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# Dynamical Properties in the Bilayer Quantum Hall Ferromagnet

## Abstract

The spectral functions of the pseudospin correlation functions in the bilayer quantum Hall system at $`\nu =1`$ are investigated numerically, where the pseudospin describes the layer degrees of freedom. In the pseudospin-ferromagnetic phase, the lowest-energy excitation branch is closely connected with the ground state through the fluctuations of pseudospin $`S_y`$ and $`S_z`$, and it plays a significant role on the tunneling properties in this system. For the system with very small tunneling amplitude and layer separation smaller than the critical one, the system-size dependence of calculated spectral function $`A_{yz}`$ suggests the superfluidity on the tunneling current in the absence of impurities.

Recently the bilayer quantum Hall (QH) system  has often been investigated from the viewpoint of quantum ferromagnetism. In fact, the pseudospin can be introduced to this system by a simple definition of assigning the upper/lower layers to the pseudospin $`/`$ , and the pseudospin ferromagnetism can be realized for the total Landau level filling $`\nu =1/m`$ ($`m`$: odd integers). In particular, the $`\nu =1`$ bilayer QH system has extensively been studied both experimentally and theoretically .

The pseudospin rotational symmetry in this system is degraded because of the difference between the intralayer and interlayer Coulomb interaction for a finite layer separation $`d`$ (and of the interlayer tunneling). Since the two layers tend to have equal numbers of electrons to reduce the interaction energy, the $`z`$ component of the total pseudospin (half the difference in the numbers) tends to vanish, $`S_z=0`$, in the ground state. Thus the pseudospin will lie in the $`xy`$ plane in the pseudospin space, where the system maintains an invariance under rotations about the $`z`$ axis, i.e., the SU(2) symmetry is reduced to U(1) .

The electron correlation alone pushes the ground state for $`\nu =1/m`$ towards a ferromagnetic one , so the bilayer $`\nu =1/m`$ QH system behaves like an easy-plane itinerant-electron ferromagnet. The U(1) symmetry is further degraded in the presence of the interlayer tunneling, since the tunneling amplitude behaves like a magnetic field acting on the pseudospin, as seen in the tunneling Hamiltonian, $`H_\mathrm{T}=\mathrm{\Delta }_{\mathrm{SAS}}S_x`$. Here $`\mathrm{\Delta }_{\mathrm{SAS}}`$ is the energy difference between the symmetric and antisymmetric combinations of isolated layer states and is proportional to the interlayer-tunneling amplitude .

So a bilayer QH system is characterized by two dimensionless parameters, $`d/l`$ and $`\mathrm{\Delta }_{\mathrm{SAS}}/(e^2/ϵl)`$ ( $`l`$: the magnetic length, $`ϵ`$: dielectric constant of the host material ). For $`\nu =1`$, the phase diagram against these two parameters is obtained experimentally , and the diagram shows that the QH state disappears for $`d>d_c`$ and that the critical separation $`d_c`$ increases as $`\mathrm{\Delta }_{\mathrm{SAS}}`$ increases.

Within this QH effect region, the ground state for $`\nu =1`$ evolves continuously from tunneling-dominated (single-particle like) to correlation-dominated (many-body like) as $`\mathrm{\Delta }_{\mathrm{SAS}}`$ is decreased, and there is no intervening non-ferromagnetic region between the two regimes . Moreover, within this pseudospin-ferromagnetic region, the ground-state wavefunction is analytically given as a spin-squeezed state , where the fluctuation $`\mathrm{\Delta }S_z`$ is supressed by the electron correlation.

By using a sample with very weak interlayer tunneling ($`\mathrm{\Delta }_{\mathrm{SAS}}/(e^2/ϵl)10^6`$), Spielman et al have recently showed the huge resonant enhancement of the zero bias tunneling conductance . The possibility of the excitonic superfluidity was also discussed because of the tunneling spectroscopy reminiscent of the Josephson effect, of which controvertial predictions have been done . Very recently, further tunneling-spectroscopy measurements were performed with the in-plane magnetic field applied to the system, and the observation of a linearly-dispersing Goldstone mode in a bilayer QH ferromagnet was claimed . This in-plane field effect has been discussed in some theoretical papers .

In case of very weak interlayer tunneling as realized in these experiments , the U(1) symmetry of the system is expected to recover almost completely. Some simple model systems with this symmetry have been investigated and the tunneling properties have been discussed . The Chern-Simons Landau-Ginzburg approaches for bilayer QH systems  were also performed for the case of vanishing interlayer tunneling.

On the other hand, some discussions based a BCS-like wavefunction with a phase variable $`\varphi `$, which determines the orientation of the pseudospin magnetic moment, have also been done . This wavefunction, however, is compatible with the SU(2) symmetry, and does not reflect the U(1) symmetry of the system as well as the Hartree-Fock approximation does not. Thus an approach that fully reflects the system’s symmetry and takes small (but non-zero) tunneling amplitudes into consideration has yet to come for the study of the tunneling-current properties in this system. That is exactly the purpose of the present paper.

By the exact diagonalization method for small-size systems, we obtain the spectral functions of pseudospin correlation functions numerically. We show that in the pseudospin-ferromagnetic phase the lowest-energy excitation branch is closely connected with the ground state through the fluctuations of pseudospin $`S_y`$ and $`S_z`$, and that it plays a significant role for the tunneling properties in this system. For the system with very small tunneling amplitude and layer separation smaller than the critical one, the system-size dependence of calculated spectral function $`A_{yz}`$ suggests the superfluidity on the tunneling current in the absence of impurities.

Our numerical calculations were done for bilayer spherical systems , where each surface of the spheres is passed through by $`2S`$ flux quanta. For the case of $`\nu =1`$ we consider in this paper, $`2S=N1`$ for $`N`$-electron systems. In terms of annihilation and creation operators for the $`m`$-th spatial orbit in the lowest Landau level with pseudospin $`\sigma `$, the total pseudospin operators are given as $`S_z=_m(a_m^{}a_ma_m^{}a_m)/2`$, $`S_x=_m(a_m^{}a_m+a_m^{}a_m)/2`$, $`S_y=_m(a_m^{}a_ma_m^{}a_m)/2i`$. Pseudospin $`S_x`$ and $`S_z`$ are related with the interlayer-tunneling and interlayer-voltage part of the Hamiltonian, respectively, as $`H_\mathrm{T}=\mathrm{\Delta }_{\mathrm{SAS}}S_x`$ and $`H_\mathrm{V}=eVS_z`$. Pseudospin $`S_y`$ is related with the interlayer current $`I`$ as $`I\mathrm{\Delta }_{\mathrm{SAS}}S_y`$. Our calculations were performed for the cases of zero interlayer voltage ($`V=0`$).

