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# Temperature dependence of polaronic transport through single molecules and quantum dots

## I Introduction

In recent years there has been a growing interest in electrical transport through single molecules Chen et al. (1999); Park et al. (2000); Bockrath et al. (1997); Joachim et al. (2000) and single electronic levels in quantum dots. Schmidt et al. (1997); Fujisawa et al. (1998); Qin et al. (2001) Some molecular devices exhibit switching behavior with large on-off ratios Chen et al. (1999) increasing the motivation to construct molecular electronic devices. Joachim et al. (2000) In some cases it has been found that the transport is quite temperature dependent Chen et al. (1999) and it has been suggested Ventra et al. (2001) that this is due to the presence of low energy boson modes, such as internal rotations, which couple strongly to the molecular electronic states, and can easily be excited by small temperatures. Hone et al. (2000); Armour and Blencowe (2001) In a similar vein, in double quantum dots it has been found that there are acoustic phonons which couple strongly to the electrons Fujisawa et al. (1998); Qin et al. (2001).

Some experimental values for the phonon energy have been estimated in various papers. In Table 1 we give some numbers for reference.

We see that the boson (usually phonon) frequency in these systems is quite small, corresponding to temperatures in the range 0.5 – 50 Kelvin. In addition there was a recent proposal Armour and Blencowe (2001) to consider transport through a quantum dot to a carbon nanotube cantilever with a resonant frequency of the order of 100 MHz, corresponding to a phonon energy of 0.4 $`\mu `$eV. If the electron-phonon coupling is sufficiently large polaronic transport might be important for these systems. When the electron tunnels through it can absorb or emit bosons, thus altering its energy and the current. If the temperature is much larger than the boson energy, there are many bosons available for absorption and this might heavily influence the current.

In 1959 Holstein Holstein (1959) predicted that for a periodic one-dimensional molecular crystal with strong electron-phonon coupling there should be a crossover from coherent (band) to incoherent (hopping) transport with increasing temperature. When increasing the temperature the effective bandwidth becomes narrower, this gives rise to a decrease in coherent transport. In contrast, increasing temperature means that more and more phonons are activated and we are in a regime where phonon assisted inter-site tunneling starts to contribute to the conductivity. This coherent-incoherent crossover is believed to have been observed for the first time quite recently in single crystals of pentacene. Schön et al. (2001) One aim of this paper is to see whether a similar crossover should be seen in polaronic transport through molecules and quantum dots. This might be expected because of the mathematical similarity between the models for periodic systems and the resonant tunneling case. We might expect the tunneling amplitude between the leads and dot to be reduced by polaronic effects, thereby reducing the coherent part of the conductivity. When increasing the temperature the electrons can tunnel with boson assisted transport that enhances the tunneling, possibly leading to a crossover behavior. There have been many theoretical investigations of the effect of phonons on the transport through molecules Seminario et al. (2001); Ventra et al. (2001); Hettler et al. (2002); Boese and Schoeller (2001); Emberly and Kirczenow (2000) and quantum dots Kang (1998); Hyldgaard et al. (1994); Wingreen et al. (1989); König et al. (1996); Li et al. (1995); Haule and Bonca (1999), but none of them focuses on the temperature dependence of the current. The purpose of this paper is to clarify this aspect of the transport. Li et. al Li et al. (1995) included a Hubbard term, but did not consider multi-phonon contributions. In a recent paper Emberly and Kirczenow Emberly and Kirczenow (2000) made a thorough analysis of conductance through a molecular wire. A set of self-consistent equations where set up and solved to give the distribution functions in the leads and molecule, and then transmission probabilities were calculated. However, the temperature dependence is not addressed in that paper.

In this paper we perform the analysis for the simplest possible case, where the electrons interact with a single optical boson localized on the dot or molecule. We anticipate that this is sufficient to illustrate the main physics in the more complicated case of many bosons, such as acoustic phonons. In order to obtain analytical results we have to assume that the coupling to the leads is small and the energy level in the dot or molecule is not too close to the Fermi energy in the leads. Hewson and Newns (1980); Hewson and Meyer  By assuming that the coupling to the leads is small we can calculate the effects from the bosons locally on the molecule/dot and then assume that the effect on the leads from the bosons is negligible. This enables us to use well-known results from mesoscopic transport theory. The bosons are possibly most often phonons, but since the theory will look identical (assuming linear couping) for different types of bosons (phonons, magnons, charge oscillations) we will simply refer to ”bosons”. Even in photon assisted tunneling through quantum dots side bands have been observed when tuning the photon energy. Oosterkamp et al. (1997) In section II we will define the model we use and in section III, we discuss the approximations we have to make. Different limits for the current are derived in section IV, and in section V we discuss the differential conductivity.

## II Current through a level coupled to a local boson mode

We consider the simplest possible model Hamiltonian and neglect the spin degree of freedom and any effects of electron-electron interactions. The system we study consists of the individual entities (left lead, molecule or quantum dot, and right lead) coupled via tunneling. We assume that we are dealing with a resonant tunneling situation, but the states in the dot (or molecule or any single level system) couples to some boson mode with characteristic frequency $`\omega _0`$, as shown in Fig. 1.

The Hamiltonian is given by

$$=_1+_2+_3+_{12}+_{23},$$
(1)
where

$`_1+_3={\displaystyle \underset{𝐤_1}{}}ϵ_{𝐤_1}c_{𝐤_1}^{}c_{𝐤_1}+{\displaystyle \underset{𝐤_3}{}}ϵ_{𝐤_3}c_{𝐤_3}^{}c_{𝐤_3},`$
$`_2=ϵ_0c_2^{}c_2+\mathrm{}\omega _0a^{}a+Mc_2^{}c_2(a+a^{}),`$
$`_{12}={\displaystyle \underset{𝐤_1}{}}t(c_{𝐤_1}^{}c_2+h.c.),`$
$`_{23}={\displaystyle \underset{𝐤_3}{}}t(c_{𝐤_3}^{}c_2+h.c.).`$
Here $`ϵ_0`$ is the energy of the level in the dot/molecule and $`t`$ is the energy associated with hopping onto/off the dot. The electronic dispersion in the leads are given by $`ϵ_{𝐤_1}`$ and $`ϵ_{𝐤_3}`$. $`M`$ is the coupling to the local boson mode with energy $`\mathrm{}\omega _0`$. We disregard the spin dependence for simplicity.

First we make a unitary transformation to diagonalize the Hamiltonian $`_2`$. The price we pay for this is that extra operators attach to the tunneling term in the Hamiltonian. The transformation is $`\overline{_2}=e^S_2e^S`$, where $`S=c^{}c\frac{M}{\mathrm{}\omega _0}(a^{}a)`$. This gives us

$$\overline{}_2=\mathrm{}\omega _0a^{}a\mathrm{\Delta }c_2^{}c_2,$$
(2)
where

$$\mathrm{\Delta }=\frac{M^2}{\mathrm{}\omega _0}ϵ_0.$$
(3)
When the central system is a quantum dot $`ϵ_0`$ (and thus $`\mathrm{\Delta }`$) can be adjusted by applying a gate voltage. After the transformation the tunneling part of the Hamiltonian becomes

$`\overline{}_{12}={\displaystyle \underset{𝐤_1}{}}t(c_{𝐤_1}^{}c_2X+h.c.),`$
$`\overline{}_{23}={\displaystyle \underset{𝐤_3}{}}t(c_{𝐤_3}^{}c_2X+h.c.),`$ (4)
where

$$X=\mathrm{exp}\left[\frac{M}{\mathrm{}\omega _0}(aa^{})\right].$$
(5)
The $`X`$-factors can be absorbed into a renormalized electron creation/annihilation operator in region 2, so that we are left with the usual resonant tunneling Hamiltonian except that the Greens function for the electrons on the molecule/dot has an additional complication. $`T_\tau c(\tau )c^{}(0)T_\tau \overline{c}(\tau )\overline{c}^{}(0)=T_\tau c(\tau )c^{}(0)T_\tau X(\tau )X^{}(0)`$. A formula for the current can be derived using a Landauer-Büttiker approach. Meir and Wingreen (1992); Jauho et al. (1994) First we calculate the current from the left lead onto the dot from the rate of change of particles in the left lead. A similar expression for the current from the dot to the right lead is derived and the total current through the system is obtained by combining these two formulas. The derivation is presented in detail in Ref. Meir and Wingreen, 1992 and Jauho et al., 1994. The result is that the current is given by

$$I(V)=\frac{2e}{h}𝑑ϵ\left[f_1(ϵ)f_3(ϵ)\right]\mathrm{Im}\left[\mathrm{tr}(\mathrm{\Gamma }G_2(ϵ))\right].$$
(6)
The applied voltage across the system is $`V`$ and it enters the two Fermi functions (the equilibrium Fermi level of the leads is chosen to be zero) $`f_1(ϵ)=f(ϵeV/2)`$ and $`f_3(ϵ)=f(ϵ+eV/2)`$. Further, $`G_2(ϵ)`$ is the Green function for the quantum dot including all effects from the boson system and the tunneling to the leads. The parameter $`\mathrm{\Gamma }`$ is

$$\mathrm{\Gamma }\frac{\mathrm{\Gamma }_1\mathrm{\Gamma }_3}{\mathrm{\Gamma }_1+\mathrm{\Gamma }_3},$$
(7)
where $`\mathrm{\Gamma }_{1(3)}=2\pi t^2D_{1(3)}(ϵ)`$, $`D_{1(3)}`$ is the density of states (DOS) in the left (right) lead. $`\mathrm{\Gamma }_{1(3)}`$ is the width of the central resonance due to the tunneling to the left ($`\mathrm{\Gamma }_1`$) and right ($`\mathrm{\Gamma }_3`$) lead. The total width of the local resonance, $`\mathrm{\Gamma }_2`$, is the sum of the two, $`\mathrm{\Gamma }_2=\mathrm{\Gamma }_1+\mathrm{\Gamma }_3`$.

