36)
where $`P_2`$ has the universal form

$$P_2=P_2^1=\frac{1}{2}\left[\begin{array}{cc}1ie_1& e_2+ie_{12}\\ e_2+ie_{12}& 1+ie_1\end{array}\right].$$
(37)
Proof. Let $`=𝒞`$ and $`u=v=1`$ in Lemma 3. Then (36) and (37) follow from (15) and (17). $`\mathrm{}`$

According to (36), define a map from $`𝒞_2`$ to the $`2\times 2`$ complex matrix algebra $`𝒞^{2\times 2}`$ by

$$\varphi _2:a=a_0+a_1e_1+a_2e_2+a_3e_{12}𝒞_2\left[\begin{array}{cc}a_0+a_1i& (a_2+a_3i)\\ a_2a_3i& a_0a_1i\end{array}\right]𝒞^{2\times 2}.$$
(38)
Then we can easily derive from (36) the following properties.

Corollary 9. Let $`a,b𝒞_2=𝒞\{e_1,e_2\}`$ and $`\lambda 𝒞`$ be given. Then

* $`a=b\varphi _2(a)=\varphi _2(b).`$
* $`\varphi _2(a+b)=\varphi _2(a)+\varphi _2(b),\varphi _2(ab)=\varphi _2(a)\varphi _2(b),\varphi _2(\lambda a)=\lambda \varphi _2(a),`$ $`\varphi _2(1)=I_2.`$
* Let $`a=a_0+a_1e_1+a_2e_2+a_3e_{12}𝒞_2,`$ and denote $`a^\mathrm{\#}=\overline{a_0}\overline{a_1}e_1\overline{a_2}e_2\overline{a_3}e_{12}.`$ Then $`\varphi _2(a^\mathrm{\#})=\varphi _2^{}(a),`$ the conjugate transpose of the complex matrix $`\varphi _2(a).`$
* $`a=\frac{1}{4}[1ie,e_2+ie_{12}]\varphi _2(a)[1ie,e_2+ie_{12}]^T.`$
* $`det[\varphi _2(a)]=a_0^2+a_1^2+a_2^2+a_3^2.`$
* $`a`$ is invertible $`\varphi _2(a)`$ is invertible, in which case $`\varphi _2(a^1)=\varphi _2^1(a).`$
* The two elements $`a`$ and $`b`$ in $`𝒞_2`$ are similar, i.e., there is an invertible $`x𝒞_2`$ such that $`ax=xb`$ if and only if the two complex matrices $`\varphi _2(a)`$ and $`\varphi _2(b)`$ are similar over $`𝒞.`$

The properties in Corollary 9(a) and (b) clearly show that through the bijective map (38) the Clifford algebra $`𝒞_2,`$ i.e., the complex quaternion algebra, is algebraically isomorphic to the complex matrix algebra $`𝒞^{2\times 2},`$ and $`\varphi _2(a)`$ is a faithful matrix representation of $`a`$ in $`𝒞^{2\times 2}.`$

Notice that $`P_2`$ and $`P_2^1`$ in (37) have no relation to $`a.`$ Thus the equality in Theorem 8 can also be extended to all matrices over $`𝒞_2.`$

Theorem 10. Let $`A=A_0+A_1e_1+A_2e_2+A_3e_{12}𝒞_2^{m\times n}=𝒞^{m\times n}\{e_1,e_2\}`$ be given where $`A_0,\mathrm{},A_3𝒞^{m\times n}.`$ Then $`A`$ satisfies the following universal factorization equality

$`K_{2m}\left[\begin{array}{cc}A& 0\\ 0& A\end{array}\right]K_{2n}^1`$ $`=\left[\begin{array}{cc}A_0+A_1i& (A_2+A_3i)\\ A_2A_3i& A_0A_1i\end{array}\right],`$ (43)
where

$$K_{2t}=K_{2t}^1=\frac{1}{2}\left[\begin{array}{cc}(1ie_1)I_t& (e_2+ie_{12})I_t\\ (e_2+ie_{12})I_t& (1+ie_1)I_t\end{array}\right].$$
(44)
In particular, if $`m=n,`$ then (43) becomes a universal similarity factorization equality over $`𝒞_2.`$

According to (43), we define the complex representation of a matrix $`A=A_0+A_1e𝒞_2^{m\times n}`$ by $`\mathrm{\Phi }_2(A)=\left[\begin{array}{cc}A_0+A_1i& (A_2+A_3i)\\ A_2A_3i& A_0A_1i\end{array}\right].`$ Then the following properties are easy to verify by (43).

Corollary 11. Let $`A,B𝒞_2^{m\times n},C𝒞_2^{n\times p},`$ and $`\lambda 𝒞`$ be given. Then

* $`A=B\mathrm{\Phi }_2(A)=\mathrm{\Phi }_2(B).`$
* $`\mathrm{\Phi }_2(A+B)=\mathrm{\Phi }_2(A)+\mathrm{\Phi }_2(B).`$
* $`\mathrm{\Phi }_2(AC)=\mathrm{\Phi }_2(A)\mathrm{\Phi }_2(C),\mathrm{\Phi }_2(\lambda A)=\lambda \mathrm{\Phi }_2(A),\mathrm{\Phi }_2(I_m)=I_{2m}.`$
* Let $`A=A_0+A_1e_1+A_2e_2+A_3e_{12}`$ and denote $`A^\mathrm{\#}=A_0^{}A_1^{}e_1A_2^{}e_2A_3^{}e_{12},`$ then $`\mathrm{\Phi }_2(A^\mathrm{\#})=\mathrm{\Phi }_2^{}(A),`$ the conjugate transpose of the complex matrix $`\mathrm{\Phi }_2(A).`$
* $`A=\frac{1}{4}[(1ie_1)I_m,(e_2+ie_{12})I_m]\mathrm{\Phi }_2(A)[(1ie_1)I_n,(e_2+ie_{12})I_n]^T.`$
* $`A`$ is invertible $`\mathrm{\Phi }_2(A)`$ is invertible, in which case $`\mathrm{\Phi }_2(A^1)=\mathrm{\Phi }_2^1(A).`$
* $`p_A(A)=0,`$ where $`p_A(\lambda )=det[\lambda I_{2m}\mathrm{\Phi }_2(A)],`$ the characteristic polynomial of $`\mathrm{\Phi }_2(A).`$
* Two square matrices $`A`$ and $`B`$ are similar over $`𝒞_2,`$ i.e., there is an invertible matrix $`X`$ over $`𝒞_2`$ such that $`AX=XB`$ if and only if $`\mathrm{\Phi }_2(A)`$ and $`\mathrm{\Phi }_2(B)`$ are similar over $`𝒞.`$

In the next several results we only present the basic universal similarity factorization equalities without listing their operation properties and their extensions to matrices over $`𝒞_n.`$

Theorem 12. Let $`a𝒞_3=𝒞\{e_1,e_2,e_3\}`$ be given. Then $`a`$ can factor as

$$a=a_0+a_1e_{[3]},$$
(45)
where

$$a_0,a_1𝒞_2=𝒞\{e_1,e_2\},e_{[3]}^2=1.$$

Moreover, define $`\overline{a}=a_0a_1e_{[3]}.`$ In that case, the diagonal matrix $`D_a=\text{diag}(aI_2,\overline{a}I_2)`$ satisfies the following universal similarity factorization equality

$`P_3D_aP_3^1`$ $`=\left[\begin{array}{cc}\varphi _2(a_0)+\varphi _2(a_1)& 0\\ 0& \varphi _2(a_0)\varphi _2(a_1)\end{array}\right]`$ (48)
$`:=\varphi _3(a)^2𝒞^{2\times 2},`$ (49)
where $`\varphi _2(a_t),t=0,1,`$ is the matrix representation of $`a_t`$ in $`𝒞^{2\times 2}`$ defined in (38) and

$`P_3`$ $`={\displaystyle \frac{1}{2}}\left[\begin{array}{cc}(1+e_{[3]})P_2& (1e_{[3]})P_2\\ (1e_{[3]})P_2& (1+e_{[3]})P_2\end{array}\right],`$ (52)
$`P_3^1`$ $`={\displaystyle \frac{1}{2}}\left[\begin{array}{cc}P_2^1(1+e_{[3]})& P_2^1(1e_{[3]})\\ P_2^1(1e_{[3]})& P_2^1(1+e_{[3]})\end{array}\right],`$ (55)
where $`P_2`$ and $`P_2^1`$ are given by (37).

Proof. Notice that $`be_{[3]}=e_{[3]}b`$ holds for all $`b𝒞_2=𝒞\{e_1,e_2\}.`$ We have by applying (36) to $`a`$ in (45) that

$$P_2(aI_2)P_2^1=P_2(a_0I_2)P_2^1+P_2(a_1I_2)P_2^1e_{[3]}=\varphi _2(a_0)+\varphi _2(a_1)e_{[3]}:=\psi (a),$$

and

$$P_2(\overline{a}I_2)P_2^1=\varphi _2(a_0)\varphi _2(a_1)e_{[3]}:=\psi (\overline{a}).$$

Next we build, according to Lemma 1, a matrix and its inverse as follows

$`V`$ $`={\displaystyle \frac{1}{2}}\left[\begin{array}{cc}(1+e_{[3]})I_2& (1e_{[3]})I_2\\ (1e_{[3]})I_2& (1+e_{[3]})I_2\end{array}\right],`$ (58)
$`V^1`$ $`={\displaystyle \frac{1}{2}}\left[\begin{array}{cc}(1+e_{[3]})I_2& (1e_{[3]})I_2\\ (1e_{[3]})I_2& (1+e_{[3]})I_2\end{array}\right].`$ (61)
and then calculate to get

$$V\left[\begin{array}{cc}\psi (a)& 0\\ 0& \psi (\overline{a})\end{array}\right]V^1=\left[\begin{array}{cc}\varphi _2(a_0)+\varphi _2(a_1)& 0\\ 0& \varphi _2(a_0)\varphi _2(a_1)\end{array}\right].$$

Finally substituting $`\psi (a)=P_2(aI_2)P_2^1`$ and $`\psi (\overline{a})=P_2(\overline{a}I_2)P_2^1`$ into the left-hand side of the above equality yields (49), (52), and (55). $`\mathrm{}`$

