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# Magnetization steps in a diluted Heisenberg antiferromagnetic chain: Theory and experiments on TMMC:Cd

## I INTRODUCTION

Spin clusters with predominantly antiferromagnetic (AF) interactions exhibit steps in the equilibrium magnetization as a function of magnetic field. These magnetization steps (MST’s) arise from energy-level crossings which change the ground state. They are observed at very low temperatures when only the ground state contributes to the magnetization $`M`$. In recent years MST’s have yielded a wealth of information about AF clusters, first in diluted magnetic materials and later in molecular magnetism. An overall review of MST’s was published recently.Shapira and Bindilatti (2002) For recent reviews of the magnetic properties of molecular clusters, including MST’s, see Ref. Gatteschi, 2000.

In a molecular crystal the AF clusters are normally all of one type. The MST’s then give values of exchange constants and anisotropy parameters for that cluster type. A diluted magnetic material, on the other hand, contains numerous types of spin clusters. Different cluster types give rise to different series of MST’s. In addition to exchange constants and anisotropy parameters, the MST’s also give information concerning the populations of the different cluster types. The populations are related to the magnitudes of the MST’s in the different series. The results for the cluster populations can be used to check if the distribution of the magnetic ions is random.

Most previous studies of MST’s in diluted magnetic crystals were on three-dimensional (3D) materials,Shapira and Bindilatti (2002) although some quantum wells were also studied.Crooker et al. (1999) The present paper, however, is devoted to MST’s from a diluted AF Heisenberg chain (1D). The material studied is TMMC \[chemical formula: $`(\mathrm{CH}_3)_4\mathrm{NMnCl}_3`$\] which was diluted by replacing a large fraction of the Mn atoms by Cd. Powder samples of $`(\mathrm{CH}_3)_4\mathrm{NMn}_\mathrm{x}\mathrm{Cd}_{1\mathrm{x}}\mathrm{Cl}_3`$, with $`\mathrm{x}`$ between $`0.16`$ and $`0.5`$, were investigated. In these materials the non-magnetic $`\mathrm{Cd}^{2+}`$ ions break the chains of $`\mathrm{Mn}^{2+}`$ ions into finite segments.

Pure TMMC is probably the closest approximation to an ideal isotropic (Heisenberg) linear AF chain. For reviews of its magnetic properties, with extensive references to original works, see Refs. de Jongh and Miedema, 1974; Steiner et al., 1976; Carlin, 1986; Kahn, 1993. The 1D magnetic behavior of this compound is due to the crystallographic structure. It contains chains of Mn ions which at room temperature are along the $`c`$-axis of the hexagonal structure. The Mn ions in each chain are linked by Cl ions. The space between the combined $`\mathrm{Mn}\mathrm{Cl}_3\mathrm{Mn}`$ chains is occupied by tetramethylammonium groups.

The strongest magnetic interaction in TMMC is the isotropic exchange between nearest neighbor (NN) $`\mathrm{Mn}^{2+}`$ ions in the chain. The NN exchange constant, obtained from various experiments (e.g., Ref. Hutchings et al., 1972), is $`J/k_\mathrm{B}6.6\mathrm{K}`$, where $`k_\mathrm{B}`$ is the Boltzmann constant. Other intrachain exchange constants are believed to be much smaller, and are usually neglected. The exchange interaction between different chains is orders of magnitude smaller than the intrachain interaction, but is responsible for the long-range AF order below the Néel temperature $`T_N=0.84\mathrm{K}`$. The anisotropy in TMMC is mainly due to the dipole-dipole interaction. It is of the easy-plane type, and is two orders of magnitude smaller than the dominant exchange interaction.Walker et al. (1972)

At room temperature both TMMC and its Cd analog \[$`(\mathrm{CH}_3)_4\mathrm{NCdCl}_3`$, known as TMCC\] have isomorphous hexagonal structures (space group $`P6_{3/m}`$). Crystallographic phase transitions at lower temperatures result in a lower symmetry, and in small structural differences between TMMC and TMCC.Hutchings et al. (1972); Peercy et al. (1973); Braud et al. (1990); Peral et al. (2000) These differences are often assumed to be unimportant, although it is conceivable that even small changes in the crystal structure have some effect on the magnetic behavior, especially on spin relaxation at low temperatures.

Previous investigations of $`(\mathrm{CH}_3)_4\mathrm{NMn}_\mathrm{x}\mathrm{Cd}_{1\mathrm{x}}\mathrm{Cl}_3`$ included measurements of the susceptibility and the Néel temperature as a function of $`\mathrm{x}`$ (Ref. Dupas and Renard, 1978). These results were interpreted theoretically both by the original authors, Dupas and Renard, and by Harada et al.Harada et al. (1980) Susceptibility measurements on a related diluted linear AF chain (DMMC:Cd) were obtained and interpreted by Schouten et al.Schouten et al. (1982) The authors of both Refs. Dupas and Renard, 1978 and Schouten et al., 1982 noted the difficulties of preparing alloys with uniform Cd concentrations.

## II EQUILIBRIUM THEORY

In this section a theory for the low temperature magnetization $`M`$ of a diluted AF Heisenberg chain is presented. It is assumed that the spin system is in thermal equilibrium with a constant-temperature heat reservoir. This equilibrium theory is suitable for interpreting the data that were obtained in the slowly-varying magnetic fields (“dc fields”) of the superconducting magnets. The additional considerations needed to interpret the results obtained in pulsed fields, of several ms duration, will be discussed in Sec. III

### II.1 The Model

MST’s from finite AF chains were predicted decades ago,Bonner and Fisher (1964); Parkinson and Bonner (1985) but some more recent theoretical results are also useful. The simplest model for MST’s in a diluted magnetic material is the single–$`J`$ cluster model.Shapira and Bindilatti (2002) It includes only the largest isotropic exchange constant $`J`$ and the Zeeman energy. Other exchange constants, and all anisotropies, are ignored. This model, with the NN intrachain exchange constant chosen as $`J`$, is expected to be a good starting point for $`(\mathrm{CH}_3)_4\mathrm{NMn}_\mathrm{x}\mathrm{Cd}_{1\mathrm{x}}\mathrm{Cl}_3`$ (hereafter, TMMC:Cd). All cluster models are applicable only when $`\mathrm{x}`$ is not too high. However, for a diluted magnetic chain (1D) the single–$`J`$ model it is expected to hold at least up to $`\mathrm{x}=0.5`$. All the samples in the present study are in this range.

In the single–$`J`$ model the magnetic clusters are finite chains, each consisting of $`n`$ coupled spins. These clusters are treated as independent. The total magnetization $`M`$ is then the sum of the magnetizations of finite chains with different $`n`$. Let $`\mu _n`$ be the average magnetic moment of a chain with $`n`$ spins, and let $`N_n`$ be the number of “realizations,” per kg, of a chain with $`n`$ spins. ($`N_n`$ may also be called the “population,” per kg, of finite chains with $`n`$ spins). The magnetization per kg is then

$$M=N_n\mu _n.$$
(1)
If $`P_n`$ is the probability that a spin is in a chain with $`n`$ spins, and if $`N_{\mathrm{total}}`$ is the total number of spins per kg, then

$$N_n=N_{\mathrm{total}}P_n/n.$$
(2)
The probabilities $`P_n`$ are obtained from well known results,not (a)

$$P_n=n\mathrm{x}^{n1}(1\mathrm{x})^2.$$
(3)
This result assumes a random distribution of the magnetic ions. This crucial assumption is discussed later. Figure 1 shows the probabilities $`P_n`$ for $`n5`$, and the probability $`P_{>5}`$ that a spin is in a finite chain $`n>5`$, i.e.,

$$P_{>5}=1\underset{1}{\overset{5}{}}P_n=(65\mathrm{x})\mathrm{x}^5.$$
(4)
From Eqs. (13), the magnetization $`M`$ is given by the infinite sum

$$M=N_{\mathrm{total}}\underset{n}{}\mathrm{x}^{n1}(1\mathrm{x})^2\mu _n.$$
(5)
In practice, exact results for the average magnetic moment $`\mu _n`$ are available only for values of $`n`$ which are not too large (short chains). The infinite sum in Eq. (5) is therefore truncated at some maximum value of $`n`$, called $`n_{\mathrm{max}}`$. Chains with $`n>n_{\mathrm{max}}`$ are treated using an approximation.Shapira and Bindilatti (2002) In the present work we chose $`n_{\mathrm{max}}=5`$ because exact results for chains with up to five $`\mathrm{Mn}^{2+}`$ ions ($`S=5/2`$) were readily available from previous works.Shapira and Bindilatti (2002); Gratens et al. (2001)

When $`\mathrm{x}`$ is below $`0.50`$, less than $`11\%`$ of the spins are in chains with $`n>5`$. For this range of $`\mathrm{x}`$, the “rise and ramp” approximationShapira and Bindilatti (2002) can be used for the total contribution from chains with $`n>5`$ \[i.e., it approximates the remainder after the sum in Eq. (5) is truncated\]. The approximation smoothes the $`B`$-dependence of this remainder, i.e., MST’s from chains with $`n>5`$ are not resolved. This approach (exact treatment for $`n5`$, and an approximation for $`n>5`$) proved to be adequate for interpreting the data obtained in dc magnetic fields. However, the interpretations of some data obtained in pulsed magnetic fields also used available theoretical resultsLou et al. (2002) for $`n>5`$.

To implement the rise and ramp approximation, the so-called “short chain model” (Ref. Schouten et al., 1982) was adopted. This model is appropriate for $`\mathrm{x}<0.5`$ because more than $`99.4\%`$ of the spins are in chains with $`n10`$, and more than $`99.9\%`$ are in chains with $`n14`$. A chain with 14 spins is still short enough to be described by that model. In the short-chain model the ground state at $`B=0`$ has total spin $`S_T(0)=0`$ when $`n`$ is even, and $`S_T(0)=S`$ if $`n`$ is odd. This simple result does not hold for 3D materials, which is one of the reasons why the rise and ramp approximation is simpler and much more accurate for diluted chains than for diluted 3D materials.

