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# Current induced entanglement of nuclear spins in quantum dots

(October 10, 2002)

## Abstract

We propose an entanglement mechanism of nuclear spins in quantum dots driven by the electric current. The current accompanied by the spin flip in quantum dots gradually increases components of larger total spin of nuclei. This entangled state drastically enhances the spin relaxation rate of electrons, which can be detected by measuring a leakage current in the spin-blockade region. This mechanism is not relevant in optical experiments which examine the spin relaxation of single excitations.

The spin relaxation time of electrons in quantum dots is an important issue. The time needs to be sufficiently long for the implementation of quantum computing devices utilizing electron spins in quantum dots Loss . The relaxation time has been found to be quite long by optical opt1 ; opt2  and transport experiments Fujisawa ; Ono . In the former experiments, the transient measurements indicate a quenching of the spin relaxation on the exciton lifetime scale in self-assembled quantum dots. In the latter experiments, the tunneling current is measured through single or double quantum dots in “spin blockade” situations, where electrons cannot be transported unless the spins are flipped in the dot. The relaxation time is as long as $`200`$ $`\mu `$s from a spin-triplet excited state to spin-singlet ground state in single quantum dots Fujisawa . In weakly coupled double quantum dots, the current suppression has been observed when two electrons occupy the lowest energy level in each dot with parallel spins: an electron tunneling from one dot to the other is forbidden by the Pauli exclusion principle Ono .

In the present paper, we theoretically study a small leakage current in spin-blockade regions. The current is accompanied by the spin flip in the quantum dots. As a spin-flip mechanism, we investigate the hyperfine interaction between electrons and nuclear spins Sigurdur ; Sigurdur2 . Recent experimental results have implied its important roles in the leakage current Ono2 . We examine a formation of entangled states of nuclear spins driven by the electron transport. This mechanism is analogous to the current induced dynamic nuclear polarization (DNP) in quantum Hall systems DNP ; Machida . The DNP is created by the electron scattering between spin-polarized regions, which leads to a hysterisis in the longitudinal resistance Kronmuller ; Smet . In our case, the entanglement of nuclear spins drastically enhances the spin relaxation rate of electrons in quantum dots, which could be observed experimentally. This mechanism is not relevant in the optical experiments which examine the spin relaxation of single excitations. Hence the role of the hyperfine interaction in the spin relaxation could be quite different in transport and optical experiments.

Model: To consider the spin blockade in quantum dots, we adopt a following model. A quantum dot is weakly coupled to external leads L,R through tunnel barriers. The Coulomb blockade restricts the number of electrons in the dot to be $`N_{\mathrm{el}}`$ or $`N_{\mathrm{el}}+1`$. $`N_{\mathrm{el}}`$ electrons form a background of spin singlet. From lead L on the source side, an extra electron tunnels into the dot and occupies a single level with envelope wavefunction $`\psi (𝐫)`$. The spin of the electron is either $``$ ($`S_z=1/2`$) or $``$ ($`S_z=1/2`$) with equal probability (we assume an easy-axis of electron spins in $`z`$ direction for a while). The electron stays for a long time by the spin blockade com0  because the spin relaxation time is much longer than the tunneling time. After the spin flip in the dot, the electron immediately tunnels out to lead R on the drain side, and then the next electron is injected from lead L.

An electron occupying orbital $`\psi (𝐫)`$ interacts with $`N`$ nuclear spins, $`𝐈_k`$, by the hyperfine contact interaction. $`N10^5`$ in GaAs quantum dots. We assume nuclear spins of $`1/2`$ for simplicity. The Hamiltonian in the dot reads

$$H_{\mathrm{hf}}=A\underset{k=1}{\overset{N}{}}v_0|\psi (𝐫_k)|^2𝐒𝐈_k2\alpha 𝐒𝐈,$$
(1)
where $`v_0`$ is the volume of the crystal cell and $`𝐈=_{k=1}^N𝐈_k`$ is the total spin of nuclei. We have assumed that $`\psi (𝐫)`$ is independent of the nuclear site, $`𝐫_k`$. This is a good approximation for a large part of nuclear spins in the quantum dot, except in the vicinity of nodes of $`\psi (𝐫)`$, since the distance between nuclei is much smaller than the size of the dot, or an extension of $`\psi (𝐫)`$.

