text:
# NMR Quantum Computation: a Critical Evaluation

## I Introduction

Nuclear Magnetic Resonance (NMR) Ernst:1987 ; Goldman:1988 ; Munowitz:1988 ; Emsley:1992 ; Hore:1995 ; Freeman:1997  is almost unique among potential quantum technologies in that it has already been used to build small quantum computers Cory:1996 ; Cory:1997 ; Gershenfeld:1997 ; Jones:1998a ; Jones:2000b . Although other techniques have been used to implement quantum logic gates, such as the ion trap controlled-not gate Monroe:1995 , NMR provided the first complete implementation of a quantum algorithm Jones:1998a . Since then progress has been extremely rapid, with demonstrations of Deutsch’s algorithm Jones:1998a ; Chuang:1998a , Grover’s quantum search Chuang:1998b ; Jones:1998b ; Jones:1998c , versions of the Deutsch-Jozsa algorithm with three Linden:1998a  and five Marx:1999  qubits, and quantum counting Jones:1999a .

In addition to being one of the most successful quantum computing technologies, liquid state NMR is also among the oldest. Although explicit experimental demonstrations of NMR quantum computation only date from 1996 Cory:1996 , many “conventional” NMR experiments, such as COSY Jeener:1971 ; Aue:1976  and INEPT Morris:1979  can in retrospect be reinterpreted as quantum computations. These and related experiments, based on coherence transfer sequences, have been in use all over the world for decades, and are regularly used to study complex biomolecules containing thousands of nuclear spins Cavanagh:1996 . Even older than these are simpler experiments such as selective population transfer Pachler:1973 , which corresponds to the implementation of a controlled-not gate, although in this case the gate was not applied to spins in superposition states.

The rapid progress made in NMR quantum computation builds on this pre-existing experimental sophistication: decades of experience in manipulating nuclear spins in coherent states has inevitably resulted in a wide range of “tricks of the trade”. Given this success it may seem surprising that some early papers suggested that this approach might be limited to quantum computers containing about 10 qubits Warren:1997 ; Gershenfeld:1997b , while many more modern estimates are similar at 10–20 qubits. The explanation for this is simple: the highly developed nature of NMR experiments, in comparison with many other putative quantum technologies, means that the limits of the technique are fairly well known and understood. Thus unduly optimistic predictions about the power of NMR quantum computation may be easily debunked by experienced NMR spectroscopists.

## II Structure and scope

It is conventional when assessing proposals for quantum computation technologies to consider how the technique can be used to implement five basic elements required to build a quantum computer, and then to discuss whether these techniques can be scaled up for use in computers with large numbers of qubits. This approach is not appropriate for NMR, as it is already clear that all the five basic elements can be constructed; indeed they have all been experimentally demonstrated. Thus, the only topic remaining to be addressed is that of scaling. It is, however, useful to consider each of the five basic elements in turn, and discuss their impact upon the practicality of building a large NMR quantum computer.

The sections below are largely concerned with what might be called “conventional” liquid state NMR quantum computers, by which I mean computers implemented using standard techniques from liquid state NMR with spin-$`\frac{1}{2}`$ nuclei. I will, however, briefly discuss some relatively simple techniques, such as the use of optical pumping or the use of liquid crystal solvents, which may allow small extensions in the range accessible to NMR quantum computers without greatly altering the underlying physics. I will not consider solid-state NMR: although ultimately based on the same physical interactions the solid state NMR Hamiltonian Abragam:1961 ; Slichter:1990 ; Schmidt-Rohr:1994  is *much* more complicated than the liquid state form, and liquid and solid state NMR form two largely separate sub-fields. While some solid state NMR experiments could be considered as implementations of quantum simulations (*e.g.*, Zhang:1998 ), they have not as yet been used to build general purpose quantum computers. Similarly, while nuclei with spin quantum numbers greater than $`\frac{1}{2}`$ (quadrupolar nuclei) are of some theoretical interest Kessel:1999 ; Kessel:2000 , their use raises considerable experimental difficulties. Finally I will largely ignore proposed systems which use single isolated atomic nuclei in solid state devices, such as the proposal due to Kane Kane:1998 ; DiVincenzo:1998 ; although such systems are ultimately based upon NMR, they differ from current liquid state NMR implementations so profoundly that it is difficult to draw detailed parallels.

## III Initialization

Initialization is the process of placing a quantum computer in some well defined initial state, typically $`|\mathrm{𝟎}=|000\mathrm{}0`$, prior to beginning the computation. In principle any initial state is as good as any other, but in practice $`|\mathrm{𝟎}`$ is the most widely chosen, both because it corresponds to the traditional starting point of many quantum algorithms and because it often corresponds to the system’s energetic ground state. This is indeed the case in NMR quantum computation, where the computational basis corresponds with the natural experimental basis.

As initialization requires that the quantum computer be placed in the state $`|\mathrm{𝟎}`$, independent of its state before the beginning of the initialization process, it is clear that it cannot be achieved by any unitary process; thus initialization schemes must be quite different from quantum logic gates. As the desired initial state is usually an energetic ground state, initialization is typically achieved by cooling. This is not a practical approach within NMR, as the energy gaps involved are tiny compared with the Boltzmann factor at room temperature.

The energy gap between nuclear spin levels in NMR experiments is principally determined by the Zeeman interaction between the nucleus and the applied magnetic field (with the exception of the quadrupolar interaction, which does not occur in spin-$`\frac{1}{2}`$ nuclei, all other nuclear spin interactions are small compared with the main Zeeman interaction). The Zeeman splitting, $`\mathrm{\Delta }E=h\nu =\mathrm{}\gamma B`$, is usually described in terms of the corresponding Larmor frequency, $`\nu `$, and is proportional to the magnetic field strength, $`B`$, and the gyromagnetic ratio, $`\gamma `$, which is an intrinsic property of the nucleus. For the magnetic field strengths typically used in NMR experiments ($`2.3`$$`21.1\text{T}`$), the Larmor frequency of $`{}_{}{}^{1}\mathrm{H}`$ nuclei lies in the range $`100`$$`900\text{MHz}`$, corresponding to an energy of $`0.4`$$`3.7\mu \text{eV}`$. For all other nuclei (with the exception of the radioactive nucleus tritium, $`{}_{}{}^{3}\mathrm{H}`$), $`\gamma `$ is lower than for $`{}_{}{}^{1}\mathrm{H}`$, with a corresponding reduction in $`\mathrm{\Delta }E`$.

These energies are much smaller than the Boltzmann energy at room temperature (about $`25\text{meV}`$), and so at thermal equilibrium the excess population in the lower Zeeman level is tiny, less than one part in $`10^4`$. For this reason conventional liquid state NMR was long ruled out as a practical technology for quantum computation. In 1996, however, it was realised that it is not strictly necessary to start quantum computations from a pure state: a pseudo-pure, or effective pure state will suffice Cory:1996 .

### III.1 Pseudo-pure states

A pseudo-pure state is a mixed quantum state corresponding to a mixture of the desired quantum state, $`|\psi `$ and the maximally mixed state, $`\mathrm{𝟏}/N`$, where $`N=2^n`$ is the dimension of the Hilbert space describing the system. To perform a quantum computation it suffices to form the pseudo-pure ground state,

$$\rho =(1ϵ)\mathrm{𝟏}/N+ϵ|\mathrm{𝟎}\mathrm{𝟎}|.$$
(1)
An otherwise error-free quantum computer which begins a computation in such a state will end up in the state

$$\rho ^{}=(1ϵ)\mathrm{𝟏}/N+ϵ|\psi \psi |$$
(2)
where $`|\psi `$ is the result of the computation (assumed for the moment to be an eigenstate in the natural basis). This result may be immediately deduced by noting that any quantum computation corresponds to some unitary evolution of the quantum state; such evolutions are linear and have no effect upon $`\mathrm{𝟏}`$.

A quantum computer in this mixed state will return the correct answer with probability $`ϵ+(1ϵ)/N`$, and a wrong answer with probability $`(N1)(1ϵ)/N`$ (note that the maximally mixed state itself contains a fraction $`1/N`$ corresponding to the ground state). Clearly it is possible to determine the desired answer by statistical analysis of the results of a sufficiently large number of repetitions of the computation, where the number of repetitions required depends on $`ϵ`$. Equivalently it is possible to use an ensemble of quantum computers, and determine the ensemble averaged result of the computation; as long as the ensemble is sufficiently large this process will unambiguously point to the desired answer.

This latter approach is precisely that adopted for NMR quantum computation, and indeed for conventional NMR spectroscopy. NMR transition frequencies are so low that it is essentially impossible to detect a single transition, and so it is necessary to use macroscopic samples, typically containing about $`10^{17}`$ molecules, with an excess population of about $`10^{13}`$ nuclei in the low energy state. It might seem that the small signal from the excess population would be swamped by a huge background, but this is not the case as the maximally mixed state gives rise to no overall signal. This is because the signals from different components in the maximally mixed state cancel each other out; the operators corresponding to the effective observables in NMR spectra are all traceless. Thus the NMR signal arises entirely from the small excess population, and the signal from an NMR quantum computer in the pseudo pure state, equation (2), is identical to that from one in the pure state $`|\psi `$$`\psi |`$, except that the signal strength is reduced by a factor of $`ϵ`$.

### III.2 Assembling pseudo-pure states

While pseudo-pure states offer the theoretical possibility of performing quantum computations with mixed states, this approach is useful only if some practical procedure for assembling such states can be devised. For the simplest possible quantum computer, comprising a single qubit, the process is trivial, as the thermal equilibrium density matrix has exactly the desired form, but with larger systems the situation is more complicated. For a system of $`n`$ spin-$`\frac{1}{2}`$ nuclei, all of the same nuclear species (a homonuclear spin system), the $`2^n`$ eigenstates will be distributed across an evenly spaced ladder of $`n+1`$ groups of energy levels, with the number of (nearly degenerate) states within each group given by Pascal’s triangle; the population of each state will be determined by the Boltzmann equation. If the system contains several different nuclear species (a heteronuclear system), the situation is similar but slightly more complicated. Normally NMR experiments are conducted in the high temperature limit (see below), and so the pattern of excess populations will simply be proportional to the energy of each state.

Assembling a pseudo-pure state from such a complex mixture might seem difficult, but it is in fact a fairly conventional problem from the viewpoint of NMR Cory:1996 . The apparent problem is that reaching even a pseudo-pure state requires a non-unitary process, and the most obvious such process (relaxation to thermal equilibrium) leads to a state which is neither the desired state, nor unitarily related to it. Thus some additional non-unitary step is required.