For convenience we introduce the dimensionless parameters,

$`g_1\left({\displaystyle \frac{M}{\mathrm{}\omega _0}}\right)^2`$
$`g_2\left({\displaystyle \frac{\mathrm{\Gamma }}{\mathrm{}\omega _0}}\right)^2`$
We emphasize that there are many different energy scales associated with the system: $`k_BT`$, $`eV`$, $`\mathrm{}\omega _0`$, $`\mathrm{\Gamma }`$, $`M`$, and $`ϵ_0`$. The relative sizes of these energy scales have a significant effect on the current through the system and what approximations can be made in evaluating it.

The electrons will deposit/absorb energy from the bosonic system that has to be carried away/supplied. Therefore a question arises about how to define the temperature, particularly of the molecule or dot. We assume that the molecule/dot is in equilibrium with a bath and that the tunneling rate is small so that the system relaxes to the initial state after each tunneling event. In a quantum dot the bath can be the substrate that the quantum dot is manufactured on. For a molecule a surrounding cooling liquid Chen et al. (1999) can play the role of the bath. Otherwise, we have to assume that the deposited or absorbed energy is transferred to/from the molecule via the leads. As far as we are aware, this assumption is also (implicitly) made in all other theoretical work on this subject.

## III Approximate evaluation of the Greens function $`G_2(ϵ)`$

To be able to use Eq.(6) we have to calculate the local Green function, $`G_2(ϵ)`$. Due to the coupling to the leads finding $`G_2(ϵ)`$ is a highly non-trivial problem in many-body theory. Hewson and Newns (1980); Hewson and Meyer ; Haule and Bonca (1999) It is comparable in difficulty to the Kondo problem because of the possibility of non-perturbative effects. This is true even in equilibrium (i.e., in the absence of a bias, $`V=0`$). A recent study was made of a similar Hamiltonian (with spin) using the numerical renormalization group. Hewson and Meyer  We are interested in the non-equilibrium case where there is a bias. In order to simplify the analysis we have to rely on approximations, and the result will depend on how the $`X`$-operators from Eq.(5) are decoupled. One alternative is to assume that the coupling to the leads is small, $`\mathrm{\Gamma }_1+\mathrm{\Gamma }_3\mathrm{\Delta }`$, this is the approach taken here. This approximation is justified for small currents, as is the case in the systems considered here. If we were to include the effect on the leads from the bosons on the molecule/dot there would be a narrowing effect on $`\mathrm{\Gamma }`$. Hewson and Newns used variational and perturbation methods Hewson and Newns (1980) to show that this narrowing only takes place if the following conditions apply:

$`{\displaystyle \frac{M^2}{\mathrm{}\omega _0}}>\mathrm{\Gamma },g_1>1,\mathrm{}\omega _0>\mathrm{\Gamma }e^{g_1}`$
$`\mathrm{}\omega _0>|\mathrm{\Delta }|.`$
The conditions on the first line means that the electron-boson coupling has to be large enough to form a polaron. The last requirement on the first line means that individual boson satellites can be distinguished from each other. The second line tells us that if the level and boson satellites are too far from the Fermi level it is energetically unlikely to have virtual boson excitations, thus the leads are unaffected by the bosons. The narrowing is approximately given by

$$tte^{g_1(1/2+n_B)},$$
(8)
where $`n_B`$ is the Bose function,

$$n_B=\frac{1}{e^{\beta \mathrm{}\omega _0}1}$$
(9)
and $`\beta =1/k_BT`$.

The above considerations apply to equilibrium ($`V=0`$) whereas we are interested in the non-equilibrium situation of a finite bias, and particularly the resonant tunneling case where one of the leads’ Fermi level is close to the dot/molecule level ($`eV=\pm \mathrm{\Delta }/2`$). In that case the narrowing of the level width due to that lead (but not due to the second lead) may occur, e.g.,

$$\mathrm{\Gamma }_2=\mathrm{\Gamma }_1+\mathrm{\Gamma }_3\mathrm{\Gamma }_1+\mathrm{\Gamma }_3e^{g_1(1+2n_B)}.$$
(10)
If $`\mathrm{\Gamma }_1\mathrm{\Gamma }_3`$ this will lead to some quantitative but no significant qualitative changes in the current-voltage characteristics and so we will not consider them further.

We treat the leads as unaffected by the bosons, i.e., no narrowing of the bands in the leads. This means that we ignore the averages of the $`X`$-operators that appear in the tunneling part of the Hamiltonian, Eq.(4), the justification for this is given above. Below we will also assume that the leads give rise to a flat, energy independent, density of states. This is sometimes called the wide band limit. Wingreen et al. (1989) Otherwise $`\mathrm{\Gamma }`$ would be energy dependent. The quantum dot Green function calculated using these approximations is

$$G_2(t)=i\mathrm{\Theta }(t)e^{(i\mathrm{\Delta }\mathrm{\Gamma }_2/2)t/\mathrm{}}e^{\mathrm{\Phi }(t)}.$$
(11)
The factor $`e^{\mathrm{\Phi }(t)}`$ is due to the coupling to the boson and can be written Mahan (1990)

$`e^{\mathrm{\Phi }(t)}=e^{g_1(1+2n_B)}`$
$`\times {\displaystyle \underset{l=\mathrm{}}{\overset{\mathrm{}}{}}}I_l\left[2g_1\sqrt{n_B(1+n_B)}\right]e^{il\omega _0(t+i\beta /2)},`$ (12)
where $`I_l`$ denotes a modified Bessel function.

We Fourier transform the Green function and get an expression for the total current

$`I(V)={\displaystyle \frac{e\mathrm{\Gamma }}{h}}{\displaystyle _{\mathrm{}}^{\mathrm{}}}𝑑ϵ\left[f_1(ϵ)f_3(ϵ)\right]e^{g_1(1+2n_B)}`$
$`\times {\displaystyle \underset{l=\mathrm{}}{\overset{\mathrm{}}{}}}I_l\left[2g_1\sqrt{n_B(1+n_B)}\right]e^{l\mathrm{}\omega _0\beta /2}`$
$`\times {\displaystyle \frac{\mathrm{\Gamma }_1+\mathrm{\Gamma }_3}{(ϵ+\mathrm{\Delta }+l\mathrm{}\omega _0)^2+\frac{(\mathrm{\Gamma }_1+\mathrm{\Gamma }_3)^2}{4}}}.`$ (13)
We can interpret $`\mathrm{Im}\left[\mathrm{tr}(\mathrm{\Gamma }G_2)\right]`$, in Eq.(6), as the transmission coefficient for the tunneling. We plot this in Fig. 2 for a certain choice of parameters. The resonances to the left of $`(ϵ+\mathrm{\Delta })/\mathrm{}\omega _0`$ corresponds to absorption of bosons, and the ones to the right to emission of bosons. The middle line can be identified as the so called zero-boson transition.

The width of each satellite depends on $`\mathrm{\Gamma }_2`$ directly. When increasing the temperature the satellites increase in amplitude, indicating that it is easier to emit/absorb bosons. The asymmetry between negative and positive energies is due to the factor $`e^{l\mathrm{}\omega _0\beta /2}`$. This is a due to the fact that at low temperatures there are no available bosons to absorb.

In Fig. 3 we plot the current as a function of voltage using Eq.(13) for a set of parameters.

It show steps indicating that more and more satellites participate in conducting electrons. Note that the steps in Fig. 3 occur every second $`\mathrm{}\omega _0`$. This is simply because the satellites are positioned equidistant on each side of the central resonance, we have to increase the voltage by $`2\mathrm{}\omega _0`$ in order to cover the satellite. The first satellite starts to contribute to the current when $`eV=2\mathrm{\Delta }`$. A decrease of $`\mathrm{\Gamma }_2`$ ($`g_2`$ decrease) results in sharper steps, and a decrease in the amplitude of the current. When $`\mathrm{\Gamma }\mathrm{}\omega _0`$ (large $`g_2`$) the step structure disappears. Increasing the temperature results in the step structure being washed out to a smooth curve.

When increasing $`M`$, the amplitude of the current drops due a decrease of the factor $`e^{\left(\frac{M}{\mathrm{}\omega _0}\right)^2(1+2n_B)}`$ in Eq.(13). Increasing the temperature has the same effect. Without any coupling to the boson ($`M,g_1`$=0) we get a single resonant level without any satellites. This can be seen in Fig. 4 where we plot the current as a function of $`ϵ_0`$, the location of the energy level in the dot or molecule. The application of a gate voltage in a quantum dot would be equivalent to changing the level $`ϵ_0`$ (or $`\mathrm{\Delta }`$) .Fujisawa et al. (1998); Qin et al. (2001) We see a shoulder developing corresponding to the first boson satellite. A similar effect has been seen in a double quantum dot system. Fujisawa et al. (1998) The absence of a boson absorption peak in Fig. 4 is due to the low temperature, this comes from the factor $`e^{l\mathrm{}\omega _0\beta /2}`$. If we increased the temperature, or the electron-boson coupling, enough there would be more side bands visible.

## IV Limiting behavior for the current

In order to better understand the influence from the bosons on the current. Let us now have a look at the current in some limits.

