text:
# Detecting Population III stars through observations of near-IR cosmic infrared background anisotropies.

## 1 Introduction

The cosmic infrared background (CIB) arises from the accumulated emission of galaxy populations spanning a large range of redshifts. The earliest epoch for the production of this background occurred when star formation first began, and contributions to the CIB continue through the present epoch. The CIB is thus an integrated summary of the collective star forming events, star-burst activity, and other luminous events in cosmic history to the present time.

With the WMAP measurements (Bennett et al (2003)) the structure of the last scattering surface has been mapped and a firm cosmological model has now emerged: the Universe is flat, dominated by the vacuum energy or an exotic quintessence field and is consistent with the inflationary paradigm and a cold-dark-matter (CDM) model. In this paper, we adopt the $`\mathrm{\Lambda }`$CDM model with cosmological parameters from the WMAP and other observations: $`\mathrm{\Omega }_{\mathrm{baryon}}=0.044,h=0.71,\mathrm{\Omega }_\mathrm{m}=0.3,\mathrm{\Omega }_\mathrm{\Lambda }=0.7,\sigma _8=0.84`$. Following the last scattering at $`z1000`$, the Universe entered an era known as the ”Dark Ages”, which ended with the star formation which produced Population III stars. The WMAP polarization results (Kogut et al (2003)) show that the Universe had an optical depth since last scattering of $`\tau 0.2`$, indicating an unexpectedly early epoch of the first star formation ($`z_{}20`$). From the opposite direction in $`z`$, optical and IR telescopes are now making progress into understanding the luminosity history during the most recent epoch of the universe ($`z<5`$), but the period from recombination to the redshift of the galaxies in the Hubble Deep Field (HDF) remains largely an unexplored era. The first objects in the Universe probably formed in mini-halos of $`10^{56}M_{}`$ (e.g. Miralda-Escude (2003)) (barring the possible radiative feedback effects), which would remain largely inaccessible to current instruments and conventional methods.

A consensus based on recent numerical investigations is now emerging that fragmentation of the first collapsing clouds at redshift $`z_{}`$ was very inefficient so that the first metal-free stars were extremely massive with mass $`\genfrac{}{}{0pt}{}{_>}{^{}}100M_{}`$ (Abel et al (2002); Bromm et al (1999)). Such stars would live only a few million years, which is much less than the age of the Universe ($`2\times 10^8`$ years at $`z=20`$), making their direct detection still more difficult. It is unclear how long the era of Population III stars lasted and when the Population II stars formed with metallicities $`10^3`$ solar (Schneider et al (2002)). On the other hand the net radiation produced by these massive stars will give substantial contributions to the total diffuse background light (Rees (1978)) and since their light is red-shifted much of that contribution will be today in the infrared bands (Bond et al (1986)) contributing significantly to the near-IR CIB.

Observationally, the CIB is difficult to distinguish from the generally brighter foregrounds from the local matter within the Solar system, and the stars and ISM of the Galaxy. A number of investigations have attempted to extract the isotropic component (mean level) of the CIB from ground- and satellite-based data (see Hauser & Dwek (2001) for a recent review). These analyses of the COBE data have revealed the CIB at far-IR wavelengths $`\lambda >100`$$`\mu `$m(Hauser et al (1998)), and probably at near-IR wavelengths from 1 \- 3 $`\mu `$m (Dwek & Arendt (1998); Gorjian et al (2001); Cambresy et al (2001)) with additional support from analysis of data from IRTS (Matsumoto et al (2000)). However, none of the reported detections of the isotropic CIB are very robust (especially at near–IR wavelengths), because all are dominated by the systematic uncertainties associated with the modeling and removal of the strong foreground emission. Furthermore, the near-IR colors of the mean CIB do not differ greatly from those of the foregrounds, limiting the use of spectral information in distinguishing the true CIB from residual Galactic or solar system emission. Because of the difficulty of exactly accounting for the contributions of these bright foregrounds when measuring the CIB directly, and the difficulty in detecting all the contributing sources individually, it was proposed to measure the structure or anisotropy of the CIB via its angular power spectrum (Kashlinsky et al (1996)). For a relatively conservative set of assumptions about clustering of distant galaxies, fluctuations in the brightness of the CIB have a distinct spectral and spatial signal, and these signals can be more readily discerned than the actual mean level of the CIB.

In Fig. 1, we summarize the current near-IR CIB measurements and compare the measured CIB at 1.25 and 2.2 $`\mu `$m to the total flux from the observed galaxy populations. There is a statistically significant excess over the CIB expected from normal galaxies; e.g. at 1.25 $`\mu `$m (J band) and 2.2 $`\mu `$m (K band), while an integration of the measured galaxy counts gives only 30-40% of the observed CIB (Kashlinsky & Odenwald 2000b ; Gardner (1996); Madau & Pozzetti (2000)). If this deficit CIB does not come from undetected low surface brightness emission associated with local galaxies, it must come from fainter galaxies at high $`z`$.

The measurements of CIB structure or fluctuations lead to similar conclusions (Kashlinsky & Odenwald 2000a ; Matsumoto et al (2000); Kashlinsky et al (2002); Odenwald et al (2003)). The detection of CIB fluctuations at $`0.7^\mathrm{o}`$ from COBE DIRBE bands at 1.25 to 5 micron (Kashlinsky & Odenwald 2000a ) shows a signal $`23`$ times that expected from normal galaxy populations evolving via a present day IMF with the observed star formation rates out to $`z34`$ (Jimenez & Kashlinsky (1999)). Recently, using combined 2MASS calibration data with long net exposures, it became possible to remove resolved galaxies and measure the near-IR CIB fluctuations spectrum from a few arcsec to a few arcmin. We argued that this signal originated from faint galaxies (K$`\genfrac{}{}{0pt}{}{_>}{^{}}19`$) at high $`z`$ (Kashlinsky et al (2002); Odenwald et al (2003)), and is significantly larger that what is expected from normal galaxy populations. This suggests that the excess originates from still earlier epochs.

## 2 CIB flux and Population III

The near-IR CIB signals detected in the 2MASS long integration data (Kashlinsky et al (2002); Odenwald et al (2003)) could come from the Population III stars (Magliochetti et al (2003); Kashlinsky et al (1999); Cooray, A. et al (2003); Santos et al (2002); Salvaterra & Ferrara (2003)). The argument can be generalized and shown to be nearly model-independent provided Population III stars were very massive.

Massive, metal-free stars will be dominated by radiation pressure and would radiate close to the Eddington limit: $`LL_{\mathrm{Edd}}=\frac{4\pi Gm_pc}{\sigma _T}M1.3\times 10^{38}M/M_{}`$ erg/sec, where $`\sigma _T`$ is the cross section due to electron (Thompson) scattering. The energy spectrum for emission from these stars will be nearly featureless and close to that of a black body at $`T10^{4.85}`$K (Schaerer (2002); Tumlinson et al (2003)). Unlike stars with higher metallicity, Population III stars are not expected to have significant mass-loss during their lifetime (Baraffe et al (2001)). If sufficiently massive ($`\genfrac{}{}{0pt}{}{_>}{^{}}240M_{}`$, see Bond et al (1984)) such stars would also avoid SN explosions and collapse directly to black holes. In this case their numbers could significantly exceed the minimum that would be required to produce the metallicities observed in Population II stars. The lifetime of these stars will be independent of mass: $`t_LϵMc^2/L3\times 10^6`$ years, where $`ϵ=0.007`$ is the efficiency of the hydrogen burning. These numbers are in good agreement with detailed computations (Schaerer (2002)).

