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# Two-body tunnel transitions in a Mn4 Single-Molecule Magnet

## Abstract

The one-body tunnel picture of single-molecule magnets (SMMs) is not always sufficient to explain the measured tunnel transitions. An improvement to the picture is proposed by including also two-body tunnel transitions such as spin-spin cross-relaxation (SSCR) which are mediated by dipolar and weak superexchange interactions between molecules. A Mn4 SMM is used as a model system. At certain external fields, SSCRs lead to additional quantum resonances which show up in hysteresis loop measurements as well defined steps.

Single-molecule magnets (SMMs) are one of the best systems for studying quantum tunneling of large moments. Since SMMs occur as assemblies in crystals, there is the possibility of a small electronic interaction of adjacent molecules. This leads to very small superexchange interactions that depend strongly on the distance and the nonmagnetic atoms in the exchange pathway. Until now, such an intermolecular exchange interaction has been assumed to be negligibly small. However, our recent studies on about 50 SMMs suggest that in most SMMs exchange interactions lead to a significant influence on the tunnel process. Recently, this intermolecular exchange interaction was used to couple antiferromagnetically two SMMs, each acting as a bias on its neighbor, resulting in quantum behavior different from that of individual SMMs .

In this contribution, we show that dipolar and/or exchange interactions can lead to collective quantum processes. The one-body tunnel picture of SMMs is therefore not always sufficient to explain the measured tunnel transitions. We propose to improve the picture by including also two-body tunnel transitions such as spin-spin cross relaxation (SSCR) which are mediated by dipolar and weak superexchange interactions between molecules . We use here a different Mn4 SMM to show that at certain external fields SSCRs lead to additional quantum resonances which show up in hysteresis loop measurements as well-defined steps.

The single-crystal X-ray structure of

\[Mn4O3Cl(O2CCH3)3(dbm)3\] has been reported . It crystallizes in the monoclinic $`P2_1/n`$ space group with $`Z=4`$. The molecule has the trigonal pyramidal \[Mn$`{}_{}{}^{\mathrm{III}}{}_{3}{}^{}`$MnIVO3Cl\]6+ core. A virtual $`C_3`$ symmetry axis runs through the MnIV and Cl atoms and defines the magnetic z-axis of each molecule. The four molecules within a unit cell are canted at an angle of 8.97 with respect to one another. DC and AC magnetic susceptibility measurements indicate a well isolated $`S=9/2`$ ground state .

All measurements were performed using an array of micro-SQUIDs . The high sensitivity allows us to study single crystals of SMM.

Fig. 1 shows typical hysteresis loops for a single crystal of Mn4. When the applied field is near an avoided level crossing, the magnetization relaxes faster, yielding steps separated by plateaus. A closer examination of the tunnel transitions however shows fine structures which cannot be explained by the one-body tunnel picture (giant spin model). We suggest that these additional steps are due to a collective quantum process, called spin-spin cross-relaxation (SSCR), involving pairs of SMMs which are coupled by dipolar and/or exchange interactions. We used different techniques to show that different species due to loss of solvent or other defects are not the reason of the observed additional resonance transitions. Such SSCR processes were recently observed in the thermally activated regime of a LiYF4 single crystal doped with Ho ions  and on other Mn4 SMMs .

It is important to note that in reality a SMM is coupled to many other SMMs which in turn are coupled to many other SMMs. This represents a complicated many-body problem leading to quantum processes involving more than two SMMs. However, the more SMMs that are involved, the lower is the probability for occurrence. In the limit of small exchange couplings and transverse terms, we therefore consider only processes involving one or two SMMs. The mutual couplings between all SMMs should lead mainly to broadenings and small shifts of the observed quantum steps.

The question arises whether such transitions also play a role in other SMMs like Fe8 and Mn12. A diagonalization of the spin-Hamiltonian of such molecules shows clearly that SSCR should occur also. However, it turns out that these transitions are very close to the single spin tunnel transitions and only broaden them. Nevertheless, such transitions should be included in a quantitative description of the relaxation rates, in particular in the thermally activated regime or for high applied fields.


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# The shape of a tridiagonal pair11footnote 1 Keywords. Leonard pair, tridiagonal pair, Askey scheme, 𝑞-Racah polynomial, subconstituent algebra. 2000 Mathematics Subject Classification. Primary 17B37; Secondary 05E35, 15A21, 33C45, 33D45.

## 1 Introduction

Throughout this paper, $`𝕂`$ will denote a field and $`V`$ will denote a vector space over $`𝕂`$ with finite positive dimension. Let $`A:VV`$ denote a linear transformation and let $`W`$ denote a subspace of $`V`$. We call $`W`$ an eigenspace of $`A`$ whenever $`W0`$ and there exists $`\theta 𝕂`$ such that

$`W=\{vV|Av=\theta v\}.`$
We say $`A`$ is diagonalizable whenever $`V`$ is spanned by the eigenspaces of $`A`$.

We now recall the notion of a tridiagonal pair.

###### Definition 1.1

 By a tridiagonal pair on $`V`$, we mean an ordered pair $`A,A^{}`$ where $`A:VV`$ and $`A^{}:VV`$ are linear transformations which satisfy the following four conditions.

1. Each of $`A,A^{}`$ is diagonalizable.
2. There exists an ordering $`V_0,V_1,\mathrm{},V_d`$ of the eigenspaces of $`A`$ such that

$$A^{}V_iV_{i1}+V_i+V_{i+1}(0id),$$
(1)
where $`V_1=0`$, $`V_{d+1}=0`$.
3. There exists an ordering $`V_0^{},V_1^{},\mathrm{},V_\delta ^{}`$ of the eigenspaces of $`A^{}`$ such that

$$AV_i^{}V_{i1}^{}+V_i^{}+V_{i+1}^{}(0i\delta ),$$
(2)
where $`V_1^{}=0`$, $`V_{\delta +1}^{}=0`$.
4. There does not exist a subspace $`W`$ of $`V`$ such that $`AWW`$, $`A^{}WW`$, $`W0`$, $`WV`$.

###### Note 1.2

According to a common notational convention, $`A^{}`$ denotes the conjugate-transpose of $`A`$. We are not using this convention. In a tridiagonal pair $`A,A^{}`$ the linear transformations $`A`$ and $`A^{}`$ are arbitrary subject to (i)–(iv) above.

In order to motivate our results we recall a few facts about tridiagonal pairs. Let $`A,A^{}`$ denote a tridiagonal pair on $`V`$ and let the integers $`d,\delta `$ be as in Definition 1.1(ii), (iii) respectively. By \[6, Lemma 4.5\] we have $`d=\delta `$; we call this common value the diameter of $`A,A^{}`$. An ordering of the eigenspaces of $`A`$ (resp. $`A^{}`$) is called standard whenever it satisfies (1) (resp. (2)). We comment on the uniqueness of the standard ordering. Let $`V_0,V_1,\mathrm{},V_d`$ denote a standard ordering of the eigenspaces of $`A`$. Then the ordering $`V_d,V_{d1},\mathrm{},V_0`$ is standard and no other ordering is standard. A similar result holds for the eigenspaces of $`A^{}`$. Let $`V_0,V_1,\mathrm{},V_d`$ (resp. $`V_0^{},V_1^{},\mathrm{},V_d^{}`$) denote a standard ordering of the eigenspaces of $`A`$ (resp. $`A^{}`$). By \[6, Corollary 5.7\], for $`0id`$ the spaces $`V_i`$, $`V_i^{}`$ have the same dimension; we denote this common dimension by $`\rho _i`$. By the construction $`\rho _i0`$. By \[6, Corollary 5.7\] and \[6, Corollary 6.6\], the sequence $`\rho _0,\rho _1,\mathrm{},\rho _d`$ is symmetric and unimodal; that is $`\rho _i=\rho _{di}`$ for $`0id`$ and $`\rho _{i1}\rho _i`$ for $`1id/2`$. We refer to the sequence $`(\rho _0,\rho _1,\mathrm{},\rho _d)`$ as the shape vector of $`A,A^{}`$.

The following special case has received a lot of attention. By a Leonard pair we mean a tridiagonal pair which has shape vector $`(1,1,\mathrm{},1)`$. There is a natural correspondence between the Leonard pairs and a family of orthogonal polynomials consisting of the $`q`$-Racah polynomials  and some related polynomials of the Askey-scheme , , . There is a classification of Leonard pairs in . This classification amounts to a linear algebraic version of a theorem of D. Leonard ,  concerning the $`q`$-Racah polynomials. See , , , , , , , ,  for more information about Leonard pairs.

In this paper our focus is on general tridiagonal pairs. We will discuss the following conjecture.

###### Conjecture 1.3

(Ito, Tanabe, Terwilliger ) Let $`(\rho _0,\rho _1,\mathrm{},\rho _d)`$ denote the shape vector of a tridiagonal pair. Then

$`\rho _i\left({\displaystyle \genfrac{}{}{0pt}{}{d}{i}}\right)(0id).`$
In the present paper we will prove Conjecture 1.3 for a certain type of tridiagonal pair. We will describe this type shortly. For now we review some more facts about general tridiagonal pairs.

Let $`A,A^{}`$ denote a tridiagonal pair on $`V`$. By \[6, Theorem 10.1\] there exists a sequence $`\beta ,\gamma ,\gamma ^{},\varrho ,\varrho ^{}`$ of scalars taken from $`𝕂`$ such that both

$`[A,A^2A^{}\beta AA^{}A+A^{}A^2\gamma (AA^{}+A^{}A)\varrho A^{}]`$ $`=`$ $`0,`$ (3)
$`[A^{},A^2A\beta A^{}AA^{}+AA^2\gamma ^{}(A^{}A+AA^{})\varrho ^{}A]`$ $`=`$ $`0,`$ (4)
where $`[r,s]`$ means $`rssr`$. The sequence is unique if the diameter is at least $`3`$. The equations (3), (4) are known as the tridiagonal relations , . An ordering of the eigenvalues of $`A`$ (resp. $`A^{}`$) will be called standard whenever the corresponding ordering of the eigenspaces of $`A`$ (resp. $`A^{}`$) is standard. Let $`\theta _0,\theta _1,\mathrm{},\theta _d`$ (resp. $`\theta _0^{},\theta _1^{},\mathrm{},\theta _d^{}`$) denote a standard ordering of the eigenvalues of $`A`$ (resp. $`A^{}`$). By \[6, Theorem 11.1\] we have

$`\theta _{i1}^2\beta \theta _{i1}\theta _i+\theta _i^2\gamma (\theta _{i1}+\theta _i)`$ $`=`$ $`\varrho (1id),`$ (5)
$`\theta _{i1}^2\beta \theta _{i1}^{}\theta _i^{}+\theta _i^2\gamma ^{}(\theta _{i1}^{}+\theta _i^{})`$ $`=`$ $`\varrho ^{}(1id).`$ (6)
By \[6, Theorem 4.6\] there exists a unique sequence $`U_0,U_1,\mathrm{},U_d`$ consisting of subspaces of $`V`$ such that

