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# Quantum spin liquids: a large-𝑆 route.

## 1 Introduction

Frustrated magnets have recently become a focus of experimental studies . Frustration disrupts long-range spin order—even at low temperatures—and leads to the formation of a spin-liquid state, in which spins move in a random yet strongly correlated fashion. A very large degeneracy of the classical ground state makes these magnets strongly susceptible to a variety of perturbations  and thereby leads to a plethora of possible thermodynamic phases. It is also thought that the interplay of strong correlations and quantum effects may yield quantum ground states without magnetic order. Low-temperature properties of such magnets will be quite distinct from those of the familiar Bose or Fermi liquids. Therefore quantum ground states and low-energy excitations of frustrated magnets arouse considerable interest.

The ultimate example of strong frustration is the Heisenberg antiferromagnet on the pyrochlore lattice . In magnets of this kind spins form a three-dimensional network of corner-sharing tetrahedra (Fig. 1). A nearly perfect realization of this model is found in ZnCr2O4  where Cr3+ ions have spin $`S=3/2`$. Recent theoretical studies of such systems have concentrated on the case $`S=1/2`$ , for which the quantum effects are most prominent.

The purpose of this paper is to demonstrate viability of an alternative approach: the large-$`S`$ route. There are several reasons to take this circuitous path. First, the method provides a systematic way to study quantum effects as a function of $`S`$. Second, because the very concept of a frustrated magnet is defined in the classical context, staying close to the classical limit puts the discussion on firmer ground. Third, magnets of this kind have propensity toward spin-Peierls order even in the classical limit . Therefore, there is a reasonable chance of finding nonclassical states—such as valence-bond solids and liquids—in pyrochlore antiferromagnets at large $`S`$.

It must be realized that the large-$`S`$ problem is highly nontrivial: the starting point ($`S=\mathrm{}`$) has an extensive degeneracy . The original problem for the three-dimensional pyrochlore lattice remains unsolved. Below I describe a few positive results that have been obtained recently for homologues of the pyrochlore antiferromagnet in one and two spatial dimensions. Sec. 2 outlines a degenerate perturbation theory, due to Henley, that is based on a series expansion in powers of $`1/S`$. To the first order in $`1/S`$, the theory yields a valence-bond solid for one two-dimensional “pyrochlore” and a valence-bond liquid for another. By design, the ad hoc series expansion misses effects nonanalytical in $`1/S`$ (cf. Haldane’s gap). Sec. 3 describes such an effect in a one-dimensional “pyrochlore” chain with a spin-Peierls ground state. In that model, the quantum melting of a valence-bond solid produces qualitatively different valence-bond liquids for integer and half-integer spins.

## 2 A $`1/S`$ expansion for antiferromagnets on pyrochlore-like lattices

The starting point of the $`1/S`$ expansion is the limit $`S\mathrm{}`$. The ground states are found by minimizing the exchange energy $`J_{ij}(𝐒_i𝐒_j)=𝒪(S^2)`$ with respect to classical Heisenberg spin variables $`\{𝐒_i\}`$. In the case of the pyrochlore antiferromagnet, the total spin of every tetrahedron must vanish (Fig. 1). A simple counting argument  reveals that the manifold of classical vacua is formidably large: it contains one continuous degree of freedom per tetrahedron.

The next term in the $`1/S`$ expansion contains a quantum correction coming from zero-point fluctuations of spin waves :

$$E^{(1)}=\mathrm{const}+\underset{a}{}\frac{1}{2}\mathrm{}\omega _a=𝒪(S),$$
(1)
where $`\{\omega _a\}`$ are spin-wave frequencies. Because magnon spectra are not the same in different ground states, the quantum correction (1) lifts the classical degeneracy. Ordinarily, quantum fluctuations select a few collinear ground states related to each other by symmetries of the lattice . In some special cases, the residual degeneracy may be quite large and not linked to any obvious lattice symmetry .

The pyrochlore lattice presents such an exception: Henley has found that an infinite number of collinear states are selected by zero-point fluctuations . These vacua are not related to each other by lattice symmetries and most are not even periodic. The exact number of the degenerate ground states is not known. This accidental degeneracy has been linked by Henley to certain transformations that leave the spin-wave spectrum $`\{\omega _a\}`$ invariant. The transformations consist of flipping every spin on a (potentially infinite) subset of tetrahedra.

To determine which of the colinear ground states have the lowest zero-point energy, Henley has expressed the sum over the spin-wave frequencies (1) as the trace of an operator dependent on the spin values in a given ground state. The result can be expanded as an infinite sum of multi-spin potentials. In a collinear spin configuration polarized along $`\widehat{𝐧}`$, this interaction can be expressed in terms of Ising variables $`\sigma _i=(𝐒_i\widehat{𝐧})/S=\pm 1`$, subject to the constraint

$$_{i=1}^4\sigma _i=0\text{ on every tetrahedron.}$$
(2)
The zero-point energy reads

$$E^{(1)}=\frac{3}{8}JS\underset{\mathrm{}}{}\underset{i=1}{\overset{6}{}}\sigma _i+\mathrm{}\text{(pyrochlore lattice).}$$
(3)
The six-spin interaction couples spins residing around regular hexagons that exist in the pyrochlore lattice (Fig. 1). The omitted terms, representing multi-spin interactions of higher orders, are not necessarily small. However, at least in the two-dimensional models discussed below, their omission does not affect the selection of ground states. One can check, with the aid of Henley’s symmetry, that all ground states of the truncated Hamiltonian (3) have the same zero-point energy (1).