### II.2  Qualitative shape of the magnetization curve at low temperatures

#### II.2.1 Clusters of one type

Consider first an ensemble of identical finite chains, all with the same $`n`$. (In the language of Ref. Shapira and Bindilatti, 2002, this is an ensemble of “realizations” of a chain “type” with $`n`$ spins.) At low temperatures, $`k_BT|J|`$, the qualitative variation of $`\mu _n`$ with $`B`$ depends on whether $`n`$ is even or odd. When $`n`$ is odd the zero-field-ground-state total spin $`S_T(0)=S`$ aligns rapidly at low $`B`$. This alignment is given by the Brillouin function (BF) for spin $`S`$. The rapid rise of $`\mu _n`$ at low $`B`$ ends when the BF approaches saturation. After the BF saturates, there is a magnetic-field interval in which $`\mu _n`$ is nearly constant. At still higher $`B`$ a series of MST’s appears. The fields at these MST’s depend on $`n`$. Once this series of MST’s is completed, $`\mu _n`$ reaches its true saturation value $`\mu _{n,\mathrm{max}}=ng\mu _\mathrm{B}S`$.

When $`n`$ is even, $`S_T(0)=0`$. Therefore, no initial fast rise of $`\mu _n`$ occurs at low $`B`$, in contrast to the case of odd $`n`$. However, at high magnetic fields a series of MST’s still appears. At the completion of this series, $`\mu _n`$ reaches its true saturation value.

#### II.2.2 Total magnetization $`M`$

Chains with all values of $`n`$ contribute to the total magnetization $`M`$. When $`k_BT|J|`$, the chains with odd values of $`n`$ produce a fast rise of $`M`$ at low $`B`$. This rise follows the BF for spin $`S`$. After this fast rise is completed, and before the appearance of the first MST of significant size, there exists a field interval in which $`M`$ stays approximately constant. This (nearly) constant value, $`M_s`$, is the “apparent saturation value” (see Ref. Shapira and Bindilatti, 2002). At still higher fields, MST’s series from chains with $`n2`$ appear. Once the last MST of significant size is completed, $`M`$ reaches its true saturation value $`M_0`$. As discussed later, the magnetic field required to saturate the magnetization of a chain remains finite even when $`n\mathrm{}`$, so that $`M`$ reaches true saturation at a finite $`B`$.

### II.3 Apparent saturation value

The true saturation value of the magnetization is

$$M_0=N_{\mathrm{total}}g\mu _\mathrm{B}S.$$
(6)
The apparent saturation value is

$$M_s=\underset{n=\mathrm{odd}}{}N_{\mathrm{total}}\mathrm{x}^{n1}(1\mathrm{x})^2g\mu _\mathrm{B}S,$$
(7)
where the sum is only over odd $`n`$. Therefore,

$$M_s/M_0=\underset{n=\mathrm{odd}}{}\mathrm{x}^{n1}(1\mathrm{x})^2.$$
(8)
This infinite geometric series can be summed,not (b)

$$M_s/M_0=(1\mathrm{x})/(1+\mathrm{x}).$$
(9)
It is noteworthy that an exact analytical expression for $`M_s`$ was not obtained for 3D materials.Shapira and Bindilatti (2002) A rough approximation was then used for the net contribution from clusters with $`n>n_{\mathrm{max}}`$. This approximation was used only for $`\mathrm{x}0.1`$. In contrast, Eq. (9) for a diluted chain is exact, within the framework of the short-chain model. It should be very accurate for $`\mathrm{x}0.5`$.

### II.4 MST’s from Chains with $`n5`$

All chains with $`n2`$ give rise to MST’s. The magnetic fields $`B_i`$ at the MST’s from chains composed of spins $`S=5/2`$ were given earlier for $`n=2`$ (pairs, or dimers), $`n=3`$ (triplets, or trimers), $`n=4`$ (quartets, or tetramers), and $`n=5`$ (quintets, or pentamers).Gratens et al. (2001) For completeness, the values of the reduced fields $`b_i=g\mu _\mathrm{B}B_i/|J|`$ are repeated here.

For $`n=2`$ there are five MST’s at $`b_i=2,4,6,8,10`$. For $`n=3`$ there are five MST’s are at $`b_i=7,`$ $`9`$, $`11`$, $`13`$, $`15`$. For $`n=4`$ there are ten MST’s at $`b_i=0.95`$, $`2.04`$, $`3.39`$, $`5.02`$, $`6.87`$, $`8.85`$, $`10.88`$, $`12.94`$, $`15.00`$, $`17.07`$. For $`n=5`$ there are ten MST’s at $`b_i=4.62`$, $`5.89`$, $`7.18`$, $`8.49`$, $`9.86`$, $`11.29`$, $`12.83`$, $`14.48`$, $`16.24`$, $`18.09`$.

Figure 2 shows the zero-temperature values of $`\mu _n`$ as a function of $`b`$ for $`n=1,2,3,4,5`$. At finite $`T`$ the ground state of a chain is not the only contributor to $`\mu _n`$. It is then necessary to include all energy levels in the calculations of $`\mu _n`$. The procedures for such calculations were discussed in Ref. Shapira and Bindilatti, 2002.

### II.5  Rise and ramp approximation for chains with $`n>5`$

The total contribution of chains with $`n>5`$ to $`M`$ is approximated by a sum of two terms: 1) a fast rise at low $`B`$, which follows the BF for spin $`S`$, and 2) a linear “ramp” from $`B=0`$ up to an effective saturation field $`B_s`$.

The fast rise at low $`B`$ is due to chains with odd $`n`$, starting with $`n=7`$. Its magnitude is

$$(\mathrm{\Delta }M)_{\mathrm{rise}}=M_0\mathrm{x}^6(1\mathrm{x})/(1+\mathrm{x}).$$
(10)
The linear ramp approximates the superposition of numerous MST’s from all chains with $`n>5`$. The ramp is given by

$$M_{\mathrm{ramp}}=\{\begin{array}{c}(\mathrm{\Delta }M)_{\mathrm{ramp}}(B/B_s),\text{ for }BB_s\hfill \\ (\mathrm{\Delta }M)_{\mathrm{ramp}},\text{ for }B>B_s,\hfill \end{array}$$
(11)
where

$`(\mathrm{\Delta }M)_{\mathrm{ramp}}`$ $`=`$ $`P_{>5}M_0(\mathrm{\Delta }M)_{\mathrm{rise}}`$ (12)
$`=`$ $`M_0\mathrm{x}^5(64\mathrm{x}^2)/(1+\mathrm{x}).`$
The reduced field $`b_s(n)`$ where the magnetization of a finite chain with $`n`$ spins reaches saturation at $`T=0`$ increases with $`n`$. However, in the limit $`n\mathrm{}`$ it is still finite,Parkinson and Bonner (1985); Gratens et al. (2001) namely, $`b_s(n=\mathrm{})=8S`$. It can be shown that the $`n`$-dependence of $`b_s(n)`$ is given by the equation

$$b_s(n)=8S\mathrm{cos}^2(\pi /2n).$$
(13)
For chains with $`n>5`$ the change of this function is only $`7\%`$. In the present case of $`S=5/2`$, $`b_s(n)`$ changes from $`18.7`$ to $`20.0`$ when $`n`$ increases from $`6`$ to $`\mathrm{}`$. The value $`b_s=19`$, corresponding to

$$g\mu _\mathrm{B}B_s=19|J|,$$
(14)
will be used in Eqs. (11) for the ramp.

Figure 3(a) shows the predicted zero-temperature magnetization curve for $`S=5/2`$ when $`\mathrm{x}=0.50`$. Figure 3(b) is an expanded view for the range of magnetic fields relevant to the present experiments. The integers in this figure are the values of $`n`$ for the finite chains responsible for each MST.

### II.6 Random Distribution

Some of the preceding results used the probabilities $`P_n`$ for a random distribution of the magnetic ions. Although a random distribution is often found in diluted magnetic materials, non-random distributions were also observed.Shapira and Bindilatti (2002) In the case of TMMC:Cd, difficulties of obtaining a uniform Mn distribution were reported in the literature.Dupas and Renard (1978); Schouten et al. (1982) Therefore, the possibility of a non-random distribution cannot be ignored. The effects on the magnetization curve caused by departures from a random distribution were discussed in Ref. Shapira and Bindilatti, 2002. For example, a tendency of the magnetic ions to cluster together is expected to decrease $`M_s`$.

## III NON-EQUILIBRIUM EFFECTS

### III.1 Non-Equilibrium Effects

Experiments are normally conducted with the sample in contact with, or near, a thermal reservoir of constant temperature, e.g., a liquid helium bath at a temperature $`T_{\mathrm{bath}}`$. In some experiments the sample is not in thermal equilibrium either within itself and/or with the thermal reservoir. That is, the time for reaching complete equilibrium (both internal and with the reservoir) is not short compared to the time of the experiment. Such non-equilibrium cases require special considerations.