$`V=U_0+U_1+\mathrm{}+U_d(\text{direct sum}),`$ (7)
$`(A\theta _iI)U_iU_{i+1}(0i<d),(A\theta _dI)U_d=0,`$ (8)
$`(A^{}\theta _i^{}I)U_iU_{i1}(0<id),(A^{}\theta _0^{}I)U_0=0.`$ (9)
By \[6, Corollary 5.7\] the space $`U_i`$ has dimension $`\rho _i`$ for $`0id`$, where $`(\rho _0,\rho _1,\mathrm{},\rho _d)`$ is the shape vector for $`A,A^{}`$. We call the sequence $`U_0,U_1,\mathrm{},U_d`$ the split decomposition for $`A,A^{}`$ (with respect to the orderings $`\theta _0,\theta _1,\mathrm{},\theta _d`$ and $`\theta _0^{},\theta _1^{},\mathrm{},\theta _d^{}`$). For $`0id`$ let $`F_i:VV`$ denote the linear transformation which satisfies both

$`(F_iI)U_i=0,`$ (10)
$`F_iU_j=0\text{if}ji,(0jd).`$ (11)
In other words $`F_i`$ is the projection map from $`V`$ onto $`U_i`$. We observe

$`F_iF_j=\delta _{ij}F_i(0i,jd),`$
$`F_0+F_1+\mathrm{}+F_d=I,`$
$`F_iV=U_i(0id).`$
In view of (8), (9) we define

$`R`$ $`=`$ $`A{\displaystyle \underset{h=0}{\overset{d}{}}}\theta _hF_h,`$ (12)
$`L`$ $`=`$ $`A^{}{\displaystyle \underset{h=0}{\overset{d}{}}}\theta _h^{}F_h`$ (13)
and observe

$`RU_iU_{i+1}(0i<d),RU_d=0,`$ (14)
$`LU_iU_{i1}(0<id),LU_0=0.`$ (15)
Combining (14), (15) with (7) we find

$`R^{d+1}=0,L^{d+1}=0.`$ (16)
We call $`R`$ (resp. $`L`$) the raising map (resp. lowering map) for $`A,A^{}`$ with respect to $`U_0,U_1,\mathrm{},U_d`$.

We now describe the type of tridiagonal pair for which we will prove Conjecture 1.3.

###### Definition 1.4

For the rest of this paper, we assume $`𝕂`$ is algebraically closed with characteristic 0. We fix a nonzero scalar $`q𝕂`$ which is not a root of unity. We let $`A,A^{}`$ denote a tridiagonal pair on $`V`$ which satisfies (3), (4) where

$`\beta =q^2+q^2,\gamma =\gamma ^{}=\varrho =\varrho ^{}=0.`$ (17)
###### Note 1.5

The scalar $`q`$ which appears in  is the same as $`q^2`$ in the present paper. We make this adjustment for notational convenience.

Before proceeding we discuss the significance of assumption (17) from several points of view. Let $`A,A^{}`$ denote the tridiagonal pair in Definition 1.4. Evaluating (3), (4) using (17) we obtain

$`A^3A^{}[3]A^2A^{}A+[3]AA^{}A^2A^{}A^3`$ $`=`$ $`0,`$ (18)
$`A^3A[3]A^2AA^{}+[3]A^{}AA^2AA^3`$ $`=`$ $`0.`$ (19)
We are using the notation

$`[n]={\displaystyle \frac{q^nq^n}{qq^1}}n=0,1,\mathrm{}`$ (20)
The equations (18), (19) are known as the $`q`$-Serre relations, and are among the defining relations for the quantum affine algebra $`U_q(\widehat{sl_2})`$. See  and  for more information on $`U_q(\widehat{sl_2})`$.

Assumption (17) has the following significance for the eigenvalues. Let $`A,A^{}`$ denote the tridiagonal pair in Definition 1.4. Let $`\theta _0,\theta _1,\mathrm{},\theta _d`$ (resp. $`\theta _0^{},\theta _1^{},\mathrm{},\theta _d^{}`$) denote a standard ordering of the eigenvalues of $`A`$ (resp. $`A^{}`$). Evaluating (5) using $`\beta =q^2+q^2`$, $`\gamma =0`$, $`\varrho =0`$ we find either $`\theta _i=q^2\theta _{i1}`$ for $`1id`$ or $`\theta _i=q^2\theta _{i1}`$ for $`1id`$. Replacing $`\theta _0,\theta _1,\mathrm{},\theta _d`$ by $`\theta _d,\theta _{d1},\mathrm{},\theta _0`$ if necessary we may assume $`\theta _i=q^2\theta _{i1}`$ for $`1id`$. In this case there exists $`a𝕂`$ such that

$`\theta _i=aq^{2id}(0id).`$ (21)
Similarly replacing $`\theta _0^{},\theta _1^{},\mathrm{},\theta _d^{}`$ by $`\theta _d^{},\theta _{d1}^{},\mathrm{},\theta _0^{}`$ if necessary, there exists $`a^{}𝕂`$ such that

$`\theta _i^{}=a^{}q^{d2i}(0id).`$ (22)
Assumption (17) has the following significance for the raising and lowering maps. Let $`A,A^{}`$ denote the tridiagonal pair in Definition 1.4. Let $`U_0,U_1,\mathrm{},U_d`$ denote the split decomposition with respect to (21), (22) and let $`R`$ (resp. $`L`$) denote the corresponding raising (resp. lowering) map. By \[6, Theorem 12.2\] the maps $`R,L`$ satisfy the $`q`$-Serre relations

$`R^3L[3]R^2LR+[3]RLR^2LR^3`$ $`=`$ $`0,`$ (23)
$`L^3R[3]L^2RL+[3]LRL^2RL^3`$ $`=`$ $`0.`$ (24)
We emphasize that each of the pairs $`R,L`$ and $`A,A^{}`$ satisfy the $`q`$-Serre relations. Each of $`R,L`$ is nilpotent on $`V`$ and each of $`A,A^{}`$ is diagonalizable on $`V`$.

The following is our main result.

###### Theorem 1.6

Let $`A,A^{}`$ denote the tridiagonal pair in Definition 1.4 and let $`(\rho _0,\rho _1,\mathrm{},\rho _d)`$ denote the corresponding shape vector. Then

$`\rho _i\left({\displaystyle \genfrac{}{}{0pt}{}{d}{i}}\right)(0id).`$
In order to prove Theorem 1.6, for $`0id`$ we display a spanning set for $`U_i`$ consisting of $`(\genfrac{}{}{0pt}{}{d}{i})`$ vectors. We proceed as follows.

###### Theorem 1.7

Let $`A,A^{}`$ denote the tridiagonal pair in Definition 1.4. Let $`U_0,U_1,\mathrm{},U_d`$ denote the split decomposition with respect to (21), (22) and let $`R,L`$ denote the corresponding raising and lowering maps. Let $`v`$ denote a nonzero vector in $`U_0`$. Then $`V`$ is spanned by the vectors of the form

$`L^{i_1}R^{i_2}L^{i_3}R^{i_4}\mathrm{}R^{i_n}v,`$
where $`i_1,i_2,\mathrm{},i_n`$ ranges over all sequences such that $`n`$ is a nonnegative even integer, and $`i_1,i_2,\mathrm{}i_n`$ are integers satisfying $`0i_1<i_2<\mathrm{}<i_nd`$.

We prove Theorem 1.7 at the end of Section 2. In order to illustrate Theorem 1.7 we now restate it in concrete terms for $`d=3`$.

###### Corollary 1.8

With reference to Theorem 1.7, for $`d=3`$ the space $`V`$ is spanned by the vectors

$`v,Rv,R^2v,R^3v,LR^2v,LR^3v,L^2R^3v,RL^2R^3v.`$
Combining Theorem 1.7 with (14), (15) we routinely obtain the following theorem.

###### Theorem 1.9

Let $`A,A^{}`$ denote the tridiagonal pair in Definition 1.4. Let $`U_0,U_1,\mathrm{},U_d`$ denote the split decomposition with respect to (21), (22) and let $`R,L`$ denote the corresponding raising and lowering maps. Let $`v`$ denote a nonzero vector in $`U_0`$. Then for $`0id`$ the space $`U_i`$ is spanned by the vectors of the form

$`L^{i_1}R^{i_2}L^{i_3}R^{i_4}\mathrm{}R^{i_n}v,`$
where $`i_1,i_2,\mathrm{},i_n`$ ranges over all sequences such that (i) $`n`$ is a nonnegative even integer; (ii) $`i_1,i_2,\mathrm{}i_n`$ are integers satisfying $`0i_1<i_2<\mathrm{}<i_nd`$ and $`i=_{h=1}^ni_h(1)^h`$.

###### Corollary 1.10

With reference to Theorem 1.9, for $`d=3`$ the following (i)–(iv) hold.

1. The space $`U_0`$ is spanned by

$`v.`$
2. The space $`U_1`$ is spanned by

$`Rv,LR^2v,L^2R^3v.`$
3. The space $`U_2`$ is spanned by

$`R^2v,LR^3v,RL^2R^3v.`$
4. The space $`U_3`$ is spanned by

$`R^3v.`$

## 2 The algebra $`𝒜`$

Our next goal is to prove Theorem 1.7. In order to do this we undertake a careful investigation of the $`q`$-Serre relations. We begin with a definition.

###### Definition 2.1

We let $`𝒜`$ denote the associative $`𝕂`$-algebra with identity generated by symbols $`x,y`$ subject to the $`q`$-Serre relations

$`x^3y[3]x^2yx+[3]xyx^2yx^3`$ $`=`$ $`0,`$
$`y^3x[3]y^2xy+[3]yxy^2xy^3`$ $`=`$ $`0.`$
###### Remark 2.2

The algebra $`𝒜`$ in Definition 2.1 is often called the positive part of $`U_q(\widehat{sl_2})`$.

###### Definition 2.3

Referring to Definition 2.1, we let $`\sigma _0:𝒜𝒜`$ denote the $`𝕂`$-algebra isomorphism which sends $`x`$ to $`y`$ and $`y`$ to $`x`$. We let $`\sigma _1:𝒜𝒜`$ denote the $`𝕂`$-algebra antiisomorphism which stabilizes each of $`x,y`$. The action of $`\sigma _1`$ inverts the word order. We observe $`\sigma _0,\sigma _1`$ commute. We define $`\sigma =\sigma _0\sigma _1`$ and observe each of $`\sigma _0,\sigma _1,\sigma `$ is an involution.

###### Example 2.4

Applying each of $`\sigma _0,\sigma _1,\sigma `$ to $`xyx^2y^2`$ we get

$`yxy^2x^2,y^2x^2yx,x^2y^2xy`$
respectively.

We now state a lemma which we will find useful. We first recall some notation. Let $`n`$ denote a nonnegative integer. With reference to (20) we define

$`[n]!=[n][n1]\mathrm{}[2][1].`$
We interpret $`[0]!=1`$. We also define

$`\left[{\displaystyle \genfrac{}{}{0pt}{}{n}{i}}\right]={\displaystyle \frac{[n]!}{[i]![ni]!}}(0in).`$
###### Lemma 2.5

\[10, Proposition 7.1.5\] The following relations hold in $`𝒜`$. Let $`r`$ denote a positive integer. Then

$`{\displaystyle \underset{i=0}{\overset{2r+1}{}}}(1)^i\left[{\displaystyle \genfrac{}{}{0pt}{}{2r+1}{i}}\right]x^iy^rx^{2r+1i}`$ $`=`$ $`0,`$ (25)
$`{\displaystyle \underset{i=0}{\overset{2r+1}{}}}(1)^i\left[{\displaystyle \genfrac{}{}{0pt}{}{2r+1}{i}}\right]y^ix^ry^{2r+1i}`$ $`=`$ $`0.`$ (26)
###### Remark 2.6

The relations (25), (26) are often called the higher order $`q`$-Serre relations \[10, p.57\].