In fact there are two elements commonly used in NMR pulse sequences with non-unitary effects: magnetic field gradients and phase cycling. The first of these relies on the fact that the sample forms a macroscopic ensemble; by applying Hamiltonians which vary over the sample the *ensemble averaged* evolution can be non-unitary. This is most commonly achieved by momentarily destroying the spatial homogeneity of the main magnetic field (a $`B_0`$ field gradient pulse Keeler:1994 ), but similar effects can be achieved using spatially inhomogeneous RF fields (a $`B_1`$ field gradient pulse Zhang:1995 ). The second approach relies on combining the results of several subtly different NMR experiments by post-processing; as this is done by classical methods, such processing is not confined to unitary transformations. In conventional NMR this is referred to as phase cycling Bodenhausen:1984 , and plays a central role in many experiments, although for many purposes it has now been replaced by the use of gradient techniques.

Both of these approaches have been used to assemble pseudo-pure states. The original approach of Cory *et al.* Cory:1996 , based on magnetic field gradients, is in many ways the most satisfying, but an alternative “temporal averaging” scheme based on phase cycling Knill:1998  has also proved extremely popular. Recently Knill *et al.* have described a simple and general approach Knill:1999  for building pseudo-pure states in a system of any size; their scheme may be used with either gradient or phase cycling techniques.

In addition to these schemes, another quite different approach, logical labeling, was suggested very early on by Gershenfeld and Chuang Gershenfeld:1997 . Their approach is based on the observation that while the thermal equilibrium spin density matrix for an $`n`$ spin system ($`n>1`$) does not have the desired form, equation (1), subsets of energy levels can be chosen which *do* have the correct pattern of populations; the computation is then performed within this subset of states. Although theoretically elegant this scheme appears to be more complex than the other approaches, and only two experimental implementations have been reported Vandersypen:1999 ; Dorai:1999 .

### III.3 Scaling the system up

While pseudo-pure states provide a practical approach for building small NMR quantum computers it is not possible to simply scale this approach up to larger systems. The basic problem is the size of $`ϵ`$, or rather the manner in which $`ϵ`$ scales with $`n`$, the number of spins in the system.

The exact value of $`ϵ`$ will vary with details of the scheme used to prepare the pseudo-pure state, and so it is more useful to consider an upper bound, which gives the maximum amount of pseudo-pure state which can possibly be extracted from thermal equilibrium. This is equal to the population difference between the lowest and highest energy states Warren:1997 , which for an $`n`$ spin homonuclear spin system is given by

$$ϵ=\frac{2\mathrm{sinh}(nh\nu /2kT)}{2^n\mathrm{cosh}^n(h\nu /2kT)}$$
(3)
where $`h\nu `$ is the Zeeman splitting. In the high temperature limit ($`h\nu kT`$) this expression simplifies to

$$ϵ\frac{nh\nu /kT}{2^n}.$$
(4)
Thus, in the high temperature limit the amount of pseudo-pure state which can be obtained decreases *exponentially* with the size of the spin system. To overcome this it is necessary to use an exponentially large sample, or some equivalent approach such as repeating the experiment an exponentially large number of times. It therefore seems that the pseudo-pure state approach does not scale.

In passing it should be noted that this is by no means a feature unique to NMR quantum computation: it occurs for any ensemble quantum computation scheme in the high temperature limit. Physically this is because such a system has $`2^n`$ levels, and the population deviations must be distributed among them; hence the excess population in any one state is inevitably exponentially small.

The exponentially small size of $`ϵ`$ has caused some authors to dismiss NMR quantum computation as a practical approach; while this point of view has merit it may, as discussed below, be over hasty. More recently, it has been suggested Braunstein:1998  that NMR might not be quantum mechanical at all! As NMR experiments are conducted in the high temperature limit, the density matrix is close to a maximally mixed state, and such high temperature states can always be decomposed as a mixture of product states (that is, states containing no entanglement between different nuclei). As NMR states can be described without invoking entanglement, they can therefore be modeled classically, although the classical models involved may be somewhat contrived. While this conclusion is clearly correct it has proved difficult to develop classical models which fully describe NMR experiments Schack:1999 , and the real significance of these observations remains unclear.

### III.4 High fields and low temperatures

As the problem with using pseudo-pure states arises from operating in the high temperature limit, the most obvious solution is to use either low temperatures or high fields, so that this limit no longer applies. Unfortunately NMR lies so far into the high temperature regime that this approach is unlikely to lead to success.

The critical fields and temperatures required are given by $`\mathrm{}\gamma BkT`$; for $`{}_{}{}^{1}\mathrm{H}`$ nuclei and a magnetic field strength of $`21.1\text{T}`$ (the largest NMR magnet currently available) this corresponds to $`T0.043\text{K}`$. Reaching such temperatures is possible, but clearly the sample will no longer remain in the liquid state! At such low temperatures only solid state NMR is possible. Alternatively if the sample is held at room temperature then a magnet with a field strength $`B150000\text{T}`$ will be required; this lies far beyond anything which is likely to be achieved in the foreseeable future.

The arguments above do not entirely rule out the possibility that some combination of high fields and low temperatures might one day be used to achieve reasonable polarizations, and thus interesting pseudo-pure states (in particular, it may be possible to generate high polarizations under one set of conditions and then observe them in another), but in the short term this does not seem a particularly sensible approach. There are, however, a wide range of alternatives.

### III.5 Optical pumping

A more subtle approach to increasing spin polarization is to use techniques such as optical pumping; this has the effect of decreasing the apparent temperature of the spin system without affecting the rest of the sample. Optical pumping techniques are in fact quite widely used within NMR, but it is not yet clear whether they can be usefully applied within NMR quantum computation.

The best known optical pumping process within NMR is the spin-exchange optical pumping of noble gas nuclei Walker:1997 , most notably the spin-$`\frac{1}{2}`$ nuclei $`{}_{}{}^{3}\mathrm{He}`$ and $`{}_{}{}^{129}\mathrm{Xe}`$ and the quadrupolar nucleus $`{}_{}{}^{131}\mathrm{Xe}`$. The process involves conventional optical pumping of the electron spin states of alkali metal atoms, followed by spin exchange in binary collision pairs (He) or van der Waals complexes (Xe). The resulting highly polarized noble gases have been used in a variety of NMR experiments, including NMR imaging Albert:1994 . Unfortunately noble gases are unsuitable for constructing NMR quantum computers as they consist of isolated atoms, that is systems containing only a single spin. It is in principle possible to transfer the polarization from the noble gas to more interesting species using a variety of cross polarization techniques Gaede:1995 ; Navon:1996 ; Pietrass:1999 , although it has so far proved difficult to obtain high transfer efficiency except when transferring polarization to surface species in microporous materials.

The second common form of optical pumping in NMR is quite different: optical pumping in bulk semiconductors such as Si, GaAs and InP Lampel:1968 . This approach, which is related to the DNP schemes described below, is confined to solid state systems, and it is difficult to see how it might be used to improve current liquid state implementations of NMR quantum computers.

### III.6 Other approaches

There are many other techniques which can be used to increase the initial polarization in NMR experiments: the low sensitivity of NMR is perhaps its biggest drawback in conventional spectroscopic studies, and seeking to improve sensitivity is a common research topic.

Perhaps the most important technique for sensitivity enhancement is the nuclear Overhauser effect (NOE), which arises from the correlated relaxation of two or more nuclei. If the polarization of one nucleus is perturbed from its equilibrium value cross relaxation will transfer some of this perturbation to other nearby nuclei. This technique is widely used, both to enhance the polarization of low sensitivity nuclei, and to probe internuclear distances Neuhaus:1989 . The maximum polarization gain which can be achieved, however, is proportional to $`\gamma _S/\gamma _I`$, where $`\gamma _S`$ and $`\gamma _I`$ are the gyromagnetic ratios of the sensitive and insensitive nuclei respectively, and so this method cannot be used to increase the polarization of $`{}_{}{}^{1}\mathrm{H}`$, which has the highest gyromagnetic ratio among stable nuclei.

A better approach for $`{}_{}{}^{1}\mathrm{H}`$ nuclei is to use the original Overhauser effectOverhauser:1953 ; Overhauser:1953b , which transfers polarization from electrons to nuclei. Initially greeted with scepticism Abragam:1989 , Overhauser’s theoretical predictions were confirmed by Carver and Slichter Carver:1953 , who demonstrated huge Overhauser enhancements in the spectrum of metallic $`{}_{}{}^{7}\mathrm{Li}`$. The Overhauser effect, and related phenomena collectively known as Dynamic Nuclear Polarization or DNP Hall:1997 ; Wind:1985 ; Muller-Warmutht:1983 , can be used to generate quite large polarization enhancements in a range of solid systems containing unpaired electrons, and when combined with optical techniques for pumping the electron polarization Lampel:1968 ; Patel:1999  dramatic enhancements can be observed Iinuma:2000 . However the technique performs poorly in the liquid state.

Another technique which gives enhanced polarizations is Chemically Induced Dynamic Nuclear Polarization, or CIDNP Hore:1993 . Despite the name CIDNP is unrelated to DNP; instead the non-equilibrium polarizations arise from a spin sorting mechanism which takes place during chemical reactions. This intriguing effect has proved a powerful tool for investigating a range of biomolecular systems Hore:1993 ; Lyon:1999 , but the polarizations achievable are unlikely to be useful for quantum computation.

Yet another possible approach is a family of experiments using *para*-hydrogen induced polarization, or PHIP Natterer:1997 . When hydrogen molecules are cooled into their rotational ground state, the Pauli principle dictates that the nuclear spin wavefunction of the two $`{}_{}{}^{1}\mathrm{H}`$ nuclei must be antisymmetric, and so the two nuclei must have *opposite* spin states. If *para*-hydrogen is used in an addition reaction, for example adding $`\text{H}_2`$ across a carbon–carbon double bond, then the product of the reaction will also have non-equilibrium spin states; these can be converted into a greatly enhanced polarization by conventional NMR pulse sequences. As *para*-hydrogen has a pure nuclear spin state it should in principle be possible to produce completely polarized molecules; in practice the enhancements are usually somewhat smaller Natterer:1997 .

Unlike many of the schemes discussed above, PHIP works well in the liquid state using fairly “normal” organic molecules, and so may prove useful in NMR quantum computation. Unfortunately the scheme only allows the production of molecules which are highly polarized at two sites, and while it is in principle possible to use two or more addition reactions within the same molecule to produce polarization at four or more sites creating an entire spin system by PHIP addition reactions does not seem a plausible process. However, as discussed below, in some cases it may suffice to produce high polarizations at a single spin; in this case PHIP may indeed turn out to be a useful approach.

### III.7 Reinitialization

One important point, frequently neglected in discussions of this kind, is that the methods described above are essentially methods for initializing an entire quantum computer at the start of a computation. They do not obviously permit the selective reinitialization of individual qubits in the middle of a computation. This makes it difficult to implement effective error correction schemes, as discussed in section VI below.