Thermal equilibrium is usually maintained if 1) the magnetic field $`B`$ is swept slowly (“dc fields”), and 2) the sample is in good thermal contact with the reservoir. These conditions are often fulfilled in superconducting magnets when the sample is immersed in liquid helium. There are, however, exceptional cases of non-equilibrium behavior even for slowly varying $`B`$ and good thermal contact. These have been discussed extensively in connection with macroscopic quantum tunnelling. A well known example is $`\mathrm{Mn}_{12}`$-acetate.Gatteschi (2000); Friedman et al. (1996); Thomas et al. (1996); Chudnovsky and Tejada (1998); Barbara and Gunther (1999)

Departures from thermal equilibrium with the reservoir due to imperfect thermal contact were observed and discussed for a wide range of sweep rates, $`dB/dt`$, from typical sweep rates in “dc magnets” to the very fast rates in pulsed magnets.Shapira et al. (1989); Bindilatti et al. (1991); Foner (1994); Shapira et al. (1999); Chiorescu et al. (2000); Nakano and Miyashita (2001); Shapira et al. (2001); Waldmann et al. (2002); Inagaki et al. (2003) The extreme case of a sample isolated from the thermal reservoir (adiabatic conditions) was discussed by Wolf long ago, assuming thermal equilibrium within the sample.Wolf (1959) The magnetocaloric effect leads to cooling when any one of the MST’s is approached. Such “cooling by adiabatic magnetization” has been observed many times in both dc fields and pulsed fields.Shapira et al. (1989, 1999, 2001); Waldmann et al. (2002); not (c)

### III.2  Some non-equilibrium models for pulsed magnetic fields

#### III.2.1  Classification of non-equilibrium behaviors

Non-equilibrium behavior in pulsed fields of milliseconds duration is relevant to the interpretation of the present pulsed field data. For this purpose it will be useful to distinguish between three types of non-equilibrium situations:

1. The spin-lattice relaxation is fast enough so that thermal equilibrium within the sample is established in a time which is very short compared to the pulse duration. The non-equilibrium behavior is then due to an inadequate heat flow between the liquid-helium bath and the sample, i.e., the sample-bath equilibration time is not short compared to the pulse duration. The “Inadequate Heat Flow” models are appropriate for this situation.
2. The time for establishing thermal equilibrium within the sample is not short compared to the pulse duration, but there is adequate sample-to-bath heat flow. The non-equilibrium is then governed by the slow spin-lattice relaxation processes. There are many such processes. Here, only spin-flips associated with level crossings or with cross-relaxation (CR) will be discussed.Ajiro et al. (1998); Wernsdorfer et al. (2002)
3. Both the time for reaching equilibrium within the sample, and the time for reaching a sample-to-bath equilibrium are not short compared to the pulse duration. Some such cases were considered in the literature.Chiorescu et al. (2000); Nakano and Miyashita (2001); Waldmann et al. (2002); Giraud et al. (2001)

#### III.2.2 Inadequate Heat Flow (IHF) Models

The phonon bottleneck (PB) phenomenon has been known for a long time.van Vleck (1941); Abragam and Bleaney (1970) Treatments of this phenomenon in the context of the magnetization process of magnetic clusters led to the development of several IHF models.Bindilatti et al. (1991); Shapira et al. (1999); Chiorescu et al. (2000); Nakano and Miyashita (2001); Waldmann et al. (2002); Inagaki et al. (2003) The common feature of these models is that the spin and phonon subsystems, within the sample, are very nearly in thermal equilibrium. The spin temperature $`T_s`$, the phonon temperature, and the sample temperature are the same. However, the sample and the helium bath are not in thermal equilibrium ($`T_sT_{\mathrm{bath}}`$). Different IHF models treat the sample-to-bath heat flow differently. For a solid sample in contact with a liquid-helium bath the heat flow was assumed to be limited by the Kapitza resistance.Bindilatti et al. (1991); Shapira et al. (1999); Inagaki et al. (2003) Many of the qualitative features of the magnetization curve are common to all IHF models; they do not depend on the detailed treatment of the heat flow.

Because the sample is internally in equilibrium, the equilibrium theory in Sec. II still applies. The absence of equilibrium with the helium bath enters only in the time dependence (and, hence, the $`B`$-dependence) of the spin temperature $`T_s`$. This dependence has been calculated using various IHF models.Bindilatti et al. (1991); Shapira et al. (1999); Chiorescu et al. (2000); Nakano and Miyashita (2001); Waldmann et al. (2002) Approaching the energy-level crossing (strictly, anticrossing) associated with each MST, $`T_s`$ decreases. After passing through the anticrossing region, $`T_s`$ increases. If some heat flows between the sample and the bath then the latter increase is large enough that $`T_s`$ is temporarily above $`T_{\mathrm{bath}}`$. Miyashita and co-workersNakano and Miyashita (2001) have called this behavior of $`T_s`$ “the magnetic Foehn effect.”

The $`B`$-dependence $`T_s`$ can lead to the following qualitative effects: 1) The $`dM/dB`$ peaks are narrower than the thermal width. 2) The $`dM/dB`$ peaks are asymmetric, i.e., the rise of $`dM/dB`$ as the MST is approached is faster than the fall after passing through the MST. This is true both for increasing and decreasing $`B`$. 3) The magnetization and $`dM/dB`$ exhibit hysteresis. 4) Under some conditions, a small “satellite” MST appears after the main MST. All these effects have been observed experimentally.

#### III.2.3 Cross Relaxation (CR) Model

A severe non-equilibrium behavior, not explainable by IHF models, was observed in pulsed field experiments by Ajiro et al.Ajiro et al. (1998) It was interpreted in terms of CR between pairs and singles, and also between the pairs themselves. More recently, CR was discussed in the context of tunneling theory.Wernsdorfer et al. (2002); Giraud et al. (2001) CR can involve both ground and excited states.

CR is one of the mechanisms of spin relaxation. It involves simultaneous spin flips in weakly coupled clusters. The model of Ajiro et al. also includes a single spin flip in only one of the clusters. The later is actually not a CR process, and is better described as tunneling. In this model the spin relaxation rate is appreciable only at some values of $`B`$.

The simplified picture used in Ref. Ajiro et al., 1998 ignored small level repulsions near level crossings. (Level repulsion is included in more detailed models that are based on tunneling.Wernsdorfer et al. (2002); Giraud et al. (2001)) In this simplified picture the relaxation rate can be fast only if simultaneous CR spin flips, or a single spin flip, do not change the total energy of the spin system. For a single spin flip, in one cluster, this happens at energy-level crossings for this cluster. These level crossings include those of excited states. For CR between two weakly coupled clusters the energy-level separation in one cluster should match a level separation in the other. The two clusters may be of the same type (e.g., two coupled pairs) or of different types (e.g., a pair and a single). A similar criterion for energy-level separations applies to CR between three, or more, coupled clusters.

In the equilibrium theory, the $`dM/dB`$ peaks associated with MST’s from $`\mathrm{Mn}^{2+}`$ pairs occur at fields

$$g\mu _\mathrm{B}B_i=2i|J|,$$
(15)
where $`i=1,2,\mathrm{},(2S+1)`$. In the model of Ajiro et al. these peaks from pairs are called the “fundamental” peaks, and they are labeled as $`\mathrm{P}_i`$. Specializing to pairs composed of $`\mathrm{Mn}^{2+}`$ ions, there are five such peaks. In addition to the fundamental peaks, other peaks are also predicted. The most pronounced are the “second harmonic” peaks $`\mathrm{P}_{m/2}`$ at fields $`B_m=m(B_1/2)`$, with $`m=1\text{ to }10`$. The five peaks for odd $`m`$ were observed clearly by Ajiro et al. The peaks for even $`m`$ coincide with the fundamental peaks.

In addition to the second-harmonic peaks, fifteen third harmonic peaks $`\mathrm{P}_{k/3}`$ at $`B_k=k(B_1/3)`$, were predicted. Many of these were also observed. Fourth and sixth harmonic peaks were also discussed. These results are from a model which involves only singles and pairs. The model can be extended to include other clusters.

Some of the simultaneous spin-flip transitions which can give rise to $`\mathrm{P}_{1/2}`$ (the first of the ten second-harmonic peaks) are shown in Figs. 4(a) and 4(b). Note that in either case, each of the two simultaneous spin flips increase the component of the spin along $`B`$ by one unit. Figure 5 shows a few level crossings that may contribute to various peaks: the first three fundamental peaks $`\mathrm{P}_1`$, $`\mathrm{P}_2`$, $`\mathrm{P}_3`$; the third and fifth second-harmonic peaks, $`\mathrm{P}_{3/2}`$ and $`\mathrm{P}_{5/2}`$; and the second third-harmonic peak, $`\mathrm{P}_{2/3}`$. Cross relaxation processes may also contribute to some of the same peaks, e.g., to $`\mathrm{P}_{2/3}`$.

## IV EXPERIMENTAL TECHNIQUES

### IV.1 Sample preparation

The procedure of growing crystals of TMMC:Cd followed Ref. Dupas and Renard, 1978. The samples were grown by evaporation from water solutions of $`\mathrm{MnCl}_2.4\mathrm{H}_2\mathrm{O}`$, $`(\mathrm{CH}_3)_4\mathrm{NCl}`$, $`\mathrm{CdCl}_2.2\mathrm{H}_2\mathrm{O}`$, and some $`\mathrm{HCl}`$ acid. The solutions were maintained at $`30^\mathrm{o}\mathrm{C}`$. As already noted, the Cd concentration in the crystallized samples is about $`50`$ times larger than in the starting solution.Dupas and Renard (1978); Schouten et al. (1982) Because the Cd concentration in the solution decreases rapidly as the crystal growth progresses, a large solution volume ($`300\mathrm{ml}`$) was used to crystalize a “product” of TMMC:Cd with a total mass of about $`100\mathrm{mg}`$. The large starting volume increased the uniformity of the Cd concentration in the product.

Physically, the product consisted of many needle-shaped crystals. The long dimension of a needle (up to $`4\mathrm{mm}`$) was parallel to the hexagonal axis. The color gradually changed from pink towards white as the Mn concentration $`\mathrm{x}`$ decreased. Each of the magnetization measurements, in both dc magnetic fields and in pulsed fields, used only a portion of the product, typically $`30\mathrm{mg}`$.

The Mn concentration $`\mathrm{x}`$, was determined from the high-temperature dc susceptibility, $`\chi =M/B`$, measured using a SQUID magnetometer. The magnetic field $`B`$ = $`0.1\mathrm{T}`$ was well within the range where $`\chi `$ is independent of $`B`$. In the temperature range from $`150\mathrm{K}`$ to $`300\mathrm{K}`$, the data for $`\chi `$ were well described by a sum of a Curie-Weiss susceptibility and a constant due to the diamagnetism of the lattice. The concentration $`\mathrm{x}`$ was obtained from the Curie constant $`C`$. Strictly, the Curie-Weiss law is accurate only in the limit of very high temperatures. The percentage error in the Curie constant, resulting from the use of data between $`150\mathrm{K}`$ and $`300\mathrm{K}`$, depends on the Mn concentration. Based on the results in Ref. Dong et al., 1988, for the samples used here the error in $`C`$, and hence in $`\mathrm{x}`$, was less $`2\%`$. The percentage error in the Curie-Weiss temperature $`\theta `$ is larger than for $`C`$, but $`\theta `$ does not enter into the determination of $`\mathrm{x}`$.