### IV.1 $`M=0`$

If we put the coupling between the boson and the electrons to zero, we get:

$$I(V)=\frac{e}{h}_{\mathrm{}}^{\mathrm{}}𝑑ϵ\left[f_1(ϵ)f_3(ϵ)\right]\frac{\mathrm{\Gamma }_1\mathrm{\Gamma }_3}{(ϵϵ_0)^2+\frac{(\mathrm{\Gamma }_1+\mathrm{\Gamma }_3)^2}{4}}.$$
(14)
This would correspond to resonant tunneling without any bosons.

#### IV.1.1 $`k_BT\mathrm{\Gamma },eV`$

In this limit Eq.(14) reduces to the linear response expression

$$\frac{I}{V}=\frac{4e^2}{h}\frac{\pi \mathrm{\Gamma }}{k_BT\mathrm{cosh}^2\left(\frac{ϵ_0}{k_BT}\right)}$$
(15)
A similar form was used by Qin et. al Qin et al. (2001) to fit their experimental data.

#### IV.1.2 $`T=0`$

If the temperature goes to zero we can approximate the Fermi functions with step functions. Then, the integral over $`ϵ`$ can be performed and the result is

$$\underset{T0}{lim}I(V)=\frac{2e\mathrm{\Gamma }}{h}\left[\mathrm{tan}^1\left(\frac{eV2ϵ_0}{\mathrm{\Gamma }_1+\mathrm{\Gamma }_3}\right)+\mathrm{tan}^1\left(\frac{eV+2ϵ_0}{\mathrm{\Gamma }_1+\mathrm{\Gamma }_3}\right)\right].$$
(16)
Further, if $`eV`$ and $`2ϵ_0`$ is small compared to $`\mathrm{\Gamma }_1+\mathrm{\Gamma }_3`$ we can use the property that $`\mathrm{tan}^1(x)x`$, and we get

$$\underset{\stackrel{T0}{(eV,2ϵ_0)/(\mathrm{\Gamma }_1+\mathrm{\Gamma }_3)1}}{lim}I=\frac{4e^2\mathrm{\Gamma }}{h(\mathrm{\Gamma }_1+\mathrm{\Gamma }_3)}V,$$
(17)
i.e., a linear regime at low voltages. If, on the other hand, we take $`V\mathrm{}`$ in Eq.(16) we get

$$\underset{\stackrel{T0}{V\mathrm{}}}{lim}I=\frac{e\mathrm{\Gamma }}{\mathrm{}}.$$
(18)
This means that the whole resonant level contributes maximal to the current.

### IV.2 $`M0`$

#### IV.2.1 $`eVk_BT,\mathrm{}\omega _0`$

In this case we get the same limit as in Eq.(18) even if $`M0`$ from Eq.(13). This can be seen in Fig. 3 where all curves tend to the same value at large $`V`$. If we have that $`eV\mathrm{\Delta },k_BT`$ we can replace $`f_1(ϵ)f_3(ϵ)`$ by a factor 1, and the integral would extend between $`eV/2`$ and $`eV/2`$. But since $`eV`$ is greater than all other energies we extend the integral from $`\mathrm{}`$ to $`\mathrm{}`$. The integral gives a contribution $`\pi `$. All parts coming from the boson gives 1 and we again have the limit

$$I(eV\mathrm{\Delta },k_BT)\frac{e\mathrm{\Gamma }}{\mathrm{}}.$$
(19)
This limit can be seen in Fig. 3 where all curves tend to the same limit at high applied voltage.

#### IV.2.2 $`k_BT\mathrm{}\omega _0`$

Let us now investigate the limit $`k_BT\mathrm{}\omega _0`$. In this limit (corresponding to low temperatures) we can approximate the Bose function as $`n_Be^{\mathrm{}\omega _0/k_BT}1`$. All terms corresponding to positive $`l`$ vanishes. This is a result of the physical fact that positive $`l`$ corresponds to boson absorption but at $`T=0`$ there are no bosons. The Bessel function can be approximated as $`I_l(z)\frac{1}{l!}(z/2)^2`$ when $`z0`$. Then we get that the current becomes

$`I_{k_BT\mathrm{}\omega _0}={\displaystyle \frac{2e\mathrm{\Gamma }}{h}}e^{g_1}{\displaystyle _{\mathrm{}}^{\mathrm{}}}𝑑ϵ\left[f_1(ϵ)f_3(ϵ)\right]`$
$`\times {\displaystyle \underset{l=\mathrm{}}{\overset{0}{}}}{\displaystyle \frac{g_1^{|l|}}{|l|!}}{\displaystyle \frac{\frac{\mathrm{\Gamma }_1+\mathrm{\Gamma }_3}{2}}{(ϵ+\mathrm{\Delta }+l\mathrm{}\omega _0)^2+\frac{(\mathrm{\Gamma }_1+\mathrm{\Gamma }_3)^2}{4}}}.`$ (20)
#### IV.2.3 $`k_BT\mathrm{}\omega _0`$

For high temperatures we approximate the Bose function as $`n_Bk_BT/\mathrm{}\omega _0`$. The argument in the Bessel function is large and we can use the property

$$I_l(z)\frac{e^z}{\sqrt{2\pi z}},z1.$$
(21)
Using this, the current becomes

$`I_{k_BT\mathrm{}\omega _0}={\displaystyle \frac{2e\mathrm{\Gamma }}{h}}{\displaystyle \frac{e^{g_1\frac{\mathrm{}\omega _0}{4k_BT}}}{\sqrt{4\pi g_1k_BT/\mathrm{}\omega _0}}}{\displaystyle _{\mathrm{}}^{\mathrm{}}}𝑑ϵ\left[f_1(ϵ)f_3(ϵ)\right]`$
$`\times {\displaystyle \underset{l=\mathrm{}}{\overset{\mathrm{}}{}}}{\displaystyle \frac{\frac{\mathrm{\Gamma }_1+\mathrm{\Gamma }_3}{2}}{(ϵ+\mathrm{\Delta }+l\mathrm{}\omega _0)^2+\frac{(\mathrm{\Gamma }_1+\mathrm{\Gamma }_3)^2}{4}}}.`$ (22)
### IV.3 Saddle point approximation

If $`g_21`$ (i.e., $`\mathrm{\Gamma }\mathrm{}\omega _0`$) we can evaluate the current using a saddle-point approximation similar to that used previously in Ref. Schotte, 1966 and Armour and Blencowe, 2001. The exponential factor, $`e^{\mathrm{\Phi }(t)}X(t)X^{}(0)`$, in Eq.(12) can be written as

$$e^{g_1[(n_B+1)(1e^{i\omega _0t})+n_B(1e^{i\omega _0t})]}.$$
(23)
We approximate the exponential function in the exponent, $`e^z1+z+z^2/2`$, and we get:

$$G_2(t)ie^{i(\mathrm{\Delta }+g_1\mathrm{}\omega _0)t/\mathrm{}\mathrm{\Gamma }_2t/2\mathrm{}g_1/2(1+2n_B)(\omega _0t)^2}.$$
(24)
Let us assume that we can neglect the term linear in $`t`$ in the exponent compared to the quadratic one, i.e., $`g_1g_2`$. We Fourier transform the resulting Green function and get that the relevant factor entering Eq.(6) becomes

$$\mathrm{Im}\left[G_2(ϵ)\right]\frac{\mathrm{exp}\left[\frac{(g_1\mathrm{}\omega _0+\mathrm{\Delta }+ϵ)^2}{2g_1(\mathrm{}\omega _0)^2(1+2n_B)}\right]}{\omega _0\sqrt{g_1(1+2n_B)}}.$$
(25)
This approximation gives a broad Gaussian line shape covering all the boson satellites. This is in contrast to the individual boson satellites shown in Fig. 2. Using the saddle point approximation would give a Gaussian line shape in $`I(ϵ_0)`$, whereas a Lorentzian line shape occurs in the regime, $`k_BT\mathrm{\Gamma }\mathrm{}\omega _0`$, illustrated in Fig. 4.

The current using Eq.(25) is plotted in Fig. 5, and compared to the full expression, Eq.(13).

In this figure we can clearly see that the saddle point approximation cannot reproduce the actual current. Only for a small range of bias voltages, for low temperature and large coupling is there an agreement.

## V Differential conductance

The differential conductance, defined by

$$C=\frac{dI}{dV},$$
(26)
more clearly reveals the effect of the bosons. In general this is given by

$`C={\displaystyle \frac{e^2\mathrm{\Gamma }\beta }{h}}{\displaystyle _{\mathrm{}}^{\mathrm{}}}𝑑ϵ\left\{f_1(ϵ)\left[1f_1(ϵ)\right]+f_3(ϵ)\left[1f_3(ϵ)\right]\right\}`$
$`\times e^{g_1(1+2n_B)}{\displaystyle \underset{l=\mathrm{}}{\overset{\mathrm{}}{}}}I_l\left[2g_1\sqrt{n_B(1+n_B)}\right]`$
$`\times e^{l\mathrm{}\omega _0\beta /2}{\displaystyle \frac{\frac{\mathrm{\Gamma }_1+\mathrm{\Gamma }_3}{2}}{(ϵ+\mathrm{\Delta }+l\mathrm{}\omega _0)^2+\frac{(\mathrm{\Gamma }_1+\mathrm{\Gamma }_3)^2}{4}}}.`$ (27)
Later we will set $`eV=2\mathrm{\Delta }`$, which corresponds to resonant transport through the zero phonon feature. If we let the temperature go to zero in this expression we can approximate the Fermi functions together with the temperature as a delta function, $`\beta n_f(ϵ)[1n_f(ϵ)]\delta (ϵ)`$, and again only negative $`l`$ contributes, corresponding to emission of bosons, and we get

$`[C(V)]_{T0}={\displaystyle \frac{e^2\mathrm{\Gamma }_1\mathrm{\Gamma }_3}{2h}}e^{g_1}{\displaystyle \underset{l=\mathrm{}}{\overset{0}{}}}{\displaystyle \frac{g_1^{|l|}}{|l|!}}`$
$`\times [{\displaystyle \frac{1}{(\mathrm{\Delta }+l\mathrm{}\omega _0+eV/2)^2+\frac{(\mathrm{\Gamma }_1+\mathrm{\Gamma }_3)^2}{4}}}`$
$`+{\displaystyle \frac{1}{(\mathrm{\Delta }+l\mathrm{}\omega _0eV/2)^2+\frac{(\mathrm{\Gamma }_1+\mathrm{\Gamma }_3)^2}{4}}}].`$ (28)
We define

$$(C_{\mathrm{res}})^0[C(eV=2\mathrm{\Delta })]_{T0}.$$
(29)
For the particular case $`\mathrm{\Delta }\mathrm{}\omega _0,g_1\mathrm{}\omega _0`$, this simplifies to $`(C_{\mathrm{res}})^0\frac{2e^2}{h}\frac{\mathrm{\Gamma }}{\mathrm{\Gamma }_1+\mathrm{\Gamma }_3}e^{g_1}`$, showing how polaronic effects reduce the differential conductance.

