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# How did the metals in a giant star originate?

*Nature* 422 (2003), (issue 24 April)

The chemical composition of stars with extremely low metal contents (taking “metals” to mean all elements other than hydrogen and helium) provides us with information on the masses of the stars that produced the first metals. Such a direct connection is not possible, however, if the surface of the star has been polluted by enriched material, either dredged from the star’s interior or transferred from a companion star. Here we argue that, in the case of HE0107-5240 (ref. 1), the most iron poor star known, the oxygen abundance could be a discriminant: a ratio of \[O/Fe\] exceeding +3.5 would favour a pristine origin of metals, whereas an \[O/Fe\] ratio of less than +3 would favour the pollution hypothesis. Using this criterion, we suggest how the required information on oxygen abundance might be obtained.

HE0107-5240 shows carbon, nitrogen and sodium enhanced, respectively, by factors of $`10^4`$, $`10^{2.3}`$ and 10 relative to iron,whereas magnesium, which is usually more abundant in metal-poor stars, is present in almost the same amounts as iron; no single supernova (SNII) model seems to show this pattern\[¡2¿\]. Although several models may be worth considering, we evaluate two here: a pristine origin due to the combined enrichment of at least two SNIIs, or a pollution of the surface of the star after its formation.

If the metals are pristine, then HE0107-5240 must have formed from a cloud enriched by the ejecta of at least two zero-metallicity SNIIs of quite different initial masses. The first supernova, which was presumably rather massive, would have produced the light elements observed in HE0107-5240, but none of the heavier ones, because of an extensive fallback, up to the base of the helium shell. This would have prevented the ratios \[C/N\] and\[Mg/C\] from becoming too high. The second supernova, which was less massive,would have provided all of the elements heavier than and including magnesium.

In the case of pollution enrichment, on the contrary, HE0107 -5240 would be either a low-mass, zero-metallicity star that accreted matter enriched by the first generation of SNII, or a second-generation low-mass star of very low metallicity. The high \[C,N,Na/Fe\] ratios would be the result of subsequent enrichment of the surface of the star, due either to an internal process or to the accretion of matter synthesized by an Asymptotic Giant Branch (AGB) star in a binary system.

One way to discriminate between pristine and pollution origins of C and N is to measure the abundance of oxygen. In the pristine case, the more massive supernova would provide a large amount of oxygen, leading to a high \[O/Fe\] ($`>+3.5`$), as can be derived from the yields of zero-metal massive stars\[¡2¿\]. In the pollution case, a lower \[O/Fe\] is expected ($`<+3.0`$), as implied by the yields of zero-metal, intermediate-mass stars\[¡3¿\]. An upper limit of 0.1 pm (where 1 pm is $`10^{12}`$ m) on the equivalent width of the \[OI\] 630-nm line would provide a limit on oxygen, namely \[O/H\] $`<+2.3`$ or \[O/Fe\] $`<+3`$. With the Ultraviolet Visual Echelle Spectrograph on the 8.2m VLT telescope, we estimate that such a limit could be achieved in about 30 h of exposure. The situation is slightly better for OH ultraviolet lines, for which we estimate that an upper limit of \[O/Fe\] $`<+2.0`$ could be derived even at moderate signal-to-noise

ratios ($`>20`$), which should be achieved in about 4 h of exposure. At this signal-to-noise ratio, discrimination between \[O/Fe\]$`<+3.0`$ and \[O/Fe\]$`>+3.5`$ is possible; however, lower oxygen abundances would be very difficult to measure, whatever the signal-to-noise ratio. As high-resolution spectra have already been obtained,including the ultraviolet region containing the OH lines, for a total of about 30 h of exposure (ESO/ST-ECF Science Archive Facility), it may now be possible to carry out the test that we propose.

Among extremely metal-poor stars, oxygen has been observed only in CS 22949-037 (ref. 4), for which \[O/Fe\]=+2.0; all other known stars have oxygen features that are below the detection threshold. However, CS 29498-043 (ref. 5) has a very similar pattern of marked overabundance of the lighter elements; its oxygen abundance, which has not yet been measured, may prove to be strongly enhanced as well.

We note that the high \[C/N\] observed in HE0107-5240 is difficult to explain in terms of pollution, whether internal or from an AGB companion, because of the high abundance of primary nitrogen in both cases. We argue that a pristine origin is more likely, which implies that the \[O/Fe\] ratio is higher than in any other known metal-poor star.


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# Robust Quantum Computation with Quantum Dots

## Abstract

Quantum computation in solid state quantum dots faces two significant challenges: Decoherence from interactions with the environment and the difficulty of generating local magnetic fields for the single qubit rotations. This paper presents a design of composite qubits to overcome both challenges. Each qubit is encoded in the degenerate ground-state of four (or six) electrons in a system of five quantum dots arranged in a two-dimensional pattern. This decoherence-free subspace is immune to both collective and local decoherence, and resists other forms of decoherence, which must raise the energy. The gate operations for universal computation are simple and physically intuitive, and are controlled by modifying the tunneling barriers between the dots—Control of local magnetic fields is not required. A controlled-phase gate can be implemented in a single pulse.

A quantum computer with a sufficient number of quantum bits “qubits” (on the order of 1000) would be able to solve certain problems that are intractable on classical computers. Building such a device is a formidable task, and several radically differing designs have been proposed nielsen00 . One promising approach is to encode quantum information using the spin of single electrons confined in semiconductor quantum dots loss98a ; burkard99a ; hu00a ; friesen03a . Universal quantum computation divincenzo95b ; barenco95a  in this approach uses a tunable kinetic exchange interaction between the dots (resulting in a Heisenberg interaction) and one-qubit rotations, which can be obtained by applying local magnetic fields in at least two directions.

The one-qubit rotations are much more difficult to control experimentally than the kinetic exchange interaction. This spurred a number of proposals of quantum computation schemes using the exchange interaction alone divincenzo00a ; kempe01b ; levy02a ; lidar02a ; bacon00a ; lidar00a . To use this single interaction, the quantum information must be encoded in multiple (two or more) spins.

Decoherence due to interactions with the environment pose a much larger problem for qubits than for classical bits, and there has been a tremendous effort on developing ways of protecting quantum information from decoherence bacon00a ; lidar00a ; gottesman96a ; knill97a ; calderbank97a ; duan97a ; kane98a ; burkard99b ; steane99a ; viola00a ; ioffe02a ; meier03a ; wu02a . To shield quantum information from the environment, Zanardi and Rasetti zanardi97a  first proposed encoding quantum information in in the “noiseless” singlet subspace of 4 (or more) 2-level systems. This subspace, often called a Decoherence Free Subspace (DFS), is immune to collective decoherence, that is, environment-induced dephasing that acts equally on each constituent element of the composite qubit bacon00a ; lidar00a ; kielpinski01a ; lidar98a ; lidar99a ; kempe01a ; lidar03a .

Bacon, Brown, and Whaley (BBW) proposed creating a supercoherent qubit from the 4-spin DFS by generating an energy gap from the singlet subspace to the rest of the Hilbert space bacon01a . Decoherence must overcome this energy gap and is suppressed exponentially for temperatures much smaller than this gap barnes00a . To create the gap, BBW use equal antiferromagnetic interactions between all pairs of four $`s=1/2`$ spins. The Hamiltonian is simply $`𝐇=J_{i<j}𝐒_i𝐒_j`$, and the eigenvalues $`E(S)=(J/2)(S(S+1)3)`$ depend only on the total spin $`S`$. The quantum information is encoded in the doubly degenerate singlet ground state.

Building four quantum dots with equal tunneling rates between each pair is challenging. Tunneling rates decay exponentially with the separation between dots. Arranging the dots on the vertices of a three-dimensional tetrahedron would work, but it is far preferable to build two-dimensional structures. A square arrangement will have much weaker tunneling across the diagonal of the square than along the edges of the square.

We propose adding an extra dot (and not an extra electron) in the middle of a square arrangement of four dots, as shown in Fig. (1). We separate the outer four dots so the direct tunneling between them is negligible. Since the ground state wave function of the middle dot will have $`s`$-wave character, the effective interaction between each pair of the outer four dots will be equal if the four tunnelings between the outer and middle dots are made equal (e.g. by tuning gates located above or below each tunneling region).

This design is inspired by the superexchange process, which uses empty (or filled) auxiliary quantum dots to mediate interactions between dots that are too widely separated to interact directly recher00a ; manousakis02a ; auerbach94 . Electrons (or holes) can reach distant quantum dots by hopping through the auxiliary dots.

We need to verify that four electrons can be placed in the five-dot system. We model the system with a Hubbard Hamiltonian using one orbital per quantum dot:

$`H`$ $`=`$ $`{\displaystyle \underset{i,j,\sigma }{}}t_{ij}c_{i\sigma }^{}c_{j\sigma }+{\displaystyle \underset{i}{}}\left(U_in_in_i\mu _in_i\right)`$ (1)
where $`t_{ij}`$ is the hopping amplitude between dots $`i`$ and $`j`$, $`U_i`$ is the Coulomb repulsion between two electrons on dot $`i`$, $`n_i=n_i+n_i`$ is the total number of electrons on dot $`i`$, and $`\mu _i`$ is the onsite potential of dot $`i`$ burkard99a . The calculations used $`t_{ij}=1`$, $`U_i=8`$, and an equal overall potential on each dot of $`\mu _i=\mu `$. The total occupancy of the ground state of the system calculated by exact diagonalization in the grand canonical ensemble is shown in Fig. (2). The largest region of stability contains five electrons, which is to be expected in the large $`U`$ limit, but there are significant ranges of the chemical potential $`\mu `$ for which the ground state has four and six electrons. In these regions, the ground state is a doubly degenerate singlet, and quantum computation in this supercoherent subspace is possible.

The Hamiltonian used to generate Fig. (2) has equal onsite potentials at every dot, and thus has electron-hole symmetry. Raising the potential of just the middle dot breaks this symmetry and increases the range of chemical potentials yielding the $`N=4`$ ground state while lowering this potential increases the range of the $`N=6`$ ground state. Quantum computation is possible using either the $`N=4`$ or $`N=6`$ ground states, and the gate operations for the two cases are identical.

A simple way of describing eigenstates of the 5-dot composite qubit is shown in Fig. (3) using valence-bond representation auerbach94 . The ground states contain two separate singlet bonds. There are three ways to construct these bonds: Dot number 1 is bonded to any of the other three outer dots, and then the other bond is formed between the two outer dots not bonded to dot 1. Valence-bond states are not orthogonal in general, and two orthogonal states may be formed from the three states in Fig. (3). There are several ways to form two orthogonal states, and we will use $`|0=|\mathrm{a}`$ and $`|1=(|\mathrm{b}+|\mathrm{c})/\sqrt{3}`$.

The information encoded in the degenerate total-spin singlet subspace of the 5-dot composite qubit is immune to collective decoherence, that is, decoherence affecting all spins equally bacon00a ; lidar00a ; zanardi97a ; kielpinski01a ; lidar98a ; lidar99a ; kempe01a ; lidar03a ; bacon01a . It is also immune to local decoherence affecting only a single dot. To see this, consider a magnetic field or an extra electron coupling only to dot 1 in Fig. (3). The singlet bond connecting to spin 1 will be mixed with a triplet bond. However, this occurs equally to all three eigenstates in Fig. (3), so the degeneracy between these states is not broken. More complicated mechanisms affecting multiple spins can cause decoherence, but these mechanisms must overcome the energy gap to the first excited state.

We now demonstrate the physically intuitive gate operations on the 5-dot qubit that allow universal quantum computation. Notice that $`|0=|\mathrm{a}`$ in Fig. (3) is odd under an exchange of sites 1 and 2, denoted by $`12`$, and this state is also odd under $`34`$. The other ground state $`|1=(|\mathrm{b}+|\mathrm{c})/\sqrt{2}`$ is even under both operations.

