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# Multiparty Quantum Coin Flipping

## 1 Introduction

### 1.1 The problem

Consider $`k`$ parties out of which at least $`g1`$ are honest and at most $`(kg)`$ are dishonest; which players are dishonest is fixed in advance but unknown to the honest players. The players can communicate over broadcast channels. Initially they do not share randomness, but they can privately flip coins; the probabilities below are with respect to the private random coins. A coin-flipping protocol establishes among the honest players a bit $`b`$ such that

* if all players are honest, $`\mathrm{Pr}[b=0]=\mathrm{Pr}[b=1]=\frac{1}{2}`$
* if at least $`g`$ players are honest, then $`\mathrm{Pr}[b=0],\mathrm{Pr}[b=1]\frac{1}{2}+\epsilon `$

$`\epsilon `$ is called the bias; a small bias implies that colluding dishonest players cannot strongly influence the outcome of the protocol. Players may abort the protocol.

### 1.2 Related work

Classically, if a (weak) majority of the players is bad then no bias $`<\frac{1}{2}`$ can be achieved and hence no meaningful protocols exist . For example, if we only have two players and one of them is dishonest, then no protocols with bias $`<\frac{1}{2}`$ exist. For a minority of bad players, quite non-trivial protocols exist. For example, Feige  elegantly showed that $`(\frac{1}{2}+\delta )`$-fraction of good players can achieve bias $`\frac{1}{2}\mathrm{\Omega }(\delta ^{1.65})`$, while achieving bias better than $`\frac{1}{2}\delta `$ is impossible.

Allowing quantum bits (qubits) to be sent instead of classical bits changes the situation dramatically. Surprisingly, already in the two-party case coin flipping with bias $`<\frac{1}{2}`$ is possible, as was first shown by Aharonov et al. . The best known bias is $`\frac{1}{4}`$ and this is optimal for a special class of three-round protocols ; for a bias of $`\epsilon `$ at least $`\mathrm{\Omega }(\mathrm{log}\mathrm{log}\frac{1}{\epsilon })`$ rounds of communication are necessary . Kitaev (unpublished, see ) showed that in the two-party case no bias smaller than $`\frac{1}{\sqrt{2}}\frac{1}{2}`$ is possible.

A weak version of the coin-flipping problem is one in which we know in advance that outcome 0 benefits Alice and outcome 1 benefits Bob. In this case, we only need to bound the probabilities of a dishonest Alice convincing Bob that the outcome is 0 and a dishonest Bob convincing Alice that the outcome is 1. In the classical setting, a standard argument shows that even weak coin flipping with a bias $`<\frac{1}{2}`$ is impossible when a majority of the players is dishonest. In the quantum setting, this scenario was first studied under the name quantum gambling . Subsequently, Spekkens and Rudolph  gave a quantum protocol for weak coin flipping with bias $`\frac{1}{\sqrt{2}}\frac{1}{2}`$ (i.e., no party can achieve the desired outcome with probability greater than $`\frac{1}{\sqrt{2}}`$). This was recently improved to $`0.192`$ by Mochon . Notice that this is a better bias than in the best strong coin flipping protocol of .

We also remark that Kitaev’s lower bound for strong coin flipping does not apply to weak coin flipping. Indeed, Mochon’s protocol has a better bound than Kitaev’s lower bound. Thus, weak protocols with arbitrarily small $`\epsilon >0`$ may be possible. The only known lower bounds for weak coin flipping are that the protocol of  is optimal for a restricted class of protocols  and that a protocol must use at least $`\mathrm{\Omega }(\mathrm{log}\mathrm{log}\frac{1}{\epsilon })`$ rounds of communication to achieve bias $`\epsilon `$ (shown in  for strong coin flipping but the proof also applies to weak coin flipping).

### 1.3 Our contribution

In this paper, we focus on quantum coin flipping for more than two players. However, for our multiparty quantum protocols we will first need a new two-party quantum protocol for *coin flipping with penalty for cheating*. In this problem, players can be heavily penalized for cheating, which will allow us to achieve lower cheating probability as a function of the penalty. This primitive and the quantum protocol for it are presented in Section 2; they may be of independent interest.

One way to classically model communication between more than two parties is by a primitive called *broadcast*. When a player sends a bit to the other players he broadcasts it to all the players at once . However, when we deal with qubits such a broadcast channel is not possible since it requires to clone or copy the qubit to be broadcast and cloning a qubit is not possible . In Section 3 we develop a proper quantum version of the broadcast primitive, which generalizes the classical broadcast. Somewhat surprisingly, we show that our quantum broadcast channel is essentially as powerful as a combination of pairwise quantum channels and a classical broadcast channel. This could also be of independent interest.

Using this broadcast primitive we obtain our main result:

###### Theorem 1

For $`k`$ parties out of which $`g`$ are honest, the optimal achievable bias is $`(\frac{1}{2}\mathrm{\Theta }(\frac{g}{k}))`$.

We prove Theorem 1 by giving an efficient protocol with bias $`(\frac{1}{2}\mathrm{\Omega }(\frac{g}{k}))`$ in Section 4 and showing a lower bound of $`(\frac{1}{2}\mathrm{O}(\frac{g}{k}))`$ in Section 5. Our protocol builds upon our two-party coin-flipping with penalties which we develop in Section 2, and the classical protocol of Feige  which allows to reduce the number of participants in the protocol without significantly changing the fraction of good players present. Our lower bound extends the lower bound of Kitaev .

To summarize, we show that quantum coin flipping is significantly more powerful than classical coin flipping. Moreover, we give tight tradeoffs between the number of cheaters tolerated and the bias of the resulting coin achievable by quantum coin-flipping protocols. We also remark that the fact that we obtain tight bounds in the quantum setting is somewhat surprising. For comparison, such tight bounds are unknown for the classical setting.

In the remainder of the paper, we assume some familiarity with quantum computing. We recommend the book of Nielsen and Chuang  for background information on this topic.

### 1.4 Semidefinite programming

Some of our proofs make use of duality in semidefinite programming. For a review of semidefinite programming, see e.g., . Semidefinite programming is a generalization of linear programming. In addition to linear constraints, semidefinite programs (SDPs) may have constraints that require that a square matrix of variables is positive semidefinite, i.e., that is is symmetric and all its eigenvalues are nonnegative.

We make use of the following basic properties of semidefinite matrices. Let $`A`$, $`B`$, and $`C`$ denote square matrices acting on some linear space $`𝒱`$ and $`𝒲𝒱`$ a subspace. If $`A`$ is positive semidefinite, we write $`A0`$. We define $`AB:AB0`$. Then

$$AB|\psi :\psi |A|\psi \psi |B|\psi $$

$$A=B+C\text{ and }C0AB$$

$$AB\mathrm{tr}_𝒲(A)\mathrm{tr}_𝒲(B)$$

Here $`\mathrm{tr}_𝒲(A)`$ denotes the partial trace.

In the Lagrange-multiplier approach, a constrained optimization problem (called the *primal* problem)

$$\underset{x0}{\mathrm{max}}f(x)\text{ subject to }g(x)a\text{for fixed }a>0$$

is reformulated as an unconstrained optimization problem

$$\underset{x}{\mathrm{max}}\underset{\lambda 0}{inf}f(x)\lambda (g(x)a),$$

which is bounded from above by the constrained optimization problem (the *dual* problem)

$$\underset{\lambda 0}{\mathrm{min}}\lambda a\text{ subject to }(f\lambda g)(x)0\text{ for all }x0.$$

In linear programming, $`(f\lambda g)(x)0`$ for all $`x0`$ if and only if $`f\lambda g0`$. Therefore the preceding optimization problem can be simplified to

$$\underset{\lambda 0}{\mathrm{min}}\lambda a\text{ subject to }f\lambda g0.$$

The same construction applies to SDPs using matrices as variables and $`AB:=\mathrm{tr}(A^{}B)`$. A feasible solution of the dual yields an upper bound on the optimal value of the primal problem. Strong duality (i.e., that the optimal values coincide) does not hold in general; however, we will not need this below.

## 2 Two-party coin flipping with penalty for cheating

We consider the following model for coin flipping. We have two parties: Alice and Bob, among whom at least one is assumed to be honest. If no party is caught cheating, the winner gets 1 coin, the loser gets 0 coins. If honest Alice catches dishonest Bob, Bob loses $`v`$ coins but Alice wins 0 coins. Similarly, if honest Bob catches dishonest Alice, she loses $`v`$ coins but Bob wins 0 coins.

###### Theorem 2

If Alice (Bob) is honest, the expected win by dishonest Bob (Alice) is at most $`\frac{1}{2}+\frac{1}{\sqrt{v}}`$, for $`v4`$.

###### Proof 2.3.

The protocol is as follows. Let $`\delta =\frac{2}{\sqrt{v}}`$. For $`a\{0,1\}`$, define $`|\psi _a=\sqrt{\delta }|a|a+\sqrt{1\delta }|2|2^3^3`$.

1. Alice picks $`a\{0,1\}`$ uniformly at random, generates the state $`|\psi _a`$ and sends the second register to Bob.
2. Bob stores this state in a quantum memory, picks $`b\{0,1\}`$ uniformly at random and sends $`b`$ to Alice.
3. Alice then sends $`a`$ and the first register to Bob and Bob verifies if the joint state of the two registers is $`|\psi _a`$ by measuring it in a basis consisting of $`|\psi _a`$ and everything orthogonal to it. If the test is passed, the result of coin flip is $`ab`$, otherwise Bob catches Alice cheating.

Theorem 2 follows immediately from the following two lemmas.

###### Lemma 2.4.

Bob cannot win with probability more than $`\frac{1}{2}+\frac{1}{\sqrt{v}}`$, thus his expected win is at most $`\frac{1}{2}+\frac{1}{\sqrt{v}}`$.

###### Proof 2.5.

Let $`\rho _a`$ be the density matrix of the second register of $`|\psi _a`$. Then, for the trace distance between $`\rho _0`$ and $`\rho _1`$ we have $`\rho _0\rho _1_t=2\delta `$.

The trace distance is a measure for the distinguishability of quantum states analogous to the total-variation distance of probability distributions; see e.g., . In particular, the probability of Bob winning is at most $`\frac{1}{2}+\frac{\rho _0\rho _1_t}{4}=\frac{1}{2}+\frac{\delta }{2}=\frac{1}{2}+\frac{1}{\sqrt{v}}`$.

###### Lemma 2.6.

Dishonest Alice’s expected win is at most $`\frac{1}{2}+\frac{1}{\sqrt{v}}`$.

###### Proof 2.7.

Alice is trying to achieve $`ab=0`$, which is equivalent to $`a=b`$. We describe the optimal strategy of Alice as a semidefinite program.

The variables are semidefinite matrices over subspaces of $`𝒳𝒜`$, where $`𝒳`$ is Alice’s private storage, $`𝒜^3`$ holds the first qutrit of the state to be sent in the protocol and $`^3`$ holds the second qutrit. For $`a,b\{0,1\}`$, let $`\rho _{ba}𝒜`$ denote the state that Bob has in the last round, when he has sent $`b`$ and Alice has sent $`a`$ (and some qutrit). For $`b\{0,1\}`$, let $`\rho _b𝒳𝒜`$ denote the state before Alice decides on $`a`$. Finally, let $`\rho _{\text{initial}}𝒳𝒜`$ denote the state that Alice prepares initially and of which she sends the $``$ part to Bob.

Then we have the following constraints. The initial state is an arbitrary density matrix:

$$\mathrm{tr}(\rho _{\text{initial}})=1$$
(1)
When Alice learns $`b`$, she cannot touch $``$ anymore, but she can apply an arbitrary unitary $`U_b`$ on $`𝒳𝒜`$ to store her choice $`a`$ in $`𝒳`$ and to prepare the $`𝒜`$ register in the desired state:

$$\mathrm{tr}_{𝒳𝒜}(\rho _{\text{initial}})=\mathrm{tr}_{𝒳𝒜}(\rho _b)\text{for all }b\{0,1\}$$
(2)
She will then measure $`𝒳`$ register in the computational basis to obtain $`a`$. Therefore we have

$$\mathrm{tr}_𝒳(\rho _b)=\rho _{b0}+\rho _{b1}\text{for all }b\{0,1\}.$$
(3)
Note that this implies $`\mathrm{tr}(\rho _{b0})+\mathrm{tr}(\rho _{b1})=1`$, so that in general the $`\rho _{ba}`$ are not density matrices.