In Fig. 6 we plot the differential conductance as a function of the applied voltage for different values of temperature and coupling parameters.

The peak at $`eV=2\mathrm{\Delta }`$ correspond to the zero-boson peak, and in the consecutive peaks one/two/three$`\mathrm{}`$, and so on, bosons are emitted or absorbed. As seen in this figure increasing the temperature, or the level widths, drastically affects the shape of the differential conductance.

In Fig. 7 we plot the differential conductance on resonance with the zero phonon line as a function of temperature for a range of parameters.

In this figure we see that the differential conductance generally decreases with increasing temperature, in contrast to the non-monotonic dependence found by Holstein Holstein (1959) for periodic molecular crystals. The corresponding crossover behavior does not occur for transport through molecules/quantum dots, since this would be indicated by an upturn in Fig. 7 when increasing the temperature. The absence of a crossover can also be seen by looking at Fig. 3 from that the slope at $`eV=2\mathrm{\Delta }`$ (i.e., the differential conductance) is almost constant when changing $`g_1`$ from 0 to 0.5. If we were to calculate the differential conductance in the limit when $`k_BT\mathrm{}\omega _0`$ from Eq.(22) we see that the temperature dependence of the differential conductance is governed by the pre-factor $`\frac{e^{g_1\frac{\mathrm{}\omega _0}{4k_BT}}}{\sqrt{4\pi g_1k_BT/\mathrm{}\omega _0}}`$ and this is a strictly decreasing function of the temperature, for reasonably values of $`g_1`$. Thus, there will never be an upturn in the differential conductance when increasing the temperature. This general behavior is not changed when $`g_1`$ is changed. Even an increased applied voltage, meaning that more boson satellites contributes, was not able to induce a crossover. However, changing $`\mathrm{\Gamma }`$ does alter the amplitude of the differential conductance, as seen in Fig. 7.

As mentioned above the temperature behavior is dominated by $`\mathrm{\Gamma }`$. If we put $`M=0`$ in Eq.(27) we can write the differential conductance as

$$[C_{res}]_{M0}=\frac{e^2\mathrm{\Gamma }}{h}\frac{\stackrel{~}{\mathrm{\Gamma }}}{k_BT}_{\mathrm{}}^{\mathrm{}}𝑑y[f^{}(y)+f^{}(y+\frac{2ϵ_0}{k_BT})]\frac{1}{y^2+(\stackrel{~}{\mathrm{\Gamma }}/k_BT)^2},$$
(30)
where $`\stackrel{~}{\mathrm{\Gamma }}(\mathrm{\Gamma }_1+\mathrm{\Gamma }_3)/2`$. If we now take $`ϵ_0=0`$ or $`k_BTϵ_0`$ we will have that the differential conductance is a universal function of $`\stackrel{~}{\mathrm{\Gamma }}/k_BT`$, i.e,

$$[C_{res}]_{M0}=F(\stackrel{~}{\mathrm{\Gamma }}/k_BT).$$
(31)
This can be seen in the lower graph in Fig. 7, where the two graphs for $`g_1=0`$ (but $`g_2=0.02`$ and $`2.0`$ respectively) collapse on the same line when the temperature axis is rescaled.

## VI Conclusion

In conclusion we see that the polaronic transport through a single molecule or quantum dot does not clearly exhibit the crossover from coherent to incoherent transport expected for the case of a periodic molecular crystal considered by Holstein Holstein (1959). The general behavior of the temperature dependence of the differential conductance is in large unaffected by the presence of the bosons. The temperature dependence is mostly determined by the linewidth (due to coupling to the leads) of the resonant energy level. The bosons produce side bands corresponding to absorption and emission of bosons. We also stressed that because of the interaction of the polaron on the dot or molecule with the leads there are potentially some very interesting problems in many-body physics Hewson and Newns (1980); Hewson and Meyer  to be explored in the model system we have considered.

U. Lundin acknowledges the support from the Swedish Foundation for International Cooperation in Research and Higher Education (STINT). This work was also supported by the Australian Research Council (ARC).


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# Cascade Boltzmann - Langevin approach to higher-order current correlations in diffusive metal contacts

## Abstract

The Boltzmann - Langevin approach is extended to calculations of third and fourth cumulants of current in diffusive-metal contacts. These cumulants result from indirect correlations between current fluctuations, which may be considered as ”noise of noise”. The calculated third cumulant coincides exactly with its quantum-mechanical value. The fourth cumulant tends to its quantum-mechanical value $`e^3I/105`$ at high voltages and to a positive value $`2e^2T/3R`$ at $`V=0`$ changing its sign at $`eV20T`$.

The fluctuation - dissipation theorem relates the spectral density of noise in equilibrium with the corresponding linear response of the system. This is why the second cumulant of current presents new information about the system only under nonequilibrium conditions. Nonequilibrium noise in mesoscopic systems has been extensively studied in the past decade. Unlike the second cumulant of current, its higher cumulants are not related with any average characteristics of the system even in equilibrium. Hence these quantities may be also of experimental interest.

In recent years, higher-order correlations of currents in mesoscopic systems received considerable attention of theorists. This work was pioneered by Levitov and Lesovik, who calculated the distribution of charge transmitted through a single-channel quantum contact. Subsequently, these calculations were extended to phase-coherent diffusive contacts in the zero-temperature limit. Very recently, the third cumulant of current was calculated for quasi-one-dimensional diffusive-metal contacts for arbitrary temperatures and voltages using the nonlinear $`\sigma `$-model and Keldysh formalism.

Along with the fully quantum-mechanical approach, higher-order correlations have been studied using a semiclassical description, which ignores quantum interference of wave functions yet takes into account the Fermi statistics of electrons. Semiclassical calculations of higher-order cumulants were performed for double-barrier structures using a master equation and for chaotic cavities based on the minimal correlation approach.

A semiclassical Boltzmann - Langevin approach has been very successful in describing the second cumulant of current in diffusive contacts. In particular, it gives the same value of the shot noise $`S_I=2eI/3`$ as a fully quantum-mechanical treatment. This is not surprising because the corrections to semiclassical values from quantum-interference effects like weak localization and mesoscopic fluctuations of conductance in dirty metals contain a small parameter $`1/p_Fl_{imp}`$, and the absence of this parameter in the noise magnitude implies that quantum interference is irrelevant to shot noise. As the values of higher cumulants obtained by Lee et al. either do not contain the quantum-interference prefactor as compared to the second cumulant, they can be also obtained semiclassically. This conclusion is supported by recent numerical results, which were obtained in a semiclassical model with exclusion principle.

The present paper extends the semiclassical Boltzmann - Langevin approach to calculations of the third and fourth cumulants of current for diffusive-metal contacts. We show that the main contribution to these quantities still results from second-order correlation functions of the Langevin sources in the Boltzmann - Langevin equation, whereas the effect of higher-order correlations of these sources is negligibly small in the diffusive case. As the result involves several hierarchically coupled second-order correlators, this approach may be termed ”cascade”.

The Boltzmann-Langevin equation for fluctuations reads

$$\left[\frac{}{t}+𝐯\frac{}{𝐫}+e\mathrm{𝐄𝐯}\frac{}{\epsilon }\right]\delta f(𝐩,𝐫,t)+\delta I$$

$$=e\delta 𝐄𝐯\frac{f}{\epsilon }+\delta J^{ext},$$
(1)
where $`\delta I`$ is the linearized collision integral and $`\delta J^{ext}`$ is the random extraneous flux. Fluctuations of physical quantities are expressed in terms of the fluctuations of the distribution function $`\delta f`$. For example, the fluctuation of current density is given by an expression

$$\delta 𝐣(𝐫,t)=e\underset{𝐩}{}𝐯\delta f(𝐩,𝐫,t).$$
(2)
In principle, the $`n`$th-order correlation function of any physical quantity may be calculated provided that the correlation functions of the extraneous sources $`\delta J^{ext}`$ are known up to $`n`$th order.