For a flat Universe the co-moving volume per unit solid angle contained in the cosmic time interval $`dt`$ is $`dV=c(1+z)^1d_L^2dt`$, where $`d_L`$ is the luminosity distance. The flux per unit frequency interval from each of the Population III stars will be $`Lb_\nu ^{}(1+z)/4\pi d_L^2`$, where $`b_\nu `$ is the fraction of the total energy spectrum emitted per unit frequency and $`\nu ^{}=\nu (1+z)`$ is the rest-frame frequency. (The Population III SED is normalized so that $`b_\nu 𝑑\nu =1`$). The co-moving mass density in these stars is $`Mn(M,t)𝑑M=\mathrm{\Omega }_{\mathrm{baryon}}\frac{3H_0^2}{8\pi G}f_{}`$, where $`f_{}`$ is the fraction of the total baryonic mass in the Universe locked in Population III stars at time $`t`$. The net flux per unit frequency from a population of such stars with mass function $`n(M)dM`$ is given by:

$$\frac{d}{dt}I_\nu =\frac{Ln(M,t)𝑑M}{4\pi d_L^2}(1+z)b_\nu ^{}\frac{dV}{dt}=\frac{c}{4\pi }b_\nu ^{}\frac{L}{M}f_{}\rho _{\mathrm{baryonic}}$$
(1)
Here $`b_\nu Ln(M,t)b_\nu 𝑑M/Ln(M,t)𝑑M`$ denotes the mean Population III SED averaged over their initial mass function and $`\frac{L}{M}Ln(M,t)𝑑M/Mn(M,t)𝑑M`$. For a Gaussian density field $`f_{}5\times 10^23\times 10^3`$, if on average Population III formed in 2–3 sigma regions (see below). Provided that $`L/M=`$ constant, this result does not depend on the details of the initial mass function of Population III stars (cf. Fig. 5 in ref. Salvaterra & Ferrara (2003)). (Note that for the present day stellar populations their mass-to-light ratio depends strongly on stellar mass and $`\frac{L}{M}`$ is much smaller than the Population III value of $`4\pi Gm_pc/\sigma _T3.3\times 10^4L_{}/M_{}`$ leading to substantially smaller net fluxes). Assuming no significant mass loss (Baraffe et al (2001)) during their lifetime $`t_L`$ for Population III stars, these stars will produce CIB flux of amplitude:

$$\nu I_\nu =\frac{3}{8\pi }\frac{1}{4\pi R_H^2}\frac{c^5}{G}ϵ\mathrm{\Omega }_{\mathrm{baryon}}\frac{1}{t_L}f_{}\nu ^{}b_\nu ^{}\frac{dt}{1+z}$$
(2)
Note that $`c^5/G`$ is the maximal luminosity that can be achieved by gravitational processes and enters here because the nuclear burning of stars evolves in gravitational equilibrium with the (radiation) pressure. This result, eq. 2, has a simple meaning illustrating its model-independence: the cumulative bolometric flux produced is $`L_{\mathrm{max}}=c^5/G10^{26}L_{}`$ distributed over the surface of the Hubble radius, $`4\pi R_H^2`$, times the model-dependent dimensionless factors. The spectral distribution of the produced diffuse background will be determined by $`\overline{b_\nu }f_{}(1+z)^1b_\nu 𝑑t/f_{}(1+z)^1𝑑t`$, which is the mean SED averaged over the first star epoch (hereafter assumed to have duration $`t_{}`$). The value of $`L_{\mathrm{max}}/4\pi R_H^2`$ is $`3\times 10^8\mathrm{nW}/\mathrm{m}^2/\mathrm{sr}`$ so even with small values of $`\mathrm{\Omega }_{\mathrm{baryon}},ϵ,f_{}`$, the net flux from Population III stars would be substantial. The K-band roughly coincides with the Lyman limit (912 Å) at $`z_{}20`$ so much of the emitted flux would contribute today in the near IR bands. If there was a population of massive black holes, as seems likely to result from Population III evolution, their accretion processes will emit radiation at a much higher efficiency of $`ϵ0.1`$ (and perhaps as high as $`ϵ0.4`$ very close to the event horizon). At the same time, the K-band CIB excess over the total contribution from the observed galaxy populations ($`9`$$`\mathrm{nW}/\mathrm{m}^2/\mathrm{sr}`$up to K$`24`$), is $`1015`$$`\mathrm{nW}/\mathrm{m}^2/\mathrm{sr}`$and can be completely accounted for by the contribution from Population III stars at high redshifts.

The first stars formed in rare regions of the density field that reached the turn-around over-density while the bulk of the matter was still in a linear regime (density contrast $`<1`$). These regions stopped expanding and began collapsing, forming the first generation of stars if certain conditions are met. For a Gaussian density field, as required for the CDM models, this would specify the value of $`f_{}`$ at each time. The power spectrum of the mass distribution on large scales preserved the Harrison-Zeldovich power spectrum index ($`n1`$), but on scales less than the horizon scale at the matter-radiation equality, the spectrum was modified by the different growth-rates of sub- and super-horizon modes. This led to a gradual decrease of $`n`$ toward the very small scale value of $`n\genfrac{}{}{0pt}{}{_<}{^{}}2`$, suppressing the small scale power and leading to late collapse and galaxy formation. In this picture, it is surprising that the the first stars started forming at $`z_{}=20_9^{+10}`$, as indicated by the WMAP polarization measurements, but the most straightforward explanation is that the earliest stars formed out of very high peaks of the density field, leading to smaller $`f_{}`$.

Assuming a spherical model for growth and collapse of density fluctuations, any density fluctuation that reached the dimensionless density contrast $`\delta _{\mathrm{col}}=1.68`$ will collapse. Consequently, if $`\sigma _M`$ is the rms fluctuation at $`z`$ over a sphere containing the total mass $`M`$, then $`\eta \delta _{\mathrm{col}}/\sigma _M`$ measures the numbers of standard deviations for that mass to collapse at that redshift. Here, $`\sigma _M`$ is related to the underlying power spectrum via $`\sigma _M^2=\frac{1}{2\pi ^2}P(k;z)W(kr_M)k^2𝑑k`$ where $`r_M=1.4(M/10^{12}h^1M_{})^{1/3}(\mathrm{\Omega }/0.3)^{1/3}h^1`$Mpc is the co-moving linear scale containing mass $`M`$, and $`W(x)=(3j_1(x)/x)^2`$. As they collapse, the primordial clouds will quickly heat up to their virial temperature, $`T_{\mathrm{vir}}`$, and only efficient cooling will enable isothermal collapse, where gas pressure is smaller than gravity (or $`T<T_{\mathrm{vir}}`$).

The details of what determines the collapse and formation of Population III stars are not yet clear, but molecular cooling is critical in the initial stages of metal-free collapse. Molecular cooling is effective at $`T\genfrac{}{}{0pt}{}{_>}{^{}}400`$ K (Santos et al (2002)), but some simulations suggest that rotational $`H_2`$ cooling can effectively dissipate binding energy of the cloud only if $`T>2000`$ K (Miralda-Escude (2003)). We have evaluated the rms mass density fluctuation, $`\sigma _M`$, for the $`\mathrm{\Lambda }`$CDM model as a function of its virial temperature, assuming a molecular weight of $`\mu =1`$. The left panel of Fig. 2 shows the resulting $`\eta `$ vs $`z`$ for $`T_{\mathrm{vir}}=`$ 400K and 2000K. For a Gaussian density field and $`\eta >1`$ the value of $`f_{}\mathrm{erfc}(\eta /\sqrt{2})`$. One can see that Population III stars had to form out of 2 to 3 sigma fluctuations, which for a Gaussian distribution correspond to $`f_{}`$ varying between $`5\times 10^2`$ and $`3\times 10^3`$. Departures from spherical symmetry would accelerate the collapse, decreasing $`\eta `$ and increasing $`f_{}`$. Because $`\eta `$ is a decreasing function of decreasing $`z`$, and $`f_{}`$ is a (rapidly) increasing function of decreasing $`\eta `$, the average $`\overline{f_{}}`$ will be dominated by the late times of Population III evolution.