Now Bob checks $`\rho _{ba}`$. This gives rise to the following objective function for Alice’s optimal cheating strategy:

$$\begin{array}{c}\mathrm{max}\underset{\beta \{0,1\}}{}\underset{\alpha \{0,1\}}{}\mathrm{Pr}[b=\beta ]\mathrm{Pr}[a=\alpha |b=\beta ]\hfill \\ \hfill \left(\delta _{\alpha \beta }\mathrm{Pr}[\rho _{\beta \alpha }\text{ passes}]v\mathrm{Pr}[\rho _{\beta \alpha }\text{ fails}]\right)\end{array}$$
(4)
Here the Kronecker-Delta $`\delta _{\alpha \beta }=1`$ if and only if $`\alpha =\beta `$ measures whether Alice managed to get $`a`$ and $`b`$ to match. Maximizing (4) is equivalent to maximizing

$$\begin{array}{c}\mathrm{max}\underset{\beta \{0,1\}}{}\underset{\alpha \{0,1\}}{}\mathrm{Pr}[b=\beta ]\mathrm{Pr}[a=\alpha |b=\beta ]\hfill \\ \hfill \mathrm{Pr}[\rho _{\beta \alpha }\text{ passes}]\left(\delta _{\alpha \beta }+v\right).\end{array}$$
(5)
Bob plays honestly, therefore $`\mathrm{Pr}[b=0]=\mathrm{Pr}[b=1]=\frac{1}{2}`$. Moreover, $`\mathrm{Pr}[a=\alpha |b=\beta ]=\mathrm{tr}(\rho _{\beta ,\alpha })`$ and

$$\mathrm{Pr}[\rho _{\beta \alpha }\text{ passes}]=\mathrm{tr}\left(|\psi _\alpha \psi _\alpha |\frac{\rho _{\beta ,\alpha }}{\mathrm{tr}(\rho _{\beta ,\alpha })}\right).$$

Hence, $`\mathrm{Pr}[a=\alpha |b=\beta ]\mathrm{Pr}[\rho _{\beta \alpha }\text{ passes}]=\psi _\alpha |\rho _{\beta \alpha }|\psi _\alpha `$. Substituting this into (5) and discarding the constant factor $`\frac{1}{2}`$ gives the final objective function

$$\mathrm{max}\underset{\beta \{0,1\}}{}\underset{\alpha \{0,1\}}{}\psi _\alpha |\rho _{\beta \alpha }|\psi _\alpha \left(\delta _{\alpha \beta }+v\right).$$
(6)
We now proceed to constructing the dual of the SDP formed by the objective function (6) together with the constraints (1), (2), and (3). The Lagrange ansatz is

$$\begin{array}{c}\underset{𝒫}{\mathrm{max}}\underset{𝒟}{inf}\underset{a,b\{0,1\}}{}\mathrm{tr}\left((\delta _{ab}+v)|\psi _a\psi _a|\rho _{ba}\right)\hfill \\ \hfill +\underset{b\{0,1\}}{}\mathrm{tr}\left(L_b\left(\mathrm{tr}_𝒳(\rho _b)\rho _{b0}\rho _{b1}\right)\right)\\ \hfill \underset{b\{0,1\}}{}\mathrm{tr}\left(M_b\mathrm{tr}_{𝒳𝒜}(\rho _b\rho _{\text{initial}})\right)\\ \hfill \mathrm{tr}(\lambda (\rho _{\text{initial}}\mathrm{𝟙}))\end{array}$$
(7)
where $`𝒫`$ are the primal variables as before, i.e.,

$$\begin{array}{c}𝒫=\{(\rho _{\text{initial}},\rho _0,\rho _1,\rho _{00},\rho _{01},\rho _{10},\rho _{11}):\hfill \\ \hfill \rho _{\text{initial}},\rho _0,\rho _1S(𝒳𝒜),\\ \hfill \rho _{00},\rho _{01},\rho _{10},\rho _{11}S(𝒜)\}\end{array}$$

and the dual variables (Lagrange multipliers) are

$$\begin{array}{c}𝒟=\{(L_0,L_1,M_0,M_1,\lambda ):\hfill \\ \hfill L_0,L_1H(𝒜),M_0,M_1H(),\lambda \}.\end{array}$$

Here $`H(𝒱)`$ and $`S(𝒱)`$ denote the Hermitian and semidefinite matrices, respectively, operating on the linear space $`𝒱`$. Collecting the primal variables in (7), we get for $`\rho _{\text{initial}}`$

$$\mathrm{tr}\left(\left(M_0+M_1\lambda \mathrm{𝟙}_{}\right)\rho _{\text{initial}}\right).$$

For $`\rho _b`$, $`b\{0,1\}`$, we obtain

$$\mathrm{tr}\left(\left(L_b(\mathrm{𝟙}_𝒜M_b)\right)\mathrm{tr}_𝒳(\rho _b)\right).$$

For $`\rho _{ba}`$, $`a,b\{0,1\}`$, we obtain

$$\mathrm{tr}\left(\left(L_b+(\delta _{ab}+v)|\psi _a\psi _a|\right)\rho _{ba}\right).$$

The terms in (7) not involving primal variables are just $`\lambda `$. Hence, the following dual SDP will give an upper bound on the optimal value of our primal SDP:

minimize $`\lambda \text{ subject to}`$ (8)
$`M_0+M_1`$ $`\lambda \mathrm{𝟙}_{}`$ (9)
$`L_b`$ $`\mathrm{𝟙}_𝒜M_b\text{ for all }b\{0,1\}`$ (10)
$`(v+\delta _{ab})|\psi _a\psi _a|`$ $`L_b\text{ for all }a,b\{0,1\}`$ (11)
$`(L_0,L_1,M_0,M_1,\lambda )`$ $`𝒟`$ (12)
We now construct a feasible solution for the dual SDP. We restrict our attention to $`M_0`$ and $`M_1`$ of the form

$$M_0=\left(\begin{array}{c}m_0\\ & m_1\\ & & m_2\end{array}\right)\text{ and }M_1=\left(\begin{array}{c}m_1\\ & m_0\\ & & m_2\end{array}\right)$$

for some $`m_0`$, $`m_1`$, $`m_2`$ with

$$m_00,m_10,m_2=\frac{1}{2}(m_0+m_1).$$
(13)
Moreover, we also impose the restriction $`L_b=\mathrm{𝟙}_𝒜M_b`$ for $`b\{0,1\}`$. Since then $`\lambda m_0+m_1`$, our goal reduces to minimizing $`m_0`$ and $`m_1`$ subject to

$`L_0(v+1)|\psi _0\psi _0|`$ $`0`$ (14)
$`L_0v|\psi _1\psi _1|`$ $`0`$ (15)
$`L_1v|\psi _0\psi _0|`$ $`0`$ (16)
$`L_1(v+1)|\psi _1\psi _1|`$ $`0.`$ (17)
Constraints (14) and (17) are satisfied if

$`m_0`$ $`(v+1)\delta `$ (18)
$`m_2`$ $`(v+1)(1\delta )`$ (19)
$`m_0m_2`$ $`(v+1)(1\delta )m_0+(v+1)\delta m_2.`$ (20)
Similarly, Constraints (15) and (16) require that

$`m_1`$ $`v\delta `$ (21)
$`m_2`$ $`v(1\delta )`$ (22)
$`m_1m_2`$ $`v(1\delta )m_1+v\delta m_2.`$ (23)
A solution to the system (13),(18)-(23) is

$$\begin{array}{ccc}m_0\hfill & =\frac{1}{2}(1+v)(\hfill & 2\delta (1+2v)\hfill \\ & & +\sqrt{44\delta +(\delta +2\delta v)^2})\hfill \\ m_1\hfill & \multicolumn{2}{c}{=\frac{1}{2}v\left(2+\delta +2\delta v\sqrt{44\delta +(\delta +2\delta v)^2}\right).}\end{array}$$

From this and the definition of $`\delta `$, we get that there is feasible solution of the dual SDP with

$`\lambda `$ $`=m_0+m_1`$
$`=2v+{\displaystyle \frac{1+\sqrt{v}2v+\sqrt{12\sqrt{v}+5v+4v^2}}{\sqrt{v}}}`$
$`2v+1+{\displaystyle \frac{1}{4\sqrt{v}}}.`$
From the earlier transformations of the primal objective function, it follows that the optimal expected payoff of Alice is bounded from above by $`\frac{1}{2}\lambda v\frac{1}{2}+\frac{1}{8\sqrt{v}}`$.

## 3 The multiparty model

### 3.1 Adversaries

In this work, we assume computationally unbounded adversaries. However, they have to obey quantum mechanics and cannot read the private memory of the honest players (but they can communicate secretly with each other). Moreover, we assume that they can only access the message space in between rounds or when according to the protocol it is their turn to send a message.

### 3.2 The broadcast channel

A classical broadcast channel allows one party to send a classical bit to all the other players. In the quantum setting this would mean that a qubit would be sent to all the other players. However, when there are more than two players in total we would have to clone or copy the qubit in order to send it to the other players. Even if the sender knows a classical preparation of the state he wants to send, we cannot allow him to prepare copies because he may be a cheater and send different states to different parties. It is well known that it is impossible to clone a qubit , because cloning is not a unitary operation. This means that we will have to take a slightly different approach. Quantum broadcast channels have been studied in an information-theoretic context before  but not in the presence of faulty or malicious parties.

Our quantum broadcast channel works as follows. Suppose there are $`k`$ players in total and that one player wants to broadcast a qubit that is in the state $`\alpha |0+\beta |1`$. What will happen is that the channel will create the $`k`$-qubit state $`\alpha |0^k+\beta |1^k`$ and send one of the $`k`$ qubits to each of the other players. The state $`\alpha |0^k+\beta |1^k`$ can be easily created from $`\alpha |0+\beta |1`$ by taking $`k1`$ fresh qubits in the state $`|0^{k1}`$. This joint state can be written as $`\alpha |0^k+\beta |10^{k1}`$. Next we flip the last $`k1`$ bits conditional on the first bit being a $`1`$, thus obtaining the desired state $`\alpha |0^k+\beta |1^k`$. This last operation can be implemented with a series of controlled-not operations. Note that this state is not producing $`k`$ copies of the original state, which would be the $`k`$-fold product state $`(\alpha |0+\beta |1)\mathrm{}(\alpha |0+\beta |1)`$.

###### Theorem 3.8.

In the following sense, a quantum broadcast channel between $`k`$ parties is comparable to models where the parties have a classical broadcast channel and/or pairwise quantum channels:

* If all parties are honest:

1. One use of the quantum broadcast channel can be simulated with $`2(k1)`$ uses of pairwise quantum channels.
    2. One use of a classical broadcast channel can be simulated with one use of the quantum broadcast channel.
    3. One use of a pairwise quantum channel can be simulated by $`k+1`$ uses of the quantum broadcast channel.
* If all but one of the parties are dishonest, using one of the simulations above in place of the original communication primitive does not confer extra cheating power.

###### Proof 3.9.

We first give the simulations and argue that they work in case all players are honest.

1. The sender takes $`k1`$ fresh qubits in state $`|0^k`$. He applies $`k1`$ times CNOT where the subsystem to be broadcast is the control of the CNOT and the fresh qubits are the destination. He then sends each of the $`k1`$ qubits via the pairwise quantum channels to the $`k1`$ other parties. Each recipient $`j`$ flips a (private) classical random bit $`r_j`$ and if $`r_j=1`$ performs a $`\sigma _z`$ phase flip on the received qubit. Here $`\sigma _z=\left(\begin{array}{cc}1& 0\\ 0& 1\end{array}\right)`$ is the Pauli matrix that multiplies the relative phase between the $`|0`$ and the $`|1`$ state by $`1`$. He then sends $`r_j`$ back to the sender. The sender computes the parity of the $`r_j`$ and if it is odd, he performs a $`\sigma _z`$ phase flip on his part of the broadcast state, thus restoring the correct relative phase. (This randomization is a countermeasure; its utility is explained below.)
2. When the sender wants to broadcast bit $`b\{0,1\}`$, he uses the quantum broadcast channel on qubit $`|b`$. The recipients immediately measure their qubit in the computational basis to obtain the classical bit.
3. The quantum broadcast channel can be used to create an EPR pair $`\frac{1}{\sqrt{2}}(|00+|11)`$ between two players $`P_i`$ and $`P_j`$ with the assistance of the other $`(k2)`$ players. $`i`$ and $`j`$ are determined by the protocol.

First one player broadcasts the state $`\frac{1}{\sqrt{2}}(|0+|1)`$, resulting in the $`k`$ qubit state $`|\phi =\frac{1}{\sqrt{2}}(|0^k+|1^k)`$. Now one after the other, the $`k2`$ remaining players perform a Hadamard transformation on their qubit, measure it in the computational basis, and broadcast the classical result. Next, if $`P_i`$ receives a $`1`$ he applies a phase flip $`\sigma _z`$ to his part of $`|\phi `$ ($`P_j`$ does nothing). After this operation, $`|\phi `$ will be an EPR state between $`P_i`$ and $`P_j`$ unentangled with the other $`k2`$ parties. Using a shared EPR pair, a protocol called teleportation  can be used to simulate a private quantum channel between $`P_i`$ and $`P_j`$. Teleportation requires the transmission of two bits of classical information.