We now give the higher order $`q`$-Serre relations in a modified form. We will use the following notation. For all integers $`n,k`$ with $`k`$ nonnegative we define

$`[n]_k=[n][n1]\mathrm{}[nk+1].`$
We interpret $`[n]_0=1`$.

###### Lemma 2.7

The following relations hold in $`𝒜`$. Let $`r`$ denote a positive integer and let $`n`$ denote an integer at least $`2r+1`$. Then for $`0in`$ we have

$`x^iy^rx^{ni}={\displaystyle \underset{\xi =0}{\overset{r}{}}}{\displaystyle \frac{[i]_\xi [ri]_{r\xi }[ni]_r}{[\xi ]_\xi [r\xi ]_{r\xi }[n\xi ]_r}}x^\xi y^rx^{n\xi }`$ (27)
$`+{\displaystyle \underset{\zeta =0}{\overset{r1}{}}}{\displaystyle \frac{[i]_{r+1}[in+r1]_{r\zeta 1}[ni]_\zeta }{[n\zeta ]_{r+1}[r\zeta 1]_{r\zeta 1}[\zeta ]_\zeta }}x^{n\zeta }y^rx^\zeta .`$ (28)
Proof: We abbreviate $`w_i=x^iy^rx^{ni}`$ for $`0in`$. We obtain a system of $`n2r`$ linear equations relating $`w_0,w_1,\mathrm{},w_n`$ as follows. For $`0jn2r1`$ we multiply each term in (25) on the left by $`x^j`$ and on the right by $`x^{n2r1j}`$. The result is a linear equation relating $`w_j,w_{j+1},\mathrm{},w_{j+2r+1}`$. This yields a system of $`n2r`$ linear equations involving $`w_0,w_1,\mathrm{},w_n`$. We now solve this system to obtain each of $`w_0,w_1,\mathrm{},w_n`$ in terms of $`w_0,w_1,\mathrm{},w_r`$ and $`w_{nr+1},w_{nr+2},\mathrm{},w_n`$. We define a $`(n+1)\times (2r+1)`$ matrix $`S`$ as follows. For $`0in`$ and $`rjr`$ the entry $`S_{ij}=q^{2ij}`$. For $`0in`$ let $`S_i`$ denote row $`i`$ of $`S`$. Observe that for $`0jn2r1`$ the vectors $`S_j,S_{j+1},\mathrm{},S_{j+2r+1}`$ satisfy the same equation as the one for $`w_j,w_{j+1},\mathrm{},w_{j+2r+1}`$ which we mentioned above. Observe $`S_0,S_1,\mathrm{},S_{2r}`$ are linearly independent since $`S`$ is essentially Vandermonde. Therefore $`S_0,S_1,\mathrm{},S_{2r}`$ is a basis for $`𝕂^{2r+1}`$. Consider the linear transformation $`\epsilon `$ from $`𝕂^{2r+1}`$ to $`\text{Span}(w_0,w_1,\mathrm{},w_n)`$ which sends $`S_i`$ to $`w_i`$ for $`0i2r`$. From our above comments $`\epsilon `$ sends $`S_i`$ to $`w_i`$ for $`0in`$. For $`0in`$ we have

$`S_i={\displaystyle \underset{\xi =0}{\overset{r}{}}}{\displaystyle \frac{[i]_\xi [ri]_{r\xi }[ni]_r}{[\xi ]_\xi [r\xi ]_{r\xi }[n\xi ]_r}}S_\xi `$ (29)
$`+{\displaystyle \underset{\zeta =0}{\overset{r1}{}}}{\displaystyle \frac{[i]_{r+1}[in+r1]_{r\zeta 1}[ni]_\zeta }{[n\zeta ]_{r+1}[r\zeta 1]_{r\zeta 1}[\zeta ]_\zeta }}S_{n\zeta }.`$ (30)
This can be verified using Cramer’s rule. Applying $`\epsilon `$ to each term in (29), (30) we obtain (27), (28). $`\mathrm{}`$

###### Remark 2.8

Applying each of $`\sigma _0,\sigma _1,\sigma `$ to the relations in Lemma 2.7, we obtain additional relations involving $`x,y`$ which hold in $`𝒜`$.

The following fact is an immediate consequence of Lemma 2.7 and Remark 2.8.

###### Corollary 2.9

The following linear dependencies hold in $`𝒜`$. Let $`r`$ denote a positive integer and let $`n`$ denote an integer at least $`2r+1`$.

1. For $`r+1inr`$ the element $`x^iy^rx^{ni}`$ is contained in

$`\text{Span}\{x^\xi y^rx^{n\xi }|\mathrm{\hspace{0.33em}0}\xi r\}+\text{Span}\{x^{n\zeta }y^rx^\zeta |\mathrm{\hspace{0.33em}0}\zeta r1\}.`$
2. For $`rinr1`$ the element $`x^iy^rx^{ni}`$ is contained in

$`\text{Span}\{x^\xi y^rx^{n\xi }|\mathrm{\hspace{0.33em}0}\xi r1\}+\text{Span}\{x^{n\zeta }y^rx^\zeta |\mathrm{\hspace{0.33em}0}\zeta r\}.`$
3. For $`r+1inr`$ the element $`y^ix^ry^{ni}`$ is contained in

$`\text{Span}\{y^\xi x^ry^{n\xi }|\mathrm{\hspace{0.33em}0}\xi r\}+\text{Span}\{y^{n\zeta }x^ry^\zeta |\mathrm{\hspace{0.33em}0}\zeta r1\}.`$
4. For $`rinr1`$ the element $`y^ix^ry^{ni}`$ is contained in

$`\text{Span}\{y^\xi x^ry^{n\xi }|\mathrm{\hspace{0.33em}0}\xi r1\}+\text{Span}\{y^{n\zeta }x^ry^\zeta |\mathrm{\hspace{0.33em}0}\zeta r\}.`$

###### Definition 2.10

Let $`n`$ denote a nonnegative integer. By a word of length n in $`𝒜`$, we mean an expression of the form

$$a_1a_2\mathrm{}a_n,$$
(31)
where $`a_i=x`$ or $`a_i=y`$ for $`1in`$. We interpret the word of length 0 as the identity element in $`𝒜`$. We say this word is trivial. By the height of the word (31) we mean the integer

$`|\{i|\mathrm{\hspace{0.33em}1}in,a_i=x\}||\{i|\mathrm{\hspace{0.33em}1}in,a_i=y\}|.`$
###### Definition 2.11

A word is said to be balanced whenever it has height 0. We observe that a balanced word has even length.

###### Example 2.12

We list the balanced words of length $`4`$.

$`x^2y^2,xyxy,xy^2x,y^2x^2,yxyx,yx^2y.`$
###### Definition 2.13

Let $`a_1a_2\mathrm{}a_n`$ denote a word in $`𝒜`$. By the height vector of $`a_1a_2\mathrm{}a_n`$ we mean the sequence $`(h_0,h_1,\mathrm{},h_n)`$, where $`h_i`$ denotes the height of the word $`a_{i+1}a_{i+2}\mathrm{}a_n`$ for $`0in`$. We observe that the height vector of $`a_1a_2\mathrm{}a_n`$ is the unique sequence $`(h_0,h_1,\mathrm{},h_n)`$ such that (i) $`h_n=0`$; (ii) for $`1in`$, $`h_{i1}h_i=1`$ if $`a_i=x`$ and $`h_{i1}h_i=1`$ if $`a_i=y`$.

###### Example 2.14

The word $`x^2yx^3y^2x`$ has height vector

$`(3,2,1,2,1,0,1,0,1,0).`$
###### Definition 2.15

Let $`a_1a_2\mathrm{}a_n`$ denote a word in $`𝒜`$ and let $`(h_0,h_1,\mathrm{},h_n)`$ denote the corresponding height vector. We say $`a_1a_2\mathrm{}a_n`$ is height-symmetric whenever $`h_i=h_{ni}`$ for $`0in`$. We observe that $`a_1a_2\mathrm{}a_n`$ is height-symmetric if and only if $`a_ia_{ni+1}`$ for $`1in`$. We remark that a height-symmetric word is balanced and invariant under $`\sigma `$.

###### Example 2.16

We list the height-symmetric words of length 4.

$`x^2y^2,xyxy,y^2x^2,yxyx.`$
###### Definition 2.17

Let $`a_1a_2\mathrm{}a_n`$ denote a word in $`𝒜`$ and let $`(h_0,h_1,\mathrm{},h_n)`$ denote the corresponding height vector. We say $`a_1a_2\mathrm{}a_n`$ is nil whenever at least one of $`h_0,h_1,\mathrm{},h_n`$ is negative.

###### Example 2.18

We list the nil balanced words of length 4.

$`x^2y^2,xyxy,xy^2x,yx^2y.`$
We mention a few subspaces of $`𝒜`$.

###### Definition 2.19

We let $``$ denote the linear subspace of $`𝒜`$ spanned by the balanced words. We observe $``$ is a $`𝕂`$-subalgebra of $`𝒜`$ which is invariant under each of $`\sigma _0,\sigma _1,\sigma `$. We let $`^{sym}`$ denote the linear subspace of $``$ spanned by the height-symmetric words. We let $`^{nil}`$ denote the linear subspace of $``$ spanned by the nil balanced words. We observe $`^{nil}`$ is a two sided ideal of $``$ which is invariant under $`\sigma `$.

###### Theorem 2.20

Let $`i,j,m,n`$ denote nonnegative integers such that $`i+n=j+m`$. Define $`b=y^ix^my^nx^j`$ and observe $`b`$ is a balanced word. Then

$`b^{sym}+^{nil}.`$ (32)
Proof: We proceed by induction on $`\text{min}(m,n)`$. First assume $`\text{min}(m,n)=0`$. Then $`b`$ is height-symmetric. Therefore $`b^{sym}`$ so (32) holds. Next assume $`\text{min}(m,n)>0`$. Replacing $`b`$ by $`b^\sigma `$ if necessary we may assume $`mn`$. Assume for the moment that $`m=n`$. Then $`b`$ is height-symmetric. Therefore $`b^{sym}`$ so (32) holds. Next assume $`m>n`$. We may assume $`nj`$; otherwise $`b^{nil}`$. By Corollary 2.9(i), $`b`$ is contained in

$`\text{Span}\{y^ix^\xi y^nx^{i+n\xi }|\mathrm{\hspace{0.33em}0}\xi n\}+\text{Span}\{y^ix^{i+n\zeta }y^nx^\zeta |\mathrm{\hspace{0.33em}0}\zeta n1\}.`$ (33)
By the induction hypothesis, for $`0\xi n1`$ the word $`y^ix^\xi y^nx^{i+n\xi }`$ is contained in $`^{sym}+^{nil}`$. For $`\xi =n`$ the word $`y^ix^\xi y^nx^{i+n\xi }`$ is height-symmetric and therefore contained in $`^{sym}`$. For $`0\zeta n1`$ the word $`y^ix^{i+n\zeta }y^nx^\zeta `$ is contained in $`^{nil}`$. Apparently the space displayed in (33) is contained in $`^{sym}+^{nil}`$. It follows $`b^{sym}+^{nil}`$ as desired. $`\mathrm{}`$

###### Lemma 2.21

For $`b^{sym}+^{nil}`$ we have $`bb^\sigma ^{nil}`$.