The right panel of Fig. 2 shows that the total diffuse background light produced during the first star era should be substantial and measurable. Much of the diffuse flux produced by the Population III stars will today be observable in the near-IR, and could be responsible for the observed excess near-IR CIB. If $`z_f`$ is large the net bolometric flux from Population III is smaller, but because of the redshift effects a larger fraction of the bolometric flux will be observed today in the near-IR bands. Furthermore, the near-IR part of the CIB emission from Population III would be increased because much of the shorter wavelengths emission gets absorbed and re-emitted at these bands by Lyman and free-free emission from the ionized nebulae around Population III stars (Santos et al (2002)). Dashed line shows the total CIB flux evaluated from the DIRBE 1.25 to 3.5 $`\mu `$m bands. Taken at face value that would imply that the first star era lasted until $`z_f\genfrac{}{}{0pt}{}{_<}{^{}}15`$. However, Population III stars only contribute a fraction of the observed CIB.

## 3 CIB anisotropies from Population III

The contribution of Population III stars to the CIB will possess a spatial structure that is related to that of density fluctuations from which the stars formed. At particular spatial scales and wavelengths it may prove easier to distinguish the Population III contribution from the various foregrounds through the spatial structure rather than the measurement of the mean (isotropic) intensity.

In the limit of small angles the 2-dimensional angular power spectrum, $`P_2(q)`$, of the CIB fluctuations that arise from clustering of Population III systems with the 3-dimensional power spectrum $`P_3(k)`$ is given by the modified Limber equation (Kashlinsky & Odenwald 2000a ):

$$P_2(q)=\frac{1}{c}\left(\frac{dI_\nu ^{}}{dt}\right)^2\frac{P_3(qd_A^1;z)}{d_A^2}𝑑t$$
(3)
where $`d_A`$ is the comoving angular diameter distance. The power spectrum $`P_3`$ is in turn related to the underlying $`\mathrm{\Lambda }`$CDM model power spectrum and its evolution and growth. On larger angular scales ($`\theta \genfrac{}{}{0pt}{}{_>}{^{}}`$ a few arcmin) the power spectrum is in the linear regime and we evaluate the growth rate of fluctuations using linear theory for the $`\mathrm{\Lambda }`$-dominated cosmology.

On sufficiently small scales the primordial power spectrum of the density field will be modified by non-linear gravitational effects. Fig. 3 shows the density field for the $`\mathrm{\Lambda }`$CDM model at various high redshifts. The linear power spectrum was taken to be that of the $`\mathrm{\Lambda }`$CDM for the WMAP cosmological parameters. The non-linear evolution of the density field was modeled analytically using the approximation from ref. (Peacock & Dodds (1996)). For reference 1 arcmin subtends the comoving scale of $`1.5h^1`$Mpc at $`z`$ between 6 and 15 for WMAP cosmological parameters and a dark energy equation of state with $`w=1`$. The dotted line shows the linearly evolved density field at $`z=15`$. On sub-arcminute scales the density field is in the quasi-linear to non-linear regime (density contrast $`\genfrac{}{}{0pt}{}{_>}{^{}}0.2`$) for the $`\mathrm{\Lambda }`$CDM model. There the spectrum due to clustering evolution was modified significantly and the fluctuations amplitude has increased from its primordial value, especially since the effective spectral index on these scales for $`\mathrm{\Lambda }`$CDM model was $`n\genfrac{}{}{0pt}{}{_<}{^{}}2`$.

To within a factor of order unity, the square of the fractional fluctuation of the CIB on angular scale $`\pi /q`$ is $`\delta _{\mathrm{CIB}}^2=(\delta I_\nu )^2/I_\nu ^2I_\nu ^2q^2P_2(q)/2\pi `$. The meaning of eq. 3 can be demonstrated by assuming $`dI_\nu ^{}/dt`$=constant during the Population III phase of duration $`t_{}`$. In this case the fractional fluctuation due to clustering of early star systems becomes:

$$\delta _{\mathrm{CIB}}^2=\frac{\pi }{t_{}}\mathrm{\Delta }^2(qd_A^1;z)𝑑t$$
(4)
Here $`\mathrm{\Delta }(k)=[\frac{1}{2\pi ^2}\frac{k^2P_3(k)}{ct_{}}]^{1/2}`$ is the fluctuation in number of sources within a volume $`k^2ct_{}`$. In other words, the fractional fluctuation on angular scale $`\pi /q`$ in the CIB from Population III stars is given by the average value of the r.m.s. fluctuation from Population III spatial clustering over a cylinder of length $`ct_{}`$ and diameter $`k^1`$. At $`z=20`$ the Universe is $`2\times 10^8`$ years old which is much larger than the age of the individual Population III stars, $`t_L3\times 10^6`$ years. If the first stars lasted for only one generation forming at $`z_{}`$, the relative CIB fluctuations will be $`\delta _{\mathrm{CIB}}\sqrt{\pi }\mathrm{\Delta }(qd_A^1;z)|_z_{}`$.

Several points are worth noting about eq. 3: Firstly, the value of $`\mathrm{\Delta }(k)`$ is inversely proportional to $`\sqrt{t_{}}`$ and thus measures the duration of the first star era. The density perturbations grow with decreasing $`z`$, so most of the contribution to the integral in eq. 3 comes from the low end of $`z`$. The overall dependence on $`t_{}`$ wins out and the longer the Population III phase, the smaller are the relative fluctuations of the CIB from them. Secondly, in the Harrison-Zeldovich regime of the power spectrum, $`P_3k`$, one would have $`\delta _{\mathrm{CIB}}q^{1.5}`$. Finally, the transition to the Harrison-Zeldovich regime occurs in the linear regime at all relevant redshifts and happens at the co-moving scale equal to the horizon scale at the matter-radiation equality. This feature would occur at different angular scales as the redshift of the Population III era decreases. All this would allow probes of the epoch of the first stars, its duration, and the primordial power spectrum at high redshifts on scales that are currently not probed well. Interestingly, a short duration for the first stars will lead to smaller CIB flux, but larger relative fluctuations and vice versa.