For the case of all but one party being dishonest:

1. If the sender is honest, the recipients obtain exactly the same subsystems as for the quantum broadcast channel.

If one of the recipients is honest, he may receive an arbitrary quantum subsystem up to the randomized relative phase. However, exactly the same can be achieved with a quantum broadcast channel with $`k1`$ cheating parties, who each perform a Hadamard transformation on their subsystem followed by a measurement in the computational basis.
2. If the sender is honest, all recipients obtain the same computational-basis state.

If one of the recipients is honest, he obtains a classical bit that is possibly randomized in case the dishonest sender does not broadcast a basis state. Since the sender can flip a coin himself, this does not give more cheating power.
3. If the sender is honest, we can assume without loss of generality that all cheating action is done after the EPR pair has been established, because the (merged) cheaters can easily recreate the original broadcast state and also compensate any phase flipping of the honest sender. However, after the EPR pair has been established, the sender unilaterally performs his part of the teleportation circuit and measurements and sends the two bits of classical information. So the most general cheating action is to apply a quantum operation after the reception of the two classical bits. Furthermore, we can even assume that the cheating action is done *after* the correction circuit of teleportation (this is similar to the teleportation of quantum gates ) and, hence, amounts to cheating on a pairwise quantum channel.

If one of the recipients is honest, the best the cheaters can aim for is to give an arbitrary quantum state to the honest recipient. This they can also achieve over a pairwise quantum channel.

## 4 Multiparty quantum protocols

We will first consider the case of only one good player (i.e., $`g=1`$) among $`k`$ players and later extend our results to general $`g`$.

#### One honest player.

We need to construct a protocol with bias $`\frac{1}{2}\mathrm{\Omega }(\frac{1}{k})`$. Before proceeding to our actual protocol, let us consider a simple protocol which trivially extends the previous work in the two-party setting, but does not give us the desired result. The protocols is as follows: player $`1`$ flips a random coin with player $`2`$, player $`3`$ flips a random coin with player $`4`$ and so forth. In each pair, the player with the higher id wins if the coin is $`1`$ and the one with the lower id if the coin is $`0`$. The winners repeat the procedure. With each round of the tournament, half of the remaining players are eliminated (if there is an odd number of players at any moment, the one with the highest id advances to the next round). When there are only two players left, the coin they flip becomes the output of the protocol. (Above we assume we have private point-to-point quantum channels and a classical broadcast channel, which is justified by Theorem 3.8.)

The elimination step can be implemented using the weak two-party coin-flipping protocol by Spekkens and Rudolph  and the last round by the the strong two-party coin-flipping protocol by Ambainis . If there is only one good player, the probability that he makes it to the last round is

$$\left(1\frac{1}{\sqrt{2}}\right)^{1+\mathrm{log}k};$$

in this case, the probability that the bad players can determine the output coin is $`\frac{3}{4}`$. In case the good player gets eliminated, the bad players can completely determine the coin. Hence, the overall probability that the bad players can determine the coin is

$$1\frac{1}{4}\left(1\frac{1}{\sqrt{2}}\right)^{1+\mathrm{log}k}1\frac{1}{4k^{1.78}},$$

which corresponds to bias

$$\frac{1}{2}\mathrm{\Omega }\left(\frac{1}{k^{1.78}}\right).$$

Using the protocol by Mochon  improves the exponent slightly to $`1.7`$ but not all the way to $`1`$. To improve the bound above to the desired value $`\frac{1}{2}\mathrm{\Omega }(\frac{1}{k})`$, we will use our coin-flipping protocol with penalty from Section 2. The idea is that in normal quantum coin-flipping protocols for two parties, there are three outcomes for a given player: “win,” “lose,” and “abort.” Looking at the elimination tournament above, if an honest player loses a given coin flipping round, he does not complain and the bad player wins the game. However, if the honest player detects cheating, he can and will abort the entire process, which corresponds to the failure of the dishonest players to fix the coin. Of course, if there are few elimination rounds left, bad players might be willing to risk the abort if they gain significant benefits in winning the round. However, if the round number is low, abort becomes prohibitively expensive: a dishonest player might not be willing to risk it given there are plenty more opportunities for the honest player to “lose normally.” Thus, instead of regular two-party coin-flipping protocols, which do not differentiate between losing and aborting, we can employ our protocol for coin flipping with penalty, where the penalties are very high at the original rounds, and eventually get lower towards the end of the protocol. Specific penalties are chosen in a way which optimizes the final bias we get, and allows us to achieve the desired bias $`\frac{1}{2}\mathrm{\Omega }(\frac{1}{k})`$.

###### Theorem 4.10.

There is a strong quantum coin-flipping protocol for $`k`$ parties with bias at most $`\frac{1}{2}\frac{c}{k}`$ for some constant $`c`$, even with $`(k1)`$ bad parties.

###### Proof 4.11.

We assume that $`k=2^n`$ for some $`n>0`$, as it changes $`c`$ by at most a constant factor. Let $`Q_v`$ be the maximum expected win in a two-party protocol with penalty $`v`$. Consider the following protocol with $`n`$ rounds numbered $`1`$ to $`n`$.

At the beginning of round $`i`$, we have $`2^{n+1i}`$ parties remaining. We divide them into pairs. Each pair performs the two-party coin-flipping protocol with penalty $`(2^{ni}1)`$. The party with the lower id plays Alice and wins if the outcome is $`0`$; the party with the higher id plays Bob and wins if the outcome is $`1`$. The winners proceed to round $`(i+1)`$.

At the beginning of round $`(n2)`$, there are just $`8`$ parties remaining. They perform three rounds of regular coin flipping with no penalty using the protocol of , in which no cheater can determine the coin with probability more than $`\frac{3}{4}`$. This results in maximum probability of $`\frac{63}{64}`$ for fixing the outcome when there is at least one good player among the $`8`$. The result of the last round is the result of our $`2^n`$-party protocol.

Assume that the honest player has won the first $`(nj)`$ coin flips and advanced to round $`(j+1)`$. Assume that the all other players in round $`(j+1)`$ are dishonest. Let $`P_j`$ be the maximum probability with which $`(2^j1)`$ dishonest players can fix the outcome in this case.

###### Lemma 4.12.

$$1P_j(1P_{j1})(1Q_{2^{j1}1})$$
(24)
###### Proof 4.13.

Let $`p_w`$, $`p_l`$, $`p_c`$ be the probabilities of the honest player winning, losing and catching the other party cheating in the round $`(j+1)`$ of the protocol. Notice that $`p_w+p_l+p_c=1`$. Then, the probability $`P_j`$ of $`2^j1`$ dishonest parties fixing the coin is at most $`p_l+p_wP_{j1}`$. (If the honest player loses, they win immediately. If he wins, they can still bias the coin in $`j1`$ remaining rounds to probability at most $`P_{j1}`$. If he catches his opponent cheating, he exits the protocol and the dishonest players have no more chances to cheat him.) Using $`p_w=1p_lp_c`$, we have

$$\begin{array}{c}P_jp_l+p_wP_{j1}=P_{j1}+(1P_{j1})p_lP_{j1}p_c\hfill \\ \hfill =P_{j1}+(1P_{j1})\left(p_l\frac{P_{j1}}{1P_{j1}}p_c\right)\end{array}$$
(25)
Next, notice that $`P_{j1}1\frac{1}{2^{j1}}`$. This is because $`2^{j1}1`$ bad players could just play honestly when they face the good player and fix the coin flip if two bad players meet in the last round. Therefore, $`\frac{P_{j1}}{1P_{j1}}2^{j1}1`$ and (25) becomes

$$P_jP_{j1}+(1P_{j1})(p_l(2^{j1}1)p_c)$$

The term $`p_l(2^{j1}1)p_c`$ is at most $`Q_{2^{j1}1}`$ because we can interpret it as the expected payoff of the cheater that plays with the honest player. Hence,

$$P_jP_{j1}+(1P_{j1})Q_{2^{j1}1},$$

which is equivalent to the desired (24).

By applying the lemma inductively, we obtain

$`1P_n`$ $`(1P_8){\displaystyle \underset{j=4}{\overset{n}{}}}(1Q_{2^{j1}1})`$
$`{\displaystyle \frac{1}{64}}{\displaystyle \underset{j=4}{\overset{n}{}}}(1Q_{2^{j1}1}).`$
Using the bound in Theorem 2 we get

$`1P_n`$ $`{\displaystyle \frac{1}{64}}{\displaystyle \underset{j=3}{\overset{n1}{}}}(1Q_{2^j1})`$
$`{\displaystyle \frac{1}{64}}{\displaystyle \underset{j=3}{\overset{n1}{}}}\left({\displaystyle \frac{1}{2}}{\displaystyle \frac{1}{\sqrt{2^j1}}}\right)`$
$`{\displaystyle \frac{1}{82^n}}{\displaystyle \underset{j=3}{\overset{\mathrm{}}{}}}\left(1{\displaystyle \frac{2}{\sqrt{2^j1}}}\right).`$
The last product is a positive constant. Therefore, for some constant $`c>0`$ we have $`1P_n\frac{c}{2^n}=\frac{c}{k}`$, which means that the bias is at most $`\frac{1}{2}\mathrm{\Omega }(\frac{1}{k})`$.

#### Extending to many honest players.

We can extend Theorem 4.10 to any number $`g1`$ of good players by using the classical lightest-bin protocol of Feige . This protocol allows us to reduce the total number of players until a single good player is left without significantly changing the fraction of good players, after which we can run the quantum protocol of Theorem 4.10 to get the desired result. Specifically, Lemma 8 from  implies that starting from $`g=\delta k`$ good players out of $`k`$ players, the players can (classically) select a sub-committee of $`\mathrm{O}(\frac{1}{\delta })=\mathrm{O}(\frac{k}{g})`$ players containing at least one good player with probability at least $`\frac{1}{2}`$. Now this sub-committee can use the quantum protocol of Theorem 4.10 to flip a coin with bias $`\frac{1}{2}\mathrm{\Omega }(\frac{g}{k})`$, provided it indeed contains at least one honest player. But since the latter happens with probability at least $`\frac{1}{2}`$, the final bias is at most $`\frac{1}{2}\frac{1}{2}\mathrm{\Omega }(\frac{g}{k})=\frac{1}{2}\mathrm{\Omega }(\frac{g}{k})`$, as desired.

## 5 Lower bound

### 5.1 The two-party bound

For completeness and to facilitate the presentation of our generalization, we reproduce here Kitaev’s unpublished proof  that any two-party strong quantum coin-flipping protocol must have bias at least $`\frac{1}{\sqrt{2}}`$. The model here is that the two parties communicate over a quantum channel.

###### Definition 5.14.

Let $`:=𝒜`$ denote the Hilbert space of the coin-flipping protocol composed of Alice’s private space, the message space, and Bob’s private space. A $`2N`$-round two-party coin-flipping protocol is a tuple

$`(`$ $`U_{A,1},\mathrm{},U_{A,N},U_{B,1},\mathrm{},U_{B,N},`$
$`\mathrm{\Pi }_{A,0},\mathrm{\Pi }_{A,1},\mathrm{\Pi }_{B,0},\mathrm{\Pi }_{B,1})`$
where

* $`U_{A,j}`$ is a unitary operator on $`𝒜`$ for $`j=1,\mathrm{},N`$,
* $`U_{B,j}`$ is a unitary operator on $``$ for $`j=1,\mathrm{},N`$,
* $`\mathrm{\Pi }_{A,0}`$ and $`\mathrm{\Pi }_{A,1}`$ are projections from $`𝒜`$ onto orthogonal subspaces of $`𝒜`$ (representing Alice’s final measurements for outcome $`0`$ and $`1`$, respectively),
* $`\mathrm{\Pi }_{B,0}`$ and $`\mathrm{\Pi }_{B,1}`$ are projections from $``$ onto orthogonal subspaces of $``$ (representing Bob’s final measurements for outcome $`0`$ and $`1`$, respectively),

so that for

$`|\psi _N:=`$ $`(1_𝒜U_{B,N})(U_{A,N}1_{})(1_𝒜U_{B,N1})`$
$`(U_{A,N1}1_{})\mathrm{}(1_𝒜U_{B,1})(U_{A,1}1_{})|0`$
holds

$`(\mathrm{\Pi }_{A,0}1_{}1_{})|\psi _N`$ $`=(1_𝒜1_{}\mathrm{\Pi }_{B,0})|\psi _N`$ (26)
$`(\mathrm{\Pi }_{A,1}1_{}1_{})|\psi _N`$ $`=(1_𝒜1_{}\mathrm{\Pi }_{B,1})|\psi _N`$ (27)
$`(\mathrm{\Pi }_{A,0}1_{}1_{})|\psi _N`$ $`=(\mathrm{\Pi }_{A,1}1_{}1_{})|\psi _N`$ (28)
The first two conditions ensure that when Alice and Bob are honest, they both get the same value for the coin and the third condition guarantees that when Alice and Bob are honest, their coin is not biased. A player aborts if her or his final measurement does not produce outcome $`0`$ or $`1`$; of course, it is no restriction to delay this action to the end of the protocol.