Basic idea: The Hamiltonian (1) indicates that $`N`$ nuclear spins interact with a common “field” of electron spin although there is no direct interaction between them (dipole-dipole interaction between nuclear spins is weak and neglected). This field results in the entanglement among the nuclear spins. To illustrate this, let us consider the simplest case of $`N=2`$ and begin with a polarized state of nuclear spins $`|I_z=1/2_1|I_z=1/2_2`$. An electron with spin $`|`$ tunnels into the dot and is spin-flipped by the hyperfine interaction. Then the state of nuclear spins becomes $`(|1/2_1|1/2_2+|1/2_1|1/2_2)/\sqrt{2}=|J=1,M=0`$, where $`J`$ and $`M`$ are the total spin and its $`z`$ component, respectively. This is an entangled state. After the electron tunnels out of the dot, the next electron is injected with $`|`$ (or $`|`$). The spin-flip probability of the second electron is proportional to $`|1,1;()|H_{\mathrm{hf}}|1,0;()|^2=2\alpha ^2`$. This value is twice the probability in the case of non-entangled states $`|1/2_1|1/2_2`$ or $`|1/2_1|1/2_2`$. In general, the capability of state $`|J,M`$ to flip an electron spin is $`(J\pm M)(JM+1)`$.

In presence of easy-axis: We formulate the entanglement of $`N`$ nuclear spins. In the initial state, they are not entangled at all and oriented randomly

$`\mathrm{\Psi }^{(0)}`$ $`=`$ $`(c_1|1/2_1+d_1|1/2_1)\mathrm{}`$ (2)
$``$ $`(c_N|1/2_N+d_N|1/2_N).`$
$`\{c_k,d_k\}`$ are randomly distributed $`(|c_k|^2+|d_k|^2=1)`$. By the transformation of the basis set from $`\{|I_z_1|I_z_2\mathrm{}\}`$ to the total spin of all the nuclei, $`\{|J,M\}`$ ($`JN/2`$, $`JMJ`$), Eq. (2) is rewritten as

$$\mathrm{\Psi }^{(0)}=\underset{J,M,\lambda }{}C_{J,M,\lambda }^{(0)}|J,M,\lambda ,$$
(3)
where the coefficients $`\{C_{J,M,\lambda }^{(0)}\}`$ are randomly distributed ($`_{J,M,\lambda }|C_{J,M,\lambda }^{(0)}|=1`$). Index $`\lambda `$ distinguishes states with the same $`J`$ and $`M`$. The number of such states is given by

$$K(N,J)=(2J+1)\frac{N!}{(\frac{N+2J+2}{2})!(\frac{N2J}{2})!}.$$
(4)
After the injection of the first electron, say, $`|`$, the time evolution of the dot state by $`H_{\mathrm{hf}}`$ is

$`e^{iH_{\mathrm{hf}}t/\mathrm{}}\mathrm{\Psi }^{(0)}|={\displaystyle \underset{J,M,\lambda }{}}C_{J,M,\lambda }^{(0)}{\displaystyle \frac{e^{i\alpha Jt/\mathrm{}}}{2J+1}}\left[JM+1+(J+M)e^{i\alpha (2J+1)t/\mathrm{}}\right]|J,M,\lambda |`$
$`+{\displaystyle \underset{J,M,\lambda }{}}C_{J,M,\lambda }^{(0)}\sqrt{(J+M)(JM+1)}{\displaystyle \frac{e^{i\alpha Jt/\mathrm{}}}{2J+1}}(1e^{i\alpha (2J+1)t/\mathrm{}})|J,M1,\lambda |.`$ (5)
The expansion to the lowest order in $`\alpha t/\mathrm{}`$ yields the spin-flip probability, $`P^{(0)}=F^{(0)}(\alpha t/\mathrm{})^2`$, with

$$F^{(0)}=\underset{J,M,\lambda }{}|C_{J,M,\lambda }^{(0)}|^2(J\pm M)(JM+1)$$
(6)
(the lower sign indicates the electron spin flip from $`|`$ to $`|`$). When $`N1`$, $`|C_{J,M,\lambda }^{(0)}|^2`$ can be replaced by $`1/2^N`$ (law of large number). Then $`F^{(0)}=(1/2^N)_{J,M}K(N,J)(J\pm M)(JM+1)=N/2`$. $`P^{(0)}=(N/2)(\alpha t/\mathrm{})^2`$ is identical to the spin-flip probability which would be evaluated on the assumption that one of the nuclear spins is flipped with the electron spin.

