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# Field-tuned quantum tunneling in a supramolecule dimer [Mn4]2

## Abstract

Field-tuned quantum tunneling in two single-molecule magnets coupled antiferromagnetically and formed a supramolecule dimer is studied. We obtain step-like magnetization curves by means of the numerically exact solution of the time-dependent Schrődinger equation. The steps in magnetization curves show the phenomenon of quantum resonant tunneling quantitatively. The effects of the sweeping rate of applied field is discussed. These results obtained from quantum dynamical evolution well agree with the recent experiment\[W.Wernsdorfer et al. Nature 416(2002)406\].

APCS Number: 75.50.Xx,75.45.+j,76.20.+q

The macroscopic quantum phenomena in molecular magnets has become a very attractive researching field. Many properties of these nanometer-sized magnetic particles and clusters, such as Mn12($`s=10`$), Fe8($`s=10`$) and Mn4($`s=\frac{9}{2}`$) systems, have been well studied- both experimentally and theoretically. Theoretically, studying the phenomenon of quantum resonant tunneling of these molecular magnets could be based on Landau-Zener (LZ) transitions,, or based on numerically the solution of the time-dependent Schrődinger equation,. In Landau-Zener model, the magnetization curves could be obtained in a static and approximate way. Recently a supermolecular dimer \[Mn4\]2 is reported to be synthesized successfully by Werndorfer et al.. In this kind of supermolecular dimer, two single-molecule magnets Mn4 antiferromagnetic coupled each other, which results in its quantum behavior quite different from two individual Mn4 molecule without coupling. In this paper, we calculate magnetization curves of a supermolecular dimer \[Mn4\]$`_2,`$a single-molecule magnets, by numerically exact solution of the time-dependent Schrődinger equation.

Following Wernsdorfer et al., the model Hamiltonian of the supermolecular dimer \[Mn4\]2 is

$$H=H_1+H_2+JS_1S_2,$$
(1)
where $`J`$ is the weak antiferromagnetic supercharging coupling constant. H1 and H2 are Hamiltonian for two individual Mn4 molecules in the supermolecular dimer. It is known that the model Hamiltonian of an individual Mn4 molecule is

$$H_i=DS_{zi}^2+E(S_{xi}^2S_{yi}^2)g\mu _BS_{zi}h_z(t),i=1,2,$$
(2)
where $`D`$ and $`E`$ are the axial anisotropic constants. $`h_z(t)`$ is the applied sweeping field along easy axis. We can easily obtain the energy eigenvalues of whole Hamiltonian $`H`$ (Figure 1). In experiment the sweeping rate of $`h_z(t)`$ is very slow, so we can simulate it as a step-increased field, which means the $`h_z`$ increases a value $`\mathrm{\Delta }h_z`$ every $`\tau `$ time step and keeps constant during the $`\tau `$ time intervals. Note that we can not use a sweeping rate as slow as experiment due to the limitation of our computing time. However, we can obtain the key macroscopic quantum phenomena in our calculation with relatively high sweeping rate. In this paper, we select $`D=0.72k,J=0.1k,`$and $`E=0.0317k`$. Dynamic evolution follows time-dependent schrődinger equation and can be calculated by

$$|\mathrm{\Psi }\left(t\right)=|\mathrm{\Psi }\left(t_0+n\tau \right)=\mathrm{exp}[iH(t_0+(n1)\tau )\tau ]|\mathrm{\Psi }\left(t_0+(n1)\tau \right),$$
(3)
Meanwhile, $`|\mathrm{\Psi }\left(t\right)`$ can be expanded as

$$|\mathrm{\Psi }\left(t\right)=\underset{m_1=s}{\overset{𝑆}{}}\underset{m_2=s}{\overset{𝑆}{}}a_{m_1,m_2}\left(t\right)|m_1,m_2,S=\frac{9}{2},$$
(4)
where $`|m_1,m_2`$ are the eigenstates of $`H_0`$ that is

$$H_0=DS_{z1}^2DS_{z1}^2+JS_{z1}S_{z2}g\mu _B(S_{z1}+S_{z2})h_z(t),$$
(5)
We assume the initial states to be at $`|\frac{9}{2},\frac{9}{2}`$, and the whole evolution process can be obtained by equation (4) step by step. In Ref., Wernsdorfer report five points (Figure 4 of Ref.) of resonant tunneling that result in the steps in hysteresis loops. They considered the first point is caused by the resonant transition from $`|\frac{9}{2},\frac{9}{2}`$ to$`|\frac{9}{2},\frac{9}{2}`$, and the fourth point is caused by those from $`|\frac{9}{2},\frac{9}{2}`$ to$`|\frac{9}{2},\frac{5}{2}`$. However, under the model Hamiltonian of Equation(1) and Equation(2), the transitions of these points are quenched for a half integer spin due to the parity symmetry,. Therefore, there must be some kind of transverse field components resulted from the influence of the environmental degrees, such as hyperfine and dipolar couplings, and it can be approximated a Gaussian distribution with a width $`\sigma =0.035T`$ for such additional transverse environmental field. In this paper, we simply assume it to be a constant and $`h_x=0.01T`$ along x axis, but do not lose the essential physics, the macroscopic quantum phenomena.

The magnetization along the $`z`$ axis can be simply defined by $`M=<S_{z1}+S_{z2}>`$. In Figure 2, we plot the magnetization curve responding to a time-dependent applied field with a constant transverse field $`h_x=0.01T`$. There are three steps in the magnetization curve. In order to know the details of state transitions, the states ($`|\mathrm{\Psi }\left(t\right)`$) near to two sides of resonant points are recorded in our simulation and they are shown in Table 1, where the occupied probabilities ($`\left|a_{m_1,m_2}\left(t\right)\right|^2`$) are neglected to zeros if they less than $`10^3`$. Therefore, we can get clear information of the process of evolution and transition. Figure 1 and Table 1 show that the first step occurs at $`h_z=0.198T`$ from $`|\frac{9}{2},\frac{9}{2}`$ to$`|\frac{9}{2},\frac{7}{2}`$ (and$`|\frac{7}{2},\frac{9}{2}`$), and the second step occurs at $`h_z=0.731T`$ from $`|\frac{9}{2},\frac{9}{2}`$ to$`|\frac{9}{2},\frac{5}{2}`$ (and$`|\frac{5}{2},\frac{9}{2}`$). These two resonant points fit well to experimental results (i.e. the point 2 and the point 4 of Fig.4 in Ref.). The third step occurs at $`h_z=0.812T`$ from $`|\frac{9}{2},\frac{5}{2}`$ (and$`|\frac{5}{2},\frac{9}{2}`$) to$`|\frac{7}{2},\frac{5}{2}`$ (or$`|\frac{5}{2},\frac{7}{2}`$). There is no step at $`h_z0.33T`$ in our magnetization curve, but the experiment reports a point of resonant tunneling (the point 1 in Fig.4 of Ref.). The reason is that we have used a too fast sweep rate in our simulation. We will interpret it more detail late. In our magnetization curve, since the step at $`h_z0.33T`$ from $`|\frac{9}{2},\frac{9}{2}`$ to$`|\frac{9}{2},\frac{9}{2}`$ does not occur, therefore the step at $`h_z=0.87T`$ from $`|\frac{9}{2},\frac{9}{2}`$ to$`|\frac{7}{2},\frac{9}{2}`$ (point 4 in the Fig.4 of Ref.) can not occur naturally.

In order to interpret why there is no step at $`h_z=0.33T`$ in our magnetization curve, we firstly consider a utmost-slow process. At any $`t`$ value, the eigenstates and eigenvalues (Figure 1) of whole Hamiltonian $`H(t)`$ can be calculated by

$$H(t)|\mathrm{\Phi }(E)=E|\mathrm{\Phi }(E),$$
(6)
Note that no matter how weak it is, the system always interact with environment which cause dissipation. Therefore, in a very very slow process, we can assume that the state $`|\mathrm{\Psi }(t)`$ of system evaluating from a initial state $`|\mathrm{\Psi }(0)`$ will always relax to the ground state $`|\mathrm{\Phi }(E_{\mathrm{min}})`$ of $`H(t)`$. Figure 3 shows the magnetization curve of this utmost-slow process. There are two steps at $`h_z0.3363T`$ and $`h_z0.3363T`$ in the curve. It means that the point of resonant tunneling at $`h_z0.3363T`$ (point 1 of Fig.4 of Ref.) occurs when the sweeping rate of applied field is very slow. In figure 2, the sweeping rate of applied field in our calculation is $`c=\frac{\mathrm{\Delta }h_z}{\tau }=\frac{10^5}{10^8}=1000`$ $`Tesla/s`$, which is much more larger than the ones in experiment ($`0.140`$ $`Tesla/s`$, $`0.035`$ $`Tesla/s`$ and $`0.004Tesla/s`$). Due to the limitation of our computer time, we can not do the calculation for a sweeping rate of applied field as slow as the one in experiment. We now try to simulate the magnetization process (Figure 4) only in a very sharp range of $`h_z`$ with sweeping rates as slow as the ones used in experiment. In our figure 4, (a) is calculated over a range of $`h_z`$ from $`0.3364`$ $`Tesla`$ to $`0.3362`$ $`Tesla`$ with parameters $`\tau =10^8s`$ and $`\mathrm{\Delta }h_z=10^9Tesla`$ (the sweeping rate $`0.10`$ $`Tesla/s`$); (b) is calculated over a range of $`h_z`$ from $`0.336295`$ $`Tesla`$ to $`0.336275`$ $`Tesla`$ with parameters $`\tau =10^8s`$ and $`\mathrm{\Delta }h_z=10^{10}`$ $`Tesla`$ ( the sweeping rate $`0.01Tesla/s`$); (c) is the combination of (a) and (b). A very clear step occurs at $`h_z0.336283T`$ point, and it shows that the slower sweeping rate induces the higher step occurred. The recorded states (Table 2) at transition point $`h_z0.3363`$ $`Tesla`$ show that the resonant tunneling is from $`|\frac{9}{2},\frac{9}{2}`$ to$`|\frac{9}{2},\frac{9}{2}`$ (and$`|\frac{9}{2},\frac{9}{2}`$). All these results fit well with the results of experiment. Therefore, it clear show that the reason for no step at point about $`h_z0.3363Tesla`$ is from too fast sweeping rate of the applied field in theoretical simulation. There are some small oscillations in the magnetization curve. It is caused from quantum fluctuations.

