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# Electron Magnetic Resonance: The Modified Bloch Equation

## I Introduction

The importance of magnetic resonance methods to chemical analysis, solid-state physics, biological structure determination and medicine is well recognized. In magnetic resonance experiments, a material is placed in dc and oscillating magnetic fields and the power absorption is measured. The power absorption exhibits spectra containing resonances, from which valuable information about the system is obtained.

The Bloch equation describing the dynamics of the magnetic moment operator $`\stackrel{}{\mu }`$ is:

$$\frac{d\stackrel{}{\mu }}{dt}=\frac{\mu _0\gamma }{\mathrm{}}\stackrel{}{B}\times \stackrel{}{\mu }.$$
(1)
Its solution is discussed in textbook theoretical treatments of magnetic resonance . Here, $`\mu _0=\frac{e\mathrm{}}{2m}`$ is the Bohr magneton, and $`\gamma `$ is a dimensionless constant. SI units are employed throughout. This equation has played a major role in understanding magnetic resonance experiments ever since it was first derived by Bloch in 1946 . In the usual treatment, coupling to the surrounding, i.e., to additional degrees of freedom of the system (often described as a thermodynamic bath), is incorporated into the description by adding phenomenological relaxation (decay) terms to the Bloch equation . The additional phenomenological decay terms arise when the bath degrees of freedom of the system are adiabatically eliminated from the description. The external magnetic field in magnetic resonance experiments has a temporally-constant strong component, and a weaker oscillating component of radio-frequency or microwave radiation, which in one common configuration is linearly polarized and perpendicular to the dc component:

$`\stackrel{}{B}=B_0\widehat{z}+B_1\left(e^{i\omega t}+e^{i\omega t}\right)\widehat{x};B_1B_0.`$ (2)
It is a straightforward generalization to treat the case when the magnetic field contains a rotating oscillating field: $`\stackrel{}{B}_\mathrm{c}=B_0\widehat{z}+\sqrt{2}B_1[\widehat{x}\mathrm{cos}(\omega t)\widehat{y}\mathrm{sin}(\omega t)]`$. Here we consider linear polarization. For atomic and molecular systems it is an excellent approximation to neglect the spatial dependence of the oscillating field because the wavelength is so much larger than the size of the atom or molecule.

The power absorption $`P`$ of a magnetic moment $`\stackrel{}{\mu }`$ in the external field $`\stackrel{}{B}`$ is given by:

$$P=\left[\stackrel{}{\mu }\frac{d\stackrel{}{B}}{dt}\right]_t=\left[\stackrel{}{B}\frac{d\stackrel{}{\mu }}{dt}\right]_t,$$
(3)
where $`\mathrm{}`$ stands for quantum expectation value and $`\left[\mathrm{}\right]_t`$ for time averaging. Power can only be absorbed if $`\stackrel{}{B}`$ and $`\stackrel{}{\mu }`$ oscillate out of phase, and $`\stackrel{}{\mu }`$ has a component along $`\frac{d\stackrel{}{B}}{dt}`$. The Bloch equation without relaxation terms, Eq. (1), results in no power absorption, since clearly, $`\stackrel{}{B}\left(\stackrel{}{B}\times \stackrel{}{\mu }\right)=0`$. In this treatment, the phase shift between the oscillations of $`\stackrel{}{B}`$ and $`\stackrel{}{\mu }`$, necessary for power absorption, exists only because of the relaxation terms. Without those, Eq. (1), implies that power absorption is impossible.

This theoretical framework is adequate for the description of both NMR (Nuclear Magnetic Resonance) and ESR (Electron Spin resonance). It is generally not correct for EMR (Electron Magnetic Resonance). The Bloch equation is not the correct equation of motion for the magnetic moment operator of an electron with non-vanishing orbital angular momentum. Orbital angular momentum effects in magnetic resonance phenomena can be important, not just in gases, but even in solids, e.g., the transition and lanthanide ions doped in crystals where quenching (the modification of the magnetic susceptibility to values close to those produced by electron spin alone due to large crystal field splittings) does not occur . Here we show that, due to diamagnetic effects arising from the electronic orbital angular momentum, the Bloch equations are replaced by a set of coupled operator equations for the magnetic moment $`\stackrel{}{\mu }`$ (which incorporates a magnetic field induced magnetic moment contribution), the coordinate $`\stackrel{}{r}`$ and the velocity operator $`\stackrel{}{\mathrm{\Pi }}/m`$, defined below. The interaction Hamiltonian has non-linear terms arising from a magnetic field induced magnetic moment. As a result, the magnetic moment has an oscillatory component along $`\frac{d\stackrel{}{B}}{dt}`$ and oscillates out of phase with the external field. Hence, power absorption does not vanish, even when coupling to the environment is not included.

In Sec. II we define the magnetic moment operator, including the magnetic field induced magnetic moment contribution, and in Sec. III we derive the Heisenberg equations of motion for a magnetic moment $`\stackrel{}{\mu }`$ in the magnetic field $`\stackrel{}{B}`$. Three coupled equations are obtained in this way, Eqs. (12), (13), and (14) below. Based on these equations, Sec. IV develops general considerations of power absorption in EMR experiments. Since, unlike the Bloch equation, these coupled equations can not be solved in closed form, we solve them in time-dependent perturbation theory, and calculate the power absorption using this analysis. In Sec. V we focus on the example of an electron bound in a $`p`$-atomic-orbital, and derive Eq. (46) for the power absorption to leading order in the fields for this case. Section VI presents a summary and conclusion.

## II The Hamiltonian and the Magnetic Moment Operator

The Hamiltonian for an electron, with charge $`q=e`$ and mass $`m`$ in a spherically symmetric potential $`\widehat{V}(r)`$ and an external magnetic field $`\stackrel{}{B}(t)`$, can be written in terms of the kinetic velocity operator $`\widehat{\stackrel{}{\mathrm{\Pi }}}/m`$ :

$`\widehat{H}=\widehat{V}(r)+{\displaystyle \frac{\widehat{\mathrm{\Pi }}^2}{2m}},`$ (4)
$`\widehat{\stackrel{}{\mathrm{\Pi }}}\widehat{\stackrel{}{p}}q\widehat{\stackrel{}{A}},`$ (5)
$`\widehat{\stackrel{}{A}}{\displaystyle \frac{1}{2}}\stackrel{}{B}\times \widehat{\stackrel{}{r}}.`$ (6)
For simplicity, we have neglected the electron spin (which can be re-introduced rather easily as shown in Sec. VI) and chosen a symmetric gauge. The coordinate operator $`\widehat{\stackrel{}{r}}`$, the conjugate momentum operator $`\widehat{\stackrel{}{p}}`$, and the velocity operator $`\widehat{\stackrel{}{\mathrm{\Pi }}}/m`$, satisfy the commutation relations: $`[r_i,p_j]=[r_i,\mathrm{\Pi }_j]=i\mathrm{}\delta _{ij}`$, and $`[\mathrm{\Pi }_i,\mathrm{\Pi }_j]=i\mathrm{}qϵ_{ijk}B_k`$, where $`ϵ_{ijk}`$ is the anti-symmetric Levi-Chivita tensor.

The gauge-invariant operator for the orbital magnetic dipole moment of the electron is given by

$`\widehat{\stackrel{}{\mu }}={\displaystyle \frac{q}{2m}}\widehat{\stackrel{}{r}}\times \widehat{\stackrel{}{\mathrm{\Pi }}}.`$ (7)
The magnetic moment operator defined in Eq. (7) is gauge invariant. This can be seen by considering the gauge transformation matrix $`U=\mathrm{exp}[i\frac{q}{\mathrm{}}\chi ]`$ in terms of the gauge function $`\chi (\stackrel{}{r},t)`$. Under the gauge transformation, the vector potential and the magnetic moment are transformed as follows: $`\stackrel{}{A}\stackrel{}{A}^{}=\stackrel{}{A}+\chi `$, and $`\widehat{\stackrel{}{\mu }}\widehat{\stackrel{}{\mu }}^{}=U[\frac{q}{2m}\widehat{\stackrel{}{r}}\times (\widehat{\stackrel{}{p}}q\widehat{\stackrel{}{A}^{}})]U^{}=\widehat{\stackrel{}{\mu }}`$.

The Hamiltonian of Eq. (4) can be written in terms of the magnetic moment in the following form:

$`\widehat{H}=\widehat{V}(r)+{\displaystyle \frac{\widehat{p}^2}{2m}}\widehat{\stackrel{}{\mu }}\stackrel{}{B}+{\displaystyle \frac{q^2}{8m}}\left[(\stackrel{}{B}\widehat{\stackrel{}{r}})^2B^2\widehat{r^2}\right].`$ (8)
Neglecting all terms of order $`B^2`$ gives: $`\widehat{H}^{}=\widehat{V}(r)+\frac{\widehat{p}^2}{2m}\widehat{\stackrel{}{\mu ^{}}}\stackrel{}{B}`$ and $`\widehat{\stackrel{}{\mu ^{}}}\frac{q}{2m}\widehat{\stackrel{}{r}}\times \widehat{\stackrel{}{p}}`$, as used in standard textbook treatments of magnetic resonance. Here, we consider the effect of not neglecting these second order terms, i.e., using $`\widehat{H}`$ (not $`\widehat{H}^{}`$) with the full $`\widehat{\stackrel{}{\mu }}`$ (not $`\widehat{\stackrel{}{\mu ^{}}}`$).

