# Out-of-equilibrium Kondo effect in Double Quantum Dots

## Abstract

The out-of-equilibrium transport properties of a double quantum dot system in the Kondo regime are studied theoretically by means of a two-impurity Anderson hamiltonian with interimpurity hopping. The hamiltonian is solved by means of a non-equilibrium generalization of the slave-boson mean-field theory. It is demonstrated that measurements of the differential conductance $`dI/dV`$, for the appropriate values of voltages and tunneling couplings, can give a direct observation of the coherent superposition between the many-body Kondo states of each dot. For large voltages and arbitrarily large interdot tunneling, there is a critical voltage above which the physical behaviour of the system again resembles that of two decoupled quantum dots.

Recent experiments  have shown that new physics emerge when the transport properties of quantum dots (QD’s) at temperatures (T) below the Kondo temperature ($`T_K`$) are studied. QD’s offer the intriguing possibility of a continuous tuning of the relevant parameters governing the Kondo effect  as well as the possibility of studying Kondo physics when the system is driven out of equilibrium in different ways. These experimental breakthroughs have opened up a new way for the study of strongly correlated electrons in artificial systems. The Kondo anomaly appearing in the density of states (DOS) of the QD reflects the formation of a quantum-coherent many-body state. Motivated by the recent experimental advances in the study of double quantum dots (DQD)  it is thus interesting to study what happens when two QD’s in the Kondo regime are coupled. Previous theoretical studies of this problem at equilibrium have focused on the competition between Kondo effect and antiferromagnetic coupling generated via superexchange  or via capacitive coupling between dots.   
In this Letter we focus on the study of a DQD in the Kondo regime driven out of equilibrium by means of a DC voltage bias. There have hitherto been only few attemps to study this problem  but a clear picture of the problem is yet missing. Following the recent work of Aono et al  and Georges and Meir  we employ the slave boson (SB) technique  in a mean field approximation (MFA) and generalize it to a non-equilibrium situation. This MFA allows us to include nonperturbatively the interdot tunneling term (i.e coherence between dots). The different physical regimes that appear as the ratio $`\tau _c=t_C/\mathrm{\Gamma }`$ changes ($`t_C`$ is the interdot tunneling coupling and $`\mathrm{\Gamma }`$ is the single particle broadening coming from the coupling to leads) can be explored by measuring the non-linear transport properties of the system. Our results can be summarized in Figs. 1 and 2: the differential conductance dI/dV of the DQD directly measures the transition (as $`\tau _c`$ increases) from two isolated Kondo impurities to a coherent superposition of the many-body Kondo states of each dot, which form bonding and anti-bonding combinations. This coherent state which occurs for $`\tau _c>1`$ is reflected as a splitting of the zero-bias anomaly in the dI/dV curves. This splitting depends non-trivially on the voltage and on the many-body parameters of the problem. For large voltages, we find that there is a critical voltage above which the coherent configuration is unstable and the physical behaviour of the system again resembles that of two decoupled QD’s, i.e two Kondo singularities pinned at each chemical potential, even for $`\tau _c>1`$. This instability is reflected as a drastic drop of the current leading to singular regions of negative differential conductance (NDC).   
Model: In typical experiments, $`U_{\mathrm{intradot}},\mathrm{\Delta }ϵ>>T`$ ($`U_{\mathrm{intradot}}`$ is the strong on-site Coulomb interaction on each dot, $`\mathrm{\Delta }ϵ`$ is the average level separation), which allows one to consider a single state in each QD. We can model the DQD with a (N=2) fold degenerate two-impurity Anderson hamiltonian with an extra term accounting for interdot tunneling. Each impurity is coupled to a diferent Fermi sea of chemical potential $`\mu _L`$ and $`\mu _R`$, respectively. In the limit $`U_{\mathrm{intradot}}\mathrm{}`$ (on each QD) and $`U_{\mathrm{interdot}}0`$ , the hamiltonian may be written in terms of auxiliary SB operators  plus constraints:

$`H`$ $`=`$ $`{\displaystyle \underset{k_{\alpha \{L,R\}},\sigma }{}}ϵ_{k_\alpha }c_{k_\alpha ,\sigma }^{}c_{k_\alpha ,\sigma }+{\displaystyle \underset{\alpha \{L,R\},\sigma }{}}ϵ_{\alpha \sigma }f_{\alpha \sigma }^{}f_{\alpha \sigma }`$ (1)   
$`+`$ $`{\displaystyle \frac{t_C}{N}}{\displaystyle \underset{\sigma }{}}(f_{L\sigma }^{}b_Lb_R^{}f_{R\sigma }+f_{R\sigma }^{}b_Rb_L^{}f_{L\sigma })`$ (2)   
$`+`$ $`{\displaystyle \frac{1}{\sqrt{N}}}{\displaystyle \underset{k_{\alpha \{L,R\}},\sigma }{}}V_\alpha (c_{k_\alpha ,\sigma }^{}b_\alpha ^{}f_{\alpha \sigma }+f_{\alpha \sigma }^{}b_\alpha c_{k_\alpha ,\sigma })`$ (3)   
$`+`$ $`{\displaystyle \underset{\alpha \{L,R\}}{}}\lambda _\alpha ({\displaystyle \underset{\sigma }{}}f_{\alpha \sigma }^{}f_{\alpha \sigma }+b_\alpha ^{}b_\alpha 1).`$ (4)   
$`c_{k_\alpha ,\sigma }^{}(c_{k_\alpha ,\sigma })`$ are the creation (annihilation) operators for electrons in the lead $`\alpha `$. To simplify the notation we consider henceforth that $`V_L=V_R=V_0`$ and $`ϵ_{L\sigma }=ϵ_{R\sigma }=ϵ_0`$ (i.e, $`T_K`$ is the same for both dots at equilibrium. The generalization to different $`T_K`$’s is straightforward). The even-odd symmetry is broken by the interdot coupling $`t_C`$. In the SB representation, the annihilation operator for electrons in the QD’s, $`c_{\alpha \sigma }`$ is decomposed into the SB operator $`b_\alpha ^{}`$ which creates an empty state and a pseudo fermion operator $`f_{\alpha \sigma }`$ which annihilates the singly occupied state with spin $`\sigma `$ in the dot $`\alpha `$: $`c_{\alpha \sigma }b_\alpha ^{}f_{\alpha \sigma }`$ ($`c_{\alpha \sigma }^{}f_{\alpha \sigma }^{}b_\alpha `$). In the last term of (1), the charge operator $`\widehat{Q}_\alpha =_\sigma f_{\alpha \sigma }^{}f_{\alpha \sigma }+b_\alpha ^{}b_\alpha `$ has been introduced. This term represents the constraint $`\widehat{Q}_\alpha =1`$ in each dot with Lagrange multiplier $`\lambda _\alpha `$. This constraint prevents double occupancy in the limit $`U\mathrm{}`$.   
Solution: In the lowest order, we assume that the SB operator is a constant c-number $`b_\alpha (t)/\sqrt{N}=b_\alpha (t)/\sqrt{N}=\stackrel{~}{b}_\alpha `$ neglecting the fluctuations around the average $`b_\alpha (t)`$ of the SB. At T=0, this MFA is correct for describing spin fluctuations (Kondo regime). Mixed-Valence behavior (characterized by strong charge fluctuations) cannot be described by the MFA. This restricts our non-equilibrium calculation to low voltages $`V<<ϵ_0`$. Charge fluctuations can be included as thermal or quantum fluctuations ($`1/N`$ corrections).  Defining $`\stackrel{~}{V}_\alpha =V_0\stackrel{~}{b}_\alpha `$ and $`\stackrel{~}{t}_C=t_C\stackrel{~}{b}_L\stackrel{~}{b}_R`$ we obtain from the constraints and the equation of motion of the SB operators the selfconsistent set of four equations with four unknowns ($`\stackrel{~}{b}_L,\stackrel{~}{b}_R,\lambda _L,\lambda _R`$):