Increasing the tunneling between the middle dot and dots 1 and 2, denoted by $`H_{12}`$ in Fig. (4), respects the $`12`$ and $`34`$ symmetries and does not mix the ground states, but $`H_{12}`$ does break the degeneracy of the ground state. Thus it acts in the pseudospin space of $`|0`$ and $`|1`$ as a magnetic field in the $`\widehat{z}`$ direction:

$$H_{12}\left(\begin{array}{cc}\hfill 1& \hfill 0\\ \hfill 0& \hfill 1\end{array}\right).$$
(2)
The tunnelings from the middle dot to dots 3 and 4 could have been increased to implement the same gate, so effectively $`H_{34}=H_{12}`$. Adiabatic variation of the tunneling rates is required to avoid mixing with excited states. Adiabaticity is also required in the conventional single-quantum-dot qubit implementation to avoid mixing with states containing dots occupied by two electrons loss98a ; hu00a ; schliemann01a .

To perform arbitrary $`SU`$(2) rotations of the single composite qubit, we need to be able to perform rotations about two directions in pseudospin space. Therefore a gate in addition to $`H_{12}`$ is required. Varying three tunnelings in the 5-dot composite qubit can produce a rotation about the $`\widehat{x}`$ axis in pseudospin space, but a simpler gate can be formed by increasing the tunneling between the middle dot and dots 1 and 4, denoted by $`H_{14}`$ in Fig. (4). This operation breaks the $`12`$ and $`34`$ symmetries, and can be shown to be

$$H_{14}\left(\begin{array}{cc}\hfill 1& \hfill \sqrt{3}\\ \hfill \sqrt{3}& \hfill 1\end{array}\right),$$
(3)
which represents a rotation at an angle of 120 degrees from the $`\widehat{z}`$ axis divincenzo00a ; bacon00a . Again, increasing the tunnelings to dots 2 and 3 would implement the same gate, so $`H_{23}=H_{14}`$. With $`H_{12}`$ and $`H_{14}`$, any $`SU`$(2) rotation can be performed on the composite qubit. The one-qubit operations are similar to operations described for the 4-spin DFS, but in that case the interaction takes place directly between the spins and not through an auxiliary fifth dot bacon00a ; lidar00a ; kempe01a .

To form a two-qubit gate, two tunnelings must be turned on between adjacent qubits—A single tunneling interaction performs no operation due to the immunity of the composite qubit to local decoherence. An example of a two-composite-qubit gate is shown in Fig. (5) in which tunneling between pairs of outer dots on adjacent qubits has been turned on. This operation preserves the symmetries $`12`$ and $`78`$. Thus its action in the basis of $`\{|00,|01,|10,|11\}`$ has the general form

$$H_{2\mathrm{q}\mathrm{u}\mathrm{b}\mathrm{i}\mathrm{t}}=\left(\begin{array}{cccc}A& 0& 0& 0\\ 0& B& 0& 0\\ 0& 0& B& 0\\ 0& 0& 0& C\end{array}\right)$$
(4)
which has been verified by exact diagonalization of the 10-dot 8-electron Hubbard model for the two-dot system. During both the single- and two-composite qubit gate operations, the system stays in the total singlet subspace and remains immune to collective decoherence bacon00a .

Combining $`H_{2\mathrm{q}\mathrm{u}\mathrm{b}\mathrm{i}\mathrm{t}}`$ with single qubit rotations on the individual dots allows the controlled-phase gate $`\overline{𝐂}_P`$ to be implemented with a single pulse in which six tunneling rates are varied:

$`\overline{𝐂}_P`$ $`=`$ $`\mathrm{exp}\left({\displaystyle \frac{i}{\mathrm{}}}{\displaystyle \left(H_{12}(t)+H_{2\mathrm{q}\mathrm{u}\mathrm{b}\mathrm{i}\mathrm{t}}(t)+H_{78}(t)\right)}\right)\mathrm{d}t`$ (9)
$`=`$ $`\left(\begin{array}{cccc}\hfill 1& \hfill 0& \hfill 0& \hfill 0\\ \hfill 0& \hfill 1& \hfill 0& \hfill 0\\ \hfill 0& \hfill 0& \hfill 1& \hfill 0\\ \hfill 0& \hfill 0& \hfill 0& \hfill 1\end{array}\right)`$
where $`H_{12}`$, $`H_{2\mathrm{q}\mathrm{u}\mathrm{b}\mathrm{i}\mathrm{t}}`$, and $`H_{78}`$ all commute nielsen00 ; bacon00a ; kempe01a .

Finally, it is interesting to note that the 5-dot configuration is actually more stable than a 4-dot setup to variations in the hopping parameters. Varying a single tunneling rate in Fig. (1) does not break the degeneracy of the ground state. Such a change modifies the effective interactions of a single outer dot with each of the other outer dots, and simply shifts the ground-state energy preserving the degeneracy. In contrast, varying one of the six tunneling rates in the 4-dot setup splits the ground states.

In summary, a five-dot composite qubit design was presented that operates in a decoherence-free subspace. Universal quantum computation is easily implemented by varying tunneling rates in a simple, physically intuitive manner—Generation of local magnetic fields is not required to perform the gate operations. Each qubit is encoded in the degenerate singlet ground-state of four (or six) electrons in a system of five quantum dots arranged in a two-dimensional pattern. This supercoherent subspace is immune to both collective and local decoherence, and resists other forms of decoherence, which must raise the energy.

We thank J. Levy and D. A. Lidar for stimulating discussions. Support from DARPA QuIST (MIPR 02 N699-00) and DOD HPCMO CHSSI is gratefully acknowledged.


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# Searches for Giant Pulses from Extragalactic Pulsars

## 1 Introduction

While pulsar flux densities are typically quoted as averaged quantities, individual pulses in fact follow a distribution of pulse intensities, with some pulses having intensities of more than 10 times the mean Hesse & Wielebinski (1974). Many pulsars show approximately normal distributions of pulse intensities about a mean, while some show bimodal distributions, with a finite probability of zero power (e.g. Lyne & Graham-Smith 1998). Other pulsars show asymmetric distributions, with a long tail towards high values of pulse intensity. The Crab pulsar (B0531+21) is an extreme example of this case, with a ‘giant’ pulse more than 10 times the mean intensity occurring once every 1000 pulses Hankins & Rickett (1975); Lundgren et al. (1995). Such pulses have also been detected from the the millisecond pulsars B1821$``$24 and B1937+21 Cognard et al. (1996); Romani & Johnston (2001) and, very recently, from the young pulsar B0540$``$69 Johnston & Romani (2003). We explore how this giant-pulse phenomenon can be exploited to detect pulsars that may not be detectable through standard periodicity searches. While the main motivation for such a search is the detection of distant, Crab-like pulsars in other galaxies, searches for isolated, dispersed pulses may also be more sensitive than periodicity searches to pulsars seen through the Galactic scattering disk, pulsars with very fast spin periods and pulsars in short binary orbits. There is also the possibility of detecting other classes of radio bursting objects, as discussed in Cordes & McLaughlin (2003) (hereafter Paper I).

In Paper I, we discussed issues related to the detection of fast radio transients from astrophysical sources. We described search algorithms and methodology and in particular discussed the impact of interstellar scintillation and scattering on such searches. In this paper, we apply the methodology of Paper I to searches for giant pulses from extragalactic pulsars. We describe our searches for single radio pulses from M33, PSR B0540$``$69 in the Large Magellanic Cloud, and several other galaxies. While no giant pulses have been conclusively detected in these searches, we hope that they can serve as blueprints for future, more sensitive searches for radio transients. Although giant pulses from B0540$``$69 have recently been detected by Johnston & Romani (2003; hereafter JR03), we present the results of our earlier null search here and discuss the implications of our search for the giant-pulse properties of B0540$``$69.

The outline of this paper is as follows. In §2, we describe the giant-pulse phenomenon seen in the Crab pulsar and a few others. In §3, we explore the capabilities of single-pulse searches for detecting distant pulsars and compare the sensitivities of single-pulse and standard periodicity searches. In §4, we present results for several targets, including the nearby spiral galaxy M33, B0540$``$69 and a few other galaxies. Conclusions and a look to the future are offered in §5.

## 2 The Giant-Pulse Phenomenon

In one hour of observation, the largest measured peak pulse flux of the Crab is roughly $``$ 105 Jy at 430 MHz for a duration of roughly 100 $`\mu `$s Hankins & Rickett (1975), corresponding to an implied brightness temperature of 1031 K. Recently, pulses with flux $``$ $`10^3`$ Jy at 5 GHz for a duration of only 2 ns have been detected from the Crab Hankins et al. (2003). These ‘nano-giant’ pulses imply brightness temperatures of 1038 K, by far the most luminous emission from any astronomical object. For many years, this phenomenon was thought to be uniquely characteristic of the Crab. However, giant pulses have since been detected from the Crab-like pulsar B0540$``$69 and the millisecond pulsars PSRs B1937+21 and B1821$``$24. For B0540$``$69, the largest measured peak pulse flux in one hour is approximately 4 Jy Johnston & Romani (2003). From both millisecond pulsars, the largest measured peak pulse flux in one hour is $``$ 103 Jy at 430 MHz Cognard et al. (1996); Romani & Johnston (2001).

As shown in Figure 2, the giant pulses detected from the Crab and PSRs B0540$``$69, B1937+21 and B1821$``$24 represent the most luminous pulsed emission detected from any pulsar. While PSRs B1937+21 and B1821$``$24 are ‘recycled’ millisecond pulsars with very different ages, spin periods and surface magnetic field strengths than the Crab and PSR B0540$``$69, all four pulsars have similarly high values of magnetic field at the light cylinder $`B_{lc}`$ ($`B_{lc}10^{8.46}P^{\frac{5}{2}}\dot{P}^{\frac{1}{2}}`$ G, where $`P`$ is pulsar period is seconds and $`\dot{P}`$ is period derivative). This suggests that giant-pulse physics may depend on conditions there, rather than at the stellar surface. All four pulsars also show high-energy emission at the same phase as their giant pulses, suggesting a relationship between the two phenomena and that the giant-pulse emission process occurs high in the magnetosphere. In Table 1 we list the radio pulsars with the highest values of the magnetic field at the light cylinder.

Lundgren et al. (1995) found that the distribution of Crab pulse fluxes is bimodal, with separate components of the probability distribution function (PDF) describing the normal and giant pulses. As shown in Figure 2, the flux distribution of giant pulses, defined to be those with fluxes exceeding the detection threshold determined by the Crab nebula, can be roughly described by a power law for flux densities above the turnover at $``$ 200 Jy. The differential distribution $`dN/dSS^\alpha `$ with index $`\alpha `$ 3.5. Similarly, the giant-pulse intensity distribution for PSR B1937+21 can be described by a power law of index 2.8 Cognard et al. (1996). Unlike the Crab’s giant pulses, however, the giant pulses of PSR B1937+21 appear to be the extreme of a continuous distribution of pulse intensities. The giant pulses of PSR B1821$``$24 are less well-studied but seem to be adequately described by a power law of index 3 $``$ 5 Romani & Johnston (2001). Too few pulses have been detected from PSR B0540$``$69 to constrain their flux density distribution Johnston & Romani (2003).

## 3 Detectability of Giant Pulses

The vast majority of the over 1500 radio pulsars known were discovered through searches for periodic signals using Fourier methods. Because these searches incorporate many pulses from a single source, they are generally more sensitive than single-pulse searches. However, there are some conditions under which a single-pulse search may be more sensitive than a search for periodicity. In this section, we describe how searches for single pulses may be more effective than periodicity searches at detecting distant, giant-pulse emitting pulsars.

Finding distant pulsars in other galaxies is important as, of the roughly 1500 radio pulsars known, only $``$ 25 are extragalactic, all located in the Magellanic Clouds (A. G. Lyne, personal communication). Detection of extragalactic pulsars would allow us to study pulsar populations in other galaxies and to probe the interstellar medium in those galaxies as well as the intervening intergalactic medium. Finding more young pulsars like the Crab is crucial for understanding neutron star formation, supernovae and the early stages of pulsar evolution. However, Crab-like pulsars in our Galaxy are difficult to detect due to propagation processes, particularly scattering, through the Galactic plane. Searching for extragalactic pulsars is attractive because such searches may not suffer as greatly from such effects. We show how giant-pulse searches may be the most effective way of detecting these distant pulsars and use the properties of the Crab pulsar to infer to what distances we would be able to detect similar pulsars in other galaxies. We also compare the efficacy of searches for single pulses with that of traditional periodicity searches.