## III Heisenberg equations

The magnetic moment $`\widehat{\stackrel{}{\mu }}`$ satisfies the Heisenberg equation of motion: $`\frac{d\widehat{\stackrel{}{\mu }}}{dt}=\frac{\widehat{\stackrel{}{\mu }}}{t}+\frac{i}{\mathrm{}}[\widehat{H},\widehat{\stackrel{}{\mu }}]`$. Straight-forward algebra gives,

$$\frac{\widehat{\stackrel{}{\mu }}}{t}=\frac{q}{2m}\widehat{\stackrel{}{r}}\times \frac{}{t}\widehat{\stackrel{}{\mathrm{\Pi }}}=\frac{q^2}{4m}\widehat{\stackrel{}{r}}\times \left(\frac{}{t}\stackrel{}{B}\times \widehat{\stackrel{}{r}}\right)=\frac{q^2}{4m}\left[\left(\widehat{\stackrel{}{r}}\frac{\stackrel{}{B}}{t}\right)\widehat{\stackrel{}{r}}\widehat{r^2}\frac{\stackrel{}{B}}{t}\right],$$
(9)
$`{\displaystyle \frac{i}{\mathrm{}}}[\widehat{H},\widehat{\stackrel{}{\mu }}]`$ $`=`$ $`{\displaystyle \frac{q^2}{2m^2c^2}}\left\{(\widehat{\stackrel{}{r}}\widehat{\stackrel{}{p}})\stackrel{}{B}(\widehat{\stackrel{}{r}}\stackrel{}{B})\widehat{\stackrel{}{p}}+{\displaystyle \frac{q}{2c}}\left(\widehat{\stackrel{}{r}}\stackrel{}{B}\right)\left(\stackrel{}{B}\times \widehat{\stackrel{}{r}}\right)i\mathrm{}\stackrel{}{B}\right\}`$ (10)
$`=`$ $`{\displaystyle \frac{q^2}{2m^2c^2}}\left\{\widehat{\stackrel{}{r}}\times (\stackrel{}{B}\times \widehat{\stackrel{}{\mathrm{\Pi }}})i\mathrm{}\stackrel{}{B}\right\},`$ (11)
and, collecting terms, we get:

$$\frac{d\widehat{\stackrel{}{\mu }}}{dt}=\frac{q^2}{4m}\left[\left(\widehat{\stackrel{}{r}}\frac{\stackrel{}{B}}{t}\right)\widehat{\stackrel{}{r}}\widehat{r^2}\frac{\stackrel{}{B}}{t}\right]+\frac{q^2}{2m^2}\left[\widehat{\stackrel{}{r}}\times (\stackrel{}{B}\times \widehat{\stackrel{}{\mathrm{\Pi }}})i\mathrm{}\stackrel{}{B}\right].$$
(12)
The right hand side of Eq. (12) is not equal to $`\frac{\mu _0}{\mathrm{}}\stackrel{}{B}\times \stackrel{}{\mu }\frac{q^2}{2m^2}\left[\stackrel{}{B}\times (\stackrel{}{r}\times \widehat{\stackrel{}{\mathrm{\Pi }}})\right]`$. The Bloch equations are replaced by operator equations whose consistent solution must treat the Heisenberg equation of motions for $`\widehat{\stackrel{}{\mu }}(t)`$ as well as $`\widehat{\stackrel{}{r}}(t)`$ and $`\widehat{\stackrel{}{\mathrm{\Pi }}}(t)`$:

$`{\displaystyle \frac{d\widehat{\stackrel{}{r}}}{dt}}=\widehat{\stackrel{}{\mathrm{\Pi }}}/m,`$ (13)
$`{\displaystyle \frac{d\widehat{\stackrel{}{\mathrm{\Pi }}}}{dt}}={\displaystyle \frac{\widehat{\stackrel{}{\mathrm{\Pi }}}}{t}}{\displaystyle \frac{i}{\mathrm{}}}[\widehat{\stackrel{}{\mathrm{\Pi }}},V(\widehat{r})]{\displaystyle \frac{i}{\mathrm{}}}[\widehat{\stackrel{}{\mathrm{\Pi }}},\widehat{\stackrel{}{\mathrm{\Pi }}}^2/2m].`$ (14)
From these equations we see that energy can be absorbed by the system even under conditions of negligible or no coupling to the environment since $`d\stackrel{}{\mu }/dt`$ is no longer perpendicular to $`\stackrel{}{B}`$. This power absorption in magnetic resonance systems containing electronic orbital angular momentum can also be interpreted as being due to the rate of change of the electric dipole moment in the presence of an electric field. This is evident from the relation:

$$\frac{\widehat{H}}{t}=\frac{e}{2m}\left(\frac{d\stackrel{}{B}}{dt}\times \stackrel{}{r}\right)\stackrel{}{\mathrm{\Pi }}=\stackrel{}{\mu }\frac{d\stackrel{}{B}}{dt}=\stackrel{}{E}\frac{d\stackrel{}{\mu _E}}{dt}.$$
(15)
Here the electron electric dipole moment is $`\stackrel{}{\mu }_E=q\stackrel{}{r}=e\stackrel{}{r}`$, its time derivative is $`d\stackrel{}{\mu }_E/dt=e\stackrel{}{\mathrm{\Pi }}/m`$, and the electric field is given by $`\stackrel{}{E}=\stackrel{}{A}/t`$. Clearly, additional power aborption may result due to coupling to a bath.

The time derivative of the magnetic dipole moment in Eq. (12) can not be written simply in terms of the cross product of the external field and the dipole moment, hence a closed-form analytic solution of the operator equations in the Heisenberg representation is not available. Instead a perturbative solution can be used, as described below.

## IV Power absorption

Substituting the magnetic field of Eq. (2) into the Hamiltonian in Eq. (8), we find that the Hamiltonian can be separated into a sum of time-independent and time-dependent parts:

$`\widehat{H}=\widehat{H}_0+\widehat{H}_1(t),`$ (16)
$`\widehat{H}_0=\widehat{V}(r)+{\displaystyle \frac{\widehat{p}^2}{2m}}B_0{\displaystyle \frac{q}{2m}}(\widehat{x}\widehat{p}_y\widehat{y}\widehat{p}_x)+B_0^2{\displaystyle \frac{q^2}{8m}}(x^2+y^2),`$ (17)
$`\widehat{H}_1(t)=B_1\left(e^{i\omega t}+e^{i\omega t}\right)\widehat{h}_1;\widehat{h}_1{\displaystyle \frac{q}{2m}}(\widehat{y}\widehat{p}_z\widehat{z}\widehat{p}_y)+{\displaystyle \frac{q^2}{4m}}B_0xz,`$ (18)
where a term $`\widehat{H}_2(t)`$ of order $`B_1^2`$ has been neglected. Realistic magnetic fields strengths impose a hierarchy between these terms because usually $`|B_0||B_1|`$.

For comparison, two frequently used Hamiltonians which give the regular Bloch equation, Eq. (1), are: $`\widehat{H}^\mathrm{B}=\widehat{H}_0^\mathrm{B}+\widehat{H}_1^\mathrm{B}(t)`$, with:

$`\widehat{H}_0^\mathrm{B}=\widehat{H}_0^{}=\widehat{V}(r)+{\displaystyle \frac{\widehat{p}^2}{2m}}B_0\widehat{\mu }_z^{},`$ (19)
$`\widehat{H}_1^\mathrm{B}(t)=\widehat{H}_1^{}=B_1\left(e^{i\omega t}+e^{i\omega t}\right)\widehat{h}_1^{};\widehat{h}_1^{}=\widehat{\mu }_x^{},`$ (20)
obtained when all second order terms in the fields are neglected, as usual; and the Hamiltonian for a pure spin system:

$`\widehat{H}_0^\mathrm{B}=g_s\mu _0\widehat{\stackrel{}{s}}\stackrel{}{B}_0,`$ (21)
$`\widehat{H}_1^\mathrm{B}=g_s\mu _0\widehat{\stackrel{}{s}}\stackrel{}{B}_1\left(e^{i\omega t}+e^{i\omega t}\right).`$ (22)
In both these cases for which the Bloch equation applies, the time-independent and time-dependent parts of the Hamiltonian commute: $`[\widehat{H}_0^\mathrm{B},\widehat{H}_1^\mathrm{B}]=0`$, while $`[\widehat{H}_0,\widehat{H}_1]0`$. Either way, the time-independent Hamiltonian can be diagonalized in terms of a complete basis-set $`\{|m\}`$:

$`\widehat{H}_0|m=E_m|m,`$ (23)
and the time-dependent electron wave function can be written (in the Schrödinger representation) as a linear combination of these basis-set states:

$`|\mathrm{\Psi }(t)={\displaystyle \underset{m}{}}c_m(t)e^{iE_mt/\mathrm{}}|m,`$ (24)
with time-dependent coefficients, $`c_m(t)`$, that satisfy a set of coupled equations,

$$\frac{dc_m}{dt}=\frac{i}{\mathrm{}}\underset{l}{}e^{i\omega _{lm}t}m|\widehat{H}_1|lc_l,$$
(25)
where $`\omega _{lm}(E_lE_m)/\mathrm{}`$. Power is absorbed by the system at the following rate:

$`𝒫(\omega )=\left[{\displaystyle \frac{dE}{dt}}\right]_t`$ $`=`$ $`\left[{\displaystyle \frac{d}{dt}}{\displaystyle \underset{m}{}}E_m|c_m|^2\right]_t`$ (26)
$`=`$ $`{\displaystyle \underset{m}{}}{\displaystyle \underset{l}{}}i\omega _{lm}c_m^{}c_le^{i\omega _{lm}t}m|\widehat{H}_1|l`$ (27)
$`=`$ $`{\displaystyle \underset{m}{}}{\displaystyle \underset{l}{}}c_m^{}c_le^{i\omega _{lm}t}m\left|{\displaystyle \frac{i}{\mathrm{}}}[\widehat{H}_0,\widehat{H}_1]\right|l.`$ (28)
Three different cases can be considered:

* Pure spin system with no coupling to the environment.
* Pure spin system with coupling to the environment.
* Diamagnetic system (magnetic field induced magnetic moment due to orbital angular momentum) with no coupling to the environment.

In the first case of a pure spin system with no coupling to the environment, as well as in the case of the approximate Hamiltonian leading to the regular Bloch equation; $`[\widehat{H}_0^\mathrm{B},\widehat{H}_1^\mathrm{B}]=0`$. As a result, the power absorption is identically zero. In this case it would be wrong to apply perturbation theory to the expansion of Eq. (27). This can be understood on very general terms: a time-dependent perturbation which commutes with the time-independent Hamiltonian can not induce transitions.

Different magnetic systems (including in particular pure spin systems) with coupling to the environment were considered in the literature within two basically different approaches. In the first approach, $`T_1`$ and $`T_2`$ processes are included when considering the dynamics, and power absorption can thereby occur . The $`T_1`$ and $`T_2`$ processes can be described by relaxation terms added to the Bloch equation; the resulting dynamics can no longer be described by a Hamiltonian.