The problem of finding the ground states thus reduces to minimizing the multi-spin interaction (3) over the Ising variables $`\{\sigma _i\}`$, subject to the constraint (2). It remains unsolved for the pyrochlore lattice. We have succeeded in solving it for two other lattices built from corner-sharing tetrahedra: the checkerboard and the pyrochlore wafer (Fig. 2). The checkerboard is a projection of the pyrochlore lattice onto a plane. Because it has loops of length 4 (around empty squares), the zero-point potential starts with four-spin interactions :

$$E^{(1)}=\frac{1}{2}JS\underset{\mathrm{}}{}\underset{i=1}{\overset{4}{}}\sigma _i+\mathrm{}\text{(checkerboard).}$$
(4)
For the pyrochlore wafer, a slice of the three-dimensional pyrochlore lattice, the effective zero-point energy is given by Eq. 3.

It is convenient to switch from spin variables $`\sigma _i`$ to bond variables $`\tau _{ij}=\sigma _i\sigma _j=(𝐒_i𝐒_j)/S^2`$, defined for nearest-neighbor links $`ij`$. In terms of these, the constraint (2) requires that exactly two non-adjacent bonds be frustrated ($`\tau _{ij}=1`$) on every tetrahedron. The zero-point effective potentials acquire the following form :

$$\underset{i=1}{\overset{4}{}}\sigma _i=\tau _{12}\tau _{34}=\tau _{23}\tau _{41},\underset{i=1}{\overset{6}{}}\sigma _i=\tau _{12}\tau _{34}\tau _{56}=\tau _{23}\tau _{45}\tau _{61}.$$
(5)
Note that the lattices in question contain two sublattices of tetrahedra and that the multi-spin interactions (5) involve bonds of tetrahedra belonging to the same sublattice—see Fig. 2. Thus the problem reduces to independent minimizations of the bond energies (5) on the two tetrahedral sublattices. Although not every bond configuration $`\{\tau _{ij}\}`$ corresponds to a physical spin configuration $`\{\sigma _i\}`$, those that minimize the bond potentials (5) do yield legitimate spin states .

In the checkerboard case, the bond potential (5) is minimized when every two bonds facing each other across an empty square \[Fig. 2(a)\] are in the same state (e.g., $`\tau _{12}=\tau _{34}=+1`$ and $`\tau _{23}=\tau _{41}=1`$). The ground states of each tetrahedral sublattice fall into two disjoint classes. In one class, which can be called “horizontal stripes”, tetrahedra of a given row are in the same bond state. The frustrated bonds are either all vertical, or all diagonal. Because every row can be in one of the two states, there are $`2^{L/2}`$ vacua for each sublattice. The second class—vertical stripes—is related to the first by a 90-degree rotation of the (sub)lattice. A more detailed derivation will be given elsewhere .

At zero temperature, the system is frozen in one of the striped ground states breaking the rotational symmetry of the lattice. There are two Ising order parameters: each sublattice of tetrahedra independently chooses to have vertical or horizontal stripes. The discrete nature of the order parameter guarantees survival of the long-range order at low temperatures $`T<T_c`$. The stripes will have a finite extent $`\xi 𝒪(\mathrm{}^{a/T})`$ enabling the system to move between ground states with the same orientational order on a time scale of order $`\xi `$. Thermal expectation values for the bond variables $`\tau _{ij}`$ must therefore be averaged over all ground states with a specified orientational order. For example, when both sublattices of tetrahedra have horizontal stripes, the horizontal links always have antiparallel spins ($`\tau _{ij}=+1`$), while all other bonds have uncorrelated spins ($`\tau _{ij}=0`$). Another thermal state, with horizontal and vertical stripes on the two sublattices of tetrahedra, is depicted in Fig. 2(a). This state has antiparallel spins around one half of the empty squares and strongly resembles the valence-bond solid found in the ground state of the $`S=1/2`$ system .

Apart from the number of dimensions, the checkerboard and pyrochlore lattices have one other important difference: on the checkerboard, diagonal bonds are not equivalent to vertical or horizontal ones. This is why the valence-bond order parameter on the checkerboard is of the Ising, rather than $`Z_3`$, type. The pyrochlore wafer \[Fig. 2(b)\] is free from this defect. What classical ground states are selected by quantum fluctuations there?

The 6-spin potential (3) translates into the interaction (5) involving three bonds around a hexagon. Again, the interaction takes place between tetrahedra of the same sublattice. The 3-bond energy is minimized when zero or two bonds are frustrated ($`\tau _{ij}=1`$). While superficially this looks like the ground-state rule for the checkerboard, the properties of the ground states are entirely different. In particular, there is no valence-bond order. Moreover, the connected valence-bond correlations $`\tau _{ij}\tau _{kl}\tau _{ij}\tau _{kl}`$ are extremely short-ranged. This can be proven by mapping the ground states of the bond potential (5) onto classical dimer coverings of the triangular lattice, whose properties are well known .