In addition to the small angular scale increase due to non-linear gravitational evolution, the fluctuations in the distribution of Population III systems will be amplified because, as Fig. 2 shows, these systems had to form out of rare peaks of the primordial density field. Consequently, their 2-point correlation function will be amplified (Kaiser (1984); Jensen & Szalay (1986); Politzer & Wise (1984); Kashlinsky (1987, 1998)) over that given by the $`\mathrm{\Lambda }`$CDM power spectrum, $`\xi =\frac{1}{2\pi ^2}P_3(k)j_0(kr)k^2𝑑k`$. Adopting a Press-Schechter prescription for the formation of collapsed objects (Press & Schechter (1974)) from a correlated density field leads to the following expression for the amplification of the 2-point correlation function (Kashlinsky (1998)):

$$\xi _\eta =\xi \underset{m=0}{\overset{\mathrm{}}{}}\frac{\eta ^{2m}}{m!\delta _{\mathrm{col}}^{2m}}\xi ^m\left[\frac{H_{m+1}^2(\eta /\sqrt{2})}{2\eta ^2}+\frac{H_{m+2}^2(\eta /\sqrt{2})}{4(m+1)\delta _{\mathrm{col}}^2}\right]$$
(5)
where $`H_n`$ are Hermite polynomials. At large values of $`\eta `$ this reduces to $`\xi _\eta \mathrm{exp}(\eta ^4\xi /\delta _{\mathrm{col}}^2)1`$. At small values of $`\xi 1`$ (and sufficiently large angular scales) the amplification factor is linear and equal to $`\eta ^4/\delta _{\mathrm{col}}^2`$. At very small scales the amplification is non-linear in $`\xi `$ and will exceed the linear amplification value leading to larger CIB fluctuations. We computed the resultant CIB fluctuations using the linear bias amplification approximation, but note that this gives a lower limit on the resultant CIB fluctuations.

There will also be shot-noise fluctuations due to individual Population III systems entering the beam. The relative magnitude of these fluctuations will be $`N_{\mathrm{beam}}^{1/2}`$, where $`N_{\mathrm{beam}}`$ is the number of the Population III systems within the beam. This component will be important at very small angular scales, where $`N_{\mathrm{beam}}1`$, and will contribute to the power spectrum: $`P_{\mathrm{SN}}=1/n_2`$, where $`n_2=cn_3d_L^2(1+z)^1𝑑t`$ is the projected angular number density of Population III systems. Detection of the shot-noise component in the CIB power spectrum at small angular scales will give a direct measure of both the duration of the first star era and constrain the makeup and masses of the Population III systems. The three-dimensional number density can be evaluated from the Press-Schechter (Press & Schechter (1974)) formalism, but in the appropriate limits ($`\eta >1`$) it becomes $`n_3\rho _{\mathrm{baryon}}M^1\mathrm{erfc}(\eta (z)/\sqrt{2})`$. Fig. 4 shows that the mean projected surface density of Population III systems $`n_2`$ for $`T_{\mathrm{vir}}>`$ 400 K and 2000 K. One can see that unless the Population III era was very short, the shot noise correction to the CIB would be small on scales greater than a few arcseconds.

Essentially all of the flux emitted at rest wavelength less than 912 Å will be absorbed by the Lyman continuum absorption in the surrounding medium (Yoshii & Peterson (1994)) and the contribution to the CIB will be cut off at $`\lambda <912(1+z_f)`$ Å. At longer wavelengths the flux, including emission from the nebulae around each star, will propagate without significant attenuation. Population III stars emit as black bodies at $`\mathrm{log}T4.85`$ (Schaerer (2002)) and the Lyman limit at $`z20`$ is shifted to $`2\mu `$m in the observer’s frame. The 2MASS J band filter contains emission out to 1.4 $`\mu `$m and represents the shortest wavelength where excess in the CIB over that from normal galaxies has been measured (Cambresy et al (2001); Kashlinsky et al (2002)). If the measured excesses in CIB fluctuations (Kashlinsky et al (2002); Kashlinsky & Odenwald 2000a ) and isotropic component (Cambresy et al (2001)) at J band are indeed attributable to Population III, their era must have lasted until $`z\genfrac{}{}{0pt}{}{_<}{^{}}14`$.

Fig. 5 shows the resultant CIB fluctuations from Population III stars at 1.25, 2.2 and 3.5 micron or J, K and L photometric bands. The assumed CIB fluxes from Population III are listed near the tops of the panels. At 2.2 micron the galaxies contribute around 9 $`\mathrm{nW}/\mathrm{m}^2/\mathrm{sr}`$whereas the net CIB flux is around 20-25 $`\mathrm{nW}/\mathrm{m}^2/\mathrm{sr}`$; hence the assumed excess of 10-15 $`\mathrm{nW}/\mathrm{m}^2/\mathrm{sr}`$is attributed to the Population III stars for the purposes of this discussion and is taken to be 12 $`\mathrm{nW}/\mathrm{m}^2/\mathrm{sr}`$in the figure. The situation is similar at 3.5 micron (Dwek & Arendt (1998); Gorjian et al (2001)) and the excess was taken to be 5 $`\mathrm{nW}/\mathrm{m}^2/\mathrm{sr}`$(Wright (2003)). The excess in the J band over the total flux from normal galaxies was taken from (Cambresy et al (2001)). The clustered component of the CIB fluctuation displayed in the figure can be rescaled to other CIB fluxes via eq. 4. Thin colored lines assume constant rate of production of the Population III fraction of the CIB and the flat SED with $`b_\nu =`$ constant. All Population III stars were assumed to start forming at $`z_{}=20`$, but different colored lines correspond to different values of $`z_f`$, the redshift of the end of the first star era. Thick colored lines correspond to a Population III contribution produced by black-body emitters in the Rayleigh-Jeans regime ($`b_\nu \nu ^2`$) with the rate of flux production $`f_{}`$. We also computed CIB fluctuations with the rate of flux production $`f_{}`$ for more realistic SED from Santos et al (2002) which include the Lyman-$`\alpha `$ and free-free emission from the surrounding nebula. Thin and thick dashed colored lines correspond to two possible extremes: SEDs from their Fig. 3 (completely opaque nebula to ionizing photons) and Fig. 5 (completely transparent nebula). Because they do not differ significantly from the more simple SEDs the lines are shown only for some values of $`z_f`$ to avoid overcrowding in the Figure. The graphs show the relative model-independence of the relative CIB fluctuations on the SED for a fixed total CIB flux; the latter contains the bulk of information on the details of Population III emission distribution between various NIR bands. For a given Population III CIB isotropic component, the fluctuations are largest for large values of $`z_f`$ because the duration of the first star era is the smallest. Because of the Lyman continuum absorption there would be no appreciable CIB fluctuations at J band if $`z_f\genfrac{}{}{0pt}{}{_>}{^{}}14`$ (no blue lines in the left panel) and the contribution to the other scenarios will come from $`z13`$, rather than $`z=20`$ when the first star era was assumed to start. This would be broadly consistent with the limits on sky brightness fluctuations at 4 $`\mu `$m from Xu et al (2003).

Both DIRBE and 2MASS data indicate CIB anisotropies at amplitudes larger than the contribution from normal galaxy populations (Kashlinsky & Odenwald 2000a ; Kashlinsky et al (2002)) and are consistent with significant contributions due to Population III. However, because the measured signal contains contributions from remaining galaxies (all galaxies for DIRBE and $`K19`$ galaxies for 2MASS), it is difficult to isolate the contribution from the Population III stars.

## 4 Prospects for measuring CIB from Population III

Population III stars, if massive, should have left a unique and measurable signature in the near-IR CIB anisotropies over angular scales from $`1`$ arcminute to several degrees as Fig. 5 shows. As is the case for measurement of the mean isotropic CIB, detection of these fluctuations depends on the identification and removal of various foreground emission (and noise) contributions: atmosphere (for ground-based measurements), zodiacal light from the Solar system, Galactic cirrus emission, and instrument noise.