Values of $`\mathrm{x}`$ for several portions of the $`100\mathrm{mg}`$ product obtained from a single solution were close to each other. A quantitative comparison between experimental dc magnetization data and theoretical simulations was carried only for samples $`2`$, $`4`$, and $`5`$ in Table 1. To increase the confidence in this comparison, values of $`\mathrm{x}`$ were determined for the very same three samples. As a check, the Mn and Cd weight percents for these three samples were also determined directly by atomic emission spectroscopy with inductively coupled plasma (ICP-AES). The values of $`\mathrm{x}`$ deduced from ICP-AES were in reasonable agreement with the values from the susceptibility (see Table 1).

The magnetization of several other samples ($`1^{}`$, $`3^{}`$, $`4^{}`$, and $`5^{}`$ in Table 1) was also measured in dc fields. However, for these samples each value of $`\mathrm{x}`$ is from susceptibility data on a different portion of the same product. Samples $`4`$ and $`4^{}`$ are two different portions of the same product, as are samples $`5`$ and $`5^{}`$.

X-ray powder diffraction patterns were obtained at room temperature using Cu-$`\mathrm{K}_\alpha `$ radiation. Data were taken on two samples from the same products as those of samples 1\* and 4 (or 4\*). The diffraction patterns for both samples were very similar to the pattern obtained, with the same equipment, on pure TMCC ($`\mathrm{x}=0`$). No additional, or missing, diffraction peaks were observed. These results are consistent with a single crystallographic phase.

### IV.2 Magnetization in dc magnetic fields

Magnetization data in slowly varying magnetic fields (so-called “dc fields”) were taken with a vibrating sample magnetometer (VSM). The VSM operated in $`18\mathrm{T}`$ superconducting magnets. The sample was in direct contact with a liquid $`{}_{}{}^{3}\mathrm{He}`$ bath, which was in an insert dewar. The temperature $`0.55\mathrm{K}`$ was reached by pumping on the $`{}_{}{}^{3}\mathrm{He}`$ bath. The field-sweep time (zero to $`18\mathrm{T}`$) was about $`1\mathrm{hour}`$.

### IV.3 Differential Susceptibility in pulsed magnetic fields

The differential susceptibility, $`dM/dB`$, was measured in pulsed magnetic fields up to $`50\mathrm{T}`$ ($`500\mathrm{kG}`$). The techniques have been described earlier.Shapira et al. (1999) The shape of the field pulse ($`B`$ versus time) was approximately a half cycle of a weakly damped sine wave, with a rise time of $`3.1\mathrm{ms}`$, and fall time of $`4.3\mathrm{ms}`$. For each sample, data were first taken with the sample in the pickup coils, and shortly thereafter with the sample outside the pickup coils. The signal from the sample was obtained by taking the difference.

The powder samples used in the pulse field experiments were obtained by crushing the mm-size needles of the growth products. Each sample, consisting of $`20`$ to $`30\mathrm{mg}`$ fine powder (grain size less than $`0.1\mathrm{mm}`$), was placed in a thin-walled ($`0.25\mathrm{mm}`$) cylindrical capsule made of Delrin. The capsule was immersed in a liquid $`{}_{}{}^{4}\mathrm{He}`$ bath which was maintained at $`1.5\mathrm{K}`$. The Delrin capsule had a small hole at its bottom. The hole (covered by a tissue paper) allowed a direct contact between the sample and the bath of superfluid helium. However, previous experiments have indicated that despite such a direct contact the sample may not be in thermal equilibrium with the bath during the $`7.4\mathrm{ms}`$ field pulse.Shapira et al. (1999, 2001)

## V MAGNETIZATION IN DC MAGNETIC FIELDS

### V.1 Experimental Results

#### V.1.1 Gross Features

Figure 6(a) shows magnetization data at $`0.55\mathrm{K}`$ for samples 2, 4, and 5. These “dc data” were actually obtained with a sweep rate of $`0.3\mathrm{T}/\mathrm{min}`$. No hysteresis was observed. The (very small) corrections for lattice diamagnetism and addenda are included in Fig. 6, so that the magnetization $`M`$ is that of the $`\mathrm{Mn}^{2+}`$ ions. The numerical derivatives, $`dM/dB`$, of these curves are shown in Fig. 6(b). The Mn concentrations $`\mathrm{x}`$, measured on the very same samples, are given in Table 1.

The main features in Fig. 6(a) are: 1) a fast rise of $`M`$ at low H, 2) a large MST near $`9`$ or $`10\mathrm{T}`$, and 3) a smaller MST near $`4\mathrm{T}`$. There are also indications of other MST’s at higher fields. For example, sample 2, for which the data extend to slightly higher fields than for the other samples, shows the beginning of a large MST near the top of the field. These main features of the dc magnetization curves agree with theoretical predictions for the equilibrium magnetization, such as those in Fig. 3(b). The range of the reduced field $`b`$ that corresponds to the experimental data in Fig. 6 extends up to about $`4`$. The exact maximum value of $`b`$ is slightly different for different curves in this figure.

The fast rise of the $`M`$ at low $`B`$ corresponds to the alignment of the zero-field-ground-state spin, $`S_T(0)`$, of finite chains with odd $`n`$. The main contribution to this fast rise is from the singles ($`n=1`$). The large MST observed near $`9`$ or $`10\mathrm{T}`$ corresponds, essentially, to the first MST from pairs (clusters with $`n=2`$). Other contributions to this observed MST are from some longer chains that have a MST at nearly the same field. For example, the second MST from quartets (chains with $`n=4`$) is predicted to occur at a field which is only $`2\%`$ higher than that of the first MST from pairs. Neither the triplets ($`n=3`$) nor the quintets ($`n=5`$) have a MST near this field. The total contribution of chains with $`n>2`$ to the observed MST near $`9`$ or $`10\mathrm{T}`$ is expected to be smaller than the contribution from the pairs. The reason is that for $`\mathrm{x}=0.5`$ the populations $`N_n`$ of these longer chains are small compared to the population $`N_2`$ of the pairs.

For sample 2, a substantial portion of the second MST from pairs is also seen at the highest fields. The peak in the derivative $`dM/dB`$ for this sample, near the top of the field in Fig. 6(b), is close to the expected field for this MST, i.e., $`B_2=2B_1=17.4\mathrm{T}`$. The beginning of the second MST from pairs is also seen in the derivative curve for sample 4.

The relatively small MST near $`4\mathrm{T}`$, seen in Figs. 6(a) and (b), is identified as the first MST from the chains with $`n=4`$ (so-called “string quartets”). The first MST from the quartets is predicted to occur at $`B=0.475B_1`$, where $`B_1`$ is the field at the first MST from pairs. The experimental results in Table 1 are in reasonable agreement with this prediction. The second MST from quartets which, as already noted, is predicted to occur at a field which is only $`2\%`$ higher than $`B_1`$, was not resolved at $`0.55\mathrm{K}`$. This was expected because at $`0.55\mathrm{K}`$ the broadening of any MST due to the finite temperature (“thermal broadening”) is more than $`10\%`$ of $`B_1`$. The third MST from the quartets is also predicted to occur within the field range of Fig. 6. However, the predictions for this MST were not fully confirmed by the data. For example, in Fig. 6(b) the derivative curve for sample 5 exhibits a small peak near $`15\mathrm{T}`$. For the same sample, the predicted field at the third MST from the quartets is higher by about $`1\mathrm{T}`$.

Some features of the experimental results in Fig. 6 depend on the Mn concentration $`\mathrm{x}`$. The first MST from the quartets stands out more clearly as $`\mathrm{x}`$ increases. This trend is expected from the probability curves in Fig. 1. The cluster populations $`N_n`$ are related to these probabilities by Eq. (2). As $`\mathrm{x}`$ increases there is an increase in population ratios $`N_4`$/$`N_2`$ between quartets and pairs, and $`N_4`$/$`N_1`$ between quartets and singles. Therefore, as $`\mathrm{x}`$ increases, the MST from quartets stands out more clearly in comparison with the MST from pairs, and also in comparison with fast magnetization rise at low fields.

Another feature that depends on $`\mathrm{x}`$ is the value of the magnetic field at the large MST near $`9`$ or $`10\mathrm{T}`$. In Fig. 6(b) the peak associated with this MST shifts to slightly higher fields as $`\mathrm{x}`$ increases. The field at this peak is expected to be very close to $`B_1`$. Numerical values as a function of $`\mathrm{x}`$ are listed in Table 1. The change of $`B_1`$ is attributed to a slight dependence of the NN exchange constant $`J`$ on the Mn concentration.

#### V.1.2 NN Exchange Constant

The NN intrachain exchange constant $`J`$ was obtained from the field $`B_1`$ of the first MST from pairs, using Eq. (15) and assuming $`g=2.00`$ for the $`\mathrm{Mn}^{2+}`$ ion. Values of $`J`$ for all the samples are given in Table 1. The exchange constant for $`\mathrm{x}=0.5`$, $`J/k_\mathrm{B}=6.5\mathrm{K}`$, is about $`10\%`$ higher than for $`\mathrm{x}=0.22`$. This $`10\%`$ change is too large to be accounted for by the unresolved MST from the quartets. As already mentioned, $`J/k_\mathrm{B}6.6\mathrm{K}`$ for pure TMMC ($`\mathrm{x}=1`$). We are not aware of any theoretical calculation of the $`\mathrm{x}`$-dependence of $`J`$ in this system.

### V.2 Comparison with Simulations

Figures 79 compare the experimental results with numerical simulations based on equilibrium theory for the single-$`J`$ model (Section II). The comparison is for the normalized magnetization $`m=M/M_0`$, where $`M_0`$ is the true saturation magnetization. The “experimental” curves use the measured $`M`$ (Fig. 6) and the calculated saturation magnetization $`M_0`$ for the Mn concentration $`\mathrm{x}`$. The simulations assume a random distribution of the Mn ions, and use the values of $`J`$ and $`\mathrm{x}`$(Suscept.) given in Table 1 for that sample. Clusters with $`n5`$ are treated exactly, and the rise-and-ramp approximation is used for the total contribution of larger clusters. There are no adjustable parameters in the simulations.