From the radiometer equation, we calculate the maximum distance to which a giant pulse like those observed from the Crab pulsar could be detected. Following the notation of §3.4 of Paper I and assuming matched filtering to a pulse that is temporally resolved, the maximum detectable distance scales with the Crab Nebula’s distance $`D_C=2`$ kpc as

$`D_{\mathrm{max}}`$ $`=`$ $`S/N_{\mathrm{min}}^{1/2}D_C\left({\displaystyle \frac{S_{\mathrm{GP}}}{S_{\mathrm{sys}}}}\right)^{1/2}\left(N_{\mathrm{pol}}\mathrm{\Delta }\nu W\right)^{1/4}`$ (1)
$``$ $`0.85\mathrm{Mpc}\left({\displaystyle \frac{S/N_{\mathrm{min}}}{5}}\right)^{\frac{1}{2}}\left({\displaystyle \frac{S_{\mathrm{sys}}}{5\mathrm{Jy}^1}}\right)^{\frac{1}{2}}\left({\displaystyle \frac{S_{\mathrm{GP}}}{10^5\mathrm{Jy}}}\right)^{\frac{1}{2}}`$
$`\times \left[\left({\displaystyle \frac{\mathrm{\Delta }\nu }{10\mathrm{MHz}}}\right)\left({\displaystyle \frac{W}{0.1\mathrm{ms}}}\right)\left({\displaystyle \frac{N_{\mathrm{pol}}}{2}}\right)\right]^{\frac{1}{4}}`$
where $`S/N_{\mathrm{min}}`$ is the S/N threshold, $`S_{\mathrm{sys}}=T_{\mathrm{sys}}/G`$ is the system noise in Jansky units (system temperature divided by the telescope gain), $`\mathrm{\Delta }\nu `$ is the receiver bandwidth, $`W`$ is the pulse width, assumed larger than the post-detection time constant, or sampling interval, $`\tau `$, $`N_{\mathrm{pol}}`$ is the number of independent polarization channels summed and $`S_{\mathrm{max}}`$ is the peak flux density of the giant pulse in the time of observation. We have assumed in deriving Eq. 1 that pulses are dedispersed and that any residual pulse smearing (e.g. from scattering) is less than $`W`$. Using fiducial values for an Arecibo 430-MHz search ($`\mathrm{\Delta }\nu =10`$ MHz, $`N_{\mathrm{pol}}=2`$, $`W0.1`$ ms, $`S_{\mathrm{sys}}=5`$ Jy), and a threshold $`S/N_{\mathrm{min}}`$ = 5, we calculate $`D_{\mathrm{max}}`$ 0.85 Mpc for Crab-like pulsars in a one-hour observation (i.e. $`S_{\mathrm{max}}10^5`$ Jy). For millisecond pulsars like PSR B1937+21 ($`D=3.6`$ kpc) and PSR B1821$``$24 ($`D5.5`$ kpc) for which $`S_{\mathrm{max}}10^3`$ Jy in one hour, $`D_{\mathrm{max}}0.15`$ to 0.23 Mpc.

Given the distribution of giant-pulse intensities measured by Lundgren et al. (1995), we calculate the number of Crab-like giant pulses detectable out to a distance $`D_{\mathrm{max}}`$ in such a search. As shown in Figure 3, Crab-like pulsars within several irregular and spiral galaxies in the Local Group, at distances less than 1 Mpc, would be detectable at rates greater than one pulse per hour. These include the LMC, SMC, M31, M33, NGC6822 and IC1613. If giant pulses an order of magnitude greater than the Crab’s are emitted, then another 7 galaxies in the 2 to 4.3 Mpc range, including M81, M82, M83, M94, M63, M51 and M101, might be accessible. Making the naive assumption that all pulsars of the Crab’s age ($``$ 1000 yr) or less will emit giant pulses, and assuming a pulsar birthrate of 1 per 100 years, we estimate that at least 10 giant-pulse emitting pulsars should be within each spiral galaxy similar to our own. Searching for these young pulsars is attractive as such searches may not be as impeded by dispersion and scattering as are searches for pulsars within our own galaxy.

It is useful to compare single-pulse and periodicity searches and the resultant maximum distances to which an isolated pulsar would be detectable through the two methods. Letting Dmax,SP and Dmax,FFT be the maximum distances to which we could detect a pulsar through a search for single pulses and through a FFT-based standard periodicity search, their ratio,

$$\frac{\mathrm{D}_{\mathrm{max},\mathrm{SP}}}{\mathrm{D}_{\mathrm{max},\mathrm{FFT}}}=\left(\frac{S/N_{\mathrm{min}}(\mathrm{FFT})}{S/N_{\mathrm{min}}(\mathrm{SP})}\right)^{\frac{1}{2}}\left(\frac{S_{\mathrm{max}}}{S_{\mathrm{avg}}}\right)^{\frac{1}{2}}\left(\frac{\tau }{T}\right)^{\frac{1}{4}}\left(\frac{W}{P}\right)^{\frac{1}{4}},$$
(2)
depends on the thresholds for the periodicity and single-pulse searches $`S/N_{\mathrm{min}}(\mathrm{FFT})`$ and $`S/N_{\mathrm{min}}(\mathrm{SP})`$, the post-detection time constant $`\tau `$ (optimally equal to the pulse width $`W`$), the total time integrated $`T`$, the maximum pulse giant pulse flux density, $`S_{\mathrm{max}}`$, seen in that time, the average flux $`S_{\mathrm{avg}}`$, and the period of the pulsar $`P`$. For typical parameters ($`S/N_{\mathrm{min}}(\mathrm{SP})`$ = 5, $`S/N_{\mathrm{min}}(\mathrm{FFT})`$ = 8, $`T`$ = 3600 s, $`\tau `$ = 0.1 ms and $`W/P`$ = 0.05), we find that a search for single pulses can detect pulsars to greater distances than the periodicity search when $`S_{\mathrm{max}}/S_{\mathrm{avg}}>1.7\times 10^4`$. The Crab pulsar, with $`S_{\mathrm{max}}/S_{\mathrm{avg}}=1.5\times 10^5`$ satisfies this criterion while PSR B1937+21, with $`S_{\mathrm{max}}/S_{\mathrm{avg}}=4.2\times 10^3`$, does not.

A more detailed analysis in the Appendix compares the two methods for different pulse-amplitude distributions. For distributions that are strictly power-law in form and with a large range of pulse amplitudes, single pulse searches are superior to periodicity searches for power-law indices $`\alpha `$ in the range of $`1\alpha 3`$ when the number of pulse periods investigated ranges from $`10`$ to $`10^5`$. For the Crab pulsar, $`\alpha 3.5`$, but single-pulse detection is superior to a periodicity search because pulses comprise both a power-law distribution and a component of much weaker but more frequent pulses, We find that in some circumstances, single-pulse searches are more effective than searches for periodicity, even in the absence of giant pulses. These regimes are further outlined in the Appendix and show that pulsar searches should always incorporate single-pulse searches in addition to standard periodicity searches. The computational time needed for the single-pulse search is typically a small fraction ($`<10\%`$) of the total search time. We note that the relative sensitivites of single-pulse and periodicity searches will depend on the extent and nature of radio frequency interference (RFI), with single-pulse searches being more affected by bursty, aperiodic RFI.

## 4 Searches for Extragalactic Pulsars

We now describe the results of searches for giant pulses from the nearby spiral galaxy M33, PSR B0540$``$69 in the LMC and from several other galaxies. While these searches were designed to detect giant pulses from pulsars, they are sensitive to other transient radio sources and serve as practical examples of applying the methodology described in Paper I. They also illustrate the challenges of searches for fast radio transients in the presence of RFI.

### 4.1 M33

As shown in Figure 3, all of the galaxies in the Local Group are within the range of detection of Crab-like giant pulses. The spiral galaxy M33, at a distance of approximately 840 kpc Freedman et al. (1991, 2001), is an excellent candidate for giant-pulse detection because its light derives mainly from blue, supergiant stars (i.e. progenitors of neutron stars). It is also visible with Arecibo, currently the most sensitive instrument for single-pulse searches at $``$ meter wavelengths. Our Arecibo search used a radio frequency of 430 MHz, optimal because of the steep spectral indices of pulsars and the low dispersion and scattering expected towards M33. The entire galaxy was covered with $`16\times 9^{}`$-diameter beams, as shown in Figure 4.1. In Table 2 we list beam number, RA and DEC in J2000 coordinates, the number of pointings at each beam and the total observation time per beam. Each beam was observed five to ten times for 900 or 1800 seconds over MJDs from 51054 to 52406 (i.e. from 29 August 1998 to 12 May 2002). The total amount of time spent per beam over these dates ranged from 1.75 to 3.0 hours. Two off-source positions were also observed, to provide an independent test of the reality of any detected signals. Observations were done with the Arecibo Observatory Fourier Transform Machine (AOFTM, `http://www.naic.edu/~aoftm/`), which covers a 10-MHz bandwidth with 1024 frequency channels and uses a sampling time of 102.4 $`\mu `$s.

Due to the high latitude ($`|b|30^o`$) of M33, the predicted Galactic contribution to the dispersion measure (DM) along the line of sight is only $``$ 50 pc cm-3 Cordes & Lazio (2002). As the orientation of M33 is nearly face-on Garcia-Gomez & Athanassoula (1991), we take Galactic and extragalactic DM contributions to be equal and estimate the maximum dispersion smearing expected across a 10-kHz frequency channel to be $``$ 0.1 ms. To allow for errors in the model and any regions of enhanced electron density along the line of sight, our searched DMs ranged from 0 pc cm-3 to 250 pc cm-3. Scaling from the Green Bank measurements of Lundgren et al. (1995), as in Figure 3, we estimate that more than one pulse per hour should be detectable from a Crab-like pulsar in M33 above a S/N threshold of 5, corresponding to a threshold of 0.5 Jy. Assuming a pulsar birthrate of 0.01 yr-1, we expect there to be roughly 10 pulsars of the Crab’s age or less in our Galaxy. Because the mass of M33 is roughly 10 times less than that of our Galaxy Méndez et al. (1999); Corbelli & Salucci (2000); Sakamoto et al. (2003), we might expect 10 times fewer young, Crab-like pulsars. However, evidence suggests that the supernova rate per unit mass is higher in M33 than in our Galaxy Berkhuijsen (1984); Gordon et al. (1998). Because these mass and supernova rate estimates are highly uncertain, it is difficult to predict how many Crab-like pulsars there might be in M33, but we expect it to be of order $``$ 10. Furthermore, since giant pulses are also emitted by millisecond pulsars like PSRs B1821$``$24 and B1937+21, the number of detectable pulsars may be larger.

Because RFI contaminated much of our data, our actual threshold was often significantly higher than that calculated from radiometer noise alone. In some cases, RFI was minor and did not greatly influence our sensitivity to pulses of astrophysical origin. In other cases, however, the RFI was quite strong and significant portions of the data had to be discarded from the analysis. This was done with interactive tools for displaying and selecting subsets of data in time and DM space.

For each beam, we applied the search algorithms described in Paper I to create diagnostic plots like those shown in Figures 4.1, 4.1 and 4.1 and inspected the results for evidence of high-DM pulses of an astrophysical origin. In Paper I similar plots for the giant-pulsing pulsars PSRs B0531+21 and B1937+21 are shown. For our M33 search, a signal-to-noise threshold of 4 was used and each time series was smoothed in seven stages (where adjacent samples were summed in each stage), corresponding to a maximum time resolution of $`2^7\times 102.4\mu s`$ 13 ms. If a pulse is detected in several of the smoothed time series, only the highest S/N pulse is recorded. Most beams, like that shown in Figure 4.1, show an excess of pulses at low DM due to RFI but show no evidence for high DM pulses. For some beams, the most dramatic example of which is shown in Figure 4.1, we detect an excess number of pulses at a well-defined, non-zero DM. For other beams, as shown in Figure 4.1, we detect individual strong pulses at high DM. While these features are tantalizing and, in some cases, consistent with originating from a pulsar in M33, no features repeat on multiple pointings at the same position. However, this is not inconsistent with the predictions of Figure 3. For each beam, we summed all of the DM histograms (i.e. upper right panels of Figures 4.1, 4.1 and 4.1) to determine if low-level excesses of pulses at a specific DM were present. However, no features were apparent in these combined histograms.