In another approach introduced by Kubo and coworkers , which we would like to compare to, it is assumed that a Hamiltonian completely defines the dynamics:

$`\widehat{H}^{\prime \prime }=\widehat{H}_0^{\prime \prime }+\widehat{H}_1^{}(t),`$ (29)
$`\widehat{H}_1^{}(t)=B_1\left(e^{i\omega t}+e^{i\omega t}\right)\widehat{h}_1^{};\widehat{h}_1^{}\mu _x^{}={\displaystyle \frac{q}{2m}}(\widehat{y}\widehat{p}_z\widehat{z}\widehat{p}_y).`$ (30)
$`H_0^{\prime \prime }`$ effectively incorporates the coupling to the environment; although the coupling is not explicitly specified, it is assumed that $`[\widehat{H}_0^{\prime \prime },\widehat{H}_1^{}]0`$. The power absorption therefore does not vanish, and can be calculated using, for example, a linear-response theory .

We now show that the power absorption of a diamagnetic system with no coupling to the environment is very similar to power absorption of a pure spin system with coupling to the environment when the coupling to the environment is considered within linear-response theory as in Ref. . We show that in both cases the power absorption does not vanish and is given by a similar (though not identical) expression. The similarities and differences are derived and discussed below. The essential point is that as soon as $`[\widehat{H}_0,\widehat{H}_1]0`$, power absorption does not vanish, and, using the fact that for realistic magnetic fields $`B_1B_0`$, time-dependent perturbation theory can be applied.

The first-order solution of Eq. (25) with initial condition at $`t=0`$, $`c_m(0)=b_m`$ is:

$$c_m=b_m+\frac{1}{\mathrm{}}B_1\underset{l}{}m|\widehat{h}_1|l\left[\frac{e^{i(\omega \omega _{lm})t}1}{\omega \omega _{lm}}\frac{e^{i(\omega \omega _{ml})t}1}{\omega \omega _{ml}}\right]b_l.$$
(31)
Substituting this result into Eq. (27), and applying the rotating wave approximation in the usual way, the power absorption is obtained:

$$𝒫(\omega )=2B_1^2\underset{E_n>E_m}{}\frac{\omega _{nm}}{\mathrm{}}|n|\widehat{h}_1|m|^2\left(|b_m|^2|b_n|^2\right)\left[\frac{\mathrm{sin}(\omega \omega _{nm})t}{\omega \omega _{nm}}\right]_t.$$
(32)
In the limit $`t\mathrm{}`$, we find:

$`𝒫(\omega )=2B_1^2\omega \chi _x^{\prime \prime },`$ (33)
$`\chi _x^{\prime \prime }=\pi {\displaystyle \underset{m,n}{}}|n|\widehat{h}_1|m|^2\left(|b_m|^2|b_n|^2\right)\delta (E_nE_m\mathrm{}\omega ).`$ (34)
In the case of a pure spin system with coupling to the environment $`\widehat{h}_1=\widehat{\mu }_x`$. Eq. (34) gives the static magnetic susceptibility and with Eq. (33) is identical to the results obtained by Kubo and Nagamiya  in their Eqs. (18.4) and (19.17). We note that they have obtained this result within a different treatment, using a density matrix formalism, but under the same assumptions as those supporting the perturbative treatment we have used, namely, that the system is linear and in a steady-state. In the density matrix treatment, $`|b_m|^2`$ and $`|b_n|^2`$ in Eq. (34) are replaced by the densities $`\rho (E_m)`$ and $`\rho (E_n)`$, respectively.

We note here that this expression for the power absorption is correct only as long as a perturbative treatment is appropriate. As soon as a significant part of the population occupies the excited states a nonperturbative treatment would be necessary. The power absorption would necessarily cease as the system continues to absorb energy from the field and evolves to higher energy states if no coupling to the environment were present, but this is not contained in a perturbation theory or linear response approach. Here we study the power absorption only within the perturbative regime. We note that the time scale from turning on the fields till a significant change in the population could be noticed can in principle be quite large.

In the case considered here, of no coupling to the environment but inclusion of orbital effects, $`\widehat{h}_1=\frac{q}{2m}(\widehat{y}\widehat{p}_z\widehat{z}\widehat{p}_y)+\frac{q^2}{4m}B_0\widehat{x}\widehat{z}`$, while in the case of coupling to the environment but no orbital effects, $`\widehat{h}_1=\widehat{\mu }_x^{}=\frac{q}{2m}(\widehat{y}\widehat{p}_z\widehat{z}\widehat{p}_y)`$. Moreover, the spectrum and hence the resonance frequencies are different in these two cases. In either case, once the Bloch equation is modified, whether by relaxation terms or by terms of second order in the external fields, power absorption can ensue. Furthermore, while the numerical details of this power absorption may differ, the general behavior is the same in these two cases. The power absorption is given by Eq. (33) with a somewhat different quantum susceptibility in the two cases. In both cases, the quantum susceptibility is obtained by substituting the appropriate energy eigenvalues and coupling Hamiltonians into Eq. (34).

To summarize this section: focusing on the regime where a linear response theory applies, we have solved for the power absorption using time-dependent perturbation theory. We have derived Eqs. (33, 34) for the power absorption and for the susceptibility. This result is similar to that obtained by Kubo and coworkers in Ref.  but there are several differences: the coupling Hamiltonian $`\widehat{h}_1`$ is different, the quantum susceptibilities of the two systems are slightly different, and the spectral position is shifted. These are small corrections. Their order of magnitude is determined by the ratio between the magnetic energy and the total energy of the system. Hence, it seems that it would be difficult to experimentally observe a difference between the result for the susceptibility obtained using our approach and the standard result for cw applications where a linear response theory applies. The major difference is in justifying the linear response treatment. We have shown that it applies only if $`[\widehat{H}_0,\widehat{H}_1]0`$. This condition for a consistent application of perturbation theory holds in Kubo’s derivation only if coupling to the environment is included, while for our case here no such coupling is required.

## V Power absorption of an electron bound in a $`p`$-atomic-orbital

As an example, we study power absorption of an electron bound by the Coulomb potential, $`V(r)=Ze^2/(4\pi ϵ_0r)`$, in a $`p`$-orbital ($`l=1`$), and placed in the external time-dependent magnetic field of Eq. (2). Neglecting spin effects, the complete Hamiltonian can be written as above. As a basis set we choose the three wave functions:

$$\stackrel{}{r}|\psi _\pm =\frac{\pm 1}{\sqrt{2}}(x\pm iy)f(r),\stackrel{}{r}|\psi _0=zf(r),$$
(35)
where for principal quantum number $`n=2`$,

$$f(r)\frac{1}{4}\frac{1}{\sqrt{2\pi }}\left(\frac{Z}{a_0}\right)^{5/2}\mathrm{exp}\left[\frac{Z}{2a_0}r\right],$$
(36)
and the Bohr radius is defined as $`a_04\pi ϵ_0\mathrm{}^2/(me^2)`$. These basis functions are eigenfunctions of the free Hamiltonian when no magnetic fields are present, as well as of $`\widehat{H}_0^{}`$, (but not of $`\widehat{H}`$ or even $`\widehat{H}_0`$). The $`l=1`$ manifold spanned by this basis set is not closed under the complete Hamiltonian. The orbital angular momentum $`l`$ is not a good quantum number due to the terms in the Hamiltonian of second order in the external magnetic field, which do not commute with the angular momentum operator. The coupling to other manifolds is small, however, and the energy difference between the different manifolds is large. We therefore neglect the coupling to other manifolds, and consider the action of $`\widehat{H}`$ only within the $`l=1`$ subspace. A general solution of the time-dependent problem is then given by

$`|\mathrm{\Psi }(t)=c_0(t)e^{iE_0t/\mathrm{}}|\psi _0+c_+(t)e^{iE_+t/\mathrm{}}|\psi _++c_{}(t)e^{iE_{}t/\mathrm{}}|\psi _{},`$

and the time-dependent perturbative analysis of the coefficients of the previous section applies with $`m=0,+,`$.

The diagonal matrix elements of $`\widehat{H}`$ in this basis set are:

$`E_0\psi _0|\widehat{H}_0|\psi _0={\displaystyle \frac{}{8}}+{\displaystyle \frac{12}{}}(\mu _0B_0)^2,`$ (37)
$`E_\pm \psi _\pm |\widehat{H}_0|\psi _\pm ={\displaystyle \frac{}{8}}\pm \mu _0B_0+{\displaystyle \frac{15}{}}(\mu _0B_0)^2,`$ (38)
where $`\frac{Z^2e^2}{4\pi ϵ_0a_0}`$. The level spacings are given by,

$`\mathrm{}\omega _+E_+E_0=\mu _0B_0\left(1+3{\displaystyle \frac{\mu _0B_0}{}}\right)>0,`$ (39)
$`\mathrm{}\omega _{}E_0E_{}=\mu _0B_0\left(13{\displaystyle \frac{\mu _0B_0}{}}\right)>0,`$ (40)
where $`\mathrm{}\omega _{}>0`$ assuming $`3\mu _0B_0<`$. The oscillating field couples $`|\psi _0`$ and $`|\psi _\pm `$:

$`\psi _0|\widehat{h}_1|\psi _\pm =\psi _\pm |\widehat{h}_1|\psi _0={\displaystyle \frac{\mu _0}{\sqrt{2}}}\left[112{\displaystyle \frac{\mu _0B_0}{}}\right].`$ (41)
The leading order contribution to the power absorption is:

$`𝒫_0(\omega )`$ $`=`$ $`{\displaystyle \frac{\pi }{\mathrm{}^2}}\left(\mu _0B_0\right)\left(\mu _0B_1\right)^2`$ (43)
$`\times \left\{\left(|b_{}|^2|b_0|^2\right)\delta (\omega \omega _{})+\left(|b_0|^2|b_+|^2\right)\delta (\omega \omega _+)\right\}.`$
The next order correction to this power absorption is:

$`𝒫_1(\omega )`$ $`=`$ $`{\displaystyle \frac{24\pi }{\mathrm{}^2}}{\displaystyle \frac{(\mu _0B_0)}{}}\left(\mu _0B_0\right)\left(\mu _0B_1\right)^2`$ (45)
$`\times \left\{\left(|b_{}|^2|b_0|^2\right)\delta (\omega \omega _{})+\left(|b_+|^2|b_0|^2\right)\delta (\omega \omega _+)\right\}.`$
Higher order terms are of third order in $`B_1`$. At temperature $`T=0`$, $`b_0=b_+=0`$ and $`b_{}=1`$, and we obtain:

$`𝒫(\omega )`$ $`=`$ $`{\displaystyle \frac{\pi }{\mathrm{}^2}}\left(\mu _0B_0\right)\left(\mu _0B_1\right)^2\left(1+24{\displaystyle \frac{\mu _0B_0}{}}\right)\delta \left[\omega {\displaystyle \frac{\mu _0B_0}{\mathrm{}}}\left(13{\displaystyle \frac{\mu _0B_0}{}}\right)\right].`$ (46)
Note that for realistic experimental conditions, $`\left(\mu _0B_1\right)^2`$ is small enough to justify the perturbative treatment and as a result $`𝒫(\omega )`$ is very small.

