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# References

Radiative Lifetimes of Single Excitons in Semiconductor Quantum Dots- Manifestation of the Spatial Coherence Effect

E. Dekela, D.V. Regelmana, D. Gershonia, E. Ehrenfreunda, W.V. Schoenfeldb and P.M. Petroff b
aDepartment of Physics Technion–Israel Institute of Technology, Haifa 32000, Israel

bMaterials Department, University of California, Santa Barbara, CA 93106, USA

Using time correlated single photon counting combined with temperature dependent diffraction limited confocal photoluminescence spectroscopy we accurately determine, for the first time, the intrinsic radiative lifetime of single excitons confined within semiconductor quantum dots. Their lifetime is one (two) orders of magnitude longer than the intrinsic radiative lifetime of single excitons confined in semiconductor quantum wires (wells) of comparable confining dimensions. We quantitatively explain this long radiative time in terms of the reduced spatial coherence between the confined exciton dipole moment and the radiation electromagnetic field.

PACS numbers: 78.66.Fd, 71.35.-y, 71.45.Gm, 85.30.Vw

In intrinsic direct bandgap semiconductors the interaction of excitons with the electromagnetic radiation field leads to a stationary state called exciton-polariton. This elementary excitation is a coherent state of the entire macroscopic three dimensional (3D) crystal, and as such it does not decay radiatively . In geometrically restricted semiconductor quantum structures such as quantum wells (QWs), wires (QWRs) or dots (QDs) the situation is different. In these systems, the translational symmetry of the crystalline potential is removed in one, two or three directions, respectively. As a result, the three dimensional electromagnetic radiation field interacts with excitons of lower dimensionality (2D, 1D or 0D, respectively). This dimensionality difference gives rise to exciton-polariton modes that are not stationary states. These modes have finite energy width, $`\mathrm{\Delta }E`$, and consequently they do decay radiatively, \[2-5\] with intrinsic radiative lifetime $`\mathrm{}/\mathrm{\Delta }E`$, which, for typical $`GaAs/AlGaAs`$ QWs, amounts to a few tens of picoseconds, while for QWRs of comparable dimensions it is considerably longer.. This counter-intuitive result was explained in terms of the reduced exciton-coherence volume, imposed by the additional lateral confinement.

The arguments of this exciton-polariton theory explain also the considerably longer photoluminescence (PL) decay times which were measured in these systems.\[7-9\] They result from the thermal distribution of the excitonic population, where only a small fraction occupies the optically active part of the available excitonic phase space. Consequently, the dimensional dependent density of energy states reveals itself in the temperature dependence of the radiative decay times. Indeed, both theory and experiment show that these are proportional to the temperature, $`T`$, in QWs  and to $`\sqrt{T}`$ in QWRs. When these considerations are applied to QDs, longer intrinsic radiative lifetimes are expected, and their characteristic $`\delta `$-function like density of energy states leads to $`T`$ independent radiative decay times. Though numerous experimental studies of the PL decay times from QD assemblies  and more recently from single QDs , have already been carried out, this theoretically expected behavior has never been observed.

In this Letter we report on the first experimental determination of the radiative lifetime of single excitons confined within semiconductor QDs. We determine this fundamental property of 0D excitons by applying time correlated single photon counting combined with confocal microscopy to single self assembled quantum dots (SAQDs). The temporal evolution of the PL emission following pulse excitation at various intensities is measured and the PL intensity is quantitatively analyzed taking into account the interaction between a number of excitons (multiexcitons) confined within one QD. Our intensity and temporal analysises unambiguously determine the intrinsic radiative lifetime of single QD excitons. We show that they are few nanoseconds (ns) long and $`T`$ independent.

We studied two types of SAQDs. Both were fabricated by molecular beam epitaxial deposition of a defect free coherently strained epitaxial layer of $`InAs`$ on either directly on a $`GaAs`$ layer by the partially covered islands method (PCI sample) or on an $`AlGaAs`$ host layer (AHL sample). The layer sequences, compositions and widths are reported elsewhere. During the growth of the strained layers, the samples were not rotated. Thus, a gradient in the QDs density was formed and low density areas, in which the average distance between neighboring QDs is larger than the spatial resolution of our microscope were found on their surfaces. A key difference between the two samples is their non-radiative decay rates. The presence of $`Al`$ within the SAQDs’ host layers of the AHL sample gives rise to very efficient non-radiative recombination centers, close to the SAQDs. Therefore, at low excitation densities their PL decay time is extremely short. It is shown below that in spite of this difference, the determined radiative lifetimes of single excitons in both samples are roughly the same, as expected from the dimensional considerations.

The PL was excited by a synchronously mode-locked 3 ps pulsed dye-laser through a low temperature confocal microscope, which is described elsewhere. The system provides spectral and spatial resolutions of 0.2 meV and $``$0.5 $`\mu m`$, respectively. In addition, a thermoelectrically cooled avalanche silicon photodiode was used for photon counting with temporal resolution of 200 ps.

In Fig.1a(1b) we present by solid lines temporally integrated PL spectra from a single PCI (AHL) SAQD for various $`1.75`$ eV pulsed excitation powers. At the lowest power PL spectrum of Fig.1a a single narrow spectral line is observed at energy of 1.284 eV. We denote this line by $`A_1`$. Its linewidth is limited by our setup resolution. As the excitation power increases, a satellite spectral line ($`A_2`$) appears 3.5 meV below $`A_1`$ and a higher energy spectral line, ($`B_1`$) emerges at 1.324 eV, 40 meV above $`A_1`$. At yet higher excitation power line $`B_1`$ develops a 1.5 meV lower in energy satellite ($`B_2`$). Further increase in the excitation power results in an increase in the number of satellites which gradually form spectral emission bands to the lower energy side of the lines $`A_1`$ and $`B_1`$. In addition, new higher energy groups of lines, $`C`$, $`D`$ and $`E`$, respectively, gradually emerge and develop their own satellites and lower energy bands. The various lines are marked by letters which represent the energy group to which they belong and numerical subscripts which represent their appearance order with increasing the excitation power. As the power increases, after reaching maximum, the intensity of the emission from the various spectral lines ceases to increase and it remains constant with further increase in the power. This is in marked difference from their behavior under continuous wave (cw) excitation mode, where they gradually disappear.

The behavior of the PL spectra from the AHL sample (Fig.1b) is similar, except for two major differences: First, only two groups of lines, A and B, are observed. Second, the satellite spectral line $`A_2`$ appears before the line $`A_1`$. We explain the first difference by the different dimensions of the two dots. Whereas the first, larger one, has 4-5 confined electron levels, the second one has only two. The second difference is due to the efficient non-radiative decay process associated with the $`Al`$ atoms in the AHL sample. At low excitation densities, before it is saturated, it inhibits the observation of the line $`A_1`$. Our model simulations are presented in the figures by gray lines.

In Fig.2a(2c) we present the PL intensity of the single SAQD spectral line $`A_1`$($`B_2`$) from the PCI(AHL) sample as a function of time after the excitation pulse. The PL transients were measured at 20K for various excitation powers. In general, for each spectral line there are two distinct time domains. In the first, the emission intensity rises and in the second, it decays. As a rule we noted (not shown) that the lower is the energy of a given spectral group of lines, the longer are their rise and decay times. Within a given group of lines, however, lower energy lines rise and decay faster. Our model calculations for the $`A_1`$($`B_2`$) line of the PCI(AHL) sample are presented for comparison in Fig.2b(2d). Clearly, the rise time of a particular spectral line, strongly depends on the excitation power. The higher the power is, the longer is the rise time, while the decay time is hardly affected. We note that the temporal behavior of the spectral lines from the different samples is very similar. The main difference is the density of excitation needed to observe the PL from the second sample. This difference, like the difference in the order by which the spectral lines appear with increasing excitation power is explained by the vast efficiency difference between the non-radiative recombinations in the two samples. In the inset to Figs.2a(2c) we display by symbols the measured rise time of the spectral line $`A_1`$($`B_2`$), as a function of the excitation power. Our model calculations are presented for comparison in the inset to Fig.2b(2d). Similar measurements and calculations are presented in Fig.3a and Fig.3b, respectively, for the spectral line $`A_1`$ of an SAQD from the PCI sample, at higher sample temperature of 70K.

The PL spectrum of a semiconductor QD excited by a short laser pulse is due to optical transitions between multiexciton states. The excitation generates population of electron-hole (e-h) pairs within the dot. The many e-h pairs form a correlated quantum state which we define as a multiexciton. The photoexcited carriers reach thermal distribution on a very short time scale compared with the time required for radiative recombination of an e-h pair. Thus, at cryogenic temperatures, the specific excited multiexciton rapidly relaxes to its ground level. A radiative annihilation of one of the e-h pairs that compose the multiexciton may then occur by the emission of a photon, which carries the energy difference between the annihilated multiexcitonic ground level and that of the newly generated one. The new multiexciton, with one less e-h pair quickly relaxes to its ground level and eventually recombines by losing yet another e-h pair. The process continues sequentially, until the dot remains empty of excitons. For a small number of QD excitons ($`2`$), the probability of non-radiative recombination becomes increasingly important. First, since the non-radiative decay channels are no longer screened by the carriers in the QD and its vicinity. Second, since the radiative recombination has fewer channels and its rate is much slower.

In order to understand the spectral evolution of the SAQD PL with excitation power and with time, a knowledge of the various multiexcitons energies and recombination rates is required. Our model provides a straightforward way for calculating these energies using a minimal set of parameters (i.e., the single carrier energy levels and the exchange energies between these levels), which can be directly obtained from the PL spectrum itself.. The recombination rates are given by the model in terms of the QD single exciton radiative lifetime ($`\tau _1`$) through the use of the dipole approximation, together with symmetry and total angular momentum conservation considerations. These energies and rates are used for calculating the spectra in Fig.1, where a Gaussian spectral broadening of 0.5 meV for each discrete multiexcitonic level was used, and the statistical nature of the pulse photogeneration was taken into account. Thus, $`<N_X>`$ in Fig.1 represents the average number of photogenerated pairs (or the multiexciton order) in the QD by each laser pulse. Since the spectra in Fig.1 are temporally integrated, each multiexciton of order $`N_X`$ contributes exactly one radiative recombination to the measured spectrum. From this simple argument, it follows that the comparison between the calculated spectra of Fig.1 and the measured spectral density of counts per pulse at saturation, directly yields the collection efficiency of our setup. This calculated number is almost model independent since the number of photons per recombination is easily obtained from total spin conservation considerations. The efficiency obtained from Fig.1, $``$5$`\times 10^5`$, does not depend on the efficiency of excitation or on the non-radiative processes and it is in a very good agreement with our estimates based on measuring the reflected laser light.