It is unlikely that interstellar scintillation is responsible for features, such as those shown in Figures 4.1 and 4.1, appearing only sporadically. Assuming a Galactic scale height of 1 kpc for $`C_n^2`$ (the electron-density fluctuation spectral coefficient; see Paper I) and a source velocity of 200 km/s (e.g. Arzoumanian et al. 2002) and applying the results of the Appendix of Paper I, we find that a source in M33 should have a scintillation timescale of only $``$ 35 seconds and a scintillation bandwidth of only $``$ 20 kHz at 430 MHz, rendering ISS unimportant in modulating source intensities during or between our observations. At 1400 MHz, these timescales and bandwidths would be much larger (roughly 141 seconds and 3.6 MHz) and would be important to consider.

Unfortunately, for the time being, our search for giant pulses from M33 pulsars remains inconclusive. It could be that the Crab and PSR B0540$``$69 are unusual pulsars and that there are no similar, giant-pulse emitting pulsars in M33. It is also possible that we have detected giant pulses from M33 pulsars, but they are either too sporadic or too weak to be distinguished from the many pulses due to RFI. Sensitive, multiple-beam and/or multiple-site observations are necessary to conclusively assess the reality of the signals we have detected.

In addition to the single-pulse search, a periodicity search was performed on all of the M33 data, typically using 8-Mpoint FFTs (i.e. roughly 14 minutes of data at our 102.4 $`\mu `$s sampling rate). While the chances of detecting a pulsar in M33 through such a search are very small (the pulsar would have to have an average flux density of approximately 30 times that of the Crab’s), we were sensitive to pulsars within our own Galaxy along the line of sight to M33. No periodic sources were detected in this search down to a limiting sensitivity of 0.2 mJy (assuming a duty cycle of 0.05).

### 4.2 PSR B0540$``$69

With a period of 50.3 ms, a period derivative of $`4.8\times 10^{13}`$ s s-1, and hence a spin-down age of roughly 1660 years, pulsar B0540$``$69 has more similar spin-down parameters to the Crab pulsar than any other known pulsar. Furthermore, as shown in Table 1, the magnetic field at the light cylinder of this pulsar, the strength of which seems to be correlated with giant-pulse emission, is fifth among known radio pulsars. Although it is roughly 50 kpc away in the LMC, it is a strong X-ray and optical source. The DM of PSR B$`054069`$ measured by Manchester et al. (1993) is $`146\pm 4`$ pc cm-3. They measure a 640 MHz flux of 0.4 mJy, roughly the same flux that the Crab would have at the distance of the LMC. While its integrated radio emission is weak, we might expect PSR B0540$``$69 to emit giant pulses similar to those detected from the Crab. The detection of such pulses from PSR B0540$``$69 would allow us to compare the shapes and phases of giant pulses with those at high energies, determine the dispersion measure more accurately and perhaps measure polarization of strong giant pulses.

With this in mind, we obtained a total of 55 observations of PSR B0540$``$69 between September 7, 1994 and September 26, 1994 with the Parkes Radiotelescope in New South Wales, Australia. These include 15 observations at a center frequency of 660 MHz, with 256 0.125-MHz channels covering a 32-MHz bandpass, and 40 observations at a center frequency of 1520 MHz, with 64 5-MHz channels covering a 320-MHz bandpass. At both frequencies, a sampling time of 0.6 ms was used. Most of our pointings were one-hr long, bringing the total number of hours on source to 14.4 hours at 660 MHz and 38.1 hours at 1520 MHz. Our 5$`\sigma `$ single-pulse detection thresholds calculated from radiometer noise were 4 Jy and 0.5 Jy at 660 and 1520 MHz, respectively. Actual thresholds were significantly higher in some pointings due to RFI, but most RFI could be excised by discarding subsets of the data from the analysis.

Given the parameters above, we would expect to detect Crab-like giant pulses up to S/Ns of 9 and 17 at the lower and upper frequencies, respectively, in our total observation times at the two frequencies (assuming a spectral index of $`2`$). In Figures 4.2 and 4.2, we plot the signal-to-noises and DMs of all pulses detected above a 5$`\sigma `$ threshold at both frequencies. Our data at 660 MHz do not show any evidence for giant pulses at the DM of B0540$``$69. At 1520 MHz, the strongest non-zero DM pulse has a amplitude of 7$`\sigma `$ and a DM of 146 pc cm-3. While this is tantalizing, several pulsars nearly as strong are detected at other DMs, and we cannot claim detection of giant pulses with our data. Given the large scattering timescales measured by JR03, it is unlikely that scintillation played a role in modulating the fluxes of pulses during our observation.

While the 1384-MHz JR03 observations benefited from a new Parkes receiver with lower system temperature and a slightly lower observing frequency, the main difference between their observations and the observations reported here is the channel bandwidth. They used 0.5-MHz filters, implying smearing of only 230 $`\mu `$s for a DM of 146 pc cm-3. Our 5-MHz filters caused a DM smearing of 1.8 ms, much more than the scatter-broadened giant-pulse width of 0.4 ms measured by JR03. Given the peak giant-pulse fluxes and widths reported by JR03, we would expect to detect their strongest pulse at a signal-to-noise of $`8\sigma `$. Adding in the effects of a slightly higher observing frequency and increased system noise, the pulse signal-to-noise distribution in Figure 4.2 is consistent with their observations.

Our non-detection of giant pulses at 660 MHz is more difficult to understand. Given the 0.4-ms scatter-broadened width of the pulses detected by JR03, we expect 10-ms of scatter broadening at 660 MHz, much greater than the 0.5-ms expected DM smearing across one of our 0.125-MHz channels. If the spectral index of PSR B0540$``$69 is indeed as steep as $`4.4`$, as the observations by JR03 suggest, we would expect to detect pulses as strong as 20$`\sigma `$ in our data. A spectral index of $`3`$ or higher is required to explain our null results at 660 MHz.

### 4.3 Other Galaxies

During our search for giant pulses from PSR B0540$``$69, we observed several other galaxies. While it is unlikely that a pulsar could be detected in any of these galaxies, aside from the LMC, these searches are constraining for some of the other source populations discussed in Section 2 of Paper I. In Table 3, we list these targets, along with Right Ascension, Declination, Galactic longitude, Galactic latitude, estimated distance and the number of pointings $`N_p`$ at each object. Each pointing was 1800-seconds long and for most pointings we used a central frequency of 435 MHz, with 256 channels of width 0.125-MHz and a sampling time of 0.42 ms. Galaxies NGC253, NGC300, Fornax, NGC6300 and NGC7793 were all covered by a single Parkes beam, while 6 separate pointings were necessary to cover the 2 deg2 error box of the high-energy LMC source 3EG J0533$``$69 Hartman et al. (1999). We performed a search for single pulses on all of the pointings, but did not find any conclusive evidence for isolated dispersed pulses from any of these galaxies. In Figure 4.3, we present results for the LMC pointing with the 16-ms X-ray pulsar J0537$``$6910 in the beam. This pulsar is interesting as it has a $`B_{lc}`$ which is over twice that of the Crab or PSR B1937+21. We detect an excess of pulses at a DM of 113 pc cm-3, consistent with the DMs of pulsars already detected in the LMC Crawford et al. (2001). However, because of the presence of RFI which manifests itself as dispersed radio pulses at many DMs, it is impossible to assess the reality of this signature. More sensitive and/or multiple beam/multiple site observations are required.

## 5 Conclusions

We have described the capabilities of searches for extragalactic giant pulses and the results of several searches towards extragalactic targets. We find that giant pulses from Crab-like pulsars should be detectable from all galaxies in the Local Group. We explore different pulse-amplitude power distributions and intensity cutoffs and find that single-pulse searches are superior to periodicity searches in certain cases. We emphasize that this kind of search should be done along with standard periodicity searches for pulsars because of the small additional computational efforts and the possibly large gains. The example results from searches for giant pulses from extragalactic pulsars illustrate the methodology and challenges of any search for transient radio signals. We have detected several intriguing dispersed pulses of possibly astrophysical origin from the spiral galaxy M33 with a search using the Arecibo radiotelescope at 430 MHz. Assessment of the astrophysical nature of these pulses must wait for more sensitive multiple-beam and/or multiple-site observing systems. We have detected no convincing signatures of giant pulses from the young LMC pulsar B0540$``$69 or from several other galaxies in searches with the Parkes radio telescope.

While the results of the M33 search presented here are inconclusive, they illustrate both the capabilities and difficulties in single-pulse searches and serve as a pilot study for future searches. To increase the capabilities of single-pulse searches, systems with multiple beams or multiple antennas are necessary in order to perform coincidence tests which will discriminate between pulses of astrophysical and terrestrial origins. Larger collecting areas are needed to increase our sensitivity to pulses from pulsars and other transient sources in other galaxies. Multi-beam systems for the Arecibo and Green Bank telescopes will likely be built within the next few years. Observing with multiple beams will allow us to distinguish RFI from real signals and would remove much of the ambiguity in interpreting the results of our M33 search. On a longer time scale, large radio arrays such as the Square Kilometer Array (SKA) will be developed. With a planned field of view over 100 times that of Arecibo and a sensitivity over 20 times that of Arecibo, the SKA will revolutionize single-pulse searches. While the SKA will not be operational for many years, single-pulse searches in the meantime, especially with multiple beams, are essential for optimizing routines for RFI excision and for processing large amounts of data.

We thank Simon Johnston and Froney Crawford for useful discussions. MAM is supported by an NSF Math and Physical Sciences Distinguished Research Fellowship. Arecibo Observatory is operated by the National Astronomy and Ionosphere Center, which is operated by Cornell University under cooperative agreement with the National Science Foundation (NSF). The Parkes Observatory is part of the Australia Telescope which is funded by the Commonwealth of Australia for operation as a National Facility managed by CSIRO.

## Appendix A Periodicity Searches vs. Single-Pulse Searches

This appendix considers the detectability of pulsars with respect to two broad search techniques: one that exploits the inherent periodicity and another that identifies individual, large-amplitude pulses. Burns & Clark (1969) made a brief comparison of these techniques but, for the most part, pulsar astronomers have relied on periodicity searches. Consider a time interval of length $`T`$ in which there are $`N_p`$ pulse periods. Pulse intensity maxima are described by a continuous probability density function (PDF) $`f_\mathrm{S}(S)`$ and its integral, the cumulative distribution function (CDF) $`F_\mathrm{S}(S)`$.

### A.1  Single-Pulse Search Detection

Given system noise $`S_{\mathrm{sys}}`$ expressed in Janskys, the signal-to-noise ratio (S/N) of the pulse peak $`S_{\mathrm{max}}`$ in the sum of $`N_{\mathrm{pol}}`$ polarization channels when the pulse is match filtered is

$`\left(S/N\right)_{\mathrm{SP}}=\eta (N_{\mathrm{pol}}\mathrm{\Delta }\nu W)^{1/2}S_{\mathrm{sys}}^1S_{\mathrm{max}},`$ (A1)
where $`\eta 1`$ is a pulse-shape-dependent factor, $`\mathrm{\Delta }\nu `$ is the total bandwidth and $`W`$ is the pulse width. For a Gaussian pulse shape, $`\eta =(\pi /8\mathrm{ln}2)^{1/4}0.868`$. Single pulse detection would entail specifying some threshold $`S/N`$ of at least 3 and probably much larger, depending on how many statistical trials were made in a survey.

