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# Quantum computation with unknown parameters

## Abstract

We show how it is possible to realize quantum computations on a system in which most of the parameters are practically unknown. We illustrate our results with a novel implementation of a quantum computer by means of bosonic atoms in an optical lattice. In particular we show how a universal set of gates can be carried out even if the number of atoms per site is uncertain.

Scalable quantum computation requires the implementation of quantum gates with a very high fidelity. This implies that the parameters describing the physical system on which the gates are performed have to be controlled with a very high precision, something which it is very hard to achieve in practice. In fact, in several systems only very few parameters can be very well controlled, whereas other posses larger uncertainties. These uncertainties may prevent current experiments from reaching the threshold of fault tolerant quantum computation (i.e. gate fidelities of the order of $`0.9999`$ tolerancia ), that is, the possibility of building a scalable quantum computer. For example, in quantum computers based on trapped ions or neutral atoms cold-atoms , the relative phase of the lasers driving a Raman transition can be controlled very precisely, whereas the corresponding Rabi frequency $`\mathrm{\Omega }`$ has a larger uncertainty $`\mathrm{\Delta }\mathrm{\Omega }`$. If we denote by $`T`$ the time required to execute a gate (of the order of $`\mathrm{\Omega }^1`$), then a high gate fidelity requires $`T\mathrm{\Delta }\mathrm{\Omega }1`$ (equivalently, $`\mathrm{\Delta }\mathrm{\Omega }/\mathrm{\Omega }1`$), which may very hard to achieve, at least to reach the above mentioned threshold.

In this letter we show how to achieve a very high gate fidelity even when most of the parameters describing the system cannot be adjusted to precise values. Our method is based on the technique of adiabatic passage, combined with some of the ideas of quantum control theory. We will illustrate our method with a novel implementation of quantum computing using atoms confined in optical lattices QC-mott . If the number of atoms in each of the potential well is uncertain, which is one of the problems with this kind of experiments, most of the parameters will have an uncertainty of the order of the parameter itself (e.g. $`|\mathrm{\Delta }\mathrm{\Omega }|\mathrm{\Omega }`$), which under normal circumstances will give rise to very poor fidelities and even impede the performance of quantum gates. As we will show, using our method not only quantum computation is possible but even very high fidelities could be achieved.

The use of adiabatic passage techniques to implement quantum gates is, of course, not a new idea. In fact, several methods to perform certain quantum gates using Berry phases have been put forward recently holonomias2 ; holonomias ; Duan . Furthermore, adiabatic passage techniques have been proposed as a way of implementing a universal set of holonomies Duan , i.e. quantum gates which are carried out by varying certain parameters and whose outcome only depends on geometrical properties of the paths in parameter space holonomias2 . In all these proposals, physical implementations of standard quantum computation have been adapted so that the quantum gates are performed in an adiabatic way giving rise to holonomies. Despite its clear fundamental interest, it is not clear yet if such a novel way of implementing the quantum gates may offer real benefits with respect to the original proposals. In contrast, in our illustrative example adiabatic passage is required to perform quantum gates and therefore it is an essential tool not only to achieve the desired precision but also to build a quantum computer at all.

The outline of the paper is as follows. First we will show how to produce a universal set of gates (Hadamard, phase, and CNOT) starting from two Hamiltonians in which only one parameter is precisely controlled. Then we will show that this method eliminates an important obstacle in a particular physical scenario that has been proposed for quantum computation QC-mott , namely a set of atoms in optical lattices interacting via cold collisions.

Let us consider a set of qubits that can be manipulated according to the single qubit Hamiltonian

$$H_1=\frac{\mathrm{\Delta }}{2}\sigma _z+\frac{\mathrm{\Omega }}{2}(\sigma _+e^{i\phi }+\sigma _{}e^{i\phi }),$$
(1)
and the two–qubit Hamiltonian

$$H_2=\stackrel{~}{\mathrm{\Delta }}|1111|+\frac{\stackrel{~}{\mathrm{\Omega }}}{2}\mathrm{I}1(\sigma _+e^{i\phi }+\sigma _{}e^{i\phi }).$$
(2)
As mentioned above, we will assume that most of the parameters appearing in these Hamiltonians are basically unknown. On the other hand, we will not consider any randomness in these parameters (the corresponding errors could be corrected with standard error correction methods Nielsen , as long as they are small). In particular we will assume that only $`\phi `$ can be precisely controlled. For the other parameters we will assume that: (1) they are given by an unknown (single valued) function of some experimentally controllable parameters; (2) they can be set to zero. For example, we may have $`\mathrm{\Omega }=f(I)`$, where $`I`$ is a parameter that can be experimentally controlled, and we only know about $`f`$ that $`f(0)=0`$ and that we can reach some value $`\mathrm{\Omega }_mf(I_m)0`$ for some $`I_m`$ unknown . Below we analyze a particular physical scenario which exactly corresponds to this situation. However, we want to stress that this situation can be naturally found in more general scenarios. For example, for atomic qubits the states $`|0`$ and $`|1`$ may correspond to two degenerate atomic (ground state) levels which are driven by two lasers of the same frequency and different polarization. The corresponding Hamiltonian is given by (1), where the parameters $`\phi ,\mathrm{\Omega },\mathrm{\Delta }`$ describe the relative phase of the lasers, the Rabi frequency and detuning of the two-photon Raman transition, respectively. The Rabi frequency can be changed by adjusting the intensity of the lasers, and the detuning and the phase difference by using appropriate modulators. In practice, $`\mathrm{\Omega }`$ ($`\mathrm{\Delta }`$) can be set to zero very precisely by switching off the lasers (modulators) and $`\phi `$ can be very precisely controlled to any number between 0 and $`2\pi `$. However, fixing $`\mathrm{\Omega }`$ or $`\mathrm{\Delta }`$ to a precise value (for example, $`23.098`$ kHz) may be much more challenging.

The idea of obtaining perfect gates with unknown parameters relies on the combination of adiabatic passage techniques holonomias2  and ideas of quantum control Bang . Let us recall the basic idea of adiabatic passage. Suppose we have a Hamiltonian that depends parametrically on a set of parameters, denoted by $`p`$, which are changed adiabatically with time along a given trajectory $`p(t)`$. After a time $`T`$, the unitary operator corresponding to the evolution is given by

$$U(T)=\underset{\alpha }{}e^{i(\varphi _\alpha +\psi _\alpha )}|\mathrm{\Phi }_\alpha [p(T)]\mathrm{\Phi }_\alpha [p(0)]|.$$
(3)
Here, $`|\mathrm{\Phi }_\alpha (p)`$ are the eigenstates of the Hamiltonian for which the parameters take on the values $`p`$. The phase $`\varphi _\alpha `$ is a dynamical phase that explicitly depends on how the parameters $`p`$ are changed with time, whereas the phase $`\psi _\alpha `$ is a purely geometrical phase ands depends on the trajectory described in the parameter space. Our basic idea to perform any given gate is first to design the change of the parameters in the Hamiltonians (1)-(2) such that the eigenvectors evolve according to the desired gate, and then to repeat the procedure changing the parameters appropriately in order to cancel the geometric and dynamical phases.

Let us first show how to perform the phase gate $`U=e^{i\theta \sigma _z/2}`$. We set $`\mathrm{\Delta }=0`$ for all times. The parameters $`(\mathrm{\Omega },\phi )`$ have to be changed as follows \[see Fig. 1(a)\] :

$`(0,0)`$ $`\stackrel{(i)}{}`$ $`(\mathrm{\Omega }_m,0)\stackrel{(ii)}{}(\mathrm{\Omega }_m,\theta /2)\stackrel{(iii)}{}(\mathrm{\Omega }_m,\theta /2+\pi )`$ (4)
$`\stackrel{(iv)}{}`$ $`(\mathrm{\Omega }_m,\theta +\pi )\stackrel{(v)}{}(0,\theta +\pi )`$
Steps (i,ii) and (iv,v) are performed adiabatically and require a time $`T`$. The double arrow of step (iii) indicates a sudden change of parameters. Note that $`\mathrm{\Omega }(0)=\mathrm{\Omega }(2T)=0`$, $`\mathrm{\Omega }(t)=\mathrm{\Omega }(2Tt)`$ and $`\phi (t)=\pi +\theta \phi (2Tt)`$, which does not require the knowledge of the function $`f`$ but implies a precise control of the phase. A simple analysis shows that (i-v) achieve the desired transformation $`|0e^{i\theta /2}|0`$, $`|1e^{i\theta /2}|1`$. Note also that the dynamical and geometrical phases acquired in the adiabatic processes (i-v) cancel out.

The Hadamard gate can be performed in a similar fashion. In the space of $`[\mathrm{\Delta },\mathrm{\Omega }_x=\mathrm{\Omega }\mathrm{cos}(\phi )]`$, the protocol is

$`(0,\mathrm{\Omega }_m)`$ $`\stackrel{(i)}{}`$ $`(\mathrm{\Delta }_m,\mathrm{\Omega }_m)\stackrel{(ii)}{}(\mathrm{\Delta }_m,0)\stackrel{(iii)}{}(\mathrm{\Delta }_m,\mathrm{\Omega }_m)\stackrel{(iv)}{}`$
$`(0,\mathrm{\Omega }_m)`$ $`\stackrel{(v)}{}`$ $`(0,\mathrm{\Omega }_m)\stackrel{(vi)}{}(\mathrm{\Delta },\mathrm{\Omega }_m)\stackrel{(vii)}{}(\mathrm{\Delta },0),`$ (5)
as shown in Fig. 1(b-c). In order to avoid the dynamical phases, we have to make sure that steps (i-v) are run in half the time as (vi-vii). More precisely, if $`t<T`$, we must ensure that $`\mathrm{\Delta }(t)=\mathrm{\Delta }(Tt)`$, $`\mathrm{\Omega }_x(t)=\mathrm{\Omega }_x(Tt)`$, $`\mathrm{\Delta }(T+t)=\mathrm{\Delta }(t/2)`$ and $`\mathrm{\Omega }_x(T+t)=\mathrm{\Omega }_x(t/2)`$. With this requisite we get $`\frac{1}{\sqrt{2}}(|0+|1)|0`$, $`\frac{1}{\sqrt{2}}(|0|1)|1`$. Again, the whole procedure does not require us to know $`\mathrm{\Omega }`$ or $`\mathrm{\Delta }`$, but rather to control the evolution of the experimental parameters which determine them.