The mapping is illustrated in Figs. 2(b) and (c). Treat the tetrahedra of one sublattice as sites of a triangular lattice. Every two tetrahedra contributing frustrated bonds to the same hexagon (such as $`\alpha `$ and $`\beta `$) generate a dimer linking the corresponding sites of the triangular lattice. Because each tetrahedron contributes exactly one frustrated bond to some hexagon, every site of the dual lattice is connected by a dimer to another site.

## 3 Nonperturbative effects: the Berry phase

To demonstrate potential significance of effects nonperturbative in $`1/S`$, consider a toy model of four antiferromagnetically coupled spins on a flexible tetrahedron. On a regular tetrahedron, the ground state is a spin singlet with the degeneracy $`2S+1`$. A high degree of symmetry and a non-Kramers degeneracy induce the Jahn–Teller effect. For $`S>1/2`$, the sum of elastic and magnetic energies is minimized by three distorted states. In each of these the “molecule” is flattened along one of its principal axes (left panel of Fig. 3) .

Taking into account the kinetic energy of the atoms introduces tunneling events between the three potential wells. The tunneling splits the degenerate ground states into a singlet and a doublet (middle panel of Fig. 3). The nontrivial result is an oscillatory dependence of the order of the levels on $`S`$: the ground state is a singlet for integer spins and a non-Kramers doublet for half-integer spins.

At large $`S`$, the difference can be traced to a Berry phase acquired by the spins as the system moves between the three distorted states (the right panel of Fig. 3). In the process, depicting one of the potential tunneling paths, three spins make full $`2\pi `$ rotations in the same plane. The overall amplitude thus acquires a geometric phase $`e^{6\pi iS}`$, i.e. $`+1`$ if $`S`$ is integer and $`1`$ if it is half-integer.

Consider now a generalization of this toy model to $`d=1+1`$ dimensions: a chain of such tetrahedra weakly coupled through vibrational modes of the lattice \[Fig. 4(a)\]. The low-energy sector of the model consists of three distorted spin-singlet ground states on each site and can be described by the quantum $`q=3`$ Potts model. Elastic interactions cause the distortions of the tetrahedra to be correlated with one another. Assume, for the sake of the argument, that a uniform distortion of the chain is favored. Then, in the absence of tunneling, the chain has spin-Peierls order with a $`Z_3`$ ferrodistortive order. Low-energy spin-singlet excitations are domain walls with a finite energy gap $`\mathrm{\Delta }`$. As the tunneling $`\mathrm{\Gamma }`$ is turned on, the spin-Peierls order weakens. The singlet energy gap vanishes at a quantum critical point \[Fig. 4(b)\]. The nature of the quantum-disordered phase depends on the sign of the tunneling amplitude $`\mathrm{\Gamma }`$ and thus on whether $`S`$ is integer or half-integer.

The physics of low-energy singlet states is described by the quantum 3-state Potts model with the Hamiltonian

$$H=2\underset{i}{}\left[\mathrm{cos}\left(\frac{2\pi }{3}(\theta _{i+1}\theta _i)\right)+\mathrm{\Gamma }\mathrm{cos}\left(\frac{2\pi }{3}p_i\right)\right].$$
(6)
Here $`\theta _i=0,1,2`$ is the Potts variable, while $`p_i=0,1,2`$ is its conjugate momentum. On the $`\mathrm{\Gamma }>0`$ side, the quantum-disordered state also has a gap to singlet excitations. For $`\mathrm{\Gamma }<0`$, the disordered state is gapless.

It is thus seen that the quantum melting of a valence-bond solid on the chain proceeds in different ways for integer and half-integer spins. The quantum-disorderd phase has gapped singlet excitations when $`S`$ is integer. For half-integer $`S`$, the liquid has gapless excitations in the form of valence-bond fluctuations.

## References


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# Magnetic field dependent transmission phase of a double dot system in a quantum ring

## Abstract

The Aharonov-Bohm effect is measured in a four-terminal open ring geometry based on a Ga\[Al\]As heterostructure. Two quantum dots are embedded in the structure, one in each of the two interfering paths. The number of electrons in the two dots can be controlled independently. The transmission phase is measured as electrons are added to or taken away from the individual quantum dots. Although the measured phase shifts are in qualitative agreement with theoretical predictions, the phase evolution exhibits unexpected dependence on the magnetic field. For example, phase lapses are found only in certain ranges of magnetic field.

In mesoscopic systems the conductance and the quantum mechanical transmission of charge carriers between contacts are intimately related. The corresponding transmission amplitude is a complex number with magnitude and phase. The phase difference of interfering paths in coherent quantum rings can be detected in the conductance by measuring Aharonov-Bohm (AB) oscillations. Keeping the transmission phase of one of the interfering paths constant (reference path), the phase change of the other can be measured. This technique opens the attractive possibility to investigate the transmission phase which contains information about the system complementary to the transmission probability. Multiterminal devices are required for such experiments in order to circumvent the generalized Onsager symmetry relations Buttiker86  restricting the transmission phase to values of 0 or $`\pi `$ in two-terminal devices.