The spin density operators are given as $`S_z(𝛀)=[\mathrm{\Psi }_{}^{}(𝛀)\mathrm{\Psi }_{}(𝛀)\mathrm{\Psi }_{}^{}(𝛀)\mathrm{\Psi }_{}(𝛀)]/2`$, $`S_x(𝛀)=[\mathrm{\Psi }_{}^{}(𝛀)\mathrm{\Psi }_{}(𝛀)+\mathrm{\Psi }_{}^{}(𝛀)\mathrm{\Psi }_{}(𝛀)]/2`$, $`S_y(𝛀)=[\mathrm{\Psi }_{}^{}(𝛀)\mathrm{\Psi }_{}(𝛀)\mathrm{\Psi }_{}^{}(𝛀)\mathrm{\Psi }_{}(𝛀)]/2i`$, where a unit vector $`𝛀`$ denotes a position on each sphere. Their ‘Fourier transforms’ are given by $`S_{LM}^\alpha =𝑑𝛀Y_{LM}(𝛀)S_\alpha (𝛀)`$, where $`\alpha =x,y,z`$, and $`Y_{LM}(𝛀)`$ is a spherical harmonics for angular momentum $`L`$ and its $`z`$-component $`M`$. In particular, the components for $`L=M=0`$ are related with the pseudospin operators as $`S_{00}^\alpha =S_\alpha /\sqrt{4\pi }`$.

The spectral functions  of pseudospin correlation functions at zero temperature are given as

$`A_{\alpha \beta }(L,\omega )`$ $`=`$ $`{\displaystyle \underset{i}{}}\mathrm{\Phi }_0|\left(S_{LM}^\alpha \right)^{}|\mathrm{\Phi }_i\mathrm{\Phi }_i|S_{LM}^\beta |\mathrm{\Phi }_0`$ (2)
$`\times \delta (\omega E_i+E_0),`$
where $`|\mathrm{\Phi }_0`$ and $`|\mathrm{\Phi }_i`$ are the ground state and the $`i`$-th eigenstate of the Hamiltonian, respectively. The diagonal element $`A_{\alpha \alpha }(L,\omega )`$ among these spectral functions is real and non-negative because of their definitions in Eq. (2). Among the off-diagonal elements, $`A_{yz}(L,\omega )`$ is closely related with the finite-wavevector conductance $`g`$ on the interlayer current because $`g(L,\omega )i^1\mathrm{\Delta }_{\mathrm{SAS}}A_{yz}(L,\omega )`$ from the Kubo formula. We note that $`A_{yz}(L,\omega )`$ is purely imaginary and that the spectral functions in Eq. (2) are independent of $`M`$ because of the rotational symmetry of the system.

Table I shows the fluctuations of pseudospin $`S_z`$ and expectation values of pseudospin $`S_x`$ in the $`\nu =1`$ ground state for $`N=10`$, $`d/l=1.0`$, and $`t\mathrm{\Delta }_{\mathrm{SAS}}/(e^2/ϵl)=10^4`$, $`10^5`$, $`10^6`$. For such small $`\mathrm{\Delta }_{\mathrm{SAS}}`$, the values are proportional to $`\mathrm{\Delta }_{\mathrm{SAS}}`$, because $`\mathrm{\Delta }_{\mathrm{SAS}}`$ is proportional to the interlayer tunneling amplitude and behaves like a magnetic field along the $`x`$ axis in the pseudospin space. Table I indicates that the U(1) symmetry in the easy-plane ferromagnet is recovered almost completely in case of very small $`\mathrm{\Delta }_{\mathrm{SAS}}`$. In fact, for $`t10^3`$, intra- and inter-layer correlations between electrons in the ground state are found to be little dependent on the value of $`t`$. On the other hand, the interlayer-tunneling features are strongly dependent on it.

In Fig. 1, the excitation spectra and spectral functions in the $`\nu =1`$ bilayer QH system are shown for $`N=10`$, $`d/l=1.0`$, and $`t=10^6`$. The excitation spectra are shown by open circles in Fig. 1(a). In Fig. 1(b) and (c), the strength for each excitation in the spectral functions $`A_{yy}(L,\omega )`$ and $`A_{zz}(L,\omega )`$ is shown against the angular momentum $`L`$ and excitation energy $`\omega `$ by the area of the corresponding circle, respectively. We note that the energy is measured from the ground-state energy and that the unit is $`e^2/ϵl`$.

The lowest-energy excitation branch can be seen for $`0L3`$ in Fig. 1(a). We made sure that the energy values in this branch (in particular, the one for $`L=0`$) are quite dependent on the system size $`N`$ and that these ones decrease as $`N`$ increases. This branch is expected to be seen as a linearly-dispersing excitation mode  for sufficiently large $`N`$ and very small $`\mathrm{\Delta }_{\mathrm{SAS}}`$. This pseudospin-wave excitation branch is closely connected with the ground state through the fluctuations of pseudospin $`S_y`$ and $`S_z`$.

As seen in Table I, the U(1) symmetry is recovered almost completely for $`t10^4`$. In fact, we made sure that the result for the spectral function $`A_{xx}`$ is almost the same as that for $`A_{yy}`$ shown in Fig. 1(b), and that each pair of excited states corresponding to $`A_{xx}`$ and $`A_{yy}`$, respectively, is nearly degenerate. On the other hand, as seen in Fig. 1(c), most of the spectral weights for $`A_{zz}`$ are occupied by the lowest-energy excitation branch. This is also the case for $`A_{yz}`$, because $`A_{yz}`$ and $`A_{zz}`$ include the same factor for each term in Eq. (2).

In Table II, the strength of $`i^1A_{yz}(L,\omega )`$ in the lowest-energy excitation branch in the $`\nu =1`$ pseudospin ferromagnet is shown for $`N=10`$, $`d/l=1.0`$, and $`t=10^4`$, $`10^5`$, $`10^6`$. It indicates that these values of strength are proportional to $`t`$, i.e., to $`\mathrm{\Delta }_{\mathrm{SAS}}`$. Thus the tunneling conductance is considered to be proportional to the square of $`\mathrm{\Delta }_{\mathrm{SAS}}`$, because $`g(L,\omega )i^1\mathrm{\Delta }_{\mathrm{SAS}}A_{yz}(L,\omega )`$. It is also found that the strength increases as angular momentum $`L`$ decreases. That is, the long-wavelength part of the pseudospin-wave excitation mode plays a significant role on the interlayer-tunneling properties in this system.

In Table III, the strength of $`i^1A_{yz}(L,\omega )/t`$ in the lowest-energy excitation branch in the $`\nu =1`$ pseudospin ferromagnet is shown for $`d/l=1.0`$, $`L=0`$, $`1`$, $`2`$, and $`N=6`$, $`8`$, $`10`$. It has a system-size dependence varying approximately as $`N^\lambda `$ ($`\lambda 3`$). This is also the case for $`d/l=0.5`$. For larger layer separations such as $`d/l=1.5`$ and $`2.0`$, however, such a system-size dependence is not obtained. In fact, for $`d/l=1.5`$ and $`2.0`$, the strength increases or decreases as $`N`$ increases, and the system-size dependence is much weaker than that for $`d/l=0.5`$ and $`1.0`$.

For sufficiently small $`\mathrm{\Delta }_{\mathrm{SAS}}`$ ( $`0.01e^2/ϵl`$ ), it is known that the pseudospin ferromagnetism is destroyed for layer separation $`d`$ larger than the critical one $`d_c1.3l`$ . Among the values of layer separation adopted by us, $`d/l=0.5`$ and $`1.0`$ belong to the case of $`d<d_c`$, and $`d/l=1.5`$ and $`2.0`$ satisfy $`d>d_c`$. As mentioned above, our results for $`d<d_c`$ show a system-size dependence of the spectral function $`A_{yz}`$ varying approximately as $`N^\lambda `$ ($`\lambda 3`$), which is much stronger than usual $`N`$-linear dependence. On the other hand, the possible superfluidity on the tunneling current in this system is considered to show an $`N`$-square dependence. It is not clear whether this discrepancy between our result and predicted one results from small system sizes in our calculations or not. At least, however, the system-size dependence of $`A_{yz}`$ in our results is much stronger than $`N`$-linear one and so suggests the superfluidity on the tunneling current in the absence of impurities. For clarifying interlayer tunneling properties in this system, further studies of the impurity effects  and numerical calculations for larger systems are desired.