For PDFs with long tails, one should take into account the fact that $`f_\mathrm{S}`$ is truncated at the maximum likely intensity in the interval. Assuming that all pulses have the same width $`W`$, we define the maximum pulse intensity likely to occur in the interval from the constraint $`[1F_\mathrm{S}(S_{\mathrm{max}})]N_p=1`$, implying

$`F_\mathrm{S}(S_{\mathrm{max}})=1N_p^1.`$ (A2)
### A.2 Periodicity Search Detection

In a search for a periodic signal in the time series, the Fourier analysis effectively measures the period-averaged mean intensity for the time interval. The period-averaged intensity is defined to be $`S_\varphi =\zeta (W/P)S_{\mathrm{avg}}`$, where $`S_{\mathrm{avg}}`$ is the mean peak intensity, $`\zeta `$ is a shape-dependent constant $`1`$ and $`P`$ is the pulse period. For a Gaussian pulse with FWHM $`W`$, $`\zeta =\sqrt{\pi /\mathrm{ln}2}/21.06`$. In terms of the pulse-peak PDF, the ensemble mean of the peak intensity is

$`S_{\mathrm{avg}}{\displaystyle 𝑑SSf_\mathrm{S}(S)}.`$ (A3)
However, recognizing that PDFs with long tails yield a maximum intensity in a finite number of pulse periods, we define a modified mean intensity,

$`S_{\mathrm{avg}}^{}={\displaystyle \frac{_0^{S_{\mathrm{max}}}𝑑SSf_\mathrm{S}(S)}{_0^{S_{\mathrm{max}}}𝑑Sf_\mathrm{S}(S)}}=\left(1N_p^1\right)^1{\displaystyle _0^{S_{\mathrm{max}}}}𝑑SSf_\mathrm{S}(S).`$ (A4)
The S/N for a periodicity search over an interval $`TN_pP`$ is

$`\left(S/N\right)_{\mathrm{FFT}}=(N_{\mathrm{pol}}\mathrm{\Delta }\nu T)^{1/2}S_{\mathrm{sys}}^1S_\varphi h__\mathrm{\Sigma },`$ (A5)
where the harmonic sum is

$`h__\mathrm{\Sigma }=N_h^{1/2}{\displaystyle \underset{\mathrm{}=1}{\overset{N_h}{}}}R_{\mathrm{}},`$ (A6)
with $`R_{\mathrm{}}`$ equal to the ratio of the $`\mathrm{}`$-th harmonic’s Fourier amplitude to that of the DC value. The leading factor $`N_h^{1/2}`$ takes into account that the threshold increases as the number of harmonics summed increases. For a Gaussian pulse shape,

$`R_{\mathrm{}}=\mathrm{exp}\left[\left({\displaystyle \frac{\pi W\mathrm{}}{2P\sqrt{\mathrm{ln}2}}}\right)^2\right],`$ (A7)
and the number of harmonics maximizing $`h__\mathrm{\Sigma }`$ is $`N_{h}^{}{}_{\mathrm{max}}{}^{}P/2W`$. The value of the harmonic sum at the maximum is well approximated by $`h_{_\mathrm{\Sigma }}^{}{}_{\mathrm{max}}{}^{}1/2\left(P/W\right)^{1/2}`$. The $`S/N`$ of the periodicity search using the harmonic sum is then

$`\left(S/N\right)_{\mathrm{FFT}}`$ $`=`$ $`(\zeta /2)(N_{\mathrm{pol}}\mathrm{\Delta }\nu W)^{1/2}S_{\mathrm{sys}}^1N_P^{1/2}S_{\mathrm{avg}}^{}.`$ (A8)
### A.3 Comparing Single-Pulse and Periodicity Detection

A comparison of the two techniques is best done by considering the ratio of the two signal-to-noise ratios:

$`r`$ $``$ $`{\displaystyle \frac{\left(S/N\right)_{\mathrm{SP}}}{\left(S/N\right)_{\mathrm{FFT}}}}`$ (A9)
$`=`$ $`\left({\displaystyle \frac{2\eta }{\zeta N_p^{1/2}}}\right){\displaystyle \frac{S_{\mathrm{max}}}{S_{\mathrm{avg}}^{}}}`$
$`=`$ $`\left({\displaystyle \frac{1}{N_p}}\right)^{1/2}{\displaystyle \frac{2\eta S_{\mathrm{max}}}{\zeta \left(1N_p^1\right)^1_0^{S_{\mathrm{max}}}𝑑SSf_\mathrm{S}(S)}}.`$
### A.4 Unimodal Distributions

Inspection of Eq. A9 indicates that in order for $`r>1`$, $`S_{\mathrm{max}}/S_{\mathrm{avg}}^{}>\zeta N_p^{1/2}/2\eta `$, which is a large number for typical observation times $`T`$ and pulse periods $`P`$. Some unimodal PDFs satisfy this criterion for large $`N_p`$ while many do not.

We first consider an exponential PDF,

$`f_\mathrm{S}(S)=S_{\mathrm{avg}}^1e^{S/S_{\mathrm{avg}}}U(S),`$ (A10)
where $`U`$ is the unit step function. For this case the maximum pulse intensity encountered in $`N_p`$ trials is

$`S_{\mathrm{max}}=S_{\mathrm{avg}}\mathrm{ln}N_p,`$ (A11)
the renormalized average is

$`S_{\mathrm{avg}}^{}=S_{\mathrm{avg}}\left[1{\displaystyle \frac{\mathrm{ln}N_p}{N_p1}}\right]`$ (A12)
and ratio of $`S/N`$ for the two search methods becomes

$`r={\displaystyle \frac{2\eta \mathrm{ln}N_p}{\zeta N_p^{1/2}\left[1\mathrm{ln}N_P/(N_p1)\right]}}.`$ (A13)
For this case, $`r>1`$ only for $`N_p47`$.

We next consider a power law PDF. A truncated power law PDF can be written in the form

$`f_\mathrm{S}(S)`$ $`=`$ $`𝒩S^\alpha ,S_1SS_2`$ (A14)
$`𝒩`$ $`=`$ $`\{\begin{array}{cc}(\mathrm{ln}S_2/S_1)^1\hfill & \alpha =1\hfill \\ & \\ {\displaystyle \frac{(1\alpha )}{(S_2^{1\alpha }S_1^{1\alpha })}}\hfill & \alpha 1.\hfill \end{array}`$ (A18)
For a flat PDF ($`\alpha =0`$) all pulse intensities are equally probable, so we expect that as $`N_p`$ gets large, the maximum and minimum intensities will equal the cutoff values. Letting $`S_{\mathrm{max}}S_2`$, we find

$`r={\displaystyle \frac{4\eta }{\zeta N_p^{1/2}}}{\displaystyle \frac{1}{\left(1+S_1/S_2\right)}}.`$ (A19)
Asymptotically, the maximum $`r`$ results for $`S_2/S_11`$,

$`r_{\mathrm{max}}{\displaystyle \frac{4\eta }{\zeta N_p^{1/2}}},`$ (A20)
which yields $`r>1`$ only for $`N_p<11`$.

We will not consider power laws with $`\alpha <0`$. For $`\alpha >0`$, larger amplitudes are less probable, so we expect that the maximum encountered out of $`N_p`$ pulses generally will be less than $`S_2`$. We find that

$$S_{\mathrm{max}}=\{\begin{array}{cc}S_1\left(\frac{S_2}{S_1}\right)^{1N_p^1},\hfill & \alpha =1\hfill \\ & \\ \frac{S_2}{\left[\left({\displaystyle \frac{N_p1}{N_p}}\right)\left(1+\left({\displaystyle \frac{S_2}{S_1}}\right)^{\alpha 1}{\displaystyle \frac{1}{N_p1}}\right)\right]^{{\displaystyle \frac{1}{\alpha 1}}}}\hfill & \alpha 1\hfill \end{array}$$
(A21)
Using $`S_{\mathrm{max}}`$ we evaluate111Note that we evaluate $`S_{\mathrm{avg}}^{}`$ by integrating from the actual lower cutoff $`S_1`$ to the effective upper cutoff $`S_{\mathrm{max}}`$. This is valid only for monotonically decreasing PDFs, i.e. $`\alpha >0`$. For a flat PDF, moreover, we should let $`S_{\mathrm{max}}S_2`$. $`S_{\mathrm{avg}}^{}`$

$$S_{\mathrm{avg}}^{}=\{\begin{array}{cc}\frac{S_{\mathrm{max}}S_1}{\mathrm{ln}S_{\mathrm{max}}/S_1}\hfill & \alpha =1\hfill \\ & \\ \frac{S_1S_{\mathrm{max}}\mathrm{ln}S_{\mathrm{max}}/S_1}{S_{\mathrm{max}}S_1}\hfill & \alpha =2\hfill \\ & \\ S_{\mathrm{max}}\left(\frac{\alpha 1}{\alpha 2}\right)\left[\frac{\left({\displaystyle \frac{S_{\mathrm{max}}}{S_1}}\right)^{\alpha 2}1}{\left({\displaystyle \frac{S_{\mathrm{max}}}{S_1}}\right)^{\alpha 1}1}\right]\hfill & \alpha 1,2.\hfill \end{array}$$
(A22)
For steeper power laws with $`\alpha >0`$, the S/N ratio $`r>1`$ only for small $`N_p`$ for $`\alpha 1`$. For intermediate cases, $`1.5\alpha 2.5`$, $`r`$ has a maximum at $`N_p1`$. For steep power laws (e.g. $`\alpha 3`$) the ratio $`r>1`$ again only for small $`N_p`$ and decreases monotonically.

Figure A.4 shows $`r`$ for several power-law cases and for the exponential PDF and illustrates the statements made in the preceding paragraph. The values for $`r`$ are small for nearly flat PDFs because the pulses Fourier-analyzed in a long-train of pulses have amplitudes that do not deviate much from the peak pulse. For very steep power laws (e.g. $`\alpha 3`$), the probability of seeing a large pulse near the upper cutoff, $`S_2`$, is too small to outweigh the $`N_p^{1/2}`$ increase in S/N of the Fourier method, even for very large $`N_p`$. For intermediate cases, where $`r`$ has a distinct maximum, the likelihood of seeing a large pulse outweighs the $`N_p^{1/2}`$ increase in S/N of the Fourier method.

For $`\alpha >1`$ and $`\alpha 2`$ we can express $`r`$ in the limit where $`S_2/S_11`$ using Eq. A21-A22:

$`r\left({\displaystyle \frac{2\eta }{\zeta }}\right)\left({\displaystyle \frac{\alpha 2}{\alpha 1}}\right)\times \{\begin{array}{cc}N_p^{{\displaystyle \frac{3\alpha }{2(\alpha 1)}}},\hfill & N_p(S_2/S_1)^{\alpha 1}\hfill \\ & \\ \left({\displaystyle \frac{S_2}{S_1}}\right)N_p^{1/2},\hfill & N_p(S_2/S_1)^{\alpha 1}.\hfill \end{array}`$ (A26)
For small $`N_p`$, $`r`$ scales as $`rN_p^{(3\alpha )/2(\alpha 1)}`$ until $`S_{\mathrm{max}}S_2`$ and then $`r`$ decreases as $`N_p^{1/2}`$. Note that $`r`$ has an increasing branch only if $`1<\alpha <3`$, consistent with Figure A.4. If there is an increasing branch, then we expect a maximum approximately where the two scaling laws in Eq. A26 are equal:

$`N_{p}^{}{}_{\mathrm{max}}{}^{}\left({\displaystyle \frac{S_2}{S_1}}\right)^{\alpha 1}.`$ (A27)
For $`S_2/S_1=10^5`$, we expect the maximum for $`\alpha =3/2`$ to be at $`N_p10^{5/2}`$, consistent with the exact expressions evaluated in the Figure. The maxima for $`\alpha =2`$ and $`\alpha =5/2`$ are then expected at $`N_{p}^{}{}_{\mathrm{max}}{}^{}10^5`$ and $`10^{15/2}`$ and are thus off the scale of Figure A.4.

We conclude that for certain power laws, intensity cutoffs and numbers of pulses, single-pulse searches can be superior to periodicity searches.

For the Crab pulsar at 146 MHz, Argyle & Gower (1972) find $`\alpha 2.5`$ over at least two orders of magnitude of flux density (c.f. Figure 4-9 of Manchester & Taylor 1977). This slope is consistent with the fact that the Crab pulsar is more easily detected (and was discovered through) using its giant pulses. At 812 MHz Lundgren et al. (1995) find $`\alpha 3.5`$ over 1.2 orders of magnitude. They also infer that the PDF for all pulses (giant and normal) is bimodal. Therefore, even though the slope found by Lundgren et al. would suggest that single-pulse detection would be inferior to a periodicity search, the apparent bimodality appears to change this conclusion, as we show below.

