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# Quantum Feedback Control of Atomic Motion in an Optical Cavity LA-UR-03-6826

## Abstract

We study quantum feedback cooling of atomic motion in an optical cavity. We design a feedback algorithm that can cool the atom to the ground state of the optical potential with high efficiency despite the nonlinear nature of this problem. An important ingredient is a simplified state-estimation algorithm, necessary for a real-time implementation of the feedback loop. We also describe the critical role of parity dynamics in the cooling process and present a simple theory that predicts the achievable steady-state atomic energies.

The control of quantum systems is a problem that lies at the heart of several fields, including atom optics and nanomechanics. Many of the techniques developed thus far for controlling quantum systems in an initially unknown state involve the use of dissipative processes to achieve a well-defined final state, as in the laser cooling methods in atom optics Metcalf99 . A different paradigm for cooling involves modifying the system Hamiltonian based on information provided by measurements (i.e., quantum feedback control). Such a strategy for control is generally applicable to quantum as well as classical systems Raizen98 ; Belavkin99 ; Doherty00 ; Armen02 ; Vitali03 ; Hopkins03 ; Geremia03 . As quantum-limited measurement techniques become more available, quantum feedback control is likely to soon be an essential element in atom-optical and nanomechanical toolkits.

One of the most promising avenues for the study of quantum feedback control centers on experiments in cavity quantum electrodynamics (CQED), where a single quantum system may be monitored continuously in real time, as has been demonstrated in a series of pioneering experiments Hood98 ; Mabuchi99 ; Hood00 ; Pinkse00 . Furthermore, the optical potential due to the cavity light provides an easily adjustable means for applying forces on the atom. Feedback has been shown to increase the storage time for atoms in such an experimental system Fischer02 . Despite these efforts, however, CQED feedback cooling has not yet been conclusively demonstrated, highlighting the need for a deeper theoretical understanding of this system as well as more sophisticated, higher performance cooling algorithms. Our goal here is to develop approximate estimation and control algorithms for cooling the atomic motion in such a CQED system—an “active cooling” approach that is distinct from passive cavity cooling methods Horak97 . We will then analyze the performance of these algorithms both analytically and through numerical simulations. This problem is particularly interesting due to the nonlinear form of the measurement operator, a situation distinct from previous studies of nonlinear quantum feedback control Doherty00 ; Wiseman02 . An important issue that we address here is whether the (Gaussian) estimation methods developed for linear systems are still effective in this problem.

The setup we are considering is an atom in a microcavity in the strong-coupling regime, as in the aforementioned CQED experiments Hood98 ; Mabuchi99 ; Hood00 ; Pinkse00 , but where the output light is monitored via homodyne detection Wiseman93 , which gives information about the atomic position in the cavity Quadt95 . We consider the case where the light is resonant with the cavity, but the detuning from atomic resonance is much larger than the natural atomic linewidth. We thus analyze the coupled atom-cavity system after adiabatic elimination of the cavity and internal atomic dynamics Doherty98 . The resulting stochastic master equation (SME) in Itô form Kloeden92  for the atomic motion conditioned on the homodyne measurement, describing the observer’s best estimate for the atomic state, is

$$\begin{array}{ccc}\hfill d\rho & =& i[H_{\mathrm{eff}},\rho ]dt\mathrm{\Gamma }[\mathrm{cos}^2(\stackrel{~}{k}X),[\mathrm{cos}^2(\stackrel{~}{k}X),\rho ]]dt\hfill \\ & & \sqrt{2\eta \mathrm{\Gamma }}\{[\mathrm{cos}^2(\stackrel{~}{k}X),\rho ]_+2\mathrm{cos}^2(\stackrel{~}{k}X)\rho \}dW.\hfill \end{array}$$
(1)
The effective atomic Hamiltonian is

$$H_{\mathrm{eff}}=\pi P^2V_{\mathrm{max}}\mathrm{cos}^2(\stackrel{~}{k}X),$$
(2)
and $`dW`$ is given in terms of the scaled photodetector current (measurement record) $`d\stackrel{~}{r}`$ by