Ring and ring-like interference geometries have been exploited for many types of experiments Yacoby95 ; Buks96 ; Schuster97 ; Ji00 ; Ji02 ; Buks98 ; Sprinzak00 ; Kobayashi02 ; Holleitner01 ; Holleitner02 ; Fuhrer01 . The electronic phase in particular was studied in a series of pioneering publications Yacoby95 ; Buks96 ; Schuster97 ; Ji00 ; Ji02 . The transmission phase through a two-terminal device with a single quantum dot has been investigated Yacoby95  and it was concluded that electron transport through a Coulomb blockaded quantum dot is at least partially phase coherent. The phase of the reflection coefficient of a quantum dot in the integer quantum Hall regime was measured in Ref. Buks96, . Later, the transmission phase of a quantum dot was studied in a multi-terminal configuration Schuster97 . It was found that the transmission phase changes by about $`\pi `$ across a typical Coulomb blockade resonance, as expected. Between resonances the experiment exhibits so-called phase lapses rather than the almost constant phase expected in the simplest model. Similar experiments were carried out on a Kondo-correlated system in Refs. Ji00,  and Ji02, .

A large number of theoretical papers (for a review see Hackenbroich01 ) has addressed the issue of the phase lapses and suggested possible explanations. It was argued that the transmission phase has to be distinguished from the Friedel phase which fulfills a general sum rule and is a monotonous function of energy, while the transmission phase can show phase lapses of $`\pi `$ when the transmission goes through zero Lee99 ; Buttiker99 ; Buttiker00 . It was also pointed out that the measured phase may depend on the details of the entire interferometer, on interactions Koenig02 , and on the dot-lead coupling Silva02 . The phase determined experimentally is the transmission phase through the dot, only if the system is unitary Entin02 , i.e. it couples negligibly to its environment. A tunneling-Hamiltonian approach predicted the phase to be influenced by the number and width of leads connecting to the ring Aharony02 ; Gefen02 . In a scattering matrix approach, however, the limit of many occupied modes in the channels reflects the energy dependence of the resonance phase shift Weidenmuller02 . The equivalence of the tunneling-Hamiltonian formulation and the scattering matrix approach are discussed in Kubala02 . Theoretical proposals have considered the situation of two quantum dots in an AB interferometer and the possible coupling of the dots via phase coherent transport through the leads Konig02 ; Kubala02b . In the context of spintronics two coupled quantum dots in an AB interferometer may be used for detecting entanglement of spin states Loss00 .

Here we investigate the phase evolution of a system of two quantum dots with negligible mutual electrostatic interaction embedded in two arms of a four-terminal AB ring. Phase measurements in this unique system are desirable, because both arms of the ring including the two dots can be tuned individually, but the phase coherence of the entire system provides an inherent coupling mechanism Konig02  and makes transport through the dots interdependent. The arrangement enables us to control and analyze the effect of the interferometer reference arm on the measured phase experimentally. The phase evolution of the system is studied when a single electron is added to either of the two quantum dots, to both quantum dots simultaneously, or when an electron is transferred from one dot to the other. The observed phase shifts agree qualitatively with theoretical expectations at elevated magnetic fields. Unexpectedly, the phase evolution is found to depend on the magnetic field and occasional phase lapses occur in certain field ranges. These observations highlight the need to consider nonlocal coherent effects in the entire system.

The sample is a Ga\[Al\]As heterostructure containing a two-dimensional electron gas 37 nm below the surface. The lateral pattern was fabricated with the biased tip of an atomic force microscope which locally oxidizes the GaAs surface. Details of this fabrication technique are described in Ref. Held99, . Figure 1(a) shows a micrograph of the oxidized pattern. Lateral gate electrodes marked pg1 through pg4 are used to tune the conductance in each of the four quadrants of the ring. All measurements were carried out at 100 mK in a dilution refrigerator.

The ring was characterized in the open regime where each quadrant supports 2-4 lateral modes. A pronounced AB effect is observed in a local measurement setup in which the current and voltage contacts are the same two terminals of the ring Sigrist03 . The AB signal is maximized with a non-local setup: a bias voltage $`V_{\mathrm{bias}}`$ was applied to terminal A \[see Fig. 1(b)\]. The lower and upper contacts (B and D) were grounded via current-voltage converters measuring the currents $`I_\text{B}`$ and $`I_\text{D}`$. The non-local voltage $`V_{\mathrm{nl}}`$ was measured at terminal C. Figure 1(c) shows the AB oscillations in $`V_{\mathrm{nl}}`$. Their period $`\mathrm{\Delta }B=\mathrm{\Phi }_0/A=4.8`$ mT is consistent with the area $`A=0.85`$ $`\mu `$m2 of the ring.