The dashed line in Fig. 5 shows the small scale atmospheric fluctuations at 2 $`\mu `$m after one hour of integration of ground based measurement (Odenwald et al (2003)). At large angular scales atmospheric gradients will become important, making measurements there even more difficult. Atmospheric effects can be highly variable on a wide range of time scales, yet they can be completely avoided with space–based experiments. Zodiacal emission from interplanetary dust (IPD) is the brightest foreground at most IR wavelengths over most of the sky. There are some structures in this emission associated with particular asteroid families, comets, and an earth–resonant ring, but these structures tend to be confined to low ecliptic latitudes or otherwise localized. The main IPD cloud is generally modeled with a smooth density distribution. Observationally, intensity fluctuations of the main IPD cloud have been limited to $`<0.2`$% at 25 $`\mu `$m (Abraham et al (1997)). Extrapolating this limit to other wavelengths using the mean high–latitude zodiacal light spectrum yields the limits shown in Figure 5. Because the Earth is moving with respect to (i.e. orbiting within) the IPD cloud, the zodiacal light varies over time. Likewise, any zodiacal light fluctuations will not remain fixed in celestial coordinates. Therefore repeated observations of a field on timescales of weeks to months should be able to distinguish and reject any zodiacal light fluctuations from the invariant Galactic and CIB fluctuations.

Intensity fluctuations of the Galactic foregrounds are perhaps the most difficult to distinguish from those of the CIB. Stellar emission may exhibit structure from binaries, clusters and associations, and from large scale tidal streams ripped from past and present dwarf galaxy satellites of the Milky Way. At mid- to far-IR wavelengths, stellar emission is minimized by virtue of being far out on the Rayleigh–Jeans tail of the stellar spectrum (apart from certain rare classes of dusty stars). At near-IR wavelengths stellar emission is important, but with sufficient sensitivity and angular resolution most Galactic stellar emission, and related structure, can be resolved and removed. IR emission from the ISM (cirrus) is intrinsically diffuse and cannot be resolved. Cirrus emission is known to extend to wavelengths as short as 3 $`\mu `$m. Statistically, the structure of the cirrus emission can be modeled with power–law distributions. Using the mean cirrus spectrum, measurements made in the far-IR can be scaled to 3.5 $`\mu `$m, providing the estimated fluctuation contribution from cirrus that is shown in Figure 5. The extrapolation to shorter wavelengths is highly uncertain, because cirrus (diffuse ISM) emission has not been detected at these wavelengths, and the effects of extinction may become more significant than those of emission, but the cirrus contribution is expected to be several orders of magnitude lower than the CIB fluctuations.

The current detections of CIB anisotropies from DIRBE and 2MASS are above all these foregrounds. The level of anisotropy compares favorably with theoretical expectations and may indeed contain a significant signal from Population III stars. However, the anisotropy may also contain contributions from galaxies made up of Populations II and I stars, which may be significant and uncertain at high $`z`$ because of unknown evolution effects. Hence it is important to be able to remove galaxy contribution in future measurements. Galaxies with normal stellar populations fainter than $`K24`$ contribute little to the CIB. At fainter magnitudes (and larger redshifts) the emission is likely to be dominated by Population III stellar populations and protogalaxies. Because each unit mass of Population III emits a factor of $`10^5`$ more light that the normal (Population I, II) stellar populations, the diffuse flux from (massive) Population III stars would dominate emission from faint normal galaxies (say $`K\genfrac{}{}{0pt}{}{_>}{^{}}24`$). The figure shows that CIB fluctuations from Population III would be the dominant source of diffuse light fluctuations on arcminute and degree scales even if Population III stars epoch was briefer, and their diffuse flux smaller, than the current CIB numbers suggest. Their angular power spectrum should be very different from other sources of diffuse emission and its measurement thus presents a way to actually discover Population III and measure the duration of their era and their spatial distribution. The latter would provide direct information on primordial power spectrum on scales and at epochs that are not easily attainable by conventional surveys. This measurement would be imperative to make and is feasible with the present day space technology.

## 5 Observational requirements

There are several ways in which observations could verify the analysis of this paper. The James Webb Space Telescope (JWST) will be capable of resolving individual Population III objects in their supernova phase, or as young black holes accreting substantial mass flows. Alternatively, if the Population III objects are sufficiently clustered in space and time, the aggregations would resemble proto-galaxies and could be recognized. Observations of these objects are among the foremost objectives of the JWST.

The following would be the optimal set of parameters for an observation designed to map the contribution of the first star era to CIB anisotropies: 1) In order to make certain that the signal is not contaminated by distant galaxies with normal stellar populations, one would need to conduct a deep enough survey in order to identify and eliminate normal galaxies from the field. In practice, as Fig. 1 indicates, going to K$`24`$ would be sufficient. With the current technology this would take $`1.5`$ hours for a 1 meter space telescope. 2) A direct signature of Population III signal is that there should be no CIB fluctuations at wavelengths $`912(1+z_f)^1`$ Å. That spectral drop would provide an indication of the epoch corresponding to the end of first star era. At longer wavelengths the spectral energy distribution of the CIB fluctuations would probe the history of energy emission and its re-distribution by the nearby gas during the first star era. At wavelengths $`\genfrac{}{}{0pt}{}{_>}{^{}}10\mu \mathrm{m}`$ zodiacal light fluctuations may become dominant. 3) On angular scales from a few arcminutes to $`10^{}`$ Population III would produce CIB anisotropies with a distinct and measurable angular spectrum, but its measurement will be limited by the cosmic or sampling variance. If the power spectrum is determined from fraction $`f_{\mathrm{sky}}`$ of the sky by sampling in concentric rings of radius $`q\pi /\theta `$ and width $`\mathrm{\Delta }q`$, the relative uncertainty on $`P_2(q)`$ will be $`(2\pi )^1\frac{\theta }{180^{}}\sqrt{\frac{q}{\mathrm{\Delta }q}}f_{\mathrm{sky}}^{1/2}`$. In order to get accurate and independent measurements, it is necessary to have small $`\mathrm{\Delta }q/q0.050.1`$; thus for reliable results on scales up to $`\theta `$ one would need to cover area a few times larger. Shaded regions in the left panel of Fig. 5 show the one sigma cosmic variance uncertainty with $`\mathrm{\Delta }q/q=0.05`$ for a total of 1, 100 and 1,000 deg<sup>2</sup> areas covered. In order to get reliable results on scales up to $`\theta \genfrac{}{}{0pt}{}{_>}{^{}}1^{}`$ one would need to observe areas of $`\genfrac{}{}{0pt}{}{_>}{^{}}10^{}`$ across.

The black box in Fig. 6 shows what parameters the ideal space mission should have for such a measurement with cross-hatched region in the right panel displaying the magnitude range where Population III stars are expected to dominate CIB anisotropies. For comparison other currently operating or planned NASA missions in the near-IR are also shown. Some of the datasets overlap with the required parameter space, but a large part of the desired parameter space can not be reached with these other data sets.

Direct observations of the CIB fluctuations with the needed fidelity and angular range is not easy. The foreground objects (stars and low-redshift galaxies, and the interstellar medium) are bright and abundant. However, they do not have the same spatial and spectral distributions as the predicted CIB fluctuations. The first observational requirement is to measure the fluctuations as a function of spatial scale and wavelength, with sufficient corroborating evidence to show that the fluctuations are not the residual of some foreground process.

The predicted fluctuations turn down at angular scales greater than subtended by the horizon at decoupling seen at the first star era, and this must be verified. Masking out contributions from individual galaxies requires angular resolutions of the order of 1 arcsec and adequate depth to remove galaxies of K $`\genfrac{}{}{0pt}{}{_<}{^{}}2324`$. Observing fluctuations on the order of 3 degrees in size with reasonable resolution of the spatial scale and reasonable signal-to-noise ratio requires a map of the order of 1000 deg<sup>2</sup> in size, about 1/40 of the whole sky. Taken at face value, we need a map of the order of $`10^{10}`$ pixels, to be built up as a mosaic of exposures with individual detectors and telescope pointings.