For sample 2, with $`\mathrm{x}=0.22`$, the agreement between experiment and theory is reasonably good (Fig. 7). The difference between the measured and simulated magnetizations is a few percent. It is comparable to the total experimental uncertainty, mainly from the uncertainty in $`\mathrm{x}`$. The observed magnitude of the first MST from the pairs is in agreement with the simulation. However, the associated experimental $`dM/dB`$ peak is somewhat broader than in the simulation. Physical mechanisms that broaden MST’s were discussed in Ref. Shapira and Bindilatti, 2002. In the present case thermal broadening at the experimental temperature, $`T=0.55\mathrm{K}`$, is expected to be the strongest of these mechanisms. It is the only broadening mechanism that was included in the simulations. Non-thermal causes of line broadening include the dipole-dipole interaction and local strains associated with the random replacement of Mn by Cd. Because non-thermal broadening was neglected in the simulation, it is not surprising that the experimental $`dM/dB`$ peaks are somewhat broader. The numerical differentiation of $`M`$ with respect to $`B`$ also broadens the experimental peak slightly.

Figure 8 shows that for $`\mathrm{x}=0.25`$ the agreement between experiment and simulation is, again, reasonably good. However, the observed $`dM/dB`$ peak at $`4.3\mathrm{T}`$, from the first MST for quartets, is somewhat larger than expected. The simplest interpretation is that the number of quartets is larger than given by a random distribution. The behavior of the derivative $`dm/dB`$ near $`15\mathrm{T}`$ is attributed to the third MST from quartets.

Figure 9 shows that the agreement between experiment and simulation for $`\mathrm{x}=0.48`$ is only fair. The measured magnetization is somewhat smaller than expected, over the entire field range. In particular, the initial rise of the measured magnetization is smaller than in the simulation. This discrepancy suggests that the Mn ions have a slight tendency to bunch together, compared to a random distribution.Shapira and Bindilatti (2002) Also, the peak of $`dm/dB`$ near $`15\mathrm{T}`$ is at a lower field than predicted for the third MST from the quartets. The reason for this behavior is unclear. In our view, despite these discrepancies the agreement between experiment and theory is still reasonable.

## VI DIFFERENTIAL SUSCEPTIBILITY IN PULSED FIELDS

Pulsed-field data for $`dM/dB`$ were taken on powder samples with $`\mathrm{x}0.50`$ (from the same product as samples $`5`$ and $`5^{}`$), $`\mathrm{x}0.22`$ (same product as $`2`$ and $`2^{}`$), and $`\mathrm{x}0.16`$ (same product as $`1^{}`$). As noted in Sec. IV, each sample was in direct contact with a liquid-helium bath, maintained at $`T_{\mathrm{bath}}=1.5\mathrm{K}`$. However, such a direct contact does not ensure thermal equilibrium with the bath during the $`7.4\mathrm{ms}`$ pulse.

The pulsed-field data are presented next. Non-equilibrium features are pointed out, and many of them are then interpreted. However, some aspects of the non-equilibrium behavior are still not fully understood.

### VI.1 Experimental Results in Pulsed Fields

Figure 10 shows some $`dM/dB`$ data for $`\mathrm{x}0.50`$. Part (a) of this figure shows an “up trace” (increasing $`B`$) and a “down trace” (decreasing $`B`$) obtained during the same field pulse. Part (b) gives an expanded view of a portion of the down trace.

Results for $`\mathrm{x}0.22`$ are shown in Fig. 11(a). This figure covers the wide range of $`dM/dB`$ values that is required to display the large hysteresis in low fields. Data taken during the same field pulse, but which cover a much narrower range of $`dM/dB`$ values, are shown in Fig. 11(b).

Results obtained for $`\mathrm{x}0.16`$ during a pulse with a maximum magnetic field $`B_{\mathrm{max}}=17\mathrm{T}`$ are shown in Fig. 12(a). Figure 12(b) shows the decreasing-field portion of a trace obtained during another field pulse for which the maximum field was $`34\mathrm{T}`$. \[Unlike all the other pulsed-field data in the present paper, the data in Fig. 12(b) have not been corrected for the monotonic background, because no “background shot” (with the sample out of the pickup coils) was taken in this case.\] Figure 13 shows an expanded, and slightly smoother, view of the field-down portion of the Fig. 12(a).

### VI.2 Discussion of non-equilibrium effects

The pulsed-field data do not provide any new information about the exchange constant $`J`$. However, these data show interesting non-equilibrium effects. The discussion below focuses primarily on: 1) those features of the data that indicate the absence of thermal equilibrium; 2) the change of the non-equilibrium behavior with the Mn concentration $`\mathrm{x}`$; and 3) physical mechanisms that can give rise to such non-equilibrium effects.

#### VI.2.1 $`\mathrm{x}0.50`$

Consider first those pulsed-field results in Fig. 10 that are below $`15\mathrm{T}`$. There is a prominent peak near $`10\mathrm{T}`$. It stands out more clearly in the down trace (decreasing $`B`$) than in the up trace. This peak corresponds to the first MST from pairs. The down trace also shows a smaller peak just below $`5\mathrm{T}`$. This smaller peak corresponds to the first MST from the quartets. Although both of these peaks were also observed in the dc data for the equilibrium magnetization \[Fig. 6(b)\], at least two features of the pulsed-field data indicate departures from equilibrium with the helium bath, at $`T_{\mathrm{bath}}=1.5\mathrm{K}`$. First, the up and down traces below $`15\mathrm{T}`$ are different, i.e., there is an hysteresis in this field range. Second, the widths of both the peak near $`10\mathrm{T}`$ and near $`5\mathrm{T}`$ are substantially smaller than the equilibrium width at the bath temperature.

The “width” of a MST will always refer to the full width at half maximum of the associated peak in $`dM/dB`$. The various contributions to the equilibrium width were discussed in Ref. Shapira and Bindilatti, 2002. Often, temperature broadening is important. The thermal width at the temperature $`T`$ is

$$(\delta B)_T=3.53k_\mathrm{B}T/g\mu _\mathrm{B}.$$
(16)
Because non-thermal broadening mechanisms are also present in equilibrium, the thermal width is a lower limit for the actual equilibrium width. The calculated thermal width, $`(\delta B)_T=3.9\mathrm{T}`$ for the actual bath temperature $`T_{\mathrm{bath}}=1.5\mathrm{K}`$, is shown in Fig. 10(b).

To obtain the experimental width it is necessary to choose a baseline for the peak in $`dM/dB`$. Such a choice is not always obvious. In Fig. 10(b), two possible choices for the peak near $`10\mathrm{T}`$ are indicated by the dashed lines 1 and 2. Baseline 1 leads to a full width at half maximum of $`2.2\mathrm{T}`$. Baseline 2 leads to a width of $`1.9\mathrm{T}`$. On this basis we conclude that the experimental width is substantially smaller than the equilibrium width.

The choice of a baseline for the peak near $`5\mathrm{T}`$ is also not obvious. The particular choice shown as a dashed line leads to a width of $`1.2\mathrm{T}`$. Although other choices may lead to a larger experimental width, it seems that any reasonable choice will lead to a width that is smaller than the thermal width. Thus, the experimental widths of both of the peaks in Fig. 10(b) are smaller than the width that would have occurred had the sample been in equilibrium with the helium bath.

Figure 10 also shows the second MST from pairs, near $`20\mathrm{T}`$. This peak is broader than the first peak from the pairs. A significant feature of this peak is that it is asymmetric. As a function of time, the rise of $`dM/dB`$ as the peak is approached is faster than the fall after passing through the peak. This asymmetry is observed in both increasing and decreasing $`B`$. An asymmetry of this type is expected from models that assume an inadequate heat flow (Sec. III.2). The data in Fig. 10 therefore suggest that the non-equilibrium behavior for $`\mathrm{x}0.50`$ is due to inadequate sample-to-bath heat flow.

The IHF scenario can also account for the hysteresis below about $`15\mathrm{T}`$. When the thermal contact with the bath is poor, strong magneto-caloric effects are expected from the singles (clusters with $`n=1`$). These effects are analogous to those involved in the cooling of a paramagnet by adiabatic demagnetization (and warming by adiabatic magnetization). Of course, the actual processes in the present case are not truly adiabatic, because there is some heat flow between the sample and the bath. In our view, no feature of the data in Fig. 10 requires CR for its explanation. The observed non-equilibrium effects seem to be explainable by an inadequate sample-to-bath heat flow.

Another issue (not directly related to the non-equilibrium behavior) involves the third MST from pairs, seen in Fig. 10 near $`30\mathrm{T}`$. Compared to the first and second MST’s from pairs, the third MST is less well defined. Specifically, $`dM/dB`$ hardly decreases on the high-field side of the third MST. This behavior is explained by the three small MST’s from quartets, triplets, and quintets that are expected between the third and fourth MST’s from pairs (see the MST’s near $`b=7`$ in Fig. 3). For $`\mathrm{x}=0.5`$ the predicted combined size of these three small MST’s is comparable to the size of one MST from pairs.

#### VI.2.2 Non-equilibrium behavior for $`\mathrm{x}0.16`$

The absence of thermal equilibrium with the helium bath is very evident in the pulsed-field data for $`\mathrm{x}0.16`$.

1. A pronounced hysteresis is seen in Fig. 12(a).
2. In the down portion of the pulse (see Fig. 13) the widths of the peaks near $`10`$, $`5`$, and $`2.7\mathrm{T}`$ are $`1.4`$, $`0.9`$, and $`0.6\mathrm{T}`$, respectively. These values are small compared to a thermal width of $`3.9\mathrm{T}`$ at $`T_{\mathrm{bath}}=1.5\mathrm{K}`$. A width that is smaller than the thermal width implies a non-equilibrium behavior.
3. The peak near $`5\mathrm{T}`$ is very pronounced in the pulsed-field data shown in Figs. 12(a) and 13, but is barely seen in dc data on a sample from the same product. The dc data, shown in Fig. 14, should be representative of equilibrium behavior. Therefore, the pronounced peak in the pulsed field data is regarded as a non-equilibrium effect.
4. The second MST from pairs, near $`18\mathrm{T}`$, is barely observed in Fig. 12(b), and the third MST from pairs, near $`27\mathrm{T}`$, is totally absent. The corresponding field-up trace (not shown) exhibits a similar behavior. Once again the pulsed field data are contrasted with the equilibrium magnetization data in Fig. 14. The latter data, which extend up to $`17.5\mathrm{T}`$, show a significant portion of the second MST from pairs, and they indicate that in equilibrium the sizes of the second and first MST’s from pairs are comparable. That is, unlike the behavior in pulsed fields, the second MST is not small compared to the first. In equilibrium, all MST’s from pairs are expected to be comparable, which is inconsistent with the results of Fig. 12(b).