### III.8 Computational solutions

In addition to the physical approaches outlined above, two computational approaches might allow the problem of low spin polarization to be bypassed.

The first approach, due to Schulman and Vazirani Schulman:1998 , uses computational methods to purify mixed states. Their scheme works by concentrating the polarization from a large number of weakly polarized spins into a small number of spins which become strongly polarized; alternatively the calculation can be though of as occurring inside a small effectively pure subspace within the large spin space. Unfortunately the size of the subspace which may be extracted is $`O(ϵ^2n)`$, and so an $`n`$ spin quantum computer requires a spin system with $`O(n/ϵ^2)`$ spins; for the values of $`ϵ`$ achievable by direct cooling the resulting overhead is enormous. If, however, the polarization can be substantially increased by other means then this might provide a good method for further purification.

Another recent theoretical discovery may allow all these problems to be sidestepped, as it may be possible to perform many important quantum computations without starting from a pure (or even pseudo-pure) ground state. It has been known for some time that some quantum computations can be performed with a starting state comprising one pure qubit together with a number of qubits in the maximally mixed state Knill:1998b ; more recently it has been shown that Shor’s quantum factoring algorithm can be performed in this way Parker:2000  (but see section VII below). If this proves to be a useful approach then it could simplify the problem of constructing an NMR quantum computer, as single qubit pure states may be substantially easier to reach than their multi qubit equivalents (for example, by using *para*-hydrogen based schemes).

## IV Gates

In comparison with initialization, building quantum gates is a relatively simple process for NMR quantum computers. Indeed, as described above, many conventional NMR pulse sequences used in the molecular sciences can be viewed as sequences of quantum gates.

Any quantum gate can be built out of one qubit and two qubit gates Barenco:1995a , and early work concentrated on building these gates in two qubit NMR quantum computers (NMR systems containing two spins). Unlike many other proposed implementations of quantum computation, these gates cannot simply be transferred to larger spin systems without modification, and there was some initial concern that this transfer might prove difficult, involving an exponential increase in the complexity of the gate design. In fact, while the gates do need to be modified, the transfer can be done fairly simply, and approaches are known for doing this with only quadratic overhead. More recently some authors have moved on from simply imitating gates used in “conventional” quantum computers, and started designing gates which harness the full power of the NMR Hamiltonian directly.

### IV.1 One qubit gates

One qubit gates are easy to implement in NMR as they correspond to rotations of a single spin within its own subspace. This is most simply described using the Bloch vector model Hore:1995 ; Bloch:1956  in which the state of a spin (or indeed any qubit) is represented by a point on the surface of the Bloch sphere. One qubit gates correspond to rotations on this sphere, and can be achieved using resonant radiofrequency (RF) fields; the power and length of the RF pulse determines the rotation angle, while the phase of the RF radiation corresponds with the rotation axis within the $`xy`$ plane. Rotations around other axes can be achieved by composite rotations, implemented by applying several RF pulses in sequence Freeman:1997 .

This description assumes that it is possible to apply RF pulses selectively to individual qubits. In more conventional proposals for implementing quantum computation such qubit selection is achieved using spatial localisation: each qubit is stored on some physical object with a well defined location. This approach is not possible within NMR for three reasons. Firstly, each qubit is not stored on a single spin, but rather in an ensemble of spins distributed throughout the sample. Secondly, as the sample is in the liquid state individual spins are in continual rapid motion. Thirdly, the wavelength of RF radiation (around 1 metre) is huge compared with the separation between spins, rendering conventional spatial localisation impossible (although this could in principle be overcome by using techniques from magnetic resonance imaging (MRI) combined with enormous field gradients Callaghan:1993 ; Zhang:1998b ).

Instead of using spatial selection, NMR quantum computation relies on frequency selection to pick out individual qubits. Different nuclear species have different gyromagnetic ratios, and thus different resonance frequencies; therefore RF pulses on resonance with one spin will have little or no effect on other spins. With two or more nuclei of the same type the situation is slightly more complex, but even these will have different resonance frequencies as different chemical environments will result in different chemical shift (shielding) interactions Hore:1995 . In this case it is necessary to use low power selective RF pulses (“soft” pulses) Freeman:1997 , or their multipulse equivalents, Dante sequences Morris:1978 , in order to excite one spin while leaving other spins with only slightly different resonance frequencies untouched (the excitation bandwidth of an RF pulse depends on its power). This approach works well in small spin systems, but will be difficult in large systems as discussed below.

### IV.2 Two qubit gates

Two qubit gates are slightly more complex, as they require some sort of interaction between pairs of spins. In liquid state NMR quantum computers this is provided by scalar spin–spin coupling Hore:1995 . The NMR Hamiltonian describing two weakly coupled spins is

$$=\omega _II_z+\omega _SS_z+\pi J_{IS}2I_zS_z$$
(5)
where, following NMR practice, the spin operators are described using product operators Sorensen:1983 ; Hore:2000 , and energies are written as multiples of $`\mathrm{}`$. The one spin angular momentum operators $`I_z`$ and $`S_z`$ are simply scaled versions of the Pauli matrices (the use of I and S to describe two spin systems is traditional Solomon:1955 ); $`\omega _I`$ and $`\omega _S`$ are the resonance frequencies (Larmor frequencies) of the two spins, and $`J_{IS}`$ is the scalar spin–spin coupling (J-coupling), usually measured in Hertz. Note that this simplified Hamiltonian is only correct in the *weak coupling limit*, that is when $`|2\pi J||\omega _I\omega _S|`$.

The most obvious way to implement a two qubit gate, such as the controlled-not gate, is to use soft pulse techniques to selectively excite one spin only when its neighbouring spin is in one of its two eigenstates Barenco:1995b ; these two transitions have different energies as they are split by spin–spin coupling. This direct approach, picking out one transition from the multiplet corresponding to transitions of a single spin, is in fact identical to the old selective population transfer experiment Pachler:1973 , and so this is the oldest method for building quantum logic gates. More recently this approach has been used to build two and three qubit gates directly Linden:1998a ; Dorai:1999 ; Arvind:1999 .

This direct approach is, however, relatively unpopular. Instead, most authors Cory:1996 ; Cory:1997 ; Gershenfeld:1997 ; Jones:1998a ; Chuang:1998a ; Chuang:1998b ; Jones:1998b ; Jones:1998c ; Marx:1999 ; Jones:1999a ; Vandersypen:1999 ; Cory:1998a ; Cory:1998b ; Laflamme:1998 ; Nielsen:1998 ; Madi:1998 ; Jones:1998d ; Linden:1999a ; Linden:1999b ; Leung:1999 ; Linden:1999c ; Price:1999a ; Price:1999b ; Jones:1999b ; Collins:1999 ; Jones:2000c  prefer to use multipulse NMR techniques Ernst:1987 ; Goldman:1988 ; Munowitz:1988 ; Emsley:1992 ; Freeman:1997  to sculpt the Hamiltonian, equation (5), into a more suitable form. This is analogous to the replacement of selective population transfer by the INEPT pulse sequence Morris:1979 . The basic idea behind Hamiltonian sculpting is to use spin echoes Freeman:1997 ; Hahn:1950 ; Bagguley:1992  to refocus specific interactions in the Hamiltonian, thus creating an effective Hamiltonian obtained by rescaling elements of the original Hamiltonian, or indeed completely deleting them. While this approach to implementing two qubit gates can be described in a variety of different ways, they are all fundamentally equivalent. The central feature is the implementation of a controlled phase gate Jones:1998d , such as

$$\mathit{\varphi }=\left(\begin{array}{cccc}1& 0& 0& 0\\ 0& 1& 0& 0\\ 0& 0& 1& 0\\ 0& 0& 0& e^{i\varphi }\end{array}\right).$$
(6)
This can be decomposed in product operator notation as

$$\mathit{\varphi }=\mathrm{exp}\left[i\times {\scriptscriptstyle \frac{1}{2}}\varphi \times \left(({\scriptscriptstyle \frac{1}{2}}E)+I_z+S_z2I_zS_z\right)\right].$$
(7)
The first term ($`{\scriptscriptstyle \frac{1}{2}}E`$) can be ignored as it simply corresponds to an (undetectable) global phase; the remaining three terms can be achieved by sculpting the Hamiltonian, equation (5), into the desired form.

More recently a third approach for implementing two qubit gates has been suggested Jones:2000a . Once again this method relies on the use of controlled phase gates, but the phase shifts are generated not by using conventional dynamic phases, but instead by geometric phases Shapere:1989 , such as Berry’s phase Berry:1984 . Berry phases have been demonstrated in a wide variety of systems Shapere:1989 , including NMR Suter:1987 ; Goldman:1996  and the closely related technique of NQR Tycko:1987 ; Appelt:1994 ; Jones:1995 ; Jones:1997 . They can be used to implement controlled phase shift gates in NMR systems Jones:2000a , but it seems that this approach has few advantages for NMR quantum computation over the more conventional dynamic approach; the idea may, however, prove useful in other systems Ekert:2000a .

### IV.3 Gate times

It is not sufficient simply to show that a gate can in principle be implemented; it is also important to consider how long it takes to implement it. As discussed in section V below, what matters is not the absolute time taken, but how this compares with the natural decoherence time. It is, therefore, important to consider what factors limit the rate at which NMR quantum, logic gates operate.

One qubit gates are not only simple to build, they are also rapid to operate. As single qubit gates correspond to rotations, a reasonable measure is provided by the inverse of the time required to perform a $`2\pi `$ rotation. For a fully heteronuclear spin system (that is, a spin system containing only one spin of any given nuclear species) this rate is limited only by the available RF power and the breakdown voltages of the RF coils; typical values lie in the range $`10`$$`100\text{kHz}`$. For a homonuclear spin system the situation is more complex as it is necessary to use selective excitation. In this case the gate rate is constrained by the frequency difference between the resonances which must be excited and those which must be left untouched. This can be seen either by considering a Fourier spectral model of excitation Ernst:1987 , or by analysis of the “jump and return” pulse sequence Plateau:1982 . Thus in homonuclear spin systems the one qubit gate rate is often below $`1000\text{Hz}`$.

Two qubit gates are typically much slower. If they are implemented by direct selective excitation, then the situation is the same as for one qubit gates in homonuclear systems, except that the relevant frequency splitting is the scalar coupling between the spins, $`J_{IS}`$. A similar argument applies if the gates are implemented using multiple pulse techniques: the relevant rate is the inverse of the time required to achieve the “antiphase” condition, $`1/2J_{IS}`$. Scalar couplings are quite variable, but they are frequently less than $`10\text{Hz}`$; thus the gate times required for two qubit gates can be quite long. In our two qubit NMR quantum computer based on cytosine, a two qubit gate takes about $`70\text{ms}`$. If implemented using geometric phases Jones:2000a , the time required is even greater.