Theorem 13. Let $`a𝒞_4=𝒞\{e_1,e_2,e_3,e_4\}`$ be given. Then $`a`$ can factor as

$$a=a_0+a_1e_{123}+a_2e_{124}+a_3e_{43}=a_0+e_{123}a_1+e_{124}a_2+e_{43}a_3,$$
(62)
where

$$a_0,a_1,a_2,a_3𝒞_2=𝒞\{e_1,e_2\},$$

$$e_{123}^2=1,e_{124}^2=1,e_{43}=e_{123}e_{124}=e_{124}e_{123}.$$

In that case, $`aI_4`$ satisfies the following universal similarity factorization equality

$`P_4(aI_4)P_4^1`$ $`=\left[\begin{array}{cc}\varphi _2(a_0)+\varphi _2(a_1)& \varphi _2(a_2)+\varphi _2(a_3)\\ \varphi _2(a_2)\varphi _2(a_3)& \varphi _2(a_0)\varphi _2(a_1)\end{array}\right]`$ (65)
$`:=\varphi _4(a)𝒞^{4\times 4},`$ (66)
where $`\varphi _2(a_t),t=0,\mathrm{},3,`$ is the matrix representation of $`a_t`$ in $`𝒞^{2\times 2}`$ defined in (38) and

$$P_4=P_4^1=\frac{1}{2}\left[\begin{array}{cc}(1+e_{[3]})P_2& (e_{124}e_{43})P_2\\ (e_{124}+e_{43})P_2& (1e_{[3]})P_2\end{array}\right],$$
(67)
where $`P_2`$ is given in (37).

Proof. Note that the commutative rules $`be_{123}=e_{123}b,be_{124}=e_{124}b,be_{43}=e_{43}b`$ hold for all $`b𝒞_2=𝒞\{e_1,e_2\}.`$ Thus, it follows from (36) that

$`P_2(aI_2)P_2^1`$
$`=P_2(a_0I_2)P_2^1+P_2(a_1I_2)P_2^1e_{123}+P_2(a_2I_2)P_2^1e_{124}+P_2(a_3I_2)P_2^1e_{43}`$
$`=\varphi _2(a_0)+\varphi _2(a_1)e_{123}+\varphi _2(a_2)e_{124}+\varphi _2(a_3)e_{43}`$
$`:=\psi (a).`$
Next building, according to Lemma 3, a matrix and its inverse as follows

$$V=V^1=\frac{1}{2}\left[\begin{array}{cc}(1+e_{123})I_2& (e_{124}e_{43})I_2\\ (e_{124}+e_{43})I_2& (1e_{123})I_2\end{array}\right],$$

and applying them to $`\psi (a)`$ given above, we obtain

$$V\left[\begin{array}{cc}\psi (a)& 0\\ 0& \psi (a)\end{array}\right]V^1=\left[\begin{array}{cc}\varphi _2(a_0)+\varphi _2(a_1)& \varphi _2(a_2)+\varphi _2(a_3)\\ \varphi _2(a_2)\varphi _2(a_3)& \varphi _2(a_0)\varphi _2(a_1)\end{array}\right].$$

Finally substituting $`\psi (a)=P_2(aI_2)P_2^1`$ into its left-hand side yields (66) and (67). $`\mathrm{}`$

By induction, we have the following two general results.

Theorem 14. Suppose that there is an independent invertible matrix $`P_n`$ over $`𝒞_n=𝒞\{e_1,\mathrm{},e_n\}`$ with $`n`$ even such that

$$P_n(aI_{2^{\frac{n}{2}}})P_n^1:=\varphi _n(a)𝒞^{2^{\frac{n}{2}}\times 2^{\frac{n}{2}}}=𝒞(2^{\frac{n}{2}})$$
(68)
holds for all $`a𝒞_n.`$ Now let $`a𝒞_{n+1}=𝒞\{e_1,\mathrm{},e_{n+1}\}.`$ Then $`a`$ can factor as

$$a=a_0+a_1e_{[n+1]}=a_0+e_{[n+1]}a_1,$$
(69)
where

$$a_0,a_1𝒞_n=𝒞\{e_1,\mathrm{},e_n\},e_{[n+1]}^2=(1)^{\frac{1}{2}(n+1)(n+2)}:=r.$$

Moreover define $`\overline{a}=a_0a_1e_{[n+1]}.`$ In that case, $`D_a=\text{diag}(aI_{2^{\frac{n}{2}}},\overline{a}I_{2^{\frac{n}{2}}})`$ satisfies the following universal similarity factorization equality

$`P_{n+1}D_aP_{n+1}^1`$ $`=\left[\begin{array}{cc}\varphi _n(a_0)+\sqrt{r}\varphi _n(a_1)& 0\\ 0& \varphi _n(a_0)\sqrt{r}\varphi _n(a_1)\end{array}\right]`$ (72)
$`:=\varphi _{n+1}(a)^2𝒞(2^{\frac{n}{2}}),`$ (73)
where

$$P_{n+1}=\frac{1}{2}\left[\begin{array}{cc}(1+\frac{1}{\sqrt{r}}e_{[n+1]})P_n& (\sqrt{r}e_{[n+1]})P_n\\ \frac{1}{r}(\sqrt{r}e_{[n+1]})P_n& (1+\frac{1}{\sqrt{r}}e_{[n+1]})P_n\end{array}\right],$$
(74)
and

$$P_{n+1}^1=\frac{1}{2}\left[\begin{array}{cc}P_n^1(1+\frac{1}{\sqrt{r}}e_{[n+1]})& P_n^1(\sqrt{r}e_{[n+1]})\\ P_n^1\frac{1}{r}(\sqrt{r}e_{[n+1]})& P_n^1(1+\frac{1}{\sqrt{r}}e_{[n+1]})\end{array}\right].$$
(75)
Proof. Note that the commutative rule $`be_{[n+1]}=e_{[n+1]}b`$ holds for all $`b𝒞_n=𝒞\{e_1,\mathrm{},e_n\}.`$ By applying (68) to (69), we obtain

$`P_n(aI_{2^{\frac{n}{2}}})P_n^1`$ $`=P_n(aI_{2^{\frac{n}{2}}})P_n^1+P_n(a_1I_{2^{\frac{n}{2}}})P_n^1e_{[n+1]}`$
$`=\varphi _n(a_0)+\varphi _n(a_1)e_{[n+1]}:=\psi (a).`$
and

$$P_n(\overline{a}I_{2^{\frac{n}{2}}})P_n^1=\varphi _n(a_0)\varphi _n(a_1)e_{[n+1]}:=\psi (\overline{a}).$$

Next, setting

$$V=\frac{1}{2}\left[\begin{array}{cc}(1+\frac{1}{\sqrt{r}}e_{[n+1]})I_{2^{\frac{n}{2}}}& (\sqrt{r}e_{[n+1]})I_{2^{\frac{n}{2}}}\\ \frac{1}{\sqrt{r}}(\sqrt{r}e_{[n+1]})I_{2^{\frac{n}{2}}}& (1+\frac{1}{\sqrt{r}}e_{[n+1]})I_{2^{\frac{n}{2}}}\end{array}\right],$$

$$V^1=\frac{1}{2}\left[\begin{array}{cc}(1+\frac{1}{\sqrt{r}}e_{[n+1]})I_{2^{\frac{n}{2}}}& (\sqrt{r}e_{[n+1]})I_{2^{\frac{n}{2}}}\\ \frac{1}{r}(\sqrt{r}e_{[n+1]})I_{2^{\frac{n}{2}}}& (1+\frac{1}{\sqrt{r}}e_{[n+1]})I_{2^{\frac{n}{2}}}\end{array}\right],$$

and applying them to $`D_a=\text{diag}(\psi (a),\psi (\overline{a}))`$ we get

$$V\left[\begin{array}{cc}\psi (a)& 0\\ 0& \psi (\overline{a})\end{array}\right]=\left[\begin{array}{cc}\varphi _n(a_0)+\sqrt{r}\varphi _n(a_1)& 0\\ 0& \varphi _n(a_0)\sqrt{r}\varphi _n(a_1)\end{array}\right].$$

Finally, substituting $`\psi (a)=P_n(aI_{2^{\frac{n}{2}}})P_n^1`$ and $`\psi (\overline{a})=P_n(\overline{a}I_{2^{\frac{n}{2}}})P_n^1`$ into its left-hand side yields the desired results. $`\mathrm{}`$

Theorem 15. Suppose that there is an independent invertible matrix $`P_n`$ over $`𝒞_n=𝒞\{e_1,\mathrm{},e_n\}`$ with $`n`$ even such that

$$P_n(aI_{2^{\frac{n}{2}}})P_n^1:=\varphi _n(a)𝒞(2^{\frac{n}{2}})$$
(76)
holds for all $`a𝒞_n.`$ Now, let $`a𝒞_{n+2}=𝒞\{e_1,\mathrm{},e_{n+2}\}.`$ Then it can factor as

$$a=a_0+a_1e_{[n]}e_{n+1}+a_2e_{[n]}e_{n+2}+a_3\mu _{n+2},$$
(77)
where

$$a_0,a_1,a_2,a_3𝒞_n=𝒞\{e_1,\mathrm{},e_n\},$$

$$(e_{[n]}e_{n+1})^2=(e_{[n]}e_{n+2})^2=(1)^{\frac{1}{2}(n+1)(n+2)}=r,$$

$$\mu _{n+2}=(e_{[n]}e_{n+1})(e_{[n]}e_{n+2})=(e_{[n]}e_{n+2})(e_{[n]}e_{n+1}).$$

In that case, $`aI_{2^{\frac{n+1}{2}}}`$ satisfies the following universal similarity factorization equality

$`P_{n+2}(aI_{2^{\frac{n+1}{2}}})P_{n+2}^1`$ $`=\left[\begin{array}{cc}\varphi _n(a_0)+\sqrt{r}\varphi _n(a_1)& r[\varphi _n(a_2)+\sqrt{r}\varphi _n(a_3)]\\ \varphi _n(a_2)\sqrt{r}\varphi _n(a_3)& \varphi _n(a_0)\sqrt{r}\varphi _n(a_1)\end{array}\right]`$
$`:=\varphi _{n+2}(a)𝒞(2^{\frac{n+1}{2}}),`$
where

$$P_{n+2}=\frac{1}{2}\left[\begin{array}{cc}(1+\frac{1}{\sqrt{r}}e_{[n+1]})P_n& (e_{[n]}e_{n+2}\frac{1}{\sqrt{r}}\mu _{n+2})P_n\\ \frac{1}{r}(e_{[n]}e_{n+2}+\frac{1}{\sqrt{r}}\mu _{n+2})P_n& (1\frac{1}{\sqrt{r}}e_{[n+1]})P_n\end{array}\right],$$

$$P_{n+2}^1=\frac{1}{2}\left[\begin{array}{cc}P_n^1(1+\frac{1}{\sqrt{r}}e_{[n+1]})& P_n^1(e_{[n]}e_{n+2}\frac{1}{\sqrt{r}}\mu _{n+2})\\ P_n^1\frac{1}{r}(e_{[n]}e_{n+2}+\frac{1}{\sqrt{r}}\mu _{n+2})& P_n^1(1\frac{1}{\sqrt{r}}e_{[n+1]})\end{array}\right].$$

The proof of this result is analogous to that of Theorem 13, and is therefore omitted here.