$`\stackrel{~}{b}_{L(R)}^2+{\displaystyle \frac{1}{N}}{\displaystyle \underset{\sigma }{}}f_{L(R)\sigma }^{}f_{L(R)\sigma }={\displaystyle \frac{1}{N}}`$ (5)   
$`{\displaystyle \frac{\stackrel{~}{V}_{L(R)}}{N}}{\displaystyle \underset{k_{L(R)},\sigma }{}}c_{k_{L(R)},\sigma }^{}f_{L(R)\sigma }`$ (6)   
$`+{\displaystyle \frac{\stackrel{~}{t}_C}{N}}{\displaystyle \underset{\sigma }{}}f_{R(L)\sigma }^{}f_{L(R)\sigma }+\lambda _{L(R)}\stackrel{~}{b}_{L(R)}^2=0`$ (7)   
In order to solve (2) we need to calculate the non-equilibrium distribution functions: $`G_{\alpha \sigma ,k_\alpha ^{^{}}\sigma }^<(tt^{})ic_{k_\alpha ^{^{}}\sigma }^{}(t^{})f_{\alpha \sigma }(t)`$ and $`G_{\alpha \sigma ,\alpha ^{^{}}\sigma }^<(tt^{})if_{\alpha ^{^{}}\sigma }^{}(t^{})f_{\alpha \sigma }(t)`$. They can be derived by applying the analytic continuation rules of Ref.  to the equation of motion of the time-ordered Green’s function along a complex contour (Keldysh, Kadanoff-Baym or a more general choice). This allows us to relate $`G_{\alpha \sigma ,k_\alpha ^{^{}}\sigma }^<(tt^{})`$ with $`G_{\alpha \sigma ,\alpha ^{^{}}\sigma }^<(tt^{})`$ and $`G_{\alpha \sigma ,\alpha ^{^{}}\sigma }^r(tt^{})i\theta (tt^{})\{f_{\alpha \sigma }(t),f_{\alpha ^{^{}}\sigma }^{}(t^{})\}`$ and close the set of equations (2) in Fourier space:

$`{\displaystyle \frac{\stackrel{~}{\mathrm{\Gamma }}_{L(R)}}{\mathrm{\Gamma }}}i{\displaystyle \frac{dϵ}{2\pi }G_{L,L(R,R)}^<(ϵ)}={\displaystyle \frac{1}{N}}`$ (8)   
$`{\displaystyle \frac{\stackrel{~}{\mathrm{\Gamma }}_{L(R)}}{\mathrm{\Gamma }}}(\stackrel{~}{ϵ}_{L(R)}ϵ_0)=i{\displaystyle \frac{dϵ}{2\pi }G_{L,L(R,R)}^<(ϵ)(ϵ\stackrel{~}{ϵ}_{L(R)})},`$ (9)   
with $`\stackrel{~}{ϵ}_\alpha =ϵ_0+\lambda _\alpha `$ and $`\stackrel{~}{\mathrm{\Gamma }}_\alpha =\stackrel{~}{b}_\alpha ^2\mathrm{\Gamma }`$. For $`t_C=0`$ , $`\stackrel{~}{ϵ}_\alpha `$ and $`\stackrel{~}{\mathrm{\Gamma }}_\alpha `$ give, respectively, the position and the width of the Kondo peaks in the dot $`\alpha `$ (at equilibrium, and in the Kondo regime, $`\sqrt{\stackrel{~}{ϵ}_\alpha ^2+\stackrel{~}{\mathrm{\Gamma }}_\alpha ^2}T_K^0=De^{\pi |ϵ_0|/\mathrm{\Gamma }}`$). The distribution functions in the QD’s are: $`G_{L,L(R,R)}^<(ϵ)=\frac{2i(\stackrel{~}{\mathrm{\Gamma }}_{L(R)}f_{L(R)}(ϵ)[(ϵ\stackrel{~}{ϵ}_{R(L)})^2+\stackrel{~}{\mathrm{\Gamma }}_{R(L)}^2]+\stackrel{~}{\mathrm{\Gamma }}_{R(L)}f_{R(L)}(ϵ)\stackrel{~}{t}_C^2)}{[(ϵ\stackrel{~}{ϵ}_L+i\stackrel{~}{\mathrm{\Gamma }}_L)(ϵ\stackrel{~}{ϵ}_R+i\stackrel{~}{\mathrm{\Gamma }}_R)\stackrel{~}{t}_C^2][(ϵ\stackrel{~}{ϵ}_Li\stackrel{~}{\mathrm{\Gamma }}_L)(ϵ\stackrel{~}{ϵ}_Ri\stackrel{~}{\mathrm{\Gamma }}_R)\stackrel{~}{t}_C^2]}`$. $`f_{L(R)}(ϵ)`$ is the Fermi-Dirac function in the left (right) lead. Note that the presence of $`\stackrel{~}{t}_C^2`$ in the denominators indicates that the interdot tunneling enters nonperturbatively in the calculations and, then, coherent effects between dots are fully included. Due to the interdot tunneling, the Kondo singularities of each dot at $`\stackrel{~}{ϵ}_L`$ and $`\stackrel{~}{ϵ}_R`$ combine into coherent superpositions at $`ϵ_\pm =\frac{1}{2}\{(\stackrel{~}{ϵ}_L+\stackrel{~}{ϵ}_R)\pm \sqrt{(\stackrel{~}{ϵ}_L\stackrel{~}{ϵ}_R)^2+4\stackrel{~}{t}_C^2}\}`$. Of course, at equilibrium $`\stackrel{~}{b}_L=\stackrel{~}{b}_R=\stackrel{~}{b}`$, $`\lambda _L=\lambda _R=\lambda `$, we recover the results of Refs.. Note that the formation of coherent superpositions of the Kondo singularity is not trivially related with its single-particle counterpart (formation of bonding and antibonding states at $`ϵ_0\pm t_C`$). Let’s focus for simplicity in the equilibrium case ($`\stackrel{~}{ϵ}_L=\stackrel{~}{ϵ}_R`$), the splitting is given by $`\delta ϵ_+ϵ_{}=2\stackrel{~}{t}_C`$ which is a many-body parameter (given by the strong renormalization of the interdot tunneling due to the Kondo effect). $`\delta `$ depends non-linearly on the single-particle splitting $`\delta _0=2t_C`$ (see Inset of Fig. 3a). In the Kondo limit, $`\{[(\stackrel{~}{ϵ}+\stackrel{~}{t}_C)^2+\stackrel{~}{\mathrm{\Gamma }}^2][(\stackrel{~}{ϵ}\stackrel{~}{t}_C)^2+\stackrel{~}{\mathrm{\Gamma }}^2]\}^{1/4}=T_K^0e^{\frac{\pi t_C}{\mathrm{\Gamma }}(\frac{\stackrel{~}{\mathrm{\Gamma }}}{\mathrm{\Gamma }}\frac{1}{2})}`$. From the solution of Eq. 3 we obtain the current $`I=\frac{2e}{\mathrm{}}Re\{_{k_L,\sigma }\stackrel{~}{V}_LG_{L\sigma ,k_L\sigma }^<(t,t)\}`$ and DOS in each QD: $`\rho _{L(R)}(ϵ)=\frac{1}{\pi }Im\{\frac{\stackrel{~}{b}_{L(R)}^2(ϵ\stackrel{~}{ϵ}_{R(L)}+i\stackrel{~}{\mathrm{\Gamma }}_{R(L)})}{[(ϵ\stackrel{~}{ϵ}_L+i\stackrel{~}{\mathrm{\Gamma }}_L)(ϵ\stackrel{~}{ϵ}_R+i\stackrel{~}{\mathrm{\Gamma }}_R)\stackrel{~}{t}_C^2]}\}`$.   
Results: We solve numerically (for T=0) the set of non-linear equations (3) for different voltages $`\mu _L=V/2`$ and $`\mu _R=V/2`$, $`ϵ_0=3.5,D=60`$ (Kondo regime with $`T_K^010^3`$) and different values for the rest of parameters (all energies in units of $`\mathrm{\Gamma }`$). Depending on the ratio $`\tau _c=t_C/\mathrm{\Gamma }`$ we find two different physical scenarios for $`\tau _c<1`$ and $`\tau _c1`$.