The C-NOT gate requires the combination of two two-qubit processes using $`H_2`$ and one local gate. The first process involves changing the parameters $`[\stackrel{~}{\mathrm{\Delta }},\stackrel{~}{\mathrm{\Omega }}_x=\stackrel{~}{\mathrm{\Omega }}\mathrm{cos}(\phi )]`$ of Eq. (2) according to

$`(\stackrel{~}{\mathrm{\Delta }}_m,0)`$ $`\stackrel{(i)}{}`$ $`(\stackrel{~}{\mathrm{\Delta }}_m,\stackrel{~}{\mathrm{\Omega }}_m)\stackrel{(ii)}{}(0,\stackrel{~}{\mathrm{\Omega }}_m)\stackrel{(iii)}{}(0,\stackrel{~}{\mathrm{\Omega }}_m)`$ (6)
$`\stackrel{(iv)}{}`$ $`(\stackrel{~}{\mathrm{\Delta }}_m,\stackrel{~}{\mathrm{\Omega }}_m)\stackrel{(v)}{}(\stackrel{~}{\mathrm{\Delta }}_m,0).`$
This procedure gives rise to the transformation

$$U_1=|00|\mathrm{I}1+e^{i\xi }|11|i\sigma _y,$$
(7)
where $`\xi =_0^T\delta (t)𝑑t`$ is an unknown dynamical phase. The second operation required is a NOT on the first qubit $`U_2=(|01|+|10|)\mathrm{I}1`$. Finally, if $`\stackrel{~}{\mathrm{\Delta }}^{(1)}(t)`$ denotes the evolution of $`\stackrel{~}{\mathrm{\Delta }}`$ in Eq. (6), we need to follow a path such that $`\stackrel{~}{\mathrm{\Delta }}^{(3)}(t)=\stackrel{~}{\mathrm{\Delta }}^{(1)}(t)`$, $`\stackrel{~}{\mathrm{\Omega }}^{(3)}(t)=0`$. If the timing is correct, we achieve the transformation

$$U_3=(|00|+e^{i\xi }|11|)\mathrm{I}1.$$
(8)
Everything combined gives us the CNOT up to a global unimportant phase $`U_{cnot}=|00|\mathrm{I}1+|11|i\sigma _y=e^{i\xi }U_2U_3U_2U_1`$.

In Fig. 2(a) we illustrate the performance of our method, as well as its sensitivity against non–adiabatic processes. As a figure of merit we have chosen the gate fidelity Nielsen  $`=|\mathrm{Tr}\{U_{ideal}^{}U_{real}\}|^2/d^2`$, where $`d`$ is the dimensionality of the space ($`2`$ for local gates, $`4`$ for two-qubit gates), $`U_{ideal}`$ is the gate that we wish to produce and $`U_{real}`$ is the actual operation performed. As expected, for fixed parameters $`\{\mathrm{\Delta }_m/\mathrm{\Omega }_m=\stackrel{~}{\mathrm{\Delta }}_m/\stackrel{~}{\mathrm{\Omega }}_m=1/10,\phi _m=\pi /4\}`$, the adiabatic theorem applies when the processes are performed with a sufficiently slow speed. Typically a time $`T300/\mathrm{\Omega }_m,300/\stackrel{~}{\mathrm{\Omega }}_m`$ is required for the desired fidelity $`=110^4`$.

Let us now consider a set of bosonic atoms confined in a periodic optical lattice at sufficiently low temperature (such that only the first Bloch band is occupied). The atoms have two relevant internal (ground) levels, $`|a`$ and $`|b`$, in which the qubit is stored. This set-up has been considered in Ref. QC-mott  where it has been shown how single quantum gates can be realized using lasers and two–qubit gates by displacing the atoms that are in a particular internal state to the next neighbor location. The basic ingredients of such a proposal have been recently realized experimentally Bloch2 . However, in this and all other schemes so far williams  it is assumed that there is a single atom per lattice site since otherwise even the concept of qubit is no longer valid. In present experiments, in which the optical lattice is loaded with a Bose-Einstein condensate Jaksch1 ; Bloch1 , this is not the case (since zero temperature is required and the number of atoms must be identical to the number of lattice sites). We show now a novel implementation in which, with the help of the methods presented above, one overcomes this problem.

For us a qubit will be formed by an aggregate of atoms at some lattice site. The number of atoms forming each qubit is completely unknown. The only requirement is that there is at least one atom per site superfluid . We will denote by $`n_k`$ the number of atoms in the $`k`$–th well and identify the states of the corresponding qubit as

$$|0_k=\frac{a_k^{n_k}}{\sqrt{n!}}|\text{v}ac,|1_k=b_k^{}\frac{a_k^{(n_k1)}}{\sqrt{(n_k1)!}}|\text{v}ac,$$
(9)
where $`a_k^{}`$ ($`b_k^{}`$) are the creation operators for one atom in levels $`|a`$ and $`|b`$, respectively. The quantum gates will be realized using lasers, switching the tunneling between neighboring sites, and using the atom–atom interaction.

In the absence of any external field, the Hamiltonian describing our system is

$$H=J_k^{(b)}\underset{k}{}(b_{k+1}^{}b_k+b_k^{}b_{k+1})+\frac{U_{bb}}{2}\underset{k}{}b_k^{}b_k^{}b_kb_k.$$
(10)
Here, $`U_{bb}`$ and $`J_k^{(b)}`$ describe the interactions between and the tunneling of atoms in state $`|b`$. We will assume that $`J_k^{(b)}`$ can be set to zero and increased by adjusting the intensities of the lasers which create the optical lattice. We have assumed that the atoms in state $`|a`$ do not interact at all and do not hop, something which may be achieved by tuning the scattering lengths and the optical lattice. Both restrictions will be relaxed later on. The Hamiltonian (10) possesses a very important property when all $`J_k^{(b)}=0`$, namely it has no effect on the computational basis (i.e. $`H|\mathrm{\Psi }=0`$ for all states $`|\mathrm{\Psi }`$ in the Hilbert space generated by the qubits). Otherwise, it would produce a non–trivial evolution that would spoil the computation.

We show now how a single qubit gate on qubit $`k`$ can be realized using lasers. First, during the whole operation we set $`J_k^{(b)}=0`$ in order to avoid hopping. The laser interaction is described by the Hamiltonian

$$H_{las}^{(k)}=\frac{\mathrm{\Delta }_k}{2}(a_k^{}a_kb_k^{}b_k)+\frac{\mathrm{\Omega }_k}{2}(e^{i\phi }a_k^{}b_k+e^{i\phi }b_k^{}a_k).$$
(11)
For $`U_{bb}|\mathrm{\Delta }_k|,|\mathrm{\Omega }_k|`$, we can project the total Hamiltonian acting on site $`k`$ by an effective Hamiltonian acting on the qubit which resembles (1), with $`\mathrm{\Delta }=\mathrm{\Delta }_k`$ and $`\mathrm{\Omega }=\mathrm{\Omega }_k\sqrt{n_k1}`$. Thus, using the methods exposed above we can achieve the Hadamard and phase gates with a high precision, even though the coupling between the bosonic ensemble and light depends on the number of atoms.

For the realization of the two-qubit Hamiltonian (2) we need to combine several elements. First of all we need the Raman coupling of Eq. (11) to operate on the second well. Second, we need to tilt the lattice using a magnetic field Bloch1  which couples to states $`|a`$ and $`|b`$ differently, $`H_{tilt}=_kkg(a_k^{}a_kb_k^{}b_k)`$. And finally we must allow virtual hopping of atoms of the type $`|b`$ ($`J^{(b)}|U_{bb}g|`$). After adiabatic elimination we find that the effective Hamiltonian depends on the number of particles in the second site, $`n_2`$,

$$H_2^{eff}=\frac{J_b^2}{gU_{bb}}|1111|+\sqrt{n_21}\stackrel{~}{\mathrm{\Omega }}\mathrm{I}1\sigma _x.$$
(12)
The identification with Eq. (2) is evident, and once more the use of adiabatic passage will produce gates which are independent of the number of particles.

We have studied the different sources of error which may affect our proposal: (i) $`U_{bb}`$ is finite and (ii) atoms in state $`|a`$ may hop and interact. These last phenomena are described by additional contributions to Eq. (10) which are of the form $`J_k^{(a)}(a_k^{}a_{k+1}+a_{k+1}^{}a_k)`$, $`U_{aa}a_k^{}a_k^{}a_ka_k`$, and $`U_{ab}a_k^{}b_k^{}a_kb_k`$. The consequences of both imperfections are: (i) more than one atom per well can be excited, (ii) the occupation numbers may change due to hopping of atoms and (iii) by means of virtual transitions the effective Hamiltonian differs from (1) and (2). The effects (i)-(ii) are eliminated if $`(\mathrm{\Omega }/U_{bb})^21`$ and $`(J_k^{(a)}/U_{bb})^21`$. Once these conditions are met, we may analyze the remaining errors with a perturbative study of the Hamiltonians (11) and (10) plus the terms ($`J^{(a)},U_{ab},U_{aa}`$) that we did not consider before. In Eq. (11), the virtual excitation of two atoms increments the parameter $`\mathrm{\Delta }`$ by an unknown amount, $`\mathrm{\Delta }_{eff}\mathrm{\Delta }+2\mathrm{\Omega }^2n_k/(\mathrm{\Delta }+U_{ab}U_{bb})`$. If $`U_{ab}U_{bb}`$ and $`\mathrm{\Omega }^2n_kT/U_{bb}1`$, this shift may be neglected. In the two-qubit gates the energy shifts are instead due to virtual hopping of all types of atoms. They are of the order of $`\mathrm{max}(J^{(b)},J^{(a)})^2/g^2J^2/U_{bb}`$, and for $`J^2T/U_{bb}1`$ they also may be neglected.