Kogan and Shulman calculated the second-order correlation function of the extraneous sources based on very simple physical considerations. The collision integral in the Boltzmann equation is of the form

$$I(𝐩,𝐫,t)=\underset{𝐩^{}}{}\left[J(𝐩𝐩^{})J(𝐩^{}𝐩)\right],$$
(3)
where $`J(𝐩𝐩^{})`$ and $`J(𝐩^{}𝐩)`$ are the outgoing and incoming scattering fluxes from and to state $`𝐩`$. It is natural to assume that all scattering events are local in space and the scattering fluxes between different pairs of states are statistically independent. Furthermore, since scattering events at different instants of time are independent, the scattering between each pair of states presents a Poissonian process whose second-order correlation function $`\delta J(t_1)\delta J(t_2)`$ is proportional to its average rate

$$J(𝐩𝐩^{})=W(𝐩,𝐩^{})f(𝐩,𝐫,t)[1f(𝐩^{},𝐫,t)],$$
(4)
where $`W(𝐩,𝐩^{})`$ is the classical scattering probability and the factor $`1f`$ takes into account the Pauli principle. Hence the correlation function of extraneous sources related with randomness of scattering may be written in a form

$$\delta J^{ext}(𝐩_1,𝐫_1,t_1)\delta J^{ext}(𝐩_2,𝐫_2,t_2)=\delta (𝐫_1𝐫_2)\delta (t_1t_2)$$

$$\times \{\delta _{𝐩_1𝐩_2}\underset{𝐩^{}}{}[J(𝐩_1𝐩^{})+J(𝐩^{}𝐩_1)]J(𝐩_1𝐩_2)$$

$$J(𝐩_2𝐩_1)\}.$$
(5)
The correlation function is positive if $`𝐩_1=𝐩_2`$ and negative if $`𝐩_1𝐩_2`$. In the latter case the only correlation is possible through scattering from $`𝐩_1`$ to $`𝐩_2`$ and vice versa, but this results in fluctuations of the corresponding occupancies of opposite signs.

In the case of a diffusive metal and low frequencies, the Boltzmann - Langevin scheme is greatly simplified. It is convenient to introduce a fluctuation of electric potential $`\delta \varphi `$ and random extraneous current

$$\delta 𝐣^{ext}(𝐫,t)=e\tau \underset{𝐩}{}𝐯\delta J^{ext}(𝐩),$$
(6)
where $`\tau `$ is the elastic scattering time. The fluctuation of current density is given by an expression

$$\delta 𝐣=\sigma \delta \varphi +\delta 𝐣^{ext},$$
(7)
where $`\sigma `$ is the metal conductivity. Because pile-up of charge is forbidden in the quasi-static limit, one easily obtains from the condition of current conservation that

$$\sigma ^2\delta \varphi =𝐣^{ext}.$$
(8)
The correlation function of extraneous currents

$$\delta j_\alpha ^{ext}(𝐫_1,t_1)\delta j_\beta ^{ext}(𝐫_2,t_2)=2\sigma \delta _{\alpha \beta }\delta (𝐫_1𝐫_2)\delta (t_1t_2)$$

$$\times d\epsilon f(\epsilon ,𝐫_1)[1f(\epsilon ,𝐫_1)]$$
(9)
is easily obtained from Eq. (5). Expressions (7) - (9) form a complete set of equations for calculating the second cumulant of current.

It is natural to use the same notion of independent scattering events for determining the correlation functions of Langevin sources of higher order. According to the ideas of Kogan and Shulman, the Langevin source is a fluctuation of the difference between the outgoing and incoming scattering fluxes into a given state $`(𝐩,𝐫)`$. Since each scattering flux between a pair of states is assumed to be a Poissonian process, all its cumulants are proportional to the average scattering rate $`1/\tau `$. Hence the third- and fourth-order correlation functions of extraneous currents (6) are proportional to $`\tau ^3`$ (see Appendix for details). As will be shown below, the contribution from these correlations is negligibly small as compared to another mechanism related with second-order correlations of Langevin sources. These correlations may be called indirect, or ”cascade”. The point is that the second-order correlation function of extraneous sources is a functional of the distribution function $`f`$ and hence may also fluctuate as the current itself. One may roughly imagine these fluctuations as fluctuations of Nyquist noise of a resistor caused by fluctuations of its temperature. A fluctuation $`\delta f`$ results in a fluctuation

$$\delta \delta j_\alpha ^{ext}(𝐫_1,t_1)\delta j_\beta ^{ext}(𝐫_2,t_2)=2\sigma \delta _{\alpha \beta }\delta (𝐫_1𝐫_2)\delta (t_1t_2)$$

$$\times d\epsilon [12f(\epsilon ,𝐫_1)]\delta f(\epsilon ,𝐫_1,t_1).$$

Note that the time scale for the fluctuation $`\delta f`$ is set by a characteristic relaxation time and hence they are slow as compared to the duration of a scattering event. As $`\delta f`$ is also correlated with fluctuations of other quantities, this ”noise of noise” results in higher-order correlations of currents. Hence even Gaussian extraneous sources may produce non-Gaussian fluctuations.

In a symbolic form, the expression for indirect third-order correlations may be written in a form

$$\delta I_1\delta I_2\delta I_3=P_{123}\left\{\frac{\delta \delta I_1\delta I_2}{\delta f_4}\delta f_4\delta I_3\right\},$$
(10)
where $`P_{123}`$ denotes a summation over all inequivalent permutations of indices $`(123)`$ and $`\delta \mathrm{}/\delta f_4`$ denotes a functional derivative with respect to $`f(\epsilon _4,𝐫_4,t_4)`$. The products imply a convolution over the arguments of the distribution functions with repeating indices. The irreducible fourth-order correlation function is presented by three groups of terms

$$:\delta I_1\delta I_2\delta I_3\delta I_4:=P_{1234}\{\frac{\delta ^2\delta I_1\delta I_2}{\delta f_5\delta f_6}\delta f_5\delta I_3\delta f_6\delta I_4$$

$$+\frac{\delta \delta I_1\delta I_2}{\delta f_5}\frac{\delta \delta f_5\delta I_3}{\delta f_6}\delta f_6\delta I_4$$

$$+\frac{\delta \delta I_1\delta I_2}{\delta f_5}\delta f_5\delta f_6\frac{\delta \delta I_3\delta I_4}{\delta f_6}\}.$$
(11)
The corresponding contributions are schematically illustrated by diagrams in Fig. 1.

To evaluate expressions (10) and (11), one must know the second-order correlation function of fluctuations $`\delta f`$. In the quasi-static limit, the Boltzmann - Langevin equation may be easily transformed into a stochastic diffusion equation for the fluctuation $`\delta f(\epsilon ,𝐫,t)`$

$$D^2\delta f(\epsilon ,𝐫)=\delta 𝐅^{ext},$$
(12)
where

$$\delta 𝐅^{ext}(\epsilon )=\frac{\tau }{N_F}\underset{𝐩}{}𝐯\delta J^{ext}(𝐩)\delta (\epsilon _𝐩\epsilon ),$$
(13)
so one obtains from (5) that

$$\delta F_\alpha ^{ext}(\epsilon ,𝐫)\delta F_\beta ^{ext}(\epsilon ^{},𝐫^{})=2\frac{D}{N_F}\delta (𝐫𝐫^{})\delta (tt^{})$$

$$\delta (\epsilon \epsilon ^{})\delta _{\alpha \beta }f(\epsilon )[1f(\epsilon )],$$
(14)
$$\delta F_\alpha ^{ext}(\epsilon ,𝐫)\delta j_\beta ^{ext}(𝐫^{})=2eD\delta (𝐫𝐫^{})\delta (tt^{})$$

$$\times \delta _{\alpha \beta }f(\epsilon )[1f(\epsilon )],$$
(15)
where $`D`$ is the diffusion coefficient and $`N_F`$ is the Fermi density of states.

Consider the case of a quasi-one-dimensional diffusive wire of length $`L`$ connecting two massive electrodes with a voltage drop $`V`$ across it. In this case, all quantities may be considered as depending only on the longitudinal coordinate $`x`$ along the wire. The solution of Eq. (12) is of the form

$$\delta f(x)=\frac{1}{DS_0}\underset{0}{\overset{L}{}}𝑑x^{}K(x,x^{})d^2r_{}\delta F_x^{ext}(\epsilon ,x,𝐫_{}),$$

$$K(x,x^{})=\theta (xx^{})x/L,$$
(16)
where $`S_0`$ is the area of the cross-section of the wire and $`𝐫_{}`$ are the transverse coordinates. Because the pile-up of charge in the contact is forbidden in the quasi-static limit, the fluctuation of current is independent of $`x`$ and is obtained by averaging the extraneous current over the contact volume

$$\delta I=\underset{0}{\overset{L}{}}\frac{dx}{L}d^2r_{}\delta j_x^{ext}.$$
(17)
The low-frequency Fourier transform of the correlation function of $`\delta I(t_1)`$ and $`\delta I(t_2)`$ is given by

$$\delta I(\omega _1)\delta I(\omega _2)=\delta (\omega _1+\omega _2)$$

$$\times \frac{4\pi }{RL}\underset{0}{\overset{L}{}}𝑑x𝑑\epsilon f(\epsilon ,x)[1f(\epsilon ,x)],$$
(18)
where $`R`$ is the resistance of the contact. By giving the distribution function a variance $`\delta f(\epsilon ,x)`$, one easily obtains the functional derivative of Eq. (18) with respect to $`f(\epsilon ,x,\omega _3)`$ in the form

$$\frac{\delta \delta I(\omega _1)\delta I(\omega _2)}{\delta f(\epsilon ,x,\omega _3)}=\delta (\omega _1+\omega _2\omega _3)\frac{4\pi }{RL}[12f(\epsilon ,x)].$$
(19)
The second functional derivative of the same quantity is just