$$dW=d\stackrel{~}{r}(t)/\sqrt{\eta }+\sqrt{8\eta \mathrm{\Gamma }}\mathrm{cos}^2(\stackrel{~}{k}X)dt.$$
(3)
The physical interpretation of Eqs. (1) and (3) is that the photocurrent is a direct measurement of $`\mathrm{cos}^2(\stackrel{~}{k}X)`$ within the adiabatic approximation. In these expressions, we are using scaled units such that position is measured in units of $`\sqrt{\mathrm{}/(m\omega _{\mathrm{HO}})}`$, momentum is measured in units of $`\sqrt{\mathrm{}m\omega _{\mathrm{HO}}}`$, and time is measured in units of $`2\pi /\omega _{\mathrm{HO}}`$, where $`\omega _{\mathrm{HO}}:=\alpha gk\sqrt{2\mathrm{}/|m\mathrm{\Delta }|}`$ is the oscillation frequency in the harmonic approximation for one of the optical potential wells, $`g`$ is the CQED coupling constant, $`m`$ is the atomic mass, $`\mathrm{\Delta }`$ is the detuning from the atomic resonance, $`\eta `$ is the photodetection efficiency, $`\alpha `$ is the mean cavity photon number in the absence of the atom, $`k`$ is the optical spatial frequency, $`\stackrel{~}{k}:=k\sqrt{\mathrm{}/(m\omega _{\mathrm{HO}})}`$, $`V_{\mathrm{max}}:=\pi /\stackrel{~}{k}^2`$, $`\mathrm{\Gamma }:=2\alpha ^2g^4/(\mathrm{\Delta }^2\kappa \omega _{\mathrm{HO}})`$ is the effective measurement strength, $`\kappa `$ is the energy decay rate of the cavity, and $`dr(t)=\sqrt{\kappa /\omega _{\mathrm{HO}}}d\stackrel{~}{r}(t)`$ is the physical photocurrent. The model thus has only three independent parameters, $`\stackrel{~}{k}`$, $`\mathrm{\Gamma }`$, and $`\eta `$, in addition to any parameters that specify how the optical potential is modulated. For the atomic parameters, we consider cesium driven on the D2 line, so that $`m=2.21\times 10^{25}\mathrm{kg}`$ and $`k=11732\mathrm{cm}^1`$. For the cavity parameters, we choose values similar to those used in recent CQED experiments Hood98 ; Mabuchi99 ; Hood00 , yielding $`\kappa /2\pi =40`$ MHz, $`g/2\pi =120`$ MHz, and $`\alpha =1`$. We also assume an optical detuning of $`\mathrm{\Delta }/2\pi =4\mathrm{GHz}`$ to the red of the atomic resonance. The corresponding scaled parameters are $`\mathrm{\Gamma }=23.6`$ and $`\stackrel{~}{k}=0.155`$. The scaled depth of the optical potential is $`V_{\mathrm{max}}=131`$, so that the lowest two band energies are within 1% of their values in the harmonic approximation. We also choose the idealized detection efficiency of $`\eta =1`$. However, cooling performance similar to that shown below is achievable even in the presence of detector inefficiency ($`\eta `$ well below $`0.5`$) as well as other real-world limitations such as hardware propagation and computation delays inprep .

While integration of the SME in order to obtain a state estimate is sensible in principle, in practice it is much too difficult to integrate the SME in real time. To solve this problem we must simplify the estimator. We make a Gaussian ansatz for the atomic Wigner function (which, equivalently, prescribes how the Weyl-ordered moments of the atomic state factorize). In doing so, we reduce the effort of integrating a partial differential equation to the much more manageable effort of integrating a set of five coupled ordinary differential equations for the two means $`X`$ and $`P`$ and the three variances $`V_x`$, $`V_p`$, and $`C_{xp}:=XP+PXXP`$ EPAPS . The tracking behavior of the Gaussian estimator is illustrated in Fig. 1, which compares the evolution of the position mean and variance for an atom evolving according to Eq. (1) with the same quantities from a Gaussian estimator evolution beginning with a different initial condition. The estimator rapidly locks on to the true solution. The ability of the estimator to track both quantities well is crucial to the success of the control algorithm that we present here.