To quantitatively determine the influence of these errors we have simulated the evolution of two atomic ensembles with an effective Hamiltonian which results of applying second order perturbation theory to Eq. (10), and which takes into account all important processes. The results are shown in Figs. 2(c-d). For the two-qubit gate we have assumed $`U_{aa}=U_{ab}`$, $`J^{(a)}=J^{(b)}=J`$, $`J_m=0.05U_{ab}`$, $`\mathrm{\Omega }_m=J_m^2/10`$, $`g=U_{bb}+U_{ab}/2`$ and operation time, $`T=200/\mathrm{\Omega }_m`$, while changing the ratio $`U_{bb}/U_{ab}`$ and the populations of the wells. For the local gates we have assumed $`\mathrm{\Delta }_m=1`$, $`\mathrm{\Omega }_m=U_{bb}/10`$ and different occupation numbers $`n_k`$, and we have also changed $`U_{bb}/\mathrm{\Omega }_m`$.

We extract several conclusions. First, the stronger the interaction between atoms in state $`|b`$, the smaller the energy shifts. Typically, a ratio $`U_{bb}=10^4U_{ab}`$ is required to make $`=110^4`$. Second, the larger the number of atoms per well, the poorer the fidelity of the local gates \[Figs. 2(b-c)\]. And finally, the fidelity of the two-qubit gate presents a small dependence on the population imbalance between wells.

In this work we have shown that it is possible to perform quantum computation even when the constants in the governing Hamiltonians are unknown. We have developed a scheme based on performing adiabatic passage with one-qubit (1) and two-qubit (2) Hamiltonians. With selected paths and appropriate timing, it is possible to perform a universal set of gates (Hadamard gate, phase gate and a CNOT). These procedures cannot only be used for quantum computing but also for quantum simulation Guifre . Finally, based on the preceding ideas, we have proposed a scheme for quantum computing with cold atoms in a tunable optical lattice. Our scheme works even when the number of atoms per lattice site is uncertain. Note that, these ideas also apply to some other setups like the microtraps recently realized in Ref. Ertmer .

We thank D. Liebfried and P. Zoller for discussions and the EU project EQUIP (contract IST-1999-11053).


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# UV-isomerisation in nematic elastomers as a route to photo-mechanical transducer

## 1 Introduction

It has recently been demonstrated nishi ; hogan\_paper  that properly designed liquid crystalline elastomers (LCE) can exhibit very strong photo-mechanical effects. Typical LCE are permanently crosslinked networks of polymer chains incorporating mesogenic groups either directly into the backbone or as side-groups, attached end-on or side-on to a flexible backbone. Such materials, which have been synthetically available for a few years fink81 , couple the mobile anisotropic properties of liquid crystals to the rubber-elastic matrix; many novel and interesting physical effects arise from this association. For example, the mechanical shape of a monodomain nematic LCE kupfer91  strongly depends on the underlying nematic order, which is a function of temperature. As the liquid-crystalline assembly undergoes the nematic-isotropic transition, it loses the associated anisotropy of polymer backbone chains induced by the coupling to nematic order. This leads to the macroscopic shape change of the sample, a uniaxial contraction, which can be utilised as a thermally-driven artificial muscle degen . The contraction can reach more than $`300\%`$, with a stress rising up to $`100`$kPa, wermter01 ; thermal01  and is theoretically well understood since the late 80s gelling ; khokhlov .

The nematic order parameter could be manipulated by means other than temperature, for example by applying an external stress or electric field, although the latter has been so far shown to have only a small effect. Another interesting way of affecting the nematic order is by introducing photo-isomerisable groups in their chemical structure, so that the mesogenic rod-like molecular shapes can be contorted by absorption of an appropriate photon. Several such groups are known in radiation chemistry, e.g. stilbenes or imines stilbene ; imine , but the most studied material in the context of liquid crystals is certainly azobenzene azobenzene ; eisen78 , Fig. 1. As their N=N bond is in the equilibrium trans state, the mesogenic moieties are straight and rigid, and as such contibute to the formation of the overall nematic order. In the metastable cis state the N=N bond is strongly bent so that the molecular group no longer has the rod-like shape. Thus, the proportion of cis isomers reduces the nematic order and shifts the clearing point to lower temperatures, as any other non-mesogenic impurity would. The resonant frequencies of radiation used to produce these molecular transformations are approximately the same in dense polymer systems as in dilute solutions eisen78 : $`365`$ nm for trans$``$cis and $`465`$ nm to achieve the back (cis$``$trans) reaction, which also occurs on heating. When azobenzene groups are incorporated into the polymer chains of a network crosslinked into a uniaxially aligned nematic elastomer,111One should also mention the important work on non-aligned nematic side-chain azopolymers keller ; ikeda . the photo-induced reduction of nematic order (fully analogous to heating) results in a uniaxial contraction of the sample, or an increase in force if the sample is mechanically restricted.

Such photo-mechanical effect in a monodomain nematic elastomer has been reported for the first time by Finkelmann et al. nishi  and studied in some detail by Hogan et al. hogan\_paper . However, photo-induced mechanical actuation has been performed much earlier, using ordinary isotropic polymer networks czech ; eisen80 , in which the required initial anisotropy has been induced by load. The magnitude of these effects was $`10^2`$-$`10^3`$ times smaller, with strains of 0.15-0.25%, and was caused by mechanical contraction of (aligned) network crosslinks containing azobenzene groups. The large uniaxial contraction on irradiation of nematic rubbers is a much more spectacular effect with an entirely different physical origin.

The main obstacle to turn this effect into a number of appealing application is its rather slow dynamics nishi ; hogan\_paper . On irradiation, the response was taking minutes, sometimes hours, to reach its saturation and it was similarly slow to relax. Could this be caused by a slow mechanical relaxation in the nematic elastomer, some time being necessary to change its conformation, or is it just the photo-isomerisation kinetics that is so slow? At the first glance, the first option appears quite reasonable because it is indeed known that nematic elastomers are notoriously slow in their mechanical relaxation clarkePRL ; hottaJPCM . In addition, it is known that although the kinetics of cis$``$trans isomerisation in dilute solutions is very fast, in the range of milliseconds ikeda2 , the effect in dense polymer melts has always been reported slow too keller ; ikeda ; eisen80 , suggesting the possible role of polymer dynamics.

To answer this fundamental question, and to try to validate more quantitatively the models of isomerisation kinetics, we have studied the photo-mechanical response of monodomain nematic rubber with azobenzene-containing mesogenic groups in end-on side chains (thus affecting the nematic ordering, but not having the direct mechanical effect of network crosslinks nishi ; eisen80 ). We measured the force exerted upon UV-irradiation on the clamps restricting the sample length. Such a configuration requires no physical movement of chains in the network, as opposed to the measurements of changing length of a freely-suspended sample nishi ; hogan\_paper , when the slow polymer relaxation could be a greater issue. We, however, found no increase in the speed of photo-mechanical response. The conclusion that the rate-limiting process is the photo-isomerisation itself has been further proven by the simultaneous measurement of nematic order parameter, the dynamics of which exactly matched the mechanical response.

This paper is organised as follows. The next section gives very brief description of material preparation, since we use the same (or very similar) materials to those studied in the pioneering work nishi ; hogan\_paper , as well as the details of experimental approach. Section 3 describes the photo-mechanical response in the “UV-on” and “UV-off” states, at different temperatures. Section 4 gives the results of parallel measurement of the nematic order parameter and relates its magnitude to the simple linear model of population dynamics of photo-isomerisation. This data analysis confirms the validity of linear model and identifies its key parameters. In the Conclusions we summarise the results and prospects.

## 2 Experimental

### 2.1 Preparation of nematic LCE

The starting materials and resultant aligned, monodomain nematic liquid crystal elastomer were prepared in our laboratory. The procedure for making the side-chain polysiloxanes by reacting the terminal vinyl group in the mesogenic moiety with the Si-H bond of the polysiloxane chain, as well as the two-step crosslinking technique with a uniaxial stress applied after the first stage of crosslinking to produce and freeze the monodomain nematic alignment, has been developed over the years by Finkelmann et al. kupfer91 ; kupfer94 . A number of minor modifications made to the original procedure are described in hogan\_paper ; thermal01 . The azobenzene compounds were all synthesised according to standard literature techniques boden83 ; vogel ; moreuv . These compounds, and the final composition of the nematic elastomer, are given in Fig. 2. This choice of components and concentrations was dictated by the results of hogan\_paper , where the photo-mechanical response was maximised for this combination. We consciously avoided placing the azobenzene groups into network crosslinks, as in nishi ; hogan\_paper ; eisen80 , in order to eliminate the direct mechanical coupling to the network: our purpose here is to study the effect induced purely by the changing nematic order.

The main mesogenic, rod-like units MBB2224’-methoxyphenyl-4-(4”-buteneoxy)benzoate. are known to produce a wide-range nematic phase and also reasonably stable under UV-irradiation (a number of stray photo-chemical reactions could occur in such complex organic compounds). The photo-isomerisable rod-like groups were BMAzo333\[4-(4”-buteneoxy)-4’-methyloxy\]azobenzene.. Both these end-on side groups have a 4-carbon spacer, which induces a parallel orientation of the rods to the siloxane backbone resulting in a prolate chain anisotropy in the nematic phase, with its principal radii of gyration $`R_{}>R_{}`$ spacer . The di-vinyl crosslinking agent is the flexible, non-mesogenic DiUB444di-1,4-(11-undeceneoxy)benzene. which is known to have only a minor mechanical effect on the nematic network, preserving soft elasticity and allowing sharp near-critical evolution on phase transformation. The polymer backbone onto which all these compounds were grafted was polyhydromethylsiloxane (PHMS), containing approximately 60 SiH groups per chain, obtained from ACROS Chemicals. The polymer network was crosslinked via an hydrosilation reaction, in the presence of a commercial platinum catalyst COD, obtained from Wacker Chemie. The final composition of the elastomer is, per Si unit, 72% MBB, 18% BMAzo and 10% DiUB (the latter figure means that, on average, there are 9 mesogenic side groups between crosslinking points.