Proof: There exists $`b_0^{sym}`$ and there exists $`b_1^{nil}`$ such that $`b=b_0+b_1`$. Observe $`b_0^\sigma =b_0`$ so $`bb^\sigma =b_1b_1^\sigma `$. By assumption $`b_1^{nil}`$. Recall $`\sigma `$ leaves $`^{nil}`$ invariant so $`b_1^\sigma ^{nil}`$. By these comments $`bb^\sigma ^{nil}`$. $`\mathrm{}`$

###### Corollary 2.22

Let $`i,j,m,n`$ denote nonnegative integers such that $`i+n=j+m`$. Define $`b=y^ix^my^nx^j`$ and recall $`b`$ is a balanced word. Then

$`bb^\sigma ^{nil}.`$
Proof: Immediate from Theorem 2.20 and Lemma 2.21. $`\mathrm{}`$

###### Corollary 2.23

For nonnegative integers $`i,j`$ we have

$`[y^ix^i,y^jx^j]^{nil}.`$
Proof: Apply Corollary 2.22 with $`m=i`$ and $`n=j`$. $`\mathrm{}`$

In order to state the next theorem we make a definition.

###### Definition 2.24

Let $`a_1a_2\mathrm{}a_n`$ denote a word in $`𝒜`$. Observe that there exists a unique sequence $`(i_1,i_2,\mathrm{},i_r)`$ consisting of positive integers such that $`a_1a_2\mathrm{}a_n`$ is one of $`x^{i_1}y^{i_2}x^{i_3}\mathrm{}y^{i_r}`$ or $`x^{i_1}y^{i_2}x^{i_3}\mathrm{}x^{i_r}`$ or $`y^{i_1}x^{i_2}y^{i_3}\mathrm{}x^{i_r}`$ or $`y^{i_1}x^{i_2}y^{i_3}\mathrm{}y^{i_r}`$. We call the sequence $`(i_1,i_2,\mathrm{},i_r)`$ the signature of $`a_1a_2\mathrm{}a_n`$.

###### Example 2.25

Each of the words $`yx^2y^2x`$, $`xy^2x^2y`$ has signature $`(1,2,2,1)`$.

###### Definition 2.26

Let $`a_1a_2\mathrm{}a_n`$ denote a word in $`𝒜`$ and let $`(i_1,i_2,\mathrm{},i_r)`$ denote the corresponding signature. We say $`a_1a_2\mathrm{}a_n`$ is reducible whenever there exists an integer $`s`$ $`(2sr1)`$ such that $`i_{s1}i_s<i_{s+1}`$. We say a word is irreducible whenever it is not reducible.

###### Example 2.27

A word of length less than 4 is irreducible. The only reducible words of length 4 are $`xyx^2`$ and $`yxy^2`$.

In the following lemma we give a necessary and sufficient condition for a given nontrivial word to be irreducible.

###### Lemma 2.28

Let $`a_1a_2\mathrm{}a_n`$ denote a nontrivial word in $`𝒜`$ and let $`(i_1,i_2,\mathrm{},i_r)`$ denote the corresponding signature. Then the following (i), (ii) are equivalent.

1. The word $`a_1a_2\mathrm{}a_n`$ is irreducible.
2. There exists an integer $`t`$ $`(1tr)`$ such that

$`i_1<i_2<\mathrm{}<i_{t1}<i_ti_{t+1}i_{t+2}\mathrm{}i_{r1}i_r.`$

Proof: Routine using Definition 2.26. $`\mathrm{}`$

Consider the algebra $`𝒜`$ as a vector space over $`𝕂`$. It turns out that the set of irreducible words in $`𝒜`$ forms a basis for $`𝒜`$. However, in order to prove Theorem 1.7 all we need is that this set spans $`𝒜`$. We will prove this much for now and use the result to obtain Theorem 1.7. For the sake of completeness, in Section 3 we will prove that the set of irreducible words in $`𝒜`$ is a basis for $`𝒜`$.

###### Theorem 2.29

The irreducible words in $`𝒜`$ form a spanning set for $`𝒜`$.

Proof: Let $`\lambda =(\lambda _1,\lambda _2,\mathrm{},\lambda _r)`$ denote a finite sequence of positive integers. We say this sequence is nonincreasing whenever $`\lambda _{i1}\lambda _i`$ for $`2ir`$. Let $`\mathrm{\Psi }`$ denote the set consisting of the nonincreasing finite sequences of positive integers. There exists a certain linear order on $`\mathrm{\Psi }`$ called the reverse lexicographical order. This is defined as follows. Let $`\lambda =(\lambda _1,\lambda _2,\mathrm{},\lambda _r)`$ and $`\mu =(\mu _1,\mu _2,\mathrm{},\mu _s)`$ denote elements in $`\mathrm{\Psi }`$. Then $`\lambda `$ is less than $`\mu `$ in the reverse lexicographical order whenever (i) $`r<s`$; or (ii) $`r=s`$ and there exists an integer $`k`$ $`(1kr)`$ such that $`\lambda _i=\mu _i`$ $`(k+1ir)`$, $`\lambda _k<\mu _k`$. Let $`\lambda =(\lambda _1,\lambda _2,\mathrm{},\lambda _r)`$ denote a finite sequence of positive integers. We let $`\overline{\lambda }`$ denote the rearrangement of $`\lambda `$ into a nonincreasing sequence. In other words $`\overline{\lambda }=(\mu _1,\mu _2,\mathrm{},\mu _r)`$ where $`\{\mu _1,\mu _2,\mathrm{},\mu _r\}=\{\lambda _1,\lambda _2,\mathrm{},\lambda _r\}`$ as multisets and the sequence $`(\mu _1,\mu _2,\mathrm{},\mu _r)`$ is nonincreasing. We call $`\overline{\lambda }`$ the rearrangement of $`\lambda `$. Let $`\lambda =(\lambda _1,\lambda _2,\mathrm{},\lambda _r)`$ denote a finite sequence of positive integers. By an inversion in $`\lambda `$ we mean an ordered pair $`(i,j)`$ of integers such that $`1i<jr`$ and $`\lambda _i<\lambda _j`$. We observe $`\lambda =\overline{\lambda }`$ if and only if $`\lambda `$ has no inversions. We assume the present theorem is false and obtain a contradiction. By a counterexample we mean a word in $`𝒜`$ which is not contained in the span of the irreducible words. By assumption there exists a counterexample. Let $`w`$ denote a counterexample and let $`\lambda =(\lambda _1,\lambda _2,\mathrm{},\lambda _r)`$ denote the corresponding signature. Without loss, we assume that among all the counterexamples, the rearrangement $`\overline{\lambda }`$ is minimal with respect to the reverse lexicographical order. Moreover, without loss we may assume that among all the counterexamples for which the rearranged signature is equal to $`\overline{\lambda }`$, the signature $`\lambda `$ has a minimal number of inversions. Since $`w`$ is a counterexample it is reducible. Therefore there exists an integer $`s`$ $`(2sr1)`$ such that $`\lambda _{s1}\lambda _s<\lambda _{s+1}`$. By the construction there exist words $`w_1,w_2`$ in $`𝒜`$ such that $`w=w_1x^{\lambda _{s1}}y^{\lambda _s}x^{\lambda _{s+1}}w_2`$ or $`w=w_1y^{\lambda _{s1}}x^{\lambda _s}y^{\lambda _{s+1}}w_2`$. We treat the first case; the second case is treated in a similar manner. By Corollary 2.9(ii) (with $`i=\lambda _{s1}`$, $`r=\lambda _s`$, $`n=\lambda _{s1}+\lambda _{s+1}`$) we find $`w`$ is contained in

$`\text{Span}\{w_1x^\xi y^{\lambda _s}x^{\lambda _{s1}+\lambda _{s+1}\xi }w_2|\mathrm{\hspace{0.33em}0}\xi \lambda _s1\}`$ (34)
$`+\text{Span}\{w_1x^{\lambda _{s1}+\lambda _{s+1}\zeta }y^{\lambda _s}x^\zeta w_2|\mathrm{\hspace{0.33em}0}\zeta \lambda _s\}.`$ (35)
By our minimality assumptions no word which appears in (34) is a counterexample and no word which appears in (35) is a counterexample. Therefore the sum displayed in (34), (35) is contained in the span of the irreducible words. The word $`w`$ is contained in this space so $`w`$ is in the span of the irreducible words. This contradicts our assumption that $`w`$ is a counterexample. The result follows. $`\mathrm{}`$

We are now ready to prove Theorem 1.7.

Proof of Theorem 1.7: By (23), (24) there exists an $`𝒜`$-module structure on $`V`$ such that $`x.v=Rv`$ and $`y.v=Lv`$ for all $`vV`$. Let $`b`$ denote a balanced word in $`𝒜`$. Using (14) and (15) we find each of $`U_0,U_1,\mathrm{},U_d`$ is invariant under $`b`$. In particular $`U_0`$ is invariant under $`b`$. Let $`i`$ denote a nonnegative integer. The word $`y^ix^i`$ is balanced so it leaves $`U_0`$ invariant. From (16) we find $`x^{d+1}`$ vanishes on $`V`$. In particular $`x^{d+1}`$ vanishes on $`U_0`$. Therefore $`y^ix^i`$ vanishes on $`U_0`$ for $`i>d`$. We claim the elements $`y^ix^i`$ $`(0id)`$ mutually commute on $`U_0`$. To see this, observe by (14), (15) that each nil word of $`𝒜`$ vanishes on $`U_0`$. In particular each nil word in $``$ vanishes on $`U_0`$ so $`^{nil}`$ vanishes on $`U_0`$. By this and Corollary 2.23 we find $`[y^ix^i,y^jx^j]`$ vanishes on $`U_0`$ for $`0i,jd`$. We have now shown the elements $`y^ix^i`$ $`(0id)`$ mutually commute on $`U_0`$. Since $`𝕂`$ is algebraically closed there exists a nonzero $`vU_0`$ which is a common eigenvector of the $`y^ix^i`$ $`(0id)`$. Let $`W`$ denote the subspace of $`V`$ spanned by the vectors of the form

$`y^{i_1}x^{i_2}y^{i_3}x^{i_4}\mathrm{}x^{i_n}.v,`$ (36)
where $`i_1,i_2,\mathrm{},i_n`$ ranges over all sequences such that $`n`$ is a nonnegative even integer, and $`i_1,i_2,\mathrm{}i_n`$ are integers satisfying $`0i_1<i_2<\mathrm{}<i_nd`$. We show $`W=V`$. Observe $`vW`$ so $`W0`$. By Definition 1.1(iv) the space $`V`$ is irreducible as a module for $`A,A^{}`$. In order to show $`W=V`$ we show $`W`$ is invariant under each of $`A,A^{}`$. Using Lemma 2.28 and Theorem 2.29 we routinely find $`𝒜.v=W`$. From this we find $`W`$ is invariant under each of $`x,y`$. It follows $`W`$ is invariant under each of $`R,L`$. Using (14), (15) we find the vector (36) is contained in $`U_i`$ where $`i=_{h=1}^ni_h(1)^h`$. By this and (10), (11) the vector (36) is an eigenvector for each of $`F_0,F_1,\mathrm{},F_d`$. We now see $`W`$ is invariant under each of $`F_0,F_1,\mathrm{},F_d`$. By these comments and (12), (13) we find $`W`$ is invariant under each of $`A,A^{}`$. We conclude $`W=V`$ and the result follows. $`\mathrm{}`$

Proof of Theorem 1.9: Combine Theorem 1.7 with (14) and (15). $`\mathrm{}`$

Proof of Theorem 1.6: For $`0id`$, the spanning set for $`U_i`$ given in Theorem 1.9 has cardinality $`\left(\genfrac{}{}{0pt}{}{d}{i}\right)`$. $`\mathrm{}`$

## 3 Comments and suggestions for further research

In this section we give some comments and suggestions for further research. We begin with a comment.