Realizable magnetic fields are, for example, $`B_0=5`$ T and $`B_1=5\times 10^4`$ T. The relative strength of the correction term $`𝒫_1`$ as compared to the leading order term $`𝒫_0`$, is determined by the dimensionless parameter $`24\mu _0B_0/`$, which for $`B_0=5`$ T and $`Z=6`$ (carbon) is equal to $`1\times 10^5`$. $`𝒫_1`$ as well as the higher order terms are thus but small corrections to $`𝒫_0(\omega )`$.

## VI Conclusions and Summary

In this paper we have studied the dynamics of the gauge-invariant operator for the magnetic dipole moment $`\stackrel{}{\mu }`$ of an electronic system in an external magnetic field $`\stackrel{}{B}`$. In addition to the intrinsic magnetic moment of the electron it includes a field induced magnetic moment arising from the electronic orbital angular momentum, i.e., a diamagnetic contribution. We have derived the Heisenberg equation of motion for this magnetic moment in a general magnetic field and shown that this modified Bloch equation is coupled to two other Heisenberg equations for the position and velocity operators. While we could not solve this set of equations exactly and in closed form, we have solved it perturbatively using time-dependent perturbation theory and calculated the power absorption of the magnetic moment in a time-dependent magnetic field under magnetic-resonance conditions. Under the assumption of a steady-state, we have found an expression for the quantum susceptibility in terms of matrix elements of a coupling Hamiltonian $`\widehat{h}_1`$. Finally, we have explicitly calculated the integrated power absorption for the example of a $`p`$-orbital electron and found that it is given by Eq. (46).

Several generalizations can be easily considered. Upon generalizing to include electron spin, the Hamiltonian and the magnetic moment operator become,

$$\widehat{H}=\widehat{V}(r)+\frac{\widehat{\mathrm{\Pi }}^2}{2m}\widehat{\stackrel{}{\mu }}_s\stackrel{}{B},$$
(47)
$$\widehat{\stackrel{}{\mu }}=\frac{q}{2m}(\widehat{\stackrel{}{r}}\times \widehat{\stackrel{}{\mathrm{\Pi }}}+g_s\mathrm{}\widehat{\stackrel{}{s}})=\frac{e}{2m}\widehat{\stackrel{}{r}}\times \widehat{\stackrel{}{\mathrm{\Pi }}}g_s\mu _0\widehat{\stackrel{}{s}},$$
(48)
respectively, where $`\widehat{\stackrel{}{\mu }}_s=g_s\mu _0\widehat{\stackrel{}{s}}`$, and $`g_s`$ is the electron spin gyromagnetic ratio ($`g_s2.002`$). The last term on the right hand side of Eq. (48) is the intrinsic spin magnetic moment operator of the electron, $`\widehat{\stackrel{}{\mu }}_s`$. Incorporation of this term into the modified Bloch equation yields the following term on the right hand side of Eq. (12 ): $`\frac{\mu _0g_s}{\mathrm{}}\stackrel{}{B}\times \widehat{\stackrel{}{\mu }}_s`$, i.e., the generalized Bloch equation becomes,

$$\frac{d\widehat{\stackrel{}{\mu }}}{dt}=\frac{e^2}{4m}\left[\left(\widehat{\stackrel{}{r}}\frac{\stackrel{}{B}}{t}\right)\widehat{\stackrel{}{r}}\widehat{r^2}\frac{\stackrel{}{B}}{t}\right]+\frac{e^2}{2m^2}\left[\widehat{\stackrel{}{r}}\times (\stackrel{}{B}\times \widehat{\stackrel{}{\mathrm{\Pi }}})i\mathrm{}\stackrel{}{B}\right]+\frac{(\mu _0g_s)^2}{\mathrm{}}\stackrel{}{B}\times \widehat{\stackrel{}{s}}.$$
(49)
Inclusion of spin-orbit coupling of the form $`\alpha (r)\stackrel{}{s}\stackrel{}{l}`$ into the Hamiltonian is also straightforward. The modified Bloch equation then has additional terms on the right hand side proportional to $`\alpha (r)\stackrel{}{s}\times \stackrel{}{l}`$ and $`\alpha (r)(\stackrel{}{s}\stackrel{}{r})(\stackrel{}{B}\stackrel{}{r})`$. The latter term is due to the magnetically induced magnetic moment. Furthermore, one can also readily include ligand field effects, exchange coupling effects, etc., within the formulation considered here. Ligand field terms in the Hamiltonian commute with the magnetically induced magnetic moment, as do spin exchange terms, but orbital angular momentum exchange coupling terms do not, and therefore contribute additional terms to the extended Bloch equation due of the magnetically induced magnetic moment.

How do our results differ from previous treatments of magnetic resonance phenomena? It is useful to divide such a comparison into two subjects: the equations of motion and the mechanism of power absorption.

We have shown that the Bloch equation, Eq. (1), is not the correct Heisenberg equation for a magnetic moment $`\stackrel{}{\mu }`$ in the magnetic field $`\stackrel{}{B}`$ when orbital angular momentum is present. A modified Bloch equation, Eq. (12), is obtained. Upon inclusion of spin, the factor of $`g_s`$ in the term $`\frac{\mu _0g_s}{\mathrm{}}\stackrel{}{B}\times \widehat{\stackrel{}{\mu }}_s`$, which is equivalent to the last term on the right hand side of Eq. (49), further precludes writing a Bloch equation of the form of Eq. (1) with $`\widehat{\stackrel{}{\mu }}`$ replaced with $`\widehat{\stackrel{}{\mu }}_l+\widehat{\stackrel{}{\mu }}_s`$. The modified equation can not be written in terms of $`\stackrel{}{\mu }`$ and $`\stackrel{}{B}`$ alone. It contains the position and kinetic velocity operators and therefore must be solved together with dynamical equations for these operators. In general, $`d\stackrel{}{\mu }/dt`$ is not perpendicular to $`\stackrel{}{B}`$, and $`\stackrel{}{\mu }`$ oscillates out of phase with $`\stackrel{}{B}`$. This results in a non-vanishing power absorption.

In the usual picture, correct for pure spin systems, power is absorbed only because of the coupling of the spin system to the environment. Without this coupling the magnetic moment $`\stackrel{}{\mu }`$ would oscillate in phase with $`\stackrel{}{B}`$, $`d\stackrel{}{\mu }/dt`$ would be perpendicular to $`\stackrel{}{B}`$ at all times, and no power would be absorbed. Coupling to the environment dephases the oscillations of $`\stackrel{}{\mu }`$ and $`\stackrel{}{B}`$ and induces a nonvanishing component of $`d\stackrel{}{\mu }/dt`$ along $`\stackrel{}{B}`$. In the case considered here, of a magnetic moment that explicitly contains a diamagnetic contribution, the power absorption does not vanish even when coupling to the environment is not included because the magnetic moment has a component which oscillates out of phase with the external field as a result of non-linear terms in the interaction Hamiltonian arising from a magnetic field induced magnetic moment. The phase difference between oscillations of the magnetic field and oscillations of the magnetic dipole moment of a bound electron in this field, is an intrinsic feature of the system and need not be induced by additional couplings to a bath that gives rise to dissipation. This power absorption can be interpreted, as evident from Eq. (15), as being due to the rate of change of the electric dipole moment in the presence of an electric field. Additional power aborption may result due to coupling to a bath.

For cw power absorption, dissipation of energy from the atomic system to the environment is required in order to ensure that the system stays in thermal equilibrium, so that power absorption can be maintained under steady-state conditions. Hence, for truly cw power absorption, as opposed to pulsed magnetic resonance experiments, the two systems depend on coupling to the environment to maintain a steady state and eventually will behave similarly. The results presented here indicate that diamagnetic systems would behave differently from pure-spin systems during the initial time when the turning on of the fields occur. For pure spin systems the time scale for initiation of power absorption would be set by the coupling to the environment while for diamagnetic systems it would be an intrinsic time scale indifferent to the environment. Without a relaxation mechanism, no power would be absorbed by a pure spin system, while the diamagnetic system will absorb power upon the turning on of the fields only until the population of levels reach a new equilibrium. We note that as soon as the population is changed significantly, second and higher order effects become important and a first-order time-dependent perturbation theory would not suffice.

###### Acknowledgements.

Useful discussions with Garnett Bryantt are gratefully acknowledged. This research was supported by The Israel Science Foundation (B. S. is supported by grant No. 181/00 and Y. B. B. by grant No. 212/01).


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# References

Kelvin force in a Layer of Magnetic Fluid
Adrian Lange

Institut für Theoretische Physik, Universität Magdeburg, Postfach 4120, D-39016 Magdeburg, Germany

## Abstract

The Kelvin force in a layer of magnetic fluid subjected to a homogeneous magnetic field and local heating is studied. The study is motivated by the question about the corresponding Kelvin force density \[M. Liu, Phys. Rev. Lett. 84, 2762 (2000)\]. It is shown that the usual and the newly proposed formulation of the Kelvin force are entirely equivalent. It is only when approximations are introduced that differences arise.

