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# Cluster Beam Deposition and in situ Characterization of Carbyne-rich Carbon Films

## Abstract

Nanostructured carbon films produced by supersonic cluster beam deposition have been studied by in situ Raman spectroscopy. Raman spectra show the formation of a sp2 solid with a very large fraction of sp-coordinated carbyne species showing a long-term stability under ultra high vacuum. Distinct Raman contribution from polyyne and cumulene species have been observed. The long-term stability and the behavior of carbyne-rich films under different gas exposure have been characterized showing different evolution for different sp configurations. Our experiments confirm theoretical predictions and demonstrate the possibility of easily producing a stable carbyne-rich pure carbon solid. The stability of the sp2-sp network has important implications for astrophysics and for the production of novel carbon-based systems.

Linear carbon chains with sp hybridization are considered as fundamental constituents of the interstellar medium bib1 ; bib2 . They are abundant in circumstellar shells bib1  and their presence can account for many features of the diffuse interstellar bands bib1 ; bib2 . The efforts to synthesise and study in laboratory these species has stimulated the discovery of C60 bib3 . Several gas-phase studies of carbon clusters with linear or cyclic structure have suggested that they can be elemental building blocks of three-dimensional fullerenes and nanotubes bib4 .

Sp carbon chains can present alternating single and triple bonds (polyyne) or only double bonds (polycumulene) bib5 . Theoretical calculations suggest that polycumulenes are less stable than polyynes bib5 ; bib6 . Both species are characterized by an extremely high reactivity against oxygen and a strong tendency to interchain crosslinking bib7 , thus rendering the direct observation of a pure carbyne-assembled solid still a major challenge. Isolated carbynic species have been investigated in the gas phase in order to determine their geometry bib4 ; bib8 ; their electronic and vibrational structure has been studied for non-interacting clusters embedded in matrices of cold rare gases bib9 .

Sp carbon chains have also been proposed as the elemental building blocks of a carbon allotrope called carbyne bib7 . Carbyne story is very controversial: the first claims of direct observation of carbyne date back from the sixties bib10 ; bib7  however, up to now, no firm and unambiguous evidence of the existence of this allotrope has been provided bib7 . Experimental results, mainly based on crystallographic recognition supporting the identification of crystalline carbyne, have been object of strong criticism up to a complete rejection of the carbyne concept bib7 ; bib11 .

Although the occurrence of crystalline carbyne is still matter of debate, carbyne-rich or carbynoid solids have been produced by synthetic strategies mainly based on chemical routes. These include oxidative coupling reactions, dehydrohalogenation of polymers, polycondensation reactions of halides, electrochemical reductive carbonization, condensation of end-capped chain molecules produced in the gas-phase bib12 ; bib13 ; bib14 ; bib15 . In these systems polyyne chains, assembled together, are preserved against crosslinking and chemical decomposition by the presence of metal-based species and molecular groups terminating and separating the chains.

A different approach to the synthesis of carbyne is the high temperatures and high-pressure treatment of carbon-based materials. Resistive heating of graphite, high-energy laser or ion irradiation of carbon have been suggested as possible methods to produce carbynoid materials bib16 . However no definitive confirmation of the validity of these methods has been reported so far.

Raman spectroscopy is one of the techniques of choice for the study of carbon-based materials and for the identification of carbyne bib7 ; bib17 . The presence of a Raman band at roughly 2100 cm-1, generated by the carbon triple bond is admitted to be one of the strongest arguments in favour of the presence of carbynes bib7 ; bib14 . Raman spectra of carbynoid materials are characterized by G and D bands in the 1200-1700 cm-1 range as in amorphous carbon and by the presence of the band in the 2100 cm-1 region bib7 ; bib14 . For carbyne-rich materials this band should have an intensity comparable or even greater than the amorphous contribution.

Raman spectra from chemically stabilized carbynoid systems are reported in literature, due to the high reactivity and fast ageing of the carbyne species, no Raman spectra are reported for pure carbon systems.

In this Letter we show that it is possible to produce nanostructured carbon films rich of carbyne species by depositing pure carbon clusters from a supersonic beam. We have characterized these films by in situ Raman spectroscopy determining the contribution to the spectra coming from the polyyne and cumulene species. We have also studied the ageing of the film and the effect of different gas exposure.

The deposition of carbon clusters was performed by means of an UHV cluster beam apparatus (CLARA, cluster assembling roaming apparatus) described in detail in bib18 . Cluster beams are generated by a pulsed microplasma cluster source (PMCS) bib19 . Cluster mass distribution is monitored prior to deposition by a reflectron time-of-flight mass spectrometer. Cluster mass distribution is peaked around 600 atoms per cluster and it extends up to several thousands atoms per cluster. Cluster kinetic energy is roughly 0.3 eV/atom so that the deposition occurs in the low energy regime, in which negligible fragmentation of clusters takes place. In previous works we have demonstrated that low-energy carbon cluster deposition allow the production of nanostructured films retaining the memory of the precursor clusters bib20 ; bib21 .

In order to perform both the synthesis and the analysis of the films under UHV conditions, we have connected CLARA with a small chamber equipped with a substrate holder capable of 3-axis translation and rotation around vertical axis. Nanostructured carbon films with a thickness of 200 nm were grown on a silicon substrate at room temperature. After the deposition the sample was positioned (by $`90^{}`$ rotation) in front of a fused quartz viewport. Raman measurements in back-scattering geometry have been performed in situ with a Jobin-Yvon T64000 spectrometer, in triple grating configuration (1800 gr/mm gratings) and with the 532 nm line of a frequency doubled Nd-Yag Coherent DPSS 532 laser. The detector was a liquid nitrogen cooled CCD camera. The instrument spectral resolution is below 3 cm-1.

Cluster-assembled carbon films have been previously characterized ex situ by Raman spectroscopy bib21 . The films have an amorphous structure with a main sp2 hybridization character. The G and D features reveal a substantial amount of distortion of bond lengths and angles bib22 . A weak peak at about 2100 cm-1 was observed. Due to the high reactivity of carbyne this peak could be attributed to a residual presence of a primeval larger carbynoid population. Although a definitive attribution based solely on ex situ data cannot be considered as definitive.

Figure 1 shows the comparison between the ex situ and in situ Raman spectra of two films deposited in the same conditions. G and D bands are almost identical whereas the peak at 2100 cm-1 has dramatically increased in intensity in the in situ spectrum (we will refer to it as “C” peak). This peak has a remarkably strong intensity and appears to be structured and composed of a main broad peak at about 2100 cm-1 and a weaker shoulder centered around 1980 cm-1, as evidenced by a two-gaussian fit (see Fig. 1). The relative C peak intensity, expressed by the ratio between its integrated intensity and the D-G band integrated intensity ($`I_{Crel}=I_C/I_{D,G}`$) is roughly 45%.

Raman spectra confirm the formation, of a carbynoid material with a substantial presence of sp linear structures among a sp2 hybridized disordered network, although it is not possible to quantify the amount of sp hybridized C atoms, since the Raman cross section of this kind of vibrations is unknown. Compared to other carbynoid systems reported in literature bib7 , the C peak at 2100 cm-1 presents a low-frequency shoulder at 1980 cm-1. This is caused by the presence of both cumulenic and polyynic chains coexisting in the film and giving spectral contributions at different frequencies bib23 . The broadening of the two components can be ascribed to the sp chain length distribution and to disorder bib7 .

These observations show that a carbyne-rich material can be formed by assembling carbon clusters at very low energies without high temperature and high pressure or chemical reactions inducing carbyne formation from polymers or hydrocarbons.

We have studied the carbynoid material stability through the evolution of the C peak intensity, keeping the sample in UHV for several days (at a pressure of about $`210^9`$ Torr) and collecting Raman spectra at fixed time intervals (Fig. 2). We observed a slow decrease of the intensity of both the two components of the C peak. Again no evident changes in the shape of G and D bands has been observed. This allows us to study the C peak intensity evolution by means of the previously defined integrated intensity ratio $`I_{Crel}`$. It is also reasonable to assume a relationship between the intensity of the carbyne peaks and their concentration, even though it is not possible to make a quantitative evaluation.

The temporal evolution of I$`_{Crel}`$ is well described by an exponential decay plus a constant (Fig. 3). This provides an estimate of the characteristic decay time constant and of the residual non-reacted fraction of carbynes. The sample kept in UHV showed a characteristic decay time of the order of 22 hours, resulting in a reduction of I$`_{Crel}`$ to a 29% of the as-deposited value. It is worth noting that this residual intensity is almost one order of magnitude greater than the intensity measured in ex situ samples, and that it remains stable even after 18 days from the deposition. In addition, the relative stability of D and G bands reveals that the amorphous structure is not significantly affected by the changes and rearrangements occurring to the carbynoid component.

This observation addresses a very important and unexpected point concerning carbyne stability: in our cluster-assembled films polyyne and cumulene species survive the soft landing and are stabilized in a pure carbon environment. The carbyne interaction with other types of clusters is such that after a spontaneous degradation, probably due to crosslinking, the amount of carbynoid species remains quantitatively very high and constant.

The introduction of dry air into the deposition chamber strongly modifies the Raman spectrum as shown in Fig. 4. As in the UHV experiment we have collected several Raman spectra as a function of exposure time of the film to the gas. We observed a fast decrease of the C peak intensity, (see Fig. 3) with a decay time constant of 35 minutes and a residual intensity of 3.6%, comparable with what observed in ex situ measurements bib21 . The two components of the C peak behave differently under dry air exposure. After several decay times a two gaussian fit shows the complete disappearance of the lower frequency peak generated by the cumulene fraction. This indicates a more pronounced stability of the polyyne configuration against oxygen exposure, confirming the theoretical predictions bib7 ; bib23 . At the same time we have observed a 20 cm-1 blue shift of the position of the two peaks. According to Akagi et al. bib24 , the frequency of carbynic Raman peaks has an inverse dependence on the number of carbon atoms composing the chain. This behaviour suggests the attribution of the observed blue shift to a decrease in the average chain length of the deposited carbynes. Remarkably there was no clear evidence for a similar shift in UHV experiments.

In order to further clarify the role of oxygen, we have repeated the measurements exposing a film to 500 mbar of pure nitrogen (N2). We have observed an intermediate behavior for both the decay time and the residual intensity in comparison with the UHV and dry air behavior. A blue shift of about 10 cm-1 was also observed, but no disappearance of the cumulene peak took place.

The experimental results reported here provide new elements for the interpretation of the carbyne puzzle and are of relevance for areas where carbon clusters play an important role such as the composition of the interstellar medium and the existence of new allotropic forms of carbon. Low energy cluster beam deposition in an oxygen free environment appears to be a viable technique for the production of a pure carbon nanostructured material extremely rich of carbynoid species. The unexpected high stability of polyyne and cumulene species interacting with each other and with fullerene-like type of clusters once deposited bib20 , suggest the existence of cluster-cluster reaction mechanism leading to the formation of networks where the sp bondings are stabilized. These networks composed by sp2 and sp linkages may be a disordered analogue of a new phase of carbon called graphyne and theoretically predicted by Baughman et al. bib25 . The doping of this material with alkali metals or stabilising molecular groups may lead to observation of novel structural and functional properties in these systems.