In conclusion, We have studied the phenomenon of quantum resonant tunneling in a supermolecular dimer \[Mn4\]2 of single-molecule magnets by numerically exact solution of the time-dependent Schrődinger equation. We obtain step-like magnetization curves which demonstrate quantum tunneling quantitatively. We have calculated and discussed the affect to steps caused by different sweeping rate of applied field. It shows that some steps can not occur at some resonant points when the sweeping rate is too fast, but they could appear when the sweeping rate becomes enough slow. At a very narrow region near resonant point, we slow down the sweeping rate of applied field, some quantum resonant tunnelling appeared in experiment can appear. Meanwhile, theoretical calculation show that more slow rate induces more higher transition step. The results of our calculation fit very well with the experiment. Note that since we do not take into account the effects of dissipation caused by environment, the magnetization curves we obtain can not reach a reversal saturation value even if the applied field increase to infinitive value. Therefore, if we want to calculate a whole hysteresis loop, a proper mechanism of dissipation should be taken into account.

This work is supported by National Natural Science Foundation of China.

caption

Table1: Occupied probabilities $`\left|a_{m_1,m_2}\left(t\right)\right|^2`$ at spin states $`|m_1,m_2`$ (Equation (5)) at some points of the evolution process (Figure 2). The values are neglected to zero if they are smaller than $`0.001`$.

| $`h_z(Tesla)`$ | -0.34 | -0.32 | 0.19 | 0.21 | 0.72 | 0.74 | 0.80 | 0.82 | 0.9 |
| --- | --- | --- | --- | --- | --- | --- | --- | --- | --- |
| $`|\frac{9}{2},\frac{9}{2}`$ | 0.9986 | 0.9987 | 0.9987 | 0.9861 | 0.9855 | 0.9719 | 0.9718 | 0.9718 | 0.9717 |
| $`|\frac{9}{2},\frac{7}{2}`$ | 0 | 0 | 0 | 0.0062 | 0.0061 | 0.0060 | 0.0062 | 0.0061 | 0.0060 |
| $`|\frac{7}{2},\frac{9}{2}`$ | 0 | 0 | 0 | 0.0062 | 0.0061 | 0.0060 | 0.0062 | 0.0061 | 0.0060 |
| $`|\frac{9}{2},\frac{5}{2}`$ | 0 | 0 | 0 | 0 | 0 | 0.0068 | 0.0067 | 0.0053 | 0.0053 |
| $`|\frac{5}{2},\frac{9}{2}`$ | 0 | 0 | 0 | 0 | 0 | 0.0068 | 0.0067 | 0.0053 | 0.0053 |
| $`|\frac{7}{2},\frac{5}{2}`$ | 0 | 0 | 0 | 0 | 0 | 0 | 0 | 0.0013 | 0.0013 |
| $`|\frac{5}{2},\frac{7}{2}`$ | 0 | 0 | 0 | 0 | 0 | 0 | 0 | 0.0013 | 0.0013 |
| $`Total`$ | 0.9986 | 0.9987 | 0.9987 | 0.9985 | 0.9977 | 0.9975 | 0.9977 | 0.9973 | 0.9970 |

Table2: Occupied probabilities $`\left|a_{m_1,m_2}\left(t\right)\right|^2`$ at spin states $`|m_1,m_2`$ (Equation (5)) at some points of the evolution process (Figure 4). The values are neglected to zero if they are smaller than $`0.0001`$.

| Figure 4 | (a) | | (b) | |
| --- | --- | --- | --- | --- |
| $`h_z(Tesla)`$ | -0.3364 | -0.3362 | -0.336295 | -0.336275 |
| $`|\frac{9}{2},\frac{9}{2}`$ | 1 | 0.9966 | 1 | 0.9679 |
| $`|\frac{9}{2},\frac{9}{2}`$ | 0 | 0.0016 | 0 | 0.0160 |
| $`|\frac{9}{2},\frac{9}{2}`$ | 0 | 0.0016 | 0 | 0.0160 |
| $`Total`$ | 1 | 0.9998 | 1 | 0.9999 |


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# Ray Helicity: a Geometric Invariant for Multi-dimensional Resonant Wave Conversion

## Abstract

For a multicomponent wave field propagating into a multidimensional conversion region, the rays are shown to be helical, in general. For a ray-based quantity to have a fundamental physical meaning it must be invariant under two groups of transformations: congruence transformations (which shuffle components of the multi-component wave field) and canonical transformations (which act on the ray phase space). It is shown that for conversion between two waves there is a new invariant not previously discussed: the intrinsic helicity of the ray.

PACS numbers: 03.65 Sq,42.15 Dp,42.25 Bs

For linear propagation of an $`N`$-component wave field in a (weakly) non-uniform multi-dimensional medium, the field is usefully represented by a family of rays, along which the wave phase, amplitude, and polarization propagate. (The theory is referred to as ray-tracing, WKB, or eikonal.) In a local region where two waves of different polarization have (nearly) the same frequency and wave-vector, resonant conversion occurs, and a ray of one wave splits into two rays, one of each type. In a conversion region, the WKB theory breaks down and a local theory must be developed which governs the pairwise interaction of the two resonant waves. Such a theory is represented by a $`2\times 2`$ local wave equation.

The ray equations are Hamiltonian with the determinant of the full $`N\times N`$ dispersion matrix playing the role of the Hamiltonian. In a conversion region, the local ray geometry can be used to guide the reduction from the original $`N\times N`$ theory to the local $`2\times 2`$ form , construct the local transformations which recasts the local $`2\times 2`$ wave equation into the simplest possible form, and find the local coordinates in which the $`2\times 2`$ wave equation separates. The new results reported here are: 1) In a conversion region, the six-dimensional ray phase space is locally foliated by four-dimensional invariant subspaces. Within these four-dimensional subspaces, the ray dynamics is hyperbolic in one two-dimensional subspace, and elliptic in the other (i.e. pure hyperbolic motion is not possible). 2) There is one quantity, not previously identified, that is invariant under all local congruence transformations and canonical transformations: the ray helicity.

Linear wave conversion is ubiquitous throughout physics (see, for example, references given in ). While there is a large literature on conversion in one dimension, there are relatively few studies of the multi-dimensional case (see Refs.  in physics, and  in mathematics).

We start with a general $`N`$-component field $`\mathrm{\Psi }=(\psi _1,\psi _2,\mathrm{},\psi _N)`$ in a weakly non-uniform medium. Assume the medium has three spatial dimensions for concreteness and is time-stationary, but note that the methods described can be extended to include non-stationary media as well . Denote a point in space as $`𝐱=(x_1,x_2,x_3)`$. The wave equation can always be cast into the standard form :

$$d^3x^{}𝑑t^{}D_{mn}(𝐱,𝐱^{},tt^{})\psi _n(𝐱^{},t^{})=0,m=1,2\mathrm{}N.$$
(1)
We assume that the wave kernel $`𝐃`$ is an $`N\times N`$ matrix-valued fuction of its arguments satisfying $`D_{mn}(𝐱,𝐱^{},tt^{})=D_{nm}^{}(𝐱^{},𝐱,t^{}t)`$, which gives non-dissipative wave propagation. The goal is to find the multi-component field $`\mathrm{\Psi }(𝐱,t)`$ throughout a given space-time region with fitting to appropriate initial/boundary conditions. A standard tool for this analysis is the eikonal, or WKB, method. An ansatz is used of the form $`\mathrm{\Psi }(𝐱,t)=e^{i\theta (𝐱)i\omega t}\stackrel{~}{\psi }(𝐱)\widehat{𝐞}(𝐱)`$, where $`\theta (𝐱)`$ is a rapidly varying phase, $`\stackrel{~}{\psi }(𝐱)`$ is a slowly varying scalar amplitude function (assumed real), and $`\widehat{𝐞}(𝐱)`$ is a slowly varying (complex) polarization vector. The WKB approximation breaks down near caustics and in conversion regions. The theory of caustics is well-developed , while the conversion problem in multi-dimensions is our present concern.

Starting with the wave kernel and using the Weyl calculus , we next construct the dispersion matrix, an $`N\times N`$ matrix-valued function on the ray phase space denoted $`𝐃(𝐱,𝐤)`$. From now on we denote a point in the six-dimensional ray phase space by $`𝐳(𝐱,𝐤)=(z_1,z_2,z_3,z_4,z_5,z_6)`$. If (1) is conservative (as we assume), then $`𝐃(𝐳)`$ is Hermitian at each point $`𝐳`$: $`𝐃^{}(𝐳)=𝐃(𝐳)`$. Ray propagation requires $`D(𝐳)det(𝐃)=0`$. This single scalar condition upon the six coordinates $`𝐳`$ defines the dispersion surface which is, generically, a smooth five-dimensional surface, though it may have local singularities. Conversion occurs in the vicinity of the spatial point $`𝐱_{}`$ where two different WKB waves of frequency $`\omega `$, with distinct polarization and dispersion characteristics, have nearly equal wavevectors . In the ray phase space, this requires that two branches of the dispersion surface are in close proximity near the point $`𝐳_{}=(𝐱_{},𝐤_{})`$.

Away from conversion regions (and caustics), the amplitude and polarization vary slowly following a ray. Within conversion regions, however, the polarization and amplitude vary rapidly and the WKB ansatz is no longer valid. Instead, the field locally has the form $`\mathrm{\Psi }(𝐱,t)=e^{i𝐤_{}(𝐱𝐱_{})i\omega t}\left[\psi _\alpha (𝐱)\widehat{𝐞}_\alpha +\psi _\beta (𝐱)\widehat{𝐞}_\beta \right]`$, where $`\widehat{𝐞}_\alpha `$ and $`\widehat{𝐞}_\beta `$ are the uncoupled polarizations evaluated at the conversion point. The algorithm for finding these two constant polarization vectors has been discussed elsewhere (see  for a proposed algorithm). We assume the uncoupled polarizations are given. The complex scalar amplitude functions, $`\psi _\alpha `$ and $`\psi _\beta `$, include all the effects of the coupling and have rapid variation in both amplitude and phase in the conversion region, but (after multiplication by $`exp[i𝐤_{}(𝐱𝐱_{})i\omega t]`$) they connect smoothly onto the incoming and outgoing WKB wavefunctions.