In order to reduce these two qubit gate times it is necessary to increase the size of the spin–spin coupling constant. In general this is not possible, as $`J_{IS}`$ is fixed by the chemical system chosen (it is, of course, possible to choose a new system with a larger coupling constant, but this approach is obviously quite limited). It is, however, possible to change the apparent size of $`J_{IS}`$ by partially reintroducing dipolar couplings. The scalar coupling is in fact a quite small effect in comparison with the principal spin–spin coupling interaction, dipolar coupling. This arises from the direct magnetic interaction between two magnetic dipoles, and in the high field approximation Ernst:1987

$$_D=\frac{\mu _0\gamma _I\gamma _S\mathrm{}(13\mathrm{cos}^2\theta )}{8\pi r^3}\left(3I_zS_zIS\right),$$
(8)
where $`r`$ is the length of the internuclear vector $`𝒓`$, and $`\theta `$ is the angle between $`𝒓`$ and the magnetic field. In solid samples this results in coupling between one spin and all its neighbours, but in liquids and solutions rapid motion causes $`𝒓`$, and thus $`\theta `$, to fluctuate, so that $`_D`$ is replaced by its isotropic average, which is zero. For this reason dipolar coupling has little direct effect in liquid state spectra (it cannot be entirely neglected, as it is one of the main sources of spin relaxation). The scalar coupling is a correction to the dipolar coupling which arises from the Fermi contact interaction: valence electrons can interact with two or more nuclei and thus mediate an interaction between them. Like dipolar coupling scalar coupling is anisotropic, but its isotropic average is non-zero; thus the relatively small isotropic scalar coupling is the dominant spin–spin interaction in the liquid state.

Dipolar coupling is removed because isotropic tumbling reduces it to its isotropic average. If the motion is *anisotropic* then the average may become non-zero; this can occur if the anisotropy of the molecular magnetic susceptibility causes molecules to align slightly with the magnetic field, resulting in small residual dipolar couplings. The effect is largest when the magnetic susceptibility is high, and this approach has proved helpful in investigating proteins bound to oligonucleotides Tjandra:1997 . Larger alignments, and thus larger residual couplings, can be observed using liquid crystalline solvents or cosolvents Bax:1997 , which align strongly in the magnetic field and then themselves act to order other dissolved molecules.

This approach has been used Yannoni:1999  to implement Grover’s quantum search on a two qubit NMR quantum computer based on chloroform dissolved in a liquid crystal solvent. The effective Hamiltonian in this system is

$$=\omega _II_z+\omega _SS_z+\pi (J_{IS}+2D)2I_zS_z$$
(9)
where $`D`$ is the residual dipolar coupling Yannoni:1999 , allowing the gate rate to be increased by a factor of $`8`$. It is not yet clear how generally useful this approach will be.

### IV.4 Two qubit gates in larger systems

The description above is not only confined to one and two qubit gates; it is in fact confined to such gates in two qubit computers. If these gates are to be used to build networks with three or more qubits it is necessary to consider how they will function in larger spin systems.

The situation for one qubit gates is relatively straightforward, as these can still be implemented using selective RF pulses (although the problem of frequency selection, discussed below, becomes more serious). For two qubit gates, however, a more detailed analysis is necessary. For a general $`n`$ spin system, the Hamiltonian is

$$=\underset{i}{}\omega _iI_z^i+\underset{i<k}{}\pi J_{ik}2I_z^iI_z^k,$$
(10)
including $`n`$ Larmor frequency terms for each spin, and a total of $`n(n1)/2`$ spin–spin coupling terms, connecting every pair of spins. In real systems some of the $`J_{ik}`$ coupling constants will be so small that they can be neglected, but it is still useful to consider the most general case. Consider, for example, a system of three spins, conventionally called $`I`$, $`R`$ and $`S`$; in this case there will be three Larmor frequency terms, and three spin–spin couplings, $`J_{IR}`$, $`J_{IS}`$, and $`J_{RS}`$.

It is in principle relatively simple to implement gates using the direct method. Each transition is split into four (under the influence of two couplings); if selective excitation is applied at just one of these four frequencies this corresponds to a doubly controlled three qubit gate, such as the Toffoli gate. Alternatively by exciting two transitions two qubit gates, such as controlled-not, can be achieved. In practice in large spin systems it will become difficult to pick out the right set of transition frequencies, and it is likely that some transitions will overlap.

The more common approach is to use Hamiltonian sculpting to convert equation (10) into the desired form. Clearly this requires refocusing the $`n2`$ additional Larmor frequency terms, as well as the $`(n1)(n2)/2`$ extra spin–spin couplings. This can be achieved using spin echoes Linden:1999a ; Jones:1999b . Unfortunately it is not possible to use just a single echo to refocus all the interactions; instead it is necessary to consider how the echo sequences interact with one another. The simplest method is to nest spin echoes applied to each spin within one another, but this naïve approach requires an exponentially large number of refocusing pulses. Fortunately this problem can be sidestepped by using efficient refocusing sequences Jones:1999b ; Leung:1999b , which allow refocusing to be achieved with a quadratic overhead.

It is rare to find a large spin system where all the couplings have significant size. Coupling is a fairly local effect and so large coupling constants are only found between spins that are fairly close within the spin system; thus the coupling network is described by a non-complete graph Jones:1999b . This greatly simplifies the problem: not only does it reduce the number of couplings which have to be refocused, but it also simplifies the echo patterns needed to refocus the Larmor frequencies Linden:1999c ; Jones:1999b . Thus the overhead required for refocusing echoes is greatly reduced.

It might seem that it would not be possible to implement all the desired logic gates in such a spin system, as some of the requisite spin–spin couplings are missing. In fact this is not a problem, as long as every pair of spins is connected by some chain of couplings. Quantum swap gates Madi:1998 ; Linden:1999b  can be used to move quantum information along this chain; the overhead imposed by these swap gates is at worst linear in the size of the spin system. In most cases the advantages of using a partially coupled spin system significantly outweigh the disadvantages.

### IV.5 Multiqubit gates

As described above, NMR techniques can be used to implement conventional one and two qubit gates, and thus any desired quantum network. This approach, imitating existing theoretical models of quantum computers, was adopted by all the early papers on NMR quantum computation. It is not clear, however, that this is the best approach: it might be more sensible to consider what types of gates NMR systems are good at providing, and then seeing whether these are valuable in quantum computation. To take a simple example the natural two qubit gate for NMR systems is the controlled phase shift, not the controlled-not gate, and in many quantum algorithms phase shifts are exactly what is needed. For example, NMR quantum computers can readily implement Grover’s quantum search without using an ancilla qubit to convert oracle calls into phase shifts Chuang:1998b ; Jones:1998b ; Jones:1998c .

A more complex, but more interesting, example is the implementation of multiqubit gates. As the NMR Hamiltonian, equation (10), contains terms connecting multiple pairs of qubits, it should be possible to use this Hamiltonian to build certain multiqubit gates directly. This was briefly discussed above, when considering the direct implementation of Toffoli gates in a multi-spin system, but Hamiltonian sculpting should allow the approach to be used more widely. To date this idea has received only brief analysis Price:1999b , but this is likely to be a productive source of gates in the next few years.

### IV.6 The problem of selective excitation

From the descriptions above it might seem that implementing quantum logic gates in NMR quantum computers is essentially solved, and that the solutions scale fairly well. This is almost, but not quite, true as one major problem remains: selective excitation.

All the techniques described above rest on the assumption that it is possible to address individual qubits, so that interactions can be refocused. For NMR quantum computation (or indeed any NMR pulse sequence) this is achieved using frequency selection, rather than more conventional spatial localisation techniques, and this approach is only possible if the NMR transitions all have well separated frequencies; in particular it is simplest if the separation between any pair of Larmor frequencies is much greater than the width of the NMR multiplets, that is the sum of the spin–spin couplings. Note that in contrast with conventional NMR experiments it is not sufficient simply to selectively excite one spin; it is also essential that other spins remain *completely* unaffected.

With small spin systems this is fairly easy to achieve, but with larger systems it can become quite difficult. For example, the range of Larmor frequencies found for $`{}_{}{}^{1}\mathrm{H}`$ nuclei in simple organic compounds, and working at a $`{}_{}{}^{1}\mathrm{H}`$ frequency of about $`500\text{MHz}`$ is only about $`5000\text{Hz}`$, and this limited frequency range can soon “fill up”. Increasing the number of spins not only increases the number of NMR multiplets, but also increases the width of each multiplet by introducing more spin–spin couplings. With other nuclei the situation is similar, although usually less serious (the $`{}_{}{}^{1}\mathrm{H}`$ frequency range is unusually narrow).

A partial solution is provided by turning to heteronuclear spin systems. As the NMR frequencies of different nuclei are very different, it is trivial to achieve nucleus selective, and thus spin selective, excitation. The comparative simplicity of heteronuclear NMR quantum computation explains its early, and enduring, popularity. Unfortunately this approach can not be continued indefinitely, as the number of suitable nuclei is small, the obvious candidates being $`{}_{}{}^{1}\mathrm{H}`$, $`{}_{}{}^{13}\mathrm{C}`$, $`{}_{}{}^{15}\mathrm{N}`$, $`{}_{}{}^{19}\mathrm{F}`$ and $`{}_{}{}^{31}\mathrm{P}`$.

It seems likely that the problem of selective excitation will prove a serious difficulty in constructing large NMR quantum computers. Although it is difficult to assess exactly what the limit will be, it is notable that the largest number of spins of one nuclear type used to date is six $`{}_{}{}^{1}\mathrm{H}`$ nuclei Linden:1999c ; one other paper has described computations involving four $`{}_{}{}^{13}\mathrm{C}`$ nuclei and three $`{}_{}{}^{1}\mathrm{H}`$ nuclei Knill:1999 , while all other authors have used at most three spins of any one nuclear type. Assuming that it is practical to address six spins of each of the five nuclei listed above, this suggests a limit of around 30 qubits imposed by the problem of selective excitation. Actually designing and synthesising such a spin system is another problem entirely.

## V Decoherence

In order to perform large quantum computations it is essential that errors be kept under control. In practice this means that the decoherence time must be very long in comparison with the gate time, although methods of error correction (see section VI) allow this criterion to be slightly relaxed. The situation for NMR quantum computation might appear extremely good, as systems with very long relaxation times are known: for example, the spin–lattice relaxation time ($`T_1`$) of $`{}_{}{}^{129}\mathrm{Xe}`$ can be thousands of seconds Haake:1998 . As scalar spin–spin coupling constants can reach hundreds of Hertz, and dipolar couplings can be even larger, a naïve calculation suggests that it should be possible to implement about $`10^4`$$`10^6`$ gates before decoherence becomes a serious problem.