#### VI.2.3 IHF and CR Scenarios for $`\mathrm{x}0.16`$

The large hysteresis at low fields \[Fig. 12(a)\] is not uncommon in pulsed field experiments on diluted magnetic materials.Foner (1994); Ajiro et al. (1998) In the present case the hysteresis is largely due to the slow response of the singles to the rapidly changing $`B`$. In the up portion of the pulse the alignment of the spins of the singles is not completed until $`B`$ is above $`10\mathrm{T}`$. In the down portion of the pulse these spins remain largely aligned until $`B`$ drops below $`1\mathrm{T}`$. For $`\mathrm{x}0.16`$, the majority of the spins ($`70\%`$ for a random distribution) are singles, so that the hysteresis is very pronounced.

MST’s from pairs and larger clusters stand out more clearly in the down portion of the field pulse because the singles remain largely aligned until $`B`$ drops below $`1\mathrm{T}`$. For this reason the field-down portion of the traces in Figs. 13 and 12(b) is discussed first.

Spin-lattice relaxation times are often longer for lower $`\mathrm{x}`$, which is the likely cause of the more pronounced non-equilibrium behavior for $`\mathrm{x}0.16`$ compared to $`\mathrm{x}0.50`$. An important issue in the data interpretation is whether the spin-lattice relaxation is fast enough to maintain equilibrium within the sample. In that case the IHF scenario would apply (see Sec. III.2.2). An alternative is a more severe non-equilibrium behavior which is better described by the CR scenario, including single spin flips near level crossings of excited states (Sec. III.2.3).Ajiro et al. (1998); Wernsdorfer et al. (2002)

Below we consider both the IHF and CR scenarios for the down portion of the pulse. The preferred scenario cannot be chosen on the basis of the fields at which the MST’s occur, because the differences are often small compared to the experimental accuracy. However, the two scenarios lead to different relative sizes of the peaks in $`dM/dB`$. The poor agreement of the observed relative sizes with those predicted by the IHF scenario will suggest that the CR scenario is preferable for this Mn concentration.

Consider first the IHF scenario. In this scenario the magnetization of each cluster type is the equilibrium magnetization at $`T_s`$. For the low $`T_s`$ indicated by the small widths of the observed MST’s (in the down portion of the pulse), this magnetization is that of the ground state. The largest peak in Fig. 12, just below $`10\mathrm{T}`$, is mainly due to the first MST from pairs. The second largest peak, near $`5\mathrm{T}`$ is the first MST from quartets. It is predicted to occur at a field which is $`0.48`$ times that of the first peak for pairs. The second $`dM/dB`$ peak from quartets should be at a field which is $`2\%`$ higher than the first peak from pairs. The structure of the peak near $`10\mathrm{T}`$ is possibly due to a superposition of these two MST’s, although it is much wider than $`2\%`$.

In the IHF scenario the field at the first MST for finite chains with even $`n`$ can be estimated from the energy levels given in Ref. Lou et al., 2002. For $`n`$ between $`4`$ and $`10`$, this field is nearly proportional to $`1/n`$. A similar approximate dependence on $`n`$ holds for AF rings (closed chains).Gatteschi (2000) On this basis the small sharp peak near $`2.7\mathrm{T}`$ (in Fig. 12) is due to octets or sextets. There is also an indication of a small peak near $`2.0\mathrm{T}`$, which would be attributed to larger clusters.

Although the IHF scenario accounts for the fields of many of the observed MST’s, this scenario is very questionable for this Mn concentration. Assuming that the Mn cations are randomly distributed, the number of quartets for $`\mathrm{x}=0.16`$ is smaller than the number of pairs by a factor of $`39`$. For sextets and octets the factors are $`1.5\times 10^3`$ and $`6\times 10^4`$, respectively. Therefore, unless the deviations from random distribution are extremely large, it should not have been possible to observe MST’s from sextets or octets if the behavior followed the IHF scenario. The first MST from quartets might have been detectable, but it should have been very small compared to the MST from pairs. This was not the case in the pulse field experiments (Figs. 12 and 13). As predicted, the equilibrium data in Fig. 14, for nearly the same $`\mathrm{x}`$, indicate that the first MST from quartets is much less pronounced than the first MST from pairs.

In Fig. 12(b) the first MST from pairs stands out clearly but the second MST from pairs is barely visible, and the third is totally absent. These results also are not well understood within the IHF scenario, although some indication of such a behavior appeared in simulations by Nakano and Miyashita for iron clusters with ring structure.Nakano and Miyashita (2001)

In the CR scenario the MST’s in Figs. 12(b) and 13 (both for decreasing B) are interpreted as follows. The peak just below $`10\mathrm{T}`$ is the first fundamental peak $`\mathrm{P}_1`$, with some contributions from $`\mathrm{P}_{2/2}`$, $`\mathrm{P}_{3/3}`$, etc. The peak at $`5\mathrm{T}`$ is the second harmonic peak $`\mathrm{P}_{1/2}`$. The small peak at $`2.7\mathrm{T}`$ is the third-harmonic peak $`\mathrm{P}_{1/3}`$ or the fourth-harmonic peak $`\mathrm{P}_{1/4}`$. The broad peak near $`6.6\mathrm{T}`$ is possibly $`\mathrm{P}_{2/3}`$. Because this interpretation uses only pairs and singles,Ajiro et al. (1998) it is not open to objections based on the low populations of quartets and larger clusters. The CR scenario also accounts for some features of the up trace in Fig. 12(a). The large peak near $`5\mathrm{T}`$ is attributed to the CR process of the type shown in Fig. 4(b), except that the directions of both spin flips are reversed. This process allows the singles to relax toward a state with a higher magnetization. The magnetization of the pairs also increases by this process.

The process in Fig. 4(b) involves only one single and one pair, and is the simplest CR process between singles and pairs. It accounts for the $`\mathrm{P}_{1/2}`$. More complicated CR processes can lead to other “harmonic peaks,” such as $`\mathrm{P}_{1/3}`$, $`\mathrm{P}_{2/3}`$, $`\mathrm{P}_{3/4}`$. These peaks are expected to be smaller than $`\mathrm{P}_{1/2}`$. The peak $`\mathrm{P}_{1/3}`$ may involve processes such as a CR between a pair and two singles, or between a pair and a single which undergoes a double spin flip. The peak $`\mathrm{P}_{2/3}`$ may involve a spin flip in a single and spin flips in two pairs, etc. In the up trace the observed peak at $`3.2\mathrm{T}`$, and the small peaks at $`6.4`$, and $`7.4\mathrm{T}`$ may correspond to the $`\mathrm{P}_{1/3}`$, $`\mathrm{P}_{2/3}`$ and $`\mathrm{P}_{3/4}`$ harmonics. The peak observed near $`10\mathrm{T}`$ is a superposition of the first fundamental peak from pairs, $`\mathrm{P}_1`$, and the harmonics $`\mathrm{P}_{2/2}`$, $`\mathrm{P}_{3/3}`$, etc.

As already noted, in Fig. 12(b) the second MST from pairs is barely visible, and the third is totally absent. These results suggest that for $`\mathrm{x}0.16`$, the spin relaxation for pairs in fields above $`15\mathrm{T}`$ is very slow compared to a millisecond. As $`B`$ sweeps through a region where a MST from pairs should have occurred, the pairs are unable to relax towards the new ground state. We speculate that the slow spin relaxation for pairs is mainly due to a reduction of CR between pairs and singles, and that this reduction is related to the saturation of the singles in fields above $`15\mathrm{T}`$. CR between different pairs, or between pairs and larger clusters, is expected to become slower as $`\mathrm{x}`$ decreases.Abragam and Bleaney (1970) Among the three samples, such CR processes should be least efficient for $`\mathrm{x}0.16`$.

#### VI.2.4 Non-equilibrium behavior for $`\mathrm{x}0.22`$

Non-equilibrium behavior is also evident for $`\mathrm{x}0.22`$. The large low-field hysteresis for this Mn concentration, in Fig. 11(a), is somewhat similar to the hysteresis in Fig. 12(a) for $`\mathrm{x}0.16`$. In the up trace, the large peak near $`4.5\mathrm{T}`$ is identified as the $`\mathrm{P}_{1/2}`$ peak, and is attributed to the cross relaxation process in Fig. 4(b), with the arrows reversed.

The down trace in Fig. 11(b) exhibits large peaks near $`8.9\mathrm{T}`$ and $`4.4\mathrm{T}`$ approximately, and a small peak near $`2.1\mathrm{T}`$. The widths at half height of these peaks, $`1.3`$, $`0.9`$, and $`0.7\mathrm{T}`$, respectively, are all much smaller than thermal width of $`3.9\mathrm{T}`$ at $`T_{\mathrm{bath}}`$. These widths, which are similar to those for $`\mathrm{x}0.16`$, indicate non-equilibrium behavior.

The largest peak in Fig. 11(b), at $`8.9\mathrm{T}`$, is undoubtedly the first fundamental peak from pairs, $`\mathrm{P}_1`$. The second fundamental peak $`\mathrm{P}_2`$ is also observed near $`18\mathrm{T}`$. The CR scenario predicts large second-harmonic peaks $`\mathrm{P}_{1/2}`$, $`\mathrm{P}_{3/2}`$, $`\mathrm{P}_{5/2}`$ at $`4.5`$, $`13.4`$, and $`22.3\mathrm{T}`$, respectively. These fields are close to $`4.4`$, $`13.4`$, and $`21.8\mathrm{T}`$, of large peaks in Fig. 11(b). The peak observed near $`2.1\mathrm{T}`$ is consistent with $`\mathrm{P}_{1/4}`$. It is possible, but far from certain, that the small peaks at $`6.2`$ and $`12.0\mathrm{T}`$ are $`\mathrm{P}_{2/3}`$ and $`\mathrm{P}_{4/3}`$.