The gas-phase chemical models of interstellar clouds take into account the presence of different carbon nanoparticles such as carbyne, fullerenes, polycyclic aromatic hydrocarbons etc. bib1 ; bib26 . These species are related by very complex reaction pathways to produce and destroy one species from the others. Our observations suggest that cluster-cluster interaction can produce large carbonaceous grains where carbyne species are present and stable.

In conclusion, we have characterized by in situ Raman spectroscopy nanostructured carbon films produced by supersonic cluster beam deposition in UHV conditions. Raman spectra show the presence of a large quantity of polyyne and polycumulene moieties in the films, giving origin to peaks at 2100 cm-1 and 1980 cm-1 respectively. The carbyne species are substantially stable in an oxygen free environment. We have characterized carbyne reactivity as a function of time in UHV and in the presence of dry air and nitrogen showing that oxygen almost completely destroys the carbyne fraction of the films. We have demonstrated that polycumulenes are less stable against oxygen compared to polyynes. The decay kinetics of the carbynoids exposed to gas gives information about the chemical and thermodynamical nature of the degradation processes. We have shown that sp carbon clusters can be assembled and stabilized at room temperature in a pure carbon environment allowing the spectroscopic characterization of different type of bondings. Moreover we have demonstrated the usefulness of in situ Raman spectroscopy for the study of nanostructured carbon. Our experiments open new perspectives for the production and the study of the long-sought sp carbon allotropes.


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# Conductance through a One-Dimensional Correlated System: Relation to Persistent Currents and Role of the Contacts

(July 25, 2002)

## Abstract

Based on a recent proposal \[O.P. Sushkov, Phys. Rev. B 64, 155319 (2001)\], we relate the quantum conductance through a sample in which electrons are strongly correlated to the persistent current of a large ring, composed of the sample and a non-interacting lead. A scaling law in the lead length allows to extrapolate to a well-defined value of the conductance, depending only on intrinsic properties of the sample and the nature of the contacts between the sample and the lead. For strongly disordered samples, the conductance is found to be enhanced by the interaction.

Viewing quantum transport as a scattering problem Landauer57 ; Buttiker86  generated a new understanding of the electronic conductance. This approach is able to explain a wealth of experimental results Imry  in mesoscopic systems when electron-electron (e-e) correlations are not important. To include these correlations is non-trivial and remains one of the major challenges in the field (see e.g. Zotos ). While none of the proposals to calculate the conductance for a correlated system is well suited for numerical calculations meir ; pastawski  or free of certain assumptions berkovits , such an issue becomes crucial in present day’s research exploring electronic transport through nanosystems (carbon nanotubes nanotubes , molecules molecular\_electronics , and point contacts sushkov ), where the Coulomb repulsion leads to important correlations.

Reservoirs and leads are key elements in the scattering approach, and possess very clear physical meanings since the measurement is made with electrodes which behave as electron reservoirs. In a good electrode, the electron density $`n_e`$ is large, the ratio $`r_s`$ between Coulomb and Fermi energy is small, hence the e-e interaction is negligible. In contrast, $`n_e`$ in a nanosample can be very small, yielding a large ratio $`r_s`$ and important e-e correlations.

The dimensionless conductance $`g`$ does not only depend on the intrinsic properties of the sample, but also on the way it is connected to the electrodes. The quality of the contacts is particularly important for correlated electrons. For a clean Luttinger liquid attached to non-interacting leads through reflectionless contacts, it has been found safi  that the interactions do not influence $`g`$. In the other extreme, if the contacts are tunnel barriers, the interactions lead to Coulomb blockade kouwenhoven , thereby dominating $`g`$. In carbon nanotubes, various transport regimes are observed depending on the nature of the contacts nanotubes .

As shown by Kohn kohn  and Thouless Thouless , $`g`$ is also related to the sensitivity of the sample’s eigenstates to a change of the boundary conditions. This sensitivity can be tested by closing a system to a ring and measuring the persistent current as the response to an enclosed magnetic flux $`\varphi `$. At zero temperature, the persistent current is given by $`J=E/\varphi `$, where $`E`$ is the ground state energy of the many-body system. Interactions play an important role for $`J`$, and it is generally accepted that they account for the large difference between experiments and one-particle calculations reviewpercurr . There have been various attempts shastry ; berkovits  to link $`J`$ and $`g`$ for an interacting ring. However, the ring built from the sample itself does not contain any reservoirs in which energy relaxation can take place. Negative zero-frequency conductivities occur fye , unlike in the dissipative case in which we are interested here.

As pointed out in Refs. meir ; sushkov , at zero temperature, not only for the non-interacting case, but also for correlated samples, $`g`$ is given by $`|t(E_F)|^2`$, the probability for an electron at the Fermi energy $`E_F`$ to be elastically transmitted through the sample. Moreover, if one replaces the massive electrodes (with negligible e-e correlations) used in a real measurement by very long non-interacting one-dimensional leads, one can expect that they have a similar effect pastawski . Sushkov recently proposed sushkov  that $`|t(E_F)|^2`$ can be extracted from the persistent current of a much larger ring, composed of the sample itself, together with a long lead closing the system. This has the considerable advantage that a ground state property ($`J`$) suffices to determine $`g`$. However, one needs the $`J`$ of the combined system (sample plus lead), and not the one of the system alone as in previous works berkovits ; Thouless ; shastry ; kohn .

In the following, we adapt the approach of Ref. sushkov  to calculate $`g`$ for one-dimensional interacting electrons using the Density Matrix Renormalization Group (DMRG) algorithm white ; peter . We check that a scaling law allows to extrapolate to an infinite lead, yielding $`g`$ as a property of the sample and the way it is connected to the lead. The nature of the contacts turns out to play a major role. Then, we extend our analysis to disordered samples, where we find that, similarly to the case of persistent currents sjwp , repulsive interactions may increase $`g`$ for strong disorder.

We first present an alternative derivation of Sushkov’s result sushkov , pointing out the main assumptions, for the non-interacting case. As depicted in the upper inset of Fig. 1, we consider a sample (S, hashed region) closed to a ring by a non-interacting and disorder-free lead (L), and threaded by a flux $`\varphi `$. The total length $`L=L_\mathrm{S}+L_\mathrm{L}`$ consists of the sample length $`L_\mathrm{S}`$ and the lead length $`L_\mathrm{L}`$. The one-particle eigenstates of the total system satisfy

$$\mathrm{det}(IM_\mathrm{S}M_\mathrm{L})=0,$$
(1)
with the transfer matrices of the sample and the lead

$$\begin{array}{ccc}\hfill M_\mathrm{S}& =& \frac{1}{\mathrm{sin}\phi }\left(\begin{array}{cc}e^{i\alpha }/\mathrm{sin}\theta & i\mathrm{cot}\theta +\mathrm{cos}\phi \\ i\mathrm{cot}\theta +\mathrm{cos}\phi & e^{i\alpha }/\mathrm{sin}\theta \end{array}\right)\hfill \\ \hfill M_\mathrm{L}& =& e^{i\mathrm{\Phi }}\left(\begin{array}{cc}e^{ikL_\mathrm{L}}& 0\\ 0& e^{ikL_\mathrm{L}}\end{array}\right),\hfill \end{array}$$
(2)
respectively. Here, $`\mathrm{\Phi }=2\pi \varphi /\varphi _0`$ where $`\varphi _0`$ is the flux quantum. The scattering is characterized by the angle $`\theta `$, the phase-shift $`\alpha `$, and the angle $`\phi `$ (equal to $`\pi /2`$ if right-left symmetry is respected). These angles are functions of $`k`$, the wave-vector in the lead. The transmission amplitude is given by $`t=e^{i\alpha }\mathrm{sin}\theta \mathrm{sin}\phi `$. With (2), the quantizing condition (1) can then be written as

$$\mathrm{cos}\mathrm{\Phi }=\frac{1}{|t|}\mathrm{cos}(kL+\delta \alpha ),$$
(3)
with the relative phase-shift $`\delta \alpha =\alpha kL_\mathrm{S}`$. The persistent current carried by a one-particle state (with energy $`ϵ`$) is $`j(\varphi )=(ϵ/k)(\varphi /k)^1`$. We work at $`\mathrm{\Phi }=\pi /2`$ and establish two crucial assumptions: i) $`|(\delta \alpha )/k|L`$; ii) $`ϵ/k\mathrm{}^2k/m`$. The first one states that the Wigner time associated with the scattering region is negligible compared with the time spent in the leads. Notice that we work with a relative Wigner time $`\tau _W=(m/\mathrm{}^2k)(\delta \alpha )/k`$, that is, the difference between the delay time of the scattering region and that of a potential-free region having the same length. The second assumption implies that the dispersion relation is essentially unaffected by the scattering potential.

The persistent current of $`N`$ non-interacting spinless fermions (for simplicity we take $`N`$ even) is given by riedel

$$J(\mathrm{\Phi }=\pi /2)=\frac{e\mathrm{}}{mL}k_F|t(k_F)|.$$
(4)
Denoting by $`J^0`$ the persistent current of a clean ring of length $`L`$, the conductance may be expressed as sushkov

$$g=\underset{L_\mathrm{L}\mathrm{}}{lim}\left(\frac{J(\pi /2)}{J^0(\pi /2)}\right)^2.$$
(5)
With interaction stafford , assumptions i) and ii) always hold in the large $`L`$ limit. Moreover, the use of Eq. (5) implies that the one-particle states of the correlated system can still be indexed by the lead wave-vectors $`k`$. That is, adding an infinite non-interacting lead to a finite non Fermi-liquid sample restores the Fermi-liquid behavior. This assumption, which has been used in the perturbative calculation of transport through Hubbard chains connected to reservoirs oguri , requires that the interactions are completely switched off in the one dimensional lead. Otherwise the Luttinger liquid behavior kane\_fisher  sets in, and one cannot obtain a result which is independent of the length of the auxiliary lead. In this, our approach differs from Sushkov’s, where the interactions in the lead are kept (within the Hartree-Fock approximation).

Eq. (5) allows to calculate $`g`$ from ground-state energies. We do this for spinless fermions (polarized electrons) in a ring described by the Hamiltonian

$$H=\underset{i=1}{\overset{L}{}}(c_i^{}c_{i1}+c_{i1}^{}c_i)+\underset{i=2}{\overset{L_\mathrm{S}}{}}U\left[n_i\frac{1}{2}\right]\left[n_{i1}\frac{1}{2}\right]$$
(6)
where $`c_i`$ ($`c_i^{}`$) is the annihilation (creation) operator at site $`i`$, $`n_i=c_i^{}c_i`$ the number operator, and the flux-dependent boundary condition enters through $`c_0=\mathrm{exp}(i\mathrm{\Phi })c_L`$. The interaction is restricted to nearest neighbors and effective in the sample, but vanishing in the lead. It is equilibrated by a compensating potential that prevents the particles from emptying the interacting region. The form of the Hamiltonian allows to have particle-hole symmetry at half filling. We work with a number of fermions $`N=L/2`$, such that the mean density is always $`1/2`$ independently of $`L_\mathrm{S}`$ and $`L_\mathrm{L}`$.