## 3 Conclusions

In this article we have established a set of universal similarity factorization equalities for elements over the complex Clifford algebra $`𝒞_n.`$ These equalities reveal two basic facts about $`𝒞_n:`$

* Each element $`a`$ in $`𝒞_n`$ has a complex matrix representation $`\varphi _n(a).`$ Moreover, a diagonal matrix constructed by the element $`a`$ is uniformly similar to its complex matrix representation $`\varphi _n(a).`$
* Conversely, each element $`a`$ in $`𝒞_n`$ could be regarded as an eigenvalue of its complex representation matrix $`\varphi _n(a).`$ In other words, all complex matrices with the form $`\varphi _n(a)`$ can uniformly be diagonalized over $`𝒞_n.`$

Based on the above two facts, one easily see that almost all known results in complex matrix theory can be extended to complex Clifford algebras. On the other hand, some problems related to complex matrices can also transform to the problems related to Clifford numbers. One such a problem (see ) is concerning the exponential $`e^A`$ of a complex matrix $`A.`$ In fact, we can see from Theorems 14 and 15 that for any $`a𝒞_n,`$ there is

$$P_n(e^aI)P_n^1=e^{\varphi _n(a)},$$

or

$$P_n\text{diag}(e^aI,e^{\overline{a}}I)P_n^1=e^{\varphi _n(a)},$$

which implies that the exponential of a complex matrix $`\varphi _n(a)`$ can be determined by the exponential of its corresponding Clifford numbers.


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# Resonant tunnelling and quenching of tunnel splitting in Wess-Zumino nanospin systems

Recently, the oscillations of the level splitting of the nanospin systems with magnetic field along the hard axis has been studied by many authors theoretically and experimentally. This oscillation phenomenon is semiclassically understood as a result of the interference between instanton and anti-instanton in the Euclidean space. However, although this instanton method gives exact evaluation of the oscillation of the ground level splitting, it does not give a satisfactory explanation of how the quenching disappears at higher magnetic field and how higher level splitting behaves with magnetic field.

On the other hand, there have been many works about complex periodic orbit theory for the tunnelling systems. This theory is based on the extension of well-known periodic orbit theory by including tunneling paths going through energy barrier. The tunnelling path have a minimal Euclidean action with a given energy, so they can be regarded as a ’bounce’, ’instanton’, or ’periodic instanton’. The advantage of complex periodic orbit theory is that for tunnelling systems it gives energy levels and their splittings throughout whole energy range. It is worth while to see how the geometrical phase can be incorperated with the complex periodic orbit theory, because, to our knowledge, for the systems with geometrical phase the theory has not been applied so far.

The purpose of this Letter is to apply the complex periodic orbit theory to the nanospin system showing geometrical phase effect, and to give semiclassical explanation for the existence of the level-splitting oscillations at low magnetic field and the absence of the oscillations at higher magnetic field for excited states as well as ground state. As will be shown clearly, we find out that the mechanism of the disappearance of quenching is the exact cancellation of quenching with the divergence of resonant tunnelling, which is very novel feature not reported so far. This strong correlation between quenching and resonant tunnelling seems to be inherent property in Wess-Zumino tunnelling systems.

Let us start with the Hamiltonian of system with magnetic field along the hard axis,

$$=K_1S_z^2+K_2S_y^2g\mu _BHS_z,$$
(1)
where $`K_1`$ and $`K_2`$ are anisotropy coefficients with $`K_1>K_2`$, and $`g`$ and $`\mu _B`$ are the gyromagnetic ratio and the Bohr magneton, respectively. The effctive Euclidean action for this Hamiltonian is obtained by expressing it in $`(\theta ,\varphi )`$\- representation and integrating over $`\theta `$,

$$S_E=iS_W+S\sqrt{\lambda }𝑑\tau \left[\frac{1}{2}m(\varphi )\dot{\varphi }^2+V(\varphi )\right]$$
(2)
where $`S_W`$ denotes the Wess-Zumino term which is expressed as

$$S_W=S𝑑\tau \dot{\varphi }(1\frac{h}{1\lambda \mathrm{sin}^2\varphi }),$$
(3)
and the position dependent mass and effective potential are

$`m(\varphi )`$ $`=`$ $`{\displaystyle \frac{1}{1\lambda \mathrm{sin}^2\varphi }},`$ (4)
$`V(\varphi )`$ $`=`$ $`{\displaystyle \frac{1}{2}}\mathrm{sin}^2\varphi (1{\displaystyle \frac{h^2}{1\lambda \mathrm{sin}^2\varphi }}).`$ (5)
Here we put $`\lambda \frac{K_2}{K_1}`$ and $`h=\frac{H}{H_c}`$ with $`H_c\frac{2K_1S}{g\mu _B}`$. Note that the geometrical phase factor $`S_W`$ does not change under analytic continuation of Euclidean time into real time, i.e., $`\tau it`$. This means that one should consider the phase effect of $`S_W`$ for the path in real space in the same way as for the tunnelling path in the Euclidean space. This point of view is somewhat different from that of Ref. where only the phase effect of tunnelling path is taken. The lack of the contribution of real path to the phase effect has created unreasonable oscillation of level splitting with temperature.

Now, we apply complex periodic orbit theory to this effective Hamiltonian system with Wess-Zumino term. In the regime of $`h<h_11\lambda `$, as depicted in Fig. 1 (a), the potential shows a simple barrier between $`\varphi =0`$ and $`\pi `$. Let us first consider the energy range of $`E<E_b`$, $`E_b`$ being the energy of the barrier top. A periodic orbit starting from $`\varphi =\varphi _1`$ can be considered as a combination of four elements; (tunnelling segment + tunnelling segment ), (real segment + real segment), (tunnelling segment + real segment), and (real segment + tunnelling segment). With a prescription for Maslov index for tunnelling segment in Ref., we can write semiclassical trace of Green’s function in terms of a periodic orbit sum as

$`g(E)`$ $`=`$ $`{\displaystyle \frac{T}{i}}{\displaystyle \underset{m=0}{\overset{1}{}}}{\displaystyle \underset{N=0}{\overset{\mathrm{}}{}}}[(e^{\theta +i\frac{\pi }{2}})^2+(e^{iWi\frac{\pi }{2}})^2`$ (6)
$`+`$ $`(e^{\theta +i\frac{\pi }{2}})(e^{iWi\frac{\pi }{2}})e^{i\alpha }e^{im\pi }`$ (7)
$`+`$ $`(e^{iWi\frac{\pi }{2}})(e^{\theta +i\frac{\pi }{2}})e^{i\alpha }e^{im\pi }]^N`$ (8)
where $`T`$ is the period of the real orbit in the well, $`W`$ is the action for the real segment, i.e., $`W(E)=_{\varphi _1}^{\varphi _1}𝑑\varphi m(\varphi )\frac{d\varphi }{dt}`$, $`\theta `$ is the action for the tunnelling segment, i.e., $`\theta (E)=_{\varphi _1}^{\pi \varphi _1}𝑑\varphi m(\varphi )\frac{d\varphi }{d\tau }`$, and $`\alpha =S\pi (1\frac{h}{\sqrt{1\lambda }})`$ is the geometrical phase for an element corresponding to $`\pi `$ increment in $`\varphi `$ axis. The first two terms correspond to the elements (tunnelling segment + tunnelling segment) and (real segment + real segment), respectively. These elements represent oscillatory motions confined in the wells and barriers, which do not enclose $`z`$-axis and thus have no geometrical phase factor. While, the next two terms, (tunelling segment + real segment) and (real segment + tunnelling segment) represent half rotations in the direction of increasing $`\varphi `$ and decreasing $`\varphi `$, respectively, so that they have the geometrical phase factor $`e^{i\alpha }`$ or $`e^{i\alpha }`$ according to the rotation direction. The contributions of nonperiodic orbits ending at $`\varphi _1+\pi `$ in the combinations are removed by introducing $`m`$ sum. Using the same approximation as Ref., we can write the sum as

$$g(E)\underset{k}{}\frac{1}{E(E_k\pm \frac{2}{T}\mathrm{cos}\alpha e^\theta )}$$
(9)
where $`E_k`$ is the EBK(Einstein-Brillouin-Keller) energies determined by $`2W(E_k)=2\pi (k+1/2)`$, $`k`$ being integer, and $`T=\frac{d(2W)}{dE}`$. Since the poles of $`g(E)`$ indicate the eigenvalues of the system, we can see the oscillation of the energy splitting and the quenching fields are determined by $`\alpha (h)=\pi (n+1/2)`$, $`n`$ being integer. It is noted that these quenching fields do not shift in excited energy level splittings.