Intuitively, an algorithm that responds to the wave-packet centroid, raising the optical potential while the atom is climbing one side of a well, should cool the atom. However, such a strategy eventually breaks down due to uncontrolled pumping of energy into the wave-packet variances. The key to obtaining an effective control algorithm is to consider the energy evolution due to the Hamiltonian part of the SME: $`_tH_{\mathrm{eff}}_{\mathrm{fb}}=(_tV_{\mathrm{max}})\mathrm{cos}^2(\stackrel{~}{k}X)`$. From this expression, it is clear that a “bang-bang” strategy is optimal for cooling if we consider only cyclic modulations of the potential amplitude within a limited range. The potential should be switched to the extreme low value when the quantity $`\mathrm{cos}^2(\stackrel{~}{k}X)`$ is maximized and to the extreme high value when this quantity is minimized. We denote these extreme values of the potential by $`(1\epsilon )^2V_{\mathrm{max}}`$ and $`(1+\epsilon )^2V_{\mathrm{max}}`$. Such a control strategy is sensitive to energy in both the centroids and variances of the atom. Of course, it is not possible to tell whether $`\mathrm{cos}^2(\stackrel{~}{k}X)`$ is at an extremum based only on information at the current time. Thus, to complete the feedback algorithm, we fit a quadratic curve to the history of this quantity at each time step and trigger on the slope of this curve at the current time.

An example of the cooling algorithm in action is shown in Fig. 2, which compares the energy evolution for an ensemble of atoms (where each atom is cooled separately in an independent simulation) undergoing cooling for $`\epsilon =0.1`$ with the energy evolution without any cooling (i.e., free evolution in the optical potential). Without cooling, the atoms simply heat up due to the measurement back-action (or equivalently, the stochastic cavity decay process), until they are eventually lost from the optical potential. The heating rate is set by the second term in the SME: $`_tH_{\mathrm{eff}}_{\mathrm{meas}}=8\pi \mathrm{\Gamma }\mathrm{cos}^2(\stackrel{~}{k}X)\mathrm{sin}^2(\stackrel{~}{k}X)`$. The cooling algorithm is able to counteract the measurement heating, and the atoms settle to a steady-state energy much lower than the initial energy. Also shown in Fig. 2 is the cooling performance of a much simpler algorithm, which arises by noting that the photocurrent is a direct measure of $`\mathrm{cos}^2(\stackrel{~}{k}X)`$ (plus noise), and that it should be possible to cool the atoms by triggering on the photocurrent signal itself (an approach similar in spirit to the “differentiating feedback” strategy in Ref. Fischer02 ). In this case, the same quadratic curve-fitting procedure is used to temper the measurement noise. Although cooling to a steady state still occurs in this case, the cooling performance is substantially worse than for the Gaussian estimator. This indicates that the Gaussian estimator acts as a nearly optimal filter (in the same sense as a Kalman filter Doherty99 ) for the relevant information in the photodetector signal. The results shown were generated assuming initial conditions and curve-fit details as follows, although the results do not sensitively depend on these values: The atoms begin in a coherent state ($`V_x=V_p=1/2`$), and each has an initial centroid energy corresponding to a displacement from the well center of 58% of the distance to the edge of the well, chosen so the atoms are clearly trapped but not particularly cold. The initial locations of the atoms are distributed uniformly between the bottom of the well and this maximum distance. The Gaussian estimator begins with the (impure-state) initial conditions $`X_\mathrm{e}=6`$, $`P_\mathrm{e}=0`$, $`V_X^\mathrm{e}=V_P^\mathrm{e}=1/\sqrt{2}`$, and $`C_\mathrm{e}=0`$. The estimator is evolved in steps of $`\mathrm{\Delta }t=0.0005`$, and at each step the quadratic curve is fitted to the values of $`\mathrm{cos}^2(\stackrel{~}{k}X)`$ computed from the 300 most recent estimator steps.

The cooling performance is further illustrated in Fig. 3, which shows the populations in the lowest four bands of the optical potential. Most of the steady-state population is in the lowest two bands, accounting for 94% of the population, and these two bands are almost equally populated. We now show that this behavior can be understood in terms of the parity of the atomic state. The atomic parity is invariant under Hamiltonian evolution in the atomic potential (and hence the influence of the control algorithm). However, the measurement term in the SME causes the atomic parity to diffuse according to