There are many technical challenges associated with such a project. Ideally the observations would be taken in space, to avoid the limitations of atmospheric noise, and to enable observations at the full range of wavelengths from 1 to 5 $`\mu `$m. In addition, we would require software to stitch together exposures from different detectors, taken at different times with different telescope orientations, and different amounts of zodiacal light and cosmic ray hits on the detectors, while preserving accurate calibration. It is essential to preserve large-scale photometric accuracy to enable measurements of fluctuations on scales larger than a single field of view (Fixsen et al (2000)). To understand and eliminate the effects of interstellar dust and PAH clouds, it will be necessary to provide photometric bands that maximize the detectability of these sources of interference. In addition, observations over wide ranges of foreground brightness would enable recognition of unexpected effects. Such a project would produce a large database of space observations of low-contrast, extended features, and could lead to unexpected discoveries.

To summarize, the measurement of CIB fluctuations from the Population III star era is imperative to make and is feasible with the present day space technology.


format: text

text:
# The pseudomorphic to bulk fcc phase transition of thin Ni films on Pd(100)

## I Introduction

Heterogeneous epitaxy is a widely exploited technique to fabricate artificial materials, since it allows to introduce a controlled degree of distortion of the interatomic bond length and orientation, which finally allows one to tune the electronic properties of nanostructured devices. In the case of semiconductors, the strain of a film growing on a heterogeneous substrate can be retained up to a thickness of several hundreds of nanometers (coherent growth). Beyond this critical thickness, the strain is released through the formation of a pattern of misfit dislocations, which propagate from the interface to the surface and drive the gradual relaxation (decoherence) of the growing film to its bulk structure. Thanks to the high degree of long range order, the mechanism for semiconductor decoherence can be followed and described in much detail.tsao  While a reduced misfit is required for coherent semiconductor growth, thin artificial phases with a lattice structure much different from the bulk one can be stabilized for metal film growth. In the case of oxide substrates, the decoherence of metal films through and ordered network of misfit dislocations is usually observed when the misfit does not exceed $``$ 10 %.renaud  On the other hand, the metal bonding allows the strain to be released on a much smaller thickness scale, thus reducing the average domain size of the growing film, i.e. the probability of detecting any long range order behaviour. Things are getting more complicated when metal on metal heteroepitaxy is considered, since intermixing phenomena have also to be taken into account, which can either favour the stabilization of pseudomorphic films via surfactant effect (like for the Fe/Au(100) systemopitz ; feau ) or inhibit the coherent growth via substrate roughening and alloying (like for the Co/Cu(111) systemdemiguel ).

In the past ten years, metal heteroepitaxy has been widely applied to study magnetic systems, since the magnetic behavior of metals (both spin orientation and magnetic moment)moroni  and their chemical reactivity can be modified by appropriate distortion of their lattice structure. These metastable artificial phases are decomposed into their ground structural phase when the films exceed a critical thickness of a few layers. These transformations are usually observed to be rather sharp and occur through a rather abrupt non-diffusive distortion mechanism, which is accompanied by a strong morphological reorganization, like for the much studied Fe/Cu(100) system,kalki ; fecu  thus smearing the mechanisms of domain growth.

In fact, most of the studies have been performed by means of LEED, ion scattering and STM, i.e. surface sensitive techniques. The behavior of the interface and of the layers beneath the surface is poorly known and is usually obtained by photoelectron diffraction (XPD) experiments at a Synchrotron facility, where the photoelectron kinetic energy can be effectively tuned to change the penetration depth. On the other hand, XPD data require a rather complex analysis, whose reliability is hampered when the number of scatterers (penetration depth) is increased.fadley  Grazing incidence x-ray diffraction (GIXRD) is certainly the best suited technique to study the structure of a buried interface and the layered structure of thin films.renaud  Recently, a combination of XPD and GIXRD techniques has been applied to study the structural dependence on thickness of Fe films on Cu3Au(100) from a pseudomorphic phase to the bcc one.bruno  The structural transformation has been shown to be characterized by phase coexistence over a thickness range of a few monolayers.

Hereafter, we have applied GIXRD to study the structure of thin Ni films grown on Pd(100). The epitaxial growth of ultrathin Ni films on the Pd(100) surface has been recently studied by means of LEED, XPS and XPD with a laboratory x-ray source.rizzi  This study has shown that in the early stages of the deposition there is the formation of a tetragonally strained face centered (fct) Ni phase with the same lateral lattice spacing of the substrate (i.e. 3.89 Å) and a vertical compression of 0.24 Å. When the film thickness exceeds a critical value of approximately 9-12 layers, the film transforms into its bulk-like Ni fcc structure (lattice parameter of 3.52 Å). The measured strain of the fct phase is found to be in full agreement with the elasticity theory, but some open questions still remain. In particular, although capable to measure very nicely the tetragonal strain adopted by the Ni film, the XPD data did not yield any clear information on how the phase transition develops as the critical thickness is approached nor it was straightforward to extract information on the film/substrate interface. For all these reasons we decided to perform a more detailed study on this system taking advantage of the unique possibilities to acquire both XPS, XPD and GIXRD data offered by the ALOISA beamline at ELETTRA Synchrotron (Trieste Italy).

An effective critical thickness for the pseudomorphic growth has been found. The transformation into the Ni bulk-like structure is shown to involve the interface as well, where the intermixing increases. In addition, the number of layers in the residual pseudomorphic fct phase does not change during the transformation, but simply its domains shrink. The transformation thus proceeds via lateral growth of the bulk-like Ni phase. The increase of the intermixing beyond the critical thickness is attributed to the lateral propagation of the defects, which drive the transformation of the pseudomorphic phase.

## II Experimental

Both electron spectroscopy and X-Ray surface diffraction measurements have been performed in situ at the ALOISA beamline, where a wide photon energy range (130-8000 eV), coupled to a multiple detection system, is available.aloisa  The UHV experimental chamber (base pressure in the 10-11 mBar range) hosts hemispherical electron analyzers and X-Ray detectors. The emission direction from the sample surface can be freely selected for any orientation of the surface. The sample is mounted on a 6–degrees–of–freedom manipulator, specially designed to select with great accuracy (0.01) the orientation of the surface with respect to the incoming photon beam. The temperature of the sample, measured by thermocouples, can be varied by resistive heating and liquid nitrogen cooling.

The Pd(100) substrate was prepared by Ar+ sputtering at 1 keV and annealing to 970 K. The substrate order was checked by RHEED, while XPS surveys at grazing incidence (of the order of the critical angle) were used to check for residual contamination. Nickel was evaporated from a carefully outgassed electron bombardment cell (Omicron) provided with a water cooled shield. A quartz microbalance allowed us to tune the deposition flux at a constant rate of $``$ 0.6 Å/min (10 % accuracy) before deposition. The absolute calibration of the growth rate was determined a posteriori by measuring the x-ray reflectivity (XRR) at fixed scattering angle while scanning the photon energy between 3 and 8 keV. The interference between the x-ray scattering from the substrate-film and film-vacuum interfaces gives rise to maxima and minima as a function of the perpendicular momentum transfer. Fitting to the XRR curves with a simple model of regularly bulk spaced layers, thus yields the film effective thickness (from the position of maxima and minima) and the width of the interfaces (from the amplitude of the oscillation), as shown in Fig. 1.