###### Lemma 3.1

The quotient algebra $`/^{nil}`$ is generated by the elements

$`y^ix^i+^{nil}(0i<\mathrm{}).`$
Moreover $`/^{nil}`$ is commutative.

Proof: The first assertion is immediate from Theorem 2.29. The last assertion follows from this and Corollary 2.23. $`\mathrm{}`$

Just before Theorem 2.29 we asserted that the set of irreducible words in $`𝒜`$ is a basis for $`𝒜`$. We will now prove this assertion.

###### Theorem 3.2

The set of irreducible words in $`𝒜`$ is a basis for $`𝒜`$.

Proof: Let $`X`$ denote the set of irreducible words in $`𝒜`$. Then $`X`$ spans $`𝒜`$ by Theorem 2.29. For $`0n<\mathrm{}`$ let $`X_n`$ denote the set of irreducible words in $`𝒜`$ which have length $`n`$. Of course $`X=_{n=0}^{\mathrm{}}X_n`$. For $`0n<\mathrm{}`$ let $`𝒜_n`$ denote the subspace of $`𝒜`$ spanned by the words of length $`n`$. Since the $`q`$-Serre relations are homogeneous we have

$`𝒜={\displaystyle \underset{n=0}{\overset{\mathrm{}}{}}}𝒜_n(\text{direct sum}).`$ (37)
By the construction $`X_n𝒜_n`$ for $`0n<\mathrm{}`$. By these comments we find $`X_n`$ spans $`𝒜_n`$ for $`0n<\mathrm{}`$. We show

$`|X_n|=\text{dim}(𝒜_n)(0n<\mathrm{}).`$ (38)
Let $`v`$ denote an indeterminate. In what follows, we consider formal power series in $`v`$ which have coefficients in $``$. Line (38) will follow once we show

$`{\displaystyle \underset{n=0}{\overset{\mathrm{}}{}}}|X_n|v^n={\displaystyle \underset{n=0}{\overset{\mathrm{}}{}}}\text{dim}(𝒜_n)v^n.`$ (39)
We claim

$`{\displaystyle \underset{n=0}{\overset{\mathrm{}}{}}}\text{dim}(𝒜_n)v^n={\displaystyle \underset{m=1}{\overset{\mathrm{}}{}}}(1v^{2m})^1(1v^{2m1})^2.`$ (40)
To see (40), recall $`𝒜`$ is the positive part of $`U_q(\widehat{sl_2})`$ and hence isomorphic to the Verma module for $`\widehat{sl_2}`$ \[21, p. 123\] as a graded vector space. Apparently the left-hand side of (40) is equal to the formal character of the Verma module. This character is inverse to the principally specialized Weyl denominator and is therefore equal to the right-hand side of (40) \[7, p. 181\]. We now have (40). For $`0n<\mathrm{}`$, by a partition of $`n`$ we mean a sequence of positive integers $`\lambda =(\lambda _1,\lambda _2,\mathrm{},\lambda _r)`$ such that $`\lambda _{i1}\lambda _i`$ for $`2ir`$ and $`_{i=1}^r\lambda _i=n`$. We call $`\lambda _1,\lambda _2,\mathrm{},\lambda _r`$ the parts of $`\lambda `$. We sometimes write $`n=|\lambda |`$. Let $`p_n`$ denote the number of partitions of $`n`$. Let $`p_n^{}`$ denote the number of partitions of $`n`$ whose parts are mutually distinct. The following two generating functions are well known:

$`{\displaystyle \underset{n=0}{\overset{\mathrm{}}{}}}p_nv^n`$ $`=`$ $`{\displaystyle \underset{m=1}{\overset{\mathrm{}}{}}}(1v^m)^1,`$
$`{\displaystyle \underset{n=0}{\overset{\mathrm{}}{}}}p_n^{}v^n`$ $`=`$ $`{\displaystyle \underset{m=1}{\overset{\mathrm{}}{}}}(1v^{2m1})^1.`$
See for example \[1, Theorem 1.1\]. For $`0n<\mathrm{}`$ let $`Y_n`$ denote the set of ordered pairs $`(\lambda ,\mu )`$ such that (i) $`\lambda `$ is a partition whose parts are mutually distinct; (ii) $`\mu `$ is a partition; (iii) $`|\lambda |+|\mu |=n`$. From the construction

$`{\displaystyle \underset{n=0}{\overset{\mathrm{}}{}}}|Y_n|v^n`$ $`=`$ $`\left({\displaystyle \underset{n=0}{\overset{\mathrm{}}{}}}p_n^{}v^n\right)\left({\displaystyle \underset{n=0}{\overset{\mathrm{}}{}}}p_nv^n\right)`$ (41)
$`=`$ $`{\displaystyle \underset{m=1}{\overset{\mathrm{}}{}}}(1v^{2m})^1(1v^{2m1})^2.`$
We show

$`|X_n|=|Y_n|(0n<\mathrm{}).`$ (42)
To obtain (42), for $`0n<\mathrm{}`$ we display a bijection $`\epsilon :Y_nX_n`$. Let $`(\lambda ,\mu )`$ denote an element of $`Y_n`$ and write $`\lambda =(\lambda _1,\lambda _2,\mathrm{},\lambda _r)`$, $`\mu =(\mu _1,\mu _2,\mathrm{},\mu _s)`$. The image of $`(\lambda ,\mu )`$ under $`\epsilon `$ is the following word in $`𝒜`$:

$`\mathrm{}x^{\lambda _4}y^{\lambda _3}x^{\lambda _2}y^{\lambda _1}x^{\mu _1}y^{\mu _2}x^{\mu _3}y^{\mu _4}\mathrm{}.`$ (43)
By the construction the word (43) is irreducible with length $`n`$. Therefore the word (43) is contained in $`X_n`$. Using Lemma 2.28 we find $`\epsilon :Y_nX_n`$ is a bijection. We now have (42). Combining (40), (41), (42) we obtain (39) and (38) follows. We conclude $`X_n`$ is a basis of $`𝒜_n`$ for $`0n<\mathrm{}`$. By this and (37) we find $`X`$ is a basis for $`𝒜`$. $`\mathrm{}`$

###### Remark 3.3

The following is a specialization of the Jacobi triple product identity \[7, p. 185\]:

$`{\displaystyle \underset{n=\mathrm{}}{\overset{\mathrm{}}{}}}(v)^{n^2}={\displaystyle \underset{m=1}{\overset{\mathrm{}}{}}}(1v^{2m})(1v^{2m1})^2.`$ (44)
If we set $`v=e^{\pi iz}`$ for $`i,z`$ with $`i^2=1`$ and $`\text{Im}(z)>0`$, then either side of (44) is equal to the theta function $`\theta _4(z)`$. See \[5, pp. 103–105\] for more detail.

We give a suggestion for future research.

###### Problem 3.4

Let $`\beta ,\gamma ,\gamma ^{},\varrho ,\varrho ^{}`$ denote a sequence of scalars taken from $`𝕂`$. Let $`𝒯`$ denote the associative $`𝕂`$-algebra with identity generated by symbols $`x,y`$ subject to the tridiagonal relations

$`[x,x^2y\beta xyx+yx^2\gamma (xy+yx)\varrho y]`$ $`=`$ $`0,`$
$`[y,y^2x\beta yxy+xy^2\gamma ^{}(yx+xy)\varrho ^{}x]`$ $`=`$ $`0.`$
Find analogs of the higher order $`q`$-Serre relations which hold in $`𝒯`$. Find a basis for the $`𝕂`$-vector space $`𝒯`$.

###### Problem 3.5

Let the algebra $`𝒯`$ be as in Problem 3.4. An element of $`𝒯`$ is called central whenever it commutes with every element of $`𝒯`$. By definition the center of $`𝒯`$ is the $`𝕂`$-subalgebra of $`𝒯`$ consisting of the central elements of $`𝒯`$. Describe the center of $`𝒯`$. Find a generating set for this center.

## 4 Acknowledgment

The authors thank Georgia Benkart, Vyjayanthi Chari, Arjeh Cohen, Atsushi Matsuo, Anne Schilling, and Kenichiro Tanabe for helpful discussions on the subject of this paper. The authors thank Michio Jimbo for providing a proof of (40).

Tatsuro Ito Department of Computational Science Faculty of Science Kanazawa University Kakuma-machi, Kanazawa 920–1192, Japan E-mail: ito@kappa.s.kanazawa-u.ac.jp

Paul Terwilliger Department of Mathematics University of Wisconsin 480 Lincoln drive Madison, Wisconsin, 53706, USA E-mail: terwilli@math.wisc.edu


text:
# Photon-assisted tunneling in a Fe8 Single-Molecule Magnet

## Abstract

The low temperature spin dynamics of a Fe8 Single-Molecule Magnet was studied under circularly polarized electromagnetic radiation allowing us to establish clearly photon-assisted tunneling. This effect, while linear at low power, becomes highly non-linear above a relatively low power threshold. This non-linearity is attributed to the nature of the coupling of the sample to the thermostat. These results are of great importance if such systems are to be used as quantum computers.

Molecular nanomagnets have attracted much interest in recent years both from experimental and theoretical point of view Sessoli93b ; Barra96 ; Thomas96 ; Friedman96 ; Aubin98 ; Prokofev98 ; WW\_Science99 ; Yoo\_Jae00 ; Fernandez01 ; Hill02 ; Chudnovsky02 ; Fernandez02 ; Dressel03 . These systems are organometallic clusters characterized by a large spin ground state with a predominant uniaxial anisotropy. These features yield a pronounced barrier for magnetization reversal and therefore a hysteretic behavior below a blocking temperature. The quantum nature of these system makes them very appealing for phenomena occurring on the mesoscopic scale, i.e. at the boundary between classical and quantum physics. Up to now the most thoroughly investigated systems were a dodecanuclear mixed-valence manganese-oxo cluster with acetate ligands (hereafter Mn12-ac) Sessoli93b  and an octanuclear iron(III) oxo-hydroxo cluster of formula \[Fe8O2(OH)12(tacn)6\]8+ where tacn is a macrocyclic ligand, (hereafter Fe8Barra96 , both having a ground spin state $`S=10`$, but substantially differing in their anisotropy. Indeed, while the first is essentially tetragonal with a barrier of 67 K, the latter is orthorhombic with a barrier of 25 K, leading to an enhancement of the ground-state tunneling rate compared to Mn12-ac.