###### Lemma 5.15.

Fix an arbitrary two-party quantum coin-flipping protocol. Let $`p_1`$ and $`p_1`$ denote the probability that Alice or Bob, respectively, can force the outcome of the protocol to be $`1`$ if the other party follows the protocol. Denote by $`p_1`$ the probability for outcome $`1`$ when there are no cheaters. Then $`p_1p_1p_1`$.

Hence, if $`p_1=\frac{1}{2}`$, then $`\mathrm{max}\{p_1,p_1\}\frac{1}{\sqrt{2}}`$. To prove Lemma 5.15, we construct the view of a run of the protocol from an honest Alice’s point of view, with Bob wanting to bias the protocol towards $`1`$. The problem of optimizing Bob’s strategy is a semidefinite program.

###### Lemma 5.16.

The optimal strategy of Bob trying to force outcome $`1`$ is the solution to the following SDP over the semidefinite matrices $`\rho _{A,0},\mathrm{},\rho _{A,N}`$ operating on $`𝒜`$:

maximize $`\mathrm{tr}\left((\mathrm{\Pi }_{A,1}1_{})\rho _{A,N}\right)\text{ subject to}`$ (29)
$`\mathrm{tr}_{}(\rho _{A,0})`$ $`=|00|_𝒜`$ (30)
$`\mathrm{tr}_{}(\rho _{A,j})`$ $`=\mathrm{tr}_{}(U_{A,j}\rho _{A,j1}U_{A,j}^{})(1jN)`$ (31)
###### Proof 5.17.

Alice starts with her private memory in state $`|0_𝒜`$ and we permit Bob to determine the $``$ part of the initial state. Therefore all Alice knows is that initially, the space accessible to her is in state $`\rho _{A,0}`$ with $`\mathrm{tr}_{}(\rho _{A,0})=|00|_𝒜`$. Alice sends the first message, transforming the state to $`\rho _{A,0}^{}:=U_{A,1}\rho _{A,0}U_{A,1}^{}`$. Now Bob can do any unitary operation on $``$ leading to $`\rho _{A,1}`$, so the only constraint is $`\mathrm{tr}_{}(\rho _{A,1})=\mathrm{tr}_{}(\rho _{A,0}^{})`$. In the next round, honest Alice applies $`U_{A,2}`$, then Bob can do some operation that preserves the partial trace, and so forth. The probability for Alice outputting $`1`$ is $`\mathrm{tr}((\mathrm{\Pi }_{A,1}1_{})\rho _{A,N})`$ because the final state for Alice is $`\rho _{A,N}`$ and she performs an orthogonal measurement on $`𝒜`$ with projections $`\mathrm{\Pi }_{A,0}`$, $`\mathrm{\Pi }_{A,1}`$, and $`1_𝒜\mathrm{\Pi }_{A,0}\mathrm{\Pi }_{A,1}`$ (which represents “abort”).

###### Lemma 5.18.

The dual SDP to the primal SDP in Lemma 5.16 is

minimize $`0|Z_{A,0}|0\text{ subject to}`$ (32)
$`Z_{A,j}1_{}`$ $`U_{A,j+1}^{}(Z_{A,j+1}1_{})U_{A,j+1}`$ (33)
$`(\text{for all }j:0jN1)`$
$`Z_{A,N}`$ $`=\mathrm{\Pi }_{A,1}`$ (34)
over the Hermitian matrices $`Z_{A,0},\mathrm{}Z_{A,N}`$ operating on $`𝒜`$.

###### Proof 5.19.

We form the dual of the SDP in Lemma 5.16 as follows: it is equivalent to maximizing over the $`\rho _{A,j}`$ the minimum of

$$\begin{array}{c}\mathrm{tr}((\mathrm{\Pi }_{A,1}1_{})\rho _{A,N})\mathrm{tr}(Z_{A,0}(\mathrm{tr}_{}(\rho _{A,0})|00|_{}))\hfill \\ \hfill \underset{j=1}{\overset{N}{}}\mathrm{tr}(Z_{A,j}\mathrm{tr}_{}(\rho _{A,j}U_{A,j}\rho _{A,j1}U_{A,j}^{}))\end{array}$$
(35)
subject to the operators $`Z_{A,j}`$ on $``$ being Hermitian (for $`0jN`$). In the sum above, the terms containing $`\rho _{A,j}`$ for $`0j<N`$ are

$$\begin{array}{c}\mathrm{tr}(Z_{A,j}\mathrm{tr}_{}(\rho _{A,j}))\hfill \\ \hfill +\mathrm{tr}(Z_{A,j+1}\mathrm{tr}_{}(U_{A,j+1}\rho _{A,j}U_{A,j+1}^{})),\end{array}$$

which equals

$$\begin{array}{c}\mathrm{tr}(((Z_{A,j}1_{})+\hfill \\ \hfill U_{A,j+1}^{}(Z_{A,j+1}1_{})U_{A,j+1})\rho _{A,j}).\end{array}$$

Since this term must be non-positive, we arrive at the inequality (33).

For $`j=N`$, we obtain the dual equality constraint (34) and the dual objective function becomes the only summand of (35) that does not involve any $`\rho _{A,j}`$.

###### Proof 5.20 (Proof of Lemma 5.15).

Let $`Z_{A,j}`$ and $`Z_{B,j}`$ ($`0jN`$) denote the optimal solutions for the dual SDPs for a cheating Bob and a cheating Alice, respectively. For each $`j`$, $`0jN`$, let

$$\begin{array}{c}|\psi _j:=(1_𝒜U_{B,j})(U_{A,j}1_{})\mathrm{}\hfill \\ \hfill (1_𝒜U_{B,1})(U_{A,1}1_{})|0\end{array}$$

denote the state of the protocol in round $`j`$ when both parties are honest. Let $`F_j:=\psi _j|(Z_{A,j}1_{}Z_{B,j})|\psi _j`$. We claim

$`p_1p_1`$ $`=F_0`$ (36)
$`F_j`$ $`F_{j+1}(0j<N)`$ (37)
$`F_N`$ $`=p_1.`$ (38)
Combining (36)–(38), we obtain the desired $`p_1p_1p_1`$. We now proceed to prove these claims.

Note that the primal SDP from Lemma 5.16 is strictly feasible: Bob playing honestly yields a feasible solution that is strictly positive. The strong-duality theorem of semidefinite programming states that in this case, the optimal value of the primal and the dual SDPs are the same, and therefore $`p_1=0|_𝒜Z_{A,0}|0_𝒜`$ and $`p_1=0|_{}Z_{B,0}|0_{}`$ and

$`p_1p_1`$ $`=0|_𝒜Z_{A,0}|0_𝒜0|_{}1_{}|0_{}0|_{}Z_{B,0}|0_{}`$
$`=0|(Z_{A,0}1_{}Z_{B,0})|0=F_0.`$
The inequalities (37) hold because of the constraints (33). Equality (38) holds because by constraint (34) we have

$$\begin{array}{c}\phi |(Z_{A,N}1_{}Z_{B,N})|\phi =\hfill \\ \hfill (\mathrm{\Pi }_{A,1}1_{}1_{})(1_𝒜1_{}\mathrm{\Pi }_{B,1})|\phi ^2\end{array}$$

for any $`|\phi `$; $`|\psi _N`$ is the final state of the protocol when both players are honest, so by equation (27),

$$\begin{array}{c}(\mathrm{\Pi }_{A,1}1_{}1_{})(1_𝒜1_{}\mathrm{\Pi }_{B,1})|\psi _N^2\hfill \\ \hfill =(\mathrm{\Pi }_{A,1}1_{}1_{})|\psi _N^2=p_1.\end{array}$$

### 5.2 More than two parties

We will now extend Kitaev’s lower bound to $`k`$ parties. As with the upper bounds, we first start with a single honest player ($`g=1`$), and then extend the result further to any $`g`$.

###### Theorem 5.21.

Any strong quantum coin-flipping protocol for $`k`$ parties has bias at least

$$\frac{1}{2}\frac{\mathrm{ln}2}{k}\mathrm{O}\left(\frac{1}{k^2}\right)$$

if it has to deal with up to $`(k1)`$ bad parties.

We consider the model of private pairwise quantum channels between the parties; by Theorem 3.8 the results immediately carry over to the quantum broadcast channel.

###### Definition 5.22.

Let $`:=𝒜_1\mathrm{}𝒜_k`$ denote the Hilbert space composed of the private spaces of $`k`$ parties and the message space. An $`N`$-round $`k`$-party coin-flipping protocol is a tuple

$$(i_1,\mathrm{},i_N,U_1,\mathrm{},U_N,\mathrm{\Pi }_{1,0},\mathrm{\Pi }_{1,1},\mathrm{},\mathrm{\Pi }_{k,0},\mathrm{\Pi }_{k,1})$$

where

* $`i_j`$ with $`1i_jk`$, $`1jN`$, indicates whose turn it is to access the message space in round $`j`$,
* $`U_j`$ is a unitary operator on $`𝒜_{i_j}`$ for $`j=1,\mathrm{},N`$,
* for $`1ik`$, $`\mathrm{\Pi }_{i,0}`$ and $`\mathrm{\Pi }_{i,1}`$ are projections from $`𝒜_i`$ to orthogonal subspaces of $`𝒜_i`$ (representing the measurement that party $`i`$ performs to determine outcome $`0`$ or $`1`$, respectively),

so that for $`|\psi _N:=\stackrel{~}{U}_{i_N}\mathrm{}\stackrel{~}{U}_{i_1}|0`$ and each pair $`1i<i^{}k`$ and any $`b\{0,1\}`$ holds

$`\stackrel{~}{\mathrm{\Pi }}_{i,b}|\psi _N`$ $`=\stackrel{~}{\mathrm{\Pi }}_{i^{},b}|\psi _N`$ (39)
$`\stackrel{~}{\mathrm{\Pi }}_{i,b}|\psi _N`$ $`=\stackrel{~}{\mathrm{\Pi }}_{i,1b}|\psi _N.`$ (40)
Here $`\stackrel{~}{U}_j`$ denotes the extension of $`U_j`$ to all of $``$ that acts as identity on the tensor factors $`𝒜_i^{}`$ for $`i^{}i_j`$; $`\stackrel{~}{\mathrm{\Pi }}_{i,b}:=(1_{𝒜_1}\mathrm{}1_{𝒜_{i1}}\mathrm{\Pi }_{i,b}1_{𝒜_{i+1}}\mathrm{}1_{𝒜_k})`$ is the extension of $`\mathrm{\Pi }_{i,b}`$ to $``$.

###### Lemma 5.23.

Fix an arbitrary quantum coin flipping protocol. For $`b\{0,1\}`$, let $`p_b`$ be the probability of outcome $`b`$ in case all players are honest. Let $`p_{i,b}`$ denote the probability that party $`i`$ can be convinced by the other parties that the outcome of the protocol is $`b\{0,1\}`$. Then

$$p_{1,b}\mathrm{}p_{k,b}p_b$$

###### Proof 5.24 (Proof of Lemma 5.23).

The optimal strategy for $`k1`$ bad players trying to force outcome $`1`$ is the solution to the SDP from Lemma 5.16 where all the cheating players are merged into a single cheating player.

Let $`(Z_{i,j})_{0jN}`$ denote the optimal solution for the dual SDP for good player $`i`$, $`1ik`$. For each $`j`$, $`0jN`$, let $`|\psi _j:=\stackrel{~}{U}_j\mathrm{}\stackrel{~}{U}_1|0`$ denote the state of the protocol in round $`j`$ when all parties are honest. Let $`F_j:=\psi _j|(Z_{1,j}\mathrm{}Z_{k,j}1_{})|\psi _j`$. By a similar argument as in the proof of Lemma 5.15, we have

$`p_{1,1}\mathrm{}p_{k,1}`$ $`=F_0`$ (41)
$`F_j`$ $`F_{j+1}(0j<N)`$ (42)
$`F_N`$ $`=p_1`$ (43)
Hence, $`p_{1,1}\mathrm{}p_{k,1}p_1`$. Repeating the argument with the cheaters aiming for outcome 0 completes the proof.

Theorem 5.21 is an immediate consequence.

###### Proof 5.25 (Proof of Theorem 5.21).

Using the notation of Lemma 5.23, we have $`p_0=\frac{1}{2}`$. Let $`q=\mathrm{max}_ip_{i,0}`$ denote the maximum probability of any player forcing output $`0`$. By Lemma 5.23, $`q^kp_{1,0}\mathrm{}p_{k,0}\frac{1}{2}`$, from which follows that

$$q\left(\frac{1}{2}\right)^{1/k}1\frac{\mathrm{ln}2}{k}\mathrm{O}\left(\frac{1}{k^2}\right).$$

By Theorem 3.8 this result applies both to private pairwise quantum channels and the quantum broadcast channel.