For each Ni film, we measured both in-plane XRD and XPS from the Pd 3d core level and the valence band (VB), while XPD polar scans from the Ni 2p3/2 were surveyed for a better comparison with previous experiments. The in-plane XRD measurements consist of radial scans across the ($`\overline{2}`$ 0 0) peak in the Pd(100) reciprocal lattice. These measurements were taken scanning the photon energy in a broad range under a suitable $`\theta `$-$`2\theta `$ scattering geometry. The observation of diffraction peaks in radial scans allows us to determine the lateral lattice spacing $`d`$ through the Bragg condition $`2d\mathrm{sin}\theta =hc/E`$. Out-of-plane XRD (rod scans) has been taken for a few selected films in the critical thickness range, to determine the perpendicular distribution of the Ni layer spacings in the pseudomorphic phase. The ($`\overline{2}`$ 0 L) rods of the Pd(100) substrate were taken at a photon energy of 7000 eV with a sampling of $`\mathrm{\Delta }`$L =0.03, up to L =2.2. Rod scan simulations were performed by the Vlieg’s program ROD.vlieg

Both Pd 3d and valence band photoemission spectra were taken at a photon energy of 500 eV with a photon energy resolution of $`125`$ meV. The surface was kept at a grazing angle of 4, in transverse magnetic (i.e. $`p`$) polarization and the electron spectrometer was placed along the surface normal with a kinetic energy resolution of 170 meV. XPD polar scans of the Ni 2p3/2 peak (at h$`\nu `$ = 1270 eV) were measured in the same scattering conditions by rotating the electron analyzer in the scattering plane. We considered emission along the two main symmetry direction $`100`$ and $`110`$ of the substrate unit cell. We followed the procedure of Ref. bruno2,  to extract the anisotropy component from the XPD polar scans by subtracting an isotropic component, which accounts for both geometrical (field of view, illuminated area) and physical (photoemission matrix symmetry, escape depth, surface roughness) factors.

## III Results

### III.1 Photoemission

The Pd 3d XPS data (with an overall energy resolution of about 200 meV) are reported in Fig. 2. The Pd 3d5/2 peak of the clean substrate can be fitted with two components, one corresponding to the bulk peak (335.25 eV) and the other to the surface (334.85 eV) , in agreement with previously reported data.todorova  Upon Ni deposition the surface component is replaced by an interface one (from 5 Å and beyond), which is shifted by 1.0 eV (335.8 eV) from the bulk component, towards higher binding energies, as can be clearly seen in Fig. 2, where the bulk and interface components are well resolved in the 16 Å thickness film. The bulk component disappears after the deposition of 22 Å of Ni.

The intensity variation of the Pd 3d5/2 peak with the film thickness is reported in Fig. 3 (upper panel). The bulk and interface components do not follow the same trend. While the bulk component can be nicely fitted with a simple exponential decay, where the only fitting parameter is the Ni film thickness, i.e. the growth rate, the interface component requires a more complex function with an extra parameter $`\gamma `$, which represents the degree of intermixing between the film and the substrate. It is important to note that the growth rate, as determined from the fitting procedure of the bulk component intensity (0.63$`\pm `$0.07 Å/min), is in full agreement with the one obtained from the reflectivity curves. The increasing weight of the interface component is well represented in Fig. 3(lower panel), where the ratio between the experimental values and the attenuation law, obtained from the bulk component, is reported. According to the figure, the interface component is the dominating one at 16 Å and beyond.

The formation of an intermixed phase already at the beginning of the deposition is also witnessed by the VB photoemission data of Fig. 4, taken just after the deposition of 2.5 Å of Ni. The upper part of the figure shows the difference spectra obtained by subtracting the clean Pd VB spectrum, multiplied by the proper attenuation factor, from the 2.5 Å Ni/Pd(100) spectrum. The result represents the film VB, where the peak at a binding energy of 5 eV cannot be found in the VB of neither pure Ni(100) nor Pd(100). It is worth to remind that the so-called “6 eV satellite” of the Ni 2p spectrum is found shifted to lower binding energies in the 2.5 Å film with respect to the same satellite for a 22 ML thick film.rizzi  Both the VB behaviour and the shift to higher binding energy of the Pd 3d5/2 core level are the fingerprint of the intermixing process at the Ni/Pd interface, i.e. to the formation of a NiPd alloy in agreement with literature data.hillebrecht

From the structural point of view, the intermixing at the interface determines an enhanced pseudomorphism at the early stages of Ni deposition. This can be observed from the thickness dependence of the forward scattering peaks originated by focussing from close-compact atom row directions in Ni 2p3/2 XPD polar scans, as shown in Fig. 5. At 2.5 Å, the fcc characteristic peaks are closer to the nominal fcc position (at 45 and 54.7 from the surface normal) than at higher thickness. By increasing the film thickness, the forward scattering peaks shift away from the surface normal, indicating an increase of the vertical compression due to the elastic strain. The strain is released beyond 16 Å by the transformation into the bulk-like Ni structure, in full agreement with previous XPD studies.rizzi

### III.2 X-ray diffraction

The Ni film transformation from the pseudomorphic fct phase to the bulk-like one does not occur through a continuous relaxation of the strained lattice cell, rather domains of bulk-like symmetry are formed beyond 16 Å, which grow in size as the thickness is increased. This transformation is clearly seen in Fig. 6, where in-plane radial scans across the substrate ($`\overline{2}`$ 0 0) XRD peak are shown for a few film thicknesses. Besides the substrate peak, a new feature appears at a thickness of 16 Å, corresponding to a lattice spacing of $`3.65`$ Å. This feature evolves shortly into a well defined peak (see scan at 22 Å) which gradually shifts towards the 3.52 Å lattice parameter of fcc Ni. The appearance of the Ni bulk-like peak at $`3.65`$ Å is the fingerprint of a structural phase transition.

For a better understanding of the structural transformation, we have studied the layer spacing distribution in the pseudomorphic fct Ni film. The XRD ($`\overline{2}`$ 0 L) rod scans are shown in Fig. 7 for a few films in the range of the critical thickness of 12-16 Å. The XRD scan along the substrate peak rod puts in evidence the x-ray scattering interference between the Ni pseudomorphic layers which are confined between the film-substrate and film-vacuum interfaces. If the deposition is homogeneous on the substrate, well defined interference oscillations can be seen along the rod scans, as in the case of the 8 and 12 Å film thickness. The number of maxima and minima and their position is related to the number of Ni layers in the pseudomorphic structure, while the amplitude of the oscillations to the sharpness of the Ni film interfaces (the larger is the amplitude the sharper is the interface). The increased number of maxima and minima from the 8 Å film to the 12 Å one is thus reflecting the increased number of Ni layers in the pseudomorphic structure. The rod scan taken at 18 Å, where the Ni film structural transition has already started, is still showing a few faint modulations indicating that residual domains of the pseudomorphic phase are still co-existing with the fcc Ni phase. Most strikingly, the maxima and minima of the 18 Å phase still occur at the same perpendicular momentum transfer of the 12 Å film, i.e. the residual domains of the pseudomorphic phase contain the same number of Ni layers. The strong damping of the maxima and minima amplitude indicates both an increase of the pseudomorphic fct phase roughness and the deprival of the pseudomorphic Ni layers due to the shrinking of the corresponding domains. At the thickness of 22 Å, the whole film has been transformed into the Ni bulk-like phase and the rod scan displays a structureless smooth behavior, which is characteristic of a bulk-truncated crystal surface.