Now, consider the regime of $`h>h_1`$. In this case the barrier top becomes local mininum and then equivalent two barriers and new meta-stable well appear as shown in Fig. 1 (b). Eq.(9) is still valid in the energy range of $`E<E_m`$. Consider the energy range of $`E_m<E<E_b`$, $`E_m`$ being the local minimum energy. In this structure one can expect that the resonant tunnelling may happen due to the states in the meta-stable well. As will be shown below, however, the resonant tunnelling does not take place, since it compensates the quenching of the level splittings. As a result, there is no more oscillations of level splittings. The periodic orbit sum can be done simply if one attaches a small correction

$$\left(1\frac{e^{2\theta _m+i\pi }}{1e^{2iW_mi\pi }}\right)^1$$
(10)
to each segment and replace the contribution of tunnelling segment by

$$\frac{e^{2\theta _m+i\pi }e^{iW_mi\pi /2}}{1e^{2iW_mi\pi }}$$
(11)
where $`W_m(E)=_{\varphi _2}^{\pi \varphi _2}𝑑\varphi m(\varphi )\frac{d\varphi }{dt}`$ and $`\theta _m(E)=_{\varphi _1}^{\varphi _2}𝑑\varphi m(\varphi )\frac{d\varphi }{d\tau }`$. The small correction, Eq.(10), comes from the consideration of possible paths, leaving from $`\varphi _1`$ or $`\varphi _1+\pi `$ and returning back after some oscillatory motion in the meta-stable well, and their repetition between two segments. In fact, this small correction does not play any important role under the approximation used in getting the final $`g(E)`$. The contribution of the new tunnelling segment, Eq.(11), shows all possible oscillatory motions in the meta-stable well between two equivalent tunnelling subsegments. Then, the trace of Green’s function can be written approximately as

$$g(E)\underset{k}{}\frac{1}{E(E_k\pm \frac{1}{T}\frac{\mathrm{cos}\alpha }{\mathrm{cos}W_m}e^{2\theta _m})}$$
(12)
Here, it is noted that the geometrical phase effect $`\mathrm{cos}\alpha `$ is modulated by the action of meta-stable state. This effect is the main point in this Letter and will be discussed in detail soon. Note that in the limit $`EE_m`$, Eq.(12) gives smaller energy splittings than those given by Eq.(9), i.e., shows a discrepancy of factor 2. This fact leads to a discontinuity at $`E=E_m`$ in energy splittings (see Fig.3). To remove this discrepancy at $`E=E_m`$, one should use an uniform approximation which may also give a smooth behavior near $`E_b`$ as well as near $`E_m`$. However, we do not use the uniform approximation because the simple complex periodic orbit theory used here is sufficient for our purpose of this Letter.

If the energy is larger than $`E_b`$, the particle motion is simple rotation and the poles of the trace of Green’s function appear when

$$S_{rot}(E)\pm 2\alpha =2\pi k,k=integer,$$
(13)
where the action $`S_{rot}(E)=_0^{2\pi }𝑑\varphi m(\varphi )\frac{d\varphi }{dt}`$ and this condition gives EBK energies $`E_k`$ for $`E>E_b`$. In this energy range the energy splitting does not come from tunnelling, but rather from the Zeeman effect. Indeed, this simple semicalssical evalution of EBK energies gives exact eigenvalues for uniaxial spin system of $`=S_z^2HS_z`$ which is not a tunnelling system but an example of simple rotational orbit. In this uniaxial spin system the mass is $`1/2`$, the potential is $`H^2/4`$, and $`\alpha =\pi (SH/2)`$, and then from Eq.(13) the EBK energies is given as $`E_k=k^2kH`$ where $`k`$ is integer or half integer according to the spinvalue $`S`$.

All actions, $`W(E)`$, $`\theta (E)`$, $`W_m(E)`$, $`\theta _m(E)`$, and $`S_{rot}(E)`$ are analytically calculated by the complete elliptic integrals of the first and third kind (see Table 1).

In Fig.2 (a) the whole energy spectrum with $`h`$ are shown for $`S=10`$ case. The solid line and the dashed line denote the barrier energy $`E_b`$ and the local minimum energy $`E_m`$, respectively, with $`h`$. In order to avoid complicated view, we draw only EBK energies for $`E<E_b`$ without showing the splitting of the EBK energies. For the comparison we draw the result of direct diagonalization for the same system. In this direct numerical calculation we take the energy such that $`E=0`$ at the well minimum. In fact, the effective potential in Eq.(5) has been derived after the same energy translation. We can see that the entire behaviour of energy spectrum with $`h`$ is very similar to the result of direct diagonalization except for the region of $`EE_b`$. As mentioned before, an uniform approximation would give a consistent explanation for this transition region. In our semiclassical evaluation of the energy spectrum the physics in the energy range of $`E>E_b`$ is very different from that in the range of $`E<E_b`$; the former is the Zeeman splitting and the latter is tunnelling splitting. However, in quantum mechanical result these seem to be mixed around $`EE_b`$ and no abrupt change at $`E=E_b`$ is shown.

Fig.3 shows the lowest three level splittings, $`\mathrm{\Delta }E_0`$, $`\mathrm{\Delta }E_1`$, and $`\mathrm{\Delta }E_2`$. Here, the solid lines describe the results of complex periodic orbit theory($`\mathrm{\Delta }E_i^s`$), while the dashed lines show the result of direct diagonalization($`\mathrm{\Delta }E_i^q`$). It should be emphasized that in the evaluation of the actions related to tunnelling segment, i.e., $`\theta (E)`$, $`W_m(E)`$, and $`\theta _m(E)`$, the energy value used is not the EBK energies $`E_k`$, but $`E_k^{}`$ determined from the condition $`2W(E_k^{})=2\pi k`$. This choice of energy is consistent with usual instanton method where the ground state splitting is represented in terms of Euclidean action at the well minimum energy $`E_{min}`$(action of instanton) instead of that at the ground state energy $`E_0`$. The discrepancies between the quantal results ($`\mathrm{\Delta }E_i^q`$) and the semiclassical results ($`\mathrm{\Delta }E_i^s`$) would be resolved provided that the quantum fluctuations around the tunnelling path are taken into account. It is very interesting to see that the quenching of the level splitting does not exist at higher $`h`$, and for $`\mathrm{\Delta }E_0`$ the number of quenching is $`S`$ and $`\mathrm{\Delta }E_i`$ has $`(Si)`$ quenchings in the range of $`0<h<1`$. This can be understood if one knows the role of $`\mathrm{cos}W_m`$ in Eq.(12). The factor $`1/\mathrm{cos}W_m`$ diverges at $`2W_m=2\pi (n+1/2)`$, $`n`$ being integer, showing the resonant tunnelling, which means that if $`E_k^{}`$ coincides with the EBK energy $`E_j^{meta}`$ in the meta-stable well the level splitting becomes divergent. The fact that in the range of $`E_m<E_i<E_b`$ the splittings $`\mathrm{\Delta }E_i`$ $`(i=0,1,2,3)`$ do not show any quenching and any resonant tunnelling implies that the quenching fields are same with those of resonant tunnelling. This exact coincidences are shown in Fig. 4. The dashed lines denote the EBK energies in the meta-stable well, $`E_j^{meta}`$. Note that the cross points with $`E_0^{}(=0)`$, $`E_1^{}`$, and $`E_2^{}`$ (the fields of resonant tunnelling) are located exactly on quenching fields given by the condition $`\mathrm{cos}\alpha (h)=0`$, which is the mechanism for the disappearance of the level-splitting oscillation.

In conclusion we examine the energy spectrum of the quantum tunnelling Wess-Zumino spin system by means of the complex periodic orbit theory. All important features in the spectrum can be understood within this semiclassical scheme. Especially, we find out that the absence of the oscillation of the level splittings at higher magnetic field has its physical origin in the exact cancellation of quenching with the resonant tunnelling phenomena. It is more reasonable to conclude that this cancellation is an inherent property of Wess-Zumino tunnelling system.

We thank Stephen Creagh and C.-H. Kim for useful discussions.


text:
# EXAFS indication of double-well potential for oxygen vibration in Ba1-xKxBiO3

## I Introduction

Though superconductivity in BaPb1-xBixO3 (BPBO) was discovered significantly earlier  than in cuprates, the question of the nature of superconducting state in this oxide as well as in cognate system Ba1-xKxBiO3 (BKBO) is still unsolved.

The structures of crystal lattice of copper oxide high temperature superconductors (HTSC’s) and bismuth-based oxides have some important common characteristics. The both oxide classes have perovskite-like lattice with CuOn ($`n`$=4, 5, 6) or Bi(Pb)O6 complexes joined by the common oxygen ions. In bismuthates, the intersection of octahedral complexes in the three crystallographic directions determines their three-dimensional cubic structure. The CuOn complexes are joined in CuO2 planes, which makes the two-dimensional structure of copper-oxides.

Because of strong hybridisation of covalent Bi(Pb)$`6s`$, Cu$`3d`$ – O$`2p_\sigma `$ bonds, the above mentioned complexes are the most tightly bound items of the perovskite-like structure. Therefore such important peculiarities of perovskite structure as lattice instability in respect to soft tilting mode of CuOn or BiO6 complexes (see for review ) and highly anisotropic thermal factors of oxygen ions vibration , which point out the large amplitude of rotation oscillations, are inherent to the both classes of superconducting oxides and cause anharmonic vibrations of oxygen atoms that may be described by movement in a double-well potential . These structural instabilities of perovskite-like lattice can be related with the transition to superconducting state .

The layered structure of copper oxide compounds, presence of several non-equivalent copper positions, and a number of different Cu-O bonds complicate the local structure analysis. At the same time, the simplicity of cubic three-dimensional structure of BPBO-BKBO systems makes the interpretation of experimental data easier to a great extent. Relatively low temperatures of superconducting transition $`T_c13`$ K in BaPb0.75Bi0.25O3  and $`T_c30`$ K in Ba0.6K0.4BiO3 , the values of superconducting gap $`2\mathrm{\Delta }(0)/kT_c=3.6\pm 0.1`$ for BPBO  and $`2\mathrm{\Delta }(0)/kT_c=3.5\pm 0.5`$ for BKBO , and a sizeable oxygen isotope effect  allow one to rely on standard BCS-theory of superconductivity, not excluding a possible realisation of other mechanisms. The simpler electronic structure of $`sp`$ valence band of BPBO-BKBO systems in comparison with $`dp`$ band of cuprates favours the establishment of relationship of crystal and electronic structures in these compounds.