Phase sequences were established on a Perkin Elmer Pyris 1 differential scanning calorimeter, which correlated with the critical temperature obtained by the thermal expansion measurements and optical microscopy between crossed polars. The permanently aligned monodomain networks were prepared by the two-step crosslinking reaction under load kupfer91 . In the resulting elastomeric material a broad nematic liquid crystalline phase was observed, between $`T_{\mathrm{ni}}=79^\mathrm{o}`$C and the glass transition at $`T_g0^\mathrm{o}`$C; optical microscopy, X-ray scattering and mechanical testing confirmed that this was indeed the nematic phase.

### 2.2 Mechanical measurements

Our mechanical setup is a custom-built device measuring the force exerted by the sample, and allowing to impose a fixed length and accurately maintain the temperature of the sample; see thermal01 ; clarkePRL  for more detail. The accuracy of the force measurements is $`\pm `$ 4.$`10^5`$ N ($`\pm `$ 0.4 mg).

The rectangular samples ($``$10$`\times `$2.5$`\times `$0.27 mm) were mounted with rigid clamps. The thermocouple was then placed behind the sample, as close as possible. As long as the temperature variations are slow, this enables us to measure the temperature of the sample. Of course, concerning the temperature measurements, the ideal would have been to imbed the thermocouple directly into the sample during crosslinking, but this would have affected both mechanical properties and the nematic order. As a compromise, we placed the thermocouple between the sample and the clamp during one of the experiments. No difference was found from the case with a thermocouple close behind the sample.

The UV radiation was produced by a Merck-4.L lamp (power 4W) providing a narrow band at $`365\pm 20`$ nm. The window of the thermally controlled compartment, allowing the passage of the radiation, was a single standard microscope slide, causing a $`10`$% loss. The intensity of the radiation reaching the sample was $`6`$ mW/cm2 (measured by a calibrated photodiode) and kept constant during the experiments.

The sequence of a typical experiment was as follows:

* The mechanical history of the sample is first eliminated by annealing, to start all experiments from the same conditions. The unconstrained sample was heated to $``$120 oC and then cooled (slower than 0.3 oC/min) to the ambient temperature.
* The temperature was set to a value that will then be kept as constant as possible; the sample was clamped and equilibrated at this temperature.
* The length of the sample was increased from the natural relaxed value to a marginally higher value. Thus the force exerted on the sample increased to a stable value above noise. The sample is equilibrated at this small extension.555More precisely, we wait for the force decay to be slow enough to be ignored. The complete stress relaxation would probably take weeks, or even be endless clarkePRL ; hottaJPCM
* At last, the elastomer is exposed to UV radiation. The force increases with time and eventually reaches saturation. The force and the temperature of the sample are constantly logged on the computer.
* The source of UV radiations is switched off and the sample is screened from all light. The force decreases with time and, finally, both the force and the temperature reach the initial values, set before the UV irradiation.
* After final equilibration, the temperature of the sample was given a small variation ($`\pm 23^\mathrm{o}`$) and the force variation logged in order to verify the underlying thermo-mechanical coefficient required in the subsequent data analysys.

The data for the force, transformed into stress by calibrating and dividing over the (constant) sample cross-section area, and the temperature were then used in the analysis of the process kinetics.

### 2.3 Birefringence measurements

The optical birefringence $`\mathrm{\Delta }n=n_{}n_{}`$ is one of the main, and very accurate, measures of the degree of orientational order in liquid crystals. It was determined using the method based on measuring the lock-in phase difference $`\theta `$ between the split parts of polarised laser beam, one passing through the birefringent sample, the other through the rotating analyser. The phase between the two beams is measured by an integer number of periods, $`N`$, plus $`\theta `$, and is related to $`\mathrm{\Delta }n`$ through eq. (1), where $`\lambda `$ is the wavelength of the laser, $`d`$ the thickness of the sample.

$$\mathrm{\Delta }n=\frac{\lambda }{d}\left(N+\frac{\theta }{2\pi }\right)$$
(1)
The details of this fast and accurate method are described in lim+ho . In our experiments, we have continuously logged the values of $`\mathrm{\Delta }n`$ as function of time, before, during and after UV irradiation. The kinetics of nematic order change, directly reflecting the population dynamics of cis and trans azobenzene isomers, was then compared with that of the mechanical response.

## 3 Photo-mechanical response

As long as no radiation is applied, the local nematic order parameter $`Q`$ is a function of temperature. If the monodomain texture is established in an elastomer, then the overall degree of director alignment has the same magnitude.666As opposed to, e.g., polydomain nematic where the local order is $`Q`$, but globally the degree of director alignment is zero. In this case the elastomer’s natural length along the director is determined by this order parameter. Therefore, this natural length is very sensitive to temperature variations, see Fig. 3(a). If, on the other hand, the sample shape is rigidly constrained, then instead a force is exerted on the clamps, Fig. 3(b), which is in direct proportion to the internal strain due to the underlying changing natural length thermal01 . However, one can notice a difference between the two representations of this thermo-mechanical effect: the length of the freely suspended sample, proportional to the nematic order $`Q(T)`$, changes in an abrupt near-critical fashion near the $`T_{\mathrm{ni}}`$. In contrast, the sample clamped at room temperature ends up under increasing uniaxial stress on heating and, accordingly, the transition to isotropic phase near the $`T_{\mathrm{ni}}`$ occurs in a diffuse supercritical fashion.

This strong dependence on temperature has an adverse effect on our photo-mechanical measurements. Figure 5 shows an example set of raw data on irradiating a sample clamped in the dynamometer. As the sample, absorbing UV, was heated by radiation,777This was checked by blocking the UV radiation in the setup remaining otherwise unchanged. In this case neither temperature, nor force increase has occurred. a slight temperature increase (of $`0.5^\mathrm{o}`$C) caused an additional force increase not related to the photo-isomerisation.

Thus, for more clarity, in the remaining of this paper we present the results corrected for these unwanted temperature variations. For the proper temperature adjustment one subtracts from the raw measured force the value it would have without the UV, at the current (increasing) temperature. To find the latter, we simply record, independently, the variation of force against temperature as in Fig. 3(b).

The force responses were recorded at various initial temperatures and adjusted to the fixed value of temperature as described above. The amplitude of mechanical response depends on temperature, being more steep in the vicinity of $`T_{\mathrm{ni}}`$, see hogan\_paper  for more details. Figure 6 shows the set of such stress increases at different temperatures. The overall magnitude of the effect is given by the saturation level $`\mathrm{\Delta }\sigma _{max}`$, the difference between the value the stress finally reached and its value before the UV to be switched on. The magnitude of $`\mathrm{\Delta }\sigma _{max}`$ varies over our range of temperatures, but remains in the range of 1.5-3.5 kPa. To specifically compare the rates of the response, we plot in Figs. 7 and 8 the normalised results for the increase in stress $`\mathrm{\Delta }\sigma /\mathrm{\Delta }\sigma _{max}`$ on irradiation, and the corresponding thermal relaxation of stress in the dark.

As the stress again reaches its initial value after the UV radiation is switched off, one could expect the effect to be repeatable. Figure 9 shows such a test of repeatability, a crucial characteristics if one to have a practical application in mind. Overall, the effect is clearly reproducible, however, a small decay was found when repeating the light/dark cycle many times. We attribute this weakening to the destruction of few azobenzene groups (photo-bleaching), after several trans$``$cis$``$trans cycles (one must remember the equilibrium reached upon UV-irradiation is dynamic, so that the molecules are continuously cycling from cis down to trans and back up again).

## 4 Order parameter and population dynamics

The linear population dynamics model presented here is derived from the one proposed in hogan\_paper . Despite the good agreement with experiment, one could argue that it is not the only possibility. And indeed, at this point, only the final predictions made in eqs (6) and (7) were compared with experimental results. This dynamics could instead be explained in terms of a mechanical relaxation in the polymer network, the times measured being in fact those needed for the polymer chains to respond. So, it was crucial to check experimentally the main ideas expressed in the simple analysis of isomerisation dynamics.

An answer, albeit qualitative, is given by Fig. 10 in which both the birefringence and the stress variations ($`\mathrm{\Delta }n`$ and the negative of $`\mathrm{\Delta }\sigma `$, respectively) are plotted. The stress variation has been inverted \[we actually plot $`\sigma _{initial}\sigma (t)`$\] for an illustrating purpose, to superpose both data sets and show they have the same characteristic dynamics. We do not say the relaxation times are equal, but they clearly are of the same order of magnitude. This result is important. First of all it proves the nematic order (closely reflected by $`\mathrm{\Delta }n`$) actually diminishes upon UV irradiation. Secondly it shows that this order decreases and then increases with a speed roughly as the stress variations, and is therefore the rate-limiting process in this photo-actuation.