Using the DMRG algorithm as described in Ref. peter , we calculate the ground-state energies $`E(\mathrm{\Phi })`$ at $`\mathrm{\Phi }=0`$ and $`\mathrm{\Phi }=\pi `$, to obtain the stiffness $`D=(L/2)|E(0)E(\pi )|`$ (which is simpler to calculate than $`J`$). When the flux-dependence of the ground-state energy is sinusoidal, which is the case in one-dimensional localized systems, $`D`$ is directly proportional to the maximum $`J`$. We will use such an identification to calculate $`g`$ from Eq. (5), taking $`D`$ instead of $`J`$ stafford .

An obvious requirement for Eq. (5) to be useful is that the resulting $`g`$ should be independent of $`L_\mathrm{L}`$, since the lead is an auxiliary element of the procedure. Therefore, the first numerical step is to compute $`D`$ for increasing $`L_\mathrm{L}`$ with given $`L_\mathrm{S}`$ and $`U`$ (Fig. 1). We find a very clear asymptotic behavior, described by the scaling law

$$D(U,L_\mathrm{S},L_\mathrm{L})=D_{\mathrm{}}(U,L_\mathrm{S})\mathrm{exp}\left(\frac{C(U,L_\mathrm{S})}{L}\right),$$
(7)
where the intrinsic value $`D_{\mathrm{}}`$ is independent of the length of the auxiliary lead. This asymptotic value $`D_{\mathrm{}}`$ is then used to determine the conductance as $`g=(D_{\mathrm{}}/D_{\mathrm{}}^0)^2`$, where $`D_{\mathrm{}}^0`$ corresponds to the clean non-interacting ring. The sign of $`C`$ tau\_W  depends on the parity of the number of sites $`L_\mathrm{S}`$ in the sample: $`C>0`$ for even $`L_\mathrm{S}`$ (filled symbols) and $`C<0`$ for odd $`L_\mathrm{S}`$ (open symbols).

The method also works for non-polarized electrons (Hubbard model with on-site interaction), and the size-scaling again allows to obtain intrinsic values (lower inset in Fig. 1). In the sequel we concentrate on the spinless case (Hamiltonian (6)), which contains the main features we are interested in, and allows to reach larger samples.

Having verified the consistency of our approach, we now study the systems of interest. In Fig. 2 we present the conductance, as a function of $`U`$, for various sample lengths $`L_\mathrm{S}`$. One observes a monotonic decrease with increasing $`U`$, and a very clear even-odd asymmetry according to the parity of $`L_\mathrm{S}`$. Samples with odd $`L_\mathrm{S}`$ exhibit almost perfect transmission up to large values of $`U`$, while an even $`L_\mathrm{S}`$ results in a decrease of $`g(U)`$ already at weak interaction. For odd $`L_\mathrm{S}`$, particle hole symmetry leads to degenerate sample configurations with $`(L_\mathrm{S}\pm 1)/2`$ particles in the interacting region. This is similar to a Coulomb blockade resonance. The traveling particle can thus become trapped for a long time ($`\tau _W>0`$), consistent with negative $`C`$ tau\_W . Since the two configurations are coupled by processes which transfer particles through the interacting sample, one obtains perfect transmission, as in the perturbative treatment of Ref. oguri .

On the other hand, an even number of sites implies that the transport of one particle through the sample takes place via a virtual state with an energy of order $`U`$ above the ground-state. Thus, no resonance can be expected and the transmission, which is suppressed already by moderate $`U`$, is a fast process with $`\tau _W<0`$, consistent with $`C>0`$. In addition, increasing $`L_\mathrm{S}`$ reduces $`g`$ linearly for small $`U`$, and exponentially for $`U>2`$, consistent with the Mott-insulating behavior.

The even-odd asymmetry, and the perfect transmission for the odd case, point to the importance of the contacts. In order to investigate their role, we introduce a position dependent interaction strength $`U_i`$ which increases linearly from $`0`$ to its maximum value $`U`$, inside the “contacts” of length $`L_\mathrm{A}`$ (see inset of Fig. 3). As shown in Fig. 3, these smooth contacts increase $`g`$, at constant effective length $`L_{\mathrm{eff}}=L_\mathrm{S}L_\mathrm{A}`$ of the sample. The effect is pronounced in the case of even $`L_\mathrm{S}`$ and the conductance approaches the ideal situation of perfect transmission expected for reflectionless contacts when we improve the smoothing safi . While the form of the contacts preserves the right-left symmetry, the smoothing leads to an extension of the perfect transmission at odd $`L_\mathrm{S}`$ towards higher values of $`U`$. However, we found that asymmetric contacts destroy the perfect transmission. The strong influence of the contacts is crucial when describing experiments since it seems impossible to connect a nanosample via reflectionless contacts. It also shows the limitation of other approaches relating the conductance of an interacting sample to its intrinsic properties, without taking into account the way it is connected to the electrodes.

While clean interacting systems are of physical interest (e.g. carbon nanotubes), it is also important to consider the generic case of disordered systems. To this end, we add the term $`W_{i=1}^{L_\mathrm{S}}v_in_i`$ to the Hamiltonian (6), where $`W`$ is the disorder strength and the $`v_i`$ are distributed equally in $`[1/2,1/2]`$. We have checked that $`D`$ scales with $`L`$ as before (Eq. (7)), ensuring a well-defined limiting value for $`g`$. The even-odd dependence of $`g`$ disappears when disorder is introduced. The combined effect of disorder and interactions on $`g`$ is shown in Fig. 4. In the ballistic regime (at $`W=1`$ the mean free path exceeds $`L_\mathrm{S}`$) the effect of $`W`$ is weak at small $`U`$, and it becomes more pronounced at stronger $`U`$ (when the disorder pins the Mott insulator, reinforcing the localization). At large $`W`$, $`g`$ for individual samples exhibits peaks as a function of $`U`$ whenever a charge reorganization occurs, similarly to the case of the $`D`$ calculated without the lead sjwp . Very remarkably, the ensemble average of $`\mathrm{ln}g`$ is increased by a moderate repulsive $`U`$, showing the non-trivial interplay of disorder and interactions in a transport problem.

In conclusion, starting from a recent proposal sushkov , we have provided a well-defined procedure for calculating the conductance $`g`$ of interacting one-dimensional wires, and used it to investigate correlation and disorder effects. While the interaction reduces $`g`$ for spinless fermions in the presence of weak or moderate disorder, a moderate repulsive interaction increases $`g`$ at strong disorder. We also determined the crucial role of the sample-to-lead contacts on the conductance.

We thank O. Sushkov and C. Stafford for useful discussions, P. Schmitteckert and Ph. Brune for their DMRG programs. RAM acknowledges the financial support from the European Union’s Human Potential Program (contract HPRN-CT-2000-00144). RAJ and DW thank the INT at the University of Washington for its hospitality and support during completion of this work.


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# Order-disorder criticality, wetting, and morphological phase transitions in the irreversible growth of far-from-equilibrium magnetic films

## 1 Introduction

The preparation and characterization of magnetic nanowires and films is of great interest for the development of advanced microelectronic devices. Therefore, the study of the behavior of magnetic materials in confined geometries, e.g. thin films, has attracted both experimental  and theoretical  attention. From the theoretical point of view, most of the work has been devoted to the study of equilibrium properties of thin magnetic films  and magnetic materials, see e.g. . In contrast, the aim of this work is to study the properties of thin magnetic film growth under far-from-equilibrium conditions, by means of extensive Monte Carlo simulations. Within this context, this work is related to many recent investigations concerned with irreversible growth processes. Indeed, the study of growth systems under far-from-equilibrium conditions is a subject that has drawn great attention during the last decades. Nowadays, this interdisciplinary field has experienced a rapid progress due to its interest in many subfields of physics, chemistry, and even biology, as well as by its relevance in numerous technological applications such as the development of nanoscale devices, polymer science, crystal and polycrystalline growth, gelation, fracture propagation, epidemic spreading, colloids, etc. .

For the purpose of studying the properties of thin magnetic film growth under far-from-equilibrium conditions, a variant of the irreversible Eden growth model , in which particles are replaced by spins that can adopt two different orientations, is investigated. Our study is performed in confined (stripped) geometries, which resemble recent experiments where the growth of quasi-one-dimensional strips of Fe on a Cu(111) vicinal surface  and Fe on a W(110) stepped substratum  have been performed. Also, in a related context, the study of the growth of metallic multilayers has shown a rich variety of new physical features. Particularly, the growth of magnetic layers of Ni and Co separated by a Cu spacer layer has recently been studied .

The growth of magnetic films with competing short-range magnetic fields, which account for the interaction of the growing films with the substrate, is also investigated in the present work. The competing situation considered leads to rich and complex physical phenomena that exhibit a delicate and subtle interplay between finite-size effects, wetting, and interface growth mechanisms. Besides the technological and scientific interest that may arise from the nonequilibrium nature of the model investigated, as already pointed out, this kind of nonequilibrium wetting phenomena also appears closely related to very interesting equilibrium wetting transitions, which have attracted so far considerable experimental and theoretical attention. For instance, surface enrichment and wetting layers have been observed experimentally in a great variety of systems, such as e.g. polymer mixtures , adsorption of simple gases on alkali metal surfaces , hydrocarbons on mica , etc. From the theoretical point of view, the study of wetting transitions at interfaces has been carried out by means of different approaches, such as the mean field Ginzburg-Landau method , transfer matrix and Pfaffian techniques , density matrix renormalization group methods , solving the Cahn-Hilliard equation , using Molecular Dynamic simulations , solving self-consistent field equations , and by means of extensive Monte Carlo simulations .

Finally, it should also be remarked that, although the discussion is presented here in terms of a magnetic language, the relevant physical concepts could be extended to other systems such as fluids, polymers, and binary mixtures.

This manuscript is organized as follows: in Section 2 details on the model and the simulation method are given, Section 3 is devoted to the order-disorder critical behavior of magnetic Eden films, Section 4 deals with the study of interfacial phase transitions that arise when competing short-range magnetic fields are considered, while the conclusions are finally stated in Section 5.

## 2 The model and the simulation method

In the classical Eden model  on the square lattice, the growth process starts by adding particles to the immediate neighborhood (the perimeter) of a seed particle. Subsequently, particles are stuck at random to perimeter sites. This growth process leads to the formation of compact clusters with a self-affine interface . The magnetic Eden model (MEM)  considers an additional degree of freedom due to the spin of the growing particles. In the present work the MEM is studied in $`(d+1)`$dimensional rectangular geometries for $`d=1,2`$, as described in .