### A.5 Bimodal Distribution

A bimodal distribution provides a finite phase space for $`r>1`$, even for large pulse numbers $`N_p1`$. Consider the bimodal distribution

$`f_\mathrm{S}(S)=(1g)\delta (SS_1)+g\delta (SS_2).`$ (A28)
The only interesting case is when the interval contains at least one pulse with intensity $`S_2`$, requiring $`gN_p1`$ or $`g>g_{\mathrm{min}}`$ where $`g_{\mathrm{min}}=N_p^1`$. In this case we have

$`r={\displaystyle \frac{2\eta S_2}{\zeta N_p^{1/2}\left[(1g)S_1+gS_2\right]}}.`$ (A29)
To have $`r>1`$ requires $`g_{\mathrm{min}}<g<g_{\mathrm{max}}`$ where

$`g_{\mathrm{max}}={\displaystyle \frac{(2\eta /\zeta )N_p^{1/2}S_1/S_2}{1S_1/S_2}}.`$ (A30)
Figure A.5 shows regions in the two dimensional space of $`g`$ and $`S_1/S_2`$ for which $`r>1`$. The regions are a function of $`N_p`$.

A special case of interest for the bimodal PDF is where the lowest intensity pulses are null pulses (i.e. $`S_1=0`$). Then

$`r={\displaystyle \frac{2\eta }{g\zeta N_p^{1/2}}}.`$ (A31)
Single pulse detection is superior to a periodicity search when

$`N_p^1<g<(2\eta /\zeta )N_p^{1/2}.`$ (A32)
This regime corresponds to values of $`g`$ between the solid and dashed lines in Figure A.5 for small values of $`S_1/S_2`$.

Under some other special circumstances, searches for single pulses are more effective than periodicity searches. For large duty cycles, the single-pulse detection scheme becomes exponentially better once the pulse width exceeds the pulse period. Using the general expressions in Eq. A5 through Eq. A7 when calculating $`r`$ as a function of duty cycle, $`W/P`$, we find as a typical trend that the periodicity search is superior for $`W/P1`$ and if the single-pulse amplitude PDF does not have a large dynamic range in amplitudes, as described in the previous subsection. However, for $`W/P1`$, the single-pulse search is generally superior, no matter the form for the amplitude PDF.

These results imply that sources with small spin and small orbital periods may be detected in single-pulse searches when they would be missed completely in periodicity searches. Similarly, distant pulsars viewed through deep scattering volumes and thus having large scattering measures are likely to be missed in periodicity searches. In this case, the scattering time is a strong function of frequency, and so too will be the relative sensitivities of single-pulse and periodicity searches.


text:
# Oxygen-stripes in La0.5Ca0.5MnO3 from ab initio calculations

\[

## Abstract

We investigate the electronic, magnetic and orbital properties of La0.5Ca0.5MnO3 perovskite by means of an ab initio electronic structure calculation within the Hartree-Fock approximation. Using the experimental crystal structure reported by Radaelli et al. \[Phys. Rev B 55, 3015 (1997)\], we find a charge-ordering stripe-like ground state. The periodicity of the stripes, and the insulating CE-type magnetic structure are in agreement with neutron x-ray and electron diffraction experiments. However, the detailed structure is more complex than that envisaged by simple models of charge and orbital order on Mn d-levels alone, and is better described as a charge-density wave of oxygen holes, coupled to the Mn spin/orbital order.

\]

Understanding the physics displayed by manganite oxide compounds R1-xDxMnO3 (R=rare-earth atom, D=divalent substituent) has stimulated much experimental and theoretical work . Changing the composition $`x`$, they show a variety of phenomena, such as ferromagnetic (FM), anti-ferromagnetic (AF), charge and orbital ordering (CO and OO) revealing that charge, spin and and lattice degrees of freedom are closely interrelated.

In the present work, we concentrate on the half-doped case of La1-xCaxMnO3 that has been extensively studied . For $`x=0`$, LaMnO3, there is a collective Jahn Teller (JT) distortion of the structure that gives rise to a splitting of the $`e_g`$ levels. As a consequence of that, the structure is orthorhombic, the Mn $`e_g`$-levels are singly occupied and all Mn ions are Mn3+. For the other extreme doping ($`x=1`$), CaMnO3 is pseudo-cubic as the $`e_g`$-levels are empty and Mn4+ does not couple to the lattice distortion. In LaMnO3, the splitting of the $`e_g`$ orbitals favors the cooperative JT distortions and the appearance of OO. This fact allowed Goodenough  and Kugel and Khomskii  to explain the magnetic structure of this compound. Their explanation assumed unpolarized O2- ions and was based on the idea that magnetic ordering is dictated by the orientation of the orbitals involved.

The regime of intermediate doping is complex, magnetically and structurally, but even at the level of the local electronic structure there are several experiments that present contradictory results. Some of them claim a mixed valence picture of Mn3+ and Mn4+ while others found features that do not reconcile with this image. For example, by doing Oxygen K-edge electron-energy-loss spectra, it was concluded that carriers in La1-xSrxMnO3 (0$`x`$ 0.7) have a significant oxygen-$`p`$ hole character . Some x-ray absorption studies at the Mn K-edge in Ca-doped LaMnO3 revealed a picture that does not match with a mixture of Mn3+ and Mn4+ for intermediate dopings . On the contrary, Tyson *et al.*  performed a Mn $`K_\beta `$ x-ray emission experiment in the same compound and found that their data was compatible with a Mn3+/Mn4+ mixing for intermediate compositions. Similar contradictions have been found using neutron diffraction , photo-emission and x-ray spectroscopy techniques . These contradictory features motivate the need for a clarifying picture regarding the valence state of the Mn ions in manganite systems. One of the goals of the present work is to provide an ab initio quantum mechanical calculation to investigate the local electronic structure of the compound in order to establish the nature of the charge carriers.

In this letter we report the theoretical finding of oxygen-stripes in La0.5Ca0.5MnO3 by means of an ab initio spin-unrestricted Hartree-Fock (HF)  study . Our results were obtained by means of the code CRYSTAL98  that uses a few localized basis functions per atom to solve self-consistently the HF equations. In the present work, the basis set for the different atoms are those optimized for previous calculations  and the crystal structure is taken from the experimental work reported by Radaelli et al . So, the present study takes into account the actual JT distortions and the size of the atoms involved. It is expected that the periodic HF approximation will correctly describe the physics involved in this system as it has been successful in describing other magnetic insulators as well as strongly correlated materials .

The crystal structure for La0.5Ca0.5MnO3 can be indexed in space group $`P2_1/m`$  with 3 inequivalent Mn atoms per unit cell. Two Mn ions are associated with JT distorted MnO6 octahedra (that we will label as d1 and d2). Although in a similar environment of local O distortions, these two sites are not identical. The third Mn belongs to an almost undistorted octahedra. The cell of the crystal structure has one axis ($`b`$) longer than the other two ones ($`a,c`$). We will call basal planes the Mn-O planes perpendicular to the $`b`$ axis. The magnetic ordering for this compound was coined CE-type . It consists of FM zigzag chains that are coupled AFM (see Fig. 1)

As it was previously reported  for LaMnO3 and CaMnO3 within the HF approximation, Mulliken population analysis (MPA) gives charges for Mn and O ions that deviates substantially from the formal valence picture. In these works, MPA results for LaMnO3 give Mn+2.2 and O-1.7 to be compared with the formal values Mn+3 and O-2 whereas in CaMnO3, Mn+2.2 and O-1.3 should be contrasted with Mn+4 and O-2. However, the MPA for the spin values do not show such deviation. In LaMnO3, the Mn spin was 1.98  and in CaMnO3, $`\frac{3.2}{2}`$ ; that is, very close to the formal valence spin values of 2 and $`\frac{3}{2}`$, respectively. In both cases, the spin for the O atoms was also close to the formal picture being mainly spin unpolarized. The origin of the difference between charge and spin values is the strong hybridization between Mn and O bands with the subsequent screening of Mn charge by electrons in the surrounding O atoms. In the half doped case, we find that MPA also shows deviations from the formal valence picture with all Mn having about the same charge. For the oxygens, almost all of them have a formal charge close to O-1.6, but there are some holes leading to O-1.2, as we will detail further on.

Regarding the magnetic properties of this system, we found that the ground state is correctly predicted to have the CE-type ordering in agreement with neutron experiments . The FM state and the A-type AFM state both have energies that are above the CE-type state by at least 1.1 eV and 0.9 eV per unit cell, respectively . Presumably, the FM and A-type states have similar energies because the coupling between basal planes is weak.

We found that the ground state for the half doped case is almost doubly degenerate. One of the solutions is visualized in the spin-density map depicted in Fig. 1, that clearly shows that the Mn ions display OO. As an aid to understand the map, we draw in the same figure, a sketch of the corresponding orbital and crystal structure with shading showing the value of the spin polarization (S). Some oxygens have spin-polarized holes (see Table 1). For the solution shown, holes are located on O atoms forming the long bonds of one of the distorted octahedra d1. The other (nearly degenerate) solution has oxygen holes instead along the long bonds of octahedra d2, with the corner-Mn orbital always in the direction of the O-hole . So, within the HF approximation, not just the Mn ions but also the oxygens play an important role. Indeed, as seen in Table 1, charge modulation occurs principally on the oxygens rather than on Mn atoms.

The origin of the spin-polarized O-holes can be understood in terms of the OO. For the analysis, we will consider only the atoms within a zigzag chain because the oxygens between chains are unpolarized (which is consistent with the AFM coupling between adjacent Mn). As can be seen in Fig. 1, the OO around Mn(d2) resembles LaMnO3. Along the long bond of d2, we found no spin-polarized O-holes which is consistent with Goodenough’s ideas. However, around Mn(d1) the OO is different. In the long bond of d1, both Mn and O orbitals lie along the same line allowing for a transfer of charge from the O to the Mn, and rendering the O with a hole . Due to exchange, this O-hole has opposite spin to its two adjacent Mn ions.

As the spin-polarized oxygens are always AF aligned with the neighboring Mn spin, the Mn-O complex forms a state analogous to the Zhang-Rice singlet in the cuprates : the corner-Mn with the O-hole forms a low spin-state that gives a total S $``$ $`\frac{3}{2}`$ (see Fig. 2). This connects to the usual models of d-orbital occupancy alone, where a hybrid Mn-O state stands in place of a Mn4+ ion. Since we find S $`=2`$ for the remaining Mn atoms, they match the conventional picture of Mn3+ ions. So, although the chemistry is quite complex involving holes on some oxygens, due to the strong hybridization they are not independent degrees of freedom and the system should be viewed in terms of hybridized bands, possibly supporting the use of simplified single-band models.

The breaking of symmetry due to the localization of holes on oxygens in only one of the distorted octahedra appears to highlight the very small symmetry breaking in the experimental crystal structure, where slightly different octahedra d1 and d2 have been reported . Namely, in the $`a`$-$`c`$ plane, the octahedra have long Mn-O distances of 2.07 and 2.06 Å and short Mn-O distances of 1.93 and 1.92 Å, respectively. However, we performed a relaxation by increasing the distance between the corner-Mn and O-hole by 4 $`\%`$ and the energy went down by 0.5eV per unit cell, suggesting that a full relaxation is needed. It is worth asking if a further refinement can be performed taking into account the features suggested by our results. In fact, a recent refinement for the structure of Pr0.6Ca0.4MnO3  produces local ordering not dissimilar to the results of our model.

We now compare our results with electron-microscopy experiments (EM). As can be seen in Fig. 1, the CO and OO doubles the pseudo-cubic unit cell in one direction (vertical in Fig. 1) as reported in EM . Note that the unit cell is further doubled in the horizontal direction due to the magnetic ordering although this can not be explicitly seen in EM. It is important to note that either of the doubly degenerate solutions (either holes on d1 or holes on d2) produce identical periodicity for the diffraction pattern. In a real sample, there will always be some perturbation to stabilize one of the solutions.

In experiments, although La and Ca are on average randomly distributed, little is known about local arrangement within a range of a unit cell. We investigated this issue by checking the influence of different distributions for La and Ca within the planes just above and below the basal ones. We found that if the concentration of Ca is higher in the region above a particular octahedron (thus enhancing the symmetry breaking between d1 and d2), then holes locate in that octahedron and the energy is lowered by 3.8 eV per unit cell. This result suggest that the local environment is important and should be taking into account in future refinements.