We use the multiexcitons calculated recombination rates as input parameters to a set of coupled rate equations which describe the temporal behavior of the pulsed photoexcited single QD. The rate equations are analytically solved for the cw and pulsed excitation modes. The cw solution yields a direct determination of the radiative lifetime $`\tau _1`$. For this task one uses the determined efficiency of the experimental system and the cw excitation power dependence of the PL spectrum. As mentioned above, when the cw excitation power increases the various SAQD PL discrete spectral lines reach maximum emission and then lose intensity with further increase in the power (not shown). The steady-state number of QD excitons when a certain line reaches maximum is thereby given by comparison with the analytic solution of the rate equations. The calibrated emission intensity at these conditions, accurately determines $`\tau _1`$.

Another independent way of determining $`\tau _1`$ is demonstrated by the curves in Figs.2b and 2d which represent the solution to the rate equations of the pulsed excitation mode. Two parameters are used for generating all the simulated transient curves. Namely, $`\tau _1`$ and the ratio between it and the non radiative lifetime ($`\tau _{nr}`$). From the comparison between the measured data (Figs.2a,2c and their insets) and the calculated ones (Figs.2b, 2d and their insets) we find that the best fit for the PCI sample is obtained when $`\tau _1/\tau _{nr}5`$. For this and higher ratios, $`\tau _{nr}`$ can be directly obtained from the PL decay time of $`A_1`$, which exponentially decays within $`0.8\pm 0.1`$ ns ($`\tau `$ in Fig.2a). Consequently, $`\tau _1`$ that we deduced for the PCI SAQDs at this temperature is $`4\pm 1`$ ns, in very good agreement with its PL efficiency determination..

We state here that the determination of $`\tau _1`$ is not very sensitive to $`\tau _{nr}`$ since it is determined mainly from the power dependence of the rise time. Thus, variations in $`\tau _1/\tau _{nr}`$ ratio from zero to almost infinity yields only up to a factor of two change in the deduced $`\tau _1`$. Similarly, we determined $`\tau _1`$ of the AHL SAQDs to be $`5\pm 1`$ ns, and more than 2 orders of magnitude longer than their $`\tau _{nr}`$.

The decay time of the PL in the PCI sample is found to rapidly increase with $`T`$, while the rise time hardly changes. This is evident from the PL decay time of the $`A_1`$ line at 70K ($`\tau `$ in Fig.3a), which is $`5\pm 1`$ ns long. We believe that this is due to reduction in the non-radiative rate due to thermal activation of trapped charges that act as non radiative centers in the vicinity of the SAQD. The best fits in Fig.3b were obtained with $`\tau _1/\tau _{nr}1`$. This means that at this temperature the non-radiative rate can be neglected, and the radiative time which determines the PL rise time, now determines its decay time as well. The AHL sample non-radiative rates are activated with increasing $`T`$ and they become even faster. They render the temporal resolution of the emission from discrete PL lines at elevated $`T`$, nearly impossible.

The lifetime that we obtain for both samples, using these two independent experimental methods, amounts to 4-6 ns, and it is temperature independent. This is much longer than the measured PL decay times from single SAQDs and from SAQD assemblies, where typically, like here, low temperature sample dependent decay times of subnanosecond are reported. We show here that this is because at low excitation densities the decay time depends crucially on the non-radiative recombinations, while at high excitation densities one measures faster decays of multiexcitons. Our approach, which is independent of the measured PL decay time, clearly circumvent these impediments. We demonstrated that only at 70K, when the non-radiative decay process of the PCI sample is blocked, the PL decay is purely radiative and $`\tau _1`$ can be directly obtained from its measurement. We also demonstrated that even for the QDs in the AHL sample long radiative lifetimes are deduced, in spite of their very fast non radiative decay rates.

The QD single exciton radiative lifetime is much longer than the intrinsic radiative time of higher dimensional systems such as wires and wells. Following the arguments of Andreani, and Citrin who calculated the intrinsic radiative lifetimes of single excitons in semiconductor QWs and QWRs, respectively, we find for excitons in spherical QDs:

$$\tau _0^{QD}=nm_0c/e^2fk_{ex}^2,$$
(1)
where $`n`$ ,$`m_0`$, $`e`$ and $`c`$ are the material index of refraction, electronic mass, electron charge and speed of light, respectively, $`f`$ is the confined exciton oscillator strength and $`k_{ex}=n\omega /c`$ is the exciton wavevector in the material. For exciton energy $`\mathrm{}\omega `$=1.35 eV and $`f`$=0.5 for QDs of these dimensions, we get $`\tau _0^{QD}`$=4.2 ns, in reasonable agreement with our temperature independent experimental findings. We therefore conclude that the long QDs single exciton radiative lifetimes that we measured are due to the small spatial phase coherence between the 3D confined excitonic dipole and the electromagnetic radiation field in the semiconductor matter.

Acknowledgments – The work was supported by the Israel Science Foundation and by the Israel-US Binational Science Foundation.

Figure Captions

* a)(b))PL spectra from a single SAQD from the PCI(AHL) sample for various pulsed excitation powers. The gray lines and right axes represent our model simulations.
* The intensity of line $`A_1`$($`B_2`$) from a single SAQD of the PCI(AHL) sample $`vs.`$ time after the excitation pulse measured a)(c)) for various excitation powers and calculated b)(d)) for various average number of photogenerated QD excitons, $`<N_x>`$. The insets to a) and c) ( b) and d)) display the measured (calculated) rise times of the PL, $`vs.`$ excitation power( $`<N_x>`$).
* The intensity of line $`A_1`$ from SAQD from the PCI sample $`vs.`$ time at 70K. a)(b))Measured (calculated) for various powers ($`<N_x>`$ values). The inset display the measured (calculated) rise time of the PL $`vs.`$ the excitation power ($`<N_x>`$).


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# 𝑒^± Pair Cascades and Precursors in Gamma-Ray Bursts

## 1 Introduction

The non-thermal $`\gamma `$-ray spectrum of Gamma-Ray Burst sources (GRBs) is thought to arise in shocks which develop beyond the radius at which the relativistic fireball from the initial event has become optically thin to scattering. However, the observed spectra are hard, with a significant fraction of the energy above the $`\gamma \gamma \text{e}^\pm `$ formation energy threshold, and a high compactness parameter can result in new pairs being formed outside the originally optically thin shocks responsible for the primary radiation. New pairs can be made as some of the initial energetic photons are backscattered and interact with other incoming photons. Such effects have been considered by Madau & Thompson (2000) and Thompson & Madau (2000), who investigated the acceleration of new pairs for a particular fireball model. Dermer & Böttcher (2000) considered the effect of pair formation for an external shock model of GRB, in which the compactness parameter is relatively low, while Madau, Blandford & Rees (2000) investigated the effects of Compton echos produced by pairs.

Here we present a simplified discussion of the generic effects of pair formation in a specific class of models. We suppose that the central engine gives rise to an unsteady baryonic wind, which is relativistic, carries a magnetic field, and lasts for a time $`t_w`$. A fraction of the wind energy is converted into $`\gamma `$-rays via internal shocks; the remaining wind energy drives a blast wave which decelerates as it sweeps up the external medium, and gives rise to the afterglow emission. The $`\gamma `$-rays would propagate ahead of the blast wave, leading to pair production (and an associated deposition of momentum) into the external medium. The pair cascades saturate after the external (pair-enriched) medium reaches a critical bulk Lorentz factor, which is generally below that of the original relativistic wind. For external baryonic densities similar to those in molecular clouds the pairs can achieve scattering optical depths $`\tau _\pm \text{ }<1`$. Even for less extreme external densities the effect of the additional pairs can be substantial, increasing the radiative efficiency of the blast wave and leading to distortions of the original spectrum. This provides a potential tool for diagnosing the compactness parameter of the bursts and thus the radial distance at which shocks producing an observed luminosity can occur. It also provides a tool for diagnosing the baryonic density of the external environment of the bursts, and testing the association with star-forming regions.

## 2 Scattering and Two-photon Pair Formation

Consider an initial input radiation spectrum produced by the fireball of the form

$$\varphi (ϵ)=\frac{F}{m_ec^2ϵ_o^2q}(ϵ/ϵ_o)^\beta \text{cm}\text{-2}\text{s}\text{-1};\text{for}ϵϵ_o,$$
(1)
where $`F=L/4\pi d_L^2`$ is the observed energy flux, $`ϵ=h\nu /m_ec^2`$ is photon energy in electron rest-mass units, $`ϵ_o0.21.0`$ is the break energy above which the photon number spectral index $`\beta 23`$, and below which the spectral slope is flatter, e.g. $`\alpha 2/3`$ for a simple low-energy cutoff synchrotron spectrum (although for the present purposes the exact low energy slope is unimportant), with $`q1`$ a normalization constant. For most values of the low and high energy slopes, the majority of the photons in the spectrum are near the break frequency.

For an $`\text{e}^\pm `$ moving away radially from the source of radiation with a velocity characterized by a Lorentz factor $`\mathrm{\Gamma }`$, taking into account the Klein-Nishina drop-off in the scattering cross section above $`ϵ1`$, the effective fraction of photons contributing to accelerating the electron is $`_{ϵ_o}^\mathrm{\Gamma }\varphi (ϵ)𝑑ϵ=q^1ϵ_o^{\beta 2}(\beta 1)^1[\mathrm{\Gamma }^1ϵ_o^1]q^1ϵ_o^1(\beta 1)^1`$ for $`\beta >1`$. At a distance $`r`$ in front of the radiation source, an $`\text{e}^\pm `$ can be accelerated to a maximum value of $`\mathrm{\Gamma }`$ satisfying

$$\frac{L}{4\pi r^2}\frac{1}{qϵ_o(\beta 1)}(\sigma _T/2)\mathrm{\Delta }t\mu m_ec^2\mathrm{\Gamma },$$
(2)
where the cross section near $`ϵ1`$ is approximately $`\sigma _T/2`$, $`\mu m_e`$ is the effective mass per scatterer (equation ), and $`\mathrm{\Delta }t`$ is the effective duration of the light pulse as seen by the electron. The latter is either $`\mathrm{\Delta }tr/2c\mathrm{\Gamma }^2`$ (impulsive regime at small radii), or $`\mathrm{\Delta }tt_w`$ (wind regime), depending on which one is smallest at a given radius, where $`t_w`$ is the duration of the wind, or essentially the burst duration as seen by a distant observer. Equation (2) says that the total time-integrated momentum of the radiation intercepted by the electrons in the Thompson limit is converted into their kinetic energy of motion, taking into account the effective mean mass per scatterer. (This follows directly from the mean rate of momentum transfer per particle in a steady flow, e.g., as discussed in Madau & Thompson, 2000, their equation (2), (10) and (23), noting that our definition of $`\mu `$ differs from theirs.) Here we define $`\mu `$ as the effective mass per scattering electron or positron in units of electron mass,

$$\mu m_e=\frac{\mathrm{mass}}{\mathrm{scatterer}}=m_p\frac{[1+2(n_\pm /n_p)(m_e/m_p)]}{[1+(2n_\pm /n_p)]}\{\begin{array}{cc}m_p\hfill & \text{ for }n_\pm n_p\text{:}\hfill \\ (2n_\pm /n_p)^1m_p\hfill & \text{ for }1<2n_\pm /n_p<m_p/m_e\text{;}\hfill \\ m_e\hfill & \text{ for }2n_\pm /n_p>m_p/m_e\text{.}\hfill \end{array}$$
(3)
Defining a reference radius

$$r_{}=L\sigma _T/16\pi m_ec^3=5\times 10^{19}L_{w50}\text{cm},$$
(4)
from equation (2) the maximum $`\text{e}^\pm `$ Lorentz factor is

$$\mathrm{\Gamma }_\pm (r)\{\begin{array}{cc}\mu ^{1/3}\left(\frac{1}{qϵ_o(\beta 1)}\right)^{1/3}\left(r_{}/r\right)^{1/3},\hfill & \text{for }\mathrm{\Delta }t(r/2c\mathrm{\Gamma }^2)\text{;}\hfill \\ \mu ^1\left(\frac{1}{qϵ_o(\beta 1)}\right)\left(\frac{2ct_w}{r_{}}\right)\left(r_{}/r\right)^2,\hfill & \text{for }\mathrm{\Delta }tt_w\text{.}\hfill \end{array}$$
(5)
The transition from the $`\mathrm{\Gamma }r^{1/3}`$ to the steeper $`\mathrm{\Gamma }r^2`$ occurs at a critical radius $`r_cr_{}`$, for which the Lorentz factor is $`\mathrm{\Gamma }_c`$,