The electron tunnels off the dot immediately after the spin is flipped. Then the wavefunction $`\mathrm{\Psi }^{(0)}`$ shrinks to

$`\mathrm{\Psi }^{(1)}={\displaystyle \frac{1}{\sqrt{F^{(0)}}}}{\displaystyle \underset{J,M,\lambda }{}}C_{J,M,\lambda }^{(0)}\sqrt{(J\pm M)(JM+1)}`$
$`\times |J,M1,\lambda .`$ (7)
$`\mathrm{\Psi }^{(1)}`$ is partly entangled since it contains more components of larger $`J`$ and smaller $`|M|`$. The degree of the entanglement increases each time an electron is injected, spin-flipped, and ejected out of the dot. After $`n`$ events, the state of nuclear spins becomes

$`\mathrm{\Psi }^{(n)}`$ $`=`$ $`{\displaystyle \underset{J,M,\lambda }{}}C_{J,M,\lambda }^{(n)}|J,M,\lambda ,`$ (8)
$`C_{J,M1,\lambda }^{(n)}`$ $`=`$ $`\sqrt{{\displaystyle \frac{(J\pm M)(JM+1)}{F^{(n1)}}}}C_{J,M,\lambda }^{(n1)},`$ (9)
$`F^{(n)}`$ $`=`$ $`{\displaystyle \underset{J,M,\lambda }{}}|C_{J,M,\lambda }^{(n)}|^2(J\pm M)(JM+1).`$ (10)
$`F^{(n)}`$ is expressed as

$`F^{(n)}`$ $`=`$ $`f^{(n)}/f^{(n1)},`$
$`f^{(n)}`$ $`=`$ $`{\displaystyle \frac{1}{2^N}}{\displaystyle \underset{J,M}{}}K(N,J)\left[(J\pm M)(JM+1)\right]^n.`$ (11)
Figure 1 shows the distribution of (a) the total spin $`J`$ and (b) its $`z`$ component $`M`$. The spin-flip processes increase the weight of larger $`J`$ and smaller $`|M|`$. Although $`M`$ changes less faster than $`J`$, this means that the total nuclear spins tend to develop in the plane perpendicular to the easy-axis of electron spins.

This entangled state enhances the spin-flip probability. For the $`(n+1)`$th electron, the probability is given by $`P^{(n)}=F^{(n)}(\alpha t/\mathrm{})^2`$. $`P^{(n)}`$ with fixed $`t`$ is shown by solid line in Fig. 2(a). Using Eq. (11), we find that $`F^{(n)}(N/2)n`$ for $`1nN/2`$, and $`F^{(n)}(N/2)^2`$ for $`N/2n`$. Therefore the probability increases with $`n`$ linearly ($`P^{(n)}nP^{(0)}`$) and finally saturates ($`P^{(n)}(N/2)P^{(0)}`$).

In absence of easy-axis: Until now, we have assumed the presence of easy-axis of electron spins. In the absence of the axis, the spin of the $`n`$th electron is oriented in an arbitrary direction, $`\mathrm{cos}\theta ^{(n)}|+\mathrm{sin}\theta ^{(n)}e^{i\phi ^{(n)}}|`$. In this case, the previous formulation can be applied after the rotation of $`\{C_{J,M,\lambda }^{(n)}\}`$, $`C_{J,M,\lambda }^{(n)}=_{M^{}=J}^JU(J,\theta ^{(n)},\phi ^{(n)})_{M,M^{}}C_{J,M^{},\lambda }^{(n)}`$, to align the $`z`$ axis parallel to the spin direction. If the spin direction of incident electrons is completely random, we can average over the $`z`$-component of the total spin. Then the coefficients $`\{C_{J,M,\lambda }^{(n)}\}`$ in Eq. (9) are replaced by the averaged values $`\{\overline{C}_{J,\lambda }^{(n)}\}`$. They develop by

$$\left|\overline{C}_{J,\lambda }^{(n)}\right|^2=\frac{1}{\sqrt{G^{(n1)}}}\frac{2}{3}J(J+1)\left|\overline{C}_{J,\lambda }^{(n1)}\right|^2,$$
(12)
where

$`G^{(n)}`$ $`=`$ $`g^{(n)}/g^{(n1)},`$
$`g^{(n)}`$ $`=`$ $`{\displaystyle \frac{1}{2^N}}{\displaystyle \underset{J}{}}K(N,J)(2J+1)\left[{\displaystyle \frac{2}{3}}J(J+1)\right]^n.`$ (13)
As in the previous case, components of larger $`J`$ increase with $`n`$, which enlarge the spin-flip probability by the factor of $`2J(J+1)/3`$. The probability is given by $`P(n)=G^{(n)}(\alpha t/\mathrm{})^2`$, which is shown by broken line in Fig. 2(a). This behaves as $`P^{(n)}(2n/3)P^{(0)}`$ for $`1nN/2`$, and $`P^{(n)}(N/3)P^{(0)}`$ for $`N/2n`$, with fixed $`t`$.