For $`d>d_c`$, such a strong system-size dependence does not appear in our numerical results. Significant differences between the two cases of $`d>d_c`$ and $`d<d_c`$ are expected to become clearer in larger systems because of the differences in the system-size dependence. These qualitative differences between the two cases are consistent with the results in a recent experiment . Lastly we note that the spectral weights of $`i^1A_{yz}`$ occupied by the lowest-energy excitation branch decrease rapidly as the layer separation increases.

The author thanks Allan H. MacDonald, John Schliemann, and Yogesh Joglekar for fruitful discussion with them. He is also grateful to Hisatoshi Yokoyama for valuable conversations on spectral functions, and to Anju Sawada for valuable experimental information about the bilayer QH system. He was supported for the research in the USA by Japan Society for the Promotion of Science.


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# Pulsar motions from neutrino oscillations induced by a violation of the equivalence principle

## I Acknowledgments

This work was partially supported by CONICET-Argentina, CONACYT- México, Universidad Nacional Autónoma de México under grants DGAPA-IN117198 and DGAPA-IN100397, and Centro Latino Americano de Física. M. B. also acknowledges support from SRE (México).


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# Discovery of Associated Absorption Lines in an X-Ray Warm Absorber: HST-FOS Observations of MR2251-1781footnote 11footnote 1Based on Observations with the NASA/ESA Hubble Space Telescope, obtained at the Space Telescope Science Institute, which is operated by AURA, Inc., under NASA contract NAS 5-26555.

## 1 Introduction

Absorption due to O VII and O VIII in the X-ray and O VI in the UV can in some cases be modeled by a single UV/X-ray absorber (Mathur 1994; Mathur, Wilkes, & Elvis 1998), offering a unique way to determine the physical conditions of the absorbing material in active galactic nuclei (AGNs). As more X-ray/UV absorbers have been found (e.g., Mathur 1994; Mathur, Elvis, & Wilkes 1995; Mathur, Elvis, & Singh 1995; Mathur, Wilkes, & Aldcroft 1997; Shields & Hamann 1997; Mathur et al. 1998; Hamann, Netzer, & Shields 2000) it has become clear these share common characteristics. Though not all of these absorbers can be readily modeled by a single zone, all are composed of highly ionized, low density, high column density, outflowing gas sitting outside the broad emission line region (BELR). The X-ray/UV absorbers are therefore an important nuclear component of AGNs, representing a wind or outflow carrying away significant kinetic energy at a mass-loss rate comparable to the accretion rate needed to power the AGN (Mathur et al. 1995). The properties of these absorbers can be invoked in AGN models developed to explain such outflows (see Elvis 2000 and references therein), and will aid in expanding such models into a wider unification scenario (Elvis 2000).

It remains to be determined how common X-ray/UV absorbers are. In a sample of eight Seyfert galaxies, Crenshaw et al. (1999) found six of them showed both UV and X-ray absorption, strengthening the UV/X-ray connection. The question remains whether X-ray absorbers are physically related to UV absorbers in all AGN (two of the Seyferts of the Crenshaw et al. sample were not X-ray warm absorbers and showed no UV absorption), or, if not, in what fraction of cases does the unified model apply. To help answer these questions, we initiated an HST program to search for UV absorption in two radio-quiet QSOs with known X-ray warm absorbers.

Mathur et al. (1998) reported UV absorption in the first of these objects, PG1114+445. Here we present the detection of UV absorption in our second candidate, MR2251$``$178, a low-redshift ($`z_{em}=0.0640`$) radio-quiet QSO. In addition to being the first X-ray selected QSO (Ricker et al. 1978), MR2251$``$178 was the object for which Halpern (1984) originally suggested the presence of partially ionized, optically thin material: the X-ray warm absorber.

In §2 we describe the HST observations and the analysis of the UV absorption lines. Section 3 relates the UV absorption to the X-ray absorption seen in ASCA data analyzed by Reynolds (1997) and presents some simple physical quantities based on the assumption that the UV and X-ray absorbers are the same. We present our conclusions in §4.

## 2 The HST spectra

On 1996 February 2, MR2251$``$178 was observed using three gratings of the Faint Object Spectrograph onboard HST. The target was centered in the 1” circular aperture through a four step peak-up sequence to ensure a pointing accuray of 0$`\text{ .}^{\prime \prime }`$12. Two exposures totalling 5740s were obtained using the G130H grating and blue side of the detector. The exposures using the red side and the G190H and G270H gratings were 1730s and 300s, respectively.

The data were reduced using the standard pipeline processing and calibration files, and the individual G130H spectra were combined. The final spectra are shown in Figure 1. Absorption lines of  Ly$`\alpha `$, C IV and N V can be clearly seen, as predicted from the X-ray/UV models. The strong absorption lines of  Ly$`\alpha `$ and C IV are superposed on the emission lines of  Ly$`\alpha `$ and C IV. Weaker absorption due to the N V doublet is seen against the continuum; no measurable N V emission is present. The spectra do not show absorption due to low-ionization Mg II indicating the X-ray absorber is highly ionized.

There is an inherent uncertainty involved in measuring an absorption line lying on top of a broad emission line profile because the unabsorbed shape of the emission line is unknown. We therefore used two methods to measure the line equivalent widths (EWs) as in Mathur et al. (1998). We made an initial measurement using the IRAF SPLOT task to fit Gaussians across the absorption in the emission line profiles. A single Gaussian was used for  Ly$`\alpha `$ and N V lines, and the C IV doublet is deblended into two Gaussians. Results for the EWs and FWHMs are listed in Table 1. We estimate the errors on the EWs for  Ly$`\alpha `$ and C IV to be $``$40%. The continuum is more readily determined on either side of the N V lines, hence the error on the SPLOT measurement is estimated at $``$10%. The C IV and N V doublet ratios are both $``$1.7, so the doublets may be partially saturated, though not as severely as in PG1114+445. Higher resolution spectra would be needed to address the degree of saturation. Also, though it is probable the individual lines will break into multiple components at higher resolution (Ly$`\alpha `$ in fact has two components; see §3.1), we treat them as single lines here.

To obtain a more accurate estimate of the absorption line EWs, we used the SPECFIT (Kriss 1994) task under STSDAS to simultaneously fit the underlying continuum and the emission and absorption line profiles. The continuum was characterized by a simple power law, the emission lines were fit with multiple Gaussians, and each absorption line was fit with a single Gaussian. First, the power-law continuum was fit to featureless parts of the spectrum on either side of the emission lines and the absorption to be measured. The parameters of the power-law continuum – the slope and the normalization – were then fixed in subsequent fits. The parameters of the Gaussians used to fit the emission lines (flux, centroid, FWHM and skew) and the absorption lines (flux, centroid and FWHM) were allowed to vary freely. The fits to the  Ly$`\alpha `$, N V and C IV emission/absorption profiles are shown in Figure 2, and the corresponding EW and FWHM of the absorption fits are given in Table 1. The results of the SPLOT and SPECFIT methods are qualitatively similar, although the SPECFIT values are systematically larger due to the higher continuum provided by fitting the emission lines. These differences are unimportant to the discussion.