Keywords: Kelvin force; Magnetic fluids;

| Contact author: | Adrian Lange, Fax: +49-391-6711205 |
| --- | --- |
|  | email: adrian.lange@physik.uni-magdeburg.de |

Two prominent directions of interest can be identified among the present studies of phenomena occuring in magnetic fluids (MFs). These are the study of unconventional fluid dynamics phenomena such as the “negative viscosity” effect and the Weissenberg effect (for a review see ) and the proposal of new theoretical concepts . Both directions are interwoven in the observation of a novel convective instability in a horizontal MF layer  and in the subsequent discussion about the correct form of the magnetic (or Kelvin) force density .

This first discussion about the range of validity of the Kelvin force was followed by a second one  triggered by a paper announcing that a pendulum experiment had confirmed the invalidation of the Kelvin force in MFs . The claim was not accomplished according to  and the resulting need for a clarification entailed an extended paper . A clarification as in the pendulum experiment is lacking for the convection experiment. The aim of the present paper is to show that the usual and the proposed formulation of the Kelvin force are entirely equivalent. It is only when one introduces approximations that differences arise.

In  a horizontal layer of MF (stable colloidal suspension of magnetite nanoparticles dispersed in kerosene) between two glass plates is locally heated by a focused laser beam. It passes perpendicularly through the layer in the presence of a homogeneous vertical magnetic field. The absorption of the light by the fluid generates a temperature gradient and subsequently a refractive index gradient. This gradient is optically equivalent to a diverging lens, leading to an enhancement of the beam divergence. As result, depending on the strength of the magnetic field different diffraction patterns appear .

To explain the observed phenomena, the form of the magnetic force inside the fluid has to be known. Therefore a horizontal layer of MF is considered which is subjected to a homogeneous vertical magnetic induction. Since the temperature and the concentration of the fluid may vary, the magnetic field in the fluid is inhomogeneous and give rise to a finite Kelvin force density, $`𝐟_\mathrm{K}`$. It can be derived from the Helmholtz force

$$𝐟_\mathrm{K}=\mu _0\mathrm{grad}\left[\frac{H_{int}^2}{2}\rho \frac{\chi }{\rho }\right]\mu _0\frac{H_{int}^2}{2}\mathrm{grad}\chi ,$$
(1)
where $`\chi =\alpha \rho (1+\beta _1\alpha \rho )`$ is the susceptibility of the MF, $`\rho `$ its density, $`H_{int}`$ the absolute value of the magnetic field inside the fluid, and $`\mu _0=4\pi \times 10^7`$ H/m. Higher order terms in $`\rho `$ are included in $`\chi `$ in order to determine the Kelvin force beyond the dilute limit. This limit is given by $`\beta _10`$, i.e. $`\chi =\chi _L`$ which is the susceptibility according to Langevins theory which assumes non-interacting particles. In this approximation $`\chi _L`$ depends linearly on the density , $`\chi _L=\alpha \rho =\mu _0m^2\rho /(3kTm_{eff})`$, where $`m_{eff}`$ is the effective mass of a ferromagnetic particle with its ‘attached’ carrier liquid molecules , $`m`$ the magnitude of the magnetic moment of the particles, $`T`$ the temperature, and $`k`$ the Boltzmann constant. The coefficient $`\beta _1`$ of the quadratic term in $`\rho `$ was determined in different microscopic models  which all provide the same value $`\beta _1=1/3`$. In the presence of a uniform external magnetic induction $`𝐁_{ext}`$, the internal field is given by $`𝐇_{int}=𝐁_{ext}/(\mu _0(1+\chi ))`$. Inserting all expressions in Eq. (1), the Kelvin force follows as

$$𝐟_\mathrm{K}(\chi )=\frac{B_{ext}^2}{\mu _0}\frac{\chi _L^2\left\{1+\beta _1\left[3\chi _L\left(1+\beta _1\chi _L\right)1\right]\right\}}{(1+\chi )^3}\frac{\mathrm{grad}\chi _L}{\chi _L}.$$
(2)
In  a variant form for the Kelvin force is proposed. By defining a different susceptibility $`\overline{\chi }`$ via $`𝐌=(\overline{\chi }/\mu _0)𝐁_{int}`$ with $`\overline{\chi }=\chi /(1+\chi )`$ the Helmholtz force has now the variant form

$`𝐟_\mathrm{V}`$ $`=`$ $`\mathrm{grad}\left[{\displaystyle \frac{B_{int}^2}{2\mu _0}}\rho {\displaystyle \frac{\overline{\chi }}{\rho }}\right]{\displaystyle \frac{B_{int}^2}{2\mu _0}}\mathrm{grad}\overline{\chi }`$ (3)
$`=`$ $`{\displaystyle \frac{B_{int}^2}{2\mu _0}}\mathrm{grad}\left[\rho {\displaystyle \frac{\overline{\chi }}{\rho }}\overline{\chi }\right]+{\displaystyle \frac{\rho }{2\mu _0}}{\displaystyle \frac{\overline{\chi }}{\rho }}\mathrm{grad}B_{int}^2.`$
$`𝐁_{int}`$ ($`𝐌`$) is the magnetic induction (magnetization) in the fluid and $`B_{int}`$ its absolute value. Due to the uniform form of the external induction and the continuity of the magnetic induction across the interface, the last term is zero and the first term gives with the definition of $`\overline{\chi }`$

$$𝐟_\mathrm{V}(\chi )=\frac{B_{ext}^2}{2\mu _0}\mathrm{grad}\left[\frac{\beta _1\alpha ^2\rho ^2\chi ^2}{(1+\chi )^2}\right].$$
(4)
Executing the differentiation in Eq. (4) leads exactly to the same result as in Eq. (2). Therefore both formulations are indeed physically equivalent under the inclusion of a quadratic term in $`\rho `$. The equivalence is true also for higher terms in $`\rho `$ provided that the susceptibility can be written as $`\chi =\alpha \rho \left[1+_{i=1}^{\mathrm{}}\beta _i(\alpha \rho )^i\right]`$. Thus there is no a priori reason to prefer Eq. (3) over Eq. (1) because both formulations lead to the same result as long as the definition of $`\overline{\chi }`$ is used in Eq. (3). This very basic fact independent on the relation of $`\chi `$ on $`\rho `$ has to be emphasized since it recedes in the wake of the discussion .

The discussion about the range of validity of $`𝐟_\mathrm{K}`$ in  is based on the simultaneous approximation that $`\chi \rho `$ and $`\overline{\chi }\rho `$. The concurrent correctness of both relations has to be checked very cautiously. Since $`\rho =\chi _L/\alpha `$ with constant $`\alpha `$, the proportionality to the density $`\rho `$ is equivalent with the proportionality to the Langevin susceptibility $`\chi _L`$. Restricting the dependence of the susceptibilities on $`\chi _L`$ up to the third order, one has

$$\chi =\chi _L\left[1+\beta _1\chi _L+\beta _2\chi _L^2\right]+O(\chi _L^4)$$
(5)
and

$`\overline{\chi }`$ $``$ $`\chi (1\chi +\chi ^2\mathrm{})`$
$`=`$ $`\chi _L\left[1+(\beta _11)\chi _L+(\beta _2+12\beta _1)\chi _L^2\right]+O(\chi _L^4),`$ (6)
where the expansion (6) is valid for $`\chi 1`$ only. Assuming a linear dependence of $`\chi `$ on $`\chi _L`$, i.e. $`\beta _1=\beta _2=0`$, the expansion (6) implies necessarily that $`\overline{\chi }`$ depends on higher order terms of $`\chi _L`$. Figure 1 shows the linear behaviour of $`\chi =\chi _L`$ (dashed line) and the nonlinear behaviour of $`\overline{\chi }=\chi _L(1\chi _L+\chi _L^2)`$ (solid line) for $`0\chi _L0.5`$. A nonlinear dependence of $`\overline{\chi }`$ on $`\chi _L`$ in the region, where $`\chi \chi _L`$ holds, is confirmed also by measurements (see Fig. 1(b) in ).

From Fig. 1 it becomes evident that in the region $`\chi =\chi _L`$ a subregion $`\chi _L0.06`$ exists, where additionally $`\overline{\chi }=\chi _L`$ is fulfilled. Inserting $`\chi =\chi _L`$ in Eqs. (2,4), the resulting force density

$$𝐟_\mathrm{K}(\chi )=𝐟_\mathrm{V}(\chi )=\frac{B_{ext}^2}{\mu _0}\frac{\chi _L\mathrm{grad}\chi _L}{(1+\chi _L)^3}$$
(7)
is nonzero. This agreement confirms the above general statement that the usual and the variant form of the Kelvin force density are equivalent provided they are functions of $`\chi `$ $`(`$see Eqs. (2,4)$`)`$. But inserting $`\chi =\chi _L`$, $`𝐌=\chi 𝐇_{int}`$ in Eq. (1) and $`\overline{\chi }=\chi _L`$, $`𝐌=(\overline{\chi }/\mu _0)𝐁_{int}`$ in Eq. (3), respectively, one gets

$$𝐟_\mathrm{K}=\mu _0(𝐌\mathrm{grad})𝐇_{int}$$
(8)
versus

$$𝐟_\mathrm{V}=(𝐌\mathrm{grad})𝐁_{int}.$$
(9)
Where the first expression gives a nonzero force density equal to (7), it is zero in the second case. The reason for the difference between the nonzero result of Eq. (7) and the zero one of Eq. (9) is the following: the variant form of the Helmholtz force (3) is a direct function of any approximation of $`\overline{\chi }`$ whereas the correct definition of $`\overline{\chi }`$ was incorporated into $`𝐟_\mathrm{V}(\chi )`$ $`(`$see Eq. (4)$`)`$. That is the deeper reason why approximations cause differences if the two formulae for the Helmholtz force are used. It has to be noted that this discrepancy is limited to a small subregion $`\chi =\chi _L0.06`$ which is outside the usual experimental fluids. The lowest susceptibility of commercially available fluids is 0.13 .