$`r_c=`$ $`2.2\times 10^{14}\mu ^{2/5}\left(qϵ_o(\beta 1)\right)^{2/5}L_{w50}^{2/5}t_w^{3/5}`$
$`\mathrm{\Gamma }_c=`$ $`6.1\times 10^1\mu ^{1/5}\left(qϵ_o(\beta 1)\right)^{2/15}L_{w50}^{1/5}t_w^{1/5}.`$ (6)
A second criterion for a maximum $`\text{e}^\pm `$ Lorentz factor comes from the pair formation threshold, since the incident photon $`ϵ`$ and the back-scattered photon $`ϵ_r`$ must satisfy $`ϵϵ_r2`$. The back-scattered photon, has, in the reference frame of the scattering $`\text{e}^\pm `$ moving with $`\mathrm{\Gamma }_\pm `$, an energy of at most $`ϵ_r^{}\text{ }<1/2`$; this photon cannot give rise to a further pair unless it collides with another photon with, in the lab frame, an energy exceeding $`4\mathrm{\Gamma }_\pm `$. Thus the fraction of incident photons able to make pairs through the two-photon mechanism against target photons backscattered from $`\text{e}^\pm `$ moving with $`\mathrm{\Gamma }_\pm `$ is $`q^1ϵ_o^2_{4\mathrm{\Gamma }}^{\mathrm{}}\varphi (ϵ)𝑑ϵ=q^1ϵ_o^{\beta 2}(\beta 1)^1(4\mathrm{\Gamma })^{1\beta }`$. The maximum Lorentz factor achievable by pairs before the two-photon cascade cuts off is that for which the compactness parameter has dropped to unity,

$$\mathrm{}(r)=\frac{L}{4\pi r^2}\frac{ϵ_o^{\beta 2}}{q(\beta 1)}\frac{\sigma _T/3}{m_ec^2}\frac{1}{(4\mathrm{\Gamma }_\pm )^{\beta 1}}\mathrm{\Delta }t1,$$
(7)
where the effective duration is as before. The maximum Lorentz factor for pair formation is then

$$\mathrm{\Gamma }_\pm (r)\{\begin{array}{cc}\left(\frac{2^{32\beta }}{3(\beta 1)}\right)^{1/(\beta +1)}\left(\frac{ϵ_o}{q}\right)^{(\beta 2)/(\beta +1)}(r_{}/r)^{1/(\beta +1)},\hfill & \text{for }\mathrm{\Delta }t(r/2c\mathrm{\Gamma }^2)\text{;}\hfill \\ \left(\frac{4^{2\beta }}{3(\beta 1)}\right)^{1/(\beta 1)}\left(\frac{ϵ_o}{q}\right)^{(\beta 2)/(\beta 1)}\left(\frac{ct_w}{r_{}}\right)^{1/(\beta 1)}(r_{}/r)^{2/(\beta 1)},\hfill & \text{for }\mathrm{\Delta }tt_w\hfill \end{array}.$$
(8)
This yields a critical radius and Lorentz factor for the transition between the impulsive and wind dominated regimes of

$`r_c=`$ $`\left({\displaystyle \frac{2^{73\beta }}{9(\beta 1)^2}}\right)^{\frac{1}{\beta +3}}\left({\displaystyle \frac{ϵ_o}{q}}\right)^{\frac{2\beta 4}{\beta +3}}r_{}\left({\displaystyle \frac{ct_w}{r_{}}}\right)^{\frac{\beta +1}{\beta +3}}5\times 10^{14}L_{w50}^{2/5}t_{w1}^{3/5},`$
$`\mathrm{\Gamma }_c=`$ $`\left({\displaystyle \frac{2^{2(\beta 1)}}{3(\beta 1)}}\right)^{\frac{1}{\beta +3}}\left({\displaystyle \frac{ϵ_o}{q}}\right)^{\frac{\beta 2}{\beta +3}}\left({\displaystyle \frac{r_{}}{ct_w}}\right)^{\frac{1}{\beta +3}}3\times 10^1L_{w50}^{1/5}t_{w1}^{1/5},`$ (9)
where the numerical values in the second equation of both lines are calculated for $`\beta =2`$, $`ϵ_oq1`$, $`L=10^{50}L_{w50}`$ erg s<sup>-1</sup> and $`t_w=10t_{w1}`$ s. (At early times $`t<t_w`$ the radius $`r_c`$ is smaller, $`t^{3/5}`$, since it takes $`t_w`$ for the entire photon energy to build up). The maximum pair Lorentz factor is shown in Figure 1 for nominal parameter values. The pair formation limit (9) is somewhat more restrictive than the scattering limit (6). Also, unlike the scattering limit, the pair formation limit depends exponentially on the photon number slope $`\beta `$. However, for the canonical value $`\beta =2`$ the two power law dependences are the same and the numerical values are close to each other. In what follows we shall use the pair formation limit of equations (8) and (9).

## 3 Pair-precursor and Kinematics

Given a certain external baryon density $`n_p`$ at a radius $`r`$ outside the shocks producing the GRB primordial spectrum, the initial Thomson scattering optical depth is $`\tau _in_p\sigma _Tr`$ and a fraction $`\tau _i`$ of the primordial photons will be scattered back, initiating a pair cascade. Since the photon flux drops as $`r^2`$, for a uniform (or decreasing) external ion density most of the scattering occurs between $`r`$ and $`r/2`$, and the scattering and pair formation may be approximated as a local phenomenon. This pair-dominated plasma, as long as its density $`n_\pm \text{ }<n_p(m_p/2m_e)`$, is initially held back by the inertia of its constituent ions component, provided that the pairs remain coupled to the baryons. (The latter is likely to be the case in the presence of even weak magnetic fields, e.g. Madau & Thompson 2000, or plasma wave scattering, e.g. Lightman, 1982. Moreover, the initial magnetic field strength can also increase as consequence of instabilities caused by an initial pair streaming relative to ions. In what follows, we assume that this coupling is effective).

The pairs (together with the ions) start acquiring a significant velocity $`\mathrm{\Gamma }_\pm \text{ }>1`$ only after their density $`n_\pm \text{ }>n_p(m_p/2m_e)`$, when the effective mass per scatterer $`\mu m_em_e`$. After the pairs start being accelerated, the pair cascade can continue multiplying as long as the compactness parameter of equation (8) is $`\mathrm{}\text{ }>1`$. Both the compactness $`\mathrm{}`$ and the maximum $`\mathrm{\Gamma }_\pm `$ decrease for increasing radius according to equations (7) and (8), and the cascade process shuts off for $`\mathrm{}\text{ }<1`$ at a radius where the maximum $`\mathrm{\Gamma }_\pm 1`$,

$$r_{\mathrm{}}(4r_{}ct_w/3)^{1/2}4\times 10^{15}L_{w50}^{1/2}t_{w1}^{1/2}\text{cm}.$$
(10)
On the other hand, the blast wave producing the shock(s) responsible for the afterglow spectrum starts decelerating (i.e. its initial Lorentz factor $`\mathrm{\Gamma }_f\eta =10^2\eta _2`$ starts to decrease as a negative power law in radius) at the deceleration radius

$$r_d(3Lt_w/4\pi n_pm_pc^2\eta ^2)^{1/3}3\times 10^{15}L_{w50}^{1/3}t_{w1}^{1/3}\eta _2^{2/3}n_3^{1/3}\text{cm},$$
(11)
where we normalized to an external baryon density $`n_p=10^3n_3\mathrm{cm}^3`$. (This expression is valid provided that the deceleration radius exceeds $`ct_w\eta ^2`$. Otherwise the deceleration starts before the outflow is over, and $`t_w`$ should be replaced by $`t`$ in the expression). A larger value $`n_p10^3n_3\mathrm{cm}^3`$ would give $`r_d\text{ }<r_{\mathrm{}}`$. (Such a higher density would, e.g., be required for pair effects to be important in an external shock model, where the $`\gamma `$-rays arise at $`r_d`$). In an internal shock model the primary $`\gamma `$-rays themselves arise at a smaller radius

$$r_ict_v\eta ^23\times 10^{13}t_{v1}\eta _2^2\text{cm}$$
(12)
where $`t_v=10^1t_{v1}\text{ }>10^3`$ s is the variability timescale in the outflow. The criterion for an $`\text{e}^\pm `$ cascade to form ahead of the fireball producing a primary spectrum (1) is that $`r_i`$ (or $`r_d`$ for an external shock model) is smaller than $`r_{\mathrm{}}`$. Pair formation occurs then for $`rr_{\mathrm{}}`$.

The minimum number of pairs is formed just inside $`r_{\mathrm{}}`$, where they are created essentially at rest, and their density can reach $`n_\pm (m_p/2m_e)n_p10^3n_p`$, at which point the mass per scatterer has become comparable to the electron mass. This represents an increase in the electron (or positron) scattering opacity by a multiplication factor of $`k_p2\times 10^3`$. As the density exceeds this value at $`r_{\mathrm{}}`$ the pairs are pushed by scattering beyond $`r_{\mathrm{}}`$, where the condition $`\mathrm{}<1`$ prevents further multiplication.