$$\frac{\delta ^2\delta I(\omega _1)\delta I(\omega _2)}{\delta f(\epsilon _3,x_3,\omega _3)\delta f(\epsilon _4,x_4,\omega _4)}=\delta (\omega _1+\omega _2\omega _3\omega _4)$$

$$\times \delta (\epsilon _3\epsilon _4)\delta (x_3x_4)\frac{8\pi }{RL}.$$
(20)
The right-hand side of Eq. (10) allows three inequivalent permutations of indices. Hence the low-frequency Fourier transform of the third cumulant of current

$$S_3(\omega _1,\omega _2)=d(t_1t_3)d(t_2t_3)$$

$$\times \mathrm{exp}[i\omega _1(t_1t_3)+i\omega _2(t_2t_3)]\delta I(t_1)\delta I(t_2)\delta I(t_3)$$

is given by an expression

$$S_3(0,0)=12\frac{e}{RL^2}𝑑\epsilon 𝑑x𝑑x^{}[12f(\epsilon ,x)]K(x,x^{})$$

$$\times f(\epsilon ,x^{})[1f(\epsilon ,x^{})].$$
(21)
The first, second, and the third terms in the right-hand side of Eq. (11) allow 6, 12, and 3 inequivalent permutations of indices, respectively. Hence the low-frequency Fourier transform of fourth cumulant of current

$$S_4(\omega _1,\omega _2,\omega _3)=d(t_1t_4)d(t_2t_4)d(t_3t_4)$$

$$\times \mathrm{exp}[i\omega _1(t_1t_4)+i\omega _2(t_2t_4)+i\omega _3(t_3t_4)]$$

$$\times :\delta I(t_1)\delta I(t_2)\delta I(t_3)\delta I(t_4):$$

may be written in a form

$$S_4(0,0,0)=6S_{41}+12S_{42}+3S_{43},$$
(22)
where

$$S_{41}=16\frac{e^2}{RL^3}𝑑\epsilon \underset{0}{\overset{L}{}}𝑑x\underset{0}{\overset{L}{}}𝑑x_1K(x,x_1)$$

$$\times f(\epsilon ,x_1)[1f(\epsilon ,x_1)]$$

$$\times \underset{0}{\overset{L}{}}dx_2K(x,x_2)f(\epsilon ,x_2)[1f(\epsilon ,x_2)],$$
(23)
$$S_{42}=8\frac{e^2}{RL^3}𝑑\epsilon \underset{0}{\overset{L}{}}𝑑x[12f(\epsilon ,x)]$$

$$\times \underset{0}{\overset{L}{}}dx_1K(x,x_1)[12f(\epsilon ,x_1)]$$

$$\times \underset{0}{\overset{L}{}}dx_2K(x,x_2)f(\epsilon ,x_2)[1f(\epsilon ,x_2)],$$
(24)
and

$$S_{43}=8\frac{e^2}{RL^3}𝑑\epsilon \underset{0}{\overset{L}{}}𝑑x_1[12f(\epsilon ,x_1)]$$

$$\times \underset{0}{\overset{L}{}}dx_2[12f(\epsilon ,x_2)]$$

$$\times \underset{0}{\overset{L}{}}dxK(x_1,x)K(x_2,x)f(\epsilon ,x)[1f(\epsilon ,x)].$$
(25)
The distribution function inside the contact is given by an expression

$$f(\epsilon ,x)=\left(1\frac{x}{L}\right)f_0(\epsilon +eV/2)+\frac{x}{L}f_0(\epsilon eV/2),$$
(26)
where $`f_0(\epsilon )`$ is the Fermi distribution function. The integration in Eqs. (21) - (25) is easily performed. One obtains that the third cumulant is equal

$$S_3=\frac{1}{15}\frac{e}{R}\frac{eV\mathrm{cosh}(eV/T)+12T\mathrm{sinh}(eV/T)13eV}{\mathrm{cosh}(eV/T)1}.$$
(27)
This is essentially the same expression that was obtained by Gutman and Gefen using the nonlinear $`\sigma `$-model. It gives

$$S_3=\frac{1}{15}\frac{e^2V}{R}$$
(28)
at high voltages in agreement with Lee et al. and

$$S_3=\frac{1}{3}\frac{e^2V}{R}$$
(29)
in the low-voltage or high-temperature limit.

The fourth cumulant of current is given by an expression

$$S_4=\frac{1}{420}\frac{e^2}{R}\frac{1}{\mathrm{sinh}^3(eV/2T)}[eV\mathrm{cosh}\left(\frac{3eV}{2T}\right)$$

$$20T\mathrm{sinh}\left(\frac{3eV}{2T}\right)313eV\mathrm{cosh}\left(\frac{eV}{2T}\right)$$

$$+684T\mathrm{sinh}\left(\frac{eV}{2T}\right)].$$
(30)
It gives

$$S_4=\frac{1}{105}\frac{e^3V}{R}$$
(31)
in the high-voltage limit in agreement with the results of Lee et al.. In equilibrium at $`V=0`$ only the last term in Eq. (22) is nonzero and

$$S_4=\frac{2}{3}\frac{e^2T}{R}$$
(32)
This result seems to be new. The positive sign of $`S_4`$ in equilibrium is in a qualitative agreement with the shape of distribution function of current numerically obtained by Belzig and Nazarov. The behavior of $`S_4(V)`$ is shown in Fig. 2. The fourth cumulant changes its sign at $`eV20T`$, hence the distribution of current changes from super-Gaussian to sub-Gaussian as the voltage increases.

It has been proposed recently that the third cumulant of noise may be used for determining the effective charge of quasiparticles. In other words, it may give the same information as the shot noise even at low voltages $`eVT`$. Since the fourth cumulant is nonzero even at zero voltage, one may obtain a nontrivial information about the system from measurements of equilibrium fluctuations. Measurements of fluctuations of noise power, which are termed ”the second spectral density” and are closely related with the Fourier transform of the fourth cumulant,  were successfully implemented by a number of authors who studied the $`1/f`$ noise.

In summary, we have shown that higher cumulants of current in diffusive-metal contacts may be described by the semiclassical Boltzmann - Langevin theory. The semiclassical fluctuations appear to be non-Gaussian both in equilibrium and at high voltages. The present approach may be also applied to semiclassical non-diffusive systems. In this case, one has to take into account also higher-order local correlators of extraneous sources.

The author acknowledges a helpful discussion with Sh. M. Kogan. This work was supported by Russian Foundation for Basic Research, grant 01-02-17220, and by an INTAS Open grant, and by an INTAS Open grant 2001-1B-14.

APPENDIX

The third central moment of $`\delta J^{ext}`$ is easily found from the same considerations as the second moment. Much like the second-order correlator, it is local in space. As the collision integral involves only single-particle transitions between pairs of states, the triple correlator $`\delta J^{ext}(𝐩_1)\delta J^{ext}(𝐩_2)\delta J^{ext}(𝐩_3)`$ is nonzero only if at least two of these states coincide. We also make use of the fact that the third-order correlator of a scattering flux from one state to another, which is assumed to be Poissonian, is proportional to the average scattering rate between these states. The sign of the contribution from each scattering process should be determined by multiplying the signs of occupancy changes in states $`𝐩_1`$, $`𝐩_2`$, and $`𝐩_3`$ when the corresponding scattering event takes place. Hence the correlator may be written in a form

$$\delta J^{ext}(𝐩_1,𝐫_1,t_1)\delta J^{ext}(𝐩_2,𝐫_2,t_2)\delta J^{ext}(𝐩_3,𝐫_3,t_3)$$

$$=\delta (𝐫_1𝐫_2)\delta (𝐫_2𝐫_3)\delta (t_1t_2)\delta (t_2t_3)$$

$$\times \{\delta _{𝐩_1𝐩_2}\delta _{𝐩_2𝐩_3}\underset{𝐩^{}}{}[J(𝐩^{}𝐩_1)J(𝐩_1𝐩^{})]$$

$$+\delta _{𝐩_1𝐩_2}\left[J(𝐩_1𝐩_3)J(𝐩_3𝐩_1)\right]$$

$$+\delta _{𝐩_2𝐩_3}\left[J(𝐩_2𝐩_1)J(𝐩_1𝐩_2)\right]$$

$$+\delta _{𝐩_1𝐩_3}[J(𝐩_1𝐩_2)J(𝐩_2𝐩_1)]\},$$
$`(A1)`$
where the scattering fluxes $`J`$ are given by Eq. (4). It is easily verified that this correlator conserves the total number of electrons at a given point.