If any individual segment is tuned close to pinch off with a negative voltage applied to the corresponding plunger gate, a quantum dot is induced exhibiting Coulomb blockade. As an example, Fig. 1(d) shows the conductance of segment 1 \[A to D in Fig. 1(b)\] as a function of $`V_{\mathrm{pg1}}`$ with segment 3 completely pinched off and segments 2 and 4 open. Clear Coulomb blockade oscillations are observed. The location of the quantum dot can be estimated from the lever arms of gates pg1 to pg4. The dots form within the segments and not at the openings to the contacts. From Coulomb blockade diamonds measured as a function of forward bias we find a typical Coulomb charging energy of 1 meV, which corresponds in a disc capacitor model roughly to the area of a single segment. More details about the characterisation of the ring can be found in Ref. Sigrist03, .

We proceed to study Coulomb blockade in the measurement configuration of Fig. 1(a). For the following experiments we have carefully chosen a series of conductance peaks of one well defined quantum dot in segment 1 (dot 1) and another one in segment 2 (dot 2). Segments 3 and 4 are open. The current signals $`I_\text{B}`$ and $`I_\text{D}`$ are shown in color as a function of the gate voltages $`V_{\mathrm{pg1}}`$ and $`V_{\mathrm{pg2}}`$ in Figs. 2b and c. The current $`I_\text{B}`$ ($`I_\text{D}`$) shows predominantly the Coulomb maxima of the dot in segment 2 (segment 1) while those of the other dot are much weaker. The non-local voltage in Fig. 2(a) displays clear signatures of conductance resonances of both quantum dots. The lever arm of gate voltage 1 (2) on the dot in segment 2 (1) is about a factor of six smaller than for the direct gate voltage. There are stripes with an intermediate slope in all three quantities which we attribute to the formation of standing waves between the two quantum dots near lead A. This resonator is coupled in series to both quantum dots, a fact which leads to a corresponding modulation of the dot currents in certain ranges of gate voltages and magnetic fields.

In order to study the phase evolution of the transmission through the quantum dots we measure $`V_{\mathrm{nl}}`$ as a function of magnetic field. The results presented below were obtained in a regime where the coupling to the leads was strong enough, but the dots were still well defined. By tuning $`V_{\mathrm{pg1}}`$ and $`V_{\mathrm{pg2}}`$ we follow the trace labeled ‘linear2’ in Fig. 2(a), staying on a conductance maximum in dot 1 while stepping through a conductance peak in dot 2. As shown in Fig. 3(a) the current $`I_\text{B}`$ shows the expected Coulomb peak of dot 2 as a function of plunger gate voltage, while $`I_\text{D}`$ changes little. At each gate voltage setting the AB oscillations are measured. The non-local voltage in Fig. 3(b) shows a pronounced AB signal which is strongest in the range of the conductance maximum. A set of specific traces of $`V_{\mathrm{nl}}`$ versus magnetic field is depicted in Fig. 3(c). The vertical lines connect minima in the lowest trace with maxima in the uppermost trace. This corresponds to a phase shift of $`\pi `$.

The multi-probe conductance formula Buttiker86  gives for the non-local voltage in our setup:

$$V_{\mathrm{nl}}=\frac{T_{\text{CA}}}{T_{\text{CC}}}V_{\mathrm{bias}}.$$

The transmission coefficients $`T_{ij}`$ from probe $`j`$ to $`i`$ are named according to Fig. 1(b). Considering only oscillations with a periodicity of $`h/e`$ we assume $`T_{\text{CC}}=_{i\text{C}}T_{\text{C}i}`$ to be constant. In this case AB oscillations in $`V_{\mathrm{nl}}`$ reflect the interference contribution to $`T_{\text{CA}}`$ from which the phase difference between the two interfering transmission amplitudes can be directly read Schuster97 . In contrast, phase changes seen in the two currents do not directly reflect the difference of transmission phases of the dots. In the following we therefore consider only phase shifts of the AB oscillations in $`V_{\mathrm{nl}}`$.

We have analyzed such phase shifts quantitatively for all four traces indicated by the arrows in Fig. 2(a). The fast Fourier transform of each magnetic field sweep was multiplied with the filter function $`f(\omega )=(\sigma \omega )^2/2\mathrm{exp}[1(\sigma \omega )^2/2]`$ with $`\sigma =h/(e\sqrt{2}\pi A)`$ in order to obtain the pure $`h/e`$-periodic contribution. The inverse fast Fourier transform of the filtered data gives the oscillatory component of $`V_{\mathrm{nl}}`$ as a function of magnetic field which is plotted in Fig. 4. We have verified that this filtering procedure does not influence the phase of the AB oscillations by carefully comparing filtered data with raw data.