$$d𝒫=\sqrt{8\eta \mathrm{\Gamma }}\left[𝒫\mathrm{cos}(2\stackrel{~}{k}X)𝒫\mathrm{cos}(2\stackrel{~}{k}X)\right]dW,$$
(4)
where $`𝒫`$ is the parity operator. In fact, this is an unbiased, nonstationary diffusion process that causes $`𝒫`$ to “purify” at late times to the extreme values $`\pm 1`$ of pure parity, so that the homodyne measurement acts like a QND measurement of the atomic parity. Since the atomic initial condition described above corresponds to $`𝒫=0`$, the measurement process drives the atoms to states with either pure even or pure odd parity with equal probability. The obvious consequence of this effect for cooling is that only half of the atoms can be cooled to the ground band, while the remaining half can be cooled at best to the first excited band EPAPS . However, due to this purification effect (which means that the observer knows the final state of the atom on each individual run), cooling to the first excited band is essentially equivalent to cooling to the ground state, since the atom can be driven between these two bands with an additional coherent process (e.g., modulation via an additional classical optical potential).

Much of the residual energy (excitation out of the lowest two bands) is due to the inability of the Gaussian estimator to perfectly track the true atomic state. In this light, the cooling performance is quite impressive, especially considering the highly non-Gaussian nature of the first excited state, toward which half the atoms are cooling. To show this behavior explicitly, we can remove the estimator from the problem, and repeat the same ensemble of simulations where the cooling algorithm operates based on the value of $`\mathrm{cos}^2(\stackrel{~}{k}X)`$ computed with respect to the actual atomic wave function. These results are also shown in Fig. 3, and in this case the lowest two bands account for 98% of the atomic population.

The steady-state atomic energies can be well described by a simple analytic theory, which we now derive. We will assume that the atomic energy is near the ground-state energy $`E_0`$, so that we can make the harmonic approximation for the potential. We will further assume for the moment that all the energy $`\mathrm{\Delta }E`$ in excess of $`E_0`$ is associated with the wave-packet centroid (i.e., the wave packet is not squeezed). Then the quantity $`V_{\mathrm{max}}\mathrm{cos}^2(\stackrel{~}{k}X)`$ exhibits oscillations of peak-to-peak magnitude $`\mathrm{\Delta }E`$. Assuming that the switching occurs at the extremal times, the energy-evolution expression above leads to a coarse-grained cooling rate of $`_tH_{\mathrm{eff}}_{\mathrm{fb}}=8\epsilon (H_{\mathrm{eff}}E_0)`$. On the other hand, the heating rate discussed above can be rewritten as $`_tH_{\mathrm{eff}}_{\mathrm{meas}}=4\mathrm{\Gamma }\stackrel{~}{k}^4H_{\mathrm{eff}}`$. Steady state occurs when these two rates sum to zero:

$$H_{\mathrm{eff}}_{\mathrm{ss}}=\frac{E_0+E_1}{2(1\beta )}.$$
(5)
Here, $`\beta :=\mathrm{\Gamma }\stackrel{~}{k}^4/2\epsilon `$, and we have made the replacement $`E_0(E_0+E_1)/2`$ in view of the above parity considerations, where $`E_1`$ is the energy of the first excited band.

We can also derive a theory for the other extreme, where we assume all the excess energy is associated purely with squeezing of the wave packet and not with the centroid. In this case, the oscillations of $`V_{\mathrm{max}}\mathrm{cos}^2(\stackrel{~}{k}X)`$ are of peak-to-peak magnitude $`\sqrt{H_{\mathrm{eff}}^2E_0^2}`$. Then the $`(1\beta )^1`$ dependence in Eq. (5) is replaced by $`(1\beta ^2)^{1/2}`$. In the regime $`\beta 1`$ where this theory should be valid, this prediction is always below that of Eq. (5), and thus the centroid-only theory more faithfully represents the physical cooling limit.

Eq. (5) is compared with simulated late-time energies in Fig. 4. The simulated energies are in good agreement with the simple theory, although they are generally higher than the simple theoretical prediction. Again, much of this discrepancy is due to the imperfect tracking behavior of the Gaussian estimator, and the simulated energies from cooling based on perfect knowledge of the actual wave function are in better agreement. Qualitatively, we see a transition between ineffective and effective cooling with $`\epsilon `$; essentially, $`\epsilon `$ must be large enough that the cooling rate exceeds the heating rate, ensuring that the system is controllable. Beyond this transition, the system displays a remarkable insensitivity to the value of the switching amplitude; we observe similar robustness to the changes in the other parameters $`\mathrm{\Gamma }`$, $`\stackrel{~}{k}`$, and $`\eta `$.