In fact this calculation is meaningless for two reasons. First, these extremely long relaxation times are always spin–lattice relaxation times; the spin–spin relaxation times ($`T_2`$), which provide a better measure of the decoherence rate, are much shorter (typically below ten seconds). Secondly, the relaxation times and gate rates are taken from different spin systems, and it is not possible to simultaneously achieve them in a single molecule. The long relaxation times observed for $`{}_{}{}^{129}\mathrm{Xe}`$ gas arise precisely because Xe gas atoms have only weak interactions with their neighbours, and such systems are of little apparent use for quantum computation as they provide no mechanism for logic gates. As the scalar coupling is related to an underlying dipolar coupling, and dipolar coupling is one of the two principal sources of relaxation in spin-$`\frac{1}{2}`$ nuclei, spin systems suitable for constructing NMR quantum computers inevitably possess shorter relaxation times.

One further feature of decoherence in NMR quantum computation deserves consideration. As NMR systems are ensemble quantum computers, the effect of decoherence is not simply to introduce errors, as occurs with more conventional designs. Rather these errors must be averaged over the ensemble, and if, as is often the case, these errors are fairly random in character, the overall effect is that the error terms will largely cancel out. Thus the principal effect of decoherence is to reduce the apparent signal strength. This is clearly visible in some quantum counting experiments Jones:1999a ; Cummins:2000 , where decoherence appears as an exponential decay in signal.

It is difficult to estimate a realistic limit to NMR quantum computation arising from decoherence; however, current experiments have been performed involving hundreds of logic gates Jones:1999a ; Cummins:2000 , and it seems likely that the limit is about one thousand gates.

## VI Quantum error correction

Quantum error correction, and its companion fault tolerant computation Shor:1995 ; Steane:1996 ; DiVincenzo:1996 ; Preskill:1998 ; Steane:1998 ; Steane:1999 , play a central role in considerations of the practicality of large quantum computers: while small quantum computers may handle errors fairly well the fragility of highly entangled states renders large quantum computations highly vulnerable. Error correction tackles this by diagnosing these errors and correcting them, while fault tolerant computation provides methods for minimizing the spread of errors, and in particular reducing the impact of errors in error correction schemes. Simple examples of such schemes have been implemented on NMR quantum computers Cory:1998b ; Leung:1999 .

The importance of these techniques can hardly be overstated; until their discovery many authors believed that it would be completely impossible to build a large quantum computer as it would be hopelessly error prone. Unfortunately this benefit comes at a price: error correction involves a substantial overhead as each logical qubit must be encoded using many ancilla qubits. While this overhead has been substantially reduced by new codes Steane:1999  it is still at least an order of magnitude. More importantly, however, this assumes that it is possible to reuse ancilla qubits in order to repeatedly correct errors; in turn this requires the ability to reinitialize ancilla qubits at will. With current NMR quantum computers this cannot be achieved, and it is necessary to use a supply of fresh ancilla qubits at each stage. In this case the overhead becomes so large as to be completely impractical.

## VII Read-out

Once a quantum computation has been performed it is necessary to use some read-out scheme in order to extract the result. As NMR quantum computation is implemented using an ensemble of spin systems, read-out involves ensemble measurements, and thus expectation values. This can have a number of profound consequences.

In simple cases NMR read-out is little different from more conventional schemes. Suppose that a quantum computation ends with the answer qubits in eigenstates. In this case it is only necessary to determine whether each qubit is in state $`|0`$ or $`|1`$, which is equivalent to determining the expectation value of $`\sigma _z`$. This can be achieved either by exciting the corresponding spin with an RF pulse and observing the phase of the NMR signal Jones:1998a ; Jones:1999a , or by examining the multiplet structure in the NMR spectrum of a neighbouring spin, or by a combination of these techniques Chuang:1998a .

A more interesting situation occurs when the algorithm ends with one or more answer qubits in superposition states. A conventional quantum computer will return one of the corresponding answers at random, while an ensemble quantum computer will return an ensemble average over the set of all possible answers Gershenfeld:1997 ; Jones:1999a . In most cases this result is not particularly useful, and it is necessary to recast the algorithm so that a single well defined result is obtained Gershenfeld:1997 ; Jones:1999a . In some special cases, however, ensemble measurements can be advantageous Jones:1999a .

A similar situation arises when NMR techniques are used to implement phenomena such as quantum teleportation Nielsen:1998 ; Bennett:1993 . Traditional teleportation schemes use strong measurements to project an unknown quantum state into the Bell basis; classical results from these measurements are then used to determine which of a set of unitary transformations must be used to finish the protocol. In NMR teleportation, however, such projective measurements and classical readout cannot be used. Instead it is necessary to use conditional evolution to perform the final unitary transformation Nielsen:1998 .

This lack of projective measurements may also have consequences for quantum computation using a single pure qubit Knill:1998b ; Parker:2000 . The model of Knill and Laflamme Knill:1998b  assumes only ensemble measurements, and so accurately reflects the nature of NMR quantum computation, while the work of Parker and Plenio Parker:2000  assumes that projective measurements can be made. It remains to be seen how significant this difference actually is.

## VIII Conclusions

It is useful to draw some overall conclusions about the potential usefulness of liquid state NMR as a technique for implementing *large* quantum computers. For *small* quantum computers liquid state NMR techniques are well ahead of the competition: indeed in most areas of experimental quantum information processing there quite simply is no competition! However, there are several serious difficulties with extending this approach to large systems, and it seems unlikely that any very large liquid state NMR quantum computer will ever be built.

The issue most commonly raised is initialization: the pseudo-pure states used in NMR are far from pure, with typical polarizations below $`10^4`$, and, more seriously, an exponential fall off as the size of the computer is increased. This alone would appear to limit liquid state NMR quantum computers to about $`30`$ qubits.

In fact this assessment is probably too pessimistic. There are many techniques for increasing signal strengths, and while none of them offer an immediate solution, several have potential. Furthermore, recent theoretical results suggest that pure states may be less important than previously believed. If low polarizations were the only difficulty preventing the construction of a large scale NMR quantum computer, then it seems highly likely that a solution would be found. Unfortunately there are other, more serious, problems.

Constructing quantum logic gates in small systems is easy, indeed almost trivial; this simplicity explains the rapid initial progress in NMR quantum computation. Early concerns about a potential exponential increase in the complexity of implementing these gates have proved unfounded, with the discovery of methods for implementing two qubit gates in multi-spin systems with (at worst) quadratic overhead. Little thought has, however, been paid to the problem of selective excitation and the crowding of frequency space; in my personal opinion this is likely to be the first serious barrier to building NMR quantum computers with many more than ten qubits.

The problem of decoherence is, of course, common to all potential implementations of quantum computers. The relatively long decoherence times of nuclear spins, which appear to make them good candidates as qubits, arise because they interact only weakly with their environment. Unfortunately these weak interactions are also manifested as low gate rates, and so the ratio of decoherence time to gate time is not as large as one might hope. Nevertheless NMR decoherence processes are fairly well behaved, and are not likely to prove an insuperable problem in systems of ten qubits.

The difficulty of performing practical quantum error correction schemes, arising from the lack of selective reinitialization, is a serious problem for building *large* quantum computers; this, however, is only likely to become an issue if all other difficulties are solved.

The inability to perform projective measurements, and the difficulty of dealing with ensemble averaged data, is probably not a serious problem in its own right. This property makes it difficult to use NMR experiments to test fundamental questions in quantum mechanics, but has few major implications for computation. Indeed in some cases, such as when considering the effects of decoherence, it can actually be an advantage. Unlike some other issues, however, this limitations appears to be inherent in the liquid state NMR experiment, and it is not at all clear how it can be bypassed.

Finally, it is interesting to compare current liquid state NMR quantum computers with Kane’s radically different, but ultimately related, proposal for a solid state NMR quantum computer Kane:1998 . It is notable that Kane’s proposal keeps many of the advantages of NMR, but also manages to tackle some of the most serious difficulties described above. Firstly, Kane’s proposal uses external “gates” to modulate both the Larmor frequencies and the spin–spin coupling constants of nuclei. This should remove all the difficulties with implementing quantum logic gates. Secondly, the proposal includes a scheme for making projective measurements on single spins, thus also providing a simple initialization scheme.

Even if, as seems likely, a large liquid state NMR quantum computer is never built, quantum computation will still owe much to NMR. By providing the first working quantum computers, no matter how small, NMR has reinvigorated the field. Tricks long known to NMR spectroscopists are now being applied in NMR quantum computations, and many of these will have applications in other technologies. NMR quantum computation has had, and still has, much to offer.

## Acknowledgements

I thank Mark Bowdrey, Holly Cummins, Patrick Hayden, Peter Hore, Charles Lyon and Tanja Pietraß for helpful conversations. I am grateful to the Royal Society of London for a University Research Fellowship.


format: text

text:
# TUM-HEP-366/00 LPT-Orsay/00-16 Final State Interactions and 𝜀'/𝜀: A Critical Look

## 1 Introduction

One of the crucial issues for our understanding of CP violation is the question whether the size of the observed direct CP violation in $`K_L\pi \pi `$ decays, expressed in terms of the ratio $`\epsilon ^{}/\epsilon `$, can be described within the Standard Model. Experimentally the grand average, including the results from NA31 , E731 , KTeV  and NA48  reads

$$\mathrm{Re}(\epsilon ^{}/\epsilon )=(21.2\pm 4.6)\times 10^4.$$
(1)
There are different opinions whether this result can be accommodated within the Standard Model. In  the central value of the predicted $`\epsilon ^{}/\epsilon `$ is typically by a factor of 2-3 below the data, with an estimated theoretical uncertainty of the order of $`60÷100`$ %. The result in Eq. (1), then, can only be accommodated if all relevant parameters are chosen simultaneously close to their extreme values. Higher values of $`\epsilon ^{}/\epsilon `$, compatible with the data within one standard deviation have been found, instead, in . Recent reviews can be found in .

More recently, following the previous work of Truong , it has been pointed out by Pallante and Pich  that the inclusion of final state interactions substantially affects the estimates of $`\epsilon ^{}/\epsilon `$. The size of the effect is parametrized in terms of dispersive correction factors $`_I`$ multiplying the corresponding isospin amplitudes $`A_I`$. With $`_01.4`$ and $`_20.9`$, as found in their numerical evaluation, a substantial enhancement of $`\epsilon ^{}/\epsilon `$ was obtained. Indeed, by including these factors, the authors of Ref.  find that the central value $`\epsilon ^{}/\epsilon =7.0\times 10^4`$ of  gets increased to $`15\times 10^4`$ which is much closer to the experimental average (1). Similar results, although with a different dispersive approach, have been found in .