The main difference between $`\mathrm{x}0.22`$ and $`\mathrm{x}0.16`$ is that for the higher Mn concentration there are still prominent MST’s above $`10\mathrm{T}`$. For $`\mathrm{x}0.50`$ the second and third MST’s from pairs are even more pronounced \[see Fig. 10(a)\]. These results suggest that at these fields the spin relaxation rate for pairs increases rapidly with Mn concentration. We tentatively attribute this trend to the expected increase with $`\mathrm{x}`$ of the efficacy of CR processes involving pairs, and pairs and larger clusters.

#### VI.2.5 Summary of the analysis of non-equilibrium behavior

A definitive interpretation of the observed non-equilibrium behavior in pulsed fields is still lacking. However, it appears that for $`\mathrm{x}0.50`$ the non-equilibrium behavior is better explained by the IHF scenario. For $`\mathrm{x}0.16`$ and $`\mathrm{x}0.22`$ the data are better explained by spin flips associated with CR and with level crossings. The data suggest that at the high magnetic fields where the magnetization of singles is saturated, the spin relaxation rate for pairs increases rapidly with increasing $`\mathrm{x}`$. This increase is tentatively attributed to the $`\mathrm{x}`$-dependence of CR processes involving pairs.

###### Acknowledgements.

We thank R. Muccillo (USP) and J. A. Adario (MIT) for X-rays measurements. The work in Brazil was supported by FAPESP (Fundação de Amparo à Pesquisa do Estado de São Paulo, Brazil) under contract number 99/10359–7. The authors APF, NFOJ and VB acknowledge support from CNPq (Conselho Nacional de Desenvolvimento Científico e Tecnológico, Brazil). Travel funds for YS were provided by FAPESP.


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# The Many Worlds of Uncertainty

## 1 Introduction

The status of the uncertainty relations varies between the different interpretations of quantum mechanics. At one end of the scale, for Heisenberg they showed the fundamental limits of applicability of the wave and particle pictures separately. At the other end, in hidden variable theories they are merely statistical mechanical relations of no foundational significance. The aim of the current paper is to explore their meanings within a certain neo-Everettian many worlds interpretation. We will also look at questions that have been linked with the uncertainty relations since Heisenberg’s uncertainty principle: those of joint and repeated measurement of non-commuting (or otherwise ‘incompatible’) observables. This will have implications beyond the uncertainty relations, as we will see the fundamentally different way in which statistical statements are interpreted in the neo-Everett theory that we use.

## 2 Neo-Everettian Many Worlds

It is firstly necessary briefly to describe the interpretation with which we will explore the uncertainty relations. This has been described (with full references) in , and is a variant of the many worlds theory started by Everett .

The salient points are these. As with all Everett-style theories, the measurement problem is solved by having all possible outcomes of an interaction instantiated. The ‘worlds’ of which there are ‘many’ are not defined by a precise rule, but rather are structures identified “for all practical purposes”. They are structures marked out by their usefulness, explanatory relevance and persistence over time, as high-order rather than fundamental ontology. They occur at all levels: there are structures of decoherent branches that persist over large timescales and act in ways that we would call ‘a universe’, and within them can be identified other substructures.

To take the old example, within the state of a Schroödinger Cat experiment we would be able to identify two structures that persisted stably over time: one of a cat alive (and unbroken apparatus) and one of a dead cat (and associated apparatus). These are not, of course, the only structures identifiable in that state (we need only to change basis), but they persist in a stable state over timescales relevant to the experiment, and indeed after the diabolical device is opened they become elements in the decoherence basis. The identification of the cats is not precise: just as, in everyday life, we chose to call an imprecisely defined and constantly changing bundle of atoms ‘a cat’, so when we look at the quantum state of the system we see something that looks like that which we would normally refer to as ‘an alive cat’, and something that looks like a dead cat. We therefore say we have two worlds, one in which there is an alive cat, and one in which there is a dead one111These worlds at this point only extend as far as the bounds of the apparatus - the theory is local..

One unusual feature of this type of many worlds theory is that, while at larger scales decoherence picks out the relevant structures for us, at very small scales there can be more than one basis in which we find relevant structures. This will, of course, depend on what we are looking for and how the system is evolving – again, the identification of structures is not fundamental.

## 3 The Uncertainty Relations

Before coming on to the uncertainty relations that we will be looking at, it is worth saying with what we will *not* be dealing.

We will not be using the ‘textbook’ form of the uncertainty relations, the Robertson relation for non-commuting observables:

$$\mathrm{\Delta }A\mathrm{\Delta }B\frac{1}{2}|[A,B]|$$
(1)
where

$$\mathrm{\Delta }A=A^2A^2\mathrm{\Delta }B=B^2B^2$$

There are various standard problems with this formulation (summarized in )222The stronger relation owing to Schrödinger,
$$(\mathrm{\Delta }A)^2(\mathrm{\Delta }B)^2\frac{1}{4}|[A,B]|^2+\frac{1}{4}\{(AA),(BB)\}^2$$
will also not be dealt with, as it suffers from the same problems.. For present purposes the main problems are:

* These relations tell us nothing when one of the observables is in an eigenstate as then the right hand side of the inequality is zero. There are also other situations when they give no information – for example, in a spin-half system, because $`[S_x,S_z]=\mathrm{i}\mathrm{}S_y`$, if $`S_y=0`$ then the relations tell us nothing about $`S_x`$ and $`S_z`$. This is even though they are non-commuting observables of the system, which are considered the objects of the uncertainty relations on this view. They are not, therefore, fully general inequalities.
* The relations work only for Gaussian (or near-Gaussian) distributions. The interpretation of the quantities $`\mathrm{\Delta }A`$ and $`\mathrm{\Delta }B`$ as spreads only works for such distributions.

Neither will we look at any uncertainty relations including time – given the status of time these will be very different objects from other uncertainty relations. Lastly, we will not be looking at entropic uncertainty relations, for the very reason that Deutsch  champions them: they deal not with fundamentals (which we wish to look at to analyse from a neo-Everettian perspective) but with operational situations.

We will be using the uncertainty relations owing to Uffink :

$$\delta \theta W(\widehat{A})\mathrm{}\mathrm{arcos}\left(\frac{1+\beta \alpha }{\alpha }\right)$$
(2)
The quantities are defined as follows: $`\widehat{A}`$ is an operator that generates a group of states $`|\psi _\theta `$ by

$$|\psi _\theta =\mathrm{e}^{\frac{\mathrm{i}\theta \widehat{A}}{\mathrm{}}}|\psi $$

$`\delta \theta `$ is the smallest value of $`\theta ^{}`$ such that

$$|\psi _\theta |\psi _{\theta +\theta ^{}}|=\beta <1$$

$`W(\widehat{A})`$ is the smallest interval in the distribution $`\psi |a`$ (where $`\widehat{A}|a=a|a`$) in which a fraction $`\alpha <1`$ is contained:

$$_W|\psi |a|^2\mathrm{da}=\alpha $$

Finally it is a requirement of the relation that $`\beta 2\alpha 1`$.

If we chose $`\beta `$ such that states become more-or-less distinguishable once their overlap reaches it, the quantity $`\delta \theta `$ is therefore the expected error in estimated a given state: states in the range $`|\psi _{\theta \delta \theta }`$ to $`|\psi _{\theta +\delta \theta }`$ are indistinguishable by any measurements.

The ‘minimal interpretation’  of these identities is that they are relations between constraints on different probability distributions of the same state, for groups and their generators333The most famous of these in the context of uncertainty relations are position and momentum, each of which acts as the generator of the other group. The set of spacial translations is generated by
$$1\frac{\mathrm{i}}{\mathrm{}}𝐩.\mathrm{𝐝𝐱}^{}$$
and that of translations in momentum space by
$$1\frac{\mathrm{i}}{\mathrm{}}𝐱.\mathrm{𝐝𝐩}^{}$$
. They do not fully define the distributions, but give conditions they must necessarily follow. $`\delta \theta `$ gives a constraint on the $`\psi |\psi _\theta `$ probability distribution: the more spread out the probability distribution, the less sharply we would be able to estimate the state, even given multiple measurements on an ensemble of similarly prepared states.

To go beyond this minimal interpretation in the direction of our many worlds theory we will need to make an assumption about probability. The interpretation of probability is an enormous problem for Everett-style theories, and one which we will not make any attempt to solve here. We will instead make the (hopefully minimal) assumption that probabilities are attached in a basic way to worlds. For whichever part of a state we take to be a single ‘world’, the square of the associated coefficient is the probability given to that world. Beyond this, we keep silence444It is worth pointing out that in our neo-Everett view there is no ontological classical probability: all such probability arises because of quantum probabilities. We therefore cannot say, for example, “We are entangled with a given world but we do not know which one”: if we cannot tell by any means which of a bunch of worlds we are entangled with then its relative state is a superposition of those worlds..

The standard interpretation of a probability distribution in quantum mechanics is as the distribution of the outcomes of measurements on an ensemble of similarly prepared states. Given this, the relations (2) are statistical relations for an ensemble of states, and therefore give only a statistical relation for an individual system. However, in our neo-Everettian interpretation we do not need to invoke an ensemble to make sense of our statistics as we have one within a single state – an ensemble of worlds and their associated probabilities. Probability distributions are therefore distributions of probability over *worlds*, and refer to single systems.

For an example, take a single qubit system in the state $`\frac{1}{\sqrt{2}}(|+|)`$. Standardly the probability distribution would be described as something like: “do measurements in the $`\{|,|\}`$ basis on a large number of similarly prepared systems, and roughly 50% will be up and 50% down.”. In the neo-Everett theory it refers ontologically to the fact that within the single qubit system itself can be identified two worlds in the $`\{|,|\}`$ basis, both of which have associated probability 0.5. The former description is, of course, still how we would gain epistemic access to the distribution: we can of course only access one world at a time by measurement.