The uncoupled polarizations are used to reduce the full $`N\times N`$ dispersion matrix to the following $`2\times 2`$ reduced dispersion matrix

$$𝐃(𝐳)=\left(\begin{array}{cc}D_{\alpha \alpha }(𝐳)& D_{\alpha \beta }(𝐳)\\ D_{\alpha \beta }^{}(𝐳)& D_{\beta \beta }(𝐳)\end{array}\right)$$
(2)
with $`D_{jk}(𝐳)\widehat{𝐞}_j^{}𝐃(𝐳)\widehat{𝐞}_k`$ $`j,k=(\alpha ,\beta )`$. We now consider only the reduced dispersion matrix (which is also Hermitian). Following Littlejohn and Flynn , we use the fact that any $`2\times 2`$ Hermitian matrix can be expanded using the Pauli matrices as a basis:

$$𝐃(𝐳)B_\mu (𝐳)\sigma ^\mu =\left(\begin{array}{cc}B_0(𝐳)+B_3(𝐳)& B_1(𝐳)+iB_2(𝐳)\\ B_1(𝐳)iB_2(𝐳)& B_0(𝐳)B_3(𝐳)\end{array}\right).$$
(3)
Here, the components of the ‘four-vector’ $`B=(B_0,B_1,B_2,B_3)`$ are real scalar functions of $`𝐳`$ which are assumed to be independent in the region of interest. Taking the determinant gives $`det(𝐃)=B_0^2B_1^2B_2^2B_3^2=\eta ^{\mu \nu }B_\mu B_\nu `$, with the Minkowski tensor $`\eta diag(1,1,1,1)`$. Note that $`det(𝐃)=0`$ implies that $`B`$ must lie on the ‘light’ cone in ‘$`B`$-space’.

Rays are propagated on the dispersion surface using $`D(𝐳)=B^\mu B_\mu (𝐳)`$ as the ray Hamiltonian. Hamilton’s equations are most compactly written in terms of the Poisson bracket. For any two scalar functions, $`f(𝐳)`$ and $`g(𝐳)`$, the Poisson bracket is defined to be $`\{f,g\}_zfJ_zg`$ where the $`6\times 6`$ matrix $`J`$ is defined as

$$J\left(\begin{array}{cc}0& 1\\ 1& 0\end{array}\right)$$
(4)
with ‘$`0`$’ and ‘$`1`$’ the $`3\times 3`$ null and identity matrices, respectively. The ray Hamiltonian $`D(𝐳)`$ generates the ray evolution equations via:

$$\dot{𝐳}\frac{d𝐳}{d\sigma }=\{D,𝐳\}=J_zD.$$
(5)
Thus, $`\dot{𝐱}=_kD`$ and $`\dot{𝐤}=_xD`$. Following a ray, any scalar function $`f(𝐳)`$ changes as $`\dot{f}=\{D,f\}=\{\eta ^{\nu \rho }B_\nu B_\rho ,f\}`$. In particular, the coordinates in ‘B-space’ change as

$$\dot{B}_\mu =2\mathrm{\Omega }_\mu ^\nu B_\nu ,\mu =0,1,2,3.$$
(6)
Here $`\mathrm{\Omega }_\mu ^\nu =\eta ^{\nu \rho }\mathrm{\Omega }_{\rho \mu }`$ is a $`4\times 4`$ matrix composed of all pairwise Poisson brackets of the components $`B_\mu (𝐳)`$: $`\mathrm{\Omega }_{\rho \mu }(𝐳)\{B_\rho ,B_\mu \}=\{B_\mu ,B_\rho \}`$. The matrix $`\mathrm{\Omega }`$ plays a fundamental role in the theory; since all of its entries are Poisson brackets, the entire matrix is invariant under canonical transformations. Infinitesimal Lorentz transformations are generated by anti-symmetric matrices (meaning that the $`4\times 4`$ matrix $`\mathrm{\Lambda }(\sigma )=1+\sigma \eta \mathrm{\Omega }`$ satisfies $`\stackrel{~}{\mathrm{\Lambda }}(\sigma )\eta \mathrm{\Lambda }(\sigma )=\eta +𝒪(\sigma ^2)`$). Hence, we can associate a one-parameter family of Lorentz transformations with the ray propagation. The key idea is that the equations (6) are simply Hamilton’s equations written in a non-canonical coordinate system. (Recalling that phase space is six-dimensional, and there are only four $`B_\mu `$, we must supplement (6) by two further evolution equations for another pair of coordinates, as will be shown.) Note also that, when $`BB^{}=AB`$ for any constant linear transformation $`A`$ (not just a Lorentz transformation), the matrix of Poisson brackets $`\mathrm{\Omega }`$ transforms via $`\mathrm{\Omega }^{}=A\mathrm{\Omega }\stackrel{~}{A}`$.

The geometrical picture is as follows (see Figure (1)): the ray phase space is six-dimensional and plays the role of the base space. Over each point $`𝐳`$ there is a fiber consisting of the space of $`2\times 2`$ Hermitian matrices (‘$`D`$-space’). Equivalently, the fiber consists of the space of four-vectors $`B`$ (‘$`B`$-space’). The fiber space is four-dimensional. For each $`𝐳`$, assign a particular $`𝐃(𝐳)`$ and assume that this assignment changes smoothly as we vary the base point $`𝐳`$. This assignment defines a six-dimensional surface, denoted $`𝒮`$. We note that a ray trajectory in the phase space (a solution of (5)) is associated with a well-defined curve in $`𝒮`$ and, hence, with a well-defined curve in the fiber space. This curve obeys (6) in $`B`$-space.

The mapping between the six-dimensional section $`𝒮`$ and the six-dimensional ray phase space is smooth and one-to-one. However, the mapping from $`𝒮`$ to the four-dimensional $`D`$\- and $`B`$-spaces cannot be one-to-one. This can be clarified by an appropriate choice of local coordinates. We have assumed that the four components $`B_\mu (𝐳)`$ are locally independent functions of $`𝐳`$, hence we can use them as four local (non-canonical) coordinates in the ray phase space. These are supplemented by two further independent coordinates, call them $`F_1(𝐳)`$ and $`F_2(𝐳)`$. We can choose $`F_1`$ and $`F_2`$ to satisfy $`\{F_1,B_\mu \}=\{F_2,B_\mu \}=0,\mu =0,\mathrm{}3`$, but $`F_1`$ and $`F_2`$ are otherwise arbitrary (note that this implies $`\{F_1,F_2\}0`$). This gives us a local six-dimensional (non-canonical) coordinate system $`(B_0(𝐳),B_1(𝐳),B_2(𝐳),B_3(𝐳),F_1(𝐳),F_2(𝐳))`$. The $`B`$-coordinates change via (6), while the $`F_1`$ and $`F_2`$ do not change along the ray since they have zero Poisson bracket with the $`B_\mu `$’s. This implies that the rays lie in surfaces of constant ($`F_1,F_2`$) and, therefore, there is a natural foliation of the six-dimensional phase space, with each four-dimensional leaf labeled by the two invariants $`F_1`$ and $`F_2`$. Within each four-dimensional leaf, the three-dimensional image of the light cone $`B^\mu B_\mu (𝐳)=0`$ is a slice of the dispersion surface $`D(𝐳)=0`$. Note that we do not need to assume that we are near the apex of this cone, nor have we linearized the coordinate functions. These properties of the local ray dynamics are purely a consequence of the fact that the ray Hamiltonian is the determinant of a generic $`2\times 2`$ Hermitian matrix.

We now fix attention upon a particular leaf (i.e. fixed values of ($`F_1,F_2`$)). After restricting to a fixed leaf, the ray motion can either be viewed in the phase space (where the ray equations (5) are canonical), or in $`B`$-space (where the ray equations (6) are non-canonical). Extracting the geometrical invariants, and their physical implications, is more direct using the non-canonical coordinates.

Under a congruence transformation $`𝐐`$ with constant entries, the $`2\times 2`$ reduced dispersion matrix transforms via $`𝐃𝐃^{}𝐐^{}𝐃𝐐`$, and the determinant as $`det(𝐃^{})=Q^2det(𝐃)`$ where $`det(𝐐)Q`$. First consider $`𝐐`$ with unit determinant, $`Q=1`$. Direct calculation shows that the related four-vector $`B`$ and matrix $`\mathrm{\Omega }`$ transform to $`B_\nu ^{}=\mathrm{\Lambda }_\nu ^\mu B_\mu `$ and $`\mathrm{\Omega }^{}=\mathrm{\Lambda }\mathrm{\Omega }\stackrel{~}{\mathrm{\Lambda }}`$, respectively, where $`\mathrm{\Lambda }`$ is the $`4\times 4`$ Lorentz matrix with entries  $`(\mathrm{\Lambda }^1)_\nu ^\mu =\frac{1}{2}tr\left(\sigma _\mu 𝐐^{}\sigma _\nu 𝐐\right)`$. Notice that two $`𝐐`$’s that differ by an overall minus sign are related to the same Lorentz transformation.