As explained in the Introduction, the proportion of cis isomers influences the macroscopic shape of the elastomer through the decrease in the nematic order parameter $`Q`$. The photo-isomerization of small molecular weight azobenzene compounds, in solution, is known to follow simple first order kinetics. Only minor modifications were found when the reaction occurs in a dense polymer matrix eisen78 . We will therefore assume, as was done in Ref. nishi ; hogan\_paper , that the population dynamics is first order, and more precisely described by equation

$$\frac{}{t}n(t,T)=\eta n\frac{1}{\tau _{tc}}n+\frac{1}{\tau _{ct}}(n_0n)$$
(2)
where $`n`$ denotes the number of trans azobenzene moieties, $`n_0`$ the total number of trans plus cis isomers (which is constant and given by the initial composition, Fig. 2). $`\tau _{tc}`$ and $`\tau _{ct}`$ are the characteristic times of spontaneous trans$``$cis and cis$``$trans transformations, respectively. Unlike the cis$``$trans transition, the trans$``$cis process does not occur spontaneously on heating. Accordingly, we shall neglect $`\tau _{tc}`$ compared with $`\tau _{ct}`$. The forced UV isomerisation occurs with the rate $`\eta 1/\tau _{uv}`$ the radiation intensity.

One can easily obtain the number of cis isomers upon irradiation

$$n_{cis}(t)=n_0\left(1\tau _{\mathrm{eff}}/\tau _{ct}\right)\left(1\mathrm{exp}^{t/\tau _{\mathrm{eff}}}\right)$$
(3)
where the light is switched on at $`t=0`$ and the notation

$$\tau _{\mathrm{eff}}=\frac{1}{\eta +1/\tau _{ct}}=\frac{\tau _{ct}}{1+\eta \tau _{ct}}$$

is used. Setting $`\eta `$ to $`0`$, and assuming in eqn (3) that $`n_{cis}=n_{cis}(\mathrm{})`$ (that is, that the saturation is reached on irradiation, which is the case experimentally), the relaxation dynamic is given by

$$n_{cis}(t)=n_{cis}(\mathrm{})\mathrm{exp}^{t/\tau _{ct}}$$
(4)
where the light is switched off at $`t=0`$.

And now, how to take in account the destabilising effect of the contorted cis isomers? As was done in hogan\_paper , we shall simply consider them as impurities shifting the critical temperature of nematic-isotropic transition. Thus, as the mechanical properties of the elastomer are depending on $`TT_{\mathrm{ni}}`$, this is equivalent to shifting the actual temperature of the material. We will assume this shift to be linear, eqn (5). This approximation is justified by the rather small value of the factor (in front of $`TT_{\mathrm{ni}}`$) this shift will be found to equal. This factor $`\beta `$ is positive: the impurities weaken the order of the nematic liquid crystal:

$$T_{\mathrm{eff}}=T_{measured}+\beta n_{cis}$$
(5)
The experimentally measured relation between stress and temperature, an example of which is given by Fig. 3(b), can then be used to obtain the stress variation generated by this effective temperature shift. The stress-temperature relation, over the whole range of available temperatures, is of course highly non-linear. However, again, as the relative effective temperature shift, or the relative stress increase, are small in our experiments, one can approximate it as a linear function around each particular experimental temperature. So, finally, the following relation stands for the measured stress under irradiation

$$\sigma (t)\sigma _{initial}=\mathrm{\Delta }\sigma _{max}\left(1\mathrm{exp}^{t/\tau _{\mathrm{eff}}}\right)$$
(6)
while the relaxation is described by

$$\sigma (t)\sigma _{initial}=\mathrm{\Delta }\sigma _{max}\mathrm{exp}^{t/\tau _{ct}}$$
(7)
with

$$\mathrm{\Delta }\sigma _{max}=a\beta n_0\left(1\tau _{\mathrm{eff}}/\tau _{ct}\right),$$

$`a`$ being the slope of the discussed linear stress-temperature relation (which can be easily obtained experimentally) at the temperature of irradiation. $`\sigma _{initial}`$ is the stress set at the beginning of the experiment, before any UV to be applied (equal in our case to 21.7 kPa for all measurements).

Does this rather simple model fit our results? $`\mathrm{\Delta }\sigma _{max}`$ is directly obtained by subtracting the initial stress $`\sigma _{initial}`$ from the steady-state saturation value reached under irradiation. Then, only one free parameter remains: the characteristic time, $`\tau _{\mathrm{eff}}`$ for the excitation and $`\tau _{ct}`$ for the relaxation. An example is given for both excitation and relaxation in the log-linear plots in Fig. 11. If eqs (6) and (7) are correct then these curves should be linear. This appears to be true, except for very short times where one can notice respectively anomalously fast (at the beginning of the forced excitation) and slow responses (at the beginning of the thermal relaxation). This small deviation from the linear model could be caused by a slightly more complicated isomerisation kinetics, perhaps dependent on a less trivial shape of the energy barrier separating the isomer states. But it is not caused by the actual non-linearity of the stress-temperature relation, Fig. 3(b), for explicitly taking into account this non-linearity does not improve the data fits at all. Whatever the physical reason, the correction at short times is small and does not challenge the overall hypothesis of linear dynamics.

Fitting the time dependence of stress increase on irradiation, or the decrease on thermal relaxation, provides values of $`\tau _{\mathrm{eff}}`$ and $`\tau _{ct}`$ at different temperatures, and thus the value of the isomerisation rate

$$\tau _{uv}\frac{1}{\eta }=\frac{1}{1/\tau _{\mathrm{eff}}1/\tau _{ct}}.$$

Figure 12 is an Arrhenius plot of these characteristic times enabling us to estimate the energy barriers for the isomerisation. We find $`E_a=`$0.5 eV for the light-induced trans to cis reaction ($`\tau _{uv}`$) and $`E_a=`$0.77 eV for the spontaneous thermal relaxation ($`\tau _{ct}`$). These times and activation energies are of the same order of magnitude as those obtained by Eisenbach eisen78  when studying the population dynamics of photo-isomerisable azobenzene compounds in an ordinary isotropic polymer matrix. In the framework of this model, we can also calculate the factor

$$\beta n_0=\frac{\mathrm{\Delta }\sigma _{max}}{b\left(1\tau _{\mathrm{eff}}/\tau _{ct}\right)},$$

as all the terms in the right hand side are accessible experimentally. This product, reflecting the ultimate efficiency of the material as a transducer (assuming $`\tau _{\mathrm{eff}}/\tau _{ct}1`$), is equal to 4.0 $`\pm `$ 1 oC, which is very close to the value found in hogan\_paper  by a different method.

## Conclusion

In this work, we have explored the response of a novel photo-mechanical transducer generating the deformations of forces many orders of magnitude higher than the effects known before. The explanations given to the phenomenon, based on the direct effect of photo-isomerisation on the nematic order parameter and that on the mechanical state of nematic rubber, have been accurately validated. We point out that the actuation speed is dominated by the photo-isomerisation dynamics, which appears to be very slow in a dense polymer matrix. On the one hand, the isomerisation rate $`\eta `$ can be easily increased by simply using more intense radiation. On the other hand, even leaving aside adverse effects of photo-degradation, the overall magnitude of the response, reflected by the effective temperature shift, should be ultimately limited at $`\beta n_0`$ ($``$oC in our material).

For practical applications, as well as for a better understanding of the fundamental phenomenon, it would be very interesting to check these assertions, using various intensities of light. The maximum temperature shift obtained with our elastomer could seem small, but can however generate noticeable contractions or forces. Its intensity should be magnified in the vicinity of the critical temperature, because of the higher slope of the underlying thermo-mechanical behaviour there (see Fig. 3). It would therefore be useful to synthesise elastomers with transition temperatures close to the ambient 20oC.

This research was made possible due to the Visiting Fellowship (Stage de Maîtrise) of JC, provided by the École Normale Supérieure de Cachan. We thank EPSRC UK for the support of ART. Invaluable experimental help of Sébastien Courty, Laurent Costier, Atsushi Hotta and Richard Gymer is gratefully appreciated, as are the discussions with Mark Warner and Yong Mao.


text:
# Semi–analytical solution of the Kondo model in a magnetic field

## I Introduction

The single impurity Kondo or $`s`$$`d`$ model (SIKM) kondo

$$H_{\mathrm{SIKM}}=\underset{\stackrel{}{k}\sigma }{}ϵ_\stackrel{}{k}^{}c_{\stackrel{}{k}\sigma }^{}c_{\stackrel{}{k}\sigma }^{}+J\underset{\stackrel{}{k}\stackrel{}{k}^{}}{}\underset{\alpha \beta }{}c_{\stackrel{}{k}\alpha }^{}\stackrel{}{S}\stackrel{}{\sigma }_{\alpha \beta }^{}c_{\stackrel{}{k}^{}\beta }^{}$$
(1)
is, together with its close relative, the single impurity Anderson model (SIAM) anderson , one of the fundamental models in the theory of correlated electron systems. It has been studied extensively over the past four decades hewson , but despite its simplicity, no complete analytic solution exists that provides information on both thermodynamic and dynamical quantities. For example, the Bethe ansatz solution bethe ; hewson  has solved all universal properties of the Kondo problem including its high– to low–temperature crossover behavior. But the Bethe ansatz requires the limit of infinite conduction band width and cannot be used to calculate dynamical quantities beyond the low–energy limit.

Thus, numerical methods, like Wilson’s numerical renormalization group (NRG) Wilson ; hewson  or quantum Monte–Carlo (QMC) fye , in connection with maximum–entropy methods MEM  have to be employed to access dynamical quantities on all energy scales. In both methods, evaluation of dynamical properties, and quantities related to them, like the Korringa–Shiba relation or the Friedel sum rule hewson , suffer from unavoidable numerical errors. QMC simulations, in addition, cannot be used at zero temperature and are restricted to comparatively large values of $`J`$.fye  Moreover, a reliable evaluation of single– and two–particle spectra and related quantities in an external magnetic field, as well as their comparison and interpretation within a local Fermi liquid picture hewson  become rather problematic costi ; logan4 , especially in the limit of vanishing external magnetic field. Approximate analytical techniques, like perturbation expansions or $`1/N`$–expansions hewson , typically only describe certain properties of the Kondo model correctly. A notable exception in this respect is the so–called local moment approach (LMA) logan . This perturbative approach is very accurate in most cases logan2 , including those of nonvanishing external magnetic fields.logan3 ; logan4

Besides its relevance for the study of moment formation in metals, the SIKM (1) has gained new importance as input for investigating non–dilute correlated electron systems like heavy fermion materials within dynamical mean–field theory (DMFT).DMFT  Here a reliable method for calculating single–particle correlation functions, especially close to the Fermi energy, is extremely important.