In Fig. 1 we plot the I-V curves (for clarity, we show only the $`V0`$ region) for $`\tau _c1`$. The two main features of these curves are: i) An increase of the linear conductance $`𝒢=dI/dV|_{V=0}`$ as $`\tau _c`$ increases; ii) a saturation, followed by a drop, of the current for large voltages. This drop sharpens as $`\tau _c1`$. These features are more pronounced in a plot of the dI/dV (inset of Fig. 1). As $`\tau _c`$ increases, the zero-bias anomaly (originating from the Kondo resonance in the DOS of the dots) becomes broader and broader until it saturates into a flat region of value $`2e^2/h`$ (unitary limit) for $`\tau _c=1`$. The reduction of the current at larger V is reflected as NDC regions in the dI/dV curves. For $`\tau _c=1`$ this NDC becomes singular. For $`\tau _c>1`$, and contrary to the previous case, $`𝒢`$ decreases for increasing values of $`\tau _c`$ (Fig. 2a). This reduction of $`𝒢`$ can be atributed to the formation of the coherent superposition of the Kondo states. This can be clearly seen as a splitting $`\mathrm{\Delta }=2\delta `$ in the dI/dV curves (Fig. 2c): Increasing $`\tau _c`$, the zero-bias conductance decreases whereas two maxima at $`\pm V_{peak}`$ show up (the arrow shows the splitting $`\mathrm{\Delta }=2V_{peak}`$ for the maximum value of $`\tau _c`$ in the figure). Fig. 2c demonstrates that the dI/dV curves of a DQD in the Kondo regime directly measure the coherent combination between the two many-body states in the QD’s. For larger voltages, the sharp drop of the current (Fig. 2a) reflects as strong NDC singularities in the dI/dV curves (Fig. 2b).

The position of these singularities moves towards higher $`|V|`$ as $`\tau _c`$ increases. In order to explain the results of Figs. 1 and 2, we plot in Fig. 3a $`ϵ_\pm `$ as a function of $`V0`$ for different values of $`\tau _c`$. For $`\tau _c=0`$ (thick solid line) , this corresponds to a plot of $`\stackrel{~}{ϵ}_L`$ and $`\stackrel{~}{ϵ}_R`$ (i.e the positions of the Kondo resonances for the decoupled QD’s) as a function of $`V`$. We obtain, as expected, that each Kondo resonance is pinned at the chemical potential of its own lead, $`\stackrel{~}{ϵ}_L=\mu _L=V/2`$ and $`\stackrel{~}{ϵ}_R=\mu _R=V/2`$. As the interdot coupling is turned on, the voltage dependence becomes strongly non-linear. For low V, the curves for $`\tau _c0`$ do not coincide with the curves for $`\tau _c=0`$ (i.e, $`\mu _{L/R}`$). This situation, however, changes as we increase $`V`$; the level positions $`ϵ_\pm `$ converge towards the chemical potentials $`\mu _{L/R}`$ in a non-trivial way.