The Lorentz transformations leave the Minkowski tensor $`\eta `$ invariant $`\stackrel{~}{\mathrm{\Lambda }}\eta \mathrm{\Lambda }=\eta `$. The Minkowski tensor satisfies $`\eta ^2=1`$, implying that $`\mathrm{\Lambda }^1=\eta \stackrel{~}{\mathrm{\Lambda }}\eta `$. Therefore, $`\eta \mathrm{\Omega }`$ transforms via the similarity transformation $`\eta \mathrm{\Omega }^{}=\stackrel{~}{\mathrm{\Lambda }}^1\left(\eta \mathrm{\Omega }\right)\stackrel{~}{\mathrm{\Lambda }}`$, and its characteristic polynomial is invariant under Lorentz transformations. Some algebra shows that $`P(\lambda )=det(\eta \mathrm{\Omega }\lambda )=\lambda ^4\frac{1}{2}tr((\eta \mathrm{\Omega })^2)\lambda ^2+det(\eta \mathrm{\Omega })`$. If we use the standard parametrization for generators of the Lorentz group :

$$\mathrm{\Omega }\left(\begin{array}{cccc}0& \gamma _1& \gamma _2& \gamma _3\\ \gamma _1& 0& \omega _3& \omega _2\\ \gamma _2& \omega _3& 0& \omega _1\\ \gamma _3& \omega _2& \omega _1& 0\end{array}\right)$$
(7)
then we find $`P(\lambda )=\lambda ^4+(\omega ^2\gamma ^2)\lambda ^2(\gamma \omega )^2`$. Notice that $`P(\lambda )`$ depends only upon $`\lambda ^2`$, hence the roots of $`P(\lambda )=0`$ come in plus-minus pairs. Generically, $`P(0)`$ is strictly negative, while $`P(\lambda ^2)`$ is concave upward as a function of $`\lambda ^2`$. Therefore, as a function of $`\lambda ^2`$, $`P=0`$ will have one negative root and one positive root. This implies, in turn, that as a function of $`\lambda `$, $`P=0`$ will have a pair of $`\pm `$ pure imaginary roots, and a pair of $`\pm `$ real roots. This implies that the ray motion will be a combination of elliptic and hyperbolic behaviors.

This parametrization (7) provides a useful physical interpretation for the meaning of $`\mathrm{\Omega }`$. Fix a point $`𝐳=𝐳_0`$ on the ray where $`\mathrm{\Omega }_0\mathrm{\Omega }(𝐳_0)`$ is evaluated. Now use $`\mathrm{\Omega }_0`$ to generate a one-parameter family of Lorentz transformations in $`B`$-space ($`\sigma `$ is the ray orbit parameter) $`B(\sigma )=\mathrm{\Lambda }(\sigma )B(0)exp(\sigma \eta \mathrm{\Omega }_0)B(0)`$. This provides a local approximation to the ray orbit in $`B`$-space. In that space, the ray evolution will be a combination of a rotation (generated by the $`\omega `$-subspace) and a ‘boost’, generated by the $`\gamma `$-subspace . Hence, the orbit in $`B`$-space will generically be a combination of elliptic and hyperbolic motions. But, a ray orbit in $`B`$-space is the smooth image of a ray orbit in the original phase space, hence ray orbits generated by generic $`2\times 2`$ dispersion matrices will have a combination of elliptic and hyperbolic motions. Purely hyperbolic motion is not possible.

The above discussion demonstrates that ray dynamics in a multi-dimensional conversion is a combination of elliptic and hyperbolic motions (and degenerate versions of these motions such as occurs, for example, when $`\omega =0`$). However, we have not yet exhausted all possible congruence transformations. Now consider congruence transformations that are pure scale transformations (i.e. diagonal matrices with $`|det(𝐐)|Q1`$). From $`det(𝐃^{})=Q^2det(𝐃)`$ we have $`\eta ^{\mu \nu }B_\mu ^{}B_\nu ^{}=Q^2\eta ^{\mu \nu }B_\mu B_\nu `$. Thus the light-cone is invariant, but the numerical value of the determinant off the light-cone can change. Using $`B^{}=\mathrm{\Lambda }B`$ we find that $`\mathrm{\Lambda }`$ now preserves the Minkowski tensor only to an overall scale factor: $`\stackrel{~}{\mathrm{\Lambda }}\eta \mathrm{\Lambda }=Q^2\eta `$, implying $`\mathrm{\Lambda }`$ is not a Lorentz transformation, but a conformal one. We still have $`\mathrm{\Omega }^{}=\mathrm{\Lambda }\mathrm{\Omega }\stackrel{~}{\mathrm{\Lambda }}`$, and therefore $`\eta \mathrm{\Omega }^{}=Q^2\stackrel{~}{\mathrm{\Lambda }}^1\eta \mathrm{\Omega }\stackrel{~}{\mathrm{\Lambda }}`$. This implies that the characteristic polynomial of $`\eta \mathrm{\Omega }^{}`$ is $`P^{}(\lambda )det(\eta \mathrm{\Omega }^{}\lambda )=det(\stackrel{~}{\mathrm{\Lambda }}^1(Q^2\eta \mathrm{\Omega }\lambda )\stackrel{~}{\mathrm{\Lambda }})=Q^8P(\lambda /Q^2)`$. Therefore $`P^{}(\lambda )=\lambda ^4+(\omega ^2\gamma ^2)\lambda ^2Q^4(\gamma \omega )^2Q^8`$, and we arrive, finally, at the result that the ratio

$$K\frac{\omega ^2\gamma ^2}{\gamma \omega }$$
(8)
is the sole quantity that is invariant under all (constant) congruence transformations of the $`2\times 2`$ reduced dispersion matrix. As mentioned earlier, the entries of $`\mathrm{\Omega }`$ are Poisson brackets, hence the entire matrix is invariant under canonical transformations, and we have uncovered a new quantity that is invariant under both sets of transformations.

In a separate paper we shall discuss how to exploit the connection with the Lorentz group to construct the normal form of the reduced dispersion matrix. If $`\gamma `$ and $`\omega `$ are not already parallel, it is possible to make them so by performing a ‘boost’ in the direction $`\omega \times \gamma `$ with an appropriate choice of boost parameter. Hence, there is a set of frames where $`\omega `$ and $`\gamma `$ are parallel. In such a frame, the invariant we have uncovered reduces to a simple function $`K=\kappa \kappa ^1`$ with $`\kappa \omega ^{}/\gamma ^{}`$. The primes indicate that these are measured in these special frames. This reveals that the invariant $`\kappa `$ has a natural interpretation as the helicity of a ray and measures the rate at which it ‘rotates’ relative to the rate of exponentiation. The sign of $`\kappa `$ (the ‘handedness’ of the ray helix, as defined in the four-dimensional $`B`$-space) is also invariant. We shall also discuss how to solve the related $`2\times 2`$ wave equation using generalizations of the fourier transform, and how to incorporate these new results into numerical ray tracing codes.

###### Acknowledgements.

This work was supported by the US Dept. of Energy, Office of Fusion Energy Sciences. We would like to thank Robert Littlejohn for helpful suggestions and comments.


text:
# Extended Dynamical Mean Field Theory Study of the Periodic Anderson Model

## Abstract

We investigate the competition of the Kondo and the RKKY interactions in heavy fermion systems. We solve a periodic Anderson model using Extended Dynamical Mean Field Theory (EDMFT) with QMC. We monitor simultaneously the evolution of the electronic and magnetic properties. As the RKKY coupling increases the heavy fermion quasiparticle unbinds and a local moment forms. At a critical RKKY coupling there is an onset of magnetic order. Within EDMFT the two transitions occur at different points and the disapparence of the magnetism is not described by a local quantum critical point.

The interaction between local moments and conduction electrons is a long standing problem in condensed matter physics. As discussed early on doniach (1, 2), two competing interactions, the Kondo exchange between the conduction electrons and the moments, and the indirect exchange among the moments mediated by the RKKY interaction, are central to this problem.

The physics at high temperatures is well understood. Moments and conduction electrons retain their identities and interact weakly with each other. The central question in this field is to understand the characteristics of the state that develops as the temperature is lowered. When the RKKY interaction is much larger than the Kondo energy, the moments order magnetically and the conduction electrons follow their magnetization without undergoing a strong renormalizations. The spin entropy is mostly quenched by the ordering of the local moments. When the RKKY interaction is much weaker than the Kondo energy, the spin entropy is absorbed by the interaction of the moments and the conduction electrons. This results in the formation of a heavy Fermi liquid of quasiparticles which are composites of local moment spins bound to the conduction electrons. The description of the low temperature state, when both the RKKY and the Kondo interactions are of comparable magnitude, has been an important unresolved question. It has received renewed theoretical interest motivated by the intensive experimental investigation stewart (3) of two materials, YbRh2Si2 YbRh (4) and CeCu6-xAux CeCu (5), which can be driven continuously from the paramagnetic (PM) phase to the antiferromagnetic (AF) phase by application of pressure, alloying and magnetic field. Near the quantum critical point, RKKY and Kondo interactions are both essential and need to be treated on the same footing. It has not been possible coleman0 (6, 7) to describe the quantum phase transition in these materials within the standard Hertz-Millis-Moriya (HMM) framework hertz (8, 9, 10) so far.

The interplay of Kondo and RKKY interactions has been addressed using slave boson mean field methods and large-N expansions largen (11). This method can capture the Kondo effect and the Fermi liquid phase. The introduction of bond variables allows some description of the effects of magnetic correlations in the heavy Fermi liquid state. However the simultaneous description of the antiferromagnetism and heavy Fermi liquid behavior within this technique is still an open problem. Furthermore, mean field methods can not capture the incoherent part of the electron Green’s function which is important near the transition. This problem becomes more tractable near the PM metal to spin glass transition sengupta (12).

With the development of Dynamical Mean Field Theory (DMFT) gabi1 (13), which can treat both the AF states and the Kondo effect, it has been possible to make further progress in this problem jarrell (14, 15). An extension of DMFT (EDMFT) subir (16), which allows a better treatment of the competition between the exchange interaction and kinetic energy, was first applied in the context of a one-band model by Parcollet and Georges olivier (17) and more recently by Haule et al. haule (18) who established that the increasing exchange reduces the coherence temperature. The Kondo lattice with magnetic frustration in the large-N limit was recently studied by Burdin et al. burdin (19) who found a paramagnet to spin liquid quantum phase transition. Si et al. si0 (20) considered the $`SU(2)`$ Kondo lattice model in the view point that the model can be described in terms of the criticality of an impurity model in a self-consistent medium. They concluded that in 2D and within EDMFT this model a) has a quantum critical point, b) the quantum critical point has nonuniversal exponents, and c) a numerical calculation si1 (21) of this exponent has remarkable similarity to some of the experimental observations in the CeCu6-xAux system. However, no study of the magnetism had been carried out and this is the subject of this paper.