For $`\chi =\chi _L>0.06`$ a truncation in the expansion of $`\overline{\chi }`$ after the linear order is deficient (see Fig. 1). If one inserts instead the entire term $`\overline{\chi }=\chi _L(1\chi _L+\chi _L^2)`$ in Eq. (3), one obtains a nonzero force density also for $`𝐟_\mathrm{V}`$,

$$𝐟_\mathrm{V}=\frac{B_{ext}^2}{\mu _0}(13\chi _L)\chi _L\mathrm{grad}\chi _L,$$
(10)
which is a good approximation of (7) for small $`\chi _L`$.

These theoretical calculations as well as the experimental measurements in  show apparently that (i) a linear dependence of $`\chi `$ on the density results not necessarily in a linear dependence of $`\overline{\chi }`$ on the density and (ii) nonlinear contributions of $`\rho `$ are relevant for $`\overline{\chi }`$ even in the region $`\chi 1`$. (iii) The two formulae for the Helmholtz force are entirely equivalent. It is only when one introduces approximations that differences arise in a small subregion, $`\chi =\overline{\chi }=\chi _L0.06`$.


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# Super-Eddington outburst of V4641 Sgr

## 1 Introduction

The X-ray transient V4641 Sgr (SAX J1819.3-2525) was discovered by BeppoSAX and RXTE observatories in Feb 1999 (in’t Zand et al. (1999), Markwardt et al. (1999)). During most of 1999 the source demonstrated only weak X-ray activity (see e.g in’t Zand et al. (2000)), until September 1999 when series of very bright and short X-ray flares occurred within less than $`1.52`$ days. During the brightest flare, detected by the All Sky Monitor aboard RXTE the source reached the level of $``$12.2 Crab within a few hours (Smith, Levine & Morgan (1999)). Subsequently the X-ray flux from V4641 Sgr rapidly decreased and totally disappeared within less than $`0.3`$ day. On the decaying part of this giant outburst a pointed TOO RXTE observation of the source has been performed (see e.g. Markwardt et al. (1999)).

Analysis of optical images showed that the newly discovered X-ray transient can be associated with a variable star discovered by Goranskij (Goranskij (1978, 1990), Samus et al. (1999)). Previous unusual activity of this star was observed in 1978 (Goranskij, 1978), indicating that V4641 Sgr might be a recurrent transient with the recurrence time of $`20`$ years.

During the giant outburst in Sep., 1999 strong variability of V4641 Sgr was observed at all wavelengths – radio (Hjellming et al. (1999)), optical (Stubbings (1999), Kato et al. (1999)), X-rays (1-12 keV) and hard X-rays (20–100 keV) (McCollough et al. (1999)). The maximal observed optical brightness was at the level of $`m_\mathrm{V}8.8`$ (Stubbings (1999)). Spectroscopic observations in the optical band performed during the outburst indicated a presence of a high velocity wind (Charles et al. (1999)).

The VLA images, obtained on Sep.16.03, soon after the brightest 12.2 Crab flare (occurred on Sep.15.7, 1999), revealed an elongated extended radio source with a size of $`0.25\mathrm{}`$ (e.g. Hjellming et al. (2000)). This led to a suggestion that V4641 Sgr might be a new Galactic superluminal source. However, determination of the jet velocity was complicated by quick decay of the radio flux and the absence of any direct observations of the apparent motion, in contrast to the three previously known Galactic superluminal sources GRS1915+105, GRO J1655-40 and XTE J1748-288.

Optical spectroscopy and photometry of the source performed during the quiescence measured all major parameters of the binary system (Orosz et al. (2001), Table 1), including the mass of the primary $`M_{\mathrm{primary}}`$8.7–11.7$`M_{}`$ and of the secondary $`M_{\mathrm{secondary}}`$5.5–8.1$`M_{}`$, making V4641 Sgr a firm black hole candidate in a binary system with a high mass companion. The distance to the source was constrained in the range of 7–12 kpc(Orosz et al. (2001), Chaty et al. (2000)), which exceeds significantly the initial distance estimates of 0.5 kpc (e.g. Hjellming et al. (2000)). Chaty et al. (2000) and Orosz et al. (2001) infer slightly different distance estimates, but this difference do not influence strongly on our results. In our paper we will use the estimate obtained by Orosz et al. (2001).

Based primarily on the optical data: (i) significant brightening of the source during the outburst, by $`\mathrm{\Delta }m_V5`$, unusual for an HMXB transient and (ii) large peak optical flux, $`m_{\mathrm{V},\mathrm{peak}}8.5`$, Revnivtsev et al. (2002) suggested that in Sept.1999 V4641 Sgr might have had an episode of a super-Eddington accretion. Super-Eddington accretion rate led to a formation of a massive optically thick and geometrically extended envelope/outflow which enshrouded the central black hole. The envelope, being optically thick in the optical and X-ray bands absorbed/reprocessed the primary emission of the central source and re-emitted bulk of the accretion energy in the UV and EUV bands. Being the direct consequence of near- or super-Eddington accretion onto the black hole, the envelope vanishes during the subsequent evolution of the source when the apparent luminosity drops well below the Eddington value. In this paper we present the results of analysis of the data of Rossi X-ray Timing Explorer data and demonstrate that the X-ray data provides additional strong evidence in support of such picture.

In Sects. 2 and 3 we describe results of analysis of the RXTE data. In Sect. 4 we summarize the overall picture emerging from the RXTE data and discuss the X-ray evidence of the extended optically thick envelope surrounding the X-ray source during the maximum of its activity in Sept.1999.

## 2 Observations and data analysis

In our analysis we used publicly available RXTE data of V4641 Sgr . This includes 11 pointed observations in Sep., 1999, 61 sets of the observations scanning over the Galactic bulge region, performed from Feb.5, 1999 till Oct.24 1999, and three sets of scans over the Galactic bulge in Oct. 2000. In addition to this we used light curves of V4641 Sgr obtained by RXTE All Sky Monitor (ASM) in three energy channels (1.2–3–5–12.2 keV). The RXTE/ASM lightcurves of V4641 Sgr were provided by the RXTE/ASM team (http://xte.mit.edu/ASM\_lc.html).

The data reduction of PCA was performed with the help of standard procedures from FTOOLS/LHEASOFT 5.1 package. In order to avoid possible additional problems with the xenon edge at 4.8 keV (that became more pronounced with Epoch 4 response matrix) for our spectral analysis we used only first layer data from all Proportional Counter Units (PCUs). To be convinced that our procedure allow us to perform the spectral analysis correctly we extracted the PCA spectrum of Crab Nebulae from the observation 1999 Sep.13. Here we also used only the first layer data of all PCUs. The spectrum then was fitted by the conventional model: the power law with a photon index $`\mathrm{\Gamma }2.06`$ with interstellar absorption ($`N_\mathrm{H}L`$ was fixed at the value of 4$`\times 10^{21}`$ cm<sup>-2</sup>). Residuals do not exceed the value of about 1%. Therefore in subsequent analysis we used the value 1% as a rough estimation of systematic uncertainties in the energy band 3–20 keV. In reality it appears that the uncertainties in the response matrix do not exceed 10% at energies up to $``$40–50 keV therefore in some cases we used PCA data to illustrate approximate behavior of the source at these energies. For the estimation of the PCA background we used VLE-based model when the source is sufficiently bright ($`>`$40 cnts/s/PCA) and L7\_240 model when the source is weak. The nominal accuracy of the background estimation ($``$1–2% of the background value, see e.g. http://lheawww.gsfc.nasa.gov/$``$keith/dasmith/Epoch4/ systematics\_l7\_240.htm) allows us to follow a source behavior down to a level of the order of 0.1–0.5 mCrab. At such low level of the source activity the Galactic diffuse emission can also become important. We estimated the contribution of the diffuse emission basing on the results of e.g. Yamauchi & Koyama (1993), Yamasaki et al. (1997) and found it small ($`<`$0.1-0.5 mCrab) at the position of the source ($`l=6.774`$, $`b=4.789`$).

For the reduction of HEXTE data we used standard tasks of FTOOLS/LHEASOFT 5.1 package. For the HEXTE spectral analysis we used Archive mode (64 energy channels for total energy band 15-250 keV, 16 sec time resolution). We analyzed Cluster A and Cluster B data separately and found that in each case their results are consistent with each other. During fitting procedures we left normalizations of HEXTE clusters to be free parameters. Then, for plotting purposes the HEXTE different clusters points were averaged. Note here that absolute normalizations of HEXTE spectra on figures were adjusted to match the PCA spectra.

## 3 RXTE results

### 3.1 Long term behavior of the source in 1999

To follow the flux history of V4641 Sgr in 1999 we used publicly available data of RXTE/PCA scans over the Galactic Center region, that were performed almost bi-weekly during the whole year. The statistical significance of the data and the accuracy of the background subtraction allow us to detect any source down to the level of approximately 1–2 mCrab (if the Galactic diffuse emission do not contribute much to the detected X-ray flux at the position of the source). The method of Galactic Center map construction and the extraction of the source flux is described in Revnivtsev, Sunyaev (2002).

For the first time the V4641 Sgr was statistically significantly detected in PCA scan on Feb.18, 1999 (Markwardt et al. (1999)) and since then it was seen in almost every scan. We present the obtained light curve of V4641 Sgr in Fig. 1. The results of our analysis (61 data points) are in agreement with the 7 data points reported in Markwardt et al. (1999) and Markwardt et al. (1999).

After almost 6 months of moderate X-ray activity, during the first half of Sep.1999 V4641 Sgr demonstrated several X-ray outbursts. The first, the weak one, was detected by BeppoSAX and RXTE/ASM on Sep.10.1, 1999. The source X-ray flux reached $``$300 mCrab (in’t Zand et al. (2000)). On Sep.14–15, 1999 three more powerful flares were detected. The segment of the light curve of V4641 Sgr around Sep.14–15, 1999 is presented in Fig. 1(lower panel). It is seen that the source rose up to 4, 12 and 2 Crabs on Sep.14.9, Sep.15.7 and Sep.15.9 respectively. The observed large changes in X-ray flux (factor of 10 at least) occurred on the time scales of one–two hours. The X-ray luminosities of the source in the energy band 1–12 keV during these outbursts could be estimated to be $`110^{39}`$ ergs/s, $`3.410^{39}`$ and $`710^{38}`$ ergs/s respectively (with adopted distance to V4641 Sgr $``$9.5 kpc, Orosz et al. (2001)).