A probability distribution is therefore a set of worlds and their associated probabilities. The uncertainty relations (2) refer to two such sets that can be identified within the same state – the $`|\psi _\theta `$-worlds and the $`|a`$-worlds, both of which sets are found in the (single) state $`|\psi `$. The relations constrain what, given any set of $`|a`$-worlds, the spread of the associated set of $`|\psi _\theta `$-worlds is, and *vice-versa*. They are not in one sense fundamental: for any state we could look at the states of a group generator $`\widehat{A}`$ and the states of the group and work out $`\delta \theta `$, $`W(\widehat{A})`$ and we would find that they satisfy (2). However the relations do tell us more than that: that we would find this for *any* group and its generator in *any* state.

Fundamentally, the relations (2) for a neo-Everettian say that it is impossible physically to have a state whose worlds corresponding to groups and their generators have probability distributions the spreads of which violate (2). Furthermore, this is the kind of interpretation that is given to *all* statistical statements in neo-Everett theory: they are concerning the worlds of a single system and their associated probabilities, which is very different from the standard interpretation. As we shall see below, this will lead to physical conclusions different from the standard interpretation, as probabilistic statements constrain individual systems and not just ensembles.

## 4 Measurements

### 4.1 Joint Measurement

> *The uncertainty principle refers to the degree of indeterminateness in the possible present knowledge of the simultaneous values of various quantities with which the quantum theory deals…*

Ever since these fateful words of Heisenberg \[6, p20\] (and the subsequent notorious microscope exposition), the uncertainty relations have been regarded in large portions of the literature to be fundamentally statements about the joint measurement of non-commuting observables. “You can’t measure position and momentum simultaneously” is a very common statement and, more generally, “you can’t simultaneously measure two non-commuting observables exactly”. Such conclusion are almost invariably drawn from inequalities such as (1) and pose a number of problems555quite apart from – as was pointed out in §3 – the silence of (1) on matters where one or other of the states is an eigenstate..

To begin with, such a statement is, in point of fact, false. It is fairly uncontroversial that if there is a simultaneous eigenstate of two quantities then on any reasonable theory of measurement we will be able to perform a measurement giving us these quantities. Non-commuting observables do not share *complete* sets of simultaneous eigenkets, but nothing stops them sharing *some*. For example \[7, p33\], a system with angular momentum $`l=0`$ is in a simultaneous eigenstate of $`L_x=0`$ and $`L_z=0`$, even though they do not commute.

Furthermore, and fundamentally, the relations (1) (and indeed our relations (2)) are independent of a theory of measurement – they are relations pertaining to statistical distributions. Until a connection is made between the statistics of many measurements and the state of a system in a singular, given measurement situation, these relations can tell us nothing about what is or is not allowed in one measurement. Indeed, on the ‘standard’ view of the relations the distributions referred to are gained by two *separate* sets of multiple measurements on similarly prepared states, there is not a joint measurement in sight.

Our neo-Everett theory does, however, give us the connection between statistics and singular states – *and* a measurement theory666A measurement of the first kind (state preparation), in the $`\{0,1\}`$ basis, would be written:
$$|\mathrm{Ready}(a|0+b|1)a|R(0)|0+b|R(1)|1$$
In words: at the start of the experiment we identify a structure that is a measuring device set to ‘ready’, and a quantum state in a superposition of 0 and 1. Afterwards we see two structures (‘worlds’), one where the readout of the device is ‘0’ and the state of the system under measurement is $`|0`$, and one where they are ‘1’ and $`|1`$. – and thus we are allowed to try and draw some inferences from the uncertainty relations within it.

We concluded in the previous section that the uncertainty relations tell us what set of $`|a`$-worlds corresponds to a given set of $`|\psi _\theta `$-worlds (and *vice-versa*), for the worlds of a single system. We can therefore see that the set of, say, $`|a`$-worlds that corresponds to a single state $`|\psi _\theta `$ cannot be an eigenstate of $`|a`$; that is, within the state in which we can identify a single $`|\psi _\theta `$-world we identify many $`|a`$-worlds. This is true for *all* single $`|\psi _\theta `$\- and $`|a`$\- worlds: there is never a structure in which we can identify only one $`|\psi _\theta `$-world and one $`|a`$-world.

The implications of this for the question of joint measurement are fairly straightforward. A measuring device cannot couple to a world which is both a given $`|\psi _\theta `$-world and an eigenvalue of $`\widehat{A}`$ because such a world does not exist. Such a coupling would be what is meant in our neo-Everett interpretation by ‘measurement’, so we conclude that a joint measurement of $`\theta `$ and $`\widehat{A}`$ is not possible.

We are able in this case, unlike with the relations (1), to be sure that our conclusion is universally valid; as  points out, (1) depends on the actual state being used, but (2) does not. This means we do not have the problems that (1) has – there is no possibility of joint eigenstates or of the relation being meaningless in some states.

The question now is how much of this comes from the uncertainty relations themselves. The simple fact that the states are not jointly measurable comes from their lack of shared eigenkets, and there will be many other states and observables that are not jointly measurable but which are not linked by uncertainty relations. What we can say is that the uncertainty relations relate a sub-set of states which are not jointly measurable to the underlying group structure that connects them. Without the relations they would be disparate phenomena, and the content of the relations is in relating them. Lack of joint measurement is a consequence (in a neo-Everettian framework) of the group structure, but not all states which are not jointly measurable are groups and their generators.

### 4.2 Repeated Measurements

We now move on to a situation that has been linked to the uncertainty relations (although to a lesser extent that joint measurements): repeated measurements. In this situation we perform a $`\theta `$-measurement, then an *a*-measurement, and then a $`\theta `$-measurement. As is well known, we will find that the final measurement of $`\theta `$ bears no relation to the initial. This is often taken to be a consequence of the uncertainty relations: that the two distributions cannot be equally sharp and so somehow the information about the original measurement is lost when the second measurement takes place. In our neo-Everett picture we can see fairly clearly what is going on, which we have represented here in Figure 1.

A brief note is needed first on the figure itself. The worlds represented are those of the measuring device; as the figure makes clear, more than one other world can be identified in what are given here as single lines. The diagonal lines do *not* represent the splitting of worlds (a concept alien to neo-Everett theory); they can be thought of as, in a highly schematic way, showing the passage of time between the state in which we can identify one measuring device-structure, and when we can see two. Note further that we have simplified $`|\psi _{\theta _i}`$ as $`|\theta _i`$. Finally, normalisation is omitted throughout.

We will assume for simplicity that we are dealing with the very restricted sets of observable outcomes $`\theta _1,\theta _2,a_1,a_2`$. The quantities $`\alpha ,\beta ,\gamma ,\delta ,ϵ,\zeta `$ on the diagram are the relative phases of the worlds. For example, the first decomposition comes from:

$`|R(\theta _1)|\theta _1`$ $`=`$ $`\left({\displaystyle \underset{i}{}}|a_ia_i|\mathrm{𝟣}\right).\left(|R(\theta _1)|\theta _1\right)`$
$`=`$ $`a_1|\theta _1|a_1|R(\theta _1)+a_2|\theta _1|a_2|R(\theta _1)`$
$`=`$ $`\alpha |a_1|R(\theta _1)+\beta |a_2|R(\theta _1)`$
We therefore have:
$`\alpha =a_1|\theta _1,\beta =a_2|\theta _1,\gamma =\theta _1|a_1,\delta =\theta _2|a_1,ϵ=\theta _1|a_2,\zeta =\theta _2|a_2`$.

We prepare our state by measuring $`\theta `$. We then take this state as the start of our worlds-decomposition. The measuring device is in the state $`R(\theta _1)`$ and the system $`|\theta _1`$. The state of the system can also be identified, structurally, as a superposition of the two $`|a`$ states; therefore, when a subsequent $`a`$-measurement is carried out we find that we can identify two states of the measuring device – $`|R(a_1)`$ and $`|R(a_2)`$. We now have two measurement worlds, corresponding to the $`|a_1`$ and $`|a_2`$ worlds. Each of these worlds in turn is a superposition of the two $`|\theta `$ states, and so we move to the last part of the diagram. Now if there were no decoherence at measurement, if the phase information between worlds is not lost to the correlations with the environment, then at this stage we would simply add up all four final states to see what our overall structure looks like. Not surprisingly, it all adds up to our initial state $`|R(\theta _1)|\theta _1`$: if there is no decoherence, repeated measurement gets the initial answer the second time around. However, with decoherence the worlds at measurement become independent of each other (for all practical purposes) and cannot interfere. Thus we are left with four structures rather than one by the end of the experiment, and the information about the original state we prepared is lost as this is carried in the phases of the worlds.

## 5 Conclusion

We have analyzed the uncertainty relations in terms of a neo-Everettian picture of quantum mechanics and found that they relate constraints on probability distributions over worlds for single systems. As a consequence we recover a view of the impossibility of joint measurement which is invalid on traditional arguments. We have also clearly analyzed a repeated measurement scenario in terms of neo-Everettian worlds.
We have found that a single world in one basis is a whole set of worlds in another, and each way of decomposing into a worlds-system is equally valid. When the bases are related as group and generator their probability distributions must satisfy the uncertainty relations (2). We have seen that a neo-Everettian interpretation of such statistical relations is fundamentally different from that in the standard interpretation as they refer to single systems not ensembles. This has consequences far beyond the interpretation of the uncertainty relations. To give one example, the concept of quantum information is statistical, its definition using the density matrix of probabilities for the state, so it will have a very different physical interpretation in a neo-Everett theory from in one with an ensemble theory of probability.
The impossibility of joint measurement and the loss of information in repeated measurements that we have seen are not fundamentally *consequences* of the uncertainty relations – they are consequences of the state and how the different distributions are connected. Moreover, there are other pairs of observables not linked by uncertainty relations that are nevertheless not jointly measurable. However the relations do link together as a single set of phenomena that which would otherwise have been disparate, by revealing consequences of the underlying group structure. They are not fundamental, but neither are they empty of interesting content.

### Thanks

Many thanks to Harvey Brown for pointing me in the direction of Uffink’s work, and also for suggesting the term ‘neo-Everettian’ for the interpretation of quantum mechanics used here. Some of the work here was presented at the 12th Annual Foundations of Physics conference, and I am grateful for the comments and suggestions received there.