Our goal is to address these issues within the periodic Anderson model (PAM), focusing more on the evolution of the electronic structure at finite temperatures and not too close to the phase transition. We solve the model using EDMFT and a continuous field Hubbard-Stratonovich QMC method as an impurity solver motome (22, 23).

The PAM Hamiltonian is given by:

$$H=\underset{\stackrel{}{k}\sigma }{}ϵ_\stackrel{}{k}n_{\stackrel{}{k}\sigma }^c+V\underset{i\sigma }{}(c_{i\sigma }^{}f_{i\sigma }+f_{i\sigma }^{}c_{i\sigma })+E_f\underset{i\sigma }{}n_{i\sigma }^f$$

$$+U\underset{i}{}\left(n_i^f1/2\right)\left(n_i^f1/2\right)+\frac{J}{2}\underset{ij}{}S_{i,z}^fS_{j,z}^f$$
(1)
where $`c_{i\sigma }`$ ($`f_{i\sigma }`$) annihilates a conduction (localized f-) electron of spin $`\sigma `$ at site $`i`$. $`n_{i\sigma }^a=a_{i\sigma }^{}a_{i\sigma }`$, with $`a=c,f`$, and $`S_{i,z}^f=n_i^fn_i^f`$. We introduce an independent RKKY interaction which can be induced by hybridization of the f-electron with either the c-electrons or the electrons in the other orbitals which are not included explicitly gabi0 (24). There is experimental evidence that the spin fluctuations rosch (25, 26) near the critical doping are of quasi-2D nature in CeCu6-xAux. For technical convenience, we take a short range Ising AF RKKY exchange of the form $`J_\stackrel{}{q}=J_{RKKY}(\mathrm{cos}q_x+\mathrm{cos}q_y)/2`$. For the c-band we take the dispersion, $`ϵ_\stackrel{}{k}=(\mathrm{cos}k_x+\mathrm{cos}k_y+\mathrm{cos}k_z)/3`$.

We then make the EDMFT approximation subir (16, 22, 23). To describe the AF phase gabi1 (13) we introduce formally two effective impurity models and use the symmetry that electrons at one impurity site is equivalent to the electrons on the other with opposite spins. The self-consistent condition involves the self-energies of both spins. The EDMFT equations in the PM phase are obtained when the self-energies do not depend on spin. The local Green’s functions and the self-energies are obtained from the quantum impurity model:

$$S_0=_0^\beta 𝑑\tau _0^\beta 𝑑\tau ^{}\underset{\sigma }{}f_{0,\sigma }^{}(\tau )𝒢_{0,\sigma }^1(\tau \tau ^{})f_{0,\sigma }(\tau ^{})$$

$$\frac{1}{2}_0^\beta 𝑑\tau _0^\beta 𝑑\tau ^{}\varphi _0(\tau )𝒟_0^1(\tau \tau ^{})\varphi _0(\tau ^{})$$

$$+U_0^\beta 𝑑\tau \left[n_{0,}^f(\tau )1/2\right]\left[n_{0,}^f(\tau )1/2\right]$$

$$_0^\beta 𝑑\tau \varphi _0(\tau )\left[n_{0,}^f(\tau )n_{0,}^f(\tau )\right].$$
(2)
$`𝒢_0`$ and $`𝒟_0`$ play a role of the dynamical Weiss functions and describe the effect of the environment on the f electron and its spin. Their behavior is obtained from a self-consistent solution of the EDMFT equations:

$$G_{ff,\sigma }^{imp}(ip_n)=\underset{\stackrel{}{k}}{}\frac{\xi _\sigma (k,ip_n)}{[\xi _\sigma (\stackrel{}{k},ip_n)][\xi _\sigma (\stackrel{}{k},ip_n)]\eta (\stackrel{}{k},ip_n)^2},$$
(3)
$$D^{imp}(i\omega _n)=\underset{\stackrel{}{q}}{}J_\stackrel{}{q}/[1J_\stackrel{}{q}\mathrm{\Pi }(i\omega _n)].$$
(4)
In Eq.3 we used

$$\xi _\sigma (\stackrel{}{k},ip_n)=ip_n+\mu \sigma [J_{\stackrel{}{q}=0}+𝒟_0(i0)]S_z$$

$$E_f\mathrm{\Sigma }_\sigma (ip_n)V^2\frac{ip_n+\mu }{(ip_n+\mu )^2ϵ_\stackrel{}{k}^2},$$

$`\eta (\stackrel{}{k},ip_n)=V^2ϵ_\stackrel{}{k}/[(ip_n+\mu )^2ϵ_\stackrel{}{k}^2]`$, and $`S_z=G_{ff,}^{imp}(0^{})G_{ff,}^{imp}(0^{})`$. The f-electron and the boson self-energies are obtained by the local Dyson equations. $`p_n`$ and $`\omega _n`$ are the fermion and boson Matsubara frequencies, respectively. The boson self-energy and the experimentally relevant spin susceptibility are related by ping (23):

$$[\chi (\stackrel{}{q},i\omega _n)]^1=J_\stackrel{}{q}+[\mathrm{\Pi }(i\omega _n)]^1$$
(5)
We use QMC ping (23) to solve the impurity problem described by Eq.(2). Eqs.(3) and (4) are then applied. This forms one iteration loop from which the new dynamical Weiss functions are obtained for the next iteration until convergence. We use $`U=3.0`$, $`V=0.6`$, $`E_f=0.5`$, and $`\mu =0.0`$. The number of time slices in QMC is $`L=16`$ for $`\beta 8.0`$, $`L=32`$ for $`8.0\beta 20.0`$, and $`L=64`$ for $`16.0\beta 32.0`$. The number of QMC sweeps is typically $`10^6`$. We measure the energies in terms of the Kondo temperature at zero $`J_{RKKY}`$ coupling, $`T_k^0=1/\beta _k^01/8.0`$, which is determined from the position of the peak in the local susceptibility vs temperature plot (see Fig. 3 below).

Fig. 1 describes the EDMFT phase diagram of the PAM as temperature and $`J_{RKKY}`$ are varied. Within EDMFT the PAM exhibits a first order phase transition. There are two lines, $`J_{c1}`$ and $`J_{c2}`$, betweens which we find two EDMFT solutions. The strength of the first order phase transition, which is reflected in the size of the coexistence region, is non-monotonic in temperature. It is large at high (region I) and low (region II) temperatures. At the boundaries of the coexistence region, the magnetization $`S_z`$ and the static local susceptibility are discontinuous. Along the line $`J_{c2}`$ the transition becomes stronger first order as the temperature is lowered, while along the $`J_{c1}`$ line it becomes weaker ping1 (27). The overall transition tends to be more strongly first order at low temperatures. As we increase $`J_{RKKY}`$ at fixed $`T`$, the f-electron becomes more localized ($`\mathrm{Im}[𝒢_0^1(ip_n)]p_n`$ becomes smaller at low frequencies) while the local spin fluctuations are strongly enhanced in the neighborhood of the $`J_{c2}`$ line ($`𝒟_0(i\omega _n)`$ becomes bigger at low frequencies) ping1 (27). EDMFT self-consistency is crucial in obtaining the results, which are absent in the simple impurity model.

An important question is the effect of the RKKY interaction on the quasiparticle mass. The RKKY interaction partially locks the spins and thus reduces the effective mass and the spin entropy. But it also serves as an additional interaction among the quasiparticles which increases the effective mass. To address this question, we plot at $`T/T_k^0=1.0`$ the inverse quasiparticle residue $`Z^1`$ as a function of $`J_{RKKY}`$ in Fig. 2. $`Z^1`$, which is proportional to the effective electron mass, gets enhanced as the transition is approached from both sides. This mass enhancement is not included in the HMM. We predict that the mass enhancement of the majority carriers is larger than that of the minority carriers in the AF phase. In the inset to Fig. 2 we display the extrapolation of the self-energy to zero Matsubara frequency which is a measure of the quasiparticle lifetime. Notice that in the PM side, the inelastic effects increase as the transition is approached, an effect which is also absent in weak coupling approaches. This trend was observed in earlier EDMFT studies olivier (17, 18). Given the parameters we use, the f-electron is delocalized ping1 (27) throughout the phase diagram. However, as $`J_{RKKY}`$ is increased, the f-electron becomes more localized.

We now turn to the evolution of the magnetic properties as a function of temperature and $`J_{RKKY}`$ . In Fig. 3 we plot the local susceptibility. Following the PM solution we sweep the phase diagram from $`J_{RKKY}=0`$ up to the line $`J_{c2}`$ in Fig. 1. In this procedure, the position of the Kondo peak moves towards lower temperature and its height has an increment of about $`37\%`$. If we solve the EDMFT equations without forcing any magnetic order, either the PM or AF solution can appear. For $`J_{RKKY}/T_k^02.00`$, we see the Neel cusp first occurs below the Kondo peak which disappears as $`J_{RKKY}`$ increases further. This happens before the Kondo temperature goes to zero, consistent with the HMM.

To further test the local critical scenario si0 (20) we follow the evolution of the PM solution as a function of temperature and frequency. In Fig. 4 we plot $`1/\chi _{AF}(i\omega _n)`$, which is defined as $`1/\chi (\stackrel{}{q},i\omega _n)`$ at $`\stackrel{}{q}=(\pi ,\pi )`$, as $`J_{RKKY}`$ is changed. One can see from the inset that, as the transition is approached, the zero frequency value $`1/\chi _{AF}(i0)`$ vanishes. From the curvature of the lines one can see that the frequency dependences of $`1/\chi _{AF}(i\omega _n)`$ does not seem to be consistent with a sublinear behavior required by the local quantum critical scenario. In stead, it is compatible with the standard HMM picture and a recent large-N study pankov1 (28).

In summary we have studied the PAM within EDMFT. In the parameter regime studied, we found that the heavy quasiparticles first form, and then undergo a magnetic phase transition. This would indicate that the HMM description of the quantum phase transition would apply to this model. On the other hand, we also find a large enhancement of the effective mass and reduction of the quasiparticle lifetime, which are beyond the standard model.