Our picture is supported by an analysis of the density of states (DOS) (Fig. 3). In the valence band, the oxygens on d1 show a net down polarization (yet the other oxygens are almost unpolarized) and the spin-polarized contribution of each type of Mn is essentially up. The top of the valence band is mainly populated by oxygen bands showing the charge-transfer insulator character of this system. The spin-polarized holes just at the bottom of the conduction band indicate that the origin of the gap is probably the localization of the charge produced by the oxygen-stripes that develop in the system, as a charge density wave (CDW).

In conclusion, we performed an ab initio study for the half doped case of La1-xCaxMnO3 considering the experimental structure  and working within the HF approximation. In contrast to the conventional model of CO that produces insulating behavior by the alternation of Mn3+ and Mn4+, our model yields an insulator because of ordering of O-holes. Nevertheless, the spin character is exactly as predicted by the conventional models, because each O-hole is bound into a local low spin state with the neighboring corner-Mn ion. The essential physics might be described with an effective Hamiltonian involving only Mn bands, but this issue requires further investigation . Interestingly, we find that this hybridized low-spin state further orders in a broken-symmetry CDW with AFM order. The unit cell and the periodicity of the oxygen-stripes are in agreement with neutron diffraction experiments. However, the O-hole density is substantial and not obviously compatible with the very small difference between d1 and d2 octahedra reported in Ref.. Since the (La,Ca) disorder will favor locally broken symmetry states, it is likely that these short scale fluctuations will restore the average symmetry of d1 and d2. Future work should allow the structure to relax within a theoretical calculation or to get a further refinement of the experimental crystal structure for La0.5Ca0.5MnO3.

The authors are indebted to Iberio de P. R. Moreira for helpful assistance with the CRYSTAL code and fruitful discussions. We are grateful for valuable suggestions from M. Calderón, N. Mathur, D. Khomskii, V. Heine, and especially L. Colombi Ciacchi. V. F. acknowledges support from the National Research Council of Argentina (CONICET) and Fundación Antorchas (Argentina). M. D. T. thanks Royal Society for support. P.B.L. acknowledges support from EPSRC.


text:
# 1 Introduction

## 1 Introduction

The hyperfine (hf) splitting in deuterium ground state has been measured with high accuracy. The most precise experimental result for it was obtained with an atomic deuterium maser and constitutes

$$\nu _{\mathrm{exp}}=\mathrm{\hspace{0.17em}327\hspace{0.17em}384.352\hspace{0.17em}522\hspace{0.17em}2}(17)\text{kHz}.$$
(1)
Meanwhile the theoretical calculation including higher order pure QED corrections gives

$$\nu _{\mathrm{QED}}=\mathrm{\hspace{0.17em}327\hspace{0.17em}339.27}(7)\text{kHz}.$$
(2)
The last number was obtained by using the theoretical result for the hydrogen hf splitting from Ref.

$$\mathrm{1\hspace{0.17em}420\hspace{0.17em}451.95}(14)\text{kHz}$$

which does not include proton structure and recoil radiative correction, and combining it with the theoretical ratio of the hf constants in hydrogen and deuterium from Ref.

$$\mathrm{4.339\hspace{0.17em}387\hspace{0.17em}6}(8)$$

based on the ratio of the nuclear magnetic moments and including the reduced mass effect in $`|\psi (0)|^2`$.

It was recognized long ago that the discrepancy

$$\nu _{\mathrm{exp}}\nu _{\mathrm{QED}}=\mathrm{\hspace{0.17em}45}\text{kHz}$$
(3)
is due to the effects caused by the finite size of deuteron. Such effects are obviously much larger in deuterium than in hydrogen. Corresponding contributions to the deuterium hf splitting were discussed long ago with some intuitive arguments , and then in more detail in Refs. .

We believe that in the past the most systematic treatment of such effects, which are due to the electron-deuteron interaction of second order in $`\alpha `$, was performed in Ref. . The effective hamiltonian of the hf interaction of second order in $`\alpha =e^2/4\pi `$ was derived therein from the elastic forward scattering amplitude of virtual photons off the deuteron.

In particular, the low-energy theorem for forward Compton scattering  was generalized in  to the case of virtual photons and a target with arbitrary spin. The corresponding contribution of the momentum transfers $`k`$, bounded from above by the inverse deuteron size $`\varkappa =\mathrm{\hspace{0.17em}45.7}`$ MeV, to the relative correction to the deuterium hyperfine structure is

$$\mathrm{\Delta }_{el}^d=\frac{3\alpha }{8\pi }\left(\mu _d2\frac{3}{\mu _d}\right)\frac{m_e}{m_p}\mathrm{ln}\frac{\varkappa }{m_e}.$$
(4)
Here $`m_e`$ and $`m_p`$ are the electron and proton masses, respectively, $`\mu _d=0.857`$ is the deuteron magnetic moment. The relative corrections $`\mathrm{\Delta }`$’s are defined here and below as the ratios of the corresponding contributions to the $`ed`$ scattering amplitude to the spin-dependent Born term in this amplitude,

$$T_0=\frac{2\pi \alpha }{3m_em_p}\mu _d(𝝈𝐬),$$
(5)
where $`𝐬`$ is the deuteron spin.

At larger momentum transfers, $`k>\varkappa `$, the amplitude of the Compton scattering on a deuteron is just the coherent sum of those amplitudes on free proton and neutron. This correction equals

$$\mathrm{\Delta }_{in}^{pn}=\frac{3\alpha }{4\pi }\frac{1}{\mu _d}(\mu _p^2\mathrm{\hspace{0.17em}2}\mu _p\mathrm{\hspace{0.17em}3}+\mu _n^2)\frac{m_e}{m_p}\mathrm{ln}\frac{m_\rho }{\varkappa }.$$
(6)
Here $`\mu _p=\mathrm{\hspace{0.17em}2.79}`$ and $`\mu _n=\mathrm{\hspace{0.17em}1.91}`$ are the proton and neutron magnetic moments; $`m_\rho =770`$ MeV is the usual hadronic scale.

Strong numerical cancellation between $`\mathrm{\Delta }_{el}`$ and $`\mathrm{\Delta }_{in}`$ is worth mentioning.

The next correction to the deuterium hyperfine structure (hfs), obtained in Ref. , is induced by the deuteron virtual excitations due to spin currents only. It is

$$\mathrm{\Delta }_{in}^{(1)}=\frac{3\alpha }{8\pi }\frac{(\mu _p\mu _n)^2}{\mu _d}\frac{m_e}{m_p}\mathrm{ln}\frac{m_p}{\varkappa }.$$
(7)
There is also a correction due to a finite distribution of the deuteron charge and magnetic moment333In the case of hydrogen this problem was considered many years ago by Zemach .. In the zero-range approximation used in Ref.  this correction is

$$\mathrm{\Delta }_f=\alpha \frac{m_e}{3\varkappa }(1+2\mathrm{ln}2).$$
(8)
## 2 Leading inelastic nuclear correction
to deuterium hyperfine structure

Leading inelastic nuclear correction is on the relative order $`\alpha m_e/\varkappa `$ (as well as the Zemach correction (8)). The corresponding effect calculated in Ref.  is additionally enhanced by a large factor $`\mu _p\mu _n=4.7`$. In the present paper we consider two more effects on the same order $`\alpha m_e/\varkappa `$. Though both of them are proportional to $`\mu _p+\mu _n=0.88`$ (and thus are essentially smaller numerically than that considered in ), we believe that their investigation is worth attention.

We use the gauge $`A_0=\mathrm{\hspace{0.17em}0}`$ where the photon propagator is

$$D_{im}(\omega ,\stackrel{}{k})=\frac{d_{im}}{\omega ^2\stackrel{}{k}^2},d_{im}=\delta _{im}\frac{k_ik_m}{\omega ^2};D_{00}=D_{0m}=\mathrm{\hspace{0.17em}0}.$$
(9)
The electron-deuteron nuclear-spin-dependent scattering amplitude generated by the two-photon exchange is

$$T=\mathrm{\hspace{0.17em}4}\pi \alpha i\frac{d^4k}{(2\pi )^4}\frac{d_{im}d_{jn}}{k^4}\frac{\gamma _i(\widehat{l}\widehat{k}+m_e)\gamma _j}{k^2\mathrm{\hspace{0.17em}2}lk}M_{mn}.$$
(10)
Here $`l_\mu =(m_e,0,0,0)`$ is the electron momentum. The structure $`\gamma _i(\widehat{l}\widehat{k}+m_e)\gamma _j`$ reduces to $`i\omega ϵ_{ijl}\sigma _l`$ where $`\stackrel{}{\sigma }`$ is the electron spin. We calculate the nuclear matrix elements entering the deuteron Compton amplitude $`M_{mn}`$ in the zero-range approximation (zra) which allows us to obtain all the results in a closed analytical form.

The inelastic $`1/\varkappa `$ contribution to hfs is induced by the combined action of the convection and spin currents. Since the convection current is spin-independent, all the intermediate states are triplet ones, as well as the ground state. Therefore, here the spin current operator

$$\frac{e}{2m_p}i𝐤\times [\mu _p𝝈_p\mathrm{exp}(i𝐤𝐫_p)+\mu _n𝝈_n\mathrm{exp}(i𝐤𝐫_n)]$$

simplifies to

$$\frac{e}{2m_p}i[𝐤\times 𝐬][\mu _p\mathrm{exp}(i𝐤𝐫_p)+\mu _n\mathrm{exp}(i𝐤𝐫_n)].$$
(11)
In the initial state $`|\mathrm{\hspace{0.17em}0}`$ the deuteron is at rest. But in the excited state the system of nucleons as a whole moves with the momentum $`𝐤`$, so that its wave function is $`|n\mathrm{exp}(i𝐤𝐑)`$, where $`|n`$ refers to the deuteron internal degrees of freedom and is a function of $`𝐫=𝐫_p𝐫_n`$; $`𝐑=(𝐫_p+𝐫_n)/2`$ is the deuteron centre of mass coordinate. Thus, a typical matrix element of the spin current can be written as

$$\frac{e}{2m_p}i𝐤\times n|\mathrm{exp}(i𝐤𝐑)𝐬[\mu _p\mathrm{exp}(i𝐤𝐫_p)+\mu _n\mathrm{exp}(i𝐤𝐫_n)]|0$$

$$=\frac{e}{2m_p}i𝐤\times n|𝐬[\mu _p\mathrm{exp}(i𝐤𝐫/2)+\mu _n\mathrm{exp}(i𝐤𝐫/2)]|0.$$
(12)
As to a typical matrix element of the convection current, it transforms now as follows:

$$\frac{e}{2m_p}n|\mathrm{exp}(i𝐤𝐑)\widehat{𝐩}_p\mathrm{exp}(i𝐤𝐫_p)+\mathrm{exp}(i𝐤𝐫_p)\widehat{𝐩}_p|0$$

$$=\frac{e}{2m_p}n|(\widehat{𝐩}+\frac{𝐤}{2})\mathrm{exp}(i𝐤𝐫/2)+\mathrm{exp}(i𝐤𝐫/2)\widehat{𝐩}|0=\frac{e}{m_p}n|\widehat{𝐩}\mathrm{exp}(i𝐤𝐫/2)|0;$$
(13)
here $`\widehat{𝐩}`$ acts on the relative coordinate $`𝐫`$.