The authors would like to thank Andrew Doherty and Sze Tan for helpful discussions. This research was performed in part using the resources of the Advanced Computing Laboratory, Institutional Computing Initiative, and LDRD program of Los Alamos National Laboratory.


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# Elementary excitations in the cyclic molecular nanomagnet Cr8

## Abstract

Combining recent Cr8\_INS  and new inelastic neutron scattering data for the molecular cyclic cluster Cr8 produces a deep understanding of the low lying excitations in bipartite antiferromagnetic Heisenberg rings. The existence of the $`L`$-band, the lowest rotational band, and the $`E`$-band, essentially spin wave excitations, is confirmed spectroscopically. The different significance of these excitations and their physical nature is clearly established by high-energy and $`Q`$-dependence data.

Recent advances in inorganic chemistry resulted in compounds with some tens of magnetic metal ions linked by organic ligands forming well defined magnetic nanoclusters. Being neither simple paramagnets nor bulk magnets, these molecular nanomagnets often exhibit fascinating quantum effects. For instance, quantum tunneling of the magnetization has been observed in the metal complexes Mn12 or Fe8 Mn12\_Fe8 .

Antiferromagnetic (AF) cyclic clusters represent another class of molecular nanomagnets. In these compounds the metal ions within a single molecule form almost perfect rings. The decanuclear wheel Fe10 has become the prototype KLT\_Fe10 , but wheels with different metal ions and varying (even) number of centers were realized wheels . The magnetization exhibits step-like field dependencies at low temperatures - a spectacular manifestation of quantum size effects in these nanomagnets DG\_ferricwheels .

Numerous experiments showed that these compounds are well described by the minimal spin Hamiltonian

$$H=J\underset{i=1}{\overset{N}{}}\text{S}_i\text{S}_{i+1}+D\underset{i=1}{\overset{N}{}}S_{i,z}^2+g\mu _B\text{S}\text{B}$$
(1)
with isotropic Heisenberg coupling and weak uniaxial magnetic anisotropy of the easy-axis type ($`N`$ is the number of spin centers, $`S_i`$ the spin length with $`\text{S}_{N+1}=\text{S}_1`$, and $`z`$ the uniaxial anisotropy axis) Cr8\_dipdip . The Heisenberg interaction is dominant ($`|D/J|<0.03`$); these objects are thus excellent experimental realizations of (bipartite) AF Heisenberg rings with weak magnetic anisotropy.

The observed steps in the magnetization curves provided a first phenomenological insight into the structure of the excitations of finite AF Heisenberg rings KLT\_Fe10 . The lowest states are those with minimal energy for each value of the total spin $`S=0,1,2,\mathrm{}`$. Their energies follow the Landé rule $`E(S)S(S+1)`$ as for a rigid rotator, and the notion of rotational modes was introduced JS\_rotationalbands . A subsequent numerical study OW\_spindynamics  showed that a complete description of the lowest lying excitations implies a set of $`N1`$ parallel rotational bands \[Fig. 1(b)\]. These bands were divided into $`L`$\- and $`E`$-band according to the selection rule that all transitions from the $`L`$-band to states neither belonging to the $`L`$\- nor to the $`E`$-band (the quasi continuum) have negligible transition matrix elements. The $`L`$\- and $`E`$-bands reflect the fact that the Hamiltonian can be approximated by an interaction between the two sublattice spin vectors. The $`L`$-band then corresponds to maximal sublattice spins, while the $`E`$-band appears with one sublattice spin decreased by one OW\_spindynamics ; AH\_fws . For the states of the $`L`$-band the shift quantum number $`q`$ defofq  toggles between $`q=0`$ and $`q=N/2`$ as function of $`S`$; the $`E`$-band embraces the lowest states with $`q0,N/2`$.

Recently, the cyclic cluster \[Cr8F8(L-d9)16\]$``$0.25C6H14 with L=O2CC(CH3)3, or Cr8, was investigated by inelastic neutron scattering (INS) Cr8\_INS . The eight Cr3+ ions form an octagon linked by F ions and pivalate ligands. The experimental data were successfully fitted to Eq. (1) with $`J=1.46`$ meV and $`D=0.038`$ meV Cr8\_dipdip . According to the black box character of this analysis, however, no insight concerning the elementary excitations was obtained. In this work, this INS data is reanalyzed unearthing in particular the first experimental evidence for the $`E`$-band. Adding new data clearly showing the different character of the $`L`$\- and $`E`$-excitations and their physical nature, this work arrives at a complete experimental confirmation of the theoretical picture of the excitations in bipartite AF Heisenberg rings.