For the case $`d=1`$, the MEM is investigated on the square lattice using a rectangular geometry $`L\times M`$ (with $`ML`$). The location of each site on the lattice is specified through its rectangular coordinates $`(i,j)`$, ($`1iL`$, $`1jM`$). The starting seed for the growing cluster is a column of parallel-oriented spins placed at $`j=1`$ and film growth takes place along the positive longitudinal direction (i.e. $`j2`$). Periodic boundary conditions are adopted along the transverse direction. Then, assuming that each spin $`S_{ij}`$ can be either up or down (i.e. $`S_{ij}=\pm 1`$), clusters are grown by selectively adding spins to perimeter sites, which are defined as the nearest-neighbor (NN) empty sites of the already occupied ones. Considering a ferromagnetic interaction of strength $`J>0`$ between NN spins, the energy $`E`$ of a given configuration of spins is given by

$$E=\frac{J}{2}\underset{ij,i^{^{}}j^{^{}}}{}S_{ij}S_{i^{^{}}j^{^{}}},$$
(1)
where $`ij,i^{^{}}j^{^{}}`$ means a summation taken over all occupied NN sites.

Analogously, the MEM in $`(2+1)`$ dimensions is studied using a $`L\times L\times M`$ rectangular geometry ($`ML`$). Each site on the lattice is now identified through the rectangular coordinates $`(i,j,k)`$, ($`1i,jL`$, $`1kM`$), and the starting seed for the growing film is taken to be a plane of $`L\times L`$ parallel-oriented spins placed at $`k=1`$. The energy of the spin configuration is now calculated by extending the summation in Eq.(1) to the three coordinates $`(i,j,k)`$. For further details on the MEM defined in retangular geometries see also .

The last part of this paper (see Section 4) is devoted to the study of the $`(2+1)`$-dimensional MEM with competing short-range magnetic fields applied along one of the transverse directions. In this case, the periodic boundary conditions along the $`j`$direction are changed to open ones, and competing surface magnetic fields $`H>0`$ ($`H^{}=H`$) acting on the sites placed at $`j=1`$ ($`j=L`$) are considered . Then, the energy of a given configuration of spins in this case will be given by

$$E=\frac{J}{2}\left(\underset{ijk,i^{^{}}j^{^{}}k^{^{}}}{}S_{ijk}S_{i^{^{}}j^{^{}}k^{^{}}}\right)H\left(\underset{ik,\mathrm{\Sigma }_1}{}S_{i1k}\underset{ik,\mathrm{\Sigma }_L}{}S_{iLk}\right),$$
(2)
where $`ijk,i^{^{}}j^{^{}}k^{^{}}`$ means that the summation in the first term is taken over all occupied NN sites, while $`ik,\mathrm{\Sigma }_1`$, $`ik,\mathrm{\Sigma }_L`$ denote summations carried over occupied sites on the surfaces $`\mathrm{\Sigma }_1`$, $`\mathrm{\Sigma }_L`$ (defined as the $`j=1`$ and $`j=L`$ planes, respectively). Throughout this work we set the Boltzmann constant equal to unity ($`k_B1`$) and consider the absolute temperature, energy, and magnetic fields measured in units of the coupling constant $`J`$.

The growth process of a MEM film consists in adding further spins to the growing film taking into account the corresponding interaction energies. A spin is added to the film with a probability proportional to the Boltzmann factor $`\mathrm{exp}(\mathrm{\Delta }E/T)`$, where $`\mathrm{\Delta }E`$ is the total energy change involved. At each step, the probabilities of adding up and down spins to a given site have to be evaluated for all perimeter sites. After proper normalization of the probabilities, the growing site and the orientation of the spin are determined through standard Monte Carlo techniques. Although both the interaction energy (as given either by Eq.(1) or Eq.(2)) and the Boltzmann probability distribution considered for the MEM are similar to those used for the Ising model , it must be stressed that these two models operate under extremely different conditions, namely the MEM describes the irreversible growth of a magnetic material and the Ising model is suitable for the study of a magnetic system under equilibrium conditions. In the MEM, the position and orientation of all deposited spins remain fixed. During the growth process, the system develops a rough growing interface and evolves mainly along the longitudinal direction. Some lattice sites can remain empty even well within the system’s bulk, but, since at each growth step all perimeter sites are candidates for becoming occupied, these holes are gradually filled. Hence, far behind the active growing interface, the system is compact and frozen. When the growing interface is close to reaching the limit of the sample, the relevant properties of the irreversibly frozen cluster’s bulk (in the region where the growing process has definitively stopped) are computed, the useless frozen bulk is thereafter erased, and finally the growing interface is shifted toward the lowest possible longitudinal coordinate. Hence, repeatedly applying this procedure, the growth process is not limited by the lattice length $`M`$. In the present work clusters having up to $`10^9`$ spins have typically been grown.

## 3 Order-disorder critical behavior of magnetic Eden films

Magnetic Eden films grown on a stripped geometry of finite linear dimension $`L`$ at low temperatures show an intriguing behavior that we call spontaneous magnetization reversal. In fact, we have observed that long clusters are constituted by a sequence of well ordered magnetic domains of average length $`l_DL`$. Let $`l_R`$ be the characteristic length for the occurrence of the spontaneous magnetization reversal. Since $`l_RL`$, we then conclude that the phenomenon has two characteristic length scales, namely $`l_D`$ and $`l_R`$, such that $`l_Dl_RL`$. Hence, the spontaneous magnetization reversal is essentially due to the small size of the thin film and it becomes irrelevant in the thermodynamic limit. Figure 1 shows a snapshot configuration of the $`(1+1)`$dimensional MEM where this phenomenon can be recognized. Here the reversal occurring between a domain of spins up (on the left side) and other one constituted by spins down (on the right), as well as the interface between both domains, can be clearly observed. The magnetization change occurs quite abruptly within the characteristic length $`l_RL`$.

In ordinary thermally driven phase transitions, the system changes from a disordered state at high temperatures to a spontaneously ordered state at temperatures below some critical value $`T_c`$, where a second-order phase transition takes place. Regarding the Ising model, one has that, in the absence of an external magnetic field ($`H=0`$), the low-temperature ordered phase is a state with non-vanishing spontaneous magnetization ($`\pm M_{sp}`$). This spontaneous symmetry breaking is possible in the thermodynamic limit only. In fact, it is found that the magnetization $`M`$ of a finite sample formed by $`N`$ particles, defined by

$$M(T,H=0)=\frac{1}{N}\underset{i=1}{\overset{N}{}}S_i(T,H=0),$$
(3)
can pass with a finite probability from a value near $`+M_{sp}`$ to another near $`M_{sp}`$, as well as in the opposite direction. Consequently, the magnetization of a finite system, averaged over a sufficiently large observation time, vanishes irrespective of the temperature. That is, the equation $`M(T,H=0)0`$ holds if the observation time ($`t_{obs}`$) becomes larger than the ergodic time ($`t_{erg}`$), which is defined as the time needed to observe the system passing from $`\pm M_{sp}`$ to $`M_{sp}`$. Since Monte Carlo simulations are restricted to finite samples, the standard procedure to avoid the problems treated in the foregoing discussion is to consider the absolute magnetization as an order parameter . Turning back to the MEM, we find that the phenomenon of magnetization reversal also causes the magnetization of the whole cluster to vanish even for very low (but non-zero) temperatures, provided that the film’s total length $`l_F`$ (which plays the role of $`t_{obs}`$) is much larger than $`l_D`$ (which plays the role of $`t_{erg}`$). Therefore, as in the case of the Ising model , in order to overcome shortcomings derived from the finite-size nature of Monte Carlo simulations we have measured the mean absolute column magnetization, given by

$$|m(j,L,T)|=\frac{1}{L}|\underset{i=1}{\overset{L}{}}S_{ij}|.$$
(4)
It is found that $`|m(j;L,T)|`$ exhibits a transient growing period with a characteristic length of order $`L`$, followed by the attainment of a stationary regime, which is independent of the orientation of the seed.

The mean column magnetization given by Eq.(4) is a fluctuating quantity that can assume $`L+1`$ values. Then, for given values of both $`L`$ and $`T`$, the probability distribution of the mean column magnetization $`(P_L(m))`$ can straightforwardly be evaluated, since it represents the normalized histogram of $`m`$ taken over a sufficiently large number of columns in the stationary region . In the thermodynamic limit ($`L\mathrm{}`$) the probability distribution $`(P_{\mathrm{}}(m))`$ of the order parameter of an equilibrium system at criticality is universal (up to re-scaling of the order parameter) and thus it contains very useful and interesting information on the universality class of the system . For example, $`P_L(m)`$ contains information about all momenta of the order parameter $`m`$, including universal ratios such as the Binder cumulant .

Figure 2 shows the thermal dependence of $`P_L(m)`$ versus $`m`$, as obtained for the $`(1+1)`$dimensional MEM. We can observe that at high temperatures $`P_L(m)`$ is a Gaussian centered at $`m=0`$. As the temperature gets lowered, the distribution broadens and develops two peaks at $`m=\pm 1`$. Further decreasing the temperature causes these peaks to become dominant while the distribution turns distinctly non-Gaussian, exhibiting a minimum just at $`m=0`$. It should be pointed out that the emergence of the maxima at $`m=\pm 1`$ is quite abrupt. This behavior reminds us the order parameter probability distribution characteristic of the one-dimensional Ising model. In fact, for the well studied $`d`$dimensional Ising model , we know that for $`T>T_c`$, $`P_L(M)`$ is a Gaussian centered at $`M=0`$, given by

$$P_L(M)\mathrm{exp}\left(\frac{M^2L^d}{2T\chi }\right),$$
(5)
where the susceptibility $`\chi `$ is related to order parameter fluctuations by

$$\chi =\frac{L^d}{T}\left(M^2M^2\right).$$
(6)
Decreasing the temperature, the order parameter probability distribution broadens, it becomes non-Gaussian, and near $`T_c`$ it splits into two peaks that get the more separated the lower the temperature. For $`T<T_c`$ and linear dimensions $`L`$ much larger than the correlation length $`\xi `$ of order parameter fluctuations, one may approximate $`P_L(M)`$ near the peaks by a double-Gaussian distribution, i.e.

$$P_L(M)\mathrm{exp}\left(\frac{(MM_{sp})^2L^d}{2T\chi }\right)+\mathrm{exp}\left(\frac{(M+M_{sp})^2L^d}{2T\chi }\right),$$
(7)
where $`M_{sp}`$ is the spontaneous magnetization, while the susceptibility $`\chi `$ is now given by

$$\chi =\frac{L^d}{T}\left(M^2|M|^2\right).$$
(8)
From Eq.(5) it turns out that the Gaussian squared width $`\sigma ^2`$ associated with high temperature distributions is very close to the 2nd moment of the order parameter, i.e.

$$\sigma ^2M^2.$$
(9)
It should be noticed that this equation is a straightforward consequence of the Gaussian shape of the order parameter probability distribution and, thus, it holds for the MEM as well. From the well known one-dimensional exact solution for a chain of $`L`$ spins  one can establish the relationship

$$\chi =\frac{1}{T}\mathrm{exp}(2/T);$$
(10)
then, Eqs.(6) and (10) lead us to

$$M^2=\frac{1}{L}\mathrm{exp}(2/T)$$
(11)
(where it has been taken into account that $`M=0`$ due to finite-size effects, irrespective of temperature). From Eqs.(9) and (11) we can see that the high-temperature Gaussian probability distribution broadens exponentially as $`T`$ gets lowered, until it develops delta-like peaks at $`M=\pm 1`$ as a consequence of a boundary effect on the widely extended distribution. It should be noted that for $`d2`$ this phenomenon is prevented by the finite critical temperature which splits the Gaussian, as implied by Eq.(7).