The last X-ray flare finished on $``$Sep.15.95, 1999 by the rapid drop in X-ray flux from the level of $``$100 mCrabs by a factor of 10 and after this the source returned to the quiescent state - $``$1 mCrab. Note, that at such low flux levels some contamination from the Galactic diffuse emission is possible. Our estimates of the contribution of the Galactic diffuse emission at the position of V4641 Sgr showed that it is small, but not negligible. As a very conservative estimation of the source flux the detected 1 mCrab flux at the position of V4641 Sgr should be treated as the upper limit.

### 3.2 Orbital modualtion of the X-ray flux

In spite of the fact that the significance of the source detection in the RXTE/ASM data is lower than in the RXTE/PCA data (during one day of observations), ASM points have advantage from the point of view of their quasi-uniform coverage over the period of Feb.-Sep., 1999. This helps us to search for the source period in X-ray data. Periodicities of V4641 Sgr were sought by means of the Lomb-Scargle periodograms (Lomb (1976), Scargle (1982), Press et al. (1992)). In Fig. 2 we present the Lomb-Scarge periodogram obtained for V4641 Sgr lightcurve taken in the period of steady state activity $``$Mar.13– Aug.20, 1999 ($``$TJD11250-11410)

It is seen that almost at the position of detected optical period $`P=2.8173`$ days(Orosz et al. (2001)) a peak at the X-ray Lomb-Scarge periodogram is present. This peak corresponds to the period $`P_\mathrm{x}=2.84\pm 0.03`$ days. The uncertainty of the period value was estimated by a Monte-Carlo bootstrap method, assuming the gaussian distribution of values of ASM lightcurve points. The false-alarm probability of this detection (taking into account the number of trial periods) is slightly less than $`10^3`$, if we assume the exponential distribution of Lomb-Scargle power values. It is not very high significance to rely on X-ray data alone. However, the marginally detected X-ray periodicity has the value of the period that coincides within 1-$`\sigma `$ errors with the firmly detected optical one $`P=2.8173`$ days. This strongly supports the detection of the binary period in X-rays.

We have folded the lightcurve of V4641 Sgr with the measured optical period of the system in order to search for the orbital dependence of the X-ray flux. The obtained orbital profile of the X-ray flux(1.5-3.0 keV, lowest ASM energy channel) is presented in Fig. 3. In order to make the comparison of optical and X-ray folded lightcurves easier we have used the same reference time $`T_0`$ as Orosz et al.(2001) in their Fig. 3. It is seen that the folded X-ray lightcurve demonstrates peak, when the black hole is located between the observer and the optical star, and the minimum - when the star is located between the observer and the black hole. We also detected strong dependence of the amplitude of orbital modulations of X-ray flux on the photon energies: for the lowest energies, 1.5-3.0 keV, the amplitude of the sinusoidal variations is $`36\pm 8`$%, in the energy band 3-5 keV – $`25\pm 5`$%, and in the energy band 5-12 keV the modulations is undetectable with an upper limit $`<15`$%(2$`\sigma `$). It should be noted, that the observed energy dependence of the X-ray orbital modulations and the position of the X-ray minimum on this modulation suggest that the detected X-ray variations could be caused by an absorption in the line of sight near the optical star. This suggests that the inclination of the system is close to 65–70, in agreement with the optical data (Orosz et al. (2001)).

### 3.3 The spectral evolution of the source

#### 3.3.1 Period of “quiescent” activity in Feb.-Sep.,1999

The scan observations give us an important opportunity to follow the spectral shape of the source during a year. Unfortunately the acceptable “on-source” exposure of a scan observation is only of the order of 10–20 secs. Therefore the statistics in the obtained spectra is quite poor. During the period Feb.-Sep. 1999 the source was detected with quite soft spectrum – which could be roughly described by the model of bremsstrahlung emission with temperatures $`kT`$2–3 keV or by multicolor disk model (Shakura &S unyaev (1973)) with the inner disk temperature $`kT1.5`$ keV. The typical spectrum of V4641 Sgr at that time is presented in Fig. 4(upper panel).

The spectrum of V4641 Sgr obtained by BeppoSAX observatory on Mar.13, 1999 (see in’t Zand et al. (2000)) has the statistically significant emission line at the energy $`7`$ keV with equivalent width $``$270 eV. Therefore we also searched for the emission line in the PCA scan data. Unfortunately, due to poor statistics, the emission line could not be detected in a single PCA scan observation with an upper limit on its equivalent width $`EW<`$0.7-1.0 keV. However, a fit to spectrum of V4641 Sgr , averaged over the period Feb.18–Sep.02, 1999 gives an emission line at the energy $`E_{\mathrm{line}}=6.60\pm 0.08`$ keV with the equivalent width $`EW=360\pm 90`$ eV.

The X-ray spectrum of the source strongly changed in the beginning of Sep 1999 after the dip in the light curve (see Fig. 1). The photon spectral index hardens - to $`\alpha 1`$ \- and the emission line became stronger - $`EW`$1–2 keV (with typical uncertainty $`\sigma _{\mathrm{EW}}`$200-300 eV). The spectrum averaged over Sep.6-12, 1999 is presented in Fig. 4(lower panel). The spectrum resembles the one obtained by BeppoSAX on Sep.10, 1999 (in’t Zand et al. (2000)). Note, that approximately simultaneously with the dramatic changes in the X-ray spectral properties of the source the increase of the source optical activity was detected (Kato et al. (1999)).

#### 3.3.2 Period of flaring activity (Sep.14.8-15.9, 1999)

During the outburst activity on Sep.14-15, 1999, the source demonstrated at least three powerful X-ray flares (Fig. 1), two of which were detected by the ASM instrument. ASM data indicated that during the flares the spectral hardness of the source was generally anticorrelated with the X-ray flux.

Between the two ASM flares, on $``$Sep.14.9, the source flux dropped by a factor of 20 at least and became undetectable by the ASM. Fortunately, at this time, on Sep.15.1, 1999 a PCA scan observation was performed, allowing us to investigate the spectrum of V4641 Sgr between the two flares. During this observation a remarkable spectrum was obtained (Fig. 5). The spectrum is dominated by the emission line at $`E_{\mathrm{line}}=6.63\pm 0.08`$ keV with enormous equivalent width of $`EW=2.4\pm 0.3`$ keV. Remarkably, this spectrum is very similar to an X-ray spectrum of SS433 (e.g. Margon (1984)).

#### 3.3.3 The pointed RXTE observation (Sep. 15.89-15.95, 1999)

The third of the detected bright flares occurred during the decaying part of the outburst and was missed by the ASM because of $``$1.5 hour gap between the ASM points. Coincidentally, it occurred during the pointed observation of RXTE. As it was previously mentioned by Markwardt et al. (1999) the spectrum of the source at the peak of the X-ray light curve during this RXTE observation was quite hard and resembled the typical spectra of the black holes in the low/hard spectral state with the 3–50 keV photon index $`\alpha <`$2.0, the cutoff at the energies 100-200 keV, and pronounced fluorescent Fe line at 6.4 keV.

However, time resolved spectral analysis of the RXTE/PCA data revealed significant quantitative and qualitative evolution of the source spectrum during $`1500`$ sec of the pointed RXTE observation. In Fig. 6 we present the light curve of the source with 16 sec time resolution, softness ratio (3–5 keV to 15–20 keV), the centroid energy of the Gaussian line and its equivalent width as a function of time. The position of the line and its equivalent width were determined using a simple power law + Gaussian line approximation of the spectrum in the 3–12 keV energy band. In the uppermost panel we also show behavior of the integrated fractional rms (in percents) of the source flux variations (3–20 keV energy band, 0.5-10 Hz frequency range). In order to illustrate the spectral evolution of V4641 Sgr we show in Fig. 7 the broad band spectra accumulated during four intervals, marked in Fig. 6 (lower panel) by the horizontal lines.

As is apparent from Figs.6 and 7 the RXTE observation can be divided into two parts with qualitatively different spectral properties with the boundary at $`t1100`$ sec (in the units of Fig. 6) corresponding to the final drop of the X-ray flux and change of the iron line energy from $`6.4`$ keV to $`6.66.8`$ keV.

During the first part the source had a strong emission line centered at $``$6.4 keV with the equivalent width varying between 200 and 900 eV, sufficiently hard spectrum extending to the hard X-ray energies and significant aperiodic variability with fractional rms $`1540\%`$. In order to qualitatively illustrate the character of the spectral evolution, we show in Fig. 8 three spectra, accumulated during individual 16 sec intervals, corresponding to significantly different values of the line equivalent width and fractional rms.

The Figs.6 and 8 demonstrate that the spectral evolution can be qualitatively understood as a result of absorption/reprocession in the extended medium with varying absorption column density. Indeed, assuming that the primary spectrum does not change significantly, decrease of the absorption column density would lead to the apparent softening of the outgoing spectrum and decrease of the equivalent width of the fluorescent iron line. If the absorbing/reprocessing medium has a significant spatial extend with the light crossing time of $`1050`$ sec. the variations of the primary emission would be smeared out in the reprocessed emission, the effect depending on the fraction of the scattered/reprocessed emission in the outgoing radiation. Thus, decrease of the absorption column density would lead to increase of the apparent fractional rms. It should be noted, that absorption by the neutral medium with solar element abundances does not adequately explain the observed spectra – certain ionization of the absorbing gas is required by the data. The maximal $`N_\mathrm{H}L`$ value should be of the order of $``$few$`\times 10^{23}`$cm<sup>-2</sup>.

We have not found any strong soft component in the spectrum during this part of the observation. However, this issue is rather complicated taking into account the absence of the spectral data at energies lower than 3 keV.

After the final drop of the X-ray flux at $`t1100`$ sec a significant softening of the spectrum occurred and the line shifted from $`6.4`$ keV to $`6.66.8`$ keV indicating a significant change of the emission regime.

At the maximum of X-ray lightcurve, when the absorption was presumably weak the source had ordinary hard spectrum, typical for black holes in the low spectral state (Fig. 7 and 9). Remarkably, V4641 Sgr have demonstrated this type of spectrum while it’s luminosity exceeded by $``$10 times that of Cyg X-1 in the hard and, probably by $``$3-5 times in the soft spectral states. Let us mention that masses of black holes in both systems are comparable. Therefore the difference in luminosity might give an information about the accretion rate.