For radii $`r<r_{\mathrm{}}`$, and as long as the blast wave has not reached that radius, pair formation exceeding the above value $`n_\pm 10^3n_p`$ can continue to occur, with the pairs being accelerated by scattering until they reach the maximum Lorentz factor (8). Pair production will be most copious at smaller radii $`r_i<r<r_c`$, where the pairs are accelerated to a maximum Lorentz factor $`\mathrm{\Gamma }_\pm (r)\text{ }<\mathrm{\Gamma }_c(r/r_c)^{1/3}`$. At each step of the cascade the Lorentz factor of the new generation of pairs approximately doubles, and the maximum pair multiplication factor of the cascade can be estimated from the number $`s`$ of pair generations required to go from $`\mathrm{\Gamma }1`$ to $`\mathrm{\Gamma }_\pm (r)`$ given by equation (8). At $`r_c`$ this is $`s(r_c)\mathrm{log}\mathrm{\Gamma }_c/\mathrm{log}25`$, and for $`r_i\text{ }<r`$ it is limited to $`s(r_i)\text{ }<7.5`$. This represents an extra multiplication factor $`k_a2^s\mathrm{\Gamma }_c(r/r_c)^{1/3}30170`$ in the electron opacity for $`r_irr_c`$, in addition to the previous factor $`k_p2\times 10^3`$ achieved before acceleration starts. The critical value is

$$k_c=k_pk_a(r_c)(m_p/m_e)\mathrm{\Gamma }_c5\times 10^4L_{w50}^{1/5}t_{w1}^{1/5},$$
(13)
with $`k(r)=k_c(r/r_c)^{1/3}`$ for $`r_ir_c`$, while $`k(r)k_c(r/r_c)^2`$ for $`r_crr_{\mathrm{}}`$ drops to $`m_p/m_e`$ at $`r_{\mathrm{}}`$, and to zero beyond that. In a more detailed calculation, the number of cascades depends somewhat on the radiation spectral index $`\beta `$, here set equal to 2. For a steeper spectrum, the number of cascades is reduced ( e.g. Ramirez-Ruiz et al. 2000). The maximum pair optical depth is achieved at $`r_c`$,

$$\tau _{\pm c}k_cn_p\sigma _Tr_c=\mathrm{min}[2\times 10^5n_pL_{w50}^{3/5}t_{w1}^{2/5},1].$$
(14)
The pair opacity scales as $`\tau _\pm r^{2/3}`$ for $`r_i\text{ }<r\text{ }<r_c`$ and $`\tau _\pm r^1`$ for $`r_c\text{ }<r\text{ }<r_{\mathrm{}}`$. For an external density greater than

$$n_{p,c}10^5L_{w50}^{3/5}t_{w1}^{2/5}\mathrm{cm}^3,$$
(15)
the pair density inside $`r_c`$ is prevented from multiplying beyond a value corresponding to $`\tau _\pm 1`$, due to self-shielding. The number of pairs created at $`r_c`$ is

$$N_{\pm c}n_pk_c(4\pi /3)r_c^33\times 10^{49}n_pL_{w50}^{7/5}t_{w1}^{8/5},$$
(16)
which scales as $`N_\pm r^{8/3},r`$ for $`r`$ below or above $`r_c`$. The maximum value for $`n_p=n_{p,c}`$ is $`N_{\pm ,c,mx}3\times 10^{54}L_{w50}^{4/5}t_{w1}^{6/5}`$ at $`r=r_c`$, and $`N_{\pm ,\mathrm{},mx}3\times 10^{55}L_{w50}^{9/10}t_{w1}^{11/10}`$ at $`r_{\mathrm{}}`$. The pair cloud extends over a range of radii comparable to $`r`$, much larger than the photon pulse radial width $`ct_w`$.

Figure 2 shows the schematic world-lines of three blast waves expanding into an external medium. At each radius $`r_i<r<r_{\mathrm{}}`$ pairs form ahead of $`r_i`$. While for $`rr_{\mathrm{}}`$ the pairs are sub-relativistic and do not propagate significantly, for smaller radii they move relativistically with an initial speed $`\mathrm{\Gamma }_\pm `$, with $`\mathrm{\Gamma }_\pm <\eta `$ in general, although at very small radii, and for times $`t<t_w`$, $`\mathrm{\Gamma }_\pm >\eta `$ may be possible. If the blast wave did not exist, then the pair-enriched material (moving out with a Lorentz factor that is larger at smaller r) would pile up at a radius $`r_l`$ after a time $`r_l/c`$. However, the pair-rich external medium would generally carry less energy and inertia than the relativistic wind itself; it therefore starts being decelerated by the external medium at a smaller radius than a blast wave with the same Lorentz factor would be, so that the latter always overtakes it and sweeps up the pair-enriched external medium. The resultant outer shock is more likely to be radiative, but may be weaker, because the ambient material might already be moving outward relativistically before the blast wave hits it.

For a relatively low external density such as $`n_p=10^3\mathrm{cm}^3`$, as in curve (a) of Figure 2, the radius $`r_c<r_d`$, and the pairs are swept up by a fireball expanding at its original speed $`\eta `$ constant, and deceleration of the fireball begins sometime after the pairs have been swept up. In this case the main afterglow, produced by the deceleration of the pair-enriched fireball will be characterized by a larger emission measure than in the usual case, due to the extra pairs in the swept-up matter, but will not otherwise exhibit any irregularities in its time development. For a larger external density such as $`10^6\mathrm{cm}^3`$, corresponding to curve (b) of Figure 2, the radius $`r_cr_d`$ and the main part of the afterglow, caused by the deceleration of the fireball baryons and the pairs formed at early stages, continues to sweep up further pairs which were formed at or beyond the deceleration radius (in curve (c), with low $`\eta `$, deceleration occurs at radii $`r>r_{\mathrm{}}`$). These new pairs change the emission measure of the deceleration shock, since their optical depth $`\tau _\pm 1`$ is larger than that of the swept up baryonic electrons. If $`\tau _\pm 1`$ is reached, the original spectrum may be modified by Comptonization, and may approach a quasi-thermal shape. We note that the optical depth cannot substantially exceed unity. This is because high-energy non-thermal photons would be comptonised by pairs , and after a few scatterings would be degraded below the pair-production threshold. So, however intense the radiation incident on its inner edge, a shell of pair-dominated plasma cannot build up an opacity much larger than unity. It will come to a quasi-steady state in which the luminosity from its outer surface (comptonised synchrotron radiation and annihilation radiation) equals the non-thermal radiation shining on its inner surface.

## 4 Observable Pair-precursor Effects

The energy in the accelerated pairs is $`E_\pm N_\pm \mathrm{\Gamma }_\pm r^3r^{7/3}`$ for $`r\text{ }<r_c`$ and $`E_\pm r^1`$ for $`r_c\text{ }<r\text{ }<r_{\mathrm{}}`$. The maximum number of pairs created is

$$E_{\pm c}N_\pm m_ec^2\mathrm{\Gamma }_c=\mathrm{min}[10^{45}n_pL_{w50}t_{w1},10^{50}L_{w50}^{2/5}t_{w1}^{3/5}]\mathrm{erg},$$
(17)
where the second number is the limit $`N_{\pm ,mx}`$ obtained for $`n_p=n_{pc}`$, at which the saturation value of $`\tau _\pm 1`$ is obtained. The pair energy never exceeds more than a fraction of the initial wind energy, so the deceleration radius (equation ) is unaffected, while the pairs which are produced and accelerated ahead of the blast wave, are decelerated at a (smaller) radius

$$r_{d\pm }2.5\times 10^{15}E_{\pm 50}^{1/3}n_3^{1/3}(\mathrm{\Gamma }_\pm /30)^{2/3}\mathrm{cm},$$
(18)
before the ejecta itself starts to decelerate.

The total number of protons in the ejecta wind is $`N_p=E/\eta m_pc^2=(2/3)\times 10^{52}L_{w50}t_{w1}\eta _2^1`$. The number of protons in the (pair enriched) external medium which are swept up by the time the blast wave reaches its deceleration radius $`r_d`$ is $`N_{ps}=N_p\eta ^1=(2/3)\times 10^{50}L_{w50}t_{w1}\eta _2^2`$. The maximum number of swept-up pairs can exceed the number of baryons by a large factor. However the inertia of the pairs is less than that of the baryonic ejecta, since $`(N_{\pm ,c,mx}/N_p)5\times 10^2L_{w50}^{1/5}t_{w1}^{1/5}\eta _2\text{ }<(m_p/m_e)(\eta /\mathrm{\Gamma }_c)=6\times 10^3L_{w50}^{1/5}t_{w1}^{1/5}\eta _2`$ at $`r_c`$, and $`(N_{\pm ,\mathrm{},mx}/N_p)5\times 10^3L_{w50}^{1/10}t_{w1}^{1/10}\eta _2(m_p/m_e)\eta =2\times 10^5\eta _2`$ at $`r_{\mathrm{}}`$.

The pairs will modify the usual properties of the deceleration shocks and the afterglow emission. The total energy available in the afterglow is not changed: it is still, essentially, the kinetic energy of the relativistic wind, minus the fraction dissipated (and converted into prompt gamma rays) in internal shocks. But the lepton/proton ratio in the ejecta can be much larger than usual. This increases the radiative efficiency significantly, since most of the particles are $`\text{e}^\pm `$. The resultant radiation will thus be softer than in the usual picture, because the same energy density has to be shared among a larger number of particles ($`N_\pm /N_p1`$). In the reverse shock that occurs after the baryonic+pair ejecta starts being decelerated by the external medium, the comoving frame peak random electron Lorentz factor is $`\gamma _{\pm ,m,r}(E\eta ^1/N_\pm m_ec^2)`$. Even for $`\tau _\pm `$ substantially less than unity, e.g. for an external density $`n=10^3n_3\mathrm{cm}^3`$ (below the critical value $`n_{p,c}`$) for which the deceleration radius $`r_dr_c`$, the reverse shock random lepton Lorentz factor is $`\gamma _{\pm ,m,r}30E_{w51}^{1/5}t_{w1}^{3/5}n_3^1\eta _2^1`$. The pairs should not affect, however, the random turbulent magnetic field strength, which is in pressure equilibrium with the forward shock at some fraction $`ϵ_B`$ of the equipartition value, $`B^{}(ϵ_B8\pi nm_pc^2)^{1/2}\eta 6\times ϵ_B^{1/2}n_3^{1/2}\eta _2`$ G. Thus the observed reverse synchrotron peak frequency

$$\nu _{\pm ,sy,r}10^6B^{}\gamma ^2\eta (1+z)^16\times 10^{13}E_{w51}^{2/5}t_{w1}^{6/5}ϵ_B^{1/2}n_3^{3/2}\eta _2^1(1+z)^1\mathrm{Hz}$$
(19)
would be in the far IR, as opposed to the optical/UV of the usual baryon-dominated prompt reverse flash.