This paper raises a large number of questions that require further investigations. The first one is the connection between our results and those reported in EDMFT studies of the Kondo lattice models by Si et al. si0 (20, 21, 29). Our model is in the mixed valence region where the charge fluctuations can not be neglected. To reconcile the difference in the results one could study the Anderson model in a regime of parameters that is closer to the Kondo lattice model. This probably will require the use of a different impurity solver, to test if the PM-AF transition becomes more weakly first order as the Kondo limit (larger $`U`$ and more negative $`E_f`$) is approached. The second question is the relevance of the EDMFT results to real materials and how the mean field theory should be interpreted. EDMFT is a mean field treatment of the spatial degrees of freedom and breaks down in the immediate vicinity of the transition. Clearly in the coexistence region of the upper part of the phase diagram (region I), EDMFT is unreliable pankov (30). In finite dimensions the system has a non-trivial anomalous dimension and the transition is second order. There is a region in the vicinity of the transition where non-Gaussian thermal fluctuations are important in reality and they are absent in the EDMFT theory. But outside the vicinity of this transition we expect the predictions of the theory such as the weak enhancement of the effective mass to be observable. Indeed, while EDMFT induces a spurious first order transition, in the high temperature regime where the semiclassical evaluation of the free energy is valid, EDMFT gives a very accurate determination of the location of the first order phase transition.pankov (30, 27)

The EDMFT solution existed between $`J_{c1}(T)`$ and $`J_{c2}(T)`$ lines at low temperatures (region II) suggests a crossover to a different regime where non-local effects become important. This has been recently observed in the YbRh2Si2 system gegenwart (31). Here again EDMFT is not reliable in the vicinity of the transition and some element of non-locality becomes important. To improve the description of this region and to reduce the strength of the first order phase transitions and other deficiencies of EDMFT, in particular the fact that the spins in the bath are treated classically rather than quantum mechanically, a different extension of DMFT to treat a cluster of spins in a self-consistent medium is needed. This line of work will lead to a two impurity Kondo or Anderson model jones1 (32, 33) in a self-consistently determined bath which is known to have a different critical point than the spin model in a random magnetic field.

This research was supported by NSF under Grants No. DMR-0096462 and No. DMR-9983156 and by the Center for Materials Theory at Rutgers University. We thank P. Coleman, V. Dobrosavljevic, S. Florens, A. Georges, S. Pankov, and Q. Si for helpful discussions.


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# Experimental Controlled-NOT Logic Gate for Single Photons in the Coincidence Basis

## Abstract

We report a proof-of-principle demonstration of a probabilistic controlled-NOT gate for single photons. Single-photon control and target qubits were mixed with a single ancilla photon in a device constructed using only linear optical elements. The successful operation of the controlled-NOT gate relied on post-selected three-photon interference effects which required the detection of the photons in the output modes.

There has been considerable interest in a linear optics approach to quantum computing , in which probabilistic two-qubit logic operations are implemented using linear optical elements and measurements made on a set of $`n`$ additional (ancilla) photons. Here we report a proof-of-principle demonstration of a probabilistic controlled-NOT (CNOT) gate using a single ancilla photon. Two of the required single-photons were produced using parametric down-conversion  while a third photon was obtained from an attenuated laser pulse. The use of only one ancilla photon required that all three photons be detected, in which case the device was known to have correctly performed a CNOT logic operation.

Logic operations are inherently nonlinear, so it is somewhat surprising that they can be performed using simple linear optical elements . The necessary nonlinearity is obtained by mixing the input photons with $`n`$ ancilla photons using linear elements, and then measuring the state of the ancilla photons after the interaction. The measurement process is nonlinear , since a single-photon detector either records a photon or not, and it projects out the desired logical output state provided that certain results are obtained from the measurements. The results of the operation are known to be correct whenever these specific measurement results are obtained, which occurs with a failure rate that scales as $`\frac{1}{n}`$  or $`\frac{1}{n^2}`$  in the limit of large $`n`$, depending on the approach that is used.

In a series of earlier experiments , we demonstrated several elementary logic gates for single photons, including a quantum parity check and a destructive CNOT gate. The latter device produced only a single output (the target qubit) and was equivalent to an exclusive OR gate, since the control qubit was destroyed. As a result, destructive CNOT gates cannot be used for reversible computing or to demonstrate the generation of entanglement, for example. Here we describe the demonstration of a full CNOT gate whose output includes both the target and control qubits. Although the gate is probabilistic and the presence of both output qubits must eventually be verified by subsequent measurements (the so-called coincidence basis), the quantum features of both outputs can still be investigated. For example, the generation of entanglement can be demonstrated using Bell’s inequalities and both outputs of such a gate can be fed into subsequent logic gates, provided that one can eventually verify that both outputs were produced.

We have previously shown  that a CNOT gate can be implemented using the simple beam splitter arrangement shown in Figure 1(a). Here the logical value of each of the qubits is represented by the polarization state of a single photon, where a horizontal polarization state $`|H`$ represents a value of 0 and a vertical polarization state $`|V`$ represents a value of 1. In addition to the two input photons, a pair of ancilla photons in an entangled state $`|\varphi ^+=\frac{1}{\sqrt{2}}(|00+|11)`$ are incident on two polarizing beam splitters as shown. Polarization-sensitive detectors measure the state of the ancilla photons in an appropriate basis when they leave the beam splitters, and corrections to the output may be required based on the results of these measurements . Provided that one and only one photon is found in each of these detectors, the output of the device will correspond to that of a CNOT gate . This corresponds to the case of $`n=2`$ and the device succeeds in producing the correct output with a probability of $`\frac{1}{4}`$.

The basic operation of this controlled-NOT gate can be roughly understood as follows: The lower beam splitter performs the logical function of a controlled-NOT gate except that one of its input qubits is destroyed in the lower detector (a destructive CNOT gate). The destruction of one of the input qubits can be avoided by first copying (encoding) the value of that qubit onto two output qubits. One of the copies is then input into the destructive CNOT gate while the remaining copy serves as one of the required logical outputs. A quantum encoder of that kind can be implemented using the upper beam splitter and the entangled ancilla photons as described in Ref. . The net result of these operations is a full CNOT gate with both of the input qubits preserved.

From an experimental point of view, the main difficulty with the CNOT gate of Figure 1(a) is its reliance on heralded entangled ancilla pairs , which have not yet been reliably demonstrated. However, the need for a pair of ancilla photons in an entangled state can be avoided using the one-ancilla CNOT gate shown in Figure 1(b). This device is equivalent to that of Figure 1(a) except that a single ancilla enters the upper beam splitter where a detector was previously located. If the ancilla photon is in an equal superposition of $`|0`$ and $`|1`$, then it can be shown that the value of the control photon will be copied (encoded) into the two output ports of the upper beam splitter just as before. However, the price that must be paid for using a single ancilla photon instead of an entangled ancilla pair is that the correct logical output will only be produced if a single photon actually exits from each of the three output ports of the device. Without reliable quantum non-demolition devices , this condition can only be verified by eventually detecting the output qubit photons as shown Figure 1(b). This type of “coincidence basis” operation prohibits the use of the device in a scalable approach to quantum computing, but it does provide a convenient means of demonstrating the operation of a CNOT logic gate for single photons .

The operation of the CNOT gate shown in Figure 1(b) can be understood by considering an input state consisting of the single ancilla photon in the required superposition state $`\frac{1}{\sqrt{2}}(|0_A+|1_A)`$, and an arbitrary initial two-photon state of the control and target photons, $`\alpha _1|0_c0_t+\alpha _2|0_c1_t+\alpha _3|1_c0_t+\alpha _4|1_c1_t`$, where $`_{i=1}^4|\alpha _i|^2=1`$. It can be shown that (under ideal experimental conditions) this initial state is transformed into an output state of the form:

$`|\psi _{out}=`$ (1)
$`{\displaystyle \frac{1}{2\sqrt{2}}}|0_A\left(\alpha _1|0_c0_t+\alpha _2|0_c1_t+\alpha _3|1_c1_t+\alpha _4|1_c0_t\right)`$
$`+{\displaystyle \frac{1}{2\sqrt{2}}}|1_A\left(\alpha _1|0_c1_t+\alpha _2|0_c0_t+\alpha _3|1_c0_t+\alpha _4|1_c1_t\right)`$
$`+{\displaystyle \frac{\sqrt{3}}{2}}|\psi _{}`$
where $`|\psi _{}`$ represents the normalized combination of amplitudes that are orthogonal to the “coincidence basis” measurement condition of one photon in each of the three output modes.

The first term in equation (1) indicates that the detection of a single photon in the $`|0`$ state by $`D_A`$ projects the output in the control and target modes into the desired CNOT transform  of the input. This occurs with a probability of $`\frac{1}{8}`$, which reflects the probabilistic nature of the device. The second term in equation (1) shows that the overall success probability could be increased to $`\frac{1}{4}`$ by also accepting events in which $`D_A`$ registers a single photon in the $`|1`$ state, provided that feed-forward control techniques  are used to bit-flip the output target state.

A simplified schematic of the experimental apparatus used to demonstrate the CNOT gate of Figure 1(b) is shown in Figure 2. Two of the three photons were produced using a pulsed laser beam passing through a nonlinear crystal (parametric down-conversion ), while the third photon was obtained by attenuating the laser pulses themselves to the point that each pulse had only a small probability of containing a single photon. Since the frequency of the laser beam was doubled before the down-conversion process, the down-converted photons had the same frequency as the photons obtained directly from the laser beam. Furthermore, the use of short laser pulses followed by narrow-band interference filters ensured that all three photons were very nearly indistinguishable .

Single-mode optical fibers were used to connect the beam splitters and other components, which reduced the possibility of an error due to mode mismatch. Errors due to changes in the state of polarization of the photons were minimized using standard optical-fiber polarization controllers. The required $`45^o`$ rotation of PBS-2 was accomplished by using a calibrated fiber polarization rotator (fpc) between the two beam splitters, and rotating the definitions of $`|0`$ and $`|1`$ by $`45^o`$ in the remaining ports of PBS-2. The polarization states of the input photons could be varied by rotating half-wave plates placed before the beams entered the optical fibers, as shown in Figure 2. This allowed the logical inputs to the device to consist of arbitrary superposition states.