#### Extending to many honest players.

Extension to any number of honest players follows almost immediately from Theorem 5.21. Indeed, take any protocol $`\mathrm{\Pi }`$ for $`k`$ parties tolerating $`(kg)`$ cheaters. Arbitrarily partition our players into $`k^{}=\frac{k}{g}`$ groups and view each each as one “combined player.” We get an induced protocol $`\mathrm{\Pi }^{}`$ with $`k^{}`$ “super-players” which achieves at least the same bias $`\epsilon `$ as $`\mathrm{\Pi }`$, and can tolerate up to $`(k^{}1)`$ bad players. By Theorem 5.21, $`\epsilon \frac{1}{2}\mathrm{O}(\frac{1}{k^{}})=\frac{1}{2}\mathrm{O}(\frac{g}{k})`$.

## Acknowledgements

We thank L. Fortnow and J.-H. Hoepman for useful discussions.


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# Hund’s rule Magnetism in C60 ions?

## 1 Introduction

Magnetism without transition metals is a potentially exciting subject. As an example, carbon magnetism has generated some recent interest, in connection with some fullerene-derived carbon-only magnetic materials Makarova01 ; Wood02 . In these materials however the fullerene cage is disrupted into some sort of three-dimensional bonding network. In this paper we focus on carbon magnetism that may occur in isolated fullerene ions, and in ionic fullerene compounds where electrons are added or subtracted to C60 molecules that preserve their overall molecular integrity.

Unconventional properties, including magnetism, of negative C60 ions have in fact been previously discussed in the literature. Due to the high symmetry of the molecule, the threefold degenerate $`t_{1u}`$ molecular orbital of C60 will, when partly filled, be affected by Coulomb exchange Martin93 ; Han00 ; Lueders02 , which favors molecular Hund’s rule magnetism, quite similar to that leading to the atomic magnetic moments in ordinary $`d`$ and $`f`$ elements and compounds. In addition to displaying Hund-rule physics, a high-symmetry molecule will however also undergo Jahn-Teller (JT) distortions. The JT ground state favors electron spin pairing, generally leading to larger energy gains for low-spin states than for high-spin states. Molecular Hund-rule exchange and JT are therefore competing effects from the point of view of magnetism. Past studies indicated that in C$`{}_{}{}^{n}{}_{60}{}^{}`$ ions the JT interaction is in fact somewhat stronger than Coulomb exchange, leading to low-spin ground states Lueders02 ; Bergomi ; AMT ; MTA ; Brouet01 . 111Low-spin ground state is also observed in a number of diradicals Rajca93 ; Rajca00 , but the situation there is quite different from C60 ions. In ideal icosahedral C60 ions the degenerate orbitals require a regular first Hund rule with maximum spin. Density-functional theory (DFT) calculations do of course confirm that. A low-spin ground state may be eventually obtained if, upon lowering the icosahedral symmetry by means of a JT distortion, the corresponding energy gain happened to be large enough to reverse the undistorted high-spin situation. In the aromatic diradicals instead, two distant unpaired spins interact somewhat weakly through the molecular backbone, and a Heitler-London singlet ground state appears to be achieved, no distortions involved.  Nonetheless, the balance between JT and Hund’s rule is to some degree compound dependent, leading to a close match in certain chemical environments. Spin gaps of the order of 100 meV between the $`S=0`$ ground state and the $`S=1`$ excitation of the C$`{}_{}{}^{2}{}_{60}{}^{}`$ or equivalently of the C$`{}_{}{}^{4}{}_{60}{}^{}`$ion were reported in NMR studies of compounds like K4C60 and Na2C60, but a narrower 10 meV gap has been suggested for the $`n=2`$ fluctuating charge state in CsC60 Brouet99 . The magnetism of TDAE-C60 Allemand ; Narymbetov  can also be attributed to a spin triplet in charge fluctuating C$`{}_{}{}^{2}{}_{60}{}^{}`$ states Arovas95 .

The main question which we wish to address here is what ground-state spin is to be expected for positive C$`{}_{}{}^{n+}{}_{60}{}^{}`$ ions. The calculations will be done in parallel for C$`{}_{}{}^{n+}{}_{60}{}^{}`$ and C$`{}_{}{}^{n}{}_{60}{}^{}`$ so as to emphasize the analogies and the differences that will emerge. Zero-point effects are also approximately included, and their effect is shown to be non negligible.

Data on C$`{}_{}{}^{n+}{}_{60}{}^{}`$ molecular ions do not appear to be readily available. In particular the published photoemission spectra of C60 Bruhwiler97 ; Canton02  imply C$`{}_{}{}^{+}{}_{60}{}^{}`$ final states. This $`n=1`$ state is affected by JT but clearly not by Hund’s rule. Some charge-transfer compounds contain nominal C$`{}_{}{}^{2+}{}_{60}{}^{}`$ ions. While it is presently unclear whether higher charge states are accessible, acceptor compounds with nominal (AsF6)2C60 and (SbF6)2C60 stoichiometries have been described, containing again C$`{}_{}{}^{2+}{}_{60}{}^{}`$ molecular ions. Recent data, including anomalously short spin-lattice relaxation times Panich02 , strongly suggest the possibility of magnetism of the C$`{}_{}{}^{2+}{}_{60}{}^{}`$ ions.

Here we address the question of magnetism of C$`{}_{}{}^{n+}{}_{60}{}^{}`$ ions by addressing quantitatively the competition between JT and Coulomb exchange in these ions. Both JT and intra-molecular exchange terms are calculated to be individually stronger in C$`{}_{}{}^{n+}{}_{60}{}^{}`$ than in C$`{}_{}{}^{n}{}_{60}{}^{}`$ Lueders02 ; Manini01 . Preliminary calculations and estimates based on the adiabatic approximation Lueders02  did foreshadow the predominance of Hund’s rule exchange in C$`{}_{}{}^{n+}{}_{60}{}^{}`$, as opposed to the predominance of JT in C$`{}_{}{}^{n}{}_{60}{}^{}`$. In the adiabatic approximation however, the JT effect is postulated to be static, neglecting zero-point motion of the carbon nuclei (responsible for turning JT from static to dynamic, even at $`T=0`$). This simplification might be unsafe, as it is known to underestimate the JT energy gain MTA . In turn, it might seriously impair our understanding of the competition between high spin and low spin, through the neglect of very large corrections associated to the different zero-point vibrational quantum kinetic energy associated with states of different spin. Here we estimate these zero-point effects and include them in the coupled JT-Hund’s rule problem, thus correcting the adiabatic result. An accurate evaluation of this correction is in fact quite generally a formidable task. We show here that one lucky feature of C$`{}_{}{}^{n+}{}_{60}{}^{}`$ ions is that their strong e-v coupling makes the basic zero-point correction a good approximation to the true result. Our bottom-line conclusion will be that whereas quantum corrections to the ground state energy are confirmed to be large, they do not reverse the ground-state spin state for any of the C$`{}_{}{}^{n+}{}_{60}{}^{}`$ ions. In particular the prediction that C$`{}_{}{}^{2+}{}_{60}{}^{}`$ should be magnetic is maintained. It is in fact reinforced, with the $`S=1`$ ground state about 30 meV lower than the lowest $`S=0`$ state.

This prediction does not of course imply that compounds containing C$`{}_{}{}^{n+}{}_{60}{}^{}`$ will by necessity be magnetic. Electron kinetic energy associated with hopping between molecules do in principle favor band electron spin pairing, and a standard nonmagnetic metallic state. However, any insulating states that could arise due to very narrow bands, such as a Mott or more probably a Mott-JT insulatorFabrizio97 , is very likely to be magnetic. In this regard it seems interesting that both (AsF6)2C60 and (SbF6)2C60 acceptor intercalated materials, nominally containing doubly positive fullerene ions were indeed found to be electrical insulators, with activation gaps of 0.22 and 0.64 eV respectively Datars96 .

The starting point of this paper will be the static, adiabatic JT-distorted state of all C$`{}_{}{}^{n\pm }{}_{60}{}^{}`$ ions treated in the simplest model Hamiltonians that includes both e-v and e-e interactions. Each of these static JT wells, or “valleys”, is characterized by a reduction of symmetry from icosahedral to some subgroup. New vibrational frequencies arise at each such valley. We determine these frequencies by evaluation of the Hessian energy matrix at the energy minimum ManyModes . We use the lowering of the zero-point vibrational energies from the undistorted to the JT distorted state to estimate the leading quantum correction to the adiabatic approximation. The next-order quantum correction would arise from weak tunneling between equivalent valleys. This is the conceptually important step that leads from static to dynamic JT, with full restoration of the undistorted icosahedral symmetry. The associated energy correction expected is however relatively minor in C$`{}_{}{}^{n+}{}_{60}{}^{}`$, in view of the large e-v couplings. In the limit of infinite coupling the tunneling corrections vanish, and all quantum effects coincide exactly with the zero-point lowering. Therefore, a direct quantitative check that the tunneling corrections are reasonably small already in the weakest coupling case of C$`{}_{}{}^{1}{}_{60}{}^{}`$, and already negligible in C$`{}_{}{}^{1+}{}_{60}{}^{}`$ justifies us in neglecting them for all other charge states. The accuracy of this neglect is, it should be noted, particularly good for the positive ions C$`{}_{}{}^{n+}{}_{60}{}^{}`$, where the e-v coupling is larger than in C$`{}_{}{}^{n}{}_{60}{}^{}`$.

This paper is organized as follows. Sect. 2 introduces the model and the parameters used in this calculation, which is then described in Sect. 3, along with the properties of the JT valleys for all values $`n`$ and $`S`$. The zero-point non-adiabatic corrections are described in Sect. 4, and the overall results are finally discussed in Sect. 5.

## 2 The model Hamiltonian

We begin by reviewing here the model Hamiltonian previously introduced in Ref. Lueders02  to describe the electron-vibration coupling and Coulomb exchange of holes in the $`h_u`$ fivefold-degenerate highest occupied molecular orbital (HOMO), and of electrons in the threefold-degenerate $`t_{1u}`$ lowest unoccupied molecular orbital (LUMO) of C60:

$$\widehat{H}=\widehat{H}_0+\widehat{T}_{\mathrm{vib}}+\widehat{V}_{\mathrm{vib}}+\widehat{H}_{\mathrm{e}\mathrm{v}}+\widehat{H}_{\mathrm{e}\mathrm{e}}$$
(1)
where

$`\widehat{H}_0`$ $`=`$ $`ϵ{\displaystyle \underset{\sigma m}{}}\widehat{c}_{\sigma m}^{}\widehat{c}_{\sigma m},`$ (2)
$`\widehat{T}_{\mathrm{vib}}`$ $`=`$ $`{\displaystyle \underset{i\mathrm{\Lambda }\mu }{}}{\displaystyle \frac{\mathrm{}\omega _{i\mathrm{\Lambda }}}{2}}\widehat{P}_{i\mathrm{\Lambda }\mu }^2,`$ (3)
$`\widehat{V}_{\mathrm{vib}}`$ $`=`$ $`{\displaystyle \underset{i\mathrm{\Lambda }\mu }{}}{\displaystyle \frac{\mathrm{}\omega _{i\mathrm{\Lambda }}}{2}}\widehat{Q}_{i\mathrm{\Lambda }\mu }^2,`$ (4)
$`\widehat{H}_{\mathrm{e}\mathrm{v}}`$ $`=`$ $`{\displaystyle \underset{ri\mathrm{\Lambda }}{}}{\displaystyle \frac{k^\mathrm{\Lambda }g_{i\mathrm{\Lambda }}^r\mathrm{}\omega _{i\mathrm{\Lambda }}}{2}}{\displaystyle \underset{\sigma mm^{}\mu }{}}C_{mm^{}}^{r\mathrm{\Lambda }\mu }\widehat{Q}_{i\mathrm{\Lambda }\mu }\widehat{c}_{\sigma m}^{}\widehat{c}_{\sigma m^{}},`$ (5)
$`\widehat{H}_{\mathrm{e}\mathrm{e}}`$ $`=`$ $`{\displaystyle \frac{1}{2}}{\displaystyle \underset{\sigma ,\sigma ^{}}{}}{\displaystyle \underset{\genfrac{}{}{0pt}{}{mm^{}}{kk^{}}}{}}w_{\sigma ,\sigma ^{}}(m,m^{};k,k^{})\widehat{c}_{\sigma m}^{}\widehat{c}_{\sigma ^{}m^{}}^{}\widehat{c}_{\sigma ^{}k^{}}\widehat{c}_{\sigma k}.`$ (6)
are respectively the one-electron Hamiltonian, the vibron kinetic energy, the harmonic restoring potential toward the equilibrium configuration of neutral C60, the electron-vibron coupling (in the linear JT approximation) Manini01 ; hbyh , and finally the mutual Coulomb matrix element representing intra-molecular repulsion between the holes/electrons Lueders02 . Here $`\widehat{c}_{\sigma m}^{}`$ denote creation operators of either a hole in the HOMO or an electron in the LUMO, described by the single-particle wave functions $`\phi _{m\sigma }(𝐫)`$. $`\sigma `$ indicates the spin projection; $`m`$ labels the component within the degenerate electronic multiplets, according to the $`C_5`$ character from the $`I_hD_5C_5`$ group chain hbyh ; Butler81 . $`i`$ enumerates the vibration modes of symmetry $`\mathrm{\Lambda }`$ (2 $`A_g`$, 8 $`H_h`$, and 6 $`G_g`$ modes, the latter being JT active in the hole case only). $`C_{mm^{}}^{r\mathrm{\Lambda }\mu }`$ are Clebsch-Gordan coefficients Butler81  of the icosahedral group $`I_h`$, for coupling $`h_u`$/$`t_{1u}`$ states to phonons of symmetry $`\mathrm{\Lambda }`$. $`r`$ is a multiplicity label, relevant for $`h_u`$ holes and $`H_g`$ vibrations only, where it takes two values, 1 and 2 Manini01 ; Butler81 . $`\widehat{Q}_{i\mathrm{\Lambda }\mu }`$ are the dimensionless molecular normal-mode vibration coordinates (measured from the adiabatic equilibrium configuration of neutral C60, in units of the length scale $`x_0(\omega _{i\lambda })=\sqrt{\mathrm{}/(\omega _{i\lambda }m_\mathrm{C})}`$ associated with each harmonic oscillator where $`m_\mathrm{C}`$ is the mass of the C atom), and $`\widehat{P}_{i\mathrm{\Lambda }\mu }`$ the corresponding conjugate momenta. Finally, spin-orbit, exceedingly small in C60 TMG , is neglected throughout.