At first let us take as intermediate states $`|n`$ in the corresponding nuclear Compton amplitude just plane waves, eigenstates of $`\widehat{𝐩}`$. In this way we take into account all the states with $`l0`$, which are free ones in our zero range approximation, and in addition the $`{}_{}{}^{3}S_{1}^{}`$ wave function in the free form $`\psi _p(r)=\mathrm{sin}pr/pr`$ (the deviation of the $`{}_{}{}^{3}S_{1}^{}`$ wave function from the free one will be considered below). Then, with the zra deuteron wave function

$$\psi _0(r)=\sqrt{\frac{\varkappa }{2\pi }}\frac{\mathrm{exp}(\varkappa r)}{r},$$
(14)
the only matrix element entering the amplitude is

$$\psi _0|\mathrm{exp}(\pm i𝐤𝐫/2)|𝐩=\frac{\sqrt{8\pi \varkappa }}{(𝐩\pm 𝐤/2)^2+\varkappa ^2}.$$
(15)
In this way the amplitude itself simplifies to

$`M_{mn}^{(2)}`$ $`=`$ $`\left({\displaystyle \frac{e}{2m_p}}\right)^22\varkappa \omega {\displaystyle \frac{d𝐩}{\pi ^2}\left\{\frac{\mu _p}{[(𝐩𝐤/2)^2+\varkappa ^2]^2}+\frac{\mu _n}{[(𝐩𝐤/2)^2+\varkappa ^2][(𝐩+𝐤/2)^2+\varkappa ^2]}\right\}}`$ (16)
$`\times {\displaystyle \frac{\mathrm{\hspace{0.17em}2}p_miϵ_{nrs}k_rs_s\mathrm{\hspace{0.17em}2}p_niϵ_{mrs}k_rs_s}{\omega ^2(p^2+k^2/4+\varkappa ^2)^2/m_p^2}}.`$
Due to the account for the motion of the system as a whole in the intermediate states, this expression differs from the corresponding one from our previous paper  in two respects. First, in  the operator $`𝐩_p`$ in (13) was identified with $`𝐩`$. Thus, therein instead of $`2p_{m,n}`$ in the analogue of the present formula (16), we obtained $`(2pk/2)_{m,n}`$. At present, in (16) the term proportional to $`\mu _n`$ is an odd function of $`𝐩`$, and therefore vanishes after integration over $`d𝐩`$. Second, in the denominator the energy difference has acquired the contribution $`k^2/4m_p`$ , which is the kinetic energy of the $`pn`$ system as a whole, and thus $`(p^2+\varkappa ^2)/m_p`$ has transformed into $`(p^2+k^2/4+\varkappa ^2)/m_p`$.

Now we substitute (16) into (10) and take the integral over $`\omega `$ under the condition $`\omega \varkappa ^2/m`$. For the relative correction to the hf structure we obtain

$`\mathrm{\Delta }_{in}^{(2)}`$ $`=`$ $`{\displaystyle \frac{2\alpha \varkappa \mu _pm_e}{\pi ^4\mu _dm_p}}{\displaystyle \frac{d𝐩d𝐤}{k^4}\frac{𝐩𝐤}{[(𝐩𝐤/2)^2+\varkappa ^2]^2}\left[\frac{m_p}{p^2+k^2/4+\varkappa ^2}\frac{3}{2k}\right]}.`$ (17)
The result of integration over $`𝐩`$ and then over $`𝐤`$ reads

$$\mathrm{\Delta }_{in}^2=\alpha \frac{\mu _p}{\mu _d}\frac{m_e}{\varkappa }\frac{6\alpha }{\pi }\frac{\mu _p}{\mu _d}\frac{m_e}{m_p}\mathrm{ln}\frac{m_p}{\varkappa }.$$
(18)
The logarithmic contribution here originates from integration of the term $`3/2k`$ in the square brackets in (17) over the range $`\varkappa ^2/m_pk\varkappa `$. The result (18) differs from the corresponding one of  by a term proportional to $`\mu _p+\mu _n`$, which is relatively small numerically. It is only natural that our present account for the motion of the proton-neutron system as a whole in the intermediate states results in the correction proportional to $`\mu _p+\mu _n`$.

Let us calculate now the correction $`\mathrm{\Delta }_{in}^{(3)}`$ corresponding to the effect of deviation of the intermediate $`{}_{}{}^{3}S_{1}^{}`$ wave function $`\mathrm{\Psi }_p(r)`$ from the free one. In the zra $`\mathrm{\Psi }_p(r)`$ reads

$$\mathrm{\Psi }_p(r)=\frac{\mathrm{sin}pr}{pr}\frac{1}{\varkappa +ip}\frac{\mathrm{exp}(ipr)}{r}=\frac{\varkappa \mathrm{sin}prp\mathrm{cos}pr}{pr(\varkappa +ip)}.$$
(19)
It follows, for instance, from the orthogonality to the deuteron wave function (14). We use below the function

$$\rho _p(r_1,r_2)=\mathrm{\Psi }_p(r_1)\mathrm{\Psi }_p^{}(r_2)\psi _p(r_1)\psi _p^{}(r_2)=\frac{p\mathrm{cos}p(r_1+r_2)\varkappa \mathrm{sin}p(r_1+r_2)}{(\varkappa ^2+p^2)pr_1r_2}.$$
(20)
Then, after integration over $`\omega `$ the expression for $`\mathrm{\Delta }_{in}^{(3)}`$ reads

$`\mathrm{\Delta }_{in}^{(3)}={\displaystyle \frac{4\alpha (\mu _p+\mu _n)m_e}{\pi ^3\mu _dm_p}}{\displaystyle 𝑑k𝑑pp^2𝑑𝐫_1𝑑𝐫_2\psi _0(r_1)\psi _0(r_2)\rho _p(r_1,r_2)}`$
$`\times {\displaystyle \frac{\mathrm{sin}kr_1}{kr_1}}\left[{\displaystyle \frac{\mathrm{sin}kr_2}{kr_2}}{\displaystyle \frac{(1+\varkappa r_2)}{(kr_2)^2}}\left({\displaystyle \frac{\mathrm{sin}kr_2}{kr_2}}\mathrm{cos}kr_2\right)\right]\left[{\displaystyle \frac{m_p}{p^2+k^2/4+\varkappa ^2}}{\displaystyle \frac{3}{2k}}\right].`$ (21)
The integral over $`p`$ is

$`{\displaystyle _0^{\mathrm{}}}𝑑p{\displaystyle \frac{p^2\rho _p(r_1,r_2)}{p^2+k^2/4+\varkappa ^2}}={\displaystyle \frac{2\pi }{r_1r_2k^2}}\left[(Q+\varkappa )\mathrm{exp}[Q(r_1+r_2)]2\varkappa \mathrm{exp}[Q(r_1+r_2)]\right],`$ (22)
where $`Q=\sqrt{\varkappa ^2+k^2/4}`$. Now we integrate (2) over $`r_1`$, $`r_2`$, and then over $`k`$. The final result for the discussed correction reads:

$$\mathrm{\Delta }_{in}^{(3)}=\alpha \frac{\mu _p+\mu _n}{\mu _d}\frac{m_e}{\varkappa }\frac{1}{3}(22\mathrm{ln}2)+\frac{3\alpha }{\pi }\frac{\mu _p+\mu _n}{\mu _d}\frac{m_e}{m_p}\mathrm{ln}\frac{m_p}{\varkappa }.$$
(23)
Again, it is only natural that due to common selection rules the contribution of the $`{}_{}{}^{3}S_{1}^{}`$ intermediate state is proportional to $`\mu _p+\mu _n`$. Let us note also that the first term in (23) is additionally suppressed by a small numerical factor $`(22\mathrm{ln}2)/3=0.20`$.

At last, we wish to come back to the effect due to a finite distribution of the deuteron charge and magnetic moment. The Zemach correction $`\mathrm{\Delta }_f`$ (8) can be also easily derived in the present approach. Using the identity

$$\psi _0|\widehat{𝐩}\mathrm{exp}(i𝐤𝐫/2)|\psi _0=\frac{𝐤}{4}\psi _0|\mathrm{exp}(i𝐤𝐫/2)|\psi _0,$$

we obtain the corresponding amplitude:

$`M_{mn}^f`$ $`=`$ $`\left({\displaystyle \frac{e}{2m_p}}\right)^2(\mu _p+\mu _n)\omega \left[F^2(k)1\right]{\displaystyle \frac{k_miϵ_{nrs}k_rs_sk_niϵ_{mrs}k_rs_s}{\omega ^2(p^2+k^2/4+\varkappa ^2)^2/m_p^2}},`$ (24)
where $`F(k)`$ is the deuteron form factor in the zero-range approximation

$`F(k)=\psi _0|\mathrm{exp}(i𝐤𝐫/2)|\psi _0={\displaystyle \frac{4\varkappa }{k}}\mathrm{arctan}{\displaystyle \frac{k}{4\varkappa }}.`$ (25)
Let us note that in our approximation both electric and magnetic form factors, which in the present case enter the convection current and spin current matrix elements respectively, coincide and equal $`F(k)`$.

The integration over $`\omega `$ leads to the following result for the relative correction $`\mathrm{\Delta }_f`$

$`\mathrm{\Delta }_f={\displaystyle \frac{8\alpha (\mu _p+\mu _n)m_e}{\pi \mu _d}}{\displaystyle _0^{\mathrm{}}}{\displaystyle \frac{dk}{k^2}}[F^2(k)1]=\alpha {\displaystyle \frac{\mu _p+\mu _n}{\mu _d}}{\displaystyle \frac{m_e}{\varkappa }}{\displaystyle \frac{1}{3}}(1+2\mathrm{ln}2).`$ (26)
There is no logarithmic term in $`\mathrm{\Delta }_f`$ since $`F^2(k)1k^2`$ for $`k\varkappa `$. In fact, the result (26) agrees with (8) since to our accuracy $`\mu _p+\mu _n=\mu _d`$.

The corrections (18), (23), (26) combine into a compact result

$$\mathrm{\Delta }_c=\alpha \frac{\mu _n}{\mu _d}\frac{m_e}{\varkappa }\frac{3\alpha }{\pi }\frac{\mu _p\mu _n}{\mu _d}\frac{m_e}{m_p}\mathrm{ln}\frac{m_p}{\varkappa }.$$
(27)
Let us notice that its logarithmic part coincides with the corresponding logarithmic term in  (see formula (27) therein). This is quite natural: the log is dominated by small $`k`$, so that extra power of $`k`$, which arises from the recoil of the $`pn`$ system as a whole, cannot influence it.

The leading term in (27) coincides with the result of Ref. 444We are sorry for misquoting the result of Ref.  in our paper .. However, we could not find any correspondence between our arguments and those of Ref. . In particular, it is stated explicitly in Ref.  that the motion of the intermediate $`pn`$ system as a whole is neglected therein.

## 3 Discussion of results

Our total result for the nuclear-structure corrections to the deuterium hf structure, comprising all the contributions, (4), (6), (7), (27), is

$$\mathrm{\Delta }=\alpha \frac{\mu _n}{\mu _d}\frac{m_e}{\varkappa }\frac{3\alpha }{\pi }\frac{\mu _p\mu _n}{\mu _d}\frac{m_e}{m_p}\mathrm{ln}\frac{m_p}{\varkappa }$$
(28)
$$+\frac{3\alpha }{8\pi }\frac{(\mu _p\mu _n)^2}{\mu _d}\frac{m_e}{m_p}\mathrm{ln}\frac{m_p}{\varkappa }$$

$$+\frac{3\alpha }{8\pi }\frac{1}{\mu _d}(\mu _d^2\mathrm{\hspace{0.17em}2}\mu _d\mathrm{\hspace{0.17em}3})\frac{m_e}{m_p}\mathrm{ln}\frac{\varkappa }{m_e}+\frac{3\alpha }{4\pi }\frac{1}{\mu _d}(\mu _p^2\mathrm{\hspace{0.17em}2}\mu _p\mathrm{\hspace{0.17em}3}+\mu _n^2)\frac{m_e}{m_p}\mathrm{ln}\frac{m_\rho }{\varkappa }.$$

Numerically this correction to the hf splitting in deuterium constitutes

$$\mathrm{\Delta }\nu =\mathrm{\hspace{0.17em}50}\text{kHz}.$$
(29)
It should be compared with the lacking $`45`$ kHz (see (3)). We believe that the agreement is quite satisfactory if one recalls the crude nuclear model (zra) used here; in particular the deuteron form factors, as calculated in the zra, are certainly harder than the real ones, and thus in zra the negative Zemach correction is underestimated.

Let us mention here that in a recent paper  elastic contributions and the Zemach effect were considered in a quite different theoretical technique, but with some phenomenological desription of the deuteron form factors. The result is smaller than the corresponding part of ours by 13 kHz.

Clearly, the nuclear effects discussed are responsible for the bulk of the difference between the pure QED calculations and the experimental value of the deuterium hf splitting. The calculation of this correction, including accurate treatment of nuclear effects, would serve as one more sensitive check of detailed models of deuteron structure.

## Acknowledgements

We are extremely grateful to J.L. Friar for insistently attracting our attention to the role of the $`{}_{}{}^{3}S_{1}^{}`$ positive-energy state in the inelastic contribution. The investigation was supported in part by the Russian Foundation for Basic Research through Grants Nos. 03-02-17612, 03-02-16510, and through Grant for Leading Scientific Schools.