In order for the three photons to be indistinguishable, it was also necessary for them to arrive at the appropriate beam splitters at the same time. The required path length adjustments were optimized by maximizing the visibilities of various two-photon  and three-photon interference effects . The visibilities of these interference patterns were typically in the range of 85 - 95% for two-photon interference effects  at PBS-1, and 60 - 70% for three-photon (ie. gated two-photon) interference effects  at PBS-2. The lower values for the three-photon interference effects were primarily due to the use of interference filters with a relatively wide bandwidth of 10 nm , and a decreased signal-noise-ratio as described in reference . The use of smaller bandwidth filters would be expected to substantially increase the three-photon visibility , at the cost of lower counting rates.

The output of the device was measured using polarization analyzers followed by single-photon detectors, and events were only accepted if all three detectors registered a photon. In accordance with Equation (1), $`D_A`$ only accepted ancilla photons in the logical state $`|0`$, which was accomplished by fixing the orientation of $`\theta _A`$ at $`0^o`$ in the computational basis (which was physically rotated by $`45^o`$ due to the orientation of PBS-2). In this initial demonstration, feed-forward control techniques  were not used to accept events in which the ancilla photon was found in the logical state $`|1`$. Since the attenuated laser pulses correspond to weak coherent states, it was necessary to minimize the probability of there being two photons in a given pulse by reducing the probability of a single photon to roughly $`10^3`$.

Using these techniques, it was possible to measure the output of the device for all possible combinations of logical inputs (0 or 1) as well as superposition states. The results of these measurements when the input qubits both had specific values of 0 or 1 are summarized in Figure 3. The correct results from an ideal CNOT gate  correspond to the four larger peaks, while the smaller peaks correspond to incorrect results. It can be seen that the output of the device is clearly correct, aside from overall technical errors of roughly 21%. For a given input state, the distribution of errors among the three incorrect output states was primarily determined by the extent to which they depended on destructive three-photon quantum interference effects. In addition, minor changes in the polarization states of the photons in the optical fibers allowed small contributions from the output state associated with the detection of an ancilla photon in the state $`|1`$.

It is important to demonstrate that quantum logic gates maintain the quantum-mechanical coherence of the input qubits when the latter are in superposition states of 0 and 1. As an example of this coherence, Figure 4 shows the results obtained when the incident control qubit was in the superposition state $`\frac{1}{\sqrt{2}}(|0+|1)`$ while the target was in the state $`|0`$. In that case, the two output qubits should be produced in an entangled state of the form $`\frac{1}{\sqrt{2}}(|00+|11)`$, which is the state $`|\varphi ^+`$. This is an important example, since a CNOT gate is expected to produce entanglement between two independent input photons. The data in the figure corresponds to the number of three-fold coincidence counts as a function of the target analyzer, with the control analyzer set to the logical value 0. In that case, a detection of a control photon collapses the entangled state to just the first term, so that the target photon should also be found with logical value 0. The data of Figure 4 are consistent with that prediction. When the analyzer in the path of the control photon was set to logical value 1 instead, then the entangled state collapsed to the second term and the target photon was found with logical value 1, as expected. Analogous results were found in a basis rotated by $`45^{}`$. Although these results demonstrate entanglement between the two photons and nonlocal measurement results, the data extracted from these plots was not sufficient to allow a violation of Bell’s inequality using the two output photons .

In summary, we have experimentally demonstrated the operation of a probabilistic CNOT gate for single photons in the coincidence basis using linear optical elements and a single ancilla photon. Although the presence of the output qubits must eventually be verified, the properties of both the control and target qubits can be investigated before they are detected. Input qubits with specific values in the computational basis produced output states that corresponded to those of a CNOT gate aside from technical errors on the order of 20%. Superpositions of input states were found to produce entanglement of the output qubits. Although the use of a single ancilla photon limits the performance of the current device, which is not scalable, larger numbers of ancilla photons can be combined with more general linear optics techniques  to reduce the probability of error and produce an approach that is scalable.

This work was supported by ARO, NSA, ARDA, ONR, and IR&D funding.


text:
# Decoherence in a Josephson junction qubit

## Abstract

The zero-voltage state of a Josephson junction biased with constant current consists of a set of metastable quantum energy levels. We probe the spacings of these levels by using microwave spectroscopy to enhance the escape rate to the voltage state. The widths of the resonances give a measurement of the coherence time of the two metastable states involved in the transitions. We observe a decoherence time shorter than that expected from dissipation alone in resonantly isolated 20x5 $`(\mu \mathrm{m})^2`$ area Al/AlOx/Al junctions at 60 mK. The data is well fit by a model that includes the dephasing effects of both low-frequency current noise and the escape rate to the voltage state. We discuss implications for quantum computation using current-biased Josephson junction qubits, including limits on the minimum number of levels needed in the well to obtain an acceptable error limit per gate.

Research in the 1980s definitively showed that the phase difference across a single current-biased Josephson junction can behave quantum-mechanically Voss and Webb (1981); Martinis et al. (1985). The recent proposal that an isolated current-biased Josephson junction could serve as a qubit Ramos et al. (2001) in a quantum computer has preceeded a resurgence of interest in this simple system Martinis et al. (2002); Yu et al. (2002); Blais et al. (2002); Johnson et al. (2003).

Designing a quantum computer based on isolated Josephson junctions raises many issues. Isolation of the junction from its bias leads must be achieved by controlling the high frequency electromagnetic environment that the junction couples to Martinis et al. (1985). At the very least, this isolation must be effective around the resonant frequency of the junction. In addition, at lower frequencies, current noise will tend to cause decoherence in the junction state. Also, during typical gate operations the junction must operate in a strongly anharmonic regime that can be reached by applying a large bias current through the junction. In this high bias regime however, there is an increased escape rate from the upper qubit state. In this Letter, we describe how both the escape rate and low frequency current noise cause decoherence and report results on measurements of these effects in Al/AlOx/Al Josephson junctions.

Consider a Josephson junction shunted by capacitance $`C`$, having a critical current $`I_0`$, and a parallel shunting impedance $`R(\omega )`$ due to the external wiring (see Fig. 1). The supercurrent $`I`$ through the junction is given by the Josephson relation $`I=I_0\mathrm{sin}(\gamma )`$, and the voltage by $`V=(\mathrm{\Phi }_0/2\pi )\mathrm{d}\gamma /\mathrm{dt}`$, where $`\gamma `$ is the gauge-invariant phase difference between the superconducting wavefunctions on each side of the junction. For $`I<I_0`$, the phase $`\gamma `$ may be trapped in a metastable well of the Josephson washboard potential, $`U=(\mathrm{\Phi }_0/2\pi )I_0\mathrm{cos}\gamma (\mathrm{\Phi }_0/2\pi )I\gamma `$, or it may be in a running state with a non-zero average dc voltage see eg. M. Tinkham (1996).

Quantizing the single junction system in the absence of dissipation leads to metastable states that are localized in the wells (see Fig. 2) and adds the possibility of escape to the continuum running states by quantum tunneling from the $`i`$th level with a rate $`\mathrm{\Gamma }_i\mathrm{}`$. The energy barrier $`\mathrm{\Delta }U=(I_0\mathrm{\Phi }_0/\pi )(\sqrt{1(I/I_0)^2}(I/I_0)\mathrm{acos}(I/I_0))`$ to the continuum decreases as the bias current is increased, leading to a rapid increase in the tunneling rate with bias current Alvarez (1988):

$$\mathrm{\Gamma }_i\mathrm{}=\omega _p\frac{\left(432N_s\right)^{i+1/2}}{\left(2\pi \right)^{1/2}i!}e^{36N_s/5}$$
(1)
where $`\omega _p=\sqrt{\frac{2\pi I_0}{\mathrm{\Phi }_0C}}\left(1\left(I/I_0\right)^2\right)^{1/4}`$ is the classical oscillation frequency and $`N_s=\mathrm{\Delta }U/\mathrm{}\omega _p`$ is approximately the number of levels in the well. As the energy barrier is lowered, the energy of the states in the well move closer together and the well becomes more anharmonic until, at $`I=I_0`$, the energy barrier disappears.

The observed escape rate of the system from the zero-voltage state to the finite voltage state at a given bias point is $`\mathrm{\Gamma }=\mathrm{\Sigma }_{i=0}^n\mathrm{\Gamma }_i\mathrm{}P_i`$, where $`P_i`$ is the probability of the junction being in the $`i`$th state. An ac current, $`I_{ac}`$ (either external or thermally generated) can induce transitions between levels $`i`$ and $`j`$ in the well with a rate $`\mathrm{\Gamma }_{ij}\left|\frac{\mathrm{\Phi }_0}{2\pi }I_{ac}i|\gamma |j\right|^2`$. Since $`\mathrm{\Gamma }_1\mathrm{}500\mathrm{\Gamma }_0\mathrm{}`$ for typical junction parameters, one expects to see a large enhancement in the escape rate if a microwave source is used to resonantly excite the system from the ground state $`|0`$ to the first excited state $`|1`$ (see Fig. 3).Martinis et al. (1985)

Each microwave resonance in this system will be broadened due to the interaction of the junction with noise transmitted via the wiring and described by the interaction Hamiltonian $`H_{int}=(\mathrm{\Phi }_0/2\pi )I_{noise}\gamma `$. Thermal noise and dissipation at the transition frequencies will cause changes in the populations of the states. At low frequencies, the resonant terms are insignificant and the noise only causes dephasing.