In this paper, we propose a new non–perturbative semi–analytical approach to the Kondo problem based on Wegner’s flow equation method wegner  and previous work on applications of flow equations to strong–coupling problems strong\_coupling ; Hofstetter\_Kehrein . We will show that to a very good approximation, many physical quantities of the Kondo model can be calculated from a resonant level model (RLM), where the interacting features of the Kondo model are encoded in a non–constant effective hybridization function of this resonant level model. Surprisingly, this noninteracting effective model describes both universal low–energy properties like the Wilson ratio as well as high–energy power laws and logarithmic corrections with very good accuracy. Due to the noninteracting nature of this effective model this mapping allows immediate insights into the physics of the SIKM, for example the dependence of its static and dynamical quantities on a local magnetic field.

After presenting our approach in the next section, we will discuss several static quantities at $`T=0`$ as a function of a local magnetic field and derive analytical expressions for their asymptotic behavior. As an example for a dynamical quantity, we will then discuss the spin–structure factor and the Korringa–Shiba relation. An outlook on potential future applications of our approach concludes this paper.

## II Mapping to a resonant level model

### II.1 Principles of the flow-equation method

The general framework of the flow equation methodwegner  and its application to the Kondo model has been explained in detail in Ref. Hofstetter\_Kehrein, . Here we will only repeat the main steps in order to make this paper self–contained, and refer to Ref. Hofstetter\_Kehrein,  for more details.

The key idea of the flow equation approach consists in performing a continuous sequence of infinitesimal unitary transformations on a given Hamiltonian

$$\frac{dH(B)}{dB}=[\eta (B),H(B)].$$
(2)
With an anti–Hermitian generator $`\eta (B)`$ the solution of equation (2) describes a family of unitarily equivalent Hamiltonians $`H(B)`$ parameterized by the flow parameter $`B`$. By choosing $`\eta (B)`$ appropriatelywegner  one can set up a framework that diagonalizes a many–particle Hamiltonian $`H(B=0)`$, i.e. $`H(B=\mathrm{})`$ becomes diagonal.

The concrete realization of this approach for the Kondo model was discussed in Ref. Hofstetter\_Kehrein, . The starting point is the bosonized formboson  of the Hamiltonian (1). Since we will be mainly interested in describing the basic ideas of our approach, we restrict ourselves to a linear dispersion relation. Notice, however, that the flow equation approach can also be used for a nontrivial conduction band density of states as it does not rely on the integrability of the model.perspective  With a linear dispersion relation the Kondo problem becomes effectively one–dimensional, the charge density excitations in (1) decouple, and we only need to look at the spin density part

$$H=H_0\frac{J}{\sqrt{8\pi ^2}}_x\mathrm{\Phi }(0)S^z+\frac{J}{4\pi a}(e^{i\sqrt{2}\mathrm{\Phi }(0)}S^{}+\mathrm{h}.\mathrm{c}.)$$
(3)
with $`H_0=_{q>0}q\sigma (q)\sigma (q)`$. Here $`\sigma (p)=\frac{1}{\sqrt{2|p|}}_q(c_{p+q}^{}c_q^{}c_{p+q}^{}c_q^{})`$ are the bosonic spin density modes with the bosonic spin density field defined by $`\mathrm{\Phi }(x)=i_{q0}\frac{\sqrt{|q|}}{q}e^{iqxa|q|/2}\sigma (q)`$. For simplicity we have set the Fermi velocity $`v_F=1`$. $`a`$ is proportional to the inverse conduction band width. All our latter results will be expressed as universal functions of the low–energy Kondo scale $`T_\mathrm{K}`$, and we can consider (3) to be equivalent to our original Kondo Hamiltonian if $`T_\mathrm{K}a^1`$.

Eq. (3) was used as the starting point $`H(B=0)`$ of the flow equation approach in Ref. Hofstetter\_Kehrein, . Away from the Toulouse point the unitary equivalence of the flow holds only approximately, but this approximation can be controlled by a small parameterstrong\_coupling  and yields very accurate results. During the flow the Hamiltonian can be parameterized as

$`H(B)`$ $`=`$ $`H_0+{\displaystyle \underset{p}{}}g_p(B)(C_p^{}(\lambda (B))S^{}+\mathrm{h}.\mathrm{c}.)`$
$`+{\displaystyle \underset{p}{}}\omega _p(B)[C_p^{}(\lambda (B_p)),C_p^{}(\lambda (B_p))].`$
Here $`B_p\stackrel{\mathrm{def}}{=}p^2`$, and $`C_p^{}(\lambda ),C_p^{}(\lambda )`$ denote normalized vertex operators with scaling dimension $`\lambda >0`$ in momentum space,

$`C_p^{}(\lambda )`$ $`\stackrel{\mathrm{def}}{=}`$ $`\left({\displaystyle \frac{\mathrm{\Gamma }(\lambda ^2)}{2\pi aL}}\right)^{1/2}|pa|^{(1\lambda ^2)/2}{\displaystyle _{L/2}^{L/2}}𝑑xe^{ipx+i\lambda \mathrm{\Phi }(x)}`$
$`C_p^{}(\lambda )`$ $`\stackrel{\mathrm{def}}{=}`$ $`\left({\displaystyle \frac{\mathrm{\Gamma }(\lambda ^2)}{2\pi aL}}\right)^{1/2}|pa|^{(1\lambda ^2)/2}{\displaystyle _{L/2}^{L/2}}𝑑xe^{ipxi\lambda \mathrm{\Phi }(x)}`$
that obey $`\mathrm{\Omega }|C_p^{}(\lambda )C_p^{}^{}(\lambda )|\mathrm{\Omega }=\delta _{pp^{}}\theta (p)`$ and $`\mathrm{\Omega }|C_p^{}(\lambda )C_p^{}^{}(\lambda )|\mathrm{\Omega }=\delta _{pp^{}}\theta (p)`$. For the special case $`\lambda =1`$ they fulfill fermionic anticommutation relations $`\{C_p^{}(1),C_p^{}^{}(1)\}=\delta _{pp^{}}`$ and can therefore be interpreted as creation and annihilation operators for fermions.

In Ref. Hofstetter\_Kehrein,  the following flow equations for the parameters in (II.1) have been derived

$`{\displaystyle \frac{dg_p}{dB}}`$ $`=`$ $`p^2g_p+{\displaystyle \frac{2\pi }{\mathrm{\Gamma }(\lambda ^2)}}{\displaystyle \underset{qp}{}}{\displaystyle \frac{p+q}{pq}}g_pg_q^2|qa|^{\lambda ^21}`$ (5)
$`+{\displaystyle \frac{1}{4}}g_p\mathrm{ln}(B/a^2){\displaystyle \frac{d\lambda ^2}{dB}}`$
$`{\displaystyle \frac{d\omega _q}{dB}}`$ $`=`$ $`{\displaystyle \frac{2\pi }{\mathrm{\Gamma }(\lambda ^2)}}qg_q^2|qa|^{\lambda ^21}`$ (6)
and a differential equation for the flow of the scaling dimension

$$\frac{d\lambda ^2}{dB}=\frac{8\pi \lambda ^2(1\lambda ^2)}{\mathrm{\Gamma }(\lambda ^2)}\underset{q}{}g_qg_q|qa|^{\lambda ^21}.$$
(7)
It can be shownHofstetter\_Kehrein  that one always finds $`\lambda \stackrel{B\mathrm{}}{}1`$ in the strong–coupling phase of the Kondo model, i.e. in the low–energy limit the vertex operators in (II.1) become fermions. In the following we will use an improved version of the above flow equations by taking into account that all approximations should be performed with respect to the interacting ground state: It turns out that the only necessary modification in (5), (6) and (7) is that the exponent in $`|qa|^{\lambda ^21}`$ gets replaced by $`\lambda ^2(B_q)1`$, i.e. it is not a running exponent anymore.Kehrein\_tobepublished

### II.2 Equivalence to a resonant level model

Now we will compare this system of differential equations with the flow equations for a resonant level model (RLM). This will lead to the key result of this paper: the RLM can be used as an effective model for the complicated strong–coupling Kondo model.

The Hamiltonian of the resonant level model is given by

$$H_{\mathrm{RLM}}=\underset{k}{}ϵ_k^{}c_k^{}c_k^{}+ϵ_d^{}d^{}d+\underset{k}{}V_k^{}(c_k^{}d+d^{}c_k^{})$$
(8)
Following the same flow equation approach as previously in the SIKM, we establish a solution to the RLM (8). A detailed description of the flow equation solution can be found in Ref. SIAM, . One finds the following flow equations for the parameters in (8)

$`{\displaystyle \frac{dV_k}{dB}}`$ $`=`$ $`V_k(ϵ_dϵ_k)^2+{\displaystyle \underset{qk}{}}V_k^{}V_q^2{\displaystyle \frac{ϵ_k+ϵ_q2ϵ_d}{ϵ_kϵ_q}}`$ (9)
$`{\displaystyle \frac{dϵ_d}{dB}}`$ $`=`$ $`2{\displaystyle \underset{k}{}}V_k^2(ϵ_kϵ_d)`$ (10)
$`{\displaystyle \frac{dϵ_k}{dB}}`$ $`=`$ $`2V_k^2(ϵ_kϵ_d)`$ (11)
It should be noted that this yields the exact analytical solution. Having established the flow equations to solve both the SIKM and the RLM, respectively, one can now show an approximate equivalence of these two models. We introduce the substitution

$`V_k^2={\displaystyle \frac{2\pi }{\mathrm{\Gamma }(\lambda ^2(B_k))}}g_k^2|ka|^{\lambda ^2(B_k)1}`$ (12)
and notice that with this substitution the two set of flow equations (5,6) and (911) become equivalent for $`ϵ_d=0`$ in the RLM, with the exception of the logarithmic term in (5). Thus we now have established an approximate mapping of the SIKM onto the RLM by means of (12) in the sense that their flow equation diagonalization is identical. We shall refer to this relation by introducing the effective hybridization function $`\mathrm{\Delta }_{\mathrm{eff}}(ϵ)=\pi _kV_k^2\delta (ϵϵ_k)`$: the RLM with this non–trivial hybridization function can be used as an effective model for the SIKM in the Kondo limit (small coupling limit) $`\rho _0J0`$. Since this noninteracting RLM is a simple, quadratic Hamiltonian, this mapping will allow us to read off and understand many properties of the complicated many–body Kondo physics in an intuitive and straightforward way. It will turn out that the deviations of $`\mathrm{\Delta }_{\mathrm{eff}}(ϵ)`$ from a constant hybridization function encode the quasiparticle interaction and therefore the many–body Kondo physics in this quadratic effective Hamiltonian.