The observed FWHM of the absorption lines is 1.3 - 3.0 Å ($`>`$300 km s-1) with SPLOT and 1.4 - 3.3 Å ($`>`$320 km s-1) with SPECFIT. For each ion the total absorption is likely resolved given the $``$230  km s-1 resolution of FOS, so the absorber is dispersed in velocity space. In a higher resolution spectrum, however, the absorption lines may split into multiple components. The average absorption redshift for the five lines is $`<`$z$`>`$=0.063, blueshifted by 300  km s-1 from the QSO emission redshift of $`z_{em}=0.0640`$ (Bergeron et al. 1983). We expect that O VI absorption is also present, but it lies below the blue cutoff of the G130H grating at the redshift of MR2251$``$178.

MR2251$``$178 was also observed in 1998 Dec by J. Stocke with HST-STIS over the wavelength range 1250–1300Å. The  Ly$`\alpha `$ absorption line breaks into a broad component and a narrow component at the $``$12  km s-1 resolution of the STIS G140M grating. Figure 3 shows the  Ly$`\alpha `$ region and a fit to the absorption profile produced with SPECFIT as described previously. The resulting line centers, EWs and FWHMs of the two components are listed in Table 1.

## 3 The X-Ray/UV Absorber

High-ionization UV absorption lines due to  Ly$`\alpha `$, N V, and C IV are seen in the HST spectrum of MR2251$``$178, as predicted by UV/X-ray models. Mathur et al. (1998) estimate the chance probability that a radio-quiet QSO will have both associated UV and X-ray ionized absorption to be $`1.7\times 10^3`$. This strongly suggests the two absorption systems are physically related.

### 3.1 Physical Properties of the Ionized Gas

To explore the possibility that the UV and X-ray absorption lines arise in the same component of the nuclear material of the AGN, we need to compare the properties of the UV and X-ray absorbers.

We took the measurements of the X-ray absorber in MR2251$``$178 from the analysis of ASCA data (obtained 6 Nov 1993) by Reynolds (1997; Komossa 2001 obtains a similar result using ROSAT data from the same epoch). The total equivalent hydrogen column density of the X-ray absorber is $`N_\mathrm{H}=5\times 10^{21}`$ atoms cm-2, determined by fitting the warm absorber with a one-zone model using the CLOUDY photoionization code (Ferland 1996). Reynolds constrained the optical depths of the O VII/O VIII edges in a simple two-edge model with a power-law continuum ($`\alpha =1.73`$). We used these values as an input to CLOUDY to derive the column densities of the UV ions seen in absorption in the HST data. The standard “Table AGN” (Mathews & Ferland 1987) continuum (with a resulting ionization parameter of $`U=1.0.)`$444U is defined as the dimensionless ratio of ionizing photon to hydrogen number density. was used with the assumption of solar abundances. The shape of the observed UV continuum of MR2251$``$178 (Figure 1) is consistent with that in ”Table AGN.” Table 1 lists the CLOUDY predictions for the ionic column densities of H I, N V, and C IV, as derived from the X-ray data.

To compare these predictions to what is observed in the UV, it is necessary to convert the equivalent widths to column densities. As discussed in $`\mathrm{\S }`$2, the lines may be somewhat saturated, thus the column densities can be calculated only if the velocity dispersion parameter ($`b`$ parameter) of the lines is known. If the lines are resolved, then $`b`$ 450  km s-1 \[$`b=`$FWHM/(4ln2)1/2; the FWHM is given in Table 1\] for  Ly$`\alpha `$ and $``$ 200 - 270  km s-1 for C IV and N V. The X-ray prediction for the column density of hydrogen, $`N_{\mathrm{HI}}=8\times 10^{14}`$ cm-2, is therefore about a factor of 2 larger than the minimum value measured in the FOS data ($`N_{\mathrm{HI}}4\times 10^{14}`$ cm-2). Agreement between the UV and X-ray values is achieved for $`b200`$  km s-1, implying the line breaks into at least two components at higher resolution, as is shown in the STIS data (§2).555A weak feature at $``$ 1295.5 Å may also be  Ly$`\alpha `$ redshifted relative to the quasar, as has been observed in C IV lines of NGC 5548 (Mathur, Elvis, & Wilkes 1999); this feature would not contribute significantly to $`N_\text{}\text{I}`$. A curve-of-growth analysis using the new $`b`$-values ($``$65 and $``$280  km s-1) results in a combined total  Ly$`\alpha `$ column density of $`7\times 10^{14}`$, in good agreement with the X-ray prediction for H I.

The X-ray predicted values for the N V and C IV are smaller than those calculated from the UV equivalent width measurements. For N V, the X-ray prediction is $`N_{\mathrm{NV}}=1.6\times 10^{14}`$ cm-2, while the UV equivalent width measurement gives $`N_{\mathrm{HI}}=8\times 10^{14}`$ cm-2, assuming the lines are resolved. Similarly for C IV, the X-ray prediction of $`N_{\mathrm{CIV}}=1.6\times 10^{13}`$ cm-2 is more than an order of magnitude smaller than the UV measurement of $`N_{\mathrm{CIV}}7\times 10^{14}`$ cm-2. The X-ray predictions for $`N_{\mathrm{NV}}`$ and especially $`N_{\mathrm{CIV}}`$ lie on the linear part of the curve of growth. If the UV and X-ray absorbers are the same, we predict these absorbers should break into multiple components – each with lower $`b`$ – in UV data of higher resolution, leading to values in closer agreement with the X-ray predictions. Kinematically complex UV absorption lines have already been seen in high-resolution data of Mrk 509 (Crenshaw, Boggess & Wu 1995), NGC 4151 (Weymann et al. 1997), NGC 3516 (Kriss et al. 1996, Crenshaw et al. 1999), and NGC 5548 (Mathur et al. 1999; Crenshaw & Kraemer 1999).

Also, note the column densities derived here from the X-ray data are based on the Table AGN continuum. The shape of the actual MR2251$``$178 continuum in the unobserved EUV region may greatly affect the predicted column densities (Mathur et al. 1995). A better match between the observed & predicted values may be obtained if the spectral energy distribution of MR2251$``$178 has a different shape. In any case, the X-ray absorber is a large contributor to the absorption measured for C IV and N V in the UV, providing support for the idea that the UV and X-ray absorption is occurring in the same material.

### 3.2 Variability

Halpern (1984) found that the warm absorber in MR2251$``$178 was highly variable. ASCA data of MR2251$``$178 obtained in 1996 – near the epoch of the HST-FOS data – show a decrease in X-ray intensity from log $`\xi `$ = 1.35 in 1993 to log $`\xi `$ = 0.96 in 1996 (Otani, Kii, & Miya 1998), where $`\xi `$ is an ionization parameter defined as $`\xi L/nR^2`$. If the ionization parameter $`U`$ varied similarly, then in 1996 $`U=0.61`$ and the X-ray-predicted column densities would be $`N_{\mathrm{CIV}}=3.9\times 10^{14}`$ cm-2 and $`N_{\mathrm{NV}}=2.1\times 10^{15}`$ cm-2, closer to the values measured in the UV data. In this case, $`N_{\mathrm{HI}}`$ grows to $`3.4\times 10^{15}`$ cm-2.