Figure 3 shows the thermal evolution of the probability distribution as obtained for the $`(2+1)`$dimensional MEM. Notice that now $`m`$ is defined by an average over transverse planes constituted by $`L\times L`$ spins, analogously to Eq.(4). Hence, $`m`$ takes now $`L^2+1`$ possible values. For high temperatures, the probability distribution corresponds to a Gaussian centered at $`m=0`$. At lower temperatures we observe the onset of two maxima located at $`m=\pm M_{sp}`$ $`(0<M_{sp}<1)`$, which become sharper and approach $`m=\pm 1`$ as $`T`$ is gradually decreased. These low-temperature probability distributions clearly reflect the occurrence of the magnetization reversal effect already discussed for the case of $`(1+1)`$dimensional magnetic films.

Figure 4 shows the location of the maximum of the probability distribution as a function of temperature for both $`(d+1)`$-dimensional MEM models (with $`d=1,2`$), where only maxima located at $`m0`$ are considered, since the distributions are symmetric around $`m=0`$. After inspection of figure 4, it becomes apparent the different qualitative behavior of both systems. Indeed, while for the $`d=2`$ case we observe a smooth transition from the $`m_{max}=0`$ value characteristic of high temperatures to nonzero $`m_{max}`$ values that correspond to lower temperatures, the curve obtained for $`d=1`$ shows instead a Heaviside-like jump. In contrast to the $`(1+1)`$dimensional case, the behavior exhibited by the $`(2+1)`$-dimensional MEM (e.g. as displayed by figures 3 and 4) is the signature of a thermal continuous phase transition that takes place at a finite critical temperature.

From the finite-size scaling theory, developed for the treatment of finite-size effects at criticality and under equilibrium conditions , it is well known that if a thermally driven phase transition occurs at a temperature $`T_c>0`$ in the thermodynamic limit, then in a confined geometry of linear dimension $`L`$ this transition becomes smeared out over the temperature region $`\mathrm{\Delta }T(L)`$ around a shifted effective transition temperature $`T_c(L)`$, which are related to $`L`$ through phenomenological exponents. Indeed, it is found that

$$\mathrm{\Delta }T(L)L^\theta $$
(12)
and

$$|T_c(L)T_c|L^\lambda ,$$
(13)
where the rounding and shift exponents are given by $`\theta =\lambda =\nu ^1`$, respectively, and where $`\nu `$ is the exponent that characterizes the divergence of the correlation length at criticality.

Furthermore, from well-established finite-size scaling relations, the following Ansätze hold just at criticality:

$$|m(L,T=T_c)|L^{\beta /\nu }$$
(14)
and

$$\chi _{max}(L)L^{\gamma /\nu },$$
(15)
where $`\beta `$ and $`\gamma `$ are the order parameter and the susceptibility critical exponents, respectively. Note that $`\chi _{max}(L)`$, as given by Eq.(15), refers to the maximum of $`\chi (L,T)`$ as a function of $`T`$ for a fixed lattice size $`L`$.

In order to describe quantitatively the critical behavior of the MEM in $`(2+1)`$-dimensions, we may test the validity of the scaling relations given in Eqs.(12)-(15). As in the case of equilibrium systems, in the present case various “effective” $`L`$-dependent critical temperatures can also be defined. In particular, we will define $`T_{c1}(L)`$ as the value that corresponds to $`|m|=0.5`$ for fixed $`L`$, and $`T_{c2}(L)`$ as the one corresponding to the maximum of the susceptibility for a given $`L`$, assuming that the susceptibility is related to order parameter fluctuations in the same manner as for equilibrium systems (as given by Eqs.(6) and (8)). Then, $`T_c`$ can be obtained from plots of $`T_{cn}(L)`$ versus $`L^1`$ (for $`n=1,2`$), as is shown in figure 5. Following this procedure we find that both $`T_{c1}(L)`$ and $`T_{c2}(L)`$ extrapolate (approximately) to the same value, allowing us to evaluate the critical temperature $`T_c=0.69\pm 0.01`$ in the thermodynamic limit.

After determining $`T_c`$, the correlation length exponent $`\nu `$ can be evaluated by means of Eq.(13), making the replacement $`\lambda =1/\nu `$. Indeed, taking $`T_c`$ at the mean, maximum and minimum values allowed by the error bars, we obtain six log-log plots of $`|T_{cn}(L)T_c|`$ versus $`L`$ for $`n=1,2`$. The slope of each of these plots, not shown here for the sake of space, yields a value for $`\nu `$. The obtained values are:

$$\nu =1.08(T_c=0.68),\nu =1.00(T_c=0.69),$$

$$\nu =0.88(T_c=0.70)\mathrm{for}\mathrm{n}=1,$$
(16)
and

$$\nu =1.20(T_c=0.68),\nu =1.08(T_c=0.69),$$

$$\nu =0.95(T_c=0.70)\mathrm{for}\mathrm{n}=2.$$
(17)
Thus our estimate is given by $`\nu =1.04\pm 0.16`$, where the error bars reflect the error derived from the evaluation of $`T_c`$, as well as the statistical error.

Studying the susceptibility $`\chi `$ as a function of the temperature for several different lattice sizes, it is found that $`\chi `$ exhibits a peak, which becomes sharper and shifts toward lower temperatures as $`L`$ is increased. Hence, Eq.(15) can be used to evaluate $`\gamma /\nu `$ from the slope of a log-log plot of $`\chi _{max}`$ versus $`L`$, as figure 6 shows. The linear fit yields $`\gamma /\nu =2.02\pm 0.04`$. Using this value and the value formerly obtained for $`\nu `$ we thus determine $`\gamma =2.10\pm 0.36`$.

Figure 7 shows log-log plots of $`|m|(T=T_c)`$ versus $`L`$ for the mean, maximum and minimum allowed values of $`T_c`$. Considering only the larger lattices, the linear fits to the data according to Eq.(14) yield the following estimates: $`\beta /\nu =0.11`$, $`\beta /\nu =0.16`$ and $`\beta /\nu =0.19`$. We then assume the value $`\beta /\nu =0.15\pm 0.04`$, where the error bars reflect the error derived from the evaluation of $`T_c`$, as well as the statistical error. From this value and the value formerly obtained for $`\nu `$ we thus determine $`\beta =0.16\pm 0.05`$.

In this manner, we conclude that magnetic Eden films grown on stripped $`(d+1)`$-dimensional geometries are non-critical for $`d=1`$, in the sense that the ordered phase is trivially found only at $`T=0`$. However, MEM films exhibit a continuous order-disorder phase transition at the critical temperature $`T_c=0.69\pm 0.01`$ for $`d=2`$. Furthermore, the critical exponents of the MEM in $`(2+1)`$ dimensions, as obtained using a finite-size scaling analysis, are: $`\nu =1.04\pm 0.16`$, $`\gamma =2.10\pm 0.36`$, and $`\beta =0.16\pm 0.05`$.

## 4 Study of the $`(2+1)`$-dimensional MEM with competing short-range magnetic fields: Wetting and morphological phase transitions

In this section, we will study the interfacial phase transitions that arise in the $`(2+1)`$-dimensional MEM, when competing short-range magnetic fields applied along one of the transverse directions are considered. As described in Section II, we will assume competing surface magnetic fields $`H>0`$ ($`H^{}=H`$) acting on the surfaces $`j=1`$ and $`j=L`$. Hence, the energy associated to a given spin configuration acquires an additional term due to the interaction of the surface spins with the applied magnetic fields (see Eq.(2)).

As shown in figure 8, magnetic Eden films that grow in a confined geometry with competing surface fields exhibit a very rich phase diagram, which is composed of eight regions. These regions are delimited by several distinct, well-defined transition curves. As will be shown below, the bulk order-disorder (finite-size) critical point $`T_c(L)`$, the Ising-like quasi-wetting transition curve $`T_w(L,H)`$, and two morphological transitions associated to the curvature of the growing interface (namely, from convex to non-defined to concave), can be quantitatively located. Moreover, in order to gain some insight into the physics involved in this complex phase diagram, some typical snapshot configurations characteristic of the various different growth regimes are obtained (see figure 9) and discussed. Finally, the phase diagram in the thermodynamic limit will be drawn (see inset of figure 8) by extrapolating finite-size results (see figure 10).

The ($`L`$dependent) bulk order-disorder critical temperature can be identified with the peak of the susceptibility at zero surface field. For $`L=12`$, the critical point so defined is $`T_c(L=12)=0.84`$, and is shown in figure 8 by a vertical straight line. So, the left (right) hand side part of the phase diagram corresponds to the ordered (disordered) growth regime that involves Regions $`I,II,III,IV`$, and $`A`$ (Regions $`V,VI`$, and $`B`$).

Using a standard procedure , the localization-delocalization transition curve (on the $`HT`$ plane) corresponding to the up-down interface running along the walls can be computed, considering that a point with coordinates $`(H_w,T_w)`$ on this curve maximizes $`\chi (H,T)`$. So, the size-dependent localization-delocalization transition curve is obtained, as shown in figure 8 (open squares). As in the case of the Ising model, this quasi-wetting transition refers to a transition between a nonwet state that corresponds to a localized interface bound to one of the confinement walls, and a wet state associated with a delocalized domain interface centered between roughly equal domains of up and down spins. The localization-delocalization transition in a confined system is indeed the precursor of the true wetting transition, which occurs in the thermodynamic limit . In fact, there is observed a finite jump in the wetting layer thickness that takes place as a result of the finite size of the system. As the lattice size is increased, the magnitude of the jump grows and diverges in the $`L\mathrm{}`$ limit, as expected for a continuous wetting transition.

Since the MEM is a nonequilibrium kinetic growth model, it also allows the identification of another kind of phase transition, namely a morphological transition associated with the curvature of the growing interface of the system. To avoid confusion, we would like to remark that the term interface is used here for the transverse interface between occupied and empty lattice sites, while it was used above for the longitudinal interface between up and down spin domains. To explore this phenomenon quantitatively, the behavior of the contact angles between the growth interface and the confinement walls (as functions of temperature and magnetic field) have to be investigated. Clearly, two different contact angles should be defined in order to locate this transition, namely $`\theta _D`$ for the angle corresponding to the dominant spin cluster, and $`\theta _{ND}`$ for the one that corresponds to the non-dominant spin cluster. Both contact angles can straightforwardly be determined by measuring the location of the growth interface averaged over a sufficiently long growing time. In this way, three different growth regimes can be distinguished: (i) the concave growth regime that occurs when the system partially wets the walls on both sides (i.e. for $`\theta _D,\theta _{ND}<\frac{\pi }{2}`$), (ii) the convex growth regime that occurs for $`\theta _D,\theta _{ND}>\frac{\pi }{2}`$, and (iii) the regime of non-defined curvature that occurs otherwise. The corresponding transition curves obtained for confined magnetic Eden films are shown on the $`HT`$ phase diagram of figure 8, where open (filled) circles refer to the transition between non-defined and concave (convex) growth regimes.