For holes, the JT model defined by Eq. (3), (4), (5), for C$`{}_{}{}^{n+}{}_{60}{}^{}`$ is conventionally denoted as $`h^n(A+G+H)`$: $`h^n`$ refers to the hole occupancy of the $`h_u`$ HOMO, and $`A`$, $`G`$, $`H`$ refer to the 2 nondegenerate $`A_g`$, 6 fourfold-degenerate $`G_g`$ and 8 fivefold-degenerate $`H_g`$ molecular vibration modes that are linearly coupled to $`h_u`$ in icosahedral symmetry Manini01 ; hbyh ; CeulemansII . For electrons, the JT model is $`t^n(A+H)`$, $`t^n`$ referring to $`n`$ electrons occupying the $`t_{1u}`$ LUMO, linearly coupled to the 2 $`A_g`$ and 8 $`H_g`$ vibrational modes only. In all calculations we shall adopt the numerical values of the e-v coupling parameters $`g_{i\mathrm{\Lambda }}^r`$, listed in Table 1, previously obtained from first-principles Density DFT electronic structure calculations in Ref. Manini01 . A recent DFT calculation Saito02  based on a different functional reported couplings that are similar on the whole to those of Table 1, the main difference concerning a closer competition between $`D_{3h}`$ and $`D_{5d}`$ valleys for the distortion of C$`{}_{}{}^{1}{}_{60}{}^{}`$. The JT stabilization energy based on the DFT parameters of Ref. Manini01  is only about one fifth of that found based on the intermediate neglect of differential overlap (INDO) model Bendale92 . We think that these earlier calculations, as well as more recent Hartree-Fock (HF) estimates gosia03  also suggesting large e-v couplings and energy gains are somewhat less dependable. We believe the smaller DFT JT gains more realistic for two main reasons: (i) the HF calculations miss an important loss of correlation energy due to opening of the JT gap; (ii) preliminary results indicate that the HOMO photoemission spectrum based on the DFT parameters MGTunpublish  is in very good agreement with experiment Bruhwiler97 ; Canton02 . By contrast, for C$`{}_{}{}^{}{}_{60}{}^{}`$, DFT computed electron-phonon couplings vzr ; Schl ; Antropov ; Green96  appear to be significantly smaller than those obtained from photoemission of C$`{}_{}{}^{}{}_{60}{}^{}`$ Gunnarsson . While we can offer no explanation for that discrepancy in negative ions, we note that the DFT-derived couplings used here for C$`{}_{}{}^{n+}{}_{60}{}^{}`$ are probably also slightly underestimated, however probably only by some 10 to 20%.

The e-v couplings $`g_{i\mathrm{\Lambda }}^r`$ in Eq. (5) are dimensionless, measured in the units of the corresponding harmonic vibrational energy quantum $`\mathrm{}\omega _{i\mathrm{\Lambda }}`$. Modes (e.g. the second $`G_g`$ mode) with $`g_{i\mathrm{\Lambda }}^r1`$ are thus only weakly coupled; conversely, modes (e.g. the lowest $`H_g`$ mode) with a large $`g_{i\mathrm{\Lambda }}^r>1`$ are strongly e-v coupled. The numerical factors $`k^{A_g}=5^{\frac{1}{2}}`$, $`k^{G_g}=\left(5/4\right)^{\frac{1}{2}}`$, $`k^{H_g}=1`$ for the HOMO, and $`k^{A_g}=3^{\frac{1}{2}}`$, $`k^{H_g}=6^{\frac{1}{2}}`$ for the LUMO are introduced for compatibility with the normalization of the e-v parameters in Ref. Manini01 .

The Coulomb matrix elements are defined by:

$`w_{\sigma ,\sigma ^{}}(m,m^{};k,k^{})={\displaystyle \mathrm{d}^3r\mathrm{d}^3r^{}}`$ (7)
$`\phi _{m\sigma }^{}(𝐫)\phi _{m^{}\sigma ^{}}^{}(𝐫^{})u_{\sigma ,\sigma ^{}}(𝐫,𝐫^{})`$ $`\phi _{k\sigma }(𝐫)\phi _{k^{}\sigma ^{}}(𝐫^{})`$
where $`u_{\sigma ,\sigma ^{}}(𝐫,𝐫^{})`$ is an effective Coulomb repulsion, screened by all other electrons of the molecule (eventually also by electrons in all other molecules in a solid state compound; but we shall focus here on the isolated ion). A detailed symmetry analysis Lueders02  shows that, assuming spin-independence of the orbitals, this set of coefficients can be expressed as

$$w_{\sigma ,\sigma ^{}}(m,m^{};k,k^{})=\underset{r,r^{},\mathrm{\Lambda }}{}F^{r,r^{},\mathrm{\Lambda }}\left(\underset{\mu }{}C_{mk}^{r\mathrm{\Lambda }\mu }C_{m^{}k^{}}^{r^{}\mathrm{\Lambda }\mu }\right)$$
(8)
in terms of a minimal set of independent Slater-type parameters $`F^{r,r^{},\mathrm{\Lambda }}`$ Cowan . A DFT estimate of these parameters was previously obtained in Ref. Lueders02 , and for our calculation we adopt those values of the Coulomb parameters. They are reproduced for completeness in Table 2. Other sets of couplings, obtained by means of a simple (and clever) model for the HOMO and LUMO orbitals Nikolaev02  and by a fit to multi-configuration HF calculations gosia03 , are in substantial agreement with each other, but they are both much larger than the DFT couplings of Ref. Lueders02 , due to complete neglect of screening. We believe that the actual Coulomb parameters of C60 lie somewhere in between the DFT couplings used here and the “bare” ones of Ref. Nikolaev02 ; gosia03 , but most likely closer to the DFT ones, due to the large polarizability of C60.

For the HOMO Coulomb parameters we use the shorthands

$`F_1=F^{A_g},F_2=F^{G_g},F_3=F^{1,1,H_g},`$ (9)
$`F_4=F^{2,2,H_g},F_5=F^{1,2,H_g}.`$
The Coulomb energy connected with the total molecular charge fluctuation in the HOMO, conventionally called the hole “Hubbard U” is given by the combination

$$U=\left(\frac{F_1}{5}\frac{4F_2}{45}\frac{F_3}{9}\frac{F_4}{9}\right).$$
(10)
For electrons in the LUMO, we have instead an electron Hubbard U given by $`U=F^{A_g}/3F^{H_g}/3`$ and a Hund-rule exchange $`J=F^{H_g}/2`$.

In either case, of electron or of holes, $`U`$ defines an average Coulomb repulsion within the multiplet of states of that molecular ion C$`{}_{}{}^{n\pm }{}_{60}{}^{}`$, such that the average energy for each $`n`$

$$E^{\mathrm{ave}}(n)=ϵn+U\frac{n(n1)}{2}.$$
(11)
We observe that $`U`$ differs from a more common definition of the Hubbard repulsion in lattice models, which involves the lowest state in each $`n`$-configuration: $`U^{\mathrm{min}}=E^{\mathrm{min}}(n+1)+E^{\mathrm{min}}(n1)2E^{\mathrm{min}}(n)`$. This second definition is inconvenient here, since it depends wildly on $`n`$. The Hubbard U’s are given here for completeness, and because they will be useful in different contexts. However we must recall that the $`U`$ term is irrelevant for the determination of the ground-state spin of each C$`{}_{}{}^{n\pm }{}_{60}{}^{}`$ ion.

## 3 The adiabatic JT valleys

Though a rather idealized description of real C$`{}_{}{}^{n\pm }{}_{60}{}^{}`$ ions, the model Hamiltonian (1), does nevertheless not lend itself to an exact solution. The vibronic eigenstates are generally complicated combinations in the direct product of each (up to 252-dimensional) fixed-$`n`$ electronic space, times the infinite-dimensional space of the vibrational degrees of freedom. Even with the help of spin and orbital symmetries, exact solutions of the quantum problem (1) are only available in two limiting cases, namely the limit of weak e-v coupling MTA ; Reno ; Delos96  and that of infinitely strong e-v coupling AMT ; ManyModes ; CeulemansII ; Moate97 . For C$`{}_{}{}^{n\pm }{}_{60}{}^{}`$, where the couplings range from intermediate to large, some approximations are therefore called for. If the phonon kinetic term $`\widehat{T}_{\mathrm{vib}}`$ is neglected in the so-called adiabatic approximation, the distortion operators $`\widehat{Q}_{i\mathrm{\Lambda }\mu }`$ are replaced by c-number coordinates. This approximation yields the leading ground-state energy lowering $`(g_{i\mathrm{\Lambda }}^r)^2\mathrm{}\omega _{i\mathrm{\Lambda }}`$, exact in the limit of large e-v couplings $`g_{i\mathrm{\Lambda }}^r\mathrm{}`$. \[Note however that, in this limit, both initial assumptions of harmonic vibrations (4) and of linear e-v coupling (5) become anyway questionable\]. In Sect. 4 we shall deal with the leading quantum corrections to the adiabatic approximation $`(g_{i\mathrm{\Lambda }}^r)^0\mathrm{}\omega _{i\mathrm{\Lambda }}`$ by taking zero-point energy shifts into account.

The classical treatment of the vibration coordinates breaks the full molecular symmetry (here icosahedral symmetry) in all configurations possessing a nonzero distortion $`Q_{i\mathrm{\Lambda }\mu }`$ ($`\mathrm{\Lambda }=G_g,H_g`$). Therefore states of different icosahedral symmetry representations are in general intermixed, leaving only the total number of holes $`n`$, the total spin $`S`$ and its projection $`S_z`$ conserved in the adiabatic ground state. Here we will assume the orbitals to remain basically unchanged upon JT distortion, thus neglecting any small JT-induced change of the Coulomb Hamiltonian $`\widehat{H}_{\mathrm{e}\mathrm{e}}`$. The latter is therefore still determined according to Eqs. (6,7,8) by the same parameters $`F_i`$ of Table 2, as in the undistorted icosahedral configuration. We will also assume no change of the vibration frequencies $`\omega _{i\mathrm{\Lambda }}`$ and couplings $`g_{i\mathrm{\Lambda }}^r`$ upon charging. While this is of course at variance with much established evidence showing vibration frequency shifts in the percent range per each added electron, it is perfectly in line with the other approximations intrinsic in our model, and in its solution. We leave the $`A_g`$ modes out of the adiabatic calculation, since despite their nonzero linear e-v coupling they simply contribute a trivial spin- and symmetry-independent term

$`E^{A_g}(n)={\displaystyle \frac{1}{8}}n^2{\displaystyle \underset{i}{}}g_{iA_g}^2\mathrm{}\omega _{iA_g}`$ $`=`$ $`an^2;`$ (12)
$`a=1.79\mathrm{meV}(\mathrm{HOMO}),a`$ $`=`$ $`2.90\mathrm{meV}(\mathrm{LUMO}),`$
to the total energy $`E^{\mathrm{ave}}(n)`$ \[Eq. (11)\], which could effectively be included into $`U`$. Because of particle-hole symmetry (exchanging creation and annihilation operators) of the Hamiltonian (excluding $`H_0`$, the $`A_g`$ modes and the average $`U`$ contribution), positive charges $`n>5`$ can always be mapped onto $`n5`$, and negative $`n>3`$ onto $`n3`$.