### 3.3 Physical Implications

As noted, the UV absorption indicates the material is flowing outward from the UV/X-ray absorber at $``$300  km s-1. With the assumption that the UV and X-ray absorbers are the same we can determine the physical conditions and mass outflow rate of the absorbing material. We use the total hydrogen column of $`N_\mathrm{H}`$ = 5$`\times 10^{21}`$ cm-2 and the ionization parameter $`U=1.0`$ from the CLOUDY modeling of the X-ray data. The distance of the absorber from the nucleus is constrained by $`U=(Q/4\pi r^2n_Hc)^{1/2}`$, where $`Q`$ is the rate of ionizing photons. We used the HST data at 1339 Å rest wavelength to scale the standard Table AGN continuum to the luminosity of MR2251$``$178 ($`L_{bol}=5\times 10^{45}`$ ergs s-1). Integrating $`L_\nu /(h\nu )`$ over $`\nu 13.6`$eV gives $`Q=6h^2\times 10^{54}`$ s-1, where $`h`$ is the Hubble constant in units of 100  km s-1 Mpc-1. This puts the distance of the absorber from the nucleus at $`r=3.0\times 10^{18}n_5^{1/2}`$ cm (where $`H_\mathrm{o}=75`$  km s-1 Mpc-1 and $`n_5`$ is the density in units of $`10^5`$ cm-3).

The absorption extends below the continuum level (Figure 1), and so must cover a substantial fraction of the BELR as well as the continuum source. The absorber may lie outside the BELR or it could also be cospatial with it if most of the emission is beamed from the far side of the BELR. The size of the BELR in MR2251$``$178 can be estimated by scaling the BELR of NGC 5548 ($`L_{bol}=5\times 10^{44}`$ ergs s-1) by $`L^{1/2}`$ (Davidson & Netzer 1979; but see Kaspi et al. 2000). The distance – determined from reverberation mapping – of the BELR from the central continuum in NGC 5548 is $`r10`$ light-days (Clavel et al. 1991), so the absorber in MR2251$``$178 must be at least $``$32 light-days, or $`r8.2\times 10^{16}`$ cm from the central source. The corresponding upper limit on the density is then $`n<1.34\times 10^8`$ cm-3. To check the radius estimate, we specified as an input to CLOUDY the luminosity of MR2251$``$178 at a rest wavelength of 1339 Å, log($`\nu L_\nu `$) = 43.78, and varied the input radius to obtain the ionization parameter output previously. The radius at which $`U=1.0`$ was $`r=8.76\times 10^{16}`$ cm. For a covering factor of $`f=0.1`$, the column density and particle density of the aborber imply a mass of $`M=47f_{0.1}n_5^1M_{}`$. The mass outflow rate (Mathur et al. 1995) would then be $`\dot{M}_{out}=0.9f_{0.1}M_{}`$ yr-1, the same rate needed to power MR2251$``$178 at 10% efficiency. The rate of kinetic energy carried away in the flow is $`\dot{M}v_{out}^2/2=8\times 10^{40}`$ ergs cm-2 s-1.

## 4 Conclusions

The HST FOS UV spectrum of MR2251$``$178 exhibits associated high-ionization, UV absorption lines, as predicted from models of the X-ray ionized absorber. The X-ray/UV absorber is situated outside the BELR or cospatial with it and outflowing with a line-of-sight velocity of $``$300  km s-1. The mass outflow rate of 0.9 M yr-1 for a 10% covering factor is equivalent to the accretion rate onto the nuclear black hole.

We expect future higher resolution observations will reveal each of the C IV and N V absorption lines breaking into at least two components.

The rarity of both UV and X-ray absorbers individually in radio-quiet QSOs virtually requires that the X-ray and UV absorbers are closely physically related. The consistency of the column densities obtained from both UV and X-ray data suggests the absorbers are perhaps identical. At a minimum, the X-ray absorber makes a substantial contribution to the absorption seen in the UV. Thus, the absorber in MR2251$``$178 satisfies both statistical as well as physical tests of our X-ray/UV absorber model.


text:
# Effective pseudo-potentials of hydrodynamic origin

## 1 Introduction

It is well-known that a particle which is moving under the influence of an external force such as gravity in a viscous fluid sets up a disturbance flow in the fluid which, in the low Reynolds number limit, decays with distance like $`r^1`$. The long-range character of these force-driven flows manifests itself in many situations. One example involves collective diffusive behavior. A pair of Brownian spheres has been predicted Batchelor (1976) and measured Crocker (1997) to diffuse in a correlated manner. On the basis of these long-range correlations, Crocker et al. (2000) have developed a new technique for the microrheology of complex materials. Recently, Dufresne et al. (2000) experimentally and theoretically showed the diffusive behavior of a pair of Brownian spheres to be strongly influenced even by distant solid boundaries. Long-range flows also have a significant influence on the properties of sedimenting systems, giving rise to numerous divergent integrals (see e.g. Hinch 1988). For example, Caflisch & Luke (1985) have predicted velocity fluctuations in sedimenting particulate suspensions to diverge with system size, and Brenner (1999) has drawn attention to the fact that sedimenting particles’ long-range interaction with cell walls can screen the flows and cut off the divergent fluctuations. In addition, long-range hydrodynamic coupling has provided a plausible interpretation Squires & Brenner (2000) for the experiment of Larsen & Grier (1997), which measured an apparent attraction between like-charged colloidal spheres in the proximity of a similarly-charged wall.

It is also well-known that there are other ways to move particles which do not give rise to such long-range disturbance velocity fields. One example is electrophoresis (e.g. Anderson 1989), wherein charged particles move under the influence of an applied electric field. A charged particle in solution attracts oppositely charged counter-ions from the solution, which form a screening ‘double-layer’ (e.g. Russel et al. 1989, chap. 4). The particle/double layer system is electrically neutral, so an applied electric field exerts no net force on the ensemble. However, the charged particle and the counter-ions are driven in opposite directions, giving an apparent ‘slip velocity’ at the edge of the double layer, and a net motion to the particle. Since velocity fields with $`r^1`$ decay arise only from a net force on the fluid, electrophoretic (and all force-free) flow fields must decay at least as fast as $`r^2`$.

In this paper we will demonstrate that this difference between the long-range disturbance flows due to forced and force-free motions can be exploited to cause particles to behave as though they were subject to equilibrium forces derived from an effective potential. As an example, we will discuss the electrophoretic ‘levitation’ of a heavy charged sphere off a wall, for which an effective pseudo-potential $`\mathrm{\Phi }_{\text{ps}}`$ can be determined exactly. We will then present a method for making like-charged colloidal spheres near a wall behave as though there was an apparent attraction between them, so that layered like-charged colloidal crystals can be grown. Throughout this work, we use the term ‘pseudo-potential’ to emphasize that the hydrodynamic component of $`\mathrm{\Phi }_{\text{ps}}`$ arises not from a force, but from persistent low-Reynolds number flows which entrain each particle.