We begin the discussion with Fig. 4(a) corresponding to trace ‘linear2’ in Fig. 2(a). The dashed horizontal line indicates the maximum in $`V_{\mathrm{nl}}`$ averaged over $`B`$. The AB amplitude is strongest close to this line, as expected, but displays a pronounced $`B`$-dependence, i.e. it is significantly larger for $`B>30`$ mT than below. The phase shift can be directly read from the shift of AB maxima or minima as a function of $`V_{\mathrm{pg2}}`$. The general trend is a shift to larger magnetic fields with increasing $`V_{\mathrm{pg2}}`$. The expected phase shift of $`\pi `$ across the conductance resonance is clearly discernible for $`B>50`$ mT. However, there is a dip in the AB amplitude at $`V_{\mathrm{pg2}}68`$ mV which has a strong phase shift associated with it. At $`B40`$ mT and $`V_{\mathrm{pg2}}68`$ mV \[arrow in Fig. 4(a)\] the AB amplitude is zero and a phase lapse of $`\pi `$ can be identified. This phase lapse lies in the flank of the peak of the field averaged $`V_{\mathrm{nl}}`$ and occurs at a point of zero AB amplitude, similar to the phase lapses observed in Ref. Schuster97,  and in agreement with the general theoretical discussion of phase lapses in Ref. Buttiker99, . The novel aspect here is the occurrence of the phase lapse only in a limited range of magnetic field. Beyond this field range the phase lapse disappears in favor of a continuous phase evolution of order $`\pi `$.

Along trace ‘diag1’ in Fig. 2(a) an electron is added to both dots simultaneously. In this case we expect a phase shift of $`\pi \pi =0`$ since the phase difference between the arms of the ring remains constant. In the experiment the phase shift in Fig. 4(b) is indeed small for $`B>50`$ mT, it amounts to about $`\pi /10`$. At lower fields, however, phase lapses and related strong phase shifts occur like that observed for trace ‘linear2’.

When we measure along trace ‘linear1’ \[Fig. 4(c)\] the gross trend of the phase shift differs in sign from that in Fig. 4(a), in agreement with the fact that we tune the dot in the other segment. In the coupling regime of the quantum dots where AB oscillations are observable, Coulomb resonances can occur close to each other. This is the case for this sweep as indicated by the two dashed blue horizontal lines in Fig. 4(c). In such a case the question arises how the transmission phases of individual resonances combine to the observed phase shift. In our measurement we find that the phase accumulation across the first resonance just above $`V_{\mathrm{pg1}}=60`$ mV is about $`\pi `$ for $`B`$ between 30 and 70 mT, as expected. At higher fields the phase shift weakens. At $`V_{\mathrm{pg1}}55`$ mV and between -40 and -50 mT, phase lapses occur which influence the phase evolution at higher magnetic fields but cannot compensate the accumulated phase completely. At the top edge of the figure, the second resonance leads to a further phase accumulation in the same direction as the first.

Along trace ‘diag2’ \[Fig. 4(d)\] an electron is removed from dot 2 and added to dot 1. As expected, AB oscillation maxima shift in the same direction as in ‘linear1’. However, at $`B=80`$ mT, for example, the phase accumulated between $`V_{\mathrm{pg1}}=68`$ mV and $`56`$ mV is only slightly more than $`\pi `$ rather than $`2\pi `$. Again, the phase evolution is influenced by occasional phase lapses.

Summarizing the observations we can make the following statements. We have succeeded in measuring the AB phase in a four terminal quantum ring with two dots embedded in two different segments. The AB oscillations tend to be well developed and suitable for phase measurements only at slightly elevated magnetic fields. In the range between 50 and 80 mT the expected phase shifts across Coulomb-blockade resonances are typically observed. Phase lapses occur occasionally in finite magnetic field ranges at specific gate voltages. They are accompanied by a vanishing AB amplitude. Even outside the $`B`$-ranges where phase lapses occur, the phase evolution can be strongly modified by their presence. Following the argument of Büttiker and coworkers Buttiker99 ; Buttiker00 , the transmission amplitude follows a certain curve in the complex plane as a function of gate voltage. A phase lapse accompanied with a zero in transmission occurs when this line goes through the origin. A change in magnetic field may shift this curve a little leading to a strong, but continuous phase shift accompanied with small transmission. The appearance of phase lapses in finite magnetic field ranges impedes the definition of a magnetic field independent transmission phase. A conceivable origin of the phase lapses is the finite width of the ring segments accommodating several modes. In the magnetic field range investigated, the classical cyclotron radius is larger or comparable to the ring radius. A small influence of Lorentz force effects cannot be excluded at the highest fields.

Our samples differ from those in Ref. Schuster97,  by design and in view of the technological approach. We have adopted the general idea of using reflecting walls to guide the electrons ballistically around the ring without loosing too many of them into the contacts. Compared to Ref. Schuster97  the most noticeable feature of our structure is the second dot in the reference arm. Its addition gives individual control over the accumulated phases in both arms. Since the reference dot is kept on a conductance resonance, i.e. in the position of maximum slope of the phase evolution, while the other is swept through a resonance, the reference dot is very sensitive to phase changes. Should the reference dot be tuned slightly off its resonance during the sweep ‘linear 2’, one would expect a pronounced influence on the measured phase evolution. The fact that we still observe a phase change of about $`\pi `$ on trace ‘linear2’, when dot 2 is tuned through a conductance resonance, lets us conclude that the transmission phase through dot 1 is rather stable and the observed phase shift is dominated by dot 2.