As anticipated above, we will now introduce and discuss some characteristic snapshot pictures, in order to provide qualitative explanations that account for the different growth regimes observed. Let us begin with Region $`I`$ (see figure 8), that corresponds to the Ising-like nonwet state and the convex growth regime. In this region, the temperature is low and the system grows in an ordered state, i.e. the dominant spin domain prevails and the deposited particles tend to have their spins all pointing in the same direction. Small clusters with the opposite orientation may appear preferably on the surface where the non-dominant orientation field is applied. These “drops” might grow and drive a magnetization reversal, thus changing the sign of the dominant domain. Indeed, the formation of sequences of well-ordered domains are characteristic of the ordered phase of confined (finite-size) spin systems such as the Ising magnet . Due to the open boundary conditions, perimeter sites at the confinement walls experience a missing neighbor effect, that is, the number of NN sites is lower than for the case of perimeter sites on the bulk. Since $`H`$ is too weak to compensate this effect, the system grows preferentially along the center of the sample as compared to the walls, and the resulting growing interface exhibits a convex shape. So, Region $`I`$ corresponds to the Ising-like nonwet state and the convex growth regime. A typical snapshot configuration characteristic of Region $`I`$ is shown in figure 9(a).

Let us now consider an increase in the surface magnetic fields, such as the system may be driven into Region $`II`$ (see figure 8). Since the temperature is kept low, the system is still in its ordered phase and neighboring spins grow preferably parallel-oriented. The surface fields in this region are stronger and thus capable of compensating the missing NN sites on the surfaces. But, since the fields on both surfaces have opposite signs, it is found that, on the one hand, the field that has the same orientation as the dominant spin cluster favors the growth of surface spins, while on the other hand, the sites on the surface with opposite field have a lower probability to be chosen during the growth process. Hence, the contact angle corresponding to the dominant spin cluster is then $`\theta _D<\frac{\pi }{2}`$, while the non-dominant is $`\theta _{ND}>\frac{\pi }{2}`$. Thus, on the disfavored side the growing interface becomes pinned and the curvature of the growing interface is not defined. Figure 9(b) shows a typical snapshot corresponding to Region $`II`$.

Keeping $`H`$ fixed within Region $`II`$ but increasing the temperature, thermal noise will enable the formation of drops on the disfavored side that eventually may nucleate into larger clusters as the temperature is increased even further. This process may lead to the emergence of an up-down interface, separating oppositely oriented domains, running in the longitudinal direction (i.e. parallel to the walls). Since sites along the up-down interface are surrounded by oppositely oriented NN spins, they have a low growing probability. So, in this case the system grows preferably along the confinement walls and the growing interface is concave (figure 9(c)). Then, as the temperature is increased, the system crosses to Region $`A`$ (see figure 8) and the onset of two competitive growth regimes is observed, namely: (i) one exhibiting a non-defined growing curvature that appears when a dominant spin orientation is present, as in the case shown in figure 9(b); (ii) another that appears when an up-down interface is established and the system has a concave growth interface, as is shown in figure 9(c).

On further increasing the temperature and for large enough fields, the formation of a stable longitudinal up-down interface that pushes back the growing interface is observed. So, the system adopts the concave growth regime (see figure 9(c) corresponding to Region $`IV`$ in figure 8). Increasing the temperature beyond $`T_c(L)`$, a transition from a low-temperature ordered state (Region $`IV`$) to a high-temperature disordered state (Region $`VI`$, see figure 9(e)), both within the concave growth regime, is observed. Analogously, for small enough fields, a temperature increase drives the system from the ordered convex growth regime (Region $`I`$) to the disordered convex growth regime (Region $`V`$, see figure 9(d)). As shown in figure 8, there is also an intermediate fluctuating state (Region $`B`$) between Regions $`V`$ and $`VI`$, characterized by the competition between the disordered convex growth regime and the disordered concave one.

Finally, a quite unstable and small region (Region $`III`$ in figure 8) that exhibits the interplay among the growth regimes of the contiguous regions, can also be identified. Since the width of Region $`III`$ is of the order of the rounding observed in $`T_c(L)`$, large fluctuations between ordered and disordered states are observed, as well as from growth regimes of non-defined curvature to convex ones. However, figure 9(f) shows a snapshot configuration that is the fingerprint of Region $`III`$, that may prevail in the thermodynamic limit, namely a well defined spin up-down interface with an almost flat growing interface.

Let us now extrapolate our results to show that the rich variety of phenomena found in a confined geometry is still present in the thermodynamic limit ($`L\mathrm{}`$), leading to the phase diagram shown in the inset of figure 8. As clearly seen by comparison with the finite-size results, the crossover Regions $`A`$ and $`B`$ collapse in this limit, so only the six regions that correspond to well identified growth regimes (as illustrated by the snapshot configurations of figure 9) appear to remain.

In order to illustrate the extrapolation procedure, the following seven representative points of the finite-size phase diagram are discussed in detail: (i) the points labeled $`P_1`$, $`P_1^{}`$, $`P_2`$, and $`P_2^{}`$, that correspond to the intersections of the $`H=0.6`$ line with the various transition curves shown in figure 8, and (ii) the points labeled $`P_3`$, $`P_3^{}`$, and $`P_4`$, that refer to the intersection point between Regions $`I,II,III`$, and $`A`$, the minimum of the limiting curve between Regions $`IV`$-$`VI`$ and $`A`$-$`B`$, and the zero-field transition point, respectively.

Figure 10 shows plots of $`T`$ versus $`L^1`$ for $`12L48`$ corresponding to the points $`P_1,P_1^{},P_2,`$ and $`P_2^{}`$. Also shown in the figure are the fits to the data extrapolated to $`L^1=0`$. The results from the extrapolations are: $`T_1=0.67\pm 0.01`$, $`T_1^{}=0.66\pm 0.01,`$ and $`T_2=1.30\pm 0.02`$, $`T_2^{}=1.29\pm 0.01,`$ pointing out that, within error bars, $`P_iP_i^{}`$ $`(i=1,2)`$ in the $`L\mathrm{}`$ limit. Using the same procedure, the extrapolations of $`P_3`$ and $`P_3^{}`$ (not shown here) give: $`H_3=0.30\pm 0.01`$, $`H_3^{}=0.31\pm 0.02,`$ and $`T_3=0.69\pm 0.01`$, $`T_3^{}=0.71\pm 0.03`$. So, one has $`P_3P_3^{}`$ for $`L\mathrm{}`$ within error bars. Finally, the extrapolation of $`P_4`$ is $`T_4=T_c=0.69\pm 0.01`$.

Using the above-mentioned extrapolation procedure, the phase diagram in the thermodynamic limit can be drawn, as shown in the inset of figure 8. By comparison with the finite-size phase diagram of figure 8, one can note that, as anticipated, the crossover Regions $`A`$ and $`B`$ appear in the phase diagram just as a consequence of the finite-size nature of confined geometries, since they collapse in the $`L\mathrm{}`$ limit. Moreover, we conjecture that Region $`III`$ may remain in the thermodynamic limit. Although this (very tiny!) region corresponds to a physically well-characterized growth regime, since one expects that the system in this region may grow in an ordered phase with a delocalized up-down domain interface and a convex growing interface, statistical errors due to large fluctuations close to criticality hinder a more accurate location of this region. The unambiguous clarification of our conjecture remains as an open question that will require a huge computational effort.

Besides an Ising-like continuous wetting transition, coupled morphological transitions in the growing interface, which arise from the MEM’s kinetic growth process, have also been identified. Comparing the equilibrium wetting phase diagram of the Ising model  and that of the MEM, it follows that the nonequilibrium nature of the latter introduces new and rich physical features of interest: the nonwet (wet) Ising phase splits out into Regions $`I`$ and $`II`$ (Regions $`III`$ and $`IV`$), both within the ordered regime ($`T<T_c`$) but showing an additional transition in the interface growth mode. Also, the disordered state of the Ising system ($`T>T_c`$) splits out into Regions $`V`$ and $`VI`$ exhibiting a transition in the interface growth mode.

## 5 Conclusions

In the present work we have studied the growth of magnetic Eden films with ferromagnetic interactions between nearest-neighbor spins in a $`(d+1)`$dimensional rectangular geometry (for $`d=1,2`$), by means of extensive Monte Carlo simulations. For both dimensions the phenomenon of spontaneous magnetization reversal is observed at low temperatures. Indeed, MEM films grown at low temperatures are constituted by a sequence of magnetic domains, each of them with a well-defined magnetization, such that the magnetization of adjacent domains is antiparallel. Furthermore, it is found that the $`(1+1)`$dimensional MEM is non-critical, while the $`(2+1)`$dimensional MEM undergoes a thermally driven second-order phase transition at finite temperature, which is evaluated by extrapolating some “effective” $`L`$-dependent critical temperatures to the thermodynamic limit ($`L\mathrm{}`$). Using a finite-size scaling theory, some relevant critical exponents that characterize the behavior of the $`(2+1)`$dimensional MEM at criticality are determined. The observed behavior is reminiscent to that of the equilibrium Ising model, although it should be stressed that the MEM is a far-from-equilibrium growing system.

Finally, the $`(2+1)`$dimensional MEM with competing surface magnetic fields, which may account for the interaction of the growing magnetic films with the substrate, is investigated. An Ising-like localization-delocalization wetting transition and, on the other hand, a morphological transition associated with the curvature of the growing interface, are located. In this way, eight different regions on the $`HT`$ phase diagram for a finite-size lattice are identified. Moreover, the characteristic behavior of typical growth processes within each region are discussed, and qualitative explanations that account for the observed features are provided. Extrapolating the results obtained for various lattice sizes, the phase diagram corresponding to the $`L\mathrm{}`$ limit is also determined. It is composed of six different regions, since two crossover regions identified in the finite-size phase diagram appear to collapse in the thermodynamic limit. The phase diagram obtained shows new and rich physical features of interest, which arise as a consequence of the nonequilibrium nature of the model investigated.

We expect that the present study will contribute to the fields of irreversible growth processes in confined geometries and nonequilibrium wetting phenomena, and we hope that it will stimulate further experimental and theoretical work in these topics of widespread technological and scientific interest.

ACKNOWLEDGMENTS. Work supported by CONICET, UNLP, and ANPCyT (Argentina).


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# The effects of matter density uncertainties on neutrino oscillations in the Earth

## References


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# Variability-Selected Quasars in MACHO Project Magellanic Cloud Fields

## 1 Introduction

Techniques to find quasars, largely successful in other regions of the sky, have had limited results towards the Magellanic Clouds (Tinney, 1999; Schmidtke et al., 1999; Dobrzycki et al., 2002). Crowding, recent star formation and significant dust extinction cause major quasar surveys to avoid these regions entirely, resulting in very few quasars known over the substantial sky coverage of the Magellanic Clouds. The most successful selection method to date in this region has been at X-ray wavelengths. Although many tens of sources background to the Magellanic Clouds have been identified in the X-rays (Kahabka et al., 1999; Haberl & Pietsch, 1999; Sasaki, Haberl & Pietsch, 2000), counterparts to these sources at other wavelengths have been stymied by postitional uncertainties; targeted X-ray follow-up has allowed optical identification of $`20`$ extragalactic sources in the Magellanic Cloud region (Crampton et al., 1997; Schmidtke et al., 1999). The MACHO lightcurve database (Alcock et al., 1997, 2000) provides an opportunity to search for quasars behind the Magellanic Clouds via an alternative method: optical variability.