Consider now the fourth-order irreducible correlator of extraneous sources. The term ”irreducible” means that only the part of the correlator that cannot be decoupled into products of second-order correlators is considered. This correlator is zero for a Gaussian noise but is proportional to the average rate for a Poissonian process. Using the same ideas, the irreducible correlator may be written in a form

$$:\delta J^{ext}(𝐩_1,𝐫_1,t_1)\delta J^{ext}(𝐩_2,𝐫_2,t_2)\delta J^{ext}(𝐩_3,𝐫_3,t_3)\delta J^{ext}(𝐩_4,𝐫_4,t_4):=$$

$$\delta (𝐫_1𝐫_2)\delta (𝐫_2𝐫_3)\delta (𝐫_3𝐫_4)\delta (t_1t_2)\delta (t_2t_3)\delta (t_3t_4)$$

$$\times \{\delta _{𝐩_1𝐩_2}\delta _{𝐩_2𝐩_3}\delta _{𝐩_3𝐩_4}\underset{𝐩^{}}{}[J(𝐩^{}𝐩_1)+J(𝐩_1𝐩^{})]\delta _{𝐩_1𝐩_2}\delta _{𝐩_2𝐩_3}[J(𝐩_1𝐩_4)+J(𝐩_4𝐩_1)]$$

$$\delta _{𝐩_1𝐩_2}\delta _{𝐩_2𝐩_4}\left[J(𝐩_1𝐩_3)+J(𝐩_3𝐩_1)\right](\delta _{𝐩_1𝐩_3}\delta _{𝐩_3𝐩_4}+\delta _{𝐩_2𝐩_3}\delta _{𝐩_3𝐩_4})\left[J(𝐩_1𝐩_2)+J(𝐩_2𝐩_1)\right]$$

$$+\delta _{𝐩_1𝐩_2}\delta _{𝐩_3𝐩_4}\left[J(𝐩_1𝐩_3)+J(𝐩_3𝐩_1)\right]$$

$$+(\delta _{𝐩_1𝐩_3}\delta _{𝐩_2𝐩_4}+\delta _{𝐩_1𝐩_4}\delta _{𝐩_2𝐩_3})[J(𝐩_1𝐩_2)+J(𝐩_2𝐩_1)]\}.$$
$`(A2)`$
In the diffusive limit, it is convenient to pass from extraneous fluxes in the Boltzmann - Langevin equation to extraneous currents in the drift-diffusion equation by means of Eq. (6). The third-order correlator of extraneous currents is of the form

$$\delta j_\alpha ^{ext}(𝐫_1,t_1)\delta j_\beta ^{ext}(𝐫_2,t_2)\delta j_\gamma ^{ext}(𝐫_3,t_3)$$

$$=\delta (𝐫_1𝐫_2)\delta (𝐫_2𝐫_3)\delta (t_1t_2)\delta (t_2t_3)$$

$$\times \tau ^3e^3\underset{\mathrm{𝐩𝐩}^{}}{}(v_\alpha v_\beta v_\gamma v_\alpha ^{}v_\beta v_\gamma v_\alpha v_\beta ^{}v_\gamma v_\alpha v_\beta v_\gamma ^{})$$

$$\times [J(𝐩^{}𝐩)J(𝐩𝐩^{})].$$
$`(A3)`$
Though the scattering fluxes $`J`$ are proportional to $`1/\tau `$, the bracketed difference vanishes in equilibrium and is proportional to the anisotropic part of the distribution function in the case of applied bias. As this part is proportional to $`\tau `$ in the diffusive approximation, Eq. (A3) is at least of the order of $`\tau ^3`$.

The fourth-order irreducible correlator of extraneous currents is of the form

$$:\delta j_\alpha ^{ext}(𝐫_1,t_1)\delta j_\beta ^{ext}(𝐫_2,t_2)\delta j_\gamma ^{ext}(𝐫_3,t_3)\delta j_\delta ^{ext}(𝐫_4,t_4):$$

$$=\frac{16}{15}e^2l_{imp}^2\sigma \delta (𝐫_1𝐫_2)\delta (𝐫_2𝐫_3)\delta (𝐫_3𝐫_4)$$

$$\times \delta (t_1t_2)\delta (t_2t_3)\delta (t_3t_4)(\delta _{\alpha \beta }\delta _{\gamma \delta }+\delta _{\alpha \gamma }\delta _{\beta \delta }+\delta _{\alpha \delta }\delta _{\beta \gamma })$$

$$𝑑\epsilon f(\epsilon ,𝐫_1)[1f(\epsilon ,𝐫_1)],$$
$`(A4)`$
where $`\sigma `$ is the conductivity. Hence the fourth-order correlator is also of the order $`\tau ^3`$.


text:
# A catalogue of dust clouds in the Galaxy

## 1 Introduction

Dust clouds are fundamental to understand many issues in the Galaxy. Optical obscuration is an obstacle to the study of Galactic structure from the perspective of star clusters and H II Regions. However, dust association to molecular gas, and velocity determinations (e.g. Blitz et al. bli (1982), Dame et al. dam (1987)) make them excellent tracers of related structures in the Galaxy. Since some clouds are actively forming stars, with protostellar objects and/or embedded clusters (e.g. Lawson et al. law (1996), Lada et al. lad2 (1996)), clouds are interesting targets to search for new IR clusters. Near infra-red (NIR) surveys such as the Two Micron All Sky Survey (2MASS – Skrutskie et al. skr (1997)) are opening this possibility (e.g. Dutra & Bica 2000a ).

Much information on dust clouds remains strewn throughout many catalogues, and subsequent studies often refer to a particular designation. A unified catalogue would be useful for searches of new clouds, especially for surveys in wavelengths other than optical. Similar to catalogue efforts in other fields, such as those dealing with galaxies, open clusters or globular clusters, the present study aims at providing a step forward to an overall catalogue of dust clouds. In Sect. 2 input catalogues are gathered. In Sect. 3 merging and cross-identification procedures are given, and results are presented. In Sect. 4 some catalogue properties and prospective work are discussed.

## 2 Input catalogues

Input catalogues dealing mostly with low-latitude clouds ($`|b|`$ $`<`$ 25), their acronyms and number of entries (prior to cross-identifications) are given in Table 1. Barnard (bar (1919), bar2 (1927)) first catalogued clouds in the northern and equatorial zones. Lynds (lyn (1962)) built the largest set of dark clouds (LDN) north of $`\delta `$ = -33 using the Palomar Sky Survey (PSS), including some high-latitude clouds. Sandqvist and Lindroos (san (1976)) detected clouds in the PSS for -33$`{}_{}{}^{}<\delta <`$ -46. Sandqvist (san2 (1977)) found clouds south of $`\delta `$ = -42.5 using the ESO (B) Atlas. Bernes (ber (1977)) looked for bright nebulae mainly related to LDN’s, and reported some new dust clouds. Zealey et al. (zea (1983)) compiled cometary globules – as a rule ’bright dark’ nebulae with reflection and absorption components. Feitzinger & Stüwe (fei (1984)) inspected ESO/SERC plates and provided two catalogues: (i) extended clouds, and (ii) globules ($``$ 6 or less). Hartley et al. (har (1986)) presented the largest southern set of clouds from a search on ESO/SERC J plates for $`\delta `$ $``$ -35 .

Some Table 1 catalogues deal with dense cloud cores and isolated small clouds. Myers et al. (mye (1983)) identified small clouds using the PSS for low-mass star formation studies by means of CO. Clemens & Barvainis (cle (1988)) used the PSS for small cloud searches and studied their optical, IR and millimeter properties. Vilas-Boas et al. (vil (1994)) investigated small clouds from ESO/SERC J plates, extinction maps and previous studies, located in nearby clouds or complexes such as Coalsack and Vela. Bourke et al. (bou (1995)) analysed clouds with opacity class A from Hartley et al., two of them new. Dense clouds can harbour embedded cores of Young Stellar Objects (YSO) or Pre-Main-Sequence (PMS) stars. Parker (par (1988)) provided accurate positions for 147 Lynds clouds with opacity class 6. Lee & Myers (lee (1999)) listed the largest set of dense cores, with opacity classes 5 and 6 from Lynds and A from Hartley et al. Parker (par (1988)) and Lee & Myers (lee (1999)) studied the relation of dense cores to IRAS sources, and in turn to YSO and PMS. Finally, Vilas-Boas et al. (vil2 (2000)) studied cores in Lupus, Corona Australis, Scorpius and Vela.

The input data were complemented with objects from individual studies or small lists: (i) 21 nearby clouds and complexes (Cambrésy cam (1999)) with extinction maps from star counts; (ii) 23 nearby clouds and complexes as studied in CO (Dame et al. dam (1987)); (iii) molecular clouds from individual studies such as TMC-1 and TMC-2 (Churchwell et al. chu (1978)), OMC-1 (Ziurys et al. ziu (1981)), OMC-2 and OMC-3 (Chini et al. chi (1997)), Heiles 2 (Heiles hei (1968)) and MT 1 (Maddalena & Thaddeus mad (1985)); (iv) 2 cometary globules – CG – and 7 Gum Nebula Dark Clouds –GDC (Reipurth rei (1983)); and finally, (v) a pre-cometary globule (Lefloch & Lazareff lef (1995)). The total number of entries from catalogues and lists preferentially including low-latitude clouds is 5654.

The acronyms and number of entries of the input catalogues dealing mostly with high-latitude clouds are given in Table 2. Most of them deal with CO studies, but searches based on far infra-red (FIR) dust emission atlases such as IRAS provided most entries. High-latitude clouds present low visual extinction (translucent – van Dishoeck et al. van (1991)) and are therefore difficult to be detected on photographic surveys. Magnani et al. (mag (1985)) and Keto & Myers (ket (1986)) studied high-latitude clouds in CO (the latter study includes some lower-latitude clouds). Magnani et al. (mag2 (1996)) compiled list of clouds taken from the literature, providing properties and references for clouds with the acronyms UT , ir, HSVMT, G, Stark and 3C. The acronym HRK stands for clouds in regions studied in HI, CO and IR (Heiles et al. hei3 (1988)). FIR emission excess with respect to H I indicates cold clouds where hydrogen appears in molecular form (de Vries et al. vri (1987)). Désert et al. (des (1988)) used the IRAS 100 $`\mu `$m data coupled to the Berkeley H I survey (Heiles & Habing hei2 (1974)) to detect 516 infrared excess clouds (IREC) for $`|b|`$ $`>`$ 5. Reach et al. (rea (1998)) used DIRBE/COBE in conjunction with the Leiden-Dwingeloo H I survey (Hartmann & Burton han (1997)) to create higher resolution maps. From the IR excesses they retrieved 60 previous clouds and found 81 new ones (DIR – Diffuse Infrared Clouds). Also included were 2 new clouds studied in CO by Hartmann et al. (vri (1987)), and the absorption component of the Draco Nebula (Goerigk et al. goe (1983)).