Leakage current: The enhancement of the spin-flip probability is reflected by the leakage current. Instead of calculating the current in the previous situations, now we consider the case in the presence of magnetic field: Zeeman energy for electrons is much larger than the hyperfine interaction, whereas that for nuclear spins is negligible. Then $`H_{\mathrm{hf}}`$ can be treated as a perturbation. The magnetic field makes an easy-axis of electron spins. We also take into account the electron-phonon interaction for the energy conservation at the spin flip Sigurdur2 . The Hamiltonian in the dot reads $`H=H_{\mathrm{el}}+H_{\mathrm{ph}}+H_{\mathrm{hf}}+H_{\mathrm{el}\mathrm{ph}}`$, where $`H_{\mathrm{el}}=E_\mathrm{Z}(a_{}^{}a_{}a_{}^{}a_{})`$, $`H_{\mathrm{ph}}=_𝐪\mathrm{}\omega _𝐪b_𝐪^{}b_𝐪`$, and $`H_{\mathrm{el}\mathrm{ph}}=_\sigma _𝐪\beta _𝐪a_\sigma ^{}a_\sigma (b_𝐪^{}+b_𝐪)`$, with $`a_\sigma ^{}`$, $`a_\sigma `$ ($`b_𝐪^{}`$, $`b_𝐪`$) being creation and annihilation operators for an electron in the dot (phonon). The spin-flip processes in the lowest order in $`H_{\mathrm{hf}}+H_{\mathrm{el}\mathrm{ph}}`$ (first orders in $`H_{\mathrm{hf}}`$ and in $`H_{\mathrm{el}\mathrm{ph}}`$) change the nuclear spin state in the same way as in Eq. (9) com1 .

The spin-flip rate for the $`(n+1)`$th electron is $`\mathrm{\Gamma }^{(n)}F^{(n)}`$. The time interval between $`n`$th and $`(n+1)`$th electron transports is $`\mathrm{\Delta }t^{(n)}1/\mathrm{\Gamma }^{(n)}`$. Thus the current is given by $`I(t)=e\mathrm{\Gamma }^{(n)}`$ at $`t=_{j=0}^n\mathrm{\Delta }t^{(j)}`$. This current is shown in Fig. 2(b), as a function of $`t`$ (solid line). The approximate form of $`F^{(n)}`$ yields an asymptotic form of the current

$$\{\begin{array}{cccc}I(t)\hfill & \hfill & e\mathrm{\Gamma }^{(0)}e^{\mathrm{\Gamma }^{(0)}t}\hfill & (tt_{\mathrm{sat}})\hfill \\ I(t)\hfill & \hfill & e(N/2)\mathrm{\Gamma }^{(0)}\hfill & (t_{\mathrm{sat}}t).\hfill \end{array}$$
(14)
The current grows with time drastically and finally saturates. The saturation time is given by $`t_{\mathrm{sat}}=\mathrm{ln}(N/2)/\mathrm{\Gamma }^{(0)}`$, where $`\mathrm{\Gamma }^{(0)}`$ is the spin-flip rate of an electron with the non-entangled state of nuclear spins. The increase in the current continues until the entangled state is broken by dephasing effects.