The forward shock afterglow radiation, normally in the $`\gamma `$/X-ray range, would be unaffected outside $`r_{\mathrm{}}`$. However, up to about the time when deceleration starts, there will be a “pair pick-up” photon pulse, when the protons and electrons of the relativistic wind moving with $`\eta >\mathrm{\Gamma }_c`$ sweep up the pair-enriched external medium. The protons are not decelerated by the pairs, so there is only a subsonic reverse compression wave in the proton ejecta, but there will be a mildly relativistic forward shock in the picked-up pairs. The $`\text{e}^\pm `$ random Lorentz factor will be equal to the bulk kinetic energy it has in the proton frame, e.g. $`\gamma _{\pm ,m,f}\eta /\mathrm{\Gamma }_\pm 3L_{w50}^{1/5}t_{w1}^{1/5}\eta _2`$ near $`r_c`$. The comoving random magnetic field in the shocked pair fluid is $`B^{}(8\pi ϵ_BN_{\pm ,c}m_ec^2/4r_c^3)^{1/2}(\eta /\mathrm{\Gamma }_\pm )`$ $`20ϵ_B^{1/2}L_{w50}^{1/5}t_{w1}^{1/10}n_3^{1/2}\eta _2`$ G for $`n_p=10^3n_3\mathrm{cm}^3`$, corresponding to a pair-pickup pulse synchrotron peak frequency in the observer frame of

$$\nu _{\pm ,sy,f}2\times 10^{10}ϵ_B^{1/2}L_{w50}^{1/5}t_{w1}^{5/10}n_3^{1/2}\eta _2^3(1+z)^1\mathrm{Hz},$$
(20)
and a synchrotron power law above this frequency.

There could also be additional pair-precursor signatures which are not associated with the ejecta blast wave, but with the dynamics of the pre-accelerated pair-enriched plasma. The r-dependent $`\mathrm{\Gamma }_\pm `$ of the pair-enriched external plasma will lead to internal shocks. Pair regions at $`r<r_c`$ whose $`\mathrm{\Gamma }_\pm `$ differ by order unity will collide at radii $`r\mathrm{\Gamma }_\pm ^2r^{1/3}`$, so for sufficiently short variability times these shocks would occur between $`r_i`$ and $`r_c`$, i.e. up to an observer time $`t_cr_c/c\mathrm{\Gamma }_c^215t_{w1}`$ s, independent of the wind luminosity $`L`$. (For $`r_c<r<r_{\mathrm{}}`$ the collision radii are $`r^3`$, so the shocks would tend to pile up at $`r_{\mathrm{}}`$ at an observer timescale $`t_{\mathrm{}}r_{\mathrm{}}/c`$ 1 day, provided the main part of the fireball wind has not caught up with it before. This could be the case for a jet-like wind for pairs in a rim of angular width $`\mathrm{\Gamma }_c^1`$ around the jet). The pair internal shocks at $`rr_c`$ can produce a Fermi accelerated power law $`\text{e}^\pm `$ spectrum above $`\gamma _{\pm m}1`$ and a turbulent comoving field $`B_\pm ^{}\text{ }<2\times 10^2`$ G, leading to a synchrotron spectrum whose observer-frame peak frequency $`\nu _{\pm m}6\times 10^9`$ Hz would be self-absorbed, with a power law extension above it which would be optically thin at higher frequencies.

The above observational signatures would be present even if $`\tau _\pm `$ is low, as expected for external ion densities $`n_p\text{ }<n_{p,c}10^5L_{w50}^{3/5}t_{w1}^{2/5}\mathrm{cm}^3`$ around the burst. An additional effect of interest, for external densities in excess of this which lead to a pair screen of optical depth $`\tau _\pm 1`$, is that a quasi-thermal pulse of X-rays could accompany the burst, caused by upscattering of diffuse progenitor stellar photons. A collapsing massive progenitor leading to a GRB is likely to be highly super-Eddington for sometime after the GRB event, e.g. $`L_{}10^4L_{Ed}10^{43}L_{43}`$ erg/s. The density of photons of energy $`ϵ_{}10`$ eV near $`r_c`$, which would be quasi-isotropized due to the condition $`\tau _\pm 1`$ at $`r_c`$ (and beyond, where $`\mathrm{\Gamma }_\pm 1`$ at $`r_{\mathrm{}}`$), would be $`n_{}10^{13}L_{43}ϵ_{10}^1L_{w50}^{4/5}t_{w1}^{6/5}\mathrm{cm}^3`$ near $`r_c`$. The screen with $`\tau _\pm 1`$ moving with $`\mathrm{\Gamma }_c30`$ sweeps up a total number of photons $`N_{}3\times 10^{57}L_{43}ϵ_{10}^1L_{w50}^{2/5}t_{w1}^{3/5}`$. The mean energy per photon and the time-integrated total energy of the upscattered precursor is

$`ϵ_X`$ $`10ϵ_{10}L_{w50}^{2/5}t_{w1}^{2/5}(1+z)^1\mathrm{keV}`$
$`E_X`$ $`5\times 10^{49}L_{43}ϵ_{10}^1L_{w50}^{4/5}t_{w1}^{1/5}(1+z)^1\mathrm{erg}.`$ (21)
This would last until the pairs are swept up by the ejecta, $`t_X\text{ }<t_cr_c/c\mathrm{\Gamma }_c^215t_{w1}`$ s.

## 5 Discussion

We have discussed, in the context of a standard internal/external shock model of gamma-ray bursts (which are normally assumed to occur after the original fireball has become optically thin) the $`\gamma \gamma \text{e}^\pm `$ cascades triggered by the back-scattering of seed gamma-ray photons on the external medium. This effect can modify the initial scattering optical depth of the outflow at radii $`r\text{ }<r_{\mathrm{}}4\times 10^{15}L_{w50}^{1/2}t_{w1}^{1/2}\text{cm}`$ (equation ), which is comparable to the radii of external shocks of equation (11) at which the afterglow begins, and is generally larger than the typical internal shock radii given by equation (12). The spectral effects of the pairs on the burst and the afterglow can be substantial, and within radii $`r_l`$ they can affect the dynamics.

Pair production can increase the optical depth outside of the shocks by up to $`\text{ }<10^5`$; self-shielding ensures that the maximum scattering optical depths achievable by the pairs is $`\tau _\pm 1`$. For typical interstellar densities the pair opacity $`\tau _\pm 1`$, which does not significantly affect the gamma-ray spectrum. The number of pairs may nonetheless be large enough to increase the radiative efficiency and soften significantly the radiation spectrum of the afterglow reverse shock, where the same energy is shared among a number of $`\text{e}^\pm `$ which can exceed that of the original $`e^{}`$ and $`p^+`$ of the ejecta.

The pair production processes themselves (determining $`r_c,r_l`$, equations , ) just depend on the “seed” $`\gamma `$-ray photon flux (which are here postulated to come from internal shocks). The manifestations depend on the external density and on the initial dimensionless entropy or bulk Lorentz factor $`\eta `$. The external baryon density $`n_{ext}`$ determines the optical depth that can be built up through back-scattering and pair multiplication. This affects whether the pair optical depth gets up to unity, with smearing and reprocessing of the primordial $`\gamma `$-ray spectrum, or whether it merely makes the blast wave more radiative. Madau and Thompson (2000) have made this point, in the context of a specific fireball model.

The external density (along with the initial Lorentz factor $`\eta `$) determines when the outer shock and the reverse shock become important and whether this happens within the radius already polluted with pairs (and pre-accelerated by radiation pressure before the shock hits). There are two rather different cases depending on whether or not $`\eta ^2`$ is less than $`r_l/ct_w`$). In the former case the external shock responsible for the afterglow occurs beyond the region “polluted” by new pairs, while in the second case the afterglow shock may experience, after starting out in the canonical manner, a “resurgence” or second kick as its radiative efficiency is boosted by running into an $`\text{e}^\pm `$-enriched gas. Internal shocks in the pair-dominated external plasma can lead to self-absorbed radiation at $`10^910^{10}`$ Hz, while the swept-up pairs can also contribute a $`10^{11}10^{12}`$ Hz ‘prompt’ signal, which precedes the onset of the standard deceleration afterglow phase.

Additional effects are expected when $`\tau _\pm 1`$. This requires external baryon densities at radii $`r<r_{\mathrm{}}`$ of $`n_p\text{ }>n_{c,p}10^5L_{w50}^{2/5}t_{w1}^{3/5}\mathrm{cm}^3`$. Such high densities would only be expected if the burst is associated with a massive star in which prior mass loss led to a dense circumstellar envelope The pair optical depth saturates to $`\tau _\pm 1`$ and in addition to an increased efficiency and softer spectrum of the afterglow reverse shock, the original gamma-ray spectrum of the GRB will be modified as well. The specific nature of this spectral modification depends on the value of the luminosity, which influences (equation ) the bulk Lorentz factor of the reprocessing pair cloud before it has been swept up by the ejecta, and also on the extent to which the outflow is beamed. One of the consequences of such a critical external density leading to $`\tau _\pm 1`$ would be the presence of an X-ray quasi-thermal pulse, whose total energy may be a few percent of the total burst energy. In the case of even more extreme densities, there are other interesting possibilities. For instance, dense blobs of Fe-enriched thermal plasma would emit strong recombination features, as well as annihilation radiation features, if the normal electron density were augmented by extra pairs.

Even in isotropic situations, the spectrum would be modified by transmission through a pair plasma of optical depth unity. The effect is maximal for photons of energy $`m_ec^2`$ in the frame of the pair plasma: for higher energies, the Klein-Nishina cross-section is smaller; for lower energies, the scatterings are almost elastic. If, for instance, $`\mathrm{\Gamma }_c40`$, the gamma-ray spectrum around photon energies $`ϵ\mathrm{\Gamma }_cm_ec^220`$ MeV would be depressed by a factor $`1`$ relative to its original value, smoothly rejoining its original value above and below that energy. For a beamed primary output, however, there would be a suppression at lower energies (where the scattering is in the Thompson regime) because the scattered photons would be spread over a wider angle. Pair-induced processes would therefore yield evidence on the beaming properties of the bursts.

Irrespective of the external density, the processes discussed here suggest that bursts and afterglows may have a more complex spectrum and time-structure than ’standard’ models suggest. But the effects are especially interesting when the external density is high: they probe the environment of GRBs, and thus can offer clues to the nature of the progenitor stars, and their location within the host galaxy. For instance, a quasi-thermal X-ray pulse accompanying the gamma-ray emission could be indicative of an external circum-burst density of at least $`10^410^5\mathrm{cm}^3`$. While quasi-thermal X-ray pulses might also arise due to other reasons, e.g. from an underlying optically thick central engine, if the X-ray luminosity scales as equation (21) and is accompanied by radio or far-IR signals such as in equations (19)(20), this could be indicative of birth in a dense environment from a massive progenitor.

Detailed Monte Carlo simulations (Ramirez-Ruiz et al., 2001) should provide a more detailed assessment of the self-consistent spectrum of a GRB in the presence of self-induced pair formation.