We shall first briefly review the hydrodynamics of forced- and force-free motion. Colloidal particles ($`1\mu m`$) and their typical velocities ($`1\mu m/s`$) are small enough that inertial effects are entirely negligible. In this limit, a rigid sphere of radius $`a`$ moves due to an external force $`𝐅`$ at velocity $`𝐔_\mathrm{𝟎}=b_0𝐅`$, where $`b_0=(6\pi \eta a)^1`$ is the Stokes mobility. This motion sets up a disturbance flow in the surrounding fluid

$$𝐮(𝐑)=\frac{1}{8\pi \eta }\left(\frac{𝐈}{R}+\frac{\mathrm{𝐑𝐑}}{R^3}\right)𝐅\frac{a^2}{24\pi \eta }\left(\frac{𝐈}{R^3}+\frac{3\mathrm{𝐑𝐑}}{R^5}\right)𝐅,$$
(1.1)
where $`\eta `$ is the fluid viscosity and $`𝐑=𝐫𝐫_0`$ is the vector connecting the observation point $`𝐫`$ and the center of the sphere $`𝐫_0`$. This can be re-expressed using fundamental singularities of the Stokes equation as

$$𝐮(𝐫)=\frac{1}{8\pi \eta }\left\{𝐒(𝐑)\frac{a^2}{3}\left(\frac{1}{R}\right)\right\}𝐅,$$
(1.2)
The first term represents the flow due to a point force, known as a Stokeslet, which decays like $`R^1`$. The second term is the Green’s function for a point source dipole, also called a potential dipole, which decays like $`R^3`$. The flow far from a forced sphere is dominated by the Stokeslet, which depends on neither the size nor the velocity of the sphere.

By contrast, a charged insulating sphere with a thin double-layer moving due to a uniform electric field $`𝐄_{\mathrm{}}`$ sets up a disturbance flow outside the double layer (e.g. Russel et al. 1989, p. 256),

$$𝐮_E(𝐑)=\frac{ϵ\zeta }{4\pi \eta }\frac{a^3}{2}\left(\frac{𝐈}{R^3}+\frac{3\mathrm{𝐑𝐑}}{R^5}\right)𝐄_{\mathrm{}},$$
(1.3)
where $`ϵ`$ is the dielectric constant of the fluid and $`\zeta `$ is the potential difference across the double-layer. Here the sphere moves at velocity $`𝐕_\mathrm{𝟎}=M_0𝐄_{\mathrm{}}`$, where $`M_0=ϵ\zeta /4\pi \eta `$ is the electrophoretic mobility. This flow is exclusively potential dipole flow and decays like $`R^3`$.

Walls affect these flows significantly, since the fluid velocity must vanish identically on solid boundaries. Image singularities, analogous to image charges in electrostatics, can often be found which exactly cancel a flow set up on the wall. In this paper, we shall make extensive use of the flow due to a Stokeslet (point force) $`F\widehat{𝐳}`$ oriented perpendicular to a wall, which Blake (1971) found to be

$$𝐮(𝐑)=\frac{F}{8\pi \eta }\left(𝐒(𝐑)𝐒(𝐑^i)+2h^2\left\{_0_0\left(\frac{1}{r}\right)\right\}|_{𝐑^i}2h\left\{\frac{𝐒(𝐫)}{z_0}\right\}|_{𝐑^i}\right)\widehat{𝐳},$$
(1.4)
where $`𝐑^i=𝐑+2h\widehat{𝐳}`$ is the vector between the images and the observation point, derivatives with respect to the source point $`𝐫_0`$ (denoted by $`_0`$) should be taken first, and then the position $`𝐑^i`$ inserted in place of $`𝐫`$. The flow due to the images decays like $`R^1`$, whereas the image flow for a source dipole Blake & Chwang (1974), which will not be required in this paper, decays like $`R^3`$.

The velocity of a sphere forced toward a wall has two contributions: it moves at $`𝐔_\mathrm{𝟎}`$ due to the applied force, and it is advected with the flow set up by the image singularities. Evaluating the image flow from (1.4) at $`r_0`$ results in an $`O(a/h)`$ wall correction to the (scalar) mobility for motion perpendicular to the wall (e.g. Happel & Brenner 1983):

$$b_{}(h)=b_0\left(1\frac{9a}{8h}+O\left[\frac{a^3}{h^3}\right]\right).$$
(1.5)
The correction to the electrophoretic mobility can be derived in similar fashion, but is slightly more complicated because the wall gives both hydrodynamic and electrostatic contributions. Since the image flow (and electrostatic image potential) for electrophoretic motion decays like $`R^3`$, the wall correction to the electrophoretic mobility is $`O(a^3/h^3)`$, and has been calculated using the method of reflections by Keh & Anderson (1985) to give

$$M_{}(h)=M_0\left(1\frac{5a^3}{8h^3}+O\left[\frac{a^5}{h^5}\right]\right).$$
(1.6)
Throughout this paper, we will treat $`a/h`$ and $`a/r`$ as small, and so neglect this $`O(a^3/h^3)`$ variation in $`M_{}`$.

## 2 Electrophoretic ‘levitation’

These two motions and their respective flows can be superposed, since Stokes’ flow is linear. A charged sphere which sediments due to a force $`F_\mathrm{g}`$ towards a planar electrode and which is electrophoretically driven upwards due to a uniform electric field $`𝐄_{\mathrm{}}`$ will have a velocity $`v`$ given by

$$v=b_{}(h)F_\mathrm{g}+M_{}(h)E_{\mathrm{}},$$
(2.7)
with $`b_{}(h)`$ and $`M_{}(h)`$ given by (1.5) and (1.6) respectively. If the bulk electrophoretic velocity is less than the bulk sedimentation velocity, so that $`\psi =M_0E_{\mathrm{}}/b_0F_\mathrm{g}<1`$, there will be a unique height

$$\frac{h_0}{a}=\frac{9}{8(1\psi )}+O(a^2)$$
(2.8)
where the two velocities exactly balance and a non-Brownian sphere will come to rest. A sphere started above $`h_0`$ falls faster than electrophoresis drives it up, and it moves down towards the plane. Similarly, a sphere below $`h_0`$ falls too slowly, and electrophoresis drives it up. Thus $`h_0`$ is a stable steady location. On the other hand, $`h_0`$ would be an unstable steady point for a sphere falling away from a wall.