However, even for these relatively simple systems there is no agreement so far on a number of crucial aspects: crystal structure symmetry and lattice dynamics , electronic structure , bismuth valence state . The most part of unusual properties of BaBiO3-family compounds mentioned in early review  are still unexplained.

In addition, the average structural data contradicts the local ones. Integral crystallographic methods point to the simple cubic lattice in BKBO ($`x>0.37`$) . In contrast to this, the EXAFS-analysis of four nearest spheres of bismuth environment  reveals a local tilting of octahedra by 4–5, and Raman spectra evidence for a local lowering of symmetry from simple cubic .

EXAFS-analysis of the nearest oxygen octahedral environment of Bi in metallic BKBO compound with $`x=0.4`$ previously was made in harmonic approach  and pointed out at least one unresolved problem. Temperature dependence of Debye-Waller factor $`\sigma ^2(T)`$ found by Heald et al.  can be described in Einstein approximation, which is suitable for harmonic systems, only if one takes into account the temperature independent factor of 0.0025 Å2. The attempt to explain this fact due to some static disorder with doping was denied since $`\sigma ^2(T)`$ of the next Bi-Ba and Bi-Bi shells show the absence of any disorder. Similar weakly varying $`\sigma ^2(T)`$ dependence was found in . Thus, it was observed that amplitude of low temperature Bi-O vibrations in metallic BKBO compound with $`x=0.4`$ is too high (more than twice larger than in metallic BaPbO3 compound) .

Besides, our careful measurements  of temperature dependent EXAFS-spectra of undoped BaBiO3 which were also treated in harmonic approach showed absolutely abnormal increasing of $`\sigma ^2`$ values of both Bi-O bonds with temperature decreasing from 90 K. We explained these anomalies by the influence of anharmonic rotational vibrations of oxygen octahedra which become pronounced at low temperatures , the model of connection of superconductivity with rotation mode asymmetry was proposed .

The above contradictions in description for local structure lead us to necessity of EXAFS analysis of the nearest Bi-O shell in anharmonic approach.

In the present paper we report the results of temperature dependent EXAFS-investigation of BPBO-BKBO systems firstly treated in anharmonic approach based on the idea of such an analysis for apical oxygen atoms in YBa2Cu3O7-δ proposed by J. Mustre de Leon et al.  We have analysed EXAFS function $`\chi (k)`$, using the new program “VIPER for Windows” , by construction of the model potentials of atomic vibrations, subsequent calculation of the pair radial distribution function, and calculation of the model $`\chi (k)`$. This new approach for the EXAFS-analysis of Bi-based oxides gives us an opportunity to investigate the character of oxygen atom vibrations and, in combination with our previous local electronic structure studies by XANES (x-ray absorption near edge structure) spectroscopy , to understand the nature of the structural phase transitions in these systems and to explain practically all above contradictions.

In Sec. II we describe the experimental details and present the procedure of data treatment. The general results are given in Sec. III. In Sec. IV we relate the local crystal structure with local electronic structure, which is the base of our processing of experimental data. In Sec. V we discuss the possible superconductive mechanism and demonstrate how the oscillations of oxygen atoms in double-well potential contributes to superconductivity in BKBO.

## II Experimental and data analysis

In this work we have investigated ceramic samples of BaPbO3 and BKBO with $`x=`$ 0, 0.4, 0.5 synthesised as described in . The materials were examined by x-ray powder diffraction for phase purity. The samples were controlled by transport and susceptibility measurements. BaBiO3 showed semiconductor-like behaviour, the compositions BKBO with $`x=0.4`$ and 0.5 showed typical metallic $`\rho (T)`$ dependence and superconducting properties with $`T_c30`$ K and $`T_c16`$ K, correspondingly. BaPbO3 samples were metallic but not superconducting at all temperatures.

For the XAS measurements, a crushed fine powder was precipitated onto a micropore substrate. The thickness of samples was about two absorption lengths at the chosen absorption edge.

The x-ray absorption spectra were collected at D-21 line (XAS-13) of DCI (LURE,Orsay, France) synchrotron operated at energy 1.85 GeV and the average current $`250`$ mA of positron beam at the $`L_3`$ edges of Bi (13040.6 eV) and Pb (13426 eV). Energy resolution of the double-crystal Si  monochromator (detuned to reject 50% of the incident signal in order to minimise harmonic contamination) with a 0.4 mm slit at 13 keV was about 2–3 eV. The low temperature measurements were carried out using a liquid helium circulation type cryostat with a temperature control of $`\pm 1`$ K.

The background in the experimental spectra was removed as described in , taking care to remove the low frequency oscillations. EXAFS-functions $`\chi (k)k^2`$ obtained from absorption spectra were Fourier transformed in the wave number range $`k`$ from 1.5 to 16.5 Å-1, using Kaiser-Bessel windowing function. Back Fourier transform was done using a Hanning window from $`1`$ to $`2`$ Å corresponding to the first Bi-O near-neighbour shell. In such a case, the number of independent experimental points  was $`N_{exp}=2\mathrm{\Delta }k\mathrm{\Delta }r/\pi +211`$.

The model EXAFS-function for pair atomic absorber-scatterer oscillations is constructed as follows. Suppose we know the potential of these oscillations as a parametric function of interatomic distance. Solving the stationary Srödinger equation for the particle with reduced mass of the atomic pair , one obtains a pair radial distribution function (PRDF) of atoms in $`i`$-th sphere:

$$g_i(r)=N_i\underset{n}{}|\mathrm{\Psi }_n(r)|^2e^{E_n/kT}/\underset{n}{}e^{E_n/kT},$$
(1)
where $`N_i`$ is the coordination number, $`E_n`$ and $`\mathrm{\Psi }_n`$ are $`n`$-th energy level and its corresponding wave function. Given PRDF’s, the model EXAFS function calculated as

$$\chi (k)=\frac{1}{k}\underset{i}{}F_i(k)\underset{r_{min}}{\overset{r_{max}}{}}g_i(r)\mathrm{sin}[2kr+\varphi _i(k)]/r^2𝑑r,$$
(2)
where $`k=\sqrt{2m_e/\mathrm{}^2(EE_{th})}`$ is the photoelectron wave number referenced to the ionisation threshold $`E_{th}`$, $`r_{min}`$ and $`r_{max}`$ are determined by the windowing function of back Fourier transform. The phase shift $`\varphi _i(k)`$ and scattering amplitude $`F_i(k)`$ were calculated using FEFF-6 code  for six-shell cluster with crystallographic data from neutron diffraction study  and using default set of the FEFF-6 parameters. The potential parameters were extracted from the model-to-experimental EXAFS-function fits.

## III General results

In Fig. 1 (left) we show the experimental $`\chi (k)k^2`$ for BKBO x=0, 0.4, 0.5 and for BaPbO3 measured at $`L_3`$ Bi(Pb) absorption edge at 7 K. Good signal-to-noise ratio seen even for maximal wave number values $`k16`$ Å-1 indicates the high spectra quality. The absence of signal on the Fourier transform in the low-$`r`$ range Fig. 1 (right) testifies for correct background removal procedure.

### A BaBiO3

EXAFS-researches  of BaBiO3 confirm the results of crystallographic works . According to them, there exist two inequivalent bismuth positions characterised by two Bi-O bond lengths. The equality of coordination numbers of the two BiO6 spheres points out that the BaBiO3 structure represents the ordered alternation of small and large BiO6 octahedra in barium lattice. Such an alternation together with static rotation distortion around  axis produce the monoclinic distortion of cubic lattice  (Fig. 2). As will be shown in Sec. IV, to the larger soft octahedra corresponds the configuration BiO6, and to the smaller rigid octahedra corresponds BiL2O6. Here, L2 denotes the hole pair in antibonding Bi$`6s`$O$`2p_\sigma ^{}`$ orbital of the octahedral complex.

In Fig. 3(a) the experimental $`\chi (k)k^2`$ EXAFS for BaBiO3 at 7 K for the first Bi-O near-neighbour shell is shown. The pronounced beating near 8 Å-1 evidences for existence of at least two different lengths of Bi-O bonds. In all previous EXAFS-researches  the EXAFS-function was quite successfully fitted in harmonic approximation as a sum of two independent harmonic functions with different bond lengths and Debye-Waller factors. However, temperature dependencies of Debye-Waller factors contradict to the harmonic Einstein model . This argues against the independence of oxygen atom vibrations in two neighbouring octahedra.

In this work, we model the oscillatory Bi-O potential as follows. Inequivalence of the two types of BiO6 octahedra is due to presence or absence of a hole pair in the hybridised molecular orbitals Bi$`6s`$O$`2p_\sigma ^{}`$ (see Sec. IV). Suppose, the movement of oxygen atoms may transfer a hole pair from one octahedron to another. Such a movement exchanges the roles of two inequivalent octahedra and requires a double-well form of oscillatory Bi-O potential. Here, we take a parabolic form of each well $`U_1=\kappa _1(rr_1)^2/2`$ and $`U_2=\kappa _2(rr_2)^2/2`$ which are joined continuously. Given the calculated $`\chi (k)`$, defined by Eqs. (1) and (2), we perform a least-squares fit between the model and experimental $`\chi (k)`$ over the range $`k=`$ 2–16 Å-1 (see Fig. 3(a)). The six parameters determined by the fit were $`E_{th}`$, $`r_1`$, $`r_2`$, $`\kappa _1`$, $`\kappa _2`$, and $`N`$. The number of parameters here is the same as for fitting in the harmonic approximation.

The analysis of parameters of double-well potential allows one to draw the following conclusions on the oscillations of oxygen atoms in BaBiO3. (i) At low temperatures there exist two explicit peaks on PRDF, that is why x-ray and neutron diffraction detect the static distortions in BaBiO3. (ii) Even at low temperatures, the tunnelling probability between the two wells is non-zero. As it will be discussed in Sec. IV, such a tunnelling is equivalent to the dynamic exchange BiL2O$`{}_{6}{}^{}`$ BiO6 and explains observed activation conductivity in BaBiO3. (iii) The temperature rise leads to gradual increase of probability of interwell tunnelling and to the structural transition to cubic phase found at 750–800 K . (iv) Non-equidistance of energy levels implies that oscillations of breathing- or stretching types with several frequencies exist: $`\omega _0=E_1E_0`$, $`\omega _1=E_2E_0`$, $`\omega _2=E_3E_0`$, etc. The latter are gradually manifested at high temperatures. (v) The positions of minima of double-well potential in our model are the average positions. They are spaced widely at maximal octahedra tilting and spaced closely at minimal octahedra tilting. In the latter case the probability of interwell tunnelling is maximal. In this sense the tunnelling frequency $`\omega _0`$ is bounded by soft rotation mode frequency.