This research has been supported by NASA NAG5-9192, the Guggenheim Foundation, the Sackler Foundation, NSF PHY94-07194 and the Royal Society. We are grateful to R. D. Blandford, C. Dermer, P. Madau, C. Thompson and the referee for useful comments.


text:
# 1 Introduction

## 1 Introduction

Single-$`W`$ production processes present an opportunity to study the anomalous triple gauge-couplings(TGC) in the experiments at LEP2 and at future $`e^+e^{}`$ linear colliders. For their precise predictions of cross sections the inclusion of an initial state radiative correction(ISR) is inevitable in the event-generator. As a tool for the ISR the structure function(SF) and the parton shower methods has been widely used for $`e^+e^{}`$ annihilation processes. For the case of the single-$`W`$ production processes, however, the main contribution comes from non-annihilation type diagrams. The universal factorization method used for the annihilation processes is obviously inappropriate. The main problem lies in choosing the energy scale of the factorization. A previous study on the two photon process has shown that the SF and QED parton shower(QEDPS) methods are able to reproduce precisely the exact $`O(\alpha )`$ results even for non-annihilation processes, as long as the appropriate energy scale is used.

In this report a general method to find the energy scale for SF and QEDPS is proposed. Then numerical results of testing SF and QEDPS for $`e^{}e^+e^{}\overline{\nu }_eu\overline{d}`$ and $`e^{}e^+e^{}\overline{\nu }_e\mu ^+\nu _\mu `$ are presented. Systematic errors are also discussed.

## 2 Calculation method

### 2.1 Energy Scale Determination

The factorization theorem for QED radiative corrections in the leading-logarithmic approximation is valid independent of the structure of the matrix element of the kernel process. Hence SF and QEDPS must be applicable to any $`e^+e^{}`$ scattering processes. However, choice of the energy scale in SF and QEDPS is not a trivial matter. For simple processes considered so far like $`e^+e^{}`$ annihilation and two-photon process with only multi-peripheral diagrams, the evolution energy scale could be found by the exact perturbative calculations. However, this is not always the case when more complicated processes are concerned. Hence a way to find a suitable energy scale without knowing exact loop calculations should be established somehow.

First let us look at the general consequence of the soft photon approximation. The cross section with radiations in the soft-photon limit is given by the Born cross section multiplied by the following factor up to the double-log term as

$`{\displaystyle \frac{d\sigma _{soft}(s)}{d\mathrm{\Omega }}}`$ $`=`$ $`{\displaystyle \frac{d\sigma _0(s)}{d\mathrm{\Omega }}}`$ (1)
$`\times `$ $`\left|\mathrm{exp}\left[{\displaystyle \frac{\alpha }{\pi }}\mathrm{ln}\left({\displaystyle \frac{E}{k_c}}\right){\displaystyle \underset{i,j}{}}{\displaystyle \frac{e_ie_j\eta _i\eta _j}{\beta _{ij}}}\mathrm{ln}\left({\displaystyle \frac{1+\beta _{ij}}{1\beta _{ij}}}\right)\right]\right|^2,`$
$`\beta _{ij}`$ $`=`$ $`\left(1{\displaystyle \frac{m_i^2m_j^2}{(p_ip_j)^2}}\right)^{\frac{1}{2}},`$ (2)
where $`m_j`$($`p_j`$) are the mass(momentum) of the $`j`$-th charged particle, $`k_c`$ the maximum energy of the soft photon(the value to separate soft- and hard-photons), $`E`$ the beam energy and $`e_j`$ the electric charge in unit of the $`e^+`$ charge. The factor $`\eta _j`$ is $`1`$ for the initial particles and $`+1`$ for the final particles. The indices ($`i,j`$) run over all the charged particles in the initial and final states.

For the two-photon process, $`e^{}(p_{})e^+(p_+)e^{}(q_{})e^+(q_+)\mu ^{}(k_{})\mu ^+(k_+)`$, it is shown in ref. that the soft-photon factor in Eq.(1) with a ($`p_{}q_{}`$)-term reproduces the $`O(\alpha )`$ corrections up to the double-log term in the soft-photon limit. This implies that one is able to read off the possible evolution energy scale in SF from Eq.(1) without doing explicit loop calculations.111 A similar idea is independently proposed by Montagna et al. in. The point is the observation that the energy scale $`s=(p_{}+p_+)^2`$ does not appear in the soft-photon corrections even they are included in the general formula Eq.(1). In the case of the two-photon process we have ignored those terms in SF which come from the photon bridged between different charged lines, because the contributions from the box diagrams with a photon exchange between $`e^+`$ and $`e^{}`$ is known to be small. Fortunately the infrared part of the loop corrections is already included in Eq.(1) and there is no need to know the full form of the loop diagram. Let us look at two terms with, for example ($`p_{}p_+`$)- and ($`q_{}p_+`$)-terms. The momentum of $`e^{}`$ is almost the same before and after the scattering($`p_{}q_{}`$). Only the difference appears in $`\eta _j\eta _k=+1`$ for a ($`p_{}p_+`$)-term and $`\eta _j\eta _k=1`$ for a ($`q_{}p_+`$)-term. Then these terms compensate each other after summing them up for the forward scattering which is the dominant kinematical region of this process. This is the mechanism that the energy scale $`s=(p_{}+p_+)^2`$ does not appear in the soft-photon correction despite that it exists in Eq.(1).

When some experimental cuts are imposed, for example the final $`e^{}`$ is tagged in a large angle, this cancellation is not perfect but partial and the energy scale $`s`$ must appear in the soft-photon correction. In this case the annihilation type diagrams will also give a contribution. Then it may happen that the usual SF and QEDPS for the annihilation processes are justified to be used for the ISR with the energy scale $`s`$. To find the most dominant energy scale under the given experimental cuts an easy way is to integrate numerically the soft-photon cross section given by Eq.(1) over the allowed kinematical region. Thus in order to determine the energy scale it is sufficient to know the infrared behavior of the radiative process using the soft-photon factor.

Let us determine the energy-scale of the QED radiative corrections to the single-$`W`$ production process,

$`e^{}(p_{})+e^+(p_+)`$ $``$ $`e^{}(q_{})+\overline{\nu }_e(q_\nu )+u(k_u)+\overline{d}(k_d).`$ (3)
The soft-photon correction factor in Eq.(1) is numerically integrated with the Born matrix element of the process (3) only with the $`t`$-channel diagrams without any cut on the final fermions. In order to separate the contribution from each term, we take terms up to $`O(\alpha )`$ in Taylor expansion of exponential function in Eq.(1). Parameters used in the calculation will be explained in section 4. The results are shown in Table 1. One can see that the main contribution comes from an electron charged-line ($`p_{}q_{}`$-term) and a positron charged-line ($`p_+k_uk_d`$-terms=$`p_+k_u`$-term + $`p_+k_d`$-term + $`k_uk_d`$-term), while all other contributions are negligiblly small. Like the two-photon processes the energy scale $`s`$ does not appear in the soft-photon correction.

The above results clearly indicate that one should apply SF or QEDPS to the electron and positron charged-lines individually with the energy scale of their momentum-transfer squared.

### 2.2 Structure Function Method

The analytic solution of the DGLAP evolution function in the leading-logarithmic order is known as the structure function. With SF the QED corrected cross section is given by

$`\sigma _{total}(s)`$ $`=`$ $`{\displaystyle 𝑑x_I𝑑x_F𝑑x_{I+}𝑑x_u𝑑x_dD_e^{}(x_I,t_{})D_e^{}(x_F,t_{})}`$ (4)
$`D_{e^+}(x_{I+},t_+)D_u(x_u,s_{ud})D_d(x_d,s_{ud})\sigma _0(\widehat{s}),`$
where $`\sigma _0`$ is the Born cross section and $`D`$’s are the SF. The energy scales $`t_{}=(p_{}q_{})^2`$, $`t_+=(p_+(k_u+k_d))^2`$ and $`s_{ud}=(k_u+k_d)^2`$ are chosen following the result of the last section. After(before) the photon radiation the initial(final) momenta $`p_\pm `$($`q_\pm `$) become $`\widehat{p}_\pm `$ ($`\widehat{q}_\pm `$)

$`\widehat{p}_{}`$ $`=`$ $`x_Ip_{},\widehat{q}_{}={\displaystyle \frac{1}{x_F}}q_{},\mathrm{}`$ (5)
respectively. Then the CM energy squared, $`s`$, is scaled as $`\widehat{s}=x_Ix_{I+}s`$.

### 2.3 Parton Shower Method

Instead of the analytic formula of SF a Monte Calro method based on the parton shower algorithm in QED can be used to solve DGLAP equation in the LL approximation. Its detailed algorithm of the QEDPS is found in ref. for the $`e^+e^{}`$ annihilation processes, in ref. for the Bhabha process, and in ref. for the two-photon process. The same energy scale as the SF method is used in QEDPS also. Significant difference between SF and QEDPS is that the QEDPS can treat the transverse momentum of the emitted photons correctly by imposing the exact kinematics at the $`ee\gamma `$ splitting. It does not affect the total cross sections so much when the final $`e^{}`$ has no cut. However, the finite recoiling of the final $`e^\pm `$ can result some effects on the tagged cross sections.

In return for the exact kinematics at the $`ee\gamma `$ splitting, $`e^\pm `$ are no more on-shell after a photon emission. On the other hand the matrix element of the hard scattering process must be calculated with on-shell external particles. A trick to map the off-shell four-momenta of the initial $`e^\pm `$ to those at on-shell is needed. The following method is used in the calculations.

1. $`\widehat{s}=(\widehat{p}_{}+\widehat{p}_+)^2`$ is calculated, where $`\widehat{p}_\pm `$ are the four-momenta of the initial $`e^\pm `$ after the photon emission by QEDPS. $`\widehat{s}`$ is positive even for the off-shell $`e^\pm `$.
2. New four-momenta of initial $`e^\pm `$ in their rest-frame, $`\stackrel{~}{p}_\pm `$, are defined as $`\stackrel{~}{p}_\pm ^2=m_e^2`$ (on-shell) and $`\widehat{s}=(\stackrel{~}{p}_{}+\stackrel{~}{p}_+)^2`$. All four-momenta of final particles are generated in the rest-frame of $`\stackrel{~}{p}_++\stackrel{~}{p}_{}`$.
3. All four-momenta are rotated and boosted to match the three-momenta of $`\stackrel{~}{p}_\pm `$ with those of $`\widehat{p}_\pm `$.

This method respects the direction of the final $`e^\pm `$ rather than the CM energy of the collision. The total energy does not conserve then because of the virtuarity of the initial $`e^\pm `$. The violation of the energy conservation is of the order of $`10^6`$ GeV or less, and the probability of the violation more than 1 MeV is $`10^4`$.