## 3 Catalogue construction and contents

The procedures for catalogue construction and cross-identifications follow those outlined for the LMC and SMC extended objects (Bica & Schmitt bic (1995), Bica et al. bic1 (1999)). Available electronic catalogues were retrieved from CDS and remaining ones were typed. The original coordinates (usually either B1950.0 $`\alpha ,\delta `$ or in $`l,b`$) were transformed to J2000.0 $`\alpha ,\delta `$ and to homogeneous $`l,b`$ values. All catalogues were merged into one file and sorted by $`l`$. Equivalent objects were merged into a single line considering positions and angular dimensions. This was complemented with available properties such as optical opacity class. Previous cross-identifications were examined. Revisions occurred and many new equivalences were found. Doubts on optical clouds were inspected on Digitized Sky Survey (DSS and XDSS) images and/or sky charts generated by means of the Guide Star Catalogue. Recent catalogues dealing with small nebulae (Sect. 2) and that by Hartley et al. (har (1986)) produced accurate coordinates, which is not always the case of early works.

Studies in Sect. 2 and Hilton & Lahullas (hil (1995)) provided distances from several methods (e.g. related stars or OB complexes, background and foreground stars, kinematical). Studies in Sect.2 and Otrupcek et al.s (otr (2000)) provided LSR CO (in a few cases H I) velocities. Velocity and distance estimates were additional contraints for the definition of clouds and their physically related groups.

Opacity classes were reduced to Lynds’ (lyn (1962)) scale. Internal variations in some clouds were averaged. For detailed values we refer to the original studies. Optical opacity class has been a useful parameter for cloud classifications and selections. We provide FIR contrast parameters for similar purposes. Schlegel et al. (sch (1998)) built an all-sky reddening $`(E(BV))_{FIR}`$ map based on 100 $`\mu `$m dust thermal emission with resolution of $``$ 6, and temperature corrections based on lower resolution DIRBE maps. We extracted the reddening central value in the direction of each cloud and 4 background surrounding positions distant 1.3$`\times `$ the cloud’s major axis dimension for those larger than 10. For smaller clouds the background distance was 2$`\times `$ the major axis dimension. We computed the background average value, its fluctuation, and 2 contrast parameters. $`\mathrm{\Delta }`$ is defined as the difference between centre and background values, and $`\rho `$ as the ratio of these quantities. Note that $`\mathrm{\Delta }`$ can present negative and $`\rho `$ $`<`$ 1 values, since background contributions can be substantial, especially as one approaches the Plane (Dutra & Bica 2000b ). Neighbouring clouds, position uncertainties, irregular shapes and extensions can also disturb. Although clouds are concentrated to the Plane $``$ 3750 clouds present positive FIR contrast ($`\mathrm{\Delta }`$ $`>0`$ and $`\rho `$ $`>`$ 1). Selections for a variety of studies can be obtained from such parameters, from candidates to line-of-sight near projections to isolated dense clouds. As cautionary remark, the present discrete cloud FIR values and parameters should not be taken as true dust column densities and their combinations, especially for small clouds owing to the low resolution of the temperature maps, coupled to other limitations.

Some newly identified clouds are included: (i) Magnani et al. (mag3 (2000)) detected CO along 133 directions for $`b`$ $`<`$ -30, 58 were new detections and 75 were related to 26 previous clouds. We compared Reach et al.’s (rea (1998)) FIR maps with CO detections by Magnani et al. (mag3 (2000)). As a result we found evidence of 16 new clouds indicated by the acronym CODIR (one additional cloud turned out to be IREC 267); (ii) We were not particularly searching for new clouds in the present study, but during the cross-identification process and inspections of optical images and FIR maps we found 15 uncatalogued clouds (DBDN). They are 2 low-latitude globules, 10 high-latitude and 3 transition zone extended clouds. (iii) The dust clouds recently reported by Dutra & Bica (dut4 (2001)) using the 2MASS Atlas. These 5 clouds (DBIRDN) are opaque in the $`K_s`$ band and are projected onto the central bulge. Some of them are probably giant molecular clouds near the Centre.

From $``$ 6500 input entries, cross-identifications led to 5004 clouds and complexes in the unified catalogue, which will be available in electronic form at CDS (Strasbourg) via anonymous ftp to cdsarc.u-strasbg.fr (130.79.128.5). Each entry occupies 2 catalogue lines. The first line shows by columns: (1) and (2) Galactic coordinates, (3) and (4) J2000.0 $`\alpha ,\delta `$, (5) and (6) major and minor axes dimensions in arc minutes, (7) optical opacity class, (8) designation(s). In line 2 columns (1) to (5) list FIR central reddening, background reddening, fluctuation and contrast parameters $`\mathrm{\Delta }`$ and $`\rho `$. Subsequent fields are distances in kpc preceded by ‘d=’, and CO or H I LSR velocities preceded by ‘vCO=’ or ‘vHI=’, respectively. Finally, comments occupy the last part of line 2: (i) further designations (preceded by ’&’) with respect to column (8) of line 1; (ii) hyerarchical relations among dark and/or bright nebulae (e.g. LBN for Lynds lyn2 (1963) and Sh2- for Sharpless sha (1959)), as indicated by in (within), inc (includes) or rel (related). Note that dust cloud designations are not mixed to those of bright clouds, since such possible relations are given only in line 2. Concerning IREC clouds we include the remarks by Désert et al. (des (1988)) on those disturbed by bad IR or HI pixels. Dust cloud acronyms in the catalogue other than those indicated in the present references, are taken from the references themselves.

## 4 Some catalogue properties and prospective work

Fig. 1 shows $`l`$ and $`b`$ histograms for the resulting 5004 dust clouds. The $`l`$ histogram presents a minimum towards the Anticentre and maximum in the Galactic Centre direction. In the $`b`$ histogram the clouds are strongly concentrated to the Plane, 89 % located in the low-latitude zone. In the high-latitude zone there occur 525 clouds. A few clouds populate the Polar Caps. The present sample of high-latitude clouds is a factor $``$ 2 larger than that recently compiled by Bhatt (2000) in a study of possible connection of part of them to the Per OB3/CasTau and Sco OB2 associations.

Angular size histograms are shown in Fig. 2 in terms of cloud major axis dimension. Each histogram is limited to 250, but some clouds and complexes exceed 1000. For the total sample (Panel a) the distribution is exponential, dominated by globules and cloud cores. For the high-latitude sample (Panel b) the distribution is $``$ gaussian, and the peak occurs for clouds of size 80’-90’.

The present effort to merge and cross-identify dust cloud catalogues allows one to conclude that $``$ 1500 have a previously reported equivalent object. Chronology (Tables 1 and 2) and usage help decide which acronym(s) to adopt. Just to mention a few examples: (i) Barnard’s early catalogue has some clouds overlapping with those of large southern catalogues, e.g. B 232, FeSt1-252 and HMSTG 343.7+4.0 are equivalent objects; (ii) the northern/equatorial and southern largest catalogues have an overlapping zone, e.g the small cloud LDN 1701 = HMSTG 354.0+3.5 = Sc16, the latter designation is from Vilas-Boas et al. (vil2 (2000)); (iii) the small dust cloud in the Gum Nebula GDC 6 has counterparts in HMSTG 267.6-6.4 and BHR 40, but its neighbour GDC 3 remains to date with a single designation; (iv) at high latitudes MBM 2 = IREC 155 originate from 2 different methods (CO and IR/H I excess); (v) IREC and DIR clouds have many equivalences, e.g. IREC 7 = DIR 009-30; (vi) catalogues typical of high and low latitude zones have clouds in common, e.g. LDN 317 = IREC 10, and FeSt1-223 = IREC 445. The catalogue is not intended to be complete, but it includes all cross-identified acronyms, and provides a tool to converge information. Doubt on any cross-identification or parameter can be analysed by accessing the original catalogues.

Finally, we address prospective work. A promising approach is the identification of dust clouds in the $`K_s`$ band with 2MASS (Dutra & Bica dut4 (2001)). The present catalogue is a tool to verify whether NIR clouds have an optical counterpart or not. Recently, 2MASS reported in http://www.ipac.caltech.edu/2mass/gallery/fest1-457atlas.jpg a 3-band image and description of a cloud identified as FeSt1-457 (Feitzinger & Stüwe fei (1984)). This was a near-position match. A detailed cross-identification with all available information shows that one is dealing with 2 different objects. The 2MASS object (included as 2MASS-DN1.7+3.6 in the present catalogue) has a small angular size ($`4^{}\times 3^{}`$) with no optical counterpart on DSS or XDSS images, while FeSt1-457 is a large cloud ($`70^{}`$) with medium optical opacity (class 4). If both clouds are nearby, that in 2MASS may be a related globule, but it may turn out to be a more distant object. This application shows the importance of a unified catalogue for searches of new clouds.

###### Acknowledgements.

We are indebted to Prof. Harm Habing and an anonymous referee for interesting suggestions and remarks. We made use of electronic catalogues from CDS (Simbad and VizieR). We employed the Guide Star Catalog and Digitized Sky Survey images (DSS and XDSS), both produced at the Space Telescope Science Institute under U.S. Government grants NAS5-26555 and NAG W-2166. The Canadian Astronomy Data Centre (CADC) interface was used for DSS and XDSS extractions. We acknowledge support from the Brazilian institution CNPq. CD acknowledges FAPESP for a post-doc fellowship (proc. 00/11864-6).