In this experiment, the transmission phase was measured in a system where two Coulomb blockaded quantum dots are embedded in a four-terminal quantum ring. We have shown that the phase evolution can be determined with individual control over the electron occupancy in each dot. The experiments demonstrate that the measured transmission phase depends on the magnetic field range analyzed. Phase lapses can arise at certain magnetic fields, while at others they give way to a continuous phase evolution. In certain magnetic field ranges the phase behavior is in agreement with theoretical expectations, but its behavior is much more complex than anticipated. This possibly suggests that structural resonances, in addition to the dots, play a role in the overall transmission phase of the system.

###### Acknowledgements.

We thank M. Büttiker, Y. Gefen, M. Heiblum, H. Weidenmüller for valuable discussions. Financial support by the Swiss Science Foundation (Schweizerischer Nationalfonds) is gratefully acknowledged.


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# Coulomb three-body systems and charge transfer collisions in a configuration-space approach

## Abstract

Some low-energy three-body muon- and electron-transfer processes are considered within the Faddeev-Hahn formulation using two-, six-, and ten-state close-coupling approximation. We test our approach in bound-state problems for systems H$`{}_{}{}^{+}{}_{2}{}^{}`$ and ($`\mu ^{}`$dd)+ within six- and ten-state schemes, where $`d`$ is a deuteron and $`\mu `$ a muon. We present results in the six-state model for muonium formation from hydrogen. We also present results for muon-transfer rates from muonic hydrogen isotopes to bare nuclei S16 and Ar18 in reasonable agreement with experiment. For these heavier targets a polarization potential is included and Coulomb potentials are treated exactly without approximation or cut off.

A theoretical description of low-energy three-body rearrangement reaction with the exchange of a heavy particle invalidates the simplifying Born-Oppenheimer approximation and requires a full quantum treatment. Here we study several three-body charge-transfer reactions and bound-state problems using the Faddeev-Hahn formulation  where the full wave function is broken into two components. In the case of three charged particles composed of positive and negative charges there are at most two asymptotic two-cluster bound configurations. The two components of the wave function carry the asymptotic boundary condition in these two channels. For numerical treatment we employ two-, six-, and ten-state close-coupling schemes.

After testing the approach to the bound states H$`{}_{}{}^{+}{}_{2}{}^{}`$ and ($`\mu ^{}`$dd)+ we consider charge-transfer reactions. Hydrogen has three isotopes: protium H, deuterium D, and tritium T. It may be an important test for any formulation to predict reaction rates as a function of isotopes. Muonium (Mu) is composed of a positive muon $`\mu ^+`$ and an electron and can be treated as an ultra-light hydrogenic isotope compared to protium, deuterium and tritium, because the proton is about nine times heavier than the muon. Because of differences in mass, muonium formation can demonstrate rather different dynamical properties than the reactions of other isotopes of hydrogen. For this reason we consider the reaction for muonium production in muon-hydrogen collision: $`\mu ^++\text{H}_{1s}\text{Mu}_{1s}+`$ H+.

Due to interest in the possibility of muon-catalyzed fusion of the hydrogen isotopes, a study of muon transfer from hydrogen isotopes to nuclei XZ+ with charge $`Z`$ is of great interest. There have been several experimental measurements of muon transfer from muonic hydrogen isotopes 1Hμ and 2Hμ to bare nuclei H, He, C, O, Ne, S, Ar, Kr, Xe etc. denoted by (Hμ)1s \+ XZ+ $``$ (Xμ)(Z-1)+ \+ H+. The rates increase by few orders of magnitude as one moves from the light nuclei H, He to the heavy ones. These reactions are very relevant as a small contamination of these heavier elements will significantly influence the process of muon-catalyzed fusion of hydrogen isotopes. Muon-transfer reaction with these nuclei has very strong final-state Coulomb interaction and is a real challenge to any theoretical formulation. Here we report results for muon transfer rates for S16+ and A18+.

The well-known Faddeev equations in momentum space  are supposed to be the most adequate way of considering rearrangement scattering problems at low energies. However, a direct application of the integral Faddeev equations to Coulombic three-body systems is impossible due to long-range character of the Coulomb interaction. The Coulomb interaction brings in significant singularities in the kernels of these equations.

Recently, we formulated a few-body quantum-mechanical description of direct charge-transfer reaction from hydrogen to different nuclei using Faddeev-Hahn-type equations in the close-coupling approximation . In this approach the three-body wave function is taken as $`\mathrm{\Psi }=\mathrm{\Psi }_1(\stackrel{}{r}_{23},\stackrel{}{\rho }_1)+\mathrm{\Psi }_2(\stackrel{}{r}_{13},\stackrel{}{\rho }_2),`$ where $`\stackrel{}{r}_i,i=1,2,3`$ is the position vector of particle $`i`$, $`\stackrel{}{r}_{ij}=\stackrel{}{r}_i\stackrel{}{r}_j`$, and $`\stackrel{}{\rho }_k`$ is the relative position of $`k`$ from the center of mass (cm) of $`i`$ and $`j`$. Here $`\mathrm{\Psi }_1(\stackrel{}{r}_{23},\stackrel{}{\rho }_1)`$ is quadratically integrable over the variable $`\stackrel{}{r}_{23}`$, and $`\mathrm{\Psi }_2(\stackrel{}{r}_{13},\stackrel{}{\rho }_2)`$ over the variable $`\stackrel{}{r}_{13}`$. These components satisfy the Faddeev-Hahn equations