Notice that the above mapping between the SIKM and the RLM becomes exact at the Toulouse point Toulouse  $`\rho _0J=2\pi (2\sqrt{2})`$ since $`\lambda ^2(B)=1`$ for all flow parameters $`B`$. One easily verifies that the effective RLM then has a constant hybridization function, $`\mathrm{\Delta }_{\mathrm{eff}}(ϵ)=\frac{\pi }{4}\rho _0J^2`$. In this case, our mapping just reduces to the observation already made by Toulouse that the partition function of the Kondo model for this specific coupling constant $`J`$ is exactly equivalent to the partition function of a quadratic Hamiltonian.Toulouse

In order to specify the function $`\mathrm{\Delta }_{\mathrm{eff}}(ϵ)`$ in the Kondo limit it is best to not directly use relation (12), but to determine the effective hybridization function from matching a correlation function in the SIKM and the RLM. We have chosen the $`S^+(t)S^{}(0)`$–correlation function, evaluated it with respect to (II.1) for $`B=0`$, and then chose $`\mathrm{\Delta }_{\mathrm{eff}}(ϵ)`$ in the RLM such that this coincided with the $`d^{}(t)d(0)`$–correlation function. The resulting $`\mathrm{\Delta }_{\mathrm{eff}}(ϵ)`$ agrees with (12) in the high– and low–energy regimes, with deviations only in the crossover region. However, the mapping from the Kondo model to the effective RLM becomes better since this procedure manages to partly also take the logarithmic term in (5) into account.

The resulting effective hybridization function can be scaled into a dimensionless form with one dimensionful parameter $`\mathrm{\Delta }_{\mathrm{eff}}^0T_\mathrm{K}`$

$$\mathrm{\Delta }_{\mathrm{eff}}(ϵ)=\mathrm{\Delta }_{\mathrm{eff}}^0\stackrel{~}{\mathrm{\Delta }}_{\mathrm{eff}}(ϵ/\mathrm{\Delta }_{\mathrm{eff}}^0).$$
(13)
$`\stackrel{~}{\mathrm{\Delta }}_{\mathrm{eff}}(x)`$ is a universal function in the Kondo limit ($`\rho _0J0`$). It is depicted in Fig. 1 for $`\rho _0J=0.1`$, and coincides with its universal form for $`|x|30`$ ($`|ϵ|60T_\mathrm{K}`$, i.e. this should be sufficient for most practical purposesnumerics ). For larger energies the effective hybridization function begins to cross over into linear behavior with logarithmic corrections depending on the bare coupling $`\rho _0J`$.

The following function provides an excellent fit (see Fig. 1)

$$\stackrel{~}{\mathrm{\Delta }}_{\mathrm{eff}}(x)=\begin{array}{c}1+\frac{1}{2}a_1\mathrm{ln}\left(1+\left(\frac{x}{a_0}\right)^2\right)\hfill \\ +a_2\left(\mathrm{arctan}\left|\frac{x}{a_0}\right|\left|\frac{x}{a_0}\right|\right)\left(1\mathrm{ln}\left|\frac{x}{a_0}\right|\right)\hfill \end{array}$$
(14)
with the parameters from Table 1.

A similar analysis based on the comparison of flow equations shows that the above mapping between the SIKM and the noninteracting RLM can be extended to the case of a Kondo Hamiltonian (1) with a nonvanishing local magnetic field $`h`$

$$H_{\mathrm{SIKM}}+g\mu _BhS_z$$
(15)
by setting $`ϵ_d=g\mu _Bh`$ in the RLM. However, the mapping with the above effective hybridization function becomes less accurate for $`g\mu _B|h|T_\mathrm{K}`$ due to the approximate nature of the flow equation solution (57). We will discuss this point in more detail below.

Summing up, as long as we are interested in static quantities in a local magnetic field smaller than approximately $`T_\mathrm{K}`$ and/or dynamical correlation functions for energies smaller than approximately $`60T_\mathrm{K}`$, we can use the RLM with the effective hybridization function (14) to describe the physics of the SIKM in the small coupling limit. The only undetermined parameter in the RLM is the energy scale $`\mathrm{\Delta }_{\mathrm{eff}}^0`$ that explicitly depends on $`J`$. This overall energy scale is proportional to $`T_\mathrm{K}`$. Notice that the non–perturbative behavior of this energy scale

$$T_\mathrm{K}e^{1/\rho _0J}$$
(16)
follows correctly from the original flow equations (57), compare Ref. Hofstetter\_Kehrein, .

### II.3 Calculation of physical quantities

Once the mapping between the SIKM (1) and the effective RLM (8) has been established, one can readily calculate physical quantities for the Kondo model. One complication arises from the fact that operators of the original SIKM have to be transformed by a unitary transformation analogous to (2). In the language of the effective resonant level model they will thus in general correspond to more complicated many–particle operators. Since the intention of this paper is to demonstrate the potential of our mapping in a pedagogical setting, we will concentrate on two quantities that remain simple under these transformations: i) the $`z`$-component of the spin operator $`S_z`$, which becomes $`S_z=d^{}d1/2`$, and ii) the Hamiltonian itself.

From the latter we obtain the internal energy $`U_{\mathrm{imp}}=HH_0`$ and the Sommerfeld coefficient, $`\gamma _{\mathrm{imp}}(h)`$. A straightforward calculation in the noninteracting RLM yields

$$\gamma _{\mathrm{imp}}(h)=\frac{\pi ^2k_\mathrm{B}^2}{3}\rho _d(0)\left(1\mathrm{\Lambda }^{}(0)\right)$$
(17)
where $`\mathrm{\Lambda }^{}(\omega )`$ denotes the derivative of

$$\mathrm{\Lambda }(\omega )=\frac{1}{\pi }\mathrm{P}𝑑ϵ\frac{\mathrm{\Delta }_{\mathrm{eff}}(ϵ)}{\omega ϵ}$$

and $`\mathrm{P}\mathrm{}`$ is the principal value integral. Here $`\rho _d(ϵ)`$ is the impurity orbital density of states of the RLM

$$\rho _d(ϵ)=\frac{1}{\pi }\frac{\mathrm{\Delta }_{\mathrm{eff}}(ϵ)}{(ϵg\mu _Bh\mathrm{\Lambda }(ϵ))^2+\mathrm{\Delta }_{\mathrm{eff}}^2(ϵ)}.$$
(18)
The result (17) for $`\gamma _{\mathrm{imp}}`$ has some interesting implications. First, because $`d^{}`$ is connected to $`S_+`$, it is apparent that the low–energy excitations in the system are controlled by spin degrees of freedom, a well–known feature of the Kondo physics. However, in our approach this result can be read off directly from equ. (17). Second, $`\rho _d(0)1/\mathrm{\Delta }_{\mathrm{eff}}(0)1/T_\mathrm{K}`$, i.e. we obtain the correct scaling behavior for $`\gamma _{\mathrm{imp}}`$ directly from the behavior of $`\mathrm{\Delta }_{\mathrm{eff}}(ϵ)`$. There is, however, a nontrivial correction coming from the factor in parenthesis in (17). Note that for $`\mathrm{\Delta }_{\mathrm{eff}}(ϵ)=`$const. this correction is one, but for the strongly $`ϵ`$–dependent $`\mathrm{\Delta }_{\mathrm{eff}}(ϵ)`$ in Fig. 1 it is of the order of two. As we will demonstrate later, this difference is directly responsible for obtaining the correct Wilson ratio in our approach.

From the mapping $`S_z=d^{}d1/2`$ it is easy to calculate $`\chi _{zz}(\omega +i\delta )=(g\mu _B)^2d^{}d;d^{}d_{\omega +i\delta }`$. Since the correlation function has to be evaluated within the RLM, one obtains for the imaginary part at $`T=0`$

$$\chi _{zz}^{\prime \prime }(\omega )=(g\mu _B)^2\pi \underset{\omega }{\overset{0}{}}𝑑\omega ^{}\rho _d(\omega ^{})\rho _d(\omega +\omega ^{}).$$
(19)
Again, this result provides direct access to an interpretation of the behavior of $`\chi _{zz}(\omega +i\delta )`$ in terms of the physics of the resonant level model.