### B BaPbO3

The experimental $`\chi (k)k^2`$ EXAFS for BaPbO3 for the first Pb-O near-neighbour shell at all temperatures represents a sinusoid with no beatings and phase breaks (Fig. 4) and fitted well, using a single parabolic potential. This means that all Pb-O bonds in BaPbO3 are equivalent and the breathing-type distortion is absent.

### C Ba1-xKxBiO3

The experimental $`\chi (k)k^2`$ EXAFS function for BKBO ($`x=0.4`$) at 7 K for the first Bi-O near-neighbour shell is shown in Fig. 5(a), solid curve. Also, the model calculated in harmonic approach (as in ) is shown as a dash-dot curve. It is seen that in the range $`k12`$ Å-1 the harmonic approach fails. This argues for the anharmonic Bi-O vibration behaviour similar to BaBiO3 case also in superconducting compositions BKBO. To a possible tendency in the cubic superconducting materials towards the same type of distortions as in BaBiO3 was pointed earlier .

The K doping of BaBiO3 leads to partial replacement of the larger soft octahedra BiO6 by the smaller rigid octahedra BiL2O6 (see details in Sec. IV). This causes a decrease and disappearance of static breathing and tilting distortions, but keeps the different rigidities of Bi-O bonds. Hence, the movement of an oxygen atom depends on that to which neighbouring octahedra this atom belongs. If the neighbouring octahedra are different, the oxygen atom oscillates in double-well potential as in BaBiO3. If the octahedra are equal, the oxygen atom oscillates in single-parabolic potential as in BaPbO3 (see Fig. 6). The statistical weights of these two cases depend on the potassium content $`x`$, and are $`(1x)`$ and $`x`$, correspondingly. Here, the force constants of the two parabolas are assumed to be equal since their independent varying does not improve the fits, and the number of fitting parameters equals 7. The resulting model curve is presented in Fig. 5(a), dotted. It is seen from Fig. 5(b) that the total PRDF is unsplit, so it is not surprising that crystallographic measurements reveal the cubic structure  (e.g. at $`T=10`$ K $`a=4.2742(1)`$). Meanwhile, the first momentum of the radial distribution function derived from our model is in a good agreement with the diffraction data , which validates our calculated amplitudes and phases.

In this paragraph we address to the important question of statistical grounds for the choice among several possible models. Consider, first, the statistical chi-square function (labelled just like EXAFS-function, but this is the different value)

$$\chi ^2=\frac{N_{exp}}{M}\underset{i}{\overset{M}{}}\left(\frac{\chi _{exp}(k_i)\chi _{mod}(k_i)}{\epsilon _i}\right)^2,$$
(3)
where M is the number of data points in the fit, $`N_{exp}`$ was introduced above, $`\epsilon _i`$ are the individual errors in the experimental data points. The latter were calculated as average of $`\sqrt{1/I_0+1/I_t}`$, $`I_0`$ and $`I_t`$ being the intensities measured in the transmission EXAFS experiment. The $`\chi ^2`$ value must follow the $`\chi ^2`$ distribution law with degrees of freedom $`\nu =N_{exp}P`$, where $`P`$ is the number of parameters varied during the fit. That is $`\chi ^2`$ must be less than the critical value $`X_\nu ^c`$ of the $`\chi ^2`$ distribution with $`\nu `$ degrees of freedom and the confidence level $`c`$. For our model in Fig. 5(a) $`\nu _2=117=4`$ and $`\chi _2^2=5.3<X_4^{0.95}=9.5`$, but for single-Gaussian model $`\nu _1=114=7`$ and $`\chi _1^2=16.8>X_7^{0.95}=14.1`$. Thus, our model meets the $`\chi ^2`$-test while the simple harmonic model does not. It is quite natural that having increased the number of parameters we got decreased $`\chi ^2`$ value. But what the gain should be? The comparison between the two models can be performed on the basis of $`F`$-test. If the difference $`\chi _1^2\chi _2^2`$ is physically meaningful, not due to presence of the noise, that is if the simpler model cannot describe some features in principle, this difference must not follow the $`\chi ^2`$ distribution law with $`\nu _1\nu _2`$ degrees of freedom. Provided that $`\chi _2^2`$ follows the $`\chi ^2`$ distribution with $`\nu _2`$ degrees of freedom, the value $`F(\nu _1\nu _2,\nu _2)=(\chi _1^2/\chi _2^21)\nu _2/(\nu _1\nu _2)`$ must not follow Fisher’s $`F`$-distribution with $`\nu _1\nu _2`$ and $`\nu _2`$ degrees of freedom. That is $`F`$ must be greater than the critical value $`F_{\nu _1\nu _2,\nu _2}^c`$ of the $`F`$ distribution with $`\nu _1\nu _2`$ and $`\nu _2`$ degrees of freedom and the confidence level $`c`$. Comparing the two models in Fig. 5(a), we find $`F(3,4)=2.89`$, which is equal to $`F_{3,4}^{0.84}`$. Therefore, we can claim with 84% probability that we propose a better model than the simplest single-Gaussian.

The complete results for Bi(Pb) octahedral ($`N=6`$) oxygen environment in BaPbO3 and Ba1-xKxBiO3 with $`x=`$ 0, 0.4, 0.5 at various temperatures are listed in Table I. The uncertainties in the EXAFS distances and force constants are less than $`\pm 0.4\%`$ and $`\pm 50\%`$, respectively. (These increments cause an increase of less than $`10\%`$ in the value of misfit.) It is seen from Figs. 3 and 5 that, in general, the positions of potential minima are not equal to the positions of PRDF’s maxima. Because of that, among other parameters, we give the values of PRDF’s centers of gravity, i.e. values that can be defined crystallographically. For BaBiO3, the centers of gravity were calculated for the two peaks of PRDF separately.

The parameters of potentials were obtained through the fit and, of course, depend on the form of the model potentials. To elucidate this influence, we constructed the model EXAFS function, using the polynomial of degree four: $`U=\kappa (rr_0)^2/2+\xi (rr_0)^4+\kappa ^2/(16\xi )`$, where the last term is introduced to zero the minimum values (Fig. 7). The number of fitting parameters here is the same as for double-parabolic potential. It turned out, that for the both potential forms the mean frequencies of Bi-O oscillations are practically identical for all temperatures. Because of this, in the present work we use double-parabolic potentials with parameters of clear meaning (potential minima positions and force constants) rather than a polynomial potential with abstract coefficients. Since the model EXAFS function weakly depends on the shape and value of interwell energy barrier $`U_0`$, we can not determine the $`U_0`$ value from EXAFS measurements exactly.

It worth to notice that in the case of BaBiO3 the above model of oxygen vibrations has some limitation due to the existence of the static rotation (tilting) distortion $`11^{}`$. Thus, the distances observed from EXAFS spectra treatment are measured along Bi-O-Bi zigzag curve, but not along the Bi-Bi () direction as in BKBO. This may result in some difference between $`\kappa 1`$ and $`\kappa 2`$ values (see Fig. 3(b) and Table I) and some deviation of calculated frequency from real ones in BaBiO3.

## IV Relationship between the local crystal and local electronic structures

### A BaBiO3

The co-existence in BaBiO3 of two different types of octahedra with two different Bi-O bond lengths and strengths reflects the different electronic structures of BiO6 complexes.

Octahedral complexes represent the most tightly bound items of the perovskite-like structures because of strong covalence of Bi$`6s`$-O$`2p_\sigma `$ bonds. The valence band structure of BaBiO3 is determined by overlapping of Bi$`6s`$ and O$`2p`$ orbitals , and, owing to strong Bi$`6s`$-O$`2p_\sigma `$ hybridisation, the octahedra can be considered as quasi-molecular complexes . Each complex has ten electron levels consisting of a pair of bonding Bi$`6s`$-O$`2p_\sigma `$, six nonbonding O$`2p_\pi `$, and a pair of antibonding Bi$`6s`$O$`2p_\sigma ^{}`$ orbitals. A unit cell, which includes two octahedra, has 38 valence electrons (10 from two bismuth ions, 4 from two barium ions, and 24 from six oxygen atoms). However, the numbers of occupied states in the two octahedtral complexes are different: octahedron BiL2O6 carries 18 electrons and has one free level or a hole pair L2 in the upper antibonding Bi$`6s`$O$`2p_\sigma ^{}`$ orbital, in octahedron BiO6 with 20 electrons both antibonding orbitals are filled (Fig. 8). It is quite natural that BiL2O6 octahedra have stiff (quasi-molecular) Bi-O bonds and the smaller radius, and BiO6 octahedra represent non-stable molecules with filled antibonding orbitals and the larger radius. Because the sum of two nearest octahedra radii overcomes the lattice parameter $`a`$, the octahedral system must tilt around  axis, producing a monoclinic distortion in BaBiO3 (see Fig. 2).

The assumption of equal electron filling for nearest octahedra (BiL1O$`{}_{6}{}^{}+`$BiL1O6) contradicts to experiments, since in this case equal Bi-O bond lengths and local magnetic ordering should be observed.

Therefore our new scheme of bismuth disproportionation 2BiL1O$`{}_{6}{}^{}`$ BiL2O6+BiO6 is in full agreement with charge balance, presence of two types of octahedron complexes and absence of any local magnetic moment .

Because Ba2+ in perovskite-type lattice is bound by pure ionic bond, the electron density is concentrated mainly in octahedra volume $`V_0`$ . Hence, the energy of the highest occupied level $`E_f`$ is related to the octahedron radius $`R`$ and the number of valence electrons $`N`$ in a unit cell as

$$E_fh^2N^{2/3}/m_eV_0^{2/3}h^2N^{2/3}/m_eR^2,$$
(4)
where $`h`$ is the Planck’s constant, $`m_e`$ is the electron mass. This qualitative relation leaves out of account the deviation of Fermi surface from sphere . Nevertheless, the value of $`E_f`$, which transforms to the Fermi level $`E_F`$ at spatial overlapping of equal octahedra in the crystal, is in close connection with the octahedron radius and with the number of valence electrons.