Recently it has also been proposed that molecular nanomagnets could be used as quantum computers by implementing Grover s algorithm Leuenberger01 . For this to occur it is necessary to be able to generate an arbitrary superpositions of eigenstates of these systems. The suggested way to do this was through the use of multifrequency coherent magnetic radiation in the microwave and radiofrequency range. This would first introduce and amplify the desired phase for each $`M`$ state and this information could be finally read-out by standard magnetic resonance techniques. In this approach advantage is taken from the non-equidistance of the $`M`$ levels of the ground multiplet arising from the large axial anisotropy of these systems, which allows coherent populations of the different $`M`$ levels. A recent theoretical work pointed out that a very accurate control of pulse shape technique, both in amplitude, duration and choice of frequency is needed to fulfill the condition to design quantum computing devices in molecular nanomagnets Zhou02 . In addition to such basic difficulties, we will see below that the microwave power cannot exceed a critical value above which non-linear effects occur. In particular the phonons associated with spin relaxation are crucially influencing the dynamics of the system.

In order to investigate the feasibility of the proposed process any preliminary experiment should aim to understand the effects of microwave absorption on the spin dynamics of these systems at low temperature. The main issues addressed in this letter concern: (i) controlled increasing of excited state populations through the absorption of microwave radiation, (ii) mechanism of photon-assisted tunneling, and (iii) subsequent heating occurring after relaxation.

The measurements were performed on a new magnetometer, involving 10 $`\times `$ 10 $`\mu `$m2 micro-Hall bars Kent94 ; Kent00b  in a dilution refrigerator equipped with three coils allowing to apply a field in any direction, at sweeping rates up to 1 T/s. Continuous radiation, in the FIR region, was generated by a couple of Gunn diodes (Radiometer Physics GmbH), working at fundamental frequencies of 95 GHz and 115 GHz, and equipped with double and triple harmonic generators and calibrated attenuators. We irradiated the sample using a 6 mm waveguide equipped with infrared filters in order to reduce heating. The circular polarization, induced by filters, was maximized around 97%. The study was performed on a 0.1 mm Fe8 single crystal synthesized according to the standard procedure.

As schematically depicted in Fig. 1, microwave radiation with a frequencies of 115 GHz corresponds to the energy separation between the ground states $`M=\pm S`$ and the first excited states $`M=\pm (S1)`$ of Fe8 in zero applied magnetic field Barra96 ; Hill02 . If the radiation is linearly polarized, the populations of the first excited states ($`M=\pm (S1)`$) in both wells will be enhanced equally (equal transition probability for $`\mathrm{\Delta }M=\pm 1`$). On the opposite, the use of circular polarization has the advantage to distinguish between $`\mathrm{\Delta }M=+1`$ (left polarization, $`\sigma ^{}`$ photons) or $`\mathrm{\Delta }M=1`$ (right polarization, $`\sigma ^+`$ photons) Abragam70 , and the population of only one of the two excited states will be enhanced (Fig. 1). An excess of tunneling from one well to the other is then expected. Therefore, circular polarization can help to distinguish between spin-phonons relaxation, and spin-phonons relaxation modified by the absorption of photons. The first equally affect the two sides of the barrier, i.e. the two branches of the hysteresis loop, while the second modifies the population of only one side of the barrier, i.e. one branch of the hysteresis loop. Any difference observed between the two branches of the hysteresis loop, has to be traced back to photon absorption.

Fig. 2a shows the hysteresis loops of a Fe8 single crystal with the easy axis parallel to the applied field, measured at 60 mK under irradiation. The tunneling transition near zero field is strongly enhanced for a radiation at 115 GHz. This is in agreement with a photon induced population transfer from $`M=10`$ to $`M=9`$, and agrees with earlier HF-EPR studies showing strong zero field absorption at about 116 GHz Barra96 ; Hill02 . Fig. 2a also shows the expected asymmetry of the hysteresis loops in the presence of circularly polarized radiation. In particular, the height of the zero-field step (first tunnel resonance, $`n=0`$), obtained when sweeping the field from negative saturation, is much less affected than when sweeping from positive saturation. Besides, the effect of a radiation at 95 GHz (Fig. 2b) with no level matching is quite comparable to that of temperature (Fig. 2c) (heating induced by large power irradiation). These results establish clearly that tunneling is assisted by photons for the matching frequency of 115 GHz. Similar qualitative effects were also observed in a field of 0.22 T, corresponding to the second tunnel resonance ($`n=1`$).

For the quantitative study of the power dependence of photons-induced tunneling, we first cooled the sample from 5 K down to 0.04 K in a field of $`H_z`$ = 1.4 T yielding a positive saturated magnetization state. Then, in the presence of continuous microwave radiation at 115 GHz and power $`\rho `$, we swept the applied field at a constant rate over the zero field resonance transition and measured the fraction of molecules which reversed their spin. This procedure yields the total tunnel probability $`P(\rho )`$. The photon induced tunneling probability $`P_{EPR}(\rho )`$ was evaluated from:

$$P_{EPR}(\rho )=P(\rho )n_{10}P_{\pm 10}$$
(1)
where the ground state tunnel probability $`n_{10}P_{\pm 10}`$ was measured in the absence of radiation WW\_EPL00 . The obtained $`P_{EPR}(\rho )`$ first increases linearly with $`\rho `$ and then becomes highly non-linear (Fig. 3).

In order to give a simple explanation of the observed behavior, we developed a scenario in which the spin temperature increases rapidly with the absorbed microwave power. We used the generalized master equation formalism as described by Leuenberger and Loss Leuenberger00  but with photon induced transition probabilities $`\mathrm{\Gamma }_{\mathrm{RF}}`$ between the energy states $`M=\pm S`$ and $`\pm (S1)`$. At low temperature ($`T<<1`$ K), it is sufficient to consider only the six lowest levels (Fig. 1) with occupation numbers $`n_M`$ where $`M=\pm S,\pm (S1),\pm (S2)`$. As initial condition we have chosen positive saturation of the sample, i.e. $`n_SN`$, where N is the number of molecules. We yield for small microwave power $`\rho `$ and $`P_{EPR}<<1`$:

$$P_{EPR}\frac{2\mathrm{\Gamma }_{\mathrm{RF}}\mathrm{\Delta }_{\pm 9}}{9g\mu _\mathrm{B}\mu _0dH_z/dt}+\underset{M=9,8}{}\frac{\mathrm{\Delta }_{\pm M}e^{E_{10,M}/k_BT_S}}{\tau _Mg\mu _\mathrm{B}M\mu _0dH_z/dt}$$
(2)
where $`\tau _M`$ is the lifetime of the excited level $`M`$, $`E_{10,M}`$ is the energy gap between the levels $`10`$ and $`M`$, $`\mathrm{\Delta }_{\pm M}`$ is the tunnel splitting of the levels $`\pm M`$, and $`T_S`$ is the spin temperature. All constants of this model were found by measuring the overall transition rate via excited spin levels $`P_{th}(T)`$ due to thermal activation, as described in WW\_EPL00 . The spin temperature $`T_S`$ were determined by mapping $`P_{EPR}(\rho )`$ onto $`P_{th}(T)`$ such as $`P_{EPR}(\rho )=P_{th}(T_0=T_S)`$ (Fig. 4). We obtained a nearly linear variation of $`T_S`$ versus $`\rho `$ (inset of Fig. 3).

The energy transfer from the spin system to the thermostat involves contributions of the electromagnetic radiation bath, the phonon bath and the spin bath. However, at low temperatures ($`T<1`$ K) the phonon specific heat is vanishingly small and the photon bath completely negligible. The specific heat $`C_S`$ of the spin bath is greatly influenced by weak dipolar fields giving a flat distribution of Schottky anomalies with a nearly constant specific heat Gomes98 ; Mettes01 . The electromagnetic power absorbed by the spin system, $`dW/dt=\mathrm{}\omega (1n_{S1}/N)\mathrm{\Gamma }_{\mathrm{RF}}\mathrm{}\omega \mathrm{\Gamma }_{\mathrm{RF}}`$ Abragam70 , passes to the thermostat via spin–lattice and spin–spin relaxation. The effect of the latter should be more important due to their larger specific heat. Neglecting the phonon specific heat, the heat transfer equation can be written:

$$dW/dt=C_SdT/dt+C_S(T_ST_0)/\tau _S$$
(3)
where $`T_0`$ is the cryostat temperature and $`\tau _S`$ is a diffusion time for magnetic excitations. At equilibrium $`(dT/dt=0)`$, the spin-bath temperature is therefore $`T_S=T_0+\mathrm{}\omega \mathrm{\Gamma }_{\mathrm{RF}}\tau _S/C_S`$. Because $`C_S`$ is almost temperature independent between 0.3 and 0.8 K Gomes98 ; Mettes01 , $`T_S`$ increases nearly linearly with the microwave power which is in good agreement with our observation (inset of Fig. 3).

Finally, the microwave absorption at 95 GHz and for $`n=1`$ at 115 GHz might be due to spin–spin interactions which broaden strongly the energy levels. Such a broadening has already been observed by EPR linewidth measurements Hill02  and spin–spin cross–relaxation measurements Giraud01 ; WW\_PRL02 .

In conclusion, the use of circularly polarized microwaves allowed us to show for the first time the phenomenon of photon-assisted tunneling in magnetism, using a single molecule magnet Fe8. In accordance with the selection rules for EPR spectroscopy Abragam70 , circularly polarized radiation promotes the transition $`M`$ = -10 to -9 with $`\mathrm{\Delta }M`$ = +1, giving an effect of magnetic dichroism at millimeter wavelengths. At lowest microwave powers, the tunnel probability increases linearly with the power, whereas at higher powers we enter in a non-linear regime resulting from an increase of the spin temperature $`T_S`$.

This work was supported by the European Union TMR network MOLNANOMAG, HPRN-CT-1999-0012.


text:
# Mathematical Features of continuity equation

## 1 introduction

In 2002 the author devised a method for solving nonlinear differential equations. Using this method one can solve many important non linear differential equations in physics.
In an endeavor to solve hydrodynamical equations governing the interstellar media, we came to a very important result about continuity equation. This result helped us to find exact solutions for hydrodynamical equations in an straightforward and simple way.
In the following section we will write the result in the form of a theorem. Although we have come to the result using the new method, but in proving the theorem we do not use our method. what we will do is simply substituting the driven result in continuity equation.