$`(EH_0V_{23}U_P)\mathrm{\Psi }_1(\stackrel{}{r}_{23},\stackrel{}{\rho }_1)`$ $`=`$ $`(V_{23}+V_{12}U_C)\mathrm{\Psi }_2(\stackrel{}{r}_{13},\stackrel{}{\rho }_2),`$ (1)
$`(EH_0V_{13}U_C)\mathrm{\Psi }_2(\stackrel{}{r}_{13},\stackrel{}{\rho }_2)`$ $`=`$ $`(V_{13}+V_{12}U_P)\mathrm{\Psi }_1(\stackrel{}{r}_{23},\stackrel{}{\rho }_1).`$ (2)
Here $`H_0`$ is the total kinetic energy operator, $`V_{ij}`$ the pair Coulomb potential, $`E`$ the total cm energy, $`U_P=9Z^2/(4\rho ^4)`$ the polarization potential (included with a short-range cut off for only muon transfer to Ar and S), $`U_C`$ the final-state Coulomb interaction between 2 and bound state (13). The close-coupling equations based on these equations are projected on the total angular momentum $`J=0`$ appropriate at low energies and then solved numerically by discretization.

For the binding energy of H$`{}_{}{}^{+}{}_{2}{}^{}`$, the present 6- \[2$`\times `$(1s-2s-2p)\] and the 10-state \[2$`\times `$(1s-2s-2p-3s-3p)\] approximations to the close-coupling expansion produce 0.66 au and 0.62 au, respectively, compared to the accurate result of 0.597139 au . For the spectral levels of the muonic molecular ion $`(\mu ^{}dd)^+`$ the six- and ten-state models lead to $`326.4`$ eV and $`325.2`$ eV, respectively, for the ground-state energy compared to the accurate variational result of $`325.0735`$ eV . The corresponding numbers for the lowest excited state are $`33.1`$ eV, $`35.0`$ eV, and $`35.8444`$ eV , respectively.

Cross sections $`\sigma _{ex}`$ for muon production are presented in Fig. 1 as function of $`k^{(2)}=3.7\times \sqrt{E(\text{eV})}`$ together with the theoretical results of work . There is substantial difference between the two calculations at low energies. We found that the contribution of $`p`$-waves in sub-systems is reasonable and ranges up to $`2040\%`$.

Finally, we present the results of muon transfer from H isotopes to Ar and S. In this case the transfer takes place mostly to two levels of the muonic nuclei and we consider only these two levels in the present calculation. The muon is captured predominantly in the 10$`s`$ and $`10p`$ states of Ar and $`9s`$ and $`9p`$ states of S . We compare the results in Table 1 with available experiments quoted in Ref. . The correct order of magnitude for the rates is already produced without a polarization potential. A previous calculation of muon-transfer rates to lighter nuclei (He, C, O)  is also in agreement with experiment and a very recent calculation . From this and previous studies  we conclude that the present formulation is equally suitable for bound states as well as three-body charge transfer reactions involving large final-state Coulomb interaction.


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# Spin singlet formation in MgTi2O4: evidence of a helical dimerization pattern

## I Figure captions

Fig. 1 Bottom: The synchrotron x-ray diffraction pattern of MgTi2O4 at background level taken at 200K, $`\lambda =0.5`$Å (the strongest line has an amplitude of 32000 counts). The top to bottom rows of ticks mark the positions of MgTi2O4, Ti2O3 and MgO Bragg peaks respectively. The triangles mark the superlattice reflections, the circles mark an unidentified impurity. The inset shows a portion of the refined high-resolution neutron diffraction pattern of MgTi2O4 at 200K. The top and bottom rows of ticks mark the positions of MgTi2O4 and Ti2O3 Bragg reflections respectively. The splitting of the cubic peaks is apparent upon comparison to the spinel pattern taken at 275K. Top: The tetragonal lattice constants of MgTi2O4 and Ti-Ti bond lengths as functions of temperature. The solid lines are guides for eye.

Fig. 2 The Ti-Ti bond structure in tetragonal MgTi2O4 at 200K. The red and purple bonds represent the shortest (dimerized) and the longest bonds in the MgTi2O4 structure respectively. The dashed and solid blue bonds mark the intermediate $`i_1=3.002(5)`$Å and $`i_2=3.0099(3)`$Å Ti-Ti distances respectively. A portion of the Ti tetrahedral connectivity is also shown. The inset shows a fragment of the spinel structure in the same orientation, visualized using cation-anion polyhedra. One of the ‘helices’ is outlined in yellow.

Fig. 3 Electronic density of states (DOS) for cubic (top) and the tetragonal (bottom) MgTi2O4. The contribution of Ti and O is indicated with different line styles (the Mg contribution to DOS in negligible in this energy range). The vertical line marks the Fermi energy.