## 3 Numerical Calculations

### 3.1 Cross sections with no cut

Total and differential cross sections of semi-leptonic process $`e^{}e^+e^{}\overline{\nu }_eu\overline{d}`$ and leptonic one $`e^{}e^+e^{}\overline{\nu }_e\mu ^+\nu _\mu `$, are calculated with the radiative correction by SF or QEDPS. Feynman diagrams of the semi-leptonic process are shown in Fig.1. Fortran codes to calculate the amplitudes are automatically produced by $`\mathrm{𝙶𝚁𝙰𝙲𝙴}`$ system. All fermion-masses are kept finite in the calculations. Numerical integrations of the matrix element squared in the four-body phase space are done using $`\mathrm{𝙱𝙰𝚂𝙴𝚂}`$. For a test with no experimental cuts, only the $`t`$-channel diagrams(non-annihilation diagrams) are taken into account. Standard model parameters used in the calculations are summarized in Table2. The on-shell relation strict at the tree-level is employed to determine weak couplings. Some of electro-weak corrections could be taken into account through the $`G_\mu `$-scheme and running coupling constant. In this report, however, we do not include those effects because here we are interested in looking at the pure QED radiative corrections to the Born cross section.

It has been pointed out that a tiny violation of the gauge invariance caused by the inclusion of a finite $`W`$-boson width results a wrong cross section for single-$`W`$ production. To cure this problem the fermion-loop scheme has been proposed. It is reported in ref., however, that no significant difference is seen between the fermion-loop scheme and the fixed width scheme. Thus in this report the fixed width scheme, together with an appropriately modified current, described in  is employed.

For the total energy of the emitted photons both methods, SF and QEDPS, must give the same spectrum once the same energy scale is used. This is confirmed for the semi-leptonic process as shown in Fig.2 at the CM energy of 200 GeV. We choose the same energy-evolution scale as SF described by Eq.(4). Total cross sections as a function of the CM energies at LEP2 with no cuts are shown in Fig.3. The effect of the QED radiative corrections on the total cross sections are obtained to be 7 to 8% in the LEP2 energy region. If one used an inappropriate energy scale, say $`s`$, in SF, the ISR effect is overestimated about 4% as seen in Fig.3. The result of SF is consistent with the QEDPS around 0.2% if the proper energy scale is employed.

There is some ambiguity to choose the energy-evolution scale in the leading-log order. For example the transverse-momentum squared or the invariant-mass squared of $`u\overline{d}`$ (or $`\mu \overline{\nu }_\mu `$) systems could be a candidate of the energy scale. It is found that even these energy scales are chosen in QEDPS instead of $`(p_+(k_u+k_d))^2`$, the total cross sections change by only 0.6%, which must be allocated to the theoretical uncertainty.

The energy and angular distributions of the hard photon from QEDPS are compared with those obtained from the exact matrix elements. The cross sections of the radiative process $`e^{}e^+e^{}\overline{\nu }_eu\overline{d}\gamma `$ are calculated based on the exact amplitudes generated by $`\mathrm{𝙶𝚁𝙰𝙲𝙴}`$ and integrated numerically in five-body phase space using $`\mathrm{𝙱𝙰𝚂𝙴𝚂}`$. Again only the $`t`$-channel diagrams(non-annihilation diagrams) are taken into account. To compare the distributions the soft-photon corrections for the radiative process must be included. For this purpose QEDPS is implemented into the $`e^{}\overline{\nu }_eu\overline{d}\gamma `$ calculations with a careful treatment to avoid a double-counting of the radiation effect. The definition of the hard photon is

1. $`E_\gamma >1`$ GeV,
2. opening angle between the photon and the nearest final-state charged particles is greater than $`5^{}`$.

The distributions of the hard photons are in good agreement as seen in Fig.4. The total cross section of the hard photon emission agrees each other in 2% level. We also calculated the radiative cross-section without soft-photon correction. If the soft-photon correction is not included in the radiative process, we find a 30% overestimation of the radiative cross-section with above experimental cuts.

### 3.2 Cross sections with experimental cut

It is also investigated how large the effects of the QED radiative corrections is for the single-$`W`$ production when realistic experimental conditions are imposed. The experimental cuts applied here are $`\theta _e^{}<5^{}`$, $`M_{q\overline{q}}>45\text{GeV}`$, $`E_\mu >20\text{GeV}`$. For this study all the diagrams, not only the $`t`$-channel diagrams but also the $`s`$-channel, are taken into account in the calculations. The dominance of the signal from $`t`$-channel diagrams is 97%(90%) for the hadronic(leptonic) decay of the $`W`$ boson, respectively. Total cross sections as a function of the CM energies at LEP2 with these cuts are shown in Fig.5. The QED radiative corrections on the total cross sections are found to be 7 to 8% in this LEP2 energy range. If one uses the inappropriate energy scale $`s`$ in SF, the ISR effect is overestimated by around 5%, which is larger than those of the no-cut case. SF with the proper energy scale shows a deviation from QEDPS around 0.5% for $`e^{}\overline{\nu }_eu\overline{d}`$ process and 1.0% for $`e^{}\overline{\nu }_e\mu ^+\nu _\mu `$. The agreement between QEDPS and SF becomes worse than the no-cut case, because the finite transverse-momentum of the emitted photons by QEDPS changes the acceptance of the above electron-veto requirement. Hence for the realistic experimental conditions the finite transverse-momentum of emitted photons should not be ignored.

Finally a possible effect of the systematic error of the ISR effect on the anomalous TGC measurements is investigated. If the inappropriate energy scale is used in the ISR tools such as the CM-energy squared, the total cross sections with the experimental cuts includes 5% systematic error. Even if one used one of proper energy scales, there is 0.6% uncertainty on the cross sections due to ambiguity of the energy scale selection. These uncertainty of the total cross sections limits the experimental sensitivity of the anomalous TGC measurements. Total cross-sections of $`e\nu _eud`$ and $`e\nu _e\mu \nu _\nu `$ processes with experimental cuts as a function of the anomalous TGC is summarized in Fig.6. The cross sections are obtained at the CM-energy of 200 GeV with all diagrams. A bound shown in dashed lines shows $`\pm 5`$% cross section variation from its standard model value. If one used the inappropriate energy scale, it affects $`\pm 0.05`$ on $`\mathrm{\Delta }\kappa `$ measurement and $`\pm 0.4`$ on $`\lambda `$ measurement. The ambiguity of the energy-scale selection gives the systematic error of less than 0.01 on $`\mathrm{\Delta }\kappa `$ and 0.1 on $`\lambda `$.

## 4 Conclusions

The method to apply the QED radiative correction to the non-annihilation process was established. The conventional method, SF with the energy scale $`s`$ gave about 4% overestimation in the LEP2 energies. The uncertainty due to the energy-scale determination was estimated to be about 0.6%. This uncertainty may affect the anomalous TGC measurements less than 0.01 on $`\mathrm{\Delta }\kappa `$ and 0.1 on $`\lambda `$. If one wants to look at the hard photon spectrum, the soft-photon correction to these radiative processes are needed.

In this report we have treated two processes $`e^{}e^+e^{}\overline{\nu }_eu\overline{d}`$ and $`e^{}e^+e^{}\overline{\nu }_e\mu ^+\nu _\mu `$. The CP conjugate processes $`e^{}e^+e^+\nu _e\overline{u}d`$ and $`e^{}e^+e^+\nu _e\mu ^{}\overline{\nu }_\mu `$ give the same results and the other channels $`e^{}e^+e\nu _ecs`$ and $`e^{}e^+e\nu _e\tau \nu _\tau `$ will show slightly different results due to their masses. On the other hand the self CP-conjugate process $`e^{}e^+e^{}\overline{\nu }_ee^+\nu _e`$ has an additional complexity, because two energy scales $`t_{}=(p_e^{}q_e^{})^2`$ and $`\stackrel{~}{t}_{}=(p_e^{}q_e^{}q_{\overline{\nu }_e})^2`$ can appear simultaneously.

Authors would like to thank members of the four-fermion working group of the LEP2 Monte Calro Workshop at CERN, in particular A. Ballesterero, G. Montagna, F. Piccinini, G. Passarino for useful discussions.

This work was supported in part by the Ministry of Education, Science and Culture under the Grant-in-Aid No. 11206203 and 11440083.


text:
# Do As antisites destroy the ferromagnetism of (Ga,Mn)As?

## Abstract

The effect of the inclusion of As antisites in the diluted magnetic semiconductor (Ga,Mn)As is studied within density functional theory in the local spin density approximation. In the case of homogeneous distribution of Mn ions we find that the ferromagnetism is largely weakened by the presence of the antisites. This is due to compensation of the free holes which mediate the long range ferromagnetic order. In contrast, when two Mn ions are coupled through only one As ion, ferromagnetic and antiferromagnetic order compete. In this case the magnetic ground state depends on: i) the position of the As antisites relative to the Mn, and ii) the As antisite concentration. We explain our results using a model of competing antiferromagnetic super-exchange and ferromagnetic double-exchange via localized Zener carriers. The strong dependence of the ferromagnetic order on the microscopic configuration accounts for the large variation in experimental data.

In the past ten years the study of diluted magnetic semiconductors (DMS) has been strongly revitalized since the discovery of ferromagnetic order in In1-xMnxAs Ohno1  and Ga1-xMnxAs Ohno2 ; Ohno3 ; Ohno4 . The potential utility of room temperature ferromagnetism in a semiconductor based system is enormous. On one hand, DMS could be replace the existing metallic magnetic elements in storage media Prinz . Here their better compatibility with existing semiconductors and MBE-growth technology over their metallic counterparts is a great advantage. On the other hand DMS can be used as spin injectors into semiconductors Aws1 ; Sch1 . This is a critical step in the physical realization of quantum computation based on the spin degree of freedom in a solid state device DDV . In fact, although it has been shown that spin can be coherently transported over several micrometers in GaAs Aws2 ; Aws3 , its injection from metallic magnetic contacts is largely unsuccessful if not impossible Schm1 . This is due to the large mismatch between the resistances of the metallic contacts and the semiconductor. The use of DMS solves this problem Aws1 ; Sch1  and (Ga,Mn)As together with GaAs and (Al,Ga)As represent to date the most promising material system for the injection, storage and manipulation of spins in semiconductors.

Although there is general agreement on the carrier- (hole-) mediated origin of the ferromagnetism in (Ga,Mn)As, the detailed mechanism is still debated. The Zener model in the mean field approximation Diet1  provides a good starting point. However its prediction of the Curie temperature as a function of Mn and hole concentration largely overestimates the actual value if a dynamic description of the Mn spins is considered McD . Moreover recent density functional theory (DFT) results us1  show that the $`p`$-$`d`$ coupling in (Ga,Mn)As is very strong and the mean field approximation cannot be completely justified. Finally DFT calculations based on the coherent-potential approximation (CPA) Akai  suggest that the ferromagnetic order in (Ga,Mn)As may result from the competition between ferromagnetic double-exchange and antiferromagnetic super-exchange interactions.