The voltage $`V`$ for which $`ϵ^+ϵ^{}`$ coincides with the chemical potential difference $`V`$ gives the position of the peak in the positive side of the dI/dV (Fig.2c). This voltage is the solution of the equation $`\delta (V_{\mathrm{peak}})=V_{\mathrm{peak}}`$ where $`\delta (V)\sqrt{(\stackrel{~}{ϵ}_L\stackrel{~}{ϵ}_R)^2+4\stackrel{~}{t}_C^2}`$, with $`\stackrel{~}{ϵ}_{L/R}`$ given by Eq. (3). Note the implicit (and non-trivial) voltage dependence of $`\delta (V)`$. $`\stackrel{~}{\mathrm{\Gamma }}_L`$, $`\stackrel{~}{\mathrm{\Gamma }}_R`$ and $`\stackrel{~}{t}_C`$ follow a similar behavior as a function of $`V`$ (Figs. 3b, 3c and 3d). For $`VV_{\mathrm{peak}}`$, we find numerically that $`\delta (V)V`$, a relationship that becomes asymptotically exact as $`V\mathrm{}`$. The equation $`\delta (V)=V`$, has stable solutions $`\stackrel{~}{t}_C0`$ for $`[\frac{(\stackrel{~}{ϵ}_L\stackrel{~}{ϵ}_R)}{V}]^2<1`$, while for $`[\frac{(\stackrel{~}{ϵ}_L\stackrel{~}{ϵ}_R)}{V}]^2>1`$, the only stable solution is $`\stackrel{~}{t}_C=0`$, corresponding to current $`I=0`$. We denote the crossover voltage where $`[\frac{(\stackrel{~}{ϵ}_L\stackrel{~}{ϵ}_R)}{V}]^2=1`$ by $`V^{}`$. For finite voltages $`V>V_{\mathrm{peak}}`$, on the other hand, the relation $`\delta (V)=V`$ is only approximate, so that at the crossover $`V^{}`$, the quantity $`\stackrel{~}{t}_C`$ and hence $`I`$ drop to a much smaller, but still finite, value instead. Nevertheless the crossover at $`VV^{}`$ still indicates the beginning of the NDC region.

To illustrate this, we plot in Fig. 4 the left and right QD’s DOS for $`\tau _c=1`$. At equilibrium (V=0), the Kondo singularity at $`ϵ=0`$ splits into the $`ϵ_\pm `$ combinations. For $`V/T_K^0=2`$ the coherence is still preserved but the physical picture utterly changes for higher voltages ($`V/T_K^0=4`$ and $`V/T_K^0=6`$). In this case, the previous configuration is no longer stable, the coherence between dots is lost ($`\stackrel{~}{t}_C0`$), the dots are almost decoupled and the Kondo resonances in each dot are pinned again at their own chemical potential: the weight of the left (right) DOS at $`ϵ=\mu _{R(L)}`$ is almost zero (even though $`\tau _c=1`$).   
This instability resembles that of the SB at $`T0`$ in the single impurity Anderson hamiltonian.  In the MFA the SB behaves as the order parameter associated with the conservation of $`Q`$. When $`\stackrel{~}{b}0`$ the gauge symmetry $`bbe^{i\theta }`$, $`ffe^{i\theta }`$ associated with charge conservation is broken and the MFA has two phases $`\stackrel{~}{b}0`$ and $`\stackrel{~}{b}=0`$ separated by a second order phase transition. It is important to point out that the fluctuations do not destroy completely this $`\stackrel{~}{b}0`$ behavior (the SB fluctuations develop power law behavior replacing the transition by a smooth crossover). We speculate that in our problem this zero-temperature transition at finite V may be also robust against fluctuations but $`1/N`$ corrections are needed to substantiate this argument. Work in this direction is in progress.

In closing, we have demonstrated that the non-linear transport properties $`(dI/dV)`$ of a DQD in the Kondo regime directly measures the transition (as $`t_C`$ increases) from two isolated Kondo impurities to a coherent bonding and antibonding superposition of the many-body Kondo states of each dot. While for $`t_C<\mathrm{\Gamma }`$ the conductance maximum is at $`V=0`$, for $`t_C>\mathrm{\Gamma }`$ the transport is optimized for a finite $`V`$ matching the splitting between these two bonding and antibonding states. For large voltages (and $`t_C\mathrm{\Gamma }`$) there is a critical voltage above which the coherent superposition is unstable and the physical behavior of the system again resembles that of two decoupled QD’s. This leads a strong reduction of the current and singular regions of negative differential conductance. Concerning the observability of these effects: In our MFA the maximum value of $`\delta `$ ranges from $`\delta 20T_K^0500T_K^0`$ (inset of Fig. 3a) giving, for the experiment of Ref.  ($`\mathrm{\Gamma }150\mu eV`$), $`\delta 3\mu eV75\mu eV`$ (30mK-750mK) which is within the resolution limits of present day techniques.   
This work was supported by the NSF grant DMR 97-08499, DOE grant DE-FG02-99ER45970 and by the MEC of Spain grant PF 98-07497938.