### 3.4 Short-term variability

The only data suitable to study short term variability of V4641 Sgr during the period of flaring activity in Sept.1999 are that of the pointed RXTE observation discussed in the previous subsection. The brief description of the source variability during this observation can be found in Wijnands & van der Klis (2000). During the first $``$1100 sec of the observation the V4641 Sgr was found to be strongly variable (rms amplitude $``$50%) with a power law power spectrum in the $`10^25`$ Hz frequency range. At the frequency of $`5`$ Hz the power spectrum changed from $`Pf^1`$ to $`Pf^2`$. It is interesting to note that in spite of similarity of the spectral properties of V4641 Sgr with the spectral properties of Cyg X-1 in the hard state the power spectrum of V4641 Sgr flux variability is more similar to that of Cyg X-1 in the soft state.

We discuss below change of the aperiodic variability properties with time, photon energy dependence of the fractional rms and time delay of the reflected emission.

As was shown in the previous subsection, during the RXTE observation the source demonstrated a strong spectral evolution accompanied with significant change of the fractional rms (Fig. 6). Similar to the spectral properties, the variability level changed significantly after the rapid drop of the X-ray flux at $`t`$1100-th sec (Fig. 6). The fractional rms droped from $`3040\%`$ to the level, undetectable with PCA, with the $`2\sigma `$ upper limit of $``$1–2% in the $`510^310`$ Hz frequency band.

A notable feature of the energy dependence of the fractional rms is the decrease near the energy of the Fe $`K_\alpha `$ line. Note that some indications on such behavior could be noticed in Fig. 3 of Wijnands & van der Klis (2000). However the authors concentrated on the properties averaged the entire outburst. In Fig. 10 we present the dependence of rms amplitude of the source variability calculated for two different periods - intervals $`<`$300-th second in the time units of Fig. 6 (high EW of the line) and $``$400–700-th sec (low EW of the line). One can see that there exist a definite dip approximately at the position of the Fe 6.4 keV fluorescent line. Moreover, it is seen that the stronger the line in the source’s energy spectrum, the stronger the dip at the rms-energy dependence. The presented rms-energy dependence clearly demonstrate that the fluorescent Fe line is less variable than the continuum. The simplest interpretation of this fact could be the smearing of the reprocessed emission (in particular the flux in the Fe fluorescent line) because of the finite light crossing time of the reprocessing medium (see e.g. discussion in Revnivtsev et al. (1999), or Gilfanov et al. (2000)).

The reprocessing in medium of large light crossing time can also result in the time delay between the direct continuum emission and the photons of the reprocessed spectrum, in particular – the Fe line photons. In order to check this hypothesis we have crosscorrelate the continuum flux of V4641 Sgr and the flux in the fluorescent Fe line. Flux in the Fe line was taken from the spectral approximation used for Fig. 6. In order to avoid possible contamination by long term trend in the parameters we used only data during the period with relatively stable value of equivalent width of the fluorescent line – from $``$350-th to $``$700-th seconds (in the time units of Fig. 6). The obtained crosscorrelation is presented in Fig. 11. The time interval of the acceptable data is rather short and we could not calculate the uncertainties on the crosscorrelation function directly from the data. Therefore we estimated the error bars using Monte Carlo bootstrap method. From Fig. 11 one can see that the crosscorelation function is strongly asymmetric with respect to the zero delay, implying that the flux in the Fe fluorescent line is delayed with respect to the continuum flux. The approximate time of the delay is $`\tau `$50 sec.

## 4 Discussion

### 4.1 V4641 Sgr – Summary

Based on the available RXTE data of the Galactic Center scans, ASM monitoring and RXTE pointed observation the overall picture of the V4641 Sgr evolution can be summarized as follows:

1. During approximately a half of a year after its discovery V4641 Sgr remained in the “quiet” state (Fig. 1) with X-ray luminosity at the level of $`L_X10^{36}`$ erg/sec (flux $`1020`$ mCrab) and a soft spectrum (Fig. 4).
2. A “landmark” in V4641 Sgr evolution was a dip which started on Sept.2 and lasted for $`10`$ days (Fig. 1). The source luminosity droped by a factor of $`10`$. After the dip the source spectrum changed dramatically (Fig. 5) and the optical emission increased by $`\mathrm{\Delta }m_V`$2 (Kato et al. (1999)).

Interestingly, the apparent size of the radio jet can be reconciled with the constrains on the binary system inclination angle only assuming that the ejection occurred before Sept.6. It seems plausible to associate the jet ejection with the X-ray dip.
3. On Sept.14.9 a period of flaring activity started (Fig. 1, lower panel, Fig. 12). Although, due to fastness of the events, the data are rather sparse, comparison of the optical and X-ray light curves (Fig. 12) suggests sufficiently smooth evolution of the optical light, probably reflecting change of the bolometric luminosity and/or mass accretion rate. The X-ray flux, on the contrary, changed in a rather irregular fashion. Three bright X-ray flares were detected during rising and decaying parts of the optical light curve, with a deep minimum at the epoch of the maximal optical/bolometric luminosity. The source spectrum (Fig. 5) during the X-ray minimum had a strong emission line at $`6.6`$ keV with equivalent width of $`2.4`$ keV, indicating dominant contribution of the reflected/reprocessed emission. During the brightest flare the source reached flux level of 12.2 Crab corresponding to the 1-10 keV luminosity of $`(34)10^{39}`$ erg/sec or exceeded Eddington luminosity for a 10 $`M_{}`$ black hole.
4. The final phase of the third flare was studied by collimated instruments aboard RXTE. The spectral evolution during the flare can be understood in terms of absorption by ionized medium of varying column density. Strong fluorescent line of iron present in the spectra had smaller fractional rms than the continuum flux and was delayed with respect to the continuum by $`2550`$ sec.
5. In the period of low absorption the source demonstrated a hard spectrum typical for black holes in the low spectral state (Fig. 9). Its luminosity, however, exceeded by a factor of $`10`$ and $`23`$ respectively the Cyg X-1 luminosity in the hard and the soft spectral states.
6. An orbital modulation of the X-ray flux during the period of quiescence was detected with fractional amplitude of $`30\%`$. The phase and energy dependence of the orbital modulation is consistent with obscuration by the matter in the vicinity of the optical companion, in which case the inclination of the binary system should be close to $`6570\mathrm{°}`$

### 4.2 Super-Eddington accretion and optically thick envelope

Earlier, we have suggested (Revnivtsev et al. (2002)), that the optical data collected during the period of flaring activity of V4641 Sgr can be naturally understood assuming formation of an optically thick warm ($`T10^5`$ K) envelope/outflow enshrouding the central source. The envelope is a direct consequence of significantly super-Eddington accretion and disappears when the mass accretion rate decreases below the Eddington value. Such an envelope, being optically thick at the optical wavelengths due to free-free processes and in the X-ray band due to absorption by the metals and Compton scattering, absorbs and re-emits bulk of the central source luminosity. In such a picture, smooth behavior of the optical light reflects evolution of the bolometric luminosity and, possibly, of the mass accretion rate. The bright X-ray flares occurred on the rising and decaying part of the optical light curve are a result of the changes in geometry and/or optical depth of the envelope.

At the peak of the optical light (which likely corresponded to the peak of the bolometric luminosity and the maximum in the optical depth of the envelope) the central source was almost completely obscured, which caused deep minimum in the X-ray flux. The weak X-ray emission observed in the scanning observation could be a result of reprocession of the primary X-rays by surrounding warm Compton thick gas. This is in good qualitative agreement with the actually observed spectrum (Fig. 5) which is extremely hard and has very strong fluorescent line of iron with equivalent width of $`2.4`$ keV. The line centroid energy, $`E6.7`$ keV requires significant ionization of iron. An alternative explanation of the observed large equivalent width of the line could be thermal emission from optically thin gas in the base of the jet, similarly to interpretation of the spectra of SS433. The picture could be clarified if the hard X-ray data was available.

The only broad band spectroscopical data available is that of the RXTE pointed observation performed in the end of the outburst. Coincidentally, it caught the tail of a short flare occurred during decaying part of the outburst. The spectral evolution observed by RXTE can be understood as an effect of absorption by ionized gas with the column density decreasing with time. This picture is further supported by the study of variability of the iron K<sub>α</sub> emission. We found that fractional rms of the iron K<sub>α</sub> flux is smaller than that of the surrounding continuum (Fig. 10). This result can be easily understood as smearing of the variations on the time scales shorter than the light crossing time of the reprocessing media. In addition, the finite light crossing time of the reprocessing media should cause time delay of the reprocessed emission with respect to the primary flux – in a good agreement with the observed behavior (Fig. 11). The amplitude of the observed time delay, $`\tau 50`$ sec, corresponds to the linear size of $`10^{12}`$ cm, i.e. is of the order of the Roche lobe of the binary system, as should be expected.

## 5 Conclusions

1. We argue that X–ray data are broadly consistent with the assumption that 1999 September outburst of V4641 was caused by the episode of super-Eddington accretion onto a black hole accompanied by a formation of an extended envelope. The properties of the source during this outburst are similar to those of SS433 suggesting that formation of the envelope/outflow is a generic characteristic of the supercritical accretion as predicted by many theoretical models.
2. It is interesting however that hard spectrum, resembling the spectrum of Cygnus X-1 during low state, was observed from V4641 at the luminosity level more than order of magnitude larger than in Cygnus X-1.
3. Using ASM data during the extended period of relatively quiescent state of the source prior to the giant outburst we marginally detected periodicity in the 1.5-12 keV energy band, consistent with the optically determined orbital period.
4. Almost two weeks prior to outburst dramatic evolution of spectrum is observed, associated with the significant decrease of the source X-ray flux. If the subsequently observed extended radio source is due to ejection happened at this time (and not during the major outburst), then expansion velocity would be at the level of 0.7-0.8 c – similar to the velocity observed in several galactic jet sources.

###### Acknowledgements.

This research has made use of data obtained through the High Energy Astrophysics Science Archive Research Center Online Service, provided by the NASA/Goddard Space Flight Center.