So far, basically all molecular nanomagnets of interest (including Mn12 and Fe8 mentioned above) represent Heisenberg systems with weak anisotropy. It is thus of general importance to arrive at an understanding of the internal spin structure due to Heisenberg interactions. Remarkably, the $`L`$-band was also found in other finite AF Heisenberg systems with completely different topology, theoretically JS\_rotationalbands ; OW\_spindynamics  and experimentally JS\_Fe30 . Thus, the features which are confirmed here experimentally in detail for AF Heisenberg rings are expected to be generic for a much broader class of AF Heisenberg systems OW\_spindynamics .

Experiments were performed on 4 g of perdeuterated polycrystalline sample of Cr8, prepared as described in Cr8\_synthesis . High-energy-resolution INS experiments were done on the IN6 spectrometer of the Institute Laue-Langevin (Grenoble, France) with incident neutron energies of 2.35 meV and 4.86 meV for temperatures from 2 K to 23 K. Measurements with energy transfer up to 15 meV were performed on the MARI spectrometer of the Rutherford Appleton Laboratory ISIS (Oxfordshire, United Kingdom) at a temperature of 2.5 K. The details of the experiments and data correction were as in Cr8\_INS .

The measurements of the INS intensity as function of energy transfer are compiled in Fig. 1(a). The similarity of this figure with Fig. 3(c) in Ref. OW\_spindynamics  is striking peaks\_notation . In Fig. 1(a) the $`01`$ transition is split into two close peaks at 0.68 meV and 0.87 meV because of the magnetic anisotropy. The other transitions appear as single peaks because of their larger widths. The splitting of the $`S=1`$ spin multiplet (0.19 meV) is smaller than its center of gravity (0.81 meV), showing that Cr8 indeed represents an AF Heisenberg system with weak anisotropy. In the following, only averaged energies and integrated intensities will be discussed. The energy diagram for an octanuclear spin-3/2 Heisenberg ring is given in Fig. 1(b) with observed transitions indicated.

Apparently, the transitions $`01`$, $`12`$, and $`23`$ correspond to transitions within the $`L`$-band, the transitions $`01^{}`$, $`01^{\prime \prime }`$, and $`11^{}`$ to transitions from the $`L`$-band to the $`E`$-band OW\_spindynamics ; peaks\_notation . Thus, Fig. 1 establishes the first spectroscopic evidence for the $`L`$-band and the first experimental evidence for the $`E`$-band at all. The characteristic properties of the two types of bands will be explored in more detail in the following. The transition energies for the $`11^{}`$ and the $`L`$-band transition $`34`$ are very close in Cr8. The peak assigned as $`11^{}`$ in Fig. 1(a) thus actually consists of two distinct contributions, and will not be considered further.

The experimentally determined and theoretically expected energies and transition matrix elements are listed in Table 1. The errors of the matrix elements reflect the good agreement of observed and expected temperature dependence of peak intensities. With $`J`$=-1.46 meV Cr8\_INS  the agreement between experimental and exact energies of an octanuclear spin-3/2 Heisenberg ring \[Fig. 1(b)\] is excellent. Table 1 also demonstrates that the energies of the $`L`$-band states closely follow the Landé-rule. As a further characteristic of the $`L`$-band, the oscillator strengths (which are proportional to the $`|M|^2`$ of Table 1) for the $`SS+1`$ transitions increase as $`f_S=f_0(S+1)`$ OW\_spindynamics . In view of the experimental difficulties to determine $`|M|^2`$, this behavior is well observed in experiment.