According to expression (4), the local electronic structure is connected with the local crystal structure. In the left of Fig. 9(a), the case of hypothetical simple cubic structure of BaBiO3 is shown. Real monoclinic structure arises from combined breathing (alternating octahedra with different radii $`R`$) and rotation distortions, which, according to (4), leads to the lowering of the energy $`E_f`$ of the highest occupied Bi$`6s`$O$`2p_\sigma ^{}`$ orbital in BiO6 octahedron in comparison with energy $`E_h`$ of unoccupied Bi$`6s`$O$`2p_\sigma ^{}`$ orbital in BiL2O6 octahedron. Hence, the repetitive sequence of empty level $`E_h`$ on the background of fully filled valence band represents the electronic structure of the ground state of BaBiO3 (Fig. 9(a), right). In such a system there are no free carriers and conductivity occurs at hopping of carrier pair from one octahedron to another with the activation energy $`E_a=E_hE_f`$. In this process the movement of hole pair in real space leads to change of large octahedra to small ones and vice versa or to a dynamic exchange BiL2O$`{}_{6}{}^{}`$ BiO6, in full accordance with vibrations in double-well potential showed in Fig. 3, and causes the hole-type conductivity. In this case, the activation energy $`E_a`$ means the pair localisation energy.

This picture agrees with results of investigation of temperature dependencies of conductivity and Hall coefficient: $`n(T)=n_0\mathrm{exp}(E_a^{}/k_BT)`$ , where the value of hole concentration $`n_0=1.1\times 10^{22}`$ cm-3 coincides with the concentration of unit cells, and the activation energy $`E_a^{}=0.24`$ eV, if one takes into account that in the case of two-particle activation conductivity, the number of hole pairs is equal to the number of BiL2O6 complexes (concentration of which is half $`n_0`$), and the activation energy $`E_a=2E_a^{}=0.48`$ eV. It should be mentioned that the possibility of the two-particle (bipolaron) conductivity as a most probable mechanism of conductivity in BaBiO3 was pointed to earlier .

Pair splitting and hopping of a single electron from one octahedron to another cost energy and lead to electronic structure reconstruction of the both octahedral complexes. Such a splitting can be achieved under optical excitation, which was observed experimentally as a photoconductivity peak at the photon energy $`h\nu =1.9`$ eV . The optical gap $`E_g`$ is the energy difference between the excited and ground states. In the excited state, BaBiO3 has the local lattice of equivalent octahedra BiL1O6 and possesses the non-compensated spin. Admittedly, it must have anti-ferromagnetic ordering, as the ground state in undoped cuprates La2CuO4 and Nd2CuO4. Such optical excitation leads to the local dynamical lattice deformation observed in Raman spectra as a breathing mode $``$570 cm-1 of giant amplitude under resonant coinciding of photon energy of Ar+ laser with $`E_g`$ . Using lasers with other quantum energies destroys this resonant effect and leads to abrupt decrease of breathing mode amplitude .

Thus, the scheme proposed accounts for the nature of the two energy gaps in BaBiO3. The activation energy $`E_a`$ appears in transport measurements and is connected with coherent delocalisation of hole pairs owing to dynamic exchange BiL2O$`{}_{6}{}^{}`$ BiO6. The optical gap is radically differs from a traditional gap in semiconductors. It corresponds to energy difference between the excited and ground states.

### B BaPbO3

In BaPbO3, each octahedron also has ten molecular orbitals, nine of which are filled and one, antibonding Pb$`6s`$O$`2p_\sigma ^{}`$, is unoccupied as in octahedron BiL2O6, since lead has one electron less than bismuth. Thus, all the octahedral complexes represent the bound molecules PbL2O6 with equal radii. At spatial overlapping of PbL2O6 in crystal BaPbO3, wave functions of Pb$`6s`$O$`2p_\sigma ^{}`$ states become delocalised, unoccupied levels $`E_h`$ of neighbouring octahedra split into a free carrier band, and, merging with the top of valence band consisting of initially filled Pb$`6s`$O$`2p_\sigma ^{}`$ orbitals, make the half filled conduction band (Fig. 9(b)). It is important to notice that unoccupied Bi(Pb)$`6s`$O$`2p_\sigma ^{}`$ orbitals in the case of absence of spatial overlapping in BaBiO3 behave as localised hole pairs, but transform to the conduction band at the spatial overlapping in BaPbO3. Because of this, BaBiO3 appears to be a semiconductor of $`p`$-type, and BaPbO3 — a semimetal of $`n`$-type. Since the radius of PbL2O6 complex is slightly greater than that of BiL2O6 complex, the Fermi level $`E_F`$ in BaPbO3, according to expression (4), lies lower in comparison with $`E_f`$ in BaBiO3, which agrees with results of photoelectron spectroscopy .

Thus, the lead valence state PbL2O6 in BaPbO3 is similar to the bismuth state in BiL2O6 complexes in BaBiO3. According to Fig. 4, oxygen atoms in BaPbO3 oscillate in the parabolic potential without any exchange between equal PbL2O6 octahedra. Therefore, there is no charge pair transfer in semimetallic BaPbO3 and the itinerant electrons behave as usual Fermi liquid.

### C Ba1-xKxBiO3

The doping of BaBiO3 by lead or potassium leads to decrease of integral structural lattice distortions and causes essential changes in both local crystal and electronic systems. Firstly, we discuss the changes in electronic structure of BKBO as a simpler case, and then will extend the obtained conclusions to the BPBO system.

Since K+ ion has one valence electron instead of two of Ba2+ ion, the substitution of each two Ba2+ for two K+ ions produces an additional unoccupied level or hole pair in a Bi$`6s`$O$`2p_\sigma ^{}`$ orbital and modifies the BiO6 complex to the BiL2O6. As a result, the ratio of the numbers of BiL2O6 and BiO6 complexes changes from $`1:1`$ in BaBiO3 to $`(1+x):(1x)`$ and equals $`7:3`$ in Ba0.6K0.4BiO3 and $`3:1`$ in Ba0.5K0.5BiO3. The spatial overlapping of BiL2O6 complexes appear, which, taking into account their small radii and rigid bonds, contracts the lattice. This leads to decrease and disappearance (at $`x>0.37`$) of both static rotation- and breathing-type distortions. The lattice is forced to contract, despite the ionic radii of Ba2+ and K+ are practically equal.

Structural changes are accompanied by essential changes in physical properties of BKBO: at $`x0.37`$ the phase transition insulator-metal occurs and the superconductivity arises that remains up to the dopant concentration $`x=0.5`$ corresponding to the solubility limit of potassium in BaBiO3. The type of the temperature dependence of conductivity changes from semiconducting to metallic one, Hall coefficient changes its sign, and, in the normal state, BKBO compound with $`x>0.37`$ behaves as a metal with $`n`$-type conductivity .

These changes are well described in the framework of the above scheme (Fig. 9 for BKBO). At the low dopant amount ($`x<0.37`$), the contraction of the larger (soft) and the stretching of the smaller (rigid) octahedra bring, according to expression (4), $`E_h`$ and $`E_f`$ energies close together and the activation energy $`E_a=E_hE_f`$ decreases. As dopant concentration rises, the number of BiL2O6 octahedra increases, and at $`x>0.37`$, in the lattice arise the three-dimensional chains of spatially overlapped BiL2O6 octahedral complexes , their unoccupied levels split and form the conductivity band, which is equivalent to the percolation threshold reaching that determines the insulator-metal phase transition. Here, the itinerant electrons show Fermi liquid behaviour with Fermi level $`E_F`$ as in BaPbO3. However, in contrast to the picture in BaPbO3, in the BKBO structure there exist complexes BiO6 through which itinerant electrons can not move because all the levels in these complexes are occupied. The movement of electrons occupying the upper Bi$`6s`$O$`2p_\sigma ^{}`$ orbital is possible only in pairing state at the dynamic exchange BiL2O$`{}_{6}{}^{}`$ BiO6, since the unpairing costs energy consumption. But, in contrast to the case of BaBiO3, the static rotation- and breathing-type distortions of the octahedra disappear, their mean radii become approximately equal (and equal to half the lattice parameter), and the pair localisation energy approaches zero: $`E_a=E_hE_f0`$ (Fig. 9(d)). In this case, the delocalised carrier pairs can freely move through the octahedral system that explains the appearance of superconductivity in BKBO ($`x>0.37`$). This scheme of the local electronic structure is in full agreement with the picture of local oxygen vibration in double-well potential (see Figs.5,6,7).

The unpairing of electrons, as in BaBiO3, is possible under optical excitation and is manifested by a pseudo-gap observed in reflectivity spectra even in the metallic phase of BPBO-BKBO systems. For instance, in BKBO with $`x=0.4`$ the pseudo-gap is about 0.5 eV  and about 0.6 eV  in BPBO with $`x=0.25`$.

Our model suggests that in the metallic phase two carrier types are present: itinerant electrons and pairs of initially (in BaBiO3) localised carriers. The co-existence of the two carrier types was confirmed by experiments on investigation of conductivity, Hall effect, and thermoelectric power , as well as by photoemission spectra  and Raman spectra investigations . These results are in a good agreement with observed zero-bias conductance . The change in carriers behaviour from localised to itinerant at doping of BaBiO3 by potassium was pointed to in x-ray absorption spectra analysis at the O $`K`$ edge . The analysis of EPR spectra  showed the presence of the localised carrier pairs, which also was confirmed by the observation of two-particle tunnelling in the normal-state of BKBO .