The interesting paper of Pallante and Pich stimulated us to give a closer look to the whole procedure followed to obtain the correction factors $`_I`$. The phenomenological application of the Muskhelishvili-Omnès equation to the $`K\pi \pi `$ case requires some arguable assumptions (see Section 4). However, even within those assumptions, we found a major objection which unfortunately makes the calculation of Ref.  questionable. On the basis of symmetry arguments only, one can show that there is a point, out of the physical cut, where the amplitudes induced by left-handed operators are expected to vanish. As demonstrated below, the authors of Ref.  made an assumption on the value of the derivative of the amplitude at this point which is not justified. All their results rely on this assumption. We will show that, by replacing the latter condition with others, equally acceptable on physical grounds, it is possible to obtain very different values of the correction factors $`_I`$. Thus we conclude that the results found in  are subject to substantial uncertainties.

In spite of this, we found some interesting application of the dispersive analysis to non-perturbative calculations of weak amplitudes. For example, lattice calculations could provide a condition which replaces the arbitrary assumption on the derivative of the amplitude and fix unambiguously the factors $`_I`$ (under the hypotheses inherent to the use of the Muskhelishvili-Omnès equation in $`K\pi \pi `$ decays).

Our paper is organized as follows. In section 2 we present general formulae for the Muskhelishvili-Omnès solution of dispersion relations applied to $`K\pi \pi `$ amplitudes, focusing on the assumptions needed to obtain the final result. Using these formulae we demonstrate in Section 3 that the evaluation of the dispersive factors $`_I`$ along the lines proposed in  is ambiguous. In particular we stress that there is no justification to use the numerical values of $`_I`$ found in  in conjunction with present lattice and large-$`N_C`$ calculations of hadronic matrix elements. Similar comments apply to . In Section 4 we briefly illustrate how modifications of the technique developed in  could in principle improve the accuracy of the predictions for $`\epsilon ^{}/\epsilon `$ in conjunction with future lattice calculations. We conclude in Section 5.

## 2 General formulae

In this section we recall the basic ingredients used to derive the solution of the Muskhelishvili-Omnès equation  in the case of $`K\pi \pi `$ amplitudes. The starting point is the $`N`$-subtracted dispersion relation. We denote by $`A(s)`$ the decay amplitude of a kaon of mass $`m_K=\sqrt{s}`$ into two pions of mass $`m_\pi `$. The invariant mass of the two pions is taken as $`(p_1+p_2)^2=s`$, corresponding to the insertion of a weak operator carrying zero momentum. The following discussion applies as well to the case where $`A(s)`$ is the $`K\pi \pi `$ matrix element of a local operator renormalized at a fixed scale $`\mu `$.

Following Ref.  we assume that $`A(s)`$ is analytic in the cut $`s`$ plane, with the cut going from $`4m_\pi ^2`$ to $`\mathrm{}`$ 111 These analiticity properties of $`A(s)`$ are certainly not fully correct. However one can argue that Eq. (2) still holds to a reasonable accuracy in a region close to the physical point (see Section 4).. Further assuming that $`s^NA(s)0`$ for $`s\mathrm{}`$, we can write

$$A(s)=P_{N1}(s,s_0)+\frac{(ss_0)^N}{\pi }_{4m_\pi ^2}^{\mathrm{}}𝑑z\frac{\mathrm{Im}A(z)}{(zs_0)^N(zsiϵ)},$$
(2)
where $`P_{N1}(s,s_0)`$ is a $`N1`$ degree $`s`$ polynomial, the coefficients of which are to be fixed by $`N`$ independent conditions on the amplitude and $`s_0`$ denotes the subtraction point (in general one could choose $`N`$ different subtraction points), which has to lie outside the physical cut. Writing the imaginary part of the amplitude as

$$\mathrm{Im}A(s)=A(s)e^{i\delta (s)}\mathrm{sin}\delta (s),$$
(3)
the dispersion relation (2) becomes a Muskhelishvili-Omnès equation . Here $`\delta (s)`$ is the strong phase of the amplitude, which in the elastic region is equal to the phase shift of the $`\pi \pi `$ scattering appropriate to a given isospin channel 222 Note that even in the elastic region $`\delta (s)`$ can be identified with the phase shift measured from $`\pi \pi `$ scattering only if the dependence of the latter on the kaon mass is negligible. We thank G. Colangelo for pointing this out to us.. The general solution of this equation is given by

$$A(s)=Q_{N1}(s)O(s),$$
(4)
where

$$O(s)=\mathrm{exp}\left(\frac{1}{\pi }_{4m_\pi ^2}^{\mathrm{}}𝑑z\frac{\delta (z)}{(zsiϵ)}\right)$$
(5)
and $`Q_{N1}(s)`$ is a $`N1`$ degree polynomial. Equation (4) shows explicitly that $`N`$ independent conditions on $`A(s)`$ and the knowledge of the phase on the whole cut are sufficient to fully determine the amplitude. Note that there is no longer any reference to the subtraction point $`s_0`$ of the original dispersion relation.

We point out that, if we were able to obtain a number of conditions on $`A(s)`$ larger than $`N`$, we could reduce the sensitivity of the solution to the knowledge of $`\delta (s)`$ at large $`s`$. Indeed, we can always rewrite the solution (4) as

$`A(s)`$ $`=`$ $`Q_{N1}(s)\mathrm{exp}\left({\displaystyle \underset{i=0}{\overset{M}{}}}c_is^i\right)`$ (6)
$`\times \mathrm{exp}\left({\displaystyle \frac{s^{M+1}}{\pi }}{\displaystyle _{4m_\pi ^2}^{\mathrm{}}}𝑑z{\displaystyle \frac{\delta (z)}{z^{M+1}(zsiϵ)}}\right),`$
where the product of the first two terms is completely determined by $`N+M`$ independent conditions. If possible, this could be useful since, in practice, $`\delta (s)`$ can be extracted from the data only up to the inelastic threshold.

To make contact with the work of Pallante and Pich , we now discuss two examples on how $`A(s)`$ is determined from a specific set of conditions in the case $`N=2`$. In this case, corresponding to an amplitude going at most linearly in $`s`$ for large $`s`$, two conditions on the amplitude are required:

1. In order to fix the coefficients of $`Q_1(s)`$, a possible set of conditions is given by the knowledge of the amplitudes at two different points $`s_1`$ and $`s_2`$, namely

$$A(s_1)=A_1,A(s_2)=A_2.$$
(7)
In this case, one finds

$$A(s)=\frac{A_1O(s_2)(ss_2)+A_2O(s_1)(s_1s)}{(s_1s_2)O(s_1)O(s_2)}O(s).$$
(8)
We stress that, although the r.h.s of this equation is written in terms of $`s_{1,2}`$, the physical amplitude is obviously independent of the choice of these points, provided that $`A_{1,2}`$ are given by Eq. (7).
2. A different set of conditions can be given by

$$A(s_1)=0,A^{}(s_1)=C,$$
(9)
namely by knowing the point $`s_1`$ where the amplitude vanishes, or assumes a specific value, and its first derivative in that point. With the conditions in Eq. (9) the solution is particularly simple and takes the form

$$A(s)=C(ss_1)O(s_1)^1O(s).$$
(10)

## 3 Why we are not able to compute universal dispersive factors

We now critically examine the procedure followed by Pallante and Pich  to compute the so-called dispersive factors $`_I`$ for the $`I=0`$ and $`I=2`$ amplitudes. To this end, we start by summarizing the main steps of the procedure adopted in Ref. .

On the basis of the lowest-order chiral Lagrangian, Pallante and Pich assume that the solution of the Muskhelishvili-Omnès equation is given by

$$A_I(s)=C_I(sm_\pi ^2)\mathrm{\Omega }_I(s),$$
(11)
where

$$\mathrm{\Omega }_I(s)=\frac{O_I(s)}{O_I(m_\pi ^2)}e^{i\delta _I(s)}_I(s).$$
(12)
Here $`O_I`$ is given by Eq. (5) with $`\delta `$ replaced by $`\delta _I`$, the experimental elastic $`\pi \pi (I)`$ phase shift, integrated up to a certain cutoff. This solution corresponds to the case in Eq. (10) with $`s_1=m_\pi ^2`$, i.e. the authors of Ref.  impose $`A_I(m_\pi ^2)=0`$ and implicitly assume the knowledge of $`A_I^{}(m_\pi ^2)=C_I`$.333 The need of these two assumptions is common also to Ref. , as pointed out in . In order to fulfill the latter condition, they assume without justification that the matrix element at the physical point,

$$_I=\pi \pi (I)|_{\mathrm{eff}}|K|_{s=m_K^2},$$
(13)
provided by non-perturbative methods such as lattice QCD or large $`N_C`$ estimates, corresponds to $`C_I(sm_\pi ^2)|_{s=m_K^2}`$. Their solution can thus be written as

$$A_I(s)=_I\frac{(sm_\pi ^2)}{(m_K^2m_\pi ^2)}e^{i\delta _I(s)}_I(s)$$
(14)
and the dispersive factors $`_I`$ are simply given by

$$_I_I(m_K^2)=\left|\frac{A_I(m_K^2)}{_I}\right|=\left|\frac{O_I(m_K^2)}{O_I(m_\pi ^2)}\right|.$$
(15)
We have the following comments on this approach:

* One of the two conditions used to determine the solution is $`A_I(m_\pi ^2)=0`$. This is justified in Ref.  on the basis of the lowest-order chiral realization of $`(8_L,1_R)`$ and $`(27_L,1_R)`$ operators. The zero at $`s=m_\pi ^2`$ of the amplitudes induced by these operators actually holds beyond the lowest order . Indeed, it is a consequence of the vanishing of these amplitudes in the $`SU(3)`$ limit, as follows by an old result by Cabibbo and Gell-Mann . In modern language, we can rephrase the result of Ref.  by saying that the on-shell $`K2\pi `$ matrix element of any local $`(8_L,1_R)`$ operator invariant under $`CPS`$ symmetry  vanishes in the absence of $`SU(3)`$ breaking. Therefore we think that this condition is well justified in the case of $`(8_L,1_R)`$ operators and, particularly, in the case of $`Q_6`$ considered in .
* Our main criticism is related to the determination of the second condition on $`A_I(s)`$, namely the one on $`A_I^{}(m_\pi ^2)`$. Chiral perturbation theory alone cannot fix the value of this derivative, which must be known from some non-perturbative information. In their procedure, Pallante and Pich implicitly assume that the matrix elements determined by non-perturbative methods such as lattice or large $`N_C`$, fix the value of $`A_I^{}(m_\pi ^2)`$ according to the condition

$$A_I^{}(s=m_\pi ^2)=C_I=\frac{_I}{m_K^2m_\pi ^2}.$$
(16)
This assumption, which may look reasonable on the basis of the lowest-order chiral Lagrangian, actually involves an ambiguity of the same order of the dispersive correction itself. To illustrate this point, we make a different choice of the initial conditions (while keeping the same $`_I`$): we use $`_I`$ to fix the value of the amplitude at threshold, via the relation

$$A_I(s=4m_\pi ^2)=_I\frac{3m_\pi ^2}{m_K^2m_\pi ^2}.$$
(17)
In other words, we assume that $`_I(sm_\pi ^2)/(m_K^2m_\pi ^2)`$ provides a good approximation to the real amplitude near $`s=4m_\pi ^2`$ instead of the point $`s=m_\pi ^2`$ as was implicitly employed in . One may argue that this is also a reasonable choice because strong-interaction phases vanish at threshold, but of course this condition is as arbitrary as the one adopted in . Using this condition and $`A(s=m_\pi ^2)=0`$, from Eq. (8) we find

$$A_I(s)=_I\frac{(sm_\pi ^2)O_I(s)}{(m_K^2m_\pi ^2)O_I(4m_\pi ^2)}.$$
(18)
With the same parameterization of the phase $`\delta _0(s)`$ as in Ref.  and our choice (18), the dispersive factor for $`(8_L,1_R)`$ operators is

$$_0^{\mathrm{threshold}}=\left|\frac{O_0(m_K^2)}{O_0(4m_\pi ^2)}\right|1.1$$
(19)
instead of

$$_0^{\mathrm{PP}}=\left|\frac{O_0(m_K^2)}{O_0(m_\pi ^2)}\right|1.4.$$
(20)
With $`_0=1.1`$ (and $`_2=1.0`$) the central value $`\epsilon ^{}/\epsilon =7.0\times 10^4`$ of  gets increased to $`9\times 10^4`$, instead of $`15\times 10^4`$ found in . While the first enhancement is well within the theoretical uncertainties quoted by the various analyses , the second one would have a considerable impact on the predicted value of $`\epsilon ^{}/\epsilon `$.

Other choices of the initial conditions, equally acceptable under similar assumptions, would lead to still different results for $`_0`$. This exercise illustrates that, unless one knows the value of $`s`$ at which a given non-perturbative method provides the correct value of the amplitude (and/or its derivative), it is impossible to unambiguously compute the appropriate correction factor due to final state interactions.
* In the case of $`\mathrm{\Delta }I=3/2`$ matrix elements of $`(8_L,8_R)`$ operators, such as $`Q_8^{(3/2)}`$ considered in Ref. , the amplitude does not vanish at $`s=m_\pi ^2`$. Still the authors of  claim that the correction factor is $`_2=|O_2(m_K^2)/O_2(m_\pi ^2)|0.9`$. We can reproduce this result assuming that the dispersion relation requires only one subtraction and that the non-perturbative calculations give the correct amplitude at $`s=m_\pi ^2`$. This condition, however, appears even more arbitrary than the one used to determine $`A^{}(m_\pi ^2)`$ in the case of $`(8_L,1_R)`$ operators. Indeed in this case the point $`s=m_\pi ^2`$ does not play any special rôle. It is therefore not surprising that in a different but consistent framework, as the one discussed in , non-perturbative corrections to $`Q_8^{(3/2)}`$ are found to enhance, rather than suppress, lattice and large-$`N_C`$ estimates.

Let us then summarize the main point we want to make. While the full amplitude clearly does not depend on the choice of the value of $`s`$ at which the conditions on the amplitude are placed, the dispersive correction factors are obviously dependent on this choice as we explicitly demonstrated above. As presently we are not in a position to state precisely which value of $`s`$ the exisiting non-perturbative approaches, like lattice, $`1/N`$, etc., correspond to, it is not possible to determine uniquely the corresponding factors $`_I`$ to be incorporated in each of those methods.

Before concluding this section, we comment on other attempts present in literature to include FSI effects in $`\epsilon ^{}/\epsilon `$. The approach of Ref.  is somehow similar to the one of Ref. . In this paper, however, the integral over the cut is divided in two parts: a low-energy region from threshold up to $`\mu ^2`$ and a high-energy region from $`\mu ^2`$ up to $`\mathrm{}`$. By identifying the scale $`\mu `$ with the renormalization scale of the inserted operator, the high-energy region is claimed to be estimated in perturbation theory. The results thus obtained are in qualitative agreement with those of Ref.  and show a rough independence from the unphysical scale $`\mu `$. We stress, however, that the matching procedure adopted in this paper cannot be justified theoretically. Since we do not see a way of deriving consistently the formulae of Ref.  from first principles, we are skeptical about the approach followed in this paper.

Other recipes to include a posteriori FSI effects in non-perturbative calculations of weak amplitudes were presented in the recent literature . For these we have objections similar to those made to : it is not clear to us how to relate the theoretical values of the amplitudes, computed with some non-perturbative method, to the physical ones which include FSI. In cases where the results of non-perturbative calculations are unable to reproduce the experimental phases, it is not possible to extract unambiguously the absolute value of the amplitudes. Since corrections may be applied only if this issue is under control, we think these procedures to incorporate empirically correcting factors to account for FSI do not help to improve the accuracy of the calculation. These attempts provide at best estimates of the theoretical uncertainties, as for instance discussed in .

## 4 Further developments

In spite of the criticism discussed before, we believe the Truong-Pallante-Pich approach is interesting and deserves further investigation. For this reason, in this section we briefly discuss possible applications of this technique to improve the accuracy of theoretical predictions for $`K\pi \pi `$ matrix elements. We first want to state the assumptions needed to make this approach useful:

1. In general, in order to fix the number $`N`$ of subtractions in the dispersion relation, hence the degree of the polynomial $`Q_{N1}`$, one has to make an ansatz on the behaviour of the amplitude as $`s\mathrm{}`$. In the present case, however, Eq. (2) should be understood as an approximate equation, valid in a limited $`s`$ region close to the physical point. Indeed other sources of non-analiticity besides the cut starting at $`4m_\pi ^2`$ can appear in $`A(s)`$ due to the identification of $`s`$ with kaon mass, that is a parameter of the underlying theory. Still the solution of Eq. (2) can give a good estimate of the true amplitude if these further sources of non-analiticity are well represented by a polynomial expansion in the considered region. This is for instance the case in an effective theory where the pions are the only dynamical fields, or in the quenched approximation of QCD. In this context the number of subtractions is no longer related to the behaviour of the amplitude at large $`s`$, rather to the accuracy one needs to achieve. Large values of $`N`$ are obviously preferable, although in practice they are hardly attainable. Therefore, following Refs. , we assume that $`N=2`$ provides a reasonable approximation.
2. Above the inelastic threshold, $`\delta (s)`$ is no longer the $`\pi \pi `$ phase shift and cannot be directly extracted from the experimental data. In addition, even in the elastic region, the phase of $`A(s)`$ can be identified with the experimental $`\pi \pi `$ phase shift only assuming that the dependence of the $`\pi \pi `$ scattering amplitude on the kaon mass is negligible. Were we able to compute the weak amplitude for a large number of points, we could reduce the sensitivity of the solution to the value of $`\delta (s)`$ at large $`s`$, as shown in Eq. (6). As already stressed, this possibility is presently rather remote. In practice, the integral entering $`O(s)`$ has to be restricted to the elastic region, unless some further assumptions on the amplitudes of the other channels are made. These issues entail some uncertainties which have been partially discussed in Ref. .

Under these assumptions, we now envisage a possible implementation of this approach in lattice simulations. It has been shown that, even in the presence of chiral symmetry breaking and of the Maiani-Testa theorem , lattice calculations can obtain the physical matrix elements at threshold, corresponding to $`s=4m_\pi ^2`$ . This information, once available, combined with the constraint $`A(s=m_\pi ^2)=0`$ and with the ansatz that the amplitude grows linearly in $`s`$, is sufficient to determine the physical result for the real kaon mass (see Eq. (8)) in the case of $`(8_L,1_R)`$ operators.

Concerning $`\mathrm{\Delta }I=3/2`$ matrix elements of $`(8_L,8_R)`$ operators, one may argue that one condition is not enough to fully determine the amplitude. We stress, however, that in this case the extrapolation between the $`\pi \pi `$ threshold and the physical kaon mass is expected to be smoother, resulting in a correction factor which can be approximated by unity with high accuracy.

The evaluation of the amplitude at $`s>4m_\pi ^2`$ is particularly difficult with lattice simulations since these are performed in the Euclidean space-time. Proposals, however, exist for overcoming this problem . We finally stress that the region $`s<4m_\pi ^2`$ is not accessible to lattice calculations, as well as to any other approach, if the particles ought to be on-shell and the inserted operator carries zero momentum.

## 5 Conclusions

We have critically discussed the issue of final state interactions effects in the evaluation of the ratio $`\epsilon ^{}/\epsilon `$. Whereas we cannot exclude possible substantial enhancements of $`\epsilon ^{}/\epsilon `$ through FSI over lattice and large-$`N_C`$ estimates, our analysis demonstrates that the present calculation of the dispersive factors $`_I`$ is subject to considerable uncertainties, which prevent to draw any definite conclusion on the importance of these effects.

We summarize the main point of this paper. While the full amplitude clearly does not depend on the choice of the value of $`s`$ at which the conditions on the amplitude are placed, the dispersive correction factors are obviously dependent on this choice. As presently we are not in a position to state precisely which value of $`s`$ the exisiting non-perturbative calculations correspond to, it is not possible to determine uniquely the corresponding factors $`_I`$ to be incorporated in each of those methods.

On the other hand, we have shown that the Muskhelishvili-Omnès approach could be useful to reduce, or at least to better estimate, the uncertainties on the physical amplitudes, once lattice results on the matrix elements at threshold will be available.

## Acknowledgments

We are indebted to G. Colangelo for critical comments and discussions about the validity of dispersion relations in this context. We also thank E. Pallante and A. Pich for correspondence.
This work has been supported in part by the German Bundesministerium für Bildung und Forschung under contract 06TM874 and 05HT9WOA0. E.F. and G.I. acknowledge a partial support by the TMR Network under the EEC contract ERBFMRX-CT980169 (EURODA$`\mathrm{\Phi }`$NE). G.M. thanks the T31 group at the Technische Universität München where part of this work has been done. L.S. acknowledges a partial support by the M.U.R.S.T.


text:
# 𝐵→𝑋_𝑠𝜏⁺𝜏⁻ in a CP spontaneously broken two Higgs doublet model

## Abstract

The differential branching ratio, CP asymmetry and lepton polarization $`P_N`$ for $`BX_s\tau ^+\tau ^{}`$ in a CP spotaneously broken two Higgs doublet model are computed. It is shown that contributions of neutral Higgs bosons to the decay are quite significant when $`\mathrm{tan}\beta `$ is large and $`P_N`$ can reach five persent.