## 2  Theorem

For all density and velocity Functions in the Form, $`\rho =\rho (G(f(x,y,z,t)))`$ and $`\stackrel{}{v}=\stackrel{}{v}(G(f(x,y,z,t)))`$ the continuity equation, $`\frac{\rho }{t}+.(\rho \stackrel{}{v})=0`$ can be written as an ordinary equation if, $`f(x,y,z,t)=\alpha x+\beta y+\gamma z+\lambda t`$.
Here $`G(f)`$ is any arbitrary function of $`f`$.
Proof:
According to the stated conditions, Continuity equation can be written as,

$$\frac{d\rho }{dG}\frac{dG}{df}\frac{f}{t}+\frac{dG}{df}\frac{d(\rho \stackrel{}{v})}{dG}.\stackrel{}{}f=0.$$
(1)
As a result we will have,

$$\lambda \frac{d\rho }{dG}+\frac{d}{dG}(\rho \stackrel{}{v}).(\alpha \widehat{i}+\beta \widehat{j}+\gamma \widehat{k})=0$$
(2)
Integrating from both sides of the above equation will result in;

$$\rho +\rho \stackrel{}{v}.\widehat{\kappa }=c$$
(3)
c is a constant of integration and

$$\widehat{\kappa }=\alpha \widehat{i}+\beta \widehat{j}+\gamma \widehat{k}.$$
(4)
Therefore in these cases we can always write $`\rho `$ in terms of $`\stackrel{}{v}`$ as;

$$\rho =\frac{c}{1+\stackrel{}{v}.\widehat{\kappa }}.$$
(5)
## 3 discussion

Although very simple, we believe that this result is an important result; Firstly, because we used this to find out explicit solution for Naiver stokes equations in cases that had not been solved previously(2). secondly, there is always a probability that, from explicit solutions one may come to physical results that could not be driven out from numerical analysis. At present, those who are concerned with nonlinear physical applications, containing continuity equation, use numerical methods for describing different physical phenomena. One may check out the above result for new out comes.

## 4 references

1-S.Otarod and J.Ghanbari, Separation of variables for a nonlinear Differential Equations. Electronic Journal of Differential Equations, Problem section. 2002-2.
2-S.Otarod and J.Ghanbari, Analytical Solution Of Hydrodynamical Equations. The common project of Razi and Ferdowsi University. Phys.Depts of Razi and Ferdowsi University. Iran. 2003.


text:
# Nanomechanical Analog of a Laser: Amplification of Mechanical Oscillations by Stimulated Zeeman Transitions

## Abstract

We propose a magnetomechanical device that exhibits many properties of a laser. The device is formed by a nanocantilever and dynamically polarized paramagnetic nuclei of a solid sample in a strong external magnetic field. The corresponding quantum oscillator and effective two-level systems are coupled by the magnetostatic dipole-dipole interaction between a permanent magnet on the cantilever tip and the magnetic moments of the spins, so that the entire system is effectively described by the Jaynes–Cummings model. We consider the possibility of observing transient and cw lasing in this system, and show how these processes can be used to improve the sensitivity of magnetic resonance force microscopy.

The invention of masers and lasers in the middle of the twentieth century firstlaser  has engendered whole new fields of science and myriads of applications. This success of laser science and technology demonstrates the value of the basic principles of laser devices and encourages one to look for other systems in which these principles can be realized.

Regardless of the frequency range and other details of a practical implementation, all laser-like devices involve one or more quantum-mechanical oscillators resonantly interacting with a continuously pumped multilevel quantum system. In the ubiquitous optical laser, the oscillator is realized by a mode of a high-Q electromagnetic cavity, a mode resonant with optical transitions of bound electrons in the active medium. Masers use microwave transitions of gas molecules or electron spins of a paramagnetic solid in a strong magnetic field. Finally, the active medium of a free-electron laser is a relativistic electron beam, whose energy levels can be defined by a specially configured magnetic field fel .

This relative diversity of possible realizations of the active medium is not, however, matched by the demonstrated realizations of the other essential part of a lasing system, the oscillator. The authors are aware of only one laser-like device that used an oscillator different from a field mode of an electromagnetic cavity—the nuclear-magnetic-resonance (NMR) laser nuclearchaos . In that device, nuclear spins of a solid sample were inductively coupled to a resonant LC circuit. Although many properties of an LC circuit are strikingly different from those of a cavity resonator, one can argue that the underlying physics in the two cases is the same: The oscillations correspond to normal modes of a complex electromagnetic system, whether it consists of an electromagnetic field confined by reflecting walls or of coupled electric and magnetic fields of capacitive and inductive elements.

In this Letter, we propose a laser-like device in which the oscillator is realized by a fundamentally different kind of a device—a nanomechanical resonator, e.g., a nanoscale cantilever or doubly clamped beam. Recent advances in nanofabrication and detection techniques have pushed the fundamental-mode frequencies of nanomechanical oscillators to the microwave range henry\_1GHz , approaching the point where their properties begin to be limited by quantum effects quantum . In addition, micro- and nanoelectromechanical oscillators generally exhibit low noise and high quality factors, which naturally has led to applications for integrated high-frequency signal generation and processing mems . These properties make it possible to use long-term coherent response of a high-frequency nanomechanical oscillator in a laser-like device.

Similarly to the case of NMR laser and solid-state masers, we propose to use nuclear or electron spins in a strong external magnetic field as the active medium of a “mechanical laser”. A nanomechanical oscillator can be effectively coupled to the magnetic moments of such spins by incorporating a small ferromagnetic tip on its surface. At microscopic distances between the cantilever and the sample, the coupling between the tip and the spins is essentially magnetostatic.

Systems consisting of a micro- or nanomechanical cantilever coupled to resonant magnetic spins of a solid sample have been extensively studied in the context of magnetic resonance force microscopy (MRFM) mrfm\_rev . However, in all MRFM experiments performed so far, the fundamental frequency of the cantilever was orders of magnitude below the Larmor frequency of the magnetic spins. Resonant transfer of energy quanta from spins to the mechanical oscillator is impossible in this case. Therefore, the resonance is achieved by using an RF or microwave field to modulate the sample magnetization at the cantilever frequency mrfm\_rev .

For the device proposed here, it is essential that the motion of the mechanical oscillator be resonantly coupled to the free precession of magnetic spins, which means that the frequency of the used mechanical mode must be close to the Larmor frequency of the sample sidles92 . For conventional experiments with external magnetic fields of a few Tesla, the Larmor frequencies are of the order of tens of megahertz and tens of gigahertz for nuclear and electron magnetic resonance, respectively slichter . Given that the highest fundamental-mode frequency of nanomechanical oscillators measured so far is slightly above 1 GHz henry\_1GHz , resonant coupling between mechanical oscillators and electron spins in strong magnetic fields seems unfeasible at this time. Operation in low magnetic fields, on the other hand, would prevent complete polarization of electrons and make the system more sensitive to ambient magnetic fields. In the rest of this Letter, we will therefore concentrate on the case involving nuclear spins.

Figure 1 shows a schematic of the proposed device. A nanomechanical oscillator—a cantilever in this case—is positioned near a sample that contains precessing nuclear spins, some of which are shown schematically in the figure. A ferromagnet on the cantilever tip creates a magnetic field, which can be approximated as the field of a magnetic dipole. When superposed on the uniform external field $`𝐁_\mathrm{𝟎}`$, this field modifies the total magnetic field seen by nuclear spins and, therefore, their Larmor frequency. As a result, only a certain slice of the sample, known as the sensitive slice, will have the Larmor frequency resonant with the frequency of the used mode of the cantilever mrfm\_rev .

The rotating transverse component of nuclear magnetization couples to the ferromagnetic tip via a dipolar magnetostatic interaction, with the resulting force driving cantilever oscillations. Conversely, a moving ferromagnet creates an AC magnetic field, oscillating at the frequency of the cantilever motion, inside the sample. This RF field can drive transitions between Zeeman levels of nuclear spins—stimulated transitions in the language of standard rate-equation laser theory. The resulting coupled interaction—spins driving the cantilever and the cantilever, in turn, driving the spins—leads to a kind of positive feedback that arises in all laser-like systems.

Although a variety of nanomechanical devices could be used—involving, for example, torsional or flexural modes—we focus here on nanocantilevers, which are especially convenient for scanning with small tip-sample separations. The device we propose can then be aptly termed a “cantilaser”. To provide a concrete example, we will assume the following parameters for the cantilever: fundamental-mode frequency $`\omega _c/2\pi =20`$ MHz, effective spring constant $`k_c=0.1`$ N/m, quality factor $`Q=10^5`$, the transverse magnetic field gradient (due to the ferromagnetic tip) $`\frac{𝐁_{}(𝐫)}{x}=1`$ G/Å$`=10^6`$ T/m within the sensitive slice. This magnetic field gradient can be created by a rare-earth-metal magnet at a distance of about 1 micron high\_grad\_MRFM . At such relatively large distances, one can usually neglect all nonmagnetic interactions between the cantilever and the sample. Note also that the intrinsic Q factor of a nanomechanical oscillator can be effectively increased by a few orders of magnitude using positive feedback pos\_feedback  or parametric pumping darrel .

For the parameters of the nuclear spin subsystem, we will take values representative of crystalline materials slichter : transverse relaxation time $`T_2=50\mu `$s and nuclear gyromagnetic ratio $`\gamma _n=2\pi \times 10`$ MHz/T. The bulk of the sample material will be resonant with the cantilever oscillations in an external field of $`B_0=\omega _c/\gamma _n=2`$ T.

In order to observe lasing in any system, one must introduce a pumping mechanism to compensate for the energy dissipated in both the oscillator and the active medium. For nuclear spins, such pumping can be produced by dynamic nuclear polarization (DNP) slichter . In this mechanism, microwave or optical radiation is used to saturate an electron transition, causing them to preferentially absorb photons of only one circular polarization. Some of the absorbed angular momentum is then transferred from the electrons to the nuclei of the sample through various equilibration processes. This technique has been successfully employed to pump the NMR laser at the liquid helium temperature (4.2 K) using a microwave source as in Fig. 1, with the effective pumping time as low as $`T_p=0.2`$ s nuclearchaos . We will use this pumping rate and the equilibrium longitudinal polarization $`M_{eq}=0.3`$ that is achievable in a 2-Tesla external field.

The dynamics of the cantilaser can be described by the Hamiltonian

$$\widehat{H}=\mathrm{}\omega _c\widehat{a}^{}\widehat{a}+\mathrm{}\gamma _n\underset{i}{}𝐁_i\widehat{𝐒}_i+\mathrm{}(\widehat{a}^{}+\widehat{a})\underset{i}{}2𝐠_i\widehat{𝐒}_i+\widehat{H}_r,$$

where $`a^{}`$ and $`a`$ are the creation and annihilation operators of the cantilever mode, $`\widehat{𝐒}_i`$ is the spin operator of $`i`$th nucleus, $`\widehat{𝐁}_i`$ is the the external field at the site of the $`i`$th spin, $`𝐠_i=\frac{\gamma _n}{2}\frac{𝐁(𝐫_i)}{x}\sqrt{\frac{\mathrm{}\omega _c}{2k_c}}`$ is the vector constant of the coupling between the $`i`$th spin and the cantilever, and $`\widehat{H}_r`$ describes relaxation-inducing couplings to the environment. This Hamiltonian was first considered by Jaynes and Cummings, who used it describe quantum behavior of masers jcmodel . In the same paper, they also showed that the corresponding dynamics can usually be described by semiclassical equations, which treat the resonator classically and the spins quantum mechanically.