The $`E`$-band essentially represents AF spin wave excitations OW\_spindynamics . In the classical limit, these are expected at energies $`ϵ(q)=2S_i|J\mathrm{sin}(q2\pi /N)|`$ PWA\_spinwaves ; GM\_sumrules . The four $`S=1^{}`$ spin levels belong to $`q=1,7`$ and $`q=3,5`$, the $`S=1^{\prime \prime }`$ spin levels to $`q=2,6`$ \[Fig. 1(b)\]. The spin wave nature of these states is indicated by the agreement of the observed energies with $`ϵ(q=1,3,5,7)=3.10`$ meV and $`ϵ(q=2,6)=4.38`$ meV, especially as these values should be larger for $`S_i=3/2`$ by several ten percent due to quantum effects GM\_sumrules ; SI\_INS32 . The observed $`E`$-band transition intensities further confirm this picture: $`|M|^2`$ is (i) significantly smaller than for the $`L`$-transitions and (ii) larger for $`01^{}`$ than for $`01^{\prime \prime }`$ reflecting the expected $`\sqrt{1\mathrm{cos}(q2\pi /N)}/\sqrt{1+\mathrm{cos}(q2\pi /N)}`$ dependence GM\_sumrules .

A critical test of the internal structure of the wave functions is provided by the selection rule distinguishing $`L`$\- and $`E`$-bands: The oscillator strengths for transitions from the $`L`$-band to states of the quasi continuum are virtually zero GM\_sumrules ; OW\_spindynamics . As they cannot be calibrated precisely, the experimental oscillator strengths do not allow to show this directly from sum rules OW\_spindynamics . But Fig. 2, presenting an INS measurement for energies up to 13 meV, demonstrates that at small temperatures no further transitions than the $`01`$, $`01^{}`$, and $`01^{\prime \prime }`$ transitions could be detected. If it were not for the selection rule, several transitions starting at 6.5 meV were to be expected, see Fig. 1(b). This provides the most compelling evidence that the wave functions of the states of the rotational bands are (semi)classical in nature OW\_spindynamics .

The different nature of the $`L`$\- and $`E`$-excitations, in turn, becomes most apparent from the $`Q`$-dependence of the INS intensity. Experimental results are shown in Fig. 3 for the $`L`$-transitions $`01`$, $`12`$, $`23`$, and the $`E`$-transition $`01^{}`$, respectively. For the $`L`$-transitions, the $`Q`$-dependencies are very similar to each other and exhibit a pronounced oscillatory behavior, in clear contrast to the almost flat $`Q`$-dependence of the $`E`$-transition.

Due to the high spatial symmetry of cyclic clusters, the $`Q`$-dependence of the INS intensity can be calculated analytically OW\_INS . Classifying eigen states as $`|\tau q`$, $`\tau `$ denoting further quantum numbers, the $`Q`$-dependence is, up to a constant factor, completely specified by the transfer in shift quantum number $`\mathrm{\Delta }q=qq^{}`$ (and the radius of the ring, 4.427 Å). For all transitions within the $`L`$-band holds $`\mathrm{\Delta }q=N/2`$. For transitions from the $`L`$\- to the $`E`$-band one has to take into account the degeneracy of spin levels with $`q`$ and $`Nq`$ as enforced by symmetry, and quasi degeneracies due to the $`|\mathrm{sin}(q2\pi /N)|`$-like dependence of energy on $`q`$ which cannot be resolved experimentally. Accordingly, the transition $`01^{}`$ is the sum of four transitions with $`\mathrm{\Delta }q=1,3,5,7`$. The theoretical curves are also presented in Fig. 3. The agreement with experiment is convincing. This analysis provides a direct determination of the different spatial symmetry properties of the $`L`$\- and $`E`$-bands, and demonstrates a Néel-structure of the $`L`$-band wave functions.

Fig. 3(a) indicates that the intensity of the $`01`$ transition does not drop to zero for $`Q0`$, in contrast to the theoretical curve. This is also evident with better resolution from the 2 K data shown in Fig. 4. The inset explicitly shows the presence of INS intensity at low $`Q`$. For cyclic clusters, because of their symmetry, the INS intensity drops to zero quadratically in $`Q`$ for $`qq^{}`$, i.e. follows $`\delta _{q,q^{}}+𝒪(Q^2)`$ for $`Q0`$ OW\_INS . Accordingly, the observed nonzero intensity for $`Q0`$ suggests that the spin Hamiltonian for Cr8 has to be extended by small terms with lower symmetry. Such terms are currently under strong debate MA\_levelcrossings ; OW\_butterflies  as they would represent sources of decoherence for a mesoscopic tunneling of the Néel-vector, which was predicted for cyclic clusters AC\_NVT . INS at low momentum transfer can be a powerful tool to detect and analyze these terms.