For each charge $`n`$ and spin $`S`$ and as a function of the vibration coordinates $`𝐐`$, the lowest adiabatic potential surface $`V_{n,S}^{\mathrm{ad}}(𝐐)`$ is obtained as the sum of the lowest eigenvalue of $`\widehat{H}_{\mathrm{e}\mathrm{e}}+\widehat{H}_{\mathrm{e}\mathrm{v}}(𝐐`$) in the $`n`$-electron spin-$`S`$ sector, plus the harmonic restoring term $`V_{\mathrm{vib}}(𝐐)`$. Allowing the 64 ($`6\times 4`$ $`G_g`$ 222The $`G_g`$ modes are irrelevant for the negative ions, but relevant for positive ions plus $`8\times 5`$ $`H_g`$.) vibration coordinates $`𝐐`$ to relax, we determine the optimal distortions $`𝐐_{\mathrm{min}}`$ by full minimization of $`V_{n,S}^{\mathrm{ad}}(𝐐)`$ in the space of all vibration coordinates $`𝐐`$. Details of this minimization were previously reported in Ref. Lueders02 ; Leuven02 .

Table 3 summarizes the optimal adiabatic energies $`E_{\mathrm{adiab}}(n,S)=V_{n,S}^{\mathrm{ad}}(𝐐_{\mathrm{min}})`$. The separate vibration, e-v, and exchange contributions are specified. The results show that the adiabatic valley minima of positive C60 ions are systematically lower for high-spin states, while the adiabatic outcome for negative ions favors marginally low spin, and is essentially uncertain, with small and poorly reliable energy differences between high- and low-spin states.

Positive and negative ions differ qualitatively also in the geometric nature of the JT distortions characterizing the minimal valleys in the space of coordinates $`𝐐`$. The $`t^nH`$ model applicable to electrons in C$`{}_{}{}^{n}{}_{60}{}^{}`$ leads to a flat continuous manifold of equivalent points. The valleys are really troughs, which could be imagined as “Mexican hats” AMT ; ob72 ; ob96 ; the study of these 2-dimensional ($`n=1,2`$) and 3-dimensional ($`n=3`$) troughs is a classic topic in JT physics ob96 ; ChoB97 .

Conversely, for holes in C$`{}_{}{}^{n+}{}_{60}{}^{}`$ the $`h^n(G+H)`$ JT model gives rise to discrete sets of isolated minima Manini01 ; hbyh ; CeulemansII ; Moate96 . The nature and symmetry of these discrete valleys depends on the details of the e-v couplings and on the interplay with Coulomb interaction. We shall describe here in some detail the minima obtained in this calculation.

To identify these minima, we generate about a hundred randomly distributed distortions away from the $`I_h`$ high-symmetry point, and let the vibration coordinates relax from there to the closest energy minimum, by combined standard (simplex and conjugate-gradients) minimization algorithms. We then apply the symmetry operations of the icosahedral group to the each minimum found, locating all possible equivalent minima. Although the method employed is not exhaustive, the application of symmetry and the thoroughness of our search, carried out with a large variety of starting points guarantees in practice the retrieval of all relevant minima. We can readily discard, for example, the few cases where minimization led to saddle points or to secondary, local minima, based on simple comparison of the energy values. In this way, for each $`n`$ and $`S`$, we finally obtain the set of equivalent valleys that are global adiabatic energy minima for C$`{}_{}{}^{n+}{}_{60}{}^{}`$. The amount of “radial” distortion at the adiabatic minima for each mode is tabulated in the Appendix.

In Table 4 we summarize some global properties of the JT energy valleys for C$`{}_{}{}^{n\pm }{}_{60}{}^{}`$ in all spin sectors. In these many-mode JT systems, the local symmetry of an optimal distortion is described in terms of the subgroup $`G_{\mathrm{local}}I_h`$ of symmetry operations which leave that minimum invariant. The minima in the simple $`n=1`$ $`S=\frac{1}{2}`$ case, where e-e interactions are irrelevant, are believed to be six valleys of $`D_{5d}`$ symmetry Manini01 ; hbyh ; CeulemansII  – the alternative possibility of ten $`D_{3d}`$ valleys apparently disfavored by the specific couplings obtained for fullerene Manini01 . Table 4 reveals a symmetry between the minima for $`n=4`$ $`S=2`$ and $`n=1`$ $`S=\frac{1}{2}`$, as well as for $`n=2`$ $`S=1`$ and $`n=3`$ $`S=\frac{3}{2}`$. These symmetries are at first sight surprising, but can be readily explained by applying a particle-hole transformation to the fermion operators of only one spin kind, in the fully spin-polarized states. This transformation maps the Hamiltonian matrices of an $`n`$-particle states (apart from a constant exchange term) into those of $`(5n)`$ particle states, with a sign change of the vibron interaction $`\widehat{H}_{\mathrm{e}\mathrm{v}}`$ that shifts each minimum $`𝐐_{\mathrm{min}}`$to the opposite locations $`𝐐_{\mathrm{min}}`$. We have therefore $`V_{4,2}^{\mathrm{ad}}(𝐐)=V_{1,1/2}^{\mathrm{ad}}(𝐐)+C`$, with $`C=\frac{2}{3}F_2\frac{5}{6}F_3\frac{5}{6}F_4=238`$ meV. The same connection between the $`n=2`$ $`S=1`$ and the $`n=3`$ $`S=\frac{3}{2}`$ adiabatic potentials involves an energy shift $`C=\frac{2}{9}F_2\frac{5}{18}F_3\frac{5}{18}F_4=80`$ meV. The same symmetry relates $`n=5`$ $`S=\frac{5}{2}`$ to $`n=0`$ $`S=0`$, where no JT distortion takes place.

In general, the number of JT valleys (third column of Table 4) is related to the local symmetry. It is basically given by the ratio $`|I_h|/|G_{\mathrm{local}}|`$ of the order of the icosahedral group (120) to the order of the invariant subgroup $`G_{\mathrm{local}}`$. However, $`n=5`$ holes make an exception to this rule. Here, at half filling, in addition to the $`I_h`$ symmetry, the system is particle-hole symmetric, i.e. invariant under exchange of creation and annihilation operators of both spin kinds. This transformation leaves the Coulomb Hamiltonian $`\widehat{H}_{\mathrm{e}\mathrm{e}}`$ invariant, and again changes sign of the vibronic interaction $`\widehat{H}_{\mathrm{e}\mathrm{v}}`$: hence, given any minimum $`𝐐_{\mathrm{min}}`$, its opposite $`𝐐_{\mathrm{min}}`$ is also an equivalent minimum of the potential energy surface. For $`S=\frac{1}{2}`$, this leads to a doubling of the minima: the local $`C_{2h}`$ symmetry would lead to 30 minima, but 30 additional equivalent minima are added in the opposite positions by particle-hole symmetry. For $`S=\frac{3}{2}`$ instead, the number of minima remains 30, since for each minimum there is one of the $`I_h`$ symmetry operations, a $`C_2`$ rotation, that transforms this minimum into its opposite point333The real-space inversion, acting on the real-space displacements, leaves all JT-active normal-mode coordinates invariant, since they are even ($`g`$) under inversion..

Table 4 contains also some information about the connectivity of the minima in $`𝐐`$ space. In many cases, the specification of the number of first, second, etc. neighbors of a given minimum is sufficient to clarify completely the topology of the minima in the 64-dimensional space. In particular, the $`D_{5d}`$ wells of the $`n=1`$ $`S=\frac{1}{2}`$, of the $`n=2`$ $`S=0`$, and of the $`n=4`$ $`S=2`$ surfaces are located on the six vertexes of five-dimensional regular simplexes, generalizations of the 3D tetrahedron, each minimum being equidistant to all the others. In analogy, the connectivity of the 10 $`D_{3d}`$ minima for $`n=4`$ $`S=0`$ is the same as that depicted in Fig. 1b of Ref. hbyh  for a different situation. For the other cases of lower symmetry, the number of neighbors of any given order must be complemented by some extra connectivity information, for which we refer to previous work Leuven02 . We only observe that for $`n=2`$ $`S=1`$ (equivalently for $`n=3`$ $`S=\frac{3}{2}`$), each of the 15 minima is linked to four nearest-neighbor minima, which, in turn, are linked to more minima, forming a completely connected regular polytope. For $`n=3`$ $`S=\frac{1}{2}`$ and $`n=4`$ $`S=1`$, the 30 minima are divided into 6 pentagonal “clusters” of five nearest-neighboring minima. In contrast, for $`n=5`$ $`S=\frac{1}{2}`$, nearest-neighbor wells come in pairs. Finally, the 30 $`C_{2h}`$ minima for $`n=5`$ $`S=\frac{3}{2}`$, show the largest connectivity, and sit at the vertexes of a highly symmetric polytope.

Figure 1 pictures the electronic state of the holes at the adiabatic valleys of C$`{}_{}{}^{n+}{}_{60}{}^{}`$. As typical of JT, distortions are such that relatively large gaps open between empty and filled levels. For $`n>1`$ this single-determinant picture is only approximate: it represents the dominant uncorrelated configuration within the fully correlated exact electronic ground state at each well.

The adiabatic valleys described above are the joint result of e-v couplings and of e-e Coulomb interactions. One can understand better the specific role of Coulomb interaction for the JT distortion by comparing the number and symmetry of the valleys described above to those obtained by the same procedure in a hypothetical noninteracting case, obtained by setting all $`F_j=0`$. Doing that, we find basically the same general picture of valleys for $`n=1`$ (obviously), but also for $`n=2`$, $`n=3`$, $`n=4`$ $`S=1,\mathrm{\hspace{0.17em}2}`$ and $`n=5`$ $`S=\frac{3}{2},\frac{5}{2}`$. In all remaining cases the e-e correlations also introduces a qualitative change in the topology and local symmetry of the minima. Without interactions, 15 $`D_{2h}`$ minima would replace the 10 $`D_{3d}`$ minima for $`n=4`$ $`S=0`$; and 20 $`D_{3d}`$ minima replace the 60 $`C_{2h}`$ minima for $`n=5`$ $`S=1/2`$. In all cases (except of course $`n=1`$ and the symmetric $`n=4`$ $`S=2`$), the amount of distortion is a few per cent larger in the uncorrelated case than when exchange is included, as expected from competing interactions. For example, without correlation, the total distortion for $`n=2`$ $`S=0`$ would be 3.16, i.e. exactly twice the distortion for $`n=1`$, as routinely occurs in JT when exchange plays no role.

## 4 Zero-point quantum corrections

The vibrational quantum kinetic energy, a quantity neglected at the adiabatic level, does in fact contribute quite substantially to the JT energetics of these multi-mode systems characterized by intermediate couplings. The zero-point energy gain associated to the softening of the vibrational frequency at the JT-distorted minima is illustrated in Fig. 2. It represents the leading quantum correction to the static JT energetics ManyModes ; Leuven02 ; LeuvenError . To compute this correction for each charge $`n`$ and spin $`S`$, by finite differences we evaluate the Hessian matrix of the second-order derivatives of the lowest adiabatic potential sheet, at each of the adiabatic JT minima:

$$(n,S)_{\alpha \alpha ^{}}=\frac{^2V_{n,S}^{\mathrm{ad}}(𝐐)}{Q_\alpha Q_\alpha ^{}}|_{𝐐_{\mathrm{min}}(n,S)}$$
(13)
where $`\alpha `$ is a collective index for $`\{i\mathrm{\Lambda }\mu \}`$. The normal-mode frequencies $`\stackrel{~}{\omega }_j`$ in each well are computed by taking the square roots of the eigenvalues of the dynamical matrix defined by

$$𝒟(n,S)_{\alpha \alpha ^{}}=\delta _{\alpha \alpha ^{}}\omega _\alpha ^2+\omega _\alpha ^{1/2}\left[(n,S)_{\alpha \alpha ^{}}\delta _{\alpha \alpha ^{}}\omega _\alpha \right]\omega _\alpha ^{}^{1/2}.$$
(14)
The $`\delta _{\alpha \alpha ^{}}\omega _\alpha `$ term removes the restoring term from $`\widehat{V}_{\mathrm{vib}}`$ in $`V_{n,S}^{\mathrm{ad}}`$, and the $`\omega _\alpha ^{1/2}`$ are introduced by the standard change of variables to correct for the different “mass” coefficients of different coordinates $`Q_\alpha `$ in $`\widehat{T}_{\mathrm{vib}}`$. By retaining the harmonic expansion of the adiabatic potential around a minimum the quantum ground state energy of this potential well is estimated at $`_j\frac{1}{2}\mathrm{}\stackrel{~}{\omega }_j`$ above the classical minimum, due to zero-point motion. As illustrated in Fig. 2, the difference between this and the original zero-point energy $`_\alpha \frac{1}{2}\mathrm{}\omega _\alpha `$ at the neutral-molecule harmonic minimum provides the leading quantum correction

$$E_{\mathrm{zero}}(n,S)=\frac{1}{2}\left[\underset{j}{}\mathrm{}\stackrel{~}{\omega }_j(n,S)\underset{i\mathrm{\Lambda }\mu }{}\mathrm{}\omega _{i\mathrm{\Lambda }}\right],$$
(15)
to the “classical” valley energy $`E_{\mathrm{adiab}}`$. $`E_{\mathrm{zero}}(n,S)`$ in JT problems is systematically found to be negative in sign, corresponding to softer vibrations, and a shallower valley bottom at the new minima than for the $`n=0`$ non-JT molecule. Table 3 reports the zero-point correction computed as described above, and the estimate of the ground-state energy obtained by adding the correction $`E_{\mathrm{zero}}`$ to $`E_{\mathrm{adiab}}`$.