Optical variability has been studied by many groups as a means of constraining models of the quasar central engine (Hook et al., 1994; Cristiani et al., 1997; Sirola et al., 1998; Hawkings, 2002, and references therein), as well as a method of quasar identification behind globular clusters (Meusinger & Brunzendorf, 2002). Although a handful of gravitationally-lensed quasars have well-sampled lightcurves on the timescale of years (Alcalde et al., 2002; Hjorth et al., 2002), most studies have had short time baselines and poor resolution. In one of the largest optical monitoring programs, Giveon et al. (1999) observed a sample of 42 quasars over 7 years with an average sampling interval of 40 days. Long-term optical variability of quasars in this study show no strong evidence for underlying periodic structure. This is in sharp contrast to the majority of stellar sources in the Magellanic Clouds which either do not vary or do so periodically. We have used this difference to separate quasar candidates from the overwhelming stellar background in the Clouds.

A comprehensive search for quasars behind both the Large and Small Magellanic Clouds (LMC and SMC, respectively) is motivated in part by the lack of a suitable reference frame against which to measure the proper motion of the Clouds. Previous proper motion estimates have suffered from an insufficient number or poorly distributed set of reference objects (Jones, Klemola & Lin, 1994; Kroupa & Bastian, 1997; Anguita, Loyola & Pedreros, 2000). Since the proper motion of the Clouds is expected to be only a few mas/year, a well distributed set of point-like background quasars could significantly improve the accuracy of this measurement, constraining the orbital history of these galaxies. These objects may also prove useful as light beacons for absorption line studies of the interstellar medium in the Magellanic Clouds (Gibson et al., 2000; Prochaska, Ryan-Weber & Staveley-Smith, 2002), as has been done for suspected extragalactic X-ray sources in this region (Kahabka et al., 2001; Haberl et al, 2001). Finally, this search was also motivated by interest in the quasars themselves, in hope that the dense time sampling of the MACHO lightcurves will provide clues to the physical mechanisms underlying quasar light variation.

We discuss the MACHO database and our optical variability quasar candidate selection methods in § 2. In § 3, we describe spectroscopic follow-up observations and present 47 quasars discovered behind the Magellanic Clouds. In § 4, MACHO lightcurves are presented for these quasars. Finally, in § 5 we summarize our results and discuss future quasar searches in this region. Finding charts, light curves and spectra for the quasars in this paper are available on request from the authors or on a website given at the end of § 5.

## 2 Quasar Candidate Selection

### 2.1 The MACHO Database

The MACHO project monitored the Magellanic Clouds for the purpose of detecting microlensing events between 1992 July and 2000 January (Alcock et al., 1997, 2000). The Mount Stromlo Observatory 1.27-meter telescope system provided simultaneous imaging in a red ($`\lambda \lambda 5900`$$`7800\text{Å}`$) and blue ($`\lambda \lambda 4370`$$`5900\text{Å}`$) filter, over a 0.5 $`\mathrm{}^{}`$ field of view with a scale of $`0.63^{\prime \prime }`$ per pixel. We monitored 82 fields (35 $`\mathrm{}^{}`$) in the LMC, and 6 fields (2.5 $`\mathrm{}^{}`$) in the SMC; the location of these fields is shown in Figures 1 and 2. Average sampling frequencies varied from 2 to 10 days between fields. Exposure times were 300-s and 600-s for the LMC and SMC, respectively. Photometric transformations from MACHO passbands to standard $`V`$\- and $`R`$-band magnitudes proceeded using the calibrations discussed in Alcock et al. (1999). Since the MACHO passbands are non-standard and these photometric transformation were determined for stars and not for emission-line quasars, the $`(VR)`$ quasar colors in this paper should be approached with caution. We consider only measurements with photometric errors less than 5%; the average MACHO quasar lightcurve contains 600 good photometric measurements over 7.5 years.

Selection of the quasar candidates, described below, was performed on the first 5.7 years of MACHO data; the final 7.5-year MACHO light curves are presented in the lightcurve analysis of § 4. Due to limited data access at the time of selection in the outer LMC MACHO fields, the variability search discussed in § 2.2 was spatially restricted to the SMC and 30 MACHO LMC fields. In § 2.3, the full spatial coverage of the MACHO database was searched for variable counterparts to known radio and X-ray sources. The final MACHO Magellanic Cloud database, 37.5$`\mathrm{}^{}`$ over 7.5 years, has recently become readily accessible and variability selection will be run on the outer LMC fields not analysed in this paper.

### 2.2 Quasar Candidate Variability Selection

At the time of candidate selection, the long-term optical photometric behavior of quasars was not adequately constrained to fully automate quasar selection in the MACHO database. Instead, the selection method was designed to automatically reject known classes of variable stars, with the final step being a selection by eye. The MACHO database contained 9 Active Galactic Nuclei (AGN) listed in Table 1 which had been previously cross-identified with X-ray sources by Schmidtke et al. (1999) and one AGN which was serendipitously discovered by Blanco & Heathcote (1986). Two additional sources in the MACHO database were presented by Dobrzycki et al. (2002) subsequent to candidate selection. Lightcurves for these sources, shown in Figure 3, provided a training set around which the selection method was developed. The final subjective step was to select, by eye, lightcurves similar to these known sources. Since our goal was to identify a robust set of quasars, rather than a complete census of quasars behind the Clouds, we deemed this level of subjectivity to be acceptable.

Variability selection was run on 30 MACHO LMC fields (15$`\mathrm{}^{}`$) containing 12 million objects and 6 MACHO SMC fields (2.5$`\mathrm{}^{}`$) containing 2 million objects. Candidate selection began with the Level 1 MACHO database, a data subset containing 140,000 objects flagged as having a significant deviation from a constant brightness lightcurve (Alcock et al., 2000). We required objects to have a minimum of 50 photometric measurements in $`V`$\- and $`R`$-bands. Weighted average magnitudes were calculated from the standard equation:

$$\overline{V}\underset{i=1}{\overset{N}{}}\frac{V_i}{\sigma _{V,i}^2}/\underset{i=1}{\overset{N}{}}\frac{1}{\sigma _{V,i}^2}.$$
(1)
where $`N`$ is the total number of individual photometric measurements $`V_i`$ with associated errors $`\sigma _{V,i}`$. We considered candidates between $`16\overline{V}20`$ which is one magnitude brighter (fainter) than the MACHO photometric completeness (saturation) limits. Candidates were required to have weighted average colors bluer than $`(\overline{VR})1.0`$. This color cut eliminated long-period quasi-periodic variable stars, while retaining all of the training set AGNs. An example lightcurve of a long period variable is shown in the top right panel of Figure 4; the majority of these stars are extremely red and otherwise difficult to remove from the final quasar candidate list.

Two statistics were used to quantify the amount of lightcurve variability. First, the intrinsic variability for each candidate quasar lightcurve was calculated as:

$$\widehat{\sigma _V}\sqrt{\frac{\left(V_i\overline{V}\right)^2}{N1}\frac{\sigma _{V,i}^2}{N}}$$
(2)
This quantity is an estimate of the true source variability in the absence of photometric errors. The first term is the total variance measured from the lightcurve data, while the second is an estimate of the variance due to photometric measurement errors alone. We note that the photometric error estimate supplied by the photometry code Sodophot (Alcock et al., 1997) is known to have some bias for bright stars. This bias is on the order of 0.01 magnitudes and should have only a small effect on the current data. Giveon et al. (1999) monitored a sample of 42 quasars monthly for 7 years, measuring intrinsic variabilities between $`0.05\widehat{\sigma _B}0.32`$ in the $`B`$-band. We therefore require the intrinsic variability of MACHO candidate quasars to be larger than 0.05 magnitudes ($`\widehat{\sigma _V}0.05`$). The second variability statistic calculated for each lightcurve is the variability index (Welch & Stetson, 1993). This index is a measure of correlated variability between the MACHO $`V`$\- and $`R`$-bands, defined as:

$$I\sqrt{\frac{1}{N(N1)}}\underset{i=1}{\overset{N}{}}\left(\frac{V_i\overline{V}}{\sigma _{V,i}}\right)\left(\frac{R_i\overline{R}}{\sigma _{R,i}}\right)$$
(3)
This quantity approaches zero for uncorrelated variability. Quasar variability is expected to be highly correlated between the MACHO passbands; we require $`I1.5`$ for our candidates. This limit was set slightly below the minimum $`I`$-value determined from the training set AGN. Due to MACHO noise characteristics the two variability statistics described above are not redundant. Systematic noise terms in the MACHO system which affect a single filter can cause large $`\widehat{\sigma _V}`$ values, but may be eliminated as this variability is not correlated in the second filter. Conversely, variable observing conditions, such as seeing and sky brightness, can cause correlated variability, but these measurements often have large photometric errors and can be rejected based on our $`\widehat{\sigma _V}`$ cut.

Periodic variable stars, such as Cepheid and RR Lyrae stars, were removed using the MACHO Variable Star Catalogue. This catalogue contains period information for the majority of variable MACHO objects as determined from a super-smoother algorithm which models folded lightcurves (Cook et al., 1995). We reject as candidate lightcurves for which a period ($`\tau `$) was found at high significance in both passbands over the range $`0.1\tau 500`$ days. This cut did not include aliased frequencies ($`\tau =1/n`$ days, $`n`$=1,2,..). An example lightcurve of a typical RR Lyrae star in the MACHO database rejected by our periodicity cut is shown in the top right panel of Figure 4.

In the final quasar candidate selection step, each candidate lightcurve was examined by eye to remove objects with spurious noise characteristics or quasi-periodic components. Roughly 2500 light curves were examined by eye; a total of 360 lightcurves were considered candidate quasars. A fraction of lightcurves rejected by eye were due to noise effects above the thresholds set by our variability cuts. However, the majority of rejected candidates were quasi-periodic lightcurves characteristic of blue variable stars, known to the microlensing community as a ’Bumper’ stars (Cook et al., 1995). An example of such a lightcurve is shown in the bottom left panel of Figure 4. These stars typically have strong Balmer emission lines at the velocity of the Clouds and are associated with the Be star phenomena (Keller et al., 2002). These blue variables often have quasi-repeatable outbursts and can be eliminated from the candidate list. As designed, our quasar selection technique successfully recovered all of the previously known quasar/AGNs in the search region.