### D BaPb1-xBixO3

Practically the same changes in electronic structure arise at the doping of BaBiO3 by lead. The electronic structure of octahedral PbL2O6 complex is entirely equivalent to that of BiL2O6 complex. Unoccupied levels of overlapping octahedra in BaPbO3 form the conduction band, as at overlapping of BiL2O6 in BKBO. At the doping of BaPbO3 by bismuth ($`0<x<0.37`$), the case is similar to BKBO ($`x>0.37`$). However, in BPBO the following combinations of neighbouring octahedra are possible: PbL2O6-PbL2O6, PbL2O6-BiL2O6, PbL2O6-BiO6, BiL2O6-BiO6. This leads to different local shifts of $`E_h`$ and $`E_f`$ energies, depending on different octahedra neighbouring pairs. At the further increase of bismuth content, the number of filled BiO6 octahedra rises, the tilting and breathing distortions enlarge, the pair localisation energy raises, the spatial overlapping of unoccupied levels in PbL2O6 octahedra disappears, which destroys the metallic type of conductivity and the system becomes a semiconductor with $`p`$-type conductivity.

Thus, superconductive properties of BPBO in our model are connected with dynamic exchange PbL2O$`{}_{6}{}^{}`$ BiO6. Unfortunately, it is practically impossible to observe the double-well-potential oxygen vibrations for superconducting BPBO compositions ($`0<x<0.35`$) by EXAFS study because of overlapping of Pb $`L_3`$ and Bi $`L_3`$ edges. Though an analysis of EXAFS spectra for these compounds is possible under elaborate treatment procedure , the precise enough values can be obtained only for interatomic distances, but not for amplitude factors. For this reason, we do not present the EXAFS data of BPBO ($`0<x<1`$) in this paper.

### E Photoemission spectra anomalies

The analysis of photoemission spectra has revealed a serious contradiction concerning the experimental observation of the splitting of the Bi$`4f`$(5/2, 7/2) spectral lines in superconducting compounds BKBO  at the absence of any peculiarities of those lines in parent BaBiO3 . The contradiction consists in that that though the analysis of x-ray diffraction and EXAFS data points to existence of two different Bi-O bonds in BaBiO3, no splitting of Bi$`4f`$ doublet lines was observed, which indicates the absence of considerable difference in bismuth valence states. The doping of BaBiO3 by potassium relieves the monoclinic distortion and equalises the Bi-O bond lengths up to $`a/2`$. However, the Bi$`4f`$ spectral lines become broaden  and, at measurements on a high resolution spectrometer, even split , which, in contrast with simple cubic lattice in BKBO ($`x>0.37`$), points to existence of two different bismuth valence states.

The above scheme of local electronic structure completely resolves this issue. Indeed, in BaBiO3 the binding energies of the Bi$`4f`$ core levels in different BiL2O6 and BiO6 octahedra are almost equal and hence, the Bi$`4f`$ doublet lines in photoemission spectra are unsplit (Fig. 10(a)). Contrary to that, in Ba0.6K0.4BiO3, the binding energies of the Bi$`4f`$ core levels in the different octahedra $`E_1^{}`$, $`E_2^{}`$ and $`E_1`$, $`E_2`$ differ on $`\mathrm{\Delta }E=E_hE_FE_a`$, which causes the broadening (see curve $`x=0.5`$ in Fig. 10(a) from  and splitting (see curve $`x=0.4`$ in Fig. 10(b) from  of the Bi$`4f`$ doublet lines. The value of the splitting coincides well with our estimation of $`E_a=0.48`$ eV, and the ratio of intensities $`I`$ of the core-level peaks corresponding to the binding energies in different octahedral complexes BiO6 and BiL2O6 is in accordance with the relative content of these complexes in Ba0.6K0.4BiO3: $`I(E_1^{})/I(E_1)I(E_2^{})/I(E_2)3/7`$.

## V On possible nature of superconducting state

Essentially anharmonic character of oxygen ion oscillations in soft rotation mode is the base of anharmonic model of the high temperature superconductivity . It was shown that anharmonic coupling constant $`\lambda _s`$ exceeds the constant in harmonic approach $`\lambda _{ph}`$:

$$\lambda _s/\lambda _{ph}J_s^2d^2\overline{\omega }/J_{ph}^2u^2\omega _s1,$$
(5)
which explains high critical temperatures in cuprate HTSC compounds as well as in BPBO-BKBO systems. Here, $`d`$ and $`\omega _s`$ are the amplitude and frequency of oscillation in a double-well potential, $`u^2`$ is the mean-square displacement of the ions with the mean frequency $`\overline{\omega }`$ in harmonic approach, $`J_{ph}^2`$ and $`J_s^2`$ are, respectively, the deformation potentials of harmonic and anharmonic oscillations averaged on the Fermi surface.

In that model, the oscillatory movement of oxygen ions in rotation mode with a large amplitude in the direction perpendicular to the Bi(Pb)-O bonds was considered. A considerable gain in value of the coupling constant in expression (5) is due to low frequency of soft rotation mode ($`\omega _s<\overline{\omega }`$) and the excess of its amplitude over amplitude of harmonic oscillations ($`d^2u^2`$).

Meanwhile, previous  as well as recent ( and references therein) electronic structure calculations showed that such a movement hardly affects the Bi-O bond lengths, keeping $`sp(\sigma )`$ nearest-neighbour interaction nearly constant. Thus, despite the existence of double-well potential in rotation (tilting) mode, Meregalli and Savrasov  obtained very small anharmonic contribution to $`\lambda `$. Also, they assumed the breathing-type oxygen vibrations to be harmonic with small amplitude and high frequency and found too small $`\lambda 0.3`$ to explain high $`T_c`$ in BKBO.

Our investigation firstly showed that in BKBO the double-well vibrations with strong deformation potential also exist along the Bi-O-Bi direction. Such vibrations have the breathing-like character and low frequency bounded by soft rotation mode. Thus, our results resolve the above issue and explain the reason for strong electron-phonon coupling in Bi-based oxides. Also, to these vibrations we can assign the low-frequency part, below 40 meV, of phonon density of states observed in neutron scattering for superconducting BKBO  and absent in calculations . Besides, the anomalous phonon softening along  direction  becomes clear due to our observation of coherent breathing-like vibrations along  axis.

Hardy and Flocken  evaluated values of $`\lambda `$, using abstract model double-well potentials:

$$\lambda (T)=N(0)\underset{kk^{}}{\overset{\mathrm{FS}}{}}\underset{n^{}>n}{}\frac{|n|M_{kk^{}}|n^{}|^2}{E_n^{}E_n}(f_nf_n^{}),$$
(6)
where $`N(0)`$ is the density of electron states at the Fermi level, $`M_{kk^{}}`$ is the e-ph matrix element between electronic states $`|k`$ and $`|k^{}`$ on the Fermi surface, $`|n`$ and $`|n^{}`$ are the oscillatory states with energies $`E_n`$ and $`E_n^{}`$, $`f_n`$ and $`f_n^{}`$ are the thermal weighting factors; $`f_n=\mathrm{exp}(E_n/kT)/_n^{}\mathrm{exp}(E_n^{}/kT)`$.

Given the oscillatory energies from our EXAFS-experiment, we have calculated $`\lambda `$ in terms of arbitrary multiplicative constant which is proportional to $`N(0)`$ and $`M_{kk^{}}`$ (Fig. 11). Although “phonon” part of $`\lambda `$ is the strongest for BaBiO3, this composition is not superconducting. On the one hand, because of pair localisation energy $`E_a`$. On the other, the rotation oscillations of rigid BiL2O6 octahedra and ordinary phonons (of stretching and bending types) differ in collective character of motion in BiO2 planes. In BaBiO3, rigid BiL2O6 octahedra are separated by soft BiO6 octahedra and are not spatially overlapped. The partial replacement of the larger soft octahedra by the smaller rigid ones at the potassium doping leads to decrease and disappearance of localisation energy $`E_a`$ (Fig. 9(c,d)) and to spatial coherence of rotation oscillations with length of several lattice parameters, depending on the doping level $`x`$. For superconducting compositions, $`T_c`$ means the temperature up to which $`\lambda `$ is considerably decreased (Fig. 11) and/or the coherence in oscillations of neighbouring octahedra is thermally destroyed by ordinary phonons.

The ground state of BaBiO3 can be considered as a bipolaronic state as well, and the movement of carrier pairs correlated with oxygen atoms oscillations at the dynamic exchange BiL2O$`{}_{6}{}^{}`$ BiO6 evidences for possible application of bipolaron theory , which is supported by the small size of the pair (octahedron size) and by the existence of the pair state above $`T_c`$.

## VI Conclusion

From the EXAFS investigation of BPBO-BKBO systems, the local crystal structure peculiarities connected with non-equivalence of BiL2O6-BiO6 octahedra were observed. It was found that oxygen vibrations are well described using double-well potentials, which leads to the strong electron-phonon coupling due to coherent modulation of Bi-O bond lengths with low frequency and causes correlated carrier pair movement with oxygen ions oscillations. The underlying relationship between the local crystal and local electronic structures was established that explains the full list of unusual properties of BPBO-BKBO systems: the existence of two energy gaps (transport $`E_a`$ and optical $`E_g`$) in BaBiO3; the mechanism of two-particle conductivity in BaBiO3; the co-existence of two different carrier types; pseudo-gap observation in metallic compositions of BKBO and BPBO; the observation of localised pairs from EPR spectra; the observation of low-frequency ($`<40`$ meV) phonons; the nature of concentration and temperature phase transitions; the contradictions between local (Raman, and EXAFS) and integral structural methods for metallic BKBO; the anomalies of XPS spectra in BaBiO3 and BKBO. We observed the correlated movement of carrier pairs and low-frequency breathing-like oxygen octahedra vibrations, which corresponds to superconducting state. The model proposed combines some principal features of the real-space pairing , anharmonic models  and bipolaron theory  of high-$`T_c`$ superconductivity.

The likeness of rotation mode peculiarities of BiO6 octahedra and CuOn complexes and the anomalies in temperature dependencies of Debye-Waller factors in cuprates  allow one to hope that similar model approach can be applied to the Cu-based superconductors.

###### Acknowledgements.

We acknowledge LURE Program Committee for beamtime providing, Professors S. Benazeth and J. Purans for help during x-ray absorption measurements. We are also grateful to Professor A. P. Rusakov for high-quality BKBO samples and to Dr. A. V. Kuznetsov and Dr. A. A. Ivanov for helpful discussions. The work is supported by RFBR (Grant No. 99-02-17343) and Program “Superconductivity” (Grant No. 99010).