Note that all these models agree on the following important points: i) Mn2+ ions substitute the Ga3+ cations in the zincblende lattice providing local $`S=5/2`$ spins, and ii) there are free holes in the system although the actual concentration is much smaller than the density of Mn ions Ohno3 ; Ohno4 . This latter point suggests that some mechanism of compensation must be taking place, most likely the presence of intrinsic donor defects such as As antisites (AsGa) or Ga vacancy-interstitial As pairs (VGa-Asi), which are usually found in low-temperature GaAs Dab . In the above models the compensation mechanism is implicitly incorporated in the mean field description of the GaAs valence band, since the hole concentration is a free parameter. As a result the local effects of magnetic and chemical disorder are neglected.

In this paper we consider explicitly the effects of the inclusion of AsGa in (Ga,Mn)As at different dilutions, and study how the chemical environment modifies the magnetic interaction between the Mn ions. We perform DFT calculations within the local spin density approximation (LSDA), and consider large GaAs cells in which Mn ions and AsGa are inserted. We study the dependence of the magnetic coupling between Mn ions on: i) Mn concentration, ii) AsGa concentration, iii) relative positions of the Mn ions and the AsGa defects. The main result of our analysis is that, for a uniform distribution of Mn ions, AsGa antisites strongly weaken the ferromagnetic coupling. However, at least for moderate concentrations, the compensation does not follow the expected nominal valences of Mn and As (that is one AsGa does not completely compensate the holes from two Mn ions). Moreover when two Mn ions are separated by only one As atom (so that they occupy two corners of a zincblende tetrahedron with an As atom in the center), ferromagnetic coupling is possible even far above compensation if As antisites are located at the other two tetrahedral positions to form Mn2As3 complex (see Fig.3c).

Our calculations are performed using the code siesta Siesta1 ; Siesta2 ; Siesta3 , which is an efficient implementation of DFT-LSDA based on pseudopotentials and a numerical localized atomic orbital basis set. This method combines good accuracy and small computational cost compared to other methods based on plane-waves. We have described in a previous paper us1  the calculation details and the prescriptions one needs to optimize the basis set and the pseudopotentials. Here we just mention that we use Troullier-Martins pseudopotentials TM  with non linear core corrections Lou82  and Kleinman-Bylander factorization KB1 , and the Ceperley-Alder CA  form of the exchange-correlation potential.

We construct 64 (cubic) and 32 (rectangular) atom GaAs cells in which we include two Mn ions and a variable number of AsGa antisites. These correspond to Mn concentrations of $`x`$=0.0625 (to date the largest concentration obtained experimentally) and $`x`$=0.125 respectively. We investigate two different Mn configurations for each concentration: 1) the Mn ions occupy positions as far apart as possible (i.e. the corner and the middle of the cubic cell), 2) the Mn atoms occupy two corners of a tetrahedron and are coordinated through a single As ion (see Fig.3). We call these two configurations separated and close respectively. The cells are then periodically repeated using 18 $`k`$-points in the irreducible cubic Brillouin zone. Note that the periodic boundary conditions fix the magnetic coupling between Mn ions that occupy equivalent positions in adjacent cells to be ferromagnetic but that the coupling between the two Mn ions in the same cell can be ferromagnetic or antiferromagnetic. We calculate the ground-state properties of these systems for both ferromagnetic (FM) and antiferromagnetic (AF) alignment of the Mn ions within the cells.

The energy differences between the AF and FM aligned configurations, $`\mathrm{\Delta }_{\mathrm{FA}}`$, and the magnetization per Mn ion, $`M_{\mathrm{Mn}}`$, for the separated arrangement are presented in Fig.1 as a function of the number of AsGa antisites. The magnetization per Mn ion is defined to be half of the magnetization of the cell, calculated in the FM aligned phase.

First we note that the ferromagnetic coupling is strongly weakened by AsGa antisite doping. This is consistent with the picture of magnetic coupling mediated by free carriers (holes): AsGa antisites contribute electrons into the system and therefore compensate the holes. We also note that in the case of no antisites the ferromagnetic order is much stronger in the case of large Mn concentration, which again supports the model of carrier-induced ferromagnetism. Within this model, the ferromagnetic coupling should disappear when the compensation is complete. However the figure suggests that the compensation mechanism does not follow the nominal atomic valence, since a single AsGa antisite per cell is not sufficient to destroy the ferromagnetic coupling. Above compensation (one AsGa for two Mn ions) antiferromagnetic coupling is obtained for large Mn concentration, while the system stays ferromagnetic at low concentration. This is consistent with the onset of antiferromagnetic super-exchange coupling, the mechanism which is believed to be responsible for the magnetic order in the II-VI DMS 26 , at compensation. Super-exchange is a short range interaction and therefore is less important in the low concentration limit where the Mn ions are well separated. It is worth noting that for $`x`$=0.125 and large antisite concentrations ($`n`$ AsGa=2) the magnetic order is quite sensitive to the actual position of the antisite respect to the Mn ions. Different AsGa arrangements may result either in ferromagnetic or antiferromagnetic coupling.

If we now consider the magnetization per Mn ion (Fig.1b) we note that there is a monotonic increase of the total magnetic moment on antisite doping. This can be understood by looking at the density of states of Fig.2 (see also Ref.us1, ). At the Fermi energy the DOS of the majority spin band is the result of the hybridization between the Mn $`d`$ states with $`t_2`$ symmetry and the $`p`$ states coming mainly from AsGa. In fact the two donor levels of isolated AsGa in GaAs are known to lie 0.54 eV and 0.75 eV above the GaAs valence band Dab  and to overlap with the exchange split Mn $`d`$ levels of low dilution (Ga,Mn)As us1 . In contrast the DOS of the minority spin band is dominated by antisite levels, the first Mn $`d`$ states lying far above $`E_\mathrm{F}`$. Therefore by increasing the antisite concentration, $`E_\mathrm{F}`$ is shifted towards higher energy, thus increasing the occupation of the Mn $`d`$ shell in the majority spin band. This enhances the total magnetic moment of the system. Finally note that a magnetization of 4.5$`\mu _\mathrm{B}`$ is in very good agreement with recent x-ray magnetic circular dichroism measurements Ohl1 .

Let us now turn our attention to the close configuration. In this case we expect the short range super-exchange to play a more important rôle since the Mn ions are much closer to each other. Moreover the magnetic coupling within a cell is expected to be quite sensitive to the position of the antisites with respect to the Mn ions. We consider the three different situations sketched in Fig.3: a) the antisites are far from the Ga2Mn2As1 complex, b) one antisite occupies a tetrahedral site (Ga1Mn2As2), c) two antisites occupy the tetrahedral sites (Mn2As3).

In Fig.4 we show $`\mathrm{\Delta }_{\mathrm{FA}}`$ and $`M_{\mathrm{Mn}}`$ as a function of the AsGa concentration for the different antisite arrangements of Fig.3. For the sake of brevity we present data only for $`x`$=0.0625, noting that similar conclusions can be made also for $`x`$=0.125.

From Fig.4 it is very clear that, when the AsGa defects are in the vicinity of the Mn ions (configurations (b) and (c) of Fig.3), the system is almost insensitive to the AsGa concentration. In contrast when the AsGa antisites are far from the Mn ions the magnetic coupling undergoes a FM to AF transition with increasing antisite concentration.

Consider first configuration (a). In this case both the $`\mathrm{\Delta }_{\mathrm{FA}}`$ and $`M_{\mathrm{Mn}}`$ curves look very similar to the curves we found for the separated arrangement (Fig.1). However, in stark contrast with the separated case, an AF alignment can now also be found for large AsGa concentrations. Recalling the fact that the Mn $`d`$ shell is more than half-filled, and that it is antiferromagnetically coupled with the As $`p`$ shell of the intermediate atom us1 , we propose that super-exchange coupling stabilizes the AF phase as soon as the free-holes are completely compensated. However this mechanism is extremely short range and therefore effective only when the Mn ions are separated by one As.

We now turn our attention to situations (b) and (c). In both cases the ferromagnetic alignment is stable and almost insensitive to the total AsGa concentration. This is a strong indicator that the dominant interaction in these cases is one that depends only on the local chemical properties. To shed some light on this aspect we present the results of Mülliken population analyses Mul ; us1  of the system.

The Mülliken orbital (or atomic) population is the projection of the charge density onto a particular orbital (or atom). Although the absolute values depend on the chosen basis set, it is a useful quantity for understanding the charge distribution within a given material. In table 1 we present the Mülliken orbital population for the two Mn ions and the intermediate As ion of the complexes of Fig.3. The most obvious feature is the larger polarization of the As-$`p`$ orbitals in Mn2As3 compared with Ga2Mn2As1. This is accompanied by a small decrease in Mn-$`d`$ polarization, although this latter effect could be an artifact from the overlap component of the orbital population us1 . It is also interesting to note that the total atomic population of the As atom increases going from (a) to (b) to (c), while the $`p`$ component of the population decreases. Therefore if we start from the situation in which two AsGa antisites are located far from the Mn-As-Mn complex, then we move each antisite in turn to one of the two other corners of the tetrahedron, then i) the charge on the middle As atom increases, ii) the spin-polarization of the $`p`$ shell of the middle As atom increases, and iii) the total population of the $`p`$-shell of the middle As atom decreases. And most importantly the magnetic coupling changes from antiferromagnetic to ferromagnetic.

In 1960 de Gennes observed DG  that in an antiferromagnetic crystal the presence of a bound carrier (electron or hole) which is Zener coupled to the local spins always induces a distortion in the antiferromagnetic lattice. In that spirit we propose that the observed transition from antiferromagnetic to ferromagnetic coupling between Ga2Mn2As1 and Mn2As3 results from the onset of ferromagnetic double-exchange coupling mediated by a bound Zener carrier. This is further supported by recent calculations us2  in which we show that the actual ground state for Ga1Mn2As2 is not one of perfect ferromagnetic alignment, but instead the Mn magnetic moments are canted with respect to each other.

In conclusion we have shown that the AsGa antisites’ inclusion in (Ga,Mn)As can result in a variety of different behaviors depending on the microscopic arrangement of the Mn ions and the AsGa antisites. In particular we have shown that when the Mn ions are uniformly distributed in the crystal, AsGa antisites weaken the ferromagnetic order. In contrast if the Mn ions occupy two corners of the zincblende tetrahedron several magnetic arrangements are possible depending on the positions of the antisites. In particular ferromagnetic coupling is obtained if antisites occupy the other positions in the tetrahedron. This suggests that a way to obtain high $`T_\mathrm{c}`$ in (Ga,Mn)As is either to reduce the As antisite concentration, or to deposit Mn and As antisites with a strongly inhomogeneous distribution.

This work made use of MRL Central Facilities supported by the National Science Foundation under award No. DMR96-32716. This work is supported by the DARPA/ONR under the grant N0014-99-1-1096, by ONR grant N00014-00-10557, by NSF-DMR under the grant 9973076 and by ACS PRF under the grant 33851-G5.