### 2.3 Additional Candidate Selection Methods

We have additionally searched for optically-variable counterparts in the error boxes of suspected extragalactic radio and X-ray sources in several Magellanic Cloud surveys. This allowed us to extend our search to the full spatial coverage of the MACHO database (37.5$`\mathrm{}^{}`$), as explained in § 2.1. In the LMC, we have searched the LMC radio catalogues of Marx, Dickey & Mebold (1997) and Filipovic et al. (1998) and the X-ray catalogue of Haberl & Pietsch (1999); in the SMC we have searched the radio catalogue of Filipovic et al. (1997) and the X-ray catalogues of Kahabka et al. (1999) and Sasaki, Haberl & Pietsch (2000). Photometric constraints, described in the previous section, are relaxed in this search: any aperiodic MACHO variable ($`\widehat{\sigma _V}>0`$) inside the $`1\sigma `$ spatial error box of a cataloged source (typically $`15^{\prime \prime }`$) is considered a candidate. We identified variable, aperiodic MACHO counterparts in the $`1\sigma `$ error boxes for $`5\%`$ of the cataloged objects. In the last column of Tables 2 and 3, we note which quasars were identified by this method.

## 3 Spectroscopic Confirmation of 47 MACHO Quasars

Follow-up spectroscopic observations for our quasar candidates were obtained with the Anglo-Australian Telescope and 2dF multifiber spectrograph (AAT+2dF) in 1999 October and 2001 January. Additional observations were made with the Australian National University 2.3m and Double Beam Spectrograph (ANU+DBS) over 8 nights between 1999 March and 2000 November. The AAT+2dF is a fiber-fed spectrograph with $`2^{\prime \prime }`$ diameter fibers and 200 fibers available per pointing. These observations were made through the 300B grating covering $`\lambda \lambda 3800`$$`7800\text{Å}`$ with $`4.3\text{Å}`$ pixels. The 2dF data were reduced using the standard 2dFdr reduction pipeline software (Bailey, Glazebrook & Bridges, 2002). Observations with the ANU+DBS were made through a single, $`2^{\prime \prime }`$ wide slit in combination with a low resolution $`2.2\text{Å}`$ per pixel blue grating ($`\lambda \lambda 3500`$$`6000\text{Å}`$) and a red $`4.0\text{Å}`$ per pixel grating ($`\lambda \lambda 6000`$$`9000\text{Å}`$). These data were reduced with IRAF single long-slit spectra reduction procedures. A total of 259 candidate quasars were observed: spectra for 220 candidates were obtained in six separate AAT+2dF pointings, 39 candidates were observed in single pointing with the 2.3m+DBS. The remaining $`100`$ candidates will be observed in future observing runs.

Spectroscopic follow-up revealed a total of 47 previously unknown quasars behind the Magellanic Clouds: 38 behind the LMC and 9 quasars behind the SMC. The quasars cover the redshift interval $`0.2<z<2.8`$ and range in apparent magnitude between $`16.6\overline{V}20.1`$ mag. For the majority of objects, redshifts were determined from two or more broad lines; rest-frame spectra for all 47 newly discovered quasars are shown in Figure 5. All objects appear unresolved in MACHO images. Absolute magnitudes were computed assuming a consensus cosmology of $`\mathrm{\Omega }_m=0.3`$, $`\mathrm{\Omega }_\mathrm{\Lambda }=0.7`$ and Ho = 75 km s-1Mpc-1 and are corrected for reddening. Values for reddening vary in the Magellanic Clouds due to patchy dust distribution, and accurate estimates do not yet exist in the directions of all of our quasars. We instead adopted, for each Cloud, a single reddening value of $`E(BV)=0.12`$ and $`0.05`$ (Dutra et al., 2001) for the LMC and SMC, respectively, and a Galactic extinction law.

The spatial distribution of the discovered MACHO quasars is shown relative to the Magellanic Clouds in Figures 1 and 2. In the LMC, quasars appear concentrated to the South of the LMC bar due to several 2dF spectroscopic pointings in this region. Given that $`100`$ quasar candidates have not yet been spectroscopically followed up in this region, and subjectivity in the candidate selection process, our quasar sample is unlikely to be complete. In Tables 2 and 3 we list for each source a MACHO ID number, equatorial coordinates $`\alpha `$(J2000) and $`\delta `$(J2000), weighted average apparent $`\overline{V}`$ magnitude and $`(\overline{VR})`$ color, the redshift, z, the mean absolute magnitude, $`M_V`$, and the number of $`V`$-band photometric measurements, $`n_V`$, available in the MACHO database. We also note if the object was selected as a candidate based on optical variability inside the error box of a suspected extragalactic radio and X-ray source. Histograms of the quasars, distributed as a function of redshift, apparent and absolute magnitude, are shown in Figure 8.

### 3.1 Candidate List Contamination: Be/Ae Stars

The primary contamination during spectroscopic follow-up of our quasar candidates were emission-line main sequence stars (Be/Ae stars) in the Magellanic Clouds. These stars display strong Balmer emission/absorption lines at the velocity of the Clouds and are known to be photometrically variable (Hubert & Floquet, 1998). Of the 258 quasar candidates observed, 188 were emission-line Be/Ae stars. The brightest ($`V16.5`$), more well studied, emission-line stars have a strong periodic component to their lightcurves (‘Bumpers’; Cook et al., 1995) and were already removed from the quasar candidate list. However, fainter Be/Ae stars appear to be quasi- to aperiodic variables and were thus included as quasar candidates. An example Bumper light curve is compared to a fainter Be/Ae star in the bottom panels of Figure 4. These objects have very similar spectra, despite significantly different lightcurve behavior. A preliminary analysis of this type of blue variable star is presented in Keller et al. (2002).

## 4 MACHO Quasar Lightcurves

$`V`$-band lightcurves for all quasars listed in Tables 1, 2 and 3 are presented in Figures 3, 6, and 7. The lightcurves have on average 600 photometric measurements in both $`V`$\- and $`R`$-band, spanning 7.5 years. The zero point of the time axis of these plots corresponds to JD 2448623.5, or UT 1992 January 2.0. We have searched for close quasar pair candidates in a $`15^{\prime \prime }`$ radius around each source, but find no aperiodic lightcurves at these distances. We note that, unlike the previously discovered sources listed in Table 1 which are predominately AGN, the majority of MACHO sources would be classified as quasars based on the usual absolute luminosity criteria of $`M_B=23`$ (strict classification is prohibited by the fact that we determine $`M_V`$ rather than $`M_B`$ magnitudes).

Similar to the results of Giveon et al. (1999), we find that the majority of quasars become bluer in $`(VR)`$ as they brighten. To quantify this, we calculate the Spearman’s rank correlation probability ($`P_r`$) between magnitude and color measurements for each source. The correlation is in the same sense for all quasars (bluer $`VR`$ colors at brighter $`V`$ magnitudes), and is highly significant at a $`4.5\sigma `$ level or greater ($`P_r<3\times 10^5`$) for 95% of the quasar lightcurves. In contrast, the majority (63%) of contaminating Be/Ae stars in our spectroscopic sample became redder as they brightened at similar significance levels. This distinction will be used to improve future quasar selection criteria.

In Figure 9, the $`V`$-band intrinsic variability, as defined in Eqn. 2, is plotted as a function of quasar absolute luminosity and redshift. For the more homogeneous subset of quasars discovered via our variability-only method (Fig. 9, solid points), we find according to the Spearman’s rank test, a very weak correlation at the $`2.2\sigma `$ level between variability and absolute luminosity ($`\widehat{\sigma _V}`$ \- $`M_V`$) in the sense that intrinsically luminous quasars tend to be less variable. For the full set of objects shown in Figure 9, the same correlation between $`\widehat{\sigma _V}`$ \- $`M_V`$ was more significant at the $`3.3\sigma `$ level. No correlation was found between the intrinsic source variability and redshift ($`\widehat{\sigma _V}`$ \- $`z`$) for our quasar subset. For the full set, a weak negative correlation between variability and redshift is detected at the $`2.5\sigma `$ level. Several groups have claimed a similar correlation between variability and absolute luminosity (Hook et al., 1994; Cristiani et al., 1997; Giveon et al., 1999), however, both positive and negative correlations have been claimed between variability and redshift. These results are difficult to interpret due to strong correlations between redshift and absolute luminosity, as well as varying definitions of variability. The quasar light curves presented in this paper have sufficient time resolution to allow power spectrum and other detailed lightcurve analyses. It is hoped that such work will be easier to interpret and have interesting implications for the physical mechanisms driving the AGN/quasar variability.

## 5 Discussion and Summary

We present 47 quasars discovered behind the Magellanic Clouds: 38 behind the LMC and 9 behind the SMC, significantly increasing the number density of known quasars in this region. The quasars cover the redshift interval $`0.2<z<2.8`$ and apparent mean magnitudes $`16.6\overline{V}20.1`$. Candidate quasars were identified based on aperiodic variability in the MACHO database. MACHO light curves are presented for the newly discovered quasars as well as 12 quasar/AGNs identified in previous studies. The primary contamination during spectroscopic follow-up were quasi- or aperiodic Be/Ae stars in the Magellanic Clouds. Spectroscopic follow-up of quasar candidates in the MACHO database is not yet complete. In the outer LMC, 52 MACHO fields have become accessible for variability-only (§ 2.2) selection since the original candidate selection was run. In addition, $`100`$ candidates have not yet been followed-up from the search presented in this paper. We therefore expect the MACHO database to yield many more sources in the future.

A similar photometric variability selection has been applied to another microlensing database in the Magellanic Clouds, OGLE-II (Eyer, 2002), but has not yet been followed-up spectroscopically. We have checked our sample of quasars against the OGLE candidate list presented by Eyer. Four of the MACHO quasars are listed as candidates in this paper, (OGLE candidates: L92, L114, L155, S12), eight OGLE candidates are within $`1^{\prime \prime }`$ of spectroscopically confirmed Be stars (L51, L87, L103, L121, L148, L153, S8, S25) and six OGLE candidates are common to our list which have not yet been followed-up spectroscopically. Despite similar quasar candidate selection strategies, the majority of the OGLE candidates did not make our candidate list. This is due in part to our final subjective rejection of Be/Bumper lightcurves: 24 objects classified as quasar candidates by Eyer were considered Be/Bumper star candidates according to MACHO photometry; the remaining objects in the OGLE list either did not pass our minimum variability cut or fell outside MACHO fields. Continued follow-up of both MACHO and OGLE candidates is certain to increase significantly the number quasars in the Magellanic Cloud region.

Quasars behind the Magellanic Clouds are extremely useful tools with which to study the Clouds themselves. Our motivation for this study was to uncover a robust set of reference objects against which to measure the proper motion of the Magellanic Clouds. First epoch Hubble Space Telescope images have been scheduled for a subset of quasars presented in this paper; second epoch imaging is expected to allow an estimation of the Cloud’s orbital motion with sufficient accuracy to constraint models of the Galactic halo. Quasars are also invaluable tools for a variety of other studies, for example as probes of the Clouds’ interstellar medium. We therefore provide finding charts, lightcurves and spectra for all quasars presented in this paper, available electronically at http://www.ucolick.org/$``$mgeha/MACHO or on request from the authors.

We would like to thank Terry Bridges for help with 2dF observations and reductions. This work was performed under the auspices of the U.S. Department of Energy, National Nuclear Security Administration by the University of California, Lawrence Livermore National Laboratory under contract No. W-7405-Eng-48. DM is supported by FONDAP Center for Astrophysics 15010003. MG was supported in part by a grant from IGPP-LLNL UCRP.