For C$`{}_{}{}^{n}{}_{60}{}^{}`$, the zero-point corrections favor low-spin states for both $`n=2`$ (already a $`S=0`$ ground state at the adiabatic level) and $`n=3`$, where the zero-point correction only affects $`S=1/2`$, lowering it well below the uncorrected $`S=3/2`$. Note however that in the $`t^nH`$ JT for the anions, the two ($`n=1`$ and 2) and three ($`n=3`$) “soft” modes along the trough are associated to vanishing frequencies $`\stackrel{~}{\omega }_j`$. They formally contribute a vanishing zero-point energy to the first sum of Eq. (15). In our calculation this produces unreasonably large (negative) zero-point corrections, larger even than the adiabatic energies. These null terms are correct only in the limit of infinite coupling, where the “size” of the flat trough is infinite, and indeed the free pseudorotational motion carries no zero-point energy. For C$`{}_{}{}^{n}{}_{60}{}^{}`$, where coupling is finite, and not especially large, the trough has a finite size of order $`g^2`$, which provides some amount of quantum confinement, associated to a zero-point kinetic energy of order $`g^2`$, as was described in Ref. AMT ; ob96 . These extra “confinement” corrections should be especially sizable when the vibrational wavefunctions have the nontrivial nodal structure due to the boundary conditions associated to an electronic Berry phase, i.e. for $`n=1`$, $`n=2`$ $`S=1`$, and $`n=3`$ $`S=1/2`$ AMT , but should not change the conclusion that all C$`{}_{}{}^{n}{}_{60}{}^{}`$ ions should favor low spin.

To get an estimate of the validity of the approximations employed here, we can compare with the ground state energy of C$`{}_{}{}^{}{}_{60}{}^{}`$ obtained by means of an essentially exact calculation (a Lanczos diagonalization on a truncated, but well converged, basis) of our Hamiltonian (1) with the same parameters. The exact energy gain obtained is $`76`$ meV, which falls in between the adiabatic ($`38`$ meV) and zero-point corrected ($`152`$ meV) values. Not surprisingly, in this rather weakly coupled case, the zero-point correction largely overshoots the correct value. As charges $`n>1`$ are associated to larger distortions, thus effectively to stronger couplings, we expect that the zero-point corrected energy should be of better quality there. However, the relative size of the zero-point and confinement corrections to the adiabatic energy makes the whole strong-coupling expansion rather questionable for all the anions. Thus the C$`{}_{}{}^{n}{}_{60}{}^{}`$ results as reported here serve mostly for comparison with those of the cations. For cations we expect in fact the quality of our zero-point corrected results to be substantially better.

In the C$`{}_{}{}^{n+}{}_{60}{}^{}`$ ions too, in fact, the zero-point energy corrections are rather large, but here the magnitude of the adiabatic energy gains is even larger. The difference with the anions is due both to the larger couplings and to the structure of localized minima as opposed to a flat trough. Comparison of Table 3 and Table 4 shows that situations with a larger number of minima generally yield larger values of the correction $`|E_{\mathrm{zero}}|`$. Quantum kinetic energy in this respect behaves a bit like statistical entropy, in that it favors numerous shallower minima against few deeper ones. The zero-point correction peaks at $`150`$ meV for $`n=5`$ $`S=\frac{1}{2}`$, where the minima are shallow and the lowest vibrational frequency is as small as $`\stackrel{~}{\omega }_110`$ meV in this case. On the contrary, few well spaced minima, as for $`n=1`$ $`S=1/2`$ and $`n=2`$ $`S=0`$ are associated to a smaller zero-point gain of the order $`100`$ meV. In the close competition between Coulomb physics (Hund’s rules) and JT physics (anti-Hund behavior), the zero-point correction is not irrelevant. As shown by the last column of Table 3, it reduces drastically the large adiabatic spin gap between the high-spin ground state and the lowest spin excitations for $`n=4`$ and for $`n=5`$. Remarkably, the zero-point correction favors the high-spin state instead in C$`{}_{}{}^{2+}{}_{60}{}^{}`$: the excitation energy to $`S=0`$ is enhanced by the quantum correction from 13 meV to 33 meV. Thus although the estimated spin gap is not especially large nor especially reliable, this circumstance makes in our view the prediction of a $`S=1`$ magnetic C$`{}_{}{}^{2+}{}_{60}{}^{}`$ ion stronger than for the other cations.

Could we go beyond the zero point correction, and get more accurate results? Not easily at this stage. The zero-point correction represents the $`g^0`$ term of a large-coupling expansion, where the adiabatic energy $`E_{\mathrm{adiab}}`$ is the leading ($`g^2`$) term. The next corrections to be considered, of order $`g^2`$ and higher, are associated with anharmonicity of the valleys and tunneling amongst them (in the holes case), and also to mixing of the upper adiabatic potential surfaces with the associated geometric-phase effects AMT ; hbyh ; noberry ; baer02 . A full quantitative description of these effects would imply a much more sophisticate treatment of the quantum problem than the simple semiclassic expansion applied here, and that is beyond the scope of the present paper. To get an estimate of the importance of these higher-order corrections, we can again compare, now for C$`{}_{}{}^{+}{}_{60}{}^{}`$ the adiabatic ($`69`$ meV) and the zero-point corrected ($`120`$ meV) ground-state energy gains to the exact on, obtained by a well converged Lanczos diagonalization, which is $`103`$ meV. We see that although $`E_{\mathrm{zero}}`$ still overshoots the quantum corrections the adiabatic gain, the residual error of 17 meV is now fairly small. The accuracy expected for the zero-point corrected energy gains for all other cations C$`{}_{}{}^{n+>1+}{}_{60}{}^{}`$ is even better. In fact, the distortions there are larger, tunneling is suppressed, and the approximation of isolated harmonic JT valleys should be much better than for $`n=1`$. Thus, even if a check with the Lanczos method would be too cumbersome here because of the excessive basis size required for $`n>1`$, our zero-point corrected results of Table 3 should be regarded as practically exact, for the assumed coupling parameters.

## 5 Discussion and Conclusions

The main output of this paper is a determination of the ground state spin, energy, and distortion magnitude of JT distorted C$`{}_{}{}^{n+}{}_{60}{}^{}`$ molecular ions.

Calculations include both e-e and e-v interactions as derived from earlier first-principles calculations, as well as very important quantum vibrational effects, due to the small mass of the carbon nuclei. The latter are taken into account approximately by including the changes of vibrational zero-point energy from the undistorted to the different distorted states. These zero-point corrections are shown to be generally large. In C$`{}_{}{}^{3}{}_{60}{}^{}`$ they are even capable of turning a high-spin ground state into a low-spin one. As the coupling and thus the distortions are fairly large, quadratic and higher-order (in $`𝐐`$) e-v interactions and vibration anharmonicity could also be relevant. The present calculation was however carried out strictly in the linear e-v coupling approximation.

The parameters used in this calculation, both for e-e and e-v interaction could be somewhat underestimated by the local density approximation used in their determination, as discussed in Ref. Lueders02 ; Manini01 . Consequently, both the Coulomb repulsion and the JT effective e-e attraction calculated within the local density approximation might need some correcting in their absolute values. The balance between these two opposing interactions is delicate in C$`{}_{}{}^{n}{}_{60}{}^{}`$ ions (as demonstrated by the presence of both high-spin and low-spin local ground states in different chemical environments Brouet01 ; Arovas95 ; Kiefl ; Zimmer95 ; Lukyanchuk95 ; Prassides99 ; Schilder94 ), but low-spin ground states are generally believed to prevail, in accord with the present calculation. Contrary to that, in C$`{}_{}{}^{n+}{}_{60}{}^{}`$, Hund-rule magnetism and high-spin ground states are predicted to dominate. Experimentally, so far we found no evidence concerning gas phase C$`{}_{}{}^{n+}{}_{60}{}^{}`$ ions that we could usefully address. We do not know at this moment whether the lifetime of positive ions against fragmentation would permit experiments to be conducted, and if so whether the ground-state spins and JT distortions could be determined and compared with our predictions. Singly charged C$`{}_{}{}^{+}{}_{60}{}^{}`$ ions have been created in solution Reed00 , in molecular-beam photoemission Bruhwiler97 ; Canton02 , and in storage rings Tomita01 : but they are irrelevant to our present question.

More encouragingly, higher positive charge states have been pursued in solid-state acceptor compounds Datars95 ; Panich03 . The interplay of intra-molecular physics with electron hopping in a hypothetical fullerene-cation based solid-state conducting compound is very interesting. Our results suggest that magnetism should be important in these compounds, at least so long as the hole bands remain relatively narrow. The HOMO bands of the proposed acceptor compounds (AsF6)2C60 and (SbF6)2C60 can indeed be expected to be rather narrow. In (AsF6)2C60, based on a bct unit cell with lattice parameters $`a=b=12.8`$ Å, $`c=12.4`$ Å, we can extract a fullerene-fullerene inter-center distance 10.97 Å, significantly larger than 10.02 Å of pure C60. On the other hand, the on-site Hubbard U estimated for holes is comparable to or slightly larger than that for electrons. It seems reasonable therefore to surmise that hole-doped (AsF6)2C60 could be, like the electron-doped K3NH3C60 splitDMFT , as well as A4C60 Capone01 ; Capone02 , a Mott-JT insulator. Unlike the electron-doped compounds, where the JT distorted C$`{}_{}{}^{n}{}_{60}{}^{}`$ molecular ion was in a low-spin configuration ($`S=1/2`$ for $`n=3`$, $`S=0`$ for $`n=2,4`$), we expect in the divalent acceptor fullerene compound that the positive C$`{}_{}{}^{2+}{}_{60}{}^{}`$ ions should be in a high-spin, $`S=1`$ JT-distorted state. If so, they would constitute an exciting example of molecular Hund’s rule magnetism. The magnetic coupling between neighboring C$`{}_{}{}^{2+}{}_{60}{}^{}`$ $`S=1`$ ions in these compounds should most likely be weak and antiferromagnetic Reed00review . It might be interesting to pursue this and to seek a Néel state of some kind at very low temperatures. Pressure studies of the electron-doped compounds have revealed insulator-metal transitions such as that of Rb4C60 Kerkoud , and also insulator-superconductor transitions such as that of K3NH3C60 Margadonna01 . Pressure studies of fullerene acceptors could be an interesting line to pursue in the future. More generally, the realization of a well characterized fullerene hole conductor remains a worthy challenge for the future.

## Acknowledgments

We are indebted to M. Wierzbowska, G. Santoro, G. Onida, and L. Reatto for useful discussions. This work was supported by the European Union, contracts ERBFMRXCT970155 (TMR FULPROP), covering in particular the postdoctoral work of M. Lüders; by HPRI-CT-1999-00048 (MINOS) and the CINECA Casalecchio Supercomputing Center for computing time and for a fellowship; and by MIUR COFIN01, and FIRB RBAU017S8R of MIUR.

## Appendix A Appendix

Tables 5 and 6 report the individual amount of JT distortion associated to each normal mode of C60 at any equivalent adiabatic minimum of C$`{}_{}{}^{n\pm }{}_{60}{}^{}`$, for all spin-$`S`$ sectors. The distortions are given in the dimensionless units of the coordinate operators $`|\widehat{Q}_{i\mathrm{\Lambda }}|`$. The appropriate length scales $`x_0(\omega _{i\mathrm{\Lambda }})=\sqrt{\mathrm{}/(\omega _{i\mathrm{\Lambda }}m_\mathrm{C})}`$ for the $`G_g`$ and $`H_g`$ modes of C60 are: 76.3, 70.4, 60.3, 50.3, 46.1, 43.0, and 103.7, 80.9, 62.6, 59.8, 50.1, 47.0, 43.9, 42.1 pm, respectively. For C$`{}_{}{}^{n}{}_{60}{}^{}`$ the amount of “radial” distortion is independent of the point chosen along the trough. As expected, the modes characterized by the strongest coupling show the largest distortion. The mode associated to the largest distortion is therefore the lowest $`H_g`$ mode (see Table 1) in the cations. Note also that the $`G_g`$ modes do not contribute to the distortions of $`D_5`$ symmetry, but contribute to all the lower-symmetry minima.