Considering just the ground state $`|0`$ and the first excited state $`|1`$, transitions arise from thermal excitation from $`|0`$ to $`|1`$, a $`1/RC`$ decay rate from $`|1`$ to $`|0`$, and tunneling to the continuum, $`\mathrm{\Gamma }_i\mathrm{}`$ for $`i=0`$ and $`1`$. At temperature $`T`$, the combined thermal and dissipative transition rates are:Chow et al. (1988)

$$\mathrm{\Gamma }_{01}=\frac{1}{RC(\mathrm{exp}(\mathrm{\Delta }E/kT)1)}$$
(2)
$$\mathrm{\Gamma }_{10}=\frac{1}{RC(1\mathrm{exp}(\mathrm{\Delta }E/kT))}$$
(3)
where $`\mathrm{\Delta }E=E_1E_0`$ is the difference in energy between the two levels. For $`kT\mathrm{\Delta }E`$, the upward thermal transition rate is much smaller than the downward rate. From Eqn. 1 the tunneling to the continuum is much smaller for the ground state than the excited state in the anharmonic region of interest where $`\mathrm{\Delta }U/\mathrm{}\omega 3`$.Alvarez (1988) Thus we expect that the spectroscopic width of the $`|0|1`$ transition is

$`\mathrm{\Delta }\omega =\mathrm{\Gamma }_1\mathrm{}+\mathrm{\Gamma }_0\mathrm{}+\mathrm{\Gamma }_{01}+\mathrm{\Gamma }_{10}\mathrm{\Gamma }_{10}+\mathrm{\Gamma }_1\mathrm{}`$
$`1/RC+\mathrm{\Gamma }_1\mathrm{}`$ (4)
Equations 1 and Decoherence in a Josephson junction qubit imply that the level broadening, $`\mathrm{\Delta }\omega `$, depends on bias through the $`\mathrm{\Gamma }_1\mathrm{}`$ term and should exceed $`1/RC`$ as the bias current approaches $`I_0`$.

To understand results on a real junction we must also take into account the dephasing effects of any current noise in the system. For sufficiently low frequencies, we can model this non-resonant decoherence mechanism as a simple smearing of the response with bias. This should result in a broadening of the spectroscopic width that depends on how sensitive the resonant frequency, $`\omega `$, is to changes in current, $`\omega /I`$. An rms current noise $`\sigma _I`$ should produce an additional contribution to the spectroscopic width of $`2\sigma _I\omega /I`$. Including this current noise contribution in the previous form for the spectroscopic width gives:

$$\mathrm{\Delta }\omega 1/RC+\mathrm{\Gamma }_1\mathrm{}+2\sigma _I\omega /I$$
(5)
Both the second and third terms in Eq. (5) depend on bias, so that care must be taken in disentangling the two effects.

Using double angle evaporation, we fabricated $`20\times 5`$ $`(\mu m)^2`$ Al/AlOx/Al Josephson junctions with $`J_c14`$ $`\mathrm{A}/\mathrm{cm}^2`$. Direct measurements of the junction current-voltage characteristics showed a subgap resistance of more than $`10^4`$ $`\mathrm{\Omega }`$ at 20 mK. Escape rate measurements were made in an Oxford Instruments Model 200 dilution refrigerator with a 20 mK base temperature. We were able to tune the critical current of the junction by means of a superconducting magnet. The junctions were partially isolated from the bias leads by a 10 nH surface mount series inductor and a 10 pF capacitive shunt across the dissipative $`50`$ $`\mathrm{\Omega }`$ transmission line leads (see Fig. 1). This isolation scheme was designed so that at the plasma frequency, the effective shunt resistance due to the leads would be stepped up from $`50`$ $`\mathrm{\Omega }`$ to much more than $`10^3`$ $`\mathrm{\Omega }`$, increasing the intrinsic Q of the system. To perform escape rate measurements, we start a timer and then ramp the current slowly (5 mA/s) using an HP 33120A function generator through a $`47`$ k$`\mathrm{\Omega }`$ resistor and monitor the junction voltage with a 2SK170 FET followed by an SRS560 amplifier. This output voltage is used to trigger the stop of timing, which is handled by a 20 MHz clock. Escape events were binned in time with width $`t_w`$ $`50ns`$ to create a histogram $`H(t_i)`$. The escape rate is then $`\mathrm{\Gamma }(t_j)=\frac{1}{t_w}\mathrm{ln}\left[\mathrm{\Sigma }_{i=j}^{\mathrm{}}H(t_i)/\mathrm{\Sigma }_{i=j+1}^{\mathrm{}}H(t_i)\right]`$. We convert the time axis to current by calibrating the ramp current as a function of time.

We determine the spacing of the energy levels by comparing escape rate curves with $`(\mathrm{\Gamma }_m)`$ and without $`(\mathrm{\Gamma }_0)`$ a small microwave drive current applied. Figure 3 shows $`\mathrm{\Delta }\mathrm{\Gamma }/\mathrm{\Gamma }_0=(\mathrm{\Gamma }_m\mathrm{\Gamma }_0)/\mathrm{\Gamma }_0`$ for a 5.5 GHz microwave signal. We chose the power so that $`\mathrm{\Delta }\mathrm{\Gamma }/\mathrm{\Gamma }_010`$ on resonance to ensure the occupancy of $`|1`$ is small. Two Lorentzian peaks are apparent, corresponding to the $`|0|1`$ and $`|1|2`$ transitions. By measuring $`\mathrm{\Delta }\mathrm{\Gamma }/\mathrm{\Gamma }_0`$ for different applied microwave frequency, we can measure how the bias current changes the energy level spacing of the $`|0|1`$ transition (see Fig. 4a).

The data in Fig. 4a also allows us to compute $`\omega /I`$ and convert the full width at half-maximum $`\mathrm{\Delta }I`$ measured at each frequency (see Fig. 4b) to a width in frequency, $`\mathrm{\Delta }\omega `$, or the spectroscopic coherence time associated with the two levels, $`\tau =1/\mathrm{\Delta }\omega `$.

Figure 5 shows the coherence time $`\tau `$ as a function of the center current of each $`|0|1`$ peak. We note that the coherence time decreases markedly as $`I`$ approaches $`I_014.12\mu A`$, consistent with escape rate limiting of the lifetime of the upper state and excess low frequency current noise as in Eq. 5.

In principle, it is possible for the effective shunting impedance $`R(\omega )`$ to vary with frequency in such a way as to generate the changes in $`\tau (\omega )`$ seen in Fig. 5. We can rule out this explanation for the overall behavior of $`\tau (\omega )`$ by changing the critical current of the junction and remeasuring at the same frequency. Such a process changes $`\mathrm{\Gamma }_i\mathrm{}`$ but not $`R(\omega )`$ in Eq. 5. Results for two different $`I_0`$’s are plotted in Fig. 6a and 6b. Comparison of Figs. 6a and 6b reveals that the coherence time at fixed frequency is lower for larger $`I_0`$. Since this measurement is at fixed frequency, the effect can not be due to $`R`$ varying with frequency.

To distinguish the effects of current noise and escape-rate broadening in Eq. 5, we need to obtain an independent measure of the junction parameters. For the low critical current data, we fit the escape rate curves without microwaves Büttiker et al. (1983) and find $`I_0=10.65\pm 0.01\mu A`$, $`C=3.7\pm 0.3pF`$, and $`T=60\pm 3mK`$. The 60 mK temperature was 40 mK above the base temperature, probably due to self-heating. We also numerically solved Schrödinger’s equation (with hard wall boundary conditions) and chose $`I_0`$ and $`C`$ to fit the data in Fig. 4a (dashed line). This yielded $`I_0=10.645\pm 0.01\mu A`$ and $`C=3.7\pm 0.1pF`$. The same analysis for the high $`I_0`$ case gives $`I_0=14.12\pm 0.01\mu A`$ and $`C=3.7\pm 0.1pF`$. The quantitative disagreement in Fig. 4 may come from not including corrections to the center peak locations due to current noise Berkley et al. (2002), the energy level shifting due to damping, or a frequency dependent impedance (such as is suggested at 5.2 GHz in Fig. 6b).

We now fit the coherence time data in Fig. 6 by varying $`I_0`$ and $`C`$ and comparing the results with the previously determined parameters. We find $`\mathrm{\Gamma }_1\mathrm{}`$ by solving Schrödinger’s equation numerically. To estimate the rms current noise, $`\sigma _I`$, we note that the full current width at half maximum shown in Fig. 4b never drops below 10 nA. We thus assign $`\sigma _I5`$ nA. To get a unique fit, we also assume $`RC1/\left(2\sigma _I\omega /I\right)`$. The solid lines in Fig. 6 show the results of this procedure. The dashed lines show the contribution to the broadening due to the escape rate alone, while the dotted lines represent the current noise contribution. The parameters for the lifetime fits, $`I_0=14.12\mu A,C=3.7pF`$ and $`I_0=10.645\mu A,C=3.7pF`$, agree with the parameters obtained from Fig. 4, verifying the inclusion of current noise and escape-rate-limited coherence in the model of Eqn. 5. We note that as the bias current approaches $`I_0`$ (low frequency), the escape rate term begins to dominate the lifetime, while for lower currents (high frequency), the noise broadening dominates.

To conclude, we have measured the resonance width of the transition between the lowest two quantum states in a Josephson junction qubit as a function of bias current, and found that the lifetime of the excited state falls rapidly as the bias current $`I`$ approaches $`I_0`$. A model including continuous dephasing from tunneling as well as from current noise explains quantitatively the reduced coherence time. This ability to predict and calculate such junction behavior is crucial to the use of junctions in quantum computers and one of the reasons junctions are a good candidate qubit.

For designs where low-frequency current noise is not a significant issue Martinis et al. (2002), consideration of the above results in conjunction with Eqn. 1 suggests the following qubit design criterion. To obtain at least $`N_{op}`$ gate operations before decoherence occurs from tunneling alone, with each gate operation taking approximately $`N_g2\pi /\omega `$ time, requires at least $`N_s>\frac{5}{36}\mathrm{ln}(N_{op}N_p)+\frac{5}{24}\mathrm{ln}(432N_s)`$ levels in the well. For $`N_{op}=10^6`$ and $`N_g=10`$, we find $`N_s>4`$. In the opposite limit, where current noise dominates, the junction must be biased at low currents during gate operations.

###### Acknowledgements.

We acknowledge support from DOD and the Center for Superconductivity Research and thank J.M. Martinis, F. Strauch, P. Johnson, and A. Dragt for many useful discussions about this system.