Considering the nuclear spins in their respective rotating frames (as defined by the local field $`𝐁_i`$ and field gradient $`\frac{𝐁(𝐫_i)}{x}`$ sidles92 ) and using the slowly-varying-amplitude approximation for the cantilever, we can write such semiclassical equations in the form

$$\begin{array}{c}\dot{A}+\kappa A=gNM_{},\hfill \\ \dot{M_{}}+\mathrm{\Gamma }_{}M_{}=gM_zA,\hfill \\ \dot{M_z}+\mathrm{\Gamma }_{}(M_zM_{eq})=g(M_{}A^{}+M_{}^{}A)/2,\hfill \end{array}$$
(1)
where $`A`$ is the (generally complex) amplitude of cantilever oscillations, normalized by the amplitude, $`\sqrt{\mathrm{}\omega _c/(2k_c)}2.610^{13}`$ m, of zero-energy quantum motion, $`\kappa =\omega _c/2Q630\mathrm{s}^1`$ is the cantilever decay rate, $`N`$ is the number of resonant spins in the sensitive slice, $`M_{}`$ and $`M_z`$ are the normalized ($`|M_{}|^2+M_z^21`$) transverse and longitudinal (with respect to $`𝐁_\mathrm{𝟎}`$) components of nuclear polarization, $`\mathrm{\Gamma }_{}=T_2^1=2010^3\mathrm{s}^1`$ and $`\mathrm{\Gamma }_{}=T_p^1=5\mathrm{s}^1`$ are the effective transverse and longitudinal polarization relaxation rates, and $`g=\frac{\gamma _n}{2}\left|\frac{𝐁_{}(𝐫)}{z}\right|\sqrt{\frac{\mathrm{}\omega _c}{2k_c}}8.0\mathrm{s}^1`$ is the scalar coupling constant of the interaction between the cantilever and the nuclear spins.

In equations (1) we implicitly assumed that all resonant nuclei in the sensitive slice are spin-half and that they all see the same strength and gradient of the magnetic field. The latter is an obvious simplification since in MRFM experiments, the magnetic-resonance frequency and coupling strength varies continuously over the sensitive slice suter . However, the same problem of inhomogeneous broadening and nonuniform coupling arises in most quantum optics and laser setups haken , and it was found experimentally haroche83 ; kimble95  that equations of the form (1) still correctly reproduce most features of the coupled spin–oscillator dynamics. In this Letter, we will therefore restrict our analysis to the simplest model of Eqs. (1)

It is easy to find the steady-state solutions of Eqs. (1). The nontrivial lasing solution may exist only in the case of population inversion, $`M_{eq}<0`$, and is given by $`A_{cw}=\sqrt{(N|M_{eq}|N_t)\mathrm{\Gamma }_{}/\kappa },`$ where $`N_t=\kappa \mathrm{\Gamma }_{}/g^2`$ is the threshold population inversion. Substituting $`M_{eq}=0.3`$ and other parameter values given above, we find that in order to support cw lasing, the number of atoms in the sensitive slice should be $`N>N_{cw}=N_t/|M_{eq}|0.6510^6`$. This may seem like a large number; however, even an atomically thin sensitive slice of a homogeneous sample contains of the order of $`10^7`$ nuclei if the diameter of the sensitive slice is just $`1\mu `$m. Much larger sensitive slices have been used in nuclear MRFM experiments so far, so exceeding the lasing threshold seems quite feasible.

One of the more interesting transient phenomena predicted by the Jaynes–Cummings model is the coherent oscillation of population between the oscillator and spins jcmodel , an effect similar to the oscillations of energy between two weakly coupled classical harmonic oscillators. Also known as ringing superradiance, this phenomenon has been observed in different quantum-optical systems haroche83 ; kimble95 . In order for the energy oscillations to be observable in a cantilaser, the effective frequency of the oscillations, equal to $`\sqrt{|M_{eq}|N}g`$ jcmodel , should be larger than the fastest relaxation rate of the system, $`\mathrm{\Gamma }_{}`$. We can therefore roughly estimate the minimum number of atoms necessary to observe the oscillations as $`N_{sr}=\mathrm{\Gamma }_{}^2/(|M_{eq}|g^2)2010^6`$. As we show below, our numerical simulations support the validity of this estimate.

Another interesting transient predicted by the Jaynes-Cummings model is a solitary pulse that irreversibly depletes the energy stored in the active medium. Known as giant pulses in the standard laser theory haken , these transients can appear if $`\mathrm{\Gamma }_{}>|M_{eq}|Ng^2/\mathrm{\Gamma }_{}>\kappa `$, which implies $`N_{sr}>N>N_{cw}`$. Such a giant pulse reduces the population inversion to zero and therefore consumes one half of the total potential energy of the active medium (i.e., the sensitive slice, which can in principle be adjusted to encompass most of the sample suter ). This is in contrast to the case of ringing superradiance, where all of the available energy oscillates back and forth between the cantilever and spins.

Figure 2 shows three characteristic transient outputs of a cantilaser, obtained by numerical integration of Eqs. (1). As the number of resonant nuclei in the sensitive slice decreases from $`N=20010^6N_{sr}`$ to $`N=510^6N_{sr}`$, the frequency and amplitude of energy oscillations decreases until just one “giant” pulse is observed. If one further keeps decreasing the number of atoms, the single pulse becomes longer and smaller in amplitude until it disappears completely as the number of atoms goes below the cw lasing threshold $`N_{cw}`$. Note that the tails of the output transients always decay at the time scale of $`\kappa ^1`$ because cantilever decay is the dominant mechanism of energy dissipation here. In contrast, the coherent oscillations, if present at all, decay at the time scale of $`\mathrm{\Gamma }_{}^1=T_2`$ since spin-spin relaxation is the dominant mechanism for the loss of coherence.

The initial conditions for pulsed transients used in the simulations of Fig. 2 can be produced by a Q-switching technique haken . Note that the initial nuclear polarization, $`M_{}(0)=0,M_z(0)=M_{eq}`$, is simply the equilibrium polarization achieved in the presence of dynamic nuclear pumping and negligible interaction with the cantilever. Also, the initial cantilever amplitude corresponds to thermal vibrations of the cantilever at the temperature $`T=4.2`$ K: $`A(0)=A_{th}=\sqrt{2k_BT/(\mathrm{}\omega _c)}94`$, where $`k_B`$ is the Boltzmann constant.

Since a cantilaser shares so much in its design and principles of operation with MRFM setups, it is natural to consider whether the effects describe above can be used to improve the sensitivity of nuclear MRFM. The single-shot sensitivity of the first nuclear MRFM experiment rugar94  was approximately $`10^{13}`$ thermally polarized nuclear spins at room temperature or about $`10^{11}`$ nuclear spins at 4.2 K (nuclear polarizability is inversely proportional to temperature). Since then, the sensitivity of MRFM experiments has been improved to about 100 Bohr magnetons 100spins , a magnetic moment that is created by roughly $`10^8`$ nuclear spins at 4.2 K. The closest competing technology—scanning SQUID-based magnetometry—has so far demonstrated a sensitivity of $`10^5`$ Bohr magnetons squidNMR , or $`10^{11}`$ nuclear spins at 4.2 K.

To consider the MRFM sensitivity of a cantilaser, we will calculate the ratio of power spectral density of lasing outputs to the power spectral density of thermomechanical noise. Since the resonant frequency of the cantilever and the Zeeman transition frequency of spins coincide, we can express all energy quantities in terms of the number of energy quanta $`\mathrm{}\omega _c`$. The power of the thermomechanical noise is then proportional to $`n_{th}=A_{th}^2/2=k_BT/(\mathrm{}\omega _c)4400`$, and its bandwidth is $`\mathrm{\Delta }\omega _{th}=\kappa `$. Well above the lasing threshold, the power of the cw lasing signal is $`n_{cw}=A_{cw}^2/2\mathrm{\Gamma }_{}N|M_{eq}|/(2\kappa )N/840`$, and its bandwidth is $`\mathrm{\Delta }\omega _{cw}\kappa (n_{th}+1/2)/n_{cw}`$ haken . The signal-to-noise ratio for the cw output is then $`SNR_{cw}=\frac{n_{cw}/\mathrm{\Delta }\omega _{cw}}{n_{th}/\mathrm{\Delta }\omega _{th}}\left(n_{cw}/n_{th}\right)^2\left(N/3.710^6\right)^2`$. The quadratic increase in $`SNR_{cw}`$ with the number of atoms reflects the spectral narrowing of the cw signal at high output power, a fact that is well known and used in optical lasers haken .

For both kinds of pulsed outputs we considered (ringing superradiance and single pulses), the efficiency of the energy transfer from spins to the cantilever mode is of the order of unity. The peak cantilever amplitude of a pulse in both cases then corresponds to mode population of about $`n_{pulse}=N|M_{eq}|/2`$. Since all pulsed outputs eventually decay at the time scale of $`\kappa ^1`$, their bandwidth can be taken to be $`\mathrm{\Delta }\omega _{pulse}\kappa `$. Proceeding as above, we find $`SNR_{pulse}=N|M_{eq}|/(2n_{th})N/29000`$. A cantilaser operating in the pulsed mode would therefore have a single-shot sensitivity of about $`310^4`$ nuclear spins at 4.2 K, which is at least three orders of magnitude better than the sensitivity of any existing alternative. A large part of this improvement derives from the hyperpolarization of nuclei by DNP processes, but the near-unity efficiency of energy transfer between spins and cantilever in pulsed transients is also significant.

We conclude by considering different possible perspectives upon mechanical lasing—from the standpoints of quantum optics, NMR spectroscopy, and MRFM. From the perspective of quantum optics, the cantilaser is very similar to a cavity QED system cqed , albeit one with weak but comparable coupling strength and longitudinal relaxation, $`g\mathrm{\Gamma }_{}(\mathrm{\Gamma }_{},\kappa )`$, and high thermal population, $`n_{th}1`$. Since such combinations of parameters are not available in quantum optical systems or NMR laser, this opens up new possibilities for studying coherent quantum phenomena in coupled oscillator–atom systems.

In conventional NMR studies, the possibility of a positive feedback between the sample and the detecting resonance circuit has been long recognized. Bloembergen first considered the back action of the detecting coil on the sample almost 50 years ago bloembergen54 . Unfortunately, such back action tends to shorten the signal pulses and therefore broaden spectral features. This explains why this positive-feedback effect, known to NMR practitioners as radiative damping, is generally undesirable in high-resolution NMR spectroscopy. In contrast, MRFM experimentalists are not interested in fine details of NMR spectra. Since the ultimate goal of MRFM is atom-by-atom 3D mapping of nanoscopic objects, the required spectral resolution should only be sufficient to distinguish between different nuclear species. MRFM practitioners are therefore willing to trade fine spectral resolution for signal strength and spatial resolution. This is exactly what a mechanical laser provides, by embracing and fully exploiting the positive feedback in the coupled oscillator–spin system.

We are grateful for support of this work from DARPA DSO/MOSAIC under ONR grant N00014-02-1-0602, and from the NSF under grant ECS-0116776. We also thank Ed Myers and John Sidles for helpful comments.