The origin of the CP violation has been one of main issues in high energy physics. The measurements of electric dipole moments of the neutron and electron and the matter-antimatter asymmetry in the universe indicate that one needs new sources of CP violation in addition to the CP violation come from CKM matrix, which has been one of motivations to search new theoretical models beyond the standard model (SM).

The minimal extension of the SM is to enlarge the Higgs sectors of the SM. It has been shown that if one adheres to the natural flavor conservation (NFC) in the Higgs sector, then a minimum of three Higgs doublets are necessary in order to have spontaneous CP violations . However, the constraint can be evaded if one allows the real and image parts of $`\varphi _1^+\varphi _2`$ have different self-couplings and adds a linear term of Re($`\varphi _1^+\varphi _2`$) in the Higgs potential (see below Eq. (1) ). Then, one can construct a CP spontaneously broken (and $`Z_2`$-symmetry softly broken) two Higgs doublet (2HDM), which is the minimal among the extensions of the SM that provide new source of CP violation.

Rare decays $`BX_sl^+l^{}(l=e,\mu )`$ have been extensively investigated in both SM and the beyond . The inclusive decay $`BX_s\tau ^+\tau ^{}`$ has also been investigated in the SM, the model II 2HDM and SUSY models with and without including the contributions of NHB . In this note we investigate the inclusive decay $`BX_s\tau ^+\tau ^{}`$ with emphasis on CP violation effect in a CP spontaniously broken 2HDM in which the up-type quarks get masses from Yukawa couplings to the one Higgs doublet $`H_2`$ and down-type quarks and leptons get masses from Yukawa couplings to the another Higgs doublet $`H_1`$. The contributions from exchanging neutral Higgs bosons now is enhanced roughly by a factor of $`tg^2\beta `$ and can compete with those from exchanging $`\gamma ,Z`$ when $`tg\beta `$ is large enough. We shall be interested in the large $`\mathrm{tan}\beta `$ limit in this note.

Consider two complex $`Y=1`$ $`SU(2)_w`$ doublet scalar fields, $`\varphi _1`$ and $`\varphi _2`$. The Higgs potential which spontaneously breaks $`SU(2)\times U(1)`$ down to $`U(1)_{EM}`$ can be written in the following form :

$`V(\varphi _1,\varphi _2)`$ $`=`$ $`{\displaystyle \underset{i=1,2}{}}[m_i^2\varphi _i^+\varphi _i+\lambda _i(\varphi _i^+\varphi _i)^2]+m_3^2Re(\varphi _1^+\varphi _2)`$ (1)
$`+\lambda _3[(\varphi _1^+\varphi _1)(\varphi _2^+\varphi _2)]+\lambda _4[\text{Re}(\varphi _1^+\varphi _2)]^2+\lambda _5[\text{Im}(\varphi _1^+\varphi _2)]^2`$
Hermiticity requires that all parameters are real so that the potential is CP conservative. It is easy to see that the minimum of the potential is at $`<\varphi _1>=v_1`$ and $`<\varphi _2>=v_2e^{i\xi },`$ thus breaking $`SU(2)\times U(1)`$ down to $`U(1)_{EM}`$ and simutaneously breaking CP, as desired.

In the case of large $`\mathrm{tan}\beta `$, if we neglect all terms proptional to $`c_\beta `$ and taken $`s_\beta =1`$ in the mass-squared matrix of neutral Higgs, one would get that one of the Higgs boson mass is 0, obviously which is conflict with current experiments. So instead, below we will discuss a special case in which a analytical solution of the mass matrix can be obtained.

Assuming $`4\lambda _1c_\beta ^2=\lambda _4\lambda _5`$ and neglecting other terms proptional to $`c_\beta `$ in the mass-squared matrix, one obtains the masses of neutral Higgs bosons

$`m_{H_1^0}^2=2(\lambda _4\lambda _5)v^2s_\psi ^2,m_{H_2^0}^2=2(\lambda _4\lambda _5)v^2c_\psi ^2,m_{H_3^0}^2=4(\lambda _2+\lambda _3)v^2`$ (2)
with the mixing angle $`\psi =\frac{\xi }{2}`$.

Then it is straightforward to obtain the couplings of neutral Higgs to fermions

$`H_1^0\overline{f}f:{\displaystyle \frac{igm_f}{2m_wc_\beta }}(s_{\xi /2}+ic_{\xi /2}\gamma _5);H_2^0\overline{f}f:{\displaystyle \frac{igm_f}{2m_wc_\beta }}(c_{\xi /2}+is_{\xi /2}\gamma _5),`$ (3)
where $`f`$ represents down-type quarks and leptons. The coupling of $`H_3^0`$ to f is not enhenced by tan$`\beta `$ and will not be given explicitly. The couplings of the charged Higgs bosons to fermions are the same as those in the model II 2HDM. This is in contrary with the model III  in which the couplings of the charged Higgs to fermions are quite different from model II. It is easy to see from Eq. (3) that the contributions come from exchanging NHB is proportional to $`\sqrt{2}G_Fs_{\xi /2}c_{\xi /2}m_f^2/\mathrm{cos}^2\beta `$, so that we have the constraint $`\sqrt{|\mathrm{sin}\xi |}\mathrm{tan}\beta <50`$ from the neutron EDM, and the constraint from the electron EDM is not stronger this. The constraints on $`\mathrm{tan}\beta `$ due to effects arising from the charged Higgs are the same as those in the model II and can be found in ref. .

The transition rate for $`bs\tau ^+\tau ^{}`$ can be computed in the framework of the QCD corrected effective weak Hamiltonian

$$H_{eff}=\frac{4G_F}{\sqrt{2}}V_{tb}V_{ts}^{}(\underset{i=1}{\overset{10}{}}C_i(\mu )O_i(\mu )+\underset{i=1}{\overset{10}{}}C_{Q_i}(\mu )Q_i(\mu ))$$
(4)
where $`O_i(i=1,\mathrm{},10)`$ is the same as that given in the ref., $`Q_i`$’s come from exchanging the neutral Higgs bosons and are defined in Ref. .

The coefficients $`C_i`$’s at $`\mu =m_W`$ have been given in the ref. and $`C_{Q_i}`$’s are (neglecting the $`O(tg\beta )`$ term)

$`C_{Q_1}(m_W)`$ $`=`$ $`{\displaystyle \frac{m_bm_\tau tg^2\beta x_t}{2sin^2\theta _W}}\{{\displaystyle \underset{i=H_1,H_2}{}}{\displaystyle \frac{A_i}{m_i^2}}(f_1B_i+f_2E_i)\},`$
$`C_{Q_2}(m_W)`$ $`=`$ $`{\displaystyle \frac{m_bm_\tau tg^2\beta x_t}{2sin^2\theta _W}}\{{\displaystyle \underset{i=H_1,H_2}{}}{\displaystyle \frac{D_i}{m_i^2}}(f_1B_i+f_2E_i)\},`$
$`C_{Q_3}(m_W)`$ $`=`$ $`{\displaystyle \frac{m_be^2}{m_\tau g_s^2}}(C_{Q_1}(m_W)+C_{Q_2}(m_W)),`$
$`C_{Q_4}(m_W)`$ $`=`$ $`{\displaystyle \frac{m_be^2}{m_\tau g_s^2}}(C_{Q_1}(m_W)C_{Q_2}(m_W)),`$
$`C_{Q_i}(m_W)`$ $`=`$ $`0,i=5,\mathrm{},10`$ (5)
where

$`A_{H_1}`$ $`=`$ $`s_{\xi /2},D_{H_1}=ic_{\xi /2},A_{H_2}=c_{\xi /2},D_{H_2}=is_{\xi /2},`$
$`B_{H_1}`$ $`=`$ $`{\displaystyle \frac{ic_{\xi /2}s_{\xi /2}}{2}},B_{H_2}={\displaystyle \frac{c_{\xi /2}+is_{\xi /2}}{2}}`$
$`E_{H_1}`$ $`=`$ $`{\displaystyle \frac{1}{2}}(s_{\xi /2}c_1+c_{\xi /2}c_2),E_{H_2}={\displaystyle \frac{1}{2}}(c_{\xi /2}c_1+s_{\xi /2}c_2)`$
$`c_1`$ $`=`$ $`x_{H^\pm }+{\displaystyle \frac{c_\xi }{2s_{\xi /2}^2}}x_{H_1}(c_\xi +is_\xi )+{\displaystyle \frac{1}{2s_{\xi /2}^2}}x_{H_1}`$
$`c_2`$ $`=`$ $`i[x_{H^\pm }+{\displaystyle \frac{c_{\xi /2}x_{H_1}}{s_{\xi /2}}}(s_\xi ic_\xi )].`$ (6)
The QCD corrections to coefficients $`C_i`$ and $`C_{Q_i}`$ can be incooperated in the standard way by using the renormalization group equations . The explict expressions of the invariant dilepton mass distribution, CP asymmetries $`A_{CP}^i`$ (i=1,2) in branching ratio and in forward-backward (F-B) asymmetry and normal polarization of lepton $`P_N`$ for $`BX_s\tau ^+\tau ^{}`$ can be found in ref. .

The following parameters have been used in the numerical calculations: $`m_t=175Gev,m_b=5.0Gev,m_c=1.6Gev,m_\tau =1.77Gev,\eta =1.724,`$ $`m_{H_1}=100Gev,m_{H^\pm }=200Gev.`$

From the numerical results, the following conclusions can be drawn. A. The contributions of NHB to the differential branching ratio $`d\mathrm{\Gamma }/ds`$ are significant when $`\mathrm{tan}\beta `$ is not smaller than 30 and the masses of NHB are in the reasonable region. For tan$`\beta `$=30, $`d\mathrm{\Gamma }/ds`$ is enhenced by a factor of 6 compared to SM. B. The direct CP violation in branching ratio $`A_{CP}^1`$ is of order $`10^4`$ which is hard to be measured. C. The direct CP violation in F-B $`A_{CP}^2`$ can reach about a few percents and is strongly dependent of the CP violation phase $`\xi `$ and comes mainly from exchanging NHBs, as expected. D. The CP-violating polarization $`P_N`$ is also strongly dependent of the CP violation phase $`\xi `$ and can be as large as 5% for some values of $`\xi `$, which should be within the luminosity reach of coming B factord comes mainly from NHB contributions in the most of range of $`\xi `$. So it is possible to discriminate the model from the other 2HDMs by measuring the CP-violated observables such as $`A_{CP}^2`$, $`P_N`$ if the nature chooses large $`\mathrm{tan}\beta `$. 222 This research was supported in part by the National Nature Science Foundation of China and the post doctoral foundation of China. S.H. Zhu gratefully acknowledges the support of K.C. Wong Education Foundation, Hong Kong.