A sphere undergoing Brownian motion will have a probability distribution $`P(h)`$ of being located at $`h`$ which is given by the steady Fokker-Planck equation (see e.g. Batchelor 1977)

$$\frac{P}{t}=0=𝐉\left[𝐯(h)Pk_BT𝐛(h)P\right],$$
(2.9)
where $`k_\mathrm{B}T𝐛`$ is a tensor diffusivity. This equation has solution $`P(h)=P_0\mathrm{exp}(\mathrm{\Phi }_{\text{ps}}/k_BT)`$, where $`\mathrm{\Phi }_{\text{ps}}`$ is a non-equilibrium ‘pseudo-potential’

$$\mathrm{\Phi }_{\text{ps}}(h)=F_\mathrm{g}h^h\frac{M_{}(h^{})E_{\mathrm{}}}{b_{}(h^{})}𝑑h^{}.$$
(2.10)
Inserting the values of $`b_{}`$ and $`M_{}`$ from (1.5) and (1.6) and keeping terms to $`O(a/h)`$, we integrate (2.10) to obtain

$$\mathrm{\Phi }_{\text{ps}}(h)F_\mathrm{g}h\frac{M_0E_{\mathrm{}}}{b_0}\left[h+\frac{9a}{8}\mathrm{ln}\left(\frac{h}{a}\frac{9}{8}\right)\right],$$
(2.11)
which can be expanded about its minimum at $`h_0`$ to give an approximately harmonic well

$$\frac{\mathrm{\Phi }_{\text{ps}}}{k_BT}\frac{8}{9}\frac{F_\mathrm{g}a}{k_BT}\left[\frac{(1\psi )^2}{\psi }\right]\frac{(hh_0)^2}{2a^2}+\frac{\mathrm{\Phi }_{\text{ps}}(h_0)}{k_BT}.$$
(2.12)
If one viewed only the motion of a single sphere in this configuration, one would not be able to distinguish between this non-equilibrium pseudo-potential and a true thermodynamic potential. However, the physical distinction is crucial: the only force on the sphere/double layer system is $`F_\mathrm{g}`$, directed toward the wall.

## 3 Multi-particle pseudo-potential interactions

Even though the electrophoretically ‘levitated’ particle is stationary, it drives a long-range flow. Far from the sphere, the flow is always dominated by the force-driven motion, since it decays the most slowly. Streamlines for the flow around a hovering sphere, described in section 2, are shown in figure 1.

A second identical sphere, placed at the same height and at some distance $`r`$ away from the original sphere, will both set up a long-range flow as well as be entrained by the flow set up by the first sphere. Forcing two spheres perpendicular to the wall induces a relative velocity between them Squires & Brenner (2000), in the plane of the wall, as is evident from the streamlines in figure 1. This relative velocity of sphere 1 arises from its entrainment in the flow set up by the images of sphere 2, and is found to $`O(a/h)`$ and $`O(a/r)`$ from (1.4) to be

$$\dot{x}_1=\dot{x}_2=\frac{3}{2\pi \eta }\frac{rh^3}{(r^2+4h^2)^{5/2}}F_g,$$
(3.13)
where $`x`$ is the coordinate parallel to the wall, along the line joining the spheres, as in figure 2. Two spheres forced away from a wall move together as they leave the wall, whereas two spheres falling towards a wall move apart. In this case, we observe that the relative motion between two non-Brownian hovering spheres resembles the motion due to an effective repulsive force, even though it does not arise from a force. Example trajectories for two such spheres are shown by the solid curves in figure 2, with arrows showing the collapse onto these trajectories from various initial configurations.

## 4 Like-charge colloidal crystal formation

Finally, we explore the possibility of setting up an attractive interaction between the spheres, which can lead to crystal formation. Since forcing two spheres toward a wall led to an effective repulsion, forcing them off of the wall will give an effective attraction. One way to do this would be to electrophoretically drive neutrally buoyant charged spheres into a similarly-charged wall. This would require the wall to possess a static surface charge density and to simultaneously passes a current.

As we have seen, the far-field hydrodynamic flows are dominated by the net force on the body and its charge cloud. In this case, the net force $`F_\mathrm{w}`$ on each is given by its electrostatic repulsion from the static charge on the wall, found by integrating an electrostatic stress tensor over the surface of the sphere (see, e.g. Russel et al. 1989). Under the linear superposition approximation, the repulsive force the wall exerts on the sphere is found to be

$$\frac{F_\mathrm{w}}{k_\mathrm{B}T}=4\pi Z\sigma _\mathrm{g}\lambda _\mathrm{B}\frac{e^{\kappa a}}{1+\kappa a}e^{\kappa h},$$
(4.14)
where $`Z`$ is the effective charge on the sphere, $`\sigma _\mathrm{g}`$ is the charge density on the wall, $`\kappa ^1`$ is the Debye screening length and $`\lambda _\mathrm{B}`$ is the Bjerrum length($`.7`$ nm in water at room temperature). This force sets up a flow around each sphere like in figure 1, with flow arrows reversed. The lateral component of the flow now draws the spheres together.

Two non-Brownian spheres separated by distance $`r`$ are immobilized at the height $`h_0`$ where $`𝐌𝐄_{\mathrm{}}=𝐛(h_0,r)𝐅_\mathrm{w}(h_0)`$. The equivalent force on each sphere which would be necessary to drive this motion in a quiescent fluid is

$$F_{x_1}\frac{\dot{x_1}}{b_{x_1x_1}b_{x_1x_2}},$$
(4.15)
where $`b_{x_1x_2}`$ is the coefficient of $`𝐛`$ which gives the mobility sphere 1 in the $`\widehat{𝐱}`$ direction due to a force on sphere 1 in the same direction, and so on. Using (3.13), and neglecting the weak dependence of $`h_0`$ upon $`r`$, this can be integrated to yield a pseudo-potential

$$\mathrm{\Phi }_{\text{ps}}(r,h_0)U_\mathrm{p}(r)\frac{3h_0^3F_\mathrm{w}(h_0)}{2\pi \eta }^r\frac{r(4h_0^2+r^2)^{5/2}}{b_{x_1x_1}(h_0)b_{x_1x_2}(r,h_0)}𝑑r,$$
(4.16)
where $`U_\mathrm{p}`$ is the true pair potential between the spheres. Although $`b_{x_2x_1}`$ is $`O(a)`$, in practice it is small compared to $`b_{x_1x_1},`$ and its neglect allows the direct integration of (4.16) to give

$$\mathrm{\Phi }_{\text{ps}}(r,h_0)U_\mathrm{p}(r)\frac{F_\mathrm{w}(h_0)}{1\frac{9a}{16h_0}}\frac{3h_0^3a}{(4h_0^2+r^2)^{3/2}}.$$
(4.17)
The true pair potential between charged spheres, $`U_\mathrm{p}`$, is given in linear superposition approximation by (e.g. Larsen & Grier 1997),

$$\frac{U_\mathrm{p}}{k_BT}=Z^2\lambda _B\left(\frac{e^{\kappa a}}{1+\kappa a}\right)^2\frac{e^{\kappa r}}{r}.$$
(4.18)
Equation (4.17) is identical to that derived by Squires & Brenner (2000) in their analysis of the experiment of Larsen & Grier (1997) which measured the effective interaction between like-charged colloidal spheres near a single charged wall. Although the two formulae were derived in the same fashion, they have very different physical consequences. In that experiment, a pair of spheres was repeatedly released from the same height $`h_0`$ and then re-trapped; therefore, a net force systematically drove the spheres away from the wall throughout the experiment. Consequently, there was a systematic relative motion of the spheres towards each other which had been interpreted to arise from an attractive force. In an equilbrium system, where the spheres fluctuate into the wall as often as away, one would expect no systematic relative motion, and this hydrodynamic effect would be of no physical consequence.

Similarly, the pseudo-potential of equation (4.17) does not describe an attractive force between two like-charged colloids. However, in the present situation, similarly-charged spheres actually do respond as though there was an attraction. The effect of electrophoresis is to ‘pin’ the spheres at some height without applying a force, so that the long-range flow is dominated by the forced motion and entrains neighboring spheres accordingly. A collection of spheres can thus aggregate to form clusters–a behavior which might otherwise seem to arise from an attractive force.