The $`E`$-band was identified as spin waves. In contrast, the above experiments unambiguously demonstrated the Néel-like structure of the $`L`$-band: it exactly represents the degrees of freedom due to a combined rotation of the oppositely oriented total spins on each sublattice as they appear in the spin wave theory of antiferromagnets PWA\_spinwaves  (a nice description is given in PWA\_Lband ). Accordingly, in the limit of infinite $`N`$ the $`L`$-band would evolve into the essentially classical Néel-ground state, if it were not for the strong quantum fluctuations in one-dimensional chains.

Thus, finite AF Heisenberg rings, approximated experimentally by molecular cyclic clusters, are rather classical and in this sense closer to higher dimensional than to one-dimensional AF systems. The internal spin structure of cyclic clusters, as confirmed here by experiment, is well described by the usual spin wave theory for antiferromagnets. The important new feature in these systems, however, is that the lowest excitations as relevant for low temperature experiments are not the spin wave excitations as in extended antiferromagnets, but the quantized rotation of the Néel-type ground state configuration.

By extension, this suggests that for Heisenberg systems, where the correct ground state is obtained by a classical assignment of up and down spins to each center as it is the basis for the Néel-state, a (semi)classical approach is adequate. This includes a large number of molecular systems, e.g. the cyclic metal clusters, the iron icosidodecahedron {Mo72Fe30} JS\_Fe30 , molecular grids OW\_Mn3x3 , but also single molecule magnets like Mn12 and Fe8. We conclude: In the majority of cases the internal spin structure of molecular nanomagnets, being truly quantum mechanical objects, is essentially classical.

###### Acknowledgements.

We thank R. Caciuffo, G. Amoretti, and V. Dobrovitski for enlightening discussions, and C. D. Frost for help with INS experiments. We thank the Deutsche Forschungsgemeinschaft, the Department of Energy (Grant No. DE-FG02-86ER45271), and the FIRB program of the Italian Ministry of University and Research.


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# Orientation effects in bipolar nebulae: Can disks do it?

## 1. Observations

We collected a sample of bipolar planetary nebula and symbiotic nebula from the literature that contained sufficient data to produce a reasonabble spectral energy distribution (SED). After constructing the SEDs we compared the luminosity emitted in each band relative to the total luminosity as a function of inclination angle. The inclination angles were determined by the three authors independently, being in agreement within 10-15o for nearly all objects, with an exceptional 30o difference in a couple of cases. In Figure 1 we show the plot with the relative luminosities for each band as a function of the inclination. One can clearly see the increase in the relative FIR flux as well as the decrease of JHK and BVR with inceasing inclination.

## 2. Model

In an attempt to explain this observed behavior, we propose that the systems are composed of a dusty disk being irradiated by a star or binary. This radiation heats up the dust that is responsible for the radiation emitted in the FIR. The combined effect of this re-radiation with the extinction produced by the disk is what would create the observed effect.

We use a simple 2-D radiative transfer model that calculates the temperature of the grains of a disk defined within a square grid. By requiring conservation of luminosity and iterating we determine the temperature of the dust in each cell. Secondary radiation is not yet accounted for.

For the dust characteristics we adopt typical interstellar grains with Rv = 3.1 with properties as calculated by Li & Draine (2001) and a gas to dust ratio of 125. For the disk we obtained temperature maps from which we calculated a random sample of star-disk systems with sin(i) distributed random inclination angles. This simple method assumes a general temperature, taken here as the average temperature obtained from the 2-D code. We also obtain attenuation functions from the 2-D code that will be used to calculate the extinction of the starlight when intercepted by the disk. Also from the code we obtain the amount of starlight absorbed by the disk. For this component, we assume that the energy is re-radiated in the FIR as a blackbody with the average temperature mentioned before. Figure 1 shows one example of such a model run.

## 3. Conclusions

The results show that a disk with sufficient density and size is able to produce the general, observed behavior. It is interesting to note that the simple model did not do well when we considered a double system with a luminous cold star as well as the hot ionizing one. On the other hand, the more precise 2-D code copes well with that binary and in fact needs it to reproduce the observed results. These results are only preliminary and much more detail should be accounted for to be able to pin-point the actual disk structure needed. Even so, we can safely say that, yes, disks can do it!

## References

Li, A. & Draine, B.T. 2001 ApJ554, 778