Even in the absence of magnetic field, the electron energies for $`|`$ and $`|`$ could be split in $`H_{\mathrm{el}}`$, $`e.g`$. by spin-singlet or -triplet formation with an electron trapped in the other dot, in double dot systems. In this case, the easy-axis of electrons would be absent (if the crystal field is weak enough). The perturbation with respect to $`H_{\mathrm{hf}}+H_{\mathrm{el}\mathrm{ph}}`$ changes the nuclear spin state following Eq. (12). The spin-flip rate is $`\mathrm{\Gamma }^{(n)}G^{(n)}`$. The leakage current $`I(t)`$ is represented by broken line in Fig. 2(b). It is written approximately as

$$\{\begin{array}{cccc}I(t)\hfill & \hfill & e(2\mathrm{\Gamma }^{(0)}/3)e^{2\mathrm{\Gamma }^{(0)}t/3}\hfill & (tt_{\mathrm{sat}})\hfill \\ I(t)\hfill & \hfill & e(N/3)\mathrm{\Gamma }^{(0)}\hfill & (t_{\mathrm{sat}}t),\hfill \end{array}$$
(15)
where $`t_{\mathrm{sat}}=3\mathrm{ln}(N/2)/(2\mathrm{\Gamma }^{(0)})`$. The enhancement of the current is less prominent than in the presence of easy-axis.

Discussion: We have proposed the current induced entanglement of nuclear spins in quantum dots. The current accompanied by the spin flip in the dots gradually increases components of larger total spin of nuclei, which significantly enhances the spin relaxation of electrons. As a result, the leakage current in the spin-blockade region grows drastically with time and finally saturates. This mechanism is not relevant in the optical experiments which examine the spin relaxation of single excitations.

The saturation time of the leakage current is of the same order as $`1/\mathrm{\Gamma }^{(0)}`$, spin relaxation time with non-entangled state of nuclear spins, which is $`100`$ ns or much larger Fujisawa ; Ono . The current is enhanced during the dephasing time $`T_2`$. When the entangled state is broken, the current is suppressed. Possibly this would result in a current fluctuation with time which has been observed recently Ono2 . The characteristic time of the fluctuation is $`T_2`$.

A possible origin of the dephasing is the dipole-dipole interaction between nuclear spins. Note that, among $`N`$ nuclear spins participating in the formation of total spin, $`|J,M`$, this interaction conserves the total spin, and hence does not destroy the entangled state. The interaction between one of the $`N`$ spins and a spin surrounding the dot results in the dephasing. Estimating $`T_2`$ in our case and analyzing evolution of nuclear spins after the dephasing are beyond the present paper.

We discuss the validity of our simple models. We have disregarded the spatial variation of the envelope wavefunction of electrons in the quantum dot. Although the entanglement of nuclear spins is generally seen in the presence of the variation (see Eq. (4) in Ref. Khaetskii2 ), the enhancement of the spin relaxation is more effective with larger total spin $`J`$. Hence the capability to flip an electron spin is determined by the effective number $`N_{\mathrm{eff}}`$ of nuclear spins which feel the same electron field, $`\psi (𝐫)=`$ const., since $`J_{\mathrm{max}}=N_{\mathrm{eff}}/2`$. The generalized evolution of nuclear spins is an interesting problem.

If the contribution from higher energy levels of electrons in quantum dots is not negligible, through electron-phonon interaction Sigurdur ; Sigurdur2  or spin-orbit (SO) interaction Khaetskii , it should be taken into account carefully. Particularly, the coexistence of hyperfine and SO interactions would complicate the evolution of the nuclear spin state because the terms of $`|`$ and $`|`$ are mixed on the right side of Eq. (5). We have also disregarded higher-order tunneling processes Averin , which could play a role in the spin relaxation of electrons Fujisawa . However, the processes do not influence the entanglement of nuclear spins discussed here.

Finally, we comment an analogy between our mechanism and the Dicke effect of superradiance Dicke ; Brandes . The spontaneous emission of photons is enhanced from $`N`$ atoms with two levels (pseudo-spin $`S_z=\pm 1/2`$) if all of them are excited initially. This is due to the formation of pseudo-spin state $`|J,M`$ with $`J=N/2`$. (Starting from $`|J,J`$, the state of $`N`$ atoms changes like a cascade, $`|J,J`$, $`|J,J1,\mathrm{}`$, emitting photons.) A similar effect has been proposed for the emission of phonons from $`N`$ equivalent quantum dots Brandes ; Brandes2 . The atoms (quantum dots) correspond to the nuclear spins in our model, while the emission of photons (phonons) to the spin flip of electrons. A main difference is the initialization. $`N`$ excited states have to be prepared by the pumping in the Dicke effect, whereas the initialization is not necessary in our mechanism.

The author gratefully acknowledges discussions with K. Kawamura, R. Fukuda, S. Komiyama, T. Inoshita, A. Shimizu, and K. Ono. Numerical calculations for Figs. 1 and 2 were performed by M. Murata.