## III Results

One quantity that can be calculated analytically is the low–energy limit of the spin structure factor $`S(\omega )\stackrel{\mathrm{def}}{=}\chi _{zz}^{\prime \prime }(\omega )/\omega `$,

$$S(0)=\underset{\omega 0}{lim}\frac{\chi _{zz}^{\prime \prime }(\omega )}{\omega }.$$
(20)
For a vanishing local magnetic field $`S(0)`$ is just the spin relaxation rate accessible in e.g. spin resonance experiments. With the result for $`\chi _{zz}^{\prime \prime }(\omega )`$ from (19) we obtain

$$S(0)=(g\mu _B)^2\frac{1}{\pi }\frac{\mathrm{\Delta }_{\mathrm{eff}}^2(0)}{\left((g\mu _Bh)^2+\mathrm{\Delta }_{\mathrm{eff}}^2(0)\right)^2},$$
(21)
which leads to the curve shown in Fig. 2. Eq. (21) is of particular importance because it explicitly demonstrates universality, $`T_\mathrm{K}^2S(\omega )=f(g\mu _Bh/T_\mathrm{K})`$, and allows to directly fit e.g. experimental data from ESR or NMR experiments and extract the Kondo

temperature. Note furthermore that the result (21) is not only valid in the Kondo limit, but also holds at the Toulouse point of the anisotropic Kondo model and everywhere in between. Since it does not depend on the details of $`\mathrm{\Delta }_{\mathrm{eff}}(ϵ)`$ it will also be true for general band structures $`ϵ_\stackrel{}{k}`$ in (1) and thus is eventually the result for $`S(0)`$ in DMFT calculations.

The full frequency dependent $`\chi _{zz}^{\prime \prime }(\omega )`$ has to be calculated numerically using the form of the effective hybridization function in Fig. 1. The results for three values of the external field, $`h=0`$, $`g\mu _Bh=T_\mathrm{K}`$ and $`g\mu _Bh=5T_\mathrm{K}`$

are displayed in Fig. 3. These correlation functions provide a good example for the usefulness of our mapping to the effective RLM since one can directly interpret the structures and their frequency and field dependencies in terms of analytical formulas derived for the RLM. E.g. the high–frequency behavior of $`\chi _{zz}^{\prime \prime }(\omega )`$ follows directly from equ. (19) and the behavior of the effective hybridization function $`\mathrm{\Delta }_{\mathrm{eff}}(ϵ)`$ at large energies (which is linear with logarithmic corrections, see Fig. 1): $`\chi _{zz}^{\prime \prime }(\omega )`$ decays like $`1/\omega `$ with logarithmic corrections, in agreement with (expensive) numerical results Costi99 .

For the dependence of the dynamical susceptibility on the local magnetic field one makes use of the fact that the local magnetic field corresponds to the on–site energy in the effective RML. Therefore it is obvious that the observed shift of the resonance peak in $`\chi _{zz}^{\prime \prime }(\omega )`$ is due to the shifted center of the resonant level. Furthermore, the depletion of the maximum value is related to the decreasing occupation of the resonant level, which corresponds directly to the increasing local magnetization in the SIKM. At the same time, one observes a decrease of the total spectral weight in $`\chi _{zz}^{\prime \prime }(\omega )`$, which can be accounted for by a transfer to a finite expectation value of $`S_z`$ in the SIKM. There is, however, also a non–trivial effect, namely the increasing broadening of the resonance peak with increasing magnetic field. For a RLM with a constant $`\mathrm{\Delta }_{\mathrm{eff}}(ϵ)`$ such a behavior does not occur; it is entirely related to the fact that with increasing magnetic field the system starts to notice the energy dependence of the effective hybridization.

The quantity not yet fixed in our calculation is $`T_\mathrm{K}`$, or more precisely the proportionality constant in $`T_\mathrm{K}\mathrm{\Delta }_{\mathrm{eff}}(0)`$. This can most conveniently be done by using Wilson’s definition of the Kondo temperaturehewson

$$\chi _0(h=0)=(g\mu _B)^2\frac{w}{4T_\mathrm{K}},$$
(22)
where $`\chi _0`$ is the static magnetic susceptibility and $`w=0.413`$ the Wilson number. $`\chi _0`$ can be obtained from the imaginary part of the dynamic susceptibility (19) via

$$\chi _0=\frac{2}{\pi }\underset{0}{\overset{\mathrm{}}{}}𝑑\omega \frac{\chi _{zz}^{\prime \prime }(\omega )}{\omega }$$
(23)
and must in general be evaluated numerically. At the Toulouse point one can, however, give an analytic answer since $`\mathrm{\Delta }_{\mathrm{eff}}(\omega )=\mathrm{const}.`$ and thus

$$\chi _0(h)=(g\mu _B)^2\frac{1}{\pi }\frac{\mathrm{\Delta }_{\mathrm{eff}}(0)}{h^2+\mathrm{\Delta }_{\mathrm{eff}}(0)^2}.$$
(24)
Therefore at the Toulouse point the Korringa–Shiba relationKorringaShiba

$$R_\mathrm{S}=\frac{(g\mu _\mathrm{B})^2}{2\pi \chi _0^2}\underset{\omega 0}{lim}\frac{\chi _{zz}^{\prime \prime }(\omega )}{\omega }$$
(25)
is independent of the local magnetic field

$$R_\mathrm{S}=\frac{(g\mu _B)^2S(0)}{2\pi \chi _0^2(h)}=\frac{1}{2}.$$
(26)
In the following we will discuss $`\chi _0(h)`$ and the Korringa–Shiba relation for the Kondo limit $`\rho _0J0`$. The quantity $`\chi _0(h)`$ is particularly convenient for a comparison with NRG results.

In Fig. 4 the circles represent the values of $`\chi _0(h)`$ calculated via (23) with the effective hybridization function from Fig. 1, and the full line represents the result of an NRG calculation. We observe excellent agreement for all values of the local magnetic field: notice that the curves agree without fit parameters. This example clearly demonstrates that the nontrivial form of the effective hybridization in Fig. 1 encodes the many–particle physics of the SIKM in a trivial noninteracting effective model.

The result in Fig. 4 can readily be combined with relations (17) and (21) to obtain the Wilson ratioWilson

$$R_\mathrm{W}=\frac{4\pi ^2k_\mathrm{B}^2}{3(g\mu _\mathrm{B})^2}\frac{\chi _{\mathrm{imp}}(h)}{\gamma _{\mathrm{imp}}(h)}.$$
(27)
Our results for the Wilson ratio and the Korringa–Shiba relation obtained within the effective RLM are collected in Fig. 5. For the Wilson ratio we would actually have to calculate the quantity $`\chi _{\mathrm{imp}}`$ and not $`\chi _0`$.Wilson  However, for the case of small $`\rho _0J`$ considered here, both quantities are equivalent.chen  One observes that both $`R_\mathrm{W}`$ and $`R_\mathrm{S}`$ are independent of the local magnetic field up to approximately $`g\mu _BhT_\mathrm{K}`$, and then start to

decrease (Shiba ratio), respectively increase (Wilson ratio). The exact Bethe ansatz solution bethe  gives $`R_\mathrm{W}(h)=2`$ independent of the magnetic field strength (see also Ref. logan3, ), and local Fermi liquid theory yields $`R_\mathrm{S}=1`$ for $`h0`$.hewson  Our limiting values as $`h0`$ miss these exact results by approximately 5%. Notice that the term $`(1\mathrm{\Lambda }^{}(0))`$ in (17) is very important to obtain this correct value for $`R_\mathrm{W}(h=0)`$. Remarkably, our simple noninteracting effective model therefore correctly describes the Wilson ratio in the Kondo limit (for not too large magnetic fields), which is a hallmark of strong–coupling Kondo physics.

Let us finally analyze the accuracy of our effective model. Since Fig. 4 demonstrates that integral quantities like $`\chi _0(h)`$ are obtained with very good accuracy for all magnetic fields, one can infer from Fig. 5 that quantities depending on low–energy details in frequency space like $`\gamma _{\mathrm{imp}}`$ and $`S(0)`$ are more susceptible to our approximations for increasing magnetic fields. This suggests that for such low–energy quantities our effective model can be employed with very good accuracy (5% error) for magnetic fields below $`T_\mathrm{K}`$, and with good accuracy (20% error) still up to approximately $`5T_\mathrm{K}`$.

## IV Summary and outlook

Summing up, we have shown that the resonant level model with a nontrivial hybridization function $`\mathrm{\Delta }_{\mathrm{eff}}(ϵ)`$ can be used as an effective model for the single impurity Kondo model. The key observation was the fact that the flow equation solutions of both models are approximately identical if a suitable $`\mathrm{\Delta }_{\mathrm{eff}}(ϵ)`$ is chosen for the RLM (Fig. 1). In this mapping the impurity orbital occupation number $`n_d1/2`$ plays the role of the Kondo impurity spin $`S_z`$. The impurity orbital energy corresponds to the local magnetic field acting on $`S_z`$.

In contrast with the conventional approach where effective models describe the vicinity of the low–energy renormalization group fixed pointsWilson ; hewson , our effective model very accurately describes both certain low– and high–energy properties of the original Kondo model: compare for example our discussion of the dynamical spin–spin correlation function in Fig. 3. It also yields thermodynamic quantities that are in excellent agreement with much more expensive numerical methods (see Fig. 4). The nontrivial behavior of the effective hybridization function encodes the quasiparticle interaction, which leads to e.g. the correct Wilson ratio for small magnetic fields (with 5% accuracy). Notice, however, that our effective model does not allow the correct evaluation of higher–order correlation functions beyond the low–energy limit,

In conclusion, our approach describes many aspects of the complicated many–body Kondo physics for not too large magnetic fields within a simple noninteracting model. Therefore one can very easily and intuitively understand certain properties of the Kondo model, e.g. the dependence of correlation functions on a local magnetic field (Fig. 3). One main prospect of our approach is to look at other correlation functions using this effective model, in particular the $`T`$–matrix for applications in the framework of DMFT calculations. Future prospects also include cluster problems and the single impurity Anderson model. Work along these lines is in progress.

###### Acknowledgements.

We acknowledge valuable conversations with N. Andrei, R. Bulla, W. Hofstetter, D. Logan, A. Rosch, M. Vojta and D. Vollhardt. This work was supported by the DFG collaborative research center SFB 484 and NSF grant DMR-0073308.