The layer spacings and fillings for the 8 and 12 Å films have been obtained by fitting the rod scans with the structural model reported in Table 1. Due to the large number of fitting parameters, we have fixed the inner layer spacings to the value determined by PED analysis after Ref. rizzi, , and we focussed our attention to the substrate-film and film-vacuum interfaces, where XRD yields the best sensitivity. With these constraints, we have found that the topmost layer is also compressed, in excellent agreement with previous XPD studies,rizzi  while the layers close to the film-substrate interface are expanded, confirming the vertical pseudomorphism indicated by the present XPD scan on very thin Ni films (Fig. 5). Concerning the buried interface, we admitted Ni/Pd intermixing for two layers. While this model yields an excellent fitting for the thinnest film, a larger number of layers might be affected by the intermixing in the 12 Å film, as indicated by the incomplete layer filling of a few buried Ni layers (3rd to 5th) with respect to the intermediate ones. Alternatively, this finding could be the fingerprint of the formation of extended morphological defects at the Ni-Pd interface, when the critical thickness is achieved.

## IV Discussion

The evolution of the Ni/Pd(100) film, as a function of the thickness, is described by the following sequence. In the early deposition stage a couple of intermixed layers are formed with strict pseudomorphic structure. Further deposition leads to the formation of strained layers whose lattice cell is pseudomorphic to the lateral substrate lattice, but presents a perpendicular compression in agreement with the elastic force constant model. This elastically strained structure builds up to a critical thickness of 12-16 Å, corresponding to a maximum of 10 layers (including at least 2 intermixed layers at the substrate-film interface), not all of them equally occupied. Beyond this thickness, domains of bulk-like structure are formed and the whole film structure is gradually changed through a first order phase transition. Phase co-existence is clearly observed up to 18 Å. The strain release at the phase transition is not complete and the bulk-like phase gradually relaxes to the orthomorphic fcc phase with increasing thickness.

The formation of a few deposit layers with a full pseudomorphic structure (as indicated by XPD scan in Fig. 5 and rod scan analysis in table 1) was also observed for very thin films (2-3 monolayers) of Fe on Cu3Au(100) bruno ; lin  and Ni on Cu(100).mueller  The highly strained structure of these layers is probably stabilized by the intermixing and might be a general behavior of metal heteroepitaxy, whenever alloying or surface segregation is chemically favoured. In the present system and before the phase transition, the degree of intermixing remains constant, i.e. the concentration of substrate atoms is much smaller in the next deposited layers. From the 3rd layer on, a compressed vertical spacing is established, in agreement with the value predicted by the elastic theory for the given in-plane expansion, dictated by the substrate lattice.

The sequence of rod scans in Fig. 7 clearly shows that there exists a maximum number of Ni layers that can be stabilized into a pseudomorphic structure (10 layers, included the intermixed ones), thus defining an effective critical thickness for the structural phase transition. This configuration is established at a bulk equivalent thickness of 12 Å. The fact that the maximum number of layers with pseudomorphic fct structure does not change throughout the transition, but simply the fct domains decrease their homogeneity and size, indicates that the transition takes place through the lateral growth of the Ni bulk-like domains at the expense of the pseudomorphic fct phase. Thus the Ni bulk-like domains are not floating on top of the pseudomorphic fct phase nor the transition simply proceeds from top to the bottom, rather, when formed, the Ni bulk-like domains involve locally all the film layers, down to the Ni/Pd interface. A possible model for the Ni bulk-like domains could be that of wedges, with the apex at the substrate-film interface, which expand at the expense of the pseudomorphic phase. Since the phase transition involves three-dimensional domains, it must be of the first order type. No time evolution of the diffracted peaks has been observed at room temperature on the time scale of the experiments (a few hours for the rod scans), which indicates that the transition is kinetically slowed down by the film defects.

At the critical thickness, the intermixing at the Ni/Pd interface (almost constant up to the critical thickness) increases strongly (as indicated by XPS analysis in Fig. 3). It is very tempting to associate the increase of the intermixing with the propagation of a defect from the Ni/Pd interface (whose early formation might be witnessed by the incomplete layer filling of the buried Ni layers at the critical thickness), which drives the transformation of the pseudomorphic fct phase. The Ni/Pd lattice mismatch of $``$ 10 %, although not so small, might still allow the formation of an ordered pattern of misfit dislocations originated by the stacking faults at the interface, which would yield characteristic satellites of the Bragg’s peaks in the radial scans.renaud  While we have not checked by in-plane XRD for these feature on non-equivalent diffraction peaks other than the ($`\overline{2}`$ 0 0) one, LEED pictures taken at the critical thickness were reported to display a Moiré pattern with $`(10\times 10)`$ periodicity.rizzi  These patterns clearly show one order of extra spots decorating the integer peaks along the $`011`$ substrate symmetry directions, i.e. the direction of close-compact atom rows on the fcc(100) surface. From comparison with the present data (in particular with the intermixing behaviour), we can say that the strain release indicated by the extra spots is not limited to the Ni film surface, rather the Moiré pattern is originated by defects extending down to the substrate. The Ni/Pd(100) system, where the Ni film undergoes a structural transition between two phases with the same face centered (100) surface symmetry, resembles the behavior of the Fe/Cu(100) system, where a more dramatic structural change, from an fcc(100) to a bcc(110) phase, takes place. In the latter case, the transition of the Fe film was described through the formation of shear planes (from the film surface down to the substrate) along close-compact atom rows, which separate domains of different structural phase, like for a martensitic phase transition.kalki

Concerning the growth of the newly formed bulk-like Ni domains, a mechanism like that driving the decoherence in semiconductor heteroepitaxy can be envisaged. The domain walls, either shear planes or misfit dislocations, propagate laterally on the Pd substrate, leaving behind a strongly intermixed region. This picture is fully consistent with the increase of the Ni/Pd intermixing, which is observed to continue beyond the critical thickness (as indicated both by XPS analysis and by the Ni/Pd interface width obtained by the XRR analysis, Fig. 1)

Finally the newly formed bulk-like Ni film is still strained at small thickness (see radial scan at 22 Å in Fig. 6) and the relaxation to its bulk fcc structure proceeds gradually with increasing thickness. This gradual relaxation, witnessed by the radial scans of the in-plane lattice parameters, is also seen in the perpendicular layered structure of the film. In fact the simple bulk structural models used to simulate the XRR energy scans yields a fitting quality which clearly improves from the 22 to 30 Å film (see Fig. 1). Such a behavior is not surprising, since it has been observed for other metal films. As an example, the bulk structure of Fe deposited on Cu3Au(100) (where the 7% lattice mismatch is even smaller than the present one) is not fully recovered even for film thickness of the order of hundred of monolayers.rochow ; schirmer

## V Conclusions

We studied the growth of Ni on Pd(100) by XPS (both core levels and VB), XPD, XRR and XRD (both in- and out-of-plane) techniques. In particular, we followed the structural evolution of the Ni films as a function of the thickness. After the formation of a couple of intermixed layers, (which preserve a perpendicular spacing close to the substrate one) a laterally pseudomorphic phase, with a perpendicular strain in agreement with the elastic theory, takes place. This pseudomorphic fct structure is stable up to 10 layers. Further Ni deposition leads to a gradual structural transformation of the whole film into a Ni bulk-like fcc phase. This phase transition, accompanied by a strong increase of intermixing at the Ni/Pd interface, proceeds through the lateral growth of the Ni bulk-like domains at the expense of the pseudomorphic fct phase. The latter domains preserve their layered structure (maximum number of layers and corresponding spacings), while shrinking. Residual strain is still observed in the Ni bulk-like phase at a thickness of 30 Å.