Spheres which are not neutrally buoyant have a similar pseudo-potential, with $`F_\mathrm{w}F_\mathrm{g}`$ in place of $`F_\mathrm{w}`$ in (4.17). Note that both the depth and the range of this potential can be tuned independently–the range by adjusting the electric field $`E_{\mathrm{}}`$ to give different heights $`h_0`$ and the overall magnitude of the attraction by adjusting the relative density of the particle to affect $`F_\mathrm{g}`$. Furthermore, one could study the freezing and melting of the crystals we’ll describe next by simply adjusting $`E_{\mathrm{}}`$ during an experiment.

Brownian motion considerably complicates the above picture. Again, the probability distribution for the spheres’ positions obey the steady Fokker-Planck equation (2.9). An interesting fact is that there is a persistent non-zero probability current $`𝐉`$ in the steady state. The probability current can only be zero when

$$\mathrm{\Phi }_{\text{ps}}=𝐛^1𝐮$$
(4.19)
has a solution. In equilibrium systems, $`𝐮=𝐛𝐅`$ so that $`𝐅=\mathrm{\Phi }_{\text{ps}}`$ as expected. Here $`𝐮=𝐛𝐅+𝐮_E`$, and (4.19) will not in general have a solution. Physically, this is because the equivalent force required to give velocity $`𝐮_E`$ would be non-conservative. Vertical fluctuations take the pair into regions of stronger or weaker attraction, leading to persistent closed orbits of $`𝐉`$. When these vertical fluctuations are relatively small, $`𝐉`$ is small and the effective pseudo-potential is well approximated by (4.17). A comparison betweeen (4.17) and simulated results is shown in figure 3. The lower two pseudo-potential wells (a) and (b) are deep enough that bound states form. The simulated pseudo-potentials $`\mathrm{\Phi }_{\mathrm{ps}}/k_BT`$ are thus simply $`\mathrm{log}g(r)`$, where $`g(r)`$ is the the pair correlation function obtained from simulations of a pair of spheres. We used the method described by Crocker & Grier (1996) to simulate the shallowest potential well (c), since it is not deep enough for bound states.

We have run simulations which account for Brownian motion to demonstrate that spheres can indeed self-assemble into a quasi-2D crystal. We use the dynamical equations

$$𝐯=𝐛𝐅+𝐌𝐄$$
(4.20)
where $`𝐯,𝐛`$ and so on are multiparticle quantities. We retain terms up to $`O(a)`$ in $`𝐛`$ and $`𝐌`$ and use a box of side $`100a`$ with periodic boundaries. Brownian motion is accounted for in standard fashion Ermak & McCammon (1978); Grassia et al. (1995), wherein $`𝐃=k_BT𝐛`$ is a position-dependent tensor diffusivity. We use as input parameters the values $`Z=7300`$, $`\kappa ^1=.275\mu m`$ and $`2a=.652\mu m`$ as in the experiments of Larsen & Grier (1997) and the value $`\sigma _\mathrm{g}=.4\sigma _s`$ for the (unmeasured) charge density on the wall which Squires & Brenner (2000) found as the best fit to the experimental data. We choose these values because 1) the effects we are discussing are most pronounced with long screening lengths and high surface charge densities, so that the spheres tend to ‘hover’ at an appreciable distance from the wall, and 2) these effects may bear some relation to these particular experiments. We started nineteen spheres in a hexagonal crystal, then simulated their dynamics until it was clear that the qualitative features would not change. This was typically approximately a minute or less of real time. Figure 3 shows the resulting suspensions at the end of each run for three different field strengths. The strongest field, for which $`h_0=2\mu m`$, yields a hexagonal crystal, whereas a weaker field, for which $`h_0=2.2\mu m`$, is strong enough to yield a dense phase, but not strong enough to retain orientational order. We loosely term this an istropic ‘liquid’ phase. Finally, for an even weaker field, for which $`h_0=2.5\mu m`$, the attraction is sufficiently weak that the spheres spread out to fill the box as an isotropic ‘gas’.

## 5 Discussion and conclusions

While we have specifically investigated the combination of electrophoretically-driven motion and body-force motion, the present results have a wider validity. Our results will hold whenever motion using body forces such as gravity, electrostatic repulsion or attraction, magnetic forces, etc. are combined with force-free motion. There are many ways to achieve the latter. Since any self-propelled motion can not result in a net force or torque on the system, all swimmers generate flows decaying faster than $`r^1`$ Lighthill (1976). There are also other types of “phoretic” motion, which involve particle motion due to fields which interact with the particle’s surface (e.g. Anderson 1989), such as thermophoresis (motion due to thermal gradients) and diffusophoresis (motion due to solute concentration gradients). Similarly, the thermocapillary motion of bubbles Young et al. (1959), driven by thermal surface tension gradients, is force-free.

Having shown that like-charged colloidal crystals can self-assemble into ordered crystals due to long-range persistent non-equilibrium hydrodynamic flows, it is natural to ask whether there could be any connection between these crystals and those observed by Larsen & Grier (1997). These metastable crystallites formed near the charged glass walls of the experimental cells, and persisted for times orders of magnitude longer than purely repulsive Brownian spheres should. This response can certainly be understood within the present picture, and would require a force-free motion to drive the spheres into the charge cloud of the walls. A spurious current in the cell could do this; however, it is unlikely that this explains Larsen and Grier’s crystals, for two reasons: 1) there are no electrodes on the top and bottom walls of their cells, and 2) the crystals were observed to form on both the top and bottom walls, whereas a net current in the cell would likely drive the spheres to one wall or the other. Another possible current source, suggested by D. S. Fisher, is the dissociation of ionic groups on the glass surface. Other possible mechanisms for force-free motion include thermal or electrolyte concentration gradients; however, it is not clear which if any of these mechanisms are present or responsible for the crystals. It is generally believed that a novel long-ranged attraction between confined like-charged colloids, whose origin remains controversial, gives rise to this behavior (e.g. Hansen & Lowen 2000). The present work provides a non-equilibrium mechanism whose origins are well-known and understood which would mimic an attractive interaction and could drive like-charge colloidal crystallization, so its potential role should be investigated further.

Two-dimensional colloidal crystals have been formed on electrodes via electrophoretic deposition Bohmer (1996); Trau et al. (1997), and Solomentsev et al. (1997) has proposed a electrohydrodynamic model, which bears some similarity to the present work, for its explanation. The crucial difference between the our work and that of Solomentsev et al. (1997) and is that in the latter, the particles are first deposited on the electrode, and then electro-osmotic flows drive adjacent particles towards one another. These electro-osmotic flows are much shorter-ranged than the body-force driven flows described here, and are highly screened by the close proximity of the wall.

In conclusion, we have used the difference in flow fields set up by force-driven motion and force-free motion to show that persistent long-range viscous flowfields can be set up, resulting in particle motion which mimics an effective potential. This appears surprising at first, since the system is out of equilibrium, and yet behaves as though it is an equilibrium system with an effective potential which is hydrodynamically driven. Given the general nature of this effect, these persistent flowfields are likely to find various applications in self-assembly and microfluidic contexts.

###### Acknowledgements.

This work was supported under the NSF Division of Mathematical Sciences grant DMS-9733030.